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PubMed2006

Renewable hydrogen from nonvolatile fuels by reactive flash volatilization.

Droplets of nonvolatile fuels such as soy oil and glucose-water solutions can be flash evaporated by catalytic partial oxidation to produce hydrogen in high yields with a total time in the reactor of less than 50 milliseconds. Pyrolysis, coupled with catalytic oxidation of the fuels and their fragments upon impact with a hot rhodium-cerium catalyst surface, avoids the formation of deactivating carbon layers on the catalyst. The catalytic reactions of these products generate approximately 1 megawatt of heat per square meter, which maintains the catalyst surface above 800 degrees C at high drop impact rates. At these temperatures, heavy fuels can be catalytically transformed directly into hydrogen, carbon monoxide, and other small molecules in very short contact times without the formation of carbon.

Journal Article↗
PubMed1990

Cometary delivery of organic molecules to the early Earth.

It has long been speculated that Earth accreted prebiotic organic molecules important for the origins of life from impacts of carbonaceous asteroids and comets during the period of heavy bombardment 4.5 x 10(9) to 3.8 x 10(9) years ago. A comprehensive treatment of comet-asteroid interaction with the atmosphere, surface impact, and resulting organic pyrolysis demonstrates that organics will not survive impacts at velocities greater than about 10 kilometers per second and that even comets and asteroids as small as 100 meters in radius cannot be aerobraked to below this velocity in 1-bar atmospheres. However, for plausible dense (10-bar carbon dioxide) early atmospheres, we find that 4.5 x 10(9) years ago Earth was accreting intact cometary organics at a rate of at least approximately 10(6) to 10(7) kilograms per year, a flux that thereafter declined with a half-life of approximately 10(8) years. These results may be put in context by comparison with terrestrial oceanic and total biomasses, approximately 3 x 10(12) kilograms and approximately 6 x 10(14) kilograms, respectively.

Amino Acids↗
PubMed1974

Choline content of rat brain.

The free choline concentration in the rat brain was found to be 26.3 nanomoles per gram of brain tissue. This value was obtained through use of 6-second microwave irradiation for killing animals and inactivating enzymes, followed by a pyrolysis-gas chromatographic assay procedure. The identities of compounds measured from brain samples were verified by mass spectrometry.

Acetylcholine↗
PubMed1999

Ultrasonic deposition of high-selectivity nanoporous carbon membranes

Ultrasonic deposition creates a thin film of polymer on a tubular, macroporous, stainless steel support. Using polyfurfuryl alcohol as the nanoporous carbon precursor and a pyrolysis temperature of 723 kelvin, a membrane was prepared with the following permeances, measured in moles per square meter per Pascal per second: nitrogen, 1.8 x 10(-12); oxygen, 5.6 x 10(-11); helium, 3.3 x 10(-10); and hydrogen, 6.1 x 10(-10). The ideal separation factors as compared to that for nitrogen are 30:1, 178:1, and 331:1 for oxygen, helium, and hydrogen, respectively.

Journal Article↗
PubMed1978

Formation of mutagens in beef and beef extract during cooking.

Mutagens, distinguishable from benzo[a]pyrene and from mutagenic amino acid and protein pyrolysis products, are formed when ground beef is cooked in a home hamburger cooking appliance or when beef stock is concentrated, by boiling, to a paste known commercially as beef extract. "Well-done" hamburgers contain about 0.14 part per million of the mutagens, and beef bouillon cubes which contain beef extract about 0.1 part per million. Since such mutagens may be potentially carcionogenic and are formed during ordinary cooking procedures, their occurrence raises questions about possible risks to human health.

Animals↗
PubMed1985

Characterization of bacteria by particle beam mass spectrometry.

A technique is described for detecting and characterizing bacteria on a single-particle basis by mass spectrometry. The method involves generation of a particle beam of single whole cells which are rapidly volatilized and ionized in vacuum in the ion source of a quadrupole mass spectrometer. The particle beam can be generated, with minimal sample handling, from a naturally occurring aerosol or from a solution of bacteria that can be dispersed as an aerosol. The mass spectrum is generated by successively measuring the average intensities of different mass peaks. The average intensity is obtained by measuring the ion intensity distribution at the particular mass (m/e) for ion pulses from more than 1,000 bacteria particles. Bacillus cereus, Bacillus subtilis, and Pseudomonas putida samples were analyzed to test the capability of the instrument for differentiating among species of bacteria. Significant ion-intensity information was produced over the m/e range of 50 to 300, an improvement over previous pyrolysis-mass spectrometry results. The complex mass spectra contained a few unique peaks which could be used for the differentiation of the bacteria. A statistical analysis of the variations in peak intensities among the three bacteria provided a quantitative measure of the reproducibility of the instrument and its ability to differentiate among bacteria. The technique could lead to a new rapid method for the analysis of microorganisms and could be used for the detection of airborne pathogens on a continuous, real-time basis.

Journal Article↗
PubMed1990

Pyrolytic methylation-gas chromatography of whole bacterial cells for rapid profiling of cellular Fatty acids.

A novel, on-line derivatization technique has been developed which enables generation of fatty acid methyl ester (FAME) profiles from microorganisms by gas chromatography-mass spectrometry without the need for laborious and time-consuming sample preparation. Microgram amounts of bacterial cells are directly applied to a thin ferromagnetic filament and covered with a single drop of methanolic solution of tetramethylammonium hydroxide. After air drying, the filament is inserted into a special gas chromatograph inlet equipped with a high-frequency coil, thus enabling rapid inductive heating of the ferromagnetic filament. This so-called Curie-point heating technique is shown to produce patterns of bacterial FAMEs which are qualitatively and quantitatively nearly identical to those obtained from extracts of methylated lipids prepared by conventional sample pretreatment methods. Relatively minor differences involve the loss of hydroxy-substituted fatty acids by the pyrolytic approach as well as strongly enhanced signals of FAMEs derived from mycolic acids. This type of pyrolysis enables on-line derivatization and thermal extraction of volatile derivatives for analysis, whereas the residual components remain on a disposable probe (ferromagnetic wire) of a pyrolytic device. The reduced sample size (micrograms instead of milligrams) and the lack of sample preparation requirements open up the possibility of rapid microbiological identification of single colonies (thus overcoming the need for time-consuming subculturing) as well as analysis of FAME profiles directly from complex environmental samples.

Journal Article↗
PubMed1994

Preferential degradation of phenolic lignin units by two white rot fungi.

The differential biodegradation of phenolic and nonphenolic (C-4-etherified) lignin units in wheat straw treated with the white rot fungi Pleurotus eryngii and Phanerochaete chrysosporium was investigated under solid-state fermentation conditions. Two analytical techniques applied to permethylated straw were used for this purpose, i.e., alkaline CuO degradation and analytical pyrolysis (both followed by gas chromatography-mass spectrometry for product identification). Despite differences in the enzymatic machinery produced, both ligninolytic fungi caused a significant decrease in the relative amount of phenolic lignin units during the degradation process. Nevertheless, no differences in the biodegradation rates of phenolic and etherified cinnamic acids were observed. Changes in lignin composition and cinnamic acid content were also analyzed in the phenolic and nonphenolic lignin moieties. The results obtained are discussed in the context of the enzymatic mechanisms of lignin biodegradation.

Basidiomycota↗
PubMed1996

Analysis of Lignin-Polysaccharide Complexes Formed during Grass Lignin Degradation by Cultures of Pleurotus Species.

A brown material, precipitable with ethanol, was formed during wheat straw and lignin degradation by liquid cultures of different species of Pleurotus. Fourier transform infrared spectroscopy and cross-polarization and magic-angle-spinning (sup13)C nuclear magnetic resonance spectroscopy showed that most of the precipitable material was formed from exopolysaccharide secreted by the fungus but it also contained an aromatic fraction. The results of acid hydrolysis, methylation analysis, and Smith degradation indicated that the major exopolysaccharide produced by these fungi is a (1(symbl)3)-(beta)-glucan branched at C-6 every two or three residues along the main chain. The presence of lignin or straw in the culture medium had little effect on the composition and structure of the extracellular polysaccharide. Cross-polarization and magic-angle-spinning (sup13)C nuclear magnetic resonance spectroscopy provided an estimation of the aromatic content of the lignin-polysaccharide complexes, assigning 20% of the total (sup13)C signal in the material recovered from cultures of Pleurotus eryngii in lignin medium to aromatic carbon. Analytical pyrolysis indicated that the aromatic fractions of the lignin-polysaccharide complexes were derived from lignin, since products characteristic of pyrolytic breakdown of H (p-hydroxyphenylpropane), G (guaiacylpropane), and S (syringylpropane) lignin units were identified. These complexes cannot be fractionated by treatment with polyvinylpyrrolidone or extraction with lignin solvents, suggesting that the two polymers were chemically linked. Moreover, differences in composition with respect to the original lignin indicated that this macromolecule was modified by the fungi during the process of formation of the lignin-polysaccharide complexes.

Journal Article↗
PubMed1970

Measurement of CO(2) Assimilation in Soils: an Experiment for the Biological Exploration of Mars.

A method is described for the measurement of CO(2) assimilation by microorganisms in soils. A determination involves exposing soil to CO(2), pyrolyzing the exposed soil, trapping the organic pyrolysis products on a column of firebrick coated with CuO, combusting the trapped organics by heating, and measuring the radioactivity in the CO(2) produced in the combustion. The detection of significant levels of C in the trapped organic fraction appears to be an unambiguous indication of biological activity. The CO(2) which is adsorbed or exchanged into soils by nonbiological processes does not interfere. The method easily detects the CO(2) fixed by 10 to 10 algae after light exposure for 3 to 24 hr. Assimilation of C is also demonstrable in dark-exposed soils containing 10 to 10 heterotrophic bacteria. Possible applications of the method in the biological exploration of Mars are discussed.

Journal Article↗
PubMed1972

Separation of prodigiosenes and identification as prodigiosin syntrophic pigment from mutant pairs of Serratia marcescens.

Countercurrent distribution is capable of resolving mixtures of closely related prodigiosene pigments. Syntrophic pigment produced by several pairs of Serratia marcescens color mutants was identified as prodigiosin (2-methyl-3-amyl-6-methoxyprodigiosene) by countercurrent distribution, soda lime pyrolysis, and other techniques. The metabolic block of mutant strain H-462, derived from parent strain HY, was located between the blocks of mutant strains OF and WF, both derived from parent strain Nima.

Bacteriological Techniques↗
PubMed1975

Basis for the resistance of several algae to microbial decomposition.

The basis for the resistance of certain algae to microbial decomposition in natural waters was investigated using Pediastrum duplex, Staurastrum sp., and Fischerella muscicola as test organisms. Enzyme preparations previously found to convert susceptible algae into spheroplasts had no such effect on the resistant species, although glucose and galacturonic acid was released from P. duplex walls. Little protein or lipid but considerable carbohydrate was found in the walls of the refractory organisms, but resistance was not correlated with the presence of a unique sugar monomer. A substance present in Staurastrum sp. walls was characterized as lignin or lignin-like on the basis of its extraction characteristics, infrared spectrum, pyrolysis pattern, and content of an aromatic building block. Sporopollenin was found in P. duplex, and cellulose in Staurastrum sp. Cell walls of the algae were fractionated, and the fractions least susceptible to microbial degradation were the sporopollenin of P. duplex, the polyaromatic component of Staurastrum sp., and two F. muscicola fractions containing several sugar monomers. The sporopollenin content of P. duplex, the content of lignin or a related constituent of Staurastrum sp., and the resistance of the algae to microbial attack increased with age. It is suggested that resistance results from the presence of sporopollenin in P. duplex, a lignin-like material in Staurastrum sp., and possibly heteropolysaccharides in F. muscicola.

Bacteria↗
PubMed1983

Preparation and physicochemical and immunological characterization of polysaccharide-outer membrane protein complexes of Neisseria meningitidis.

A crude complex containing group C polysaccharide, outer membrane proteins, and lipopolysaccharide (LPS) was isolated from the cell-free culture liquid of Neisseria meningitidis serogroup C, serotype 2a. Group C polysaccharide and LPS were removed from this complex, resulting in an outer membrane complex and a purified complex, respectively. Analysis by electron microscopy showed the outer membrane origin of the crude complex and the outer membrane complex, whereas such a structure was absent in the purified complex. Sodium dodecyl sulfate-polyacrylamide gel electrophoresis patterns of the three complexes were identical. Pyrolysis-mass spectrometry data correlated well with those obtained by the biochemical assays and suggested a low LPS content in the purified complex and a low polysaccharide content in the outer membrane complex. The purified complex was shown to be nonpyrogenic and could be prepared with the same yield as that of purified polysaccharide. The immunogenic activities of the complexes were studied in mice. The antibodies were measured by the enzyme-linked immunosorbent assay; and the bactericidal antibody assay. All complexes induced immunoglobulin G antibodies to group C polysaccharide as well as to the serotype antigen, although the removal of polysaccharide and LPS resulted in a reduction of the immunogenic activities of outer membrane complex and purified complex, respectively. A second dose of all complexes produced a clear booster effect of both antibody responses. The antibodies were bactericidal.

Animals↗
PubMed1999

DNA banding pattern polymorphism in vancomycin-resistant Enterococcus faecium and criteria for defining strains.

The degree of DNA banding pattern polymorphism exhibited by vancomycin-resistant Enterococcus faecium (VREM) strains isolated on a renal unit over an 11-month period was investigated. Thirty VREM strains from different patients were analyzed by pulsed-field gel electrophoresis (PFGE; with extended run and optimal pulse times), ribotyping, plasmid profile analysis, biotyping, pyrolysis mass spectrometry, and antibiogram analysis. PFGE resolved 17 banding patterns which formed four distinct clusters at the 82% similarity level. Intercluster band differences ranged from 14 to 31 bands. The strains in one cluster, which contained seven patterns that differed from each other by one to seven bands and from the common pattern by five bands, were confirmed to be a single strain by four of the five other typing methods. The strains in a second cluster with eight patterns, which differed from each other by 1 to 12 bands, contained two subclusters. This subdivision was supported by ribotyping and biotyping. However, it was unclear whether these subclusters represented distinct strains. In one strain, marked polymorphism (patterns that differed from each other by up to four bands) was observed in the ribotype pattern. This study demonstrates the high degree of DNA banding pattern polymorphism found for some strains of VREM and illustrates the complexity involved in defining such strains.

Anti-Bacterial Agents↗
PubMed1984

Respiratory exposures associated with silicon carbide production: estimation of cumulative exposures for an epidemiological study.

Silicon carbide is produced by heating a mixture of petroleum coke and silica sand to approximately 2000 degrees C in an electric furnace for 36 hours. During heating, large amounts of carbon monoxide are released, sulphur dioxide is produced from residual sulphur in the coke, and hydrocarbon fume is produced by pyrolysis of the coke. Loading and unloading furnaces causes exposures to respirable dust containing crystalline silica, silicon carbide, and hydrocarbons. In the autumn of 1980 extensive measurements were made of personal exposures to air contaminants. Eight hour time weighted exposures to sulphur dioxide ranged from less than 0.1 ppm to 1.5 ppm and respirable participate exposures ranged from 0.01 mg/m3 to 9.0 mg/m3. Geometric mean particulate exposures for jobs ranged from 0.1 mg/m3 to 1.46 mg/m3. The particulate contained varying amounts of alpha-quartz, ranging from less than 1% to 17%, and most quartz exposures were substantially below the threshold limit value of 100 micrograms/m3. Only traces of cristobalite (less than 1%) were found in the particulate. Median exposures to air contaminants in each job were estimated. Since the operations at the plant had been stable over the past 30 years, it was possible to estimate long term exposures of workers to sulphur dioxide, respirable particulate, quartz, total inorganic material, and extractable organic material. Cumulative exposure (average concentration times exposure duration) for each of the air contaminants was estimated for each worker using his job history. There was sufficient independent variability in the sulphur dioxide and respirable particulate cumulative exposures to make an assessment of their independent effects feasible. The theoretical basis for using the cumulative exposure index and its shortcomings for epidemiological applications were presented.

Air Pollutants, Occupational↗
PubMed1986

Gaseous and adsorbed PAH in an iron foundry.

The increased risk of lung cancer among foundry workers is assumed to be associated with the inhalation of gaseous and particle bound polycyclic aromatic hydrocarbons (PAH). These compounds are produced during pyrolysis of carbon containing loading material in the moulding sand. The concentrations of 20 PAH, some of which are carcinogenic, have been determined in the dusty casting area of an iron foundry by means of gas chromatography and mass spectrometry. The total dust was fractionated by means of a precision cascade impactor. It was possible to differentiate the PAH load in microgram/mg dust in seven particle size fractions ranging from 0.36- greater than or equal to 24.95 microns. Initially, there was an increase of the adsorbed PAH mass concentration with increasing particle diameter up to a maximum of 1.1 microgram/mg in the dust of the 1.57 micron fraction. Thereafter there was a continuous decrease of PAH mass concentration with increasing particle size. When the differing weights of the seven fractions are taken into account, however, the total PAH load of the individual fractions increases steadily with increasing particle size. The inhalable fine dust, 31.4% of the total dust, contains 49.9% of the total adsorbed PAH. The gas phase contained on average three times more carcinogenic PAH with four and five rings than was adsorbed on the dust. Thus the percentage of the gaseous substances amounts to 77% of the total PAH load at the place of work in an iron foundry.

Adsorption↗
PubMed1989

Risk of cancer from the use of tar bitumen in road works.

Tar bitumens are increasingly being used as a binder in road works. They consist of a standard product of about 70% bitumen and 25-30% tar. Tar bitumens are classifiable as the pyrolysis products of organic materials and are applied hot. Depending on the temperature used there are emissions of various intensities of polycyclic aromatic hydrocarbons (PAH), some of which are carcinogenic. A total of 250 one hour air samples was taken at breathing height on 20 days at 11 road works sites. The region of road paving operations in the immediate neighbourhood of the finishing machine operator and the screedmen were the chosen sampling points. A total of 19 unsubstituted chromatography/mass spectrometry. These included benzo[b]fluoranthene, benzo[a]pyrene, chrysene, dibenzo[a,h]anthracene, and indeno[1,2,3-cd]pyrene, all of which are carcinogenic. The median concentrations of chrysene and of benzo[b,j + k] fluoranthenes (determined en masse) were 9.3 and 2.8 micrograms/m3 respectively. The median concentrations of benzo[a]pyrene (BaP) and indeno[1,2,3,-cd]pyrene were 0.7 and 0.2 micrograms/m3 respectively. Dibenzo[a,h]anthracene had the lowest median concentration with about 0.03 micrograms/m3. Of the resulting shift means, the BaP concentration was over 1 microgram/m3 in about 50% of the cases, over 2 micrograms/m3 in 35%, and over 5 micrograms/m3 in about 15%. Even when the temperature of the paving mix was only between 120 degrees and 135 degrees C. 4.8% of the concentrations (identical to 3 samples) were greater than 2 micrograms BaP/m3, this value was exceeded in 34.9% of the determinations (identical to 30 samples) when the temperature of the tar bitumen was between 135 degrees and 150 degrees C. The highest concentration measured here was 17.8 micrograms BaP/m3. The recommended maximum paving temperature of the paving mix of 150 degrees C was exceeded in about 23% of all cases. The maximum concentration determined under any condition was 22 microgram/m(3). Thus the employment of tar bitumen as a binding material during road paving operations must be regarded as causing a considerable risk to health. The primary task is to ascertain whether tar bitumen can be replaced as a binder in paving for roads and what safety measures are practicable.

Air Pollutants, Occupational↗