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Selectively Coupling Ru Single Atoms to PtNi Concavities for High‐Performance Methanol Oxidation via d‐Band Center Regulation

Von Wiley-VCH zur Verfügung gestellt

Single atom-cavity coupling enables the superior activity and stability of Ru single atoms tailored PtNi nano-catalysts towards methanol oxidation, synthesized by the selective ALD. The modulated d-band center and higher diffusion barrier accounts for the unparallel activity and stability on the Ru single atoms coupled to PtNi cavities, respectively.


Abstract

Single atom tailored metal nanoparticles represent a new type of catalysts. Herein, we demonstrate a single atom-cavity coupling strategy to regulate performance of single atom tailored nano-catalysts. Selective atomic layer deposition (ALD) was conducted to deposit Ru single atoms on the surface concavities of PtNi nanoparticles (Ru-ca-PtNi). Ru-ca-PtNi exhibits a record-high activity for methanol oxidation reaction (MOR) with 2.01 A mg−1 Pt. Also, Ru-ca-PtNi showcases a significant durability with only 16 % activity loss. Operando electrochemical Fourier transform infrared spectroscopy (FTIR) and theoretical calculations demonstrate Ru single atoms coupled to cavities accelerate the CO removal by regulating d-band center position. Further, the high diffusion barrier of Ru single atoms in concavities accounts for excellent stability. The developed Ru-ca-PtNi via single atom-cavity coupling opens an encouraging pathway to design highly efficient single atom-based (electro)catalysts.

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