Cu-THQ-EFG Composite for Highly Selective Electrochemical CO2 Reduction to Formate at Low Overpotentials

Abstract

Metal organic framework (MOFs) are promising materials for electrocatalysis. However, the active sites of bulk MOFs crystal normally cannot be fully utilized because of the slow reagent penetration of pores and blockage of active sites. Herein, we report a facile way to deposit copper-benzoquinoid (Cu-THQ) on the edge-functionalized graphene (EFG) which prevented material’s aggregation. EFG used as a substrate provides higher electrical conductivity and stability in water than previously utilized graphene oxide (GO). Besides, the plate-like morphology of EFG proved to be more beneficial to support the MOF, because of the functional groups on its edge regions and much lower resistance compared to the sheet GO. Therefore, EFG can boost the resultant material’s catalytic activity for CO2 electroreduction (CO2RR). Furthermore, Cu-THQ exhibits high selectivity for formate formation in CO2RR. Representing as the only CO2 reduced liquid product, formate can be separated from gaseous products and further extracted from the electrolyte for practical use. The electrocatalytic results of Cu-THQ-EFG indicate the composite exhibits a higher current density of −3 mA/cm2 and faradaic efficiency of −0.25 V vs. RHE, corresponding to 50 mV of overpotential. Moreover, it features a less negative on-set potential of −0.22 V vs. RHE, which is close to the equilibrium potential of CO2RR (−0.2 V vs. RHE) and is 0.16 V more positive than the on-set potential of Cu-THQ-GO (−0.38 V vs. RHE).