Sample records for improving co2 efficiency

  1. Investigation of operating parameters on CO2 splitting by dielectric barrier discharge plasma

    NASA Astrophysics Data System (ADS)

    Pan, CHEN; Jun, SHEN; Tangchun, RAN; Tao, YANG; Yongxiang, YIN

    2017-12-01

    Experiments of CO2 splitting by dielectric barrier discharge (DBD) plasma were carried out, and the influence of CO2 flow rate, plasma power, discharge voltage, discharge frequency on CO2 conversion and process energy efficiency were investigated. It was shown that the absolute quantity of CO2 decomposed was only proportional to the amount of conductive electrons across the discharge gap, and the electron amount was proportional to the discharge power; the energy efficiency of CO2 conversion was almost a constant at a lower level, which was limited by CO2 inherent discharge character that determined a constant gap electric field strength. This was the main reason why CO2 conversion rate decreased as the CO2 flow rate increase and process energy efficiency was decreased a little as applied frequency increased. Therefore, one can improve the CO2 conversion by less feed flow rate or larger discharge power in DBD plasma, but the energy efficiency is difficult to improve.

  2. Solvent Effects on the Photothermal Regeneration of CO 2 in Monoethanolamine Nanofluids

    DOE PAGES

    Nguyen, Du; Stolaroff, Joshuah; Esser-Kahn, Aaron

    2015-11-02

    We present that a potential approach to reduce energy costs associated with carbon capture is to use external and renewable energy sources. The photothermal release of CO 2 from monoethanolamine mediated by nanoparticles is a unique solution to this problem. When combined with light-absorbing nanoparticles, vapor bubbles form inside the capture solution and release the CO 2 without heating the bulk solvent. The mechanism by which CO 2 is released remained unclear, and understanding this process would improve the efficiency of photothermal CO 2 release. Here we report the use of different cosolvents to improve or reduce the photothermal regenerationmore » of CO 2 captured by monoethanolamine. We found that properties that reduce the residence time of the gas bubbles (viscosity, boiling point, and convection direction) can enhance the regeneration efficiencies. The reduction of bubble residence times minimizes the reabsorption of CO 2 back into the capture solvent where bulk temperatures remain lower than the localized area surrounding the nanoparticle. These properties shed light on the mechanism of release and indicated methods for improving the efficiency of the process. We used this knowledge to develop an improved photothermal CO 2 regeneration system in a continuously flowing setup. Finally, using techniques to reduce residence time in the continuously flowing setup, such as alternative cosolvents and smaller fluid volumes, resulted in regeneration efficiency enhancements of over 200%.« less

  3. Solvent Effects on the Photothermal Regeneration of CO 2 in Monoethanolamine Nanofluids

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Nguyen, Du; Stolaroff, Joshuah; Esser-Kahn, Aaron

    We present that a potential approach to reduce energy costs associated with carbon capture is to use external and renewable energy sources. The photothermal release of CO 2 from monoethanolamine mediated by nanoparticles is a unique solution to this problem. When combined with light-absorbing nanoparticles, vapor bubbles form inside the capture solution and release the CO 2 without heating the bulk solvent. The mechanism by which CO 2 is released remained unclear, and understanding this process would improve the efficiency of photothermal CO 2 release. Here we report the use of different cosolvents to improve or reduce the photothermal regenerationmore » of CO 2 captured by monoethanolamine. We found that properties that reduce the residence time of the gas bubbles (viscosity, boiling point, and convection direction) can enhance the regeneration efficiencies. The reduction of bubble residence times minimizes the reabsorption of CO 2 back into the capture solvent where bulk temperatures remain lower than the localized area surrounding the nanoparticle. These properties shed light on the mechanism of release and indicated methods for improving the efficiency of the process. We used this knowledge to develop an improved photothermal CO 2 regeneration system in a continuously flowing setup. Finally, using techniques to reduce residence time in the continuously flowing setup, such as alternative cosolvents and smaller fluid volumes, resulted in regeneration efficiency enhancements of over 200%.« less

  4. Technological Innovations of Carbon Dioxide Injection in EAF-LF Steelmaking

    NASA Astrophysics Data System (ADS)

    Wei, Guangsheng; Zhu, Rong; Wu, Xuetao; Dong, Kai; Yang, Lingzhi; Liu, Runzao

    2018-06-01

    In this study, the recent innovations and improvements in carbon dioxide (CO2) injection technologies for electric arc furnace (EAF)-ladle furnace (LF) steelmaking processes have been reviewed. The utilization of CO2 in the EAF-LF steelmaking process resulted in improved efficiency, purity and environmental impact. For example, coherent jets with CO2 and O2 mixed injection can reduce the amount of iron loss and dust generation, and submerged O2 and powder injection with CO2 in an EAF can increase the production efficiency and improve the dephosphorization and denitrification characteristics. Additionally, bottom-blowing CO2 in an EAF can strengthen molten bath stirring and improve nitrogen removal, while bottom-blowing CO2 in a LF can increase the rate of desulfurization and improve the removal of inclusions. Based on these innovations, a prospective process for the cyclic utilization of CO2 in the EAF-LF steelmaking process is introduced that is effective in mitigating greenhouse gas emissions from the steelmaking shop.

  5. Technological Innovations of Carbon Dioxide Injection in EAF-LF Steelmaking

    NASA Astrophysics Data System (ADS)

    Wei, Guangsheng; Zhu, Rong; Wu, Xuetao; Dong, Kai; Yang, Lingzhi; Liu, Runzao

    2018-03-01

    In this study, the recent innovations and improvements in carbon dioxide (CO2) injection technologies for electric arc furnace (EAF)-ladle furnace (LF) steelmaking processes have been reviewed. The utilization of CO2 in the EAF-LF steelmaking process resulted in improved efficiency, purity and environmental impact. For example, coherent jets with CO2 and O2 mixed injection can reduce the amount of iron loss and dust generation, and submerged O2 and powder injection with CO2 in an EAF can increase the production efficiency and improve the dephosphorization and denitrification characteristics. Additionally, bottom-blowing CO2 in an EAF can strengthen molten bath stirring and improve nitrogen removal, while bottom-blowing CO2 in a LF can increase the rate of desulfurization and improve the removal of inclusions. Based on these innovations, a prospective process for the cyclic utilization of CO2 in the EAF-LF steelmaking process is introduced that is effective in mitigating greenhouse gas emissions from the steelmaking shop.

  6. Thermodynamic analysis of performance improvement by reheat on the CO2 transcritical power cycle

    NASA Astrophysics Data System (ADS)

    Tuo, Hanfei

    2012-06-01

    The CO2 transcritical rankine power cycle has been widely investigated recently, because of its better temperature glide matching between sensible heat source and working fluid in vapor generator, and its desirable qualities, such as moderate critical point, little environment impact and low cost. A reheat CO2 transcritical power cycle with two stage expansion is presented to improve baseline cycle performance in this paper. Energy and exergy analysis are carried out to investigate effects of important parameters on cycle performance. The main results show that reheat cycle performance is sensitive to the variation of medium pressures and the optimum medium pressures exist for maximizing work output and thermal efficiency, respectively. Reheat cycle is compared to baseline cycle under the same conditions. More significant improvements by reheat are obtained at lower turbine inlet temperatures and larger high cycle pressure. Work output improvement is much higher than thermal efficiency improvement, because extra waste heat is required to reheat CO2. Based on second law analysis, exergy efficiency of reheat cycle is also higher than that of baseline cycle, because more useful work is converted from waste heat. Reheat with two stage expansion has great potential to improve thermal efficiency and especially net work output of a CO2 transcritical power cycle using a low-grade heat source.

  7. Root Zone Cooling and Exogenous Spermidine Root-Pretreatment Promoting Lactuca sativa L. Growth and Photosynthesis in the High-temperature Season

    PubMed Central

    Sun, Jin; Lu, Na; Xu, Hongjia; Maruo, Toru; Guo, Shirong

    2016-01-01

    Root zone high-temperature stress is a major factor limiting hydroponic plant growth during the high-temperature season. The effects of root zone cooling (RZC; at 25°C) and exogenous spermidine (Spd) root-pretreatment (SRP, 0.1 mM) on growth, leaf photosynthetic traits, and chlorophyll fluorescence characteristics of hydroponic Lactuca sativa L. grown in a high-temperature season (average temperature > 30°C) were examined. Both treatments significantly promoted plant growth and photosynthesis in the high-temperature season, but the mechanisms of photosynthesis improvement in the hydroponic grown lettuce plants were different between the RZC and SRP treatments. The former improved plant photosynthesis by increasing stoma conductance (Gs) to enhance CO2 supply, thus promoting photosynthetic electron transport activity and phosphorylation, which improved the level of the photochemical efficiency of photosystem II (PSII), rather than enhancing CO2 assimilation efficiency. The latter improved plant photosynthesis by enhancing CO2 assimilation efficiency, rather than stomatal regulation. Combination of RZC and SRP significantly improved PN of lettuce plants in a high-temperature season by both improvement of Gs to enhance CO2 supply and enhancement of CO2 assimilation. The enhancement of photosynthetic efficiency in both treatments was independent of altering light-harvesting or excessive energy dissipation. PMID:27047532

  8. Root Zone Cooling and Exogenous Spermidine Root-Pretreatment Promoting Lactuca sativa L. Growth and Photosynthesis in the High-temperature Season.

    PubMed

    Sun, Jin; Lu, Na; Xu, Hongjia; Maruo, Toru; Guo, Shirong

    2016-01-01

    Root zone high-temperature stress is a major factor limiting hydroponic plant growth during the high-temperature season. The effects of root zone cooling (RZC; at 25°C) and exogenous spermidine (Spd) root-pretreatment (SRP, 0.1 mM) on growth, leaf photosynthetic traits, and chlorophyll fluorescence characteristics of hydroponic Lactuca sativa L. grown in a high-temperature season (average temperature > 30°C) were examined. Both treatments significantly promoted plant growth and photosynthesis in the high-temperature season, but the mechanisms of photosynthesis improvement in the hydroponic grown lettuce plants were different between the RZC and SRP treatments. The former improved plant photosynthesis by increasing stoma conductance (G s) to enhance CO2 supply, thus promoting photosynthetic electron transport activity and phosphorylation, which improved the level of the photochemical efficiency of photosystem II (PSII), rather than enhancing CO2 assimilation efficiency. The latter improved plant photosynthesis by enhancing CO2 assimilation efficiency, rather than stomatal regulation. Combination of RZC and SRP significantly improved P N of lettuce plants in a high-temperature season by both improvement of G s to enhance CO2 supply and enhancement of CO2 assimilation. The enhancement of photosynthetic efficiency in both treatments was independent of altering light-harvesting or excessive energy dissipation.

  9. China's Pathways to Achieving 40% ~ 45% Reduction in CO{sub 2} Emissions per Unit of GDP in 2020: Sectoral Outlook and Assessment of Savings Potential

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Zheng, Nina; Fridley, David; Zhou, Nan

    2011-09-30

    Achieving China’s goal of reducing its carbon intensity (CO{sub 2} per unit of GDP) by 40% to 45% percent below 2005 levels by 2020 will require the strengthening and expansion of energy efficiency policies across the buildings, industries and transport sectors. This study uses a bottom-up, end-use model and two scenarios -- an enhanced energy efficiency (E3) scenario and an alternative maximum technically feasible energy efficiency improvement (Max Tech) scenario – to evaluate what policies and technical improvements are needed to achieve the 2020 carbon intensity reduction target. The findings from this study show that a determined approach by Chinamore » can lead to the achievement of its 2020 goal. In particular, with full success in deepening its energy efficiency policies and programs but following the same general approach used during the 11th Five Year Plan, it is possible to achieve 49% reduction in CO{sub 2} emissions per unit of GDP (CO{sub 2} emissions intensity) in 2020 from 2005 levels (E3 case). Under the more optimistic but feasible assumptions of development and penetration of advanced energy efficiency technology (Max Tech case), China could achieve a 56% reduction in CO{sub 2} emissions intensity in 2020 relative to 2005 with cumulative reduction of energy use by 2700 Mtce and of CO{sub 2} emissions of 8107 Mt CO{sub 2} between 2010 and 2020. Energy savings and CO{sub 2} mitigation potential varies by sector but most of the energy savings potential is found in energy-intensive industry. At the same time, electricity savings and the associated emissions reduction are magnified by increasing renewable generation and improving coal generation efficiency, underscoring the dual importance of end-use efficiency improvements and power sector decarbonization.« less

  10. What China can learn from international policy experiences to improve industrial energy efficiency and reduce CO 2 emissions?

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Liu, Xu; Shen, Bo; Price, Lynn

    China’s industrial sector dominates the country’s total energy consumption and energy efficiency in the industry sector is crucial to help China reach its energy and CO 2 emissions reduction goals. There are many energy efficiency policies in China, but the motivation and willingness of enterprises to improve energy efficiency has weakened. This report first identifies barriers that enterprises face to be self-motivated to implement energy efficiency measures. Then, this report reviews international policies and programs to improve energy efficiency and evaluates how these policies helped to address the identified barriers. Lastly, this report draws conclusions and provides recommendations to Chinamore » in developing policies and programs to motivate enterprises to improve energy efficiency.« less

  11. Electrochemical separation of hydrogen from reformate using PEM fuel cell technology

    NASA Astrophysics Data System (ADS)

    Gardner, C. L.; Ternan, M.

    This article is an examination of the feasibility of electrochemically separating hydrogen obtained by steam reforming a hydrocarbon or alcohol source. A potential advantage of this process is that the carbon dioxide rich exhaust stream should be able to be captured and stored thereby reducing greenhouse gas emissions. Results are presented for the performance of the anode of proton exchange membrane (PEM) electrochemical cell for the separation of hydrogen from a H 2-CO 2 gas mixture and from a H 2-CO 2-CO gas mixture. Experiments were carried out using a single cell state-of-the-art PEM fuel cell. The anode was fed with either a H 2-CO 2 gas mixture or a H 2-CO 2-CO gas mixture and hydrogen was evolved at the cathode. All experiments were performed at room temperature and atmospheric pressure. With the H 2-CO 2 gas mixture the hydrogen extraction efficiency is quite high. When the gas mixture included CO, however, the hydrogen extraction efficiency is relatively poor. To improve the efficiency for the separation of the gas mixture containing CO, the effect of periodic pulsing on the anode potential was examined. Results show that pulsing can substantially reduce the anode potential thereby improving the overall efficiency of the separation process although the anode potential of the CO poisoned and pulsed cell still lies above that of an unpoisoned cell.

  12. Promoting helix pitch and trichome length to improve biomass harvesting efficiency and carbon dioxide fixation rate by Spirulina sp. in 660 m2 raceway ponds under purified carbon dioxide from a coal chemical flue gas.

    PubMed

    Cheng, Jun; Guo, Wangbiao; Ameer Ali, Kubar; Ye, Qing; Jin, Guiyong; Qiao, Zhanshan

    2018-08-01

    The helix pitch and trichome length of Spirulina sp. were promoted to improve the biomass harvesting efficiency and CO 2 fixation rate in 660 m 2 raceway ponds aerated with food-grade CO 2 purified from a coal chemical flue gas. The CO 2 fixation rate was improved with increased trichome length of the Spirulina sp. in a raceway pond with double paddlewheels, baffles, and CO 2 aerators (DBA raceway pond). The trichome length has increased by 33.3 μm, and CO 2 fixation rate has increased by 42.3% and peaked to 51.3 g/m 2 /d in a DBA raceway pond. Biomass harvesting efficiency was increased with increased helix pitch. When the day-average greenhouse temperature was 33 °C and day-average sunlight intensity was 72,100 lu×, the helix pitch of Spirulina sp. was increased to 56.2 μm. Hence the biomass harvesting efficiency was maximized to 75.6% and biomass actual yield was increased to 35.9 kg in a DBA raceway pond. Copyright © 2018 Elsevier Ltd. All rights reserved.

  13. Efficient utilization of greenhouse gases in a gas-to-liquids process combined with CO2/steam-mixed reforming and Fe-based Fischer-Tropsch synthesis.

    PubMed

    Zhang, Chundong; Jun, Ki-Won; Ha, Kyoung-Su; Lee, Yun-Jo; Kang, Seok Chang

    2014-07-15

    Two process models for carbon dioxide utilized gas-to-liquids (GTL) process (CUGP) mainly producing light olefins and Fischer-Tropsch (F-T) synthetic oils were developed by Aspen Plus software. Both models are mainly composed of a reforming unit, an F-T synthesis unit and a recycle unit, while the main difference is the feeding point of fresh CO2. In the reforming unit, CO2 reforming and steam reforming of methane are combined together to produce syngas in flexible composition. Meanwhile, CO2 hydrogenation is conducted via reverse water gas shift on the Fe-based catalysts in the F-T synthesis unit to produce hydrocarbons. After F-T synthesis, the unreacted syngas is recycled to F-T synthesis and reforming units to enhance process efficiency. From the simulation results, it was found that the carbon efficiencies of both CUGP options were successfully improved, and total CO2 emissions were significantly reduced, compared with the conventional GTL processes. The process efficiency was sensitive to recycle ratio and more recycle seemed to be beneficial for improving process efficiency and reducing CO2 emission. However, the process efficiency was rather insensitive to split ratio (recycle to reforming unit/total recycle), and the optimum split ratio was determined to be zero.

  14. Predicting the ultimate potential of natural gas SOFC power cycles with CO2 capture - Part B: Applications

    NASA Astrophysics Data System (ADS)

    Campanari, Stefano; Mastropasqua, Luca; Gazzani, Matteo; Chiesa, Paolo; Romano, Matteo C.

    2016-09-01

    An important advantage of solid oxide fuel cells (SOFC) as future systems for large scale power generation is the possibility of being efficiently integrated with processes for CO2 capture. Focusing on natural gas power generation, Part A of this work assessed the performances of advanced pressurised and atmospheric plant configurations (SOFC + GT and SOFC + ST, with fuel cell integration within a gas turbine or a steam turbine cycle) without CO2 separation. This Part B paper investigates such kind of power cycles when applied to CO2 capture, proposing two ultra-high efficiency plant configurations based on advanced intermediate-temperature SOFCs with internal reforming and low temperature CO2 separation process. The power plants are simulated at the 100 MW scale with a set of realistic assumptions about FC performances, main components and auxiliaries, and show the capability of exceeding 70% LHV efficiency with high CO2 capture (above 80%) and a low specific primary energy consumption for the CO2 avoided (1.1-2.4 MJ kg-1). Detailed results are presented in terms of energy and material balances, and a sensitivity analysis of plant performance is developed vs. FC voltage and fuel utilisation to investigate possible long-term improvements. Options for further improvement of the CO2 capture efficiency are also addressed.

  15. Mixed-Matrix Membranes Containing Carbon Nanotubes Composite with Hydrogel for Efficient CO2 Separation.

    PubMed

    Zhang, Haiyang; Guo, Ruili; Hou, Jinpeng; Wei, Zhong; Li, Xueqin

    2016-10-26

    In this study, a carbon nanotubes composite coated with N-isopropylacrylamide hydrogel (NIPAM-CNTs) was synthesized. Mixed-matrix membranes (MMMs) were fabricated by incorporating NIPAM-CNTs composite filler into poly(ether-block-amide) (Pebax MH 1657) matrix for efficient CO 2 separation. The as-prepared NIPAM-CNTs composite filler mainly plays two roles: (i) The extraordinary smooth one-dimensional nanochannels of CNTs act as the highways to accelerate CO 2 transport through membranes, increasing CO 2 permeability; (ii) The NIPAM hydrogel layer coated on the outer walls of CNTs acts as the super water absorbent to increase water content of membranes, appealing both CO 2 permeability and CO 2 /gas selectivity. MMM containing 5 wt % NIPAM-CNTs exhibited the highest CO 2 permeability of 567 barrer, CO 2 /CH 4 selectivity of 35, and CO 2 /N 2 selectivity of 70, transcending 2008 Robeson upper bound line. The improved CO 2 separation performance of MMMs is mainly attributed to the construction of the efficient CO 2 transport pathways by NIPAM-CNTs. Thus, MMMs incorporated with NIPAM-CNTs composite filler can be used as an excellent membrane material for efficient CO 2 separation.

  16. Photocatalytic degradation properties of V-doped TiO2 to automobile exhaust.

    PubMed

    Wang, Tong; Shen, Dongya; Xu, Tao; Jiang, Ruiling

    2017-05-15

    To improve the photocatalytic degradation properties of titanium dioxide (TiO 2 ) used as raw materials for purifying automobile exhaust (AE), the vanadium (V)-doped TiO 2 samples were prepared. The photocatalytic degradation efficiencies of V-doped TiO 2 to each component in AE were evaluated under ultraviolet (UV) and visible light irradiation, respectively. Results indicated that the photocatalytic activity of V-doped TiO 2 to AE was higher than that of pure TiO 2 , and the optimal V dopant content of TiO 2 was 1.0% under UV light irradiation. The degradation efficiencies of V-doped TiO 2 to NOx and HC were higher than those to CO 2 and CO in AE because of the reversible reaction between CO 2 and CO. In addition, it was found that the photocatalytic degradation efficiencies of V-doped TiO 2 to each component in AE were also increased under visible light irradiation. The V-doped TiO 2 also showed higher degradation efficiencies to NOx and HC than those to CO 2 and CO under visible light irradiation. The V doped TiO 2 presented higher photocatalytic activity to CO 2 than that to CO, but the reversible reaction between CO and CO 2 was not found under visible light irradiation. The photocatalytic reactions of pure and V-doped TiO 2 samples to each component in AE followed the first order kinetic pathway under the two light irradiations. It is concluded that the V doping is a feasible method to improve the photocatalytic degradation properties of TiO 2 to AE for air purification, developing a sustainable environmental purification technology based on TiO 2 materials. Copyright © 2017 Elsevier B.V. All rights reserved.

  17. High efficiency of CO2-activated graphite felt as electrode for vanadium redox flow battery application

    NASA Astrophysics Data System (ADS)

    Chang, Yu-Chung; Chen, Jian-Yu; Kabtamu, Daniel Manaye; Lin, Guan-Yi; Hsu, Ning-Yih; Chou, Yi-Sin; Wei, Hwa-Jou; Wang, Chen-Hao

    2017-10-01

    A simple method for preparing CO2-activated graphite felt as an electrode in a vanadium redox flow battery (VRFB) was employed by the direct treatment in a CO2 atmosphere at a high temperature for a short period. The CO2-activated graphite felt demonstrates excellent electrochemical activity and reversibility. The VRFB using the CO2-activated graphite felts in the electrodes has coulombic, voltage, and energy efficiencies of 94.52%, 88.97%, and 84.15%, respectively, which is much higher than VRFBs using the electrodes of untreated graphite felt and N2-activated graphite felt. The efficiency enhancement was attributed to the higher number of oxygen-containing functional groups on the graphite felt that are formed during the CO2-activation, leading to improving the electrochemical behaviour of the resultant VRFB.

  18. Integrating Waste Heat from CO 2 Removal and Coal-Fired Flue Gas to Increase Plant Efficiency

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Irvin, Nick; Kowalczyk, Joseph

    In project DE-FE0007525, Southern Company Services demonstrated heat integration methods for the capture and sequestration of carbon dioxide produced from pulverized coal combustion. A waste heat recovery technology (termed High Efficiency System) from Mitsubishi Heavy Industries America was integrated into an existing 25-MW amine-based CO 2 capture process (Kansai Mitsubishi Carbon Dioxide Recovery Process®1) at Southern Company’s Plant Barry to evaluate improvements in the energy performance of the pulverized coal plant and CO 2 capture process. The heat integration system consists of two primary pieces of equipment: (1) the CO 2 Cooler which uses product CO 2 gas from themore » capture process to heat boiler condensate, and (2) the Flue Gas Cooler which uses air heater outlet flue gas to further heat boiler condensate. Both pieces of equipment were included in the pilot system. The pilot CO 2 Cooler used waste heat from the 25-MW CO 2 capture plant (but not always from product CO 2 gas, as intended). The pilot Flue Gas Cooler used heat from a slipstream of flue gas taken from downstream of Plant Barry’s air heater. The pilot also included a 0.25-MW electrostatic precipitator. The 25-MW High Efficiency System operated for approximately six weeks over a four month time period in conjunction with the 25-MW CO 2 capture facility at Plant Barry. Results from the program were used to evaluate the technical and economic feasibility of full-scale implementation of this technology. The test program quantified energy efficiency improvements to a host power plant that could be realized due to the High Efficiency System. Through the execution of this project, the team verified the integrated operation of the High Efficiency System and Kansai Mitsubishi Carbon Dioxide Recovery Process®. The ancillary benefits of the High Efficiency System were also quantified, including reduced water consumption, a decrease in toxic air emissions, and better overall air quality control systems performance.« less

  19. Modification of nanostructured calcium carbonate for efficient gene delivery.

    PubMed

    Zhao, Dong; Wang, Chao-Qun; Zhuo, Ren-Xi; Cheng, Si-Xue

    2014-06-01

    In this study, a facile method to modify nanostructured calcium carbonate (CaCO3) gene delivery systems by adding calcium phosphate (CaP) component was developed. CaCO3/CaP/DNA nanoparticles were prepared by the co-precipitation of Ca(2+) ions with plasmid DNA in the presence of carbonate and phosphate ions. For comparison, CaCO3/DNA nanoparticles and CaP/DNA co-precipitates were also prepared. The effects of carbonate ion/phosphate ion (CO3(2-)/PO4(3-)) ratio on the particle size and gene delivery efficiency were investigated. With an appropriate CO3(2-)/PO4(3-) ratio, the co-existence of carbonate and phosphate ions could control the size of co-precipitates effectively, and CaCO3/CaP/DNA nanoparticles with a decreased size and improved stability could be obtained. The in vitro gene transfections mediated by different nanoparticles in 293T cells and HeLa cells were carried out, using pGL3-Luc as a reporter plasmid. The gene transfection efficiency of CaCO3/CaP/DNA nanoparticles could be significantly improved as compared with CaCO3/DNA nanoparticles and CaP/DNA co-precipitates. The confocal microscopy study indicated that the cellular uptake and nuclear localization of CaCO3/CaP/DNA nanoparticles were significantly enhanced as compared with unmodified CaCO3/DNA nanoparticles. Copyright © 2014 Elsevier B.V. All rights reserved.

  20. Ag-doped Co3O4 catalyst derived from heterometallic MOF for syngas production by electrocatalytic reduction of CO2 in water

    NASA Astrophysics Data System (ADS)

    Zhang, Shi-Yuan; Yang, Yuan-Yuan; Zheng, Yue-Qing; Zhu, Hong-Lin

    2018-07-01

    Electrocatalytic reduction of CO2 to useful fuels or chemicals is a promising path for carbon recycling. In this study, a novel mixed-metallic MOF [Ag4Co2(pyz)PDC4][Ag2Co(pyz)2PDC2] was synthesized, and it transformed into Ag doped Co3O4 catalyst, which exhibits excellent electro-catalytic performance for reduction of CO2 in water to syngas (H2 + CO). The as-prepared Ag/Co3O4 material exhibits a high selectivity of CO in 0.1 M KHCO3 aqueous solution (CO2 saturated) with the corresponding faradaic efficiency up to 55.6%. Compared with the Ag/Co3O4 electrode, the maximum faradaic efficiency (FE) of CO of pure Co3O4 is 21.3% at - 1.8 V vs. SCE. The results show that the presence of Ag can improve the efficiency of CO significantly, thereby inhibiting the production of H2. The stability of the samples can be maintained for more than 10 h at - 1.8 V vs. SCE. The ratio of production between H2 and CO can be controlled by varying the potential values.

  1. A data driven model for the impact of IFT and density variations on CO2 sequestration in porous media

    NASA Astrophysics Data System (ADS)

    Nomeli, Mohammad; Riaz, Amir

    2017-11-01

    CO2 storage in geological formations is one of the most promising solutions for mitigating the amount of greenhouse gases released into the atmosphere. One of the important issues for CO2 storage in subsurface environments is the sealing efficiency of low-permeable cap-rocks overlying potential CO2 storage reservoirs. A novel model is proposed to find the IFT of the systems (CO2/brine-salt) in a range of temperatures (300-373 K), pressures (50-250 bar), and up to 6 molal salinity applicable to CO2 storage in geological formations through a machine learning-assisted modeling of experimental data. The IFT between mineral surfaces and CO2/brine-salt solutions determines the efficiency of enhanced oil or gas recovery operations as well as our ability to inject and store CO2 in geological formations. Finally, we use the new model to evaluate the effects of formation depth on the actual efficiency of CO2 storage. The results indicate that, in the case of CO2 storage in deep subsurface environments as a global-warming mitigation strategy, CO2 storage capacity are improved with reservoir depth.

  2. Plasma-assisted CO2 conversion: optimizing performance via microwave power modulation

    NASA Astrophysics Data System (ADS)

    Britun, Nikolay; Silva, Tiago; Chen, Guoxing; Godfroid, Thomas; van der Mullen, Joost; Snyders, Rony

    2018-04-01

    Significant improvement in the energy efficiency of plasma-assisted CO2 conversion is achieved with applied power modulation in a surfaguide microwave discharge. The obtained values of CO2 conversion and energy efficiency are, respectively, 0.23 and 0.33 for a 0.95 CO2  +  0.05 N2 gas mixture. Analysis of the energy relaxation mechanisms shows that power modulation can potentially affect the vibrational-translational energy exchange in plasma. In our case, however, this mechanism does not play a major role, likely due to the low degree of plasma non-equilibrium in the considered pressure range. Instead, the gas residence time in the discharge active zone together with plasma pulse duration are found to be the main factors affecting the CO2 conversion efficiency at low plasma pulse repetition rates. This effect is confirmed experimentally by the in situ time-resolved two-photon absorption laser-induced fluorescence measurements of CO molecular density produced in the discharge as a result of CO2 decomposition.

  3. Global metabolic rewiring for improved CO2 fixation and chemical production in cyanobacteria.

    PubMed

    Kanno, Masahiro; Carroll, Austin L; Atsumi, Shota

    2017-03-13

    Cyanobacteria have attracted much attention as hosts to recycle CO 2 into valuable chemicals. Although cyanobacteria have been engineered to produce various compounds, production efficiencies are too low for commercialization. Here we engineer the carbon metabolism of Synechococcus elongatus PCC 7942 to improve glucose utilization, enhance CO 2 fixation and increase chemical production. We introduce modifications in glycolytic pathways and the Calvin Benson cycle to increase carbon flux and redirect it towards carbon fixation. The engineered strain efficiently uses both CO 2 and glucose, and produces 12.6 g l -1 of 2,3-butanediol with a rate of 1.1 g l -1  d -1 under continuous light conditions. Removal of native regulation enables carbon fixation and 2,3-butanediol production in the absence of light. This represents a significant step towards industrial viability and an excellent example of carbon metabolism plasticity.

  4. Global metabolic rewiring for improved CO2 fixation and chemical production in cyanobacteria

    NASA Astrophysics Data System (ADS)

    Kanno, Masahiro; Carroll, Austin L.; Atsumi, Shota

    2017-03-01

    Cyanobacteria have attracted much attention as hosts to recycle CO2 into valuable chemicals. Although cyanobacteria have been engineered to produce various compounds, production efficiencies are too low for commercialization. Here we engineer the carbon metabolism of Synechococcus elongatus PCC 7942 to improve glucose utilization, enhance CO2 fixation and increase chemical production. We introduce modifications in glycolytic pathways and the Calvin Benson cycle to increase carbon flux and redirect it towards carbon fixation. The engineered strain efficiently uses both CO2 and glucose, and produces 12.6 g l-1 of 2,3-butanediol with a rate of 1.1 g l-1 d-1 under continuous light conditions. Removal of native regulation enables carbon fixation and 2,3-butanediol production in the absence of light. This represents a significant step towards industrial viability and an excellent example of carbon metabolism plasticity.

  5. China's growing CO2 emissions--a race between increasing consumption and efficiency gains.

    PubMed

    Peters, Glen P; Weber, Christopher L; Guan, Dabo; Hubacek, Klaus

    2007-09-01

    China's rapidly growing economy and energy consumption are creating serious environmental problems on both local and global scales. Understanding the key drivers behind China's growing energy consumption and the associated CO2 emissions is critical for the development of global climate policies and provides insight into how other emerging economies may develop a low emissions future. Using recently released Chinese economic input-output data and structural decomposition analysis we analyze how changes in China's technology, economic structure, urbanization, and lifestyles affect CO2 emissions. We find that infrastructure construction and urban household consumption, both in turn driven by urbanization and lifestyle changes, have outpaced efficiency improvements in the growth of CO2 emissions. Net trade had a small effect on total emissions due to equal, but significant, growth in emissions from the production of exports and emissions avoided by imports. Technology and efficiency improvements have only partially offset consumption growth, but there remains considerable untapped potential to reduce emissions by improving both production and consumption systems. As China continues to rapidly develop there is an opportunity to further implement and extend policies, such as the Circular Economy, that will help China avoid the high emissions path taken by today's developed countries.

  6. Micromotor-Based Biomimetic Carbon Dioxide Sequestration: Towards Mobile Microscrubbers.

    PubMed

    Uygun, Murat; Singh, Virendra V; Kaufmann, Kevin; Uygun, Deniz A; de Oliveira, Severina D S; Wang, Joseph

    2015-10-26

    We describe a mobile CO2 scrubbing platform that offers a greatly accelerated biomimetic sequestration based on a self-propelled carbonic anhydrase (CA) functionalized micromotor. The CO2 hydration capability of CA is coupled with the rapid movement of catalytic micromotors, and along with the corresponding fluid dynamics, results in a highly efficient mobile CO2 scrubbing microsystem. The continuous movement of CA and enhanced mass transport of the CO2 substrate lead to significant improvements in the sequestration efficiency and speed over stationary immobilized or free CA platforms. This system is a promising approach to rapid and enhanced CO2 sequestration platforms for addressing growing concerns over the buildup of greenhouse gas. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  7. Technology advancement of the electrochemical CO2 concentrating process

    NASA Technical Reports Server (NTRS)

    Schubert, F. H.; Woods, R. R.; Hallick, T. M.; Heppner, D. B.

    1978-01-01

    The overall objectives of the present program are to: (1) improve the performance of the electrochemical CO2 removal technique by increasing CO2 removal efficiencies at pCO2 levels below 400 Pa, increasing cell power output and broadening the tolerance of electrochemical cells for operation over wide ranges of cabin relative humidity; (2) design, fabricate, and assemble development hardware to continue the evolution of the electrochemical concentrating technique from the existing level to an advanced level able to efficiently meet the CO2 removal needs of a spacecraft air revitalization system (ARS); (3) develop and incorporate into the EDC the components and concepts that allow for the efficient integration of the electrochemical technique with other subsystems to form a spacecraft ARS; (4) combine ARS functions to enable the elimination of subsystem components and interfaces; and (5) demonstrate the integration concepts through actual operation of a functionally integrated ARS.

  8. Oxygen Vacancies in ZnO Nanosheets Enhance CO2 Electrochemical Reduction to CO.

    PubMed

    Geng, Zhigang; Kong, Xiangdong; Chen, Weiwei; Su, Hongyang; Liu, Yan; Cai, Fan; Wang, Guoxiong; Zeng, Jie

    2018-05-22

    As electron transfer to CO 2 is generally considered to be the critical step during the activation of CO 2 , it is important to develop approaches to engineer the electronic properties of catalysts to improve their performance in CO 2 electrochemical reduction. Herein, we developed an efficient strategy to facilitate CO 2 activation by introducing oxygen vacancies into electrocatalysts with electronic-rich surface. ZnO nanosheets rich in oxygen vacancies exhibited a current density of -16.1 mA cm -2 with a Faradaic efficiency of 83 % for CO production. Based on density functional theory (DFT) calculations, the introduction of oxygen vacancies increased the charge density of ZnO around the valence band maximum, resulting in the enhanced activation of CO 2 . Mechanistic studies further revealed that the enhancement of CO production by introducing oxygen vacancies into ZnO nanosheets originated from the increased binding strength of CO 2 and the eased CO 2 activation. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  9. Improved Efficiency of Miscible CO(2) Floods and Enhanced Prospects for CO(2) Flooding Heterogeneous Reservoirs.

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Grigg, R.B.; Schechter, D.S.

    The overall goal of this project was to improve the efficiency of miscible C0{sub 2} floods and enhance the prospects for flooding heterogeneous reservoirs. This objective was accomplished through experimental and modeling research in three task areas: (1) foams for selective mobility control in heterogeneous reservoirs,( 2) reduction of the amount of C0{sub 2} required in C0{sub 2} floods, and (3) low IFT processe and the possibility of C0{sub 2} flooding in fractured reservoirs. This report provides results from the three-year project for each of the three task areas.

  10. Copper nanoparticle interspersed MoS2 nanoflowers with enhanced efficiency for CO2 electrochemical reduction to fuel.

    PubMed

    Shi, Guodong; Yu, Luo; Ba, Xin; Zhang, Xiaoshu; Zhou, Jianqing; Yu, Ying

    2017-08-15

    Electrocatalytic conversion of carbon dioxide (CO 2 ) has been considered as an ideal method to simultaneously solve the energy crisis and environmental issue around the world. In this work, ultrasmall Cu nanoparticle interspersed flower-like MoS 2 was successfully fabricated via a facile microwave hydrothermal method. The designed optimal hierarchical Cu/MoS 2 composite not only exhibited remarkably enhanced electronic conductivity and specific surface area but also possessed improved CO 2 adsorption capacity, resulting in a significant increase in overall faradaic efficiency and a 7-fold augmentation of the faradaic efficiency of CH 4 in comparison with bare MoS 2 . In addition, the Cu/MoS 2 composite had superior stability with high efficiency retained for 48 h in the electrochemical process. It is anticipated that the designed Cu/MoS 2 composite electrocatalyst may provide new insights for transition metal sulfides and non-noble particles applied to CO 2 reduction.

  11. Reduced and Validated Kinetic Mechanisms for Hydrogen-CO-sir Combustion in Gas Turbines

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Yiguang Ju; Frederick Dryer

    2009-02-07

    Rigorous experimental, theoretical, and numerical investigation of various issues relevant to the development of reduced, validated kinetic mechanisms for synthetic gas combustion in gas turbines was carried out - including the construction of new radiation models for combusting flows, improvement of flame speed measurement techniques, measurements and chemical kinetic analysis of H{sub 2}/CO/CO{sub 2}/O{sub 2}/diluent mixtures, revision of the H{sub 2}/O{sub 2} kinetic model to improve flame speed prediction capabilities, and development of a multi-time scale algorithm to improve computational efficiency in reacting flow simulations.

  12. Reduction of CO2 to C1 products and fuel

    USGS Publications Warehouse

    Mill, T.; Ross, D.

    2002-01-01

    Photochemical semiconductor processes readily reduced CO2 to a broad range of C1 products. However the intrinsic and solar efficiencies for the processes were low. Improved quantum efficiencies could be realized utilizing quantum-sized particles, but at the expense of using less of the visible solar spectrum. Conversely, semiconductors with small bandgaps used more of the visible solar spectrum at the expense of quantum efficiency. Thermal reduction of CO2 with Fe(II) was thermodynamically favored for forming many kinds of organic compounds and occurred readily with olivine and other Fe(II) minerals above 200??C to form higher alkanes and alkenes. No added hydrogen was required.

  13. Effects of recent energy system changes on CO2 projections for the United States.

    PubMed

    Lenox, Carol S; Loughlin, Daniel H

    2017-09-21

    Recent projections of future United States carbon dioxide (CO 2 ) emissions are considerably lower than projections made just a decade ago. A myriad of factors have contributed to lower forecasts, including reductions in end-use energy service demands, improvements in energy efficiency, and technological innovations. Policies that have encouraged these changes include renewable portfolio standards, corporate vehicle efficiency standards, smart growth initiatives, revisions to building codes, and air and climate regulations. Understanding the effects of these and other factors can be advantageous as society evaluates opportunities for achieving additional CO 2 reductions. Energy system models provide a means to develop such insights. In this analysis, the MARKet ALlocation (MARKAL) model was applied to estimate the relative effects of various energy system changes that have happened since the year 2005 on CO 2 projections for the year 2025. The results indicate that transformations in the transportation and buildings sectors have played major roles in lowering projections. Particularly influential changes include improved vehicle efficiencies, reductions in projected travel demand, reductions in miscellaneous commercial electricity loads, and higher efficiency lighting. Electric sector changes have also contributed significantly to the lowered forecasts, driven by demand reductions, renewable portfolio standards, and air quality regulations.

  14. Improved CO sub 2 enhanced oil recovery -- Mobility control by in-situ chemical precipitation

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Ameri, S.; Aminian, K.; Wasson, J.A.

    1991-06-01

    The overall objective of this study has been to evaluate the feasibility of chemical precipitation to improve CO{sub 2} sweep efficiency and mobility control. The laboratory experiments have indicated that carbonate precipitation can alter the permeability of the core samples under reservoir conditions. Furthermore, the relative permeability measurements have revealed that precipitation reduces the gas permeability in favor of liquid permeability. This indicates that precipitation is occurring preferentially in the larger pores. Additional experimental work with a series of connected cores have indicated that the permeability profile can be successfully modified. However, Ph control plays a critical role in propagationmore » of the chemical precipitation reaction. A numerical reservoir model has been utilized to evaluate the effects of permeability heterogeneity and permeability modification on the CO{sub 2} sweep efficiency. The computer simulation results indicate that the permeability profile modification can significantly enhance CO{sub 2} vertical and horizontal sweep efficiencies. The scoping studies with the model have further revealed that only a fraction of high permeability zones need to be altered to achieve sweep efficiency enhancement. 64 refs., 30 figs., 16 tabs.« less

  15. Highly efficient and autocatalytic H2O dissociation for CO2 reduction into formic acid with zinc

    PubMed Central

    Jin, Fangming; Zeng, Xu; Liu, Jianke; Jin, Yujia; Wang, Lunying; Zhong, Heng; Yao, Guodong; Huo, Zhibao

    2014-01-01

    Artificial photosynthesis, specifically H2O dissociation for CO2 reduction with solar energy, is regarded as one of the most promising methods for sustainable energy and utilisation of environmental resources. However, a highly efficient conversion still remains extremely challenging. The hydrogenation of CO2 is regarded as the most commercially feasible method, but this method requires either exotic catalysts or high-purity hydrogen and hydrogen storage, which are regarded as an energy-intensive process. Here we report a highly efficient method of H2O dissociation for reducing CO2 into chemicals with Zn powder that produces formic acid with a high yield of approximately 80%, and this reaction is revealed for the first time as an autocatalytic process in which an active intermediate, ZnH− complex, serves as the active hydrogen. The proposed process can assist in developing a new concept for improving artificial photosynthetic efficiency by coupling geochemistry, specifically the metal-based reduction of H2O and CO2, with solar-driven thermochemistry for reducing metal oxide into metal. PMID:24675820

  16. Surface Immobilization of Transition Metal Ions on Nitrogen-Doped Graphene Realizing High-Efficient and Selective CO2 Reduction.

    PubMed

    Bi, Wentuan; Li, Xiaogang; You, Rui; Chen, Minglong; Yuan, Ruilin; Huang, Weixin; Wu, Xiaojun; Chu, Wangsheng; Wu, Changzheng; Xie, Yi

    2018-05-01

    Electrochemical conversion of CO 2 to value-added chemicals using renewable electricity provides a promising way to mitigate both global warming and the energy crisis. Here, a facile ion-adsorption strategy is reported to construct highly active graphene-based catalysts for CO 2 reduction to CO. The isolated transition metal cyclam-like moieties formed upon ion adsorption are found to contribute to the observed improvements. Free from the conventional harsh pyrolysis and acid-leaching procedures, this solution-chemistry strategy is easy to scale up and of general applicability, thus paving a rational avenue for the design of high-efficiency catalysts for CO 2 reduction and beyond. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  17. Effects of fully open-air [CO2] elevation on leaf photosynthesis and ultrastructure of Isatis indigotica fort.

    PubMed

    Hao, Xingyu; Li, Ping; Feng, Yongxiang; Han, Xue; Gao, Ji; Lin, Erda; Han, Yuanhuai

    2013-01-01

    Traditional Chinese medicine relies heavily on herbs, yet there is no information on how these herb plants would respond to climate change. In order to gain insight into such response, we studied the effect of elevated [CO2] on Isatis indigotica Fort, one of the most popular Chinese herb plants. The changes in leaf photosynthesis, chlorophyll fluorescence, leaf ultrastructure and biomass yield in response to elevated [CO2] (550±19 µmol mol(-1)) were determined at the Free-Air Carbon dioxide Enrichment (FACE) experimental facility in North China. Photosynthetic ability of I. indigotica was improved under elevated [CO2]. Elevated [CO2] increased net photosynthetic rate (P N), water use efficiency (WUE) and maximum rate of electron transport (J max) of upper most fully-expended leaves, but not stomatal conductance (gs), transpiration ratio (Tr) and maximum velocity of carboxylation (V c,max). Elevated [CO2] significantly increased leaf intrinsic efficiency of PSII (Fv'/Fm') and quantum yield of PSII(ΦPS II ), but decreased leaf non-photochemical quenching (NPQ), and did not affect leaf proportion of open PSII reaction centers (qP) and maximum quantum efficiency of PSII (Fv/Fm). The structural chloroplast membrane, grana layer and stroma thylakoid membranes were intact under elevated [CO2], though more starch grains were accumulated within the chloroplasts than that of under ambient [CO2]. While the yield of I. indigotica was higher due to the improved photosynthesis under elevated [CO2], the content of adenosine, one of the functional ingredients in indigowoad root was not affected.

  18. Electrochemical carbon dioxide concentrator subsystem development

    NASA Technical Reports Server (NTRS)

    Koszenski, E. P.; Heppner, D. B.; Bunnell, C. T.

    1986-01-01

    The most promising concept for a regenerative CO2 removal system for long duration manned space flight is the Electrochemical CO2 Concentrator (EDC), which allows for the continuous, efficient removal of CO2 from the spacecraft cabin. This study addresses the advancement of the EDC system by generating subsystem and ancillary component reliability data through extensive endurance testing and developing related hardware components such as electrochemical module lightweight end plates, electrochemical module improved isolation valves, an improved air/liquid heat exchanger and a triple redundant relative humidity sensor. Efforts included fabrication and testing the EDC with a Sabatier CO2 Reduction Reactor and generation of data necessary for integration of the EDC into a space station air revitalization system. The results verified the high level of performance, reliability and durability of the EDC subsystem and ancillary hardware, verified the high efficiency of the Sabatier CO2 Reduction Reactor, and increased the overall EDC technology engineering data base. The study concluded that the EDC system is approaching the hardware maturity levels required for space station deployment.

  19. Nuclear techniques for the on-line bulk analysis of carbon in coal-fired power stations.

    PubMed

    Sowerby, B D

    2009-09-01

    Carbon trading schemes usually require large emitters of CO(2), such as coal-fired power stations, to monitor, report and be audited on their CO(2) emissions. The emission price provides a significant additional incentive for power stations to improve efficiency. In the present paper, previous work on the bulk determination of carbon in coal is reviewed and assessed. The most favourable method is that based on neutron inelastic scattering. The potential role of on-line carbon analysers in improving boiler efficiency and in carbon accounting is discussed.

  20. Impact of co-pretreatment of calcium hydroxide and steam explosion on anaerobic digestion efficiency with corn stover.

    PubMed

    Ji, Jinli; Zhang, Jiyu; Yang, Liutianyi; He, Yanfeng; Zhang, Ruihong; Liu, Guangqing; Chen, Chang

    2017-06-01

    Anaerobic digestion (AD) is an effective way to utilize the abundant resource of corn stover (CS). In this light, Ca(OH) 2 pretreatment alone, steam explosion (SE) pretreatment alone, and co-pretreatment of Ca(OH) 2 and SE were applied to improve the digestion efficiency of CS. Results showed that AD of co-pretreated CS with 1.0% Ca(OH) 2 and SE at 1.5 MPa achieved the highest cumulative methane yield of [Formula: see text], which was 61.54% significantly higher (p < .01) than untreated CS. The biodegradability value of CS after co-pretreatment enhanced from 43.03% to 69.52%. Methane yield could be well fitted by the first-order model and the modified Gompertz model. In addition, composition and structural changes of CS after pretreatment were analyzed by a fiber analyzer, scanning electron microscopy, Fourier transform infrared spectroscopy, and X-ray diffraction. The validated results indicated that co-pretreatment of Ca(OH) 2 and SE was efficient to improve the digestion performance of CS and might be a suitable method for agricultural waste pretreatment in the future AD industry.

  1. The role of polymer dots on efficiency enhancement of organic solar cells: Improving charge transport property

    NASA Astrophysics Data System (ADS)

    Li, Jinfeng; Zhang, Xinyuan; Liu, Chunyu; Li, Zhiqi; He, Yeyuan; Zhang, Zhihui; Shen, Liang; Guo, Wenbin; Ruan, Shengping

    2017-07-01

    In this work, poly(9,9-dioctylfluorene)-co-(4,7-di-2-thienyl-2,1,3-benzothiadiazole) (PF-5DTBT) and copolymer poly(styrene-co-maleic anhydride) (PSMA) dots were prepared as additive for active layer doping to enhance the power conversion efficiency (PCE) of organic solar cells (OSCs), which based on poly[N-9″-hepta-decanyl-2,7-carbazole-alt-5,5-(4‧,7‧-di-2-thienyl-2‧,1‧,3‧-benzothiadiazole) (PCDTBT) and [6,6]-phenyl C71 butyric acid methyl-ester (PC71BM). A high efficiency of 7.40% was achieved due to increase of short-circuit current (Jsc) and fill factor (FF). The operation mechanism of OSCs doping with polymer dots was investigated, which demonstrated that the efficiency enhancement ascribes to improvement of electrical properties, such as exciton generation, exction dissociation, charge transport, and charge collection.

  2. Improving yield potential in crops under elevated CO2: Integrating the photosynthetic and nitrogen utilization efficiencies

    PubMed Central

    Kant, Surya; Seneweera, Saman; Rodin, Joakim; Materne, Michael; Burch, David; Rothstein, Steven J.; Spangenberg, German

    2012-01-01

    Increasing crop productivity to meet burgeoning human food demand is challenging under changing environmental conditions. Since industrial revolution atmospheric CO2 levels have linearly increased. Developing crop varieties with increased utilization of CO2 for photosynthesis is an urgent requirement to cope with the irreversible rise of atmospheric CO2 and achieve higher food production. The primary effects of elevated CO2 levels in most crop plants, particularly C3 plants, include increased biomass accumulation, although initial stimulation of net photosynthesis rate is only temporal and plants fail to sustain the maximal stimulation, a phenomenon known as photosynthesis acclimation. Despite this acclimation, grain yield is known to marginally increase under elevated CO2. The yield potential of C3 crops is limited by their capacity to exploit sufficient carbon. The “C fertilization” through elevated CO2 levels could potentially be used for substantial yield increase. Rubisco is the rate-limiting enzyme in photosynthesis and its activity is largely affected by atmospheric CO2 and nitrogen availability. In addition, maintenance of the C/N ratio is pivotal for various growth and development processes in plants governing yield and seed quality. For maximizing the benefits of elevated CO2, raising plant nitrogen pools will be necessary as part of maintaining an optimal C/N balance. In this review, we discuss potential causes for the stagnation in yield increases under elevated CO2 levels and explore possibilities to overcome this limitation by improved photosynthetic capacity and enhanced nitrogen use efficiency. Opportunities of engineering nitrogen uptake, assimilatory, and responsive genes are also discussed that could ensure optimal nitrogen allocation toward expanding source and sink tissues. This might avert photosynthetic acclimation partially or completely and drive for improved crop production under elevated CO2 levels. PMID:22833749

  3. Improving yield potential in crops under elevated CO(2): Integrating the photosynthetic and nitrogen utilization efficiencies.

    PubMed

    Kant, Surya; Seneweera, Saman; Rodin, Joakim; Materne, Michael; Burch, David; Rothstein, Steven J; Spangenberg, German

    2012-01-01

    Increasing crop productivity to meet burgeoning human food demand is challenging under changing environmental conditions. Since industrial revolution atmospheric CO(2) levels have linearly increased. Developing crop varieties with increased utilization of CO(2) for photosynthesis is an urgent requirement to cope with the irreversible rise of atmospheric CO(2) and achieve higher food production. The primary effects of elevated CO(2) levels in most crop plants, particularly C(3) plants, include increased biomass accumulation, although initial stimulation of net photosynthesis rate is only temporal and plants fail to sustain the maximal stimulation, a phenomenon known as photosynthesis acclimation. Despite this acclimation, grain yield is known to marginally increase under elevated CO(2). The yield potential of C(3) crops is limited by their capacity to exploit sufficient carbon. The "C fertilization" through elevated CO(2) levels could potentially be used for substantial yield increase. Rubisco is the rate-limiting enzyme in photosynthesis and its activity is largely affected by atmospheric CO(2) and nitrogen availability. In addition, maintenance of the C/N ratio is pivotal for various growth and development processes in plants governing yield and seed quality. For maximizing the benefits of elevated CO(2), raising plant nitrogen pools will be necessary as part of maintaining an optimal C/N balance. In this review, we discuss potential causes for the stagnation in yield increases under elevated CO(2) levels and explore possibilities to overcome this limitation by improved photosynthetic capacity and enhanced nitrogen use efficiency. Opportunities of engineering nitrogen uptake, assimilatory, and responsive genes are also discussed that could ensure optimal nitrogen allocation toward expanding source and sink tissues. This might avert photosynthetic acclimation partially or completely and drive for improved crop production under elevated CO(2) levels.

  4. Constructing Ordered Three-Dimensional TiO2 Channels for Enhanced Visible-Light Photocatalytic Performance in CO2 Conversion Induced by Au Nanoparticles.

    PubMed

    Xue, Hairong; Wang, Tao; Gong, Hao; Guo, Hu; Fan, Xiaoli; Gao, Bin; Feng, Yaya; Meng, Xianguang; Huang, Xianli; He, Jianping

    2018-03-02

    As a typical photocatalyst for CO 2 reduction, practical applications of TiO 2 still suffer from low photocatalytic efficiency and limited visible-light absorption. Herein, a novel Au-nanoparticle (NP)-decorated ordered mesoporous TiO 2 (OMT) composite (OMT-Au) was successfully fabricated, in which Au NPs were uniformly dispersed on the OMT. Due to the surface plasmon resonance (SPR) effect derived from the excited Au NPs, the TiO 2 shows high photocatalytic performance for CO 2 reduction under visible light. The ordered mesoporous TiO 2 exhibits superior material and structure, with a high surface area that offers more catalytically active sites. More importantly, the three-dimensional transport channels ensure the smooth flow of gas molecules, highly efficient CO 2 adsorption, and the fast and steady transmission of hot electrons excited from the Au NPs, which lead to a further improvement in the photocatalytic performance. These results highlight the possibility of improving the photocatalysis for CO 2 reduction under visible light by constructing OMT-based Au-SPR-induced photocatalysts. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  5. Regeneration of 2-amino-2-methyl-1-propanol used for carbon dioxide absorption.

    PubMed

    Zhang, Pei; Shi, Yao; Wei, Jianwen; Zhao, Wei; Ye, Qing

    2008-01-01

    To improve the efficiency of the carbon dioxide cycling process and to reduce the regeneration energy consumption, a sterically hindered amine of 2-amino-2-methyl-1-propranol (AMP) was investigated to determine its regeneration behavior as a CO2 absorbent. The CO2 absorption and amine regeneration characteristics were experimentally examined under various operating conditions. The regeneration efficiency increased from 86.2% to 98.3% during the temperature range of 358 to 403 K. The most suitable regeneration temperature for AMP was 383 K, in this experiment condition, and the regeneration efficiency of absorption/regenerationruns descended from 98.3% to 94.0%. A number of heat-stable salts (HSS) could cause a reduction in CO2 absorption capacity and regeneration efficiency. The results indicated that aqueous AMP was easier to regenerate with less loss of absorption capacity than other amines, such as, monoethanolamine (MEA), diethanolamine (DEA), diethylenetriamine (DETA), and N-methyldiethanolamine (MDEA).

  6. Efficiency trends for new commercial jet aircraft 1960-2008

    DOT National Transportation Integrated Search

    2009-11-01

    Concerns about aviations growing climate impact have revived interest in CO2 emission standards for new aircraft. To date, commercial aviation has been perceived to produce continuous improvements in efficiency by quickly adopting fuel-efficient t...

  7. Amorphizing of Cu Nanoparticles toward Highly Efficient and Robust Electrocatalyst for CO2 Reduction to Liquid Fuels with High Faradaic Efficiencies.

    PubMed

    Duan, Yan-Xin; Meng, Fan-Lu; Liu, Kai-Hua; Yi, Sha-Sha; Li, Si-Jia; Yan, Jun-Min; Jiang, Qing

    2018-04-01

    Conversion of carbon dioxide (CO 2 ) into valuable chemicals, especially liquid fuels, through electrochemical reduction driven by sustainable energy sources, is a promising way to get rid of dependence on fossil fuels, wherein developing of highly efficient catalyst is still of paramount importance. In this study, as a proof-of-concept experiment, first a facile while very effective protocol is proposed to synthesize amorphous Cu NPs. Unexpectedly, superior electrochemical performances, including high catalytic activity and selectivity of CO 2 reduction to liquid fuels are achieved, that is, a total Faradaic efficiency of liquid fuels can sum up to the maximum value of 59% at -1.4 V, with formic acid (HCOOH) and ethanol (C 2 H 6 O) account for 37% and 22%, respectively, as well as a desirable long-term stability even up to 12 h. More importantly, this work opens a new avenue for improved electroreduction of CO 2 based on amorphous metal catalysts. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  8. Methanol from CO2 by organo-cocatalysis: CO2 capture and hydrogenation in one process step.

    PubMed

    Reller, Christian; Pöge, Matthias; Lißner, Andreas; Mertens, Florian O R L

    2014-12-16

    Carbon dioxide chemically bound to alcohol-amines was hydrogenated to methanol under retrieval of these industrially used CO2 capturing reagents. The energetics of the process can be seen as a partial cancellation of the exothermic heat of reaction of the hydrogenation with the endothermic one of the CO2 release from the capturing reagent. The process provides a means to significantly improve the energy efficiency of CO2 to methanol conversions.

  9. Conversion of CO2 to CO using radio-frequency atmospheric pressure plasmas

    NASA Astrophysics Data System (ADS)

    Foote, Alexander; Dedrick, James; O'Connell, Deborah; North, Michael; Gans, Timo

    2016-09-01

    Low temperature plasmas can be used for the in situ generation of CO, from relatively non-toxic CO2 . CO is very useful in many industrial chemical processes and so, via low temperature plasmas, CO2, a waste product, can be converted into a valuable chemical. The key challenges in using this method, for CO production, are optimising the energy efficiency, maximising the conversion of CO2 into CO and then separating the CO from the other species produced in the plasma. Very high yields of CO, greater than 90%, have been achieved at atmospheric pressure using argon as a carrier gas with admixtures up to 1.5% with energy efficiencies of up to 4%. The plasma generated in continuous and spatially homogeneous and is driven at a frequency of 40.68 MHz. A zero dimensional global model has also been used to simulate the chemical kinetics of the plasma to determine the dominant dissociation processes and is in good agreement with the experimentally determined yields. The model is used to determine how important a role the vibrational states of CO2 are, in a highly collisional plasma, to the production of CO and there can provide insight into how to improve the energy efficiency and suppress unwanted reactions.

  10. Microfluidic study for investigating migration and residual phenomena of supercritical CO2 in porous media

    NASA Astrophysics Data System (ADS)

    Park, Gyuryeong; Wang, Sookyun; Lee, Minhee; Um, Jeong-Gi; Kim, Seon-Ok

    2017-04-01

    The storage of CO2 in underground geological formation such as deep saline aquifers or depleted oil and gas reservoirs is one of the most promising technologies for reducing the atmospheric CO2 release. The processes in geological CO2 storage involves injection of supercritical CO2 (scCO2) into porous formations saturated with brine and initiates CO2 flooding with immiscible displacement. The CO2 migration and porewater displacement within geological formations, and , consequentially, the storage efficiency are governed by the interaction of fluid and rock properties and are affected by the interfacial tension, capillarity, and wettability in supercritical CO2-brine-mineral systems. This study aims to observe the displacement pattern and estimate storage efficiency by using micromodels. This study aims to conduct scCO2 injection experiments for visualization of distribution of injected scCO2 and residual porewater in transparent pore networks on microfluidic chips under high pressure and high temperature conditions. In order to quantitatively analyze the porewater displacement by scCO2 injection under geological CO2 storage conditions, the images of invasion patterns and distribution of CO2 in the pore network are acquired through a imaging system with a microscope. The results from image analysis were applied in quantitatively investigating the effects of major environmental factors and scCO2 injection methods on porewater displacement process by scCO2 and storage efficiency. The experimental observation results could provide important fundamental information on capillary characteristics of reservoirs and improve our understanding of CO2 sequestration progress.

  11. Effect of the co-sensitization sequence on the performance of dye-sensitized solar cells with porphyrin and organic dyes.

    PubMed

    Fan, Suhua; Lu, Xuefeng; Sun, Hong; Zhou, Gang; Chang, Yuan Jay; Wang, Zhong-Sheng

    2016-01-14

    To obtain a broad spectral response in the visible region, TiO2 film is co-sensitized with a porphyrin dye (FNE57 or FNE59) and an organic dye (FNE46). It is found that the stepwise co-sensitization in one single dye solution followed by in another single dye solution is better than the co-sensitization in a cocktail solution in terms of photovoltaic performance. The stepwise co-sensitization first with a porphyrin dye and then with an organic dye outperforms that in a reverse order. DSSC devices based on co-sensitizers FNE57 + FNE46 and FNE59 + FNE46 with a quasi-solid-state gel electrolyte generate power conversion efficiencies of 7.88% and 8.14%, respectively, which exhibits remarkable efficiency improvements of 61% and 35%, as compared with devices sensitized with the porphyrin dyes FNE57 and FNE59, respectively. Co-sensitization brings about a much improved short-circuit photocurrent due to the complementary absorption of the two sensitizers. The observed enhancement of incident monochromatic photon-to-electron conversion efficiency from individual dye sensitization to co-sensitization is attributed to the improved charge collection efficiency rather than to the light harvesting efficiency. Interestingly, the open-circuit photovoltage for the co-sensitization system comes between the higher voltage for the porphyrin dye (FNE57 or FNE59) and the lower voltage for the organic dye (FNE46), which is well correlated with their electron lifetimes. This finding indicates that not only the spectral complementation but also the electron lifetime should be considered to select dyes for co-sensitization.

  12. Combustion characteristics of an SI engine fueled with biogas fuel

    NASA Astrophysics Data System (ADS)

    Chen, Lei; Long, Wuqiang; Song, Peng

    2017-04-01

    An experimental research of the effect of H2 substitution and CO2 dilution on CH4 combustion has been carried out on a spark ignition engine. The results show that H2 addition could improve BMEP, thermal efficiency, CO and THC emissions. NOX emissions increased for higher low heating value (LHV) of H2 than CH4. CO2 dilution could effective reduce NOX emission of H2-CH4 combustion. Although engine performance, thermal efficiency and exhaust get unacceptable under high fuel dilution ratio (F.D.R.) conditions, it could be solved by decreasing F.D.R. and/or increasing hydrogen substitution ratio (H.S.R.).

  13. On the potential for BECCS efficiency improvement through heat recovery from both post-combustion and oxy-combustion facilities.

    PubMed

    Dowell, N Mac; Fajardy, M

    2016-10-20

    In order to mitigate climate change to no more than 2 °C, it is well understood that it will be necessary to directly remove significant quantities of CO 2 , with bioenergy CCS (BECCS) regarded as a promising technology. However, BECCS will likely be more costly and less efficient at power generation than conventional CCS. Thus, approaches to improve BECCS performance and reduce costs are of importance to facilitate the deployment of this key technology. In this study, the impact of biomass co-firing rate and biomass moisture content on BECCS efficiency with both post- and oxy-combustion CO 2 capture technologies was evaluated. It was found that post-combustion capture BECCS (PCC-BECCS) facilities will be appreciably less efficient than oxy-combustion capture BECCS (OCC-BECCS) facilities. Consequently, PCC-BECCS have the potential to be more carbon negative than OCC-BECCS per unit electricity generated. It was further observed that the biomass moisture content plays an important role in determining the BECCS facilities' efficiency. This will in turn affect the enthalpic content of the BECCS plant exhaust and implies that exhaust gas heat recovery may be an attractive option at higher rates of co-firing. It was found that there is the potential for the recovery of approximately 2.5 GJ heat per t CO 2 at a temperature of 100 °C from both PCC-BECCS and OCC-BECCS. On- and off-site applications for this recovered heat are discussed, considering boiler feedwater pre-heating, solvent regeneration and district heating cases.

  14. Reduced SnO2 Porous Nanowires with a High Density of Grain Boundaries as Catalysts for Efficient Electrochemical CO2 -into-HCOOH Conversion.

    PubMed

    Kumar, Bijandra; Atla, Veerendra; Brian, J Patrick; Kumari, Sudesh; Nguyen, Tu Quang; Sunkara, Mahendra; Spurgeon, Joshua M

    2017-03-20

    Electrochemical conversion of CO 2 into energy-dense liquids, such as formic acid, is desirable as a hydrogen carrier and a chemical feedstock. SnO x is one of the few catalysts that reduce CO 2 into formic acid with high selectivity but at high overpotential and low current density. We show that an electrochemically reduced SnO 2 porous nanowire catalyst (Sn-pNWs) with a high density of grain boundaries (GBs) exhibits an energy conversion efficiency of CO 2 -into-HCOOH higher than analogous catalysts. HCOOH formation begins at lower overpotential (350 mV) and reaches a steady Faradaic efficiency of ca. 80 % at only -0.8 V vs. RHE. A comparison with commercial SnO 2 nanoparticles confirms that the improved CO 2 reduction performance of Sn-pNWs is due to the density of GBs within the porous structure, which introduce new catalytically active sites. Produced with a scalable plasma synthesis technology, the catalysts have potential for application in the CO 2 conversion industry. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  15. Gliding Arc Plasmatron: Providing an Alternative Method for Carbon Dioxide Conversion.

    PubMed

    Ramakers, Marleen; Trenchev, Georgi; Heijkers, Stijn; Wang, Weizong; Bogaerts, Annemie

    2017-06-22

    Low-temperature plasmas are gaining a lot of interest for environmental and energy applications. A large research field in these applications is the conversion of CO 2 into chemicals and fuels. Since CO 2 is a very stable molecule, a key performance indicator for the research on plasma-based CO 2 conversion is the energy efficiency. Until now, the energy efficiency in atmospheric plasma reactors is quite low, and therefore we employ here a novel type of plasma reactor, the gliding arc plasmatron (GAP). This paper provides a detailed experimental and computational study of the CO 2 conversion, as well as the energy cost and efficiency in a GAP. A comparison with thermal conversion, other plasma types and other novel CO 2 conversion technologies is made to find out whether this novel plasma reactor can provide a significant contribution to the much-needed efficient conversion of CO 2 . From these comparisons it becomes evident that our results are less than a factor of two away from being cost competitive and already outperform several other new technologies. Furthermore, we indicate how the performance of the GAP can still be improved by further exploiting its non-equilibrium character. Hence, it is clear that the GAP is very promising for CO 2 conversion. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  16. Exceptionally High Efficient Co-Co2P@N, P-Codoped Carbon Hybrid Catalyst for Visible Light-Driven CO2-to-CO Conversion.

    PubMed

    Fu, Wen Gan

    2018-05-02

    Artificial photosynthesis has attracted wide attention, particularly the development of efficient solar light-driven methods to reduce CO2 to form energy-rich carbon-based products. Because CO2 reduction is an uphill process with a large energy barrier, suitable catalysts are necessary to achieve this transformation. In addition, CO2 adsorption on a catalyst and proton transfer to CO2 are two important factors for the conversion reaction,and catalysts with high surface area and more active sites are required to improve the efficiency of CO2 reduction. Here, we report a visible light-driven system for CO2-to-CO conversion that consists of a heterogeneous hybrid catalyst of Co and Co2P nanoparticles embedded in carbon nanolayers codoped with N and P (Co-Co2P@NPC) and a homogeneous Ru(II)-based complex photosensitizer. The average generation rate of CO of the system was up to 35,000 μmol h-1 g-1 with selectivity of 79.1% in 3 h. Linear CO production at an exceptionally high rate of 63,000 μmol h-1 g-1 was observed in the first hour of reaction. Inspired by this highly active catalyst, we also synthesized Co@NC and Co2P@NPC materials and explored their structure, morphology, and catalytic properties for CO2 photoreduction. The results showed that the nanoparticle size, partially adsorbed H2O molecules on the catalyst surface, and the hybrid nature of the systems influenced their photocatalytic CO2 reduction performance. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  17. Highly efficient and autocatalytic H2₂ dissociation for CO₂ reduction into formic acid with zinc.

    PubMed

    Jin, Fangming; Zeng, Xu; Liu, Jianke; Jin, Yujia; Wang, Lunying; Zhong, Heng; Yao, Guodong; Huo, Zhibao

    2014-03-28

    Artificial photosynthesis, specifically H2O dissociation for CO2 reduction with solar energy, is regarded as one of the most promising methods for sustainable energy and utilisation of environmental resources. However, a highly efficient conversion still remains extremely challenging. The hydrogenation of CO2 is regarded as the most commercially feasible method, but this method requires either exotic catalysts or high-purity hydrogen and hydrogen storage, which are regarded as an energy-intensive process. Here we report a highly efficient method of H2O dissociation for reducing CO2 into chemicals with Zn powder that produces formic acid with a high yield of approximately 80%, and this reaction is revealed for the first time as an autocatalytic process in which an active intermediate, ZnH(-) complex, serves as the active hydrogen. The proposed process can assist in developing a new concept for improving artificial photosynthetic efficiency by coupling geochemistry, specifically the metal-based reduction of H2O and CO2, with solar-driven thermochemistry for reducing metal oxide into metal.

  18. Carbon-doped SnS2 nanostructure as a high-efficiency solar fuel catalyst under visible light.

    PubMed

    Shown, Indrajit; Samireddi, Satyanarayana; Chang, Yu-Chung; Putikam, Raghunath; Chang, Po-Han; Sabbah, Amr; Fu, Fang-Yu; Chen, Wei-Fu; Wu, Chih-I; Yu, Tsyr-Yan; Chung, Po-Wen; Lin, M C; Chen, Li-Chyong; Chen, Kuei-Hsien

    2018-01-12

    Photocatalytic formation of hydrocarbons using solar energy via artificial photosynthesis is a highly desirable renewable-energy source for replacing conventional fossil fuels. Using an L-cysteine-based hydrothermal process, here we synthesize a carbon-doped SnS 2 (SnS 2 -C) metal dichalcogenide nanostructure, which exhibits a highly active and selective photocatalytic conversion of CO 2 to hydrocarbons under visible-light. The interstitial carbon doping induced microstrain in the SnS 2 lattice, resulting in different photophysical properties as compared with undoped SnS 2 . This SnS 2 -C photocatalyst significantly enhances the CO 2 reduction activity under visible light, attaining a photochemical quantum efficiency of above 0.7%. The SnS 2 -C photocatalyst represents an important contribution towards high quantum efficiency artificial photosynthesis based on gas phase photocatalytic CO 2 reduction under visible light, where the in situ carbon-doped SnS 2 nanostructure improves the stability and the light harvesting and charge separation efficiency, and significantly enhances the photocatalytic activity.

  19. Low Work Function 2.81 eV Rb2CO3-Doped Polyethylenimine Ethoxylated for Inverted Organic Light-Emitting Diodes.

    PubMed

    Kim, Jeonggi; Kim, Hyo-Min; Jang, Jin

    2018-06-06

    We report a low work function (2.81 eV), Rb 2 CO 3 -doped polyethyleneimine ethoxylated (PEIE) which is used for highly efficient and long-lifetime, inverted organic light-emitting diodes (OLEDs). Doping Rb 2 CO 3 into PEIE decreases the work function of Li-doped ZnO (LZO) by 1.0 eV and thus significantly improves electron injection ability into the emission layer (EML). The inverted OLED with PEIE:Rb 2 CO 3 interfacial layer (IL) exhibits higher efficiency and longer operation lifetime than those of the device with a PEIE IL. It is found also that Mg-doped ZnO (MZO) can be used instead of LZO as electron transporting layer. Rb 2 CO 3 shows a low work function of 2.81 eV. The OLED with MZO/PEIE:Rb 2 CO 3 exhibits low operating voltage of 5.0 V at 1000 cd m -2 and low efficiency roll-off of 11.8% at high luminance of 10 000 cd m -2 . The results are due to the suppressed exciton quenching at the MZO/organic EML interface.

  20. Wood Combustion Behaviour in a Fixed Bed Combustor

    NASA Astrophysics Data System (ADS)

    Tokit, Ernie Mat; Aziz, Azhar Abdul; Ghazali, Normah Mohd

    2010-06-01

    Waste wood is used as feedstock for Universiti Teknologi Malaysia's newly-developed two-stage incinerator system. The research goals are to optimize the operation of the thermal system to the primary chamber, to improve its combustion efficiency and to minimize its pollutants formation. The combustion process is evaluated with the variation of fuel's moisture content. For optimum operating condition, where the gasification efficiency is 95.53%, the moisture content of the fuel is best set at 17%; giving outlet operating temperature of 550°C and exhaust gas concentrations with 1213 ppm of CO, 6% of CO2 and 14% of O2 respectively. In line to the experimental work, a computational fluid dynamics software, Fluent is used to simulate the performance of the primary chamber. Here the predicted optimum gasification efficiency stands at 95.49% with CO, CO2 and O2 concentrations as 1301 ppm, 6.5% and 13.5% respectively.

  1. New Directions for the Photocatalytic Reduction of CO2: Supramolecular, scCO2 or Biphasic Ionic Liquid-scCO2 Systems

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Grills, D.C.; Fujita, E.

    2010-09-02

    There is an urgent need for the discovery of carbon-neutral sources of energy to avoid the consequences of global warming caused by ever-increasing atmospheric CO{sub 2} levels. An attractive possibility is to use CO{sub 2} captured from industrial emissions as a feedstock for the production of useful fuels and precursors such as carbon monoxide and methanol. An active field of research to achieve this goal is the development of catalysts capable of harnessing solar energy for use in artificial photosynthetic processes for CO{sub 2} reduction. Transition-metal complexes are excellent candidates, and it has already been shown that they can bemore » used to reduce CO{sub 2} with high quantum efficiency. However, they generally suffer from poor visible light absorption, short catalyst lifetimes, and poor reaction rates. In this Perspective, the field of photocatalytic CO{sub 2} reduction is introduced, and recent developments that seek to improve the efficiency of such catalytic processes are highlighted, especially CO{sub 2} reduction with supramolecules and molecular systems in supercritical CO{sub 2} (scCO{sub 2}) or biphasic ionic liquid-scCO{sub 2} mixtures.« less

  2. A lyophilized and thermal two step synthesis of CoFe alloy nanoparticles embedded in N-doped carbon nanosheets/carbon nanotubes for highly-efficient oxygen evolution reaction.

    PubMed

    Liu, Yang; Li, Feng; Yang, Haidong; Li, Jing; Ma, Ping; Zhu, Yan; Ma, Jiantai

    2018-05-22

    There is a vital need to explore highly-efficient and stable nonprecious-metal catalysts for oxygen evolution reaction (OER) to reduce the overpotential and further improve the energy conversion efficiency. Herein, we report a unique and cost-effective lyophilized and thermal two step procedure to synthesize high-performance CoFe alloy nanoparticles embedded in N-doped carbon nanosheets interspersed with carbon nanotubes (CoFe-N-CN/CNTs) hybrid. The lyophilization step during catalysts preparation is beneficial to uniform the dispersion of carbon-like precursors and avoid the agglomeration of metal particles. Meanwhile, the inserted CNTs and doped N in this hybrid provide better electrical conductivity, more chemically active sites, improved mass transport capability and effective gas adsorption/release channels. And all these lead to a high specific surface area of 240.67 m2 g-1, favorable stability and remarkable OER activities with an overpotential of only 285 mV at the current density of 10 mA cm-2 and a Tafel slope of 51.09 mV dec-1 in 1.0 M KOH electrolyte, which is even superior to commercial IrO2 catalysts. The CoFe-N-CN/CNTs hybrid thus exhibits great potential as a highly efficient and earth-abundant anode OER electrocatalyst. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. Lvad pump speed increase is associated with increased peak exercise cardiac output and vo2, postponed anaerobic threshold and improved ventilatory efficiency.

    PubMed

    Vignati, Carlo; Apostolo, Anna; Cattadori, Gaia; Farina, Stefania; Del Torto, Alberico; Scuri, Silvia; Gerosa, Gino; Bottio, Tomaso; Tarzia, Vincenzo; Bejko, Jonida; Sisillo, Erminio; Nicoli, Flavia; Sciomer, Susanna; Alamanni, Francesco; Paolillo, Stefania; Agostoni, Piergiuseppe

    2017-03-01

    Peak exercise cardiac output (CO) increase is associated with an increase of peak oxygen uptake (VO 2 ), provided that arteriovenous O 2 difference [Δ(Ca-Cv)O 2 ] does not decrease. At anaerobic threshold, VO 2 , is related to CO. We tested the hypothesis that, in heart failure (HF) patients with left ventricular assistance device (LVAD), an acute increase of CO obtained through changes in LVAD pump speed is associated with peak exercise and anaerobic threshold VO 2 increase. Fifteen of 20 patients bearing LVAD (Jarvik 2000) enrolled in the study successfully performed peak exercise evaluation. All patients had severe HF as shown by clinical evaluation, laboratory tests, echocardiography, spirometry with alveolar-capillary diffusion, and maximal cardiopulmonary exercise testing (CPET). CPETs with non-invasive CO measurements at rest and peak exercise were done on 2days at LVAD pump speed set randomly at 2 and 4. Increasing LVAD pump speed from 2 to 4 increased CO from 3.4±0.9 to 3.8±1.0L/min (ΔCO 0.4±0.6L/min, p=0.04) and from 5.3±1.3 to 5.9±1.4L/min (ΔCO 0.6±0.7L/min, p<0.01) at rest and peak exercise, respectively. Similarly, VO 2 increased from 788±169 to 841±152mL/min (ΔVO 2 52±76mL/min, p=0.01) and from 568±116 to 619±124mL/min (ΔVO 2 69±96mL/min, p=0.02) at peak exercise and at anaerobic threshold, respectively. Δ(Ca-Cv)O 2 did not change significantly, while ventilatory efficiency improved (VE/VCO 2 slope from 39.9±5.4 to 34.9±8.3, ΔVE/VCO 2 -5.0±6.4, p<0.01). In HF, an increase in CO with a higher LVAD pump speed is associated with increased peak VO 2 , postponed anaerobic threshold, and improved ventilatory efficiency. Copyright © 2016 Elsevier Ireland Ltd. All rights reserved.

  4. Performance Enhancement of Organic Light-Emitting Diodes Using Electron-Injection Materials of Metal Carbonates

    NASA Astrophysics Data System (ADS)

    Shin, Jong-Yeol; Kim, Tae Wan; Kim, Gwi-Yeol; Lee, Su-Min; Shrestha, Bhanu; Hong, Jin-Woong

    2016-05-01

    Performance of organic light-emitting diodes was investigated depending on the electron-injection materials of metal carbonates (Li2CO3 and Cs2CO3 ); and number of layers. In order to improve the device efficiency, two types of devices were manufactured by using the hole-injection material (Teflon-amorphous fluoropolymer -AF) and electron-injection materials; one is a two-layer reference device ( ITO/Teflon-AF/Alq3/Al ) and the other is a three-layer device (ITO/Teflon-AF/Alq3/metal carbonate/Al). From the results of the efficiency for the devices with hole-injection layer and electron-injection layer, it was found that the electron-injection layer affects the electrical properties of the device more than the hole-injection layer. The external-quantum efficiency for the three-layer device with Li2CO3 and Cs2CO3 layer is improved by approximately six and eight times, respectively, compared with that of the two-layer reference device. It is thought that a use of electron-injection layer increases recombination rate of charge carriers by the active injection of electrons and the blocking of holes.

  5. Enhancing CO2 Electroreduction with the Metal-Oxide Interface.

    PubMed

    Gao, Dunfeng; Zhang, Yi; Zhou, Zhiwen; Cai, Fan; Zhao, Xinfei; Huang, Wugen; Li, Yangsheng; Zhu, Junfa; Liu, Ping; Yang, Fan; Wang, Guoxiong; Bao, Xinhe

    2017-04-26

    The electrochemical CO 2 reduction reaction (CO 2 RR) typically uses transition metals as the catalysts. To improve the efficiency, tremendous efforts have been dedicated to tuning the morphology, size, and structure of metal catalysts and employing electrolytes that enhance the adsorption of CO 2 . We report here a strategy to enhance CO 2 RR by constructing the metal-oxide interface. We demonstrate that Au-CeO x shows much higher activity and Faradaic efficiency than Au or CeO x alone for CO 2 RR. In situ scanning tunneling microscopy and synchrotron-radiation photoemission spectroscopy show that the Au-CeO x interface is dominant in enhancing CO 2 adsorption and activation, which can be further promoted by the presence of hydroxyl groups. Density functional theory calculations indicate that the Au-CeO x interface is the active site for CO 2 activation and the reduction to CO, where the synergy between Au and CeO x promotes the stability of key carboxyl intermediate (*COOH) and thus facilitates CO 2 RR. Similar interface-enhanced CO 2 RR is further observed on Ag-CeO x , demonstrating the generality of the strategy for enhancing CO 2 RR.

  6. From photons to biomass and biofuels: evaluation of different strategies for the improvement of algal biotechnology based on comparative energy balances.

    PubMed

    Wilhelm, Christian; Jakob, Torsten

    2011-12-01

    Microalgal based biofuels are discussed as future sustainable energy source because of their higher photosynthetic and water use efficiency to produce biomass. In the context of climate CO2 mitigation strategies, algal mass production is discussed as a potential CO2 sequestration technology which uses CO2 emissions to produce biomass with high-oil content independent on arable land. In this short review, it is presented how complete energy balances from photon to harvestable biomass can help to identify the limiting processes on the cellular level. The results show that high productivity is always correlated with high metabolic costs. The overall efficiency of biomass formation can be improved by a photobioreactor design which is kinetically adapted to the rate-limiting steps in cell physiology. However, taking into account the real photon demand per assimilated carbon and the energy input for biorefinement, it becomes obvious that alternative strategies must be developed to reach the goal of a real CO2 sequestration.

  7. Development of an activity-directed selection system enabled significant improvement of the carboxylation efficiency of Rubisco.

    PubMed

    Cai, Zhen; Liu, Guoxia; Zhang, Junli; Li, Yin

    2014-07-01

    Photosynthetic CO(2) fixation is the ultimate source of organic carbon on earth and thus is essential for crop production and carbon sequestration. Ribulose-1,5-bisphosphate carboxylase/oxygenase (Rubisco) catalyzes the first step of photosynthetic CO(2) fixation. However, the extreme low carboxylation efficiency of Rubisco makes it the most attractive target for improving photosynthetic efficiency. Extensive studies have focused on re-engineering a more efficient enzyme, but the effort has been impeded by the limited understanding of its structure-function relationships and the lack of an efficient selection system towards its activity. To address the unsuccessful molecular engineering of Rubisco, we developed an Escherichia coli-based activity-directed selection system which links the growth of host cell solely to the Rubisco activity therein. A Synechococcus sp. PCC7002 Rubisco mutant with E49V and D82G substitutions in the small subunit was selected from a total of 15,000 mutants by one round of evolution. This mutant showed an 85% increase in specific carboxylation activity and a 45% improvement in catalytic efficiency towards CO(2). The small-subunit E49V mutation was speculated to influence holoenzyme catalysis through interaction with the large-subunit Q225. This interaction is conserved among various Rubisco from higher plants and Chlamydomonas reinhardtii. Knowledge of these might provide clues for engineering Rubisco from higher plants, with the potential of increasing the crop yield.

  8. Self-Nanoemulsifying Drug Delivery System of Coenzyme (Q10) with Improved Dissolution, Bioavailability, and Protective Efficiency on Liver Fibrosis.

    PubMed

    Khattab, Abeer; Hassanin, Lobna; Zaki, Nashwah

    2017-07-01

    The aim of our investigation is to develop and characterize self-nanoemulsifying drug delivery systems (SNEDDS) of CoQ 10 to improve its water solubility, dissolution rate, and bioavailability, and then evaluate its biochemical and physiological effect on liver cirrhosis in rats compared with CoQ 10 powder. SNEDDS are isotropic and thermodynamically stable mixture of oil, surfactant, co-surfactant, and drug that form an oil/water nanoemulsion when added to aqueous phases with soft agitation. Upon administration, self-nanoemulsifying system becomes in contact with gastrointestinal fluid and forms o/w nanoemulsion by the aid of gastrointestinal motility. When the nanoemulsion is formed in the gastrointestinal tract, it presents the drug in a solubilized form inside small nano-sized droplets that provide a large surface area for enhancing the drug release and absorption. Solubility of CoQ 10 in various oils, surfactants, and co-surfactants were studied to identify the components of SNEDDS; pseudo-ternary phase diagrams were plotted to identify the efficient self-emulsifying regions. CoQ 10 -loaded SNEDDS were prepared using isopropyl myristate as oil; Cremophor El, Labrasol, or Tween80 as surfactant; and Transcutol as co-surfactant. The amount of CoQ 10 in each vehicle was 3%. The formulations that passed thermostability evaluation test were assessed for particle size analysis, morphological characterization, refractive index, zeta potential, viscosity, electroconductivity, drug release profile, as well as ex vivo permeability. Pharmacokinetics and hepatoprotective efficiency of the optimized SNEDDS of CoQ 10 compared with CoQ 10 suspension were performed. Results showed that all optimized formulae have the ability to form a good and stable nanoemulsion when diluted with water; the mean droplet size of all formulae was in the nanometric range (11.7-13.5 nm) with optimum polydispersity index values (0.2-0.21). All formulae showed negative zeta potential (-11.3 to -17.2), and maximum drug loading efficiency. One hundred percent of CoQ 10 was released from most formulae within 30 min. One hundred percent of CoQ 10 was permeated from all formulae through 10 h. The pharmacokinetic study in rabbits revealed a significant increase in bioavailability of CoQ 10 SNEDDS to 2.1-fold compared with CoQ 10 suspension after oral administration. Comparative effect of the optimized formulae on acute liver injury compared with CoQ 10 powder was also studied; it was found that all the liver biochemical markers as alanine transferase (ALT), aspartate amino transferase (AST), alkaline phosphatase (ALP), total protein (TP), and albumin were significantly improved at p < 0.05. Also, histochemical and histopthological studies confirm the biochemical results. Our results suggest the potential use of SNEDDS to increase the solubility of liphophilic drug as poorly water-soluble CoQ 10 and improve its oral absorption, so it can be more efficient to improve liver damage compared to CoQ 10 powder. These results demonstrated that CoQ 10 SNEDDS inhibited thioacetamide (TAA)-induced liver fibrosis mainly through suppression of collagen production.

  9. Mixed matrix membranes with fast and selective transport pathways for efficient CO2 separation

    NASA Astrophysics Data System (ADS)

    Hou, Jinpeng; Li, Xueqin; Guo, Ruili; Zhang, Jianshu; Wang, Zhongming

    2018-03-01

    To improve CO2 separation performance, porous carbon nanosheets (PCNs) were used as a filler into a Pebax MH 1657 (Pebax) matrix, fabricating mixed matrix membranes (MMMs). The PCNs exhibited a preferential horizontal orientation within the Pebax matrix because of the extremely large 2D plane and nanoscale thickness of the matrix. Therefore, the micropores of the PCNs provided fast CO2 transport pathways, which led to increased CO2 permeability. The reduced pore size of the PCNs was a consequence of the overlapping of PCNs and the polymer chains penetrating into the pores of the PCNs. The reduction in the pore size of the PCNs improved the CO2/gas selectivity. As a result, the CO2 permeability and CO2/CH4 selectivity of the Pebax membrane with 10 wt% PCNs-loading (Pebax-PCNs-10) were 520 barrer and 51, respectively, for CO2/CH4 mixed-gas. The CO2 permeability and CO2/N2 selectivity of the Pebax-PCNs-10 membrane were 614 barrer and 61, respectively, for CO2/N2 mixed-gas.

  10. Enhancing CO 2 electroreduction with the metal–oxide interface

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Gao, Dunfeng; Zhang, Yi; Zhou, Zhiwen

    2017-04-09

    Here, the electrochemical CO 2 reduction reaction (CO 2RR) typically uses transition metals as the catalysts. To improve the efficiency, tremendous efforts have been dedicated to tuning the morphology, size, and structure of metal catalysts and employing electrolytes that enhance the adsorption of CO 2. We report here a strategy to enhance CO 2RR by constructing the metal–oxide interface. We demonstrate that Au–CeO x shows much higher activity and Faradaic efficiency than Au or CeO x alone for CO 2RR. In situ scanning tunneling microscopy and synchrotron-radiation photoemission spectroscopy show that the Au–CeO x interface is dominant in enhancing COmore » 2 adsorption and activation, which can be further promoted by the presence of hydroxyl groups. Density functional theory calculations indicate that the Au–CeO x interface is the active site for CO 2 activation and the reduction to CO, where the synergy between Au and CeO x promotes the stability of key carboxyl intermediate (*COOH) and thus facilitates CO 2RR. Similar interface-enhanced CO 2RR is further observed on Ag–CeO x, demonstrating the generality of the strategy for enhancing CO 2RR.« less

  11. Visible-light-sensitive titanium dioxide nanoplatform for tumor-responsive Fe2+ liberating and artemisinin delivery

    PubMed Central

    Zhang, Huijuan; Zhang, Hongling; Zhu, Xing; Zhang, Xiaoge; Chen, Qianqian; Chen, Jianjiao; Hou, Lin; Zhang, Zhenzhong

    2017-01-01

    Artemisinin is a kind of Fe2+-dependent drugs. Artemisinin and Fe2+ co-transport systems can improve its anti-tumor effect. In this study, a visible light-sensitive nanoplatform (HA-TiO2-IONPs/ART) was developed. Detailed investigation demonstrated that HA-TiO2-IONPs/ART could realize Fe2+ and artemisinin synchronous co-delivery and tumor-responsive release. This feature enhanced the anti-tumor efficiency of artemisinin significantly. In vitro results proved that hyaluronic acid modification could improve the biocompatibility, dispersion stability and cytophagy ability of nanocarriers. Furthermore, this drug delivery system could generate reactive oxygen species under visual light irradiation. In vitro and in vivo experiments demonstrated that HA-TiO2-IONPs/ART combining with laser irradiation displayed the best anti-tumor efficacy. This study affords a promising idea to improve the curative efficiency of artemisinin analogs for cancer therapy. PMID:28938592

  12. U.S. energy sector impacts of technology innovation, fuel price, and electric sector CO 2 policy: Results from the EMF 32 model intercomparison study

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Hodson, Elke L.; Brown, Maxwell; Cohen, Stuart

    We study the impact of achieving technology innovation goals, representing significant technology cost reductions and performance improvements, in both the electric power and end-use sectors by comparing outputs from four energy-economic models through the year 2050. We harmonize model input assumptions and then compare results in scenarios that vary natural gas prices, technology cost and performance metrics, and the implementation of a representative national electricity sector carbon dioxide (CO 2) policy. Achieving the representative technology innovation goals decreases CO 2 emissions in all models, regardless of natural gas price, due to increased energy efficiency and low-carbon generation becoming more costmore » competitive. For the models that include domestic natural gas markets, achieving the technology innovation goals lowers wholesale electricity prices, but this effect diminishes as projected natural gas prices increase. Higher natural gas prices lead to higher wholesale electricity prices but fewer coal capacity retirements. Some of the models include energy efficiency improvements as part of achieving the high-technology goals. Absent these energy efficiency improvements, low-cost electricity facilitates greater electricity consumption. The effect of implementing a representative electricity sector CO 2 policy differs considerably depending on the cost and performance of generating and end-use technologies. The CO 2 policy influences electric sector evolution in the cases with reference technology assumptions but has little to no influence in the cases that achieve the technology innovation goals. This outcome implies that meeting the representative technology innovation goals achieves a generation mix with similar CO 2 emissions to the representative CO 2 policy but with smaller increases to wholesale electricity prices. Finally, higher natural gas prices, achieving the representative technology innovation goals, and the combination of the two, increases the amount of renewable generation that is cost-effective to build and operate while slowing the growth of natural-gas fired generation, which is the predominant generation type in 2050 under reference conditions.« less

  13. Changes in the salinity tolerance of sweet pepper plants as affected by nitrogen form and high CO2 concentration.

    PubMed

    Piñero, María C; Pérez-Jiménez, Margarita; López-Marín, Josefa; Del Amor, Francisco M

    2016-08-01

    The assimilation and availability of nitrogen in its different forms can significantly affect the response of primary productivity under the current atmospheric alteration and soil degradation. An elevated CO2 concentration (e[CO2]) triggers changes in the efficiency and efficacy of photosynthetic processes, water use and product yield, the plant response to stress being altered with respect to ambient CO2 conditions (a[CO2]). Additionally, NH4(+) has been related to improved plant responses to stress, considering both energy efficiency in N-assimilation and the overcoming of the inhibition of photorespiration at e[CO2]. Therefore, the aim of this work was to determine the response of sweet pepper plants (Capsicum annuum L.) receiving an additional supply of NH4(+) (90/10 NO3(-)/NH4(+)) to salinity stress (60mM NaCl) under a[CO2] (400μmolmol(-1)) or e[CO2] (800μmolmol(-1)). Salt-stressed plants grown at e[CO2] showed DW accumulation similar to that of the non-stressed plants at a[CO2]. The supply of NH4(+) reduced growth at e[CO2] when salinity was imposed. Moreover, NH4(+) differentially affected the stomatal conductance and water use efficiency and the leaf Cl(-), K(+), and Na(+) concentrations, but the extent of the effects was influenced by the [CO2]. An antioxidant-related response was prompted by salinity, the total phenolics and proline concentrations being reduced by NH4(+) at e[CO2]. Our results show that the effect of NH4(+) on plant salinity tolerance should be globally re-evaluated as e[CO2] can significantly alter the response, when compared with previous studies at a[CO2]. Copyright © 2016 Elsevier GmbH. All rights reserved.

  14. CO2 Plasma-Treated TiO2 Film as an Effective Electron Transport Layer for High-Performance Planar Perovskite Solar Cells.

    PubMed

    Wang, Kang; Zhao, Wenjing; Liu, Jia; Niu, Jinzhi; Liu, Yucheng; Ren, Xiaodong; Feng, Jiangshan; Liu, Zhike; Sun, Jie; Wang, Dapeng; Liu, Shengzhong Frank

    2017-10-04

    Perovskite solar cells (PSCs) have received great attention because of their excellent photovoltaic properties especially for the comparable efficiency to silicon solar cells. The electron transport layer (ETL) is regarded as a crucial medium in transporting electrons and blocking holes for PSCs. In this study, CO 2 plasma generated by plasma-enhanced chemical vapor deposition (PECVD) was introduced to modify the TiO 2 ETL. The results indicated that the CO 2 plasma-treated compact TiO 2 layer exhibited better surface hydrophilicity, higher conductivity, and lower bulk defect state density in comparison with the pristine TiO 2 film. The quality of the stoichiometric TiO 2 structure was improved, and the concentration of oxygen-deficiency-induced defect sites was reduced significantly after CO 2 plasma treatment for 90 s. The PSCs with the TiO 2 film treated by CO 2 plasma for 90 s exhibited simultaneously improved short-circuit current (J SC ) and fill factor. As a result, the PSC-based TiO 2 ETL with CO 2 plasma treatment affords a power conversion efficiency of 15.39%, outperforming that based on pristine TiO 2 (13.54%). These results indicate that the plasma treatment by the PECVD method is an effective approach to modify the ETL for high-performance planar PSCs.

  15. Effects of recent energy system changes on CO2 projections for the United States

    EPA Science Inventory

    Recent projections of United States carbon dioxide (CO2) emissions are considerably lower than those made just a decade ago. A myriad of factors have contributed to lower forecasts, including reductions in end-use energy service demands, improvements in energy efficiency, techno...

  16. Sinusoidal potential cycling operation of a direct ethanol fuel cell to improving carbon dioxide yields

    NASA Astrophysics Data System (ADS)

    Majidi, Pasha; Pickup, Peter G.

    2014-12-01

    A direct ethanol fuel cell has been operated under sinusoidal (AC) potential cycling conditions in order to increase the yield of carbon dioxide and thereby increase cell efficiency relative to operation at a fixed potential. At 80 °C, faradaic yields of CO2 as high as 25% have been achieved with a PtRu anode catalyst, while the maximum CO2 production at constant potential was 13%. The increased yields under cycling conditions have been attributed to periodic oxidative stripping of adsorbed CO. These results will be important in the optimization of operating conditions for direct ethanol fuel cells, where the benefits of potential cycling are projected to increase as catalysts that produce CO2 more efficiently are implemented.

  17. Revealing the Origin of Activity in Nitrogen-Doped Nanocarbons towards Electrocatalytic Reduction of Carbon Dioxide.

    PubMed

    Xu, Junyuan; Kan, Yuhe; Huang, Rui; Zhang, Bingsen; Wang, Bolun; Wu, Kuang-Hsu; Lin, Yangming; Sun, Xiaoyan; Li, Qingfeng; Centi, Gabriele; Su, Dangsheng

    2016-05-23

    Carbon nanotubes (CNTs) are functionalized with nitrogen atoms for reduction of carbon dioxide (CO2 ). The investigation explores the origin of the catalyst's activity and the role of nitrogen chemical states therein. The catalysts show excellent performances, with about 90 % current efficiency for CO formation and stability over 60 hours. The Tafel analyses and density functional theory calculations suggest that the reduction of CO2 proceeds through an initial rate-determining transfer of one electron to CO2 , which leads to the formation of carbon dioxide radical anion (CO2 (.-) ). The initial reduction barrier is too high on pristine CNTs, resulting in a very high overpotentials at which the hydrogen evolution reaction dominates over CO2 reduction. The doped nitrogen atoms stabilize the radical anion, thereby lowering the initial reduction barrier and improving the intrinsic activity. The most efficient nitrogen chemical state for this reaction is quaternary nitrogen, followed by pyridinic and pyrrolic nitrogen. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  18. Climatic sensitivity, water-use efficiency, and growth decline in boreal jack pine (Pinus banksiana) forests in Northern Ontario

    NASA Astrophysics Data System (ADS)

    Dietrich, Rachel; Bell, F. Wayne; Silva, Lucas C. R.; Cecile, Alice; Horwath, William R.; Anand, Madhur

    2016-10-01

    Rises in atmospheric carbon dioxide (atmCO2) levels are known to stimulate photosynthesis and increase intrinsic water-use efficiency (iWUE) in trees. Stand-level increases in iWUE depend on the physiological response of dominant species to increases in atmCO2, while tree-level response to increasing atmCO2 depends on the balance between the direct effects of atmCO2 on photosynthetic rate and the indirect effects of atmCO2 on drought conditions. The aim of this study was to characterize the response of boreal jack pine (Pinus banksiana) stands in Northern Ontario to changes in atmCO2 and associated climatic change over the past 100 years. The impact of changes in growing season length, temperature, and precipitation, as well as atmCO2 on tree growth, was determined using stable carbon isotopes and dendrochronological analysis. Jack pine stands in this study were shown to be in progressive decline. As expected, iWUE was found to increase in association with rising atmCO2. However, increases in iWUE were not directly coupled with atmCO2, suggesting that the degree of iWUE improvement is limited by alternative factors. Water-use efficiency was negatively associated with tree growth, suggesting that warming- and drought-induced stomatal closure has likely led to deviations from expected atmCO2-enhanced growth. This finding corroborates that boreal forest stands are likely to face continued stress under future climatic warming.

  19. Substantial air quality and climate co-benefits achievable now with sectoral mitigation strategies in China.

    PubMed

    Peng, Wei; Yang, Junnan; Wagner, Fabian; Mauzerall, Denise L

    2017-11-15

    China is the world's top carbon emitter and suffers from severe air pollution. We examine near-term air quality and CO 2 co-benefits of various current sector-based policies in China. Using a 2015 base case, we evaluate the potential benefits of four sectoral mitigation strategies. All scenarios include a 20% increase in conventional air pollution controls as well as the following sector-specific fuel switching or technology upgrade strategies. Power sector (POW): 80% replacement of small coal power plants with larger more efficient ones; Industry sector (IND): 10% improvement in energy efficiency; Transport sector (TRA): replacement of high emitters with average vehicle fleet emissions; and Residential sector (RES): replacement of 20% of coal-based stoves with stoves using liquefied petroleum gas (LPG). Conducting an integrated assessment using the regional air pollution model WRF-Chem, we find that the IND scenario reduces national air-pollution-related deaths the most of the four scenarios examined (27,000, 24,000, 13,000 and 23,000 deaths reduced annually in IND, POW, TRA and RES, respectively). In addition, the IND scenario reduces CO 2 emissions more than 8times as much as any other scenario (440, 53, 0 and 52Mt CO 2 reduced in IND, POW, TRA and RES, respectively). We also examine the benefits of an industrial efficiency improvement of just 5%. We find the resulting air quality and health benefits are still among the largest of the sectoral scenarios, while the carbon mitigation benefits remain more than 3 times larger than any other scenario. Our analysis hence highlights the importance of even modest industrial energy efficiency improvements and air pollution control technology upgrades for air quality, health and climate benefits in China. Copyright © 2017 Elsevier B.V. All rights reserved.

  20. The effects of ultrasonic agitation on supercritical CO2 copper electroplating.

    PubMed

    Chuang, Ho-Chiao; Yang, Hsi-Min; Wu, Guan-Lin; Sánchez, Jorge; Shyu, Jenq-Huey

    2018-01-01

    Applying ultrasound to the electroplating process can improve mechanical properties and surface roughness of the coating. Supercritical electroplating process can refine grain to improve the surface roughness and hardness. However, so far there is no research combining the above two processes to explore its effect on the coating. This study aims to use ultrasound (42kHz) in supercritical CO 2 (SC-CO 2 ) electroplating process to investigate the effect of ultrasonic powers and supercritical pressures on the properties of copper films. From the results it was clear that higher ultrasonic irradiation resulted in higher current efficiency, grain refinement, higher hardness, better surface roughness and higher internal stress. SEM was also presented to verify the correctness of the measured data. The optimal parameters were set to obtain the deposit at pressure of 2000psi and ultrasonic irradiation of 0.157W/cm 3 . Compared with SC-CO 2 electroplating process, the current efficiency can be increased from 77.57% to 93.4%, the grain size decreases from 24.34nm to 22.45nm, the hardness increases from 92.87Hv to 174.18Hv, and the surface roughness decreases from 0.83μm to 0.28μm. Therefore, this study has successfully integrated advantages of ultrasound and SC-CO 2 electroplating, and proved that applied ultrasound to SC-CO 2 electroplating process can significantly improve the mechanical properties of the coating. Copyright © 2017 Elsevier B.V. All rights reserved.

  1. Boosting the catalytic performance of MoSx cocatalysts over CdS nanoparticles for photocatalytic H2 evolution by Co doping via a facile photochemical route

    NASA Astrophysics Data System (ADS)

    Lei, Yonggang; Hou, Jianhua; Wang, Fang; Ma, Xiaohua; Jin, Zhiliang; Xu, Jing; Min, Shixiong

    2017-10-01

    Low-crystalline or amorphous molybdenum sulfides (MoSx), bearing abundant unsaturated active sites, have been identified as efficient catalysts for electrocatalytic and photocatalytic H2 evolution reactions, however, their intrinsic activity is still low and need to be further improved for large-scale applications. In this paper, we report that low-crystalline MoSx doped with Co (Co-MoSx) as efficient cocatalysts could be loaded on CdS nanoparticles through a facile and controllable photochemical reduction method and showed high performances in catalyzing H2 evolution under visible light irradiation (≥420 nm). The photochemical loading of Co-MoSx was accomplished by using an in-situ formed molecular complex precursor and photogenerated electrons on CdS as reductants under mild conditions. The optimized CdS/Co-MoSx (Co:Mo = 1:4, 2 mol% loading) photocatalyst exhibited a catalytic H2 evolution rate of 535 μmol h-1, which is 1.8 times higher than that of CdS/MoSx, and an apparent quantum efficiency (AQE) of 23.5% was achieved over CdS/Co-MoSx photocatalyst at 420 nm. Co-MoSx catalyst also shows a long-term stability without noticeable activity degradation. Notably, Co-MoSx cocatalyst was found more efficient than that of noble metals in catalyzing photocatalytic H2 evolution on CdS. The formation of CoMoS phase, the enhanced electrocatalytic activity as well as reduced electron transfer resistance due to the doping effects of Co ions, account for the enhanced catalytic activity of this Co-MoSx cocatalyst.

  2. Exchange-coupled Fe3O4/CoFe2O4 nanoparticles for advanced magnetic hyperthermia

    NASA Astrophysics Data System (ADS)

    Glassell, M.; Robles, J.; Das, R.; Phan, M. H.; Srikanth, H.

    Iron oxide nanoparticles especially Fe3O4, γ-Fe2O3 have been extensively studied for magnetic hyperthermia because of their tunable magnetic properties and stable suspension in superparamagnetic regime. However, their relatively low heating capacity hindered practical application. Recently, a large improvement in heating efficiency has been reported in exchange-coupled nanoparticles with exchange coupling between soft and hard magnetic phases. Here, we systematically studied the effect of core and shell size on the heating efficiency of the Fe3O4/CoFe2O4 core/shell nanoparticles. The nanoparticles were synthesized using thermal decomposition of organometallic precursors. Transmission electron microscopy (TEM) showed formation of spherical shaped Fe3O4 and Fe3O-/CoFe2O4 nanoparticles. Magnetic measurements showed high magnetization (≅70 emu/g) and superparamagnetic behavior for the nanoparticles at room temperature. Magnetic hyperthermia results showed a large increase in specific absorption rate (SAR) for 8nm Fe3O4/CoFe2O4 compared to Fe3O4 nanoparticles of the same size. The heating efficiency of the Fe3O4/CoFe2O4 with 1 nm CoFe2O4 (shell) increased from 207 to 220 W/g (for 800 Oe) with increase in core size from 6 to 8 nm. The heating efficiency of the Fe3O4/CoFe2O4 with 2 nm CoFe2O4 (shell) and core size of 8 nm increased from 220 to 460 W/g (for 800 Oe). These exchange-coupled Fe3O4/CoFe2O4 core/shell nanoparticles can be a good candidate for advanced hyperthermia application.

  3. Electrocatalytic Reduction of CO 2 at Au Nanoparticle Electrodes: Effects of Interfacial Chemistry on Reduction Behavior

    DOE PAGES

    Andrews, Evan; Katla, Sai; Kumar, Challa; ...

    2015-09-12

    Nanoscale Au electrocatalysts demonstrate the extraordinary ability to reduce CO 2 at low overpotentials with high selectivity to CO. Here, we investigate the role of surface chemistry on CO 2 reduction behavior using Au 25 and 5 nm Au nanoparticles. Onset potentials for CO 2 reduction at Au 25 nanoparticles in Nafion binders are shifted anodically by 190 mV while the hydrogen evolution reaction is shifted cathodically by 300 mV relative to Au foil. The net effect of this beneficial separation in onset potentials is relatively high Faradayic efficiencies for CO (90% at 0.8 V versus RHE) at high currentmore » densities. Experimental results show Faradayic efficiencies for CO are greatest using electrodes made with Nafion-immobilized Au 25 nanoparticles. Likewise, CO 2 reduction onset potential shifts are greater for smaller nanoparticles and when Nafion binders are used instead of (sulfonate-free) polyvinylidene fluoride. X-ray photoelectron spectroscopy analysis reveals Au nanoparticles may react with the sulfonates of Nafion binders. Here, the results suggest sulfonate interfaces may alter the binding energies of key species or lead to favorable reconstructions, either of which ultimately results in remarkable improvements in Faradayic efficiencies relative to Au foil electrodes.« less

  4. Augmenting the Calvin-Benson-Bassham cycle by a synthetic malyl-CoA-glycerate carbon fixation pathway.

    PubMed

    Yu, Hong; Li, Xiaoqian; Duchoud, Fabienne; Chuang, Derrick S; Liao, James C

    2018-05-22

    The Calvin-Benson-Bassham (CBB) cycle is presumably evolved for optimal synthesis of C3 sugars, but not for the production of C2 metabolite acetyl-CoA. The carbon loss in producing acetyl-CoA from decarboxylation of C3 sugar limits the maximum carbon yield of photosynthesis. Here we design a synthetic malyl-CoA-glycerate (MCG) pathway to augment the CBB cycle for efficient acetyl-CoA synthesis. This pathway converts a C3 metabolite to two acetyl-CoA by fixation of one additional CO 2 equivalent, or assimilates glyoxylate, a photorespiration intermediate, to produce acetyl-CoA without net carbon loss. We first functionally demonstrate the design of the MCG pathway in vitro and in Escherichia coli. We then implement the pathway in a photosynthetic organism Synechococcus elongates PCC7942, and show that it increases the intracellular acetyl-CoA pool and enhances bicarbonate assimilation by roughly 2-fold. This work provides a strategy to improve carbon fixation efficiency in photosynthetic organisms.

  5. Metallic nanocatalysts for electrochemical CO2 reduction in aqueous solutions.

    PubMed

    Wang, Yuanxing; Niu, Cailing; Wang, Dunwei

    2018-05-16

    How to effectively and efficiently reduce carbon dioxide (CO 2 ) to value-added chemicals represent a frontier in catalysis research. Due to the high activation energy needs and the endothermic nature of CO 2 reduction, the reactions are difficult to carry out. When H 2 O is present, hydrogen evolution reactions (HER) often compete favorably with CO 2 reduction reactions. For these reactions, catalysts are of critical importance to CO 2 reduction. In this article, we review the various metal nanocatalysts for electrochemical CO 2 reduction (ECR) reactions. In recognition of the importance of H 2 O to CO 2 reduction, we focus our discussions on systems in aqueous solutions. Nanostructured metal catalysts are chosen for the discussions because they represent the most effective catalysts for ECR. After a brief introduction of the fundamental principles of ECR, we devote the rest of the article on the discussions of various types of nanostructured metallic catalysts, which are categorized by their compositions and working mechanisms. Lastly, strategies for improving reaction efficiency and selectivity are discussed. Copyright © 2018 Elsevier Inc. All rights reserved.

  6. Hierarchical Co(OH)2 nanostructures/glassy carbon electrode derived from Co(BTC) metal-organic frameworks for glucose sensing

    NASA Astrophysics Data System (ADS)

    He, Juan; Lu, Xingping; Yu, Jie; Wang, Li; Song, Yonghai

    2016-07-01

    A novel Co(OH)2/glassy carbon electrode (GCE) has been fabricated via metal-organic framework (MOF)-directed method. In the strategy, the Co(BTC, 1,3,5-benzentricarboxylic acid) MOFs/GCE was firstly prepared by alternately immersing GCE in Co2+ and BTC solution based on a layer-by-layer method. And then, the Co(OH)2 with hierarchical flake nanostructure/GCE was constructed by immersing Co(BTC) MOFs/GCE into 0.1 M NaOH solution at room temperature. Such strategy improves the distribution of hierarchical Co(OH)2 nanostructures on electrode surface greatly, enhances the stability of nanomaterials on the electrode surface, and increases the use efficiency of the Co(OH)2 nanostructures. Scanning electron microscopy, energy dispersive X-ray spectroscopy, X-ray powder diffraction, energy dispersive spectroscopy, Fourier transform infrared spectroscopy, and Raman spectra were used to characterize the Co(BTC) MOFs/GCE and Co(OH)2/GCE. Based on the hierarchical Co(OH)2 nanostructures/GCE, a novel and sensitive nonenzymatic glucose sensor was developed. The good performance of the resulted sensor toward the detection of glucose was ascribed to hierarchical flake nanostructures, good mechanical stability, excellent distribution, and large specific surface area of Co(OH)2 nanostructures. The proposed preparation method is simple, efficient, and cheap .

  7. Silver Nanoparticles with Surface-Bonded Oxygen for Highly Selective CO 2 Reduction

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Jiang, Kun; Kharel, Priti; Peng, Yande

    Here, the surface electronic structures of catalysts need to be carefully engineered in CO 2 reduction reaction (CO 2RR), where the hydrogen evolution side reaction usually takes over under a significant overpotential, and thus dramatically lows the reaction selectivity. Surface oxides can play a critical role in tuning the surface oxidation state of metal catalysts for a proper binding with CO 2RR reaction intermediates, which may significantly improve the catalyst activity and selectivity. Here, we demonstrate the importance of surface-bonded oxygen on silver nanoparticles in altering the reaction pathways and improving the CO 2RR performances. A comparative investigation on air-annealedmore » Ag (Air-Ag) catalyst with or without the post-treatment of H 2 thermal annealing (H 2-Ag) was performed. In Air-Ag, the subsurface chemically bonded O species (O-Ag δ+) was identified by angle resolved X-ray photoelectron spectroscopy and X-ray absorption spectroscopy techniques, and contributed to the improved CO selectivity rather than H 2 in CO 2RR electrolysis. As a result, while the maximal CO Faradaic efficiency of H 2-Ag is at ~ 30 %, the Air-Ag catalyst presented a high CO selectivity of more than 90 % under a current density of ~ 21 mA/cm 2.« less

  8. Silver Nanoparticles with Surface-Bonded Oxygen for Highly Selective CO 2 Reduction

    DOE PAGES

    Jiang, Kun; Kharel, Priti; Peng, Yande; ...

    2017-09-12

    Here, the surface electronic structures of catalysts need to be carefully engineered in CO 2 reduction reaction (CO 2RR), where the hydrogen evolution side reaction usually takes over under a significant overpotential, and thus dramatically lows the reaction selectivity. Surface oxides can play a critical role in tuning the surface oxidation state of metal catalysts for a proper binding with CO 2RR reaction intermediates, which may significantly improve the catalyst activity and selectivity. Here, we demonstrate the importance of surface-bonded oxygen on silver nanoparticles in altering the reaction pathways and improving the CO 2RR performances. A comparative investigation on air-annealedmore » Ag (Air-Ag) catalyst with or without the post-treatment of H 2 thermal annealing (H 2-Ag) was performed. In Air-Ag, the subsurface chemically bonded O species (O-Ag δ+) was identified by angle resolved X-ray photoelectron spectroscopy and X-ray absorption spectroscopy techniques, and contributed to the improved CO selectivity rather than H 2 in CO 2RR electrolysis. As a result, while the maximal CO Faradaic efficiency of H 2-Ag is at ~ 30 %, the Air-Ag catalyst presented a high CO selectivity of more than 90 % under a current density of ~ 21 mA/cm 2.« less

  9. Air pollutant emissions and mitigation potential through the adoption of semi-coke coals and improved heating stoves: Field evaluation of a pilot intervention program in rural China.

    PubMed

    Liu, Yafei; Zhang, You; Li, Chuang; Bai, Yun; Zhang, Daoming; Xue, Chunyu; Liu, Guangqing

    2018-05-15

    Pollutant emissions from incomplete combustion of raw coal in low-efficiency residential heating stoves greatly contribute to winter haze in China. Semi-coke coals and improved heating stoves are expected to lower air pollutant emissions and are vigorously promoted by the Chinese government in many national and local plans. In this study, the thermal performance and air pollutant emissions from semi-coke combustion in improved heating stoves were measured in a pilot rural county and compared to the baseline of burning raw coal to quantify the mitigation potential of air pollutant emissions. A total of five stove-fuel combinations were tested, and 27 samples from 27 different volunteered households were obtained. The heating efficiency of improved stoves increased, but fuel consumption appeared higher with more useful energy output compared to traditional stoves. The emission factors of PM 2.5 , SO 2 , and CO 2 of semi-coke burning in specified improved stoves were lower than the baseline of burning raw coal chunk, but no significant NOx and CO decreases were observed. The total amount of PM 2.5 and SO 2 emissions per household in one heating season was lower, but CO, CO 2 , and NOx increased when semi-coke coal and specified improved stoves were deployed. Most differences were not statistically significant due to the limited samples and large variation, indicating that further evaluation would be needed to make conclusions that could be considered for policy. Copyright © 2018 Elsevier Ltd. All rights reserved.

  10. Hollow structured carbon-supported nickel cobaltite nanoparticles as an efficient bifunctional electrocatalyst for the oxygen reduction and evolution reaction

    DOE PAGES

    Wang, Jie; Han, Lili; Lin, Ruoqian; ...

    2016-01-05

    Here, the exploration of efficient electrocatalysts for both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is essential for fuel cells and metal-air batteries. In this study, we developed 3D hollow-structured NiCo 2O 4/C nanoparticles with interconnected pores as bifunctional electrocatalysts, which are transformed from solid NiCo 2 alloy nanoparticles through the Kirkendall effect. The unique hollow structure of NiCo 2O 4 nanoparticles increases the number of active sites and improves contact with the electrolyte to result in excellent ORR and OER performances. In addition, the hollow-structured NiCo 2O 4/C nanoparticles exhibit superior long-term stability for both themore » ORR and OER compared to commercial Pt/C. The template- and surfactant-free synthetic strategy could be used for the low-cost and large-scale synthesis of hollow-structured materials, which would facilitate the screening of high-efficiency catalysts for energy conversion.« less

  11. Improved brain and muscle mitochondrial respiration with CoQ. An in vivo study by 31P-MR spectroscopy in patients with mitochondrial cytopathies.

    PubMed

    Barbiroli, B; Iotti, S; Lodi, R

    1999-01-01

    We used in vivo phosphorus magnetic resonance spectroscopy (31P-MRS) to study the effect of CoQ10 on the efficiency of brain and skeletal muscle mitochondrial respiration in ten patients with mitochondrial cytopathies. Before CoQ, brain [PCr] was remarkably lower in patients than in controls, while [Pi] and [ADP] were higher. Brain cytosolic free [Mg2+] and delta G of ATP hydrolysis were also abnormal in all patients. MRS also revealed abnormal mitochondrial function in the skeletal muscles of all patients, as shown by a decreased rate of PCr recovery from exercise. After six-months of treatment with CoQ (150 mg/day), all brain MRS-measurable variables as well as the rate of muscle mitochondrial respiration were remarkably improved in all patients. These in vivo findings show that treatment with CoQ in patients with mitochondrial cytopathies improves mitochondrial respiration in both brain and skeletal muscles, and are consistent with Lenaz's view that increased CoQ concentration in the mitochondrial membrane increases the efficiency of oxidative phosphorylation independently of enzyme deficit.

  12. Enhanced charge separation of rutile TiO2 nanorods by trapping holes and transferring electrons for efficient cocatalyst-free photocatalytic conversion of CO2 to fuels.

    PubMed

    Wu, Jing; Lu, Hongwei; Zhang, Xuliang; Raziq, Fazal; Qu, Yang; Jing, Liqiang

    2016-04-11

    Modification with chloride and phosphate anions, and coupling with carbon nanotubes could effectively trap holes and transfer the electrons of rutile nanorods, respectively, so as to greatly promote photogenerated charge separation, leading to an obviously-improved cocatalyst-free photocatalytic conversion of CO2 to CH4 and CO, along with the positive effects of constructed phosphate bridges.

  13. Evaluating the Environmental Performance of the U.S. Next Generation Air Transportation System

    NASA Technical Reports Server (NTRS)

    Graham, Michael; Augustine, Stephen; Ermatinger, Christopher; Difelici, John; Thompson, Terence R.; Marcolini, Michael A.; Creedon, Jeremiah F.

    2009-01-01

    The environmental impacts of several possible U.S. Next Generation Air Transportation scenarios have been quantitatively evaluated for noise, air-quality, fuel-efficiency, and CO2 impacts. Three principal findings have emerged. (1) 2025 traffic levels about 30% higher than 2006 are obtained by increasing traffic according to FAA projections while also limiting traffic at each airport using reasonable ratios of demand to capacity. NextGen operational capabilities alone enable attainment of an additional 10-15% more flights beyond that 2025 baseline level with negligible additional noise, air-quality, and fuel-efficiency impacts. (2) The addition of advanced engine and airframe technologies provides substantial additional reductions in noise and air-quality impacts, and further improves fuel efficiency. 2025 environmental goals based on projected system-wide improvement rates of about 1% per year for noise and fuel-efficiency (an air-quality goal is not yet formulated) are achieved using this new vehicle technology. (3) Overall air-transport "product", as measured by total flown distance or total payload distance, increases by about 50% relative to 2006, but total fuel consumption and CO2 production increase by only about 40% using NextGen operational capabilities. With the addition of advanced engine/airframe technologies, the increase in total fuel consumption and CO2 production can be reduced to about 30%.

  14. Acclimation of two tomato species to high atmospheric CO sub 2 : I. Sugar and starch concentrations

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Yelle, S.; Beeson, R.C. Jr.; Trudel, M.J.

    Lycopersicon esculentum Mill. cv Vedettos and Lycopersicon chmielewskii Rick, LA1028, were exposed to two CO{sub 2} concentrations for 10 weeks. Tomato plants grown at 900 microliters per liter contained more starch and more sugars than the control. However, we found no significant accumulation of starch and sugars in the young leaves of L. esculentum exposed to high CO{sub 2}. Carbon exchange rates were significantly higher in CO{sub 2}-enriched plants for the first few weeks of treatment but thereafter decreased as tomato plants acclimated to high atmospheric CO{sub 2}. This indicates that the long-term decline of photosynthetic efficiency of leaf 5more » cannot be attributed to an accumulation of sugar and/or starch. The average concentration of starch in leaves 5 and 9 was always higher in L. esculentum than in L. chmielewskii (151.7% higher). A higher proportion of photosynthates was directed into starch for L. esculentum than for L. chmielewskii. However, these characteristics did not improve the long-term photosynthetic efficiency of L. chmielewskii grown at high CO{sub 2} when compared with L. esculentum. The chloroplasts of tomato plants exposed to the higher CO{sub 2} concentration exhibited a marked accumulation of starch. The results reported here suggest that starch and/or sugar accumulation under high CO{sub 2} cannot entirely explain the loss of photosynthetic efficiency of high CO{sub 2}-grown plants.« less

  15. Low-coordinated surface atoms of CuPt alloy cocatalysts on TiO2 for enhanced photocatalytic conversion of CO2.

    PubMed

    Lee, Sooho; Jeong, Sunil; Kim, Whi Dong; Lee, Seokwon; Lee, Kangha; Bae, Wan Ki; Moon, Jun Hyuk; Lee, Sangheon; Lee, Doh C

    2016-05-21

    We report the photocatalytic conversion of CO2 to CH4 using CuPt alloy nanoclusters anchored on TiO2. As the size of CuPt alloy nanoclusters decreases, the photocatalytic activity improves significantly. Small CuPt nanoclusters strongly bind CO2 intermediates and have a stronger interaction with the TiO2 support, which also contributes to an increased CH4 generation rate. The alloying and size effects prove to be the key to efficient CO2 reduction, highlighting a strategic platform for the design of photocatalysts for CO2 conversion.

  16. Liquid Hydrocarbon Production from CO2 : Recent Development in Metal-Based Electrocatalysis.

    PubMed

    Daiyan, Rahman; Lu, Xunyu; Ng, Yun Hau; Amal, Rose

    2017-11-23

    Rising levels of CO 2 accumulation in the atmosphere have attracted considerable interest in technologies capable of CO 2 capture, storage and conversion. The electrochemical reduction of CO 2 into high-value liquid organic products could be of vital importance to mitigate this issue. The conversion of CO 2 into liquid fuels by using photovoltaic cells, which can readily be integrated in the current infrastructure, will help realize the creation of a sustainable cycle of carbon-based fuel that will promote zero net CO 2 emissions. Despite promising findings, significant challenges still persist that must be circumvented to make the technology profitable for large-scale utilization. With such possibilities, this Minireview presents the current high-performing catalysts for the electrochemical reduction of CO 2 to liquid hydrocarbons, address the limitations and unify the current understanding of the different reaction mechanisms. The Minireview also explores current research directions to improve process efficiencies and production rate and discusses the scope of using photo-assisted electrochemical reduction systems to find stable, highly efficient catalysts that can harvest solar energy directly to convert CO 2 into liquid hydrocarbons. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  17. Enhancing visible light photocatalytic and photocharge separation of (BiO){sub 2}CO{sub 3} plate via dramatic I{sup −} ions doping effect

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Liang, Lei; Cao, Jing; Anhui Collaborative Innovation Center of Advanced Functional Composite, Huaibei, 235000, Anhui

    Highlights: • Novel I-(BiO){sub 2}CO{sub 3} was prepared by a facile chemical precipitation method. • I{sup −} ions impurity level located on the top of valence band of (BiO){sub 2}CO{sub 3}. • I{sup −} ions doping largely improved photocatalytic activity of I-(BiO){sub 2}CO{sub 3}. • I-(BiO){sub 2}CO{sub 3} displayed excellent photocharge separation efficiency. - Abstract: Novel I{sup −} ions doped (BiO){sub 2}CO{sub 3} (I-(BiO){sub 2}CO{sub 3}) photocatalysts were successfully synthesized via a facile chemical precipitation method. Under visible light (λ > 400 nm), I-(BiO){sub 2}CO{sub 3} displayed much higher activity for rhodamine B and dichlorophenol degradation than the undoped (BiO){submore » 2}CO{sub 3}. The pseudo-first-order rate constant k{sub app} of RhB degradation over 15.0% I-(BiO){sub 2}CO{sub 3} was 0.54 h{sup −1}, which is 11.3 times higher than that of (BiO){sub 2}CO{sub 3}. The doped I{sup −} ions formed an impurity level on the top of valence band of (BiO){sub 2}CO{sub 3} and induced much more visible light to be absorbed. The enhanced photocurrent and surface photovoltage properties were detected, which strongly ensures the efficient separation of electrons and holes in I-(BiO){sub 2}CO{sub 3} system under visible light. It provides a facile way to improve the photocatalytic activity of the wide-band-gap (BiO){sub 2}CO{sub 3} via intense doping effect of I{sup −} ions.« less

  18. Shape-Dependent Electrocatalytic Reduction of CO2 to CO on Triangular Silver Nanoplates.

    PubMed

    Liu, Subiao; Tao, Hongbiao; Zeng, Li; Liu, Qi; Xu, Zhenghe; Liu, Qingxia; Luo, Jing-Li

    2017-02-15

    Electrochemical reduction of CO 2 (CO 2 RR) provides great potential for intermittent renewable energy storage. This study demonstrates a predominant shape-dependent electrocatalytic reduction of CO 2 to CO on triangular silver nanoplates (Tri-Ag-NPs) in 0.1 M KHCO 3 . Compared with similarly sized Ag nanoparticles (SS-Ag-NPs) and bulk Ag, Tri-Ag-NPs exhibited an enhanced current density and significantly improved Faradaic efficiency (96.8%) and energy efficiency (61.7%), together with a considerable durability (7 days). Additionally, CO starts to be observed at an ultralow overpotential of 96 mV, further confirming the superiority of Tri-Ag-NPs as a catalyst for CO 2 RR toward CO formation. Density functional theory calculations reveal that the significantly enhanced electrocatalytic activity and selectivity at lowered overpotential originate from the shape-controlled structure. This not only provides the optimum edge-to-corner ratio but also dominates at the facet of Ag(100) where it requires lower energy to initiate the rate-determining step. This study demonstrates a promising approach to tune electrocatalytic activity and selectivity of metal catalysts for CO 2 RR by creating optimal facet and edge site through shape-control synthesis.

  19. Preparation of transition metal composite graphite felt cathode for efficient heterogeneous electro-Fenton process.

    PubMed

    Liang, Liang; Yu, Fangke; An, Yiran; Liu, Mengmeng; Zhou, Minghua

    2017-01-01

    A composite graphite felt (GF) modified with transition metal was fabricated and used as cathode in heterogeneous electro-Fenton (EF) for methyl orange (MO) degradation. Characterized by scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS), the morphology and surface physicochemical properties of the cathodes after modification were observed considerably changed. After loading metals, the current response became higher, the accumulation of H 2 O 2 and the degradation efficiency of MO were improved. Under the same conditions, GF-Co had the highest catalytic activity for electro-reduction of O 2 to H 2 O 2 and MO degradation. At pH 3, 99 % of MO degradation efficiency was obtained using GF-Co after 120 min treatment and even at initial pH 9, 82 % of that was obtained. TOC removal efficiency reached 93.8 % using GF-Co at pH 3 after 120 min treatment while that was 12.3 % using GF. After ten-time runs, the mineralization ratio of the GF-Co was still 89.5 %, suggesting that GF-Co was very promising for wastewater treatment. The addition of isopropanol proved that · OH played an important role in degradation of MO.

  20. Improved characteristics of conventional and inverted polymer photodetectors using phosphonic acid-based self-assembled monolayer treatment for interfacial engineering of Ga-doped ZnO electrodes

    NASA Astrophysics Data System (ADS)

    Kajii, Hirotake; Mohri, Yoshinori; Okui, Hiyuto; Kondow, Masahiko; Ohmori, Yutaka

    2018-03-01

    The characteristics of conventional and inverted polymer photodetectors based on a blend of a donor, poly(3-hexylthiophene) (P3HT), and an acceptor, fullerene derivative [6,6]phenyl-C61-butyric acid methyl ester (PCBM) using Ga-doped ZnO (GZO) electrodes modified by phosphonic acid-based self-assembled monolayer (SAM) treatment in a short time are investigated. Fluoroalkyl SAM, 1H,1H,2H,2H-perfluorooctane phosphonic acid (FOPA) treatment leads to efficient hole extraction from the active layer. The characteristics of the conventional device with GZO modified by FOPA treatment are almost the same as those with indium tin oxide modified by FOPA. Cs2CO3 and aminoalkyl SAM, 11-aminoundecylphosphonic acid (11-AUPA) treatments suppress the hole injection from GZO to the organic layer. For the inverted devices with GZO cathodes using Cs2CO3 and 11-AUPA, the dark current decreases, which results in the improved photodetector detectivity. An inverted device with both Cs2CO3 and 11-AUPA exhibits incident-photon-to-current conversion efficiency (IPCE) of approximately 65% (80%) at 0 V (-6 V) under light irradiation (λ = 500 nm), high on/off ratio, and improved durability. Improved open-circuit voltage and IPCE at low voltages are achieved by these treatments, which are related with the improved internal built-in field, the reduction of recombination probability in the vicinity of GZO, and the modified charge collection efficiency.

  1. Eco-friendly synthesis of core-shell structured (TiO2/Li2CO3) nanomaterials for low cost dye-sensitized solar cells.

    PubMed

    Karuppuchamy, S; Brundha, C

    2016-12-01

    Core-shell structured TiO 2 /Li 2 CO 3 electrode was successfully synthesized by eco-friendly solution growth technique. TiO 2 /Li 2 CO 3 electrodes were characterized using X-ray Diffractometer (XRD), Scanning electron microscopy (SEM) and photocurrent-voltage measurements. The synthesized core-shell electrode material was sensitized with tetrabutylammonium cis-di(thiocyanato)-N,N'-bis(4-carboxylato-4'-carboxylic acid-2,2'-bipyridine)ruthenate(II) (N-719). The performance of dye-sensitized solar cells (DSCs) based on N719 dye modified TiO 2 /Li 2 CO 3 electrodes was investigated. The effect of various shell thickness on the photovoltaic performance of the core-shell structured electrode is also investigated. We found that Li 2 CO 3 shells of all thicknesses perform as inert barriers which improve open-circuit voltage (V oc ) of the DSCs. The energy conversion efficiency was greatly dependent on the thickness of Li 2 CO 3 on TiO 2 film, and the highest efficiency of 3.7% was achieved at the optimum Li 2 CO 3 shell layer. Copyright © 2015 Elsevier Inc. All rights reserved.

  2. Final Report: Utilizing Alternative Fuel Ignition Properties to Improve SI and CI Engine Efficiency

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Wooldridge, Margaret; Boehman, Andre; Lavoie, George

    Experimental and modeling studies were completed to explore leveraging physical and chemical fuel properties for improved thermal efficiency of internal combustion engines. Fundamental studies of the ignition chemistry of ethanol and iso-octane blends and constant volume spray chamber studies of gasoline and diesel sprays supported the core research effort which used several reciprocating engine platforms. Single cylinder spark ignition (SI) engine studies were carried out to characterize the impact of ethanol/gasoline, syngas (H 2 and CO)/gasoline and other oxygenate/gasoline blends on engine performance. The results of the single-cylinder engine experiments and other data from the literature were used to trainmore » a GT Power model and to develop a knock criteria based on reaction chemistry. The models were used to interpret the experimental results and project future performance. Studies were also carried out using a state of the art, direct injection (DI) turbocharged multi- cylinder engine with piezo-actuated fuel injectors to demonstrate the promising spray and spark timing strategies from single-cylinder engine studies on the multi-cylinder engine. Key outcomes and conclusions of the studies were: 1. Efficiency benefits of ethanol and gasoline fuel blends were consistent and substantial (e.g. 5-8% absolute improvement in gross indicated thermal efficiency (GITE)). 2. The best ethanol/gasoline blend (based on maximum thermal efficiency) was determined by the engine hardware and limits based on component protection (e.g. peak in-cylinder pressure or maximum turbocharger inlet temperature) – and not by knock limits. Blends with <50% ethanol delivered significant thermal efficiency gains with conventional SI hardware while maintain good safety integrity to the engine hardware. 3. Other compositions of fuel blends including syngas (H 2 and CO) and other dilution strategies provided significant efficiency gains as well (e.g. 5% absolute improvement in ITE). 4. When the combination of engine and fuel system is not knock limited, multiple fuel injection events maintain thermal efficiency while improving engine-out emissions (e.g. CO, UHC, and particulate number).« less

  3. Co-sensitization of natural dyes for improved efficiency in dye-sensitized solar cell application

    NASA Astrophysics Data System (ADS)

    Kumar, K. Ashok; Subalakshmi, K.; Senthilselvan, J.

    2016-05-01

    In this paper, a new approach of co-sensitized DSSC based on natural dyes is investigated to explore the possible way to improve the power conversion efficiency. To realize this purpose 10 DSSC devices were fabricated using mono-sensitization and co-sensitization of ethanolic extracts of natural dye sensitizers obtained from Cactus fruit, Jambolana fruit, Curcumin and Bermuda grass. The optical absorption spectrum of the mono and hybrid dye extracts were studied by UV-Visible absorption spectrum. It shows the characteristic absorption peaks in visible region corresponds to the presence of natural pigments of anthocyanin, betacyanin and chlorophylls. Absorption spectrum of hybrid dyes reveals a wide absorption band in visible region with improved extinction co-efficient and it is favorable for increased light harvesting nature. The power conversion efficiency of DSSC devices were calculated using J-V curve and the maximum efficiency achieved in the present work is noted to be ~0.61% for Cactus-Bermuda co-sensitized DSSC.

  4. N,N'-Bis((6-methoxylpyridin-2-yl)methylene)-p-phenylenediimine based d(10) transition metal complexes and their utilization in co-sensitized solar cells.

    PubMed

    Wei, Liguo; Yang, Yulin; Fan, Ruiqing; Na, Yong; Wang, Ping; Dong, Yuwei; Yang, Bin; Cao, Wenwu

    2014-08-07

    N,N'-Bis((6-methoxylpyridin-2-yl)methylene)-p-phenylenediimine based four-coordinated d(10) transition metal complexes (named ML, M = Zn, Cd, Hg) were synthesized and employed as co-sensitizers and co-adsorbents in combination with a ruthenium complex N719 in dye sensitized solar cells. After co-sensitization, not only the incident-photon-to-current conversion efficiency is enhanced but also the dark current is reduced. A short circuit current density of 14.46 mA cm(-2), an open circuit voltage of 0.74 V and a fill factor of 0.62 corresponding to an overall conversion efficiency of 6.65% under AM 1.5 G solar irradiation were achieved when ZnL was used as a co-sensitizer, which are much higher than that for DSSCs only sensitized by N719 (5.22%) under the same conditions. The improvement in efficiency is attributed to the fact that N,N'-bis((6-methoxylpyridin-2-yl)methylene)-p-phenylenediimine coordinated complexes overcome the deficiency of N719 absorption in the low wavelength region of the visible spectrum, prevent its aggregation, offset competitive visible light absorption of I3(-) and reduce charge recombination due to formation of an effective cover layer of the dye molecules on the TiO2 surface. As a result, the synthesized complexes are promising candidates as co-adsorbents and co-sensitizers for highly efficient DSSCs.

  5. Arbuscular mycorrhiza improve growth, nitrogen uptake, and nitrogen use efficiency in wheat grown under elevated CO2.

    PubMed

    Zhu, Xiancan; Song, Fengbin; Liu, Shengqun; Liu, Fulai

    2016-02-01

    Effects of the arbuscular mycorrhizal (AM) fungus Rhizophagus irregularis on plant growth, carbon (C) and nitrogen (N) accumulation, and partitioning was investigated in Triticum aestivum L. plants grown under elevated CO2 in a pot experiment. Wheat plants inoculated or not inoculated with the AM fungus were grown in two glasshouse cells with different CO2 concentrations (400 and 700 ppm) for 10 weeks. A (15)N isotope labeling technique was used to trace plant N uptake. Results showed that elevated CO2 increased AM fungal colonization. Under CO2 elevation, AM plants had higher C concentration and higher plant biomass than the non-AM plants. CO2 elevation did not affect C and N partitioning in plant organs, while AM symbiosis increased C and N allocation into the roots. In addition, plant C and N accumulation, (15)N recovery rate, and N use efficiency (NUE) were significantly higher in AM plants than in non-AM controls under CO2 enrichment. It is concluded that AM symbiosis favors C and N partitioning in roots, increases C accumulation and N uptake, and leads to greater NUE in wheat plants grown at elevated CO2.

  6. The effect of atmospheric carbon dioxide concentrations on the performance of the mangrove Avicennia germinans over a range of salinities.

    PubMed

    Reef, Ruth; Winter, Klaus; Morales, Jorge; Adame, Maria Fernanda; Reef, Dana L; Lovelock, Catherine E

    2015-07-01

    By increasing water use efficiency and carbon assimilation, increasing atmospheric CO2 concentrations could potentially improve plant productivity and growth at high salinities. To assess the effect of elevated CO2 on the salinity response of a woody halophyte, we grew seedlings of the mangrove Avicennia germinans under a combination of five salinity treatments [from 5 to 65 parts per thousand (ppt)] and three CO2 concentrations (280, 400 and 800 ppm). We measured survivorship, growth rate, photosynthetic gas exchange, root architecture and foliar nutrient and ion concentrations. The salinity optima for growth shifted higher with increasing concentrations of CO2 , from 0 ppt at 280 ppm to 35 ppt at 800 ppm. At optimal salinity conditions, carbon assimilation rates were significantly higher under elevated CO2 concentrations. However, at salinities above the salinity optima, salinity had an expected negative effect on mangrove growth and carbon assimilation, which was not alleviated by elevated CO2 , despite a significant improvement in photosynthetic water use efficiency. This is likely due to non-stomatal limitations to growth at high salinities, as indicated by our measurements of foliar ion concentrations that show a displacement of K(+) by Na(+) at elevated salinities that is not affected by CO2 . The observed shift in the optimal salinity for growth with increasing CO2 concentrations changes the fundamental niche of this species and could have significant effects on future mangrove distribution patterns and interspecific interactions. © 2014 Scandinavian Plant Physiology Society.

  7. C4 grasses prosper as carbon dioxide eliminates desiccation in warmed semi-arid grasslands

    USDA-ARS?s Scientific Manuscript database

    Global warming is predicted to induce desiccation in many world regions through increases in evaporative demand. Rising CO2 may counter that trend by improving plant water use efficiency (WUE). However, it is not clear how important this CO2-enhanced WUE might be in off-setting warming-induced desi...

  8. A Comparison of Supercritical Carbon Dioxide Power Cycle Configurations with an Emphasis on CSP Applications (Presentation)

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Neises, T.; Turchi, C.

    2013-09-01

    Recent research suggests that an emerging power cycle technology using supercritical carbon dioxide (s-CO2) operated in a closed-loop Brayton cycle offers the potential of equivalent or higher cycle efficiency versus supercritical or superheated steam cycles at temperatures relevant for CSP applications. Preliminary design-point modeling suggests that s-CO2 cycle configurations can be devised that have similar overall efficiency but different temperature and/or pressure characteristics. This paper employs a more detailed heat exchanger model than previous work to compare the recompression and partial cooling cycles, two cycles with high design-point efficiencies, and illustrates the potential advantages of the latter. Integration of themore » cycles into CSP systems is studied, with a focus on sensible heat thermal storage and direct s-CO2 receivers. Results show the partial cooling cycle may offer a larger temperature difference across the primary heat exchanger, thereby potentially reducing heat exchanger cost and improving CSP receiver efficiency.« less

  9. Long-term CO2 rise has increased photosynthetic efficiency and water use efficiency but did not stimulate diameter growth of tropical trees

    NASA Astrophysics Data System (ADS)

    Groenendijk, P.; Zuidema, P.; Sleen, P. V. D.; Vlam, M.; Ehlers, I.; Schleucher, J.

    2014-12-01

    Tropical forests are a crucial component of the global carbon cycle, and their responses to atmospheric changes may shift carbon cycling and climate systems. Dynamic Global Vegetation Models (DGVMs) are the major tools to simulate tropical forest responses to climate change. One of the main determinants of these simulated responses is the effect of CO2 on tropical tree physiology and growth, the 'CO2 fertilization effect'. The paucity of CO2 enrichment experiments in the tropics importantly limits insights into the CO2 fertilization effect as well as the validation of DGVMs. However, use can be made of the 40% rise in atmospheric CO2 concentration since the onset of the Industrial Revolution. The effects of the historical CO2 rise on tree physiology and growth can be obtained from stable isotopes, isotopomers and tree diameter increments obtained in tree-ring studies. We studied the physiological and growth responses of 12 tree species in Bolivia, Cameroon and Thailand to 150 years of CO2 enrichment. Analyses of 13C of wood cellulose revealed strong, long-term increases in leaf intercellular CO2 concentrations for all study species and a marked improvement of intrinsic water use efficiency (iWUE). For a subset of one species per site, we studied the Deuterium isotopomers (isomers with isotopic atoms) of glucose in wood to obtain a direct estimate of the photorespiration-to-photosynthesis ratio. We found that this ratio consistently and strongly decreased over the past century, thus increasing the effeciency and rate of photosynthesis. In spite of these strong physiological responses to increased CO2levels, we did not find evidence for increased tree diameter growth for any of the sites, or for sites combined. Possible reasons for the lack of a growth stimulation include increased (leaf) temperature, insufficient availability of nutrients or a shift in biomass investment in trees. Our results suggest that the strong CO2 fertilization of tropical tree growth often assumed in DGVMs does not hold and that these models may overestimate future biomass production in tropical forests. Empirical information on responses of tropical trees to historical CO2rise as presented here can be used to validate and possibly adapt (components of) DGVMs and improve the projections of tropical forest structure under climate change.

  10. Toward solar biodiesel production from CO2 using engineered cyanobacteria.

    PubMed

    Woo, Han Min; Lee, Hyun Jeong

    2017-05-01

    Metabolic engineering of cyanobacteria has received attention as a sustainable strategy to convert carbon dioxide to various biochemicals including fatty acid-derived biodiesel. Recently, Synechococcus elongatus PCC 7942, a model cyanobacterium, has been engineered to convert CO2 to fatty acid ethyl esters (FAEEs) as biodiesel. Modular pathway has been constructed for FAEE production. Several metabolic engineering strategies were discussed to improve the production levels of FAEEs, including host engineering by improving CO2 fixation rate and photosynthetic efficiency. In addition, protein engineering of key enzyme in S. elongatus PCC 7942 was implemented to address issues on FAEE secretions toward sustainable FAEE production from CO2. Finally, advanced metabolic engineering will promote developing biosolar cell factories to convert CO2 to feasible amount of FAEEs toward solar biodiesel. © FEMS 2017. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.

  11. [Effects of enhanced CO2 fertilization on phytoremediation of DEHP-polluted soil].

    PubMed

    Diao, Xiao-Jun; Wang, Shu-Guang; Mu, Nan

    2013-03-01

    Low efficiency of remediation is one of the key issues to be solved in phytoremediation technology. Based on the necessity of reducing CO2 emission in China and the significance of CO2 in plant photosynthesis, this paper studied the effects of enhanced CO2 fertilization on the phytoremediation of polluted soil, selecting the C3 plant mung bean (Vigna radiate) and the C4 plant maize (Zea mays) as test plants for phytoremediation and the DEHP as the target pollutant. DEHP pollution had negative effects on the growth and rhizosphere micro-environment of the two plants. After enhanced CO2 fertilization, the aboveground dry mass of the two plants and the alkaline phosphatase activity in the rhizosphere soils of the two plants increased, the COD activity in the leaves of the two plants decreased, the microbial community in the rhizosphere soils shifted, and the numbers of the microbes with DEHP-tolerance in the rhizosphere soils increased. These changes indicated that enhanced CO2 fertilization could promote the plant growth and the plant tolerance to DEHP stress, and improve the rhizosphere micro-environment. Enhanced CO2 fertilization also increased the DEHP uptake by the two plants, especially their underground parts. All these effects induced the residual DEHP concentration in the rhizospheres of the two plants, especially that of mung bean, decreased obviously, and the phytoremediation efficiency increased. Overall, enhanced CO2 fertilization produced greater effects on C3 plant than on C4 plant. It was suggested that enhanced CO2 fertilization could be a useful measure to enhance the efficiency of phytoremediation.

  12. Prospects for improving CO2 fixation in C3-crops through understanding C4-Rubisco biogenesis and catalytic diversity.

    PubMed

    Sharwood, Robert E; Ghannoum, Oula; Whitney, Spencer M

    2016-06-01

    By operating a CO2 concentrating mechanism, C4-photosynthesis offers highly successful solutions to remedy the inefficiency of the CO2-fixing enzyme Rubisco. C4-plant Rubisco has characteristically evolved faster carboxylation rates with low CO2 affinity. Owing to high CO2 concentrations in bundle sheath chloroplasts, faster Rubisco enhances resource use efficiency in C4 plants by reducing the energy and carbon costs associated with photorespiration and lowering the nitrogen investment in Rubisco. Here, we show that C4-Rubisco from some NADP-ME species, such as maize, are also of potential benefit to C3-photosynthesis under current and future atmospheric CO2 pressures. Realizing this bioengineering endeavour necessitates improved understanding of the biogenesis requirements and catalytic variability of C4-Rubisco, as well as the development of transformation capabilities to engineer Rubisco in a wider variety of food and fibre crops. Copyright © 2016 Elsevier Ltd. All rights reserved.

  13. Case study on incentive mechanism of energy efficiency retrofit in coal-fueled power plant in China.

    PubMed

    Yuan, Donghai; Guo, Xujing; Cao, Yuan; He, Liansheng; Wang, Jinggang; Xi, Beidou; Li, Junqi; Ma, Wenlin; Zhang, Mingshun

    2012-01-01

    An ordinary steam turbine retrofit project is selected as a case study; through the retrofit, the project activities will generate emission reductions within the power grid for about 92,463 tCO(2)e per annum. The internal rate of return (IRR) of the project is only -0.41% without the revenue of carbon credits, for example, CERs, which is much lower than the benchmark value of 8%. Only when the unit price of carbon credit reaches 125 CNY/tCO(2), the IRR could reach the benchmark and an effective carbon tax needs to increase the price of carbon to 243 CNY/tce in order to make the project financially feasible. Design of incentive mechanism will help these low efficiency enterprises improve efficiency and reduce CO(2) emissions, which can provide the power plants sufficient incentive to implement energy efficiency retrofit project in existing coal-fuel power generation-units, and we hope it will make a good demonstration for the other low efficiency coal-fueled power generation units in China.

  14. Case Study on Incentive Mechanism of Energy Efficiency Retrofit in Coal-Fueled Power Plant in China

    PubMed Central

    Yuan, Donghai; Guo, Xujing; Cao, Yuan; He, Liansheng; Wang, Jinggang; Xi, Beidou; Li, Junqi; Ma, Wenlin; Zhang, Mingshun

    2012-01-01

    An ordinary steam turbine retrofit project is selected as a case study; through the retrofit, the project activities will generate emission reductions within the power grid for about 92,463 tCO2e per annum. The internal rate of return (IRR) of the project is only −0.41% without the revenue of carbon credits, for example, CERs, which is much lower than the benchmark value of 8%. Only when the unit price of carbon credit reaches 125 CNY/tCO2, the IRR could reach the benchmark and an effective carbon tax needs to increase the price of carbon to 243 CNY/tce in order to make the project financially feasible. Design of incentive mechanism will help these low efficiency enterprises improve efficiency and reduce CO2 emissions, which can provide the power plants sufficient incentive to implement energy efficiency retrofit project in existing coal-fuel power generation-units, and we hope it will make a good demonstration for the other low efficiency coal-fueled power generation units in China. PMID:23365532

  15. Process controls for improving bioleaching performance of both Li and Co from spent lithium ion batteries at high pulp density and its thermodynamics and kinetics exploration.

    PubMed

    Niu, Zhirui; Zou, Yikan; Xin, Baoping; Chen, Shi; Liu, Changhao; Li, Yuping

    2014-08-01

    Release of Co and Li from spent lithium ion batteries (LIBs) by bioleaching has attracted growing attentions. However, the pulp density was only 1% or lower, meaning that a huge quantity of media was required for bioleaching. In this work, bioleaching behavior of the spent LIBs at pulp densities ranging from 1% to 4% was investigated and process controls to improve bioleaching performance at pulp density of 2% were explored. The results showed that the pulp density exerted a considerable influence on leaching performance of Co and Li. The bioleaching efficiency decreased respectively from 52% to 10% for Co and from 80% to 37% for Li when pulp density rose from 1% to 4%. However, the maximum extraction efficiency of 89% for Li and 72% for Co was obtained at pulp density of 2% by process controls. Bioleaching of the spent LIBs has much greater potential to occur than traditional chemical leaching based on thermodynamics analysis. The product layer diffusion model described best bioleaching behavior of Co and Li. Copyright © 2014 Elsevier Ltd. All rights reserved.

  16. Plant growth responses to elevated atmospheric CO2 are increased by phosphorus sufficiency but not by arbuscular mycorrhizas.

    PubMed

    Jakobsen, Iver; Smith, Sally E; Smith, F Andrew; Watts-Williams, Stephanie J; Clausen, Signe S; Grønlund, Mette

    2016-11-01

    Capturing the full growth potential in crops under future elevated CO 2 (eCO 2 ) concentrations would be facilitated by improved understanding of eCO 2 effects on uptake and use of mineral nutrients. This study investigates interactions of eCO 2 , soil phosphorus (P), and arbuscular mycorrhizal (AM) symbiosis in Medicago truncatula and Brachypodium distachyon grown under the same conditions. The focus was on eCO 2 effects on vegetative growth, efficiency in acquisition and use of P, and expression of phosphate transporter (PT) genes. Growth responses to eCO 2 were positive at P sufficiency, but under low-P conditions they ranged from non-significant in M. truncatula to highly significant in B. distachyon Growth of M. truncatula was increased by AM at low P conditions at both CO 2 levels and eCO 2 ×AM interactions were sparse. Elevated CO 2 had small effects on P acquisition, but enhanced conversion of tissue P into biomass. Expression of PT genes was influenced by eCO 2 , but effects were inconsistent across genes and species. The ability of eCO 2 to partly mitigate P limitation-induced growth reductions in B. distachyon was associated with enhanced P use efficiency, and requirements for P fertilizers may not increase in such species in future CO 2 -rich climates. © The Author 2016. Published by Oxford University Press on behalf of the Society for Experimental Biology.

  17. The effect of improving cow productivity, fertility, and longevity on the global warming potential of dairy systems.

    PubMed

    Bell, M J; Wall, E; Russell, G; Simm, G; Stott, A W

    2011-07-01

    This study compared the environmental impact of a range of dairy production systems in terms of their global warming potential (GWP, expressed as carbon dioxide equivalents, CO(2)-eq.) and associated land use, and explored the efficacy of reducing said impact. Models were developed using the unique data generated from a long-term genetic line × feeding system experiment. Holstein-Friesian cows were selected to represent the UK average for milk fat plus protein production (control line) or were selected for increased milk fat plus protein production (select line). In addition, cows received a low forage diet (50% forage) with no grazing or were on a high forage (75% forage) diet with summer grazing. A Markov chain approach was used to describe the herd structure and help estimate the GWP per year and land required per cow for the 4 alternative systems and the herd average using a partial life cycle assessment. The CO(2)-eq. emissions were expressed per kilogram of energy-corrected milk (ECM) and per hectare of land use, as well as land required per kilogram of ECM. The effects of a phenotypic and genetic standard deviation unit improvement on herd feed utilization efficiency, ECM yield, calving interval length, and incidence of involuntary culling were assessed. The low forage (nongrazing) feeding system with select cows produced the lowest CO(2)-eq. emissions of 1.1 kg/kg of ECM and land use of 0.65 m(2)/kg of ECM but the highest CO(2)-eq. emissions of 16.1t/ha of the production systems studied. Within the herd, an improvement of 1 standard deviation in feed utilization efficiency was the only trait of those studied that would significantly reduce the reliance of the farming system on bought-in synthetic fertilizer and concentrate feed, as well as reduce the average CO(2)-eq. emissions and land use of the herd (both by about 6.5%, of which about 4% would be achievable through selective breeding). Within production systems, reductions in CO(2)-eq. emissions per kilogram of ECM and CO(2)-eq. emissions per hectare were also achievable by an improvement in feed utilization. This study allowed development of models that harness the biological trait variation in the animal to improve the environmental impact of the farming system. Genetic selection for efficient feed use for milk production according to feeding system can bring about reductions in system nutrient requirements, CO(2)-eq. emissions, and land use per unit product. Copyright © 2011 American Dairy Science Association. Published by Elsevier Inc. All rights reserved.

  18. Improved performance of CdSe/CdS/PbS co-sensitized solar cell with double-layered TiO2 films as photoanode

    NASA Astrophysics Data System (ADS)

    Zhang, Xiaolong; Lin, Yu; Wu, Jihuai; Jing, Jing; Fang, Biaopeng

    2017-07-01

    Improving the photovoltaic performance of CdSe/CdS/PbS co-sensitized double-layered TiO2 solar cells is reported. Double-layered TiO2 films with TiO2 microspheres as the light blocking layers were prepared. PbS, CdS and CdSe quantum dots (QDs) were assembled onto TiO2 photoanodes by simple successive ionic layer absorption and reaction (SILAR) to fabricate CdSe/CdS/PbS co-sensitized solar cells. An improved power conversion efficiency (PCE) of 5.11% was achieved for CdSe/CdS/PbS co-sensitized solar cells at one sun illumination (AM 1.5 G, 100 mW cm-2), which had an improvement of 22.6% over that of the CdSe/CdS co-sensitized solar cells (4.17%). This enhancement is mainly attributed to their better ability of the absorption of solar light with the existence of PbS QDs, the reduction of charge recombination of the excited electron and longer lifetime of electrons, which have been proved with the photovoltaic studies and electrochemical impedance spectroscopy (EIS).

  19. DFT study on bimetallic Pt/Cu(1 1 1) as efficient catalyst for H2 dissociation

    NASA Astrophysics Data System (ADS)

    Liu, Ji; Fan, Xiaofeng; Sun, Chang Q.; Zhu, Weiguang

    2018-05-01

    To design a catalyst for the dissociation of H2 with better CO-tolerance performance is very important for proton exchange membrane fuel cells (PEMFCs) towards high efficiency. With slab model, the catalytic properties of overlayer Pt on Cu substrate (Pt/Cu) are analyzed by first-principle calculations. The CO saturation coverage (40%) on Pt2/Cu is found to be lower than that of pure Pt (about 75%). The dissociation barrier from H2 to H is less than 0.4 eV under the saturation coverage of CO. On the basis of kinetics of proton formation, the CO-tolerance ability on double-layer Pt with Cu is found to be greatly improved compared with that on pure Pt. It is expected that Pt overlayer on Cu(1 1 1) is a potential anode material with lower cost for PEMFCs.

  20. Design Guidelines for High-Performance Particle-Based Photoanodes for Water Splitting: Lanthanum Titanium Oxynitride as a Model.

    PubMed

    Landsmann, Steve; Maegli, Alexandra E; Trottmann, Matthias; Battaglia, Corsin; Weidenkaff, Anke; Pokrant, Simone

    2015-10-26

    Semiconductor powders are perfectly suited for the scalable fabrication of particle-based photoelectrodes, which can be used to split water using the sun as a renewable energy source. This systematic study is focused on variation of the electrode design using LaTiO2 N as a model system. We present the influence of particle morphology on charge separation and transport properties combined with post-treatment procedures, such as necking and size-dependent co-catalyst loading. Five rules are proposed to guide the design of high-performance particle-based photoanodes by adding or varying several process steps. We also specify how much efficiency improvement can be achieved using each of the steps. For example, implementation of a connectivity network and surface area enhancement leads to thirty times improvement in efficiency and co-catalyst loading achieves an improvement in efficiency by a factor of seven. Some of these guidelines can be adapted to non-particle-based photoelectrodes. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  1. C4 grasses prosper as carbon dioxide eliminates desiccation in warmed semi-arid grassland.

    PubMed

    Morgan, Jack A; LeCain, Daniel R; Pendall, Elise; Blumenthal, Dana M; Kimball, Bruce A; Carrillo, Yolima; Williams, David G; Heisler-White, Jana; Dijkstra, Feike A; West, Mark

    2011-08-03

    Global warming is predicted to induce desiccation in many world regions through increases in evaporative demand. Rising CO(2) may counter that trend by improving plant water-use efficiency. However, it is not clear how important this CO(2)-enhanced water use efficiency might be in offsetting warming-induced desiccation because higher CO(2) also leads to higher plant biomass, and therefore greater transpirational surface. Furthermore, although warming is predicted to favour warm-season, C(4) grasses, rising CO(2) should favour C(3), or cool-season plants. Here we show in a semi-arid grassland that elevated CO(2) can completely reverse the desiccating effects of moderate warming. Although enrichment of air to 600 p.p.m.v. CO(2) increased soil water content (SWC), 1.5/3.0 °C day/night warming resulted in desiccation, such that combined CO(2) enrichment and warming had no effect on SWC relative to control plots. As predicted, elevated CO(2) favoured C(3) grasses and enhanced stand productivity, whereas warming favoured C(4) grasses. Combined warming and CO(2) enrichment stimulated above-ground growth of C(4) grasses in 2 of 3 years when soil moisture most limited plant productivity. The results indicate that in a warmer, CO(2)-enriched world, both SWC and productivity in semi-arid grasslands may be higher than previously expected.

  2. Removing CO2 and moisture from air

    NASA Technical Reports Server (NTRS)

    Tepper, E. H.

    1977-01-01

    Foamed-aluminum blocks act as passive heat exchanger to improve efficiency. Improved closed-cycle atmospheric scrubber, level of carbon dioxide, and water vapor are reduced without affecting temperature of airstream. Exchangers draw impurities from air without additional heaters of auxillary equipment.

  3. Response surface method for modeling the removal of carbon dioxide from a simulated gas using water absorption enhanced with a liquid-film-forming device.

    PubMed

    Nguyen, Diem-Mai Kim; Imai, Tsuyoshi; Dang, Thanh-Loc Thi; Kanno, Ariyo; Higuchi, Takaya; Yamamoto, Koichi; Sekine, Masahiko

    2018-03-01

    This paper presents the results from using a physical absorption process to absorb gaseous CO 2 mixed with N 2 using water by producing tiny bubbles via a liquid-film-forming device (LFFD) that improves the solubility of CO 2 in water. The influence of various parameters-pressure, initial CO 2 concentration, gas-to-liquid ratios, and temperature-on the CO 2 removal efficiency and its absorption rate in water were investigated and estimated thoroughly by statistical polynomial models obtained by the utilization of the response surface method (RSM) with a central composite design (CCD). Based on the analysis, a high efficiency of CO 2 capture can be reached in conditions such as low pressure, high CO 2 concentration at the inlet, low gas/liquid ratio, and low temperature. For instance, the highest removal efficiency in the RSM-CCD experimental matrix of nearly 80% occurred for run number 20, which was conducted at 0.30MPa, CO 2 concentration of 35%, gas/liquid ratio of 0.71, and temperature of 15°C. Furthermore, the coefficients of determination, R 2 , were 0.996 for the removal rate and 0.982 for the absorption rate, implying that the predicted values computed by the constructed models correlate strongly and fit well with the experimental values. The results obtained provide essential information for implementing this method properly and effectively and contribute a promising approach to the problem of CO 2 capture in air pollution treatment. Copyright © 2017. Published by Elsevier B.V.

  4. Novel CO 2 Foam Concepts and Injection Schemes for Improving CO 2 Sweep Efficiency in Sandstone and Carbonate Hydrocarbon Formations

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Nguyen, Quoc; Hirasaki, George; Johnston, Keith

    2015-02-05

    We explored cationic, nonionic and zwitterionic surfactants to identify candidates that have the potential to satisfy all the key requirements for CO 2 foams in EOR. We have examined the formation, texture, rheology and stability of CO 2 foams as a function of the surfactant structure and formulation variables including temperature, pressure, water/CO 2 ratio, surfactant concentration, salinity and concentration of oil. Furthermore, the partitioning of surfactants between oil and water as well as CO 2 and water was examined in conjunction with adsorption measurements on limestone by the Hirasaki lab to develop strategies to optimize the transport of surfactantsmore » in reservoirs.« less

  5. Effect of co-crystallization on singlet fission efficiency in pentacene derivatives

    NASA Astrophysics Data System (ADS)

    Wang, Xiaopeng; Sanders, Samuel; Campos, Luis; Sfeir, Matthew; Marom, Noa

    Singlet fission (SF), the conversion of one singlet exciton into two triplet excitons, may lead to a twofold increase in the efficiency of organic photovoltaics. Since SF has been observed in crystalline pentacene, this material has drawn interest both experimentally and theoretically. Recently, it has been shown that SF efficiency in rubrene may be improved by modifying the crystal packing. Here, we study the effect of co-crystallization with small molecule H-bond donors on SF efficiency in pentacene derivatives. Five co-crystals are synthetized and their photoluminescence (PL) and absorption spectra are measured. First-principles calculations based on many-body perturbation theory (MBPT) are then employed to study their excitonic properties. By combining experiment and theory, we demonsrate that excitonic properties, including singlet-triplet gaps, exciton binding energies, and exciton localization, are significantly modulated in pentacene co-crystals. Consequently, co-crystallization becomes an effective strategy for improving SF efficiency in molecular crystals of organic semiconductors.

  6. Increasing Gas Hydrate Formation Temperature for Desalination of High Salinity Produced Water with Secondary Guests

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Cha, Jong-Ho; Seol, Yongkoo

    We suggest a new gas hydrate-based desalination process using water-immiscible hydrate formers; cyclopentane (CP) and cyclohexane (CH) as secondary hydrate guests to alleviate temperature requirements for hydrate formation. The hydrate formation reactions were carried out in an isobaric condition of 3.1 MPa to find the upper temperature limit of CO2 hydrate formation. Simulated produced water (8.95 wt % salinity) mixed with the hydrate formers shows an increased upper temperature limit from -2 °C for simple CO2 hydrate to 16 and 7 °C for double (CO2 + CP) and (CO2 + CH) hydrates, respectively. The resulting conversion rate to double hydratemore » turned out to be similar to that with simple CO2 hydrate at the upper temperature limit. Hydrate formation rates (Rf) for the double hydrates with CP and CH are shown to be 22 and 16 times higher, respectively, than that of the simple CO2 hydrate at the upper temperature limit. Such mild hydrate formation temperature and fast formation kinetics indicate increased energy efficiency of the double hydrate system for the desalination process. Dissociated water from the hydrates shows greater than 90% salt removal efficiency for the hydrates with the secondary guests, which is also improved from about 70% salt removal efficiency for the simple hydrates.« less

  7. Ultrasound-assisted extraction and quantitation of oils from Syzygium aromaticum flower bud (clove) with supercritical carbon dioxide.

    PubMed

    Yang, Yu-Chiao; Wei, Ming-Chi; Hong, Show-Jen

    2014-01-03

    This study evaluated ultrasound-assisted supercritical carbon dioxide (USC-CO2) extraction for determining the extraction yields of oils and the contents of eugenol, β-caryophyllene, eugenyl acetate and α-humulene from clove buds. Compared to traditional SC-CO2 extraction, USC-CO2 extraction might provide a 13.5% increase in the extraction yield for the oil while utilizing less severe operating parameters, such as temperature, pressure, CO2 flow rate and the time consumed by the process. Our results were comparable to those obtained using the heat reflux extraction method, though the yield was improved by 20.8% using USC-CO2. In kinetic studies, the USC-CO2 extraction of clove oil followed second-order kinetics. The activation energy for the oil extraction was 76.56kJ/mol. The USC-CO2 procedure facilitated the use of mild extraction conditions, improved extraction efficiency and the quality of products and is a potential method for industry. Copyright © 2013 Elsevier B.V. All rights reserved.

  8. Can Advances in Science and Technology Prevent Global Warming? A Critical Review of Limitations and Challenges

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Huesemann, Michael H.

    The most stringent emission scenarios published by the Intergovernmental Panel on Climate Change (IPCC) would result in the stabilization of atmospheric carbon dioxide (CO2) at concentrations of approximately 550 ppm which would produce a global temperature increase of at least 2 C by 2100. Given the large uncertainties regarding the potential risks associated with this degree of global warming, it would be more prudent to stabilize atmospheric CO2 concentrations at or below current levels which, in turn, would require a greater than 20-fold reduction (i.e., ?95%) in per capita carbon emissions in industrialized nations within the next 50 to 100more » years. Using the Kaya equation as a conceptual framework, this paper examines whether CO2 mitigation approaches such as energy efficiency improvements, carbon sequestration, and the development of carbon-free energy sources would be sufficient to bring about the required reduction in per capita carbon emissions without creating unforeseen negative impacts elsewhere. In terms of energy efficiency, large improvements (?5-fold) are in principle possible given aggressive investments in R&D and if market imperfections such as corporate subsidies are removed. However, energy efficiency improvements per se will not result in a reduction in carbon emissions if, as predicted by the IPCC, the size of the global economy has expanded 12-26 fold by 2100. Terrestrial carbon sequestration via reforestation and improved agricultural soil management has many environmental advantages but has only limited CO2 mitigation potential because the global terrestrial carbon sink (ca. 200 Gt C) is small relative to the size of fossil fuel deposits (?4000 Gt C). By contrast, very large amounts of CO2 can potentially be removed from the atmosphere via sequestration in geologic formations and oceans, but carbon storage is not permanent and is likely to create many unpredictable environmental consequences. Renewable solar energy can in theory provide large amounts of carbon-free power. However, biomass and hydroelectric energy can only be marginally expanded and large-scale solar energy installations (i.e., wind, photovoltaics, and direct thermal) are likely to have significant negative environmental impacts. Expansion of nuclear energy is highly unlikely due to concerns over reactor safety, radioactive waste management, weapons proliferation, and cost. In view of the serious limitations and liabilities of many proposed CO2 mitigation approaches it appears that there remain only few no-regrets options such as drastic energy efficiency improvements, extensive terrestrial carbon sequestration, and cautious expansion of renewable energy generation. These promising CO2 mitigation technologies have the potential to bring about the required 20-fold reduction in per capita carbon emission only if population and economic growth are halted without delay. Thus, addressing the problem of global warming requires not only technological research and development but also a reexamination of core values that mistakenly equate material consumption and economic growth to happiness and well-being.« less

  9. Role of Co-Sensitizers in Dye-Sensitized Solar Cells.

    PubMed

    Krishna, Narra Vamsi; Krishna, Jonnadula Venkata Suman; Mrinalini, Madoori; Prasanthkumar, Seelam; Giribabu, Lingamallu

    2017-12-08

    Co-sensitization is a popular route towards improved efficiency and stability of dye-sensitized solar cells (DSSCs). In this context, the power conversion efficiency (PCE) values of DSSCs incorporating Ru- and porphyrin-based dyes can be improved from 8-11 % to 11-14 % after the addition of additives, co-adsorbents, and co-sensitizers that reduce aggregation and charge recombination in the device. Among the three supporting material types, co-sensitizers play a major role to enhance the performance and stability of DSSCs, which is requried for commercialization. In this Minireview, we highlight the role co-sensitizers play in improving photovoltaic performance of devices containing Ru- and porphyrin-based sensitizers. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  10. Benefits of Leapfrogging to Superefficiency and Low Global Warming Potential Refrigerants in Room Air Conditioning

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Shah, Nihar; Wei, Max; Letschert, Virginie

    2015-10-01

    Hydrofluorocarbons (HFCs) emitted from uses such as refrigerants and thermal insulating foam, are now the fastest growing greenhouse gases (GHGs), with global warming potentials (GWP) thousands of times higher than carbon dioxide (CO2). Because of the short lifetime of these molecules in the atmosphere, mitigating the amount of these short-lived climate pollutants (SLCPs) provides a faster path to climate change mitigation than control of CO2 alone. This has led to proposals from Africa, Europe, India, Island States, and North America to amend the Montreal Protocol on Substances that Deplete the Ozone Layer (Montreal Protocol) to phase-down high-GWP HFCs. Simultaneously, energymore » efficiency market transformation programs such as standards, labeling and incentive programs are endeavoring to improve the energy efficiency for refrigeration and air conditioning equipment to provide life cycle cost, energy, GHG, and peak load savings. In this paper we provide an estimate of the magnitude of such GHG and peak electric load savings potential, for room air conditioning, if the refrigerant transition and energy efficiency improvement policies are implemented either separately or in parallel. We find that implementing HFC refrigerant transition and energy efficiency improvement policies in parallel for room air conditioning, roughly doubles the benefit of either policy implemented separately. We estimate that shifting the 2030 world stock of room air conditioners from the low efficiency technology using high-GWP refrigerants to higher efficiency technology and low-GWP refrigerants in parallel would save between 340-790 gigawatts (GW) of peak load globally, which is roughly equivalent to avoiding 680-1550 peak power plants of 500MW each. This would save 0.85 GT/year annually in China equivalent to over 8 Three Gorges dams and over 0.32 GT/year annually in India equivalent to roughly twice India’s 100GW solar mission target. While there is some uncertainty associated with emissions and growth projections, moving to efficient room air conditioning (~30% more efficient than current technology) in parallel with low-GWP refrigerants in room air conditioning could avoid up to ~25 billion tonnes of CO2 in 2030, ~33 billion in 2040, and ~40 billion in 2050, i.e. cumulative savings up to 98 billion tonnes of CO2 by 2050. Therefore, superefficient room ACs using low-GWP refrigerants merit serious consideration to maximize peak load reduction and GHG savings.« less

  11. Measurements and modeling of CO 2 concentration and isotopes to improve process-level understanding of Arctic and boreal carbon cycling. Final Report

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Keeling, Ralph F.

    The major goal of this project was to improve understanding of processes that control the exchanges of CO 2 between the atmosphere and the land biosphere on decadal and longer time scales. The approach involves measuring the changes in atmospheric CO 2 concentration and the isotopes of CO 2 ( 13C/ 12C and 18O/ 16O) at background stations and uses these and other datasets to challenge and improve numerical models of the earth system. The project particularly emphasized the use of these data to improve understanding of changes occurring in boreal and arctic ecosystems over the past 50 years andmore » to seek from these data improved understanding of large-scale processes impacting carbon cycling, such as the responses to warming, CO 2 fertilization, and disturbance. The project also led to advances in the understanding of changes in water-use efficiency of land ecosystems globally based on trends in 13C/ 12C. The core element of this project was providing partial support for continuing measurements of CO 2 concentrations and isotopes from the Scripps CO 2 program, initiated by C. D. Keeling in the 1960s. The measurements included analysis of flasks collected at an array of ten stations distributed from the Arctic to the Antarctic. The project also supported modeling studies and interpretive work to help understand the origins of the large ~50% increase in the amplitude of the atmospheric CO 2 cycle detected at high northern latitudes between 1960 and present and to understand the long-term trend in carbon 13C/ 12C of CO 2. The seasonal cycle work was advanced through collaborations with colleagues at MPI Jena and Imperial College« less

  12. Potentiel des méthodes de séparation et stockage du CO2 dans la lutte contre l'effet de serreThe role of CO2 capture and sequestration in mitigation of climate change

    NASA Astrophysics Data System (ADS)

    Jean-Baptiste, Philippe; Ducroux, René

    2003-06-01

    Increasing atmospheric level of greenhouse gases are causing global warming and putting at risk the global climate system. The main anthropogenic greenhouse gas is CO 2. Technical solutions exist to reduce CO 2 emission and stabilise atmospheric CO 2 concentration, including energy saving and energy efficiency, switch to lower carbon content fuels like natural gas and to energy sources that operate with zero CO 2 emissions such as renewable or nuclear energy, enhance the natural sinks for CO 2 (forests, soils, etc.), and last but not least, sequester CO 2 from fossil fuels combustion. The purpose of this paper is to provide an overview of the technology and cost for capture and storage of CO 2. Some of the factors that will influence application, including environmental impact, cost and efficiency, are also discussed. Capturing CO 2 and storing it in underground geological reservoirs appears as the best environmentally acceptable option. It can be done with existing technology; however, substantial R&D is needed to improve available technology and to lower the cost. Applicable to large CO 2 emitting industrial facilities such as power plants, cement factories, steel industry, etc., which amount to more than 30% of the global anthropogenic CO 2 emission, it represents a valuable tool in the battle against global warming. To cite this article: P. Jean-Baptiste, R. Ducroux, C. R. Geoscience 335 (2003).

  13. Performance improvement of gel- and solid-state dye-sensitized solar cells by utilization the blending effect of poly (vinylidene fluoride-co-hexafluropropylene) and poly (acrylonitrile-co-vinyl acetate) co-polymers

    NASA Astrophysics Data System (ADS)

    Venkatesan, Shanmugam; Obadja, Nesia; Chang, Ting-Wei; Chen, Li-Tung; Lee, Yuh-Lang

    2014-12-01

    Poly (vinylidene fluoride-co-hexafluropropylene) (PVDF-HFP) and poly (acrylonitrile-co-vinyl acetate) (PAN-VA) are used as gelator to prepare gel- and solid-state polymer electrolytes for dye sensitized solar cells (DSSCs) applications. The electrolytes prepared using PVDF-HFP have higher conductivities than those prepared using PAN-VA. In blended polymers, the conductivities of the electrolytes increase with increasing composition of PVDF-HFP; at 75% PVDF-HFP, conductivity of the blended polymer surpassed that of pure polymers. It is also found that the viscosity of the electrolyte prepared by PAN-VA (1.2 kPaS) is much lower than that by PVDF-HFP (11 kPaS). Therefore, increasing PAN-VA composition can decrease the viscosity of the electrolyte, improving the penetration of electrolytes in the TiO2 matrix. By controlling the ratio of PVDF-HFP/PAN-VA, the conductivity and viscosity of the electrolyte can be regulated and an optimal ratio based on the conversion efficiency of the gel- and solid state DSSCs is obtained at the ratio of 3/1. The highest efficiency achieved by the gel- and solid-state cells using the blending polymers are 6.3% and 4.88%, respectively, which are higher than those prepared using pure polymers (5.53% and 4.56%, respectively). The introduction of TiO2 fillers to the solid electrolyte can further increase the cell efficiency to 5.34%.

  14. Chemical Method to Improve CO{sub 2} Flooding Sweep Efficiency for Oil Recovery Using SPI-CO{sub 2} Gels

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Burns, Lyle D.

    2009-04-14

    The problem in CO{sub 2} flooding lies with its higher mobility causing low conformance or sweep efficiency. This is an issue in oilfield applications where an injected fluid or gas used to mobilize and produce the oil in a marginal field has substantially higher mobility (function of viscosity and density and relative permeability) relative to the crude oil promoting fingering and early breakthrough. Conformance is particularly critical in CO{sub 2} oilfield floods where the end result is less oil recovered and substantially higher costs related to the CO{sub 2}. The SPI-CO{sub 2} (here after called “SPI”) gel system is amore » unique silicate based gel system that offers a technically effective solution to the conformance problem with CO{sub 2} floods. This SPI gel system remains a low viscosity fluid until an external initiator (CO{sub 2}) triggers gelation. This is a clear improvement over current technologies where the gels set up as a function of time, regardless of where it is placed in the reservoir. In those current systems, the internal initiator is included in the injected fluid for water shut off applications. In this new research effort, the CO{sub 2} is an external initiator contacted after SPI gel solution placement. This concept ensures in the proper water wet reservoir environment that the SPI gel sets up in the precise high permeability path followed by the CO{sub 2}, therefore improving sweep efficiency to a greater degree than conventional systems. In addition, the final SPI product in commercial quantities is expected to be low cost over the competing systems. This Phase I research effort provided “proof of concept” that SPI gels possess strength and may be formed in a sand pack reducing the permeability to brine and CO{sub 2} flow. This SPI technology is a natural extension of prior R & D and the Phase I effort that together show a high potential for success in a Phase II follow-on project. Carbon dioxide (CO{sub 2}) is a major by-product of hydrocarbon combustion for energy, chemical and fertilizer plants. For example, coal fired power plants emit large amounts of CO{sub 2} in order to produce electrical energy. Carbon dioxide sequestration is gaining attention as concerns mount over possible global climate change caused by rising emissions of greenhouse gases. Removing the CO{sub 2} from the energy generation process would make these plants more environmentally friendly. In addition, CO{sub 2} flooding is an attractive means to enhance oil and natural gas recovery. Capture and use of the CO{sub 2} from these plants for recycling into CO{sub 2} flooding of marginal reservoirs provides a “dual use” opportunity prior to final CO{sub 2} sequestration in the depleted reservoir. Under the right pressure, temperature and oil composition conditions, CO{sub 2} can act as a solvent, cleaning oil trapped in the microscopic pores of the reservoir rock. This miscible process greatly increases the recovery of crude oil from a reservoir compared to recovery normally seen by waterflooding. An Enhanced Oil Recovery (EOR) project that uses an industrial source of CO{sub 2} that otherwise would be vented to the atmosphere has the added environmental benefit of sequestering the greenhouse gas.« less

  15. Improving carbon dioxide yields and cell efficiencies for ethanol oxidation by potential scanning

    NASA Astrophysics Data System (ADS)

    Majidi, Pasha; Pickup, Peter G.

    2014-12-01

    An ethanol electrolysis cell with aqueous ethanol supplied to the anode and nitrogen at the cathode has been operated under potential cycling conditions in order to increase the yield of carbon dioxide and thereby increase cell efficiency relative to operation at a fixed potential. At ambient temperature, faradaic yields of CO2 as high as 26% have been achieved, while only transient CO2 production was observed at constant potential. Yields increased substantially at higher temperatures, with maximum values at Pt anodes reaching 45% at constant potential and 65% under potential cycling conditions. Use of a PtRu anode increased the cell efficiency by decreasing the anode potential, but this was offset by decreased CO2 yields. Nonetheless, cycling increased the efficiency relative to constant potential. The maximum yields at PtRu and 80 °C were 13% at constant potential and 32% under potential cycling. The increased yields under cycling conditions have been attributed to periodic oxidative stripping of adsorbed CO, which occurs at lower potentials on PtRu than on Pt. These results will be important in the optimization of operating conditions for direct ethanol fuel cells and for the electrolysis of ethanol to produce clean hydrogen.

  16. Promoting Ethylene Selectivity from CO2 Electroreduction on CuO Supported onto CO2 Capture Materials.

    PubMed

    Yang, Hui-Juan; Yang, Hong; Hong, Yu-Hao; Zhang, Peng-Yang; Wang, Tao; Chen, Li-Na; Zhang, Feng-Yang; Wu, Qi-Hui; Tian, Na; Zhou, Zhi-You; Sun, Shi-Gang

    2018-03-09

    Cu is a unique catalyst for CO 2 electroreduction, since it can catalyze CO 2 reduction to a series of hydrocarbons, alcohols, and carboxylic acids. Nevertheless, such Cu catalysts suffer from poor selectivity. High pressure of CO 2 is considered to facilitate the activity and selectivity of CO 2 reduction. Herein, a new strategy is presented for CO 2 reduction with improved C 2 H 4 selectivity on a Cu catalyst by using CO 2 capture materials as the support at ambient pressure. N-doped carbon (N x C) was synthesized through high-temperature carbonization of melamine and l-lysine. We observed that the CO 2 uptake capacity of N x C depends on both the microporous area and the content of pyridinic N species, which can be controlled by the carbonization temperature (600-800 °C). The as-prepared CuO/N x C catalysts exhibit a considerably higher C 2 H 4 faradaic efficiency (36 %) than CuO supported on XC-72 carbon black (19 %), or unsupported CuO (20 %). Moreover, there is a good linear relationship between the C 2 H 4 faradaic efficiency and CO 2 uptake capacity of the supports for CuO. The local high CO 2 concentration near Cu catalysts, created by CO 2 capture materials, was proposed to increase the coverage of CO intermediate, which is favorable for the coupling of two CO units in the formation of C 2 H 4 . This study demonstrates that pairing Cu catalysts with CO 2 capture supports is a promising approach for designing highly effective CO 2 reduction electrocatalysts. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  17. Equilibrium model analysis of waste plastics gasification using CO2 and steam.

    PubMed

    Kannan, P; Lakshmanan, G; Al Shoaibi, A; Srinivasakannan, C

    2017-12-01

    Utilization of carbon dioxide (CO 2 ) in thermochemical treatment of waste plastics may significantly help to improve CO 2 recycling, thus simultaneously curtailing dioxins/furans and CO 2 emissions. Although CO 2 is not such an effective gasifying agent as steam, a few investigations have explored the utilization of CO 2 in conjunction with steam to achieve somewhat higher carbon conversion. This work presents a comparative evaluation study of CO 2 and steam gasification of a typical post-consumer waste plastics mixture using an Aspen Plus equilibrium model. The effect of flow rate of gasifying medium (CO 2 and/or steam) and gasification temperature on product gas composition, carbon conversion, and cold gas efficiency has been analyzed. Simulation results demonstrate that CO 2 can serve as a potential gasifying agent for waste plastics gasification. The resulting product gas was rich in CO whereas CO 2 -steam blends yield a wider H 2 /CO ratio, thus extending the applications of the product gas.

  18. Conversion of CO2 into cyclic carbonates by a Co(ii) metal-organic framework and the improvement of catalytic activity via nanocrystallization.

    PubMed

    Ji, Xiao-He; Zhu, Ning-Ning; Ma, Jian-Gong; Cheng, Peng

    2018-02-06

    The Co(ii) metal-organic framework (MOF) {[Co(μ 3 -L)(H 2 O)]·0.5H 2 O} n (1, H 2 L = thiazolidine 2,4-dicarboxylic acid) with rich Lewis acid sites was used as a catalyst for the conversion of CO 2 and propylene oxide into propylene carbonate with a yield of up to 98% under 50 °C and 1 atm. 1 exhibited excellent reusability, which could be regenerated easily for at least five runs without a decrease in the yield. Importantly, we synthesized two types of nano-crystals (N1 and N2) of 1 with polyvinylpyrrolidone (PVP) and hexadecyltrimethylammonium bromide (CTAB) as surfactants, respectively, and investigated their catalytic properties in comparison with that of 1 in the powder phase. A significant enhancement in both catalytic efficiency and product yield was observed when 1 was nano-crystallized. This is the first investigation about the relationship between the morphology and the catalytic parameters of MOFs. The results showed a strategy for efficiently applying MOFs as catalysts towards CO 2 conversion, which could also be used in other MOF-catalyzed processes.

  19. Role of Additives in Composite PEI/Oxide CO 2 Adsorbents: Enhancement in the Amine Efficiency of Supported PEI by PEG in CO 2 Capture from Simulated Ambient Air

    DOE PAGES

    Sakwa-Novak, Miles A.; Tan, Shuai; Jones, Christopher W.

    2015-10-20

    Supported amines are promising candidate adsorbents for the removal of CO 2 from flue gases and directly from ambient air. The incorporation of additives into polymeric amines such as poly(ethylenimine) (PEI) supported on mesoporous oxides is an effective strategy to improve the performance of the materials. Here, several practical aspects of this strategy are addressed with regards to direct air capture. The influence of three additives (CTAB, PEG200, PEG1000) was systematically explored under dry simulated air capture conditions (400 ppm of CO 2, 30 °C). With SBA-15 as a model support for poly(ethylenimine) (PEI), the nature of the additive inducedmore » heterogeneities in the deposition of organic on the interior and exterior of the particles, an important consideration for future scale up to practical systems. The PEG200 additive increased the observed thermodynamic performance (~60% increase in amine efficiency) of the adsorbents regardless of the PEI content, while the other molecules had less positive effects. A threshold PEG200/PEI value was identified at which the diffusional limitations of CO 2 within the materials were nearly eliminated. The threshold PEG/PEI ratio may have physical origin in the interactions between PEI and PEG, as the optimal ratio corresponded to nearly equimolar OH/reactive (1°, 2°) amine ratios. As a result, the strategy is shown to be robust to the characteristics of the host support, as PEG200 improved the amine efficiency of PEI when supported on two varieties of mesoporous γ-alumina with PEI.« less

  20. Role of Additives in Composite PEI/Oxide CO 2 Adsorbents: Enhancement in the Amine Efficiency of Supported PEI by PEG in CO 2 Capture from Simulated Ambient Air

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Sakwa-Novak, Miles A.; Tan, Shuai; Jones, Christopher W.

    Supported amines are promising candidate adsorbents for the removal of CO 2 from flue gases and directly from ambient air. The incorporation of additives into polymeric amines such as poly(ethylenimine) (PEI) supported on mesoporous oxides is an effective strategy to improve the performance of the materials. Here, several practical aspects of this strategy are addressed with regards to direct air capture. The influence of three additives (CTAB, PEG200, PEG1000) was systematically explored under dry simulated air capture conditions (400 ppm of CO 2, 30 °C). With SBA-15 as a model support for poly(ethylenimine) (PEI), the nature of the additive inducedmore » heterogeneities in the deposition of organic on the interior and exterior of the particles, an important consideration for future scale up to practical systems. The PEG200 additive increased the observed thermodynamic performance (~60% increase in amine efficiency) of the adsorbents regardless of the PEI content, while the other molecules had less positive effects. A threshold PEG200/PEI value was identified at which the diffusional limitations of CO 2 within the materials were nearly eliminated. The threshold PEG/PEI ratio may have physical origin in the interactions between PEI and PEG, as the optimal ratio corresponded to nearly equimolar OH/reactive (1°, 2°) amine ratios. As a result, the strategy is shown to be robust to the characteristics of the host support, as PEG200 improved the amine efficiency of PEI when supported on two varieties of mesoporous γ-alumina with PEI.« less

  1. Climate stabilization wedges in action: a systems approach to energy sustainability for Hawaii Island.

    PubMed

    Johnson, Jeremiah; Chertow, Marian

    2009-04-01

    Pacala and Socolow developed a framework to stabilize global greenhouse gas levels for the next fifty years using wedges of constant size representing an increasing use of existing technologies and approaches for energy efficiency, carbon free generation, renewables, and carbon storage. The research presented here applies their approach to Hawaii Island, with modifications to support local scale analysis and employing a "bottom-up" methodology that allows for wedges of various sizes. A discretely bounded spatial unit offers a testing ground for a holistic approach to improving the energy sector with the identification of local options and limitations to the implementation of a comprehensive energy strategy. Nearly 80% of total primary energy demand across all sectors for Hawaii Island is currently met using petroleum-based fuels.The Sustainable Energy Plan scenario included here presents an internally consistent set of recommendations bounded by local constraints in areas such as transportation efficiency, centralized renewable generation (e.g., geothermal, wind), reduction in transmission losses, and improved building efficiency. This scenario shows thatthe demand for primary energy in 2030 could be reduced by 23% through efficiency measures while 46% could be met by renewable generation, resulting in only 31% of the projected demand being met by fossil fuels. In 2030, the annual releases of greenhouse gases would be 3.2 Mt CO2-eq/year under the Baseline scenario, while the Sustainable Energy Plan would reduce this to 1.2 Mt CO2-eq/year--an annual emissions rate 40% below 2006 levels and 10% below 1990 levels. The total for greenhouse gas emissions during the 24-year study period (2007 to 2030) is 59.9 Mt CO2-eq under the Baseline scenario and 32.5 Mt CO2-eq under the Sustainable Energy Plan scenario. Numerous combinations of efficiency and renewable energy options can be employed in a manner that stabilizes the greenhouse gas emissions of Hawaii Island.

  2. Wet air co-oxidation of decabromodiphenyl ether (BDE209) and tetrahydrofuran.

    PubMed

    Zhao, Hongxia; Zhang, Feifang; Qu, Baocheng; Xue, Xingya; Liang, Xinmiao

    2009-09-30

    The wet air co-oxidation (WACO) of a major commercial polybrominated diphenyl ether flame retardant congener, decabromodiphenyl ether (BDE209), was investigated using tetrahydrofuran (THF) as an initiator in a stainless autoclave at temperature range of 120-170 degrees C and 0.5MPa oxygen pressure. Compared to the single oxidation of BDE209 under the same conditions, the addition of THF in the reaction system greatly improved the removal efficiency of BDE209. The effect of temperature on the reaction was studied. The removals of BDE209 and Br increased with increasing temperature. In addition, the effect of NaNO(2) as the catalyst on the WACO was also investigated and the results showed that the addition of NaNO(2) could improve the Br removal efficiency.

  3. Isoleucine 309 acts as a C4 catalytic switch that increases ribulose-1,5-bisphosphate carboxylase/oxygenase (rubisco) carboxylation rate in Flaveria.

    PubMed

    Whitney, Spencer M; Sharwood, Robert E; Orr, Douglas; White, Sarah J; Alonso, Hernan; Galmés, Jeroni

    2011-08-30

    Improving global yields of important agricultural crops is a complex challenge. Enhancing yield and resource use by engineering improvements to photosynthetic carbon assimilation is one potential solution. During the last 40 million years C(4) photosynthesis has evolved multiple times, enabling plants to evade the catalytic inadequacies of the CO(2)-fixing enzyme, ribulose-1,5-bisphosphate carboxylase/oxygenase (rubisco). Compared with their C(3) ancestors, C(4) plants combine a faster rubisco with a biochemical CO(2)-concentrating mechanism, enabling more efficient use of water and nitrogen and enhanced yield. Here we show the versatility of plastome manipulation in tobacco for identifying sequences in C(4)-rubisco that can be transplanted into C(3)-rubisco to improve carboxylation rate (V(C)). Using transplastomic tobacco lines expressing native and mutated rubisco large subunits (L-subunits) from Flaveria pringlei (C(3)), Flaveria floridana (C(3)-C(4)), and Flaveria bidentis (C(4)), we reveal that Met-309-Ile substitutions in the L-subunit act as a catalytic switch between C(4) ((309)Ile; faster V(C), lower CO(2) affinity) and C(3) ((309)Met; slower V(C), higher CO(2) affinity) catalysis. Application of this transplastomic system permits further identification of other structural solutions selected by nature that can increase rubisco V(C) in C(3) crops. Coengineering a catalytically faster C(3) rubisco and a CO(2)-concentrating mechanism within C(3) crop species could enhance their efficiency in resource use and yield.

  4. Isoleucine 309 acts as a C4 catalytic switch that increases ribulose-1,5-bisphosphate carboxylase/oxygenase (rubisco) carboxylation rate in Flaveria

    PubMed Central

    Whitney, Spencer M.; Sharwood, Robert E.; Orr, Douglas; White, Sarah J.; Alonso, Hernan; Galmés, Jeroni

    2011-01-01

    Improving global yields of important agricultural crops is a complex challenge. Enhancing yield and resource use by engineering improvements to photosynthetic carbon assimilation is one potential solution. During the last 40 million years C4 photosynthesis has evolved multiple times, enabling plants to evade the catalytic inadequacies of the CO2-fixing enzyme, ribulose-1,5-bisphosphate carboxylase/oxygenase (rubisco). Compared with their C3 ancestors, C4 plants combine a faster rubisco with a biochemical CO2-concentrating mechanism, enabling more efficient use of water and nitrogen and enhanced yield. Here we show the versatility of plastome manipulation in tobacco for identifying sequences in C4-rubisco that can be transplanted into C3-rubisco to improve carboxylation rate (VC). Using transplastomic tobacco lines expressing native and mutated rubisco large subunits (L-subunits) from Flaveria pringlei (C3), Flaveria floridana (C3-C4), and Flaveria bidentis (C4), we reveal that Met-309-Ile substitutions in the L-subunit act as a catalytic switch between C4 (309Ile; faster VC, lower CO2 affinity) and C3 (309Met; slower VC, higher CO2 affinity) catalysis. Application of this transplastomic system permits further identification of other structural solutions selected by nature that can increase rubisco VC in C3 crops. Coengineering a catalytically faster C3 rubisco and a CO2-concentrating mechanism within C3 crop species could enhance their efficiency in resource use and yield. PMID:21849620

  5. Combined Embedding of N/F-Doping and CaCO3 Surface Modification in the TiO2 Photoanode for Dye-Sensitized Solar Cells.

    PubMed

    Park, Su Kyung; Yun, Tae Kwan; Bae, Jae Young

    2016-03-01

    N/F-doping and CaCO3 surface modification was carried out in TiO2 photoelectrodes for dye-sensitized solar cells (DSSCs). The combined effect of the N/F doped TiO2 and the CaCO3 coating showed a great increase of the short-circuit current (J(sc)), and photoelectric conversion efficiency (η) of the prepared cells; the efficiency (η) was improved from 7.00% of a commercial TiO2 photoelectrode to 7.90% of an uncoated N/F-doped electrode, and to 9.09% of a N/F-doped and CaCO3 surface modified electrode. An enhanced photoresponse in N/F-doped TiO2 nanoparticles generate more photo-excited electrons, as supported by measured UV-Vis diffuse reflectance spectra. A successive CaCO3 surface modification then forms a barrier on the surface of the N/F-doped TiO2 particles; the higher basicity of the CaCO3 modified TiO2 facilitates the dye adsorption, as supported by the direct measurement of the amount of adsorbed dye.

  6. Efficient hydrogen evolution catalysis using ternary pyrite-type cobalt phosphosulphide

    NASA Astrophysics Data System (ADS)

    Cabán-Acevedo, Miguel; Stone, Michael L.; Schmidt, J. R.; Thomas, Joseph G.; Ding, Qi; Chang, Hung-Chih; Tsai, Meng-Lin; He-Hau, Jr.; Jin, Song

    2015-12-01

    The scalable and sustainable production of hydrogen fuel through water splitting demands efficient and robust Earth-abundant catalysts for the hydrogen evolution reaction (HER). Building on promising metal compounds with high HER catalytic activity, such as pyrite structure cobalt disulphide (CoS2), and substituting non-metal elements to tune the hydrogen adsorption free energy could lead to further improvements in catalytic activity. Here we present a combined theoretical and experimental study to establish ternary pyrite-type cobalt phosphosulphide (CoPS) as a high-performance Earth-abundant catalyst for electrochemical and photoelectrochemical hydrogen production. Nanostructured CoPS electrodes achieved a geometrical catalytic current density of 10 mA cm-2 at overpotentials as low as 48 mV, with outstanding long-term operational stability. Integrated photocathodes of CoPS on n+-p-p+ silicon micropyramids achieved photocurrents up to 35 mA cm-2 at 0 V versus the reversible hydrogen electrode (RHE), onset photovoltages as high as 450 mV versus RHE, and the most efficient solar-driven hydrogen generation from Earth-abundant systems.

  7. Plasma for electrification of chemical industry: a case study on CO2 reduction

    NASA Astrophysics Data System (ADS)

    van Rooij, G. J.; Akse, H. N.; Bongers, W. A.; van de Sanden, M. C. M.

    2018-01-01

    Significant growth of the share of (intermittent) renewable power in the chemical industry is imperative to meet increasingly stricter limits on CO2 exhaust that are being implemented within Europe. This paper aims to evaluate the potential of a plasma process that converts input CO2 into a pure stream of CO to aid in renewable energy penetration in this sector. A realistic process design is constructed to serve as a basis for an economical analysis. The manufacturing cost price of CO is estimated at 1.2 kUS ton-1 CO. A sensitivity analysis shows that separation is the dominant cost factor, so that improving conversion is currently more effective to lower the price than e.g. energy efficiency.

  8. Integration of Photothermal Effect and Heat Insulation to Efficiently Reduce Reaction Temperature of CO2 Hydrogenation.

    PubMed

    Zhang, Wenbo; Wang, Liangbing; Wang, Kaiwen; Khan, Munir Ullah; Wang, Menglin; Li, Hongliang; Zeng, Jie

    2017-02-01

    The photothermal effect is applied in CO 2 hydrogenation to reduce the reaction temperature under illumination by encapsulating Pt nanocubes and Au nanocages into a zeolitic imidazolate framework (ZIF-8). Under illumination, the heat generated by the photothermal effect of Au nanocages is mainly insulated in the ZIF-8 to form a localized high-temperature region, thereby improving the catalytic activity of Pt nanocubes. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  9. CdS/CdSe quantum dots and ZnPc dye co-sensitized solar cells with Au nanoparticles/graphene oxide as efficient modified layer.

    PubMed

    Chen, Cong; Cheng, Yu; Jin, Junjie; Dai, Qilin; Song, Hongwei

    2016-10-15

    Co-sensitization by using two or more sensitizers with complementary absorption spectra to expand the spectral response range is an effective approach to enhance device performance of quantum dot sensitized solar cells (QDSSCs). To improve the light-harvesting in the visible/near-infrared (NIR) region, organic dye zinc phthalocyanine (ZnPc) was combined with CdS/CdSe quantum dots (QDs) for co-sensitized solar cells based on ZnO inverse opals (IOs) as photoanode. The resulting co-sensitized device shows an efficient panchromatic spectral response feature to ∼750nm and presents an overall conversion efficiency of 4.01%, which is superior to that of the individual ZnPc-sensitized solar cells and CdS/CdSe-sensitized solar cells. Meanwhile, an Au nanoparticles/graphene oxide (Au NPs/GO) composite layer was successfully prepared to modify Cu2S counter electrode for the co-sensitized solar cells. Reducing the carrier recombination process by GO and catalytic process of Au NPs leads to increased power conversion efficiency(PCE) from 4.01 to 4.60% and sustainable stability remains ∼85% of its original value after 60min light exposure. In this paper, introduction of the organic dyes as co-sensitizer and Au NPs/GO as counter electrode modified layer has been proved to be an effective route to improve the performance of QDSSCs. Copyright © 2016 Elsevier Inc. All rights reserved.

  10. Boosting Photovoltaic Performance of Dye-Sensitized Solar Cells Using Silver Nanoparticle-Decorated N,S-Co-Doped-TiO2 Photoanode

    PubMed Central

    Lim, Su Pei; Pandikumar, Alagarsamy; Lim, Hong Ngee; Ramaraj, Ramasamy; Huang, Nay Ming

    2015-01-01

    A silver nanoparticle-decorated N,S-co-doped TiO2 nanocomposite was successfully prepared and used as an efficient photoanode in high-performance dye-sensitized solar cells (DSSCs) with N719 dye. The DSSCs assembled with the N,S-TiO2@Ag-modified photoanode demonstrated an enhanced solar-to-electrical energy conversion efficiency of 8.22%, which was better than that of a DSSC photoanode composed of unmodified TiO2 (2.57%) under full sunlight illumination (100 mWcm−2, AM 1.5 G). This enhanced efficiency was mainly attributed to the reduced band gap energy, improved interfacial charge transfer, and retarded charge recombination process. The influence of the Ag content on the overall efficiency was also investigated, and the optimum Ag content with N,S-TiO2 was found to be 20 wt%. Because of the enhanced solar energy conversion efficiency of the N,S-TiO2@Ag nanocomposite, it should be considered as a potential photoanode for high-performance DSSCs. PMID:26146362

  11. Post Waterflood CO2 Miscible Flood in Light Oil, Fluvial-Dominated Deltaic Reservoir, Class I

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Bou-Mikael, Sami

    This report demonstrates the effectiveness of the CO2 miscible process in Fluvial Dominated Deltaic reservoirs. It also evaluated the use of horizontal CO2 injection wells to improve the overall sweep efficiency. A database of FDD reservoirs for the gulf coast region was developed by LSU, using a screening model developed by Texaco Research Center in Houston. The results of the information gained in this project is disseminated throughout the oil industry via a series of SPE papers and industry open forums.

  12. Evaluation and Enhancement of Carbon Dioxide Flooding Through Sweep Improvement

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Hughes, Richard

    2009-09-30

    Carbon dioxide displacement is a common improved recovery method applied to light oil reservoirs (30-45{degrees}API). The economic and technical success of CO{sub 2} floods is often limited by poor sweep efficiency or large CO{sub 2} utilization rates. Projected incremental recoveries for CO{sub 2} floods range from 7% to 20% of the original oil in place; however, actual incremental recoveries range from 9% to 15% of the original oil in place, indicating the potential for significant additional recoveries with improved sweep efficiency. This research program was designed to study the effectiveness of carbon dioxide flooding in a mature reservoir to identifymore » and develop methods and strategies to improve oil recovery in carbon dioxide floods. Specifically, the project has focused on relating laboratory, theoretical and simulation studies to actual field performance in a CO{sub 2} flood in an attempt to understand and mitigate problems of areal and vertical sweep efficiency. In this work the focus has been on evaluating the status of existing swept regions of a mature CO{sub 2} flood and developing procedures to improve the design of proposed floods. The Little Creek Field, Mississippi has been studied through laboratory, theoretical, numerical and simulation studies in an attempt to relate performance predictions to historical reservoir performance to determine sweep efficiency, improve the understanding of the reservoir response to CO{sub 2} injection, and develop scaling methodologies to relate laboratory data and simulation results to predicted reservoir behavior. Existing laboratory information from Little Creek was analyzed and an extensive amount of field data was collected. This was merged with an understanding of previous work at Little Creek to generate a detailed simulation study of two portions of the field – the original pilot area and a currently active part of the field. This work was done to try to relate all of this information to an understanding of where the CO{sub 2} went or is going and how recovery might be improved. New data was also generated in this process. Production logs were run to understand where the CO{sub 2} was entering the reservoir related to core and log information and also to corroborate the simulation model. A methodology was developed and successfully tested for evaluating saturations in a cased-hole environment. Finally an experimental and theoretical program was initiated to relate laboratory work to field scale design and analysis of operations. This work found that an understanding of vertical and areal heterogeneity is crucial for understanding sweep processes as well as understanding appropriate mitigation techniques to improve the sweep. Production and injection logs can provide some understanding of that heterogeneity when core data is not available. The cased-hole saturation logs developed in the project will also be an important part of the evaluation of vertical heterogeneity. Evaluation of injection well/production well connectivities through statistical or numerical techniques were found to be as successful in evaluating CO{sub 2} floods as they are for waterfloods. These are likely to be the lowest cost techniques to evaluate areal sweep. Full field simulation and 4D seismic techniques are other possibilities but were beyond the scope of the project. Detailed simulation studies of pattern areas proved insightful both for doing a “post-mortem” analysis of the pilot area as well as a late-term, active portion of the Little Creek Field. This work also evaluated options for improving sweep in the current flood as well as evaluating options that could have been successful at recovering more oil. That simulation study was successful due to the integration of a large amount of data supplied by the operator as well as collected through the course of the project. While most projects would not have the abundance of data that Little Creek had, integration of the available data continues to be critical for both the design and evaluation stages of CO{sub 2} floods. For cases where data availability is limited, running injection/production logs and/or running cased-hole saturation tools to provide an indication of vertical heterogeneity will be important.« less

  13. Photocatalytic reduction of CO2 to CO over copper decorated g-C3N4 nanosheets with enhanced yield and selectivity

    NASA Astrophysics Data System (ADS)

    Shi, Guodong; Yang, Lin; Liu, Zhuowen; Chen, Xiao; Zhou, Jianqing; Yu, Ying

    2018-01-01

    Photocatalytic reduction of CO2 to fuel has attracted considerable attention due to the consumption of fossil fuels and serious environmental problems. Although there are many photocatalysts reported for CO2 reduction, the improvement of activity and selectivity is still in great need of. In this work, a series of Cu nanoparticle decorated g-C3N4 nanosheets with different Cu loadings were fabricated by a facile secondary calcination and subsequent microwave hydrothermal method. The designed catalysts shown good photocatalytic activity and selectivity for CO2 reduction to CO. The optimal sample exhibited a 3-fold augmentation of the CO yield in comparison with pristine g-C3N4 under visible light. It is revealed that with the loading of Cu nanoparticles, the resulting photocatalyst possessed an improved charge carrier transfer and separation efficiency as well as increased surface reactive sites, resulting in a significant enhancement of CO yield. It is anticipated that the designed Cu/C3N4 photocatalyst may provide new insights for two dimensional layer materials and non-noble particles applied to CO2 reduction.

  14. Effective cellular internalization, cell cycle arrest and improved pharmacokinetics of Tamoxifen by cholesterol based lipopolymeric nanoparticles.

    PubMed

    Mazumdar, Samrat; Italiya, Kishan S; Sharma, Saurabh; Chitkara, Deepak; Mittal, Anupama

    2018-05-30

    The present study aims at the development of cholesterol based lipopolymeric nanoparticles for improved entrapment, better cell penetration and improved pharmacokinetics of Tamoxifen (TMX). Self-assembling cholesterol grafted lipopolymer, mPEG-b-(CB-{g-chol}-co-LA) was synthesized from poly(ethyleneglycol)-block-2-methyl-2-carboxyl-propylenecarboxylic acid-co-poly (l-lactide) [mPEG-b-(CB-{g-COOH}-co-LA)] copolymer followed by carbodiimide coupling for attaching cholesterol. Lipopolymeric nanoparticles were prepared using o/w solvent evaporation technique, which were subsequently characterized to determine its particle size, entrapment efficiency, release pattern and compared with mPEG-PLA nanoparticles. Further, in order to assess the in vitro efficacy, cytotoxicity studies, uptake, apoptosis assay and cell cycle analysis were performed in breast cancer cell lines (MCF-7 and 4T1). Finally, the pharmacokinetic profile of TMX loaded mPEG-b-(CB-{g-chol}-co-LA) lipopolymeric nanoparticles was also performed. TMX loaded lipopolymeric nanoparticles of particle size 151.25 ± 3.74 (PDI 0.123) and entrapment efficiency of 73.62 ± 3.08% were formulated. The haemolytic index, protein binding and in vitro drug release of the optimized nanoparticles were found to be comparable to that of the TMX loaded mPEG-PLA nanoparticles. Lipopolymeric nanoparticles demonstrated improved IC 50 values in breast cancer cells (22.2 μM in 4T1; 18.8 μM in MCF-7) than free TMX (27.6 μM and 23.5 μM respectively) and higher uptake efficiency. At IC 50 values, TMX loaded lipopolymeric nanoparticles induced apoptosis and cell cycle arrest (G 0 /G 1 phase) to similar extent as that of free drug. Pharmacokinetic studies indicated ∼2.5-fold increase in the half-life (t 1/2 ) (p < 0.001) and ∼2.7-fold (p < 0.001) increase in the mean residence time (MRT) of TMX following incorporation into lipopolymeric nanoparticles. Thus, mPEG-b-(CB-{g-chol}-co-LA) lipopolymeric nanoparticles offer a more promising approach for delivery of Tamoxifen in breast cancer by improving drug internalization and prolonging the mean residence time of the drug indicating possibility of dose reduction and hence bypassing the adverse effects of TMX therapy. Copyright © 2018 Elsevier B.V. All rights reserved.

  15. In Situ-Grown ZnCo2O4 on Single-Walled Carbon Nanotubes as Air Electrode Materials for Rechargeable Lithium–Oxygen Batteries

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Liu, Bin; Xu, Wu; Yan, Pengfei

    2015-10-12

    Although lithium-oxygen (Li-O2) batteries have great potential to be used as one of the next generation energy storage systems due to their ultrahigh theoretical specific energy, there are still many significant barriers before their practical applications. These barriers include electrolyte and electrode instability, poor ORR/OER efficiency and cycling capability, etc. Development of a highly efficient catalyst will not only enhance ORR/OER efficiency, it may also improve the stability of electrolyte because the reduced charge voltage. Here we report the synthesis of nano-sheet-assembled ZnCo2O4 spheres/single walled carbon nanotubes (ZCO/SWCNTs) composites as high performance air electrode materials for Li-O2 batteries. The ZCOmore » catalyzed SWCNTs electrodes delivered high discharge capacities, decreased the onset of oxygen evolution reaction by 0.9 V during charge processes, and led to more stable cycling stability. These results indicate that ZCO/SWCNTs composite can be used as highly efficient air electrode for oxygen reduction and evolution reactions. The highly enhanced catalytic activity by uniformly dispersed ZnCo2O4 catalyst on nanostructured electrodes is expected to inspire« less

  16. Development of an advanced Sabatier CO2 reduction subsystem

    NASA Technical Reports Server (NTRS)

    Kleiner, G. N.; Cusick, R. J.

    1981-01-01

    A preprototype Sabatier CO2 reduction subsystem was successfully designed, fabricated and tested. The lightweight, quick starting (less than 5 minutes) reactor utlizes a highly active and physically durable methanation catalyst composed of ruthenium on alumina. The use of this improved catalyst permits a simple, passively controlled reactor design with an average lean component H2/CO2 conversion efficiency of over 99% over a range of H2/CO2 molar ratios of 1.8 to 5 while operating with process flows equivalent to a crew size of up to five persons. The subsystem requires no heater operation after start-up even during simulated 55 minute lightside/39 minute darkside orbital operation.

  17. Efficient co-delivery of immiscible hydrophilic/hydrophobic chemotherapeutics by lipid emulsions for improved treatment of cancer

    PubMed Central

    Zhang, Bo; Song, Yunmei; Wang, Tianqi; Yang, Shaomei; Zhang, Jing; Liu, Yongjun; Zhang, Na; Garg, Sanjay

    2017-01-01

    Combinational nanomedicine is becoming a topic of much interest in cancer therapy, although its translation into the clinic remains extremely challenging. One of the main obstacles lies in the difficulty to efficiently co-deliver immiscible hydrophilic/hydrophobic drugs into tumor sites. The aim of this study was to develop co-loaded lipid emulsions (LEs) to co-deliver immiscible hydrophilic/hydrophobic drugs to improve cancer therapy and to explore the co-delivery abilities between co-loaded LEs and mixture formulation. Multiple oxaliplatin/irinotecan drug–phospholipid complexes (DPCs) were formulated. Co-loaded LEs were prepared using DPC technique to efficiently encapsulate both drugs. Co-loaded LEs exhibited uniform particle size distribution, desired stability and synchronous release profiles in both drugs. Co-loaded LEs demonstrated superior anti-tumor activity compared with the simple solution mixture and the mixture of single-loaded LEs. Furthermore, co-loaded nanocarriers could co-deliver both drugs into the same cells more efficiently and exhibited the optimized synergistic effect. These results indicate that co-loaded LEs could be a desired formulation for enhanced cancer therapy with potential application prospects. The comparison between co-loaded LEs and mixture formulation is significant for pharmaceutical designs aimed at co-delivery of multiple drugs. PMID:28435264

  18. Efficient co-delivery of immiscible hydrophilic/hydrophobic chemotherapeutics by lipid emulsions for improved treatment of cancer.

    PubMed

    Zhang, Bo; Song, Yunmei; Wang, Tianqi; Yang, Shaomei; Zhang, Jing; Liu, Yongjun; Zhang, Na; Garg, Sanjay

    2017-01-01

    Combinational nanomedicine is becoming a topic of much interest in cancer therapy, although its translation into the clinic remains extremely challenging. One of the main obstacles lies in the difficulty to efficiently co-deliver immiscible hydrophilic/hydrophobic drugs into tumor sites. The aim of this study was to develop co-loaded lipid emulsions (LEs) to co-deliver immiscible hydrophilic/hydrophobic drugs to improve cancer therapy and to explore the co-delivery abilities between co-loaded LEs and mixture formulation. Multiple oxaliplatin/irinotecan drug-phospholipid complexes (DPCs) were formulated. Co-loaded LEs were prepared using DPC technique to efficiently encapsulate both drugs. Co-loaded LEs exhibited uniform particle size distribution, desired stability and synchronous release profiles in both drugs. Co-loaded LEs demonstrated superior anti-tumor activity compared with the simple solution mixture and the mixture of single-loaded LEs. Furthermore, co-loaded nanocarriers could co-deliver both drugs into the same cells more efficiently and exhibited the optimized synergistic effect. These results indicate that co-loaded LEs could be a desired formulation for enhanced cancer therapy with potential application prospects. The comparison between co-loaded LEs and mixture formulation is significant for pharmaceutical designs aimed at co-delivery of multiple drugs.

  19. CoCoNUT: an efficient system for the comparison and analysis of genomes

    PubMed Central

    2008-01-01

    Background Comparative genomics is the analysis and comparison of genomes from different species. This area of research is driven by the large number of sequenced genomes and heavily relies on efficient algorithms and software to perform pairwise and multiple genome comparisons. Results Most of the software tools available are tailored for one specific task. In contrast, we have developed a novel system CoCoNUT (Computational Comparative geNomics Utility Toolkit) that allows solving several different tasks in a unified framework: (1) finding regions of high similarity among multiple genomic sequences and aligning them, (2) comparing two draft or multi-chromosomal genomes, (3) locating large segmental duplications in large genomic sequences, and (4) mapping cDNA/EST to genomic sequences. Conclusion CoCoNUT is competitive with other software tools w.r.t. the quality of the results. The use of state of the art algorithms and data structures allows CoCoNUT to solve comparative genomics tasks more efficiently than previous tools. With the improved user interface (including an interactive visualization component), CoCoNUT provides a unified, versatile, and easy-to-use software tool for large scale studies in comparative genomics. PMID:19014477

  20. Electrocatalytic activity of cobalt phosphide-modified graphite felt toward VO2+/VO2+ redox reaction

    NASA Astrophysics Data System (ADS)

    Ge, Zhijun; Wang, Ling; He, Zhangxing; Li, Yuehua; Jiang, Yingqiao; Meng, Wei; Dai, Lei

    2018-04-01

    A novel strategy for improving the electro-catalytic properties of graphite felt (GF) electrode in vanadium redox flow battery (VRFB) is designed by depositing cobalt phosphide (CoP) onto GF surface. The CoP powder is synthesized by direct carbonization of Co-based zeolitic imidazolate framework (ZIF-67) followed by phosphidation. Cyclic voltammetry results confirm that the CoP-modified graphite felt (GF-CoP) electrode has excellent reversibility and electro-catalytic activity to the VO2+/VO2+ cathodic reaction compared with the pristine GF electrode. The cell using GF-CoP electrode shows apparently higher discharge capacity over that based on GF electrode. The cell using GF-CoP electrode has the capacity of 67.2 mA h at 100 mA cm-2, 32.7 mA h larger than that using GF electrode. Compared with cell using GF electrode, the voltage efficiency of the cell based on GF-CoP electrode increases by 5.9% and energy efficiency by 5.4% at a current density of 100 mA cm-2. The cell using GF-CoP electrode can reach 94.31% capacity retention after 50 cycles at a current density of 30 mA cm-2. The results show that the CoP can effectively promote the VO2+/VO2+ redox reaction, implying that metal phosphides are a new kind of potential catalytic materials for VRFB.

  1. Effect of Electric Field on CO2 Photoreduction by TiO2 Film

    NASA Astrophysics Data System (ADS)

    Huang, Zhengfeng; Cheng, Xudong; Dong, Peimei; Zhang, Xiwen

    2017-02-01

    To mitigate the greenhouse effect, many studies have been carried out to improve the CO2 conversion efficiency of TiO2. Modification of TiO2 has been intensively investigated, but the influence of an electric field on photoreduction by this material remains largely unknown. Accordingly, in this study, we explored the effect of an electric field on the photoreduction process using a porous TiO2-Ti material. The results indicated that the CO yield improved 85-fold (equivalent to 4772 μmol/g h) when a 30-kV voltage was applied during the reduction process. To make the electric field effect fully functional, we also explored the effect of water on the photoreduction process, finding that TiO2 showed the highest conversion rate when the humidity was controlled at 50% relative humidity (RH).

  2. Energy efficiency and reduction of CO2 emissions from campsites management in a protected area.

    PubMed

    Del Moretto, Deny; Branca, Teresa Annunziata; Colla, Valentina

    2018-09-15

    Campsites can be a pollution source, mainly due to the energy consumption. In addition, the green areas, thanks to the direct CO 2 sequestration and the shading, indirectly prevent the CO 2 emissions related to energy consumption. The methodology presented in this paper allowed assessing the annual CO 2 emissions directly related to the campsite management and the consequent environmental impact in campsite clusters in Tuscany. The software i-Tree Canopy was exploited, enabling to evaluate in terms of "canopy" the tonnes of CO 2 sequestered by the vegetation within each campsite. Energy and water consumptions from 2012 to 2015 were assessed for each campsite. As far as the distribution of sequestered CO 2 is concerned, the campsites ranking was in accordance to their size. According to the indicator "T-Tree" or canopy cover, a larger area of the canopy cover allows using less outdoor areas covered by trees for the sequestration of the remaining amount of pollutants. The analysis shows that the considered campsites, that are located in a highly naturalistic Park, present significant positive aspects both in terms of CO 2 emission reductions and of energy efficiency. However, significant margins of improvement are also possible and they were analysed in the paper. Copyright © 2018 Elsevier Ltd. All rights reserved.

  3. Variation among soybean cultivars in mesophyll conductance and leaf water use efficiency

    USDA-ARS?s Scientific Manuscript database

    Improving water use efficiency (WUE) may prove a useful way to adapt crop species to drought. Since the recognition of the importance of mesophyll conductance to CO2 movement from inside stomatal pores to the sites of photosynthetic carboxylation, there has been interest in how much intraspecific v...

  4. CdS/CdSe co-sensitized SnO2 photoelectrodes for quantum dots sensitized solar cells

    NASA Astrophysics Data System (ADS)

    Lin, Yibing; Lin, Yu; Meng, Yongming; Tu, Yongguang; Zhang, Xiaolong

    2015-07-01

    SnO2 nanoparticles were synthesized by hydrothermal method and applied to photo-electrodes of quantum dots-sensitized solar cells (QDSSCs). After sensitizing SnO2 films via CdS quantum dots, CdSe quantum dots was decorated on the surface of CdS/SnO2 photo-electrodes to further improve the power conversion efficiency. CdS and CdSe quantum dots were deposited by successive ionic layer absorption and reaction method (SILAR) and chemical bath deposition method (CBD) respectively. Scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray diffraction (XRD) were used to identify the surface profile and crystal structure of SnO2 photo-electrodes before and after deposited quantum dots. After CdSe co-sensitized process, an overall power conversion efficiency of 1.78% was obtained in CdSe/CdS/SnO2 QDSSC, which showed 66.4% improvement than that of CdS/SnO2 QDSSC.

  5. Efficient electrolyzer for CO2 splitting in neutral water using earth-abundant materials.

    PubMed

    Tatin, Arnaud; Comminges, Clément; Kokoh, Boniface; Costentin, Cyrille; Robert, Marc; Savéant, Jean-Michel

    2016-05-17

    Low-cost, efficient CO2-to-CO+O2 electrochemical splitting is a key step for liquid-fuel production for renewable energy storage and use of CO2 as a feedstock for chemicals. Heterogeneous catalysts for cathodic CO2-to-CO associated with an O2-evolving anodic reaction in high-energy-efficiency cells are not yet available. An iron porphyrin immobilized into a conductive Nafion/carbon powder layer is a stable cathode producing CO in pH neutral water with 90% faradaic efficiency. It is coupled with a water oxidation phosphate cobalt oxide anode in a home-made electrolyzer by means of a Nafion membrane. Current densities of approximately 1 mA/cm(2) over 30-h electrolysis are achieved at a 2.5-V cell voltage, splitting CO2 and H2O into CO and O2 with a 50% energy efficiency. Remarkably, CO2 reduction outweighs the concurrent water reduction. The setup does not prevent high-efficiency proton transport through the Nafion membrane separator: The ohmic drop loss is only 0.1 V and the pH remains stable. These results demonstrate the possibility to set up an efficient, low-voltage, electrochemical cell that converts CO2 into CO and O2 by associating a cathodic-supported molecular catalyst based on an abundant transition metal with a cheap, easy-to-prepare anodic catalyst oxidizing water into O2.

  6. [Effects of CO2 fertilization on photosynthesis and growth of cut Anthurium andraeanum in solar greenhouse in winter].

    PubMed

    Yang, Ke Bin; Meng, Fan Zhi; Guo, Xian Feng

    2017-06-18

    Aiming at the problem of the acute shortage of CO 2 in winter production of cut Anthurium andraeanum in solar greenhouse, the effect of CO 2 fertilization on photosynthetic characteristics and growth performance of A. andraeanum 'Fire' was investigated. Three treatments with different concentrations of CO 2 were designed, i.e., 700, 1000 and 1300 Μmol·mol -1 , with receiving no extra CO 2 as the control. The results showed that for the CO 2 -fertilized plants, the photosynthetic rate, intercellular CO 2 concentration and water use efficiency were significantly greater than those in the control plants after CO 2 fertilization for 60 days, and the largest increase range was observed in the 1000 Μmol·mol -1 CO 2 treatment, whereas the stomata conductance was significantly reduced compared with the control. Meanwhile, the contents of soluble sugar, starch and soluble protein in CO 2 -fertilized plants were significantly higher than those in control plants. Moreover, the quality of cut flowers with CO 2 fertilization was remarkably superior to control flowers in term of the parameters including spathe size, spathe color, peduncle length, leaf growth performance and peduncle growth rate. The most superior improvement was observed in the 1000 Μmol·mol -1 CO 2 treatment. It was therefore concluded that CO 2 fertilization of 1000 Μmol·mol -1 could effectively improve the winter production of cut A. andraeanum in solar greenhouse.

  7. Pilot-Scale Silicone Process for Low-Cost Carbon Dioxide Capture. Final Scientific/Technical Report

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Hancu, Dan; Wood, Benjamin; Genovese, Sarah

    GE Global Research has developed, over the last 8 years, a platform of cost effective CO 2 capture technologies based on a non-aqueous aminosilicone solvent (GAP-1m). As demonstrated in a previous funded DOE project (DE-FE0007502), the GAP-1m solvent has increased CO 2 working capacity, lower volatility and corrosivity than the benchmark aqueous amine technology. The current report describes the cooperative program between GE Global Research (GE GRC), and the National Carbon Capture Center (NCCC) to design, construct, and operate a pilot-scale process using GAP-1m solvent to demonstrate its performance at 0.5 MWe. (i) Performance of the GAP-1m solvent was demonstratedmore » in a 0.5 MWe pilot with real flue gas for over 900 hrs. of operation using two alternative desorption designs: a Continuous Stirred Tank Reactor (CSTR), and a Steam Stripper Column (SSC). The CSTR is a one-stage separation unit with reduced space requirements, and capital cost. The alternative is a multi-stage separation column, with improved desorption efficiency. Testing the two desorber options allowed us to identify the most cost effective, and space efficient desorber solution. (ii) CSTR Campaign: The CSTR desorber unit was designed, fabricated and integrated with the pilot solvent test unit (PSTU), replacing the PSTU Steam Stripper Column at NCCC. Solvent management and waste water special procedures were implemented to accommodate operation of the non-aqueous solvent in the PSTU. Performance of the GAP-1m solvent with the CSTR was demonstrated for over 500 hrs. while varying temperature of the desorption (230 – 265 oF), solvent circulation rate (GAP-1m : CO 2 (molar) = 1.5 – 4), and flue gas flow rates (0.2 – 0.5 MWe). Solvent carry-over in the CO 2 product was minimized by maintaining water content below 5 wt.%, and desorption pressure at 7 psig. CO 2 capture efficiency achieved was 95% at 0.25 MWe (GAP-1m : CO 2 = 4 (molar), 230 oF desorption), and 65% at 0.5 MWe (GAP-1m : CO 2 (molar) = 1.5, 248 oF). Solvent loss was dominated by thermal degradation of the rich solvent. (iii) Steam Stripper Column Campaign: Higher expected cost of the solvent vs. aqueous amines makes solvent management a top priority to maintain the low cost for the process. During the testing of the GAP-1m solvent with the CSTR, thermal degradation of the rich solvent was found to be the main mechanism in solvent loss. Small amounts of water in the working solution were found to be an effective way to enable steam stripping, thereby lowering desorption temperature, and hence reducing thermal degradation. Steam stripping also increased working capacity by 30% due to a more efficient desorption. The concept was first tested in a glass stripping column (lab scale, GE GRC), optimized in a continuous bench scale system (2 kWe, GE GRC), and demonstrated in a 0.5 MWe PSTU at NCCC. No special system modifications were required to the PSTU to accommodate the testing of the non-aqueous GAP-1 solvent with the regenerator column. SSC was found to be more robust towards solvent entrainment (H 2O < 35 wt.%). 90 – 95% CO 2 capture efficiency was achieved under stoichiometric conditions at 0.5 MWe (235 oF desorption, 2 psig and 19 wt. % H 2O). Both CO 2 capture efficiency and specific duty reached optimum conditions at 18 wt.% H 2O. Low amine degradation (< 0.05 wt.%/day) was recorded over 350 hrs. of operation. Controlled water addition to GAP-1m solvent decreased the desorption temperature, thermal degradation, and improved the CO 2 working capacity due to more efficient absorption and desorption processes. Under these conditions, the GAP-1m solvent exhibited a 25% increased working capacity, and 10% reduction in specific steam duty vs. MEA, at 10 oF lower desorption temperature. (iv) Techno-economic Analysis: The pilot-scale PSTU engineering data were used to update the capture system process models, and the techno-economic analysis was performed for a 550 MW coal fired power plant. The 1st year CO 2 removal cost for the aminosilicone-based carbon-capture process was evaluated at $48/ton CO 2 using the steam stripper column. This is a 20% reduction compared to MEA, primarily due to lower overall capital cost. CO 2 cost using the CSTR desorber is dominated by the economics of the solvent make-up. The steam stripper desorber is the preferred unit operation due to a more efficient desorption, and reduced solvent make-up rate. Further reduction in CO 2 capture cost is expected by lowering the manufacturing cost of the solvent, implementing flowsheet optimization and/or implementing the next generation aminosilicone solvent with improved stability and increased CO 2 working capacity.« less

  8. CoP/WS2 nanoflake heterostructures as efficient electrocatalysts for significant improvement in hydrogen evolution activity

    NASA Astrophysics Data System (ADS)

    Chen, Yajie; Kang, Chuanhong; Wang, Ruihong; Ren, Zhiyu; Fu, Huiying; Xiao, Yuting; Tian, Guohui

    2018-06-01

    The CoP/WS2 nanoflake composites were synthesized via the sulfuration and subsequent phosphidation using the pre-prepared WO2.72 nanowires as precursors. Originally, WO2.72 nanowires were prepared and followed by sulfuration to obtain WS2 nanoflakes. The as-prepared WS2 nanoflakes were used as substrates, on which the Co3O4 nanoparticles were uniformly anchored to construct the Co3O4/WS2 nanoflakes. Finally, the Co3O4/WS2 composites were subjected to phosphidation and in-situ converted into CoP/WS2 nanoflakes. Because of the dual functionalities of both CoP and WS2, the abundant interfaces as well as their synergy, the CoP/WS2 nanoflakes exhibited much higher electrocatalytic activity, smaller overpotential (-81 mV), lower Tafel slope (62 mV decade-1), and higher stability toward hydrogen-evolution reaction than those for the single CoP and WS2.

  9. Oxidatively-Stable Linear Poly(propylenimine)-Containing Adsorbents for CO2 Capture from Ultra-Dilute Streams.

    PubMed

    Pang, Simon H; Lively, Ryan P; Jones, Christopher W

    2018-05-29

    Aminopolymer-based solid sorbents have been widely investigated for CO2 capture from dilute streams such as flue gas or ambient air. However, the oxidative stability of the most well-studied aminopolymer, poly(ethylenimine) (PEI), is limited, causing it to lose its CO2 capture capacity after exposure to oxygen at elevated temperatures. Here we demonstrate the use of linear poly(propylenimine) (PPI), synthesized via a simple cationic ring-opening polymerization, as a more oxidatively-stable alternative to PEI with high CO2 capacity and amine efficiency. The performance of linear PPI/SBA-15 composites is investigated over a range of CO2 capture conditions (CO2 partial pressure, adsorption temperature) to examine the trade-off between adsorption capacity and sorption site accessibility, which may be expected to be more limited in linear polymers relative to the prototypical hyperbranched PEI. Linear PPI/SBA-15 composites are more efficient at CO2 capture and retain 65-83% of their CO2 capacity after exposure to a harsh oxidative treatment, compared to 20-40% retention for linear PEI. Additionally, we demonstrate long-term stability of linear PPI sorbents over 50 adsorption/desorption cycles with no loss in performance. Combined with other strategies for improving oxidative stability and adsorption kinetics, linear PPI may play a role as a component of stable, solid adsorbents in commercial applications for CO2 capture. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  10. Presidential Green Chemistry Challenge: 2004 Academic Award

    EPA Pesticide Factsheets

    Presidential Green Chemistry Challenge 2004 award winners, Professors Charles A. Eckert and Charles L. Liotta, use supercritical CO2 as a solvent to combine reactions and separations, improve efficiency, and reduce waste.

  11. Visible-light-driven N-(BiO)2CO3/Graphene oxide composites with improved photocatalytic activity and selectivity for NOx removal

    NASA Astrophysics Data System (ADS)

    Chen, Meijuan; Huang, Yu; Yao, Jie; Cao, Jun-ji; Liu, Yuan

    2018-02-01

    N-doped (BiO)2CO3 (NBOC)/graphene oxide (GO) composite obtained from three-dimensional hierarchical microspheres is successfully synthesized by one-pot hydrothermal method for the first time. In this synthesis, citrate ion plays a critical role in N doping. The obtained samples are used to degrade gaseous nitrogen oxides (NOx) at parts-per-billion (ppb) level under visible-light irradiation. NBOC-GO composite with 1.0 wt% graphene oxide (GO) displays the highest photocatalytic NO removal efficiency, which is 4.3 times higher than that of pristine (BiO)2CO3. Moreover, NBOC-GO composite significantly inhibits toxic NO2 intermediate production, indicating its high selectivity for NO conversion. Compared with regular GO, N doping considerably improves the catalytic performance of NBOC-GO composite, which increases NO removal by 74.6% and fully inhibits NO2 generation. The improved photocatalytic activity is mainly ascribed to extended optical absorption ability and enhanced separation efficiency of photogenerated charge carriers over NBOC-GO composite. Both results of electron spin resonance and theoretical analysis of band structure indicate that NO removal is dominated by oxidation with rad OH and rad O2- radicals. The photocatalytic activity improvement mechanism over the NBOC-GO composite is proposed accordingly based on systematic characterizations. This study demonstrates a feasible route to fabricating Bi-containing composites with high selectivity and stability for air pollution control and provides a new insight into the associated photocatalytic mechanisms.

  12. Elevated CO2 does not offset greater water stress predicted under climate change for native and exotic riparian plants

    USGS Publications Warehouse

    Perry, Laura G.; Shafroth, Patrick B.; Blumenthal, Dana M.; Morgan, Jack A.; LeCain, Daniel R.

    2013-01-01

    In semiarid western North American riparian ecosystems, increased drought and lower streamflows under climate change may reduce plant growth and recruitment, and favor drought-tolerant exotic species over mesic native species. We tested whether elevated atmospheric CO2 might ameliorate these effects by improving plant water-use efficiency. We examined the effects of CO2 and water availability on seedlings of two native (Populus deltoids spp. monilifera, Salix exigua) and three exotic (Elaeagnus angustifolia, Tamarix spp., Ulmus pumila) western North American riparian species in a CO2-controlled glasshouse, using 1-m-deep pots with different water-table decline rates. Low water availability reduced seedling biomass by 70–97%, and hindered the native species more than the exotics. Elevated CO2 increased biomass by 15%, with similar effects on natives and exotics. Elevated CO2 increased intrinsic water-use efficiency (Δ13Cleaf), but did not increase biomass more in drier treatments than wetter treatments. The moderate positive effects of elevated CO2 on riparian seedlings are unlikely to counteract the large negative effects of increased aridity projected under climate change. Our results suggest that increased aridity will reduce riparian seedling growth despite elevated CO2, and will reduce growth more for native Salix and Populus than for drought-tolerant exotic species.

  13. Elevated CO2 does not offset greater water stress predicted under climate change for native and exotic riparian plants

    USGS Publications Warehouse

    Perry, Laura G.; Shafroth, Patrick B.; Blumenthal, Dana M.; Morgan, Jack A.; LeCain, Daniel R.

    2013-01-01

    * In semiarid western North American riparian ecosystems, increased drought and lower streamflows under climate change may reduce plant growth and recruitment, and favor drought-tolerant exotic species over mesic native species. We tested whether elevated atmospheric CO2 might ameliorate these effects by improving plant water-use efficiency. * We examined the effects of CO2 and water availability on seedlings of two native (Populus deltoides spp. monilifera, Salix exigua) and three exotic (Elaeagnus angustifolia, Tamarix spp., Ulmus pumila) western North American riparian species in a CO2-controlled glasshouse, using 1-m-deep pots with different water-table decline rates. * Low water availability reduced seedling biomass by 70–97%, and hindered the native species more than the exotics. Elevated CO2 increased biomass by 15%, with similar effects on natives and exotics. Elevated CO2 increased intrinsic water-use efficiency (Δ13Cleaf), but did not increase biomass more in drier treatments than wetter treatments. * The moderate positive effects of elevated CO2 on riparian seedlings are unlikely to counteract the large negative effects of increased aridity projected under climate change. Our results suggest that increased aridity will reduce riparian seedling growth despite elevated CO2, and will reduce growth more for native Salix and Populus than for drought-tolerant exotic species.

  14. Lattice Boltzmann simulations of supercritical CO2-water drainage displacement in porous media: CO2 saturation and displacement mechanism.

    PubMed

    Yamabe, Hirotatsu; Tsuji, Takeshi; Liang, Yunfeng; Matsuoka, Toshifumi

    2015-01-06

    CO2 geosequestration in deep aquifers requires the displacement of water (wetting phase) from the porous media by supercritical CO2 (nonwetting phase). However, the interfacial instabilities, such as viscous and capillary fingerings, develop during the drainage displacement. Moreover, the burstlike Haines jump often occurs under conditions of low capillary number. To study these interfacial instabilities, we performed lattice Boltzmann simulations of CO2-water drainage displacement in a 3D synthetic granular rock model at a fixed viscosity ratio and at various capillary numbers. The capillary numbers are varied by changing injection pressure, which induces changes in flow velocity. It was observed that the viscous fingering was dominant at high injection pressures, whereas the crossover of viscous and capillary fingerings was observed, accompanied by Haines jumps, at low injection pressures. The Haines jumps flowing forward caused a significant drop of CO2 saturation, whereas Haines jumps flowing backward caused an increase of CO2 saturation (per injection depth). We demonstrated that the pore-scale Haines jumps remarkably influenced the flow path and therefore equilibrium CO2 saturation in crossover domain, which is in turn related to the storage efficiency in the field-scale geosequestration. The results can improve our understandings of the storage efficiency by the effects of pore-scale displacement phenomena.

  15. Electrocatalytic reduction of CO2 with CCC-NHC pincer nickel complexes.

    PubMed

    Cope, James D; Liyanage, Nalaka P; Kelley, Paul J; Denny, Jason A; Valente, Edward J; Webster, Charles Edwin; Delcamp, Jared H; Hollis, T Keith

    2017-08-22

    A CCC-NHC pincer Ni(ii)Cl complex was prepared according to the metallation/transmetallation methodology. It was fully characterized by electrochemical, NMR spectroscopic, theoretical, and X-ray crystallographic methods. The complex and its cation were evaluated for electrocatalytic reduction of CO 2 under a variety of conditions and found to provide some of the fastest catalytic rates and highest substrate selectivities (CO 2 vs. H + ) reported. Rates improved in the presence of water and, significantly, catalysis occurred at the first reduction potential, presumably at the Ni(i) state. Controlled potential electrolysis (CPE) was found to yield CO at 34% and formate at 47% Faradaic efficiency (FE).

  16. Synthesis of Mesoporous Co2+-Doped TiO2 Nanodisks Derived from Metal Organic Frameworks with Improved Sodium Storage Performance.

    PubMed

    Hong, Zhensheng; Kang, Meiling; Chen, Xiaohui; Zhou, Kaiqiang; Huang, Zhigao; Wei, Mingdeng

    2017-09-20

    TiO 2 is a most promising anode candidate for rechargeable Na-ion batteries (NIBs) because of its appropriate working voltage, low cost, and superior structural stability during chage/discharge process. Nevertheless, it suffers from intrinsically low electrical conductivity. Herein, we report an in situ synthesis of Co 2+ -doped TiO 2 through the thermal treatment of metal organic frameworks precursors of MIL-125(Ti)-Co as a superior anode material for NIBs. The Co 2+ -doped TiO 2 possesses uniform nanodisk morphology, a large surface area and mesoporous structure with narrow pore distribution. The reversible capacity, Coulombic efficiency (CE) and rate capability can be improved by Co 2+ doping in mesoporous TiO 2 anode. Co 2+ -doped mesoporous TiO 2 nanodisks exhibited a high reversible capacity of 232 mAhg -1 at 0.1 Ag 1- , good rate capability and cycling stability with a stable capacity of about 140 mAhg -1 at 0.5 Ag 1- after 500 cycles. The enhanced Na-ion storage performance could be due to the increased electrical conductivity revealed by Kelvin probe force microscopy measurements.

  17. Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption

    NASA Astrophysics Data System (ADS)

    Zheng, Xueli; Zhang, Bo; de Luna, Phil; Liang, Yufeng; Comin, Riccardo; Voznyy, Oleksandr; Han, Lili; García de Arquer, F. Pelayo; Liu, Min; Dinh, Cao Thang; Regier, Tom; Dynes, James J.; He, Sisi; Xin, Huolin L.; Peng, Huisheng; Prendergast, David; Du, Xiwen; Sargent, Edward H.

    2018-02-01

    The efficiency with which renewable fuels and feedstocks are synthesized from electrical sources is limited at present by the sluggish oxygen evolution reaction (OER) in pH-neutral media. We took the view that generating transition-metal sites with high valence at low applied bias should improve the activity of neutral OER catalysts. Here, using density functional theory, we find that the formation energy of desired Ni4+ sites is systematically modulated by incorporating judicious combinations of Co, Fe and non-metal P. We therefore synthesized NiCoFeP oxyhydroxides and probed their oxidation kinetics with in situ soft X-ray absorption spectroscopy (sXAS). In situ sXAS studies of neutral-pH OER catalysts indicate ready promotion of Ni4+ under low overpotential conditions. The NiCoFeP catalyst outperforms IrO2 and retains its performance following 100 h of operation. We showcase NiCoFeP in a membrane-free CO2 electroreduction system that achieves a 1.99 V cell voltage at 10 mA cm-2, reducing CO2 into CO and oxidizing H2O to O2 with a 64% electricity-to-chemical-fuel efficiency.

  18. Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption

    DOE PAGES

    Zheng, Xueli; Zhang, Bo; De Luna, Phil; ...

    2017-11-20

    The efficiency with which renewable fuels and feedstocks are synthesized from electrical sources is limited at present by the sluggish oxygen evolution reaction (OER) in pH-neutral media. Here, we took the view that generating transition metal sites with high valence at low applied bias should improve the activity of neutral OER catalysts. Using density functional theory, we find that the formation energy of desired Ni 4+ sites is systematically modulated by incorporating judicious combinations of Co, Fe and non-metal phosphorus. Here we synthesized NiCoFeP oxyhydroxides and probed their oxidation kinetics by employing in situ soft X-ray absorption (sXAS). In situmore » sXAS studies of neutral-pH OER catalysts indicate ready promotion of Ni 4+ under low overpotential conditions. NiCoFeP catalyst outperforms IrO 2 and retains its performance following 100 hours of operation. We showcase NiCoFeP in a membrane-free CO 2 electroreduction system that achieves a 1.99 V cell voltage at 10 mA cm -2, reducing CO 2 into CO and oxidizing H 2O to O 2 with a 64% electricity-to-chemical-fuel efficiency.« less

  19. Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Zheng, Xueli; Zhang, Bo; De Luna, Phil

    The efficiency with which renewable fuels and feedstocks are synthesized from electrical sources is limited at present by the sluggish oxygen evolution reaction (OER) in pH-neutral media. Here, we took the view that generating transition metal sites with high valence at low applied bias should improve the activity of neutral OER catalysts. Using density functional theory, we find that the formation energy of desired Ni 4+ sites is systematically modulated by incorporating judicious combinations of Co, Fe and non-metal phosphorus. Here we synthesized NiCoFeP oxyhydroxides and probed their oxidation kinetics by employing in situ soft X-ray absorption (sXAS). In situmore » sXAS studies of neutral-pH OER catalysts indicate ready promotion of Ni 4+ under low overpotential conditions. NiCoFeP catalyst outperforms IrO 2 and retains its performance following 100 hours of operation. We showcase NiCoFeP in a membrane-free CO 2 electroreduction system that achieves a 1.99 V cell voltage at 10 mA cm -2, reducing CO 2 into CO and oxidizing H 2O to O 2 with a 64% electricity-to-chemical-fuel efficiency.« less

  20. Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption.

    PubMed

    Zheng, Xueli; Zhang, Bo; De Luna, Phil; Liang, Yufeng; Comin, Riccardo; Voznyy, Oleksandr; Han, Lili; García de Arquer, F Pelayo; Liu, Min; Dinh, Cao Thang; Regier, Tom; Dynes, James J; He, Sisi; Xin, Huolin L; Peng, Huisheng; Prendergast, David; Du, Xiwen; Sargent, Edward H

    2018-02-01

    The efficiency with which renewable fuels and feedstocks are synthesized from electrical sources is limited at present by the sluggish oxygen evolution reaction (OER) in pH-neutral media. We took the view that generating transition-metal sites with high valence at low applied bias should improve the activity of neutral OER catalysts. Here, using density functional theory, we find that the formation energy of desired Ni 4+ sites is systematically modulated by incorporating judicious combinations of Co, Fe and non-metal P. We therefore synthesized NiCoFeP oxyhydroxides and probed their oxidation kinetics with in situ soft X-ray absorption spectroscopy (sXAS). In situ sXAS studies of neutral-pH OER catalysts indicate ready promotion of Ni 4+ under low overpotential conditions. The NiCoFeP catalyst outperforms IrO 2 and retains its performance following 100 h of operation. We showcase NiCoFeP in a membrane-free CO 2 electroreduction system that achieves a 1.99 V cell voltage at 10 mA cm -2 , reducing CO 2 into CO and oxidizing H 2 O to O 2 with a 64% electricity-to-chemical-fuel efficiency.

  1. Supercritical carbon dioxide design strategies: from drug carriers to soft killers.

    PubMed

    Aguiar-Ricardo, Ana; Bonifácio, Vasco D B; Casimiro, Teresa; Correia, Vanessa G

    2015-12-28

    The integrated use of supercritical carbon dioxide (scCO(2)) and micro- and nanotechnologies has enabled new sustainable strategies for the manufacturing of new medications. 'Green' scCO(2)-based methodologies are well suited to improve either the synthesis or materials processing leading to the assembly of three-dimensional multifunctional constructs. By using scCO(2) either as C1 feedstock or as solvent, simple, economic, efficient and clean routes can be designed to synthesize materials with unique properties such as polyurea dendrimers and oxazoline-based polymers/oligomers. These new biocompatible, biodegradable and water-soluble polymeric materials can be engineered into multifunctional constructs with antimicrobial activity, targeting moieties, labelling units and/or efficiently loaded with therapeutics. This mini-review highlights the particular features exhibited by these materials resulting directly from the followed supercritical routes. © 2015 The Author(s).

  2. Defining the extreme substrate specificity of Euonymus alatus diacylglycerol acetyltransferase, an unusual membrane-bound O-acyltransferase

    DOE PAGES

    Bansal, Sunil; Durrett, Timothy P.

    2016-11-08

    Euonymus alatus diacylglycerol acetyltransferase (EaDAcT) synthesizes the unusually structured 3-acetyl-1,2-diacylglycerols (acetyl-TAG) found in the seeds of a few plant species. A member of the membrane-bound O-acyltransferase (MBOAT) family, EaDAcT transfers the acetyl group from acetyl-CoA to sn-1,2-diacylglycerol (DAG) to produce acetyl-TAG. In vitro assays demonstrated that the enzyme is also able to utilize butyryl-CoA and hexanoyl-CoA as acyl donors, though with much less efficiency compared with acetyl-CoA. Acyl-CoAs longer than eight carbons were not used by EaDAcT. This extreme substrate specificity of EaDAcT distinguishes it from all other MBOATs which typically catalyze the transfer of much longer acyl groups. Inmore » vitro selectivity experiments revealed that EaDAcT preferentially acetylated DAG molecules containing more double bonds over those with less. However, the enzyme was also able to acetylate saturated DAG containing medium chain fatty acids, albeit with less efficiency. Interestingly, EaDAcT could only acetylate the free hydroxyl group of sn-1,2-DAG but not the available hydroxyl groups in sn-1,3-DAG or in monoacylglycerols (MAG). Consistent with its similarity to the jojoba wax synthase, EaDAcT could acetylate fatty alcohols in vitro to produce alkyl acetates. Likewise, when coexpressed in yeast with a fatty acyl-CoA reductase capable of producing fatty alcohols, EaDAcT synthesized alkyl acetates although the efficiency of production was low. As a result, this improved understanding of EaDAcT specificity confirms that the enzyme preferentially utilizes acetyl-CoA to acetylate sn-1,2-DAGs and will be helpful in engineering the production of acetyl-TAG with improved functionality in transgenic plants.« less

  3. Defining the extreme substrate specificity of Euonymus alatus diacylglycerol acetyltransferase, an unusual membrane-bound O-acyltransferase

    PubMed Central

    Bansal, Sunil; Durrett, Timothy P.

    2016-01-01

    Euonymus alatus diacylglycerol acetyltransferase (EaDAcT) synthesizes the unusually structured 3-acetyl-1,2-diacylglycerols (acetyl-TAG) found in the seeds of a few plant species. A member of the membrane-bound O-acyltransferase (MBOAT) family, EaDAcT transfers the acetyl group from acetyl-CoA to sn-1,2-diacylglycerol (DAG) to produce acetyl-TAG. In vitro assays demonstrated that the enzyme is also able to utilize butyryl-CoA and hexanoyl-CoA as acyl donors, though with much less efficiency compared with acetyl-CoA. Acyl-CoAs longer than eight carbons were not used by EaDAcT. This extreme substrate specificity of EaDAcT distinguishes it from all other MBOATs which typically catalyze the transfer of much longer acyl groups. In vitro selectivity experiments revealed that EaDAcT preferentially acetylated DAG molecules containing more double bonds over those with less. However, the enzyme was also able to acetylate saturated DAG containing medium chain fatty acids, albeit with less efficiency. Interestingly, EaDAcT could only acetylate the free hydroxyl group of sn-1,2-DAG but not the available hydroxyl groups in sn-1,3-DAG or in monoacylglycerols (MAG). Consistent with its similarity to the jojoba wax synthase, EaDAcT could acetylate fatty alcohols in vitro to produce alkyl acetates. Likewise, when coexpressed in yeast with a fatty acyl-CoA reductase capable of producing fatty alcohols, EaDAcT synthesized alkyl acetates although the efficiency of production was low. This improved understanding of EaDAcT specificity confirms that the enzyme preferentially utilizes acetyl-CoA to acetylate sn-1,2-DAGs and will be helpful in engineering the production of acetyl-TAG with improved functionality in transgenic plants. PMID:27688773

  4. Defining the extreme substrate specificity of Euonymus alatus diacylglycerol acetyltransferase, an unusual membrane-bound O-acyltransferase

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Bansal, Sunil; Durrett, Timothy P.

    Euonymus alatus diacylglycerol acetyltransferase (EaDAcT) synthesizes the unusually structured 3-acetyl-1,2-diacylglycerols (acetyl-TAG) found in the seeds of a few plant species. A member of the membrane-bound O-acyltransferase (MBOAT) family, EaDAcT transfers the acetyl group from acetyl-CoA to sn-1,2-diacylglycerol (DAG) to produce acetyl-TAG. In vitro assays demonstrated that the enzyme is also able to utilize butyryl-CoA and hexanoyl-CoA as acyl donors, though with much less efficiency compared with acetyl-CoA. Acyl-CoAs longer than eight carbons were not used by EaDAcT. This extreme substrate specificity of EaDAcT distinguishes it from all other MBOATs which typically catalyze the transfer of much longer acyl groups. Inmore » vitro selectivity experiments revealed that EaDAcT preferentially acetylated DAG molecules containing more double bonds over those with less. However, the enzyme was also able to acetylate saturated DAG containing medium chain fatty acids, albeit with less efficiency. Interestingly, EaDAcT could only acetylate the free hydroxyl group of sn-1,2-DAG but not the available hydroxyl groups in sn-1,3-DAG or in monoacylglycerols (MAG). Consistent with its similarity to the jojoba wax synthase, EaDAcT could acetylate fatty alcohols in vitro to produce alkyl acetates. Likewise, when coexpressed in yeast with a fatty acyl-CoA reductase capable of producing fatty alcohols, EaDAcT synthesized alkyl acetates although the efficiency of production was low. As a result, this improved understanding of EaDAcT specificity confirms that the enzyme preferentially utilizes acetyl-CoA to acetylate sn-1,2-DAGs and will be helpful in engineering the production of acetyl-TAG with improved functionality in transgenic plants.« less

  5. Synthesis of highly efficient CaO-based, self-stabilizing CO2 sorbents via structure-reforming of steel slag.

    PubMed

    Tian, Sicong; Jiang, Jianguo; Yan, Feng; Li, Kaimin; Chen, Xuejing

    2015-06-16

    Capturing anthropogenic CO2 in a cost-effective and highly efficient manner is one of the most challenging issues faced by scientists today. Herein, we report a novel structure-reforming approach to convert steel slag, a cheap, abundant, and nontoxic calcium-rich industrial waste, as the only feedstock into superior CaO-based, self-stabilizing CO2 sorbents. The CO2 capture capacity of all the steel slag-derived sorbents was improved more than 10-fold compared to the raw slag, with the maximum uptake of CO2 achieving at 0.50 gCO2 gsorbent(-1). Additionally, the initial steel slag-derived sorbent could retain 0.25 gCO2 gsorbent(-1), that is, a decay rate of only 12% over 30 carbonation-calcination cycles, the excellent self-stabilizing property allowed it to significantly outperform conventional CaO, and match with most of the existing synthetic CaO-based sorbents. A synergistic effect that facilitated CO2 capture by CaO-based sorbents was clearly recognized when Mg and Al, the most common elements in steel slag, coexisted with CaO in the forms of MgO and Al2O3, respectively. During the calcium looping process, MgO served as a well spacer to increase the porosity of sorbents together with Al2O3 serving as a durable stabilizer to coresist the sintering of CaCO3 grains at high temperatures.

  6. CO 2 elevation improves photosynthetic performance in progressive warming environment in white birch seedlings.

    PubMed

    Zhang, Shouren; Dang, Qing-Lai

    2013-01-01

    White birch (Betula paperifera Mash) seedlings were exposed to progressively warming in greenhouses under ambient and elevated CO 2 concentrations for 5 months to explore boreal tree species' potential capacity to acclimate to global climate warming and CO 2 elevation. In situ foliar gas exchange, in vivo carboxylation characteristics and chlorophyll fluorescence were measured at temperatures of 26 (o)C and 37 (o)C. Elevated CO 2 significantly increased net photosynthetic rate (Pn) at both measurement temperatures, and Pn at 37 (o)C was higher than that at 26 (o)C under elevated CO 2. Stomatal conductance (gs) was lower at 37 (o)C than at 26 (o)C, while transpiration rate (E) was higher at 37 (o)C than that at 26 (o)C. Elevated CO 2 significantly increased instantaneous water-use efficiency (WUE) at both 26 (o)C and 37 (o)C, but WUE was markedly enhanced at 37 (o)C under elevated CO 2. The effect of temperature on maximal carboxylation rate (Vcmax), PAR-saturated electron transport rate (Jmax) and triose phosphate utilization (TPU) varied with CO 2, and the Vcmax and Jmax were significantly higher at 37 (o)C than at 26 (o)C under elevated CO 2. However, there were no significant interactive effects of CO 2 and temperature on TPU. The actual photochemical efficiency of PSII (DF/ Fm'), total photosynthetic linear electron transport rate through PSII (JT) and the partitioning of JT to carboxylation (Jc) were higher at 37 (o)C than at 26 (o)C under elevated CO 2. Elevated CO 2 significantly suppressed the partitioning of JT to oxygenation (Jo/JT). The data suggest that the CO 2 elevation and progressive warming greatly enhanced photosynthesis in white birch seedlings in an interactive fashion.

  7. Conversion of H2 and CO2 to CH4 and acetate in fed-batch biogas reactors by mixed biogas community: a novel route for the power-to-gas concept.

    PubMed

    Szuhaj, Márk; Ács, Norbert; Tengölics, Roland; Bodor, Attila; Rákhely, Gábor; Kovács, Kornél L; Bagi, Zoltán

    2016-01-01

    Applications of the power-to-gas principle for the handling of surplus renewable electricity have been proposed. The feasibility of using hydrogenotrophic methanogens as CH4 generating catalysts has been demonstrated. Laboratory and scale-up experiments have corroborated the benefits of the CO2 mitigation via biotechnological conversion of H2 and CO2 to CH4. A major bottleneck in the process is the gas-liquid mass transfer of H2. Fed-batch reactor configuration was tested at mesophilic temperature in laboratory experiments in order to improve the contact time and H2 mass transfer between the gas and liquid phases. Effluent from an industrial biogas facility served as biocatalyst. The bicarbonate content of the effluent was depleted after some time, but the addition of stoichiometric CO2 sustained H2 conversion for an extended period of time and prevented a pH shift. The microbial community generated biogas from the added α-cellulose substrate with concomitant H2 conversion, but the organic substrate did not facilitate H2 consumption. Fed-batch operational mode allowed a fourfold increase in volumetric H2 load and a 6.5-fold augmentation of the CH4 formation rate relative to the CSTR reactor configuration. Acetate was the major by-product of the reaction. Fed-batch reactors significantly improve the efficiency of the biological power-to-gas process. Besides their storage function, biogas fermentation effluent reservoirs can serve as large-scale bio CH4 reactors. On the basis of this recognition, a novel concept is proposed, which merges biogas technology with other means of renewable electricity production for improved efficiency and sustainability.

  8. Nitrogen-based catalysts for the electrochemical reduction of CO2 to CO.

    PubMed

    Tornow, Claire E; Thorson, Michael R; Ma, Sichao; Gewirth, Andrew A; Kenis, Paul J A

    2012-12-05

    The synthesis and application of carbon-supported, nitrogen-based organometallic silver catalysts for the reduction of CO(2) is studied using an electrochemical flow reactor. Their performance toward the selective formation of CO is similar to the performance achieved when using Ag as the catalyst, but comparatively at much lower silver loading. Faradaic efficiencies of the organometallic catalyst are higher than 90%, which are comparable to those of Ag. Furthermore, with the addition of an amine ligand to Ag/C, the partial current density for CO increases significantly, suggesting a possible co-catalyst mechanism. Additional improvements in activity and selectivity may be achieved as greater insight is obtained on the mechanism of CO(2) reduction and on how these complexes assemble on the carbon support.

  9. Open framework metal chalcogenides as efficient photocatalysts for reduction of CO2 into renewable hydrocarbon fuel.

    PubMed

    Sasan, Koroush; Lin, Qipu; Mao, Chengyu; Feng, Pingyun

    2016-06-07

    Open framework metal chalcogenides are a family of porous semiconducting materials with diverse chemical compositions. Here we show that these materials containing covalent three-dimensional superlattices of nanosized supertetrahedral clusters can function as efficient photocatalysts for the reduction of CO2 to CH4. Unlike dense semiconductors, metal cations are successfully incorporated into the channels of the porous semiconducting materials to further tune the physical properties of the materials such as electrical conductivity and band gaps. In terms of the photocatalytic properties, the metal-incorporated porous chalcogenides demonstrated enhanced solar energy absorption and higher electrical conductivity and improved photocatalytic activity.

  10. Doping Y 2O 3 with Mn 4+ for energy-efficient lighting

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Ming, Wenmei; Shi, Hongliang; Du, Mao-Hua

    Developing energy-efficient LEDs that emit warm white light requires new red phosphors with appropriate emission wavelengths and band widths. Mn 4+-activated Y 2O 3 is a potential red LED phosphor with narrow emission and improved emission wavelength compared to previously known Mn 4+-activated oxide phosphors. Here in this work, the dopability and the oxidation state of Mn in Y 2O 3 are investigated based on the formation energies of native defects, Mn dopants, and divalent co-dopants (i.e., Ca, Sr, Cd, and Zn) calculated using hybrid density functional theory. We found that Mn 4+ is difficult to form in Y 2Omore » 3 without co-doping. Stabilizing Mn 4+ on Y 3+ sites (forming Mn + Y donors) requires the co-doping of compensating acceptors (Ca or Sr) in oxygen-rich growth environments.« less

  11. Computational Modeling of Photocatalysts for CO2 Conversion Applications

    NASA Astrophysics Data System (ADS)

    Tafen, De; Matranga, Christopher

    2013-03-01

    To make photocatalytic conversion approaches efficient, economically practical, and industrially scalable, catalysts capable of utilizing visible and near infrared photons need to be developed. Recently, a series of CdSe and PbS quantum dot-sensitized TiO2 heterostructures have been synthesized, characterized, and tested for reduction of CO2 under visible light. Following these experiments, we use density functional theory to model these heterostructured catalysts and investigate their CO2 catalytic activity. In particular, we study the nature of the heterostructure interface, charge transport/electron transfer, active sites and the electronic structures of these materials. The results will be presented and compared to experiments. The improvement of our understanding of the properties of these materials will aid not only the development of more robust, visible light active photocatalysts for carbon management applications, but also the development of quantum dot-sensitized semiconductor solar cells with high efficiencies in solar-to-electrical energy conversion.

  12. Doping Y 2O 3 with Mn 4+ for energy-efficient lighting

    DOE PAGES

    Ming, Wenmei; Shi, Hongliang; Du, Mao-Hua

    2018-03-28

    Developing energy-efficient LEDs that emit warm white light requires new red phosphors with appropriate emission wavelengths and band widths. Mn 4+-activated Y 2O 3 is a potential red LED phosphor with narrow emission and improved emission wavelength compared to previously known Mn 4+-activated oxide phosphors. Here in this work, the dopability and the oxidation state of Mn in Y 2O 3 are investigated based on the formation energies of native defects, Mn dopants, and divalent co-dopants (i.e., Ca, Sr, Cd, and Zn) calculated using hybrid density functional theory. We found that Mn 4+ is difficult to form in Y 2Omore » 3 without co-doping. Stabilizing Mn 4+ on Y 3+ sites (forming Mn + Y donors) requires the co-doping of compensating acceptors (Ca or Sr) in oxygen-rich growth environments.« less

  13. Incorporation of MoS2 nanosheets in CoSb3 matrix as an efficient novel strategy to enhance its thermoelectric performance

    NASA Astrophysics Data System (ADS)

    Yadav, Suchitra; Chaudhary, Sujeet; Pandya, Dinesh K.

    2018-03-01

    The nanocomposite approach is considered as an effective way to improve the thermoelectric properties of bulk materials and we have exploited it by simultaneous though independent tackling of the electron and phonon transports. In the present study, through the strategy of anchoring the CoSb3 nanoparticles on the 2-dimensional nanosheets of MoS2, we demonstrate a controlled interplay of the newly created CoSb3/MoS2 interfaces in nanocomposites of varying concentration of MoS2 via significant enhancement of the phonon scattering without deterioration of electron transport. A concurrent occurrence of low energy carrier filtering on account of the interfacial potential barrier helps in beneficial manipulation of grain to grain carrier transport. The dimensionless figure of merit ZT maximizes to 0.53 at 600 K for the CoSb3/MoS2 nanocomposite containing 3 wt% of MoS2, 4-fold increase over the pristine CoSb3 in the 300-600 K range. This study paves the way towards improvement of the thermoelectric performance of p-type CoSb3 using 2D MoS2 as an interfacial additive.

  14. Effects of iron and calcium carbonate on contaminant removal efficiencies and microbial communities in integrated wastewater treatment systems.

    PubMed

    Zhao, Zhimiao; Song, Xinshan; Zhang, Yinjiang; Zhao, Yufeng; Wang, Bodi; Wang, Yuhui

    2017-12-01

    In the paper, we explored the influences of different dosages of iron and calcium carbonate on contaminant removal efficiencies and microbial communities in algal ponds combined with constructed wetlands. After 1-year operation of treatment systems, based on the high-throughput pyrosequencing analysis of microbial communities, the optimal operating conditions were obtained as follows: the ACW10 system with Fe 3+ (5.6 mg L -1 ), iron powder (2.8 mg L -1 ), and CaCO 3 powder (0.2 mg L -1 ) in influent as the adjusting agents, initial phosphorus source (PO 4 3- ) in influent, the ratio of nitrogen to phosphorus (N/P) of 30 in influent, and hydraulic retention time (HRT) of 1 day. Total nitrogen (TN) removal efficiency and total phosphorus (TP) removal efficiency were improved significantly. The hydrolysis of CaCO 3 promoted the physicochemical precipitation in contaminant removal. Meanwhile, Fe 3+ and iron powder produced Fe 2+ , which improved contaminant removal. Iron ion improved the diversity, distribution, and metabolic functions of microbial communities in integrated treatment systems. In the treatment ACW10, the dominant phylum in the microbial community was PLANCTOMYCETES, which positively promoted nitrogen removal. After 5 consecutive treatments in ACW10, contaminant removal efficiencies for TN and TP respectively reached 80.6% and 57.3% and total iron concentration in effluent was 0.042 mg L -1 . Copyright © 2017 Elsevier Ltd. All rights reserved.

  15. Bias flow rate and ventilation efficiency during adult high-frequency oscillatory ventilation: a lung model study.

    PubMed

    Nagano, Osamu; Yumoto, Tetsuya; Nishimatsu, Atsunori; Kanazawa, Shunsuke; Fujita, Takahisa; Asaba, Sunao; Yamanouchi, Hideo

    2018-04-19

    Bias flow (BF) is essential to maintain mean airway pressure (MAP) and to washout carbon dioxide (CO 2 ) from the oscillator circuit during high-frequency oscillatory ventilation (HFOV). If the BF rate is inadequate, substantial CO 2 rebreathing could occur and ventilation efficiency could worsen. With lower ventilation efficiency, the required stroke volume (SV) would increase in order to obtain the same alveolar ventilation with constant frequency. The aim of this study was to assess the effect of BF rate on ventilation efficiency during adult HFOV. The R100 oscillator (Metran, Japan) was connected to an original lung model internally equipped with a simulated bronchial tree. The actual SV was measured with a flow sensor placed at the Y-piece. Carbon dioxide (CO 2 ) was continuously insufflated into the lung model ([Formula: see text]CO 2 ), and the partial pressure of CO 2 (PCO 2 ) in the lung model was monitored. Alveolar ventilation ([Formula: see text]A) was estimated as [Formula: see text]CO 2 divided by the stabilized value of PCO 2 . [Formula: see text]A was evaluated by setting SV from 80 to 180 mL (10 mL increments, n = 5) at a frequency of 8 Hz, a MAP of 25 cmH 2 O, and a BF of 10, 20, 30, and 40 L/min (study 1). Ventilation efficiency was calculated as [Formula: see text]A divided by the actual minute volume. The experiment was also performed with an actual SV of 80, 100, and 120 mL and a BF from 10 to 60 L/min (10 L/min increments: study 2). Study 1: With the same setting SV, the [Formula: see text]A with a BF of 20 L/min or more was significantly higher than that with a BF of 10 L/min. Study 2: With the same actual SV, the [Formula: see text]A and the ventilation efficiency with a BF of 30 L/min or more were significantly higher than those with a BF of 10 or 20 L/min. Increasing BF up to 30 L/min or more improved ventilation efficiency in the R100 oscillator.

  16. Optimizing Rubisco and its regulation for greater resource use efficiency.

    PubMed

    Carmo-Silva, Elizabete; Scales, Joanna C; Madgwick, Pippa J; Parry, Martin A J

    2015-09-01

    Rubisco catalyses the carboxylation of ribulose-1,5-bisphosphate (RuBP), enabling net CO2 assimilation in photosynthesis. The properties and regulation of Rubisco are not optimal for biomass production in current and projected future environments. Rubisco is relatively inefficient, and large amounts of the enzyme are needed to support photosynthesis, requiring large investments in nitrogen. The competing oxygenation of RuBP by Rubisco decreases photosynthetic efficiency. Additionally, Rubisco is inhibited by some sugar phosphates and depends upon interaction with Rubisco activase (Rca) to be reactivated. Rca activity is modulated by the chloroplast redox status and ADP/ATP ratios, thereby mediating Rubisco activation and photosynthetic induction in response to irradiance. The extreme thermal sensitivity of Rca compromises net CO2 assimilation at moderately high temperatures. Given its central role in carbon assimilation, the improvement of Rubisco function and regulation is tightly linked with irradiance, nitrogen and water use efficiencies. Although past attempts have had limited success, novel technologies and an expanding knowledge base make the challenge of improving Rubisco activity in crops an achievable goal. Strategies to optimize Rubisco and its regulation are addressed in relation to their potential to improve crop resource use efficiency and climate resilience of photosynthesis. © 2014 Rothamsted Research Ltd. Plant, Cell & Environment published by John Wiley & Sons Ltd.

  17. Multiwell CO2 injectivity: impact of boundary conditions and brine extraction on geologic CO2 storage efficiency and pressure buildup.

    PubMed

    Heath, Jason E; McKenna, Sean A; Dewers, Thomas A; Roach, Jesse D; Kobos, Peter H

    2014-01-21

    CO2 storage efficiency is a metric that expresses the portion of the pore space of a subsurface geologic formation that is available to store CO2. Estimates of storage efficiency for large-scale geologic CO2 storage depend on a variety of factors including geologic properties and operational design. These factors govern estimates on CO2 storage resources, the longevity of storage sites, and potential pressure buildup in storage reservoirs. This study employs numerical modeling to quantify CO2 injection well numbers, well spacing, and storage efficiency as a function of geologic formation properties, open-versus-closed boundary conditions, and injection with or without brine extraction. The set of modeling runs is important as it allows the comparison of controlling factors on CO2 storage efficiency. Brine extraction in closed domains can result in storage efficiencies that are similar to those of injection in open-boundary domains. Geomechanical constraints on downhole pressure at both injection and extraction wells lower CO2 storage efficiency as compared to the idealized scenario in which the same volumes of CO2 and brine are injected and extracted, respectively. Geomechanical constraints should be taken into account to avoid potential damage to the storage site.

  18. CO2 Capture by Injection of Flue Gas or CO2-N2 Mixtures into Hydrate Reservoirs: Dependence of CO2 Capture Efficiency on Gas Hydrate Reservoir Conditions.

    PubMed

    Hassanpouryouzband, Aliakbar; Yang, Jinhai; Tohidi, Bahman; Chuvilin, Evgeny; Istomin, Vladimir; Bukhanov, Boris; Cheremisin, Alexey

    2018-04-03

    Injection of flue gas or CO 2 -N 2 mixtures into gas hydrate reservoirs has been considered as a promising option for geological storage of CO 2 . However, the thermodynamic process in which the CO 2 present in flue gas or a CO 2 -N 2 mixture is captured as hydrate has not been well understood. In this work, a series of experiments were conducted to investigate the dependence of CO 2 capture efficiency on reservoir conditions. The CO 2 capture efficiency was investigated at different injection pressures from 2.6 to 23.8 MPa and hydrate reservoir temperatures from 273.2 to 283.2 K in the presence of two different saturations of methane hydrate. The results showed that more than 60% of the CO 2 in the flue gas was captured and stored as CO 2 hydrate or CO 2 -mixed hydrates, while methane-rich gas was produced. The efficiency of CO 2 capture depends on the reservoir conditions including temperature, pressure, and hydrate saturation. For a certain reservoir temperature, there is an optimum reservoir pressure at which the maximum amount of CO 2 can be captured from the injected flue gas or CO 2 -N 2 mixtures. This finding suggests that it is essential to control the injection pressure to enhance CO 2 capture efficiency by flue gas or CO 2 -N 2 mixtures injection.

  19. Directions for Optimization of Photosynthetic Carbon Fixation: RuBisCO's Efficiency May Not Be So Constrained After All.

    PubMed

    Cummins, Peter L; Kannappan, Babu; Gready, Jill E

    2018-01-01

    The ubiquitous enzyme Ribulose 1,5-bisphosphate carboxylase-oxygenase (RuBisCO) fixes atmospheric carbon dioxide within the Calvin-Benson cycle that is utilized by most photosynthetic organisms. Despite this central role, RuBisCO's efficiency surprisingly struggles, with both a very slow turnover rate to products and also impaired substrate specificity, features that have long been an enigma as it would be assumed that its efficiency was under strong evolutionary pressure. RuBisCO's substrate specificity is compromised as it catalyzes a side-fixation reaction with atmospheric oxygen; empirical kinetic results show a trend to tradeoff between relative specificity and low catalytic turnover rate. Although the dominant hypothesis has been that the active-site chemistry constrains the enzyme's evolution, a more recent study on RuBisCO stability and adaptability has implicated competing selection pressures. Elucidating these constraints is crucial for directing future research on improving photosynthesis, as the current literature casts doubt on the potential effectiveness of site-directed mutagenesis to improve RuBisCO's efficiency. Here we use regression analysis to quantify the relationships between kinetic parameters obtained from empirical data sets spanning a wide evolutionary range of RuBisCOs. Most significantly we found that the rate constant for dissociation of CO 2 from the enzyme complex was much higher than previous estimates and comparable with the corresponding catalytic rate constant. Observed trends between relative specificity and turnover rate can be expressed as the product of negative and positive correlation factors. This provides an explanation in simple kinetic terms of both the natural variation of relative specificity as well as that obtained by reported site-directed mutagenesis results. We demonstrate that the kinetic behaviour shows a lesser rather than more constrained RuBisCO, consistent with growing empirical evidence of higher variability in relative specificity. In summary our analysis supports an explanation for the origin of the tradeoff between specificity and turnover as due to competition between protein stability and activity, rather than constraints between rate constants imposed by the underlying chemistry. Our analysis suggests that simultaneous improvement in both specificity and turnover rate of RuBisCO is possible.

  20. In situ photodeposition of amorphous CoSx on the TiO2 towards hydrogen evolution

    NASA Astrophysics Data System (ADS)

    Chen, Feng; Luo, Wei; Mo, Yanping; Yu, Huogen; Cheng, Bei

    2018-02-01

    Cocatalyst modification of photocatalysts is an important strategy to enhance the photocatalytic performance by promoting effective separation of photoinduced electron-hole pairs and providing abundant active sites. In this study, a facile in situ photodeposition method was developed to prepare amorphous CoSx-modified TiO2 photocatalysts. It was found that amorphous CoSx nanoparticles were solidly loaded on the TiO2 surface, resulting in a greatly improved photocatalytic H2-evolution performance. When the amount of amorphous CoSx was 10 wt%, the hydrogen evolution rate of the CoSx/TiO2 reached 119.7 μmol h-1, which was almost 16.7 times that of the pure TiO2. According to the above experimental results, a reasonable mechanism of improved photocatalytic performance is proposed for the CoSx/TiO2 photocatalysts, namely, the photogenerated electrons of TiO2 can rapidly transfer to amorphous CoSx nanoparticles due to the solid contact between them, and then amorphous CoSx can provide plenty of sulfur active sites to rapidly adsorb protons from solution to produce hydrogen by the photogenerated electrons. Considering the facile synthesis method, the present cheap and highly efficient amorphous CoSx-modified TiO2 photocatalysts would have great potential for practical use in photocatalytic H2 production.

  1. Efficient androst-1,4-diene-3,17-dione production by co-expressing 3-ketosteroid-Δ1 -dehydrogenase and catalase in Bacillus subtilis.

    PubMed

    Shao, M; Sha, Z; Zhang, X; Rao, Z; Xu, M; Yang, T; Xu, Z; Yang, S

    2017-01-01

    3-ketosteroid-Δ 1 -dehydrogenase (KSDD), a flavin adenine dinucleotide (FAD)-dependent enzyme involved in sterol metabolism, specifically catalyses the conversion of androst-4-ene-3,17-dione (AD) to androst-1,4-diene-3,17-dione (ADD). However, the low KSDD activity and the toxic effects of hydrogen peroxide (H 2 O 2 ) generated during the biotransformation of AD to ADD with FAD regeneration hinder its application on AD conversion. The aim of this work was to improve KSDD activity and eliminate the toxic effects of the generated H 2 O 2 to enhance ADD production. The ksdd gene obtained from Mycobacterium neoaurum JC-12 was codon-optimized to increase its expression level in Bacillus subtilis, and the KSDD activity reached 12·3 U mg -1 , which was sevenfold of that of codon-unoptimized gene. To improve AD conversion, catalase was co-expressed with KSDD in B. subtilis 168/pMA5-ksdd opt -katA to eliminate the toxic effects of H 2 O 2 generated during AD conversion. Finally, under optimized bioconversion conditions, fed-batch strategy was carried out and the ADD yield improved to 8·76 g l -1 . This work demonstrates the potential to improve enzyme activity by codon-optimization and eliminate the toxic effects of H 2 O 2 by co-expressing catalase. This study showed the highest ADD productivity ever reported and provides a promising strain for efficient ADD production in the pharmaceutical industry. © 2016 The Society for Applied Microbiology.

  2. Solid Solution Photocatalyst with Spontaneous Polarization Exhibiting Low Recombination Toward Efficient CO2 Photoreduction.

    PubMed

    Zhou, Peng; Wang, Xin; Yan, Shicheng; Zou, Zhigang

    2016-08-23

    Decreasing the recombination of photogenerated carriers is a major challenge for efficiently converting solar energy into chemical energy by photocatalysis. Here, we have demonstrated that growth of a polar GaN:ZnO solid solution single crystal along its polarization axis is beneficial to efficient separation of photogenerated carriers, owing to the periodic potential barriers and wells generated from the periodically positive and negative atom arrangements in crystal structure. Local charge imbalance caused by replacing Ga(3+) with Zn(2+) leads to a polarization vector in the {0 0 0 1} planes of GaN:ZnO solid solution, thus forming a 1 D electron transport path along [2 1‾  1‾  0] in the {0 0 0 1} planes of GaN:ZnO solid solution to decrease recombination. Shorting the hole-transport distance by synthesizing porous nanoplates can further decrease recombination under the polarization field and improve the performance of polar photocatalyst in photoreduction of CO2 into CH4 . © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. Tailoring gas-phase CO2 electroreduction selectivity to hydrocarbons at Cu nanoparticles

    NASA Astrophysics Data System (ADS)

    Merino-Garcia, I.; Albo, J.; Irabien, A.

    2018-01-01

    Copper-based surfaces appear as the most active catalysts for CO2 electroreduction to hydrocarbons, even though formation rates and efficiencies still need to be improved. The aim of the present work is to evaluate the continuous gas-phase CO2 electroreduction to hydrocarbons (i.e. ethylene and methane) at copper nanoparticulated-based surfaces, paying attention to particle size influence (ranging from 25-80 nm) on reaction productivity, selectivity, and Faraday efficiency (FE) for CO2 conversion. The effect of the current density and the presence of a microporous layer within the working electrode are then evaluated. Copper-based gas diffusion electrodes are prepared by airbrushing the catalytic ink onto carbon supports, which are then coupled to a cation exchange membrane (Nafion) in a membrane electrode assembly. The results show that the use of smaller copper nanoparticles (25 nm) leads to a higher ethylene production (1148 μmol m-2 s-1) with a remarkable high FE (92.8%), at the same time, diminishing the competitive hydrogen evolution reaction in terms of FE. This work demonstrates the importance of nanoparticle size on reaction selectivity, which may be of help to design enhanced electrocatalytic materials for CO2 valorization to hydrocarbons.

  4. Energy-Efficiency and Air-Pollutant Emissions-Reduction Opportunities for the Ammonia Industry in China

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Ma, Ding; Hasanbeigi, Ali; Chen, Wenying

    As one of the most energy-intensive and polluting industries, ammonia production is responsible for significant carbon dioxide (CO 2) and air-pollutant emissions. Although many energy-efficiency measures have been proposed by the Chinese government to mitigate greenhouse gas emissions and improve air quality, lack of understanding of the cost-effectiveness of such improvements has been a barrier to implementing these measures. Assessing the costs, benefits, and cost-effectiveness of different energy-efficiency measures is essential to advancing this understanding. In this study, a bottom-up energy conservation supply curve model is developed to estimate the potential for energy savings and emissions reductions from 26 energy-efficiencymore » measures that could be applied in China’s ammonia industry. Cost-effective implementation of these measures saves a potential 271.5 petajoules/year for fuel and 5,443 gigawatt-hours/year for electricity, equal to 14% of fuel and 14% of electricity consumed in China’s ammonia industry in 2012. These reductions could mitigate 26.7 million tonnes of CO 2 emissions. This study also quantifies the co-benefits of reducing air-pollutant emissions and water use that would result from saving energy in China’s ammonia industry. This quantitative analysis advances our understanding of the cost-effectiveness of energy-efficiency measures and can be used to augment efforts to reduce energy use and environmental impacts.« less

  5. Improved production of transgenic Dioscorea zingiberensis (Dioscoreaceae) by Agrobacterium tumefaciens-mediated transformation.

    PubMed

    Shi, L; Fan, J Q; Hu, C G; Luo, J; Yao, J L

    2012-02-03

    The establishment of high-efficiency Agrobacterium-mediated transformation techniques could improve the production of Dioscorea zingiberensis, a medicinal species with a high diosgenin content. We co-cultivated embryogenic calli induced from mature seeds with A. tumefaciens strain EHA105. A binary vector, pCAMBIA1381, which contains the gfp and hpt genes under the control of the ubiquitin promoter and the CaMV 35S promoter, respectively, was used for transformation. Pre-culture, basic medium, acetosyringone, and bacterial density were evaluated to establish the most efficient protocol. The optimal conditions consisted of MS medium without CaCl(2) for pre- and co-cultivation, three days for pre-culture, addition of 200 μM AS, and an OD(600) of 0.5. The transgenic plants grown under selection were confirmed by PCR analysis and Southern blot analysis. This protocol produced transgenic D. zingiberensis plants in seven months, with a transformation efficiency of 6%.

  6. Decomposing Fuel Economy and Greenhouse Gas Regulatory Standards in the Energy Conversion Efficiency and Tractive Energy Domain

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Pannone, Greg; Thomas, John F; Reale, Michael

    The three foundational elements that determine mobile source energy use and tailpipe carbon dioxide (CO2) emissions are the tractive energy requirements of the vehicle, the on-cycle energy conversion efficiency of the propulsion system, and the energy source. The tractive energy requirements are determined by the vehicle's mass, aerodynamic drag, tire rolling resistance, and parasitic drag. Oncycle energy conversion of the propulsion system is dictated by the tractive efficiency, non-tractive energy use, kinetic energy recovery, and parasitic losses. The energy source determines the mobile source CO2 emissions. For current vehicles, tractive energy requirements and overall energy conversion efficiency are readily availablemore » from the decomposition of test data. For future applications, plausible levels of mass reduction, aerodynamic drag improvements, and tire rolling resistance can be transposed into the tractive energy domain. Similarly, by combining thermodynamic, mechanical efficiency, and kinetic energy recovery fundamentals with logical proxies, achievable levels of energy conversion efficiency can be established to allow for the evaluation of future powertrain requirements. Combining the plausible levels of tractive energy and on-cycle efficiency provides a means to compute sustainable vehicle and propulsion system scenarios that can achieve future regulations. Using these principles, the regulations established in the United States (U.S.) for fuel consumption and CO2 emissions are evaluated. Fleet-level scenarios are generated and compared to the technology deployment assumptions made during rule-making. When compared to the rule-making assumptions, the results indicate that a greater level of advanced vehicle and propulsion system technology deployment will be required to achieve the model year 2025 U.S. standards for fuel economy and CO2 emissions.« less

  7. Exploring the impact of determining factors behind CO2 emissions in China: A CGE appraisal.

    PubMed

    Xiao, Bowen; Niu, Dongxiao; Wu, Han

    2017-03-01

    Along with the arrival of the post-Kyoto Protocol era, the Chinese government faces ever greater pressure to reduce greenhouse gases (GHGs). Hence, this paper aims to discuss the drivers of carbon dioxide (CO 2 ) emissions and their impact on society as a whole. First, we analyzed the background and overall situations of CO 2 emissions in China. Then, we reviewed previous studies to explore the determinants behind China's CO 2 emissions. It is widely acknowledged that energy efficiency, energy mix, and economy structure are three key factors contributing to CO 2 emissions. To explore the impacts of those three factors on the economy and CO 2 emissions, we established a computable general equilibrium (CGE) model. The following results were found: (1) The decline of a secondary industry can cause an emission reduction effect, but this is at the expense of the gross domestic product (GDP), whereas the development of a tertiary industry can boost the economy and help to reduce CO 2 emissions. (2) Cutting coal consumption can contribute significantly to emission reduction, which is accompanied by a great loss in the whole economy. (3) Although the energy efficiency improvement plays a positive role in promoting economic development, a backfire effect can weaken the effects of emission reduction and energy savings. Copyright © 2016 Elsevier B.V. All rights reserved.

  8. Incorporating nitrogen atoms into cobalt nanosheets as a strategy to boost catalytic activity toward CO2 hydrogenation

    NASA Astrophysics Data System (ADS)

    Wang, Liangbing; Zhang, Wenbo; Zheng, Xusheng; Chen, Yizhen; Wu, Wenlong; Qiu, Jianxiang; Zhao, Xiangchen; Zhao, Xiao; Dai, Yizhou; Zeng, Jie

    2017-11-01

    Hydrogenation of CO2 into fuels and useful chemicals could help to reduce reliance on fossil fuels. Although great progress has been made over the past decades to improve the activity of catalysts for CO2 hydrogenation, more efficient catalysts, especially those based on non-noble metals, are desired. Here we incorporate N atoms into Co nanosheets to boost the catalytic activity toward CO2 hydrogenation. For the hydrogenation of CO2, Co4N nanosheets exhibited a turnover frequency of 25.6 h-1 in a slurry reactor under 32 bar pressure at 150 °C, which was 64 times that of Co nanosheets. The activation energy for Co4N nanosheets was 43.3 kJ mol-1, less than half of that for Co nanosheets. Mechanistic studies revealed that Co4N nanosheets were reconstructed into Co4NHx, wherein the amido-hydrogen atoms directly interacted with the CO2 to form HCOO* intermediates. In addition, the adsorbed H2O* activated amido-hydrogen atoms via the interaction of hydrogen bonds.

  9. ZIF-67-derived hollow nanocages with layered double oxides shell as high-Efficiency catalysts for CO oxidation

    NASA Astrophysics Data System (ADS)

    Kong, Wenpeng; Li, Jing; Chen, Yao; Ren, Yuqing; Guo, Yonghua; Niu, Shengli; Yang, Yanzhao

    2018-04-01

    Constructing non-precious hybrid metal oxides with specific morphology as cost-effective and highly efficient catalysts is a promising way for the automotive exhaust purification. In this work, we report a facile strategy for the fabrication of a unique hollow Co-Ni layered double oxides (HLDO) nanocages by using zeolitic imidazole frameworks (ZIFs) as template. The synthesis of intermediate core-shell and hollow Co-Ni layered double hydroxides (HLDH) nanoflakes as well as the corresponding Co-Ni oxides products were successfully controlled, and the formation process was also explained. Among ZIF-67-derived oxides, HLDO exhibits excellent catalytic activities (complete conversion of CO into CO2 at 118 °C) and long-term stability for CO oxidation. The remarkable catalytic activities of HLDO can be attributed to high surface area (258 m2 g-1) inherited from the HLDH, which could provide more active sites for CO oxidation. In addition, active oxygen species indicated by the O 1 s XPS spectrum and improved synergistic effect between NiO and Co3O4 reflected by H2-TPR, further explain the enhanced performance of the HLDO catalysts. The presented strategy for controlled design and synthesis of hollow multicomponent metal oxides will provide prospects in developing highly effective catalysts.

  10. In Situ Fabrication and Reactivation of Highly Selective and Stable Ag Catalysts for Electrochemical CO2 Conversion.

    PubMed

    Ma, Ming; Liu, Kai; Shen, Jie; Kas, Recep; Smith, Wilson A

    2018-06-08

    In this work, the highly selective and stable electrocatalytic reduction of CO 2 to CO on nanostructured Ag electrocatalysts is presented. The Ag electrocatalysts are synthesized by the electroreduction of Ag 2 CO 3 formed by in situ anodic-etching of Ag foil in a KHCO 3 electrolyte. After 3 min of this etching treatment, the Ag 2 CO 3 -derived nanostructured Ag electrocatalysts are capable of producing CO with up to 92% Faradaic efficiency at an overpotential as low as 290 mV, which surpasses all of the reported Ag catalysts at identical conditions to date. In addition, the anodic-etched Ag retained ∼90% catalytic selectivity in the electroreduction of CO 2 to CO for more than 100 h. The Ag 2 CO 3 -derived Ag is able to facilitate the activation of CO 2 via reduction of the activation energy barrier of the initial electron transfer and provide an increased number of active sites, resulting in the dramatically improved catalytic activity for the reduction of CO 2 to CO.

  11. Effective Approach for Increasing the Heteroatom Doping Levels of Porous Carbons for Superior CO2 Capture and Separation Performance.

    PubMed

    Abdelmoaty, Yomna H; Tessema, Tsemre-Dingel; Norouzi, Nazgol; El-Kadri, Oussama M; Turner, Joseph B McGee; El-Kaderi, Hani M

    2017-10-18

    Development of efficient sorbents for carbon dioxide (CO 2 ) capture from flue gas or its removal from natural gas and landfill gas is very important for environmental protection. A new series of heteroatom-doped porous carbon was synthesized directly from pyrazole/KOH by thermolysis. The resulting pyrazole-derived carbons (PYDCs) are highly doped with nitrogen (14.9-15.5 wt %) as a result of the high nitrogen-to-carbon ratio in pyrazole (43 wt %) and also have a high oxygen content (16.4-18.4 wt %). PYDCs have a high surface area (SA BET = 1266-2013 m 2 g -1 ), high CO 2 Q st (33.2-37.1 kJ mol -1 ), and a combination of mesoporous and microporous pores. PYDCs exhibit significantly high CO 2 uptakes that reach 2.15 and 6.06 mmol g -1 at 0.15 and 1 bar, respectively, at 298 K. At 273 K, the CO 2 uptake improves to 3.7 and 8.59 mmol g -1 at 0.15 and 1 bar, respectively. The reported porous carbons also show significantly high adsorption selectivity for CO 2 /N 2 (128) and CO 2 /CH 4 (13.4) according to ideal adsorbed solution theory calculations at 298 K. Gas breakthrough studies of CO 2 /N 2 (10:90) at 298 K showed that PYDCs display excellent separation properties. The ability to tailor the physical properties of PYDCs as well as their chemical composition provides an effective strategy for designing efficient CO 2 sorbents.

  12. Molecularly Engineered Ru(II) Sensitizers Compatible with Cobalt(II/III) Redox Mediators for Dye-Sensitized Solar Cells.

    PubMed

    Wu, Kuan-Lin; Huckaba, Aron J; Clifford, John N; Yang, Ya-Wen; Yella, Aswani; Palomares, Emilio; Grätzel, Michael; Chi, Yun; Nazeeruddin, Mohammad Khaja

    2016-08-01

    Thiocyanate-free isoquinazolylpyrazolate Ru(II) complexes were synthesized and applied as sensitizers in dye-sensitized solar cells (DSCs). Unlike most other successful Ru sensitizers, Co-based electrolytes were used, and resulting record efficiency of 9.53% was obtained under simulated sunlight with an intensity of 100 mW cm(-2). Specifically, dye 51-57dht.1 and an electrolyte based on Co(phen)3 led to measurement of a JSC of 13.89 mA cm(-2), VOC of 900 mV, and FF of 0.762 to yield 9.53% efficiency. The improved device performances were achieved by the inclusion of 2-hexylthiophene units onto the isoquinoline subunits, in addition to lengthening the perfluoroalkyl chain on the pyrazolate chelating group, which worked to increase light absorption and decrease recombination effects when using the Co-based electrolyte. As this study shows, Ru(II) sensitizers bearing sterically demanding ligands can allow successful utilization of important Co electrolytes and high performance.

  13. Metal-Organic Frameworks Derived Porous Core/Shell Structured ZnO/ZnCo2O4/C Hybrids as Anodes for High-Performance Lithium-Ion Battery.

    PubMed

    Ge, Xiaoli; Li, Zhaoqiang; Wang, Chengxiang; Yin, Longwei

    2015-12-09

    Metal-organic frameworks (MOFs) derived porous core/shell ZnO/ZnCo2O4/C hybrids with ZnO as a core and ZnCo2O4 as a shell are for the first time fabricated by using core/shell ZnCo-MOF precursors as reactant templates. The unique MOFs-derived core/shell structured ZnO/ZnCo2O4/C hybrids are assembled from nanoparticles of ZnO and ZnCo2O4, with homogeneous carbon layers coated on the surface of the ZnCo2O4 shell. When acting as anode materials for lithium-ion batteries (LIBs), the MOFs-derived porous ZnO/ZnCo2O4/C anodes exhibit outstanding cycling stability, high Coulombic efficiency, and remarkable rate capability. The excellent electrochemical performance of the ZnO/ZnCo2O4/C LIB anodes can be attributed to the synergistic effect of the porous structure of the MOFs-derived core/shell ZnO/ZnCo2O4/C and homogeneous carbon layer coating on the surface of the ZnCo2O4 shells. The hierarchically porous core/shell structure offers abundant active sites, enhances the electrode/electrolyte contact area, provides abundant channels for electrolyte penetration, and also alleviates the structure decomposition induced by Li(+) insertion/extraction. The carbon layers effectively improve the conductivity of the hybrids and thus enhance the electron transfer rate, efficiently prevent ZnCo2O4 from aggregation and disintegration, and partially buffer the stress induced by the volume change during cycles. This strategy may shed light on designing new MOF-based hybrid electrodes for energy storage and conversion devices.

  14. Physiological and molecular alterations in plants exposed to high [CO2] under phosphorus stress.

    PubMed

    Pandey, Renu; Zinta, Gaurav; AbdElgawad, Hamada; Ahmad, Altaf; Jain, Vanita; Janssens, Ivan A

    2015-01-01

    Atmospheric [CO2] has increased substantially in recent decades and will continue to do so, whereas the availability of phosphorus (P) is limited and unlikely to increase in the future. P is a non-renewable resource, and it is essential to every form of life. P is a key plant nutrient controlling the responsiveness of photosynthesis to [CO2]. Increases in [CO2] typically results in increased biomass through stimulation of net photosynthesis, and hence enhance the demand for P uptake. However, most soils contain low concentrations of available P. Therefore, low P is one of the major growth-limiting factors for plants in many agricultural and natural ecosystems. The adaptive responses of plants to [CO2] and P availability encompass alterations at morphological, physiological, biochemical and molecular levels. In general low P reduces growth, whereas high [CO2] enhances it particularly in C3 plants. Photosynthetic capacity is often enhanced under high [CO2] with sufficient P supply through modulation of enzyme activities involved in carbon fixation such as ribulose-1,5-bisphosphate carboxylase/oxygenase (Rubisco). However, high [CO2] with low P availability results in enhanced dry matter partitioning towards roots. Alterations in below-ground processes including root morphology, exudation and mycorrhizal association are influenced by [CO2] and P availability. Under high P availability, elevated [CO2] improves the uptake of P from soil. In contrast, under low P availability, high [CO2] mainly improves the efficiency with which plants produce biomass per unit P. At molecular level, the spatio-temporal regulation of genes involved in plant adaptation to low P and high [CO2] has been studied individually in various plant species. Genome-wide expression profiling of high [CO2] grown plants revealed hormonal regulation of biomass accumulation through complex transcriptional networks. Similarly, differential transcriptional regulatory networks are involved in P-limitation responses in plants. Analysis of expression patterns of some typical P-limitation induced genes under high [CO2] suggests that long-term exposure of plants to high [CO2] would have a tendency to stimulate similar transcriptional responses as observed under P-limitation. However, studies on the combined effect of high [CO2] and low P on gene expression are scarce. Such studies would provide insights into the development of P efficient crops in the context of anticipated increases in atmospheric [CO2]. Copyright © 2015 Elsevier Inc. All rights reserved.

  15. Tuning anion-functionalized ionic liquids for improved SO2 capture.

    PubMed

    Cui, Guokai; Zheng, Junjie; Luo, Xiaoyan; Lin, Wenjun; Ding, Fang; Li, Haoran; Wang, Congmin

    2013-09-27

    You can have your cake and eat it too: A "dual-tuning" strategy for improving the capture of SO2 was developed by introducing electron-withdrawing sites on the anions to produce several kinds of functionalized ionic liquids. Those functionalized with a halogen group exhibited improved performance over their non-halogenated counterparts, leading to highly efficient and reversible capture. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  16. Influences of the (NH2)2CO concentration on magnetic photocatalytic composites

    NASA Astrophysics Data System (ADS)

    Liŭ, Dan; Li, Ziheng; Wang, Wenquan; Liú, Dan; Wang, Guoqiang; Lin, Junhong; He, Yingqiao; Li, Xiangru

    2016-11-01

    Magnetic photocatalytic Fe3O4@TiO2 composites have been fabricated by changing the concentration of (NH2)2CO. Samples were named as low (NH2)2CO concentration group which the (NH2)2CO concentration in the synthesis process was below 2.25 mol/L and high (NH2)2CO concentration group which the (NH2)2CO concentration was above 2.5 mol/L. Photocatalytic degradation experiments of methyl orange showed that the final degradation rates of low (NH2)2CO concentration group samples were higher than that of high (NH2)2CO concentration group, even better than P25 at the same test conditions. And it was interesting that samples of low (NH2)2CO concentration group had smaller values of BET surface areas than that of high (NH2)2CO concentration group. It indicated that the improvement of photocatalytic activity which was effected by BET surface areas was not obvious. There were two main factors enhancing the photocatalytic property of low (NH2)2CO concentration group: First, diffusing reflection spectra showed that the low (NH2)2CO concentration group samples had lower reflectivity, this suggested that the structure improved the efficiency of light absorption; Second, NH4+ would take up the active sites on the surface of the TiO2 particles, the FT-IR test results showed that the samples of the low (NH2)2CO concentration group samples bonded less NH4+, thus leading to the higher photocatalytic activity. It had enlightenment role for optimizing the performance of photocatalytic materials.

  17. Plasma catalytic reforming of methane

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Bromberg, L.; Cohn, D.R.; Rabinovich, A.

    1998-08-01

    Thermal plasma technology can be efficiently used in the production of hydrogen and hydrogen-rich gases from methane and a variety of fuels. This paper describes progress in plasma reforming experiments and calculations of high temperature conversion of methane using heterogeneous processes. The thermal plasma is a highly energetic state of matter that is characterized by extremely high temperatures (several thousand degrees Celsius) and high degree of dissociation and substantial degree of ionization. The high temperatures accelerate the reactions involved in the reforming process. Hydrogen-rich gas (50% H{sub 2}, 17% CO and 33% N{sub 2}, for partial oxidation/water shifting) can bemore » efficiently made in compact plasma reformers. Experiments have been carried out in a small device (2--3 kW) and without the use of efficient heat regeneration. For partial oxidation/water shifting, it was determined that the specific energy consumption in the plasma reforming processes is 16 MJ/kg H{sub 2} with high conversion efficiencies. Larger plasmatrons, better reactor thermal insulation, efficient heat regeneration and improved plasma catalysis could also play a major role in specific energy consumption reduction and increasing the methane conversion. A system has been demonstrated for hydrogen production with low CO content ({approximately} 1.5%) with power densities of {approximately} 30 kW (H{sub 2} HHV)/liter of reactor, or {approximately} 10 m{sup 3}/hr H{sub 2} per liter of reactor. Power density should further increase with increased power and improved design.« less

  18. Substantial Air Quality and Climate Co-benefits Achievable Now with Industrial Efficiency Improvements in China

    NASA Astrophysics Data System (ADS)

    Mauzerall, D. L.; Peng, W.; Wagner, F.; Yang, J.

    2016-12-01

    China is the world's top carbon emitter and suffers from severe air pollution. It has recently made commitments to improve air quality and peak its carbon emissions by 2030. Here we examine near-term air quality and implications for CO2 emissions of various sector-based policies in China that are widely discussed and technically plausible for immediate implementation. For each sector, we consider the effect of a 20% increase in the installation rate of available air pollution control devices, along with the following sector-specific policies. Power sector (POW): 80% replacement of small coal power plants with larger more efficient ones; Industry sector (IND): 20% improvement in energy efficiency; Transport sector (TRA): replacement of high emitters with average vehicle fleet emissions; and Residential sector (RES): replacement of 20% of coal-based stoves with those using liquefied petroleum gas. We conduct an integrated assessment using the air pollution model WRF-Chem and epidemiological concentration-response relationships to evaluate a 2015 base case and various counterfactual scenarios. We find that the IND scenario would reduce both the total national air-pollution-related deaths and carbon emissions the most of the four sectorial scenarios examined. Benefits of addressing the industrial sector remain large even when efficiency improvements are smaller than 20%. Moreover, we find that simultaneously implementing all the measures in all four sectors (combined, COMB) leads to slightly larger air quality and health benefits than obtained by summing the benefits achieved from the four sectorial scenarios individually. This is because nonlinearity in atmospheric chemistry leads to a larger reduction in fine particulate concentrations when emissions from all sectors are reduced simultaneously. The resulting lower concentrations imply a lower position on the concave human premature mortality relative risk curve with fewer associated deaths. While much effort has focused on reducing emissions from the power and transportation sectors, our analysis highlights the importance of efficiency improvements in the industrial sector as a mechanism to simultaneously improve air quality and public health while reducing CO2 emissions.

  19. High-performance multilayer composite membranes with mussel-inspired polydopamine as a versatile molecular bridge for CO2 separation.

    PubMed

    Li, Panyuan; Wang, Zhi; Li, Wen; Liu, Yanni; Wang, Jixiao; Wang, Shichang

    2015-07-22

    It is desirable to develop high-performance composite membranes for efficient CO2 separation in CO2 capture process. Introduction of a highly permeable polydimethylsiloxane (PDMS) intermediate layer between a selective layer and a porous support has been considered as a simple but efficient way to enhance gas permeance while maintaining high gas selectivity, because the introduced intermediate layer could benefit the formation of an ultrathin defect-free selective layer owing to the circumvention of pore penetration phenomenon. However, the selection of selective layer materials is unfavorably restricted because of the low surface energy of PDMS. Various highly hydrophilic membrane materials such as amino group-rich polyvinylamine (PVAm), a representative facilitated transport membrane material for CO2 separation, could not be facilely coated over the surface of the hydrophobic PDMS intermediate layer uniformly. Inspired by the hydrophilic nature and strong adhesive ability of polydopamine (PDA), PDA was therefore selected as a versatile molecular bridge between hydrophobic PDMS and hydrophilic PVAm. The PDA coating endows a highly compatible interface between both components with a large surface energy difference via multiple-site cooperative interactions. The resulting multilayer composite membrane with a thin facilitated transport PVAm selective layer exhibits a notably enhanced CO2 permeance (1887 GPU) combined with a slightly improved CO2/N2 selectivity (83), as well as superior structural stability. Similarly, the multilayer composite membrane with a hydrophilic CO2-philic Pebax 1657 selective layer was also developed for enhanced CO2 separation performance.

  20. Assessment of Energy Efficiency Improvement and CO2 Emission Reduction Potentials in India's Cement Industry

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Morrow, III, William R.; Hasanbeigi, Ali; Xu, Tengfang

    2012-12-03

    India’s cement industry is the second largest in the world behind China with annual cement production of 168 Mt in 2010 which accounted for slightly greater than six percent of the world’s annual cement production in the same year. To produce that amount of cement, the industry consumed roughly 700 PJ of fuel and 14.7 TWh of electricity. We identified and analyzed 22 energy efficiency technologies and measures applicable to the processes in the Indian cement industry. The Conservation Supply Curve (CSC) used in this study is an analytical tool that captures both the engineering and the economic perspectives ofmore » energy conservation. Using a bottom-up electricity CSC model and compared to an electricity price forecast the cumulative cost-effective plant-level electricity savings potential for the Indian cement industry for 2010- 2030 is estimated to be 83 TWh, and the cumulative plant-level technical electricity saving potential is 89 TWh during the same period. The grid-level CO2 emissions reduction associated with cost-effective electricity savings is 82 Mt CO2 and the electric grid-level CO2 emission reduction associated with technical electricity saving potential is 88 Mt CO2. Compared to a fuel price forecast, an estimated cumulative cost-effective fuel savings potential of 1,029 PJ with associated CO2 emission reduction of 97 Mt CO2 during 2010-2030 is possible. In addition, a sensitivity analysis with respect to the discount rate used is conducted to assess the effect of changes in this parameter on the results. The result of this study gives a comprehensive and easy to understand perspective to the Indian cement industry and policy makers about the energy efficiency potential and its associated cost over the next twenty years.« less

  1. Significantly improved efficiency of organic solar cells incorporating Co3O4 NPs in the active layer

    NASA Astrophysics Data System (ADS)

    Yousaf, S. Amber; Ikram, M.; Ali, S.

    2018-03-01

    Effect of various concentrations of fabricated cobalt oxide (Co3O4) nanoparticles (NPs) in the active layer of different donors and acceptors based hybrid organic bulk heterojunction-BHJ devices were investigated using inverted architecture. The organic active layer comprising different donors P3HT (poly(3-hexylthiophene-2,5-diyl) and PTB7 (Poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b] thiophenediyl

  2. 75 FR 20111 - Energy Conservation Program: Energy Conservation Standards for Residential Water Heaters, Direct...

    Federal Register 2010, 2011, 2012, 2013, 2014

    2010-04-16

    ... the ``three heating products'') must be designed to ``achieve the maximum improvement in energy... and CO 2 savings are performed with different computer models, leading to different time frames for... of EPCA sets forth a variety of provisions designed to improve energy efficiency. Part A\\1\\ of Title...

  3. Experimental research on microscopic displacement mechanism of CO2-water alternative flooding in low permeability reservoir

    NASA Astrophysics Data System (ADS)

    Han, Hongyan; Zhu, Weiyao; Long, Yunqian; Song, Hongqing; Huang, Kun

    2018-02-01

    This paper provides an experimental method to deal with the problems of low oil recovery ratio faced with water flooding utilizing the CO2/water alternate displacement technology. A series of CO2/water alternate flooding experiments were carried out under 60°C and 18.4MPa using high temperature / pressure microscopic visualization simulation system. Then, we used the image processing technique and software to analyze the proportion of remaining oil in the displacement process. The results show that CO2 can extract the lighter chemical components in the crude oil and make it easier to form miscible phase, which can reduce the viscosity and favorable mobility ratio of oil. What’s more, the displacement reduces the impact of gas channeling, which can achieve an enlarged sweeping efficiency to improve filtration ability. In addition, the CO2 dissolved in oil and water can greatly reduce the interfacial tension, which can increase the oil displacement efficiency in a large extent. Generally speaking, the recovery rate of residual oil in the micro - model can be elevated up to 15.89% ∼ 16.48% under formation condition by alternate displacement.

  4. Graphene-Based Photocatalysts for CO2 Reduction to Solar Fuel.

    PubMed

    Low, Jingxiang; Yu, Jiaguo; Ho, Wingkei

    2015-11-05

    Recently, photocatalytic CO2 reduction for solar fuel production has attracted much attention because of its potential for simultaneously solving energy and global warming problems. Many studies have been conducted to prepare novel and efficient photocatalysts for CO2 reduction. Graphene, a two-dimensional material, has been increasingly used in photocatalytic CO2 reduction. In theory, graphene shows several remarkable properties, including excellent electronic conductivity, good optical transmittance, large specific surface area, and superior chemical stability. Attributing to these advantages, fabrication of graphene-based materials has been known as one of the most feasible strategies to improve the CO2 reduction performance of photocatalysts. This Perspective mainly focuses on the recent important advances in the fabrication and application of graphene-based photocatalysts for CO2 reduction to solar fuels. The existing challenges and difficulties of graphene-based photocatalysts are also discussed for future application.

  5. International Experiences with Quantifying the Co-Benefits of Energy-Efficiency and Greenhouse-Gas Mitigation Programs and Policies

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Williams, Christopher; Hasanbeigi, Ali; Price, Lynn

    Improving the efficiency of energy production and consumption and switching to lower carbon energy sources can significantly decrease carbon dioxide (CO2) emissions and reduce climate change impacts. A growing body of research has found that these measures can also directly mitigate many non-climate change related human health hazards and environmental damage. Positive impacts of policies and programs that occur in addition to the intended primary policy goal are called co-benefits. Policy analysis relies on forecasting and comparing the costs of policy and program implementation and the benefits that accrue to society from implementation. GHG reduction and energy efficiency policies andmore » programs face political resistance in part because of the difficulty of quantifying their benefits. On the one hand, climate change mitigation policy benefits are often global, long-term, and subject to large uncertainties, and subsidized energy pricing can reduce the direct monetary benefits of energy efficiency policies to below their cost. On the other hand, the co-benefits that accrue from these efforts’ resultant reductions in conventional air pollution (such as improved health, agricultural productivity, reduced damage to infrastructure, and local ecosystem improvements) are generally near term, local, and more certain than climate change mitigation benefits and larger than the monetary value of energy savings. The incorporation of co-benefits into energy efficiency and climate mitigation policy and program analysis therefore might significantly increase the uptake of these policies. Faster policy uptake is especially important in developing countries because ongoing development efforts that do not consider co-benefits may lock in suboptimal technologies and infrastructure and result in high costs in future years. Over the past two decades, studies have repeatedly documented that non-climate change related benefits of energy efficiency and fuel conversion efforts, as a part of GHG mitigation strategies, can be from between 30% to over 100% of the costs of such policies and programs strategies. Policy makers around the world are increasingly interested in including both GHG and non-GHG impacts in analyses of energy efficiency and fuel switching policies and programs and a set of methodologies has matured from the efforts of early moving jurisdictions such as the European Union, the United States, and Japan.« less

  6. Analysis of the impact path on factors of China's energy-related CO2 emissions: a path analysis with latent variables.

    PubMed

    Chen, Wenhui; Lei, Yalin

    2017-02-01

    Identifying the impact path on factors of CO 2 emissions is crucial for the government to take effective measures to reduce carbon emissions. The most existing research focuses on the total influence of factors on CO 2 emissions without differentiating between the direct and indirect influence. Moreover, scholars have addressed the relationships among energy consumption, economic growth, and CO 2 emissions rather than estimating all the causal relationships simultaneously. To fill this research gaps and explore overall driving factors' influence mechanism on CO 2 emissions, this paper utilizes a path analysis model with latent variables (PA-LV) to estimate the direct and indirect effect of factors on China's energy-related carbon emissions and to investigate the causal relationships among variables. Three key findings emanate from the analysis: (1) The change in the economic growth pattern inhibits the growth rate of CO 2 emissions by reducing the energy intensity; (2) adjustment of industrial structure contributes to energy conservation and CO 2 emission reduction by raising the proportion of the tertiary industry; and (3) the growth of CO 2 emissions impacts energy consumption and energy intensity negatively, which results in a negative impact indirectly on itself. To further control CO 2 emissions, the Chinese government should (1) adjust the industrial structure and actively develop its tertiary industry to improve energy efficiency and develop low-carbon economy, (2) optimize population shifts to avoid excessive population growth and reduce energy consumption, and (3) promote urbanization steadily to avoid high energy consumption and low energy efficiency.

  7. Lidar measurements of the column CO2 mixing ratio made by NASA Goddard's CO2 Sounder during the NASA ASCENDS 2014 Airborne campaign.

    NASA Astrophysics Data System (ADS)

    Ramanathan, A. K.; Mao, J.; Abshire, J. B.; Kawa, S. R.

    2015-12-01

    Remote sensing measurements of CO2 from space can help improve our understanding of the carbon cycle and help constrain the global carbon budget. However, such measurements need to be sufficiently accurate to detect small (1 ppm) changes in the CO2 mixing ratio (XCO2) against a large background (~ 400 ppm). Satellite measurements of XCO2 using passive spectrometers, such as those from the Japanese GOSAT (Greenhouse gas Observing Satellite) and the NASA OCO-2 (Orbiting Carbon Observatory-2) are limited to daytime sunlit portions of the Earth and are susceptible to biases from clouds and aerosols. For this reason, NASA commissioned the formulation study of ASCENDS a space-based lidar mission. NASA Goddard Space Flight Center's CO2 Sounder lidar is one candidate approach for the ASCENDS mission. The NASA GSFC CO2 Sounder measures the CO2 mixing ratio using a pulsed multi-wavelength integrated path differential absorption (IPDA) approach. The CO2 Sounder has flown in the 2011, 2013 and 2014 ASCENDS airborne campaigns over the continental US, and has produced measurements in close agreement with in situ measurements of the CO2 column. In 2014, the CO2 Sounder upgraded its laser with a precision step-locked diode laser source to improve the lidar wavelength position accuracy. It also improved its optical receiver with a low-noise, high efficiency, HgCdTe avalanche photo diode detector. The combination of these two technologies enabled lidar XCO2 measurements with unprecedented accuracy. In this presentation, we show analysis from the ASCENDS 2014 field campaign, exploring: (1) Horizontal XCO2 gradients measured by the lidar, (2) Comparisons of lidar XCO2 measurements against the Parameterized Chemistry Transport Model (PCTM), and (3) Lidar column water vapor measurements using a HDO absorption line that occurs next to the CO2 absorption line. This can reduce the uncertainty in the dry air column used in XCO2 retrievals.

  8. Assessment of Energy Efficiency Improvement in the United States Petroleum Refining Industry

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Morrow, William R.; Marano, John; Sathaye, Jayant

    2013-02-01

    Adoption of efficient process technologies is an important approach to reducing CO 2 emissions, in particular those associated with combustion. In many cases, implementing energy efficiency measures is among the most cost-effective approaches that any refiner can take, improving productivity while reducing emissions. Therefore, careful analysis of the options and costs associated with efficiency measures is required to establish sound carbon policies addressing global climate change, and is the primary focus of LBNL’s current petroleum refining sector analysis for the U.S. Environmental Protection Agency. The analysis is aimed at identifying energy efficiency-related measures and developing energy abatement supply curves andmore » CO 2 emissions reduction potential for the U.S. refining industry. A refinery model has been developed for this purpose that is a notional aggregation of the U.S. petroleum refining sector. It consists of twelve processing units and account s for the additional energy requirements from steam generation, hydrogen production and water utilities required by each of the twelve processing units. The model is carbon and energy balanced such that crud e oil inputs and major refinery sector outputs (fuels) are benchmarked to 2010 data. Estimates of the current penetration for the identified energy efficiency measures benchmark the energy requirements to those reported in U.S. DOE 2010 data. The remaining energy efficiency potential for each of the measures is estimated and compared to U.S. DOE fuel prices resulting in estimates of cost- effective energy efficiency opportunities for each of the twelve major processes. A combined cost of conserved energy supply curve is also presented along with the CO 2 emissions abatement opportunities that exist in the U.S. petroleum refinery sector. Roughly 1,200 PJ per year of primary fuels savings and close to 500 GWh per y ear of electricity savings are potentially cost-effective given U.S. DOE fuel price forecasts. This represents roughly 70 million metric tonnes of CO 2 emission reductions assuming 2010 emissions factor for grid electricity. Energy efficiency measures resulting in an additional 400 PJ per year of primary fuels savings and close to 1,700 GWh per year of electricity savings, and an associated 24 million metric tonnes of CO 2 emission reductions are not cost-effective given the same assumption with respect to fuel prices and electricity emissions factors. Compared to the modeled energy requirements for the U.S. petroleum refining sector, the cost effective potential represents a 40% reduction in fuel consumption and a 2% reduction in electricity consumption. The non-cost-effective potential represents an additional 13% reduction in fuel consumption and an additional 7% reduction in electricity consumption. The relative energy reduction potentials are mu ch higher for fuel consumption than electricity consumption largely in part because fuel is the primary energy consumption type in the refineries. Moreover, many cost effective fuel savings measures would increase electricity consumption. The model also has the potential to be used to examine the costs and benefits of the other CO 2 mitigation options, such as combined heat and power (CHP), carbon capture, and the potential introduction of biomass feedstocks. However, these options are not addressed in this report as this report is focused on developing the modeling methodology and assessing fuels savings measures. These opportunities to further reduce refinery sector CO 2 emissions and are recommended for further research and analysis.« less

  9. Enhanced Photocatalytic Reduction of CO2 to CO through TiO2 Passivation of InP in Ionic Liquids.

    PubMed

    Zeng, Guangtong; Qiu, Jing; Hou, Bingya; Shi, Haotian; Lin, Yongjing; Hettick, Mark; Javey, Ali; Cronin, Stephen B

    2015-09-21

    A robust and reliable method for improving the photocatalytic performance of InP, which is one of the best known materials for solar photoconversion (i.e., solar cells). In this article, we report substantial improvements (up to 18×) in the photocatalytic yields for CO2 reduction to CO through the surface passivation of InP with TiO2 deposited by atomic layer deposition (ALD). Here, the main mechanisms of enhancement are the introduction of catalytically active sites and the formation of a pn-junction. Photoelectrochemical reactions were carried out in a nonaqueous solution consisting of ionic liquid, 1-ethyl-3-methylimidazolium tetrafluoroborate ([EMIM]BF4), dissolved in acetonitrile, which enables CO2 reduction with a Faradaic efficiency of 99% at an underpotential of +0.78 V. While the photocatalytic yield increases with the addition of the TiO2 layer, a corresponding drop in the photoluminescence intensity indicates the presence of catalytically active sites, which cause an increase in the electron-hole pair recombination rate. NMR spectra show that the [EMIM](+) ions in solution form an intermediate complex with CO2(-), thus lowering the energy barrier of this reaction. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  10. How Well Do We Know the Future of CO2 Emissions? Projecting Fleet Emissions from Light Duty Vehicle Technology Drivers.

    PubMed

    Martin, Niall P D; Bishop, Justin D K; Boies, Adam M

    2017-03-07

    While the UK has committed to reduce CO 2 emissions to 80% of 1990 levels by 2050, transport accounts for nearly a fourth of all emissions and the degree to which decarbonization can occur is highly uncertain. We present a new methodology using vehicle and powertrain parameters within a Bayesian framework to determine the impact of engineering vehicle improvements on fuel consumption and CO 2 emissions. Our results show how design changes in vehicle parameters (e.g., mass, engine size, and compression ratio) result in fuel consumption improvements from a fleet-wide mean of 5.6 L/100 km in 2014 to 3.0 L/100 km by 2030. The change in vehicle efficiency coupled with increases in vehicle numbers and fleet-wide activity result in a total fleet-wide reduction of 41 ± 10% in 2030, relative to 2012. Concerted internal combustion engine improvements result in a 48 ± 10% reduction of CO 2 emissions, while efforts to increase the number of diesel vehicles within the fleet had little additional effect. Increasing plug-in and all-electric vehicles reduced CO 2 emissions by less (42 ± 10% reduction) than concerted internal combustion engines improvements. However, if the grid decarbonizes, electric vehicles reduce emissions by 45 ± 9% with further reduction potential to 2050.

  11. Stability improvement of gel-state dye-sensitized solar cells by utilization the co-solvent effect of propionitrile/acetonitrile and 3-methoxypropionitrile/acetonitrile with poly(acrylonitrile-co-vinyl acetate)

    NASA Astrophysics Data System (ADS)

    Venkatesan, Shanmugam; Su, Song-Chuan; Kao, Shon-Chen; Teng, Hsisheng; Lee, Yuh-Lang

    2015-01-01

    Propionitrile (PPN) or 3-methoxypropionitrile (MPN) is mixed with acetonitrile (ACN) to prepare ACN/PPN and ACN/MPN co-solvents and used to fabricate polymer gel electrolytes (PGEs) of dye-sensitized solar cells (DSSCs), aiming at improving the stability of gel-state DSSCs. Co-solvents with various ratios are utilized to prepare PGEs using poly(acrylonitrile-co-vinyl acetate) (PAN-VA) as the gelator. The ratio effects of the co-solvents on the properties of PGEs and the performances of the corresponding DSSCs are studied. The results show that in-situ gelation of the gel-electrolytes can still be performed at the presence of 40% PPN or 30% MPN. However, increasing the composition of PPN and MPN in the co-solvents triggers a decrease in the diffusivity and conductivity of the PGEs, but an increase in the viscosity. Therefore, the energy conversion efficiencies of the cells decrease as a result. However, the introduction of PPN and MPN elevates the gel-to-liquid transition temperature (Tp) of the PGEs which significantly increases the stability of the gel-state DSSCs. Comparing between the effects of the two co-solvents, PPN and MPN have similar effect on elevation of Tp, but the conductivity of PGEs and the corresponding cell efficiency are higher for the ACN/PPN system, attributed to its lower viscosity compared with ACN/MPN system. By using the ACN/PPN (60/40) co-solvent at the presence of TiO2 fillers, gel-state cell with an efficiency of 8.3% can be achieved, which is even higher than that obtained by the liquid state cell (8%). After 500 h test at 60 °C, the cell can retain 95.4% of its initial efficiency.

  12. On the complementary relationship between marginal nitrogen and water-use efficiencies among Pinus taeda leaves grown under ambient and CO2-enriched environments

    PubMed Central

    Palmroth, Sari; Katul, Gabriel G.; Maier, Chris A.; Ward, Eric; Manzoni, Stefano; Vico, Giulia

    2013-01-01

    Background and Aims Water and nitrogen (N) are two limiting resources for biomass production of terrestrial vegetation. Water losses in transpiration (E) can be decreased by reducing leaf stomatal conductance (gs) at the expense of lowering CO2 uptake (A), resulting in increased water-use efficiency. However, with more N available, higher allocation of N to photosynthetic proteins improves A so that N-use efficiency is reduced when gs declines. Hence, a trade-off is expected between these two resource-use efficiencies. In this study it is hypothesized that when foliar concentration (N) varies on time scales much longer than gs, an explicit complementary relationship between the marginal water- and N-use efficiency emerges. Furthermore, a shift in this relationship is anticipated with increasing atmospheric CO2 concentration (ca). Methods Optimization theory is employed to quantify interactions between resource-use efficiencies under elevated ca and soil N amendments. The analyses are based on marginal water- and N-use efficiencies, λ = (∂A/∂gs)/(∂E/∂gs) and η = ∂A/∂N, respectively. The relationship between the two efficiencies and related variation in intercellular CO2 concentration (ci) were examined using A/ci curves and foliar N measured on Pinus taeda needles collected at various canopy locations at the Duke Forest Free Air CO2 Enrichment experiment (North Carolina, USA). Key Results Optimality theory allowed the definition of a novel, explicit relationship between two intrinsic leaf-scale properties where η is complementary to the square-root of λ. The data support the model predictions that elevated ca increased η and λ, and at given ca and needle age-class, the two quantities varied among needles in an approximately complementary manner. Conclusions The derived analytical expressions can be employed in scaling-up carbon, water and N fluxes from leaf to ecosystem, but also to derive transpiration estimates from those of η, and assist in predicting how increasing ca influences ecosystem water use. PMID:23299995

  13. A Model of Carbon Capture and Storage with Demonstration of Global Warming Potential and Fossil Fuel Resource Use Efficiency

    NASA Astrophysics Data System (ADS)

    Suebsiri, Jitsopa

    Increasing greenhouse gas concentration in the atmosphere influences global climate change even though the level of impact is still unclear. Carbon dioxide capture and storage (CCS) is increasingly seen as an important component of broadly based greenhouse gas reduction measures. Although the other greenhouse gases are more potent, the sheer volume of CO 2 makes it dominant in term of its effect in the atmosphere. To understand the implications, CCS activities should be studied from a full life cycle perspective. This thesis outlines the successful achievement of the objectives of this study in conducting life cycle assessment (LCA), reviewing the carbon dioxide implications only, combining two energy systems, coal-fired electrical generations and CO2 used for enhanced oil recovery (EOR). LCA is the primary approach used in this study to create a tool for CCS environmental evaluation. The Boundary Dam Power Station (BDPS) and the Weyburn-Midale CO 2 EOR Project in Saskatchewan, Canada, are studied and adopted as case scenarios to find the potential for effective application of CCS in both energy systems. This study demonstrates two levels of retrofitting of the BDPS, retrofit of unit 3 or retrofit of all units, combined with three options for CO 2 geological storage: deep saline aquifer, CO2 EOR, and a combination of deep saline aquifer storage and CO2 EOR. Energy output is considered the product of combining these two energy resources (coal and oil). Gigajoules (GJ) are used as the fundamental unit of measurement in comparing the combined energy types. The application of this tool effectively demonstrates the results of application of a CCS system concerning global warming potential (GWP) and fossil fuel resource use efficiency. Other environmental impacts could be analyzed with this tool as well. In addition, the results demonstrate that the GWP reduction is directly related to resource use efficiency. This means the lower the GWP of CCS, the lower resource use efficiency as well. Three processes, coal mining, power production including CO2 capture unit operation, and crude oil usage, must be included when the GWP of CCS is calculated. Moreover, the results from the sensitivity analysis of power generation efficiency present not only a significant reduction of GWP, but also a competitive solution for improving or at least preventing the decrease of fossil fuel resource use efficiency when CCS is applied.

  14. Thermophilic anaerobic co-digestion of garbage, screened swine and dairy cattle manure.

    PubMed

    Liu, Kai; Tang, Yue-Qin; Matsui, Toru; Morimura, Shigeru; Wu, Xiao-Lei; Kida, Kenji

    2009-01-01

    Methane fermentation characteristics of garbage, swine manure (SM), dairy cattle manure (DCM) and mixtures of these wastes were studied. SM and DCM showed much lower volatile total solid (VTS) digestion efficiencies and methane yield than those of garbage. VTS digestion efficiency of SM was significantly increased when it was co-digested with garbage (Garbage: SM=1:1). Co-digestion of garbage, SM and DCM with respect to the relative quantity of each waste discharged in the Kikuchi (1: 16: 27) and Aso (1: 19: 12) areas indicated that co-digestion with garbage would improve the digestion characteristic of SM and DCM as far as the ratio of DCM in the wastes was maintained below a certain level. When the mixed waste (Garbage: SM: DCM=1:19:12) was treated using a thermophilic UAF reactor, methanogens responsible for the methane production were Methanoculleus and Methanosarcina species. Bacterial species in the phylum Firmicutes were dominant bacteria responsible for the digestion of these wastes. As the percentage of garbage in the mixed wastes used in this study was low (2-3%) and the digestion efficiency of DCM was obviously improved, the co-digestion of SM and DCM with limited garbage was a prospective method to treat the livestock waste effectively and was an attractive alternative technology for the construction of a sustainable environment and society in stock raising area.

  15. Hybrid photosynthesis-powering biocatalysts with solar energy captured by inorganic devices.

    PubMed

    Zhang, Tian; Tremblay, Pier-Luc

    2017-01-01

    The biological reduction of CO 2 driven by sunlight via photosynthesis is a crucial process for life on earth. However, the conversion efficiency of solar energy to biomass by natural photosynthesis is low. This translates in bioproduction processes relying on natural photosynthesis that are inefficient energetically. Recently, hybrid photosynthetic technologies with the potential of significantly increasing the efficiency of solar energy conversion to products have been developed. In these systems, the reduction of CO 2 into biofuels or other chemicals of interest by biocatalysts is driven by solar energy captured with inorganic devices such as photovoltaic cells or photoelectrodes. Here, we explore hybrid photosynthesis and examine the strategies being deployed to improve this biotechnology.

  16. Engineered yeast with a CO2-fixation pathway to improve the bio-ethanol production from xylose-mixed sugars.

    PubMed

    Li, Yun-Jie; Wang, Miao-Miao; Chen, Ya-Wei; Wang, Meng; Fan, Li-Hai; Tan, Tian-Wei

    2017-03-06

    Bio-ethanol production from lignocellulosic raw materials could serve as a sustainable potential for improving the supply of liquid fuels in face of the food-to-fuel competition and the growing energy demand. Xylose is the second abundant sugar of lignocelluloses hydrolysates, but its commercial-scale conversion to ethanol by fermentation is challenged by incomplete and inefficient utilization of xylose. Here, we use a coupled strategy of simultaneous maltose utilization and in-situ carbon dioxide (CO 2 ) fixation to achieve efficient xylose fermentation by the engineered Saccharomyces cerevisiae. Our results showed that the introduction of CO 2 as electron acceptor for nicotinamide adenine dinucleotide (NADH) oxidation increased the total ethanol productivity and yield at the expense of simultaneous maltose and xylose utilization. Our achievements present an innovative strategy using CO 2 to drive and redistribute the central pathways of xylose to desirable products and demonstrate a possible breakthrough in product yield of sugars.

  17. Heterogenised Molecular Catalysts for the Reduction of CO2 to Fuels.

    PubMed

    Windle, Christopher D; Reisner, Erwin

    2015-01-01

    CO(2) conversion provides a possible solution to curtail the growing CO(2) levels in our atmosphere and reduce dependence on fossil fuels. To this end, it is essential to develop efficient catalysts for the reduction of CO(2). The structure and activity of molecular CO(2) reduction catalysts can be tuned and they offer good selectivity with reasonable stability. Heterogenisation of these molecules reduces solvent restrictions, facilitates recyclability and can dramatically improve activity by preventing catalyst inactivation and perturbing the kinetics of intermediates. The nature and morphology of the solid-state material upon which the catalyst is immobilised can significantly influence the activity of the hybrid assembly. Although work in this area began forty years ago, it has only drawn substantial attention in recent years. This review article gives an overview of the historical development of the field.

  18. Combination of Aryl Diselenides/Hydrogen Peroxide and Carbon Nanotube-Rhodium Nanohybrid for Naphthols Oxidation: An Efficient Route towards Trypanocidal Quinones.

    PubMed

    de Carvalho, Renato L; Jardim, Guilherme A M; Santos, Augusto; Araujo, Maria H; Oliveira, Willian X C; Bombaça, Ana Cristina; Menna-Barreto, Rubem F S; Gopi, Elumalai; Gravel, Edmond; Doris, Eric; da Silva Júnior, Eufrânio Nunes

    2018-06-14

    We report a combination of aryl diselenides/hydrogen peroxide and carbon nanotube-rhodium nanohybrid for naphthols oxidation towards synthesis of 1,4-naphthoquinones and evaluation of their relevant trypanocidal activity. Under a combination of (PhSe)2/H2O2 in the presence of O2 in i-PrOH/Hexane, several benzenoid (A-ring) substituted quinones were prepared in moderate to high yields. We also studied the contribution of RhCNT as co-catalyst in this process and, in some cases, yields were improved. This method provides an efficient and versatile alternative for preparing A-ring modified naphthoquinonoid compounds with relevant biological profile. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  19. DOE Office of Scientific and Technical Information (OSTI.GOV)

    Shah, Nihar K.; Wei, Max; Letschert, Virginie

    Hydrofluorocarbons (HFCs) emitted from uses such as refrigerants and thermal insulating foam, are now the fastest growing greenhouse gases (GHGs), with global warming potentials (GWP) thousands of times higher than carbon dioxide (CO2). Because of the short lifetime of these molecules in the atmosphere,1 mitigating the amount of these short-lived climate pollutants (SLCPs) provides a faster path to climate change mitigation than control of CO2 alone. This has led to proposals from Africa, Europe, India, Island States, and North America to amend the Montreal Protocol on Substances that Deplete the Ozone Layer (Montreal Protocol) to phase-down high-GWP HFCs. Simultaneously, energymore » efficiency market transformation programs such as standards, labeling and incentive programs are endeavoring to improve the energy efficiency for refrigeration and air conditioning equipment to provide life cycle cost, energy, GHG, and peak load savings. In this paper we provide an estimate of the magnitude of such GHG and peak electric load savings potential, for room air conditioning, if the refrigerant transition and energy efficiency improvement policies are implemented either separately or in parallel.« less

  20. Engineering the iron-oxidizing chemolithoautotroph Acidithiobacillus ferrooxidans for biochemical production.

    PubMed

    Kernan, Timothy; Majumdar, Sudipta; Li, Xiaozheng; Guan, Jingyang; West, Alan C; Banta, Scott

    2016-01-01

    There is growing interest in developing non-photosynthetic routes for the conversion of CO2 to fuels and chemicals. One underexplored approach is the transfer of energy to the metabolism of genetically modified chemolithoautotrophic bacteria. Acidithiobacillus ferrooxidans is an obligate chemolithoautotroph that derives its metabolic energy from the oxidation of iron or sulfur at low pH. Two heterologous biosynthetic pathways have been expressed in A. ferrooxidans to produce either isobutyric acid or heptadecane from CO2 and the oxidation of Fe(2+). A sevenfold improvement in productivity of isobutyric acid was obtained through improved media formulations in batch cultures. Steady-state efficiencies were lower in continuous cultures, likely due to ferric inhibition. If coupled to solar panels, the photon-to-fuel efficiency of this proof-of-principle process approaches estimates for agriculture-derived biofuels. These efforts lay the foundation for the utilization of this organism in the exploitation of electrical energy for biochemical synthesis. © 2015 Wiley Periodicals, Inc.

  1. Porous dendritic copper: an electrocatalyst for highly selective CO2 reduction to formate in water/ionic liquid electrolyte.

    PubMed

    Huan, Tran Ngoc; Simon, Philippe; Rousse, Gwenaëlle; Génois, Isabelle; Artero, Vincent; Fontecave, Marc

    2017-01-01

    Copper is currently extensively studied because it provides promising electrodes for carbon dioxide electroreduction. The original combination, reported here, of a nanostructured porous dendritic Cu-based material, characterized by electron microcopy (SEM, TEM) and X-ray diffraction methods, and a water/ionic liquid mixture as the solvent, contributing to CO 2 solubilization and activation, results in a remarkably efficient (large current densities at low overpotentials), stable and selective (large faradic yields) electrocatalytic system for the conversion of CO 2 into formic acid, a product with a variety of uses. These results provide new directions for the further improvement of Cu electrodes.

  2. New method of writing long-period fiber gratings using high-frequency CO2 laser

    NASA Astrophysics Data System (ADS)

    Guo, Gao-Ran; Song, Ying; Zhang, Wen-Tao; Jiang, Yue; Li, Fang

    2016-11-01

    In the paper, the Long period fiber gratings (LPFG) were fabricated in a single-mode fiber using a high frequency CO2 laser system with the point-to-point technique. The experimental setup consists of a CO2 laser controlling system, a focusing system located at a motorized linear stage, a fiber alignment stage, and an optical spectrum analyzer to monitor the transmission spectrum of the LPFG. The period of the LPFG is precisely inscribed by periodically turning on/off the laser shutter while the motorized linear stage is driven to move at a constant speed. The efficiency of fiber writing process is improved.

  3. Co3O4-x-Carbon@Fe2-yCoyO3 Heterostructural Hollow Polyhedrons for the Oxygen Evolution Reaction.

    PubMed

    Xu, Wangwang; Xie, Weiwei; Wang, Ying

    2017-08-30

    Hollow heterostructured nanomaterials have received tremendous interest in new-generation electrocatalyst applications. However, the design and fabrication of such materials remain a significant challenge. In this work, we present Co 3 O 4-x -carbon@Fe 2-y Co y O 3 heterostructural hollow polyhedrons that have been fabricated by facile thermal treatment followed by solution-phase growth for application as efficient oxygen evolution reaction (OER) electrocatalysts. Starting from a single ZIF-67 hollow polyhedron, a novel complex structured composite material constructed from Co 3 O 4-x nanocrystallite-embedded carbon matrix embedded with Fe 2-y Co y O 3 nanowires was successfully prepared. The Co 3 O 4-x nanocrystallite with oxygen vacancies provides both heterogeneous nucleation sites and growth platform for Fe 2-y Co y O 3 nanowires. The resultant heterostructure combines the advantages of Fe 2-y Co y O 3 nanowires with the large surface area and surface defects of Co 3 O 4-x nanocrystallite, resulting in improved electrocatalytic activity and electrical conductivity. As a result, such novel heterostructured OER electrocatalysts exhibit much lower onset potential (1.52 V) and higher current density (70 mA/cm 2 at 1.7 V) than Co 3 O 4-x -carbon hollow polyhedrons (onset 1.55 V, 35 mA/cm 2 at 1.7 V) and pure Co 3 O 4 hollow polyhedrons (onset 1.62 V, 5 mA/cm 2 at 1.7 V). Furthermore, the design and synthesis of metal-organic framework (MOF)-derived nanomaterials in this work offer new opportunities for developing novel and efficient electrocatalysts in electrochemical devices.

  4. Bio-inspired cofacial Fe porphyrin dimers for efficient electrocatalytic CO2 to CO conversion: Overpotential tuning by substituents at the porphyrin rings

    PubMed Central

    Zahran, Zaki N.; Mohamed, Eman A.; Naruta, Yoshinori

    2016-01-01

    Efficient reduction of CO2 into useful carbon resources particularly CO is an essential reaction for developing alternate sources of fuels and for reducing the greenhouse effect of CO2. The binuclear Ni, Fe−containing carbon monoxide dehydrogenase (CODHs) efficiently catalyzes the reduction of CO2 to CO. The location of Ni and Fe at proper positions allows their cooperation for CO2 to CO conversion through a push−pull mechanism. Bio−inspired from CODHs, we used several cofacial porphyrin dimers with different substituents as suitable ligands for holding two Fe ions with suitable Fe−Fe separation distance to efficiently and selectively promote CO2 to CO conversion with high turnover frequencies, TOFs. The substituents on the porphyrin rings greatly affect the catalysis process. By introducing electron-withdrawing/-donating groups, e.g. electron-withdrawing perfluorophenyl, at all meso positions of the porphyrin rings, the catalysis overpotential, η was minimized by ≈0.3 V compared to that obtained by introducing electron-donating mesityl groups. The Fe porphyrin dimers among reported catalysts are the most efficient ones for CO2 to CO conversion. Control experiments indicate that the high performance of the current CO2 to CO conversion catalysts is due to the presence of binuclear Fe centers at suitable Fe−Fe separation distance. PMID:27087483

  5. Bio-inspired cofacial Fe porphyrin dimers for efficient electrocatalytic CO2 to CO conversion: Overpotential tuning by substituents at the porphyrin rings.

    PubMed

    Zahran, Zaki N; Mohamed, Eman A; Naruta, Yoshinori

    2016-04-18

    Efficient reduction of CO2 into useful carbon resources particularly CO is an essential reaction for developing alternate sources of fuels and for reducing the greenhouse effect of CO2. The binuclear Ni, Fe-containing carbon monoxide dehydrogenase (CODHs) efficiently catalyzes the reduction of CO2 to CO. The location of Ni and Fe at proper positions allows their cooperation for CO2 to CO conversion through a push-pull mechanism. Bio-inspired from CODHs, we used several cofacial porphyrin dimers with different substituents as suitable ligands for holding two Fe ions with suitable Fe-Fe separation distance to efficiently and selectively promote CO2 to CO conversion with high turnover frequencies, TOFs. The substituents on the porphyrin rings greatly affect the catalysis process. By introducing electron-withdrawing/-donating groups, e.g. electron-withdrawing perfluorophenyl, at all meso positions of the porphyrin rings, the catalysis overpotential, η was minimized by ≈0.3 V compared to that obtained by introducing electron-donating mesityl groups. The Fe porphyrin dimers among reported catalysts are the most efficient ones for CO2 to CO conversion. Control experiments indicate that the high performance of the current CO2 to CO conversion catalysts is due to the presence of binuclear Fe centers at suitable Fe-Fe separation distance.

  6. Bio-inspired cofacial Fe porphyrin dimers for efficient electrocatalytic CO2 to CO conversion: Overpotential tuning by substituents at the porphyrin rings

    NASA Astrophysics Data System (ADS)

    Zahran, Zaki N.; Mohamed, Eman A.; Naruta, Yoshinori

    2016-04-01

    Efficient reduction of CO2 into useful carbon resources particularly CO is an essential reaction for developing alternate sources of fuels and for reducing the greenhouse effect of CO2. The binuclear Ni, Fe-containing carbon monoxide dehydrogenase (CODHs) efficiently catalyzes the reduction of CO2 to CO. The location of Ni and Fe at proper positions allows their cooperation for CO2 to CO conversion through a push-pull mechanism. Bio-inspired from CODHs, we used several cofacial porphyrin dimers with different substituents as suitable ligands for holding two Fe ions with suitable Fe-Fe separation distance to efficiently and selectively promote CO2 to CO conversion with high turnover frequencies, TOFs. The substituents on the porphyrin rings greatly affect the catalysis process. By introducing electron-withdrawing/-donating groups, e.g. electron-withdrawing perfluorophenyl, at all meso positions of the porphyrin rings, the catalysis overpotential, η was minimized by ≈0.3 V compared to that obtained by introducing electron-donating mesityl groups. The Fe porphyrin dimers among reported catalysts are the most efficient ones for CO2 to CO conversion. Control experiments indicate that the high performance of the current CO2 to CO conversion catalysts is due to the presence of binuclear Fe centers at suitable Fe-Fe separation distance.

  7. Carbon and water vapor fluxes of different ecosystems in Oklahoma

    USDA-ARS?s Scientific Manuscript database

    Information on exchange of energy, carbon dioxide (CO2), and water vapor (H2O) for major terrestrial ecosystems is vital to quantify carbon and water balances on a large-scale. It is also necessary to develop, test, and improve crop models and satellite-based production efficiency and evapotranspira...

  8. Chemical Reactions of Portland Cement with Aqueous CO2 and Their Impacts on Cement's Mechanical Properties under Geologic CO2 Sequestration Conditions.

    PubMed

    Li, Qingyun; Lim, Yun Mook; Flores, Katharine M; Kranjc, Kelly; Jun, Young-Shin

    2015-05-19

    To provide information on wellbore cement integrity in the application of geologic CO2 sequestration (GCS), chemical and mechanical alterations were analyzed for cement paste samples reacted for 10 days under GCS conditions. The reactions were at 95 °C and had 100 bar of either N2 (control condition) or CO2 contacting the reaction brine solution with an ionic strength of 0.5 M adjusted by NaCl. Chemical analyses showed that the 3.0 cm × 1.1 cm × 0.3 cm samples were significantly attacked by aqueous CO2 and developed layer structures with a total attacked depth of 1220 μm. Microscale mechanical property analyses showed that the hardness and indentation modulus of the carbonated layer were 2-3 times greater than for the intact cement, but those in the portlandite-dissolved region decreased by ∼50%. The strength and elastic modulus of the bulk cement samples were reduced by 93% and 84%, respectively. The properties of the microscale regions, layer structure, microcracks, and swelling of the outer layers combined to affect the overall mechanical properties. These findings improve understanding of wellbore integrity from both chemical and mechanical viewpoints and can be utilized to improve the safety and efficiency of CO2 storage.

  9. Scatter-Reducing Sounding Filtration Using a Genetic Algorithm and Mean Monthly Standard Deviation

    NASA Technical Reports Server (NTRS)

    Mandrake, Lukas

    2013-01-01

    Retrieval algorithms like that used by the Orbiting Carbon Observatory (OCO)-2 mission generate massive quantities of data of varying quality and reliability. A computationally efficient, simple method of labeling problematic datapoints or predicting soundings that will fail is required for basic operation, given that only 6% of the retrieved data may be operationally processed. This method automatically obtains a filter designed to reduce scatter based on a small number of input features. Most machine-learning filter construction algorithms attempt to predict error in the CO2 value. By using a surrogate goal of Mean Monthly STDEV, the goal is to reduce the retrieved CO2 scatter rather than solving the harder problem of reducing CO2 error. This lends itself to improved interpretability and performance. This software reduces the scatter of retrieved CO2 values globally based on a minimum number of input features. It can be used as a prefilter to reduce the number of soundings requested, or as a post-filter to label data quality. The use of the MMS (Mean Monthly Standard deviation) provides a much cleaner, clearer filter than the standard ABS(CO2-truth) metrics previously employed by competitor methods. The software's main strength lies in a clearer (i.e., fewer features required) filter that more efficiently reduces scatter in retrieved CO2 rather than focusing on the more complex (and easily removed) bias issues.

  10. Effects of water quality and dietary potassium on performance and carcass characteristics of yearling steers.

    PubMed

    Sexson, J L; Wagner, J J; Engle, T E; Spears, J W

    2010-01-01

    Four hundred thirty-two crossbred yearling steers (339 kg +/- 4.8) were used to investigate the effects of water quality and dietary potassium concentration and source on feedlot performance and carcass merit. The study was conducted using a 2 x 3 factorial treatment arrangement. Factors evaluated included 2 water sources: 1) a blend of reverse osmosis and well water (RO; 608 +/- 164 mg/L of SO(4)) and 2) 100% well water with SO(4) concentration of 1,933 +/- 53 mg/L and 3 dietary K treatments. Potassium treatments included 0.75% K with supplemental K from potassium chloride (0.75% K-KCl), 0.75% K with supplemental K from potassium carbonate (0.75% K-K(2)CO(3)), and 1.0% K with supplemental K from potassium carbonate (1.0% K-K(2)CO(3)). Interactions between water quality and dietary treatments were not significant. Dry matter intake tended (P = 0.10) to be greater for steers consuming RO water compared with well water and was not affected by dietary treatment. Feed efficiency (P = 0.04) and NE(g) recovery (P = 0.04) were greater for 1.0% K-K(2)CO(3) compared with 0.75% K-KCl but were not affected by water quality. Final BW was heavier (P < 0.001) and ADG was greater (P = 0.04) for RO water compared with well water but were not affected by diet. Carcasses from steers that consumed RO water tended (P = 0.08) to be heavier than carcasses from steers consuming well water. Dietary treatment did not affect HCW (P = 0.52). Yield grade calculated from carcass measurements was not affected by dietary treatment or water quality. Carcasses from steers consuming well water had greater (P = 0.04) marbling scores than RO water. These data demonstrate that steers consuming RO water achieved improved feedlot performance. Steers fed 1.0% K-K(2)CO(3) were more efficient and demonstrated improved energy recovery compared with steers fed 0.75% K-KCl. Improved efficiency and energy recovery may be related to a reduction (P = 0.06) in the liver abscess rate for steers consuming 1.0% K-K(2)CO(3). Dietary cation-anion balance was positively related to ADG (P < 0.01) and NE(g) (P = 0.03) recovery but negatively related to marbling score (P = 0.04).

  11. Modeling of Single and Dual Reservoir Porous Media Compressed Gas (Air and CO2) Storage Systems

    NASA Astrophysics Data System (ADS)

    Oldenburg, C. M.; Liu, H.; Borgia, A.; Pan, L.

    2017-12-01

    Intermittent renewable energy sources are causing increasing demand for energy storage. The deep subsurface offers promising opportunities for energy storage because it can safely contain high-pressure gases. Porous media compressed air energy storage (PM-CAES) is one approach, although the only facilities in operation are in caverns (C-CAES) rather than porous media. Just like in C-CAES, PM-CAES operates generally by injecting working gas (air) through well(s) into the reservoir compressing the cushion gas (existing air in the reservoir). During energy recovery, high-pressure air from the reservoir is mixed with fuel in a combustion turbine to produce electricity, thereby reducing compression costs. Unlike in C-CAES, the storage of energy in PM-CAES occurs variably across pressure gradients in the formation, while the solid grains of the matrix can release/store heat. Because air is the working gas, PM-CAES has fairly low thermal efficiency and low energy storage density. To improve the energy storage density, we have conceived and modeled a closed-loop two-reservoir compressed CO2 energy storage system. One reservoir is the low-pressure reservoir, and the other is the high-pressure reservoir. CO2 is cycled back and forth between reservoirs depending on whether energy needs to be stored or recovered. We have carried out thermodynamic and parametric analyses of the performance of an idealized two-reservoir CO2 energy storage system under supercritical and transcritical conditions for CO2 using a steady-state model. Results show that the transcritical compressed CO2 energy storage system has higher round-trip efficiency and exergy efficiency, and larger energy storage density than the supercritical compressed CO2 energy storage. However, the configuration of supercritical compressed CO2 energy storage is simpler, and the energy storage densities of the two systems are both higher than that of PM-CAES, which is advantageous in terms of storage volume for a given power rating.

  12. Towards Carbon-Neutral CO2 Conversion to Hydrocarbons.

    PubMed

    Mattia, Davide; Jones, Matthew D; O'Byrne, Justin P; Griffiths, Owen G; Owen, Rhodri E; Sackville, Emma; McManus, Marcelle; Plucinski, Pawel

    2015-12-07

    With fossil fuels still predicted to contribute close to 80 % of the primary energy consumption by 2040, methods to limit further CO2 emissions in the atmosphere are urgently needed to avoid the catastrophic scenarios associated with global warming. In parallel with improvements in energy efficiency and CO2 storage, the conversion of CO2 has emerged as a complementary route with significant potential. In this work we present the direct thermo-catalytic conversion of CO2 to hydrocarbons using a novel iron nanoparticle-carbon nanotube (Fe@CNT) catalyst. We adopted a holistic and systematic approach to CO2 conversion by integrating process optimization-identifying reaction conditions to maximize conversion and selectivity towards long chain hydrocarbons and/or short olefins-with catalyst optimization through the addition of promoters. The result is the production of valuable hydrocarbons in a manner that can approach carbon neutrality under realistic industrial process conditions. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  13. Surface Ligand Promotion of Carbon Dioxide Reduction through Stabilizing Chemisorbed Reactive Intermediates.

    PubMed

    Wang, Zhijiang; Wu, Lina; Sun, Kun; Chen, Ting; Jiang, Zhaohua; Cheng, Tao; Goddard, William A

    2018-05-23

    We have explored functionalizing metal catalysts with surface ligands as an approach to facilitate electrochemical carbon dioxide reduction reaction (CO 2 RR). To provide a molecular level understanding of the mechanism by which this enhancement occurs, we combine in situ spectroscopy analysis with an interpretation based on quantum mechanics (QM) calculations. We find that a surface ligand can play a critical role in stabilizing the chemisorbed CO 2 , which facilitates CO 2 activation and leads to a 0.3 V decrease in the overpotential for carbon monoxide (CO) formation. Moreover, the presence of the surface ligand leads to nearly exclusive CO production. At -0.6 V (versus reversible hydrogen electrode, RHE), CO is the only significant product with a faradic efficiency of 93% and a current density of 1.9 mA cm -2 . This improvement corresponds to 53-fold enhancement in turnover frequency compared with the Ag nanoparticles (NPs) without surface ligands.

  14. Remote operated vehicle with CO{sub 2} blasting (ROVCO{sub 2}): Volume 1. Final report, September 1993--July 1996

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    NONE

    1996-06-01

    This report documents the second phase of the Remote Operated Vehicle with CO{sub 2} Blasting (ROVCO{sub 2}) Program. The ROVCO{sub 2} Program`s goal is to develop and demonstrate a tool to improve the productivity of concrete floor decontamination. The second phase integrated non-developmental subsystems on to the ROVCO{sub 2} system and performed quantitative decontamination effectiveness, productivity, and reliability testings. The report documents these development activities and the analysis of cost and performance. The results show that the ROVCO{sub 2} system is an efficient decontamination tool.

  15. Effect of Nozzle Geometry on the Microstructure and Properties of HVAF-Sprayed WC-10Co4Cr and Cr3C2-25NiCr Coatings

    NASA Astrophysics Data System (ADS)

    Matikainen, V.; Koivuluoto, H.; Vuoristo, P.; Schubert, J.; Houdková, Š.

    2018-04-01

    Thermally sprayed hard metal coatings are the industrial standard solution for numerous demanding applications to improve wear resistance. In the aim of improving coating quality by utilising finer particle size distributions, several approaches have been studied to control the spray temperature. The most viable solution is to use the modern high velocity air-fuel (HVAF) spray process, which has already proven to produce high-quality coatings with dense structures. In HVAF spray process, the particle heating and acceleration can be efficiently controlled by changing the nozzle geometry. In this study, fine WC-10Co4Cr and Cr3C2-25NiCr powders were sprayed with three nozzle geometries to investigate their effect on the particle temperature, velocity and coating microstructure. The study demonstrates that the particle melting and resulting carbide dissolution can be efficiently controlled by changing the nozzle geometry from cylindrical to convergent-divergent. Moreover, the average particle velocity was increased from 780 to over 900 m/s. The increase in particle velocity significantly improved the coating structure and density. Further evaluation was carried out to resolve the effect of particle in-flight parameters on coating structure and cavitation erosion resistance, which was significantly improved in the case of WC-10Co4Cr coatings with the increasing average particle velocity.

  16. Design of a secondary ionization target for direct production of a C- beam from CO2 pulses for online AMS.

    PubMed

    Salazar, Gary; Ognibene, Ted

    2013-01-01

    We designed and optimized a novel device "target" that directs a CO 2 gas pulse onto a Ti surface where a Cs + beam generates C - from the CO 2 . This secondary ionization target enables an accelerator mass spectrometer to ionize pulses of CO 2 in the negative mode to measure 14 C/ 12 C isotopic ratios in real time. The design of the targets were based on computational flow dynamics, ionization mechanism and empirical optimization. As part of the ionization mechanism, the adsorption of CO 2 on the Ti surface was fitted with the Jovanovic-Freundlich isotherm model using empirical and simulation data. The inferred adsorption constants were in good agreement with other works. The empirical optimization showed that amount of injected carbon and the flow speed of the helium carrier gas improve the ionization efficiency and the amount of 12 C - produced until reaching a saturation point. Linear dynamic range between 150 and 1000 ng of C and optimum carrier gas flow speed of around 0.1 mL/min were shown. It was also shown that the ionization depends on the area of the Ti surface and Cs + beam cross-section. A range of ionization efficiency of 1-2.5% was obtained by optimizing the described parameters.

  17. Electron density modulation of NiCo2S4 nanowires by nitrogen incorporation for highly efficient hydrogen evolution catalysis.

    PubMed

    Wu, Yishang; Liu, Xiaojing; Han, Dongdong; Song, Xianyin; Shi, Lei; Song, Yao; Niu, Shuwen; Xie, Yufang; Cai, Jinyan; Wu, Shaoyang; Kang, Jian; Zhou, Jianbin; Chen, Zhiyan; Zheng, Xusheng; Xiao, Xiangheng; Wang, Gongming

    2018-04-12

    Metal sulfides for hydrogen evolution catalysis typically suffer from unfavorable hydrogen desorption properties due to the strong interaction between the adsorbed H and the intensely electronegative sulfur. Here, we demonstrate a general strategy to improve the hydrogen evolution catalysis of metal sulfides by modulating the surface electron densities. The N modulated NiCo 2 S 4 nanowire arrays exhibit an overpotential of 41 mV at 10 mA cm -2 and a Tafel slope of 37 mV dec -1 , which are very close to the performance of the benchmark Pt/C in alkaline condition. X-ray photoelectron spectroscopy, synchrotron-based X-ray absorption spectroscopy, and density functional theory studies consistently confirm the surface electron densities of NiCo 2 S 4 have been effectively manipulated by N doping. The capability to modulate the electron densities of the catalytic sites could provide valuable insights for the rational design of highly efficient catalysts for hydrogen evolution and beyond.

  18. Designing overall stoichiometric conversions and intervening metabolic reactions

    DOE PAGES

    Chowdhury, Anupam; Maranas, Costas D.

    2015-11-04

    Existing computational tools for de novo metabolic pathway assembly, either based on mixed integer linear programming techniques or graph-search applications, generally only find linear pathways connecting the source to the target metabolite. The overall stoichiometry of conversion along with alternate co-reactant (or co-product) combinations is not part of the pathway design. Therefore, global carbon and energy efficiency is in essence fixed with no opportunities to identify more efficient routes for recycling carbon flux closer to the thermodynamic limit. Here, we introduce a two-stage computational procedure that both identifies the optimum overall stoichiometry (i.e., optStoic) and selects for (non-)native reactions (i.e.,more » minRxn/minFlux) that maximize carbon, energy or price efficiency while satisfying thermodynamic feasibility requirements. Implementation for recent pathway design studies identified non-intuitive designs with improved efficiencies. Specifically, multiple alternatives for non-oxidative glycolysis are generated and non-intuitive ways of co-utilizing carbon dioxide with methanol are revealed for the production of C 2+ metabolites with higher carbon efficiency.« less

  19. Fe2P as a novel efficient catalyst promoter in Pd/C system for formic acid electro-oxidation in fuel cells reaction

    NASA Astrophysics Data System (ADS)

    Wang, Fulong; Xue, Huaiguo; Tian, Zhiqun; Xing, Wei; Feng, Ligang

    2018-01-01

    Developing catalyst promoter for Pd/C catalyst is significant for the catalytic ability improvement in energy transfer related electrochemical reactions. Herein, we demonstrate Fe2P as an efficient catalyst promoter in Pd/C catalyst system for formic acid electro-oxidation in fuel cells reactions. Adding Fe2P in the Pd/C catalyst system greatly increases the performances for formic acid oxidation by 3-4 times; the CO stripping technique displays two kinds of active sites formation in the Pd-Fe2P/C catalyst system coming from the interaction of Pd, Fe2P and Pd oxide species and both are more efficient for formic acid and CO-species electrooxidation. The smaller charge transfer resistance and Tafel slope for formic acid oxidation indicate the improvements in kinetics by Fe2P in the Pd-Fe2P/C system. The nanostructured hybrid units of Pd, Fe2P and carbon are evidently visible in the high resolution microscopy images and XPS technique confirmes the electronic effect in the catalyst system. The promotion effect of Fe2P in the catalyst system arising from the structure, composition and electronic effect changes is discussed with the help from multiple physical and electrochemical techniques. It is concluded that Fe2P as a significant catalyst promoter will have potential application in energy transfer related electrochemical reactions.

  20. Bifunctional composite catalysts using Co3O4 nanofibers immobilized on nonoxidized graphene nanoflakes for high-capacity and long-cycle Li-O2 batteries.

    PubMed

    Ryu, Won-Hee; Yoon, Taek-Han; Song, Sung Ho; Jeon, Seokwoo; Park, Yong-Joon; Kim, Il-Doo

    2013-09-11

    Designing a highly efficient catalyst is essential to improve the electrochemical performance of Li-O2 batteries for long-term cycling. Furthermore, these batteries often show significant capacity fading due to the irreversible reaction characteristics of the Li2O2 product. To overcome these limitations, we propose a bifunctional composite catalyst composed of electrospun one-dimensional (1D) Co3O4 nanofibers (NFs) immobilized on both sides of the 2D nonoxidized graphene nanoflakes (GNFs) for an oxygen electrode in Li-O2 batteries. Highly conductive GNFs with noncovalent functionalization can facilitate a homogeneous dispersion in solution, thereby enabling simple and uniform attachment of 1D Co3O4 NFs on GNFs without restacking. High first discharge capacity of 10 500 mAh/g and superior cyclability for 80 cycles with a limited capacity of 1000 mAh/g were achieved by (i) improved catalytic activity of 1D Co3O4 NFs with large surface area, (ii) facile electron transport via interconnected GNFs functionalized by Co3O4 NFs, and (iii) fast O2 diffusion through the ultrathin GNF layer and porous Co3O4 NF networks.

  1. Solar Reforming of Carbon Dioxide to Produce Diesel Fuel

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Dennis Schuetzle; Robert Schuetzle

    2010-12-31

    This project focused on the demonstration of an innovative technology, referred to as the Sunexus CO2 Solar Reformer, which utilizes waste CO2 as a feedstock for the efficient and economical production of synthetic diesel fuel using solar thermal energy as the primary energy input. The Sunexus technology employs a two stage process for the conversion of CO2 to diesel fuel. A solar reforming system, including a specially designed reactor and proprietary CO2 reforming catalyst, was developed and used to convert captured CO2 rich gas streams into syngas (primarily hydrogen and carbon monoxide) using concentrated solar energy at high conversion efficiencies.more » The second stage of the system (which has been demonstrated under other funding) involves the direct conversion of the syngas into synthetic diesel fuel using a proprietary catalyst (Terra) previously developed and validated by Pacific Renewable Fuels and Chemicals (PRFC). The overall system energy efficiency for conversion of CO2 to diesel fuel is 74%, due to the use of solar energy. The results herein describe modeling, design, construction, and testing of the Sunexus CO2 Solar Reformer. Extensive parametric testing of the solar reformer and candidate catalysts was conducted and chemical kinetic models were developed. Laboratory testing of the Solar Reformer was successfully completed using various gas mixtures, temperatures, and gas flow rates/space velocities to establish performance metrics which can be employed for the design of commercial plants. A variety of laboratory tests were conducted including dry reforming (CO2 and CH{sub 4}), combination dry/steam reforming (CO2, CH{sub 4} & H{sub 2}O), and tri-reforming (CO2, CH{sub 4}, H{sub 2}O & O{sub 2}). CH{sub 4} and CO2 conversions averaged 95-100% and 50-90% per reformer cycle, respectively, depending upon the temperatures and gas space velocities. No formation of carbon deposits (coking) on the catalyst was observed in any of these tests. A 16 ft. diameter, concentrating solar dish was modified to accommodate the Sunexus CO2 Solar Reformer and the integrated system was installed at the Pacific Renewable Fuels and Chemicals test site at McClellan, CA. Several test runs were conducted without catalyst during which the ceramic heat exchanger in the Sunexus Solar Reformer reached temperatures between 1,050 F (566 C) and 2,200 F (1,204 C) during the test period. A dry reforming mixture of CO2/CH{sub 4} (2.0/1.0 molar ratio) was chosen for all of the tests on the integrated solar dish/catalytic reformer during December 2010. Initial tests were carried out to determine heat transfer from the collimated solar beam to the catalytic reactor. The catalyst was operated successfully at a steady-state temperature of 1,125 F (607 C), which was sufficient to convert 35% of the 2/1 CO2/CH{sub 4} mixture to syngas. This conversion efficiency confirmed the results from laboratory testing of this catalyst which provided comparable syngas production efficiencies (40% at 1,200 F [650 C]) with a resulting syngas composition of 20% CO, 16% H{sub 2}, 39% CO2 and 25% CH{sub 4}. As based upon the laboratory results, it is predicted that 90% of the CO2 will be converted to syngas in the solar reformer at 1,440 F (782 C) resulting in a syngas composition of 50% CO: 43% H{sub 2}: 7% CO2: 0% CH{sub 4}. Laboratory tests show that the higher catalyst operating temperature of 1,440 F (782 C) for efficient conversion of CO2 can certainly be achieved by optimizing solar reactor heat transfer, which would result in the projected 90% CO2-to-syngas conversion efficiencies. Further testing will be carried out during 2011, through other funding support, to further optimize the solar dish CO2 reformer. Additional studies carried out in support of this project and described in this report include: (1) An Assessment of Potential Contaminants in Captured CO2 from Various Industrial Processes and Their Possible Effect on Sunexus CO2 Reforming Catalysts; (2) Recommended Measurement Methods for Assessing Contaminant Levels in Captured CO2 Streams; (3) An Assessment of Current Commercial Scale Fisher-Tropsch (F-T) Technologies for the Conversion of Syngas to Fuels; (4) An Overview of CO2 Capture Technologies from Various Industrial Sources; and (5) Lifecycle Analysis for the Capture and Conversion of CO2 to Synthetic Diesel Fuel. Commercial scale Sunexus CO2 Solar Reformer plant designs, proposed in this report, should be able to utilize waste CO2 from a wide variety of industrial sources to produce a directly usable synthetic diesel fuel that replaces petroleum derived fuel, thus improving the United States energy security while also sequestering CO2. Our material balance model shows that every 5.0 lbs of CO2 is transformed using solar energy into 6.26 lbs (1.0 U.S. gallon) of diesel fuel and into by-products, which includes water. Details are provided in the mass and energy model in this report.« less

  2. TSA and BIX-01294 Induced Normal DNA and Histone Methylation and Increased Protein Expression in Porcine Somatic Cell Nuclear Transfer Embryos

    PubMed Central

    Ding, Biao; Zuo, Xiaoyuan; Li, Hui; Ding, Jianping; Li, Yunsheng; Huang, Weiping; Zhang, Yunhai

    2017-01-01

    The poor efficiency of animal cloning is mainly attributed to the defects in epigenetic reprogramming of donor cells’ chromatins during early embryonic development. Previous studies indicated that inhibition of histone deacetylases or methyltransferase, such as G9A, using Trichostatin A (TSA) or BIX-01294 significantly enhanced the developmental efficiency of porcine somatic cell nuclear transfer (SCNT) embryos. However, potential mechanisms underlying the improved early developmental competence of SCNT embryos exposed to TSA and BIX-01294 are largely unclear. Here we found that 50 nM TSA or 1.0 μM BIX-01294 treatment alone for 24 h significantly elevated the blastocyst rate (P < 0.05), while further improvement was not observed under combined treatment condition. Furthermore, co-treatment or TSA treatment alone significantly reduced H3K9me2 level at the 4-cell stage, which is comparable with that in in vivo and in vitro fertilized counterparts. However, only co-treatment significantly decreased the levels of 5mC and H3K9me2 in trophectoderm lineage and subsequently increased the expression of OCT4 and CDX2 associated with ICM and TE lineage differentiation. Altogether, these results demonstrate that co-treatment of TSA and BIX-01294 enhances the early developmental competence of porcine SCNT embryos via improvements in epigenetic status and protein expression. PMID:28114389

  3. TSA and BIX-01294 Induced Normal DNA and Histone Methylation and Increased Protein Expression in Porcine Somatic Cell Nuclear Transfer Embryos.

    PubMed

    Cao, Zubing; Hong, Renyun; Ding, Biao; Zuo, Xiaoyuan; Li, Hui; Ding, Jianping; Li, Yunsheng; Huang, Weiping; Zhang, Yunhai

    2017-01-01

    The poor efficiency of animal cloning is mainly attributed to the defects in epigenetic reprogramming of donor cells' chromatins during early embryonic development. Previous studies indicated that inhibition of histone deacetylases or methyltransferase, such as G9A, using Trichostatin A (TSA) or BIX-01294 significantly enhanced the developmental efficiency of porcine somatic cell nuclear transfer (SCNT) embryos. However, potential mechanisms underlying the improved early developmental competence of SCNT embryos exposed to TSA and BIX-01294 are largely unclear. Here we found that 50 nM TSA or 1.0 μM BIX-01294 treatment alone for 24 h significantly elevated the blastocyst rate (P < 0.05), while further improvement was not observed under combined treatment condition. Furthermore, co-treatment or TSA treatment alone significantly reduced H3K9me2 level at the 4-cell stage, which is comparable with that in in vivo and in vitro fertilized counterparts. However, only co-treatment significantly decreased the levels of 5mC and H3K9me2 in trophectoderm lineage and subsequently increased the expression of OCT4 and CDX2 associated with ICM and TE lineage differentiation. Altogether, these results demonstrate that co-treatment of TSA and BIX-01294 enhances the early developmental competence of porcine SCNT embryos via improvements in epigenetic status and protein expression.

  4. The importance of nodule CO2 fixation for the efficiency of symbiotic nitrogen fixation in pea at vegetative growth and during pod formation.

    PubMed

    Fischinger, Stephanie Anastasia; Schulze, Joachim

    2010-05-01

    Nodule CO2 fixation is of pivotal importance for N2 fixation. The process provides malate for bacteroids and oxaloacetate for nitrogen assimilation. The hypothesis of the present paper was that grain legume nodules would adapt to higher plant N demand and more restricted carbon availability at pod formation through increased nodule CO2 fixation and a more efficient N2 fixation. Growth, N2 fixation, and nodule composition during vegetative growth and at pod formation were studied in pea plants (Pisum sativum L.). In parallel experiments, 15N2 and 13CO2 uptake, as well as nodule hydrogen and CO2 release, was measured. Plants at pod formation showed higher growth rates and N2 fixation per plant when compared with vegetative growth. The specific activity of active nodules was about 25% higher at pod formation. The higher nodule activity was accompanied by higher amino acid concentration in nodules and xylem sap with a higher share of asparagine. Nodule 13CO2 fixation was increased at pod formation, both per plant and per 15N2 fixed unit. However, malate concentration in nodules was only 40% of that during vegetative growth and succinate was no longer detectable. The data indicate that increased N2 fixation at pod formation is connected with strongly increased nodule CO2 fixation. While the sugar concentration in nodules at pod formation was not altered, the concentration of organic acids, namely malate and succinate, was significantly lower. It is concluded that strategies to improve the capability of nodules to fix CO2 and form organic acids might prolong intensive N2 fixation into the later stages of pod formation and pod filling in grain legumes.

  5. Direct membrane-carbonation photobioreactor producing photoautotrophic biomass via carbon dioxide transfer and nutrient removal.

    PubMed

    Kim, Hyun-Woo; Cheng, Jing; Rittmann, Bruce E

    2016-03-01

    An advanced-material photobioreactor, the direct membrane-carbonation photobioreactor (DMCPBR), was tested to investigate the impact of directly submerging a membrane carbonation (MC) module of hollow-fiber membranes inside the photobioreactor. Results demonstrate that the DMCPBR utilized over 90% of the supplied CO2 by matching the CO2 flux to the C demand of photoautotrophic biomass growth. The surface area of the submerged MC module was the key to control CO2 delivery and biomass productivity. Tracking the fate of supplied CO2 explained how the DMCPBR reduced loss of gaseous CO2 while matching the inorganic carbon (IC) demand to its supply. Accurate fate analysis required that the biomass-associated C include soluble microbial products as a sink for captured CO2. With the CO2 supply matched to the photosynthetic demand, light attenuation limited the rate microalgal photosynthesis. The DMCPBR presents an opportunity to improve CO2-deliver efficiency and make microalgae a more effective strategy for C-neutral resource recovery. Copyright © 2015 Elsevier Ltd. All rights reserved.

  6. High Selectivity Gas Separation Membrane Assemblies

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Nachlas, Jesse; Corn, Isaac; Wegst, Ulrike

    Global energy consumption is projected to be more than double of today’s levels by 2050. Economic and environmental pressures are putting significant limits on fossil fuel resources, and there is a significant push for improved efficiency in many industrial processes. Membranes for gas separation represent a significant opportunity for reduced energy consumption and improved efficiencies in a wide range of industrial applications by replacing typical high temperature processes or energy intensive processes with low temperature energy efficient processes. Carbon membranes represent an attractive class of membrane materials that offer the potential to improve the reliability, corrosion resistance and temperature capabilitymore » of polymeric membranes, which limit their adoption for many industrial applications. However, there are still a number of technical hurdles which must be overcome before carbon membranes can be made commercially ready including elimination of manufacturing defects, and improved performance (permeability and selectivity) relative to polymeric membranes. Examples of potential application of carbon membranes include production of oxygen enriched air (OEA) for combustion applications, separation of carbon dioxide (CO 2) from flue gas to improve the commercial feasibility of CO 2 sequestration, separation of hydrogen from CO/CO 2 during hydrogen manufacturing, and separation of H 2 from hydrocarbons during refinery operations to improve the kinetics of cracking reactions. As a result of these benefits there is a strong driving force to develop processing technologies capable of producing carbon membranes and possessing high reliability, for a wide range of applications. The DOE provides significant support for research and development is this area, as they have recognized the significant impact a low cost carbon membrane technology can have on energy consumption and polluting emissions across a broad range of industrial applications. In this SBIR Phase I project, we developed a novel polymer precursor composition, which led to highly reproducible crack-free porous carbon membranes that were capable of producing 30-50% oxygen for OEA from a pressurized air feed, thereby meeting the primary Phase I objective, and possessing a selectivity of ~20:1 for CO 2/N 2 separation. We also successfully developed a method for fabricating a ceramic support from low-cost fly ash. In general, the effectiveness of a carbon membrane at separating various gases is a function of the pore structure and size. The novel processing method utilized is capable of accurately controlling pore structure during the fabrication process opening the possibility to create a membrane technology platform that can operate across a broad range of gas compositions and applications. Nanoporous carbon membrane technology offers a very attractive option for important industrial gas separation processes that are typically energy intensive and expensive to install and operate. Highly efficient gas separation represents a key enabling technology for increasing efficiency and lowering cost in various applications involving advanced power generation systems, metallurgical operations and chemical processes. These benefits will be translated to the public through lower cost for goods and services in addition to lower cost for energy. Increased national security will come from decreased dependence on imported oil by making local resources, such as coal and natural gas, competitive in energy generation markets. Finally, making low cost oxygen available in these industries results in cleaner power production and reduced emissions of polluting gases.« less

  7. Preparation of astaxanthin-loaded DNA/chitosan nanoparticles for improved cellular uptake and antioxidation capability.

    PubMed

    Wang, Qian; Zhao, Yingyuan; Guan, Lei; Zhang, Yaping; Dang, Qifeng; Dong, Ping; Li, Jing; Liang, Xingguo

    2017-07-15

    DNA/chitosan co-assemblies were initially used as nanocarriers for efficient astaxanthin encapsulation and delivery. The obtained astaxanthin-loaded DNA/chitosan (ADC) colloidal system was transparent and homogenous, with astaxanthin content up to 65μg/ml. Compared to free astaxanthin, ADC nanoparticles with an astaxanthin concentration as low as 3.35nM still showed a more powerful cytoprotective effect on H 2 O 2 -induced oxidative cell damage, and improved cell viability from 49.9% to 61.9%. The ROS scavenging efficiency of ADC nanoparticles was as high as 54.3%, which was 2-fold higher than that of free astaxanthin. Besides this, ADC nanoparticles were easily engulfed by Caco-2 cells in a short time, indicating that the encapsulated astaxanthin could be absorbed through endocytosis by intestinal epithelial cells. The improved antioxidation capability and facilitated cellular uptake enabled the ADC nanoparticles to be good candidates for efficient delivery and absorption of astaxanthin. Copyright © 2017 Elsevier Ltd. All rights reserved.

  8. What Can China Do? China's Best Alternative Outcome for Energy Efficiency and CO2 Emissions

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    G. Fridley, David; Zheng, Nina; T. Aden, Nathaniel

    After rapid growth in economic development and energy demand over the last three decades, China has undertaken energy efficiency improvement efforts to reduce its energy intensity under the 11th Five Year Plan (FYP). Since becoming the world's largest annual CO{sub 2} emitter in 2007, China has set reduction targets for energy and carbon intensities and committed to meeting 15% of its total 2020 energy demand with non-fossil fuel. Despite having achieved important savings in 11th FYP efficiency programs, rising per capita income and the continued economic importance of trade will drive demand for transport activity and fuel use. At themore » same time, an increasingly 'electrified' economy will drive rapid power demand growth. Greater analysis is therefore needed to understand the underlying drivers, possible trajectories and mitigation potential in the growing industrial, transport and power sectors. This study uses scenario analysis to understand the likely trajectory of China's energy and carbon emissions to 2030 in light of the current and planned portfolio of programs, policies and technology development and ongoing urbanization and demographic trends. It evaluates the potential impacts of alternative transportation and power sector development using two key scenarios, Continued Improvement Scenario (CIS) and Accelerated Improvement Scenario (AIS). CIS represents the most likely path of growth based on continuation of current policies and meeting announced targets and goals, including meeting planned appliance efficiency standard revisions, fuel economy standards, and industrial targets and moderate phase-out of subcritical coal-fired generation with additional non-fossil generation. AIS represents a more aggressive trajectory of accelerated improvement in energy intensity and decarbonized power and transport sectors. A range of sensitivity analysis and power technology scenarios are tested to evaluate the impact of additional actions such as carbon capture and sequestration (CCS) and integrated mine-mouth generation. The CIS and AIS results are also contextualized and compared to model scenarios in other published studies. The results of this study show that China's energy and CO{sub 2} emissions will not likely peak before 2030, although growth is expected to slow after 2020. Moreover, China will be able to meet its 2020 carbon intensity reduction target of 40 to 45% under both CIS and AIS, but only meet its 15% non-fossil fuel target by 2020 under AIS. Under both scenarios, efficiency remains a key resource and has the same, if not greater, mitigation potential as new technologies in transport and power sectors. In the transport sector, electrification will be closely linked the degree of decarbonization in the power sector and EV deployment has little or no impact on China's crude oil import demand. Rather, power generation improvements have the largest sector potential for overall emission mitigation while mine-mouth power generation and CCS have limited mitigation potential compared to fuel switching and efficiency improvements. Comparisons of this study's results with other published studies reveal that CIS and AIS are within the range of other national energy projections but alternative studies rely much more heavily on CCS for carbon reduction. The McKinsey study, in particular, has more optimistic assumptions for reductions in crude oil imports and coal demand in its abatement scenario and has much higher gasoline reduction potential for the same level of EV deployment. Despite these differences, this study's scenario analysis of both transport and power sectors illustrate the necessity for continued efficiency improvements and aggressive power sector decarbonization in flattening China's CO{sub 2} emissions.« less

  9. Biosurfactant as an Enhancer of Geologic Carbon Storage: Microbial Modification of Interfacial Tension and Contact Angle in Carbon dioxide/Water/Quartz Systems.

    PubMed

    Park, Taehyung; Joo, Hyun-Woo; Kim, Gyeong-Yeong; Kim, Seunghee; Yoon, Sukhwan; Kwon, Tae-Hyuk

    2017-01-01

    Injecting and storing of carbon dioxide (CO 2 ) in deep geologic formations is considered as one of the promising approaches for geologic carbon storage. Microbial wettability alteration of injected CO 2 is expected to occur naturally by microorganisms indigenous to the geologic formation or microorganisms intentionally introduced to increase CO 2 storage capacity in the target reservoirs. The question as to the extent of microbial CO 2 wettability alteration under reservoir conditions still warrants further investigation. This study investigated the effect of a lipopeptide biosurfactant-surfactin, on interfacial tension (IFT) reduction and contact angle alteration in CO 2 /water/quartz systems under a laboratory setup simulating in situ reservoir conditions. The temporal shifts in the IFT and the contact angle among CO 2 , brine, and quartz were monitored for different CO 2 phases (3 MPa, 30°C for gaseous CO 2 ; 10 MPa, 28°C for liquid CO 2 ; 10 MPa, 37°C for supercritical CO 2 ) upon cultivation of Bacillus subtilis strain ATCC6633 with induced surfactin secretion activity. Due to the secreted surfactin, the IFT between CO 2 and brine decreased: from 49.5 to 30 mN/m, by ∼39% for gaseous CO 2 ; from 28.5 to 13 mN/m, by 54% for liquid CO 2 ; and from 32.5 to 18.5 mN/m, by ∼43% for supercritical CO 2 , respectively. The contact angle of a CO 2 droplet on a quartz disk in brine increased: from 20.5° to 23.2°, by 1.16 times for gaseous CO 2 ; from 18.4° to 61.8°, by 3.36 times for liquid CO 2 ; and from 35.5° to 47.7°, by 1.34 times for supercritical CO 2 , respectively. With the microbially altered CO 2 wettability, improvement in sweep efficiency of injected and displaced CO 2 was evaluated using 2-D pore network model simulations; again the increment in sweep efficiency was the greatest in liquid CO 2 phase due to the largest reduction in capillary factor. This result provides novel insights as to the role of naturally occurring biosurfactants in CO 2 storage and suggests that biostimulation of biosurfactant production may be a feasible technique for enhancement of CO 2 storage capacity.

  10. Biosurfactant as an Enhancer of Geologic Carbon Storage: Microbial Modification of Interfacial Tension and Contact Angle in Carbon dioxide/Water/Quartz Systems

    PubMed Central

    Park, Taehyung; Joo, Hyun-Woo; Kim, Gyeong-Yeong; Kim, Seunghee; Yoon, Sukhwan; Kwon, Tae-Hyuk

    2017-01-01

    Injecting and storing of carbon dioxide (CO2) in deep geologic formations is considered as one of the promising approaches for geologic carbon storage. Microbial wettability alteration of injected CO2 is expected to occur naturally by microorganisms indigenous to the geologic formation or microorganisms intentionally introduced to increase CO2 storage capacity in the target reservoirs. The question as to the extent of microbial CO2 wettability alteration under reservoir conditions still warrants further investigation. This study investigated the effect of a lipopeptide biosurfactant—surfactin, on interfacial tension (IFT) reduction and contact angle alteration in CO2/water/quartz systems under a laboratory setup simulating in situ reservoir conditions. The temporal shifts in the IFT and the contact angle among CO2, brine, and quartz were monitored for different CO2 phases (3 MPa, 30°C for gaseous CO2; 10 MPa, 28°C for liquid CO2; 10 MPa, 37°C for supercritical CO2) upon cultivation of Bacillus subtilis strain ATCC6633 with induced surfactin secretion activity. Due to the secreted surfactin, the IFT between CO2 and brine decreased: from 49.5 to 30 mN/m, by ∼39% for gaseous CO2; from 28.5 to 13 mN/m, by 54% for liquid CO2; and from 32.5 to 18.5 mN/m, by ∼43% for supercritical CO2, respectively. The contact angle of a CO2 droplet on a quartz disk in brine increased: from 20.5° to 23.2°, by 1.16 times for gaseous CO2; from 18.4° to 61.8°, by 3.36 times for liquid CO2; and from 35.5° to 47.7°, by 1.34 times for supercritical CO2, respectively. With the microbially altered CO2 wettability, improvement in sweep efficiency of injected and displaced CO2 was evaluated using 2-D pore network model simulations; again the increment in sweep efficiency was the greatest in liquid CO2 phase due to the largest reduction in capillary factor. This result provides novel insights as to the role of naturally occurring biosurfactants in CO2 storage and suggests that biostimulation of biosurfactant production may be a feasible technique for enhancement of CO2 storage capacity. PMID:28744272

  11. Plant RuBisCo assembly in E. coli with five chloroplast chaperones including BSD2.

    PubMed

    Aigner, H; Wilson, R H; Bracher, A; Calisse, L; Bhat, J Y; Hartl, F U; Hayer-Hartl, M

    2017-12-08

    Plant RuBisCo, a complex of eight large and eight small subunits, catalyzes the fixation of CO 2 in photosynthesis. The low catalytic efficiency of RuBisCo provides strong motivation to reengineer the enzyme with the goal of increasing crop yields. However, genetic manipulation has been hampered by the failure to express plant RuBisCo in a bacterial host. We achieved the functional expression of Arabidopsis thaliana RuBisCo in Escherichia coli by coexpressing multiple chloroplast chaperones. These include the chaperonins Cpn60/Cpn20, RuBisCo accumulation factors 1 and 2, RbcX, and bundle-sheath defective-2 (BSD2). Our structural and functional analysis revealed the role of BSD2 in stabilizing an end-state assembly intermediate of eight RuBisCo large subunits until the small subunits become available. The ability to produce plant RuBisCo recombinantly will facilitate efforts to improve the enzyme through mutagenesis. Copyright © 2017 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.

  12. Supercritical CO2 foamed polycaprolactone scaffolds for controlled delivery of 5-fluorouracil, nicotinamide and triflusal.

    PubMed

    Salerno, Aurelio; Saurina, Javier; Domingo, Concepción

    2015-12-30

    The manufacture of porous polycaprolactone (PCL) scaffolds containing three different drugs, namely 5-fluorouracil, nicotinamide and triflusal, was investigated in this work with the aim of obtaining bioactive systems with controlled drug delivery capabilities. The scaffolds were prepared by means of a supercritical CO2 (scCO2) foaming technique by optimizing the drug loading process. This was achieved by dissolving the drugs in organic solvents miscible with scCO2 and by mixing these drug/solvent solutions with PCL powder. The as prepared mixtures were further compressed to eliminate air bubbles and finally processed by the scCO2 foaming technique. ScCO2 saturation and foaming conditions were optimized to create the porosity within the samples and to allow for the concomitant removal of the organic solvents. Physical and chemical properties of porous scaffolds, as well as drug content and delivery profiles, were studied by HPLC. The results of this study demonstrated that the composition of the starting PCL/drug/solvent mixtures affected polymer crystallization, scaffold morphology and pore structure features. Furthermore, it was found that drug loading efficiency depended on both initial solution composition and drug solubility in scCO2. Nevertheless, in the case of highly scCO2-soluble drugs, such as triflusal, loading efficiency was improved by adding a proper amount of free drug inside of the pressure vessel. The drug delivery study indicated that release profiles depended mainly upon scaffolds composition and pore structure features. Copyright © 2015 Elsevier B.V. All rights reserved.

  13. Efficient parallel simulation of CO2 geologic sequestration insaline aquifers

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Zhang, Keni; Doughty, Christine; Wu, Yu-Shu

    2007-01-01

    An efficient parallel simulator for large-scale, long-termCO2 geologic sequestration in saline aquifers has been developed. Theparallel simulator is a three-dimensional, fully implicit model thatsolves large, sparse linear systems arising from discretization of thepartial differential equations for mass and energy balance in porous andfractured media. The simulator is based on the ECO2N module of the TOUGH2code and inherits all the process capabilities of the single-CPU TOUGH2code, including a comprehensive description of the thermodynamics andthermophysical properties of H2O-NaCl- CO2 mixtures, modeling singleand/or two-phase isothermal or non-isothermal flow processes, two-phasemixtures, fluid phases appearing or disappearing, as well as saltprecipitation or dissolution. The newmore » parallel simulator uses MPI forparallel implementation, the METIS software package for simulation domainpartitioning, and the iterative parallel linear solver package Aztec forsolving linear equations by multiple processors. In addition, theparallel simulator has been implemented with an efficient communicationscheme. Test examples show that a linear or super-linear speedup can beobtained on Linux clusters as well as on supercomputers. Because of thesignificant improvement in both simulation time and memory requirement,the new simulator provides a powerful tool for tackling larger scale andmore complex problems than can be solved by single-CPU codes. Ahigh-resolution simulation example is presented that models buoyantconvection, induced by a small increase in brine density caused bydissolution of CO2.« less

  14. Efficient formation of benzylic quaternary centers via palladium catalysis.

    PubMed

    Gottumukkala, Aditya L; Suljagic, Jasmin; Matcha, Kiran; de Vries, Johannes G; Minnaard, Adriaan J

    2013-09-01

    Four's a crowd: An efficient protocol for the formation of benzylic quaternary centers via arylation of enones using a catalyst made from Pd(O2 CCF3 )2 and 2,2'-bipyridine is developed. For cyclic substrates, catalyst loadings as low as 1 mol % Pd are enough to afford excellent yields (>90%) using a variety of arylboronic acids. In case of acyclic substrates, the addition of KSbF6 was found to improve conversions and yields. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  15. Catalytic Hydrogenation of Carbon Dioxide with Ammonia-Borane by Pincer-type Phosphorus Compound: A Theoretical Prediction.

    PubMed

    Zeng, Guixiang; Maeda, Satoshi; Taketsugu, Tetsuya; Sakaki, Shigeyoshi

    2016-10-01

    Theoretically designed pincer-type phosphorus compound is found to be active for the hydrogenation of carbon dioxide (CO 2 ) with ammonia-borane. DFT, ONIOM(CCSD(T):MP2), and CCSD(T) computational results demonstrated that the reaction occurs through the phosphorus-ligand cooperative catalysis function, which provides an unprecedented protocol for metal-free CO 2 conversion. The phosphorus compounds with the NNN ligand are more active than those with the ONO ligand. The conjugate and planar ligand considerably improves the efficiency of the catalyst.

  16. Current and Future Greenhouse Gas Emissions from Global Crop Intensification and Expansion

    NASA Astrophysics Data System (ADS)

    Carlson, K. M.; Gerber, J. S.; Mueller, N. D.; O'Connell, C.; West, P. C.

    2014-12-01

    Food systems currently contribute up to one-third of total anthropogenic greenhouse gas emissions, and these emissions are expected to rise as demand for agricultural products increases. Thus, improving the greenhouse gas emissions efficiency of agriculture - the tons or kilocalories of production per ton of CO2 equivalent emissions - will be critical to support a resilient future global system. Here, we model and evaluate global, 2000-era, spatially explicit relationships between a suite of greenhouse gas emissions from various agronomic practices (i.e., fertilizer application, peatland draining, and rice cultivation) and crop yields. Then, we predict potential emissions from future crop production increases achieved through intensification and extensification, including CO2 emissions from croplands replacing non-urban land cover. We find that 2000-era yield-scaled agronomic emissions are highly heterogeneous across crops types, crop management practices, and regions. Rice agriculture produces more total CO2-equivalent emissions than any other crop. Moreover, inundated rice in just a few countries contributes the vast majority of these rice emissions. Crops such as sunflower and cotton have low efficiency on a caloric basis. Our results suggest that intensification tends to be a more efficient pathway to boost greenhouse gas emissions efficiency than expansion. We conclude by discussing potential crop- and region-specific agricultural development pathways that may boost the greenhouse gas emissions efficiency of agriculture.

  17. Robust RNAi enhancement via human Argonaute-2 overexpression from plasmids, viral vectors and cell lines

    PubMed Central

    Börner, Kathleen; Niopek, Dominik; Cotugno, Gabriella; Kaldenbach, Michaela; Pankert, Teresa; Willemsen, Joschka; Zhang, Xian; Schürmann, Nina; Mockenhaupt, Stefan; Serva, Andrius; Hiet, Marie-Sophie; Wiedtke, Ellen; Castoldi, Mirco; Starkuviene, Vytaute; Erfle, Holger; Gilbert, Daniel F.; Bartenschlager, Ralf; Boutros, Michael; Binder, Marco; Streetz, Konrad; Kräusslich, Hans-Georg; Grimm, Dirk

    2013-01-01

    As the only mammalian Argonaute protein capable of directly cleaving mRNAs in a small RNA-guided manner, Argonaute-2 (Ago2) is a keyplayer in RNA interference (RNAi) silencing via small interfering (si) or short hairpin (sh) RNAs. It is also a rate-limiting factor whose saturation by si/shRNAs limits RNAi efficiency and causes numerous adverse side effects. Here, we report a set of versatile tools and widely applicable strategies for transient or stable Ago2 co-expression, which overcome these concerns. Specifically, we engineered plasmids and viral vectors to co-encode a codon-optimized human Ago2 cDNA along with custom shRNAs. Furthermore, we stably integrated this Ago2 cDNA into a panel of standard human cell lines via plasmid transfection or lentiviral transduction. Using various endo- or exogenous targets, we demonstrate the potential of all three strategies to boost mRNA silencing efficiencies in cell culture by up to 10-fold, and to facilitate combinatorial knockdowns. Importantly, these robust improvements were reflected by augmented RNAi phenotypes and accompanied by reduced off-targeting effects. We moreover show that Ago2/shRNA-co-encoding vectors can enhance and prolong transgene silencing in livers of adult mice, while concurrently alleviating hepatotoxicity. Our customizable reagents and avenues should broadly improve future in vitro and in vivo RNAi experiments in mammalian systems. PMID:24049077

  18. Current Issues in Molecular Catalysis Illustrated by Iron Porphyrins as Catalysts of the CO2-to-CO Electrochemical Conversion.

    PubMed

    Costentin, Cyrille; Robert, Marc; Savéant, Jean-Michel

    2015-12-15

    Recent attention aroused by the reduction of carbon dioxide has as main objective the production of useful products, the "solar fuels", in which solar energy would be stored. One route to this goal is the design of photochemical schemes that would operate this conversion using directly sun light energy. An indirect approach consists in first converting sunlight energy into electricity then using it to reduce CO2 electrochemically. Conversion of carbon dioxide into carbon monoxide is thus a key step through the classical dihydrogen-reductive Fischer-Tropsch chemistry. Direct and catalytic electrochemical CO2 reduction already aroused active interest during the 1980-1990 period. The new wave of interest for these matters that has been growing since 2012 is in direct conjunction with modern energy issues. Among molecular catalysts, electrogenerated Fe(0) porphyrins have proved to be particularly efficient and robust. Recent progress in this field has closely associated the search of more and more efficient catalysts in the iron porphyrin family with an unprecedentedly rigorous deciphering of mechanisms. Accordingly, the coupling of proton transfer with electron transfer and breaking of one of the two C-O bonds of CO2 have been the subjects of relentless scrutiny and mechanistic analysis with systematic investigation of the degree of concertedness of these three events. Catalysis of the electrochemical CO2-to-CO conversion has thus been a good testing ground for the mechanism diagnostic strategies and the all concerted reactivity model proposed then. The role of added Brönsted acids, both as H-bond providers and proton donors, has been elucidated. These efforts have been a preliminary to the inclusion of the acid functionalities within the catalyst molecule, giving rise to considerable increase of the catalytic efficiency. The design of more and more efficient catalysts made it necessary to propose "catalytic Tafel plots" relating the turnover frequency to the overpotential as a rational way of benchmarking the catalysts within iron porphyrins and among all available molecular catalysts, independently of the characteristics of the electrolytic cell in use. To be reliable, such assignments of the intrinsic characteristics of catalysts are grounded in the accurate elucidation of mechanisms. Without forgetting the importance of large scale electrolysis, not only mobilization of all resources of nondestructive techniques such as cyclic voltammetry was necessary to achieve this challenge, but also new approaches, such as foot-of-the-wave analysis combined with raising of scan rate, had to be applied. The latest improvement in catalyst design was to render it water-soluble while preserving, or even augmenting, its catalytic efficiency. The replacement of the nonaqueous solvents so far used by water makes the CO2-to-CO half-cell reaction much more attractive for applications, allowing its association with a water-oxidation anode through a proton-exchange membrane. Manipulation of pH and buffering then allow CO2-to-CO conversions from those involving complete CO-selectivity to ones with prescribed CO-H2 mixtures. Overall, it appears that not only are iron porphyrins the most efficient catalysts of the CO2-to-CO electrochemical conversion but also they can serve to illustrate general issues concerning the field of molecular catalysis as a whole, including other reductive or oxidative processes.

  19. Comparative study of the anchorage and the catalytic properties of nanoporous TiO2 films modified with ruthenium (II) and rhenium (I) carbonyl complexes

    NASA Astrophysics Data System (ADS)

    Oyarzún, Diego P.; Chardon-Noblat, Sylvie; Linarez Pérez, Omar E.; López Teijelo, Manuel; Zúñiga, César; Zarate, Ximena; Shott, Eduardo; Carreño, Alexander; Arratia-Perez, Ramiro

    2018-02-01

    In this article we study the anchoring of cis-[Ru(bpyC4pyr)(CO)2(CH3CN)2]2+, cis-[Ru(bpy)2(CO)2]2+ and cis-[Ru(bpyac)(CO)2Cl2], onto nanoporous TiO2 employing electropolymerization, electrostatic interaction and chemical bonding. Also, the [Re(bpyac)(CO)3Cl] rhenium(I) complex for chemical anchorage was analyzed. The characterization of TiO2/Ru(II) and TiO2/Re(I) nanocomposite films was performed by field emission scanning electron microscopy (FESEM), electron dispersive X-ray spectroscopy (EDS) and Raman spectroscopy. In addition, for the more stable nanocomposites obtained, the catalytic properties (solar energy conversion and CO2 reduction) were evaluated. The efficiency improvement in redox process derived from the (photo)electrochemical evidence indicates that modified nanoporous TiO2 structures enhance the rate of charge transfer reactions.

  20. Assessment of environmental impact on air quality by cement industry and mitigating measures: a case study.

    PubMed

    Kabir, G; Madugu, A I

    2010-01-01

    In this study, environmental impact on air quality was evaluated for a typical Cement Industry in Nigeria. The air pollutants in the atmosphere around the cement plant and neighbouring settlements were determined using appropriate sampling techniques. Atmospheric dust and CO2 were prevalent pollutants during the sampling period; their concentrations were recorded to be in the range of 249-3,745 mg/m3 and 2,440-2,600 mg/m3, respectively. Besides atmospheric dust and CO2, the air pollutants such as NOx, SOx and CO were in trace concentrations, below the safe limits approved by FEPA that are 0.0062-0.093 mg/m3 NOx, 0.026 mg/m3 SOx and 114.3 mg/m3 CO, respectively. Some cost-effective mitigating measures were recommended that include the utilisation of readily available and low-cost pozzolans material to produce blended cement, not only could energy efficiency be improved, but carbon dioxide emission could also be minimised during clinker production; and the installation of an advance high-pressure grinding rolls (clinker-roller-press process) to maximise energy efficiency to above what is obtainable from the traditional ball mills and to minimise CO2 emission from the power plant.

  1. Catholyte-Free Electrocatalytic CO2 Reduction to Formate.

    PubMed

    Lee, Wonhee; Kim, Young Eun; Youn, Min Hye; Jeong, Soon Kwan; Park, Ki Tae

    2018-04-16

    Electrochemical reduction of carbon dioxide (CO 2 ) into value-added chemicals is a promising strategy to reduce CO 2 emission and mitigate climate change. One of the most serious problems in electrocatalytic CO 2 reduction (CO 2 R) is the low solubility of CO 2 in an aqueous electrolyte, which significantly limits the cathodic reaction rate. This paper proposes a facile method of catholyte-free electrocatalytic CO 2 reduction to avoid the solubility limitation using commercial tin nanoparticles as a cathode catalyst. Interestingly, as the reaction temperature rises from 303 K to 363 K, the partial current density (PCD) of formate improves more than two times with 52.9 mA cm -2 , despite the decrease in CO 2 solubility. Furthermore, a significantly high formate concentration of 41.5 g L -1 is obtained as a one-path product at 343 K with high PCD (51.7 mA cm -2 ) and high Faradaic efficiency (93.3 %) via continuous operation in a full flow cell at a low cell voltage of 2.2 V. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  2. Cofactor and CO2 donor regulation involved in reductive routes for polymalic acid production by Aureobasidium pullulans CCTCC M2012223.

    PubMed

    Zou, Xiang; Tu, Guangwei; Zan, Zhanquan

    2014-10-01

    Polymalic acid (PMA) is a water-soluble polyester with many attractive properties for biomedical application. Its monomer L-malic acid is widely used in the food industry and also a potential C4 platform chemical. Cofactor and CO2 donor involved in the reductive routes were investigated for PMA production by Aureobasidium pullulans. Biotin as the key cofactor of pyruvate carboxylase was favor for the PMA biosynthesis. Na2CO3 as CO2 donor can obviously improved PMA titer when compared with no CO2 supplier NaOH, and also exhibit more advantages than the other donor CaCO3 because of its water-soluble characteristic. A combinational process with addition of biotin 70 mg/L and Na2CO3 as the CO2 donor was scaled-up in 50 L fermentor, achieving the high product 34.3 g/L of PMA and productivity of 0.41 g/L h. This process provides an efficient and economical way for PMA and malic acid production, and is promising for industrial application.

  3. Improved Efficiency and Stability of Perovskite Solar Cells Induced by CO Functionalized Hydrophobic Ammonium-Based Additives.

    PubMed

    Wu, Zhifang; Raga, Sonia R; Juarez-Perez, Emilio J; Yao, Xuyang; Jiang, Yan; Ono, Luis K; Ning, Zhijun; Tian, He; Qi, Yabing

    2018-01-01

    Because of the rapid rise of the efficiency, perovskite solar cells are currently considered as the most promising next-generation photovoltaic technology. Much effort has been made to improve the efficiency and stability of perovskite solar cells. Here, it is demonstrated that the addition of a novel organic cation of 2-(6-bromo-1,3-dioxo-1H-benzo[de]isoquinolin-2(3H)-yl)ethan-1-ammonium iodide (2-NAM), which has strong Lewis acid and base interaction (between CO and Pb) with perovskite, can effectively increase crystalline grain size and reduce charge carrier recombination of the double cation FA 0.83 MA 0.17 PbI 2.51 Br 0.49 perovskite film, thus boosting the efficiency from 17.1 ± 0.8% to 18.6 ± 0.9% for the 0.1 cm 2 cell and from 15.5 ± 0.5% to 16.5 ± 0.6% for the 1.0 cm 2 cell. The champion cell shows efficiencies of 20.0% and 17.6% with active areas of 0.1 and 1.0 cm 2 , respectively. Moreover, the hysteresis behavior is suppressed and the stability is improved. The result provides a promising route to further elevate efficiency and stability of perovskite solar cells by the fine tuning of triple organic cations. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  4. Synergistic Enhancement of Electrocatalytic CO 2 Reduction with Gold Nanoparticles Embedded in Functional Graphene Nanoribbon Composite Electrodes

    DOE PAGES

    Rogers, Cameron; Perkins, Wade S.; Veber, Gregory; ...

    2017-02-24

    Regulating the complex environment accounting for the stability, selectivity, and activity of catalytic metal nanoparticle interfaces represents a challenge to heterogeneous catalyst design. Here in this paper, we demonstrate the intrinsic performance enhancement of a composite material composed of gold nanoparticles (AuNPs) embedded in a bottom-up synthesized graphene nanoribbon (GNR) matrix for the electrocatalytic reduction of CO 2. Electrochemical studies reveal that the structural and electronic properties of the GNR composite matrix increase the AuNP electrochemically active surface area (ECSA), lower the requisite CO 2 reduction overpotential by hundreds of millivolts (catalytic onset > -0.2 V versus reversible hydrogen electrodemore » (RHE)), increase the Faraday efficiency (>90%), markedly improve stability (catalytic performance sustained over >24 h), and increase the total catalytic output (>100-fold improvement over traditional amorphous carbon AuNP supports). The inherent structural and electronic tunability of bottom-up synthesized GNR-AuNP composites affords an unrivaled degree of control over the catalytic environment, providing a means for such profound effects as shifting the rate-determining step in the electrocatalytic reduction of CO 2 to CO, and thereby altering the electrocatalytic mechanism at the nanoparticle surface.« less

  5. Enabling catalytic oxidation of Li2O2 at the liquid-solid interface: the evolution of an aprotic Li-O2 battery.

    PubMed

    Feng, Ningning; He, Ping; Zhou, Haoshen

    2015-02-01

    We show that by using a suitable soluble redox mediator, the charging overpotential can be reduced and the round-trip efficiency can be improved in an aprotic Li-O2 battery. Not only do we explore a new redox couple, 10-methyl-10H-phenothiazine, as a soluble catalyst that improves the electrochemical performance, but we also propose possible challenges that need to be overcome for the future improvement of aprotic Li-O2 batteries. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  6. Magnetic hyperthermia and pH-responsive effective drug delivery to the sub-cellular level of human breast cancer cells by modified CoFe2O4 nanoparticles.

    PubMed

    Oh, Yunok; Moorthy, Madhappan Santha; Manivasagan, Panchanathan; Bharathiraja, Subramaniyan; Oh, Junghwan

    2017-02-01

    Magnetic iron oxide nanoparticles (MNPs) have been extensively utilized in a wide range of biomedical applications including magnetic hyperthermia agent. To improve the efficiency of the MNPs in therapeutic applications, in this study, we have synthesized CoFe 2 O 4 nanoparticles and its surface was further functionalized with meso-2,3-dimercaptosuccinic acid (DMSA). The anticancer agent, Doxorubucin (DOX) was conjugated with CoFe 2 O 4 @DMSA nanoparticle to evaluate the combined effects of thermotherapy and chemotherapy. The drug delivery efficiency of the DOX loaded CoFe 2 O 4 @DMSA nanoparticles were examined based on magnetically triggered delivery of DOX into the subcellular level of cancer cells by using MDA-MB-231 cell line. The amine part of the DOX molecules were effectively attached through an electrostatic interactions and/or hydrogen bonding interactions with the carboxylic acid groups of the DMSA functionalities present onto the surface of the CoFe 2 O 4 nanoparticles. The DOX loaded CoFe 2 O 4 @DMSA nanoparticles can effectively uptake with cancer cells via typical endocytosis process. After endocytosis, DOX release from CoFe 2 O 4 nanoparticles was triggered by intracellular endosomal/lysosomal acidic environments and the localized heat can be generated under an alternating magnetic field (AMF). In the presence of AMF, the released DOX molecules were accumulated with high concentrations into the subcellular level at a desired sites and exhibited a synergistic effect of an enhanced cell cytotoxicity by the combined effects of thermal-chemotherapy. Importantly, pH- and thermal-responsive Dox-loaded CoFe 2 O 4 nanoparticles induced significant cellular apoptosis more efficiently mediated by active mitochondrial membrane and ROS generation than the free Dox. Thus, the Dox-loaded CoFe 2 O 4 @DMSA nanoparticles can be used as a potential therapeutic agent in cancer therapy by combining the thermo-chemotherapy techniques. Copyright © 2016. Published by Elsevier B.V.

  7. A comparative study of biomass integrated gasification combined cycle power systems: Performance analysis.

    PubMed

    Zang, Guiyan; Tejasvi, Sharma; Ratner, Albert; Lora, Electo Silva

    2018-05-01

    The Biomass Integrated Gasification Combined Cycle (BIGCC) power system is believed to potentially be a highly efficient way to utilize biomass to generate power. However, there is no comparative study of BIGCC systems that examines all the latest improvements for gasification agents, gas turbine combustion methods, and CO 2 Capture and Storage options. This study examines the impact of recent advancements on BIGCC performance through exergy analysis using Aspen Plus. Results show that the exergy efficiency of these systems is ranged from 22.3% to 37.1%. Furthermore, exergy analysis indicates that the gas turbine with external combustion has relatively high exergy efficiency, and Selexol CO 2 removal method has low exergy destruction. Moreover, the sensitivity analysis shows that the system exergy efficiency is more sensitive to the initial temperature and pressure ratio of the gas turbine, whereas has a relatively weak dependence on the initial temperature and initial pressure of the steam turbine. Copyright © 2018 Elsevier Ltd. All rights reserved.

  8. Electron transport, pep carboxylase activity, and maximal net co2 assimilation exhibit coordinated and proportional decline with loss of hydraulic conductance during water stress in Zea mays

    USDA-ARS?s Scientific Manuscript database

    Efforts to improve the photosynthetic performance of species are presently focused on leaf-level traits (e.g., quantum efficiency, mesophyll osmoregulation, stress protein regulation). Here, we emphasize that efforts to improve plant performance in arid environments would benefit from also consider...

  9. Heterogeneous catalytic conversion of CO2: a comprehensive theoretical review.

    PubMed

    Li, Yawei; Chan, Siew Hwa; Sun, Qiang

    2015-05-21

    The conversion of CO2 into fuels and useful chemicals has been intensively pursued for renewable, sustainable and green energy. However, due to the negative adiabatic electron affinity (EA) and large ionization potential (IP), the CO2 molecule is chemically inert, thus making the conversion difficult under normal conditions. Novel catalysts, which have high stability, superior efficiency and low cost, are urgently needed to facilitate the conversion. As the first step to design such catalysts, understanding the mechanisms involved in CO2 conversion is absolutely indispensable. In this review, we have summarized the recent theoretical progress in mechanistic studies based on density functional theory, kinetic Monte Carlo simulation, and microkinetics modeling. We focus on reaction channels, intermediate products, the key factors determining the conversion of CO2 in solid-gas interface thermocatalytic reduction and solid-liquid interface electrocatalytic reduction. Furthermore, we have proposed some possible strategies for improving CO2 electrocatalysis and also discussed the challenges in theory, model construction, and future research directions.

  10. Atmospheric CO2 capture by algae: Negative carbon dioxide emission path.

    PubMed

    Moreira, Diana; Pires, José C M

    2016-09-01

    Carbon dioxide is one of the most important greenhouse gas, which concentration increase in the atmosphere is associated to climate change and global warming. Besides CO2 capture in large emission point sources, the capture of this pollutant from atmosphere may be required due to significant contribution of diffuse sources. The technologies that remove CO2 from atmosphere (creating a negative balance of CO2) are called negative emission technologies. Bioenergy with Carbon Capture and Storage may play an important role for CO2 mitigation. It represents the combination of bioenergy production and carbon capture and storage, keeping carbon dioxide in geological reservoirs. Algae have a high potential as the source of biomass, as they present high photosynthetic efficiencies and high biomass yields. Their biomass has a wide range of applications, which can improve the economic viability of the process. Thus, this paper aims to assess the atmospheric CO2 capture by algal cultures. Copyright © 2016 Elsevier Ltd. All rights reserved.

  11. Final report : CO2 reduction using biomimetic photocatalytic nanodevices.

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Garcia, Robert M.; Shelnutt, John Allen; Medforth, Craig John

    2009-11-01

    Nobel Prize winner Richard Smalley was an avid champion for the cause of energy research. Calling it 'the single most important problem facing humanity today,' Smalley promoted the development of nanotechnology as a means to harness solar energy. Using nanotechnology to create solar fuels (i.e., fuels created from sunlight, CO{sub 2}, and water) is an especially intriguing idea, as it impacts not only energy production and storage, but also climate change. Solar irradiation is the only sustainable energy source of a magnitude sufficient to meet projections for global energy demand. Biofuels meet the definition of a solar fuel. Unfortunately, themore » efficiency of photosynthesis will need to be improved by an estimated factor of ten before biofuels can fully replace fossil fuels. Additionally, biological organisms produce an array of hydrocarbon products requiring further processing before they are usable for most applications. Alternately, 'bio-inspired' nanostructured photocatalytic devices that efficiently harvest sunlight and use that energy to reduce CO{sub 2} into a single useful product or chemical intermediate can be envisioned. Of course, producing such a device is very challenging as it must be robust and multifunctional, i.e. capable of promoting and coupling the multi-electron, multi-photon water oxidation and CO{sub 2} reduction processes. Herein, we summarize some of the recent and most significant work towards creating light harvesting nanodevices that reduce CO{sub 2} to CO (a key chemical intermediate) that are based on key functionalities inspired by nature. We report the growth of Co(III)TPPCl nanofibers (20-100 nm in diameter) on gas diffusion layers via an evaporation induced self-assembly (EISA) method. Remarkably, as-fabricated electrodes demonstrate light-enhanced activity for CO{sub 2} reduction to CO as evidenced by cyclic voltammograms and electrolysis with/without light irradiation. To the best of our knowledge, it is the first time to observe such a light-enhanced CO{sub 2} reduction reaction based on nanostructured cobalt(III) porphyrin catalysts. Additionally, gas chromatography (GC) verifies that light irradiation can improve CO production by up to 31.3% during 2 hours of electrolysis. In addition, a variety of novel porphyrin nano- or micro-structures were also prepared including nanospheres, nanotubes, and micro-crosses.« less

  12. Organic-Inorganic Hybrid Interfacial Layer for High-Performance Planar Perovskite Solar Cells.

    PubMed

    Yang, Hao; Cong, Shan; Lou, Yanhui; Han, Liang; Zhao, Jie; Sun, Yinghui; Zou, Guifu

    2017-09-20

    4,7-Diphenyl-1,10-phenanthroline (Bphen) is an efficient electron transport and hole blocking material in organic photoelectric devices. Here, we report cesium carbonate (Cs 2 CO 3 ) doped Bphen as cathode interfacial layer in CH 3 NH 3 PbI 3-x Cl x based planar perovskite solar cells (PSCs). Investigation finds that introducing Cs 2 CO 3 suppresses the crystallization of Bphen and benefits a smooth interface contact between the perovskite and electrode, resulting in the decrease in carrier recombination and the perovskite degradation. In addition, the matching energy level of Bphen film in the PSCs effectively blocks the holes diffusion to cathode. The resultant power conversion efficiency (PCE) achieves as high as 17.03% in comparison with 12.67% of reference device without doping. Besides, experiments also demonstrate the stability of PSCs have large improvement because the suppressed crystallization of Bphen by doping Cs 2 CO 3 as a superior barrier layer blocks the Ag atom and surrounding moisture access to the vulnerable perovskite layer.

  13. Slow induction of photosynthesis on shade to sun transitions in wheat may cost at least 21% of productivity.

    PubMed

    Taylor, Samuel H; Long, Stephen P

    2017-09-26

    Wheat is the second most important direct source of food calories in the world. After considerable improvement during the Green Revolution, increase in genetic yield potential appears to have stalled. Improvement of photosynthetic efficiency now appears a major opportunity in addressing the sustainable yield increases needed to meet future food demand. Effort, however, has focused on increasing efficiency under steady-state conditions. In the field, the light environment at the level of individual leaves is constantly changing. The speed of adjustment of photosynthetic efficiency can have a profound effect on crop carbon gain and yield. Flag leaves of wheat are the major photosynthetic organs supplying the grain of wheat, and will be intermittently shaded throughout a typical day. Here, the speed of adjustment to a shade to sun transition in these leaves was analysed. On transfer to sun conditions, the leaf required about 15 min to regain maximum photosynthetic efficiency. In vivo analysis based on the responses of leaf CO 2 assimilation ( A ) to intercellular CO 2 concentration ( c i ) implied that the major limitation throughout this induction was activation of the primary carboxylase of C3 photosynthesis, ribulose-1,5-bisphosphate carboxylase/oxygenase (Rubisco). This was followed in importance by stomata, which accounted for about 20% of the limitation. Except during the first few seconds, photosynthetic electron transport and regeneration of the CO 2 acceptor molecule, ribulose-1,5-bisphosphate (RubP), did not affect the speed of induction. The measured kinetics of Rubisco activation in the sun and de-activation in the shade were predicted from the measurements. These were combined with a canopy ray tracing model that predicted intermittent shading of flag leaves over the course of a June day. This indicated that the slow adjustment in shade to sun transitions could cost 21% of potential assimilation.This article is part of the themed issue 'Enhancing photosynthesis in crop plants: targets for improvement'. © 2017 The Authors.

  14. In situ preparation of NiS2/CoS2 composite electrocatalytic materials on conductive glass substrates with electronic modulation for high-performance counter electrodes of dye-sensitized solar cells

    NASA Astrophysics Data System (ADS)

    Li, Faxin; Wang, Jiali; Zheng, Li; Zhao, Yaqiang; Huang, Niu; Sun, Panpan; Fang, Liang; Wang, Lei; Sun, Xiaohua

    2018-04-01

    The electrocatalytic composite materials of honeycomb structure NiS2 nanosheets loaded with metallic CoS2 nanoparticles are in situ prepared on F doped SnO2 conductive glass (FTO) substrates used as counter electrodes of DSSCs through chemical bath deposition (CBD) and sulfidizing process. Single crystalline NiS2 honeycomb structure array lay a foundation for the large surface area of NiS2/CoS2 composite CEs. The formed NiS2/CoS2 nanointerface modulates electronic structure of composite CEs from the synergetic interactions between CoS2 nanoparticles and NiS2 nanosheets, which dramatically improves the electrocatalytic activity of NiS2/CoS2 composite CEs; Metallic CoS2 nanoparticles covering NiS2 nanosheets electrodes adjusts the electrodes' structure and then reduces the series resistance (Rs) and the Nernst diffusion resistance (Zw) of counter electrodes. The improvement of these areas greatly enhances the electrocatalytic performance of CEs and the short circuit current density (Jsc) and Fill factor (FF) of DSSCs. Impressively, the DSSC based on NiS2/CoS2-0.1 CE shows the best photovoltaic performance with photovoltaic conversion efficiency of 8.22%, which is 24.36% higher than that (6.61%) of the DSSC with Pt CE. And the NiS2/CoS2-0.1 CE also displays a good stability in the iodine based electrolyte. This work indicates that rational construction of composite electrocatalytic materials paves an avenue for high-performance counter electrodes of DSSCs.

  15. Design of electrolyzer for carbon dioxide conversion to fuels and chemicals

    NASA Astrophysics Data System (ADS)

    Rosen, Jonathan S.

    The stabilization of global atmospheric CO2 levels requires a transition towards a renewable energy based economy as well as methods for handling current CO2 output from fossil fuels. Challenges with renewable energy intermittency have thus far limited the use of these alternative energy sources to only a fraction of the current energy portfolio. To enable more widespread use of renewable energy systems, methods of large scale energy storage must be developed to store excess renewable energy when demand is low and allow for combined use of energy storage and renewable systems when demand is high. To date, no one technique has demonstrated energy storage methods on the gigawatt scale needed for integration with renewable sources; therefore the development of suitable energy storage technologies, such as CO2 electrolysis to fuels is needed. In this work, research efforts have focused on two major thrusts related to electrochemical methods of CO 2 conversion to fuels. The first thrust focuses on the synthesis and design of highly efficient anode and cathode catalysts with emphasis on understanding structure-property relationships. A second thrust focuses on the design of novel electrochemical devices for CO2 conversion and integration of synthesized materials into flow cell systems. On the anode side, the synthesis of highly active catalysts using abundant transition metals is crucial to reducing capital costs and enabling widespread use of electrochemical CO2 conversion devices. Highly active mesoporous Co3O4 and metal-substituted Co3O4 water oxidation catalysts were designed to investigate the role of the spinel structure on water oxidation activity. Further analysis of metal substituted samples reveal the importance of the octahedral sites in the spinel structure, which was later used to design an Mg-Co3O4 sample with improved water oxidation activity. The design of efficient cathode materials which can selectivity reduce CO2 to fuels and chemicals is critical to the widespread use of CO2 electrolysis. A nanoporous Ag material was synthesized through a dealloying technique able to operate with less than 0.5 V overpotential and high selectivity towards CO. CO is a valuable intermediate chemical which can used in Fischer-Tropsch or Gas-to-liquids technologies to produce liquids fuels. A detailed investigation of nanostructured Ag catalysts found stepped sites to be responsible for enhanced CO2 reduction activity due to improved stabilization of the COOH intermediate on the catalyst surface. In addition, an low-cost Zn dendrite electrocatalyst was developed using an electroplating technique. Low coordinated sites formed through electrodeposition demonstrated the suppression of hydrogen evolution while maintaining CO activity. The Zn dendrite electrocatalyst was further examined using a newly developed in situ X-ray absorption technique able to probe catalyst stability and crystalline structure under CO2 reduction operating conditions. A final hurdle in the realization of CO2 electrolysis technologies is the integration of catalysts into working flow cell devices. To address this issue and enable testing in a practical system, a highly efficient and robust CO2 electrolysis flow cell was designed including the scale up of the previous nanoporous Ag synthesis procedure. Using the modified porous Ag catalyst, currents in the Amp regime were demonstrated approaching rates needed for energy storage applications. Stability on the order of days was successfully demonstrated due to use of robust system components and conditions suitable for process scale up.

  16. Effect of Nb and F co-doping on Li1.2Mn0.54Ni0.13Co0.13O2 cathode material for high-performance lithium-ion batteries

    NASA Astrophysics Data System (ADS)

    Ming, Lei; Zhang, Bao; Cao, Yang; Zhang, Jia-Feng; Wang, Chun-Hui; Wang, Xiao-Wei; Li, Hui

    2018-04-01

    The Li1.2Mn0.54-xNbxCo0.13Ni0.13O2-6xF6x (x=0, 0.01, 0.03, 0.05) is prepared by traditional solid-phase method, and the Nb and F ions have been successfully doped into Mn and O sites of layered materials Li1.2Mn0.54Co0.13Ni0.13O2, respectively. The incorporating Nb ion in Mn site could effectively restrain the migration of transtion metal ions during long-term cycling, and keep the stability of the crystal structure. The Li1.2Mn0.54-xNbxCo0.13Ni0.13O2-6xF6x shows suppressed voltage fade and higher capacity retention of 98.1 after 200 cycles at rate of 1 C. The replacement of O2- by the strongly electronegative F- was beneficial for suppressed the structure change of Li2MnO3 from the eliminating of oxygen in initial charge process. Therefore, the initial coulomb efficiency of doped Li1.2Mn0.54-xNbxCo0.13Ni0.13O2-6xF6x gets improved, which is higher than that of pure Li1.2Mn0.54Co0.13Ni0.13O2. In addition, the Nb and F co-doping could effectively enhance the transfer of lithium-ion and electrons, and thus improving rate performance.

  17. Design of experimental system for supercritical CO2 fracturing under confining pressure conditions

    NASA Astrophysics Data System (ADS)

    Wang, H.; Lu, Q.; Li, X.; Yang, B.; Zheng, Y.; Shi, L.; Shi, X.

    2018-03-01

    Supercritical CO2 has the characteristics of low viscosity, high diffusion and zero surface tension, and it is considered as a new fluid for non-polluting and non-aqueous fracturing which can be used for shale gas development. Fracturing refers to a method of utilizing the high-pressure fluid to generate fractures in the rock formation so as to improve the oil and gas flow conditions and increase the oil and gas production. In this article, a new type of experimental system for supercritical CO2 fracturing under confining pressure conditions is designed, which is based on characteristics of supercritical CO2, shale reservoir and down-hole environment. The experimental system consists of three sub-systems, including supercritical CO2 generation system, supercritical CO2 fracturing system and data analysis system. It can be used to simulate supercritical CO2 fracturing under geo-stress conditions, thus to study the rock initiation pressure, the formation of the rock fractures, fractured surface morphology and so on. The experimental system has successfully carried out a series of supercritical CO2 fracturing experiments. The experimental results confirm the feasibility of the experimental system and the high efficiency of supercritical CO2 in fracturing tight rocks.

  18. A Small Decrease in Rubisco Content by Individual Suppression of RBCS Genes Leads to Improvement of Photosynthesis and Greater Biomass Production in Rice Under Conditions of Elevated CO2.

    PubMed

    Kanno, Keiichi; Suzuki, Yuji; Makino, Amane

    2017-03-01

    Rubisco limits photosynthesis at low CO2 concentrations ([CO2]), but does not limit it at elevated [CO2]. This means that the amount of Rubisco is excessive for photosynthesis at elevated [CO2]. Therefore, we examined whether a small decrease in Rubisco content by individual suppression of the RBCS multigene family leads to increases in photosynthesis and biomass production at elevated [CO2] in rice (Oryza sativa L.). Our previous studies indicated that the individual suppression of RBCS decreased Rubisco content in rice by 10-25%. Three lines of BC2F2 progeny were selected from transgenic plants with individual suppression of OsRBCS2, 3 and 5. Rubisco content in the selected lines was 71-90% that of wild-type plants. These three transgenic lines showed lower rates of CO2 assimilation at low [CO2] (28 Pa) but higher rates of CO2 assimilation at elevated [CO2] (120 Pa). Similarly, the biomass production and relative growth rate (RGR) of the two lines were also smaller at low [CO2] but greater than that of wild-type plants at elevated [CO2]. This greater RGR was caused by the higher net assimilation rate (NAR). When the nitrogen use efficiency (NUE) for the NAR was estimated by dividing the NAR by whole-plant leaf N content, the NUE for NAR at elevated [CO2] was higher in these two lines. Thus, a small decrease in Rubisco content leads to improvements of photosynthesis and greater biomass production in rice under conditions of elevated CO2. © The Author 2017. Published by Oxford University Press on behalf of Japanese Society of Plant Physiologists. All rights reserved. For permissions, please email: journals.permissions@oup.com.

  19. Metal-Organic Framework-Stabilized CO2/Water Interfacial Route for Photocatalytic CO2 Conversion.

    PubMed

    Luo, Tian; Zhang, Jianling; Li, Wei; He, Zhenhong; Sun, Xiaofu; Shi, Jinbiao; Shao, Dan; Zhang, Bingxing; Tan, Xiuniang; Han, Buxing

    2017-11-29

    Here, we propose a CO 2 /water interfacial route for photocatalytic CO 2 conversion by utilizing a metal-organic framework (MOF) as both an emulsifier and a catalyst. The CO 2 reduction occurring at the CO 2 /water interface produces formate with remarkably enhanced efficiency as compared with that in conventional solvent. The route is efficient, facile, adjustable, and environmentally benign, which is applicable for the CO 2 transformation photocatalyzed by different kinds of MOFs.

  20. CO2 plume management in saline reservoir sequestration

    USGS Publications Warehouse

    Frailey, S.M.; Finley, R.J.

    2011-01-01

    A significant difference between injecting CO2 into saline aquifers for sequestration and injecting fluids into oil reservoirs or natural gas into aquifer storage reservoirs is the availability and use of other production and injection wells surrounding the primary injection well(s). Of major concern for CO2 sequestration using a single well is the distribution of pressure and CO2 saturation within the injection zone. Pressure is of concern with regards to caprock integrity and potential migration of brine or CO2 outside of the injection zone, while CO2 saturation is of interest for storage rights and displacement efficiency. For oil reservoirs, the presence of additional wells is intended to maximize oil recovery by injecting CO2 into the same hydraulic flow units from which the producing wells are withdrawing fluids. Completing injectors and producers in the same flow unit increases CO2 throughput, maximizes oil displacement efficiency, and controls pressure buildup. Additional injectors may surround the CO2 injection well and oil production wells in order to provide external pressure to these wells to prevent the injected CO2 from migrating from the pattern between two of the producing wells. Natural gas storage practices are similar in that to reduce the amount of "cushion" gas and increase the amount of cycled or working gas, edge wells may be used for withdrawal of gas and center wells used for gas injection. This reduces loss of gas to the formation via residual trapping far from the injection well. Moreover, this maximizes the natural gas storage efficiency between the injection and production wells and reduces the areal extent of the natural gas plume. Proposed U.S. EPA regulations include monitoring pressure and suggest the "plume" may be defined by pressure in addition to the CO2 saturated area. For pressure monitoring, it seems that this can only be accomplished by injection zone monitoring wells. For pressure, these wells would not need to be very close to the injection well, compared to monitoring wells intended to measure CO2 saturation via fluid sampling or cased-hole well logs. If pressure monitoring wells become mandated, these wells could be used for managing the CO2 saturation and aquifer pressure distribution. To understand the relevance and effectiveness of producing and injecting brine to improve storage efficiency, direct the plume to specific pore space, and redistribute the pressure, numerical models of CO2 injection into aquifers are used. Simulated cases include various aquifer properties at a single well site and varying the number and location of surrounding wells for plume management. Strategies in terms of completion intervals can be developed to effectively contact more vertical pore space in relatively thicker geologic formations. Inter-site plume management (or cooperative) wells for the purpose of pressure monitoring and plume management may become the responsibility of a consortium of operators or a government entity, not individual sequestration site operators. ?? 2011 Published by Elsevier Ltd.

  1. Large area silicon sheet by EFG

    NASA Technical Reports Server (NTRS)

    1980-01-01

    Recent advances toward silicon growth stations and improved electronic quality of multiplesilicon are discussed. These advances were made in large measure by studies in which the composition of the gas environment around the meniscus area was varied. By introducing gases such as CO2, CO, and CH4 into this region, reproducible increases in diffusion length and cell performance were realized, with the best large area (5 cm x 10 cm) cells exceeding 11% efficiency.

  2. Efficient Domino Hydroformylation/Benzoin Condensation: Highly Selective Synthesis of α-Hydroxy Ketones.

    PubMed

    Dong, Kaiwu; Sang, Rui; Soule, Jean-Francois; Bruneau, Christian; Franke, Robert; Jackstell, Ralf; Beller, Matthias

    2015-12-07

    An improved domino hydroformylation/benzoin condensation to give α-hydroxy ketones has been developed. Easily available olefins are smoothly converted into the corresponding α-hydroxy ketones in high yields with excellent regioselectivities. Key to success is the use of a specific catalytic system consisting of a rhodium/phosphine complex and the CO2 adduct of an N-heterocyclic carbene. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. Allocation of secondary metabolites, photosynthetic capacity, and antioxidant activity of Kacip Fatimah (Labisia pumila Benth) in response to CO2 and light intensity.

    PubMed

    Ibrahim, Mohd Hafiz; Jaafar, Hawa Z E; Karimi, Ehsan; Ghasemzadeh, Ali

    2014-01-01

    A split plot 3 by 4 experiment was designed to investigate and distinguish the relationships among production of secondary metabolites, soluble sugar, phenylalanine ammonia lyase (PAL; EC 4.3.1.5) activity, leaf gas exchange, chlorophyll content, antioxidant activity (DPPH), and lipid peroxidation under three levels of CO2 (400, 800, and 1200 μ mol/mol) and four levels of light intensity (225, 500, 625, and 900 μ mol/m(2)/s) over 15 weeks in Labisia pumila. The production of plant secondary metabolites, sugar, chlorophyll content, antioxidant activity, and malondialdehyde content was influenced by the interactions between CO2 and irradiance. The highest accumulation of secondary metabolites, sugar, maliondialdehyde, and DPPH activity was observed under CO2 at 1200 μ mol/mol + light intensity at 225 μ mol/m(2)/s. Meanwhile, at 400 μ mol/mol CO2 + 900 μ mol/m(2)/s light intensity the production of chlorophyll and maliondialdehyde content was the highest. As CO2 levels increased from 400 to 1200 μ mol/mol the photosynthesis, stomatal conductance, f v /f m (maximum efficiency of photosystem II), and PAL activity were enhanced. The production of secondary metabolites displayed a significant negative relationship with maliondialdehyde indicating lowered oxidative stress under high CO2 and low irradiance improved the production of plant secondary metabolites that simultaneously enhanced the antioxidant activity (DPPH), thus improving the medicinal value of Labisia pumila under this condition.

  4. CO2 Dissociation using the Versatile Atmospheric Dielectric Barrier Discharge Experiment (VADER)

    NASA Astrophysics Data System (ADS)

    Lindon, Michael Allen

    As of 2013, the Carbon Dioxide Information Analysis Center (CDIAC) estimates that the world emits approximately 36 trillion metric tons of Carbon Dioxide (CO2) into the atmosphere every year. These large emissions have been correlated to global warming trends that have many consequences across the globe, including glacial retraction, ocean acidification and increased severity of weather events. With green technologies still in the infancy stage, it can be expected that CO2 emissions will stay this way for along time to come. Approximately 41% of the emissions are due to electricity production, which pump out condensed forms of CO2. This danger to our world is why research towards new and innovative ways of controlling CO2 emissions from these large sources is necessary. As of now, research is focused on two primary methods of CO2 reduction from condensed CO2 emission sources (like fossil fuel power plants): Carbon Capture and Sequestration (CCS) and Carbon Capture and Utilization (CCU). CCS is the process of collecting CO2 using absorbers or chemicals, extracting the gas from those absorbers and finally pumping the gas into reservoirs. CCU on the other hand, is the process of reacting CO2 to form value added chemicals, which can then be recycled or stored chemically. A Dielectric Barrier discharge (DBD) is a pulsed, low temperature, non-thermal, atmospheric pressure plasma which creates high energy electrons suitable for dissociating CO2 into its components (CO and O) as one step in the CCU process. Here I discuss the viability of using a DBD for CO2 dissociation on an industrial scale as well as the fundamental physics and chemistry of a DBD for CO2 dissociation. This work involved modeling the DBD discharge and chemistry, which showed that there are specific chemical pathways and plasma parameters that can be adjusted to improve the CO2 reaction efficiencies and rates. Experimental studies using the Versatile Atmospheric dielectric barrier Discharge ExpeRiment (VADER) demonstrated how different factors, like voltage, frequency and the addition of a photocatalyst, change the efficiency of CO2 dissociation in VADER and the plasma chemistry involved.

  5. Use of magnetic nanoparticles to enhance bioethanol production in syngas fermentation.

    PubMed

    Kim, Young-Kee; Lee, Haryeong

    2016-03-01

    The effect of two types of nanoparticles on the enhancement of bioethanol production in syngas fermentation by Clostridium ljungdahlii was examined. Methyl-functionalized silica and methyl-functionalized cobalt ferrite-silica (CoFe2O4@SiO2-CH3) nanoparticles were used to improve syngas-water mass transfer. Of these, CoFe2O4@SiO2-CH3 nanoparticles showed better enhancement of syngas mass transfer. The nanoparticles were recovered using a magnet and reused five times to evaluate reusability, and it was confirmed that their capability for mass transfer enhancement was maintained. Both types of nanoparticles were applied to syngas fermentation, and production of biomass, ethanol, and acetic acid was enhanced. CoFe2O4@SiO2-CH3 nanoparticles were more efficient for the productivity of syngas fermentation due to improved syngas mass transfer. The biomass, ethanol, and acetic acid production compared to a control were increased by 227.6%, 213.5%, and 59.6%, respectively by addition of CoFe2O4@SiO2-CH3 nanoparticles. The reusability of the nanoparticles was confirmed by reuse of recovered nanoparticles for fermentation. Copyright © 2016 Elsevier Ltd. All rights reserved.

  6. Hybrid life-cycle assessment (LCA) of CO2 emission with management alternatives for household food wastes in Japan.

    PubMed

    Inaba, Rokuta; Nansai, Keisuke; Fujii, Minoru; Hashimoto, Seiji

    2010-06-01

    In this study, we conducted a hybrid life-cycle assessment (LCA) to evaluate reductions in CO(2) emissions by food waste biogasification of household food wastes in Japan. Two alternative scenarios were examined. In one alternative (Ref), all combustible municipal solid wastes (MSWs), including food waste, are incinerated. In the other (Bio), food waste is biogasified, while the other combustible wastes are incinerated. An inventory analysis of energy and material flow in the MSW management system was conducted. Subsequently, the inventory data were summarized into an input-output format, and a make-use input-output framework was applied. Furthermore, a production equilibrium model was established using a matrix representing the input- output relationship of energy and materials among the processes and sectors. Several levels of power generation efficiency from incineration were applied as a sensitivity analysis. The hybrid LCA indicated that the difference between the Bio and Ref scenarios, from the perspective of CO( 2) emissions, is relatively small. However, a 13-14% reduction of CO(2) emissions of the total waste management sector in Japan may be achieved by improving the efficiency of power generation from incineration from 10% to 25%.

  7. Carbon Monoxide Is Involved in Hydrogen Gas-Induced Adventitious Root Development in Cucumber under Simulated Drought Stress

    PubMed Central

    Chen, Yue; Wang, Meng; Hu, Linli; Liao, Weibiao; Dawuda, Mohammed M.; Li, Chunlan

    2017-01-01

    Hydrogen gas (H2) and carbon monoxide (CO) are involved in plant growth and developmental processes and may induce plant tolerance to several stresses. However, the independent roles and interaction effect of H2 and CO in adventitious root development under drought conditions have still not received the needed research attention. We hypothesize that there exists crosstalk between H2 and CO during adventitious root development under drought stress. The results of our current study revealed that 50% (v/v) hydrogen-rich water (HRW), 500 μM Hemin (the CO donor) and 30% (w/v) CO aqueous solution apparently promoted the development of adventitious roots in cucumber explants (Cucumis Sativus L.) under drought stress. H2 and CO increased relative water content (RWC), leaf chlorophyll content (chlorophyll a, b, and a+b), and chlorophyll fluorescence parameters [photochemical efficiency of photosystem II (PSII), PSII actual photochemical efficiency and photochemical quench coefficient] under drought condition. When the CO scavenger hemoglobin (Hb) or zinc protoporphyrin IX (ZnPPIX) was added to HRW/CO aqueous solution, the positive effect of HRW/CO aqueous solution on RWC, leaf chlorophyll content, and chlorophyll fluorescence parameters were reversed. Additionally, superoxide dismutases, peroxidase, catalase, and ascorbate peroxidase was significantly increased in the explants treated with HRW and CO aqueous solution under drought stress, thus alleviating oxidative damage, as indicated by decreases in thiobarbituric acid reactive substances (TBARS), hydrogen peroxide (H2O2), and superoxide radical (O2-) levels. H2 and CO also improved the levels of water soluble carbohydrate, total soluble protein, and proline content. However, the above CO/H2-mediated effects were reversed by CO scavenger Hb or CO specific synthetic inhibitor ZnPPIX. Therefore, CO may be involved in H2-induced adventitious rooting under drought stress and alleviate oxidative damage by enhancing RWC, leaf chlorophyll content, chlorophyll fluorescence parameters, metabolic constituent content, activating anti-oxidant enzymes and reducing TBARS, O2-, and H2O2 levels. PMID:28223992

  8. Extracts of Crataegus oxyacantha and Rosmarinus officinalis Attenuate Ischemic Myocardial Damage by Decreasing Oxidative Stress and Regulating the Production of Cardiac Vasoactive Agents.

    PubMed

    Cuevas-Durán, Raúl Enrique; Medrano-Rodríguez, Juan Carlos; Sánchez-Aguilar, María; Soria-Castro, Elizabeth; Rubio-Ruíz, María Esther; Del Valle-Mondragón, Leonardo; Sánchez-Mendoza, Alicia; Torres-Narvaéz, Juan Carlos; Pastelín-Hernández, Gustavo; Ibarra-Lara, Luz

    2017-11-14

    Numerous studies have supported a role for oxidative stress in the development of ischemic damage and endothelial dysfunction. Crataegus oxyacantha ( Co ) and Rosmarinus officinalis ( Ro ) extracts are polyphenolic-rich compounds that have proven to be efficient in the treatment of cardiovascular diseases. We studied the effect of extracts from Co and Ro on the myocardial damage associated with the oxidative status and to the production of different vasoactive agents. Rats were assigned to the following groups: (a) sham; (b) vehicle-treated myocardial infarction (MI) (MI-V); (c) Ro extract-treated myocardial infarction (MI- Ro ); (d) Co extract-treated myocardial infarction (MI- Co ); or (e) Ro+Co -treated myocardial infarction (MI- Ro+Co ). Ro and Co treatments increased total antioxidant capacity, the expression of superoxide dismutase (SOD)-Cu 2+ /Zn 2+ , SOD-Mn 2+ , and catalase, with the subsequent decline of malondialdehyde and 8-hydroxy-2'-deoxyguanosine levels. The extracts diminished vasoconstrictor peptide levels (angiotensin II and endothelin-1), increased vasodilators agents (angiotensin 1-7 and bradikinin) and improved nitric oxide metabolism. Polyphenol treatment restored the left intraventricular pressure and cardiac mechanical work. We conclude that Ro and Co treatment attenuate morphological and functional ischemic-related changes by both an oxidant load reduction and improvement of the balance between vasoconstrictors and vasodilators.

  9. Extracts of Crataegus oxyacantha and Rosmarinus officinalis Attenuate Ischemic Myocardial Damage by Decreasing Oxidative Stress and Regulating the Production of Cardiac Vasoactive Agents

    PubMed Central

    Cuevas-Durán, Raúl Enrique; Medrano-Rodríguez, Juan Carlos; Sánchez-Aguilar, María; Soria-Castro, Elizabeth; Del Valle-Mondragón, Leonardo; Sánchez-Mendoza, Alicia; Torres-Narvaéz, Juan Carlos; Pastelín-Hernández, Gustavo; Ibarra-Lara, Luz

    2017-01-01

    Numerous studies have supported a role for oxidative stress in the development of ischemic damage and endothelial dysfunction. Crataegus oxyacantha (Co) and Rosmarinus officinalis (Ro) extracts are polyphenolic-rich compounds that have proven to be efficient in the treatment of cardiovascular diseases. We studied the effect of extracts from Co and Ro on the myocardial damage associated with the oxidative status and to the production of different vasoactive agents. Rats were assigned to the following groups: (a) sham; (b) vehicle-treated myocardial infarction (MI) (MI-V); (c) Ro extract-treated myocardial infarction (MI-Ro); (d) Co extract-treated myocardial infarction (MI-Co); or (e) Ro+Co-treated myocardial infarction (MI-Ro+Co). Ro and Co treatments increased total antioxidant capacity, the expression of superoxide dismutase (SOD)-Cu2+/Zn2+, SOD-Mn2+, and catalase, with the subsequent decline of malondialdehyde and 8-hydroxy-2′-deoxyguanosine levels. The extracts diminished vasoconstrictor peptide levels (angiotensin II and endothelin-1), increased vasodilators agents (angiotensin 1–7 and bradikinin) and improved nitric oxide metabolism. Polyphenol treatment restored the left intraventricular pressure and cardiac mechanical work. We conclude that Ro and Co treatment attenuate morphological and functional ischemic-related changes by both an oxidant load reduction and improvement of the balance between vasoconstrictors and vasodilators. PMID:29135932

  10. Amidine-Functionalized Poly(2-vinyl-4,4-dimethylazlactone) for Selective and Efficient CO 2 Fixing

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Barkakaty, Balaka; Browning, Katie L.; Sumpter, Bobby

    Development of novel polymeric materials capable of efficient CO 2 capture and separation under ambient conditions is crucial for cost-effective and practical industrial applications. Here we report the facile synthesis of a new CO 2-responsive polymer through post-polymerization modification of poly(2 vinyl-4,4-dimethylazlactone) (PVDMA). The reactive pendant azlactone groups of PVDMA are easily modified with 4-(N-methyltetrahydropyrimidine) benzyl alcohol (PBA) without any by-product formation. FTIR and TGA experiments show the new PBA functionalized polymer powder can reversibly capture CO 2 at room temperature and under atmospheric pressure. CO2 capture was selective, showing a high fixing efficiency even with a mixed gas systemmore » (20% CO 2, 80% N 2) similar to flue gas. CO 2 release occurred at room temperature and release profiles were investigated as a function of temperature. Density Functional Theory (DFT) calculations coupled with modeling and simulation reveal the presence of two CO 2 binding sites in the PBA functionalized polymer resulting in a two-step CO 2 release at room temperature. Finally, we find that the ease of material preparation, high fixing efficiency, and robust release characteristics suggest that post-polymerization modification may be a useful route to designing new materials for CO 2 capture.« less

  11. Amidine-Functionalized Poly(2-vinyl-4,4-dimethylazlactone) for Selective and Efficient CO 2 Fixing

    DOE PAGES

    Barkakaty, Balaka; Browning, Katie L.; Sumpter, Bobby; ...

    2016-02-12

    Development of novel polymeric materials capable of efficient CO 2 capture and separation under ambient conditions is crucial for cost-effective and practical industrial applications. Here we report the facile synthesis of a new CO 2-responsive polymer through post-polymerization modification of poly(2 vinyl-4,4-dimethylazlactone) (PVDMA). The reactive pendant azlactone groups of PVDMA are easily modified with 4-(N-methyltetrahydropyrimidine) benzyl alcohol (PBA) without any by-product formation. FTIR and TGA experiments show the new PBA functionalized polymer powder can reversibly capture CO 2 at room temperature and under atmospheric pressure. CO2 capture was selective, showing a high fixing efficiency even with a mixed gas systemmore » (20% CO 2, 80% N 2) similar to flue gas. CO 2 release occurred at room temperature and release profiles were investigated as a function of temperature. Density Functional Theory (DFT) calculations coupled with modeling and simulation reveal the presence of two CO 2 binding sites in the PBA functionalized polymer resulting in a two-step CO 2 release at room temperature. Finally, we find that the ease of material preparation, high fixing efficiency, and robust release characteristics suggest that post-polymerization modification may be a useful route to designing new materials for CO 2 capture.« less

  12. Heterogenised Molecular Catalysts for the Reduction of CO₂ to Fuels.

    PubMed

    Windle, Christopher D; Reisner, Erwin

    2015-08-19

    CO2 conversion provides a possible solution to curtail the growing CO2 levels in our atmosphere and reduce dependence on fossil fuels. To this end, it is essential to develop efficient catalysts for the reduction of CO2. The structure and activity of molecular CO2 reduction catalysts can be tuned and they offer good selectivity with reasonable stability. Heterogenisation of these molecules reduces solvent restrictions, facilitates recyclability and can dramatically improve activity by preventing catalyst inactivation and perturbing the kinetics of intermediates. The nature and morphology of the solid-state material upon which the catalyst is immobilised can significantly influence the activity of the hybrid assembly. Although work in this area began forty years ago, it has only drawn substantial attention in recent years. This review article gives an overview of the historical development of the field.

  13. Supercritical CO2 extraction of beta-carotene from a marine strain of the cyanobacterium Synechococcus species.

    PubMed

    Montero, Olimpio; Macías-Sánchez, Maria Dolores; Lama, Carmen M; Lubián, Luis M; Mantell, Casimiro; Rodríguez, Miguel; de la Ossa, Enrique M

    2005-12-14

    Dynamic extraction of carotenoids from a marine strain of Synechococcus sp. (Cyanophyceae) with supercritical CO2 (SC-CO2) was investigated with regard to operation pressure and temperature effects on extraction efficiency. Extraction yield (milligrams of pigment per gram of dry weight) for SC-CO2) was compared with the extraction yield for dimethylformamide (DMF). Carotenoids extracted with SC-CO2 were beta-carotene (Ct), zeaxanthin (Z), beta-cryptoxanthin (Cr), and equinenone; chlorophyll a was poorly extracted, whereas myxoxanthophyll, another major carotenoid, was not extracted under any experimental condition. The highest relative yield, which is defined here as y(r) = [(mg of pigment(SC-CO2)/mg of pigment(DMF))] x 100, was 76.1 +/- 8.6% for Ct, but it rose to 87.0 +/- 3.4% when 15% ethanol was used as cosolvent. The pressure effect on y(r) was found to be significant (p < 0.05) for both Cr and Z, along with total carotenoids, whereas the effect of square T (TT) was significant for only Ct. From empirical correlations, pairwise pressure (bar) and temperature (degrees C), respectively, for optimal extraction were determined to be (358, 50) for Ct, (454, 59) for Cr, and (500, 60) for Z. Cell disruption by sonication or detergent treatment of the biomass did not improve the extraction efficiency. Matrix structure together with material state could explain the low carotenoid extraction yield obtained with SC-CO2 as compared to DMF in Synechococcus sp. However, the process can be applied to selective extraction of different carotenoids.

  14. Enhanced interfacial electron transfer of inverted perovskite solar cells by introduction of CoSe into the electron-transporting-layer

    NASA Astrophysics Data System (ADS)

    Chen, Shanshan; Yang, Songwang; Sun, Hong; Zhang, Lu; Peng, Jiajun; Liang, Ziqi; Wang, Zhong-Sheng

    2017-06-01

    To improve the electron transfer at the interface between the perovskite film and the electron-transporting-material (ETM) layer, CoSe doped [6,6]-phenyl C61-butyric acid methyl ester (PCBM) is employed as the ETM layer for the inverted planar perovskite solar cell with NiO as the hole-transporting-material layer. Introduction of CoSe (5.8 wt%) into the PCBM layer improves the conductivity of the ETM layer and decreases the photoluminescence intensity, thus enhancing the interfacial electron extraction and reducing the electron transfer resistance at the perovskite/ETM interface. As a consequence, the power conversion efficiency is enhanced from 11.43% to 14.91% by 30% due to the noted increases in short-circuit current density from 17.95 mA cm-2 to 19.85 mA cm-2 and fill factor from 0.60 to 0.70. This work provides a new strategy to improve the performance of inverted perovskite solar cells.

  15. Bimetallic platinum group metal-free catalysts for high power generating microbial fuel cells

    NASA Astrophysics Data System (ADS)

    Kodali, Mounika; Santoro, Carlo; Herrera, Sergio; Serov, Alexey; Atanassov, Plamen

    2017-10-01

    M1-M2-N-C bimetallic catalysts with M1 as Fe and Co and M2 as Fe, Co, Ni and Mn were synthesized and investigated as cathode catalysts for oxygen reduction reaction (ORR). The catalysts were prepared by Sacrificial Support Method in which silica was the template and aminoantipyrine (AAPyr) was the organic precursor. The electro-catalytic properties of these catalysts were investigated by using rotating ring disk (RRDE) electrode setup in neutral electrolyte. Fe-Mn-AAPyr outperformed Fe-AAPyr that showed higher performances compared to Fe-Co-AAPyr and Fe-Ni-AAPyr in terms of half-wave potential. In parallel, Fe-Co-AAPyr, Co-Mn-AAPyr and Co-Ni-AAPyr outperformed Co-AAPyr. The presence of Co within the catalyst contributed to high peroxide production not desired for efficient ORR. The catalytic capability of the catalysts integrated in air-breathing cathode was also verified. It was found that Co-based catalysts showed an improvement in performance by the addition of second metal compared to simple Co- AAPyr. Fe-based bimetallic materials didn't show improvement compared to Fe-AAPyr with the exception of Fe-Mn-AAPyr catalyst that had the highest performance recorded in this study with maximum power density of 221.8 ± 6.6 μWcm-2. Activated carbon (AC) was used as control and had the lowest performances in RRDE and achieved only 95.6 ± 5.8 μWcm-2 when tested in MFC.

  16. Development of a preprototype sabatier CO2 reduction subsystem

    NASA Technical Reports Server (NTRS)

    Kleiner, G. N.; Birbara, P.

    1980-01-01

    A preoprototype Sabatier CO2 Reduction Subsystem was successfully designed, fabricated and tested. The lightweight, quick starting reactor utilizes a highly active and physically durable methanation catalyst composed of ruthenium on alumina. The use of this improved catalyst permits a single straight through plug flow design with an average lean component H2/CO2 conversion efficiency of over 99% over a range of H2/CO2 molar ratios of 1.8 to 5 while operating with flows equivalent to a crew size of one person steadystate to 3 persons cyclical (equivalent to 5 persons steady state). The reactor requires no heater operation after start-up even during simulated 55 minute lightside/39 minute darkside orbital operation over the above range of molar ratios and crew loadings. The subsystem's operation and performance is controlled by a microprocessor and displayed on a nineteen inch multi-colored cathode ray tube.

  17. Influence of Na+, K+, Mn2+, Fe2+ and Zn2+ ions on the electrodeposition of Ni-Co alloys: Implications for the recycling of Ni-MH batteries

    NASA Astrophysics Data System (ADS)

    Blanco, S.; Orta-Rodriguez, R.; Delvasto, P.

    2017-01-01

    A hydrometallurgical recycling procedure for the recovery of a mixed rare earths sulfate and an electrodeposited Ni-Co alloy has been described. The latter step was found to be complex, due to the presence of several ions in the battery electrode materials. Electrochemical evaluation of the influence of the ions on the Ni-Co alloy deposition was carried out by cyclic voltammetry test. It was found that ions such as K+, Fe2+ and Mn2+ improved the current efficiency for the Ni-Co deposition process on a copper surface. On the other hand, Na+ and Zn2+ ions exhibited a deleterious behaviour, minimizing the values of the reduction current. The results were used to suggest the inclusion of additional steps in the process flow diagram of the recycling operation, in order to eliminate deleterious ions from the electroplating solution.

  18. Temperature dependence of spin-orbit torques in Pt/Co/Pt multilayers

    NASA Astrophysics Data System (ADS)

    Chen, Shiwei; Li, Dong; Cui, Baoshan; Xi, Li; Si, Mingsu; Yang, Dezheng; Xue, Desheng

    2018-03-01

    We studied the current-induced spin-orbit torques in a perpendicularly magnetized Pt (1 nm)/Co (0.8 nm)/Pt (5 nm) heterojunction by harmonic Hall voltage measurements. Owing to similar Pt/Co/Pt interfaces, the spin-orbit torques originated from the Rashba effect are reduced, but the contribution from the spin Hall effect is still retained because of asymmetrical Pt thicknesses. When the temperature increases from 50 to 300 K, two orthogonal components of the effective field, induced by spin-orbit torques, reveal opposite temperature dependencies: the field-like term (transverse effective field) decreases from 2.3 to 2.1 (10-6 Oe (A cm-2)-1), whereas the damping-like term (longitudinal effective field) increases from 3.7 to 4.8 (10-6 Oe (A cm-2)-1). It is noticed that the damping-like term, usually smaller than the field-like term in the similar Pt/Co interfaces, is twice as large as the field-like term. As a result, the damping-like spin-orbit torque reaches an efficiency of 0.15 at 300 K. Such a temperature-dependent damping-like term in a Pt/Co/Pt heterojunction can efficiently reduce the switching current density which is 2.30  ×  106 A cm-2 at 300 K, providing an opportunity to further improve and understand spin-orbit torques induced by spin Hall effect.

  19. Extramitochondrial domain rich in carbonic anhydrase activity improves myocardial energetics.

    PubMed

    Schroeder, Marie A; Ali, Mohammad A; Hulikova, Alzbeta; Supuran, Claudiu T; Clarke, Kieran; Vaughan-Jones, Richard D; Tyler, Damian J; Swietach, Pawel

    2013-03-05

    CO2 is produced abundantly by cardiac mitochondria. Thus an efficient means for its venting is required to support metabolism. Carbonic anhydrase (CA) enzymes, expressed at various sites in ventricular myocytes, may affect mitochondrial CO2 clearance by catalyzing CO2 hydration (to H(+) and HCO3(-)), thereby changing the gradient for CO2 venting. Using fluorescent dyes to measure changes in pH arising from the intracellular hydration of extracellularly supplied CO2, overall CA activity in the cytoplasm of isolated ventricular myocytes was found to be modest (2.7-fold above spontaneous kinetics). Experiments on ventricular mitochondria demonstrated negligible intramitochondrial CA activity. CA activity was also investigated in intact hearts by (13)C magnetic resonance spectroscopy from the rate of H(13)CO3(-) production from (13)CO2 released specifically from mitochondria by pyruvate dehydrogenase-mediated metabolism of hyperpolarized [1-(13)C]pyruvate. CA activity measured upon [1-(13)C]pyruvate infusion was fourfold higher than the cytoplasm-averaged value. A fluorescent CA ligand colocalized with a mitochondrial marker, indicating that mitochondria are near a CA-rich domain. Based on immunoreactivity, this domain comprises the nominally cytoplasmic CA isoform CAII and sarcoplasmic reticulum-associated CAXIV. Inhibition of extramitochondrial CA activity acidified the matrix (as determined by fluorescence measurements in permeabilized myocytes and isolated mitochondria), impaired cardiac energetics (indexed by the phosphocreatine-to-ATP ratio measured by (31)P magnetic resonance spectroscopy of perfused hearts), and reduced contractility (as measured from the pressure developed in perfused hearts). These data provide evidence for a functional domain of high CA activity around mitochondria to support CO2 venting, particularly during elevated and fluctuating respiratory activity. Aberrant distribution of CA activity therefore may reduce the heart's energetic efficiency.

  20. Efficient electrochemical refrigeration power plant using natural gas with ∼100% CO2 capture

    NASA Astrophysics Data System (ADS)

    Al-musleh, Easa I.; Mallapragada, Dharik S.; Agrawal, Rakesh

    2015-01-01

    We propose an efficient Natural Gas (NG) based Solid Oxide Fuel Cell (SOFC) power plant equipped with ∼100% CO2 capture. The power plant uses a unique refrigeration based process to capture and liquefy CO2 from the SOFC exhaust. The capture of CO2 is carried out via condensation and purification using two rectifying columns operating at different pressures. The uncondensed gas mixture, comprising of relatively high purity unconverted fuel, is recycled to the SOFC and found to boost the power generation of the SOFC by 22%, when compared to a stand alone SOFC. If Liquefied Natural Gas (LNG) is available at the plant gate, then the refrigeration available from its evaporation is used for CO2 Capture and Liquefaction (CO2CL). If NG is utilized, then a Mixed Refrigerant (MR) vapor compression cycle is utilized for CO2CL. Alternatively, the necessary refrigeration can be supplied by evaporating the captured liquid CO2 at a lower pressure, which is then compressed to supercritical pressures for pipeline transportation. From rigorous simulations, the power generation efficiency of the proposed processes is found to be 70-76% based on lower heating value (LHV). The benefit of the proposed processes is evident when the efficiency of 73% for a conventional SOFC-Gas turbine power plant without CO2 capture is compared with an equivalent efficiency of 71.2% for the proposed process with CO2CL.

  1. Photocatalytic Degradation of 4-Nitrophenol by C, N-TiO2: Degradation Efficiency vs. Embryonic Toxicity of the Resulting Compounds

    NASA Astrophysics Data System (ADS)

    Osin, Oluwatomiwa A.; Yu, Tianyu; Cai, Xiaoming; Jiang, Yue; Peng, Guotao; Cheng, Xiaomei; Li, Ruibin; Qin, Yao; Lin, Sijie

    2018-06-01

    The photocatalytic activity of TiO2 based photocatalysts can be improved by structural modification and elemental doping. In this study, through rational design, one type of carbon and nitrogen co-doped TiO2 (C, N-TiO2) photocatalyst with mesoporous structure was synthesized with improved photocatalytic activity in degrading 4-nitrophenol under simulated sunlight irradiation. The photocatalytic degradation efficiency of the C, N-TiO2 was much higher than the anatase TiO2 (A-TiO2) based on absorbance and HPLC analyses. Moreover, using zebrafish embryos, we showed that the intermediate degradation compounds generated by photocatalytic degradation of 4-nitrophenol had higher toxicity than the parent compound. A repeated degradation process was necessary to render complete degradation and non-toxicity to the zebrafish embryos. Our results demonstrated the importance of evaluating the photocatalytic degradation efficiency in conjunction with the toxicity assessment of the degradation compounds.

  2. Photocatalytic Degradation of 4-Nitrophenol by C, N-TiO2: Degradation Efficiency vs. Embryonic Toxicity of the Resulting Compounds.

    PubMed

    Osin, Oluwatomiwa A; Yu, Tianyu; Cai, Xiaoming; Jiang, Yue; Peng, Guotao; Cheng, Xiaomei; Li, Ruibin; Qin, Yao; Lin, Sijie

    2018-01-01

    The photocatalytic activity of TiO 2 based photocatalysts can be improved by structural modification and elemental doping. In this study, through rational design, one type of carbon and nitrogen co-doped TiO 2 (C, N-TiO 2 ) photocatalyst with mesoporous structure was synthesized with improved photocatalytic activity in degrading 4-nitrophenol under simulated sunlight irradiation. The photocatalytic degradation efficiency of the C, N-TiO 2 was much higher than the anatase TiO 2 (A-TiO 2 ) based on absorbance and HPLC analyses. Moreover, using zebrafish embryos, we showed that the intermediate degradation compounds generated by photocatalytic degradation of 4-nitrophenol had higher toxicity than the parent compound. A repeated degradation process was necessary to render complete degradation and non-toxicity to the zebrafish embryos. Our results demonstrated the importance of evaluating the photocatalytic degradation efficiency in conjunction with the toxicity assessment of the degradation compounds.

  3. Cu-BTC/aminated graphite oxide composites as high-efficiency CO2 capture media.

    PubMed

    Policicchio, Alfonso; Zhao, Yunxia; Zhong, Qin; Agostino, Raffaele G; Bandosz, Teresa J

    2014-01-08

    CO2 adsorption isotherms on Cu-BTC/aminated graphite oxide composites were measured in the pressure range up to 1.5 MPa at three different temperatures close to ambient. Adsorption capacity, isosteric heat of adsorption, and regenerability were investigated. They are considered as significant factors determining the practical application of materials for CO2 capture. The results indicate a significant improvement in the performance of the composites as CO2 adsorbents in comparison with the parent Cu-BTC MOF. Among all samples analyzed, the composite of Cu-BTC and modified graphite oxide with the highest N content (MOF/GO-U3) is the best performing sample. On its surface 13.41 mmol/g CO2 was adsorbed at room temperature and 1.5 MPa. A high selectivity for CO2 adsorption over that of CH4 was found. The selectivities for CO2 adsorption over N2 are governed by the properties of the MOF phase. A relatively low heat of CO2 adsorption and the high degree of surface homogeneity cause that the composites can be fully regenerated and used in multicycle adsorption with the minimum energy demand.

  4. Control system of an excitation power supply for fast axial flow CO2 lasersupda

    NASA Astrophysics Data System (ADS)

    Li, Bo; Jia, Xinting; Yuan, Hao; Gao, Yuhu; Wang, Youqing

    2009-08-01

    A switching power control system of fast axial flow CO2 lasers based on DSP is presented. The key techniques are described in detail, include the control principle, realization method and program design. The experiment showed that the system make the laser discharge stably and work in multi-mode. The discharge current can be adjusted from 3mA to 85mA continuously. 20-2000Hz frequency, 0-100% duty cycle laser pulse is achieved. The power supply can improve the processing efficiency and quality.

  5. One crop breeding cycle from starvation? How engineering crop photosynthesis for rising CO2 and temperature could be one important route to alleviation.

    PubMed

    Kromdijk, Johannes; Long, Stephen P

    2016-03-16

    Global climate change is likely to severely impact human food production. This comes at a time when predicted demand for primary foodstuffs by a growing human population and changing global diets is already outpacing a stagnating annual rate of increase in crop productivity. Additionally, the time required by crop breeding and bioengineering to release improved varieties to farmers is substantial, meaning that any crop improvements needed to mitigate food shortages in the 2040s would need to start now. In this perspective, the rationale for improvements in photosynthetic efficiency as a breeding objective for higher yields is outlined. Subsequently, using simple simulation models it is shown how predicted changes in temperature and atmospheric [CO2] affect leaf photosynthetic rates. The chloroplast accounts for the majority of leaf nitrogen in crops. Within the chloroplast about 25% of nitrogen is invested in the carboxylase, Rubisco, which catalyses the first step of CO2 assimilation. Most of the remaining nitrogen is invested in the apparatus to drive carbohydrate synthesis and regenerate ribulose-1:5-bisphosphate (RuBP), the CO2-acceptor molecule at Rubisco. At preindustrial [CO2], investment in these two aspects may have been balanced resulting in co-limitation. At today's [CO2], there appears to be over-investment in Rubisco, and despite the counter-active effects of rising temperature and [CO2], this imbalance is predicted to worsen with global climate change. By breeding or engineering restored optimality under future conditions increased productivity could be achieved in both tropical and temperate environments without additional nitrogen fertilizer. Given the magnitude of the potential shortfall, better storage conditions, improved crop management and better crop varieties will all be needed. With the short time-scale at which food demand is expected to outpace supplies, all available technologies to improve crop varieties, from classical crop breeding to crop genetic engineering should be employed. This will require vastly increased public and private investment to support translation of first discovery in laboratories to replicated field trials, and an urgent re-evaluation of regulation of crop genetic engineering. © 2016 The Authors.

  6. Photo-reduction of CO2 Using a Rhenium Complex Covalently Supported on a Graphene/TiO2 Composite.

    PubMed

    Cui, Shi-Cong; Sun, Xue-Zhong; Liu, Jin-Gang

    2016-07-07

    One of the promising solutions for decreasing atmospheric CO2 is artificial photosynthesis, in which CO2 can be photoconverted into solar fuels. In this study, a rhenium complex Re(PyBn)(CO)3 Cl (PyBn=1-(2-picolyl)-4-phenyl-1H-1,2,3-triazole) was covalently grafted onto the surface of reduced graphene oxide (rGO). This was further combined with TiO2 to fabricate a novel catalyst composite TiO2 -rGO-Re(PyBn)(CO)3 Cl for CO2 photo-reduction. This hybrid composite demonstrated high selectivity conversion of CO2 into CO under xenon-lamp irradiation. Compared with the unsupported homogeneous catalyst Re(PyBn)(CO)3 Cl, the covalent immobilized catalyst composite TiO2 -rGO-Re(PyBn)(CO)3 Cl enhanced the turnover number six times and significantly improved catalyst stability. During the process of CO2 photo-reduction, intermediate species with lifetimes longer than hundreds of microseconds were observed and the formation of CO products was revealed using timeresolved infrared spectroscopy. A plausible mechanism for CO2 photo-reduction by the TiO2 -rGO-Re(PyBn)(CO)3 Cl catalyst composite has been suggested. The obtained results have implications for the future design of efficient catalyst composites for CO2 photo-conversion. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  7. In situ evolution of highly dispersed amorphous CoO x clusters for oxygen evolution reaction

    DOE PAGES

    Chen, Dawei; Dong, Chung-Li; Zou, Yuqin; ...

    2017-07-24

    Electrocatalytic water splitting is a key technique to produce hydrogen fuels, which can be considered as an efficient strategy to store renewable energy. Oxygen evolution reaction (OER) that occurs at the anode side requires a four-electron transfer under highly oxidizing conditions. OER has a large overpotential and therefore determines the overall efficiency. Certain electrocatalysts can efficiently help to improve the reaction kinetics. Owing to the high cost of precious metals such as Pt, Ru, and Ir, non-precious metal oxide catalysts have been vigorously investigated under alkaline conditions. Herein, we synthesized novel highly dispersed amorphous CoO x for the first timemore » in the form of a cluster favorable to enhance the OER activity using a facile method via the air dielectric barrier discharge (DBD) plasma. Compared with the pristine biopolymer–cobalt complex, the amorphous CoO x cluster exhibits a much higher current density and a lower overpotential for OER, e.g., the overpotential of 290 mV at 10 mA cm -2 and the overpotential of only 350 mV at 300 mA cm -1. The excellent electrocatalytic OER activity was attributed to the unsaturated catalytic sites on the amorphous CoO x cluster. In addition, we studied the reaction mechanism, and it was observed that pure O 2 DBD plasma could lead to the evolution of crystalline CoO x; however, the presence of N 2 and O 2 in DBD plasma could ensure the facile evolution of amorphous CoO x clusters. This study provides a new strategy, therefore, to design amorphous materials for electrocatalysis and beyond.« less

  8. In situ evolution of highly dispersed amorphous CoO x clusters for oxygen evolution reaction

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Chen, Dawei; Dong, Chung-Li; Zou, Yuqin

    Electrocatalytic water splitting is a key technique to produce hydrogen fuels, which can be considered as an efficient strategy to store renewable energy. Oxygen evolution reaction (OER) that occurs at the anode side requires a four-electron transfer under highly oxidizing conditions. OER has a large overpotential and therefore determines the overall efficiency. Certain electrocatalysts can efficiently help to improve the reaction kinetics. Owing to the high cost of precious metals such as Pt, Ru, and Ir, non-precious metal oxide catalysts have been vigorously investigated under alkaline conditions. Herein, we synthesized novel highly dispersed amorphous CoO x for the first timemore » in the form of a cluster favorable to enhance the OER activity using a facile method via the air dielectric barrier discharge (DBD) plasma. Compared with the pristine biopolymer–cobalt complex, the amorphous CoO x cluster exhibits a much higher current density and a lower overpotential for OER, e.g., the overpotential of 290 mV at 10 mA cm -2 and the overpotential of only 350 mV at 300 mA cm -1. The excellent electrocatalytic OER activity was attributed to the unsaturated catalytic sites on the amorphous CoO x cluster. In addition, we studied the reaction mechanism, and it was observed that pure O 2 DBD plasma could lead to the evolution of crystalline CoO x; however, the presence of N 2 and O 2 in DBD plasma could ensure the facile evolution of amorphous CoO x clusters. This study provides a new strategy, therefore, to design amorphous materials for electrocatalysis and beyond.« less

  9. An Effective Way to Optimize the Functionality of Graphene-Based Nanocomposite: Use of the Colloidal Mixture of Graphene and Inorganic Nanosheets

    NASA Astrophysics Data System (ADS)

    Jin, Xiaoyan; Adpakpang, Kanyaporn; Young Kim, In; Mi Oh, Seung; Lee, Nam-Suk; Hwang, Seong-Ju

    2015-06-01

    The best electrode performance of metal oxide-graphene nanocomposite material for lithium secondary batteries can be achieved by using the colloidal mixture of layered CoO2 and graphene nanosheets as a precursor. The intervention of layered CoO2 nanosheets in-between graphene nanosheets is fairly effective in optimizing the pore and composite structures of the Co3O4-graphene nanocomposite and also in enhancing its electrochemical activity via the depression of interaction between graphene nanosheets. The resulting CoO2 nanosheet-incorporated nanocomposites show much greater discharge capacity of ~1750 mAhg-1 with better cyclability and rate characteristics than does CoO2-free Co3O4-graphene nanocomposite (~1100 mAhg-1). The huge discharge capacity of the present nanocomposite is the largest one among the reported data of cobalt oxide-graphene nanocomposite. Such a remarkable enhancement of electrode performance upon the addition of inorganic nanosheet is also observed for Mn3O4-graphene nanocomposite. The improvement of electrode performance upon the incorporation of inorganic nanosheet is attributable to an improved Li+ ion diffusion, an enhanced mixing between metal oxide and graphene, and the prevention of electrode agglomeration. The present experimental findings underscore an efficient and universal role of the colloidal mixture of graphene and redoxable metal oxide nanosheets as a precursor for improving the electrode functionality of graphene-based nanocomposites.

  10. Spinel Co3O4 nanomaterials for efficient and stable large area carbon-based printed perovskite solar cells.

    PubMed

    Bashir, Amna; Shukla, Sudhanshu; Lew, Jia Haur; Shukla, Shashwat; Bruno, Annalisa; Gupta, Disha; Baikie, Tom; Patidar, Rahul; Akhter, Zareen; Priyadarshi, Anish; Mathews, Nripan; Mhaisalkar, Subodh G

    2018-02-01

    Carbon based perovskite solar cells (PSCs) are fabricated through easily scalable screen printing techniques, using abundant and cheap carbon to replace the hole transport material (HTM) and the gold electrode further reduces costs, and carbon acts as a moisture repellent that helps in maintaining the stability of the underlying perovskite active layer. An inorganic interlayer of spinel cobaltite oxides (Co 3 O 4 ) can greatly enhance the carbon based PSC performance by suppressing charge recombination and extracting holes efficiently. The main focus of this research work is to investigate the effectiveness of Co 3 O 4 spinel oxide as the hole transporting interlayer for carbon based perovskite solar cells (PSCs). In these types of PSCs, the power conversion efficiency (PCE) is restricted by the charge carrier transport and recombination processes at the carbon-perovskite interface. The spinel Co 3 O 4 nanoparticles are synthesized using the chemical precipitation method, and characterized by X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM) and UV-Vis spectroscopy. A screen printed thin layer of p-type inorganic spinel Co 3 O 4 in carbon PSCs provides a better-energy level matching, superior efficiency, and stability. Compared to standard carbon PSCs (PCE of 11.25%) an improved PCE of 13.27% with long-term stability, up to 2500 hours under ambient conditions, is achieved. Finally, the fabrication of a monolithic perovskite module is demonstrated, having an active area of 70 cm 2 and showing a power conversion efficiency of >11% with virtually no hysteresis. This indicates that Co 3 O 4 is a promising interlayer for efficient and stable large area carbon PSCs.

  11. Cytosolic co-delivery of miRNA-34a and docetaxel with core-shell nanocarriers via caveolae-mediated pathway for the treatment of metastatic breast cancer

    NASA Astrophysics Data System (ADS)

    Zhang, Li; Yang, Xin; Lv, Yaqi; Xin, Xiaofei; Qin, Chao; Han, Xiaopeng; Yang, Lei; He, Wei; Yin, Lifang

    2017-04-01

    Co-delivery of microRNAs and chemotherapeutic drugs into tumor cells is an attractive strategy for synergetic breast cancer therapy due to their complementary mechanisms. In this work, a core-shell nanocarrier coated by cationic albumin was developed to simultaneously deliver miRNA-34a and docetaxel (DTX) into breast cancer cells for improved therapeutic effect. The co-delivery nanocarriers showed a spherical morphology with an average particle size of 183.9 nm, and they efficiently protected miRNA-34a from degradation by RNase and serum. Importantly, the nanocarriers entered the cytosol via a caveolae-mediated pathway without entrapment in endosomes/lysosomes, thus improving the utilization of the cargo. In vitro, the co-delivery nanocarriers suppressed the expression of anti-apoptosis gene Bcl-2 at both transcription and protein levels, inhibited tumor cell migration and efficiently induced cell apoptosis and cytotoxicity. In vivo, the co-delivery nanocarriers prolonged the blood circulation of DTX, enhanced tumor accumulation of the cargo and significantly inhibited tumor growth and metastasis in 4T1-tumor bearing mice models. Taken together, the present nanocarrier co-loading with DTX and miRNA-34a is a new nanoplatform for the combination of insoluble drugs and gene/protein drugs and provides a promising strategy for the treatment of metastatic breast cancer.

  12. Antidiabetic effects of cinnamon oil in diabetic KK-Ay mice.

    PubMed

    Ping, Hua; Zhang, Guijun; Ren, Guixing

    2010-01-01

    The hypoglycemic effect of cinnamon oil (CO) in a type 2 diabetic animal model (KK-A(y) mice) was studied. The main component of CO was cinnamaldehyde, and other nineteen components were also determined. CO was administrated at doses of 25, 50 and 100mg/kg for 35 days. It was found that fasting blood glucose concentration was significantly decreased (P<0.05) with the 100mg/kg group (P<0.01) the most efficient compared with the diabetic control group. In addition, there was significant decrease in plasma C-peptide, serum triglyceride, total cholesterol and blood urea nitrogen levels while serum high density lipoprotein (HDL)-cholesterol levels were significantly increased after 35 days. Meanwhile, glucose tolerance was improved, and the immunoreactive of pancreatic islets beta-cells was promoted. These results suggest that CO had a regulative role in blood glucose level and lipids, and improved the function of pancreatic islets. Cinnamon oil may be useful in the treatment of type 2 diabetes mellitus. Copyright (c) 2010 Elsevier Ltd. All rights reserved.

  13. Design of experiment analysis of CO2 dielectric barrier discharge conditions on CO production

    NASA Astrophysics Data System (ADS)

    Becker, Markus; Ponduri, Srinath; Engeln, Richard; van de Sanden, Richard; Loffhagen, Detlef

    2016-09-01

    Dielectric barrier discharges (DBD) are frequently used for the generation of CO from CO2 which is of particular interest for syngas production. It has been found by means of fluid modelling in that the CO2 conversion frequency in a CO2 DBD depends linearly on the specific energy input (SEI) while the energy efficiency of CO production is only weakly dependent on the SEI. Here, the same numerical model as in is applied to study systematically the influence of gas pressure, applied voltage amplitude and frequency on the CO2 conversion frequency and the energy efficiency of CO production based on a 2-level 3-factor full factorial experimental design. It is found that the operating conditions of the CO2 DBD for CO production can be chosen to either have an optimal throughput or a better energy efficiency. This work was partly supported by the German Research Foundation within the Collaborative Research Centre Transregio 24.

  14. Microfluidic diffusivity meter: a tool to optimize CO2 driven enhanced oil recovery

    NASA Astrophysics Data System (ADS)

    Puneeth, S. B.; Kim, Young Ho; Goel, Sanket

    2017-02-01

    As the energy demands continue to swell with growing population and there persists a lack of unexploited oilfields, the prime focus of any nation would be to maximize the oil recovery factor from existing oil fields. CO2-Enhanced oil recovery is a process to improve the recovery of crude oil from an oil field and works at high pressure and in very deep conditions. CO2 and oil are miscible at high pressure, resulting in low viscosity and oil swells. This swelling can be measured based on mathematical calculations in real time and correlated with the CO2 concentration. This process has myriad advantages over its counterparts which include being able to harness oil trapped in reservoirs besides being cheaper and more efficient. A Diffusivity meter is inevitable in the measurement of the diffusion co-efficient of two samples. Diffusivity meters currently available in the market are weighed down by disadvantages like the requirement of large samples for testing, high cost and complexity. This elicits the need for a Microfluidic based diffusivity meter capable of analyzing Nano-liter sample volumes besides being more precise and affordable. The scope of this work involves the design and development of a Microfluidic robust and inexpensive prototype diffusivity meter using a capillary tube and endorsing its performance by comparison of results with known diffusivity range and supervision of the results with an electronic microscope coupled to PC and Data Acquisition System. The prototype produced at the end of the work is expected to outweigh disadvantages in existing products in terms of sample size, efficiency and time saving.

  15. Direct conversion of CO 2 to meso/macro-porous frameworks of surface-microporous graphene for efficient asymmetrical supercapacitors

    DOE PAGES

    Chang, Liang; Stacchiola, Dario J.; Hu, Yun Hang

    2017-10-11

    CO 2 conversion to useful materials is the most attractive approach to control its content in the atmosphere. An ideal electrode material for supercapacitors should possess suitable meso/macro-pores as electrolyte reservoirs and rich micro-pores as places for the adsorption of electrolyte ions. In this paper, we designed and synthesized such an ideal material, meso/macro-porous frameworks of surface-microporous graphene (MFSMG), from CO 2via its one-step exothermic reaction with potassium. Furthermore, the MFSMG electrode exhibited a high gravimetric capacitance of 178 F g -1 at 0.2 A g -1 in 2 M KOH and retained 85% capacitance after increasing current density bymore » 50 times. The combination of the MFSMG electrode and the activated carbon (AC) electrode constructed an asymmetrical AC//MFSMG capacitor, leading to a high capacitance of 242.4 F g -1 for MFSMG and 97.4 F g -1 for AC. With the extended potential, the asymmetrical capacitor achieved an improved energy density of 9.43 W h kg -1 and a power density of 3504 W kg -1. Finally, this work provides a novel solution to solve the CO 2 issue and creates an efficient electrode material for supercapacitors.« less

  16. Plastid transformation for Rubisco engineering and protocols for assessing expression.

    PubMed

    Whitney, Spencer M; Sharwood, Robert E

    2014-01-01

    The assimilation of CO2 within chloroplasts is catalyzed by the bi-functional enzyme ribulose-1,5-bisphosphate carboxylase/oxygenase, Rubisco. Within higher plants the Rubisco large subunit gene, rbcL, is encoded in the plastid genome, while the Rubisco small subunit gene, RbcS is coded in the nucleus by a multi-gene family. Rubisco is considered a poor catalyst due to its slow turnover rate and its additional fixation of O2 that can result in wasteful loss of carbon through the energy requiring photorespiratory cycle. Improving the carboxylation efficiency and CO2/O2 selectivity of Rubisco within higher plants has been a long-term goal which has been greatly advanced in recent times using plastid transformation techniques. Here we present experimental methodologies for efficiently engineering Rubisco in the plastids of a tobacco master-line and analyzing leaf Rubisco content.

  17. Differential CO2 effect on primary carbon metabolism of flag leaves in durum wheat (Triticum durum Desf.).

    PubMed

    Aranjuelo, Iker; Erice, Gorka; Sanz-Sáez, Alvaro; Abadie, Cyril; Gilard, Françoise; Gil-Quintana, Erena; Avice, Jean-Christophe; Staudinger, Christiana; Wienkoop, Stefanie; Araus, Jose L; Bourguignon, Jacques; Irigoyen, Juan J; Tcherkez, Guillaume

    2015-12-01

    C sink/source balance and N assimilation have been identified as target processes conditioning crop responsiveness to elevated CO2 . However, little is known about phenology-driven modifications of C and N primary metabolism at elevated CO2 in cereals such as wheat. Here, we examined the differential effect of elevated CO2 at two development stages (onset of flowering, onset of grain filling) in durum wheat (Triticum durum, var. Sula) using physiological measurements (photosynthesis, isotopes), metabolomics, proteomics and (15) N labelling. Our results show that growth at elevated CO2 was accompanied by photosynthetic acclimation through a lower internal (mesophyll) conductance but no significant effect on Rubisco content, maximal carboxylation or electron transfer. Growth at elevated CO2 altered photosynthate export and tended to accelerate leaf N remobilization, which was visible for several proteins and amino acids, as well as lysine degradation metabolism. However, grain biomass produced at elevated CO2 was larger and less N rich, suggesting that nitrogen use efficiency rather than photosynthesis is an important target for improvement, even in good CO2 -responsive cultivars. © 2015 John Wiley & Sons Ltd.

  18. Evident Enhancement of Photoelectrochemical Hydrogen Production by Electroless Deposition of M-B (M = Ni, Co) Catalysts on Silicon Nanowire Arrays.

    PubMed

    Yang, Yong; Wang, Mei; Zhang, Peili; Wang, Weihan; Han, Hongxian; Sun, Licheng

    2016-11-09

    Modification of p-type Si surface by active and stable earth-abundant electrocatalysts is an effective strategy to improve the sluggish kinetics for the hydrogen evolution reaction (HER) at p-Si/electrolyte interface and to develop highly efficient and low-cost photocathodes for hydrogen production from water. To this end, Si nanowire (Si-NW) array has been loaded with highly efficient electrocatalysts, M-B (M = Ni, Co), by facile and quick electroless plating to build M-B catalyst-modified Si nanowire-array-textured photocathodes for water reduction to H 2 . Compared with the bare Si-NW array, composite Si-NWs/M-B arrays display evidently enhanced photoelectrochemical (PEC) performance. The onset potential (V phon ) of cathodic photocurrent is positively shifted by 530-540 mV to 0.44-0.45 V vs RHE, and the short-circuit current density (J sc ) is up to 19.5 mA cm -2 in neutral buffer solution under simulated 1 sun illumination. Impressively, the half-cell photopower conversion efficiencies (η hc ) of the optimized Si-NWs/Co-B (2.53%) and Si-NWs/Ni-B (2.45%) are comparable to that of Si-NWs/Pt (2.46%). In terms of the large J sc , V phon , and η hc values, as well as the high Faradaic efficiency, Si-NWs/M-B electrodes are among the top performing Si photocathodes which are modified with HER electrocatalysts but have no buried solid/solid junction.

  19. Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction

    PubMed Central

    2017-01-01

    Conversion of carbon monoxide (CO), a major one-carbon product of carbon dioxide (CO2) reduction, into value-added multicarbon species is a challenge to addressing global energy demands and climate change. Here we report a modular synthetic approach for aqueous electrochemical CO reduction to carbon–carbon coupled products via self-assembly of supramolecular cages at molecular–materials interfaces. Heterobimetallic cavities formed by face-to-face coordination of thiol-terminated metalloporphyrins to copper electrodes through varying organic struts convert CO to C2 products with high faradaic efficiency (FE = 83% total with 57% to ethanol) and current density (1.34 mA/cm2) at a potential of −0.40 V vs RHE. The cage-functionalized electrodes offer an order of magnitude improvement in both selectivity and activity for electrocatalytic carbon fixation compared to parent copper surfaces or copper functionalized with porphyrins in an edge-on orientation. PMID:28979945

  20. Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction

    DOE PAGES

    Gong, Ming; Cao, Zhi; Liu, Wei; ...

    2017-09-13

    Conversion of carbon monoxide (CO), a major one-carbon product of carbon dioxide (CO 2) reduction, into value-added multicarbon species is a challenge to addressing global energy demands and climate change. Here in this paper, we report a modular synthetic approach for aqueous electrochemical CO reduction to carbon-carbon coupled products via self-assembly of supramolecular cages at molecular-materials interfaces. Heterobimetallic cavities formed by face-to-face coordination of thiol-terminated metalloporphyrins to copper electrodes through varying organic struts convert CO to C2 products with high faradaic efficiency (FE = 83% total with 57% to ethanol) and current density (1.34 mA/cm 2) at a potential ofmore » -0.40 V vs RHE. The cage-functionalized electrodes offer an order of magnitude improvement in both selectivity and activity for electrocatalytic carbon fixation compared to parent copper surfaces or copper functionalized with porphyrins in an edge-on orientation.« less

  1. Sonochemical surface functionalization of exfoliated LDH: Effect on textural properties, CO2 adsorption, cyclic regeneration capacities and subsequent gas uptake for simultaneous methanol synthesis.

    PubMed

    Ezeh, Collins I; Huang, Xiani; Yang, Xiaogang; Sun, Cheng-Gong; Wang, Jiawei

    2017-11-01

    To improve CO 2 adsorption, amine modified Layered double hydroxide (LDH) were prepared via a two stage process, SDS/APTS intercalation was supported by ultrasonic irradiation and then followed by MEA extraction. The prepared samples were characterised using Scanning electron microscope-Energy dispersive X-ray spectroscopy (SEM-EDX), X-ray Photoelectron Spectroscopy (XPS), X-ray diffraction (XRD), Temperature Programmed Desorption (TPD), Brunauer-Emmett-Teller (BET), and Thermogravimetric analysis (TGA), respectively. The characterisation results were compared with those obtained using the conventional preparation method with consideration to the effect of sonochemical functionalization on textural properties, adsorption capacity, regeneration and lifetime of the LDH adsorbent. It is found that LDHs prepared by sonochemical modification had improved pore structure and CO 2 adsorption capacity, depending on sonic intensity. This is attributed to the enhanced deprotonation of activated amino functional groups via the sonochemical process. Subsequently, this improved the amine loading and effective amine efficiency by 60% of the conventional. In addition, the sonochemical process improved the thermal stability of the adsorbent and also, reduced the irreversible CO 2 uptake, CUirrev, from 0.18mmol/g to 0.03mmol/g. Subsequently, improving the lifetime and ease of regenerating the adsorbent respectively. This is authenticated by subjecting the prepared adsorbents to series of thermal swing adsorption (TSA) cycles until its adsorption capacity goes below 60% of the original CO 2 uptake. While the conventional adsorbent underwent a 10 TSA cycles before breaking down, the sonochemically functionalized LDH went further than 30 TSA cycles. Copyright © 2017 Elsevier B.V. All rights reserved.

  2. Recent Advances in Bismuth-Based Nanomaterials for Photoelectrochemical Water Splitting.

    PubMed

    Bhat, Swetha S M; Jang, Ho Won

    2017-08-10

    In recent years, bismuth-based nanomaterials have drawn considerable interest as potential candidates for photoelectrochemical (PEC) water splitting owing to their narrow band gaps, nontoxicity, and low costs. The unique electronic structure of bismuth-based materials with a well-dispersed valence band comprising Bi 6s and O 2p orbitals offers a suitable band gap to harvest visible light. This Review presents significant advancements in exploiting bismuth-based nanomaterials for solar water splitting. An overview of the different strategies employed and the new ideas adopted to improve the PEC performance of bismuth-based nanomaterials are discussed. Morphology control, the construction of heterojunctions, doping, and co-catalyst loading are several approaches that are implemented to improve the efficiency of solar water splitting. Key issues are identified and guidelines are suggested to rationalize the design of efficient bismuth-based materials for sunlight-driven water splitting. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. Graphene-Based Photocatalysts for Solar-Fuel Generation.

    PubMed

    Xiang, Quanjun; Cheng, Bei; Yu, Jiaguo

    2015-09-21

    The production of solar fuel through photocatalytic water splitting and CO2 reduction using photocatalysts has attracted considerable attention owing to the global energy shortage and growing environmental problems. During the past few years, many studies have demonstrated that graphene can markedly enhance the efficiency of photocatalysts for solar-fuel generation because of its unique 2D conjugated structure and electronic properties. Herein we summarize the recent advances in the application of graphene-based photocatalysts for solar-fuel production, including CO2 reduction to hydrocarbon fuel and water splitting to H2. A brief overview of the fundamental principles for splitting of water and reduction of CO2 is given. The different roles of graphene in these graphene-based photocatalysts for improving photocatalytic performance are discussed. Finally, the perspectives on the challenges and opportunities for future research in this promising area are also presented. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  4. Removal of 10-nm contaminant particles from Si wafers using CO2 bullet particles.

    PubMed

    Kim, Inho; Hwang, Kwangseok; Lee, Jinwon

    2012-04-11

    Removal of nanometer-sized contaminant particles (CPs) from substrates is essential in successful fabrication of nanoscale devices. The particle beam technique that uses nanometer-sized bullet particles (BPs) moving at supersonic velocity was improved by operating it at room temperature to achieve higher velocity and size uniformity of BPs and was successfully used to remove CPs as small as 10 nm. CO2 BPs were generated by gas-phase nucleation and growth in a supersonic nozzle; appropriate size and velocity of the BPs were obtained by optimizing the nozzle contours and CO2/He mixture fraction. Cleaning efficiency greater than 95% was attained. BP velocity was the most important parameter affecting removal of CPs in the 10-nm size range. Compared to cryogenic Ar or N2 particles, CO2 BPs were more uniform in size and had higher velocity and, therefore, cleaned CPs more effectively.

  5. CO2 Capture by Absorption with Potassium Carbonate

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Gary T. Rochelle; Eric Chen; Babatunde Oyenekan

    The objective of this work is to improve the process for CO{sub 2} capture by alkanolamine absorption/stripping by developing an alternative solvent, aqueous K{sub 2}CO{sub 3} promoted by piperazine. Ethylenediamine was detected in a degraded solution of MEA/PZ solution, suggesting that piperazine is subject to oxidation. Stripper modeling has demonstrated that vacuum strippers will be more energy efficient if constructed short and fat rather than tall and skinny. The matrix stripper has been identified as a configuration that will significantly reduce energy use. Extensive measurements of CO{sub 2} solubility in 7 m MEA at 40 and 60 C have confirmedmore » the work by Jou and Mather. Corrosion of carbon steel without inhibitors increases from 19 to 181 mpy in lean solutions of 6.2 m MEA/PZ as piperazine increases from 0 to 3.1 m.« less

  6. CESM-simulated 21st Century Changes in Large Scale Crop Water Requirements and Yields

    NASA Astrophysics Data System (ADS)

    Levis, S.; Badger, A.; Drewniak, B. A.; O'Neill, B. C.; Ren, X.

    2014-12-01

    We assess potential changes in crop water requirements and corresponding yields relative to the late 20th century in major crop producing regions of the world by using the Community Land Model (CLM) driven with 21st century meteorology from RCP8.5 and RCP4.5 Community Earth System Model (CESM) simulations. The RCP4.5 simulation allows us to explore the potential for averted societal impacts when compared to the RCP8.5 simulation. We consider the possibility for increased yields and improved water use efficiency under conditions of elevated atmospheric CO2 due to the CO2 fertilization effect (also known as concentration-carbon feedback). We address uncertainty in the current understanding of plant CO2 fertilization by repeating the simulations with and without the CO2 fertilization effect. Simulations without CO2 fertilization represent the radiative effect of elevated CO2 (i.e., warming) without representing the physiological effect of elevated CO2 (enhanced carbon uptake and increased water use efficiency by plants during photosynthesis). Preliminary results suggest that some plants may suffer from increasing heat and drought in much of the world without the CO2 fertilization effect. On the other hand plants (especially C3) tend to grow more with less water when models include the CO2 fertilization effect. Performing 21st century simulations with and without the CO2 fertilization effect brackets the potential range of outcomes. In this work we use the CLM crop model, which includes specific crop types that differ from the model's default plant functional types in that the crops get planted, harvested, and potentially fertilized and irrigated according to algorithms that attempt to capture human management decisions. We use an updated version of the CLM4.5 that includes cotton, rice, and sugarcane, spring wheat, spring barley, and spring rye, as well as temperate and tropical maize and soybean.

  7. Critical Role of Water and Oxygen Defects in C-O Scission during CO2 Reduction on Zn2GeO4(010).

    PubMed

    Yang, Jing; Li, Yanlu; Zhao, Xian; Fan, Weiliu

    2018-03-27

    Exploration of catalyst structure and environmental sensitivity for C-O bond scission is essential for improving the conversion efficiency because of the inertness of CO 2 . We performed density functional theory calculations to understand the influence of the properties of adsorbed water and the reciprocal action with oxygen vacancy on the CO 2 dissociation mechanism on Zn 2 GeO 4 (010). When a perfect surface was hydrated, the introduction of H 2 O was predicted to promote the scission step by two modes based on its appearance, with the greatest enhancement from dissociative adsorbed H 2 O. The dissociative H 2 O lowers the barrier and reaction energy of CO 2 dissociation through hydrogen bonding to preactivate the C-O bond and assisted scission via a COOH intermediate. The perfect surface with bidentate-binding H 2 O was energetically more favorable for CO 2 dissociation than the surface with monodentate-binding H 2 O. Direct dissociation was energetically favored by the former, whereas monodentate H 2 O facilitated the H-assisted pathway. The defective surface exhibited a higher reactivity for CO 2 decomposition than the perfect surface because the generation of oxygen vacancies could disperse the product location. When the defective surface was hydrated, the reciprocal action for vacancy and surface H 2 O on CO 2 dissociation was related to the vacancy type. The presence of H 2 O substantially decreased the reaction energy for the direct dissociation of CO 2 on O 2c1 - and O 3c2 -defect surfaces, which converts the endoergic reaction to an exoergic reaction. However, the increased decomposition barrier made the step kinetically unfavorable and reduced the reaction rate. When H 2 O was present on the O 2c2 -defect surface, both the barrier and reaction energy for direct dissociation were invariable. This result indicated that the introduction of H 2 O had little effect on the kinetics and thermodynamics. Moreover, the H-assisted pathway was suppressed on all hydrated defect surfaces. These results provide a theoretical perspective for the design of highly efficient catalysts.

  8. Estimation of the quantum efficiency of the photodissociation of HbO2 and HbCO

    NASA Astrophysics Data System (ADS)

    Gisbrecht, A. I.; Mamilov, S. A.; Esman, S. S.; Asimov, M. M.

    2016-01-01

    The paper presents our results on the study of the efficiency of inter-fractional changes in hemoglobin molecules depending on the laser radiation parameters. The evaluation of the quantum efficiency of light interaction in vivo with oxyhemoglobin (HbO2) and carboxyhemoglobin (HbCO) in the blood at wavelengths for 525 and 605 nm is presented. The photodissociation yield of 11% for HbO2 and 79% for HbCO are measured at the wavelength of 525 nm and 10 % for HbO2 and 76 % for HbCO at a wavelength of 605 nm. Thus, the quantum yield of photodissociation of the HbCO is considerably higher, which ensures high efficiency of photodecomposition of the HbCO in the blood. The obtained results can be used in the clinical phototherapy practice for effective treatment of CO poisoning.

  9. Achieving 12.8% Efficiency by Simultaneously Improving Open-Circuit Voltage and Short-Circuit Current Density in Tandem Organic Solar Cells.

    PubMed

    Qin, Yunpeng; Chen, Yu; Cui, Yong; Zhang, Shaoqing; Yao, Huifeng; Huang, Jiang; Li, Wanning; Zheng, Zhong; Hou, Jianhui

    2017-06-01

    Tandem organic solar cells (TOSCs), which integrate multiple organic photovoltaic layers with complementary absorption in series, have been proved to be a strong contender in organic photovoltaic depending on their advantages in harvesting a greater part of the solar spectrum and more efficient photon utilization than traditional single-junction organic solar cells. However, simultaneously improving open circuit voltage (V oc ) and short current density (J sc ) is a still particularly tricky issue for highly efficient TOSCs. In this work, by employing the low-bandgap nonfullerene acceptor, IEICO, into the rear cell to extend absorption, and meanwhile introducing PBDD4T-2F into the front cell for improving V oc , an impressive efficiency of 12.8% has been achieved in well-designed TOSC. This result is also one of the highest efficiencies reported in state-of-the-art organic solar cells. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  10. Mg-Doped CuFeO 2 Photocathodes for Photoelectrochemical Reduction of Carbon Dioxide

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Gu, Jing; Wuttig, Anna; Krizan, Jason W.

    2013-05-22

    Mg-doped CuFeO 2 delafossite is reported to be photoelectrochemically active for CO 2 reduction. The material was prepared via conventional solid-state methods, and subsequently assembled into an electrode as a pressed pellet. Addition of a Mg 2+ dopant is found to substantially improve the conductivity of the material, with 0.05% Mg-doped CuFeO 2 electrodes displaying photocathodic currents under visible irradiation. Photocurrent is found to onset at irradiation wavelengths of ~800 nm with the incident photon-to-current efficiency reaching a value of 14% at 340 nm using an applied electrode potential of –0.4 V vs SCE. Photoelectrodes were determined to have amore » –1.1 V vs SCE conduction band edge and were found capable of the reduction of CO 2 to formate at 400 mV of underpotential. The conversion efficiency is maximized at –0.9 V vs SCE, with H 2 production contributing as a considerable side reaction. Lastly, these results highlight the potential to produce Mg-doped p-type metal oxide photocathodes with a band structure tuned to optimize CO 2 reduction.« less

  11. Evolution of C4 plants: a new hypothesis for an interaction of CO2 and water relations mediated by plant hydraulics

    PubMed Central

    Osborne, Colin P.; Sack, Lawren

    2012-01-01

    C4 photosynthesis has evolved more than 60 times as a carbon-concentrating mechanism to augment the ancestral C3 photosynthetic pathway. The rate and the efficiency of photosynthesis are greater in the C4 than C3 type under atmospheric CO2 depletion, high light and temperature, suggesting these factors as important selective agents. This hypothesis is consistent with comparative analyses of grasses, which indicate repeated evolutionary transitions from shaded forest to open habitats. However, such environmental transitions also impact strongly on plant–water relations. We hypothesize that excessive demand for water transport associated with low CO2, high light and temperature would have selected for C4 photosynthesis not only to increase the efficiency and rate of photosynthesis, but also as a water-conserving mechanism. Our proposal is supported by evidence from the literature and physiological models. The C4 pathway allows high rates of photosynthesis at low stomatal conductance, even given low atmospheric CO2. The resultant decrease in transpiration protects the hydraulic system, allowing stomata to remain open and photosynthesis to be sustained for longer under drying atmospheric and soil conditions. The evolution of C4 photosynthesis therefore simultaneously improved plant carbon and water relations, conferring strong benefits as atmospheric CO2 declined and ecological demand for water rose. PMID:22232769

  12. Evolution of C4 plants: a new hypothesis for an interaction of CO2 and water relations mediated by plant hydraulics.

    PubMed

    Osborne, Colin P; Sack, Lawren

    2012-02-19

    C(4) photosynthesis has evolved more than 60 times as a carbon-concentrating mechanism to augment the ancestral C(3) photosynthetic pathway. The rate and the efficiency of photosynthesis are greater in the C(4) than C(3) type under atmospheric CO(2) depletion, high light and temperature, suggesting these factors as important selective agents. This hypothesis is consistent with comparative analyses of grasses, which indicate repeated evolutionary transitions from shaded forest to open habitats. However, such environmental transitions also impact strongly on plant-water relations. We hypothesize that excessive demand for water transport associated with low CO(2), high light and temperature would have selected for C(4) photosynthesis not only to increase the efficiency and rate of photosynthesis, but also as a water-conserving mechanism. Our proposal is supported by evidence from the literature and physiological models. The C(4) pathway allows high rates of photosynthesis at low stomatal conductance, even given low atmospheric CO(2). The resultant decrease in transpiration protects the hydraulic system, allowing stomata to remain open and photosynthesis to be sustained for longer under drying atmospheric and soil conditions. The evolution of C(4) photosynthesis therefore simultaneously improved plant carbon and water relations, conferring strong benefits as atmospheric CO(2) declined and ecological demand for water rose.

  13. Thermally Deposited Palladium-Tungsten Carbide and Platinum-Tungsten Carbide Counter Electrodes for a High Performance Dye-Sensitized Solar Cell Based on Organic T-/T₂ Electrolyte.

    PubMed

    Towannang, Madsakorn; Thiangkaew, Anongnad; Maiaugree, Wasan; Ratchaphonsaenwong, Kunthaya; Jarernboon, Wirat; Pimanpang, Samuk; Amornkitbamrung, Vittaya

    2018-02-01

    Tungsten carbide (WC) particles (~1 μm) were dispersed in DI water and dropped onto conductive glass. The resulting WC films were used as dye-sensitized solar cell (DSSC) counter electrodes. The performance of the WC DSSC based on the organic thiolate/disulfide (T-/T2) electrolyte was ~0.78%. The cell efficiency was greatly improved after decorating palladium (Pd) or platinum (Pt) nanoparticles on WC particles with a promising efficiency of ~2.15% for Pd-WC DSSC and ~4.62% for Pt-WC DSSC. The efficiency improvement of the composited (Pd-WC and Pt-WC) cells is attributed to co-functioning catalysts, the large electrode interfacial area and a low charge-transfer resistance at the electrolyte/counter electrode interface.

  14. Scale-up and large-scale production of Tetraselmis sp. CTP4 (Chlorophyta) for CO2 mitigation: from an agar plate to 100-m3 industrial photobioreactors.

    PubMed

    Pereira, Hugo; Páramo, Jaime; Silva, Joana; Marques, Ana; Barros, Ana; Maurício, Dinis; Santos, Tamára; Schulze, Peter; Barros, Raúl; Gouveia, Luísa; Barreira, Luísa; Varela, João

    2018-03-23

    Industrial production of novel microalgal isolates is key to improving the current portfolio of available strains that are able to grow in large-scale production systems for different biotechnological applications, including carbon mitigation. In this context, Tetraselmis sp. CTP4 was successfully scaled up from an agar plate to 35- and 100-m 3 industrial scale tubular photobioreactors (PBR). Growth was performed semi-continuously for 60 days in the autumn-winter season (17 th October - 14 th December). Optimisation of tubular PBR operations showed that improved productivities were obtained at a culture velocity of 0.65-1.35 m s -1 and a pH set-point for CO 2 injection of 8.0. Highest volumetric (0.08 ± 0.01 g L -1 d -1 ) and areal (20.3 ± 3.2 g m -2 d -1 ) biomass productivities were attained in the 100-m 3 PBR compared to those of the 35-m 3 PBR (0.05 ± 0.02 g L -1 d -1 and 13.5 ± 4.3 g m -2 d -1 , respectively). Lipid contents were similar in both PBRs (9-10% of ash free dry weight). CO 2 sequestration was followed in the 100-m 3 PBR, revealing a mean CO 2 mitigation efficiency of 65% and a biomass to carbon ratio of 1.80. Tetraselmis sp. CTP4 is thus a robust candidate for industrial-scale production with promising biomass productivities and photosynthetic efficiencies up to 3.5% of total solar irradiance.

  15. Effect of Nb and F Co-doping on Li1.2Mn0.54Ni0.13Co0.13O2 Cathode Material for High-Performance Lithium-Ion Batteries

    PubMed Central

    Ming, Lei; Zhang, Bao; Cao, Yang; Zhang, Jia-Feng; Wang, Chun-Hui; Wang, Xiao-Wei; Li, Hui

    2018-01-01

    The Li1.2Mn0.54−xNbxCo0.13Ni0.13O2−6xF6x (x = 0, 0.01, 0.03, 0.05) is prepared by traditional solid-phase method, and the Nb and F ions are successfully doped into Mn and O sites of layered materials Li1.2Mn0.54Co0.13Ni0.13O2, respectively. The incorporating Nb ion in Mn site can effectively restrain the migration of transition metal ions during long-term cycling, and keep the stability of the crystal structure. The Li1.2Mn0.54−xNbxCo0.13Ni0.13O2−6xF6x shows suppressed voltage fade and higher capacity retention of 98.1% after 200 cycles at rate of 1 C. The replacement of O2− by the strongly electronegative F− is beneficial for suppressed the structure change of Li2MnO3 from the eliminating of oxygen in initial charge process. Therefore, the initial coulombic efficiency of doped Li1.2Mn0.54−xNbxCo0.13Ni0.13O2−6xF6x gets improved, which is higher than that of pure Li1.2Mn0.54Co0.13Ni0.13O2. In addition, the Nb and F co-doping can effectively enhance the transfer of lithium-ion and electrons, and thus improving rate performance. PMID:29675405

  16. 40 CFR 86.1868-12 - CO2 credits for improving the efficiency of air conditioning systems.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... Creditvalue (g/mi) Reduced reheat, with externally-controlled, variable-displacement compressor (e.g. a compressor that controls displacement based on temperature setpoint and/or cooling demand of the air...-controlled, fixed-displacement or pneumatic variable displacement compressor (e.g. a compressor that controls...

  17. 40 CFR 86.1868-12 - CO2 credits for improving the efficiency of air conditioning systems.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ..., engine displacement, transmission class and configuration, interior volume, climate control system type... Creditvalue (g/mi) Reduced reheat, with externally-controlled, variable-displacement compressor (e.g. a compressor that controls displacement based on temperature setpoint and/or cooling demand of the air...

  18. Hydrogen depolarized carbon dioxide concentrator performance improvements and cell pair structural tests. [for manned space station

    NASA Technical Reports Server (NTRS)

    Huddleston, J. D.; Aylward, J. R.

    1973-01-01

    The investigations and testing associated with the CO2 removal efficiency and voltage degradation of a hydrogen depolarized carbon oxide concentrator are reported. Also discussed is the vibration testing of a water vapor electrolysis cell pair. Performance testing of various HDC cell pairs with Cs2CO3 electrolyte provided sufficient parametric and endurance data to size a six man space station prototype CO2 removal system as having 36 HDC cell pairs, and to verify a life capability exceeding six moths. Testing also demonstrated that tetramethylammonium carbonate is an acceptable HDC electrolyte for operating over the relative humidity range of 30 to 90 percent and over a temperature range of 50 to 80 F.

  19. Revealing the arc dynamics in a gliding arc plasmatron: a better insight to improve CO2 conversion

    NASA Astrophysics Data System (ADS)

    Ramakers, Marleen; Medrano, Jose A.; Trenchev, Georgi; Gallucci, Fausto; Bogaerts, Annemie

    2017-12-01

    A gliding arc plasmatron (GAP) is very promising for CO2 conversion into value-added chemicals, but to further improve this important application, a better understanding of the arc behavior is indispensable. Therefore, we study here for the first time the dynamic arc behavior of the GAP by means of a high-speed camera, for different reactor configurations and in a wide range of operating conditions. This allows us to provide a complete image of the behavior of the gliding arc. More specifically, the arc body shape, diameter, movement and rotation speed are analyzed and discussed. Clearly, the arc movement and shape relies on a number of factors, such as gas turbulence, outlet diameter, electrode surface, gas contraction and buoyance force. Furthermore, we also compare the experimentally measured arc movement to a state-of-the-art 3D-plasma model, which predicts the plasma movement and rotation speed with very good accuracy, to gain further insight in the underlying mechanisms. Finally, we correlate the arc dynamics with the CO2 conversion and energy efficiency, at exactly the same conditions, to explain the effect of these parameters on the CO2 conversion process. This work is important for understanding and optimizing the GAP for CO2 conversion.

  20. Modeling syngas-fired gas turbine engines with two dilutants

    NASA Astrophysics Data System (ADS)

    Hawk, Mitchell E.

    2011-12-01

    Prior gas turbine engine modeling work at the University of Wyoming studied cycle performance and turbine design with air and CO2-diluted GTE cycles fired with methane and syngas fuels. Two of the cycles examined were unconventional and innovative. The work presented herein reexamines prior results and expands the modeling by including the impacts of turbine cooling and CO2 sequestration on GTE cycle performance. The simple, conventional regeneration and two alternative regeneration cycle configurations were examined. In contrast to air dilution, CO2 -diluted cycle efficiencies increased by approximately 1.0 percentage point for the three regeneration configurations examined, while the efficiency of the CO2-diluted simple cycle decreased by approximately 5.0 percentage points. For CO2-diluted cycles with a closed-exhaust recycling path, an optimum CO2-recycle pressure was determined for each configuration that was significantly lower than atmospheric pressure. Un-cooled alternative regeneration configurations with CO2 recycling achieved efficiencies near 50%, which was approximately 3.0 percentage points higher than the conventional regeneration cycle and simple cycle configurations that utilized CO2 recycling. Accounting for cooling of the first two turbine stages resulted in a 2--3 percentage point reduction in un-cooled efficiency, with air dilution corresponding to the upper extreme. Additionally, when the work required to sequester CO2 was accounted for, cooled cycle efficiency decreased by 4--6 percentage points, and was more negatively impacted when syngas fuels were used. Finally, turbine design models showed that turbine blades are shorter with CO2 dilution, resulting in fewer design restrictions.

  1. Cocatalysts in Semiconductor-based Photocatalytic CO2 Reduction: Achievements, Challenges, and Opportunities.

    PubMed

    Ran, Jingrun; Jaroniec, Mietek; Qiao, Shi-Zhang

    2018-02-01

    Ever-increasing fossil-fuel combustion along with massive CO 2 emissions has aroused a global energy crisis and climate change. Photocatalytic CO 2 reduction represents a promising strategy for clean, cost-effective, and environmentally friendly conversion of CO 2 into hydrocarbon fuels by utilizing solar energy. This strategy combines the reductive half-reaction of CO 2 conversion with an oxidative half reaction, e.g., H 2 O oxidation, to create a carbon-neutral cycle, presenting a viable solution to global energy and environmental problems. There are three pivotal processes in photocatalytic CO 2 conversion: (i) solar-light absorption, (ii) charge separation/migration, and (iii) catalytic CO 2 reduction and H 2 O oxidation. While significant progress is made in optimizing the first two processes, much less research is conducted toward enhancing the efficiency of the third step, which requires the presence of cocatalysts. In general, cocatalysts play four important roles: (i) boosting charge separation/transfer, (ii) improving the activity and selectivity of CO 2 reduction, (iii) enhancing the stability of photocatalysts, and (iv) suppressing side or back reactions. Herein, for the first time, all the developed CO 2 -reduction cocatalysts for semiconductor-based photocatalytic CO 2 conversion are summarized, and their functions and mechanisms are discussed. Finally, perspectives in this emerging area are provided. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  2. Mechanistic Investigations of Water Oxidation by a Molecular Cobalt Oxide Analogue: Evidence for a Highly Oxidized Intermediate and Exclusive Terminal Oxo Participation.

    PubMed

    Nguyen, Andy I; Ziegler, Micah S; Oña-Burgos, Pascual; Sturzbecher-Hohne, Manuel; Kim, Wooyul; Bellone, Donatela E; Tilley, T Don

    2015-10-14

    Artificial photosynthesis (AP) promises to replace society's dependence on fossil energy resources via conversion of sunlight into sustainable, carbon-neutral fuels. However, large-scale AP implementation remains impeded by a dearth of cheap, efficient catalysts for the oxygen evolution reaction (OER). Cobalt oxide materials can catalyze the OER and are potentially scalable due to the abundance of cobalt in the Earth's crust; unfortunately, the activity of these materials is insufficient for practical AP implementation. Attempts to improve cobalt oxide's activity have been stymied by limited mechanistic understanding that stems from the inherent difficulty of characterizing structure and reactivity at surfaces of heterogeneous materials. While previous studies on cobalt oxide revealed the intermediacy of the unusual Co(IV) oxidation state, much remains unknown, including whether bridging or terminal oxo ligands form O2 and what the relevant oxidation states are. We have addressed these issues by employing a homogeneous model for cobalt oxide, the [Co(III)4] cubane (Co4O4(OAc)4py4, py = pyridine, OAc = acetate), that can be oxidized to the [Co(IV)Co(III)3] state. Upon addition of 1 equiv of sodium hydroxide, the [Co(III)4] cubane is regenerated with stoichiometric formation of O2. Oxygen isotopic labeling experiments demonstrate that the cubane core remains intact during this stoichiometric OER, implying that terminal oxo ligands are responsible for forming O2. The OER is also examined with stopped-flow UV-visible spectroscopy, and its kinetic behavior is modeled, to surprisingly reveal that O2 formation requires disproportionation of the [Co(IV)Co(III)3] state to generate an even higher oxidation state, formally [Co(V)Co(III)3] or [Co(IV)2Co(III)2]. The mechanistic understanding provided by these results should accelerate the development of OER catalysts leading to increasingly efficient AP systems.

  3. Through-Space Charge Interaction Substituent Effects in Molecular Catalysis Leading to the Design of the Most Efficient Catalyst of CO2-to-CO Electrochemical Conversion.

    PubMed

    Azcarate, Iban; Costentin, Cyrille; Robert, Marc; Savéant, Jean-Michel

    2016-12-28

    The starting point of this study of through-space substituent effects on the catalysis of the electrochemical CO 2 -to-CO conversion by iron(0) tetraphenylporphyrins is the linear free energy correlation between through-structure electronic effects and the iron(I/0) standard potential that we established separately. The introduction of four positively charged trimethylanilinium groups at the para positions of the tetraphenylporphyrin (TPP) phenyls results in an important positive deviation from the correlation and a parallel improvement of the catalytic Tafel plot. The assignment of this catalysis boosting effect to the Coulombic interaction of these positive charges with the negative charge borne by the initial Fe 0 -CO 2 adduct is confirmed by the negative deviation observed when the four positive charges are replaced by four negative charges borne by sulfonate groups also installed in the para positions of the TPP phenyls. The climax of this strategy of catalysis boosting by means of Coulombic stabilization of the initial Fe 0 -CO 2 adduct is reached when four positively charged trimethylanilinium groups are introduced at the ortho positions of the TPP phenyls. The addition of a large concentration of a weak acid-phenol-helps by cleaving one of the C-O bonds of CO 2 . The efficiency of the resulting catalyst is unprecedented, as can be judged by the catalytic Tafel plot benchmarking with all presently available catalysts of the electrochemical CO 2 -to-CO conversion. The maximal turnover frequency (TOF) is as high as 10 6 s -1 and is reached at an overpotential of only 220 mV; the extrapolated TOF at zero overpotential is larger than 300 s -1 . This catalyst leads to a highly selective formation of CO (practically 100%) in spite of the presence of a high concentration of phenol, which could have favored H 2 evolution. It is also very stable, showing no significant alteration after more than 80 h of electrolysis.

  4. Use of Industrial Waste (Al-Dross, Red Mud, Mill Scale) as Fluxing Agents in the Sulfurization of Fe-Ni-Cu-Co Alloy by Carbothermic Reduction of Calcium Sulfate

    NASA Astrophysics Data System (ADS)

    Heo, Jung Ho; Jeong, Eui Hyuk; Nam, Chul Woo; Park, Kyung Ho; Park, Joo Hyun

    2018-06-01

    The use of industrial waste [mill scale (MS), red mud (RM), Al-dross (AD)] as fluxing agents in the sulfurization of Fe-Ni-Cu-Co alloy to matte (Fe-Ni-Cu-Co-S) by carbothermic reduction of CaSO4 was investigated at 1673 K (1400 °C). The sulfurization efficiency (SE) was 76 (± 2) pct at RM or AD single fluxing. However, SE drastically increased to approximately 89 pct at a `5AD + 5MS' combination, which was equivalent to reagent-grade chemical `5Al2O3 + 5Fe2O3' fluxing (SE = 88 pct). The present results can be used to improve the cost-effective recovery of rare metals (Ni and Co) from deep sea manganese nodules.

  5. Use of Industrial Waste (Al-Dross, Red Mud, Mill Scale) as Fluxing Agents in the Sulfurization of Fe-Ni-Cu-Co Alloy by Carbothermic Reduction of Calcium Sulfate

    NASA Astrophysics Data System (ADS)

    Heo, Jung Ho; Jeong, Eui Hyuk; Nam, Chul Woo; Park, Kyung Ho; Park, Joo Hyun

    2018-03-01

    The use of industrial waste [mill scale (MS), red mud (RM), Al-dross (AD)] as fluxing agents in the sulfurization of Fe-Ni-Cu-Co alloy to matte (Fe-Ni-Cu-Co-S) by carbothermic reduction of CaSO4 was investigated at 1673 K (1400 °C). The sulfurization efficiency (SE) was 76 (± 2) pct at RM or AD single fluxing. However, SE drastically increased to approximately 89 pct at a `5AD + 5MS' combination, which was equivalent to reagent-grade chemical `5Al2O3 + 5Fe2O3' fluxing (SE = 88 pct). The present results can be used to improve the cost-effective recovery of rare metals (Ni and Co) from deep sea manganese nodules.

  6. Boosting Photocatalytic Hydrogen Production of a Metal-Organic Framework Decorated with Platinum Nanoparticles: The Platinum Location Matters.

    PubMed

    Xiao, Juan-Ding; Shang, Qichao; Xiong, Yujie; Zhang, Qun; Luo, Yi; Yu, Shu-Hong; Jiang, Hai-Long

    2016-08-01

    Improving the efficiency of electron-hole separation and charge-carrier utilization plays a central role in photocatalysis. Herein, Pt nanoparticles of ca. 3 nm are incorporated inside or supported on a representative metal-organic framework (MOF), UiO-66-NH2 , denoted as Pt@UiO-66-NH2 and Pt/UiO-66-NH2 , respectively, for photocatalytic hydrogen production via water splitting. Compared with the pristine MOF, both Pt-decorated MOF nanocomposites exhibit significantly improved yet distinctly different hydrogen-production activities, highlighting that the photocatalytic efficiency strongly correlates with the Pt location relative to the MOF. The Pt@UiO-66-NH2 greatly shortens the electron-transport distance, which favors the electron-hole separation and thereby yields much higher efficiency than Pt/UiO-66-NH2 . The involved mechanism has been further unveiled by means of ultrafast transient absorption and photoluminescence spectroscopy. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  7. The Role of Electrode-Catalyst Interactions in Enabling Efficient CO2 Reduction with Mo(bpy)(CO)4 As Revealed by Vibrational Sum-Frequency Generation Spectroscopy.

    PubMed

    Neri, Gaia; Donaldson, Paul M; Cowan, Alexander J

    2017-10-04

    Group 6 metal carbonyl complexes ([M(bpy)(CO) 4 ], M = Cr, Mo, W) are potentially promising CO 2 reduction electrocatalysts. However, catalytic activity onsets at prohibitively negative potentials and is highly dependent on the nature of the working electrode. Here we report in situ vibrational SFG (VSFG) measurements of the electrocatalyst [Mo(bpy)(CO) 4 ] at platinum and gold electrodes. The greatly improved onset potential for electrocatalytic CO 2 reduction at gold electrodes is due to the formation of the catalytically active species [Mo(bpy)(CO) 3 ] 2- via a second pathway at more positive potentials, likely avoiding the need for the generation of [Mo(bpy)(CO) 4 ] 2- . VSFG studies demonstrate that the strength of the interaction between initially generated [Mo(bpy)(CO) 4 ] •- and the electrode is critical in enabling the formation of the active catalyst via the low energy pathway. By careful control of electrode material, solvent and electrolyte salt, it should therefore be possible to attain levels of activity with group 6 complexes equivalent to their much more widely studied group 7 analogues.

  8. The effect of CO2 on the plasma remediation of NxOy

    NASA Astrophysics Data System (ADS)

    Gentile, Ann C.; Kushner, Mark J.

    1996-04-01

    Plasma remediation is being investigated for the removal of oxides of nitrogen (NxOy) from atmospheric pressure gas streams. In previous works we have investigated the plasma remediation of NxOy from N2/O2/H2O mixtures using repetitively pulsed dielectric barrier discharges. As combustion effluents contain large percentages of CO2, in this paper we discuss the consequences of CO2 in the gas mixture on the efficiency of remediation and on the end products. We find that there is a small increase in the efficiency of total NxOy remediation (molecules/eV) with increasing CO2 fraction, however the efficiency of NO remediation alone generally decreases with increasing CO2. This differential is more pronounced at low energy deposition per pulse. More remediation occurs through the reduction channel with increasing CO2 while less NO2 and HNOx are produced through the oxidation channel. CO is produced by electron impact of CO2 though negligible amounts of cyanides are generated.

  9. Two-Stage Separation of V(IV) and Al(III) by Crystallization and Solvent Extraction from Aluminum-Rich Sulfuric Acid Leaching Solution of Stone Coal

    NASA Astrophysics Data System (ADS)

    Shi, Qihua; Zhang, Yimin; Liu, Tao; Huang, Jing; Liu, Hong

    2017-10-01

    To improve separation of V(IV) and Al(III) from aluminum-rich sulfuric acid leaching solution of stone coal, the two-stage separation by crystallization and solvent extraction methods have been developed. A co-extraction coefficient ( k) was put forward to evaluate comprehensively co-extraction extent in different solutions. In the crystallization stage, 68.2% of aluminum can be removed from the solution. In the solvent extraction stage, vanadium was selectively extracted using di-2-ethylhexyl phosphoric acid/tri-n-butyl phosphate from the crystalline mother solution, followed by H2SO4 stripped efficiently. A V2O5 product with purity of 98.39% and only 0.10% Al was obtained after oxidation, precipitation, and calcination. Compared with vanadium extraction from solution without crystallization, the counter-current extraction stage of vanadium can be decreased from 6 to 3 and co-extraction coefficient ( k) decreased from 2.51 to 0.58 with two-stage separation. It is suggested that the aluminum removal by crystallization can evidently weaken the influence of aluminum co-extraction on vanadium extraction and improve the selectivity of solvent extraction for vanadium.

  10. Pilot plant test of the advanced flash stripper for CO2 capture.

    PubMed

    Lin, Yu-Jeng; Chen, Eric; Rochelle, Gary T

    2016-10-20

    Alternative stripping processes have been proposed to reduce energy use for CO 2 capture, but only a few have been applied to pilot-scale experiments. This paper presents the first pilot plant test results of one of the most promising stripper configurations, the advanced flash stripper with cold and warm rich solvent bypass. The campaign using aqueous piperazine was carried out at UT Austin in 2015. The advanced flash stripper improves the heat duty by over 25% compared to previous campaigns using the two-stage flash, achieving 2.1 GJ per tonne CO 2 of heat duty and 32 kJ mol -1 CO 2 of total equivalent work. The bypass control strategy proposed minimized the heat duty. The test successfully demonstrated the remarkable energy performance and the operability of this advanced system. An Aspen Plus® model was validated using the pilot plant data and used to explore optimum operating and design conditions. The irreversibility analysis showed that the pilot plant performance has attained 50% thermodynamic efficiency and further energy improvement should focus on the absorber and the cross exchanger by increasing absorption rate and solvent capacity.

  11. Multi-Fluid Geothermal Energy Systems: Using CO2 for Dispatchable Renewable Power Generation and Grid Stabilization

    NASA Astrophysics Data System (ADS)

    Buscheck, T. A.; Bielicki, J. M.; Randolph, J.; Chen, M.; Hao, Y.; Sun, Y.

    2013-12-01

    Abstract We present an approach to use CO2 to (1) generate dispatchable renewable power that can quickly respond to grid fluctuations and be cost-competitive with natural gas, (2) stabilize the grid by efficiently storing large quantities of energy, (3) enable seasonal storage of solar thermal energy for grid integration, (4) produce brine for power-plant cooling, all which (5) increase CO2 value, rendering CO2 capture to be commerically viable, while (6) sequestering huge quantities of CO2. These attributes reduce carbon intensity of electric power, and enable cost-competitive, dispatchable power from major sources of renewable energy: wind, solar, and geothermal. Conventional geothermal power systems circulate brine as the working fluid to extract heat, but the parasitic power load for this circulation can consume a large portion of gross power output. Recently, CO2 has been considered as a working fluid because its advantageous properties reduce this parasitic loss. We expand on this idea by using multiple working fluids: brine, CO2, and N2. N2 can be separated from air at lower cost than captured CO2, it is not corrosive, and it will not react with the formation. N2 also can improve the economics of energy production and enable energy storage, while reducing operational risk. Extracting heat from geothermal reservoirs often requires submersible pumps to lift brine, but these pumps consume much of the generated electricity. In contrast, our approach drives fluid circulation by injecting supplemental, compressible fluids (CO2, and N2) with high coefficients of thermal expansion. These fluids augment reservoir pressure, produce artesian flow at the producers, and reduce the parasitic load. Pressure augmentation is improved by the thermosiphon effect that results from injecting cold/dense CO2 and N2. These fluids are heated to reservoir temperature, greatly expand, and increase the artesian flow of brine and supplemental fluid at the producers. Rather than using pumps, the thermosiphon directly converts reservoir thermal energy into mechanical energy for fluid circulation. Because stored pressure drives fluid production, the response time is faster than that of conventional geothermal power, already considered to be dispatchable. For conventional geothermal, the parasitic power load is in phase with gross power output. In contrast, our approach can time-shift much of the parasitic power load, which is dominated by the power required to separate N2 from air and compress it for injection. Because N2 is readily available, it can be injected intermittently. Thus, most of the parasitic power load can be shifted to coincide with minimum power demand or when there is a surplus of renewable power. Such a time-shift also allows net power output to be nearly equal to gross power output during peak demand. Energy storage can be almost 100 percent efficient because it is achieved by shifting the parasitic load, which is more efficient than other methods used to store energy and stabilize the grid. This work was performed under the auspices of the U.S. DOE by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

  12. Novel Blue Organic Dye for Dye-Sensitized Solar Cells Achieving High Efficiency in Cobalt-Based Electrolytes and by Co-Sensitization.

    PubMed

    Hao, Yan; Saygili, Yasemin; Cong, Jiayan; Eriksson, Anna; Yang, Wenxing; Zhang, Jinbao; Polanski, Enrico; Nonomura, Kazuteru; Zakeeruddin, Shaik Mohammed; Grätzel, Michael; Hagfeldt, Anders; Boschloo, Gerrit

    2016-12-07

    Blue and green dyes as well as NIR-absorbing dyes have attracted great interest because of their excellent ability of absorbing the incident photons in the red and near-infrared range region. A novel blue D-π-A dye (Dyenamo Blue), based on the diketopyrrolopyrrole (DPP)-core, has been designed and synthesized. Assembled with the cobalt bipyridine-based electrolytes, the device with Dyenamo Blue achieved a satisfying efficiency of 7.3% under one sun (AM1.5 G). The co-sensitization strategy was further applied on this blue organic dye together with a red D-π-A dye (D35). The successful co-sensitization outperformed a panchromatic light absorption and improved the photocurrent density; this in addition to the open-circuit potential result in an efficiency of 8.7%. The extended absorption of the sensitization and the slower recombination reaction between the blue dye and TiO 2 surface inhibited by the additional red sensitizer could be the two main reasons for the higher performance. In conclusion, from the results, the highly efficient cobalt-based DSSCs could be achieved with the co-sensitization between red and blue D-π-A organic dyes with a proper design, which showed us the possibility of applying this strategy for future high-performance solar cells.

  13. Ternary mixed metal Fe-doped NiCo2O4 nanowires as efficient electrocatalysts for oxygen evolution reaction

    NASA Astrophysics Data System (ADS)

    Yan, Kai-Li; Shang, Xiao; Li, Zhen; Dong, Bin; Li, Xiao; Gao, Wen-Kun; Chi, Jing-Qi; Chai, Yong-Ming; Liu, Chen-Guang

    2017-09-01

    Designing mixed metal oxides with unique nanostructures as efficient electrocatalysts for water electrolysis has been an attractive approach for the storage of renewable energies. The ternary mixed metal spinel oxides FexNi1-xCo2O4 (x = 0, 0.1, 0.25, 0.5, 0.75, 0.9, 1) have been synthesized by a facile hydrothermal approach and calcination treatment using nickel foam as substrate. Fe/Ni ratios have been proved to affect the nanostructures of FexNi1-xCo2O, which imply different intrinsic activity for oxygen evolution reaction (OER). SEM images show that Fe0.5Ni0.5Co2O4 has the uniform nanowires morphology with about 30 nm of the diameter and 200-300 nm of the length. The OER measurements show that Fe0.5Ni0.5Co2O4 exhibits the better electrocatalytic performances with lower overpotential of 350 mV at J = 10 mA cm-2. In addition, the smaller Tafel slope of 27 mV dec-1 than other samples with different Fe/Ni ratios for Fe0.5Ni0.5Co2O4 is obtained. The improved OER activity of Fe0.5Ni0.5Co2O4 may be attributed to the synergistic effects from ternary mixed metals especially Fe-doping and the uniform nanowires supported on NF. Therefore, synthesizing Fe-doped multi-metal oxides with novel nanostructures may be a promising strategy for excellent OER electrocatalysts and it also provides a facile way for the fabrication of high-activity ternary mixed metal oxides electrocatalysts.

  14. Allocation of Secondary Metabolites, Photosynthetic Capacity, and Antioxidant Activity of Kacip Fatimah (Labisia pumila Benth) in Response to CO2 and Light Intensity

    PubMed Central

    Jaafar, Hawa Z. E.; Karimi, Ehsan; Ghasemzadeh, Ali

    2014-01-01

    A split plot 3 by 4 experiment was designed to investigate and distinguish the relationships among production of secondary metabolites, soluble sugar, phenylalanine ammonia lyase (PAL; EC 4.3.1.5) activity, leaf gas exchange, chlorophyll content, antioxidant activity (DPPH), and lipid peroxidation under three levels of CO2 (400, 800, and 1200 μmol/mol) and four levels of light intensity (225, 500, 625, and 900 μmol/m2/s) over 15 weeks in Labisia pumila. The production of plant secondary metabolites, sugar, chlorophyll content, antioxidant activity, and malondialdehyde content was influenced by the interactions between CO2 and irradiance. The highest accumulation of secondary metabolites, sugar, maliondialdehyde, and DPPH activity was observed under CO2 at 1200 μmol/mol + light intensity at 225 μmol/m2/s. Meanwhile, at 400 μmol/mol CO2 + 900 μmol/m2/s light intensity the production of chlorophyll and maliondialdehyde content was the highest. As CO2 levels increased from 400 to 1200 μmol/mol the photosynthesis, stomatal conductance, f v/f m (maximum efficiency of photosystem II), and PAL activity were enhanced. The production of secondary metabolites displayed a significant negative relationship with maliondialdehyde indicating lowered oxidative stress under high CO2 and low irradiance improved the production of plant secondary metabolites that simultaneously enhanced the antioxidant activity (DPPH), thus improving the medicinal value of Labisia pumila under this condition. PMID:24683336

  15. Lithium salt doped conjugated polymers as electron transporting materials for highly efficient blue polymer light-emitting diodes

    NASA Astrophysics Data System (ADS)

    Huang, Fei; Shih, Ping-I.; Liu, Michelle S.; Shu, Ching-Fong; Jen, Alex K.-Y.

    2008-12-01

    Highly efficient blue polymer light-emitting diodes (PLEDs) are fabricated using a conjugated polymer, poly[9,9-bis(2-(2-(2-diethanol-amino-ethoxy) ethoxy) ethyl) fluorene-alt-4, 4'-phenylether] as an electron transporting layer (ETL). It was found that the performance of these blue-emitting devices could be greatly improved if the ETL was doped with LiF or Li2CO3 salts. A bis[(4,6-di-fluorophenyl)-pyridinato-N, C2] (picolinate) Ir(III) (FIrpic) complex based blue phosphorescent PLED exhibited a maximum luminance efficiency of 20.3 cd/A with a luminance of 1600 cd/m2 at the current density of 7.9 mA/cm2 and drive voltage of 8.0 V.

  16. Montmorillonite-supported Pd0, Fe0, Cu0 and Ag0 nanoparticles: Properties and affinity towards CO2

    NASA Astrophysics Data System (ADS)

    Bouazizi, Nabil; Barrimo, Diana; Nousir, Saadia; Ben Slama, Romdhane; Roy, René; Azzouz, Abdelkrim

    2017-04-01

    This study reports the carbon dioxide (CO2) adsorption on montmorillonite (NaMt) incorporating Cu0, Fe0, Pd0 and Ag0 as metallic nanoparticles (MNPs). The changes in structural, textural, morphological and adsorption properties of the resulting materials (NaMt-MNPs) were investigated. Electron microscopy and X-ray diffraction showed that dispersion of fine MNPs occurs mainly within the interlayer space of NaMt, producing a slight structure expansion. This was accompanied by a visible enhancement of the affinity towards CO2, as supported by thermal programmed desorption measurements. NaMt-MNPs displayed high CO2 retention capacity (CRC) of ca. 657 μmol/g for NaMt-Cu as compared to NaMt. This was explained in terms of increased number of available adsorption sites due to enlarged interlayer spaces caused by MNP insertion. The differences in CO2 adsorption capacities clearly demonstrate the key role of MNPs in improving the surface properties and adsorption capacity. The results reported herein open new prospects for clay supported metal nanoparticles as efficient adsorbents for CO2.

  17. Bimetallic core-based cuboctahedral core-shell nanoclusters for the formation of hydrogen peroxide (2e- reduction) over water (4e- reduction): role of core metals.

    PubMed

    Mahata, Arup; Pathak, Biswarup

    2017-07-13

    The design of an efficient and selective catalyst for hydrogen peroxide (H 2 O 2 ) formation is highly sought due to its industrial importance. As alternatives to a conventional Pd-Au alloy-based catalyst, three cuboctahedral core-shell nanoclusters (Au 19 @Pt 60 , Co 19 @Pt 60 and Au 10 Co 9 @Pt 60 NCs) have been investigated. Their catalytic activities toward H 2 O 2 formation have been compared with that of pure Pt cuboctahedral NC (Pt 79 ). Much attention has been devoted to thermodynamic and kinetic parameters to find out the feasibility of the two-electron (2e - ) over the four-electron (4e - ) oxygen reduction reaction (ORR) to improve the product selectivity (H 2 O vs. H 2 O 2 ). Elementary steps corresponding to H 2 O 2 formation are significantly improved over the Au 10 Co 9 @Pt 60 NC catalyst compared with the pure core-shell NCs and periodic surface based catalysts. Furthermore, the Au 10 Co 9 @Pt 60 NC favours H 2 O 2 formation via the much desired Langmuir-Hinshelwood mechanism. The potential-dependent study shows that the H 2 O 2 formation is thermodynamically favourable up to 0.43 V on the Au 10 Co 9 @Pt 60 NC and thus the overpotential for the 2e - ORR process is significantly lowered. Besides, the Au 10 Co 9 @Pt 60 NC is highly selective for H 2 O 2 formation over H 2 O formation.

  18. Enhancing CO2 electrolysis through synergistic control of non-stoichiometry and doping to tune cathode surface structures

    PubMed Central

    Ye, Lingting; Zhang, Minyi; Huang, Ping; Guo, Guocong; Hong, Maochun; Li, Chunsen; Irvine, John T. S.; Xie, Kui

    2017-01-01

    Sustainable future energy scenarios require significant efficiency improvements in both electricity generation and storage. High-temperature solid oxide cells, and in particular carbon dioxide electrolysers, afford chemical storage of available electricity that can both stabilize and extend the utilization of renewables. Here we present a double doping strategy to facilitate CO2 reduction at perovskite titanate cathode surfaces, promoting adsorption/activation by making use of redox active dopants such as Mn linked to oxygen vacancies and dopants such as Ni that afford metal nanoparticle exsolution. Combined experimental characterization and first-principle calculations reveal that the adsorbed and activated CO2 adopts an intermediate chemical state between a carbon dioxide molecule and a carbonate ion. The dual doping strategy provides optimal performance with no degradation being observed after 100 h of high-temperature operation and 10 redox cycles, suggesting a reliable cathode material for CO2 electrolysis. PMID:28300066

  19. An investigation of the reduction of carbon dioxide in a silent electric discharge

    NASA Technical Reports Server (NTRS)

    Luce, R. S.; Greenough, B. (Editor)

    1978-01-01

    The reduction of CO2 to O2 and CO in a silent electric discharge was studied. It was found that current alone (in the ionized plasma induced by the silent electric discharge) was reponsible for the CO2 reduction process. Voltage and frequency were important only in so far as they induced current in the plasma. Pressure and temperature were of minimum influence in the process. The large power consumption in the process was recognized as resulting from the low power factor of the reactor vessel which electrically behaved like a capacitor. The power factor was subsequently improved by adding an inductive element to make the reactor vessel capacitance part of a resonant circuit. It was found that the CO2 reduction process was most efficient in terms of power vs reduction rate when a voltage was employed that was only slightly higher than that needed to induce the plasma.

  20. Efficient Hydrogen Storage and Production Using a Catalyst with an Imidazoline-Based, Proton-Responsive Ligand.

    PubMed

    Wang, Lin; Onishi, Naoya; Murata, Kazuhisa; Hirose, Takuji; Muckerman, James T; Fujita, Etsuko; Himeda, Yuichiro

    2017-03-22

    A series of new imidazoline-based iridium complexes has been developed for hydrogenation of CO 2 and dehydrogenation of formic acid. One of the proton-responsive complexes bearing two -OH groups at ortho and para positions on a coordinating pyridine ring (3 b) can catalyze efficiently the chemical fixation of CO 2 and release H 2 under mild conditions in aqueous media without using organic additives/solvents. Notably, hydrogenation of CO 2 can be efficiently carried out under CO 2 and H 2 at atmospheric pressure in basic water by 3 b, achieving a turnover frequency of 106 h -1 and a turnover number of 7280 at 25 °C, which are higher than ever reported. Moreover, highly efficient CO-free hydrogen production from formic acid in aqueous solution employing the same catalyst under mild conditions has been achieved, thus providing a promising potential H 2 -storage system in water. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  1. Sensitization of Nanocrystalline Metal Oxides with a Phosphonate-Functionalized Perylene Diimide for Photoelectrochemical Water Oxidation with a CoOx Catalyst.

    PubMed

    Kirner, Joel T; Finke, Richard G

    2017-08-23

    A planar organic thin film composed of a perylene diimide dye (N,N'-bis(phosphonomethyl)-3,4,9,10-perylenediimide, PMPDI) with photoelectrochemically deposited cobalt oxide (CoO x ) catalyst was previously shown to photoelectrochemically oxidize water (DOI: 10.1021/am405598w). Herein, the same PMPDI dye is studied for the sensitization of different nanostructured metal oxide (nano-MO x ) films in a dye-sensitized photoelectrochemical cell architecture. Dye adsorption kinetics and saturation decreases in the order TiO 2 > SnO 2 ≫ WO 3 . Despite highest initial dye loading on TiO 2 films, photocurrent with hydroquinone (H 2 Q) sacrificial reductant in pH 7 aqueous solution is much higher on SnO 2 films, likely due to a higher driving force for charge injection into the more positive conduction band energy of SnO 2 . Dyeing conditions and SnO 2 film thickness were subsequently optimized to achieve light-harvesting efficiency >99% at the λ max of the dye, and absorbed photon-to-current efficiency of 13% with H 2 Q, a 2-fold improvement over the previous thin-film architecture. A CoO x water-oxidation catalyst was photoelectrochemically deposited, allowing for photoelectrochemical water oxidation with a faradaic efficiency of 31 ± 7%, thus demonstrating the second example of a water-oxidizing, dye-sensitized photoelectrolysis cell composed entirely of earth-abundant materials. However, deposition of CoO x always results in lower photocurrent due to enhanced recombination between catalyst and photoinjected electrons in SnO 2 , as confirmed by open-circuit photovoltage measurements. Possible future studies to enhance photoanode performance are discussed, including alternative catalyst deposition strategies or structural derivatization of the perylene dye.

  2. Sensitization of Nanocrystalline Metal Oxides with a Phosphonate-Functionalized Perylene Diimide for Photoelectrochemical Water Oxidation with a CoO x Catalyst

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Kirner, Joel T.; Finke, Richard G.

    A planar organic thin film composed of a perylene diimide dye (N,N'-bis(phosphonomethyl)-3,4,9,10-perylenediimide, PMPDI) with photoelectrochemically deposited cobalt oxide (CoO x) catalyst was previously shown to photoelectrochemically oxidize water (DOI: 10.1021/am405598w). Herein, the same PMPDI dye is studied for the sensitization of different nanostructured metal oxide (nano-MO x) films in a dye-sensitized photoelectrochemical cell architecture. Dye adsorption kinetics and saturation decreases in the order TiO 2 > SnO 2 >> WO 3. Despite highest initial dye loading on TiO 2 films, photocurrent with hydroquinone (H 2Q) sacrificial reductant in pH 7 aqueous solution is much higher on SnO 2 films, likelymore » due to a higher driving force for charge injection into the more positive conduction band energy of SnO 2. Dyeing conditions and SnO 2 film thickness were subsequently optimized to achieve light-harvesting efficiency >99% at the λmax of the dye, and absorbed photon-to-current efficiency of 13% with H 2Q, a 2-fold improvement over the previous thin-film architecture. A CoO x water-oxidation catalyst was photoelectrochemically deposited, allowing for photoelectrochemical water oxidation with a faradaic efficiency of 31 ± 7%, thus demonstrating the second example of a water-oxidizing, dye-sensitized photoelectrolysis cell composed entirely of earth-abundant materials. However, deposition of CoO x always results in lower photocurrent due to enhanced recombination between catalyst and photoinjected electrons in SnO 2, as confirmed by open-circuit photovoltage measurements. Possible future studies to enhance photoanode performance are also discussed, including alternative catalyst deposition strategies or structural derivatization of the perylene dye.« less

  3. Sensitization of Nanocrystalline Metal Oxides with a Phosphonate-Functionalized Perylene Diimide for Photoelectrochemical Water Oxidation with a CoO x Catalyst

    DOE PAGES

    Kirner, Joel T.; Finke, Richard G.

    2017-07-20

    A planar organic thin film composed of a perylene diimide dye (N,N'-bis(phosphonomethyl)-3,4,9,10-perylenediimide, PMPDI) with photoelectrochemically deposited cobalt oxide (CoO x) catalyst was previously shown to photoelectrochemically oxidize water (DOI: 10.1021/am405598w). Herein, the same PMPDI dye is studied for the sensitization of different nanostructured metal oxide (nano-MO x) films in a dye-sensitized photoelectrochemical cell architecture. Dye adsorption kinetics and saturation decreases in the order TiO 2 > SnO 2 >> WO 3. Despite highest initial dye loading on TiO 2 films, photocurrent with hydroquinone (H 2Q) sacrificial reductant in pH 7 aqueous solution is much higher on SnO 2 films, likelymore » due to a higher driving force for charge injection into the more positive conduction band energy of SnO 2. Dyeing conditions and SnO 2 film thickness were subsequently optimized to achieve light-harvesting efficiency >99% at the λmax of the dye, and absorbed photon-to-current efficiency of 13% with H 2Q, a 2-fold improvement over the previous thin-film architecture. A CoO x water-oxidation catalyst was photoelectrochemically deposited, allowing for photoelectrochemical water oxidation with a faradaic efficiency of 31 ± 7%, thus demonstrating the second example of a water-oxidizing, dye-sensitized photoelectrolysis cell composed entirely of earth-abundant materials. However, deposition of CoO x always results in lower photocurrent due to enhanced recombination between catalyst and photoinjected electrons in SnO 2, as confirmed by open-circuit photovoltage measurements. Possible future studies to enhance photoanode performance are also discussed, including alternative catalyst deposition strategies or structural derivatization of the perylene dye.« less

  4. Holey graphene frameworks for highly selective post-combustion carbon capture

    PubMed Central

    Chowdhury, Shamik; Balasubramanian, Rajasekhar

    2016-01-01

    Atmospheric CO2 concentrations continue to rise rapidly in response to increased combustion of fossil fuels, contributing to global climate change. In order to mitigate the effects of global warming, development of new materials for cost-effective and energy-efficient CO2 capture is critically important. Graphene-based porous materials are an emerging class of solid adsorbents for selectively removing CO2 from flue gases. Herein, we report a simple and scalable approach to produce three-dimensional holey graphene frameworks with tunable porosity and pore geometry, and demonstrate their application as high-performance CO2 adsorbents. These holey graphene macrostructures exhibit a significantly improved specific surface area and pore volume compared to their pristine counterparts, and can be effectively used in post-combustion CO2 adsorption systems because of their intrinsic hydrophobicity together with good gravimetric storage capacities, rapid removal capabilities, superior cycling stabilities, and moderate initial isosteric heats. In addition, an exceptionally high CO2 over N2 selectivity can be achieved under conditions relevant to capture from the dry exhaust gas stream of a coal burning power plant, suggesting the possibility of recovering highly pure CO2 for long-term sequestration and/or utilization for downstream applications. PMID:26879393

  5. Holey graphene frameworks for highly selective post-combustion carbon capture.

    PubMed

    Chowdhury, Shamik; Balasubramanian, Rajasekhar

    2016-02-16

    Atmospheric CO2 concentrations continue to rise rapidly in response to increased combustion of fossil fuels, contributing to global climate change. In order to mitigate the effects of global warming, development of new materials for cost-effective and energy-efficient CO2 capture is critically important. Graphene-based porous materials are an emerging class of solid adsorbents for selectively removing CO2 from flue gases. Herein, we report a simple and scalable approach to produce three-dimensional holey graphene frameworks with tunable porosity and pore geometry, and demonstrate their application as high-performance CO2 adsorbents. These holey graphene macrostructures exhibit a significantly improved specific surface area and pore volume compared to their pristine counterparts, and can be effectively used in post-combustion CO2 adsorption systems because of their intrinsic hydrophobicity together with good gravimetric storage capacities, rapid removal capabilities, superior cycling stabilities, and moderate initial isosteric heats. In addition, an exceptionally high CO2 over N2 selectivity can be achieved under conditions relevant to capture from the dry exhaust gas stream of a coal burning power plant, suggesting the possibility of recovering highly pure CO2 for long-term sequestration and/or utilization for downstream applications.

  6. Holey graphene frameworks for highly selective post-combustion carbon capture

    NASA Astrophysics Data System (ADS)

    Chowdhury, Shamik; Balasubramanian, Rajasekhar

    2016-02-01

    Atmospheric CO2 concentrations continue to rise rapidly in response to increased combustion of fossil fuels, contributing to global climate change. In order to mitigate the effects of global warming, development of new materials for cost-effective and energy-efficient CO2 capture is critically important. Graphene-based porous materials are an emerging class of solid adsorbents for selectively removing CO2 from flue gases. Herein, we report a simple and scalable approach to produce three-dimensional holey graphene frameworks with tunable porosity and pore geometry, and demonstrate their application as high-performance CO2 adsorbents. These holey graphene macrostructures exhibit a significantly improved specific surface area and pore volume compared to their pristine counterparts, and can be effectively used in post-combustion CO2 adsorption systems because of their intrinsic hydrophobicity together with good gravimetric storage capacities, rapid removal capabilities, superior cycling stabilities, and moderate initial isosteric heats. In addition, an exceptionally high CO2 over N2 selectivity can be achieved under conditions relevant to capture from the dry exhaust gas stream of a coal burning power plant, suggesting the possibility of recovering highly pure CO2 for long-term sequestration and/or utilization for downstream applications.

  7. High-speed high-efficiency 500-W cw CO2 laser hermetization of metal frames of microelectronics devices

    NASA Astrophysics Data System (ADS)

    Levin, Andrey V.

    1996-04-01

    High-speed, efficient method of laser surface treatment has been developed using (500 W) cw CO2 laser. The principal advantages of CO2 laser surface treatment in comparison with solid state lasers are the basis of the method. It has been affirmed that high efficiency of welding was a consequence of the fundamental properties of metal-IR-radiation (10,6 mkm) interaction. CO2 laser hermetization of metal frames of microelectronic devices is described as an example of the proposed method application.

  8. Ocean Acidification Affects the Phyto-Zoo Plankton Trophic Transfer Efficiency

    PubMed Central

    Cripps, Gemma; Flynn, Kevin J.; Lindeque, Penelope K.

    2016-01-01

    The critical role played by copepods in ocean ecology and biogeochemistry warrants an understanding of how these animals may respond to ocean acidification (OA). Whilst an appreciation of the potential direct effects of OA, due to elevated pCO2, on copepods is improving, little is known about the indirect impacts acting via bottom-up (food quality) effects. We assessed, for the first time, the chronic effects of direct and/or indirect exposures to elevated pCO2 on the behaviour, vital rates, chemical and biochemical stoichiometry of the calanoid copepod Acartia tonsa. Bottom-up effects of elevated pCO2 caused species-specific biochemical changes to the phytoplanktonic feed, which adversely affected copepod population structure and decreased recruitment by 30%. The direct impact of elevated pCO2 caused gender-specific respiratory responses in A.tonsa adults, stimulating an enhanced respiration rate in males (> 2-fold), and a suppressed respiratory response in females when coupled with indirect elevated pCO2 exposures. Under the combined indirect+direct exposure, carbon trophic transfer efficiency from phytoplankton-to-zooplankton declined to < 50% of control populations, with a commensurate decrease in recruitment. For the first time an explicit role was demonstrated for biochemical stoichiometry in shaping copepod trophic dynamics. The altered biochemical composition of the CO2-exposed prey affected the biochemical stoichiometry of the copepods, which could have ramifications for production of higher tropic levels, notably fisheries. Our work indicates that the control of phytoplankton and the support of higher trophic levels involving copepods have clear potential to be adversely affected under future OA scenarios. PMID:27082737

  9. Regulation of leaf-gas exchange strategies of woody plants under elevated CO2

    NASA Astrophysics Data System (ADS)

    Belmecheri, S.; Guerrieri, R.; Voelker, S.

    2016-12-01

    Estimates of vegetation water use efficiency (WUE) have increasingly been assessed using both eddy covariance and plant stable isotope techniques but these data have often lead to differing conclusions. Eddy covariance can provide forest ecosystem-level responses of coupled carbon and water exchanges to recent global change phenomena. These direct observations, however, are generally less than one or two decades, thus documenting ecosystem-level responses at elevated [CO2] concentrations (350-400 ppm). Therefore, eddy covariance data cannot directly address plant physiological mechanisms and adaptation to climate variability and anthropogenic factors, e.g., increasing atmospheric [CO2]. By contrast, tree based carbon isotope approaches can retrospectively assess intrinsic WUE over long periods and have documented physiological responses to ambient atmospheric [CO2] (ca), which have often been contextualized within generalized strategies for stomatal regulation of leaf gas-exchange. These include maintenance of a constant leaf internal [CO2] (ci), a constant drawdown in [CO2] (ca - ci), and a constant ci/ca . Tree carbon isotope studies, however, cannot account for changes in leaf area of individual trees or canopies, which makes scaling up a difficult task. The limitations of these different approaches to understanding how forest water use efficiency has been impacted by rising [CO2] has contributed to the uncertainty in global terrestrial carbon cycling and the "missing" terrestrial carbon sink. We examined stable C isotope ratios (d13C) from woody plants over a wide range of [CO2] (200-400 ppm) to test for patterns of ci-regulation in response to rising ca. The analyses are not consistent with any of the leaf gas-exchange regulation strategies noted above. The data suggest that ca - ci is still recently increasing in most species but that the rate of increase is less than expected from paleo trees which grew at much lower [CO2]. This evidence demonstrates that a broadly conserved suite of functional traits allow woody plants to adapt their leaf gas exchange to elevated [CO2]. To improve projections of how rising [CO2] will affect terrestrial carbon uptake, dynamic global vegetation models should incorporate leaf gas exchange responses that mimic these adaptive responses to [CO2].

  10. Product lifetime, energy efficiency and climate change: A case study of air conditioners in Japan.

    PubMed

    Nishijima, Daisuke

    2016-10-01

    This study proposed a modelling technique for estimating life-cycle CO2 emissions of durable goods by considering changes in product lifetime and energy efficiency. The stock and flow of durable goods was modelled by Weibull lifetime distributions and the trend in annual energy efficiency (i.e., annual electricity consumption) of an "average" durable good was formulated as a reverse logistic curve including a technologically critical value (i.e., limit energy efficiency) with respect to time. I found that when the average product lifetime is reduced, there is a trade-off between the reduction in emissions during product use (use phase), due to the additional purchases of new, more energy-efficient air conditioners, and the increase in emissions arising from the additional production of new air conditioners stimulated by the reduction of the average product lifetime. A scenario analysis focused on residential air conditioners in Japan during 1972-2013 showed that for a reduction of average lifetime of 1 year, if the air conditioner energy efficiency limit can be improved by 1.4% from the estimated current efficiency level, then CO2 emissions can be reduced by approximately the same amount as for an extension of average product lifetime of 1 year. Copyright © 2016 Elsevier Ltd. All rights reserved.

  11. Water-use responses of ‘living fossil’ conifers to CO2 enrichment in a simulated Cretaceous polar environment

    PubMed Central

    Llorens, Laura; Osborne, Colin P.; Beerling, David J.

    2009-01-01

    Background and Aims During the Mesozoic, the polar regions supported coniferous forests that experienced warm climates, a CO2-rich atmosphere and extreme seasonal variations in daylight. How the interaction between the last two factors might have influenced water use of these conifers was investigated. An experimental approach was used to test the following hypotheses: (1) the expected beneficial effects of elevated [CO2] on water-use efficiency (WUE) are reduced or lost during the 24-h light of the high-latitude summer; and (2) elevated [CO2] reduces plant water use over the growing season. Methods Measurements of leaf and whole-plant gas exchange, and leaf-stable carbon isotope composition were made on one evergreen (Sequoia sempervirens) and two deciduous (Metasequoia glyptostroboides and Taxodium distichum) ‘living fossil’ coniferous species after 3 years' growth in controlled-environment simulated Cretaceous Arctic (69°N) conditions at either ambient (400 µmol mol−1) or elevated (800 µmol mol−1) [CO2]. Key Results Stimulation of whole-plant WUE (WUEP) by CO2 enrichment was maintained over the growing season for the three studied species but this pattern was not reflected in patterns of WUE inferred from leaf-scale gas exchange measurements (iWUEL) and δ13C of foliage (tWUEL). This response was driven largely by increased rates of carbon uptake, because there was no overall CO2 effect on daily whole-plant transpiration or whole-plant water loss integrated over the study period. Seasonal patterns of tWUEL differed from those measured for iWUEL. The results suggest caution against over simplistic interpretations of WUEP based on leaf isotopic composition. Conclusions The data suggest that the efficiency of whole-tree water use may be improved by CO2 enrichment in a simulated high-latitude environment, but that transpiration is relatively insensitive to atmospheric CO2 in the living fossil species investigated. PMID:19447810

  12. Water-use responses of 'living fossil' conifers to CO2 enrichment in a simulated Cretaceous polar environment.

    PubMed

    Llorens, Laura; Osborne, Colin P; Beerling, David J

    2009-07-01

    During the Mesozoic, the polar regions supported coniferous forests that experienced warm climates, a CO(2)-rich atmosphere and extreme seasonal variations in daylight. How the interaction between the last two factors might have influenced water use of these conifers was investigated. An experimental approach was used to test the following hypotheses: (1) the expected beneficial effects of elevated [CO(2)] on water-use efficiency (WUE) are reduced or lost during the 24-h light of the high-latitude summer; and (2) elevated [CO(2)] reduces plant water use over the growing season. Measurements of leaf and whole-plant gas exchange, and leaf-stable carbon isotope composition were made on one evergreen (Sequoia sempervirens) and two deciduous (Metasequoia glyptostroboides and Taxodium distichum) 'living fossil' coniferous species after 3 years' growth in controlled-environment simulated Cretaceous Arctic (69 degrees N) conditions at either ambient (400 micromol mol(-1)) or elevated (800 micromol mol(-1)) [CO(2)]. Stimulation of whole-plant WUE (WUE(P)) by CO(2) enrichment was maintained over the growing season for the three studied species but this pattern was not reflected in patterns of WUE inferred from leaf-scale gas exchange measurements (iWUE(L)) and delta(13)C of foliage (tWUE(L)). This response was driven largely by increased rates of carbon uptake, because there was no overall CO(2) effect on daily whole-plant transpiration or whole-plant water loss integrated over the study period. Seasonal patterns of tWUE(L) differed from those measured for iWUE(L). The results suggest caution against over simplistic interpretations of WUE(P) based on leaf isotopic composition. The data suggest that the efficiency of whole-tree water use may be improved by CO(2) enrichment in a simulated high-latitude environment, but that transpiration is relatively insensitive to atmospheric CO(2) in the living fossil species investigated.

  13. Rational Design of Bi Nanoparticles for Efficient Electrochemical CO 2 Reduction: The Elucidation of Size and Surface Condition Effects

    DOE PAGES

    Zhang, Zhiyong; Chi, Miaofang; Veith, Gabriel M.; ...

    2016-08-08

    Here we report an efficient electrochemical conversion of CO 2 to CO on surface-activated bismuth nanoparticles (NPs) in acetonitrile (MeCN) under ambient conditions, with the assistance of 1-butyl-3-methylimidazolium trifluoromethanesulfonate ([bmim][OTf]). Through the comparison between electrodeposited Bi films (Bi-ED) and different types of Bi NPs, we, for the first time, demonstrate the effects of catalyst’s size and surface condition on organic phase electrochemical CO 2 reduction. Our study reveals that the surface inhibiting layer (hydrophobic surfactants and Bi 3+ species) formed during the synthesis and purification process hinders the CO 2 reduction, leading to a 20% drop in Faradaic efficiency formore » CO evolution (FE CO). Bi particle size showed a significant effect on FE CO when the surface of Bi was air-oxidized, but this effect of size on FE CO became negligible on surface-activated Bi NPs. After the surface activation (hydrazine treatment) that effectively removed the native inhibiting layer, activated 36-nm Bi NPs exhibited an almost-quantitative conversion of CO 2 to CO (96.1% FE CO), and a mass activity for CO evolution (MA CO) of 15.6 mA mg –1, which is three-fold higher than the conventional Bi-ED, at ₋2.0 V (vs Ag/AgCl). Ultimately, this work elucidates the importance of the surface activation for an efficient electrochemical CO 2 conversion on metal NPs and paves the way for understanding the CO 2 electrochemical reduction mechanism in nonaqueous media.« less

  14. Resource use efficiency of closed plant production system with artificial light: Concept, estimation and application to plant factory

    PubMed Central

    KOZAI, Toyoki

    2013-01-01

    Extensive research has recently been conducted on plant factory with artificial light, which is one type of closed plant production system (CPPS) consisting of a thermally insulated and airtight structure, a multi-tier system with lighting devices, air conditioners and fans, a CO2 supply unit, a nutrient solution supply unit, and an environment control unit. One of the research outcomes is the concept of resource use efficiency (RUE) of CPPS. This paper reviews the characteristics of the CPPS compared with those of the greenhouse, mainly from the viewpoint of RUE, which is defined as the ratio of the amount of the resource fixed or held in plants to the amount of the resource supplied to the CPPS. It is shown that the use efficiencies of water, CO2 and light energy are considerably higher in the CPPS than those in the greenhouse. On the other hand, there is much more room for improving the light and electric energy use efficiencies of CPPS. Challenging issues for CPPS and RUE are also discussed. PMID:24334509

  15. Wind increases leaf water use efficiency.

    PubMed

    Schymanski, Stanislaus J; Or, Dani

    2016-07-01

    A widespread perception is that, with increasing wind speed, transpiration from plant leaves increases. However, evidence suggests that increasing wind speed enhances carbon dioxide (CO2 ) uptake while reducing transpiration because of more efficient convective cooling (under high solar radiation loads). We provide theoretical and experimental evidence that leaf water use efficiency (WUE, carbon uptake per water transpired) commonly increases with increasing wind speed, thus improving plants' ability to conserve water during photosynthesis. Our leaf-scale analysis suggests that the observed global decrease in near-surface wind speeds could have reduced WUE at a magnitude similar to the increase in WUE attributed to global rise in atmospheric CO2 concentrations. However, there is indication that the effect of long-term trends in wind speed on leaf gas exchange may be compensated for by the concurrent reduction in mean leaf sizes. These unintuitive feedbacks between wind, leaf size and water use efficiency call for re-evaluation of the role of wind in plant water relations and potential re-interpretation of temporal and geographic trends in leaf sizes. © 2015 The Authors. Plant, Cell & Environment published by John Wiley & Sons Ltd.

  16. Resource use efficiency of closed plant production system with artificial light: concept, estimation and application to plant factory.

    PubMed

    Kozai, Toyoki

    2013-01-01

    Extensive research has recently been conducted on plant factory with artificial light, which is one type of closed plant production system (CPPS) consisting of a thermally insulated and airtight structure, a multi-tier system with lighting devices, air conditioners and fans, a CO2 supply unit, a nutrient solution supply unit, and an environment control unit. One of the research outcomes is the concept of resource use efficiency (RUE) of CPPS.This paper reviews the characteristics of the CPPS compared with those of the greenhouse, mainly from the viewpoint of RUE, which is defined as the ratio of the amount of the resource fixed or held in plants to the amount of the resource supplied to the CPPS.It is shown that the use efficiencies of water, CO2 and light energy are considerably higher in the CPPS than those in the greenhouse. On the other hand, there is much more room for improving the light and electric energy use efficiencies of CPPS. Challenging issues for CPPS and RUE are also discussed.

  17. Corn silage versus corn silage:alfalfa hay mixtures for dairy cows: effects of dietary potassium, calcium, and cation-anion difference.

    PubMed

    Erdman, R A; Piperova, L S; Kohn, R A

    2011-10-01

    Corn silage (CS) has replaced alfalfa hay (AH) and haylage as the major forage fed to lactating dairy cows, yet many dairy producers believe that inclusion of small amounts of alfalfa hay or haylage improves feed intake and milk production. Alfalfa contains greater concentrations of K and Ca than corn silage and has an inherently higher dietary cation-anion difference (DCAD). Supplemental dietary buffers such as NaHCO(3) and K(2)CO(3) increase DCAD and summaries of studies with these buffers showed improved performance in CS-based diets but not in AH-based diets. We speculated that improvements in performance with AH addition to CS-based diets could be due to differences in mineral and DCAD concentrations between the 2 forages. The objective of this experiment was to test the effects of forage (CS vs. AH) and mineral supplementation on production responses using 45 lactating Holstein cows during the first 20 wk postpartum. Dietary treatments included (1) 50:50 mixture of AH and CS as the forage (AHCS); (2) CS as the sole forage; and (3) CS fortified with mineral supplements (CaCO(3) and K(2)CO(3)) to match the Ca and K content of the AHCS diet (CS-DCAD). Feed intake and milk production were equivalent or greater for cows fed the CS and CS-DCAD diets compared with those fed the AHCS diet. Fat percentage was greater in cows fed the CS compared with the AHCS diet. Fat-corrected milk (FCM; 3.5%) tended to be greater in cows fed the CS and CS-DCAD diets compared with the AHCS diet. Feed efficiencies measured as FCM/dry matter intake were 1.76, 1.80, and 1.94 for the AHCS, CS, and CS-DCAD diets, respectively. The combined effects of reduced feed intake and increased FCM contributed to increased feed efficiency with the CS-DCAD diet, which contained 1.41% K compared with 1.18% K in the CS diet, and we speculate that this might be the result of added dietary K and DCAD effects on digestive efficiency. These results indicate no advantage to including AH in CS-based diets, but suggest that improving mineral supplementation in CS-based diets may increase feed efficiency. Copyright © 2011 American Dairy Science Association. Published by Elsevier Inc. All rights reserved.

  18. Efficient biological conversion of carbon monoxide (CO) to carbon dioxide (CO2) and for utilization in bioplastic production by Ralstonia eutropha through the display of an enzyme complex on the cell surface.

    PubMed

    Hyeon, Jeong Eun; Kim, Seung Wook; Park, Chulhwan; Han, Sung Ok

    2015-06-25

    An enzyme complex for biological conversion of CO to CO2 was anchored on the cell surface of the CO2-utilizing Ralstonia eutropha and successfully resulted in a 3.3-fold increase in conversion efficiency. These results suggest that this complexed system may be a promising strategy for CO2 utilization as a biological tool for the production of bioplastics.

  19. CO2 emissions, real output, energy consumption, trade, urbanization and financial development: testing the EKC hypothesis for the USA.

    PubMed

    Dogan, Eyup; Turkekul, Berna

    2016-01-01

    This study aims to investigate the relationship between carbon dioxide (CO2) emissions, energy consumption, real output (GDP), the square of real output (GDP(2)), trade openness, urbanization, and financial development in the USA for the period 1960-2010. The bounds testing for cointegration indicates that the analyzed variables are cointegrated. In the long run, energy consumption and urbanization increase environmental degradation while financial development has no effect on it, and trade leads to environmental improvements. In addition, this study does not support the validity of the environmental Kuznets curve (EKC) hypothesis for the USA because real output leads to environmental improvements while GDP(2) increases the levels of gas emissions. The results from the Granger causality test show that there is bidirectional causality between CO2 and GDP, CO2 and energy consumption, CO2 and urbanization, GDP and urbanization, and GDP and trade openness while no causality is determined between CO2 and trade openness, and gas emissions and financial development. In addition, we have enough evidence to support one-way causality running from GDP to energy consumption, from financial development to output, and from urbanization to financial development. In light of the long-run estimates and the Granger causality analysis, the US government should take into account the importance of trade openness, urbanization, and financial development in controlling for the levels of GDP and pollution. Moreover, it should be noted that the development of efficient energy policies likely contributes to lower CO2 emissions without harming real output.

  20. Biodegradable Hollow Mesoporous Silica Nanoparticles for Regulating Tumor Microenvironment and Enhancing Antitumor Efficiency

    PubMed Central

    Kong, Miao; Tang, Jiamin; Qiao, Qi; Wu, Tingting; Qi, Yan; Tan, Songwei; Gao, Xueqin; Zhang, Zhiping

    2017-01-01

    There is accumulating evidence that regulating tumor microenvironment plays a vital role in improving antitumor efficiency. Herein, to remodel tumor immune microenvironment and elicit synergistic antitumor effects, lipid-coated biodegradable hollow mesoporous silica nanoparticle (dHMLB) was constructed with co-encapsulation of all-trans retinoic acid (ATRA), doxorubicin (DOX) and interleukin-2 (IL-2) for chemo-immunotherapy. The nanoparticle-mediated combinational therapy provided a benign regulation on tumor microenvironment through activation of tumor infiltrating T lymphocytes and natural killer cells, promotion of cytokines secretion of IFN-γ and IL-12, and down-regulation of immunosuppressive myeloid-derived suppressor cells, cytokine IL-10 and TGF-β. ATRA/DOX/IL-2 co-loaded dHMLB demonstrated significant tumor growth and metastasis inhibition, and also exhibited favorable biodegradability and safety. This nanoplatform has great potential in developing a feasible strategy to remodel tumor immune microenvironment and achieve enhanced antitumor effect. PMID:28900509

  1. Wireless Sensors and Networks for Advanced Energy Management

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Hardy, J.E.

    Numerous national studies and working groups have identified low-cost, very low-power wireless sensors and networks as a critical enabling technology for increasing energy efficiency, reducing waste, and optimizing processes. Research areas for developing such sensor and network platforms include microsensor arrays, ultra-low power electronics and signal conditioning, data/control transceivers, and robust wireless networks. A review of some of the research in the following areas will be discussed: (1) Low-cost, flexible multi-sensor array platforms (CO{sub 2}, NO{sub x}, CO, humidity, NH{sub 3}, O{sub 2}, occupancy, etc.) that enable energy and emission reductions in applications such as buildings and manufacturing; (2) Modelingmore » investments (energy usage and savings to drive capital investment decisions) and estimated uptime improvements through pervasive gathering of equipment and process health data and its effects on energy; (3) Robust, self-configuring wireless sensor networks for energy management; and (4) Quality-of-service for secure and reliable data transmission from widely distributed sensors. Wireless communications is poised to support technical innovations in the industrial community, with widespread use of wireless sensors forecasted to improve manufacturing production and energy efficiency and reduce emissions. Progress being made in wireless system components, as described in this paper, is helping bring these projected improvements to reality.« less

  2. CO₂-neutral wastewater treatment plants or robust, climate-friendly wastewater management? A systems perspective.

    PubMed

    Larsen, Tove A

    2015-12-15

    CO2-neutral wastewater treatment plants can be obtained by improving the recovery of internal wastewater energy resources (COD, nutrients, energy) and reducing energy demand as well as direct emissions of the greenhouse gases N2O and CH4. Climate-friendly wastewater management also includes the management of the heat resource, which is most efficiently recovered at the household level, and robust wastewater management must be able to cope with a possible resulting temperature decrease. At the treatment plant there is a substantial energy optimization potential, both from improving electromechanical devices and sludge treatment as well as through the implementation of more energy-efficient processes like the mainstream anammox process or nutrient recovery from urine. Whether CO2 neutrality can be achieved depends not only on the actual net electricity production, but also on the type of electricity replaced: the cleaner the marginal electricity the more difficult to compensate for the direct emissions, which can be substantial, depending on the stability of the biological processes. It is possible to combine heat recovery at the household scale and nutrient recovery from urine, which both have a large potential to improve the climate friendliness of wastewater management. Copyright © 2015 Elsevier Ltd. All rights reserved.

  3. Two-dimensional TiO2-based nanosheets co-modified by surface-enriched carbon dots and Gd2O3 nanoparticles for efficient visible-light-driven photocatalysis

    NASA Astrophysics Data System (ADS)

    Lu, Dingze; Fang, Pengfei; Ding, Junqian; Yang, Minchen; Cao, Yufei; Zhou, Yawei; Peng, Kui; Kondamareddy, Kiran Kumar; Liu, Min

    2017-02-01

    Two-dimensional TiO2-based nanosheets (TNSs) co-modified by surface-enriched carbon dots (CDs) and Gd2O3 nanoparticles: (Gd-C-TNSs), capable of exhibiting visible-light-driven photo catalysis were synthesized using a two-pot hydrothermal route. The samples had a sheet-like structure, thickness of approximately 3.6 nm, large specific surface area of 240-350 cm2/g. The CDs (2-3 nm) and Gd2O3 nanoparticles (1-2 nm) were highly dispersed over the surface of the nanosheets. The co-modification by Gd2O3 nanoparticles and CDs influenced the crystallinity, crystal structure, and surface area of the TNSs, and improved the visible-light absorption. Surface photocurrent and fluorescence spectral studies revealed that the photo-generated charge carrier separation efficiency could be improved by an appropriate amount of modification. A very high efficiency was obtained using 0.5 at% Gd/Ti and 3.0 g/L of CDs. The visible-light-induced photocatalytic activity is enhanced under the isolated Cr(VI) system, isolated Rhodamin B (RhB) system, and the synergism between RhB degradation and Cr(VI) reduction for the Gd-C-TNSs photocatalysts. Initially, the photocatalytic activity gradually increased with an increase in the amount of CDs, and then decreased after attaining a maximum, in the case where 0.5 at% Gd/Ti and 3.0 g/L of CDs were used. The enhancement in the photocatalytic activity was attributed to the synergetic effect of the Gd2O3 nanoparticles, TNSs, and CDs in the Gd-C-TNSs composites. The effect led to a fast separation and slow recombination of photo-induced electron-hole pairs. An alternate mechanism for enhanced visible-light photocatalytic activity was also considered.

  4. Serial lantern-shaped draft tube enhanced flashing light effect for improving CO2 fixation with microalgae in a gas-lift circumflux column photobioreactor.

    PubMed

    Ye, Qing; Cheng, Jun; Guo, Wangbiao; Xu, Junchen; Li, Ke; Zhou, Junhu

    2018-05-01

    A novel serial lantern-shaped draft tube (LDT) that generates vortices is proposed to increase radial velocity between dark and light regions for improving CO 2 fixation with microalgae in a gas-lift circumflux column (GCC) photobioreactor. Clockwise vortices are generated in the downflow outerloop of the GCC photobioreactor with LDT. Radial velocity was improved from 1.50 to 4.35 × 10 -2  m/s, thereby decreased liquid cycle period between dark and light regions by 1.9 times. Mixing time decreased by 21%, and mass transfer coefficient increased by 26% with LDT. Liquid radial velocity in the downflow outerloop and mass transfer coefficient in the GCC photobioreactor both first increased and then decreased when single-lantern height was increased. Peak CO 2 fixation rate increased from 0.62 to 0.87 g/L/d, microalgal biomass yield increased by 50%. Removal efficiencies of pollutants (chemical oxygen demand, ammonium, tilmicosin, and ethinylestradiol) in wastewater were 62-90% with microalgae growth in GCC photobioreactor with LDT. Copyright © 2018 Elsevier Ltd. All rights reserved.

  5. Feasibility Study of Regenerative Burners in Aluminum Holding Furnaces

    NASA Astrophysics Data System (ADS)

    Hassan, Mohamed I.; Al Kindi, Rashid

    2014-09-01

    Gas-fired aluminum holding reverberatory furnaces are currently considered to be the lowest efficiency fossil fuel system. A considerable volume of gas is consumed to hold the molten metal at temperature that is much lower than the flame temperature. This will lead to more effort and energy consumption to capture the excessive production of the CO2. The concern of this study is to investigate the feasibility of the regenerative-burners' furnaces to increase the furnace efficiency to reduce gas consumption per production and hence result in less CO2 production. Energy assessments for metal holding furnaces are considered at different operation conditions. Onsite measurements, supervisory control and data acquisition data, and thermodynamics analysis are performed to provide feasible information about the gas consumption and CO2 production as well as area of improvements. In this study, onsite measurements are used with thermodynamics modeling to assess a 130 MT rectangular furnace with two regenerative burners and one cold-air holding burner. The assessment showed that the regenerative burner furnaces are not profitable in saving energy, in addition to the negative impact on the furnace life. However, reducing the holding and door opening time would significantly increase the operation efficiency and hence gain the benefit of the regenerative technology.

  6. Testing of an Amine-Based Pressure-Swing System for Carbon Dioxide and Humidity Control

    NASA Technical Reports Server (NTRS)

    Lin, Amy; Smith, Frederick; Sweterlitsch, Jeffrey; Graf, John; Nalette, Tim; Papale, William; Campbell, Melissa; Lu, Sao-Dung

    2007-01-01

    In a crewed spacecraft environment, atmospheric carbon dioxide (CO2) and moisture control is crucial. Hamilton Sundstrand has developed a stable and efficient amine-based CO2 and water vapor sorbent, SA9T, that is well-suited for use in a spacecraft environment. The sorbent is efficiently packaged in pressure-swing regenerable beds that are thermally linked to improve removal efficiency and minimize vehicle thermal loads. Flows are all controlled with a single spool valve. This technology has been baselined for the new Orion spacecraft. However, more data was needed on the operational characteristics of the package in a simulated spacecraft environment. A unit was therefore tested with simulated metabolic loads in a closed chamber at Johnson Space Center during the last third of 2006. Tests were run at a variety of cabin temperatures and with a range of operating conditions varying cycle time, vacuum pressure, air flow rate, and crew activity levels. Results of this testing are presented and potential flight operational strategies discussed.

  7. CO 2 water-alternating-gas injection for enhanced oil recovery: Optimal well controls and half-cycle lengths

    DOE PAGES

    Chen, Bailian; Reynolds, Albert C.

    2018-03-11

    We report that CO 2 water-alternating-gas (WAG) injection is an enhanced oil recovery method designed to improve sweep efficiency during CO 2 injection with the injected water to control the mobility of CO 2 and to stabilize the gas front. Optimization of CO 2 -WAG injection is widely regarded as a viable technique for controlling the CO 2 and oil miscible process. Poor recovery from CO 2 -WAG injection can be caused by inappropriately designed WAG parameters. In previous study (Chen and Reynolds, 2016), we proposed an algorithm to optimize the well controls which maximize the life-cycle net-present-value (NPV). However,more » the effect of injection half-cycle lengths for each injector on oil recovery or NPV has not been well investigated. In this paper, an optimization framework based on augmented Lagrangian method and the newly developed stochastic-simplex-approximate-gradient (StoSAG) algorithm is proposed to explore the possibility of simultaneous optimization of the WAG half-cycle lengths together with the well controls. Finally, the proposed framework is demonstrated with three reservoir examples.« less

  8. The long-run effects of economic, demographic, and political indices on actual and potential CO2 emissions.

    PubMed

    Adom, Philip Kofi; Kwakwa, Paul Adjei; Amankwaa, Afua

    2018-07-15

    This study examines the long-run drivers of potential and actual CO 2 emissions in Ghana, a sub-Saharan Africa country. The use of the former helps address the reverse causality problem and capture the true long-run effects. The Stock-Watson dynamic OLS is used with data from 1970 to 2014. The result shows that potential CO 2 emissions improve model efficiency. Income (except in "other sector") and financial development (except in manufacturing and construction sector) have compelling positive and negative effects on actual and potential CO 2 emissions, respectively. A higher price (oil and electricity) reduces actual and potential CO 2 emissions, but electricity price is more vital in residential, buildings and commercial and public services sector, while oil price is crucial in the transport sector. Democracy lowers actual and potential CO 2 emissions in the aggregate (insignificant) and transport sectors but raises it in the manufacturing and construction sector. The effect is, however, inconsistent for the remaining sectors. Urbanization raises aggregate actual and potential CO 2 emissions, but the effect is inconsistent for the transport sector. The findings have important implications for policy formulation. Copyright © 2018 Elsevier Ltd. All rights reserved.

  9. CO 2 water-alternating-gas injection for enhanced oil recovery: Optimal well controls and half-cycle lengths

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Chen, Bailian; Reynolds, Albert C.

    We report that CO 2 water-alternating-gas (WAG) injection is an enhanced oil recovery method designed to improve sweep efficiency during CO 2 injection with the injected water to control the mobility of CO 2 and to stabilize the gas front. Optimization of CO 2 -WAG injection is widely regarded as a viable technique for controlling the CO 2 and oil miscible process. Poor recovery from CO 2 -WAG injection can be caused by inappropriately designed WAG parameters. In previous study (Chen and Reynolds, 2016), we proposed an algorithm to optimize the well controls which maximize the life-cycle net-present-value (NPV). However,more » the effect of injection half-cycle lengths for each injector on oil recovery or NPV has not been well investigated. In this paper, an optimization framework based on augmented Lagrangian method and the newly developed stochastic-simplex-approximate-gradient (StoSAG) algorithm is proposed to explore the possibility of simultaneous optimization of the WAG half-cycle lengths together with the well controls. Finally, the proposed framework is demonstrated with three reservoir examples.« less

  10. The dependence of the CO2 removal efficiency of LiOH on humidity and mesh size. [in spacecraft life support systems

    NASA Technical Reports Server (NTRS)

    Davis, S. H.; Kissinger, L. D.

    1978-01-01

    The effect of humidity on the CO2 removal efficiency of small beds of anhydrous LiOH has been studied. Experimental data taken in this small bed system clearly show that there is an optimum humidity for beds loaded with LiOH from a single lot. The CO2 efficiency falls rapidly under dry conditions, but this behavior is approximately the same in all samples. The behavior of the bed under wet conditions is quite dependent on material size distribution. The presence of large particles in a sample can lead to rapid fall off in the CO2 efficiency as the humidity increases.

  11. Application of sodium carbonate prevents sulphur poisoning of catalysts in automated total mercury analysis

    NASA Astrophysics Data System (ADS)

    McLagan, David S.; Huang, Haiyong; Lei, Ying D.; Wania, Frank; Mitchell, Carl P. J.

    2017-07-01

    Analysis of high sulphur-containing samples for total mercury content using automated thermal decomposition, amalgamation, and atomic absorption spectroscopy instruments (USEPA Method 7473) leads to rapid and costly SO2 poisoning of catalysts. In an effort to overcome this issue, we tested whether the addition of powdered sodium carbonate (Na2CO3) to the catalyst and/or directly on top of sample material increases throughput of sulphur-impregnated (8-15 wt%) activated carbon samples per catalyst tube. Adding 5 g of Na2CO3 to the catalyst alone only marginally increases the functional lifetime of the catalyst (31 ± 4 g of activated carbon analyzed per catalyst tube) in relation to unaltered catalyst of the AMA254 total mercury analyzer (17 ± 4 g of activated carbon). Adding ≈ 0.2 g of Na2CO3 to samples substantially increases (81 ± 17 g of activated carbon) catalyst life over the unaltered catalyst. The greatest improvement is achieved by adding Na2CO3 to both catalyst and samples (200 ± 70 g of activated carbon), which significantly increases catalyst performance over all other treatments and enables an order of magnitude greater sample throughput than the unaltered samples and catalyst. It is likely that Na2CO3 efficiently sequesters SO2, even at high furnace temperatures to produce Na2SO4 and CO2, largely negating the poisonous impact of SO2 on the catalyst material. Increased corrosion of nickel sampling boats resulting from this methodological variation is easily resolved by substituting quartz boats. Overall, this variation enables an efficient and significantly more affordable means of employing automated atomic absorption spectrometry instruments for total mercury analysis of high-sulphur matrices.

  12. Improved online δ18O measurements of nitrogen- and sulfur-bearing organic materials and a proposed analytical protocol

    USGS Publications Warehouse

    Qi, H.; Coplen, T.B.; Wassenaar, L.I.

    2011-01-01

    It is well known that N2 in the ion source of a mass spectrometer interferes with the CO background during the δ18O measurement of carbon monoxide. A similar problem arises with the high-temperature conversion (HTC) analysis of nitrogenous O-bearing samples (e.g. nitrates and keratins) to CO for δ18O measurement, where the sample introduces a significant N2 peak before the CO peak, making determination of accurate oxygen isotope ratios difficult. Although using a gas chromatography (GC) column longer than that commonly provided by manufacturers (0.6 m) can improve the efficiency of separation of CO and N2 and using a valve to divert nitrogen and prevent it from entering the ion source of a mass spectrometer improved measurement results, biased δ18O values could still be obtained. A careful evaluation of the performance of the GC separation column was carried out. With optimal GC columns, the δ18O reproducibility of human hair keratins and other keratin materials was better than ±0.15 ‰ (n = 5; for the internal analytical reproducibility), and better than ±0.10 ‰ (n = 4; for the external analytical reproducibility).

  13. Simultaneous stimulation of sedoheptulose 1,7-bisphosphatase, fructose 1,6-bisphophate aldolase and the photorespiratory glycine decarboxylase-H protein increases CO2 assimilation, vegetative biomass and seed yield in Arabidopsis.

    PubMed

    Simkin, Andrew J; Lopez-Calcagno, Patricia E; Davey, Philip A; Headland, Lauren R; Lawson, Tracy; Timm, Stefan; Bauwe, Hermann; Raines, Christine A

    2017-07-01

    In this article, we have altered the levels of three different enzymes involved in the Calvin-Benson cycle and photorespiratory pathway. We have generated transgenic Arabidopsis plants with altered combinations of sedoheptulose 1,7-bisphosphatase (SBPase), fructose 1,6-bisphophate aldolase (FBPA) and the glycine decarboxylase-H protein (GDC-H) gene identified as targets to improve photosynthesis based on previous studies. Here, we show that increasing the levels of the three corresponding proteins, either independently or in combination, significantly increases the quantum efficiency of PSII. Furthermore, photosynthetic measurements demonstrated an increase in the maximum efficiency of CO 2 fixation in lines over-expressing SBPase and FBPA. Moreover, the co-expression of GDC-H with SBPase and FBPA resulted in a cumulative positive impact on leaf area and biomass. Finally, further analysis of transgenic lines revealed a cumulative increase of seed yield in SFH lines grown in high light. These results demonstrate the potential of multigene stacking for improving the productivity of food and energy crops. © 2016 The Authors. Plant Biotechnology Journal published by Society for Experimental Biology and The Association of Applied Biologists and John Wiley & Sons Ltd.

  14. Fabrication of β-CoV3O8 nanorods embedded in graphene sheets and their application for electrochemical charge storage electrode

    NASA Astrophysics Data System (ADS)

    Jeong, Gyoung Hwa; Lee, Ilbok; Lee, Donghyun; Lee, Hea-Min; Baek, Seungmin; Kwon, O.-Pil; Kumta, Prashant N.; Yoon, Songhun; Kim, Sang-Wook

    2018-05-01

    The fabrication of β-CoV3O8 nanorods embedded in graphene sheets and their application as electrochemical charge storage electrodes is reported. From the surfactant treatment of raw graphite, graphene was directly prepared and its nanocomposite with β-CoV3O8 nanorods distributed between graphene layers (β-CoV3O8-G) was synthesized by a hydrothermal method. When applied as an anode in lithium-ion batteries, the β-CoV3O8-G anode exhibits greatly improved charge and discharge capacities of 790 and 627 mAh · g-1, respectively, with unexpectedly high initial efficiency of 82%. The observed discharge capacity reflected that at least 3.7 mol of Li+ is selectively accumulated within the β-CoV3O8 phase (LixCoV3O8, x > 3.7), indicative of significantly improved Li+ uptake when compared with aggregated β-CoV3O8 nanorods. Moreover, very distinct peak plateaus and greatly advanced cycling performance are observed, showing more improved Li+ storage within the β-CoV3O8 phase. As a supercapacitor electrode, moreover, our composite electrode exhibits very high peak pseudocapacitances of 2.71 F · cm-2 and 433.65 F · g-1 in the β-CoV3O8 phase with extremely stable cycling performance. This remarkably enhanced performance in the individual electrochemical charge storage electrodes is attributed to the novel phase formation of β-CoV3O8 and its optimized nanocomposite structure with graphene, which yield fast electrical conduction through graphene, easy accessibility of ions through the open multilayer nanosheet structure, and a relaxation space between the β-CoV3O8-G.

  15. Enhanced Adsorption Efficiency through Materials Design for Direct Air Capture over Supported Polyethylenimine.

    PubMed

    Sayari, Abdelhamid; Liu, Qing; Mishra, Prashant

    2016-10-06

    Until recently, carbon capture and sequestration (CCS) was regarded as the most promising technology to address the alarming increase in the concentration of anthropogenic CO 2 in the atmosphere. There is now an increasing interest in carbon capture and utilization (CCU). In this context, the capture of CO 2 from air is an ideal solution to supply pure CO 2 wherever it is needed. Here, we describe innovative materials for direct air capture (DAC) with unprecedented efficiency. Polyethylenimine (PEI) was supported on PME, which is an extra-large-pore silica (pore-expanded MCM-41) with its internal surfaces fully covered by a uniform layer of readily accessible C 16 chains from cetyltrimethylammonium (CTMA + ) cations. The CTMA + layer plays a key role in enhancing the amine efficiency toward dry or humid ultradilute CO 2 (400 ppm CO 2 /N 2 ) to unprecedented levels. At the same PEI content, the amine efficiency of PEI/PME was two to four times higher than that of the corresponding calcined mesoporous silica loaded with PEI or with different combinations of C 16 chains and PEI. Under humid conditions, the amine efficiency of 40 wt % PEI/PME reached 7.31 mmolCO2 /g PEI , the highest ever reported for any supported PEI in the presence of 400 ppm CO 2 . Thus, amine accessibility, which reflects both the state of PEI dispersion and the adsorption efficiency, is intimately associated with the molecular design of the adsorbent. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  16. High speed pulsed laser cutting of LiCoO2 Li-ion battery electrodes

    NASA Astrophysics Data System (ADS)

    Lutey, Adrian H. A.; Fortunato, Alessandro; Carmignato, Simone; Fiorini, Maurizio

    2017-09-01

    Laser cutting of Li-ion battery electrodes represents an alternative to mechanical blanking that avoids complications associated with tool wear and allows assembly of different cell geometries with a single device. In this study, laser cutting of LiCoO2 Li-ion battery electrodes is performed at up to 5m /s with a 1064nm wavelength nanosecond pulsed fiber laser with a maximum average power of 500W and a repetition rate of up to 2MHz . Minimum average cutting power for cathode and anode multi-layer films is established for 12 parameter groups with velocities over the range 1 - 5m /s , varying laser pulse fluence and overlap. Within the tested parameter range, minimum energy per unit cut length is found to decrease with increasing repetition rate and velocity. SEM analysis of the resulting cut edges reveals visible clearance widths in the range 20 - 50 μm , with cut quality found to improve with velocity due to a reduction in lateral heat conduction losses. Raman line map spectra reveal changes in the cathode at 60 μm from the cut edge, where bands at 486cm-1 and 595cm-1 , corresponding to the Eg and A1g modes of LiCoO2 , are replaced with a single wide band centered at 544cm-1 , and evidence of carbon black is no longer present. No changes in Raman spectra are observed in the anode. The obtained results suggest that further improvements in cutting efficiency and quality could be achieved by increasing the repetition rate above 2MHz , thereby improving ablation efficiency of the metallic conductor layers. The laser source utilized in the present study nonetheless represents an immediately available solution for repeatability and throughput that are superior to mechanical blanking.

  17. Combined Cycle Power Generation Employing Pressure Gain Combustion

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Holley, Adam

    The Phase I program assessed the potential benefit of applying pressure gain combustion (PGC) technology to a natural gas combined cycle power plant. A conceptual design of the PGC integrated gas turbine was generated which was simulated in a detailed system modeling tool. The PGC integrated system was 1.93% more efficient, produced 3.09% more power, and reduced COE by 0.58%. Since the PGC system used had the same fuel flow rate as the baseline system, it also reduced CO 2 emissions by 3.09%. The PGC system did produce more NOx than standard systems, but even with the performanceand cost penaltiesmore » associated with the cleanup system it is better in every measure. This technology benefits all of DOE’s stated program goals to improve plant efficiency, reduce CO 2 production, and reduce COE.« less

  18. U.S. DOE NETL methodology for estimating the prospective CO 2 storage resource of shales at the national and regional scale

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Levine, Jonathan S.; Fukai, Isis; Soeder, Daniel J.

    While the majority of shale formations will serve as reservoir seals for stored anthropogenic carbon dioxide (CO2), hydrocarbon-bearing shale formations may be potential geologic sinks after depletion through primary production. Here in this paper we present the United States-Department of Energy-National Energy Technology Laboratory (US-DOE-NETL) methodology for screening-level assessment of prospective CO 2 storage resources in shale using a volumetric equation. Volumetric resource estimates are produced from the bulk volume, porosity, and sorptivity of the shale and storage efficiency factors based on formation-scale properties and petrophysical limitations on fluid transport. Prospective shale formations require: (1) prior hydrocarbon production using horizontalmore » drilling and stimulation via staged, high-volume hydraulic fracturing, (2) depths sufficient to maintain CO 2 in a supercritical state, generally >800 m, and (3) an overlying seal. The US-DOE-NETL methodology accounts for storage of CO 2 in shale as a free fluid phase within fractures and matrix pores and as an sorbed phase on organic matter and clays. Uncertainties include but are not limited to poorly-constrained geologic variability in formation thickness, porosity, existing fluid content, organic richness, and mineralogy. Knowledge of how these parameters may be linked to depositional environments, facies, and diagenetic history of the shale will improve the understanding of pore-to-reservoir scale behavior, and provide improved estimates of prospective CO 2 storage.« less

  19. U.S. DOE NETL methodology for estimating the prospective CO 2 storage resource of shales at the national and regional scale

    DOE PAGES

    Levine, Jonathan S.; Fukai, Isis; Soeder, Daniel J.; ...

    2016-05-31

    While the majority of shale formations will serve as reservoir seals for stored anthropogenic carbon dioxide (CO2), hydrocarbon-bearing shale formations may be potential geologic sinks after depletion through primary production. Here in this paper we present the United States-Department of Energy-National Energy Technology Laboratory (US-DOE-NETL) methodology for screening-level assessment of prospective CO 2 storage resources in shale using a volumetric equation. Volumetric resource estimates are produced from the bulk volume, porosity, and sorptivity of the shale and storage efficiency factors based on formation-scale properties and petrophysical limitations on fluid transport. Prospective shale formations require: (1) prior hydrocarbon production using horizontalmore » drilling and stimulation via staged, high-volume hydraulic fracturing, (2) depths sufficient to maintain CO 2 in a supercritical state, generally >800 m, and (3) an overlying seal. The US-DOE-NETL methodology accounts for storage of CO 2 in shale as a free fluid phase within fractures and matrix pores and as an sorbed phase on organic matter and clays. Uncertainties include but are not limited to poorly-constrained geologic variability in formation thickness, porosity, existing fluid content, organic richness, and mineralogy. Knowledge of how these parameters may be linked to depositional environments, facies, and diagenetic history of the shale will improve the understanding of pore-to-reservoir scale behavior, and provide improved estimates of prospective CO 2 storage.« less

  20. Using Polymer Alternating Gas to Enhance Oil Recovery in Heavy Oil

    NASA Astrophysics Data System (ADS)

    Yang, Yongzhi; Li, Weirong; Zhou, Tiyao; Dong, Zhenzhen

    2018-02-01

    CO2 has been used to recover oil for more than 40 years. Currently, about 43% of EOR production in U.S. is from CO2 flooding. CO2 flooding is a well-established EOR technique, but its density and viscosity nature are challenges for CO2 projects. Low density (0.5 to 0.8 g/cm3) causes gas to rise upward in reservoirs and bypass many lower portions of the reservoir. Low viscosity (0.02 to 0.08 cp) leads to poor volumetric sweep efficiency. So water-alternating-gas (WAG) method was used to control the mobility of CO2 and improve sweep efficiency. However, WAG process has some other problems in heavy oil reservoir, such as poor mobility ratio and gravity overriding. To examine the applicability of carbon dioxide to recover viscous oil from highly heterogeneous reservoirs, this study suggests a new EOR method--polymer-alternating gas (PAG) process. The process involves a combination of polymer flooding and CO2 injection. To confirm the effectiveness of PAG process in heavy oils, a reservoir model from Liaohe Oilfield is used to compare the technical and economic performance among PAG, WAG and polymer flooding. Simulation results show that PAG method would increase oil recovery over 10% compared with other EOR methods and PAG would be economically success based on assumption in this study. This study is the first to apply PAG to enhance oil recovery in heavy oil reservoir with highly heterogeneous. Besides, this paper provides detailed discussions and comparison about PAG with other EOR methods in this heavy oil reservoir.

  1. Efficient Reservoir Simulation with Cubic Plus Association and Cross-Association Equation of State for Multicomponent Three-Phase Compressible Flow with Applications in CO2 Storage and Methane Leakage

    NASA Astrophysics Data System (ADS)

    Moortgat, J.

    2017-12-01

    We present novel simulation tools to model multiphase multicomponent flow and transport in porous media for mixtures that contain non-polar hydrocarbons, self-associating polar water, and cross-associating molecules like methane, ethane, unsaturated hydrocarbons, CO2 and H2S. Such mixtures often occur when CO2 is injected and stored in saline aquifers, or when methane is leaking into groundwater. To accurately predict the species transfer between aqueous, gaseous and oleic phases, and the subsequent change in phase properties, the self- and cross-associating behavior of molecules needs to be taken into account, particularly at the typical temperatures and pressures in deep formations. The Cubic-Plus-Association equation-of-state (EOS) has been demonstrated to be highly accurate for such problems but its excessive computational cost has prevented widespread use in reservoir simulators. We discuss the thermodynamical framework and develop sophisticated numerical algorithms that allow reservoir simulations with efficiencies comparable to a simple cubic EOS. This approach improves our predictive powers for highly nonlinear fluid behavior related to geological carbon sequestration, such as density driven flow and natural convection (solubility trapping), evaporation of water into the CO2-rich gas phase, and competitive dissolution-evaporation when CO2 is injected in, e.g., methane saturated aquifers. Several examples demonstrate the accuracy and robustness of this EOS framework for complex applications.

  2. Increasing water use efficiency along the C3 to C4 evolutionary pathway: a stomatal optimization perspective.

    PubMed

    Way, Danielle A; Katul, Gabriel G; Manzoni, Stefano; Vico, Giulia

    2014-07-01

    C4 photosynthesis evolved independently numerous times, probably in response to declining atmospheric CO2 concentrations, but also to high temperatures and aridity, which enhance water losses through transpiration. Here, the environmental factors controlling stomatal behaviour of leaf-level carbon and water exchange were examined across the evolutionary continuum from C3 to C4 photosynthesis at current (400 μmol mol(-1)) and low (280 μmol mol(-1)) atmospheric CO2 conditions. To this aim, a stomatal optimization model was further developed to describe the evolutionary continuum from C3 to C4 species within a unified framework. Data on C3, three categories of C3-C4 intermediates, and C4 Flaveria species were used to parameterize the stomatal model, including parameters for the marginal water use efficiency and the efficiency of the CO2-concentrating mechanism (or C4 pump); these two parameters are interpreted as traits reflecting the stomatal and photosynthetic adjustments during the C3 to C4 transformation. Neither the marginal water use efficiency nor the C4 pump strength changed significantly from C3 to early C3-C4 intermediate stages, but both traits significantly increased between early C3-C4 intermediates and the C4-like intermediates with an operational C4 cycle. At low CO2, net photosynthetic rates showed continuous increases from a C3 state, across the intermediates and towards C4 photosynthesis, but only C4-like intermediates and C4 species (with an operational C4 cycle) had higher water use efficiencies than C3 Flaveria. The results demonstrate that both the marginal water use efficiency and the C4 pump strength increase in C4 Flaveria to improve their photosynthesis and water use efficiency compared with C3 species. These findings emphasize that the advantage of the early intermediate stages is predominantly carbon based, not water related. © The Author 2014. Published by Oxford University Press on behalf of the Society for Experimental Biology.

  3. A Direct Detection 1.6μm DIAL with Three Wavelengths for Measurements of Vertical CO2 Concentration and Temperature Profiles in the Atmosphere

    NASA Astrophysics Data System (ADS)

    Nagasawa, C.; Abo, M.; Shibata, Y.; Nagai, T.; Tsukamoto, M.

    2012-12-01

    We report the new 1.6 μm DIAL system that can measure the temperature profiles with the CO2 concentration profiles in the atmosphere because of improvement of measurement accuracy of the CO2 density and mixing ratio (ppm). We have developed a direct detection 1.6 μm differential absorption lidar (DIAL) technique to perform range-resolved measurements of vertical CO2 concentration profiles in the atmosphere [Sakaizawa et al. 2009]. Our 1.6 μm DIAL system consists of the Optical Parametric Generator (OPG) transmitter that excited by the LD pumped Nd:YAG laser with high repetition rate (500 Hz) and the receiving optics that included the near-infrared photomultiplier tube with high quantum efficiency operating at the photon counting mode and the telescope with larger aperture than that of the coherent detection method. Laser beams of three wavelengths around a CO2 absorption line is transmitted alternately to the atmosphere for measurements of CO2 concentration and temperature profiles. Moreover, a few retrieval algorithms of CO2-DIAL are also performed for improvement of measurement accuracy. The accurate vertical CO2 profiles in the troposphere are highly desirable in the inverse techniques to improve quantification and understanding of the global budget of CO2 and also global climate changes [Stephens et al. 2007]. In comparison with the ground-based monitoring network, CO2 measurements for vertical profiles in the troposphere have been limited to campaign-style aircraft and commercial airline observations with the limited spatial and temporal coverage. This work was financially supported by the System Development Program for Advanced Measurement and Analysis of the Japan Science and Technology Agency. References Sakaizawa, D., C. Nagasawa, T. Nagai, M. Abo, Y. Shibata, H. Nagai, M. Nakazato, and T. Sakai, Development of a 1.6μm differential absorption lidar with a quasi-phase-matching optical parametric oscillator and photon-counting detector for the vertical CO2 profile, Applied Optics, Vol.48, No.4, pp.748-757, 2009. Stephens, B. B. et al., Weak Northern and Strong Tropical Land Carbon Uptake from Vertical Profiles of Atmospheric CO2, Science 316, pp.1732-1735, 2007.

  4. The increase of current atmospheric CO2 and temperature can benefit leaf gas exchanges, carbohydrate content and growth in C4 grass invaders of the Cerrado biome.

    PubMed

    Faria, A P de; Marabesi, M A; Gaspar, M; França, M G C

    2018-06-01

    Leaf gas exchanges, carbohydrate metabolism and growth of three Brazilian Cerrado invasive African grasses were evaluated after growing for 75 days under doubled CO 2 concentration and temperature elevated by 3 °C. Results showed that although the species presented photosynthetic C4 metabolism, they all had some kind of positive response to increased CO 2 . Urochloa brizantha and Megathyrsus maximus showed increased height for all induced environmental conditions. Urochloa decumbens showed only improvement in water use efficiency (WUE), while U. brizantha showed increased CO 2 assimilation and M. maximus presented higher biomass accumulation under doubled CO 2 concentration. The most significant improvement of increased CO 2 in all three species appears to be the increase in WUE. This improvement probably explains the positive increase of photosynthesis and biomass accumulation presented by U. brizantha and M. maximus, respectively. The increase in temperature affected leaf carbohydrate content of M. maximus by reducing sucrose, glucose and fructose content. These reductions were not related to thermal stress since photosynthesis and growth were not harmed. Cellulose content was not affected in any of the three species, just the lignin content in U. decumbens and M. maximus. All treatments promoted lignin content reduction in U. brizantha, suggesting a delay in leaf maturation of this species. Together, the results indicate that climate change may differentially promote changes in leaf gas exchanges, carbohydrate content and growth in C4 plant species studied and all of them could benefit in some way from these changes, constituting a threat to the native Cerrado biodiversity. Copyright © 2018 Elsevier Masson SAS. All rights reserved.

  5. Substrate-dependent structural and CO sensing properties of LaCoO3 epitaxial films

    NASA Astrophysics Data System (ADS)

    Liu, Haifeng; Sun, Hongjuan; Xie, Ruishi; Zhang, Xingquan; Zheng, Kui; Peng, Tongjiang; Wu, Xiaoyu; Zhang, Yanping

    2018-06-01

    LaCoO3 thin films were grown on different (0 0 1) oriented LaAlO3, SrTiO3 and (LaAlO3)0.3(Sr2AlTaO6)0.7 by the polymer assisted deposition method, respectively. All the LaCoO3 thin films are in epitaxial growth on these substrates, with tetragonal distortion of CoO6 octahedrons. Due to different in-plane lattice mismatch, the LaCoO3 film on LaAlO3 has the largest tetragonal distortion of CoO6 octahedrons while the film grown on (LaAlO3)0.3(Sr2AlTaO6)0.7 has the smallest tetragonal distortion. The relative contents of the surface absorbed oxygen species are found to increase for the LaCoO3 epitaxial films grown on (0 0 1) oriented (LaAlO3)0.3(Sr2AlTaO6)0.7, SrTiO3 and LaAlO3 substrates, sequentially. The film sensors exhibit good CO sensing properties at 150 °C, and the LaCoO3 film on LaAlO3 shows the highest response but the film on (LaAlO3)0.3(Sr2AlTaO6)0.7 shows the lowest. It reveals that the larger degree of Jahn-Teller-like tetragonal distortion of CoO6 octahedrons may greatly improve the surface absorbing and catalytic abilities, corresponding to more excellent CO sensing performance. The present study suggests that the formation of epitaxial films is an efficient methodology for controlling the octahedral distortion and thereby improving the gas sensing performance of perovskite transition metal oxides.

  6. Investigations on the Synthesis and Properties of Fe2O3/Bi2O2CO3 in the Photocatalytic and Fenton-like Process

    NASA Astrophysics Data System (ADS)

    Sun, Dongxue; Shen, Tingting; Sun, Jing; Wang, Chen; Wang, Xikui

    2018-01-01

    Catalyst of Bi2O2CO3 and Fe2O3 modified Bi2O2CO3 (Fe2O3/Bi2O2CO3) were prepared by hydrothermal method and characterized by X-ray diffractions (XRD), scanning electron microscopy (SEM), transmission electron microscope (TEM) and UV-vis DRS. The catalytic activity of Bi2O2CO3 and Fe2O3/Bi2O2CO3 were comparatively investigated in the photodegradation and Fento-like process. Rhodamine B(RhB) was selected as the target pollutant under the irradiation of 300 W xenon lamp. The results indicated that Fe2O3 plays a great role in the enhancing the treatment efficiency and the and the maximum reaction rate was achieved at the Fe2O3 loading of 1.5%. The Fenton-like degradation rate constant of RhB with bare Bi2O2CO3 in dark is 0.4 min-1, while that with 1.5 Fe2O3/Bi2O2CO3 increases to 28.4 min-1 under visible light irradiation, a 71-fold improvement. It is expected to shed a new light for the constructing novel composite photocatalyst and also provide a potential method for the removal of dyes in the aqueous system.

  7. Toward a stable solid-electrolyte-interfaces on nickel-rich cathodes: LiPO2F2 salt-type additive and its working mechanism for LiNi0.5Mn0.25Co0.25O2 cathodes

    NASA Astrophysics Data System (ADS)

    Zhao, Weimin; Zheng, Guorui; Lin, Min; Zhao, Wengao; Li, Dongjiang; Guan, Xiaoyun; Ji, Yajuan; Ortiz, Gregorio F.; Yang, Yong

    2018-03-01

    Although the LiNi0.5Mn0.25Co0.25O2 holds the merits of high theoretical capacities and a relatively high operating voltage, the battery performance suffers from the severe cycling decay due to the unstable solid electrolyte interface on the cathode. Herein, we present LiPO2F2 as a salt-type electrolyte additive to enhance the cycling stability of large-size crystallite LiNi0.5Mn0.25Co0.25O2 cathodes. Results demonstrate that 1 wt% LiPO2F2 can significantly improve not only the initial coulombic efficiency by 3%, but also the cycling stability and rate capability at 25 °C. Furthermore, the discharge capacity of LiNi0.5Mn0.25Co0.25O2 cathodes still maintain 156 mAh g-1 after 100 cycles even when the temperature increases to 55 °C. In-depth experimental characterization and theoretical calculation indicate that a new stable and thin (e.g. 15-20 nm) film formed on the surface of the cathodes, with composition of LiPO2F2, LiF, etc., which significantly reduces charge transfer impedance of the electrodes, and therefore significantly improves the cycling and rate performance of LiNi0.5Mn0.25Co0.25O2.

  8. Artificially evolved Synechococcus PCC6301 Rubisco variants exhibit improvements in folding and catalytic efficiency.

    PubMed

    Greene, Dina N; Whitney, Spencer M; Matsumura, Ichiro

    2007-06-15

    The photosynthetic CO2-fixing enzyme, Rubisco (ribulose-1,5-bisphosphate carboxylase/oxygenase), is responsible for most of the world's biomass, but is a slow non-specific catalyst. We seek to identify and overcome the chemical and biological constraints that limit the evolutionary potential of Rubisco in Nature. Recently, the horizontal transfer of Calvin cycle genes (rbcL, rbcS and prkA) from cyanobacteria (Synechococcus PCC6301) to gamma-proteobacteria (Escherichia coli) was emulated in the laboratory. Three unique Rubisco variants containing single (M259T) and double (M259T/A8S, M259T/F342S) amino acid substitutions in the L (large) subunit were identified after three rounds of random mutagenesis and selection in E. coli. Here we show that the M259T mutation did not increase steady-state levels of rbcL mRNA or L protein. It instead improved the yield of properly folded L subunit in E. coli 4-9-fold by decreasing its natural propensity to misfold in vivo and/or by enhancing its interaction with the GroES-GroEL chaperonins. The addition of osmolites to the growth media enhanced productive folding of the M259T L subunit relative to the wild-type L subunit, while overexpression of the trigger factor and DnaK/DnaJ/GrpE chaperones impeded Rubisco assembly. The evolved enzymes showed improvement in their kinetic properties with the M259T variant showing a 12% increase in carboxylation turnover rate (k(c)cat), a 15% improvement in its K(M) for CO2 and no change in its K(M) for ribulose-1,5-bisphosphate or its CO2/O2 selectivity. The results of the present study show that the directed evolution of the Synechococcus Rubisco in E. coli can elicit improvements in folding and catalytic efficiency.

  9. Down-conversion emission of Ce3+-Tb3+ co-doped CaF2 hollow spheres and application for solar cells

    NASA Astrophysics Data System (ADS)

    Cheng, Yufei; Wang, Yongbo; Teng, Feng; Dong, Hua; Chen, Lida; Mu, Jianglong; Sun, Qian; Fan, Jun; Hu, Xiaoyun; Miao, Hui

    2018-03-01

    Luminescent downconversion is a promising way to harvest ultraviolet sunlight and transform it into visible light that can be absorbed by solar cells, and has potential to improve their photoelectric conversion efficiency. In this work, the uniform hollow spheres and well dispersed CaF2 phosphors doped with rare-earth Ce3+ and Tb3+ ions are prepared by a one-step hydrothermal synthesis method. Benefiting from the stronger ability of absorption and emission and excellent transparency property, we demonstrate that the application of the doped nanocrystals can efficiently improve visible light transmittance. The chosen phosphors are added in the SiO2 sols so as to get the anti-reflection coatings with wavelength conversion bi-functional films, promoting the optical transmittance in the visible and near-infrared range which matches with the range of the band gap energy of silicon semiconductor. Optimized photoelectric conversion efficiency of 14.35% and the external quantum efficiency over 70% from 450 to 950 nm are obtained through the silicon solar cells with 0.10 g phosphors coating. Compared with the pure glass devices, the photoelectric conversion efficiency is enhanced by 0.69%. This work indicates that fluorescent downconversion not only can serve as proof of principles for improving photoelectric conversion efficiency of solar cells but also may be helpful to practical application in the future.

  10. Improving Photosynthesis

    PubMed Central

    Evans, John R.

    2013-01-01

    Photosynthesis is the basis of plant growth, and improving photosynthesis can contribute toward greater food security in the coming decades as world population increases. Multiple targets have been identified that could be manipulated to increase crop photosynthesis. The most important target is Rubisco because it catalyses both carboxylation and oxygenation reactions and the majority of responses of photosynthesis to light, CO2, and temperature are reflected in its kinetic properties. Oxygenase activity can be reduced either by concentrating CO2 around Rubisco or by modifying the kinetic properties of Rubisco. The C4 photosynthetic pathway is a CO2-concentrating mechanism that generally enables C4 plants to achieve greater efficiency in their use of light, nitrogen, and water than C3 plants. To capitalize on these advantages, attempts have been made to engineer the C4 pathway into C3 rice (Oryza sativa). A simpler approach is to transfer bicarbonate transporters from cyanobacteria into chloroplasts and prevent CO2 leakage. Recent technological breakthroughs now allow higher plant Rubisco to be engineered and assembled successfully in planta. Novel amino acid sequences can be introduced that have been impossible to reach via normal evolution, potentially enlarging the range of kinetic properties and breaking free from the constraints associated with covariation that have been observed between certain kinetic parameters. Capturing the promise of improved photosynthesis in greater yield potential will require continued efforts to improve carbon allocation within the plant as well as to maintain grain quality and resistance to disease and lodging. PMID:23812345

  11. 2-.mu.m fiber amplified spontaneous emission (ASE) source

    NASA Technical Reports Server (NTRS)

    Jiang, Shibin (Inventor); Wu, Jianfeng (Inventor); Geng, Jihong (Inventor)

    2007-01-01

    A 2-.mu.m fiber Amplified Spontaneous Emission (ASE) source provides a wide emission bandwidth and improved spectral stability/purity for a given output power. The fiber ASE source is formed from a heavy metal oxide multicomponent glass selected from germanate, tellurite and bismuth oxides and doped with high concentrations, 0.5-15 wt. %, thulium oxides (Tm.sub.2O.sub.3) or 0.1-5 wt% holmium oxides (Ho.sub.2O.sub.3) or mixtures thereof. The high concentration of thulium dopants provide highly efficient pump absorption and high quantum efficiency. Co-doping of Tm and Ho can broaden the ASE spectrum.

  12. Research on oxygen recovery systems for use in space capsules

    NASA Technical Reports Server (NTRS)

    Selman, J. R.; Steunenberg, R. K.; Cairns, E. J.

    1973-01-01

    An improved electrochemical process was investigated for the recovery of oxygen from the atmospheres of manned space capsules. The objective of the proposed system is to recover the oxygen from CO2 with high efficiency and to recover the additional amount of oxygen from water that is required to provide a total oxygen makeup stream of about 2.0 lb/man-day. The carbon from the CO2 must be converted into a readily disposable or usable form. The results are given of initial experiments with a porous stainless steel cathode in a LiCl-KCl electrolyte with small additions of oxide, carbonate, and hydroxide.

  13. Combining observations in the reflective solar and thermal domains for improved carbon and energy flux estimation

    USDA-ARS?s Scientific Manuscript database

    This study investigates the utility of integrating remotely sensed estimates of leaf chlorophyll (Cab) into a therma-based Two-Source Energy Balance (TSEB) model that estimates land-surface CO2 and energy fluxes using an analytical, light-use-efficiency (LUE) based model of canopy resistance. The LU...

  14. Decreased CO2 availability and inactivation of Rubisco limit photosynthesis in cotton plants under heat and drought stress in the field

    USDA-ARS?s Scientific Manuscript database

    Heat and drought stresses are often coincident and constitute major factors limiting global crop yields. Selection of cultivars with superior tolerance to these stresses under production environments will facilitate efforts to improve yield and water use efficiencies in a climatically changing world...

  15. Charged Covalent Triazine Frameworks for CO2 Capture and Conversion.

    PubMed

    Buyukcakir, Onur; Je, Sang Hyun; Talapaneni, Siddulu Naidu; Kim, Daeok; Coskun, Ali

    2017-03-01

    The quest for the development of new porous materials addressing both CO 2 capture from various sources and its conversion into useful products is a very active research area and also critical in order to develop a more sustainable and environmentally-friendly society. Here, we present the first charged covalent triazine framework (cCTF) prepared by simply heating nitrile functionalized dicationic viologen derivatives under ionothermal reaction conditions using ZnCl 2 as both solvent and trimerization catalyst. It has been demonstrated that the surface area, pore volume/size of cCTFs can be simply controlled by varying the synthesis temperature and the ZnCl 2 content. Specifically, increasing the reaction temperature led to controlled increase in the mesopore content and facilitated the formation of hierarchical porosity, which is critical to ensure efficient mass transport within porous materials. The resulting cCTFs showed high specific surface areas up to 1247 m 2 g -1 , and high physicochemical stability. The incorporation of ionic functional moieties to porous organic polymers improved substantially their CO 2 affinity (up to 133 mg g -1 , at 1 bar and 273 K) and transformed them into hierarchically porous organocatalysts for CO 2 conversion. More importantly, the ionic nature of cCTFs, homogeneous charge distribution together with hierarchical porosity offered a perfect platform for the catalytic conversion of CO 2 into cyclic carbonates in the presence of epoxides through an atom economy reaction in high yields and exclusive product selectivity. These results clearly demonstrate the promising aspect of incorporation of charged units into the porous organic polymers for the development of highly efficient porous organocatalysts for CO 2 capture and fixation.

  16. Exclusive Ni-N4 Sites Realize Near-Unity CO Selectivity for Electrochemical CO2 Reduction.

    PubMed

    Li, Xiaogang; Bi, Wentuan; Chen, Minglong; Sun, Yuexiang; Ju, Huanxin; Yan, Wensheng; Zhu, Junfa; Wu, Xiaojun; Chu, Wangsheng; Wu, Changzheng; Xie, Yi

    2017-10-25

    Electrochemical reduction of carbon dioxide (CO 2 ) to value-added carbon products is a promising approach to reduce CO 2 levels and mitigate the energy crisis. However, poor product selectivity is still a major obstacle to the development of CO 2 reduction. Here we demonstrate exclusive Ni-N 4 sites through a topo-chemical transformation strategy, bringing unprecedentedly high activity and selectivity for CO 2 reduction. Topo-chemical transformation by carbon layer coating successfully ensures preservation of the Ni-N 4 structure to a maximum extent and avoids the agglomeration of Ni atoms to particles, providing abundant active sites for the catalytic reaction. The Ni-N 4 structure exhibits excellent activity for electrochemical reduction of CO 2 with particularly high selectivity, achieving high faradaic efficiency over 90% for CO in the potential range from -0.5 to -0.9 V and gives a maximum faradaic efficiency of 99% at -0.81 V with a current density of 28.6 mA cm -2 . We anticipate exclusive catalytic sites will shed new light on the design of high-efficiency electrocatalysts for CO 2 reduction.

  17. Carbon-armored Co9S8 nanoparticles as all-pH efficient and durable H2-evolving electrocatalysts.

    PubMed

    Feng, Liang-Liang; Li, Guo-Dong; Liu, Yipu; Wu, Yuanyuan; Chen, Hui; Wang, Yun; Zou, Yong-Cun; Wang, Dejun; Zou, Xiaoxin

    2015-01-14

    Splitting water to produce hydrogen requires the development of non-noble-metal catalysts that are able to make this reaction feasible and energy efficient. Herein, we show that cobalt pentlandite (Co9S8) nanoparticles can serve as an electrochemically active, noble-metal-free material toward hydrogen evolution reaction, and they work stably in neutral solution (pH 7) but not in acidic (pH 0) and basic (pH 14) media. We, therefore, further present a carbon-armoring strategy to increase the durability and activity of Co9S8 over a wider pH range. In particular, carbon-armored Co9S8 nanoparticles (Co9S8@C) are prepared by direct thermal treatment of a mixture of cobalt nitrate and trithiocyanuric acid at 700 °C in N2 atmosphere. Trithiocyanuric acid functions as both sulfur and carbon sources in the reaction system. The resulting Co9S8@C material operates well with high activity over a broad pH range, from pH 0 to 14, and gives nearly 100% Faradaic yield during hydrogen evolution reaction under acidic (pH 0), neutral (pH 7), and basic (pH 14) media. To the best of our knowledge, this is the first time that a transition-metal chalcogenide material is shown to have all-pH efficient and durable electrocatalytic activity. Identifying Co9S8 as the catalytically active phase and developing carbon-armoring as the improvement strategy are anticipated to give a fresh impetus to rational design of high-performance noble-metal-free water splitting catalysts.

  18. Excellent photocatalytic hydrogen production over CdS nanorods via using noble metal-free copper molybdenum sulfide (Cu2MoS4) nanosheets as co-catalysts

    NASA Astrophysics Data System (ADS)

    Hong, Sangyeob; Kumar, D. Praveen; Reddy, D. Amaranatha; Choi, Jiha; Kim, Tae Kyu

    2017-02-01

    Charge carrier recombination and durability issues are major problems in photocatalytic hydrogen (H2) evolution processes. Thus, there is a very important necessitate to extend an efficient photocatalyst to control charge-carrier dynamics in the photocatalytic system. We have developed copper molybdenum sulfide (Cu2MoS4) nanosheets as co-catalysts with CdS nanorods for controlling charge carriers without recombination for use in photocatalytic H2 evolution under simulated solar light irradiation. Effective control and utilization of charge carriers are possible by loading Cu2MoS4 nanosheets onto the CdS nanorods. The loading compensates for the restrictions of CdS, and stimulated synergistic effects, such as efficient photoexcited charge separation, lead to an improvement in photostability because of the layered structure of the Cu2MoS4nanosheets. These layered Cu2MoS4 nanosheets have emerged as novel and active replacements for precious noble metal co-catalysts in photocatalytic H2 production by water splitting. We have obtained superior H2 production rates by using Cu2MoS4 loaded CdS nanorods. The physicochemical properties of the composites are analyzed by diverse characterization techniques.

  19. MoS2 quantum dots@TiO2 nanotube composites with enhanced photoexcited charge separation and high-efficiency visible-light driven photocatalysis

    NASA Astrophysics Data System (ADS)

    Zhao, Fenfen; Rong, Yuefei; Wan, Junmin; Hu, Zhiwen; Peng, Zhiqin; Wang, Bing

    2018-03-01

    MoS2 quantum dots (QDs) that are 5 nm in size were deposited on the surface of ultrathin TiO2 nanotubes (TNTs) with 5 nm wall thickness by using an improved hydrothermal method to form a MoS2 QDs@TNT visible-light photocatalyst. The ultrathin TNTs with high percentage of photocatalytic reactive facets were fabricated by the commercially available TiO2 nanoparticles (P25) through an improved hydrothermal method, and the MoS2 QDs were acquired by using a surfactant-assisted technique. The novel MoS2 QDs@TNT photocatalysts showed excellent photocatalytic activity with a decolorization rate of 92% or approximately 3.5 times more than that of pure TNTs for the high initial concentration of methylene blue solution (20 mg l-1) within 40 min under visible-light irradiation. MoS2 as the co-catalysts favored the broadening of TNTs into the visible-light absorption scope. The quantum confinement and edge effects of the MoS2 QDs and the heterojunction formed between the MoS2 QDs and TNTs efficiently extended the lifetime of photoinduced charges, impeded the recombination of photoexcited electron-hole pairs, and improved the visible-light-driven high-efficiency photocatalysis.

  20. A Co3O4-CDots-C3N4 three component electrocatalyst design concept for efficient and tunable CO2 reduction to syngas.

    PubMed

    Guo, Sijie; Zhao, Siqi; Wu, Xiuqin; Li, Hao; Zhou, Yunjie; Zhu, Cheng; Yang, Nianjun; Jiang, Xin; Gao, Jin; Bai, Liang; Liu, Yang; Lifshitz, Yeshayahu; Lee, Shuit-Tong; Kang, Zhenhui

    2017-11-28

    Syngas, a CO and H 2 mixture mostly generated from non-renewable fossil fuels, is an essential feedstock for production of liquid fuels. Electrochemical reduction of CO 2 and H + /H 2 O is an alternative renewable route to produce syngas. Here we introduce the concept of coupling a hydrogen evolution reaction (HER) catalyst with a CDots/C 3 N 4 composite (a CO 2 reduction catalyst) to achieve a cheap, stable, selective and efficient route for tunable syngas production. Co 3 O 4 , MoS 2 , Au and Pt serve as the HER component. The Co 3 O 4 -CDots-C 3 N 4 electrocatalyst is found to be the most efficient among the combinations studied. The H 2 /CO ratio of the produced syngas is tunable from 0.07:1 to 4:1 by controlling the potential. This catalyst is highly stable for syngas generation (over 100 h) with no other products besides CO and H 2 . Insight into the mechanisms balancing between CO 2 reduction and H 2 evolution when applying the HER-CDots-C 3 N 4 catalyst concept is provided.

  1. 3D Graphene-Ni Foam as an Advanced Electrode for High-Performance Nonaqueous Redox Flow Batteries.

    PubMed

    Lee, Kyubin; Lee, Jungkuk; Kwon, Kyoung Woo; Park, Min-Sik; Hwang, Jin-Ha; Kim, Ki Jae

    2017-07-12

    Electrodes composed of multilayered graphene grown on a metal foam (GMF) were prepared by directly growing multilayer graphene sheets on a three-dimensional (3D) Ni-foam substrate via a self-catalyzing chemical vapor deposition process. The multilayer graphene sheets are successfully grown on the Ni-foam substrate surface, maintaining the unique 3D macroporous structure of the Ni foam. The potential use of GMF electrodes in nonaqueous redox flow batteries (RFBs) is carefully examined using [Co(bpy) 3 ] +/2+ and [Fe(bpy) 3 ] 2+/3+ redox couples. The GMF electrodes display a much improved electrochemical activity and enhanced kinetics toward the [Co(bpy) 3 ] +/2+ (anolyte) and [Fe(bpy) 3 ] 2+/3+ (catholyte) redox couples, compared with the bare Ni metal foam electrodes, suggesting that the 2D graphene sheets having lots of interdomain defects provide sufficient reaction sites and secure electric-conduction pathways. Consequently, a nonaqueous RFB cell assembled with GMF electrodes exhibits high Coulombic and voltage efficiencies of 87.2 and 90.9%, respectively, at the first cycle. This performance can be maintained up to the 50th cycle without significant efficiency loss. Moreover, the importance of a rational electrode design for improving electrochemical performance is addressed.

  2. Rational construction of a stable Zn4O-based MOF for highly efficient CO2 capture and conversion.

    PubMed

    Zhou, Hui-Fang; Liu, Bo; Hou, Lei; Zhang, Wen-Yan; Wang, Yao-Yu

    2018-01-11

    By employing a carboxylate ligand derived from benzene-1,4-dicarboxylate, a chemically stable Zn 4 O-based self-penetrating metal-organic framework has been rationally synthesized, which exhibits high CO 2 adsorption and efficient catalytic conversion for CO 2 cycloaddition.

  3. Mineral Carbonation Potential of CO2 from Natural and Industrial-based Alkalinity Sources

    NASA Astrophysics Data System (ADS)

    Wilcox, J.; Kirchofer, A.

    2014-12-01

    Mineral carbonation is a Carbon Capture and Storage (CSS) technology where gaseous CO2 is reacted with alkaline materials (such as silicate minerals and alkaline industrial wastes) and converted into stable and environmentally benign carbonate minerals (Metz et al., 2005). Here, we present a holistic, transparent life cycle assessment model of aqueous mineral carbonation built using a hybrid process model and economic input-output life cycle assessment approach. We compared the energy efficiency and the net CO2 storage potential of various mineral carbonation processes based on different feedstock material and process schemes on a consistent basis by determining the energy and material balance of each implementation (Kirchofer et al., 2011). In particular, we evaluated the net CO2 storage potential of aqueous mineral carbonation for serpentine, olivine, cement kiln dust, fly ash, and steel slag across a range of reaction conditions and process parameters. A preliminary systematic investigation of the tradeoffs inherent in mineral carbonation processes was conducted and guidelines for the optimization of the life-cycle energy efficiency are provided. The life-cycle assessment of aqueous mineral carbonation suggests that a variety of alkalinity sources and process configurations are capable of net CO2 reductions. The maximum carbonation efficiency, defined as mass percent of CO2 mitigated per CO2 input, was 83% for CKD at ambient temperature and pressure conditions. In order of decreasing efficiency, the maximum carbonation efficiencies for the other alkalinity sources investigated were: olivine, 66%; SS, 64%; FA, 36%; and serpentine, 13%. For natural alkalinity sources, availability is estimated based on U.S. production rates of a) lime (18 Mt/yr) or b) sand and gravel (760 Mt/yr) (USGS, 2011). The low estimate assumes the maximum sequestration efficiency of the alkalinity source obtained in the current work and the high estimate assumes a sequestration efficiency of 85%. The total CO2 storage potential for the alkalinity sources considered in the U.S. ranges from 1.3% to 23.7% of U.S. CO2 emissions, depending on the assumed availability of natural alkalinity sources and efficiency of the mineral carbonation processes.

  4. Photocatalytic acceptorless alkane dehydrogenation: scope, mechanism, and conquering deactivation with carbon dioxide.

    PubMed

    Chowdhury, Abhishek Dutta; Julis, Jennifer; Grabow, Kathleen; Hannebauer, Bernd; Bentrup, Ursula; Adam, Martin; Franke, Robert; Jackstell, Ralf; Beller, Matthias

    2015-01-01

    Alkane dehydrogenation is of special interest for basic science but also offers interesting opportunities for industry. The existing dehydrogenation methodologies make use of heterogeneous catalysts, which suffer from harsh reaction conditions and a lack of selectivity, whereas homogeneous methodologies rely mostly on unsolicited waste generation from hydrogen acceptors. Conversely, acceptorless photochemical alkane dehydrogenation in the presence of trans-Rh(PMe3 )2 (CO)Cl can be regarded as a more benign and atom efficient alternative. However, this methodology suffers from catalyst deactivation over time. Herein, we provide a detailed investigation of the trans-Rh(PMe3 )2 (CO)Cl-photocatalyzed alkane dehydrogenation using spectroscopic and theoretical investigations. These studies inspired us to utilize CO2 to prevent catalyst deactivation, which leads eventually to improved catalyst turnover numbers in the dehydrogenation of alkanes that include liquid organic hydrogen carriers. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  5. Renewable and high efficient syngas production from carbon dioxide and water through solar energy assisted electrolysis in eutectic molten salts

    NASA Astrophysics Data System (ADS)

    Wu, Hongjun; Liu, Yue; Ji, Deqiang; Li, Zhida; Yi, Guanlin; Yuan, Dandan; Wang, Baohui; Zhang, Zhonghai; Wang, Peng

    2017-09-01

    Over-reliance on non-renewable fossil fuel leads to steadily increasing concentration of atmospheric CO2, which has been implicated as a critical factor contributing to global warming. The efficient conversion of CO2 into useful product is highly sought after both in academic and industry. Herein, a novel conversion strategy is proposed to one-step transform CO2/H2O into syngas (CO/H2) in molten salt with electrolysis method. All the energy consumption in this system are contributed from sustainable energy sources: concentrated solar light heats molten salt and solar cell supplies electricity for electrolysis. The eutectic Li0.85Na0.61K0.54CO3/nLiOH molten electrolyte is rationally designed with low melting point (<450 °C). The synthesized syngas contains very desirable content of H2 and CO, with tuneable molar ratios (H2/CO) from 0.6 to 7.8, and with an efficient faradaic efficiency of ∼94.5%. The synthesis of syngas from CO2 with renewable energy at a such low electrolytic temperature not only alleviates heat loss, mitigates system corrosion, and heightens operational safety, but also decreases the generation of methane, thus increases the yield of syngas, which is a remarkable technological breakthrough and this work thus represents a stride in sustainable conversion of CO2 to value-added product.

  6. A Strategy to Enhance the Efficiency of Quantum Dot-Sensitized Solar Cells by Decreasing Electron Recombination with Polyoxometalate/TiO2 as the Electronic Interface Layer.

    PubMed

    Chen, Li; Chen, Weilin; Li, Jianping; Wang, Jiabo; Wang, Enbo

    2017-07-21

    Electron recombination occurring at the TiO 2 /quantum dot sensitizer/electrolyte interface is the key reason for hindering further efficiency improvements to quantum dot sensitized solar cells (QDSCs). Polyoxometalate (POM) can act as an electron-transfer medium to decrease electron recombination in a photoelectric device owing to its excellent oxidation/reduction properties and thermostability. A POM/TiO 2 electronic interface layer prepared by a simple layer-by-layer self-assembly method was added between fluorine-doped tin oxide (FTO) and mesoporous TiO 2 in the photoanode of QDSCs, and the effect on the photovoltaic performance was systematically investigated. Photovoltaic experimental results and the electron transmission mechanism show that the POM/TiO 2 electronic interface layer in the QDSCs can clearly suppress electron recombination, increase the electron lifetime, and result in smoother electron transmission. In summary, the best conversion efficiency of QDSCs with POM/TiO 2 electronic interface layers increases to 8.02 %, which is an improvement of 25.1 % compared with QDSCs without POM/TiO 2 . This work first builds an electron-transfer bridge between FTO and the quantum dot sensitizer and paves the way for further improved efficiency of QDSCs. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  7. Adaptation to high CO2 concentration in an optimal environment: radiation capture, canopy quantum yield and carbon use efficiency

    NASA Technical Reports Server (NTRS)

    Monje, O.; Bugbee, B.

    1998-01-01

    The effect of elevated [CO2] on wheat (Triticum aestivum L. Veery 10) productivity was examined by analysing radiation capture, canopy quantum yield, canopy carbon use efficiency, harvest index and daily C gain. Canopies were grown at either 330 or 1200 micromoles mol-1 [CO2] in controlled environments, where root and shoot C fluxes were monitored continuously from emergence to harvest. A rapidly circulating hydroponic solution supplied nutrients, water and root zone oxygen. At harvest, dry mass predicted from gas exchange data was 102.8 +/- 4.7% of the observed dry mass in six trials. Neither radiation capture efficiency nor carbon use efficiency were affected by elevated [CO2], but yield increased by 13% due to a sustained increase in canopy quantum yield. CO2 enrichment increased root mass, tiller number and seed mass. Harvest index and chlorophyll concentration were unchanged, but CO2 enrichment increased average life cycle net photosynthesis (13%, P < 0.05) and root respiration (24%, P < 0.05). These data indicate that plant communities adapt to CO2 enrichment through changes in C allocation. Elevated [CO2] increases sink strength in optimal environments, resulting in sustained increases in photosynthetic capacity, canopy quantum yield and daily C gain throughout the life cycle.

  8. Planar-Structure Perovskite Solar Cells with Efficiency beyond 21.

    PubMed

    Jiang, Qi; Chu, Zema; Wang, Pengyang; Yang, Xiaolei; Liu, Heng; Wang, Ye; Yin, Zhigang; Wu, Jinliang; Zhang, Xingwang; You, Jingbi

    2017-12-01

    Low temperature solution processed planar-structure perovskite solar cells gain great attention recently, while their power conversions are still lower than that of high temperature mesoporous counterpart. Previous reports are mainly focused on perovskite morphology control and interface engineering to improve performance. Here, this study systematically investigates the effect of precise stoichiometry, especially the PbI 2 contents on device performance including efficiency, hysteresis and stability. This study finds that a moderate residual of PbI 2 can deliver stable and high efficiency of solar cells without hysteresis, while too much residual PbI 2 will lead to serious hysteresis and poor transit stability. Solar cells with the efficiencies of 21.6% in small size (0.0737 cm 2 ) and 20.1% in large size (1 cm 2 ) with moderate residual PbI 2 in perovskite layer are obtained. The certificated efficiency for small size shows the efficiency of 20.9%, which is the highest efficiency ever recorded in planar-structure perovskite solar cells, showing the planar-structure perovskite solar cells are very promising. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  9. Increasing algal photosynthetic productivity by integrating ecophysiology with systems biology.

    PubMed

    Peers, Graham

    2014-11-01

    Oxygenic photosynthesis is the process by which plants, algae, and cyanobacteria convert sunlight and CO2 into chemical energy and biomass. Previously published estimates suggest that algal photosynthesis is, at best, able to convert approximately 5-7% of incident light energy to biomass and there is opportunity for improvement. Recent analyses of in situ photophysiology in mass cultures of algae and cyanobacteria show that cultivation methods can have detrimental effects on a cell's photophysiology - reinforcing the need to understand the complex responses of cell biology to a highly variable environment. A systems-based approach to understanding the stresses and efficiencies associated with light-energy harvesting, CO2 fixation, and carbon partitioning will be necessary to make major headway toward improving photosynthetic yields. Copyright © 2014 Elsevier Ltd. All rights reserved.

  10. A highly efficient CMOS nanoplasmonic crystal enhanced slow-wave thermal emitter improves infrared gas-sensing devices

    PubMed Central

    Pusch, Andreas; De Luca, Andrea; Oh, Sang S.; Wuestner, Sebastian; Roschuk, Tyler; Chen, Yiguo; Boual, Sophie; Ali, Zeeshan; Phillips, Chris C.; Hong, Minghui; Maier, Stefan A.; Udrea, Florin; Hopper, Richard H.; Hess, Ortwin

    2015-01-01

    The application of plasmonics to thermal emitters is generally assisted by absorptive losses in the metal because Kirchhoff’s law prescribes that only good absorbers make good thermal emitters. Based on a designed plasmonic crystal and exploiting a slow-wave lattice resonance and spontaneous thermal plasmon emission, we engineer a tungsten-based thermal emitter, fabricated in an industrial CMOS process, and demonstrate its markedly improved practical use in a prototype non-dispersive infrared (NDIR) gas-sensing device. We show that the emission intensity of the thermal emitter at the CO2 absorption wavelength is enhanced almost 4-fold compared to a standard non-plasmonic emitter, which enables a proportionate increase in the signal-to-noise ratio of the CO2 gas sensor. PMID:26639902

  11. High Efficiency Low Cost CO2 Compression Using Supersonic Shock Wave Technology

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Williams, J; Aarnio, M; Grosvenor, A

    2010-12-31

    Development and testing results from a supersonic compressor are presented. The compressor achieved record pressure ratio for a fully-supersonic stage and successfully demonstrated the technology potential. Several tasks were performed in compliance with the DOE award objectives. A high-pressure ratio compressor was retrofitted to improve rotordynamics behavior and successfully tested. An outside review panel confirmed test results and design approach. A computational fluid dynamics code used to analyze the Ramgen supersonic flowpath was extensively and successfully modified to improve use on high-performance computing platforms. A comprehensive R&D implementation plan was developed and used to lay the groundwork for a futuremore » full-scale compressor demonstration. Conceptual design for a CO2 demonstration compressor was developed and reviewed.« less

  12. Improving Energy Efficiency for the Vehicle Assembly Industry: A Discrete Event Simulation Approach

    NASA Astrophysics Data System (ADS)

    Oumer, Abduaziz; Mekbib Atnaw, Samson; Kie Cheng, Jack; Singh, Lakveer

    2016-11-01

    This paper presented a Discrete Event Simulation (DES) model for investigating and improving energy efficiency in vehicle assembly line. The car manufacturing industry is one of the highest energy consuming industries. Using Rockwell Arena DES package; a detailed model was constructed for an actual vehicle assembly plant. The sources of energy considered in this research are electricity and fuel; which are the two main types of energy sources used in a typical vehicle assembly plant. The model depicts the performance measurement for process- specific energy measures of painting, welding, and assembling processes. Sound energy efficiency model within this industry has two-fold advantage: reducing CO2 emission and cost reduction associated with fuel and electricity consumption. The paper starts with an overview of challenges in energy consumption within the facilities of automotive assembly line and highlights the parameters for energy efficiency. The results of the simulation model indicated improvements for energy saving objectives and reduced costs.

  13. Preparation and use of tetra-alkyl cobalt dicarbollide for extraction of cesium and strontium into hydrocarbon solvents

    DOEpatents

    Miller, Rebecca L.; Pinkerton, Anthony B.; Abney, Kent D.; Kinkead, Scott A.

    1997-01-01

    Preparation and use of tetra-C-alkyl cobalt dicarbollide for extraction of cesium and strontium into hydrocarbon solvents. Tetra-C-alkyl derivatives of cobalt dicarbollide, Co(C.sub.2 R.sub.2 B.sub.9 H.sub.9).sub.2.sup.- (CoB.sub.2 R.sub.4.sup.- ; R=CH.sub.3 and C.sub.6 H.sub.13) are demonstrated to be significant cesium and strontium extractants from acidic and alkaline solutions into non-toxic organic solvent systems. Extractions using mesitylene and diethylbenzene are compared to those with nitrobenzene as the organic phase. CoB.sub.2 -hexyl.sub.4.sup.- in diethylbenzene shows improved selectivity (10.sup.4) for Cs over Na in acidic solution. In dilute alkaline solution, CoB.sub.2 -hexyl.sub.4.sup.- extracts Cs less efficiently, but more effectively removes Sr from higher base concentrations. A general synthesis of tetra-C-alkyl cobalt dicarbollides is described.

  14. Preparation and use of tetra-alkyl cobalt dicarbollide for extraction of cesium and strontium into hydrocarbon solvents

    DOEpatents

    Miller, R.L.; Pinkerton, A.B.; Abney, K.D.; Kinkead, S.A.

    1997-02-11

    Preparation and use of tetra-C-alkyl cobalt dicarbollide for extraction of cesium and strontium into hydrocarbon solvents. Tetra-C-alkyl derivatives of cobalt dicarbollide, Co(C{sub 2}R{sub 2}B{sub 9}H{sub 9}){sub 2}{sup {minus}}(CoB{sub 2}R{sub 4}{sup {minus}}; R=CH{sub 3} and C{sub 6}H{sub 13}) are demonstrated to be significant cesium and strontium extractants from acidic and alkaline solutions into non-toxic organic solvent systems. Extractions using mesitylene and diethylbenzene are compared to those with nitrobenzene as the organic phase. CoB{sub 2}-hexyl{sub 4}{sup {minus}} in diethylbenzene shows improved selectivity (10{sup 4}) for Cs over Na in acidic solution. In dilute alkaline solution, CoB{sub 2}-hexyl{sub 4}{sup {minus}} extracts Cs less efficiently, but more effectively removes Sr from higher base concentrations. A general synthesis of tetra-C-alkyl cobalt dicarbollides is described. 6 figs.

  15. Engineered Escherichia coli with Periplasmic Carbonic Anhydrase as a Biocatalyst for CO2 Sequestration

    PubMed Central

    Jo, Byung Hoon; Kim, Im Gyu; Seo, Jeong Hyun; Kang, Dong Gyun

    2013-01-01

    Carbonic anhydrase is an enzyme that reversibly catalyzes the hydration of carbon dioxide (CO2). It has been suggested recently that this remarkably fast enzyme can be used for sequestration of CO2, a major greenhouse gas, making this a promising alternative for chemical CO2 mitigation. To promote the economical use of enzymes, we engineered the carbonic anhydrase from Neisseria gonorrhoeae (ngCA) in the periplasm of Escherichia coli, thereby creating a bacterial whole-cell catalyst. We then investigated the application of this system to CO2 sequestration by mineral carbonation, a process with the potential to store large quantities of CO2. ngCA was highly expressed in the periplasm of E. coli in a soluble form, and the recombinant bacterial cell displayed the distinct ability to hydrate CO2 compared with its cytoplasmic ngCA counterpart and previously reported whole-cell CA systems. The expression of ngCA in the periplasm of E. coli greatly accelerated the rate of calcium carbonate (CaCO3) formation and exerted a striking impact on the maximal amount of CaCO3 produced under conditions of relatively low pH. It was also shown that the thermal stability of the periplasmic enzyme was significantly improved. These results demonstrate that the engineered bacterial cell with periplasmic ngCA can successfully serve as an efficient biocatalyst for CO2 sequestration. PMID:23974145

  16. High-Density Nanosharp Microstructures Enable Efficient CO2 Electroreduction.

    PubMed

    Saberi Safaei, Tina; Mepham, Adam; Zheng, Xueli; Pang, Yuanjie; Dinh, Cao-Thang; Liu, Min; Sinton, David; Kelley, Shana O; Sargent, Edward H

    2016-11-09

    Conversion of CO 2 to CO powered by renewable electricity not only reduces CO 2 pollution but also is a means to store renewable energy via chemical production of fuels from CO. However, the kinetics of this reaction are slow due its large energetic barrier. We have recently reported CO 2 reduction that is considerably enhanced via local electric field concentration at the tips of sharp gold nanostructures. The high local electric field enhances CO 2 concentration at the catalytic active sites, lowering the activation barrier. Here we engineer the nucleation and growth of next-generation Au nanostructures. The electroplating overpotential was manipulated to generate an appreciably increased density of honed nanoneedles. Using this approach, we report the first application of sequential electrodeposition to increase the density of sharp tips in CO 2 electroreduction. Selective regions of the primary nanoneedles are passivated using a thiol SAM (self-assembled monolayer), and then growth is concentrated atop the uncovered high-energy planes, providing new nucleation sites that ultimately lead to an increase in the density of the nanosharp structures. The two-step process leads to a new record in CO 2 to CO reduction, with a geometric current density of 38 mA/cm 2 at -0.4 V (vs reversible hydrogen electrode), and a 15-fold improvement over the best prior reports of electrochemical surface area (ECSA) normalized current density.

  17. Tuning of CO2 Reduction Selectivity on Metal Electrocatalysts.

    PubMed

    Wang, Yuhang; Liu, Junlang; Wang, Yifei; Al-Enizi, Abdullah M; Zheng, Gengfeng

    2017-11-01

    Climate change, caused by heavy CO 2 emissions, is driving new demands to alleviate the rising concentration of atmospheric CO 2 levels. Enlightened by the photosynthesis of green plants, photo(electro)chemical catalysis of CO 2 reduction, also known as artificial photosynthesis, is emerged as a promising candidate to address these demands and is widely investigated during the past decade. Among various artificial photosynthetic systems, solar-driven electrochemical CO 2 reduction is widely recognized to possess high efficiencies and potentials for practical application. The efficient and selective electroreduction of CO 2 is the key to the overall solar-to-chemical efficiency of artificial photosynthesis. Recent studies show that various metallic materials possess the capability to play as electrocatalysts for CO 2 reduction. In order to achieve high selectivity for CO 2 reduction products, various efforts are made including studies on electrolytes, crystal facets, oxide-derived catalysts, electronic and geometric structures, nanostructures, and mesoscale phenomena. In this Review, these methods for tuning the selectivity of CO 2 electrochemical reduction of metallic catalysts are summarized. The challenges and perspectives in this field are also discussed. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  18. Photosynthesis of Scenedesmus obliquus in outdoor open thin-layer cascade system in high and low CO2 in Belgium.

    PubMed

    de Marchin, Thomas; Erpicum, Michel; Franck, Fabrice

    2015-12-10

    Two outdoor open thin-layer cascade systems operated as batch cultures with the alga Scenedesmus obliquus were used to compare the productivity and photosynthetic acclimations in control and CO2 supplemented cultures in relation with the outdoor light irradiance. We found that the culture productivity was limited by CO2 availability. In the CO2 supplemented culture, we obtained a productivity of up to 24gdwm(-2)day(-1) and found a photosynthetic efficiency (value based on the PAR solar radiation energy) of up to 5%. In the CO2 limited culture, we obtained a productivity of up to 10gdwm(-2)day(-1) while the photosynthetic efficiency was up to 3.3% and decreased to 2.1% when the integrated daily PAR increased. Fluorescence and oxygen evolution measurements showed that ETR and oxygen evolution light saturation curves, as well as light-dependent O2 uptake were similar in algal samples from both cultures when the CO2 limitation was removed. In contrast, we found that CO2 limitation conducted to a decreased PSII photochemical efficiency and an increased light-induced heat-dissipation in the control culture compared to the CO2 supplemented culture. These features are in line with a lower light use efficiency and may therefore contribute to the lower productivity observed in absence of CO2 supplementation in outdoor mass cultures of S. obliquus. Copyright © 2015 Elsevier B.V. All rights reserved.

  19. Genotypically Identifying Wheat Mesophyll Conductance Regulation under Progressive Drought Stress

    PubMed Central

    Olsovska, Katarina; Kovar, Marek; Brestic, Marian; Zivcak, Marek; Slamka, Pavol; Shao, Hong Bo

    2016-01-01

    Photosynthesis limitation by CO2 flow constraints from sub-stomatal cavities to carboxylation sites in chloroplasts under drought stress conditions is, at least in some plant species or crops not fully understood, yet. Leaf mesophyll conductance for CO2 (gm) may considerably affect both photosynthesis and water use efficiency (WUE) in plants under drought conditions. The aim of our study was to detect the responses of gm in leaves of four winter wheat (Triticum aestivum L.) genotypes from different origins under long-term progressive drought. Based on the measurement of gas-exchange parameters the variability of genotypic responses was analyzed at stomatal (stomata closure) and non-stomatal (diffusional and biochemical) limits of net CO2 assimilation rate (AN). In general, progressive drought caused an increasing leaf diffusion resistance against CO2 flow leading to the decrease of AN, gm and stomatal conductance (gs), respectively. Reduction of gm also led to inhibition of carboxylation efficiency (Vcmax). On the basis of achieved results a strong positive relationship between gm and gs was found out indicating a co-regulation and mutual independence of the relationship under the drought conditions. In severely stressed plants, the stomatal limitation of the CO2 assimilation rate was progressively increased, but to a less extent in comparison to gm, while a non-stomatal limitation became more dominant due to the prolonged drought. Mesophyll conductance (gm) seems to be a suitable mechanism and parameter for selection of improved diffusional properties and photosynthetic carbon assimilation in C3 plants, thus explaining their better photosynthetic performance at a whole plant level during periods of drought. PMID:27551283

  20. Electronic Modulation of Electrocatalytically Active Center of Cu7S4 Nanodisks by Cobalt-Doping for Highly Efficient Oxygen Evolution Reaction.

    PubMed

    Li, Qun; Wang, Xianfu; Tang, Kai; Wang, Mengfan; Wang, Chao; Yan, Chenglin

    2017-12-26

    Cu-based electrocatalysts have seldom been studied for water oxidation because of their inferior activity and poor stability regardless of their low cost and environmentally benign nature. Therefore, exploring an efficient way to improve the activity of Cu-based electrocatalysts is very important for their practical application. Modifying electronic structure of the electrocatalytically active center of electrocatalysts by metal doping to favor the electron transfer between catalyst active sites and electrode is an important approach to optimize hydrogen and oxygen species adsorption energy, thus leading to the enhanced intrinsic electrocatalytic activity. Herein, Co-doped Cu 7 S 4 nanodisks were synthesized and investigated as highly efficient electrocatalyst for oxygen evolution reaction (OER) due to the optimized electronic structure of the active center. Density-functional theory (DFT) calculations reveal that Co-engineered Cu 7 S 4 could accelerate electron transfer between Co and Cu sites, thus decrease the energy barriers of intermediates and products during OER, which are crucial for enhanced catalytic properties. As expected, Co-engineered Cu 7 S 4 nanodisks exhibit a low overpotential of 270 mV to achieve current density of 10 mA cm -2 as well as decreased Tafel slope and enhanced turnover frequencies as compared to bare Cu 7 S 4 . This discovery not only provides low-cost and efficient Cu-based electrocatalyst by Co doping, but also exhibits an in-depth insight into the mechanism of the enhanced OER properties.

  1. Strong electroluminescence from SiO{sub 2}-Tb{sub 2}O{sub 3}-Al{sub 2}O{sub 3} mixed layers fabricated by atomic layer deposition

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Rebohle, L., E-mail: l.rebohle@hzdr.de; Braun, M.; Wutzler, R.

    2014-06-23

    We report on the bright green electroluminescence (EL) with power efficiencies up to 0.15% of SiO{sub 2}-Tb{sub 2}O{sub 3}-mixed layers fabricated by atomic layer deposition and partly co-doped with Al{sub 2}O{sub 3}. The electrical, EL, and breakdown behavior is investigated as a function of the Tb and the Al concentration. Special attention has been paid to the beneficial role of Al{sub 2}O{sub 3} co-doping which improves important device parameters. In detail, it increases the maximum EL power efficiency and EL decay time, it nearly doubles the fraction of excitable Tb{sup 3+} ions, it shifts the region of high EL powermore » efficiencies to higher injection currents, and it reduces the EL quenching over the device lifetime by an approximate factor of two. It is assumed that the presence of Al{sub 2}O{sub 3} interferes the formation of Tb clusters and related defects. Therefore, the system SiO{sub 2}-Tb{sub 2}O{sub 3}-Al{sub 2}O{sub 3} represents a promising alternative for integrated, Si-based light emitters.« less

  2. Decorating CoP and Pt Nanoparticles on Graphitic Carbon Nitride Nanosheets to Promote Overall Water Splitting by Conjugated Polymers.

    PubMed

    Pan, Zhiming; Zheng, Yun; Guo, Fangsong; Niu, Pingping; Wang, Xinchen

    2017-01-10

    The splitting of water into H 2 and O 2 using solar energy is one of the key steps in artificial photosynthesis for the future production of renewable energy. Here, we show the first use of CoP and Pt nanoparticles as dual co-catalysts to modify graphitic carbon nitride (g-C 3 N 4 ) polymer to achieve overall water splitting under visible light irradiation. Our findings demonstrate that loading dual co-catalysts on delaminated g-C 3 N 4 imparts surface redox sites on the g-C 3 N 4 nanosheets that can not only promote catalytic kinetics but also promote charge separation and migration in the soft interface, thus improving the photocatalytic efficiency for overall water splitting. This robust, abundant, and stable photocatalyst based on covalent organic frameworks is demonstrated to hold great promise by forming heterojunctions with CoP and Pt for catalyzing the direct splitting of water into stoichiometric H 2 and O 2 using energy from photons. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. Twin defects engineered Pd cocatalyst on C3N4 nanosheets for enhanced photocatalytic performance in CO2 reduction reaction

    NASA Astrophysics Data System (ADS)

    Lang, Qingqing; Hu, Wenli; Zhou, Penghui; Huang, Tianlong; Zhong, Shuxian; Yang, Lining; Chen, Jianrong; Bai, Song

    2017-12-01

    Photocatalytic conversion of CO2 to value-added chemicals, a potential route to addressing the depletion of fossil fuels and anthropogenic climate change, is greatly limited by the low-efficient semiconductor photocatalyst. The integration of cocatalyst with light-harvesting semiconductor is a promising approach to enhancing the photocatalytic performance in CO2 reduction reaction. The enhancement is greatly determined by the catalytic active sites on the surface of cocatalyst. Herein, we demonstrate that the photocatalytic performance in the CO2 reduction reaction is greatly promoted by twin defects engineered Pd cocatalyst. In this work, Pd nanoicosahedrons with twin defects were in situ grown on C3N4 nanosheets, which effectively improve the photocatalytic performance in reduction of CO2 to CO and CH4 in comparison with Pd nanotetrahedrons without twin defects. It is proposed that the twin boundary (TB) terminations on the surface of Pd cocatalysts are highly catalytic active sites for CO2 reduction reaction. Based on the proposed mechanism, the photocatalytic activity and selectivity in CO2 reduction were further advanced through reducing the size of Pd icosahedral cocatalyst resulted from the increased surface density of TB terminations. The defect engineering on the surface of cocatalyst represents a novel route in realizing high-performance photocatalytic applications.

  4. Twin defects engineered Pd cocatalyst on C3N4 nanosheets for enhanced photocatalytic performance in CO2 reduction reaction.

    PubMed

    Lang, Qingqing; Hu, Wenli; Zhou, Penghui; Huang, Tianlong; Zhong, Shuxian; Yang, Lining; Chen, Jianrong; Bai, Song

    2017-12-01

    Photocatalytic conversion of CO 2 to value-added chemicals, a potential route to addressing the depletion of fossil fuels and anthropogenic climate change, is greatly limited by the low-efficient semiconductor photocatalyst. The integration of cocatalyst with light-harvesting semiconductor is a promising approach to enhancing the photocatalytic performance in CO 2 reduction reaction. The enhancement is greatly determined by the catalytic active sites on the surface of cocatalyst. Herein, we demonstrate that the photocatalytic performance in the CO 2 reduction reaction is greatly promoted by twin defects engineered Pd cocatalyst. In this work, Pd nanoicosahedrons with twin defects were in situ grown on C 3 N 4 nanosheets, which effectively improve the photocatalytic performance in reduction of CO 2 to CO and CH 4 in comparison with Pd nanotetrahedrons without twin defects. It is proposed that the twin boundary (TB) terminations on the surface of Pd cocatalysts are highly catalytic active sites for CO 2 reduction reaction. Based on the proposed mechanism, the photocatalytic activity and selectivity in CO 2 reduction were further advanced through reducing the size of Pd icosahedral cocatalyst resulted from the increased surface density of TB terminations. The defect engineering on the surface of cocatalyst represents a novel route in realizing high-performance photocatalytic applications.

  5. Selective growth of chirality-enriched semiconducting carbon nanotubes by using bimetallic catalysts from salt precursors.

    PubMed

    Zhao, Xiulan; Yang, Feng; Chen, Junhan; Ding, Li; Liu, Xiyan; Yao, Fengrui; Li, Meihui; Zhang, Daqi; Zhang, Zeyao; Liu, Xu; Yang, Juan; Liu, Kaihui; Li, Yan

    2018-04-19

    Bimetallic catalysts play important roles in the selective growth of single-walled carbon nanotubes (SWNTs). Using the simple salts (NH4)6W7O24·6H2O and Co(CH3COO)2·4H2O as precursors, tungsten-cobalt catalysts were prepared. The catalysts were composed of W6Co7 intermetallic compounds and tungsten-dispersed cobalt. With the increase of the W/Co ratio in the precursors, the content of W6Co7 was increased. Because the W6Co7 intermetallic compound can enable the chirality specified growth of SWNTs, the selectivity of the resulting SWNTs is improved at a higher W/Co ratio. At a W/Co ratio of 6 : 4 and under optimized chemical vapor deposition conditions, we realized the direct growth of semiconducting SWNTs with the purity of ∼96%, in which ∼62% are (14, 4) tubes. Using salts as precursors to prepare tungsten-cobalt bimetallic catalysts is flexible and convenient. This offers an efficient pathway for the large-scale preparation of chirality enriched semiconducting SWNTs.

  6. ZnSe quantum dots modified with a Ni(cyclam) catalyst for efficient visible-light driven CO2 reduction in water.

    PubMed

    Kuehnel, Moritz F; Sahm, Constantin D; Neri, Gaia; Lee, Jonathan R; Orchard, Katherine L; Cowan, Alexander J; Reisner, Erwin

    2018-03-07

    A precious metal and Cd-free photocatalyst system for efficient CO 2 reduction in water is reported. The hybrid assembly consists of ligand-free ZnSe quantum dots (QDs) as a visible-light photosensitiser combined with a phosphonic acid-functionalised Ni(cyclam) catalyst, NiCycP. This precious metal-free photocatalyst system shows a high activity for aqueous CO 2 reduction to CO (Ni-based TON CO > 120), whereas an anchor-free catalyst, Ni(cyclam)Cl 2 , produced three times less CO. Additional ZnSe surface modification with 2-(dimethylamino)ethanethiol (MEDA) partially suppresses H 2 generation and enhances the CO production allowing for a Ni-based TON CO of > 280 and more than 33% selectivity for CO 2 reduction over H 2 evolution, after 20 h visible light irradiation ( λ > 400 nm, AM 1.5G, 1 sun). The external quantum efficiency of 3.4 ± 0.3% at 400 nm is comparable to state-of-the-art precious metal photocatalysts. Transient absorption spectroscopy showed that band-gap excitation of ZnSe QDs is followed by rapid hole scavenging and very fast electron trapping in ZnSe. The trapped electrons transfer to NiCycP on the ps timescale, explaining the high performance for photocatalytic CO 2 reduction. With this work we introduce ZnSe QDs as an inexpensive and efficient visible light-absorber for solar fuel generation.

  7. Optimization of Agrobacterium-Mediated Transformation in Soybean.

    PubMed

    Li, Shuxuan; Cong, Yahui; Liu, Yaping; Wang, Tingting; Shuai, Qin; Chen, Nana; Gai, Junyi; Li, Yan

    2017-01-01

    High transformation efficiency is a prerequisite for study of gene function and molecular breeding. Agrobacterium tumefaciens -mediated transformation is a preferred method in many plants. However, the transformation efficiency in soybean is still low. The objective of this study is to optimize Agrobacterium -mediated transformation in soybean by improving the infection efficiency of Agrobacterium and regeneration efficiency of explants. Firstly, four factors affecting Agrobacterium infection efficiency were investigated by estimation of the rate of GUS transient expression in soybean cotyledonary explants, including Agrobacterium concentrations, soybean explants, Agrobacterium suspension medium, and co-cultivation time. The results showed that an infection efficiency of over 96% was achieved by collecting the Agrobacterium at a concentration of OD 650 = 0.6, then using an Agrobacterium suspension medium containing 154.2 mg/L dithiothreitol to infect the half-seed cotyledonary explants (from mature seeds imbibed for 1 day), and co-cultured them for 5 days. The Agrobacterium infection efficiencies for soybean varieties Jack Purple and Tianlong 1 were higher than the other six varieties. Secondly, the rates of shoot elongation were compared among six different concentration combinations of gibberellic acid (GA 3 ) and indole-3-acetic acid (IAA). The shoot elongation rate of 34 and 26% was achieved when using the combination of 1.0 mg/L GA 3 and 0.1 mg/L IAA for Jack Purple and Tianlong 1, respectively. This rate was higher than the other five concentration combinations of GA 3 and IAA, with an 18 and 11% increase over the original laboratory protocol (a combination of 0.5 mg/L GA 3 and 0.1 mg/L IAA), respectively. The transformation efficiency was 7 and 10% for Jack Purple and Tianlong 1 at this optimized hormone concentration combination, respectively, which was 2 and 6% higher than the original protocol, respectively. Finally, GUS histochemical staining, PCR, herbicide (glufosinate) painting, and QuickStix Kit for Liberty Link ( bar ) were used to verify the positive transgenic plants, and absolute quantification PCR confirmed the exogenous gene existed as one to three copies in the soybean genome. This study provides an improved protocol for Agrobacterium -mediated transformation in soybean and a useful reference to improve the transformation efficiency in other plant species.

  8. Efficient hydrogen storage and production using a catalyst with an imidazoline-based, proton-responsive ligand

    DOE PAGES

    Wang, Lin; Onishi, Naoya; Murata, Kazuhisa; ...

    2016-12-28

    A series of new imidazoline-based iridium complexes has been developed for hydrogenation of CO 2 and dehydrogenation of formic acid. One of the proton-responsive complexes bearing two –OH groups at ortho and para positions on a coordinating pyridine ring (3 b) can catalyze efficiently the chemical fixation of CO 2 and release H 2 under mild conditions in aqueous media without using organic additives/solvents. Notably, hydrogenation of CO 2 can be efficiently carried out under CO 2 and H 2 at atmospheric pressure in basic water by 3 b, achieving a turnover frequency of 106 h –1 and a turnovermore » number of 7280 at 25 °C, which are higher than ever reported. Furthermore, highly efficient CO-free hydrogen production from formic acid in aqueous solution employing the same catalyst under mild conditions has been achieved, thus providing a promising potential H 2-storage system in water.« less

  9. Regional hospital improves efficiency with co-generation retrofit.

    PubMed

    Knutson, D; Anderson, L

    1999-11-01

    Feasibility analysis of the co-generation retrofit of the Red Deer Regional Hospital pointed to a reasonable payback of capital cost and increased efficiency in operation of the facility. Budget restrictions nearly stopped the project from proceeding. Innovative construction procedures proposed by the Facility Management Group, in particular, Mr Keith Metcalfe, Director of Maintenance, allowed a worthwhile project to reach successful completion. We feel that this model can perhaps be used by similar facilities in the future to achieve their energy efficiency goals.

  10. CO2 Removal and Atmosphere Revitalization Systems for Next Generation Space Flight

    NASA Technical Reports Server (NTRS)

    Luna, Bernadette; Mulloth, Lila M.; Varghese, Mini M.; Hogan, John Andrew

    2010-01-01

    Removal of metabolic CO2 from breathing air is a vital process for life support in all crewed space missions. A CO2 removal processor called the Low Power CO2 Removal (LPCOR) system is being developed in the Bioengineering Branch at NASA Ames Research Center. LPCOR utilizes advanced adsorption and membrane gas separation processes to achieve substantial power and mass reduction when compared to the state-of-the-art carbon dioxide removal assembly (CORA) of the US segment of the International Space Station (ISS). LPCOR is an attractive alternative for use in commercial spacecraft for short-duration missions and can easily be adapted for closed-loop life support applications. NASA envisions a next-generation closed-loop atmosphere revitalization system that integrates advanced CO2 removal, O2 recovery, and trace contaminant control processes to improve overall system efficiency. LPCOR will serve as the front end to such a system. LPCOR is a reliable air revitalization technology that can serve both the near-term and long-term human space flight needs of NASA and its commercial partners.

  11. Does Long-Term Elevation of CO2 Concentration Increase Photosynthesis in Forest Floor Vegetation? (Indiana Strawberry in a Maryland Forest).

    PubMed

    Osborne, C. P.; Drake, B. G.; LaRoche, J.; Long, S. P.

    1997-05-01

    As the partial pressure of CO2 (pCO2) in the atmosphere rises, photorespiratory loss of carbon in C3 photosynthesis will diminish and the net efficiency of light-limited photosynthetic carbon uptake should rise. We tested this expectation for Indiana strawberry (Duchesnea indica) growing on a Maryland forest floor. Open-top chambers were used to elevate the pCO2 of a forest floor habitat to 67 Pa and were paired with control chambers providing an ambient pCO2 of 38 Pa. After 3.5 years, D. indica leaves grown and measured in the elevated pCO2 showed a significantly greater maximum quantum efficiency of net photosynthesis (by 22%) and a lower light compensation point (by 42%) than leaves grown and measured in the control chambers. The quantum efficiency to minimize photorespiration, measured in 1% O2, was the same for controls and plants grown at elevated pCO2. This showed that the maximum efficiency of light-energy transduction into assimilated carbon was not altered by acclimation and that the increase in light-limited photosynthesis at elevated pCO2 was simply a function of the decrease in photorespiration. Acclimation did decrease the ribulose-1,5-bisphosphate carboxylase/oxygenase and light-harvesting chlorophyll protein content of the leaf by more than 30%. These changes were associated with a decreased capacity for light-saturated, but not light-limited, photosynthesis. Even so, leaves of D. indica grown and measured at elevated pCO2 showed greater light-saturated photosynthetic rates than leaves grown and measured at the current atmospheric pCO2. In situ measurements under natural forest floor lighting showed large increases in leaf photosynthesis at elevated pCO2, relative to controls, in both summer and fall. The increase in efficiency of light-limited photosynthesis with elevated pCO2 allowed positive net photosynthetic carbon uptake on days and at locations on the forest floor that light fluxes were insufficient for positive net photosynthesis in the current atmospheric pCO2.

  12. In vivo free-breathing DTI and IVIM of the whole human heart using a real-time slice-followed SE-EPI navigator-based sequence: A reproducibility study in healthy volunteers.

    PubMed

    Moulin, Kevin; Croisille, Pierre; Feiweier, Thorsten; Delattre, Benedicte M A; Wei, Hongjiang; Robert, Benjamin; Beuf, Olivier; Viallon, Magalie

    2016-07-01

    In this study, we proposed an efficient free-breathing strategy for rapid and improved cardiac diffusion-weighted imaging (DWI) acquisition using a single-shot spin-echo echo planar imaging (SE-EPI) sequence. A real-time slice-following technique during free-breathing was combined with a sliding acquisition-window strategy prior Principal Component Analysis temporal Maximum Intensity Projection (PCAtMIP) postprocessing of in-plane co-registered diffusion-weighted images. This methodology was applied to 10 volunteers to quantify the performance of the motion correction technique and the reproducibility of diffusion parameters. The slice-following technique offers a powerful head-foot respiratory motion management solution for SE-EPI cDWI with the advantage of a 100% duty cycle scanning efficiency. The level of co-registration was further improved using nonrigid motion corrections and was evaluated with a co-registration index. Vascular fraction f and the diffusion coefficients D and D* were determined to be 0.122 ± 0.013, 1.41 ± 0.09 × 10(-3) mm(2) /s and 43.6 ± 9.2 × 10(-3) mm(2) /s, respectively. From the multidirectional dataset, the measured mean diffusivity was 1.72 ± 0.09 × 10(-3) mm(2) /s and the fractional anisotropy was 0.36 ± 0.02. The slice-following DWI SE-EPI sequence is a promising solution for clinical implementation, offering a robust improved workflow for further evaluation of DWI in cardiology. Magn Reson Med 76:70-82, 2016. © 2015 Wiley Periodicals, Inc. © 2015 Wiley Periodicals, Inc.

  13. Efficient reduction of CO2 to CO with high current density using in situ or ex situ prepared Bi-based materials.

    PubMed

    Medina-Ramos, Jonnathan; DiMeglio, John L; Rosenthal, Joel

    2014-06-11

    The development of inexpensive electrocatalysts that can promote the reduction of CO2 to CO with high selectivity, efficiency, and large current densities is an important step on the path to renewable production of liquid carbon-based fuels. While precious metals such as gold and silver have historically been the most active cathode materials for CO2 reduction, the price of these materials precludes their use on the scale required for fuel production. Bismuth, by comparison, is an affordable and environmentally benign metal that shows promise for CO2 conversion applications. In this work, we show that a bismuth-carbon monoxide evolving catalyst (Bi-CMEC) can be formed under either aqueous or nonaqueous conditions using versatile electrodeposition methods. In situ formation of this thin-film catalyst on an inexpensive carbon electrode using an organic soluble Bi(3+) precursor streamlines preparation of this material and generates a robust catalyst for CO2 reduction. In the presence of appropriate imidazolium based ionic liquid promoters, the Bi-CMEC platform can selectively catalyze conversion of CO2 to CO without the need for a costly supporting electrolyte. This inexpensive system can catalyze evolution of CO with current densities as high as jCO = 25-30 mA/cm(2) and attendant energy efficiencies of ΦCO ≈ 80% for the cathodic half reaction. These metrics highlight the efficiency of Bi-CMEC, since only noble metals have been previously shown to promote this fuel forming half reaction with such high energy efficiency. Moreover, the rate of CO production by Bi-CMEC ranges from approximately 0.1-0.5 mmol·cm(-2)·h(-1) at an applied overpotential of η ≈ 250 mV for a cathode with surface area equal to 1.0 cm(2). This CO evolution activity is much higher than that afforded by other non-noble metal cathode materials and distinguishes Bi-CMEC as a superior and inexpensive platform for electrochemical conversion of CO2 to fuel.

  14. Modeling and optimization of a concentrated solar supercritical CO2 power plant

    NASA Astrophysics Data System (ADS)

    Osorio, Julian D.

    Renewable energy sources are fundamental alternatives to supply the rising energy demand in the world and to reduce or replace fossil fuel technologies. In order to make renewable-based technologies suitable for commercial and industrial applications, two main challenges need to be solved: the design and manufacture of highly efficient devices and reliable systems to operate under intermittent energy supply conditions. In particular, power generation technologies based on solar energy are one of the most promising alternatives to supply the world energy demand and reduce the dependence on fossil fuel technologies. In this dissertation, the dynamic behavior of a Concentrated Solar Power (CSP) supercritical CO2 cycle is studied under different seasonal conditions. The system analyzed is composed of a central receiver, hot and cold thermal energy storage units, a heat exchanger, a recuperator, and multi-stage compression-expansion subsystems with intercoolers and reheaters between compressors and turbines respectively. The effects of operating and design parameters on the system performance are analyzed. Some of these parameters are the mass flow rate, intermediate pressures, number of compression-expansion stages, heat exchangers' effectiveness, multi-tank thermal energy storage, overall heat transfer coefficient between the solar receiver and the environment and the effective area of the recuperator. Energy and exergy models for each component of the system are developed to optimize operating parameters in order to lead to maximum efficiency. From the exergy analysis, the components with high contribution to exergy destruction were identified. These components, which represent an important potential of improvement, are the recuperator, the hot thermal energy storage tank and the solar receiver. Two complementary alternatives to improve the efficiency of concentrated solar thermal systems are proposed in this dissertation: the optimization of the system's operating parameters and optimization of less efficient components. The parametric optimization is developed for a 1MW reference CSP system with CO2 as the working fluid. The component optimization, focused on the less efficient components, comprises some design modifications to the traditional component configuration for the recuperator, the hot thermal energy storage tank and the solar receiver. The proposed optimization alternatives include the heat exchanger's effectiveness enhancement by optimizing fins shapes, multi-tank thermal energy storage configurations for the hot thermal energy storage tank and the incorporation of a transparent insulation material into the solar receiver. Some of the optimizations are conducted in a generalized way, using dimensionless models to be applicable no only to the CSP but also to other thermal systems. This project is therefore an effort to improve the efficiency of power generation systems based on solar energy in order to make them competitive with conventional fossil fuel power generation devices. The results show that the parametric optimization leads the system to an efficiency of about 21% and a maximum power output close to 1.5 MW. The process efficiencies obtained in this work, of more than 21%, are relatively good for a solar-thermal conversion system and are also comparable with efficiencies of conversion of high performance PV panels. The thermal energy storage allows the system to operate for several hours after sunset. This operating time is approximately increased from 220 to 480 minutes after optimization. The hot and cold thermal energy storage also lessens the temperature fluctuations by providing smooth changes of temperatures at the turbines' and compressors' inlets. Additional improvements in the overall system efficiency are possible by optimizing the less efficient components. In particular, the fin's effectiveness can be improved in more than 5% after its shape is optimized, increments in the efficiency of the thermal energy storage of about 5.7% are possible when the mass is divided into four tanks, and solar receiver efficiencies up to 70% can be maintained for high operating temperatures (~ 1200°C) when a transparent insulation material is incorporated to the receiver. The results obtained in this dissertation indicate that concentrated solar systems using supercritical CO2 could be a viable alternative to satisfying energy needs in desert areas with scarce water and fossil fuel resources.

  15. Multifunctional organized mesoporous tin oxide films templated by graft copolymers for dye-sensitized solar cells.

    PubMed

    Park, Jung Tae; Ahn, Sung Hoon; Roh, Dong Kyu; Lee, Chang Soo; Kim, Jong Hak

    2014-07-01

    The synthesis of organized mesoporous SnO2 films with high porosity, larger pores, and good interconnectivity, obtained by sol-gel templating with an amphiphilic graft copolymer, poly(vinyl chloride)-graft-poly(oxyethylene methacrylate), is reported. An improved performance of dye-sensitized solar cells (DSSCs) is demonstrated by the introduction of a 400 nm thick organized mesoporous SnO2 interfacial (om-SnO2 IF) layer between nanocrystalline TiO2 (nc-TiO2 ) and a fluorine-doped tin oxide substrate. To elucidate the improved efficiency, the structural, optical, and electrochemical properties of the devices were characterized by SEM, UV/Vis spectroscopy, noncontact 3D surface profilometry, intensity-modulated photocurrent/voltage spectroscopy, incident photon-to-electron conversion efficiency, and electrochemical impedance spectroscopy measurements. The energy-conversion efficiency of the solid polymerized ionic liquid based DSSC fabricated with the om-SnO2 IF/nc-TiO2 photoanode reached 5.9% at 100 mW cm(-2) ; this is higher than those of neat nc-TiO2 (3.5%) and organized mesoporous TiO2 interfacial/nc-TiO2 layer (5.4%) photoanodes. The improved efficiency is attributed to the antireflective property, cascadal energy band gap, good interconnectivity, and high electrical conductivity of the om-SnO2 IF layer, which results in enhanced light harvesting, increased electron transport, reduced charge recombination, and decreased interfacial/internal resistance. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  16. Response of Quercus velutina growth and water use efficiency to climate variability and nitrogen fertilization in a temperate deciduous forest in the northeastern USA.

    PubMed

    Jennings, Katie A; Guerrieri, Rossella; Vadeboncoeur, Matthew A; Asbjornsen, Heidi

    2016-04-01

    Nitrogen (N) deposition and changing climate patterns in the northeastern USA can influence forest productivity through effects on plant nutrient relations and water use. This study evaluates the combined effects of N fertilization, climate and rising atmospheric CO2on tree growth and ecophysiology in a temperate deciduous forest. Tree ring widths and stable carbon (δ(13)C) and oxygen (δ(18)O) isotopes were used to assess tree growth (basal area increment, BAI) and intrinsic water use efficiency (iWUE) ofQuercus velutinaLamb., the dominant tree species in a 20+ year N fertilization experiment at Harvard Forest (MA, USA). We found that fertilized trees exhibited a pronounced and sustained growth enhancement relative to control trees, with the low- and high-N treatments responding similarly. All treatments exhibited improved iWUE over the study period (1984-2011). Intrinsic water use efficiency trends in the control trees were primarily driven by changes in stomatal conductance, while a stimulation in photosynthesis, supported by an increase in foliar %N, contributed to enhancing iWUE in fertilized trees. All treatments were predominantly influenced by growing season vapor pressure deficit (VPD), with BAI responding most strongly to early season VPD and iWUE responding most strongly to late season VPD. Nitrogen fertilization increasedQ. velutinasensitivity to July temperature and precipitation. Combined, these results suggest that ambient N deposition in N-limited northeastern US forests has enhanced tree growth over the past 30 years, while rising ambient CO2has improved iWUE, with N fertilization and CO2having synergistic effects on iWUE. © The Author 2016. Published by Oxford University Press. All rights reserved. For Permissions, please email: journals.permissions@oup.com.

  17. Intense laser beams; Proceedings of the Meeting, Los Angeles, CA, Jan. 23, 24, 1992

    NASA Technical Reports Server (NTRS)

    Wade, Richard C. (Editor); Ulrich, Peter B. (Editor)

    1992-01-01

    Various papers on intense laser beams are presented. Individual topics addressed include: novel methods of copper vapor laser excitation, UCLA IR FEL, lasing characteristics of a large-bore copper vapor laser (CVL), copper density measurement of a large-bore CVL, high-power XeCl excimer laser, solid state direct-drive circuit for pumping gas lasers, united energy model for FELs, intensity and frequency instabilities in double-mode CO2 lasers, comparison of output power stabilities of CO and CO2 lasers, increasing efficiency of sealed-off CO lasers, thermal effects in singlet delta oxygen generation, optical extraction from the chemical oxygen-iodine laser medium, generation and laser diagnostic analysis of bismuth fluoride. Also discussed are: high-Q resonator design for an HF overtone chemical lasers, improved coatings for HF overtone lasers, scaled atmospheric blooming experiment, simulation on producing conjugate field using deformable mirrors, paraxial theory of amplitude correction, potential capabilities of adaptive optical systems in the atmosphere, power beaming research at NASA, system evaluations of laser power beaming options, performance projections for laser beam power to space, independent assessment of laser power beaming options, removal of atmospheric CFCs by lasers, efficiency of vaporization cutting by CVL.

  18. Altered Physiological Function, Not Structure, Drives Increased Radiation-Use Efficiency of Soybean Grown at Elevated CO2

    USDA-ARS?s Scientific Manuscript database

    Previous studies of elevated carbon dioxide concentration ([CO2]) on crop canopies have found that radiation-use efficiency is increased more than radiation-interception efficiency. It is assumed that increased radiation-use efficiency is due to changes in leaf-level physiology; however, canopy stru...

  19. Transgenic tobacco plants with improved cyanobacterial Rubisco expression but no extra assembly factors grow at near wild-type rates if provided with elevated CO2

    PubMed Central

    Occhialini, Alessandro; Lin, Myat T.; Andralojc, P. John; Hanson, Maureen R.; Parry, Martin A. J.

    2015-01-01

    SUMMARY Introducing a carbon concentrating mechanism and a faster Rubisco from cyanobacteria into higher plant chloroplasts could improve photosynthetic performance by increasing the rate of CO2 fixation while decreasing losses caused by photorespiration. We previously demonstrated that tobacco plants will grow photoautotrophically using Synechococcus elongatus Rubisco, although the plants exhibited considerably slower growth than wild-type and required supplementary CO2. Because of concerns that vascular plant assembly factors might not be adequate for assembly of a cyanobacterial Rubisco, prior transgenic plants included the cyanobacterial chaperone RbcX or the carboxysomal protein CcmM35. Here we show that neither RbcX nor CcmM35 is needed for assembly of active cyanobacterial Rubisco. Furthermore, by altering the gene regulatory sequences on the Rubisco transgenes, cyanobacterial Rubisco expression was enhanced and the transgenic plants grew at near wild-type growth rates, though still requiring elevated CO2. We performed detailed kinetic characterization of the enzymes produced with and without the RbcX and CcmM35 cyanobacterial proteins. These transgenic plants exhibit photosynthetic characteristics that confirm the predicted benefits of non-native forms of Rubisco with higher carboxylation rate constants in vascular plants and the potential nitrogen use efficiency that may be gained provided that adequate CO2 can be concentrated near the enzyme. PMID:26662726

  20. Complete Decomposition of Li 2 CO 3 in Li–O 2 Batteries Using Ir/B 4 C as Noncarbon-Based Oxygen Electrode

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Song, Shidong; Xu, Wu; Zheng, Jianming

    Incomplete decomposition of Li2CO3 during charge process is a critical barrier for rechargeable Li-O2 batteries. Here we report complete decomposition of Li2CO3 in Li-O2 batteries using ultrafine iridium-decorated boron carbide (Ir/B4C) nanocomposite as oxygen electrode. The systematic investigation on charging the Li2CO3 preloaded Ir/B4C electrode in an ether-based electrolyte demonstrates that Ir/B4C electrode can decompose Li2CO3 with an efficiency close to 100% at below 4.37 V. In contrast, the bare B4C without Ir electrocatalyst can only decompose 4.7% of preloaded Li2CO3. The reaction mechanism of Li2CO3 decomposition in the presence of Ir/B4C electrocatalyst has been further investigated. A Li-O2 batterymore » using Ir/B4C as oxygen electrode material shows highly enhanced cycling stability than that using bare B4C oxygen electrode. These results clearly demonstrate that Ir/B4C is an effecitive oxygen electrode amterial to completely decompose Li2CO3 at relatively low charge voltages and is of significant importance in improving the cycle performanc of aprotic Li-O2 batteries.« less

  1. Enhanced electrochemical performance and storage property of LiNi0.815Co0.15Al0.035O2 via Al gradient doping

    NASA Astrophysics Data System (ADS)

    Duan, Jianguo; Hu, Guorong; Cao, Yanbing; Tan, Chaopu; Wu, Ceng; Du, Ke; Peng, Zhongdong

    2016-09-01

    LiNi1-x-yCoxAlyO2 is a commonly used Ni-rich cathode material because of its relatively low cost, excellent rate capability and high gravimetric energy density. Surface modification is an efficient way to overcome the shortcomings of Ni-rich cathodes such as poor cycling stability and poor thermal stability. A high-powered concentration-gradient cathode material with an average composition of LiNi0.815Co0.15Al0.035O2 (LGNCAO) has been successfully synthesized by using spherical concentration-gradient Ni0.815Co0.15Al0.035(OH)2 (GNCA)as the starting material. An efficient design of the Al3+ precipitation method is developed, which enables obtaining spherical GNCA with ∼10 μm particle size and high tap density. In LGNCAO, the nickel and cobalt concentration decreases gradually whereas the aluminum concentration increases from the centre to the outer layer of each particle. Electrochemical performance and storage properties of LGNCAO have been investigated comparatively. The LGNCAO displays better electrochemical performance and improved storage stability than LNCAO.

  2. Materials, properties, and applications of nitrogen-doped organic semiconductors

    NASA Astrophysics Data System (ADS)

    Chan, Calvin Kar-Fai

    As organic semiconducting materials draw increasing attention for many promising applications, including efficient organic light-emitting diodes (OLEDs), large-area organic photovoltaic (OPV) cells, and flexible organic thin-film transistors (OTFTs), chemical doping of organic materials is emerging as an important technique for overcoming performance deficiencies and material limitations of intrinsic organic films. Although p-doping has been amply demonstrated, molecular n-type doping has been difficult to study because of the inherent instability of easily oxidized n-dopants. In this work, the facile use of two low ionization energy (IE) small molecules that are suitable for n-doping a wide range of organic electronic materials is demonstrated. Cobaltocene (CoCp2) and its derivative, decamethylcobaltocene ( CoCp*2 ), were found to have fairly low IEs for organic compounds. Co-deposition of the n-dopants with different host molecules results in pronounced shifts of the Fermi-level towards unoccupied molecular states, indicating a significant increase in electron concentration. The Fermi-level shifts, measured with ultra-violet photoemission spectroscopy (UPS), are correlated with excess carrier densities using a model based on Fermi-Dirac (F-D) statistics and a Gaussian distributed density of states. The calculated electron densities suggest full dopant ionization at low concentrations, and diminished efficiency at high donor concentrations. The concentration of incorporated dopants is examined by chemical composition analysis of doped films using X-ray photoemission spectroscopy (XPS). Atomic concentration depth profiling determined by Rutherford backscattering (RBS) suggests that the incorporation of CoCp2 and CoCp*2 is well-controlled and the dopants are minimally diffusive. Organic films n-doped using CoCp2 and CoCp*2 show several orders of magnitude increase in current density resulting from both enhanced electron injection and increased electron conductivity in the bulk. Increases in the bulk conductivity suggest both improved electron mobility and higher electron concentrations. These findings are applied with previous work on p-doping to fabricate organic p-i-n homojunction devices that exhibit strong rectification and large built-in potentials. Heterojunction OPVs using undoped CuPc and n-doped C60 display significant increases in open-circuit voltage (Voc), short-circuit current (Isc), fill-factor (FF), and efficiency.

  3. Does long-term elevation of CO{sub 2} concentration increase photosynthesis in forest floor vegetation? Indiana strawberry in a Maryland forest

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Osborne, C.P.; Long, S.P.; Drake, B.G.

    1997-05-01

    As the partial pressure of CO{sub 2} (pCO{sub 2}) in the atmosphere rises, photorespiratory loss of carbon in C, photosynthesis will diminish and the net efficiency of light-limited photosynthetic carbon uptake should rise. Indiana strawberry (Duchesnea indica) growing on a Maryland forest floor was tested. Open-top chambers were used to elevate the pCO{sub 2} of a forest floor habitat to 67 Pa and were paired with control chambers with an ambient pCO{sub 2} of 38 Pa. After 3.5 years, D. indica leaves in the elevated pCO{sub 2} showed a significantly greater maximum quantum efficiency of net photosynthesis (by 22%) andmore » a lower light compensation point (by 42%) than leaves in the control chambers. The quantum efficiency to minimize photorespiration was the same for controls and plants grown at elevated pCO{sub 2}, showing the maximum efficiency of light-energy transduction into assimilated carbon was not altered by acclimation and the increase in light-limited photosynthesis at elevated pCO{sub 2} was a function of the decrease in photorespiration. Acclimation did decrease the ribulose-1,5-bisphosphate carboxylase/oxygenase and light-harvesting chlorophyll protein content of the leaf by more than 30%. These changes were associated with a decreased capacity for light-saturated, but not light-limited, photosynthesis. Leaves of D. indica grown and measured at elevated pCO{sub 2} showed greater light-saturated photosynthetic rates than leaves grown and measured at the current atmospheric pCO{sub 2}. In situ measurements under natural lighting showed large increases in leaf photosynthesis at elevated pCO{sub 2}, relative to controls, in both summer and fall. The increase in efficiency of light-limited photosynthesis with elevated pCO{sub 2} allowed positive net photosynthetic carbon uptake on days and at locations on the forest floor that light fluxes were insufficient for positive net photosynthesis in the current atmospheric pCO{sub 2}. 33 refs., 3 figs., 3 tabs.« less

  4. Process for CO.sub.2 capture using zeolites from high pressure and moderate temperature gas streams

    DOEpatents

    Siriwardane, Ranjani V [Morgantown, WV; Stevens, Robert W [Morgantown, WV

    2012-03-06

    A method for separating CO.sub.2 from a gas stream comprised of CO.sub.2 and other gaseous constituents using a zeolite sorbent in a swing-adsorption process, producing a high temperature CO.sub.2 stream at a higher CO.sub.2 pressure than the input gas stream. The method utilizes CO.sub.2 desorption in a CO.sub.2 atmosphere and effectively integrates heat transfers for optimizes overall efficiency. H.sub.2O adsorption does not preclude effective operation of the sorbent. The cycle may be incorporated in an IGCC for efficient pre-combustion CO.sub.2 capture. A particular application operates on shifted syngas at a temperature exceeding 200.degree. C. and produces a dry CO.sub.2 stream at low temperature and high CO.sub.2 pressure, greatly reducing any compression energy requirements which may be subsequently required.

  5. Formation of methotrexate-PLLA-PEG-PLLA composite microspheres by microencapsulation through a process of suspension-enhanced dispersion by supercritical CO2

    PubMed Central

    Chen, Ai-Zheng; Wang, Guang-Ya; Wang, Shi-Bin; Li, Li; Liu, Yuan-Gang; Zhao, Chen

    2012-01-01

    Background The aim of this study was to improve the drug loading, encapsulation efficiency, and sustained-release properties of supercritical CO2-based drug-loaded polymer carriers via a process of suspension-enhanced dispersion by supercritical CO2 (SpEDS), which is an advanced version of solution-enhanced dispersion by supercritical CO2 (SEDS). Methods Methotrexate nanoparticles were successfully microencapsulated into poly (L-lactide)-poly(ethylene glycol)-poly(L-lactide) (PLLA-PEG-PLLA) by SpEDS. Methotrexate nanoparticles were first prepared by SEDS, then suspended in PLLA-PEG-PLLA solution, and finally microencapsulated into PLLA-PEG-PLLA via SpEDS, where an “injector” was utilized in the suspension delivery system. Results After microencapsulation, the composite methotrexate (MTX)-PLLA-PEG-PLLA microspheres obtained had a mean particle size of 545 nm, drug loading of 13.7%, and an encapsulation efficiency of 39.2%. After an initial burst release, with around 65% of the total methotrexate being released in the first 3 hours, the MTX-PLLA-PEG-PLLA microspheres released methotrexate in a sustained manner, with 85% of the total methotrexate dose released within 23 hours and nearly 100% within 144 hours. Conclusion Compared with a parallel study of the coprecipitation process, microencapsulation using SpEDS offered greater potential to manufacture drug-loaded polymer microspheres for a drug delivery system. PMID:22787397

  6. Buffer Gas Acquisition and Storage

    NASA Technical Reports Server (NTRS)

    Parrish, Clyde F.; Lueck, Dale E.; Jennings, Paul A.; Callahan, Richard A.; Delgado, H. (Technical Monitor)

    2001-01-01

    The acquisition and storage of buffer gases (primarily argon and nitrogen) from the Mars atmosphere provides a valuable resource for blanketing and pressurizing fuel tanks and as a buffer gas for breathing air for manned missions. During the acquisition of carbon dioxide (CO2), whether by sorption bed or cryo-freezer, the accompanying buffer gases build up in the carbon dioxide acquisition system, reduce the flow of CO2 to the bed, and lower system efficiency. It is this build up of buffer gases that provide a convenient source, which must be removed, for efficient capture Of CO2 Removal of this buffer gas barrier greatly improves the charging rate of the CO2 acquisition bed and, thereby, maintains the fuel production rates required for a successful mission. Consequently, the acquisition, purification, and storage of these buffer gases are important goals of ISRU plans. Purity of the buffer gases is a concern e.g., if the CO, freezer operates at 140 K, the composition of the inert gas would be approximately 21 percent CO2, 50 percent nitrogen, and 29 percent argon. Although there are several approaches that could be used, this effort focused on a hollow-fiber membrane (HFM) separation method. This study measured the permeation rates of CO2, nitrogen (ND, and argon (Ar) through a multiple-membrane system and the individual membranes from room temperature to 193K and 10 kpa to 300 kPa. Concentrations were measured with a gas chromatograph that used a thermoconductivity (TCD) detector with helium (He) as the carrier gas. The general trend as the temperature was lowered was for the membranes to become more selective, In addition, the relative permeation rates between the three gases changed with temperature. The end result was to provide design parameters that could be used to separate CO2 from N2 and Ar.

  7. The influence of CdS intermediate layer on CdSe/CdS co-sensitized free-standing TiO2 nanotube solar cells

    NASA Astrophysics Data System (ADS)

    Ren, Xuefeng; Yu, Libo; Li, Zhen; Song, Hai; Wang, Qingyun

    2018-01-01

    We build CdSe quantum dots (QDs) sensitized TiO2 NT solar cells (CdSe/TiO2 solar cells) by successive ionic layer adsorption reaction (SILAR) method on free-standing translucent TiO2 nanotube (NT) film. The best power conversion efficiency (PCE) 0.74% is obtained with CdSe/TiO2 NT solar cells, however, it is very low. Hence, we introduced the CdS QDs layer located between CdSe QDs and TiO2 NT to achieve an enhanced photovoltaic performance. The J-V test results indicated that the insert of CdS intermediate layer yield a significant improvement of PCE to 2.52%. Combining experimental and theoretical analysis, we find that the effects caused by a translucent TiO2 nanotube film, a better lattices match between CdS and TiO2, and a new formed stepwise band edges structure not only improve the light harvesting efficiency but also increase the driving force of electrons, leading to the improvement of photovoltaic performance.

  8. Laboratory Kinetic Studies of OH and CO2 Relevant to Upper Atmospheric Radiation Balance

    NASA Technical Reports Server (NTRS)

    Nelson, David D.; Villalta, Peter; Zahniser, Mark S.; Kolb, Charles E.

    1997-01-01

    The purpose of this project was to quantify the rates of two processes which are crucial to our understanding of radiative energy balance in the upper atmosphere. The first process is radiative emission from vibrationally hot OH radicals following the H + O3 reaction in the upper mesosphere. The importance of this process depends strongly on the OH radiative emission coefficients. Our goal was to measure the OH permanent dipole moment in excited vibrational states and to use these measurements to construct an improved OH dipole moment function and improved radiative emission coefficients. Significant progress was made on these experiments including the construction of a supersonic jet source for vibrationally excited OH radicals. Unfortunately, our efforts to transport the OH radicals into a second lower pressure vacuum chamber were not successful, and we were unable to make improved dipole moment measurements for OH. The second key kinetic process which we attempted to quantify during this project is the rate of relaxation of bend-excited CO2 by oxygen atoms. Since excitation of the bending vibrational mode of CO2 is the major cooling mechanism in the upper mesosphere/lower thermosphere, the cooling rate of this region depends crucially on the rate of energy transfer out of this state. It is believed that the most efficient transfer mechanism is via atomic oxygen but the rate for this process has not been directly measured in the laboratory at appropriate temperatures and even the room temperature rate remains controversial. We attempted to directly measure the relaxation rate Of CO2 (010) by oxygen atoms using the discharge flow technique. This experiment was set up at Aerodyne Research. Again, significant progress was achieved in this experiment. A hot CO2 source was set up, bend excited CO2 was detected and the rate of relaxation of bend excited CO2 by He atoms was measured. Unfortunately, the project ran out of time before the oxygen atom kinetic studies could be implemented.

  9. Cyanobacterial-based approaches to improving photosynthesis in plants.

    PubMed

    Zarzycki, Jan; Axen, Seth D; Kinney, James N; Kerfeld, Cheryl A

    2013-01-01

    Plants rely on the Calvin-Benson (CB) cycle for CO(2) fixation. The key carboxylase of the CB cycle is ribulose-1,5-bisphosphate carboxylase/oxygenase (RubisCO). Efforts to enhance carbon fixation in plants have traditionally focused on RubisCO or on approaches that can help to remedy RubisCO's undesirable traits: its low catalytic efficiency and photorespiration. Towards reaching the goal of improving plant photosynthesis, cyanobacteria may be instrumental. Because of their evolutionary relationship to chloroplasts, they represent ideal model organisms for photosynthesis research. Furthermore, the molecular understanding of cyanobacterial carbon fixation provides a rich source of strategies that can be exploited for the bioengineering of chloroplasts. These strategies include the cyanobacterial carbon concentrating mechanism (CCM), which consists of active and passive transporter systems for inorganic carbon and a specialized organelle, the carboxysome. The carboxysome encapsulates RubisCO together with carbonic anhydrase in a protein shell, resulting in an elevated CO(2) concentration around RubisCO. Moreover, cyanobacteria differ from plants in the isoenzymes involved in the CB cycle and the photorespiratory pathways as well as in mechanisms that can affect the activity of RubisCO. In addition, newly available cyanobacterial genome sequence data from the CyanoGEBA project, which has more than doubled the amount of genomic information available for cyanobacteria, increases our knowledge on the CCM and the occurrence and distribution of genes of interest.

  10. Design of experimental setup for supercritical CO2 jet under high ambient pressure conditions

    NASA Astrophysics Data System (ADS)

    Shi, Huaizhong; Li, Gensheng; He, Zhenguo; Wang, Haizhu; Zhang, Shikun

    2016-12-01

    With the commercial extraction of hydrocarbons in shale and tight reservoirs, efficient methods are needed to accelerate developing process. Supercritical CO2 (SC-CO2) jet has been considered as a potential way due to its unique fluid properties. In this article, a new setup is designed for laboratory experiment to research the SC-CO2 jet's characteristics in different jet temperatures, pressures, standoff distances, ambient pressures, etc. The setup is composed of five modules, including SC-CO2 generation system, pure SC-CO2 jet system, abrasive SC-CO2 jet system, CO2 recovery system, and data acquisition system. Now, a series of rock perforating (or case cutting) experiments have been successfully conducted using the setup about pure and abrasive SC-CO2 jet, and the results have proven the great perforating efficiency of SC-CO2 jet and the applications of this setup.

  11. Design of experimental setup for supercritical CO2 jet under high ambient pressure conditions.

    PubMed

    Shi, Huaizhong; Li, Gensheng; He, Zhenguo; Wang, Haizhu; Zhang, Shikun

    2016-12-01

    With the commercial extraction of hydrocarbons in shale and tight reservoirs, efficient methods are needed to accelerate developing process. Supercritical CO 2 (SC-CO 2 ) jet has been considered as a potential way due to its unique fluid properties. In this article, a new setup is designed for laboratory experiment to research the SC-CO 2 jet's characteristics in different jet temperatures, pressures, standoff distances, ambient pressures, etc. The setup is composed of five modules, including SC-CO 2 generation system, pure SC-CO 2 jet system, abrasive SC-CO 2 jet system, CO 2 recovery system, and data acquisition system. Now, a series of rock perforating (or case cutting) experiments have been successfully conducted using the setup about pure and abrasive SC-CO 2 jet, and the results have proven the great perforating efficiency of SC-CO 2 jet and the applications of this setup.

  12. Mitigation of power sector environmental emissions through energy efficiency improvements: The case of Pakistan

    DOE Office of Scientific and Technical Information (OSTI.GOV)

    Shrestha, R.M.; Biswas, W.K.; Jalal, A.I.

    1998-11-01

    This paper assesses the potential of selected efficient electrical appliances for avoiding power generation and for mitigation of selected air pollutants from the power sector in Pakistan from technical as well as national, utility and user perspectives. The study shows that about 14, 21 and 35% of the total CO{sub 2}, SO{sub 2} and NO{sub x} emissions in the business as usual (BAU) case could be avoided by the adoption of selected efficient appliances during 1997--2015 from the national perspective, while the corresponding figures from the user perspective are 12, 17 and 29%, respectively. All selected efficient appliances would bemore » cost effective to the users if electricity prices were set at the long-run marginal cost of supply.« less

  13. Engineering chloroplasts to improve Rubisco catalysis: prospects for translating improvements into food and fiber crops.

    PubMed

    Sharwood, Robert E

    2017-01-01

    494 I. 495 II. 496 III. 496 IV. 499 V. 499 VI. 501 VII. 501 VIII. 502 IX. 505 X. 506 507 References 507 SUMMARY: The uncertainty of future climate change is placing pressure on cropping systems to continue to provide stable increases in productive yields. To mitigate future climates and the increasing threats against global food security, new solutions to manipulate photosynthesis are required. This review explores the current efforts available to improve carbon assimilation within plant chloroplasts by engineering Rubisco, which catalyzes the rate-limiting step of CO 2 fixation. Fixation of CO 2 and subsequent cycling of 3-phosphoglycerate through the Calvin cycle provides the necessary carbohydrate building blocks for maintaining plant growth and yield, but has to compete with Rubisco oxygenation, which results in photorespiration that is energetically wasteful for plants. Engineering improvements in Rubisco is a complex challenge and requires an understanding of chloroplast gene regulatory pathways, and the intricate nature of Rubisco catalysis and biogenesis, to transplant more efficient forms of Rubisco into crops. In recent times, major advances in Rubisco engineering have been achieved through improvement of our knowledge of Rubisco synthesis and assembly, and identifying amino acid catalytic switches in the L-subunit responsible for improvements in catalysis. Improving the capacity of CO 2 fixation in crops such as rice will require further advances in chloroplast bioengineering and Rubisco biogenesis. © 2016 The Author. New Phytologist © 2016 New Phytologist Trust.

  14. Electrolytes Based on TEMPO–Co Tandem Redox Systems Outperform Single Redox Systems in Dye‐sensitized Solar Cells

    PubMed Central

    Cong, Jiayan; Hao, Yan; Boschloo, Gerrit

    2014-01-01

    Abstract A new TEMPO–Co tandem redox system with TEMPO and Co(bpy)3 2+/3+ has been investigated for the use in dye‐sensitized solar cells (DSSCs). A large open‐circuit voltage (V OC) increase, from 862 mV to 965 mV, was observed in the tandem redox system, while the short‐circuit current density (J SC) was maintained. The conversion efficiency was observed to increase from 7.1 % for cells containing the single Co(bpy)3 2+/3+ redox couple, to 8.4 % for cells containing the TEMPO–Co tandem redox system. The reason for the increase in V OC and overall efficiency is ascribed to the involvement of partial regeneration of the sensitizing dye molecules by TEMPO. This assumption can be verified through the observed much faster regeneration dynamics exhibited in the presence of the tandem system. Using the tandem redox system, the faster recombination problem of the single TEMPO redox couple is resolved and the mass‐transport of the metal‐complex‐based electrolyte is also improved. This TEMPO–Co tandem system is so far the most effienct tandem redox electrolyte reported not involving iodine. The current results show a promising future for tandem system as replacements for single redox systems in electrolytes for DSSCs. PMID:25504818

  15. Ocean acidification of a coastal Antarctic marine microbial community reveals a critical threshold for CO2 tolerance in phytoplankton productivity

    NASA Astrophysics Data System (ADS)

    Deppeler, Stacy; Petrou, Katherina; Schulz, Kai G.; Westwood, Karen; Pearce, Imojen; McKinlay, John; Davidson, Andrew

    2018-01-01

    High-latitude oceans are anticipated to be some of the first regions affected by ocean acidification. Despite this, the effect of ocean acidification on natural communities of Antarctic marine microbes is still not well understood. In this study we exposed an early spring, coastal marine microbial community in Prydz Bay to CO2 levels ranging from ambient (343 µatm) to 1641 µatm in six 650 L minicosms. Productivity assays were performed to identify whether a CO2 threshold existed that led to a change in primary productivity, bacterial productivity, and the accumulation of chlorophyll a (Chl a) and particulate organic matter (POM) in the minicosms. In addition, photophysiological measurements were performed to identify possible mechanisms driving changes in the phytoplankton community. A critical threshold for tolerance to ocean acidification was identified in the phytoplankton community between 953 and 1140 µatm. CO2 levels ≥ 1140 µatm negatively affected photosynthetic performance and Chl a-normalised primary productivity (csGPP14C), causing significant reductions in gross primary production (GPP14C), Chl a accumulation, nutrient uptake, and POM production. However, there was no effect of CO2 on C : N ratios. Over time, the phytoplankton community acclimated to high CO2 conditions, showing a down-regulation of carbon concentrating mechanisms (CCMs) and likely adjusting other intracellular processes. Bacterial abundance initially increased in CO2 treatments ≥ 953 µatm (days 3-5), yet gross bacterial production (GBP14C) remained unchanged and cell-specific bacterial productivity (csBP14C) was reduced. Towards the end of the experiment, GBP14C and csBP14C markedly increased across all treatments regardless of CO2 availability. This coincided with increased organic matter availability (POC and PON) combined with improved efficiency of carbon uptake. Changes in phytoplankton community production could have negative effects on the Antarctic food web and the biological pump, resulting in negative feedbacks on anthropogenic CO2 uptake. Increases in bacterial abundance under high CO2 conditions may also increase the efficiency of the microbial loop, resulting in increased organic matter remineralisation and further declines in carbon sequestration.

  16. Efficiency of radial transport of ices in protoplanetary disks probed with infrared observations: the case of CO2

    NASA Astrophysics Data System (ADS)

    Bosman, Arthur D.; Tielens, Alexander G. G. M.; van Dishoeck, Ewine F.

    2018-04-01

    Context. Radial transport of icy solid material from the cold outer disk to the warm inner disk is thought to be important for planet formation. However, the efficiency at which this happens is currently unconstrained. Efficient radial transport of icy dust grains could significantly alter the composition of the gas in the inner disk, enhancing the gas-phase abundances of the major ice constituents such as H2O and CO2. Aim. Our aim is to model the gaseous CO2 abundance in the inner disk and use this to probe the efficiency of icy dust transport in a viscous disk. From the model predictions, infrared CO2 spectra are simulated and features that could be tracers of icy CO2, and thus dust, radial transport efficiency are investigated. Methods: We have developed a 1D viscous disk model that includes gas accretion and gas diffusion as well as a description for grain growth and grain transport. Sublimation and freeze-out of CO2 and H2O has been included as well as a parametrisation of the CO2 chemistry. The thermo-chemical code DALI was used to model the mid-infrared spectrum of CO2, as can be observed with JWST-MIRI. Results: CO2 ice sublimating at the iceline increases the gaseous CO2 abundance to levels equal to the CO2 ice abundance of 10-5, which is three orders of magnitude more than the gaseous CO2 abundances of 10-8 observed by Spitzer. Grain growth and radial drift increase the rate at which CO2 is transported over the iceline and thus the gaseous CO2 abundance, further exacerbating the problem. In the case without radial drift, a CO2 destruction rate of at least 10-11 s-1 or a destruction timescale of at most 1000 yr is needed to reconcile model prediction with observations. This rate is at least two orders of magnitude higher than the fastest destruction rate included in chemical databases. A range of potential physical mechanisms to explain the low observed CO2 abundances are discussed. Conclusions: We conclude that transport processes in disks can have profound effects on the abundances of species in the inner disk such as CO2. The discrepancy between our model and observations either suggests frequent shocks in the inner 10 AU that destroy CO2, or that the abundant midplane CO2 is hidden from our view by an optically thick column of low abundance CO2 due to strong UV and/or X-rays in the surface layers. Modelling and observations of other molecules, such as CH4 or NH3, can give further handles on the rate of mass transport.

  17. Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper.

    PubMed

    Li, Christina W; Ciston, Jim; Kanan, Matthew W

    2014-04-24

    The electrochemical conversion of CO2 and H2O into liquid fuel is ideal for high-density renewable energy storage and could provide an incentive for CO2 capture. However, efficient electrocatalysts for reducing CO2 and its derivatives into a desirable fuel are not available at present. Although many catalysts can reduce CO2 to carbon monoxide (CO), liquid fuel synthesis requires that CO is reduced further, using H2O as a H(+) source. Copper (Cu) is the only known material with an appreciable CO electroreduction activity, but in bulk form its efficiency and selectivity for liquid fuel are far too low for practical use. In particular, H2O reduction to H2 outcompetes CO reduction on Cu electrodes unless extreme overpotentials are applied, at which point gaseous hydrocarbons are the major CO reduction products. Here we show that nanocrystalline Cu prepared from Cu2O ('oxide-derived Cu') produces multi-carbon oxygenates (ethanol, acetate and n-propanol) with up to 57% Faraday efficiency at modest potentials (-0.25 volts to -0.5 volts versus the reversible hydrogen electrode) in CO-saturated alkaline H2O. By comparison, when prepared by traditional vapour condensation, Cu nanoparticles with an average crystallite size similar to that of oxide-derived copper produce nearly exclusive H2 (96% Faraday efficiency) under identical conditions. Our results demonstrate the ability to change the intrinsic catalytic properties of Cu for this notoriously difficult reaction by growing interconnected nanocrystallites from the constrained environment of an oxide lattice. The selectivity for oxygenates, with ethanol as the major product, demonstrates the feasibility of a two-step conversion of CO2 to liquid fuel that could be powered by renewable electricity.

  18. Rechargeable Al-CO2 Batteries for Reversible Utilization of CO2.

    PubMed

    Ma, Wenqing; Liu, Xizheng; Li, Chao; Yin, Huiming; Xi, Wei; Liu, Ruirui; He, Guang; Zhao, Xian; Luo, Jun; Ding, Yi

    2018-05-21

    The excessive emission of CO 2 and the energy crisis are two major issues facing humanity. Thus, the electrochemical reduction of CO 2 and its utilization in metal-CO 2 batteries have attracted wide attention because the batteries can simultaneously accelerate CO 2 fixation/utilization and energy storage/release. Here, rechargeable Al-CO 2 batteries are proposed and realized, which use chemically stable Al as the anode. The batteries display small discharge/charge voltage gaps down to 0.091 V and high energy efficiencies up to 87.7%, indicating an efficient battery performance. Their chemical reaction mechanism to produce the performance is revealed to be 4Al + 9CO 2 ↔ 2Al 2 (CO 3 ) 3 + 3C, by which CO 2 is reversibly utilized. These batteries are envisaged to effectively and safely serve as a potential CO 2 fixation/utilization strategy with stable Al. © 2018 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  19. Magnetic Resonance Imaging-Guided Multi-Drug Chemotherapy and Photothermal Synergistic Therapy with pH and NIR-Stimulation Release.

    PubMed

    Yang, Ji-Chun; Chen, Yang; Li, Yu-Hao; Yin, Xue-Bo

    2017-07-12

    The combination of multidrug chemotherapy and photothermal therapy (PTT) enhances cancer therapeutic efficacy. Herein, we develop a simple and smart pH/NIR dual-stimulus-responsive degradable mesoporous CoFe 2 O 4 @PDA@ZIF-8 sandwich nanocomposite. The mesoporous CoFe 2 O 4 core acts as T 2 -weighted magnetic resonance (MR) imaging probe, PTT agent, and loading platform of hydrophilic doxorubicin (DOX). A polydopamine (PDA) layer is used to avoid the premature leakage of DOX before arriving at tumor site, enhance PTT efficiency, and facilitate the integration of ZIF-8 (a kind of metal-organic framework). The ZIF-8 shell serves to encapsulate hydrophobic camptothecin (CPT) and as the switch for the pH and NIR stimulation-responsive release of the two drugs. Therefore, T 2 -weighted MR imaging-guided multidrug chemotherapy and PTT synergistic treatment is achieved. Two kinds of anticancer drugs, hydrophilic DOX and hydrophobic CPT, are successfully loaded in CoFe 2 O 4 and ZIF-8, respectively, so no mutual interference between the two drugs exists. A unique two-stage stepwise release process is exhibited for CPT and DOX with an interval of 12 h to improve the anticancer efficacy under the acidic microenvironment of tumor tissue. NIR irradiation achieves the burst drug-release and PTT after laser stimulation, simultaneously. With this smart design, high drug concentration is achieved at the tumor site by quick release, especially for the therapeutic drugs that show nonlinear pharmacokinetics, and PTT is integrated efficiently. Furthermore, negligible biotoxicity and a remarkable synergic antitumor effect of the hybrid nanocomposites are validated by HepG2 cells and tumor-bearing mice as models. Our multidrug delivery-releasing composite improves tumor therapeutic efficiency significantly compared with a single-drug chemotherapy system. The simple multifunctional composite system can be applied as an effective platform for personal nanomedicine with diagnosis, smart drug delivery, and cancer treatment through its remarkable photothermal property and controllable multidrug release.

  20. Down-shifting in Ce3+-Tb3+ co-doped SiO2-LaF3 nano-glass-ceramics for photon conversion in solar cells

    NASA Astrophysics Data System (ADS)

    Velázquez, J. J.; Rodríguez, V. D.; Yanes, A. C.; del-Castillo, J.; Méndez-Ramos, J.

    2012-10-01

    95SiO2-5LaF3 sol-gel derived nano-glass-ceramics single doped with Ce3+ or Tb3+ and co-doped with Ce3+-Tb3+ were synthesized by thermal treatment of precursor glasses. Precipitation of LaF3 nanocrystals during ceramming process was confirmed by X-ray diffraction with mean size ranging from 12 to 15 nm. An exhaustive spectroscopic analysis has been carried out. As a result, it was found that the green emission of Tb3+ ions was greatly enhanced through down shifting process, due to efficient energy transfer from Ce3+ to Tb3+ ions in the glass-ceramics, which is favored by the reduction of the interionic distances when the dopant ions are partitioned into LaF3 nanocrystals. These results suggest the use of these materials to improve the efficiency of solar cells.

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