Abstract
Comprehending the oxygen vacancy distribution in oxide ion conductors requires structural insights over various length scales: from the local coordination preferences to the possible formation of agglomerates comprising a large number of vacancies. In Y-doped ceria, 89Y NMR enables differentiation of yttrium sites by quantification of the oxygen vacancies in their first coordination sphere. Because of the extremely low sensitivity of 89Y, longer-range information was so far not available from NMR. Herein, we utilize metal ion-based dynamic nuclear polarization, where polarization from Gd(III) dopants provides large sensitivity enhancements homogeneously throughout the bulk of the sample. This enables following 89Y–89Y homonuclear dipolar correlations and probing the local distribution of yttrium sites, which show no evidence of the formation of oxygen vacancy rich regions. The presented approach can provide valuable structural insights for designing oxide ion conductors.
Highlights
Comprehending the oxygen vacancy distribution in oxide ion conductors requires structural insights over various length scales: from the local coordination preferences to the possible formation of agglomerates comprising a large number of vacancies
Homonuclear dipolar correlations and probing the local distribution of yttrium sites, which show no evidence of the formation of oxygen vacancy rich regions
Based on diffraction data, the existence of nanodomains of Y2O3 within CeO2 has been proposed[6] and is supported by other experimental findings.[7−10] On the other hand, nuclear magnetic resonance (NMR) data suggested the preferred formation of yttrium pairs, but the absence of larger clusters,[11] in line with a structural model proposed by Małecka et al.[12,13] for Yb3+doped ceria
Summary
Comprehending the oxygen vacancy distribution in oxide ion conductors requires structural insights over various length scales: from the local coordination preferences to the possible formation of agglomerates comprising a large number of vacancies.
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