N,S-Codoped Mesoporous Carbons Derived from Polymer Micelle-Based Assemblies for the Oxygen Reduction Reaction

The fabrication of high-performance metal-free carbon catalysts for the oxygen reduction reaction (ORR) is of practical importance for the energy sector. A novel fabrication strategy was used to prepare high-performance N,S-codoped mesoporous carbons (NSMPCs) as ORR catalysts, involving the preparation of poly(3-aminothiophenol)-based assemblies followed by subsequent pyrolysis. The N and S heteroatoms of the poly(3-aminothiophenol) are incorporated into the NSMPCs by pyrolysis, forming abundant catalytic active sites. The mesopores of NSMPCs locate on their surface, which are derived from the degradation of the micelle templates. These shallow mesopores greatly enhance the specific surface area and promote the mass transfer for the ORR. Moreover, the embedded graphene (or carbon nanotube) in the NSMPCs facilitates electron transport during the ORR. These factors are synergistically modulated to boost the catalytic performances of NSMPCs. As a result, NSMPCs exhibit superb catalytic performances, close to or better than those of the best performing metal-free carbon ORR catalysts reported to date and commercial Pt/C in alkaline electrolyte. This synergistic strategy provides a facile pathway for the fabrication of advanced metal-free carbon ORR catalysts.