2,2′-((4-乙氧基-1,2-亚苯基)双(氧基))双(N,N-双(2-乙基己基)乙酰胺)对U(Ⅵ)、Pu(Ⅳ)的萃取行为研究

doi:10.7538/tws.2021.youxian.107

摘要/Abstract

摘要： 为开发Pu(Ⅳ)的高选择性萃取剂，实现废液中微量钚的回收，以正十二烷作为稀释剂，研究2,2′-((4-乙氧基-1,2-亚苯基)双(氧基))双(N,N-双(2-乙基己基)乙酰胺)(4-EthoxyBenzoDODA)对U(Ⅵ)、Pu(Ⅳ)的萃取行为，以及两相混合振荡时间、水相硝酸浓度和有机相萃取剂浓度对U(Ⅵ)、Pu(Ⅳ)萃取分配比的影响。硝酸的萃取实验结果表明，4-EthoxyBenzoDODA(KH=0.14)比BenzoDODA(KH=0.44)碱性弱，更有利于选择萃取离子势较强的Pu(Ⅳ)。对U(Ⅵ)、Pu(Ⅳ)的萃取实验表明，Pu(Ⅳ)对U(Ⅵ)的分离因子最高可达6.9，Pu(Ⅳ)对Eu(Ⅲ)的分离因子最高可达223。采用斜率法分析了4.0 mol/L HNO₃浓度下U(Ⅵ)萃合物的组成，主要为UO₂(NO₃)₂·L)、Pu(Ⅳ)(Pu(NO₃)₄·L和Pu(NO₃)₄·L2共存。使用硝酸肼或者硝酸羟胺等还原反萃剂，可以将负载有机相中98%的Pu反萃至水相中。结果表明，4-EthoxyBenzoDODA对Pu(Ⅳ)具有一定的选择性。

关键词: 铀, 钚, 选择性萃取剂, 分离因子

Abstract: To develop a highly selective extractant for Pu(Ⅳ), 2,2′-((4-ethoxy-1,2-phenylene)bis(oxy)) bis (N,N-bis(2-ethylhexyl)acetamide), short for 4-EthoxyBenzoDODA, has been evaluated as a novel extractant in n-dodecane diluent for the extraction of U(Ⅵ) and Pu(Ⅳ). The effect of contact time of two phases, HNO₃ concentration and extractant concentration on the distribution ratios of U(Ⅵ) and Pu(Ⅳ) was investigated. Acid uptake studies suggested that 4-EthoxyBenzoDODA (KH=0.14) was less basic as compared to BenzoDODA (KH=0.44), making it more conducive to selectively extract Pu(Ⅳ) with stronger ionic potential. Extraction experiments showed that the maximum of SFPu/U, SFPu/Eu were 6.9, 223 respectively. Slope analysis indicated extraction of 1∶1 (ML) species with U(Ⅵ) and mixed 1∶1 (ML) and 1∶2 (ML2) species with Pu(Ⅳ) at 4.0 mol/L HNO₃ 98% of Pu in the loaded organic phase can be stripped to the aqueous phase using reductive stripping agent such as hydrazine nitrate and hydroxylamine nitrate. The results showed that the 4-EthoxyBenzoDODA exhibited good selectivity toward Pu.

Key words: uranium, plutonium, selective extractant, separation factor

丁琪秀, 葛晓, 朱浩玮, 陈琦, 吕洪彬, 郑卫芳, 晏太红. 2,2′-((4-乙氧基-1,2-亚苯基)双(氧基))双(N,N-双(2-乙基己基)乙酰胺)对U(Ⅵ)、Pu(Ⅳ)的萃取行为研究[J]. 同位素, 2022, 35(5): 415-423.

DING Qixiu, GE Xiao, ZHU Haowei, CHEN Qi, LYU Hongbin, ZHENG Weifang, YAN Taihong. Liquid-liquid Extraction of U(Ⅵ) and Pu(Ⅳ) with 2,2′-((4-Ethoxy-1,2-phenylene) bis (oxy)) bis (N,N-bis(2-ethylhexyl)acetamide)[J]. Journal of Isotopes, 2022, 35(5): 415-423.

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