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。

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2024-07-01 DOI:10.1002/anie.202411546
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

摘要

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

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.

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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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