Clouds of venus: a preliminary assessment of microstructure

The multimodal microstructure of the Venus cloud system has been examined. In addition to confirmed H(2)SO(4) droplets and suspected elemental sulfur, a highly concentrated aerosol population has been observed extending above, within, and below the cloud system. These aerosols appear to cycle through the cloud droplets, but can never be removed by the weak precipitation mechanisms present. All cloud particles are likely laced with aerosol contaminants. Sedimentation and decomposition of H(2)SO(4) in the droplets of the lower cloud region contribute more than 7 watts per square meter of heat flux equaling one-fourth of the solar net flux at 50 kilometers.     

Large volcanic aerosol load in the stratosphere linked to Asian monsoon transport

The Nabro stratovolcano in Eritrea, northeastern Africa, erupted on 13 June 2011, injecting approximately 1.3 teragrams of sulfur dioxide (SO(2)) to altitudes of 9 to 14 kilometers in the upper troposphere, which resulted in a large aerosol enhancement in the stratosphere. The SO(2) was lofted into the lower stratosphere by deep convection and the circulation associated with the Asian summer monsoon while gradually converting to sulfate aerosol. This demonstrates that to affect climate, volcanic eruptions need not be strong enough to inject sulfur directly to the stratosphere.     

单纯形优化法在混凝除磷试验中的应用研究

以天津市纪庄子污水厂二级出水作为研究对象,利用单纯形优化方法,探讨不同混凝剂优化混凝除磷的最优条件。本实验对两种混凝剂硫酸铁、硫酸铝的混凝除磷效果进行了研究,利用单纯形优化方法对两种混凝剂的主要影响因素(混凝剂投加量和pH)进行了优化,从而得出了两种混凝剂去除二级出水中磷的最优条件。结果表明:通过18～25次实验,单纯形即可确定两种混凝剂除磷的最优条件。每种混凝剂的去除率都至少增加了30%。硫酸铁、硫酸铝两种混凝剂对总磷的最大去除率分别为87.25%,95.60%。每种混凝剂对正磷酸盐的去除率大于总磷的去除率。硫酸铁、硫酸铝两种混凝剂除磷的总磷残余浓度分别为0.35 mg.L-1,0.12 mg.L-1,达到0.5 mg.L-1以下的城市污水再生利用景观环境用水水质标准(GB/T18921-2002)。     

Solid ammonium sulfate aerosols as ice nuclei: a pathway for cirrus cloud formation

Laboratory measurements support a cirrus cloud formation pathway involving heterogeneous ice nucleation by solid ammonium sulfate aerosols. Ice formation occurs at low ice-saturation ratios consistent with the formation of continental cirrus and an interhemispheric asymmetry observed for cloud onset. In a climate model, this mechanism provides a widespread source of ice nuclei and leads to fewer but larger ice crystals as compared with a homogeneous freezing scenario. This reduces both the cloud albedo and the longwave heating by cirrus. With the global ammonia budget dominated by agricultural practices, this pathway might further couple anthropogenic activity to the climate system.     

A thiosulfate shunt in the sulfur cycle of marine sediments

The oxidation of sulfide, generated by bacterial sulfate reduction, is a key process in the biogeochemistry of marine sediments, yet the pathways and oxidants are poorly known. By the use of (35)S-tracer studies of the S cycle in marine and freshwater sediments, a novel shunt function of thiosulfate (S(2)O(3)(2-)) was identified. The S(2)O(3)(2-) constituted 68 to 78 percent of the immediate HS(-)-oxidation products and was concurrently (i) reduced back to HS(-), (ii) oxidized to SO(4)(2-), and (iii) disproportionated to HS(-) + SO(4)(2-). The small thiosulfate pool is thus involved in a dynamic HS(-) - S(2)O(3)(2-) cycle in anoxic sediments. The disproportionation of thiosulfate may help account for the large difference in isotopic composition ((34)S/(32)S) of sulfate and sulfides in sediments and sedimentary rocks.     

Natural Versus Anthropogenic Factors Affecting Low-Level Cloud Albedo over the North Atlantic

Cloud albedo plays a key role in regulating Earth's climate. Cloud albedo depends on column-integrated liquid water content and the density of cloud condensation nuclei, which consists primarily of submicrometer-sized aerosol sulfate particles. A comparison of two independent satellite data sets suggests that, although anthropogenic sulfate emissions may enhance cloud albedo immediately adjacent to the east coast of the United States, over the central North Atlantic Ocean the variability in albedo can be largely accounted for by natural marine and atmospheric processes that probably have remained relatively constant since the beginning of the industrial revolution.     

Disulfate ion as an intermediate to sulfuric Acid in Acid rain formation

The oxidation of the bisulfite ion by dissolved oxygen to produce sulfate ion involves the formation of a previously undetected intermediate. This intermediate has a fairly strong Raman band at 1090 wave numbers and a weak Raman band at 740 wave numbers, both of which are probably due to sulfur-oxygen stretches. The intermediate is proposed to be the disulfate ion S(2)O(7)(2-), which hydrolyzes into H(+) and either SO(4)(2-) or HSO(4)(2-) with a half-life of about 52 seconds at 25 degrees C.     

Identification of hydroxymethanesulfonate in fog water

Previous studies have suggested that hydroxymethanesulfonate ion (HMSA) can be an important species in fog and cloud water. Formation of HMSA explains observed excesses of sulfur in the S(IV) state (+4 oxidation state) and formaldehyde (CH(2)O) in fogs and clouds. HMSA was determined in fog water by a novel ion-pairing chromatographic technique. Concentrations in samples collected in Bakersfield, California, within 5 kilometers of major sources of sulfur dioxide (SO(2)), were as high as 300 micromoles per liter. Total CH(2)O and S(IV) concentrations, which were measured independently, ranged from 10 to 200 and 5 to more than 300 micromoles per liter, respectively. Concentrations of CH(2)O, S(IV), and HMSA at Buttonwillow, California, which is 15 kilometers from the nearest source of SO(2), were less than those at Bakersfield but not absent. These data confirm that HMSA forms in atmospheric water droplets and can reach appreciable concentrations. HMSA represents an important source of acidity for water droplets and may also play a role in long-distance transport and transformation of SO(2).     

Calibration of sulfate levels in the archean ocean

The size of the marine sulfate reservoir has grown through Earth's history, reflecting the accumulation of oxygen into the atmosphere. Sulfur isotope fractionation experiments on marine and freshwater sulfate reducers, together with the isotope record, imply that oceanic Archean sulfate concentrations were <200 microM, which is less than one-hundredth of present marine sulfate levels and one-fifth of what was previously thought. Such low sulfate concentrations were maintained by volcanic outgassing of SO2 gas, and severely suppressed sulfate reduction rates allowed for a carbon cycle dominated by methanogenesis.     

催化光度法测定痕量8—羟基喹啉

研究了在硫酸环境中８－羟基喹啉对碘催化亚砷酸与硫酸铈氧化还原反应的抑制作用及其动力学条件。据此建立了动力学的直接光度法测定痕量８－羟基喹啉的新方法。结果表明,在０２２５ｍｏｌ／ＬＨ２ＳＯ４,０００１２５ｍｏｌ／ＬＡｓ２Ｏ３,０００１ｍｏｌ／ＬＣｅ（ＳＯ４）２,００１ｍｇ／ＬＩ,０５ｇ／ＬＮａＣｌ环境中测定８－羟基喹啉,其线性范围为００２０～０２７ｍｇ／Ｌ,表观摩尔吸光系数为２７×１０５Ｌ·ｍｏｌ１·ｃｍ１,Ｓａｎｄｅｌ灵敏度为０５３８μｇ／ｃｍ２。用本法对药物硫酸羟基喹啉钾中的８－羟基喹啉含量的测定,结果满意。     

不同钼水平对生长猪肝脏、肾脏亚硫酸氧化酶活性及尿中SO_3~(2-)、SO_4~(2-)的影响

在生长猪低钼低硒基础饲粮内,分别添加0、10、100ppm钼(钼酸铵),测定了猪肝、肾组织亚硫酸氧化酶活性、尿中SO_3~2-/SO_4~(2-)以及尿中SO_3~(2-)和SO_4~(2-)日排出量。结果初步表明:加钼能提高组织亚硫酸氧化酶活性,减少尿中SO_3~(2-)排出,提高SO_4~(2-)排出,降低尿中SO_2~(2-)/SO_4~(2-)。肝脏亚硫酸氧化酶活性与尿中SO_3~(2-)/SO_4~(2-)和SO_3~(2-)排出呈显著的强负相关,肾脏亚硫酸氧化酶活性与尿中SO_4~(2-)的排出量呈中等正相关。     

Magmatic vapor source for sulfur dioxide released during volcanic eruptions: evidence from mount pinatubo

Sulfur dioxide (SO(2)) released by the explosive eruption of Mount Pinatubo on 15 June 1991 had an impact on climate and stratospheric ozone. The total mass of SO(2) released was much greater than the amount dissolved in the magma before the eruption, and thus an additional source for the excess SO(2) is required. Infrared spectroscopic analyses of dissolved water and carbon dioxide in glass inclusions from quartz phenocrysts demonstrate that before eruption the magma contained a separate, SO(2)-bearing vapor phase. Data for gas emissions from other volcanoes in subduction-related arcs suggest that preeruptive magmatic vapor is a major source of the SO(2) that is released during many volcanic eruptions.     

模拟酸沉降下南方两种森林土壤对SO42-及NO3-的吸附

通过 3种模拟酸沉降溶液对福建和贵阳两种森林土壤样品的连续浸泡试验 ,研究了土壤对酸沉降中 SO42 -和 NO3-的吸附 ,以及盐基离子输入对这种吸附的影响 .结果表明 ,2种土壤对 SO42 -均有一定的吸附能力 ,但福建土壤的吸附量比贵阳土壤大 .土壤对 SO42 - 的吸附与酸沉降中 SO42 - 浓度及土壤水溶性 SO42 - 含量有关 ,但高浓度的盐基离子输入会降低 SO42 -的吸附量 .土壤对 NO3-的吸附主要发生在表土中 ,且比 SO42 -的吸附量低 ,但比预料的要高     

SO2在矿质颗粒物表面非均相反应研究进展

我国秋冬季雾霾频发,对人类健康造成巨大威胁。大气中SO_2经系列物理化学反应产生的硫酸盐气溶胶是雾霾产生的元凶,其中矿质颗粒物参与的SO_2表面非均相反应尤为重要,因此,厘清矿质颗粒物表面硫酸盐的形成机制是解析大气雾霾形成的关键科学问题。本文综述了SO_2在不同类型氧化型矿质颗粒物表面非均相反应的研究进展,讨论了多污染物共存体系、湿度和光照对SO_2非均相反应的影响,并对目前矿质颗粒物表面非均相反应研究中存在的问题进行了评述,旨在加深对矿质颗粒物促进硫酸盐形成机制的认识,助力揭示我国雾霾的成因,进而为雾霾治理提供理论指导。     

Photolysis of sulfuric acid vapor by visible solar radiation

Atmospheric field measurements and models of the stratospheric sulfate aerosol layer led to the suggestion that sulfuric acid (H2SO4) must photolyze at high altitudes. We propose that excitation of vibrational overtones of H2SO4 and its hydrate in the near-infrared and visible leads to photolysis, forming sulfur trioxide (SO3) and water. On the basis of absorption cross sections calculated with ab initio methods calibrated to experimental measurements, we estimated J values that are sufficient to explain stratospheric and mesospheric sulfur dioxide (SO2) concentrations and the observation of the sulfate layer.     

A determination of the cloud feedback from climate variations over the past decade

Estimates of Earth's climate sensitivity are uncertain, largely because of uncertainty in the long-term cloud feedback. I estimated the magnitude of the cloud feedback in response to short-term climate variations by analyzing the top-of-atmosphere radiation budget from March 2000 to February 2010. Over this period, the short-term cloud feedback had a magnitude of 0.54 ± 0.74 (2σ) watts per square meter per kelvin, meaning that it is likely positive. A small negative feedback is possible, but one large enough to cancel the climate's positive feedbacks is not supported by these observations. Both long- and short-wave components of short-term cloud feedback are also likely positive. Calculations of short-term cloud feedback in climate models yield a similar feedback. I find no correlation in the models between the short- and long-term cloud feedbacks.     

Reduction of tropical cloudiness by soot

Measurements and models show that enhanced aerosol concentrations can augment cloud albedo not only by increasing total droplet cross-sectional area, but also by reducing precipitation and thereby increasing cloud water content and cloud coverage. Aerosol pollution is expected to exert a net cooling influence on the global climate through these conventional mechanisms. Here, we demonstrate an opposite mechanism through which aerosols can reduce cloud cover and thus significantly offset aerosol-induced radiative cooling at the top of the atmosphere on a regional scale. In model simulations, the daytime clearing of trade cumulus is hastened and intensified by solar heating in dark haze (as found over much of the northern Indian Ocean during the northeast monsoon).     

Cloud-radiative forcing and climate: results from the Earth radiation budget experiment

The study of climate and climate change is hindered by a lack of information on the effect of clouds on the radiation balance of the earth, referred to as the cloud-radiative forcing. Quantitative estimates of the global distributions of cloud-radiative forcing have been obtained from the spaceborne Earth Radiation Budget Experiment (ERBE) launched in 1984. For the April 1985 period, the global shortwave cloud forcing [-44.5 watts per square meter (W/m(2))] due to the enhancement of planetary albedo, exceeded in magnitude the longwave cloud forcing (31.3 W/m(2)) resulting from the greenhouse effect of clouds. Thus, clouds had a net cooling effect on the earth. This cooling effect is large over the mid-and high-latitude oceans, with values reaching -100 W/m(2). The monthly averaged longwave cloud forcing reached maximum values of 50 to 100 W/m(2) over the convectively disturbed regions of the tropics. However, this heating effect is nearly canceled by a correspondingly large negative shortwave cloud forcing, which indicates the delicately balanced state of the tropics. The size of the observed net cloud forcing is about four times as large as the expected value of radiative forcing from a doubling of CO(2). The shortwave and longwave components of cloud forcing are about ten times as large as those for a CO(2) doubling. Hence, small changes in the cloud-radiative forcing fields can play a significant role as a climate feedback mechanism. For example, during past glaciations a migration toward the equator of the field of strong, negative cloud-radiative forcing, in response to a similar migration of cooler waters, could have significantly amplified oceanic cooling and continental glaciation.     

Erratum

In the report "Cloud droplet deposition in subalpine balsam fir forests: Hydrological and chemical inputs" by G. M. Lovett et al. (24 Dec., p. 1303), two errors appeared in Table 2 on page 1304. The cloud deposition of SO(4)(2-), incorrectly reported as 275.8 kg ha(-1) year(-1), should have been 137.9 kg ha(-1) year(-1). The percentage of the sum contributed by clouds, reported as 81 for SO(4)(2-), should have been 68.     

Direct kinetic measurements of Criegee intermediate (CH₂OO) formed by reaction of CH₂I with O₂

Ozonolysis is a major tropospheric removal mechanism for unsaturated hydrocarbons and proceeds via "Criegee intermediates"--carbonyl oxides--that play a key role in tropospheric oxidation models. However, until recently no gas-phase Criegee intermediate had been observed, and indirect determinations of their reaction kinetics gave derived rate coefficients spanning orders of magnitude. Here, we report direct photoionization mass spectrometric detection of formaldehyde oxide (CH(2)OO) as a product of the reaction of CH(2)I with O(2). This reaction enabled direct laboratory determinations of CH(2)OO kinetics. Upper limits were extracted for reaction rate coefficients with NO and H(2)O. The CH(2)OO reactions with SO(2) and NO(2) proved unexpectedly rapid and imply a substantially greater role of carbonyl oxides in models of tropospheric sulfate and nitrate chemistry than previously assumed.