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水锰矿氧化水溶性硫化物过程及其影响因素
引用本文:罗瑶,李珊,谭文峰,刘凡,蔡崇法,邱国红.水锰矿氧化水溶性硫化物过程及其影响因素[J].环境科学,2016,37(4):1539-1545.
作者姓名:罗瑶  李珊  谭文峰  刘凡  蔡崇法  邱国红
作者单位:华中农业大学资源与环境学院, 农业部长江中下游耕地保育重点实验室, 武汉 430070;华中农业大学资源与环境学院, 农业部长江中下游耕地保育重点实验室, 武汉 430070;华中农业大学资源与环境学院, 农业部长江中下游耕地保育重点实验室, 武汉 430070;华中农业大学资源与环境学院, 农业部长江中下游耕地保育重点实验室, 武汉 430070;华中农业大学资源与环境学院, 农业部长江中下游耕地保育重点实验室, 武汉 430070;华中农业大学资源与环境学院, 农业部长江中下游耕地保育重点实验室, 武汉 430070
基金项目:国家自然科学基金项目(41171375,41571228); 教育部新世纪优秀人才计划项目(NCET-12-0862); 霍英东教育基金会高等院校青年教师基金项目(141024); 湖北省自然科学基金项目(2012FFA031,2014CFA016); 中央高校基本科研业务费专项(2662015JQ002,2013PY029,2013PY030)
摘    要:作为表生环境中易生成且分布广泛的氧化锰矿物,水锰矿参与水溶性硫化物的氧化反应,影响其迁移、转化和归趋.本研究考察了水锰矿氧化水溶性硫化物(S~(2-))的过程与产物,探讨了初始pH、氧气对反应速率与中间产物的影响,X-射线衍射仪(XRD)、傅里叶变换红外光谱仪(FTIR)和透射电镜(TEM)表征水锰矿与水溶性硫化物反应固相产物晶体结构、组分和微观形貌;分光光度计、高效液相色谱仪和离子色谱仪分析S~(2-)及其氧化物的浓度与变化趋势.结果表明水锰矿氧化S~(2-)产物主要为单质S,起始pH降低可加速S~(2-)的初始氧化反应,对产物组成并无显著影响;有氧环境中单质S会进一步氧化生成S_2O_3~(2-),且水锰矿表现出良好的催化作用与化学稳定性,反应约10 h,晶体结构保持稳定.

关 键 词:水锰矿  水溶性硫化物  pH  氧化还原  催化
收稿时间:2015/10/5 0:00:00
修稿时间:2015/11/16 0:00:00

Oxidation Process of Dissolvable Sulfide by Manganite and Its Influencing Factors
LUO Yao,LI Shan,TAN Wen-feng,LIU Fan,CAI Chong-fa and QIU Guo-hong.Oxidation Process of Dissolvable Sulfide by Manganite and Its Influencing Factors[J].Chinese Journal of Environmental Science,2016,37(4):1539-1545.
Authors:LUO Yao  LI Shan  TAN Wen-feng  LIU Fan  CAI Chong-fa and QIU Guo-hong
Institution:Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture, College of Resources and Environment, Huazhong Agricultural University, Wuhan 430070, China;Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture, College of Resources and Environment, Huazhong Agricultural University, Wuhan 430070, China;Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture, College of Resources and Environment, Huazhong Agricultural University, Wuhan 430070, China;Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture, College of Resources and Environment, Huazhong Agricultural University, Wuhan 430070, China;Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture, College of Resources and Environment, Huazhong Agricultural University, Wuhan 430070, China;Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River), Ministry of Agriculture, College of Resources and Environment, Huazhong Agricultural University, Wuhan 430070, China
Abstract:As one of the manganese oxides, which are easily generated and widely distributed in supergene environment, manganite participates in the oxidation of dissolvable sulfide (S2-), and affects the migration, transformation, and the fate of sulfides. In the present work, the redox mechanism was studied by determining the intermediates, and the influence of initial pH and oxygen atmosphere on the processes were studied. The chemical composition, crystal structures and micromorphologies were characterized by XRD, FTIR and TEM. The concentration of S2- and its oxidation products were analyzed using spectrophotometer, high performance liquid chromatograph and ion chromatograph. The results indicated that elemental sulfur was formed as the major oxidation product of S2- oxidation, and decreased pH could accelerate the oxidation rate of S2- in the initial stage, however, there was no significant influence on final products. Elemental S could be further oxidized to S2O32- when the reaction system was bubbled with oxygen, and manganite exhibited excellent catalytic performance and chemical stability during the oxidation of dissolvable sulfide by oxygen. After reaction of more than 10 h, the crystal structure of manganite remained stable.
Keywords:manganite  dissolvable sulfide  pH  redox  catalysis
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