Molecular Level Modulation of Anthraquinone‐containing Resorcinol‐formaldehyde Resin Photocatalysts for H2O2 Production with Exceeding 1.2 % Efficiency

Designing polymeric photocatalysts at the molecular level to modulate the photogenerated charge behavior is a promising and challenging strategy for efficient hydrogen peroxide (H2O2) photosynthesis. Here, we introduce electron‐deficient 1,4‐dihydroxyanthraquinone (DHAQ) into the framework of resorc...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2023-03, Vol.62 (12), p.n/a
Main Authors: Zhao, Chen, Wang, Xinyao, Yin, Yanfeng, Tian, Wenming, Zeng, Guang, Li, Haitao, Ye, Sheng, Wu, Limin, Liu, Jian
Format: Article
Language:English
Subjects:
Anthraquinone
Anthraquinones
Density functional theory
Donor/Acceptor Ratio
Formaldehyde
Formaldehyde resins
H2O2 Production
Hydrogen peroxide
Isotopic labeling
Molecular Level Modulation
Oxidation
Photocatalysis
Photocatalysts
Photosynthesis
Radioactive labeling
Resorcinol
Resorcinol-Formaldehyde Resin
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Summary:Designing polymeric photocatalysts at the molecular level to modulate the photogenerated charge behavior is a promising and challenging strategy for efficient hydrogen peroxide (H2O2) photosynthesis. Here, we introduce electron‐deficient 1,4‐dihydroxyanthraquinone (DHAQ) into the framework of resorcinol‐formaldehyde (RF) resin, which modulates the donor/acceptor ratio from the perspective of molecular design for promoting the charge separation. Interestingly, H2O2 can be produced via oxygen reduction and water oxidation pathways, verified by isotopic labeling and in situ characterization techniques. Density functional theory (DFT) calculations elucidate that DHAQ can reduce the energy barrier for H2O2 production. RF‐DHAQ exhibits excellent overall photosynthesis of H2O2 with a solar‐to‐chemical conversion (SCC) efficiency exceeding 1.2 %. This work opens a new avenue to design polymeric photocatalysts at the molecular level for high‐efficiency artificial photosynthesis. Electron‐deficient 1,4‐dihydroxyanthraquinone (DHAQ) molecules were adopted to modulate the donor/acceptor ratio in resorcinol‐formaldehyde (RF) resin at the molecular level. The RF‐DHAQ with matching donor and acceptor displays enhanced charge separation ability, lower energy barrier and overall photosynthesis of hydrogen peroxide (H2O2) by dual‐pathway with solar‐to‐chemical conversion efficiency exceeding 1.2 %.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202218318