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Article Abstract
Ruthenium-based catalysts are pivotal as cost-effective alternatives to Pt for alkaline hydrogen oxidation reaction (HOR). However, they typically face irreversible deactivation above 0.2 V vs. RHE due to synergistic Ru oxidation/OH over-adsorption. We propose a Taichi-inspired TiN-TiO heterophase-segregated electron-relay mechanism that dynamically balances bidirectional electron flow (Ru→TiN electron donation and TiO→Ru electron replenishment), achieving complete activity retention (100%) even under 1.1 V operation. This potential-adaptive regulation can significantly inhibit electron redistribution and band compression under the high potential induced electric field, and effectively alleviate the d-band upshift and OH adsorption energy surge. Spatially decoupled Ti(TiN)-Ru bridge sites simultaneously adsorb OH (E = -1.40 eV) and decouple H/OH adsorption domains, eliminating competitive binding. This configuration delivers triple synergies: 1) geometric isolation of reactive intermediates adsorption, 2) potential-responsive Ru stabilization, and 3) accelerated Volmer kinetics via interfacial hydroxyl migration. The Ru/TiN-TiO catalyst achieves 100% activity retention at 1.1 V vs. RHE (vs. >60% loss for Ru/TiN) with 73.23% metallic Ru preserved after 10 h operation. This work resolves the intrinsic activity-stability trade-off in Ru HOR catalysts and establishes dynamic charge-relay interfaces as a universal design paradigm for oxidation-prone electrocatalysts.
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| http://dx.doi.org/10.1002/anie.202512285 | DOI Listing |
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