Shape‐Dependent Interactions of Palladium Nanocrystals with Hydrogen |
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Authors: | Anna Klinkova Pavel V. Cherepanov Ilya G. Ryabinkin Martin Ho Muthupandian Ashokkumar Artur F. Izmaylov Daria V. Andreeva Eugenia Kumacheva |
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Affiliation: | 1. Department of Chemistry, University of Toronto, Toronto, Ontario, Canada;2. Physical Chemistry II, University of Bayreuth, Bayreuth, Germany;3. Physical and Environmental Sciences, University of Toronto Scarborough, Toronto, Ontario, Canada;4. The School of Chemistry, University of Melbourne, Melbourne, Victoria, Australia |
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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. |
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Keywords: | hydrogen palladium nanoparticles shape control temperature‐programmed spectroscopy thermal stability |
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