Theoretical design of one-dimensional dual site metal-organic framework ribbon for CO2RR

Abstract

Electrochemical conversion of carbon dioxide into value-added products is promising to alleviate greenhouse gas emission and energy demands. Metal-organic framework (MOF) based materials provide a platform for rational design of electrocatalyst for CO2 reduction reaction (CO2RR). Herein, we designed a series of novel one-dimensional dual site metal-organic framework ribbons (TM2-MOF), and systematically explored their electronic structures and CO2RR catalytic performance using density functional theory calculations. Based on the calculated free energy of CO2 adsorption, it is found that these Sc2-MOF, Ti2-MOF, and V2-MOF monolayers could spontaneously adsorb CO2 molecules and activate them. Furthermore, thermodynamic free energy analysis revealed that the V2-MOF surface exhibits the lowest reaction energy barrier and outstanding CO2RR catalytic performance, with the energy barrier of the rate-determining step being only 0.564 eV. The innovative design of this material not only provides a theoretical basis for the development of high-efficiency catalysts for CO2 conversion but also offers a valuable reference for other types of electrocatalytic reactions.