Tricycloquinazoline Based 2D Conductive Metal‐Organic Frameworks as Promising Electrocatalysts for CO2 Reduction
2021
Developing highly efficient electrocatalysts for CO 2 reduction is of critical importance. Good conductivity and abundant catalytic sites feature ideal electrocatalysts. Two-dimensional conductive metal-organic frameworks (2D c -MOFs) are promising candidates in this regard as efficient electrocatalysts for CO 2 reduction reaction (CO 2 RR). Herein, a nitrogen-rich tricycloquinazoline (TQ) based multitopic catechol ligand was employed to coordinate with transition metal ions (Cu 2+ and Ni 2+ ), which therefore, 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 vs RHE. Theoretical calculations and experimental results further indicated that, 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 . The current work reveals strong dependence of both metal centers and the N -rich ligands on the electrocatalytic performance, and provide new possibilities to develop novel 2D c -MOF-based electrocatalysts toward efficient CO 2 RR.
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