An Anion‐Regulation Strategy for Scalable Fe‐Rich NiFe Electrodes With Disorder Lattices Toward Industrial Water Electrolysis

ABSTRACT Elevating Fe‐involved sites in NiFe catalysts can accelerate water‐oxidation kinetics, but it remains challenging to fabricate scalable, durable Fe‐rich NiFe‐based electrodes. We demonstrate that anion regulation is an effective and scalable strategy for fabricating Fe‐rich NiFe catalysts with improved catalytic activity and durability. The Fe content has increased by 70%–90% in the NiFe layer deposited in a chloride‐type electrolyte relative to a sulfate‐type electrolyte. The Fe‐rich electrode exhibits an overpotential of 243 mV@100 mA cm ⁻² and demonstrates excellent stability for 100 h at 1000 mA cm ⁻² . Scaling electrodes to 10 × 10 cm ² and implementing them in an industrial‐level anion‐exchange membrane water electrolysis (AEMWE) with 14 cells, it achieves a voltage of 2.0 V@1500 mA cm ⁻² and a stable voltage of 1.74 V@500 mA cm ⁻² for over 200 h. A key insight from EXAFS and in situ Raman reveals that the Fe‐rich electrode exhibits pronounced coordination defects and greater lattice disorder. DFT calculations also indicate that increasing the Fe content reduces the binding energy of ^* O by NiFeOOH. This study presents a practical approach to enhancing the activity and stability of NiFe electrodes, demonstrating potential for large‐scale applications of AEMWEs.