Molecular-Scale Insight into the Structure, Stability, and Electrochemistry of Ceria Nanoparticles

摘要

Cerium's unique chemistry has been exploited in numerous applications, ranging from catalysis to oxygen storage. However, structural ambiguities in Ce materials impair efforts to understand these oxidation and catalysis mechanisms, particularly for nanosized ceria (CeO2), which exhibits increased catalytic efficacy compared with bulk ceria. Guided by the aqueous chemistry of other tetravalent metals (e.g., Th?, Pu?, Zr~(IV)), we use a molecular-scale approach to examine the electronic and structural influences driving Ce chemistry. Specifically, we report the isolation, structural characterization, and electrochemical behavior of two polynuclear Ce~(IV) clusters that can be considered as the smallest CeO2 nanoparticles.