The effect of gas-phase chemistry on aqueous-phase sulfur dioxide oxidation rates     

William R. Stockwell 《Journal of Atmospheric Chemistry》1994,19(3):317-329

The rates and mechanisms of both gas and liquid phase reactions for the oxidation of sulfur dioxide play an important role in the production of atmospheric acids and aerosol particles. Rhodeet al. (1981) concluded that sulfate production rates were highly non-linear functions of sulfur dioxide emission rates. Their modelling study used an HO _x termination mechanism for the HO—SO₂ reaction in the gas-phase. Stockwell and Calvert (1983) determined that one of the products of the overall reaction of HO with sulfur dioxide was an HO₂ radical. The National Research Council (1983) using a version of the Rhodeet al. (1981) model modified to include HO₂ production from the HO—SO₂ reaction concluded that sulfate production becomes much more linear with respect to reductions in sulfur dioxide emissions. However, the cause of this increased linearity was not explained by the National Research Council report. It is demonstrated that the increased linearity is due to the coupling of gas-phases and aqueous phase chemistry. The gas-phase sulfur dioxide oxidation mechanism has a very significant effect on hydrogen perodide production rates.  相似文献   

热化学硫酸盐还原作用对碳酸盐岩气藏的化学改造——以川东北地区长兴组-飞仙关组气藏为例   总被引：20，自引：0，他引：20       下载免费PDF全文

杜春国  郝芳  邹华耀  张俊  朱扬明  王存武 《地质学报》2007,81(1):119-126

目前在川东北地区长兴组—飞仙关组已发现普光、渡口河、铁山坡、罗家寨等多个高含H2S的大、中型气田。通过天然气地球化学特征、流体包裹体盐度和岩心及薄片的镜下详细观察后认为,川东北地区长兴组—飞仙关组的大多数气藏遭受了热化学硫酸盐还原作用(TSR)的化学改造,TSR的改造主要表现在3个方面:1使C2 重烃相对于CH4、12C相对于13C优先被消耗,造成天然气干燥系数变大和碳同位素变重;2由于TSR产生的大量淡水的加入,使气藏的原生地层水被稀释,造成地层水盐度降低;3TSR相关流体(烃类和H2S等)与储层岩石之间的相互作用使储层被溶蚀和硬石膏发生蚀变,造成储层孔隙度增大,从而对改善其物性具有重要意义。  相似文献   

Desalinization of running waters: III. Changes in the structure of diatom assemblages caused by a decreasing salt load and changing ion spectra in the river Wipper (Thuringia, Germany)     

Horst Ziemann  Ludwig Kies  Claus-Jürgen Schulz   《Limnologica》2001,31(4):257-280

Salt-loaded effluents were introduced into the river Wipper during the mining period for almost a century. Beginning with the year 1990, the waste water load was strongly reduced due to the termination of the potash industry. Prior to 1990, monthly means of the chloride concentrations at times exceeded 6,000 mg l⁻¹ in the strongly polluted sections. Maximum concentrations reached twice these values. Up to 1998, mean annual chloride concentrations decreased to values below 2,000 mg l⁻¹. This led to more balanced fluctuations in salinity which had been pronounced before, depending on discharge and short-term changes in production. Similarly, the physiologically adverse ion conditions improved due to decrasing potassium and increasing calcium proportions.

In 1963/64, 1986 and 1998, samples of epilithic, epiphytic and epipsammic diatoms were taken at locations of different salinities along the river and examined for the effects of the salinization on the structure of the diatom assemblages. These structures changed in dependence on salinity. Increasing salt concentrations coincided with decreasing oligohalophilic and increasing mesohalophilic and polyhalophilic species numbers. Above a chloride concentration of about 3,000 mg l⁻¹, the proportion of the latter exceed that of the former (halobion index > 50). Corresponding to different conditions of salinization along the river, characteristic diatom assemblages occur differring from each other and which are specific for the river section. Spring and autumn aspects of the diatom assemblages show also salt-dependent differences. The assemblages found in 1998 after decrease of salinization have changed markedly in comparison to those from 1963/64 and 1986. Halobiontic species predominating formerly occurred only occasionally or not at all. They were replaced by oligohalobic-indifferent forms.

An ecological assessment of the changes was performed based on the halobion index calculated from all the samples. For the strongly salinized section of the river Wipper, a shift from -mesohalobic/polyhalobic conditions in 1963/64 and 1986 to -oligohalobic/β-mesohalobic conditions in 1998 was found. However, constant -oligohalobic conditions are still not given. With regard to the transition from -oligohalobic (limnetic) to β-mesohalobic (brackish) conditions, a maximum chloride concentration of 600 mg l⁻¹ was found. To guarantee -oligohalobic conditions, a maximum chloride concentration of 400 mg l⁻¹ should not be exceeded.  相似文献   

Trace metals in acid sediments and waters, Pimpama catchment, southeast Queensland, Australia   总被引：2，自引：1，他引：2  

M. Preda  M. E. Cox 《Environmental Geology》2001,40(6):755-768

The Pimpama River floodplain has developed over the last several thousand years as a result of sea-level fluctuations that shaped the lower catchment and enabled the formation of sedimentary pyrite. The subsequent production of sulfuric acid due to the oxidation of this pyrite enhances the breakdown of metal-bearing sediments and can lead to leaching of major and trace metals into the waters of the region. The seasonal pattern of rainfall and current land-use activities are important aspects that intensify the natural production of acid and influence the release and distribution of metals. To identify the source and migration of metals in the Pimpama catchment and to understand the impact of pyrite oxidation on the distribution of metals in sediments and waters, several components of the drainage system were analyzed: bedrock, sediments from river bed and bank, and water. The elements analyzed in this study (V, Cr, Co, Ni, Cu, Zn and Pb) are all present in the bedrock material which explains their occurrence in the unconsolidated sediments of the floodplain. These metals concentrate in the upper section of the sedimentary sequence and their presence is related to clay minerals such as smectite, organic matter and iron phases. However, Zn, Mo and Co occur in higher amounts than the local background and within standard shale. This comparison suggests that the diagenetic processes alone cannot explain the higher concentrations and it is concluded that these metals also have an anthropogenic source. The formation of sulfuric acid creates conditions for higher mobility of some metals, such as Cr, Co, Ni, Cu, Zn, but does not affect less mobile ones such as Mo and Pb. Over the longterm, the production of acid influences the breakdown of mineral phases and enhances the process of weathering. Over the short term, every rain event leaches acid from sediments and mobilizes metals resulting in a substantial reduction in the quality of river water. Received: 2 October 1998 · Accepted: 16 February 1999  相似文献   

Covariations in oceanic dimethyl sulfide,its oxidation products and rain acidity at Amsterdam Island in the Southern Indian Ocean   总被引：5，自引：0，他引：5  

B. C. Nguyen  N. Mihalopoulos  J. P. Putaud  A. Gaudry  L. Gallet  W. C. Keene  J. N. Galloway 《Journal of Atmospheric Chemistry》1992,15(1):39-53

Simultaneous measurements of rain acidity and dimethyl sulfide (DMS) at the ocean surface and in the atmosphere were performed at Amsterdam Island over a 4 year period. During the last 2 years, measurements of sulfur dioxide (SO₂) in the atmosphere and of methane sulfonic acid (MSA) and non-sea-salt-sulfate (nss-SO₄ ^2-) in rainwater were also performed. Covariations are observed between the oceanic and atmospheric DMS concentrations, atmospheric SO₂ concentrations, wet deposition of MSA, nss-SO₄ ^2-, and rain acidity. A comparable summer to winter ratio of DMS and SO₂ in the atmosphere and MSA in precipitation were also observed. From the chemical composition of precipitation we estimate that DMS oxidation products contribute approximately 40% of the rain acidity. If we consider the acidity in excess, then DMS oxidation products contribute about 55%.  相似文献   

离子色谱法测定五氧化二铌和五氧化二钽中痕量氟氯和硫酸根离子的前处理方法     

刘肖 滕曼蔡亚岐  牟世芬 《岩矿测试》2006,25(4):319-322

采用马弗炉将样品与NaOH混合进行熔融煅烧，热去离子水提取、离心、稀释后过OnGuard Ⅱ H柱和过滤膜进行前处理，抑制型电导离子色谱法检测，测定了Ta2O5和Nb2O5的氟离子、氯离子和硫酸根离子。该方法对三种被测阴离子的检测限（s／N=3）在0．15～0．70μg／g（以固体样品实际浓度计）或0．136～0．623μg／L（以溶液浓度计），标准曲线线性范围均在两个数量级以上，方法的精密度（RSD，n=7）小于5．46％，回收率为88％～106％，具有灵敏度高、选择性好、重现性佳、对环境友好等特点，用于实际样品的检测，结果令人满意。  相似文献   

Sulfate Attack on Concrete in an Inland Salt Lake Environment   总被引：2，自引：0，他引：2  

董荣珍马保国  贺行洋朱洪波 卫军 《中国地质大学学报(英文版)》2006,17(4):342-348

INTRODUCTIONSulfate attack is one of the reasons for concretestructures deteriorating earlier than usual,thusshowing poor durability.The SO42-from the sur-rounding environment such as ocean,saline,groundwater,and even the concrete itself,reacts with thehydration products of cement,whichleads to the de-terioration of the concrete(Li et al.,2000;Kang,1995;Neville,1983;Samarai,1976).The deteriora-tionincludes three processes:the external swelling,cracking,peeling,and disjointing caused by …  相似文献   

察尔汗盐湖盐田渗漏及其工程地质条件分析     

王石军 《化工矿产地质》1998,20(4):301-307

１９８１年以来对察尔汗盐湖三次渗漏试验结果表明,盐田渗漏是盐田土层与外界条件综合作用的结果,在盐田建设和生产管理过程中,应结合不同地点的土层特性、工程地质条件和其它有关条件,采取不同的处理措施。  相似文献   

A Three-Dimensional Global Model Study of Carbonyl Sulfide in the Troposphere and the Lower Stratosphere   总被引：4，自引：0，他引：4  

Erik Kjellström 《Journal of Atmospheric Chemistry》1998,29(2):151-177

Global distributions of carbonyl sulfide and carbon disulfide have been calculated with a three-dimensional global model of the atmospheric general circulation (ECHAM). The model calculates a global sink strength for carbonyl sulfide of 0.3 Tg S yr^-1, with vegetation uptake being the largest sink. With this sink strength, the sources have to be close to the lower limit of the present estimate in the literature. The calculated mixing ratios are higher in the Southern Hemisphere than in the Northern Hemisphere. This interhemispheric gradient is the opposite of what is observed demonstrating that the present knowledge of the distribution of sinks and sources is not fully adequate. The model calculations support the idea that the open oceans could act as a net sink of carbonyl sulfide. The calculated stratospheric photolysis of carbonyl sulfide constitutes about 4% of the total sink of carbonyl sulfide. A stratospheric production of sulfate from carbonyl sulfide of 0.013 Tg S yr^-1 is obtained, which is 3 to 12 times less than what is needed to maintain the stratospheric sulfate aerosol layer. Although these results are associated with uncertainties, due to the low upper boundary and coarse vertical resolution of the model, they support recent findings of a low stratospheric production of sulfate from carbonyl sulfide. Instead, sulfur dioxide transported from the troposphere is calculated to be the most important precursor for the stratospheric sulfate aerosol layer.  相似文献   

中国地区气溶胶的辐射强迫及其气候响应试验   总被引：15，自引：3，他引：12  

胡荣明  石广玉 《大气科学》1998,22(6):917-525

根据国内测定的排放因子数据和国家、部委及各省市统计年鉴公布的排放源数据,得到的中国大陆的1°×1°网格精度的SO2的排放分布,计算了中国地区人为扰动气溶胶的辐射强迫。应用近期开发的二维能量平衡模式计算了由该种气溶胶所引起的中国地区地面温度变化。模式结果表明,最大辐射强迫和最大地面温度变化都集中在中国的沿海和四川地区。最大辐射强迫达3 W/m2。  相似文献