Journal of Energy Chemistry ›› 2023, Vol. 76 ›› Issue (1): 639-647.DOI: 10.1016/j.jechem.2022.10.003

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Ultrathin organic polymer with p-π conjugated structure for simultaneous photocatalytic disulfide bond generation and CO2 reduction

Linquan Houa, Zhunyun Tangb, Guojiang Maoc, Shiheng Yind, Bei Longa, Tao Ouyangb,*, Guo-Jun Denga, Atif Alie, Ting Songa,*   

  1. aKey Laboratory for Green Organic Synthesis and Application of Hunan Province, Key Laboratory of Environmentally Friendly Chemistry and Application of Ministry of Education, College of Chemistry, Xiangtan University, Xiangtan 411105, Hunan, China;
    bHunan Key Laboratory for Micro-Nano Energy Materials and Device, School of Physics and Optoelectronics, Xiangtan University, Xiangtan 411105, Hunan, China;
    cSchool of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang 453007, Henan, China;
    dAnalytical and Testing Center, South China University of Technology, Guangzhou 510640, Guangdong, China;
    eDepartment of Chemistry and State Key Laboratory of Synthetic Chemistry, The University of Hong Kong, Pokfulam Road, Hong Kong 999077, China
  • Received:2022-07-12 Revised:2022-09-21 Accepted:2022-10-02 Published:2023-01-10
  • Contact: *E-mail addresses: ouyangtao@xtu.edu.cn (T. Ouyang), songtg@xtu.edu.cn (T. Song).

Abstract: Combining photocatalytic organic reactions with CO2 reduction is an efficient solar energy utilization mode, but it is still limited by the organic species that can be matched and the low conversion. Herein, ultrathin organic polymer with p-π conjugated structure (TPP) was rationally designed and prepared, and showed a high yield of CO (15.2 mmol g-1) and conversion of SS coupled products (100%), far exceeding the organic polymer with PO structure. The enhanced photoredox activity of TPP is ascribed to the orbital interaction between the p-orbital on phosphorus and the π-orbitals of aromatic, which can accelerate the photoinduced charge carrier separation and improve the CO2 adsorption capacity. TPP can also be used for the dehydrocoupling of various benzyl mercaptans to the corresponding SS bond products. This work provides a new concept for the efficient synthesis of disulfide bonds combined with CO2 reduction in a photoreaction system.

Key words: Photocatalytic coupled reaction, Disulfide bond, CO2 reduction, High activity, Organic polymer