Abstract
Abstract Developing highly active, cost-effective, and environmental friendly oxygen evolution reaction (OER) electrocatalysts facilitates various (photo)electrochemical processes. In this work, Fe3N nanoparticles encapsulated into N-doped graphene nanoshells (Fe3N@NG) as OER electrocatalysts in alkaline media were reported. Both the experimental and theoretical comparison between Fe3N@NG and Fe3N/NG, specifically including in situ Mossbauer analyses, demonstrated that the NG nanoshells improved interfacial electron transfer process from Fe3N to NG to form high-valence Fe4+ ions (Fe4+@NG), thus modifying electronic properties of the outer NG shells and subsequently electron transfer from oxygen intermediate to NG nanoshells for OER catalytic process. Meanwhile, the NG nanoshells also protected Fe-based cores from forming OER inactive and insulated Fe2O3, leading to high OER stability. As a result, the as-formed Fe4+@NG shows one of the highest electrocatalytic efficiency among reported Fe-based OER electrocatalysts, which can as well highly improve the photoelectrochemical water oxidation when used as the co-catalysts for the Fe2O3 nanoarray photoanode.
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