Synergistic catalysis between atomically dispersed Fe and a pyrrolic-N-C framework for CO2 electroreduction

Abstract

Atomically dispersed Fe immobilized within N-doped carbon nanosheets (Fe-SA) is successfully synthesized. The optimal Fe-SA catalyst achieves a high faradaic efficiency of ca. 90% for CO₂ electroreduction toward CO at a low overpotential of 0.47 V. A series of controlled tests show that there is a synergistic effect between the Fe centers and the pyrrolic-N-C framework which facilitates catalytic activity. Specifically, pyrrolic-N-C sites with high local electron density increase the initial CO₂ adsorption while positively charged Fe enhances the water dissociation to provide a proton source for further CO₂ reduction.