Ammonia mediated electrostatic adsorption synthesis of paired subnanoclusters with enhanced hydrogen oxidation performance.
basic_science · Level V
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- Record sourced from PubMed, PMID 42265133.
- Also identified by DOI 10.1038/s41467-026-74322-3.
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Abstract
Sub-nanoclusters (sub-NCs) hold promise for the alkaline hydrogen oxidation reaction yet struggle with precise atomic dispersion and structural stability. Here, we report an ammonia-mediated electrostatic adsorption strategy that enables the synthesis of tunable paired metal-metal oxide sub-NCs, exemplified by Pt<sub>SA</sub>RuRh-MO<sub>x</sub> (SA represents single-atom sites, M = Cr, Mo, V, Ti, Ta, Zr). Electrostatic interactions between cationic PtRuRh<sup>δ+</sup> and oxo-/fluoro-anions (e.g., CrO<sub>4</sub><sup>2-</sup>, MoO<sub>4</sub><sup>2-</sup>, VO<sub>3</sub><sup>-</sup>, TiF<sub>6</sub><sup>2-</sup>, TaF<sub>7</sub><sup>2-</sup> and ZrF<sub>6</sub><sup>2-</sup>) control phase pairing during pyrolysis. The optimized Pt<sub>SA</sub>RuRh-CrO<sub>x</sub> demonstrates competitive mass activity (13.81 A mg<sup>-1</sup>, 58-fold that of commercial Pt/C) and delivers a peak power density of 1.43 W cm<sup>-2</sup> in an alkaline membrane fuel cell, with stable operation exceeding 200 h. In situ spectroscopy and simulations reveal that the synergistic Ru/Rh sites, electronically modulated by the paired CrO<sub>x</sub>, collectively optimize H*/OH* adsorption and weaken CO* binding. This work establishes a generalizable synthetic route for the precise construction of paired sub-NCs for advanced energy conversion applications.