Study of metal aerosol systems as a sink for atmospheric SO2

The chemical removal of SO₂ in the presence of different aerosol systems has been investigated in laboratory experiments using a dynamic flow reactor. The aerosols consisted of wetted particles containing one of the following substances: MnCl₂, Mn(NO₃)₂, MnSO₄, CuCl₂, Cu(NO₃)₂, CuSO₄, FeCl₃, NaCl. The SO₂ removal rate R was measured as a function of the SO₂ gas phase concentration (SO₂)_g, the spatial metal concentration C_Me, and the relative humidity rH in the reactor. A first-order dependence with regard to (SO₂)_g was observed for each type of aerosol. For the Mn(II) and Cu(II) aerosols R was found to be a non-linear function of C_Me except for MnSO₄ and Cu(NO₃)₂ particles. The removal rate showed a significant increase with the relative humidity particularly when rH was close to the deliquescence point of the wetted particles. Among the Mn(II) and Cu(II) aerosols investigated Mn(NO₃)₂ was found to be most efficient for the chemical removal of SO₂ at atmospheric background conditions, especially in haze and fog droplets. The results further indicate that the catalytic oxidation of S(IV) in such aerosol systems may be as efficient as its oxidation by H₂O₂ in cloud water.     

The characterization and distribution of aerosol and gaseous species in the winter monsoon over the western pacific ocean

In order to obtain a better understanding of the behavior of aerosols and SO₂ in the longrange transport through a marine boundary layer, a simple box-model is applied to the evaluation of the residence times of the species from the concentrations of gases and aerosols measured simulataneously on two islands in the West Pacific Ocean in the north-west monsoon. For Aitken and large particles, the residence time is varied from 3.7 to 7.4 days depending on the particle size, and their flux to the sea is equal to or slightly smaller than that of the free atmosphere. The residence time of giant particles is about one day and their flux to the sea is three times larger than that of the free atmosphere. The residence time of SO₂ is 15 hr, and the relative SO₂ mass flows of the deposition to the sea, of the diffusion to the free atmosphere and of the transformation to SO₄ ^2- are approximately 4, 1 and 1, respectively.     

Sulfur dioxide in the North American Arctic

Determinations of atmospheric sulfur dioxide were made across the North American Aretic using gas chromatography with a detection limit of 25 parts per trillion by volume and a precision of 25% or better. The vertical distribution of sulfur dioxide in the Arctic atmosphere in April, 1986 was highly variable, with concentrations ranging from the detection limit to 15 parts-per-billion by volume (ppbv). While SO₂ exceeded 10 ppbv in an exceptional haze layer in the Alaskan Arctic, sulfur dioxide was sometimes in the 1 – 5 ppbv range when the haze was absent. This was particularly true for the Canadian Arctic in the vicinity of Alert. In the lower stratosphere over Ellesmere Island, sulfur dioxide was 0.85 ppbv.     

Effect of monochloramine on isolated fulvic acid

Monochloramine is interesting both as a selective oxidant of fulvic acid and as a drinking water disinfectant. In this study, the controlled reaction of aquatic fulvic acid with monochloramine did not result in products detectable by ether extraction-gas chromatography-flame ionization detection techniques. Evidence of a reaction was shown by bleaching of the fulvic acid solution (decreased absorbance at 465 nm) and chlorine substitution. Chlorine-containing products were quantified by the total carbon adsorbable organic halide (TOX) parameter. Bleaching and organic chlorine formation were much less extensive than in the reaction of free chlorine with fulvic acid. Monochloramine was shown to produce an organic chlorine fraction more hydrophilic and with higher molecular size than that produced by chlorine and fulvic acid. Results suggest that monochloramine may be useful tool for the investigation of certain humic functionalities because it reacts rather selectively and to a small extent with aquatic fulvic acid.     

Effects of high CO2 levels on surface temperature and atmospheric oxidation state of the early Earth

One-dimensional radiative-convective and photochemical models are used to examine the effects of enhanced CO₂ concentrations on the surface temperature of the early Earth and the composition of the prebiotic atmosphere. Carbon dioxide concentrations of the order of 100–1000 times the present level are required to compensate for an expected solar luminosity decrease of 25–30%, if CO₂ and H₂O were the only greenhouse gases present. The primitive stratosphere was cold and dry, with a maximum H₂O volume mixing ratio of 10^–6. The atmospheric oxidation state was controlled by the balance between volcanic emission of reduced gases, photo-stimulated oxidation of dissolved Fe⁺² in the oceans, escape of hydrogen to space, and rainout of H₂O₂ and H₂CO. At high CO₂ levels, production of hydrogen owing to rainout of H₂O₂ would have kept the H₂ mixing ratio above 2×10^–4 and the ground-level O₂ mixing ratio below 10^–11, even if no other sources of hydrogen were present. Increased solar UV fluxes could have led to small changes in the ground-level mixing ratios of both O₂ and H₂.     

Field studies of methane emission from termite nests into the atmosphere and measurements of methane uptake by tropical soils

The flux of CH₄ and CO₂ from termite nests into the atmosphere has been measured in a broad-leafed-type savannah in South Africa. Measurements were carried out on nests of species of six genera, i.e., Hodotermes, Macrotermes, Odontotermes, Trinervitermes, Cubitermes, and Amitermes. The flux rates of CH₄ relative to the flux rate of CO₂ in terms of carbon obtained for the individual species showed ratios of 2.9×10^-3, 7.0×10^-4, 6.7×10^-5, 8.7×10^-3, 2.0×10^-3 and 4.2×10^-3, respectively. Using data published on the assimulation efficiencies of termites, the flux of carbon as CH₄ accounts for 6.0×10^-5 to 2.6×10^-3 of the carbon ingested which results in a global CH₄ emission by termites of 2 to 5×10¹² g/yr. Methane is decomposed in the soil with average decomposition rates of 52 g/m²/h. The annual CH₄ consumption in the tropics and subtropics is estimated to be 21×10¹² g which exceeds the CH₄ emission rate by termites.     

An FTIR product study of the photooxidation of dimethyl disulfide

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.     

Accommodation coefficient for trace gas uptake using deposition profile measurement in an annular reactor

A simple and inexpensive procedure is presented for the measurement of gaseous accommodation coefficients upon liquid or solid surfaces. The gas of interest is passed in laminar flow through an annular reactor and the profile of deposition is subsequently determined. The Cooney-Kim-Davies theoretical treatment of deposition in cylindrical systems is adapted to describe uptake on the walls of the annular reactor as a function of accommodation coefficient and diffusion coefficient. The accommodation coefficient () of ammonia on oxalic acid is determined in both cylindrical and annular systems and good agreement is found. Uptake of nitrogen dioxide on wet alkaline surfaces yields a value for of 2.5×10^–4, and on solely wet surfaces a value of 8.7×10^–5. Nitric and nitrous acids deposit to aqueous sodium carbonate/glycerol surfaces with values of of 1.5 × 10^–2 and 4.3×10^–3, respectively.     

Investigations on distributions and fluxes of sea-air CO_2 of the expedition areas in the Arctic Ocean

揋reenhouse effect?causing global warming has been an important issue of studying climate change. In the latest 100 years, the earth surface temperature has been increased by about 0.4℃—0.8℃[1,2]. And this has been becoming a hotspot of the world[3,4]     

黄骅坳陷二氧化碳气成因类型及分布规律

二氧化碳气是经济价值很高且应用前景十分广阔的非烃气体。黄骅坳陷二氧化碳气有多种成因类型,即有机成因、热变质成因和壳 幔混源成因,其中前两种分布较广泛。对于不同成因的二氧化碳气,其分布控制因素有所不同。有机成因二氧化碳气主要分布于生油凹陷周围,是烃类气体的次要伴生产物,并远离大断裂分布。热变质成因二氧化碳气主要分布在深部碳酸盐岩发育、岩浆活动较强烈的地区,并在大断裂附近富集;二氧化碳的含量比有机成因的高,但比壳 幔混源成因的低。壳 幔混源成因二氧化碳气主要出现在深大断裂附近,其分布虽然局限,但纯度是最高的。二氧化碳富集的地区常常是次生溶蚀作用较强的地区,因此也是寻找深部次生优质油气储层的有利地区。