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 | Lan, Jian-Hui1,2; Chai, Zhi-Fang1,2,3,4; Shi, Wei-Qun1,2 |
| 刊名 | Science bulletin
 |
| 出版日期 | 2017-08-15 |
| 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 |
| 通讯作者 | Shi, wei-qun(shiwq@ihep.ac.cn) |
| 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. |
| 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 |
| WOS类目 | Multidisciplinary Sciences |
| 语种 | 英语 |
| WOS记录号 | WOS:000409432100008 |
| 出版者 | SCIENCE PRESS |
| URI标识 | http://www.irgrid.ac.cn/handle/1471x/2177011 |
| 专题 | 高能物理研究所 |
| 通讯作者 | Shi, Wei-Qun |
| 作者单位 | 1.Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China 2.Chinese Acad Sci, Inst High Energy Phys, Key Lab Biomed Effects Nanomat & Nanosafety, Beijing 100049, Peoples R China 3.Soochow Univ, Sch Radiol & Interdisciplinary Sci RAD X, Suzhou 215123, Peoples R China 4.Soochow Univ, Collaborat Innovat Ctr Radiat Med Jiangsu Higher, Suzhou 215123, Peoples R China |
| 推荐引用方式 GB/T 7714 | Lan, Jian-Hui,Chai, Zhi-Fang,Shi, Wei-Qun. A combined dft and molecular dynamics study of u(vi)/calcite interaction in aqueous solution[J]. Science bulletin,2017,62(15):1064-1073. |
| APA | Lan, Jian-Hui,Chai, Zhi-Fang,&Shi, Wei-Qun.(2017).A combined dft and molecular dynamics study of u(vi)/calcite interaction in aqueous solution.Science bulletin,62(15),1064-1073. |
| MLA | Lan, Jian-Hui,et al."A combined dft and molecular dynamics study of u(vi)/calcite interaction in aqueous solution".Science bulletin 62.15(2017):1064-1073. |
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来源：高能物理研究所
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