Nature Communications · 2022 · 297 citations · 47 references
Natural SciencesChemistryMaterials ScienceCatalysisMaterials ChemistryPhysical ChemistryCatalyst DesignCatalyst PreparationCatalyst SynthesisCatalytic MaterialsCluster ChemistrySupported CatalystsActive SitesHydrogen EvolutionHydrogen Evolution CatalystsHydrogen Evolution ReactionHydrogen GenerationNoble Metal ClustersOverpotentialSingle-atom Catalysts
Abstract Platinum is the most efficient catalyst for hydrogen evolution reaction in acidic conditions, but its widespread use has been impeded by scarcity and high cost. Herein, Pt atomic clusters (Pt ACs) containing Pt-O-Pt units were prepared using Co/N co-doped carbon (CoNC) as support. Pt ACs are anchored to single Co atoms on CoNC by forming strong interactions. Pt-ACs/CoNC exhibits only 24 mV overpotential at 10 mA cm −2 and a high mass activity of 28.6 A mg −1 at 50 mV, which is more than 6 times higher than commercial Pt/C with any Pt loadings. Spectroscopic measurements and computational modeling reveal the enhanced hydrogen generation activity attributes to the charge redistribution between Pt and O atoms in Pt-O-Pt units, making Pt atoms the main active sites and O linkers the assistants, thus optimizing the proton adsorption and hydrogen desorption. This work opens an avenue to fabricate noble-metal-based ACs stabilized by single-atom catalysts with desired properties for electrocatalysis.
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Generalized Gradient Approximation Made Simple
John P. Perdew, Kieron Burke, Matthias Ernzerhof · Physical Review Letters · 1996 · 211.5K citations · Full text
Natural Sciences, Chemistry, Physics +16