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Cerium oxyhydroxide clusters: formation, structure, and reactivity.

Frederic Aubriet1, Jean-Jacques Gaumet, Wibe A de Jong

  • 1Laboratoire de Spectrométrie de Masse et Chimie Laser, Institut Jean Barriol Fedération de Recherche 2843, Université Paul Verlaine-Metz, Metz, France.

The Journal of Physical Chemistry. A
|May 13, 2009
PubMed
Summary

Researchers created cerium oxyhydroxide cluster anions using laser pulses. These clusters, formed with nitrogen gas and water, exhibit varying hydroxylation, with specific structures influencing water molecule bonding and stability.

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Synthesis of Nine-atom Deltahedral Zintl Ions of Germanium and their Functionalization with Organic Groups
08:15

Synthesis of Nine-atom Deltahedral Zintl Ions of Germanium and their Functionalization with Organic Groups

Published on: February 11, 2012

Area of Science:

  • Materials Science
  • Inorganic Chemistry
  • Surface Science

Background:

  • Cerium oxide (ceria) and its derivatives are crucial in catalysis and materials science.
  • Understanding the structure and properties of cerium-based clusters is key to developing advanced materials.
  • Laser ablation techniques offer a method for generating novel cluster species.

Purpose of the Study:

  • To synthesize and characterize cerium oxyhydroxide cluster anions.
  • To investigate the hydroxylation behavior and structural properties of these clusters.
  • To explore the influence of cluster size and structure on stability and reactivity.

Main Methods:

  • Laser ablation of ceric oxide particles in a nitrogen gas atmosphere.
  • Mass spectrometry to detect and analyze cluster anions.
  • Density Functional Theory (DFT) modeling to elucidate structures and energetics.

Main Results:

  • Cerium oxyhydroxide cluster anions, [Ce(x)O(y)(OH)(z)](-), were successfully produced.
  • Hydroxylation extent varies with cluster size, with notable deviations for Ce(3) and Ce(6) clusters.
  • DFT calculations confirmed hydrolysis, identified symmetric structures, and explained hydroxylation trends based on specific cluster architectures.
  • Evidence for reduced cerium (Ce(III)) species and superoxide derivatives was observed.
  • Ce(13) clusters showed enhanced stability, suggesting a dehydrated Keggin-type structure.

Conclusions:

  • The hydroxylation of cerium oxyhydroxide clusters is strongly dependent on their size and specific atomic arrangement.
  • Structural factors, such as hexagonal versus octahedral configurations, dictate the degree of hydrolysis.
  • Larger clusters exhibit a greater propensity for incorporating reduced Ce(III) centers.
  • The formation of stable, dehydrated Keggin-type structures is possible for specific cerium cluster sizes.