Electrochemical Reduction of CO 2 via Single-Atom Catalysts Supported on α-In 2 Se 3

• Published in: The journal of physical chemistry letters 2023-07, Vol.14 (26), p.6110-6118
• Main Authors: Yang, Yun, Liu, Shixi, Fu, Gang
• Format: Article
• Language: English
• ISSN: 1948-7185; 1948-7185
• DOI: 10.1021/acs.jpclett.3c01202

In this work, the electrochemical CO reduction reaction (CO RR) over transition metal and α-In Se monolayer catalysts was investigated by density functional theory (DFT) and an effective screening medium method-reference interaction site model (ESM-RISM). On the basis of the scaling relationship between the adsorption free energies of intermediates, we constructed the relationships between oxygen-bound intermediates with *O and carbon-bound intermediates with *CHO. The calculation results indicate that *OCHO intermediates are more favorable for the first hydrogenation of CO on M@In Se catalysts; thus, the adsorption energy of oxygen-bound species determines the catalytic performance of M@In Se . The Co@In Se ↓-C was predicted to be the most promising catalyst with a low limiting potential of -0.385 V as determined by the computational hydrogen electrode method. Constant potential calculations also demonstrate that the M@In Se catalysts hold great potential for highly efficient CO RR. This work provides a fundamental understanding for the rational design of ferroelectric single-atom catalysts for the purpose of highly efficient electrocatalytic CO reduction.