Molecular Level Modulation of Anthraquinone-containing Resorcinol-formaldehyde Resin Photocatalysts for H2 O2 Production with Exceeding 1.2 % Efficiency

Chen Zhao; Xinyao Wang; Yanfeng Yin; Wenming Tian; Guang Zeng; Haitao Li; Sheng Ye; Limin Wu; Jian Liu

doi:10.1002/anie.202218318

Molecular Level Modulation of Anthraquinone-containing Resorcinol-formaldehyde Resin Photocatalysts for H₂ O₂ Production with Exceeding 1.2 % Efficiency

Angew Chem Int Ed Engl. 2023 Mar 13;62(12):e202218318. doi: 10.1002/anie.202218318. Epub 2023 Feb 8.

Authors

Chen Zhao^{1

2}, Xinyao Wang^{1

2}, Yanfeng Yin³, Wenming Tian³, Guang Zeng¹, Haitao Li¹, Sheng Ye⁴, Limin Wu^{5

6}, Jian Liu^{1

6

7}

Affiliations

¹ State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, China.
² Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
³ State Key Laboratory of Molecular Reaction Dynamics and the Dynamic Research Center for Energy and Environmental Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
⁴ College of Science & School of Plant Protection, Anhui Agricultural University, Hefei, 230036, China.
⁵ Department of Materials Science and State Key Laboratory of Molecular Engineering of Polymers, Fudan University, 200433, Shanghai, China.
⁶ Inner Mongolia University, Hohhot, Inner Mongolia, 010021, P. R. China.
⁷ DICP-Surrey Joint Centre for Future Materials, Department of Chemical and Process Engineering and Advanced Technology Institute, University of Surrey, Guilford, Surrey GU27XH, UK.

PMID: 36578144
DOI: 10.1002/anie.202218318

Abstract

Designing polymeric photocatalysts at the molecular level to modulate the photogenerated charge behavior is a promising and challenging strategy for efficient hydrogen peroxide (H₂ O₂ ) 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, H₂ O₂ 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 H₂ O₂ production. RF-DHAQ exhibits excellent overall photosynthesis of H₂ O₂ 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.

Keywords: Donor/Acceptor Ratio; H2O2 Production; Molecular Level Modulation; Photocatalysis; Resorcinol-Formaldehyde Resin.

Abstract

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