Peering into the Formation of Cerium Oxide Colloidal Particles in Solution by In Situ Small-Angle X-ray Scattering
- Elifkübra ÖzkanElifkübra ÖzkanInstitute of Physical Chemistry, Justus-Liebig University, Heinrich-Buff-Ring 17, 35392 Giessen, GermanyUmicore AG & Co. KG, Rodenbacher Chaussee 4, 63457 Hanau, GermanyMore by Elifkübra Özkan
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- Felix BadaczewskiFelix BadaczewskiInstitute of Physical Chemistry, Justus-Liebig University, Heinrich-Buff-Ring 17, 35392 Giessen, GermanyCenter for Materials Research (LaMa), Justus-Liebig University, Heinrich-Buff-Ring 16, 35392 Giessen, GermanyMore by Felix Badaczewski
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- Pascal CopPascal CopInstitute of Physical Chemistry, Justus-Liebig University, Heinrich-Buff-Ring 17, 35392 Giessen, GermanyMore by Pascal Cop
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- Sebastian WernerSebastian WernerInstitute of Physical Chemistry, Justus-Liebig University, Heinrich-Buff-Ring 17, 35392 Giessen, GermanyMore by Sebastian Werner
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- Alexander HofmannAlexander HofmannUmicore AG & Co. KG, Rodenbacher Chaussee 4, 63457 Hanau, GermanyMore by Alexander Hofmann
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- Martin VotsmeierMartin VotsmeierUmicore AG & Co. KG, Rodenbacher Chaussee 4, 63457 Hanau, GermanyTechnical University Darmstadt, 64287 Darmstadt, GermanyMore by Martin Votsmeier
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- Heinz AmenitschHeinz AmenitschInstitute of Inorganic Chemistry, Graz University of Technology, Stremayrgasse 9, 8010 Graz, AustriaMore by Heinz Amenitsch
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- Bernd M. Smarsly*Bernd M. Smarsly*Email: [email protected]Institute of Physical Chemistry, Justus-Liebig University, Heinrich-Buff-Ring 17, 35392 Giessen, GermanyCenter for Materials Research (LaMa), Justus-Liebig University, Heinrich-Buff-Ring 16, 35392 Giessen, GermanyMore by Bernd M. Smarsly
Abstract
The formation of CeO2 colloidal particles upon heating an aqueous solution of (NH4)2Ce(NO3)6 to 100 °C was investigated by time-resolved in situ SAXS analysis using synchrotron radiation, providing absolute intensity data. In particular, the experiments were performed by applying different temperatures between room temperature and 100 °C as well as under variation of the ionic strength and concentration. Using validated SAXS evaluation tools (SASfit and McSAS software), the analyses revealed the presence of two types of particle populations possessing average dimensions of ca. 2 nm and 5–15 nm, with the latter being agglomerates of the 2 nm particles rather than single crystallites. The analysis revealed not only the changes in the size, but also the relative volume fractions of these two CeO2 particle populations as a function of the aforementioned parameters. Increasing the temperature increases the number of the 5−15 nm agglomerates on one hand by the enhanced nucleation rate of the primary particles. On the other hand, especially at high temperatures (90 and 100 °C) the larger agglomerate particles precipitate, resulting in interesting trends in the fractions of the two populations as a function of time, temperature, ionic strength, and precursor concentration. The experimental studies are complemented by calculating colloidal interaction energies based on classical DLVO theory. Thereby, this study provides detailed insight into the nucleation, growth, and agglomeration of CeO2 nanoparticles. The primary objective of this study is to provide a better understanding of the nucleation and growth of particles by the hydrolysis of the tetravalent cerium ion in aqueous solutions.
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