Atomistic Understanding of Two-dimensional Electrocatalysts from First Principles

Two-dimensional electrocatalysts have attracted great interest in recent years for renewable energy applications. However, the atomistic mechanisms are still under debate. Here we review the first-principles studies of the atomistic mechanisms of common 2D electrocatalysts. We first introduce the first-principles models for studying heterogeneous electrocatalysis then discuss the common 2D electrocatalysts with a focus on N doped graphene, single metal atoms in graphene, and transition metal dichalcogenides. The reactions include hydrogen evolution, oxygen evolution, oxygen reduction, and carbon dioxide reduction. Finally, we discuss the challenges and the future directions to improve the fundamental understanding of the 2D electrocatalyst at atomic level.