Role of heteroatom-doping in enhancing catalytic activities and the stability of single-atom catalysts for oxygen reduction and oxygen evolution reactions.

Single-atom catalysts (SACs) are promising as efficient electrocatalysts for clean energy technologies such as fuel cells, water splitting, and metal-air batteries. Still, the unsatisfactory loading density and stability of the catalytic active centers limit their applications. Herein, a doping strategy is explored to achieve highly efficient and stable SACs for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The stability, electronic structures, and ORR/OER overpotentials of S-doped transition metal-nitrogen-carbon SAC structures were investigated using first-principles calculation methods. An intrinsic descriptor linking the intrinsic properties of catalysts and the catalytic activity was established for screening the best SACs. The theoretical predictions are well consistent with the experimental results, which provide a theoretical basis for understanding the catalytic mechanism and an approach for the rational design of SACs for clean energy conversion and storage.