Interstitial Cobalt in Pt Shell of Pd@Pt Mesoporous Core-Shell Nanospheres with Strong d-d Orbital Hybridization for Enhanced Electrocatalytic Ammonia Oxidation.
basic_science · Level V
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- Record sourced from PubMed, PMID 40926392.
- Also identified by DOI 10.1002/adma.202511476.
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Abstract
Ammonia oxidation reaction (AOR) is critical for efficient ammonia utilization as a hydrogen carrier, yet state-of-the-art Pt-based catalysts suffer significant activity loss due to strong <sup>*</sup>NO<sub>x</sub> species (<sup>*</sup>NO, <sup>*</sup>NO<sub>2</sub>) adsorption. Herein, Pd@Pt mesoporous core-shell nanospheres with interstitial Co in Pt shell (Pd@Pt-Co MCSN) are demonstrated as an excellent AOR electrocatalyst, which achieves a mass activity of 293.6 A g<sup>-1</sup> at 0.7 V versus RHE, 4.8-fold higher than commercial Pt/C. The interstitial Co dopant tunes the d-d orbital hybridization state, optimizes the Pt d-band center position, and facilitates electron transfer from Co to Pt, which effectively weakens the adsorption of toxic <sup>*</sup>NO<sub>x</sub> and lowers the energy barrier for N-N coupling. When integrated into a Zn-NH<sub>3</sub> battery, the catalyst enables efficient NH<sub>3</sub>-to-H<sub>2</sub> conversion with a Faradaic efficiency of 96.8% and stable operation for 30 hours at 12 mA cm<sup>-2</sup>. The work may provide a new design concept to develop advanced electrocatalysts for AOR.