Grinter, DC;
Allan, M;
Yang, HJ;
Salcedo, A;
Murgida, GE;
Shaw, B-J;
Pang, CL;
... Thornton, G; + view all
(2021)
Ce=O Terminated CeO2.
Angewandte Chemie International Edition
10.1002/anie.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:14337851:media:anie202101771:anie202101771-math-0001 ×urn:x-wiley:14337851:media:anie202101771:anie202101771-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 CeO2 |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/anie.202101771 |
| Publisher version: | http://dx.doi.org/10.1002/anie.202101771 |
| Language: | English |
| Additional information: | © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. |
| Keywords: | Science & Technology, Physical Sciences, Chemistry, Multidisciplinary, Chemistry, 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/10128123 |
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