Chinese Journal of Catalysis ›› 2023, Vol. 46: 28-35.DOI: 10.1016/S1872-2067(22)64205-0

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A covalent organic framework inspired by C3N4 for photosynthesis of hydrogen peroxide with high quantum efficiency

Chaochen Shaoa,b, Qing Hea,b, Mochun Zhanga,b, Lin Jiaa,b, Yujin Jia,b, Yongpan Hua,b, Youyong Lia,b, Wei Huanga,b,*(), Yanguang Lia,b,*()   

  1. aInstitute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, Jiangsu, China
    bJiangsu Key Laboratory for Advanced Negative Carbon Technologies, Soochow University, Suzhou 215123, Jiangsu, China
  • Received:2022-10-05 Accepted:2022-12-05 Online:2023-03-18 Published:2023-02-21
  • Contact: *E-mail: yanguang@suda.edu.cn (Y. Li), weihuang@suda.edu.cn (W. Huang)
  • About author:

    1Contributed equally to this work.

  • Supported by:
    National Natural Science Foundation of China(22002100);National Natural Science Foundation of China(U2002213);The Natural Science Foundation of Jiangsu Province(BK20220027);Collaborative Innovation Center of Suzhou Nano Science and Technology, the 111 Project and Joint International Research Laboratory of Carbon-Based Functional Materials and Devices

Abstract:

Carbon nitride (C3N4) has been the main research focus for photocatalytic H2O2 synthesis that may enable the on-site and on-demand H2O2 production under mild conditions. Its potential is unfortunately shadowed by the narrow light absorption and fast charge recombination. Building on the understanding of the inherent merits and pitfalls of C3N4, we here propose to assemble active heptazine motifs with functional linkers in ordered molecular frameworks for highly efficient photocatalytic H2O2 production. Herein, a heptazine-based covalent organic framework is synthesized via the Schiff-base reaction. It has enhanced light absorption and charge separation. When irradiated with visible light in the presence of sacrificial electron donors, the sample exhibits an excellent H2O2 production rate of 11986 μmol h-1 g-1 and an apparent quantum efficiency up to 38% at 420 nm, outperforming most organic or inorganic competitors in our best knowledge. Impressively, the catalyst can also endure long time operation that affords the linear H2O2 accumulation to a practically usable concentration.

Key words: H2O2 production, Photocatalysis, Oxygen reduction, Covalent organic frameworks, Carbon nitride