Stainless Steel Activation for Efficient Alkaline Oxygen Evolution in Advanced Electrolyzers

Abstract Designing robust and cost‐effective electrocatalysts for efficient alkaline oxygen evolution reaction (OER) is of great significance in the field of water electrolysis. In this study, an electrochemical strategy to activate stainless steel (SS) electrodes for efficient OER is introduced. By cycling the SS electrode within a potential window that encompasses the Fe(II)↔Fe(III) process, its OER activity can be enhanced to a great extent compared to using a potential window that excludes this redox reaction, decreasing the overpotential at current density of 100 mA cm⁻² by 40 mV. Electrochemical characterization, Inductively Coupled Plasma – Optical Emission Spectroscopy, and operando Raman measurements demonstrate that the Fe leaching at the SS surface can be accelerated through a Fe → γ‐Fe₂O₃ → Fe₃O₄ or FeO → Fe²⁺ (aq.) conversion process, leading to the sustained exposure of Cr and Ni species. While Cr leaching occurs during its oxidation process, Ni species display higher resistance to leaching and gradually accumulate on the SS surface in the form of OER‐active Fe‐incorporated NiOOH species. Furthermore, a potential‐pulse strategy is also introduced to regenerate the OER‐activity of 316‐type SS for stable OER, both in the three‐electrode configuration (without performance decay after 300 h at 350 mA cm⁻²) and in an alkaline water electrolyzer (≈30 mV cell voltage increase after accelerated stress test‐AST). The AST‐stabilized cell can still reach 1000 and 4000 mA cm⁻² at cell voltages of 1.69 and 2.1 V, which makes it competitive with state‐of‐the‐art electrolyzers based on ion‐exchange membrane using Ir‐based anodes.