Amorphous/Crystalline Phases Mixed Nanosheets Array Rich in Oxygen Vacancies Boost Oxygen Evolution Reaction of Spinel Oxides in Alkaline Media

As promising oxygen evolution reaction (OER) catalysts, spinel-type oxides face the bottleneck of weak adsorption for oxygen-containing intermediates, so it is challenging to make a further breakthrough in remarkably lowering the OER overpotential. In this study, a novel strategy is proposed to substantially enhance the OER activity of spinel oxides based on amorphous/crystalline phases mixed spinel FeNi2O4 nanosheets array, enriched with oxygen vacancies, in situ grown on a nickel foam (NF). This unique architecture is achieved through a one-step millisecond laser direct writing method. The presence of amorphous phases with abundant oxygen vacancies significantly enhances the adsorption of oxygen-containing intermediates and changes the rate-determining step from OH*-> O* to O*-> OOH*, which greatly reduces the thermodynamic energy barrier. Moreover, the crystalline phase interweaving with amorphous domains serves as a conductive shortcut to facilitate rapid electron transfer from active sites in the amorphous domain to NF, guaranteeing fast OER kinetics. Such an anodic electrode exhibits a nearly ten fold enhancement in OER intrinsic activity compared to the pristine counterpart. Remarkably, it demonstrates record-low overpotentials of 246 and 315 mV at 50 and 500 mA cm-2 in 1 m KOH with superior long-term stability, outperforming other NiFe-based spinel oxides catalysts. An amorphous/crystalline phase mixed nanosheetss array rich in oxygen vacancies is constructed to enhance both oxygen-containing intermediates adsorptions and the charge transfer rate of spinel FeNi2O4. As demonstrated by theoretical and experimental investigations, the energy barrier of oxygen evolution reaction rate-limiting step is greatly reduced. The excellent oxygen revolution reaction performance and synthesis of large-area electrodes manifest high potential for industrial applications. image