One-step pyrolysis synthesis of ternary (P,S,N)-doped graphene as an efficient metal-free electrocatalyst for the oxygen reduction reaction

• Published in: Dalton transactions : an international journal of inorganic chemistry 2023-04, Vol.52 (14), p.4389-4397
• Main Authors: Wu, Yujun, Shuang, Wei, Yang, Lin, Cao, Chuanbao
• Format: Article
• Language: English
• Subjects: Catalytic activity; Chemical reduction; Chemical synthesis; Coupling; Density functional theory; Electrocatalysts; Energy conversion; Energy storage; Graphene; Oxygen reduction reactions; Pyrolysis
• ISSN: 1477-9226; 1477-9234
• DOI: 10.1039/d2dt04124c

Graphene-based materials have been regarded recently as a promising substance for electrochemical energy conversion and storage devices owing to their unique structure and extraordinary properties. Herein, an enormously facile one-step pyrolysis approach is reported for the fabrication of ternary (P,S,N)-doped graphene, which is further investigated as an efficient metal-free electrocatalyst for the oxygen reduction reaction (ORR). Furthermore, optimized ternary-doped graphene can deliver excellent ORR catalytic activity that favors the four-electron ORR process and outstanding long-term durability (90.54% current retention after 20000 s which is far superior to that of commercial Pt/C) owing to the preferable synergetic coupling effect between P, S and N. Density functional theory (DFT) calculations were performed to reveal the synergetic coupling effect between doping elements in the ORR process. This work provides an extremely simple one-step pyrolysis method for the synthesis of P,S,N-doped graphene for electrochemical energy conversion and storage devices. Ternary (P,S,N)-doped graphene was prepared by an extremely facile one-step pyrolysis approach to act as an efficient metal-free electrocatalyst for the ORR owing to the preferable synergetic coupling effect between P, S and N.