Cadmium-based metal-organic frameworks for high-performance electrochemical CO_(2) reduction to CO over wide potential range

摘要

Electrochemical CO_(2)reduction(ECR)powered by renewable energy sources provides a sustainable avenue to producing carbon-neutral fuels and chemicals.The design and development of high performance,cost-effective,and stable catalysts for ECR remain a focus of intense research.Here,we report a novel electrocatalyst,two-dimensional cadmium-based 1,4-benzenedicarboxylate metal-organic frameworks(Cd-BDC MOFs)which can effectively convert CO_(2)to CO with a faradaic efficiency(FE)of more than80.0%over the voltage range between-0.9 and-1.1 V(versus reversible hydrogen electrode,vs.RHE)in 0.1 mol·L^(-1) CO_(2)-saturated KHCO_(3)solution with an H-type cell,reaching up to 88.9%at-1.0 V(vs.RHE).The performance outperforms commercial CdO and many other MOF-based materials demonstrated in prior literature.The catalytic property can be readily tuned by manipulating synthesis conditions as well as electrolyte type.Especially,high CO FEs exceeding 90.0%can be attained on the Cd-BDC electrode at potentials ranging from-0.16 to-1.06 V(vs.RHE)in 0.5 mol·L^(-1) KHCO_(3)solution by using a gas diffusion electrode cell system.The maximum CO FE approaches~97.6%at-0.26 V(vs.RHE)and the CO partial geometric current density is as high as about 108.1 mA·cm^(-2) at-1.1 V(vs.RHE).This work offers an efficient,low cost,and alternative electrocatalyst for CO_(2)transformation.