Electrocatalytic activity of MoSi2N4 monolayers decorated with single transition metal atoms: a computational study

Two-dimensional (2D) MoSi2N4 is a newly created material that has superstability and ultrahigh carrier mobility. Besides, the hydrogen evolution reaction activity was proved excellent by doping transition metal (TM) atoms and introducing N vacancies. But, the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) of 2D MoSi2N4 is unclear even. We have explored the electrocatalytic properties (OER/ORR) of MoSi2N4 by introducing Si vacancies and attaching various TM atoms. The structure and optoelectronic characteristics of MoSi2N4 have been researched in detail using density functional theory calculations. By analyzing the density of states, the free energy change diagram and contour maps of TM@V-Si-MoSiN, the results show that Co@V-Si-MoSiN has the lowest OER overpotential (0.53 V) among all samples. Additionally, the d-band center is used to explain the electrocatalytic origin of the OER and ORR of TM@V-Si-MoSiN. Our discoveries expand the 2D TM@V-Si-MoSiN applicability in the realm of catalysis.

Automated summary

This study investigates the electrocatalytic properties of 2D MoSi2N4 and finds that Co@V-Si-MoSiN has the lowest overpotential in the oxygen evolution reaction. This discovery expands the applicability of 2D TM@V-Si-MoSiN in the field of catalysis.