Chem Sci. 2022 Jul 5;13(28):8388-8394. doi: 10.1039/d2sc02222b. eCollection 2022 Jul 20.
The electroreduction of CO2 to CH4 has attracted extensive attention. However, it is still a challenge to achieve high current density and faradaic efficiency (FE) for producing CH4 because the reaction involves eight electrons and four protons. In this work, we designed Cu nanoparticles supported on N-doped carbon (Cu-np/NC). It was found that the catalyst exhibited outstanding performance for the electroreduction of CO2 to CH4. The FE toward CH4 could be as high as 73.4% with a high current density of 320 mA cm-2. In addition, the mass activity could reach up to 6.4 A mgCu-1. Both experimental and theoretical calculations illustrated that the pyrrolic N in NC could accelerate the hydrogenation of *CO to the *CHO intermediate, resulting in high current density and excellent selectivity for CH4. This work conducted the first exploration of the effect of N-doped species in composites on the electrocatalytic performance of CO2 reduction.