硫代砷酸根在黄铁矿(001)晶面吸附的第一性原理研究  

First-principles study of adsorption of thioarsenates on(001)surface of pyrite

作　　者：陆成龙 曾祥峰[2] 王少锋 夏德铭 王钰琪 贾永锋[2] LU Chenglong;ZENG Xiangfeng;WANG Shaofeng;XIA Deming;WANG Yuqi;JIA Yongfeng(School of Environmental Science and Technology,Dalian University of Technology,Dalian 116024,China;Shenyang Institute of Applied Ecology,Chinese Academy of Sciences,Shenyang 110016,China)

机构地区：[1]大连理工大学环境学院,辽宁大连116024 [2]中国科学院沈阳应用生态研究所,辽宁沈阳110016

出　　处：《大连理工大学学报》2025年第1期23-29,共7页Journal of Dalian University of Technology

基　　金：国家重点研发计划资助项目(2020YFC1807800);国家自然科学基金资助项目(42173063)。

摘　　要：硫代砷酸根是地下水中重要的砷形态,其在黄铁矿表面的吸附解吸是决定砷迁移性的重要机制.然而,由于硫代砷酸根具有复杂的形态,难以通过实验研究在分子水平理解并预测其在黄铁矿表面的吸附性质.采用密度泛函理论(DFT)计算对不同硫代砷酸根在黄铁矿表面的吸附构型和吸附能开展了研究.结果表明,多种硫代砷酸根能够在黄铁矿(001)晶面上形成多种稳定吸附构型;质子化程度、吸附构型、吸附位点是决定硫代砷酸根在黄铁矿表面吸附性质的重要因素;硫代砷酸根在吸附过程中会发生明显的内部结构变化.研究成果为认清地下水等还原环境中砷形态转化及矿物-水界面吸附解吸机理提供了科学依据.Thioarsenates are important arsenic species in groundwater,and their adsorption and desorption on pyrite surfaces are important mechanisms determining arsenic mobility.However,due to the complex species of thioarsenates,it is difficult to understand and predict their adsorption properties on pyrite surfaces at molecular level through experimental studies.Density functional theory(DFT)calculation is used to investigate the adsorption configurations and energies of different thioarsenates on pyrite surfaces.The results show that various thioarsenates can form multiple stable adsorption configurations on the(001)surface of pyrite.The protonation state,adsorption configuration and adsorption sites are important factors determining the adsorption properties of thioarsenates on pyrite surfaces,and significant internal structural changes occur during the adsorption process.The research findings provide a scientific basis for understanding the transformation of arsenic species and the adsorption and desorption mechanism at the mineral-water interface in reducing environments such as groundwater.

关 键 词：硫代砷酸根 黄铁矿 构型 吸附能 密度泛函理论(DFT)计算 

分 类 号：X51[环境科学与工程—环境工程]