Redox behaviour of a ceria–zirconia inverse model catalyst

Michael Allan; David Grinter; Simran Dhaliwal; Chris Muryn; Thomas Forrest; Francesco Maccherozzi; Sarnjeet S. Dhesi; Geoff Thornton

doi:10.1016/j.susc.2018.12.005

Redox behaviour of a ceria–zirconia inverse model catalyst

Michael Allan, David Grinter, Simran Dhaliwal, Chris Muryn, Thomas Forrest, Francesco Maccherozzi, Sarnjeet S. Dhesi, Geoff Thornton^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

Abstract

The redox behaviour modification following the addition of zirconia to ceria nanostructures supported on Rh(111) has been investigated using a combination of Low Energy Electron Diffraction (LEED) and X-ray Photoemission Electron Microscopy (XPEEM). Soft X-ray irradiation was employed to reduce ZrO_2-x(111) supported on Rh(111) and, by introducing oxygen, the reoxidation process of the thin film was monitored. Ceria was then depositied with zirconia. Using XPEEM, we determined that the mixed metal oxide formed a phase-separated structure with CeO₂(111) nanoparticles on top of the zirconia. Upon exposure of CeO_2-x/ZrO_2-x/Rh(111) to X-ray illumination, the zirconia no longer undergoes any observable reduction while at the same time the ceria is reduced. Our results indicate a synergy between the zirconia and ceria in the phase-separated system expected in the working catalyst, with oxygen transfer between the metal oxides. This sheds light on the mechanism of the enhancement of catalytic properties seen with the addition of zirconia to ceria and highlights the oxygen storage and release ability of ceria.

Original language	English
Pages (from-to)	8-13
Number of pages	6
Journal	Surface Science
Volume	682
Early online date	11 Dec 2018
DOIs	https://doi.org/10.1016/j.susc.2018.12.005
Publication status	Published - Apr 2019

Keywords

Ceria–zirconia
Oxygen transfer
Redox
X-ray photoelectron microscopy

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10.1016/j.susc.2018.12.005

https://discovery.ucl.ac.uk/id/eprint/10063835/

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@article{eccea522c8774e66965d507a1ccea50c,

title = "Redox behaviour of a ceria–zirconia inverse model catalyst",

abstract = "The redox behaviour modification following the addition of zirconia to ceria nanostructures supported on Rh(111) has been investigated using a combination of Low Energy Electron Diffraction (LEED) and X-ray Photoemission Electron Microscopy (XPEEM). Soft X-ray irradiation was employed to reduce ZrO2-x(111) supported on Rh(111) and, by introducing oxygen, the reoxidation process of the thin film was monitored. Ceria was then depositied with zirconia. Using XPEEM, we determined that the mixed metal oxide formed a phase-separated structure with CeO2(111) nanoparticles on top of the zirconia. Upon exposure of CeO2-x/ZrO2-x/Rh(111) to X-ray illumination, the zirconia no longer undergoes any observable reduction while at the same time the ceria is reduced. Our results indicate a synergy between the zirconia and ceria in the phase-separated system expected in the working catalyst, with oxygen transfer between the metal oxides. This sheds light on the mechanism of the enhancement of catalytic properties seen with the addition of zirconia to ceria and highlights the oxygen storage and release ability of ceria.",

keywords = "Ceria–zirconia, Oxygen transfer, Redox, X-ray photoelectron microscopy",

author = "Michael Allan and David Grinter and Simran Dhaliwal and Chris Muryn and Thomas Forrest and Francesco Maccherozzi and Dhesi, {Sarnjeet S.} and Geoff Thornton",

note = "Funding Information: This work was supported by the E uropean Research Council Advanced Grant ENERGYSURF (GT), European Cooperation in Science and Technology Action CM1104 , EPSRC through grant EP/L015277/1 , the Royal Society through a Wolfson Merit Award to GT, and the Alexander von Humboldt Stiftung. We acknowledge Diamond Light Source for access to beamline I06 under proposal SI17343. Publisher Copyright: {\textcopyright} 2018 Elsevier B.V. Copyright: Copyright 2019 Elsevier B.V., All rights reserved.",

year = "2019",

month = apr,

doi = "10.1016/j.susc.2018.12.005",

language = "English",

volume = "682",

pages = "8--13",

journal = "Surface Science",

issn = "0039-6028",

publisher = "Elsevier BV",

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TY - JOUR

T1 - Redox behaviour of a ceria–zirconia inverse model catalyst

AU - Allan, Michael

AU - Grinter, David

AU - Dhaliwal, Simran

AU - Muryn, Chris

AU - Forrest, Thomas

AU - Maccherozzi, Francesco

AU - Dhesi, Sarnjeet S.

AU - Thornton, Geoff

N1 - Funding Information: This work was supported by the E uropean Research Council Advanced Grant ENERGYSURF (GT), European Cooperation in Science and Technology Action CM1104 , EPSRC through grant EP/L015277/1 , the Royal Society through a Wolfson Merit Award to GT, and the Alexander von Humboldt Stiftung. We acknowledge Diamond Light Source for access to beamline I06 under proposal SI17343. Publisher Copyright: © 2018 Elsevier B.V. Copyright: Copyright 2019 Elsevier B.V., All rights reserved.

PY - 2019/4

Y1 - 2019/4

N2 - The redox behaviour modification following the addition of zirconia to ceria nanostructures supported on Rh(111) has been investigated using a combination of Low Energy Electron Diffraction (LEED) and X-ray Photoemission Electron Microscopy (XPEEM). Soft X-ray irradiation was employed to reduce ZrO2-x(111) supported on Rh(111) and, by introducing oxygen, the reoxidation process of the thin film was monitored. Ceria was then depositied with zirconia. Using XPEEM, we determined that the mixed metal oxide formed a phase-separated structure with CeO2(111) nanoparticles on top of the zirconia. Upon exposure of CeO2-x/ZrO2-x/Rh(111) to X-ray illumination, the zirconia no longer undergoes any observable reduction while at the same time the ceria is reduced. Our results indicate a synergy between the zirconia and ceria in the phase-separated system expected in the working catalyst, with oxygen transfer between the metal oxides. This sheds light on the mechanism of the enhancement of catalytic properties seen with the addition of zirconia to ceria and highlights the oxygen storage and release ability of ceria.

AB - The redox behaviour modification following the addition of zirconia to ceria nanostructures supported on Rh(111) has been investigated using a combination of Low Energy Electron Diffraction (LEED) and X-ray Photoemission Electron Microscopy (XPEEM). Soft X-ray irradiation was employed to reduce ZrO2-x(111) supported on Rh(111) and, by introducing oxygen, the reoxidation process of the thin film was monitored. Ceria was then depositied with zirconia. Using XPEEM, we determined that the mixed metal oxide formed a phase-separated structure with CeO2(111) nanoparticles on top of the zirconia. Upon exposure of CeO2-x/ZrO2-x/Rh(111) to X-ray illumination, the zirconia no longer undergoes any observable reduction while at the same time the ceria is reduced. Our results indicate a synergy between the zirconia and ceria in the phase-separated system expected in the working catalyst, with oxygen transfer between the metal oxides. This sheds light on the mechanism of the enhancement of catalytic properties seen with the addition of zirconia to ceria and highlights the oxygen storage and release ability of ceria.

KW - Ceria–zirconia

KW - Oxygen transfer

KW - Redox

KW - X-ray photoelectron microscopy

U2 - 10.1016/j.susc.2018.12.005

DO - 10.1016/j.susc.2018.12.005

M3 - Article

AN - SCOPUS:85058688689

SN - 0039-6028

VL - 682

SP - 8

EP - 13

JO - Surface Science

JF - Surface Science

ER -

Redox behaviour of a ceria–zirconia inverse model catalyst

Abstract

Keywords

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