Energy of the Isolated Metastable Iron-Nickel FCC Nanocluster with a Carbon Atom in the Tetragonal Interstice.

PubMed

Bondarenko, Natalya V; Nedolya, Anatoliy V

2017-12-01

The energy of the isolated iron-nickel nanocluster was calculated by molecular mechanics method using Lennard-Jones potential. The cluster included a carbon atom that drifted from an inside octahedral interstice to a tetrahedral interstice in [Formula: see text] direction and after that in <222> direction to the surface. In addition, one of 14 iron atoms was replaced by a nickel atom, the position of which was changing during simulation.The energy of the nanocluster was estimated at the different interatomic distances. As a result of simulation, the optimal interatomic distances of Fe-Ni-C nanocluster was chosen for the simulation, in which height of the potential barrier was maximal and face-centered cubic (FCC) nanocluster was the most stable.It is shown that there were three main positions of a nickel atom that significantly affected nanocluster's energy.The calculation results indicated that position of the carbon atom in the octahedral interstice was more energetically favorable than tetrahedral interstice in the case of FCC nanocluster. On the other side, the potential barrier was smaller in the direction [Formula: see text] than in the direction <022>.This indicates that there are two ways for carbon atom to drift to the surface of the nanocluster.

Voronoi analysis of the short–range atomic structure in iron and iron–carbon melts

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

Sobolev, Andrey; Mirzoev, Alexander

2015-08-17

In this work, we simulated the atomic structure of liquid iron and iron–carbon alloys by means of ab initio molecular dynamics. Voronoi analysis was used to highlight changes in the close environments of Fe atoms as carbon concentration in the melt increases. We have found, that even high concentrations of carbon do not affect short–range atomic order of iron atoms — it remains effectively the same as in pure iron melts.

Tailoring Thermal Conductivity of Single-stranded Carbon-chain Polymers through Atomic Mass Modification

PubMed Central

Liao, Quanwen; Zeng, Lingping; Liu, Zhichun; Liu, Wei

2016-01-01

Tailoring the thermal conductivity of polymers is central to enlarge their applications in the thermal management of flexible integrated circuits. Progress has been made over the past decade by fabricating materials with various nanostructures, but a clear relationship between various functional groups and thermal properties of polymers remains to be established. Here, we numerically study the thermal conductivity of single-stranded carbon-chain polymers with multiple substituents of hydrogen atoms through atomic mass modification. We find that their thermal conductivity can be tuned by atomic mass modifications as revealed through molecular dynamics simulations. The simulation results suggest that heavy homogeneous substituents do not assist heat transport and trace amounts of heavy substituents can in fact hinder heat transport substantially. Our analysis indicates that carbon chain has the biggest contribution (over 80%) to the thermal conduction in single-stranded carbon-chain polymers. We further demonstrate that atomic mass modifications influence the phonon bands of bonding carbon atoms, and the discrepancies of phonon bands between carbon atoms are responsible for the remarkable drops in thermal conductivity and large thermal resistances in carbon chains. Our study provides fundamental insight into how to tailor the thermal conductivity of polymers through variable substituents. PMID:27713563

Earthquake dating: an application of carbon-14 atom counting.

PubMed

Tucker, A B; Woefli, W; Bonani, G; Suter, M

1983-03-18

Milligram-sized specimens of detrital charcoal from soil layers associated with prehistoric earthquakes on the Wasatch fault in Utah have been dated by direct atom counting of carbon-14 with a tandem Van de Graaff accelerator. The measured ratios of carbon-14 to carbon-12 correspond to ages of 7800, 8800, and 9000 years with uncertainties of +/- 600 years.

Carbon concentration measurements by atom probe tomography in the ferritic phase of high-silicon steels

DOE PAGES

Rementeria, Rosalia; Poplawsky, Jonathan D.; Aranda, Maria M.; ...

2016-12-19

Current studies using atom probe tomography (APT) show that bainitic ferrite formed at low temperature contains more carbon than what is consistent with the paraequilibrium phase diagram. However, nanocrystalline bainitic ferrite exhibits a non-homogeneous distribution of carbon atoms in arrangements with specific compositions, i.e. Cottrell atmospheres, carbon clusters, and carbides, in most cases with a size of a few nanometers. The ferrite volume within a single platelet that is free of these carbon-enriched regions is extremely small. Proximity histograms can be compromised on the ferrite side, and a great deal of care should be taken to estimate the carbon contentmore » in regions of bainitic ferrite free from carbon agglomeration. For this purpose, APT measurements were first validated for the ferritic phase in a pearlitic sample and further performed for the bainitic ferrite matrix in high-silicon steels isothermally transformed between 200 °C and 350 °C. Additionally, results were compared with the carbon concentration values derived from X-ray diffraction (XRD) analyses considering a tetragonal lattice and previous APT studies. In conclusion, the present results reveal a strong disagreement between the carbon content values in the bainitic ferrite matrix as obtained by APT and those derived from XRD measurements. Those differences have been attributed to the development of carbon-clustered regions with an increased tetragonality in a carbon-depleted matrix.« less

Coke formation and carbon atom economy of methanol-to-olefins reaction.

PubMed

Wei, Yingxu; Yuan, Cuiyu; Li, Jinzhe; Xu, Shutao; Zhou, You; Chen, Jingrun; Wang, Quanyi; Xu, Lei; Qi, Yue; Zhang, Qing; Liu, Zhongmin

2012-05-01

The methanol-to-olefins (MTO) process is becoming the most important non-petrochemical route for the production of light olefins from coal or natural gas. Maximizing the generation of the target products, ethene and propene, and minimizing the production of byproducts and coke, are major considerations in the efficient utilization of the carbon resource of methanol. In the present work, the heterogeneous catalytic conversion of methanol was evaluated by performing simultaneous measurements of the volatile products generated in the gas phase and the confined coke deposition in the catalyst phase. Real-time and complete reaction profiles were plotted to allow the comparison of carbon atom economy of methanol conversion over the catalyst SAPO-34 at varied reaction temperatures. The difference in carbon atom economy was closely related with the coke formation in the SAPO-34 catalyst. The confined coke compounds were determined. A new type of confined organics was found, and these accounted for the quick deactivation and low carbon atom economy under low-reaction-temperature conditions. Based on the carbon atom economy evaluation and coke species determination, optimized operating conditions for the MTO process are suggested; these conditions guarantee high conversion efficiency of methanol. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Carbon fiber CVD coating by carbon nanostructured for space materials protection against atomic oxygen

NASA Astrophysics Data System (ADS)

Pastore, Roberto; Bueno Morles, Ramon; Micheli, Davide

2016-07-01

adhesion and durability in the environment. Though these coatings are efficient in protecting polymer composites, their application imposes severe constraints. Their thermal expansion coefficients may differ markedly from those of polymer composite substrates: as a result, cracks develop in the coatings on thermal cycling and AO can penetrate through them to the substrate. In addition to the technicalities of forming an effective barrier, such factors as cost, convenience of application and ease of repair are important considerations in the selection of a coating for a particular application. The latter issues drive the aerospace research toward the development of novel light composite materials, like the so called polymer nanocomposites, which are materials with a polymer matrix and a filler with at least one dimension less than 100 nanometers. Current interest in nanocomposites has been generated and maintained because nanoparticle-filled polymers exhibit unique combinations of properties not achievable with traditional composites. These combinations of properties can be achieved because of the small size of the fillers, the large surface area the fillers provide, and in many cases the unique properties of the fillers themselves. In particular, the carbon fiber-based polymeric composite materials are the basic point of interest: the aim of the present study is to find new solution to produce carbon fiber-based composites with even more upgraded performances. One intriguing strategy to tackle such an issue has been picked out in the coupling between the carbon fibers and the carbon nanostructures. That for two main reasons: first, carbon nanostructures have shown fancy potentialities for any kind of technological applications since their discovery, second, the chemical affinity between fiber and nanostructure (made of the same element) should be a likely route to approach the typical problems due to thermo-mechanical compatibility. This work is joined in such framework

Carbon Nanotube Devices Engineered by Atomic Force Microscopy

NASA Astrophysics Data System (ADS)

Prisbrey, Landon

This dissertation explores the engineering of carbon nanotube electronic devices using atomic force microscopy (AFM) based techniques. A possible application for such devices is an electronic interface with individual biological molecules. This single molecule biosensing application is explored both experimentally and with computational modeling. Scanning probe microscopy techniques, such as AFM, are ideal to study nanoscale electronics. These techniques employ a probe which is raster scanned above a sample while measuring probe-surface interactions as a function of position. In addition to topographical and electrostatic/magnetic surface characterization, the probe may also be used as a tool to manipulate and engineer at the nanoscale. Nanoelectronic devices built from carbon nanotubes exhibit many exciting properties including one-dimensional electron transport. A natural consequence of onedimensional transport is that a single perturbation along the conduction channel can have extremely large effects on the device's transport characteristics. This property may be exploited to produce electronic sensors with single-molecule resolution. Here we use AFM-based engineering to fabricate atomic-sized transistors from carbon nanotube network devices. This is done through the incorporation of point defects into the carbon nanotube sidewall using voltage pulses from an AFM probe. We find that the incorporation of an oxidative defect leads to a variety of possible electrical signatures including sudden switching events, resonant scattering, and breaking of the symmetry between electron and hole transport. We discuss the relationship between these different electronic signatures and the chemical structure/charge state of the defect. Tunneling through a defect-induced Coulomb barrier is modeled with numerical Verlet integration of Schrodinger's equation and compared with experimental results. Atomic-sized transistors are ideal for single-molecule applications due to their

A Molecular Dynamics of Cold Neutral Atoms Captured by Carbon Nanotube Under Electric Field and Thermal Effect as a Selective Atoms Sensor.

PubMed

Santos, Elson C; Neto, Abel F G; Maneschy, Carlos E; Chen, James; Ramalho, Teodorico C; Neto, A M J C

2015-05-01

Here we analyzed several physical behaviors through computational simulation of systems consisting of a zig-zag type carbon nanotube and relaxed cold atoms (Rb, Au, Si and Ar). These atoms were chosen due to their different chemical properties. The atoms individually were relaxed on the outside of the nanotube during the simulations. Each system was found under the influence of a uniform electric field parallel to the carbon nanotube and under the thermal effect of the initial temperature at the simulations. Because of the electric field, the cold atoms orbited the carbon nanotube while increasing the initial temperature allowed the variation of the radius of the orbiting atoms. We calculated the following quantities: kinetic energy, potential energy and total energy and in situ temperature, molar entropy variation and average radius of the orbit of the atoms. Our data suggest that only the action of electric field is enough to generate the attractive potential and this system could be used as a selected atoms sensor.

Simple method for determination of selenium in biological materials by flameless atomic-absorption spectrometry using a carbon-tube atomizer.

PubMed

Ishizaki, M

1978-03-01

A method for determination of selenium in biological materials by flameless atomic-absorption spectrometry using a carbon-tube atomizer is described. The sample is burned by an oxygen-flask combustion procedure, the resulting solution is treated with a cation-exchange resin to eliminate interfering cations, the selenium is extracted with dithizone in carbon tetrachloride and the resulting selenium dithizonate is combined with nickel nitrate in the carbon tube to enhance the sensitivity for selenium and avoid volatilization losses. The method measures selenium concentrations as low as 0.01 mug/g with a relative standard deviation of 8%.

Atomic layer confined vacancies for atomic-level insights into carbon dioxide electroreduction

NASA Astrophysics Data System (ADS)

Gao, Shan; Sun, Zhongti; Liu, Wei; Jiao, Xingchen; Zu, Xiaolong; Hu, Qitao; Sun, Yongfu; Yao, Tao; Zhang, Wenhua; Wei, Shiqiang; Xie, Yi

2017-02-01

The role of oxygen vacancies in carbon dioxide electroreduction remains somewhat unclear. Here we construct a model of oxygen vacancies confined in atomic layer, taking the synthetic oxygen-deficient cobalt oxide single-unit-cell layers as an example. Density functional theory calculations demonstrate the main defect is the oxygen(II) vacancy, while X-ray absorption fine structure spectroscopy reveals their distinct oxygen vacancy concentrations. Proton transfer is theoretically/experimentally demonstrated to be a rate-limiting step, while energy calculations unveil that the presence of oxygen(II) vacancies lower the rate-limiting activation barrier from 0.51 to 0.40 eV via stabilizing the formate anion radical intermediate, confirmed by the lowered onset potential from 0.81 to 0.78 V and decreased Tafel slope from 48 to 37 mV dec-1. Hence, vacancy-rich cobalt oxide single-unit-cell layers exhibit current densities of 2.7 mA cm-2 with ca. 85% formate selectivity during 40-h tests. This work establishes a clear atomic-level correlation between oxygen vacancies and carbon dioxide electroreduction.

Comparison of carbon onions and carbon blacks as conductive additives for carbon supercapacitors in organic electrolytes

NASA Astrophysics Data System (ADS)

Jäckel, N.; Weingarth, D.; Zeiger, M.; Aslan, M.; Grobelsek, I.; Presser, V.

2014-12-01

This study investigates carbon onions (∼400 m2 g-1) as a conductive additive for supercapacitor electrodes of activated carbon and compares their performance with carbon black with high or low internal surface area. We provide a study of the electrical conductivity and electrochemical behavior between 2.5 and 20 mass% addition of each of these three additives to activated carbon. Structural characterization shows that the density of the resulting film electrodes depends on the degree of agglomeration and the amount of additive. Addition of low surface area carbon black (∼80 m2 g-1) enhances the power handling of carbon electrodes but significantly lowers the specific capacitance even when adding small amounts of carbon black. A much lower decrease in specific capacitance is observed for carbon onions and the best values are seen for carbon black with a high surface area (∼1390 m2 g-1). The overall performance benefits from the addition of any of the studied additives only at either high scan rates and/or electrolytes with high ion mobility. Normalization to the volume shows a severe decrease in volumetric capacitance and only at high current densities nearing 10 A g-1 we can see an improvement of the electrode capacitance.

Atomic carbon emission from photodissociation of CO2. [planetary atmospheric chemistry

NASA Technical Reports Server (NTRS)

Wu, C. Y. R.; Phillips, E.; Lee, L. C.; Judge, D. L.

1978-01-01

Atomic carbon fluorescence, C I 1561, 1657, and 1931 A, has been observed from photodissociation of CO2, and the production cross sections have been measured. A line emission source provided the primary photons at wavelengths from threshold to 420 A. The present results suggest that the excited carbon atoms are produced by total dissociation of CO2 into three atoms. The cross sections for producing the O I 1304-A fluorescence through photodissociation of CO2 are found to be less than 0.01 Mb in the wavelength region from 420 to 835 A. The present data have implications with respect to photochemical processes in the atmospheres of Mars and Venus.

Molybdenum and carbon atom and carbon cluster sputtering under low-energy noble gas plasma bombardment

NASA Astrophysics Data System (ADS)

Oyarzabal, Eider

Exit-angle resolved Mo atom sputtering yield under Xe ion bombardment and carbon atom and cluster (C2 and C3) sputtering yields under Xe, Kr, Ar, Ne and He ion bombardment from a plasma are measured for low incident energies (75--225 eV). An energy-resolved quadrupole mass spectrometer (QMS) is used to detect the fraction of un-scattered sputtered neutrals that become ionized in the plasma; the angular distribution is obtained by changing the angle between the target and the QMS aperture. A one-dimensional Monte Carlo code is used to simulate the interaction of the plasma and the sputtered particles between the sample and the QMS. The elastic scattering cross-sections of C, C2 and C3 with the different bombarding gas neutrals is obtained by varying the distance between the sample and the QMS and by performing a best fit of the simulation results to the experimental results. Because the results obtained with the QMS are relative, the Mo atom sputtering results are normalized to the existing data in the literature and the total sputtering yield for carbon (C+C 2+C3) for each bombarding gas is obtained from weight loss measurements. The absolute sputtering yield for C, C2 and C 3 is then calculated from the integration of the measured angular distribution, taking into account the scattering and ionization of the sputtered particles between the sample and the QMS. The angular sputtering distribution for Mo has a maximum at theta=60°, and this maximum becomes less pronounced as the incident ion energy increases. The results of the Monte Carlo TRIDYN code simulation for the angular distribution of Mo atoms sputtered by Xe bombardment are in agreement with the experiments. For carbon sputtering under-cosine angular distributions of the sputtered atoms and clusters for all the studied bombarding gases are also observed. The C, C2 and C3 sputtering yield data shows a clear decrease of the atom to cluster (C/C2 and C/C3) sputtering ratio as the incident ion mass increases

Understanding the detection of carbon in austenitic high-Mn steel using atom probe tomography.

PubMed

Marceau, R K W; Choi, P; Raabe, D

2013-09-01

A high-Mn TWIP steel having composition Fe-22Mn-0.6C (wt%) is considered in this study, where the need for accurate and quantitative analysis of clustering and short-range ordering by atom probe analysis requires a better understanding of the detection of carbon in this system. Experimental measurements reveal that a high percentage of carbon atoms are detected as molecular ion species and on multiple hit events, which is discussed with respect to issues such as optimal experimental parameters, correlated field evaporation and directional walk/migration of carbon atoms at the surface of the specimen tip during analysis. These phenomena impact the compositional and spatial accuracy of the atom probe measurement and thus require careful consideration for further cluster-finding analysis. Copyright © 2013 Elsevier B.V. All rights reserved.

Spatial Distributions of Metal Atoms During Carbon SWNTs Formation: Measurements and Modelling

NASA Technical Reports Server (NTRS)

Cau, M.; Dorval, N.; Attal-Tretout, B.; Cochon, J. L.; Loiseau, A.; Farhat, S.; Hinkov, I.; Scott, C. D.

2004-01-01

Experiments and modelling have been undertaken to clarify the role of metal catalysts during single-wall carbon nanotube formation. For instance, we wonder whether the metal catalyst is active as an atom, a cluster, a liquid or solid nanoparticle [1]. A reactor has been developed for synthesis by continuous CO2-laser vaporisation of a carbon-nickel-cobalt target in laminar helium flow. The laser induced fluorescence technique [2] is applied for local probing of gaseous Ni, Co and CZ species throughout the hot carbon flow of the target heated up to 3500 K. A rapid depletion of C2 in contrast to the spatial extent of metal atoms is observed in the plume (Fig. 1). This asserts that C2 condenses earlier than Ni and Co atoms.[3, 4]. The depletion is even faster when catalysts are present. It may indicate that an interaction between metal atoms and carbon dimers takes place in the gas as soon as they are expelled from the target surface. Two methods of modelling are used: a spatially I-D calculation developed originally for the arc process [5], and a zero-D time dependent calculation, solving the chemical kinetics along the streamlines [6]. The latter includes Ni cluster formation. The peak of C2 density is calculated close to the target surface where the temperature is the highest. In the hot region, C; is dominant. As the carbon products move away from the target and mix with the ambient helium, they recombine into larger clusters, as demonstrated by the peak of C5 density around 1 mm. The profile of Ni-atom density compares fairly well with the measured one (Fig. 2). The early increase is due to the drop of temperature, and the final decrease beyond 6 mm results from Ni cluster formation at the eutectic temperature (approx.1600 K).

Raman spectroscopy as a tool to investigate the structure and electronic properties of carbon-atom wires

PubMed Central

Milani, Alberto; Tommasini, Matteo; Russo, Valeria; Li Bassi, Andrea; Lucotti, Andrea; Cataldo, Franco

2015-01-01

Summary Graphene, nanotubes and other carbon nanostructures have shown potential as candidates for advanced technological applications due to the different coordination of carbon atoms and to the possibility of π-conjugation. In this context, atomic-scale wires comprised of sp-hybridized carbon atoms represent ideal 1D systems to potentially downscale devices to the atomic level. Carbon-atom wires (CAWs) can be arranged in two possible structures: a sequence of double bonds (cumulenes), resulting in a 1D metal, or an alternating sequence of single–triple bonds (polyynes), expected to show semiconducting properties. The electronic and optical properties of CAWs can be finely tuned by controlling the wire length (i.e., the number of carbon atoms) and the type of termination (e.g., atom, molecular group or nanostructure). Although linear, sp-hybridized carbon systems are still considered elusive and unstable materials, a number of nanostructures consisting of sp-carbon wires have been produced and characterized to date. In this short review, we present the main CAW synthesis techniques and stabilization strategies and we discuss the current status of the understanding of their structural, electronic and vibrational properties with particular attention to how these properties are related to one another. We focus on the use of vibrational spectroscopy to provide information on the structural and electronic properties of the system (e.g., determination of wire length). Moreover, by employing Raman spectroscopy and surface enhanced Raman scattering in combination with the support of first principles calculations, we show that a detailed understanding of the charge transfer between CAWs and metal nanoparticles may open the possibility to tune the electronic structure from alternating to equalized bonds. PMID:25821689

Chemical control of electrical contact to sp² carbon atoms.

PubMed

Frederiksen, Thomas; Foti, Giuseppe; Scheurer, Fabrice; Speisser, Virginie; Schull, Guillaume

2014-04-16

Carbon-based nanostructures are attracting tremendous interest as components in ultrafast electronics and optoelectronics. The electrical interfaces to these structures play a crucial role for the electron transport, but the lack of control at the atomic scale can hamper device functionality and integration into operating circuitry. Here we study a prototype carbon-based molecular junction consisting of a single C60 molecule and probe how the electric current through the junction depends on the chemical nature of the foremost electrode atom in contact with the molecule. We find that the efficiency of charge injection to a C60 molecule varies substantially for the considered metallic species, and demonstrate that the relative strength of the metal-C bond can be extracted from our transport measurements. Our study further suggests that a single-C60 junction is a basic model to explore the properties of electrical contacts to meso- and macroscopic sp(2) carbon structures.

Chemical control of electrical contact to sp2 carbon atoms

NASA Astrophysics Data System (ADS)

Frederiksen, Thomas; Foti, Giuseppe; Scheurer, Fabrice; Speisser, Virginie; Schull, Guillaume

2014-04-01

Carbon-based nanostructures are attracting tremendous interest as components in ultrafast electronics and optoelectronics. The electrical interfaces to these structures play a crucial role for the electron transport, but the lack of control at the atomic scale can hamper device functionality and integration into operating circuitry. Here we study a prototype carbon-based molecular junction consisting of a single C60 molecule and probe how the electric current through the junction depends on the chemical nature of the foremost electrode atom in contact with the molecule. We find that the efficiency of charge injection to a C60 molecule varies substantially for the considered metallic species, and demonstrate that the relative strength of the metal-C bond can be extracted from our transport measurements. Our study further suggests that a single-C60 junction is a basic model to explore the properties of electrical contacts to meso- and macroscopic sp2 carbon structures.

48 CFR 204.470 - U.S.-International Atomic Energy Agency Additional Protocol.

Code of Federal Regulations, 2010 CFR

2010-10-01

... 48 Federal Acquisition Regulations System 3 2010-10-01 2010-10-01 false U.S.-International Atomic Energy Agency Additional Protocol. 204.470 Section 204.470 Federal Acquisition Regulations System DEFENSE... Information Within Industry 204.470 U.S.-International Atomic Energy Agency Additional Protocol. ...

48 CFR 204.470 - U.S.-International Atomic Energy Agency Additional Protocol.

Code of Federal Regulations, 2011 CFR

2011-10-01

... 48 Federal Acquisition Regulations System 3 2011-10-01 2011-10-01 false U.S.-International Atomic Energy Agency Additional Protocol. 204.470 Section 204.470 Federal Acquisition Regulations System DEFENSE... Information Within Industry 204.470 U.S.-International Atomic Energy Agency Additional Protocol. ...

48 CFR 204.470 - U.S.-International Atomic Energy Agency Additional Protocol.

Code of Federal Regulations, 2012 CFR

2012-10-01

... 48 Federal Acquisition Regulations System 3 2012-10-01 2012-10-01 false U.S.-International Atomic Energy Agency Additional Protocol. 204.470 Section 204.470 Federal Acquisition Regulations System DEFENSE... Information Within Industry 204.470 U.S.-International Atomic Energy Agency Additional Protocol. ...

48 CFR 204.470 - U.S.-International Atomic Energy Agency Additional Protocol.

Code of Federal Regulations, 2014 CFR

2014-10-01

... 48 Federal Acquisition Regulations System 3 2014-10-01 2014-10-01 false U.S.-International Atomic Energy Agency Additional Protocol. 204.470 Section 204.470 Federal Acquisition Regulations System DEFENSE... Information Within Industry 204.470 U.S.-International Atomic Energy Agency Additional Protocol. ...

48 CFR 204.470 - U.S.-International Atomic Energy Agency Additional Protocol.

Code of Federal Regulations, 2013 CFR

2013-10-01

... 48 Federal Acquisition Regulations System 3 2013-10-01 2013-10-01 false U.S.-International Atomic Energy Agency Additional Protocol. 204.470 Section 204.470 Federal Acquisition Regulations System DEFENSE... Information Within Industry 204.470 U.S.-International Atomic Energy Agency Additional Protocol. ...

Carbon-, sulfur-, and phosphorus-based charge transfer reactions in inductively coupled plasma-atomic emission spectrometry

NASA Astrophysics Data System (ADS)

Grindlay, Guillermo; Gras, Luis; Mora, Juan; de Loos-Vollebregt, Margaretha T. C.

2016-01-01

In this work, the influence of carbon-, sulfur-, and phosphorus-based charge transfer reactions on the emission signal of 34 elements (Ag, Al, As, Au, B, Ba, Be, Ca, Cd, Co, Cr, Cu, Fe, Ga, Hg, I, In, Ir, K, Li, Mg, Mn, Na, Ni, P, Pb, Pd, Pt, S, Sb, Se, Sr, Te, and Zn) in axially viewed inductively coupled plasma-atomic emission spectrometry has been investigated. To this end, atomic and ionic emission signals for diluted glycerol, sulfuric acid, and phosphoric acid solutions were registered and results were compared to those obtained for a 1% w w- 1 nitric acid solution. Experimental results show that the emission intensities of As, Se, and Te atomic lines are enhanced by charge transfer from carbon, sulfur, and phosphorus ions. Iodine and P atomic emission is enhanced by carbon- and sulfur-based charge transfer whereas the Hg atomic emission signal is enhanced only by carbon. Though signal enhancement due to charge transfer reactions is also expected for ionic emission lines of the above-mentioned elements, no experimental evidence has been found with the exception of Hg ionic lines operating carbon solutions. The effect of carbon, sulfur, and phosphorus charge transfer reactions on atomic emission depends on (i) wavelength characteristics. In general, signal enhancement is more pronounced for electronic transitions involving the highest upper energy levels; (ii) plasma experimental conditions. The use of robust conditions (i.e. high r.f. power and lower nebulizer gas flow rates) improves carbon, sulfur, and phosphorus ionization in the plasma and, hence, signal enhancement; and (iii) the presence of other concomitants (e.g. K or Ca). Easily ionizable elements reduce ionization in the plasma and consequently reduce signal enhancement due to charge transfer reactions.

Atomic scale observation of oxygen delivery during silver–oxygen nanoparticle catalysed oxidation of carbon nanotubes

PubMed Central

Yue, Yonghai; Yuchi, Datong; Guan, Pengfei; Xu, Jia; Guo, Lin; Liu, Jingyue

2016-01-01

To probe the nature of metal-catalysed processes and to design better metal-based catalysts, atomic scale understanding of catalytic processes is highly desirable. Here we use aberration-corrected environmental transmission electron microscopy to investigate the atomic scale processes of silver-based nanoparticles, which catalyse the oxidation of multi-wall carbon nanotubes. A direct semi-quantitative estimate of the oxidized carbon atoms by silver-based nanoparticles is achieved. A mechanism similar to the Mars–van Krevelen process is invoked to explain the catalytic oxidation process. Theoretical calculations, together with the experimental data, suggest that the oxygen molecules dissociate on the surface of silver nanoparticles and diffuse through the silver nanoparticles to reach the silver/carbon interfaces and subsequently oxidize the carbon. The lattice distortion caused by oxygen concentration gradient within the silver nanoparticles provides the direct evidence for oxygen diffusion. Such direct observation of atomic scale dynamics provides an important general methodology for investigations of catalytic processes. PMID:27406595

Effect of carbon and alloying solute atoms on helium behaviors in α-Fe

NASA Astrophysics Data System (ADS)

Zhang, Yange; You, Yu-Wei; Xu, Yichun; Liu, C. S.; Chen, J. L.; Luo, G.-N.

2017-02-01

Helium bubbles could strongly degrade the mechanical properties of ferritic steels in fission and fusion systems. The formation of helium bubble is directly affected by the interactions between helium and the compositions in steels, such as solute atoms, carbon and irradiation defects. We thereby performed systematical first-principles calculations to investigate the interactions of solute-helium and carbon-solute-helium. It is found that substitutional helium is more attractive than interstitial helium to all the considered 3p, 4p, 5p and 6p solutes. The attraction between carbon and substitutional helium suggests the carbon-solute-helium complex can be formed stably. By examining the charge density difference and thermal stability, it is found that the ternary complex shows stronger attraction with He than that of solute-helium pair for some solutes (S, Se, In, Te, Pb and Bi) and the complex could existed in iron stably at 700 K. The present theoretical results may be helpful for exploring alloy additions to mitigate the formation of large helium bubbles.

Diagnostics of Carbon Nanotube Formation in a Laser Produced Plume: An Investigation of the Metal Catalyst by Laser Ablation Atomic Fluorescence Spectroscopy

NASA Technical Reports Server (NTRS)

deBoer, Gary; Scott, Carl

2003-01-01

atoms survive for several milliseconds while the gaseous carbon atoms and small molecules nucleate more rapidly. Additional experiments and the development of in situ methods for carbon nanotube detection would allow these results to be interpreted from the perspective of carbon nanotube formation.

Monte Carlo Approach for Estimating Density and Atomic Number From Dual-Energy Computed Tomography Images of Carbonate Rocks

NASA Astrophysics Data System (ADS)

Victor, Rodolfo A.; Prodanović, Maša.; Torres-Verdín, Carlos

2017-12-01

We develop a new Monte Carlo-based inversion method for estimating electron density and effective atomic number from 3-D dual-energy computed tomography (CT) core scans. The method accounts for uncertainties in X-ray attenuation coefficients resulting from the polychromatic nature of X-ray beam sources of medical and industrial scanners, in addition to delivering uncertainty estimates of inversion products. Estimation of electron density and effective atomic number from CT core scans enables direct deterministic or statistical correlations with salient rock properties for improved petrophysical evaluation; this condition is specifically important in media such as vuggy carbonates where CT resolution better captures core heterogeneity that dominates fluid flow properties. Verification tests of the inversion method performed on a set of highly heterogeneous carbonate cores yield very good agreement with in situ borehole measurements of density and photoelectric factor.

Carbon Displacement-Induced Single Carbon Atomic Chain Formation and its Effects on Sliding of SiC Fibers in SiC/graphene/SiC Composite

DOE PAGES

Wallace, Joseph B.; Chen, Di; Shao, Lin

2015-11-03

Understanding radiation effects on the mechanical properties of SiC composites is important to their application in advanced reactor designs. By means of molecular dynamics simulations, we found that due to strong interface bonding between the graphene layers and SiC, the sliding friction of SiC fibers is largely determined by the frictional behavior between graphene layers. Upon sliding, carbon displacements between graphene layers can act as seed atoms to induce the formation of single carbon atomic chains (SCACs) by pulling carbon atoms from the neighboring graphene planes. The formation, growth, and breaking of SCACs determine the frictional response to irradiation.

Carbon nanotube-clamped metal atomic chain

PubMed Central

Tang, Dai-Ming; Yin, Li-Chang; Li, Feng; Liu, Chang; Yu, Wan-Jing; Hou, Peng-Xiang; Wu, Bo; Lee, Young-Hee; Ma, Xiu-Liang; Cheng, Hui-Ming

2010-01-01

Metal atomic chain (MAC) is an ultimate one-dimensional structure with unique physical properties, such as quantized conductance, colossal magnetic anisotropy, and quantized magnetoresistance. Therefore, MACs show great potential as possible components of nanoscale electronic and spintronic devices. However, MACs are usually suspended between two macroscale metallic electrodes; hence obvious technical barriers exist in the interconnection and integration of MACs. Here we report a carbon nanotube (CNT)-clamped MAC, where CNTs play the roles of both nanoconnector and electrodes. This nanostructure is prepared by in situ machining a metal-filled CNT, including peeling off carbon shells by spatially and elementally selective electron beam irradiation and further elongating the exposed metal nanorod. The microstructure and formation process of this CNT-clamped MAC are explored by both transmission electron microscopy observations and theoretical simulations. First-principles calculations indicate that strong covalent bonds are formed between the CNT and MAC. The electrical transport property of the CNT-clamped MAC was experimentally measured, and quantized conductance was observed. PMID:20427743

Plasmon enhanced Raman scattering effect for an atom near a carbon nanotube

DOE PAGES

Bondarev, I. V.

2015-01-01

Quantum electrodynamics theory of the resonance Raman scattering is developed for an atom in a close proximity to a carbon nanotube. The theory predicts a dramatic enhancement of the Raman intensity in the strong atomic coupling regime to nanotube plasmon near-fields. This resonance scattering is a manifestation of the general electromagnetic surface enhanced Raman scattering effect, and can be used in designing efficient nanotube based optical sensing substrates for single atom detection, precision spontaneous emission control, and manipulation.

Effects of Al addition on atomic structure of Cu-Zr metallic glass

NASA Astrophysics Data System (ADS)

Li, Feng; Zhang, Huajian; Liu, Xiongjun; Dong, Yuecheng; Yu, Chunyan; Lu, Zhaoping

2018-02-01

The atomic structures of Cu52Zr48 and Cu45Zr48Al7 metallic glasses (MGs) have been studied by molecular dynamic simulations. The results reveal that the molar volume of the Cu45Zr48Al7 MG is smaller than that of the Cu52Zr48 MG, although the size of the Al atom is larger than that of the Cu atom, implying an enhanced atomic packing density achieved by introducing Al into the ternary MG. Bond shortening in unlike atomic pairs Zr-Al and Cu-Al is observed in the Cu45Zr48Al7 MG, which is attributed to strong interactions between Al and (Zr, Cu) atoms. Meanwhile, the atomic packing efficiency is enhanced by the minor addition of Al. Compared with the Cu52Zr48 binary MG, the potential energy of the ternary MG decreases and the glass transition temperature increases. Structural analyses indicate that more Cu- and Al-centered full icosahedral clusters emerge in the Cu45Zr48Al7 MG as some Cu atoms are substituted by Al. Furthermore, the addition of Al leads to more icosahedral medium-range orders in the ternary MG. The increase of full icosahedral clusters and the enhancement of the packing density are responsible for the improved glass-forming ability of Cu45Zr48Al7.

Atomic Layer Epitaxy of Aluminum Nitride: Unraveling the Connection between Hydrogen Plasma and Carbon Contamination.

PubMed

Erwin, Steven C; Lyons, John L

2018-06-13

Atomistic control over the growth of semiconductor thin films, such as aluminum nitride, is a long-sought goal in materials physics. One promising approach is plasma-assisted atomic layer epitaxy, in which separate reactant precursors are employed to grow the cation and anion layers in alternating deposition steps. The use of a plasma during the growth-most often a hydrogen plasma-is now routine and generally considered critical, but the precise role of the plasma is not well-understood. We propose a theoretical atomistic model and elucidate its consequences using analytical rate equations, density functional theory, and kinetic Monte Carlo statistical simulations. We show that using a plasma has two important consequences, one beneficial and one detrimental. The plasma produces atomic hydrogen in the gas phase, which is important for removing methyl radicals left over from the aluminum precursor molecules. However, atomic hydrogen also leads to atomic carbon on the surface and, moreover, opens a channel for trapping these carbon atoms as impurities in the subsurface region, where they remain as unwanted contaminants. Understanding this dual role leads us to propose a solution for the carbon contamination problem which leaves the main benefit of the plasma largely unaffected.

Carbon nanomaterials used as conductive additives in lithium ion batteries.

PubMed

Zhang, Qingtang; Yu, Zuolong; Du, Ping; Su, Ce

2010-06-01

As the vital part of lithium ion batteries, conductive additives play important roles in the electrochemical performance of lithium ion batteries. They construct a conductive percolation network to increase and keep the electronic conductivity of electrode, enabling it charge and discharge faster. In addition, conductive additives absorb and retain electrolyte, allowing an intimate contact between the lithium ions and active materials. Carbon nanomaterials are carbon black, Super P, acetylene black, carbon nanofibers, and carbon nanotubes, which all have superior properties such as low weight, high chemical inertia and high specific surface area. They are the ideal conductive additives for lithium ion batteries. This review will discuss some registered patents and relevant papers about the carbon nanomaterials that are used as conductive additives in cathode or anode to improve the electrochemical performance of lithium ion batteries.

Catalytic conversion of alcohols having at least three carbon atoms to hydrocarbon blendstock

DOEpatents

Narula, Chaitanya K.; Davison, Brian H.

2018-04-17

A method for producing a hydrocarbon blendstock, the method comprising contacting at least one saturated acyclic alcohol having at least three and up to ten carbon atoms with a metal-loaded zeolite catalyst at a temperature of at least 100.degree. C. and up to 550.degree. C., wherein the metal is a positively-charged metal ion, and the metal-loaded zeolite catalyst is catalytically active for converting the alcohol to the hydrocarbon blendstock, wherein the method directly produces a hydrocarbon blendstock having less than 1 vol % ethylene and at least 35 vol % of hydrocarbon compounds containing at least eight carbon atoms.

Catalytic conversion of alcohols having at least three carbon atoms to hydrocarbon blendstock

DOEpatents

Narula, Chaitanya K.; Davison, Brian H.

2015-11-13

A method for producing a hydrocarbon blendstock, the method comprising contacting at least one saturated acyclic alcohol having at least three and up to ten carbon atoms with a metal-loaded zeolite catalyst at a temperature of at least 100°C and up to 550°C, wherein the metal is a positively-charged metal ion, and the metal-loaded zeolite catalyst is catalytically active for converting the alcohol to the hydrocarbon blendstock, wherein the method directly produces a hydrocarbon blendstock having less than 1 vol % ethylene and at least 35 vol % of hydrocarbon compounds containing at least eight carbon atoms.

Smooth Scaling of Valence Electronic Properties in Fullerenes: From One Carbon Atom, to C60, to Graphene

DTIC Science & Technology

2012-09-18

Smooth scaling of valence electronic properties in fullerenes: from one carbon atom , to C60, to graphene Greyson R. Lewis,1 William E. Bunting,1...pacitance scaling lines of the fullerenes. Lastly, it is found that points representing the carbon atom and the graphene limit lie on scaling lines for...icosahedral fullerenes, so their quantum capacitances and their detachment energies scale smoothly from one C atom , through C60, to graphene. I

Polarizabilities and van der Waals C{sub 6} coefficients of fullerenes from an atomistic electrodynamics model: Anomalous scaling with number of carbon atoms

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

Saidi, Wissam A., E-mail: alsaidi@pitt.edu; Norman, Patrick

2016-07-14

The van der Waals C{sub 6} coefficients of fullerenes are shown to exhibit an anomalous dependence on the number of carbon atoms N such that C{sub 6} ∝ N{sup 2.2} as predicted using state-of-the-art quantum mechanical calculations based on fullerenes with small sizes, and N{sup 2.75} as predicted using a classical-metallic spherical-shell approximation of the fullerenes. We use an atomistic electrodynamics model where each carbon atom is described by a polarizable object to extend the quantum mechanical calculations to larger fullerenes. The parameters of this model are optimized to describe accurately the static and complex polarizabilities of the fullerenes bymore » fitting against accurate ab initio calculations. This model shows that C{sub 6} ∝ N{sup 2.8}, which is supportive of the classical-metallic spherical-shell approximation. Additionally, we show that the anomalous dependence of the polarizability on N is attributed to the electric charge term, while the dipole–dipole term scales almost linearly with the number of carbon atoms.« less

A first principle study for the adsorption and absorption of carbon atom and the CO dissociation on Ir(100) surface

NASA Astrophysics Data System (ADS)

Erikat, I. A.; Hamad, B. A.

2013-11-01

We employ density functional theory to examine the adsorption and absorption of carbon atom as well as the dissociation of carbon monoxide on Ir(100) surface. We find that carbon atoms bind strongly with Ir(100) surface and prefer the high coordination hollow site for all coverages. In the case of 0.75 ML coverage of carbon, we obtain a bridging metal structure due to the balance between Ir-C and Ir-Ir interactions. In the subsurface region, the carbon atom prefers the octahedral site of Ir(100) surface. We find large diffusion barrier for carbon atom into Ir(100) surface (2.70 eV) due to the strong bonding between carbon atom and Ir(100) surface, whereas we find a very small segregation barrier (0.22 eV) from subsurface to the surface. The minimum energy path and energy barrier for the dissociation of CO on Ir(100) surface are obtained by using climbing image nudge elastic band. The energy barrier of CO dissociation on Ir(100) surface is found to be 3.01 eV, which is appreciably larger than the association energy (1.61 eV) of this molecule.

A first principle study for the adsorption and absorption of carbon atom and the CO dissociation on Ir(100) surface.

PubMed

Erikat, I A; Hamad, B A

2013-11-07

We employ density functional theory to examine the adsorption and absorption of carbon atom as well as the dissociation of carbon monoxide on Ir(100) surface. We find that carbon atoms bind strongly with Ir(100) surface and prefer the high coordination hollow site for all coverages. In the case of 0.75 ML coverage of carbon, we obtain a bridging metal structure due to the balance between Ir-C and Ir-Ir interactions. In the subsurface region, the carbon atom prefers the octahedral site of Ir(100) surface. We find large diffusion barrier for carbon atom into Ir(100) surface (2.70 eV) due to the strong bonding between carbon atom and Ir(100) surface, whereas we find a very small segregation barrier (0.22 eV) from subsurface to the surface. The minimum energy path and energy barrier for the dissociation of CO on Ir(100) surface are obtained by using climbing image nudge elastic band. The energy barrier of CO dissociation on Ir(100) surface is found to be 3.01 eV, which is appreciably larger than the association energy (1.61 eV) of this molecule.

High performance current and spin diode of atomic carbon chain between transversely symmetric ribbon electrodes.

PubMed

Dong, Yao-Jun; Wang, Xue-Feng; Yang, Shuo-Wang; Wu, Xue-Mei

2014-08-21

We demonstrate that giant current and high spin rectification ratios can be achieved in atomic carbon chain devices connected between two symmetric ferromagnetic zigzag-graphene-nanoribbon electrodes. The spin dependent transport simulation is carried out by density functional theory combined with the non-equilibrium Green's function method. It is found that the transverse symmetries of the electronic wave functions in the nanoribbons and the carbon chain are critical to the spin transport modes. In the parallel magnetization configuration of two electrodes, pure spin current is observed in both linear and nonlinear regions. However, in the antiparallel configuration, the spin-up (down) current is prohibited under the positive (negative) voltage bias, which results in a spin rectification ratio of order 10(4). When edge carbon atoms are substituted with boron atoms to suppress the edge magnetization in one of the electrodes, we obtain a diode with current rectification ratio over 10(6).

High performance current and spin diode of atomic carbon chain between transversely symmetric ribbon electrodes

PubMed Central

Dong, Yao-Jun; Wang, Xue-Feng; Yang, Shuo-Wang; Wu, Xue-Mei

2014-01-01

We demonstrate that giant current and high spin rectification ratios can be achieved in atomic carbon chain devices connected between two symmetric ferromagnetic zigzag-graphene-nanoribbon electrodes. The spin dependent transport simulation is carried out by density functional theory combined with the non-equilibrium Green's function method. It is found that the transverse symmetries of the electronic wave functions in the nanoribbons and the carbon chain are critical to the spin transport modes. In the parallel magnetization configuration of two electrodes, pure spin current is observed in both linear and nonlinear regions. However, in the antiparallel configuration, the spin-up (down) current is prohibited under the positive (negative) voltage bias, which results in a spin rectification ratio of order 104. When edge carbon atoms are substituted with boron atoms to suppress the edge magnetization in one of the electrodes, we obtain a diode with current rectification ratio over 106. PMID:25142376

Silicon solar cell performance deposited by diamond like carbon thin film ;Atomic oxygen effects;

NASA Astrophysics Data System (ADS)

Aghaei, Abbas Ail; Eshaghi, Akbar; Karami, Esmaeil

2017-09-01

In this research, a diamond-like carbon thin film was deposited on p-type polycrystalline silicon solar cell via plasma-enhanced chemical vapor deposition method by using methane and hydrogen gases. The effect of atomic oxygen on the functioning of silicon coated DLC thin film and silicon was investigated. Raman spectroscopy, field emission scanning electron microscopy, atomic force microscopy and attenuated total reflection-Fourier transform infrared spectroscopy were used to characterize the structure and morphology of the DLC thin film. Photocurrent-voltage characteristics of the silicon solar cell were carried out using a solar simulator. The results showed that atomic oxygen exposure induced the including oxidation, structural changes, cross-linking reactions and bond breaking of the DLC film; thus reducing the optical properties. The photocurrent-voltage characteristics showed that although the properties of the fabricated thin film were decreased after being exposed to destructive rays, when compared with solar cell without any coating, it could protect it in atomic oxygen condition enhancing solar cell efficiency up to 12%. Thus, it can be said that diamond-like carbon thin layer protect the solar cell against atomic oxygen exposure.

Carbon-hydrogen defects with a neighboring oxygen atom in n-type Si

NASA Astrophysics Data System (ADS)

Gwozdz, K.; Stübner, R.; Kolkovsky, Vl.; Weber, J.

2017-07-01

We report on the electrical activation of neutral carbon-oxygen complexes in Si by wet-chemical etching at room temperature. Two deep levels, E65 and E75, are observed by deep level transient spectroscopy in n-type Czochralski Si. The activation enthalpies of E65 and E75 are obtained as EC-0.11 eV (E65) and EC-0.13 eV (E75). The electric field dependence of their emission rates relates both levels to single acceptor states. From the analysis of the depth profiles, we conclude that the levels belong to two different defects, which contain only one hydrogen atom. A configuration is proposed, where the CH1BC defect, with hydrogen in the bond-centered position between neighboring C and Si atoms, is disturbed by interstitial oxygen in the second nearest neighbor position to substitutional carbon. The significant reduction of the CH1BC concentration in samples with high oxygen concentrations limits the use of this defect for the determination of low concentrations of substitutional carbon in Si samples.

Reactions of Atomic Carbon with Butene Isomers: Implications for Molecular Growth in Carbon-Rich Environments

DOE PAGES

Bourgalais, J.; Spencer, Michael; Osborn, David L.; ...

2016-10-31

We carried out the product detection studies of C( 3P) atom reactions with butene (C 4H 8) isomers (but-1-ene, cis-but-2-ene, trans-but-2-ene) in a flow tube reactor at 353 K and 4 Torr under multiple collision conditions. Ground state carbon atoms are generated by 248 nm laser photolysis of tetrabromomethane, CBr 4, in a buffer of helium. Thermalized reaction products are detected using synchrotron tunable VUV photoionization and time-of-flight mass spectrometry. The temporal profiles of the detected ions are used to discriminate products from side or secondary reactions. Furthermore, for the C( 3P) + trans-but-2-ene and C( 3P) + cis-but-2-ene reactions,more » various isomers of C 4H 5 and C 5H 7 are identified as reaction products formed via CH 3 and H elimination. Assuming equal ionization cross sections for all C 4H 5 and C 5H 7 isomers, C 4H 5:C 5H 7 branching ratios of 0.63:1 and 0.60:1 are derived for the C( 3P) + trans-but-2-ene and the C( 3P) + cis-but-2-ene reactions, respectively. For the C( 3P) + but-1-ene reaction, two reaction channels are observed: the H-elimination channel, leading to the formation of the ethylpropargyl isomer, and the C 3H 3 + C 2H 5 channel. Assuming equal ionization cross sections for ethylpropargyl and C 3H 3 radicals, a branching ratio of 1:0.95 for the C 3H 3 + C 2H 5 and H + ethylpropargyl channels is derived. Finally, the experimental results are compared to previous H atom branching ratios and used to propose the most likely mechanisms for the reaction of ground state carbon atoms with butene isomers.« less

Transfer-free synthesis of graphene-like atomically thin carbon films on SiC by ion beam mixing technique

NASA Astrophysics Data System (ADS)

Zhang, Rui; Chen, Fenghua; Wang, Jinbin; Fu, Dejun

2018-03-01

Here we demonstrate the synthesis of graphene directly on SiC substrates at 900 °C using ion beam mixing technique with energetic carbon cluster ions on Ni/SiC structures. The thickness of 7-8 nm Ni films was evaporated on the SiC substrates, followed by C cluster ion bombarding. Carbon cluster ions C4 were bombarded at 16 keV with the dosage of 4 × 1016 atoms/cm2. After thermal annealing process Ni silicides were formed, whereas C atoms either from the decomposition of the SiC substrates or the implanted contributes to the graphene synthesis by segregating and precipitating process. The limited solubility of carbon atoms in silicides, involving SiC, Ni2Si, Ni5Si2, Ni3Si, resulted in diffusion and precipitation of carbon atoms to form graphene on top of Ni and the interface of Ni/SiC. The ion beam mixing technique provides an attractive production method of a transfer-free graphene growth on SiC and be compatible with current device fabrication.

Performance of carbon material derived from starch mixed with flame retardant as electrochemical capacitor

NASA Astrophysics Data System (ADS)

Tsubota, Toshiki; Morita, Masaki; Murakami, Naoya; Ohno, Teruhisa

2014-12-01

Carbon materials derived from starch with an added flame retardant, such as melamine polyphosphate, melamine sulfate, guanylurea phosphate, or guanidine phosphate, were synthesized for investigating the performance as the electrode of an electrochemical capacitor. The yield after the heat treatment of the carbonization reaction increased by the addition of these flame retardants up to 800 °C. Although both the specific surface area and electrical resistivity are almost independent of the addition of the flame retardants, the capacitance values are improved with the addition of the flame retardants. The nitrogen atoms derived from the flame retardants are introduced to some extent into the synthesized carbon material. Moreover, the phosphorous atoms or the sulfur atoms derived from the flame retardants are doped into the synthesized carbon material. The method applied in this study, that is, the addition of flame retardants before the carbonization process can be used for the doping of the hetero atom such as N, P and S into the carbon material.

Buckling behaviors of single-walled carbon nanotubes inserted with a linear carbon-atom chain.

PubMed

Zhu, Chunhua; Chen, Yinfeng; Liu, Rumeng; Zhao, Junhua

2018-08-17

Buckling behaviors of single-walled carbon nanotubes (SWCNTs) inserted with a linear carbon-atom chain (CAC) (the composite structures are also called carbon nanowires (CNWs)) under torsion and bending as well as compression are studied using molecular dynamics (MD) simulations, respectively. Our MD results show that the critical buckling angles (or strains) of CNWs under the three presented kinds of loading patterns can be two times those of corresponding independent SWCNTs for long CNWs, while the buckling improvement is not obvious for short ones. The main reason is that the radial van der Waals force between the CAC and the SWCNT is very small for a short CNW, while it increases with increasing length and then tends to a constant for a long CNW. The obtained MD results agree well with those from available theoretical models. These findings will be a great help towards understanding the stability and reliability of the special CNT structures, and designing flexible CNT-based devices.

Adsorption Energies of Carbon, Nitrogen, and Oxygen Atoms on the Low-temperature Amorphous Water Ice: A Systematic Estimation from Quantum Chemistry Calculations

NASA Astrophysics Data System (ADS)

Shimonishi, Takashi; Nakatani, Naoki; Furuya, Kenji; Hama, Tetsuya

2018-03-01

We propose a new simple computational model to estimate the adsorption energies of atoms and molecules to low-temperature amorphous water ice, and we present the adsorption energies of carbon (3 P), nitrogen (4 S), and oxygen (3 P) atoms based on quantum chemistry calculations. The adsorption energies were estimated to be 14,100 ± 420 K for carbon, 400 ± 30 K for nitrogen, and 1440 ± 160 K for oxygen. The adsorption energy of oxygen is consistent with experimentally reported values. We found that the binding of a nitrogen atom is purely physisorption, while that of a carbon atom is chemisorption, in which a chemical bond to an O atom of a water molecule is formed. That of an oxygen atom has a dual character, with both physisorption and chemisorption. The chemisorption of atomic carbon also implies the possibility of further chemical reactions to produce molecules bearing a C–O bond, though this may hinder the formation of methane on water ice via sequential hydrogenation of carbon atoms. These properties would have a large impact on the chemical evolution of carbon species in interstellar environments. We also investigated the effects of newly calculated adsorption energies on the chemical compositions of cold dense molecular clouds with the aid of gas-ice astrochemical simulations. We found that abundances of major nitrogen-bearing molecules, such as N2 and NH3, are significantly altered by applying the calculated adsorption energy, because nitrogen atoms can thermally diffuse on surfaces, even at 10 K.

Atoms in carbon cages as a source of interstellar diffuse lines

NASA Technical Reports Server (NTRS)

Ballester, J. L.; Antoniewicz, P. R.; Smoluchowski, R.

1990-01-01

A model to describe the resonance absorption lines of various atoms trapped in closed carbon cages is presented. These systems may be responsible for some of the as yet unexplained diffuse interstellar bands. Model potentials for possible atom-C60 systems are obtained and used to calculate the resonance lines. The trapped atoms considered are O, N, Si, Mg, Al, Na, and S, and in all cases the resonance lines are shifted toward the red as compared to the isolated atoms. The calculated wavelengths are compared to the range of wavelengths observed for the diffuse interstellar bands, and good agreement is found for Mg and Si resonance lines. Other lines may be caused by other than resonance transitions or by trapped molecules. The oscillator strengths and the abundances are evaluated and compared with observation. Mechanisms to explain the observed band width of the lines and the existence of certain correlated pairs of lines are discussed.

Optimization of metal atomic ratio of PdxRuyNiz on carbon support for ethanol oxidation

NASA Astrophysics Data System (ADS)

Charoen, Kanin; Warakulwit, Chompunuch; Prapainainar, Chaiwat; Seubsai, Anusorn; Chareonpanich, Metta; Prapainainar, Paweena

2017-11-01

The catalytic activity of palladium (Pd) on an alloy catalyst on carbon supports with regards to ethanol oxidation was enhanced by systematically varying the atomic ratio of Pd, ruthenium (Ru), and nickel (Ni) alloy catalyst. Each atomic ratio catalyst was investigated so as to find the highest current density per mass of palladium. Functionalized carbon black (C) and reduced graphene oxide (rGO) were used as carbon supports. The PdxRuyNiz/carbon catalysts were prepared by impregnation and reduction method with sodium borohydride (NaBH4) being used as the reducing agent. Fourier transform infrared spectroscopy (FT-IR) and thermogravimetric analysis (TGA) were used to characterize the functionalized carbon supports, and the synthesized PdxRuyNiz/carbon catalysts were characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM-EDS), and inductively coupled plasma (ICP). The electrical properties of catalyst were performed by cyclic voltammetry (CV), chronoamperometry (CA), and CO-stripping to investigate the catalytic activity compared to 20%wt synthesized Pd/C. The results showed that Pd:Ru:Ni = 60:0:40 on rGO (Pd60Ni40/rGO) had the best metal atomic ratio and support for the electro-oxidation of ethanol. The maximum current density and the electrochemical surface area were 11,074 mA cm-2 mg-1Pd and 55.6 m2 g-1Pd, which were 1.7 and 2.67 times the corresponding values of synthesized Pd/C, respectively.

Topological Characterization of Carbon Graphite and Crystal Cubic Carbon Structures.

PubMed

Siddiqui, Wei Gao Muhammad Kamran; Naeem, Muhammad; Rehman, Najma Abdul

2017-09-07

Graph theory is used for modeling, designing, analysis and understanding chemical structures or chemical networks and their properties. The molecular graph is a graph consisting of atoms called vertices and the chemical bond between atoms called edges. In this article, we study the chemical graphs of carbon graphite and crystal structure of cubic carbon. Moreover, we compute and give closed formulas of degree based additive topological indices, namely hyper-Zagreb index, first multiple and second multiple Zagreb indices, and first and second Zagreb polynomials.

Effects of chemical states of carbon on deuterium retention in carbon-containing materials

NASA Astrophysics Data System (ADS)

Oyaidzu, Makoto; Kimura, Hiromi; Nakahata, Toshihiko; Nishikawa, Yusuke; Tokitani, Masayuki; Oya, Yasuhisa; Iwakiri, Hirotomo; Yoshida, Naoaki; Okuno, Kenji

2007-08-01

Deuterium retention behavior in highly oriented pyrolytic graphite (HOPG), poly-crystalline diamond, poly-crystalline SiC, sintered WC, and converted B 4C were investigated to reveal tritium behavior in re-deposition and co-deposition layers. Such layers would contain carbon, when the first wall and/or divertor were made of graphite or carbon-containing materials. Furthermore, the employment of other materials such as tungsten, and first wall conditioning such as boronization would complicate the layers. No different deuterium trapping sites due to carbon from those in HOPG were found in all the samples, where two deuterium trapping processes were observed: hot atom chemical trapping of energetic deuterium by a dangling bond of carbon and thermochemical trapping of thermalized deuterium in a constituent atom vacancy surrounded by carbons. Additionally, the latter reaction could be easily counteracted by or competed with the other deuterium trapping reactions by constituent atoms.

Theoretical Kinetics Analysis for Ḣ Atom Addition to 1,3-Butadiene and Related Reactions on the Ċ4H7 Potential Energy Surface.

PubMed

Li, Yang; Klippenstein, Stephen J; Zhou, Chong-Wen; Curran, Henry J

2017-10-12

found that abstraction from the central carbon atoms is the dominant channel (>70%) at temperatures in the range of 298-2000 K. Finally, by incorporating our calculated rate constants for both Ḣ atom addition and abstraction into our recently developed 1,3-butadiene model, we show that laminar flame speed predictions are significantly improved, emphasizing the value of this study.

Conductivity enhancement of carbon aerogel by modified gelation using self additive

NASA Astrophysics Data System (ADS)

Singh, Ashish; Kohli, D. K.; Bhartiya, Sushmita; Singh, Rashmi; Rajak, Gaurav; Singh, M. K.; Karnal, A. K.

2018-04-01

Carbon aerogels having high surface area and open pore structure are being studied for many electrochemical applications such as fuel cells and super capacitors. Moderate electrical conductivity of resorcinol - formaldehyde (R-F) derived carbon aerogel limits its utility in these applications. The current manuscript briefs about the synthesis of composite carbon aerogel using carbon aerogel itself as additive during gelation of water based carbon aerogel and study the effect on its conductivity and surface properties. The additive carbon aerogel was synthesized and pre-treated at higher temperature to achieve enhancement in conductivity. The composite carbon aerogel (CCA) samples were characterized for surface area properties, morphology, electrical conductivity and specific capacitance. The surface area properties of CCA showed improvement and specific surface area of ˜1798 m2/g with total pore volume of 1.7 cm3/g. was obtained. The electrical conductivity of the composite carbon aerogel with 5 wt % additive showed improvement over the plain carbon aerogel with respective values of 144 S/m and 128 S/m. The specific capacitance evaluated for CA and CCA are 102 and 118 F/g at scan rate of 10mV/s with improvement of ˜16%.

Low-temperature Condensation of Carbon

NASA Astrophysics Data System (ADS)

Krasnokutski, S. A.; Goulart, M.; Gordon, E. B.; Ritsch, A.; Jäger, C.; Rastogi, M.; Salvenmoser, W.; Henning, Th.; Scheier, P.

2017-10-01

Two different types of experiments were performed. In the first experiment, we studied the low-temperature condensation of vaporized graphite inside bulk liquid helium, while in the second experiment, we studied the condensation of single carbon atoms together with H2, H2O, and CO molecules inside helium nanodroplets. The condensation of vaporized graphite leads to the formation of partially graphitized carbon, which indicates high temperatures, supposedly higher than 1000°C, during condensation. Possible underlying processes responsible for the instant rise in temperature during condensation are discussed. This suggests that such processes cause the presence of partially graphitized carbon dust formed by low-temperature condensation in the diffuse interstellar medium. Alternatively, in the denser regions of the ISM, the condensation of carbon atoms together with the most abundant interstellar molecules (H2, H2O, and CO), leads to the formation of complex organic molecules (COMs) and finally organic polymers. Water molecules were found not to be involved directly in the reaction network leading to the formation of COMs. It was proposed that COMs are formed via the addition of carbon atoms to H2 and CO molecules ({{C}}+{{{H}}}2\\to {HCH},{HCH}+{CO}\\to {{OCCH}}2). Due to the involvement of molecular hydrogen, the formation of COMs by carbon addition reactions should be more efficient at high extinctions compared with the previously proposed reaction scheme with atomic hydrogen.

Atomic hydrogen cleaning of EUV multilayer optics

NASA Astrophysics Data System (ADS)

Graham, Samuel, Jr.; Steinhaus, Charles A.; Clift, W. Miles; Klebanoff, Leonard E.; Bajt, Sasa

2003-06-01

Recent studies have been conducted to investigate the use of atomic hydrogen as an in-situ contamination removal method for EUV optics. In these experiments, a commercial source was used to produce atomic hydrogen by thermal dissociation of molecular hydrogen using a hot filament. Samples for these experiments consisted of silicon wafers coated with sputtered carbon, Mo/Si optics with EUV-induced carbon, and bare Si-capped and Ru-B4C-capped Mo/Si optics. Samples were exposed to an atomic hydrogen source at a distance of 200 - 500 mm downstream and angles between 0-90° with respect to the source. Carbon removal rates and optic oxidation rates were measured using Auger electron spectroscopy depth profiling. In addition, at-wavelength peak reflectance (13.4 nm) was measured using the EUV reflectometer at the Advanced Light Source. Data from these experiments show carbon removal rates up to 20 Ê/hr for sputtered carbon and 40 Ê/hr for EUV deposited carbon at a distance of 200 mm downstream. The cleaning rate was also observed to be a strong function of distance and angular position. Experiments have also shown that the carbon etch rate can be increased by a factor of 4 by channeling atomic hydrogen through quartz tubes in order to direct the atomic hydrogen to the optic surface. Atomic hydrogen exposures of bare optic samples show a small risk in reflectivity degradation after extended periods. Extended exposures (up to 20 hours) of bare Si-capped Mo/Si optics show a 1.2% loss (absolute) in reflectivity while the Ru-B4C-capped Mo/Si optics show a loss on the order of 0.5%. In order to investigate the source of this reflectivity degradation, optic samples were exposed to atomic deuterium and analyzed using low energy ion scattering direct recoil spectroscopy to determine any reactions of the hydrogen with the multilayer stack. Overall, the results show that the risk of over-etching with atomic hydrogen is much less than previous studies using RF discharge cleaning

Atomic hydrogen cleaning of EUV multilayer optics

NASA Astrophysics Data System (ADS)

Graham, Samuel, Jr.; Steinhaus, Charles A.; Clift, W. Miles; Klebanoff, Leonard E.; Bajt, Sasa

2003-06-01

Recent studies have been conducted to investigate the use of atomic hydrogen as an in-situ contamination removal method for EUV optics. In these experiments, a commercial source was used to produce atomic hydrogen by thermal dissociation of molecular hydrogen using a hot filament. Samples for these experiments consisted of silicon wafers coated with sputtered carbon, Mo/Si optics with EUV-induced carbon, and bare Si-capped and Ru-B4C-capped Mo/Si optics. Samples were exposed to an atomic hydrogen source at a distance of 200 - 500 mm downstream and angles between 0-90° with respect to the source. Carbon removal rates and optic oxidation rates were measured using Auger electron spectroscopy depth profiling. In addition, at-wavelength peak reflectance (13.4 nm) was measured using the EUV reflectometer at the Advanced Light Source. Data from these experiments show carbon removal rates up to 20 Å/hr for sputtered carbon and 40 Å/hr for EUV deposited carbon at a distance of 200 mm downstream. The cleaning rate was also observed to be a strong function of distance and angular position. Experiments have also shown that the carbon etch rate can be increased by a factor of 4 by channeling atomic hydrogen through quartz tubes in order to direct the atomic hydrogen to the optic surface. Atomic hydrogen exposures of bare optic samples show a small risk in reflectivity degradation after extended periods. Extended exposures (up to 20 hours) of bare Si-capped Mo/Si optics show a 1.2% loss (absolute) in reflectivity while the Ru-B4C-capped Mo/Si optics show a loss on the order of 0.5%. In order to investigate the source of this reflectivity degradation, optic samples were exposed to atomic deuterium and analyzed using low energy ion scattering direct recoil spectroscopy to determine any reactions of the hydrogen with the multilayer stack. Overall, the results show that the risk of over-etching with atomic hydrogen is much less than previous studies using RF discharge cleaning

Atomic resolution Z-contrast imaging and energy loss spectroscopy of carbon nanotubes and bundles

NASA Astrophysics Data System (ADS)

Lupini, A. R.; Chisholm, M. F.; Puretzky, A. A.; Eres, G.; Melechko, A. V.; Schaaff, G.; Lowndes, D. H.; Geohegan, D. B.; Schittenhelm, H.; Pennycook, S. J.; Wang, Y.; Smalley, R. E.

2002-03-01

Single-wall carbon nanotubes and bundles were studied by a combination of techniques, including conventional imaging and diffraction, atomic resolution Z-contrast imaging in an aberration corrected STEM and electron energy loss spectroscopy (EELS). EELS is ideally suited for the analysis of carbon based structures because of the ability to distinguish between the different forms, specifically nanotubes, graphite, amorphous carbon and diamond. Numerous attempts were made to synthesize crystals of single walled carbon nanotubes, using both solution and vapor deposition of precursor structures directly onto TEM grids for in-situ annealing. The range of structures produced will be discussed.

Functionalizing carbon nitride with heavy atom-free spin converters for enhanced 1 O 2 generation

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

Wu, Wenting; Han, Congcong; Zhang, Qinhua

advanced photosensitizers for singlet oxygen (1O2) generation. However, the intersystem crossing (ISC) process is quite insufficient in carbon nitride, limiting the 1O2 generation. Here, we report a facile and general strategy to confined benzophenone as a heavy atom-free spin converter dopant in carbon nitride via the facile copolymerization. With proper energy level matching between the heavy atom-free spin converter and various ligands based on carbon nitride precursors, the proper combination can decrease the singlet-triplet energy gap (DEST) and hence generate 1O2 effectively. Due to its significant and selectivity for 1O2 generation, the as-prepared carbon nitride-based photosensitizer shows a high selectivemore » photooxidation activity for 1,5-dihydroxy-naphthalene (1,5-DHN). The product yield reached 71.8% after irradiation for 60 min, which was higher than that of cyclometalated PtII complexes (53.6%) in homogeneous photooxidation. This study can broaden the application of carbon nitride in the field of selective heterogeneous photooxidation due to simple operation, low cost, and high efficiency, making it a strong candidate for future industrialization.« less

Metal atom oxidation laser

DOEpatents

Jensen, R.J.; Rice, W.W.; Beattie, W.H.

1975-10-28

A chemical laser which operates by formation of metal or carbon atoms and reaction of such atoms with a gaseous oxidizer in an optical resonant cavity is described. The lasing species are diatomic or polyatomic in nature and are readily produced by exchange or other abstraction reactions between the metal or carbon atoms and the oxidizer. The lasing molecules may be metal or carbon monohalides or monoxides.

Effect of carbon and nitrogen addition on nitrous oxide and carbon dioxide fluxes from thawing forest soils

NASA Astrophysics Data System (ADS)

Haohao, Wu; Xingkai, Xu; Cuntao, Duan; TuanSheng, Li; Weiguo, Cheng

2017-07-01

Packed soil-core incubation experiments were done to study the effects of carbon (glucose, 6.4 g C m-2) and nitrogen (NH4Cl and KNO3, 4.5 g N m-2) addition on nitrous oxide (N2O) and carbon dioxide (CO2) fluxes during thawing of frozen soils under two forest stands (broadleaf and Korean pine mixed forest and white birch forest) with two moisture levels (55 and 80% water-filled pore space). With increasing soil moisture, the magnitude and longevity of the flush N2O flux from forest soils was enhanced during the early period of thawing, which was accompanied by great NO3--N consumption. Without N addition, the glucose-induced cumulative CO2 fluxes ranged from 9.61 to 13.49 g CO2-C m-2, which was larger than the dose of carbon added as glucose. The single addition of glucose increased microbial biomass carbon but slightly affected soil dissolved organic carbon pool. Thus, the extra carbon released upon addition of glucose can result from the decomposition of soil native organic carbon. The glucose-induced N2O and CO2 fluxes were both significantly correlated to the glucose-induced total N and dissolved organic carbon pools and influenced singly and interactively by soil moisture and KNO3 addition. The interactive effects of glucose and nitrogen inputs on N2O and CO2 fluxes from forest soils after frost depended on N sources, soil moisture, and vegetation types.

The atomic scale structure of CXV carbon: wide-angle x-ray scattering and modeling studies.

PubMed

Hawelek, L; Brodka, A; Dore, J C; Honkimaki, V; Burian, A

2013-11-13

The disordered structure of commercially available CXV activated carbon produced from finely powdered wood-based carbon has been studied using the wide-angle x-ray scattering technique, molecular dynamics and density functional theory simulations. The x-ray scattering data has been converted to the real space representation in the form of the pair correlation function via the Fourier transform. Geometry optimizations using classical molecular dynamics based on the reactive empirical bond order potential and density functional theory at the B3LYP/6-31g* level have been performed to generate nanoscale models of CXV carbon consistent with the experimental data. The final model of the structure comprises four chain-like and buckled graphitic layers containing a small percentage of four-fold coordinated atoms (sp(3) defects) in each layer. The presence of non-hexagonal rings in the atomic arrangement has been also considered.

Metal atom oxidation laser

DOEpatents

Jensen, R.J.; Rice, W.W.; Beattie, W.H.

1975-10-28

A chemical laser which operates by formation of metal or carbon atoms and reaction of such atoms with a gaseous oxidizer in an optical resonant cavity is described. The lasing species are diatomic or polyatomic in nature and are readily produced by exchange or other abstraction reactions between the metal or carbon atoms and the oxidizer. The lasing molecules may be metal or carbon monohalides or monoxides. (auth)

Quantum decoherence in electronic current flowing through carbon nanotubes induced by thermal atomic vibrations

NASA Astrophysics Data System (ADS)

Ishizeki, Keisuke; Sasaoka, Kenji; Konabe, Satoru; Souma, Satofumi; Yamamoto, Takahiro

2018-06-01

We theoretically investigate quantum decoherence in electronic currents flowing through metallic carbon nanotubes caused by thermal atomic vibrations using the time-dependent Schrödinger equation for an open system. We reveal that the quantum coherence of conduction electrons decays exponentially with tube length at a fixed temperature, and that the decay rate increases with temperature. We also find that the phase relaxation length due to the thermal atomic vibrations is inversely proportional to temperature.

Self-assembly of endohedral metallofullerenes: a decisive role of cooling gas and metal–carbon bonding† †Electronic supplementary information (ESI) available: Additional information on metal–carbon bonding and MD simulations. See DOI: 10.1039/c5nr08645k Click here for additional data file.

PubMed Central

Deng, Qingming; Heine, Thomas

2016-01-01

The endohedral metallofullerene (EMF) self-assembly process in Sc/carbon vapor in the presence and absence of an inert cooling gas (helium) is systematically investigated using quantum chemical molecular dynamics simulations. It is revealed that the presence of He atoms accelerates the formation of pentagons and hexagons and reduces the size of the self-assembled carbon cages in comparison with analogous He-free simulations. As a result, the Sc/C/He system simulations produce a larger number of successful trajectories (i.e. leading to Sc-EMFs) with more realistic cage-size distribution than simulations of the Sc/C system. The main Sc encapsulation mechanism involves nucleation of several hexagons and pentagons with Sc atoms already at the early stages of carbon vapor condensation. In such proto-cages, both Sc–C σ-bonds and coordination bonds between Sc atoms and the π-system of the carbon network are present. Sc atoms are thus rather labile and can move along the carbon network, but the overall bonding is sufficiently strong to prevent dissociation even at temperatures around 2000 kelvin. Further growth of the fullerene cage results in the encapsulation of one or two Sc atoms within the fullerene. In agreement with experimental studies, an extension of the simulations to Fe and Ti as the metal component showed that Fe-EMFs are not formed at all, whereas Ti is prone to form Ti-EMFs with small cage sizes, including Ti@C28-T d and Ti@C30-C 2v(3). PMID:26815243

Activation of extended red emission photoluminescence in carbon solids by exposure to atomic hydrogen and UV radiation

NASA Technical Reports Server (NTRS)

Furton, Douglas G.; Witt, Adolf N.

1993-01-01

We report on new laboratory results which relate directly to the observation of strongly enhanced extended red emission (ERE) by interstellar dust in H2 photodissociation zones. The ERE has been attributed to photoluminescence by hydrogenated amorphous carbon (HAC). We are demonstrating that exposure to thermally dissociated atomic hydrogen will restore the photoluminescence efficiency of previously annealed HAC. Also, pure amorphous carbon (AC), not previously photoluminescent, can be induced to photoluminesce by exposure to atomic hydrogen. This conversion of AC into HAC is greatly enhanced by the presence of UV irradiation. The presence of dense, warm atomic hydrogen and a strong UV radiation field are characteristic environmental properties of H2 dissociation zones. Our results lend strong support to the HAC photoluminescence explanation for ERE.

Small angle neutron and X-ray studies of carbon structures with metal atoms

NASA Astrophysics Data System (ADS)

Lebedev, V. T.; Szhogina, A. A.; Bairamukov, V. Yu

2017-05-01

Encapsulation of metal atoms inside carbon single-wall cages or within multi-layer cells has been realized using molecular precursors and high temperature processes transforming them into desirable structures. Endohedral fullerenols Fe@C60(OH)X with 3d-metal (iron) have been studied by SANS in aqueous solutions where they form stable globular clusters with radii R C ∼ 10-12 nm and aggregation numbers N C ∼ 104. This self-assembly is a crucial feature of paramagnetic fullerenols as perspective contrast agents for Magneto-Resonance Imaging in medicine. Cellular carbon-metal structures have been created by the pyrolysis of diphthalocyanines of lanthanides and actinides. It was established that these ultra porous matrices consist of globular cells of molecular precursor size (∼ 1 nm) which are aggregated into superstructures. This provides retain of metal atoms inside matrices which may serve for safety storage of spent fuel of nuclear power plants.

The effect of defects on the catalytic activity of single Au atom supported carbon nanotubes and reaction mechanism for CO oxidation.

PubMed

Ali, Sajjad; Fu Liu, Tian; Lian, Zan; Li, Bo; Sheng Su, Dang

2017-08-23

The mechanism of CO oxidation by O 2 on a single Au atom supported on pristine, mono atom vacancy (m), di atom vacancy (di) and the Stone Wales defect (SW) on single walled carbon nanotube (SWCNT) surface is systematically investigated theoretically using density functional theory. We determine that single Au atoms can be trapped effectively by the defects on SWCNTs. The defects on SWCNTs can enhance both the binding strength and catalytic activity of the supported single Au atom. Fundamental aspects such as adsorption energy and charge transfer are elucidated to analyze the adsorption properties of CO and O 2 and co-adsorption of CO and O 2 molecules. It is found that CO binds stronger than O 2 on Au supported SWCNT. We clearly demonstrate that the defected SWCNT surface promotes electron transfer from the supported single Au atom to O 2 molecules. On the other hand, this effect is weaker for pristine SWCNTs. It is observed that the high density of spin-polarized states are localized in the region of the Fermi level due to the strong interactions between Au (5d orbital) and the adjacent carbon (2p orbital) atoms, which influence the catalytic performance. In addition, we elucidate both the Langmuir-Hinshelwood (LH) and Eley-Rideal (ER) mechanisms of CO oxidation by O 2 . For the LH pathway, the barriers of the rate-limiting step are calculated to be 0.02 eV and 0.05 eV for Au/m-SWCNT and Au/di-SWCNT, respectively. To regenerate the active sites, an ER-like reaction occurs to form a second CO 2 molecule. The ER pathway is observed on Au/m-SWCNT, Au/SW-SWCNT and Au/SWCNT in which the Au/m-SWCNT has a smaller barrier. The comparison with a previous study (Lu et al., J. Phys. Chem. C, 2009, 113, 20156-20160.) indicates that the curvature effect of SWCNTs is important for the catalytic property of the supported single Au. Overall, Au/m-SWCNT is identified as the most active catalyst for CO oxidation compared to pristine SWCNT, SW-SWCNT and di-SWCNT. Our findings give a

Carbon based thirty six atom spheres

DOEpatents

Piskoti, Charles R.; Zettl, Alex K.; Cohen, Marvin L.; Cote, Michel; Grossman, Jeffrey C.; Louie, Steven G.

2005-09-06

A solid phase or form of carbon is based on fullerenes with thirty six carbon atoms (C.sub.36). The C.sub.36 structure with D.sub.6h symmetry is one of the two most energetically favorable, and is conducive to forming a periodic system. The lowest energy crystal is a highly bonded network of hexagonal planes of C.sub.36 subunits with AB stacking. The C.sub.36 solid is not a purely van der Waals solid, but has covalent-like bonding, leading to a solid with enhanced structural rigidity. The solid C.sub.36 material is made by synthesizing and selecting out C.sub.36 fullerenes in relatively large quantities. A C.sub.36 rich fullerene soot is produced in a helium environment arc discharge chamber by operating at an optimum helium pressure (400 torr). The C.sub.36 is separated from the soot by a two step process. The soot is first treated with a first solvent, e.g. toluene, to remove the higher order fullerenes but leave the C.sub.36. The soot is then treated with a second solvent, e.g. pyridine, which is more polarizable than the first solvent used for the larger fullerenes. The second solvent extracts the C.sub.36 from the soot. Thin films and powders can then be produced from the extracted C.sub.36. Other materials are based on C.sub.36 fullerenes, providing for different properties.

The interaction of a gold atom with carbon nanohorn and carbon nanotube tips and their complexes with a CO molecule: A first principle calculation

NASA Astrophysics Data System (ADS)

Khongpracha, P.; Probst, M.; Limtrakul, J.

2008-07-01

The interactions of a gold atom with: (a) a single-wall carbon nanohorn (SWNH) conic tip; (b) with a single-wall carbon nanotube (SWNT) tip; and (c) their complexes with a CO molecule were studied using first-principle calculations based on density functional theory. The analysis of the pyramidalization angle (θp) as well as the π-orbital misalignment angles indicate that there should be many reactive carbon sites on the tips of SWNH and SWNT. It was found that SWNH provides reactive sites that can more selectively interact with the target atom. We identified five sites on both the SWNT tip and the nanohorn where attachment of a gold atom leads to a stable complex. This metal is found to be bi-coordinated with the tip of SWNH, while it is mono-coordinated with the SWNT tip. The largest interaction energies are -10.75 kcal/mol and -16.17 kcal/mol, respectively. The CO probe molecule binds to Au on the Au/SWNH or Au/SWNT tips with interaction energies of -22.34 and -18.29 kcal/mol, respectively. The main contributions of the interaction with both carbon nanostructures stems from σ-donation and π-backbonding. The results suggest that SWNHs could be one of the promising candidates for the development of high-specifity nanosensors.

Carbon atom and cluster sputtering under low-energy noble gas plasma bombardment

NASA Astrophysics Data System (ADS)

Oyarzabal, E.; Doerner, R. P.; Shimada, M.; Tynan, G. R.

2008-08-01

Exit-angle resolved carbon atom and cluster (C2 and C3) sputtering yields are measured during different noble gas (Xe, Kr, Ar, Ne, and He) ion bombardments from a plasma, for low incident energies (75-225 eV). A quadrupole mass spectrometer (QMS) is used to detect the fraction of sputtered neutrals that is ionized in the plasma and to obtain the angular distribution by changing the angle between the target normal and the QMS aperture. A one-dimensional Monte Carlo code is used to simulate the interaction of the plasma and the sputtered particles in the region between the sample and the QMS. The effective elastic scattering cross sections of C, C2, and C3 with the different bombarding gas neutrals are obtained by varying the distance between the sample and the QMS and by performing a best fit of the simulation results to the experimental results. The total sputtering yield (C+C2+C3) for each bombarding gas is obtained from weight-loss measurements and the sputtering yield for C, C2, and C3 is then calculated from the integration of the measured angular distribution, taking into account the scattering and ionization of the sputtered particles between the sample and the QMS. We observe undercosine angular distributions of the sputtered atoms and clusters for all the studied bombarding gases and a clear decrease of the atom to cluster (C2 and C3) sputtering ratio as the incident ion mass increases, changing from a carbon atom preferential erosion for the lower incident ion masses (He, Ne, and Ar) to a cluster preferential erosion for the higher incident ion masses (Kr and Xe).

Theoretical Kinetics Analysis for $$\\dot{H}$$ Atom Addition to 1,3-Butadiene and Related Reactions on the $$\\dot{C}$$ 4H 7 Potential Energy Surface

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

Li, Yang; Klippenstein, Stephen J.; Zhou, Chong-Wen

abstraction by $$\\dot{H}$$ atoms have also been calculated, and it is found that abstraction from the central carbon atoms is the dominant channel (> 70%) at temperatures in the range 298 – 2000 K. Lastly, by incorporating our calculated rate constants for both H-atom addition and abstraction into our recently developed 1,3-butadiene model, we show that laminar flame speed predictions are significantly improved, emphasizing the value of this study.« less

Self-Assembled Fe-N-Doped Carbon Nanotube Aerogels with Single-Atom Catalyst Feature as High-Efficiency Oxygen Reduction Electrocatalysts

DOE PAGES

Zhu, Chengzhou; Fu, Shaofang; Song, Junhua; ...

2017-02-06

In this study, self-assembled M–N-doped carbon nanotube aerogels with single-atom catalyst feature are for the first time reported through one-step hydrothermal route and subsequent facile annealing treatment. By taking advantage of the porous nanostructures, 1D nanotubes as well as single-atom catalyst feature, the resultant Fe–N-doped carbon nanotube aerogels exhibit excellent oxygen reduction reaction electrocatalytic performance even better than commercial Pt/C in alkaline solution.

Insights into the Electronic Structure of Ozone and Sulfur Dioxide from Generalized Valence Bond Theory: Addition of Hydrogen Atoms.

PubMed

Lindquist, Beth A; Takeshita, Tyler Y; Dunning, Thom H

2016-05-05

Ozone (O3) and sulfur dioxide (SO2) are valence isoelectronic species, yet their properties and reactivities differ dramatically. In particular, O3 is highly reactive, whereas SO2 is chemically relatively stable. In this paper, we investigate serial addition of hydrogen atoms to both the terminal atoms of O3 and SO2 and to the central atom of these species. It is well-known that the terminal atoms of O3 are much more amenable to bond formation than those of SO2. We show that the differences in the electronic structure of the π systems in the parent triatomic species account for the differences in the addition of hydrogen atoms to the terminal atoms of O3 and SO2. Further, we find that the π system in SO2, which is a recoupled pair bond dyad, facilitates the addition of hydrogen atoms to the sulfur atom, resulting in stable HSO2 and H2SO2 species.

Gas-phase reactions of carbon dioxide with atomic transition-metal and main-group cations: room-temperature kinetics and periodicities in reactivity.

PubMed

Koyanagi, Gregory K; Bohme, Diethard K

2006-02-02

The chemistry of carbon dioxide has been surveyed systematically with 46 atomic cations at room temperature using an inductively-coupled plasma/selected-ion flow tube (ICP/SIFT) tandem mass spectrometer. The atomic cations were produced at ca. 5500 K in an ICP source and allowed to cool radiatively and to thermalize by collisions with Ar and He atoms prior to reaction downstream in a flow tube in helium buffer gas at 0.35 +/- 0.01 Torr and 295 +/- 2 K. Rate coefficients and products were measured for the reactions of first-row atomic ions from K(+) to Se(+), of second-row atomic ions from Rb(+) to Te(+) (excluding Tc(+)), and of third-row atomic ions from Cs(+) to Bi(+). CO(2) was found to react in a bimolecular fashion by O atom transfer only with 9 early transition-metal cations: the group 3 cations Sc(+), Y(+), and La(+), the group 4 cations Ti(+), Zr(+), and Hf(+), the group 5 cations Nb(+) and Ta(+), and the group 6 cation W(+). Electron spin conservation was observed to control the kinetics of O atom transfer. Addition of CO(2) was observed for the remaining 37 cations. While the rate of addition was not measurable some insight was obtained into the standard free energy change, DeltaG(o), for CO(2) ligation from equilibrium constant measurements. A periodic variation in DeltaG(o) was observed for first row cations that is consistent with previous calculations of bond energies D(0)(M(+)-CO(2)). The observed trends in D(0) and DeltaG(o) are expected from the variation in electrostatic attraction between M(+) and CO(2) which follows the trend in atomic-ion size and the trend in repulsion between the orbitals of the atomic cations and the occupied orbitals of CO(2). Higher-order CO(2) cluster ions with up to four CO(2) ligands also were observed for 24 of the atomic cations while MO(2)(+) dioxide formation by sequential O atom transfer was seen only with Hf(+), Nb(+), Ta(+), and W(+).

Development of carbon electrodes for electrochemistry, solid-state electronics and multimodal atomic force microscopy imaging

NASA Astrophysics Data System (ADS)

Morton, Kirstin Claire

Carbon is one of the most remarkable elements due to its wide abundance on Earth and its many allotropes, which include diamond and graphite. Many carbon allotropes are conductive and in recent decades scientists have discovered and synthesized many new forms of carbon, including graphene and carbon nanotubes. The work in this thesis specifically focuses on the fabrication and characterization of pyrolyzed parylene C (PPC), a conductive pyrocarbon, as an electrode material for diodes, as a conductive coating for atomic force microscopy (AFM) probes and as an ultramicroelectrode (UME) for the electrochemical interrogation of cellular systems in vitro. Herein, planar and three-dimensional (3D) PPC electrodes were microscopically, spectroscopically and electrochemically characterized. First, planar PPC films and PPC-coated nanopipettes were utilized to detect a model redox species, Ru(NH3) 6Cl3. Then, free-standing PPC thin films were chemically doped, with hydrazine and concentrated nitric acid, to yield p- and n-type carbon films. Doped PPC thin films were positioned in conjunction with doped silicon to create Schottky and p-n junction diodes for use in an alternating current half-wave rectifier circuit. Pyrolyzed parylene C has found particular merit as a 3D electrode coating of AFM probes. Current sensing-atomic force microscopy imaging in air of nanoscale metallic features was undertaken to demonstrate the electronic imaging applicability of PPC AFM probes. Upon further insulation with parylene C and modification with a focused ion beam, a PPC UME was microfabricated near the AFM probe apex and utilized for electrochemical imaging. Subsequently, scanning electrochemical microscopy-atomic force microscopy imaging was undertaken to electrochemically quantify and image the spatial location of dopamine exocytotic release, elicited mechanically via the AFM probe itself, from differentiated pheochromocytoma 12 cells in vitro.

Unraveling the formation of HCPH(X2A') molecules in extraterrestrial environments: crossed molecular beam study of the reaction of carbon atoms, C(3Pj), with phosphine, PH3(X1A1).

PubMed

Guo, Y; Gu, X; Zhang, F; Sun, B J; Tsai, M F; Chang, A H H; Kaiser, R I

2007-05-03

The reaction between ground state carbon atoms, C(3P(j)), and phosphine, PH3(X(1)A1), was investigated at two collision energies of 21.1 and 42.5 kJ mol(-1) using the crossed molecular beam technique. The chemical dynamics extracted from the time-of-flight spectra and laboratory angular distributions combined with ab initio calculations propose that the reaction proceeds on the triplet surface via an addition of atomic carbon to the phosphorus atom. This leads to a triplet CPH3 complex. A successive hydrogen shift forms an HCPH2 intermediate. The latter was found to decompose through atomic hydrogen emission leading to the cis/trans-HCPH(X(2)A') reaction products. The identification of cis/trans-HCPH(X(2)A') molecules under single collision conditions presents a potential pathway to form the very first carbon-phosphorus bond in extraterrestrial environments like molecular clouds and circumstellar envelopes, and even in the postplume chemistry of the collision of comet Shoemaker-Levy 9 with Jupiter.

Revisit of the Saito-Dresselhaus-Dresselhaus C2 ingestion model: on the mechanism of atomic-carbon-participated fullerene growth.

PubMed

Wang, Wei-Wei; Dang, Jing-Shuang; Zhao, Xiang; Nagase, Shigeru

2017-11-09

We introduce a mechanistic study based on a controversial fullerene bottom-up growth model proposed by R. Saito, G. Dresselhaus, and M. S. Dresselhaus. The so-called SDD C 2 addition model has been dismissed as chemically inadmissible but here we prove that it is feasible via successive atomic-carbon-participated addition and migration reactions. Kinetic calculations on the formation of isolated pentagon rule (IPR)-obeying C 70 and Y 3 N@C 80 are carried out by employing the SDD model for the first time. A stepwise mechanism is proposed with a considerably low barrier of ca. 2 eV which is about 3 eV lower than a conventional isomerization-containing fullerene growth pathway.

PROGEN: An automated modelling algorithm for the generation of complete protein structures from the α-carbon atomic coordinates

NASA Astrophysics Data System (ADS)

Mandal, Chhabinath; Linthicum, D. Scott

1993-04-01

A modelling algorithm (PROGEN) for the generation of complete protein atomic coordinates from only the α-carbon coordinates is described. PROGEN utilizes an optimal geometry parameter (OGP) database for the positioning of atoms for each amino acid of the polypeptide model. The OGP database was established by examining the statistical correlations between 23 different intra-peptide and inter-peptide geometric parameters relative to the α-carbon distances for each amino acid in a library of 19 known proteins from the Brookhaven Protein Database (BPDB). The OGP files for specific amino acids and peptides were used to generate the atomic positions, with respect to α-carbons, for main-chain and side-chain atoms in the modelled structure. Refinement of the initial model was accomplished using energy minimization (EM) and molecular dynamics techniques. PROGEN was tested using 60 known proteins in the BPDB, representing a wide spectrum of primary and secondary structures. Comparison between PROGEN models and BPDB crystal reference structures gave r.m.s.d. values for peptide main-chain atoms between 0.29 and 0.76 Å, with a grand average of 0.53 Å for all 60 models. The r.m.s.d. for all non-hydrogen atoms ranged between 1.44 and 1.93 Å for the 60 polypeptide models. PROGEN was also able to make the correct assignment of cis- or trans-proline configurations in the protein structures examined. PROGEN offers a fully automatic building and refinement procedure and requires no special or specific structural considerations for the protein to be modelled.

Core-shell carbon nanosphere-TiO2 composite and hollow TiO2 nanospheres prepared by atomic layer deposition

NASA Astrophysics Data System (ADS)

Bakos, L. P.; Justh, N.; Hernádi, K.; Kiss, G.; Réti, B.; Erdélyi, Z.; Parditka, B.; Szilágyi, I. M.

2016-10-01

Core-shell carbon-TiO2 composite and hollow TiO2 nanospheres were prepared using carbon nanospheres as hard-templates, coating them with TiO2 using atomic layer deposition, and subsequent burning out of the carbon cores. The bare carbon, the composite carbon-TiO2 and the hollow TiO2 nanospheres were characterized with TG/DTA-MS, FTIR, XRD and SEM-EDX.

Angular distribution of photoelectrons from atomic oxygen, nitrogen and carbon. [in upper atmosphere

NASA Technical Reports Server (NTRS)

Manson, S. J.; Kennedy, D. J.; Starace, A. F.; Dill, D.

1974-01-01

The angular distributions of photoelectrons from atomic oxygen, nitrogen, and carbon are calculated. Both Hartree-Fock and Hartree-Slater (Herman-Skillman) wave functions are used for oxygen, and the agreement is excellent; thus only Hartree-Slater functions are used for carbon and nitrogen. The pitch-angle distribution of photoelectrons is discussed, and it is shown that previous approximations of energy-independent isotropic or sin squared theta distributions are at odds with the authors' results, which vary with energy. This variation with energy is discussed, as is the reliability of these calculations.

The Reception of J. H. van't Hoff's Theory of the Asymmetric Carbon Atom

ERIC Educational Resources Information Center

Snelders, H. A. M.

1974-01-01

Discusses Jacobus Henricus van't Hoff's revolutionary theory of the asymmetric carbon atom and its early reception among his contemporaries in the Netherlands. Indicates that the extension of the new idea to practical problems gives the impetus to the development of stereochemistry. (CC)

Atomic Layer Deposition on Gram Quantities of Multi-Walled Carbon Nanotubes

DTIC Science & Technology

2009-06-03

the amount of reactant that is lost to the vacuum pump . Recent work has demonstrated the feasibility of ALD on gram quantities of nanopowders in a...and left to outgas under vacuum for 24 h. Vacuum was obtained using a dual-stage rotary vane pump . Pressure was monitored with a Baratron capacitance...Atomic layer deposition on gram quantities of multi-walled carbon nanotubes This article has been downloaded from IOPscience. Please scroll down to

Direct in situ observations of single Fe atom catalytic processes and anomalous diffusion at graphene edges

PubMed Central

Zhao, Jiong; Deng, Qingming; Avdoshenko, Stanislav M.; Fu, Lei; Eckert, Jürgen; Rümmeli, Mark H.

2014-01-01

Single-atom catalysts are of great interest because of their high efficiency. In the case of chemically deposited sp2 carbon, the implementation of a single transition metal atom for growth can provide crucial insight into the formation mechanisms of graphene and carbon nanotubes. This knowledge is particularly important if we are to overcome fabrication difficulties in these materials and fully take advantage of their distinct band structures and physical properties. In this work, we present atomically resolved transmission EM in situ investigations of single Fe atoms at graphene edges. Our in situ observations show individual iron atoms diffusing along an edge either removing or adding carbon atoms (viz., catalytic action). The experimental observations of the catalytic behavior of a single Fe atom are in excellent agreement with supporting theoretical studies. In addition, the kinetics of Fe atoms at graphene edges are shown to exhibit anomalous diffusion, which again, is in agreement with our theoretical investigations. PMID:25331874

Decomposition of the fluoroethylene carbonate additive and the glue effect of lithium fluoride products for the solid electrolyte interphase: an ab initio study.

PubMed

Okuno, Yukihiro; Ushirogata, Keisuke; Sodeyama, Keitaro; Tateyama, Yoshitaka

2016-03-28

Additives in the electrolyte solution of lithium-ion batteries (LIBs) have a large impact on the performance of the solid electrolyte interphase (SEI) that forms on the anode and is a key to the stability and durability of LIBs. We theoretically investigated effects of fluoroethylene carbonate (FEC), a representative additive, that has recently attracted considerable attention for the enhancement of cycling stability of silicon electrodes and the improvement of reversibility of sodium-ion batteries. First, we intensively examined the reductive decompositions by ring-opening, hydrogen fluoride (HF) elimination to form a vinylene carbonate (VC) additive and intermolecular chemical reactions of FEC in the ethylene carbonate (EC) electrolyte, by using density functional theory (DFT) based molecular dynamics and the blue-moon ensemble technique for the free energy profile. The results show that the most plausible product of the FEC reductive decomposition is lithium fluoride (LiF), and that the reactivity of FEC to anion radicals is found to be inert compared to the VC additive. We also investigated the effects of the generated LiF on the SEI by using two model systems; (1) LiF molecules distributed in a model aggregate of organic SEI film components (SFCs) and (2) a LiF aggregate interfaced with the SFC aggregate. DFT calculations of the former system show that F atoms form strong bindings with the Li atoms of multiple organic SFC molecules and play as a joint connecting them. In the latter interface system, the LiF aggregate adsorbs the organic SFCs through the F-Li bindings. These results suggest that LiF moieties play the role of glue in the organic SFC within the SEI film. We also examined the interface structure between a LiF aggregate and a lithiated silicon anode, and found that they are strongly bound. This strong binding is likely to be related to the effectiveness of the FEC additive in the electrolyte for the silicon anode.

Diamond like carbon coatings: Categorization by atomic number density

NASA Technical Reports Server (NTRS)

Angus, John C.

1986-01-01

Dense diamond-like hydrocarbon films grown at the NASA Lewis Research Center by radio frequency self bias discharge and by direct ion beam deposition were studied. A new method for categorizing hydrocarbons based on their atomic number density and elemental composition was developed and applied to the diamond-like hydrocarbon films. It was shown that the diamond-like hydrocarbon films are an entirely new class of hydrocarbons with atomic number densities lying between those of single crystal diamond and adamantanes. In addition, a major review article on these new materials was completed in cooperation with NASA Lewis Research Center personnel.

Ionized Carbon Atoms in Orion

NASA Image and Video Library

2016-10-12

The dusty side of the Sword of Orion is illuminated in this striking infrared image from the European Space Agency's Hershel Space Observatory. This immense nebula is the closest large region of star formation, situated about 1,500 light years away in the constellation of Orion. The parts that are easily observed in visible light, known alternatively as the Orion Nebula or Messier 42, correspond to the light blue regions. This is the glow from the warmest dust, illuminated by clusters of hot stars that have only recently been born in this chaotic region. The red spine of material running from corner to corner reveals colder, denser filaments of dust and gas that are scattered throughout the Orion nebula. In visible light this would be a dark, opaque feature, hiding the reservoir of material from which stars have recently formed and will continue to form in the future. Herschel data from the PACS instrument observations, at wavelengths of 100 and 160 microns, is displayed in blue and green, respectively, while SPIRE 250-micron data is shown in red. Within the inset image, the emission from ionized carbon atoms (C+), overlaid in yellow, was isolated and mapped out from spectrographic data obtained by the HIFI instrument. http://photojournal.jpl.nasa.gov/catalog/PIA21073

Influence of carbon conductive additives on electrochemical double-layer supercapacitor parameters

NASA Astrophysics Data System (ADS)

Kiseleva, E. A.; Zhurilova, M. A.; Kochanova, S. A.; Shkolnikov, E. J.; Tarasenko, A. B.; Zaitseva, O. V.; Uryupina, O. V.; Valyano, G. V.

2018-01-01

Electrochemical double-layer capacitors (EDLC) offer energy storage technology, highly demanded for rapid transition processes in transport and stationary applications, concerned with fast power fluctuations. Rough structure of activated carbon, widely used as electrode material because of its high specific area, leads to poor electrode conductivity. Therefore there is the need for conductive additive to decrease internal resistance and to achieve high specific power and high specific energy. Usually carbon blacks are widely used as conductive additive. In this paper electrodes with different conductive additives—two types of carbon blacks and single-walled carbon nanotubes—were prepared and characterized in organic electrolyte-based EDLC cells. Electrodes are based on original wood derived activated carbon produced by potassium hydroxide high-temperature activation at Joint Institute for High Temperatures RAS. Electrodes were prepared from slurry by cold-rolling. For electrode characterization cyclic voltammetry, impedance spectra analysis, equivalent series resistance measurements and galvanostatic charge-discharge were used.

The Kinetics of Oxygen Atom Recombination in the Presence of Carbon Dioxide

NASA Astrophysics Data System (ADS)

Jamieson, C. S.; Garcia, R. M.; Pejakovic, D.; Kalogerakis, K.

2009-12-01

Understanding processes involving atomic oxygen is crucial for the study and modeling of composition, energy transfer, airglow, and transport dynamics in planetary atmospheres. Significant gaps and uncertainties exist in the understanding of these processes and often the relevant input from laboratory measurements is missing or outdated. We are conducting laboratory experiments to measure the rate coefficient for O + O + CO2 recombination and investigating the O2 excited states produced following the recombination. These measurements will provide key input for a quantitative understanding and reliable modeling of the atmospheres of the CO2 planets and their airglow. An excimer laser providing pulsed output at either 193 nm or 248 nm is employed to produce O atoms by dissociating carbon dioxide, nitrous oxide, or ozone. In an ambient-pressure background of CO2, O atoms recombine in a time scale of a few milliseconds. Detection of laser-induced fluorescence at 845 nm following two-photon excitation near 226 nm monitors the decay of the oxygen atom population. From the temporal evolution of the signal the recombination rate coefficient is extracted. Fluorescence spectroscopy is used to detect the products of O-atom recombination and subsequent relaxation in CO2. This work is supported by the US National Science Foundation’s (NSF) Planetary Astronomy Program. Rosanne Garcia’s participation was funded by the NSF Research Experiences for Undergraduates (REU) Program.

Rational Design of Single Molybdenum Atoms Anchored on N-Doped Carbon for Effective Hydrogen Evolution Reaction.

PubMed

Chen, Wenxing; Pei, Jiajing; He, Chun-Ting; Wan, Jiawei; Ren, Hanlin; Zhu, Youqi; Wang, Yu; Dong, Juncai; Tian, Shubo; Cheong, Weng-Chon; Lu, Siqi; Zheng, Lirong; Zheng, Xusheng; Yan, Wensheng; Zhuang, Zhongbin; Chen, Chen; Peng, Qing; Wang, Dingsheng; Li, Yadong

2017-12-11

The highly efficient electrochemical hydrogen evolution reaction (HER) provides a promising pathway to resolve energy and environment problems. An electrocatalyst was designed with single Mo atoms (Mo-SAs) supported on N-doped carbon having outstanding HER performance. The structure of the catalyst was probed by aberration-corrected scanning transmission electron microscopy (AC-STEM) and X-ray absorption fine structure (XAFS) spectroscopy, indicating the formation of Mo-SAs anchored with one nitrogen atom and two carbon atoms (Mo 1 N 1 C 2 ). Importantly, the Mo 1 N 1 C 2 catalyst displayed much more excellent activity compared with Mo 2 C and MoN, and better stability than commercial Pt/C. Density functional theory (DFT) calculation revealed that the unique structure of Mo 1 N 1 C 2 moiety played a crucial effect to improve the HER performance. This work opens up new opportunities for the preparation and application of highly active and stable Mo-based HER catalysts. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Direct assessment of the metabolic origin of carbon atoms in glutamate from illuminated leaves using 13 C-NMR.

PubMed

Abadie, Cyril; Lothier, Jérémy; Boex-Fontvieille, Edouard; Carroll, Adam; Tcherkez, Guillaume

2017-12-01

Glutamate (Glu) is the cornerstone of nitrogen assimilation and photorespiration in illuminated leaves. Despite this crucial role, our knowledge of the flux to Glu de novo synthesis is rather limited. Here, we used isotopic labelling with 13 CO 2 and 13 C-NMR analyses to examine the labelling pattern and the appearance of multi-labelled species of Glu molecules to trace the origin of C-atoms found in Glu. We also compared this with 13 C-labelling patterns in Ala and Asp, which reflect citrate (and thus Glu) precursors, that is, pyruvate and oxaloacetate. Glu appeared to be less 13 C-labelled than Asp and Ala, showing that the Glu pool was mostly formed by 'old' carbon atoms. There were modest differences in intramolecular 13 C- 13 C couplings between Glu C-2 and Asp C-3, showing that oxaloacetate metabolism to Glu biosynthesis did not involve C-atom redistribution by the Krebs cycle. The apparent carbon allocation increased with carbon net photosynthesis. However, when expressed relative to CO 2 fixation, it was clearly higher at low CO 2 while it did not change in 2% O 2 , as compared to standard conditions. We conclude that Glu production from current photosynthetic carbon represents a small flux that is controlled by the gaseous environment, typically upregulated at low CO 2 . © 2017 The Authors. New Phytologist © 2017 New Phytologist Trust.

Hydrogen atom addition to the surface of graphene nanoflakes: A density functional theory study

NASA Astrophysics Data System (ADS)

Tachikawa, Hiroto

2017-02-01

Polycyclic aromatic hydrocarbons (PAHs) provide a 2-dimensional (2D) reaction surface in 3-dimensional (3D) interstellar space and have been utilized as a model of graphene surfaces. In the present study, the reaction of PAHs with atomic hydrogen was investigated by means of density functional theory (DFT) to systematically elucidate the binding nature of atomic hydrogen to graphene nanoflakes. PAHs with n = 4-37 were chosen, where n indicates the number of benzene rings. Activation energies of hydrogen addition to the graphene surface were calculated to be 5.2-7.0 kcal/mol at the CAM-B3LYP/6-311G(d,p) level, which is almost constant for all PAHs. The binding energies of hydrogen atom were slightly dependent on the size (n): 14.8-28.5 kcal/mol. The absorption spectra showed that a long tail is generated at the low-energy region after hydrogen addition to the graphene surface. The electronic states of hydrogenated graphenes were discussed on the basis of theoretical results.

Photochemical Escape of Atomic Carbon from Mars

NASA Astrophysics Data System (ADS)

Fox, J. L.; Hac, A. B.

2009-12-01

Determining the escape rate of C over time is necessary to reconstructing the time-dependent history of volatiles on Mars. We report initial results from a one-dimensional spherical Monte Carlo calculation of photochemical escape fluxes and rates of atomic carbon from the Martian atmosphere. This model has recently been used to estimate the photochemical escape flux of O from Mars. We include as sources photodissociation of CO, dissociative recombination of CO+, photoelectron-impact dissociation of CO, photodissociative ionization and photoelectron impact dissociative ionization. Dissociative recombination of CO2+ has been suggested as a source of C (in the channel that produces C + O2) but later studies have found that the yield of this channel is negligible. We test the potential importance of this reaction by comparing the final results produced by including it and excluding it. Finally we compare the range of the escape rate to that of C in ions that have been modeled or measured by ASPERA instruments on MEX and Phobos.

Adsorption properties of carbon dioxide enchanced oil recovery additives

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

Patton, J.T.; Holbrook, S.T.

1990-01-01

The selection of the optimum foaming agent (surfactant) for enhancing oil production by carbon dioxide flooding is based on foamability and adsorption. Measurements of adsorption on carbonate cores from New Mexico reservoirs showed large adsorption differences between three commercial, high-foaming surfactants. An ethoxylated alcohol structure was at least adsorbed, 0.64 mg/cc pore volume; an ethoxylated alcohol sulfate was next, 0.74 mg/cc pore volume; the highest adsorbed was a glyceryl sulfonate, 2.30 mg/cc pore volume. Commercial application of the foaming additive involves injecting alternate slugs of surfactant solution and carbon dioxide. Surfactant concentration should be determined to allow for the adsorptionmore » above. 9 refs., 27 figs., 6 tabs.« less

Specific Adaptation of Gas Atomization Processing for Al-Based Alloy Powder for Additive Manufacturing

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

Anderson, Iver; Siemon, John

The initial three atomization attempts resulted in “freeze-outs” within the pour tubes in the pilot-scale system and yielded no powder. Re-evaluation of the alloy liquidus temperatures and melting characteristics, in collaboration with Alcoa, showed further superheat to be necessary to allow the liquid metal to flow through the pour tube to the atomization nozzle. A subsequent smaller run on the experimental atomization system verified these parameters and was successful, as were all successive runs on the larger pilot scale system. One alloy composition froze-out part way through the atomization on both pilot scale runs. SEM images showed needle formation andmore » phase segregations within the microstructure. Analysis of the pour tube freeze-out microstructures showed that large needles formed within the pour tube during the atomization experiment, which eventually blocked the melt stream. Alcoa verified the needle formation in this alloy using theoretical modeling of phase solidification. Sufficient powder of this composition was still generated to allow powder characterization and additive manufacturing trials at Alcoa.« less

Enhancement of neutron radiation dose by the addition of sulphur-33 atoms.

PubMed

Porras, I

2008-04-07

The use of neutrons in radiotherapy allows the possibility of producing nuclear reactions in a specific target inserted in the medium. (10)B is being used to induce reactions (n, alpha), a technique called boron neutron capture therapy. I have studied the possibility of inducing a similar reaction using the nucleus of (33)S, for which the reaction cross section presents resonances for keV neutrons, the highest peak occurring at 13.5 keV. Here shown, by means of Monte Carlo simulation of point-like sources of neutrons in this energy range, is an enhancement effect on the absorbed dose in water by the addition of (33)S atoms. In addition to this, as the range of the alpha particle is of the order of a mammalian cell size, the energy deposition via this reaction results mainly inside the cells adjacent to the interaction site. The main conclusion of the present work is that the insertion of these sulphur atoms in tumoral cells would enhance the effect of neutron irradiation in the keV range.

Fullerene-like chemistry at the interior carbon atoms of an alkene-centered C26H12 geodesic polyarene.

PubMed

Bronstein, Hindy E; Scott, Lawrence T

2008-01-04

The title compound (1) undergoes 1,2-addition reactions of both electrophilic and nucleophilic reagents preferentially at the "interior" carbon atoms of the central 6:6-bond to give fullerene-type adducts 2, 3, 4, and 5. Such fullerene-like chemistry is unprecedented for a topologically 2-dimensional polycyclic aromatic hydrocarbon and qualifies this geodesic polyarene as a "bridge" between the old flat world of polycyclic aromatic hydrocarbons (PAHs) and the new round world of fullerenes. The relief of pyramidalization strain, as in the addition reactions of fullerenes, presumably contributes to the atypical mode of reactivity seen in 1. Molecular orbital calculations, however, reveal features of the nonalternant pi system in 1 that may also play an important role. Thus, the fullerene-like chemistry of 1 may be driven by two or more factors, the relative importances of which are difficult to discern.

Roles of additives and surface control in slurry atomization

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

Tsai, S.C.

1990-01-01

This report focuses on the effects of interparticle forces on the rheology and airblast atomization of micronized coal water slurry (CWS). We found that the CWS flow behavior index is determined by the relative importance of the interparticle van der Waals attraction and the interparticle electrostatic repulsion. The former intensifies as the Hamaker constant increases and the interparticle distance reduces while the latter increases as the particle surface charge density increases. The interparticle attraction causes particle aggregation, which breaks down at high shear rates, and thus leads to slurry pseudoplastic behavior. In contrast, the interparticle repulsion prevents particle aggregation andmore » thus leads to Newtonian behavior. Both atomized at low atomizing air pressures (less than 270 kPa) using twin-fluid jet atomizers of various distributor designs. We found that the atomized drop sizes of micronized coal water slurries substantially decrease as the atomizing air pressure exceeds a threshold value. The effects of coal volume fraction, coal particle surface charge, liquid composition and liquid viscosity on slurry atomization can be accounted for by their effects on slurry rheology. 26 refs.« less

Specific Adaptation of Gas Atomization Processing for Al-Based Alloy Powder for Additive Manufacturing

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

Anderson, Iver; Siemon, John

The charge for each gas atomization experiment was provided by Alcoa and consisted of cast blocks cut into 1 inch by 1 inch square rods of the chosen aluminum alloys. The atmosphere in the melting chamber and connected atomization system was evacuated with a mechanical pump prior to backfilling with ultrahigh purity (UHP grade) Ar. The melt was contained in a bottom tapped alumina crucible with an alumina stopper rod to seal the exit while heating to a pouring temperature of 1000 – 1400°C. When the desired superheat was reached, the stopper rod was lifted and melt flowed through pourmore » tube and was atomized with Ar from a 45-22-052-409 gas atomization nozzle (or atomization die), having a jet apex angle of 45 degrees with 22 cylindrical gas jets (each with diameter of 1.32 mm or 0.052 inches) arrayed around the axis of a 10.4 mm central bore. The Ar atomization gas supply regulator pressure was set to produce nozzle manifold pressures for the series of runs at pressures of 250-650 psi. Secondary gas halos of Ar+O 2 and He also were added to the interior of the spray chamber at various downstream locations for additional cooling of the atomized droplets, surface passivation, and to prevent coalescence of the resulting powder.« less

Carbon Nanotube Chopped Fiber for Enhanced Properties in Additive Manufacturing

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

Menchhofer, Paul A.; Johnson, Joseph E.; Lindahl, John M.

2016-06-06

Nanocomp Technologies, Inc. is working with Oak Ridge National Laboratory to develop carbon nanotube (CNT) composite materials and evaluate their use in additive manufacturing (3D printing). The first phase demonstrated feasibility and improvements for carbon nanotube (CNT)- acrylonitrile butadiene styrene (ABS) composite filaments use in additive manufacturing, with potential future work centering on further improvements. By focusing the initial phase on standard processing methods (developed mainly for the incorporation of carbon fibers in ABS) and characterization techniques, a basis of knowledge for the incorporation of CNTs in ABS was learned. The ability to understand the various processing variables is criticalmore » to the successful development of these composites. From the degradation effects on ABS (caused by excessive temperatures), to the length of time the ABS is in the melt state, to the order of addition of constituents, and also to the many possible mixing approaches, a workable flow sequence that addresses each processing step is critical to the final material properties. Although this initial phase could not deal with each of these variables in-depth, a future study is recommended that will build on the lessons learned for this effort.« less

Understanding Function and Performance of Carbon Additives in Lead-Acid Batteries

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

Enos, D. G.; Ferreira, S. R.; Barkholtz, H. M.

While the low cost and strong safety record of lead-acid batteries make them an appealing option compared to lithium-ion technologies for stationary storage, they can be rapidly degraded by the extended periods of high rate, partial state-of-charge operation required in such applications. Degradation occurs primarily through a process called hard sulfation, where large PbSO 4 crystals are formed on the negative battery plates, hindering charge acceptance and reducing battery capacity. Various researchers have found that the addition of some forms of excess carbon to the negative active mass in lead-acid batteries can mitigate hard sulfation, but the mechanism through whichmore » this is accomplished is unclear. In this work, the effect of carbon composition and morphology was explored by characterizing four discrete types of carbon additives, then evaluating their effect when added to the negative electrodes within a traditional valve-regulated lead-acid battery design. The cycle life for the carbon modified cells was significantly larger than an unmodified control, with cells containing a mixture of graphitic carbon and carbon black yielding the greatest improvement. The carbons also impacted other electrochemical aspects of the battery (e.g., float current, capacity, etc.) as well as physical characteristics of the negative active mass, such as the specific surface area.« less

Understanding Function and Performance of Carbon Additives in Lead-Acid Batteries

DOE PAGES

Enos, D. G.; Ferreira, S. R.; Barkholtz, H. M.; ...

2017-10-31

While the low cost and strong safety record of lead-acid batteries make them an appealing option compared to lithium-ion technologies for stationary storage, they can be rapidly degraded by the extended periods of high rate, partial state-of-charge operation required in such applications. Degradation occurs primarily through a process called hard sulfation, where large PbSO 4 crystals are formed on the negative battery plates, hindering charge acceptance and reducing battery capacity. Various researchers have found that the addition of some forms of excess carbon to the negative active mass in lead-acid batteries can mitigate hard sulfation, but the mechanism through whichmore » this is accomplished is unclear. In this work, the effect of carbon composition and morphology was explored by characterizing four discrete types of carbon additives, then evaluating their effect when added to the negative electrodes within a traditional valve-regulated lead-acid battery design. The cycle life for the carbon modified cells was significantly larger than an unmodified control, with cells containing a mixture of graphitic carbon and carbon black yielding the greatest improvement. The carbons also impacted other electrochemical aspects of the battery (e.g., float current, capacity, etc.) as well as physical characteristics of the negative active mass, such as the specific surface area.« less

Performance evaluation of different diamond-like carbon samples as charge state conversion surfaces for neutral atom imaging detectors in space applications

NASA Astrophysics Data System (ADS)

Brigitte Neuland, Maike; Allenbach, Marc; Föhn, Martina; Wurz, Peter

2017-04-01

sample [6] to our latest measurements of a Boron-doped CVD diamond sample. We additionally measured the B-concentration in the sample to prove our predictions of the B-concentration needed to reach sufficient conductibility for the sample not getting electrostatically charged during instrument operation. The results of narrower scattering cones and higher ionisation efficiency show that diamond-like carbon still is the preferred material for charge state conversion surfaces and that new surface technologies offer improved diamond conversion surfaces with different properties and hence the possibility for improvement of the performance of neutral atom imaging instruments. References: [1] P. Wurz, Detection of Energetic Neutral Atoms, in The Outer Heliosphere: Beyond the Planets, Copernicus Gesellschaft e.V., Katlenburg-Lindau, Germany, 2000, p. 251-288. [2] P. Wurz, R. Schletti, M.R. Aellig, Surf. Sci. 373(1997), 56-66. [3] D.J. McComas et al., Geophys. Res. Lett. 38(2011), L18101. [4] N.A. Schwadron et al., J. of Phys.. Conf. Series 767(2016): 012025 [5] P. Wahlström, J.A. Scheer, A. Riedo, P. Wurz and M. Wieser, J. Spacecr. Rockets 50 (2013): 402-410. [6] M.B. Neuland, J.A. Scheer, A. Riedo and P. Wurz, Appl. Surf. Sci. 313(2014):293-303.

Model studies of hydrogen atom addition and abstraction processes involving ortho-, meta-, and para-benzynes.

PubMed

Clark, A E; Davidson, E R

2001-10-31

H-atom addition and abstraction processes involving ortho-, meta-, and para-benzyne have been investigated by multiconfigurational self-consistent field methods. The H(A) + H(B)...H(C) reaction (where r(BC) is adjusted to mimic the appropriate singlet-triplet energy gap) is shown to effectively model H-atom addition to benzyne. The doublet multiconfiguration wave functions are shown to mix the "singlet" and "triplet" valence bond structures of H(B)...H(C) along the reaction coordinate; however, the extent of mixing is dependent on the singlet-triplet energy gap (DeltaE(ST)) of the H(B)...H(C) diradical. Early in the reaction, the ground-state wave function is essentially the "singlet" VB function, yet it gains significant "triplet" VB character along the reaction coordinate that allows H(A)-H(B) bond formation. Conversely, the wave function of the first excited state is predominantly the "triplet" VB configuration early in the reaction coordinate, but gains "singlet" VB character when the H-atom is close to a radical center. As a result, the potential energy surface (PES) for H-atom addition to triplet H(B)...H(C) diradical is repulsive! The H3 model predicts, in agreement with the actual calculations on benzyne, that the singlet diradical electrons are not coupled strongly enough to give rise to an activation barrier associated with C-H bond formation. Moreover, this model predicts that the PES for H-atom addition to triplet benzyne will be characterized by a repulsive curve early in the reaction coordinate, followed by a potential avoided crossing with the (pi)1(sigma*)1 state of the phenyl radical. In contrast to H-atom addition, large activation barriers characterize the abstraction process in both the singlet ground state and first triplet state. In the ground state, this barrier results from the weakly avoided crossing of the dominant VB configurations in the ground-state singlet (S0) and first excited singlet (S1) because of the large energy gap between S0

Chemical and biological consequences of using carbon dioxide versus acid additions in ocean acidification experiments

USGS Publications Warehouse

Yates, Kimberly K.; DuFore, Christopher M.; Robbins, Lisa L.

2013-01-01

Use of different approaches for manipulating seawater chemistry during ocean acidification experiments has confounded comparison of results from various experimental studies. Some of these discrepancies have been attributed to whether addition of acid (such as hydrochloric acid, HCl) or carbon dioxide (CO2) gas has been used to adjust carbonate system parameters. Experimental simulations of carbonate system parameter scenarios for the years 1766, 2007, and 2100 were performed using the carbonate speciation program CO2SYS to demonstrate the variation in seawater chemistry that can result from use of these approaches. Results showed that carbonate system parameters were 3 percent and 8 percent lower than target values in closed-system acid additions, and 1 percent and 5 percent higher in closed-system CO2 additions for the 2007 and 2100 simulations, respectively. Open-system simulations showed that carbonate system parameters can deviate by up to 52 percent to 70 percent from target values in both acid addition and CO2 addition experiments. Results from simulations for the year 2100 were applied to empirically derived equations that relate biogenic calcification to carbonate system parameters for calcifying marine organisms including coccolithophores, corals, and foraminifera. Calculated calcification rates for coccolithophores, corals, and foraminifera differed from rates at target conditions by 0.5 percent to 2.5 percent in closed-system CO2 gas additions, from 0.8 percent to 15 percent in the closed-system acid additions, from 4.8 percent to 94 percent in open-system acid additions, and from 7 percent to 142 percent in open-system CO2 additions.

Intramolecular addition of benzylic radicals onto ketenimines. Synthesis of 2-alkylindoles.

PubMed

Alajarín, Mateo; Vidal, Angel; Ortín, María-Mar

2003-12-07

The inter- and intramolecular addition of free radicals onto ketenimines is studied. All the attempts to add intermolecularly several silicon, oxygen or carbon centered radicals to N-(4-methylphenyl)-C,C-diphenyl ketenimine were unsuccessful. In contrast, the intramolecular addition of benzylic radicals, generated from xanthates, onto the central carbon of a ketenimine function with its N atom linked to the ortho position of the aromatic ring occurred under a variety of reaction conditions. These intramolecular cyclizations provide a novel radical-mediated synthesis of 2-alkylindoles.

Structural modifications of graphyne layers consisting of carbon atoms in the sp- and sp{sup 2}-hybridized states

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

Belenkov, E. A., E-mail: belenkov@csu.ru; Mavrinskii, V. V.; Belenkova, T. E.

2015-05-15

A model scheme is proposed for obtaining layered compounds consisting of carbon atoms in the sp- and (vnsp){sup 2}-hybridized states. This model is used to find the possibility of existing the following seven basic structural modifications of graphyne: α-, β1-, β2-, β3-, γ1-, γ2-, and γ3-graphyne. Polymorphic modifications β3 graphyne and γ3 graphyne are described. The basic structural modifications of graphyne contain diatomic polyyne chains and consist only of carbon atoms in two different crystallographically equivalent states. Other nonbasic structural modifications of graphyne can be formed via the elongation of the carbyne chains that connect three-coordinated carbon atoms and viamore » the formation of graphyne layers with a mixed structure consisting of basic layer fragments, such as α-β-graphyne, α-γ-graphyne, and β-γ-graphyne. The semiempirical quantum-mechanical MNDO, AM1, and PM3 methods and ab initio STO6-31G basis calculations are used to find geometrically optimized structures of the basic graphyne layers, their structural parameters, and energies of their sublimation. The energy of sublimation is found to be maximal for γ2-graphyne, which should be the most stable structural modification of graphyne.« less

Direct determination and speciation of mercury compounds in environmental and biological samples by carbon bed atomic absorption spectroscopy

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

Skelly, E.M.

A method was developed for the direct determination of mercury in water and biological samples using a unique carbon bed atomizer for atomic absorption spectroscopy. The method avoided sources of error such as loss of volatile mercury during sample digestion and contamination of samples through added reagents by eliminating sample pretreatment steps. The design of the atomizer allowed use of the 184.9 nm mercury resonance line in the vacuum ultraviolet region, which increased sensitivity over the commonly used spin-forbidden 253.7 nm line. The carbon bed atomizer method was applied to a study of mercury concentrations in water, hair, sweat, urine,more » blood, breath and saliva samples from a non-occupationally exposed population. Data were collected on the average concentration, the range and distribution of mercury in the samples. Data were also collected illustrating individual variations in mercury concentrations with time. Concentrations of mercury found were significantly higher than values reported in the literature for a ''normal'' population. This is attributed to the increased accuracy gained by eliminating pretreatment steps and increasing atomization efficiency. Absorption traces were obtained for various solutions of pure and complexed mercury compounds. Absorption traces of biological fluids were also obtained. Differences were observed in the absorption-temperatures traces of various compounds. The utility of this technique for studying complexation was demonstrated.« less

Additive manufacturing of magnetic shielding and ultra-high vacuum flange for cold atom sensors.

PubMed

Vovrosh, Jamie; Voulazeris, Georgios; Petrov, Plamen G; Zou, Ji; Gaber, Youssef; Benn, Laura; Woolger, David; Attallah, Moataz M; Boyer, Vincent; Bongs, Kai; Holynski, Michael

2018-01-31

Recent advances in the understanding and control of quantum technologies, such as those based on cold atoms, have resulted in devices with extraordinary metrological performance. To realise this potential outside of a lab environment the size, weight and power consumption need to be reduced. Here we demonstrate the use of laser powder bed fusion, an additive manufacturing technique, as a production technique relevant to the manufacture of quantum sensors. As a demonstration we have constructed two key components using additive manufacturing, namely magnetic shielding and vacuum chambers. The initial prototypes for magnetic shields show shielding factors within a factor of 3 of conventional approaches. The vacuum demonstrator device shows that 3D-printed titanium structures are suitable for use as vacuum chambers, with the test system reaching base pressures of 5 ± 0.5 × 10 -10 mbar. These demonstrations show considerable promise for the use of additive manufacturing for cold atom based quantum technologies, in future enabling improved integrated structures, allowing for the reduction in size, weight and assembly complexity.

The effects of atomic oxygen on the thermal emittance of high temperature radiator surfaces

NASA Technical Reports Server (NTRS)

Rutledge, Sharon K.; Hotes, Deborah L.; Paulsen, Phillip E.

1989-01-01

Radiator surfaces on high temperature space power systems such as SP-100 space nuclear power system must maintain a high emittance level in order to reject waste heat effectively. One of the primary materials under consideration for the radiators is carbon-carbon composite. Since carbon is susceptible to attack by atomic oxygen in the low earth orbital environment, it is important to determine the durability of carbon composites in this environment as well as the effect atomic oxygen has on the thermal emittance of the surface if it is to be considered for use as a radiator. Results indicate that the thermal emittance of carbon-carbon composite (as low as 0.42) can be enhanced by exposure to a directed beam of atomic oxygen to levels above 0.85 at 800 K. This emittance enhancement is due to a change in the surface morphology as a result of oxidation. High aspect ratio cones are formed on the surface which allow more efficient trapping of incident radiation. Erosion of the surface due to oxidation is similar to that for carbon, so that at altitudes less than approximately 600 km, thickness loss of the radiator could be significant (as much as 0.1 cm/year). A protective coating or oxidation barrier forming additive may be needed to prevent atomic oxygen attack after the initial high emittance surface is formed. Textured surfaces can be formed in ground based facilities or possibly in space if emittance is not sensitive to the orientation of the atomic oxygen arrival that forms the texture.

Selective determination of arsenic(III) and arsenic(V) with ammonium pyrrolidinedithiocarbamate, sodium diethyldithiocarbamate and dithizone by means of flameless atomic-absorption spectrophotometry with a carbon-tube atomizer.

PubMed

Kamada, T

The extraction behaviour of arsenic(III) and arsenic(V) with ammonium pyrrolidinedithiocarbamate, sodium diethyldithiocarbamate and dithizone in organic solvents has been investigated by means of nameless atomic-absorption spectrophotometry with a carbon-tube atomizer. The selective extraction of arsenic(III) and differential determination of arsenic(III) and arsenic(V) have been developed. With ammonium pyrrolidinedithiocarbamate and methyl isobutyl ketone or nitrobenzene, when the aqueous phase/solvent volume ratio is 5 and the injection volume in the carbon tube is 20 mul, the sensitivities for 1% absorption are 0.4 and 0.5 part per milliard of arsenic, respectively. The relative standard deviations are ca. 3%. Interference by many metal ions can be prevented by masking with EDTA. The proposed methods are applied satisfactorily for determination of As(III) and As(V) in various types of water.

Interaction between single gold atom and the graphene edge: A study via aberration-corrected transmission electron microscopy

NASA Astrophysics Data System (ADS)

Wang, Hongtao; Li, Kun; Cheng, Yingchun; Wang, Qingxiao; Yao, Yingbang; Schwingenschlögl, Udo; Zhang, Xixiang; Yang, Wei

2012-04-01

Interaction between single noble metal atoms and graphene edges has been investigated via aberration-corrected and monochromated transmission electron microscopy. A collective motion of the Au atom and the nearby carbon atoms is observed in transition between energy-favorable configurations. Most trapping and detrapping processes are assisted by the dangling carbon atoms, which are more susceptible to knock-on displacements by electron irradiation. Thermal energy is lower than the activation barriers in transition among different energy-favorable configurations, which suggests electron-beam irradiation can be an efficient way of engineering the graphene edge with metal atoms.Interaction between single noble metal atoms and graphene edges has been investigated via aberration-corrected and monochromated transmission electron microscopy. A collective motion of the Au atom and the nearby carbon atoms is observed in transition between energy-favorable configurations. Most trapping and detrapping processes are assisted by the dangling carbon atoms, which are more susceptible to knock-on displacements by electron irradiation. Thermal energy is lower than the activation barriers in transition among different energy-favorable configurations, which suggests electron-beam irradiation can be an efficient way of engineering the graphene edge with metal atoms. Electronic supplementary information (ESI) available: Additional Figures for characterization of mono-layer CVD graphene samples with free edges and Pt atoms decorations and analysis of the effect of electron irradiation; supporting movie on edge evolution. See DOI: 10.1039/c2nr00059h

Effects of labile carbon addition on a headwater stream food web

Treesearch

Heidi S. Wilcox; J. Bruce Wallace; Judy L. Meyer; Jonathan P. Benstead

2005-01-01

We added dextrose for two 8-week periods (summer and autumn) to a highly heterotrophic headwater stream in North Carolina, U.S.A., to examine the responses of its benthic food web to increased labile carbon. We hypothesized that addition of labile carbon would elevate microbial abundance and activity, resulting in greater resource availability and higher...

Atomic Covalent Functionalization of Graphene

PubMed Central

Johns, James E.; Hersam, Mark C.

2012-01-01

Conspectus Although graphene’s physical structure is a single atom thick, two-dimensional, hexagonal crystal of sp2 bonded carbon, this simple description belies the myriad interesting and complex physical properties attributed to this fascinating material. Because of its unusual electronic structure and superlative properties, graphene serves as a leading candidate for many next generation technologies including high frequency electronics, broadband photodetectors, biological and gas sensors, and transparent conductive coatings. Despite this promise, researchers could apply graphene more routinely in real-world technologies if they could chemically adjust graphene’s electronic properties. For example, the covalent modification of graphene to create a band gap comparable to silicon (~1 eV) would enable its use in digital electronics, and larger band gaps would provide new opportunities for graphene-based photonics. Towards this end, researchers have focused considerable effort on the chemical functionalization of graphene. Due to its high thermodynamic stability and chemical inertness, new methods and techniques are required to create covalent bonds without promoting undesirable side reactions or irreversible damage to the underlying carbon lattice. In this Account, we review and discuss recent theoretical and experimental work studying covalent modifications to graphene using gas phase atomic radicals. Atomic radicals have sufficient energy to overcome the kinetic and thermodynamic barriers associated with covalent reactions on the basal plane of graphene but lack the energy required to break the C-C sigma bonds that would destroy the carbon lattice. Furthermore, because they are atomic species, radicals substantially reduce the likelihood of unwanted side reactions that confound other covalent chemistries. Overall, these methods based on atomic radicals show promise for the homogeneous functionalization of graphene and the production of new classes of two

Initial evaluation and comparison of plasma damage to atomic layer carbon materials using conventional and low T{sub e} plasma sources

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

Jagtiani, Ashish V.; Miyazoe, Hiroyuki; Chang, Josephine

2016-01-15

The ability to achieve atomic layer precision is the utmost goal in the implementation of atomic layer etch technology. Carbon-based materials such as carbon nanotubes (CNTs) and graphene are single atomic layers of carbon with unique properties and, as such, represent the ultimate candidates to study the ability to process with atomic layer precision and assess impact of plasma damage to atomic layer materials. In this work, the authors use these materials to evaluate the atomic layer processing capabilities of electron beam generated plasmas. First, the authors evaluate damage to semiconducting CNTs when exposed to beam-generated plasmas and compare thesemore » results against the results using typical plasma used in semiconductor processing. The authors find that the beam generated plasma resulted in significantly lower current degradation in comparison to typical plasmas. Next, the authors evaluated the use of electron beam generated plasmas to process graphene-based devices by functionalizing graphene with fluorine, nitrogen, or oxygen to facilitate atomic layer deposition (ALD). The authors found that all adsorbed species resulted in successful ALD with varying impact on the transconductance of the graphene. Furthermore, the authors compare the ability of both beam generated plasma as well as a conventional low ion energy inductively coupled plasma (ICP) to remove silicon nitride (SiN) deposited on top of the graphene films. Our results indicate that, while both systems can remove SiN, an increase in the D/G ratio from 0.08 for unprocessed graphene to 0.22 to 0.26 for the beam generated plasma, while the ICP yielded values from 0.52 to 1.78. Generally, while some plasma-induced damage was seen for both plasma sources, a much wider process window as well as far less damage to CNTs and graphene was observed when using electron beam generated plasmas.« less

The Formation of Formaldehyde on Interstellar Carbonaceous Grain Analogs by O/H Atom Addition

NASA Astrophysics Data System (ADS)

Potapov, Alexey; Jäger, Cornelia; Henning, Thomas; Jonusas, Mindaugas; Krim, Lahouari

2017-09-01

An understanding of possible scenarios for the formation of astrophysically relevant molecules, particularly complex organic molecules, will bring us one step closer to the understanding of our astrochemical heritage. In this context, formaldehyde is an important molecule as a precursor of methanol, which in turn is a starting point for the formation of more complex organic species. In the present experiments, for the first time, following the synthesis of CO, formaldehyde has been produced on the surface of interstellar grain analogs, hydrogenated fullerene-like carbon grains, by O and H atom bombardment. The formation of H2CO is an indication for a possible methanol formation route in such systems.

Embedding Carbon Fibre Structures in Metal Matrixes for Additive Manufacturing

NASA Astrophysics Data System (ADS)

Frostevarg, Jan; Robertson, Stephanie; Benavides, Vicente; Soldatov, Alexander

It is possible to reinforce structures and components using carbon fibres for applications in electronics and medicine, but most commonly used in reinforcing resin fibre composites for personal protection equipment and light weight constructions. Carbon fibres act as stress redistributors while having increased electrical and thermal conductivities. These properties could also be utilized in metal matrixes, if the fibres are properly fused to the metal and the structure remains intact. Another recently developed high potential carbon structure, carbon nanotube- (CNT) yarns, has similar but even greater mechanical properties than common carbon fibres. Via laser cladding, these reinforcing materials could be used in a plethora of applications, either locally (or globally) as surface treatments or as structural reinforcements using multi-layer laser cladding (additive manufacturing). The challenges of embedding carbon fibres or CNT-yarns in a CuAl mixture and SnPb solder wire using lasers are here investigated using high speed imaging and SEM. It is revealed that the carbon fibres have very high buoyancy in the molten metal and quickly degrades when irradiated by the laser. Wetting of the fibres is shown to be improved by a Tungsten coating and embedding of the structures after processing are evaluated using SEM and Raman spectroscopy.

Roles of additives and surface control in slurry atomization

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

Tsai, S.C.

1992-01-01

This project studies the rheology and airblast atomization of micronized coal slurries. Its major objectives are (1) to promote further understanding of the mechanisms and the roles of additives in airblast atomization of coal water slurry (CWS), and (2) to investigate the impacts of coal particle surface properties and interparticle forces on CWS rheology. We have found that the flow behavior index (n) of a suspension (or slurry) is determined by the relative importance of the interparticle van der Waals attraction and the interparticle electrostatic repulsion. The interparticle attraction, measured by the Hamaker constant scaled to the thermal energy atmore » 25[degrees]C (A/kT), causes particle aggregation, which breaks down at high shear rates, and thus leads to slurry pseudoplastic behavior (n< 1). At a constant particle volume fraction and surface charge density (qualitatively measured by the zeta potential in deionized water), n decreases linearly as A/kT increases. The relative viscosity of the pseudoplastic suspension with respect to that of the suspending liquid is found to be independent of particle density and correlate well with the particle Peclet number which equals the particle diffusional relaxation time multiplied by shear rate. Specifically, the relative viscosities of the pseudoplastic glycerol/water coal slurry and the ethylene glycol/glycerol sand slurry, at same volume fractions as well as similar particle size distributions and liquid viscosities, as functions of the particle Peclet number fall along the same line.« less

Effects of Atomic-Scale Structure on the Fracture Properties of Amorphous Carbon - Carbon Nanotube Composites

NASA Technical Reports Server (NTRS)

Jensen, Benjamin D.; Wise, Kristopher E.; Odegard, Gregory M.

2015-01-01

The fracture of carbon materials is a complex process, the understanding of which is critical to the development of next generation high performance materials. While quantum mechanical (QM) calculations are the most accurate way to model fracture, the fracture behavior of many carbon-based composite engineering materials, such as carbon nanotube (CNT) composites, is a multi-scale process that occurs on time and length scales beyond the practical limitations of QM methods. The Reax Force Field (ReaxFF) is capable of predicting mechanical properties involving strong deformation, bond breaking and bond formation in the classical molecular dynamics framework. This has been achieved by adding to the potential energy function a bond-order term that varies continuously with distance. The use of an empirical bond order potential, such as ReaxFF, enables the simulation of failure in molecular systems that are several orders of magnitude larger than would be possible in QM techniques. In this work, the fracture behavior of an amorphous carbon (AC) matrix reinforced with CNTs was modeled using molecular dynamics with the ReaxFF reactive forcefield. Care was taken to select the appropriate simulation parameters, which can be different from those required when using traditional fixed-bond force fields. The effect of CNT arrangement was investigated with three systems: a single-wall nanotube (SWNT) array, a multi-wall nanotube (MWNT) array, and a SWNT bundle system. For each arrangement, covalent bonds are added between the CNTs and AC, with crosslink fractions ranging from 0-25% of the interfacial CNT atoms. The SWNT and MWNT array systems represent ideal cases with evenly spaced CNTs; the SWNT bundle system represents a more realistic case because, in practice, van der Waals interactions lead to the agglomeration of CNTs into bundles. The simulation results will serve as guidance in setting experimental processing conditions to optimize the mechanical properties of CNT

Single-Atom Catalysts of Precious Metals for Electrochemical Reactions.

PubMed

Kim, Jiwhan; Kim, Hee-Eun; Lee, Hyunjoo

2018-01-10

Single-atom catalysts (SACs), in which metal atoms are dispersed on the support without forming nanoparticles, have been used for various heterogeneous reactions and most recently for electrochemical reactions. In this Minireview, recent examples of single-atom electrocatalysts used for the oxygen reduction reaction (ORR), hydrogen oxidation reaction (HOR), hydrogen evolution reaction (HER), formic acid oxidation reaction (FAOR), and methanol oxidation reaction (MOR) are introduced. Many density functional theory (DFT) simulations have predicted that SACs may be effective for CO 2 reduction to methane or methanol production while suppressing H 2 evolution, and those cases are introduced here as well. Single atoms, mainly Pt single atoms, have been deposited on TiN or TiC nanoparticles, defective graphene nanosheets, N-doped covalent triazine frameworks, graphitic carbon nitride, S-doped zeolite-templated carbon, and Sb-doped SnO 2 surfaces. Scanning transmission electron microscopy, extended X-ray absorption fine structure measurement, and in situ infrared spectroscopy have been used to detect the single-atom structure and confirm the absence of nanoparticles. SACs have shown high mass activity, minimizing the use of precious metal, and unique selectivity distinct from nanoparticle catalysts owing to the absence of ensemble sites. Additional features that SACs should possess for effective electrochemical applications were also suggested. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Electrochemical behavior of adrenaline at the carbon atom wire modified electrode

NASA Astrophysics Data System (ADS)

Xue, Kuan-Hong; Liu, Jia-Mei; Wei, Ri-Bing; Chen, Shao-Peng

2006-09-01

Electrochemical behavior of adrenaline at an electrode modified by carbon atom wires (CAWs), a new material, was investigated by cyclic voltammetry combined with UV-vis spectrometry, and forced convection method. As to the electrochemical response of redox of adrenaline/adrenalinequinone couple in 0.50 M H 2SO 4, at a nitric acid treated CAW modified electrode, the anodic and cathodic peak potentials Epa and Epc shifted by 87 mV negatively and 139 mV in the positive direction, respectively, and standard heterogeneous rate constant k0 increased by 16 times compared to the corresponding bare electrode, indicating the extraordinary activity of CAWs in electrocatalysis for the process.

The Formation of Formaldehyde on Interstellar Carbonaceous Grain Analogs by O/H Atom Addition

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

Potapov, Alexey; Jäger, Cornelia; Henning, Thomas

An understanding of possible scenarios for the formation of astrophysically relevant molecules, particularly complex organic molecules, will bring us one step closer to the understanding of our astrochemical heritage. In this context, formaldehyde is an important molecule as a precursor of methanol, which in turn is a starting point for the formation of more complex organic species. In the present experiments, for the first time, following the synthesis of CO, formaldehyde has been produced on the surface of interstellar grain analogs, hydrogenated fullerene-like carbon grains, by O and H atom bombardment. The formation of H{sub 2}CO is an indication formore » a possible methanol formation route in such systems.« less

Rotational Spectrum and Carbon Atom Structure of Dihydroartemisinic Acid

NASA Astrophysics Data System (ADS)

Evangelisti, Luca; Seifert, Nathan A.; Spada, Lorenzo; Pate, Brooks

2016-06-01

Dihydroartemisinic acid (DHAA, C15H24O2, five chiral centers) is a precursor in proposed low-cost synthetic routes to the antimalarial drug artemisinin. In one reaction process being considered in pharmaceutical production, DHAA is formed from an enantiopure sample of artemisinic acid through hydrogenation of the alkene. This reaction needs to properly set the stereochemistry of the asymmetric carbon for the synthesis to produce artemisinin. A recrystallization process can purify the diastereomer mixture of the hydrogenation reaction if the unwanted epimer is produced in less than 10% abundance. There is a need in the process analytical chemistry to rapidly (less than 1 min) measure the diastereomer excess and current solutions, such a HPLC, lack the needed measurement speed. The rotational spectrum of DHAA has been measured at 300:1 signal-to-noise ratio in a chirped-pulsed Fourier transform microwave spectrometer operating from 2-8 GHz using simple heating of the compound. The 13C isotope analysis provides a carbon atom structure that confirms the diastereomer. This structure is in excellent agreement with quantum chemistry calculations at the B2PLYPD3/ 6-311++G** level of theory. The DHAA spectrum is expected to be fully resolved from the unwanted diastereomer raising the potential for fast diastereomer excess measurement by rotational spectroscopy in the pharmaceutical production process.

Density-functional theory study of dimethyl carbonate synthesis by methanol oxidative carbonylation on single-atom Cu1/graphene catalyst

NASA Astrophysics Data System (ADS)

Sun, Wei; Shi, Ruina; Wang, Xuhui; Liu, Shusen; Han, Xiaoxia; Zhao, Chaofan; Li, Zhong; Ren, Jun

2017-12-01

The mechanism for dimethyl carbonate (DMC) synthesis by oxidation carbonylation of methanol on a single-atom Cu1/graphene catalyst was investigated by density-functional theory calculations. Carbon vacancies in graphene can significantly enhance the interaction between Cu atoms and graphene supports, and provide an increased transfer of electrons from Cu atoms to the graphene sheet. Compared with Cu-doped divacancy graphene (Cu/DG), Cu-doped monovacancy graphene (Cu/MG) provides a stronger interaction between adsorbents and the catalyst surface. Among the reaction processes over Cu1/graphene catalysts, CO insertion into methoxide was more favorable than dimethoxide. The rate-limiting step on the Cu/DG surface is the carbomethoxide reaction with methoxide, which is exothermic by 164.6 kJ mol-1 and has an activation barrier of 190.9 kJ mol-1 energy. Compared with that on the Cu crystal surface, Cu4 and Cu3Rh clusters, and the Cu2O(111) surface, the rate-determining step for DMC formation on Cu/MG, which is CO insertion into methoxide, needs to overcome the lowest barrier of 73.5 kJ mol-1 and is exothermic by 44.6 kJ mol-1. Therefore, Cu/MG was beneficial to the formation of DMC as a single-atom catalyst.

Additive-free carbon nanotube dispersions, pastes, gels, and doughs in cresols.

PubMed

Chiou, Kevin; Byun, Segi; Kim, Jaemyung; Huang, Jiaxing

2018-05-29

Cresols are a group of naturally occurring and massively produced methylphenols with broad use in the chemical industry. Here, we report that m -cresol and its liquid mixtures with other isomers are surprisingly good solvents for processing carbon nanotubes. They can disperse carbon nanotubes of various types at unprecedentedly high concentrations of tens of weight percent, without the need for any dispersing agent or additive. Cresols interact with carbon nanotubes by charge transfer through the phenolic hydroxyl proton and can be removed after processing by evaporation or washing, without altering the surface of carbon nanotubes. Cresol solvents render carbon nanotubes polymer-like rheological and viscoelastic properties and processability. As the concentration of nanotubes increases, a continuous transition of four states can be observed, including dilute dispersion, thick paste, free-standing gel, and eventually a kneadable, playdough-like material. As demonstrated with a few proofs of concept, cresols make powders of agglomerated carbon nanotubes immediately usable by a broad array of material-processing techniques to create desirable structures and form factors and make their polymer composites.

Potential energy surfaces for atomic oxygen reactions: Formation of singlet and triplet biradicals as primary reaction products with unsaturated organic molecules

NASA Technical Reports Server (NTRS)

Jaffe, Richard L.

1987-01-01

The experimental study of the interaction of atomic oxygen with organic polymer films under LEO conditions has been hampered by the inability to conduct detailed experiments in situ. As a result, studies of the mechanism of oxygen atom reactions have relied on laboratory O-atom sources that do not fully reproduce the orbital environment. For example, it is well established that only ground electronic state O atoms are present at LEO, yet most ground-based sources are known to produce singlet O atoms and molecules and ions in addition to O(3P). Engineers should not rely on such facilities unless it can be demonstrated either that these different O species are inert or that they react in the same fashion as ground state atoms. Ab initio quantum chemical calculations have been aimed at elucidating the biradical intermediates formed during the electrophilic addition of ground and excited-state O atoms to carbon-carbon double bonds in small olefins and aromatic molecules. These biradicals are critical intermediates in any possible insertion, addition and elimination reaction mechanisms. Through these calculations, we will be able to comment on the relative importance of these pathways for O(3P) and O(1D) reactions. The reactions of O atoms with ethylene and benzene are used to illustrate the important features of the mechanisms of atomic oxygen reaction with unsaturated organic compounds and polymeric materials.

The long-range non-additive three-body dispersion interactions for the rare gases, alkali, and alkaline-earth atoms

NASA Astrophysics Data System (ADS)

Tang, Li-Yan; Yan, Zong-Chao; Shi, Ting-Yun; Babb, James F.; Mitroy, J.

2012-03-01

The long-range non-additive three-body dispersion interaction coefficients Z111, Z112, Z113, and Z122 are computed for many atomic combinations using standard expressions. The atoms considered include hydrogen, the rare gases, the alkali atoms (up to Rb), and the alkaline-earth atoms (up to Sr). The term Z111 arising from three mutual dipole interactions is known as the Axilrod-Teller-Muto coefficient or the DDD (dipole-dipole-dipole) coefficient. Similarly, the terms Z112, Z113, and Z122 arise from the mutual combinations of dipole (1), quadrupole (2), and octupole (3) interactions between atoms and they are sometimes known, respectively, as dipole-dipole-quadrupole, dipole-dipole-octupole, and dipole-quadrupole-quadrupole coefficients. Results for the four Z coefficients are given for the homonuclear trimers, for the trimers involving two like-rare-gas atoms, and for the trimers with all combinations of the H, He, and Li atoms. An exhaustive compilation of all coefficients between all possible atomic combinations is presented as supplementary data.

Large-Area Atomic Oxygen Facility Used to Clean Fire-Damaged Artwork

NASA Technical Reports Server (NTRS)

Rutledge, Sharon K.; Banks, Bruce A.; Steuber, Thomas J.; Sechkar, Edward A.

2000-01-01

In addition to completely destroying artwork, fires in museums and public buildings can soil a displayed artwork with so much accumulated soot that it can no longer be used for study or be enjoyed by the public. In situations where the surface has not undergone extensive charring or melting, restoration can be attempted. However, soot deposits can be very difficult to remove from some types of painted surfaces, particularly when the paint is fragile or flaking or when the top surface of the paint binder has been damaged. Restoration typically involves the use of organic solvents to clean the surface, but these solvents may cause the paint layers to swell or leach out. Also, immersion of the surface or swabbing during solvent cleaning may move or remove pigment through mechanical contact, especially if the fire damage extends into the paint binder. A noncontact technique of removing organic deposits from surfaces was developed out of NASA research on the effects of oxygen atoms on various materials. Atomic oxygen is present in the atmosphere surrounding the Earth at the altitudes where satellites typically orbit. It can react chemically with surface coatings or deposits that contain carbon. In the reaction, the carbon is converted to carbon monoxide and some carbon dioxide. Water vapor is also a byproduct of the reaction if the surface contains carbon-hydrogen bonds. To study this reaction, NASA developed Earth-based facilities to produce atomic oxygen for material exposure and testing. A vacuum facility designed and built by the Electro-Physics Branch of the NASA Glenn Research Center at Lewis Field to provide atomic oxygen over a large area for studying reactions in low Earth orbit has been used to successfully clean several full-size paintings. (This facility can accommodate paintings up to 1.5 by 2.1 m. The atomic oxygen plasma is produced between two large parallel aluminum plates using a radiofrequency power source operating at roughly 400 W. Atomic oxygen is

Microwave absorption properties of carbon nanocoils coated with highly controlled magnetic materials by atomic layer deposition.

PubMed

Wang, Guizhen; Gao, Zhe; Tang, Shiwei; Chen, Chaoqiu; Duan, Feifei; Zhao, Shichao; Lin, Shiwei; Feng, Yuhong; Zhou, Lei; Qin, Yong

2012-12-21

In this work, atomic layer deposition is applied to coat carbon nanocoils with magnetic Fe(3)O(4) or Ni. The coatings have a uniform and highly controlled thickness. The coated nanocoils with coaxial multilayer nanostructures exhibit remarkably improved microwave absorption properties compared to the pristine carbon nanocoils. The enhanced absorption ability arises from the efficient complementarity between complex permittivity and permeability, chiral morphology, and multilayer structure of the products. This method can be extended to exploit other composite materials benefiting from its convenient control of the impedance matching and combination of dielectric-magnetic multiple loss mechanisms for microwave absorption applications.

In silico carbon molecular beam epitaxial growth of graphene on the h-BN substrate: carbon source effect on van der Waals epitaxy

NASA Astrophysics Data System (ADS)

Lee, Jonghoon; Varshney, Vikas; Park, Jeongho; Farmer, Barry L.; Roy, Ajit K.

2016-05-01

during the initial phase of graphene growth simulation using a carbon trimer beam is captured. An initially sp hybridized carbon atom (red colored) becomes sp2 hybridized as a result of additional covalent bonding with the impinging carbon trimer. As the bond angle around the red carbon changes from 180 degree (sp) to 120 degree (sp2), nearby carbon atoms enclose to form a hexagon structure composed of 6 carbon atoms. See DOI: 10.1039/c6nr01396a

High-pressure combustor exhaust emissions with improved air-atomizing and conventional pressure-atomizing fuel nozzles

NASA Technical Reports Server (NTRS)

Ingebo, R. D.; Norgren, C. T.

1973-01-01

A high-pressure combustor segment 0.456 meter (18 in.) long with a maximum cross section of 0.153 by 0.305 meter (6 by 12 in.) was tested with specially designed air-atomizing and conventional pressure-atomizing fuel nozzles at inlet-air temperatures of 340 to 755 k (610 deg to 1360 R), reference velocities of 12.4 to 26.1 meters per second (41 to 86 ft/sec), and fuel-air ratios of 0.008 to 0.020. Increasing inlet-air pressure from 4 to 20 atmospheres generally increased smoke number and nitric oxide, but decreased carbon monoxide and unburned hydrocarbon concentrations with air-atomizing and pressure-atomizing nozzles. Emission indexes for carbon monoxide and unburned hydrocarbons were lower at 4, 10, and 20 atmospheres, and nitric oxide emission indexes were lower at 10 and 20 atmospheres with air-atomizing than with pressure-atomizing nozzles.

Nonlinear tapping dynamics of multi-walled carbon nanotube tipped atomic force microcantilevers

NASA Astrophysics Data System (ADS)

Lee, S. I.; Howell, S. W.; Raman, A.; Reifenberger, R.; Nguyen, C. V.; Meyyappan, M.

2004-05-01

The nonlinear dynamics of an atomic force microcantilever (AFM) with an attached multi-walled carbon nanotube (MWCNT) tip is investigated experimentally and theoretically. We present the experimental nonlinear frequency response of a MWCNT tipped microcantilever in the tapping mode. Several unusual features in the response distinguish it from those traditionally observed for conventional tips. The MWCNT tipped AFM probe is apparently immune to conventional imaging instabilities related to the coexistence of attractive and repulsive tapping regimes. A theoretical interaction model for the system using an Euler elastica MWCNT model is developed and found to predict several unusual features of the measured nonlinear response.

Results of industrial tests of carbonate additive to fuel oil

NASA Astrophysics Data System (ADS)

Zvereva, E. R.; Dmitriev, A. V.; Shageev, M. F.; Akhmetvalieva, G. R.

2017-08-01

Fuel oil plays an important role in the energy balance of our country. The quality of fuel oil significantly affects the conditions of its transport, storage, and combustion; release of contaminants to atmosphere; and the operation of main and auxiliary facilities of HPPs. According to the Energy Strategy of Russia for the Period until 2030, the oil-refining ratio gradually increases; as a result, the fraction of straight-run fuel oil in heavy fuel oils consistently decreases, which leads to the worsening of performance characteristics of fuel oil. Consequently, the problem of the increase in the quality of residual fuel oil is quite topical. In this paper, it is suggested to treat fuel oil by additives during its combustion, which would provide the improvement of ecological and economic indicators of oil-fired HPPs. Advantages of this method include simplicity of implementation, low energy and capital expenses, and the possibility to use production waste as additives. In the paper, the results are presented of industrial tests of the combustion of fuel oil with the additive of dewatered carbonate sludge, which is formed during coagulation and lime treatment of environmental waters on HPPs. The design of a volume delivery device is developed for the steady additive input to the boiler air duct. The values are given for the main parameters of the condition of a TGM-84B boiler plant. The mechanism of action of dewatered carbonate sludge on sulfur oxides, which are formed during fuel oil combustion, is considered. Results of industrial tests indicate the decrease in the mass fraction of discharged sulfur oxides by 36.5%. Evaluation of the prevented damage from sulfur oxide discharged into atmospheric air shows that the combustion of the fuel oil of 100 brand using carbonate sludge as an additive (0.1 wt %) saves nearly 6 million rubles a year during environmental actions at the consumption of fuel oil of 138240 t/year.

Noncontact atomic force microscopy in liquid environment with quartz tuning fork and carbon nanotube probe

NASA Astrophysics Data System (ADS)

Kageshima, Masami; Jensenius, Henriette; Dienwiebel, Martin; Nakayama, Yoshikazu; Tokumoto, Hiroshi; Jarvis, Suzanne P.; Oosterkamp, Tjerk H.

2002-03-01

A force sensor for noncontact atomic force microscopy in liquid environment was developed by combining a multiwalled carbon nanotube (MWNT) probe with a quartz tuning fork. Solvation shells of octamethylcyclotetrasiloxane on a graphite surface were detected both in the frequency shift and dissipation. Due to the high aspect ratio of the CNT probe, the long-range background force was barely detectable in the solvation region.

A square-wave wavelength modulation system for automatic background correction in carbon furnace atomic emission spectrometry

NASA Astrophysics Data System (ADS)

Bezur, L.; Marshall, J.; Ottaway, J. M.

A square-wave wavelength modulation system, based on a rotating quartz chopper with four quadrants of different thicknesses, has been developed and evaluated as a method for automatic background correction in carbon furnace atomic emission spectrometry. Accurate background correction is achieved for the residual black body radiation (Rayleigh scatter) from the tube wall and Mie scatter from particles generated by a sample matrix and formed by condensation of atoms in the optical path. Intensity modulation caused by overlap at the edges of the quartz plates and by the divergence of the optical beam at the position of the modulation chopper has been investigated and is likely to be small.

Molecular Modeling of an Electrophilic Addition Reaction with "Unexpected" Regiochemistry

ERIC Educational Resources Information Center

Best, Katherine T.; Li, Diana; Helms, Eric D.

2017-01-01

The electrophilic addition of a hydrohalic acid (HX) to an alkene is often one of the first reactions learned in second-year undergraduate organic chemistry classes. During the ensuing discussion of the mechanism, it is shown that this reaction follows Markovnikov's rule, which states that the hydrogen atom will attach to the carbon with fewer…

Tribological properties of graphene oxide and carbon spheres as lubricating additives

NASA Astrophysics Data System (ADS)

Song, Haojie; Wang, Zhiqiang; Yang, Jin

2016-10-01

The purpose of this paper was to investigate the tribological properties of carbon materials with various morphologies [i.e., graphene oxide (GO) and carbon spheres (CSs)] utilized as lubricating additives on a ball-plate tribotester. The morphology and spectroscopy characterization of GO and CSs were investigated by scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectrometry, and thermogravimetric analysis. Friction and wear properties of the sunflower seed oil filled with GO and CSs were investigated by using a MS-T3000 ball-on-disk apparatus. Results show that the sunflower seed oil containing 0.3 wt% GO nanosheets exhibited a substantial diminution in friction and wear compared with the 3.0 wt% CSs as sunflower seed oil additives. Formation of low-shear strength tribofilms containing GO and its self-lubricating behavior was the key factor in reduction of the friction and prevention from wear and deformation. In addition, friction mechanism of CSs was also discussed.

Additives to reduce susceptibility of thermosets and thermoplastics to erosion from atomic oxygen

NASA Technical Reports Server (NTRS)

Orwoll, Robert A.

1990-01-01

Polymeric materials have many attractive features such as light weight, high strength, and broad applicability in the form of films, fibers, and molded objects. In low earth orbit (LEO), these materials, when exposed on the exterior of the spacecraft, have the serious disadvantage of being susceptible to erosion by atomic oxygen (AO). AO is the most common chemical species at LEO altitudes. AO can be an extremely efficient oxidizing agent as was apparent from the extensive erosion of organic films exposed in STS missions. The mechanism for erosion involves the reaction of oxygen atoms at the surface of the substrate to form small molecular species. The susceptibility of polymeric materials varies with their chemical composition. Films with silicon atoms incorporated in the molecular structures have large coefficients of thermal expansion. This limits their utility. In an alternative approach additives were sought that mix physically and form a protective oxide layer when the film is exposed to AO. A large number of organic compounds containing silicon, germanium, or tin atoms were screened. Most were found to have very limited solubility in the polyetherimide (Ultem) films that were being protected from AO. However, one, bis(triphenyl tin) oxide, (BTO), is miscible in Ultem up to about 25 percent. Films of Ultem polyimide containing up to 25 wt percent BTO were prepared by evaporation of solvent from a solution of Ultem and BTO. The effects of AO on these films were simulated in the oxygen atmosphere of a radio frequency glow-discharge chamber. In the second part of this study, atoms were incorporated in epoxy resins. Experiments are in progress to measure the resistance of films of the cured epoxy to AO in the discharge chamber.

Cyanide Ligand Assembly by Carbon Atom Transfer to an Iron Nitride

DOE PAGES

Martinez, Jorge L.; Lin, Hsiu-Jung; Lee, Wei-Tsung; ...

2017-09-21

The new iron(IV) nitride complex PhB( iPr 2Im) 3Fe≡N reacts with two equivalents of bis(diisopropylamino)cyclopropenylidene (BAC) to provide PhB( iPr 2Im) 3Fe(CN)(N 2)(BAC). This unusual example of a four-electron reaction involves carbon atom transfer from BAC to create a cyanide ligand along with the alkyne iPr 2N-C≡C-N iPr 2. The iron complex is in equilibrium with an N 2- free species. Further reaction with CO leads to formation of a CO analogue, which can be independently prepared using NaCN as the cyanide source, while reaction with B(C 6F 5) 3 provides the cyanoborane derivative.

Merging allylic carbon-hydrogen and selective carbon-carbon bond activation.

PubMed

Masarwa, Ahmad; Didier, Dorian; Zabrodski, Tamar; Schinkel, Marvin; Ackermann, Lutz; Marek, Ilan

2014-01-09

Since the nineteenth century, many synthetic organic chemists have focused on developing new strategies to regio-, diastereo- and enantioselectively build carbon-carbon and carbon-heteroatom bonds in a predictable and efficient manner. Ideal syntheses should use the least number of synthetic steps, with few or no functional group transformations and by-products, and maximum atom efficiency. One potentially attractive method for the synthesis of molecular skeletons that are difficult to prepare would be through the selective activation of C-H and C-C bonds, instead of the conventional construction of new C-C bonds. Here we present an approach that exploits the multifold reactivity of easily accessible substrates with a single organometallic species to furnish complex molecular scaffolds through the merging of otherwise difficult transformations: allylic C-H and selective C-C bond activations. The resulting bifunctional nucleophilic species, all of which have an all-carbon quaternary stereogenic centre, can then be selectively derivatized by the addition of two different electrophiles to obtain more complex molecular architecture from these easily available starting materials.

Merging allylic carbon-hydrogen and selective carbon-carbon bond activation

NASA Astrophysics Data System (ADS)

Masarwa, Ahmad; Didier, Dorian; Zabrodski, Tamar; Schinkel, Marvin; Ackermann, Lutz; Marek, Ilan

2014-01-01

Since the nineteenth century, many synthetic organic chemists have focused on developing new strategies to regio-, diastereo- and enantioselectively build carbon-carbon and carbon-heteroatom bonds in a predictable and efficient manner. Ideal syntheses should use the least number of synthetic steps, with few or no functional group transformations and by-products, and maximum atom efficiency. One potentially attractive method for the synthesis of molecular skeletons that are difficult to prepare would be through the selective activation of C-H and C-C bonds, instead of the conventional construction of new C-C bonds. Here we present an approach that exploits the multifold reactivity of easily accessible substrates with a single organometallic species to furnish complex molecular scaffolds through the merging of otherwise difficult transformations: allylic C-H and selective C-C bond activations. The resulting bifunctional nucleophilic species, all of which have an all-carbon quaternary stereogenic centre, can then be selectively derivatized by the addition of two different electrophiles to obtain more complex molecular architecture from these easily available starting materials.

THE DYNAMICS OF HYDROGEN ATOM ABSTRACTION FROM POLYATOMIC MOLECULES.

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

LIU,X.; SUITS,A.G.

2002-11-21

The hydrogen atom abstraction reaction is an important fundamental process that is extensively involved in atmospheric and combustion chemistry. The practical significance of this type of reaction with polyatomic hydrocarbons is manifest, which has led to many kinetics studies. The detailed understanding of these reactions requires corresponding dynamics studies. However, in comparison to the A + HX {radical} AH + X reactions, the study of the dynamics of A + HR {yields} AH + R reactions is much more difficult, both experimentally and theoretically (here and in the following, A stands for an atom, X stands for a halogen atom,more » and R stands for a polyatomic hydrocarbon radical). The complication stems from the structured R, in contrast to the structureless X. First of all, there are many internal degrees of freedom in R that can participate in the reaction. In addition, there are different carbon sites from which an H atom can be abstracted, and the dynamics are correspondingly different; there are also multiple identical carbon sites in HR and in the picture of a local reaction, there exist competitions between neighboring H atoms, and so on. Despite this complexity, there have been continuing efforts to obtain insight into the dynamics of these reactions. In this chapter, some examples are presented, including the reactions of ground state H, Cl, and O atoms, with particular focus on our recent work using imaging to obtain the differential cross sections for these reactions.« less

Addition of Carbon to the Culture Medium Improves the Detection Efficiency of Aflatoxin Synthetic Fungi

PubMed Central

Suzuki, Tadahiro; Iwahashi, Yumiko

2016-01-01

Aflatoxin (AF) is a harmful secondary metabolite that is synthesized by the Aspergillus species. Although AF detection techniques have been developed, techniques for detection of AF synthetic fungi are still required. Techniques such as plate culture methods are continually being modified for this purpose. However, plate culture methods require refinement because they suffer from several issues. In this study, activated charcoal powder (carbon) was added to a culture medium containing cyclodextrin (CD) to enhance the contrast of fluorescence and improve the detection efficiency for AF synthetic fungi. Two culture media, potato dextrose agar and yeast extract sucrose agar, were investigated using both plate and liquid cultures. The final concentrations of CD and carbon in the media were 3 mg/mL and 0.3 mg/mL, respectively. Addition of carbon improved the visibility of fluorescence by attenuating approximately 30% of light scattering. Several fungi that could not be detected with only CD in the medium were detected with carbon addition. The carbon also facilitated fungal growth in the potato dextrose liquid medium. The results suggest that addition of carbon to media can enhance the observation of AF-derived fluorescence. PMID:27854283

Additive Mixing and Conformal Coating of Noniridescent Structural Colors with Robust Mechanical Properties Fabricated by Atomization Deposition.

PubMed

Li, Qingsong; Zhang, Yafeng; Shi, Lei; Qiu, Huihui; Zhang, Suming; Qi, Ning; Hu, Jianchen; Yuan, Wei; Zhang, Xiaohua; Zhang, Ke-Qin

2018-04-24

Artificial structural colors based on short-range-ordered amorphous photonic structures (APSs) have attracted great scientific and industrial interest in recent years. However, the previously reported methods of self-assembling colloidal nanoparticles lack fine control of the APS coating and fixation on substrates and poorly realize three-dimensional (3D) conformal coatings for objects with irregular or highly curved surfaces. In this paper, atomization deposition of silica colloidal nanoparticles with poly(vinyl alcohol) as the additive is proposed to solve the above problems. By finely controlling the thicknesses of APS coatings, additive mixing of noniridescent structural colors is easily realized. Based on the intrinsic omnidirectional feature of atomization, a one-step 3D homogeneous conformal coating is also readily realized on various irregular or highly curved surfaces, including papers, resins, metal plates, ceramics, and flexible silk fabrics. The vivid coatings on silk fabrics by atomization deposition possess robust mechanical properties, which are confirmed by rubbing and laundering tests, showing great potential in developing an environmentally friendly coloring technique in the textile industry.

Carbon Materials Research

DTIC Science & Technology

2006-08-01

carbon would be highly oriented pyrolytic graphite ( HOPG ), which is formed by depositing one atom at a time on a surface utilizing the pyrolysis of a... of the crystallites, and baking to 2800 K produces a polycrystalline graphite part that has high strength and conductivity. To make isotropic...pitch fibers) or flexible (Graphoil®), as well as anisotropic ( HOPG ) or isotropic ( polycrystalline graphite ). In addition, porosity, lubricity

Simple-Cubic Carbon Frameworks with Atomically Dispersed Iron Dopants toward High-Efficiency Oxygen Reduction.

PubMed

Wang, Biwei; Wang, Xinxia; Zou, Jinxiang; Yan, Yancui; Xie, Songhai; Hu, Guangzhi; Li, Yanguang; Dong, Angang

2017-03-08

Iron and nitrogen codoped carbons (Fe-N-C) have attracted increasingly greater attention as electrocatalysts for oxygen reduction reaction (ORR). Although challenging, the synthesis of Fe-N-C catalysts with highly dispersed and fully exposed active sites is of critical importance for improving the ORR activity. Here, we report a new type of graphitic Fe-N-C catalysts featuring numerous Fe single atoms anchored on a three-dimensional simple-cubic carbon framework. The Fe-N-C catalyst, derived from self-assembled Fe 3 O 4 nanocube superlattices, was prepared by in situ ligand carbonization followed by acid etching and ammonia activation. Benefiting from its homogeneously dispersed and fully accessible active sites, highly graphitic nature, and enhanced mass transport, our Fe-N-C catalyst outperformed Pt/C and many previously reported Fe-N-C catalysts for ORR. Furthermore, when used for constructing the cathode for zinc-air batteries, our Fe-N-C catalyst exhibited current and power densities comparable to those of the state-of-the-art Pt/C catalyst.

Strengthened PAN-based carbon fibers obtained by slow heating rate carbonization

PubMed Central

Kim, Min-A; Jang, Dawon; Tejima, Syogo; Cruz-Silva, Rodolfo; Joh, Han-Ik; Kim, Hwan Chul; Lee, Sungho; Endo, Morinobu

2016-01-01

Large efforts have been made over the last 40 years to increase the mechanical strength of polyacrylonitrile (PAN)-based carbon fibers (CFs) using a variety of chemical or physical protocols. In this paper, we report a new method to increase CFs mechanical strength using a slow heating rate during the carbonization process. This new approach increases both the carbon sp3 bonding and the number of nitrogen atoms with quaternary bonding in the hexagonal carbon network. Theoretical calculations support a crosslinking model promoted by the interstitial carbon atoms located in the graphitic interlayer spaces. The improvement in mechanical performance by a controlled crosslinking between the carbon hexagonal layers of the PAN based CFs is a new concept that can contribute further in the tailoring of CFs performance based on the understanding of their microstructure down to the atomic scale. PMID:27004752

Strengthened PAN-based carbon fibers obtained by slow heating rate carbonization.

PubMed

Kim, Min-A; Jang, Dawon; Tejima, Syogo; Cruz-Silva, Rodolfo; Joh, Han-Ik; Kim, Hwan Chul; Lee, Sungho; Endo, Morinobu

2016-03-23

Large efforts have been made over the last 40 years to increase the mechanical strength of polyacrylonitrile (PAN)-based carbon fibers (CFs) using a variety of chemical or physical protocols. In this paper, we report a new method to increase CFs mechanical strength using a slow heating rate during the carbonization process. This new approach increases both the carbon sp(3) bonding and the number of nitrogen atoms with quaternary bonding in the hexagonal carbon network. Theoretical calculations support a crosslinking model promoted by the interstitial carbon atoms located in the graphitic interlayer spaces. The improvement in mechanical performance by a controlled crosslinking between the carbon hexagonal layers of the PAN based CFs is a new concept that can contribute further in the tailoring of CFs performance based on the understanding of their microstructure down to the atomic scale.

Clarifying atomic weights: A 2016 four-figure table of standard and conventional atomic weights

USGS Publications Warehouse

Coplen, Tyler B.; Meyers, Fabienne; Holden, Norman E.

2017-01-01

To indicate that atomic weights of many elements are not constants of nature, in 2009 and 2011 the Commission on Isotopic Abundances and Atomic Weights (CIAAW) of the International Union of Pure and Applied Chemistry (IUPAC) replaced single-value standard atomic weight values with atomic weight intervals for 12 elements (hydrogen, lithium, boron, carbon, nitrogen, oxygen, magnesium, silicon, sulfur, chlorine, bromine, and thallium); for example, the standard atomic weight of nitrogen became the interval [14.00643, 14.00728]. CIAAW recognized that some users of atomic weight data only need representative values for these 12 elements, such as for trade and commerce. For this purpose, CIAAW provided conventional atomic weight values, such as 14.007 for nitrogen, and these values can serve in education when a single representative value is needed, such as for molecular weight calculations. Because atomic weight values abridged to four figures are preferred by many educational users and are no longer provided by CIAAW as of 2015, we provide a table containing both standard atomic weight values and conventional atomic weight values abridged to four figures for the chemical elements. A retrospective review of changes in four-digit atomic weights since 1961 indicates that changes in these values are due to more accurate measurements over time or to the recognition of the impact of natural isotopic fractionation in normal terrestrial materials upon atomic weight values of many elements. Use of the unit “u” (unified atomic mass unit on the carbon mass scale) with atomic weight is incorrect because the quantity atomic weight is dimensionless, and the unit “amu” (atomic mass unit on the oxygen scale) is an obsolete term: Both should be avoided.

Investigation of lithium ion battery electrolytes containing flame retardants in combination with the film forming electrolyte additives vinylene carbonate, vinyl ethylene carbonate and fluoroethylene carbonate

NASA Astrophysics Data System (ADS)

Dagger, Tim; Grützke, Martin; Reichert, Matthias; Haetge, Jan; Nowak, Sascha; Winter, Martin; Schappacher, Falko M.

2017-12-01

In order to address the trade-off between the safety lithium ion battery (LIB) electrolytes and their electrochemical performance, synergetic effects of flame retardant additives (FRs) in combination with film forming additives (FFAs) are investigated. Triphenyl phosphate (TPP) and a silicon-containing additive (WA) are applied as FRs to improve the onset temperature of the thermal runaway of a LIB standard electrolyte (LP57: 1 M LiPF6 in EC:EMC 3:7) about 15 K and 28 K, respectively. The application of the FRs in MCMB graphite/lithium metal and NMC111/lithium metal three-electrode cells induces insufficiencies in terms of charge/discharge cycling stability and rate capability. It is investigated if the addition of FFAs can degrade the insufficiencies that are induced by the FRs. Vinylene carbonate, vinyl ethylene carbonate and fluoroethylene carbonate are added to a mixture of LP57 with 10% FR to enhance the cycling performance via improved interphase formation. Results reveal, that the rate capability of cells containing TPP or WA is especially improved by addition of 2% or 5% FEC, respectively. Postmortem analyses of the electrodes by SEM and of the electrolyte by GC-MS are performed. Direct correlations between the cycling behavior during the C-rate study and the electrolyte decomposition products are drawn.

Investigation of diamond-like carbon samples as a charge state conversion surface for neutral atom imaging detectors in space applications

NASA Astrophysics Data System (ADS)

Brigitte Neuland, Maike; Riedo, Andreas; Scheer, Jürgen; Wurz, Peter

2014-05-01

The detection of energetic neutral atoms is a substantial requirement on every space mission mapping particle populations of a planetary magnetosphere or plasma of the interstellar medium. For imaging neutrals, these first have to be ionized. Regarding the constraints of weight, volume and power consumption, the technique of surface ionization complies with all specifications of a space mission. Particularly low energy neutral atoms, which cannot be ionized by passing through a foil, are ionized by scattering on a charge state conversion surface. Since more than 30 years intense research work is done to find suitable materials for use as charge state conversion surfaces. Crucial parameters are the ionisation efficiency of the surface material and the scattering properties. Against all expectations, insulators showed very promising characteristics for serving as conversion surfaces. Particularly diamond-like carbon was proven advantageously: While efficiently ionising incoming neutral atoms, diamond stands out by its durability and chemical inertness. In the IBEX-Lo sensor, a diamond-like carbon surface is used for ionisation of neutral atoms. Energy resolved maps of neutral atoms from the IBEX mission revealed phenomena of the interaction between heliosphere and local interstellar medium (LISM) that demand for new theory and explanations [McComas et al., 2011]. Building on the successes of the IBEX mission, a follow up mission concept to further explore the boundaries of the heliosphere already exists. The Interstellar MApping Probe (IMAP) is planned to map neutral atoms in a larger energy range and with a distinct better angular resolution and sensitivity than IBEX [McComas et al.]. The aspired performance of the IMAP sensors implies also for charge state conversion surfaces with improved characteristics. We investigated samples of diamond-like carbon, manufactured by the chemical vapour and pulsed laser deposition method, regarding their ionisation efficiency

Reactive pathways of hydrogen and carbon removal from organosilicate glass low- κ films by F atoms

NASA Astrophysics Data System (ADS)

Voronina, Ekaterina N.; Mankelevich, Yuri A.; Rakhimova, Tatyana V.

2017-07-01

Direct molecular dynamic simulation on the base of the density functional theory (DFT) method is used to study some critical reactions of F atoms with organosilicate glass (OSG) low-κ films. Here static and dynamic DFT-based approaches are applied for a variety of reactive pathways of hydrogen and carbon removal in the form of volatile products (HF, CF2 and CF3 molecules) from initial SiCH3 surface groups. These reactions constitute an important part of the proposed multi-step mechanism of OSG films damage and etching by thermal F atoms. Two models (POSS and TMCTS macromolecules and their modifications) are used to illustrate the peculiarities and dynamics of the successive reactions of F atoms with the initial SiCH3 and appeared SiCHxFy (x + y ≤ 3) surface groups. Contribution to the Topical Issue "Dynamics of Molecular Systems (MOLEC 2016)", edited by Alberto Garcia-Vela, Luis Banares and Maria Luisa Senent.

Eutectic Formation During Solidification of Ni-Based Single-Crystal Superalloys with Additional Carbon

NASA Astrophysics Data System (ADS)

Wang, Fu; Ma, Dexin; Bührig-Polaczek, Andreas

2017-11-01

γ/ γ' eutectics' nucleation behavior during the solidification of a single-crystal superalloy with additional carbon was investigated by using directional solidification quenching method. The results show that the nucleation of the γ/ γ' eutectics can directly occur on the existing γ dendrites, directly in the remaining liquid, or on the primary MC-type carbides. The γ/γ' eutectics formed through the latter two mechanisms have different crystal orientations than that of the γ matrix. This suggests that the conventional Ni-based single-crystal superalloy castings with additional carbon only guarantee the monocrystallinity of the γ matrix and some γ/ γ' eutectics and, in addition to the carbides, there are other misoriented polycrystalline microstructures existing in macroscopically considered "single-crystal" superalloy castings.

SEPARATION OF PLUTONIUM FROM ELEMENTS HAVING AN ATOMIC NUMBER NOT LESS THAN 92

DOEpatents

Fitch, F.T.; Russell, D.S.

1958-09-16

other elements having atomic numbers nnt less than 92, It has been proposed in the past to so separate plutonium by solvent extraction iato an organic solvent using triglycoldichlcride as the organic solvent. The improvement lies in the discovery that triglycoldichloride performs far more efflciently as an extractant, wher certain second organie compounds are added to it. Mentioned as satisfactory additive compounds are benzaldehyde, saturated aliphatic aldehydes containtng at least twc carbon atoms, and certain polyhydric phenols.

Toward the Atomic-Level Mass Analysis of Biomolecules by the Scanning Atom Probe.

PubMed

Nishikawa, Osamu; Taniguchi, Masahiro

2017-04-01

In 1994, a new type of atom probe instrument, named the scanning atom probe (SAP), was proposed. The unique feature of the SAP is the introduction of a small extraction electrode, which scans over a specimen surface and confines the high field, required for field evaporation of surface atoms in a small space, between the specimen and the electrode. Thus, the SAP does not require a sharp specimen tip. This indicates that the SAP can mass analyze the specimens which are difficult to form in a sharp tip, such as organic materials and biomolecules. Clean single wall carbon nanotubes (CNT), made by high-pressure carbon monoxide process are found to be the best substrates for biomolecules. Various amino acids and dipeptide biomolecules were successfully mass analyzed, revealing characteristic clusters formed by strongly bound atoms in the specimens. The mass analysis indicates that SAP analysis of biomolecules is not only qualitative, but also quantitative.

ALMA observations of atomic carbon in z ˜ 4 dusty star-forming galaxies

NASA Astrophysics Data System (ADS)

Bothwell, M. S.; Aguirre, J. E.; Aravena, M.; Bethermin, M.; Bisbas, T. G.; Chapman, S. C.; De Breuck, C.; Gonzalez, A. H.; Greve, T. R.; Hezaveh, Y.; Ma, J.; Malkan, M.; Marrone, D. P.; Murphy, E. J.; Spilker, J. S.; Strandet, M.; Vieira, J. D.; Weiß, A.

2017-04-01

We present Atacama Large Millimeter Array [C I](1 - 0) (rest frequency 492 GHz) observations for a sample of 13 strongly lensed dusty star-forming galaxies (DSFGs) originally discovered at 1.4 mm in a blank-field survey by the South Pole Telescope (SPT). We compare these new data with available [C I] observations from the literature, allowing a study of the interstellar medium (ISM) properties of ˜30 extreme DSFGs spanning a redshift range 2 < z < 5. Using the [C I] line as a tracer of the molecular ISM, we find a mean molecular gas mass for SPT-DSFGs of 6.6 × 1010 M⊙. This is in tension with gas masses derived via low-J 12CO and dust masses; bringing the estimates into accordance requires either (a) an elevated CO-to-H2 conversion factor for our sample of αCO ˜ 2.5 and a gas-to-dust ratio ˜200, or (b) an high carbon abundance X_{C I} ˜ 7× 10^{-5}. Using observations of a range of additional atomic and molecular lines (including [C I], [C II]and multiple transitions of CO), we use a modern photodissociation region code (3D-PDR) to assess the physical conditions (including the density, UV radiation field strength and gas temperature) within the ISM of the DSFGs in our sample. We find that the ISM within our DSFGs is characterized by dense gas permeated by strong UV fields. We note that previous efforts to characterize photodissociation region regions in DSFGs may have significantly under-estimated the density of the ISM. Combined, our analysis suggests that the ISM of extreme dusty starbursts at high redshift consists of dense, carbon-rich gas not directly comparable to the ISM of starbursts in the local Universe.

Experimental nutrient additions accelerate terrestrial carbon loss from stream ecosystems

Treesearch

Amy D. Rosemond; Jonathan P. Benstead; Phillip M. Bumpers; Vladislav Gulis; John S. Kominoski; David W.P. Manning; Keller Suberkropp; J. Bruce Wallace

2015-01-01

Nutrient pollution of freshwater ecosystems results in predictable increases in carbon (C) sequestration by algae. Tests of nutrient enrichment on the fates of terrestrial organic C, which supports riverine food webs and is a source of CO2, are lacking. Using whole-stream nitrogen (N) and phosphorus (P) additions spanning the equivalent of 27 years, we found that...

Simple and efficient LCAO basis sets for the diffuse states in carbon nanostructures.

PubMed

Papior, Nick R; Calogero, Gaetano; Brandbyge, Mads

2018-06-27

We present a simple way to describe the lowest unoccupied diffuse states in carbon nanostructures in density functional theory calculations using a minimal LCAO (linear combination of atomic orbitals) basis set. By comparing plane wave basis calculations, we show how these states can be captured by adding long-range orbitals to the standard LCAO basis sets for the extreme cases of planar sp 2 (graphene) and curved carbon (C 60 ). In particular, using Bessel functions with a long range as additional basis functions retain a minimal basis size. This provides a smaller and simpler atom-centered basis set compared to the standard pseudo-atomic orbitals (PAOs) with multiple polarization orbitals or by adding non-atom-centered states to the basis.

Simple and efficient LCAO basis sets for the diffuse states in carbon nanostructures

NASA Astrophysics Data System (ADS)

Papior, Nick R.; Calogero, Gaetano; Brandbyge, Mads

2018-06-01

We present a simple way to describe the lowest unoccupied diffuse states in carbon nanostructures in density functional theory calculations using a minimal LCAO (linear combination of atomic orbitals) basis set. By comparing plane wave basis calculations, we show how these states can be captured by adding long-range orbitals to the standard LCAO basis sets for the extreme cases of planar sp 2 (graphene) and curved carbon (C60). In particular, using Bessel functions with a long range as additional basis functions retain a minimal basis size. This provides a smaller and simpler atom-centered basis set compared to the standard pseudo-atomic orbitals (PAOs) with multiple polarization orbitals or by adding non-atom-centered states to the basis.

Launch Vehicle Performance for Bipropellant Propulsion Using Atomic Propellants With Oxygen

NASA Technical Reports Server (NTRS)

Palaszewski, Bryan

2000-01-01

Atomic propellants for bipropellant launch vehicles using atomic boron, carbon, and hydrogen were analyzed. The gross liftoff weights (GLOW) and dry masses of the vehicles were estimated, and the 'best' design points for atomic propellants were identified. Engine performance was estimated for a wide range of oxidizer to fuel (O/F) ratios, atom loadings in the solid hydrogen particles, and amounts of helium carrier fluid. Rocket vehicle GLOW was minimized by operating at an O/F ratio of 1.0 to 3.0 for the atomic boron and carbon cases. For the atomic hydrogen cases, a minimum GLOW occurred when using the fuel as a monopropellant (O/F = 0.0). The atomic vehicle dry masses are also presented, and these data exhibit minimum values at the same or similar O/F ratios as those for the vehicle GLOW. A technology assessment of atomic propellants has shown that atomic boron and carbon rocket analyses are considered to be much more near term options than the atomic hydrogen rockets. The technology for storing atomic boron and carbon has shown significant progress, while atomic hydrogen is not able to be stored at the high densities needed for effective propulsion. The GLOW and dry mass data can be used to estimate the cost of future vehicles and their atomic propellant production facilities. The lower the propellant's mass, the lower the overall investment for the specially manufactured atomic propellants.

Effects of irrigation and addition of nitrogen fertiliser on net ecosystem carbon balance for a grassland.

PubMed

Moinet, Gabriel Y K; Cieraad, Ellen; Turnbull, Matthew H; Whitehead, David

2017-02-01

The ability to quantify the impacts of changing management practices on the components of net ecosystem carbon balance (N B ) is required to forecast future changes in soil carbon stocks and potential feedbacks on atmospheric CO 2 concentrations. In this study we investigated seasonal changes on the components of net ecosystem carbon balance resulting from the application of irrigation and nitrogen fertiliser to a temperate grassland in New Zealand where we simulated grazing events. We made seasonal measurements of the components of N B using chamber measurements in field plots with and without irrigation and addition of nitrogen fertiliser. We developed models to determine the physiological responses of gross canopy photosynthesis (A), leaf respiration (R L ) and soil respiration (R S ) to soil and air temperature, soil water content and irradiance and we estimated annual N B for the first year after treatments were applied. Overall, irrigation and nitrogen addition had a synergistic effect to increase annual estimates of above-ground components of carbon balance (A, R L and carbon exported through simulated grazing, F export ), but there was no effect from adding nitrogen alone. Annual R S remained unchanged between treatments. The treatments resulted in increases in above-ground biomass production, but, with the high intensity of simulated grazing, these were not sufficient to offset ecosystem carbon losses, so all treatments remained a net source of carbon. There were no significant differences between treatments and annual N B ranged from -540gCm -2 y -1 for the treatment with no irrigation and no nitrogen addition and -284gCm -2 y -1 for the treatment with irrigation and nitrogen addition. Our findings from the first year of the treatments quantify the net benefits of addition of irrigation and nitrogen on increasing above-ground production for animal feed but show that this did not lead to a net increase carbon input to the soil. Copyright © 2016 Elsevier B

Ethers as Oxygen Donor and Carbon Source in Non-hydrolytic Sol-Gel: One-Pot, Atom-Economic Synthesis of Mesoporous TiO2 -Carbon Nanocomposites.

PubMed

Escamilla-Pérez, Angel Manuel; Louvain, Nicolas; Boury, Bruno; Brun, Nicolas; Mutin, P Hubert

2018-04-03

Mesoporous TiO 2 -carbon nanocomposites were synthesized using an original non-hydrolytic sol-gel (NHSG) route, based on the reaction of simple ethers (diisopropyl ether or tetrahydrofuran) with titanium tetrachloride. In this atom-economic, solvent-free process, the ether acts not only as an oxygen donor but also as the sole carbon source. Increasing the reaction temperature to 180 °C leads to the decomposition of the alkyl chloride by-product and to the formation of hydrocarbon polymers, which are converted to carbon by pyrolysis under argon. The carbon-TiO 2 nanocomposites and their TiO 2 counterparts (obtained by calcination) were characterized by nitrogen physisorption, XRD, solid state 13 C NMR and Raman spectroscopies, SEM, and TEM. The nanocomposites are mesoporous with surface areas of up to 75 m 2  g -1 and pore sizes around 10 nm. They are composed of aggregated anatase nanocrystals coated by an amorphous carbon film. Playing on the nature of the ether and on the reaction temperature allows control over the carbon content in the nanocomposites. The nature of the ether also influences the size of the TiO 2 crystallites and the morphology of the nanocomposite. To further characterize the carbon coating, the behavior of the carbon-TiO 2 nanocomposites and bare TiO 2 samples toward lithium insertion-deinsertion was investigated in half-cells. This simple NHSG approach should provide a general method for the synthesis of a wide range of carbon-metal oxide nanocomposites. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

The atomic arrangement of iimoriite-(Y), Y2(SiO4)(CO3)

USGS Publications Warehouse

Hughes, J.M.; Foord, E.E.; Jai-Nhuknan, J.; Bell, J.M.

1996-01-01

Iimoriite-(Y) from Bokan Mountain, Prince of Wales Island, Alaska has been studied using single-crystal X-ray-diffraction techniques. The mineral, ideally Y2(SiO4)(CO3), crystallizes in space group P1, with a 6.5495(13), b 6.6291(14), c 6.4395(11)A??, ?? 116.364(15), ?? 92.556(15) and ?? 95.506(17)??. The atomic arrangement has been solved and refined to an R value of 0.019. The arrangement of atoms consists of alternating (011) slabs of orthosilicate groups and carbonate groups, with no sharing of oxygen atoms between anionic complexes in adjacent slabs. Y1 atoms separate adjacent tetrahedra along [100] within the orthosilicate slab, and Y2 atoms separate adjacent carbonate groups along [100] within the carbonate slab. Adjacent orthosilicate and carbonate slabs are linked in (100) by bonding Y atoms from each slab to oxygen atoms of adjacent slabs, in the form of YO8 polyhedra. The Y1 atoms exist in Y12O14 dimers in the orthosilicate slab, and the Y2 atoms exist in continuous [011] ribbons of edge-sharing Y2O8 polyhedra in the carbonate slab.

Tunneling in hydrogen and deuterium atom addition to CO at low temperatures

NASA Astrophysics Data System (ADS)

Andersson, Stefan; Goumans, T. P. M.; Arnaldsson, Andri

2011-09-01

The hydrogen and deuterium atom addition reactions of CO to form HCO and DCO are addressed by Harmonic Quantum Transition State Theory calculations. Special attention is paid to the reactions at very low temperatures (5-20 K) where it is found that quantum tunneling leads to substantial rates of reaction. This supports experiments in the solid phase, which conclude that these reactions are driven by tunneling at low temperatures. The calculated kinetic isotope effect of kD/ kH = 1/250 is found to be lower than the experimentally deduced value of 0.08 for the surface reaction. Possible reasons for this discrepancy are discussed.

Study of additive manufactured microwave cavities for pulsed optically pumped atomic clock applications

NASA Astrophysics Data System (ADS)

Affolderbach, C.; Moreno, W.; Ivanov, A. E.; Debogovic, T.; Pellaton, M.; Skrivervik, A. K.; de Rijk, E.; Mileti, G.

2018-03-01

Additive manufacturing (AM) of passive microwave components is of high interest for the cost-effective and rapid prototyping or manufacture of devices with complex geometries. Here, we present an experimental study on the properties of recently demonstrated microwave resonator cavities manufactured by AM, in view of their applications to high-performance compact atomic clocks. The microwave cavities employ a loop-gap geometry using six electrodes. The critical electrode structures were manufactured monolithically using two different approaches: Stereolithography (SLA) of a polymer followed by metal coating and Selective Laser Melting (SLM) of aluminum. The tested microwave cavities show the desired TE011-like resonant mode at the Rb clock frequency of ≈6.835 GHz, with a microwave magnetic field highly parallel to the quantization axis across the vapor cell. When operated in an atomic clock setup, the measured atomic Rabi oscillations are comparable to those observed for conventionally manufactured cavities and indicate a good uniformity of the field amplitude across the vapor cell. Employing a time-domain Ramsey scheme on one of the SLA cavities, high-contrast (34%) Ramsey fringes are observed for the Rb clock transition, along with a narrow (166 Hz linewidth) central fringe. The measured clock stability of 2.2 × 10-13 τ-1/2 up to the integration time of 30 s is comparable to the current state-of-the-art stabilities of compact vapor-cell clocks based on conventional microwave cavities and thus demonstrates the feasibility of the approach.

Reinforcement of single-walled carbon nanotube bundles by intertube bridging

NASA Astrophysics Data System (ADS)

Kis, A.; Csányi, G.; Salvetat, J.-P.; Lee, Thien-Nga; Couteau, E.; Kulik, A. J.; Benoit, W.; Brugger, J.; Forró, L.

2004-03-01

During their production, single-walled carbon nanotubes form bundles. Owing to the weak van der Waals interaction that holds them together in the bundle, the tubes can easily slide on each other, resulting in a shear modulus comparable to that of graphite. This low shear modulus is also a major obstacle in the fabrication of macroscopic fibres composed of carbon nanotubes. Here, we have introduced stable links between neighbouring carbon nanotubes within bundles, using moderate electron-beam irradiation inside a transmission electron microscope. Concurrent measurements of the mechanical properties using an atomic force microscope show a 30-fold increase of the bending modulus, due to the formation of stable crosslinks that effectively eliminate sliding between the nanotubes. Crosslinks were modelled using first-principles calculations, showing that interstitial carbon atoms formed during irradiation in addition to carboxyl groups, can independently lead to bridge formation between neighbouring nanotubes.

Binding of dinitrogen to an iron-sulfur-carbon site

NASA Astrophysics Data System (ADS)

Čorić, Ilija; Mercado, Brandon Q.; Bill, Eckhard; Vinyard, David J.; Holland, Patrick L.

2015-10-01

Nitrogenases are the enzymes by which certain microorganisms convert atmospheric dinitrogen (N2) to ammonia, thereby providing essential nitrogen atoms for higher organisms. The most common nitrogenases reduce atmospheric N2 at the FeMo cofactor, a sulfur-rich iron-molybdenum cluster (FeMoco). The central iron sites that are coordinated to sulfur and carbon atoms in FeMoco have been proposed to be the substrate binding sites, on the basis of kinetic and spectroscopic studies. In the resting state, the central iron sites each have bonds to three sulfur atoms and one carbon atom. Addition of electrons to the resting state causes the FeMoco to react with N2, but the geometry and bonding environment of N2-bound species remain unknown. Here we describe a synthetic complex with a sulfur-rich coordination sphere that, upon reduction, breaks an Fe-S bond and binds N2. The product is the first synthetic Fe-N2 complex in which iron has bonds to sulfur and carbon atoms, providing a model for N2 coordination in the FeMoco. Our results demonstrate that breaking an Fe-S bond is a chemically reasonable route to N2 binding in the FeMoco, and show structural and spectroscopic details for weakened N2 on a sulfur-rich iron site.

Single-walled carbon nanotubes coated with ZnO by atomic layer deposition

NASA Astrophysics Data System (ADS)

Pal, Partha P.; Gilshteyn, Evgenia; Jiang, Hua; Timmermans, Marina; Kaskela, Antti; Tolochko, Oleg V.; Kurochkin, Alexey V.; Karppinen, Maarit; Nisula, Mikko; Kauppinen, Esko I.; Nasibulin, Albert G.

2016-12-01

The possibility of ZnO deposition on the surface of single-walled carbon nanotubes (SWCNTs) with the help of an atomic layer deposition (ALD) technique was successfully demonstrated. The utilization of pristine SWCNTs as a support resulted in a non-uniform deposition of ZnO in the form of nanoparticles. To achieve uniform ZnO coating, the SWCNTs first needed to be functionalized by treating the samples in a controlled ozone atmosphere. The uniformly ZnO coated SWCNTs were used to fabricate UV sensing devices. An UV irradiation of the ZnO coated samples turned them from hydrophobic to hydrophilic behaviour. Furthermore, thin films of the ZnO coated SWCNTs allowed us switch p-type field effect transistors made of pristine SWCNTs to have ambipolar characteristics.

Single-walled carbon nanotubes coated with ZnO by atomic layer deposition.

PubMed

Pal, Partha P; Gilshteyn, Evgenia; Jiang, Hua; Timmermans, Marina; Kaskela, Antti; Tolochko, Oleg V; Karppinen, Maarit; Nisula, Mikko; Kauppinen, Esko I; Nasibulin, Albert G

2016-12-02

The possibility of ZnO deposition on the surface of single-walled carbon nanotubes (SWCNTs) with the help of an atomic layer deposition (ALD) technique was successfully demonstrated. The utilization of pristine SWCNTs as a support resulted in a non-uniform deposition of ZnO in the form of nanoparticles. To achieve uniform ZnO coating, the SWCNTs first needed to be functionalized by treating the samples in a controlled ozone atmosphere. The uniformly ZnO coated SWCNTs were used to fabricate UV sensing devices. An UV irradiation of the ZnO coated samples turned them from hydrophobic to hydrophilic behaviour. Furthermore, thin films of the ZnO coated SWCNTs allowed us switch p-type field effect transistors made of pristine SWCNTs to have ambipolar characteristics.

Thermal characteristics of carbon fiber reinforced epoxy containing multi-walled carbon nanotubes

NASA Astrophysics Data System (ADS)

Lee, Jin-woo; Park, Soo-Jeong; Kim, Yun-hae; Riichi-Murakami

2018-06-01

The material with irregular atomic structures such as polymer material exhibits low thermal conductivity because of the complex structural properties. Even materials with same atomic configurations, thermal conductivity may be different based on their structural properties. It is expected that nanoparticles with conductivity will change non-conductive polymer base materials to electrical conductors, and improve the thermal conductivity even with extremely small filling amount. Nano-composite materials contain nanoparticles with a higher surface ratio which makes the higher interface percentage to the total surface of nanoparticles. Therefore, thermal resistance of the interface becomes a dominating factor determines the effective thermal conductivity in nano-composite materials. Carbon fiber has characteristic of resistance or magnetic induction and Also, Carbon nanotube (CNT) has electronic and thermal property. It can be applied for heating system. These characteristic are used as heating composite. In this research, the exothermic characteristics of Carbon fiber reinforced composite added CNT were evaluated depend on CNT length and particle size. It was found that the CNT dispersed in the resin reduces the resistance between the interfaces due to the decrease in the total resistance of the heating element due to the addition of CNTs. It is expected to improve the life and performance of the carbon fiber composite material as a result of the heating element resulting from this paper.

Fe Isolated Single Atoms on S, N Codoped Carbon by Copolymer Pyrolysis Strategy for Highly Efficient Oxygen Reduction Reaction.

PubMed

Li, Qiheng; Chen, Wenxing; Xiao, Hai; Gong, Yue; Li, Zhi; Zheng, Lirong; Zheng, Xusheng; Yan, Wensheng; Cheong, Weng-Chon; Shen, Rongan; Fu, Ninghua; Gu, Lin; Zhuang, Zhongbin; Chen, Chen; Wang, Dingsheng; Peng, Qing; Li, Jun; Li, Yadong

2018-06-01

Heteroatom-doped Fe-NC catalyst has emerged as one of the most promising candidates to replace noble metal-based catalysts for highly efficient oxygen reduction reaction (ORR). However, delicate controls over their structure parameters to optimize the catalytic efficiency and molecular-level understandings of the catalytic mechanism are still challenging. Herein, a novel pyrrole-thiophene copolymer pyrolysis strategy to synthesize Fe-isolated single atoms on sulfur and nitrogen-codoped carbon (Fe-ISA/SNC) with controllable S, N doping is rationally designed. The catalytic efficiency of Fe-ISA/SNC shows a volcano-type curve with the increase of sulfur doping. The optimized Fe-ISA/SNC exhibits a half-wave potential of 0.896 V (vs reversible hydrogen electrode (RHE)), which is more positive than those of Fe-isolated single atoms on nitrogen codoped carbon (Fe-ISA/NC, 0.839 V), commercial Pt/C (0.841 V), and most reported nonprecious metal catalysts. Fe-ISA/SNC is methanol tolerable and shows negligible activity decay in alkaline condition during 15 000 voltage cycles. X-ray absorption fine structure analysis and density functional theory calculations reveal that the incorporated sulfur engineers the charges on N atoms surrounding the Fe reactive center. The enriched charge facilitates the rate-limiting reductive release of OH* and therefore improved the overall ORR efficiency. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Inorganic carbon addition stimulates snow algae primary productivity

NASA Astrophysics Data System (ADS)

Hamilton, T. L.; Havig, J. R.

2017-12-01

Earth has experienced glacial/interglacial oscillations throughout its history. Today over 15 million square kilometers (5.8 million square miles) of Earth's land surface is covered in ice including glaciers, ice caps, and the ice sheets of Greenland and Antarctica, most of which are retreating as a consequence of increased atmospheric CO2. Glaciers are teeming with life and supraglacial snow and ice surfaces are often red due to blooms of photoautotrophic algae. Recent evidence suggests the red pigmentation, secondary carotenoids produced in part to thrive under high irradiation, lowers albedo and accelerates melt. However, there are relatively few studies that report the productivity of snow algae communities and the parameters that constrain their growth on snow and ice surfaces. Here, we demonstrate that snow algae primary productivity can be stimulated by the addition of inorganic carbon. We found an increase in light-dependent carbon assimilation in snow algae microcosms amended with increasing amounts of inorganic carbon. Our snow algae communities were dominated by typical cosmopolitan snow algae species recovered from Alpine and Arctic environments. The climate feedbacks necessary to enter and exit glacial/interglacial oscillations are poorly understood. Evidence and models agree that global Snowball events are accompanied by changes in atmospheric CO2 with increasing CO2 necessary for entering periods of interglacial time. Our results demonstrate a positive feedback between increased CO2 and snow algal productivity and presumably growth. With the recent call for bio-albedo effects to be considered in climate models, our results underscore the need for robust climate models to include feedbacks between supraglacial primary productivity, albedo, and atmospheric CO2.

Carbonyl Activation by Borane Lewis Acid Complexation: Transition States of H2 Splitting at the Activated Carbonyl Carbon Atom in a Lewis Basic Solvent and the Proton-Transfer Dynamics of the Boroalkoxide Intermediate.

PubMed

Heshmat, Mojgan; Privalov, Timofei

2017-07-06

By using transition-state (TS) calculations, we examined how Lewis acid (LA) complexation activates carbonyl compounds in the context of hydrogenation of carbonyl compounds by H 2 in Lewis basic (ethereal) solvents containing borane LAs of the type (C 6 F 5 ) 3 B. According to our calculations, LA complexation does not activate a ketone sufficiently enough for the direct addition of H 2 to the O=C unsaturated bond; but, calculations indicate a possibly facile heterolytic cleavage of H 2 at the activated and thus sufficiently Lewis acidic carbonyl carbon atom with the assistance of the Lewis basic solvent (i.e., 1,4-dioxane or THF). For the solvent-assisted H 2 splitting at the carbonyl carbon atom of (C 6 F 5 ) 3 B adducts with different ketones, a number of TSs are computed and the obtained results are related to insights from experiment. By using the Born-Oppenheimer molecular dynamics with the DFT for electronic structure calculations, the evolution of the (C 6 F 5 ) 3 B-alkoxide ionic intermediate and the proton transfer to the alkoxide oxygen atom were investigated. The results indicate a plausible hydrogenation mechanism with a LA, that is, (C 6 F 5 ) 3 B, as a catalyst, namely, 1) the step of H 2 cleavage that involves a Lewis basic solvent molecule plus the carbonyl carbon atom of thermodynamically stable and experimentally identifiable (C 6 F 5 ) 3 B-ketone adducts in which (C 6 F 5 ) 3 B is the "Lewis acid promoter", 2) the transfer of the solvent-bound proton to the oxygen atom of the (C 6 F 5 ) 3 B-alkoxide intermediate giving the (C 6 F 5 ) 3 B-alcohol adduct, and 3) the S N 2-style displacement of the alcohol by a ketone or a Lewis basic solvent molecule. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Effect of additional elements on compositional modulated atomic layered structure of hexagonal Co{sub 80}Pt{sub 20} alloy films with superlattice diffraction

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

Hinata, Shintaro; Research Fellowship Division Japan Society for the Promotion of Science; Yamane, Akira

2016-05-15

The effect of additional element on compositionally modulated atomic layered structure of hexagonal Co{sub 80}Pt{sub 20} alloy films with superlattice diffraction was investigated. In this study it is found that the addition of Cr or W element to Co{sub 80}Pt{sub 20} alloy film shows less deterioration of hcp stacking structure and compositionally modulated atomic layer stacking structure as compared to Si or Zr or Ti with K{sub u} of around 1.4 or 1.0 × 10{sup 7} erg/cm{sup 3} at 5 at.% addition. Furthermore, for O{sub 2} addition of O{sub 2} ≥ 5.0 × 10{sup −3} Pa to CoPt alloy, compositionallymore » modulated atomic layer stacking structure will be deteriorated with enhancement of formation of hcp stacking structure which leads higher K{sub u} of 1.0 × 10{sup 7} erg/cm{sup 3}.« less

New method for binder and carbon black detection at nanometer scale in carbon electrodes for lithium ion batteries

NASA Astrophysics Data System (ADS)

Pfaffmann, Lukas; Jaiser, Stefan; Müller, Marcus; Scharfer, Philip; Schabel, Wilhelm; Bauer, Werner; Scheiba, Frieder; Ehrenberg, Helmut

2017-09-01

In the current work, graphite electrodes comprising PVDF binder and carbon black are subjected to characterization. An energy selective backscatter detector is used to localize carbon black and fluorine of PVDF. Therefore, it is necessary to distinguish between graphite, amorphous carbon and fluorine rich regions. Typically, an angular selective backscatter detector is employed to obtain an image providing the material contrast of the sample. Suitable materials for that detector are e.g. alloys to observe intermetallic phases, semiconductor for ;channeling contrast;, or imaging SiO2 and Au nanoparticles in biological cells. However, this detector cannot be used to distinguish between light elements with low atomic numbers, such as C to P. In addition, the contrast of fluorine rich regions and graphite is poor in normal in-lens images due to the low difference of the atomic mass between C and F. The aim of this study is to enhance the contrast of fluorine rich regions to graphite to carbon black. Therefore, the energy selective backscatter detector is used and its advantages and setup is described. Finally this technique is applied to investigate 400 μm thick cross-sections of graphite electrodes dried at different temperatures and obtain the carbon black distribution.

Influence of Si addition on the carbon partitioning process in martensitic-austenitic stainless steels

NASA Astrophysics Data System (ADS)

Huang, Q.; Volkova, O.; De Cooman, BC; Biermann, H.; Mola, J.

2018-06-01

The effect of Si on the efficiency of carbon partitioning during quenching and partitioning (Q&P) processing of stainless steels was studied. For this purpose, 2 mass-% Si was added to a Fe-13Cr-0.47C reference steel. The Si-free (reference) and Si-added steels were subjected to Q&P cycles in dilatometer. The carbon enrichment of austenite in both steels was evaluated by determining the temperature interval between the quench temperature and the martensite start temperature of secondary martensite formed during final cooling to room temperature. In Q&P cycles with comparable martensite fractions at the quench temperature, the carbon enrichment of austenite after partitioning was similar for both steels. To compare the mechanical stability of austenite, Q&P-processed specimens of both steels were tensile tested in the temperature range 20-200 °C. The quench and partitioning temperatures were room temperature and 450 °C, respectively. Si addition had no meaningful influence on mechanical stability of austenite. The results indicate that the suppression of cementite formation by Si addition to stainless steels, as confirmed by transmission electron microscopy examinations, has no noticeable influence on the carbon enrichment of austenite in the partitioning step.

Boosting Bifunctional Oxygen Electrolysis for N-Doped Carbon via Bimetal Addition.

PubMed

Wang, Jian; Ciucci, Francesco

2017-04-01

The addition of transition metals, even in a trace amount, into heteroatom-doped carbon (M-N/C) is intensively investigated to further enhance oxygen reduction reaction (ORR) activity. However, the influence of metal decoration on the electrolysis of the reverse reaction of ORR, that is, oxygen evolution reaction (OER), is seldom reported. Moreover, further improving the bifunctional activity and corrosion tolerance for carbon-based materials remains a big challenge, especially in OER potential regions. Here, bimetal-decorated, pyridinic N-dominated large-size carbon tubes (MM'-N/C) are proposed for the first time as highly efficient and durable ORR and OER catalysts. FeFe-N/C, CoCo-N/C, NiNi-N/C, MnMn-N/C, FeCo-N/C, NiFe-N/C, FeMn-N/C, CoNi-N/C, MnCo-N/C, and NiMn-N/C are systematically investigated in terms of their structure, composition, morphology, surface area, and active site densities. In contrast to conventional monometal and N-decorated carbon, small amounts of bimetal (≈2 at%) added during the one-step template-free synthesis contribute to increased pyridinic N content, much longer and more robust carbon tubes, reduced metal particle size, and stronger coupling between the encapsulated metals and carbon support. The synergy of those factors accounts for the dramatically improved ORR and OER activity and stability. By comparison, NiFe-N/C and MnCo-N/C stand out and achieve superior bifunctional oxygen catalytic performance, exceeding most of state-of-the-art catalysts. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Reduction of nitrate in aquifer microcosms by carbon additions

USGS Publications Warehouse

Obenhuber, Donald C.; Lowrance , Richard

1991-01-01

Aquifer microcosms were used to examine the effects of NO−3 and C amendments on groundwater from the Claiborne aquifer. Nitrate concentrations of 12.17 mg L−1 in aquifer microcosms were reduced 0.92%/d to 5.84 mg L−1 by the addition of 10 mg C L−1 for 35 d. Nitrate disappearance correlated with increases in number of denitrifiers and dissolved N2O concentration and decreases in dissolved oxygen, suggesting biological denitrification. Nitrate/chloride ratios decreased in microcosms with 10 mg C L−1 added and then increased when the C addition was removed. Carbon additions of 0.4 mg C L−1 had no effect on the microbial or chemical properties of the microcosms. Nitrous oxide levels in wells sampling the Claiborne aquifer showed an increase with depth, indicating N2O production within the aquifer. Microcosms are useful tools to examine biological transformations of chemical contaminants in unconsolidated aquifer material. The remediation of NO−3 contaminated aquifers by organic infusion is possible and appears to be a function of microbial denitrification.

H-atom addition and abstraction reactions in mixed CO, H2CO and CH3OH ices - an extended view on complex organic molecule formation

NASA Astrophysics Data System (ADS)

Chuang, K.-J.; Fedoseev, G.; Ioppolo, S.; van Dishoeck, E. F.; Linnartz, H.

2016-01-01

Complex organic molecules (COMs) have been observed not only in the hot cores surrounding low- and high-mass protostars, but also in cold dark clouds. Therefore, it is interesting to understand how such species can be formed without the presence of embedded energy sources. We present new laboratory experiments on the low-temperature solid state formation of three complex molecules - methyl formate (HC(O)OCH3), glycolaldehyde (HC(O)CH2OH) and ethylene glycol (H2C(OH)CH2OH) - through recombination of free radicals formed via H-atom addition and abstraction reactions at different stages in the CO→H2CO→CH3OH hydrogenation network at 15 K. The experiments extend previous CO hydrogenation studies and aim at resembling the physical-chemical conditions typical of the CO freeze-out stage in dark molecular clouds, when H2CO and CH3OH form by recombination of accreting CO molecules and H-atoms on ice grains. We confirm that H2CO, once formed through CO hydrogenation, not only yields CH3OH through ongoing H-atom addition reactions, but is also subject to H-atom-induced abstraction reactions, yielding CO again. In a similar way, H2CO is also formed in abstraction reactions involving CH3OH. The dominant methanol H-atom abstraction product is expected to be CH2OH, while H-atom additions to H2CO should at least partially proceed through CH3O intermediate radicals. The occurrence of H-atom abstraction reactions in ice mantles leads to more reactive intermediates (HCO, CH3O and CH2OH) than previously thought, when assuming sequential H-atom addition reactions only. This enhances the probability to form COMs through radical-radical recombination without the need of UV photolysis or cosmic rays as external triggers.

Site specific atomic polarizabilities in endohedral fullerenes and carbon onions

NASA Astrophysics Data System (ADS)

Zope, Rajendra R.; Bhusal, Shusil; Basurto, Luis; Baruah, Tunna; Jackson, Koblar

2015-08-01

We investigate the polarizability of trimetallic nitride endohedral fullerenes by partitioning the total polarizability into site specific components. This analysis indicates that the polarizability of the endohedral fullerene is essentially due to the outer fullerene cage and has insignificant contribution from the encapsulated unit. Thus, the outer fullerene cages effectively shield the encapsulated clusters and behave like Faraday cages. The polarizability of endohedral fullerenes is slightly smaller than the polarizability of the corresponding bare carbon fullerenes. The application of the site specific polarizabilities to C60@C240 and C60@C180 onions shows that, compared to the polarizability of isolated C60 fullerene, the encapsulation of the C60 in C240 and C180 fullerenes reduces its polarizability by 75% and 83%, respectively. The differences in the polarizability of C60 in the two onions is a result of differences in the bonding (intershell electron transfer), fullerene shell relaxations, and intershell separations. The site specific analysis further shows that the outer atoms in a fullerene shell contribute most to the fullerene polarizability.

Site specific atomic polarizabilities in endohedral fullerenes and carbon onions.

PubMed

Zope, Rajendra R; Bhusal, Shusil; Basurto, Luis; Baruah, Tunna; Jackson, Koblar

2015-08-28

We investigate the polarizability of trimetallic nitride endohedral fullerenes by partitioning the total polarizability into site specific components. This analysis indicates that the polarizability of the endohedral fullerene is essentially due to the outer fullerene cage and has insignificant contribution from the encapsulated unit. Thus, the outer fullerene cages effectively shield the encapsulated clusters and behave like Faraday cages. The polarizability of endohedral fullerenes is slightly smaller than the polarizability of the corresponding bare carbon fullerenes. The application of the site specific polarizabilities to C60@C240 and C60@C180 onions shows that, compared to the polarizability of isolated C60 fullerene, the encapsulation of the C60 in C240 and C180 fullerenes reduces its polarizability by 75% and 83%, respectively. The differences in the polarizability of C60 in the two onions is a result of differences in the bonding (intershell electron transfer), fullerene shell relaxations, and intershell separations. The site specific analysis further shows that the outer atoms in a fullerene shell contribute most to the fullerene polarizability.

Application of gas-fluid atomization technology in ultrosonic vibration cutting titanium alloy workpiece

NASA Astrophysics Data System (ADS)

Zhou, Zhimin; Zhang, Yuangliang; Li, Xiaoyan; Sun, Baoyuan

2009-11-01

To further improve machined surface quality of diamond cutting titanium workpiece and reduce diamond tool wear, it puts forward a kind of machining technology with mixture of carbon dioxide gas, water and vegetable oil atomized mist as cooling media in the paper. The cooling media is sprayed to cutting area through gas-liquid atomizer device to achieve purpose of cooling, lubricating, and protecting diamond tool. Experiments indicate that carbon dioxide gas can touch cutting surface more adequately through using gas-liquid atomization technology, which makes iron atoms of cutting surface cause a chemical reaction directly with carbon in carbon dioxide gas and reduce graphitizing degree of diamond tool. Thus, this technology of using gas-liquid atomization and ultrasonic vibration together for cutting Titanium Alloy is able to improve machined surface quality of workpiece and slow of diamond tool wear.

Metal-Assisted Oxo Atom Addition to an Fe(III) Thiolate.

PubMed

Villar-Acevedo, Gloria; Lugo-Mas, Priscilla; Blakely, Maike N; Rees, Julian A; Ganas, Abbie S; Hanada, Erin M; Kaminsky, Werner; Kovacs, Julie A

2017-01-11

Cysteinate oxygenation is intimately tied to the function of both cysteine dioxygenases (CDOs) and nitrile hydratases (NHases), and yet the mechanisms by which sulfurs are oxidized by these enzymes are unknown, in part because intermediates have yet to be observed. Herein, we report a five-coordinate bis-thiolate ligated Fe(III) complex, [Fe III (S 2 Me2 N 3 (Pr,Pr))] + (2), that reacts with oxo atom donors (PhIO, IBX-ester, and H 2 O 2 ) to afford a rare example of a singly oxygenated sulfenate, [Fe III (η 2 -S Me2 O)(S Me2 )N 3 (Pr,Pr)] + (5), resembling both a proposed intermediate in the CDO catalytic cycle and the essential NHase Fe-S(O) Cys114 proposed to be intimately involved in nitrile hydrolysis. Comparison of the reactivity of 2 with that of a more electron-rich, crystallographically characterized derivative, [Fe III S 2 Me2 N Me N 2 amide (Pr,Pr)] - (8), shows that oxo atom donor reactivity correlates with the metal ion's ability to bind exogenous ligands. Density functional theory calculations suggest that the mechanism of S-oxygenation does not proceed via direct attack at the thiolate sulfurs; the average spin-density on the thiolate sulfurs is approximately the same for 2 and 8, and Mulliken charges on the sulfurs of 8 are roughly twice those of 2, implying that 8 should be more susceptible to sulfur oxidation. Carboxamide-ligated 8 is shown to be unreactive towards oxo atom donors, in contrast to imine-ligated 2. Azide (N 3 - ) is shown to inhibit sulfur oxidation with 2, and a green intermediate is observed, which then slowly converts to sulfenate-ligated 5. This suggests that the mechanism of sulfur oxidation involves initial coordination of the oxo atom donor to the metal ion. Whether the green intermediate is an oxo atom donor adduct, Fe-O═I-Ph, or an Fe(V)═O remains to be determined.

Comparison of adsorption behavior of PCDD/Fs on carbon nanotubes and activated carbons in a bench-scale dioxin generating system.

PubMed

Zhou, Xujian; Li, Xiaodong; Xu, Shuaixi; Zhao, Xiyuan; Ni, Mingjiang; Cen, Kefa

2015-07-01

Porous carbon-based materials are commonly used to remove various organic and inorganic pollutants from gaseous and liquid effluents and products. In this study, the adsorption of dioxins on both activated carbons and multi-walled carbon nanotube was internally compared, via series of bench scale experiments. A laboratory-scale dioxin generator was applied to generate PCDD/Fs with constant concentration (8.3 ng I-TEQ/Nm(3)). The results confirm that high-chlorinated congeners are more easily adsorbed on both activated carbons and carbon nanotubes than low-chlorinated congeners. Carbon nanotubes also achieved higher adsorption efficiency than activated carbons even though they have smaller BET-surface. Carbon nanotubes reached the total removal efficiency over 86.8 % to be compared with removal efficiencies of only 70.0 and 54.2 % for the two other activated carbons tested. In addition, because of different adsorption mechanisms, the removal efficiencies of carbon nanotubes dropped more slowly with time than was the case for activated carbons. It could be attributed to the abundant mesopores distributed in the surface of carbon nanotubes. They enhanced the pore filled process of dioxin molecules during adsorption. In addition, strong interactions between the two benzene rings of dioxin molecules and the hexagonal arrays of carbon atoms in the surface make carbon nanotubes have bigger adsorption capacity.

Effect of alcohol addition on shock-initiated formation of soot from benzene

NASA Technical Reports Server (NTRS)

Frenklach, Michael; Yuan, Tony

1988-01-01

Soot formation in benzene-methanol and benzene-ethanol argon-diluted mixtures was studied behind reflected shock waves by monitoring the attenuation of an He-Ne laser beam. The experiments were performed at temperatures 1580-2250 K, pressures 2.0-3.0 bar, and total carbon atom concentrations (2.0-2.7) x 10 to the 17th atoms/cu cm. The results obtained indicate that the addition of alcohol suppresses the formation of soot from benzene at all temperatures, and that the reduction in soot yields is increased with the amount of alcohol added. The analysis of the results indicates that the suppression effect is probably due to the oxidation of soot and soot precursors by OH and the removal of hydrogen atoms by alcohol and water molecules.

Effects of nutrient additions on ecosystem carbon cycle in a Puerto Rican tropical wet forest

Treesearch

YIQING LI; MING XU; XIAOMING ZOU

2006-01-01

Wet tropical forests play a critical role in global ecosystem carbon (C) cycle, but C allocation and the response of different C pools to nutrient addition in these forests remain poorly understood. We measured soil organic carbon (SOC), litterfall, root biomass, microbial biomass and soil physical and chemical properties in a wet tropical forest from May 1996 to July...

From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media.

PubMed

Jiao, Long; Wan, Gang; Zhang, Rui; Zhou, Hua; Yu, Shu-Hong; Jiang, Hai-Long

2018-05-09

It remains highly desired but a great challenge to achieve atomically dispersed metals in high loadings for efficient catalysis. Now porphyrinic metal-organic frameworks (MOFs) have been synthesized based on a novel mixed-ligand strategy to afford high-content (1.76 wt %) single-atom (SA) iron-implanted N-doped porous carbon (Fe SA -N-C) via pyrolysis. Thanks to the single-atom Fe sites, hierarchical pores, oriented mesochannels and high conductivity, the optimized Fe SA -N-C exhibits excellent oxygen reduction activity and stability, surpassing almost all non-noble-metal catalysts and state-of-the-art Pt/C, in both alkaline and more challenging acidic media. More far-reaching, this MOF-based mixed-ligand strategy opens a novel avenue to the precise fabrication of efficient single-atom catalysts. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Carbon dioxide adsorbents containing magnesium oxide suitable for use at high temperatures

DOEpatents

Mayorga, Steven Gerard; Weigel, Scott Jeffrey; Gaffney, Thomas Richard; Brzozowski, Jeffrey Richard

2001-01-01

Adsorption of carbon dioxide from gas streams at temperatures in the range of 300 to 500.degree. C. is carried out with a solid adsorbent containing magnesium oxide, preferably promoted with an alkali metal carbonate or bicarbonate so that the atomic ratio of alkali metal to magnesium is in the range of 0.006 to 2.60. Preferred adsorbents are made from the precipitate formed on addition of alkali metal and carbonate ions to an aqueous solution of a magnesium salt. Atomic ratios of alkali metal to magnesium can be adjusted by washing the precipitate with water. Low surface area adsorbents can be made by dehydration and CO.sub.2 removal of magnesium hydroxycarbonate, with or without alkali metal promotion. The process is especially valuable in pressure swing adsorption operations.

Geometry at the aliphatic tertiary carbon atom: computational and experimental test of the Walsh rule.

PubMed

Böhm, Stanislav; Exner, Otto

2004-02-01

The geometrical parameters of molecules of 2-substituted 2-methylpropanes and 1-substituted bicyclo[2.2.2]octanes were calculated at the B3LYP/6-311+G(d,p) level. They agreed reasonably well with the mean crystallographic values retrieved from the Cambridge Structural Database for a set of diverse non-cyclic structures with a tertiary C atom. The angle deformations at this C atom produced by the immediately bonded substituent are also closely related to those observed previously in benzene mono derivatives (either as calculated or as derived from crystallographic data). The calculated geometrical parameters were used to test the classical Walsh rule: It is evidently true that an electron-attracting substituent increases the proportion of C-atom p-electrons in the bond to the substituent and leaves more s-electrons to the remaining bonds; as a consequence the C-C-C angles at a tertiary carbon are widened and the C-C bonds shortened. However, this rule describes only part of the reality since the bond angles and lengths are controlled by other factors as well, for instance by steric crowding. Another imperfection of the Walsh rule is that the sequence of substituents does not correspond to their electronegativities, as measured by any known scale; more probably it is connected with the inductive effect, but then only very roughly.

Effect of organic additives on characteristics of carbon-coated LiCoPO4 synthesized by hydrothermal method

NASA Astrophysics Data System (ADS)

Maeyoshi, Yuta; Miyamoto, Shohei; Noda, Yusaku; Munakata, Hirokazu; Kanamura, Kiyoshi

2017-01-01

Carbon-coated LiCoPO4 particles are synthesized by one-pot hydrothermal process using three different organic additives (carboxymethylcellulose sodium salt (CMC), glucose, and ascorbic acid). The effect of the organic additives on particle size, morphology, nature of carbon coating, and electrochemical property of the resulting LiCoPO4 is investigated. CMC plays important roles to decrease the particle size and form well-covered carbon coating on the surface. Carbon-coated LiCoPO4 prepared using CMC delivers higher initial discharge capacity of 135 mA h g-1 at 0.1 C, and shows superior rate capability and cyclic performance than the other samples. The improved electrochemical characteristics are attributed to not only the fine particle which allows facile electronic and ionic transport, but also the high coverage of carbon coating which improves the electrical conductivity and prevents the irreversible reactions of the charged LiCoPO4 with electrolyte.

Lubricants or lubricant additives composed of ionic liquids containing ammonium cations

DOEpatents

Qu, Jun [Knoxville, TN; Truhan, Jr; John, J [Cookeville, TN; Dai, Sheng [Knoxville, TN; Luo, Huimin [Knoxville, TN; Blau, Peter J [Knoxville, TN

2010-07-13

A lubricant or lubricant additive is an ionic liquid alkylammonium salt. The alkylammonium salt has the structure R.sub.xNH.sub.(4-x).sup.+,[F.sub.3C(CF.sub.2).sub.yS(O).sub.2].sub.2N.sup- .- where x is 1 to 3, R is independently C.sub.1 to C.sub.12 straight chain alkyl, branched chain alkyl, cycloalkyl, alkyl substituted cycloalkyl, cycloalkyl substituted alkyl, or, optionally, when x is greater than 1, two R groups comprise a cyclic structure including the nitrogen atom and 4 to 12 carbon atoms, and y is independently 0 to 11. The lubricant is effective for the lubrication of many surfaces including aluminum and ceramics surfaces.

Synthesis of barium and strontium carbonate crystals with unusual morphologies using an organic additive

NASA Astrophysics Data System (ADS)

Chen, Long; Jiang, Jizhong; Bao, Zuben; Pan, Jian; Xu, Weibing; Zhou, Lili; Wu, Zhigang; Chen, Xu

2013-12-01

In this paper, strontium carbonate (SrCO3) and barium carbonate (BaCO3) crystals were synthesized in the presence of an organic additive-hexamethylenetetramine (HMT) using two CO2 sources. Scanning electron microscopy and X-ray powder diffractometry were used to characterize the products. The results showed that the morphologies of orthorhombic strontianite SrCO3 transformed from branch-like to flower-like, and to capsicum-like at last, while the morphologies of BaCO3 change from fiber-like to branchlike, and to rod-like finally with an increase of the molar ratio HMT/Sr2+ and HMT/Ba2+ from 0.2 to 10 using ammonium carbonate as CO2 source. When using diethyl carbonate instead of ammonium carbonate as CO2 source, SrCO3 flowers aggregated by rods and BaCO3 shuttles were formed. The possible formation mechanisms of SrCO3 and BaCO3 crystals obtained in different conditions were also discussed.

Roles of additives and surface control in slurry atomization. Final project report

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

Tsai, S.C.

1992-12-31

This project studies the rheology and airblast atomization of micronized coal slurries. Its major objectives are (1) to promote further understanding of the mechanisms and the roles of additives in airblast atomization of coal water slurry (CWS), and (2) to investigate the impacts of coal particle surface properties and interparticle forces on CWS rheology. We have found that the flow behavior index (n) of a suspension (or slurry) is determined by the relative importance of the interparticle van der Waals attraction and the interparticle electrostatic repulsion. The interparticle attraction, measured by the Hamaker constant scaled to the thermal energy atmore » 25{degrees}C (A/kT), causes particle aggregation, which breaks down at high shear rates, and thus leads to slurry pseudoplastic behavior (n< 1). At a constant particle volume fraction and surface charge density (qualitatively measured by the zeta potential in deionized water), n decreases linearly as A/kT increases. The relative viscosity of the pseudoplastic suspension with respect to that of the suspending liquid is found to be independent of particle density and correlate well with the particle Peclet number which equals the particle diffusional relaxation time multiplied by shear rate. Specifically, the relative viscosities of the pseudoplastic glycerol/water coal slurry and the ethylene glycol/glycerol sand slurry, at same volume fractions as well as similar particle size distributions and liquid viscosities, as functions of the particle Peclet number fall along the same line.« less

First-principles study on silicon atom doped monolayer graphene

NASA Astrophysics Data System (ADS)

Rafique, Muhammad; Shuai, Yong; Hussain, Nayyar

2018-01-01

This paper illustrates the structural, electronic and optical properties of individual silicon (Si) atom-doped single layer graphene using density functional theory method. Si atom forms tight bonding with graphene layer. The effect of doping has been investigated by varying the concentration of Si atoms from 3.125% to 9.37% (i.e. From one to three Si atoms in 4 × 4 pure graphene supercell containing 32 carbon atoms), respectively. Electronic structure, partial density of states (PDOS) and optical properties of pure and Si atom-doped graphene sheet were calculated using VASP (Vienna ab-initio Simulation Package). The calculated results for pure graphene sheet were then compared with Si atom doped graphene. It is revealed that upon Si doping in graphene, a finite band gap appears at the high symmetric K-point, thereby making graphene a direct band gap semiconductor. Moreover, the band gap value is directly proportional to the concentration of impurity Si atoms present in graphene lattice. Upon analyzing the optical properties of Si atom-doped graphene structures, it is found that, there is significant change in the refractive index of the graphene after Si atom substitution in graphene. In addition, the overall absorption spectrum of graphene is decreased after Si atom doping. Although a significant red shift in absorption is found to occur towards visible range of radiation when Si atom is substituted in its lattice. The reflectivity of graphene improves in low energy region after Si atom substitution in graphene. These results can be useful for tuning the electronic structure and to manipulate the optical properties of graphene layer in the visible region.

Effect of small addition of Cr on stability of retained austenite in high carbon steel

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

Hossain, Rumana; Pahlevani, Farshid, E-mail: f.pah

High carbon steels with dual phase structures of martensite and austenite have considerable potential for industrial application in high abrasion environments due to their hardness, strength and relatively low cost. To design cost effective high carbon steels with superior properties, it is crucial to identify the effect of Chromium (Cr) on the stability of retained austenite (RA) and to fully understand its effect on solid-state phase transition. This study addresses this important knowledge gap. Using standard compression tests on bulk material, quantitative X-ray diffraction analysis, nano-indentation on individual austenitic grains, transmission electron microscopy and electron backscatter diffraction–based orientation microscopy techniques,more » the authors investigated the effect of Cr on the microstructure, transformation behaviour and mechanical stability of retained austenite in high carbon steel, with varying Cr contents. The results revealed that increasing the Cr %, altered the morphology of the RA and increased its stability, consequently, increasing the critical pressure for martensitic transformation. This study has critically addressed the elastoplastic behaviour of retained austenite – and provides a deep understanding of the effect of small additions of Cr on the metastable austenite of high carbon steel from the macro- to nano-level. Consequently, it paves the way for new applications for high carbon low alloy steels. - Highlights: • Effect of small addition of Cr on metastable austenite of high carbon steel from the macro- to nano-level • A multi-scale study of elastoplastic behaviour of retained austenite in high carbon steel • The mechanical stability of retained austenite during plastic deformation increased with increasing Cr content • Effect of grain boundary misorientation angle on hardness of individual retained austenite grains in high carbon steel.« less

Neutron diffraction of acetazolamide-bound human carbonic anhydrase II reveals atomic details of drug binding

PubMed Central

Fisher, S. Zoë; Aggarwal, Mayank; Kovalevsky, Andrey Y.; Silverman, David N.; McKenna, Robert

2012-01-01

Carbonic anhydrases (CAs) catalyze the hydration of CO2 forming HCO3− and a proton, an important reaction for many physiological processes including respiration, fluid secretion, and pH regulation. As such, CA isoforms are prominent clinical targets for treating various diseases. The clinically used acetazolamide (AZM) is a sulfonamide that binds with high affinity to human CA isoform II (HCA II). There are several X-ray structures available of AZM bound to various CA isoforms, but these complexes do not show the charged state of AZM, or hydrogen (H) atom positions of the protein and solvent. Neutron diffraction is a useful technique for directly observing H atoms and the mapping of H-bonding networks that can greatly contribute to rational drug design. To this end the neutron structure of H/D exchanged HCA II crystals in complex with AZM was determined. The structure reveals the molecular details of AZM binding and the charged state of the bound drug. This represents the first determined neutron structure of a clinically used drug bound to its target. PMID:22928733

DFT Modeling of Cross-Linked Polyethylene: Role of Gold Atoms and Dispersion Interactions.

PubMed

Blaško, Martin; Mach, Pavel; Antušek, Andrej; Urban, Miroslav

2018-02-08

Using DFT modeling, we analyze the concerted action of gold atoms and dispersion interactions in cross-linked polyethylene. Our model consists of two oligomer chains (PEn) with 7, 11, 15, 19, or 23 carbon atoms in each oligomer cross-linked with one to three Au atoms through C-Au-C bonds. In structures with a single gold atom the C-Au-C bond is located in the central position of the oligomer. Binding energies (BEs) with respect to two oligomer radical fragments and Au are as high as 362-489 kJ/mol depending on the length of the oligomer chain. When the dispersion contribution in PEn-Au-PEn oligomers is omitted, BE is almost independent of the number of carbon atoms, lying between 293 and 296 kJ/mol. The dispersion energy contributions to BEs in PEn-Au-PEn rise nearly linearly with the number of carbon atoms in the PEn chain. The carbon-carbon distance in the C-Au-C moiety is around 4.1 Å, similar to the bond distance between saturated closed shell chains in the polyethylene crystal. BEs of pure saturated closed shell PEn-PEn oligomers are 51-187 kJ/mol. Both Au atoms and dispersion interactions contribute considerably to the creation of nearly parallel chains of oligomers with reasonably high binding energies.

Silicon carbide sintered body manufactured from silicon carbide powder containing boron, silicon and carbonaceous additive

NASA Technical Reports Server (NTRS)

Tanaka, Hidehiko

1987-01-01

A silicon carbide powder of a 5-micron grain size is mixed with 0.15 to 0.60 wt% mixture of a boron compound, i.e., boric acid, boron carbide (B4C), silicon boride (SiB4 or SiB6), aluminum boride, etc., and an aluminum compound, i.e., aluminum, aluminum oxide, aluminum hydroxide, aluminum carbide, etc., or aluminum boride (AlB2) alone, in such a proportion that the boron/aluminum atomic ratio in the sintered body becomes 0.05 to 0.25 wt% and 0.05 to 0.40 wt%, respectively, together with a carbonaceous additive to supply enough carbon to convert oxygen accompanying raw materials and additives into carbon monoxide.

Exotic objects of atomic physics

NASA Astrophysics Data System (ADS)

Eletskii, A. V.

2017-11-01

There has been presented a short survey of physical properties, methods of production and exploration as well as directions of practical usage of the objects of atomic physics which are not yet described in detail in modern textbooks and manuals intended for students of technical universities. The family of these objects includes negative and multicharged ions, Rydberg atoms, excimer molecules, clusters. Besides of that, in recent decades this family was supplemented with new nanocarbon structures such as fullerenes, carbon nanotubes and graphene. The textbook “Exotic objects of atomic physics” [1] edited recently contains some information on the above-listed objects of the atomic physics. This textbook can be considered as a supplement to classic courses of atomic physics teaching in technical universities.

Studies of carbon incorporation on the diamond [100] surface during chemical vapor deposition using density functional theory.

PubMed

Cheesman, Andrew; Harvey, Jeremy N; Ashfold, Michael N R

2008-11-13

Accurate potential energy surface calculations are presented for many of the key steps involved in diamond chemical vapor deposition on the [100] surface (in its 2 x 1 reconstructed and hydrogenated form). The growing diamond surface was described by using a large (approximately 1500 atoms) cluster model, with the key atoms involved in chemical steps being described by using a quantum mechanical (QM, density functional theory, DFT) method and the bulk of the atoms being described by molecular mechanics (MM). The resulting hybrid QM/MM calculations are more systematic and/or at a higher level of theory than previous work on this growth process. The dominant process for carbon addition, in the form of methyl radicals, is predicted to be addition to a surface radical site, opening of the adjacent C-C dimer bond, insertion, and ultimate ring closure. Other steps such as insertion across the trough between rows of dimer bonds or addition to a neighboring dimer leading to formation of a reconstruction on the next layer may also contribute. Etching of carbon can also occur; the most likely mechanism involves loss of a two-carbon moiety in the form of ethene. The present higher-level calculations confirm that migration of inserted carbon along both dimer rows and chains should be relatively facile, with barriers of approximately 150 kJ mol (-1) when starting from suitable diradical species, and that this step should play an important role in establishing growth of smooth surfaces.

Production of complex organic molecules: H-atom addition versus UV irradiation

NASA Astrophysics Data System (ADS)

Chuang, K.-J.; Fedoseev, G.; Qasim, D.; Ioppolo, S.; van Dishoeck, E. F.; Linnartz, H.

2017-05-01

Complex organic molecules (COMs) have been identified in different environments in star-forming regions. Laboratory studies show that COMs form in the solid state, on icy grains, typically following a 'non-energetic' (atom-addition) or 'energetic' (UV-photon absorption) trigger. So far, such studies have been largely performed for single processes. Here, we present the first work that quantitatively investigates both the relative importance and the cumulative effect of '(non-)energetic' processing. We focus on astronomically relevant CO:CH3OH = 4:1 ice analogues exposed to doses relevant for the collapse stage of dense clouds. Hydrogenation experiments result in the formation of methyl formate (MF; HC(O)OCH3), glycolaldehyde (GA; HC(O)CH2OH) and ethylene glycol (EG; H2C(OH)CH2OH) at 14 K. The absolute abundances and the abundance fractions are found to be dependent on the H-atom/CO:CH3OH-molecule ratios and on the overall deposition rate. In the case that ices are exposed to UV photons only, several different COMs are found. Typically, the abundance fractions are 0.2 for MF, 0.3 for GA and 0.5 for EG as opposed to the values found in pure hydrogenation experiments without UV in which MF is largely absent: 0.0, 0.2-0.6 and 0.8-0.4, respectively. In experiments where both are applied, overall COM abundances drop to about half of those found in the pure UV irradiation experiments, but the composition fractions are very similar. This implies COM ratios can be used as a diagnostic tool to derive the processing history of an ice. Solid-state branching ratios derived here for GA and EG compare well with observations, while the MF case cannot be explained by solid-state conditions investigated here.

Modeling and optimization of atomic layer deposition processes on vertically aligned carbon nanotubes.

PubMed

Yazdani, Nuri; Chawla, Vipin; Edwards, Eve; Wood, Vanessa; Park, Hyung Gyu; Utke, Ivo

2014-01-01

Many energy conversion and storage devices exploit structured ceramics with large interfacial surface areas. Vertically aligned carbon nanotube (VACNT) arrays have emerged as possible scaffolds to support large surface area ceramic layers. However, obtaining conformal and uniform coatings of ceramics on structures with high aspect ratio morphologies is non-trivial, even with atomic layer deposition (ALD). Here we implement a diffusion model to investigate the effect of the ALD parameters on coating kinetics and use it to develop a guideline for achieving conformal and uniform thickness coatings throughout the depth of ultra-high aspect ratio structures. We validate the model predictions with experimental data from ALD coatings of VACNT arrays. However, the approach can be applied to predict film conformality as a function of depth for any porous topology, including nanopores and nanowire arrays.

Rare Potassium-Bearing Mica in Allan Hills 84001: Additional Constraints on Carbonate Formation

NASA Technical Reports Server (NTRS)

Brearley, A. J.

1998-01-01

There have been presented several intriguing observations suggesting evidence of fossil life in martian orthopyroxenite ALH 84001. These exciting and controversial observations have stimulated extensive debate over the origin and history of ALH 84001, but many issues still remain unresolved. Among the most important is the question of the temperature at which the carbonates, which host the putative microfossils, formed. Oxygen- isotopic data, while showing that the carbonates are generally out of isotopic equilibria with the host rock, cannot constrain their temperature of formation. Both low- and high-temperature scenarios are plausible depending on whether carbonate growth occurred in an open or closed system. Petrographic arguments have generally been used to support a high-temperature origin but these appear to be suspect because they assume equilibrium between carbonate compositions that are not in contact. Some observations appear to be consistent with shock mobilization and growth from immiscible silicate-carbonate melts at high temperatures. Proponents of a low-temperature origin for the carbonates are hampered by the fact that there is currently no evidence of hydrous phases that would indicate low temperatures and the presence of a hydrous fluid during the formation of the carbonates. However, the absence of hydrous phases does not rule out carbonate formation at low temperatures, because the carbonate forming fluids may have been extremely CO2 rich, such that hydrous phases would not have been stabilized. In this study, I have carried out additional Transmission electron microscopy (TEM) studies of ALH-84001 and have found evidence of very rare phyllosilicates, which appear to be convincingly of pre-terrestrial origin. At present these observations are limited to one occurrence: further studies are in progress to determine if the phyllosilicates are more widespread.

Atomic and molecular supernovae

NASA Technical Reports Server (NTRS)

Liu, Weihong

1997-01-01

Atomic and molecular physics of supernovae is discussed with an emphasis on the importance of detailed treatments of the critical atomic and molecular processes with the best available atomic and molecular data. The observations of molecules in SN 1987A are interpreted through a combination of spectral and chemical modelings, leading to strong constraints on the mixing and nucleosynthesis of the supernova. The non-equilibrium chemistry is used to argue that carbon dust can form in the oxygen-rich clumps where the efficient molecular cooling makes the nucleation of dust grains possible. For Type Ia supernovae, the analyses of their nebular spectra lead to strong constraints on the supernova explosion models.

Site specific atomic polarizabilities in endohedral fullerenes and carbon onions

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

Zope, Rajendra R., E-mail: rzope@utep.edu; Baruah, Tunna; Computational Science Program, The University of Texas at El Paso, El Paso, Texas 79958

2015-08-28

We investigate the polarizability of trimetallic nitride endohedral fullerenes by partitioning the total polarizability into site specific components. This analysis indicates that the polarizability of the endohedral fullerene is essentially due to the outer fullerene cage and has insignificant contribution from the encapsulated unit. Thus, the outer fullerene cages effectively shield the encapsulated clusters and behave like Faraday cages. The polarizability of endohedral fullerenes is slightly smaller than the polarizability of the corresponding bare carbon fullerenes. The application of the site specific polarizabilities to C{sub 60}@C{sub 240} and C{sub 60}@C{sub 180} onions shows that, compared to the polarizability of isolatedmore » C{sub 60} fullerene, the encapsulation of the C{sub 60} in C{sub 240} and C{sub 180} fullerenes reduces its polarizability by 75% and 83%, respectively. The differences in the polarizability of C{sub 60} in the two onions is a result of differences in the bonding (intershell electron transfer), fullerene shell relaxations, and intershell separations. The site specific analysis further shows that the outer atoms in a fullerene shell contribute most to the fullerene polarizability.« less

Quantum chemical molecular dynamics simulation of single-walled carbon nanotube cap nucleation on an iron particle.

PubMed

Ohta, Yasuhito; Okamoto, Yoshiko; Page, Alister J; Irle, Stephan; Morokuma, Keiji

2009-11-24

The atomic scale details of single-walled carbon nanotube (SWNT) nucleation on metal catalyst particles are elusive to experimental observations. Computer simulation of metal-catalyzed SWNT nucleation is a challenging topic but potentially of great importance to understand the factors affecting SWNT diameters, chirality, and growth efficiency. In this work, we use nonequilibrium density functional tight-binding molecular dynamics simulations and report nucleation of sp(2)-carbon cap structures on an iron particle consisting of 38 atoms. One C(2) molecule was placed every 1.0 ps around an Fe(38) cluster for 30 ps, after which a further 410 ps of annealing simulation without carbon supply was performed. We find that sp(2)-carbon network nucleation and annealing processes occur in three sequential and repetitive stages: (A) polyyne chains on the metal surface react with each other to evolve into a Y-shaped polyyne junction, which preferentially form a five-membered ring as a nucleus; (B) polyyne chains on the first five-membered ring form an additional fused five- or six-membered ring; and (C) pentagon-to-hexagon self-healing rearrangement takes place with the help of short-lived polyyne chains, stabilized by the mobile metal atoms. The observed nucleation process resembles the formation of a fullerene cage. However, the metal particle plays a key role in differentiating the nucleation process from fullerene cage formation, most importantly by keeping the growing cap structure from closing into a fullerene cage and by keeping the carbon edge "alive" for the addition of new carbon material.

Change of Energy of the Cubic Subnanocluster of Iron Under Influence of Interstitial and Substitutional Atoms.

PubMed

Nedolya, Anatoliy V; Bondarenko, Natalya V

2016-12-01

Energy change of an iron face-centred cubic subnanocluster was evaluated using molecular mechanics method depending on the position of a carbon interstitial atom and substitutional atoms of nickel. Calculations of all possible positions of impurity atoms show that the energy change of the system are discrete and at certain positions of the atoms are close to continuous.In terms of energy, when all impurity atoms are on the same edge of an atomic cluster, their positions are more advantageous. The presence of nickel atoms on the edge of a cubic cluster resulted in decrease of potential barrier for a carbon atom and decrease in energy in the whole cluster. A similar drift of a carbon atom from central octahedral interstitial site to the surface in the direction <011> occurred under the influence of surface factors.Such configuration corresponds to decreasing symmetry and increasing the number of possible energy states of a subnanocluster, and it corresponds to the condition of spontaneous crystallization process in an isolated system.Taking into account accidental positions of the nickel atom in the iron cluster, such behaviour of the carbon atom can explain the mechanism of growth of a new phase and formation of new clusters in the presence of other kind of atoms because of surface influence.

Delaminated graphene at silicon carbide facets: atomic scale imaging and spectroscopy.

PubMed

Nicotra, Giuseppe; Ramasse, Quentin M; Deretzis, Ioannis; La Magna, Antonino; Spinella, Corrado; Giannazzo, Filippo

2013-04-23

Atomic-resolution structural and spectroscopic characterization techniques (scanning transmission electron microscopy and electron energy loss spectroscopy) are combined with nanoscale electrical measurements (conductive atomic force microscopy) to study at the atomic scale the properties of graphene grown epitaxially through the controlled graphitization of a hexagonal SiC(0001) substrate by high temperature annealing. This growth technique is known to result in a pronounced electron-doping (∼10(13) cm(-2)) of graphene, which is thought to originate from an interface carbon buffer layer strongly bound to the substrate. The scanning transmission electron microscopy analysis, carried out at an energy below the knock-on threshold for carbon to ensure no damage is imparted to the film by the electron beam, demonstrates that the buffer layer present on the planar SiC(0001) face delaminates from it on the (112n) facets of SiC surface steps. In addition, electron energy loss spectroscopy reveals that the delaminated layer has a similar electronic configuration to purely sp2-hybridized graphene. These observations are used to explain the local increase of the graphene sheet resistance measured around the surface steps by conductive atomic force microscopy, which we suggest is due to significantly lower substrate-induced doping and a resonant scattering mechanism at the step regions. A first-principles-calibrated theoretical model is proposed to explain the structural instability of the buffer layer on the SiC facets and the resulting delamination.

Conformal atomic layer deposition of alumina on millimeter tall, vertically-aligned carbon nanotube arrays.

PubMed

Stano, Kelly L; Carroll, Murphy; Padbury, Richard; McCord, Marian; Jur, Jesse S; Bradford, Philip D

2014-11-12

Atomic layer deposition (ALD) can be used to coat high aspect ratio and high surface area substrates with conformal and precisely controlled thin films. Vertically aligned arrays of multiwalled carbon nanotubes (MWCNTs) with lengths up to 1.5 mm were conformally coated with alumina from base to tip. The nucleation and growth behaviors of Al2O3 ALD precursors on the MWCNTs were studied as a function of CNT surface chemistry. CNT surfaces were modified through a series of post-treatments including pyrolytic carbon deposition, high temperature thermal annealing, and oxygen plasma functionalization. Conformal coatings were achieved where post-treatments resulted in increased defect density as well as the extent of functionalization, as characterized by X-ray photoelectron spectroscopy and Raman spectroscopy. Using thermogravimetric analysis, it was determined that MWCNTs treated with pyrolytic carbon and plasma functionalization prior to ALD coating were more stable to thermal oxidation than pristine ALD coated samples. Functionalized and ALD coated arrays had a compressive modulus more than two times higher than a pristine array coated for the same number of cycles. Cross-sectional energy dispersive X-ray spectroscopy confirmed that Al2O3 could be uniformly deposited through the entire thickness of the vertically aligned MWCNT array by manipulating sample orientation and mounting techniques. Following the ALD coating, the MWCNT arrays demonstrated hydrophilic wetting behavior and also exhibited foam-like recovery following compressive strain.

Effect of conductive additives to gel electrolytes on activated carbon-based supercapacitors

NASA Astrophysics Data System (ADS)

Barzegar, Farshad; Dangbegnon, Julien K.; Bello, Abdulhakeem; Momodu, Damilola Y.; Johnson, A. T. Charlie; Manyala, Ncholu

2015-09-01

This article is focused on polymer based gel electrolyte due to the fact that polymers are cheap and can be used to achieve extended potential window for improved energy density of the supercapacitor devices when compared to aqueous electrolytes. Electrochemical characterization of a symmetric supercapacitor devices based on activated carbon in different polyvinyl alcohol (PVA) based gel electrolytes was carried out. The device exhibited a maximum energy density of 24 Wh kg-1 when carbon black was added to the gel electrolyte as conductive additive. The good energy density was correlated with the improved conductivity of the electrolyte medium which is favorable for fast ion transport in this relatively viscous environment. Most importantly, the device remained stable with no capacitance lost after 10,000 cycles.

High performance platinum single atom electrocatalyst for oxygen reduction reaction

NASA Astrophysics Data System (ADS)

Liu, Jing; Jiao, Menggai; Lu, Lanlu; Barkholtz, Heather M.; Li, Yuping; Wang, Ying; Jiang, Luhua; Wu, Zhijian; Liu, Di-Jia; Zhuang, Lin; Ma, Chao; Zeng, Jie; Zhang, Bingsen; Su, Dangsheng; Song, Ping; Xing, Wei; Xu, Weilin; Wang, Ying; Jiang, Zheng; Sun, Gongquan

2017-07-01

For the large-scale sustainable implementation of polymer electrolyte membrane fuel cells in vehicles, high-performance electrocatalysts with low platinum consumption are desirable for use as cathode material during the oxygen reduction reaction in fuel cells. Here we report a carbon black-supported cost-effective, efficient and durable platinum single-atom electrocatalyst with carbon monoxide/methanol tolerance for the cathodic oxygen reduction reaction. The acidic single-cell with such a catalyst as cathode delivers high performance, with power density up to 680 mW cm-2 at 80 °C with a low platinum loading of 0.09 mgPt cm-2, corresponding to a platinum utilization of 0.13 gPt kW-1 in the fuel cell. Good fuel cell durability is also observed. Theoretical calculations reveal that the main effective sites on such platinum single-atom electrocatalysts are single-pyridinic-nitrogen-atom-anchored single-platinum-atom centres, which are tolerant to carbon monoxide/methanol, but highly active for the oxygen reduction reaction.

Large-Scale Fabrication of Carbon Nanotube Probe Tips For Atomic Force Microscopy Critical Dimension Imaging Applications

NASA Technical Reports Server (NTRS)

Ye, Qi Laura; Cassell, Alan M.; Stevens, Ramsey M.; Meyyappan, Meyya; Li, Jun; Han, Jie; Liu, Hongbing; Chao, Gordon

2004-01-01

Carbon nanotube (CNT) probe tips for atomic force microscopy (AFM) offer several advantages over Si/Si3N4 probe tips, including improved resolution, shape, and mechanical properties. This viewgraph presentation discusses these advantages, and the drawbacks of existing methods for fabricating CNT probe tips for AFM. The presentation introduces a bottom up wafer scale fabrication method for CNT probe tips which integrates catalyst nanopatterning and nanomaterials synthesis with traditional silicon cantilever microfabrication technology. This method makes mass production of CNT AFM probe tips feasible, and can be applied to the fabrication of other nanodevices with CNT elements.

Method of produce ultra-low friction carbon films

DOEpatents

Erdemir, Ali; Fenske, George R.; Eryilmaz, Osman Levent; Lee, Richard H.

2003-04-15

A method and article of manufacture of amorphous diamond-like carbon. The method involves providing a substrate in a chamber, providing a mixture of a carbon containing gas and hydrogen gas with the mixture adjusted such that the atomic molar ratio of carbon to hydrogen is less than 0.3, including all carbon atoms and all hydrogen atoms in the mixture. A plasma is formed of the mixture and the amorphous diamond-like carbon film is deposited on the substrate. To achieve optimum bonding an intervening bonding layer, such as Si or SiO.sub.2, can be formed from SiH.sub.4 with or without oxidation of the layer formed.

Enhanced tortuosity for electrolytes in microwave irradiated self-organized carbon-doped Ni/Co hydroxide nanocomposite electrodes with higher Ni/Co atomic ratio and rate capability for an asymmetric supercapacitor

NASA Astrophysics Data System (ADS)

Kumar, Niraj; Kumar, Viresh; Panda, H. S.

2017-11-01

We demonstrate a green, facile and rapid microwave-mediated process for fabricating carbon black (CB) incorporated Ni/Co hydroxide porous nanocomposites and study the effect of various mass loading of CB on supercapacitor performance. The structure and interactions between CB and Ni/Co hydroxide are characterized by using x-ray diffraction, Fourier-transform infrared spectroscopy and x-ray photoelectron spectroscopy, which suggest the miniaturization of the single-phase Ni/Co hydroxide formation time. A morphology study reveals that the addition of CB into Ni/Co hydroxide develops a loose network structure with well-defined architectural pores. In addition, the nanocomposites demonstrate noticeable improvements in porosity and atomic ratio of Ni/Co with an increasing percentage of carbon, which results in a higher diffusion of electrolytes, and hence electrical conduction. The developed electrode materials exhibit a maximum specific capacitance value of 1526 Fg-1 at current density 1 Ag-1 with excellent cyclic stability (92% retention at 5000 cycles), energy density (76 Wh Kg-1), power density (250 W Kg-1) and rate capability. A solid state asymmetric supercapacitor device is fabricated and utilized to brighten a commercial LED effectively for validating real usage.

Enhanced tortuosity for electrolytes in microwave irradiated self-organized carbon-doped Ni/Co hydroxide nanocomposite electrodes with higher Ni/Co atomic ratio and rate capability for an asymmetric supercapacitor.

PubMed

Kumar, Niraj; Kumar, Viresh; Panda, H S

2017-11-03

We demonstrate a green, facile and rapid microwave-mediated process for fabricating carbon black (CB) incorporated Ni/Co hydroxide porous nanocomposites and study the effect of various mass loading of CB on supercapacitor performance. The structure and interactions between CB and Ni/Co hydroxide are characterized by using x-ray diffraction, Fourier-transform infrared spectroscopy and x-ray photoelectron spectroscopy, which suggest the miniaturization of the single-phase Ni/Co hydroxide formation time. A morphology study reveals that the addition of CB into Ni/Co hydroxide develops a loose network structure with well-defined architectural pores. In addition, the nanocomposites demonstrate noticeable improvements in porosity and atomic ratio of Ni/Co with an increasing percentage of carbon, which results in a higher diffusion of electrolytes, and hence electrical conduction. The developed electrode materials exhibit a maximum specific capacitance value of 1526 Fg -1 at current density 1 Ag -1 with excellent cyclic stability (92% retention at 5000 cycles), energy density (76 Wh Kg -1 ), power density (250 W Kg -1 ) and rate capability. A solid state asymmetric supercapacitor device is fabricated and utilized to brighten a commercial LED effectively for validating real usage.

Surface modification of nitrogen-doped carbon nanotubes by ozone via atomic layer deposition

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

Lushington, Andrew; Liu, Jian; Tang, Yongji

The use of ozone as an oxidizing agent for atomic layer deposition (ALD) processes is rapidly growing due to its strong oxidizing capabilities. However, the effect of ozone on nanostructured substrates such as nitrogen-doped multiwalled carbon nanotubes (NCNTs) and pristine multiwalled carbon nanotubes (PCNTs) are not very well understood and may provide an avenue toward functionalizing the carbon nanotube surface prior to deposition. The effects of ALD ozone treatment on NCNTs and PCNTs using 10 wt. % ozone at temperatures of 150, 250, and 300 °C are studied. The effect of ozone pulse time and ALD cycle number on NCNTs and PCNTsmore » was also investigated. Morphological changes to the substrate were observed by scanning electron microscopy and high resolution transmission electron microscopy. Brunauer-Emmett-Teller measurements were also conducted to determine surface area, pore size, and pore size distribution following ozone treatment. The graphitic nature of both NCNTs and PCNTs was determined using Raman analysis while x-ray photoelectron spectroscopy (XPS) was employed to probe the chemical nature of NCNTs. It was found that O{sub 3} attack occurs preferentially to the outermost geometric surface of NCNTs. Our research also revealed that the deleterious effects of ozone are found only on NCNTs while little or no damage occurs on PCNTs. Furthermore, XPS analysis indicated that ALD ozone treatment on NCNTs, at elevated temperatures, results in loss of nitrogen content. Our studies demonstrate that ALD ozone treatment is an effective avenue toward creating low nitrogen content, defect rich substrates for use in electrochemical applications and ALD of various metal/metal oxides.« less

Addition of granular activated carbon and trace elements to favor volatile fatty acid consumption during anaerobic digestion of food waste.

PubMed

Capson-Tojo, Gabriel; Moscoviz, Roman; Ruiz, Diane; Santa-Catalina, Gaëlle; Trably, Eric; Rouez, Maxime; Crest, Marion; Steyer, Jean-Philippe; Bernet, Nicolas; Delgenès, Jean-Philippe; Escudié, Renaud

2018-07-01

The effect of supplementing granular activated carbon and trace elements on the anaerobic digestion performance of consecutive batch reactors treating food waste was investigated. The results from the first batch suggest that addition of activated carbon favored biomass acclimation, improving acetic acid consumption and enhancing methane production. Adding trace elements allowed a faster consumption of propionic acid. A second batch proved that a synergy existed when activated carbon and trace elements were supplemented simultaneously. The degradation kinetics of propionate oxidation were particularly improved, reducing significantly the batch duration and improving the average methane productivities. Addition of activated carbon favored the growth of archaea and syntrophic bacteria, suggesting that interactions between these microorganisms were enhanced. Interestingly, microbial analyses showed that hydrogenotrophic methanogens were predominant. This study shows for the first time that addition of granular activated carbon and trace elements may be a feasible solution to stabilize food waste anaerobic digestion. Copyright © 2018 Elsevier Ltd. All rights reserved.

Chiral Gold Nanoclusters: Atomic Level Origins of Chirality.

PubMed

Zeng, Chenjie; Jin, Rongchao

2017-08-04

Chiral nanomaterials have received wide interest in many areas, but the exact origin of chirality at the atomic level remains elusive in many cases. With recent significant progress in atomically precise gold nanoclusters (e.g., thiolate-protected Au n (SR) m ), several origins of chirality have been unveiled based upon atomic structures determined by using single-crystal X-ray crystallography. The reported chiral Au n (SR) m structures explicitly reveal a predominant origin of chirality that arises from the Au-S chiral patterns at the metal-ligand interface, as opposed to the chiral arrangement of metal atoms in the inner core (i.e. kernel). In addition, chirality can also be introduced by a chiral ligand, manifested in the circular dichroism response from metal-based electronic transitions other than the ligand's own transition(s). Lastly, the chiral arrangement of carbon tails of the ligands has also been discovered in a very recent work on chiral Au 133 (SR) 52 and Au 246 (SR) 80 nanoclusters. Overall, the origins of chirality discovered in Au n (SR) m nanoclusters may provide models for the understanding of chirality origins in other types of nanomaterials and also constitute the basis for the development of various applications of chiral nanoparticles. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Mechanism of formation and spatial distribution of lead atoms in quartz tube atomizers

NASA Astrophysics Data System (ADS)

Johansson, M.; Baxter, D. C.; Ohlsson, K. E. A.; Frech, W.

1997-05-01

The cross-sectional and longitudinal spatial distributions of lead atoms in a quartz tube (QT) atomizers coupled to a gas chromatograph have been investigated. A uniform analyte atom distribution over the cross-section was found in a QT having an inner diameter (i.d.) of 7 mm, whereas a 10 mm i.d. QT showed an inhomogeneous distribution. These results accentuate the importance of using QTs with i.d.s below 10 mm to fulfil the prerequirement of the Beer—Lambert law to avoid bent calibration curves. The influence of the make up gas on the formation of lead atoms from alkyllead compounds has been studied, and carbon monoxide was found equally efficient in promoting free atom formation as hydrogen. This suggests that hydrogen radicals are not essential for mediating the atomization of alkyllead in QT atomizers at ˜ 1200 K. Furthermore, thermodynamic equilibrium calculations describing the investigated system were performed supporting the experimental results. Based on the presented data, a mechanism for free lead atom formation in continuously heated QT atomizers is proposed; thermal atomization occurs under thermodynamic equilibrium conditions in a reducing gas. The longitudinal atom distribution has been further investigated applying other make up gases, N 2 and He. These results show the effect of the influx of atmospheric oxygen on the free lead atom formation. Calculations of the partial pressure of oxygen in the atomizer gas phase assuming thermodynamic equilibrium have been undertaken using a convective-diffusional model.

Does the Use of Diamond-Like Carbon Coating and Organophosphate Lubricant Additive Together Cause Excessive Tribochemical Material Removal?

DOE PAGES

Zhou, Yan; Leonard, Donovan N.; Meyer, Harry M.; ...

2015-08-22

We observe unexpected wear increase on a steel surface that rubbed against diamond-like carbon (DLC) coatings only when lubricated by phosphate-based antiwear additives. Contrary to the literature hypothesis of a competition between zinc dialkyldithiophosphate produced tribofilms and DLC-induced carbon transfer, here a new wear mechanism based on carbon-catalyzed tribochemical interactions supported by surface characterization is proposed

Quantitative measurement of solvation shells using frequency modulated atomic force microscopy

NASA Astrophysics Data System (ADS)

Uchihashi, T.; Higgins, M.; Nakayama, Y.; Sader, J. E.; Jarvis, S. P.

2005-03-01

The nanoscale specificity of interaction measurements and additional imaging capability of the atomic force microscope make it an ideal technique for measuring solvation shells in a variety of liquids next to a range of materials. Unfortunately, the widespread use of atomic force microscopy for the measurement of solvation shells has been limited by uncertainties over the dimensions, composition and durability of the tip during the measurements, and problems associated with quantitative force calibration of the most sensitive dynamic measurement techniques. We address both these issues by the combined use of carbon nanotube high aspect ratio probes and quantifying the highly sensitive frequency modulation (FM) detection technique using a recently developed analytical method. Due to the excellent reproducibility of the measurement technique, additional information regarding solvation shell size as a function of proximity to the surface has been obtained for two very different liquids. Further, it has been possible to identify differences between chemical and geometrical effects in the chosen systems.

Ab initio calculations of ionic hydrocarbon compounds with heptacoordinate carbon.

PubMed

Wang, George; Rahman, A K Fazlur; Wang, Bin

2018-04-25

Ionic hydrocarbon compounds that contain hypercarbon atoms, which bond to five or more atoms, are important intermediates in chemical synthesis and may also find applications in hydrogen storage. Extensive investigations have identified hydrocarbon compounds that contain a five- or six-coordinated hypercarbon atom, such as the pentagonal-pyramidal hexamethylbenzene, C 6 (CH 3 ) 6 2+ , in which a hexacoordinate carbon atom is involved. It remains challenging to search for further higher-coordinated carbon in ionic hydrocarbon compounds, such as seven- and eight-coordinated carbon. Here, we report ab initio density functional calculations that show a stable 3D hexagonal-pyramidal configuration of tropylium trication, (C 7 H 7 ) 3+ , in which a heptacoordinate carbon atom is involved. We show that this tropylium trication is stable against deprotonation, dissociation, and structural deformation. In contrast, the pyramidal configurations of ionic C 8 H 8 compounds, which would contain an octacoordinate carbon atom, are unstable. These results provide insights for developing new molecular structures containing hypercarbon atoms, which may have potential applications in chemical synthesis and in hydrogen storage. Graphical abstract Possible structural transformations of stable configurations of (C 7 H 7 ) 3+ , which may result in the formation of the pyramidal structure that involves a heptacoordinate hypercarbon atom.

Atomic substitutions in synthetic apatite; Insights from solid-state NMR spectroscopy

NASA Astrophysics Data System (ADS)

Vaughn, John S.

Apatite, Ca5(PO4)3X (where X = F, Cl, or OH), is a unique mineral group capable of atomic substitutions for cations and anions of varied size and charge. Accommodation of differing substituents requires some kind of structural adaptation, e.g. new atomic positions, vacancies, or coupled substitutions. These structural adaptations often give rise to important physicochemical properties relevant to a range of scientific disciplines. Examples include volatile trapping during apatite crystallization, substitution for large radionuclides for long-term storage of nuclear fission waste, substitution for fluoride to improve acid resistivity in dental enamel composed dominantly of hydroxylapatite, and the development of novel biomaterials with enhanced biocompatibility. Despite the importance and ubiquity of atomic substitutions in apatite materials, many of the mechanisms by which these reactions occur are poorly understood. Presence of substituents at dilute concentration and occupancy of disordered atomic positions hinder detection by bulk characterization methods such as X-ray diffraction (XRD) and infrared (IR) spectroscopy. Solid-state nuclear magnetic resonance (NMR) spectroscopy is an isotope-specific structural characterization technique that does not require ordered atomic arrangements, and is therefore well suited to investigate atomic substitutions and structural adaptations in apatite. In the present work, solid-state NMR is utilized to investigate structural adaptations in three different types of apatite materials; a series of near-binary F, Cl apatite, carbonate-hydroxylapatite compositions prepared under various synthesis conditions, and a heat-treated hydroxylapatite enriched in 17O. The results indicate that hydroxyl groups in low-H, near binary F,Cl apatite facilitate solid-solution between F and Cl via column reversals, which result in average hexagonal symmetry despite very dilute OH concentration ( 2 mol percent). In addition, 19F NMR spectra indicate

Functionalization of Single-Wall Carbon Nanotubes by Photo-Oxidation

NASA Technical Reports Server (NTRS)

Lebron-Colon, Marisabel; Meador, Michael A.

2010-01-01

new technique for carbon nanotube oxidation was developed based upon the photo-oxidation of organic compounds. The resulting method is more benign than conventional oxidation approaches and produces single-wall carbon nanotubes (SWCNTs) with higher levels of oxidation. In this procedure, an oxygen saturated suspension of SWNTs in a suitable solvent containing a singlet oxygen sensitizer, such as Rose Bengal, is irradiated with ultraviolet light. The resulting oxidized tubes are recovered by filtering the suspension, followed by washing to remove any adsorbed solvent and sensitizer, and drying in a vacuum oven. Chemical analysis by FT-infrared and x-ray photoelectron spectroscopy revealed that the oxygen content of the photo-oxidized SWCNT was 11.3 atomic % compared to 6.7 atomic % for SWCNT that had been oxidized by standard treatment in refluxing acid. The photo-oxidized SWCNT produced by this method can be used directly in various polymer matrixes, or can be further modified by chemical reactions at the oxygen functional groups and then used as additives. This method may also be suitable for use in oxidation of multiwall carbon nanotubes and graphenes.

Background of SAM atom-fraction profiles

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

Ernst, Frank

Atom-fraction profiles acquired by SAM (scanning Auger microprobe) have important applications, e.g. in the context of alloy surface engineering by infusion of carbon or nitrogen through the alloy surface. However, such profiles often exhibit an artifact in form of a background with a level that anti-correlates with the local atom fraction. This article presents a theory explaining this phenomenon as a consequence of the way in which random noise in the spectrum propagates into the discretized differentiated spectrum that is used for quantification. The resulting model of “energy channel statistics” leads to a useful semi-quantitative background reduction procedure, which ismore » validated by applying it to simulated data. Subsequently, the procedure is applied to an example of experimental SAM data. The analysis leads to conclusions regarding optimum experimental acquisition conditions. The proposed method of background reduction is based on general principles and should be useful for a broad variety of applications. - Highlights: • Atom-fraction–depth profiles of carbon measured by scanning Auger microprobe • Strong background, varies with local carbon concentration. • Needs correction e.g. for quantitative comparison with simulations • Quantitative theory explains background. • Provides background removal strategy and practical advice for acquisition.« less

First principles study of hydrogen adsorption on carbon nanowires.

NASA Astrophysics Data System (ADS)

Tapia, Alejandro; Aguilera, Luis; Murrieta, Gabriel; de Coss, Romeo

2007-03-01

Recently has been reported a new type of one-dimensional carbon structures. Carbon nanowires formed by a linear carbon-atom chain inside an armchair (5,5) carbon nanotube has been observed using high-resolution transmission electron microscopy. In the present work we have studied the changes in the electronic structure of a carbon nanowires and (5,5) single-walled carbon nanotubes (SWCN) when a hydrogen atom is adsorbed. We used the Density Functional Theory and the calculations where performed by the pseudopotentials LCAO method (SIESTA code) and the Generalized Gradient Approximation (GGA) for the exchange-correlation potential. We have analyzed the changes in the atomic structure, density of states (LDOS), and the local orbital population. We found charge transfer from the nanotube to the linear chain and the hydrogen atom, the electronic character of the chain and nanotube sub-systems in chain@SWCN is the same that in the corresponding isolated systems, chain or SWCN. But the hydrogen adsorption produced changes in the atomic estructure and the electronic properties. This research was supported by PRIORI-UADY under Grant No. FING-05-004 and Consejo Nacional de Ciencia y Tecnolog'ia (Conacyt) under Grants No. 43830-F and 49985-J.

Direct evidence of atomic-scale structural fluctuations in catalyst nanoparticles.

PubMed

Lin, Pin Ann; Gomez-Ballesteros, Jose L; Burgos, Juan C; Balbuena, Perla B; Natarajan, Bharath; Sharma, Renu

2017-05-01

Rational catalyst design requires an atomic scale mechanistic understanding of the chemical pathways involved in the catalytic process. A heterogeneous catalyst typically works by adsorbing reactants onto its surface, where the energies for specific bonds to dissociate and/or combine with other species (to form desired intermediate or final products) are lower. Here, using the catalytic growth of single-walled carbon nanotubes (SWCNTs) as a prototype reaction, we show that the chemical pathway may in-fact involve the entire catalyst particle, and can proceed via the fluctuations in the formation and decomposition of metastable phases in the particle interior. We record in situ and at atomic resolution, the dynamic phase transformations occurring in a Cobalt catalyst nanoparticle during SWCNT growth, using a state-of-the-art environmental transmission electron microscope (ETEM). The fluctuations in catalyst carbon content are quantified by the automated, atomic-scale structural analysis of the time-resolved ETEM images and correlated with the SWCNT growth rate. We find the fluctuations in the carbon concentration in the catalyst nanoparticle and the fluctuations in nanotube growth rates to be of complementary character. These findings are successfully explained by reactive molecular dynamics (RMD) simulations that track the spatial and temporal evolution of the distribution of carbon atoms within and on the surface of the catalyst particle. We anticipate that our approach combining real-time, atomic-resolution image analysis and molecular dynamics simulations will facilitate catalyst design, improving reaction efficiencies and selectivity towards the growth of desired structure.

Glycerol as an additional carbon source for bacterial cellulose synthesis

NASA Astrophysics Data System (ADS)

Agustin, Y. E.; Padmawijaya, K. S.; Rixwari, H. F.; Yuniharto, V. A. S.

2018-03-01

Bacterial cellulose, the fermentation result of Acetobacter xylinus can be produced when glycerol was used as an additional carbon source. In this research, bacterial cellulose produced in two different fermentation medium, Hestrin and Scharmm (HS) medium and HS medium with additional MgSO4. Concentration of glycerol that used in this research were 0%; 5%; 10%; and 15% (v/v). The optimum conditions of bacterial cellulose production on each experiment variations determined by characterization of the mechanical properties, including thickness, tensile strength and elongation. Fourier Transform Infra Red Spectroscopy (FTIR) revealed the characterization of bacterial cellulose. Results showed that the growth rate of bacterial cellulose in HS-MgSO4-glycerol medium was faster than in HS-glycerol medium. Increasing concentrations of glycerol will lower the value of tensile strength and elongation. Elongation test showed that the elongation bacterial cellulose (BC) with the addition of 4.95% (v/v) glycerol in the HS-MgSO4 medium is the highest elongation value. The optimum bacterial cellulose production was achieved when 4.95% (v/v) of glycerol added into HS-MgSO4 medium with stress at break of 116.885 MPa and 4.214% elongation.

Carbon-coated ZnO mat passivation by atomic-layer-deposited HfO2 as an anode material for lithium-ion batteries.

PubMed

Jung, Mi-Hee

2017-11-01

ZnO has had little consideration as an anode material in lithium-ion batteries compared with other transition-metal oxides due to its inherent poor electrical conductivity and large volume expansion upon cycling and pulverization of ZnO-based electrodes. A logical design and facile synthesis of ZnO with well-controlled particle sizes and a specific morphology is essential to improving the performance of ZnO in lithium-ion batteries. In this paper, a simple approach is reported that uses a cation surfactant and a chelating agent to synthesize three-dimensional hierarchical nanostructured carbon-coated ZnO mats, in which the ZnO mats are composed of stacked individual ZnO nanowires and form well-defined nanoporous structures with high surface areas. In order to improve the performance of lithium-ion batteries, HfO 2 is deposited on the carbon-coated ZnO mat electrode via atomic layer deposition. Lithium-ion battery devices based on the carbon-coated ZnO mat passivation by atomic layer deposited HfO 2 exhibit an excellent initial discharge and charge capacities of 2684.01 and 963.21mAhg -1 , respectively, at a current density of 100mAg -1 in the voltage range of 0.01-3V. They also exhibit cycle stability after 125 cycles with a capacity of 740mAhg -1 and a remarkable rate capability. Copyright © 2017 Elsevier Inc. All rights reserved.

Evaluation of soil carbon pools after the addition of prunings in subtropical orchards placed in terraces

NASA Astrophysics Data System (ADS)

Márquez San Emeterio, Layla; Martín Reyes, Marino Pedro; Ortiz Bernad, Irene; Fernández Ondoño, Emilia; Sierra Aragón, Manuel

2017-04-01

The amount of carbon that can be stored in a soil depends on many factors, such as the type of soil, the chemical composition of plant rests and the climate, and is also highly affected by land use and soil management. Agricultural ecosystems are proved to absorb a large amount of CO2 from the atmosphere through several sustainable management practices. In addition, organic materials such as leaves, grass, prunings, etc., comprise a significant type of agricultural practices as a result of waste recycling. The aim of this research was to evaluate the effects of the addition of different organic prunings on the potential for carbon sequestration in agricultural soils placed in terraces. Three subtropical orchards were sampled in Almuñécar (Granada, S Spain): mango (Mangifera indica L.), avocado (Persea americana Mill.) and cherimoya (Annonacherimola Mill.). The predominant climate is Subtropical Mediterranean and the soil is an Eutric Anthrosol. The experimental design consisted in the application of prunings from avocado, cherimoya and mango trees, placed on the surface soil underneath their correspondent trees, as well as garden prunings from the green areas surrounding the town center on the surface soils under the three orchard trees. Control experiences without the addition of prunings were also evaluated. These experiences were followed for three years. Soil samples were taken at4 cm depth. They were dried for 3-4 days and then sieved (<2 mm).Total soil organic C, water-soluble soil organic C, mineral-associated organic C and non-oxidable C were analyzed and expressed as carbon pools (Mg C ha-1for total soil organic C, or Kg C ha-1for the others). The results showed an increase of all organic carbon pools in all pruning treatments compared to the control experiences. Differences in total organic carbon pool were statistically significant between soils under avocado prunings and their control soil, and between soils under garden prunings with cherimoya and

Pairwise additivity in the nuclear magnetic resonance interactions of atomic xenon.

PubMed

Hanni, Matti; Lantto, Perttu; Vaara, Juha

2009-04-14

Nuclear magnetic resonance (NMR) of atomic (129/131)Xe is used as a versatile probe of the structure and dynamics of various host materials, due to the sensitivity of the Xe NMR parameters to intermolecular interactions. The principles governing this sensitivity can be investigated using the prototypic system of interacting Xe atoms. In the pairwise additive approximation (PAA), the binary NMR chemical shift, nuclear quadrupole coupling (NQC), and spin-rotation (SR) curves for the xenon dimer are utilized for fast and efficient evaluation of the corresponding NMR tensors in small xenon clusters Xe(n) (n = 2-12). If accurate, the preparametrized PAA enables the analysis of the NMR properties of xenon clusters, condensed xenon phases, and xenon gas without having to resort to electronic structure calculations of instantaneous configurations for n > 2. The binary parameters for Xe(2) at different internuclear distances were obtained at the nonrelativistic Hartree-Fock level of theory. Quantum-chemical (QC) calculations at the corresponding level were used to obtain the NMR parameters of the Xe(n) (n = 2-12) clusters at the equilibrium geometries. Comparison of PAA and QC data indicates that the direct use of the binary property curves of Xe(2) can be expected to be well-suited for the analysis of Xe NMR in the gaseous phase dominated by binary collisions. For use in condensed phases where many-body effects should be considered, effective binary property functions were fitted using the principal components of QC tensors from Xe(n) clusters. Particularly, the chemical shift in Xe(n) is strikingly well-described by the effective PAA. The coordination number Z of the Xe site is found to be the most important factor determining the chemical shift, with the largest shifts being found for high-symmetry sites with the largest Z. This is rationalized in terms of the density of virtual electronic states available for response to magnetic perturbations.

High performance platinum single atom electrocatalyst for oxygen reduction reaction

PubMed Central

Liu, Jing; Jiao, Menggai; Lu, Lanlu; Barkholtz, Heather M.; Li, Yuping; Wang, Ying; Jiang, Luhua; Wu, Zhijian; Liu, Di-jia; Zhuang, Lin; Ma, Chao; Zeng, Jie; Zhang, Bingsen; Su, Dangsheng; Song, Ping; Xing, Wei; Xu, Weilin; Wang, Ying; Jiang, Zheng; Sun, Gongquan

2017-01-01

For the large-scale sustainable implementation of polymer electrolyte membrane fuel cells in vehicles, high-performance electrocatalysts with low platinum consumption are desirable for use as cathode material during the oxygen reduction reaction in fuel cells. Here we report a carbon black-supported cost-effective, efficient and durable platinum single-atom electrocatalyst with carbon monoxide/methanol tolerance for the cathodic oxygen reduction reaction. The acidic single-cell with such a catalyst as cathode delivers high performance, with power density up to 680 mW cm−2 at 80 °C with a low platinum loading of 0.09 mgPt cm−2, corresponding to a platinum utilization of 0.13 gPt kW−1 in the fuel cell. Good fuel cell durability is also observed. Theoretical calculations reveal that the main effective sites on such platinum single-atom electrocatalysts are single-pyridinic-nitrogen-atom-anchored single-platinum-atom centres, which are tolerant to carbon monoxide/methanol, but highly active for the oxygen reduction reaction. PMID:28737170

High performance platinum single atom electrocatalyst for oxygen reduction reaction

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

Liu, Jing; Jiao, Menggai; Lu, Lanlu

For the large-scale sustainable implementation of polymer electrolyte membrane fuel cells in vehicles, high-performance electrocatalysts with low platinum consumption are desirable for use as cathode material during the oxygen reduction reaction in fuel cells. Here we report a carbon black-supported cost-effective, efficient and durable platinum single-atom electrocatalyst with carbon monoxide/methanol tolerance for the cathodic oxygen reduction reaction. The acidic single-cell with such a catalyst as cathode delivers high performance, with power density up to 680 mW cm –2 at 80 °C with a low platinum loading of 0.09 mgPt cm –2, corresponding to a platinum utilization of 0.13 gPt kWmore » –1 in the fuel cell. Good fuel cell durability is also observed. As a result, theoretical calculations reveal that the main effective sites on such platinum single-atom electrocatalysts are single-pyridinic-nitrogen-atom-anchored single-platinum-atom centres, which are tolerant to carbon monoxide/methanol, but highly active for the oxygen reduction reaction.« less

High performance platinum single atom electrocatalyst for oxygen reduction reaction

DOE PAGES

Liu, Jing; Jiao, Menggai; Lu, Lanlu; ...

2017-07-24

For the large-scale sustainable implementation of polymer electrolyte membrane fuel cells in vehicles, high-performance electrocatalysts with low platinum consumption are desirable for use as cathode material during the oxygen reduction reaction in fuel cells. Here we report a carbon black-supported cost-effective, efficient and durable platinum single-atom electrocatalyst with carbon monoxide/methanol tolerance for the cathodic oxygen reduction reaction. The acidic single-cell with such a catalyst as cathode delivers high performance, with power density up to 680 mW cm –2 at 80 °C with a low platinum loading of 0.09 mgPt cm –2, corresponding to a platinum utilization of 0.13 gPt kWmore » –1 in the fuel cell. Good fuel cell durability is also observed. As a result, theoretical calculations reveal that the main effective sites on such platinum single-atom electrocatalysts are single-pyridinic-nitrogen-atom-anchored single-platinum-atom centres, which are tolerant to carbon monoxide/methanol, but highly active for the oxygen reduction reaction.« less

Quantitative atomic-scale structure characterization of ordered mesoporous carbon materials by solid state NMR

DOE PAGES

Wang, Zhuoran; Opembe, Naftali; Kobayashi, Takeshi; ...

2018-02-03

In this study, solid-state (SS)NMR techniques were applied to characterize the atomic-scale structures of ordered mesoporous carbon (OMC) materials prepared using Pluronic F127 as template with resorcinol and formaldehyde as polymerizing precursors. A rigorous quantitative analysis was developed using a combination of 13C SSNMR spectra acquired with direct polarization and cross polarization on natural abundant and selectively 13C-enriched series of samples pyrolyzed at various temperatures. These experiments identified and counted the key functional groups present in the OMCs at various stages of preparation and thermal treatment. Lastly, the chemical evolution of molecular networks, the average sizes of aromatic clusters andmore » the extended molecular structures of OMCs were then inferred by coupling this information with the elemental analysis results.« less

Quantitative atomic-scale structure characterization of ordered mesoporous carbon materials by solid state NMR

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

Wang, Zhuoran; Opembe, Naftali; Kobayashi, Takeshi

In this study, solid-state (SS)NMR techniques were applied to characterize the atomic-scale structures of ordered mesoporous carbon (OMC) materials prepared using Pluronic F127 as template with resorcinol and formaldehyde as polymerizing precursors. A rigorous quantitative analysis was developed using a combination of 13C SSNMR spectra acquired with direct polarization and cross polarization on natural abundant and selectively 13C-enriched series of samples pyrolyzed at various temperatures. These experiments identified and counted the key functional groups present in the OMCs at various stages of preparation and thermal treatment. Lastly, the chemical evolution of molecular networks, the average sizes of aromatic clusters andmore » the extended molecular structures of OMCs were then inferred by coupling this information with the elemental analysis results.« less

An in situ generated carbon as integrated conductive additive for hierarchical negative plate of lead-acid battery

NASA Astrophysics Data System (ADS)

Saravanan, M.; Ganesan, M.; Ambalavanan, S.

2014-04-01

In this work, we report an in situ generated carbon from sugar as additive in the Negative Active Mass (NAM) which enhances the charge-discharge characteristics of the lead-acid cells. In situ formed sugar derived carbon (SDC) with leady oxide (LO) provides a conductive network and excellent protection against NAM irreversible lead sulfation. The effect of SDC and carbon black (CB) added negative plates are characterized by X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM), galvanostatic charge-discharge, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS), respectively. The results show that subtle changes in the addition of carbon to NAM led to subsequent changes on the performance during partial-state-of-charge (PSoC) operations in lead-acid cells. Furthermore, SDC added cells exhibit remarkable improvement in the rate capability, active material utilization, cycle performance and charge acceptance compared to that of the conventional CB added cells. The impact of SDC with LO at various synthesis conditions on the electrochemical performance of the negative plate is studied systematically.

Density functional theory study the effects of oxygen-containing functional groups on oxygen molecules and oxygen atoms adsorbed on carbonaceous materials.

PubMed

Qi, Xuejun; Song, Wenwu; Shi, Jianwei

2017-01-01

Density functional theory was used to study the effects of different types of oxygen-containing functional groups on the adsorption of oxygen molecules and single active oxygen atoms on carbonaceous materials. During gasification or combustion reactions of carbonaceous materials, oxygen-containing functional groups such as hydroxyl(-OH), carbonyl(-CO), quinone(-O), and carboxyl(-COOH) are often present on the edge of graphite and can affect graphite's chemical properties. When oxygen-containing functional groups appear on a graphite surface, the oxygen molecules are strongly adsorbed onto the surface to form a four-member ring structure. At the same time, the O-O bond is greatly weakened and easily broken. The adsorption energy value indicates that the adsorption of oxygen molecules changes from physisorption to chemisorption for oxygen-containing functional groups on the edge of a graphite surface. In addition, our results indicate that the adsorption energy depends on the type of oxygen-containing functional group. When a single active oxygen atom is adsorbed on the bridge site of graphite, it gives rise to a stable epoxy structure. Epoxy can cause deformation of the graphite lattice due to the transition of graphite from sp2 to sp3 after the addition of an oxygen atom. For quinone group on the edge of graphite, oxygen atoms react with carbon atoms to form the precursor of CO2. Similarly, the single active oxygen atoms of carbonyl groups can interact with edge carbon atoms to form the precursor of CO2. The results show that oxygen-containing functional groups on graphite surfaces enhance the activity of graphite, which promotes adsorption on the graphite surface.

Density functional theory study the effects of oxygen-containing functional groups on oxygen molecules and oxygen atoms adsorbed on carbonaceous materials

PubMed Central

Song, Wenwu; Shi, Jianwei

2017-01-01

Density functional theory was used to study the effects of different types of oxygen-containing functional groups on the adsorption of oxygen molecules and single active oxygen atoms on carbonaceous materials. During gasification or combustion reactions of carbonaceous materials, oxygen-containing functional groups such as hydroxyl(-OH), carbonyl(-CO), quinone(-O), and carboxyl(-COOH) are often present on the edge of graphite and can affect graphite’s chemical properties. When oxygen-containing functional groups appear on a graphite surface, the oxygen molecules are strongly adsorbed onto the surface to form a four-member ring structure. At the same time, the O-O bond is greatly weakened and easily broken. The adsorption energy value indicates that the adsorption of oxygen molecules changes from physisorption to chemisorption for oxygen-containing functional groups on the edge of a graphite surface. In addition, our results indicate that the adsorption energy depends on the type of oxygen-containing functional group. When a single active oxygen atom is adsorbed on the bridge site of graphite, it gives rise to a stable epoxy structure. Epoxy can cause deformation of the graphite lattice due to the transition of graphite from sp2 to sp3 after the addition of an oxygen atom. For quinone group on the edge of graphite, oxygen atoms react with carbon atoms to form the precursor of CO2. Similarly, the single active oxygen atoms of carbonyl groups can interact with edge carbon atoms to form the precursor of CO2. The results show that oxygen-containing functional groups on graphite surfaces enhance the activity of graphite, which promotes adsorption on the graphite surface. PMID:28301544

Carbon nanotube modified probes for stable and high sensitivity conductive atomic force microscopy

NASA Astrophysics Data System (ADS)

Slattery, Ashley D.; Shearer, Cameron J.; Gibson, Christopher T.; Shapter, Joseph G.; Lewis, David A.; Stapleton, Andrew J.

2016-11-01

Conductive atomic force microscopy (C-AFM) is used to characterise the nanoscale electrical properties of many conducting and semiconducting materials. We investigate the effect of single walled carbon nanotube (SWCNT) modification of commercial Pt/Ir cantilevers on the sensitivity and image stability during C-AFM imaging. Pt/Ir cantilevers were modified with small bundles of SWCNTs via a manual attachment procedure and secured with a conductive platinum pad. AFM images of topography and current were collected from heterogeneous polymer and nanomaterial samples using both standard and SWCNT modified cantilevers. Typically, achieving a good current image comes at the cost of reduced feedback stability. In part, this is due to electrostatic interaction and increased tip wear upon applying a bias between the tip and the sample. The SWCNT modified tips displayed superior current sensitivity and feedback stability which, combined with superior wear resistance of SWCNTs, is a significant advancement for C-AFM.

Sulfate reduction in sulfuric material after re-flooding: Effectiveness of organic carbon addition and pH increase depends on soil properties.

PubMed

Yuan, Chaolei; Fitzpatrick, Rob; Mosley, Luke M; Marschner, Petra

2015-11-15

Sulfuric material is formed upon oxidation of sulfidic material; it is extremely acidic, and therefore, an environmental hazard. One option for increasing pH of sulfuric material may be stimulation of bacterial sulfate reduction. We investigated the effects of organic carbon addition and pH increase on sulfate reduction after re-flooding in ten sulfuric materials with four treatments: control, pH increase to 5.5 (+pH), organic carbon addition with 2% w/w finely ground wheat straw (+C), and organic carbon addition and pH increase (+C+pH). After 36 weeks, in five of the ten soils, only treatment +C+pH significantly increased the concentration of reduced inorganic sulfur (RIS) compared to the control and increased the soil pore water pH compared to treatment+pH. In four other soils, pH increase or/and organic carbon addition had no significant effect on RIS concentration compared to the control. The RIS concentration in treatment +C+pH as percentage of the control was negatively correlated with soil clay content and initial nitrate concentration. The results suggest that organic carbon addition and pH increase can stimulate sulfate reduction after re-flooding, but the effectiveness of this treatment depends on soil properties. Copyright © 2015 Elsevier B.V. All rights reserved.

First-Principles Study of Migration Mechanisms and Diffusion of Carbon in GaN (Open Access Publisher’s Version)

DTIC Science & Technology

2015-09-21

and metal organic chemical vapor deposition (MOCVD) [18]. In the former case, carbon can contaminate the material during air exposure in standard... gallium . In addition, carbon can be found as a contaminant in the source gases or it can be etched off the susceptor that transfers heat to the substrate...split interstitial Figure 1: Split interstitials of carbon (yellow) and nitrogen (blue) surrounded by four gallium atoms (red). energy differences of

Nanoscale soldering of axially positioned single-walled carbon nanotubes: a molecular dynamics simulation study.

PubMed

Cui, Jianlei; Yang, Lijun; Zhou, Liang; Wang, Yang

2014-02-12

The miniaturization of electronics devices into the nanometer scale is indispensable for next-generation semi-conductor technology. Carbon nanotubes (CNTs) are considered to be the promising candidates for future interconnection wires. To study the carbon nanotubes interconnection during nanosoldering, the melting process of nanosolder and nanosoldering process between single-walled carbon nanotubes are simulated with molecular dynamics method. As the simulation results, the melting point of 2 nm silver solder is about 605 K because of high surface energy, which is below the melting temperature of Ag bulk material. In the nanosoldering process simulations, Ag atoms may be dragged into the nanotubes to form different connection configuration, which has no apparent relationship with chirality of SWNTs. The length of core filling nanowires structure has the relationship with the diameter, and it does not become longer with the increasing diameter of SWNT. Subsequently, the dominant mechanism of was analyzed. In addition, as the heating temperature and time, respectively, increases, more Ag atoms can enter the SWNTs with longer length of Ag nanowires. And because of the strong metal bonds, less Ag atoms can remain with the tight atomic structures in the gap between SWNT and SWNT. The preferred interconnection configurations can be achieved between SWNT and SWNT in this paper.

Self-assembly of endohedral metallofullerenes: a decisive role of cooling gas and metal-carbon bonding

NASA Astrophysics Data System (ADS)

Deng, Qingming; Heine, Thomas; Irle, Stephan; Popov, Alexey A.

2016-02-01

.e. leading to Sc-EMFs) with more realistic cage-size distribution than simulations of the Sc/C system. The main Sc encapsulation mechanism involves nucleation of several hexagons and pentagons with Sc atoms already at the early stages of carbon vapor condensation. In such proto-cages, both Sc-C σ-bonds and coordination bonds between Sc atoms and the π-system of the carbon network are present. Sc atoms are thus rather labile and can move along the carbon network, but the overall bonding is sufficiently strong to prevent dissociation even at temperatures around 2000 kelvin. Further growth of the fullerene cage results in the encapsulation of one or two Sc atoms within the fullerene. In agreement with experimental studies, an extension of the simulations to Fe and Ti as the metal component showed that Fe-EMFs are not formed at all, whereas Ti is prone to form Ti-EMFs with small cage sizes, including Ti@C28-Td and Ti@C30-C2v(3). Electronic supplementary information (ESI) available: Additional information on metal-carbon bonding and MD simulations. See DOI: 10.1039/c5nr08645k

Determination of nickel in water, food, and biological samples by electrothermal atomic absorption spectrometry after preconcentration on modified carbon nanotubes.

PubMed

Taher, Mohammad Ali; Mazaheri, Lida; Ashkenani, Hamid; Mohadesi, Alireza; Afzali, Daryoush

2014-01-01

A new and sensitive SPE method using modified carbon nanotubes for extraction and preconcentration, and electrothermal atomic absorption spectrometric determination of nickel (Ni) in real samples at ng/L levels was investigated. First, multiwalled carbon nanotubes were oxidized with concentrated HNO3, then modified with 2-(5-bormo-2-pyridylazo)-5-diethylaminophenol reagent. The adsorption was achieved quantitatively on a modified carbon nanotubes column in a pH range of 6.5 to 8.5; the adsorbed Ni(II) ions were then desorbed by passing 5.0 mL of 1 M HNO3. The effects of analytical parameters, including pH of the solution, eluent type and volume, sample volume, flow rate of the eluent, and matrix ions, were investigated for optimization of the presented procedure. The enrichment factor was 180, and the LOD for Ni was 4.9 ng/L. The method was applied to the determination of Ni in water, food, and biological samples, and reproducible results were obtained.

Initial mechanisms for the dissociation of carbon from electronically-excited nitrotoluene molecules

NASA Astrophysics Data System (ADS)

Yuan, Bing; Eilers, Hergen

2017-12-01

We calculated the photoinduced decomposition of various nitrotoluene molecules, resulting in the formation of atomic carbon, at the B3LYP/6-311++G(d,p) level of theory using Gaussian 09. In addition, we used TD-DFT (B3LYP/6-311++G(d,p)) to calculate the excitation energies. The results confirm our previously reported experimental results. Specifically, we show that the absorption of 226 nm (5.49 eV) light can lead to the decomposition of nitrotoluene molecules and the formation of atomic carbon. One 226 nm photon is sufficient for the dissociation of carbon from 2-NT and 4-NT molecules. During the dissociation process, the CH3 group provides the dissociated carbon atom and the NO2 group accepts the H atoms from either the CH3 group or the benzene ring before carbon exits the molecular system. For the second and third carbon dissociation of 2-NT, the energy barriers are 6.70 eV and 7.43 eV, respectively, and two 226 nm photons would need to be absorbed by the molecule. If extra NO is present during the first carbon dissociation of 2-NT, it gets involved in the last two decomposition steps and forms a C=NH-N=O structure which stabilizes the decomposition products and lowers the energy barrier from 5.22 eV to 4.70 eV. However, for the second and third carbon dissociation of 2-NT, the NO molecules have no apparent effect. For nitrotoluene molecules with two or three NO2 groups (i.e., 2,4-DNT, 2,6-DNT, 3,4-DNT, and 2,4,6-TNT), the first carbon dissociation energies are between 5.26 eV and 5.57 eV. The carbon dissociation pathways for these molecules are similar to those of 2-NT. In 2,4-DNT, the lowest energy barriers for the second and third carbon dissociation are 6.54 eV and 6.60 eV, respectively, which are about 1 eV higher than the energy barrier for the first carbon dissociation. In case of 2,4-DNT/NO and 2,4,6-TNT/NO, NO acts as a catalyst in the first carbon dissociation processes and forms a C=NH-N=O structure which lowers the energy barriers by 0.48 eV and 0

Quantifying the Hierarchical Order in Self-Aligned Carbon Nanotubes from Atomic to Micrometer Scale.

PubMed

Meshot, Eric R; Zwissler, Darwin W; Bui, Ngoc; Kuykendall, Tevye R; Wang, Cheng; Hexemer, Alexander; Wu, Kuang Jen J; Fornasiero, Francesco

2017-06-27

Fundamental understanding of structure-property relationships in hierarchically organized nanostructures is crucial for the development of new functionality, yet quantifying structure across multiple length scales is challenging. In this work, we used nondestructive X-ray scattering to quantitatively map the multiscale structure of hierarchically self-organized carbon nanotube (CNT) "forests" across 4 orders of magnitude in length scale, from 2.0 Å to 1.5 μm. Fully resolved structural features include the graphitic honeycomb lattice and interlayer walls (atomic), CNT diameter (nano), as well as the greater CNT ensemble (meso) and large corrugations (micro). Correlating orientational order across hierarchical levels revealed a cascading decrease as we probed finer structural feature sizes with enhanced sensitivity to small-scale disorder. Furthermore, we established qualitative relationships for single-, few-, and multiwall CNT forest characteristics, showing that multiscale orientational order is directly correlated with number density spanning 10 9 -10 12 cm -2 , yet order is inversely proportional to CNT diameter, number of walls, and atomic defects. Lastly, we captured and quantified ultralow-q meridional scattering features and built a phenomenological model of the large-scale CNT forest morphology, which predicted and confirmed that these features arise due to microscale corrugations along the vertical forest direction. Providing detailed structural information at multiple length scales is important for design and synthesis of CNT materials as well as other hierarchically organized nanostructures.

High temperature hydrogen sulfide adsorption on activated carbon - I. Effects of gas composition and metal addition

USGS Publications Warehouse

Cal, M.P.; Strickler, B.W.; Lizzio, A.A.

2000-01-01

Various types of activated carbon sorbents were evaluated for their ability to remove H2S from a simulated coal gas stream at a temperature of 550 ??C. The ability of activated carbon to remove H2S at elevated temperature was examined as a function of carbon surface chemistry (oxidation, thermal desorption, and metal addition), and gas composition. A sorbent prepared by steam activation, HNO3 oxidation and impregnated with Zn, and tested in a gas stream containing 0.5% H2S, 50% CO2 and 49.5% N2, had the greatest H2S adsorption capacity. Addition of H2, CO, and H2O to the inlet gas stream reduced H2S breakthrough time and H2S adsorption capacity. A Zn impregnated activated carbon, when tested using a simulated coal gas containing 0.5% H2S, 49.5% N2, 13% H2, 8.5% H2O, 21% CO, and 7.5% CO2, had a breakthrough time of 75 min, which was less than 25 percent of the length of breakthrough for screening experiments performed with a simplified gas mixture of 0.5% H2S, 50% CO2, and 49.5% N2.

Re-use of drinking water treatment plant (DWTP) sludge: Characterization and technological behaviour of cement mortars with atomized sludge additions

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

Husillos Rodriguez, N., E-mail: nuriah@ietcc.csic.e; Martinez Ramirez, S.; Blanco Varela, M.T.

This paper aims to characterize spray-dried DWTP sludge and evaluate its possible use as an addition for the cement industry. It describes the physical, chemical and micro-structural characterization of the sludge as well as the effect of its addition to Portland cements on the hydration, water demand, setting and mechanical strength of standardized mortars. Spray drying DWTP sludge generates a readily handled powdery material whose particle size is similar to those of Portland cement. The atomized sludge contains 12-14% organic matter (mainly fatty acids), while its main mineral constituents are muscovite, quartz, calcite, dolomite and seraphinite (or clinoclor). Its amorphousmore » material content is 35%. The mortars were made with type CEM I Portland cement mixed with 10 to 30% atomized sludge exhibited lower mechanical strength than the control cement and a decline in slump. Setting was also altered in the blended cements with respect to the control.« less

Catalytic Enantioselective Synthesis of Quaternary Carbon Stereocenters

PubMed Central

Quasdorf, Kyle W.; Overman, Larry E.

2015-01-01

Preface Quaternary carbon stereocenters–carbon atoms to which four distinct carbon substituents are attached–are common features of molecules found in nature. However, prior to recent advances in chemical catalysis, there were few methods available for constructing single stereoisomers of this important structural motif. Here we discuss the many catalytic enantioselective reactions developed during the past decade for synthesizing organic molecules containing such carbon atoms. This progress now makes it possible to selectively incorporate quaternary stereocenters in many high-value organic molecules for use in medicine, agriculture, and other areas. PMID:25503231

Enhanced performance of starter lighting ignition type lead-acid batteries with carbon nanotubes as an additive to the active mass

NASA Astrophysics Data System (ADS)

Marom, Rotem; Ziv, Baruch; Banerjee, Anjan; Cahana, Beni; Luski, Shalom; Aurbach, Doron

2015-11-01

Addition of various carbon materials into lead-acid battery electrodes was studied and examined in order to enhance the power density, improve cycle life and stability of both negative and positive electrodes in lead acid batteries. High electrical-conductivity, high-aspect ratio, good mechanical properties and chemical stability of multi-wall carbon nanotubes (MWCNT, unmodified and mofified with carboxylic groups) position them as viable additives to enhance the electrodes' electrical conductivity, to mitigate the well-known sulfation failure mechanism and improve the physical integration of the electrodes. In this study, we investigated the incorporation-effect of carbon nanotubes (CNT) to the positive and the negative active materials in lead-acid battery prototypes in a configuration of flooded cells, as well as gelled cells. The cells were tested at 25% and 30% depth-of-discharge (DOD). The positive effect of the carbon nanotubes (CNT) utilization as additives to both positive and negative electrodes of lead-acid batteries was clearly demonstrated and is explained herein based on microscopic studies.

Soil respiration characteristics in different land uses and response of soil organic carbon to biochar addition in high-latitude agricultural area.

PubMed

Ouyang, Wei; Geng, Xiaojun; Huang, Wejia; Hao, Fanghua; Zhao, Jinbo

2016-02-01

The farmland tillage practices changed the soil chemical properties, which also impacted the soil respiration (R s ) process and the soil carbon conservation. Originally, the farmland in northeast China had high soil carbon content, which was decreased in the recent decades due to the tillage practices. To better understand the R s dynamics in different land use types and its relationship with soil carbon loss, soil samples at two layers (0-15 and 15-30 cm) were analyzed for organic carbon (OC), total nitrogen (TN), total phosphorus (TP), total carbon (TC), available nitrogen (AN), available phosphorus (AP), soil particle size distribution, as well as the R s rate. The R s rate of the paddy land was 0.22 (at 0-15 cm) and 3.01 (at 15-30 cm) times of the upland. The average concentrations of OC and clay content in cultivated areas were much lower than in non-cultivated areas. The partial least squares analysis suggested that the TC and TN were significantly related to the R s process in cultivated soils. The upland soil was further used to test soil CO2 emission response at different biochar addition levels during 70-days incubation. The measurement in the limited incubation period demonstrated that the addition of biochar improved the soil C content because it had high concentration of pyrogenic C, which was resistant to mineralization. The analysis showed that biochar addition can promote soil OC by mitigating carbon dioxide (CO2) emission. The biochar addition achieved the best performance for the soil carbon conservation in high-latitude agricultural area due to the originally high carbon content.

First row transition metal atoms embedded in multivacancies in a rippled graphene system

NASA Astrophysics Data System (ADS)

Mombrú, Dominique; Faccio, Ricardo; Mombrú, Alvaro W.

2018-03-01

Ab-initio calculations based on density functional theory (DFT) have been performed to study systems where a first row transition metal atom is embedded in a rippled graphene due to the existence of an 8-order multivacancy. In addition to these cases, also the inclusion of a zinc atom, with a 3d10 electron configuration, was also studied. Structural distortions and magnetic response for each system were studied. A correlation was found for the magnitude of the rippling and the distortion in the vacancy. Variation in the trends was found for Cu and Zn cases, which were explained on the basis of the filling of the 3dx2-y2 orbital. All the systems exhibit lower magnetic moment in comparison to the metal-less system. The quenching of the magnetic moment due to the carbon atoms in the vacancy is observed for Sc and Cu.

Imaging powders with the atomic force microscope: from biominerals to commercial materials.

PubMed

Friedbacher, G; Hansma, P K; Ramli, E; Stucky, G D

1991-09-13

Atomically resolved images of pressed powder samples have been obtained with the atomic force microscope (AFM). The technique was successful in resolving the particle, domain, and atomic structure of pismo clam (Tivela stultorum) and sea urchin (Strongylocentrotus purpuratus) shells and of commercially available calcium carbonate (CaCO(3)) and strontium carbonate (SrCO(3)) powders. Grinding and subsequent pressing of the shells did not destroy the microstructure of these materials. The atomic-resolution imaging capabilities of AFM can be applied to polycrystalline samples by means of pressing powders with a grain size as small as 50 micrometers. These results illustrate that the AFM is a promising tool for material science and the study of biomineralization.

Effects of dilute substitutional solutes on interstitial carbon in α-Fe: Interactions and associated carbon diffusion from first-principles calculations

NASA Astrophysics Data System (ADS)

Liu, Peitao; Xing, Weiwei; Cheng, Xiyue; Li, Dianzhong; Li, Yiyi; Chen, Xing-Qiu

2014-07-01

By means of first-principles calculations coupled with the kinetic Monte Carlo simulations, we have systematically investigated the effects of dilute substitutional solutes on the behaviors of carbon in α-Fe. Our results uncover the following. (i) Without the Fe vacancy the interactions between most solutes and carbon are repulsive due to the strain relief, whereas Mn has a weak attractive interaction with its nearest-neighbor carbon due to the local ferromagnetic coupling effect. (ii) The presence of the Fe vacancy results in attractive interactions of all the solutes with carbon. In particular, the Mn-vacancy pair shows an exceptionally large binding energy of -0.81 eV with carbon. (iii) The alloying addition significantly impacts the atomic-scale concentration distributions and chemical potential of carbon in the Fe matrix. Among them, Mn and Cr increase the carbon chemical potential, whereas Al and Si reduce it. (iv) Within the dilute scale of the alloying solution, the solute concentration- and temperature-dependent carbon diffusivities demonstrate that Mn has a little impact on the carbon diffusion, whereas Cr (Al or Si) remarkably retards the carbon diffusion. Our results provide a certain implication for better understanding the experimental observations related with the carbon solubility limit, carbon microsegregation, and carbide precipitations in the ferritic steels.

Selective Laser Sintering of Porous Silica Enabled by Carbon Additive

PubMed Central

Chang, Shuai; Li, Liqun; Lu, Li

2017-01-01

The aim of this study is to investigate the possibility of a freeform fabrication of porous ceramic parts through selective laser sintering (SLS). SLS was proposed to manufacture ceramic green parts because this additive manufacturing technique can be used to fabricate three-dimensional objects directly without a mold, and the technique has the capability of generating porous ceramics with controlled porosity. However, ceramic printing has not yet fully achieved its 3D fabrication capabilities without using polymer binder. Except for the limitations of high melting point, brittleness, and low thermal shock resistance from ceramic material properties, the key obstacle lies in the very poor absorptivity of oxide ceramics to fiber laser, which is widely installed in commercial SLS equipment. An alternative solution to overcome the poor laser absorptivity via improving material compositions is presented in this study. The positive effect of carbon additive on the absorptivity of silica powder to fiber laser is discussed. To investigate the capabilities of the SLS process, 3D porous silica structures were successfully prepared and characterized. PMID:29144425

Selective Laser Sintering of Porous Silica Enabled by Carbon Additive.

PubMed

Chang, Shuai; Li, Liqun; Lu, Li; Fuh, Jerry Ying Hsi

2017-11-16

The aim of this study is to investigate the possibility of a freeform fabrication of porous ceramic parts through selective laser sintering (SLS). SLS was proposed to manufacture ceramic green parts because this additive manufacturing technique can be used to fabricate three-dimensional objects directly without a mold, and the technique has the capability of generating porous ceramics with controlled porosity. However, ceramic printing has not yet fully achieved its 3D fabrication capabilities without using polymer binder. Except for the limitations of high melting point, brittleness, and low thermal shock resistance from ceramic material properties, the key obstacle lies in the very poor absorptivity of oxide ceramics to fiber laser, which is widely installed in commercial SLS equipment. An alternative solution to overcome the poor laser absorptivity via improving material compositions is presented in this study. The positive effect of carbon additive on the absorptivity of silica powder to fiber laser is discussed. To investigate the capabilities of the SLS process, 3D porous silica structures were successfully prepared and characterized.

Synergic effect of atomic oxygen and outgassing phenomena on Carbon/SiC composites for space applications

NASA Astrophysics Data System (ADS)

Albano, Marta

The space environment is one of the most critical for space structures. The low earth orbit (LEO) space environment includes hazards such as atomic oxygen, UV radiation, ionizing radiation (electrons, protons), high vacuum, plasma, micrometeoroids and debris, as well as severe temperature cycles. Exposure of composites to the space environment may result in different detrimental effects via modification of their chemical, electrical, thermal, optical and mechanical properties as well as surface erosion. The high vacuum induces material outgassing (e.g. low-molecular weight residues, plasticizers and additives) and consequent contamination of nearby surfaces. At LEO altitudes the neutral atmosphere consists primarily of ATOX (˜80%) and nitrogen molecules (˜20%). ATOX, which is formed by photo-dissociation of molecular oxygen in the upper atmosphere, is a severe hazard for composites. The number density of ATOX at about 300 km altitude is ˜2 × 109 to 8 × 109 atoms/cm3, for minimum and maximum solar activity, respectively. Front surfaces (ram direction) of space vehicles orbiting at a velocity of about 8 km/s collide with the ATOX species with impingement kinetic energy of approximately 5 eV. The ATOX flux is determined by such parameters as altitude, orbital inclination, solar activity and time of day. A nominal range of values for LEO is 1014-1015 atoms/cm2 s. The Low Earth Orbit is a complex and dynamic environment where constituents vary with position, local time, season and solar activity. Effects of different constituents of the space environment on spacecraft materials play an important role in determining the system function, reliability and lifetime. This is more crucial if the structure has to be used for the re-entry as thermal protection systems for example. In this case the integrity of the surface and its coating is crucial for the success of the entire mission. During the re-entry, resistance of materials is hard tested by fast chemical reactions

Atomic-absorption determination of mercury in geological materials by flame and carbon-rod atomisation after solvent extraction and using co-extracted silver as a matrix modifier

USGS Publications Warehouse

Sanzolone, R.F.; Chao, T.T.

1983-01-01

Based on modifications and expansion of the original Tindall's solvent extraction flame atomic-absorption procedure, an atomic-absorption spectrophotometric method has been developed for the determination of mercury in geological materials. The sample is digested with nitric and hydrochloric acids in a boiling water-bath. The solution is made ammoniacal and potassium iodide and silver nitrate are added. The mercury is extracted into isobutyl methyl ketone as the tetraiodomercurate(ll). Added silver is co-extracted with mercury and serves as a matrix modifier in the carbon-rod atomiser. The mercury in the isobutyl methyl ketone extract may be determined by either the flame- or the carbon-rod atomisation method, depending on the concentration level. The limits of determination are 0.05-10 p.p.m. of mercury for the carbon-rod atomisation and 1 -200 p.p.m. of mercury for the flame atomisation. Mercury values for reference samples obtained by replicate analyses are in good agreement with those reported by other workers, with relative standard deviations ranging from 2.3 to 0.9%. Recoveries of mercury spiked at two levels were 93-106%. Major and trace elements commonly found in geological materials do not interfere.

Effects of experimental fuel additions on fire intensity and severity: unexpected carbon resilience of a neotropical forest.

PubMed

Brando, Paulo M; Oliveria-Santos, Claudinei; Rocha, Wanderley; Cury, Roberta; Coe, Michael T

2016-07-01

Global changes and associated droughts, heat waves, logging activities, and forest fragmentation may intensify fires in Amazonia by altering forest microclimate and fuel dynamics. To isolate the effects of fuel loads on fire behavior and fire-induced changes in forest carbon cycling, we manipulated fine fuel loads in a fire experiment located in southeast Amazonia. We predicted that a 50% increase in fine fuel loads would disproportionally increase fire intensity and severity (i.e., tree mortality and losses in carbon stocks) due to multiplicative effects of fine fuel loads on the rate of fire spread, fuel consumption, and burned area. The experiment followed a fully replicated randomized block design (N = 6) comprised of unburned control plots and burned plots that were treated with and without fine fuel additions. The fuel addition treatment significantly increased burned area (+22%) and consequently canopy openness (+10%), fine fuel combustion (+5%), and mortality of individuals ≥5 cm in diameter at breast height (dbh; +37%). Surprisingly, we observed nonsignificant effects of the fuel addition treatment on fireline intensity, and no significant differences among the three treatments for (i) mortality of large trees (≥30 cm dbh), (ii) aboveground forest carbon stocks, and (iii) soil respiration. It was also surprising that postfire tree growth and wood increment were higher in the burned plots treated with fuels than in the unburned control. These results suggest that (i) fine fuel load accumulation increases the likelihood of larger understory fires and (ii) single, low-intensity fires weakly influence carbon cycling of this primary neotropical forest, although delayed postfire mortality of large trees may lower carbon stocks over the long term. Overall, our findings indicate that increased fine fuel loads alone are unlikely to create threshold conditions for high-intensity, catastrophic fires during nondrought years. © 2016 John Wiley & Sons Ltd.

Combustor exhaust-emissions and blowout-limits with diesel number 2 and Jet A fuels utilizing air-atomizing and pressure-atomizing nozzles

NASA Technical Reports Server (NTRS)

Ingebo, R. D.; Norgren, C. T.

1975-01-01

The effect of fuel properties on exhaust emissions and blowout limits of a high-pressure combustor segment is evaluated using a splash-groove air-atomizing fuel injector and a pressure-atomizing simplex fuel nozzle to burn both diesel number 2 and Jet A fuels. Exhaust emissions and blowout data are obtained and compared on the basis of the aromatic content and volatility of the two fuels. Exhaust smoke number and emission indices for oxides of nitrogen, carbon monoxide, and unburned hydrocarbons are determined for comparison. As compared to the pressure-atomizing nozzle, the air-atomizing nozzle is found to reduce nitrogen oxides by 20%, smoke number by 30%, carbon monoxide by 70%, and unburned hydrocarbons by 50% when used with diesel number 2 fuel. The higher concentration of aromatics and lower volatility of diesel number 2 fuel as compared to Jet A fuel appears to have the most detrimental effect on exhaust emissions. Smoke number and unburned hydrocarbons are twice as high with diesel number 2 as with Jet A fuel.

H ATOM IRRADIATION OF CARBON GRAINS UNDER SIMULATED DENSE INTERSTELLAR MEDIUM CONDITIONS: THE EVOLUTION OF ORGANICS FROM DIFFUSE INTERSTELLAR CLOUDS TO THE SOLAR SYSTEM

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

Mennella, Vito, E-mail: mennella@na.astro.i

2010-08-01

We present the results of experiments aimed at studying the interaction of hydrogen atoms at 80 K with carbon grains covered with a water ice layer at 12 K. The effects of H processing have been analyzed, using IR spectroscopy, as a function of the water ice layer. The results confirm that exposure of the samples to H atoms induces the activation of the band at 3.47 {mu}m with no evidence for the formation of aromatic and aliphatic C-H bonds in the CH{sub 2} and CH{sub 3} functional groups. The formation cross section of the 3.47 {mu}m band has beenmore » estimated from the increase of its integrated optical depth as a function of the H atom fluence. The cross section decreases with increasing thickness of the water ice layer, indicating an increase of adsorption of H atoms in the water ice layer. A penetration depth of 100 nm has been estimated for H atoms in the porous water ice covering carbon grains. Sample warm-up at room temperature causes the activation of the IR features due to the vibrations of the CH{sub 2} and CH{sub 3} aliphatic functional groups. The evolution of the 3.47 {mu}m band carrier has been evaluated for dense and diffuse interstellar clouds, using the estimated formation cross section and assuming that the destruction cross section by energetic processing is the same as that derived for the 3.4 {mu}m band. In both environments, the presence of the 3.47 {mu}m band carrier is compatible with the evolutionary timescale limit imposed by fast cycling of materials between dense and diffuse regions of the interstellar medium. In diffuse regions the formation of the CH{sub 2} and CH{sub 3} aliphatic bands, inhibited in dense regions, takes place, masking the 3.47 {mu}m band. The activation of the CH{sub 2} and CH{sub 3} aliphatic vibrational modes at the end of H processing after sample warm-up represents the first experimental evidence supporting an evolutionary connection between the interstellar carbon grain population, which is responsible for

Photoionization and Photofragmentation of Carbon Fullerene Molecular Ions

NASA Astrophysics Data System (ADS)

Baral, Kiran Kumar

Cross sections are reported for single and double photoionization accompanied by the loss of as many as seven pairs of C atoms of C60 + and C70+ fullerene molecular ions in the photon energy range 18 eV to 150 eV. These measurements were performed at the Advanced Light Source (ALS) by merging a mass-selected ion beam with a beam of monochromatized synchrotron radiation. Threshold energies were determined for the formation of doubly and triply charged fragment ions from parent ions C60+ and C70+. The energy dependences of cross-sections for direct photoionization yielding C60 2+ and C702+ are compared with those for forming different doubly and triply charged fullerene fragment ions. Two-dimensional product ion scans were measured and quantified at four discrete photon energies: 35 eV, 65 eV, 105 eV and 140 eV, in the vacuum ultraviolet region, providing a comprehensive mapping of the product channels involving single ionization of fullerene ions C60+ and C 70+ accompanied by fragmentation. Since fullerenes are composed of even numbers of carbon atoms, the fragmentation occurs by the loss of differing numbers of carbon atom pairs. In addition to pure ionization, fragmentation product channels become relatively more important at higher photon energies.

Carbon nanosheets-based supercapacitors: Design of dual redox additives of 1, 4-dihydroxyanthraquinone and hydroquinone for improved performance

NASA Astrophysics Data System (ADS)

Xu, Dong; Sun, Xiao Na; Hu, Wei; Chen, Xiang Ying

2017-07-01

Using thiocarbanilide and Mg(OH)2 powders as carbon precursor and template, respectively, novel 2D carbon nanosheets with large area have been produced. Next, based on the cooperative effect, 1, 4-dihydroxyanthraquinone (DQ) and hydroquinone (HQ) regarded as efficient dual redox additives have been incorporated into the electrode carbon material and H2SO4 electrolyte, respectively, to largely elevate the capacitive performance of supercapacitors. More importantly, the cooperative effect results from the redox processes of DQ and HQ consecutively occurring in the electrode carbon material and aqueous H2SO4 electrolyte, respectively. Besides, the molar ratio of DQ and HQ exerts a crucial role in the determination of the electrochemical behaviors and eventually the optimum condition is the mass ratio of 1:1 concerning the DQ and porous carbon within solid electrode while retaining the HQ concentration as 20 mmol L-1 in 1 mol L-1 H2SO4 electrolyte. As a result, the maximum specific capacitance is achieved of 239 F g-1 at 3 A g-1, and furthermore the maximum energy density up to 21.1 Wh kg-1 is almost 3.5 times larger than that of the one without introducing any redox additive.

The Structures & Properties of Carbon

ERIC Educational Resources Information Center

Castellini, Olivia M.; Lisensky, George C.; Ehrlich, Jennifer; Zenner, Greta M.; Crone, Wendy C.

2006-01-01

The four main forms of carbon--diamond, graphite, buckyballs, and carbon nanotubes (CNTs)--are an excellent vehicle for teaching fundamental principles of chemical bonding, material structure, and properties. Carbon atoms form a variety of structures that are intrinsically connected to the properties they exhibit. Educators can take advantage of…

Proposal for Testing and Validation of Vacuum Ultra-Violet Atomic Laser-Induced Fluorescence as a Method to Analyze Carbon Grid Erosion in Ion Thrusters

NASA Technical Reports Server (NTRS)

Stevens, Richard

2003-01-01

Previous investigation under award NAG3-25 10 sought to determine the best method of LIF to determine the carbon density in a thruster plume. Initial reports from other groups were ambiguous as to the number of carbon clusters that might be present in the plume of a thruster. Carbon clusters would certainly affect the ability to LIF; if they were the dominant species, then perhaps the LIF method should target clusters. The results of quadrupole mass spectroscopy on sputtered carbon determined that minimal numbers of clusters were sputtered from graphite under impact from keV Krypton. There were some investigations in the keV range by other groups that hinted at clusters, but at the time the proposal was presented to NASA, there was no data from low-energy sputtering available. Thus, the proposal sought to develop a method to characterize the population only of atoms sputtered from a graphite target in a test cell. Most of the ground work had been established by the previous two years of investigation. The proposal covering 2003 sought to develop an anti-Stokes Raman shifting cell to generate VUW light and test this cell on two different laser systems, ArF and YAG- pumped dye. The second goal was to measure the lowest detectable amounts of carbon atoms by 156.1 nm and 165.7 nm LIF. If equipment was functioning properly, it was expected that these goals would be met easily during the timeframe of the proposal, and that is the reason only modest funding was requested. The PI was only funded at half- time by Glenn during the summer months. All other work time was paid for by Whitworth College. The college also funded a student, Charles Shawley, who worked on the project during the spring.

A sputtering derived atomic oxygen source for studying fast atom reactions

NASA Technical Reports Server (NTRS)

Ferrieri, Richard A.; Yung, Y. Chu; Wolf, Alfred P.

1987-01-01

A technique for the generation of fast atomic oxygen was developed. These atoms are created by ion beam sputtering from metal oxide surfaces. Mass resolved ion beams at energies up to 60 KeV are produced for this purpose using a 150 cm isotope separator. Studies have shown that particles sputtered with 40 KeV Ar(+) on Ta2O5 were dominantly neutral and exclusively atomic. The atomic oxygen also resided exclusively in its 3P ground state. The translational energy distribution for these atoms peaked at ca 7 eV (the metal-oxygen bond energy). Additional measurements on V2O5 yielded a bimodal distribution with the lower energy peak at ca 5 eV coinciding reasonably well with the metal-oxygen bond energy. The 7 eV source was used to investigate fast oxygen atom reactions with the 2-butene stereoisomers. Relative excitation functions for H-abstraction and pi-bond reaction were measured with trans-2-butene. The abstraction channel, although of minor relative importance at thermal energy, becomes comparable to the addition channel at 0.9 eV and dominates the high-energy regime. Structural effects on the specific channels were also found to be important at high energy.

Localization of carbon atoms and extended defects in silicon implanted separately with C+ and B+ ions and jointly with C+ and B+ ions

NASA Astrophysics Data System (ADS)

Jadan, M.; Chelyadinskii, A. R.; Odzhaev, V. B.

2013-02-01

The possibility to control the localization of implanted carbon in sites and interstices in silicon immediately during the implantation has been demonstrated. The formation of residual extended defects in silicon implanted separately with C+ and B+ ions and jointly with C+ and B+ ions has been shown. It has been found that the formation of residual defects can be suppressed due to annihilation of point defects at C atoms (the Watkins effect). The positive effect is attained if implanted carbon is localized over lattice sites, which is provided by its implantation with the effective current density of the scanning ion beam no lower than 1.0 μA cm-2.

Effective Hubbard model for Helium atoms adsorbed on a graphite

NASA Astrophysics Data System (ADS)

Motoyama, Yuichi; Masaki-Kato, Akiko; Kawashima, Naoki

Helium atoms adsorbed on a graphite is a two-dimensional strongly correlated quantum system and it has been an attractive subject of research for a long time. A helium atom feels Lennard-Jones like potential (Aziz potential) from another one and corrugated potential from the graphite. Therefore, this system may be described by a hardcore Bose Hubbard model with the nearest neighbor repulsion on the triangular lattice, which is the dual lattice of the honeycomb lattice formed by carbons. A Hubbard model is easier to simulate than the original problem in continuous space, but we need to know the model parameters of the effective model, hopping constant t and interaction V. In this presentation, we will present an estimation of the model parameters from ab initio quantum Monte Carlo calculation in continuous space in addition to results of quantum Monte Carlo simulation for an obtained discrete model.

Effects of argon addition on a-CNx film deposition by hot carbon filament chemical vapor deposition

NASA Astrophysics Data System (ADS)

Watanabe, Yoshihisa; Aono, Masami; Yamazaki, Ayumi; Kitazawa, Nobuaki; Nakamura, Yoshikazu

2002-07-01

Using a carbon filament which supplies carbon and heat, amorphous carbon nitride (a-CNx) films were prepared on Si (100) substrates by hot filament chemical vapor deposition. Deposition was performed in a low-pressure atmosphere of pure nitrogen and a gas mixture of nitrogen and argon. Effects of argon additions to the nitrogen atmosphere on the film microstructure and interface composition between the film and substrate were studied by field-emission scanning electron microscopy (FESEM) and x-ray photoelectron spectroscopy (XPS). FESEM observations reveal that the film prepared in a pure nitrogen atmosphere has uniform nucleation and a densely packed columnar pieces structure. The film prepared in the nitrogen and argon gas mixture exhibits preferential nucleation and a tapered structure with macroscopic voids. Depth analyses using XPS reveal that the film prepared in pure nitrogen possesses a broad interface, which includes silicon carbide as well as a-CNx, whereas a sharp interface is discerned in the film prepared in the mixed nitrogen and argon gas. We observed that silicon carbide formation is suppressed by an argon addition to the nitrogen atmosphere during deposition. copyright 2002 American Vacuum Society.

Combustor exhaust-emissions and blowout-limits with diesel number 2 and jet A fuels utilizing air-atomizing and pressure atomizing nozzles

NASA Technical Reports Server (NTRS)

Ingebo, R. D.; Norgren, C. T.

1975-01-01

Experimental tests with diesel number 2 and Jet A fuels were conducted in a combustor segment to obtain comparative data on exhaust emissions and blowout limits. An air-atomizing nozzle was used to inject the fuels. Tests were also made with diesel number 2 fuel using a pressure-atomizing nozzle to determine the effectiveness of the air-atomizing nozzle in reducing exhaust emissions. Test conditions included fuel-air ratios of 0.008 to 0.018, inlet-air total pressures and temperatures of 41 to 203 newtons per square centimeter and 477 to 811 K, respectively, and a reference velocity of 21.3 meters per second. Smoke number and unburned hydrocarbons were twice as high with diesel number 2 as with Jet A fuel. This was attributed to diesel number 2 having a higher concentration of aromatics and lower volatility than Jet A fuel. Oxides of nitrogen, carbon monoxide, and blowout limits were approximately the same for the two fuels. The air-atomizing nozzle, as compared with the pressure-atomizing nozzle, reduced oxides-of-nitrogen by 20 percent, smoke number by 30 percent, carbon monoxide by 70 percent, and unburned hydrocarbons by 50 percent when used with diesel number 2 fuel.

Carbon films produced from ionic liquid carbon precursors

DOEpatents

Dai, Sheng; Luo, Huimin; Lee, Je Seung

2013-11-05

The invention is directed to a method for producing a film of porous carbon, the method comprising carbonizing a film of an ionic liquid, wherein the ionic liquid has the general formula (X.sup.+a).sub.x(Y.sup.-b).sub.y, wherein the variables a and b are, independently, non-zero integers, and the subscript variables x and y are, independently, non-zero integers, such that ax=by, and at least one of X.sup.+ and Y.sup.- possesses at least one carbon-nitrogen unsaturated bond. The invention is also directed to a composition comprising a porous carbon film possessing a nitrogen content of at least 10 atom %.

Consideration of critical axial properties of pristine and defected carbon nanotubes under compression.

PubMed

Ranjbartoreh, A R; Su, D; Wang, G

2012-06-01

Carbon nanotubes are hexagonally configured carbon atoms in cylindrical structures. Exceptionally high mechanical strength, electrical conductivity, surface area, thermal stability and optical transparency of carbon nanotubes outperformed other known materials in numerous advanced applications. However, their mechanical behaviors under practical loading conditions remain to be demonstrated. This study investigates the critical axial properties of pristine and defected single- and multi-walled carbon nanotubes under axial compression. Molecular dynamics simulation method has been employed to consider the destructive effects of Stone-Wales and atom vacancy defects on mechanical properties of armchair and zigzag carbon nanotubes under compressive loading condition. Armchair carbon nanotube shows higher axial stability than zigzag type. Increase in wall number leads to less susceptibility of multi-walled carbon nanotubes to defects and higher stability of them under axial compression. Atom vacancy defect reveals higher destructive effect than Stone-Wales defect on mechanical properties of carbon nanotubes. Critical axial strain of single-walled carbon nanotube declines by 67% and 26% due to atom vacancy and Stone-Wales defects.

Carbon dioxide hydrogenation on Ni(110).

PubMed

Vesselli, Erik; De Rogatis, Loredana; Ding, Xunlei; Baraldi, Alessandro; Savio, Letizia; Vattuone, Luca; Rocca, Mario; Fornasiero, Paolo; Peressi, Maria; Baldereschi, Alfonso; Rosei, Renzo; Comelli, Giovanni

2008-08-27

We demonstrate that the key step for the reaction of CO 2 with hydrogen on Ni(110) is a change of the activated molecule coordination to the metal surface. At 90 K, CO 2 is negatively charged and chemically bonded via the carbon atom. When the temperature is increased and H approaches, the H-CO 2 complex flips and binds to the surface through the two oxygen atoms, while H binds to the carbon atom, thus yielding formate. We provide the atomic-level description of this process by means of conventional ultrahigh vacuum surface science techniques combined with density functional theory calculations and corroborated by high pressure reactivity tests. Knowledge about the details of the mechanisms involved in this reaction can yield a deeper comprehension of heterogeneous catalytic organic synthesis processes involving carbon dioxide as a reactant. We show why on Ni the CO 2 hydrogenation barrier is remarkably smaller than that on the common Cu metal-based catalyst. Our results provide a possible interpretation of the observed high catalytic activity of NiCu alloys.

Atomic spectrometry update - atomic mass spectrometry.

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

Bacon, J.; Crain, J. S.; McMahon, A. W.

The MS and XRF updates have been published together since their introduction in 1988. In the last few years, however, the two sections have been prepared independently of each other and it therefore seemed appropriate to publish the two sections separately. With effect from this issue, the MS Update will appear in the October issue of JAAS and the XRF Update in the November issue. The format used for the MS section is broadly similar to that used last year, with some additional sub-headings. This Update is intended to cover all atomic and stable isotopic MS techniques, but not thosemore » used in studies of fundamental nuclear physics and exotic nuclei far from stability. Also excluded are those reports in which MS is used as a tool in the study of molecular processes and of gaseous components. the review is based on critical selection of developments in instrumentation and methodology, notable for their innovation, originality or achievement of significant advances, and is not intended to be comprehensive in its coverage. Conference papers are only included if they contain enough information to show they meet these criteria, and our policy in general remains one of waiting for a development to appear in a full paper before inclusion in the review. a similar policy applies to foreign language papers unlikely to reach a wide audience. Routine applications of atomic MS are not included in this Update and the reader is referred to the Updates on Industrial Analysis: Metals, Chemicals and Advanced Materials (96/416), Environmental Analysis (96/1444) and Clinical and Biological Materials, Food and Beverages (96/2479). Also excluded are those applications, even if not routine, which use atomic spectroscopy as a tool for the study of a non-atomic property, for example, the use of stable isotope labeling of carbon or nitrogen in biomolecules in metabolic studies. There have been few general reviews on atomic MS of note in the period covered by this update. That of

Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts.

PubMed

Yin, Peiqun; Yao, Tao; Wu, Yuen; Zheng, Lirong; Lin, Yue; Liu, Wei; Ju, Huanxin; Zhu, Junfa; Hong, Xun; Deng, Zhaoxiang; Zhou, Gang; Wei, Shiqiang; Li, Yadong

2016-08-26

A new strategy for achieving stable Co single atoms (SAs) on nitrogen-doped porous carbon with high metal loading over 4 wt % is reported. The strategy is based on a pyrolysis process of predesigned bimetallic Zn/Co metal-organic frameworks, during which Co can be reduced by carbonization of the organic linker and Zn is selectively evaporated away at high temperatures above 800 °C. The spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurements both confirm the atomic dispersion of Co atoms stabilized by as-generated N-doped porous carbon. Surprisingly, the obtained Co-Nx single sites exhibit superior ORR performance with a half-wave potential (0.881 V) that is more positive than commercial Pt/C (0.811 V) and most reported non-precious metal catalysts. Durability tests revealed that the Co single atoms exhibit outstanding chemical stability during electrocatalysis and thermal stability that resists sintering at 900 °C. Our findings open up a new routine for general and practical synthesis of a variety of materials bearing single atoms, which could facilitate new discoveries at the atomic scale in condensed materials. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

High performance, rapid thermal/UV curing epoxy resin for additive manufacturing of short and continuous carbon fiber epoxy composites

DOEpatents

Lewicki, James

2018-04-17

An additive manufacturing resin system including an additive manufacturing print head; a continuous carbon fiber or short carbon fibers operatively connected to the additive manufacturing print head; and a tailored resin operatively connected to the print head, wherein the tailored resin has a resin mass and wherein the tailored resin includes an epoxy component, a filler component, a catalyst component, and a chain extender component; wherein the epoxy component is 70-95% of the resin mass, wherein the filler component is 1-20% of the resin mass, wherein the catalyst component is 0.1-10% of the resin mass, and wherein the chain extender component is 0-50% of the resin mass.

When hydroquinone meets methoxy radical: Hydrogen abstraction reaction from the viewpoint of interacting quantum atoms.

PubMed

Petković, Milena; Nakarada, Đura; Etinski, Mihajlo

2018-05-25

Interacting Quantum Atoms methodology is used for a detailed analysis of hydrogen abstraction reaction from hydroquinone by methoxy radical. Two pathways are analyzed, which differ in the orientation of the reactants at the corresponding transition states. Although the discrepancy between the two barriers amounts to only 2 kJ/mol, which implies that the two pathways are of comparable probability, the extent of intra-atomic and inter-atomic energy changes differs considerably. We thus demonstrated that Interacting Quantum Atoms procedure can be applied to unravel distinct energy transfer routes in seemingly similar mechanisms. Identification of energy components with the greatest contribution to the variation of the overall energy (intra-atomic and inter-atomic terms that involve hydroquinone's oxygen and the carbon atom covalently bound to it, the transferring hydrogen and methoxy radical's oxygen), is performed using the Relative energy gradient method. Additionally, the Interacting Quantum Fragments approach shed light on the nature of dominant interactions among selected fragments: both Coulomb and exchange-correlation contributions are of comparable importance when considering interactions of the transferring hydrogen atom with all other atoms, whereas the exchange-correlation term dominates interaction between methoxy radical's methyl group and hydroquinone's aromatic ring. This study represents one of the first applications of Interacting Quantum Fragments approach on first order saddle points. © 2018 Wiley Periodicals, Inc. © 2018 Wiley Periodicals, Inc.

Multi-functional carbon nanomaterials: Tailoring morphology for multidisciplinary applications

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

Dervishi, Enkeleda

2015-05-14

Carbon based nanomaterials are being developed to have many new properties and applications. Graphene, is a mono-layer 2D atomic thick structure formed from hexagons of carbon atoms bound together by sp^2hybrid bonds. A carbon nanotube (CNT) can be viewed as a sheet of graphene rolled up into a cylinder, usually 1-2 nanometers in diameter and a few microns thick. A few applications of graphene and carbon nanotubes include the development of Nanoelectronics, nanocomposite materials, Hydrogen storage and Li⁺ battery, etc.

Molybdoenzyme That Catalyzes the Anaerobic Hydroxylation of a Tertiary Carbon Atom in the Side Chain of Cholesterol*

PubMed Central

Dermer, Juri; Fuchs, Georg

2012-01-01

Cholesterol is a ubiquitous hydrocarbon compound that can serve as substrate for microbial growth. This steroid and related cyclic compounds are recalcitrant due to their low solubility in water, complex ring structure, the presence of quaternary carbon atoms, and the low number of functional groups. Aerobic metabolism therefore makes use of reactive molecular oxygen as co-substrate of oxygenases to hydroxylate and cleave the sterane ring system. Consequently, anaerobic metabolism must substitute oxygenase-catalyzed steps by O2-independent hydroxylases. Here we show that one of the initial reactions of anaerobic cholesterol metabolism in the β-proteobacterium Sterolibacterium denitrificans is catalyzed by an unprecedented enzyme that hydroxylates the tertiary C25 atom of the side chain without molecular oxygen forming a tertiary alcohol. This steroid C25 dehydrogenase belongs to the dimethyl sulfoxide dehydrogenase molybdoenzyme family, the closest relative being ethylbenzene dehydrogenase. It is a heterotrimer, which is probably located at the periplasmic side of the membrane and contains one molybdenum cofactor, five [Fe-S] clusters, and one heme b. The draft genome of the organism contains several genes coding for related enzymes that probably replace oxygenases in steroid metabolism. PMID:22942275

Investigating permeability and carbonation behavior of sustainable cements

NASA Astrophysics Data System (ADS)

White, C.; Blyth, A.; Scherer, G. W.; Morandeau, A. E.

2015-12-01

The durability of new sustainable cementitious materials is intimately linked with the ability for these materials to prevent the ingress of aggressive ions through their percolated pore networks. However, it is also important to be able to control and limit the detrimental chemical degradation mechanisms that occur to the cement binder once the ions have diffused through the pore network. Here, alkali-activated materials will be discussed, and recent research on measuring the permeability of this class of cements using the beam-bending method will be presented. It will be shown that the permeability can be controlled by tailoring the activator chemistry, and that the addition of free silica in the activator has a strong (favorable) influence on the resulting percolated pore network. Carbonation is one type of chemical degradation process that is known to severely shorten the service life of concrete, especially in environments containing elevated CO­2 levels. However, the exact atomic structural changes that occur to the main binder phase (calcium-silicate-hydrate gel) during carbonation remain largely unknown. Here, X-ray pair distribution function analysis is used to elucidate the local atomic structural changes that occur during carbonation of calcium-silicate-hydrate gel and calcium-aluminosilicate-hydrate gel (alkali-activated slag binder), where distinct differences in the extent of gel decalcification are measured according to the chemistry of the starting precursor material. The results will be discussed in the context of limiting the extent of carbonation in cementitious materials, with potential applications of alkali-activated materials in geological storage of CO2 due to their increased resistance to carbonation.

Effective Permeability Change in Wellbore Cement with Carbon Dioxide Reaction

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

Um, Wooyong; Jung, Hun Bok; Martin, Paul F.

2011-11-01

Portland cement, a common sealing material for wellbores for geological carbon sequestration was reacted with CO{sub 2} in supercritical, gaseous, and aqueous phases at various pressure and temperature conditions to simulate cement-CO{sub 2} reaction along the wellbore from carbon injection depth to the near-surface. Hydrated Portland cement columns (14 mm diameter x 90 mm length; water-to-cement ratio = 0.33) including additives such as steel coupons and Wallula basalt fragments were reacted with CO{sub 2} in the wet supercritical (the top half) and dissolved (the bottom half) phases under carbon sequestration condition with high pressure (10 MPa) and temperature (50 C)more » for 5 months, while small-sized hydrated Portland cement columns (7 mm diameter x 20 mm length; water-to-cement ratio = 0.38) were reacted with CO{sub 2} in dissolved phase at high pressure (10 MPa) and temperature (50 C) for 1 month or with wet CO{sub 2} in gaseous phase at low pressure (0.2 MPa) and temperature (20 C) for 3 months. XMT images reveal that the cement reacted with CO{sub 2} saturated groundwater had degradation depth of {approx}1 mm for 1 month and {approx}3.5 mm for 5 month, whereas the degradation was minor with cement exposure to supercritical CO{sub 2}. SEM-EDS analysis showed that the carbonated cement was comprised of three distinct zones; the innermost less degraded zone with Ca atom % > C atom %, the inner degraded zone with Ca atom % {approx} C atom % due to precipitation of calcite, the outer degraded zone with C atom % > Ca atom % due to dissolution of calcite and C-S-H, as well as adsorption of carbon to cement matrix. The outer degraded zone of carbonated cement was porous and fractured because of dissolution-dominated reaction by carbonic acid exposure, which resulted in the increase in BJH pore volume and BET surface area. In contrast, cement-wet CO{sub 2}(g) reaction at low P (0.2 MPa)-T (20 C) conditions for 1 to 3 months was dominated by precipitation of

Reaction and Protection of Electrical Wire Insulators in Atomic-oxygen Environments

NASA Technical Reports Server (NTRS)

Hung, Ching-Cheh; Cantrell, Gidget

1994-01-01

Atomic-oxygen erosion on spacecraft in low Earth orbit is an issue which is becoming increasingly important because of the growing number of spacecraft that will fly in the orbits which have high concentrations of atomic oxygen. In this investigation, the atomic-oxygen durability of three types of electrical wire insulation (carbon-based, fluoropolymer, and polysiloxane elastomer) were evaluated. These insulation materials were exposed to thermal-energy atomic oxygen, which was obtained by RF excitation of air at a pressure of 11-20 Pa. The effects of atomic-oxygen exposure on insulation materials indicate that all carbon-based materials erode at about the same rate as polyamide Kapton and, therefore, are not atomic-oxygen durable. However, the durability of fluoropolymers needs to be evaluated on a case by case basis because the erosion rates of fluoropolymers vary widely. For example, experimental data suggest the formation of atomic fluorine during atomic-oxygen amorphous-fluorocarbon reactions. Dimethyl polysiloxanes (silicone) do not lose mass during atomic-oxygen exposure, but develop silica surfaces which are under tension and frequently crack as a result of loss of methyl groups. However, if the silicone sample surfaces were properly pretreated to provide a certain roughness, atomic oxygen exposure resulted in a sturdy, non-cracked atomic-oxygen durable SiO2 layer. Since the surface does not crack during such silicone-atomic oxygen reaction, the crack-induced contamination by silicone can be reduced or completely stopped. Therefore, with proper pretreatment, silicone can be either a wire insulation material or a coating on wire insulation materials to provide atomic-oxygen durability.

Stimulation of terrestrial ecosystem carbon storage by nitrogen addition: a meta-analysis

PubMed Central

Yue, Kai; Peng, Yan; Peng, Changhui; Yang, Wanqin; Peng, Xin; Wu, Fuzhong

2016-01-01

Elevated nitrogen (N) deposition alters the terrestrial carbon (C) cycle, which is likely to feed back to further climate change. However, how the overall terrestrial ecosystem C pools and fluxes respond to N addition remains unclear. By synthesizing data from multiple terrestrial ecosystems, we quantified the response of C pools and fluxes to experimental N addition using a comprehensive meta-analysis method. Our results showed that N addition significantly stimulated soil total C storage by 5.82% ([2.47%, 9.27%], 95% CI, the same below) and increased the C contents of the above- and below-ground parts of plants by 25.65% [11.07%, 42.12%] and 15.93% [6.80%, 25.85%], respectively. Furthermore, N addition significantly increased aboveground net primary production by 52.38% [40.58%, 65.19%] and litterfall by 14.67% [9.24%, 20.38%] at a global scale. However, the C influx from the plant litter to the soil through litter decomposition and the efflux from the soil due to microbial respiration and soil respiration showed insignificant responses to N addition. Overall, our meta-analysis suggested that N addition will increase soil C storage and plant C in both above- and below-ground parts, indicating that terrestrial ecosystems might act to strengthen as a C sink under increasing N deposition. PMID:26813078

Design considerations regarding an atomizer for multi-element electrothermal atomic absorption spectrometry

NASA Astrophysics Data System (ADS)

Katskov, Dmitri A.; Sadagov, Yuri M.

2011-06-01

The methodology of simultaneous multi-element electrothermal atomic absorption spectrometry (ETAAS-Electrothermal Atomic Absorption Spectrometry) stipulates rigid requirements to the design and operation of the atomizer. It must provide high degree of atomization for the group of analytes, invariant respective to the vaporization kinetics and heating ramp residence time of atoms in the absorption volume and absence of memory effects from major sample components. For the low resolution spectrometer with a continuum radiation source the reduced compared to traditional ETAAS (Electrothermal Atomic Absorption Spectrometry) sensitivity should be, at least partially, compensated by creating high density of atomic vapor in the absorption pulse. The sought-for characteristics were obtained for the 18 mm in length and 2.5 mm in internal diameter longitudinally heated graphite tube atomizer furnished with 2-4.5 mg of ring shaped carbon fiber yarn collector. The collector located next to the sampling port provides large substrate area that helps to keep the sample and its residue in the central part of the tube after drying. The collector also provides a "platform" effect that delays the vaporization and stipulates vapor release into absorption volume having already stabilized gas temperature. Due to the shape of external surface of the tube, presence of collector and rapid (about 10 °C/ms) heating, an inverse temperature distribution along the tube is attained at the beginnings of the atomization and cleaning steps. The effect is employed for cleaning of the atomizer using the set of short maximum power heating pulses. Preparation, optimal maintenance of the atomizer and its compliance to the multi-element determination requirements are evaluated and discussed. The experimental setup provides direct simultaneous determination of large group of element within 3-4 order concentration range. Limits of detection are close to those for sequential single element determination in

Composite catalyst for carbon monoxide and hydrocarbon oxidation

DOEpatents

Liu, W.; Flytzani-Stephanopoulos, M.

1996-03-19

A method and composition are disclosed for the complete oxidation of carbon monoxide and/or hydrocarbon compounds. The method involves reacting the carbon monoxide and/or hydrocarbons with an oxidizing agent in the presence of a metal oxide composite catalyst. The catalyst is prepared by combining fluorite-type oxygen ion conductors with active transition metals. The fluorite oxide, selected from the group consisting of cerium oxide, zirconium oxide, thorium oxide, hafnium oxide, and uranium oxide, and may be doped by alkaline earth and rare earth oxides. The transition metals, selected from the group consisting of molybdenum, copper, cobalt, manganese, nickel, and silver, are used as additives. The atomic ratio of transition metal to fluorite oxide is less than one.

Composite catalyst for carbon monoxide and hydrocarbon oxidation

DOEpatents

Liu, Wei; Flytzani-Stephanopoulos, Maria

1996-01-01

A method and composition for the complete oxidation of carbon monoxide and/or hydrocarbon compounds. The method involves reacting the carbon monoxide and/or hydrocarbons with an oxidizing agent in the presence of a metal oxide composite catalyst. The catalyst is prepared by combining fluorite-type oxygen ion conductors with active transition metals. The fluorite oxide, selected from the group consisting of cerium oxide, zirconium oxide, thorium oxide, hafnium oxide, and uranium oxide, and may be doped by alkaline earth and rare earth oxides. The transition metals, selected from the group consisting of molybdnum, copper, cobalt, maganese, nickel, and silver, are used as additives. The atomic ratio of transition metal to fluorite oxide is less than one.

Angular distribution of hybridization in sputtered carbon thin film

NASA Astrophysics Data System (ADS)

Liu, Y.; Wang, H.; Wei, Z. C.

2017-08-01

The sp3/sp2 ratio of sputtered carbon thin film depends on the ion bombardment process and tailors the physical properties of carbon thin film. In present work, we report the angular distribution of hybridization in magnetron sputtered carbon thin film for the first time. By x-ray photoelectron spectra analyses, it is found that the sp3/sp2 ratio increases linearly with increasing the deposition angle from 0 to 90 degree, which could be attributed to the enhancement of direct knocking-out of near-surface target atoms. In addition, we also derive the sp3/sp2 ratio by simulation on complex permittivity in terahertz frequency using a modified percolation approximation tunneling model. Those derived data consist with the results from x-ray photoelectron spectroscopy.

3-D Observation of dopant distribution at NAND flash memory floating gate using Atom probe tomography

NASA Astrophysics Data System (ADS)

Lee, Ji-hyun; Chae, Byeong-Kyu; Kim, Joong-Jeong; Lee, Sun Young; Park, Chan Gyung

2015-01-01

Dopant control becomes more difficult and critical as silicon devices become smaller. We observed the dopant distribution in a thermally annealed polysilicon gate using Transmission Electron Microscopy (TEM) and Atom probe tomography (APT). Phosphorus was doped at the silicon-nitride-diffusion-barrier-layer-covered polycrystalline silicon gate. Carbon also incorporated at the gate for the enhancement of operation uniformity. The impurity distribution was observed using atom probe tomography. The carbon atoms had segregated at grain boundaries and suppressed silicon grain growth. Phosphorus atoms, on the other hand, tended to pile-up at the interface. A 1-nm-thick diffusion barrier effectively blocked P atom out-diffusion. [Figure not available: see fulltext.

Characterization of Thermoplastic Polyurethane (TPU) and Ag Carbon Black TPU Nanocomposite for Potential Application in Additive Manufacturing (Postprint)

DTIC Science & Technology

2016-12-29

APPLICATION IN ADDITIVE MANUFACTURING (POSTPRINT) Steven T. Patton, Chenggang Chen, Jianjun Hu, and Lawrence Grazulis University of Dayton Research...CARBON BLACK TPU NANOCOMPOSITE FOR POTENTIAL APPLICATION IN ADDITIVE MANUFACTURING (POSTPRINT) 5a. CONTRACT NUMBER FA8650-11-D-5401-0008 5b...and polymer nanocomposites (PNCs) are of interest for additive manufacturing (AM) and flexible electronics. Development/optimization of inks for AM

Nitrogen-doped carbon monolith for alkaline supercapacitors and understanding nitrogen-induced redox transitions.

PubMed

Wang, Da-Wei; Li, Feng; Yin, Li-Chang; Lu, Xu; Chen, Zhi-Gang; Gentle, Ian R; Lu, Gao Qing; Cheng, Hui-Ming

2012-04-23

A nitrogen-doped porous carbon monolith was synthesized as a pseudo-capacitive electrode for use in alkaline supercapacitors. Ammonia-assisted carbonization was used to dope the surface with nitrogen heteroatoms in a way that replaced carbon atoms but kept the oxygen content constant. Ammonia treatment expanded the micropore size-distributions and increased the specific surface area from 383 m(2) g(-1) to 679 m(2) g(-1). The nitrogen-containing porous carbon material showed a higher capacitance (246 F g(-1)) in comparison with the nitrogen-free one (186 F g(-1)). Ex situ electrochemical spectroscopy was used to investigate the evolution of the nitrogen-containing functional groups on the surface of the N-doped carbon electrodes in a three-electrode cell. In addition, first-principles calculations were explored regarding the electronic structures of different nitrogen groups to determine their relative redox potentials. We proposed possible redox reaction pathways based on the calculated redox affinity of different groups and surface analysis, which involved the reversible attachment/detachment of hydroxy groups between pyridone and pyridine. The oxidation of nitrogen atoms in pyridine was also suggested as a possible reaction pathway. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Atomic oxygen beam source for erosion simulation

NASA Technical Reports Server (NTRS)

Cuthbertson, J. W.; Langer, W. D.; Motley, R. W.; Vaughn, J. A.

1991-01-01

A device for the production of low energy (3 to 10 eV) neutral atomic beams for surface modification studies is described that reproduces the flux of atomic oxygen in low Earth orbit. The beam is produced by the acceleration of plasma ions onto a negatively biased plate of high-Z metal; the ions are neutralized and reflected by the surface, retaining some fraction of their incident kinetic energy, forming a beam of atoms. The plasma is generated by a coaxial RF exciter which produces a magnetically-confined (4 kG) plasma column. At the end of the column, ions fall through the sheath to the plate, whose bias relative to the plasma can be varied to adjust the beam energy. The source provides a neutral flux approximately equal to 5 x 10(exp 16)/sq cm at a distance of 9 cm and a fluence approximately equal to 10(exp 20)/sq cm in five hours. The composition and energy of inert gas beams was diagnosed using a mass spectometer/energy analyzer. The energy spectra of the beams demonstrate energies in the range 5 to 15 eV, and qualitatively show expected dependences upon incident and reflecting atom species and potential drop. Samples of carbon film, carbon-based paint, Kapton, mylar, and teflon exposed to atomic O beams show erosion quite similar to that observed in orbit on the space shuttle.

First principles study of NH3 adsorption on carbon nanowires

NASA Astrophysics Data System (ADS)

Tapia, Jorge-Alejandro; Sanchez, Alvaro-Daniel; Acosta, Cesar; Canto, Gabriel

2009-03-01

Recently has been reported a new type of one-dimensional carbon structures. Carbon nanowires formed by a linear carbon-atom chain inside an armchair (5,5) carbon nanotube has been observed using high-resolution transmission electron microscopy. Theoretical and experimental studies of the NH3 adsorption in the carbon nanotubes report changes in the electronic properties of the carbon nanotubes. In the present work we have studied the electronic and structure properties of carbon nanowires (chain@SWCNT) when NH3 atoms are adsorbed. We used the Density Functional Theory and the calculations where performed by the pseudopotentials LCAO method (SIESTA code) and the Generalized Gradient Approximation (GGA) for the exchange-correlation potential. We have analyzed the changes in the atomic structure and density of states (DOS). We found that the electronic character of the carbon chain of the chain@SWCNT system, can be modulate by NH3 adsorption. This research was supported by SEP under Grant No. PROMEP/103.5/07/2595 and the Consejo Nacional de Ciencia y Tecnolog'ia (Conacyt) under Grants No. 82497 and 60534.

Rapid oxidation/stabilization technique for carbon foams, carbon fibers and C/C composites

DOEpatents

Tan, Seng; Tan, Cher-Dip

2004-05-11

An enhanced method for the post processing, i.e. oxidation or stabilization, of carbon materials including, but not limited to, carbon foams, carbon fibers, dense carbon-carbon composites, carbon/ceramic and carbon/metal composites, which method requires relatively very short and more effective such processing steps. The introduction of an "oxygen spill over catalyst" into the carbon precursor by blending with the carbon starting material or exposure of the carbon precursor to such a material supplies required oxygen at the atomic level and permits oxidation/stabilization of carbon materials in a fraction of the time and with a fraction of the energy normally required to accomplish such carbon processing steps. Carbon based foams, solids, composites and fiber products made utilizing this method are also described.

High temperature superconductivity in distinct phases of amorphous B-doped Q-carbon

NASA Astrophysics Data System (ADS)

Narayan, Jagdish; Bhaumik, Anagh; Sachan, Ritesh

2018-04-01

Distinct phases of B-doped Q-carbon are formed when B-doped and undoped diamond tetrahedra are packed randomly after nanosecond laser melting and quenching of carbon. By changing the ratio of doped to undoped tetrahedra, distinct phases of B-doped Q-carbon with concentration varying from 5.0% to 50.0% can be created. We have synthesized three distinct phases of amorphous B-doped Q-carbon, which exhibit high-temperature superconductivity following the Bardeen-Cooper-Schrieffer mechanism. The first phase (QB1) has a B-concentration ˜17 at. % (Tc = 37 K), the second phase (QB2) has a B-concentration ˜27 at. % (Tc = 55 K), and the third phase (QB3) has a B-concentration ˜45 at. % (Tc expected over 100 K). From geometrical modeling, we derive that QB1 consists of randomly packed tetrahedra, where one out of every three tetrahedra contains a B atom in the center which is sp3 bonded to four carbon atoms with a concentration of 16.6 at. %. QB2 consists of randomly packed tetrahedra, where one out of every two tetrahedra contains a B atom in the center which is sp3 bonded to four carbon atoms with a concentration of 25 at. %. QB3 consists of randomly packed tetrahedra, where every tetrahedron contains a B atom in the center which is sp3 bonded to four carbon atoms with a concentration of 50 at. %. We present detailed high-resolution TEM results on structural characterization, and EELS and Raman spectroscopy results on the bonding characteristics of B and C atoms. From these studies, we conclude that the high electronic density of states near the Fermi energy level coupled with moderate electron-phonon coupling result in high-temperature superconductivity in B-doped Q-carbon.

Many faces of carbon

NASA Astrophysics Data System (ADS)

Wang, Qian; Zhang, Shunhong; Jena, Puru

2016-12-01

Due to the special electronic configuration, small atomic size, light mass, and flexible bonding features, carbon exhibits many different structural configurations with very different physical and chemical properties. Here we focus our discussion on three recent forms of carbon, namely, metallic carbon, magnetic carbon, and all-pentagon-based carbon. The metallic carbon can be used for metallic interconnects in future electronic circuits, nano devices and microprocessors while the magnetic carbon can have applications in spintronics. All-pentagon-based carbon nano-structure, penta-graphene, not only expands the family of carbon materials with a number of new features, but also provides the materials basis for the 2D packing of pentagons pursued by mathematicians for almost a century.

Copper-catalyzed asymmetric conjugate addition of Grignard reagents to trisubstituted enones. Construction of all-carbon quaternary chiral centers.

PubMed

Martin, David; Kehrli, Stefan; d'Augustin, Magali; Clavier, Hervé; Mauduit, Marc; Alexakis, Alexandre

2006-07-05

The copper-catalyzed asymmetric conjugate addition of Grignard reagents to trisubstituted cyclic enones affords enantioenriched all-carbon quaternary centers with up to 96% ee. The chiral ligand is a diaminocarbene, directly generated in situ. The combination of Grignard reagent and diaminocarbene is unprecedented in conjugate addition, and the additon of the phenyl group, on such enones, cannot be done by other conjugate addition methods.

Quantifying atom addition reactions on amorphous solid water: a review of recent laboratory advances

NASA Astrophysics Data System (ADS)

He, Jiao; Vidali, Gianfranco

2018-06-01

Complex organic molecules found in space are mostly formed on and in the ice mantle covering interstellar dust grains. In clouds where ionizing irradiation is insignificant, chemical reactions on the ice mantle are dominated by thermal processes. Modeling of grain surface chemistry requires detailed information from the laboratory, including sticking coefficients, binding energies, diffusion energy barriers, mechanism of reaction, and chemical desorption rates. In this talk, recent laboratory advances in obtaining these information would be reviewed. Specifically, this talk will focus on the efforts in our group in: 1) Determining the mechanism of atomic hydrogen addition reactions on amorphous solid water (ASW); 2) Measuring the chemical desorption coefficient of H+O3-->O2+OH using the time-resolved scattering technique; and 3) Measuring the diffusion energy barrier of volatile molecules on ASW. Further laboratory studies will be suggested.This research was supported by NSF Astronomy & Astrophysics Research Grant #1615897.

Atomic scale simulations of vapor cooled carbon clusters

NASA Astrophysics Data System (ADS)

Bogana, M. P.; Colombo, L.

2007-03-01

By means of atomistic simulations we observed the formation of many topologically non-equivalent carbon clusters formed by the condensation of liquid droplets, including: (i) standard fullerenes and onion-like structures, (ii) clusters showing extremely complex surfaces with both positive and negative curvatures and (iii) complex endohedral structures. In this work we offer a thorough structural characterization of the above systems, as well as an attempt to correlate the resulting structure to the actual protocol of growth. The IR and Raman responses of some exotic linear carbon structures have been further investigated, finding good agreement with experimental evidence of carbinoid structures in cluster-assembled films. Towards the aim of fully understanding the process of cluster-to-cluster coalescence dynamics, we further simulated an aerosol of amorphous carbon clusters at controlled temperatures. Various annealing temperatures and times have been observed, identifying different pathways for cluster ripening, ranging from simple coalescence to extensive reconstruction.

Synthesis of Antimony Doped Amorphous Carbon Films

NASA Astrophysics Data System (ADS)

Okuyama, H.; Takashima, M.; Akasaka, H.; Ohtake, N.

2013-06-01

We report the effects of antimony (Sb) doping on the electrical and optical properties of amorphous carbon (a-C:H) films grown on silicon and copper substrates by magnetron sputtering deposition. For film deposition, the mixture targets fabricated from carbon and antimony powders was used. The atomic concentration of carbon, hydrogen, and antimony, in the film deposited from the 1.0 mol% Sb containing target were 81, 17, 2 at.%, respectively. These elements were homogeneously distributed in the film. On the structural effect, the average continuous sp2 carbon bonding networks decreased with Sb concentration increasing, and defects in the films were increased with the Sb incorporation because atomic radius of Sb atoms is twice larger size than that of carbon. The optical gap and the electrical resistivity were carried out before and after the Sb doping. The results show that optical gap dropped from 3.15 to 3.04 eV corresponding to non-doping to Sb-doping conditions, respectively. The electrical resistivity reduced from 10.5 to 1.0 MΩm by the Sb doping. These results suggest the doping level was newly formed in the forbidden band.

Tribological improvements of carbon-carbon composites by infiltration of atomic layer deposited lubricious nanostructured ceramic oxides

NASA Astrophysics Data System (ADS)

Mohseni, Hamidreza

A number of investigators have reported enhancement in oxidation and wear resistant of carbon-carbon composites (CCC) in the presence of protective coating layers. However, application of a surface and subsurface coating system that can preserve its oxidation and wear resistance along with maintaining lubricity at high temperature remains unsolved. To this end, thermodynamically stable protective oxides (ZnO/Al2O3/ZrO2) have been deposited by atomic layer deposition (ALD) to infiltrate porous CCC and graphite foams in order to improve the thermal stability and wear resistance in low and high speed sliding contacts. Characterization of microstructural evolution was achieved by using energy dispersive x-ray spectroscopy (EDS) mapping in scanning electron microscope (SEM) coupled with focused ion beam (FIB), x-ray tomography, high resolution transmission electron microscopy (HRTEM), scanning transmission electron microscopy (STEM) and X-ray diffraction (XRD). Evaluation of the tribological properties of CCC coated with abovementioned ALD thin films were performed by employing low speed pure sliding tribometer and a high speed/frequency reciprocating rig to simulate the fretting wear behavior at ambient temperature and elevated temperatures of 400°C. It was determined with x-ray tomography imaging and EDS mapping that ALD ZnO/Al2O3/ZrO2 nanolaminates and baseline ZrO2 coatings exhibited excellent conformality and pore-filling capabilities down to ˜100 microm and 1.5 mm in the porous CCC and graphite foam, respectively, which were dependent on the exposure time of the ALD precursors. XRD and HRTEM determined the crystalline phases of {0002} textured ZnO (wurtzite), amorphous Al2O3, and {101}-tetragonal ZrO2. Significant improvements up to ˜65% in the sliding and fretting wear factors were determined for the nanolaminates in comparison to the uncoated CCC. A tribochemical sliding-induced mechanically mixed layer (MML) was found to be responsible for these improvements

Evolution of the atomic order and valence state of rare-earth atoms and uranium in a new carbon-metal composite—diphthalocyanine pyrolysate C64H32N16 Me ( Me = Y, La, Ce, Eu, and U)

NASA Astrophysics Data System (ADS)

Sovestnov, A. E.; Kapustin, V. K.; Tikhonov, V. I.; Fomin, E. V.; Chernenkov, Yu. P.

2014-08-01

The structure of a metal-carbon composite formed by the pyrolysis of diphthalocyanine of some rare-earth elements (Y, La, Ce, Eu) and uranium in the temperature range T ann = 800-1700°C has been investigated for the first time by the methods of X-ray diffraction analysis and X-ray line shift. It has been shown that, in the general case, the studied pyrolysates consist of three phases. One phase corresponds to the structure of graphite. The second phase corresponds to nitrides, carbides, and oxides of basic metal elements with a crystallite size ranging from 5 to 100 nm. The third phase is amorphous or consisting of crystallites with a size of ˜1 nm. It has been found that all the basic elements (Y, La, Ce, Eu, U) and incorporated iodine atoms in the third phase are in a chemically bound state. The previously unobserved electronic configurations have been revealed for europium. The possibility of including not only atoms of elements forming diphthalocyanine but also other elements (for example, iodine) in the composite structure is of interest, in particular, for the creation of a thermally, chemically, and radiation resistant metal-carbon matrix for the radioactive waste storage.

Water- and Plant-Mediated Responses of Ecosystem Carbon Fluxes to Warming and Nitrogen Addition on the Songnen Grassland in Northeast China

PubMed Central

Jiang, Li; Guo, Rui; Zhu, Tingcheng; Niu, Xuedun; Guo, Jixun; Sun, Wei

2012-01-01

Background Understanding how grasslands are affected by a long-term increase in temperature is crucial to predict the future impact of global climate change on terrestrial ecosystems. Additionally, it is not clear how the effects of global warming on grassland productivity are going to be altered by increased N deposition and N addition. Methodology/Principal Findings In-situ canopy CO2 exchange rates were measured in a meadow steppe subjected to 4-year warming and nitrogen addition treatments. Warming treatment reduced net ecosystem CO2 exchange (NEE) and increased ecosystem respiration (ER); but had no significant impacts on gross ecosystem productivity (GEP). N addition increased NEE, ER and GEP. However, there were no significant interactions between N addition and warming. The variation of NEE during the four experimental years was correlated with soil water content, particularly during early spring, suggesting that water availability is a primary driver of carbon fluxes in the studied semi-arid grassland. Conclusion/Significance Ecosystem carbon fluxes in grassland ecosystems are sensitive to warming and N addition. In the studied water-limited grassland, both warming and N addition influence ecosystem carbon fluxes by affecting water availability, which is the primary driver in many arid and semiarid ecosystems. It remains unknown to what extent the long-term N addition would affect the turn-over of soil organic matter and the C sink size of this grassland. PMID:23028848

Carbon doped PDMS: conductance stability over time and implications for additive manufacturing of stretchable electronics

NASA Astrophysics Data System (ADS)

Tavakoli, Mahmoud; Rocha, Rui; Osorio, Luis; Almeida, Miguel; de Almeida, Anibal; Ramachandran, Vivek; Tabatabai, Arya; Lu, Tong; Majidi, Carmel

2017-03-01

Carbon doped PDMS (cPDMS), has been used as a conductive polymer for stretchable electronics. Compared to liquid metals, cPDMS is low cost and is easier to process or to print with an additive manufacturing process. However, changes on the conductance of the carbon based conductive PDMS (cPDMS) were observed over time, in particular after integration of cPDMS and the insulating polymer. In this article we investigate the process parameters that lead to improved stability over conductance of the cPDMS over time. Slight modifications to the fabrication process parameters were conducted and changes on the conductance of the samples for each method were monitored. Results suggested that change of the conductance happens mostly after integration of a pre-polymer over a cured cPDMS, and not after integration of the cPDMS over a cured insulating polymer. We show that such changes can be eliminated by adjusting the integration priority between the conductive and insulating polymers, by selecting the right curing temperature, changing the concentration of the carbon particles and the thickness of the conductive traces, and when possible by changing the insulating polymer material. In this way, we obtained important conclusions regarding the effect of these parameters on the change of the conductance over time, that should be considered for additive manufacturing of soft electronics. Also, we show that these changes can be possibly due to the diffusion from PDMS into cPDMS.

Effect of nitrogen plasma afterglow on the surface charge effect resulted during XPS surface analysis of amorphous carbon nitride thin films

NASA Astrophysics Data System (ADS)

Kayed, Kamal

2018-06-01

The aim of this paper is to investigate the relationship between the micro structure and the surface charge effect resulted during XPS surface analysis of amorphous carbon nitride thin films prepared by laser ablation method. The study results show that the charge effect coefficient (E) is not just a correction factor. We found that the changes in this coefficient value due to incorporation of nitrogen atoms into the carbon network are related to the spatial configurations of the sp2 bonded carbon atoms, order degree and sp2 clusters size. In addition, results show that the curve E vs. C(sp3)-N is a characteristic curve of the micro structure. This means that using this curve makes it easy to sorting the samples according to the micro structure (hexagonal rings or chains).

CARd-3D: Carbon Distribution in 3D Structure Program for Globular Proteins

PubMed Central

Ekambaram, Rajasekaran; Kannaiyan, Akila; Marimuthu, Vijayasarathy; Swaminathan, Vinobha Chinnaiah; Renganathan, Senthil; Perumal, Ananda Gopu

2014-01-01

Spatial arrangement of carbon in protein structure is analyzed here. Particularly, the carbon fractions around individual atoms are compared. It is hoped that it follows the principle of 31.45% carbon around individual atoms. The results reveal that globular protein's atoms follow this principle. A comparative study on monomer versus dimer reveal that carbon is better distributed in dimeric form than in its monomeric form. Similar study on solid versus liquid structures reveals that the liquid (NMR) structure has better carbon distribution over the corresponding solid (X-Ray) structure. The carbon fraction distributions in fiber and toxin protein are compared. Fiber proteins follow the principle of carbon fraction distribution. At the same time it has another broad spectrum of carbon distribution than in globular proteins. The toxin protein follows an abnormal carbon fraction distribution. The carbon fraction distribution plays an important role in deciding the structure and shape of proteins. It is hoped to help in understanding the protein folding and function. PMID:24748753

High voltage electrochemical double layer capacitors using conductive carbons as additives

NASA Astrophysics Data System (ADS)

Michael, M. S.; Prabaharan, S. R. S.

We describe here an interesting approach towards electrochemical capacitors (ECCs) using graphite materials (as being used as conductive additives in rechargeable lithium-ion battery cathodes) in a Li + containing organic electrolyte. The important result is that we achieved a voltage window of >4 V, which is rather large, compared to the standard window of 2.5 V for ordinary electric double layer capacitors (DLCs). The capacitor performance was evaluated by cyclic voltammetry (CV) and galvanostatic charge/discharge techniques. From charge-discharge studies of the symmetrical device (for instance, SFG6 carbon electrode), a specific capacitance of up to 14.5 F/g was obtained at 16 mA/cm 2 current rate and at a low current rate (3 mA/cm 2), a higher value was obtained (63 F/g). The specific capacitance decreased about 25% after 1000 cycles compared to the initial discharge process. The performances of these graphites are discussed in the light of both double layer capacitance (DLC) and pseudocapacitance (battery-like behavior). The high capacitance obtained was not only derived from the current-transient capacitive behavior but is also attributed to pseudocapacitance associated with some kind of faradaic reaction, which could probably occur due to Li + intercalation/deintercalation reactions into graphitic layers of the carbons used. The ac impedance (electrochemical impedances spectroscopy, EIS) measurements were also carried out to evaluate the capacitor parameters such as equivalent series resistance (ESR) and frequency dependent capacitance ( Cfreq). Cyclic voltammetry measurements were also performed to evaluate the cycling behavior of the carbon electrodes and the non-rectangular shaped voltammograms revealed the non-zero time constant [ τ( RC)≠0] confirming that the current contains a transient as well as steady-state components.

Carbon Nanotube/Conductive Additive/Space Durable Polymer Nanocomposite Films for Electrostatic Charge Dissipation

NASA Technical Reports Server (NTRS)

Smith, Joseph G., Jr.; Watson, Kent A.; Delozier, Donavon M.; Connell, John W.

2003-01-01

Thin film membranes of space environmentally stable polymeric materials possessing low color/solar absorptivity (alpha) are of interest for potential applications on Gossamer spacecraft. In addition to these properties, sufficient electrical conductivity is required in order to dissipate electrostatic charge (ESC) build-up brought about by the charged orbital environment. One approach to achieve sufficient electrical conductivity for ESC mitigation is the incorporation of single wall carbon nanotubes (SWNTs). However, when the SWNTs are dispersed throughout the polymer matrix, the nanocomposite films tend to be significantly darker than the pristine material resulting in a higher alpha. The incorporation of conductive additives in combination with a decreased loading level of SWNTs is one approach for improving alpha while retaining conductivity. Taken individually, the low loading level of conductive additives and SWNTs is insufficient in achieving the percolation level necessary for electrical conductivity. When added simultaneously to the film, conductivity is achieved through a synergistic effect. The chemistry, physical, and mechanical properties of the nanocomposite films will be presented.

Absorption properties of carbon dioxide enhanced-oil-recovery additives. Final Technical report, 12 May 1987-31 August 1989

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

Patton, J.T.; Holbrook, S.T.

1990-01-01

The selection of the optimum foaming agent (surfactant) for enhancing oil production by carbon dioxide flooding is based on foamability and adsorption. Measurement of adsorption on carbonate cores from New Mexico reservoirs showed large adsorption differences between three commercial, high-foaming surfactants. An ethoxylated alcohol structure was least adsorbed, 0.64 mg/cc pore volume; an ethoxylated alcohol sulfate was next, 0.74 mg/cc pore volume; the highest adsorbed was a glyceryl sulfonate, 2.30 mg/cc pore volume. Commercial application of the foaming additive involves injecting alternate slugs of surfactant solution and carbon dioxide. Surfactant concentration should be determined to allow for the adsorption above.

Surface Roughness of Various Diamond-Like Carbon Films

NASA Astrophysics Data System (ADS)

Liu, Dongping; Liu, Yanhong; Chen, Baoxiang

2006-11-01

Atomic force microscopy is used to estimate and compare the surface morphology of hydrogenated and hydrogen-free diamond-like carbon (DLC) films. The films were prepared by using DC magnetron sputtering of a graphite target, pulsed cathodic carbon arcs, electron cyclotron resonance (ECR), plasma source ion implantation and dielectric barrier discharge (DBD). The difference in the surface structure is presented for each method of deposition. The influences of various discharge parameters on the film surface properties are discussed based upon the experimental results. The coalescence process via the diffusion of adsorbed carbon species is responsible for the formation of hydrogen-free DLC films with rough surfaces. The films with surface roughness at an atomic level can be deposited by energetic ion impacts in a highly ionized carbon plasma. The dangling bonds created by atomic hydrogen lead to the uniform growth of hydrocarbon species at the a-C:H film surfaces of the ECR or DBD plasmas.

Atomic switches: atomic-movement-controlled nanodevices for new types of computing

PubMed Central

Hino, Takami; Hasegawa, Tsuyoshi; Terabe, Kazuya; Tsuruoka, Tohru; Nayak, Alpana; Ohno, Takeo; Aono, Masakazu

2011-01-01

Atomic switches are nanoionic devices that control the diffusion of metal cations and their reduction/oxidation processes in the switching operation to form/annihilate a metal atomic bridge, which is a conductive path between two electrodes in the on-state. In contrast to conventional semiconductor devices, atomic switches can provide a highly conductive channel even if their size is of nanometer order. In addition to their small size and low on-resistance, their nonvolatility has enabled the development of new types of programmable devices, which may achieve all the required functions on a single chip. Three-terminal atomic switches have also been developed, in which the formation and annihilation of a metal atomic bridge between a source electrode and a drain electrode are controlled by a third (gate) electrode. Three-terminal atomic switches are expected to enhance the development of new types of logic circuits, such as nonvolatile logic. The recent development of atomic switches that use a metal oxide as the ionic conductive material has enabled the integration of atomic switches with complementary metal-oxide-semiconductor (CMOS) devices, which will facilitate the commercialization of atomic switches. The novel characteristics of atomic switches, such as their learning and photosensing abilities, are also introduced in the latter part of this review. PMID:27877376

Atomic Oxygen Treatment as a Method of Recovering Smoke Damaged Paintings

NASA Technical Reports Server (NTRS)

Rutledge, Sharon K.; Banks, Bruce A.; Forkapa, Mark; Stueber, Thomas; Sechkar, Edward; Malinowski, Kevin

1998-01-01

Smoke damage, as a result of a fire, can be difficult to remove from some types of painting media without causing swelling, leaching or pigment movement or removal. A non-contact technique has been developed which can remove soot from the surface of a painting by use of a gently flowing gas containing atomic oxygen. The atomic oxygen chemically reacts with the soot on the surface creating gasses such as carbon monoxide and carbon dioxide which can be removed through the use of an exhaust system. The reaction is limited to the surface so that the process can be timed to stop when the paint layer is reached. Atomic oxygen is a primary component of the low Earth orbital environment, but can be generated on Earth through various methods. This paper will discuss the results of atomic oxygen treatment of soot exposed acrylic gesso, ink on paper, and a varnished oil painting. Reflectance measurements were used to characterize the surfaces before and after treatment.

Changes in soil carbon and nutrients following 6 years of litter removal and addition in a tropical semi-evergreen rain forest

NASA Astrophysics Data System (ADS)

Tanner, Edmund Vincent John; Sheldrake, Merlin W. A.; Turner, Benjamin L.

2016-11-01

Increasing atmospheric CO2 and temperature may increase forest productivity, including litterfall, but the consequences for soil organic matter remain poorly understood. To address this, we measured soil carbon and nutrient concentrations at nine depths to 2 m after 6 years of continuous litter removal and litter addition in a semi-evergreen rain forest in Panama. Soils in litter addition plots, compared to litter removal plots, had higher pH and contained greater concentrations of KCl-extractable nitrate (both to 30 cm); Mehlich-III extractable phosphorus and total carbon (both to 20 cm); total nitrogen (to 15 cm); Mehlich-III calcium (to 10 cm); and Mehlich-III magnesium and lower bulk density (both to 5 cm). In contrast, litter manipulation did not affect ammonium, manganese, potassium or zinc, and soils deeper than 30 cm did not differ for any nutrient. Comparison with previous analyses in the experiment indicates that the effect of litter manipulation on nutrient concentrations and the depth to which the effects are significant are increasing with time. To allow for changes in bulk density in calculation of changes in carbon stocks, we standardized total carbon and nitrogen on the basis of a constant mineral mass. For 200 kg m-2 of mineral soil (approximately the upper 20 cm of the profile) about 0.5 kg C m-2 was "missing" from the litter removal plots, with a similar amount accumulated in the litter addition plots. There was an additional 0.4 kg C m-2 extra in the litter standing crop of the litter addition plots compared to the control. This increase in carbon in surface soil and the litter standing crop can be interpreted as a potential partial mitigation of the effects of increasing CO2 concentrations in the atmosphere.

Molecules Without Atoms

NASA Astrophysics Data System (ADS)

Ruth, Anthony; Collins, Laura; Gomes, Kenjiro; Janko, Boldizsar

We present a real-space representation of molecules which results in the normal bonding rules and electronic structure of chemistry without atom-centered coulomb potentials. Using a simple mapping, we can generate atomless molecules from the structure of real molecules. Additionally, molecules without atoms show similar covalent bonding energies and transfer of charge in ionic bonds as real molecules. The atomless molecules contain only the valence and conduction electronic structure of the real molecule. Using the framework of the Atoms in Molecules (AIM) theory of Bader, we prove that the topological features of the valence charge distribution of molecules without atoms are identical to that of real molecules. In particular, the charge basins of atomless molecules show identical location and quantities of representative charge. We compare the accuracy, computational cost, and intuition gained from electronic structure calculations of molecules without atoms with the use of pseudopotentials to represent atomic cores in density functional theory. A. R. acknowledges support from a NASA Space Technology Research Fellowship.

Spectroscopy and formation of lanthanum-hydrocarbon radicals formed by association and carbon-carbon bond cleavage of isoprene

NASA Astrophysics Data System (ADS)

Cao, Wenjin; Hewage, Dilrukshi; Yang, Dong-Sheng

2018-05-01

La atom reaction with isoprene is carried out in a laser-vaporization molecular beam source. The reaction yields an adduct as the major product and C—C cleaved and dehydrogenated species as the minor ones. La(C5H8), La(C2H2), and La(C3H4) are characterized with mass-analyzed threshold ionization (MATI) spectroscopy and quantum chemical computations. The MATI spectra of all three species exhibit a strong origin band and several weak vibronic bands corresponding to La-ligand stretch and ligand-based bend excitations. La(C5H8) is a five-membered metallacycle, whereas La(C2H2) and La(C3H4) are three-membered rings. All three metallacycles prefer a doublet ground state with a La 6s1-based valence electron configuration and a singlet ion. The five-membered metallacycle is formed through La addition and isoprene isomerization, whereas the two three-membered rings are produced by La addition and insertion, hydrogen migration, and carbon-carbon bond cleavage.

Technical note: Relating functional group measurements to carbon types for improved model-measurement comparisons of organic aerosol composition

NASA Astrophysics Data System (ADS)

Takahama, Satoshi; Ruggeri, Giulia

2017-04-01

Functional group (FG) analysis provides a means by which functionalization in organic aerosol can be attributed to the abundances of its underlying molecular structures. However, performing this attribution requires additional, unobserved details about the molecular mixture to provide constraints in the estimation process. We present an approach for conceptualizing FG measurements of organic aerosol in terms of its functionalized carbon atoms. This reformulation facilitates estimation of mass recovery and biases in popular carbon-centric metrics that describe the extent of functionalization (such as oxygen to carbon ratio, organic mass to organic carbon mass ratio, and mean carbon oxidation state) for any given set of molecules and FGs analyzed. Furthermore, this approach allows development of parameterizations to more precisely estimate the organic carbon content from measured FG abundance. We use simulated photooxidation products of α-pinene secondary organic aerosol previously reported by Ruggeri et al. (2016) and FG measurements by Fourier transform infrared (FT-IR) spectroscopy in chamber experiments by Sax et al. (2005) to infer the relationships among molecular composition, FG composition, and metrics of organic aerosol functionalization. We find that for this simulated system, ˜ 80 % of the carbon atoms should be detected by FGs for which calibration models are commonly developed, and ˜ 7 % of the carbon atoms are undetectable by FT-IR analysis because they are not associated with vibrational modes in the infrared. Estimated biases due to undetected carbon fraction for these simulations are used to make adjustments in these carbon-centric metrics such that model-measurement differences are framed in terms of unmeasured heteroatoms (e.g., in hydroperoxide and nitrate groups for the case studied in this demonstration). The formality of this method provides framework for extending FG analysis to not only model-measurement but also instrument

Matrix modification with silver for the electrothermal atomization of arsenic and selenium

USGS Publications Warehouse

Sanzolone, R.F.; Chao, T.T.

1981-01-01

Silver as a matrix modifier is shown to improve the carbon-rod atomization of both arsenic and selenium for atomic absorption spectrometry. Compared to nickel, the efficiency of silver is greater for arsenic and about the same for selenium. Silver fulfils two functions in its reaction, namely stabilization during the ashing stage and enhancement of absorbance in the final atomization. ?? 1981.

A voltammetric determination of caffeic acid in red wines based on the nitrogen doped carbon modified glassy carbon electrode.

PubMed

Karikalan, Natarajan; Karthik, Raj; Chen, Shen-Ming; Chen, Hsi-An

2017-04-05

We reported an electrochemical determination of caffeic acid (CA) based on the nitrogen doped carbon (NDC). The described sensor material was prepared by the flame synthesis method, which gave an excellent platform for the synthesis of carbon nanomaterials with the hetero atom dopant. The synthesized material was confirmed by various physical characterizations and it was further characterized by different electrochemical experiments. The NDC modified glassy carbon electrode (NDC/GCE) shows the superior electrocatalytic performance towards the determination of CA with the wide linear concentration range from 0.01 to 350 μM. It achieves the lowest detection limit of 0.0024 μM and the limit of quantification of 0.004 μM. The NDC/GCE-CA sensor reveals the good selectivity, stability, sensitivity and reproducibility which endorsed that the NDC is promising electrode for the determination of CA. In addition, NDC modified electrode is applied to the determination of CA in red wines and acquired good results.

Use of Atomic Fuels for Rocket-Powered Launch Vehicles Analyzed

NASA Technical Reports Server (NTRS)

Palaszewski, Bryan A.

1999-01-01

At the NASA Lewis Research Center, the launch vehicle gross lift-off weight (GLOW) was analyzed for solid particle feed systems that use high-energy density atomic propellants (ref. 1). The analyses covered several propellant combinations, including atoms of aluminum, boron, carbon, and hydrogen stored in a solid cryogenic particle, with a cryogenic liquid as the carrier fluid. Several different weight percents for the liquid carrier were investigated, and the GLOW values of vehicles using the solid particle feed systems were compared with that of a conventional oxygen/hydrogen (O2/H2) propellant vehicle. Atomic propellants, such as boron, carbon, and hydrogen, have an enormous potential for high specific impulse Isp operation, and their pursuit has been a topic of great interest for decades. Recent and continuing advances in the understanding of matter, the development of new technologies for simulating matter at its most basic level, and manipulations of matter through microtechnology and nanotechnology will no doubt create a bright future for atomic propellants and an exciting one for the researchers exploring this technology.

Capturing Gases in Carbon Honeycomb

NASA Astrophysics Data System (ADS)

Krainyukova, Nina V.

2017-04-01

In our recent paper (Krainyukova and Zubarev in Phys Rev Lett 116:055501, 2016. doi: 10.1103/PhysRevLett.116.055501) we reported the observation of an exceptionally stable honeycomb carbon allotrope obtained by deposition of vacuum-sublimated graphite. A family of structures can be built from absolutely dominant {sp}2-bonded carbon atoms, and may be considered as three-dimensional graphene. Such structures demonstrate high absorption capacity for gases and liquids. In this work we show that the formation of honeycomb structures is highly sensitive to the carbon evaporation temperature and deposition rates. Both parameters are controlled by the electric current flowing through thin carbon rods. Two distinctly different regimes were found. At lower electric currents almost pure honeycomb structures form owing to sublimation. At higher currents the surface-to-bulk rod melting is observed. In the latter case densification of the carbon structures and a large contribution of glassy graphite emerge. The experimental diffraction patterns from honeycomb structures filled with absorbed gases and analyzed by the advanced method are consistent with the proposed models for composites which are different for Ar, Kr and Xe atoms in carbon matrices.

Quantitative assessment of carbon allocation anomalies in low temperature bainite

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

Rementeria, Rosalia

Low temperature bainite is a mixture of ferrite and austenite with a high dislocation density and nanoscale precipitates produced by isothermal transformation of the austenite in high-carbon high-silicon steels. The mass balance for carbon is systematically unsuitable when considering only ferrite and austenite forming the structure, but no attempt has been made to evaluate the amount of carbon located at linear defects and precipitates. Additionally, bainitic ferrite has been recently shown to have a tetragonal crystal structure, allowing greater amounts of carbon in solid solution than those expected by the paraequilibrium phase boundaries. In order to quantify the contribution ofmore » all the carbon sinks, we have followed the evolution of carbon in ferrite and austenite, along with the precipitation of cementite and η–carbide, during the isothermal bainitic transformation at 220 and 250 °C by means of in-situ synchrotron high energy X-ray diffraction and complementary transmission electron microscopy (TEM) and atom probe tomography (APT) analyses. Furthermore, this is the first time that the mass balance for carbon is successfully achieved by considering all the transformation products together with an estimation of the carbon segregated to linear defects.« less

Quantitative assessment of carbon allocation anomalies in low temperature bainite

DOE PAGES

Rementeria, Rosalia

2017-05-24

Low temperature bainite is a mixture of ferrite and austenite with a high dislocation density and nanoscale precipitates produced by isothermal transformation of the austenite in high-carbon high-silicon steels. The mass balance for carbon is systematically unsuitable when considering only ferrite and austenite forming the structure, but no attempt has been made to evaluate the amount of carbon located at linear defects and precipitates. Additionally, bainitic ferrite has been recently shown to have a tetragonal crystal structure, allowing greater amounts of carbon in solid solution than those expected by the paraequilibrium phase boundaries. In order to quantify the contribution ofmore » all the carbon sinks, we have followed the evolution of carbon in ferrite and austenite, along with the precipitation of cementite and η–carbide, during the isothermal bainitic transformation at 220 and 250 °C by means of in-situ synchrotron high energy X-ray diffraction and complementary transmission electron microscopy (TEM) and atom probe tomography (APT) analyses. Furthermore, this is the first time that the mass balance for carbon is successfully achieved by considering all the transformation products together with an estimation of the carbon segregated to linear defects.« less

Massive carbon addition to an organic-rich Andosol increased the subsoil but not the topsoil carbon stock

NASA Astrophysics Data System (ADS)

Zieger, Antonia; Kaiser, Klaus; Ríos Guayasamín, Pedro; Kaupenjohann, Martin

2018-05-01

Andosols are among the most carbon-rich soils, with an average of 254 Mg ha-1 organic carbon (OC) in the upper 100 cm. A current theory proposes an upper limit for OC stocks independent of increasing carbon input, because of finite binding capacities of the soil mineral phase. We tested the possible limits in OC stocks for Andosols with already large OC concentrations and stocks (212 g kg-1 in the first horizon, 301 Mg ha-1 in the upper 100 cm). The soils received large inputs of 1800 Mg OC ha-1 as sawdust within a time period of 20 years. Adjacent soils without sawdust application served as controls. We determined total OC stocks as well as the storage forms of organic matter (OM) of five horizons down to 100 cm depth. Storage forms considered were pyrogenic carbon, OM of < 1.6 g cm-3 density and with little to no interaction with the mineral phase, and strongly mineral-bonded OM forming particles of densities between 1.6 and 2.0 g cm-3 or > 2.0 g cm-3. The two fractions > 1.6 g cm-3 were also analysed for aluminium-organic matter complexes (Al-OM complexes) and imogolite-type phases using ammonium-oxalate-oxalic-acid extraction and X-ray diffraction (XRD). Pyrogenic organic carbon represented only up to 5 wt % of OC, and thus contributed little to soil OM. In the two topsoil horizons, the fraction between 1.6 and 2.0 g cm-3 had 65-86 wt % of bulk soil OC and was dominated by Al-OM complexes. In deeper horizons, the fraction > 2.0 g cm-3 contained 80-97 wt % of the bulk soil's total OC and was characterized by a mixture of Al-OM complexes and imogolite-type phases, with proportions of imogolite-type phases increasing with depth. In response to the sawdust application, only the OC stock at 25-50 cm depth increased significantly (α = 0.05, 1 - β = 0.8). The increase was entirely due to increased OC in the two fractions > 1.6 g cm-3. However, there was no significant increase in the total OC stocks within the upper 100 cm. The results suggest that long-term large

Influence of oxygen on growth of carbon thin films

NASA Astrophysics Data System (ADS)

Kumar, Prabhat; Gupta, Mukul; Phase, D. M.; Stahn, Jochen

2018-04-01

In this work we studied the influence of oxygen gas on growth of carbon thin films in a magnetron sputtering process. X-ray absorption spectroscopy (XAS), x-ray and neutron reflectivity techniques were used to probe carbon thin films deposited with and without oxygen at room temperature. XAS in particularly x-ray absorption near edge spectroscopy (XANES) is powerful technique to identify the nature of hybridization of carbon atoms with other elements. In a XANES pattern, presence of C=O and C-O bonds is generally observed in spite of the fact that oxygen has not been deliberately included in the growth process. In order to confirm the presence of such features, we introduced a small amount of oxygen at 1% during the growth of carbon thin films. Though such additions do not affect the number density as observed by x-ray and neutron reflectivity, they severally affect the C K-edge spectra as evidenced by an enhancement in carbon-oxygen hybridization. Observed results are helpful in analyzing the C K-edge spectra more confidently.

[Responses of soil organic carbon and its labile fractions to nitrogen and phosphorus additions in Cunninghamia lanceolata plantations in subtropical China.

PubMed

Zhang, Xiu Lan; Wang, Fang Chao; Fang, Xiang Min; He, Ping; Zhang, Yu Fei; Chen, Fu Sheng; Wang, Hui Min

2017-02-01

A series of nitrogen (N) and phosphorus (P) addition experiments using treatments of N 0 (0 kg N·hm -2 ·a -1 ), N 1 (50 kg N·hm -2 ·a -1 ), N 2 (100 kg N·hm -2 ·a -1 ), P (50 kg P·hm -2 ·a -1 ), N 1 P and N 2 P were conducted at Cunninghamia lanceolata plantations in subtropical China. The responses of soil organic carbon (SOC), particulate organic carbon (POC) and water-soluble organic carbon (WSOC) to the nutrient addition treatments after 3 years were determined. The results showed that N and P additions had no significant effects on SOC concentration in 0-20 cm soil layer, while P addition significantly decreased soil POC content in 0-5 cm soil layer by 26.1%. The responses of WSOC to N and P addition were mainly found in 0-5 cm soil layer, and low level N and P addition significantly increased the WSOC content in 0-5 cm soil layer. Nitrogen addition had no significant effect on POC/SOC, while the POC/SOC significantly decreased by 15.9% in response to P addition in 0-5 cm soil layer. In 5-10 cm and 10-20 cm soil layers, POC/SOC was not significantly altered in N and P addition treatments. Therefore, the forest soil C stability was mainly controlled by P content in subtropical areas. P addition was liable to cause the decomposition of surface soil active organic C and increased the soil C stability in the short term treatment.

Four- and eight-membered rings carbon nanotubes: A new class of carbon nanomaterials

NASA Astrophysics Data System (ADS)

Li, Fangfang; Lu, Junzhe; Zhu, Hengjiang; Lin, Xiang

2018-06-01

A new class of carbon nanomaterials composed of alternating four- and eight-membered rings is studied by density functional theory (DFT), including single-walled carbon nanotubes (SWCNTs) double-walled carbon nanotubes (DWCNTs) and triple-walled CNTs (TWCNTs). The analysis of geometrical structure shows that carbon atoms' hybridization in novel carbon tubular clusters (CTCs) and the corresponding carbon nanotubes (CNTs) are both sp2 hybridization; The thermal properties exhibit the high stability of these new CTCs. The results of energy band and density of state (DOS) indicate that the electronic properties of CNTs are independent of their diameter, number of walls and chirality, exhibit obvious metal properties.

Shock-tube measurements of carbon to oxygen atom ratios for incipient soot formation with C2H2, C2H4 and C2H6 fuels

NASA Technical Reports Server (NTRS)

Radcliffe, S. W.; Appleton, J. P.

1971-01-01

The critical atomic carbon to oxygen ratios, Phi sub C, for incipient soot formation in shock heated acetylene, ethylene, ethane/oxygen/ argon mixtures was measured over the temperature range 2000 K to 2500 K for reactant partial pressures between 0.1 and 0.4 atoms. Absorption of light from a He-Ne laser at 6328A was was used to detect soot. It was observed that the values of Phi sub C for all three fuels increased uniformly with temperature such that at the highest temperatures Phi sub C was considerably greater than unity, i.e. greater than the value of about unity at which solid carbon should have been precipitated on a thermochemical equilibrium basis. Observations were made over periods extending up to about one millisecond, which was well in excess of the time required for the major heat release of the combustion reactions. The relevance of these experimental findings to the problem of soot formation in gas turbine combustion chambers is discussed.

Carbon Fibers Conductivity Studies

NASA Technical Reports Server (NTRS)

Yang, C. Y.; Butkus, A. M.

1980-01-01

In an attempt to understand the process of electrical conduction in polyacrylonitrile (PAN)-based carbon fibers, calculations were carried out on cluster models of the fiber consisting of carbon, nitrogen, and hydrogen atoms using the modified intermediate neglect of differential overlap (MINDO) molecular orbital (MO) method. The models were developed based on the assumption that PAN carbon fibers obtained with heat treatment temperatures (HTT) below 1000 C retain nitrogen in a graphite-like lattice. For clusters modeling an edge nitrogen site, analysis of the occupied MO's indicated an electron distribution similar to that of graphite. A similar analysis for the somewhat less stable interior nitrogen site revealed a partially localized II electron distribution around the nitrogen atom. The differences in bonding trends and structural stability between edge and interior nitrogen clusters led to a two-step process proposed for nitrogen evolution with increasing HTT.

Atomic layer deposition of ruthenium on plasma-treated vertically aligned carbon nanotubes for high-performance ultracapacitors.

PubMed

Kim, Jun Woo; Kim, Byungwoo; Park, Suk Won; Kim, Woong; Shim, Joon Hyung

2014-10-31

It is challenging to realize a conformal metal coating by atomic layer deposition (ALD) because of the high surface energy of metals. In this study, ALD of ruthenium (Ru) on vertically aligned carbon nanotubes (CNTs) was carried out. To activate the surface of CNTs that lack surface functional groups essential for ALD, oxygen plasma was applied ex situ before ALD. X-ray photoelectron spectroscopy and Raman spectroscopy confirmed surface activation of CNTs by the plasma pretreatment. Transmission electron microscopy analysis with energy-dispersive x-ray spectroscopy composition mapping showed that ALD Ru grew conformally along CNTs walls. ALD Ru/CNTs were electrochemically oxidized to ruthenium oxide (RuOx) that can be a potentially useful candidate for use in the electrodes of ultracapacitors. Electrode performance of RuOx/CNTs was evaluated using cyclic voltammetry and galvanostatic charge-discharge measurements.

Integrating Carbon Nanotubes For Atomic Force Microscopy Imaging Applications

NASA Technical Reports Server (NTRS)

Ye, Qi; Cassell, Alan M.; Liu, Hongbing; Han, Jie; Meyyappan, Meyya

2004-01-01

Carbon nanotube (CNT) related nanostructures possess remarkable electrical, mechanical, and thermal properties. To produce these nanostructures for real world applications, a large-scale controlled growth of carbon nanotubes is crucial for the integration and fabrication of nanodevices and nanosensors. We have taken the approach of integrating nanopatterning and nanomaterials synthesis with traditional silicon micro fabrication techniques. This integration requires a catalyst or nanomaterial protection scheme. In this paper, we report our recent work on fabricating wafer-scale carbon nanotube AFM cantilever probe tips. We will address the design and fabrication considerations in detail, and present the preliminary scanning probe test results. This work may serve as an example of rational design, fabrication, and integration of nanomaterials for advanced nanodevice and nanosensor applications.

Charcoal addition to soils in NE England: a carbon sink with environmental co-benefits?

PubMed

Bell, M J; Worrall, F

2011-04-01

Interest in the application of biochar (charcoal produced during the pyrolysis of biomass) to agricultural land is increasing across the world, recognised as a potential way to capture and store atmospheric carbon. Its interest is heightened by its potential co-benefits for soil quality and fertility. The majority of research has however been undertaken in tropical rather than temperate regions. This study assessed the potential for lump-wood charcoal addition (as a substitute for biochar) to soil types which are typically under arable and forest land-use in North East England. The study was undertaken over a 28 week period and found: i) No significant difference in net ecosystem respiration (NER) between soils containing charcoal and those without, other than in week 1 of the trial. ii) A significantly higher dissolved organic carbon (DOC) flux from soils containing large amounts of charcoal than from those untreated, when planted with ryegrass. iii) That when increased respiration or DOC loss did occur, neither was sufficiently large to alter the carbon sink benefits of charcoal application. iv) That charcoal incorporation resulted in a significantly lower nitrate flux in soil leachate from mineral soils. v) That charcoal incorporation caused significant increases in soil pH, from 6.98 to 7.22 on bare arable soils when 87,500 kg charcoal/ha was applied. Consideration of both the carbon sink and environmental benefits observed here suggests that charcoal application to temperate soils typical of North East England should be considered as a method of carbon sequestration. Before large scale land application is encouraged, further large scale trials should be undertaken to confirm the positive results of this research. Copyright © 2011 Elsevier B.V. All rights reserved.

Improved Process for Fabricating Carbon Nanotube Probes

NASA Technical Reports Server (NTRS)

Stevens, R.; Nguyen, C.; Cassell, A.; Delzeit, L.; Meyyappan, M.; Han, Jie

2003-01-01

An improved process has been developed for the efficient fabrication of carbon nanotube probes for use in atomic-force microscopes (AFMs) and nanomanipulators. Relative to prior nanotube tip production processes, this process offers advantages in alignment of the nanotube on the cantilever and stability of the nanotube's attachment. A procedure has also been developed at Ames that effectively sharpens the multiwalled nanotube, which improves the resolution of the multiwalled nanotube probes and, combined with the greater stability of multiwalled nanotube probes, increases the effective resolution of these probes, making them comparable in resolution to single-walled carbon nanotube probes. The robust attachment derived from this improved fabrication method and the natural strength and resiliency of the nanotube itself produces an AFM probe with an extremely long imaging lifetime. In a longevity test, a nanotube tip imaged a silicon nitride surface for 15 hours without measurable loss of resolution. In contrast, the resolution of conventional silicon probes noticeably begins to degrade within minutes. These carbon nanotube probes have many possible applications in the semiconductor industry, particularly as devices are approaching the nanometer scale and new atomic layer deposition techniques necessitate a higher resolution characterization technique. Previously at Ames, the use of nanotube probes has been demonstrated for imaging photoresist patterns with high aspect ratio. In addition, these tips have been used to analyze Mars simulant dust grains, extremophile protein crystals, and DNA structure.

Performance-Enhanced Activated Carbon Electrodes for Supercapacitors Combining Both Graphene-Modified Current Collectors and Graphene Conductive Additive

PubMed Central

Wang, Rubing; Qian, Yuting; Li, Weiwei; Zhu, Shoupu; Liu, Fengkui; Guo, Yufen; Chen, Mingliang; Li, Qi; Liu, Liwei

2018-01-01

Graphene has been widely used in the active material, conductive agent, binder or current collector for supercapacitors, due to its large specific surface area, high conductivity, and electron mobility. However, works simultaneously employing graphene as conductive agent and current collector were rarely reported. Here, we report improved activated carbon (AC) electrodes (AC@G@NiF/G) simultaneously combining chemical vapor deposition (CVD) graphene-modified nickel foams (NiF/Gs) current collectors and high quality few-layer graphene conductive additive instead of carbon black (CB). The synergistic effect of NiF/Gs and graphene additive makes the performances of AC@G@NiF/G electrodes superior to those of electrodes with CB or with nickel foam current collectors. The performances of AC@G@NiF/G electrodes show that for the few-layer graphene addition exists an optimum value around 5 wt %, rather than a larger addition of graphene, works out better. A symmetric supercapacitor assembled by AC@G@NiF/G electrodes exhibits excellent cycling stability. We attribute improved performances to graphene-enhanced conductivity of electrode materials and NiF/Gs with 3D graphene conductive network and lower oxidation, largely improving the electrical contact between active materials and current collectors. PMID:29762528

Performance-Enhanced Activated Carbon Electrodes for Supercapacitors Combining Both Graphene-Modified Current Collectors and Graphene Conductive Additive.

PubMed

Wang, Rubing; Qian, Yuting; Li, Weiwei; Zhu, Shoupu; Liu, Fengkui; Guo, Yufen; Chen, Mingliang; Li, Qi; Liu, Liwei

2018-05-15

Graphene has been widely used in the active material, conductive agent, binder or current collector for supercapacitors, due to its large specific surface area, high conductivity, and electron mobility. However, works simultaneously employing graphene as conductive agent and current collector were rarely reported. Here, we report improved activated carbon (AC) electrodes (AC@G@NiF/G) simultaneously combining chemical vapor deposition (CVD) graphene-modified nickel foams (NiF/Gs) current collectors and high quality few-layer graphene conductive additive instead of carbon black (CB). The synergistic effect of NiF/Gs and graphene additive makes the performances of AC@G@NiF/G electrodes superior to those of electrodes with CB or with nickel foam current collectors. The performances of AC@G@NiF/G electrodes show that for the few-layer graphene addition exists an optimum value around 5 wt %, rather than a larger addition of graphene, works out better. A symmetric supercapacitor assembled by AC@G@NiF/G electrodes exhibits excellent cycling stability. We attribute improved performances to graphene-enhanced conductivity of electrode materials and NiF/Gs with 3D graphene conductive network and lower oxidation, largely improving the electrical contact between active materials and current collectors.

Low-temperature field ion microscopy of carbon nanotubes

NASA Astrophysics Data System (ADS)

Ksenofontov, V. A.; Gurin, V. A.; Gurin, I. V.; Kolosenko, V. V.; Mikhailovskij, I. M.; Sadanov, E. V.; Mazilova, T. I.; Velikodnaya, O. A.

2007-10-01

The methods of high-resolution field ion microscopy with sample cooling to liquid helium temperature are used in a study of the products of gas-phase catalytic pyrolysis of hydrocarbons in the form of graphitized fibers containing carbon nanotubes. Full atomic resolution of the end cap of closed carbon nanotubes is achieved for the first time. It is found that the atomic structure of the tops of the caps of subnanometer carbon tubes consists predominantly of hexagonal rings. A possible reason for the improvement of the resolution of field ion images of nanotubes upon deep cooling is discussed.

Down-to-earth studies of carbon clusters

NASA Technical Reports Server (NTRS)

Smalley, R. E.

1990-01-01

Recent advances in supersonic beam experiments with laser-vaporization sources of clusters have provided some interesting new insights into the nature of the small clusters of carbon, and the processes through which carbon condenses. One cluster in particular, C(sub 60), appears to play a central role. It is argued that this cluster takes the shape of a soccerball: a hollow sphere composed of a shell of 60 carbon atoms connected by a lattice of hexagonal and pentagonal rings, in a pattern of overall icosahedral symmetry. Although C(sub 60) appears to be uniquely stable due to its perfect symmetry, all other even-numbered carbon clusters in the 32 to 100+ atom size range seem to favor similar closed spheroidal forms. These species are interpreted as relatively unreactive side products in condensation reactions of carbon vapor involving spiraling graphitic sheets. The prevalence of C(sub 60) in laser-vaporized carbon vapors and sooting flames suggests that it may be formed readily whenever carbon condenses. Such ready formation and extraordinary stability may have substantial astrophysical implications.

Down-to-earth studies of carbon clusters

NASA Astrophysics Data System (ADS)

Smalley, R. E.

1990-04-01

Recent advances in supersonic beam experiments with laser-vaporization sources of clusters have provided some interesting new insights into the nature of the small clusters of carbon, and the processes through which carbon condenses. One cluster in particular, C60, appears to play a central role. It is argued that this cluster takes the shape of a soccer ball: a hollow sphere composed of a shell of 60 carbon atoms connected by a lattice of hexagonal and pentagonal rings, in a pattern of overall icosahedral symmetry. Although C60 appears to be uniquely stable due to its perfect symmetry, all other even-numbered carbon clusters in the 32 to 100+ atom size range seem to favor similar closed spheroidal forms. These species are interpreted as relatively unreactive side products in condensation reactions of carbon vapor involving spiraling graphitic sheets. The prevalence of C60 in laser-vaporized carbon vapors and sooting flames suggests that it may be formed readily whenever carbon condenses. Such ready formation and extraordinary stability may have substantial astrophysical implications.

EVALUATION OF CARBON BLACK SLURRIES AS CLEAN BURNING FUELS

EPA Science Inventory

Experiments were performed to examine the pumpability, atomization and combustion characteristics of slurries made of mixtures of carbon black with No. 2 fuel oil and methanol. Carbon black-No. 2 fuel oil and carbon black-methanol slurries, with carbon black contents of up to 50 ...

Picoampere Resistive Switching Characteristics Realized with Vertically Contacted Carbon Nanotube Atomic Force Microscope Probe

NASA Astrophysics Data System (ADS)

Nakano, Haruhisa; Takahashi, Makoto; Sato, Motonobu; Kotsugi, Masato; Ohkochi, Takuo; Muro, Takayuki; Nihei, Mizuhisa; Yokoyama, Naoki

2013-11-01

The resistive switching characteristics of a TiO2/Ti structure have been investigated using a conductive atomic force microscopy (AFM) system with 5-nm-diameter carbon nanotube (CNT) probes. The resistive switching showed bipolar resistive random access memory (ReRAM) behaviors with extremely low switching currents in the order of Picoamperes when voltages were applied. From transmission electron microscopy (TEM) observation, we confirmed that filament-like nanocrystals, having a diameter of about 10 nm, existed in TiO2 films at resistive switching areas after not only set operation but also reset operation. Moreover, photoemission electron microscopy (PEEM) analysis showed that the anatase-type TiO2 structure did not change after set and reset operations. From these results, we suggested that the Picoampere resistive switching occurred at the interface between the TiO2 dielectric and conductive nanocrystal without any structural changes in the TiO2 film and nanocrystal. The resistive switching mechanism we suggested is highly promising to realize extremely low-power-consumption ReRAMs with vertically contacted CNT electrodes.

Line splitting and modified atomic decay of atoms coupled with N quantized cavity modes

NASA Astrophysics Data System (ADS)

Zhu, Yifu

1992-05-01

We study the interaction of a two-level atom with N non-degenerate quantized cavity modes including dissipations from atomic decay and cavity damps. In the strong coupling regime, the absorption or emission spectrum of weakly excited atom-cavity system possesses N + 1 spectral peaks whose linewidths are the weighted averages of atomic and cavity linewidths. The coupled system shows subnatural (supernatural) atomic decay behavior if the photon loss rates from the N cavity modes are smaller (larger) than the atomic decay rate. If N cavity modes are degenerate, they can be treated effectively as a single mode. In addition, we present numerical calculations for N = 2 to characterize the system evolution from the weak coupling to strong coupling limits.

The effects of amine/nitro/hydroxyl groups on the benzene rings of redox additives on the electrochemical performance of carbon-based supercapacitors.

PubMed

Huang, Xuan; Wang, Qian; Chen, Xiang Ying; Zhang, Zhong Jie

2016-04-21

In this work, a series of porous carbon materials with hierarchical porosities have been synthesized via a template carbonization method, in which cheap CaCO3 serves as a template and glucose as a carbon precursor. During the carbonization process, CO2 produced by the decomposition of the CaCO3 template can act as an internal activating agent, significantly improving microporosity and mesoporosity. All the carbon materials obtained by regulating the ratio of glucose to CaCO3 exhibit the amorphous features with a low graphitization degree. Among them, the carbon-1 : 2 sample shows a high BET surface area of up to 818.5 m(2) g(-1) and a large total pore volume of 1.78 cm(3) g(-1) as well as a specific capacitance of 107.0 F g(-1) at 1 A g(-1). In addition, a series of hydroquinone (HQ), p-aminophenol (PAP) and p-nitrophenol (PNP) as novel redox additives that can produce pseudo-capacitances have been added into the KOH electrolyte for promoting the total capacitive performances via redox reactions at the electrode-electrolyte interface. As expected, a 2.5-fold increase in the galvanostatic capacitance of 240.0 F g(-1) in the HQ-0.5 electrolyte occurs, compared with the conventional KOH electrolyte. Similarly, the PAP-0.5 electrolyte and the PNP-0.5 electrolyte also show a high specific capacitance of 184.0 F g(-1) at 2 A g(-1) (156.6 F g(-1) at 3 A g(-1)) and 153.0 F g(-1) at 3 A g(-1), respectively. Additionally, the three kinds of electrolytes exhibit excellent cyclic stability. The remarkable improvement of supercapacitors is attributed to the quick reversible Faradaic reactions of amine and hydroxyl groups adhering to the phenyl rings, which largely accelerates electron migration and brings additional pseudocapacitive contribution for carbon-based supercapacitors.

Soil Microbial Community Responses to Additions of Organic Carbon Substrates and Heavy Metals (Pb and Cr)

PubMed Central

Nakatsu, Cindy H.; Carmosini, Nadia; Baldwin, Brett; Beasley, Federico; Kourtev, Peter; Konopka, Allan

2005-01-01

Microcosm experiments were conducted with soils contaminated with heavy metals (Pb and Cr) and aromatic hydrocarbons to determine the effects of each upon microbial community structure and function. Organic substrates were added as a driving force for change in the microbial community. Glucose represented an energy source used by a broad variety of bacteria, whereas fewer soil species were expected to use xylene. The metal amendments were chosen to inhibit the acute rate of organic mineralization by either 50% or 90%, and lower mineralization rates persisted over the entire 31-day incubation period. Significant biomass increases were abolished when metals were added in addition to organic carbon. The addition of organic carbon alone had the most significant impact on community composition and led to the proliferation of a few dominant phylotypes, as detected by PCR-denaturing gradient gel electrophoresis of bacterial 16S rRNA genes. However, the community-wide effects of heavy metal addition differed between the two carbon sources. For glucose, either Pb or Cr produced large changes and replacement with new phylotypes. In contrast, many phylotypes selected by xylene treatment were retained when either metal was added. Members of the Actinomycetales were very prevalent in microcosms with xylene and Cr(VI); gene copy numbers of biphenyl dioxygenase and phenol hydroxylase (but not other oxygenases) were elevated in these microcosms, as determined by real-time PCR. Much lower metal concentrations were needed to inhibit the catabolism of xylene than of glucose. Cr(VI) appeared to be reduced during the 31-day incubations, but in the case of glucose there was substantial microbial activity when much of the Cr(VI) remained. In the case of xylene, this was less clear. PMID:16332740

Site-selective covalent functionalization at interior carbon atoms and on the rim of circumtrindene, a C36H12 open geodesic polyarene

PubMed Central

Cho, Hee Yeon; Ansems, Ronald B M

2014-01-01

Summary Circumtrindene (6, C36H12), one of the largest open geodesic polyarenes ever reported, exhibits fullerene-like reactivity at its interior carbon atoms, whereas its edge carbons react like those of planar polycyclic aromatic hydrocarbons (PAHs). The Bingel–Hirsch and Prato reactions – two traditional methods for fullerene functionalization – afford derivatives of circumtrindene with one of the interior 6:6 C=C bonds modified. On the other hand, functionalization on the rim of circumtrindene can be achieved by normal electrophilic aromatic substitution, the most common reaction of planar PAHs. This peripheral functionalization has been used to extend the π-system of the polyarene by subsequent coupling reactions and to probe the magnetic environment of the concave/convex space around the hydrocarbon bowl. For both classes of functionalization, computational results are reported to complement the experimental observations. PMID:24991245

Determination of atomic positions from time resolved high resolution transmission electron microscopy images.

PubMed

Hussaini, Zahra; Lin, Pin Ann; Natarajan, Bharath; Zhu, Wenhui; Sharma, Renu

2018-03-01

For many reaction processes, such as catalysis, phase transformations, nanomaterial synthesis etc., nanoscale observations at high spatial (sub-nanometer) and temporal (millisecond) resolution are required to characterize and comprehend the underlying factors that favor one reaction over another. The combination of such spatial and temporal resolution (up to 600 µs), while rich in information, produces a large number of snapshots, each of which must be analyzed to obtain the structural (and thereby chemical) information. Here we present a methodology for automated quantitative measurement of real-time atomic position fluctuations in a nanoparticle. We leverage a combination of several image processing algorithms to precisely identify the positions of the atomic columns in each image. A geometric model is then used to measure the time-evolution of distances and angles between neighboring atomic columns to identify different phases and quantify local structural fluctuations. We apply this technique to determine the atomic-level fluctuations in the relative fractions of metal and metal-carbide phases in a cobalt catalyst nanoparticle during single-walled carbon nanotube (SWCNT) growth. These measurements provided a means to obtain the number of carbon atoms incorporated into and released from the catalyst particle, thereby helping resolve carbon reaction pathways during SWCNT growth. Further we demonstrate the use of this technique to measure the reaction kinetics of iron oxide reduction. Apart from reducing the data analysis time, the statistical approach allows us to measure atomic distances with sub-pixel resolution. We show that this method can be applied universally to measure atomic positions with a precision of 0.01 nm from any set of atomic-resolution video images. With the advent of high time-resolution direct detection cameras, we anticipate such methods will be essential in addressing the metrology problem of quantifying large datasets of time

3D hybrid carbon composed of multigraphene bridged by carbon chains

NASA Astrophysics Data System (ADS)

Liu, Lingyu; Hu, Meng; Liu, Chao; Shao, Cancan; Pan, Yilong; Ma, Mengdong; Wu, Yingju; Zhao, Zhisheng; Gao, Guoying; He, Julong

2018-01-01

The element carbon possesses various stable and metastable allotropes; some of them have been applied in diverse fields. The experimental evidences of both carbon chain and graphdiyne have been reported. Here, we reveal the mystery of an enchanting carbon allotrope with sp-, sp2-, and sp3-hybridized carbon atoms using a newly developed ab initio particle-swarm optimization algorithm for crystal structure prediction. This crystalline allotrope, namely m-C12, can be viewed as braided mesh architecture interwoven with multigraphene and carbon chains. The m-C12 meets the criteria for dynamic and mechanical stabilities and is energetically more stable than carbyne and graphdiyne. Analysis of the B/G and Poisson's ratio indicates that this allotrope is ductile. Notably, m-C12 is a superconducting carbon with Tc of 1.13 K, which is rare in the family of carbon allotropes.

Addition of a thallium vertex to empty and centered nine-atom deltahedral zintl ions of germanium and tin.

PubMed

Rios, Daniel; Gillett-Kunnath, Miriam M; Taylor, Jacob D; Oliver, Allen G; Sevov, Slavi C

2011-03-21

Nickel atoms were inserted into nine-atom deltahedral Zintl ions of E(9)(4-) (E = Ge, Sn) via reactions with Ni(cod)(2) (cod = cyclooctadiene), and [Ni@Sn(9)](3-) was structurally characterized. Both the empty and the Ni-centered clusters react with TlCp (Cp = cyclopentadienyl anion) and add a thallium vertex to form the deltahedral ten-atom closo-species [E(9)Tl](3-) and [Ni@E(9)Tl](3-), respectively. The structures of [Ge(9)Tl](3-) and [Ni@Sn(9)Tl](3-) showed that, as expected, the geometry of the ten-atom clusters is that of a bicapped square antiprism where the Tl-atom occupies one of the two capping vertices. This illustrates that centering a nine-atom cluster with a nickel atom does not change its reactivity toward TlCp. All compounds were characterized by electrospray mass spectrometry.

Accurate atom-mapping computation for biochemical reactions.

PubMed

Latendresse, Mario; Malerich, Jeremiah P; Travers, Mike; Karp, Peter D

2012-11-26

The complete atom mapping of a chemical reaction is a bijection of the reactant atoms to the product atoms that specifies the terminus of each reactant atom. Atom mapping of biochemical reactions is useful for many applications of systems biology, in particular for metabolic engineering where synthesizing new biochemical pathways has to take into account for the number of carbon atoms from a source compound that are conserved in the synthesis of a target compound. Rapid, accurate computation of the atom mapping(s) of a biochemical reaction remains elusive despite significant work on this topic. In particular, past researchers did not validate the accuracy of mapping algorithms. We introduce a new method for computing atom mappings called the minimum weighted edit-distance (MWED) metric. The metric is based on bond propensity to react and computes biochemically valid atom mappings for a large percentage of biochemical reactions. MWED models can be formulated efficiently as Mixed-Integer Linear Programs (MILPs). We have demonstrated this approach on 7501 reactions of the MetaCyc database for which 87% of the models could be solved in less than 10 s. For 2.1% of the reactions, we found multiple optimal atom mappings. We show that the error rate is 0.9% (22 reactions) by comparing these atom mappings to 2446 atom mappings of the manually curated Kyoto Encyclopedia of Genes and Genomes (KEGG) RPAIR database. To our knowledge, our computational atom-mapping approach is the most accurate and among the fastest published to date. The atom-mapping data will be available in the MetaCyc database later in 2012; the atom-mapping software will be available within the Pathway Tools software later in 2012.

Wavy carbon: A new series of carbon structures explored by quantum chemical calculations

NASA Astrophysics Data System (ADS)

Ohno, Koichi; Satoh, Hiroko; Iwamoto, Takeaki; Tokoyama, Hiroaki; Yamakado, Hideo

2015-10-01

A new carbon family adopting wavy structures has been found by quantum chemical calculations. The key motif of this family is a condensed four-membered ring. Periodically wavy-carbon sheets (wavy-Cn sheets, n = 2, 6, and 8) as well as wavy-C36 tube were found to be very similar to the previously reported prism-Cn carbon tubes (n = 5, 6, and 8) in several respects, including the relative energies per one carbon atom with respect to graphene, CC bond lengths, and CCC bond angles. Because of very high relative energies with respect to graphene (206-253 kJ mol-1), the wavy-carbons may behave as energy reserving materials.

Raman fingerprints of atomically precise graphene nanoribbons

DOE PAGES

Verzhbitskiy, Ivan A.; Corato, Marzio De; Ruini, Alice; ...

2016-02-23

Bottom-up approaches allow the production of ultranarrow and atomically precise graphene nanoribbons (GNRs) with electronic and optical properties controlled by the specific atomic structure. Combining Raman spectroscopy and ab initio simulations, we show that GNR width, edge geometry, and functional groups all influence their Raman spectra. As a result, the low-energy spectral region below 1000 cm –1 is particularly sensitive to edge morphology and functionalization, while the D peak dispersion can be used to uniquely fingerprint the presence of GNRs and differentiates them from other sp 2 carbon nanostructures.

CARBON-14. A Literature Search

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

None

1965-01-01

The bibliography was prepared by the Philippine Atomic Energy Commission (PAEC) for scientists and researchers interested in the study of Carbon 14. The bibliography contains 840 entries. The references cited in this work were abstracted in the Nuclear Science Abstracts (NSA) of the U.S. Atomic Energy Commission covering the period from January 1947 to April 1963.

Quantum dynamics of hydrogen atoms on graphene. I. System-bath modeling.

PubMed

Bonfanti, Matteo; Jackson, Bret; Hughes, Keith H; Burghardt, Irene; Martinazzo, Rocco

2015-09-28

An accurate system-bath model to investigate the quantum dynamics of hydrogen atoms chemisorbed on graphene is presented. The system comprises a hydrogen atom and the carbon atom from graphene that forms the covalent bond, and it is described by a previously developed 4D potential energy surface based on density functional theory ab initio data. The bath describes the rest of the carbon lattice and is obtained from an empirical force field through inversion of a classical equilibrium correlation function describing the hydrogen motion. By construction, model building easily accommodates improvements coming from the use of higher level electronic structure theory for the system. Further, it is well suited to a determination of the system-environment coupling by means of ab initio molecular dynamics. This paper details the system-bath modeling and shows its application to the quantum dynamics of vibrational relaxation of a chemisorbed hydrogen atom, which is here investigated at T = 0 K with the help of the multi-configuration time-dependent Hartree method. Paper II deals with the sticking dynamics.

Quantum dynamics of hydrogen atoms on graphene. I. System-bath modeling

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

Bonfanti, Matteo, E-mail: matteo.bonfanti@unimi.it; Jackson, Bret; Hughes, Keith H.

2015-09-28

An accurate system-bath model to investigate the quantum dynamics of hydrogen atoms chemisorbed on graphene is presented. The system comprises a hydrogen atom and the carbon atom from graphene that forms the covalent bond, and it is described by a previously developed 4D potential energy surface based on density functional theory ab initio data. The bath describes the rest of the carbon lattice and is obtained from an empirical force field through inversion of a classical equilibrium correlation function describing the hydrogen motion. By construction, model building easily accommodates improvements coming from the use of higher level electronic structure theorymore » for the system. Further, it is well suited to a determination of the system-environment coupling by means of ab initio molecular dynamics. This paper details the system-bath modeling and shows its application to the quantum dynamics of vibrational relaxation of a chemisorbed hydrogen atom, which is here investigated at T = 0 K with the help of the multi-configuration time-dependent Hartree method. Paper II deals with the sticking dynamics.« less

Neutral Atomic Emissions from Comet Hale-Bopp

NASA Astrophysics Data System (ADS)

Oliversen, R. J.; Scherb, F.; Roesler, F. L.; Mierkiewicz, E. J.; Woodward, R. C.; Hilton, G. M.; Doane, N. E.

1997-07-01

High resolution (R=100,000) spectra of atomic oxygen, hydrogen, and carbon from Comet Hale-Bopp were obtained at the NSO McMath-Pierce main telescope from February 8 to April 19, 1997, using a 50 mm dual-etalon Fabry-Perot/CCD spectrometer. The field of view was 6 arcmin. Spectra with good signal-to-noise were obtained for the emission lines [O I] 6300 Angstroms, Hα (6563 Angstroms), and [C I] 9850 Angstroms. On several of these nights, complementary [O I] 6300 Angstroms observations were simultaneously obtained with the Wisconsin Hα Mapper (WHα M) at Kitt Peak. Additional [O I] 6300 Angstroms observations were also obtained in September 1996. These [C I] 9850 Angstroms observations are the first extensive data set of this cometary line. We will present an overview of our observations and preliminary results.

Selective Aliphatic Carbon-Carbon Bond Activation by Rhodium Porphyrin Complexes.

PubMed

To, Ching Tat; Chan, Kin Shing

2017-07-18

The carbon-carbon bond activation of organic molecules with transition metal complexes is an attractive transformation. These reactions form transition metal-carbon bonded intermediates, which contribute to fundamental understanding in organometallic chemistry. Alternatively, the metal-carbon bond in these intermediates can be further functionalized to construct new carbon-(hetero)atom bonds. This methodology promotes the concept that the carbon-carbon bond acts as a functional group, although carbon-carbon bonds are kinetically inert. In the past few decades, numerous efforts have been made to overcome the chemo-, regio- and, more recently, stereoselectivity obstacles. The synthetic usefulness of the selective carbon-carbon bond activation has been significantly expanded and is becoming increasingly practical: this technique covers a wide range of substrate scopes and transition metals. In the past 16 years, our laboratory has shown that rhodium porphyrin complexes effectively mediate the intermolecular stoichiometric and catalytic activation of both strained and nonstrained aliphatic carbon-carbon bonds. Rhodium(II) porphyrin metalloradicals readily activate the aliphatic carbon(sp 3 )-carbon(sp 3 ) bond in TEMPO ((2,2,6,6-tetramethylpiperidin-1-yl)oxyl) and its derivatives, nitriles, nonenolizable ketones, esters, and amides to produce rhodium(III) porphyrin alkyls. Recently, the cleavage of carbon-carbon σ-bonds in unfunctionalized and noncoordinating hydrocarbons with rhodium(II) porphyrin metalloradicals has been developed. The absence of carbon-hydrogen bond activation in these systems makes the reaction unique. Furthermore, rhodium(III) porphyrin hydroxide complexes can be generated in situ to selectively activate the carbon(α)-carbon(β) bond in ethers and the carbon(CO)-carbon(α) bond in ketones under mild conditions. The addition of PPh 3 promotes the reaction rate and yield of the carbon-carbon bond activation product. Thus, both rhodium

Benchmark calculations of excess electrons in water cluster cavities: balancing the addition of atom-centered diffuse functions versus floating diffuse functions.

PubMed

Zhang, Changzhe; Bu, Yuxiang

2016-09-14

Diffuse functions have been proved to be especially crucial for the accurate characterization of excess electrons which are usually bound weakly in intermolecular zones far away from the nuclei. To examine the effects of diffuse functions on the nature of the cavity-shaped excess electrons in water cluster surroundings, both the HOMO and LUMO distributions, vertical detachment energies (VDEs) and visible absorption spectra of two selected (H2O)24(-) isomers are investigated in the present work. Two main types of diffuse functions are considered in calculations including the Pople-style atom-centered diffuse functions and the ghost-atom-based floating diffuse functions. It is found that augmentation of atom-centered diffuse functions contributes to a better description of the HOMO (corresponding to the VDE convergence), in agreement with previous studies, but also leads to unreasonable diffuse characters of the LUMO with significant red-shifts in the visible spectra, which is against the conventional point of view that the more the diffuse functions, the better the results. The issue of designing extra floating functions for excess electrons has also been systematically discussed, which indicates that the floating diffuse functions are necessary not only for reducing the computational cost but also for improving both the HOMO and LUMO accuracy. Thus, the basis sets with a combination of partial atom-centered diffuse functions and floating diffuse functions are recommended for a reliable description of the weakly bound electrons. This work presents an efficient way for characterizing the electronic properties of weakly bound electrons accurately by balancing the addition of atom-centered diffuse functions and floating diffuse functions and also by balancing the computational cost and accuracy of the calculated results, and thus is very useful in the relevant calculations of various solvated electron systems and weakly bound anionic systems.

Atomic data and spectral analysis of carbon, nitrogen, oxygen and silicon ions observed with the International Ultraviolet Explorer

NASA Technical Reports Server (NTRS)

Pradhan, Anil K.

1992-01-01

According to the plan presented in the original proposal we have now completed most of the atomic calculations involving collision strengths and rate coefficients for electron impact excitation of C II, N III, and O IV ions. These have been reported in the first two publications appended with this report. We have now moved into the applications phase of the project with the new data being used to analyze the International Ultraviolet Explorer (IUE) observations of a variety of objects, as described in the third publication recently submitted (also appended). The analysis and interpretation of archival data will continue well into the next year with several collaborators that the PI and Co-PI are involved with. In addition, the atomic calculations on Si II have been started.

On the trends of Fukui potential and hardness potential derivatives in isolated atoms vs. atoms in molecules.

PubMed

Bhattacharjee, Rituparna; Roy, Ram Kinkar

2014-10-28

In the present study, trends of electronic contribution to molecular electrostatic potential [Vel(r¯)(r=0)], Fukui potential [v(+)f|(r=0) and v(-)f|(r=0)] and hardness potential derivatives [Δ(+)h(k) and Δ(-)h(k)] for isolated atoms as well as atoms in molecules are investigated. The generated numerical values of these three reactivity descriptors in these two electronically different situations are critically analyzed through the relevant formalism. Values of Vel(r¯) (when r → 0, i.e., on the nucleus) are higher for atoms in molecules than that of isolated atoms. In contrast, higher values of v(+)|(r=0) and v(-)|(r=0) are observed for isolated atoms compared to the values for atoms in a molecule. However, no such regular trend is observed for the Δ(+)h(k) and Δ(-)h(k) values, which is attributed to the uncertainty in the Fukui function values of atoms in molecules. The sum of Fukui potential and the sum of hardness potential derivatives in molecules are also critically analyzed, which shows the efficacy of orbital relaxation effects in quantifying the values of these parameters. The chemical consequence of the observed trends of these descriptors in interpreting electron delocalization, electronic relaxation and non-negativity of atomic Fukui function indices is also touched upon. Several commonly used molecules containing carbon as well as heteroatoms are chosen to make the investigation more insightful.

Additive Manufacturing of Multifunctional Components Using High Density Carbon Nanotube Yarn Filaments

NASA Technical Reports Server (NTRS)

Gardner, John M.; Sauti, Godfrey; Kim, Jae-Woo; Cano, Roberto J.; Wincheski, Russell A.; Stelter, Christopher J.; Grimsley, Brian W.; Working, Dennis C.; Siochi, Emilie J.

2016-01-01

Additive manufacturing allows for design freedom and part complexity not currently attainable using traditional manufacturing technologies. Fused Filament Fabrication (FFF), for example, can yield novel component geometries and functionalities because the method provides a high level of control over material placement and processing conditions. This is achievable by extrusion of a preprocessed filament feedstock material along a predetermined path. However if fabrication of a multifunctional part relies only on conventional filament materials, it will require a different material for each unique functionality printed into the part. Carbon nanotubes (CNTs) are an attractive material for many applications due to their high specific strength as well as good electrical and thermal conductivity. The presence of this set of properties in a single material presents an opportunity to use one material to achieve multifunctionality in an additively manufactured part. This paper describes a recently developed method for processing continuous CNT yarn filaments into three-dimensional articles, and summarizes the mechanical, electrical, and sensing performance of the components fabricated in this way.

Atomization methods for forming magnet powders

DOEpatents

Sellers, Charles H.; Branagan, Daniel J.; Hyde, Timothy A.

2000-01-01

The invention encompasses methods of utilizing atomization, methods for forming magnet powders, methods for forming magnets, and methods for forming bonded magnets. The invention further encompasses methods for simulating atomization conditions. In one aspect, the invention includes an atomization method for forming a magnet powder comprising: a) forming a melt comprising R.sub.2.1 Q.sub.13.9 B.sub.1, Z and X, wherein R is a rare earth element; X is an element selected from the group consisting of carbon, nitrogen, oxygen and mixtures thereof; Q is an element selected from the group consisting of Fe, Co and mixtures thereof; and Z is an element selected from the group consisting of Ti, Zr, Hf and mixtures thereof; b) atomizing the melt to form generally spherical alloy powder granules having an internal structure comprising at least one of a substantially amorphous phase or a substantially nanocrystalline phase; and c) heat treating the alloy powder to increase an energy product of the alloy powder; after the heat treatment, the alloy powder comprising an energy product of at least 10 MGOe. In another aspect, the invention includes a magnet comprising R, Q, B, Z and X, wherein R is a rare earth element; X is an element selected from the group consisting of carbon, nitrogen, oxygen and mixtures thereof; Q is an element selected from the group consisting of Fe, Co and mixtures thereof; and Z is an element selected from the group consisting of Ti, Zr, Hf and mixtures thereof; the magnet comprising an internal structure comprising R.sub.2.1 Q.sub.13.9 B.sub.1.

A nano universal joint made from curved double-walled carbon nanotubes

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

Cai, Kun; Cai, Haifang; Shi, Jiao

2015-06-15

A nano universal joint is constructed from curved double-wall carbon nanotubes with a short outer tube as stator and a long inner tube as a rotor. When one end of the rotor is driven (by a rotary motor) to rotate, the same rotational speed but with different rotational direction will be induced at the other end of the rotor. This mechanism makes the joint useful for designing a flexible nanodevice with an adjustable output rotational signal. The motion transmission effect of the universal joint is analyzed using a molecular dynamics simulation approach. In particular, the effects of three factors aremore » investigated. The first factor is the curvature of the stator, which produces a different rotational direction of the rotor at the output end. The second is the bonding conditions of carbon atoms on the adjacent tube ends of the motor and the rotor, sp{sup 1} or sp{sup 2} atoms, which create different attraction between the motor and the rotor. The third is the rotational speed of the motor, which can be considered as the input signal of the universal joint. It is noted that the rotor's rotational speed is usually the same as that of the motor when the carbon atoms on the adjacent ends of the motor and the rotor are sp{sup 1} carbon atoms. When they become the new sp{sup 2} atoms, the rotor experiences a jump in rotational speed from a lower value to that of the motor. The mechanism of drops in potential of the motor is revealed. If the carbon atoms on the adjacent ends are sp{sup 2} atoms, the rotor rotates more slowly than the motor, whereas the rotational speed is stable when driven by a higher speed motor.« less

A nano universal joint made from curved double-walled carbon nanotubes

NASA Astrophysics Data System (ADS)

Cai, Kun; Cai, Haifang; Shi, Jiao; Qin, Qing H.

2015-06-01

A nano universal joint is constructed from curved double-wall carbon nanotubes with a short outer tube as stator and a long inner tube as a rotor. When one end of the rotor is driven (by a rotary motor) to rotate, the same rotational speed but with different rotational direction will be induced at the other end of the rotor. This mechanism makes the joint useful for designing a flexible nanodevice with an adjustable output rotational signal. The motion transmission effect of the universal joint is analyzed using a molecular dynamics simulation approach. In particular, the effects of three factors are investigated. The first factor is the curvature of the stator, which produces a different rotational direction of the rotor at the output end. The second is the bonding conditions of carbon atoms on the adjacent tube ends of the motor and the rotor, sp1 or sp2 atoms, which create different attraction between the motor and the rotor. The third is the rotational speed of the motor, which can be considered as the input signal of the universal joint. It is noted that the rotor's rotational speed is usually the same as that of the motor when the carbon atoms on the adjacent ends of the motor and the rotor are sp1 carbon atoms. When they become the new sp2 atoms, the rotor experiences a jump in rotational speed from a lower value to that of the motor. The mechanism of drops in potential of the motor is revealed. If the carbon atoms on the adjacent ends are sp2 atoms, the rotor rotates more slowly than the motor, whereas the rotational speed is stable when driven by a higher speed motor.

Mechanics of low-dimensional carbon nanostructures: Atomistic, continuum, and multi-scale approaches

NASA Astrophysics Data System (ADS)

Mahdavi, Arash

A new multiscale modeling technique called the Consistent Atomic-scale Finite Element (CAFE) method is introduced. Unlike traditional approaches for linking the atomic structure to its equivalent continuum, this method directly connects the atomic degrees of freedom to a reduced set of finite element degrees of freedom without passing through an intermediate homogenized continuum. As a result, there is no need to introduce stress and strain measures at the atomic level. The Tersoff-Brenner interatomic potential is used to calculate the consistent tangent stiffness matrix of the structure. In this finite element formulation, all local and non-local interactions between carbon atoms are taken into account using overlapping finite elements. In addition, a consistent hierarchical finite element modeling technique is developed for adaptively coarsening and refining the mesh over different parts of the model. This process is consistent with the underlying atomic structure and, by refining the mesh to the scale of atomic spacing, molecular dynamic results can be recovered. This method is valid across the scales and can be used to concurrently model atomistic and continuum phenomena so, in contrast with most other multi-scale methods, there is no need to introduce artificial boundaries for coupling atomistic and continuum regions. Effect of the length scale of the nanostructure is also included in the model by building the hierarchy of elements from bottom up using a finite size atom cluster as the building block. To be consistent with the bravais multi-lattice structure of sp2-bonded carbon, two independent displacement fields are used for reducing the order of the model. Sparse structure of the stiffness matrix of these nanostructures is exploited to reduce the memory requirement and to speed up the formation of the system matrices and solution of the equilibrium equations. Applicability of the method is shown with several examples of the nonlinear mechanics of carbon

Optical field induced rotation of polarization in rubidium atoms with the additional magnetic field

NASA Astrophysics Data System (ADS)

Ummal Momeen, M.; Hu, Jianping

2017-11-01

We present the magnetic and optical field induced rotation of polarization in 87Rb and 85Rb atoms at geophysical magnetic fields. The line shape varies considerably in the presence of a magnetic field of the order of a few mG. Multiple Zeeman sublevel EIT systems involving rubidium atoms are investigated. Theoretical formalism of optical field induced polarization rotation in the presence of a magnetic field is discussed by considering all the Zeeman sublevels. It is noted that the ground state population distribution also plays a major role.

Cubic martensite in high carbon steel

NASA Astrophysics Data System (ADS)

Chen, Yulin; Xiao, Wenlong; Jiao, Kun; Ping, Dehai; Xu, Huibin; Zhao, Xinqing; Wang, Yunzhi

2018-05-01

A distinguished structural characteristic of martensite in Fe-C steels is its tetragonality originating from carbon atoms occupying only one set of the three available octahedral interstitial sites in the body-centered-cubic (bcc) Fe lattice. Such a body-centered-tetragonal (bct) structure is believed to be thermodynamically stable because of elastic interactions between the interstitial carbon atoms. For such phase stability, however, there has been a lack of direct experimental evidence despite extensive studies of phase transformations in steels over one century. In this Rapid Communication, we report that the martensite formed in a high carbon Fe-8Ni-1.26C (wt%) steel at room temperature induced by applied stress/strain has actually a bcc rather than a bct crystal structure. This finding not only challenges the existing theories on the stability of bcc vs bct martensite in high carbon steels, but also provides insights into the mechanism for martensitic transformation in ferrous alloys.

Toxicity and biocompatibility of carbon nanoparticles.

PubMed

Fiorito, S; Serafino, A; Andreola, F; Togna, A; Togna, G

2006-03-01

A review is presented of the literature data concerning the effects induced by carbon nanoparticles on the biological environment and the importance of these effects in human and animal health. The discovery in 1985 of fullerenes, a novel carbon allotrope with a polygonal structure made up solely by 60 carbon atoms, and in 1991 of carbon nanotubes, thin carbon filaments (1-3 microm in length and 1-3 nm in diameter) with extraordinary mechanical properties, opened a wide field of activity in carbon research. During the last few years, practical applications of fullerenes as biological as well as pharmacological agents have been investigated. Various fullerene-based compounds were tested for biological activity, including antiviral, antioxidant, and chemiotactic activities. Nanotubes consist of carbon atoms arranged spirally to form concentric cylinders, that are perfect crystals and thinner than graphite whiskers. They are stronger than steel but very flexible and lightweight and transfer heat better than any other known material. These characteristics make them suitable for various potential applications such as super strong cables and tips for scanning probe microscopes, as well as biomedical devices for drug delivery, medical diagnostic, and therapeutic applications. The effects induced by these nanostructures on rat lung tissues, as well as on human skin and human macrophage and keratinocyte cells are presented.

The adsorption of helium atoms on coronene cations

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

Kurzthaler, Thomas; Rasul, Bilal; Kuhn, Martin

2016-08-14

We report the first experimental study of the attachment of multiple foreign atoms to a cationic polycyclic aromatic hydrocarbon (PAH). The chosen PAH was coronene, C{sub 24}H{sub 12}, which was added to liquid helium nanodroplets and then subjected to electron bombardment. Using mass spectrometry, coronene cations decorated with helium atoms were clearly seen and the spectrum shows peaks with anomalously high intensities (“magic number” peaks), which represent ion-helium complexes with added stability. The data suggest the formation of a rigid helium layer consisting of 38 helium atoms that completely cover both faces of the coronene ion. Additional magic numbers canmore » be seen for the further addition of 3 and 6 helium atoms, which are thought to attach to the edge of the coronene. The observation of magic numbers for the addition of 38 and 44 helium atoms is in good agreement with a recent path integral Monte Carlo prediction for helium atoms on neutral coronene. An understanding of how atoms and molecules attach to PAH ions is important for a number of reasons including the potential role such complexes might play in the chemistry of the interstellar medium.« less

Novel carbon-rich additives preparation by degradative solvent extraction of biomass wastes for coke-making.

PubMed

Zhu, Xianqing; Li, Xian; Xiao, Li; Zhang, Xiaoyong; Tong, Shan; Wu, Chao; Ashida, Ryuichi; Liu, Wenqiang; Miura, Kouichi; Yao, Hong

2016-05-01

In this work, two extracts (Soluble and Deposit) were produced by degradative solvent extraction of biomass wastes from 250 to 350°C. The feasibilities of using Soluble and Deposit as additives for coke-making were investigated for the first time. The Soluble and Deposit, having significantly higher carbon content, lower oxygen content and extremely lower ash content than raw biomasses. All Solubles and most of Deposits can melt completely at the temperature ranged from 80 to 120°C and 140 to 180°C, respectively. The additions of Soluble or Deposit into the coke-making coal significantly improved their thermoplastic properties with as high as 9°C increase of the plastic range. Furthermore, the addition of Deposit or Soluble also markedly enhanced the coke quality through increasing coke strength after reaction (CSR) and reducing coke reactivity index (CRI). Therefore, the Soluble and Deposit were proved to be good additives for coke-making. Copyright © 2016 Elsevier Ltd. All rights reserved.

Solvent-driven reductive activation of carbon dioxide by gold anions.

PubMed

Knurr, Benjamin J; Weber, J Mathias

2012-11-14

Catalytic activation and electrochemical reduction of CO(2) for the formation of chemically usable feedstock and fuel are central goals for establishing a carbon neutral fuel cycle. The role of solvent molecules in catalytic processes is little understood, although solvent-solute interactions can strongly influence activated intermediate species. We use vibrational spectroscopy of mass-selected Au(CO(2))(n)(-) cluster ions to probe the solvation of AuCO(2)(-) as a model for a reactive intermediate in the reductive activation of a CO(2) ligand by a single-atom catalyst. For the first few solvent molecules, solvation of the complex preferentially occurs at the CO(2) moiety, enhancing reductive activation through polarization of the excess charge onto the partially reduced ligand. At higher levels of solvation, direct interaction of additional solvent molecules with the Au atom diminishes reduction. The results show how the solvation environment can enhance or diminish the effects of a catalyst, offering design criteria for single-atom catalyst engineering.

Carbon-containing cathodes for enhanced electron emission

DOEpatents

Cao, Renyu; Pan, Lawrence; Vergara, German; Fox, Ciaran

2000-01-01

A cathode has electropositive atoms directly bonded to a carbon-containing substrate. Preferably, the substrate comprises diamond or diamond-like (sp.sup.3) carbon, and the electropositive atoms are Cs. The cathode displays superior efficiency and durability. In one embodiment, the cathode has a negative electron affinity (NEA). The cathode can be used for field emission, thermionic emission, or photoemission. Upon exposure to air or oxygen, the cathode performance can be restored by annealing or other methods. Applications include detectors, electron multipliers, sensors, imaging systems, and displays, particularly flat panel displays.

HPAM: Hirshfeld Partitioned Atomic Multipoles

PubMed Central

Elking, Dennis M.; Perera, Lalith; Pedersen, Lee G.

2011-01-01

An implementation of the Hirshfeld (HD) and Hirshfeld-Iterated (HD-I) atomic charge density partitioning schemes is described. Atomic charges and atomic multipoles are calculated from the HD and HD-I atomic charge densities for arbitrary atomic multipole rank lmax on molecules of arbitrary shape and size. The HD and HD-I atomic charges/multipoles are tested by comparing molecular multipole moments and the electrostatic potential (ESP) surrounding a molecule with their reference ab initio values. In general, the HD-I atomic charges/multipoles are found to better reproduce ab initio electrostatic properties over HD atomic charges/multipoles. A systematic increase in precision for reproducing ab initio electrostatic properties is demonstrated by increasing the atomic multipole rank from lmax = 0 (atomic charges) to lmax = 4 (atomic hexadecapoles). Both HD and HD-I atomic multipoles up to rank lmax are shown to exactly reproduce ab initio molecular multipole moments of rank L for L ≤ lmax. In addition, molecular dipole moments calculated by HD, HD-I, and ChelpG atomic charges only (lmax = 0) are compared with reference ab initio values. Significant errors in reproducing ab initio molecular dipole moments are found if only HD or HD-I atomic charges used. PMID:22140274

A screened independent atom model for the description of ion collisions from atomic and molecular clusters

NASA Astrophysics Data System (ADS)

Lüdde, Hans Jürgen; Horbatsch, Marko; Kirchner, Tom

2018-05-01

We apply a recently introduced model for an independent-atom-like calculation of ion-impact electron transfer and ionization cross sections to proton collisions from water, neon, and carbon clusters. The model is based on a geometrical interpretation of the cluster cross section as an effective area composed of overlapping circular disks that are representative of the atomic contributions. The latter are calculated using a time-dependent density-functional-theory-based single-particle description with accurate exchange-only ground-state potentials. We find that the net capture and ionization cross sections in p-X n collisions are proportional to n α with 2/3 ≤ α ≤ 1. For capture from water clusters at 100 keV impact energy α is close to one, which is substantially different from the value α = 2/3 predicted by a previous theoretical work based on the simplest-level electron nuclear dynamics method. For ionization at 100 keV and for capture at lower energies we find smaller α values than for capture at 100 keV. This can be understood by considering the magnitude of the atomic cross sections and the resulting overlaps of the circular disks that make up the cluster cross section in our model. Results for neon and carbon clusters confirm these trends. Simple parametrizations are found which fit the cross sections remarkably well and suggest that they depend on the relevant bond lengths.

Nano-soldering to single atomic layer

DOEpatents

Girit, Caglar O [Berkeley, CA; Zettl, Alexander K [Kensington, CA

2011-10-11

A simple technique to solder submicron sized, ohmic contacts to nanostructures has been disclosed. The technique has several advantages over standard electron beam lithography methods, which are complex, costly, and can contaminate samples. To demonstrate the soldering technique graphene, a single atomic layer of carbon, has been contacted, and low- and high-field electronic transport properties have been measured.

Effects of mineral additives on biochar formation: carbon retention, stability, and properties.

PubMed

Li, Feiyue; Cao, Xinde; Zhao, Ling; Wang, Jianfei; Ding, Zhenliang

2014-10-07

Biochar is being recognized as a promising tool for long-term carbon sequestration, and biochar with high carbon retention and strong stability is supposed to be explored for that purpose. In this study, three minerals, including kaolin, calcite (CaCO3), and calcium dihydrogen phosphate [Ca(H2PO4)2], were added to rice straw feedstock at the ratio of 20% (w/w) for biochar formation through pyrolysis treatment, aiming to improve carbon retention and stabilization in biochar. Kaolin and CaCO3 had little effect on the carbon retention, whereas Ca(H2PO4)2 increased the carbon retention by up to 29% compared to untreated biochar. Although the carbon loss from the kaolin-modified biochar with hydrogen peroxide oxidation was enhanced, CaCO3 and Ca(H2PO4)2 modification reduced the carbon loss by 18.6 and 58.5%, respectively. Moreover, all three minerals reduced carbon loss of biochar with potassium dichromate oxidation from 0.3 to 38.8%. The microbial mineralization as CO2 emission in all three modified biochars was reduced by 22.2-88.7% under aerobic incubation and 5-61% under anaerobic incubation. Enhanced carbon retention and stability of biochar with mineral treatment might be caused by the enhanced formation of aromatic C, which was evidenced by cross-polarization magic angle spinning (13)C nuclear magnetic resonance spectra and Fourier transform infrared spectroscopy analysis. Our results indicated that the three minerals, especially Ca(H2PO4)2, were effective in increasing carbon retention and strengthening biochar stabilization, which provided a novel idea that people could explore and produce the designated biochar with high carbon sequestration capacity and stability.

Experimental and theoretical investigation of radiation and dynamics properties in laser-produced carbon plasmas

NASA Astrophysics Data System (ADS)

Min, Qi; Su, Maogen; Wang, Bo; Cao, Shiquan; Sun, Duixiong; Dong, Chenzhong

2018-05-01

The radiation and dynamics properties of laser-produced carbon plasma in vacuum were studied experimentally with aid of a spatio-temporally resolved emission spectroscopy technique. In addition, a radiation hydrodynamics model based on the fluid dynamic equations and the radiative transfer equation was presented, and calculation of the charge states was performed within the time-dependent collisional radiative model. Detailed temporal and spatial evolution behavior about plasma parameters have been analyzed, such as velocity, electron temperature, charge state distribution, energy level population, and various atomic processes. At the same time, the effects of different atomic processes on the charge state distribution were examined. Finally, the validity of assuming a local thermodynamic equilibrium in the carbon plasma expansion was checked, and the results clearly indicate that the assumption was valid only at the initial (<80 ns) stage of plasma expansion. At longer delay times, it was not applicable near the plasma boundary because of a sharp drop of plasma temperature and electron density.

Crystallized and amorphous vortices in rotating atomic-molecular Bose-Einstein condensates

PubMed Central

Liu, Chao-Fei; Fan, Heng; Gou, Shih-Chuan; Liu, Wu-Ming

2014-01-01

Vortex is a topological defect with a quantized winding number of the phase in superfluids and superconductors. Here, we investigate the crystallized (triangular, square, honeycomb) and amorphous vortices in rotating atomic-molecular Bose-Einstein condensates (BECs) by using the damped projected Gross-Pitaevskii equation. The amorphous vortices are the result of the considerable deviation induced by the interaction of atomic-molecular vortices. By changing the atom-molecule interaction from attractive to repulsive, the configuration of vortices can change from an overlapped atomic-molecular vortices to carbon-dioxide-type ones, then to atomic vortices with interstitial molecular vortices, and finally into independent separated ones. The Raman detuning can tune the ratio of the atomic vortex to the molecular vortex. We provide a phase diagram of vortices in rotating atomic-molecular BECs as a function of Raman detuning and the strength of atom-molecule interaction. PMID:24573303

A Compact, High-Flux Cold Atom Beam Source

NASA Technical Reports Server (NTRS)

Kellogg, James R.; Kohel, James M.; Thompson, Robert J.; Aveline, David C.; Yu, Nan; Schlippert, Dennis

2012-01-01

The performance of cold atom experiments relying on three-dimensional magneto-optical trap techniques can be greatly enhanced by employing a highflux cold atom beam to obtain high atom loading rates while maintaining low background pressures in the UHV MOT (ultra-high vacuum magneto-optical trap) regions. Several techniques exist for generating slow beams of cold atoms. However, one of the technically simplest approaches is a two-dimensional (2D) MOT. Such an atom source typically employs at least two orthogonal trapping beams, plus an additional longitudinal "push" beam to yield maximum atomic flux. A 2D atom source was created with angled trapping collimators that not only traps atoms in two orthogonal directions, but also provides a longitudinal pushing component that eliminates the need for an additional push beam. This development reduces the overall package size, which in turn, makes the 2D trap simpler, and requires less total optical power. The atom source is more compact than a previously published effort, and has greater than an order of magnitude improved loading performance.

Advanced Electrochemistry of Individual Metal Clusters Electrodeposited Atom by Atom to Nanometer by Nanometer.

PubMed

Kim, Jiyeon; Dick, Jeffrey E; Bard, Allen J

2016-11-15

Metal clusters are very important as building blocks for nanoparticles (NPs) for electrocatalysis and electroanalysis in both fundamental and applied electrochemistry. Attention has been given to understanding of traditional nucleation and growth of metal clusters and to their catalytic activities for various electrochemical applications in energy harvesting as well as analytical sensing. Importantly, understanding the properties of these clusters, primarily the relationship between catalysis and morphology, is required to optimize catalytic function. This has been difficult due to the heterogeneities in the size, shape, and surface properties. Thus, methods that address these issues are necessary to begin understanding the reactivity of individual catalytic centers as opposed to ensemble measurements, where the effect of size and morphology on the catalysis is averaged out in the measurement. This Account introduces our advanced electrochemical approaches to focus on each isolated metal cluster, where we electrochemically fabricated clusters or NPs atom by atom to nanometer by nanometer and explored their electrochemistry for their kinetic and catalytic behavior. Such approaches expand the dimensions of analysis, to include the electrochemistry of (1) a discrete atomic cluster, (2) solely a single NP, or (3) individual NPs in the ensemble sample. Specifically, we studied the electrocatalysis of atomic metal clusters as a nascent electrocatalyst via direct electrodeposition on carbon ultramicroelectrode (C UME) in a femtomolar metal ion precursor. In addition, we developed tunneling ultramicroelectrodes (TUMEs) to study electron transfer (ET) kinetics of a redox probe at a single metal NP electrodeposited on this TUME. Owing to the small dimension of a NP as an active area of a TUME, extremely high mass transfer conditions yielded a remarkably high standard ET rate constant, k 0 , of 36 cm/s for outer-sphere ET reaction. Most recently, we advanced nanoscale

Macroevolutionary trends of atomic composition and related functional group proportion in eukaryotic and prokaryotic proteins.

PubMed

Zhang, Yu-Juan; Yang, Chun-Lin; Hao, You-Jin; Li, Ying; Chen, Bin; Wen, Jian-Fan

2014-01-25

To fully explore the trends of atomic composition during the macroevolution from prokaryote to eukaryote, five atoms (oxygen, sulfur, nitrogen, carbon, hydrogen) and related functional groups in prokaryotic and eukaryotic proteins were surveyed and compared. Genome-wide analysis showed that eukaryotic proteins have more oxygen, sulfur and nitrogen atoms than prokaryotes do. Clusters of Orthologous Groups (COG) analysis revealed that oxygen, sulfur, carbon and hydrogen frequencies are higher in eukaryotic proteins than in their prokaryotic orthologs. Furthermore, functional group analysis demonstrated that eukaryotic proteins tend to have higher proportions of sulfhydryl, hydroxyl and acylamino, but lower of sulfide and carboxyl. Taken together, an apparent trend of increase was observed for oxygen and sulfur atoms in the macroevolution; the variation of oxygen and sulfur compositions and their related functional groups in macroevolution made eukaryotic proteins carry more useful functional groups. These results will be helpful for better understanding the functional significances of atomic composition evolution. Copyright © 2013 Elsevier B.V. All rights reserved.

Adsorptive removal of sulfate from acid mine drainage by polypyrrole modified activated carbons: Effects of polypyrrole deposition protocols and activated carbon source.

PubMed

Hong, Siqi; Cannon, Fred S; Hou, Pin; Byrne, Tim; Nieto-Delgado, Cesar

2017-10-01

Polypyrrole modified activated carbon was used to remove sulfate from acid mine drainage water. The polypyrrole modified activated carbon created positively charged functionality that offered elevated sorption capacity for sulfate. The effects of the activated carbon type, approach of polymerization, preparation temperature, solvent, and concentration of oxidant solution over the sulfate adsorption capacity were studied at an array of initial sulfate concentrations. A hardwood based activated carbon was the more favorable activated carbon template, and this offered better sulfate removal than when using bituminous based activated carbon or oak wood activated carbon as the template. The hardwood-based activated carbon modified with polypyrrole removed 44.7 mg/g sulfate, and this was five times higher than for the pristine hardwood-based activated carbon. Various protocols for depositing the polypyrrole onto the activated carbon were investigated. When ferric chloride was used as an oxidant, the deposition protocol that achieved the most N + atomic percent (3.35%) while also maintaining the least oxygen atomic percent (6.22%) offered the most favorable sulfate removal. For the rapid small scale column tests, when processing the AMD water, hardwood-based activated carbon modified with poly pyrrole exhibited 33 bed volume compared to the 5 bed volume of pristine activated carbons. Copyright © 2017 Elsevier Ltd. All rights reserved.

Influence of Different Defects in Vertically Aligned Carbon Nanotubes on TiO2 Nanoparticle Formation through Atomic Layer Deposition.

PubMed

Acauan, Luiz; Dias, Anna C; Pereira, Marcelo B; Horowitz, Flavio; Bergmann, Carlos P

2016-06-29

The chemical inertness of carbon nanotubes (CNT) requires some degree of "defect engineering" for controlled deposition of metal oxides through atomic layer deposition (ALD). The type, quantity, and distribution of such defects rules the deposition rate and defines the growth behavior. In this work, we employed ALD to grow titanium oxide (TiO2) on vertically aligned carbon nanotubes (VACNT). The effects of nitrogen doping and oxygen plasma pretreatment of the CNT on the morphology and total amount of TiO2 were systematically studied using transmission electron microscopy, Raman spectroscopy, and thermogravimetric analysis. The induced chemical changes for each functionalization route were identified by X-ray photoelectron and Raman spectroscopies. The TiO2 mass fraction deposited with the same number of cycles for the pristine CNT, nitrogen-doped CNT, and plasma-treated CNT were 8, 47, and 80%, respectively. We demonstrate that TiO2 nucleation is dependent mainly on surface incorporation of heteroatoms and their distribution rather than structural defects that govern the growth behavior. Therefore, selecting the best way to functionalize CNT will allow us to tailor TiO2 distribution and hence fabricate complex heterostructures.

Enhanced Production of Green Tide Algal Biomass through Additional Carbon Supply

PubMed Central

de Paula Silva, Pedro H.; Paul, Nicholas A.; de Nys, Rocky; Mata, Leonardo

2013-01-01

Intensive algal cultivation usually requires a high flux of dissolved inorganic carbon (Ci) to support productivity, particularly for high density algal cultures. Carbon dioxide (CO2) enrichment can be used to overcome Ci limitation and enhance productivity of algae in intensive culture, however, it is unclear whether algal species with the ability to utilise bicarbonate (HCO3 −) as a carbon source for photosynthesis will benefit from CO2 enrichment. This study quantified the HCO3 − affinity of three green tide algal species, Cladophora coelothrix, Cladophora patentiramea and Chaetomorpha linum, targeted for biomass and bioenergy production. Subsequently, we quantified productivity and carbon, nitrogen and ash content in response to CO2 enrichment. All three species had similar high pH compensation points (9.7–9.9), and grew at similar rates up to pH 9, demonstrating HCO3 − utilization. Algal cultures enriched with CO2 as a carbon source had 30% more total Ci available, supplying twenty five times more CO2 than the control. This higher Ci significantly enhanced the productivity of Cladophora coelothrix (26%), Chaetomorpha linum (24%) and to a lesser extent for Cladophora patentiramea (11%), compared to controls. We demonstrated that supplying carbon as CO2 can enhance the productivity of targeted green tide algal species under intensive culture, despite their clear ability to utilise HCO3 −. PMID:24324672

Enhanced production of green tide algal biomass through additional carbon supply.

PubMed

de Paula Silva, Pedro H; Paul, Nicholas A; de Nys, Rocky; Mata, Leonardo

2013-01-01

Intensive algal cultivation usually requires a high flux of dissolved inorganic carbon (Ci) to support productivity, particularly for high density algal cultures. Carbon dioxide (CO2) enrichment can be used to overcome Ci limitation and enhance productivity of algae in intensive culture, however, it is unclear whether algal species with the ability to utilise bicarbonate (HCO3 (-)) as a carbon source for photosynthesis will benefit from CO2 enrichment. This study quantified the HCO3 (-) affinity of three green tide algal species, Cladophora coelothrix, Cladophora patentiramea and Chaetomorpha linum, targeted for biomass and bioenergy production. Subsequently, we quantified productivity and carbon, nitrogen and ash content in response to CO2 enrichment. All three species had similar high pH compensation points (9.7-9.9), and grew at similar rates up to pH 9, demonstrating HCO3 (-) utilization. Algal cultures enriched with CO2 as a carbon source had 30% more total Ci available, supplying twenty five times more CO2 than the control. This higher Ci significantly enhanced the productivity of Cladophora coelothrix (26%), Chaetomorpha linum (24%) and to a lesser extent for Cladophora patentiramea (11%), compared to controls. We demonstrated that supplying carbon as CO2 can enhance the productivity of targeted green tide algal species under intensive culture, despite their clear ability to utilise HCO3 (-).