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151.
Harald Geiger Ian Barnes Karl H. Becker Birger Bohn Theo Brauers Birgit Donner Hans-Peter Dorn Manfred Elend Carlos M. Freitas Dinis Dirk Grossmann Heinz Hass Holger Hein Axel Hoffmann Lars Hoppe Frank Hülsemann Dieter Kley Björn Klotz Hans G. Libuda Tobias Maurer Djuro Mihelcic Geert K. Moortgat Romeo Olariu Peter Neeb Dirk Poppe Lars Ruppert Claudia G. Sauer Oleg Shestakov Holger Somnitz William R. Stockwell Lars P. Thüner Andreas Wahner Peter Wiesen Friedhelm Zabel Reinhard Zellner Cornelius Zetzsch 《Journal of Atmospheric Chemistry》2002,42(1):323-357
Within the German Tropospheric Research Programme (TFS) numerous kinetic and mechanistic studies on the tropospheric reaction/degradation of the following reactants were carried out: oxygenated VOC, aromatic VOC, biogenic VOC, short-lived intermediates, such as alkoxy and alkylperoxy radicals.At the conception of the projects these selected groups were classes of VOC or intermediates for which the atmospheric oxidation mechanisms were either poorly characterised or totally unknown. The motivation for these studies was the attainment of significant improvements in our understanding of the atmospheric chemical oxidation processes of these compounds, particularly with respect to their involvement in photooxidant formation in the troposphere. In the present paper the types of experimental investigations performed and the results obtained within the various projects are briefly summarised. The major achievements are highlighted and discussed in terms of their contribution to improving our understanding of the chemical processes controlling photosmog formation in the troposphere. 相似文献
152.
This study demonstrates that oxalate has a strong inhibiting effect onFe-catalyzed S(IV) oxidation by oxygen in aqueous solution. While thepseudo-first order rate constant of S(IV) oxidation was determined to be1.6 × 103 M-1 s-1 in experimentswithout oxalate, the oxidation of S(IV) was totally inhibited at a molarconcentration ratio of iron:oxalate = 1:5 at an oxalate concentration of 4M. Under these conditions, the Fe(II)/Fe(III) ratio remained nearlyconstant during the observed reaction time. The determined rate constants wereindependent of the initial oxidation state of iron. However, with increasingconcentrations of oxalate, a longer induction period is observed forexperiments with iron initially in the Fe(II) oxidation state. 相似文献
153.
154.
Ionosonde data from sixteen stations are used to study the semiannual and annual variations in the height of the ionospheric F2-peak, hmF2. The semiannual variation, which peaks shortly after equinox, has an amplitude of about 8 km at an average level of solar activity (10.7 cm flux = 140 units), both at noon and midnight. The annual variation has an amplitude of about 11 km at northern midlatitudes, peaking in early summer; and is larger at southern stations, where it peaks in late summer. Both annual and semiannual amplitudes increase with increasing solar activity by day, but not at night. The semiannual variation in hmF2 is unrelated to the semiannual variation of the peak electron density NmF2, and is not reproduced by the CTIP and TIME-GCM computational models of the quiet-day thermosphere and ionosphere. The semiannual variation in hmF2 is approximately isobaric, in that its amplitude corresponds quite well to the semiannual variation in the height of fixed pressure-levels in the thermosphere, as represented by the MSIS empirical model. The annual variation is not isobaric. The annual mean of hmF2 increases with solar 10.7 cm flux, both by night and by day, on average by about 0.45 km/flux unit, rather smaller than the corresponding increase of height of constant pressure-levels in the MSIS model. The discrepancy may be due to solar-cycle variations of thermospheric winds. Although geomagnetic activity, which affects thermospheric density and temperature and therefore hmF2 also, is greatest at the equinoxes, this seems to account for less than half the semiannual variation of hmF2. The rest may be due to a semiannual variation of tidal and wave energy transmitted to the thermosphere from lower levels in the atmosphere. 相似文献
155.
J. M. C. Plane 《Annales Geophysicae》2000,18(7):807-814
It is proposed that a component of meteoric smoke, sodium bicarbonate (NaHCO3), provides particularly effective condensation nuclei for noctilucent clouds. This assertion is based on three conditions being met. The first is that NaHCO3 is present at sufficient concentration (104 cm–3) in the upper mesosphere between 80 and 90 km. It is demonstrated that there is strong evidence for this based on recent laboratory measurements coupled with atmospheric modelling. The second condition is that the thermodynamics of NaHCO3(H2O)n cluster formation allow spontaneous nucleation to occur under mesospheric conditions at temperatures below 140 K. The Gibbs free energy changes for forming clusters with n = 1 and 2 were computed from quantum calculations using hybrid density functional/Hartree-Fock (B3LYP) theory and a large basis set with added polarization and diffuse functions. The results were then extrapolated to higher n using an established dependence of the free energy on cluster size and the free energy for the sublimation of H2O to bulk ice. A 1-dimensional model of sodium chemistry was then employed to show that spontaneous nucleation to form ice particles (n > 100) should occur between 84 and 89 km in the high-latitude summer mesosphere. The third condition is that other metallic components of meteoric smoke are less effective condensation nuclei, so that the total number of potential nuclei is small relative to the amount of available H2O. Quantum calculations indicate that this is probably the case for major constituents such as Fe(OH)2, FeO3 and MgCO3. 相似文献
156.
157.
The implicit time integration scheme of Stott and Harwood (1993) was proposed as an efficient scheme for use in three-dimensional chemical models of the atmosphere. The scheme was designed for chemistry schemes using chemical families, in which species with short lifetimes are grouped into longer-lived families. Further study with more complex chemistry, more species and reactions showed the scheme to be non-convergent and unstable under certain conditions; particularly for the perturbed chemical scenarios of polar stratospheric winters. In this work the scheme has been improved by revising the treatment of families and the convergence properties of the scheme. The new scheme has been named IMPACT (IMPlicit Algorithm for Chemical Time-stepping). It remains easy to implement and produces simulations that compare well with integrations using more accurate higher order schemes. 相似文献
158.
Fog and rain water chemistry at Mt. Fuji: A case study during the September 2002 campaign 总被引:2,自引:0,他引:2
Koichi Watanabe Yusaku Takebe Nobuhiro Sode Yasuhito Igarashi Hiroshi Takahashi Yukiko Dokiya 《Atmospheric Research》2006,82(3-4):652
Measurements of fog and rain water chemistry at the summit of Mt. Fuji, the highest peak in Japan, as well as at Tarobo, the ESE slope of Mt. Fuji in September 2002. The pH of fog and rain water sampled at Mt. Fuji varied over a range of 4.0–6.8. Acidic fogs (pH < 5.0) were observed at the summit when the air mass came from the industrial regions on the Asian continent. The ratio of [SO42−]/[NO3−] in the fog water was lower at Tarobo than at the summit. High concentrations of Na+ and Cl− were determined in the rain water sampled at the summit, possibly because of the long-range transport of sea-salt particles raised by a typhoon through the middle troposphere. The vertical transport of sea-salt particles would influence the cloud microphysical properties in the middle troposphere. Significant loss of Mg2+ was seen in the rain water at the summit. The concentrations of peroxides in the fog and rain water were relatively large (10–105 μM). The potential capacity for SO2 oxidation seems to be strong from summer to early autumn at Mt. Fuji. The fog water peroxide concentrations displayed diurnal variability. The peroxide concentrations in the nighttime were significantly higher than those in the daytime. 相似文献
159.
160.
Alexander Zdravkov Irena Kostova Jordan Kortenski 《International Journal of Coal Geology》2007,71(4):488
Several Mio-Pliocene aged lignite seams occur as part of a non-marine transgressive sequence in the Elhovo graben in south-eastern Bulgaria. The present study is focused on 45 samples collected from three boreholes in the eastern part of the basin. Petrographic data along with ash and sulphur contents were used in order to determine the lateral and vertical variations of the coal facies and depositional environment of the Elhovo lignite.The lignite seams accumulated in a rheotrophic, low-lying mire with high pH value and are characterized by high ash yields and sulphur contents. Despite of the neutral to weakly alkaline environment the bacterial activity was limited and the tissue preservation and gelification were mainly controlled by the redox conditions.Vegetation rich in decay resistant conifers dominated in the Elhovo basin together with mesophytic angiosperm species. The absence of algal remains and sapropelic coal indicated that open water areas were not present during peat accumulation. The latter processed in an environment, characterized by low subsidence rate, in which prior to the burial the woods were subjected to severe mechanical destruction. According to our interpretation, the enhanced impregnation of the tissues bacteria and fungi played only a secondary role in the process of humification. The lignite from borehole 122 and partly from BH 145 deposited in an environment characterized by relatively low (ground)water table, whereas to the south an area dominated by a flooded forest swamp (BH 104) formed. This is suggested by the better tissue preservation and gelification of the organic matter in BH 104. The vertical variation of the maceral composition in the studied lignite is interpreted as a consequence of vegetational changes, rather than to changes in the depositional environment. The low contents of inertinite macerals indicate that despite of the low water level the environment was relatively wet and the thermal and oxidative destruction of the tissues was limited.Peat accumulation was terminated by a major flooding event and a short term establishment of a lake. In contrast to the West Maritsa basin, no seam formed in the Elhovo basin during the filling stage of the lake. 相似文献