Abstract

The layered transition metal oxyhydroxides have received increasing interest owing to the efficient energy conversion performance and material stability during oxygen evolution reaction (OER). In particular, Fe-doped Ni oxyhydroxides (NiOOH) have shown the record-high OER performance in alkaline media among various catalysts. Theoretically, under-coordinated facets including Ni4+, exposed at the edges of NiOOH, were predicted to perform highly active OER. Therefore, here we suggest a rational catalyst design that exposes NiOOH edges with Fe-doping, which could improve dramatically the OER performance. This unique structure was successfully prepared by electro-anodization process of Fe‑doped Ni octahedral nanocrystals. After anodization, metallic surface of the nanocrystal was transformed to vertically aligned β‑Fe/NiOOH layers with exposed Ni4+ edge sites. Electrochemical OER and anion exchange membrane based single-cell tests recorded the overpotential of 210 mV at a current density of 10 mA cm−2GEO and stable operation for 5 days, respectively. In-situ/operando studies revealed that the cycle of Ni oxidation state between +2 and +4 assisted by Fe dopant is the key engine that greatly accelerates OER kinetics, and that the aligned β‑Fe/NiOOH layers on Ni octahedra are stable under harsh OER conditions.

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