Endogenous <sup>17</sup>O Dynamic Nuclear Polarization of Gd-Doped CeO<sub>2</sub> from 100 to 370 K

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  • Michael A. Hope
    Institut des Sciences et Ingéniere Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), Lausanne CH-1015, Switzerland
  • Snædís Björgvinsdóttir
    Institut des Sciences et Ingéniere Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), Lausanne CH-1015, Switzerland
  • David M. Halat
    Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.
  • Georges Menzildjian
    Centre de RMN à; Très Hauts Champs, Université de Lyon (CNRS/ENS de Lyon/UCB-Lyon 1), Villeurbanne 69100, France
  • Zhuoran Wang
    Centre de RMN à; Très Hauts Champs, Université de Lyon (CNRS/ENS de Lyon/UCB-Lyon 1), Villeurbanne 69100, France
  • Bowen Zhang
    Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS, U.K.
  • Judith L. MacManus-Driscoll
    Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS, U.K.
  • Anne Lesage
    Centre de RMN à; Très Hauts Champs, Université de Lyon (CNRS/ENS de Lyon/UCB-Lyon 1), Villeurbanne 69100, France
  • Moreno Lelli
    Magnetic Resonance Center (CERM), Department of Chemistry “Ugo Schiff”, University of Florence, Sesto Fiorentino 50019, Italy
  • Lyndon Emsley
    Institut des Sciences et Ingéniere Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), Lausanne CH-1015, Switzerland
  • Clare P. Grey
    Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.
  • DSpace at Cambridge pro (8.1)

書誌事項

公開日
2021-08-18
権利情報
  • https://doi.org/10.15223/policy-029
  • https://doi.org/10.15223/policy-037
  • https://doi.org/10.15223/policy-045
DOI
  • 10.1021/acs.jpcc.1c04479
  • 10.17863/cam.73922
公開者
American Chemical Society (ACS)

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説明

17O NMR is an invaluable tool to study the structure and dynamics of oxide materials, but remains challenging to apply in many systems. Even with isotopic enrichment, studies of samples with low masses and/or concentrations of the active species, such as thin films or interfaces, are limited by low sensitivity. Here we show how endogenous dynamic nuclear polarisation (DNP) can dramatically improve sensitivity in the oxide-ion conductor Gd-doped CeO2, with a 17O enhancement factor of 652 at 100 K. This is the highest enhancement observed so far by endogenous DNP or Gd3+ DNP, which is explained in terms of the electron paramagnetic resonance characteristics. The DNP properties are studied as a function of Gd concentration for both enriched and natural abundance samples and the buildup behaviour shows that spin diffusion in 17O-enriched samples improves sensitivity by relaying hyperpolarisation throughout the sample. Notably, efficient hyperpolarisation could still be achieved at elevated temperatures, with enhancement factors of 320 at room temperature and 150 at 370 K, paving the way for characterisation of materials under operational conditions. Finally, the application of endogenous Gd3+ DNP is illustrated with the study of interfaces in vertically aligned nanocomposite thin films comprised of Gd-CeO2 nanopillars embedded in a SrTiO3 matrix, where DNP affords selective enhancement of the different phases and enables a previously infeasible two-dimensional correlation experiment to be performed showing spin diffusion between Gd-CeO2 and the solid–solid interface.

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