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Molecularly well-defined Ni sites at heterogeneous interfaces were derived from the incorporation of Ni ions into heteroatom-doped graphene. The molecular Ni sites on graphene were redox-active. However, they showed poor activity toward oxygen evolution reaction (OER) in KOH aqueous solution. We demonstrated for the first time that the presence of Fe ions in the solution could bond at the vicinity of the Ni sites with a distance of 2.7 Å, generating molecularly sized and heterogeneous Ni-Fe sites anchored on doped graphene. These Ni-Fe sites exhibited markedly improved OER activity. The Pourbaix diagram confirmed the formation of the Ni-Fe sites and revealed that the Ni-Fe sites adsorbed HO ions with a bridge geometry, which facilitated the OER electrocatalysis.

In situ formation of molecular Ni-Fe active sites on heteroatom-doped graphene as a heterogeneous electrocatalyst toward oxygen evolution