Theoretical design of one-dimensional dual site metal–organic framework ribbons for the CO2RR

Abstract

Electrochemical conversion of carbon dioxide into value-added products shows promise for alleviating greenhouse gas emission and energy demands. Metal–organic framework (MOF) based materials provide a platform for the rational design of electrocatalysts for the 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 outstanding CO₂RR catalytic performance with a limiting potential of −0.564 V. 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.