Atomically Dispersed Fe-Co Bimetallic Catalysts for the Promoted Electroreduction of Carbon Dioxide

The electroreduction reaction of CO(2) (ECO(2)RR) requires high-performance catalysts to convert CO(2) into useful chemicals. Transition metal-based atomically dispersed catalysts are promising for the high selectivity and activity in ECO(2)RR. This work presents a series of atomically dispersed Co, Fe bimetallic catalysts by carbonizing the Fe-introduced Co-zeolitic-imidazolate-framework (C–Fe–Co–ZIF) for the syngas generation from ECO(2)RR. The synergistic effect of the bimetallic catalyst promotes CO production. Compared to the pure C–Co–ZIF, C–Fe–Co–ZIF facilitates CO production with a CO Faradaic efficiency (FE) boost of 10%, with optimal FE(CO) of 51.9%, FE(H2) of 42.4% at − 0.55 V, and CO current density of 8.0 mA cm(−2) at − 0.7 V versus reversible hydrogen electrode (RHE). The H(2)/CO ratio is tunable from 0.8 to 4.2 in a wide potential window of − 0.35 to − 0.8 V versus RHE. The total FE(CO+H2) maintains as high as 93% over 10 h. The proper adding amount of Fe could increase the number of active sites and create mild distortions for the nanoscopic environments of Co and Fe, which is essential for the enhancement of the CO production in ECO(2)RR. The positive impacts of Cu–Co and Ni–Co bimetallic catalysts demonstrate the versatility and potential application of the bimetallic strategy for ECO(2)RR. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-021-00746-9.