title: Shape-Dependent Interactions of Palladium Nanocrystals with Hydrogen.
abstract: Elucidation of the nature of hydrogen interactions with palladium nanoparticles is expected to play an important role in the development of new catalysts and hydrogen-storage nanomaterials. A facile scaled-up synthesis of uniformly sized single-crystalline palladium nanoparticles with various shapes, including regular nanocubes, nanocubes with protruded edges, rhombic dodecahedra, and branched nanoparticles, all stabilized with a mesoporous silica shell is developed. Interaction of hydrogen with these nanoparticles is studied by using temperature-programmed desorption technique and by performing density functional theory modeling. It is found that due to favorable arrangement of Pd atoms on their surface, rhombic dodecahedral palladium nanoparticles enclosed by {110} planes release a larger volume of hydrogen and have a lower desorption energy than palladium nanocubes and branched nanoparticles. These results underline the important role of {110} surfaces in palladium nanoparticles in their interaction with hydrogen. This work provides insight into the mechanism of catalysis of hydrogenation/dehydrogenation reactions by palladium nanoparticles with different shapes.
authors.affiliation: Department of Chemistry, University of Toronto, Toronto, Ontario, M5S 3H6, Canada.
authors.forename: Anna
authors.initials: A
authors.lastname: Klinkova
authors.affiliation: Physical Chemistry II, University of Bayreuth, Bayreuth, 95440, Germany.
authors.forename: Pavel V
authors.initials: PV
authors.lastname: Cherepanov
authors.affiliation: Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Ontario, M1C 1A4, Canada.
authors.forename: Ilya G
authors.initials: IG
authors.lastname: Ryabinkin
authors.affiliation: Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Ontario, M1C 1A4, Canada.
authors.forename: Martin
authors.initials: M
authors.lastname: Ho
authors.affiliation: The School of Chemistry, University of Melbourne, Melbourne, Victoria, 3010, Australia.
authors.forename: Muthupandian
authors.initials: M
authors.lastname: Ashokkumar
authors.affiliation: Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Ontario, M1C 1A4, Canada.
authors.forename: Artur F
authors.initials: AF
authors.lastname: Izmaylov
authors.affiliation: Physical Chemistry II, University of Bayreuth, Bayreuth, 95440, Germany.
authors.forename: Daria V
authors.initials: DV
authors.lastname: Andreeva
authors.affiliation: Department of Chemistry, University of Toronto, Toronto, Ontario, M5S 3H6, Canada.
authors.forename: Eugenia
authors.initials: E
authors.lastname: Kumacheva
keywords: hydrogen; palladium nanoparticles; shape control; temperature-programmed spectroscopy; thermal stability