The origin of elastic anomalies in thin films of oxygen deficient ceria, CeO2 - X

Anna Kossoy; Anatoly I. Frenkel; Yishay Feldman; Ellen Wachtel; Alla Milner; Igor Lubomirsky

doi:10.1016/j.ssi.2010.09.001

The origin of elastic anomalies in thin films of oxygen deficient ceria, CeO_{2 - X}

Anna Kossoy, Anatoly I. Frenkel, Yishay Feldman, Ellen Wachtel, Alla Milner, Igor Lubomirsky

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

44 Scopus citations

Abstract

Self-supported films of CeO_1.95 display time-scale dependent elastic moduli, a phenomenon which has been termed the chemical strain effect. In order to probe the possible structural origins of this behavior, extended X-ray absorption fine structure spectroscopy and X-ray diffraction were used. Evidence was found that, although this oxygen deficient ceria appears to maintain the fluorite structure on average, the mean Ce-O bond length is shorter than the mean Ce-oxygen vacancy distance. This finding is consistent with crystallographic data from more strongly reduced ceria in which the oxygen vacancies are ordered. By studying strain induced structural changes, we show that it is possible to relate this lattice distortion to the chemical strain effect. Similar conclusions were previously reached for films of Ce _0.8Gd_0.2O_1.9. Since the ionic radii of both Gd³⁺ and Ce³⁺ are larger than that of Ce⁴⁺, we suggest that when cation dopants are larger than the host, ceria compounds containing a high concentration of oxygen vacancies may exhibit elastic anomalies.

Original language	English
Pages (from-to)	1473-1477
Number of pages	5
Journal	Solid State Ionics
Volume	181
Issue number	33-34
DOIs	https://doi.org/10.1016/j.ssi.2010.09.001
State	Published - 25 Oct 2010
Externally published	Yes

Bibliographical note

Funding Information:
I.L. wishes to acknowledge the US–Israel Binational Science Foundation , the Israel Ministry of Science and the Israeli Science Foundation for support. This research is made possible in part by the generosity of the Harold Perlman Family. AIF gratefully acknowledges the support of this work by U.S. DOE Grant No. DE-FG02-03ER15476 . The use of the NSLS beamlines was supported by U.S. DOE Contract No. DE-AC02-98CH10886 . Beamlines X18B and X19A at the NSLS are supported in part by the Synchrotron Catalysis Consortium, U.S. DOE Grant No. DE-FG02-05ER15688 .

Funding

I.L. wishes to acknowledge the US–Israel Binational Science Foundation , the Israel Ministry of Science and the Israeli Science Foundation for support. This research is made possible in part by the generosity of the Harold Perlman Family. AIF gratefully acknowledges the support of this work by U.S. DOE Grant No. DE-FG02-03ER15476 . The use of the NSLS beamlines was supported by U.S. DOE Contract No. DE-AC02-98CH10886 . Beamlines X18B and X19A at the NSLS are supported in part by the Synchrotron Catalysis Consortium, U.S. DOE Grant No. DE-FG02-05ER15688 .

Funders	Funder number
Israel Ministry of Science
Synchrotron Catalysis Consortium	DE-FG02-05ER15688
U.S. Department of Energy	DE-AC02-98CH10886, DE-FG02-03ER15476
United States-Israel Binational Science Foundation
Israel Science Foundation

Keywords

Chemical strain
Elasticity
Extended X-ray absorption fine structure spectroscopy (EXAFS)
Gadolinium-doped ceria
Thermal expansion

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10.1016/j.ssi.2010.09.001

Cite this

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title = "The origin of elastic anomalies in thin films of oxygen deficient ceria, CeO2 - X",

abstract = "Self-supported films of CeO1.95 display time-scale dependent elastic moduli, a phenomenon which has been termed the chemical strain effect. In order to probe the possible structural origins of this behavior, extended X-ray absorption fine structure spectroscopy and X-ray diffraction were used. Evidence was found that, although this oxygen deficient ceria appears to maintain the fluorite structure on average, the mean Ce-O bond length is shorter than the mean Ce-oxygen vacancy distance. This finding is consistent with crystallographic data from more strongly reduced ceria in which the oxygen vacancies are ordered. By studying strain induced structural changes, we show that it is possible to relate this lattice distortion to the chemical strain effect. Similar conclusions were previously reached for films of Ce 0.8Gd0.2O1.9. Since the ionic radii of both Gd3+ and Ce3+ are larger than that of Ce4+, we suggest that when cation dopants are larger than the host, ceria compounds containing a high concentration of oxygen vacancies may exhibit elastic anomalies.",

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note = "Funding Information: I.L. wishes to acknowledge the US–Israel Binational Science Foundation , the Israel Ministry of Science and the Israeli Science Foundation for support. This research is made possible in part by the generosity of the Harold Perlman Family. AIF gratefully acknowledges the support of this work by U.S. DOE Grant No. DE-FG02-03ER15476 . The use of the NSLS beamlines was supported by U.S. DOE Contract No. DE-AC02-98CH10886 . Beamlines X18B and X19A at the NSLS are supported in part by the Synchrotron Catalysis Consortium, U.S. DOE Grant No. DE-FG02-05ER15688 .",

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AU - Kossoy, Anna

AU - Frenkel, Anatoly I.

AU - Feldman, Yishay

AU - Wachtel, Ellen

AU - Milner, Alla

AU - Lubomirsky, Igor

N1 - Funding Information: I.L. wishes to acknowledge the US–Israel Binational Science Foundation , the Israel Ministry of Science and the Israeli Science Foundation for support. This research is made possible in part by the generosity of the Harold Perlman Family. AIF gratefully acknowledges the support of this work by U.S. DOE Grant No. DE-FG02-03ER15476 . The use of the NSLS beamlines was supported by U.S. DOE Contract No. DE-AC02-98CH10886 . Beamlines X18B and X19A at the NSLS are supported in part by the Synchrotron Catalysis Consortium, U.S. DOE Grant No. DE-FG02-05ER15688 .

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N2 - Self-supported films of CeO1.95 display time-scale dependent elastic moduli, a phenomenon which has been termed the chemical strain effect. In order to probe the possible structural origins of this behavior, extended X-ray absorption fine structure spectroscopy and X-ray diffraction were used. Evidence was found that, although this oxygen deficient ceria appears to maintain the fluorite structure on average, the mean Ce-O bond length is shorter than the mean Ce-oxygen vacancy distance. This finding is consistent with crystallographic data from more strongly reduced ceria in which the oxygen vacancies are ordered. By studying strain induced structural changes, we show that it is possible to relate this lattice distortion to the chemical strain effect. Similar conclusions were previously reached for films of Ce 0.8Gd0.2O1.9. Since the ionic radii of both Gd3+ and Ce3+ are larger than that of Ce4+, we suggest that when cation dopants are larger than the host, ceria compounds containing a high concentration of oxygen vacancies may exhibit elastic anomalies.

AB - Self-supported films of CeO1.95 display time-scale dependent elastic moduli, a phenomenon which has been termed the chemical strain effect. In order to probe the possible structural origins of this behavior, extended X-ray absorption fine structure spectroscopy and X-ray diffraction were used. Evidence was found that, although this oxygen deficient ceria appears to maintain the fluorite structure on average, the mean Ce-O bond length is shorter than the mean Ce-oxygen vacancy distance. This finding is consistent with crystallographic data from more strongly reduced ceria in which the oxygen vacancies are ordered. By studying strain induced structural changes, we show that it is possible to relate this lattice distortion to the chemical strain effect. Similar conclusions were previously reached for films of Ce 0.8Gd0.2O1.9. Since the ionic radii of both Gd3+ and Ce3+ are larger than that of Ce4+, we suggest that when cation dopants are larger than the host, ceria compounds containing a high concentration of oxygen vacancies may exhibit elastic anomalies.

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KW - Extended X-ray absorption fine structure spectroscopy (EXAFS)

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