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CeOx-Induced Spatial and Electronic Modulation for General Direct Oxo Coupling in Transition Metal Hydroxides
Shuang Liu1, Tao Yang1,2, Zhi Fang3
1Institute For Carbon Neutrality, Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing, China.
None:
Electrochemical water splitting has emerged as a sustainable paradigm for hydrogen generation, where sluggish kinetics of the oxygen evolution reaction (OER) catalyzed by transition metal-based materials remain the critical bottleneck. Herein, we present a strategy that anchors CeOx nanoparticles (∼2 nm) onto two-dimensional Ni(OH)2 nanosheets, enabling dual modulation of spatial configuration and electronic states to accelerate O-O coupling. Spatially, interfacial lattice distortion between CeOx and Ni(OH)2 optimizes Ni-Ni dual-metal sites with reduced interatomic spacing. Electronically, dynamic modulation through reversible Ce3+/Ce4+ redox cycling positions Ce as an electronic regulation hub, stabilizing Ni species at the catalytically favorable +3 oxidation state through Ce─O─Ni interactions. This synergistic effect shifts the pathway from adsorbate evolution mechanism (AEM) to oxide pathway mechanism (OPM). The prepared CeOx@Ni(OH)2 achieves an overpotential of 152 mV at 10 mA cm-2 and operates continuously over 2000 h with limited performance decay. When integrated into an alkaline anion exchange membrane water electrolyzer (AEMWE), it requires 1.91 V to attain 1 A cm-2 and maintains stable operation for 450 h. This OPM activation strategy shows potential applicability across CeOx-loaded transition metal hydroxides, including Ni(OH)2, Co(OH)2, NiCo, and NiFe layered double hydroxides, offering a promising approach for alkaline OER enhancement.
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