A doping-adsorption-pyrolysis strategy for constructing atomically dispersed cobalt sites anchored on a N-doped carbon framework as an efficient bifunctional electrocatalyst for hydrogen evolution and oxygen reduction.

Abstract

Renewable energy technology development focuses on the exploration of economical and efficient non-precious metal catalysts to replace precious metal catalysts in electrocatalytic reactions including oxygen reduction (ORR) and hydrogen evolution (HER). Herein, we synthesized a cobalt single atom catalyst anchored on a N-doped carbon framework by a doping-adsorption-pyrolysis strategy. The optimized Co SAs/CN-3 catalyst showed excellent HER and ORR bifunctional electrocatalytic performance, which could be attributed to the highly dispersed Co–N4 active sites, large specific surface area and abundant pore structure. Density functional theory shows that the isolated active Co–N4 site shows low hydrogen adsorption Gibbs free energy, and promotes the adsorption of H and oxygen-containing intermediates in HER and ORR. This work not only provides a new idea for the construction of transition metal catalysts with atomic accuracy but also provides powerful guidance for the development of efficient bifunctional electrocatalysts.