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  Role of Dissolved and Molecular Oxygen on Cu and PtCu Alloy Particle Structure during Laser Ablation Synthesis in Liquids

Marzun, G., Bönnemann, H., Lehmann, C., Spliethoff, B., Weidenthaler, C., & Barcikowski, S. (2017). Role of Dissolved and Molecular Oxygen on Cu and PtCu Alloy Particle Structure during Laser Ablation Synthesis in Liquids. ChemPhysChem, 18(9), 1175-1184. doi:10.1002/cphc.201601315.

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Marzun, Galina1, 2, Author
Bönnemann, Helmut3, Author           
Lehmann, Christian4, Author           
Spliethoff, Bernd4, Author           
Weidenthaler, Claudia5, Author           
Barcikowski, Stephan1, 2, Author
Affiliations:
1Technical Chemistry I and Center for Nanointegration Duisburg-Essen (CENIDE), University of Duisburg-Essen, 45141, Essen, Germany., ou_persistent22              
2NanoEnergieTechnikZentrum (NETZ), University of Duisburg-Essen, 47057, Duisburg, Germany., ou_persistent22              
3Research Group Bönnemann, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445600              
4Service Department Lehmann (EMR), Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445625              
5Research Group Weidenthaler, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1950291              

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Free keywords: alloys; colloids; copper; platinum; laser chemistry
 Abstract: The role of molecular oxygen dissolved in the solvent is often discussed as being an influential factor on particle oxidation during pulsed laser ablation in liquids. However, the formation of the particles during laser synthesis takes place under extreme conditions that enable the decomposition of the liquid medium. Reactive species of the solvent may then affect particle formation due to a chemical reaction in the reactive plasma. Experimental results show a difference between the role of dissolved molecular oxygen and the contribution from the oxygen in water molecules. Using a metallic Cu target in air-saturated water, laser ablation led to 20.5 wt % Cu, 11.5 wt %  Cu2O, and 68 wt % CuO nanoparticles, according to X-ray diffraction results. In contrast to particles obtained in air-saturated water, no CuO was observed in the colloid synthesized in a Schlenk ablation chamber in completely oxygen-free water. Under these conditions, less-oxidized nanoparticles (25 wt % Cu and 75 wt % Cu2O) were synthesized. The results show that nanoparticle oxidation during laser synthesis is mainly caused by reactive oxygen species from the decomposition of water molecules. However, the addition of molecular oxygen promotes particle oxidation. Storage of the Cu colloid in the presence of dissolved oxygen leads, due to aging, to nanostructures with a higher oxidation state than the freshly prepared colloid. The XRD pattern of the sample prepared in air-saturated acetone showed no crystalline phases, which is possibly due to small crystallites or low particle concentration. Concentration of the particles by centrifugation showed that in the large fraction (>20 nm), even less oxidized nanoparticles (46 wt % Cu and 54 wt % Cu2O) were present, although the solubility of molecular oxygen is higher in acetone than in water. The nanoparticles in acetone were stable due to a Cu-catalyzed graphite layer formed on their surfaces. The influence of the solvent on alloy synthesis is also crucial. Laser ablation of PtCu3 in air-saturated water led to separated large CuO and Pt-rich spherical nanoparticles, whereas homogeneous PtCu3 alloy nanoparticles were formed in acetone.

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Language(s): eng - English
 Dates: 2017-03-202017-05-05
 Publication Status: Published online
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/cphc.201601315
 Degree: -

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Title: ChemPhysChem
Source Genre: Journal
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Publ. Info: Weinheim, Germany : Wiley-VCH
Pages: - Volume / Issue: 18 (9) Sequence Number: - Start / End Page: 1175 - 1184 Identifier: ISSN: 1439-4235
CoNE: https://pure.mpg.de/cone/journals/resource/954925409790