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

Bibliographic Details
Title: A photocatalytic redox cycle over a polyimide catalyst drives efficient solar-to-H2O2 conversion
Authors: Wenwen Chi, Yuming Dong, Bing Liu, Chengsi Pan, Jiawei Zhang, Hui Zhao, Yongfa Zhu, Zeyu Liu
Source: Nature Communications, Vol 15, Iss 1, Pp 1-10 (2024)
Publisher Information: Nature Portfolio, 2024.
Publication Year: 2024
Collection: LCC:Science
Subject Terms: Science
More Details: 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.
Document Type: article
File Description: electronic resource
Language: English
ISSN: 2041-1723
Relation: https://doaj.org/toc/2041-1723
DOI: 10.1038/s41467-024-49663-6
Access URL: https://doaj.org/article/1a370bd3c6e74c0db7ac5b4888878de9
Accession Number: edsdoj.1a370bd3c6e74c0db7ac5b4888878de9
Database: Directory of Open Access Journals
More Details
ISSN:20411723
DOI:10.1038/s41467-024-49663-6
Published in:Nature Communications
Language:English