NiCoP-stabilized single atoms for efficient hydrogen evolution: A first-principles study

Abstract

The efficient production of hydrogen through water electrolysis can be regarded as a pragmatic strategy for the generation of clean, low-carbon, safe, and highly efficient energy. However, to overcome the significant overpotential, the sluggish hydrogen evolution reaction (HER) requires a significant energy input. A good atomic-level electrocatalyst design strategy plays a crucial role in improving HER performance. In this work, density functional theory (DFT) calculations are systematically applied to investigate single metal-atom electrocatalysts stabilized on NiCoP supports (M@NiCoP). Initially, a computational evaluation of the thermodynamic and electrochemical stability of all the catalysts was conducted. Subsequently, the hydrogen adsorption Gibbs free energies of these catalysts were calculated, to screen out materials that exhibited both good performance and stability. The research result indicates that Sn@NiCoP and Pt@NiCoP exhibited excellent stability and catalytic activity, especially the ΔG_H∗ of Pt@NiCoP catalyst with only 0.01 eV (pH = 0), which outperforms the current Pt/C catalyst. This research offers theoretical predictions regarding the design of low-cost HER electrocatalysts. Moreover, it has pioneered new methods for stabilizing single-atom (SAC) catalysts.