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从放射性废水到饮用水:阳离子多孔芳香框架高效去除痕量锝酸根/高铼酸根

From Radioactive Effluent to Drinking Water: Efficient Removal of Trace TcO /ReO by Cationic Porous Aromatic Framework.

作者信息

Pang Long-Sheng, Liao Xiangjun, Zhao Chao-Yue, Li Cheng-Peng, Liu Zhong, Ma Shengqian

机构信息

College of Chemistry, Tianjin Key Laboratory of Structure and Performance for Functional Molecules, Tianjin Normal University, Tianjin, 300387, China.

Ningbo Key Laboratory of Agricultural Germplasm Resources Mining and Environmental Regulation, College of Science and Technology, Ningbo University, Ningbo, Zhejiang, 315300, China.

出版信息

Adv Sci (Weinh). 2025 Mar;12(9):e2414604. doi: 10.1002/advs.202414604. Epub 2025 Jan 14.

Abstract

Efficient removal of TcO from radioactive effluents while recovering drinking water remains a challenge. Herein, an excellent ReO (a nonradioactive surrogate of TcO ) scavenger is presented through covalently bonding imidazolium poly(ionic liquids) polymers with an ionic porous aromatic framework (iPAF), namely iPAF-P67, following an adsorption-site density-addition strategy. It shows rapid sorption kinetics, high uptake capacity, and exceptional selectivity toward ReO . Notably, the residual concentration of TcO /ReO in the radioactive wastewater after iPAF-P67 treatment is as low as 0.046 ppb, fully meeting the drinking water standards of World Health Organization (WHO, 0.159 ppb) and United States Environmental Protection Agency (U.S. EPA, 0.053 ppb). Density functional theory (DFT) calculations show that the imidazolium groups in iPAF-P67 provide stronger electrostatic interactions and higher binding energies between iPAF-P67 and TcO anions, leading to its superior adsorption performance. Furthermore, the scale-up synthesized iPAF-P67 materials are shaped with polyethersulfone (PES) to fabricate PAF-P67/PES beads and nanofibers via phase inversion method and electrospinning technique, respectively. Both composites demonstrate outstanding ultra-purification abilities toward ReO to meet the WHO criteria even after multiple dynamic adsorption/desorption cycles. This work develops a design strategy for adsorbents applicable in the sequestration of low-concentration radioactive pollutants.

摘要

在回收饮用水的同时有效去除放射性废水中的TcO仍然是一项挑战。在此,通过将咪唑鎓聚(离子液体)聚合物与离子多孔芳香骨架(iPAF)共价键合,即iPAF-P67,遵循吸附位点密度增加策略,提出了一种优异的ReO(TcO的非放射性替代物)清除剂。它显示出快速的吸附动力学、高吸附容量以及对ReO的卓越选择性。值得注意的是,iPAF-P67处理后的放射性废水中TcO/ReO的残留浓度低至0.046 ppb,完全符合世界卫生组织(WHO,0.159 ppb)和美国环境保护局(U.S. EPA,0.053 ppb)的饮用水标准。密度泛函理论(DFT)计算表明,iPAF-P67中的咪唑鎓基团在iPAF-P67与TcO阴离子之间提供了更强的静电相互作用和更高的结合能,从而导致其优异的吸附性能。此外,通过放大合成的iPAF-P67材料分别与聚醚砜(PES)成型,通过相转化法和静电纺丝技术制备PAF-P67/PES珠粒和纳米纤维。即使经过多次动态吸附/解吸循环,两种复合材料对ReO都表现出出色的超纯化能力,符合WHO标准。这项工作开发了一种适用于封存低浓度放射性污染物的吸附剂设计策略。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bb06/11884533/6a3b4f12d0d5/ADVS-12-2414604-g006.jpg

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