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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

    Schiff Base Cationic Covalent Organic Polymers for Highly Effective Removal of ReO-4: a Chemical Analogue of 99TcO-4

      摘要
    • 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。

       

      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.

       

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