氮杂多环芳烃/离子液体萃取体系的伽马辐射效应  

Gamma Radiation Effect on Heterocyclic N-Donor Ligands in Ionic Liquids

作　　者：王月[1] 敖银勇[1,2] 袁威津 彭静[1] 李久强[1] 赵龙 翟茂林[1] WANG Yue;AO Yin-yong;YUAN Wei-jin;PENG Jing;LI Jiu-qiang;ZHAO Long;ZHAI Mao-lin(College of Chemistry and Molecular Engineering,Peking University,Radiochemistry and Radiation Chemistry Key Laboratory of Fundamental Science,Beijing National Laboratory for Molecular Science,Beijing 100871,China;Institute of Nuclear Physics and Chemistry,China Academy of Engineering Physics,Mianyang 621999,China;State Key Laboratory of Advanced Electromagnetic Engineering and Technology,School of Electrical and Electronic Engineering,Huazhong University of Science and Technology,Wuhan 430074,China)

机构地区：[1]北京大学化学与分子工程学院,放射化学与辐射化学重点学科实验室,北京分子科学国家研究中心,北京100871 [2]中国工程物理研究院核物理与化学研究所,四川绵阳621999 [3]华中科技大学电气与电子工程学院,强电磁工程与新技术国家重点实验室,湖北武汉430074

出　　处：《核化学与放射化学》2020年第6期549-555,共7页Journal of Nuclear and Radiochemistry

基　　金：国家自然科学基金项目(91126014,11475112)。

摘　　要：乏燃料后处理分离体系的辐射稳定性是其实际应用前需解决的重要问题。采用傅里叶变换红外光谱(FTIR)、超高效液相色谱/四级杆飞行时间质谱联用(UPLC/Q-TOF-MS)等方法系统研究了IB-BTP/[C2mim][NTf2]、CA-BTP/[C2mim][NTf2]和CA-BTPhen/[C2mim][NTf2]三种典型的氮杂多环芳烃/离子液体萃取分离体系的γ辐射效应,并通过Eu^3+萃取实验对辐照前后体系的萃取性能变化进行了对比。结果表明:三种萃取剂在[C2mim][NTf2]离子液体中的辐射稳定性顺序为:CA-BTP>IB-BTP≈CA-BTPhen;三种体系的辐解产物主要为[C2mim][NTf2]离子液体辐解产生的·CF3、·[C2mim]^+、·H等自由基进攻氮杂多环芳烃后生成的取代产物;即使在300 kGy的条件下,三种体系仍保持了较好的萃取能力。The radiation stability of separation systems for spent nuclear fuel reprocessing is an important problem to be solved before their practical use. In this work, the γ radiation effects on three commonly used heterocyclic N-donor ligands in ionic liquids(IB-BTP/[C2mim][NTf2], CA-BTP/[C2mim][NTf2] and CA-BTPhen/[C2mim][NTf2]) were systematically studied by using Fourier transform infrared spectroscopy(FTIR) and ultra-high performance liquid chromatography/quadrupole time-of-flight mass spectrometry(UPLC/Q-TOF-MS). The changes in extraction performance of Eu3+ before and after irradiation were also compared. The results show that in the presence of [C2mim][NTf2] ionic liquid, the order of the radiation stability of the three extracting agents is CA-BTP>IB-BTP≈CA-BTPhen;the main radiolysis products of the three systems are substitution products formed by heterocyclic N-donor ligands and radicals from [C2mim][NTf2] ionic liquids(·CF3, ·[C2mim]^+, ·H, etc.). Even at an absorbed dose of up to 300 kGy, good extraction performances are still maintained.

关 键 词：氮杂多环芳烃 离子液体 乏燃料后处理 辐射效应 

分 类 号：O644.22[理学—物理化学]