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A combined DFT and molecular dynamics study of U(VI)/calcite interaction in aqueous solution
文献类型：期刊论文
| 作者 | Chai, ZF ; Lan, JH; Shi WQ(石伟群); Chai ZF(柴之芳); Lan JH(蓝建慧); Shi, WQ
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| 刊名 | SCIENCE BULLETIN科学通报
 |
| 出版日期 | 2017 |
| 卷号 | 62期号:15页码:1064-1073 |
| 关键词 | Uranyl Incorporation Adsorption Calcite Density functional theory Molecular dynamics |
| ISSN号 | 2095-9273 |
| DOI | 10.1016/j.scib.2017.07.007 |
| 文献子类 | Article |
| 英文摘要 | Here we present a combined DFT and molecular dynamics study of uranyl (U(VI)) interaction mechanisms with the calcite (104) surface in aqueous solution. The roles of three anion ligands (CO32-, HCO3-, OH-) and solvation effect in U(VI) interaction with calcite have been evaluated. According to our calculations, water adsorbed on the calcite (1 0 4) surface prefers to exist in molecular state rather than dissociative state. Energy analysis indicate that the positively charged uranyl species prefers to form surface complexes on the surface, while neutral uranyl species may bind with the surface via both surface complexing and ion exchange reactions of U(VI) -> Ca(II). In contrast, the negatively charged uranyl species prefer to interact with the surface via ion exchange reactions of U(VI) -> Ca(II), and the one with UO2(CO3)(2)(H2O)(2-) as the reactant becomes the most favorable one in energy. We also found that uranyl adsorption increases the hydrophilic ability of the (104) surface to different extents, where the UO2(CO3)(3)Ca-2 species contributes to the largest degree of energy changes (-53 kcal/mol). Our calculations proved that the (104) surface also has the ability to immobilize U(VI) via either surface complexing or ion exchange mechanisms under different pH values. (C) 2017 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved. |
| 电子版国际标准刊号 | 2095-9281 |
| WOS关键词 | TOTAL-ENERGY CALCULATIONS ; AUGMENTED-WAVE METHOD ; CALCITE SURFACES ; ATOMISTIC SIMULATION ; URANYL ADSORPTION ; WATER INTERFACE ; BASIS-SET ; CARBONATE ; SORPTION ; LUMINESCENCE |
| WOS研究方向 | Science & Technology - Other Topics |
| 语种 | 英语 |
| CSCD记录号 | CSCD:6093380 |
| WOS记录号 | WOS:000409432100008 |
| 源URL | [http://ir.ihep.ac.cn/handle/311005/284988]  |
| 专题 | 高能物理研究所_多学科研究中心 |
| 作者单位 | 中国科学院高能物理研究所 |
| 推荐引用方式 GB/T 7714 | Chai, ZF,Lan, JH,Shi WQ,et al. A combined DFT and molecular dynamics study of U(VI)/calcite interaction in aqueous solution[J]. SCIENCE BULLETIN科学通报,2017,62(15):1064-1073. |
| APA | Chai, ZF,Lan, JH,石伟群,柴之芳,蓝建慧,&Shi, WQ.(2017).A combined DFT and molecular dynamics study of U(VI)/calcite interaction in aqueous solution.SCIENCE BULLETIN科学通报,62(15),1064-1073. |
| MLA | Chai, ZF,et al."A combined DFT and molecular dynamics study of U(VI)/calcite interaction in aqueous solution".SCIENCE BULLETIN科学通报 62.15(2017):1064-1073. |
入库方式： OAI收割
来源：高能物理研究所
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