Journal
SMALL
Volume 12, Issue 18, Pages 2450-2458Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.201600015
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Funding
- Connaught fund
- Alfred P. Sloan Foundation
- NSERC of Canada
- DAAD (German Academic Exchange Service) - BMBF (Federal Ministry of Education and Research)
- Bayreuth-Melbourne Colloid/Polymer-Network [57173303]
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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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