Regulating the electronic properties of MoSe2 to improve its CO2 electrocatalytic reduction performance via atomic doping

Abstract

Reduction of carbon dioxide (CO₂) to energy-rich hydrocarbons by electrocatalysis due to the high bond energy of CO is a great challenge. To clearly understand the mechanism of CO₂ reduction at the electronic scale, through density functional theory (DFT) calculations, the pathways of the CO₂ reduction reaction on two-dimensional (2D) MoSe₂ doped transition metals (Fe, Co, Ni and Cu) are explored. The obtained results show that Ni_MT@MoSe₂, Cu_H@MoSe₂ and Cu_MT@MoSe₂ are suitable for CO₂ reduction, which may be attributed to the moderate CO₂ adsorption energies and influence of regulated electronic properties. Cu doped MoSe₂ has excellent performance for methane (CH₄) production with lower limiting potentials. Our findings greatly contribute to a comprehensive understanding of the influencing electronic properties on CO₂ reduction and CH₄ selectivity, which provides significant guidance for further CO₂ reduction reaction catalyst design at an atomic level.