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Fast and Non-equilibrium Uptake of Hydrogen by Pd Icosahedral Nanocrystals.
Zhou, Siyu; Figueras-Valls, Marc; Shi, Yifeng; Ding, Yong; Mavrikakis, Manos; Xia, Younan.
Afiliación
  • Zhou S; School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
  • Figueras-Valls M; Department of Chemical and Biological Engineering, University of Wisconsin-Madison, Madison, WI, 53706, USA.
  • Shi Y; School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
  • Ding Y; School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
  • Mavrikakis M; Department of Chemical and Biological Engineering, University of Wisconsin-Madison, Madison, WI, 53706, USA.
  • Xia Y; School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
Angew Chem Int Ed Engl ; 62(42): e202306906, 2023 Oct 16.
Article en En | MEDLINE | ID: mdl-37528509
We report for the first time that Pd nanocrystals can absorb H via a "single-phase pathway" when particles with a proper combination of shape and size are used. Specifically, when Pd icosahedral nanocrystals of 7- and 12-nm in size are exposed to H atoms, the H-saturated twin boundaries can divide each particle into 20 smaller single-crystal units in which the formation of phase boundaries is no longer favored. As such, absorption of H atoms is dominated by the single-phase pathway and one can readily obtain PdHx with anyx in the range of 0-0.7. When switched to Pd octahedral nanocrystals, the single-phase pathway is only observed for particles of 7 nm in size. We also establish that the H-absorption kinetics will be accelerated if there is a tensile strain in the nanocrystals due to the increase in lattice spacing. Besides the unique H-absorption behaviors, the PdHx (x=0-0.7) icosahedral nanocrystals show remarkable thermal and catalytic stability toward the formic acid oxidation due tothe decrease in chemical potential for H atoms in a Pd lattice under tensile strain.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Alemania
Texto completo
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XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Alemania