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The construction of bonding interfaces between cobalt-base phosphides and N-doped carbon is considered an effective means to promote ORR catalytic performance. However, the role of different nitrogen configurations in promoting the ORR performance of cobalt-base phosphides is currently unknown. Herein, the honeycomb-like Co x P@N-doped carbon catalyst was constructed to systematically investigate the effect of different nitrogen configurations on improving the catalytic performance of Co x P. Systematic experimental investigations and density functional theory (DFT) calculations indicate that the interaction of Co with pyridinic-N not only regulates the atomic Co coordination environment but also induces strong orbital hybridization between N-p orbitals and Co-d orbitals, significantly increasing the electron density on pyridinic-N sites, which greatly increases the attraction to oxygen-containing intermediates and lowers the reaction energy barrier, thus promoting the catalytic activity for ORR. Furthermore, honeycomb morphology not only reduces the internal diffusion resistance of reactants and products as well as the relative concentration of surface reactants but also exposes more accessible active sites and increases the contact area with the electrolyte, thus greatly enhancing the oxygen reduction reaction. As expected, the asprepared catalyst exhibits ultrahigh ORR activity with a half-wave potential of 0.88 V, which is superior to that of the noble metal Pt and most previously reported non-noble metal catalysts. This study perfectly explains why cobalt-base phosphide embedded in Ndoped carbon can improve its ORR catalytic performance.

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