Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2021-03-31 , DOI: 10.1016/j.cej.2021.129546 Qing-Hua Hu , Wei Jiang , Ru-Ping Liang , Sen Lin , Jian-Ding Qiu
Rational design of anion-scavenging materials with high selectivity and stability under high acid/base extreme conditions for removing 99TcO4− is still a significant challenge. Herein, we put forward an anion exchange strategy that utilized an imidazolium-based cationic organic polymer (named ImCOP) for efficient capture of perrhenate (ReO4−), a surrogate for TcO4− with nonradioactive. ImCOP was synthesized via the quaternization reaction using tris (4-(1H-imidazol-1-yl) phenyl) amine, a tripodal flexible ligand, and 1,4-bis (bromomethyl) benzene to forming a semi-rigid structure. ImCOP exhibited high chemical stability even under 3 M HNO3 and 3 M NaOH, which was superior to those of most materials. Attributed to the charged imidazolium moieties and tertiary amine groups that produced rich adsorption sites, ImCOP can produce electrostatic interactions with ReO4−, thereby leading to a record uptake capability (1162 mg g−1) of ReO4−. Furthermore, ImCOP exhibited high selectivity for removing ReO4− in the presence of large excess of competitive anions, which was attributed to the hydrophobic surface of ImCOP. These excellent features endowed ImCOP successfully separated ReO4− from simulated Hanford waste with a high adsorption removal of 93.4%. The excellent performance suggested ImCOP would be a promising material for TcO4−/ReO4− removal, which provided a feasible pathway for designing a high-efficiency and durable material for nuclear-related environmental remediation.
中文翻译:
对于高效和选择性去除REO的咪唑类阳离子有机聚合物的合成4 - / TCO 4 -
以高选择性和稳定性的阴离子清除材料设计合理的高酸/碱极端条件下除去99 TCO 4 -仍然是一个挑战显著。在此,我们提出了用于高铼酸盐的有效捕获的咪唑鎓基阳离子有机聚合物(名为ImCOP)阴离子交换策略(REO 4 - ),用于TCO替代4 -与非放射性。通过使用三(4-(1H-咪唑-1-基)苯基)胺,三脚架柔性配体和1,4-双(溴甲基)苯的季铵化反应合成ImCOP,以形成半刚性结构。ImCOP即使在3 M HNO 3下也显示出高化学稳定性和3 M NaOH,优于大多数材料。归因于产生丰富的吸附位点的带电咪唑部分和叔胺基团,ImCOP可以产生静电相互作用与REO 4 - ,从而导致记录摄取能力(1162毫克克-1 REO的)4 - 。此外,表现出ImCOP高选择性除去REO 4 -在大量过量的竞争阴离子,这归因于ImCOP的疏水表面的存在。这些出色的功能赋予了ImCOP成功分离ReO 4的能力-由模拟的汉福德废料制成,具有93.4%的高吸附去除率。出色的性能提出ImCOP将是TCO有前途的材料4 - / REO 4 -去除,这对于设计高效率和耐用的材料与核有关的环境整治提供了一个可行的途径。