Exploring Electrocatalytic CO2 Reduction Over Materials Derived from Cu‐Based Metal‐Organic Frameworks

Abstract The direct valorization of carbon dioxide (CO 2 ) into value‐added chemicals offers an efficient and attractive approach to promoting carbon neutrality. Among the available methods, the electrocatalytic CO 2 reduction reaction (eCO 2 RR) for producing multicarbon products (C 2+ ) is gaining attention owing to its simplicity. However, achieving selective control over product formation remains a challenge. One key issue is the lack of a reliable correlation between the physicochemical properties of electrocatalytic materials and their activity and selectivity. To address this gap, we conducted a model study in which carbonized Cu x Zn y @C materials, derived from metal‐organic frameworks (MOFs), were synthesized with varying Cu/Zn ratios. The pyrolyzed bimetallic MOFs retained key properties of the original MOFs while also developing new characteristics. These subtle changes in physicochemical properties influenced product selectivity. The findings of our study revealed that higher Zn doping favors the formation of single‐carbon (C 1 ) products, whereas it is less favorable for multicarbon (C 2+ ) products. Optimizing the Cu/Zn ratio was emphasized through characterization techniques, which will help guide the design of improved electrocatalytic systems for the eCO 2 RR process.