Ce=O terminated CeO2

DOI: 10.1002/anie.202101771

Authors: David Charles Grinter (Diamond Light Source) , Michael Allan (University College London) , Hyun Jin Yang (University College London) , Agustín Salcedo (Universidad de Buenos Aires) , Gustavo E. Murgida (CNEA: Comision Nacional de Energia Atomica, Centro Atomico Constituyentes) , Bobbie-Jean Shaw (University College London (UCL)) , Chi L. Pang (University College London) , Hicham Idriss (University College London) , M. Verónica Ganduglia-Pirovano (CSIC: Consejo Superior de Investigaciones Cientificas) , Geoff Thornton (University College London)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Angewandte Chemie International Edition

State: Published (Approved)
Published: April 2021

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 CeO 2 (111)‐( [[EQUATION]] x [[EQUATION]] )R30° reconstruction of ~3 nm thick ceria islands prepared on Pt(111). This is evidenced by scanning tunnelling microscopy, low energy electron diffraction 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.

Journal Keywords: Cerium Dioxide; Multiple bonds; heterogeneous catalysis; Scanning Tunnelling Microscopy; Density functional calculations

Subject Areas: Chemistry


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Added On: 12/04/2021 09:21

Documents:
anie.202101771.pdf

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Physical Chemistry Catalysis Chemistry

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