Flexible three-dimensional covalent organic frameworks for ultra-fast and selective extraction of uranium via hydrophilic engineering

Xiao-Juan Chen; Cheng-Rong Zhang; Xin Liu; Jia-Xin Qi; Wei Jiang; Shun-Mo Yi; Cheng-Peng Niu; Yuan-Jun Cai; Ru-Ping Liang; Jian-Ding Qiu

doi:10.1016/j.jhazmat.2022.130442

Flexible three-dimensional covalent organic frameworks for ultra-fast and selective extraction of uranium via hydrophilic engineering

J Hazard Mater. 2023 Mar 5:445:130442. doi: 10.1016/j.jhazmat.2022.130442. Epub 2022 Nov 22.

Authors

Affiliations

¹ College of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, China.
² College of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, China. Electronic address: rpliang@ncu.edu.cn.
³ College of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, China; State Key Laboratory of Nuclear Resources and Environment, East China University of Technology, Nanchang 330013, China. Electronic address: jdqiu@ncu.edu.cn.

PMID: 36436454
DOI: 10.1016/j.jhazmat.2022.130442

Abstract

It has been considered challenging to develop ideal adsorbents for efficient and lower adsorption time uranium extraction, especially 3D covalent organic frameworks with interpenetrating topologies and tunable porous structures. Here, a "soft" three-dimensional (3D) covalent organic framework (TAM-DHBD) with a fivefold interpenetrating structure is prepared as a novel porous platform for the efficient extraction of radioactive uranium. The resultant TAM-DHBD appears exceptional crystallinity, prominent porosity and excellent chemical stability. Based on the strong mutual coordination between phenolic-hydroxyl/imine-N on the main chain and uranium, TAM-DHBD can effectively avert the competition of other ions, showing high selectivity for uranium extraction. Impressively, the 3D ultra-hydrophilic transport channels and multi-directional uniform pore structure of TAM-DHBD lay the foundation for the ultra-high-speed diffusion of uranium (the adsorption equilibrium can be reached within 60 min under a high-concentration environment). Furthermore, the utilization of lightweight structure not only increases the adsorption site density, but renders the adsorption process flexible, achieving a breakthrough adsorption capacity of 1263.8 mg g^-1. This work not only highlights new opportunities for designing microporous 3D COFs, but paves the way for the practical application of 3D COFs for uranium adsorption.

Keywords: Adsorption; Covalent organic frameworks; Hydrophilic; Three-dimensional structure; UO(2)(2+).