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Strongly Reducing (Diarylamino)benzene-Based Covalent Organic Framework for Metal-Free Visible Light Photocatalytic H2O2 Generation
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2020-11-13 , DOI: 10.1021/jacs.0c09684
Chidharth Krishnaraj 1, 2 , Himanshu Sekhar Jena 1 , Laurens Bourda 1, 3 , Andreas Laemont 1 , Pradip Pachfule 2 , Jérôme Roeser 2 , C. Vinod Chandran 4, 5 , Sander Borgmans 6 , Sven M. J. Rogge 6 , Karen Leus 1 , Christian V. Stevens 7 , Johan A. Martens 4, 5 , Veronique Van Speybroeck 6 , Eric Breynaert 4, 5 , Arne Thomas 2 , Pascal Van Der Voort 1
Affiliation  

Photocatalytic reduction of molecular oxygen is a promising route toward sustainable production of hydrogen peroxide (H2O2). This challenging process requires photoactive semiconductors enabling solar energy driven generation and separation of electrons and holes with high charge transfer kinetics. Covalent organic frameworks (COFs) are an emerging class of photoactive semiconductors, tunable at a molecular level for high charge carrier generation and transfer. Herein, we report two newly designed two-dimensional COFs based on a (diarylamino)benzene linker that form a Kagome (kgm) lattice and show strong visible light absorption. Their high crystallinity and large surface areas (up to 1165 m2·g–1) allow efficient charge transfer and diffusion. The diarylamine (donor) unit promotes strong reduction properties, enabling these COFs to efficiently reduce oxygen to form H2O2. Overall, the use of a metal-free, recyclable photocatalytic system allows efficient photocatalytic solar transformations.

中文翻译:

用于无金属可见光光催化生成 H2O2 的强还原(二芳基氨基)苯基共价有机骨架

分子氧的光催化还原是可持续生产过氧化氢 (H2O2) 的一条有前途的途径。这个具有挑战性的过程需要光敏半导体,以实现太阳能驱动的生成以及具有高电荷转移动力学的电子和空穴的分离。共价有机骨架 (COF) 是一类新兴的光敏半导体,可在分子水平上进行调节,以产生和转移高电荷载流子。在此,我们报告了两种新设计的基于(二芳基氨基)苯连接体的二维 COF,它们形成 Kagome (kgm) 晶格并显示出强烈的可见光吸收。它们的高结晶度和大表面积(高达 1165 m2·g–1)允许有效的电荷转移和扩散。二芳基胺(供体)单元具有很强的还原性能,使这些 COF 能够有效地减少氧气以形成 H2O2。总体而言,使用无金属、可回收的光催化系统可以实现高效的光催化太阳能转化。
更新日期:2020-11-13
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