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Quantum size effects in ambient CO oxidation catalysed by ligand-protected gold clusters
Olga Lopez-Acevedo1, Katarzyna A Kacprzak, Jaakko Akola
1Department of Physics, Nanoscience Center, University of Jyväskylä, FI-40014 Jyväskylä, Finland.
Nature Chemistry
|December 3, 2010
Summary
Ligand-protected gold clusters catalyze oxidation reactions, with electronic quantum size effects being crucial for oxygen binding. Smaller clusters below 2 nm show significant dioxygen binding, paving the way for green chemistry applications.
Area of Science:
- Nanomaterials Science
- Catalysis
- Green Chemistry
Background:
- Gold nanoparticles (Au NPs) exhibit catalytic activity in aerobic oxidation reactions.
- Existing theories involve support effects, size-dependent transitions, and electronic interactions.
Purpose of the Study:
- To investigate the role of electronic quantum size effects in gold cluster catalysis.
- To determine the influence of the HOMO-LUMO energy gap on oxygen binding and catalytic activity.
Main Methods:
- Studied ligand-protected gold clusters with diameters ranging from 1.2 to 2.4 nm.
- Characterized cluster structure and electronic properties.
- Assessed oxygen binding and catalytic oxidation of carbon monoxide (CO).
Main Results:
- Electronic quantum size effects, specifically the HOMO-LUMO gap, are critical for activated oxygen binding.
- Significant dioxygen binding occurs only for gold clusters with core diameters below 2 nm.
- Low activation barriers were observed for the CO oxidation reaction (2CO + O(2) → 2CO(2)).
Conclusions:
- The HOMO-LUMO energy gap in gold clusters dictates their ability to bind and activate oxygen.
- Nanometre-scale gold clusters below 2 nm are promising for catalytic oxidation.
- Ligand-protected gold clusters offer a viable route for developing green chemistry applications.
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