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

Abstract Achieving efficient conversion of carbon dioxide (CO 2 ) 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@WTe 2 ) and screen favorable CO 2 reduction pathways. These results demonstrate that Ni single atoms strongly bind to the WTe 2 monolayer and exist in isolated form due to the high diffusion barriers. Also, Ni‐anchored WTe 2 monolayer (Ni@WTe 2 ) possesses a considerably low limiting‐potential (−0.11 V vs reversible hydrogen electrode) to convert CO 2 to HCOOH due to moderate OCHO adsorption energy and a suppressed competing hydrogen evolution reaction (HER). Therefore, Ni@WTe 2 monolayer is a promising electrocatalytic material for the CO 2 reduction reaction (CO 2 RR). This study sheds light on strategies of designing single metal atom anchored WTe 2 catalysts for improved CO 2 RR performances.