Unifying the origin of catalytic activities for carbon-based metal-free electrocatalysts

Abstract

Carbon-based metal-free electrocatalysts (C-MFECs) have received great attention owing to their high efficiency, earth-abundance and tolerance to crossover effect. Recent research and development have demonstrated that various strategies, including heteroatom doping, defect doping, and molecular modification (doping), can induce catalytic active sites into carbon materials to create efficient and multifunctional electrocatalysts. Theoretical research has revealed that the catalytic activity in C-MFECs origins from the charge/spin redistributions induced by the change in electronic structures of doped carbon materials. In this review article, recent advances in the development of C‐MFECs are discussed and the origin of catalytic activities for all C-MFECs is unified to the heteroatom/defect/molecular doping-induced charge transfer/spin redistribution. The progress in theoretical studies of the unified mechanistic understanding is also overviewed for the rational design of C-MFECs. Finally, current challenges and future perspectives in this exciting field are presented.