A photocatalytic redox cycle over a polyimide catalyst drives efficient solar-to-H2O2 conversion

Wenwen Chi, Yuming Dong (), Bing Liu, Chengsi Pan, Jiawei Zhang, Hui Zhao, Yongfa Zhu () and Zeyu Liu
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Wenwen Chi: Jiangnan University
Yuming Dong: Jiangnan University
Bing Liu: Jiangnan University
Chengsi Pan: Jiangnan University
Jiawei Zhang: Jiangnan University
Hui Zhao: Jiangnan University
Yongfa Zhu: Tsinghua University
Zeyu Liu: Jiangsu University of Science and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Circumventing the conventional two-electron oxygen reduction pathway remains a great problem in enhancing the efficiency of H2O2 photosynthesis. A promising approach to achieve outstanding photocatalytic activity involves the utilization of redox intermediates. Here, we engineer a polyimide aerogel photocatalyst with photoreductive carbonyl groups for non-sacrificial H2O2 production. Under photoexcitation, carbonyl groups on the photocatalyst surface are reduced, forming an anion radical intermediate. The produced intermediate is oxidized by O2 to produce H2O2 and subsequently restores the carbonyl group. The high catalytic efficiency is ascribed to a photocatalytic redox cycle mediated by the radical anion, which not only promotes oxygen adsorption but also lowers the energy barrier of O2 reduction reaction for H2O2 generation. An apparent quantum yield of 14.28% at 420 ± 10 nm with a solar-to-chemical conversion efficiency of 0.92% is achieved. Moreover, we demonstrate that a mere 0.5 m2 self-supported polyimide aerogel exposed to natural sunlight for 6 h yields significant H2O2 production of 34.3 mmol m−2.

Date: 2024
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DOI: 10.1038/s41467-024-49663-6

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