MOF-Derived N-Doped Carbon-Wrapped Ni Electrocatalyst for Highly Efficient Electrochemical CO₂ Reduction to CO

Electrochemical CO2 reduction reaction (ECO2RR) represents a promising approach for attaining a neutral carbon cycle and the sustainable production of value-added chemicals. However, fabricating nonprecious metals catalysts with high selectivity within a broad potential window and excellent stability under tough electrolytic conditions remains a great challenge. Herein, we developed an in situ confining strategy to prepare metal–organic frameworks derived N-doped carbon-wrapped nickel nanoparticles for ECO2RR to CO. The optimal Ni-MOF@NC exhibited a remarkable Faradaic efficiency (FE) of 99% and a partial current density of −26.3 mA/cm2 toward CO at −1.0 V (vs RHE). The CO FE maintained a high value of over 90% within a wide potential range of −0.8 to −1.4 V (vs RHE). The well-designed control experiments reveal that the high catalytic activity is attributed to the N-doped carbon layer encapsulating the Ni particles. Furthermore, benefiting from the protective carbon–nitrogen shell, the Ni-MOF@NC composite exhibited robust durability under a high local alkaline environment. This work offers a promising design principle for constructing N-doped carbon-wrapped nickel electrocatalysts for ECO2RR with high catalytic activity and CO selectivity.