Hierarchical Ni/N/C Single‐Site Catalyst Achieving Industrial‐Level Current Density and Ultra‐Wide Potential Plateau of High CO Faradic Efficiency for CO2 Electroreduction

Abstract

AbstractThe practical applications of CO2 electroreduction to CO driven by renewable electricity should simultaneously meet the requests of industrial‐level CO partial current density (JCO) at least 100 mA cm−2, wide potential window of high CO faradic efficiency (FECO), and low cost. Herein, a new strategy is reported to construct porous hierarchical Ni/N/C single‐site catalyst with excellent catalytic activity via coating Ni‐containing ZIF‐8 on mesostructured basic magnesium carbonate template followed by pyrolysis. The abundant micropores facilitate the formation of numerous edge‐hosted Ni‐N4 sites with high intrinsic activity, and the interconnected macro/mesopores much promote CO2 delivery and CO release for the full expression of intrinsic activity. Consequently, the catalyst exhibits the industrial‐level JCO of 105–462 mA cm−2 at the potential range of −0.6∼−1.3 V with ultra‐wide high FECO plateau (>90%@−0.4∼−1.3 V), showing great promise for practical application. This study provides a general synthetic strategy to explore high‐performance hierarchical M/N/C electrocatalysts.