Journal
ACS CATALYSIS
Volume 5, Issue 2, Pages 1335-1343Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cs501612g
Keywords
Pd@Pt; core-shell; nanocatalysis; hydrogenation; p-chloronitrobenzene
Categories
Funding
- Ministry of Science and Technology of China [2012DFA40550]
- Ningbo Municipal Natural Science Foundation [2013A610038]
- National Key Basis Research Program of China [2013CB934800]
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This study investigates the structural stability of small Pd@Pt core@shell octahedral nanoparticles (NPs) and their shell thickness dependent catalytic performance for p-chloronitrobenzene hydrogenation with H-2. The 6-8 nm Pd@Pt octahedral NPs are prepared by a sequential reduction method, and the characterization results confirm that Pd@Pt octahedral NPs with one to four atomic Pt layers can be controllably synthesized. The Pd@Pt octahedral NPs with one atomic Pt layer demonstrate excellent structural stability with the maintenance of core shell structures as well as high catalytic stability during cycle to cycle catalytic p-chloronitrobenzene hydrogenation reactions. The alumina-supported Pd@Pt octahedral NPs illustrate a superior catalytic performance relative to individual Pt and Pd and their physical mixtures. Theoretical calculations by density functional theory suggest that the unexpected structural stability for Pd@Pt octahedral NPs with thin Pt shells and their corresponding catalytic stability during hydrogenation reactions can be ascribed to the strong binding between Pt surfaces and reactants/products in catalytic reactions. The enhanced catalytic performance of Pd@Pt octahedral NPs possibly originates from the core-shell interaction, which adjusts the electronic state of surface Pt atoms to be suitable for selective p-chloronitrobenzene hydrogenation.
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