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Ce=O Terminated CeO(2)

Multiply bonded lanthanide oxo groups are rare in coordination compounds and have not previously been reported for a surface termination of a lanthanide oxide. Here we report the observation of a Ce=O terminated ceria surface in a CeO(2)(111)‐([Formula: see text] × [Formula: see text] )R30° reconstr...

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Autores principales: Grinter, David C., Allan, Michael, Yang, Hyun Jin, Salcedo, Agustín, Murgida, Gustavo E., Shaw, Bobbie‐Jean, Pang, Chi L., Idriss, Hicham, Ganduglia‐Pirovano, M. Verónica, Thornton, Geoff
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8251574/
https://www.ncbi.nlm.nih.gov/pubmed/33826220
http://dx.doi.org/10.1002/anie.202101771
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author Grinter, David C.
Allan, Michael
Yang, Hyun Jin
Salcedo, Agustín
Murgida, Gustavo E.
Shaw, Bobbie‐Jean
Pang, Chi L.
Idriss, Hicham
Ganduglia‐Pirovano, M. Verónica
Thornton, Geoff
author_facet Grinter, David C.
Allan, Michael
Yang, Hyun Jin
Salcedo, Agustín
Murgida, Gustavo E.
Shaw, Bobbie‐Jean
Pang, Chi L.
Idriss, Hicham
Ganduglia‐Pirovano, M. Verónica
Thornton, Geoff
author_sort Grinter, David C.
collection PubMed
description Multiply bonded lanthanide oxo groups are rare in coordination compounds and have not previously been reported for a surface termination of a lanthanide oxide. Here we report the observation of a Ce=O terminated ceria surface in a CeO(2)(111)‐([Formula: see text] × [Formula: see text] )R30° reconstruction of ≈3 nm thick ceria islands prepared on Pt(111). This is evidenced by scanning tunnelling microscopy (STM), low energy electron diffraction (LEED) and high‐resolution electron energy loss spectroscopy (HREELS) measurements in conjunction with density functional theory (DFT) calculations. A Ce=O stretching frequency of 775 cm(−1) is observed in HREELS, compared with 766 cm(−1) calculated by DFT. The calculations also predict that the Ce=O bond is weak, with an oxygen vacancy formation energy of 0.85 eV. This could play an important role in the facile removal of lattice oxygen from CeO(2), accompanied by the reduction of Ce(IV) to Ce(III), which is a key attribute of ceria‐based systems in connection with their unique catalytic properties.
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spelling pubmed-82515742021-07-06 Ce=O Terminated CeO(2) Grinter, David C. Allan, Michael Yang, Hyun Jin Salcedo, Agustín Murgida, Gustavo E. Shaw, Bobbie‐Jean Pang, Chi L. Idriss, Hicham Ganduglia‐Pirovano, M. Verónica Thornton, Geoff Angew Chem Int Ed Engl Communications Multiply bonded lanthanide oxo groups are rare in coordination compounds and have not previously been reported for a surface termination of a lanthanide oxide. Here we report the observation of a Ce=O terminated ceria surface in a CeO(2)(111)‐([Formula: see text] × [Formula: see text] )R30° reconstruction of ≈3 nm thick ceria islands prepared on Pt(111). This is evidenced by scanning tunnelling microscopy (STM), low energy electron diffraction (LEED) and high‐resolution electron energy loss spectroscopy (HREELS) measurements in conjunction with density functional theory (DFT) calculations. A Ce=O stretching frequency of 775 cm(−1) is observed in HREELS, compared with 766 cm(−1) calculated by DFT. The calculations also predict that the Ce=O bond is weak, with an oxygen vacancy formation energy of 0.85 eV. This could play an important role in the facile removal of lattice oxygen from CeO(2), accompanied by the reduction of Ce(IV) to Ce(III), which is a key attribute of ceria‐based systems in connection with their unique catalytic properties. John Wiley and Sons Inc. 2021-05-11 2021-06-14 /pmc/articles/PMC8251574/ /pubmed/33826220 http://dx.doi.org/10.1002/anie.202101771 Text en © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH https://creativecommons.org/licenses/by/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Communications
Grinter, David C.
Allan, Michael
Yang, Hyun Jin
Salcedo, Agustín
Murgida, Gustavo E.
Shaw, Bobbie‐Jean
Pang, Chi L.
Idriss, Hicham
Ganduglia‐Pirovano, M. Verónica
Thornton, Geoff
Ce=O Terminated CeO(2)
title Ce=O Terminated CeO(2)
title_full Ce=O Terminated CeO(2)
title_fullStr Ce=O Terminated CeO(2)
title_full_unstemmed Ce=O Terminated CeO(2)
title_short Ce=O Terminated CeO(2)
title_sort ce=o terminated ceo(2)
topic Communications
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8251574/
https://www.ncbi.nlm.nih.gov/pubmed/33826220
http://dx.doi.org/10.1002/anie.202101771
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