Grinter, DC;
Allan, M;
Yang, HJ;
Salcedo, A;
Murgida, GE;
Shaw, B;
Pang, CL;
... Thornton, G; + view all
(2021)
Ce=O Terminated CeO 2.
Angewandte Chemie
10.1002/ange.202101771.
(In press).
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Abstract
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 CeO2(111)-(urn:x-wiley:00448249:media:ange202101771:ange202101771-math-0001 ×urn:x-wiley:00448249:media:ange202101771:ange202101771-math-0002 )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 CeO2, accompanied by the reduction of CeIV to CeIII, which is a key attribute of ceria-based systems in connection with their unique catalytic properties.
| Type: | Article |
|---|---|
| Title: | Ce=O Terminated CeO 2 |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/ange.202101771 |
| Publisher version: | https://doi.org/10.1002/ange.202101771 |
| Language: | English |
| Additional information: | This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ |
| Keywords: | cerium dioxide, density functional calculations, heterogeneous catalysis, multiple bonds, scanning tunnelling microscopy |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10128226 |
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