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A photocatalytic redox cycle over a polyimide catalyst drives efficient solar-to-H2O2 conversion.
Chi, Wenwen; Dong, Yuming; Liu, Bing; Pan, Chengsi; Zhang, Jiawei; Zhao, Hui; Zhu, Yongfa; Liu, Zeyu.
Affiliation
  • Chi W; International Joint Research Center for Photoresponsive Molecules and Materials, Key Laboratory of Synthetic and Biological Colloids, School of Chemical and Material Engineering, Jiangnan University, Wuxi, China.
  • Dong Y; International Joint Research Center for Photoresponsive Molecules and Materials, Key Laboratory of Synthetic and Biological Colloids, School of Chemical and Material Engineering, Jiangnan University, Wuxi, China. dongym@jiangnan.edu.cn.
  • Liu B; International Joint Research Center for Photoresponsive Molecules and Materials, Key Laboratory of Synthetic and Biological Colloids, School of Chemical and Material Engineering, Jiangnan University, Wuxi, China.
  • Pan C; International Joint Research Center for Photoresponsive Molecules and Materials, Key Laboratory of Synthetic and Biological Colloids, School of Chemical and Material Engineering, Jiangnan University, Wuxi, China.
  • Zhang J; International Joint Research Center for Photoresponsive Molecules and Materials, Key Laboratory of Synthetic and Biological Colloids, School of Chemical and Material Engineering, Jiangnan University, Wuxi, China.
  • Zhao H; International Joint Research Center for Photoresponsive Molecules and Materials, Key Laboratory of Synthetic and Biological Colloids, School of Chemical and Material Engineering, Jiangnan University, Wuxi, China.
  • Zhu Y; Department of Chemistry, Tsinghua University, Beijing, China. zhuyf@tsinghua.edu.cn.
  • Liu Z; School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang, China.
Nat Commun ; 15(1): 5316, 2024 Jun 22.
Article in En | MEDLINE | ID: mdl-38909037
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.

Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: Nat Commun Journal subject: BIOLOGIA / CIENCIA Year: 2024 Document type: Article Affiliation country:

Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: Nat Commun Journal subject: BIOLOGIA / CIENCIA Year: 2024 Document type: Article Affiliation country: