Design of single transition metal atom supported by MoTe ₂ for CO ₂ Reduction

Electrocatalytic CO 2 reduction has attracted much attention due to its potential to facilitate an artificial carbon cycle under mild conditions. In this paper, we investigate the catalytic performance of MoTe 2 and MoTe 2 -InN heterojunction-loaded single-atom catalysts (SACs) for CO 2 reduction using density-functional theory (DFT) calculations. Among the catalysts studied, Ni@MoTe 2 (-0.04 V) and Ni-MoTe 2 -InN (-0.16 V) exhibited lower limiting potentials. This improvement is attributed to the reduced energy required to activate the Ni-O 2 bond in the *OCHO + H⁺ + e⁻ → *HCOOH step. Remarkably, we observed a strong linear correlation between the adsorption energy of *OCHO and the catalytic activity for the generation of the two-electron product, HCOOH. This correlation challenges the conventional volcano-shaped relationship and serves as a reliable descriptor for predicting the limiting voltage. Furthermore, we applied this descriptor to the TM@MoTe 2 -InN system, confirming its applicability. This finding further validates that the adsorption energy of the intermediate *OCHO is an effective descriptor, significantly reducing the computational resources required for identifying high-performance catalysts. This study provides an avenue for the theoretical design of efficient electrocatalysts for CO 2 RR.