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用于光催化铀分离的多金属氧酸盐封装金属有机框架材料

Polyoxometalate-encapsulated metal-organic frameworks for photocatalytic uranium isolation.

作者信息

Dong Zhimin, Zeng Dongling, Li Zifan, Chen Junjie, Wang Youqun, Cao Xiaohong, Yang Guoping, Zhang Zhibin, Liu Yunhai, Yang Feng

机构信息

State Key Laboratory of Nuclear Resources and Environment, East China University of Technology Nanchang 330013 China

Department of Chemistry, Southern University of Science and Technology Shenzhen 518055 China

出版信息

Chem Sci. 2024 Oct 22;15(45):19126-35. doi: 10.1039/d4sc05349d.

Abstract

Recycling uranium (U) adsorption and controlled conversion is crucial for the sustainable development of nuclear energy, in which photocatalytic reduction of U(vi) from aqueous solutions is considered one of the most effective strategies. The primary challenge in the photocatalytic elimination of U(vi) resides in the demand for photocatalysts with exceptional properties for effective U(vi) adsorption and charge separation. Herein, we developed the hybrids of polyoxometalate@Cu-metal-organic frameworks (POM@Cu-MOFs) through a self-assembly strategy and demonstrated the efficient removal of U(vi) synergistic adsorption and photocatalysis. The abundant oxygen-rich groups in POM served as the adsorption sites, endowing POM@Cu-MOFs with a remarkable removal capacity (1987.4 mg g under light irradiation) to remove 99.4% of UO . The attraction of electrons from Cu atoms within Cu-MOFs effectively accelerated the carrier dynamics due to their pronounced electronegativity. A mechanism associated with the synergetic effects of adsorption and photocatalytic reduction of U(vi) was proposed. This work provides a feasible approach for efficiently eliminating U(vi) from aqueous solutions in environmental pollution cleanup using the POM@Cu-MOF photocatalyst.

摘要

回收铀(U)吸附及可控转化对核能的可持续发展至关重要,其中从水溶液中光催化还原U(VI)被认为是最有效的策略之一。光催化消除U(VI)的主要挑战在于需要具有卓越性能以实现有效U(VI)吸附和电荷分离的光催化剂。在此,我们通过自组装策略开发了多金属氧酸盐@铜金属有机框架(POM@Cu-MOFs)杂化物,并证明了其通过协同吸附和光催化实现对U(VI)的高效去除。POM中丰富的富氧基团作为吸附位点,赋予POM@Cu-MOFs显著的去除能力(光照下为1987.4 mg g),可去除99.4%的UO。由于Cu-MOFs中Cu原子的明显电负性,来自Cu原子的电子吸引有效地加速了载流子动力学。提出了一种与U(VI)吸附和光催化还原协同效应相关的机制。这项工作为利用POM@Cu-MOF光催化剂在环境污染清理中从水溶液中高效消除U(VI)提供了一种可行的方法。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f1bc/11578236/c3892876b1db/d4sc05349d-f1.jpg

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