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掺钴水钠锰矿对铅的吸附及对砷的氧化
引用本文:殷辉,冯雄汉,邱国红,谭文峰,刘凡. 掺钴水钠锰矿对铅的吸附及对砷的氧化[J]. 环境科学, 2011, 32(7): 2092-2101
作者姓名:殷辉  冯雄汉  邱国红  谭文峰  刘凡
作者单位:华中农业大学农业部亚热带农业资源与环境重点开放实验室,武汉,430070
基金项目:国家自然科学基金项目(40771102,40830527);全国优秀博士学位论文作者专项 (200767);新世纪优秀人才支持计划项目(NCET-09-0399)
摘    要:为了研究过渡金属离子掺杂对锰氧化物作为环境友好材料物理化学性质的影响,在浓盐酸还原高锰酸钾制备水钠锰矿过程中添加氯化钴,在常压回流条件下一步合成了三维纳米微球状水钠锰矿,考察了其铅吸附和砷氧化能力.应用粉晶X射线衍射、化学分析、N2物理吸附、场发射扫描电镜(FE-SEM)、X射线光电子能谱(XPS)等手段表征产物晶体结...

关 键 词:二氧化锰  水钠锰矿  钴掺杂  铅吸附  砷氧化  X射线光电子能谱
收稿时间:2010-07-18
修稿时间:2010-08-25

Lead Adsorption and Arsenite Oxidation by Cobalt Doped Birnessite
YIN Hui,FENG Xiong-han,QIU Guo-hong,TAN Wen-feng and LIU Fan. Lead Adsorption and Arsenite Oxidation by Cobalt Doped Birnessite[J]. Chinese Journal of Environmental Science, 2011, 32(7): 2092-2101
Authors:YIN Hui  FENG Xiong-han  QIU Guo-hong  TAN Wen-feng  LIU Fan
Affiliation:Key Laboratory of Subtropical Agriculture Resource and Environment, Ministry of Agriculture, Huazhong Agricultural University, Wuhan 430070, China. yinhui666@126.com
Abstract:In order to study the effects of transition metal ions on the physic-chemical properties of manganese dioxides as environmental friendly materials, three-dimensional nano-microsphere cobalt-doped birnessite was synthesized by reduction of potassium permanganate by mixtures of concentrated hydrochloride and cobalt (II) chloride. Powder X-ray diffraction, chemical analysis, N2 physical adsorption, field emission scanning electron microscopy (FE-SEM) and X-ray photoelectron spectra (XPS) were used to characterize the crystal structure, chemical composition and micro-morphologies of products. In the range of molar ratios from 0.05 to 0.20, birnessite was fabricated exclusively. It was observed that cobalt incorporated into the layers of birnessite and had little effect on the crystal structure and micromorpholgy, but crystallinity decreased after cobalt doping. Both chemical analysis and XPS results showed that manganese average oxidation state decreased after cobalt doping, and the percentage of Mn3+ increased. Co(III) OOH existed mainly in the structure. With the increase of cobalt, hydroxide oxygen percentage in molar increased from 12.79% for undoped birnessite to 13.05%, 17.69% and 17.79% for doped samples respectively. Adsorption capacity for lead and oxidation of arsenite of birnessite were enhanced by cobalt doping. The maximum capacity of Pb2+ adsorption increased in the order HB (2 538 mmol/kg) < CoB5 (2798 mmol/kg) < CoB10 (2932 mmol/kg) < CoB20 (3 146 mmol/kg). Oxidation percentage of arsenite in simulated waste water by undoped birnessite was 76.5%, those of doped ones increased by 2.0%, 12.8% and 18.9% respectively. Partial of Co3+ substitution for Mn4+ results in the increase of negative charge of the layer and the content of hydroxyl group, which could account for the improved adsorption capacity of Pb2+. After substitution of manganese by cobalt, oxidation capacity of arsenite by birnessite increases likely due to the higher standard redox potential of Co3+/Co2+ than those of Mn4+/Mn3+/Mn2+. Therefore, Co-doped birnessite is more applicable for the remediation of water polluted with heavy metal ions, implying new methods of modification of manganese dioxides in practice.
Keywords:manganese dioxide   birnessite   cobalt doping   lead adsorption   arsenite oxidation   X-ray photoelectron spectroscopy
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