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Despite of high conductivity and reducing ability, transition metal nanoparticles tend to aggregate and unavoidably impact the selectivity during the proton‐coupled reduction process of CO2RR. New strategy to regulate and utilize the electronic property of transition‐metal particles allows for effective tuning of eCO2RR activity. Through simple creation of N‐doped carbon shells surrounding Ni nanoparticles and controlling the amount and arrangement of the N atoms, successful and long‐lasting electrochemical reduction of CO2 was accomplished. The inherent HER activity was almost completely suppressed. It exhibited FECO above 90 % in a 500 mV potential window, with the optimal up to 96.5 % at −0.78 V vs RHE. In flow cell electrolysis, a current density of 289.4 mA/cm2 was achieved with Faradic efficiency of 96.4 % towards CO. The results of control experiments using different catalysts imply that electron transfer between Ni core and shells was significantly influenced by the property of N atoms. High content of graphitic nitrogen is crucial for the catalytic performance. [ABSTRACT FROM AUTHOR]

Cerium and boron are commonly used components to tune the acidic/basic property of catalysts in industry. In this work, cerium or boron‐doped copper‐based catalysts (xM−Cu/SiO2, M=Ce/B) were prepared with the ammonia‐evaporation method. Both X‐ray diffraction and Auger electron spectroscopy revealed that Cu+ content increased along with the Ce‐doping, but decreased by B‐doping. NH3‐Temperature Program Desorption results showed no change in the acidity of Ce‐doped catalysts, while significant amounts of medium‐strong acid sites appeared after B‐doping. Application in ethylene carbonate hydrogenation indicates the promoting role of Ce‐dopant in methanol production, while boron exhibits negative effects. The significant difference can be attributed to distinctive acidic/basic properties of Ce/B dopants, which affect the interaction between Cu and Si in the precursors, and thus adjust the ratio of Cu+/(Cu++Cu0). [ABSTRACT FROM AUTHOR]