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101.
The products of the 254 nm photolysis of ppm levels of DMDS have been studied as a function of the O2 partial pressure at 760 Torr (N2 + O2) and 298±2 K. The major sulfur containing compounds detected were SO2 and CH3SO3H (methane sulfonic acid, MSA) and the major carbon containing compounds were CO, HCHO, CH3OH and CH3OOH (methyl hydroperoxide). Within the experimental error limits the observed sulfur and carbon balances were approximately 100%. CH3OOH has been observed for the first time in such a photooxidation system. Its observation provides evidence for the formation of CH3 radicals by the further oxidation of the CH3S radicals formed in the primary photolysis step.From the behavior of the DMDS photolysis products as a function of the O2 partial pressure, O3 concentration and added OH radical source it is postulated that the further reactions of CH3SOH (methyl sulfenic acid), formed in the reaction OH + CH3SCCH3 CH3SOH + CH3S, are the main source of MSA in the 254 nm photolysis of DMDS.Some of the possible implications of the results of this study for the degradation mechanisms of other atmospherically important organic sulfur compounds, in particular DMS, are briefly considered. 相似文献
102.
Difunctional organic nitrates are important products of the atmospheric reaction of NO3 radicals with unsaturated hydrocarbons about which relatively little is known. In a continuation of the investigation of the atmospheric chemistry of such compounds, the UV absorption spectra of the following organic dinitrates and keto nitrates have been quantitively measured in the gas phase at 298±2 K and atmospheric pressure: 1,2-propandiol dinitrate, CH3CH(ONO2)CH2(ONO2); 1,2-butandiol dinitrate, CH3CH2CH(ONO2)CH2(ONO2); 2,3-butandiol dinitrate, CH3CH(ONO2)CH(ONO2)CH3;cis 1,4-dinitrooxy-2-butene, CH2(ONO2)CH=CHCH2(ONO2); 3,4-dinitrooxy-1-butene, CH2(ONO2CH(ONO2)CH=CH2; -nitrooxy acetone, CH3COCH2(ONO2); 1-nitrooxy-2-butanone, CH3CH2COCH2(ONO2); 3-nitrooxy-2-butanone, CH3CH(ONO2)COCH3.Although the UV spectra of the nitrates are all very similar in shape those of the keto nitrates are red-shifted compared to the dinitrates and in the spectral range of atmospheric interest (>290 nm) their absorption cross-sections are approximately a factor of 5 higher. The cross-sections of the dinitrates are a factor of 2 higher than those reported in the literature for the corresponding alkyl mononitrates.The UV absorption cross-sections of the difunctional nitrates were used in combination with solar actinic flux data to estimate photolysis frequencies and consequently atmospheric lifetimes for these compounds. The results indicate that for the saturated difunctional nitrates studied in this work photolysis will generally be somewhat some important than reaction with OH radicals as an atmospheric removal process. However, for unsaturated nitrates loss due to reaction with OH will dominate over photolysis as an atmospheric sink.Preliminary FT-IR analyses of the photolysis products of -nitrooxy acetone, 3-nitrooxy-2-butanone and 2,3-butandiol dinitrate using both mercury and fluorescent lamps indicate that NO2 is released in the primary step. The further reactions of the radicals thus produced result in the formation of CO, aldehydes and PAN. The possible significance of the results for difunctional organic nitrate as reservoirs for reactive odd nitrogen NO
y
in the atmosphere, especially during the night, is briefly discussed. 相似文献
103.
K. Mannschreck K. Bächmann K. H. Becker Th. Heil R. Kurtenbach M. Memmesheimer V. Mohnen A. Obermeier D. Poppe R. Steinbrecher Th. Schmitz A. Volz-Thomas F. Zabel 《Journal of Atmospheric Chemistry》2002,42(1):281-286
The database for volatile organic compounds (VOC data base) was created with the aim of providing an overview of tropospheric hydrocarbon measurements. The data base contains 202 substances, for which atmospheric and useful kinetic data such as rate coefficients, photolysis frequencies, mixing ratios, emission data and ozone formation potentials are compiled from available literature. The database file can be downloaded without charge from http://www.physchem.uni-wuppertal.de/voc-database. Registered users will be informed about the appearance of updates. 相似文献
104.
R. Kurtenbach R. Ackermann K. H. Becker A. Geyer J. A. G. Gomes J. C. Lörzer U. Platt P. Wiesen 《Journal of Atmospheric Chemistry》2002,42(1):395-411
In 1997 and 1998 several field campaigns for monitoring non-methane volatile organic compounds (NMVOCs) and nitrogen oxides (NOx) were carried out in a road traffic tunnel and in the city center of Wuppertal, Germany. C2–C10 aliphatic and aromatic hydrocarbons were monitored using a compact GC instrument. DOAS White and long path systems were used to measure aromatic hydrocarbons and oxygenated aromatic compounds. A formaldehyde monitor was used to measure formaldehyde. Chemiluminescence NO analysers with NO2 converter were used for measuring NO and NO2. The high mixing ratios of the NMVOCs observed in the road traffic tunnel, especially 2.9 ppbv phenol, 1.5ppbv para-cresol and 4.4 ppbv benzaldehyde, in comparison with themeasured background concentration clearly indicate that these compounds were directly emitted from road traffic. Para-Cresol was for the first timeselectively detected as primary pollutant from traffic. From the measured data a NMVOC profile of the tunnel air and the city air, normalised to benzene (ppbC/ppbC), was derived. For most compounds the observed city air NMVOC profile is almost identical with that obtained in the traffic tunnel. Since benzene originates mainly from road traffic emission, the comparison of the normalised emission ratios indicate that the road traffic emissions in Wuppertal have still the largest impact on the city air composition, which is in contrast to the German emission inventory. In both NMVOC profiles, aromatic compounds have remarkably large contributions of more than 40 ppbC%. In addtion, total NMVOC/NOx ratios from 0.6 up to 3.0ppbC/ppb in the traffic tunnel air and 3.4± 0.5 in the city air of Wuppertal were obtained. From the observed para-cresol/toluene and ortho-cresol/toluene ratios in the city air, evidence was found thatalso during daytime NO3 radical reactions play an important role in urban air. 相似文献
105.
106.
Prof. Dr. A. Becker 《International Journal of Earth Sciences》1924,14(4):364-374
Ohne Zusammenfassung 相似文献
107.
In the Basle region of Switzerland we demonstrate that rockfall blocks can be dated accurately using the radiocarbon method. Soil beneath rockfall blocks containing organic macro‐remains was sampled at four cliff sites in the Tabular Jura south‐east of Basle. A lightweight drilling rig drills a 101‐mm‐diameter hole through rockfall blocks up to 6 m in height. A downhole sampler is used to recover soil samples from below the blocks. Eighteen radiocarbon dates on charcoal, wood, needles of conifers and organic macro‐remains from 11 blocks gave dates between 970 and 440 bp . Calibrated ages range between ad 1210 and ad 1450. These results, along with field observations and historical research, suggest that a large number of blocks toppled as rockfalls within a short time interval in the epicentral area of the ad 1356 Basle earthquake. 相似文献
108.
Growth kinetics of enstatite reaction rims studied on nano-scale,Part I: Methodology,microscopic observations and the role of water 总被引:1,自引:0,他引:1
Ralf Milke Ralf Dohmen Hans-Werner Becker Richard Wirth 《Contributions to Mineralogy and Petrology》2007,154(5):519-533
The kinetics of (Mg, Fe)SiO3 pyroxene layer growth within silicate thin films with total thickness <1 μm was studied experimentally at 0.1 MPa total pressure,
controlled fO2 and temperatures from 1,000 to 1,300°C. The starting samples were produced by pulsed laser deposition. Layer thickness before
and after the experiments and layer composition as well as microstructures, grain size and shape of the interfaces were determined
by Rutherford back scattering and transmission electron microscopy assisted by focused ion beam milling. Due to the miniaturization
of the starting samples and the use of high resolution analytical methods the experimentally accessible temperature range
for rim growth experiments was extended by about 300°C towards lower temperatures. The thickness of the layers at a given
temperature increases proprotional to the square root of time, indicating a diffusion-controlled growth mechanism. The temperature
dependence of rim growth yields an apparent activation energy of 426 ± 34 kJ/mol. The small grain size in the orthopyroxene
rims implies a significant contribution of grain boundary diffusion to the bulk diffusion properties of the polycrystalline
rims. Based on microstructural observations diffusion scenarios are discussed for which the SiO2 component behaves immobile relative to the MgO component. Volume diffusion data for Mg in orthopyroxene from the literature
indicate that the measured diffusivity is probably controlled by the mobility of oxygen. The observed reaction rates are consistent
with earlier results from dry high-temperature experiments on orthopyroxene rim growth. Compared to high pressure experiments
at 1,000°C and low water fugacities, reaction rates are 3–4 orders of magnitude smaller. This observation is taken as direct
evidence for a strong effect of small amounts of water on diffusion in silicate polycrystals. In particular SiO2 changes from an immobile component at dry conditions to an extremely mobile component even at very low water fugacities. 相似文献
109.
The position of the Raman methane (CH4) symmetric stretching band (ν1) over the range 1-650 bar and 0.3-22 °C has been determined using a high-pressure optical cell mounted on a Raman microprobe. Two neon emission lines that closely bracket the CH4 band were collected simultaneously with each CH4 spectrum. The peak position was determined after least squares fitting using a summed Gaussian-Lorentzian method, resulting in a precision of ≈±0.02 cm−1 in peak position determination. The CH4ν1 band position shifts to lower wave number with increasing pressure. At a given pressure, the band shifts to lower wave number with decreasing temperature, and the magnitude of the temperature shift increases with increasing pressure. The relationship between the Raman CH4ν1 band position and temperature and pressure determined here may be used to estimate the internal pressure in natural or synthetic CH4-bearing fluid inclusions. This information, in turn, may be used to determine the density of pure CH4 fluid inclusions and the salinity of CH4-bearing aqueous inclusions. 相似文献
110.
Abiogenic methane may be produced in submarine hydrothermal systems by degassing of basalts or serpentinization of ultramafic outcrops. The latter process presumably releases little primordial helium and is therefore implicated by high CH4/3He ratios in vent fluids from the ultramafic-hosted Rainbow field and in methane plumes near ultramafic outcrops. In two segments of the Mid-Atlantic Ridge, at 5.4°N and 51°N, we have observed depth-separated CH4 and 3He plumes. In both cases, the helium plume was deeper, near the valley floor. It may be that the plumes issue from separate vents, where the helium is discharged near the volcanic axis and the methane is generated by serpentinization on the valley wall. However, at the present time the locations of the vents that produce these plumes are not known. Using a one-pass model, we investigated whether separate venting could arise from heat conduction from a primary, helium-carrying, hydrothermal circulation to a second, shallower fracture loop intersecting ultramafic rock. The model results indicate that the flow rate through the secondary loop would have to be relatively low in order for it to stay warm enough for serpentinization to proceed. In this case, some of the exothermic heat production is lost by conduction, and the temperature increase in the circulating fluid is only a fraction of that expected from a water/rock ratio of 1:1. 相似文献