Nitrogen-doped carbon nanomaterials have become some of the most effective carriers for transition metal-based electrocatalysts towards the oxygen evolution reaction. However, the specific active nitrogen species in nitrogen-doped carriers remains unclear up to now. To identify the active nitrogen species, herein, we prepare nitrogen-doped carbon nanospheres containing different types of nitrogen species and a small amount of Fe atoms. Electrochemical tests demonstrate that the Fe/nitrogen-doped carbon nanospheres with more graphitic nitrogen exhibit much higher activity for the oxygen evolution reaction than those with more pyridinic nitrogens and pyrrolic nitrogens in alkaline media, revealing that the graphitic nitrogen is the active species that greatly improves the activity of Fe catalysts. Density functional theory calculations further reveal that the graphitic nitrogen enhances the activity and stability of Fe-based catalysts mainly through increasing the adsorption energy, charge and spin densities of the Fe atoms loaded around it. These findings provide a brand-new perspective for rationally designing more effective transition metal-based electrocatalysts for the oxygen evolution reaction through controlling the active graphitic nitrogen distribution in carbon carriers.
This journal is © The Royal Society of Chemistry.