Curvature-engineered interfacial hydrogen-bond networks driving proton-coupled electron transfer boosts hydrogen oxidation in alkaline fuel cells.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41381507.
- Also identified by DOI 10.1038/s41467-025-66360-0 and PMC identifier 12749165.
- Licence recorded as CC BY-NC-ND.
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Abstract
Precise manipulation of interfacial microenvironments within the electrical double layer remains a fundamental challenge, primarily due to dynamic structural rearrangements and competitive adsorption processes during reactions. Here, we employ nanoscale curvature engineering to construct three RuIr-based electrocatalysts with precisely controlled surface curvatures, establishing a direct correlation between geometric effects and hydrogen oxidation reaction efficiency. Finite-element simulations coupled with electrochemical analysis reveal that concave nanocage (CNC) morphology enhances localized electric field, simultaneously weakening adsorbed hydrogen (H<sub>ads</sub>) binding and promoting its subsequent cooperative oxidation with more OH<sub>ads</sub>. Operando spectroscopy and ab initio molecular dynamics simulations demonstrate that high-curvature RuIr CNC drives ordered O-down H<sub>2</sub>O alignment at the electrode-electrolyte interface, strengthening hydrogen-bond networks and accelerating proton-coupled electron transfer kinetics. The optimized RuIr CNCs achieve a mass activity of 7.51 mA μg<sup>-1</sup> (three-electrode system) and enable a peak power density of 1.52 W cm<sup>-2</sup> (H<sub>2</sub>/O<sub>2</sub> anion-exchange membrane fuel cell), with stability over 150 hours.