Nickel–Nitrogen-Doped Three-Dimensional Ordered Macro-/Mesoporous Carbon as an Efficient Electrocatalyst for CO₂ Reduction to CO

Electrochemical reduction of CO2 into high value-added products is currently the effective strategy to mitigate global warming and energy storage conversion. Unfortunately, the lower selectivity, activity, and stability of electrocatalysts have been the biggest obstacle to further development. The Ni–N-doped ordered porous carbon material, which shows a unique structure and high surface area, has an excellent CO2 reduction reaction (CO2RR) activity and can also inhibit its competitive reaction-hydrogen evolution reaction (HER). Herein, we apply a simple dual-templating strategy to synthesize Ni–N-doped three-dimensional ordered macro-/mesoporous carbons (Ni–N-OMMCs) and investigate the CO2RR performance of Ni–N-OMMCs from precursors with different Ni amounts. The optimum catalyst (Ni–N-OMMC-0.6) exhibits excellent electrocatalytic activity with a maximum Faradaic efficiency of ∼98% for CO formation at −0.7 V vs the reversible hydrogen electrode (RHE) and shows a wide potential range from −0.65 to −1.0 V with a Faradaic efficiency of over 60%. In addition, after a 25 h stability test, the activity of the catalyst is only attenuated by 5.6%. This study demonstrates a promising strategy for preparing highly efficient catalysts for CO2RR.