Transition metal single-atom anchored on MoSi2N4 monolayer as highly efficient electrocatalyst for hydrogen evolution reaction

TL;DR

This study uses first-principles calculations to identify transition metal atoms anchored on MoSi2N4 monolayer as highly efficient and stable electrocatalysts for hydrogen evolution reaction, with promising practical applications.

Contribution

It demonstrates that anchoring transition metal atoms on MoSi2N4 enhances HER activity, providing a new design strategy for efficient 2D electrocatalysts.

Findings

V@MoSi2N4 shows ΔGH* = -0.07 eV, indicating high HER activity.

Ni@MoSi2N4 has ΔGH* = 0.06 eV, also indicating high HER activity.

Transition metal anchoring activates the MoSi2N4 surface for improved catalysis.

Abstract

Single-atom catalysts are considered as a promising method for efficient energy conversion, owing to their advantages of high atom utilization and low catalyst cost. However, finding a stable two-dimensional structure and high hydrogen evolution reaction (HER) performance is a current research hotspot. Herein, based on the first-principles calculations, we identify the HER properties of six catalysts (TM@MoSi2N4, TM = Sc, Ti, V, Fe, Co, and Ni) comprising transition metal atoms anchored on MoSi2N4 monolayer. The results show that the spin-polarized states appear around the Fermi level after anchoring TM atoms. Therefore, the energy level of the first available unoccupied state for accommodating hydrogen drops, regulating the bonding strength of hydrogen. Thus, the single transition metal atom activates the active site of the MoSi2N4 inert base plane, becoming a quite suitable site for the HER. Based on {\Delta}GH*, the exchange current density and volcano diagram of the corresponding catalytic system were also calculated. Among them, V@MoSi2N4 ({\Delta}GH* = -0.07 eV) and Ni@MoSi2N4 ({\Delta}GH* = 0.06 eV) systems show efficient the HER property. Our study confirms that the transition metal atom anchoring is an effective means to improve the performance of electrocatalysis, and TM@MoSi2N4 has practical application potential as a high efficiency HER electrocatalyst.