Ambient Preparation of Benzoxazine-based Phenolic Resins Enables Long-term Sustainable Photosynthesis of Hydrogen Peroxide

Xinyao Wang; Xiaowei Yang; Chen Zhao; Yutong Pi; Xiaobo Li; Zhongfan Jia; Si Zhou; Jijun Zhao; Limin Wu; Jian Liu

doi:10.1002/anie.202302829

Ambient Preparation of Benzoxazine-based Phenolic Resins Enables Long-term Sustainable Photosynthesis of Hydrogen Peroxide

Angew Chem Int Ed Engl. 2023 Jun 5;62(23):e202302829. doi: 10.1002/anie.202302829. Epub 2023 Apr 20.

Authors

Xinyao Wang^{1

2}, Xiaowei Yang³, Chen Zhao^{1

2}, Yutong Pi^{1

2}, Xiaobo Li⁴, Zhongfan Jia⁵, Si Zhou³, Jijun Zhao³, Limin Wu^{6

7}, Jian Liu^{1

6

8}

Affiliations

¹ State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
² Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
³ Key Laboratory of Materials Modification by Laser, Ion and Electron Beams (Dalian University of Technology, Ministry of Education, Dalian, 116024, China.
⁴ College of Chemistry and Life Sciences, Zhejiang Normal University, Jinhua, 321004, China.
⁵ Institute for Nanoscale Science and Technology, College of Science and Engineering, Flinders University, Sturt Road, Bedford Park, South Australia, 5042, Australia.
⁶ Inner Mongolia University, Hohhot, Inner Mongolia, 010021, P. R. China.
⁷ Department of Materials Science and State Key Laboratory of Molecular Engineering of Polymers, Fudan University, 200433, Shanghai, China.
⁸ DICP-Surrey Joint Centre for Future Materials, Department of Chemical and Process Engineering and Advanced Technology Institute, University of Surrey, Guildford, Surrey, GU2 7XH, UK.

PMID: 36965108
DOI: 10.1002/anie.202302829

Abstract

Rational design of polymer structures at the molecular level promotes the iteration of high-performance photocatalyst for sustainable photocatalytic hydrogen peroxide (H₂ O₂ ) production from oxygen and water, which also lays the basis for revealing the reaction mechanism. Here we report a benzoxazine-based m-aminophenol-formaldehyde resin (APFac) polymerized at ambient conditions, exhibiting superior H₂ O₂ yield and long-term stability to most polymeric photocatalysts. Benzoxazine structure was identified as the crucial photocatalytic active segment in APFac. Favorable adsorption of oxygen/intermediates on benzoxazine structure and commendable product selectivity accelerated the reaction kinetically in stepwise single-electron oxygen reduction reaction. The proposed benzoxazine-based phenolic resin provides the possibility of production in batches and industrial application, and sheds light on the de novo design and analysis of metal-free polymeric photocatalysts.

Keywords: Benzoxazine Structure; H2O2 Photosynthesis; Heterogeneous Photocatalysis; Oxygen Intermediate Adsorption; Phenolic Resin.

Abstract

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