Effect of H2O on the hydrolysis of UF6 in the gas phase
文献类型：期刊论文
| 作者 | Hu, Shao-Wen; Lin, Hao; Wang, Xiang-Yun; Chu, Tai-Wei |
| 刊名 | JOURNAL OF MOLECULAR STRUCTURE
 |
| 出版日期 | 2014-03-24 |
| 卷号 | 1062页码:29-34 |
| 关键词 | Uranium Hexafluoride Hydrolysis Relativistic Density Functional Theory Calculation Water Catalysis Mechanism |
| ISSN号 | 0022-2860 |
| DOI | 10.1016/j.molstruc.2014.01.015 |
| 英文摘要 | In our previous works (Hu et al., 2008, 2009), we found the theoretical evidence that indicates UF5OH is an intermediate produced in the first step of UF6 hydrolysis, UF6 + H2O. When UF6/H2O ratio is high, UF5OH may react with UF6 or another UF5OH, forming species containing U-O-U bond. In this work, we considered another situation - the hydrolysis of UF6 in excess of H2O, and explored the probable initial reactions of UF6 + 2H(2)O and UF6 + 3H(2)O systems using the same relativistic density functional theory calculations. Water molecules may form dimer or trimer and then coordinate with UF6, forming complexes UF6 center dot 2H(2)O or UF6 center dot 3H(2)O, which are more stable than UF6 center dot H2O. Compared to the conversion UF6 center dot H2O -> UF5 OH center dot HF, the energy barriers of reactions UF6 center dot 2H(2)O -> UF5OH center dot H2O center dot HF and UF6 center dot 3H(2)O -> UF5OH center dot 2H(2)O center dot HF are 4 and 6 kcal/mol lower respectively. The additional H2O molecules catalyze the reactions by bridging the hydrogen which transfers from ligand H2O to F and stabilizes the transition states. In addition, as water content increases, the reaction step UF6 + 3H(2)O becomes exothermic and the products-HF, UF5 OH and two H2O molecules-tend to bond tightly into a stable complex. (C) 2014 Elsevier B.V. All rights reserved. |
| 语种 | 英语 |
| WOS记录号 | WOS:000333490200004 |
| 出版者 | ELSEVIER SCIENCE BV |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/50361]  |
| 专题 | 中国科学院化学研究所 |
| 通讯作者 | Hu, Shao-Wen |
| 作者单位 | Peking Univ, Beijing Natl Lab Mol Sci, Radiochem & Radiat Chem Key Lab Fundamental Sci, Coll Chem & Mol Engn, Beijing 100871, Peoples R China |
| 推荐引用方式 GB/T 7714 | Hu, Shao-Wen,Lin, Hao,Wang, Xiang-Yun,et al. Effect of H2O on the hydrolysis of UF6 in the gas phase[J]. JOURNAL OF MOLECULAR STRUCTURE,2014,1062:29-34. |
| APA | Hu, Shao-Wen,Lin, Hao,Wang, Xiang-Yun,&Chu, Tai-Wei.(2014).Effect of H2O on the hydrolysis of UF6 in the gas phase.JOURNAL OF MOLECULAR STRUCTURE,1062,29-34. |
| MLA | Hu, Shao-Wen,et al."Effect of H2O on the hydrolysis of UF6 in the gas phase".JOURNAL OF MOLECULAR STRUCTURE 1062(2014):29-34. |
入库方式： OAI收割
来源：化学研究所
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