Tris(triazolo)triazine-Based Covalent Organic Frameworks for Efficiently Photocatalytic Hydrogen Peroxide Production

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Zhenwei Zhang, Dr. Qi Zhang, Yuxin Hou, Jiali Li, Shanshan Zhu, Prof. Dr. Hong Xia, Prof. Dr. Huijuan Yue, Prof. Dr. Xiaoming Liu
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引用次数: 0

Abstract

Two-dimensional covalent organic frameworks (2D-COFs) have recently emerged as fascinating scaffolds for solar-to-chemical energy conversion because of their customizable structures and functionalities. Herein, two tris(triazolo)triazine-based COF materials (namely COF-JLU51 and COF-JLU52) featuring large surface area, high crystallinity, excellent stability and photoelectric properties were designed and constructed for the first time. Remarkably, COF-JLU51 gave an outstanding H2O2 production rate of over 4200 μmol g−1 h−1 with excellent reusability in pure water and O2 under one standard sun light, that higher than its isomorphic COF-JLU52 and most of the reported metal-free materials, owing to its superior generation, separation and transport of photogenerated carriers. Experimental and theoretical researches prove that the photocatalytic process undergoes a combination of indirect 2e O2 reduction reaction (ORR) and 4e H2O oxidation reaction (WOR). Specifically, an ultrahigh yield of 7624.7 μmol g−1 h−1 with apparent quantum yield of 18.2 % for COF-JLU52 was achieved in a 1 : 1 ratio of benzyl alcohol and water system. This finding contributes novel, nitrogen-rich and high-quality tris(triazolo)triazine-based COF materials, and also designate their bright future in photocatalytic solar transformations.

用于高效光催化生产过氧化氢的三(三唑并)三嗪基共价有机框架。
二维共价有机框架(2D-COFs)因其可定制的结构和功能,最近已成为太阳能到化学能转换的迷人支架。本文首次设计并构建了两种基于三(三唑并)三嗪的 COF 材料(即 COF-JLU51 和 COF-JLU52),它们具有大表面积、高结晶度、优异的稳定性和光电特性。值得注意的是,由于 COF-JLU51 在光生载流子的生成、分离和传输方面具有优异的性能,因此它在纯水和氧气中的 H2O2 产率超过 4200 µmol g-1 h-1,并具有极佳的重复利用率,高于其同素异形体 COF-JLU52 和大多数已报道的无金属材料。实验和理论研究证明,光催化过程经历了间接 2e- O2 还原反应(ORR)和 4e- H2O 氧化反应(WOR)的组合。具体而言,在苯甲醇和水的比例为 1:1 的体系中,COF-JLU52 实现了 7624.7 µmol g-1 h-1 的超高产率,表观量子产率为 18.2%。这一发现为三(三唑并)三嗪基 COF 材料提供了新颖、富氮和高质量的材料,同时也预示着它们在光催化太阳能转化方面的广阔前景。
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
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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