Rational design of a cationic polymer network towards record high uptake of ^(99)TcO_(4)^(-)in nuclear waste  

作　　者：Jie Li Long Chen Nannan Shen Rongzhen Xie Matthew VSheridan Xijian Chen Daopeng Sheng Duo Zhang Zhifang Chai Shuao Wang 

机构地区：[1]State Key Laboratory of Radiation Medicine and Protection,School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions,Soochow University,Suzhou 215123,China [2]Institute of Nuclear Science and Technology,Sichuan University,Chengdu 610064,China

出　　处：《Science China Chemistry》2021年第7期1251-1260,共10页中国科学（化学英文版）

基　　金：supported by the National Natural Science Foundation of China(21790374,21825601,21806117,21906114,22006108);the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD);the National Key R&D Program of China(2018YFB1900203)。

摘　　要：^(99)Tc is a long-lived radionuclide present in large amounts as TcO_(4)^(-)-anion in used nuclear fuel.Its removal from the waste stream is highly desirable because of its interference capability with actinide separation and its volatile nature during the nuclear waste vitrification process.Despite the progress achieved in the past few years,the design of anion-exchange materials with optimized Tc uptake property and improved stability under the extreme condition is still a research goal beneficial for reducing the volume of secondary radioactive solid waste generated during the waste partitioning process.However,their design philosophy remains elusive,with challenges coming from charge repulsion,steric hindrance,and insufficient reactive sites within the materials.Herein,we present a design philosophy of cationic polymer network materials for TcO_(4)^(-)separation by systematic precursor screening and structure prediction.This affords an optimized material,SCU-CPN-2(SCU=Soochow University),with extremely high positive charge density while maintaining high radiation resistance.SCU-CPN-2 exhibits a record high adsorption capacity1,467 mg/g towards the surrogate ReO_(4)^(-)compared to all anion-exchange materials reported up to date.In addition to ultrafast adsorption kinetics,SCU-CPN-2 has remarkable selectivity over nitrate and sulfate,and facile recyclability.

关 键 词：PERTECHNETATE PERRHENATE adsorption adsorption capacity cationic organic polymer 

分 类 号：TL94[核科学技术—辐射防护及环境保护] TQ317[化学工程—高聚物工业]