Janus MoPC Monolayer with Superior Electrocatalytic Performance for the Evolution Reaction

Designing the earth's abundant and high-performance electro-catalysts, which possess high stability, excellent electrical conductivity, inherent active sites, and catalytic activity identical with Pt, is challenging but crucial for the hydrogen evolution reaction (HER). By first-principles structure search simulations, we identify a new two-dimensional (2D) MoPC material with the Janus structure as a promising catalyst. This novel 2D monolayer has superior stability and metallic conductivity. Especially, it exhibits a remarkable HER catalytic activity, where all of the constituent atoms, including Mo, P, and C, can uniformly act as active sites in view of the near-zero Delta GH* value. Its active site density counts up to 1.46 x 10(15) site/cm(2), larger than that of many reported materials and even comparable to Pt. The excellent HER catalytic activity can also be maintained at a very high H coverage with or without external strain. The MoPC monolayer can produce H-2 spontaneously through the favorable Volmer- Heyrovsky pathway. The detailed catalytic mechanism behind the high HER activity has been also analyzed. Our work provides a feasible action for the experimental synthesis of excellent HER catalysts.