A methodology to estimate greenhouse gases emissions in Life Cycle Inventories of wastewater treatment plants

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

Rodriguez-Garcia, G., E-mail: gonzalo.rodriguez.garcia@usc.es; Hospido, A., E-mail: almudena.hospido@usc.es; Bagley, D.M., E-mail: bagley@uwyo.edu

2012-11-15

The main objective of this paper is to present the Direct Emissions Estimation Model (DEEM), a model for the estimation of CO{sub 2} and N{sub 2}O emissions from a wastewater treatment plant (WWTP). This model is consistent with non-specific but widely used models such as AS/AD and ASM no. 1 and presents the benefits of simplicity and application over a common WWTP simulation platform, BioWin Registered-Sign , making it suitable for Life Cycle Assessment and Carbon Footprint studies. Its application in a Spanish WWTP indicates direct N{sub 2}O emissions to be 8 times larger than those associated with electricity usemore » and thus relevant for LCA. CO{sub 2} emissions can be of similar importance to electricity-associated ones provided that 20% of them are of non-biogenic origin. - Highlights: Black-Right-Pointing-Pointer A model has been developed for the estimation of GHG emissions in WWTP. Black-Right-Pointing-Pointer Model was consistent with both ASM no. 1 and AS/AD. Black-Right-Pointing-Pointer N{sub 2}O emissions are 8 times more relevant than the one associated with electricity. Black-Right-Pointing-Pointer CO{sub 2} emissions are as important as electricity if 20% of it is non-biogenic.« less

Greenhouse gas emissions from the enteric fermentation and manure storage of dairy and beef cattle in China during 1961–2010

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

Gao, Zhiling, E-mail: zhilinggao@hotmail.com; Lin, Zhi; Yang, Yuanyuan

Due to the expanding dairy and beef population in China and their contribution to global CH{sub 4} and N{sub 2}O budgets, a framework considering changes in feed, manure management and herd structure was established to indicate the trends of CH{sub 4} and N{sub 2}O emissions from the enteric formation and manure storage in China's beef and dairy production and the underlying driving forces during the period 1961–2010. From 1961 to 2010, annual CH{sub 4} and N{sub 2}O emissions from beef cattle in China increased from 2.18 Mt to 5.86 Mt and from 7.93 kt–29.56 kt, respectively, while those from dairymore » cattle increased from 0.023 to 1.09 Mt and 0.12 to 7.90 kt, respectively. These increases were attributed to the combined changes in cattle population and management practices in feeds and manure storage. Improvement in cattle genetics during the period increased the bodyweight, required dry matter intake and gross energy and thus resulted in increased enteric CH{sub 4} EFs for each category of beef and dairy cattle as well as the overall enteric EFs (i.e., Tier 1 in IPCC). However, for beef cattle, such an impact on the overall enteric EFs was largely offset by the herd structure transition from draft animal-oriented to meat animal-oriented during 1961–2010. Although the CO{sub 2}-eq of CH{sub 4} and N{sub 2}O from manure storage was less than the enteric emissions during 1961–2010 in China, it tended to increase both in beef and dairy cattle, which was mainly driven by the changes in manure management practices. - Highlights: • CH{sub 4} emissions dominated the CO{sub 2}-eq emissions from dairy and beef cattle in China. • Beef herd transition played an important role in CH{sub 4} emissions. • Changes of manure managements increased the manure EFs of CH{sub 4} and N{sub 2}O. • Manure contributed very less to the total CO{sub 2}-eq emissions but tended to grow.« less

Nitrous oxide and methane emissions following application of animal manures to grassland

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

Chadwick, D.R.; Pain, B.F.; Brookman, S.K.E.

2000-02-01

Nitrous oxide (N{sub 2}O) and methane (CH{sub 4}) emissions were measured from grassland following manure applications at three times of the year. Pig (Sus scrofa) slurry and dairy cow (Bos taurus) slurry were applied in April, at equal rates of ammoniacal-N (NH{sub 4}{sup +}-N), and in July, at equal volumetric rates (50 m{sup 3}ha{sup {minus}1}). In October, five manure types were applied to grassland plots at typical application rates: pig slurry, dilute diary cow effluent, pig farm yard manure (FYM), beef FYM and layer manure. Emissions were measured for 20, 22, and 24 d, respectively. In April, greater cumulative emissionsmore » of N{sub 2}O-N were measured following application of dairy cow slurry (1.51 kg ha{sup {minus}1}) than pig slurry (90.77 kg ha{sup {minus}1}). Cumulative CH{sub 4} emissions following application in April were significantly greater from the dairy cow slurry treatment (0.58 kg ha{sup {minus}1}) than the pig slurry treatment (0.13 kg ha{sup {minus}1}) (P < 0.05). In July, significantly greater N{sub 2}O-N emissions resulted from pig slurry-treated plots (0.57 kg ha{sup {minus}1}) than dairy cow slurry-treated plots (0.34 kg ha{sup {minus}1}). Cumulative net CH{sub 4} emissions were very low following July applications (<10 g ha{sup {minus}1}). In October, the lowest N{sub 2}O-N emission resulted from application of dilute dairy effluent, 0.15 kg ha{sup {minus}1}, with the greatest net emission from the application of pig slurry, 0.74 kg ha{sup {minus}1}. Methane emissions were greatest from the plots that received pig FYM, resulting in a mean cumulative net emission of 2.39 kg ha{sup {minus}1}.« less

Large-scale synthesis of ear-like Si{sub 3}N{sub 4} dendrites from SiO{sub 2}/Fe composites and Si powders

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

Wang Feng; Graduate School of the Chinese Academy of Sciences, Beijing 100039; Jin Guoqiang

2008-07-01

Large-scale ear-like Si{sub 3}N{sub 4} dendrites were prepared by the reaction of SiO{sub 2}/Fe composites and Si powders in N{sub 2} atmosphere. The product was characterized by field emission scanning electron microscopy, X-ray diffraction, and transmission electron microscopy. The results reveal that the product mainly consists of ear-like Si{sub 3}N{sub 4} dendrites with crystal structures, which have a length of several microns and a diameter of 100-200 nm. Nanosized ladder-like Si{sub 3}N{sub 4} was also obtained when changing the Fe content in the SiO{sub 2}/Fe composites. The Si{sub 3}N{sub 4} nanoladders have a length of hundreds nanometers to several micronsmore » and a width of 100-300 nm. The ear-like Si{sub 3}N{sub 4} dendrites are formed from a two-step growth process, the formation of inner stem structures followed by the epitaxial growth of secondary branches.« less

A color-tunable luminescent material with functionalized graphitic carbon nitride as multifunctional supports

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

Lu, Jiutian; Cao, Yudong; Fan, Hai

2015-12-15

A color-tunable luminescent material was prepared based on the composition of functionalized graphitic carbon nitride (g-C{sub 3}N{sub 4}) and europium (III). The functionalized g-C{sub 3}N{sub 4} layers not only behave as multifunctional supports including ligand coordinated with europium (III) and a support structure for the formation of the luminescent material, but exhibit excitation wavelength-dependent luminescence, thus the energy transfer between the functionalized g-C{sub 3}N{sub 4} and europium (III) can match very well by controlling the emission wavelength of functionalized g-C{sub 3}N{sub 4}. The as-prepared materials was comprehensively characterized via X-ray photoelectron spectroscopy, Fourier Transform Infrared spectroscopy, X-ray scattering techniques, Ultravioletmore » and Visible spectrophotometer, fluorescence spectrophotometer, thermogravimetric analysis, etc. The luminescent material exhibits multi-color emissions which are consistent with the characteristic emissions of europium (III) and functionalized g-C{sub 3}N{sub 4}, and the photoluminescence quality and density of the europium (III) can be greatly enhanced. The brilliant optical properties of the materials make them suiting for multipurpose applications in practical fields. - Graphical abstract: Schematic illustration of the synthesis and basic composition of the luminescent material. Inset figures were luminescence emission spectra of g-C{sub 3}N{sub 4} (A), europium (III) complex (a) and luminescent material (b) with the same concentration in (B) (K{sub ex}=350 nm) and photographs of (left) H{sub 2}O and (right) the H{sub 2}O dispersion of luminescence emission spectra under 350 nm UV radiation. The energy transfer in the luminescent material matchs very well and it exhibits multi-color emissions simultaneously. The enhanced photoluminescence quality and density of the europium (III) makes them suiting for multipurpose applications in practical fields. - Highlights: • Luminescent material exhibits multi-color emissions when excited by single wavelength. • The energy trsnsfer between functionalized g-C{sub 3}N{sub 4} and europium matches very vell. • Functionalized g-C{sub 3}N{sub 4} exhibits excitation wavelength-depengdent bright blue luminescence. • Functionalized g-C{sub 3}N{sub 4} layer provided as multifunctional supports.« less

Nitrous oxide emissions control by reburning

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

Rutar, T.; Kramlich, J.C.; Malte, P.C.

1996-12-01

Fluidized bed coal combustors emit much higher concentrations of nitrous oxide (N{sub 2}O) than do most other combustion systems. This is of concern because N{sub 2}O is highly stable in the atmosphere, and may contribute to both the greenhouse effect and to stratospheric ozone depletion. In this article laboratory results are presented on N{sub 2}O removal by the reburning (i.e., afterburning) method. The destruction of N{sub 2}O is observed during contact between hot flue gases containing N{sub 2}O and various reburning fuels. A laboratory combustion reactor is used to sequentially generate the hot combustion gas, and to put this gasmore » in contact with N{sub 2}O and reburning fuel under well-characterized conditions. The initial N{sub 2}O in the primary combustion products is between 200 and 350 ppmv (dry). The temperature of the primary combustion products is varied between 1,080 and 1,370 K, and the oxygen level of these gases is varied between 3.3 and 4.8% (dry). Five reburning fuels are tested. The rank order of reburning effectiveness (based on equal heat input by the reburning fuels) is H{sub 2} > CH{sub 4} > C{sub 2}H{sub 4} and C{sub 2}H{sub 6} > CO. Experiments are also performed with the primary combustor operated fuel rich. Without any reburning fuel added, removal of large amounts of N{sub 2}O are obtained when the fuel-air equivalence ratio of the primary combustion is about 1.1. The experimental results are presented, discussed, and compared to chemical kinetic modeling. Also, some discussions of the practical implications is presented.« less

Electrical characterization of the flowing afterglow of N{sub 2} and N{sub 2}/O{sub 2} microwave plasmas at reduced pressure

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

Afonso Ferreira, J.; Stafford, L., E-mail: luc.stafford@umontreal.ca; Leonelli, R.

2014-04-28

A cylindrical Langmuir probe was used to analyze the spatial distribution of the number density of positive ions and electrons as well as the electron energy distribution function (EEDF) in the flowing afterglow of a 6 Torr N{sub 2} and N{sub 2}/O{sub 2} plasma sustained by a propagating electromagnetic surface wave in the microwave regime. In pure N{sub 2} discharges, ion densities were in the mid 10{sup 14} m{sup −3} in the pink afterglow and in the mid 10{sup 12} m{sup −3} early in the late afterglow. In both pink and late afterglows, the ion population was much higher than the electron population,more » indicating non-macroscopically neutral media. The EEDF was close to a Maxwellian with an electron temperature of 0.5 ± 0.1 eV, except in the pink afterglow where the temperature rose to 1.1 ± 0.2 eV. This latter behavior is ascribed to N{sub 2} vibration-vibration pumping in the pink afterglow that increases the concentration of high N{sub 2} vibrational states and thus rises the electron temperature by vibration-electron collisions. After addition of small amounts of O{sub 2} in the nominally pure N{sub 2} discharge, the charged particles densities and average electron energy first strongly increased and then decreased with increasing O{sub 2} concentration. Based on these data and the evolution of the N{sub 2}{sup +}(B) band emission intensities, it is concluded that a significant change in the positive ion composition of the flowing afterglow occurs, going from N{sub 2}{sup +} in nominally pure N{sub 2} discharges to NO{sup +} after addition of trace amounts of O{sub 2} in N{sub 2}.« less

N2O EMISSIONS FROM STREAMS IN THE NEUSE RIVER WATERSHED, NORTH CAROLINA

EPA Science Inventory

The paper presents N₂O emission data from 11 sites in the Neuse River watershed. Emissions were measured using a static surface enclosure technique deployed on eight sites on the main river channel and three tributary sites. Ancillary data collected included dissolved ...

First-principles calculation on electronic structure and optical property of BaSi{sub 2}O{sub 2}N{sub 2}:Eu{sup 2+} phosphor

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

Tong, Zhi-Fang, E-mail: tongzhifang1998@126.com; Wei, Zhan-Long; Xiao, Cheng

The crystal structure, electronic structure and optical properties of BaSi{sub 2}O{sub 2}N{sub 2}:Eu{sup 2+} with varying Eu doping concentrations are computed by the density functional theory (DFT) and compared with experimental results. The results show that the lattice parameters of primitive cells of Ba{sub 1−x}Si{sub 2}O{sub 2}N{sub 2}:Eu{sub x} become smaller and Eu–N bond length shortens as Eu concentration increases. The band structure of Ba{sub 1−x}Si{sub 2}O{sub 2}N{sub 2}:Eu{sub x} exhibits a direct optical band gap and it's propitious to luminescence. The energy differences from the lowest Eu 5d state to the lowest Eu 4f state decrease with increasing Eumore » concentrations. The analysis of simulative absorption spectra indicates that the electron transition from Eu 4f states to 5d states of both Eu and Ba atoms contributes to the absorption of Ba{sub 1−x}Si{sub 2}O{sub 2}N{sub 2}:Eu{sub x}. Under the coupling effect between Eu and Ba, Ba in BaSi{sub 2}O{sub 2}N{sub 2} exhibits longer wavelength absorption and increases absorption efficiency. The emission wavelength is deduced by measuring energy differences from the lowest Eu 5d state to the lowest Eu 4f state, and the result is in good agreement with experimental value within experimental Eu{sup 2+} doping range. - Graphical abstract: The structure and optical property of BaSi{sub 2}O{sub 2}N{sub 2}:Eu{sup 2+} are computed by DFT and its absorption mechanism is analysed. Results show that absorption peak α is from the host lattice absorption. The absorption peaks β, γ and δ are from Eu 4f to Eu 5d and Ba 6s 5d states. The absorption is attributed to the coupling effect of Eu and Ba atom. - Highlights: • The crystal, electronic structure and optical properties of BaSi{sub 2}O{sub 2}N{sub 2}:Eu{sup 2+} are computed by DFT. • The lattice parameters of primitive cells reduces and Eu–N bond length shortens as Eu{sup 2+} increases. • The energy gap from Eu 5d state to Eu 4f state decrease with increasing Eu concentrations. • Both Eu and Ba atoms contributes to the absorption of Ba{sub 1−x}Si{sub 2}O{sub 2}N{sub 2}:Eu{sub x}. • The deduced emission wavelength is in good agreement with experimental value.« less

Soil-atmosphere exchange of nitrous oxide, nitric oxide, and methane under secondary succession of pasture to forest in the Atlantic lowlands of Costa Rica

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

Keller, M.; Reiners, W.A.

We investigated changes in soil-atmosphere flux of CH{sub 4}, N{sub 2}O, and NO resulting from the succession of pasture to forest in the Atlantic lowlands of Costa Rica. We studied a dozen sites intensively for over one year in order to measure rates and to understand controlling mechanisms for gas exchange. CH{sub 4} flux was controlled primarily by soil moisture content. Soil consumption of atmospheric CH{sub 4} was greatest when soils were relatively dry. Forest soils consumed CH{sub 4} while pasture soils which had poor drainage generally produced CH{sub 4}. The seasonal pattern of N{sub 2}O emissions from forest soilsmore » was related exponentially to soil water-filled pore space. Annual average N{sub 2}O emissions correlated with soil exchangeable NO{sub 3}{sup -} concentrations. Soil-atmosphere NO flux was greatest when soils were relatively dry. We found the largest NO emissions from abandoned pasture sites. Combining these data with those from another study in the Atlantic lowlands of Costa Rica that focused on deforestation, we present a 50-year chronosequence of trace gas emissions that extends from natural conditions, through disturbance and natural recovery. The soil-atmosphere fluxes of CH{sub 4} and N{sub 2}O and NO may be restored to predisturbance rates during secondary succession. The changes in trace gas emissions following deforestation, through pasture use and secondary succession, may be explained conceptually through reference to two major controlling factors, nitrogen availability and soil-atmosphere diffusive exchange of gases as it is influenced by soil moisture content and soil compaction. 59 refs., 6 figs., 3 tabs.« less

The use of a paper/wood/plastics mixing as a model waste to study the incineration of municipal solid waste in fluidized beds

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

Desroches-Ducarne, E.; Marty, E.; Martin, G.

1997-12-31

Municipal Solid Waste (MSW) incineration in fluidized beds has recently become the subject of intense research. In this paper, the authors chose to elaborate a simple model waste prepared with 4 of the main MSW components (paper, wood, PE, and PVC). The behaviors of typical French MSW and model waste during their combustion in a fluidized bed incinerator were studied. To establish the comparison, the emissions of NO, N{sub 2}O, SO{sub 2} and HCl were investigated. Moreover, experiments were performed according to statistical experimental designs to examine the effect of various operating parameters including bed temperature, excess air, limestone feedingmore » rate and waste moisture. On a qualitative point of view, the impact of the combustion conditions on the pollutants emissions was found to be the same for the two wastes. Bed temperature and excess air have, in both cases, an important impact on NO and N{sub 2}O emissions. Nitrogen oxides production was also directly related to limestone feed content. Very high sulphur and chlorine retention was obtained when limestone was added at much larger excess to the feed. N{sub 2}O emissions are less important during the model waste combustion. The nitrogen functionality seems to give rise to such a phenomenon. In MSW, nitrogen is included in high molecules which is released for a great part as HCN or remains in char, which are the main sources of N{sub 2}O. To confirm this assumption, tests for measuring the HCN/NH{sub 3} ratio for each fuel were performed.« less

Greenhouse gas emissions from home composting of organic household waste

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

Andersen, J.K., E-mail: jka@env.dtu.d; Boldrin, A.; Christensen, T.H.

2010-12-15

The emission of greenhouse gases (GHGs) is a potential environmental disadvantage of home composting. Because of a lack of reliable GHG emission data, a comprehensive experimental home composting system was set up. The system consisted of six composting units, and a static flux chamber method was used to measure and quantify the GHG emissions for one year composting of organic household waste (OHW). The average OHW input in the six composting units was 2.6-3.5 kg week{sup -1} and the temperature inside the composting units was in all cases only a few degrees (2-10 {sup o}C) higher than the ambient temperature.more » The emissions of methane (CH{sub 4}) and nitrous oxide (N{sub 2}O) were quantified as 0.4-4.2 kg CH{sub 4} Mg{sup -1} input wet waste (ww) and 0.30-0.55 kg N{sub 2}O Mg{sup -1} ww, depending on the mixing frequency. This corresponds to emission factors (EFs) (including only CH{sub 4} and N{sub 2}O emissions) of 100-239 kg CO{sub 2}-eq. Mg{sup -1} ww. Composting units exposed to weekly mixing had the highest EFs, whereas the units with no mixing during the entire year had the lowest emissions. In addition to the higher emission from the frequently mixed units, there was also an instant release of CH{sub 4} during mixing which was estimated to 8-12% of the total CH{sub 4} emissions. Experiments with higher loads of OHW (up to 20 kg every fortnight) entailed a higher emission and significantly increased overall EFs (in kg substance per Mg{sup -1} ww). However, the temperature development did not change significantly. The GHG emissions (in kg CO{sub 2}-eq. Mg{sup -1} ww) from home composting of OHW were found to be in the same order of magnitude as for centralised composting plants.« less

Impact of nitrate-enhanced leachate recirculation on gaseous releases from a landfill bioreactor cell

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

Tallec, G.; Bureau, C.; Peu, P.

2009-07-15

This study evaluates the impact of nitrate injection on a full scale landfill bioreactor through the monitoring of gaseous releases and particularly N{sub 2}O emissions. During several weeks, we monitored gas concentrations in the landfill gas collection system as well as surface gas releases with a series of seven static chambers. These devices were directly connected to a gas chromatograph coupled to a flame ionisation detector and an electron capture detector (GC-FID/ECD) placed directly on the field. Measurements were performed before, during and after recirculation of raw leachate and nitrate-enhanced leachate. Raw leachate recirculation did not have a significant effectmore » on the biogas concentrations (CO{sub 2}, CH{sub 4} and N{sub 2}O) in the gas extraction network. However, nitrate-enhanced leachate recirculation induced a marked increase of the N{sub 2}O concentrations in the gas collected from the recirculation trench (100-fold increase from 0.2 ppm to 23 ppm). In the common gas collection system however, this N{sub 2}O increase was no more detectable because of dilution by gas coming from other cells or ambient air intrusion. Surface releases through the temporary cover were characterized by a large spatial and temporal variability. One automated chamber gave limited standard errors over each experimental period for N{sub 2}O releases: 8.1 {+-} 0.16 mg m{sup -2} d{sup -1} (n = 384), 4.2 {+-} 0.14 mg m{sup -2} d{sup -1} (n = 132) and 1.9 {+-} 0.10 mg m{sup -2} d{sup -1} (n = 49), during, after raw leachate and nitrate-enhanced leachate recirculation, respectively. No clear correlation between N{sub 2}O gaseous surface releases and recirculation events were evidenced. Estimated N{sub 2}O fluxes remained in the lower range of what is reported in the literature for landfill covers, even after nitrate injection.« less

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

Ishimoto, M.; Meng, C.; Romick, G.J.

The UV spectra over the southern hemisphere nightside auroral oval have been obtained from an AFGL spectral/photometric experiment on board the low-altitude polar-orbiting S3-4 satellite. A detailed analysis of nightside auroral spectra from seven orbits between mid-May and June 1978 was performed to estimate the average energy and total energy flux of incident electrons. This study was based on observations of the N{sub 2} LBH (3-10) (1928-A) band and the N{sub 2} VK (0-5) (2604 A) band emission intensities and the application of model calculations. Comparison of the estimated quantities with the statistical satellite measurement of incident particles indicates thatmore » the LBH (3-10) band emission intensity can be used to estimate the total energy flux of incident electrons, similar to the N{sub 2}(+) 1N (0-0) (3914 A) band emission intensity in the visible region. In addition, the ratio of the LBH (3-10) to the VK (0-5) bande mission intensities indicates the average energy of incident auroral electrons in much the same way that the N{sub 2}(+)1N (0-0) and O I (6300 A) emission ratio does in the visible region. This study shows the use of different constituent emissions, model calculations, and synthetic spectra to infer the inherent possibilities in these types of studies.« less

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

Ishimoto, M.; Meng, C.; Romick, G.J.

The UV spectra over the southern hemisphere nightside auroral oval have been obtained from an AFGL spectral/photometric experiment on board the low-altitude polar-orbiting S3--4 satellite. A detailed analysis of nightside auroral spectra from seven orbits between mid-May and June 1978 was performed to estimate the average energy and total energy flux of incident electrons. This study was based on observations of the N/sub 2/ LBH (3--10) (1928 A) band and the N/sub 2/ VK (0--5) (2604 A) band emission intensities and the application of model calculations by Strickland et al. (1983) and Daniell and Strickland (1986). Comparison of the estimatedmore » quantities with the statistical satellite measurement of incident particles by Hardy et al. (1985) indicates that the LBH (3--10) band emission intensity can be used to estimate the total energy flux of incident electrons, similar to the N/sub 2//sup +/ 1N (0--0) (3914 A) band emission intensity in the visible region. In addition, the ratio of the BLH (3--10) to the VK (0--5) band emission intensities indicates the average energy of incident auroral electrons in much the same way that the N/sub 2//sup +/ IN (0--0) and O I (6300 A) emission ratio does in the visible region.« less

Synthesis and photoluminescent properties of Sr{sub (1−x)}Si{sub 2}O{sub 2}N{sub 2}: xEu{sup 2+} phosphor prepared by polymer metal complex method for WLEDs applications

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

Hassan, Dhia A., E-mail: dhia_hassan@yahoo.com; Department of Chemistry, College of Education for Pure Science, University of Basrah, Basrah 61004; Xu, Jian

2016-07-15

Highlights: • SrSi{sub 2}O{sub 2}N{sub 2}: Eu{sup 2+} phosphor was prepared by polymer metal complex (pechini method). • The annealing time was decreased from 6 h in solid state method to 3 h. • The particles are crystalline and dispersed well with average size 6.5 μm. - Abstract: Green emitting Sr{sub (1−x)}Si{sub 2}O{sub 2}N{sub 2}: xEu{sup 2+} (x = 0, 0.02, 0.04, 0.06, 0.08 and 0.1) phosphors were synthesized by polymer metal complex or pechini method. The XRD results confirm the formation of a pure phase at 1400 °C for 3 h. The SEM and particles size results indicate thatmore » the prepared phosphor consists of a polyhedral crystalline shape with well dispersed and the average particle size around 6.5 μm. The maximum PL intensity was found at 0.04% Eu{sup 2+} with a wide emission band between 460 and 640 nm and a green emission peak at 531.4 nm. The external quantum efficiency of 0.04% Eu{sup 2+} sample was 43.13%. The results indicate that pechini method is an alternative way and close in efficiency to the solid state method to prepare SrSi{sub 2}O{sub 2}N{sub 2} phosphor with higher homogeneity and more uniform size distribution for near UV and blue region applications for white light emitting diodes WLEDs.« less

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

Hume, E.E. Jr.

The green line (5577[angstrom]) is a bright, persistent component of the visible airglow produced by an electric quadrupole transition from the meta-stable second excited state ([sup 1]S[sub 0]) to the first excited state ([sup 1]D[sub 2]) of atomic oxygen. In this thesis, production and loss mechanisms important to the F-region dayglow 5577[angstrom] emission are investigated. Four major source reactions need to be incorporated in the modeling of the emission profile, photoelectron impact on atomic oxygen, dissociative recombination of O[sup +][sub 2], quenching of N[sub 2](A[sup 3][Sigma][sub u][sup +]) by atomic oxygen, and photo-dissociation of O[sub 2]. For some of themore » reactions, the properties of the rate coefficients, branching ratios, and cross sections are not well known. Models are used to determine the rate coefficients, branching ratios, and cross sections for these reactions. The impact of photoelectrons on atomic oxygen is the primary source of 5577[angstrom] dayglow emission in the thermosphere. The quenching of N[sub 2](A) by atomic oxygen is an important source of the 5577[angstrom] emission at the peak in the layer. The total quenching rate was determined using a vibrational model and a band model for N[sub 2] to study emissions at 3371[angstrom] from the Atmosphere Explorer satellite. The value of the rate coefficient deduced here agrees well with experimental values by Piper and Caledonia (1981) and Thomas and Kaufman (1985). The effective branching ratio determined by this study tends to support the results from Piper (1982) and De Souza et al. (1985). The effect of the distribution of the vibrational population of the N[sub 2](A[sup 3][Sigma][sub u][sup +]) state on the branching ratio is also discussed. The extension of the dayglow photochemistry into the twilight is also investigated. The model developed for the dayglow can reasonably reproduce the rapidly changing twilight emissions.« less

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

Dong, Wen-Wen; Xia, Liang; Peng, Zhen

Under solvothermal conditions, the reactions of Co{sup II}/Zn{sup II} ions with bent ligand 3-(pyridin-4-yl)-5-(pyrazin-2-yl)-1H-1,2,4-triazole (4-Hpzpt) afford two compounds {[M(4-pzpt)_2] guest}{sub n} (guest=H{sub 2}O, M=Co{sup II} (1), Zn{sup II} (2)). Both compounds are the thermally and hydrolytically robust 4-connected 3D NbO framework, which formed by double helical chains to give rise to 1D hollow nanochannel with uncoordinated nitrogens completely exposed on the pore surface. Compound 1 exhibits improved N{sub 2}, CO{sub 2} and H{sub 2} uptake capacities, while compound 2 displays the strong luminescent emission with obvious red shift. - Graphical abstract: Two 2-fold interpenetrated NbO-type MOFs with 1D nanochannel weremore » synthesized. Compound 1 exhibits improved N{sub 2}, CO{sub 2} and H{sub 2} uptake capacities, while compound 2 displays the strong fluorescent emission with obvious red shift. Display Omitted.« less

Cofiring lignite with hazelnut shell and cotton residue in a pilot-scale fluidized bed combustor

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

Zuhal Gogebakan; Nevin Selcuk

In this study, cofiring of high ash and sulfur content lignite with hazelnut shell and cotton residue was investigated in 0.3 MWt METU Atmospheric Bubbling Fluidized Bed Combustion (ABFBC) Test Rig in terms of combustion and emission performance of different fuel blends. The results reveal that cofiring of hazelnut shell and cotton residue with lignite increases the combustion efficiency and freeboard temperatures compared to those of lignite firing with limestone addition only. CO{sub 2} emission is not found sensitive to increase in hazelnut shell and cotton residue share in fuel blend. Cofiring lowers SO{sub 2} emissions considerably. Cofiring of hazelnutmore » shell reduces NO and N{sub 2}O emissions; on the contrary, cofiring cotton residue results in higher NO and N{sub 2}O emissions. Higher share of biomass in the fuel blend results in coarser cyclone ash particles. Hazelnut shell and cotton residue can be cofired with high ash and sulfur-containing lignite without operational problems. 32 refs., 12 figs., 11 tabs.« less

Interfacial RhO{sub x}/CeO{sub 2} sites as locations for low temperature N{sub 2}O dissociation

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

Cunningham, J.; Hickey, J.N.; Soria, J.

Temperatures required for extensive N{sub 2}O dissociation to N{sub 2}, or to N{sub 2} plus O{sub 2}, over 0.5% RhO{sub x}/CeO{sub 2} materials, and over polycrystalline Rh{sub 2}O{sub 3} or CeO{sub 2}, are compared for preoxidised and for prereduced samples on the basis of conversions achieved in pulsed-reactant, continuous-flow and recirculatory microcatalytic reactors. Influences of sample prereduction or preoxidation upon those measurements and upon results from parallel ESR and FTIR studies of N{sub 2}O interactions with such materials are presented and compared. Over partially reduced 0.5% RhO{sub x}/CeO{sub 2} materials complete dissociation of N{sub 2}O pulses to N{sub 2} plusmore » O{sub 2} is obtained at temperatures 50-100{degrees} lower than those required for extensive dissociation over prereduced Rh{sub 2}O{sub 3}. Furthermore, N{sub 2} was the sole product from the latter. Higher ongoing N{sub 2}O conversions to N{sub 2} plus O{sub 2} at 623 K over 0.5% Rh/CeO{sub 2} in pulsed-reactant than in continuous-flow mode point to regeneration of active sites under helium flushing between pulses. The TPD profile for dioxygen release from Rhodia containing samples at temperatures 350-550 K is presented. ESR measurements reveal complementary effects of outgassings at temperatures, T{sub v}, {ge} 573 K upon the availability at RhO{sub x}/CeO{sub 2} surfaces of electron-excess sites reactive towards N{sub 2}O. Differences from observations over Rh{sub 2}O{sub 3} and CeO{sub 2} can be understood by attributing the low-temperature activity of RhO{sub x}/CeO{sub 2} to electron excess sites at microinterfaces between the dispersed Rhodia component and the Ceria support.« less

Theoretical study of the interaction of N/sub 2/ with water molecules. (H/sub 2/O)/sub n/:N/sub 2/, n = 1--8

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

Curtiss, L.A.; Eisgruber, C.L.

1984-03-01

Ab initio molecular orbital calculations including correlation energy have been carried out on the interaction of a single H/sub 2/O molecule with N/sub 2/. The potential energy surface for H/sub 2/O:N/sub 2/ is found to have a minimum corresponding to a HOH xxx N/sub 2/ structure with a weak (<2 kcal mol/sup -1/) hydrogen bond. A second, less stable, configuration corresponding to a H/sub 2/O xxx N/sub 2/ structure with N/sub 2/ bonded side on to the oxygen of H/sub 2/O was found to be either a minimum or a saddle point in the potential energy surface depending on themore » level of calculation. The minimal STO-3G basis set was used to investigate the interaction of up to eight H/sub 2/O molecules with N/sub 2/. Two types of clusters, one containing only HOH xxx N/sub 2/ interactions and the other containing both HOH xxxN/sub 2/ and H/sub 2/O xxx N/sub 2/ interactions, were investigated for (N/sub 2/:(H/sub 2/O)/sub n/, n = 2--8).« less

CHEMICAL IMAGING OF THE CO SNOW LINE IN THE HD 163296 DISK

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

Qi, Chunhua; Öberg, Karin I.; Andrews, Sean M.

2015-11-10

The condensation fronts (snow lines) of H{sub 2}O, CO, and other abundant volatiles in the midplane of a protoplanetary disk affect several aspects of planet formation. Locating the CO snow line, where the CO gas column density is expected to drop substantially, based solely on CO emission profiles, is challenging. This has prompted an exploration of chemical signatures of CO freeze-out. We present ALMA Cycle 1 observations of the N{sub 2}H{sup +} J = 3−2 and DCO{sup +} J = 4−3 emission lines toward the disk around the Herbig Ae star HD 163296 at ∼0.″5 (60 AU) resolution, and evaluatemore » their utility as tracers of the CO snow line location. The N{sub 2}H{sup +} emission is distributed in a ring with an inner radius at 90 AU, corresponding to a midplane temperature of 25 K. This result is consistent with a new analysis of optically thin C{sup 18}O data, which implies a sharp drop in CO abundance at 90 AU. Thus N{sub 2}H{sup +} appears to be a robust tracer of the midplane CO snow line. The DCO{sup +} emission also has a ring morphology, but neither the inner nor the outer radius coincide with the CO snow line location of 90 AU, indicative of a complex relationship between DCO{sup +} emission and CO freeze-out in the disk midplane. Compared to TW Hya, CO freezes out at a higher temperature in the disk around HD 163296 (25 versus 17 K in the TW Hya disk), perhaps due to different ice compositions. This highlights the importance of actually measuring the CO snow line location, rather than assuming a constant CO freeze-out temperature for all disks.« less

Polymorph (C{sub 2}N{sub 2}H{sub 10}){sub 0.5}RE{sub 3}F{sub 10}·xH{sub 2}O (RE = Ho-Lu, Y) and REF{sub 3} nanocrystals: Hydrothermal synthesis, characterization and luminescence

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

Jia, Li-Ping; Zhang, Qiang; Yan, Bing, E-mail: byan@tongji.edu.cn

Graphical abstract: A hydrothermal system is developed to prepare one new polymorph of (C{sub 2}N{sub 2}H{sub 10}){sub 0.5}RE{sub 3}F{sub 10}·xH{sub 2}O and known rare earth fluorides involving REF{sub 3} nanocrystals under mild condition. Highlights: ► A new polymorph of (C{sub 2}N{sub 2}H{sub 10}){sub 0.5}RE{sub 3}F{sub 10}·xH{sub 2}O has been synthesized. ► The RE{sup 3+} radius decides the shape evolution and phase control for REF{sub 3} NCs. ► The RE{sup 3+} radius has influence on the microstructure and morphology of REF{sub 3} NCs. -- Abstract: In this paper, a solvents-thermal system is developed to prepare one new polymorph of (C{sub 2}N{submore » 2}H{sub 10}){sub 0.5}Ho{sub 3}F{sub 10}·xH{sub 2}O and rare earth fluorides REF{sub 3} nanocrystals under mild condition. It is found that the ionic radius of RE{sup 3+} is the key factor responsible for the shape evolution and phase control for rare earth fluorides nanocrystals at selected temperatures, which has an influence on the microstructure and morphology of the products to some extent. With the increase of the atomic number, the shape of fluoride changes from hexagonal REF{sub 3} phase (RE = La, Sm) to orthorhombic REF{sub 3} phase (RE = Eu-Dy), and finally to diamond structure (C{sub 2}N{sub 2}H{sub 10}){sub 0.5}Ho{sub 3}F{sub 10}·xH{sub 2}O (RE = Ho, Er, Tm, Yb, Lu, Y). In addition, the characteristic energy level transition {sup 5}D{sub 0}–{sup 7}F{sub 1} of Eu{sup 3+} splits into 585 and 591 nm emission peaks, and the dominant peak is the orange emission at 591 nm.« less

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

Suuberg, E.M.; Lilly, W.D.; Aarna, I.

This project is concerned with the mechanism of reduction of both NO and N{sub 2}O by carbons. It was recognized some years ago that NO formed during fluidized bed coal combustion can be heterogeneously reduced in-situ by the carbonaceous solid intermediates of combustion. This has been recently supplemented by the knowledge that heterogeneous reaction with carbon can also play an important role in reducing emissions of N{sub 2}, but that the NO-carbon reactions might also contribute to formation of N{sub 2}. The precise role of carbon in N{sub 2} reduction and formation has yet to be established. Interest in themore » N{sub 2} and N{sub 2}O-char reactions has been significant in connection with both combustor modeling, as well as in design of post-combustion NO{sub x} control strategies. In our studies, a DuPont thermogravimetric analyzer (TGA) is used for the char reactivity studies. The temperature and mass are recorded as function of time, using a Macintosh computer and software for simultaneous apparatus control and data acquisition. Specific surface areas of char samples were determined by the N{sub 2} BET method at 77 K. A standard flow-type adsorption device (Quantasorb) was used for the measurements. Prior to surface area analysis, all samples were outgassed in a flow of nitrogen at 573 K for 3 hours. The carbonaceous solids used were resin char, graphite, coconut char and a Wyodak coal char. As was noted in the last report, carbons derived from different original materials show quite similar behaviors, in terms of the trends, but there are significant differences in actual reaction rates. It was shown that the spread of the reaction rate data from different studies, when expressed on a mass of carbon reactant- or surface area-basis, was almost the same.« less

Environmental assessment of NH/sub 3/ injection for an industrial package boiler. Volume 1. Technical results. Final report, January 1983-January 1984

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

Castaldini, C.; DeRosier, R.; Waterland, L.R.

1986-02-01

The report discusses emission results from comprehensive flue gas sampling of a gas- and oil-fired industrial boiler equipped with Exxon's Thermal DeNO/sub x/ Ammonia Injection Process for NO/sub x/ reduction. Comprehensive emission measurements included continuous monitoring of flue gas emissions; source assessment sampling system (SASS) tests; EPA Method 5/17 for solid and condensible particulate emissions and ammonia emissions; controlled condensation system for SO/sub 2/ and SO/sub 3/; and N/sub 2/O emission sampling. Ammonia injection at a NH/sub 3//NO molar ratio of 2.52 gave a NO/sub x/ reduction of 41% from an uncontrolled level of 234 ppm to a controlled levelmore » of 137 ppm. NH/sub 3/ emissions increased from 11 ppm for the baseline to an average of 430 ppm for ammonia injection. Nitrous oxide, N/sub 2/O was reduced 68% from a 50 ppm baseline level to a 17 ppm controlled level. Total particulate emissions increased by an order of magnitude from a baseline of 17.7 ng/J to a controlled level of 182 ng/J. The increase is in part attributed to formation of ammonia sulfate and bisulfate from residual ammonia and SO/sub x/. Total organic emissions were at a moderate level and showed a relative concentration in the nonvolatile category. Organic emissions of CO and trace inorganic elements were not significantly affected by ammonia injection.« less

Integrated capture of fossil fuel gas pollutants including CO.sub.2 with energy recovery

DOEpatents

Ochs, Thomas L [Albany, OR; Summers, Cathy A [Albany, OR; Gerdemann, Steve [Albany, OR; Oryshchyn, Danylo B [Philomath, OR; Turner, Paul [Independence, OR; Patrick, Brian R [Chicago, IL

2011-10-18

A method of reducing pollutants exhausted into the atmosphere from the combustion of fossil fuels. The disclosed process removes nitrogen from air for combustion, separates the solid combustion products from the gases and vapors and can capture the entire vapor/gas stream for sequestration leaving near-zero emissions. The invention produces up to three captured material streams. The first stream is contaminant-laden water containing SO.sub.x, residual NO.sub.x particulates and particulate-bound Hg and other trace contaminants. The second stream can be a low-volume flue gas stream containing N.sub.2 and O.sub.2 if CO2 purification is needed. The final product stream is a mixture comprising predominantly CO.sub.2 with smaller amounts of H.sub.2O, Ar, N.sub.2, O.sub.2, SO.sub.X, NO.sub.X, Hg, and other trace gases.

The quenching effect of hydrogen on the nitrogen in metastable state in atmospheric-pressure N{sub 2}-H{sub 2} microwave plasma torch

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

Li, Shou-Zhe, E-mail: lisz@dlut.edu.cn; Zhang, Xin; Chen, Chuan-Jie

2014-07-15

The atmospheric-pressure microwave N{sub 2}-H{sub 2} plasma torch is generated and diagnosed by optical emission spectroscopy. It is found that a large amount of N atoms and NH radicals are generated in the plasma torch and the emission intensity of N{sub 2}{sup +} first negative band is the strongest over the spectra. The mixture of hydrogen in nitrogen plasma torch causes the morphology of the plasma discharge to change with appearance that the afterglow shrinks greatly and the emission intensity of N{sub 2}{sup +} first negative band decreases with more hydrogen mixed into nitrogen plasma. In atmospheric-pressure microwave-induced plasma torch,more » the hydrogen imposes a great influence on the characteristics of nitrogen plasma through the quenching effect of the hydrogen on the metastable state of N{sub 2}.« less

Method for synthesizing N.sub.2 O.sub.5

DOEpatents

McGuire, Raymond R.; Coon, Clifford L.; Harrar, Jackson E.; Pearson, Richard K.

1985-01-01

A method and apparatus for electrochemically synthesizing N.sub.2 O.sub.5 includes oxidizing a solution of N.sub.2 O.sub.4 /HNO.sub.3 at an anode, while maintaining a controlled potential between the N.sub.2 O.sub.4 /HNO.sub.3 solution and the anode. A potential of about 1.35 to 2.0 V vs. SCE is preferred, while a potential of about 1.80 V vs. SCE is most preferred. Thereafter, the N.sub.2 O.sub.5 is reacted with either 1.5-diacetyl-3,7-dinitro-1,3,5,7-tetraazacyclooctane (DADN) or 1,3,5,7-tetraacetyl-1,3,5,7-tetraazacyclooctane (TAT) to form cyclotetramethylenetetraamine (HMX).

Synthesis and characterization of g-C{sub 3}N{sub 4}/Cu{sub 2}O composite catalyst with enhanced photocatalytic activity under visible light irradiation

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

Peng, Biyu; Zhang, Shengsen; Yang, Siyuan

2014-08-15

The prepared g-C{sub 3}N{sub 4}/Cu{sub 2}O composite exhibited the enhanced photocatalytic activity under visible-light irradiation due to the stronger ability in separation of electron–hole pairs, which was proven by the transient photocurrent measurement. - Highlights: • The coupled Cu{sub 2}O with g-C{sub 3}N{sub 4} of narrow-band-gap semiconductor has been designed. • g-C{sub 3}N{sub 4}/Cu{sub 2}O is prepared via an alcohol-aqueous based on chemical precipitation method. • g-C{sub 3}N{sub 4}/Cu{sub 2}O exhibits the enhanced photocatalytic activity under visible-light. • The enhanced photocatalytic activity is proven by the transient photocurrent test. • A mechanism for the visible-light-driven photocatalysis of g-C{sub 3}N{sub 4}/Cu{submore » 2}O is revealed. - Abstract: To overcome the drawback of low photocatalytic efficiency brought by electron–hole pairs recombination and narrow photo-response range, a novel g-C{sub 3}N{sub 4}/Cu{sub 2}O composite photocatalyst was designed and prepared successfully. Compared with bare Cu{sub 2}O and g-C{sub 3}N{sub 4}, the g-C{sub 3}N{sub 4}/Cu{sub 2}O composite exhibited significantly enhanced photocatalytic activity for acid orange-II (AO-II) degradation under visible light irradiation. Based on energy band positions, the mechanism of enhanced visible-light photocatalytic activity was proposed.« less

Facile synthesis of nanorod-type graphitic carbon nitride/Fe{sub 2}O{sub 3} composite with enhanced photocatalytic performance

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

Wang, Jiangpeng; Li, Changqing; Cong, Jingkun

2016-06-15

Here we report a facile synthesis of nanorod-type graphitic carbon nitride/Fe{sub 2}O{sub 3} composite (Fe{sub 2}O{sub 3}-g-C{sub 3}N{sub 4}) by using Fe-melamine supramolecular framework as precursor. The chemical and optical properties of the nanocomposites are well-characterized. The Fe{sub 2}O{sub 3}-g-C{sub 3}N{sub 4} nanocomposite demonstrated excellent photocatalytic activities under visible light due to the efficient utilization of sunlight and the construction of Z-scheme electron transfer pathway. The results indicated that it could be a promising approach for the preparation of efficient g-C{sub 3}N{sub 4} nanocomposites photocatalysts by using metal-melamine supramolecular framework as precursors. - Graphical abstract: Nanorod-type graphitic carbon nitride/Fe{sub 2}O{submore » 3} composite (Fe{sub 2}O{sub 3}-g-C{sub 3}N{sub 4}) was synthesized by using Fe-melamine supramolecular framework as precursor. The Fe{sub 2}O{sub 3}-g-C{sub 3}N{sub 4} nanocomposite demonstrated excellent photocatalytic activities under visible light. Display Omitted - Highlights: • Nanorod-type graphitic carbon nitride/Fe{sub 2}O{sub 3} composite (Fe{sub 2}O{sub 3}-g-C{sub 3}N{sub 4}) was synthesized. • Fe{sub 2}O{sub 3}-g-C{sub 3}N{sub 4} showed strong optical absorption in the visible-light region. • The Fe{sub 2}O{sub 3}-g-C{sub 3}N{sub 4} nanocomposite demonstrated excellent photocatalytic activities.« less

Modeling of chemical reactions in afterburning for the reduction of N{sub 2}O

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

Gustavsson, L.; Glarborg, P.; Leckner, B.

1996-08-01

Afterburning involves burning a secondary fuel in the flue gases from a fluidized bed combustor to raise the temperature, and thereby decrease the emission of N{sub 2}O. Tests in a 12-MW circulating fluidized bed boiler used the cyclone as an afterburning combustor. The results from these tests are analyzed by chemical kinetic calculations with homogeneous hydrocarbon and nitrogen chemistry. Furthermore, a study is made of the influence on the calculation of particles in the flue gases. The deviation between calculated and measured data is small at high temperatures, but increases at the lower temperatures investigated. The influence of particles ismore » predicted to be small under conditions prevailing in the cyclone.« less

Method and apparatus for synthesizing HMX and N/sub 2/O/sub 5/. [Patent application; cyclotetramethylenetetraamine

DOEpatents

McGuire, R.R.; Coon, C.L.; Harrar, J.E.; Pearson, R.K.

1982-07-20

A method and apparatus for electrochemically synthesizing N/sub 2/O/sub 5/ includes oxidizing a solution of N/sub 2/O/sub 4//HNO/sub 3/ at an anode, while maintaining a controlled potential between the N/sub 2/O/sub 4//HNO/sub 3/ solution and the anode. A potential of about 1.35 to 2.0V vs. SCE is preferred, while a potential of about 1.80V vs. SCE is most preferred. Thereafter, the N/sub 2/O/sub 5/ is reacted with either 1.5-diacetyl-3,7-dinitro-1,3,5,7-tetraazacyclooctane (DADN) or 1,3,5,7-tetraacetyl-1,3,5,7-tetraazacyclooctane (TAT) to form cyclotetramethylenetetraamine (HMX).

Synergetic effect of MoS{sub 2} and g-C{sub 3}N{sub 4} as cocatalysts for enhanced photocatalytic H{sub 2} production activity of TiO{sub 2}

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

Yang, Xixian; Huang, Hongyu, E-mail: huanghy@ms.giec.ac.cn; Kubota, Mitsuhiro

Highlights: • A hydrogen evolution reaction of g-C{sub 3}N{sub 4}/MoS{sub 2}/TiO{sub 2} photocatalyst was synthesized. • g-C{sub 3}N{sub 4}/MoS{sub 2}/TiO{sub 2} presents highly efficient H{sub 2} evolution without noble metals. • The effect of g-C{sub 3}N{sub 4} and MoS{sub 2} co-catalyst content in the composites was studied. • The mechanism of g-C{sub 3}N{sub 4}/MoS{sub 2}/TiO{sub 2} photocatalyst under UV–vis light was discussed. - Abstract: In this paper, we report a new g-C{sub 3}N{sub 4}/MoS{sub 2}/TiO{sub 2} composite material as a high-performance photocatalyst for H{sub 2} evolution. Without a noble-metal cocatalyst, the g-C{sub 3}N{sub 4}/MoS{sub 2}/TiO{sub 2} composite reaches a highmore » H{sub 2} production rate of 125 μmol h{sup −1} when the content of the g-C{sub 3}N{sub 4}/MoS{sub 2} cocatalyst is 1.0 wt.% and the content of g-C{sub 3}N{sub 4} in this cocatalyst is 10 wt.%. This unusual photocatalytic activity is attributed to the positive synergetic effect between the MoS{sub 2} and g-C{sub 3}N{sub 4} components in this cocatalyst, which serve as an electron collector and a source of active adsorption sites, respectively.« less

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

Cui, Lin; Hu, Meng; Wang, Qianqian

Exploration of novel hard metastable phases of silicon nitride was performed using a recently developed particle-swarm optimization method within the CALYPSO software package. Three potential hard metastable phases of t-Si{sub 3}N{sub 4}, m-Si{sub 3}N{sub 4}, and o-Si{sub 3}N{sub 4} were predicted. These phases are mechanically and dynamically stable at ambient pressure based on their elastic constants and phonon dispersions. t-Si{sub 3}N{sub 4} and m-Si{sub 3}N{sub 4} exhibit lower energies than γ-Si{sub 3}N{sub 4} at pressures below 2.5 GPa and 2.9 GPa, respectively, which promise that the formers could be obtained by quenching from γ-Si{sub 3}N{sub 4}. o-Si{sub 3}N{sub 4} ismore » a better high-pressure metastable phase than CaTi{sub 2}O{sub 4}-type Si{sub 3}N{sub 4} proposed by Tatsumi et al. and it can come from the transition of γ-Si{sub 3}N{sub 4} under 198 GPa. The theoretical band gaps of t-Si{sub 3}N{sub 4}, m-Si{sub 3}N{sub 4}, and o-Si{sub 3}N{sub 4} at ambient pressure were 3.15 eV, 3.90 eV, and 3.36 eV, respectively. At ambient pressure, the Vickers hardness values of t-Si{sub 3}N{sub 4} (32.6 GPa), m-Si{sub 3}N{sub 4} (31.5 GPa), and o-Si{sub 3}N{sub 4} (36.1 GPa) are comparable to β-Si{sub 3}N{sub 4} and γ-Si{sub 3}N{sub 4}. With the pressure increasing, t-Si{sub 3}N{sub 4}, m-Si{sub 3}N{sub 4}, and o-Si{sub 3}N{sub 4} will change from the brittle to ductile state at about 15.7 GPa, 7.3 GPa and 28.9 GPa, respectively. - Graphical abstract: This figure shows the crystal structures of three Si{sub 3}N{sub 4} predicted in this manuscript, and left to right: t-Si{sub 3}N{sub 4}, m-Si{sub 3}N{sub 4} and o-Si{sub 3}N{sub 4}. - Highlights: • We explored three metastable phases of Si{sub 3}N{sub 4} — t-Si{sub 3}N{sub 4}, m-Si{sub 3}N{sub 4}, and o-Si{sub 3}N{sub 4}. • The enthalpies of t and m- are much lower than that of γ at ambient pressure. • ois one further high pressure phase than γ. • o-Si{sub 3}N{sub 4} is the most hardest phase in Si{sub 3}N4 system. • Increasing pressure will change them from brittle to ductile state.« less

Effects of phosphogypsum and superphosphate on compost maturity and gaseous emissions during kitchen waste composting

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

Yang, Fan; Beijing Municipal Research Institute of Environmental Protection, Beijing 100037; Li, Guoxue, E-mail: yangfan19870117@126.com

2015-02-15

Highlights: • Effect of phosphogypsum and superphosphate on composting gas emissions was studied. • The reduction mechanisms of composting gas were clarified in this study. • No negative effect was caused on maturity with phosphogypsum and superphosphate. • CH{sub 4} and NH{sub 3} emission was decreased with phosphogypsum and superphosphate addition. • GHG decreased by 17.4% and 7.3% with phosphogypsum and superphosphate addition. - Abstract: This study investigated the effects of phosphogypsum and superphosphate on the maturity and gaseous emissions of composting kitchen waste. Two amended compost treatments were conducted using phosphogypsum and superphosphate as additives with the addition ofmore » 10% of initial raw materials (dry weight). A control treatment was also studied. The treatments were conducted under aerobic conditions in 60-L reactors for 35 days. Maturity indexes were determined, and continuous measurements of CH{sub 4}, N{sub 2}O, and NH{sub 3} were taken. Phosphogypsum and superphosphate had no negative effects on compost maturity, although superphosphate inhibited the temperature rise in the first few days. The addition of phosphogypsum and superphosphate drastically reduced CH{sub 4} emissions (by 85.8% and 80.5%, respectively) and decreased NH{sub 3} emissions (by 23.5% and 18.9%, respectively). However, a slight increase in N{sub 2}O emissions (by 3.2% and 14.8%, respectively) was observed. Composting with phosphogypsum and superphosphate reduced total greenhouse gas emissions by 17.4% and 7.3% respectively.« less

Communication: Towards catalytic nitric oxide reduction via oligomerization on boron doped graphene

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

Cantatore, Valentina, E-mail: valcan@chalmers.se; Panas, Itai

We use density functional theory to describe a novel way for metal free catalytic reduction of nitric oxide NO utilizing boron doped graphene. The present study is based on the observation that boron doped graphene and O—N=N—O{sup −} act as Lewis acid-base pair allowing the graphene surface to act as a catalyst. The process implies electron assisted N=N bond formation prior to N—O dissociation. Two N{sub 2} + O{sub 2} product channels, one of which favoring N{sub 2}O formation, are envisaged as outcome of the catalytic process. Besides, we show also that the N{sub 2} + O{sub 2} formation pathwaysmore » are contrasted by a side reaction that brings to N{sub 3}O{sub 3}{sup −} formation and decomposition into N{sub 2}O + NO{sub 2}{sup −}.« less

Astrochemical Properties of Planck Cold Clumps

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

Tatematsu, Ken’ichi; Sanhueza, Patricio; Nguyễn Lu’o’ng, Quang

We observed 13 Planck cold clumps with the James Clerk Maxwell Telescope/SCUBA-2 and with the Nobeyama 45 m radio telescope. The N{sub 2}H{sup +} distribution obtained with the Nobeyama telescope is quite similar to SCUBA-2 dust distribution. The 82 GHz HC{sub 3}N, 82 GHz CCS, and 94 GHz CCS emission are often distributed differently with respect to the N{sub 2}H{sup +} emission. The CCS emission, which is known to be abundant in starless molecular cloud cores, is often very clumpy in the observed targets. We made deep single-pointing observations in DNC, HN{sup 13}C, N{sub 2}D{sup +}, and cyclic-C{sub 3}H{sub 2}more » toward nine clumps. The detection rate of N{sub 2}D{sup +} is 50%. Furthermore, we observed the NH{sub 3} emission toward 15 Planck cold clumps to estimate the kinetic temperature, and confirmed that most targets are cold (≲20 K). In two of the starless clumps we observed, the CCS emission is distributed as it surrounds the N{sub 2}H{sup +} core (chemically evolved gas), which resembles the case of L1544, a prestellar core showing collapse. In addition, we detected both DNC and N{sub 2}D{sup +}. These two clumps are most likely on the verge of star formation. We introduce the chemical evolution factor (CEF) for starless cores to describe the chemical evolutionary stage, and analyze the observed Planck cold clumps.« less

Energetic oxygen precipitation as a source of vibrationally excited N/sub 2//sup +/ in emissions observed at low latitudes

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

Tinsley, B.A.; Rohrbaugh, R.P.; Sahai, Y.

Observations have been made at Mt. Haleakala, Hawaii (dip lat.approx.22/sup 0/N) and Cachoeira Paulista, Brasil (dip lat.approx.12/sup 0/S) of emissions excited by particle precipitation during periods of magnetic activity. The first negative bands of N/sub 2//sup +/ were found to have a high degree of vibrational excitation at both sites, and withi the absence of emissions attributable to hydrogen and helium, this finding leads to the interpretation that the excitation was due to a flux of precipitating oxygen atoms or ions, more plausibly the former, produced by charge exchange of ring current O/sup +/ ions with exospheric neutral constituents. Moremore » laboratory work is needed to properly interpret the data, but crude estimates of the associated energy deposition and ionization production fall in the range 10/sup -1/ to 10/sup +1/mWm/sup -2/, and 10/sup 0/-10/sup 2/ cm/sup -3/s/sup -1/ respectively.« less

Enhanced performance of dye-sensitized solar cells based on organic dopant incorporated PVDF-HFP/PEO polymer blend electrolyte with g-C{sub 3}N{sub 4}/TiO{sub 2} photoanode

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

Senthil, R.A.; Theerthagiri, J.; Madhavan, J., E-mail: jagan.madhavan@gmail.com

This work describes the effect of 2-aminopyrimidine (2-APY) on poly(vinylidinefluoride-co-hexafluoropropylene) (PVDF-HFP)/polyethylene oxide (PEO) blend polymer electrolyte along with binary iodide salts (tetrabutylammonium iodide (TBAI) and potassium iodide (KI)) and iodine (I{sub 2}) were studied for enhancing the efficiency of the dye-sensitized solar cells (DSSCs) consisting of g-C{sub 3}N{sub 4}/TiO{sub 2} composite as photoanode. The g-C{sub 3}N{sub 4} was synthesized from low cost urea by thermal condensation method. It was used as a precursor to synthesize the various weight percentage ratios (5%, 10% and 15%) of g-C{sub 3}N{sub 4}/TiO{sub 2} composites by wet-impregnation method. The pure and 2-APY incorporated PVDF-HFP/PEO polymermore » blend electrolytes were arranged by wet chemical process (casting method) using DMF as a solvent. The synthesized g-C{sub 3}N{sub 4}/TiO{sub 2} composites and polymer blend electrolytes were studied and analyzed by Fourier transform infrared (FT-IR) spectroscopy, X-ray diffractometer (XRD) and scanning electron microscopy (SEM). The ionic conductivity values of the pure and 2-APY incorporated PVDF-HFP/PEO blend electrolytes were estimated to be 4.53×10{sup −5} and 1.87×10{sup −4} Scm{sup −1} respectively. The UV–vis absorption spectroscopy was carried out for the pure and different wt% of g-C{sub 3}N{sub 4}/TiO{sub 2} composites coated FTO films after N3 dye-sensitization. The 10 wt% g-C{sub 3}N{sub 4}/TiO{sub 2} composite film showed a maximum absorption compared to the others. The DSSC assembled with 10 wt% g-C{sub 3}N{sub 4}/TiO{sub 2} as photoanode using the pure polymer blend electrolyte exhibited a power conversion efficiency (PCE) of 3.17% , which was superior than that of DSSC based pure TiO{sub 2} (2.46%). However, the PCE was increased to 4.73% for the DSSC assembled using 10 wt% g-C{sub 3}N{sub 4}/TiO{sub 2} as photoanode with 2-APY incorporated polymer blend electrolyte. Hence, the present study is a successful attempt to provide a new pathway to enhance the performance of DSSCs. - Graphical abstract: In this study, the g-C{sub 3}N{sub 4} was synthesized from low cost urea and it was used as a precursor to synthesize of g-C{sub 3}N{sub 4}/TiO{sub 2} composite. The pure and 2-APY incorporated PVDF-HFP/PEO electrolytes were fabricated by solution casting method. A remarkably enhanced PCE of 4.73% was observed for 2-APY incorporated PVDF-HFP/PEO electrolyte with g-C{sub 3}N{sub 4}/TiO{sub 2} composite photoanode based DSSC. - Highlights: • 2-APY added PVDF-HFP/PEO electrolyte was prepared by solution casting method. • The g-C{sub 3}N{sub 4}/TiO{sub 2} composites were synthesized by wet-impregnation method. • DSSC with g-C{sub 3}N{sub 4}/TiO{sub 2} and 2-APY added electrolyte showed the efficiency of 4.73 %. • The g-C{sub 3}N{sub 4} and 2-APY can be a useful dopant to enhance the performance of DSSCs.« less

TiO{sub 2} nanobelts with a uniform coating of g-C{sub 3}N{sub 4} as a highly effective heterostructure for enhanced photocatalytic activities

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

Zhong, Xing; Jin, Meimei; Dong, Huaqing

2014-12-15

A novel g-C{sub 3}N{sub 4}/TiO{sub 2} nanobelt (NB) heterostructure was successfully designed and prepared. The as-prepared g-C{sub 3}N{sub 4}/TiO{sub 2} NB heterostructure exhibited high photocatalytic activity not only in the photodegradation of Rhodamine B (RhB) but also in photocatalytic H{sub 2} production. The g-C{sub 3}N{sub 4}/TiO{sub 2} NB heterostructure with a mass ratio of 1:1 demonstrated the best performance in the photodegradation of RhB, whereas a mass ratio of 3:1 demonstrated the highest H{sub 2} production rate of 46.6 μmol h{sup −1} in photocatalytic H{sub 2} production. We conclude that the synergistic effect between g-C{sub 3}N{sub 4} and TiO{sub 2}more » NBs promotes the photogenerated carrier separation in space. This valuable insight into the rational architectural design of nanostructure-based photocatalysts is expected to shed light on other photocatalytic reaction systems in the future. - Graphical abstract: A novel strategy to fabricate the g-C{sub 3}N{sub 4}/TiO{sub 2} nanobelt (NB) heterostructures was reported. The g-C{sub 3}N{sub 4}/TiO{sub 2} NB heterostructures exhibited highly effective photocatalytic activities for photodegradation of Rhodamine B and H{sub 2} production. - Highlights: • A novel strategy to fabricate the g-C{sub 3}N{sub 4}/TiO{sub 2} NB heterostructures was reported. • The heterostructure exhibited high catalytic activity in photodegradation of RhB. • The heterostructure showed good H{sub 2} productivity in photocatalytic water splitting. • The synergistic effect between g-C{sub 3}N{sub 4} and TiO{sub 2} NBs are important. • This study shows that the heterostructure can be an effective photocatalyst.« less

Scanning transmission electron microscopy analysis of Ge(O)/(graphitic carbon nitride) nanocomposite powder

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

Kawasaki, Masahiro; Sompetch, Kanganit; Sarakonsri, Thapanee, E-mail: tsarakonsri@gmail.com

2015-12-15

Analytical electron microscopy has revealed the structure of particles that were synthesized by chemical reaction of GeO{sub 2} with NaBH{sub 4} in the basic solution including graphitic carbon nitride (g-C{sub 3}N{sub 4}) powders. The g-C{sub 3}N{sub 4} was arranged by recrystallization of melamine at 600 °C under N{sub 2} gas atmosphere. The samples were dried at 60 °C or 180 °C for 4 h. The g-C{sub 3}N{sub 4} was observed as lamellae of several ten nm or less in size and had an amorphous-like structure with a distorted lattice in an area as small as a few hundred pm inmore » size. The reaction product was Ge(O) particles as fine as several nm in size and composed of Ge and O atoms. Most of the particles must be of GeO{sub 2−x} with the amorphous-like structure that has also a distorted lattice in an area of a few hundred pm in size. In the sample dried at 60 °C, the particles were found to be dispersed in a wide area on the g-C{sub 3}N{sub 4} lamella. It is hard to recognize those particles in TEM images. The particles in the sample dried at 180 °C became larger and were easily observed as isolated lumps. Hence, these powders can be regarded as GeO{sub 2}/g-C{sub 3}N{sub 4} or Ge/GeO{sub 2}/g-C{sub 3}N{sub 4} nanocomposites, and expected to be applicable to anode materials for high energy Li-ion batteries due to Ge catalysis effect, accordingly. - Graphical abstract: STEM analysis of Ge(O)/(graphitic carbon nitride) nanocomposite powder. - Highlights: • Graphitic (g)-C{sub 3}N{sub 4} powder was prepared at 600 °C by recrystallization of melamine. • Ge(O) was prepared by chemical reaction in a solution including the g-C{sub 3}N{sub 4} powders. • The products can be regarded as GeO{sub 2}/g-C{sub 3}N{sub 4} or Ge/GeO{sub 2}/g-C{sub 3}N{sub 4} nanocomposites. • GeO{sub 2} was amorphous several-nm particles and g-C{sub 3}N{sub 4} was amorphous lamella of several 10 nm in size. • We expect them to be applicable for high energy Li-ion battery anode materials.« less

Mechanism of thermal electron attachment in N/sub 2/O--CO/sub 2/ mixtures in the gas phase

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

Shimamori, H.; Fessenden, R.W.

1978-12-01

The attachment of thermal electrons to nitrous oxide in N/sub 2/O--CO/sub 2/ mixtures has been studied at room temperature in the pressure range 5--120 torr. Ionization was by pulse radiolysis and the electron concentration was measured as a function of time by microwave conductivity. Addition of even less than 0.1% CO/sub 2/ to N/sub 2/O causes a marked increase in attachment rate. However, this enhancement soon saturates in that further additions of CO/sub 2/ have less and less effect. Experiments with ternary mixtures including C/sub 2/H/sub 6/ showed a further enhancement which was much larger than the additive effects ofmore » CO/sub 2/ and C/sub 2/H/sub 6/ alone. These observations can be explained by a two step three-body process producing vibrationally excited N/sub 2/O/sup -/* if the rate constant for stabilization of N/sub 2/O/sup -/* by CO/sub 2/ is 4 x 10/sup -30/ cm/sup 6//molecule/sup 2/xsec. The decrease in effectiveness with increased CO/sub 2/ pressure is interpreted as the collisional ionization of a complex ion, (N/sub 2/OxCO/sub 2/)/sup -/*. The nonadditive effect of hydrocarbon results from the rapid reactive destruction of such complexes by collision with the hydrocarbon. A detailed quantitative treatment of the proposed mechanism was successful in explaining most features of the data. In a limited set of experiments, allene : N/sub 2/O mixtures were found to behave much like CO/sub 2/--N/sub 2/O.« less

Soot oxidation and NO{sub x} reduction over BaAl{sub 2}O{sub 4} catalyst

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

Lin, He; Li, Yingjie; Shangguan, Wenfeng

2009-11-15

This study addresses soot oxidation and NO{sub x} reduction over a BaAl{sub 2}O{sub 4} catalyst. By XRD analysis, the catalyst was shown to be of spinel structure. Temperature Programmed Oxidation (TPO) and Constant Temperature Oxidation (CTO) at 673 K show that the presence of O{sub 2} decreases the ignition temperature of soot, and it enhances the conversion of NO{sub x} to N{sub 2} and N{sub 2}O. The kinetic features of soot oxidation in the TPO test are similar to that in the TG-DTA analysis. Analysis by Diffuse Reflectance Fourier Infrared Transform Spectroscopy (DRIFTS) indicates that the nitrates formed from NO{submore » x} adsorption and the C(O) intermediates from soot oxidation are the key precursors of the redox process between soot and NO{sub x} over surfaces of the BaAl{sub 2}O{sub 4} catalyst. Moreover, DRIFTS tests suggest that nitrates act as the principal oxidants for C(O) oxidation, through which nitrates are reduced to N{sub 2} and N{sub 2}O. The O{sub 2} in the gas mixture presents a positive effect on the conversion of NO{sub x} to N{sub 2} and N{sub 2}O by promoting the oxidation of nitrites into nitrates species. (author)« less

The Li–Si–(O)–N system revisited: Structural characterization of Li{sub 21}Si{sub 3}N{sub 11} and Li{sub 7}SiN{sub 3}O

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

Casas-Cabanas, M.; Santner, H.; Palacín, M.R., E-mail: rosa.palacin@icmab.es

2014-05-01

A systematic study of the Li–Si–(O)–N system is presented. The synthetic conditions to prepare Li{sub 2}SiN{sub 2}, Li{sub 5}SiN{sub 3}, Li{sub 18}Si{sub 3}N{sub 10}, Li{sub 21}Si{sub 3}N{sub 11} and Li{sub 7}SiN{sub 3}O are described and the structure of the last two compounds has been solved for the first time. While Li{sub 21}Si{sub 3}N{sub 11} crystallizes as a superstructure of the anti-fluorite structure with Li and Si ordering, Li{sub 7}SiN{sub 3}O exhibits the anti-fluorite structure with both anion and cation disorder. - Graphical abstract: A systematic study of the Li–Si–(O)–N system is presented. Li{sub 21}Si{sub 3}N{sub 11} crystallizes as a superstructuremore » of the anti-fluorite structure with Li and Si ordering, Li{sub 7}SiN{sub 3}O exhibits the anti-fluorite structure with both anion and cation disorder. - Highlights: • Li{sub 2}SiN{sub 2}, Li{sub 5}SiN{sub 3}, Li{sub 18}Si{sub 3}N{sub 10}, Li{sub 21}Si{sub 3}N{sub 11} and Li{sub 7}SiN{sub 3}O are prepared. • The structures of Li{sub 21}Si{sub 3}N{sub 11} and Li{sub 7}SiN{sub 3}O are presented. • Li{sub 21}Si{sub 3}N{sub 11} exhibits an anti-fluorite superstructure with Li and Si ordering.« less

RADIOLYSIS OF NITROGEN AND WATER-ICE MIXTURE BY FAST IONS: IMPLICATIONS FOR KUIPER BELT OBJECTS

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

Barros, A. L. F. de; Silveira, E. F da; Bergantini, A.

The participation of condensed nitrogen in the surface chemistry of some objects in the outer solar system, such as Pluto and Triton, is very important. The remote observation of this species using absorption spectroscopy is a difficult task because N{sub 2} is not IR active in the gas phase. Water is also among the most abundant molecules in the surface of these objects; chemical reactions between N{sub 2} and H{sub 2}O induced by cosmic rays are therefore expected. Although pure N{sub 2} ice is hardly identified by IR spectroscopy, the species produced through the processing of the surface ice bymore » cosmic rays may give relevant clues indicating how abundant the N{sub 2} is in the outside layers of the surface of trans-Neptunian objects (TNOs). The objective of this work is to investigate the formation of nitrogenated species induced by cosmic-ray analogs in an ice mixture containing nitrogen and water. Experiments were performed in the GANIL Laboratory by bombarding N{sub 2}:H{sub 2}O (10:1) ice at 15 K with 40 MeV {sup 58}Ni{sup 11+} ions. Evolution of precursor and daughter species was monitored by Fourier transform infrared spectrometry. The main produced species are the nitrogen oxides NO{sub k} (k = 1–3), N{sub 2}O{sub j} (j = 1–5), N{sub 3}, and O{sub 3}. Among them, the N{sub 2}O and N{sub 3} are the most abundant, representing ∼61% of the total column density of the daughter molecules at 10{sup 13} ions cm{sup −2} fluence; the current results indicate that the yield of daughter species from this mixture is low, and this may be one of the reasons why N{sub i}O{sub j} molecules are not usually observed in TNOs.« less

Method for synthesizing HMX

DOEpatents

McGuire, Raymond R.; Coon, Clifford L.; Harrar, Jackson E.; Pearson, Richard K.

1984-01-01

A method and apparatus for electrochemically synthesizing N.sub.2 O.sub.5 cludes oxidizing a solution of N.sub.2 O.sub.4 /HNO.sub.3 at an anode, while maintaining a controlled potential between the N.sub.2 O.sub.4 /HNO.sub.3 solution and the anode. A potential of about 1.35 to 2.0 V vs. SCE is preferred, while a potential of about 1.80 V vs. SCE is most preferred. Thereafter, the N.sub.2 O.sub.5 is reacted with either 1.5-diacetyl-3,7-dinitro-1,3,5,7-tetraazacyclooctane (DADN) or 1,3,5,7-tetraacetyl-1,3,5,7-tetraazacyclooctane (TAT) to form cyclotetramethylenetetraamine (HMX).

Study on the effect of hydrogen addition on the variation of plasma parameters of argon-oxygen magnetron glow discharge for synthesis of TiO{sub 2} films

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

Saikia, Partha, E-mail: partha.008@gmail.com; Institute of Physics, Pontificia Universidad Católica de Chile, Av. Vicuña Mackenna 4860, Santiago; Saikia, Bipul Kumar

2016-04-15

We report the effect of hydrogen addition on plasma parameters of argon-oxygen magnetron glow discharge plasma in the synthesis of H-doped TiO{sub 2} films. The parameters of the hydrogen-added Ar/O{sub 2} plasma influence the properties and the structural phases of the deposited TiO{sub 2} film. Therefore, the variation of plasma parameters such as electron temperature (T{sub e}), electron density (n{sub e}), ion density (n{sub i}), degree of ionization of Ar and degree of dissociation of H{sub 2} as a function of hydrogen content in the discharge is studied. Langmuir probe and Optical emission spectroscopy are used to characterize the plasma.more » On the basis of the different reactions in the gas phase of the magnetron discharge, the variation of plasma parameters and sputtering rate are explained. It is observed that the electron and heavy ion density decline with gradual addition of hydrogen in the discharge. Hydrogen addition significantly changes the degree of ionization of Ar which influences the structural phases of the TiO{sub 2} film.« less

4f and 5d energy levels of the divalent and trivalent lanthanide ions in M{sub 2}Si{sub 5}N{sub 8} (M=Ca, Sr, Ba)

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

Kate, O.M. ten, E-mail: o.m.tenkate@tudelft.nl; Energy Materials and Devices, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, Den Dolech 2, 5600MB Eindhoven; Zhang, Z.

Optical data of Sm, Tb and Yb doped Ca{sub 2}Si{sub 5}N{sub 8} and Sr{sub 2}Si{sub 5}N{sub 8} phosphors that have been prepared by solid-state synthesis, are presented. Together with luminescence data from literature on Ce{sup 3+} and Eu{sup 2+} doping in the M{sub 2}Si{sub 5}N{sub 8} (M=Ca, Sr, Ba) hosts, energy level schemes were constructed showing the energy of the 4f and 5d levels of all divalent and trivalent lanthanide ions relative to the valence and conduction band. The schemes were of great help in interpreting the optical data of the lanthanide doped phosphors and allow commenting on the valencemore » stability of the ions, as well as the stability against thermal quenching of the Eu{sup 2+}d-f emission. Tb{sup 3+} substitutes on both a high energy and a low energy site in Ca{sub 2}Si{sub 5}N{sub 8}, due to which excitation at 4.77 eV led to emission from both the {sup 5}D{sub 3} and {sup 5}D{sub 4} levels, while excitation at 4.34 eV gave rise to mainly {sup 5}D{sub 4} emission. Doping with Sm resulted in typical Sm{sup 3+}f-f line absorption, as well as an absorption band around 4.1 eV in Ca{sub 2}Si{sub 5}N{sub 8} and 3.6 eV in Sr{sub 2}Si{sub 5}N{sub 8} that could be identified as the Sm{sup 3+} charge transfer band. Yb on the other hand was incorporated in both the divalent and the trivalent state in Ca{sub 2}Si{sub 5}N{sub 8}. - Graphical abstract: Energy level schemes showing the 4f ground states of the trivalent ( Black-Down-Pointing-Small-Triangle ) and divalent ( Black-Up-Pointing-Small-Triangle ) lanthanide ions and lowest energy 5d states of the trivalent ({nabla}) and divalent ({Delta}) ions with respect to the valence and conduction bands of Ca{sub 2}Si{sub 5}N{sub 8} (left) and Sr{sub 2}Si{sub 5}N{sub 8} (right). Highlights: Black-Right-Pointing-Pointer Construction of energy level schemes of all lanthanides within the M{sub 2}Si{sub 5}N{sub 8} hosts. Black-Right-Pointing-Pointer Construction was done by analyzing existing as well as new spectroscopic data. Black-Right-Pointing-Pointer Tb{sup 3+}d-f emission from two different Ca sites in Ca{sub 2}Si{sub 5}N{sub 8} has been observed. Black-Right-Pointing-Pointer Observation of the Sm{sup 3+} charge transfer band in Ca{sub 2}Si{sub 5}N{sub 8} and Sr{sub 2}Si{sub 5}N{sub 8}. Black-Right-Pointing-Pointer Ytterbium has been found in the divalent and trivalent state in Ca{sub 2}Si{sub 5}N{sub 8}.« less

Falloff curve and specific rate constants for the reaction NO/sub 2/ + NO/sub 2/ /r reversible/ N/sub 2/O/sub 4/

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

Borrell, P.; Cobos, C.J.; Luther, K.

1988-07-28

The rate of association of NO/sub 2/ to N/sub 2/O/sub 4/ was measured in N/sub 2/ at pressures from 1 to 207 bar. This way the reaction was observed in a large section of its falloff range. The relaxation of NO/sub 2//N/sub 2/O/sub 4/ mixtures was followed after laser flash photolysis of N/sub 2/O/sub 4/ at 248 nm. From the results the falloff curve was constructed, which gives the high- and low-pressure rate constants at 298 K (in cm/sup 3/ molecule/sup /minus/1/ s/sup /minus/1/): k/sub ass//sup infinity/ = (8.3 /plus minus/ 1.0) /times/ 10/sup /minus/13/ and k/sub ass//sup 0/ =more » (1.4 /plus minus/ 0.2) /times/ 10/sup /minus/33/(N/sub 2/). Earlier measurements believed to be in the low-pressure regime, have not been free from falloff effects. The low value of k/sup infinity/ was analyzed with the statistic adiabatic channel model, and specific rate constants, k(E,J), were calculated. They increase very steeply with energy just above the reaction threshold and go through maxima at low excess energies. These unusual effects are analyzed theoretically and the strong contributions are pointed out of the low-frequency vibrations which disappear during the dissociation of N/sub 2/O/sub 4/.« less

Light harvesting with Ge quantum dots embedded in SiO{sub 2} or Si{sub 3}N{sub 4}

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

Cosentino, Salvatore, E-mail: Salvatore.cosentino@ct.infn.it; Raciti, Rosario; Simone, Francesca

2014-01-28

Germanium quantum dots (QDs) embedded in SiO{sub 2} or in Si{sub 3}N{sub 4} have been studied for light harvesting purposes. SiGeO or SiGeN thin films, produced by plasma enhanced chemical vapor deposition, have been annealed up to 850 °C to induce Ge QD precipitation in Si based matrices. By varying the Ge content, the QD diameter can be tuned in the 3–9 nm range in the SiO{sub 2} matrix, or in the 1–2 nm range in the Si{sub 3}N{sub 4} matrix, as measured by transmission electron microscopy. Thus, Si{sub 3}N{sub 4} matrix hosts Ge QDs at higher density and more closely spaced thanmore » SiO{sub 2} matrix. Raman spectroscopy revealed a higher threshold for amorphous-to-crystalline transition for Ge QDs embedded in Si{sub 3}N{sub 4} matrix in comparison with those in the SiO{sub 2} host. Light absorption by Ge QDs is shown to be more effective in Si{sub 3}N{sub 4} matrix, due to the optical bandgap (0.9–1.6 eV) being lower than in SiO{sub 2} matrix (1.2–2.2 eV). Significant photoresponse with a large measured internal quantum efficiency has been observed for Ge QDs in Si{sub 3}N{sub 4} matrix when they are used as a sensitive layer in a photodetector device. These data will be presented and discussed, opening new routes for application of Ge QDs in light harvesting devices.« less

Effects of calcining temperature on photocatalysis of g-C{sub 3}N{sub 4}/TiO{sub 2} composites for hydrogen evolution from water

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

Qu, Ailan, E-mail: elainqal@163.com; Xu, Xinmei; Xie, Haolong

Highlights: • TiO{sub 2} promotes melon to form at 400 °C, whereas it forms at 500 °C for only melamine. • The highest photocatalytic activity was achieved when calcination was performed at 400 °C. • Coordinated N−Ti−N bonds were formed in MA/TiO{sub 2} (400) and disappeared at high temperature. • The surface area decreased and the pore size increased with increasing of temperature. • Only MA/TiO{sub 2} (400) has a narrower band gap than pure g-C{sub 3}N{sub 4}. - Abstract: A composite of graphitic carbon nitride and TiO{sub 2} (g-C{sub 3}N{sub 4}/TiO{sub 2}) with enhanced photocatalytic hydrogen evolution capacity wasmore » achieved by calcining melamine and TiO{sub 2} sol-gel precursor. Characterization results reveal that heating temperature had a great influence on the structure, surface area and properties of the composites. Compared with the polycondensation of pure melamine, the presence of TiO{sub 2} precursor can promote the formation of melon at a low temperature. The highest photocatalytic activity of g-C{sub 3}N{sub 4}/TiO{sub 2}(400) was achieved when the calcination was performed at 400 °C, exhibiting H{sub 2} production rate of 76.25 μmol/h under UV–vis light irradiation (λ > 320 nm) and 35.44 μmol/h under visible light irradiation (λ > 420 nm). The highest photocatalytic performance of g-C{sub 3}N{sub 4}/TiO{sub 2}(400) can be attributed to: (1) the strong UV–vis light absorption due to the narrow bandgap caused by synergic effect of TiO{sub 2} and g-C{sub 3}N{sub 4}, (2) high surface area and porosity, (3) the effective separation of photo-generated electron-holes owing to the favorable heterojunction between TiO{sub 2} and g-C{sub 3}N{sub 4}.« less

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

Yasui, Kanji, E-mail: kyasui@vos.nagaokaut.ac.jp; Morioka, Makoto; Kanauchi, Shingo

The influence of N{sub 2}O gas addition on the properties of zinc oxide (ZnO) films grown on a-plane (11–20) sapphire (a-Al{sub 2}O{sub 3}) substrates was investigated, using a chemical vapor deposition method based on the reaction between dimethylzinc and high-temperature H{sub 2}O produced by a catalytic H{sub 2}-O{sub 2} reaction on platinum (Pt) nanoparticles. The addition of N{sub 2}O was found to increase the size of the crystalline facets and to improve the crystal orientation along the c-axis. The electron mobility at 290 K was also increased to 234 cm{sup 2}/Vs following the addition of N{sub 2}O gas at a pressure ofmore » 3.2 × 10{sup −3 }Pa. In addition, the minimum full width at half maximum of the most intense photoluminescence peak derived from neutral donor bound excitons at 10 K decreased to 0.6 meV by the addition of N{sub 2}O gas at a pressure of 3.1 × 10{sup −2 }Pa.« less

Large-scale production of anhydrous nitric acid and nitric acid solutions of dinitrogen pentoxide

DOEpatents

Harrar, Jackson E.; Quong, Roland; Rigdon, Lester P.; McGuire, Raymond R.

2001-01-01

A method and apparatus are disclosed for a large scale, electrochemical production of anhydrous nitric acid and N.sub.2 O.sub.5. The method includes oxidizing a solution of N.sub.2 O.sub.4 /aqueous-HNO.sub.3 at the anode, while reducing aqueous HNO.sub.3 at the cathode, in a flow electrolyzer constructed of special materials. N.sub.2 O.sub.4 is produced at the cathode and may be separated and recycled as a feedstock for use in the anolyte. The process is controlled by regulating the electrolysis current until the desired products are obtained. The chemical compositions of the anolyte and catholyte are monitored by measurement of the solution density and the concentrations of N.sub.2 O.sub.4.

From Ba{sub 3}Ta{sub 5}O{sub 14}N to LaBa{sub 2}Ta{sub 5}O{sub 13}N{sub 2}: Decreasing the optical band gap of a photocatalyst

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

Anke, B.; Bredow, T.; Pilarski, M.

Yellow LaBa{sub 2}Ta{sub 5}O{sub 13}N{sub 2} was successfully synthesized as phase-pure material crystallizing isostructurally to previously reported Ba{sub 3}Ta{sub 5}O{sub 14}N and mixed-valence Ba{sub 3}Ta{sup V}{sub 4}Ta{sup IV}O{sub 15}. The electronic structure of LaBa{sub 2}Ta{sub 5}O{sub 13}N{sub 2} was studied theoretically with the range-separated hybrid method HSE06. The most stable structure was obtained when lanthanum was placed on 2a and nitrogen on 4h sites confirming Pauling's second rule. By incorporating nitrogen, the measured band gap decreases from ∼3.8 eV for the oxide via 2.74 eV for Ba{sub 3}Ta{sub 5}O{sub 14}N to 2.63 eV for the new oxide nitride, giving risemore » to an absorption band well in the visible-light region. Calculated fundamental band gaps confirm the experimental trend. The atom-projected density of states has large contributions from N2p orbitals close to the valence band edge. These are responsible for the observed band gap reduction. Photocatalytic hydrogen formation was investigated and compared with that of Ba{sub 3}Ta{sub 5}O{sub 14}N revealing significantly higher activity for LaBa{sub 2}Ta{sub 5}O{sub 13}N{sub 2} under UV-light. - Graphical abstract: X-ray powder diffraction pattern of LaBa{sub 2}Ta{sub 5}O{sub 13}N{sub 2} with the results of the Rietveld refinements. Inset: Unit cell of LaBa{sub 2}Ta{sub 5}O{sub 13}N{sub 2} and polyhedral representation of the crystal structure. - Highlights: • Synthesis of a new oxide nitride LaBa{sub 2}Ta{sub 5}O{sub 13}N{sub 2}. • Refinement of the crystal structure. • Quantum chemical calculations provided band gap close to the measured value. • New phase shows a higher photocatalytic H{sub 2} evolution rate compared to prior tested Ba{sub 3}Ta{sub 5}O{sub 14}N.« less

Topologically and geometrically flexible structural units in seven new organically templated uranyl selenates and selenite–selenates

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

Gurzhiy, Vladislav V., E-mail: vladgeo17@mail.ru; Kovrugin, Vadim M.; Tyumentseva, Olga S.

2015-09-15

Single crystals of seven novel uranyl oxysalts of selenium with protonated methylamine molecules, [C{sub 2}H{sub 8}N]{sub 2}[(UO{sub 2})(SeO{sub 4}){sub 2}(H{sub 2}O)] (I), [C{sub 2}H{sub 8}N]{sub 2}[(UO{sub 2}){sub 2}(SeO{sub 4}){sub 3}(H{sub 2}O)] (II), [C{sub 4}H{sub 15}N{sub 3}][H{sub 3}O]{sub 0.5}[(UO{sub 2}){sub 2}(SeO{sub 4}){sub 2.93}(SeO{sub 3}){sub 0.07}(H{sub 2}O)](NO{sub 3}){sub 0.5} (III), [C{sub 2}H{sub 8}N]{sub 3}[H{sub 5}O{sub 2}][(UO{sub 2}){sub 2}(SeO{sub 4}){sub 3}(H{sub 2}O){sub 2}]{sub 2}(H{sub 2}O){sub 5} (IV), [C{sub 2}H{sub 8}N]{sub 2}[H{sub 3}O][(UO{sub 2}){sub 3}(SeO{sub 4}){sub 4}(HSeO{sub 3})(H{sub 2}O)](H{sub 2}SeO{sub 3}){sub 0.2} (V), [C{sub 4}H{sub 12}N]{sub 3}[H{sub 3}O][(UO{sub 2}){sub 3}(SeO{sub 4}){sub 5}(H{sub 2}O)] (VI), and [C{sub 2}H{sub 8}N]{sub 3}(C{sub 2}H{sub 7}N)[(UO{sub 2}){sub 3}(SeO{sub 4}){submore » 4}(HSeO{sub 3})(H{sub 2}O)] (VII) have been prepared by isothermal evaporation from aqueous solutions. Their crystal structures have been solved by direct methods and their uranyl selenate and selenite–selenate units investigated using black-and-white graphs from the viewpoints of topology of interpolyhedral linkages and isomeric variations. The crystal structure of IV is based upon complex layers with unique topology, which has not been observed previously in uranyl selenates. Investigations of the statistics and local distribution of the U–O{sub br}–Se bond angles demonstrates that shorter angles associate with undulations, whereas larger angles correspond to planar areas of the uranyl selenite layers. - Graphical abstract: Crystal structures of the seven novel Se-contaning uranyl oxysalts that contain protonated organic molecules as interlayer species have been investigated from the viewpoints of topology of interpolyhedral linkages, isomeric variations and flexibility of structural units. - Highlights: • Single crystals of seven novel uranyl oxysalts were prepared by evaporation method. • The graph theory was used for investigation of topologies of structural units. • The method of orientation matrices was applied to distinguish geometrical isomers. • The flexibility of structural complexes specifies the undulation of layered structural units.« less

Solubility and diffusivity of N{sub 2}O and CO{sub 2} in (monoethanolamine + N-methyldiethanolamine + water) and in (monoethanolamine + 2-amino-2-methyl-1-propanol + water)

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

Li, M.H.; Lai, M.D.

1995-03-01

Solutions of amines are frequently used in gas-treating processes to remove acid gases, such as CO{sub 2} and H{sub 2}S, from gas streams in the natural gas and synthetic ammonia industries and petroleum chemical plants. The solubility and diffusivity of N{sub 2}O in (monoethanolamine + N-methyldiethanolamine + water) and in (monoethanolamine + 2-amino-2-methyl-l-propanol + water) were measured at 30, 35, and 40 C and at atmospheric pressure. Six (monoethanolamine + N-methyldiethanolamine + water) and five (monoethanolamine + 2-amino-2-methyl-l-propanol + water) systems were studied. The total amine mass percent in all cases was 30. The solubilities were measured by a solubilitymore » apparatus similar to that of Haimour and Sandall (1984). A wetted wall column absorber was used to obtain the diffusivity of N{sub 2}O in amines. The N{sub 2}O solubilities in amine solutions have been correlated on the basis of the excess Henry constant correlation of Wang et al. (1992). The N{sub 2}O analogy was used to estimate the solubility and diffusivity of CO{sub 2} in (monoethanolamine + N-methyldiethanolamine + water) and in (monoethanolamine + 2-amino-2-methyl-l-propanol + water).« less

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

Li, Chen; Metzler, Dominik; Oehrlein, Gottlieb S., E-mail: oehrlein@umd.edu

Angstrom-level plasma etching precision is required for semiconductor manufacturing of sub-10 nm critical dimension features. Atomic layer etching (ALE), achieved by a series of self-limited cycles, can precisely control etching depths by limiting the amount of chemical reactant available at the surface. Recently, SiO{sub 2} ALE has been achieved by deposition of a thin (several Angstroms) reactive fluorocarbon (FC) layer on the material surface using controlled FC precursor flow and subsequent low energy Ar{sup +} ion bombardment in a cyclic fashion. Low energy ion bombardment is used to remove the FC layer along with a limited amount of SiO{sub 2} frommore » the surface. In the present article, the authors describe controlled etching of Si{sub 3}N{sub 4} and SiO{sub 2} layers of one to several Angstroms using this cyclic ALE approach. Si{sub 3}N{sub 4} etching and etching selectivity of SiO{sub 2} over Si{sub 3}N{sub 4} were studied and evaluated with regard to the dependence on maximum ion energy, etching step length (ESL), FC surface coverage, and precursor selection. Surface chemistries of Si{sub 3}N{sub 4} were investigated by x-ray photoelectron spectroscopy (XPS) after vacuum transfer at each stage of the ALE process. Since Si{sub 3}N{sub 4} has a lower physical sputtering energy threshold than SiO{sub 2}, Si{sub 3}N{sub 4} physical sputtering can take place after removal of chemical etchant at the end of each cycle for relatively high ion energies. Si{sub 3}N{sub 4} to SiO{sub 2} ALE etching selectivity was observed for these FC depleted conditions. By optimization of the ALE process parameters, e.g., low ion energies, short ESLs, and/or high FC film deposition per cycle, highly selective SiO{sub 2} to Si{sub 3}N{sub 4} etching can be achieved for FC accumulation conditions, where FC can be selectively accumulated on Si{sub 3}N{sub 4} surfaces. This highly selective etching is explained by a lower carbon consumption of Si{sub 3}N{sub 4} as compared to SiO{sub 2}. The comparison of C{sub 4}F{sub 8} and CHF{sub 3} only showed a difference in etching selectivity for FC depleted conditions. For FC accumulation conditions, precursor chemistry has a weak impact on etching selectivity. Surface chemistry analysis shows that surface fluorination and FC reduction take place during a single ALE cycle for FC depleted conditions. A fluorine rich carbon layer was observed on the Si{sub 3}N{sub 4} surface after ALE processes for which FC accumulation takes place. The angle resolved-XPS thickness calculations confirmed the results of the ellipsometry measurements in all cases.« less

Microstructural evolution of diamond films from CH{sub 4}/H{sub 2}/N{sub 2} plasma and their enhanced electrical properties

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

Sankaran, K. J.; Tai, N. H., E-mail: nhtai@mx.nthu.edu.tw; Lin, I. N., E-mail: inanlin@mail.tku.edu.tw

2015-02-21

The influence of N{sub 2} concentration in CH{sub 4}/H{sub 2}/N{sub 2} plasma on microstructural evolution and electrical properties of diamond films is systematically investigated. While the diamond films grown in CH{sub 4}/H{sub 2} plasma contain large diamond grains, for the diamond films grown using CH{sub 4}/H{sub 2}/(4%)N{sub 2} plasma, the microstructure drastically changed, resulting in ultra-nanosized diamond grains with Fd3m structure and a{sub 0} = 0.356 nm, along with the formation of n-diamond (n-D), a metastable form of diamond with space group Fm3m and a{sub 0} = 0.356 nm, and i-carbon (i-C) clusters, the bcc structured carbon with a{sub 0} = 0.432 nm. In addition, these films contain widemore » grain boundaries containing amorphous carbon (a-C). The electron field emission (EFE) studies show the best EFE behavior for 4% N{sub 2} films among the CH{sub 4}/H{sub 2}/N{sub 2} grown diamond films. They possess the lowest turn-on field value of 14.3 V/μm and the highest EFE current density value of 0.37 mA/cm{sup 2} at an applied field of 25.4 V/μm. The optical emission spectroscopy studies confirm that CN species are the major criterion to judge the changes in the microstructure of the films. It seems that the grain boundaries can provide electron conduction networks to transport efficiently the electrons to emission sites for field emission, as long as they have sufficient thickness. Whether the matrix nano-sized grains are 3C-diamond, n-D or i-C is immaterial.« less

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

Hoder, T., E-mail: hoder@physics.muni.cz; Department of Physical Electronics, Faculty of Science, Masaryk University, Kotlářská 2, 611 37 Brno; Bonaventura, Z., E-mail: zbona@physics.muni.cz

Theoretical analysis of ultra-short phenomena occurring during the positive streamer propagation in atmospheric pressure air is presented. Motivated by experimental results obtained with tens-of-picoseconds and tens-of-microns precision, it is shown that when the streamer head passes a spatial coordinate, emission maxima from N{sub 2} and N{sub 2}{sup +} radiative states follow with different delays. These different delays are caused by differences in the dynamics of populating the radiative states, due to different excitation and quenching rates. Associating the position of the streamer head with the maximum value of the self-enhanced electric field, a delay of 160 ps was experimentally foundmore » for the peak emission of the first negative system of N{sub 2}{sup +}. A delay dilatation was observed experimentally on early-stage streamers and the general mechanism of this phenomenon is clarified theoretically. In the case of the second positive system of N{sub 2}, the delay can reach as much as 400 ps. In contrast to the highly nonlinear behavior of streamer events, it is shown theoretically that emission maximum delays linearly depend on the ratio of the streamer radius and its velocity. This is found to be one of the fundamental streamer features and its use in streamer head diagnostics is proposed. Moreover, radially resolved spectra are synthesized for selected subsequent picosecond moments in order to visualize spectrometric fingerprints of radial structures of N{sub 2}(C{sup 3}Π{sub u}) and N{sub 2}{sup +}(B{sup 2}Σ{sub u}{sup +}) populations created by streamer-head electrons.« less

Microbial communities and greenhouse gas emissions associated with the biodegradation of specified risk material in compost

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

Xu, Shanwei; Agriculture and Agri-Food Canada, Lethbridge Research Centre, P.O. Box 3000, Lethbridge, Alberta, Canada T1J 4B1; Reuter, Tim

Highlights: ► Addition of feathers altered bacterial and fungal communities in compost. ► Microbial communities degrading SRM and compost matrix were distinct. ► Addition of feathers may enrich for microbial communities that degrade SRM. ► Inclusion of feather in compost increased both CH{sub 4} and N{sub 2}O emissions from compost. ► Density of methanogens and methanotrophs were weakly associated with CH{sub 4} emissions. - Abstract: Provided that infectious prions (PrP{sup Sc}) are inactivated, composting of specified risk material (SRM) may be a viable alternative to rendering and landfilling. In this study, bacterial and fungal communities as well as greenhouse gasmore » emissions associated with the degradation of SRM were examined in laboratory composters over two 14 day composting cycles. Chicken feathers were mixed into compost to enrich for microbial communities involved in the degradation of keratin and other recalcitrant proteins such as prions. Feathers altered the composition of bacterial and fungal communities primarily during the first cycle. The bacterial genera Saccharomonospora, Thermobifida, Thermoactinomycetaceae, Thiohalospira, Pseudomonas, Actinomadura, and Enterobacter, and the fungal genera Dothideomycetes, Cladosporium, Chaetomium, and Trichaptum were identified as candidates involved in SRM degradation. Feathers increased (P < 0.05) headspace concentrations of CH{sub 4} primarily during the early stages of the first cycle and N{sub 2}O during the second. Although inclusion of feathers in compost increases greenhouse gas emissions, it may promote the establishment of microbial communities that are more adept at degrading SRM and recalcitrant proteins such as keratin and PrP{sup Sc}.« less

Measurements of radiological data of some amino acids in the energy range 0.122-1.330MeV

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

Lokhande, Rajkumar M., E-mail: rajml358@gmail.com; More, Chaitali V.; Surung, Bharat S.

Radiological parameters such as μ{sub m}, σ{sub t}, σ{sub e}, Z{sub eff} and N{sub eff} of amino acids, namely Lysine (C{sub 6}H{sub 15}N{sub 2}O{sub 2}), Histidine (C{sub 6}H{sub 9}N{sub 3}O{sub 2}) and Arginine (C{sub 6}H{sub 15}N{sub 4}O{sub 2}), were measured using NaI (Tl)-based gamma spectrometry. Radioactive sources used in the study are {sup 57}Co, {sup 133}Ba, {sup 137}Cs, {sup 54}Mn, {sup 60}Co and {sup 22}Na. Gamma ray transmission method in a narrow beam good geometry set up was used in the study. The measured data were compared against XCOM-based data. The agreement is within 2%.

Nitrogen chemistry during burnout in fuel-staged combustion

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

Kristensen, P.G.; Glarborg, P.; Dam-Johansen, K.

A parametric study of the chemistry of the burnout zone in reburning has been performed in laboratory plug flow reactors in the temperature range 800--1,350 K. Inlet mole fractions of NO, NH{sub 3}, HCN, CO, and O{sub 2} were varied, together with different temperatures and residence times to simulate reaction conditions in practical systems. Under lean conditions, a minimum in NO emission exists as a function of temperature. Both HCN and NH{sub 3} can act as either NO reductants or as sources for NO by oxidation. Reactions and selectivities for HCN and NH{sub 3} are controlled by the radical poolmore » produced by fuel (CO) oxidation. As increasing amounts of CO were added, temperatures for both ignition and the minimum in NO became lower. At 2% CO, 4% O{sub 2}, and 100 ms residence time, the minimum in NO was found at approximately 1,000 K. At low temperatures, significant amounts of N{sub 2}O were measured in the reactor outlet. This is attributed to N{sub 2}O formation by HCN/NO reactions and to the slow decomposition of N{sub 2}O at these temperatures. Large reductions in NO were seen under fuel-rich conditions and at high temperatures. The observed NO reduction was very much dependent on the inlet mole fraction of O{sub 2}. Detailed chemical kinetic modeling of the experiments showed reasonable predictions for overall fuel-lean conditions, but the model failed to predict experimental results under fuel-rich conditions. The present results provide guidelines for optimizing the conditions for the burnout process of reburning, as well as other processes for NO{sub x} reduction by staged combustion. The results also provide a test basis for verifying kinetic models for nitrogen chemistry at low temperatures (800--1,350 K).« less

Study of SiO{sub 2}/4H-SiC interface nitridation by post-oxidation annealing in pure nitrogen gas

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

Chanthaphan, Atthawut, E-mail: chanthaphan@asf.mls.eng.osaka-u.ac.jp; Hosoi, Takuji, E-mail: hosoi@mls.eng.osaka-u.ac.jp; Shimura, Takayoshi

An alternative and effective method to perform interface nitridation for 4H-SiC metal-oxide-semiconductor (MOS) devices was developed. We found that the high-temperature post-oxidation annealing (POA) in N{sub 2} ambient was beneficial to incorporate a sufficient amount of nitrogen atoms directly into thermal SiO{sub 2}/SiC interfaces. Although N{sub 2}-POA was ineffective for samples with thick thermal oxide layers, interface nitridation using N{sub 2}-POA was achieved under certain conditions, i.e., thin SiO{sub 2} layers (< 15 nm) and high annealing temperatures (>1350°C). Electrical characterizations of SiC-MOS capacitors treated with high-temperature N{sub 2}-POA revealed the same evidence of slow trap passivation and fast trapmore » generation that occurred in NO-treated devices fabricated with the optimized nitridation conditions.« less

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

Zheng, Rui; School of Mathematics and Information Science, North China University of Water Resources and Electric Power, Zhengzhou 450011; Zheng, Limin

Theoretical studies of the potential energy surface (PES) and bound states are performed for the N{sub 2}–N{sub 2}O van der Waals (vdW) complex. A four-dimensional intermolecular PES is constructed at the level of single and double excitation coupled-cluster method with a non-iterative perturbation treatment of triple excitations [CCSD(T)] with aug-cc-pVTZ basis set supplemented with bond functions. Two equivalent T-shaped global minima are located, in which the O atom of N{sub 2}O monomer is near the N{sub 2} monomer. The intermolecular fundamental vibrational states are assigned by inspecting the orientation of the nodal surface of the wavefunctions. The calculated frequency formore » intermolecular disrotation mode is 23.086 cm{sup −1}, which is in good agreement with the available experimental data of 22.334 cm{sup −1}. A negligible tunneling splitting with the value of 4.2 MHz is determined for the ground vibrational state and the tunneling splitting increases as the increment of the vibrational frequencies. Rotational levels and transition frequencies are calculated for both isotopomers {sup 14}N{sub 2}–N{sub 2}O and {sup 15}N{sub 2}–N{sub 2}O. The accuracy of the PES is validated by the good agreement between theoretical and experimental results for the transition frequencies and spectroscopic parameters.« less

Nitrous oxide reduction in nodules: denitrification or N/sub 2/ fixation

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

Coyne, M.S.; Focht, D.D.

1987-05-01

Detached cowpea nodules that contained a nitrous oxide reductase-positive (Nor/sup +/) rhizobium strain (8A55) and a nitrous oxide reductase-negative (Nor/sup -/) rhizobium strain (32H1) were incubated with 1% /sup 15/N/sub 2/O (95 atom% /sup 15/N) in the following three atmospheres: aerobic with C/sub 2/H/sub 2/ (10%), aerobic without C/sub 2/H/sub 2/, and anaerobic (argon atmosphere) without C/sub 2/H/sub 2/. The greatest production of /sup 15/N/sub 2/ occurred anaerobically with 8A55, yet very little was formed with 32H1. Although acetylene reduction activity was slightly higher with 32H1, about 10 times more /sup 15/N/sub 2/ was produced aerobically by 8A55 than bymore » 32H1 in the absence of acetylene. The major reductive pathway of N/sub 2/O reduction by denitrifying rhizobium strain 8A55 is by nitrous oxide reductase rather than nitrogenase.« less

Cerenkov emission of acoustic phonons electrically generated from three-dimensional Dirac semimetals

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

Kubakaddi, S. S., E-mail: sskubakaddi@gmail.com

2016-05-21

Cerenkov acoustic phonon emission is theoretically investigated in a three-dimensional Dirac semimetal (3DDS) when it is driven by a dc electric field E. Numerical calculations are made for Cd{sub 3}As{sub 2} in which mobility and electron concentration are large. We find that Cerenkov emission of acoustic phonons takes place when the electron drift velocity v{sub d} is greater than the sound velocity v{sub s}. This occurs at small E (∼few V/cm) due to large mobility. Frequency (ω{sub q}) and angular (θ) distribution of phonon emission spectrum P(ω{sub q}, θ) are studied for different electron drift velocities v{sub d} (i.e., differentmore » E) and electron concentrations n{sub e}. The frequency dependence of P(ω{sub q}, θ) shows a maximum P{sub m}(ω{sub q}, θ) at about ω{sub m} ≈ 1 THz and is found to increase with the increasing v{sub d} and n{sub e}. The value of ω{sub m} shifts to higher region for larger n{sub e}. It is found that ω{sub m}/n{sub e}{sup 1/3} and P{sub m}(ω{sub q}, θ)/n{sub e}{sup 2/3} are nearly constants. The latter is in contrast with the P{sub m}(ω{sub q}, θ)n{sub e}{sup 1/2 }= constant in conventional bulk semiconductor. Each maximum is followed by a vanishing spectrum at nearly “2k{sub f} cutoff,” where k{sub f} is the Fermi wave vector. Angular dependence of P(ω{sub q}, θ) and the intensity P(θ) of the phonon emission shows a maximum at an emission angle 45° and is found to increase with increasing v{sub d}. P(θ) is found to increase linearly with n{sub e} giving the ratio P(θ)/(n{sub e}v{sub d}) nearly a constant. We suggest that it is possible to have the controlled Cerenkov emission and generation of acoustic phonons with the proper choice of E, θ, and n{sub e}. 3DDS with large n{sub e} and mobility can be a good source of acoustic phonon generation in ∼THz regime.« less

Results of Detailed Modeling of the Narrow-Line Region of Seyfert Galaxies

NASA Technical Reports Server (NTRS)

Moore, David; Cohen, Ross D.

1996-01-01

We present model line profiles of [O II] lambda3727, [Ne III] lambda3869, [O I] lambda5007, [Fe VII] lambda6087, [Fe X] lambda6374, [O I] lambda6300, H(alpha) lambda6563, and [S 2] lambda6731. The profiles presented here illustrate explicitly the pronounced effects that collisional de-excitation, and that spatial variations in both the ionization parameter and cloud column density, have on Narrow-Line Region (NLR) model profiles. The above effects were included only qualitatively in a previous analytical treatment by Moore and Cohen. By making a direct correspondence between these model profiles and the analytical model profiles of Moore and Cohen, and by comparing with the observed profiles presented in a companion paper and also with those presented elsewhere in the literature, we strengthen some of the conclusions of Moore and Cohen. Most notably, we argue for constant ionization parameter, uniformly accelerated outflow of clouds that are individually stratified in ionization, and the interpretation of emission-line width correlations with ionization potential as a column density effect. For comparison with previous observational studies, such as our own in a companion paper, we also calculate profile parameters for some of the models, and we present and discuss the resulting line width correlations with critical density (n(sub cr)) and Ionization Potential (IP). Because the models we favor are those that produce extended profile wings as observed in high spectral resolution studies, the line width correlations of our favoured models are of particular interest. Line width correlations with n(sub cr) and/or IP result only if the width parameter is more sensitive to extended profile wings than is the Full Width at Half-Maximum (FWHM). Correlations between FWHM and n(sub cr) and/or IP result only after convolving the model profiles with a broad instrumental profile that simulates the lower spectral resolution used in early observational studies. The model in agreement with the greatest number of observational considerations has electron density decreasing outward from n(sub e) approx. equals 10(exp 6)/cu cm to n(sub e) approx. equals 10(exp 2)/cu cm and, due to collisional de-excitation effects in the lowest velocity clouds, it generates broad flat-topped profile peaks in the lines of lowest critical density (e.g., [O II] lambda3727 and [S II] lambda(lambda)6716, 6731). Because the observed profile peaks of both low and high critical density lines are often very similar, our favored model requires a contribution to NLR emission-line spectra from low-velocity, low-density, and low-ionization gas not included in the model NLR.

Process-based approach for the detection of deep gas invading the surface

DOEpatents

Romanak, Katherine; Bennett, Philip C.

2017-05-09

The present invention includes a method for determining the level of deep gas in a near surface formation that includes: measuring CO.sub.2, O.sub.2, CH.sub.4, and N.sub.2 levels in percent by volume from one or more surface or near surface geological samples; adding the water vapor content to the measured CO.sub.2, O.sub.2, CH.sub.4, and N.sub.2 levels in percent by volume; normalizing the gas mixture to 100% by volume or 1 atmospheric total pressure; and determining the ratios of: O.sub.2 versus CO.sub.2 to distinguish in-situ vadose zone CO.sub.2 from exogenous deep leakage CO.sub.2; CO.sub.2 versus N.sub.2 to distinguish whether CO.sub.2 is being removed from the near surface formation or CO.sub.2 is added from an exogenous deep leakage input; or CO.sub.2 versus N.sub.2/O.sub.2 to determine the degree of oxygen influx, consumption, or both; wherein the ratios are indicative of natural in situ CO.sub.2 or CO.sub.2 from the exogenous deep leakage input.

Production mechanism of atomic nitrogen in atmospheric pressure pulsed corona discharge measured using two-photon absorption laser-induced fluorescence

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

Teramoto, Yoshiyuki; Ono, Ryo; Oda, Tetsuji

To study the production mechanism of atomic nitrogen, the temporal profile and spatial distribution of atomic nitrogen are measured in atmospheric pressure pulsed positive corona discharge using two-photon absorption laser-induced fluorescence. The absolute atomic nitrogen density in the streamer filaments is estimated from decay rate of atomic nitrogen in N{sub 2} discharge. The results indicate that the absolute atomic nitrogen density is approximately constant against discharge energy. When the discharge voltage is 21.5 kV, production yield of atomic nitrogen produced by an N{sub 2} discharge pulse is estimated to be 2.9 - 9.8 Multiplication-Sign 10{sup 13} atoms and the energymore » efficiency of atomic nitrogen production is estimated to be about 1.8 - 6.1 Multiplication-Sign 10{sup 16} atoms/J. The energy efficiency of atomic nitrogen production in N{sub 2} discharge is constant against the discharge energy, while that in N{sub 2}/O{sub 2} discharge increases with discharge energy. In the N{sub 2}/O{sub 2} discharge, two-step process of N{sub 2} dissociation plays significant role for atomic nitrogen production.« less

Nonadiabatic dynamics of O({sup 1}D) + N{sub 2}(X{sup 1}{Sigma}{sub g}{sup +}){yields}O({sup 3}P) + N{sub 2}(X{sup 1}{Sigma}{sub g}{sup +}) on three coupled potential surfaces: Symmetry, Coriolis, spin-orbit, and Renner-Teller effects

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

Defazio, Paolo; Gamallo, Pablo; Petrongolo, Carlo

2012-02-07

We present the spin-orbit (SO) and Renner-Teller (RT) quantum dynamics of the spin-forbidden quenching O({sup 1}D) + N{sub 2}(X{sup 1}{Sigma}{sub g}{sup +}){yields}O({sup 3}P) + N{sub 2}(X{sup 1}{Sigma}{sub g}{sup +}) on the N{sub 2}O X-tilde{sup 1}A{sup '}, a-tilde{sup 3}A', and b-tilde{sup 3}A{sup '} coupled PESs. We use the permutation-inversion symmetry, propagate coupled-channel (CC) real wavepackets, and compute initial-state-resolved probabilities and cross sections {sigma}{sub j0} for the ground vibrational and the first two rotational states of N{sub 2}, j{sub 0}= 0 and 1. Labeling symmetry angular states by j and K, we report selection rules for j and for the minimum Kmore » value associated with any electronic state, showing that a-tilde{sup 3}A' is uncoupled in the centrifugal-sudden (CS) approximation at j{sub 0}= 0. The dynamics is resonance-dominated, the probabilities are larger at low K, {sigma}{sub j0} decrease with the collision energy and increase with j{sub 0}, and the CS {sigma}{sub 0} is lower than the CC one. The nonadiabatic interactions play different roles on the quenching dynamics, because the X-tilde{sup 1}A{sup '}-b-tilde{sup 3}A{sup '} SO effects are those most important while the a-tilde{sup 3}A'-b-tilde{sup 3}A{sup '} RT ones are negligible.« less

Solubility and diffusivity of N{sub 2}O and CO{sub 2} in (diethanolamine + N-methyldiethanolamine + water) and in (diethanolamine + 2-amino-2-methyl-1-propanol + water)

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

Li, M.H.; Lee, W.C.

1996-05-01

Acid gases such as CO{sub 2} and H{sub 2}S are frequently removed from natural gas, synthetic natural gas, and other process gas streams by means of absorption into aqueous alkanol-amine solutions. The solubility and diffusivity of N{sub 2}O in (diethanolamine + N-methyldiethanolamine + water) and in (diethanolamine + 2-amino-2-methyl-1-propanol + water) were measured at (30, 35, and 40)C and at atmospheric pressure. Five (diethanolamine + N-methyldiethanolamine + water) and four (diethanolamine + 2-amino-2-methyl-1-propanol + water) systems were studied. The total amine mass percent in all cases was 30. A solubility apparatus was used to measure the solubility of N{sub 2}Omore » in amine solutions. The diffusivity was measured by a wetted wall column absorber. The N{sub 2}O analogy was used to estimate the solubility and diffusivity of CO{sub 2} in (diethanolamine + N-methyldiethanolamine + water) and in (diethanolamine + 2-amino-2-methyl-1-propanol + water).« less

Combined effects of short-term rainfall patterns and soil texture on nitrogen cycling -- A Modeling Analysis

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

Gu, C.; Riley, W.J.

2009-11-01

Precipitation variability and magnitude are expected to change in many parts of the world over the 21st century. We examined the potential effects of intra-annual rainfall patterns on soil nitrogen (N) transport and transformation in the unsaturated soil zone using a deterministic dynamic modeling approach. The model (TOUGHREACT-N), which has been tested and applied in several experimental and observational systems, mechanistically accounts for microbial activity, soil-moisture dynamics that respond to precipitation variability, and gaseous and aqueous tracer transport in the soil. Here, we further tested and calibrated the model against data from a precipitation variability experiment in a tropical systemmore » in Costa Rica. The model was then used to simulate responses of soil moisture, microbial dynamics, nitrogen (N) aqueous and gaseous species, N leaching, and N trace-gas emissions to changes in rainfall patterns; the effect of soil texture was also examined. The temporal variability of nitrate leaching and NO, N{sub 2}, and N{sub 2}O effluxes were significantly influenced by rainfall dynamics. Soil texture combined with rainfall dynamics altered soil moisture dynamics, and consequently regulated soil N responses to precipitation changes. The clay loam soil more effectively buffered water stress during relatively long intervals between precipitation events, particularly after a large rainfall event. Subsequent soil N aqueous and gaseous losses showed either increases or decreases in response to increasing precipitation variability due to complex soil moisture dynamics. For a high rainfall scenario, high precipitation variability resulted in as high as 2.4-, 2.4-, 1.2-, and 13-fold increases in NH{sub 3}, NO, N{sub 2}O and NO{sub 3}{sup -} fluxes, respectively, in clay loam soil. In sandy loam soil, however, NO and N{sub 2}O fluxes decreased by 15% and 28%, respectively, in response to high precipitation variability. Our results demonstrate that soil N cycling responses to increasing precipitation variability depends on precipitation amount and soil texture, and that accurate prediction of future N cycling and gas effluxes requires models with relatively sophisticated representation of the relevant processes.« less

CW EC-QCL-based sensor for simultaneous detection of H₂O, HDO, N₂O and CH₄ using multi-pass absorption spectroscopy.

PubMed

Yu, Yajun; Sanchez, Nancy P; Griffin, Robert J; Tittel, Frank K

2016-05-16

A sensor system based on a continuous wave, external-cavity quantum-cascade laser (CW EC-QCL) was demonstrated for simultaneous detection of atmospheric H₂O, HDO, N₂O and CH₄ using a compact, dense pattern multi-pass gas cell with an effective path-length of 57.6 m. The EC-QCL with a mode-hop-free spectral range of 1225-1285 cm^-1 operating at ~7.8 µm was scanned covering four neighboring absorption lines, for H₂O at 1281.161 cm^-1, HDO at 1281.455 cm^-1, N₂O at 1281.53 cm^-1 and CH₄ at 1281.61 cm^-1. A first-harmonic-normalized wavelength modulation spectroscopy with second-harmonic detection (WMS-2f/1f) strategy was employed for data processing. An Allan-Werle deviation analysis indicated that minimum detection limits of 1.77 ppmv for H₂O, 3.92 ppbv for HDO, 1.43 ppbv for N₂O, and 2.2 ppbv for CH₄ were achieved with integration times of 50-s, 50-s, 100-s and 129-s, respectively. Experimental measurements of ambient air are also reported.

Baryon masses and axial couplings in the combined 1/N{sub c} and Chiral expansions

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

Alvaro Calle Cordon, Jose Goity

The effective theory for baryons with a combined 1/N{sub c} and chiral expansions is analyzed for non-strange baryons. Results for baryon masses and axial couplings are obtained in the small scale expansion, to be coined as the {xi}-expansion, in which the 1/N{sub c} and the low energy power countings are linked according to 1/N{sub c}=O({xi})=O(p). Masses and axial couplings are analyzed to O({xi}{sup 3}) and O({xi}{sup 2}) respectively, which correspond to next-to-next to leading order evaluations, and require one-loop contributions in the effective theory. The role of the spin-flavor approximate symmetry in baryons, consequence of the large N{sub c} limit,more » is manifested in the physical world with N{sub c}=3 in a significant way, as the analysis of its breaking in the masses and the axial couplings show. Applications to the recent lattice QCD results on baryon masses and the nucleon's axial coupling are presented. It is shown that those results are naturally described within the effective theory at the order considered in the {xi}-expansion.« less

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

Li, Yeping, E-mail: ypli@ujs.edu.cn; Huang, Liying; Xu, Jingbo

Highlights: • Novel MoO{sub 3}–C{sub 3}N{sub 4} composite was prepared by a mixing-calcination method. • The MoO{sub 3}–C{sub 3}N{sub 4} composite shows remarkably enhanced absorption of visible light. • The MoO{sub 3}–C{sub 3}N{sub 4} composite shows superior visible-light photocatalytic activity. - Abstract: Composite photocatalyst of blue MoO{sub 3}/g-C{sub 3}N{sub 4} (denoted as MoO{sub 3}–C{sub 3}N{sub 4}) was prepared by a simple mixing-calcination method. The obtained MoO{sub 3}–C{sub 3}N{sub 4} composite contains a low amount of molybdenum blue and shows remarkably enhanced absorption of visible light and high efficiency for the degradation of methylene blue dye (MB) under visible light. Themore » enhancement of visible light photocatalytic activity in MoO{sub 3}–C{sub 3}N{sub 4} is attributed to the synergetic effect: (i) the strong and wide absorption of visible light, (ii) the high separation and easy transfer of photogenerated electron–hole pairs at the heterojunction interfaces derived from the match of band position between the g-C{sub 3}N{sub 4} and MoO{sub 3}.« less

Catalysis on Mo(CO)/sub 6/-derived supported molybdenum catalysts: CO oxidation with N/sub 2/O

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

Kazusaka, A.; Howe, R.F.

1988-05-01

The catalytic nature of Mo(CO)/sub 6/ supported on ..gamma..-Al/sub 2/O/sub 3/, KOH-doped ..gamma..-Al/sub 2/O/sub 3/, and HY-zeolite was investigated in CO oxidation with N/sub 2/O in comparison with that of a conventional partially reduced MoO/sub 3//..gamma..-Al/sub 2/O/sub 3/ catalyst. Kinetic parameters of this reaction were obtained in the range 0 to 100/sup 0/C; the rate law r = kP/sub N/sub 2/O//sup 1/P/sub CO//sup 0/ was found on all catalysts, and the activation energy was estimated to be 9.1 kcal/mol on the Mo(CO)/sub 6/-derived catalysts and 7.1 kcal/mol on the partially reduced MoO/sub 3//..gamma..-Al/sub 2/O/sub 3/ catalyst. Maximum catalytic activities weremore » obtained by activating the Mo(CO)/sub 6/-derived catalysts at 400/sup 0/C. To obtain similar activity on the MoO/sub 3//..gamma..-Al/sub 2/O/sub 3/ catalyst, it was necessary to reduce at 600/sup 0/C. The former catalysts were deactivated on repeating the reaction. On the basis of these results and those of ESR studies through the activation or deactivation process, an active site on the Mo(CO)/sub 6/-derived catalysts has been proposed. Also, clear IR absorption bands due to chemisorbed CO and N/sub 2/O species were observed on the HY-zeolite-supported catalysts. A reaction mechanism is proposed from the kinetic and IR spectroscopic results.« less

Systematic analysis of α elastic scattering with the São Paulo potential

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

Charry-Pastrana, F. E., E-mail: feecharrypa@unal.edu.co; Pinilla, E. C.

2016-07-07

We describe systematically by collision energy and target mass, alpha elastic scattering angular distributions by using the São Paulo potential as the real part of the optical potential. The imaginary part is proportional to the real one by a factor N{sub i}. We find this parameter by fitting the theoretical angular distributions to the experimental cross sections through a χ{sup 2} minimization. The N{sub i} and their respective uncertainties, σ{sub Ni}, fall in the range 0.4 ≤ N{sub i} ± σ{sub N{sub i}} ≤ 0.8 for all the systems studied.

Theoretical gain optimization studies in 10. 6. mu. m CO/sub 2/--N/sub 2/ gasdynamic lasers. IV. Further results of parametric study

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

Reddy, K.P.J.; Reddy, N.M.

1984-01-01

Based on a method proposed by Reddy and Shanmugasundaram, similar solutions have been obtained for the steady inviscid quasi-one-dimensional nonreacting flow in the supersonic nozzle of CO/sub 2/--N/sub 2/--H/sub 2/O and CO/sub 2/--N/sub 2/--He gasdynamic laser systems. Instead of using the correlations of a nonsimilar function N/sub S/ for pure N/sub 2/ gas, as is done in previous publications, the N/sub S/ correlations are computed here for the actual gas mixtures used in the gasdynamic lasers. Optimum small-signal optical gain and the corresponding optimum values of the operating parameters like reservoir pressure and temperature and nozzle area ratio are computedmore » using these correlations. The present results are compared with the previous results and the main differences are discussed.« less

OH Production Enhancement in Bubbling Pulsed Discharges

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

Lungu, Cristian P.; Porosnicu, Corneliu; Jepu, Ionut

2010-10-13

The generation of active species, such as H{sub 2}O{sub 2}, O{sup *}, OH*, HO{sub 2}*, O{sub 3}, N{sub 2}{sup *}, etc, produced in aqueous solutions by HV pulsed discharges was studied in order to find the most efficient way in waste water treatment taking into account that these species are almost stronger oxidizers than ozone. Plasma was generated inside gas bubbles formed by the argon, air and oxygen gas flow between the special designed electrodes. The pulse width and pulse frequency influence was studied in order to increase the efficiency of the OH active species formation. The produced active speciesmore » were investigated by optical emission spectroscopy and correlated with electrical parameters of the discharges (frequency, pulse width, amplitude, and rise and decay time).« less

A HERSCHEL SURVEY OF THE [N II] 205 {mu}m LINE IN LOCAL LUMINOUS INFRARED GALAXIES: THE [N II] 205 {mu}m EMISSION AS A STAR FORMATION RATE INDICATOR

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

Zhao Yinghe; Gao Yu; Lu, Nanyao

2013-03-01

We present, for the first time, a statistical study of [N II] 205 {mu}m line emission for a large sample of local luminous infrared galaxies using Herschel Spectral and Photometric Imaging Receiver Fourier Transform Spectrometer (SPIRE FTS) data. For our sample of galaxies, we investigate the correlation between the [N II] luminosity (L{sub [N{sub II]}}) and the total infrared luminosity (L{sub IR}), as well as the dependence of L{sub [N{sub II]}}/L{sub IR} ratio on L{sub IR}, far-infrared colors (IRAS f{sub 60}/f{sub 100}), and the [O III] 88 {mu}m to [N II] luminosity ratio. We find that L{sub [N{sub II]}} correlatesmore » almost linearly with L{sub IR} for non-active galactic nucleus galaxies (all having L{sub IR} < 10{sup 12} L{sub Sun }) in our sample, which implies that L{sub [N{sub II]}} can serve as a star formation rate tracer which is particularly useful for high-redshift galaxies that will be observed with forthcoming submillimeter spectroscopic facilities such as the Atacama Large Millimeter/submillimeter Array. Our analysis shows that the deviation from the mean L{sub [N{sub II]}}-L{sub IR} relation correlates with tracers of the ionization parameter, which suggests that the scatter in this relation is mainly due to the variations in the hardness, and/or ionization parameter, of the ambient galactic UV field among the sources in our sample.« less

Improved cross-calibration of Thomson scattering and electron cyclotron emission with ECH on DIII-D

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

Brookman, M. W., E-mail: brookmanmw@fusion.gat.com; Austin, M. E.; McLean, A. G.

2016-11-15

Thomson scattering produces n{sub e} profiles from measurement of scattered laser beam intensity. Rayleigh scattering provides a first calibration of the relation n{sub e} ∝ I{sub TS}, which depends on many factors (e.g., laser alignment and power, optics, and measurement systems). On DIII-D, the n{sub e} calibration is adjusted against an absolute n{sub e} from the density-driven cutoff of the 48 channel 2nd harmonic X-mode electron cyclotron emission system. This method has been used to calibrate Thomson n{sub e} from the edge to near the core (r/a > 0.15). Application of core electron cyclotron heating improves the quality of cutoffmore » and depth of its penetration into the core, and also changes underlying MHD activity, minimizing crashes which confound calibration. Less fueling is needed as “ECH pump-out” generates a plasma ready to take up gas. On removal of gyrotron power, cutoff penetrates into the core as channels fall successively and smoothly into cutoff.« less

Highly spatially resolved structural and optical investigation of Bi nanoparticles in Y-Er disilicate thin films

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

Scarangella, A.; Dipartimento di Fisica e Astronomia, Università di Catania, Via S. Sofia 64, 95123 Catania; Amiard, G.

2016-08-08

Er-containing silicon compatible materials have been widely used as infrared emitters for microphotonics application. In this field, the additional introduction of a proper sensitizer permits to increase the Er excitation cross sections, thus increasing its optical efficiency. This work aims to investigate the influence of a post-transition metal, bismuth, on the optical properties of erbium-yttrium disilicate thin films synthesized by magnetron co-sputtering. After thermal treatments at 1000 °C in O{sub 2} or N{sub 2} environment, the presence of small precipitates, about 6 nm in diameter, was evidenced by transmission electron microscopy analyses. The spatially resolved chemical nature of the nanoparticles was discernedmore » in the Si and O rich environments by means of scanning transmission electron microscopy–energy dispersive X-ray and scanning transmission electron microscopy–electron energy loss spectroscopy analyses performed with nanometric resolution. In particular, metallic Bi nanoparticles were stabilized in the N{sub 2} environment, being strongly detrimental for the Er emission. A different scenario was instead observed in O{sub 2}, where the formation of Bi silicate nanoparticles was demonstrated with the support of photoluminescence excitation spectroscopy. In particular, a broad band peaked at 255 nm, correlated to the excitation band of Bi silicate nanoparticles, was identified in Er excitation spectrum. Thus Bi silicate clusters act as sensitizer for Er ions, permitting to improve Er emission up to 250 times with respect to the resonant condition. Moreover, the Er decay time increases in the presence of the Bi silicate nanoparticles that act as cages for Er ions. These last results permit to further increase Er optical efficiency in the infrared range, suggesting (Bi + Er)-Y disilicate as a good candidate for applications in microphotonics.« less

Effects of the electrical parameters and gas flow rate on the generation of reactive species in liquids exposed to atmospheric pressure plasma jets

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

Baek, Eun Jeong; Joh, Hea Min; Kim, Sun Ja

2016-07-15

In this work, an atmospheric pressure plasma jet was fabricated and studied for plasma–liquid interactions. The plasma jet consists of a quartz-covered pin electrode and outer quartz tube with a tapered nozzle. Using the current–voltage (I-V) and optical emission characteristics of the plasma jet, the plasma density and the speed of the plume were investigated. The optical emission spectra clearly indicated the excited NO, O, OH, N{sub 2}, and N{sub 2}{sup +} in the plasma plumes. Then the plasma jets were applied to the deionized water. We investigated the effects of the operating parameters such as applied voltage, pulse frequency,more » and gas flow rate on the generation of reactive species in the gas and liquid phases. The densities of reactive species including OH radicals were obtained at the plasma–liquid surface and inside the plasma-treated liquids using ultraviolet absorption spectroscopy and chemical probe method. The nitrite concentration was detected by Griess assay. The data are very suggestive that there is a strong correlation among the production of reactive oxygen and nitrogen species (RONS) in the plasmas and liquids.« less

Vector correlation between the alignment of reactant N{sub 2} (A {sup 3}Σ{sub u}{sup +}) and the alignment of product NO (A {sup 2}Σ{sup +}) rotation in the energy transfer reaction of aligned N{sub 2} (A {sup 3}Σ{sub u}{sup +}) + NO (X {sup 2}Π) → NO (A {sup 2}Σ{sup +}) + N{sub 2} (X {sup 1}Σ{sub g}{sup +})

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

Ohoyama, H., E-mail: ohyama@chem.sci.osaka-u.ac.jp

2013-12-21

The vector correlation between the alignment of reactant N{sub 2} (A {sup 3}Σ{sub u}{sup +}) and the alignment of product NO (A {sup 2}Σ{sup +}) rotation has been studied in the energy transfer reaction of aligned N{sub 2} (A {sup 3}Σ{sub u}{sup +}) + NO (X {sup 2}Π) → NO (A {sup 2}Σ{sup +}) + N{sub 2} (X {sup 1}Σ{sub g}{sup +}) under the crossed beam condition at a collision energy of ∼0.07 eV. NO (A {sup 2}Σ{sup +}) emission in the two linear polarization directions (i.e., parallel and perpendicular with respect to the relative velocity vector v{sub R}) hasmore » been measured as a function of the alignment of N{sub 2} (A {sup 3}Σ{sub u}{sup +}) along its molecular axis in the collision frame. The degree of polarization of NO (A {sup 2}Σ{sup +}) emission is found to depend on the alignment angle (θ{sub v{sub R}}) of N{sub 2} (A {sup 3}Σ{sub u}{sup +}) in the collision frame. The shape of the steric opacity function at the two polarization conditions turns out to be extremely different from each other: The steric opacity function at the parallel polarization condition is more favorable for the oblique configuration of N{sub 2} (A {sup 3}Σ{sub u}{sup +}) at an alignment angle of θ{sub v{sub R}} ∼ 45° as compared with that at the perpendicular polarization condition. The alignment of N{sub 2} (A {sup 3}Σ{sub u}{sup +}) is found to give a significant effect on the alignment of NO (A {sup 2}Σ{sup +}) rotation in the collision frame: The N{sub 2} (A {sup 3}Σ{sub u}{sup +}) configuration at an oblique alignment angle θ{sub v{sub R}} ∼ 45° leads to a parallel alignment of NO (A {sup 2}Σ{sup +}) rotation (J-vector) with respect to v{sub R}, while the axial and sideways configurations of N{sub 2} (A {sup 3}Σ{sub u}{sup +}) lead to a perpendicular alignment of NO (A {sup 2}Σ{sup +}) rotation with respect to v{sub R}. These stereocorrelated alignments of the product rotation have a good correlation with the stereocorrelated reactivity observed in the multi-dimensional steric opacity function [H. Ohoyama and S. Maruyama, J. Chem. Phys. 137, 064311 (2012)].« less

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

Goulianos, K.; /Rockefeller U.

The charged multiplicity distributions of the diffractive and non-diffractive components of hadronic interactions, as well as those of hadronic states produced in other reactions, are described well by a universal Gaussian function that depends only on the available mass for pionization, has a maximum at n{sub o} {approx_equal} 2M{sup 1/2}, where M is the available mass in GeV, and a peak to width ratio n{sub o}/D {approx_equal} 2.

g-C{sub 3}N{sub 4}/NaTaO{sub 3} organic–inorganic hybrid nanocomposite: High-performance and recyclable visible light driven photocatalyst

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

Kumar, Santosh; Kumar, Bharat; Surendar, T.

2014-01-01

Graphical abstract: High-performance and recyclable visible-light driven g-C{sub 3}N{sub 4}/NaTaO{sub 3} hybrid nanocomposite photocatalysts have been prepared by a facile ultrasonic dispersion method. The hybrid nanocomposite photocatalyst can be promising photocatalytic material for practical application in water splitting and environmental remediation. - Highlights: • Novel g-C{sub 3}N{sub 4}/NaTaO{sub 3} nanocomposites as a high performance and recyclable photocatalysts. • These catalysts exhibited significantly enhanced photocatalytic activity under UV–visible light irradiation. • More attractively, dramatic activity is generated under visible light irradiation due to the g-C{sub 3}N{sub 4} loaded. • Interestingly, the as-prepared hybrid nanocomposites possess high reusability. - Abstract: Novel g-C{submore » 3}N{sub 4}/NaTaO{sub 3} hybrid nanocomposites have been prepared by a facile ultrasonic dispersion method. Our results clearly show the formation of interface between NaTaO{sub 3} and g-C{sub 3}N{sub 4} and further loading of g-C{sub 3}N{sub 4} did not affect the crystal structure and morphology of NaTaO{sub 3}. The g-C{sub 3}N{sub 4}/NaTaO{sub 3} nanocomposites exhibited enhanced photocatalytic performance for the degradation of Rhodamine B under UV–visible and visible light irradiation compared to pure NaTaO{sub 3} and Degussa P25. Interestingly, the visible light photocatalytic activity is generated due to the loading of g-C{sub 3}N{sub 4}. A mechanism is proposed to discuss the enhanced photocatalytic activity based on trapping experiments of photoinduced radicals and holes. Under visible light irradiation, electron excited from the valance band (VB) to conduction band (CB) of g-C{sub 3}N{sub 4} could directly inject into the CB of NaTaO{sub 3}, making g-C{sub 3}N{sub 4}/NaTaO{sub 3} visible light driven photocatalyst. Since the as-prepared hybrid nanocomposites possess high reusability therefore it can be promising photocatalyst for environmental applications.« less

The cold and atmospheric-pressure air surface barrier discharge plasma for large-area sterilization applications

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

Wang Dacheng; Department of Aeronautics, Fujian Key Laboratory for Plasma and Magnetic Resonance, School of Physics and Mechanical and Electrical Engineering, Xiamen University, Xiamen, Fujian 361005; Zhao Di

2011-04-18

This letter reports a stable air surface barrier discharge device for large-area sterilization applications at room temperature. This design may result in visually uniform plasmas with the electrode area scaled up (or down) to the required size. A comparison for the survival rates of Escherichia coli from air, N{sub 2} and O{sub 2} surface barrier discharge plasmas is presented, and the air surface plasma consisting of strong filamentary discharges can efficiently kill Escherichia coli. Optical emission measurements indicate that reactive species such as O and OH generated in the room temperature air plasmas play a significant role in the sterilizationmore » process.« less

ISM Parameters in the Normal Galaxy NGC 5713

NASA Technical Reports Server (NTRS)

Lord, S. D.; Malhotra, S.; Lim, T.; Helou, G.; Beichman, C. A.; Dinerstein, H.; Hollenbach, D. J.; Hunter, D. A.; Lo, K. Y.; Lu, N. Y.;

Electron-cyclotron resonance preionization and heating in the Proto-cleo torsatron

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

Goes, L.C.S.

1986-01-01

ECR-breakdown and heating in a bifurcated torsatron topology are investigated with extraordinary mode injection from the high-field side (7.2 GHz/2 KW/10 ms). The breakdown characteristics are explained by stochastic heating enhanced by helical ripple effects. In the quasi-stationary regime (0.01 n/sub cr/ < n < 0.6 n/sub cr/), two-dimensional plasma profiles indicated heating inhomogeneities associated with RF power absorption near the UHR layer. The production of a suprathermal electron population, at the outer plasma edge, was indicated by nonthermal microwave emission and target SXR emission.

Multispecies absorption spectroscopy of detonation events at 100  kHz using a fiber-coupled, time-division-multiplexed quantum-cascade-laser system.

PubMed

Rein, Keith D; Roy, Sukesh; Sanders, Scott T; Caswell, Andrew W; Schauer, Frederick R; Gord, James R

2016-08-10

A mid-infrared fiber-coupled laser system constructed around three time-division-multiplexed quantum-cascade lasers capable of measuring the absorption spectra of CO, CO₂, and N₂O at 100 kHz over a wide range of operating pressures and temperatures is demonstrated. This system is first demonstrated in a laboratory burner and then used to measure temperature, pressure, and concentrations of CO, CO₂, and N₂O as a function of time in a detonated mixture of N₂O and C₃H₈. Both fuel-rich and fuel-lean detonation cases are outlined. High-temperature fluctuations during the blowdown are observed. Concentrations of CO are shown to decrease with time for fuel-lean conditions and increase for fuel-rich conditions.

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

Pan, Zhichen; Li, Di; Qian, Lei

We present 2.5-square-degree C{sub 2}H N = 1–0 and N{sub 2}H{sup +} J = 1–0 maps of the ρ Ophiuchi molecular cloud complex. These are the first large-scale maps of the ρ Ophiuchi molecular cloud complex with these two tracers. The C{sub 2}H emission is spatially more extended than the N{sub 2}H{sup +} emission. One faint N{sub 2}H{sup +} clump, Oph-M, and one C{sub 2}H ring, Oph-RingSW, are identified for the first time. The observed C{sub 2}H-to-N{sub 2}H{sup +} abundance ratio ([C{sub 2}H]/[N{sub 2}H{sup +}]) varies between 5 and 110. We modeled the C{sub 2}H and N{sub 2}H{sup +} abundancesmore » with 1D chemical models, which show a clear decline of [C{sub 2}H]/[N{sub 2}H{sup +}] with chemical age. Such an evolutionary trend is little affected by temperatures when they are below 40 K. At high density ( n {sub H} > 10{sup 5} cm{sup −3}), however, the time it takes for the abundance ratio to drop at least one order of magnitude becomes less than the dynamical time (e.g., turbulence crossing time of ∼10{sup 5} yr). The observed [C{sub 2}H]/[N{sub 2}H{sup +}] difference between L1688 and L1689 can be explained by L1688 having chemically younger gas in relatively less dense regions. The observed [C{sub 2}H]/[N{sub 2}H{sup +}] values are the results of time evolution, accelerated at higher densities. For the relatively low density regions in L1688 where only C{sub 2}H emission was detected, the gas should be chemically younger.« less

NuSTAR Observations of Heavily Obscured Quasars at z Is Approximately 0.5

NASA Technical Reports Server (NTRS)

Lansbury, G. B.; Alexander, D. M.; Del Moro, A.; Gandhi, P.; Assef, R. J.; Stern, D.; Aird, J.; Ballantyne, D. R.; Balokovic, M.; Bauer, F. E.;

Process-based approach for the detection of CO2 injectate leakage

DOEpatents

Romanak, Katherine; Bennett, Philip C.

2017-11-14

The present invention includes a method for distinguishing between a natural source of deep gas and gas leaking from a CO.sub.2 storage reservoir at a near surface formation comprising: obtaining one or more surface or near surface geological samples; measuring a CO.sub.2, an O.sub.2, a CH.sub.4, and an N.sub.2 level from the surface or near surface geological sample; determining the water vapor content at or above the surface or near surface geological samples; normalizing the gas mixture of the CO.sub.2, the O.sub.2, the CH.sub.4, the N.sub.2 and the water vapor content to 100% by volume or 1 atmospheric total pressure; determining: a ratio of CO.sub.2 versus N.sub.2; and a ratio of CO.sub.2 to N.sub.2, wherein if the ratio is greater than that produced by a natural source of deep gas CO.sub.2 or deep gas methane oxidizing to CO.sub.2, the ratio is indicative of gas leaking from a CO.sub.2 storage reservoir.

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

Sukri, Shahratul Ain Mohd; Heng, Lee Yook; Karim, Nurul Huda Abd

A platinum (II) salphen complex was synthesised by condensation reaction of 2,4-dihydroxylbenzaldehyde and o-phenylenediamine with potassium tetrachloroplatinate to obtain N,N′-Bis-4-(hydroxysalicylidene)-phenylenediamine-platinum (II). The structure of the complex was confirmed by {sup 1}H and {sup 13}C NMR spectroscopy, FTIR spectroscopy, CHN elemental analyses and ESI-MS spectrometry. The platinum (II) salphen complex with four donor atoms N{sub 2}O{sub 2} from its salphen ligand coordinated to platinum (II) metal centre were determined. The binding mode and interaction of this complex with calf thymus DNA was determined by UV/Vis DNA titration and emission titration. The intercalation between the DNA bases by π-π stacking due tomore » its square planar geometry and aromatic rings structures was proposed.« less

Emission-line studies of young stars. 4: The optical forbidden lines

NASA Technical Reports Server (NTRS)

Hamann, Fred

1994-01-01

Optical forbidden line strengths and profiles are discussed for a sample of 30 T Tauri stars and 12 Herbig Ae-Be stars. Transitions of (C I), (N II), (O I), (O II), (S II), (Ca II), (Cr II), (Fe II), and (Ni II) are detected. Profile variability occurred in DG Tau and probably other sources. The ensemble profiles can be divided into four generic components that may represent distinct emitting regions; (1) narrow rest-velocity lines, (2) 'low'-velocity lines (peaking at less than or approximately +/- 50 km s(exp -1)), (3) 'high'-velocity (usually greater than or approximately +/- 100 km s(exp -1)) blueshifted peaks or wings, and (4) high-velocity redshifted peaks. Among T Tauri stars, the rest-velocity lines appear most often in sources with weak and narrow permitted lines, such as the Ca II triplet. The low- and high-velocity blueshifted components usually appear together in sources with strong and broad Ca II triplet lines. If the velocity-shifted lines form in jets, the smallest (full) opening angles required by the profiles are less than or approximately 20 deg for the narrow, blueshifted (Ca II) lines of DG Tau and HL Tau. Other lines in DG Tau are much broader, implying larger opening angles or greater velocity dispersions. The variability in DG Tau also implies significant changes in the collimation or velocity coherence on timescales of a few years. RW Aur and AS 353A have blue- and redshifted line peaks that could form in oppositely directed jets. The strong (S II) lambda 6716 and lambda 6731 lines in RW Aur are exclusively redshifted and require opening angles less than or approximately 60 deg. Measurements of different profiles in the same spectrum show that the physical conditions change with the line-of-sight velocities. The most persistent trends are for more (N II) and (O II) and less (O I) lambda 5577 flux at high velocities. Constraints on the physical conditions are derived by modeling the emission lines via multilevel ions in 'coronal ionization equilibrium.' A single temperature and density cannot fully describe the line spectra in any velocity interval. Temperatures in the (O I) region are 9000 less than or approximately T(sub e) less than 14,000 K, and the ionization fraction (of H) is less than 35%. The densities derived from (O I) include n(sub e) less than or approximately 5 x 10(exp 5) to approximately 10(exp 7) cm(exp -3), but n(sub e) greater than or approximately 10(exp 6) cm(exp -3) obtains only at low velocities. In the (S II) regions the densities are lower, 10(exp 3) less than or approximately n(sub e) less than or approximately 7 x 10(exp 4) cm(exp -3), and the temperatures are probably higher, T(sub e) greater than or approximately 13,000 K. At high velocities (only) there is additional hot gas that produces (N II) and (O II), possibly most of the (S II), and little (O I). This region is characterized by T(sub e) greater than or approximately 15,000 K, n(sub e) less than or approximately 10(exp 5) cm(exp -3), and an ionization fraction greater than or approximately 50%. When combined with the spatially segregated emitting regions observed by others by spectral imaging, these results suggest decreasing n(sub e) and increasing T(sub e) away from the star in at least the high velocity gas.

New methodology for modeling annual-aircraft emissions at airports

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

Woodmansey, B.G.; Patterson, J.G.

An as-accurate-as-possible estimation of total-aircraft emissions are an essential component of any environmental-impact assessment done for proposed expansions at major airports. To determine the amount of emissions generated by aircraft using present models it is necessary to know the emission characteristics of all engines that are on all planes using the airport. However, the published data base does not cover all engine types and, therefore, a new methodology is needed to assist in estimating annual emissions from aircraft at airports. Linear regression equations relating quantity of emissions to aircraft weight using a known-fleet mix are developed in this paper. Total-annualmore » emissions for CO, NO[sub x], NMHC, SO[sub x], CO[sub 2], and N[sub 2]O are tabulated for Toronto's international airport for 1990. The regression equations are statistically significant for all emissions except for NMHC from large jets and NO[sub x] and NMHC for piston-engine aircraft. This regression model is a relatively simple, fast, and inexpensive method of obtaining an annual-emission inventory for an airport.« less

Dynamical Timescale of Pre-collapse Evolution Inferred from Chemical Distribution in the Taurus Molecular Cloud-1 (TMC-1) Filament

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

Choi, Yunhee; Lee, Jeong-Eun; Bourke, Tyler L.

We present observations and analyses of the low-mass star-forming region, Taurus Molecular Cloud-1 (TMC-1). CS ( J = 2–1)/N{sub 2}H{sup +} ( J = 1–0) and C{sup 17}O ( J = 2–1)/C{sup 18}O ( J = 2–1) were observed with the Five College Radio Astronomy Observatory and the Seoul Radio Astronomy Observatory, respectively. In addition, Spitzer infrared data and 1.2 mm continuum data observed with Max-Planck Millimetre Bolometer are used. We also perform chemical modeling to investigate the relative molecular distributions of the TMC-1 filament. Based on Spitzer observations, there is no young stellar object along the TMC-1 filament, while five Classmore » II and one Class I young stellar objects are identified outside the filament. The comparison between column densities calculated from dust continuum and C{sup 17}O 2–1 line emission shows that CO is depleted much more significantly in the ammonia peak than in the cyanopolyyne peak, while the column densities calculated from the dust continuum are similar at the two peaks. N{sub 2}H{sup +} is not depleted much in either peak. According to our chemical calculation, the differential chemical distribution in the two peaks can be explained by different timescales required to reach the same density, i.e., by different dynamical processes.« less

Method for generating O.sub.2-rich gas from air using water

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

Nakano, Anna; Nakano, Jinichiro; Bennett, James P.

The present disclosure is directed to a method for enriching an inlet air stream utilizing a number of enrichment sub-units connected in series, where each enrichment sub-unit conducts both a dissolution and degasification cycle. Each enrichment sub-unit comprises a compressor, an aeration unit, a deaeration unit, and a pump for the recirculation of water between the aeration and deaeration units. The methodology provides a manner in which the relationship between the respective Henry's coefficients of the oxygen and nitrogen in water may be exploited to enrich the O.sub.2 volume percent and diminish the N.sub.2 volume percent over repeated dissolution andmore » degasification cycles. By utilizing a number of enrichment sub-units connected in series, the water contained in each enrichment sub-unit acts to progressively increase the O.sub.2 volume percent. Additional enrichment sub-units may be added and utilized until the O.sub.2 volume percent equals or exceeds a target O.sub.2 volume percent. In a particular embodiment, air having a general composition of about 78 vol. % N.sub.2 and 21 vol. % O.sub.2 is progressively enriched to provide a final mixture of about 92% vol. % O.sub.2 and 8% vol. % N.sub.2.« less

A novel yellow-emitting SrAlSi{sub 4}N{sub 7}:Ce{sup 3+} phosphor for solid state lighting: Synthesis, electronic structure and photoluminescence properties

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

Ruan, Jian; Laboratory of Glasses and Nanostructured Functional Materials, 122 Luoshi Road, Wuhan, Hubei 430070; Xie, Rong-Jun, E-mail: Xie.Rong-Jun@nims.go.jp

2013-12-15

Ce{sup 3+}-doped and Ce{sup 3+}/Li{sup +}-codoped SrAlSi{sub 4}N{sub 7} phosphors were synthesized by gas pressure sintering of powder mixtures of Sr{sub 3}N{sub 2}, AlN, α-Si{sub 3}N{sub 4}, CeN and Li{sub 3}N. The phase purity, electronic crystal structure, photoluminescence properties of SrAlSi{sub 4}N{sub 7}:Ce{sup 3+}(Ce{sup 3+}/Li{sup +}) were investigated in this work. The band structure calculated by the DMol{sup 3} code shows that SrAlSi{sub 4}N{sub 7} has a direct band gap of 3.87 eV. The single crystal analysis of Ce{sup 3+}-doped SrAlSi{sub 4}N{sub 7} indicates a disordered Si/Al distribution and nitrogen vacnacy defects. SrAlSi{sub 4}N{sub 7} was identified as a majormore » phase of the fired powders, and Sr{sub 5}Al{sub 5}Si{sub 21}N{sub 35}O{sub 2} and AlN as minor phases. Both Ce{sup 3+} and Ce{sup 3+}/Li{sup +} doped SrAlSi{sub 4}N{sub 7} phosphors can be efficiently excited by near-UV or blue light and show a broadband yellow emission peaking around 565 nm. A highest external quantum efficiency of 38.3% under the 450 nm excitation was observed for the Ce{sup 3+}/Li{sup +}-doped SrAlSi{sub 4}N{sub 7} (5 mol%). A white light LED lamp with color temperature of 6300 K and color rendering index of Ra=78 was achieved by combining Sr{sub 0.97}Al{sub 1.03}Si{sub 3.997}N/94/maccounttest14=t0005{sub 1}8193 {sub 7}:Ce{sup 3+}{sub 0.03} with a commercial blue InGaN chip. It indicates that SrAlSi{sub 4}N{sub 7}:Ce{sup 3+} is a promising yellow emitting down-conversion phosphor for white LEDs. - Graphical abstract: One-phosphor converted white light-emitting diode (LED) was fabricated by combining a blue LED chip and a yellow-emitting SrAlSi4N7:Ce{sup 3+} phosphor (see inset), which has the color rendering index of 78 and color temperature of 6300 K. - Highlights: • We reported a new yellow nitride phosphor suitable for solid state lighting. • We solved the crystal structure and evidenced a disordered Si/Al distribution. • We fabricated a high color rendering white LEDs by using a single SrAlSi4N7:Ce.« less

Interaction of root nodule size and oxygen pressure on the rate of nitrogen fixation by cowpea and peanut

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

Sen, D.; Weaver, R.W.

1987-04-01

Size and anatomical features of nodules influence the rate of O/sub 2/ diffusion into nodules. Availability of oxygen can be a limiting factor in nitrogen fixation. Larger nodules have thicker cortices and low surface to volume ratio leading to lower rates of gaseous diffusion. Increased oxygen pressure in the environment alters the rate of nitrogen fixation but the rate of change may depend on the nodule size. This was investigated by measuring /sup 15/N/sub 2/ incorporation into nodules. Root nodules from 38 day old cowpea and peanut plants were collected and sorted into size groups having diameters of >3 mm,more » 2-3 mm, and just below 2 mm. Samples of each size group were enclosed in tubes and exposed to various combination of oxygen (8-28%) and /sup 15/N/sub 2/. With higher O/sub 2/ pressure all nodules showed increased N/sub 2/ fixation but the largest nodules showed the maximum increase. Specific activity of larger nodules was higher for N/sub 2/ fixation. For the sizes of nodules examined the largest nodules did not reflect any of the disadvantages of the large size but the benefits of higher rates of O/sub 2/ entry was evident.« less

Nitrogen fixation apparatus

DOEpatents

Chen, Hao-Lin

1984-01-01

A method and apparatus for achieving nitrogen fixation includes a volumetric electric discharge chamber. The volumetric discharge chamber provides an even distribution of an electron beam, and enables the chamber to be maintained at a controlled energy to pressure (E/p) ratio. An E/p ratio of from 5 to 15 kV/atm of O.sub.2 /cm promotes the formation of vibrationally excited N.sub.2. Atomic oxygen interacts with vibrationally excited N.sub.2 at a much quicker rate than unexcited N.sub.2, greatly improving the rate at which NO is formed.

Nitrogen fixation method and apparatus

DOEpatents

Chen, Hao-Lin

1983-01-01

A method and apparatus for achieving nitrogen fixation includes a volumetric electric discharge chamber. The volumetric discharge chamber provides an even distribution of an electron beam, and enables the chamber to be maintained at a controlled energy to pressure (E/p) ratio. An E/p ratio of from 5 to 15 kV/atm of O.sub.2 /cm promotes the formation of vibrationally excited N.sub.2. Atomic oxygen interacts with vibrationally excited N.sub.2 at a much quicker rate than unexcited N.sub.2, greatly improving the rate at which NO is formed.

Nitrogen fixation method and apparatus

DOEpatents

Chen, H.L.

1983-08-16

A method and apparatus for achieving nitrogen fixation includes a volumetric electric discharge chamber. The volumetric discharge chamber provides an even distribution of an electron beam, and enables the chamber to be maintained at a controlled energy to pressure (E/p) ratio. An E/p ratio of from 5 to 15 kV/atm of O[sub 2]/cm promotes the formation of vibrationally excited N[sub 2]. Atomic oxygen interacts with vibrationally excited N[sub 2] at a much quicker rate than unexcited N[sub 2], greatly improving the rate at which NO is formed. 1 fig.

Amorphous indium-tin-zinc oxide films deposited by magnetron sputtering with various reactive gases: Spatial distribution of thin film transistor performance

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

Jia, Junjun; Torigoshi, Yoshifumi; Shigesato, Yuzo, E-mail: yuzo@chem.aoyama.ac.jp

This work presents the spatial distribution of electrical characteristics of amorphous indium-tin-zinc oxide film (a-ITZO), and how they depend on the magnetron sputtering conditions using O{sub 2}, H{sub 2}O, and N{sub 2}O as the reactive gases. Experimental results show that the electrical properties of the N{sub 2}O incorporated a-ITZO film has a weak dependence on the deposition location, which cannot be explained by the bombardment effect of high energy particles, and may be attributed to the difference in the spatial distribution of both the amount and the activity of the reactive gas reaching the substrate surface. The measurement for themore » performance of a-ITZO thin film transistor (TFT) also suggests that the electrical performance and device uniformity of a-ITZO TFTs can be improved significantly by the N{sub 2}O introduction into the deposition process, where the field mobility reach to 30.8 cm{sup 2} V{sup –1} s{sup –1}, which is approximately two times higher than that of the amorphous indium-gallium-zinc oxide TFT.« less

Methane and nitrous oxide (N{sub 2}O) emission characteristics from automobiles

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

Koike, Noriyuki; Odaka, Matsuo

Exhaust gases discharged from automobiles are noticed as one of the reasons for recent increase in atmospheric methane and nitrous oxide concentration, which have been considered as greenhouse gases. In order to make an accurate estimation of methane and nitrous oxide discharged from automobiles, measurement methods were experimentally developed and emissions were measured for different kinds of automobiles under various driving conditions. Then, the authors have tried to estimate the annual global emissions from automobiles using these measurement results and statistical data such as the number of automobiles, the total annual mileage, and the total annual fuel consumption, etc. Themore » emissions from passenger vehicles which have been estimated from the global number of automobiles were 477.263 t/year for methane and 313.472 t/year for nitrous oxide. These numbers are higher than what had been estimated.« less

Reactant gas composition for fuel cell potential control

DOEpatents

Bushnell, Calvin L.; Davis, Christopher L.

1991-01-01

A fuel cell (10) system in which a nitrogen (N.sub.2) gas is used on the anode section (11) and a nitrogen/oxygen (N.sub.2 /O.sub.2) gaseous mix is used on the cathode section (12) to maintain the cathode at an acceptable voltage potential during adverse conditions occurring particularly during off-power conditions, for example, during power plant shutdown, start-up and hot holds. During power plant shutdown, the cathode section is purged with a gaseous mixture of, for example, one-half percent (0.5%) oxygen (O.sub.2) and ninety-nine and a half percent (99.5%) nitrogen (N.sub.2) supplied from an ejector (21) bleeding in air (24/28) into a high pressure stream (27) of nitrogen (N.sub.2) as the primary or majority gas. Thereafter the fuel gas in the fuel processor (31) and the anode section (11) is purged with nitrogen gas to prevent nickel (Ni) carbonyl from forming from the shift catalyst. A switched dummy electrical load (30) is used to bring the cathode potential down rapidly during the start of the purges. The 0.5%/99.5% O.sub.2 /N.sub.2 mixture maintains the cathode potential between 0.3 and 0.7 volts, and this is sufficient to maintain the cathode potential at 0.3 volts for the case of H.sub.2 diffusing to the cathode through a 2 mil thick electrolyte filled matrix and below 0.8 volts for no diffusion at open circuit conditions. The same high pressure gas source (20) is used via a "T" juncture ("T") to purge the anode section and its associated fuel processor (31).

Environmental assessment of a watertube boiler firing a coal-water slurry. Volume 2. Data supplement. Final report, January 1984-March 1985

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

DeRosier, R.; Waterland, L.R.

1986-02-01

This report is a compendium of detailed test sampling and analysis data obtained in field tests of a watertube industrial boiler burning a coal/water slurry (CWS). Test data reported include preliminary stack test data, boiler operating data, and complete flue-gas emission results. Flue-gas emission measurements included continuous monitoring for criteria pollutants; onsite gas chromatography (GC) for volatile hydrocarbons (Cl-C6); Methods 5/8 sampling for particulate, SO/sub 2/, and SO/sub 3/ emissions; source assessment sampling system (SASS) for total organics in two boiling point ranges (100 to 300 C and > 300 C), organic compound category information using infrared spectrometry (IR), liquidmore » column (LC) chromatography separation, and low-resolution mass spectrometry (LRMS), specific quantitation of the semivolatile organic priority pollutants using gas chromatography/mass spectrometry (GC/MS), and trace-element emissions using spark-source mass spectrometry (SSMS) and atomic absorption spectroscopy (AAS); N/sub 2/O emissions by gas chromatography/electron-capture detector (GC/ECD); and biological assay testing of SASS and ash-stream samples.« less

Amine templating effect absent in uranyl sulfates synthesized with 1,4-n-butyldiamine

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

Jouffret, Laurent J., E-mail: ljouffret@nd.edu; Wylie, Ernest M.; Burns, Peter C.

2013-01-15

Two new uranyl sulfates, (C{sub 4}H{sub 14}N{sub 2})[(UO{sub 2}){sub 2}(SO{sub 4}){sub 3}(H{sub 2}O)]{center_dot}2H{sub 2}O (NDUS2) and (C{sub 4}H{sub 14}N{sub 2})[(UO{sub 2})(SO{sub 4}){sub 2}(H{sub 2}O)]{center_dot}2H{sub 2}O (NDUS3), were synthesized and their crystal structures determined. NDUS2 was obtained in highly acidic media heat-treated at 373 K and subsequently maintained at 278 K until crystals formed after two months. NDUS3 results from the degradation of NDUS2 over the course of a few days. NDUS2 and NDUS3 crystallize in the monoclinic space group P2{sub 1}/n, a=10.9075(4) A, b=10.4513(4) A, c=17.7881(7) A, {beta}=97.908(2) Degree-Sign , V=2008.52(13) A{sup 3}, Z=4, at 140 K and a=8.8570(4) A,more » b=7.3299(3) A, c=20.4260(9) A, {beta}=95.140(2) Degree-Sign , V=1320.74(10) A{sup 3}, Z=4, at 140 K, respectively. The compounds contain interlayer 1,4-n-butyldiammonium cations that charge-balance the anionic structural units. - Graphical abstract: Amine templating effect absent in uranyl sulfates synthesized with 1,4-diaminobutane, as shown by the synthesis of two new uranyl sulfates, (C{sub 4}H{sub 14}N{sub 2})[(UO{sub 2}){sub 2}(SO{sub 4}){sub 3}(H{sub 2}O)]{center_dot}2H{sub 2}O (NDUS2) and (C{sub 4}H{sub 14}N{sub 2})[(UO{sub 2})(SO{sub 4}){sub 2}(H{sub 2}O)]{center_dot}2H{sub 2}O (NDUS3). Highlights: Black-Right-Pointing-Pointer Two layered uranyl sulfates were synthesized. Black-Right-Pointing-Pointer Amine molecules are located in the interlayers of the compounds. Black-Right-Pointing-Pointer No templating effect of the amine was observed. Black-Right-Pointing-Pointer Amine molecules are only charge balancing cations in the structures.« less

Crystal structure, chemical expansion and phase stability of HoMnO{sub 3} at high temperature

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

Selbach, Sverre M., E-mail: selbach@material.ntnu.no; Nordli Lovik, Amund; Bergum, Kristin

Anisotropic thermal and chemical expansion of hexagonal HoMnO{sub 3} was investigated by high temperature X-ray diffraction in inert (N{sub 2}) and oxidizing (air) atmospheres up to 1623 K. A second order structural phase transition directly from P6{sub 3}cm to P6{sub 3}/mmc was found at 1298{+-}4 K in N{sub 2} atmosphere, and 1318{+-}4 K in air. For the low temperature polymorph P6{sub 3}cm the contraction of the c-axis was more rapid in inert than in oxidizing atmosphere. The c-axis of the P6{sub 3}/mmc polymorph of HoMnO{sub 3} displayed anomalously high expansion above 1400 K, which is discussed in relation to chemicalmore » expansion caused by point defects. The a-axis expanded stronger in inert than oxidizing atmosphere. Anisotropic chemical and thermal expansion of the P6{sub 3}cm phase of YMnO{sub 3} in N{sub 2}, air and O{sub 2} atmospheres was found to be qualitatively similar to that of HoMnO{sub 3}. Decomposition of hexagonal HoMnO{sub 3} by two different processes occurs in oxidizing atmosphere above {approx}1200 K followed by nucleation and growth of the perovskite polymorph of HoMnO{sub 3}. A rapid, reconstructive transition from the perovskite back to the hexagonal polymorph was observed in situ at 1623 K upon reduction of the partial pressure of oxygen. A phase stability diagram of the hexagonal and orthorhombic polymorphs is proposed. Finally, distinctly non-linear electrical conductivity was observed for both HoMnO{sub 3} and YMnO{sub 3} in oxidizing atmosphere between 555 and 630 K, and shown to be associated with excess oxygen. - Graphical abstract: Chemical expansion of hexagonal HoMnO{sub 3} is observed during HTXRD in different pO{sub 2}. Oxidizing atmosphere favors the competing perovskite polymorph. Electrical conductivity anomalies related to excess oxygen are found at 550-630 K. Highlights: Black-Right-Pointing-Pointer Thermal evolution of crystal structure of HoMnO{sub 3} studied up to 1623 K in air and N{sub 2}. Black-Right-Pointing-Pointer Anisotropic chemical expansion of HoMnO{sub 3} and YMnO{sub 3} in N{sub 2}, air and O{sub 2}. Black-Right-Pointing-Pointer Hexagonal phase destabilized with respect to perovskite in oxidizing atmosphere. Black-Right-Pointing-Pointer Crystal structure and phase stability discussed in terms of point defect chemistry. Black-Right-Pointing-Pointer Electrical conductivity anomalies associated with excess oxygen at 550-630 K.« less

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

Arutyunyan, S. S., E-mail: spartakmain@gmail.com; Pavlov, A. Yu.; Pavlov, B. Yu.

The fabrication of a two-layer Si{sub 3}N{sub 4}/SiO{sub 2} dielectric mask and features of its application in the technology of non-fired epitaxially grown ohmic contacts for high-power HEMTs on AlGaN/GaN heterostructures are described. The proposed Si{sub 3}N{sub 4}/SiO{sub 2} mask allows the selective epitaxial growth of heavily doped ohmic contacts by nitride molecular-beam epitaxy and the fabrication of non-fired ohmic contacts with a resistance of 0.15–0.2 Ω mm and a smooth surface and edge morphology.

Crystal structure of a new amine nitrate: 4-dimethylaminopyridinium nitrate (C{sub 7}H{sub 11}N{sub 2})NO{sub 3}

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

Benhassan, D., E-mail: houcine-naili@yahoo.com; Rekik, W.; Naïli, H.

2015-12-15

The title compound (C{sub 7}H{sub 11}N{sub 2})NO{sub 3} (I) was obtained by the slow evaporation method at room temperature. Its crystal structure consists of organic cations (C{sub 7}H{sub 11}N{sub 2}){sup +} and nitrate anions (NO{sub 3}){sup –} linked by two types of hydrogen bonds. Each monoprotonated nitrogen atom, called bifurcated, is engaged in two N–H···O hydrogen bonds with two symmetric oxygen atoms. In addition, the crystal structure stability is established by C–H···O hydrogen bonds that ensure the formation of infinite layers, parallel to (001) plane. These layers are related together through π···π interactions established between aromatic amines.

Langmuir Probe Measurements of Inductively Coupled Plasma in CF4/AR/O2 Mixtures

NASA Technical Reports Server (NTRS)

Rao, M. V. V. S.; Cruden, Brett; Sharma, Surendra; Meyyappan, Meyya

2001-01-01

Inductively coupled plasmas of CF4:Ar:O2, which have been of importance to material processing, were studied in the GEC cell at 80:10:10, 60:20:20, and 40:30:30 mixture ratios. Radial distributions of plasma potential (V(sub p)), electron and ion number densities (n(sub e) and n(sub i)), electron temperature (T(sub e)), and electron energy distribution functions (EEDFs) were measured in the mid-plane of plasma across the electrodes in the pressure range of 10-50 mTorr, and RF power of 200 and 300 W. V(sub p), n(sub e) and n(sub i), which peak in the center of the plasma, increase with decrease of pressure. T(sub e) also increases with pressure but peaks toward the electrode edge. Both V(sub p) and T(sub e) remain nearly independent of RF power, whereas n(sub e) and n(sub i) increase with power. In all conditions the EEDFs exhibit non-Maxwellian shape and are more like Druyvesteyn form at higher energies. They exhibit a broad lip in the energy range 0-10 eV suggesting an electron loss mechanism, which could be due to via resonance electron attachment processes producing negative ions in this rich electronegative gas mixture. This behavior is more prominent towards the electrode edge.

Langmuir Probe Measurements of Inductively Coupled Plasmas in CF4/Ar/O2 Mixtures

NASA Technical Reports Server (NTRS)

Rao, M. V. V. S.; Cruden, Brett; Sharma, Surendra; Meyyappan, Meyya

2001-01-01

Inductively coupled plasmas of CF4:Ar:O2, which have been of importance to material processing, were studied in the GEC cell at 80:10:10, 60:20:20, and 40:30:30 mixture ratios. Radial distributions of plasma potential (V(sub p)), electron and ion number densities (n(sub e) and n(sub i), electron temperature (T(sub e)), and electron energy distribution functions (EEDFs) were measured in the mid-plane of plasma across the electrodes in the pressure range of 10-50 mTorr, and RF (radio frequency) power of 200 and 300 W. V(sub p), n(sub e) and n(sub i), which peak in the center of the plasma, increase with decrease of pressure. T(sub e) also increases with pressure but peaks toward the electrode edge. Both V(sub p) and T(sub e) remain nearly independent of RF power, whereas n(sub e) and n(sub i) increase with power. In all conditions the EEDFs exhibit non-Maxwellian shape and are more like Druyvesteyn form at higher energies. They exhibit a broad dip in the energy range 0-10 eV suggesting an electron loss mechanism, which could be due to via resonance electron attachment processes producing negative ions in this rich electronegative gas mixture. This behavior is more prominent towards the electrode edge.

CHEMICAL PROCESSING OF PURE AMMONIA AND AMMONIA-WATER ICES INDUCED BY HEAVY IONS

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

Bordalo, V.; Da Silveira, E. F.; Lv, X. Y.

Cosmic rays are possibly the main agents to prevent the freeze-out of molecules onto grain surfaces in cold dense clouds. Ammonia (NH{sub 3}) is one of the most abundant molecules present in dust ice mantles, with a concentration of up to 15% relative to water (H{sub 2}O). FTIR spectroscopy is used to monitor pure NH{sub 3} and NH{sub 3}-H{sub 2}O ice samples as they are irradiated with Ni and Zn ion beams (500-600 MeV) at GANIL/France. New species, such as hydrazine (N{sub 2}H{sub 4}), diazene (N{sub 2}H{sub 2} isomers), molecular hydrogen (H{sub 2}), and nitrogen (N{sub 2}) were identified aftermore » irradiation of pure NH{sub 3} ices. Nitrous oxide (N{sub 2}O), nitrogen oxide (NO), nitrogen dioxide (NO{sub 2}), and hydroxylamine (NH{sub 2}OH) are some of the products of the NH{sub 3}-H{sub 2}O ice radiolysis. The spectral band at 6.85 {mu}m was observed after irradiation of both types of ice. Besides the likely contribution of ammonium (NH{sub 4}{sup +}) and amino (NH{sub 2}) radicals, data suggest a small contribution of NH{sub 2}OH to this band profile after high fluences of irradiation of NH{sub 3}-H{sub 2}O ices. The spectral shift of the NH{sub 3} ''umbrella'' mode (9.3 {mu}m) band is parameterized as a function of NH{sub 3}/H{sub 2}O ratio in amorphous ices. Ammonia and water destruction cross-sections are obtained, as well as the rate of NH{sub 3}-H{sub 2}O (1:10) ice compaction, measured by the OH dangling bond destruction cross-section. Ammonia destruction is enhanced in the presence of H{sub 2}O in the ice and a power law relationship between stopping power and NH{sub 3} destruction cross-section is verified. Such results may provide relevant information for the evolution of molecular species in dense molecular clouds.« less

IR Bandwidth and Crystal Thickness Effects on THG Efficiency and Temporal Shaping of Quasi-Rectangular UV Pulses: Part II - Incident IR Ripple

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

Bolton, Paul R.; Limborg-Deprey, Cecile; /SLAC

We have investigated the effect of incident ir spectral bandwidth and crystal thickness, on uv pulses produced by third harmonic generation (THG) in a crystal pair. Our focus is on the third harmonic generation efficiency and longitudinal uv intensity profile parameters of SNLO predictions that are evaluated for three incident ir spectral bandwidths and a range of crystal thicknesses. These results represent a continuation of earlier work in which the effects of the same selected ir bandwidths and range of crystal thicknesses were investigated using a pair of BBO Type I crystals in a simplistic geometry for which the longitudinalmore » intensity plateau has a zero slope, 'flattop' profile. The current work is distinguished from the previous work by an imposed ripple on the ir intensity longitudinal profile and constitutes a portion of a Part II effort to which we have made reference. As with preceding work, all third harmonic data are net results at the exit of the second BBO crystal. Predictions are obtained with the modified SNLO code developed by Arlee Smith at the Sandia National Laboratories. This modification has allowed us to pursue the 'coupled' case in which the output of the first BBO crystal is used as input to the second one. This includes both the fundamental and second harmonic light. Defined parameters are consistent with previous work. The presented cases are best results. The criteria for selection of these reported cases are highest THG efficiency combined with minimum intensity ripple in the plateau. The incident ir pulse is quasi-rectangular with an imposed 5.2 % (rms) intensity ripple added to the plateau. The ir pulse bandwidth is centered at 800 nm. Second harmonic generation occurs in the first BBO crystal and THG occurs in the second crystal as a consequence of sum frequency generation. Type I phase matching is used throughout, so that for a negative uniaxial crystal: n{sub 2}{sup e}({theta}) = n{sub 1}{sup o};(SHG) (1.1) 3n{sub 3}{sup 3}({theta}) = 2n{sub 2}{sup o} + n{sub 1}{sup o};(THG) where n{sub 2}{sup e}({theta}) and n{sub 3}{sup e}({theta}) are the angle dependent extraordinary refractive indices for the second and third harmonics respectively, and n{sub 1}{sup 1} and n{sub 2}{sup o} are the ordinary refractive indices for the fundamental and second harmonic respectively. Although our goal at this stage has not been to comply with all the LCLS injector laser specifications, the results provided here represent a parameter study that can be used to determine candidate bandwidth dependent, crystal thickness combinations for the detailed design of compliant THG subsystems. This simplistic geometry better elucidates acceptance bandwidth limitations that are intrinsic to the crystal material.« less

Advanced modeling of nitrogen oxide emissions in circulating fluidized bed combustors: Parametric study of coal combustion and nitrogen compound chemistries

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

Kilpinen, P.; Kallio, S.; Hupa, M.

1999-07-01

This paper describes work-in-progress aimed at developing an emission model for circulating fluidized bed combustors using detailed homogeneous and heterogeneous chemical kinetics. The main emphasis is on nitrogen oxides (NO{sub x}, N{sub 2}O) but also unburned gases (CO, C{sub x}H{sub y}) and sulfur dioxide (SO{sub 2}) will be investigated in the long run. The hydrodynamics is described by a 1.5-dimensional model where the riser is divided into three regions: a dense bubbling bed at the bottom, a vigorously mixed splash zone, and a transport zone. The two latter zones are horizontally split into a core region and an annular region.more » The solids circulation rate is calculated from the known solids inventory and the pressure and mass balances over the entire circulation loop. The solids are divided into classes according to size and type or particle. The model assumes instantaneous fuel devolatilization at the bottom and an even distribution of volatiles in the suspension phase of the dense bed. For addition of secondary air, a complete penetration and an instantaneous mixing with the combustor gases in the core region is assumed. The temperature distribution is assumed to be known, and no energy balance is solved. A comprehensive kinetic scheme of about 300 elementary gas-phase reactions is used to describe the homogeneous oxidation of the volatiles including both hydrocarbon and volatile-nitrogen components (NH{sub 3}, HCN). Heterogeneous char combustion to CO and CO{sub 2}, and char-nitrogen conversion to NO, N{sub 2}O, and N{sub 2} are described by a single particle model that includes 15 reaction steps given in the form of 6 net reaction paths. In the paper, the model is briefly described. A special emphasis is put on the evaluation of chemistry submodels. Modeling results on nitrogen oxides' formation are compared with measured concentration profiles in a 12 MW CFBC riser from literature. The importance of accurate chemistry description on predictions is illustrated by comparing modeling results using detailed kinetics to those obtained when hydrocarbon and volatile-nitrogen oxidation are described with empirical, global kinetic rate expressions from literature. Submodels that need further improvements are discussed.« less

Alkylation of a bioinspired high spin Ni(II)N{sub 3}S{sub 2} complex with bifunctional reagents

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

Chohan, B. S., E-mail: bsc12@psu.edu

2013-12-15

Crystal structures of two S-alkylated complexes generated from the reaction of iodoacetamide and iodoethanol with an air and moisture sensitive high spin Ni(II) pentacoordinate triaminodithiolate complex, 1 are determined by X-ray structure analysis. Crystals of complex 2, [NiC{sub 16}H{sub 31}N{sub 5}O{sub 2}S{sub 2}]I{sub 2}, are triclinic, sp. gr. P-bar1 , Z = 2. Crystals of complex 3, [NiC{sub 16}H{sub 28}N{sub 3}O{sub 2}S{sub 2}]I{sub 2}, are monoclinic, sp. gr. P2{sub 1}/c, Z = 4. Structures of complexes 2 and 3 are very similar: one of the S-acetamide (2) or S-ethanol (3) groups coordinates to the Ni center through the oxygen atom formingmore » N{sub 3}S{sub 2}O hexacoordination; the other group remains unbound to the Ni and left dangling. Crystal packing shows that complexes 2 and 3 interact with the iodide counterions, and that only complex 2 interact with neighboring molecules; some of these close intermolecular contacts include H-bonding interactions.« less

Near-infrared and ultraviolet induced isomerization of crotonic acid in N{sub 2} and Xe cryomatrices: First observation of two high-energy trans C–O conformers and mechanistic insights

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

Kuş, Nihal; Department of Physics, Anadolu University, 26470 Eskişehir; Fausto, Rui, E-mail: rfausto@ci.uc.pt

2014-12-21

E-crotonic acid was isolated in cryogenic solid N{sub 2} and xenon matrices, and subjected to Laser ultraviolet (UV) and near-infrared (NIR) irradiations. In the deposited matrices, the two low-energy cis C–O E-cc and E-ct conformers, which are the only forms significantly populated in the gas phase, were observed. UV irradiation (λ= 250 nm) of the compound in N{sub 2} matrix allows for experimental detection, not just of the two low-energy cis C–O isomers of Z-crotonic acid previously observed in the experiments carried out in argon matrix [Z-cc and Z-ct; R. Fausto, A. Kulbida, and O. Schrems, J. Chem. Soc., Faradaymore » Trans. 91, 3755–3770 (1995)] but also of the never observed before high-energy forms of both E- and Z-crotonic acids bearing the carboxylic acid group in the trans arrangement (E-tc and Z-tc conformers). In turn, NIR irradiation experiments in the N{sub 2} matrix allow to produce the high-energy E-tc trans C–O conformer in a selective way, from the initially deposited E-cc form. The vibrational signatures of all the 6 rotameric structures of the crotonic acids experimentally observed, including those of the new trans C–O forms, were determined and the individual spectra fully assigned, also with support of theoretically obtained data. On the other hand, as found before for the compound isolated in argon matrix, the experiments performed in xenon matrix failed to experimental detection of the trans C–O forms. This demonstrates that in noble gas matrices these forms are not stable long enough to allow for their observation by steady state spectroscopy techniques. In these matrices, the trans C–O forms convert spontaneously into their cis C–O counterparts, by tunnelling. Some mechanistic details of the studied processes were extracted and discussed.« less

Synthesis and physico-chemical studies on neodymium(III) and samarium(III) complexes with tetraaza macrocyclic ligands

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

Goel, S.; Pandey, U.K.; Pandey, O.P.

1988-05-01

Reactions of neodymium trichloride and samarium trichloride with 6,7,13,14-R/sub 4/ - 3,10-X/sub 2/-(14)-5,7,12,14-tetraene-1,5,8,12-N/sub 4/-(2,4,9,11-N/sub 4/) (R = CH/sub 3/, X = 0 (L/sub 1//sup (1)/); R = C/sub 6/H/sub 5/, X = O (L/sub 1//sup (2)/); R = CH/sub 3/, X = S(L/sub 2//sup (1)/)) and R = C/sub 6/H/sub 5/, X = S(/sub 2//sup (2)/)) have been studied in ethanol and complexes of the type (M(L/sub 1//sup (1)/ or L/sub 1//sup (2)/))Cl/sub 3/ and (M(L/sub 2//sup (1)/ or L/sub 2//sup (2)/)(H/sub 2/O)/sub 2/)Cl/sub 3/ (M = Nd(III) and Sm(III)) have been isolated. In addition, macrocyclic complexes of Nd(III) andmore » Sm(III) with another series of tetraaza ligands, viz, 5,6,11,12-R/sub 4/-3,8-X/sub 2/-(12)-4,6,10,12-tetraene-1,4,7,10-N/sub 4/-(2,9-N/sub 2/) (R = CH/sub 3/, X = O (L/sub 3//sup (1)/); R = C/sub 6/H/sub 5/, X = O(L/sub 3//sup (2)/); R = CH/sub 3/, X = S(L/sub 4//sup (1)/); R = C/sub 6/H/sub 5/, X = S(L/sub 4//sup (2)/)), formulated as (M(L/sub 3//sup (1)/, L/sub 3//sup (2)/, L/sub 4//sup (1)/ or L/sub 4//sup (2)/)(H/sub 2/O)/sub 2/)Cl/sub 3/ (M = Nd(III) and Sm(III)) have been prepared by template condensation of Nd(III) and Sm(III) complexes of diacetylbis(semicarbazonethiosemicarbazone) or benzilibis(semicarbazonethiosemicarbazone) with diacetyl or benzil. The complexes have been identified by elemental analysis, electrical conductance, spectral and thermal measurements.« less

CONSTRAINING THE MILKY WAY'S HOT GAS HALO WITH O VII AND O VIII EMISSION LINES

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

Miller, Matthew J.; Bregman, Joel N., E-mail: mjmil@umich.edu, E-mail: jbregman@umich.edu

2015-02-10

The Milky Way hosts a hot (≈2 × 10{sup 6} K), diffuse, gaseous halo based on detections of z = 0 O VII and O VIII absorption lines in quasar spectra and emission lines in blank-sky spectra. Here we improve constraints on the structure of the hot gas halo by fitting a radial model to a much larger sample of O VII and O VIII emission line measurements from XMM-Newton/EPIC-MOS spectra compared to previous studies (≈650 sightlines). We assume a modified β-model for the halo density distribution and a constant-density Local Bubble from which we calculate emission to compare withmore » the observations. We find an acceptable fit to the O VIII emission line observations with χ{sub red}{sup 2} (dof) = 1.08 (644) for best-fit parameters of n{sub o}r{sub c}{sup 3β}=1.35±0.24 cm{sup –3} kpc{sup 3β} and β = 0.50 ± 0.03 for the hot gas halo and negligible Local Bubble contribution. The O VII observations yield an unacceptable χ{sub red}{sup 2} (dof) = 4.69 (645) for similar best-fit parameters, which is likely due to temperature or density variations in the Local Bubble. The O VIII fitting results imply hot gas masses of M(<50 kpc) = 3.8{sub −0.3}{sup +0.3}×10{sup 9} M{sub ⊙} and M(<250 kpc) = 4.3{sub −0.8}{sup +0.9}×10{sup 10} M{sub ⊙}, accounting for ≲50% of the Milky Way's missing baryons. We also explore our results in the context of optical depth effects in the halo gas, the halo gas cooling properties, temperature and entropy gradients in the halo gas, and the gas metallicity distribution. The combination of absorption and emission line analyses implies a sub-solar gas metallicity that decreases with radius, but that also must be ≥0.3 Z {sub ☉} to be consistent with the pulsar dispersion measure toward the Large Magellanic Cloud.« less

Environmental assessment of an enhanced-oil-recovery steam generator equipped with a low-NOx burner. Volume 2. Data supplement. Final report, January 1984-January 1985

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

Castaldini, C.; Waterland, L.R.; Lips, H.I.

1986-02-01

The report is a compendium of detailed test sampling and analysis data obtained in field tests of an enhanced-oil-recovery steam generator (EOR steamer) equipped with a MHI PM low-NOx crude oil burner. Test data reported include equipment calibration records, steamer operating data, and complete flue-gas emission results. Flue-gas emission measurements included continuous monitoring for criteria pollutants; onsite gas chromatography (GC) for volatile hydrocarbons (Cl-C6); Methods 5/8 sampling for particulate and SO/sub 2/ and SO/sub 3/ emissions; source assessment sampling system (SASS) for total organics in two boiling-point ranges (100 to 300 C and greater than or equal to 300 C),more » organic compound category information using infrared spectrometry (IR), and specific quantitation of the semivolatile organic priority pollutants using gas chromatography/mass spectrometry (GC/MS); Andersen impactor train measurements of emitted particle-size distribution; and N/sub 2/O emissions by gas chromatography/electron-capture detector (GC/ECD).« less

Successful N{sub 2} leptogenesis with flavour coupling effects in realistic unified models

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

Bari, Pasquale Di; King, Stephen F., E-mail: P.Di-Bari@soton.ac.uk, E-mail: king@soton.ac.uk

2015-10-01

In realistic unified models involving so-called SO(10)-inspired patterns of Dirac and heavy right-handed (RH) neutrino masses, the lightest right-handed neutrino N{sub 1} is too light to yield successful thermal leptogenesis, barring highly fine tuned solutions, while the second heaviest right-handed neutrino N{sub 2} is typically in the correct mass range. We show that flavour coupling effects in the Boltzmann equations may be crucial to the success of such N{sub 2} dominated leptogenesis, by helping to ensure that the flavour asymmetries produced at the N{sub 2} scale survive N{sub 1} washout. To illustrate these effects we focus on N{sub 2} dominatedmore » leptogenesis in an existing model, the A to Z of flavour with Pati-Salam, where the neutrino Dirac mass matrix may be equal to an up-type quark mass matrix and has a particular constrained structure. The numerical results, supported by analytical insight, show that in order to achieve successful N{sub 2} leptogenesis, consistent with neutrino phenomenology, requires a ''flavour swap scenario'' together with a less hierarchical pattern of RH neutrino masses than naively expected, at the expense of some mild fine-tuning. In the considered A to Z model neutrino masses are predicted to be normal ordered, with an atmospheric neutrino mixing angle well into the second octant and the Dirac phase δ≅ 20{sup o}, a set of predictions that will be tested in the next years in neutrino oscillation experiments. Flavour coupling effects may be relevant for other SO(10)-inspired unified models where N{sub 2} leptogenesis is necessary.« less

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

Liu Huanxin; Liang Yunxiao; Jiang Xiao

A nonmetal pentaborate [C{sub 6}H{sub 13}N{sub 2}][B{sub 5}O{sub 6}(OH){sub 4}] (1) has been synthesized by 1,4-diazabicyclo[2.2.2] octane (DABCO) and boric acid, and characterized by single-crystal X-ray diffraction, FTIR, elemental analysis, and thermogravimetric analysis. Compound 1 crystallizes in the monoclinic system with space group Cc (no. 9), a=10.205(2) A, b=14.143(3) A, c=11.003(2) A, {beta}=113.97(3){sup o}, V=1451.1(5) A{sup 3}, Z=4. The anionic units, [B{sub 5}O{sub 6}(OH){sub 4}]{sup -}, are interlinked via hydrogen bonding to form a three-dimensional (3D) supramolecular network containing large channels, in which the protonated [C{sub 6}H{sub 13}N{sub 2}]{sup +} cations are located. Second-harmonic generation (SHG) measurements on the powdermore » samples reveal that 1 exhibits SHG efficiency approximately 0.9 times that of potassium dihydrogen phosphate (KDP). - Graphical abstract: The protonated [C{sub 6}H{sub 13}N{sub 2}]{sup +} cations and the polyanions [B{sub 5}O{sub 6}(OH){sub 4}]{sup -} form a 3D supramolecular network by extensive hydrogen bonds and electrostatic attraction. This compound shows NLO properties and the SHG efficiency is approximately 0.9 times that of KDP.« less

Oxidation of CO by N/sub 2/O between 1076 and 1228 K: determination of the rate constant of the exchange reaction

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

Loirat, H.; Caralp, F.; Destriau, M.

New measurements of the rate constant of the direct reaction of CO with N/sub 2/O are reported with the principal purpose of removing some of the remaining discrepancies on its value. Experiments were performed at lower temperatures (1076-1228 K) and lower pressure (approx. 15 Torr) than those prevailing in most of previous works, by using a static reactor. It is shown that, under these experimental conditions, the reaction proceeds essentially according to the direct reaction CO + N/sub 2/O ..-->.. CO/sub 2/ + N/sub 2/ (1). The previously proposed wet mechanism is not significant under our experimental conditions. It hasmore » to be taken into account, however, to describe the observed production and consumption of molecular oxygen. The Arrhenius expression derived from these experiments is k/sub 1/ = 10/sup 14.4 +/- 0.3 exp(-(46 +- 2) kcal mol/sup -1/RT) cm/sup 3/ mol/sup -1/ s/sup -1/. A detailed analysis of the results shows that the uncertainties in side reactions do not greatly influence the value of k/sub 1/. A critical discussion of the data reported in the literature is presented. In spite of remaining uncertainties in the reaction mechanism, the present results, obtained in a low-temperature range, show that the low activation energy values of reaction 1, reported in several works performed at higher temperatures, are highly unlikely« less

HERSCHEL/SPIRE SUBMILLIMETER SPECTRA OF LOCAL ACTIVE GALAXIES {sup ,}

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

Pereira-Santaella, Miguel; Spinoglio, Luigi; Busquet, Gemma

2013-05-01

We present the submillimeter spectra from 450 to 1550 GHz of 11 nearby active galaxies observed with the SPIRE Fourier Transform Spectrometer (SPIRE/FTS) on board Herschel. We detect CO transitions from J{sub up} = 4 to 12, as well as the two [C I] fine structure lines at 492 and 809 GHz and the [N II]1461 GHz line. We used radiative transfer models to analyze the observed CO spectral line energy distributions. The FTS CO data were complemented with ground-based observations of the low-J CO lines. We found that the warm molecular gas traced by the mid-J CO transitions hasmore » similar physical conditions (n{sub H{sub 2}}{approx} 10{sup 3.2}-10{sup 3.9} cm{sup -3} and T{sub kin} {approx} 300-800 K) in most of our galaxies. Furthermore, we found that this warm gas is likely producing the mid-IR rotational H{sub 2} emission. We could not determine the specific heating mechanism of the warm gas, however, it is possibly related to the star formation activity in these galaxies. Our modeling of the [C I] emission suggests that it is produced in cold (T{sub kin} < 30 K) and dense (n{sub H{sub 2}}>10{sup 3} cm{sup -3}) molecular gas. Transitions of other molecules are often detected in our SPIRE/FTS spectra. The HF J = 1-0 transition at 1232 GHz is detected in absorption in UGC 05101 and in emission in NGC 7130. In the latter, near-infrared pumping, chemical pumping, or collisional excitation with electrons are plausible excitation mechanisms likely related to the active galactic nucleus of this galaxy. In some galaxies, few H{sub 2}O emission lines are present. Additionally, three OH{sup +} lines at 909, 971, and 1033 GHz are identified in NGC 7130.« less

Anchoring of Cu(II) onto surface of porous metal-organic framework through post-synthesis modification for the synthesis of benzimidazoles and benzothiazoles

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

Kardanpour, Reihaneh; Tangestaninejad, Shahram, E-mail: stanges@sci.ui.ac.ir; Mirkhani, Valiollah, E-mail: mirkhani@sci.ui.ac.ir

2016-03-15

Efficient synthesis of various benzimidazoles and benzothiazoles under mild conditions catalyzed by Cu(II) anchored onto UiO-66–NH{sub 2} metal organic framework is reported. In this manner, first, the aminated UiO-66 was modified with thiophene-2-carbaldehyde and then the prepared Schiff base was reacted with CuCl{sub 2}. The prepared catalyst was characterized by FT-IR, UV–vis, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), N{sub 2} adsorption, inductively coupled plasma atomic emission spectroscopy (ICP-AES) and field emission scanning electron microscopy (FE-SEM). The UiO-66–NH{sub 2}–TC–Cu was applied as a highly efficient catalyst for synthesis of benzimidazole and benzothiazole derivatives by the reaction of aldehydes with 1,2-diaminobenzenemore » or 2-aminothiophenol. The Cu(II)-containing MOF was reused several times without any appreciable loss of its efficiency. - Graphical abstract: Efficient synthesis of benzimidazoles and benzothiazoles catalyzed by Cu(II) anchored onto UiO-66–NH{sub 2} metal organic framework is reported. - Highlights: • A copper Schiff base was immobilized on UiO-66 via postsynthetic modification. • The modified MOFs were fully characterized by a variety of methods. • The catalyst was used for the preparation of benzimidazoles and benzothiazoles. • In comparison of other catalysts, our catalyst was more efficient and forceful.« less

Preparation and characterization of CNT-CeO{sub 2} nanocomposite

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

Kaur, Jasmeet, E-mail: jasmeet.dayal@gmail.com; Anand, Kanika; Singh, Ravi Chand

2015-06-24

This paper reports decoration of CeO{sub 2} nanoparticles on multi-walled carbon nanotubes through a reflux process in which Ce (NO{sub 3}) {sub 3}·6H{sub 2}O serves as precursor and hydrazine hydrate (N{sub 2}H{sub 4}.H{sub 2}O) as reducing agent. Successful deposition of cubic fluorite CeO{sub 2} nanoparticles onto multi-walled carbon nanotubes has been confirmed by x-ray diffraction (XRD), Raman spectroscopy, field-emission scanning electron microscopy (FE-SEM) and energy dispersive x-ray spectroscopy (EDS). It was found that CeO{sub 2} nanoparticles formed in the presence of CNTs were larger as compared to pure CeO{sub 2} nanoparticles. Raman analysis showed that CeO{sub 2} induced a decreasemore » in the size of the carbon grain in the CNTs. A red shift from 460 cm{sup −1} to 463 cm{sup −1} for F{sub 2g} mode of CeO{sub 2} has also been observed in Raman spectra of CNT- CeO{sub 2} nanocomposite as compared to pure CeO{sub 2}. The CeO{sub 2} coated multi-wall carbon nanotubes (CNT-CeO{sub 2}) nanocomposite would be a promising candidate for practical applications such as catalysis, sensing and power source applications.« less

Hg-sensitized photolysis of diethylamine in the absence and presence of O/sub 2/ or N/sub 2/O

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

DeStefano, G.; Heicklen, J.

1986-09-11

The Hg-sensitized photolysis of diethylamine (DEA) was studied in the absence and presence of O/sub 2/ or N/sub 2/O at room temperature. In the absence of foreign gases, the products were H/sub 2/, CH/sub 3/CH=NC/sub 2/H/sub 5/ and N,N'-diethylbutane-2,3-diamine (III), with respective quantum yields of 1.0, 1.0, and similarly ordered 0.02. Thus CH/sub 3/CHNHC/sub 2/H/sub 5/ radicals are produced exclusively and they are removed by self reaction: 2CH/sub 3/CHNHC/sub 2/H/sub 5/ ..-->.. DEA + CH/sub 3/CH=NC/sub 2/H/sub 5/ (4a) and 2CH/sub 3/CHNHC/sub 2/H/sub 5/ ..-->.. diamine III (4b), with k/sub 4a//k/sub 4b/ = 47.0 +/- 5.6. In the presence ofmore » O/sub 2/ the radicals are scavenged exclusively by abstraction of the H atom on the nitrogen to give the imine CH/sub 3/CH=NC/sub 2/H/sub 5/ as the exclusive product: (CH/sub 3/CHNHC/sub 2/H/sub 5/ + O/sub 2/ ..-->.. CH/sub 3/CH=NC/sub 2/H/sub 5/ + HO/sub 2/ (5). The Hg-sensitized photolysis of N/sub 2/O gives O(/sup 3/P) atoms, which in the presence of DEA react to give the imine and (C/sub 2/H/sub 5/)/sub 2/NOH (DEHA) as products in concerted parallel steps: O(/sup 3/P) + (C/sub 2/H/sub 5/)/sub 2/NH ..-->.. CH/sub 3/CH=NC/sub 2/H/sub 5/ + H/sub 2/O (9a) and O(/sup 3/P) + (C/sub 2/H/sub 5/)/sub 2/NH ..-->.. (C/sub 2/H/sub 5/)/sub 2/NOH (9b), with k/sub 9a//k/sub 9b/ similarly ordered 9.5 +/- 1.7.« less

Spectral survey of helium lines in a linear plasma device for use in HELIOS imaging

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

Ray, H. B., E-mail: rayhb@ornl.gov; Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831; Biewer, T. M.

2016-11-15

Fast visible cameras and a filterscope are used to examine the visible light emission from Oak Ridge National Laboratory’s Proto-MPEX. The filterscope has been configured to perform helium line ratio measurements using emission lines at 667.9, 728.1, and 706.5 nm. The measured lines should be mathematically inverted and the ratios compared to a collisional radiative model (CRM) to determine T{sub e} and n{sub e}. Increasing the number of measurement chords through the plasma improves the inversion calculation and subsequent T{sub e} and n{sub e} localization. For the filterscope, one spatial chord measurement requires three photomultiplier tubes (PMTs) connected to pelliclemore » beam splitters. Multiple, fast visible cameras with narrowband filters are an alternate technique for performing these measurements with superior spatial resolution. Each camera contains millions of pixels; each pixel is analogous to one filterscope PMT. The data can then be inverted and the ratios compared to the CRM to determine 2-dimensional “images” of T{sub e} and n{sub e} in the plasma. An assessment is made in this paper of the candidate He I emission lines for an imaging technique.« less

Dispersion of Co/CNTs via strong electrostatic adsorption method: Thermal treatment effect

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

Akbarzadeh, Omid, E-mail: omid.akbarzadeh63@gmail.com; Abdullah, Bawadi, E-mail: bawadi-abdullah@petronas.com.my; Subbarao, Duvvuri, E-mail: duvvuri-subbarao@petronas.com.my

The effect of different thermal treatment temperature on the structure of multi-walled carbon nanotubes (MWCNTs) and Co particle dispersion on CNTs support is studied using Strong electrostatic adsorption (SEA) method. The samples tested by N{sub 2}-adsorption, field emission scanning electron microscopy (FE-SEM) and transmission electron microscopy (TEM). N{sub 2}-adsorption results showed BET surface area increased using thermal treatment and TEM images showed that increasing the thermal treatment temperature lead to flaky CNTs and defects introduced on the outer surface and Co particle dispersion increased.

Estimation of GHG emissions in Egypt up to the year 2020

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

ElMahgary, Y.; Abdel-Fattah, A.I.; Shama, M.A.

1994-09-01

Within the frame of UNEP's project on the Methodologies of Determining the Costs of Abatement of GHG Emissions, a case study on Egypt was undertaken by VTT (Technical Research Centre of Finland) in cooperation with the Egyptian Environment Authority Agency (EEAA). Both the bottom-up or engineering models and the top-down or the macroeconomic models were used. In the bottom-up approach, the economic sectors were divided into seven groups: petroleum industry, power generation, heavy industry, light industry, residential and commercial sector, transport and agriculture and domestic wastes. First, a comprehensive inventory for the year 1990 was prepared for all the GHGmore » emissions mainly, but not exclusively, from energy sources. This included CO[sub 2], CH[sub 4] and N[sub 2]O. A base scenario of economic and energy growth of Egypt for business-as-usual alternative was fixed using the results of several optimization processes undertaken earlier by the National Committee of Egypt. GHG emissions of the different sources in this base scenario were then determined using LEAP model and spread sheets.« less

Single-coal-particle combustion in O{sub 2}/N{sub 2} and O{sub 2}/CO{sub 2} environments

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

Bejarano, Paula A.; Levendis, Yiannis A.

A fundamental investigation has been conducted on the combustion of single particles of a bituminous coal (45-53, 75-90, and 150-180 {mu}m), of a lignite coal (45-53 and 75-90 {mu}m), and of spherical and monodisperse synthetic chars (43 {mu}m) at increasing O{sub 2} mole fractions in either N{sub 2} or CO{sub 2} balance gases. The synthetic particles were used to facilitate the observation of combustion phenomena with minimum distractions from particle-to-particle variabilities. The laboratory setup consisted of a drop-tube furnace operated at temperatures of 1400 and 1600 K. A calibrated three-color pyrometer, interfaced with the furnace, recorded luminous particle temperature-time profiles.more » Experimental results revealed that coal particles burned at higher mean temperatures and shorter combustion times in O{sub 2}/N{sub 2} than in O{sub 2}/CO{sub 2} environments at analogous oxygen mole fractions. In the case of the bituminous coal used herein and for the experimental combustion conditions tested, measured volatile and char temperatures as in air (21% O{sub 2}) were attained with an oxygen content in the CO{sub 2} mixtures in the neighborhood of 30%. Bituminous coal volatile and char burnout times comparable to those in air (21% O{sub 2}) were attained with oxygen content in the CO{sub 2} mixtures in the range of 30-35%. In the case of the lignite coal burned, the corresponding differences in oxygen mole fractions, which result in similar particle temperatures and burnout times in the two different gas mixtures, were less pronounced. (author)« less

Note on the Occurrence of Thorite at Alter Pedroso (Portugal). Report No. 29; NOTA SOBRE UMA OCORRENCIA DE TORITE EM ALTER PEDROSO. Memoria No. 29

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

Pacheco, J.T.; Gomes, R.A.D.

1960-01-01

The first known occurrence of thorite in Portugal is reported. The mineral was found as small dark reddishbrown euhedral grains scattered in a soil sample from the hyper-alkaline syerdte region of Alter Pedroso, in prospecting for radioactive materials. Zircon, riebeckite, aegirine, feldspar, biotite, magnetite (all of these common minerals of the hyper-alkaline syenite), and a few other urddentified minerals were found in the soil associated with thorite. This suggests the weathering of a local pegmatitic differentiation of the syenite as the origin of the thorite. Microscopic examination shows the mineral to be only partially metumict, and it is probably alteredmore » to a variable degree. Euhedral grains are constituted by several nearly colorless anisotropic nuclei (n/sub p/ near 1.69, n/sub g/ near 1.71, and sometimes anomalous B+ with variable 2V averaging 10/sup 0/) surrounded by a golden-brown isotropic material (n about 1.67). Specific gravity determinations were somewhat impaired by zircon inclusions and led to a value of 4.79. The chemical composition was determined by emission and x-ray fluorescence spectrography and shows a high yttrium content. A partial semiquantitative analysis gave the following results: ThO/sub 2/ (58.0%), SiO/sub 2/ (14.5%), Fe/sub 2/O/sub 3/ (2.5%), Y/sub 2/O/sub / 3>i (2.5%), CaO (l.1%), U/sub 3/O/sub 8/ (0.5%), and PbO (0.2%). The elements Be, Mg, Al, Mn, and P were also detected. X-raypowder patterns obtained before and after heating the sample to 1000 ts C for 1 hr in air confirmed the mineral to be only slightly metamict and showed that the tetragonal phase still prevails above 950 ts C. Calculations based on these patterns led to a tetragonal unit cell with a/sub 0/ = 7.05 0.01 A, c/sub 0/ = 6.27 0.01 A, and c/sub 0//a/sub 0/ = 0.889. (auth).« less

Large N{sub c}, constituent quarks, and N, {Delta} charge radii

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

Buchmann, Alfons J.; Lebed, Richard F.

2000-11-01

We show how one may define baryon constituent quarks in a rigorous manner, given physical assumptions that hold in the large-N{sub c} limit of QCD. This constituent picture gives rise to an operator expansion that has been used to study large-N{sub c} baryon observables; here we apply it to the case of charge radii of the N and {Delta} states, using minimal dynamical assumptions. For example, one finds the relation r{sub p}{sup 2}-r{sub {Delta}{sup +}}{sup 2}=r{sub n}{sup 2}-r{sub {Delta}{sup 0}}{sup 2} to be broken only by three-body, O(1/N{sub c}{sup 2}) effects for any N{sub c}.

Electronic emission spectrum of methylnitrene

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

Carrick, P.G.; Engelking, P.C.

The A /sup 3/E--X /sup 3/A/sub 2/ultraviolet emission spectrum of methylnitrene (CH/sub 3/N) was obtained in two ways: (1) by reacting methylazide (CH/sub 3/N/sub 3/) with metastable N/sub 2/ in a flowing afterglow; and (2) by discharging a mixture of methylazide (CH/sub 3/N/sub 3/) and helium in a corona excited supersonic expansion (CESE). The origin appears at T/sub 0/ = 31 811 cm/sup -1/. Several vibrational progressions were observed leading to the determination of a number of vibrational frequencies: v/sup double-prime//sub 1/ = 2938 , v/sup X//sub 2/ = 1350, v/sup double-prime//sub 3/ = 1039, v/sup X//sub 4/ = 3065,more » and v/sup double-prime//sub 6/ = 902 cm/sup -1/. Deuterium substitution confirmed the assignments of the vibrational frequencies. The X /sup 3/A/sub 2/ state is a normal, bound local minimum on the triplet electronic potential surface, and the upper A /sup 3/E state is able to support at least one quantum of vibration, assigned to v/sup //sub 3/, predominantly a C--N stretch. A comparison of flowing afterglow hollow cathode discharge sources and corona excited supersonic expansion sources shows the advantage of the CESE method of radical production for spectroscopy.« less

Conformational stability and force field of short-chain linear chlorophosphazenes: MNDO calculations, {sup 31}P NMR, vibrational spectra, and normal coordinate analyses of Cl{sub 3}PN(PCl{sub 2}N){sub n}P(O)Cl{sub 2} and [Cl{sub 3}PN(PCl{sub 2}N){sub n}PCl{sub 3}][PCl{sub 6}] (n = 1,2)

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

Bougeard, D.; Bremard, C.; De Jaeger, R.

1992-10-29

The Raman spectra of Cl{sub 3}PN(PCl{sub 2}N){pi}P(O)Cl{sub 2} and [Cl{sub 3}PN(PCl{sub 2}N){pi}PCl{sub 3}]{sup +}PCl{sub 6}{sup {minus}} (n = 1,2) were recorded in the solid and liquid states at different temperatures. The qualitative depolarization ratios were obtained in the liquid phase. A {sup 31}P NMR study for the molecular compounds showed a coalescence phenomenon near 220 K. The potential energy around the PN bonds for the Cl{sub 3}PN(PCl{sub 2}N)P(O)Cl{sub 2} molecule and [Cl{sub 3}PN(PCl{sub 2}N){sub 2}PCl{sub 3}]{sup +} cation are derived from MNDO (modified neglect of diatomic overlap) calculations. The stable conformations are found to be trans-cis for Cl{sub 3}PN(PCl{sub 2}N)P(O)Cl{submore » 2} and [Cl{sub 3}PN(PCl{sub 2}N){sub 2}PCl{sub 3}]{sup +}. The calculated structural parameters agree well with the X-ray experimental data. The frequencies obtained by normal coordinate analysis are in good agreement with the observed ones. The MNDO calculation of the harmonic force field is in reasonable agreement with the experimental values. The force constant values assigned to torsional modes around the PN bonds correspond to low barriers for the internal rotations. The easy internal rotation around the P-N and P{double_bond}N bonds can explain the flexibility of the phosphazene backbone and the elastomeric properties of the phosphazene polymers. 46 refs., 6 figs., 3 tabs.« less

Plasma treatment effect on charge carrier concentrations and surface traps in a-InGaZnO thin-film transistors

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

Kim, Jae-Sung; Xing Piao, Ming; Jang, Ho-Kyun

2014-03-21

Various plasma treatment effects such as oxygen (O{sub 2}), nitrogen (N{sub 2}), and argon (Ar) on amorphous indium gallium zinc oxide thin-film transistors (a-IGZO TFTs) are investigated. To study oxygen stoichiometry in a-IGZO TFTs with respect to various plasma environments, X-ray photoelectron spectroscopy was employed. The results showed that oxygen vacancies were reduced by O{sub 2} and N{sub 2} plasmas while they were increased after Ar plasma treatment. Additionally, the effects of plasma treatment on trap distribution in bulk and surface channels were explored by means of low-frequency noise analysis. Details of the mechanisms used for generating and restoring trapsmore » on the surface and bulk channel are presented.« less

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

Morrill, J.S.; Benesch, W.M.

Previous model results have shown that the N{sub 2} triplet vibrational level populations in the aurora are strongly affected by cascade and quenching by atomic and molecular oxygen. As the aurora penetrates to lower altitudes (less than 100 km) the role of quenching by atomic oxygen becomes less important and processes involving N{sub 2} collisions begin to play a more prominent part. The authors are developing a model which will yield steady state vibrational level populations for both the singlet and triplet valence states of N{sub 2}. The model currently provides results for the seven low-lying N{sub 2} triplet statesmore » (A {sup 3}{Sigma}{sub u}{sup +}, B {sup 3}{Pi}{sub g}, W {sup 3}{Delta}{sub u}, B{prime}{sup 3}{Sigma}{sub u}, C{sup 3}{Pi}{sub u}, D{sup 3}{Sigma}{sub u}{sup +}, and E{sup 3}{Sigma}{sub g}{sup +}). These states are responsible for auroral emissions from the UV (Vegard-Kaplan (VK), second positive (2PG)) through the visible to the infrared (first positive (1PG), infrared afterglow (IRA), Wu-Benesch (WB)). The authors have included two additional collisional processes in the current model which were not treated previously. These are the intersystem collisional transfer of excitation (ICT) between the B state and the A, W, and B{prime} states and vibrational redistribution within the A state vibrational manifold, both due to collisions with ground state N{sub 2}. The present work compares the current model results with those of a previous model as well as ground, airborne, and rocket observations. The comparison between N{sub 2}(A) (VK) and N{sub 2}(B) (1PG) vibrational level populations predicted by this model and a number of auroral observations indicate that the current model achieves a significant improvement in the fit between calculation and observation. 81 refs., 12 figs., 2 tabs.« less

The role of support morphology on the performance of Cu/ZnO-catalyst for hydrogenation of CO{sub 2} to methanol

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

Tasfy, Sara Faiz Hanna, E-mail: miss25208@gmail.com; Zabidi, Noor Asmawati Mohd, E-mail: noorasmawati-mzabidi@petronas.com.my; Shaharun, Maizatul Shima, E-mail: maizats@petronas.com.my

The effects of SBA-15 support morphology on the activity of Cu/ZnO catalyst in the hydrogenation of CO{sub 2} to methanol was investigated. In the hydrogenation of CO{sub 2} to methanol at 210°C, 2.25 MPa, H{sub 2}/CO{sub 2} ratio of three remarkable difference was obtained using Cu/ZnO catalyst supported on SBA-15 with different morphology. The catalysts were characterized using N{sub 2}-adsorption, field emission scanning microscopy (FESEM/EDX), transmission electron microscopy (HRTEM), and temperature-programmed reduction (TPR). Characterization of the catalyst showed that support morphology, surface area, metals dispersion, and reducibility influenced the catalytic performance. On the fiber-shaped SBA-15, copper dispersion was 29 % whereasmore » on the spherical-shaped SBA-15, the dispersion was 20 %. The experimental results showed that the catalyst supported over fiber-shaped SBA-15 exhibit higher CO{sub 2} conversion (13.96 %) and methanol selectivity (91.32 %) compare to catalyst supported over spherical-shaped SBA-15.« less

Cold atmospheric plasma jet in an axial DC electric field

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

Lin, Li, E-mail: lilin@gwu.edu, E-mail: keidar@gwu.edu; Keidar, Michael, E-mail: lilin@gwu.edu, E-mail: keidar@gwu.edu

2016-08-15

Cold atmospheric plasma (CAP) jet is currently intensively investigated as a tool for new and potentially transformative cancer treatment modality. However, there are still many unknowns about the jet behavior that requires attention. In this paper, a helium CAP jet is tested in an electrostatic field generated by a copper ring. Using Rayleigh microwave scattering method, some delays of the electron density peaks for different ring potentials are observed. Meanwhile, a similar phenomenon associated with the bullet velocity is found. Chemical species distribution along the jet is analyzed based on the jet optical emission spectra. The spectra indicate that amore » lower ring potential, i.e., lower DC background electric field, can increase the amount of excited N{sub 2}, N{sub 2}{sup +}, He, and O in the region before the ring, but can decrease the amount of excited NO and HO almost along the entire jet. Combining all the results above, we discovered that an extra DC potential mainly affects the temporal plasma jet properties. Also, it is possible to manipulate the chemical compositions of the jet using a ring with certain electric potentials.« less

Concentrations of methoxyflurane and nitrous oxide in veterinary operating rooms

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

Ward, G.S.; Byland, R.R.

1982-02-01

The surgical rooms of 14 private veterinary practices were monitored to determined methoxyflurane (MOF) concentrations during surgical procedure under routine working conditions. The average room volume for these 14 rooms was 29 m3. The average MOF value for all rooms was 2.3 ppm, with a range of 0.7 to 7.4 ppm. Four of the 14 rooms exceeded the maximum recommended concentration of 2 ppm. Six rooms which had 6 or more air changes/hr averaged 1.1 ppm, whereas 8 rooms with less than 6 measurable air changes/hr averaged 3.2 ppm. Operating rooms that had oxygen flows of more than 1,000 cm3/minmore » averaged 4.4 ppm, whereas those with flows of less than 1,000 cm3/min averaged 1.5 ppm. The average time spent during a surgical procedure using MOF, for all 14 facilities, was 2 hours. Nitrous oxide (N/sub 2/O) concentrations were determined in 4 veterinary surgical rooms. The average N/sub 2/O concentration for 3 rooms without waste anesthetic gas scavenging was 138 ppm. Concentration of N/sub 2/O in the waste anesthetic gas-scavenged surgical room was 14 ppm, which was below the maximum recommended concentration of 25 ppm.« less

Estimation of Hamaker constants of ceramic materials from optical data using Lifshitz theory

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

Bergstroem, L.; Meurk, A.; Rowcliffe, D.J.

1996-02-01

The Hamaker constants of eight different ceramic materials, 6H-SiC, tetragonal, partially stabilized ZrO{sub 2} (3% Y{sub 2}O{sub 3}), {beta}-Si{sub 3}N{sub 4}, {alpha}-Al{sub 2}O{sub 3}, Y{sub 2}O{sub 3}, sapphire (single-crystal {alpha}-Al{sub 2}O{sub 3}), MgO, MgAl{sub 2}O{sub 4}, and fused silica, across air, water, and n-dodecane at room temperature and across silica at 2,000 K have been calculated from optical data using the Lifshitz theory. Spectroscopic ellipsometry was used to measure the photon energy dependence of the refractive index, n, and the extinction coefficient, k, in the visible and near-UV range on several important ceramic materials. This relatively simple, nondestructive technique hasmore » proved to yield reliable optical data on sintered, polycrystalline materials such as Si{sub 3}N{sub 4}, SiC, ZrO{sub 2}, Al{sub 2}O{sub 3}, and ZnO. For the other materials, Y{sub 2}O{sub 3}, sapphire, MgO, MgAl{sub 2}O{sub 4}, and fused silica, optical data from the literature were used to calculate the Hamaker constants. The calculated Hamaker constants were estimated to be accurate within {+-} 10%.« less

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

Rugheimer, S.; Kaltenegger, L.; Segura, A.

We model the atmospheres and spectra of Earth-like planets orbiting the entire grid of M dwarfs for active and inactive stellar models with T{sub eff} = 2300 K to T{sub eff} = 3800 K and for six observed MUSCLES M dwarfs with UV radiation data. We set the Earth-like planets at the 1 AU equivalent distance and show spectra from the visible to IR (0.4–20 μm) to compare detectability of features in different wavelength ranges with the James Webb Space Telescope and other future ground- and spaced-based missions to characterize exo-Earths. We focus on the effect of UV activity levels onmore » detectable atmospheric features that indicate habitability on Earth, namely, H{sub 2}O, O{sub 3}, CH{sub 4}, N{sub 2}O, and CH{sub 3}Cl. To observe signatures of life—O{sub 2}/O{sub 3} in combination with reducing species like CH{sub 4}—we find that early and active M dwarfs are the best targets of the M star grid for future telescopes. The O{sub 2} spectral feature at 0.76 μm is increasingly difficult to detect in reflected light of later M dwarfs owing to low stellar flux in that wavelength region. N{sub 2}O, another biosignature detectable in the IR, builds up to observable concentrations in our planetary models around M dwarfs with low UV flux. CH{sub 3}Cl could become detectable, depending on the depth of the overlapping N{sub 2}O feature. We present a spectral database of Earth-like planets around cool stars for directly imaged planets as a framework for interpreting future light curves, direct imaging, and secondary eclipse measurements of the atmospheres of terrestrial planets in the habitable zone to design and assess future telescope capabilities.« less

Reference electrode for strong oxidizing acid solutions

DOEpatents

Rigdon, Lester P.; Harrar, Jackson E.; Bullock, Sr., Jack C.; McGuire, Raymond R.

1990-01-01

A reference electrode for the measurement of the oxidation-reduction potentials of solutions is especially suitable for oxidizing solutions such as highly concentrated and fuming nitric acids, the solutions of nitrogen oxides, N.sub.2 O.sub.4 and N.sub.2 O.sub.5, in nitric acids. The reference electrode is fabricated of entirely inert materials, has a half cell of Pt/Ce(IV)/Ce(III)/70 wt. % HNO.sub.3, and includes a double-junction design with an intermediate solution of 70 wt. % HNO.sub.3. The liquid junctions are made from Corning No. 7930 glass for low resistance and negligible solution leakage.

Method and apparatus for synthesizing anhydrous HNO.sub.3

DOEpatents

Coon, Clifford L.; Harrar, Jackson E.; Pearson, Richard K.; McGuire, Raymond R.

1984-01-01

A method and apparatus for electrochemically synthesizing anhydrous HNO.sub.3 from an aqueous solution of HNO.sub.3 includes oxidizing a solution of N.sub.2 O.sub.4 /aqueous HNO.sub.3 at an anode, while maintaining a controlled potential between the N.sub.2 O.sub.4 /aqueous HNO.sub.3 solution and the anode. A potential of about 1.80V vs. SCE is preferred. Anhydrous or aqueous HNO.sub.3 may be disposed at the cathode within the electrochemical cell. Aqueous HNO.sub.3 having a water content of up to about 12% by weight is utilized to synthesize anhydrous HNO.sub.3.

Method and apparatus for synthesizing anhydrous HNO/sub 3/. [Patent application

DOEpatents

Coon, C.L.; Harrar, J.E.; Pearson, R.K.; McGuire, R.R.

1982-07-20

A method and apparatus for electrochemically synthesizing anhydrous HNO/sub 3/ from an aqueous solution of HNO/sub 3/- includes oxidizing a solution of N/sub 2/O/sub 4//aqueous HNO/sub 3/ at an anode, while maintaining a controlled potential between the N/sub 2/O/sub 4//aqueous HNO/sub 3/ solution and the anode. A potential of about 1.80V vs. SCE is preferred. Anhydrous or aqueous HNO/sub 3/ may be disposed at the cathode within the electrochemical cell. Aqueous HNO/sub 3/ having a water content of up to about 12% by weight is utilized to synthesize anhydrous HNO/sub 3/.

On the reactivity of methylbenzenes

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

Silva, Gabriel da; Bozzelli, Joseph W.

2010-11-15

Alkylated aromatic hydrocarbons, including the methylbenzenes, are a major and growing component of liquid transportation fuels. Reactivity (or lack thereof) for the methylbenzenes in combustion systems, measured by octane rating, ignition delay, and laminar flame speed, varies widely with the number and position of methyl substituents. At present this behaviour is not fully understood. This study demonstrates how the low temperature and ignition reactivity of methylbenzenes is controlled by the presence of isolated methyl groups and adjacent methyl pairs (the ortho effect); this allows for the development of octane number correlations. Introduction of an isolated methyl group, adjacent only tomore » CH ring sites, consistently increases the research octane number (RON) by around 26. This phenomenon is explained by the formation of relatively unreactive benzyl free radicals. When an adjacent pair of methyl substituents is present the RON consistently decreases by between 8 and 26, compared to the case when these methyl groups are isolated from each other (this effect generally diminishes with increasing degree of substitution). Research octane numbers for all aromatics with zero to three methyl substituents are accurately described by the empirical relationship RON = 98 + 24.2n{sub m} - 25.8n{sub p}, where n{sub m} is the total number of methyl groups and n{sub p} is the number of contiguous adjacent methyl pairs. The ortho effect is attributed to the unique oxidation chemistry of o-methylbenzyl, o-methylbenzoxyl, and o-methylphenyl type radicals here we provide a preliminary exploration of this chemistry and highlight areas requiring further research. It is shown that the o-methylbenzyl radical can react with two oxygen molecules to form 1,2-diformylbenzene + 2OH + H, a highly chain-branching process. This chemistry is expected to largely explain the two-stage ignition and negative temperature coefficient (NTC) behavior witnessed for polymethylbenzenes with adjacent methyl pairs. Similar chain branching mechanisms exist in the oxidation of o-methylbenzoxyl radicals that also form during o-xylene ignition. (author)« less

Role of acetate and nitrates in the selective catalytic reduction of NO by propene over alumina catalyst as investigated by FTIR

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

Shimizu, Kenichi; Kawabata, Hisaya; Satsuma, Atsushi

1999-06-24

It is widely accepted that selective catalytic reduction (SCR) of NO by hydrocarbons is a potential method to remove NO{sub x} practically in excess O{sub 2}. Although many studies on SCR are related to zeolitic catalysts, metal oxides are also of importance as promising SCR catalysts due to their high durability. Among oxide catalysts, {gamma}-Al{sub 2}O{sub 3} is one of the most active single oxides for SCR. The mechanism of the selective catalytic reduction (SCR) of NO by C{sub 3}H{sub 6} on Al{sub 2}O{sub 3} was investigated using in situ IR spectroscopy. Attention was focused on the reactivity of themore » adsorbed acetate and nitrates on the Al{sub 2}O{sub 3} surface. IR spectra showed that the reaction starts with the nitrates formation from NO + O{sub 2} followed by its reaction with C{sub 3}H{sub 6} to form acetate, which becomes the predominant surface species in the steady-state condition. The acetate band, which was stable in He or NO, significantly decreased when the flowing gas was switched to NO + O{sub 2}. A complementary set of experiments monitoring gas composition showed that N{sub 2} and CO{sub x} were produced by the reaction of acetate with NO + O{sub 2}. The rate of acetate consumption in NO + O{sub 2} exhibited the same order of magnitude as the NO reduction rate, indicating that the acetate is active as a reductant and takes part in the N{sub 2} formation. Nitrates can oxidize both C{sub 3}H{sub 6} and acetate, and are mostly reduced to N{sub 2}. A proposed reaction scheme explains the role of O{sub 2} in facilitating SCR of NO.« less

Selective etching of TiN over TaN and vice versa in chlorine-containing plasmas

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

Shin, Hyungjoo; Zhu Weiye; Liu Lei

2013-05-15

Selectivity of etching between physical vapor-deposited TiN and TaN was studied in chlorine-containing plasmas, under isotropic etching conditions. Etching rates for blanket films were measured in-situ using optical emission of the N{sub 2} (C{sup 3}{Pi}{sub u}{yields}B{sup 3}{Pi}{sub g}) bandhead at 337 nm to determine the etching time, and transmission electron microscopy to determine the starting film thickness. The etching selectivity in Cl{sub 2}/He or HCl/He plasmas was poor (<2:1). There was a window of very high selectivity of etching TiN over TaN by adding small amounts (<1%) of O{sub 2} in the Cl{sub 2}/He plasma. Reverse selectivity (10:1 of TaNmore » etching over TiN) was observed when adding small amounts of O{sub 2} to the HCl/He plasma. Results are explained on the basis of the volatility of plausible reaction products.« less

Molten salt corrosion of hot-pressed Si sub 3 N sub 4 /SiC-reinforced composites and effects of molten salt exposure on slow crack growth of hot-pressed Si sub 3 N sub 4

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

Henager, C.H. Jr.; Jones, R.H.

1989-11-03

Corrosion and slow crack growth of hot-pressed Si{sub 3}N{sub 4}- based ceramic materials were studied to arrive at an initial determination of the severity of Na{sub 2}SO{sub 4} molten salt environments. Slow crack growth testing revealed that Na{sub 2}SO{sub 4} molten salt exposure accelerated crack growth in hot-pressed Si{sub 3}N{sub 4} compared to crack growth in air at 1300 C. The salt exposure was observed to reduce the time to failure of precracked specimens by factors of two or three. Measured crack velocity was observed to obey a power law, V = AK{sup n}, with n = 5.2 {plus minus}more » 0.2 and A = 7.6 {times} 10{sup {minus}10}. Standard corrosion coupon tests were performed on specimens of Si{sub 3}N{sub 4}/SiC-reinforced composites and hot-pressed Si{sub 3}N{sub 4} monolithic material. Weight change measurements were performed after eight-hour immersion exposures at 950, 975, and 1000 C to Na{sub 2}SO{sub 4}. Hot-pressed Si{sub 3}N{sub 4} + 5% MgO and Si{sub 3}N{sub 4}/SiC whisker-reinforced material exhibited similar surface features after molten salt exposure. A Si{sub 3}N{sub 4}/SiC fiber-reinforced material, however, revealed complete dissolution of SiC chopped fiber reinforcements.« less

Chemi-ionization reactions of La, Pr, Tb, and Ho with atomic O and La with N{sub 2}O from 200 to 450 K

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

Ard, Shaun G.; Shuman, Nicholas S.; Martinez, Oscar

2016-08-28

The chemi-ionization rate coefficients of La, Pr, Tb, and Ho with O have been measured from 200 to 450 K using a thermalized flow tube apparatus. Both La and Tb were found to react near the calculated hard sphere collision limit, while the Pr and Ho reactions proceeded at roughly 40% of that limit at all temperatures. The efficiencies of these reactions are considered and the near thermoneutral character of the reaction with Ho can explain this case, whereas an explanation for the inefficiency of the Pr reaction remains elusive. The chemi-ionization reaction of La with N{sub 2}O was alsomore » studied and found to proceed roughly 2 orders of magnitude slower than the competing neutral oxidation pathway. The latter result disagrees with previous literature reports.« less

The reduction of nitric oxide by ammonia over polycrystalline platinum model catalysts in the presence of oxygen

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

Katona, T.; Guczi, L.; Somorjai, G.A.

1992-06-01

The reaction system of nitric oxide, ammonia, and oxygen was studied using batch-mode measurements in partial pressure ranges of 65-1000 Pa (0.5-7.6 Torr) on polycrystalline Pt foils over the temperature range 423-598 K. Under these conditions the oxidation of nitric oxide was not detectable. The ammonia oxidation reaction, using dioxygen, occurred in the temperature range 423-493 K, producing nitrogen and water as the only products. The activation energy of the nitrogen formation was found to be 86 kJ/mol. Above this temperature range, flow-mode measurements showed the formation of both nitrous oxide and nitric oxide. The reaction rate between ammonia andmore » oxygen was greatly decreased (about a factor of 10) by nitric oxide, while the reaction rate between nitric oxide and ammonia was accelerated (about 10-fold) due to the presence of oxygen. Nitric oxide reduction by ammonia in the presence of oxygen occurred in the temperature range 423-598 K. The products of the reaction were nitrogen, oxygen nitrous oxide, and water. The Arrhenius plot of the reaction showed a break near 523 K. Below this temperature the activation energy of the reaction was 13 kJ/mol, and in the higher-temperature range it was 62 kJ/mol. At 473 K, the N[sub 2]/N[sub 2]O ratio was about 0.6 and O[sub 2] formation was also monitored. At 573 K, the N[sub 2]N[sub 2]O ratio was approximately 2 and oxygen was consumed in the course of the reaction as well.« less

THE PHOTODISSOCIATION OF FORMALDEHYDE IN COMETS

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

Feldman, Paul D., E-mail: pfeldman@jhu.edu

2015-10-20

Observations of comets in the 905–1180 Å spectral band made with the Far Ultraviolet Spectroscopic Explorer in 2001 and 2004 show unusual features in the fluorescent emissions of CO and H{sub 2}. These include emission from a non-thermal high-J rotational population of CO and solar Lyα induced fluorescence from excited vibrational levels of H{sub 2}, both of which are attributed to the photodissociation of formaldehyde. In this paper we model the large number of observed H{sub 2} lines and demonstrate the dependence of the pumping on the heliocentric velocity of the comet and the solar line profiles. We also derivemore » the rotational and vibrational populations of H{sub 2} and show that they are consistent with the results of laboratory studies of the photodissociation of H{sub 2}CO. In addition to the principal series of H i and O i, the residual spectrum is found to consist mainly of the Rydberg series of C i multiplets from which we derive the mean carbon column abundance in the coma. Fluorescent emissions from N i and N{sub 2} are also searched for.« less

Heterogenous uptake of gaseous N(sub 2)O(sub 5) by sulfate aerosols

NASA Technical Reports Server (NTRS)

Leu, M. -T.; Kane, S. M.; Caloz, F.

2001-01-01

The heterogeneous uptake of gaseous N sub 2 O sub 5 by ammonium sulfate, ammonium bisulfate, and sulfuric acid aerosols as a function of relative humididty has been investigated at room temperature and atmsopheric pressure.

THE EFFECTS OF INITIAL ABUNDANCES ON NITROGEN IN PROTOPLANETARY DISKS

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

Schwarz, Kamber R.; Bergin, Edwin A.

2014-12-20

The dominant form of nitrogen provided to most solar system bodies is currently unknown, though available measurements show that the detected nitrogen in solar system rocks and ices is depleted with respect to solar abundances and the interstellar medium. We use a detailed chemical/physical model of the chemical evolution of a protoplanetary disk to explore the evolution and abundance of nitrogen-bearing molecules. Based on this model, we analyze how initial chemical abundances provided as either gas or ice during the early stages of disk formation influence which species become the dominant nitrogen bearers at later stages. We find that amore » disk with the majority of its initial nitrogen in either atomic or molecular nitrogen is later dominated by atomic and molecular nitrogen as well as NH{sub 3} and HCN ices, where the dominant species varies with disk radius. When nitrogen is initially in gaseous ammonia, it later becomes trapped in ammonia ice except in the outer disk where atomic nitrogen dominates. For a disk with the initial nitrogen in the form of ammonia ice, the nitrogen remains trapped in the ice as NH{sub 3} at later stages. The model in which most of the initial nitrogen is placed in atomic N best matches the ammonia abundances observed in comets. Furthermore, the initial state of nitrogen influences the abundance of N{sub 2}H{sup +}, which has been detected in protoplanetary disks. Strong N{sub 2}H{sup +} emission is found to be indicative of an N{sub 2} abundance greater than n{sub N{sub 2}}/n{sub H{sub 2}}>10{sup −6} in addition to tracing the CO snow line. Our models also indicate that NO is potentially detectable, with lower N gas abundances leading to higher NO abundances.« less

A Search for O2 in CO-Depleted Molecular Cloud Cores With Herschel

NASA Technical Reports Server (NTRS)

Wirstroem, Eva S.; Charnley, Steven B.; Cordiner, Martin; Ceccarelli, Cecilia

2016-01-01

The general lack of molecular oxygen in molecular clouds is an outstanding problem in astrochemistry. Extensive searches with the Submillimeter Astronomical Satellite, Odin, and Herschel have only produced two detections; upper limits to the O2 abundance in the remaining sources observed are about 1000 times lower than predicted by chemical models. Previous atomic oxygen observations and inferences from observations of other molecules indicated that high abundances of O atoms might be present in dense cores exhibiting large amounts of CO depletion. Theoretical arguments concerning the oxygen gas-grain interaction in cold dense cores suggested that, if O atoms could survive in the gas after most of the rest of the heavy molecular material has frozen out onto dust, then O2 could be formed efficiently in the gas. Using Herschel HIFI, we searched a small sample of four depletion cores-L1544, L694-2, L429, and Oph D-for emission in the low excitation O2 N(sub J)?=?3(sub 3)-1(sub 2) line at 487.249 GHz. Molecular oxygen was not detected and we derive upper limits to its abundance in the range of N(O2)/N (H2) approx. = (0.6-1.6) x10(exp -7). We discuss the absence of O2 in the light of recent laboratory and observational studies.

Measurement of the Auger parameter and Wagner plot for uranium compounds

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

Holliday, Kiel S.; Siekhaus, Wigbert; Nelson, Art J.

2013-05-15

In this study, the photoemission from the U 4f{sub 7/2} and 4d{sub 5/2} states and the U N{sub 6}O{sub 45}O{sub 45} and N{sub 67}O{sub 45}V x-ray excited Auger transitions were measured for a range of uranium compounds. The data are presented in Wagner plots and the Auger parameter is calculated to determine the utility of this technique in the analysis of uranium materials. It was demonstrated that the equal core-level shift assumption holds for uranium. It was therefore possible to quantify the relative relaxation energies, and uranium was found to have localized core-hole shielding. The position of compounds within themore » Wagner plot made it possible to infer information on bonding character and local electron density. The relative ionicity of the uranium compounds studied follows the trend UF{sub 4} > UO{sub 3} > U{sub 3}O{sub 8} > U{sub 4}O{sub 9}/U{sub 3}O{sub 7} Almost-Equal-To UO{sub 2} > URu{sub 2}Si{sub 2}.« less

Structure, luminescence and thermal quenching properties of Eu doped Sr{sub 2−x}Ba{sub x}Si{sub 5}N{sub 8} red phosphors

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

Liu, Y.H.; Chen, L.; Zhou, X.F.

Eu{sup 2+} doped Sr{sub 2-x}Ba{sub x}Si{sub 5}N{sub 8} phosphors were synthesized at 1610 ℃ for 4 h via the solid-state reaction method. The XRD results confirm that the complete solid solutions are formed. With the increase of x, the emission spectra show an obvious blue-shift from 610 nm to 585 nm under the excitation of 460 nm. The color tone can be tuned from yellow to red. The corresponding mechanism for the blue-shift of peak-wavelength is studied in detail. The results of decomposed Gaussian spectra and fluorescence lifetime show that the local coordination structure surrounding activator ions changes with increasingmore » x value. It is found that the probability of Eu occupying Sr1 and Sr2 site is dependent on Ba/Sr ratio. The variation of thermal quenching properties and the corresponding mechanism is discussed in detail. The results indicate that Eu{sup 2+} doped Sr{sub 2-x}Ba{sub x}Si{sub 5}N{sub 8} is a promising orange red-emitting phosphor for near UV or blue light-pumped white light-emitting-diodes (wLEDs). - Graphical abstract: Eu{sup 2+} doped Sr{sub 2-x}Ba{sub x}Si{sub 5}N{sub 8} solid solutions were prepared by the solid-state reaction method. The structure, luminescence and thermal quenching properties with varying Ba/Sr ratio were investigated in detail. - Highlights: • The stucture and luminescence properties of Eu doped Sr{sub 2-x}Ba{sub x}Si{sub 5}N{sub 8} phosphors were investigated. • The samples with the intermediate compositions(x=1.0,1.5) show better stability than the end members of both Sr{sub 2}Si{sub 5}N{sub 8}:Eu{sup 2+} and Ba{sub 2}Si{sub 5}N{sub 8}:Eu{sup 2+}. • The possible mechanism for the improvement of thermal quenching properties was proposed.« less

Chandra High Resolution Spectroscopy of the Circumnuclear Matter in the Broad Line Radio Galaxy, 3C 445

NASA Technical Reports Server (NTRS)

Reeves, J. N.; Gofford, J.; Braito, V.; Sambruna, R.

2010-01-01

We present evidence for X-ray line emitting and absorbing gas in the nucleus of the Broad-Line Radio Galaxy (BLRG), 3C445. A 200 ks Chandra LETG observation of 3C 445 reveals the presence of several highly ionized emission lines in the soft X-ray spectrum, primarily from the He and H-like ions of O, Ne, Mg and Si. Radiative recombination emission is detected from O VII and O VIII, indicating that the emitting gas is photoionized. The He-like emission appears to be resolved into forbidden and intercombination line components, which implies a high density of greater than 10(sup 10) cm(sup -3), while the lines are velocity broadened with a mean width of 2600 km s(sup -1). The density and widths of the ionized lines indicate an origin of the gas on sub-parsec scales in the Broad Line Region (BLR). The X-ray continuum of 3C 445 is heavily obscured by a photoionized absorber of column density N(sub H) = 2 x 10(sup 23) cm(sup -2) and ionization parameter log xi = 1.4 erg cm s(sup -1). However the view of the X-ray line emission is unobscured, which requires the absorber to be located at radii well within any parsec scale molecular torus. Instead we suggest that the X-ray absorber in 3C 445 may be associated with an outflowing, but clumpy accretion disk wind, with an observed outflow velocity of approximately 10000 km s(sup -1).

Effect of grain growth of [beta]-silicon nitride on strength, Weibull modulus, and fracture toughness

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

Hirosaki, Naota; Akimune, Yoshio; Mitomo, Mamoru

1993-07-01

[beta]-Si[sub 3]N[sub 4] powder containing 1 mol% of equimolar Y[sub 2]O[sub 3]-Nd[sub 2]O[sub 3] was gas-pressure sintered at 2,000C for 2 h (SN2), 4 h (SN4), and 8 h (SN8) in 30-MPa nitrogen gas. These materials had a microstructure of in-situ composites'' as a result of exaggerated grain growth of some [beta]-Si[sub 3]N[sub 4] grains during firing. Growth of elongated grains was controlled by the sintering time, so that the desired microstructures were obtained. SN2 had a Weibull modulus as high as 53 because of the uniform size and spatial distribution of its large grains. SN4 had a fracture toughnessmore » of 10.3 MPa[center dot]m[sup 1/2] because of toughening provided by the bridging of elongated grains, whereas SN8 showed a lower fracture toughness, possibly caused by extensive microcracking resulting from excessively large grains. Gas-pressure sintering of [beta]-Si[sub 3]N[sub 4] powder was shown to be effective in fostering selective grain growth for obtaining the desired composite microstructure.« less

Parameterization of N2O5 Reaction Probabilities on the Surface of Particles Containing Ammonium, Sulfate, and Nitrate

EPA Science Inventory

A comprehensive parameterization was developed for the heterogeneous reaction probability (γ) of N₂O₅ as a function of temperature, relative humidity, particle composition, and phase state, for use in advanced air quality models. The reaction probabilities o...

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

Gupta, Bipin Kumar, E-mail: bipinbhu@yahoo.com; Kumar, Arun; Amity Institute of Applied Science, Amity University, Noida, Uttar Pradesh 201303

Herein, a novel green emitting long-persistent Sr{sub 3}SiAl{sub 4}O{sub 11}:Eu{sup 2+}/Dy{sup 3+} phosphor was synthesized in a single phase form using facile solid state reaction method under the reducing atmosphere of 10% H{sub 2} and 90% N{sub 2}. The resulting phosphor exhibits hyper-sensitive strong broad green emission, peaking at 510 nm upon 340 nm excitation wavelength, which is attributed to the 4f{sup 6}5d{sup 1}-4f{sup 7} transitions of emission center of europium (Eu{sup 2+}) ions. Moreover, the incorporation of dysprosium (Dy{sup 3+}) ions, which act as effective hole trap centers with appropriate depth, largely enhances the photoluminescence characteristics and greatly improves the persistentmore » intense luminescence behavior of Sr{sub 3}SiAl{sub 4}O{sub 11}:Eu{sup 2+}/Dy{sup 3+} phosphor under ultraviolet (UV) excitation. In addition, with the optimum doping concentration and sufficient UV excitation time period, the as-synthesized phosphor can be persisted afterglow for time duration ∼4 h with maximum luminescence intensity. Thus, these results suggest that this phosphor could be expected as an ultimate choice for next generation advanced luminescent materials in security applications such as latent finger-marks detection, photo-masking induced phosphorescent images, and security code detection.« less

Quantitative and sensitive analysis of CN molecules using laser induced low pressure He plasma

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

Pardede, Marincan; Hedwig, Rinda; Abdulmadjid, Syahrun Nur

2015-03-21

We report the results of experimental study on CN 388.3 nm and C I 247.8 nm emission characteristics using 40 mJ laser irradiation with He and N{sub 2} ambient gases. The results obtained with N{sub 2} ambient gas show undesirable interference effect between the native CN emission and the emission of CN molecules arising from the recombination of native C ablated from the sample with the N dissociated from the ambient gas. This problem is overcome by the use of He ambient gas at low pressure of 2 kPa, which also offers the additional advantages of cleaner and stronger emission lines. The resultmore » of applying this favorable experimental condition to emission spectrochemical measurement of milk sample having various protein concentrations is shown to yield a close to linear calibration curve with near zero extrapolated intercept. Additionally, a low detection limit of 5 μg/g is found in this experiment, making it potentially applicable for quantitative and sensitive CN analysis. The visibility of laser induced breakdown spectroscopy with low pressure He gas is also demonstrated by the result of its application to spectrochemical analysis of fossil samples. Furthermore, with the use of CO{sub 2} ambient gas at 600 Pa mimicking the Mars atmosphere, this technique also shows promising applications to exploration in Mars.« less

Catalyst and method for reduction of nitrogen oxides

DOEpatents

Ott, Kevin C [Los Alamos, NM

2008-05-27

A Selective Catalytic Reduction (SCR) catalyst was prepared by slurry coating ZSM-5 zeolite onto a cordierite monolith, then subliming an iron salt onto the zeolite, calcining the monolith, and then dipping the monolith either into an aqueous solution of manganese nitrate and cerium nitrate and then calcining, or by similar treatment with separate solutions of manganese nitrate and cerium nitrate. The supported catalyst containing iron, manganese, and cerium showed 80 percent conversion at 113 degrees Celsius of a feed gas containing nitrogen oxides having 4 parts NO to one part NO.sub.2, about one equivalent ammonia, and excess oxygen; conversion improved to 94 percent at 147 degrees Celsius. N.sub.2O was not detected (detection limit: 0.6 percent N.sub.2O).

Catalyst and method for reduction of nitrogen oxides

DOEpatents

Ott, Kevin C [Los Alamos, NM

2008-08-19

A Selective Catalytic Reduction (SCR) catalyst was prepared by slurry coating ZSM-5 zeolite onto a cordierite monolith, then subliming an iron salt onto the zeolite, calcining the monolith, and then dipping the monolith either into an aqueous solution of manganese nitrate and cerium nitrate and then calcining, or by similar treatment with separate solutions of manganese nitrate and cerium nitrate. The supported catalyst containing iron, manganese, and cerium showed 80 percent conversion at 113 degrees Celsius of a feed gas containing nitrogen oxides having 4 parts NO to one part NO.sub.2, about one equivalent ammonia, and excess oxygen; conversion improved to 94 percent at 147 degrees Celsius. N.sub.2O was not detected (detection limit: 0.6 percent N.sub.2O).

Catalyst for reduction of nitrogen oxides

DOEpatents

Ott, Kevin C.

2010-04-06

A Selective Catalytic Reduction (SCR) catalyst was prepared by slurry coating ZSM-5 zeolite onto a cordierite monolith, then subliming an iron salt onto the zeolite, calcining the monolith, and then dipping the monolith either into an aqueous solution of manganese nitrate and cerium nitrate and then calcining, or by similar treatment with separate solutions of manganese nitrate and cerium nitrate. The supported catalyst containing iron, manganese, and cerium showed 80 percent conversion at 113 degrees Celsius of a feed gas containing nitrogen oxides having 4 parts NO to one part NO.sub.2, about one equivalent ammonia, and excess oxygen; conversion improved to 94 percent at 147 degrees Celsius. N.sub.2O was not detected (detection limit: 0.6 percent N.sub.2O).

LOW TEMPERATURE PROCESS FOR THE REMOVAL AND RECOVERY OF CHLORIDES AND NITRATES FROM AQUEOUS NITRATE SOLUTIONS

DOEpatents

Savolainen, J.E.

1963-01-29

A method is described for reducing the chloride content of a solution derived from the dissolution of a stainless steel clad nuclear fuel element with an aqua regia dissolution medium. The solutlon is adjusted to a nitric acid concentration in the range 5 to 10 M and is countercurrently contacted at room temperature with a gaseous oxide of nitrogen selected from NO, NO/sub 2/, N/sub 2/ O/sub 3/, and N/sub 2/O/sub 4/. Chlo ride is recovered from the contacted solution as nitrosyl chloride. After reduction of the chloride content, the solution is then contacted with gaseous NO to reduce the nitric acid molarity to a desired level. (AEC)

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

Pak, S.; Sites, J.R.

A Kaufman-type broad beam ion source, used for sputtering and etching purposes, has been operated with Ar, Kr,O/sub 2/ and N/sub 2/ gas inputs over a wide range of beam energies (200-1200 eV) and gas flow rates (1-10 sccm). The maximum ion beam current density for each gas saturates at about 2.5 mA/sq. cm. as gas flow is increased. The discharge threshold voltage necessary to produce a beam and the beam efficiency (beam current/molecular current), however, varied considerably. Kr had the lowest threshold and highest efficiency, Ar next, then N/sub 2/ and O/sub 2/. The ion beam current varied onlymore » weakly with beam energy for low gas flow rates, but showed a factor of two increase when the gas flow was higher.« less

EMBEDDED PROTOSTARS IN THE DUST, ICE, AND GAS IN TIME (DIGIT) HERSCHEL KEY PROGRAM: CONTINUUM SEDs, AND AN INVENTORY OF CHARACTERISTIC FAR-INFRARED LINES FROM PACS SPECTROSCOPY

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

Green, Joel D.; Evans, Neal J. II; Rascati, Michelle R.

2013-06-20

We present 50-210 {mu}m spectral scans of 30 Class 0/I protostellar sources, obtained with Herschel-PACS, and 0.5-1000 {mu}m spectral energy distributions, as part of the Dust, Ice, and Gas in Time Key Program. Some sources exhibit up to 75 H{sub 2}O lines ranging in excitation energy from 100 to 2000 K, 12 transitions of OH, and CO rotational lines ranging from J = 14 {yields} 13 up to J = 40 {yields} 39. [O I] is detected in all but one source in the entire sample; among the sources with detectable [O I] are two very low luminosity objects. Themore » mean 63/145 {mu}m [O I] flux ratio is 17.2 {+-} 9.2. The [O I] 63 {mu}m line correlates with L{sub bol}, but not with the time-averaged outflow rate derived from low-J CO maps. [C II] emission is in general not local to the source. The sample L{sub bol} increased by 1.25 (1.06) and T{sub bol} decreased to 0.96 (0.96) of mean (median) values with the inclusion of the Herschel data. Most CO rotational diagrams are characterized by two optically thin components ( = (0.70 {+-} 1.12) x 10{sup 49} total particles). N{sub CO} correlates strongly with L{sub bol}, but neither T{sub rot} nor N{sub CO}(warm)/N{sub CO}(hot) correlates with L{sub bol}, suggesting that the total excited gas is related to the current source luminosity, but that the excitation is primarily determined by the physics of the interaction (e.g., UV-heating/shocks). Rotational temperatures for H{sub 2}O ( = 194 +/- 85 K) and OH ( = 183 +/- 117 K) are generally lower than for CO, and much of the scatter in the observations about the best fit is attributed to differences in excitation conditions and optical depths among the detected lines.« less

Dissociative electron attachment to the gas-phase nucleobase hypoxanthine

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

Dawley, M. Michele; Tanzer, Katrin; Denifl, Stephan, E-mail: Stephan.Denifl@uibk.ac.at, E-mail: Sylwia.Ptasinska.1@nd.edu

We present high-resolution measurements of the dissociative electron attachment (DEA) to isolated gas-phase hypoxanthine (C{sub 5}H{sub 4}N{sub 4}O, Hyp), a tRNA purine base. The anion mass spectra and individual ion efficiency curves from Hyp were measured as a function of electron energy below 9 eV. The mass spectra at 1 and 6 eV exhibit the highest anion yields, indicating possible common precursor ions that decay into the detectable anionic fragments. The (Hyp − H) anion (C{sub 5}H{sub 3}N{sub 4}O{sup −}) exhibits a sharp resonant peak at 1 eV, which we tentatively assign to a dipole-bound state of the keto-N1H,N9H tautomermore » in which dehydrogenation occurs at either the N1 or N9 position based upon our quantum chemical computations (B3LYP/6-311+G(d,p) and U(MP2-aug-cc-pVDZ+)) and prior studies with adenine. This closed-shell dehydrogenated anion is the dominant fragment formed upon electron attachment, as with other nucleobases. Seven other anions were also observed including (Hyp − NH){sup −}, C{sub 4}H{sub 3}N{sub 4}{sup −}/C{sub 4}HN{sub 3}O{sup −}, C{sub 4}H{sub 2}N{sub 3}{sup −}, C{sub 3}NO{sup −}/HC(HCN)CN{sup −}, OCN{sup −}, CN{sup −}, and O{sup −}. Most of these anions exhibit broad but weak resonances between 4 and 8 eV similar to many analogous anions from adenine. The DEA to Hyp involves significant fragmentation, which is relevant to understanding radiation damage of biomolecules.« less

Japanese RDF-fired power generation system and fundamental research on RDF combustion

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

Narukawa, Kimihito; Goto, Hidenori; Chen, Y.

1997-12-31

Power generation from refuse derived fuel (RDF) is one of the new technologies for municipal solid waste (MSW) management. This technology is strongly attracting the attention of the Japanese government. The results of a feasibility study of this system in Japan is presented. To develop this highly efficient RDF-fired CFB generating process, combustibility and dechlorination characteristics of RDF were investigated by both the thermo-balance technique and combustion tests with an electric furnace. RDF combustion tests by a bench scale CFBC were carried out and then the following experimental results were obtained: (1) RDF can be combusted almost completely even inmore » small scale CFBC; (2) HCl and N{sub 2}O emissions are quite low at any conditions; and (3) NO{sub x} emissions are a little higher in single stage combustion, however they are reduced at 50% air bias ratio. Some of the results can be explained by a RDF combustion model.« less

Transient competitive complexation in biological kinetic isotope fractionation explains non-steady isotopic effects: Theory and application to denitrification in soils

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

Maggi, F.M.; Riley, W.J.

2009-06-01

The theoretical formulation of biological kinetic reactions in isotopic applications often assume first-order or Michaelis-Menten-Monod kinetics under the quasi-steady-state assumption to simplify the system kinetics. However, isotopic e ects have the same order of magnitude as the potential error introduced by these simpli cations. Both formulations lead to a constant fractionation factor which may yield incorrect estimations of the isotopic effect and a misleading interpretation of the isotopic signature of a reaction. We have analyzed the isotopic signature of denitri cation in biogeochemical soil systems by Menyailo and Hungate [2006], where high {sup 15}N{sub 2}O enrichment during N{sub 2}O productionmore » and inverse isotope fractionation during N{sub 2}O consumption could not be explained with first-order kinetics and the Rayleigh equation, or with the quasi-steady-state Michaelis-Menten-Monod kinetics. When the quasi-steady-state assumption was relaxed, transient Michaelis-Menten-Monod kinetics accurately reproduced the observations and aided in interpretation of experimental isotopic signatures. These results may imply a substantial revision in using the Rayleigh equation for interpretation of isotopic signatures and in modeling biological kinetic isotope fractionation with first-order kinetics or quasi-steady-state Michaelis-Menten-Monod kinetics.« less

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

Gabuda, S. P.; Kozlova, S. G.; Novosibirsk State University, 2, Pirogova Str., Novosibirsk 630090

We report an abnormal difference of low-temperature mobility of left-twisted and right-twisted conformations of roto symmetric molecules C{sub 6}H{sub 12}N{sub 2} (dabco) located in the same positions in crystal Zn{sub 2}(C{sub 8}H{sub 4}O{sub 4}){sub 2}⋅C{sub 6}H{sub 12}N{sub 2}. The difference between {sup 1}H NMR (Nuclear Magnetic Resonance) spin-relaxation data for left-twisted and right-twisted molecules reaches ∼3 × 10{sup 3} times at 8 K and tends to grow at lower temperatures. We argue that taking into account four-component relativistic Dirac wave functions in the vicinity of the nodal plane of dabco molecules and vacuum fluctuations due to virtual particle-antiparticle pairs canmore » explain the changes which C{sub 6}H{sub 12}N{sub 2} conformations undergo at low temperatures.« less

Nanocrystalline Cs{sub x}WO{sub 3} particles: Effects of N{sub 2} annealing on microstructure and near-infrared shielding characteristics

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

Liu, Jing-Xiao, E-mail: drliu-shi@dlpu.edu.cn; Institute of Multidisciplinary Research for Advanced Material, Tohoku University, Sendai, 980-8577,Japan; Shi, Fei

2013-10-15

In order to further improve the near-infrared shielding properties of cesium tungsten bronze (Cs{sub x}WO{sub 3}) for solar filter applications, Cs{sub x}WO{sub 3} particles were prepared by solvothermal reaction method and the effects of nitrogen annealing on the microstructure and near-infrared shielding properties of Cs{sub x}WO{sub 3} were investigated. The obtained Cs{sub x}WO{sub 3} samples were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy and spectrophotometer. The results indicate that nanosheet-like Cs{sub x}WO{sub 3} particles with hexagonal structure began to transform into nanorods after annealed at temperature higher than 600 °C. The near-infrared shielding propertiesmore » of Cs{sub x}WO{sub 3} particles could be further improved by N{sub 2} annealing at 500–700 °C. Particularly, the 500 °C-annealed Cs{sub x}WO{sub 3} samples in the N{sub 2} atmosphere showed best near-infrared shielding properties. It was suggested that the excellent near-infrared shielding ability of the 500 °C-annealed Cs{sub x}WO{sub 3} samples is correlated with its minimum O/W atomic ratio and most oxygen vacancies. Highlights: • N{sub 2} annealing could further improve the near-infrared (NIR) shielding of Cs{sub x}WO{sub 3}. • Effects of N{sub 2} annealing on microstructure and NIR shielding of Cs{sub x}WO{sub 3} were studied. • The 500 °C-N{sub 2}-annealed Cs{sub x}WO{sub 3} exhibited minimum O/W ratio and most oxygen vacancies. • The 500 °C-N{sub 2}-annealed Cs{sub x}WO{sub 3} particles exhibited best NIR shielding properties.« less

Lifecycle of laser-produced air sparks

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

Harilal, S. S., E-mail: hari@pnnl.gov; Brumfield, B. E.; Phillips, M. C.

2015-06-15

We investigated the lifecycle of laser-generated air sparks or plasmas using multiple plasma diagnostic tools. The sparks were generated by focusing the fundamental radiation from an Nd:YAG laser in air, and studies included early and late time spark dynamics, decoupling of the shock wave from the plasma core, emission from the spark kernel, cold gas excitation by UV radiation, shock waves produced by the air spark, and the spark's final decay and turbulence formation. The shadowgraphic and self-emission images showed similar spark morphology at earlier and late times of its lifecycle; however, significant differences are seen in the midlife images.more » Spectroscopic studies in the visible region showed intense blackbody-type radiation at early times followed by clearly resolved ionic, atomic, and molecular emission. The detected spectrum at late times clearly contained emission from both CN and N{sub 2}{sup +}. Additional spectral features have been identified at late times due to emission from O and N atoms, indicating some degree of molecular dissociation and excitation. Detailed spatially and temporally resolved emission analysis provides insight about various physical mechanisms leading to molecular and atomic emission by air sparks, including spark plasma excitation, heating of cold air by UV radiation emitted by the spark, and shock-heating.« less

The synthesis and crystal structure of 2-[4(S)-4,5-dihydro-4-phenyl-2-oxazolinyl]-benzenamine, and 2-[4(S)-4,5-dihydro-4-benzyl-2-oxazolinyl]-benzenamine

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

Mei Luo, E-mail: Lmhh5523385@yahoo.cn; Hai Zhangjia; Hao Yin

2010-12-15

Two oxazolines compound 1a and 1b, 2-[4(S)-4,5-dihydro-4-phenyl-2-ozazolinyl-benzenamine, and (C{sub 15}H{sub 14}N{sub 2}O), 2-[4(S)-4,5-dihydro-4-benzyl-2-ozazolinyl-benzenamine (C{sub 16}H{sub 16}N{sub 2}O) were obtained in moderate yield from the reactions of 2-aminobenzonitrile with optically active L-(+)-Phenylglycinol and L-(+)-Phenylalaninol, respectively, in chlorobenzene under dry, anaerobic conditions. ZnCl{sub 2} was dried under vacuum and acted as a Lewis acid catalyst in this reaction. The structures of 1a and 1b were determined by X-ray diffraction and NMR. There exist intra- and intermolecular N-H-N hydrogen bonds in the crystal structure.

Oxygen related recombination defects in Ta{sub 3}N{sub 5} water splitting photoanode

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

Fu, Gao; Yu, Tao, E-mail: yscfei@nju.edu.cn, E-mail: yutao@nju.edu.cn; Zou, Zhigang

2015-10-26

A key route to improving the performance of Ta{sub 3}N{sub 5} photoelectrochemical film devices in solar driving water splitting to hydrogen is to understand the nature of the serious recombination of photo-generated carriers. Here, by using the temperature-dependent photoluminescence (PL) spectrum, we confirmed that for the Ta{sub 3}N{sub 5} films prepared by nitriding Ta{sub 2}O{sub 5} precursor, one PL peak at 561 nm originates from deep-level defects recombination of the oxygen-enriched Ta{sub 3}N{sub 5} phases, and another one at 580 nm can be assigned to band recombination of Ta{sub 3}N{sub 5} itself. Both of the two bulk recombination processes may decrease themore » photoelectrochemical performance of Ta{sub 3}N{sub 5}. It was difficult to remove the oxygen-enriched impurities in Ta{sub 3}N{sub 5} films by increasing the nitriding temperatures due to their high thermodynamically stability. In addition, a broadening PL peak between 600 and 850 nm resulting from oxygen related surface defects was observed by the low-temperature PL measurement, which may induce the surface recombination of photo-generated carriers and can be removed by increasing the nitridation temperature. Our results provided direct experimental evidence to understand the effect of oxygen-related crystal defects in Ta{sub 3}N{sub 5} films on its photoelectric performance.« less

Understanding Nitrogen Fixation

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

Paul J. Chirik

The purpose of our program is to explore fundamental chemistry relevant to the discovery of energy efficient methods for the conversion of atmospheric nitrogen (N{sub 2}) into more value-added nitrogen-containing organic molecules. Such transformations are key for domestic energy security and the reduction of fossil fuel dependencies. With DOE support, we have synthesized families of zirconium and hafnium dinitrogen complexes with elongated and activated N-N bonds that exhibit rich N{sub 2} functionalization chemistry. Having elucidated new methods for N-H bond formation from dihydrogen, C-H bonds and Broensted acids, we have since turned our attention to N-C bond construction. These reactionsmore » are particularly important for the synthesis of amines, heterocycles and hydrazines with a range of applications in the fine and commodity chemicals industries and as fuels. One recent highlight was the discovery of a new N{sub 2} cleavage reaction upon addition of carbon monoxide which resulted in the synthesis of an important fertilizer, oxamide, from the diatomics with the two strongest bonds in chemistry. Nitrogen-carbon bonds form the backbone of many important organic molecules, especially those used in the fertilizer and pharamaceutical industries. During the past year, we have continued our work in the synthesis of hydrazines of various substitution patterns, many of which are important precursors for heterocycles. In most instances, the direct functionalization of N{sub 2} offers a more efficient synthetic route than traditional organic methods. In addition, we have also discovered a unique CO-induced N{sub 2} bond cleavage reaction that simultaneously cleaves the N-N bond of the metal dinitrogen compound and assembles new C-C bond and two new N-C bonds. Treatment of the CO-functionalized core with weak Broensted acids liberated oxamide, H{sub 2}NC(O)C(O)NH{sub 2}, an important slow release fertilizer that is of interest to replace urea in many applications. The synthesis of ammonia, NH{sub 3}, from its elements, H{sub 2} and N{sub 2}, via the venerable Haber-Bosch process is one of the most significant technological achievements of the past century. Our research program seeks to discover new transition metal reagents and catalysts to disrupt the strong N {triple_bond} N bond in N{sub 2} and create new, fundamental chemical linkages for the construction of molecules with application as fuels, fertilizers and fine chemicals. With DOE support, our group has discovered a mild method for ammonia synthesis in solution as well as new methods for the construction of nitrogen-carbon bonds directly from N{sub 2}. Ideally these achievements will evolve into more efficient nitrogen fixation schemes that circumvent the high energy demands of industrial ammonia synthesis. Industrially, atmospheric nitrogen enters the synthetic cycle by the well-established Haber-Bosch process whereby N{sub 2} is hydrogenated to ammonia at high temperature and pressure. The commercialization of this reaction represents one of the greatest technological achievements of the 20th century as Haber-Bosch ammonia is responsible for supporting approximately 50% of the world's population and serves as the source of half of the nitrogen in the human body. The extreme reaction conditions required for an economical process have significant energy consequences, consuming 1% of the world's energy supply mostly in the form of pollution-intensive coal. Moreover, industrial H{sub 2} synthesis via the water gas shift reaction and the steam reforming of methane is fossil fuel intensive and produces CO{sub 2} as a byproduct. New synthetic methods that promote this thermodynamically favored transformation ({Delta}G{sup o} = -4.1 kcal/mol) under milder conditions or completely obviate it are therefore desirable. Most nitrogen-containing organic molecules are derived from ammonia (and hence rely on the Haber-Bosch and H{sub 2} synthesis processes) and direct synthesis from atmospheric nitrogen could, in principle, be more energy-efficient. This is particularly attractive given the interest in direct hydrazine fuel cells.« less

Note: Cold spectra of the electronic transition A{sup 2}Σ{sup +}-X{sup 2}Π of N{sub 2}O{sup +} radical: High resolution analysis of the bands 000-100, 100-100, and 001-101

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

Lessa, L. L.; Martins, A. S.; Fellows, C. E., E-mail: fellows@if.uff.br

2015-10-28

In this note, three vibrational bands of the electronic transition A{sup 2}Σ{sup +}-X{sup 2}Π of the N{sub 2}O{sup +} radical (000-100, 100-100, and 001-101) were theoretically analysed. Starting from Hamiltonian models proposed for this kind of molecule, their parameters were calculated using a Levenberg-Marquardt fit procedure in order to reduce the root mean square deviation from the experimental transitions below to 0.01 cm{sup −1}. The main objective of this work is to obtain new and reliable values for rotational constant B″ and the spin-orbit interaction parameter A of the analysed vibrational levels of the X{sup 2}Π electronic state of thismore » molecule.« less

Influence of double- and triple-layer antireflection coatings on the formation of photocurrents in multijunction III–V solar cells

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

Musalinov, S. B.; Anzulevich, A. P.; Bychkov, I. V.

2017-01-15

The results of simulation by the transfer-matrix method of TiO{sub 2}/SiO{sub 2} double-layer and TiO{sub 2}/Si{sub 3}N{sub 4}/SiO{sub 2} triple-layer antireflection coatings for multijunction InGaP/GaAs/Ge heterostructure solar cells are presented. The TiO{sub 2}/SiO{sub 2} double-layer antireflection coating is experimentally developed and optimized. The experimental spectral dependences of the external quantum yield of the InGaP/GaAs/Ge heterostructure solar cell and optical characteristics of antireflection coatings, obtained in the simulation, are used to determine the photogenerated current densities of each subcell in the InGaP/GaAs/Ge solar cell under AM1.5D irradiation conditions (1000 W/m{sup 2}) and for the case of zero reflection loss. It ismore » shown in the simulation that the optimized TiO{sub 2}/Si{sub 3}N{sub 4}/SiO{sub 2} triple-layer antireflection coating provides a 2.3 mA/cm{sup 2} gain in the photocurrent density for the Ge subcell under AM1.5D conditions in comparison with the TiO{sub 2}/SiO{sub 2} double-layer antireflection coating under consideration. This thereby provides an increase in the fill factor of the current–voltage curve and in the output electric power of the multijunction solar cell.« less

Assessing photocatalytic power of g-C{sub 3}N{sub 4} for solar fuel production: A first-principles study involving quasi-particle theory and dispersive forces

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

Osorio-Guillén, J. M., E-mail: mario.osorio@udea.edu.co; Espinosa-García, W. F.; Grupo de Investigación en Modelamiento y Simulación Computacional, Facultad de Ingenierías, Universidad de San Buenaventura Seccional Medellín, Carrera 56C No 51-110, Medellín

2015-09-07

First-principles quasi-particle theory has been employed to assess catalytic power of graphitic carbon nitride, g-C{sub 3}N{sub 4}, for solar fuel production. A comparative study between g-h-triazine and g-h-heptazine has been carried out taking also into account van der Waals dispersive forces. The band edge potentials have been calculated using a recently developed approach where quasi-particle effects are taken into account through the GW approximation. First, it was found that the description of ground state properties such as cohesive and surface formation energies requires the proper treatment of dispersive interaction. Furthermore, through the analysis of calculated band-edge potentials, it is shownmore » that g-h-triazine has high reductive power reaching the potential to reduce CO{sub 2} to formic acid, coplanar g-h-heptazine displays the highest thermodynamics force toward H{sub 2}O/O{sub 2} oxidation reaction, and corrugated g-h-heptazine exhibits a good capacity for both reactions. This rigorous theoretical study shows a route to further improve the catalytic performance of g-C{sub 3}N{sub 4}.« less

Characteristics of supercritical turbulence from Direct Numerical Simulations of C(sub 7)H(sub 16)/N(sub 2) and O(sub 2)/H(sub 2)

NASA Technical Reports Server (NTRS)

Okong'o, N. A.; Bellan, J.

2003-01-01

Analysis of Direct Numerical Simulations (DNS) transitional states of temporal, supercritical mixing layers for C7H16/N2 and O2/H2 shows that the evolution of all layers is characterized by the formation of high-density-gradient magnitude (HDGM) regions.

Nonlinear refraction and two-photon absorption in dense 2Bi{sub 2}O{sub 3}-B{sub 2}O{sub 3} glasses

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

Paramesh, Gadige; Varma, K. B. R.

2012-06-05

High density transparent glasses (7.86 g/cc) were fabricated in the 2Bi{sub 2}O{sub 3}-B{sub 2}O{sub 3} (BBO) system. Optical band gap of the obtained glasses was found to be 2.6eV. The refractive index measured for these glasses was 2.25{+-}0.05 at {lambda}=543 nm. Nonlinear refraction and absorption studies were carried out on the BBO glasses using z-scan technique at {lambda}=532 nm of 10 ns pulse width. The nonlinear refractive index obtained was n{sub 2}=12.1x10{sup -14} cm{sup 2}/W and nonlinear absorption coefficient was {beta}=15.2 cm/GW. The n{sub 2} and {beta} values of the BBO glasses were large compared to the other reported highmore » index bismuth based oxide glass systems in the literature. These were attributed to the high density, high linear refractive index, low band gap and two photon absorption associated with these glasses. The electronic origin of large nonlinearities was discussed based on bond-orbital theory.« less

Plasma regenerated particulate trap and NO.sub.x reduction system

DOEpatents

Penetrante, Bernardino M.; Vogtlin, George E.; Merritt, Bernard T.; Brusasco, Raymond M.

2000-01-01

A non-catalytic two-stage process for removal of NO.sub.x and particulates from engine exhaust comprises a first stage that plasma converts NO to NO.sub.2 in the presence of O.sub.2 and hydrocarbons, and a second stage, which preferably occurs simultaneously with the first stage, that converts NO.sub.2 and carbon soot particles to respective environmentally benign gases that include N.sub.2 and CO.sub.2. By preconverting NO to NO.sub.2 in the first stage, the efficiency of the second stage for NO.sub.x reduction is enhanced while carbon soot from trapped particulates is simultaneously converted to CO.sub.2 when reacting with the NO.sub.2 (that converts to N.sub.2). For example, an internal combustion engine exhaust is connected by a pipe to a chamber where carbon-containing particulates are electrostatically trapped or filtered and a non-thermal plasma converts NO to NO.sub.2 in the presence of O.sub.2 and hydrocarbons. Volatile hydrocarbons (C.sub.x H.sub.y) from the trapped particulates are oxidized in the plasma and the remaining soot from the particulates reacts with the NO.sub.2 to convert NO.sub.2 to N.sub.2, and the soot to CO.sub.2. The nitrogen exhaust components remain in the gas phase throughout the process, with no accompanying adsorption.

A PROFILE ANALYSIS OF RAMAN-SCATTERED O VI BANDS AT 6825 Å AND 7082 Å IN SANDULEAK’S STAR

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

Heo, Jeong-Eun; Lee, Hee-Won; Angeloni, Rodolfo

2016-12-20

We present a detailed modeling of the two broad bands observed at 6825 and 7082 Å in Sanduleak’s star, a controversial object in the Large Magellanic Cloud. These bands are known to originate from Raman scattering of O vi  λ λ 1032 and 1038 photons with atomic hydrogen and are only observed in bona fide symbiotic stars. Our high-resolution spectrum obtained with the Magellan Inamori Kyocera Echelle spectrograph at the Magellan-Clay Telescope reveals, quite surprisingly, that the profiles of the two bands look very different: while the Raman 6825 Å band shows a single broad profile with a redward extendedmore » bump, the Raman 7082 Å band exhibits a distinct triple-peak profile. Our model suggests that the O vi emission nebula can be decomposed into a red, blue, and central emission region from an accretion disk, a bipolar outflow, and a further compact, optically thick region. We also perform Monte Carlo simulations with the aim of fitting the observed flux ratio F (6825)/ F (7082) ∼ 4.5, which indicates that the neutral region in Sanduleak’s star is characterized by the column density N{sub Hi} ∼ 1 × 10{sup 23} cm{sup −2}.« less

IC 751: A New Changing Look AGN Discovered by NuSTAR

NASA Technical Reports Server (NTRS)

Ricci, C.; Bauer, F. E.; Arevalo, P.; Boggs, S.; Brandt, W. N.; Christensen, F. E.; Craig, W. W.; Ghandi, P.; Hailey, C. J.; Harrison, F. A.;

Infrared and TPD studies of nitrates adsorbed on Tb{sub 4}O{sub 7}, La{sub 2}O{sub 3}, BaO, and MgO/{gamma}-Al{sub 2}O{sub 3}

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

Chi, Y.; Chuang, S.S.C.

2000-05-18

NO and O{sub 2} coadsorption on {gamma}-Al{sub 2}O{sub 3}-supported Tb{sub 4}O{sub 7}, La{sub 2}O{sub 3}, BaO, and MgO has been investigated by in situ infrared spectroscopy coupled with temperature-programmed decomposition and desorption. BaO/{gamma}-Al{sub 2}O{sub 3} and MgO/{gamma}-Al{sub 2}O{sub 3} possess a higher NO{sub x} storage capability than Tb{sub 4}O{sub 7}/{gamma}-Al{sub 2}O{sub 3} and La{sub 2}O{sub 3}/{gamma}-Al{sub 2}O{sub 3}. NO/O{sub 2} coadsorbed on Tb{sub 4}O{sub 7}, La{sub 2}O{sub 3}, and BaO in the form of bridging bidentate, chelating bidentate, and monodentate nitrates, and on MgO in the form of bridging bidentate and monodentate nitrates via the reaction of adsorbed NO withmore » adsorbed oxygen at 298 K. NO/O{sub 2} coadsorbed as a chelating bidentate nitrate on Tb{sub 4}O{sub 7} and La{sub 2}O{sub 3}, and as a distinctive bridging bidentate nitrate on BaO and MgO via the reaction of adsorbed NO with surface lattice oxygen at 523 K. These various forms of adsorbed nitrate differ in structure and reactivity from Tb(NO{sub 3}){sub 3}, La(NO{sub 3}){sub 3}, Ba(NO{sub 3}){sub 2}, and Mg(NO{sub 3}){sub 2}, the precursor used to prepare metal oxides for NO/O{sub 2} coadsorption. Temperature-programmed desorption (TPD) of chelating bidentate nitrate on Tb{sub 4}O{sub 7}, La{sub 2}O{sub 3}, and BaO produced primarily NO and O{sub 2}, with maxima at 640 and 670 K, respectively. TPD of bridging bidentate nitrate and monodentate nitrate on Tb{sub 4}O{sub 7}, La{sub 2}O{sub 3}, and BaO produced NO and O{sub 2} as major products and N{sub 2} and N{sub 2}O as minor products, at 320--500 K. Decomposition of bridging bidentate on MgO produced NO as a major product and N{sub 2}O as a minor product at a peak temperature of 690 K. Peak temperatures for Tb(NO{sub 3}){sub 3}, La(NO{sub 3}){sub 3}, Ba(NO{sub 3}){sub 2}, and Mg(NO{sub 3}){sub 2} decomposition occurred between those for bridging and chelating nitrates. The difference in stability between chelating and bridging bidentate nitrates on various metal oxides/{gamma}-Al{sub 2}O{sub 3} may provide a wide range of operating temperatures for NO{sub x} storage.« less

Ionic ASi{sub 2}N{sub 3} (A=Li, Na, K and Rb) stabilized by the covalent Si–N bonding: First-principles calculations

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

Zhang, Huijun; Ren, Jiadong, E-mail: jdren@ysu.edu.cn; Wu, Lailei

The structural, elastic and electronic properties of LiSi{sub 2}N{sub 3} and its substitutions by Na, K and Rb were investigated through first-principles computations. The expansion of lattice parameters of ASi{sub 2}N{sub 3} from Li, Na, K to Rb is found to be determined by the bond angle of Si–N1–Si, which suggests a possible way to improve the lithium ionic conductivity by substitutions. ASi{sub 2}N{sub 3} (A=Li, Na, K and Rb) shows the similar elastic behaviors, while the electronic band gap gradually decreases from 5.1 to 3.4 eV from LiSi{sub 2}N{sub 3} to RbSi{sub 2}N{sub 3}. Interestingly, the analysis of electronicmore » structure, crystal orbital Hamiltonian populations and Bader charges shows that the covalence of Si–N bonding is critical for the stability of ASi{sub 2}N{sub 3} phase. Among ASi{sub 2}N{sub 3} phases, there is a relatively high ionicity in NaSi{sub 2}N{sub 3}; the Si–N bond strength in [Si{sub 2}N{sub 3}]{sup −} net for KSi{sub 2}N{sub 3} and RbSi{sub 2}N{sub 3} is comparable to LiSi{sub 2}N{sub 3}, but stronger than NaSi{sub 2}N{sub 3}. - Graphic abstract: Universal trend of structural and electronic properties in alkaline metal silicon nitrides, ASi{sub 2}N{sub 3}, A=Li, Na, K and Rb. - Highlights: • Trend in structure, electronic and mechanical properties of ASi{sub 2}N{sub 3} (A=Li-Rb) were predicted. • Lattice expansion of ASi{sub 2}N{sub 3} induced by the bond angle of Si–N1–Si was found. • Calculated band gap decreases from 5.1 to 3.4 eV from LiSi{sub 2}N{sub 3} to RbSi{sub 2}N{sub 3}. • Covalent Si–N bonding is critical for the stability of ASi{sub 2}N{sub 3}.« less

Quantitative nondestructive evaluation of ceramic matrix composite by the resonance method

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

Watanabe, T.; Aizawa, T.; Kihara, J.

The resonance method was developed to make quantitative nondestructive evaluation on the mechanical properties without any troublesome procedure. Since the present method is indifferent to the geometry of specimen, both monolithic and ceramic matrix composite materials in process can be evaluated in the nondestructive manner. Al{sub 2}O{sub 3}, Si{sub 3}N{sub 4}, SiC/Si{sub 3}N{sub 4}, and various C/C composite materials are employed to demonstrate the validity and effectiveness of the present method.

Catalyst for treatment and control of post-combustion emissions

NASA Technical Reports Server (NTRS)

Upchurch, legal representative, Wilhelmina H. (Inventor); Schryer, David R. (Inventor); Upchurch, Billy T. (Inventor)

2008-01-01

The present invention utilizes two precious metals with two to five different metal-oxides in a layered matrix to convert CO, HCs, and NOx to CO.sub.2, and N.sub.2 by oxidation of two components and reduction of the other in a moderately high temperature gaseous environment containing excess oxygen.

CO{sub 2} adsorption-based separation by metal organic framework (Cu-BTC) versus zeolite (13X)

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

Zhijian Liang; Marc Marshall; Alan L. Chaffee

2009-05-15

The potential for the metal organic framework (MOF) Cu-BTC to selectively adsorb and separate CO{sub 2} is considered. Isotherms for CO{sub 2}, CH{sub 4}, and N{sub 2} were measured from 0 to 15 bar and at temperatures between 25 and 105{sup o}C. The isotherms suggest a much higher working capacity (x4) for CO{sub 2} adsorption on Cu-BTC relative to the benchmark zeolite 13X over the same pressure range. Higher CO{sub 2}/N{sub 2} and CO{sub 2}/CH{sub 4} selectivities in the higher pressure range (1-15 bar) and with lower heats of adsorption were also demonstrated. Cu-BTC was observed to be stable inmore » O{sub 2} at 25{sup o}C, but its crystallinity was reduced in humid environments. The CO{sub 2} adsorption capacity was progressively reduced upon cyclic exposure to water vapor at low relative humidity (<30%), but leveled out at 75% of its original value after several water adsorption/desorption cycles. 27 refs., 1 fig.« less

Quantitative fluid inclusion gas analysis of airburst, nuclear, impact and fulgurite glasses.

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

Parnell, John; Newsom, Horton E.; Blamey, Nigel J. F.

We present quantitative fluid inclusion gas analysis on a suite of violently-formed glasses. We used the incremental crush mass spectrometry method (Norman & Blamey, 2001) to analyze eight pieces of Libyan Desert Glass (LDG). As potential analogues we also analyzed trinitite, three impact crater glasses, and three fulgurites. The 'clear' LDG has the lowest CO{sub 2} content and O{sub 2}/Ar ratios are two orders of magnitude lower than atmospheric. The 'foamy' glass samples have heterogeneous CO{sub 2} contents and O{sub 2}/Ar ratios. N{sub 2}/Ar ratios are similar to atmospheric (83.6). H{sub 2} and He are elevated but it is difficultmore » to confirm whether they are of terrestrial or meteoritic origin. Combustion cannot account for oxygen depletion that matches the amount of CO{sub 2} produced. An alternative mechanism is required that removes oxygen without producing CO{sub 2}. Trinitite has exceedingly high CO{sub 2} which we attribute to carbonate breakdown of the caliche at ground zero. The O{sub 2}/Ar ratio for trinitite is lower than atmospheric but higher than all LDG samples. N{sub 2}/Ar ratios closely match atmospheric. Samples from Lonar, Henbury and Aouelloul impact craters have atmospheric N{sub 2}/Ar ratios. O{sub 2}/Ar ratios at Lonar and Henbury are 9.5 to 9.9 whereas the O{sub 2}/Ar ratio is 0.1 for the Aouelloul sample. In most fulgurites the N{sub 2}/Ar ratio is higher than atmospheric, possibly due to interference from CO. Oxygen ranges from 1.3 to 19.3%. Gas signatures of LDG inclusions neither match those from the craters, trinitite nor fulgurites. It is difficult to explain both the observed depletion of oxygen in the LDG and a CO{sub 2} level that is lower than it would be if the CO{sub 2} were simply a product of hydrocarbon combustion in air. One possible mechanism for oxygen depletion is that as air turbulently mixed with a hot jet of vaporized asteroid from an airburst and expanded, the atmospheric oxygen reacted with the metal vapor to form metal oxides that condensed. This observation is compatible with the model of Boslough & Crawford (2008) who suggest that an airburst incinerates organic materials over a large area, melting surface materials that then quench to form glass. Bubbles would contain a mixture of pre-existing atmosphere with combustion products from organic material and products of the reaction between vaporized cosmic materials (including metals) and terrestrial surface and atmosphere.« less

Highly-basic large-pore zeolite catalysts for NOx reduction at low temperatures

DOEpatents

Penetrante, Bernardino M.; Brusasco, Raymond M.; Merritt, Bernard T.; Vogtlin, George E.

2004-02-03

A high-surface-area (greater than 600 m2/g), large-pore (pore size diameter greater than 6.5 angstroms), basic zeolite having a structure such as an alkali metal cation-exchanged Y-zeolite is employed to convert NO.sub.x contained in an oxygen-rich engine exhaust to N.sub.2 and O.sub.2. Preferably, the invention relates to a two-stage method and apparatus for NO.sub.x reduction in an oxygen-rich engine exhaust such as diesel engine exhaust that includes a plasma oxidative stage and a selective reduction stage. The first stage employs a non-thermal plasma treatment of NO.sub.x gases in an oxygen-rich exhaust and is intended to convert NO to NO.sub.2 in the presence of O.sub.2 and added hydrocarbons. The second stage employs a lean-NO.sub.x catalyst including the basic zeolite at relatively low temperatures to convert such NO.sub.2 to environmentally benign gases that include N.sub.2, CO.sub.2, and H.sub.2 O.

Dehydration-driven evolution of topological complexity in ethylamonium uranyl selenates

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

Gurzhiy, Vladislav V., E-mail: vladgeo17@mail.ru; Krivovichev, Sergey V.; Tananaev, Ivan G.

Single crystals of four novel uranyl selenate and selenite-selenate oxysalts with protonated ethylamine molecules, (C{sub 2}H{sub 8}N){sub 2}[(UO{sub 2})(SeO{sub 4}){sub 2}(H{sub 2}O)](H{sub 2}O) (I), (C{sub 2}H{sub 8}N){sub 3}[(UO{sub 2})(SeO{sub 4}){sub 2}(HSeO{sub 4})] (II), (C{sub 2}H{sub 8}N)[(UO{sub 2})(SeO{sub 4})(HSeO{sub 3})] (III), and (C{sub 2}H{sub 8}N)(H{sub 3}O)[(UO{sub 2})(SeO{sub 4}){sub 2}(H{sub 2}O)] (IV) have been prepared by isothermal evaporation from aqueous solutions. Uranyl-containing 1D and 2D units have been investigated using topological approach and information-based complexity measurements that demonstrate the evolution of structural units and the increase of topological complexity with the decrease of H{sub 2}O content. - Graphical abstract: Single crystals ofmore » four novel uranyl selenate and selenite-selenate oxysalts with protonated ethylamine molecules have been prepared by isothermal evaporation from aqueous solutions. Structural analysis and information-based topological complexity calculations points to the possible sequence of crystalline phases formation, showing both topological and structural branches of evolution. - Highlights: • Single crystals of four novel uranyl oxysalts were prepared by evaporation method. • The graph theory was used for investigation of topologies of structural units. • Dehydration processes drives the evolution of topological complexity of 1D and 2D structural units.« less

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

Yu, Sangbae; Yoon, Daseob; Son, Junwoo, E-mail: jwson@postech.ac.kr

We report the enhancement of room-temperature electron mobility in La-doped BaSnO{sub 3} (LBSO) thin films with thermal strain induced by high temperature nitrogen (N{sub 2}) annealing. Simple annealing under an N{sub 2} environment consistently doubled the electron mobility of the LBSO films on the SrTiO{sub 3} (STO) substrates to as high as 78 cm{sup 2} V{sup −1} s{sup −1} at a carrier concentration of 4.0 × 10{sup 20 }cm{sup −3}. This enhancement is mainly attributed to annihilation of extended defects as a consequence of compressive strain induced by the difference in the thermal expansion coefficients of LBSO and STO. Our study suggests that thermalmore » strain can be exploited to reduce extended defects and to facilitate electron transport in transparent oxide semiconductors.« less

Pre-converted nitric oxide gas in catalytic reduction system

DOEpatents

Hsiao, M.C.; Merritt, B.T.; Penetrante, B.M.; Vogtlin, G.E.

1999-04-06

A two-stage catalyst comprises an oxidative first stage and a reductive second stage. The first stage is intended to convert NO to NO{sub 2} in the presence of O{sub 2}. The second stage serves to convert NO{sub 2} to environmentally benign gases that include N{sub 2}, CO{sub 2}, and H{sub 2}O. By preconverting NO to NO{sub 2} in the first stage, the efficiency of the second stage for NO{sub x} reduction is enhanced. For example, an internal combustion engine exhaust is connected by a pipe to a first chamber. An oxidizing first catalyst converts NO to NO{sub 2} in the presence of O{sub 2} and includes platinum/alumina, e.g., Pt/Al{sub 2}O{sub 3} catalyst. A flow of hydrocarbons (C{sub x}H{sub y}) is input from a pipe into a second chamber. For example, propene can be used as a source of hydrocarbons. The NO{sub 2} from the first catalyst mixes with the hydrocarbons in the second chamber. The mixture proceeds to a second reduction catalyst that converts NO{sub 2} to N{sub 2}, CO{sub 2}, and H{sub 2}O, and includes a {gamma}-Al{sub 2}O{sub 3}. The hydrocarbons and NO{sub x} are simultaneously reduced while passing through the second catalyst. 9 figs.

Study on the pulse reaction technique. VI. Kinetics of the reaction of NO with NH/sub 3/ on a V/sub 2/O/sub 5/ catalyst

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

Miyamoto, A.; Yamazaki, Y.; Hattori, T.

1982-01-01

In order to examine the applicability of the rectangular pulse technique to the determination of the kinetics of a two-components' reaction on a catalyst in the specified surface state, the kinetics of the reaction of NO with NH/sub 3/ on the V/sub 2/O/sub 5/ catalyst, that is, NO + NH/sub 3/ + VVertical BarO ..-->.. N/sub 2/ + H/sub 2/O + V-OH, has been investigated using the rectangular pulse apparatus. Chromatograms of the individual components have shown that NH/sub 3/ is strongly adsorbed on the catalyst while NO or N/sub 2/ is not or only very weakly adsorbed. The adsorptionmore » of NH/sub 3/ has been approximately described by the Langmuir adsorption isotherm. The yield of N/sub 2/ produced by the reaction has changed significantly with the pusle width. This indicates a separation of NO and NH/sub 3/ in the catalyst bed during the pulse experiments. By analyzing the experimental data with the theory of the pulse technique, the kinetics of the above-mentioned two-components' reaction has successfully been determined and it has agreed with the kinetics of the reaction of NO with NH/sub 3/ under excess oxygen conditions determined by using the continuous flow technique. On the basis of these results, the rectangular pulse technique coupled with the theoretical analsysis of the experimental data has been concluded to be a method effective for the determination of the kinetics of a multicomponents' reaction on a catalyst in the specified surface state.« less

A Chandra X-ray Study of Cygnus A. 2; The Nucleus

NASA Technical Reports Server (NTRS)

Young, Andrew J.; Wilson, Andrew; Terashima, Yuichi; Arnaud, Keith A.; Smith, David A.; White, Nicholas E. (Technical Monitor)

2002-01-01

We report Chandra Advanced CCD Imaging Spectrometer and quasi-simultaneous Rossi X-Ray Timing Explorer (RXTE) observations of the nearby, powerful radio galaxy Cygnus A, with the present paper focusing on the properties of the active nucleus. In the Chandra observation, the hard (less than a few keV) X-ray emission is spatially unresolved with a size is approximately 1" (1.5 kpc, H(sub 0) = 50 km/s/Mpc) and coincides with the radio and near-infrared nuclei. In contrast, the soft (less than 2 keV) emission exhibits a bipolar nebulosity that aligns with the optical bipolar continuum and emission-line structures and approximately with the radio jet. In particular, the soft X-ray emission corresponds very well with the [O III] (lambda)5007 and H(alpha) + [N II] lambda(lambda)6548, 6583 nebulosity imaged with Hubble Space Telescope. At the location of the nucleus, there is only weak soft X-ray emission, an effect that may be intrinsic or result from a dust lane that crosses the nucleus perpendicular to the source axis. The spectra of the various X-ray components have been obtained by simultaneous fits to the six detectors. The compact nucleus is detected to 100 keV and is well described by a heavily absorbed power-law spectrum with Gamma(sub h) = 1.52(sup + 0.12, sub -0.12) (similar to other 0.12 narrow-line radio galaxies) and equivalent hydrogen column N(sub H)(nuc) = 2.0(sup +0.1, sub -0.1) x 10(exp 23)/sq cm. This 0.2 column is compatible with the dust obscuration to the near-infrared source for a normal gas-to-dust ratio. The soft (less than 2 keV) emission from the nucleus may be described by a power-law spectrum with the same index (i.e., Gamma(sub l) = Gamma(sub h), although direct fits suggest a slightly larger value for Gamma(sub l). Narrow emission lines from highly ionized neon and silicon, as well as a "neutral" Fe K(alpha) line, are detected in the nucleus and its vicinity (r approximately less than 2 kpc). The equivalent width (EW) of the Fe K(alpha) line (182(sup +40, sub -54) eV) is in good agreement with theoretical predictions for the EW versus N(sub H)(nuc) relationship in various geometries. An Fe K edge is also seen. The RXTE observations indicate a temperature of kT = 6.9(sup +0., sub -1.0) keV for the cluster gas (discussed in Paper III of this series) and cluster emission lines of Fe K(alpha) and Fe K(beta) and/or Ni K(alpha). We consider the possibility that the extended soft X-ray emission is electron-scattered nuclear radiation. Given that 1% of the unabsorbed 2 - 10 keV nuclear radiation would have to be scattered, the necessary gas column [N(sub H)(Scattering) approx. = 3.5 x 10(exp 22)/sq cm] would absorb the X-rays rather than scatter them if the gas is cold. Thus, the scattering plasma must be highly ionized. If this ionization is achieved through photoionization by the nucleus, the ionization parameter zeta greater than 1 ergs cm/s and the electron density n(sub e) approx. = 6 cc given the observed distance of the soft X-ray emission from the nucleus. The electron column density inferred from the X-ray observations is much too low to account for the extended optical scattered light, strongly suggesting that the polarized optical light is scattered by dust. The presence of highly ionized Ne lines in the soft X-ray spectrum requires 20 ergs cm/s approximately less than zeta approximately less than 300 ergs cm/s these lines may originate closer to the nucleus than the extended soft continuum or in a lower density gas. A collisionally ionized thermal model of the extended soft X-rays cannot be ruled out but is unattractive in view of the low metal abundance required (Z = 0.03 Z(mass)). The hard X-ray to far-infrared ratio for the nucleus of Cygnus A is similar to that seen in Seyfert 1 and unobscured radio galaxies. By means of the correlation between hard X-ray luminosity and nuclear optical absolute magnitude for these classes of object, we estimate M(sub B) = -22.4 for Cygnus A, near the .borderline between Seyfert galaxies and QSOs.

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

Moradi, S.; Ganjovi, A., E-mail: Ganjovi@kgut.ac.ir; Shojaei, F.

In this work, using a two-dimensional Particle In Cell-Monte Carlo Collision simulation method, a comparative study is performed on the influences of different types of atomic and molecular gases at various background gas pressures on the generation of broadband and intense Terahertz (THz) radiation via the application of two-color laser pulses. These two modes are focused into Argon (Ar), Xenon (Xe), Nitrogen (N{sub 2}), Oxygen (O{sub 2}), and air as the background gaseous media and the plasma channel is created. It is observed that the THz radiation emission dramatically changes due to the propagation effects. A wider THz pulse ismore » emitted from the formed plasma channel at the higher gas pressures. The significant effects of the propagation features of the emitted THz pulse on its energy at the longer lengths of the plasma channel are observed.« less

Magnetic relaxation behavior of lanthanide substituted Dawson-type tungstoarsenates

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

Liu Lizhen; Li Fengyan; Xu Lin, E-mail: linxu@nenu.edu.c

2010-02-15

Two new polyoxometalate compounds [(CH{sub 3}){sub 4}N]{sub 8}[Ln(H{sub 2}O){sub 8}]{sub 2}[(alpha{sub 2}-As{sub 2}W{sub 17}O{sub 61})Ln(H{sub 2}O){sub 2}]{sub 2}.nH{sub 2}O (Ln=Er (1), Dy (2)) have been prepared by the trivacant Dawson-type anion [alpha-As{sub 2}W{sub 15}O{sub 56}]{sup 12-} and trivalent rare earth ion and characterized by single-crystal X-ray diffraction, IR spectra, thermogravimetric and electrochemical analyses. The centrosymmetric polyoxoanion, {l_brace}[(alpha{sub 2}-As{sub 2}W{sub 17}O{sub 61})Ln(H{sub 2}O){sub 2}]{sub 2}{r_brace}{sup 14-}, bounded to each other via Ln{sup 3+} connecting to terminal W-O oxygen atoms. Furthermore, the polyoxoanions are linked by [Ln(H{sub 2}O){sub 8}]{sup 3+} to form an extensive 3D supramolecular network structure depending on hydrogen bond.more » The magnetic properties of the two compounds have been studied by measuring their magnetic susceptibilities in the temperature range 2.0-300.0 K, indicating the depopulation of the stark components at low temperature and/or very weak antiferromagnetic interactions between magnetic centers. Low-temperature ac magnetic susceptibility measurements reveal a slow magnetic relaxation behavior for 2. - Graphical abstract: Two polyoxometalate compounds [(CH{sub 3}){sub 4}N]{sub 8}[Ln(H{sub 2}O){sub 8}]{sub 2}[(alpha{sub 2}-As{sub 2}W{sub 17}O{sub 61})Ln(H{sub 2}O){sub 2}]{sub 2}.nH{sub 2}O (Ln=Er (1), Dy (2)) have been prepared. The dynamic magnetic measurements for 2 display a slow relaxation of magnetization, showing a frequency-dependent susceptibility.« less

High-resolution threshold photoionization of N sub 2 O

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

Wiedmann, R.T.; Grant, E.R.; Tonkyn, R.G.

1991-07-15

Pulsed field ionization (PFI) has been used in conjunction with a coherent vuv source to obtain high-resolution threshold photoelectron spectra for the (000), (010), (020), and (100) vibrational states of the N{sub 2}O{sup +} cation. Simulations for the rotational profiles of each vibronic level were obtained by fitting the Buckingham--Orr--Sichel equations (A. D. Buckingham, B. J. Orr, and J. M. Sichel, Philos. Trans. R. Soc. London, Ser. A {bold 268}, 147 (1970)) using accurate spectroscopic constants for the ground states of the neutral and the ion. The relative branch intensities are interpreted in terms of the partial waves of themore » outgoing photoelectron to which the ionic core is coupled and in terms of the angular momentum transferred to the core. The PFI technique also allows us to report an improved value for the ionization potential of N{sub 2}O of 103 963{plus minus}5 cm{sup {minus}1}.« less

Synthesis and characterization of a 1D chain-like Cu{sub 6} substituted sandwich-type phosphotungstate with pendant dinuclear Cu–azido complexes

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

Li, Yan-Ying; Zhao, Jun-Wei, E-mail: zhaojunwei@henu.edu.cn; Wei, Qi

A novel Cu–azido complex modified hexa-Cu{sup II} substituted sandwich-type phosphotungstate [Cu(en){sub 2}]([Cu{sub 2}(en){sub 2}(μ-1,1-N{sub 3}){sub 2}(H{sub 2}O)]{sub 2}[Cu{sub 6}(en){sub 2}(H{sub 2}O){sub 2}(B-α-PW{sub 9}O{sub 34}){sub 2}])·6H{sub 2}O (1) (en=ethylene-diamine) has been prepared under hydrothermal conditions and structurally characterized by elemental analyses, IR spectra, powder X-ray diffraction (PXRD) and single-crystal X-ray diffraction. 1 displays a beautiful 1-D chain architecture constructed from sandwich-type [Cu{sub 2}(en){sub 2}(μ-1,1-N{sub 3}){sub 2}(H{sub 2}O)]{sub 2}[Cu{sub 6}(en){sub 2}(H{sub 2}O){sub 2}(B-α-PW{sub 9}O{sub 34}){sub 2}]{sup 2−} units and [Cu(en){sub 2}]{sup 2+} linkers. To our knowledge, 1 represents the first hexa-Cu{sup II} sandwiched phosphotungstate with supporting Cu–azido complexes. - Graphical abstract: Themore » first hexa-Cu{sup II} sandwiched phosphotungstate with supporting Cu–azido complexes has been prepared and characterized. Display Omitted - Highlights: • Hexa-copper-substituted phosphotungstate. • Cu–azido complexes modified hexa-Cu{sup II} substituted sandwich-type polyoxometalate. • 1-D chain architecture built by hexa-copper-substituted polyoxotungstate units.« less

PAMELA/ATIC anomaly from the meta-stable extra dark matter component and the leptophilic Yukawa interaction

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

Kyae, Bumseok, E-mail: bkyae@phya.snu.ac.kr

We present a supersymmetric model with two dark matter (DM) components explaining the galactic positron excess observed by PAMELA/HEAT and ATIC/PPB-BETS: One is the conventional (bino-like) lightest supersymmetric particle (LSP) χ, and the other is a TeV scale meta-stable neutral singlet N{sub D}, which is a Dirac fermion (N,N{sup c}). In this model, N{sub D} decays dominantly into χe{sup +}e{sup −} through an R parity preserving dimension 6 operator with the life time τ{sub N} ∼ 10{sup 26} sec. We introduce a pair of vector-like superheavy SU(2) lepton doublets (L,L{sup c}) and lepton singlets (E,E{sup c}). The dimension 6 operatormore » leading to the N{sub D} decay is generated from the leptophilic Yukawa interactions by W superset of Ne{sup c}E+Lh{sub d}E{sup c}+m{sub 3/2}l{sub 1}L{sup c} with the dimensionless couplings of order unity, and the gauge interaction by L superset of (2){sup 1/2}g' e-tilde {sup c*}e{sup c}χ+h.c. The superheavy masses of the vector-like leptons (M{sub L},M{sub E} ∼ 10{sup 16} GeV) are responsible for the longevity of N{sub D}. The low energy field spectrum in this model is just the MSSM fields and N{sub D}. Even for the case that the portion of N{sub D} is much smaller than that of χ in the total DM density [O(10{sup −10}) ∼< n{sub N{sub D}}/n{sub χ}], the observed positron excess can be explained by adopting relatively lighter masses of the vector-like leptons (10{sup 13} GeV ∼< M{sub L,E} ∼< 10{sup 16} GeV). The smallness of the electron mass is also explained. This model is easily embedded in the flipped SU(5) grand unification, which is a leptophilic unified theory.« less

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

Yahyaoui, Samia; Rekik, Walid; Laboratoire Sciences Chimiques de Rennes

The crystal structures of 1,4-diazabicyclo[2.2.2]octane (dabco)-templated iron sulfate, (C{sub 6}H{sub 14}N{sub 2})[Fe(H{sub 2}O){sub 6}](SO{sub 4}){sub 2}, were determined at room temperature and at -173 deg. C from single-crystal X-ray diffraction. At 20 deg. C, it crystallises in the monoclinic symmetry, centrosymmetric space group P2{sub 1}/n, Z=2, a=7.964(5), b=9.100(5), c=12.065(5) A, {beta}=95.426(5) deg. and V=870.5(8) A{sup 3}. The structure consists of [Fe(H{sub 2}O){sub 6}]{sup 2+} and disordered (C{sub 6}H{sub 14}N{sub 2}){sup 2+} cations and (SO{sub 4}){sup 2-} anions connected together by an extensive three-dimensional H-bond network. The title compound undergoes a reversible phase transition of the first-order at -2.3 deg. C,more » characterized by DSC, dielectric measurement and optical observations, that suggests a relaxor-ferroelectric behavior. Below the transition temperature, the compound crystallizes in the monoclinic system, non-centrosymmetric space group Cc, with eight times the volume of the ambient phase: a=15.883(3), b=36.409(7), c=13.747(3) A, {beta}=120.2304(8){sup o}, Z=16 and V=6868.7(2) A{sup 3}. The organic moiety is then fully ordered within a supramolecular structure. Thermodiffractometry and thermogravimetric analyses indicate that its decomposition proceeds through three stages giving rise to the iron oxide. - Graphical abstract: The new dabcodiium hexaaquairon(II) bis(sulfate), (C{sub 6}H{sub 14}N{sub 2})[Fe(H{sub 2}O){sub 6}](SO{sub 4}){sub 2}, was prepared and characterized. It exhibits a supramolecular structure and undergoes a reversible order-disorder phase transition at -2.3 deg. C.« less

NOx reduction by electron beam-produced nitrogen atom injection

DOEpatents

Penetrante, Bernardino M.

2002-01-01

Deactivated atomic nitrogen generated by an electron beam from a gas stream containing more than 99% N.sub.2 is injected at low temperatures into an engine exhaust to reduce NOx emissions. High NOx reduction efficiency is achieved with compact electron beam devices without use of a catalyst.

Investigation of the fabrication processes of AlGaN/AlN/GaN HEMTs with in situ Si{sub 3}N{sub 4} passivation

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

Tomosh, K. N., E-mail: sky77781@mail.ru; Pavlov, A. Yu.; Pavlov, V. Yu.

2016-10-15

The optimum mode of the in situ plasma-chemical etching of a Si{sub 3}N{sub 4} passivating layer in C{sub 3}F{sub 8}/O{sub 2} medium is chosen for the case of fabricating AlGaN/AlN/GaN HEMTs. It is found that a bias of 40–50 V at a high-frequency electrode provides anisotropic etching of the insulator through a resist mask and introduces no appreciable radiation-induced defects upon overetching of the insulator films in the region of gate-metallization formation. To estimate the effect of in situ Si{sub 3}N{sub 4} growth together with the heterostructure in one process on the AlGaN/AlN/GaN HEMT characteristics, transistors with gates without themore » insulator and with gates through Si{sub 3}N{sub 4} slits are fabricated. The highest drain current of the AlGaN/AlN/GaN HEMT at 0 V at the gate is shown to be 1.5 times higher in the presence of Si{sub 3}N{sub 4} than without it.« less

Abatement of SF{sub 6} and CF{sub 4} using an enhanced kerosene microwave plasma burner

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

Shin, Dong Hun; Hong, Yong Cheol; Cho, Soon Cheon

2006-11-15

A kerosene microwave plasma burner was presented as a tool for abatement of SF{sub 6} and CF{sub 4} gases, which cause global warming. The plasma burner operates by injecting kerosene as a liquid hydrocarbon fuel into a microwave plasma torch and by mixing the resultant gaseous hydrogen and carbon compounds with air or oxygen (O{sub 2}) gas. The abatement of SF{sub 6} and CF{sub 4}, by making use of the kerosene plasma burner, was conducted in terms of nitrogen (N{sub 2}) flow rates. The destruction and removal efficiency of the burner were achieved up to 99.9999% for 0.1 liters permore » minute (lpm) SF{sub 6} in 120 lpm N{sub 2} and 99.3% for 0.05 lpm CF{sub 4} in 60 lpm N{sub 2}, revealing that the microwave plasma burner can effectively eliminate perfluorocompounds emitted from the semiconductor industries.« less

Determination of hydrogen/deuterium ratio with neutron measurements on MAST

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

Klimek, I., E-mail: iwona.klimek@physics.uu.se; Cecconello, M.; Ericsson, G.

2014-11-15

On MAST, compressional Alfvén eigenmodes can be destabilized by the presence of a sufficiently large population of energetic particles in the plasma. This dependence was studied in a series of very similar discharges in which increasing amounts of hydrogen were puffed into a deuterium plasma. A simple method to estimate the isotopic ratio n{sub H}/n{sub D} using neutron emission measurements is here described. The inferred isotopic ratio ranged from 0.0 to 0.6 and no experimental indication of changes in radial profile of n{sub H}/n{sub D} were observed. These findings are confirmed by TRANSP/NUBEAM simulations of the neutron emission.

EXTENDED X-RAY EMISSION IN THE VICINITY OF THE MICROQUASAR LS 5039: PULSAR WIND NEBULA?

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

Durant, Martin; Kargaltsev, Oleg; Pavlov, George G.

2011-07-01

LS 5039 is a high-mass binary with a period of 4 days, containing a compact object and an O-star, one of the few high-mass binaries detected in {gamma}-rays. Our Chandra Advanced CCD Imaging Spectrometer observation of LS 5039 provided a high-significance ({approx}10{sigma}) detection of extended emission clearly visible for up to 1' from the point source. The spectrum of this emission can be described by an absorbed power-law model with photon index {Gamma} = 1.9 {+-} 0.3, somewhat softer than the point-source spectrum {Gamma} = 1.44 {+-} 0.07, with the same absorption, N{sub H} = (6.4 {+-} 0.6) x 10{supmore » 21} cm{sup -2}. The observed 0.5-8 keV flux of the extended emission is {approx_equal} 8.8 x 10{sup -14} erg s{sup -1}cm{sup -2} or 5% of the point-source flux; the latter is a factor of {approx}2 lower than the lowest flux detected so far. Fainter extended emission with comparable flux and a softer ({Gamma} {approx} 3) spectrum is detected at even greater radii (up to 2'). Two possible interpretations of the extended emission are a dust scattering halo and a synchrotron nebula powered by energetic particles escaping the binary. We discuss both of these scenarios and favor the nebula interpretation, although some dust contribution is possible. We have also found transient sources located within a narrow stripe south of LS 5039. We discuss the likelihood of these sources to be related to LS 5039.« less

Self assembled monolayers of octadecyltrichlorosilane for dielectric materials

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

Kumar, Vijay, E-mail: cirivijaypilani@gmail.com; Mechanical Engineering Department, Birla Institute of Technology and Science-Pilani; Puri, Paridhi

2016-04-13

Treatment of surfaces to change the interaction of fluids with them is a critical step in constructing useful microfluidics devices, especially those used in biological applications. Selective modification of inorganic materials such as Si, SiO{sub 2} and Si{sub 3}N{sub 4} is of great interest in research and technology. We evaluated the chemical formation of OTS self-assembled monolayers on silicon substrates with different dielectric materials. Our investigations were focused on surface modification of formerly used common dielectric materials SiO{sub 2}, Si{sub 3}N{sub 4} and a-poly. The improvement of wetting behaviour and quality of monolayer films were characterized using Atomic force microscope,more » Scanning electron microscope, Contact angle goniometer, Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) monolayer deposited oxide surface.« less

Solubility and diffusivity of nitrous oxide in ternary mixtures of water, monoethanolamine, and N-methyldiethanolamine and solution densities and viscosities

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

Hagewiesche, D.P.; Ashour, S.S.; Sandall, O.C.

1995-05-01

Recently, several researchers have suggested using aqueous mixtures of small amounts of monoethanolamine and much larger amounts of N-methyldiethanolamine for the absorption of CO{sub 2} and for the selective removal of H{sub 2}S from gas streams of mixtures of CO{sub 2} and H{sub 2}S. The densities and viscosities of aqueous N-methyldiethanolamine/monoethanolamine (MDEA/MEA) blends containing 30 and 40 mass % total amine with MEA concentrations of 5, 10, and 15 mass % of the total amine concentration were measured at temperatures of 303, 313, and 323 K. The diffusion coefficients and Henry`s law constants of N{sub 2}O in these solutions weremore » also measured and were used to estimate the diffusion coefficients and Henry`s law constants of CO{sub 2} in these solutions according to the N{sub 2}O/CO{sub 2} analogy technique.« less

Bradykinin-activated transmembrane signals are coupled via N/sub o/ or N/sub i/ to production of inositol 1,4,5-trisphosphate, a second messenger in NG108-15 neuroblastoma-glioma hybrid cells

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

Higashida, H.; Streaty, R.A.; Klee, W.

1986-02-01

The addition of bradykinin to NG108-15 cells results in a transient hyperpolarization followed by prolonged cell depolarization. Injection of inositol 1,4,5-trisphosphate or CaS into the cytoplasm of NG108-15 cells also elicits cell hyperpolarization followed by depolarization. Tetraethylammonium ions inhibit the hyperpolarizing response of cells to bradykinin or inositol 1,4,5-trisphosphate. Thus, the hyperpolarizing phase of the cell response may be due to inositol 1,4,5-trisphosphate-dependent release of stored UVCa-labelled CaS into the cytoplasm, which activates CaS -dependent K channels. The depolarizing phase of the cell response to bradykinin is due largely to inhibition of M channels, thereby decreasing the rate of Kmore » efflux from cells and, to a lesser extent, to activation of CaS -dependent ion channels and CaS channels. In contrast, injection of inositol 1,4,5-trisphosphate or CaS into the cytosol did not alter M channel activity. Incubation of NG108-15 cells with pertussis toxin inhibits bradykinin-dependent cell hyperpolarization and depolarization. Bradykinin stimulates low K/sub m/ GTPase activity and inhibits adenylate cyclase in NG108-15 membrane preparations but not in membranes prepared from cells treated with pertussis toxin. These results show that (bradykinin-receptor) complexes interact with N/sub o/ or N/sub i/ and suggest that N/sub o/ and/or N/sub i/ mediate the transduction of signals from bradykinin receptors to phospholipase C and adenylate cyclase.« less

Lifetime-vibrational interference effects in resonantly excited x-ray emission spectra of CO

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

Skytt, P.; Glans, P.; Gunnelin, K.

1997-04-01

The parity selection rule for resonant X-ray emission as demonstrated for O{sub 2} and N{sub 2} can be seen as an effect of interference between coherently excited degenerate localized core states. One system where the core state degeneracy is not exact but somewhat lifted was previously studied at ALS, namely the resonant X-ray emission of amino-substituted benzene (aniline). It was shown that the X-ray fluorescence spectrum resulting from excitation of the C1s at the site of the {open_quotes}aminocarbon{close_quotes} could be described in a picture separating the excitation and the emission processes, whereas the spectrum corresponding to the quasi-degenerate carbons couldmore » not. Thus, in this case it was necessary to take interference effects between the quasi-degenerate intermediate core excited states into account in order to obtain agreement between calculations and experiment. The different vibrational levels of core excited states in molecules have energy splittings which are of the same order of magnitude as the natural lifetime broadening of core excitations in the soft X-ray range. Therefore, lifetime-vibrational interference effects are likely to appear and influence the band shapes in resonant X-ray emission spectra. Lifetime-vibrational interference has been studied in non-resonant X-ray emission, and in Auger spectra. In this report the authors discuss results of selectively excited soft X-ray fluorescence spectra of molecules, where they focus on lifetime-interference effects appearing in the band shapes.« less

NUMERICAL CONVERGENCE IN SMOOTHED PARTICLE HYDRODYNAMICS

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

Zhu, Qirong; Li, Yuexing; Hernquist, Lars

2015-02-10

We study the convergence properties of smoothed particle hydrodynamics (SPH) using numerical tests and simple analytic considerations. Our analysis shows that formal numerical convergence is possible in SPH only in the joint limit N → ∞, h → 0, and N{sub nb} → ∞, where N is the total number of particles, h is the smoothing length, and N{sub nb} is the number of neighbor particles within the smoothing volume used to compute smoothed estimates. Previous work has generally assumed that the conditions N → ∞ and h → 0 are sufficient to achieve convergence, while holding N{sub nb} fixed.more » We demonstrate that if N{sub nb} is held fixed as the resolution is increased, there will be a residual source of error that does not vanish as N → ∞ and h → 0. Formal numerical convergence in SPH is possible only if N{sub nb} is increased systematically as the resolution is improved. Using analytic arguments, we derive an optimal compromise scaling for N{sub nb} by requiring that this source of error balance that present in the smoothing procedure. For typical choices of the smoothing kernel, we find N{sub nb} ∝N {sup 0.5}. This means that if SPH is to be used as a numerically convergent method, the required computational cost does not scale with particle number as O(N), but rather as O(N {sup 1} {sup +} {sup δ}), where δ ≈ 0.5, with a weak dependence on the form of the smoothing kernel.« less

Molybdenum disilicide composites

DOEpatents

Rodriguez, Robert P.; Petrovic, John J.

2001-01-01

Molybdenum disilicide/.beta.'-Si.sub.6-z Al.sub.z O.sub.z N.sub.8-z, wherein z=a number from greater than 0 to about 5, composites are made by use of in situ reactions among .alpha.-silicon nitride, molybdenum disilicide, and aluminum. Molybdenum disilicide within a molybdenum disilicide/.beta.'-Si.sub.6-z Al.sub.z O.sub.z N.sub.8-z eutectoid matrix is the resulting microstructure when the invention method is employed.

Anion-induced structural transformation of a sulfate-incorporated 2D Cd(II)–organic framework

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

Lee, Li-Wei; Institute of Materials Science and Engineering, National Central University, Taoyuan 320, Taiwan; Luo, Tzuoo-Tsair

2016-07-15

A Cd(II)–organic framework {[Cd_2(tpim)_4(SO_4)(H_2O)_2]·(SO_4)·21H_2O}{sub n} (1) was synthesized by reacting CdSO{sub 4}·8/3H{sub 2}O and 2,4,5-tri(4-pyridyl)imidazole (tpim) under hydrothermal conditions. A structural analysis showed that compound 1 adopts a layered structure in which the [Cd(tpim){sub 2}]{sub n} chains are linked by sulfate anions. These 2D layers are further packed into a 3D supramolecular framework via π–π interactions. The structure contains two types of SO{sub 4}{sup 2−} anions, i.e., bridging SO{sub 4}{sup 2−} and free SO{sub 4}{sup 2−} anions, the latter of which are included in the large channels of the framework. Compound 1 exhibits interesting anion exchange behavior. In the presencemore » of SCN{sup −} anions, both the bridging and free SO{sub 4}{sup 2−} anions in 1 were completely exchanged by SCN{sup −} ligands to form a 1D species [Cd(tpim){sub 2}(SCN){sub 2}] (1A), in which the SCN{sup –} moieties function as a monodentate ligand. On the other hand, when compound 1 was ion exchanged with N{sub 3}{sup −} anions in aqueous solution, the bridging SO{sub 4}{sup 2−} moieties remained intact, and only the free guest SO{sub 4}{sup 2−} were replaced by N{sub 3}{sup −} anions. The gas adsorption behavior of the activated compound 1 was also investigated. - Highlights: • An interesting anion-induced structural transformation of a sulfate-incorporated 2D Cd(II)–organic framework is reported. • The sulfate-incorporated 2D layer compound exhibits very different anion exchange behavior with respect to SCN{sup −} and N{sub 3}{sup −}. • Both the bridging and free SO{sub 4}{sup 2−} anions in the 2D structure were completely exchanged by SCN{sup −} ligands, resulting in the formation of a 1D species. However, in the case of N{sub 3}{sup −} anions, only the free guest SO{sub 4}{sup 2−} in the structure was replaced.« less

NuSTAR SPECTROSCOPY OF MULTI-COMPONENT X-RAY REFLECTION FROM NGC 1068

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

Bauer, Franz E.; Arévalo, Patricia; Walton, Dominic J.

2015-10-20

We report on high-energy X-ray observations of the Compton-thick Seyfert 2 galaxy NGC 1068 with NuSTAR, which provide the best constraints to date on its >10 keV spectral shape. The NuSTAR data are consistent with those from past and current instruments to within cross-calibration uncertainties, and we find no strong continuum or line variability over the past two decades, which is in line with its X-ray classification as a reflection-dominated Compton-thick active galactic nucleus. The combined NuSTAR, Chandra, XMM-Newton, and Swift BAT spectral data set offers new insights into the complex secondary emission seen instead of the completely obscured transmittedmore » nuclear continuum. The critical combination of the high signal-to-noise NuSTAR data and the decomposition of the nuclear and extranuclear emission with Chandra allow us to break several model degeneracies and greatly aid physical interpretation. When modeled as a monolithic (i.e., a single N{sub H}) reflector, none of the common Compton reflection models are able to match the neutral fluorescence lines and broad spectral shape of the Compton reflection hump without requiring unrealistic physical parameters (e.g., large Fe overabundances, inconsistent viewing angles, or poor fits to the spatially resolved spectra). A multi-component reflector with three distinct column densities (e.g., with best-fit values of N{sub H} of 1.4 × 10{sup 23}, 5.0 × 10{sup 24}, and 10{sup 25} cm{sup −2}) provides a more reasonable fit to the spectral lines and Compton hump, with near-solar Fe abundances. In this model, the higher N{sub H} component provides the bulk of the flux to the Compton hump, while the lower N{sub H} component produces much of the line emission, effectively decoupling two key features of Compton reflection. We find that ≈30% of the neutral Fe Kα line flux arises from >2″ (≈140 pc) and is clearly extended, implying that a significant fraction (and perhaps most) of the <10 keV reflected component arises from regions well outside a parsec-scale torus. These results likely have ramifications for the interpretation of Compton-thick spectra from observations with poorer signal-to-noise and/or more distant objects.« less

An Archival Chandra and XMM-Newton Survey of Type 2 Quasars

NASA Technical Reports Server (NTRS)

Jia, Jianjun; Ptak, Andrew Francis; Heckman, Timothy; Zakamska, Nadia L.

2013-01-01

In order to investigate obscuration in high-luminosity type 2 active galactic nuclei (AGNs), we analyzed Chandra and XMM-Newton archival observations for 71 type 2 quasars detected at 0.05 < z < 0.73, which were selected based on their [O III] lambda5007 emission lines. For 54 objects with good spectral fits, the observed hard X-ray luminosity ranges from 2 × 10(exp 41) to 5.3 × 10(exp 44) erg s(exp -1), with a median of 1.1 × 10(exp 43) erg s(exp -1). We find that the means of the column density and photon index of our sample are log N(sub H) = 22.9 cm(exp -2) and gamma = 1.87, respectively. From simulations using a more physically realistic model, we find that the absorbing column density estimates based on simple power-law models significantly underestimate the actual absorption in approximately half of the sources. Eleven sources show a prominent Fe K alpha emission line (EW>100 eV in the rest frame) and we detect this line in the other sources through a joint fit (spectral stacking). The correlation between the Fe K alpha and [O III] fluxes and the inverse correlation of the equivalent width of the Fe Ka line with the ratio of hard X-ray and [O III] fluxes is consistent with previous results for lower luminosity Seyfert 2 galaxies. We conclude that obscuration is the cause of the weak hard X-ray emission rather than intrinsically low X-ray luminosities. We find that about half of the population of optically selected type 2 quasars are likely to be Compton thick. We also find no evidence that the amount of X-ray obscuration depends on the AGN luminosity (over a range of more than three orders of magnitude in luminosity).

FT-IR remote sensing of atmospheric species: Application to global change and air pollution

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

Vazquez, G.J.

1995-12-31

In this contribution, the author describes two applications of Fourier Transform Infrared Spectroscopy to the monitoring of atmospheric compounds. Firstly, the author reports FTIR solar spectroscopy measurements carried out at ground level at NCAR and on airplanes employing a spectrometer of 0.06 cm{sup -1} resolution. Sample atmospheric spectra and fitting examples are presented for key species relevant to stratospheric chemistry and global change: ozone (O{sub 3}), a chlorofluorocarbon (CF{sub 2}Cl{sub 2}), a greenhouse gas (N{sub 2}O), HCl, NO and HNO{sub 3}. Secondly, the author briefly describes urban air pollution measurements at an intersection with heavy traffic in Tucson, AZ. Twomore » FTIR spectrometers of 1 cm{sup -1} resolution were employed to carry out long-path open-path measurements of the CO/CO{sub 2} ratio and SF{sub 6}. Two FEAT and two LPUV instruments were employed for ancillary measurements of CO, CO{sub 2}, NO, and aromatic hydrocarbons. Measurements of CO at two heights and a comparison of CO/CO{sub 2} ratios obtained by FEAT exhaust emission and FTIR ambient air measurements are reported.« less

Atomic layer deposition of tin oxide and zinc tin oxide using tetraethyltin and ozone

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

Warner, Ellis J.; Gladfelter, Wayne L., E-mail: wlg@umn.edu; Johnson, Forrest

Silicon or glass substrates exposed to sequential pulses of tetraethyltin (TET) and ozone (O{sub 3}) were coated with thin films of SnO{sub 2}. Self-limiting deposition was found using 8 s pulse times, and a uniform thickness per cycle (TPC) of 0.2 nm/cycle was observed in a small, yet reproducible, temperature window from 290 to 320 °C. The as-deposited, stoichiometric SnO{sub 2} films were amorphous and transparent above 400 nm. Interspersing pulses of diethylzinc and O{sub 3} among the TET:O{sub 3} pulses resulted in deposition of zinc tin oxide films, where the fraction of tin, defined as [at. % Sn/(at. % Sn + at. %more » Zn)], was controlled by the ratio of TET pulses, specifically n{sub TET}:(n{sub TET} + n{sub DEZ}) where n{sub TET} and n{sub DEZ} are the number of precursor/O{sub 3} subcycles within each atomic layer deposition (ALD) supercycle. Based on film thickness and composition measurements, the TET pulse time required to reach saturation in the TPC of SnO{sub 2} on ZnO surfaces was increased to >30 s. Under these conditions, film stoichiometry as a function of the TET pulse ratio was consistent with the model devised by Elliott and Nilsen. The as-deposited zinc tin oxide (ZTO) films were amorphous and remained so even after annealing at 450 °C in air for 1 h. The optical bandgap of the transparent ZTO films increased as the tin concentration increased. Hall measurements established that the n-type ZTO carrier concentration was 3 × 10{sup 17} and 4 × 10{sup 18} cm{sup −3} for fractional tin concentrations of 0.28 and 0.63, respectively. The carrier mobility decreased as the concentration of tin increased. A broken gap pn junction was fabricated using ALD-deposited ZTO and a sputtered layer of cuprous oxide. The junction demonstrated ohmic behavior and low resistance consistent with similar junctions prepared using sputter-deposited ZTO.« less

The effect of Cu/Zn molar ratio on CO{sub 2} hydrogenation over Cu/ZnO/ZrO{sub 2}/Al{sub 2}O{sub 3} catalyst

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

Shaharun, Salina, E-mail: salinashaharun@gmail.com, E-mail: maizats@petronas.com.my; Shaharun, Maizatul S., E-mail: salinashaharun@gmail.com, E-mail: maizats@petronas.com.my; Taha, Mohd F., E-mail: faisalt@petronas.com.my

2014-10-24

Catalytic hydrogenation of carbon dioxide (CO{sub 2}) to methanol is an attractive way to recycle and utilize CO{sub 2}. A series of Cu/ZnO/Al{sub 2}O{sub 3}/ZrO{sub 2} catalysts (CZAZ) containing different molar ratios of Cu/Zn were prepared by the co-precipitation method and investigated in a stirred slurry autoclave system. The catalysts were characterized by temperature-programmed reduction (TPR), field emission scanning electron microscopy-energy dispersive analysis (FESEM-EDX), X-ray diffraction (XRD) and N{sub 2} adsorption-desorption. Higher surface area, SA{sub BET} values (42.6–59.9 m{sup 2}/g) are recorded at low (1) and high (5) Cu/Zn ratios with the minimum value of 35.71 m{sup 2}/g found formore » a Cu/Zn of 3. The reducibility of the metal oxides formed after calcination of catalyst samples was also affected due to change in metal-support interaction. At a low reaction temperature of 443 K, total gas pressure of 3.0 MPa and 0.1 g/mL of the CZAZ catalyst, the selectivity to methanol decreased as the Cu/Zn molar ratio increased, and the maximum selectivity of 67.73 was achieved at Cu/Zn molar ratio of 1. With a reaction time of 3h, the best performing catalyst was CZAZ75 with Cu/Zn molar ratio of 5 giving methanol yield of 79.30%.« less

A novel organic–inorganic hybrid with Anderson type polyanions as building blocks: (C{sub 6}H{sub 10}N{sub 3}O{sub 2}){sub 2}Na(H{sub 2}O){sub 2}[Al(OH){sub 6}Mo{sub 6}O{sub 18}]·6H{sub 2}O

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

Thabet, Safa, E-mail: safathabet@hotmail.fr; Ayed, Brahim, E-mail: brahimayed@yahoo.fr; Haddad, Amor

Graphical abstract: Display Omitted Highlights: ► Synthesis of a novel inorganic–organic hybrid compound based on Anderson polyoxomolybdates. ► Characterization by X-ray diffraction, IR and UV–Vis spectroscopies of the new compound. ► Potential applications in catalysis, biochemical analysis and electrical conductivity of the organic–inorganic compound. -- Abstract: A new organic–inorganic hybrid compound based on Anderson polyoxomolybdates, (C{sub 6}H{sub 10}N{sub 3}O{sub 2}){sub 2}Na(H{sub 2}O){sub 2}[Al(OH){sub 6}Mo{sub 6}O{sub 18}]·6H{sub 2}O (1) have been isolated by the conventional solution method and characterized by single-crystal X-ray diffraction, infrared, ultraviolet spectroscopy and Thermogravimetric Analysis (TGA). This compound crystallized in the triclinic system, space group P−1, withmore » a = 94.635(1) Å, b = 10.958(1) Å, c = 11.602(1) Å, α = 67.525(1)°, β = 71.049(1)°, γ = 70.124(1)° and Z = 1. The crystal structures of the compounds exhibit three-dimensional supramolecular assembly based on the extensive hydrogen bonding interactions between organic cations, sodium cations, water molecules and Anderson polyoxoanions. The infrared spectrum fully confirms the X-ray crystal structure and the UV spectrum of the title compound exhibits an absorption peak at 210 nm.« less

Novel designs of fluidized bed combustors for low pollutant emissions

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

Lin, W.; Bleek, C.M. van den; Dam-Johansen, K.

1995-12-31

It is known that NH{sub 3}, released during the devolatilization of fuel, is an important precursor for NO formation in fluidized bed combustors. On the other hand, NH{sub 3} may be used as a reducing agent in the thermal DeNO{sub x} process to reduce NO{sub x} emission levels. In this paper, a new concept of fluidized bed combustors is proposed based on the idea of in situ reduction of NO{sub x} by self-produced NH{sub 3} from fuel without lowering the sulfur capture level. This design is intended to separate the NH{sub 3} release process under reducing conditions from the charmore » combustion process under oxidizing conditions; this self-released NH{sub 3}, together with some combustibles, is mixed with gaseous combustion products in the upper part of the combustor for a further reduction of the NO{sub x} formed during combustion. Furthermore, the combustion of the combustibles may cause the temperature to rise in this upper zone and thereby reduce the emission of N{sub 2}O. The applications of this design to bubbling and circulating fluidized bed combustors are described and the mechanisms of the main reactions involved discussed.« less

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

Kulkarni, Varsha P.; Som, Debopam; Morrison, Sean

We report Keck/Echellette Spectrograph and Imager and Very Large Telescope/Ultraviolet-Visual Echelle Spectrograph observations of three super-damped Lyα quasar absorbers with H i column densities log N{sub H} {sub i} ≥ 21.7 at redshifts 2 ≲ z ≲ 2.5. All three absorbers show similar metallicities (∼−1.3 to −1.5 dex), and dust depletion of Fe, Ni, and Mn. Two of the absorbers show supersolar [S/Zn] and [Si/Zn]. We combine our results with those for other damped Lyα a absorbers (DLAs) to examine trends between N{sub H} {sub i}, metallicity, and dust depletion. A larger fraction of the super-DLAs lie close to ormore » above the line [X/H] = 20.59 − log N{sub H} {sub i} in the metallicity versus N{sub H} {sub i} plot, compared to the less gas-rich DLAs, suggesting that super-DLAs are more likely to be rich in molecules. Unfortunately, our data for Q0230−0334 and Q0743+1421 do not cover H{sub 2} absorption lines. For Q1418+0718, some H{sub 2} lines are covered, but not detected. CO is not detected in any of our absorbers. For DLAs with log N{sub H} {sub i} < 21.7, we confirm strong correlation between metallicity and Fe depletion, and find a correlation between metallicity and Si depletion. For super-DLAs, these correlations are weaker or absent. The absorbers toward Q0230−0334 and Q1418+0718 show potential detections of weak Lyα emission, implying star formation rates of ∼1.6 and ∼0.7 M{sub ⊙} yr{sup −1}, respectively (ignoring dust extinction). Upper limits on the electron densities from C ii*/C ii or Si ii*/Si ii are low, but are higher than the median values in less gas-rich DLAs. Finally, systems with log N{sub H} {sub i} > 21.7 may have somewhat narrower velocity dispersions Δv{sub 90} than the less gas-rich DLAs, and may arise in cooler and/or less turbulent gas.« less

On the surface chemistry of molybdena-alumina catalysts prepared from Mo(CO) sub 6

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

Goldwasser, J.; Fang, S.M.; Houalla, M.

1989-01-01

Catalysts were prepared by subliming Mo(CO){sub 6} onto partially dehydroxylated (PDA) and exhaustively dehydroxylated (DA) alumina made from the same parent preparation (American Cyanamid Aero 100PHF). The chemisorption of NO and Co on these materials was studied using volumetric, chromatographic, and spectroscopic techniques. ESCA data indicated that metallic Mo crystals formed on Mo(CO){sub 6}/DA whereas on PDA both Mo{sup 4+} and some lower valence state, Mo{sup 2+} or Mo{sup 0}, were present. NO chemisorbed on both preparations at 195 K without releasing either N{sub 2}O or N{sub 2}. The chemisorption on the PDA preparations was over tenfold higher than thatmore » on the DA-supported catalysts under these conditions, but at 300 K the difference was reduced to a factor of 2. Moreover, redox chemistry occurred at this higher temperature as evidenced by the release of N{sub 2}O and N{sub 2}. The amounts of NO actually chemisorbed correlated well with the integrated IR band intensities. These data suggest that lower valence states are oxidized to Mo{sup 4+} at 300 K and that the observed IR bands stem from Mo{sup 4+}(NO){sub 2}, irrespective of the initial catalyst. Infrared spectra from residual CO remaining on decomposition of Mo(CO){sub 6} on DA and PDA showed bands which could be attributed to residual Mo(CO){sub 6} and/or to subcarbonyl species formed during decomposition. By 573 K, no residual bands could be observed. On adding-back CO at 300 K to the PDA preparation, bands at 1989 and 2170 cm{sup {minus}1} appeared, suggesting the presence of Mo{sup 4+} and residual Mo{sup 0}. Spectra from similar experiments with the DA preparation demonstrated that chemisorbed Mo(CO){sub 6} was reforming and possibly some subcarbonyl species.« less

Active nitrogen partitioning and the nighttime formation of N sub 2 O sub 5 in the stratosphere: Simultaneous in situ measurements of NO, NO sub 2 , HNO sub 3 , O sub 3 , and N sub 2 O using the BLISS diode laser spectrometer

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

Webster, C.R.; May, R.D.; Toumi, R.

1990-08-20

Simultaneous in situ measurements of NO, NO{sub 2}, HNO{sub 3}, O{sub 3}, N{sub 2}O, pressure, and temperature at 30 km have been made from Palestine. Texas (32{degree}N) on September 13, 1988, using the Jet Propulsion Laboratory Balloon-Borne Laser In-Situ Sensor (BLISS) instrument, with the NOAA dual-channel balloon UV ozone spectrometer on the same gondola. Using tunable diode laser absorption spectroscopy over a long path length, measurements were made during a 24-hour flight of the daytime concentrations of NO, NO{sub 2}, and O{sub 3} and of the diurnal variation in the concentration of NO{sub 2}. Postsunset measurements of NO{sub 2}, mademore » every half minutes throughout much of the night, show the NO{sub 2} mixing ratio falling from a sunset value of 10.5 ppbv to 5.2 ppbv at nights end. From the sunset/sunrise difference din the volume mixing ratio of NO{sub 2} is derived a value of 2.7 {plus minus} 0.4 ppbv for the sunrise N{sub 2}O{sub 5} mixing ratio, in excellent agreement with the model predictions of 2.9 ppbv at this latitude. The measured daytime NO{sub 2}/NO ratio was found to be in good agreement with model predictions at 30 km. The measured presunset sum NO + NO{sub 2} of 10.1 {plus minus} 0.8 ppbv agreed well with the measured postsunset NO{sub 2} amount of 10.5 {plus minus} 0.8 ppbv. Simultaneous measurements of the mixing ratios of HNO{sub 3} and postsunset NO{sub 2} allow an estimate of total reactive nitrogen, approximated at this time by NO{sub 2} + HNO{sub 3} + 2(N{sub 2}O{sub 5}) + ClONO{sub 2}, of 16.4 {plus minus} 1.2 ppbv at 30 km, and (from an earlier flight) of 13.7 {plus minus} 1.7 ppbv at 37 km. Using model predictions incorporating corrections for non-steady state and for diurnal chemistry, an OH mixing ratio of 8 {plus minus} 4 pptv is derived from the measured HNO{sub 3}/NO{sub 2} ratio of 0.72 {plus minus} 0.17 at 30 km.« less

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

Iwamoto, Y.; Shin, S.G.; Matsubara, H.

The grain growth behavior of ceramic materials under the existence of a liquid phase was investigated for Si{sub 3}N{sub 4}-Y{sub 2}O{sub 3}-SiO{sub 2}, TiC-Ni, and WC-Co systems. The kinetics of grain growth behavior of these systems closely fitted to the cubic relation of d{sup 3} - d{sub 0}{sup 3} = Kt. The growth rate of {beta}-Si{sub 3}N{sub 4} grain was approximately one order of magnitude larger in length direction than that in width direction. The growth rate slightly increased with increasing liquid phase content in both these directions of the {beta}-Si{sub 3}N{sub 4} grain. TiC-Ni and WC-Co cermets had amore » peak in growth rate at a certain liquid phase content. The rate constant values of these systems were much smaller by a factor of 10{sup 3}{approximately}10{sup 5} compared to the theoretical values expected from the diffusion-controlled growth model. The experimental growth rates tended to decrease with increasing contiguity of the solid phase. The grain growth behavior of these systems could be explained by the mechanism resulting from the existence of contiguous boundaries of solid phase, which suppressed the movement of solid/liquid interfaces during liquid phase sintering.« less

Erosion behavior of composite Al-Cr cathodes in cathodic arc plasmas in inert and reactive atmospheres

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

Franz, Robert, E-mail: robert.franz@unileoben.ac.at; Mendez Martin, Francisca; Hawranek, Gerhard

2016-03-15

Al{sub x}Cr{sub 1−x} composite cathodes with Al contents of x = 0.75, 0.5, and 0.25 were exposed to cathodic arc plasmas in Ar, N{sub 2}, and O{sub 2} atmospheres and their erosion behavior was studied. Cross-sectional analysis of the elemental distribution of the near-surface zone in the cathodes by scanning electron microscopy revealed the formation of a modified layer for all cathodes and atmospheres. Due to intermixing of Al and Cr in the heat-affected zone, intermetallic Al-Cr phases formed as evidenced by x-ray diffraction analysis. Cathode poisoning effects in the reactive N{sub 2} and O{sub 2} atmospheres were nonuniform as a resultmore » of the applied magnetic field configuration. With the exception of oxide islands on Al-rich cathodes, reactive layers were absent in the circular erosion zone, while nitrides and oxides formed in the less eroded center region of the cathodes.« less

STAR FORMATION AND FEEDBACK: A MOLECULAR OUTFLOW–PRESTELLAR CORE INTERACTION IN L1689N

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

Lis, D. C.; Pagani, L.; Wootten, H. A.

2016-08-20

We present Herschel ,{sup 11} ALMA Compact Array (ACA), and Caltech Submillimeter Observatory observations of the prestellar core in L1689N, which has been suggested to be interacting with a molecular outflow driven by the nearby solar-type protostar IRAS 16293-2422. This source is characterized by some of the highest deuteration levels observed in the interstellar medium. The change in the NH{sub 2}D line velocity and width across the core provides clear evidence of an interaction with the outflow, traced by the high-velocity water emission. Quiescent, cold gas characterized by narrow line widths is seen in the NE part of the core,more » while broader, more disturbed line profiles are seen in the W/SW part. Strong N{sub 2}D{sup +} and ND{sub 3} emission is detected with ACA extending S/SW from the peak of the single-dish NH{sub 2}D emission. The ACA data also reveal the presence a compact dust continuum source with a mean size of ∼1100 au, a central density of (1–2) × 10{sup 7} cm{sup −3}, and a mass of 0.2–0.4 M {sub ⊙}. The dust emission peak is displaced ∼5″ to the south with respect to the N{sub 2}D{sup +} and ND{sub 3} emission, as well as the single-dish dust continuum peak, suggesting that the northern, quiescent part of the core is characterized by spatially extended continuum emission, which is resolved out by the interferometer. We see no clear evidence of fragmentation in this quiescent part of the core, which could lead to a second generation of star formation, although a weak dust continuum source is detected in this region in the ACA data.« less

X-ray mapping in heterocyclic design: 18. X-ray diffraction study of a series of derivatives of 3-cyanopyridine-2-one with annelated heptane and octane cycles

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

Rybakov, V. B., E-mail: Rybakov20021@yandex.ru; Babaev, E. V.; Paronikyan, E. G., E-mail: Ervand.paronikyan@mail.ru

Seven new, previously unknown, bicyclic and tricyclic heterocycles based on derivatives of 3-cyanopyrid-2-ones are obtained: 2-oxo-2,5,6,7,8,9-hexahydro-1H-cyclohepta[b]pyridine-3-carbonitrile, C{sub 11}H{sub 12}N{sub 2}O (1a); 2-[2-(4-chlorophenyl)-2-oxoethoxy]-6,7,8,9-tetrahydro-5H-cyclohepta[b] pyridine-3-carbonitrile, C{sub 19}H{sub 17}ClN{sub 2}O{sub 2} (2a); (3-amino-6,7,8,9-tetrahydro-5H-cyclohepta[b]furo[3,2-e]pyridin-2-yl)(4- chlorophenyl)methanone, C{sub 19}H{sub 17}ClN{sub 2}O{sub 2} (3); 2-oxo-1,2,5,6,7,8,9,10-octahydrocycloocta[b]pyridine-3-carboxamide, C{sub 12}H{sub 16}N{sub 2}O{sub 2} (4); 2-[2-(4-chorophenyl)-2-oxoethoxy]-5,6,7,8,9,10 -hexahydrocycloocta[b]pyridine-3-carboxamide, C{sub 20}H{sub 21}ClN{sub 2}O{sub 3} (5a); 1-[2-(4-chlorophenyl)-2-oxoethyl]-2-oxo-1,2,5,6,7,8,9,10 -octahydrocycloocta[b]pyridine-3-carboxamide, C{sub 20}H{sub 21}ClN{sub 2}O{sub 3} (5b); and 2-[2-(4-chlorophenyl)-2-oxoethoxy]-5,6,7,8,9,10-hexahydrocycloocta[b] pyridine-3-carbonitrile, C{sub 20}H{sub 19}ClN{sub 2}O{sub 2}, (6). All compounds are characterized by {sup 1}H NMR spectroscopy, and their crystal structures are determined by X-ray diffraction.

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

Sutherland, J.W.

Pulse radiolysis of aqueous hydrazine solutions has been studied in the pH range 2 to 13. At times greater than about 1 ms after the pulse, a single transient species is observed (lambda/sub max/230nm). This species decayed by first-order kinetics under all conditions studied. A mechanism which accounts satisfactorily for the observed kinetic behavior is proposed. This species, identified as triazene (N/sub 3/H/sub 3/) is amphiprotic and the following acid--base equilibria are rapidly established: N/sub 3/H/sub 4//sup +/in equilibrium N/sub 3/H/sub 3//sup +/H/sup +/ (pK/sub 1/ = 4.95, ..delta..H/sub 1//sup 0/ = -4.9 kcal mol/sup -1/, ..delta..S/sub 1//sup 0/ =more » -39.2 eu) N/sub 3/H/sub 3/in equilibrium N/sub 3/H/sub 2//sup -/ + H/sup +/ or N/sub 3/H/sub 3/ + OH/sup -/ = N/sub 3/H/sub 4/O/sup -/ (pK/sub 2/ = 11.37, ..delta..H/sub 2//sup 0/ = -4.2 kcal mol/sup -1/, ..delta..S/sub 2//sup 0/ = -67 eu). pK values derived from the dependence of the first-order rate constant on pH, from the dependence of initial absorbance on pH, and from the dependence of the first-order rate constant on temperature at selected values of pH are in satisfactory agreement. The rate constants for decomposition of the acidic and basic forms of triazene are k/sub N3H4/sup +// = 1.97 X 10/sup 11/ exp(-12600/RT)s/sup -1/ and k/sub N3H2/sup -// = 2.14 X 10/sup 14/. exp(-19200/RT)s/sup -1/. For N/sub 3/H/sub 3/, which is stable relative to the faster reaction rates of its conjugate acid and base forms, k is estimated to be less than or equal to 0.001 s/sup -1/ at 24/sup 0/C. The dependence of the observed first-order rate constant on pH at constant temperature is expressed by the following equation: k/sub obsd/ = (k/sub 3//(1 + (K/sub 1//(H/sup +/)))) + (k;/sub 4//(1 + ((H/sup +/)/K/sub 2/))) (k/sub 3/ = k/sub N3H4/sup +// = 133 s/sup -1/, k/sub 4/ = k/sub N3H2/sup -// = 2 s/sup -1/, pK/sub 1/ = 4.9/sub 5/ and pK/sub 2/ = 11.3/sub 7/). Phosphate is a catalyst for the decomposition of triazene. It is shown that the conjugate acid of neutral triazene has unit positive charge and its conjugate base has unit negative charge.« less

Electron density distribution and disordered crystal structure of 15R-SiAlON, SiAl{sub 4}O{sub 2}N{sub 4}

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

Banno, Hiroki; Hanai, Takaaki; Asaka, Toru

2014-03-15

The crystal structure of SiAl{sub 4}O{sub 2}N{sub 4} was characterized by laboratory X-ray powder diffraction (CuKα{sub 1}). The title compound is trigonal with space group R3-bar m. The hexagonal unit-cell dimensions (Z=3) are a=0.301332(3) nm, c=4.18616(4) nm and V=0.3291825(5) nm{sup 3}. The initial structural model was successfully derived by the charge-flipping method and further refined by the Rietveld method. The final structural model showed the positional disordering of one of the three (Si,Al) sites. The maximum-entropy method-based pattern fitting (MPF) method was used to confirm the validity of the split-atom model, in which conventional structure bias caused by assuming intensitymore » partitioning was minimized. The reliability indices calculated from the MPF were R{sub wp}=5.05%, S (=R{sub wp}/R{sub e})=1.21, R{sub p}=3.77%, R{sub B}=1.29% and R{sub F}=1.01%. The disordered crystal structure was successfully described by overlapping three types of domains with ordered atom arrangements. The distribution of atomic positions in one of the three types of domains can be achieved in the space group R3-bar m. The atom arrangements in the other two types of domains are noncentrosymmetrical with the space group R3m. These two structural configurations are related by the pseudo-symmetry inversion. -- Graphical abstract: A bird's eye view of electron densities up to 75.3% (0.133 nm{sup −3}) of the maximum on the plane parallel to (110) with the corresponding atomic arrangements of SiAl{sub 4}O{sub 2}N{sub 4}. Highlights: • Crystal structure of SiAl{sub 4}O{sub 2}N{sub 4} is determined by laboratory X-ray powder diffraction. • The atom arrangements are represented by the split-atom model. • The maximum-entropy method-based pattern fitting method is used to confirm the validity of the model. • The disordered structure is described by overlapping three types of domains with ordered atom arrangements.« less

Neutral gas temperature estimates and metastable resonance energy transfer for argon-nitrogen discharges

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

Greig, A., E-mail: amelia.greig@anu.edu.au; Charles, C.; Boswell, R. W.

2016-01-15

Rovibrational spectroscopy band fitting of the nitrogen (N{sub 2}) second positive system is a technique used to estimate the neutral gas temperature of N{sub 2} discharges, or atomic discharges with trace amounts of a N{sub 2} added. For mixtures involving argon and N{sub 2}, resonant energy transfer between argon metastable atoms (Ar*) and N{sub 2} molecules may affect gas temperature estimates made using the second positive system. The effect of Ar* resonance energy transfer is investigated here by analyzing neutral gas temperatures of argon-N{sub 2} mixtures, for N{sub 2} percentages from 1% to 100%. Neutral gas temperature estimates are highermore » than expected for mixtures involving greater than 5% N{sub 2} addition, but are reasonable for argon with less than 5% N{sub 2} addition when compared with an analytic model for ion-neutral charge exchange collisional heating. Additional spatiotemporal investigations into neutral gas temperature estimates with 10% N{sub 2} addition demonstrate that although absolute temperature values may be affected by Ar* resonant energy transfer, spatiotemporal trends may still be used to accurately diagnose the discharge.« less

Prospects for measuring the fuel ion ratio in burning ITER plasmas using a DT neutron emission spectrometer

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

Hellesen, C.; Skiba, M., E-mail: mateusz.skiba@physics.uu.se; Dzysiuk, N.

2014-11-15

The fuel ion ratio n{sub t}/n{sub d} is an essential parameter for plasma control in fusion reactor relevant applications, since maximum fusion power is attained when equal amounts of tritium (T) and deuterium (D) are present in the plasma, i.e., n{sub t}/n{sub d} = 1.0. For neutral beam heated plasmas, this parameter can be measured using a single neutron spectrometer, as has been shown for tritium concentrations up to 90%, using data obtained with the MPR (Magnetic Proton Recoil) spectrometer during a DT experimental campaign at the Joint European Torus in 1997. In this paper, we evaluate the demands thatmore » a DT spectrometer has to fulfill to be able to determine n{sub t}/n{sub d} with a relative error below 20%, as is required for such measurements at ITER. The assessment shows that a back-scattering time-of-flight design is a promising concept for spectroscopy of 14 MeV DT emission neutrons.« less

Airborne asphyxia: an international problem

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

Friedlander, G.D.

1965-10-01

An overview is presented of air pollution which has become a real problem that affects virtually every major industrial city in the United States and Europe. Air pollution presents one of the most serious threats to the coal industry which produces about 55% of the electric power in the USA. There are meteorological and climatological factors that influence the action of air borne pollutants. The effects of SO/sub 2/ and N/sub 2/O on human health are discussed. Methods of reducing SO/sub 2/ emissions are presented. The results of studies by TVA in SO/sub 2/ monitoring and control have been appliedmore » in planning subsequent plants. There are an estimated 88 million motor vehicles on the nation's highways that contribute to air pollution. Control devices for cars can effectively reduce the amount of air contaminants released from motor vehicle exhausts. From numerous surveys, it is obvious that the sources of air pollution are numerous and complex. Total and effective remedial action must be undertaken to correct the situation.« less

An interpretation of a mysterious 3.0- to 4.6-kHz emission band observed on Voyager 2 near Neptune

NASA Technical Reports Server (NTRS)

Sonwalkar, Vikas S.; Inan, Umran S.; Bell, Timothy F.

1995-01-01

A whistler mode interpretation is provided for the narrowband signal (f approx. 3 - 4.6 kHz, Delta f approx. 200 - 800 Hz) detected by the plasma wave instrument on Voyager 2 during its encounter with Neptune. Our analysis indicates that this signal may have been generated in a limited spatial region and that it propagated to other regions of the Neptunian magnetosphere in the nonducted whistler mode with wave normal vectors lying close to the whistler mode resonance cone. The observed frequency variation of the emission along the Voyager 2 trajectory is consistent with this interpretation. The source location is estimated to be near the magnetic equator at L approx. 4 and dipole longitude of 111 deg W (260 deg W longitude in Neptune coordinate system). The source frequency and bandwidth are estimated to be 3.6 kHz and 300 Hz, respectively. The waves most likely would have been generated by energetic electrons with 2- to 20-keV parallel energy via a gyroresonance mechanism. Our interpretation of the narrowband emissions places the following limits on the Neptunian thermal plasma density and temperature: (1) N(sub e, min) greater than 0.16 el/cu cm for 1.2 R(sub N) less than R less than 5 R(sub N), (2) N(sub e, max) = 597.5/cu cm at R - 1.3 R(sub N), (3) T(sub e, max) less than 500-1000 K at R approx. 5 R(sub N). It is also possible that the weak UV aurora observed near Neptune could have been caused by the precipitation of energetic particles by the narrowband emission as a result of wave particle interactions.

Internal structure of laser supported detonation waves by two-wavelength Mach-Zehnder interferometer

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

Shimamura, Kohei; Kawamura, Koichi; Fukuda, Akio

Characteristics of the internal structure of the laser supported detonation (LSD) waves, such as the electron density n{sub e} and the electron temperature T{sub e} profiles behind the shock wave were measured using a two-wavelength Mach-Zehnder interferometer along with emission spectroscopy. A TEA CO{sub 2} laser with energy of 10 J/pulse produced explosive laser heating in atmospheric air. Results show that the peak values of n{sub e} and T{sub e} were, respectively, about 2 x 10{sup 24} m{sup -3} and 30 000 K, during the LSD regime. The temporal variation of the laser absorption coefficient profile estimated from the measuredmore » properties reveals that the laser energy was absorbed perfectly in a thin layer behind the shock wave during the LSD regime, as predicted by Raizer's LSD model. However, the absorption layer was much thinner than a plasma layer, the situation of which was not considered in Raizer's model. The measured n{sub e} at the shock front was not zero while the LSD was supported, which implies that the precursor electrons exist ahead of the shock wave.« less

Effects of aging and oxidation of palladized iron embedded in activated carbon on the dechlorination of 2-chlorobiphenyl

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

Hyeok Choi; Souhail R. Al-Abed; Shirish Agarwal

2009-06-15

Reactive activated carbon (RAC) impregnated with palladized iron has been developed to effectively treat polychlorinated biphenyls (PCBs) in the environment by coupling adsorption and dechlorination of PCBs. In this study, we addressed the dechlorination reactivity and capacity of RAC toward aqueous 2-chlorobiphenyl (2-ClBP), and its aging and longevity under various oxidizing environments. RAC containing 14.4% Fe and 0.68% Pd used in this study could adsorb 122.6 mg 2-ClBP/g RAC, and dechlorinate 56.5 mg 2-ClBP/g RAC which corresponds to 12% (yield) of its estimated dechlorination capacity. Due to Fe0 oxidation to form oxide passivating layers, Fe{sub 2}O{sub 3}/Fe{sub 3}O{sub 4} (oxide-watermore » interface) and FeOOH/FeO (oxide-metal interface), RAC reactivity decreased progressively over aging under N{sub 2} < H{sub 2}O + N{sub 2} < H{sub 2}O + O{sub 2} conditions. Considering nanoscale Fe/Pd corrosion chemistry, the decline was quite slow at only 5.6%, 19.5%, and 32.5% over one year, respectively. Dissolved oxygen played a crucial role in enhancing 2-ClBP adsorption but inhibiting its dechlorination. The reactivity change could be explained with the properties of the aged RAC including surface area, Fe0 content, and Fe species. During the aging and oxidation, the RAC showed limited dissolution of Fe and Pd. Finally, implementation issues regarding application of RAC system to contaminated sites are discussed. 25 refs., 6 figs., 1 tab.« less

Hydrothermal synthesis and characterization of a two-dimensional piperazinium cobalt–zinc phosphate via a metastable one-dimensional phase

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

Torre-Fernández, Laura; Khainakova, Olena A.; Espina, Aránzazu

2015-05-15

A two-dimensional piperazinium cobalt–zinc phosphate, formulated as (C{sub 4}N{sub 2}H{sub 12}){sub 1.5}(Co{sub 0.6}Zn{sub 0.4}){sub 2}(HPO{sub 4}){sub 2}(PO{sub 4})·H{sub 2}O (2D), was synthesized under hydrothermal conditions. The crystal structure was determined using single-crystal X-ray diffraction data (monoclinic P2{sub 1}/c, a=8.1165(3) Å, b=26.2301(10) Å, c=8.3595(4) Å, and β=110.930(5)°) and the hydrogen atom positions were optimized by DFT calculations. A single-crystal corresponding to one-dimensional metastable phase, (C{sub 4}N{sub 2}H{sub 12})Co{sub 0.3}Zn{sub 0.7}(HPO{sub 4}){sub 2}·H{sub 2}O (1D), was also isolated and the crystal structure was determined (monoclinic P2{sub 1}/c, a=8.9120(6) Å, b=14.0290(1) Å, c=12.2494(5) Å, and β=130.884(6)°). The bulk was characterized by chemical (C–H–N)more » analysis, powder X-ray diffraction (PXRD), powder X-ray thermodiffractometry (HT-XRD), transmission electron microscopy (STEM(DF)-EDX and EFTEM), and thermal analysis (TG/SDTA-MS), including activation energy data of its thermal decomposition. The magnetic susceptibility and magnetization measurements show no magnetic ordering down to 4 K. - Graphical abstract: Hydrothermal synthesis and structural characterization of a two-dimensional piperazinium cobalt–zinc phosphate, (C{sub 4}N{sub 2}H{sub 12}){sub 1.5}(Co{sub 0.6}Zn{sub 0.4}){sub 2}(HPO{sub 4}){sub 2}(PO{sub 4})·H{sub 2}O (2D), have been reported. The crystal structure of a one-dimensional piperazinium cobalt–zinc phosphate, (C{sub 4}N{sub 2}H{sub 12})Co{sub 0.3}Zn{sub 0.7}(HPO{sub 4}){sub 2}·H{sub 2}O (1D) a metastable phase during the hydrothermal synthesis, was also determined. The thermal behavior of 2D compound is strongly dependent on the selected heating rate and the magnetic susceptibility and magnetization measurements show no magnetic ordering down to 4 K. - Highlights: • A 2D piperazinium cobalt–zinc phosphate has been synthesized and characterized. • Crystal structure of 1D metastable phase was also determined. • Thermal behavior of 2D compound is strongly dependent on the selected heating rate. • Magnetic measurements show no magnetic ordering down to 4 K.« less

A Monte Carlo simulation of the effect of ion self-collisions on the ion velocity distribution function in the high-latitude F-region

NASA Technical Reports Server (NTRS)

Barghouthi, I. A.; Barakat, A. R.; Schunk, R. W.

1994-01-01

Non-Maxwellian ion velocity distribution functions have been theoretically predicted and confirmed by observations, to occur at high latitudes. These distributions deviate from Maxwellian due to the combined effect of the E x B drift and ion-neutral collisions. At high altitude and/or for solar maximum conditions, the ion-to-neutral density ratio increases and, hence, the role of ion self-collisions becomes appreciable. A Monte Carlo simulation was used to investigate the behavior of O(+) ions that are E x B-drifting through a background of neutral O, with the effect of O(+) (Coulomb) self-collisions included. Wide ranges of the ion-to-neutral density ratio n(sub i)/n(sub n) and the electrostatic field E were considered in order to investigate the change of ion behavior with solar cycle and with altitude. For low altitudes and/or solar minimum (n(sub i)/n(sub n) less than or equal to 10(exp -5)), the effect of self-collisions is negligible. For higher values of n(sub i)/n(sub n), the effect of self-collisions becomes significant and, hence, the non-Maxwellian features of the O(+) distribution are reduced. The Monte Carlo results were compared to those that used simplified collision models in order to assess their validity. In general, the simple collision models tend to be more accurate for low E and for high n(sub i)/n(sub n).

The effect of ozone on nicotine desorption from model surfaces:evidence for heterogeneous chemistry

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

Destaillats, Hugo; Singer, Brett C.; Lee, Sharon K.

Assessment of secondhand tobacco smoke exposure using nicotine as a tracer or biomarker is affected by sorption of the alkaloid to indoor surfaces and by its long-term re-emission into the gas phase. However, surface chemical interactions of nicotine have not been sufficiently characterized. Here, the reaction of ozone with nicotine sorbed to Teflon and cotton surfaces was investigated in an environmental chamber by monitoring nicotine desorption over a week following equilibration in dry or humid air (65-70 % RH). The Teflon and cotton surfaces had N{sub 2}-BET surface areas of 0.19 and 1.17 m{sup 2} g{sup -1}, and water massmore » uptakes (at 70 % RH) of 0 and 7.1 % respectively. Compared with dry air baseline levels in the absence of O{sub 3}, gas phase nicotine concentrations decrease, by 2 orders of magnitude for Teflon after 50 h at 20-45 ppb O{sub 3}, and by a factor of 10 for cotton after 100 h with 13-15 ppb O{sub 3}. The ratios of pseudo first-order rate constants for surface reaction (r) to long-term desorption (k) were r/k = 3.5 and 2.0 for Teflon and cotton surfaces, respectively. These results show that surface oxidation was competitive with desorption. Hence, oxidative losses could significantly reduce long-term re-emissions of nicotine from indoor surfaces. Formaldehyde, N-methylformamide, nicotinaldehyde and cotinine were identified as oxidation products, indicating that the pyrrolidinic N was the site of electrophilic attack by O{sub 3}. The presence of water vapor had no effect on the nicotine-O{sub 3} reaction on Teflon surfaces. By contrast, nicotine desorption from cotton in humid air was unaffected by the presence of ozone. These observations are consistent with complete inhibition of ozone-nicotine surface reactions in an aqueous surface film present in cotton but not in Teflon surfaces.« less

Updated greenhouse gas and criteria air pollutant emission factors and their probability distribution functions for electricity generating units

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

Cai, H.; Wang, M.; Elgowainy, A.

Greenhouse gas (CO{sub 2}, CH{sub 4} and N{sub 2}O, hereinafter GHG) and criteria air pollutant (CO, NO{sub x}, VOC, PM{sub 10}, PM{sub 2.5} and SO{sub x}, hereinafter CAP) emission factors for various types of power plants burning various fuels with different technologies are important upstream parameters for estimating life-cycle emissions associated with alternative vehicle/fuel systems in the transportation sector, especially electric vehicles. The emission factors are typically expressed in grams of GHG or CAP per kWh of electricity generated by a specific power generation technology. This document describes our approach for updating and expanding GHG and CAP emission factors inmore » the GREET (Greenhouse Gases, Regulated Emissions, and Energy Use in Transportation) model developed at Argonne National Laboratory (see Wang 1999 and the GREET website at http://greet.es.anl.gov/main) for various power generation technologies. These GHG and CAP emissions are used to estimate the impact of electricity use by stationary and transportation applications on their fuel-cycle emissions. The electricity generation mixes and the fuel shares attributable to various combustion technologies at the national, regional and state levels are also updated in this document. The energy conversion efficiencies of electric generating units (EGUs) by fuel type and combustion technology are calculated on the basis of the lower heating values of each fuel, to be consistent with the basis used in GREET for transportation fuels. On the basis of the updated GHG and CAP emission factors and energy efficiencies of EGUs, the probability distribution functions (PDFs), which are functions that describe the relative likelihood for the emission factors and energy efficiencies as random variables to take on a given value by the integral of their own probability distributions, are updated using best-fit statistical curves to characterize the uncertainties associated with GHG and CAP emissions in life-cycle modeling with GREET.« less

METHOD OF FIXING NITROGEN FOR PRODUCING OXIDES OF NITROGEN

DOEpatents

Harteck, P.; Dondes, S.

1959-08-01

A method is described for fixing nitrogen from air by compressing the air, irradiating the compressed air in a nuclear reactor, cooling to remove NO/ sub 2/, compressing the cooled gas, further cooling to remove N/sub 2/O and recirculating the cooled compressed air to the reactor.

Integrated Climate Change Information for Resilient Adaptation Planning

EPA Science Inventory

Awareness is growing that some air, water, and ecosystem impacts from climate change are inevitable due to the long residence times of key greenhouse gases (GHGs), including carbon dioxide (CO₂), methane (CH₄) and nitrous oxide (N₂O), which are in...

Measurements of the rate constant of HOsub2 + NOsub2 + Nsub2 --> HOsub2NOsub2 + Nsub2 using near-infrared wavelength-modulation spectroscopy and UV-visible absorption spectroscopy

NASA Technical Reports Server (NTRS)

Christensen, L. E.; Okumura, M.; Sander, S. P.; Friedl, R. R.; Miller, C. E.; Sloan, J. J.

2004-01-01

Rate coefficients for the reaction HO(sub 2)+ NO(sub 2) + N(sub 2) --> HO(sub 2)NO(sub 2) + N(sub 2) (reaction 1) were measured using simultaneous near-IR and UV spectroscopy from 220 to 298 K and from 45 to 200 Torr.

Intermixing between HfO{sub 2} and GeO{sub 2} films deposited on Ge(001) and Si(001): Role of the substrate

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

Soares, G. V.; Krug, C.; Miotti, L.

2011-03-28

Thermally driven atomic transport in HfO{sub 2}/GeO{sub 2}/substrate structures on Ge(001) and Si(001) was investigated in N{sub 2} ambient as function of annealing temperature and time. As-deposited stacks showed no detectable intermixing and no instabilities were observed on Si. On Ge, loss of O and Ge was detected in all annealed samples, presumably due to evolution of GeO from the GeO{sub 2}/Ge interface. In addition, hafnium germanate is formed at 600 deg. C. Our data indicate that at 500 deg. C and above HfO{sub 2}/GeO{sub 2} stacks are stable only if isolated from the Ge substrate.

Electron Densities in Solar Flare Loops, Chromospheric Evaporation Upflows, and Acceleration Sites

NASA Technical Reports Server (NTRS)

Aschwanden, Markus J.; Benz, Arnold O.

1996-01-01

We compare electron densities measured at three different locations in solar flares: (1) in Soft X-Ray (SXR) loops, determined from SXR emission measures and loop diameters from Yohkoh Soft X-Ray Telescope maps (n(sub e, sup SXR) = (0.2-2.5) x 10(exp 11)/ cu cm); (2) in chromospheric evaporation upflows, inferred from plasma frequency cutoffs of decimetric radio bursts detected with the 0.1-3 GHz spectrometer Phoenix of ETH Zuerich (n(sub e, sup upflow) = (0.3-11) x 10(exp 10)/cu cm; and (3) in acceleration sites, inferred from the plasma frequency at the separatrix between upward-accelerated (type III bursts) and downward-accelerated (reverse-drift bursts) electron beams [n(sub e, sup acc) = (0.6-10) x 10(exp 9)/cu cm]. The comparison of these density measurements, obtained from 44 flare episodes (during 14 different flares), demonstrates the compatibility of flare plasma density diagnostics with SXR and radio methods. The density in the upflowing plasma is found to be somewhat lower than in the filled loops, having ratios in a range n(sub e, sup upflow)/n(sub e, sup SXR) = 0.02-1.3, and a factor of 3.6 higher behind the upflow front. The acceleration sites are found to have a much lower density than the SXR-bright flare loops, i.e., n(sub e, sup acc)/n(sub e, sup SXR) = 0.005- 0.13, and thus must be physically displaced from the SXR-bright flare loops. The scaling law between electron time-of-flight distances l' and loop half-lengths s, l'/s = 1.4 +/- 0.3, recently established by Aschwanden et al. suggests that the centroid of the acceleration region is located above the SXR-bright flare loop, as envisioned in cusp geometries (e.g., in magnetic reconnection models).

Mechanism of formation of the response of a hydrogen gas sensor based on a silicon MOS diode

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

Gaman, V. I.; Balyuba, V. I.; Gritsyk, V. Yu.

2008-03-15

Experimental data on the dependence of the flat-band voltage and relaxation time for the capacitance of the space-charge region in an MOS diode (Pd-SiO{sub 2}-n-Si) on the hydrogen concentration in a hydrogen/air gaseous mixture are discussed. It is assumed that variation in the flat-band voltage U{sub fb} in an MOS structure with the thickness d = 369 nm subjected to a hydrogen/air gaseous mixture can be accounted for by the formation of dipoles in the Pd-SiO{sub 2} gap due to polarization of hydrogen atoms (H{sub a}). An analytical expression describing the dependence of variation in the flat-band voltage {Delta}U{sub fb}more » on the hydrogen concentration n{sub H{sub 2}} was derived. In MOS structures with d {<=} 4 nm (or MOS diodes), the value of {Delta}U{sub fb} is mainly controlled by passivation of the centers responsible for the presence of the surface acceptor-type centers at the SiO{sub 2}-n-Si interface by hydrogen atoms. Analytical expressions describing the dependences of {Delta}U{sub fb} and the capacitance relaxation time in the space-charge region on n{sub H{sub 2}} are derived. The values of the density of adsorption centers and the adsorption heat for hydrogen atoms at the Pd-SiO{sub 2} and SiO{sub 2}-n-Si interfaces are found.« less

Mechanism of formation of the response of a hydrogen gas sensor based on a silicon MOS diode

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

Gaman, V. I.; Balyuba, V. I.; Gritsyk, V. Yu.

2008-03-15

Experimental data on the dependence of the flat-band voltage and relaxation time for the capacitance of the space-charge region in an MOS diode (Pd-SiO{sub 2}-n-Si) on the hydrogen concentration in a hydrogen/air gaseous mixture are discussed. It is assumed that variation in the flat-band voltage U{sub fb} in an MOS structure with the thickness d = 369 nm subjected to a hydrogen/air gaseous mixture can be accounted for by the formation of dipoles in the Pd-SiO{sub 2} gap due to polarization of hydrogen atoms (H{sub a}). An analytical expression describing the dependence of variation in the flat-band voltage {delta}U{sub fb}more » on the hydrogen concentration n{sub H2} was derived. In MOS structures with d {<=} 4 nm (or MOS diodes), the value of {delta}U{sub fb} is mainly controlled by passivation of the centers responsible for the presence of the surface acceptor-type centers at the SiO{sub 2}-n-Si interface by hydrogen atoms. Analytical expressions describing the dependences of {delta}U{sub fb} and the capacitance relaxation time in the space-charge region on n{sub H2} are derived. The values of the density of adsorption centers and the adsorption heat for hydrogen atoms at the Pd-SiO{sub 2} and SiO{sub 2}-n-Si interfaces are found.« less

Applicability of modified effective-range theory to positron-atom and positron-molecule scattering

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

Idziaszek, Zbigniew; Karwasz, Grzegorz; Instytut Fizyki, Uniwersytet Mikolaja Kopernika, 87-100 Torun

2006-06-15

We analyze low-energy scattering of positrons on Ar atoms and N{sub 2} molecules using the modified effective-range theory (MERT) developed by O'Malley, et al. [J. Math. Phys. 2, 491 (1961)]. We use the formulation of MERT based on exact solutions of the Schroedinger equation with polarization potential rather than low-energy expansions of phase shifts into momentum series. We show that MERT describes the experimental data well, provided that effective-range expansion is performed both for s- and p-wave scattering, which dominate in the considered regime of positron energies (0.4-2 eV). We estimate the values of the s-wave scattering length and themore » effective range for e{sup +}-Ar and e{sup +}-N{sub 2} collisions.« less

Comparing two tetraalkylammonium ionic liquids. I. Liquid phase structure

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

Lima, Thamires A.; Paschoal, Vitor H.; Faria, Luiz F. O.

2016-06-14

X-ray scattering experiments at room temperature were performed for the ionic liquids n-butyl-trimethylammonium bis(trifluoromethanesulfonyl)imide, [N{sub 1114}][NTf{sub 2}], and methyl-tributylammonium bis(trifluoromethanesulfonyl)imide, [N{sub 1444}][NTf{sub 2}]. The peak in the diffraction data characteristic of charge ordering in [N{sub 1444}][NTf{sub 2}] is shifted to longer distances in comparison to [N{sub 1114}][NTf{sub 2}], but the peak characteristic of short-range correlations is shifted in [N{sub 1444}][NTf{sub 2}] to shorter distances. Molecular dynamics (MD) simulations were performed for these ionic liquids using force fields available from the literature, although with new sets of partial charges for [N{sub 1114}]{sup +} and [N{sub 1444}]{sup +} proposed in this work.more » The shifting of charge and adjacency peaks to opposite directions in these ionic liquids was found in the static structure factor, S(k), calculated by MD simulations. Despite differences in cation sizes, the MD simulations unravel that anions are allowed as close to [N{sub 1444}]{sup +} as to [N{sub 1114}]{sup +} because anions are located in between the angle formed by the butyl chains. The more asymmetric molecular structure of the [N{sub 1114}]{sup +} cation implies differences in partial structure factors calculated for atoms belonging to polar or non-polar parts of [N{sub 1114}][NTf{sub 2}], whereas polar and non-polar structure factors are essentially the same in [N{sub 1444}][NTf{sub 2}]. Results of this work shed light on controversies in the literature on the liquid structure of tetraalkylammonium based ionic liquids.« less

On twin density and resistivity of nanometric Cu thin films

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

Barmak, Katayun; Liu, Xuan; Darbal, Amith

2016-08-14

Crystal orientation mapping in the transmission electron microscope was used to quantify the twin boundary length fraction per unit area for five Ta{sub 38}Si{sub 14}N{sub 48}/SiO{sub 2} encapsulated Cu films with thicknesses in the range of 26–111 nm. The length fraction was found to be higher for a given twin-excluded grain size for these films compared with previously investigated SiO{sub 2} and Ta/SiO{sub 2} encapsulated films. The quantification of the twin length fraction per unit area allowed the contribution of the twin boundaries to the size effect resistivity to be assessed. It is shown that the increased resistivity of the Ta{submore » 38}Si{sub 14}N{sub 48} encapsulated Cu films compared with the SiO{sub 2} and Ta/SiO{sub 2} encapsulated films is not a result of increased surface scattering, but it is a result of the increase in the density of twin boundaries. With twin boundaries included in the determination of grain size as a mean-intercept length, the resistivity data are well described by 2-parameter Matthiessen's rule summation of the Fuchs-Sondheimer and Mayadas Shatzkes models, with p and R parameters that are within experimental error equal to those in prior reports and are p = 0.48(+0.33/−0.31) and R = 0.27 ± 0.03.« less

Synthesis of reduced carbon nitride at the reduction by hydroquinone of water-soluble carbon nitride oxide (g-C{sub 3}N{sub 4})O

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

Kharlamov, Alexey; Bondarenko, Marina, E-mail: mebondarenko@ukr.net; Kharlamova, Ganna

For the first time at the reduction by hydroquinone of water-soluble carbon nitride oxide (g-C{sub 3}N{sub 4})O reduced carbon nitride (or reduced multi-layer azagraphene) is obtained. It is differed from usually synthesized carbon nitride by a significantly large (on 0.09 nm) interplanar distance is. At the same time, the chemical bonds between atoms in a heteroatomic plane of reduced carbon nitride correspond to the bonds in a synthesized g-C{sub 3}N{sub 4}. The samples of water-soluble carbon nitride oxide were synthesized under the special reactionary conditions of a pyrolysis of melamine and urea. We believe that reduced carbon nitride consists ofmore » weakly connected carbon-nitrogen monosheets (azagraphene sheets) as well as reduced (from graphene oxide) graphene contains weakly connected graphene sheets. - Graphical abstract: XRD pattern and schematic atomic model of one layer of reduced carbon nitride, carbon nitride oxide and synthesized carbon nitride. For the first time at the reduction by hydroquinone of the water-soluble carbon nitride oxide (g-C{sub 3}N{sub 4})O is obtained the reduced carbon nitride (or reduced multi-layer azagraphene). Display Omitted - Highlights: • First the reduced carbon nitride (RCN) at the reduction of the carbon nitride oxide was obtained. • Water-soluble carbon nitride oxide was reduced by hydroquinone. • The chemical bonds in a heteroatomic plane of RCN correspond to the bonds in a synthesized g-C{sub 3}N{sub 4}. • Reduced carbon nitride consists of poorly connected heteroatomic azagraphene layers.« less

Microwave-plasma in a simple magnetized torus

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

Rypdal, K.; Fredriksen, M.; Olsen, O.M.

1997-05-01

In a magnetized torus with no poloidal field component, a weakly ionized plasma is produced by microwaves at 2.45 GHz in the O-mode as well as the X-mode. The neutral gas pressure p{sub g} ranges from 5{times}10{sup {minus}5} to 1{times}10{sup {minus}3} mbar, n{sub e}{approximately}1{minus}5{times}10{sup 16}m{sup {minus}3}, and T{sub e}{approximately}2{minus}6 eV. The O-mode is only weakly absorbed at the electron cyclotron resonance (ECR), but is partly converted to the X-mode by wall reflections. The X-mode is absorbed via the upper hybrid resonance (UHR), presumably through conversion to and absorption of electron Bernstein waves (EBW). For p{sub g}{gt}1{times}10{sup {minus}3} mbar the EBWmore » absorption is collisional, but for lower p{sub g} a collisionless transit particle mechanism could be responsible. Typically the spatial plasma distribution depends mainly on the major radius R, and the measured n{sub e}(R) increases monotonically with R from the ECR to an UHR near the outer wall. T{sub e} is determined by the particle balance, and is proportional to the ionization energy. The average n{sub e} is determined by power balance, and increases with wave power. {copyright} {ital 1997 American Institute of Physics.}« less

Oxalate co-precipitation synthesis of calcium zirconate and calcium titanate powders.

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

Hernandez-Sanchez, Bernadette A.; Tuttle, Bruce Andrew

2009-06-01

Fine powders of calcium zirconate (CaZrO{sub 3}, CZ) and calcium titanate (CaTiO{sub 3}, CT) were synthesized using a nonaqueous oxalate co-precipitation route from Ca(NO{sub 3}){sub 2}{center_dot}4 H{sub 2}O and group(IV) n-butoxides (Ti(OBu{sup n}){sub 4} or Zr(OBu{sup n}){sub 4}). Several reaction conditions and batch sizes (2-35 g) were explored to determine their influence on final particle size, morphology, and phase. Characterization of the as-prepared oxalate precursors, oven dried oxalate precursors (60-90 C), and calcined powders (635-900 C) were analyzed with TGA/DTA, XRD, TEM, and SEM. Densification and sintering studies on pressed CZ pellets at 1375 and 1400 C were also performed.more » Through the developed oxalate co-precipitation route, densification temperatures for CZ were lowered by 125 C from the 1500 C firing temperature required for conventional mixed oxide powders. Low field electrical tests of the CZ pellets indicated excellent dielectric properties with dielectric constants of {approx}30 and a dissipation factor of 0.0004 were measured at 1 kHz.« less

Fixed interface charges between AlGaN barrier and gate stack composed of in situ grown SiN and Al{sub 2}O{sub 3} in AlGaN/GaN high electron mobility transistors with normally off capability

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

Capriotti, M., E-mail: mattia.capriotti@tuwien.ac.at; Alexewicz, A.; Fleury, C.

2014-03-17

Using a generalized extraction method, the fixed charge density N{sub int} at the interface between in situ deposited SiN and 5 nm thick AlGaN barrier is evaluated by measurements of threshold voltage V{sub th} of an AlGaN/GaN metal insulator semiconductor high electron mobility transistor as a function of SiN thickness. The thickness of the originally deposited 50 nm thick SiN layer is reduced by dry etching. The extracted N{sub int} is in the order of the AlGaN polarization charge density. The total removal of the in situ SiN cap leads to a complete depletion of the channel region resulting in V{sub th} = +1 V.more » Fabrication of a gate stack with Al{sub 2}O{sub 3} as a second cap layer, deposited on top of the in situ SiN, is not introducing additional fixed charges at the SiN/Al{sub 2}O{sub 3} interface.« less

Novel ethylenediamine-gallium phosphate containing 6-fold coordinated gallium atoms with unusual four equatorial Ga–N bonds

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

Torre-Fernández, Laura; Espina, Aránzazu; Khainakov, Sergei A.

2014-07-01

A novel ethylenediamine-gallium phosphate, formulated as Ga(H{sub 2}NCH{sub 2}CH{sub 2}NH{sub 2}){sub 2}PO{sub 4}·2H{sub 2}O, was synthesized under hydrothermal conditions. The crystal structure, including hydrogen positions, was determined using single-crystal X-ray diffraction data (monoclinic, a=9.4886(3) Å, b=6.0374(2) Å, c=10.2874(3) Å, and β=104.226(3)°, space group Pc) and the bulk was characterized by chemical (Ga–P–C–H–N) and thermal analysis (TG–MS and DSC), including activation energy data of its thermo-oxidative degradation, powder X-ray diffraction (PXRD), solid-state nuclear magnetic resonance (SS-NMR) measurements, and transmission electron microscopy (TEM, SAED/NBD, and STEM BF-EDX). The crystal structure is built up of infinite zig-zag chains running along the c-axis, formedmore » by vertex-shared (PO{sub 4}) and (GaO{sub 2}N{sub 4}) polyhedra. The new compound is characterized by unusual four equatorial Ga–N bonds coming from two nonequivalent ethylenediamine molecules and exhibits strong blue emission at 430 nm (λ{sub ex}=350 nm) in the solid state at room temperature. - Graphical abstract: Single crystals of a new ethylenediamine-gallium phosphate, Ga(H{sub 2}NCH{sub 2}CH{sub 2}NH{sub 2}){sub 2}PO{sub 4}·2H{sub 2}O, were obtained and the structural features presented. This structure is one of the scarce examples of GaPO with Ga–N bonds reported. - Highlights: • A novel ethylenediamine-gallium phosphate was hydrothermally synthesized. • The new compound is characterized by unusual four equatorial Ga–N bonds. • Void-volume analysis shows cages and channels with sizes ideally suited to accommodate small molecules. • The new compound exhibits strong blue emission.« less

Properties of a weakly ionized NO gas sensor based on multi-walled carbon nanotubes

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

Zhang, Jingyuan; Zhang, Yong, E-mail: zhyong@mail.xjtu.edu.cn; Pan, Zhigang

2015-08-31

Nitric oxide NO is one of the major targets for environmental monitoring, but the existing NO sensors are limited by their low sensitivity and narrow test range. Here, a NO gas sensor employing multiwalled carbon nanotubes (MWCNTs) was fabricated, and its properties in NO–N{sub 2} mixture were investigated from both emission and ionization. The current I{sub e} passing through the nanotubes cathode was found to decrease with increasing NO concentration and increase linearly in different slopes with the extracting voltage U{sub e}. It is shown that the Schottky barrier of the MWCNTs calculated by I{sub e} increased with NO concentrationmore » due to the adsorption of NO gas, which restrained the electron emission and consequently weakened the ionization. The positive ion currents I{sub c} passing through the collecting electrode at different voltages of U{sub e} were found to monotonically decrease with increasing NO concentration, which was induced by both of the reduced electron emission and the consumption of the two excited metastable states N{sub 2}(A{sup 3}∑{sub u}{sup +}) and N{sub 2}(a′{sup 1}∑{sub u}{sup −}) by NO. The sensor exhibited high sensitivity at the low temperature of 30 °C. The calculated conductivity was found to be able to take place of I{sub c} for NO detection in a wide voltage range of 80–150 V U{sub e}.« less

Dual-pump CARS temperature and major species concentration measurements in counter-flow methane flames using narrowband pump and broadband Stokes lasers

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

Thariyan, Mathew P.; Ananthanarayanan, Vijaykumar; Bhuiyan, Aizaz H.

2010-07-15

Dual-pump coherent anti-Stokes Raman scattering (CARS) is used to measure temperature and species profiles in representative non-premixed and partially-premixed CH{sub 4}/O{sub 2}/N{sub 2} flames. A new laser system has been developed to generate a tunable single-frequency beam for the second pump beam in the dual-pump N{sub 2}-CO{sub 2} CARS process. The second harmonic output ({proportional_to}532 nm) from an injection-seeded Nd:YAG laser is used as one of the narrowband pump beams. The second single-longitudinal-mode pump beam centered near 561 nm is generated using an injection-seeded optical parametric oscillator, consisting of two non-linear {beta}-BBO crystals, pumped using the third harmonic output ({proportional_to}355more » nm) of the same Nd:YAG laser. A broadband dye laser (BBDL), pumped using the second harmonic output of an unseeded Nd:YAG laser, is employed to produce the Stokes beam centered near 607 nm with full-width-at-half-maximum of {proportional_to}250 cm{sup -1}. The three beams are focused between two opposing nozzles of a counter-flow burner facility to measure temperature and major species concentrations in a variety of CH{sub 4}/O{sub 2}/N{sub 2} non-premixed and partially-premixed flames stabilized at a global strain rate of 20 s{sup -1} at atmospheric-pressure. For the non-premixed flames, excellent agreement is observed between the measured profiles of temperature and CO{sub 2}/N{sub 2} concentration ratios with those calculated using an opposed-flow flame code with detailed chemistry and molecular transport submodels. For partially-premixed flames, with the rich side premixing level beyond the stable premixed flame limit, the calculations overestimate the distance between the premixed and the non-premixed flamefronts. Consequently, the calculated temperatures near the rich, premixed flame are higher than those measured. Accurate prediction of the distance between the premixed and the non-premixed flames provides an interesting challenge for future computations. (author)« less

DAYCENT AND ITS LAND SURFACE SUBMODEL: DESCRIPTION AND TESTING. (R824993)

EPA Science Inventory

Abstract

A land surface submodel was developed for the daily version of the CENTURY ecosystem model (DAYCENT). The goal of DAYCENT to simulate soil N₂O, NO_x, and CH₄ fluxes for terrestrial ecosystems determined the structure and ...

Improvement of hot-carrier and radiation hardnesses in metal-oxide-nitride-oxide semiconductor devices by irradiation-then-anneal treatments

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

Chang-Liao, K.S.; Hwu, J.G.

The hardnesses of hot-carrier and radiation of metal-oxide nitride-oxide semiconductor (MONOS) devices can be improved by the irradiation-then-anneal (ITA) treatments. Each treatment includes an irradiation of Co-60 with a total dose of 1M rads(SiO[sub 2]) and an anneal in N[sub 2] at 400 C for 10 min successively. This improvement can be explained by the release of SiO[sub 2]/Si interfacial strain.

Acid-catalyzed oxidation of 2,4-dichlorophenoxyacetic acid by ammonium nitrate in aqueous solution

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

Leavitt, D.D.; Abraham, M.A.

1990-04-01

2,4-Dichlorophenoxyacetic acid (2,4-D) was oxidized to CO{sub 2} and water by homogeneous, liquid-phase reaction with ammonium nitrate at temperatures between 250 and 450{degree}F and pressures below 100 psi. N{sub 2} and N{sub 2}O were produced from the thermal decomposition of the ammonium nitrate oxidant. An unexpected maximum in conversion was observed at an intermediate reaction temperature, which was consistent with rapid thermal decomposition of the NH{sub 4}NO{sub 3} oxidant. Postulated reaction pathways consisting of simultaneous oxidation of 2,4-D and decomposition of the oxidant allowed estimation of kinetic constants from best-fit analysis of the data. The proposed reaction model provided amore » mathematical description of 2,4-D conversion, which allowed extrapolation of the results to reaction conditions and reactor configurations that were not experimentally investigated.« less

Method for improving the toughness of silicon carbide-based ceramics

DOEpatents

Tein, Tseng-Ying; Hilmas, Gregory E.

1996-01-01

Method of improving the toughness of SiC-based ceramics. SiC, , AlN, Al.sub.2 O.sub.3 and optionally .alpha.-Si.sub.3 N.sub.4 are hot pressed to form a material which includes AlN polytypoids within its structure.

Synthesis of mesoporous TS-1 using a hybrid SiO{sub 2}–TiO{sub 2} xerogel for catalytic oxidative desulfurization

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

Yang, Seung-Tae; Jeong, Kwang-Eun; Jeong, Soon-Yong

2012-12-15

Graphical abstract: Display Omitted Highlights: ► Meso-TS-1 catalyst was synthesized using a SiO{sub 2}–TiO{sub 2} xerogel with an organosilane precursor. ► Hierarchical pore structure was confirmed by characterization of the materials. ► Catalytic activity was tested using oxidative desulfurization of the model sulfur compounds. ► Meso-TS-1 demonstrated significantly improved catalytic activity than TS-1. -- Abstract: Mesoporous TS-1 (M-TS-1) was synthesized using a hybrid SiO{sub 2}–TiO{sub 2} xerogel combined with an organosilane precursor. Prepared samples were characterized by XRD, UV–vis spectroscopy, SEM, and N{sub 2} adsorption–desorption measurement. M-TS-1, prepared in 2 days, showed high crystallinity and the best textural properties amongmore » the samples. The N{sub 2} adsorption–desorption isotherms of M-TS-1 exhibited a hysteresis loop at pressure higher than P/P{sub 0} = 0.4, clearly indicating the existence of mesopores. M-TS-1 has significantly larger mesopore volume (0.48 cm{sup 3}/g) than that of conventional TS-1 (0.07 cm{sup 3}/g), and showed a narrow peak centered at ca. 6.3 nm. In the oxidative desulfurization reaction, M-TS-1 was more active than conventional TS-1 at the same Ti-loading; M-TS-1 produced a dibenzothiophene (DBT) conversion of 96%, whereas conventional TS-1 produced a final DBT conversion of 5.6% after a reaction time of 180 min. Oxidative desulfurization over TS-1 was influenced both by electron density and steric hindrance in the sulfur compounds tested.« less

Peering Through the Dust: NuSTAR Observations of Two First-2Mass Red Quasars

NASA Technical Reports Server (NTRS)

Lamassa, Stephanie M.; Ricarte, Angelo; Glikman, Eilat; Urry, C. Megan; Stern, Daniel; Yaqoob, Tahir; Lansbury, George B.; Civano, Francesca; Boggs, Steve E.; Zhang, Will

2016-01-01

Some reddened quasars appear to be transitional objects in the paradigm of merger-induced black hole growth/ galaxy evolution, where a heavily obscured nucleus starts to be unveiled by powerful quasar winds evacuating the surrounding cocoon NuSTAR and XMM-Newton/Chandra observations of FIRST-2MASS-selected red quasars F2M 0830+3759 and F2M 1227+3214. We find that though F2M 0830 +3759 is moderately obscured N(sub H) = (2.1 +/- 0.2) x 10 (exp 22) per square centimeter) and F2M 1227+3214 is mildly absorbed (N(sub H),Z =3.4(+0.8/-0.7) X 10(exp -2) along the line of sight, heavier global obscuration may be present in both sources, with N(sub H) = 3.7 (+4.1/-2.6) X 10 (exp 23) per square centimeter) and less than 5.5 X 10(exp 23) per square centimeter) for F2M 0830+3759 and F2M 1227+ 3214, respectively. F2M 0830+3759 also has an excess of soft X-ray emission below 1 of dust and gas. Hard X-ray observations are able to peer through this gas and dust, revealing the properties of circumnuclear obscuration. Here, we present keV, which is well accommodated by a model where 7% of the intrinsic X-ray emission from the active galactic nucleus (AGN) is scattered into the line of sight. While F2M 1227+3214 has a dust-to-gas ratio (E(B - V)/NH) consistent with the Galactic value, the value of E(B - V)/NH for F2M 0830+3759 is lower than the Galactic standard, consistent with the paradigm that the dust resides on galactic scales while the X-ray reprocessing gas originates within the dust sublimation zone of the broad-line region. The X-ray and 6.1 µm luminosities of these red quasars are consistent with the empirical relations derived for high-luminosity, unobscured quasars, extending the parameter space of obscured AGNs previously observed by NuSTAR to higher luminosities.

SULFUR- AND SILICON-BEARING MOLECULES IN PLANETARY NEBULAE: THE CASE OF M2-48

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

Edwards, J. L.; Ziurys, L. M., E-mail: lziurys@email.arizona.edu

Molecular-line observations of the bipolar planetary nebula (PN) M2-48 have been conducted using the Sub-Millimeter Telescope and the 12 m antenna of the Arizona Radio Observatory at 1, 2, and 3 mm. M2-48 is estimated to be ∼4800 yr old, midway through the PN evolutionary track. SiO and SO{sub 2} were detected in this source—the first identification of either molecule in a PN. CN, HCN, HNC, CS, SO, HCO{sup +}, N{sub 2}H{sup +}, and several {sup 13}C isotopologues such as {sup 13}CN, H{sup 13}CN, and H{sup 13}CO{sup +} were also observed toward this object. A radiative transfer analysis of multiplemore » SiO transitions indicates a gas kinetic temperature of T {sub K} ∼ 55 K and a density of n(H{sub 2}) ∼ 9 × 10{sup 5} cm{sup –3} in M2-48, in agreement with previous CS and CO modeling. After CO, CN, and SO were found to be the most prevalent molecules in this nebula, with fractional abundances, relative to H{sub 2}, of f ∼ 3.8 × 10{sup –7} and 2.4 × 10{sup –7}, respectively. SO{sub 2} and HCN are also abundant, with f ∼ 1.2 × 10{sup –7}, indicating an [SO]/[SO{sub 2}] ratio of ∼2. Relatively high ion abundances were measured in M2-48 as well, with f ∼ 10{sup –7} for both HCO{sup +} and N{sub 2}H{sup +}. An [HCN]/[HNC] ratio of ∼2 was determined, as typically observed in other PNe, independent of age. The high abundances of SO and SO{sub 2}, along with the presence of SiO with f ∼ 2.9 × 10{sup –8}, suggest O/C > 1 in this source; furthermore, the prevalence of CN and N{sub 2}H{sup +} indicates nitrogen enrichment. The {sup 12}C/{sup 13}C ratio of ∼3 in the nebula was also established. These factors indicate hot-bottom burning occurred in the progenitor star of M2-48, suggesting an initial mass > 4 M {sub ☉}.« less

Far-Infrared Spectroscopy of Planetary Nebulae with the KAO

NASA Technical Reports Server (NTRS)

Rubin, Robert H.; Colgan, S.; Haas, M. R.; Lord, S. D.; Simpson, Janet P.

1996-01-01

We present new far-infrared line observations of the planetary nebulae (PNs) NGC 7027, NGC 7009, and NGC 6210 obtained with the Kuiper Airborne Observatory (KAO). The bulk of our data are for NGC 7027 and NGC 7009, including [Ne(V)] 24 micrometers, [O(IV)] 26 micrometers, [O(III)] (52, 88) micrometers, and [N(III)] 57 micrometers. Our data for [O(III)] (52, 88) and [N(III)] 57 in NGC 7027 represent the first measurements of these lines in this source. The large [O(III)] 52/88-micrometer flux ratio implies an electron density (cubic cm) of log N(sub e)[O(III)] = 4.19, the largest Ne ever inferred from these lines. We derive N(++)/O(++) = 0.394 +/- 0.062 for NGC 7027 and 0.179 +/- 0.043 for NGC 6210. We are able to infer the O(+3)/O(++) ionic ratio from our data. As gauged by this ionic ratio, NGC 7027 is substantially higher ionization than is NGC 7009 - consistent with our observation that the former produces copious [Ne(V)] emission while the latter does not. These data help characterize the stellar ionizing radiation field. From our [O(IV)] and [O(III)] fluxes, we are able to show that O(++) is by far the dominant oxygen ion in NGC 7009. As a result, the O/H abundance inferred using these data tends to corroborate the value found from UV/optical, collisionally excited lines. We determined accurate rest wavelengths for the [Ne(V)] 2s(2)2p(2)P(sub 1) to 2s(2)2p(2)3P(sub 0) (lambda(sub rest) = 24.316 +/- 0.008 micrometers) and [O(IV)] 2s(2)2p(2)P(sup 0, sub 3/2) to 2s(2)2p(2)P(sup 0, sub 1/2) (lambda(sub rest) = 25.887 +/- 0.007 micrometers) transitions from observations of one or both of the bright PNs NGC 7027 and NGC 7009. Our [O(IV)] value, to the best of our knowledge, is the most accurate direct determination of this lambda(sub rest). These new KAO data will be beneficial for comparison with ISO observations of these PNs.

Emission intensities and line ratios from a fast neutral helium beam

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

Ahn, J-W.; Craig, D.; Fiksel, G.

2007-08-15

The emission intensities and line ratios from a fast neutral helium beam is investigated in the Madison Symmetric Torus (MST) [R. N. Dexter, D. W. Kerst, T. W. Lovell, S. C. Prager, and J. C. Sprott, Fusion Technol. 19, 131 1991]. Predicted He I line intensities and line ratios from a recently developed collisional-radiative model are compared with experiment. The intensity of singlet lines comes mostly (>95%) from the contribution of the ground state population and is very weakly dependent on the initial metastable fraction at the observation point in the plasma core. On the other hand, the intensity ofmore » triplet lines is strongly affected by the local metastable state (2{sup 1}S and 2{sup 3}S) populations and the initial metastable fraction plays an important role in determining line intensities. The fraction of local metastable states can only be estimated by making use of electron temperature (T{sub e}), electron density (n{sub e}), and effective ion charge (Z{sub eff}) profiles as inputs to the population balance equations. This leads triplet lines to be unusable for the investigation of their local plasma parameter dependence. The ratio of singlet lines at 667.8 nm and 492.2 nm (I{sub 667}/I{sub 492}) as well as the ratio of 667.8 nm and 501.6 nm lines (I{sub 667}/I{sub 501}) has been investigated for the dependence on T{sub e} and n{sub e} both theoretically and experimentally. I{sub 667}/I{sub 492} shows strong dependence on n{sub e} with weak sensitivity to T{sub e}. Measurements and predictions agree quantitatively within a factor of 2. There has been no ratio of singlet lines identified to have strong enough T{sub e} dependence yet. The ratios are expected to be reasonably insensitive to the variation of Z{sub eff}.« less

Considering Combined or Separated Roughness and Vegetation Effects in Soil Moisture Retrievals

NASA Technical Reports Server (NTRS)

Parrens, Marie; Wigernon, Jean-Pierre; Richaume, Philippe; Al Bitar, Ahmad; Mialon, Arnaud; Fernandez-Moran, Roberto; Al-Yarri, Amen; O'Neill, Peggy; Kerr, Yann

2016-01-01

For more than six years, the Soil Moisture and Ocean Salinity (SMOS) mission has provided multi angular and full-polarization brightness temperature (TB) measurements at L-band. Geophysical products such as soil moisture (SM) and vegetation optical depth at nadir (tau(sub nad)) are retrieved by an operational algorithm using TB observations at different angles of incidence and polarizations. However, the quality of the retrievals depends on several surface effects, such as vegetation, soil roughness and texture, etc. In the microwave forward emission model used in the retrievals (L-band Microwave Emission Model, L-MEB),soil roughness is modeled with a semi-empirical equation using four main parameters (Q(sub r), H(sub r), N(sub rp), with p = H or V polarizations). At present, these parameters are calibrated with data provided by airborne studies and in situ measurements made at a local scale that is not necessarily representative of the large SMOS footprints (43 km on average) at global scale. In this study, we evaluate the impact of the calibrated values of N(sub rp) and H(sub r) on the SM and tau(sub nad) retrievals based on SMOS TB measurements (SMOS Level 3 product) over the Soil Climate Analysis Network (SCAN) network located in North America over five years (2011-2015). In this study, Qr was set equal to zero and we assumed that N(sub rH)= N(sub rV). The retrievals were performed by varying N(sub rp) from -1 to 2 by steps of 1 and H(sub r) from 0 to 0.6 by steps of 0.1. At satellite scale, the results show that combining vegetation and roughness effects in a single parameter provides the best results in terms of soil moisture retrievals, as evaluated against the in situ SM data. Even though our retrieval approach was very simplified, as we did not account for pixel heterogeneity, the accuracy we obtained in the SM retrievals was almost systematically better than those of the Level 3 product. Improved results were also obtained in terms of optical depth retrievals. These new results may have key consequences in terms of calibration of roughness effects within the algorithms of the SMOS (ESA) and the SMAP (NASA) space missions.

Method for improving the toughness of silicon carbide-based ceramics

DOEpatents

Tein, T.Y.; Hilmas, G.E.

1996-12-03

Method of improving the toughness of SiC-based ceramics is disclosed. SiC, , AlN, Al{sub 2}O{sub 3} and optionally {alpha}-Si{sub 3}N{sub 4} are hot pressed to form a material which includes AlN polytypoids within its structure. 1 fig.

Examining the impact of heterogeneous nitryl chloride production on air quality across the United States

EPA Science Inventory

The heterogeneous hydrolysis of dinitrogen pentoxide (N₂O₅) has typically been modeled as only producing nitric acid. However, recent field studies have confirmed that the presence of particulate chloride can alter the reaction product to produce nitryl chlo...

Plasma-assisted catalytic storage reduction system

DOEpatents

Penetrante, Bernardino M.; Vogtlin, George E.; Merritt, Bernard T.; Brusasco, Raymond M.

2000-01-01

A two-stage method for NO.sub.x reduction in an oxygen-rich engine exhaust comprises a plasma oxidative stage and a storage reduction stage. The first stage employs a non-thermal plasma treatment of NO.sub.x gases in an oxygen-rich exhaust and is intended to convert NO to NO.sub.2 in the presence of O.sub.2 and hydrocarbons. The second stage employs a lean NO.sub.x trap to convert such NO.sub.2 to environmentally benign gases that include N.sub.2, CO.sub.2, and H.sub.2 O. By preconverting NO to NO.sub.2 in the first stage with a plasma, the efficiency of the second stage for NO.sub.x reduction is enhanced. For example, an internal combustion engine exhaust is connected by a pipe to a first chamber in which a non-thermal plasma converts NO to NO.sub.2 in the presence of O.sub.2 and hydrocarbons, such as propene. A flow of such hydrocarbons (C.sub.x H.sub.y) is input from usually a second pipe into at least a portion of the first chamber. The NO.sub.2 from the plasma treatment proceeds to a storage reduction catalyst (lean NO.sub.x trap) that converts NO.sub.2 to N.sub.2, CO.sub.2, and H.sub.2 O, and includes a nitrate-forming catalytic site. The hydrocarbons and NO.sub.x are simultaneously reduced while passing through the lean-NO.sub.x trap catalyst. The method allows for enhanced NO.sub.x reduction in vehicular engine exhausts, particularly those having relatively high sulfur contents.

Plasma-assisted catalytic storage reduction system

DOEpatents

Penetrante, Bernardino M.; Vogtlin, George E.; Merritt, Bernard T.; Brusasco, Raymond M.

2002-01-01

A two-stage method for NO.sub.x reduction in an oxygen-rich engine exhaust comprises a plasma oxidative stage and a storage reduction stage. The first stage employs a non-thermal plasma treatment of NO.sub.x gases in an oxygen-rich exhaust and is intended to convert NO to NO.sub.2 in the presence of O.sub.2 and hydrocarbons. The second stage employs a lean NO.sub.x trap to convert such NO.sub.2 to environmentally benign gases that include N.sub.2, CO.sub.2, and H.sub.2 O. By preconverting NO to NO.sub.2 in the first stage with a plasma, the efficiency of the second stage for NO.sub.x reduction is enhanced. For example, an internal combustion engine exhaust is connected by a pipe to a first chamber in which a non-thermal plasma converts NO to NO.sub.2 in the presence of O.sub.2 and hydrocarbons, such as propene. A flow of such hydrocarbons (C.sub.x H.sub.y) is input from usually a second pipe into at least a portion of the first chamber. The NO.sub.2 from the plasma treatment proceeds to a storage reduction catalyst (lean NO.sub.x trap) that converts NO.sub.2 to N.sub.2, CO.sub.2, and H.sub.2 O, and includes a nitrate-forming catalytic site. The hydrocarbons and NO.sub.x are simultaneously reduced while passing through the lean-NO.sub.x trap catalyst. The method allows for enhanced NO.sub.x reduction in vehicular engine exhausts, particularly those having relatively high sulfur contents.

Balloon Profiles of Stratospheric NO(sub 2) and HNO(sub 3) for Testing the Heterogeneous Hydrolysis of N(sub 2)O(sub 5) on Sulfate Aerosols

NASA Technical Reports Server (NTRS)

Webster, C. R.; May, R. D.; Allen, M.; Jaegle, L.; McCormick, M. P.

1993-01-01

Simultaneous in situ measurements of stratospheric NO(sub 2), HNO(sub 3), HCI, and CH(sub 4) from 34 to 24 km were made in August 1992 from Palestine, Texas, using the Balloon-borne Laser In-Situ Sensor (BLISS)tunable diode laser spectrometer.

Low temperature annealed amorphous indium gallium zinc oxide (a-IGZO) as a pH sensitive layer for applications in field effect based sensors

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

Kumar, Narendra; Samtel Centre for Display Technologies, Indian Institute of Technology Kanpur, Kanpur-208016; Kumar, Jitendra

The use of a-IGZO instead of the conventional high-k dielectrics as a pH sensitive layer could lead to the simplification of fabrication steps of field effect based devices. In this work, the pH sensitivities of a-IGZO films directly deposited over a SiO{sub 2}/Si surface were studied utilizing electrolyte-insulator-semiconductor (EIS) structures. Annealing of the films was found to affect the sensitivity of the devices and the device with the film annealed at 400 {sup o}C in N{sub 2} ambience showed the better sensitivity, which reduced with further increase in the annealing temperature to 500 {sup o}C. The increased pH sensitivity withmore » the film annealed at 400 {sup o}C in N{sub 2} gas was attributed to the enhanced lattice oxygen ions (based on the XPS data) and improved C-V characteristics, while the decrease in sensitivity at an increased annealing temperature of 500 {sup o}C was attributed to defects in the films as well as the induced traps at the IGZO/SiO{sub 2} interface based on the stretched accumulation and the peak in the inversion region of C-V curves. This study could help to develop a sensor where the material (a-IGZO here) used as the active layer in a thin film transistors (TFTs) possibly could also be used as the pH sensitive layer without affecting the TFT characteristics, and thus obviating the need of high-K dielectrics for sensitivity enhancement.« less

B{sub K}-parameter from N{sub f}=2 twisted mass lattice QCD

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

Constantinou, M.; Panagopoulos, H.; Skouroupathis, A.

2011-01-01

We present an unquenched N{sub f}=2 lattice computation of the B{sub K} parameter which controls K{sup 0}-K{sup 0} oscillations. A partially quenched setup is employed with two maximally twisted dynamical (sea) light Wilson quarks, and valence quarks of both the maximally twisted and the Osterwalder-Seiler variety. Suitable combinations of these two kinds of valence quarks lead to a lattice definition of the B{sub K} parameter which is both multiplicatively renormalizable and O(a) improved. Employing the nonperturbative RI-MOM scheme, in the continuum limit and at the physical value of the pion mass we get B{sub K}{sup RGI}=0.729{+-}0.030, a number well inmore » line with the existing quenched and unquenched determinations.« less

Crystal structure and magnetic properties of '{alpha} Prime Prime -Fe{sub 16}N{sub 2}' containing residual {alpha}-Fe prepared by low-temperature ammonia nitridation

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

Yamashita, S.; Masubuchi, Y.; Nakazawa, Y.

2012-10-15

Slight enhancement of saturation magnetization to 219 A m{sup 2} kg{sup -1} was observed from 199 A m{sup 2} kg{sup -1} for the original {alpha}-Fe on the intermediate nitrided mixture of '{alpha} Prime Prime -Fe{sub 16}N{sub 2}' with residual {alpha}-Fe among the low temperature ammonia nitridation products under 5 T magnetic field at room temperature. The value changed not linearly against the yield as had been expected. Crystal structure refinement indicated that the phase similar to {alpha} Prime Prime -Fe{sub 16}N{sub 2} had deviations on its lattice constants and positional parameters, compared to previously reported values for {alpha} Prime Primemore » -Fe{sub 16}N{sub 2}. Spin-polarized total energy calculations were performed using the projector-augmented wave method as implemented in the Vienna ab-initio simulation package (VASP) to calculate magnetic moment on the refined crystal structure of the intermediate '{alpha} Prime Prime -Fe{sub 16}N{sub 2}'. The calculations supported the observed magnetization enhancement in the intermediate nitridation product. - Graphical abstract: Crystal structural parameters slightly change in the intermediate nitrided '{alpha} Prime Prime -Fe{sub 16}N{sub 2}' from those in {alpha} Prime Prime -Fe{sub 16}N{sub 2} to show the magnetization maxima in the mixture of '{alpha} Prime Prime -Fe{sub 16}N{sub 2}' and the residual {alpha}-F. Highlights: Black-Right-Pointing-Pointer Larger magnetization was observed than the value of Fe{sub 16}N{sub 2} on its intermediate nitrided mixture with residual {alpha}-Fe. Black-Right-Pointing-Pointer The enhancement was related to the crystal structural deviation from Fe{sub 16}N{sub 2} on the intermediate nitride. Black-Right-Pointing-Pointer It was supported by spin-polarized total energy calculation using the deviated structure.« less

Three distinct modes in a surface micro-discharge in atmospheric pressure He + N{sub 2} mixtures

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

Li, Dong; Liu, Dingxin, E-mail: liudingxin@mail.xjtu.edu.cn; He, Tongtong

2015-12-15

A surface micro-discharge in atmospheric pressure He + N{sub 2} mixtures is studied in this paper with an emphasis on the discharge modes. With the N{sub 2} admixture increasing from 0.1% to 20%, the discharge evolves from a spatially diffuse mode to a filamentary mode during positive half-cycles of the applied voltage. However during the negative half-cycles, an additional patterned mode emerges between the diffuse and the filamentary modes, which has not been reported before to exist in surface micro-discharges. In the diffuse and patterned modes, the plasmas cover almost the entirety of the mesh area during one cycle after plasma ignitionmore » in all mesh elements, and the discharge power increases linearly with the applied voltage. In contrast, plasma coverage of the mesh area is only partial in the filamentary mode and the plasma is more unstable with the discharge power increasing exponentially with the applied voltage. As the surface micro-discharge evolves through the three modes, the density of excited species changes significantly, for instance, the density of N{sub 2}{sup +}(B) drops by ∼20-fold from [N{sub 2}] = 0.2% to 20%. The N{sub 2}{sup +}(B) is predicted to be generated mainly through successive processes of Penning ionization by helium metastables and electron-impact excitation of N{sub 2}{sup +}(X), the latter is most responsible for the density decrease of N{sub 2}{sup +}(B) because much more N{sub 2}{sup +}(X) is converted to N{sub 4}{sup +}(X) as the increase of N{sub 2} fraction. Also, the electron density and electron temperature decrease with the discharge mode transition.« less

Simulation of toluene decomposition in a pulse-periodic discharge operating in a mixture of molecular nitrogen and oxygen

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

Trushkin, A. N.; Kochetov, I. V.

The kinetic model of toluene decomposition in nonequilibrium low-temperature plasma generated by a pulse-periodic discharge operating in a mixture of nitrogen and oxygen is developed. The results of numerical simulation of plasma-chemical conversion of toluene are presented; the main processes responsible for C{sub 6}H{sub 5}CH{sub 3} decomposition are identified; the contribution of each process to total removal of toluene is determined; and the intermediate and final products of C{sub 6}H{sub 5}CH{sub 3} decomposition are identified. It was shown that toluene in pure nitrogen is mostly decomposed in its reactions with metastable N{sub 2}(A{sub 3}{Sigma}{sub u}{sup +}) and N{sub 2}(a Primemore » {sup 1}{Sigma}{sub u}{sup -}) molecules. In the presence of oxygen, in the N{sub 2} : O{sub 2} gas mixture, the largest contribution to C{sub 6}H{sub 5}CH{sub 3} removal is made by the hydroxyl radical OH which is generated in this mixture exclusively due to plasma-chemical reactions between toluene and oxygen decomposition products. Numerical simulation showed the existence of an optimum oxygen concentration in the mixture, at which toluene removal is maximum at a fixed energy deposition.« less

Sensor systems for the Altair Lunar Lander:

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

Mariella, R

The Altair Lunar Lander will enable astronauts to learn to live and work on the moon for extended periods of time, providing the experience needed to expand human exploration farther into the solar system. My overriding recommendation: Use independent and complementary [sometimes referred to as 'orthogonal'] techniques to disambiguate confounding/interfering signals. E.g.: a mass spectrometer ['MS'], which currently serves as a Majority Constituent Analyzer ['MCA'] can be very valuable in detecting the presence of a gaseous specie, so long as it falls on a mass-to-charge ratio ['m/z'] that is not already occupied by a majority constituent of cabin air. Considermore » the toxic gas, CO. Both N{sub 2} and CO have parent peaks of m/z = 28, and CO{sub 2} has a fragment peak at m/z = 28 [and at 16 and 12], so the N{sub 2} and CO{sub 2} m/z=28 signals could mask low, but potentially-dangerous levels of CO. However there are numerous surface-sensitive CO detectors, as well as tunable-diode-laser-based CO sensors that could provide independent monitoring of CO. Also, by appending a gas chromatograph ['GC'] as the front-end sample processer, prior to the inlet of the MS, one can rely upon the GC to separate CO from N{sub 2} and CO{sub 2}, providing the crew with another CO monitor. If the Altair Lunar Lander is able to include a Raman-based MCA for N{sub 2}, O{sub 2}, H{sub 2}O, and CO{sub 2}, then each type of MCA would have cross-references, providing more confidence in the ongoing performance of each technique, and decreasing the risk that one instrument might fail to perform properly, without being noticed. See, also Dr. Pete Snyder's work, which states 'An orthogonal technologies sensor system appears to be attractive for a high confidence detection of presence and temporal characterization of bioaerosols.' Another recommendation: Use data fusion for event detection to decrease uncertainty: tie together the outputs from multiple sensing modalities - eNose, solid-state sensors, GC-IMS, GC-MS - via nonlinear algorithms, such as an 'artificial neural net.' MA Ryan at the JPL and Henry Abarbanel at UCSD are possible candidates to implement such an approach.« less

New Global Electron Density Observations from GPS-RO in the D- and E-Region Ionosphere

NASA Technical Reports Server (NTRS)

Wu, Dong L.

2017-01-01

A novel retrieval technique is developed for electron density (N(sub e)) in the D- and E-region (80-120 km) using the high-quality 50-Hz GPS radio occultation (GPS-RO) phase measurements. The new algorithm assumes a slow, linear variation in the F-region background when the GPS-RO passes through the D- and E-region, and extracts the N(sub e) profiles at 80-130 km from the phase advance signal caused by N(sub e). Unlike the conventional Abel function, the new approach produces a sharp N(sub e) weighting function in the lower ionosphere, and the N(sub e) retrievals are in good agreement with the IRI (International Reference Ionosphere) model in terms of monthly maps, zonal means and diurnal variations. The daytime GPS-RO N(sub e) profiles can be well characterized by the alpha-Chapman function of three parameters (N(sub mE), h(sub mE) and H), showing that the bottom of E-region is deepening and sharpening towards the summer pole. At high latitudes the monthly GPS-RO N(sub e) maps at 80-120 km reveal clear enhancement in the auroral zones, more prominent at night, as a result of energetic electron precipitation (EEP) from the outer radiation belt. The D-/E-region auroral N(sub e) is strongly correlated with K(sub p) on a daily basis. The new N(sub e) data allow further comprehensive analyses of the sporadic E (E(sub s)) phenomena in connection with the background N(sub e) in the E-region. The layered (2-10 km) and fluctuated (less than 2 km) E(sub s) components, namely N(sub e_Layer) than N(sub e_Pert), are extracted with respect to the background N( sub e_Region) on a profile-by-profile basis. The N(sub e_Layer) component has a strong but highly-refined peak at approximately 105 km, with an amplitude smaller than N(sub e_Region) approximately by an order of magnitude. The N(sub e_Pert) component, which was studied extensively in the past, is approximately 2 orders of magnitude weaker than N(sub e_Layer). Both N(sub e_Layer) and N(sub e_Pert) are subject to significant diurnal and semidiurnal variations, showing downward progression with local time in amplitude. The 11-year solar cycle dominates the N(sub e) interannual variations, showing larger N(sub e_Region) and N(sub e_Layer) but smaller N(sub e_Pert) amplitudes in the solar maximum years. Enhanced Ne profiles are often observed in the polar winter, showing good correlation with solar proton events (SPEs) and geomagnetic activity. The new methodology offers great potential for retrieving low N(sub e) in the D-region, where radio propagation and communication blackouts can occur due to enhanced ionization. For space weather applications it is recommended for GPSRO operations to raise the top of high-rate data acquisition to approximately 140 km in the future.

Water-soluble titanium alkoxide material

DOEpatents

Boyle, Timothy J.

2010-06-22

A water soluble, water stable, titanium alkoxide composition represented by the chemical formula (OC.sub.6H.sub.6N).sub.2Ti(OC.sub.6H.sub.2(CH.sub.2N(CH.sub.3).sub.2).sub- .3-2,4,6).sub.2 with a theoretical molecular weight of 792.8 and an elemental composition of 63.6% C, 8.1% H, 14.1% N, 8.1% O and 6.0% Ti.

Synthesis and crystal structure of a new 2,6-dimethyl piperazine-1,4-diium perchlorate monohydrate: [C{sub 6}H{sub 16}N{sub 2}](ClO{sub 4}){sub 2} · H{sub 2}O

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

Mleh, C. Ben; Roisnel, T.; Marouani, H., E-mail: houda.marouani@fsb.rnu.tn

2017-03-15

A proton transfer compound 2,6-dimethyl piperazine-1,4-diium perchlorate monohydrate was synthesized by slow evaporation at room temperature using 2,6-dimethyl piperazine as template. The asymmetric unit contains one organic dication, two crystal graphically independent perchlorate anions and one water molecule. Each organic entities is engaged in a large number of bifurcated and non-bifurcated N–H···O (O) and C–H···O hydrogen bonds with different species and enhanced the three dimensional supramolecular network. In addition, the diprotonated piperazine ring adopts a chair conformation with the methyl groups occupying equatorial positions.

Synthesis and photocatalytic properties of TiO{sub 2} nanostructures

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

Xia, X.H.; Liang, Y.; Wang, Z.

2008-08-04

TiO{sub 2} particles, rods, flowers and sheets were prepared by hydrothermal method via adjusting the temperature, the pressure and the concentration of TiCl{sub 4}. The as-prepared TiO{sub 2} powders were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV-vis diffuse reflectance spectra and N{sub 2} adsorption-desorption measurements. It was found that pressure is the most important factor influencing the morphology of TiO{sub 2}. The photocatalytic activity of the products was evaluated by the photodegradation of aqueous brilliant red X-3B solution under UV light. Among the as-prepared nanostructures, the flower-like TiO{sub 2}more » exhibited the highest photocatalytic activity.« less

Degradation of trimethylbenzene isomers by an enrichment culture under N{sub 2}O-reducing conditions

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

Haener, A.; Hoehener, P.; Zeyer, J.

1997-03-01

In mineral oil-contaminated soils and aquifers, monoaromatic hydrocarbons are often a major concern because of high water solubility and toxicity. Under aerobic conditions, these compounds are rapidly mineralized. However, only limited data are available on the anaerobic degradation. This study reports on the growth of an enrichment culture on 1,3,5-trimethylbenzene (TMB) and 1,2,4-TMB under N2O-reducing conditions, and provides carbon mass and electron balances for the biodegradation of 1,3,5-TMB. 43 refs., 3 figs.

Effect of carbonization temperature on the physical and electrochemical properties of supercapacitor electrode from fibers of oil palm empty fruit bunches

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

Ishak, M. M.; Deraman, M., E-mail: madra@ukm.my; Talib, I. A.

Self-adhesive carbon grains (SACG) was prepared from fibers of oil palm empty fruit bunches. The SACG green monoliths were carbonized in N{sub 2} environment at 400, 500, 600 and 700°C to produce carbon monoliths labeled as CM1, CM2, CM3 and CM4 respectively. The CMs were activated in CO{sub 2} surrounding at 800°C for 1 hour to produce activated carbon monolith electrodes (ACM1, ACM2, ACM3 and ACM4). The physical properties of the CMs and ACMs were investigated using X-ray diffraction, field emission scanning electron microscopy (FESEM) and N{sub 2} adsorption-desorption isotherm techniques. ACMs were used as electrode to fabricate symmetry supercapacitormore » cells and the cells’ performances were investigated using electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD) standard techniques. In this paper we report the physical and electrochemical properties of the ACM electrodes by analyzing the influence of the carbonization temperature on these properties.« less

Co-combustion of coal and biomass in a pressurized bubbling fluidized bed

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

Andries, J.; Verloop, M.; Hein, K.

1997-12-31

The use of biomass as an energy source in power plants has advantages compared to fossil fuel firing. Co-firing of biomass and coal offers additional advantages compared to exclusive biomass firing. The objective of the research described in this paper is to assess the effect of co-combustion of biomass (straw or Miscanthus Sinensis) and coal on the behavior of a pressurized fluidized bed combustor with regard to fuel feeding, fluidization, sintering, burnout, temperature distribution and the emission of harmful gaseous and solid components. Temperature and gas concentration profiles have been determined in the freeboard of the Delft 1.6 MW{sub th}more » PFBC test rig. The addition of up to 20% of biomass (based on heat input) has no adverse effect on the PFBC process. The feeding of the biomass is more critical than the feeding of coal, due to the more fibrous structure and the larger volumes of the biomass fuel. Dependent on the process conditions the biomass addition results locally in an increase or decrease of the temperatures. Biomass addition causes a small increase of the CO and NO and a small decrease of N{sub 2}O emissions. The influence of the biomass addition on the HCl emissions is not clear. The lower sulfur content and a larger sulfur capture efficiency result in lower SO{sub 2} emissions. The addition of biomass has a negligible influence on the combustion efficiency. A 15--30% higher cyclone catch was found for the coal/Miscanthus mixture when compared to the other fuels.« less

Insulators obtained by electron cyclotron resonance plasmas on Si or GaAs

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

Diniz, J.A.; Doi, I.; Swart, J.W

2003-03-15

Silicon oxynitride (SiO{sub x}N{sub y}) and nitride (SiN{sub x}) insulators have been deposited or grown (with or without silane in the gas mixture, respectively) by electron cyclotron resonance (ECR) plasmas on Si and/or GaAs substrates at room temperature (20 deg. C) and low pressures (up to 10 mTorr). Chemical bonding characteristics of the SiO{sub x}N{sub y} and SiN{sub x} films were evaluated using Fourier transform infrared spectrometry (FTIR). The profile measurements determined the film thickness, the deposition (or oxidation) rate and the etch rates in buffered HF (BHF). The refractive indexes and the thicknesses were determined by ellipsometry. The effectivemore » interface charge densities were determined by capacitance-voltage (C-V) measurements. With these processes and analyses, different films were obtained and optimized. Suitable gate insulators for metal-insulator-semiconductor (MIS) devices with low interface charge densities were developed: (a) SiN{sub x} films deposited by ECR-chemical vapor deposition (ECR-PECVD) on GaAs substrates; (b) SiO{sub x}N{sub y} insulators obtained by low-energy molecular nitrogen ion ({sup 28}N{sub 2}{sup +}) implantation (energy of 5 keV and dose of 1x10{sup 15}/cm{sup 2}) in Si substrates prior to high-density O{sub 2} ECR plasma oxidation; and (c) SiO{sub x}N{sub y} insulators grown (without silane in the gas mixture) by O{sub 2}/N{sub 2}/Ar ECR plasma 'oxynitridation'. Furthermore, some SiN{sub x} films also present very good masking characteristics for local oxidation of silicon process.« less

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

Barc, B.; Ryszka, M.; Spurrell, J.

Multi-photon ionization (MPI) of the RNA base uracil has been studied in the wavelength range 220–270 nm, coinciding with excitation to the S{sub 2}(ππ*) state. A fragment ion at m/z = 84 was produced by 2-photon absorption at wavelengths ≤232 nm and assigned to C{sub 3}H{sub 4}N{sub 2}O{sup +} following CO abstraction. This ion has not been observed in alternative dissociative ionization processes (notably electron impact) and its threshold is close to recent calculations of the minimum activation energy for a ring opening conical intersection to a σ(n-π)π* closed shell state. Moreover, the predicted ring opening transition leaves a COmore » group at one end of the isomer, apparently vulnerable to abstraction. An MPI mass spectrum of uracil-water clusters is presented for the first time and compared with an equivalent dry measurement. Hydration enhances certain fragment ion pathways (particularly C{sub 3}H{sub 3}NO{sup +}) but represses C{sub 3}H{sub 4}N{sub 2}O{sup +} production. This indicates that hydrogen bonding to water stabilizes uracil with respect to neutral excited-state ring opening.« less

Health-hazard evaluation report HETA 87-063-1808, Presbyterian Day Surgery Center, Albuquerque, New Mexico

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

Daniels, W.J.; Gunter, B.

1987-07-01

In response to a request from employees to evaluate exposures to waste anesthetic gases and vapors at the Presbyterian Day Surgery Unit, located in Albuquerque, New Mexico, personal and area air-sampling and leak-detection testing was carried out for nitrous oxide (N/sub 2/O) and halogenated anesthetic agents in the six operating rooms at the facility. Nitrous oxide concentrations ranged from not detectable to 95 parts per million (ppm) with a mean of 20ppm. Five of the samples exceeded the NIOSH limit of 25ppm for N/sub 2/O during anesthetic administration. Ethrane levels in 14 personal and area air samples ranged from lessmore » than the limit of detection to 3.63ppm with a mean of 0.31ppm. Isoflurane and halothane were below the limits of detection. The ventilation system in use changed the air in excess of 20 times per hour. However, during a portion of surgical procedures the system was not operating, resulting in a higher than normal exposure level in three of the operating rooms.« less

Balloon profiles of stratospheric NO[sub 2] and HNO[sub 3] for testing the heterogeneous hydrolysis of N[sub 2]O[sub 5] on sulfate aerosols

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

Webster, C.R.; May, R.D.; Allen, M.

1994-01-01

Simultaneous in situ measurements of stratospheric NO[sub 2], HNO[sub 3], HCl, and CH[sub 4] from 34 to 24 km were made in August 1992 from Palestine, Texas, using the Balloon-borne Laser In-Situ Sensor (BLISS) tunable diode laser spectrometer. Although the measurements of NO[sub 2], HNO[sub 3], and NO[sub 2]/HNO[sub 3] agree well with gas-phase model calculations near 34 km where SAGE II data show little sulfate aerosol, this is not true at the lower altitudes where SAGE II shows high aerosol loadings. At 24 km the BLISS NO[sub 2] and HNO[sub 3] measurements are 70% lower, and 50% higher, respectively,more » than the gas phase model predictions, with a measured NO[sub 2]/HNO[sub 3] ratio 5 times smaller. When the heterogeneous hydrolysis of N[sub 2]O[sub 5] and ClONO[sub 2] on sulfate aerosol of surface area densities matching the SAGE II measurements is added to the model, good agreement with the BLISS measurements is found over the whole altitude range. 24 refs., 4 figs., 1 tab.« less

Successful N{sub 2} leptogenesis with flavour coupling effects in realistic unified models

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

Bari, Pasquale Di; King, Stephen F.

2015-10-02

In realistic unified models involving so-called SO(10)-inspired patterns of Dirac and heavy right-handed (RH) neutrino masses, the lightest right-handed neutrino N{sub 1} is too light to yield successful thermal leptogenesis, barring highly fine tuned solutions, while the second heaviest right-handed neutrino N{sub 2} is typically in the correct mass range. We show that flavour coupling effects in the Boltzmann equations may be crucial to the success of such N{sub 2} dominated leptogenesis, by helping to ensure that the flavour asymmetries produced at the N{sub 2} scale survive N{sub 1} washout. To illustrate these effects we focus on N{sub 2} dominatedmore » leptogenesis in an existing model, the A to Z of flavour with Pati-Salam, where the neutrino Dirac mass matrix may be equal to an up-type quark mass matrix and has a particular constrained structure. The numerical results, supported by analytical insight, show that in order to achieve successful N{sub 2} leptogenesis, consistent with neutrino phenomenology, requires a “flavour swap scenario” together with a less hierarchical pattern of RH neutrino masses than naively expected, at the expense of some mild fine-tuning. In the considered A to Z model neutrino masses are predicted to be normal ordered, with an atmospheric neutrino mixing angle well into the second octant and the Dirac phase δ≃20{sup ∘}, a set of predictions that will be tested in the next years in neutrino oscillation experiments. Flavour coupling effects may be relevant for other SO(10)-inspired unified models where N{sub 2} leptogenesis is necessary.« less

Confinement induced binding of noble gas atoms

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

Khatua, Munmun; Pan, Sudip; Chattaraj, Pratim K., E-mail: pkc@chem.iitkgp.ernet.in

2014-04-28

The stability of Ng{sub n}@B{sub 12}N{sub 12} and Ng{sub n}@B{sub 16}N{sub 16} systems is assessed through a density functional study and ab initio simulation. Although they are found to be thermodynamically unstable with respect to the dissociation of individual Ng atoms and parent cages, ab initio simulation reveals that except Ne{sub 2}@B{sub 12}N{sub 12} they are kinetically stable to retain their structures intact throughout the simulation time (500 fs) at 298 K. The Ne{sub 2}@B{sub 12}N{sub 12} cage dissociates and the Ne atoms get separated as the simulation proceeds at this temperature but at a lower temperature (77 K) itmore » is also found to be kinetically stable. He-He unit undergoes translation, rotation and vibration inside the cavity of B{sub 12}N{sub 12} and B{sub 16}N{sub 16} cages. Electron density analysis shows that the He-He interaction in He{sub 2}@B{sub 16}N{sub 16} is of closed-shell type whereas for the same in He{sub 2}@B{sub 12}N{sub 12} there may have some degree of covalent character. In few cases, especially for the heavier Ng atoms, the Ng-N/B bonds are also found to have some degree of covalent character. But the Wiberg bond indices show zero bond order in He-He bond and very low bond order in cases of Ng-N/B bonds. The energy decomposition analysis further shows that the ΔE{sub orb} term contributes 40.9% and 37.3% towards the total attraction in the He{sub 2} dimers having the same distances as in He{sub 2}@B{sub 12}N{sub 12} and He{sub 2}@B{sub 16}N{sub 16}, respectively. Therefore, confinement causes some type of orbital interaction between two He atoms, which akins to some degree of covalent character.« less

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

Banerjee, Surajit; Christov, Plamen P.; Kozekova, Albena

trans-4-Hydroxynonenal (HNE) is the major peroxidation product of {omega}-6 polyunsaturated fatty acids in vivo. Michael addition of the N{sub 2}-amino group of dGuo to HNE followed by ring closure of N1 onto the aldehyde results in four diastereomeric 1,N{sub 2}-dGuo (1,N{sub 2}-HNE-dGuo) adducts. The (6S,8R,11S)-HNE-1,N{sub 2}-dGuo adduct was incorporated into the 18-mer templates 5'-d(TCATXGAATCCTTCCCCC)-3' and d(TCACXGAATCCTTCCCCC)-3', where X = (6S,8R,11S)-HNE-1,N{sub 2}-dGuo adduct. These differed in the identity of the template 5'-neighbor base, which was either Thy or Cyt, respectively. Each of these templates was annealed with either a 13-mer primer 5'-d(GGGGGAAGGATTC)-3' or a 14-mer primer 5'-d(GGGGGAAGGATTCC)-3'. The addition of dNTPsmore » to the 13-mer primer allowed analysis of dNTP insertion opposite to the (6S,8R,11S)-HNE-1,N{sub 2}-dGuo adduct, whereas the 14-mer primer allowed analysis of dNTP extension past a primed (6S,8R,11S)-HNE-1,N{sub 2}-dGuo:dCyd pair. The Sulfolobus solfataricus P2 DNA polymerase IV (Dpo4) belongs to the Y-family of error-prone polymerases. Replication bypass studies in vitro reveal that this polymerase inserted dNTPs opposite the (6S,8R,11S)-HNE-1,N{sub 2}-dGuo adduct in a sequence-specific manner. If the template 5'-neighbor base was dCyt, the polymerase inserted primarily dGTP, whereas if the template 5'-neighbor base was dThy, the polymerase inserted primarily dATP. The latter event would predict low levels of Gua {yields} Thy mutations during replication bypass when the template 5'-neighbor base is dThy. When presented with a primed (6S,8R,11S)-HNE-1,N{sub 2}-dGuo:dCyd pair, the polymerase conducted full-length primer extension. Structures for ternary (Dpo4-DNA-dNTP) complexes with all four template-primers were obtained. For the 18-mer:13-mer template-primers in which the polymerase was confronted with the (6S,8R,11S)-HNE-1,N{sub 2}-dGuo adduct, the (6S,8R,11S)-1,N{sub 2}-dGuo lesion remained in the ring-closed conformation at the active site. The incoming dNTP, either dGTP or dATP, was positioned with Watson-Crick pairing opposite the template 5'-neighbor base, dCyt or dThy, respectively. In contrast, for the 18-mer:14-mer template-primers with a primed (6S,8R,11S)-HNE-1,N{sub 2}-dGuo:dCyd pair, ring opening of the adduct to the corresponding N{sub 2}-dGuo aldehyde species occurred. This allowed Watson-Crick base pairing at the (6S,8R,11S)-HNE-1,N{sub 2}-dGuo:dCyd pair.« less

Hydrogen sensors based on Sc2O3/AlGaN/GaN high electron mobility transistors

NASA Astrophysics Data System (ADS)

Kang, B. S.; Mehandru, R.; Kim, S.; Ren, F.; Fitch, R. C.; Gillespie, J. K.; Moser, N.; Jessen, G.; Jenkins, T.; Dettmer, R.; Via, D.; Crespo, A.; Baik, K. H.; Gila, B. P.; Abernathy, C. R.; Pearton, S. J.

2005-05-01

Pt contacted AlGaN/GaN high electron mobility transistors with Sc2O3 gate dielectrics show reversible changes in drain-source current upon exposure to H2-containing ambients, even at room temperature. The changes in current (as high as 3 mA for relatively low gate voltage and drain-source voltage at 25 °C for the HEMTs and a change in forward current of 40 μA at a bias of 2.5 V was obtained for the MOS-diodes in response to a change in ambient from pure N2 to 10% H2/90% N2. The current changes in the latter case are almost linearly proportional to the testing temperature and reach around 400 μA at 400 °C. These signals are approximately an order of magnitude larger than for Pt /GaN Schottky diodes and a factor of 5 larger than Sc2O3/AlGaN/GaN metal-oxide semiconductor (MOS) diodes exposed under the same conditions. This shows the advantage of using a transistor structure in which the gain produces larger current changes upon exposure to hydrogen-containing ambients. The increase in current is the result of a decrease in effective barrier height of the MOS gate of 30-50 mV at 25 °C for 10%H2/90%N₂ ambients relative to pure N₂ and is due to catalytic dissociation of the H₂ on the Pt contact, followed by diffusion to the Sc₂O₃/AlGaN interface.

Crystal structure of 1-methyl-3-([2,2-dimethyl-4,6-dioxo-1,3-dioxane-5-ylidene]methyl)urea

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

Habibi, A., E-mail: habibi@khu.ac.ir; Ghorbani, H. S.; Bruno, G.

2013-12-15

The crystal structure of 1-Methyl-3-([2,2-dimethyl-4,6-dioxo-1,3-dioxane-5-ylidene]methyl)urea (C{sub 9}H{sub 12}N{sub 2}O{sub 5}) has been determined by single crystal X-ray diffraction analysis. The crystals are monoclinic, a = 5.3179(2), b = 18.6394(6), c =10.8124(3) Å, β = 100.015(2)°, Z = 4, sp. gr. P2{sub 1}/c, R = 0.0381 for 2537 reflections with I > 2σ(I). Except for C(CH{sub 3}){sub 2} group, the molecule is planar. The structure is stabilized by inter- and intramolecular N-H...O hydrogen bonds and weak C-H...O interactions.

Hydrothermal synthesis of zinc(II)-phosphonate coordination polymers with different dimensionality (0D, 2D, 3D) and dimensionality change in the solid phase (0D→3D) induced by temperature

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

Fernández-Zapico, Eva; Montejo-Bernardo, Jose; Fernández-González, Alfonso

2015-05-15

Three new zinc(II) coordination polymers, [Zn(HO{sub 3}PCH{sub 2}CH{sub 2}COO)(C{sub 12}H{sub 8}N{sub 2})(H{sub 2}O)] (1), [Zn{sub 3}(O{sub 3}PCH{sub 2}CH{sub 2}COO){sub 2}(C{sub 12}H{sub 8}N{sub 2})](H{sub 2}O){sub 3.40} (2) and [Zn{sub 5}(HO{sub 3}PCH{sub 2}CH{sub 2}COO){sub 2}(O{sub 3}PCH{sub 2}CH{sub 2}COO){sub 2}(C{sub 12}H{sub 8}N{sub 2}){sub 4}](H{sub 2}O){sub 0.32} (3), with different structural dimensionality (0D, 2D and 3D, respectively) have been prepared by hydrothermal synthesis, and their structures were determined by single-crystal X-ray diffraction. Compound 1 crystallizes in the monoclinic system (P2{sub 1}/c) forming discrete dimeric units bonded through H-bonds, while compounds 2 and 3 crystallize in the triclinic (P−1) and the monoclinic (C2/c) systems, respectively.more » Compound 3, showing three different coordination numbers (4, 5 and 6) for the zinc atoms, has also been obtained by thermal treatment of 1 (probed by high-temperature XRPD experiments). The crystalline features of these compounds, related to the coordination environments for the zinc atoms in each structure, provoke the increase of the relative fluorescence for 2 and 3, compared to the free phenanthroline. Thermal analysis (TG and DSC) and XPS studies have been also carried out for all compounds. - Graphical abstract: Three new coordination compounds of zinc with 2-carboxyethylphosphonic acid (H{sub 2}PPA) and phenanthroline have been obtained by hydrothermal synthesis. The crystalline structure depends on the different coordination environments of the zinc atoms (see two comparative Zn{sub 6}-moieties). The influence of the different coordination modes of H{sub 2}PPA with the central atom in all structures have been studied, being found new coordination modes for this ligand. Several compounds show a significant increase in relative fluorescence with respect to the free phenanthroline. - Highlights: • Compounds have been obtained modifying the reaction time and the rate of reagents. • Dimensionality and crystalline structure is a function of the zinc environments. • New coordination modes for 2-carboxyethylphosphonic acid are reported. • 3D-compound presents three different coordination environments for the zinc atoms. • Fluorescence properties are related to the structural dimensionality.« less

Correlations between critical current density, j{sub c}, critical temperature, T{sub c}, and structural quality of Y{sub 1}B{sub 2}Cu{sub 3}O{sub 7-x} thin superconducting films

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

Chrzanowski, J.; Xing, W.B.; Atlan, D.

1994-12-31

Correlations between critical current density (j{sub c}) critical temperature (T{sub c}) and the density of edge dislocations and nonuniform strain have been observed in YBCO thin films deposited by pulsed laser ablation on (001) LaAlO{sub 3} single crystals. Distinct maxima in j{sub c} as a function of the linewidths of the (00{ell}) Bragg reflections and as a function of the mosaic spread have been found in the epitaxial films. These maxima in j{sub c} indicate that the magnetic flux lines, in films of structural quality approaching that of single crystals, are insufficiently pinned which results in a decreased critical currentmore » density. T{sub c} increased monotonically with improving crystalline quality and approached a value characteristic of a pure single crystal. A strong correlation between j{sub c} and the density of edge dislocations N{sub D} was found. At the maximum of the critical current density the density of edge dislocations was estimated to be N{sub D}{approximately}1-2 x 10{sup 9}/cm{sup 2}.« less

Electron-impact dissociative excitation and ionization of N{sub 2}D{sup +}

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

Fogle, M.; Bahati, E. M.; Bannister, M. E.

Absolute cross sections for electron-impact dissociation of N{sub 2}D{sup +} producing N{sub 2}{sup +}, ND{sup +}, and N{sup +} ion fragments were measured in the 5- to 100-eV range using a crossed electron-ion beams technique. In the 5- to 20-eV region, in which dissociative excitation (DE) is the principal contributing mechanism, N{sub 2}{sup +} production dominates. The N{sub 2}{sup +} + D dissociation channel shows a large resonant-like structure in the DE cross section, as observed previously in electron impact dissociation of triatomic dihydride species [M. Fogle, E. M. Bahati, M. E. Bannister, S. H. M. Deng, C. R. Vane,more » R. D. Thomas, and V. Zhaunerchyk, Phys. Rev. A 82, 042720 (2010)]. In the dissociative ionization (DI) region, 20- to 100-eV, N{sub 2}{sup +}, ND{sup +}, and N{sup +} ion fragment production are comparable. The observance of the ND{sup +} and N{sup +} ion fragments indicate breaking of the N - N bond along certain dissociation channels.« less

Comparing the greenhouse gas emissions from three alternative waste combustion concepts

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

Vainikka, Pasi, E-mail: pasi.vainikka@vtt.fi; Tsupari, Eemeli; Sipilae, Kai

2012-03-15

Highlights: Black-Right-Pointing-Pointer Significant GHG reductions are possible by efficient WtE technologies. Black-Right-Pointing-Pointer CHP and high power-to-heat ratio provide significant GHG savings. Black-Right-Pointing-Pointer N{sub 2}O and coal mine type are important in LCA GHG emissions of FBC co-combustion. Black-Right-Pointing-Pointer Substituting coal and fuel oil by waste is beneficial in electricity and heat production. Black-Right-Pointing-Pointer Substituting natural gas by waste may not be reasonable in CHP generation. - Abstract: Three alternative condensing mode power and combined heat and power (CHP) waste-to-energy concepts were compared in terms of their impacts on the greenhouse gas (GHG) emissions from a heat and power generation system.more » The concepts included (i) grate, (ii) bubbling fluidised bed (BFB) and (iii) circulating fluidised bed (CFB) combustion of waste. The BFB and CFB take advantage of advanced combustion technology which enabled them to reach electric efficiency up to 35% and 41% in condensing mode, respectively, whereas 28% (based on the lower heating value) was applied for the grate fired unit. A simple energy system model was applied in calculating the GHG emissions in different scenarios where coal or natural gas was substituted in power generation and mix of fuel oil and natural gas in heat generation by waste combustion. Landfilling and waste transportation were not considered in the model. GHG emissions were reduced significantly in all of the considered scenarios where the waste combustion concepts substituted coal based power generation. With the exception of condensing mode grate incinerator the different waste combustion scenarios resulted approximately in 1 Mton of fossil CO{sub 2}-eq. emission reduction per 1 Mton of municipal solid waste (MSW) incinerated. When natural gas based power generation was substituted by electricity from the waste combustion significant GHG emission reductions were not achieved.« less

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

Nagai, Daisuke; Kinemuchi, Yoshiaki, E-mail: y.kinemuchi@aist.go.jp; Suzuki, Kazuyuki

Alpha″-Fe{sub 16}N{sub 2} nanoparticles (NPs) with high magnetic crystalline anisotropy are useful for practical applications such as recording media. However, due to their strongly aggregated and/or sintered form, which occurs during synthesis, the utilization of the NPs has been limited thus far. Here, we report a method for synthesizing highly dispersive α″-Fe{sub 16}N{sub 2} NPs using hydroxyapatite (HAp). The chemically and thermally stable structure of the HAp coating results in the isolation of individual NPs, such that sintering is prevented during synthesis. Additionally, the acicular shape of the HAp crystal did not hinder gas diffusion during the gas reaction. Finally,more » HAp can be removed by a chelating agent without deteriorating the magnetic properties, resulting in highly dispersive α″-Fe{sub 16}N{sub 2} NPs. - Graphical abstract: Synthesis process of highly dispersive α″-Fe{sub 16}N{sub 2} particles using hydroxyapatite coating and SEM images of nanoparticles. - Highlights: • Highly dispersed α″-Fe{sub 16}N{sub 2} NPs were synthesized using hydroxyapatite (HAp). • HAp coating was stable chemically and thermally during gas reaction of α″-Fe{sub 16}N{sub 2} synthesis. • The magnetic property of the resultant Fe{sub 16}N{sub 2} NPs are M{sub s} of 170 emu/g and H{sub C} of 2450 Oe.« less

State selected ion--molecule reactions by a TESICO technique. V. N/sub 2//sup +/(v)+Ar. -->. N/sub 2/+Ar/sup +/

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

Kato, T.; Tanaka, K.; Koyano, I.

1982-07-15

Charge transfer reactions N/sub 2//sup +/(v)+Ar..-->..Ar/sup +/+N/sub 2/ (1) have been studied by selecting the vibrational states of N/sub 2//sup +/ using the threshold electron--secondary ion coincidence (TESICO) technique. Relative cross sections sigma(v) for the individual vibrational states v = 0--3 have been determined at three collision energies, 0.3, 1.5, and 11.8 eV. Results show that Reaction (1), which is endoergic for v = 0, is considerably enhanced by the vibrational excitation of N/sub 2//sup +/ at all collision energies. While excitation of one vibrational quantum enhances the cross section substantially, excitation of additional quanta further increases the cross sectionmore » up to v = 3. The ratios sigma(2)/sigma(1) and sigma(3)/sigma(2) are, however, much smaller than sigma(1)/sigma(0) and are significantly larger at the highest collision energy than at the other two collision energies. These results are discussed in conjunction with the calculated results based on the simple two-state theory of Rapp and Francis and the Franck--Condon factors.« less

Search with COPERNICUS for interstellar N/sub 2/ in diffuse clouds

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

Lutz, B.L.; Owen, T.; Snow, T.P. Jr.

1979-01-01

Multiple Copernicus scans of the rho'/sup 1/..sigma../sub u//sup +/--X/sup 1/..sigma../sub g//sup +/(0--0) and l/sup 1/Pi/sub u/--X/sup 1/..sigma../sub g//sup +/(0--0) band regions of N/sub 2/ in the spectra of delta Sco and epsilon Per result in upper limits of N (N/sub 2/) < or =1.0--3.8 x 10/sup 12/ cm/sup -2/ and N (N/sub 2/) < or =1.2--4.4 x 10/sup 12/ cm/sup -2/, respectively, depending upon the cloud temperature. These limits are consistent with the column densities expected from current chemical models for diffuse interstellar clouds, representing relative abundances with respect to hydrogen nuclei of N (N/sub 2/)/2N (H/sub 2/)+N (H I)more » < or =0.69--2.6 x 10/sup -9/ for delta Sco and < or =0.31--1.1 x 10/sup -8/ for epsilon Per.« less

The Electron Bernstein Waves Heating Project In The TJ-II Stellarator

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

Fernandez, A.; Cappa, A.; Castejon, F.

2007-09-28

TJ-II is a middle sized flexible Heliac operating in Madrid, whose plasmas are created and heated by ECRH via two 300 kW gyrotrons at second harmonic X-mode (53.2 GHz). Neutral beam injection is used for second phase heating. Since the cut off density for the 2nd harmonic X-mode (n{sub c} = 1.7x10 {sup 19} m{sup -3}) is reached during NBI, EBWs are considered both for providing additional heating after NBI switch on and to perform kinetic studies in high-density plasmas. Previous work has shown that the most suitable scheme for launching EBWs in TJ-II is O-X-B mode conversion, which hasmore » acceptable heating efficiency for central densities above 1.2x10{sup 19} m{sup -3}, with an operating frequency of 28 GHz. In this work, the most relevant theoretical calculations are presented, including the relativistic effects both in ray trajectory and absorption, as well as the results of the optimization of the beam parameters that provide the maximum O-X conversion efficiency at the critical layer. A system based on a 28 GHz-100 ms diode gyrotron will be used to deliver 300 kW through a corrugated waveguide. The microwave beam is directed and focused by a steerable mirror located inside the vacuum vessel. A diagnostic for measuring the EBW emission has been designed and tested on the bench. It uses a section of corrugated waveguide and a glass lens to focus the emission from the plasma into the aperture of a dual polarized quad-ridged horn. It will allow us to determine the EBW mode conversion efficiency, and also provides an indication of the electron temperature evolution in overdense plasmas.« less

Chemical changes in carbon Nanotube-Nickel/Nickel Oxide Core/Shell nanoparticle heterostructures treated at high temperatures

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

Chopra, Nitin, E-mail: nchopra@eng.ua.edu; McWhinney, Hylton G.; Shi Wenwu

2011-06-15

Heterostructures composed of carbon nanotube (CNT) coated with Ni/NiO core/shell nanoparticles (denoted as CNC heterostructures) were synthesized in a wet-chemistry and single-step synthesis route involving direct nucleation of nanoparticles on CNT surface. Two different aspects of CNC heterostructures were studied here. First, it was observed that the nanoparticle coatings were more uniform on the as-produced and non-purified CNTs compared to purified (or acid treated) CNTs. These heterostructures were characterized using electron microscopy, Raman spectroscopy, and energy dispersive spectroscopy. Second, thermal stability of CNC heterostructures was studied by annealing them in N{sub 2}-rich (O{sub 2}-lean) environment between 125 and 750 deg.more » C for 1 h. A detailed X-ray photoelectron spectroscopy and Raman spectroscopy analysis was performed to evaluate the effects of annealing temperatures on chemical composition, phases, and stability of the heterostructures. It was observed that the CNTs present in the heterostructures completely decomposed and core Ni nanoparticle oxidized significantly between 600 and 750 deg. C. - Research Highlights: {yields} Heterostructures composed of CNTs coated with Ni/NiO core/shell nanoparticles. {yields} Poor nanoparticle coverage on purified CNT surface compared to non-purified CNTs. {yields} CNTs in heterostructures decompose between 600 and 750 deg. C in N{sub 2}-rich atmosphere. {yields} Metallic species in heterostructures were oxidized at higher temperatures.« less

Calorimetric gas sensor

DOEpatents

Ricco, A.J.; Hughes, R.C.; Smith, J.H.; Moreno, D.J.; Manginell, R.P.; Senturia, S.D.; Huber, R.J.

1998-11-10

A combustible gas sensor is described that uses a resistively heated, noble metal-coated, micromachined polycrystalline Si filament to calorimetrically detect the presence and concentration of combustible gases. The filaments tested to date are 2 {micro}m thick {times} 10{micro}m wide {times} 100, 250, 500, or 1000 {micro}m-long polycrystalline Si; some are overcoated with a 0.25 {micro}m-thick protective CVD Si{sub 3}N{sub 4} layer. A thin catalytic Pt film was deposited by CVD from the precursor Pt(acac){sub 2} onto microfilaments resistively heated to approximately 500 C; Pt deposits only on the hot filament. Using a constant-resistance-mode feedback circuit, Pt-coated filaments operating at ca. 300 C (35 mW input power) respond linearly, in terms of the change in supply current required to maintain constant resistance (temperature), to H{sub 2} concentrations between 100 ppm and 1% in an 80/20 N{sub 2}/O{sub 2} mixture. Other catalytic materials can also be used. 11 figs.

Calorimetric gas sensor

DOEpatents

Ricco, Antonio J.; Hughes, Robert C.; Smith, James H.; Moreno, Daniel J.; Manginell, Ronald P.; Senturia, Stephen D.; Huber, Robert J.

1998-01-01

A combustible gas sensor that uses a resistively heated, noble metal-coated, micromachined polycrystalline Si filament to calorimetrically detect the presence and concentration of combustible gases. The filaments tested to date are 2 .mu.m thick.times.10 .mu.m wide.times.100, 250, 500, or 1000 .mu.m-long polycrystalline Si; some are overcoated with a 0.25 .mu.m-thick protective CVD Si.sub.3 N.sub.4 layer. A thin catalytic Pt film was deposited by CVD from the precursor Pt(acac).sub.2 onto microfilaments resistively heated to approximately 500.degree. C.; Pt deposits only on the hot filament. Using a constant-resistance-mode feedback circuit, Pt-coated filaments operating at ca. 300.degree. C. (35 mW input power) respond linearly, in terms of the change in supply current required to maintain constant resistance (temperature), to H.sub.2 concentrations between 100 ppm and 1% in an 80/20 N.sub.2 /O.sub.2 mixture. Other catalytic materials can also be used.

Detection of interstellar N2O: A new molecule containing an N-O bond

NASA Technical Reports Server (NTRS)

Ziurys, L. M.; Apponi, A. J.; Hollis, J. M.; Snyder, L. E.

1994-01-01

A new interstellar molecule, N2O, known as nitrous oxide or 'laughing gas,' has been detected using the NRAO 12 m telescope. The J = 3 - 2, 4 - 3, 5 - 4, and 6 - 5 rotational transitions of this species at 75, 100, 125, and 150 GHz, respectively, were observed toward Sgr B2(M). The column density derived for N2O in this source is N(sub tot) approx. 10(exp 15)/sq. cm, which corresponds to a fractional abundance of approx. 10(exp -9), relative to H2. This value implies abundance ratios of N2O/NO approx. 0.1 and N2O/HNO approx. 3 in the Galactic center. Such ratios are in excellent agreement with predictions of ion-molecule models of interstellar chemistry using early-time calculations and primarily neutral-neutral reactions. N2O is the third interstellar molecule detected thus far containing an N-O bond. Such bonds cannot be so rare as previously thought.

High-k shallow traps observed by charge pumping with varying discharging times

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

Ho, Szu-Han; Chen, Ching-En; Tseng, Tseung-Yuen

2013-11-07

In this paper, we investigate the influence of falling time and base level time on high-k bulk shallow traps measured by charge pumping technique in n-channel metal-oxide-semiconductor field-effect transistors with HfO{sub 2}/metal gate stacks. N{sub T}-V{sub high} {sub level} characteristic curves with different duty ratios indicate that the electron detrapping time dominates the value of N{sub T} for extra contribution of I{sub cp} traps. N{sub T} is the number of traps, and I{sub cp} is charge pumping current. By fitting discharge formula at different temperatures, the results show that extra contribution of I{sub cp} traps at high voltage are inmore » fact high-k bulk shallow traps. This is also verified through a comparison of different interlayer thicknesses and different Ti{sub x}N{sub 1−x} metal gate concentrations. Next, N{sub T}-V{sub high} {sub level} characteristic curves with different falling times (t{sub falling} {sub time}) and base level times (t{sub base} {sub level}) show that extra contribution of I{sub cp} traps decrease with an increase in t{sub falling} {sub time}. By fitting discharge formula for different t{sub falling} {sub time}, the results show that electrons trapped in high-k bulk shallow traps first discharge to the channel and then to source and drain during t{sub falling} {sub time}. This current cannot be measured by the charge pumping technique. Subsequent measurements of N{sub T} by charge pumping technique at t{sub base} {sub level} reveal a remainder of electrons trapped in high-k bulk shallow traps.« less

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

Zhang Hongxia; Feng Jing; Zhang Milin

A novel CuO electrode material with flower-like nanostructures was fabricated at a low temperature (80 deg. C) by a simple chemical precipitation method. Scanning electron microscopy (SEM) results showed that CuO with spherical and flower-like structure can be formed under a weak alkali (C{sub 6}H{sub 12}N{sub 4}), and CuO with sheets structure can be obtained under a strong alkali (NaOH). A possible growth mechanism of CuO nanocrystals was discussed. The flower-like CuO electrode exhibited a higher specific capacitance (133.6 Fg{sup -1}) and an excellent cycle performance at a high current density of 10 mA/cm{sup 2}. Specific capacitance of flower-like CuOmore » was 405.3% higher than globular CuO (26.44 Fg{sup -1}) at 2 mA/cm{sup 2}.« less

The microstructure and tensile properties of nitrogen containing vacuum atomized Alloy 690

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

Fuchs, G.E.; Hayden, S.Z.

1991-02-01

The mechanical properties and microstructure of a heat of nitrogen containing vacuum atomized A690 have been characterized. Although wrought A690 exhibits extensive grain growth during solution annealing heat treatments, only limited grain growth was observed in P/M690N{sub 2}. The presence of the nitrogen in the P/M690N{sub 2} resulted in the formation of a fine dispersion of Ti(C,N) which limited grain growth during elevated temperature exposures. The yield and ultimate tensile strength of the P/M690N{sub 2} was significantly greater than wrought A690 and elevated temperature exposures did not greatly affect the properties of the P/M690N{sub 2}. Although the P/M690N{sub 2} didmore » exhibit appreciably higher strengths than wrought A690, the ductility was not adversely affected. In general, the resulting microstructure and, hence, mechanical properties of the P/M690N{sub 2} were very stable, uniform, and reproducible, even after long-term elevated temperature exposures of up to 24 hours at 1100{degree}C. 14 refs., 5 figs., 1 tab.« less

3-(2-Biphenyl)sydnone

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

Riddle, Gordon B.; Grossie, David A.; Turnbull, Kenneth

2010-11-16

The title compound, C{sub 14}H{sub 10}N{sub 2}O{sub 2}, is one of many sydnones which have been synthesized in order to investigate the influence of substituents and sydnone-ring stability. There is medicinal interest in the sydnone if the ring can predictably release NO. Bond lengths and angles of the sydnone ring were compared with those of other published sydnone compounds and were found to fit the average of the published data.

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

Attig, R.C.; Crawford, L.W.; Lynch, T.P.

Proof-of-Concept (POC) scale demonstration of such technology is currently being carried out at the US Department of Energy's (DOE's) Coal-Fired Flow Facility (CFFF), located at The University of Tennessee Space Institute (UTSI) in Tullahoma, Tennessee and at the Component Development and Integration Facility in Butte, Montana. The CFFF is dedicated to the evaluation of downstream (steam cycle) components and technology that may be considered for a full-scale MHD system. The objectives of the CFFF testing include the demonstration of various pollution control devices and techniques at a scale sufficient for future scale-up. The CFFF offers a unique test environment inmore » which emissions control techniques can be developed and evaluated through emissions and environmental monitoring. Results thus far have demonstrated the ability of sulfur oxide (SO{sub x}), nitrogen oxide (NO{sub x}) and particulate emissions well below the New Source Performance Standards (NSPS). Regeneration of the potassium sulfate to produce sulfur-free compounds also has been demonstrated. The experimental program at the CFFF is now aimed at determining the optimum conditions for future commercial scale designs. Because of increased interests in Air Toxics, measurements of nitrous oxide (N{sub 2}O), a potential greenhouse gas, priority pollutants (inorganic as well as organics), and chlorine-containing species (Cl{sub 2} and HCl) are also included in our ongoing efforts. Environmental monitoring activities are being pursued to develop an environmental impact assessment data base. These include the use of three ambient air sites to determine the impacts of gaseous and particulate emissions, five lake water sites to determine impacts due to process water discharges and seven sites to collect terrestrial data on possible soil contamination and tree growth. In this paper, we will summarize the status of our ongoing environmental program. 16 refs., 15 figs., 3 tabs.« less

Formaldehyde activation factor, tetrahydromethanopterin, a coenzyme of methanogenesis

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

Escalante-Semerena, J.C.; Leigh, J.A.; Rinehart, K.L. Jr.

1984-04-01

An oxygen-labile formaldehyde activation factor (FAF) was isolated in highly purified form by use of anoxic fractionation procedures. The molecular weight of FAF was determined to be 776 and that of methanopterin (MPT) 772 by fast-atom-bombardment mass spectrometry (FABMS). High-resolution FABMS measurements on MPT and FAF indicated molecular formulas of C/sub 30/H/sub 41/N/sub 6/O/sub 16/P and C/sub 30/H/sub 45/N/sub 6/O/sub 16/P, respectively. The presence of phosphorus was confirmed by 100-MHz /sup 31/P NMR. The 360-MHz /sup 1/H NMR spectrum of FAF in deuterium oxide was similar to that of MPT. A functional relationship between MPT and FAF was documented; bothmore » compounds stimulated the reductive demethylation of 2-(methylthio)ethanesulfonic acid (CH/sub 3/-S-CoM) to CH/sub 4/ when formaldehyde oxidation provided a source of electrons, and FAF replaced MPT in the CH/sub 3/-S-CoM-stimulated conversion of CO/sub 2/ to CH/sub 4/ under H/sub 2/ (the RPG effect). MPT was enzymically converted to FAF during the reduction of CH/sub 3/-S-CoM, and HCHO to CH/sub 4/ under H/sub 2/. Evidence indicates that FAF is tetrahydromethanopterin. 14 references, 8 figures.« less

Rechargeable Thin-film Lithium Batteries

DOE R&D Accomplishments Database

Bates, J. B.; Gruzalski, G. R.; Dudney, N. J.; Luck, C. F.; Yu, Xiaohua

1993-08-01

Rechargeable thin film batteries consisting of lithium metal anodes, an amorphous inorganic electrolyte, and cathodes of lithium intercalation compounds have recently been developed. The batteries, which are typically less than 6 {mu}m thick, can be fabricated to any specified size, large or small, onto a variety of substrates including ceramics, semiconductors, and plastics. The cells that have been investigated include Li TiS{sub 2}, Li V{sub 2}O{sub 5}, and Li Li{sub x}Mn{sub 2}O{sub 4}, with open circuit voltages at full charge of about 2.5, 3.6, and 4.2, respectively. The development of these batteries would not have been possible without the discovery of a new thin film lithium electrolyte, lithium phosphorus oxynitride, that is stable in contact with metallic lithium at these potentials. Deposited by rf magnetron sputtering of Li{sub 3}PO{sub 4} in N{sub 2}, this material has a typical composition of Li{sub 2.9}PO{sub 3.3}N{sub 0.46} and a conductivity at 25{degrees}C of 2 {mu}S/cm. The maximum practical current density obtained from the thin film cells is limited to about 100 {mu}A/cm{sup 2} due to a low diffusivity of Li{sup +} ions in the cathodes. In this work, the authors present a short review of their work on rechargeable thin film lithium batteries.

Electron beam-generated Ar/N{sub 2} plasmas: The effect of nitrogen addition on the brightest argon emission lines

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

Lock, E. H., E-mail: evgeniya.lock@nrl.navy.mil, E-mail: scott.walton@nrl.navy.mil; Petrova, Tz. B.; Petrov, G. M.

2016-04-15

The effect of nitrogen addition on the emission intensities of the brightest argon lines produced in a low pressure argon/nitrogen electron beam-generated plasmas is characterized using optical emission spectroscopy. In particular, a decrease in the intensities of the 811.5 nm and 763.5 nm lines is observed, while the intensity of the 750.4 nm line remains unchanged as nitrogen is added. To explain this phenomenon, a non-equilibrium collisional-radiative model is developed and used to compute the population of argon excited states and line intensities as a function of gas composition. The results show that the addition of nitrogen to argon modifies the electron energymore » distribution function, reduces the electron temperature, and depopulates Ar metastables in exchange reactions with electrons and N{sub 2} molecules, all of which lead to changes in argon excited states population and thus the emission originating from the Ar 4p levels.« less

OXIDIZING PROTO-ATMOSPHERE ON TITAN: CONSTRAINT FROM N{sub 2} FORMATION BY IMPACT SHOCK

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

Ishimaru, Ryo; Matsui, Takafumi; Sekine, Yasuhito

2011-11-01

Titan is the only satellite that possesses a thick atmosphere, composed mainly of N{sub 2} and CH{sub 4}. However, its origin and evolution remain largely unknown. Knowledge of the acquirement of a N{sub 2} atmosphere on Titan would provide insights into nitrogen evolution in planetary atmospheres as well as the formation of satellite systems around gas giants. Previous studies have proposed that the atmospheric N{sub 2} would have been converted from NH{sub 3} via shock heating by accreting satellitesimals in the highly reducing proto-atmosphere composed of NH{sub 3} and CH{sub 4}. Nevertheless, the validity of this mechanism strongly depends onmore » both the composition of the proto-atmosphere and kinetics of shock chemistry. Here, we show that a CO{sub 2}-rich oxidizing proto-atmosphere is necessary to form N{sub 2} from NH{sub 3} efficiently by atmospheric shock heating. Efficient shock production of N{sub 2} is inhibited in a reducing proto-atmosphere composed of NH{sub 3} and CH{sub 4}, because CH{sub 4} plays as the coolant gas owing to its large heat capacity. Our calculations show that the amount of N{sub 2} produced in a CO{sub 2}-rich proto-atmosphere could have reached {approx}20 times that on the present Titan. Although further quantitative analysis are required (especially, the occurrence of catalytic reactions), our results imply that the chemical composition of satellitesimals that formed the Saturnian system is required to be oxidizing if the current atmospheric N{sub 2} is derived from the shock heating in the proto-atmosphere during accretion. This supports the formation of regular satellites in an actively supplied circumplanetary disk using CO{sub 2}-rich materials originated from the solar nebula at the final stage of gas giant formation.« less

Crystal structure and high-temperature properties of the Ruddlesden–Popper phases Sr{sub 3−x}Y{sub x}(Fe{sub 1.25}Ni{sub 0.75})O{sub 7−δ} (0≤x≤0.75)

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

Samain, Louise; Amshoff, Philipp; Biendicho, Jordi J.

2015-07-15

Ruddlesden–Popper n=2 member phases Sr{sub 3−x}Y{sub x}Fe{sub 1.25}Ni{sub 0.75}O{sub 7−δ}, 0≤x≤0.75, have been investigated by X-ray and neutron powder diffraction, thermogravimetry and Mössbauer spectroscopy. Both samples as-prepared at 1300 °C under N{sub 2}(g) flow and samples subsequently air-annealed at 900 °C were studied. The as-prepared x=0.75 phase is highly oxygen deficient with δ=1, the O1 atom site being vacant, and the Fe{sup 3+}/Ni{sup 2+} ions having a square pyramidal coordination. For as-prepared phases with lower x values, the Mössbauer spectral data are in good agreement with the presence of both 5- and 4-coordinated Fe{sup 3+} ions, implying in addition amore » partial occupancy of the O3 atom sites that form the basal plane of the square pyramid. The air-annealed x=0.75 sample has a δ value of 0.61(1) and the structure has Fe/Ni ions in both square pyramids and octahedra. Mössbauer spectroscopy shows the phase to contain only Fe{sup 3+}, implying that all Ni is present as Ni{sup 3+}. Air-annealed phases with lower x values are found to contain both Fe{sup 3+} and Fe{sup 4+}. For both the as-prepared and the air-annealed samples, the Y{sup 3+} cations are found to be mainly located in the perovskite block. The high-temperature thermal expansion of as-prepared and air-annealed x=0.75 phases were investigated by high-temperature X-ray diffraction and dilatometry and the linear thermal expansion coefficient determined to be 14.4 ppm K{sup −1}. Electrical conductivity measurements showed that the air-annealed samples have higher conductivity than the as-prepared ones. - Highlights: • Ruddlesden–Popper, n=2, Sr{sub 3−x}Y{sub x}Fe{sub 1.25}Ni{sub 0.75}O{sub 7−δ}, 0≤x≤0.75, have been synthesised. • The crystal structures of the phases have been determined. • Sr{sub 2.25}Y{sub 0.75}Fe{sub 1.25}Ni{sub 0.75}O{sub 6}, made in N{sub 2}(g) has Fe{sup 3+}/Ni{sup 2+} in square pyramides. • Sr{sub 2.25}Y{sub 0.75}Fe{sub 1.25}Ni{sub 0.75}O{sub 6.4}, made in air has Fe{sup 3+}/Ni{sup 3+} in square pyramides and octahedra. • Air annealed samples have higher electrical conductivity than N{sub 2}(g) annealed.« less

Influence of periodically changing oxidizing and reducing environment on sulfur capture under PFBC conditions

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

Yrjas, P.; Hupa, M.

1997-12-31

In the literature it has been reported that sulfur capture with limestone (CaCO{sub 3}) under atmospheric fluidized bed combustion conditions reaches a maximum at about 850 C. Previously, the maximum has been attributed to the sintering of the sorbent particles which decreases the reactive surface area. Lately, also another explanation has been reported. In this case the sulfur capture decrease at higher temperatures was concluded to be due to fluctuating oxidizing/reducing conditions in the atmospheric combustor. In this paper the influence of alternating oxidizing/reducing conditions on SO{sub 2} capture at atmospheric and elevated pressure (15 bar) is reported. In themore » pressurized case, the CO{sub 2} partial pressure was kept high enough to prevent CaCO{sub 3} from calcining and therefore the CaSO{sub 4} would not form CaO but CaCO{sub 3} from calcining and therefore the CaSO{sub 4} would not form CaO but CaCO{sub 3} under reducing conditions. The experiments were done with a pressurized TGA by periodically changing the gas environment between oxidizing (O{sub 2}, SO{sub 2}, CO{sub 2} and N{sub 2}) and slightly reducing (CO, SO{sub 2}, CO{sub 2} and N{sub 2}) gas mixtures at different temperatures. The results showed that under normal pressure and slightly reducing conditions CaO formation from CaSO{sub 4} increased with temperature as expected. However, no significant amounts of CaCO{sub 3} were formed from CaSO{sub 4} at elevated pressure. It was also concluded that since the formation of CaO from CaSO{sub 4} was relatively slow it could not explain the sharp sulfur capture maximum at about 850 C. Therefore, it was assumed that the strongly reducing zones, where CaS thermodynamically is the stable compound, may play a more important role than the slightly reducing zones, concerning the sulfur capture in fluidized bed combustors.« less

Oxalyl chloride, ClC(O)C(O)Cl: UV/vis spectrum and Cl atom photolysis quantum yields at 193, 248, and 351 nm

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

Ghosh, Buddhadeb; Papanastasiou, Dimitrios K.; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado 80309

2012-10-28

Oxalyl chloride, (ClCO){sub 2}, has been used as a Cl atom photolytic precursor in numerous laboratory kinetic and photochemical studies. In this study, the UV/vis absorption spectrum of (ClCO){sub 2} and the Cl atom quantum yields in its photolysis at 193, 248, and 351 nm are reported. The UV/vis spectrum was measured between 200 and 450 nm at 296 K using diode array spectroscopy in conjunction with an absolute cross section obtained at 213.9 nm. Our results are in agreement with the spectrum reported by Baklanov and Krasnoperov [J. Phys. Chem. A 105, 97-103 (2001)], which was obtained at 11more » discrete wavelengths between 193.3 and 390 nm. Cl atom quantum yields, {Phi}({lambda}), were measured using pulsed laser photolysis coupled with time resolved atomic resonance fluorescence detection of Cl. The UV photolysis of (ClCO){sub 2} has been shown in previous studies to occur via an impulsive three-body dissociation mechanism, (COCl){sub 2}+ hv{yields} ClCO*+ Cl + CO (2), where the excited ClCO radical, ClCO*, either dissociates or stabilizes ClCO*{yields} Cl + CO (3a), {yields} ClCO (3b). ClCO is thermally unstable at the temperatures (253-298 K) and total pressures (13-128 Torr) used in our experiments ClCO + M {yields} Cl + CO + M (4) leading to the formation of a secondary Cl atom that was resolvable in the Cl atom temporal profiles obtained in the 248 and 351 nm photolysis of (ClCO){sub 2}. {Phi}(193 nm) was found to be 2.07 {+-} 0.37 independent of bath gas pressure (25.8-105.7 Torr, N{sub 2}), i.e., the branching ratio for channel 2a or the direct formation of 2Cl + 2CO in the photolysis of (ClCO){sub 2} is >0.95. At 248 nm, the branching ratio for channel 2a was determined to be 0.79 {+-} 0.15, while the total Cl atom yield, i.e., following the completion of reaction (4), was found to be 1.98 {+-} 0.26 independent of bath gas pressure (15-70 Torr, N{sub 2}). {Phi}(351 nm) was found to be pressure dependent between 7.8 and 122.4 Torr (He, N{sub 2}). The low-pressure limit of the total Cl atom quantum yield, {Phi}{sub 0}(351 nm), was 2.05 {+-} 0.24. As part of this work, rate coefficients for the thermal decomposition of ClCO were measured between 253 and 298 K at total pressures between 13 and 128 Torr (He and N{sub 2} bath gases). The N{sub 2} bath gas results were combined with the data reported in Nicovich et al. [J. Chem. Phys. 92, 3539-3544 (1990)] to yield k{sub 4}(T, N{sub 2}) = (4.7 {+-} 0.7) Multiplication-Sign 10{sup -10} exp [-(2987 {+-} 16)/T] cm{sup 3} molecule{sup -1} s{sup -1}, while the He bath gas data fit yielded k{sub 4}(T, He) = (2.3 {+-} 2.1) Multiplication-Sign 10{sup -10} exp [-(2886 {+-} 218)/T] cm{sup 3} molecule{sup -1} s{sup -1}. The quoted uncertainties are at the 2{sigma} level from the precision of the fit. In addition, the room temperature rate coefficient for the Cl + ClNO reaction was measured in this work to be (1.03 {+-} 0.10) Multiplication-Sign 10{sup -10} cm{sup 3} molecule{sup -1} s{sup -1}.« less

Relationship between pretreatment level of plasma Epstein-Barr virus DNA, tumor burden, and metabolic activity in advanced nasopharyngeal carcinoma

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

Ma, Brigette; King, Ann; Lo, Y.M. Dennis

Purpose: Plasma Epstein-Barr virus DNA (pEBV DNA) is an important prognostic marker in nasopharyngeal carcinoma (NPC). This study tested the hypotheses that pEBV DNA reflects tumor burden and metabolic activity by evaluating its relationship with tumor volume and {sup 18}F-fluorodeoxyglucose ({sup 18}F-FDG) uptake in NPC. Methods and Materials: Pre-treatment pEBV DNA analysis, {sup 18}F-FDG positron emission tomography-computed tomography scan (PET-CT) and magnetic resonance imaging (MRI) of the head and neck were performed in 57 patients. Net volume (cm{sup 3}) of the primary tumor (T{sub vol}) and regional nodes (N{sub vol}) were quantified on MRI. {sup 18}F-FDG uptake was expressed asmore » the maximum standardized uptake value (SUV{sub max}) at the primary tumor (T{sub suv}) and regional nodes (N{sub suv}). Lesions with SUV{sub max} {>=} 2.5 were considered malignant. Relationship between SUV{sub max}, natural logarithm (log) of pEBV DNA, and square root (sq) of MRI volumes was analyzed using the Wilcoxon test. A linear regression model was constructed to test for any interaction between variables and disease stage. Results: Log-pEBV DNA showed significant correlation with sq-T{sub vol} (r = 0.393), sq-N{sub vol} (r = 0.452), total tumor volume (sq-Total{sub vol} = T{sub vol} + N{sub vol}, r = 0.554), T{sub suv} (r = 0.276), N{sub suv} (r = 0.434), and total SUV{sub max} (Total{sub suv} = T{sub suv} + N{sub suv}, r = 0.457). Likewise, sq-T{sub vol} was correlated to T{sub suv} (r 0.426), and sq-N{sub vol} with N{sub suv} (r = 0.651). Regression analysis showed that only log-pEBV DNA was significantly associated with sq-Total{sub vol} (p < 0.001; parameter estimate = 8.844; 95% confidence interval = 3.986-13.703), whereas Sq-T{sub vol} was significantly associated with T{sub suv} (p = 0.002; parameter estimate = 3.923; 95% confidence interval = 1.498-6.348). Conclusion: This study supports the hypothesis that cell-free plasma EBV DNA is a marker of tumor burden in EBV-related NPC.« less

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

Luo, Huajuan; Zhao, Yanbao, E-mail: zhaoyb902@henu.edu.cn; Sun, Lei

Graphical abstract: A simple method for the synthesis of novel micrometer flower-like Cu/PVP architectures was introduced. Highlights: {yields} Micrometer flower-like copper/polyvinylpyrrolidone architectures were obtained by a simple chemical route. {yields} The amount of N{sub 2}H{sub 4}{center_dot}H{sub 2}O, the reaction temperature, the molar ratio of CuCl{sub 2} to PVP and different molecular weights of PVP play an important role in the controlling the morphology of the Cu/PVP architectures. {yields} A possible mechanism of the formation of Cu/PVP architectures was discussed. -- Abstract: Micrometer-sized flower-like Cu/polyvinylpyrrolidone (PVP) architectures are synthesized by the reduction of copper (II) salt with hydrazine hydrate in aqueousmore » solution in the presence of PVP capping agent. The resulting Cu/PVP architectures are investigated by UV-vis spectroscopy, transmission electron microscopy (TEM), X-ray powder diffraction (XRD), and scanning electron microscopy (SEM). The Cu/PVP flowers have uniform morphologies with an average diameter of 10 {mu}m, made of several intercrossing plates. The formation of Cu/PVP flowers is a new kinetic control process, and the factors such as the amount of N{sub 2}H{sub 4}{center_dot}H{sub 2}O, reaction temperature, molar ratio of CuCl{sub 2} to PVP and molecular weight of PVP have significant effect on the morphology of Cu/PVP architectures. A possible mechanism of the formation of micrometer Cu/PVP architectures was discussed.« less

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

Gao, Junkuo, E-mail: jkgao@zstu.edu.cn; Wang, Jiangpeng; Qian, Xuefeng

Here we report a novel synthetic pathway for preparation of Cu-doped g-C{sub 3}N{sub 4} (Cu-g-C{sub 3}N{sub 4}) with nanosheet morphology by using a two dimensional Cu–melamine supramolecular network as both sacrificial template and precursor. The specific surface area of Cu-g-C{sub 3}N{sub 4} is 40.86 m{sup 2} g{sup −1}, which is more than 7 times larger than that of pure g-C{sub 3}N{sub 4}. Cu-g-C{sub 3}N{sub 4} showed strong optical absorption in the visible-light region and expanded the absorption to the near-infrared region. The uniform nanosheet morphology, higher surface area and strong visible-light absorption have enabled Cu-g-C{sub 3}N{sub 4} exhibiting enhanced visiblemore » light photocatalytic activity for the photo-degradation of methylene blue (MB). The results indicate that metal–melamine supramolecular network can be promising precursors for the one step preparation of efficient metal-doped g-C{sub 3}N{sub 4} photocatalysts. - Graphical abstract: Cu-doped g-C{sub 3}N{sub 4} (Cu-g-C{sub 3}N{sub 4}) with nanosheet morphology was fabricated via a simple one step preparation by using a two dimensional Cu–melamine supra-molecular network as both sacrificial template and precursor. - Highlights: • Cu-doped g-C{sub 3}N{sub 4} (Cu-g-C{sub 3}N{sub 4}) with nanosheet morphology was prepared. • Cu-g-C{sub 3}N{sub 4} showed strong optical absorption in the visible-light region. • Cu-g-C{sub 3}N{sub 4} exhibits enhanced visible light photocatalytic activity.« less

ABIOTIC OXYGEN-DOMINATED ATMOSPHERES ON TERRESTRIAL HABITABLE ZONE PLANETS

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

Wordsworth, Robin; Pierrehumbert, Raymond

2014-04-20

Detection of life on other planets requires identification of biosignatures, i.e., observable planetary properties that robustly indicate the presence of a biosphere. One of the most widely accepted biosignatures for an Earth-like planet is an atmosphere where oxygen is a major constituent. Here we show that lifeless habitable zone terrestrial planets around any star type may develop oxygen-dominated atmospheres as a result of water photolysis, because the cold trap mechanism that protects H{sub 2}O on Earth is ineffective when the atmospheric inventory of non-condensing gases (e.g., N{sub 2}, Ar) is low. Hence the spectral features of O{sub 2} and O{submore » 3} alone cannot be regarded as robust signs of extraterrestrial life.« less

T2-weighted four dimensional magnetic resonance imaging with result-driven phase sorting

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

Liu, Yilin; Yin, Fang-Fang; Cai, Jing, E-mail: jing.cai@duke.edu

2015-08-15

Purpose: T2-weighted MRI provides excellent tumor-to-tissue contrast for target volume delineation in radiation therapy treatment planning. This study aims at developing a novel T2-weighted retrospective four dimensional magnetic resonance imaging (4D-MRI) phase sorting technique for imaging organ/tumor respiratory motion. Methods: A 2D fast T2-weighted half-Fourier acquisition single-shot turbo spin-echo MR sequence was used for image acquisition of 4D-MRI, with a frame rate of 2–3 frames/s. Respiratory motion was measured using an external breathing monitoring device. A phase sorting method was developed to sort the images by their corresponding respiratory phases. Besides, a result-driven strategy was applied to effectively utilize redundantmore » images in the case when multiple images were allocated to a bin. This strategy, selecting the image with minimal amplitude error, will generate the most representative 4D-MRI. Since we are using a different image acquisition mode for 4D imaging (the sequential image acquisition scheme) with the conventionally used cine or helical image acquisition scheme, the 4D dataset sufficient condition was not obviously and directly predictable. An important challenge of the proposed technique was to determine the number of repeated scans (N{sub R}) required to obtain sufficient phase information at each slice position. To tackle this challenge, the authors first conducted computer simulations using real-time position management respiratory signals of the 29 cancer patients under an IRB-approved retrospective study to derive the relationships between N{sub R} and the following factors: number of slices (N{sub S}), number of 4D-MRI respiratory bins (N{sub B}), and starting phase at image acquisition (P{sub 0}). To validate the authors’ technique, 4D-MRI acquisition and reconstruction were simulated on a 4D digital extended cardiac-torso (XCAT) human phantom using simulation derived parameters. Twelve healthy volunteers were involved in an IRB-approved study to investigate the feasibility of this technique. Results: 4D data acquisition completeness (C{sub p}) increases as NR increases in an inverse-exponential fashion (C{sub p} = 100 − 99 × exp(−0.18 × N{sub R}), when N{sub B} = 6, fitted using 29 patients’ data). The N{sub R} required for 4D-MRI reconstruction (defined as achieving 95% completeness, C{sub p} = 95%, N{sub R} = N{sub R,95}) is proportional to N{sub B} (N{sub R,95} ∼ 2.86 × N{sub B}, r = 1.0), but independent of N{sub S} and P{sub 0}. Simulated XCAT 4D-MRI showed a clear pattern of respiratory motion. Tumor motion trajectories measured on 4D-MRI were comparable to the average input signal, with a mean relative amplitude error of 2.7% ± 2.9%. Reconstructed 4D-MRI for healthy volunteers illustrated clear respiratory motion on three orthogonal planes, with minimal image artifacts. The artifacts were presumably caused by breathing irregularity and incompleteness of data acquisition (95% acquired only). The mean relative amplitude error between critical structure trajectory and average breathing curve for 12 healthy volunteers is 2.5 ± 0.3 mm in superior–inferior direction. Conclusions: A novel T2-weighted retrospective phase sorting 4D-MRI technique has been developed and successfully applied on digital phantom and healthy volunteers.« less

Thermally-induced solid state transformation of β‐Fe{sub 2}O{sub 3} nanoparticles in various atmospheres

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

Malina, Ondrej, E-mail: ondrej.malina@upol.cz; Kaslik, Josef, E-mail: ondrej.malina@upol.cz; Tucek, Jiri, E-mail: ondrej.malina@upol.cz

2014-10-27

To date, iron oxides have become one of the most studied nanomaterials due to their interesting and aaplication appealing physical, chemical, and biological properties in comparison with their bulk counterparts. In general, four forms of iron(III) oxide can be distinguished depending on their crystallographic and magnetic properties. In this work, one of the rare phases of iron(III) oxide, β‐Fe{sub 2}O{sub 3}, prepared by the solid state reaction was explored for the thermal transformations in various ambient atmospheres, including O{sub 2}, N{sub 2}, and CO{sub 2} atmospheres. The thermally treated products were investigated employing X-ray powder diffraction and {sup 57}Fe Mössbauermore » spectroscopy.« less

Multi-stage catalyst systems and uses thereof

DOEpatents

Ozkan, Umit S [Worthington, OH; Holmgreen, Erik M [Columbus, OH; Yung, Matthew M [Columbus, OH

2009-02-10

Catalyst systems and methods provide benefits in reducing the content of nitrogen oxides in a gaseous stream containing nitric oxide (NO), hydrocarbons, carbon monoxide (CO), and oxygen (O.sub.2). The catalyst system comprises an oxidation catalyst comprising a first metal supported on a first inorganic oxide for catalyzing the oxidation of NO to nitrogen dioxide (NO.sub.2), and a reduction catalyst comprising a second metal supported on a second inorganic oxide for catalyzing the reduction of NO.sub.2 to nitrogen (N.sub.2).

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

Hemawan, Kadek W.; Gou, Huiyang; Hemley, Russell J.

Polycrystalline diamond has been synthesized on silicon substrates at atmospheric pressure, using a microwave capillary plasma chemical vapor deposition technique. The CH{sub 4}/Ar plasma was generated inside of quartz capillary tubes using 2.45 GHz microwave excitation without adding H{sub 2} into the deposition gas chemistry. Electronically excited species of CN, C{sub 2}, Ar, N{sub 2}, CH, H{sub β}, and H{sub α} were observed in the emission spectra. Raman measurements of deposited material indicate the formation of well-crystallized diamond, as evidenced by the sharp T{sub 2g} phonon at 1333 cm{sup −1} peak relative to the Raman features of graphitic carbon. Field emission scanningmore » electron microscopy images reveal that, depending on the growth conditions, the carbon microstructures of grown films exhibit “coral” and “cauliflower-like” morphologies or well-facetted diamond crystals with grain sizes ranging from 100 nm to 10 μm.« less

Glasses having a low non-linear refractive index for laser applications

DOEpatents

Faulstich, Marga; Jahn, Walter; Krolla, Georg; Neuroth, Norbert

1980-01-01

Glass composition ranges are described which permit the introduction of laser activators into fluorphosphate glass with exceptionally high fluorine content while forming glasses of high crystallization stability and permitting the realization of large melt volumes. The high fluorine content imparts to the glasses an exceptionally low nonlinear refractive index n.sub.2 down to O,4 .times.10.sup.-13 esu.

Electrocatalytic oxidation of 2-mercaptoethanol using modified glassy carbon electrode by MWCNT in combination with unsymmetrical manganese (II) Schiff base complexes

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

Mohebbi, Sajjad, E-mail: smohebbi@uok.ac.ir; Eslami, Saadat

2015-06-15

Highlights: • High electocatalytic efficiency and stability of modified hybrid electrode GC/MWCNTs/MnSaloph. • Direct reflection of catalytic activity of manganese complexes on electrocatalytic oxidation of 2-ME. • Decreasing overpotential and increasing catalytic peak current toward oxidation of 2-ME. • Deposition of range of novel substituted N{sub 2}O{sub 2} Saloph complexes of manganese(II) on GCE/MWCNT. • Enhancement of electrocatalytic oxidation activity upon electron donating substitutions on the Saloph. - Abstract: The performance of modified hybrid glassy carbon electrode with composite of carbon nanotubes and manganese complexes for the electrocatalytic oxidation of 2-mercaptoethanol is developed. GC electrode was modified using MWCNT andmore » new N{sub 2}O{sub 2} unsymmetrical tetradentate Schiff base complexes of manganese namely Manganese Saloph complexes 1-5, with general formula Mn[(5-x-4-y-Sal)(5-x′-4-y′-Sal) Ph], where x, x′ = H, Br, NO{sub 2} and y, y′ = H, MeO. Direct immobilization of CNT on the surface of GCE is performed by abrasive immobilization, and then modified by manganese(II) complexes via direct deposition method. These novel modified electrodes clearly demonstrate the necessity of modifying bare carbon electrodes to endow them with the desired behavior and were identified by HRTEM. Also complexes were characterized by elemental analyses, MS, UV–vis and IR spectroscopy. Modified hybrid GC/MWCNT/MnSaloph electrode exhibits strong and stable electrocatalytic activity towards the electrooxidation of 2-mercaptoethanol molecules in comparison with bare glassy carbon electrode with advantages of very low over potential and high catalytic current. Such ability promotes the thiol’s electron transfer reaction. Also, electron withdrawing substituent on the Saloph was enhanced electrocatalytic oxidation activity.« less

Structural study of (N{sub 2}H{sub 5},H){sub 2.9}U{sub 1.1}Ce{sub 0.9}(C{sub 2}O{sub 4}){sub 5}·10H{sub 2}O from a conventional X-ray diffraction diagram obtained on a powder synthesized by a fast vortex process

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

Brackx, E., E-mail: Emmanuelle.brackx@cea.fr; Laval, J.P.; Dugne, O.

2015-01-15

In the context of research on U/minor actinides for nuclear fuel reprocessing in the transmutation process, developments are first studied with surrogates containing uranium and lanthanides to facilitate testing. The tests consist of precipitating and calcining a hydrazinium uranium/cerium oxalate. The structure of this oxalate had not been previously determined, but was necessary to validate the physicochemical mechanisms involved. The present study, firstly demonstrates the structural similarity of the U/Ce oxalate phase (N{sub 2}H{sub 5},H){sub 2.9}U{sub 1.1}Ce{sub 0.9}(C{sub 2}O{sub 4}){sub 5}·10H{sub 2}O, synthesized using a vortex precipitator for continuous synthesis of actinide oxalates, with previously known oxalates, crystallizing in P6{submore » 3}/mmc symmetry, obtained by more classical methods. This fast precipitation process induces massive nucleation of fine powders. Their structural and microstructural determination confirms that the raw and dried phases belong to the same structural family as (NH{sub 4}){sub 2}U{sub 2}(C{sub 2}O{sub 4}){sub 5}·0.7H{sub 2}O whose structure was described by Chapelet-Arab in P6{sub 3}/mmc symmetry, using single crystal data. However, they present an extended disorder inside the tunnels of the structure, even after drying at 100 °C, between water and hydrazinium ions. This disorder is directly related to the fast vortex method. This structure determination can be used as a basis for further semi-quantitative analysis on the U/minor actinides products formed under various experimental conditions. - Highlights: • Uranium cerium oxalate precipitate characterization by X-ray powder diffraction. • Morphology characterization by SEM analysis. • Structure determination by unit cell Rietveld refinement.« less

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

Hargreaves, L. R.; Colyer, C.; Stevenson, M. A.

A number of previous studies have suggested the possibility of two-center interference effects in the single ionization of diatomic molecules such as H{sub 2} and N{sub 2}. While interference effects have been successfully observed in the ionization of H{sub 2}, to date evidence for interference in N{sub 2} ionization has yet to be conclusively demonstrated. This study presents triply differential cross sections for electron impact ionization of N{sub 2}, measured using the (e,2e) technique. The data are probed for signatures of two-center interference effects. Evidence for interference manifesting in the cross sections is observed.

Impact of post metal annealing on gate work function engineering for advanced MOS applications

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

Kumar, S. Sachin, E-mail: ssachikl995@yahoo.in; Prasad, Amitesh; Sinha, Amrita

2016-05-06

Ultra thin HfO{sub 2} high-k gate dielectric has been deposited directly on strained Si{sub 0.81}Ge{sub 0.19} by Atomic Layer Deposition (ALD) technique. The influence of different types of metal gate electrodes (Al, Au, Pt) on electrical characteristics of Metal-Oxide-Semiconductor capacitors has been studied. Our results show that the electrical characteristics of MOS device are highly dependent on the gate electrodes used. The dependency of electrical characteristics on post metal annealing was studied in detail. The measured flat band (V{sub fb}) and hysteresis (ΔV{sub fb}) from high frequency C-V characteristics were used to study the pre-existing traps in the dielectric. Impactmore » of PMA on interface state density (D{sub it}), border trap density (N{sub bt}) and oxide trap density (Q{sub f/q}) of high-k gate stack were also examined for all the devices. The N{sub bt} and frequency dispersion significantly reduces to ~2.77x1010 cm{sup −2} and ~11.34 % respectively in case of Al electrode with a Dit value of ~4x10{sup 12} eV{sup −1}cm{sup −2} after PMA (350°C) in N{sub 2}, suggesting an improvement in device performance while Pt electrode shows a much less value of ΔVfb (~0.02 V) and Dit (~3.44x10{sup 12} eV{sup −1}cm{sup −2}) after PMA.« less

Low temperature synthesis of diamond-based nano-carbon composite materials with high electron field emission properties

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

Saravanan, A.; Huang, B. R.; Yeh, C. J.

2015-06-08

A diamond-based nano-carbon composite (d/NCC) material, which contains needle-like diamond grains encased with the nano-graphite layers, was synthesized at low substrate temperature via a bias enhanced growth process using CH{sub 4}/N{sub 2} plasma. Such a unique granular structure renders the d/NCC material very conductive (σ = 714.8 S/cm), along with superior electron field emission (EFE) properties (E{sub 0} = 4.06 V/μm and J{sub e} = 3.18 mA/cm{sup 2}) and long lifetime (τ = 842 min at 2.41 mA/cm{sup 2}). Moreover, the electrical conductivity and EFE behavior of d/NCC material can be tuned in a wide range that is especially useful for different kind of applications.

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

Capone, D.G.; Penhale, P.A.; Oremland, R.S.

N/sub 2/ (C/sub 2/H/sub 2/) fixation and primary production were measured in communities of Thalassia testudinum at two sites in Bimini Harbor (Bahamas). Production was determined by uptake of (/sup 14/C)NaHCO/sub 3/, by leaf growth measurements, and by applying an empirical formula based on leaf dimensions. The last two methods gave similar results but the /sup 14/C method gave higher values. Anaerobic sediment N/sub 2/ fixation supplied about 1/4 to 1/2 of the nitrogen demand for leaf production (by leaf growth method) and there was a significant correlation between N/sub 2/ fixation and CO/sub 2/ fixation rates when all componentsmore » of the communities were considered (macrophyte, phyllosphere epiphytes, and detrital leaves). N/sub 2/ fixation is important to production in Thalassia communities and the plant and its leaf epiphytes may be distinct entities in terms of nitrogen and carbon metabolism.« less

Thermal Fatigue Testing of ZrO2-Y2O3 Thermal Barrier Coating Systems using a High Power CO2 Laser

NASA Technical Reports Server (NTRS)

Zhu, Dongming; Miller, Robert A.

1997-01-01

In the present study, the mechanisms of fatigue crack initiation and propagation, and of coating failure, under thermal loads that simulate diesel engine conditions, are investigated. The surface cracks initiate early and grow continuously under thermal Low Cycle Fatigue (LCF) and High Cycle Fatigue (HCF) stresses. It is found that, in the absence of interfacial oxidation, the failure associated with LCF is closely related to coating sintering and creep at high temperatures. Significant LCF and HCF interactions have been observed in the thermal fatigue tests. The fatigue crack growth rate in the ceramic coating strongly depends on the characteristic HCF cycle number, N*(sub NCF), which is defined as the number of HCF cycles per LCF cycle. The crack growth rate is increased from 0.36 microns/LCF cycle for a pure LCF test to 2.8 microns/LCF cycle for a combined LCF and HCF test at N*(sub NCF) about 20,000. A surface wedging model has been proposed to account for the HCF crack growth in the coating systems. This mechanism predicts that HCF damage effect increases with increasing surface temperature swing, the thermal expansion coefficient and the elastic modulus of the ceramic coating, as well as with the HCF interacting depth. A good agreement has been found between the analysis and experimental evidence.

Turning things downside up: Adsorbate induced water flipping on Pt(111)

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

Kimmel, Greg A., E-mail: gregory.kimmel@pnnl.gov, E-mail: bruce.kay@pnnl.gov; Zubkov, Tykhon; Smith, R. Scott

2014-11-14

We have examined the adsorption of the weakly bound species N{sub 2}, O{sub 2}, CO, and Kr on the (√(37)×√(37))R25.3{sup ∘} water monolayer on Pt(111) using a combination of molecular beam dosing, infrared reflection absorption spectroscopy, and temperature programmed desorption. In contrast to multilayer crystalline ice, the adsorbate-free water monolayer is characterized by a lack of dangling OH bonds protruding into the vacuum (H-up). Instead, the non-hydrogen-bonded OH groups are oriented downward (H-down) to maximize their interaction with the underlying Pt(111) substrate. Adsorption of Kr and O{sub 2} have little effect on the structure and vibrational spectrum of the “√(37)”more » water monolayer while adsorption of both N{sub 2}, and CO are effective in “flipping” H-down water molecules into an H-up configuration. This “flipping” occurs readily upon adsorption at temperatures as low as 20 K and the water monolayer transforms back to the H-down, “√(37)” structure upon adsorbate desorption above 35 K, indicating small energy differences and barriers between the H-down and H-up configurations. The results suggest that converting water in the first layer from H-down to H-up is mediated by the electrostatic interactions between the water and the adsorbates.« less

Variability in the x-ray emission of H0538+608: An unusual AM Her-type cataclysmic variable. Thesis, Final Report

NASA Technical Reports Server (NTRS)

Catelli, Jennifer

1992-01-01

The x-ray emissions of AM Herculis-type object H0538+608 were observed using the ROSAT satellite. Evidence was found for a highly varying soft x-ray component with a much lower intensity than is typical for this class. The spectrum was well fit by a thermal bremsstrahlung model (exponential plus gaunt factor) of 35 +/- 5 KeV plus a 0.05 +/- 0.01 KeV blackbody component, with absorption by interstellar medium with a neutral hydrogen column density of log N(sub H) (atoms/sq cm) = 20.2. No obvious periodic variations were found. There was very little correlation between the hard and soft x-ray bands.

Structural silicon nitride materials containing rare earth oxides

DOEpatents

Andersson, Clarence A.

1980-01-01

A ceramic composition suitable for use as a high-temperature structural material, particularly for use in apparatus exposed to oxidizing atmospheres at temperatures of 400 to 1600.degree. C., is found within the triangular area ABCA of the Si.sub.3 N.sub.4 --SiO.sub.2 --M.sub.2 O.sub.3 ternary diagram depicted in FIG. 1. M is selected from the group of Yb, Dy, Er, Sc, and alloys having Yb, Y, Er, or Dy as one component and Sc, Al, Cr, Ti, (Mg +Zr) or (Ni+Zr) as a second component, said alloy having an effective ionic radius less than 0.89 A.

Modeling the tagged-neutron UXO identification technique using the Geant4 toolkit

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

Zhou Y.; Mitra S.; Zhu X.

2011-10-16

It is proposed to use 14 MeV neutrons tagged by the associated particle neutron time-of-flight technique (APnTOF) to identify the fillers of unexploded ordnances (UXO) by characterizing their carbon, nitrogen and oxygen contents. To facilitate the design and construction of a prototype system, a preliminary simulation model was developed, using the Geant4 toolkit. This work established the toolkit environment for (a) generating tagged neutrons, (b) their transport and interactions within a sample to induce emission and detection of characteristic gamma-rays, and (c) 2D and 3D-image reconstruction of the interrogated object using the neutron and gamma-ray time-of-flight information. Using the modeling,more » this article demonstrates the novelty of the tagged-neutron approach for extracting useful signals with high signal-to-background discrimination of an object-of-interest from that of its environment. Simulations indicated that an UXO filled with the RDX explosive, hexogen (C{sub 3}H{sub 6}O{sub 6}N{sub 6}), can be identified to a depth of 20 cm when buried in soil.« less

Effect of electronic excitation on high-temperature flows behind strong shock waves

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

Istomin, V. A.; Kustova, E. V.

2014-12-09

In the present paper, a strongly non-equilibrium one-dimensional steady-state flow behind the plane shock wave is studied. We consider a high-temperature chemically reacting five-component ionized mixture of nitrogen species (N{sub 2}/N{sub 2}{sup 2}/N/N{sup +}/e{sup −}) taking into account electronic degrees of freedom in N and N{sup +} (170 and 625 electronic energy levels respectively), and electronic-rotational-vibrational modes in N{sub 2} and N{sub 2}{sup +} (5 and 7 electronic terms). Non-equilibrium reactions of ionization, dissociation, recombination and charge-transfer are included to the kinetic scheme. The system of governing equations is written under the assumption that translation and internal energy relaxation ismore » fast whereas chemical reactions and ionization proceed on the macroscopic gas-dynamics time-scale. The developed model is applied to simulate the flow behind a plane shock wave under initial conditions characteristic for the spacecraft re-entry from an interplanetary flight (Hermes and Fire II experiments). Fluid-dynamic parameters behind the shock wave as well as transport coefficients and the heat flux are calculated for the (N{sub 2}/N{sub 2}{sup +}/N/N{sup +}/e{sup −}) mixture. The effect of electronic excitation on kinetics, dynamics and heat transfer is analyzed. Whereas the contribution of electronic degrees of freedom to the flow macroparameters is negligible, their influence on the heat flux is found to be important under conditions of Hermes re-entry.« less

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

Bauer, R.; Engel, A.; Franken, H.

This paper describes balloon borne air samples taken above Kiruna (67.9[degrees]N; 21.1[degrees]E) during EASOE, which monitored the N[sub 2]O density, as the polar vortex shifted, between altitudes of 10 and 31 km. Different air samplers were used to collect samples. The results show vertical profiles, outside, in the edge of, and inside the vertex, which reveal variation in mixing ratios as airmasses mix both vertically and horizontally near the vortex.

Synthesis, structure and photoluminescence properties of amine-templated open-framework bismuth sulfates

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

Marri, Subba R.; Behera, J.N., E-mail: jnbehera@niser.ac.in

2014-02-15

Two organically-templated bismuth sulfates of the compositions, [C{sub 6}N{sub 2}H{sub 14}] [Bi(SO{sub 4}){sub 2}(NO{sub 3})], (1) and [C{sub 4}N{sub 2}H{sub 12}]{sub 4}[Bi{sub 4}(SO{sub 4}){sub 10}(H{sub 2}O){sub 4}], (2), with open architecture have been synthesized and their structures determined by single crystal X-ray diffraction. 1 has a corrugated layered structure with 8-membered aperture wherein the SO{sub 4} tetrahedra and the BiO{sub 8} polyhedra join together to form (4, 4) net sheets of the metal centers while 2 has a three-dimensional structure possessing 8- and 12-membered channels. Both the compounds show good fluorescence properties exhibiting blue luminescence. Time-resolved fluorescence behavior of 1more » and 2 shows mean fluorescence life time of 0.9 and 1.0 ns, respectively. - Graphical abstract: Two open-framework bismuth sulfates with the layered and three-dimensional structures have been synthesized and characterized. Both the compounds show good fluorescence properties exhibiting blue luminescence. Display Omitted - Highlights: • Two organically-templated bismuth sulfates with open architecture have been synthesized and characterized. • One has a corrugated layered structure while the other one has a three-dimensional structure possessing channels. • They are novel in that open-framework three-dimensional main group metal sulfates are first to be reported. • They show good fluorescence properties exhibiting blue luminescence.« less

MODTRAN: a moderate resolution model for LOWTRAN. Technical report, 12 May 1986-11 May 1987

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

Berk, A.; Bernstein, L.S.; Robertson, D.C.

1987-07-08

This interim technical report describes a new band-model formulation for the LOWTRAN 6 atmospheric transmittance/radiation computer code. Band-model parameters for H/sub 2/O, CO/sub 2/, O/sub 3/, CO, CH/sub 4/, O/sub 2/, and N/sub 2/ were calculated using the 1986 HITRAN line atlas. They were calculated for 1 /cm bins from 0 - 17,900/cm and at five temperatures from 200 to 300K. This transmittance model and associated subroutines were integrated into LOWTRAN 6. The spectral resolution of this new option is better than 5/cm (FWHM). A preliminary version of the code was delivered to AFGL for testing. Validation against FASCOD2 calculationsmore » will be the emphasis for the remainder of this effort.« less

Nox reduction system utilizing pulsed hydrocarbon injection

DOEpatents

Brusasco, Raymond M.; Penetrante, Bernardino M.; Vogtlin, George E.; Merritt, Bernard T.

2001-01-01

Hydrocarbon co-reductants, such as diesel fuel, are added by pulsed injection to internal combustion engine exhaust to reduce exhaust NO.sub.x to N.sub.2 in the presence of a catalyst. Exhaust NO.sub.x reduction of at least 50% in the emissions is achieved with the addition of less than 5% fuel as a source of the hydrocarbon co-reductants. By means of pulsing the hydrocarbon flow, the amount of pulsed hydrocarbon vapor (itself a pollutant) can be minimized relative to the amount of NO.sub.x species removed.

Enhanced photocatalytic H{sub 2} evolution over CdS/Au/g-C{sub 3}N{sub 4} composite photocatalyst under visible-light irradiation

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

Ding, Xiaoling; University of Chinese Academy of Sciences, Beijing 100049; Li, Yingxuan, E-mail: yxli@ms.xjb.ac.cn, E-mail: cywang@ms.xjb.ac.cn

2015-10-01

A novel heterojunction structured composite photocatalyst CdS/Au/g-C{sub 3}N{sub 4} has been developed by depositing CdS/Au with a core (Au)-shell (CdS) structure on the surface of g-C{sub 3}N{sub 4}. The photocatalytic hydrogen production activity of the developed photocatalyst was evaluated under visible-light irradiation (λ > 420 nm) using methanol as a sacrificial reagent. As a result, its activity is about 125.8 times higher than that of g-C{sub 3}N{sub 4} and is even much higher than that of Pt/g-C{sub 3}N{sub 4}. The enhancement in photocatalytic activity is attributed to efficient separation of the photoexcited charges due to the anisotropic junction in themore » CdS/Au/g-C{sub 3}N{sub 4} system.« less

Atomic parity violation as a probe of new physics

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

Marciano, W.J.; Rosner, J.L.

Effects of physics beyond the standard model on electroweak observables ares studied using the Peskin-Takeuchi isospin-conserving, {ital S}, and -breaking, {ital T}, parametrization of new'' quantum loop corrections. Experimental constraints on {ital S} and {ital T} are presented. Atomic parity-violating experiments are shown to be particularly sensitive to {ital S} with existing data giving {ital S}={minus}2.7{plus minus}2.0{plus minus}1.1. That constraint has important implications for generic technicolor models which predict {ital S}{approx equal}0.1{ital N}{sub {ital T}}{ital N}{sub {ital D}} ({ital N}{sub {ital T}} is the number of technicolors, {ital N}{sub {ital D}} is the number of technidoublets).

Nighttime chemical evolution of aerosol and trace gases in a power plant plume: Implications for secondary organic nitrate and organosulfate aerosol formation, NO3 radical chemistry, and N2O5 heterogeneous hydrolysis

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

Zaveri, R.A.; Kleinman, L.; Berkowitz, C. M.

2010-06-01

Nighttime chemical evolution of aerosol and trace gases in a coal-fired power plant plume was monitored with the Department of Energy Grumman Gulfstream-1 aircraft during the 2002 New England Air Quality Study field campaign. Quasi-Lagrangian sampling in the plume at increasing downwind distances and processing times was guided by a constant-volume balloon that was released near the power plant at sunset. While no evidence of fly ash particles was found, concentrations of particulate organics, sulfate, and nitrate were higher in the plume than in the background air. The enhanced sulfate concentrations were attributed to direct emissions of gaseous H{sub 2}SO{submore » 4}, some of which had formed new particles as evidenced by enhanced concentrations of nucleation-mode particles in the plume. The aerosol species were internally mixed and the particles were acidic, suggesting that particulate nitrate was in the form of organic nitrate. The enhanced particulate organic and nitrate masses in the plume were inferred as secondary organic aerosol, which was possibly formed from NO{sub 3} radical-initiated oxidation of isoprene and other trace organic gases in the presence of acidic sulfate particles. Microspectroscopic analysis of particle samples suggested that some sulfate was in the form of organosulfates. Microspectroscopy also revealed the presence of sp{sup 2} hybridized C = C bonds, which decreased with increasing processing time in the plume, possibly because of heterogeneous chemistry on particulate organics. Constrained plume modeling analysis of the aircraft and tetroon observations showed that heterogeneous hydrolysis of N{sub 2}O{sub 5} was negligibly slow. These results have significant implications for several issues related to the impacts of power plant emissions on air quality and climate.« less

Effectiveness and Cost-Effectiveness Evaluation of an Advanced Artillery Weapon System

DTIC Science & Technology

1992-09-01

SIGXB,SIGYB, SIGMAR ,DIST,RSEARCH,R1,R2 READ ( 2, *) (PRH1(I), I-I, 5), (PRH2(I), 1-1,5), (PRH3(I), 1-1,5) READ ( 2, *) (PRK1(I), I-1, 5), (PRK2(I), 1...ISUB - 1, NSUB CALL RANNUM( 2, SEED(4), DIST, SIGMAR , 0, DISTR ) CALL RANNUM( 1, SEED(5), 0.0, 6.28319, 0, THETA ) 80 C XCS - XB + XP + DISTR*COS(THETA...SIGXB, SIGYB, RATE, RSEARCH, SIGMAR , DIST REAL DX, DY INTEGER NSUB, NAPX, NAPY COMMON /SYSTEM/ SIGXP, SIGYP, SIGXB, SIGYB, RATE, RSEARCH, NSUB

Synthesis and characterization of ferrite-semiconductor nano composite for photocatalytic degradation of aqueous nitrobenzene solution

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

Modi, K. B.; Kathad, C. R.; Raval, P. Y.

2016-05-06

Nanoparticles of semiconductor TiO{sub 2}, zinc ferrite (ZnFe{sub 2}O{sub 4}) and ZnFe{sub 2}O{sub 4}-TiO{sub 2} composite, were synthesized by auto combustion route. Subsequent characterization of synthesized photocatalysts was carried out by X-ray powder diffractometry, transmission electron microscopy, UV-Vis-Diffuse Reflectance Spectroscopy to study the structural and textural properties. The specific surface area, pore diameter and pore volume of synthesized materials were investigated by N{sub 2} adsorption analysis while the presence of TiO{sub 2} in the composite material was verified by infrared spectral analysis. The photocatalytic activity of synthesized photocatalysts was evaluated by degradation of nitrobenzene (NB) in aqueous medium under irradiationmore » of ultraviolet light. The result revealed that 77, 73 and 70% of NB was degraded using TiO{sub 2}, ZnFe{sub 2}O{sub 4} and ZnFe{sub 2}O{sub 4}-TiO{sub 2} photocatalysts after 4h in the presence of UV irradiation. The composite photocatalyst was found easy to separate from the treated solution.« less

Systematic modulation and enhancement of CO{sub 2} : N{sub 2} selectivity and water stability in an isoreticular series of bio-MOF-11 analogues

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

Li, Tao; Chen, De-Li; Sullivan, Jeanne E.

2013-02-01

An isoreticular series of cobalt-adeninate bio-MOFs (bio-MOFs 11-14) is reported. The pores of bio-MOFs 11-14 are decorated with acetate, propionate, butyrate, and valerate, respectively. The nitrogen (N{sub 2}) and carbon dioxide (CO{sub 2}) adsorption properties of these materials are studied and compared. The isosteric heats of adsorption for CO{sub 2} are calculated, and the CO{sub 2}:N{sub 2} selectivities for each material are 10 determined. As the lengths of the aliphatic chains decorating the pores in bio-MOFs 11-14 increase, the BET surface areas decrease from 1148 m{sup 2}/g to 17 m{sup 2}/g while the CO{sub 2}:N{sub 2} selectivities predicted from idealmore » adsorbed solution theory at 1 bar and 273 K for a 10:90 CO{sub 2}:N{sub 2} mixture range from 73:1 for bio-MOF-11 to 123:1 for bio-MOF-12 and finally to 107:1 for bio-MOF-13. At 298 K, the selectivities are 43:1 for bio-MOF-11, 52:1 for bio-MOF-12, and 40:1 for bio-MOF-13. Additionally, it is shown that 15 bio-MOF-14 exhibits a unique molecular sieving property that allows it to adsorb CO{sub 2} but not N{sub 2} at 273 and 298 K. Finally, the water stability of bio-MOFs 11-14 increases with increasing aliphatic chain length. Bio-MOF-14 exhibits no loss of crystallinity or porosity after soaking in water for one month.« less

Rectification induced in N{sub 2}{sup AA}-doped armchair graphene nanoribbon device

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

Chen, Tong; Wang, Ling-Ling, E-mail: llwang@hnu.edu.cn; Luo, Kai-Wu

2014-07-07

By using non-equilibrium Green function formalism in combination with density functional theory, we investigated the electronic transport properties of armchair graphene nanoribbon devices in which one lead is undoped and the other is N{sub 2}{sup AA}-doped with two quasi-adjacent substitutional nitrogen atoms incorporating pairs of neighboring carbon atoms in the same sublattice A. Two kinds of N{sub 2}{sup AA}-doped style are considered, for N dopants substitute the center or the edge carbon atoms. Our results show that the rectification behavior with a large rectifying ratio can be found in these devices and the rectifying characteristics can be modulated by changingmore » the width of graphene nanoribbons or the position of the N{sub 2}{sup AA} dopant. The mechanisms are revealed to explain the rectifying behaviors.« less

Semiconductor to metal transition by tuning the location of N{sub 2}{sup AA} in armchair graphene nanoribbons

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

Chen, Tong; Wang, Ling-Ling, E-mail: llwang@hnu.edu.cn; Li, Quan

2014-02-07

The electronic band structures and transport properties of N{sub 2}{sup AA}-doped armchair graphene nanoribbons (aGNRs) with two quasi-adjacent substitutional nitrogen atoms incorporated in pairs of neighboring carbon atoms in the same sublattice A are investigated by using non-equilibrium Green function formalism in combination with density functional theory. The results show that the coupling effect between the Pz orbitals of carbon and nitrogen atoms plays an important role in the transition between semiconductor and metal by different locations of N{sub 2}{sup AA}-doped aGNRs. And the striking negative differential resistance behaviors can be found in such devices. These tremendous properties suggest potentialmore » application of N{sub 2}{sup AA}-doped aGNRs in graphene-based nanoelectronic devices.« less

The effect of alkali metal on the surface properties of potassium doped Au-Beta zeolites

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

Sobczak, Izabela, E-mail: sobiza@amu.edu.pl; Rydz, Michal; Ziolek, Maria

2013-02-15

Graphical abstract: Display Omitted Highlights: ► Interaction of gold with K leads to the change of electronic state and redox properties of gold. ► The amount of potassium incorporated into Au-zeolites determines the size of gold particles. ► K(0.2 wt.%)/Au-Beta exhibits the best performance in decomposition of N{sub 2}O and removal of Bu{sub 2}S. -- Abstract: Beta zeolite was applied as support for gold introduced by gold-precipitation method and potassium added by impregnation or adsorption. The effect of zeolite composition and the amount of potassium introduced on the surface properties of the final materials was considered. Moreover, the interaction ofmore » gold and potassium species was found to be related to the adsorptive and catalytic behaviour of zeolites in NO reduction with propene and deodorization. K/Au-Beta(Impregnated) exhibits the best performance in the above mentioned processes because of the small gold particles (between 2 and 5 nm) and interaction of gold with potassium species leading to the change of electronic properties of the surface (the appearance of cationic gold species). Potassium added as a promoter improves the catalytic properties of Au-zeolite in N{sub 2}O decomposition and also in deodorization (increase of the ability to dibutyl sulphide oxidation). The catalysts prepared were characterized by XRD, XPS, UV–vis, TEM, pyridine adsorption combined with FTIR and test reaction (2-propanol transformation).« less

Electron density modulation in a pulsed dual-frequency (2/13.56 MHz) dual-antenna inductively coupled plasma discharge

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

Sirse, Nishant, E-mail: nishant.sirse@dcu.ie; Mishra, Anurag; Yeom, Geun Y.

The electron density, n{sub e}, modulation is measured experimentally using a resonance hairpin probe in a pulsed, dual-frequency (2/13.56 MHz), dual-antenna, inductively coupled plasma discharge produced in argon-C{sub 4}F{sub 8} (90–10) gas mixtures. The 2 MHz power is pulsed at a frequency of 1 kHz, whereas 13.56 MHz power is applied in continuous wave mode. The discharge is operated at a range of conditions covering 3–50 mTorr, 100–600 W 13.56 MHz power level, 300–600 W 2 MHz peak power level, and duty ratio of 10%–90%. The experimental results reveal that the quasisteady state n{sub e} is greatly affected by the 2 MHz power levels and slightly affected by 13.56 MHzmore » power levels. It is observed that the electron density increases by a factor of 2–2.5 on increasing 2 MHz power level from 300 to 600 W, whereas n{sub e} increases by only ∼20% for 13.56 MHz power levels of 100–600 W. The rise time and decay time constant of n{sub e} monotonically decrease with an increase in either 2 or 13.56 MHz power level. This effect is stronger at low values of 2 MHz power level. For all the operating conditions, it is observed that the n{sub e} overshoots at the beginning of the on-phase before relaxing to a quasisteady state value. The relative overshoot density (in percent) depends on 2 and 13.56 MHz power levels. On increasing gas pressure, the n{sub e} at first increases, reaching to a maximum value, and then decreases with a further increase in gas pressure. The decay time constant of n{sub e} increases monotonically with pressure, increasing rapidly up to 10 mTorr gas pressure and at a slower rate of rise to 50 mTorr. At a fixed 2/13.56 MHz power level and 10 mTorr gas pressure, the quasisteady state n{sub e} shows maximum for 30%–40% duty ratio and decreases with a further increase in duty ratio.« less

Significant mobility enhancement in extremely thin highly doped ZnO films

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

Look, David C., E-mail: david.look@wright.edu; Wyle Laboratories, Inc., 2601 Mission Point Blvd., Dayton, Ohio 45431; Air Force Research Laboratory Sensors Directorate, 2241 Avionics Circle, Wright-Patterson AFB, Ohio 45433

2015-04-13

Highly Ga-doped ZnO (GZO) films of thicknesses d = 5, 25, 50, and 300 nm, grown on 160-nm ZnO buffer layers by molecular beam epitaxy, had 294-K Hall-effect mobilities μ{sub H} of 64.1, 43.4, 37.0, and 34.2 cm{sup 2}/V-s, respectively. This extremely unusual ordering of μ{sub H} vs d is explained by the existence of a very high-mobility Debye tail in the ZnO, arising from the large Fermi-level mismatch between the GZO and the ZnO. Scattering theory in conjunction with Poisson analysis predicts a Debye-tail mobility of 206 cm{sup 2}/V-s at the interface (z = d), falling to 58 cm{sup 2}/V-s at z = d + 2 nm. Excellent fits to μ{sub H}more » vs d and sheet concentration n{sub s} vs d are obtained with no adjustable parameters.« less

Synthesis of g-C{sub 3}N{sub 4}/Ag{sub 3}PO{sub 4} heterojunction with enhanced photocatalytic performance

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

He, Peizhi; Song, Limin; Zhang, Shujuan, E-mail: songlmnk@sohu.com

2014-03-01

Graphical abstract: g-C{sub 3}N{sub 4}/Ag{sub 3}PO{sub 4} heterojunction photocatalyst with visible-light response was prepared by a facile coprecipitation method. The results show that g-C{sub 3}N{sub 4}/Ag{sub 3}PO{sub 4} possesses a much higher activity for the decomposition of RhB than that of the pure Ag{sub 3}PO{sub 4} particles. The most mechanism is that g-C{sub 3}N{sub 4}/Ag{sub 3}PO{sub 4} heterojunction photocatalyst can efficiently separate the photogenerated electron–hole pairs, enhancing the photocatalytic activity of g-C{sub 3}N{sub 4}/Ag{sub 3}PO{sub 4} composites. - Highlights: • g-C{sub 3}N{sub 4}/Ag{sub 3}PO{sub 4} heterojunction showed much higher activity than that of Ag{sub 3}PO{sub 4}. • The high activitymore » could be attributed to g-C{sub 3}N{sub 4} for modifying Ag{sub 3}PO{sub 4}. • More ·OH radicals may be significant reason to improve Ag{sub 3}PO{sub 4} activity. - Abstract: g-C{sub 3}N{sub 4}/Ag{sub 3}PO{sub 4} heterojunction photocatalyst with visible-light response was prepared by a facile coprecipitation method. The photocatalysts were characterized by X-ray powder diffraction, transmission electron microscopy, UV–vis absorption spectroscopy and Fourier transform infrared spectroscopy. The photocatalytic activities of the obtained samples were tested by using Rhodamine B (RhB) as the degradation target under visible light irradiation. g-C{sub 3}N{sub 4}/Ag{sub 3}PO{sub 4} decomposed RhB more effectively than the pure Ag{sub 3}PO{sub 4} particles did, and 2 wt.% g-C{sub 3}N{sub 4} had the highest activity. Furthermore, 2 wt.% g-C{sub 3}N{sub 4}/Ag{sub 3}PO{sub 4} degraded high-concentration RhB more potently than unmodified Ag{sub 3}PO{sub 4} did, probably because g-C{sub 3}N{sub 4}/Ag{sub 3}PO{sub 4} heterojunction photocatalyst enhanced the photocatalytic activity by efficiently separating the photogenerated electron–hole pairs.« less

Weak Hard X-Ray Emission from Two Broad Absorption Line Quasars Observed with NuStar: Compton-Thick Absorption or Intrinsic X-Ray Weakness?

NASA Technical Reports Server (NTRS)

Luo, B.; Brandt, W. N.; Alexander, D. M.; Harrison, F. A.; Stern, D.; Bauer, F. E.; Boggs, S. E.; Christensen, F. E.; Comastri, A.; Craig, W. W..;

WEAK HARD X-RAY EMISSION FROM TWO BROAD ABSORPTION LINE QUASARS OBSERVED WITH NuSTAR: COMPTON-THICK ABSORPTION OR INTRINSIC X-RAY WEAKNESS?

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

Luo, B.; Brandt, W. N.; Alexander, D. M.

We present Nuclear Spectroscopic Telescope Array (NuSTAR) hard X-ray observations of two X-ray weak broad absorption line (BAL) quasars, PG 1004+130 (radio loud) and PG 1700+518 (radio quiet). Many BAL quasars appear X-ray weak, probably due to absorption by the shielding gas between the nucleus and the accretion-disk wind. The two targets are among the optically brightest BAL quasars, yet they are known to be significantly X-ray weak at rest-frame 2-10 keV (16-120 times fainter than typical quasars). We would expect to obtain Almost-Equal-To 400-600 hard X-ray ({approx}> 10 keV) photons with NuSTAR, provided that these photons are not significantlymore » absorbed (N{sub H} {approx}< 10{sup 24} cm{sup -2}). However, both BAL quasars are only detected in the softer NuSTAR bands (e.g., 4-20 keV) but not in its harder bands (e.g., 20-30 keV), suggesting that either the shielding gas is highly Compton-thick or the two targets are intrinsically X-ray weak. We constrain the column densities for both to be N{sub H} Almost-Equal-To 7 Multiplication-Sign 10{sup 24} cm{sup -2} if the weak hard X-ray emission is caused by obscuration from the shielding gas. We discuss a few possibilities for how PG 1004+130 could have Compton-thick shielding gas without strong Fe K{alpha} line emission; dilution from jet-linked X-ray emission is one likely explanation. We also discuss the intrinsic X-ray weakness scenario based on a coronal-quenching model relevant to the shielding gas and disk wind of BAL quasars. Motivated by our NuSTAR results, we perform a Chandra stacking analysis with the Large Bright Quasar Survey BAL quasar sample and place statistical constraints upon the fraction of intrinsically X-ray weak BAL quasars; this fraction is likely 17%-40%.« less

Breakdown of Universality for Unequal-Mass Fermi Gases with Infinite Scattering Length

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

Blume, D.; Daily, K. M.

We treat small trapped unequal-mass two-component Fermi gases at unitarity within a nonperturbative microscopic framework and investigate the system properties as functions of the mass ratio {kappa}, and the numbers N{sub 1} and N{sub 2} of heavy and light fermions. While equal-mass Fermi gases with infinitely large interspecies s-wave scattering length a{sub s} are universal, we find that unequal-mass Fermi gases are, for sufficiently large {kappa} and in the regime where Efimov physics is absent, not universal. In particular, the (N{sub 1},N{sub 2})=(2,1) and (3, 1) systems exhibit three-body and four-body resonances at {kappa}=12.314(2) and 10.4(2), respectively, as well asmore » surprisingly large finite-range effects. These findings have profound implications for ongoing experimental efforts and quantum simulation proposals that utilize unequal-mass atomic Fermi gases.« less

A Volcanic Hydrogen Habitable Zone

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

Ramirez, Ramses M.; Kaltenegger, Lisa, E-mail: rmr277@cornell.edu

The classical habitable zone (HZ) is the circular region around a star in which liquid water could exist on the surface of a rocky planet. The outer edge of the traditional N{sub 2}–CO{sub 2}–H{sub 2}O HZ extends out to nearly ∼1.7 au in our solar system, beyond which condensation and scattering by CO{sub 2} outstrips its greenhouse capacity. Here, we show that volcanic outgassing of atmospheric H{sub 2} can extend the outer edge of the HZ to ∼2.4 au in our solar system. This wider volcanic-hydrogen HZ (N{sub 2}–CO{sub 2}–H{sub 2}O–H{sub 2}) can be sustained as long as volcanic H{submore » 2} output offsets its escape from the top of the atmosphere. We use a single-column radiative-convective climate model to compute the HZ limits of this volcanic hydrogen HZ for hydrogen concentrations between 1% and 50%, assuming diffusion-limited atmospheric escape. At a hydrogen concentration of 50%, the effective stellar flux required to support the outer edge decreases by ∼35%–60% for M–A stars. The corresponding orbital distances increase by ∼30%–60%. The inner edge of this HZ only moves out ∼0.1%–4% relative to the classical HZ because H{sub 2} warming is reduced in dense H{sub 2}O atmospheres. The atmospheric scale heights of such volcanic H{sub 2} atmospheres near the outer edge of the HZ also increase, facilitating remote detection of atmospheric signatures.« less

N sub 2 -fixation by freshly isolated Nostoc from coralloid roots of the cycad Macrozamia riedlei (Fisch. ex Gaud. ) Gardn

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

Lindblad, P.; Atkins, C.A.; Pate, J.S.

1991-03-01

Nitrogenase (EC 1.7.99.2) activity (acetylene reduction) and nitrogen fixation ({sup 15}N{sub 2} fixation) were measured in cyanobacteria freshly isolated from the coralloid roots of Macrozamia riedlei (Fisch. ex Gaud.) Gardn. The data indicate that cyanobacteria within cycad coralloid roots are differentiated specifically for symbiotic functioning in a microaerobic environment. Specializations include a high heterocyst frequency, enhanced permeability to O{sub 2}, and a direct dependence on the cycad for substrates to support nitrogenase activity.

Ultra-thin g-C{sub 3}N{sub 4} nanosheets wrapped silicon nanowire array for improved chemical stability and enhanced photoresponse

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

Wang, Beibei; Yu, Hongtao; Quan, Xie, E-mail: quanxie@dlut.edu.cn

2014-11-15

Highlights: • g-C{sub 3}N{sub 4}, as an oxygen free and metal free protective material for Si, was proposed. • g-C{sub 3}N{sub 4} nanosheets wrapped Si nanowire array was synthesized. • SiNW/g-C{sub 3}N{sub 4} exhibited enhancement of photoelectrochemical stability and photocurrent. - Abstract: In order to inhibit the oxidation of Si materials in aqueous solution, Si nanowire array was wrapped by ultra-thin g-C{sub 3}N{sub 4} nanosheets via an electrophoresis process. Scanning electron microscopy and transmission electron microscopy images showed that g-C{sub 3}N{sub 4} nanosheets were evenly distributed on the surface of Si nanowire array. X-ray diffraction patterns indicated that Si nanowiremore » array/g-C{sub 3}N{sub 4} nanosheets were composed of Si (4 0 0 crystal plane) and g-C{sub 3}N{sub 4} (0 0 2 and 1 0 0 crystal planes). The cyclic voltammetry curves revealed that the corrosion of Si nanowire array was restrained under the protection of g-C{sub 3}N{sub 4} nanosheets. Furthermore, the photocurrent density of Si nanowire array/g-C{sub 3}N{sub 4} nanosheets increased by nearly 3 times compared to that of bare Si nanowire array due to the effective charge separation caused by the built-in electric field at the interface. This work will facilitate the applications of Si materials in aqueous solution, such as solar energy harvest and photocatalytic pollution control.« less

Mechanical membrane for the separation of a paramagnetic constituent from a fluid

DOEpatents

Maurice, David

2017-05-02

The disclosure provides an apparatus and method for the separation of a paramagnetic component from a mixture using a mechanical membrane apparatus. The mechanical membrane comprises a supporting material having a plurality of pores where each pore is surrounded by a plurality of magnetic regions. The magnetic regions augment a magnetic field on one side of the supporting material while mitigating the field to near zero on the opposite side. In operation, a flow of fluid such as air comprising a paramagnetic component such as O.sub.2 is directed toward the mechanical membrane, and the paramagnetic component is typically attracted toward a magnetic field surrounding a pore while dimagnetic components such as N.sub.2 are generally repelled. As some portion of the fluid passes through the plurality of magnetic apertures to the opposite side of the mechanical membrane, the mechanical membrane generates a fluid enriched in the paramagnetic component. Alternately, the magnetic field may act to repel the paramagnetic component while diamagnetic components such as N.sub.2 are generally unaffected and pass to the opposite side of the mechanical membrane.

Communication: Two types of flat-planes conditions in density functional theory

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

Yang, Xiaotian Derrick; Patel, Anand H. G.; González-Espinoza, Cristina E.

Using results from atomic spectroscopy, we show that there are two types of flat-planes conditions. The first type of flat-planes condition occurs when the energy as a function of the number of electrons of each spin, N{sub α} and N{sub β}, has a derivative discontinuity on a line segment where the number of electrons, N{sub α} + N{sub β}, is an integer. The second type of flat-planes condition occurs when the energy has a derivative discontinuity on a line segment where the spin polarization, N{sub α} – N{sub β}, is an integer, but does not have a discontinuity associated withmore » an integer number of electrons. Type 2 flat planes are rare—we observed just 15 type 2 flat-planes conditions out of the 4884 cases we tested—but their mere existence has implications for the design of exchange-correlation energy density functionals. To facilitate the development of functionals that have the correct behavior with respect to both fractional number of electrons and fractional spin polarization, we present a dataset for the chromium atom and its ions that can be used to test new functionals.« less

Domain walls in supersymmetric QCD: The taming of the zoo

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

Binosi, Daniele; ter Veldhuis, Tonnis

We provide a unified picture of the domain wall spectrum in supersymmetric QCD with N{sub c} colors and N{sub f} flavors of quarks in the (anti) fundamental representation. Within the framework of the Veneziano-Yankielowicz-Taylor effective Lagrangian, we consider domain walls connecting chiral symmetry breaking vacua, and we take the quark masses to be degenerate. For N{sub f}/N{sub c}<1/2, there is one BPS saturated domain wall for any value of the quark mass m. For 1/2{<=}N{sub f}/N{sub c}<1 there are two critical masses m{sub *} and m{sub **} which depend on the number of colors and flavors only through the ratiomore » N{sub f}/N{sub c}. If mm{sub **}, there is no domain wall. We numerically determine m{sub *} and m{sub **} as a function of N{sub f}/N{sub c}, and we find that m{sub **} approaches a constant value in the limit that this ratio goes to 1.« less

The Non-Stellar Infrared Continuum of Seyfert Galaxies

NASA Technical Reports Server (NTRS)

Alonso-Herrero, Almudena; Quillen, Alice C.; Simpson, Chris; Efstathiou, Andreas; Ward, Martin J.

2000-01-01

JHKL'M (1 - 5 micrometers) imaging of a sample of Seyfert 2 galaxies is presented. We have performed an accurate estimate of the near-infrared non-stellar nuclear fluxes. We confirm that the near-infrared nuclear continuum between 1 and 2.2microns of some Seyfert 2s is dominated by stellar emission, whereas the continuum emission at longer wavelengths (lambda = 3 - 5 micrometers) is almost entirely non-stellar in origin. The non-stellar spectral energy distributions (SED) in the infrared (up to 15 micrometers) of Seyfert galaxies show a variety of shapes, and they are well reproduced with the tapered disk models of Efstathiou & Rowan-Robinson (1995). We have used two models, one including an optically thin cone component found to fit the SED of NGC 1068, and a coneless model. Although our modelling of the SEDs does not allow us to favor either model to account for all the observed SEDs, we find that the viewing angle towards the central source is well constrained by both models. The galaxies in our sample have fitted values of the viewing angle in the range Theta(sub V) = 0 deg - 64 deg, for the assumed model parameters. We have also investigated non-stellar color-color diagrams (L' - M vs. H - M and L' - M vs. H - L'). The colors of the Seyfert galaxies with viewing angles Theta(sub v) less than 30 deg are better reproduced with the cone model. These diagrams provide a good means to separate Seyfert 2s with moderate obscuration (A(sub V) approx. less than 20 mag from hard X-ray observations) from those with high obscuration. The ground-based 4.8 microns and ISO 9.6 microns luminosities are well correlated with the hard X-ray luminosities of Seyfert ls and 2s. These continuum emissions appear as a good indicator of the AGN luminosity, at least in the cases of hard X-ray Compton-thin Seyfert galaxies (N(sub H) less than or = 10(exp 24)/sq cm). We finally stress the finding that some Compton thick galaxies show bright non-stellar emission at 5 microns This suggests that the near-infrared emission in Seyfert galaxies is produced in an extended component illuminated by the central source, that is more visible from all viewing angles, providing a good explanation for the differing N(sub H)/A(sub V) ratios found in some Seyfert 2s. We discuss possible implications of mid-infrared surveys for the search of counterparts of highly obscured hard X-ray sources.

Electrochemical reduction of nitrate in the presence of an amide

DOEpatents

Dziewinski, Jacek J.; Marczak, Stanislaw

2002-01-01

The electrochemical reduction of nitrates in aqueous solutions thereof in the presence of amides to gaseous nitrogen (N.sub.2) is described. Generally, electrochemical reduction of NO.sub.3 proceeds stepwise, from NO.sub.3 to N.sub.2, and subsequently in several consecutive steps to ammonia (NH.sub.3) as a final product. Addition of at least one amide to the solution being electrolyzed suppresses ammonia generation, since suitable amides react with NO.sub.2 to generate N.sub.2. This permits nitrate reduction to gaseous nitrogen to proceed by electrolysis. Suitable amides include urea, sulfamic acid, formamide, and acetamide.

Communication: Determining the structure of the N{sub 2}Ar van der Waals complex with laser-based channel-selected Coulomb explosion

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

Wu, Chengyin, E-mail: cywu@pku.edu.cn; Liu, Yunquan; Gong, Qihuang

2014-04-14

We experimentally reconstructed the structure of the N{sub 2}Ar van der Waals complex with the technique of laser-based channel-selected Coulomb explosion imaging. The internuclear distance between the N{sub 2} center of mass and the Ar atom, i.e., the length of the van der Waals bond, was determined to be 3.88 Å from the two-body explosion channels. The angle between the van der Waals bond and the N{sub 2} principal axis was determined to be 90° from the three-body explosion channels. The reconstructed structure was contrasted with our high level ab initio calculations. The agreement demonstrated the potential application of laser-basedmore » Coulomb explosion in imaging transient molecular structure, particularly for floppy van der Waals complexes, whose structures remain difficult to be determined by conventional spectroscopic methods.« less

The FUSE Survey of 0 VI in the Galactic Halo

NASA Technical Reports Server (NTRS)

Sonneborn, George; Savage, B. D.; Wakker, B. P.; Sembach, K. R.; Jenkins, E. B.; Moos, H. W.; Shull, J. M.

2003-01-01

This paper summarizes the results of the Far-Ultraviolet Spectroscopic Explorer (FUSE) program to study 0 VI in the Milky Way halo. Spectra of 100 extragalactic objects and two distant halo stars are analyzed to obtain measures of O VI absorption along paths through the Milky Way thick disk/halo. Strong O VI absorption over the velocity range from -100 to 100 km/s reveals a widespread but highly irregular distribution of O VI, implying the existence of substantial amounts of hot gas with T approx. 3 x 10(exp 5) K in the Milky Way thick disk/halo. The overall distribution of O VI is not well described by a symmetrical plane-parallel layer of patchy O VI absorption. The simplest departure from such a model that provides a reasonable fit to the observations is a plane-parallel patchy absorbing layer with an average O VI mid-plane density of n(sub 0)(O VI) = 1.7 x 10(exp -2)/cu cm, a scale height of approx. 2.3 kpc, and a approx. 0.25 dex excess of O VI in the northern Galactic polar region. The distribution of O VI over the sky is poorly correlated with other tracers of gas in the halo, including low and intermediate velocity H I, Ha emission from the warm ionized gas at approx. l0(exp 4) K, and hot X-ray emitting gas at approx. l0(exp 6) K . The O VI has an average velocity dispersion, b approx. 60 km/s and standard deviation of 15 km/s. Thermal broadening alone cannot explain the large observed profile widths. A combination of models involving the radiative cooling of hot fountain gas, the cooling of supernova bubbles in the halo, and the turbulent mixing of warm and hot halo gases is required to explain the presence of O VI and other highly ionized atoms found in the halo. The preferential venting of hot gas from local bubbles and superbubbles into the northern Galactic polar region may explain the enhancement of O VI in the North.

STUDYING THE WHIM CONTENT OF LARGE-SCALE STRUCTURES ALONG THE LINE OF SIGHT TO H 2356-309

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

Zappacosta, L.; Nicastro, F.; Maiolino, R.

2010-07-01

We make use of a 500 ks Chandra HRC-S/LETG spectrum of the blazar H 2356-309, combined with a lower signal-to-noise ratio (S/N; 100 ks) pilot LETG spectrum of the same target, to search for the presence of warm-hot absorbing gas associated with two large-scale structures (LSSs) crossed by this sight line and to constrain its physical state and geometry. Strong (log N{sub O{sub VII}} {>=} 10{sup 16} cm{sup -2}) O VII K{alpha} absorption associated with a third LSS crossed by this line of sight (the Sculptor Wall (SW)), at z = 0.03, has already been detected in a previous work.more » Here, we focus on two additional prominent filamentary LSSs along the same line of sight, one at z = 0.062 (the Pisces-Cetus Supercluster (PCS)) and another at z = 0.128 (the 'Farther Sculptor Wall' (FSW)). The combined LETG spectrum has an S/N of {approx}11.6-12.6 per resolution element in the 20-25 A and an average 3{sigma} sensitivity to intervening O VII K{alpha} absorption line equivalent widths (EWs) of EW{sub O{sub VII}} {approx_gt} 14 mA in the available redshift range (z < 0.165). No statistically significant (i.e., {>=}3{sigma}) individual absorption is detected from any of the strong He- or H-like transitions of C, O, and Ne (the most abundant metals in gas with solar-like composition) at the redshifts of the PCS and FSW structures and down to the EW thresholds mentioned above. However, we are still able to constrain the physical and geometrical parameters of the putative absorbing gas associated with these structures, by performing a joint spectral fit of various marginal detections and upper limits of the strongest expected lines with our self-consistent hybrid-ionization WHIM spectral model. At the redshift of the PCS, we identify a warm phase with log T = 5.35{sup +0.07}{sub -0.13} K and log N{sub H} = (19.1 {+-} 0.2) cm{sup -2} possibly co-existing with a much hotter and statistically less significant phase with log T = 6.9{sup +0.1}{sub -0.8} K and log N{sub H} = 20.1{sup +0.3}{sub -1.7} cm{sup -2} (1{sigma} errors). These two separate physical phases are identified through, and mainly constrained by, C V K{alpha} (warm phase) and O VIII K{alpha} (hot phase) absorption, with single line significances of 1.5{sigma} each. For the second LSS, at z {approx_equal} 0.128, only one hot component is hinted in the data, through O VIII K{alpha} (1.6{sigma}) and Ne IX K{alpha} (1.2{sigma}). For this system, we estimate log T = 6.6{sup +0.1}{sub -0.2} K and log N{sub H} = 19.8{sup +0.4}{sub -0.8} cm{sup -2}. Our column density and temperature constraints on the warm-hot gaseous content of these two LSSs, combined with the measurements obtained for the hot gas permeating the SW, allow us to estimate the cumulative number density per unit redshifts of O VII WHIM absorbers at three different EW thresholds of 0.4 mA, 7 mA, and 25.8 mA. This is consistent with expectations only at the very low end of EW thresholds, but exceeds predictions at 7 mA and 25.8 mA (by more than 2{sigma}). We also estimate the cosmological mass density of the WHIM based on the four absorbers we tentatively detect along this line of sight, obtaining {Omega}{sup WHIM}{sub b} = (0.021{sup +0.031}{sub -0.018})(Z/Z{sub sun}){sup -1}, consistent with the cosmological mass density of the intergalactic 'missing baryons' only if we assume high metallicities (Z {approx} Z{sub sun}).« less

Novel Metal Ion Based Estrogen Mimics for Molecular Imaging

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

Rajagopalan, Raghavan

The overall objective of the SBIR Phase I proposal is to prepare and evaluate a new class of {sup 99m}Tc or {sup 94m}Tc containing estrogen-like small molecules ('estrogen mimics') for SPECT or PET molecular imaging of estrogen receptor positive (ER+) tumors. In this approach, the metal ion is integrated into the estrone skeleton by isosteric substitution of a carbon atom in the steroidal structure to give new class of mimics that are topologically similar to the native estrogen (Fig. 1). Although both N{sub 2}S{sub 2} and N{sub 3}S mimics 1 and 2 were considered as target structures, molecular modeling studymore » revealed that the presence of the acetyl group at position-15 in the N{sub 3}S mimic 2 causes steric hinderance toward binding of 2 to SHBG. Therefore, initial efforts were directed at the synthesis and evaluation of the N{sub 2}S{sub 2} mimic 1.« less

Synthesis and crystal structure of (S, S, S, S)-N, N′-bis[N-(P-toluenesulfonamido)-1,2-diphenylethyl]ethylenediamine

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

Liu, X.-G.; Zhang, T.; Hu, Y.-Y.

2013-12-15

(S, S, S, S)-N,N′-bis[N-(p-toluenesulfonamido)-1,2-diphenylethyl] ethylenediamine (C{sub 44}H{sub 46}N{sub 4}O{sub 4}S{sub 2}), has been synthesized and structurally characterized by elemental analysis, {sup 1}H-NMR, MS, IR and single-crystal X-ray diffraction. The title compound contains four chiral centers with C atoms in S configuration. Molecules are connected to one another by hydrogen bonds between sulfonamide nitrogen and sulfonyl oxygen to form chains alone a axis.

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

Levendis, Y.A.

A study was conducted to determine the efficacy of carboxylic calcium and magnesium salts (e.g., calcium magnesium acetate or CMA, CaMg{sub 2}(CH{sub 2}COOH){sub 6}) for the simultaneous removal of SO{sub 2} and NO{sub x} in oxygen-lean atmospheres. Experiments were performed in a high-temperature furnace that simulated the post-flame environment of a coal-fired boiler by providing similar temperatures and partial pressures of SO{sub 2}, NO{sub x} CO{sub 2} and O{sub 2}. When injected into a hot environment, the salts calcined and formed highly porous {open_quotes}popcorn{close_quotes}-like cenospheres. Residual MgO and/or CaCO{sub 3} and CaO reacted heterogeneously with SO{sub 2} to form MgSO{submore » 4} and/or CaCO{sub 4}. The organic components - which can be manufactured from wastes such as sewage sludge - gasified and reduced NO{sub x }to N{sub 2} efficiently if the atmosphere was moderately fuel-rich. Dry-injected CMA particles at a Ca/S ratio of 2, residence time of 1 second and bulk equivalence ratio of 1.3 removed over 90% of SO{sub 2} and NO{sub x} at gas temperatures {>=} 950{degrees}C. When the furnace isothermal zone was {<=} 950{degrees}C, Ca was essentially inert in the furnace quenching zone, while Mg continued to sorb SO{sub 2} as the gas temperature cooled at a rate of -130{degrees}C/sec. Hence, the removal of SO{sub 2} by CMA could continue for nearly the entire residence time of emissions in the exhaust stream of a power plant. Additional research is needed to improve the efficiency and reduce the cost of the relatively expensive carboxylic acid salts as dual SO{sub 2}-NO{sub x} reduction agents. For example, wet injection of the salts could be combined with less expensive hydrocarbons such as lignite or even polymers such as poly(ethylene) that could be extracted from the municipal waste stream.« less

Synthesis and crystal structures of coordination compounds of pyridoxine with zinc and cadmium sulfates

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

Furmanova, N. G., E-mail: furm@ns.crys.ras.ru; Berdalieva, Zh. I., E-mail: kakin@inbox.ru; Chernaya, T. S.

2009-03-15

The pyridoxine complexes with zinc and cadmium sulfates are synthesized. The IR absorption spectra and thermal behavior of the synthesized compounds are described. Crystals of the [M(C{sub 8}H{sub 11}O{sub 3}N){sub 2}(H{sub 2}O){sub 2}]SO{sub 4} . 3H{sub 2}O (M = Zn, Cd) compounds are investigated using X-ray diffraction. In the structures of both compounds, the M atoms are coordinated by the oxygen atoms of the deprotonated OH group and the CH{sub 2}OH group retaining its own hydrogen atom, as well as by two H{sub 2}O molecules, and have an octahedral coordination. The nitrogen atom of the heterocycle is protonated, so thatmore » the heterocycle acquires a pyridinium character. The cationic complexes form layers separated by the anions and crystallization water molecules located in between. The structural units of the crystals are joined together by a complex system of hydrogen bonds.« less

Study of nitrogen flowing afterglow with mercury vapor injection

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

Mazánková, V., E-mail: mazankova@fch.vutbr.cz; Krčma, F.; Trunec, D.

2014-10-21

The reaction kinetics in nitrogen flowing afterglow with mercury vapor addition was studied by optical emission spectroscopy. The DC flowing post-discharge in pure nitrogen was created in a quartz tube at the total gas pressure of 1000 Pa and discharge power of 130 W. The mercury vapors were added into the afterglow at the distance of 30 cm behind the active discharge. The optical emission spectra were measured along the flow tube. Three nitrogen spectral systems – the first positive, the second positive, and the first negative, and after the mercury vapor addition also the mercury resonance line at 254more » nm in the spectrum of the second order were identified. The measurement of the spatial dependence of mercury line intensity showed very slow decay of its intensity and the decay rate did not depend on the mercury concentration. In order to explain this behavior, a kinetic model for the reaction in afterglow was developed. This model showed that the state Hg(6 {sup 3}P{sub 1}), which is the upper state of mercury UV resonance line at 254 nm, is produced by the excitation transfer from nitrogen N{sub 2}(A{sup 3}Σ{sup +}{sub u}) metastables to mercury atoms. However, the N{sub 2}(A{sup 3}Σ{sup +}{sub u}) metastables are also produced by the reactions following the N atom recombination, and this limits the decay of N{sub 2}(A{sup 3}Σ{sup +}{sub u}) metastable concentration and results in very slow decay of mercury resonance line intensity. It was found that N atoms are the most important particles in this late nitrogen afterglow, their volume recombination starts a chain of reactions which produce excited states of molecular nitrogen. In order to explain the decrease of N atom concentration, it was also necessary to include the surface recombination of N atoms to the model. The surface recombination was considered as a first order reaction and wall recombination probability γ = (1.35 ± 0.04) × 10{sup −6} was determined from the experimental data. Also sensitivity analysis was applied for the analysis of kinetic model in order to reveal the main control parameters in the model.« less

Fracture resistance measurement of advanced ceramics at elevated-temperatures using Chevron-notched specimens and other novel techniques

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

Jenkins, M.G.

1995-12-31

The quasi-static fracture behavior of advanced ceramics was assessed in the temperature range of 20{degrees} to 1400{degrees}C. Chevron-notched, three-point flexure specimens and a laser-based CMOD measurement systems were used in testing. Types of materials characterized included monolithic ceramics (SiC, Si{sub 3}N{sub 4}, MgAl{sub 2}O{sub 4}), self-reinforced monoliths (acicular-grained Si{sub 3}N{sub 4}, acicular grained mullite), and ceramic matrix composites (SiC whisker/Al{sub 2}O{sub 3} matrix, TiB{sub 2} particulate/SiC matrix, SiC fibre/CVI SiC matrix, Al{sub 2}O{sub 3} fibre/CVI SiC matrix). Fracture resistance behaviour of the materials was quantified as three distinct regimes of the fracture histories. At crack initiation, the apparent fracture toughnessmore » was evaluated as the critical stress intensity factor, K{sub IC}. During stable crack propagation, the crack growth resistance was characterized by the instantaneous strain energy release rate, G{sub R} using a compliance method assuming linear-elastic unloading to calculate the effective crack lengths. At final fracture, the complete fracture process was quantified using the work-of-fracture, WOF, which can be equated to the fracture surface energy for linearelastic materials. Results indicate that the chevron-notched, three-point flexure specimen facilitates the study of fracture behavior in a wide range of brittle and quasi-brittle materials at elevated temperatures. The unique features of the chevron geometry, which are automatic, in-situ crack initiation and inherent stable crack growth, are crucial to the successful evaluation of the fracture tests.« less

Porous carbon derived via KOH activation of a hypercrosslinked porous organic polymer for efficient CO{sub 2}, CH{sub 4}, H{sub 2} adsorptions and high CO{sub 2}/N{sub 2} selectivity

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

Modak, Arindam; Bhaumik, Asim, E-mail: msab@iacs.res.in

2015-12-15

Microporous carbon having Brunauer-Emmett-Teller (BET) surface area of 2186 m{sup 2} g{sup −1} and micropore volume of 0.85 cm{sup 3} g{sup −1} has been synthesized via KOH induced high temperature carbonization of a non-conjugated hypercrosslinked organic polymer. Owing to the templating and activation by KOH, we have succeeded in making a microporous carbon from this porous polymer and the resultant carbon material showed high uptake for CO{sub 2} (7.6 mmol g{sup −1}) and CH{sub 4} (2.4 mmol g{sup −1}) at 1 atm, 273 K together with very good selectivity for the CO{sub 2}/N{sub 2} (30.2) separation. Furthermore, low pressure (1more » atm) H{sub 2} (2.6 wt%, 77 K) and water uptake (57.4 wt%, 298 K) ability of this polymer derived porous activated carbon is noteworthy. - Graphical abstract: Microporous carbon with BET surface area of 2186 m{sup 2} g{sup −1} has been synthesized via KOH activation of a porous organic polymer and it showed high uptake for CO{sub 2} (7.6 mmol g{sup −1}), CH{sub 4} (2.4 mmol g{sup −1}) and H{sub 2} (2.6 wt%) at 1 atm together with very good selectivity for CO{sub 2}. - Highlights: • Porous carbon from hypercrosslinked organic polymer. • KOH activated carbon with BET surface area 2186 m{sup 2} g{sup −1}. • High CO2 uptake (7.6 mmol g{sup −1}) and CO{sub 2}/N{sub 2} selectivity (30.2). • Porous carbon also showed high H{sub 2} (2.6 wt%) and H{sub 2}O (57.4 wt%) uptakes.« less

Valorization of GaN based metal-organic chemical vapor deposition dust a semiconductor power device industry waste through mechanochemical oxidation and leaching: A sustainable green process

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

Swain, Basudev, E-mail: Swain@iae.re.kr; Mishra, Chinmayee; Lee, Chan Gi

2015-07-15

Dust generated during metal organic vapor deposition (MOCVD) process of GaN based semiconductor power device industry contains significant amounts of gallium and indium. These semiconductor power device industry wastes contain gallium as GaN and Ga{sub 0.97}N{sub 0.9}O{sub 0.09} is a concern for the environment which can add value through recycling. In the present study, this waste is recycled through mechanochemical oxidation and leaching. For quantitative recovery of gallium, two different mechanochemical oxidation leaching process flow sheets are proposed. In one process, first the Ga{sub 0.97}N{sub 0.9}O{sub 0.09} of the MOCVD dust is leached at the optimum condition. Subsequently, the leachmore » residue is mechanochemically treated, followed by oxidative annealing and finally re-leached. In the second process, the MOCVD waste dust is mechanochemically treated, followed by oxidative annealing and finally leached. Both of these treatment processes are competitive with each other, appropriate for gallium leaching and treatment of the waste MOCVD dust. Without mechanochemical oxidation, 40.11 and 1.86 w/w% of gallium and Indium are leached using 4 M HCl, 100 °C and pulp density of 100 kg/m{sup 3,} respectively. After mechanochemical oxidation, both these processes achieved 90 w/w% of gallium and 1.86 w/w% of indium leaching at their optimum condition. - Highlights: • Waste MOCVD dust is treated through mechanochemical leaching. • GaN is hardly leached, and converted to NaGaO{sub 2} through ball milling and annealing. • Process for gallium recovery from waste MOCVD dust has been developed. • Thermal analysis and phase properties of GaN to Ga{sub 2}O{sub 3} and GaN to NaGaO{sub 2} is revealed. • Solid-state chemistry involved in this process is reported.« less

ICE CHEMISTRY ON OUTER SOLAR SYSTEM BODIES: ELECTRON RADIOLYSIS OF N{sub 2}-, CH{sub 4}-, AND CO-CONTAINING ICES

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

Materese, Christopher K.; Cruikshank, Dale P.; Sandford, Scott A.

Radiation processing of the surface ices of outer Solar System bodies may be an important process for the production of complex chemical species. The refractory materials resulting from radiation processing of known ices are thought to impart to them a red or brown color, as perceived in the visible spectral region. In this work, we analyzed the refractory materials produced from the 1.2-keV electron bombardment of low-temperature N{sub 2}-, CH{sub 4}-, and CO-containing ices (100:1:1), which simulates the radiation from the secondary electrons produced by cosmic ray bombardment of the surface ices of Pluto. Despite starting with extremely simple icesmore » dominated by N{sub 2}, electron irradiation processing results in the production of refractory material with complex oxygen- and nitrogen-bearing organic molecules. These refractory materials were studied at room temperature using multiple analytical techniques including Fourier-transform infrared spectroscopy, X-ray absorption near-edge structure (XANES) spectroscopy, and gas chromatography coupled with mass spectrometry (GC-MS). Infrared spectra of the refractory material suggest the presence of alcohols, carboxylic acids, ketones, aldehydes, amines, and nitriles. XANES spectra of the material indicate the presence of carboxyl groups, amides, urea, and nitriles, and are thus consistent with the IR data. Atomic abundance ratios for the bulk composition of these residues from XANES analysis show that the organic residues are extremely N-rich, having ratios of N/C ∼ 0.9 and O/C ∼ 0.2. Finally, GC-MS data reveal that the residues contain urea as well as numerous carboxylic acids, some of which are of interest for prebiotic and biological chemistries.« less

Effect of plastic mulching and nitrapyrin on N2O concentration and emissions in China under climate change

NASA Astrophysics Data System (ADS)

Zhao, C.; Zhu, C.

2017-12-01

Fertilized agricultural soils are the main source of atmospheric nitrous oxide (N2O). In this study, both soil N2O concentration in the profile and N2O emission were measured to quantify the effect of plastic mulching and nitrapyrin on N2O dynamic in an oasis cotton field. During the observation period, both N2O concentration and N2O emissions rapidly increased following fertigation, and soil temperature, moisture and mineral N content were the main factors influencing N2O. Temporal variation in N2O emission coincided with changes in N2O content in all soil layers, indicating that the accumulation of N2O likely drives the release of N2O into the atmosphere. The crop yields, N2O content (the sum of aqueous and gaseous phases) in the soil and N2O emissions increased linearly as the application of N fertilizer increased from 80 to 400 kg N ha-1. Plastic mulching increased the crop yields by 16-21%, increased the N2O contents by 88-99%, and reduced the cumulative N2O emissions by 19-28%, indicating that the application of plastic film reduced N2O emission probably through restricted the N2O diffusion process, and limited the N2O production through enhanced the N uptake of cotton. The addition of nitrapyrin to the N fertilizer significantly reduced the levels of N2O without influencing crop yield, with N2O content in the soil profile and cumulative N2O emissions decreasing by 25-32% and 23-42%, respectively. Overall, our result suggested the combined use of plastic film and nitrapyrin could be an efficient practice to reduce N2O emission in the oasis cotton field. Keywords: N2O emissions; plastic film mulching; nitrapyrin; climate change

Spatially explicit estimates of N2 O emissions from croplands suggest climate mitigation opportunities from improved fertilizer management.

PubMed

Gerber, James S; Carlson, Kimberly M; Makowski, David; Mueller, Nathaniel D; Garcia de Cortazar-Atauri, Iñaki; Havlík, Petr; Herrero, Mario; Launay, Marie; O'Connell, Christine S; Smith, Pete; West, Paul C

2016-10-01

With increasing nitrogen (N) application to croplands required to support growing food demand, mitigating N2 O emissions from agricultural soils is a global challenge. National greenhouse gas emissions accounting typically estimates N2 O emissions at the country scale by aggregating all crops, under the assumption that N2 O emissions are linearly related to N application. However, field studies and meta-analyses indicate a nonlinear relationship, in which N2 O emissions are relatively greater at higher N application rates. Here, we apply a super-linear emissions response model to crop-specific, spatially explicit synthetic N fertilizer and manure N inputs to provide subnational accounting of global N2 O emissions from croplands. We estimate 0.66 Tg of N2 O-N direct global emissions circa 2000, with 50% of emissions concentrated in 13% of harvested area. Compared to estimates from the IPCC Tier 1 linear model, our updated N2 O emissions range from 20% to 40% lower throughout sub-Saharan Africa and Eastern Europe, to >120% greater in some Western European countries. At low N application rates, the weak nonlinear response of N2 O emissions suggests that relatively large increases in N fertilizer application would generate relatively small increases in N2 O emissions. As aggregated fertilizer data generate underestimation bias in nonlinear models, high-resolution N application data are critical to support accurate N2 O emissions estimates. © 2016 John Wiley & Sons Ltd.

Infrared dynamics of minimal walking technicolor

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

Del Debbio, Luigi; Lucini, Biagio; Patella, Agostino

2010-07-01

We study the gauge sector of minimal walking technicolor, which is an SU(2) gauge theory with n{sub f}=2 flavors of Wilson fermions in the adjoint representation. Numerical simulations are performed on lattices N{sub t}xN{sub s}{sup 3}, with N{sub s} ranging from 8 to 16 and N{sub t}=2N{sub s}, at fixed {beta}=2.25, and varying the fermion bare mass m{sub 0}, so that our numerical results cover the full range of fermion masses from the quenched region to the chiral limit. We present results for the string tension and the glueball spectrum. A comparison of mesonic and gluonic observables leads to themore » conclusion that the infrared dynamics is given by an SU(2) pure Yang-Mills theory with a typical energy scale for the spectrum sliding to zero with the fermion mass. The typical mesonic mass scale is proportional to and much larger than this gluonic scale. Our findings are compatible with a scenario in which the massless theory is conformal in the infrared. An analysis of the scaling of the string tension with the fermion mass toward the massless limit allows us to extract the chiral condensate anomalous dimension {gamma}{sub *}, which is found to be {gamma}{sub *}=0.22{+-}0.06.« less

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

Simoes, A.Z., E-mail: alezipo@yahoo.com; Riccardi, C.S.; Dos Santos, M.L.

Bismuth ferrite thin films were deposited on Pt/Ti/SiO{sub 2}/Si substrates by a soft chemical method and spin-coating technique. The effect of annealing atmosphere (air, N{sub 2} and O{sub 2}) on the structure and electrical properties of the films are reported. X-ray diffraction analysis reveals that the film annealed in air atmosphere is a single-phase perovskite structure. The films annealed in air showed better crystallinity and the presence of a single BFO phase leading to lower leakage current density and superior ferroelectric hysteresis loops at room temperature. In this way, we reveal that BFO film crystallized in air atmosphere by themore » soft chemical method can be useful for practical applications, including nonvolatile digital memories, spintronics and data-storage media.« less

One-step in situ synthesis of graphene–TiO{sub 2} nanorod hybrid composites with enhanced photocatalytic activity

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

Sun, Mingxuan, E-mail: mingxuansun@sues.edu.cn; Li, Weibin; Sun, Shanfu

2015-01-15

Chemically bonded graphene/TiO{sub 2} nanorod hybrid composites with superior dispersity were synthesized by a one-step in situ hydrothermal method using graphene oxide (GO) and TiO{sub 2} (P25) as the starting materials. The as-prepared samples were characterized by XRD, XPS, TEM, FE-SEM, EDX, Raman, N{sub 2} adsorption, and UV–vis DRS techniques. Enhanced light absorption and a red shift of absorption edge were observed for the composites in the ultraviolet–visible diffuse reflectance spectroscopy (UV–vis DRS). Their effective photocatalytic activity was evaluated by the photodegradation of methylene blue under visible light irradiation. An enhancement of photocatalytic performance was observed over graphene/TiO{sub 2} nanorodmore » hybrid composite photocatalysts, as 3.7 times larger than that of pristine TiO{sub 2} nanorods. This work demonstrated that the synthesis of TiO{sub 2} nanorods and simultaneous conversion of GO to graphene “without using reducing agents” had shown to be a rapid, direct and clean approach to fabricate chemically bonded graphene/TiO{sub 2} nanorod hybrid composites with enhanced photocatalytic performance.« less

Method for reducing CO2, CO, NOX, and SOx emissions

DOEpatents

Lee, James Weifu; Li, Rongfu

2002-01-01

Industrial combustion facilities are integrated with greenhouse gas-solidifying fertilizer production reactions so that CO.sub.2, CO, NO.sub.x, and SO.sub.x emissions can be converted prior to emission into carbonate-containing fertilizers, mainly NH.sub.4 HCO.sub.3 and/or (NH.sub.2).sub.2 CO, plus a small fraction of NH.sub.4 NO.sub.3 and (NH.sub.4).sub.2 SO.sub.4. The invention enhances sequestration of CO.sub.2 into soil and the earth subsurface, reduces N0.sub.3.sup.- contamination of surface and groundwater, and stimulates photosynthetic fixation of CO.sub.2 from the atmosphere. The method for converting CO.sub.2, CO, NO.sub.x, and SO.sub.x emissions into fertilizers includes the step of collecting these materials from the emissions of industrial combustion facilities such as fossil fuel-powered energy sources and transporting the emissions to a reactor. In the reactor, the CO.sub.2, CO, N.sub.2, SO.sub.x, and/or NO.sub.x are converted into carbonate-containing fertilizers using H.sub.2, CH.sub.4, or NH.sub.3. The carbonate-containing fertilizers are then applied to soil and green plants to (1) sequester inorganic carbon into soil and subsoil earth layers by enhanced carbonation of groundwater and the earth minerals, (2) reduce the environmental problem of NO.sub.3.sup.- runoff by substituting for ammonium nitrate fertilizer, and (3) stimulate photosynthetic fixation of CO.sub.2 from the atmosphere by the fertilization effect of the carbonate-containing fertilizers.

INTEGRAL and XMM-Newton Spectral Studies of NGC 4388

NASA Technical Reports Server (NTRS)

Beckmann, V.; Gehrels, N.; Favre, P.; Walter, R.; Courvoisier, T. J.-L.; Petrucci, P.-O.; Malzac, J.

2004-01-01

We present first INTEGRAL and XMM-Newton observations of a Seyfert galaxy, the type 2 AGN NGC 4388. Several INTEGRAL observations performed in 2003 allow us to study the spectrum in the 20 - 300 keV range. In addition two XMM-Newton observations give detailed insight into the 0.2 - 10 keV emission. Comparison with previous observations by BeppoSAX, SIGMA and CGRO/OSSE show that the overall spectrum for soft X-rays up to the gamma-rays can be described by a highly absorbed (N(sub H approx. = 2.7 x 10(exp 23)/sq cm) and variable non-thermal component in addition to constant non-absorbed thermal emission (T approx. = 0.8 keV) of low abundance (Z approx. 5% Z (solar)), plus a constant Fe K a line. The hard X-ray component is well described by a simple power law with a mean photon index of Gamma = 1.7. During the INTEGRAL observations the flux at 100 keV increased by a factor of 1.5. The analysis of XMM-Newton data implies that the emission below 3 keV is decoupled from the AGN and probably due to extended emission as seen in Chandra observations. The constant iron line emission is apparently also decoupled from the direct emission of the central engine and likely to be generated in the obscuring material, e.g. in the molecular torus.

H I, CO, and Planck/IRAS dust properties in the high latitude cloud complex, MBM 53, 54, 55 and HLCG 92 – 35. Possible evidence for an optically thick H I envelope around the CO clouds

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

Fukui, Yasuo; Okamoto, Ryuji; Kaji, Ryohei

We present an analysis of the H I and CO gas in conjunction with the Planck/IRAS submillimeter/far-infrared dust properties toward the most outstanding high latitude clouds MBM 53, 54, 55 and HLCG 92 – 35 at b = –30° to – 45°. The CO emission, dust opacity at 353 GHz (τ{sub 353}), and dust temperature (T {sub d}) show generally good spatial correspondence. On the other hand, the correspondence between the H I emission and the dust properties is less clear than in CO. The integrated H I intensity W{sub H} {sub I} and τ{sub 353} show a large scattermore » with a correlation coefficient of ∼0.6 for a T {sub d} range from 16 K to 22 K. We find, however, that W{sub H} {sub I} and τ{sub 353} show better correlation for smaller ranges of T {sub d} every 0.5 K, generally with a correlation coefficient of 0.7-0.9. We set up a hypothesis that the H I gas associated with the highest T {sub d} ≥ 21.5 K is optically thin, whereas the H I emission is generally optically thick for T {sub d} lower than 21.5 K. We have determined a relationship for the optically thin H I gas between atomic hydrogen column density and τ{sub 353}, N{sub H} {sub I} (cm{sup −2})=(1.5×10{sup 26})⋅τ{sub 353}, under the assumption that the dust properties are uniform and we have applied this to estimate N{sub H} {sub I} from τ{sub 353} for the whole cloud. N{sub H} {sub I} was then used to solve for T {sub s} and τ{sub H} {sub I} over the region. The result shows that the H I is dominated by optically thick gas having a low spin temperature of 20-40 K and a density of 40-160 cm{sup –3}. The H I envelope has a total mass of ∼1.2 × 10{sup 4} M {sub ☉}, an order of magnitude larger than that of the CO clouds. The H I envelope properties derived by this method do not rule out a mixture of H I and H{sub 2} in the dark gas, but we present indirect evidence that most of the gas mass is in the atomic state.« less

Synthesis and White-Light Emission of ZnO/HfO2: Eu Nanocables

PubMed Central

2010-01-01

ZnO/HfO2:Eu nanocables were prepared by radio frequency sputtering with electrospun ZnO nanofibers as cores. The well-crystallized ZnO/HfO2:Eu nanocables showed a uniform intact core–shell structure, which consisted of a hexagonal ZnO core and a monoclinic HfO2 shell. The photoluminescence properties of the samples were characterized. A white-light band emission consisted of blue, green, and red emissions was observed in the nanocables. The blue and green emissions can be attributed to the zinc vacancy and oxygen vacancy defects in ZnO/HfO2:Eu nanocables, and the yellow–red emissions are derived from the inner 4f-shell transitions of corresponding Eu3+ ions in HfO2:Eu shells. Enhanced white-light emission was observed in the nanocables. The enhancement of the emission is ascribed to the structural changes after coaxial synthesis. PMID:20730130

Phase Transition and Structure of Silver Azide at High Pressure

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

D Hou; F Zhang; C Ji

2011-12-31

Silver azide (AgN{sub 3}) was compressed up to 51.3 GPa. The results reveal a reversible second-order orthorhombic-to-tetragonal phase transformation starting from ambient pressure and completing at 2.7 GPa. The phase transition is accompanied by a proximity of cell parameters a and b, a 3{sup o} rotation of azide anions, and a change of coordination number from 4-4 (four short, four long) to eight fold. The crystal structure of the high pressure phase is determined to be in I4/mcm space group, with Ag at 4a, N{sub 1} at 4d, and N{sub 2} at 8h Wyckoff positions. Both of the two phasesmore » have anisotropic compressibility: the orthorhombic phase exhibits an anomalous expansion under compression along a-axis and is more compressive along b-axis than c-axis; the tetragonal phase is more compressive along the interlayer direction than the intralayer directions. The bulk moduli of the orthorhombic and tetragonal phases are determined to be K{sub OT} = 39{+-}5 GPa with K{sub OT'} = 10{+-}7 and K{sub OT} = 57 {+-}2 GPa with K{sub OT'} = 6.6{+-}0.2, respectively.« less

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

Li, Guangci; Liu, Yunqi, E-mail: liuyq@upc.edu.cn; Liu, Di

Boehmite (AlOOH) with hierarchical flower-like structures was synthesized by the solvothermal reaction of AlCl{sub 3}.6H{sub 2}O in the presence of ethanol and toluene at 200 {sup o}C for 24 h. The product was characterized by X-ray powder diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The results show that boehmite with flower-like nanostructures, which aggregated together by the weak hydrogen bonds, was formed through dissolution-deposition process of boehmite microcrystals and the toluene has a great effect on the morphology of product in the reaction system. Meanwhile, the {gamma}-Al{sub 2}O{sub 3} was alsomore » obtained by calcination of above product at 500 {sup o}C for 2 h, and the flower-like morphology kept no change. The surface area of {gamma}-Al{sub 2}O{sub 3} powder was determined to be 166.8 m{sup 2}/g by N{sub 2} adsorption measurement. The possible formation mechanism of flower-like boehmite nanostructures was proposed and discussed.« less

N2O emissions from a nitrogen-enriched river

USGS Publications Warehouse

McMahon, P.B.; Dennehy, K.F.

1999-01-01

Nitrous oxide (N2O) emissions from the South Platte River in Colorado were measured using closed chambers in the fall, winter, and summer of 1994- 1995. The South Platte River was enriched in inorganic N (9-800 ??M) derived from municipal wastewater effluent and groundwater return flows from irrigated agricultural fields. River water was as much as 2500% supersaturated with N2O, and median N2O emission rates from the river surface ranged from less than 90 to 32 600 ??g-N m-2 d-1. Seventy-nine percent of the variance in N2O emission rates was explained by concentrations of total inorganic N in river water and by water temperature. The estimated total annual N2O emissions from the South Platte River were 2 x 1013-6 x 1013 ??g-N yr-1. This amount of annual N2O emissions was similar to the estimated annual N2O emissions from all primary municipal wastewater treatment processes in the United States (1). Results from this study indicate that N-enriched rivers could be important anthropogenic sources of N2O to the atmosphere. However, N2O emission measurements from other N-enriched rivers are needed to better quantify this source.Nitrous oxide (N2O) emissions from the South Platte River in Colorado were measured using closed chambers in the fall, winter, and summer of 1994-1995. The South Platte River was enriched in inorganic N (9-800 ??M) derived from municipal wastewater effluent and groundwater return flows from irrigated agricultural fields. River water was as much as 2500% supersaturated with N2O, and median N2O emission rates from the river surface ranged from less than 90 to 32 600 ??g-N m-2 d-1. Seventy-nine percent of the variance in N2O emission rates was explained by concentrations of total inorganic N in river water and by water temperature. The estimated total annual N2O emissions from the South Platte River were 2??1013-6??1013 ??g-N yr-1. This amount of annual N2O emissions was similar to the estimated annual N2O emissions from all primary municipal wastewater treatment processes in the United States. Results from this study indicate that N-enriched rivers could be important anthropogenic sources of N2O to the atmosphere. However, N2O emission measurements from other N-enriched rivers are needed to better quantify this source.

Potential of two-stage membrane system with recycle stream for CO{sub 2} capture from postcombustion gas

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

Dongxiao Yang; Zhi Wang; Jixiao Wang

2009-09-15

In order to restrict greenhouse gases emissions, CO{sub 2} should be captured from the postcombustion gas for further treatment, for example, geosequestration. In this work, the separation performance of the two-stage membrane system with a recycle stream was investigated using the cross-flow model. For larger CO{sub 2}/N{sub 2} selectivities that can be achieved in the lab, for example, selectivity of 52, the separation target of CO{sub 2} purity >95% and CO{sub 2} recovery >90% can be fulfilled by the two-stage system. The process cost of the two-stage membrane process was investigated. There is an optimum pressure ratio with which themore » capital cost and the energy cost can be balanced to minimize the total cost. Using the optimum pressure ratios and efficient membranes, the total cost of the two-stage system can be reduced to a range that is competitive with the process cost of the traditional chemical absorption method. For example, with feed compression applied, the total cost of the two-stage membrane system using the membrane with CO{sub 2}/N{sub 2} selectivity of 52 and CO{sub 2} permeance of 3.12 x 10{sup -3} m{sup 3} (STP) m{sup -2} s{sup -1} MPa{sup -1} is estimated to be $47.9/(ton CO{sub 2} recovered). 22 refs., 11 figs., 3 tabs.« less

Minor Merger Origin for the Circumnuclear Starburst in NGC 7742

NASA Technical Reports Server (NTRS)

Mazzuca, Lisa M.; Sarzi, M.; Knapen, J. H.; Veilleux, S.; Swaters, R.

2006-01-01

We present an emission-line diagnostic analysis of integral-field spectroscopic observations that cover the central kiloparsec of NGC 7742. This Sa galaxy hosts a spectacular nuclear starburst ring and nuclear regions characterized by low-ionization emission. The gas in the ring rotates in the opposite sense to the stars in the galaxy, suggesting a recent merging or acquisition event. The combination of integral-field measurements for the H alpha+[N II] emission lines from DensePak and the H beta and [O 111] emission from SAURON allow the construction of diagnostic diagrams that highlight the transition from star formation in the nuclear ring to excitation by high-velocity shocks or by a central AGN towards the center. DensePak measurements for the [S II] line ratio reveal very low gas densities in the nuclear ring, N(sub e) less than 100 per cubic centimeters, characteristic of massive H II regions. Comparison with MAPPINGS III models for starbursts with low gas densities show that the ring is of roughly solar metallicity. This suggests that the gas in the nuclear ring originated in a stellar system capable of substantially enriching the gas metallicity through sustained star formation. We propose that NGC 7742 cannibalised a smaller galaxy rich in metal-poor gas, and that star formation episodes in the ring have since increased the metallicity to its present value. The techniques explored here can be widely used to study similar systems, including composite (AGN+starburst) galaxies.

ASCA Observation of an "X-Ray Shadow" in the Galactic Plane

NASA Technical Reports Server (NTRS)

Park, Sangwook; Ebisawa, Ken

2001-01-01

The diffuse X-ray background (DXB) emission near the Galactic plane (l,b approximately 25.6 degrees, 0.78 degrees) has been observed with ASCA (Advanced Satellite for Cosmology and Astrophysics). The observed region is toward a Galactic molecular cloud which was recently reported to cast a deep X-ray shadow in the 0.5 - 2.0 keV band DXB. The selection of this particular region is intended to provide a constraint on the spatial distribution of the DXB emission along the line of sight: i.e., the molecular cloud is optically thick at <2 keV and so the bulk of the observed soft X-rays must originate in the foreground of the cloud, which is at approximately 3 kpc from the Sun. In the 0.8 - 9.0 keV band, the observed spectrum is primarily from multiple components of thermal plasmas. We here report a detection of soft X-ray (0.5 - 2 keV) emission from an approximately 10(exp 7) K thermal plasma. Comparisons with the ROSAT (Roentgen Satellite) data suggest that this soft X-ray emission is absorbed by N(sub H) = 1 - 3 x 10(exp 21) cm(exp -2), which implies a path-length through the soft X-ray emitting regions of approximately less than 1 kpc from the Sun.

Inventories and scenarios of nitrous oxide emissions

NASA Astrophysics Data System (ADS)

Davidson, Eric A.; Kanter, David

2014-10-01

Effective mitigation for N2O emissions, now the third most important anthropogenic greenhouse gas and the largest remaining anthropogenic source of stratospheric ozone depleting substances, requires understanding of the sources and how they may increase this century. Here we update estimates and their uncertainties for current anthropogenic and natural N2O emissions and for emissions scenarios to 2050. Although major uncertainties remain, ‘bottom-up’ inventories and ‘top-down’ atmospheric modeling yield estimates that are in broad agreement. Global natural N2O emissions are most likely between 10 and 12 Tg N2O-N yr-1. Net anthropogenic N2O emissions are now about 5.3 Tg N2O-N yr-1. Gross anthropogenic emissions by sector are 66% from agriculture, 15% from energy and transport sectors, 11% from biomass burning, and 8% from other sources. A decrease in natural emissions from tropical soils due to deforestation reduces gross anthropogenic emissions by about 14%. Business-as-usual emission scenarios project almost a doubling of anthropogenic N2O emissions by 2050. In contrast, concerted mitigation scenarios project an average decline of 22% relative to 2005, which would lead to a near stabilization of atmospheric concentration of N2O at about 350 ppb. The impact of growing demand for biofuels on future projections of N2O emissions is highly uncertain; N2O emissions from second and third generation biofuels could remain trivial or could become the most significant source to date. It will not be possible to completely eliminate anthropogenic N2O emissions from agriculture, but better matching of crop N needs and N supply offers significant opportunities for emission reductions.

Comparing two tetraalkylammonium ionic liquids. II. Phase transitions

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

Lima, Thamires A.; Paschoal, Vitor H.; Faria, Luiz F. O.

Phase transitions of the ionic liquids n-butyl-trimethylammonium bis(trifluoromethanesulfonyl)imide, [N{sub 1114}][NTf{sub 2}], and methyl-tributylammonium bis(trifluoromethanesulfonyl)imide, [N{sub 1444}][NTf{sub 2}], were investigated by differential scanning calorimetry (DSC), X-ray diffraction (XRD) measurements, and Raman spectroscopy. XRD and Raman spectra were obtained as a function of temperature at atmospheric pressure, and also under high pressure at room temperature using a diamond anvil cell (DAC). [N{sub 1444}][NTf{sub 2}] experiences glass transition at low temperature, whereas [N{sub 1114}][NTf{sub 2}] crystallizes or not depending on the cooling rate. Both the ionic liquids exhibit glass transition under high pressure. XRD and low-frequency Raman spectra provide a consistent physical picturemore » of structural ordering-disordering accompanying the thermal events of crystallization, glass transition, cold crystallization, pre-melting, and melting. Raman spectra in the high-frequency range of some specific cation and anion normal modes reveal conformational changes of the molecular structures along phase transitions.« less

Soil invertebrate fauna affect N2 O emissions from soil.

PubMed

Kuiper, Imke; de Deyn, Gerlinde B; Thakur, Madhav P; van Groenigen, Jan Willem

2013-09-01

Nitrous oxide (N2 O) emissions from soils contribute significantly to global warming. Mitigation of N2 O emissions is severely hampered by a lack of understanding of its main controls. Fluxes can only partly be predicted from soil abiotic factors and microbial analyses - a possible role for soil fauna has until now largely been overlooked. We studied the effect of six groups of soil invertebrate fauna and tested the hypothesis that all of them increase N2 O emissions, although to different extents. We conducted three microcosm experiments with sandy soil and hay residue. Faunal groups included in our experiments were as follows: fungal-feeding nematodes, mites, springtails, potworms, earthworms and isopods. In experiment I, involving all six faunal groups, N2 O emissions declined with earthworms and potworms from 78.4 (control) to 37.0 (earthworms) or 53.5 (potworms) mg N2 O-N m(-2) . In experiment II, with a higher soil-to-hay ratio and mites, springtails and potworms as faunal treatments, N2 O emissions increased with potworms from 51.9 (control) to 123.5 mg N2 O-N m(-2) . Experiment III studied the effect of potworm density; we found that higher densities of potworms accelerated the peak of the N2 O emissions by 5 days (P < 0.001), but the cumulative N2 O emissions remained unaffected. We propose that increased soil aeration by the soil fauna reduced N2 O emissions in experiment I, whereas in experiment II N2 O emissions were driven by increased nitrogen and carbon availability. In experiment III, higher densities of potworms accelerated nitrogen and carbon availability and N2 O emissions, but did not increase them. Overall, our data show that soil fauna can suppress, increase, delay or accelerate N2 O emissions from soil and should therefore be an integral part of future N2 O studies. © 2013 John Wiley & Sons Ltd.

A review of nitrous oxide mitigation by farm nitrogen management in temperate grassland-based agriculture.

PubMed

Li, Dejun; Watson, Catherine J; Yan, Ming Jia; Lalor, Stan; Rafique, Rashid; Hyde, Bernard; Lanigan, Gary; Richards, Karl G; Holden, Nicholas M; Humphreys, James

2013-10-15

Nitrous oxide (N2O) emission from grassland-based agriculture is an important source of atmospheric N2O. It is hence crucial to explore various solutions including farm nitrogen (N) management to mitigate N2O emissions without sacrificing farm profitability and food supply. This paper reviews major N management practices to lower N2O emission from grassland-based agriculture. Restricted grazing by reducing grazing time is an effective way to decrease N2O emissions from excreta patches. Balancing the protein-to-energy ratios in the diets of ruminants can also decrease N2O emissions from excreta patches. Among the managements of synthetic fertilizer N application, only adjusting fertilizer N rate and slow-released fertilizers are proven to be effective in lowering N2O emissions. Use of bedding materials may increase N2O emissions from animal houses. Manure storage as slurry, manipulating slurry pH to values lower than 6 and storage as solid manure under anaerobic conditions help to reduce N2O emissions during manure storage stage. For manure land application, N2O emissions can be mitigated by reducing manure N inputs to levels that satisfy grass needs. Use of nitrification inhibitors can substantially lower N2O emissions associated with applications of fertilizers and manures and from urine patches. N2O emissions from legume based grasslands are generally lower than fertilizer-based systems. In conclusion, effective measures should be taken at each step during N flow or combined options should be used in order to mitigate N2O emission at the farm level. Copyright © 2013 Elsevier Ltd. All rights reserved.

Oriented and ordered mesoporous ZrO{sub 2}/TiO{sub 2} fibers with well-organized linear and spring structure

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

Zhu, Luyi, E-mail: zhuly@sdu.edu.cn; Liu, Benxue; Qin, Weiwei, E-mail: jiuyuan.1001@163.com

Graphical abstract: The ultra-stable order mesoporous ZrO{sub 2}/TiO{sub 2} fibers with well-organized linear and spring structure and large surface area under higher temperatures were prepared by a simple EISA process. - Highlights: • The ZrO{sub 2}/TiO{sub 2} fibers were prepared by EISA process combined with steam heat-treatment. • The mesoporous ZrO{sub 2}/TiO{sub 2} fibers have well-organized linear and spring structure. • The fibers were composed of oval rod nanocrystals of ZrTiO{sub 4}. - Abstract: The ultra-stable order mesoporous ZrO{sub 2}/TiO{sub 2} fibers with well-organized linear and spring structure and large surface areas under higher temperatures were prepared by a (simplemore » evaporation-induced assembly) EISA process. The preparation, microstructures and formation processes were characterized by Fourier transformation infrared (FTIR), X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and N{sub 2} adsorption–absorption measurements. The fibers take on pinstripe configuration which is very orderly along or perpendicular to the axial direction of the fibers. The diameters of the pinstripe are in the region of 200–400 nm and arranges regularly, which are composed of oval rod nanocrystals of ZrTiO{sub 4}.« less

Effect of H2O on the NO emission characteristics of pulverized coal during oxy-fuel combustion.

PubMed

Lei, Ming; Sun, Cen; Zou, Chan; Mi, Hang; Wang, Chunbo

2018-04-01

The NO emission characteristics of Datong bituminous coal and Yangquan anthracite in O 2 /H 2 O/CO 2 atmospheres were investigated by using a fixed-bed reactor system, and the emission characteristics were compared with the experimental results from O 2 /N 2 and O 2 /CO 2 atmospheres, especially at low O 2 concentrations and high temperatures. The results showed that NO emissions of pulverized coal in O 2 /CO 2 environments were less than those in the O 2 /N 2 environments, regardless of the O 2 concentration and the furnace temperature. Adding H 2 O decreased the possibility of reactions between the reductive groups (NH) and the oxygen radical during devolatilization, which led to a decrease in NO emissions at 1000 °C. However, as the furnace temperature increased, "additional" nitrogen precursors (HCN and NH 3 ) generated by enhanced char-H 2 O gasification were quickly oxidized to generate a large amount of NO during char oxidation that exceeded the amount of NO reduced by NH during devolatilization. Thus, the NO emissions in O 2 /CO 2 /H 2 O atmosphere were higher than those in O 2 /CO 2 atmosphere at a low O 2 concentration. However, as the O 2 concentration increased, the NO emissions in O 2 /CO 2 /H 2 O atmosphere became lower than those in O 2 /CO 2 atmosphere because the effect of H 2 O gasification became weaker. The NO emissions of Yangquan anthracite (YQ) were higher than those of DT, but the changing trend of YQ was similar to that of DT.

Method and apparatus for generating coherent near 14 and near 16 micron radiation

DOEpatents

Krupke, William F.

1977-01-01

A method and apparatus for producing coherent radiation in CO.sub.2 vibrational-rotational transitions at wavelengths near 14 and 16 microns. This is accomplished by passing a mixture of N.sub.2 and Ar through a glow discharge producing a high vibrational temperature in the N.sub.2, passing the excited N.sub.2 through a nozzle bank creating a supersonic flow thereof, injecting the CO.sub.2 in the supersonic flow creating a population inversion in the CO.sub.2, and directing the saturating pulse of radiation near 10.6 or 9.6 microns into the excited CO.sub.2 creating a population inversion producing coherent radiation at 14 or 16 microns, respectively.

High-temperature fracture mechanism of low-Ca-doped silicon nitride

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

Tanaka, Isao; Igashira, Kenichiro; Okamoto, Taira

1995-03-01

High-purity Si{sub 3}N{sub 4} (with 2.5 wt% glassy SiO{sub 2}) doped with 0 to 450 at.ppm of Ca was prepared as a model system to investigate the effects of grain-boundary segregants on fracture phenomenology at 1,400 C. Subcritical crack-growth (SCG) resistance as well as creep resistance was degraded significantly by the presence of a small amount of Ca. The internal friction of the doped materials exhibited the superposition of a grain-boundary relaxation peak and a high-temperature background, and the apparent viscosity of the grain-boundary film was determined from the peak. Based on these experimental data, the fracture mechanism at 1,400more » C was divided into three regions: ``brittle``, SCG, and creep failure as a function of both external strain rate and Ca concentration, C{sub ca}. From the investigation of the C{sub Ca} dependence of the critical strain rate for the transition from ``brittle`` to SCG fractures, the SCG phenomenon is suggested to be triggered by small-scale, grain-boundary sliding. The C{sub Ca} dependence of ``steady-state`` creep rate was far from the theoretical dependence of diffusional creep via a solution-precipitation mechanism. The discrepancy was interpreted to be due to the presence of an impurity-insensitive creep component. This component may correspond to the lowest limit of the tensile creep rate in Si{sub 3}N{sub 4} polycrystalline materials containing intergranular glassy-SiO{sub 2} film.« less

Nitrogen and phosphorus addition impact soil N2O emission in a secondary tropical forest of South China

PubMed Central

Wang, Faming; Li, Jian; Wang, Xiaoli; Zhang, Wei; Zou, Bi; Neher, Deborah A.; Li, Zhian

2014-01-01

Nutrient availability greatly regulates ecosystem processes and functions of tropical forests. However, few studies have explored impacts of N addition (aN), P addition (aP) and N×P interaction on tropical forests N2O fluxes. We established an N and P addition experiment in a tropical forest to test whether: (1) N addition would increase N2O emission and nitrification, and (2) P addition would increase N2O emission and N transformations. Nitrogen and P addition had no effect on N mineralization and nitrification. Soil microbial biomass was increased following P addition in wet seasons. aN increased 39% N2O emission as compared to control (43.3 μgN2O-N m−2h−1). aP did not increase N2O emission. Overall, N2O emission was 60% greater for aNP relative to the control, but significant difference was observed only in wet seasons, when N2O emission was 78% greater for aNP relative to the control. Our results suggested that increasing N deposition will enhance soil N2O emission, and there would be N×P interaction on N2O emission in wet seasons. Given elevated N deposition in future, P addition in this tropical soil will stimulate soil microbial activities in wet seasons, which will further enhance soil N2O emission. PMID:25001013

Cryogenic expansion joint for large superconducting magnet structures

DOEpatents

Brown, Robert L.

1978-01-01

An expansion joint is provided that accommodates dimensional changes occurring during the cooldown and warm-up of large cryogenic devices such as superconducting magnet coils. Flattened tubes containing a refrigerant such as gaseous nitrogen (N.sub.2) are inserted into expansion spaces in the structure. The gaseous N.sub.2 is circulated under pressure and aids in the cooldown process while providing its primary function of accommodating differential thermal contraction and expansion in the structure. After lower temperatures are reached and the greater part of the contraction has occured, the N.sub.2 liquefies then solidifies to provide a completely rigid structure at the cryogenic operating temperatures of the device.

Impact of plastic mulching on nitrous oxide emissions in China's arid agricultural region under climate change conditions

NASA Astrophysics Data System (ADS)

Yu, Yongxiang; Tao, Hui; Jia, Hongtao; Zhao, Chengyi

2017-06-01

The denitrification-decomposition (DNDC) model is a useful tool for integrating the effects of agricultural practices and climate change on soil nitrous oxide (N2O) emissions from agricultural ecosystems. In this study, the DNDC model was evaluated against observations and used to simulate the effect of plastic mulching on soil N2O emissions and crop growth. The DNDC model performed well in simulating temporal variations in N2O emissions and plant growth during the observation period, although it slightly underestimated the cumulative N2O emissions, and was able to simulate the effects of plastic mulching on N2O emissions and crop yield. Both the observations and simulations demonstrated that the application of plastic film increased cumulative N2O emissions and cotton lint yield compared with the non-mulched treatment. The sensitivity test showed that the N2O emissions and lint yield were sensitive to changes in climate and management practices, and the application of plastic film made the N2O emissions and lint yield less sensitive to changes in temperature and irrigation. Although the simulations showed that the beneficial impacts of plastic mulching on N2O emissions were not gained under high fertilizer and irrigation scenarios, our simulations suggest that the application of plastic film effectively reduced soil N2O emissions while promoting yields under suitable fertilizer rates and irrigation. Compared with the baseline scenario, future climate change significantly increased N2O emissions by 15-17% without significantly influencing the lint yields in the non-mulched treatment; in the mulched treatment, climate change significantly promoted the lint yield by 5-6% and significantly reduced N2O emissions by 14% in the RCP4.5 and RCP8.5 scenarios. Overall, our results demonstrate that the application of plastic film is an efficient way to address increased N2O emissions and simultaneously enhance crop yield in the future.

Supersymmetric SO(10)-inspired leptogenesis and a new N{sub 2}-dominated scenario

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

Bari, Pasquale Di; Fiorentin, Michele Re, E-mail: pdb1d08@soton.ac.uk, E-mail: M.Re-Fiorentin@soton.ac.uk

2016-03-01

We study the supersymmetric extension of SO(10)-inspired thermal leptogenesis showing the constraints on neutrino parameters and on the reheat temperature T{sub RH} that derive from the condition of successful leptogenesis from next-to-lightest right handed (RH) neutrinos (N{sub 2}) decays and the more stringent ones when independence of the initial conditions (strong thermal leptogenesis) is superimposed. In the latter case, the increase of the lightest right-handed neutrino (N{sub 1}) decay parameters helps the wash-out of a pre-existing asymmetry and constraints relax compared to the non-supersymmetric case. We find significant changes especially in the case of large tanβ values (∼> 15). In particular,more » for normal ordering, the atmospheric mixing angle can now be also maximal. The lightest left-handed neutrino mass is still constrained within the range 010 ∼< m{sub 1}/meV ∼< 3 (corresponding to 075∼< ∑{sub i} m{sub i}/meV ∼< 12). Inverted ordering is still disfavoured, but an allowed region satisfying strong thermal leptogenesis opens up at large tanβ values. We also study in detail the lower bound on T{sub RH} finding T{sub RH}∼> 1 × 10{sup 10} GeV independently of the initial N{sub 2} abundance. Finally, we propose a new N{sub 2}-dominated scenario where the N{sub 1} mass is lower than the sphaleron freeze-out temperature. In this case there is no N{sub 1} wash-out and we find T{sub RH} ∼> 1× 10{sup 9} GeV . These results indicate that SO(10)-inspired thermal leptogenesis can be made compatible with the upper bound from the gravitino problem, an important result in light of the role often played by supersymmetry in the quest of a realistic model of fermion masses.« less

Evidence for involvement of gut-associated denitrifying bacteria in emission of nitrous oxide (N(2)O) by earthworms obtained from garden and forest soils.

PubMed

Matthies, C; Griesshammer, A; Schmittroth, M; Drake, H L

1999-08-01

Earthworms (Aporrectodea caliginosa, Lumbricus rubellus, and Octolasion lacteum) obtained from nitrous oxide (N(2)O)-emitting garden soils emitted 0.14 to 0.87 nmol of N(2)O h(-1) g (fresh weight)(-1) under in vivo conditions. L. rubellus obtained from N(2)O-emitting forest soil also emitted N(2)O, which confirmed previous observations (G. R. Karsten and H. L. Drake, Appl. Environ. Microbiol. 63:1878-1882, 1997). In contrast, commercially obtained Lumbricus terrestris did not emit N(2)O; however, such worms emitted N(2)O when they were fed (i.e., preincubated in) garden soils. A. caliginosa, L. rubellus, and O. lacteum substantially increased the rates of N(2)O emission of garden soil columns and microcosms. Extrapolation of the data to in situ conditions indicated that N(2)O emission by earthworms accounted for approximately 33% of the N(2)O emitted by garden soils. In vivo emission of N(2)O by earthworms obtained from both garden and forest soils was greatly stimulated when worms were moistened with sterile solutions of nitrate or nitrite; in contrast, ammonium did not stimulate in vivo emission of N(2)O. In the presence of nitrate, acetylene increased the N(2)O emission rates of earthworms; in contrast, in the presence of nitrite, acetylene had little or no effect on emission of N(2)O. In vivo emission of N(2)O decreased by 80% when earthworms were preincubated in soil supplemented with streptomycin and tetracycline. On a fresh weight basis, the rates of N(2)O emission of dissected earthworm gut sections were substantially higher than the rates of N(2)O emission of dissected worms lacking gut sections, indicating that N(2)O production occurred in the gut rather than on the worm surface. In contrast to living earthworms and gut sections that produced N(2)O under oxic conditions (i.e., in the presence of air), fresh casts (feces) from N(2)O-emitting earthworms produced N(2)O only under anoxic conditions. Collectively, these results indicate that gut-associated denitrifying bacteria are responsible for the in vivo emission of N(2)O by earthworms and contribute to the N(2)O that is emitted from certain terrestrial ecosystems.

HST/COS OBSERVATIONS OF GALACTIC HIGH-VELOCITY CLOUDS: FOUR ACTIVE GALACTIC NUCLEUS SIGHT LINES THROUGH COMPLEX C

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

Shull, J. Michael; Stevans, Matthew; Danforth, Charles

2011-10-01

We report ultraviolet spectra of Galactic high-velocity clouds (HVCs) in Complex C, taken by the Cosmic Origins Spectrograph (COS) on the Hubble Space Telescope (HST), together with new 21 cm spectra from the Green Bank Telescope. The wide spectral coverage and higher signal-to-noise ratio, compared to previous HST spectra, provide better velocity definition of the HVC absorption, additional ionization species (including high ions), and improved abundances in this halo gas. Complex C has a metallicity of 10%-30% solar and a wide range of ions, suggesting dynamical and thermal interactions with hot gas in the Galactic halo. Spectra in the COSmore » medium-resolution G130M (1133-1468 A) and G160M (1383-1796 A) gratings detect ultraviolet absorption lines from eight elements in low-ionization states (O I, N I, C II, S II, Si II, Al II, Fe II, P II) and three elements in intermediate- and high-ionization states (Si III, Si IV, C IV, N V). Our four active galactic nucleus sight lines toward Mrk 817, Mrk 290, Mrk 876, and PG 1259+593 have high-velocity H I and O VI column densities, log N{sub Hi}= 19.39-20.05 and log N{sub Ovi}= 13.58-14.10, with substantial amounts of kinematically associated photoionized gas. The high-ion abundance ratios are consistent with cooling interfaces between photoionized and collisionally ionized gas: N(C IV)/N(O VI) {approx} 0.3-0.5, N(Si IV)/N(O VI) {approx} 0.05-0.11, N(N V)/N(O VI) {approx} 0.07-0.13, and N(Si IV)/N(Si III) {approx}0.2.« less

Effects of soil dry-wet cycles and nitrogen fertilization on soil nitrous oxide emission: Simulation using the DNDC model

NASA Astrophysics Data System (ADS)

Hui, D.; Chen, H.; Deng, Q.; Wang, G.; Schadt, C. W.

2017-12-01

The major source of atmospheric nitrous oxide (N2O) is from croplands. A rapid pulse response of soil N2O emission to precipitation (PPT) is often reported, especially after a drought period. However, how precipitation pattern (i.e. frequency) and intensity, and nitrogen (N) fertilization would interactively influence soil N2O emission has not been well investigated. In this modeling study, we took advantage of a validated biogeochemical model (DNDC) in a cornfield and simulated soil N2O emission under manipulated precipitation treatments and three levels (Low, medium and high) of N application rate. The PPT treatments included precipitation pattern (from very frequent, to medium, and rare dry-wet cycles without changes in total annual precipitation) and intensity (from ambient, to -50%, +50%, and +100% ambient precipitation without changes in precipitation pattern). Results showed that both precipitation pattern and intensity, as well as nitrogen application rate had significant influences on the pulse responses and annual soil N2O emission. Very frequent dry-wet cycles tended to increase soil N2O emission while long drought-wet cycles had lower soil N2O emission, but the timing of N fertilization and precipitation also played an important role in the magnitude of pulse response and annual budget of N2O emission. As expected, soil N2O emission was higher under the high N application and lower under the low N application rate. Double precipitation (+100%) had the highest soil N2O emission, but showed no significant differences with +50% and ambient precipitation. The drought (-50%) treatment significantly reduced soil N2O emission. Annual soil N2O emission could be described as N2O=-6.7436+0.1098N+0.0049PPT, R2=0.86. Our results demonstrate that not only the intensity and pattern of precipitation greatly influence soil N2O emission, but also the timing of rainfall and N fertilization may play an important role in soil N2O pulse responses and annual N2O emission in cornfields. These modeling approaches inform our future work to deploy automated gas flux systems to validate and monitor these rapid N2O responses in the field.

Substantial nitrous oxide emissions from intertidal sediments and groundwater in anthropogenically-impacted West Falmouth Harbor, Massachusetts.

PubMed

Moseman-Valtierra, Serena; Kroeger, Kevin D; Crusius, John; Baldwin, Sandra; Green, Adrian; Brooks, T Wallace; Pugh, Emily

2015-01-01

Large N2O emissions were observed from intertidal sediments in a coastal estuary, West Falmouth Harbor, MA, USA. Average N2O emission rates from 41 chambers during summer 2008 were 10.7 mol N2O m(-2) h(-1)±4.43 μmol N2O m(-2) h(-1) (standard error). Emissions were highest from sediments within a known wastewater plume, where a maximum N2O emission rate was 155 μmol N2O m(-2) h(-1). Intertidal N2O fluxes were positively related to porewater ammonium concentrations at 10 and 25 cm depths. In groundwater from 7 shoreline wells, dissolved N2O ranged from 488% of saturation (56 nM N2O) to more than 13000% of saturation (1529 nM N2O) and was positively related to nitrate concentrations. Fresh and brackish porewater underlying 14 chambers was also supersaturated in N2O, ranging from 2980% to 13175% of saturation. These observations support a relationship between anthropogenic nutrient loading and N2O emissions in West Falmouth Harbor, with both groundwater sources and also local N2O production within nutrient-rich, intertidal sediments in the groundwater seepage face. N2O emissions from intertidal "hotspot" in this harbor, together with estimated surface water emissions, constituted 2.4% of the average overall rate of nitrogen export from the watershed to the estuary. This suggests that N2O emissions factors from coastal ecosystems may be underestimated. Since anthropogenic nutrient loading affects estuaries worldwide, quantification of N2O dynamics is warranted in other anthropogenically-impacted coastal ecosystems. Copyright © 2014 Elsevier Ltd. All rights reserved.

Substantial nitrous oxide emissions from intertidal sediments and groundwater in anthropogenically-impacted West Falmouth Harbor, Massachusetts

USGS Publications Warehouse

Moseman-Valtierra, Serena; Kroeger, Kevin D.; Crusius, John; Baldwin, Sandy; Green, Adrian; Brooks, Thomas W.; Pugh, E.

2015-01-01

Large N2O emissions were observed from intertidal sediments in a coastal estuary, West Falmouth Harbor, MA, USA. Average N2O emission rates from 41 chambers during summer 2008 were 10.7 mol N2O m(-2) h(-1)±4.43 μmol N2O m(-2) h(-1) (standard error). Emissions were highest from sediments within a known wastewater plume, where a maximum N2O emission rate was 155 μmol N2O m(-2) h(-1). Intertidal N2O fluxes were positively related to porewater ammonium concentrations at 10 and 25 cm depths. In groundwater from 7 shoreline wells, dissolved N2O ranged from 488% of saturation (56 nM N2O) to more than 13000% of saturation (1529 nM N2O) and was positively related to nitrate concentrations. Fresh and brackish porewater underlying 14 chambers was also supersaturated in N2O, ranging from 2980% to 13175% of saturation. These observations support a relationship between anthropogenic nutrient loading and N2O emissions in West Falmouth Harbor, with both groundwater sources and also local N2O production within nutrient-rich, intertidal sediments in the groundwater seepage face. N2O emissions from intertidal "hotspot" in this harbor, together with estimated surface water emissions, constituted 2.4% of the average overall rate of nitrogen export from the watershed to the estuary. This suggests that N2O emissions factors from coastal ecosystems may be underestimated. Since anthropogenic nutrient loading affects estuaries worldwide, quantification of N2O dynamics is warranted in other anthropogenically-impacted coastal ecosystems.

Synthesis, crystal structure and magnetic characterization of metal(II) coordination polymers based on 2-carboxyethylphosphonic acid and 1,10-phenanthroline (metal=Cu, Co, Cd)

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

Fernandez-Zapico, Eva; Montejo-Bernardo, Jose Manuel; D'Vries, Richard

2011-12-15

Three non-isostructural metal(II) coordination polymers (metal=copper, cobalt, cadmium) were synthesized under the same mild hydrothermal conditions (T=408 K) by mixture of the corresponding metal acetate with 2-carboxyethylphosphonic acid and 1,10-phenanthroline (1:1:1 M ratio) and their structures were determined by single-crystal X-ray diffraction. Cu{sub 2}(HO{sub 3}PCH{sub 2}CH{sub 2}COO){sub 2}(C{sub 12}H{sub 8}N{sub 2}){sub 2}(H{sub 2}O){sub 2} and Cd{sub 2}(HO{sub 3}PCH{sub 2}CH{sub 2}COO){sub 2}(C{sub 12}H{sub 8}N{sub 2}){sub 2} are triclinic (space group P-1) with a=7.908(5) A, b=10.373(5) A, c=11.515(5) A, {alpha}=111.683(5) Degree-Sign , {beta}=95.801(5) Degree-Sign , {gamma}=110.212(5) Degree-Sign (T=120 K), and a=8.162(5) A, b=9.500(5) A, c=11.148(5) A, {alpha}=102.623(5) Degree-Sign , {beta}=98.607(5) Degree-Sign ,more » {gamma}=113.004(5) Degree-Sign (T=293 K), respectively. In contrast, [Co{sub 2}(HO{sub 3}PCH{sub 2}CH{sub 2}COO){sub 2}(C{sub 12}H{sub 8}N{sub 2}){sub 2}({mu}-OH{sub 2})](H{sub 2}O) is orthorhombic (space group Pbcn) with a=21.1057(2) A, b=9.8231(1) A, c=15.4251(1) A (T=120 K). For these three compounds, structural features, including H-bond network and the {pi}-{pi} stacking interactions, and thermal stability are reported and discussed. None of the materials present a long-range magnetic order in the range of temperatures investigated from 300 K down to 1.8 K. - Graphical abstract: In same synthetic conditions, both the chemical and structural features of three transition metal(II) coordination polymers based on 2-carboxyethylphosphonate and 1-10 Prime -phenanthroline are influenced by the metal cation characteristics, leading to non-homologous materials with different properties, which show the high chemical versatility of this interesting system. Highlights: Black-Right-Pointing-Pointer Non-isostructural metal coordination polymers were synthesized under mild hydrothermal conditions. Black-Right-Pointing-Pointer Ligand's flexibility provides the opportunity to design compounds with tailored properties. Black-Right-Pointing-Pointer Structural changes in the secondary building units are induced by metal features.« less

Metal-free g-C{sub 3}N{sub 4} photocatalyst by sulfuric acid activation for selective aerobic oxidation of benzyl alcohol under visible light

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

Zhang, Ligang; University of Chinese Academy of Sciences, Beijing 100049; Liu, Di

2014-11-15

Highlights: • A novel visible-light-driven acid-modified g-C{sub 3}N{sub 4} was prepared. • The texture, electronic and surface property were tuned by acid modification. • Acid-modified g-C{sub 3}N{sub 4} shows much higher activity for photocatalytic activity. • Acid sites on the surface of g-C{sub 3}N{sub 4} favor efficient charge separation. - Abstract: In this work, modification of graphitic carbon nitride photocatalyst with acid was accomplished with a facile method through reflux in different acidic substances. The g-C{sub 3}N{sub 4}-based material was found to be a metal-free photocatalyst useful for the selective oxidation of benzyl alcohol with dioxygen as the oxidant undermore » visible light irradiation. Acid modification had a significant influence on the photocatalytic performance of g-C{sub 3}N{sub 4}. Among all acid tested, sulfuric acid-modified g-C{sub 3}N{sub 4} showed the highest catalytic activity and gave benzaldehyde in 23% yield for 4 h under visible light irradiation, which was about 2.5 times higher than that of g-C{sub 3}N{sub 4}. The acid modification effectively improved surface area, reduced structural size, enlarged band gap, enhanced surface chemical state, and facilitated photoinduced charge separation, contributing to the enhanced photocatalytic activity. It is hoped that our work can open promising prospects for the utilization of metal free g-C{sub 3}N{sub 4}-based semiconductor as visible-light photocatalyst for selective organic transformation.« less

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

Banerjee, Debasis; Borkowski, Lauren A.; Kim, Sun Jin

Two lithium-based metal-organic frameworks, Li{sub 2}(C{sub 14}H{sub 8}O{sub 4}) [Li{sub 2}(4,4'-BPDC) [1]; ULMOF-2, UL = ultralight; BPDC = biphenyldicarboxylate]; space group P2{sub 1}/c, a = 12.758(2) {angstrom}, b = 5.142(4) {angstrom}, c = 8.00(2) {angstrom}, {beta} = 97.23{sup o}, V = 520.6(14) {angstrom}{sup 3} and Li{sub 2}(C{sub 14}H{sub 8}O{sub 6}S) [Li{sub 2}(4,4'-SDB) [2]; ULMOF-3, UL = ultralight; SDB = sulfonyldibenzoate], space group P2{sub 1}/n, a = 5.5480(11) {angstrom}, b = 23.450(5) {angstrom}, c = 10.320(2) {angstrom}, {beta} = 96.47(3){sup o}, V = 1334.1(5) {angstrom}3, were synthesized. Compounds 1 and 2 were synthesized by solvothermal methods and were characterized using singlemore » crystal X-ray diffraction. Structure 1 consists of layers of two-dimensional antifluorite related LiO motif connected by BPDC linkers, whereas structure 2 is constructed by a combination of tetrameric lithium polyhedral clusters connected by the sulfonyldibenzoate linker. The frameworks are stable up to 575 and 500 C, respectively, under N{sub 2} atmosphere.« less

Investigation of the N2O emission strength in the U. S. Corn Belt

NASA Astrophysics Data System (ADS)

Fu, Congsheng; Lee, Xuhui; Griffis, Timothy J.; Dlugokencky, Edward J.; Andrews, Arlyn E.

2017-09-01

Nitrous oxide (N2O) has a high global warming potential and depletes stratospheric ozone. The U. S. Corn Belt plays an important role in the global anthropogenic N2O budget. To date, studies on local surface N2O emissions and the atmospheric N2O budget have commonly used Lagrangian models. In the present study, we used an Eulerian model - Weather Research and Forecasting Chemistry (WRF-Chem) model to investigate the relationships between N2O emissions in the Corn Belt and observed atmospheric N2O mixing ratios. We derived a simple equation to relate the emission strengths to atmospheric N2O mixing ratios, and used the derived equation and hourly atmospheric N2O measurements at the KCMP tall tower in Minnesota to constrain agricultural N2O emissions. The modeled spatial patterns of atmospheric N2O were evaluated against discrete observations at multiple tall towers in the NOAA flask network. After optimization of the surface flux, the model reproduced reasonably well the hourly N2O mixing ratios monitored at the KCMP tower. Agricultural N2O emissions in the EDGAR42 database needed to be scaled up by 19.0 to 28.1 fold to represent the true emissions in the Corn Belt for June 1-20, 2010 - a peak emission period. Optimized mean N2O emissions were 3.00-4.38, 1.52-2.08, 0.61-0.81 and 0.56-0.75 nmol m- 2 s- 1 for June 1-20, August 1-20, October 1-20 and December 1-20, 2010, respectively. The simulated spatial patterns of atmospheric N2O mixing ratios after optimization were in good agreement with the NOAA discrete observations during the strong emission peak in June. Such spatial patterns suggest that the underestimate of emissions using IPCC (Inter-governmental Panel on Climate Change) inventory methodology is not dependent on tower measurement location.

LUMINOUS INFRARED GALAXIES WITH THE SUBMILLIMETER ARRAY. IV. {sup 12}CO J = 6-5 OBSERVATIONS OF VV 114

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

Sliwa, Kazimierz; Wilson, Christine D.; Krips, Melanie

We present high-resolution (∼2.''5) observations of {sup 12}CO J = 6-5 toward the luminous infrared galaxy VV 114 using the Submillimeter Array. We detect {sup 12}CO J = 6-5 emission from the eastern nucleus of VV 114 but do not detect the western nucleus or the central region. We combine the new {sup 12}CO J = 6-5 observations with previously published or archival low-J CO observations, which include {sup 13}CO J = 1-0 Atacama Large Millimeter/submillimeter Array cycle 0 observations, to analyze the beam-averaged physical conditions of the molecular gas in the eastern nucleus. We use the radiative transfer codemore » RADEX and a Bayesian likelihood code to constrain the temperature (T{sub kin}), density (n{sub H{sub 2}}), and column density (N{sub {sup 1}{sup 2}CO}) of the molecular gas. We find that the most probable scenario for the eastern nucleus is a cold (T{sub kin} = 38 K), moderately dense (n{sub H{sub 2}} = 10{sup 2.89} cm{sup –3}) molecular gas component. We find that the most probable {sup 12}CO to {sup 13}CO abundance ratio ([{sup 12}CO]/[{sup 13}CO]) is 229, which is roughly three times higher than the Milky Way value. This high abundance ratio may explain the observed high {sup 12}CO/ {sup 13}CO line ratio (>25). The unusual {sup 13}CO J = 2-1/J = 1-0 line ratio of 0.6 is produced by a combination of moderate {sup 13}CO optical depths (τ = 0.4-1.1) and extremely subthermal excitation temperatures. We measure the CO-to-H{sub 2} conversion factor, α{sub CO}, to be 0.5{sup +0.6}{sub -0.3} M{sub ☉} (K km s{sup –1} pc{sup 2}){sup –1}, which agrees with the widely used factor for ultra luminous infrared galaxies of Downes and Solomon (α{sub CO} = 0.8 M{sub ☉} (K km s{sup –1} pc{sup 2}){sup –1})« less

Broad NE 8 lambda 774 emission from quasars in the HST-FOS snapshot survey (ABSNAP)

NASA Technical Reports Server (NTRS)

Hamann, Fred; Zuo, Lin; Tytler, David

1995-01-01

We discuss the strength and frequency of broad Ne VIII lambda 774 emission from quasars measured in the Hubble Space Telescope Faint Object Spectrograph (HST-FOS) snapshot survey (Absnap). Five sources in the survey have suitable redshifts (0.86 less than or equal to Z(sub em) less than or equal to 1.31), signal-to-noise ratios and no Lyman limit absorptions. Three of the five sources have a strong broad emission line near 774 A (rest), and the remaining two sources have a less securely measured line near this wavelength. We identify these lines with Ne VIII lambda 774 based on the measured wavelengths and theoretical estimates of various line fluxes (Hamann et al. 1995a). Secure Ne VIII detections occur in both radio-loud and radio-quiet sources. We tentatively conclude that broad Ne VIII lambda 774 emission is common in quasars, with typical strengths between approximately 25% and approximately 200% of O VI lambda 1034. These Ne VIII lambda 774 measurements imply that the broad emission line regions have a much hotter and more highly ionized component than previously recognized. They also suggest that quasar continua have substantial ionizing flux out to energies greater than 207 eV (greater than 15.2 ryd, lambda less than 60 A). Photoionization calculations using standard incident spectra indicate that the Ne VIII emission requires ionization parameters U greater than or = 5, total column densities N(sub H) greater than or = 10(sub 22)/sq cm and covering factors greater than or = 25%. The temperatures could be as high as approximately 10(exp 5) K. If the gas is instead collisionally ionized, strong Ne VIII would imply equilibrium temperatures in the range approximately 400,000 less than or approximately = T(sub e) less than or approximately = 10(exp 6) K. In either case, the highly ionized Ne VIII emission regions would appear as X-ray 'warm absorbers' if they lie along our line of sight to the X-ray continuum source.

Photocatalytic and photoelectrochemical performance of Ta{sub 3}N{sub 5} microcolumn films fabricated using facile reactive sputtering

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

Lin, Der-Hwa; Chang, Kao-Shuo, E-mail: kschang@mail.ncku.edu.tw; Promotion Center for Global Materials Research, National Cheng Kung University, No. 1 University Road, Tainan City 70101, Taiwan

2016-08-21

This paper presents the photocatalytic and photoelectrochemical (PEC) properties of Ta{sub 3}N{sub 5} microcolumn films. The highlights include (1) overcoming the fundamental barrier of standard reactive sputtering for fabricating microcolumns; (2) preventing unnecessary complexity from complicating facile sputtering; (3) an alternative but effective approach for fabricating Ta{sub 3}N{sub 5} without using caustic NH{sub 3} gases; (4) investigating morphology tuning for favorable photocatalysis and PEC reactions; and (5) elucidating the relationships of the structures, morphologies, and properties of Ta{sub 3}N{sub 5} microcolumns. High-resolution transmission electron microscopy and selective-area electron diffraction verified the polycrystallinity of Ta{sub 3}N{sub 5} microcolumns, of which themore » elemental compositions and stoichiometry were measured using electron-probe energy dispersive spectroscopy, Auger electron spectroscopy, and X-ray photoelectron spectroscopy. The corresponding band gap was determined to be approximately 2.1 eV. The sample exhibited a superior photodegradation capability; the photodegradation rate constant k was determined to be approximately 1.4 times higher than that of P25 under UV irradiation. A photocatalytic and PEC cycling test indicated the photodegradation reusability and photostability of the Ta{sub 3}N{sub 5} microcolumns. The incident photon-to-current efficiency performance reached 6%, suggesting that these microcolumns hold potential for application in PEC devices.« less

Thermal electron attachment to van der Waals molecules containing O/sub 2/

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

Huo, W.M.; Fessenden, R.W.; Bauschlicher C.W. Jr.

1984-12-15

Calculations on O/sub 2/xN/sub 2/ and O/sup -//sub 2/xN/sub 2/ have been carried out to explain the large enhancement in the attachment rate of thermal electrons found in van der Waals molecules containing O/sub 2/. Two geometries, T-shape and linear, are used. SCF wave functions are used to represent both the neutral molecule and the ion. The incoming electron is approximated by a plane wave. The width is determined using a shielded polarization potential. The effect of additional vibrational structures of the van der Waals molecule on the attachment process is investigated by studying the O/sub 2/--N/sub 2/ stretching modemore » using Lennard-Jones potentials. Symmetry breaking, which allows the molecule to attach a p wave electron, is shown to play a primary role. The lowering of resonance energy, due to a deeper Lennard-Jones potential of O/sup -//sub 2/xN/sub 2/ in comparison with O/sub 2/xN/sub 2/, furthers the enhancement. The calculated attachment rate is comparable to that determined by Shimamori and Fessenden, but differs from the recent values obtained by Toriumi and Hatano, who used a different set of reactions to interpret their data.« less

Initial decomposition mechanism for the energy release from electronically excited energetic materials: FOX-7 (1,1-diamino-2,2-dinitroethene, C{sub 2}H{sub 4}N{sub 4}O{sub 4})

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

Yuan, Bing; Yu, Zijun; Bernstein, Elliot R., E-mail: erb@lamar.Colostate.edu

Decomposition of the energetic material FOX-7 (1,1-diamino-2,2-dinitroethylene, C{sub 2}H{sub 4}N{sub 4}O{sub 4}) is investigated both theoretically and experimentally. The NO molecule is observed as an initial decomposition product subsequent to electronic excitation. The observed NO product is rotationally cold (<35 K) and vibrationally hot (2800 K). The initial decomposition mechanism is explored at the complete active space self-consistent field (CASSCF) level. Potential energy surface calculations at the CASSCF(12,8)/6-31G(d) level illustrate that conical intersections play an essential role in the decomposition mechanism. Electronically excited S{sub 2} FOX-7 can radiationlessly relax to lower electronic states through (S{sub 2}/S{sub 1}){sub CI} and (S{submore » 1}/S{sub 0}){sub CI} conical intersections and undergo a nitro-nitrite isomerization to generate NO product on the S{sub 0} state. The theoretically predicted mechanism is consistent with the experimental results. As FOX-7 decomposes on the ground electronic state, thus, the vibrational energy of the NO product from FOX-7 is high. The observed rotational energy distribution for NO is consistent with the final transition state structure on the S{sub 0} state. Ground state FOX-7 decomposition agrees with previous work: the nitro-nitrite isomerization has the lowest average energy barrier, the C–NH{sub 2} bond cleavage is unlikely under the given excitation conditions, and HONO formation on the ground state surface is energy accessible but not the main process.« less

Role of surface and subsurface processes in scaling N2O emissions along riverine networks

PubMed Central

Marzadri, Alessandra; Dee, Martha M.; Tonina, Daniele; Bellin, Alberto; Tank, Jennifer L.

2017-01-01

Riverine environments, such as streams and rivers, have been reported as sources of the potent greenhouse gas nitrous oxide (N2O) to the atmosphere mainly via microbially mediated denitrification. Our limited understanding of the relative roles of the near-surface streambed sediment (hyporheic zone), benthic, and water column zones in controlling N2O production precludes predictions of N2O emissions along riverine networks. Here, we analyze N2O emissions from streams and rivers worldwide of different sizes, morphology, land cover, biomes, and climatic conditions. We show that the primary source of N2O emissions varies with stream and river size and shifts from the hyporheic–benthic zone in headwater streams to the benthic–water column zone in rivers. This analysis reveals that N2O production is bounded between two N2O emission potentials: the upper N2O emission potential results from production within the benthic–hyporheic zone, and the lower N2O emission potential reflects the production within the benthic–water column zone. By understanding the scaling nature of N2O production along riverine networks, our framework facilitates predictions of riverine N2O emissions globally using widely accessible chemical and hydromorphological datasets and thus, quantifies the effect of human activity and natural processes on N2O production. PMID:28400514

Nitrous oxide emissions in the Shanghai river network: implications for the effects of urban sewage and IPCC methodology.

PubMed

Yu, Zhongjie; Deng, Huanguang; Wang, Dongqi; Ye, Mingwu; Tan, Yongjie; Li, Yangjie; Chen, Zhenlou; Xu, Shiyuan

2013-10-01

Global nitrogen (N) enrichment has resulted in increased nitrous oxide (N(2)O) emission that greatly contributes to climate change and stratospheric ozone destruction, but little is known about the N(2)O emissions from urban river networks receiving anthropogenic N inputs. We examined N(2)O saturation and emission in the Shanghai city river network, covering 6300 km(2), over 27 months. The overall mean saturation and emission from 87 locations was 770% and 1.91 mg N(2)O-N m(-2) d(-1), respectively. Nitrous oxide (N(2)O) saturation did not exhibit a clear seasonality, but the temporal pattern was co-regulated by both water temperature and N loadings. Rivers draining through urban and suburban areas receiving more sewage N inputs had higher N(2)O saturation and emission than those in rural areas. Regression analysis indicated that water ammonium (NH(4)(+)) and dissolved oxygen (DO) level had great control on N(2)O production and were better predictors of N(2)O emission in urban watershed. About 0.29 Gg N(2)O-N yr(-1) N(2)O was emitted from the Shanghai river network annually, which was about 131% of IPCC's prediction using default emission values. Given the rapid progress of global urbanization, more study efforts, particularly on nitrification and its N(2)O yielding, are needed to better quantify the role of urban rivers in global riverine N(2)O emission. © 2013 John Wiley & Sons Ltd.

Ellipsometric investigation of nitrogen doped diamond thin films grown in microwave CH{sub 4}/H{sub 2}/N{sub 2} plasma enhanced chemical vapor deposition

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

Ficek, Mateusz, E-mail: rbogdan@eti.pg.gda.pl; Institute for Materials Research; Sankaran, Kamatchi J.

2016-06-13

The influence of N{sub 2} concentration (1%–8%) in CH{sub 4}/H{sub 2}/N{sub 2} plasma on structure and optical properties of nitrogen doped diamond (NDD) films was investigated. Thickness, roughness, and optical properties of the NDD films in the VIS–NIR range were investigated on the silicon substrates using spectroscopic ellipsometry. The samples exhibited relatively high refractive index (2.6 ± 0.25 at 550 nm) and extinction coefficient (0.05 ± 0.02 at 550 nm) with a transmittance of 60%. The optical investigation was supported by the molecular and atomic data delivered by Raman studies, bright field transmission electron microscopy imaging, and X-ray photoelectron spectroscopy diagnostics. Those results revealed that whilemore » the films grown in CH{sub 4}/H{sub 2} plasma contained micron-sized diamond grains, the films grown using CH{sub 4}/H{sub 2}/(4%)N{sub 2} plasma exhibited ultranano-sized diamond grains along with n-diamond and i-carbon clusters, which were surrounded by amorphous carbon grain boundaries.« less

Influence of difference quantity La-doped TiO{sub 2} photoanodes on the performance of dye-sensitized solar cells: A strategy for choosing an appropriate doping quantity

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

Zhang, Zige; Li, Guoxiang; Cui, Zijian

2016-05-15

Facilitated by TiO{sub 2} particles adsorbing lanthanide ions in hydrosol, La-doped TiO{sub 2} was produced by a hydrothermal method. The structure, optical and photoluminescence properties of down-converting photoelectrode with the La{sup 3+} were characterized by X-ray (XRD), Scanning electron microscopy (SEM), Energy dispersive X-ray detector (EDX) and N{sub 2} adsorption-desorption isotherms measurement. The photoelectric conversion efficiency of dye-sensitized solar cells (DSSCs) fabricated with 0.05 g-La/TiO{sub 2} reached 7.02%, which gave an efficiency improved by 10.36% compared with that of cells fabricated from pure TiO{sub 2}. The improvement in efficiency was ascribed to more dyes adsorbed on the surface of TiO{submore » 2}. - Graphical abstract: (a) J–V curves of La-doped photoelectrodes with different La(NO{sub 3}){sub 3}·6H{sub 2}O amounts; (b) the curves of efficiency changing with the amount of La(NO{sub 3}){sub 3}·6H{sub 2}O. The photoelectric conversion efficiency of dye-sensitized solar cells (DSSCs) fabricated with 0.05 g-La/TiO{sub 2} reached 7.02%, which gave an efficiency improved by 10.36% compared with that of cells fabricated from pure TiO{sub 2}.« less

Cadmium-sulfide crystallites in Cd-. gamma. -glutamyl peptide complexes from Lycopersicon and Daucus

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

Reese, R.N.; Winge, D.R.

1989-04-01

Hydroponically-grown tomato plants (Lycopersicon esculentum P. Mill. cv stone) and suspension-cultured carrot cells (Daucus carota L.) exposed to 100 {mu}M cadmium salts produced metal-{gamma}-glutamyl peptide complexes containing acid labile sulfur. The properties of the complexes resemble the Cd-{gamma}-glutamyl complexes from Schizosaccharomyces pombe and Candida glabrata, known to contain a CdS crystallite core. The crystallite core is stabilized by a coating of peptides of the general structure ({gamma}-Glu-Cys){sub n}-Gly. The Cd-peptide complexes contain predominantly peptides of n{sub 2}, n{sub 3}, n{sub 4} and n{sub 3}desGly. Zn-peptide complexes were also isolated from carrot cultures grown in MS medium supplemented with 2 mMmore » Zn and cysteine. Results of preliminary characterization of these complexes are consistent with the presence of a colloidal particle similar to that of the Cd-complexes.« less

Synthesis and characterization of mangenese(III) porphyrin supported on imidazole modified chloromethylated MIL-101(Cr): A heterogeneous and reusable catalyst for oxidation of hydrocarbons with sodium periodate

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

Zadehahmadi, Farnaz; Tangestaninejad, Shahram, E-mail: stanges@sci.ui.ac.ir; Moghadam, Majid, E-mail: moghadamm@sci.ui.ac.ir

2014-10-15

In the present work, chloromethylated MIL-101(Cr) modified with imidazole, Im-MIL-101, was applied as a support for immobilizing of tetraphenylporphyrinatomangenese(III) chloride. The imidazole-bound MIL-101, Im-MIL-101, not only used as support for immobilization of manganese porphyrin but also applied as a heterogeneous axial base. The Mn(TPP)Cl@Im-MIL-101 catalyst was characterized by UV–vis, FT-IR, X-ray diffraction (XRD), N{sub 2} adsorption, field emission scanning electron microscopy (FE-SEM), energy dispersive X-ray (EDX), elemental analysis and inductively coupled plasma (ICP) methods. The catalytic activity of this new catalytic system was investigated in the alkene epoxidation and alkane hydroxylation using NaIO{sub 4} as an oxidant in CH{sub 3}CN/H{submore » 2}O at room temperature. This heterogeneous catalyst is highly efficient, stable and reusable in the oxidation of hydrocarbons. - Highlights: • MIL-101 was modified by covalent post synthetic modification. • Mn(TPP)Cl was anchored to imidazole modified MIL-101 by covalent attachment. • A heterogeneous catalyst was prepared. • The catalyst was used for epoxidation of alkenes and hydroxylation of alkanes. • The catalyst was reusable.« less

Effects of Biochar Addition on CO2 and N2O Emissions following Fertilizer Application to a Cultivated Grassland Soil

PubMed Central

Chen, Jingjing; Kim, Hyunjin; Yoo, Gayoung

2015-01-01

Carbon (C) sequestration potential of biochar should be considered together with emission of greenhouse gases when applied to soils. In this study, we investigated CO2 and N2O emissions following the application of rice husk biochars to cultivated grassland soils and related gas emissions tos oil C and nitrogen (N) dynamics. Treatments included biochar addition (CHAR, NO CHAR) and amendment (COMPOST, UREA, NO FERT). The biochar application rate was 0.3% by weight. The temporal pattern of CO2 emissions differed according to biochar addition and amendments. CO2 emissions from the COMPOST soils were significantly higher than those from the UREA and NO FERT soils and less CO2 emission was observed when biochar and compost were applied together during the summer. Overall N2O emission was significantly influenced by the interaction between biochar and amendments. In UREA soil, biochar addition increased N2O emission by 49% compared to the control, while in the COMPOST and NO FERT soils, biochar did not have an effect on N2O emission. Two possible mechanisms were proposed to explain the higher N2O emissions upon biochar addition to UREA soil than other soils. Labile C in the biochar may have stimulated microbial N mineralization in the C-limited soil used in our study, resulting in an increase in N2O emission. Biochar may also have provided the soil with the ability to retain mineral N, leading to increased N2O emission. The overall results imply that biochar addition can increase C sequestration when applied together with compost, and might stimulate N2O emission when applied to soil amended with urea. PMID:26020941

Surface Nitrification: A Major Uncertainty in Marine N2O Emissions

NASA Technical Reports Server (NTRS)

Zamora, Lauren M.; Oschlies, Andreas

2014-01-01

The ocean is responsible for up to a third of total global nitrous oxide (N2O) emissions, but uncertainties in emission rates of this potent greenhouse gas are high (approaching 100%). Here we use a marine biogeochemical model to assess six major uncertainties in estimates of N2O production, thereby providing guidance in how future studies may most effectively reduce uncertainties in current and future marine N2O emissions. Potential surface N2O production from nitrification causes the largest uncertainty in N2O emissions (estimated up to approximately 1.6 Tg N/yr (sup -1) or 48% of modeled values), followed by the unknown oxygen concentration at which N2O production switches to N2O consumption (0.8 Tg N/yr (sup -1)or 24% of modeled values). Other uncertainties are minor, cumulatively changing regional emissions by less than 15%. If production of N2O by surface nitrification could be ruled out in future studies, uncertainties in marine N2O emissions would be halved.

THE ALFALFA H I ABSORPTION PILOT SURVEY: A WIDE-AREA BLIND DAMPED Ly{alpha} SYSTEM SURVEY OF THE LOCAL UNIVERSE

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

Darling, Jeremy; Macdonald, Erin P.; Haynes, Martha P.

2011-11-20

We present the results of a pilot survey for neutral hydrogen (H I) 21 cm absorption in the Arecibo Legacy Fast Arecibo L-Band Feed Array (ALFALFA) Survey. This project is a wide-area 'blind' search for H I absorption in the local universe, spanning -650 km s{sup -1} < cz < 17, 500 km s{sup -1} and covering 517.0 deg{sup 2} (7% of the full ALFALFA survey). The survey is sensitive to H I absorption lines stronger than 7.7 mJy (8983 radio sources) and is 90% complete for lines stronger than 11.0 mJy (7296 sources). The total redshift interval sensitive tomore » all damped Ly{alpha} (DLA) systems (N{sub H{sub i}}{>=}2 Multiplication-Sign 10{sup 20} cm{sup -2}) is {Delta}z = 7.0 (129 objects, assuming T{sub s} = 100 K and covering fraction unity); for super-DLAs (N{sub H{sub i}}{>=}2 Multiplication-Sign 10{sup 21} cm{sup -2}) it is {Delta}z = 128.2 (2353 objects). We re-detect the intrinsic H I absorption line in UGC 6081 but detect no intervening absorption line systems. We compute a 95% confidence upper limit on the column density frequency distribution function f(N{sub H{sub i}},X) spanning four orders of magnitude in column density, 10{sup 19} (T{sub s} /100 K) (1/f) cm{sup -2}

Aliased tidal errors in TOPEX/POSEIDON sea surface height data

NASA Technical Reports Server (NTRS)

Schlax, Michael G.; Chelton, Dudley B.

1994-01-01

Alias periods and wavelengths for the M(sub 2, S(sub 2), N(sub 2), K(sub 1), O(sub 1), and P(sub 1) tidal constituents are calculated for TOPEX/POSEIDON. Alias wavelenghts calculated in previous studies are shown to be in error, and a correct method is presented. With the exception of the K(sub 1) constituent, all of these tidal aliases for TOPEX/POSEIDON have periods shorter than 90 days and are likely to be confounded with long-period sea surface height signals associated with real ocean processes. In particular, the correspondence between the periods and wavelengths of the M(sub 2) alias and annual baroclinic Rossby waves that plagued Geosat sea surface height data is avoided. The potential for aliasing residual tidal errors in smoothed estimates of sea surface height is calculated for the six tidal constituents. The potential for aliasing the lunar tidal constituents M(sub 2), N(sub 2) and O(sub 1) fluctuates with latitude and is different for estimates made at the crossovers of ascending and descending ground tracks than for estimates at points midway between crossovers. The potential for aliasing the solar tidal constituents S(sub 2), K(sub 1) and P(sub 1) varies smoothly with latitude. S(sub 2) is strongly aliased for latitudes within 50 degress of the equator, while K(sub 1) and P(sub 1) are only weakly aliased in that range. A weighted least squares method for estimating and removing residual tidal errors from TOPEX/POSEIDON sea surface height data is presented. A clear understanding of the nature of aliased tidal error in TOPEX/POSEIDON data aids the unambiguous identification of real propagating sea surface height signals. Unequivocal evidence of annual period, westward propagating waves in the North Atlantic is presented.

Nitrous oxide emission related to ammonia-oxidizing bacteria and mitigation options from N fertilization in a tropical soil

NASA Astrophysics Data System (ADS)

Soares, Johnny R.; Cassman, Noriko A.; Kielak, Anna M.; Pijl, Agata; Carmo, Janaína B.; Lourenço, Kesia S.; Laanbroek, Hendrikus J.; Cantarella, Heitor; Kuramae, Eiko E.

2016-07-01

Nitrous oxide (N2O) from nitrogen fertilizers applied to sugarcane has high environmental impact on ethanol production. This study aimed to determine the main microbial processes responsible for the N2O emissions from soil fertilized with different N sources, to identify options to mitigate N2O emissions, and to determine the impacts of the N sources on the soil microbiome. In a field experiment, nitrogen was applied as calcium nitrate, urea, urea with dicyandiamide or 3,4 dimethylpyrazone phosphate nitrification inhibitors (NIs), and urea coated with polymer and sulfur (PSCU). Urea caused the highest N2O emissions (1.7% of N applied) and PSCU did not reduce cumulative N2O emissions compared to urea. NIs reduced N2O emissions (95%) compared to urea and had emissions comparable to those of the control (no N). Similarly, calcium nitrate resulted in very low N2O emissions. Interestingly, N2O emissions were significantly correlated only with bacterial amoA, but not with denitrification gene (nirK, nirS, nosZ) abundances, suggesting that ammonia-oxidizing bacteria, via the nitrification pathway, were the main contributors to N2O emissions. Moreover, the treatments had little effect on microbial composition or diversity. We suggest nitrate-based fertilizers or the addition of NIs in NH4+-N based fertilizers as viable options for reducing N2O emissions in tropical soils and lessening the environmental impact of biofuel produced from sugarcane.

Nitrous oxide emission related to ammonia-oxidizing bacteria and mitigation options from N fertilization in a tropical soil

PubMed Central

Soares, Johnny R.; Cassman, Noriko A.; Kielak, Anna M.; Pijl, Agata; Carmo, Janaína B.; Lourenço, Kesia S.; Laanbroek, Hendrikus J.; Cantarella, Heitor; Kuramae, Eiko E.

2016-01-01

Nitrous oxide (N2O) from nitrogen fertilizers applied to sugarcane has high environmental impact on ethanol production. This study aimed to determine the main microbial processes responsible for the N2O emissions from soil fertilized with different N sources, to identify options to mitigate N2O emissions, and to determine the impacts of the N sources on the soil microbiome. In a field experiment, nitrogen was applied as calcium nitrate, urea, urea with dicyandiamide or 3,4 dimethylpyrazone phosphate nitrification inhibitors (NIs), and urea coated with polymer and sulfur (PSCU). Urea caused the highest N2O emissions (1.7% of N applied) and PSCU did not reduce cumulative N2O emissions compared to urea. NIs reduced N2O emissions (95%) compared to urea and had emissions comparable to those of the control (no N). Similarly, calcium nitrate resulted in very low N2O emissions. Interestingly, N2O emissions were significantly correlated only with bacterial amoA, but not with denitrification gene (nirK, nirS, nosZ) abundances, suggesting that ammonia-oxidizing bacteria, via the nitrification pathway, were the main contributors to N2O emissions. Moreover, the treatments had little effect on microbial composition or diversity. We suggest nitrate-based fertilizers or the addition of NIs in NH4+-N based fertilizers as viable options for reducing N2O emissions in tropical soils and lessening the environmental impact of biofuel produced from sugarcane. PMID:27460335

Nitrous oxide emission related to ammonia-oxidizing bacteria and mitigation options from N fertilization in a tropical soil.

PubMed

Soares, Johnny R; Cassman, Noriko A; Kielak, Anna M; Pijl, Agata; Carmo, Janaína B; Lourenço, Kesia S; Laanbroek, Hendrikus J; Cantarella, Heitor; Kuramae, Eiko E

2016-07-27

Nitrous oxide (N2O) from nitrogen fertilizers applied to sugarcane has high environmental impact on ethanol production. This study aimed to determine the main microbial processes responsible for the N2O emissions from soil fertilized with different N sources, to identify options to mitigate N2O emissions, and to determine the impacts of the N sources on the soil microbiome. In a field experiment, nitrogen was applied as calcium nitrate, urea, urea with dicyandiamide or 3,4 dimethylpyrazone phosphate nitrification inhibitors (NIs), and urea coated with polymer and sulfur (PSCU). Urea caused the highest N2O emissions (1.7% of N applied) and PSCU did not reduce cumulative N2O emissions compared to urea. NIs reduced N2O emissions (95%) compared to urea and had emissions comparable to those of the control (no N). Similarly, calcium nitrate resulted in very low N2O emissions. Interestingly, N2O emissions were significantly correlated only with bacterial amoA, but not with denitrification gene (nirK, nirS, nosZ) abundances, suggesting that ammonia-oxidizing bacteria, via the nitrification pathway, were the main contributors to N2O emissions. Moreover, the treatments had little effect on microbial composition or diversity. We suggest nitrate-based fertilizers or the addition of NIs in NH4(+)-N based fertilizers as viable options for reducing N2O emissions in tropical soils and lessening the environmental impact of biofuel produced from sugarcane.

Nitrous oxide emissions in Chinese vegetable systems: A meta-analysis.

PubMed

Wang, Xiaozhong; Zou, Chunqin; Gao, Xiaopeng; Guan, Xilin; Zhang, Wushuai; Zhang, Yueqiang; Shi, Xiaojun; Chen, Xinping

2018-08-01

China accounts for more than half of the world's vegetable production, and identifying the contribution of vegetable production to nitrous oxide (N 2 O) emissions in China is therefore important. We performed a meta-analysis that included 153 field measurements of N 2 O emissions from 21 field studies in China. Our goal was to quantify N 2 O emissions and fertilizer nitrogen (N) based-emission factors (EFs) in Chinese vegetable systems and to clarify the effects of rates and types of N fertilizer in both open-field and greenhouse systems. The results indicated that the intensive vegetable systems in China had an average N 2 O emission of 3.91 kg N 2 O-N ha -1 and an EF of 0.69%. Although the EF was lower than the IPCC default value of 1.0%, the average N 2 O emission was generally greater than in other cropping systems due to greater input of N fertilizers. The EFs were similar in greenhouse vs. open-field systems but N 2 O emissions were about 1.4 times greater in greenhouses. The EFs were not affected by N rate, but N 2 O emissions for both open-field and greenhouse systems increased with N rate. The total and fertilizer-induced N 2 O emissions, as well as EFs, were unaffected by the type of fertilizers in greenhouse system under same N rates. In addition to providing basic information about N 2 O emissions from Chinese vegetable systems, the results suggest that N 2 O emissions could be reduced without reducing yields by treating vegetable systems in China with a combination of synthetic N fertilizer and manure at optimized economic rates. Copyright © 2018 Elsevier Ltd. All rights reserved.

N2O emission characteristics and its affecting factors in rain-fed potato fields in Wuchuan County, China

NASA Astrophysics Data System (ADS)

Wang, Liwei; Wang, Cheng; Pan, Zhihua; Xu, Hui; Gao, Lin; Zhao, Peiyi; Dong, Zhiqiang; Zhang, Jingting; Cui, Guohui; Wang, Sen; Han, Guolin; Zhao, hui

2017-05-01

Representing an important greenhouse gas, nitrous oxide (N2O) emission from cultivated land is a hot topic in current climate change research. This study examined the influences of nitrogen fertilisation, temperature and soil moisture on the ammonia monooxygenase subunit A ( amoA) gene copy numbers and N2O emission characteristics. The experimental observation of N2O fluxes was based on the static chamber-gas chromatographic method. The ammonia-oxidising bacteria (AOB) and ammonia-oxidising archaea (AOA) gene copy numbers in different periods were measured by real-time polymerase chain reaction (PCR). The results indicated that rain-fed potato field was a N2O source, and the average annual N2O emission was approximately 0.46 ± 0.06 kgN2O-N/ha/year. N2O emissions increased significantly with increase in fertilisation, temperatures below 19.6 °C and soil volumetric water content under 15%. Crop rotation appreciably decreases N2O emissions by 34.4 to 52.4% compared to continuous cropping in rain-fed potato fields. The significant correlation between N2O fluxes and AOB copy numbers implied that N2O emissions were primarily controlled by AOB in rain-fed potato fields. The research has important theoretical and practical value for understanding N2O emissions from rain-fed dry farmland fields.

N2O emission characteristics and its affecting factors in rain-fed potato fields in Wuchuan County, China.

PubMed

Wang, Liwei; Wang, Cheng; Pan, Zhihua; Xu, Hui; Gao, Lin; Zhao, Peiyi; Dong, Zhiqiang; Zhang, Jingting; Cui, Guohui; Wang, Sen; Han, Guolin; Zhao, Hui

2017-05-01

Representing an important greenhouse gas, nitrous oxide (N 2 O) emission from cultivated land is a hot topic in current climate change research. This study examined the influences of nitrogen fertilisation, temperature and soil moisture on the ammonia monooxygenase subunit A (amoA) gene copy numbers and N 2 O emission characteristics. The experimental observation of N 2 O fluxes was based on the static chamber-gas chromatographic method. The ammonia-oxidising bacteria (AOB) and ammonia-oxidising archaea (AOA) gene copy numbers in different periods were measured by real-time polymerase chain reaction (PCR). The results indicated that rain-fed potato field was a N 2 O source, and the average annual N 2 O emission was approximately 0.46 ± 0.06 kgN 2 O-N/ha/year. N 2 O emissions increased significantly with increase in fertilisation, temperatures below 19.6 °C and soil volumetric water content under 15%. Crop rotation appreciably decreases N 2 O emissions by 34.4 to 52.4% compared to continuous cropping in rain-fed potato fields. The significant correlation between N 2 O fluxes and AOB copy numbers implied that N 2 O emissions were primarily controlled by AOB in rain-fed potato fields. The research has important theoretical and practical value for understanding N 2 O emissions from rain-fed dry farmland fields.

A high surface area Zr(IV)-based metal–organic framework showing stepwise gas adsorption and selective dye uptake

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

Lv, Xiu-Liang; Tong, Minman; Huang, Hongliang

2015-03-15

Exploitation of new metal–organic framework (MOF) materials with high surface areas has been attracting great attention in related research communities due to their broad potential applications. In this work, a new Zr(IV)-based MOF, [Zr{sub 6}O{sub 4}(OH){sub 4}(eddb){sub 6}] (BUT-30, H{sub 2}eddb=4,4′-(ethyne-1,2-diyl)dibenzoic acid) has been solvothermally synthesized, characterized, and explored for gases and dyes adsorptions. Single-crystal X-ray diffraction analysis demonstrates a three-dimensional cubic framework structure of this MOF, in which each Zr{sub 6}O{sub 4}(OH){sub 4} building unit is linked by 12 linear eddb ligands. BUT-30 has been found stable up to 400 °C and has a Brunauer–Emmett–Teller (BET) surface area asmore » high as 3940.6 m{sup 2} g{sup −1} (based on the N{sub 2} adsorption at 77 K) and total pore volume of 1.55 cm{sup 3} g{sup −1}. It is more interesting that this MOF exhibits stepwise adsorption behaviors for Ar, N{sub 2}, and CO{sub 2} at low temperatures, and selective uptakes towards different ionic dyes. - Graphical abstract: A new Zr(IV)-based MOF with high surface area has been synthesized and structurally characterized, which shows stepwise gas adsorption at low temperature and selective dye uptake from solution. - Highlights: • A new Zr-based MOF was synthesized and structurally characterized. • This MOF shows a higher surface area compared with its analogous UiO-67 and 68. • This MOF shows a rare stepwise adsorption towards light gases at low temperature. • This MOF performs selective uptakes towards cationic dyes over anionic ones. • Using triple-bond spacer is confirmed feasible in enhancing MOF surface areas.« less

Microwave-assisted rapid synthesis of birnessite-type MnO{sub 2} nanoparticles for high performance supercapacitor applications

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

Zhang, Xiong; Miao, Wang; Li, Chen

Highlights: • Birnessite-type MnO{sub 2} nanoparticles were prepared by the microwave-assisted reflux. • The microwave reaction duration was only 5 min. • A specific capacitance of 329 F g{sup −1} was obtained for birnessite-type MnO{sub 2}. - Abstract: Birnessite-type MnO{sub 2} nanoparticles have been successfully synthesized by the microwave-assisted reflux as short as 5 min. The microstructure and morphology of the products were characterized by X-ray diffraction, N{sub 2} adsorption–desorption isotherms, scanning electron microscopy, transmission electron microscopy. The electrochemical properties of the as-prepared MnO{sub 2} as an electrode material for supercapacitor were investigated by cyclic voltammetry and galvanostatic charge-discharge measurementsmore » in 1 M Na{sub 2}SO{sub 4} electrolyte, and a high specific capacitance of 329 F g{sup −1} was achieved at a current density of 0.2 A g{sup −1}. The specific capacitance retention was 92% after 1000 cycles at 2 A g{sup −1}, suggesting that it is a promising electrode material for supercapacitors.« less

The spin relaxation of nitrogen donors in 6H SiC crystals as studied by the electron spin echo method

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

Savchenko, D., E-mail: dariyasavchenko@gmail.com; National Technical University of Ukraine “Kyiv Polytechnic Institute,” Kyiv 03056; Shanina, B.

2016-04-07

We present the detailed study of the spin kinetics of the nitrogen (N) donor electrons in 6H SiC wafers grown by the Lely method and by the sublimation “sandwich method” (SSM) with a donor concentration of about 10{sup 17 }cm{sup −3} at T = 10–40 K. The donor electrons of the N donors substituting quasi-cubic “k1” and “k2” sites (N{sub k1,k2}) in both types of the samples revealed the similar temperature dependence of the spin-lattice relaxation rate (T{sub 1}{sup −1}), which was described by the direct one-phonon and two-phonon processes induced by the acoustic phonons proportional to T and to T{sup 9}, respectively. Themore » character of the temperature dependence of the T{sub 1}{sup −1} for the donor electrons of N substituting hexagonal (“h”) site (N{sub h}) in both types of 6H SiC samples indicates that the donor electrons relax through the fast-relaxing centers by means of the cross-relaxation process. The observed enhancement of the phase memory relaxation rate (T{sub m}{sup −1}) with the temperature increase for the N{sub h} donors in both types of the samples, as well as for the N{sub k1,k2} donors in Lely grown 6H SiC, was explained by the growth of the free electron concentration with the temperature increase and their exchange scattering at the N donor centers. The observed significant shortening of the phase memory relaxation time T{sub m} for the N{sub k1,k2} donors in the SSM grown sample with the temperature lowering is caused by hopping motion of the electrons between the occupied and unoccupied states of the N donors at N{sub h} and N{sub k1,k2} sites. The impact of the N donor pairs, triads, distant donor pairs formed in n-type 6H SiC wafers on the spin relaxation times was discussed.« less

Advanced Thomson scattering system for high-flux linear plasma generator

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

Meiden, H. J. van der; Lof, A. R.; Berg, M. A. van den

2012-12-15

An advanced Thomson scattering system has been built for a linear plasma generator for plasma surface interaction studies. The Thomson scattering system is based on a Nd:YAG laser operating at the second harmonic and a detection branch featuring a high etendue (f /3) transmission grating spectrometer equipped with an intensified charged coupled device camera. The system is able to measure electron density (n{sub e}) and temperature (T{sub e}) profiles close to the output of the plasma source and, at a distance of 1.25 m, just in front of a target. The detection system enables to measure 50 spatial channels ofmore » about 2 mm each, along a laser chord of 95 mm. By summing a total of 30 laser pulses (0.6 J, 10 Hz), an observational error of 3% in n{sub e} and 6% in T{sub e} (at n{sub e}= 9.4 Multiplication-Sign 10{sup 18} m{sup -3}) can be obtained. Single pulse Thomson scattering measurements can be performed with the same accuracy for n{sub e} > 2.8 Multiplication-Sign 10{sup 20} m{sup -3}. The minimum measurable density and temperature are n{sub e} < 1 Multiplication-Sign 10{sup 17} m{sup -3} and T{sub e} < 0.07 eV, respectively. In addition, using the Rayleigh peak, superimposed on the Thomson scattered spectrum, the neutral density (n{sub 0}) of the plasma can be measured with an accuracy of 25% (at n{sub 0}= 1 Multiplication-Sign 10{sup 20} m{sup -3}). In this report, the performance of the Thomson scattering system will be shown along with unprecedented accurate Thomson-Rayleigh scattering measurements on a low-temperature argon plasma expansion into a low-pressure background.« less

Emissions of N2O and NO from fertilized fields: Summary of available measurement data

NASA Astrophysics Data System (ADS)

Bouwman, A. F.; Boumans, L. J. M.; Batjes, N. H.

2002-12-01

Information from 846 N2O emission measurements in agricultural fields and 99 measurements for NO emissions was summarized to assess the influence of various factors regulating emissions from mineral soils. The data indicate that there is a strong increase of both N2O and NO emissions accompanying N application rates, and soils with high organic-C content show higher emissions than less fertile soils. A fine soil texture, restricted drainage, and neutral to slightly acidic conditions favor N2O emission, while (though not significant) a good soil drainage, coarse texture, and neutral soil reaction favor NO emission. Fertilizer type and crop type are important factors for N2O but not for NO, while the fertilizer application mode has a significant influence on NO only. Regarding the measurements, longer measurement periods yield more of the fertilization effect on N2O and NO emissions, and intensive measurements (≥1 per day) yield lower emissions than less intensive measurements (2-3 per week). The available data can be used to develop simple models based on the major regulating factors which describe the spatial variability of emissions of N2O and NO with less uncertainty than emission factor approaches based on country N inputs, as currently used in national emission inventories.

Investigating the role of hydrogen in silicon deposition using an energy-resolved mass spectrometer and a Langmuir probe in an Ar/H{sub 2} radio frequency magnetron discharge

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

Mensah, S. L.; Naseem, Hameed H.; Abu-Safe, Husam

2012-07-15

The plasma parameters and ion energy distributions (IED) of the dominant species in an Ar-H{sub 2} discharge are investigated with an energy resolved mass spectrometer and a Langmuir probe. The plasmas are generated in a conventional magnetron chamber powered at 150 W, 13.56 MHz at hydrogen flow rates ranging from 0 to 25 sccm with a fixed argon gas flow rate of 15 sccm. Various H{sub n}{sup +}, SiH{sub n}{sup +}, SiH{sub n} fragments (with n = 1, 2, 3) together with Ar{sup +} and ArH{sup +} species are detected in the discharge. The most important species for the filmmore » deposition is SiH{sub n} (with n = 0, 1, 2). H fragments affect the hydrogen content in the material. The flux of Ar{sup +} decreases and the flux of ArH{sup +} increases when the hydrogen flow rate is increased; however, both fluxes saturate at hydrogen flow rates above 15 sccm. Electron density, n{sub e}, electron energy, T{sub e}, and ion density, n{sub i}, are estimated from the Langmuir probe data. T{sub e} is below 1.2 eV at hydrogen flow rates below 8 sccm, and about 2 eV at flow rates above 8 sccm. n{sub e} and n{sub i} decrease with increased hydrogen flow but the ratio of n{sub i} to n{sub e} increases. The formation of H{sup +} ions with energies above 36 eV and electrons with energies greater than 2 eV contributes to the decrease in hydrogen content at hydrogen flow rates above 8 sccm. Analysis of the IEDs indicates an inter-dependence of the species and their contribution to the thin film growth and properties.« less

The impact of nitrification inhibitor DMPP on N2O, NO and N2 emissions at different soil moisture conditions in grassland soil

NASA Astrophysics Data System (ADS)

Wu, D.; Cardenas, L. M.; Sanz, S. C.; Brueggemann, N.; Loick, N.; Liu, S.; Bol, R.

2016-12-01

Emissions of gaseous forms of nitrogen from soil, such as nitrous oxide (N2O) and nitric oxide (NO), have shown great impact on global warming and atmospheric chemistry. Although in soil both nitrification and denitrification could cause N2O and NO emissions, most recent studies demonstrated that denitrification is the dominant process responsible for the increase of atmospheric N2O, while nitrification produces most of NO. The use of nitrification inhibitors (NI) has repeatedly been shown to lower both N2O and NO emissions from agricultural soils; nevertheless, the efficiency of the mitigation effect varies greatly. It is generally assumed that nitrification inhibitors have no direct effect on denitrification. However, the indirect impact, due to the reduced substrate delivery (NO3-) to microsites where denitrification occurs, may have significant effects on denitrification product stoichiometry that may significantly lower soil born N2O emissions. In the present study, soil incubation experiments were carried out in a fully automated continuous-flow incubation system under a He/O2 atmosphere. Ammonium sulfate was applied with and without NI (DMPP) to a UK grassland soil under three different soil moisture conditions (50% WFPS, 65% WFPS, 80% WFPS). With every treatment glucose was applied to supply enough carbon for denitrification. We examined the effect of DMPP on NO, N2O and N2 emissions at different soil moisture conditions which favor nitrification, a mixture of both nitrification and denitrification, or denitrification, respectively. Generally cumulative NO emissions were about 17% of cumulative N2O emissions, while N2 emissions were only detected at high soil moisture condition (80% WFPS). Higher soil moisture increased both N2O and NO emissions. DMPP application increased N2 emissions at soil moisture condition favoring denitrification. Although the application of DMPP significantly mitigated both N2O and NO emissions in all DMPP treatments, the efficiency of the mitigation effect varied with different soil moisture conditions. Overall, DMPP application mitigated about 40- 60% N2O emissions and 50-70% NO emissions during the 44-day incubation period.

Plasma-enhanced atomic layer deposition of titanium oxynitrides films: A comparative spectroscopic and electrical study

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

Sowińska, Małgorzata, E-mail: malgorzata.sowinska@b-tu.de; Henkel, Karsten; Schmeißer, Dieter

2016-01-15

The process parameters' impact of the plasma-enhanced atomic layer deposition (PE-ALD) method on the oxygen to nitrogen (O/N) ratio in titanium oxynitride (TiO{sub x}N{sub y}) films was studied. Titanium(IV)isopropoxide in combination with NH{sub 3} plasma and tetrakis(dimethylamino)titanium by applying N{sub 2} plasma processes were investigated. Samples were characterized by the in situ spectroscopic ellipsometry, x-ray photoelectron spectroscopy, and electrical characterization (current–voltage: I-V and capacitance–voltage: C-V) methods. The O/N ratio in the TiO{sub x}N{sub y} films is found to be very sensitive for their electric properties such as conductivity, dielectric breakdown, and permittivity. Our results indicate that these PE-ALD film propertiesmore » can be tuned, via the O/N ratio, by the selection of the process parameters and precursor/coreactant combination.« less

Carbon dioxide, methane, and nitrous oxide emissions from a rice-wheat rotation as affected by crop residue incorporation and temperature

NASA Astrophysics Data System (ADS)

Zou, Jianwen; Huang, Yao; Zong, Lianggang; Zheng, Xunhua; Wang, Yuesi

2004-10-01

Field measurements were made from June 2001 to May 2002 to evaluate the effect of crop residue application and temperature on CO2, CH4, and N2O emissions within an entire rice-wheat rotation season. Rapeseed cake and wheat straw were incorporated into the soil at a rate of 2.25 t hm-2 when the rice crop was transplanted in June 2001. Compared with the control, the incorporation of rapeseed cake enhanced the emissions of CO2, CH4, and N2O in the rice-growing season by 12.3%, 252.3%, and 17.5%, respectively, while no further effect was held on the emissions of CO2 and N2O in the following wheatgrowing season. The incorporation of wheat straw enhanced the emissions of CO2 and CH4 by 7.1% and 249.6%, respectively, but reduced the N2O emission by 18.8% in the rice-growing season. Significant reductions of 17.8% for the CO2 and of 12.9% for the N2O emission were observed in the following wheatgrowing season. A positive correlation existed between the emissions of N2O and CO2 ( R 2 = 0.445, n = 73, p < 0.001) from the rice-growing season when N2O was emitted. A trade-off relationship between the emissions of CH4 and N2O was found in the rice-growing season. The CH4 emission was significantly correlated with the CO2 emission for the period from rice transplantation to field drainage, but not for the entire rice-growing season. In addition, air temperature was found to regulate the CO2 emissions from the non-waterlogged period over the entire rice-wheat rotation season and the N2O emissions from the nonwaterlogged period of the rice-growing season, which can be quantitatively described by an exponential function. The temperature coefficient ( Q 10) was then evaluated to be 2.3±0.2 for the CO2 emission and 3.9±0.4 for the N2O emission, respectively.

Phases of unstable conifolds

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

Narayan, K.

2007-03-15

We explore the phase structure induced by closed string tachyon condensation of toric nonsupersymmetric conifold-like singularities described by an integral charge matrix Q=(n{sub 1}n{sub 2}-n{sub 3}-n{sub 4}), n{sub i}>0, iQ{sub i}{ne}0, initiated by Narayan [J. High Energy Phys. 03 (2006) 036]. Using gauged linear sigma model renormalization group flows and toric geometry techniques, we see a cascadelike phase structure containing decays to lower order conifold-like singularities, including, in particular, the supersymmetric conifold and the Y{sup pq} spaces. This structure is consistent with the Type II GSO projection obtained previously for these singularities. Transitions between the various phases of these geometriesmore » include flips and flops.« less

Modeling global annual N2O and NO emissions from fertilized fields

NASA Astrophysics Data System (ADS)

Bouwman, A. F.; Boumans, L. J. M.; Batjes, N. H.

2002-12-01

Information from 846 N2O emission measurements in agricultural fields and 99 measurements for NO emissions was used to describe the influence of various factors regulating emissions from mineral soils in models for calculating global N2O and NO emissions. Only those factors having a significant influence on N2O and NO emissions were included in the models. For N2O these were (1) environmental factors (climate, soil organic C content, soil texture, drainage and soil pH); (2) management-related factors (N application rate per fertilizer type, type of crop, with major differences between grass, legumes and other annual crops); and (3) factors related to the measurements (length of measurement period and frequency of measurements). The most important controls on NO emission include the N application rate per fertilizer type, soil organic-C content and soil drainage. Calculated global annual N2O-N and NO-N emissions from fertilized agricultural fields amount to 2.8 and 1.6 Mtonne, respectively. The global mean fertilizer-induced emissions for N2O and NO amount to 0.9% and 0.7%, respectively, of the N applied. These overall results account for the spatial variability of the main N2O and NO emission controls on the landscape scale.

Inhibition experiments on nitrous oxide emission from paddy soils

NASA Astrophysics Data System (ADS)

Xu, Xingkai; Boeckx, Pascal; Zhou, Likai; Van Cleemput, Oswald

2002-08-01

Rice fields using nitrogen-based fertilizers play an important role in the global N2O budget. However, our knowledge is still limited with regard to the mechanisms affecting the N2O emission and to the measures that can reduce the emission. This paper reports a study of N2O emission from paddy soils. The effects of urea, hydroquinone (HQ, a urease inhibitor), and dicyandiamide (DCD, a nitrification inhibitor) have been studied in pot experiments with and without rice plants and with and without addition of wheat straw. With no wheat straw amendment, all treatments with inhibitors, especially with HQ + DCD, had a much smaller N2O emission during the rice growing period than the urea treatment, whereas a substantially increased N2O emission was observed from a rice-free soil with inhibitors. The N2O emission from the rice-planted soil was exponentially positive correlated with the NO3--N concentration in the rice aboveground biomass. By comparing the total N2O emission from the rice-free soil and from the rice-planted soil, we found that urea application alone might induce an apparent plant-mediated N2O emission, being 0.39 +/- 0.08% of the applied urea N. Wheat straw incorporated into the flooded surface layer soil could increase the plant-mediated N2O emission significantly. However, application of HQ + DCD could reduce this emission (0.27 +/- 0.08% of the applied urea N, compared with 0.89 +/- 0.18% in the urea treatment). It also reduced the N2O emission from the rice-free soil and from the rice-planted soil. Stepwise regression analysis indicates that denitrification in the flooded surface layer soil was the main source of N2O emission from this wetland rice cultivation, particularly when wheat straw was added. A significantly nonlinear negative relation was found between the N2O emission and the CH4 emission when no wheat straw was added, but it was hard to quantify this trade-off relation when wheat straw was incorporated into the flooded surface layer soil.

Importance of aggregation and small ice crystals in cirrus clouds, based on observations and an ice particle growth model

NASA Technical Reports Server (NTRS)

Mitchell, David L.; Chai, Steven K.; Dong, Yayi; Arnott, W. Patrick; Hallett, John

1993-01-01

The 1 November 1986 FIRE I case study was used to test an ice particle growth model which predicts bimodal size spectra in cirrus clouds. The model was developed from an analytically based model which predicts the height evolution of monomodal ice particle size spectra from the measured ice water content (IWC). Size spectra from the monomodal model are represented by a gamma distribution, N(D) = N(sub o)D(exp nu)exp(-lambda D), where D = ice particle maximum dimension. The slope parameter, lambda, and the parameter N(sub o) are predicted from the IWC through the growth processes of vapor diffusion and aggregation. The model formulation is analytical, computationally efficient, and well suited for incorporation into larger models. The monomodal model has been validated against two other cirrus cloud case studies. From the monomodal size spectra, the size distributions which determine concentrations of ice particles less than about 150 mu m are predicted.

Ionothermal synthesis and structural transformation targeted by ion exchange in metal-1,3,5-benzenetricarboxylate compounds

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

Xu, Qing-Qing; State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002; Liu, Bing

Ionothermal reactions of 1,3,5-benzenetricarboxylate acid (H{sub 3}BTC) and Ni(NO{sub 3}){sub 2}, Co(NO{sub 3}){sub 2} and Cu(NO{sub 3}){sub 2} gave two discrete 32-membered ring-like allomers, [M{sub 2}(HBTC){sub 2}(NH{sub 2}CONH{sub 2}){sub 2}(H{sub 2}O){sub 4}]·3H{sub 2}O (M=Ni(1), Co(2)) and one layered [Cu{sub 2}(BTC)Cl(H{sub 2}O){sub 4}] (3). The weak interactions in 1 can be deconstructed to some degree in ion exchange by exploring the factors of divalent and trivalent metal species, metal concentration and soaking time, which are demonstrated by PXRD and N{sub 2} absorption. Cu{sup 2+} has the highest N{sub 2} adsorbance when soaking with 1, and 1 can keep structure stable whenmore » Cu{sup 2+} below 0.16 mol L{sup −1} and the soaking time within 24d. As Cu{sup 2+} beyond 0.16 mol L{sup −1} and the soaking time beyond 24d, the structure of compound 1 starts to transform with the crystal morphology from clear pale green to opaque blue. Ionothermal reactions of compound 1 with different Cu{sup 2+} amounts obtained Ni{sup 2+}-Cu{sup 2+} hetero complexes, whose PXRD patterns are similar to that of 3 and EDS indicates Cu{sup 2+}% increases with Cu{sup 2+} additions and close to 100% as Cu{sup 2+} being 1.6 mmol. It suggests that 3 is a controlled product and Cu{sup 2+} can transform discrete compound 1 into 2D compound 3. - Graphical abstract: Three compounds were synthesized through ionothermal reactions. The weak interactions in compound 1 can be deconstructed by ion exchange and discrete compound 1 can be transformed into layered compound 3. - Highlights: • Two discrete ring-like and one layered compounds were ionothermally synthesized. • Metal species, metal concentration and soaking time deconstruct the H-bondings in 1. • 1 can be transformed to 3 through ionothermal reaction, otherwise forbidden.« less

Effects of temperature on nitrous oxide (N2O) emission from intensive aquaculture system.

PubMed

Paudel, Shukra Raj; Choi, Ohkyung; Khanal, Samir Kumar; Chandran, Kartik; Kim, Sungpyo; Lee, Jae Woo

2015-06-15

This study examines the effects of temperature on nitrous oxide (N2O) emissions in a bench-scale intensive aquaculture system rearing Koi fish. The water temperature varied from 15 to 24 °C at interval of 3 °C. Both volumetric and specific rate for nitrification and denitrification declined as the temperature decreased. The concentrations of ammonia and nitrite, however, were lower than the inhibitory level for Koi fish regardless of temperature. The effects of temperature on N2O emissions were significant, with the emission rate and emission factor increasing from 1.11 to 1.82 mg N2O-N/d and 0.49 to 0.94 mg N2O-N/kg fish as the temperature decreased from 24 to 15 °C. A global map of N2O emission from aquaculture was established by using the N2O emission factor depending on temperature. This study demonstrates that N2O emission from aquaculture is strongly dependent on regional water temperatures as well as on fish production. Copyright © 2015 Elsevier B.V. All rights reserved.

Decreased N2O reduction by low soil pH causes high N2O emissions in a riparian ecosystem.

PubMed

Van den Heuvel, R N; Bakker, S E; Jetten, M S M; Hefting, M M

2011-05-01

Quantification of harmful nitrous oxide (N(2)O) emissions from soils is essential for mitigation measures. An important N(2)O producing and reducing process in soils is denitrification, which shows deceased rates at low pH. No clear relationship between N(2)O emissions and soil pH has yet been established because also the relative contribution of N(2)O as the denitrification end product decreases with pH. Our aim was to show the net effect of soil pH on N(2)O production and emission. Therefore, experiments were designed to investigate the effects of pH on NO(3)(-) reduction, N(2)O production and reduction and N(2) production in incubations with pH values set between 4 and 7. Furthermore, field measurements of soil pH and N(2)O emissions were carried out. In incubations, NO(3)(-) reduction and N(2) production rates increased with pH and net N(2)O production rate was highest at pH 5. N(2)O reduction to N(2) was halted until NO(3)(-) was depleted at low pH values, resulting in a built up of N(2)O. As a consequence, N(2)O:N(2) production ratio decreased exponentially with pH. N(2)O reduction appeared therefore more important than N(2)O production in explaining net N(2)O production rates. In the field, a negative exponential relationship for soil pH against N(2)O emissions was observed. Soil pH could therefore be used as a predictive tool for average N(2)O emissions in the studied ecosystem. The occurrence of low pH spots may explain N(2)O emission hotspot occurrence. Future studies should focus on the mechanism behind small scale soil pH variability and the effect of manipulating the pH of soils. © 2011 Blackwell Publishing Ltd.

Four dimensional magnetic resonance imaging with retrospective k-space reordering: A feasibility study

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

Liu, Yilin; Yin, Fang-Fang; Cai, Jing, E-mail: jing.cai@duke.edu

Purpose: Current four dimensional magnetic resonance imaging (4D-MRI) techniques lack sufficient temporal/spatial resolution and consistent tumor contrast. To overcome these limitations, this study presents the development and initial evaluation of a new strategy for 4D-MRI which is based on retrospective k-space reordering. Methods: We simulated a k-space reordered 4D-MRI on a 4D digital extended cardiac-torso (XCAT) human phantom. A 2D echo planar imaging MRI sequence [frame rate (F) = 0.448 Hz; image resolution (R) = 256 × 256; number of k-space segments (N{sub KS}) = 4] with sequential image acquisition mode was assumed for the simulation. Image quality of themore » simulated “4D-MRI” acquired from the XCAT phantom was qualitatively evaluated, and tumor motion trajectories were compared to input signals. In particular, mean absolute amplitude differences (D) and cross correlation coefficients (CC) were calculated. Furthermore, to evaluate the data sufficient condition for the new 4D-MRI technique, a comprehensive simulation study was performed using 30 cancer patients’ respiratory profiles to study the relationships between data completeness (C{sub p}) and a number of impacting factors: the number of repeated scans (N{sub R}), number of slices (N{sub S}), number of respiratory phase bins (N{sub P}), N{sub KS}, F, R, and initial respiratory phase at image acquisition (P{sub 0}). As a proof-of-concept, we implemented the proposed k-space reordering 4D-MRI technique on a T2-weighted fast spin echo MR sequence and tested it on a healthy volunteer. Results: The simulated 4D-MRI acquired from the XCAT phantom matched closely to the original XCAT images. Tumor motion trajectories measured from the simulated 4D-MRI matched well with input signals (D = 0.83 and 0.83 mm, and CC = 0.998 and 0.992 in superior–inferior and anterior–posterior directions, respectively). The relationship between C{sub p} and N{sub R} was found best represented by an exponential function (C{sub P}=100(1−e{sup −0.18N{sub R}}), when N{sub S} = 30, N{sub P} = 6). At a C{sub P} value of 95%, the relative error in tumor volume was 0.66%, indicating that N{sub R} at a C{sub P} value of 95% (N{sub R,95%}) is sufficient. It was found that N{sub R,95%} is approximately linearly proportional to N{sub P} (r = 0.99), and nearly independent of all other factors. The 4D-MRI images of the healthy volunteer clearly demonstrated respiratory motion in the diaphragm region with minimal motion induced noise or aliasing. Conclusions: It is feasible to generate respiratory correlated 4D-MRI by retrospectively reordering k-space based on respiratory phase. This new technology may lead to the next generation 4D-MRI with high spatiotemporal resolution and optimal tumor contrast, holding great promises to improve the motion management in radiotherapy of mobile cancers.« less

Effects of soil temperature, flooding, and organic matter addition on N2O emissions from a soil of Hongze Lake wetland, China.

PubMed

Lu, Yan; Xu, Hongwen

2014-01-01

The objectives of this study were to test the effects of soil temperature, flooding, and raw organic matter input on N2O emissions in a soil sampled at Hongze Lake wetland, Jiangsu Province, China. The treatments studied were-peat soil (I), peat soil under flooding (II), peat soil plus raw organic matter (III), and peat soil under flooding plus organic matter. These four treatments were incubated at 20°C and 35°C. The result showed that temperature increase could enhance N2O emissions rate and cumulative emissions significantly; moreover, the flooded soil with external organic matter inputs showed the lowest cumulative rise in N2O emissions due to temperature increment. Flooding might inhibit soil N2O emissions, and the inhibition was more pronounced after organic matter addition to the original soil. Conversely, organic matter input explained lower cumulative N2O emissions under flooding. Our results suggest that complex interactions between flooding and other environmental factors might appear in soil N2O emissions. Further studies are needed to understand potential synergies or antagonisms between environmental factors that control N2O emissions in wetland soils.

Nanocomposite thin films for high temperature optical gas sensing of hydrogen

DOEpatents

Ohodnicki, Jr., Paul R.; Brown, Thomas D.

2013-04-02

The disclosure relates to a plasmon resonance-based method for H.sub.2 sensing in a gas stream at temperatures greater than about 500.degree. C. utilizing a hydrogen sensing material. The hydrogen sensing material is comprised of gold nanoparticles having an average nanoparticle diameter of less than about 100 nanometers dispersed in an inert matrix having a bandgap greater than or equal to 5 eV, and an oxygen ion conductivity less than approximately 10.sup.-7 S/cm at a temperature of 700.degree. C. Exemplary inert matrix materials include SiO.sub.2, Al.sub.2O.sub.3, and Si.sub.3N.sub.4 as well as modifications to modify the effective refractive indices through combinations and/or doping of such materials. At high temperatures, blue shift of the plasmon resonance optical absorption peak indicates the presence of H.sub.2. The method disclosed offers significant advantage over active and reducible matrix materials typically utilized, such as yttria-stabilized zirconia (YSZ) or TiO.sub.2.

Near interface traps in SiO{sub 2}/4H-SiC metal-oxide-semiconductor field effect transistors monitored by temperature dependent gate current transient measurements

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

Fiorenza, Patrick; La Magna, Antonino; Vivona, Marilena

This letter reports on the impact of gate oxide trapping states on the conduction mechanisms in SiO{sub 2}/4H-SiC metal-oxide-semiconductor field effect transistors (MOSFETs). The phenomena were studied by gate current transient measurements, performed on n-channel MOSFETs operated in “gate-controlled-diode” configuration. The measurements revealed an anomalous non-steady conduction under negative bias (V{sub G} > |20 V|) through the SiO{sub 2}/4H-SiC interface. The phenomenon was explained by the coexistence of a electron variable range hopping and a hole Fowler-Nordheim (FN) tunnelling. A semi-empirical modified FN model with a time-depended electric field is used to estimate the near interface traps in the gate oxide (N{sub trap} ∼ 2 × 10{supmore » 11} cm{sup −2}).« less

Hydroxylamine diffusion can enhance N₂O emissions in nitrifying biofilms: a modeling study.

PubMed

Sabba, Fabrizio; Picioreanu, Cristian; Pérez, Julio; Nerenberg, Robert

2015-02-03

Wastewater treatment plants can be significant sources of nitrous oxide (N2O), a potent greenhouse gas. However, little is known about N2O emissions from biofilm processes. We adapted an existing suspended-growth mathematical model to explore N2O emissions from nitrifying biofilms. The model included N2O formation by ammonia-oxidizing bacteria (AOB) via the hydroxylamine and the nitrifier denitrification pathways. Our model suggested that N2O emissions from nitrifying biofilms could be significantly greater than from suspended growth systems under similar conditions. The main cause was the formation and diffusion of hydroxylamine, an AOB nitrification intermediate, from the aerobic to the anoxic regions of the biofilm. In the anoxic regions, hydroxylamine oxidation by AOB provided reducing equivalents used solely for nitrite reduction to N2O, since there was no competition with oxygen. For a continuous system, very high and very low dissolved oxygen (DO) concentrations resulted in lower emissions, while intermediate values led to higher emissions. Higher bulk ammonia concentrations and greater biofilm thicknesses increased emissions. The model effectively predicted N2O emissions from an actual pilot-scale granular sludge reactor for sidestream nitritation, but significantly underestimated the emissions when the NH2OH diffusion coefficient was assumed to be minimal. This numerical study suggests an unexpected and important role of hydroxylamine in N2O emission in biofilms.

Nitrous oxide emissions are enhanced in a warmer and wetter world

NASA Astrophysics Data System (ADS)

Griffis, Timothy J.; Chen, Zichong; Baker, John M.; Wood, Jeffrey D.; Millet, Dylan B.; Lee, Xuhui; Venterea, Rodney T.; Turner, Peter A.

2017-11-01

Nitrous oxide (N2O) has a global warming potential that is 300 times that of carbon dioxide on a 100-y timescale, and is of major importance for stratospheric ozone depletion. The climate sensitivity of N2O emissions is poorly known, which makes it difficult to project how changing fertilizer use and climate will impact radiative forcing and the ozone layer. Analysis of 6 y of hourly N2O mixing ratios from a very tall tower within the US Corn Belt—one of the most intensive agricultural regions of the world—combined with inverse modeling, shows large interannual variability in N2O emissions (316 Gg N2O-Nṡy‑1 to 585 Gg N2O-Nṡy‑1). This implies that the regional emission factor is highly sensitive to climate. In the warmest year and spring (2012) of the observational period, the emission factor was 7.5%, nearly double that of previous reports. Indirect emissions associated with runoff and leaching dominated the interannual variability of total emissions. Under current trends in climate and anthropogenic N use, we project a strong positive feedback to warmer and wetter conditions and unabated growth of regional N2O emissions that will exceed 600 Gg N2O-Nṡy‑1, on average, by 2050. This increasing emission trend in the US Corn Belt may represent a harbinger of intensifying N2O emissions from other agricultural regions. Such feedbacks will pose a major challenge to the Paris Agreement, which requires large N2O emission mitigation efforts to achieve its goals.

Preparation of high nitrogen compound and materials therefrom

DOEpatents

Huynh, My Hang V [Los Alamos, NM; Hiskey, Michael A [Los Alamos, NM

2006-10-10

The high-nitrogen compound of the formula ##STR00001## was prepared. Pyrolysis of the compound yields carbon nitrides C.sub.2N.sub.3 and C.sub.3N.sub.5. The carbon nitrides vary in their density, texture, and morphology.

Characteristics of greenhouse gas emission in three full-scale wastewater treatment processes.

PubMed

Yan, Xu; Li, Lin; Liu, Junxin

2014-02-01

Three full-scale wastewater treatment processes, Orbal oxidation ditch, anoxic/anaerobic/aerobic (reversed A2O) and anaerobic/anoxic/aerobic (A2O), were selected to investigate the emission characteristics of greenhouse gases (GHG), including carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O). Results showed that although the processes were different, the units presenting high GHG emission fluxes were remarkably similar, namely the highest CO2 and N2O emission fluxes occurred in the aerobic areas, and the highest CH4 emission fluxes occurred in the grit tanks. The GHG emission amount of each unit can be calculated from its area and GHG emission flux. The calculation results revealed that the maximum emission amounts of CO2, CH4 and N2O in the three wastewater treatment processes appeared in the aerobic areas in all cases. Theoretically, CH4 should be produced in anaerobic conditions, rather than aerobic conditions. However, results in this study showed that the CH4 emission fluxes in the forepart of the aerobic area were distinctly higher than in the anaerobic area. The situation for N2O was similar to that of CH4: the N2O emission flux in the aerobic area was also higher than that in the anoxic area. Through analysis of the GHG mass balance, it was found that the flow of dissolved GHG in the wastewater treatment processes and aerators may be the main reason for this phenomenon. Based on the monitoring and calculation results, GHG emission factors for the three wastewater treatment processes were determined. The A2O process had the highest CO2 emission factor of 319.3 g CO2/kg COD(removed), and the highest CH4 and N2O emission factors of 3.3 g CH4/kg COD(removed) and 3.6 g N2O/kg TN(removed) were observed in the Orbal oxidation ditch process.

Photoacoustic measurement of ammonia in the atmosphere: influence of water vapor and carbon dioxide

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

Rooth, R.A.; Verhage, A.J.L.; Wouters, L.W.

1990-09-01

The photoacoustic determination of the ammonia concentration in atmospheric air by absorption of CO{sub 2} laser radiation at 9.22 {mu}m is influenced by the presence of H{sub 2}O and CO{sub 2}. Kinetic cooling due to the coupling of excited CO{sub 2} and N{sub 2} levels causes important changes in phase and amplitude of the photoacoustic signal. Theoretical background is presented to deduce the correct NH{sub 3} concentration from the signal. The experimental setup used to perform field measurements is described. Adhesion of NH{sub 3} to the walls of the resonant photoacoustic cell was investigated. Temperature effects are treated. Field datamore » of NH{sub 3} and H{sub 2}O concentrations are presented. Key words: Photoacoustics, ammonia, kinetic cooling, trace gas measurements, ammonia adhesion, acoustic resonance, CO{sub 2} laser radiation, water vapor absorption, carbon dioxide absorption.« less

Flue gas adsorption by single-wall carbon nanotubes: A Monte Carlo study

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

Romero-Hermida, M. I.; Departamento de Física Condensada, Universidad de Sevilla, Av. Reina Mercedes s/n, 41012 Sevilla; Romero-Enrique, J. M.

Adsorption of flue gases by single-wall carbon nanotubes (SWCNT) has been studied by means of Monte Carlo simulations. The flue gas is modeled as a ternary mixture of N{sub 2}, CO{sub 2}, and O{sub 2}, emulating realistic compositions of the emissions from power plants. The adsorbed flue gas is in equilibrium with a bulk gas characterized by temperature T, pressure p, and mixture composition. We have considered different SWCNTs with different chiralities and diameters in a range between 7 and 20 Å. Our results show that the CO{sub 2} adsorption properties depend mainly on the bulk flue gas thermodynamic conditionsmore » and the SWCNT diameter. Narrow SWCNTs with diameter around 7 Å show high CO{sub 2} adsorption capacity and selectivity, but they decrease abruptly as the SWCNT diameter is increased. For wide SWCNT, CO{sub 2} adsorption capacity and selectivity, much smaller in value than for the narrow case, decrease mildly with the SWCNT diameter. In the intermediate range of SWCNT diameters, the CO{sub 2} adsorption properties may show a peculiar behavior, which depend strongly on the bulk flue gas conditions. Thus, for high bulk CO{sub 2} concentrations and low temperatures, the CO{sub 2} adsorption capacity remains high in a wide range of SWCNT diameters, although the corresponding selectivity is moderate. We correlate these findings with the microscopic structure of the adsorbed gas inside the SWCNTs.« less

Who contributes more to N2O emission during sludge bio-drying with two different aeration strategies, nitrifiers or denitrifiers?

PubMed

Zhang, Junya; Wang, Yuanyue; Yu, Dawei; Tong, Juan; Chen, Meixue; Sui, Qianwen; ChuLu, BuHe; Wei, Yuansong

2017-04-01

Global warming effects have drawn more and more attention to studying all sources and sinks of nitrous oxide (N 2 O). Sludge bio-drying, as an effective sludge treatment technology, is being adopted worldwide. In this study, two aeration strategies (piles I and II) were compared to investigate the primary contributors to N 2 O emission during sludge bio-drying through studying the evolution of functional genes involved in nitrification (amoA, hao, and nxrA) and denitrification (narG, nirS, nirK, norB, and nosZ) by quantitative PCR (qPCR). Results showed that the profile of N 2 O emission can be divided into three stages, traditional denitrification contributed largely to N 2 O emission at stage I (days 1-5), but N 2 O emission mainly happened at stage II (days 5-14) due to nitrifier denitrification and NH 2 OH accumulation by ammonia-oxidizing bacteria (AOB), accounting for 51.4% and 58.2% of total N 2 O emission for piles I and II, respectively. At stage III (days 14-21), nitrifier denitrification was inhibited because sludge bio-drying proceeded mainly by the physical aeration, thus N 2 O emission decreased and changed little. The improved aeration strategy availed pile I to reduce N 2 O emission much especially at stages II and III, respectively. These results indicated that nitrifier denitrification by AOB and biological NH 2 OH oxidation due to AOB made more contribution to N 2 O emission, and aeration strategy was crucial to mitigate N 2 O emission during sludge bio-drying.

Comparing N2O emissions at varying N rates from irrigated and rainfed corn in the US Midwest

NASA Astrophysics Data System (ADS)

Millar, N.; Kahmark, K.; Basso, B.; Robertson, G. P.

2011-12-01

Global N2O emissions from agriculture are estimated to be ~2.8 Pg CO2e yr-1 accounting for 60% of total anthropogenic emissions. N2O is the largest contributor to the GHG burden of cropping systems in the US, with annual estimated emissions of ~0.5 Tg primarily due to N fertilizer inputs and other soil management activities. Currently 23 million acres of corn, soybean and wheat are irrigated annually in the US with increased N2O emissions due to the practice likely under-reported in GHG inventories. Here we compare N2O emissions and yield from irrigated and rainfed corn at varying N rates between 0 and 246 kg N ha-1 from the Kellogg Biological Station in SW Michigan. Initial results show that N2O emissions increase with increasing N rate and are significantly higher from irrigated corn compared to rainfed corn at the same N rate. At increasing N rates daily emissions following an irrigation event were between 2.4 - 77.5 g N2O-N ha-1 from irrigated corn and 1.6 - 13.0 g N2O-N ha-1 from rainfed corn. Emissions data from automated and static chambers will be presented and trade-offs between N2O emissions, N fertilizer rate, crop yield and irrigation practice will be evaluated from an environmental and economic standpoint.

High-pressure sorption of nitrogen, carbon dioxide, and their mixtures on Argonne Premium Coals

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

Andreas Busch; Yves Gensterblum; Bernhard M. Krooss

2007-06-15

Gas sorption isotherms have been measured for carbon dioxide and nitrogen and their binary mixture (N{sub 2}/CO{sub 2} {approximately} 80/20) on three different moisture-equilibrated coals from the Argonne Premium Coal Sample Program by the U.S. Department of Energy, varying in rank from 0.25 to 1.68% vitrinite reflectance (VR{sub r}). The measurements were conducted at 55 C and at pressures up to 27 MPa for the pure gases and up to 10 MPa for the gas mixture. The effects of the large differences in equilibrium moisture contents (0.8 to 32.2%) on sorption capacity were estimated on the basis of the aqueousmore » solubility of CO{sub 2} and N{sub 2} at experimental conditions. Especially for the Beulah-Zap coal with an equilibrium moisture content of {approximately} 32%, the amount of dissolved CO{sub 2} contributes significantly to the overall storage capacity, whereas the amounts of N{sub 2} dissolved in the moisture water are low and can be neglected. Sorption measurements with nitrogen/carbon dioxide mixtures showed very low capacities for N{sub 2}. For Illinois coal, these excess sorption values were even slightly negative, probably due to small volumetric effects (changes in condensed phase volume). The evolution of the composition of the free gas phase in contact with the coal sample has been monitored continuously during each pressure step of the sorption tests. This composition changed strongly over time. Apparently, CO{sub 2} reaches sorption sites very quickly initially and is subsequently partly replaced by N{sub 2} molecules until concentration equilibration is reached. 18 refs., 10 figs., 2 tabs.« less

Modeling nitrous oxide emission from rivers: a global assessment.

PubMed

Hu, Minpeng; Chen, Dingjiang; Dahlgren, Randy A

2016-11-01

Estimates of global riverine nitrous oxide (N 2 O) emissions contain great uncertainty. We conducted a meta-analysis incorporating 169 observations from published literature to estimate global riverine N 2 O emission rates and emission factors. Riverine N 2 O flux was significantly correlated with NH 4 , NO 3 and DIN (NH 4  + NO 3 ) concentrations, loads and yields. The emission factors EF(a) (i.e., the ratio of N 2 O emission rate and DIN load) and EF(b) (i.e., the ratio of N 2 O and DIN concentrations) values were comparable and showed negative correlations with nitrogen concentration, load and yield and water discharge, but positive correlations with the dissolved organic carbon : DIN ratio. After individually evaluating 82 potential regression models based on EF(a) or EF(b) for global, temperate zone and subtropical zone datasets, a power function of DIN yield multiplied by watershed area was determined to provide the best fit between modeled and observed riverine N 2 O emission rates (EF(a): R 2  = 0.92 for both global and climatic zone models, n = 70; EF(b): R 2  = 0.91 for global model and R 2  = 0.90 for climatic zone models, n = 70). Using recent estimates of DIN loads for 6400 rivers, models estimated global riverine N 2 O emission rates of 29.6-35.3 (mean = 32.2) Gg N 2 O-N yr -1 and emission factors of 0.16-0.19% (mean = 0.17%). Global riverine N 2 O emission rates are forecasted to increase by 35%, 25%, 18% and 3% in 2050 compared to the 2000s under the Millennium Ecosystem Assessment's Global Orchestration, Order from Strength, Technogarden, and Adapting Mosaic scenarios, respectively. Previous studies may overestimate global riverine N 2 O emission rates (300-2100 Gg N 2 O-N yr -1 ) because they ignore declining emission factor values with increasing nitrogen levels and channel size, as well as neglect differences in emission factors corresponding to different nitrogen forms. Riverine N 2 O emission estimates will be further enhanced through refining emission factor estimates, extending measurements longitudinally along entire river networks and improving estimates of global riverine nitrogen loads. © 2016 John Wiley & Sons Ltd.

Leachate treatment in landfills is a significant N2O source.

PubMed

Wang, Xiaojun; Jia, Mingsheng; Zhang, Chengliang; Chen, Shaohua; Cai, Zucong

2017-10-15

The importance of methane (CH 4 ) emissions from landfills has been extensively documented, while the nitrous oxide (N 2 O) emissions from landfills are considered negligible. In this study, three landfills were selected to measure CH 4 and N 2 O emissions using the static chamber method. Dongbu (DB) and Dongfu (DF) landfills, both located in Xiamen city, Fujian Province, were classified as sanitary. The former started to receive solid waste from Xiamen city in 2009, and the latter was closed in 2009. Nanjing (NJ) landfill, located in Nanjing county, Fujian Province, was classified as managed. Results showed that for the landfill reservoirs, CH 4 emissions were significant, while N 2 O emissions occurred mainly in operating areas (on average, 16.3 and 19.0mgN 2 Om -2 h -1 for DB and NJ landfills, respectively) and made a negligible contribution to the total greenhouse gas emissions in term of CO 2 equivalent. However, significant N 2 O emissions were observed in the leachate treatment systems of sanitary landfills and contributed 72.8% and 45.6% of total emissions in term of CO 2 equivalent in DB and DF landfills, respectively. The N 2 O emission factor (EF) of the leachate treatment systems was in the range of 8.9-11.9% of the removed nitrogen. The total N 2 O emissions from the leachate treatment systems of landfills in Xiamen city were estimated to be as high as 8.55gN 2 O-Ncapita -1 yr -1 . These results indicated that N 2 O emissions from leachate treatment systems of sanitary landfills were not negligible and should be included in national and/or local inventories of greenhouse gas emissions. Copyright © 2017 Elsevier B.V. All rights reserved.

Preparation and characterization of V/TiO{sub 2} nanocatalyst with magnetic nucleus of iron

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

Feyzi, Mostafa; Rafiee, Hamid Reza, E-mail: rafieehr@yahoo.com; Ranjbar, Shahram

2013-11-15

Graphical abstract: - Highlights: • Fe-V/TiO{sub 2} nanocatalyst is prepared. • Combination of sol–gel and wetness impregnation methods. • Facile separation of catalyst from medium by magnet. - Abstract: A magnetic composite containing V/TiO{sub 2} was prepared by combination of sol–gel and wetness impregnation methods. The effects of synthesis temperature, different weight percents of Fe supported on TiO{sub 2}, vanadium loading and the heating rate of calcination on the structure and morphology of nanocatalyst were investigated. The optimum conditions for synthesized catalyst were 40 wt.% of Fe, 15 wt.% of V and synthesis temperature equal to 30 °C. Characterization ofmore » catalyst is carried out using XRD, TGA, DSC, SEM, FTIR and N{sub 2} physisorption measurements. The magnetic character of nanocatalyst was measured using VSM, which showed the typical paramagnetic behavior of sample at room temperature with a saturation magnetization value equal to 8.283 emu/g. The nanocatalyst has a particle size about 56 nm and can easily be separated from medium by a magnet.« less

Synthesis and characterization of Fe{sub 3}O{sub 4}: Porous carbon nanocomposites for biosensor application

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

Arora, Manju, E-mail: marora@nplindia.org; Zargar, R. A., E-mail: rayeesphy12@gmail.com

2015-08-28

Fe{sub 3}O{sub 4}:Porous carbon (Fe{sub 3}O{sub 4}:PC) nano-magnetic composites were prepared by using different weight fractions of acid treated PC by the chemical co-precipitation route and annealed at 573 K, 773 K and 973 K temperatures in inert N{sub 2} gas atmosphere for 2 hrs to obtain desired stoichiometry of nanocomposites. The structural, morphological and magnetic properties of these composites were characterized by powder XRD, TEM, EPR and VSM analytical techniques. The crystallinity of the composites, g-value and spin concentration increases with increasing annealing temperature. TEM images confirmed the formation of nanosized ferrite nanoprticles whose size increases from 23 nm to 54 nm on increasingmore » annealing temperature. Porous carbon increases porosity, coercivity and reduces saturation magnetization of these prepared nanocomposites.« less

Effective group index of refraction in non-thermal plasma photonic crystals

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

Mousavi, A.; Sadegzadeh, S., E-mail: sadegzadeh@azaruniv.edu

Plasma photonic crystals (PPCs) are periodic arrays that consist of alternate layers of micro-plasma and dielectric. These structures are used to control the propagation of electromagnetic waves. This paper presents a survey of research on the effect of non-thermal plasma with bi-Maxwellian distribution function on one dimensional PPC. A plasma with temperature anisotropy is not in thermodynamic equilibrium and can be described by the bi-Maxwellian distribution function. By using Kronig-Penny's model, the dispersion relation of electromagnetic modes in one dimensional non-thermal PPC (NPPC) is derived. The band structure, group velocity v{sub g}, and effective group index of refraction n{sub eff}(g)more » of such NPPC structure with TeO{sub 2} as the material of dielectric layers have been studied. The concept of negative group velocity and negative n{sub eff}(g), which indicates an anomalous behaviour of the PPCs, are also observed in the NPPC structures. Our numerical results provide confirmatory evidence that unlike PPCs there are finite group velocity and non-zero effective group indexes of refraction in photonic band gaps (PBGs) that lie in certain ranges of normalized frequency. In other words, inside the PBGs of NPPCs, n{sub eff}(g) becomes non-zero and photons travel with a finite group velocity. In this special case, this velocity varies alternately between 20c and negative values of the order 10{sup 3}c (c is the speed of light in vacuum)« less

Ecological controls on N2O emission in surface litter and near-surface soil of a managed grassland: modelling and measurements

NASA Astrophysics Data System (ADS)

Grant, Robert F.; Neftel, Albrecht; Calanca, Pierluigi

2016-06-01

Large variability in N2O emissions from managed grasslands may occur because most emissions originate in surface litter or near-surface soil where variability in soil water content (θ) and temperature (Ts) is greatest. To determine whether temporal variability in θ and Ts of surface litter and near-surface soil could explain this in N2O emissions, a simulation experiment was conducted with ecosys, a comprehensive mathematical model of terrestrial ecosystems in which processes governing N2O emissions were represented at high temporal and spatial resolution. Model performance was verified by comparing N2O emissions, CO2 and energy exchange, and θ and Ts modelled by ecosys with those measured by automated chambers, eddy covariance (EC) and soil sensors on an hourly timescale during several emission events from 2004 to 2009 in an intensively managed pasture at Oensingen, Switzerland. Both modelled and measured events were induced by precipitation following harvesting and subsequent fertilizing or manuring. These events were brief (2-5 days) with maximum N2O effluxes that varied from < 1 mgNm-2h-1 in early spring and autumn to > 3 mgNm-2h-1 in summer. Only very small emissions were modelled or measured outside these events. In the model, emissions were generated almost entirely in surface litter or near-surface (0-2 cm) soil, at rates driven by N availability with fertilization vs. N uptake with grassland regrowth and by O2 supply controlled by litter and soil wetting relative to O2 demand from microbial respiration. In the model, NOx availability relative to O2 limitation governed both the reduction of more oxidized electron acceptors to N2O and the reduction of N2O to N2, so that the magnitude of N2O emissions was not simply related to surface and near-surface θ and Ts. Modelled N2O emissions were found to be sensitive to defoliation intensity and timing which controlled plant N uptake and soil θ and Ts prior to and during emission events. Reducing leaf area index (LAI) remaining after defoliation to half that under current practice and delaying harvesting by 5 days raised modelled N2O emissions by as much as 80 % during subsequent events and by an average of 43 % annually. Modelled N2O emissions were also found to be sensitive to surface soil properties. Increasing near-surface bulk density by 10 % raised N2O emissions by as much as 100 % during emission events and by an average of 23 % annually. Relatively small spatial variation in management practices and soil surface properties could therefore cause the large spatial variation in N2O emissions commonly found in field studies. The global warming potential from annual N2O emissions in this intensively managed grassland largely offset those from net C uptake in both modelled and field experiments. However, model results indicated that this offset could be adversely affected by suboptimal land management and soil properties.

Appraisal of the nitrogen-15 natural-abundance method for quantifying dinitrogen fixation

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

Bremer, E.; van Kessel, C.

Several investigators have questioned the use of the {sup 15}N natural-abundance method of estimating N{sub 2} fixation because of variability in soil {delta}{sup 15}N and small differences between the {delta}{sup 15}N of soil N and atmospheric N. Investigations were conducted to compare the {sup 15}N natural-abundance and {sup 15}N-isotope-dilution methods for estimating N{sub 2} fixation of field-grown pea (Pisum sativum L.) and lentil (Lens culinaris Medik.). Spatial variability was assessed at three sites by determining the {delta}{sup 15}N of non-N{sub 2}-fixing plants. Seasonal variation in {delta}{sup 15}N for spring and winter wheat (Triticum aestivum L.), flax (Linum usitatissimum L.), barleymore » (Hordeum vulgare L.), rape (Brassica napus L.) and lentil was determined at one site. Comparisons between {delta}{sup 15}N and {sup 15}N-enriched isotope-dilution methods for estimating N{sub 2} fixation by lentil were conducted at several sites over a 3-yr period. Variability in {delta}{sup 15}N of the reference plant was site dependent: the {delta}{sup 15}N ranged from 2.8 to 9.3 at the first site, 3.4 to 8.8 at the second site, and 3.5 to 6.2 at the third site. The average {delta}{sup 15}N of four of the five non-N{sub 2}-fixing plants increased from 5.4 at 42 d after planting to 6.9 at the final harvest. The fifth non-N{sub 2}-fixing plant, rape, accumulated most of its N during the first 42 d after planting, and its {delta}{sup 15}N value declined from 8.1 at 42 d after planting to 7.3 at the final harvest. Estimates of N{sub 2} fixation were not significantly different in 18 out of 21 comparisons; in two comparisons in the {delta}{sup 15}N method and in one comparison the {sup 15}N-enriched method provided higher estimates of N{sub 2} fixation. Overall, both methods appeared to provide equally reliable estimates of N{sub 2} fixation for lentil.« less

Ultraviolet emission enhancement in ZnO thin films modified by nanocrystalline TiO2

NASA Astrophysics Data System (ADS)

Zheng, Gaige; Lu, Xi; Qian, Liming; Xian, Fenglin

2017-05-01

In this study, nanocrystalline TiO2 modified ZnO thin films were prepared by electron beam evaporation. The structural, morphological and optical properties of the samples were analyzed by X-ray diffraction (XRD), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), UV-visible spectroscopy, fluorescence spectroscopy, respectively. The composition of the films was examined by energy dispersive X-ray spectroscopy (EDX). The photoluminescent spectrum shows that the pure ZnO thin film exhibits an ultraviolet (UV) emission peak and a strong green emission band. Surface analysis indicates that the ZnO thin film contains many oxygen vacancy defects on the surface. After the ZnO thin film is modified by the nanocrystalline TiO2 layer, the UV emission of ZnO is largely enhanced and the green emission is greatly suppressed, which suggests that the surface defects such as oxygen vacancies are passivated by the TiO2 capping layer. As for the UV emission enhancement of the ZnO thin film, the optimized thickness of the TiO2 capping layer is ∼16 nm. When the thickness is larger than 16 nm, the UV emission of the ZnO thin film will decrease because the TiO2 capping layer absorbs most of the excitation energy. The UV emission enhancement in the nanocrystalline TiO2 modified ZnO thin film can be attributed to surface passivation and flat band effect.

Nitrogen-rich organic soils under warm well-drained conditions are global nitrous oxide emission hotspots.

PubMed

Pärn, Jaan; Verhoeven, Jos T A; Butterbach-Bahl, Klaus; Dise, Nancy B; Ullah, Sami; Aasa, Anto; Egorov, Sergey; Espenberg, Mikk; Järveoja, Järvi; Jauhiainen, Jyrki; Kasak, Kuno; Klemedtsson, Leif; Kull, Ain; Laggoun-Défarge, Fatima; Lapshina, Elena D; Lohila, Annalea; Lõhmus, Krista; Maddison, Martin; Mitsch, William J; Müller, Christoph; Niinemets, Ülo; Osborne, Bruce; Pae, Taavi; Salm, Jüri-Ott; Sgouridis, Fotis; Sohar, Kristina; Soosaar, Kaido; Storey, Kathryn; Teemusk, Alar; Tenywa, Moses M; Tournebize, Julien; Truu, Jaak; Veber, Gert; Villa, Jorge A; Zaw, Seint Sann; Mander, Ülo

2018-03-19

Nitrous oxide (N 2 O) is a powerful greenhouse gas and the main driver of stratospheric ozone depletion. Since soils are the largest source of N 2 O, predicting soil response to changes in climate or land use is central to understanding and managing N 2 O. Here we find that N 2 O flux can be predicted by models incorporating soil nitrate concentration (NO 3 - ), water content and temperature using a global field survey of N 2 O emissions and potential driving factors across a wide range of organic soils. N 2 O emissions increase with NO 3 - and follow a bell-shaped distribution with water content. Combining the two functions explains 72% of N 2 O emission from all organic soils. Above 5 mg NO 3 - -N kg -1 , either draining wet soils or irrigating well-drained soils increases N 2 O emission by orders of magnitude. As soil temperature together with NO 3 - explains 69% of N 2 O emission, tropical wetlands should be a priority for N 2 O management.

Morphology and structure features of ZnAl{sub 2}O{sub 4} spinel nanoparticles prepared by matrix-isolation-assisted calcination

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

Du, Xuelian, E-mail: xueliandu@126.com; Li, Liqiang; Zhang, Wenxing

2015-01-15

Graphical abstract: The substrate ZnO as the isolation medium is effective in preventing the sintering and agglomeration of ZnAl{sub 2}O{sub 4} nanoparticles, and it also prevents their contamination. High purity, well-dispersed, and single-crystal ZnAl{sub 2}O{sub 4} nanoparticles with 3.72 eV band gap were obtained. - Abstract: Well-dispersed ZnAl{sub 2}O{sub 4} spinel nanoparticles with an average crystalline size of 25.7 nm were synthesized successfully and easily by polymer-network and matrix-isolation-assisted calcination. The product microstructure and features were investigated by X-ray diffractometry, thermogravimetric and differential thermal analysis, Fourier transform-infrared spectroscopy, N{sub 2} adsorption–desorption isotherms, and energy dispersive X-ray spectra. The morphology andmore » optical performance of the as-prepared ZnAl{sub 2}O{sub 4} nanoparticles were characterized by scanning electron microscope, transmission electron microscopy, and photoluminescence spectrometer. Experimental results indicate that excess ZnO acted as the isolation medium is effective in preventing the sintering and agglomeration of ZnAl{sub 2}O{sub 4} nanoparticles, and it also prevents their contamination. Then, high purity and well-dispersed ZnAl{sub 2}O{sub 4} nanoparticles with single-crystal structure were obtained.« less

Relating N2O emissions during biological nitrogen removal with operating conditions using multivariate statistical techniques.

PubMed

Vasilaki, V; Volcke, E I P; Nandi, A K; van Loosdrecht, M C M; Katsou, E

2018-04-26

Multivariate statistical analysis was applied to investigate the dependencies and underlying patterns between N 2 O emissions and online operational variables (dissolved oxygen and nitrogen component concentrations, temperature and influent flow-rate) during biological nitrogen removal from wastewater. The system under study was a full-scale reactor, for which hourly sensor data were available. The 15-month long monitoring campaign was divided into 10 sub-periods based on the profile of N 2 O emissions, using Binary Segmentation. The dependencies between operating variables and N 2 O emissions fluctuated according to Spearman's rank correlation. The correlation between N 2 O emissions and nitrite concentrations ranged between 0.51 and 0.78. Correlation >0.7 between N 2 O emissions and nitrate concentrations was observed at sub-periods with average temperature lower than 12 °C. Hierarchical k-means clustering and principal component analysis linked N 2 O emission peaks with precipitation events and ammonium concentrations higher than 2 mg/L, especially in sub-periods characterized by low N 2 O fluxes. Additionally, the highest ranges of measured N 2 O fluxes belonged to clusters corresponding with NO 3 -N concentration less than 1 mg/L in the upstream plug-flow reactor (middle of oxic zone), indicating slow nitrification rates. The results showed that the range of N 2 O emissions partially depends on the prior behavior of the system. The principal component analysis validated the findings from the clustering analysis and showed that ammonium, nitrate, nitrite and temperature explained a considerable percentage of the variance in the system for the majority of the sub-periods. The applied statistical methods, linked the different ranges of emissions with the system variables, provided insights on the effect of operating conditions on N 2 O emissions in each sub-period and can be integrated into N 2 O emissions data processing at wastewater treatment plants. Copyright © 2018. Published by Elsevier Ltd.

Assessment of nitrous oxide and methane emissions for California agriculture

NASA Astrophysics Data System (ADS)

Horwath, W. R.; Burger, M.; Assa, Y.; Wilson, T. J.

2012-12-01

The California Global Warming Solutions Act of 2006 (AB 32) mandates comprehensive strategies to reduce nitrous oxide (N2O) and methane (CH4) emissions. In agriculture crop production, sources of N2O are related to nitrogen fertilization while CH4 emission is associated with rice production. More than half the GHG emissions from agriculture are attributed to N2O production. Currently, baseline N2O emission data for most cropping systems in the State is lacking. Estimates of CH4 emission in rice have been established from previous studies, but a lack of information exists for its expansion into the San Joaquin Delta to address subsidence issues. The paucity of N2O emission data has hampered biogeochemical modeling efforts. The objectives of this assessment are to (1) measure annual N2O and CH4 emissions for major California crops (vineyards, almonds, tomato, wheat, alfalfa, lettuce, and rice) under typical management practices, (2) characterize the effects of environmental factors on the temporal profile of N2O and CH4 emissions, and (3) determine N2O emission factors. The growth of rice in Delta peat soils produced highly variable CH4 emissions depending on tillage intensity. In 2010, standard tillage produced 184 kg CH4-C/ha while in 2011 after deep plowing placing rice residue deeper into the soil, only 26 kg CH4-C/ha was observed. In processing tomato systems, an average 2.5 kg N2O-N/ha was emitted with standard fertilization (160 kg N / ha), similar to background emissions and those from a drip irrigated system, while 4.0 to 5.8 kg N2O-N /ha y-1 was emitted at fertilizer rates of 225 and 300 kg N /ha (see Fig. 1 for example of temporal sources of emissions). About half the annual emissions were emitted within 3 d after the first seasonal rainfall event. In other tomato studies, estimated losses of fertilizer N as N2O were 0.38 ± 0.03 kg/ha y-1 in a drip irrigated system and 1.79 ± 0.21 kg/ha y-1 in furrow irrigated system, which was equivalent to 0.19% and 0.73% of the added fertilizer, respectively. In a lettuce production system, annual N2O emissions were about 1 kg N2O-N /ha y-1. In a wheat system, emissions during the growing season in the rainy season were between 1.0 and 1.5 kg N2O-N, with highest emissions occurring after anhydrous ammonium applications. Older alfalfa fields were larger sources of N2O. This two-year dataset will serve as the basis for developing mitigation practices.igure 1. Nitrous oxide emissions in tomato systems in 2009/10 during the rainy season, between starter and sidedress application of fertilizers, during the growing season and after the first rainfall after harvest.

Ion chamber absorbed dose calibration coefficients, N{sub D,w}, measured at ADCLs: Distribution analysis and stability

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

Muir, B. R., E-mail: Bryan.Muir@nrc-cnrc.gc.ca

2015-04-15

Purpose: To analyze absorbed dose calibration coefficients, N{sub D,w}, measured at accredited dosimetry calibration laboratories (ADCLs) for client ionization chambers to study (i) variability among N{sub D,w} coefficients for chambers of the same type calibrated at each ADCL to investigate ion chamber volume fluctuations and chamber manufacturing tolerances; (ii) equivalency of ion chamber calibration coefficients measured at different ADCLs by intercomparing N{sub D,w} coefficients for chambers of the same type; and (iii) the long-term stability of N{sub D,w} coefficients for different chamber types by investigating repeated chamber calibrations. Methods: Large samples of N{sub D,w} coefficients for several chamber types measuredmore » over the time period between 1998 and 2014 were obtained from the three ADCLs operating in the United States. These are analyzed using various graphical and numerical statistical tests for the four chamber types with the largest samples of calibration coefficients to investigate (i) and (ii) above. Ratios of calibration coefficients for the same chamber, typically obtained two years apart, are calculated to investigate (iii) above and chambers with standard deviations of old/new ratios less than 0.3% meet stability requirements for accurate reference dosimetry recommended in dosimetry protocols. Results: It is found that N{sub D,w} coefficients for a given chamber type compared among different ADCLs may arise from differing probability distributions potentially due to slight differences in calibration procedures and/or the transfer of the primary standard. However, average N{sub D,w} coefficients from different ADCLs for given chamber types are very close with percent differences generally less than 0.2% for Farmer-type chambers and are well within reported uncertainties. Conclusions: The close agreement among calibrations performed at different ADCLs reaffirms the Calibration Laboratory Accreditation Subcommittee process of ensuring ADCL conformance with National Institute of Standards and Technology standards. This study shows that N{sub D,w} coefficients measured at different ADCLs are statistically equivalent, especially considering reasonable uncertainties. This analysis of N{sub D,w} coefficients also allows identification of chamber types that can be considered stable enough for accurate reference dosimetry.« less

Nitrous Oxide Emissions From a Maize/Soybean Rotation Following a Precipitation Event

NASA Astrophysics Data System (ADS)

Zheng, J.; Doskey, P. V.

2011-12-01

Agricultural soils are the largest anthropogenic source of nitrous oxide (N2O), which is one of the major greenhouse gases. Emissions of N2O from agricultural soils are highly episodic and primarily occur in pulses of emissions following fertilization, spring thaw, and precipitation events. Anaerobic denitrification is the major source of N2O emitted from agricultural soils. During denitrification, NO3- is converted to NO, N2O or N2 by a diverse group of microorganisms. Precipitation is an important environmental factor regulating N2O emissions as soil water filled pore space (WFPS) controls the diffusivity and solubility of O2 and N2O, and thus, enzyme affinity and activity of denitrifying microorganisms. The primary objective of the study is to investigate N2O emission patterns and possible mechanisms responsible for N2O emissions following precipitation events. We measured plot level N2O fluxes by the static chamber technique in- and between-the-row of young soybean at the AmeriFlux site in Bondville, Illinois following a precipitation event. Gas samples were taken 12 h before a heavy rainfall, and 6, 12 and 24 h after the rain. Two distinct pulses were observed following the rainfall. The first pulse occurred 6 h after the rain, with a 3-fold increase in the rate of N2O emissions (73.2 μg m-2 h-1) compared with emissions 12 h before the rain (24.0 μg m-2 h-1). The N2O emission rate decreased to 48.2 μg m-2 h-1 12 h after the rain. The second pulse was observed 24 h after the rain, with an emission rate of 63.1 μg m-2 h-1. Phospholipid fatty acids (PLFAs) were extracted from soil samples taken from corresponding plots to estimate the total living microbial biomass. There were no significant changes in total living microbial biomass (in ng PLFAs g-1 soil) between samples taken 12 h before the rain and 6 h after the rain, although microbial activity apparently increased. Increases in gram negative bacteria and fungi were observed 24 h after the rain. The first pulse 6 h following the rain might be explained by displacement of air-filled pore space and exhalation of soil gases containing elevated levels of N2O caused by water infiltration. Microbial activity might also contribute to this N2O pulse since denitrification enzymes nar, nir, and nor can persist in dry soils. The decrease in N2O emissions between the pulses (12 h following the rain) might indicate increases in nitrous oxide reductase (nos) activities and evolution of denitrification gases as N2. The second pulse in N2O emissions occurred 24 h after the rain, when N2O production exceeded N2O consumption. Our observation of N2O emissions before and after a precipitation event exhibit a pattern similar to the dynamics of denitrification enzymes observed in incubated soils. The first in situ observation of a two-pulse pattern in N2O emissions following a precipitation event has widespread significance for designing N2O emission measurement strategies and estimating annual budgets.