ABSTRACT Constructing robust, binder‐free electrodes with intimate substrate‐catalyst contact is pivotal for advancing alkaline water electrolysis but remains impeded by complex synthesis procedures and weak interfacial adhesion. Herein, we present a rapid flash combustion synthesis strategy to fabricate a self‐anchored Ni‐Co‐Fe spinel oxide electrode (Ni 1 Co 1 Fe 1 O‐NF) via in situ substrate diffusion. By exploiting the transient high‐temperature thermal shock generated by igniting Co/Fe precursors on Ni foam, Ni atoms from the substrate are driven to diffuse outwards and react with the precursor layer. This process simultaneously establishes a compositionally graded, metallurgically bonded interface and a hierarchical porous network formed by gas expansion. The resulting Ni 1 Co 1 Fe 1 O‐NF electrode exhibits exceptional oxygen evolution reaction (OER) performance, requiring an overpotential of 254 mV to deliver a current density of 100 mA cm −2 and maintaining industrial‐level stability for over 1 week. Density functional theory (DFT) calculations reveal that the in situ incorporated Ni optimizes the electronic structure and triggers a switch from the conventional adsorbate evolution mechanism (AEM) to the energetically favorable lattice‐oxygen‐mediated (LOM) pathway. This work provides a scalable, energy‐efficient paradigm for designing monolithic, high‐performance electrodes for sustainable hydrogen production.
Liu et al. (Thu,) studied this question.