Abstract
Abstract2D conductive metal–organic frameworks (2D c‐MOFs) are promising candidates for efficient electrocatalysts for the CO2reduction reaction (CO2RR). A nitrogen‐rich tricycloquinazoline (TQ) based multitopic catechol ligand was used to coordinate with transition‐metal ions (Cu2+and Ni2+), which formed 2D graphene‐like porous sheets: M3(HHTQ)2(M=Cu, Ni; HHTQ=2,3,7,8,12,13‐Hexahydroxytricycloquinazoline). M3(HHTQ)2can be regarded as a single‐atom catalyst where Cu or Ni centers are uniformly distributed in the hexagonal lattices. Cu3(HHTQ)2exhibited superior catalytic activity towards CO2RR in which CH3OH is the sole product. The Faradic efficiency of CH3OH reached up to 53.6 % at a small over‐potential of −0.4 V. Cu3(HHTQ)2exhibited larger CO2adsorption energies and higher activities over the isostructural Ni3(HHTQ)2and the reported archetypical Cu3(HHTP)2. There is a strong dependence of both metal centers and the N‐rich ligands on the electrocatalytic performance.
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