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Reversible Transformation Mechanism between Pd4 and Pd10 Clusters and Their Catalytic Hydrogenation Activities.
Lei Li1, Xiongkai Tang1, Yani Gu1
1New Cornerstone Science Laboratory, State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and National & Local Joint Engineering Research Center of Preparation Technology of Nanomaterials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
This study reveals how palladium nanoclusters transform structurally, driven by Pd2(0) and hydrogen bonds. These transformations impact their catalytic activity in olefin hydrogenation, with Pd10 clusters showing high regioselectivity.
Area of Science:
- Materials Science
- Nanotechnology
- Catalysis
Background:
- Understanding cluster structural transformations is key to cluster growth mechanisms and structure-property relationships.
- Palladium (Pd) nanoclusters are of significant interest due to their catalytic properties.
Purpose of the Study:
- To investigate the reversible structural transformation mechanisms of two Pd nanoclusters: Pd4 and Pd10.
- To correlate the structural differences of Pd4 and Pd10 clusters with their catalytic performance in olefin hydrogenation.
Main Methods:
- UV-vis absorption spectroscopy
- Electrospray ionization mass spectrometry (ESI-MS)
- Nuclear magnetic resonance (NMR)
- Single crystal X-ray diffraction (SC-XRD)
Main Results:
- Zerovalent Pd2(0) and AcOH···OAc- hydrogen bonds are crucial for cluster transformation.
- Pd4 and Pd10 clusters exhibit distinct structural differences.
- Pd10 clusters show high regioselective hydrogenation of olefins, attributed to mobile OAc- ligands.
Conclusions:
- The study elucidates the mutual transformation mechanisms of Pd nanoclusters.
- Structural variations in Pd nanoclusters directly influence their catalytic properties.
- Mobile ligands on Pd10 clusters are vital for creating active sites in catalytic hydrogenation.
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