Abstract
Simultaneously increasing the activity and stability of the single-atom active sites of M-N-C catalysts is critical but remains a great challenge. Here, we report an Fe-N-C catalyst with nitrogen-coordinated iron clusters and closely surrounding Fe-N(4) active sites for oxygen reduction reaction in acidic fuel cells. A strong electronic interaction is built between iron clusters and satellite Fe-N(4) due to unblocked electron transfer pathways and very short interacting distances. The iron clusters optimize the adsorption strength of oxygen reduction intermediates on Fe-N(4) and also shorten the bond amplitude of Fe-N(4) with incoherent vibrations. As a result, both the activity and stability of Fe-N(4) sites are increased by about 60% in terms of turnover frequency and demetalation resistance. This work shows the great potential of strong electronic interactions between multiphase metal species for improvements of single-atom catalysts.