Boosting Electrocatalytic Reduction of CO2 to HCOOH on Ni Single Atom Anchored WTe2 Monolayer

Achieving efficient conversion of carbon dioxide (CO₂ ) to formic acid (HCOOH) at mild conditions is a promising means to reduce greenhouse gas emission and mitigate the energy crisis. Herein, spin-polarized density functional theory calculations with van der Waals corrections (DFT+D3) are performed to analyze the catalytic activity of seven metals (Ti, Fe, Ni, Cu, Zn, In, and Sn) anchored on a tungsten ditelluride monolayer (M@WTe₂ ) and screen favorable CO₂ reduction pathways. These results demonstrate that Ni single atoms strongly bind to the WTe₂ monolayer and exist in isolated form due to the high diffusion barriers. Also, Ni-anchored WTe₂ monolayer (Ni@WTe₂ ) possesses a considerably low limiting-potential (-0.11 V vs reversible hydrogen electrode) to convert CO₂ to HCOOH due to moderate OCHO adsorption energy and a suppressed competing hydrogen evolution reaction (HER). Therefore, Ni@WTe₂ monolayer is a promising electrocatalytic material for the CO₂ reduction reaction (CO₂ RR). This study sheds light on strategies of designing single metal atom anchored WTe₂ catalysts for improved CO₂ RR performances.