Tricycloquinazoline‐Based 2D Conductive Metal–Organic Frameworks as Promising Electrocatalysts for CO<sub>2</sub>Reduction
Jingjuan Liu, Dan Yang, Yi Zhou, Guang Zhang, Guolong Xing, Yunpeng Liu, Yanhang Ma, Osamu Terasaki, Shubin Yang, Long Chen
Abstract
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.