物理化学学报 >> 2011, Vol. 27 >> Issue (01): 59-64.doi: 10.3866/PKU.WHXB20110107

理论与计算化学 上一篇    下一篇

铀酰离子吸附在高岭土基面的分子动力学模拟

刘晓宇, 黎春, 田文宇, 陈涛, 王路化, 郑仲, 朱建波, 孙茂, 刘春立   

  1. 北京大学化学与分子工程学院, 应用化学研究所, 北京分子科学国家实验室, 北京100871
  • 收稿日期:2010-07-06 修回日期:2010-10-19 发布日期:2010-12-31
  • 通讯作者: 刘春立 E-mail:liucl@pku.edu.cn
  • 基金资助:

    国家自然科学基金(10775008), 教育部博士点基金(20060001032), 国防科工委军工遗留专项基金(科工计[2007]840), 中央高校基本科研业务费专项资金和北京大学仪器测试基金(第13 至18 期)资助项目

Molecular Dynamics Modeling of Uranyl Ion Adsorption onto the Basal Surfaces of Kaolinite

LIU Xiao-Yu, LI Chun, TIAN Wen-Yu, CHEN Tao, WANG Lu-Hua, ZHENG Zhong, ZHU Jian-Bo, SUN Mao, LIU Chun-Li   

  1. Beijing National Laboratory for Molecular Sciences, Department of Applied Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China
  • Received:2010-07-06 Revised:2010-10-19 Published:2010-12-31
  • Contact: LIU Chun-Li E-mail:liucl@pku.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (10775008), Research Fund for Ph.D Program of the Ministry of Education, China (20060001032), Special Foundation for High LevelWaste Disposal, China (2007-840), Fundamental Research Funds for the Central Universities, China, and Analysis Foundation (13-18) of Peking University, China.

摘要:

为研究铀酰离子在高岭土不同基面上的吸附, 对含有0.01 mol·L-1碳酸铀酰液相和9×9×3个高岭土单胞的粘土固相的模拟盒子进行了分子动力学模拟. 从模拟的截图中直观地观察到了铀酰离子的吸附位点, 由径向分布函数得到了铀酰离子与水中氧原子的配位情况. 利用原子密度剖面图讨论铀酰离子在两个基面上的吸附倾向, 并从原子密度剖面图和均方位移等角度证实了铀酰离子在硅氧面上形成了外界配合物. 从理论上证明了表面配合模型对于吸附位点所做简化的合理性.

关键词: 分子动力学模拟, 高岭土, 铀酰离子, 吸附

Abstract:

We performed a molecular dynamics simulation to investigate the adsorption of uranyl ions onto the basal surfaces of kaolinite using a simulation cell containing 0.01 mol?L-1 uranyl carbonate and 9× 9×3 kaolinite unit cells. The adsorption sites of the uranyl ions on kaolinite were clearly shown by serial snapshots and the coordination of uranyl ions to oxygen were determined using a radial distribution function. The adsorption trends of uranyl ions on two distinct basal surfaces were discussed using an atomic density profile. Outer-sphere complexation of uranyl on kaolinite was confirmed using the atomic density profile and the mean squared displacement. Confirmation of the outer-sphere complexation supports the theoretical simplification of the adsoption sites in the surface complexation model.

Key words: Molecular dynamics simulation, Kaolinite, Uranyl ion, Adsorption

MSC2000: 

  • O641