Two-Dimensional (2D) TM-Tetrahydroxyquinone Metal–Organic Framework for Selective CO(2) Electrocatalysis: A DFT Investigation

The resource utilization of CO [Formula: see text] is one of the essential avenues to realize the goal of “double carbon”. The metal–organic framework (MOF) has shown promising applications in CO [Formula: see text] catalytic reduction reactions due to its sufficient pore structure, abundant active sites and functionalizability. In this paper, we investigated the electrocatalytic carbon dioxide reduction reactions of single-atom catalysts created by MOF two-dimensional coordination network materials constructed from transition metal-tetrahydroxybenzoquinone using density function theory calculations. The results indicate that for 10 transition metals, TM-THQ single levels ranging from Sc to Zn, the metal atom binding energy to the THQ is large enough to allow the metal atoms to be stably dispersed in the THQ monolayer. The Ni-THQ catalyst does not compete with the HER reaction in an electrocatalytic CO [Formula: see text] reduction. The primary product of reduction for Sc-THQ is HCOOH, but the major product of Co-THQ is HCHO. The main product of Cu-THQ is CO, while the main product of six catalysts, Ti, V, Cr, Mn, Fe, and Zn, is CH [Formula: see text]. The limit potential and overpotential of Ti-THQ are the highest, 1.043 V and 1.212 V, respectively. The overpotentials of the other monolayer catalysts ranged from 0.172 to 0.952 V, and they were all relatively low. Therefore, we forecast that the TM-HQ monolayer will show powerful activity in electrocatalytic carbon dioxide reduction, making it a prospective electrocatalyst for carbon dioxide reduction.