Corrosion Resistant Multilayered Electrode Comprising Ni3N Nanoarray Overcoated with NiFe‐Phytate Complex for Boosted Oxygen Evolution in Seawater Electrolysis

Abstract Engineering high‐performance oxygen evolution reaction (OER) anode material with high activity, selectivity, and strong robustness against chloride corrosion is critical to advance seawater electrolysis for large‐scale production of H 2 , yet a daunting challenge. Herein it is reported for the first time, the engineer of a multilayered electrode consisting of Ni foam‐supported Ni 3 N porous nanosheet array decorated with NiFe‐phytate coordination complex overlayer (NF/Ni 3 N@NiFe‐PA) via a facile interfacial coordination assembly, for remarkably boosted and sustained OER in alkaline seawater electrolysis. Benefitting from regulated electronic state by synergism between Ni and Fe species, boosted proton‐coupled electron transfer via accelerating proton movement with the aid of incorporated phytic acid as proton transfer relay, and promoted mass transfer rendered by unique superhydrophilic and superaerophobic property, the resulting NF/Ni 3 N@NiFe‐PA demonstrates prominent OER activity in seawater. Impressively, integrating anticorrosive Ni 3 N with NiFe‐PA complex and in situ generated NiFeOOH can collaboratively contribute to chloride repelling, leading to exceptional corrosion resistance of the electrode. This work affords a novel paradigm to engineer active and corrosion‐resistive anode for selective OER in saline water electrolysis via simultaneous geometric and electronic structural manipulation.