腐殖酸与锕系金属离子相互作用的研究进展
Interactions between Humic Acids and Actinides:Recent Advances
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王会 中国科学院核辐射与核能技术重点实验室, 中国科学院高能物理研究所多学科中心, 北京 100049  
柴之芳 中国科学院核辐射与核能技术重点实验室, 中国科学院高能物理研究所多学科中心, 北京 100049  
王东琪* 中国科学院核辐射与核能技术重点实验室, 中国科学院高能物理研究所多学科中心, 北京 100049 dwang@ihep.ac.cn 
摘要: 本文从腐殖酸的结构和存在形式、与锕系金属离子相互作用等两方面简要总结了近年来相关实验和理论研究进展。研究显示,腐殖酸主要通过羧基与锕系离子形成配位复合物,进而影响锕系离子在环境中的迁移。地质环境中的pH、离子强度、矿物表面等都会对腐殖酸与锕系离子的相互作用产生影响,尤以pH的影响最为显著。在较低的pH条件下,腐殖酸的出现一般会促进锕系离子在一些矿物表面的吸附;而在中性或者碱性条件下,则会减弱锕系离子在矿物表面的驻留。腐殖酸对具有氧化活性的锕系离子表现出来的还原性主要来自于还原态的醌式结构单元以及酚羟基。在还原态硫含量较高的腐殖酸中,硫也会参与氧化还原反应。论文还从实验和理论两方面展望了未来腐殖酸与锕系相互作用的研究前景。
关键词: 腐殖酸|金属离子|锕系金属离子|配位化学
基金项目: 国家自然科学基金(No.91026000,91226105);中国科学院百人计划(No.Y2291810S3)资助项目。
Abstract: Recent advances on the experimental and computational studies of interactions between humic acids (HAs) and actinides are briefly reviewed. It appears that HAs are able to form coordination complexes with actinide cations (Ann+) mainly via their carboxylate groups, and as a consequence, influence the migration of Ann+. In geomedia, many factors may affect the interactions between HA and Ann+, including pH, ionic strength, mineral surfaces, among which the effect of pH is the most significant. In general, at low pH, HA may enhance the adsorption of Ann+ on the surface of minerals, while when pH is around or larger than7, HA plays an opposite role. In addition, HAs may reduce high valent oxidative actinide cations, and the reductivity originates from their quinoid and phenol groups. In those HAs with high presence of reduced sulfur, HAs may become more redox sensitive due to the participation of Sin the redox reactions. The paper is concluded with an outlook.
Keywords: humic acids  metallic ions  actinide cations  coordination chemistry
投稿时间:2013-10-09 修订日期:2013-10-28
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王会,柴之芳,王东琪*.腐殖酸与锕系金属离子相互作用的研究进展[J].无机化学学报,2014,30(1):37-52.
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