Theoretical Study of Ni- and Cu-Doped Molybdenum Ditelluride Electrocatalysts for Carbon Dioxide Reduction to Formic Acid and Carbon Monoxide

Under mild conditions, the effective conversion of carbon dioxide (CO2) into formic acid (HCOOH) and carbon monoxide (CO) represents a promising avenue for mitigating greenhouse gas emissions and addressing energy crises. In this work, we analyzed the electro-catalytic activities of six metals (Ti, Fe, Ni, Cu, Zn, and Cr) anchored on monolayer molybdenum telluride (TM@MoTe2) for the CO2 reduction reaction (CO2RR) from CO2 to HCOOH and CO. Compared to the reversible hydrogen electrode, the limiting potential for HCOOH production on Ni@MoTe2 is only about −0.38 V, and it is only about −0.20 V for the CO production on Cu@MoTe2. The limiting potential is concerned with the free energies of *OCHO and *COOH. Both the CO2RRs suppress the competing hydrogen evolution reaction (HER) and exhibit good selectivity for the desired reaction products. These features enable the efficient conversion of CO2 into HCOOH on Ni@MoTe2 or CO on Cu@MoTe2. Our calculations could provide valuable insights for the design and synthesis of high-performance catalysts based on MoTe2.