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PubMed2000

Development of a speciated, hourly, and gridded air pollutants emission modeling system--a case study on the precursors of photochemical smog in the Seoul metropolitan area, Korea.

A speciated, hourly, and gridded air pollutants emission modeling system (SHEMS) was developed and applied in predicting hourly nitrogen dioxide (NO2) and ozone (O3) levels in the Seoul Metropolitan Area (SMA). The primary goal of the SHEMS was to produce a systemized emission inventory for air pollutants including ozone precursors for modeling air quality in urban areas. The SHEMS is principally composed of three parts: (1) a pre-processor to process emission factors, activity levels, and spatial and temporal information using a geographical information system; (2) an emission model for each source type; and (3) a post-processor to produce report and input data for air quality models through database modeling. The source categories in SHEMS are point, area, mobile, natural, and other sources such as fugitive emissions. The emission database produced by SHEMS contains 22 inventoried compounds: sulfur dioxide, NO2, carbon monoxide, and 19 speciated volatile organic compounds. To validate SHEMS, the emission data were tested with the Urban Airshed Model to predict NO2 and O3 concentrations in the SMA during selected episode days in 1994. The results turned out to be reliable in describing temporal variation and spatial distribution of those pollutants.

Air Pollutants↗
PubMed2006

A systematic resolution of sulfur in reticulated vitreous carbon using X-ray absorption spectroscopy.

Sulfur K-edge X-ray absorption spectroscopy (XAS) was used to characterize the approximately 0.1% sulfur found both in native reticulated vitreous carbon (RVC) foam and in RVC oxidatively modified using 0.2 M KMnO4 in 2 M H2SO4. Sulfur valences and functional groups were assessed using K-edge XAS spectral curve-fitting and employing explicit sulfur compounds as models. For native RVC, these were episulfide (approximately 3%), thianthrene (approximately 9%), disulfide (approximately 10%), sulfenate ester (approximately 12%), benzothiophene (approximately 24%), N,N'-thiobisphthalimide (approximately 30%), alkyl sulfonate (approximately 1.2%), alkyl sulfate monoester (approximately 6%), and sulfate dianion (approximately 6%). Permanganate oxidation of RVC diminished sulfenic sulfur to approximately 9%, thianthrenic sulfur to approximately 7%, and sulfate dianion to approximately 1% but increased sulfate monoester to approximately 12%, and newly produced sulfone (approximately 2%) and sulfate diester (approximately 5%). A simple thermodynamic model was derived that allows proportionate functional group comparisons despite differing (approximately +/-15%) total sulfur contents between RVC batches. The limits of accuracy in the XAS curve-fitting analysis are discussed in terms of microenvironments and extended structures in RVC carbon that cannot be exactly modeled by small molecules. Sulfate esters cover approximately 0.15% of the RVC surface, increasing to approximately 0.51% following permanganate/sulfuric acid treatment. The detection of episulfide directly corroborates a proposed mechanism for the migration of elemental sulfur through carbon.

Absorption↗
PubMed2005

Characteristics of sulfur response in a micro-flame photometric detector.

A recently reported micro-flame photometric detector (microFPD) has been examined in greater detail for its sulfur response characteristics. While supporting an "upside down" flame on a stainless steel capillary burner (delivering oxygen) in a counter flowing stream of premixed hydrogen and oxygen, the extremely small flame of the muFPD (30 nL) was observed to produce linear sulfur emission as HSO(*). In this mode, linear sulfur response was obtained over four orders of magnitude with a minimum detectable flow of 2 x 10(-10) g S/s. Additionally, a broad series of sulfur compounds ranging in chemical structure were examined in the microFPD in order to determine the extent of equimolarity and reproducibility of response toward this element. Results of exploring both the linear (HSO(*)) and quadratic (S(2)(*)) modes indicate that the %RSD and equimolarity of sulfur response are comparable between that of the microFPD and a conventional flame photometric detector (FPD).

Microchemistry↗
PubMed2000

Microbiology of acidic, geothermal springs of Montserrat: environmental rDNA analysis.

DNA was extracted from water and sediment samples taken from acidic, geothermal pools on the Caribbean island of Montserrat. 16S rRNA genes were amplified by PCR, cloned, sequenced, and examined to indicate some of the organisms that might be significant components of the in situ microbiota. A clone bank representing the lowest temperature pool that was sampled (33 degrees C) was dominated by genes corresponding to two types of acidophiles: Acidiphilium-like mesophilic heterotrophs and thermotolerant Acidithiobacillus caldus. Three clone types with origins in low- and moderate- (48 degrees C) temperature pools corresponded to bacteria that could be involved in metabolism of sulfur compounds: the aerobic A. caldus and putative anaerobic, moderately thermophilic, sulfur-reducing bacteria (from an undescribed genus and from the Desulfurella group). A higher-temperature sample indicated the presence of a Ferroplasma-like organism, distinct from the other strains of these recently recognized acidophilic, iron-oxidizing members of the Euryarchaeota. Acidophilic Archaea from undescribed genera related to Sulfolobus and Acidianus were predicted to dominate the indigenous acidophilic archaeal population at the highest temperatures.

Acetobacteraceae↗
PubMed2003

Structure and catalytic properties of nanosized alumina supported platinum and palladium particles synthesized by reaction in microemulsion.

Mixtures of nanosized platinum and palladium particles have been prepared by reduction of salt-containing microemulsion droplets using hydrazine as the reducing agent. To avoid possible negative effects of the presence of sulfur compounds during the preparation the microemulsion was made using the sulfur-free nonionic polyoxyethylene 4 lauryl ether surfactant. Transmission electron microscopy showed that the as-prepared mixtures contained crystalline platinum particles of fairly homogeneous size (20 to 40 nm) with adsorbed amorphous palladium particles 2 to 5 nm in size. Catalyst samples were prepared by depositing the nanoparticles on a gamma-Al(2)O(3) support followed by heating in air at 600 degrees C. Alloyed particles of platinum and palladium with sizes ranging from 5 to 80 nm were obtained during the heating. The majority of the particles had the fcc structure and their compositional range was dependent upon the Pt:Pd molar ratio of the microemulsion. A catalyst prepared from a microemulsion with a 20:80 Pt:Pd molar ratio showed the highest catalytic activity for CO oxidation, while pure platinum and palladium catalysts showed higher sulfur resistance. These results differ from the performance of conventional wet-impregnated catalysts, where a 50:50 Pt:Pd molar ratio resulted in the highest catalytic activity as well as the highest sulfur resistance.

Journal Article↗
PubMed2005

Enzymatic and genetic characterization of carbon and energy metabolisms by deep-sea hydrothermal chemolithoautotrophic isolates of Epsilonproteobacteria.

The carbon and energy metabolisms of a variety of cultured chemolithoautotrophic Epsilonproteobacteria from deep-sea hydrothermal environments were characterized by both enzymatic and genetic analyses. All the Epsilonproteobacteria tested had all three key reductive tricarboxylic acid (rTCA) cycle enzymatic activities--ATP-dependent citrate lyase, pyruvate:ferredoxin oxidoreductase, and 2-oxoglutarate:ferredoxin oxidoreductase--while they had no ribulose 1,5-bisphosphate carboxylase (RubisCO) activity, the key enzyme in the Calvin-Benson cycle. These results paralleled the successful amplification of the key rTCA cycle genes aclB, porAB, and oorAB and the lack of success at amplifying the form I and II RubisCO genes, cbbL and cbbM. The combination of enzymatic and genetic analyses demonstrates that the Epsilonproteobacteria tested use the rTCA cycle for carbon assimilation. The energy metabolisms of deep-sea Epsilonproteobacteria were also well specified by the enzymatic and genetic characterization: hydrogen-oxidizing strains had evident soluble acceptor:methyl viologen hydrogenase activity and hydrogen uptake hydrogenase genes (hyn operon), while sulfur-oxidizing strains lacked both the enzyme activity and the genes. Although the energy metabolism of reduced sulfur compounds was not genetically analyzed and was not fully clarified, sulfur-oxidizing Epsilonproteobacteria showed enzyme activity of a potential sulfite:acceptor oxidoreductase for a direct oxidation pathway to sulfate but no activity of AMP-dependent adenosine 5'-phosphate sulfate reductase for a indirect oxidation pathway. No activity of thiosulfate-oxidizing enzymes was detected. The enzymatic and genetic characteristics described here were consistent with cellular carbon and energy metabolisms and suggest that molecular tools may have great potential for in situ elucidation of the ecophysiological roles of deep-sea Epsilonproteobacteria.

Bacterial Proteins↗
PubMed2004

Determination of vanadium in heavy oils by atomic absorption spectrometry using a graphite furnace coated with tungsten.

A simple and rapid method was established for the direct determination of vanadium in an oil sample using the tungsten-coated graphite-furnace AAS. The interference of the sulfur compound could be suppressed by choosing the ashing temperature. If the sulfur concentration in the sample is diluted to 1.0 wt% or less, the interference can be suppressed. This proposed method should make important contributions to the quality control of petroleum refineries.

Journal Article↗
PubMed2001

Dissociation of sulfur hexafluoride tracer gas in the presence of an indoor combustion source.

As an odorless, nontoxic, and inert compound, sulfur hexafluoride (SF6) is one of the most widely used tracer gases in indoor air quality studies in both controlled and uncontrolled environments. This compound may be subject to reactions with water vapor under elevated temperature to form acidic inorganic compounds such as HF and H2SO4. Thus, in the presence of unvented combustion sources such as kerosene heaters, natural gas heaters, gas log fireplaces, candles, and lamps, the SF6 dissociation may interfere with measurements of the emissions from these sources. Tests were conducted in a research house with a vent-free natural gas heater to investigate these potential interferences. It was observed that the heater operation caused about a 5% reduction of SF6 concentration, which can be an error source for the ventilation rate measurement and consequently the estimated pollutant emission rates. Further analysis indicates that this error can be much greater than the observed 5% under certain test conditions because it is a function of the ventilation flow rate. Reducing the tracer gas concentration has no effect on this error. A simple theoretical model is proposed to estimate the magnitude of this error. The second type of interference comes from the primary and secondary products of the SF6 dissociation, mainly H2SO4, SO2, HF, and fine particulate matter (PM). In the presence of approximately 5 ppm SF6, the total airborne concentrations of these species increased by a factor of 4-10. The tests were performed at relatively high SF6 concentrations, which is necessary to determine the interferences quantitatively. The second type of interference can be significantly reduced if the SF6 concentration is kept at a low ppb level.

Air Movements↗
PubMed2006

Solid-phase microextraction in the analysis of food taints and off-flavors.

Selected food taints and off flavors, for which solid phase microextraction (SPME) has been used as a method for volatiles isolation, are the subject of review. Compounds responsible for musty and earthy odor off-flavors and taints in foods are discussed. This group contains haloanisoles, geosmin, and methylisoborneol. Chlorophenols are discussed as precursors of chloroanisoles and compounds impairing the flavor of food. Also described are volatile phenolic compounds responsible for medicinal off flavors, mainly ethyl phenols and vinyl phenols. Sulfur compounds that contribute to off-flavor are also discussed. Finally, a group of volatile compounds being the products of lipid oxidation are summarized. A short review of the formation, occurrence, and information on odor properties of all of these groups of compounds is given. Examples of SPME use for the analysis of compounds belonging to all described groups are shown. Elaboration of method parameters, fiber selection, experimental conditions, and quantitation of compounds are subjects of interest. Also, applications of SPME as a method for introduction of volatiles in mechanical olfaction technologies are shortly outlined.

Food Analysis↗
PubMed1985

Control of Oxidative Sulfur Metabolism of Chlorobium limicola forma thiosulfatophilum.

A metered blend of anaerobic-grade N(2), CO(2), and H(2)S gases was introduced into an illuminated, 800-ml liquid volume, continuously stirred tank reactor. The system, described as an anaerobic gas-to-liquid phase fed-batch reactor, was used to investigate the effects of H(2)S flow rate and light energy on the accumulation of oxidized sulfur compounds formed by the photoautotroph Chlorobium limicola forma thiosulfatophilum during growth. Elemental sulfur was formed and accumulated in stoichiometric quantities when light energy and H(2)S molar flow rate levels were optimally adjusted in the presence of nonlimiting CO(2). Deviation from the optimal H(2)S and light energy levels resulted in either oxidation of sulfur or complete inhibition of sulfide oxidation. Based on these observations, a model of sulfide and sulfur oxidases electrochemically coupled to the photosynthetic reaction center of Chlorobium spp. is presented. The dynamic deregulation of oxidative pathways may be a mechanism for supplying the photosynthetic reaction center with a continuous source of electrons during periods of varying light and substrate availability, as in pond ecosystems where Chlorobium spp. are found. Possible applications for a sulfide gas removal process are discussed.

Journal Article↗
PubMed2006

Microbial desulfurization of gasoline by free whole-cells of Rhodococcus erythropolis XP.

Rhodococcus erythropolis XP could grow well with condensed thiophenes, mono-thiophenic compounds and mercaptans present in gasoline. Rhodococcus erythropolis XP was also capable of efficiently degrading the condensed thiophenes in resting cell as well as biphasic reactions in which n-octane served as a model oil phase. Free whole cells of R. erythropolis XP were adopted to desulfurize fluid catalytic cracking (FCC) and straight-run (SR) gasoline oils. About 30% of the sulfur content of FCC gasoline and 85% of sulfur in SR gasoline were reduced, respectively. Gas chromatography analysis with atomic emission detection also showed depletion of sulfur compounds in SR gasoline. Rhodococcus erythropolis XP could partly resist the toxicity of gasoline and had an application potential to biodesulfurization of gasoline.

Biodegradation, Environmental↗
PubMed2006

Structural study of two proteins SigE and ORF1 to predict their roles in the biochemical oxidation of sulfur anions via the global sulfur oxidation operon (sox).

Microbial redox reactions involving inorganic sulfur compounds in the environment are one of the major reactions of the global sulfur cycle. These reactions are mediated by phylogenetically diverse prokaryotes containing the sulfur oxidizing gene cluster (sox). The sox gene cluster of alpha-Proteobacteria comprises of at least 15 genes, which form two transcriptional units. Recently two new orfs, which code for proteins named, SigE and ORF1, were identified in Starkeya novella. Sequence analyses reveal that SigE protein has the signature sequence of ECF-type sigma factors and a helix-turn-helix (HTH) DNA binding motif whereas ORF1 is possibly an anti ECF-sigma factor, which also has the signature sequence of the dsr family of sulfate ion binding proteins. We employed homology modeling to construct the three-dimensional structures of these proteins. The model of SigE was docked on to its promoter DNA to investigate the favourable binding modes of the protein. Interactions of SigE with its anti-sigma factor ORF1 were also reported after docking these proteins. We also identified the putative sulfate ion binding residues of ORF1 by docking sulfate ion on to it. Our study provides a rational framework for understanding of the structural as well as the molecular basis of the mechanism of the regulation of sulfur oxidation reactions by SigE and ORF1 proteins via the sox operon.

Anions↗
PubMed2002

Generation of Maillard compounds from inulin during the thermal processing of Agave tequilana Weber Var. azul.

During the cooking process of Agave tequilana Weber var. azul to produce tequila, besides the hydrolysis of inulin to generate fermentable sugars, many volatiles, mainly Maillard compounds, are produced, most of which may have a significant impact on the overall flavor of tequila. Exudates (agave juice) from a tequila company were collected periodically, and color, Brix, fructose concentration, and reducing sugars were determined as inulin breakdown took place. Maillard compounds were obtained by extraction with CH(2)Cl(2), and the extracts were analyzed by GC-MS. Increments in color, Brix, and reducing sugars were observed as a function of time, but a decrease in fructose concentration was found. Many Maillard compounds were identified in the exudates, including furans, pyrans, aldehydes, and nitrogen and sulfur compounds. The most abundant Maillard compounds were methyl-2-furoate, 2,3-dihydroxy-3,5-dihydro-6-methyl-4(H)-pyran-4-one, and 5-(hydroxymethyl)furfural. In addition, a series of short- and long-chain fatty acids was also found. A large number of the volatiles in A. tequilana Weber var. azul were also detected in tequila extracts, and most of these have been reported as a powerful odorants, responsible for the unique tequila flavor.

Agave↗
PubMed2002

Effect of cultivar and storage time on the volatile flavor components of baked potato.

Tubers of five cultivars of potato were stored at 4 degrees C for 2, 3, and 8 months and baked in a conventional oven. The flavor compounds from the baked potato flesh were isolated by headspace adsorption onto Tenax and analyzed by gas chromatography-mass spectrometry. On a quantitative basis, compounds derived from lipid and Maillard reaction/sugar degradation dominated the flavor isolates, with sulfur compounds, methoxypyrazines, and terpenes making smaller contributions. Levels of 37 of the >150 detected compounds were monitored in each cultivar with time of storage. Many significant differences were found in levels of individual compounds, compound classes, and total monitored compounds for the individual effects of cultivar and storage time and for their two-way interaction. Differences may be explained by variations in levels of flavor precursors and activities of enzymes mediating flavor compound formation among cultivars and storage times. In addition, differences in agronomic conditions may partly account for variations among cultivars. Overall, of the compounds monitored, those most likely having the greatest flavor impact were 2-isopropyl-3-methyoxypyrazine, 2-isobutyl-3-methoxypyrazine, dimethyl trisulfide, decanal, and 3-methylbutanal, with methylpropanal, 2-methylbutanal, methional, and nonanal also being probable important contributors to flavor.

Food Preservation↗
PubMed2005

Homology modeling of a transcriptional regulator SoxR of the Lithotrophic sulfur oxidation (Sox) operon in alpha-proteobacteria.

Microbial oxidation of reduced inorganic sulfur compounds in the environment is one of the major reactions of the global sulfur cycle mediated by phylogenetically diverse prokaryotes. The sulfur oxidizing gene cluster (sox) of alpha-Proteobacteria comprises of at least 15 genes, which form two transcriptional units, viz soxSRT and soxVWXYZABCDEFGH. Sequence analysis reveals that SoxR belongs to the ArsR family of helix-turn-helix DNA binding proteins. Although SoxR proteins do not contain the conserved metal-binding box, ELCVCDL, but there are a number of well conserved residues present throughout the sequence that are previously identified in the known ArsR family proteins. We employed homology modeling to construct the three-dimensional structure of the SoxR from chemolithotrophic alpha-Proteobacteria Pseudaminobacter salicylatoxidans KCT001. The predicted homology model of SoxR shows an overall structural similarity with winged helix-turn-helix family proteins. Since dimerization is essential for DNA binding and repression by the ArsR family proteins we have generated the dimeric model of SoxR that enables us to predict the DNA binding residues of the protein as well as the interaction of SoxR with the predicted promoter region of sox gene cluster.

Alphaproteobacteria↗
PubMed2000

Novel bacterial and archaeal lineages from an in situ growth chamber deployed at a Mid-Atlantic Ridge hydrothermal vent.

The phylogenetic diversity was determined for a microbial community obtained from an in situ growth chamber placed on a deep-sea hydrothermal vent on the Mid-Atlantic Ridge (23 degrees 22' N, 44 degrees 57' W). The chamber was deployed for 5 days, and the temperature within the chamber gradually decreased from 70 to 20 degrees C. Upon retrieval of the chamber, the DNA was extracted and the small-subunit rRNA genes (16S rDNA) were amplified by PCR using primers specific for the Archaea or Bacteria domain and cloned. Unique rDNA sequences were identified by restriction fragment length polymorphisms, and 38 different archaeal and bacterial phylotypes were identified from the 85 clones screened. The majority of the archaeal sequences were affiliated with the Thermococcales (71%) and Archaeoglobales (22%) orders. A sequence belonging to the Thermoplasmales confirms that thermoacidophiles may have escaped enrichment culturing attempts of deep-sea hydrothermal vent samples. Additional sequences that represented deeply rooted lineages in the low-temperature eurarchaeal (marine group II) and crenarchaeal clades were obtained. The majority of the bacterial sequences obtained were restricted to the Aquificales (18%), the epsilon subclass of the Proteobacteria (epsilon-Proteobacteria) (40%), and the genus Desulfurobacterium (25%). Most of the clones (28%) were confined to a monophyletic clade within the epsilon-Proteobacteria with no known close relatives. The prevalence of clones related to thermophilic microbes that use hydrogen as an electron donor and sulfur compounds (S(0), SO(4), thiosulfate) indicates the importance of hydrogen oxidation and sulfur metabolism at deep-sea hydrothermal vents. The presence of sequences that are related to sequences from hyperthermophiles, moderate thermophiles, and mesophiles suggests that the diversity obtained from this analysis may reflect the microbial succession that occurred in response to the shift in temperature and possible associated changes in the chemistry of the hydrothermal fluid.

Archaea↗
PubMed2001

Volatile flavour components of baked potato flesh. A comparison of eleven potato cultivars.

Tubers of eleven cultivars of potato were baked and the flavour compounds from the flesh were isolated by headspace adsorption onto Tenax and analysed by gas chromatography-mass spectrometry (GC-MS). Lipid degradation and the Maillard reaction were the main sources of flavour compounds, accounting for 22-69% and 28-77%, respectively, of the total yields. Various sulfur compounds, methoxypyrazines and terpenes were also identified at lower levels. Relative aroma impact values (RAVs) were calculated by dividing compound yields by the odour threshold value. Compounds contributing most to aroma (RAV > 10,000 in at least one cultivar) were 2-isobutyl-3-methoxypyrazine, 2-isopropyl-3-methoxypyrazine, beta-damascenone, dimethyl trisulfide, decanal and 3-methylbutanal. The observed differences in yields and RAVs for compounds among cultivars would be expected to result in differences in perceived flavour.

Cooking↗
PubMed1987

A large reservoir of sulfate and sulfonate resides within plasma cells from Ascidia ceratodes, revealed by X-ray absorption near-edge structure spectroscopy.

The study of sulfur within the plasma cells of Ascidia ceratodes [Carlson, R. M. K. (1975) Proc. Natl. Acad. Sci. U.S.A. 72, 2217-2221; Frank, P., Carlson, R. M. K., & Hodgson, K. O. (1986) Inorg. Chem. 25, 470-478; Hedman, B., Frank, P., Penner-Hahn, J. E., Roe, A. L., Hodgson, K. O., Carlson, R. M. K., Brown, G., Cerino, J., Hettel, R., Troxel, T., Winick, H., & Yang, J. (1986) Nucl. Instrum. Methods Phys. Res., Sect. A 246, 797-800] has been extended with X-ray absorption near-edge structure (XANES) spectroscopy. An intense absorption feature at 2482.4 eV and a second feature at 2473.7 eV indicate a large endogenous sulfate concentration, as well as smaller though significant amounts of thiol or thioether sulfur, respectively. A strong shoulder was observed at 2481.7 eV on the low-energy side of the sulfate absorption edge, deriving from a novel type of sulfur having a slightly lower oxidation state than sulfate sulfur. The line width of the primary transition on the sulfur edge of a vanadium (III) sulfate solution was found to be broadened relative to that of sodium sulfate, possibly deriving from the formation of the VSO4+ complex ion [Britton, H. T. S., & Welford, G. (1940) J. Chem. Soc., 761-764; Duffy, J. A., & Macdonald, W. J. D. (1970) J. Chem. Soc., 977-980; Kimura, T., Morinaga, M., & Nakano, J. (1972) Nippon Kagaku Zaishi, 664-667]. Similar broadening appears to characterize the oxidized sulfur types in vanadocytes. A very good linear correlation between oxidation state and peak position (in electronvolts) was found for a series of related sulfur compounds. This correlation was used to determine a 5+ oxidation state for the additional sulfur type at 2481.7 eV. (ABSTRACT TRUNCATED AT 250 WORDS)

Animals↗