Boosting the bifunctional oxygen electrocatalytic performance of atomically dispersed Fe site via atomic Ni neighboring

Atomically dispersed metal-nitrogen-carbon complexes on carbon supports have drawn tremendous attention in the electrocatalysis fields. Herein, we managed the synthesis of atomically dispersed binary Ni x Fe 100-x -NC (x = 0–100) materials with tunable Ni/Fe ratios and investigated their underneath synergy effects for the enhancement of oxygen reduction (ORR) and oxygen evolution reactions (OER). EXAFS revealed the abundant presence of Ni(N 3 )-Fe(N 3 )-C n moieties in Ni 66 Fe 34 -NC sample. XPS fine scans indicated deep synergy of dual-site Ni/Fe that favored more charge localized over Ni/Fe sites. Electrochemical measurments showed that the Ni 66 Fe 34 -NC delivered a very high ORR half-wave potential ( E 1/2 ) of 0.85 V and a low OER overpotential of 467 mV at ∼10 mA cm −2 ( E j=10). The Fe site with Ni neighboring, as suggested by DFT simulations and in-situ Raman, was the responsible site for both ORR and OER. Furthermore, the Ni 66 Fe 34 -NC-assembled Zn-air battery afforded large specific power density and extraordinary cycling stability.