Theoretical Insights into the Reduction Mechanism of Np(VI) with Phenylhydrazine
文献类型：期刊论文
| 作者 | Li, Xiao-Bo; Wu, Qun-Yan; Wang, Cong-Zhi; Lan, Jian-Hui; Zhang, Meng; Chai, Zhi-Fang; Shi, Wei-Qun |
| 刊名 | JOURNAL OF PHYSICAL CHEMISTRY A
 |
| 出版日期 | 2021 |
| 卷号 | 125期号:28页码:6180-6188 |
| 关键词 | ELECTRON LOCALIZATION ACTINIDE PU ENERGY NP NEPTUNIUM KINETICS IONS THERMOCHEMISTRY BUTYRALDEHYDE |
| 英文摘要 | Effectively adjusting and controlling the valence state of neptunium from the spent fuel reprocessing process is essential to separating neptunium. Hydrazine and its derivatives as free-salt reductants have been experimentally demonstrated to effectively reduce Np(VI) to Np(V). We have theoretically investigated the reduction mechanisms of Np(VI) with hydrazine and three derivatives (HOC2H4N2H3, CH3N2H3, and CHON2H3) in previous works. Herein, we further explored the reduction reaction of Np(VI) with phenylhydrazine (C6H5N2H3) including the free radical ion mechanism and the free radical mechanism. Potential energy profiles (PEPs) indicate that the rate-determining step of both mechanisms is the first stage. Moreover, for the free radical ion mechanism, phenylhydrazine possesses better reduction ability to Np(VI) compared to HOC2H4N2H3, CH3N2H3, and CHON2H3, which falls completely in line with the experimental results. Additionally, the analyses of the quantum theory of atoms in molecules (QTAIM), natural bond orbitals (NBOs), electron localization function (ELF), and localized molecular orbitals (LMOs) have been put forward to elucidate the bonding evolution for the structures of the reaction pathways. This work offers insights into the reduction mechanism of Np(VI) with phenylhydrazine from the theory point of view and contributes to design more high-efficiency reductants for the separation of U/Np and Np/Pu in spent fuel reprocessing. |
| 源URL | [http://ir.nimte.ac.cn/handle/174433/21723]  |
| 专题 | 中国科学院宁波材料技术与工程研究所 2021专题_期刊论文 |
| 作者单位 | 1.Zhang, M (corresponding author), Harbin Engn Univ, Fundamental Sci Nucl Safety & Simulat Technol Lab, Coll Nucl Sci & Technol, Harbin 150001, Heilongjiang, Peoples R China. 2.Wu, QY 3.Shi, WQ (corresponding author), Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China. |
| 推荐引用方式 GB/T 7714 | Li, Xiao-Bo,Wu, Qun-Yan,Wang, Cong-Zhi,et al. Theoretical Insights into the Reduction Mechanism of Np(VI) with Phenylhydrazine[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2021,125(28):6180-6188. |
| APA | Li, Xiao-Bo.,Wu, Qun-Yan.,Wang, Cong-Zhi.,Lan, Jian-Hui.,Zhang, Meng.,...&Shi, Wei-Qun.(2021).Theoretical Insights into the Reduction Mechanism of Np(VI) with Phenylhydrazine.JOURNAL OF PHYSICAL CHEMISTRY A,125(28),6180-6188. |
| MLA | Li, Xiao-Bo,et al."Theoretical Insights into the Reduction Mechanism of Np(VI) with Phenylhydrazine".JOURNAL OF PHYSICAL CHEMISTRY A 125.28(2021):6180-6188. |
入库方式： OAI收割
来源：宁波材料技术与工程研究所
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