Rational design of covalent organic frameworks as a groundbreaking uranium capture platform through three synergistic mechanisms

IF 19.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2021-10-05 Epub Date: 2021-04-24 DOI:10.1016/j.apcatb.2021.120250

Wei-Rong Cui , Cheng-Rong Zhang , Rui-Han Xu , Xiao-Rong Chen , Wei Jiang , Ya-Jie Li , Ru-Ping Liang , Li Zhang , Jian-Ding Qiu

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引用次数: 61

Abstract

Herein, we report the first example of covalent organic framework (DHBD-TMT) linked by unsubstituted olefin-linkages for selective loading, chemical reduction and photocatalytic reduction of uranium. The unique structures of DHBD-TMT possess all the characteristics to be well suited as a capture platform for selective ligand complexation, efficient chemical reduction and photocatalytic reduction of uranium, thus exhibiting a groundbreaking uranium capture capacity (2640.8 mg g^-1). In the dark, DHBD-TMT can effectively adsorb uranium through the hydroxyl groups laced on the skeleton and reduce U^VI to U^IV in situ, leading to a higher adsorption capacity and selectivity of uranium. At the same time, the synergistic effect of the hydroquinone and triazine units in the extended π-conjugated skeleton significantly improve the photocatalytic activity of DHBD-TMT, and an additional U^VI photocatalytic reduction mechanism can occur under visible light irradiation, allowing significantly higher the capacity and faster adsorption kinetics.

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通过三种协同机制，合理设计共价有机框架作为突破性的铀捕获平台

在此，我们报告了第一个由未取代烯烃键连接的共价有机骨架(DHBD-TMT)用于铀的选择性负载，化学还原和光催化还原的例子。DHBD-TMT的独特结构具有作为选择性配体络合、高效化学还原和光催化还原铀的捕获平台的所有特征，从而显示出突破性的铀捕获能力(2640.8 mg g-1)。在黑暗中，DHBD-TMT可以通过骨架上的羟基有效吸附铀，并将UVI原位还原为UIV，从而使铀具有更高的吸附能力和选择性。同时，扩展π共轭骨架中对苯二酚和三嗪单元的协同作用显著提高了DHBD-TMT的光催化活性，并且在可见光照射下可发生额外的UVI光催化还原机制，使其容量显著提高，吸附动力学加快。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.