Issue 8, 2023

Extending the π-conjugation system of covalent organic frameworks for more efficient photocatalytic H2O2 production

Abstract

The photocatalytic oxygen reduction reaction (ORR) towards hydrogen peroxide (H2O2) is a promising but challenging alternative to the industrial anthraquinone process. Crystalline porous covalent organic frameworks (COFs), a new generation of semiconductors, have attracted significant attention because they exhibit broad visible-light harvesting, possess tunable energy levels, and facilitate facile separation and migration of photogenerated charge pairs. The modulation of the energy levels of COFs could facilitate charge transport, resulting in better photocatalytic performance. Herein, the π-conjugation system of COFs was extended via a post-sulfurization process, leading to a considerably enhanced photocatalytic activity. During the sulfurization process, imine-linked COFs were converted into thiazole-linked COFs to extend the conjugation structure of COFs in the x and y directions, resulting in higher transport of electrons. The thiazole-linked 4PE-N-S presents the best photocatalytic H2O2 generation performance with a rate of 1574 μmol g−1 h−1, which is about 5.8 and 3.7 times higher than that of imine-linked 4PE-N and 4PE-TT, respectively. Our findings provide new prospects for the design and synthesis of highly active organic photocatalysts for solar-to-chemical energy conversion.

Graphical abstract: Extending the π-conjugation system of covalent organic frameworks for more efficient photocatalytic H2O2 production

Supplementary files

Article information

Article type
Paper
Submitted
24 nov 2022
Accepted
07 mrt 2023
First published
14 mrt 2023

Green Chem., 2023,25, 3069-3076

Extending the π-conjugation system of covalent organic frameworks for more efficient photocatalytic H2O2 production

M. Deng, J. Sun, A. Laemont, C. Liu, L. Wang, L. Bourda, J. Chakraborty, K. Van Hecke, R. Morent, N. De Geyter, K. Leus, H. Chen and P. Van Der Voort, Green Chem., 2023, 25, 3069 DOI: 10.1039/D2GC04459E

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