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席夫碱型阳离子共价有机聚合物对99TcO-4化学替代物ReO-4的高效吸附分离
引用本文:何林玮,白尧尧,李坤锋,林鹏,刘夏杰,李杰,陈俊畅,张朵,张明星,马付银,陈龙,王殳凹.席夫碱型阳离子共价有机聚合物对99TcO-4化学替代物ReO-4的高效吸附分离[J].核化学与放射化学,2020,42(6):563-572.
作者姓名:何林玮  白尧尧  李坤锋  林鹏  刘夏杰  李杰  陈俊畅  张朵  张明星  马付银  陈龙  王殳凹
作者单位:苏州大学 放射医学与辐射防护国家重点实验室,江苏 苏州215123;中广核研究院有限公司,广东 深圳518028
摘    要:高锝酸根(TcO-4)的裂变产额高、环境迁移能力强、半衰期长,高效分离去除TcO-4在放射性环境治理和乏燃料后处理过程中具有重要意义。然而目前只有少数材料可以从水溶液体系中吸附TcO-4,研发动力学快和耐酸性的吸附材料仍然具有挑战。为此,通过席夫碱反应合成了两种阳离子共价有机聚合物材料(BPA-TAB-Cl和BPA-TAE-Cl)吸附ReO-4(TcO-4的非放射性类似物)。两种材料均具有超快的吸附动力学,几乎可以定量地在20 s内去除溶液中的ReO-4。即使在pH=2溶液中,材料的吸附能力也没有受到明显影响。在溶液中NO-3浓度超过ReO-4浓度100倍的情况下,两种材料也可以分别去除84%和79%的ReO-4,显示出优异的吸附选择性。在四次吸附-解吸循环之后,两种材料的吸附能力几乎没有变化。最后,吸附机理证实阴离子交换后两种材料中均存在ReO-4。结果表明,利用共价有机聚合物去除放射性污染物具有广阔前景。

关 键 词:吸附剂  阳离子共价有机聚合物  离子交换  席夫碱  

Schiff Base Cationic Covalent Organic Polymers for Highly Effective Removal of ReO4-:a Chemical Analogue of 99TcO4-
HE Lin-wei,BAI Yao-yao,LI Kun-feng,LIN Peng,LIU Xia-jie,LI Jie,CHEN Jun-chang,ZHANG Duo,ZHANG Ming-xing,MA Fu-yin,CHEN Long,WANG Shu-ao.Schiff Base Cationic Covalent Organic Polymers for Highly Effective Removal of ReO4-:a Chemical Analogue of 99TcO4-[J].Journal of Nuclear and Radiochemistry,2020,42(6):563-572.
Authors:HE Lin-wei  BAI Yao-yao  LI Kun-feng  LIN Peng  LIU Xia-jie  LI Jie  CHEN Jun-chang  ZHANG Duo  ZHANG Ming-xing  MA Fu-yin  CHEN Long  WANG Shu-ao
Affiliation:State Key Laboratory of Radiation Medicine and Protection, Soochow University, Suzhou 215123, China;China Nuclear Power Technology Research Institute Co., Ltd, Shenzhen 518028, China
Abstract:Highly remediation of TcO-4 from used nuclear fuel reprocessing and radioactive environmental governance is of great significance for its high fission yield, environmental mobility and long half-life. Only a handful of materials can extract TcO-4 from aqueous solution and solid sorbent materials with fast kinetics and acid tolerance are still highly desirable. Herein, two cationic covalent organic polymers (BPA-TAB-Cl and BPA-TAE-Cl) was synthesized for the extraction of ReO-4, a non-radioactive chemical analogue of TcO-4. Both materials exhibit ultra-fast adsorption kinetics and almost quantitative ReO-4 can be removed within 20 s. In pH=2 water solution, the extraction capability is not obviously affected. Even in 100-fold exceed NO-4 solution, both cationic networks can capture 84% and 79% of ReO-4 respectively, indicating the excellent adsorption selectivity. After four sorption-desorption cycles, the adsorption capabilities have no obvious change. Finally, investigations of mechanism undoubtedly indicate that ReO-4 exists in both materials after anion exchange. Our results display bright prospect to eliminate radioactive contaminants by porous organic polymers.
Keywords:adsorbent  cationic covalent organic polymers  anion-exchange  Schiff base  
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