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用于高效选择性回收废水中钯的联吡啶共价有机骨架气凝胶

Bipyridine covalent organic framework aerogel for highly selective recovery of palladium in wastewater.

作者信息

Liu Yang, Guo Weikang, Liu Jiale, Tao Haijuan, Yang Juan, Shuai Qin, Yamauchi Yusuke, Yuliarto Brian, Asakura Yusuke, Huang Lijin

机构信息

State Key Laboratory of Geomicrobiology and Environmental Changes, Faculty of Materials Science and Chemistry, China University of Geosciences No. 388, Lumo Road, Hongshan District Wuhan 430074 PR China

School of Chemistry and Environmental Engineering, Wuhan Institute of Technology LiuFang Campus, No. 206, Guanggu 1st Road, Donghu New & High Technology Development Zone Wuhan 430205 Hubei Province PR China.

出版信息

Chem Sci. 2025 Mar 4;16(13):5745-5754. doi: 10.1039/d4sc08674k. eCollection 2025 Mar 26.

DOI:10.1039/d4sc08674k
PMID:40046080
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11878236/
Abstract

Palladium (Pd), a rare and precious metal, is highly valued due to its non-renewable nature and significant cost. Therefore, recovering palladium from industrial wastewater is of great importance but remains a challenge. Herein, a composite aerogel adsorbent has been developed by linking a bipyridine covalent organic framework, termed TpBpy, with chitosan (CS) through robust covalent bonds. The resulting TpBpy/CS aerogel is employed for the selective separation and recovery of palladium at low concentrations in real wastewater. Experimental results reveal that the maximum adsorption capacity of the TpBpy/CS aerogel for Pd(ii) is 274.4 mg g at pH 1. Additionally, even in the presence of other coexisting ions at concentrations 100 times higher than Pd(ii), the adsorption efficiency for Pd(ii) remains above 99%. Mechanistic investigations indicate that the adsorption of Pd(ii) by the TpBpy/CS aerogels primarily occurs through the coordination between pyridine N and Pd(ii), as well as the electrostatic interaction between protonated amino groups and Pd(ii). Moreover, the TpBpy/CS aerogel demonstrates exceptional reusability, maintaining an adsorption efficiency for Pd(ii) above 99% after nine adsorption-desorption cycles. Overall, the TpBpy/CS aerogel is a promising monolithic adsorbent for the efficient recovery of Pd(ii) from acidic industrial wastewater due to its exceptional adsorption capacity and selectivity, demonstrating substantial potential for practical applications.

摘要

钯(Pd)是一种稀有贵金属,因其不可再生的性质和高昂的成本而备受重视。因此,从工业废水中回收钯至关重要,但仍然是一项挑战。在此,通过将一种称为TpBpy的联吡啶共价有机框架与壳聚糖(CS)通过坚固的共价键连接,开发了一种复合气凝胶吸附剂。所得的TpBpy/CS气凝胶用于实际废水中低浓度钯的选择性分离和回收。实验结果表明,在pH为1时,TpBpy/CS气凝胶对Pd(II)的最大吸附容量为274.4 mg/g。此外,即使存在浓度比Pd(II)高100倍的其他共存离子,对Pd(II)的吸附效率仍保持在99%以上。机理研究表明,TpBpy/CS气凝胶对Pd(II)的吸附主要通过吡啶N与Pd(II)之间的配位作用以及质子化氨基与Pd(II)之间的静电相互作用发生。此外,TpBpy/CS气凝胶表现出优异的可重复使用性,在九个吸附-解吸循环后,对Pd(II)的吸附效率保持在99%以上。总体而言,TpBpy/CS气凝胶因其出色的吸附容量和选择性,是一种从酸性工业废水中高效回收Pd(II)的有前途的整体吸附剂,具有巨大的实际应用潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37b0/11938822/7a0e9bf15994/d4sc08674k-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37b0/11938822/1a7f5f628d41/d4sc08674k-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37b0/11938822/04169b492523/d4sc08674k-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37b0/11938822/c8cc682cfe07/d4sc08674k-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37b0/11938822/900a87270207/d4sc08674k-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37b0/11938822/7a0e9bf15994/d4sc08674k-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37b0/11938822/1a7f5f628d41/d4sc08674k-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37b0/11938822/04169b492523/d4sc08674k-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37b0/11938822/c8cc682cfe07/d4sc08674k-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37b0/11938822/900a87270207/d4sc08674k-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37b0/11938822/7a0e9bf15994/d4sc08674k-f4.jpg

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