Strain and architecture-tuned reactivity in ceria nanostructures; Enhanced catalytic oxidation of CO to CO 2

Thi X T Sayle, Michelle Cantoni, Umananda M. Bhatta, Stephen C. Parker, Simon R. Hall, Günter Möbus, Marco Molinari, David Reid, Sudipta Seal, Dean C. Sayle

Research output: Contribution to journalArticle

54 Citations (Scopus)

Abstract

Atomistic simulations reveal that the chemical reactivity of ceria nanorods is increased when tensioned and reduced when compressed promising strain-tunable reactivity; the reactivity is determined by calculating the energy required to oxidize CO to CO 2 by extracting oxygen from the surface of the nanorod. Visual reactivity "fingerprints", where surface oxygens are colored according to calculated chemical reactivity, are presented for ceria nanomaterials including: nanoparticles, nanorods, and mesoporous architectures. The images reveal directly how the nanoarchitecture (size, shape, channel curvature, morphology) and microstructure (dislocations, grain-boundaries) influences chemical reactivity. We show the generality of the approach, and its relevance to a variety of important processes and applications, by using the method to help understand: TiO 2 nanoparticles (photocatalysis), mesoporous ZnS (semiconductor band gap engineering), MgO (catalysis), CeO 2/YSZ interfaces (strained thin films; solid oxide fuel cells/nanoionics), and Li-MnO 2 (lithiation induced strain; energy storage).

LanguageEnglish
Pages1811-1821
Number of pages11
JournalChemistry of Materials
Volume24
Issue number10
DOIs
Publication statusPublished - 22 May 2012
Externally publishedYes

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Chemical reactivity
Catalytic oxidation
Cerium compounds
Carbon Monoxide
Nanorods
Nanostructures
Oxygen
Nanoparticles
Photocatalysis
Solid oxide fuel cells (SOFC)
Dislocations (crystals)
Nanostructured materials
Energy storage
Catalysis
Grain boundaries
Energy gap
Semiconductor materials
Thin films
Microstructure

Cite this

Sayle, T. X. T., Cantoni, M., Bhatta, U. M., Parker, S. C., Hall, S. R., Möbus, G., ... Sayle, D. C. (2012). Strain and architecture-tuned reactivity in ceria nanostructures; Enhanced catalytic oxidation of CO to CO 2. Chemistry of Materials, 24(10), 1811-1821. https://doi.org/10.1021/cm3003436
Sayle, Thi X T ; Cantoni, Michelle ; Bhatta, Umananda M. ; Parker, Stephen C. ; Hall, Simon R. ; Möbus, Günter ; Molinari, Marco ; Reid, David ; Seal, Sudipta ; Sayle, Dean C. / Strain and architecture-tuned reactivity in ceria nanostructures; Enhanced catalytic oxidation of CO to CO 2. In: Chemistry of Materials. 2012 ; Vol. 24, No. 10. pp. 1811-1821.
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Sayle, TXT, Cantoni, M, Bhatta, UM, Parker, SC, Hall, SR, Möbus, G, Molinari, M, Reid, D, Seal, S & Sayle, DC 2012, 'Strain and architecture-tuned reactivity in ceria nanostructures; Enhanced catalytic oxidation of CO to CO 2', Chemistry of Materials, vol. 24, no. 10, pp. 1811-1821. https://doi.org/10.1021/cm3003436

Strain and architecture-tuned reactivity in ceria nanostructures; Enhanced catalytic oxidation of CO to CO 2. / Sayle, Thi X T; Cantoni, Michelle; Bhatta, Umananda M.; Parker, Stephen C.; Hall, Simon R.; Möbus, Günter; Molinari, Marco; Reid, David; Seal, Sudipta; Sayle, Dean C.

In: Chemistry of Materials, Vol. 24, No. 10, 22.05.2012, p. 1811-1821.

Research output: Contribution to journalArticle

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T1 - Strain and architecture-tuned reactivity in ceria nanostructures; Enhanced catalytic oxidation of CO to CO 2

AU - Sayle, Thi X T

AU - Cantoni, Michelle

AU - Bhatta, Umananda M.

AU - Parker, Stephen C.

AU - Hall, Simon R.

AU - Möbus, Günter

AU - Molinari, Marco

AU - Reid, David

AU - Seal, Sudipta

AU - Sayle, Dean C.

PY - 2012/5/22

Y1 - 2012/5/22

N2 - Atomistic simulations reveal that the chemical reactivity of ceria nanorods is increased when tensioned and reduced when compressed promising strain-tunable reactivity; the reactivity is determined by calculating the energy required to oxidize CO to CO 2 by extracting oxygen from the surface of the nanorod. Visual reactivity "fingerprints", where surface oxygens are colored according to calculated chemical reactivity, are presented for ceria nanomaterials including: nanoparticles, nanorods, and mesoporous architectures. The images reveal directly how the nanoarchitecture (size, shape, channel curvature, morphology) and microstructure (dislocations, grain-boundaries) influences chemical reactivity. We show the generality of the approach, and its relevance to a variety of important processes and applications, by using the method to help understand: TiO 2 nanoparticles (photocatalysis), mesoporous ZnS (semiconductor band gap engineering), MgO (catalysis), CeO 2/YSZ interfaces (strained thin films; solid oxide fuel cells/nanoionics), and Li-MnO 2 (lithiation induced strain; energy storage).

AB - Atomistic simulations reveal that the chemical reactivity of ceria nanorods is increased when tensioned and reduced when compressed promising strain-tunable reactivity; the reactivity is determined by calculating the energy required to oxidize CO to CO 2 by extracting oxygen from the surface of the nanorod. Visual reactivity "fingerprints", where surface oxygens are colored according to calculated chemical reactivity, are presented for ceria nanomaterials including: nanoparticles, nanorods, and mesoporous architectures. The images reveal directly how the nanoarchitecture (size, shape, channel curvature, morphology) and microstructure (dislocations, grain-boundaries) influences chemical reactivity. We show the generality of the approach, and its relevance to a variety of important processes and applications, by using the method to help understand: TiO 2 nanoparticles (photocatalysis), mesoporous ZnS (semiconductor band gap engineering), MgO (catalysis), CeO 2/YSZ interfaces (strained thin films; solid oxide fuel cells/nanoionics), and Li-MnO 2 (lithiation induced strain; energy storage).

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KW - mesoporous

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KW - nanorod

KW - simulated crystallization

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