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Research Article

Pyrimidine-containing covalent organic frameworks for efficient photosynthesis of hydrogen peroxide via one-step two electron oxygen reduction process

Hongyu Chen1, Hao Zhang2, Kai Chi2( ), Yan Zhao2( )
Second Medical Center and National Clinical Research Center for Geriatric Diseases, Chinese People’s Liberation Army General Hospital, Beijing 100853, China
Laboratory of Molecular Materials and Devices, Department of Materials Science, Fudan University, Shanghai 200433, China
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Graphical Abstract

Here, we developed an efficient photocatalyst by incorporating pyrimidine units into benzotrithiophene-based covalent organic framework (BTT-MD-COF), enabling the photosynthesis of H2O2 via the one-step two electron oxygen reduction pathway.

Abstract

The photocatalytic oxygen reduction reaction (ORR), particularly the one-step two-electron (2e−) pathway, is a highly promising strategy for efficient and selective hydrogen peroxide (H2O2) synthesis. However, constructing efficient photocatalysts to achieve a one-step 2e− ORR process remains a significant challenge. Herein, we developed an efficient photocatalyst by incorporating pyrimidine units into benzotrithiophene-based covalent organic framework (BTT-MD-COF), enabling the photosynthesis of H2O2 via the one-step 2e− ORR pathway with O2 and water. Under visible-light irradiation, BTT-MD-COF exhibited a high H2O2 production rate of up to 5691.2 μmol·h−1·g−1. Further experimental results and theoretical studies revealed that the introduction of pyrimidine units accelerates the separation of photoinduced electron–hole pairs and promotes Yeager-type O2 adsorption, which alters the two-step 2e− ORR process to the direct one-step 2e− process. This work offers a new avenue to create metal-free catalysts for efficient photosynthesis of H2O2.

Keywords

covalent organic frameworksphotocatalysishydrogen peroxideoxygen reduction reactionpyrimidine units

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Nano Research
Volume 17 Issue 11,
November 2024
Pages 9498-9506
DOI: 10.1007/s12274-024-6897-6
Cite this article:
Chen H, Zhang H, Chi K, et al. Pyrimidine-containing covalent organic frameworks for efficient photosynthesis of hydrogen peroxide via one-step two electron oxygen reduction process. Nano Research, 2024, 17(11): 9498-9506. https://doi.org/10.1007/s12274-024-6897-6
Topics:
Photocatalysis

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Received: 17 June 2024
Revised: 12 July 2024
Accepted: 18 July 2024
Published: 17 August 2024
© Tsinghua University Press 2024
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