Ultra-stable 3D pyridinium salt-based polymeric network nanotrap for selective 99TcO4-/ReO4- capture via hydrophobic and steric engineering.
Ultra-stable 3D pyridinium salt-based polymeric network nanotrap for selective 99TcO4-/ReO4- capture via hydrophobic and steric engineering.
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DOI：
10.1016/j.jhazmat.2023.131549
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发表时间：
2023-05
影响因子：
13.6
通讯作者：
Wei Xu;Xiu Wang;Yibao Li;Weigang Cui
中科院分区：
文献类型：
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作者：
Wei Xu;Xiu Wang;Yibao Li;Weigang Cui
从高碱性核废料中选择性捕获放射性~（99）TcO ~（4-）对于环境修复和废物处置具有重要意义。然而，具有优异的化学稳定性和对99 TcO 4-的高捕获选择性的吸附剂的组合特征尚未实现。在此，我们报告了一种超稳定的三维吡啶盐基聚合物网络（TMP-TBPM）纳米陷阱，具有显着的辐射，酸和碱稳定性，通过疏水工程和空间位阻选择性捕获ReO 4-，99 TcO 4-的非放射性替代品。批量捕获实验表明，TMP-TBPM具有高捕获容量（918.7 mg g-1）和快速吸附动力学（2 min内去除94.3%），这可归因于3D互连低密度骨架的高度可及孔道上的高密度吡啶鎓盐基单元。此外，在TMP-TBPM的三维骨架中引入大量的烷基和四苯基甲烷单元不仅大大增强了TMP-TBPM的疏水性和稳定性，而且显著提高了TMP-TBPM对99 TcO 4-/ReO 4-的亲和性，即使在高碱性条件下也能实现对99 TcO 4-/ReO 4-的可逆和选择性捕获。该研究显示了三维吡啶盐基聚合物网络纳米捕集器对高碱性核废料中99 TcO 4-/ReO 4-的巨大捕集潜力，为构建高性能阳离子聚合物吸附剂处理放射性废水提供了一种新的策略。
Selective capture of radioactive99TcO4-from highly alkaline nuclear waste is highly desirable for environmental remediation and waste disposal. However, the combined features of adsorbents with excellent chemical stability and high capture selectivity for99TcO4-have not yet been achieved. Herein, we report an ultra-stable 3D pyridinium salt-based polymeric network (TMP-TBPM) nanotrap with remarkable radiation, acid and base stability for selective capture of ReO4-via hydrophobic engineering and steric hindrance, a non-radioactive surrogate of99TcO4-. The batch capture experiments show that TMP-TBPM has high capture capacity (918.7 mg g−1) and fast sorption kinetics (94.3 % removal in 2 min), which can be attributed to the high density of pyridinium salt-based units on the highly accessible pore channels of 3D interconnected low-density skeleton. In addition, the introduction of abundant alkyl and tetraphenylmethane units into the 3D framework not only greatly enhanced the hydrophobicity and stability of TMP-TBPM, but also significantly improved the affinity toward99TcO4-/ReO4-, enabling reversible and selective capture of99TcO4-/ReO4-even under highly alkaline conditions. This study exhibits the great potential of 3D pyridinium salt-based polymeric network nanotrap for99TcO4-/ReO4-capture from highly alkaline nuclear waste, providing a new strategy to construct high-performance cationic polymeric sorbents for radioactive wastewater treatment.