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Report of 1,000 Hour Catalyst Longevity Evaluation

Description: This report presents the results of a 1,000 hour, high-pressure, catalyst longevity test for the decomposition of concentrated sulfuric acid. The reaction is used for both the sulfur-iodine (S-I) cycle and hybrid sulfur cycle. By the time of the delivery date of April 17, 2009, for project milestone no. 2NIN07TC050114, the 1% Pt/TiO2 catalyst had been in the reaction environment for 658 hours. During the first 480 hours of testing, the catalyst activity provided stable, near-equilibrium yields of 46.8% SO2 and 22.8% O2. However, product yields declined at sample exposure times >480 hours. At 658 hours of operation, catalyst activity (based on oxygen yield) declined to 57% relative to the stable period of catalyst activity. Thus, as of April 17, this catalyst did not provide the desired stability level of <10% degradation per 1,000 hours. The experiment was terminated on April 27, after 792 hours, when a fitting failed and the catalyst was displaced from the reactor such that the sample could not be recovered. Oxygen conversion at the end of the experiment was 12.5% and declining, suggesting that at that point, catalyst activity had decreased to 54% of the initial level.
Date: June 1, 2009
Creator: Ginosar, Daniel M.
Partner: UNT Libraries Government Documents Department

CATALYSTS NHI Thermochemical Systems FY 2009 Year-End Report

Description: Fiscal Year 2009 work in the Catalysts project focused on advanced catalysts for the decomposition of sulfuric acid, a reaction common to both the Sulfur-Iodine (S-I) cycle and the Hybrid Sulfur cycle. Prior years’ effort in this project has found that although platinum supported on titanium oxide will be an acceptable catalyst for sulfuric acid decomposition in the integrated laboratory scale (ILS) project, the material has short comings, including significant cost and high deactivation rates due to sintering and platinum evaporation. For pilot and larger scale systems, the catalyst stability needs to be improved significantly. In Fiscal Year 2008 it was found that at atmospheric pressure, deactivation rates of a 1 wt% platinum catalyst could be reduced by 300% by adding either 0.3 wt% iridium (Ir) or 0.3 wt% ruthenium (Ru) to the catalyst. In Fiscal Year 2009, work focused on examining the platinum group metal catalysts activity and stability at elevated pressures. In addition, simple and complex metal oxides are known to catalyze the sulfuric acid decomposition reaction. These metal oxides could offer activities comparable to platinum but at significantly reduced cost. Thus a second focus for Fiscal Year 2009 was to explore metal oxide catalysts for the sulfuric acid decomposition reaction. In Fiscal Year 2007 several commercial activated carbons had been identified for the HI decomposition reaction; a reaction specific to the S-I cycle. Those materials should be acceptable for the pilot scale project. The activated carbon catalysts have some disadvantages including low activity at the lower range of reactor operating temperature (350 to 400°C) and a propensity to generate carbon monoxide in the presence of water that could contaminate the hydrogen product, but due to limited funding, this area had low priority in Fiscal Year 2009. Fiscal Year 2009 catalyst work included five tasks: development, and testing ...
Date: September 1, 2009
Creator: Ginosar, Daniel M.
Partner: UNT Libraries Government Documents Department


Description: Two hybrid sulfur (HyS) cycle process flowsheets intended for use with high-temperature gas-cooled reactors (HTGRs) are presented. The flowsheets were developed for the Next Generation Nuclear Plant (NGNP) program, and couple a proton exchange membrane (PEM) electrolyzer for the SO2-depolarized electrolysis step with a silicon carbide bayonet reactor for the high-temperature decomposition step. One presumes an HTGR reactor outlet temperature (ROT) of 950 C, the other 750 C. Performance was improved (over earlier flowsheets) by assuming that use of a more acid-tolerant PEM, like acid-doped poly[2,2'-(m-phenylene)-5,5'-bibenzimidazole] (PBI), instead of Nafion{reg_sign}, would allow higher anolyte acid concentrations. Lower ROT was accommodated by adding a direct contact exchange/quench column upstream from the bayonet reactor and dropping the decomposition pressure. Aspen Plus was used to develop material and energy balances. A net thermal efficiency of 44.0% to 47.6%, higher heating value basis is projected for the 950 C case, dropping to 39.9% for the 750 C case.
Date: July 6, 2011
Creator: Gorensek, M.
Partner: UNT Libraries Government Documents Department

The Genome of the Epsilonproteobacterial Chemolithoautotroph Sulfurimonas dentrificans

Description: Sulfur-oxidizing epsilonproteobacteria are common in a variety of sulfidogenic environments. These autotrophic and mixotrophic sulfur-oxidizing bacteria are believed to contribute substantially to the oxidative portion of the global sulfur cycle. In order to better understand the ecology and roles of sulfur-oxidizing epsilonproteobacteria, in particular those of the widespread genus Sulfurimonas, in biogeochemical cycles, the genome of Sulfurimonas denitrificans DSM1251 was sequenced. This genome has many features, including a larger size (2.2 Mbp), that suggest a greater degree of metabolic versatility or responsiveness to the environment than seen for most of the other sequenced epsilonproteobacteria. A branched electron transport chain is apparent, with genes encoding complexes for the oxidation of hydrogen, reduced sulfur compounds, and formate and the reduction of nitrate and oxygen. Genes are present for a complete, autotrophic reductive citric acid cycle. Many genes are present that could facilitate growth in the spatially and temporally heterogeneous sediment habitat from where Sulfurimonas denitrificans was originally isolated. Many resistance-nodulation-development family transporter genes (10 total) are present; of these, several are predicted to encode heavy metal efflux transporters. An elaborate arsenal of sensory and regulatory protein-encoding genes is in place, as are genes necessary to prevent and respond to oxidative stress.
Date: August 8, 2007
Creator: Class, USF Genomics; Sievert, Stefan M.; Scott, Kathleen M.; Klotz, Martin G.; Chain, Patrick S.G.; Hauser, Loren J. et al.
Partner: UNT Libraries Government Documents Department

The Hybrid Sulfur Cycle for Nuclear Hydrogen Production

Description: Two Sulfur-based cycles--the Sulfur-Iodine (SI) and the Hybrid Sulfur (HyS)--have emerged as the leading thermochemical water-splitting processes for producing hydrogen utilizing the heat from advanced nuclear reactors. Numerous international efforts have been underway for several years to develop the SI Cycle, but development of the HyS Cycle has lagged. The purpose of this paper is to discuss the background, current status, recent development results, and the future potential for this thermochemical process. Savannah River National Laboratory (SRNL) has been supported by the U.S. Department of Energy Office of Nuclear Energy, Science, and Technology since 2004 to evaluate and to conduct research and development for the HyS Cycle. Process design studies and flowsheet optimization have shown that an overall plant efficiency (based on nuclear heat converted to hydrogen product, higher heating value basis) of over 50% is possible with this cycle. Economic studies indicate that a nuclear hydrogen plant based on this process can be economically competitive, assuming that the key component, the sulfur dioxide-depolarized electrolyzer, can be successfully developed. SRNL has recently demonstrated the use of a proton-exchange-membrane electrochemical cell to perform this function, thus holding promise for economical and efficient hydrogen production.
Date: September 8, 2005
Creator: Summers, William A.; Gorensek, Maximilian B. & Buckner, Melvin R.
Partner: UNT Libraries Government Documents Department

Addition of Tropospheric Chemistry and Aerosols to the NCAR Community Climate System Model

Description: Atmospheric chemistry and aerosols have several important roles in climate change. They affect the Earth's radiative balance directly: cooling the earth by scattering sunlight (aerosols) and warming the Earth by trapping the Earth's thermal radiation (methane, ozone, nitrous oxide, and CFCs are greenhouse gases). Atmospheric chemistry and aerosols also impact many other parts of the climate system: modifying cloud properties (aerosols can be cloud condensation nuclei), fertilizing the biosphere (nitrogen species and soil dust), and damaging the biosphere (acid rain and ozone damage). In order to understand and quantify the effects of atmospheric chemistry and aerosols on the climate and the biosphere in the future, it is necessary to incorporate atmospheric chemistry and aerosols into state-of-the-art climate system models. We have taken several important strides down that path. Working with the latest NCAR Community Climate System Model (CCSM), we have incorporated a state-of-the-art atmospheric chemistry model to simulate tropospheric ozone. Ozone is not just a greenhouse gas, it damages biological systems including lungs, tires, and crops. Ozone chemistry is also central to the oxidizing power of the atmosphere, which destroys a lot of pollutants in the atmosphere (which is a good thing). We have also implemented a fast chemical mechanism that has high fidelity with the full mechanism, for significantly reduced computational cost (to facilitate millennium scale simulations). Sulfate aerosols have a strong effect on climate by reflecting sunlight and modifying cloud properties. So in order to simulate the sulfur cycle more fully in CCSM simulations, we have linked the formation of sulfate aerosols to the oxidizing power of the atmosphere calculated by the ozone mechanisms, and to dimethyl sulfide emissions from the ocean ecosystem in the model. Since the impact of sulfate aerosols depends on the relative abundance of other aerosols in the atmosphere, we also implemented interactive simulation ...
Date: November 14, 2005
Creator: Cameron-Smith, P; Lamarque, J; Connell, P; Chuang, C; Rotman, D & Taylor, J
Partner: UNT Libraries Government Documents Department


Description: The Hybrid Sulfur (HyS) cycle (Fig. 1) is one of the simplest, all-fluids thermochemical cycles that has been devised for splitting water with a high-temperature nuclear or solar heat source. It was originally patented by Brecher and Wu in 1975 and extensively developed by Westinghouse in the late 1970s and early 1980s. As its name suggests, the only element used besides hydrogen and oxygen is sulfur, which is cycled between the +4 and +6 oxidation states. HyS comprises two steps. One is the thermochemical (&gt;800 C) decomposition of sulfuric acid (H{sub 2}SO{sub 4}) to sulfur dioxide (SO{sub 2}), oxygen (O{sub 2}), and water. H{sub 2}SO{sub 4} = SO{sub 2} + 1/2 O{sub 2} + H{sub 2}O. The other is the SO{sub 2}-depolarized electrolysis of water to H{sub 2}SO{sub 4} and hydrogen (H{sub 2}), SO{sub 2} + 2 H{sub 2}O = H{sub 2}SO{sub 4} + H{sub 2}, E{sup o} = -0.156 V, explaining the 'hybrid' designation. These two steps taken together split water into H{sub 2} and O{sub 2} using heat and electricity. Researchers at the Savannah River National Laboratory (SRNL) and at the University of South Carolina (USC) have successfully demonstrated the use of proton exchange membrane (PEM) electrolyzers (Fig. 2) for the SO{sub 2}-depolarized electrolysis (sulfur oxidation) step, while Sandia National Laboratories (SNL) successfully demonstrated the high-temperature sulfuric acid decomposition (sulfur reduction) step using a bayonet-type reactor (Fig. 3). This latter work was performed as part of the Sulfur-Iodine (SI) cycle Integrated Laboratory Scale demonstration at General Atomics (GA). The combination of these two operations results in a simple process that will be more efficient and cost-effective for the massive production of hydrogen than alkaline electrolysis. Recent developments suggest that the use of PEMs other than Nafion will allow sulfuric acid to be produced at higher concentrations (&gt;60 wt%), ...
Date: March 24, 2010
Creator: Gorensek, M. & Summers, W.
Partner: UNT Libraries Government Documents Department


Description: The primary objective of the DOE-NE Nuclear Hydrogen Initiative (NHI) is to develop the nuclear hydrogen production technologies necessary to produce hydrogen at a cost competitive with other alternative transportation fuels. The focus of the NHI is on thermochemical cycles and high temperature electrolysis that can be powered by heat from high temperature gas reactors. The Savannah River National Laboratory (SRNL) has been tasked with the primary responsibility to perform research and development in order to characterize, evaluate and develop the Hybrid Sulfur (HyS) thermochemical process. This report documents work during the first quarter of Fiscal Year 2009, for the period between January 1, 2009 and March 31, 2009. The HyS Process is a two-step hybrid thermochemical cycle that is part of the 'Sulfur Family' of cycles. As a sulfur cycle, it uses high temperature thermal decomposition of sulfuric acid to produce oxygen and to regenerate the sulfur dioxide reactant. The second step of the process uses a sulfur dioxide depolarized electrolyzer (SDE) to split water and produce hydrogen by electrochemically reacting sulfur dioxide with H{sub 2}O. The SDE produces sulfuric acid, which is then sent to the acid decomposer to complete the cycle. The DOE NHI program is developing the acid decomposer at Sandia National Laboratory for application to both the HyS Process and the Sulfur Iodine Cycle. The SDE is being developed at SRNL. During FY05 and FY06, SRNL designed and conducted proof-of-concept testing for a SDE using a low temperature, PEM fuel cell-type design concept. The advantages of this design concept include high electrochemical efficiency, small footprint and potential for low capital cost, characteristics that are crucial for successful implementation on a commercial scale. During FY07, SRNL extended the range of testing of the SDE to higher temperature and pressure, conducted a 100-hour longevity test with a ...
Date: April 15, 2009
Creator: Herman, D; David Hobbs, D; Hector Colon-Mercado, H; Timothy Steeper, T; John Steimke, J & Mark Elvington, M
Partner: UNT Libraries Government Documents Department

GeoChip 3.0 as a high-thoughput tool for analyzing microbial community composition, structure, and functional activity

Description: A new generation of functional gene arrays (FGAs; GeoChip 3.0) has been developed, with {approx}28,000 probes covering approximately 57,000 gene variants from 292 functional gene families involved in carbon, nitrogen, phosphorus and sulfur cycles, energy metabolism, antibiotic resistance, metal resistance and organic contaminant degradation. GeoChip 3.0 also has several other distinct features, such as a common oligo reference standard (CORS) for data normalization and comparison, a software package for data management and future updating and the gyrB gene for phylogenetic analysis. Computational evaluation of probe specificity indicated that all designed probes would have a high specificity to their corresponding targets. Experimental analysis with synthesized oligonucleotides and genomic DNAs showed that only 0.0036-0.025% false-positive rates were observed, suggesting that the designed probes are highly specific under the experimental conditions examined. In addition, GeoChip 3.0 was applied to analyze soil microbial communities in a multifactor grassland ecosystem in Minnesota, USA, which showed that the structure, composition and potential activity of soil microbial communities significantly changed with the plant species diversity. As expected, GeoChip 3.0 is a high-throughput powerful tool for studying microbial community functional structure, and linking microbial communities to ecosystem processes and functioning.
Date: April 1, 2010
Creator: He, Z.; Deng, Y.; Van Nostrand, J.D.; Tu, Q.; Xu, M.; Hemme, C.L. et al.
Partner: UNT Libraries Government Documents Department

The microbial methane cycle in subsurface sediments. Final project report, July 1, 1993--August 31, 1997

Description: The objectives of this study were to determine the factors controlling microbial activity and survival in the subsurface and, specifically, to determine whether microbial communities in aquitards and in aquifer microenvironments provide electron donors and/or acceptors that enhance microbial survival in aquifers. Although the original objectives were to focus on methane cycling, the authors pursued an opportunity to study sulfur cycling in aquifer systems, a process of much greater importance in microbial activity and survival, and in the mobility of metals in the subsurface. Furthermore, sulfur cycling is pertinent to the Subsurface Science Program`s study at Cerro Negro, New Mexico. The study combined field and laboratory approaches and microbiological, molecular, geochemical, and hydrogeological techniques. During drilling operations, sediments were collected aseptically and assayed for a variety of microorganisms and metabolic capabilities including total counts, viable aerobic heterotrophs, total anaerobic heterotrophs, sulfate reducing bacteria (SRB) and sulfate reduction activity (in situ and in slurries), methanogens, methanotrophs, and Fe- and S-oxidizers, among others. Geochemical analyses of sediments included organic carbon content and {sup 13}C/{sup 12}C ratio, sulfur chemistry (reduced sulfur, sulfate), {sup 34}S/{sup 32}S, {sup 13}C/{sup 12}C, {sup 14}C, tritium, etc. The authors drilled eight boreholes in the Eocene Yegua formation at four localities on the Texas A&M University campus using a hollow-stem auger drilling rig. The drilling pattern forms a T, with three well clusters along the dip direction and two along strike. Four boreholes were sampled for sediments and screened at the deepest sand interval encountered, and four boreholes were drilled to install wells in shallower sands. Boreholes range in depth from 8 to 31 m, with screened intervals ranging from 6 to 31 m. Below are the results of these field studies.
Date: December 31, 1997
Creator: Grossman, E.L.; Ammerman, J.W. & Suflita, J.M.
Partner: UNT Libraries Government Documents Department


Description: Hybrid Sulfur cycle is gaining popularity as a possible means for massive production of hydrogen from nuclear energy. Several different ways of carrying out the SO{sub 2}-depolarized electrolysis step are being pursued by a number of researchers. These alternatives are evaluated with complete flowsheet simulations and on a common design basis using Aspen Plus{trademark}. Sensitivity analyses are performed to assess the performance potential of each configuration, and the flowsheets are optimized for energy recovery. Net thermal efficiencies are calculated for the best set of operating conditions for each flowsheet and the results compared. This will help focus attention on the most promising electrolysis alternatives. The sensitivity analyses should also help identify those features that offer the greatest potential for improvement.
Date: March 16, 2007
Creator: Gorensek, M
Partner: UNT Libraries Government Documents Department


Description: A recuperative bayonet reactor design for the high-temperature sulfuric acid decomposition step in sulfur-based thermochemical hydrogen cycles was evaluated using pinch analysis in conjunction with statistical methods. The objective was to establish the minimum energy requirement. Taking hydrogen production via alkaline electrolysis with nuclear power as the benchmark, the acid decomposition step can consume no more than 450 kJ/mol SO{sub 2} for sulfur cycles to be competitive. The lowest value of the minimum heating target, 320.9 kJ/mol SO{sub 2}, was found at the highest pressure (90 bar) and peak process temperature (900 C) considered, and at a feed concentration of 42.5 mol% H{sub 2}SO{sub 4}. This should be low enough for a practical water-splitting process, even including the additional energy required to concentrate the acid feed. Lower temperatures consistently gave higher minimum heating targets. The lowest peak process temperature that could meet the 450-kJ/mol SO{sub 2} benchmark was 750 C. If the decomposition reactor were to be heated indirectly by an advanced gas-cooled reactor heat source (50 C temperature difference between primary and secondary coolants, 25 C minimum temperature difference between the secondary coolant and the process), then sulfur cycles using this concept could be competitive with alkaline electrolysis provided the primary heat source temperature is at least 825 C. The bayonet design will not be practical if the (primary heat source) reactor outlet temperature is below 825 C.
Date: June 11, 2009
Creator: Gorensek, M. & Edwards, T.
Partner: UNT Libraries Government Documents Department

Closeout Report for Hybrid Sulfur Pressurized Button Cell Test Facility

Description: This document is the Close-Out Report for design and partial fabrication of the Pressurized Button Cell Test Facility at Savannah River National Laboratory (SRNL). This facility was planned to help develop the sulfur dioxide depolarized electrolyzer (SDE) that is a key component of the Hybrid Sulfur Cycle for generating hydrogen. The purpose of this report is to provide as much information as possible in case the decision is made to resume research. This report satisfies DOE Milestone M3GSR10VH030107.0. The HyS Cycle is a hybrid thermochemical cycle that may be used in conjunction with advanced nuclear reactors or centralized solar receivers to produce hydrogen by watersplitting. The HyS Cycle utilizes the high temperature (&gt;800 C) thermal decomposition of sulfuric acid to produce oxygen and regenerate sulfur dioxide. The unique aspect of HyS is the generation of hydrogen in a water electrolyzer that is operated under conditions where dissolved sulfur dioxide depolarizes the anodic reaction, resulting in substantial voltage reduction. Low cell voltage is essential for both high thermodynamic efficiency and low hydrogen cost. Sulfur dioxide is oxidized at the anode, producing sulfuric acid that is sent to the high temperature acid decomposition portion of the cycle. Sulfur dioxide from the decomposer is cycled back to electrolyzers. The electrolyzer cell uses the membrane electrode assembly (MEA) concept. Anode and cathode are formed by spraying a catalyst, typically platinized carbon, on both sides of a Proton Exchange Membrane (PEM). SRNL has been testing SDEs for several years including an atmospheric pressure Button Cell electrolyzer (2 cm{sup 2} active area) and an elevated temperature/pressure Single Cell electrolyzer (54.8 cm{sup 2} active area). SRNL tested 37 MEAs in the Single Cell electrolyzer facility from June 2005 until June 2009, when funding was discontinued. An important result of the final months of testing was the development ...
Date: September 15, 2010
Creator: Steeper, T.
Partner: UNT Libraries Government Documents Department

Alternations of Structure and Functional Activity of Below Ground Microbial Communities at Elevated Atmospheric Carbon Dioxide

Description: The global atmospheric concentration of CO2 has increased by more than 30percent since the industrial revolution. Although the stimulating effects of elevated CO2 (eCO2) on plant growth and primary productivity have been well studied, its influences on belowground microbial communities are poorly understood and controversial. In this study, we showed a significant change in the structure and functional potential of soil microbial communities at eCO2 in a grassland ecosystem, the BioCON (Biodiversity, CO2 and Nitrogen) experimental site (http://www.biocon.umn.edu/) using a comprehensive functional gene array, GeoChip 3.0, which contains about 28,0000 probes and covers approximately 57,000 gene variants from 292 functional gene families involved in carbon, nitrogen, phosphorus and sulfur cycles as well as other functional processes. GeoChip data indicated that the functional structure of microbial communities was markedly different between ambient CO2 (aCO2) and eCO2 by detrended correspondence analysis (DCA) of all 5001 detected functional gene probes although no significant differences were detected in the overall microbial diversity. A further analysis of 1503 detected functional genes involved in C, N, P, and S cycles showed that a considerable portion (39percent) of them were only detected under either aCO2 (14percent) or eCO2 (25percent), indicating that the functional characteristics of the microbial community were significantly altered by eCO2. Also, for those shared genes (61percent) detected, some significantly (p<0.05) changed their abundance at eCO2. Especially, genes involved in labile C degradation, such as amyA, egl, and ara for starch, cellulose, and hemicelluloses, respectively, C fixation (e.g., rbcL, pcc/acc), N fixation (nifH), and phosphorus utilization (ppx) were significantly increased under eCO2, while those involved in decomposing recalcitrant C, such as glx, lip, and mnp for lignin degradation remained unchanged. This study provides insights into our understanding of belowground microbial communities and their feedbacks to terrestrial ecosystems at eCO2.
Date: May 17, 2010
Creator: He, Zhili; Xu, Meiying; Deng, Ye; Kang, Sanghoon; Wu, Liyou; Van Nostrand, Joy D. et al.
Partner: UNT Libraries Government Documents Department

GeoChip 3.0: A High Throughput Tool for Analyzing Microbial Community, Composition, Structure, and Functional Activity

Description: Microarray-based genomic technology has been widely used for microbial community analysis, and it is expected that microarray-based genomic technologies will revolutionize the analysis of microbial community structure, function and dynamics. A new generation of functional gene arrays (GeoChip 3.0) has been developed, with 27,812 probes covering 56,990 gene variants from 292 functional gene families involved in carbon, nitrogen, phosphorus and sulfur cycles, energy metabolism, antibiotic resistance, metal resistance, and organic contaminant degradation. Those probes were derived from 2,744, 140, and 262 species for bacteria, archaea, and fungi, respectively. GeoChip 3.0 has several other distinct features, such as a common oligo reference standard (CORS) for data normalization and comparison, a software package for data management and future updating, and the gyrB gene for phylogenetic analysis. Our computational evaluation of probe specificity indicated that all designed probes had a high specificity to their corresponding targets. Also, experimental analysis with synthesized oligonucleotides and genomic DNAs showed that only 0.0036percent-0.025percent false positive rates were observed, suggesting that the designed probes are highly specific under the experimental conditions examined. In addition, GeoChip 3.0 was applied to analyze soil microbial communities in a multifactor grassland ecosystem in Minnesota, USA, which demonstrated that the structure, composition, and potential activity of soil microbial communities significantly changed with the plant species diversity. All results indicate that GeoChip 3.0 is a high throughput powerful tool for studying microbial community functional structure, and linking microbial communities to ecosystem processes and functioning. To our knowledge, GeoChip 3.0 is the most comprehensive microarrays currently available for studying microbial communities associated with geobiochemical cycling, global climate change, bioenergy, agricuture, land use, ecosystem management, environmental cleanup and restoration, bioreactor systems, and human health.
Date: May 17, 2010
Creator: He, Zhili; Deng, Ye; Nostrand, Joy Van; Tu, Qichao; Xu, Meiying; Hemme, Chris et al.
Partner: UNT Libraries Government Documents Department

Measurement of gas/water uptake coefficients for trace gases active in the marine environment

Description: Ocean produced reduced sulfur compounds including dimethylsulfide (DMS), hydrogen sulfide (H{sub 2}S), carbon disulfide (CS{sub 2}), methyl mercaptan (CH{sub 3}CH) and carbonyl sulfide (OCS) deliver a sulfur burden to the atmosphere which is roughly equal to sulfur oxides produced by fossil fuel combustion. These species and their oxidation products dimethyl sulfoxide (DMSO), dimethyl sulfone (DMSO{sub 2}) and methane sulfonic acid (MSA) dominate aerosol and CCN production in clean marine air. Furthermore, oxidation of reduced sulfur species will be strongly influenced by NO{sub x}/O{sub 3} chemistry in marine atmospheres. The multiphase chemical processes for these species must be understood in order to study the evolving role of combustion produced sulfur oxides over the oceans. We have measured the chemical and physical parameters affecting the uptake of reduced sulfur compounds, their oxidation products, ozone, and nitrogen oxides by the ocean's surface, and marine clouds, fogs, and aerosols. These parameters include: gas/surface mass accommodation coefficients; physical and chemically modified (effective) Henry's law constants; and surface and liquid phase reaction constants. These parameters are critical to understanding both the interaction of gaseous trace species with cloud and fog droplets and the deposition of trace gaseous species to dew covered, fresh water and marine surfaces.
Date: February 1, 1992
Creator: Davidovits, P. (Boston Coll., Chestnut Hill, MA (United States). Dept. of Chemistry); Worsnop, D.W.; Zahniser, M.S. & Kolb, C.E. (Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics)
Partner: UNT Libraries Government Documents Department

Can sulfate fluxes in forest canopy throughfall be used to estimate atmospheric sulfur deposition

Description: The flux of sulfate is forest throughfall and stemflow (the sum of which is designated here as TF) may be an indicator of the atmospheric deposition of S, particularly if foliar leaching of internal plant S is small relative to washoff of deposition. Extensive data from 13 forests indicate that annual sulfate fluxes in TF and in atmospheric deposition are very similar, and recent studies with {sup 35}S tracers indicate that leaching is only a few percent of total TF. However, some short-term deposition/TF comparisons show large differences, and there remain questions about interpretation of tracer results. Considering the data, we conclude that TF may be used under some conditions to estimate deposition within acceptable uncertainty limits, but that some assumptions need further testing. If TF does reflect deposition, these data suggest that commonly used methods and models seriously underestimate total S deposition at some sites. 39 refs. ,4 figs., 1 tab.
Date: January 1, 1991
Creator: Lindberg, S.E.; Garten, C.T. Jr. (Oak Ridge National Lab., TN (United States)); Cape, J.N. (Institute of Terrestrial Ecology, Edinburgh (United Kingdom)) & Ivens, W. (Rijksuniversiteit Utrecht (Netherlands))
Partner: UNT Libraries Government Documents Department

Isotope studies to determine dry deposition of sulfate to deciduous and coniferous trees: Final draft

Description: Experiments have been conducted at two locations near Oak Ridge, Tennessee, with radioactive /sup 35/S (87 day half-life) to examine the cycling behavior of sulfur in yellow poplar (Liriodendron tulipifera), red maple (Acer rubrum), and loblolly pine (Pinus taeda) trees. Some findings pertain to methods development for estimating dry deposition of sulfur to forest canopies and the magnitude of sulfur emissions from natural sources (Task II). We will determine through field studies, the internal cycling, storage, and biogenic emission of sulfur, as traced by /sup 35/SO/sub 4//sup 2 -/, in environments impacted by atmospheric sulfate deposition; and will determine through isotope dilution studies, the contribution of foliar leaching and dry deposition to net throughfall (NTF) sulfate concentrations beneath deciduous and coniferous trees in such environments. 3 refs., 2 figs., 1 tab.
Date: January 1, 1988
Creator: Garten, C.T. Jr.
Partner: UNT Libraries Government Documents Department