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Oxygen Vacancy Distribution in Yttrium-Doped Ceria from (89)Y–(89)Y Correlations via Dynamic Nuclear Polarization Solid-State NMR

[Image: see text] 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, (89)Y NMR enabl...

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Autores principales: Jardón-Álvarez, Daniel, Kahn, Nitzan, Houben, Lothar, Leskes, Michal
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2021
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8006133/
https://www.ncbi.nlm.nih.gov/pubmed/33730494
http://dx.doi.org/10.1021/acs.jpclett.1c00221
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author Jardón-Álvarez, Daniel
Kahn, Nitzan
Houben, Lothar
Leskes, Michal
author_facet Jardón-Álvarez, Daniel
Kahn, Nitzan
Houben, Lothar
Leskes, Michal
author_sort Jardón-Álvarez, Daniel
collection PubMed
description [Image: see text] 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, (89)Y NMR enables differentiation of yttrium sites by quantification of the oxygen vacancies in their first coordination sphere. Because of the extremely low sensitivity of (89)Y, 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 (89)Y–(89)Y 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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spelling pubmed-80061332021-03-30 Oxygen Vacancy Distribution in Yttrium-Doped Ceria from (89)Y–(89)Y Correlations via Dynamic Nuclear Polarization Solid-State NMR Jardón-Álvarez, Daniel Kahn, Nitzan Houben, Lothar Leskes, Michal J Phys Chem Lett [Image: see text] 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, (89)Y NMR enables differentiation of yttrium sites by quantification of the oxygen vacancies in their first coordination sphere. Because of the extremely low sensitivity of (89)Y, 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 (89)Y–(89)Y 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. American Chemical Society 2021-03-17 2021-03-25 /pmc/articles/PMC8006133/ /pubmed/33730494 http://dx.doi.org/10.1021/acs.jpclett.1c00221 Text en © 2021 The Authors. Published by American Chemical Society Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Jardón-Álvarez, Daniel
Kahn, Nitzan
Houben, Lothar
Leskes, Michal
Oxygen Vacancy Distribution in Yttrium-Doped Ceria from (89)Y–(89)Y Correlations via Dynamic Nuclear Polarization Solid-State NMR
title Oxygen Vacancy Distribution in Yttrium-Doped Ceria from (89)Y–(89)Y Correlations via Dynamic Nuclear Polarization Solid-State NMR
title_full Oxygen Vacancy Distribution in Yttrium-Doped Ceria from (89)Y–(89)Y Correlations via Dynamic Nuclear Polarization Solid-State NMR
title_fullStr Oxygen Vacancy Distribution in Yttrium-Doped Ceria from (89)Y–(89)Y Correlations via Dynamic Nuclear Polarization Solid-State NMR
title_full_unstemmed Oxygen Vacancy Distribution in Yttrium-Doped Ceria from (89)Y–(89)Y Correlations via Dynamic Nuclear Polarization Solid-State NMR
title_short Oxygen Vacancy Distribution in Yttrium-Doped Ceria from (89)Y–(89)Y Correlations via Dynamic Nuclear Polarization Solid-State NMR
title_sort oxygen vacancy distribution in yttrium-doped ceria from (89)y–(89)y correlations via dynamic nuclear polarization solid-state nmr
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8006133/
https://www.ncbi.nlm.nih.gov/pubmed/33730494
http://dx.doi.org/10.1021/acs.jpclett.1c00221
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