Abstract

Rational design of iron-nitrogen-carbon (Fe-N-C) oxygen reduction reaction (ORR) catalysts simultaneously increasing the intrinsic activity and density of active site remains a huge challenge. Herein the coexistence of single-atomic Fe and Cu sites decorated nitrogen-doped porous carbon has been successfully fabricated by hydrothermal synthesis of Fe, Cu co-doped ZIF-8 in the presence of Fe and Cu foam with subsequent NH3 pyrolysis. The X-ray absorption spectra confirmed the atomically dispersed Fe and Cu species with Fe-N4 and Cu-N4 coordination structures in the resultant FeCu SACs/NC catalyst. Meanwhile, the introduction of Cu has been experimentally and theoretically demonstrated to modulate the electronic structure of Fe active sites during the desorption of *OH intermediate process, as well as increase the density of Fe active sites, thereby effectively enhancing the intrinsic activity and selectivity toward the ORR.

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