Tricycloquinazoline‐Based 2D Conductive Metal–Organic Frameworks as Promising Electrocatalysts for CO2 Reduction

Abstract 2D conductive metal–organic frameworks (2D c‐MOFs) are promising candidates for efficient electrocatalysts for the CO 2 reduction reaction (CO 2 RR). A nitrogen‐rich tricycloquinazoline (TQ) based multitopic catechol ligand was used to coordinate with transition‐metal ions (Cu 2+ and Ni 2+ ), which formed 2D graphene‐like porous sheets: M 3 (HHTQ) 2 (M=Cu, Ni; HHTQ=2,3,7,8,12,13‐Hexahydroxytricycloquinazoline). M 3 (HHTQ) 2 can be regarded as a single‐atom catalyst where Cu or Ni centers are uniformly distributed in the hexagonal lattices. Cu 3 (HHTQ) 2 exhibited superior catalytic activity towards CO 2 RR in which CH 3 OH is the sole product. The Faradic efficiency of CH 3 OH reached up to 53.6 % at a small over‐potential of −0.4 V. Cu 3 (HHTQ) 2 exhibited larger CO 2 adsorption energies and higher activities over the isostructural Ni 3 (HHTQ) 2 and the reported archetypical Cu 3 (HHTP) 2 . There is a strong dependence of both metal centers and the N‐rich ligands on the electrocatalytic performance.