Enhancing Oxygen Evolution Reaction Performance: Electrochemical Activation of the Biphasic CoNi/Zn(Fe,Al,Cr)2O4 via Controlled Aluminum Leaching Facilitated Surface Reconstruction

Abstract Given that the oxygen evolution reaction (OER) faces challenges due to its sluggish kinetics, development of efficient and robust OER catalytic electrodes is critical for reducing the cost of hydrogen production through electrochemical water splitting. In this study, a biphasic CoNi/Zn(Fe,Al,Cr) 2 O 4 coating, characterized by a densely organized stalagmite‐like microarray structure, is deposited on a commercial pure titanium plate, creating an exceptionally effective OER catalytic electrode. The formation of numerous metal/spinel oxide heterogeneous interfaces is demonstrated to enhance its electron transfer ability and conductivity. At high potentials, aluminum leaching and lattice oxygen consumption can facilitate deep surface reconstruction of highly active Fe‐doped CoNiOOH phase inducing electrochemical activation, further optimizing thermodynamic barrier of the fundamental reaction step. Ultimately, this electrode showcases exceptional OER catalytic performance (low overpotential of 248 and 335 mV to deliver the current density of 10 and 100 mA cm −2 ) compared to commercial IrO 2 catalyst (overpotential of ≈310 mV at 10 mA cm −2 ). Moreover, it demonstrates high current stability sustaining a current density of 500 mA cm −2 for 100 h. This work deepens the comprehension of the surface reconstruction process in OER and, more broadly, introduces a new avenue for designing and enhancing the performance of catalytic materials.