The Nanocrystalline SnO 2 –TiO 2 System‒Part II: Surface Energies and Thermodynamic Stability

Miagava, Joice; da Silva, Andre L.; Navrotsky, Alexandra; Castro, Ricardo H. R.; Gouvêa, Douglas; Rohrer, ed., G.

doi:10.1111/jace.13954

Title: The Nanocrystalline SnO ₂ –TiO ₂ System‒Part II: Surface Energies and Thermodynamic Stability

Abstract

The thermodynamic stability of nanocrystalline SnO ₂ –TiO ₂ solid solutions was studied experimentally. Microcalorimetry of water adsorption revealed a systematic decrease in the surface energy with increasing Ti ⁴⁺ content in the SnO ₂ ‐rich compositions, consistent with previous reports of Ti ⁴⁺ segregation on the surface. The surface energy change was accompanied by an increase in the magnitude of the heat of water adsorption, also indicating a modification of the SnO ₂ surface by Ti ⁴⁺ . Supporting the water adsorption data, calculations using high‐temperature oxide melt solution calorimetry data also suggest a decrease in the interface energies. A thermodynamic analysis showed that the observed surface energy decrease is responsible for an increase in the stability of solid solutions in the nanophase regime. Although a miscibility gap is expected in this system from bulk phase diagrams, the surface energy contribution modifies the bulk trend and promotes extensive solid solutions when the surface area is above a critical value dependent on the surface energy and the bulk enthalpy of mixing.

Authors:

Miagava, Joice ^[1]; da Silva, Andre L. ^[2]; Navrotsky, Alexandra ^[2]; Castro, Ricardo H. R. ^[2]; Gouvêa, Douglas ^[3]; Rohrer, ed., G.

Peter A. Rock Thermochemistry Laboratory &, NEAT ORU University of California Davis California 95616, Department of Metallurgical and Materials Engineering University of São Paulo São Paulo 05508‐030 Brazil
Peter A. Rock Thermochemistry Laboratory &, NEAT ORU University of California Davis California 95616
Department of Metallurgical and Materials Engineering University of São Paulo São Paulo 05508‐030 Brazil

Publication Date:: Thu Oct 15 00:00:00 EDT 2015

Sponsoring Org.:: USDOE

OSTI Identifier:: 1401402

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Journal of the American Ceramic Society

Additional Journal Information:: Journal Name: Journal of the American Ceramic Society Journal Volume: 99 Journal Issue: 2; Journal ID: ISSN 0002-7820

Publisher:: Wiley-Blackwell

Country of Publication:: United States

Language:: English

Citation Formats


                    Miagava, Joice, da Silva, Andre L., Navrotsky, Alexandra, Castro, Ricardo H. R., Gouvêa, Douglas, and Rohrer, ed., G. The Nanocrystalline SnO 2 –TiO 2 System‒Part II: Surface Energies and Thermodynamic Stability.  United States: N. p., 2015. 
Web.  doi:10.1111/jace.13954.

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                    Miagava, Joice, da Silva, Andre L., Navrotsky, Alexandra, Castro, Ricardo H. R., Gouvêa, Douglas, & Rohrer, ed., G. The Nanocrystalline SnO 2 –TiO 2 System‒Part II: Surface Energies and Thermodynamic Stability.  United States.  https://doi.org/10.1111/jace.13954

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                    Miagava, Joice, da Silva, Andre L., Navrotsky, Alexandra, Castro, Ricardo H. R., Gouvêa, Douglas, and Rohrer, ed., G. Thu .  
"The Nanocrystalline SnO 2 –TiO 2 System‒Part II: Surface Energies and Thermodynamic Stability".  United States.  https://doi.org/10.1111/jace.13954.

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@article{osti_1401402,

  title        = {The Nanocrystalline SnO 2 –TiO 2 System‒Part II: Surface Energies and Thermodynamic Stability},

  author       = {Miagava, Joice and da Silva, Andre L. and Navrotsky, Alexandra and Castro, Ricardo H. R. and Gouvêa, Douglas and Rohrer, ed., G.},

  abstractNote = {The thermodynamic stability of nanocrystalline SnO 2 –TiO 2 solid solutions was studied experimentally. Microcalorimetry of water adsorption revealed a systematic decrease in the surface energy with increasing Ti 4+ content in the SnO 2 ‐rich compositions, consistent with previous reports of Ti 4+ segregation on the surface. The surface energy change was accompanied by an increase in the magnitude of the heat of water adsorption, also indicating a modification of the SnO 2 surface by Ti 4+ . Supporting the water adsorption data, calculations using high‐temperature oxide melt solution calorimetry data also suggest a decrease in the interface energies. A thermodynamic analysis showed that the observed surface energy decrease is responsible for an increase in the stability of solid solutions in the nanophase regime. Although a miscibility gap is expected in this system from bulk phase diagrams, the surface energy contribution modifies the bulk trend and promotes extensive solid solutions when the surface area is above a critical value dependent on the surface energy and the bulk enthalpy of mixing.},

  doi          = {10.1111/jace.13954},

  journal      = {Journal of the American Ceramic Society},

  number       = 2,

  volume       = 99,

  place        = {United States},

  year         = {Thu Oct 15 00:00:00 EDT 2015},

  month        = {Thu Oct 15 00:00:00 EDT 2015}

}

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Title: The Nanocrystalline SnO 2 –TiO 2 System‒Part II: Surface Energies and Thermodynamic Stability

Abstract

Citation Formats

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Calorimetric Study: Surface Energetics and the Magnetic Transition in Nanocrystalline CoO
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First-principles calculations on the surface electronic and reactive properties of M/SnO2 (M=Ge, Mn) (110)
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