Covalent organic frameworks for direct photosynthesis of hydrogen peroxide from water, air and sunlight

Fuyang Liu, Peng Zhou, Yanghui Hou, Hao Tan, Yin Liang, Jialiang Liang, Qing Zhang, Shaojun Guo, Meiping Tong () and Jinren Ni
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Fuyang Liu: Peking University
Peng Zhou: Peking University Shenzhen Graduate School
Yanghui Hou: Peking University
Hao Tan: Peking University
Yin Liang: Peking University
Jialiang Liang: Chongqing University
Qing Zhang: Peking University
Shaojun Guo: Peking University
Meiping Tong: Peking University
Jinren Ni: Peking University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Solar-driven photosynthesis is a sustainable process for the production of hydrogen peroxide, the efficiency of which is plagued by side reactions. Metal-free covalent organic frameworks (COFs) that can form suitable intermediates and inhibit side reactions show great promise to photo-synthesize H2O2. However, the insufficient formation and separation/transfer of photogenerated charges in such materials restricts the efficiency of H2O2 production. Herein, we provide a strategy for the design of donor-acceptor COFs to greatly boost H2O2 photosynthesis. We demonstrate that the optimal intramolecular polarity of COFs, achieved by using suitable amounts of phenyl groups as electron donors, can maximize the free charge generation, which leads to high H2O2 yield rates (605 μmol g−1 h−1) from water, oxygen and visible light without sacrificial agents. Combining in-situ characterization with computational calculations, we describe how the triazine N-sites with optimal N 2p states play a crucial role in H2O activation and selective oxidation into H2O2. We further experimentally demonstrate that H2O2 can be efficiently produced in tap, river or sea water with natural sunlight and air for water decontamination.

Date: 2023
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DOI: 10.1038/s41467-023-40007-4

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