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由单重态开壳双自由基构建的用于高效光还原U(VI)的卤代氢键有机框架(XHOF)。

Halogen hydrogen-bonded organic framework (XHOF) constructed by singlet open-shell diradical for efficient photoreduction of U(VI).

作者信息

Feng Lijuan, Yuan Yihui, Yan Bingjie, Feng Tiantian, Jian Yaping, Zhang Jiacheng, Sun Wenyan, Lin Ke, Luo Guangsheng, Wang Ning

机构信息

State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou, 570228, P. R. China.

出版信息

Nat Commun. 2022 Mar 16;13(1):1389. doi: 10.1038/s41467-022-29107-9.

DOI:10.1038/s41467-022-29107-9
PMID:35296676
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8927584/
Abstract

Synthesis of framework materials possessing specific spatial structures or containing functional ligands has attracted tremendous attention. Herein, a halogen hydrogen-bonded organic framework (XHOF) is fabricated by using Cl ions as central connection nodes to connect organic ligands, 7,7,8,8-tetraaminoquinodimethane (TAQ), by forming a Cl···H hydrogen bond structure. Unlike metallic node-linked MOFs, covalent bond-linked COFs, and intermolecular hydrogen bond-linked HOFs, XHOFs represent a different kind of crystalline framework. The electron-withdrawing effect of Cl combined with the electron-rich property of the organic ligand TAQ strengthens the hydrogen bonds and endows XHOF-TAQ with high stability. Due to the production of excited electrons by TAQ under light irradiation, XHOF-TAQ can efficiently catalyze the reduction of soluble U(VI) to insoluble U(IV) with a capacity of 1708 mg-U g-material. This study fabricates a material for uranium immobilization for the sustainability of the environment and opens up a new direction for synthesizing crystalline framework materials.

摘要

具有特定空间结构或含有功能性配体的框架材料的合成引起了极大关注。在此,通过使用氯离子作为中心连接节点,通过形成Cl···H氢键结构来连接有机配体7,7,8,8-四氨基对苯二醌二甲烷(TAQ),制备了一种卤素氢键有机框架(XHOF)。与金属节点连接的金属有机框架(MOF)、共价键连接的共价有机框架(COF)和分子间氢键连接的氢键有机框架(HOF)不同,XHOF代表了一种不同类型的晶体框架。Cl的吸电子效应与有机配体TAQ的富电子性质相结合,增强了氢键,并赋予XHOF-TAQ高稳定性。由于TAQ在光照下产生激发电子,XHOF-TAQ能够以1708 mg-U g-材料的容量有效地催化将可溶性U(VI)还原为不溶性U(IV)。本研究制备了一种用于铀固定以实现环境可持续性的材料,并为合成晶体框架材料开辟了新方向。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/ee9dfcab9f50/41467_2022_29107_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/cfe303188b12/41467_2022_29107_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/9383cbce070a/41467_2022_29107_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/4c0bad67808a/41467_2022_29107_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/f7cac8642e89/41467_2022_29107_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/267977f8059a/41467_2022_29107_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/ee9dfcab9f50/41467_2022_29107_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/cfe303188b12/41467_2022_29107_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/9383cbce070a/41467_2022_29107_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/4c0bad67808a/41467_2022_29107_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/f7cac8642e89/41467_2022_29107_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/267977f8059a/41467_2022_29107_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8a89/8927584/ee9dfcab9f50/41467_2022_29107_Fig6_HTML.jpg

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