期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 12, 期 11, 页码 2964-2969出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c00221
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资金
- European Research Council (MIDNP) [803024]
- European Research Council (ERC) [803024] Funding Source: European Research Council (ERC)
Understanding the distribution of oxygen vacancies in oxide ion conductors requires structural insights at various length scales, with the current method allowing for quantification of oxygen vacancies and providing large sensitivity enhancements throughout the bulk of the sample, which is crucial for designing oxide ion conductors.
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, Y-89 NMR enables differentiation of yttrium sites by quantification of the oxygen vacancies in their first coordination sphere. Because of the extremely low sensitivity of Y-89, 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 Y-89-Y-89 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.
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