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Ionic Functionalization of Multivariate Covalent Organic Frameworks to Achieve an Exceptionally High Iodine-Capture Capacity
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2021-08-24 , DOI: 10.1002/anie.202108522
Yaqiang Xie 1 , Tingting Pan 1 , Qiong Lei 1 , Cailing Chen 1 , Xinglong Dong 1 , Youyou Yuan 2 , Jie Shen 1 , Yichen Cai 3 , Chunhui Zhou 4 , Ingo Pinnau 1 , Yu Han 1
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Adsorption-based iodine (I2) capture has great potential for the treatment of radioactive nuclear waste. In this study, we apply a “multivariate” synthetic strategy to construct ionic covalent organic frameworks (iCOFs) with a large surface area, high pore volume, and abundant binding sites for I2 capture. The optimized material iCOF-AB-50 exhibits a static I2 uptake capacity of 10.21 g g−1 at 75 °C and a dynamic uptake capacity of 2.79 g g−1 at ≈400 ppm I2 and 25 °C, far exceeding the performances of previously reported adsorbents under similar conditions. iCOF-AB-50 also exhibits fast adsorption kinetics, good moisture tolerance, and full reusability. The promoting effect of ionic groups on I2 adsorption has been elucidated by experimentally identifying the iodine species adsorbed at different sites and calculating their binding energies. This work demonstrates the essential role of balancing the textural properties and binding sites of the adsorbent in achieving a high I2 capture performance.

中文翻译:

多元共价有机框架的离子功能化以实现极高的碘捕获能力

基于吸附的碘 (I 2 ) 捕获在放射性核废料的处理方面具有巨大潜力。在这项研究中,我们应用“多元”合成策略来构建具有大表面积、高孔体积和丰富的 I 2捕获结合位点的离子共价有机框架 (iCOF) 。优化后的材料 iCOF-AB-50在 75 °C 下的静态 I 2吸收能力为 10.21 g g -1,在≈400 ppm I 2 时的动态吸收能力为 2.79 g g -1和 25 °C,远远超过先前报道的吸附剂在类似条件下的性能。iCOF-AB-50 还具有快速吸附动力学、良好的耐湿性和完全可重复使用性。离子基团对I 2吸附的促进作用已经通过实验鉴定吸附在不同位点的碘物质并计算它们的结合能来阐明。这项工作证明了平衡吸附剂的质地特性和结合位点在实现高 I 2捕获性能方面的重要作用。
更新日期:2021-09-27
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