Chinese Journal of Catalysis ›› 2022, Vol. 43 ›› Issue (4): 1042-1048.DOI: 10.1016/S1872-2067(21)63966-9

• Communication • Previous Articles     Next Articles

Precise and controllable tandem strategy triggering boosted oxygen reduction activity

Guoxing Jiang, Longhai Zhang, Wenwu Zou, Weifeng Zhang, Xiujun Wang, Huiyu Song, Zhiming Cui, Li Du**()   

  1. The Key Laboratory of Fuel Cell Technology of Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, Guangdong, China
  • Received:2021-09-25 Accepted:2021-09-25 Online:2022-03-05 Published:2022-03-01
  • Contact: Li Du*
  • About author:First author contact:

    Contributed equally to this work.

  • Supported by:
    National Natural Science Foundation of China(21975080);National Natural Science Foundation of China(21776104);Guangdong Basic and Applied Basic Research Foundation for Distinguished Young Scholar(2021B1515020025);Guangzhou Applied Basic Research Foundation(202102080460)


The development of efficient and cost-effective metal-free electrocatalysts for oxygen reduction reaction (ORR) has become crucial for electrochemical energy systems. However, reasonably validating and precisely regulating the active sites for designing optimized materials are still challenging. Herein, we report a precise and controllable tandem strategy to boost the ORR activity based on metal-free covalent organic frameworks (MFCOFs) comprising imine-N, thiophene-S, or triazine-N. Among these MFCOFs, post-tandem BTT-TAT-COF structure displayed a more positive catalytic capability and excellent electrochemical stability, indicating that the synergistic catalysis of multiple active sites induced the ORR catalytic activity through the conjugated skeleton of the structure. Density-functional theory calculations suggest that the series-connected backbone contained highly effective electrocatalytic active centers and provided synergistic catalysis. More importantly, this strategy highlights new opportunities for the advancement of efficient COF-based metal-free ORR catalysts.

Key words: Covalent organic frameworks, Metal-free electrocatalyst, Tandem strategy, Synergistic catalysis, Oxygen reduction reaction