Structure and Stability of SnO2 Nanocrystals and Surface-Bound

Wang, Hsiu-Wen; Wesolowski, David J; Proffen, Thomas E; Vlcek, Lukas; Wang, Wei; Allard, Jr, Lawrence Frederick; Kolesnikov, Alexander I; Feygenson, Mikhail; Paul, Dr. Rick L.

doi:10.1021/ja312030e

Title: Structure and Stability of SnO2 Nanocrystals and Surface-Bound

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Abstract

ABSTRACT: The structure of SnO2 nanoparticles (avg. 5 nm) with a few layers of water on the surface has been elucidated by atomic pair distribution function (PDF) methods using in situ neutron total scattering data and molecular dynamics (MD) simulations. Analysis of PDF, neutron prompt gamma, and thermogravimetric data, coupled with MD-generated surface D2O/OD configurations demonstrates that the minimum concentration of OD groups required to prevent rapid growth of nanoparticles during thermal dehydration corresponds to 0.7 monolayer coverage. Surface hydration layers not only stabilize the SnO2 nanoparticles but also induce particle-size-dependent structural modifications and are likely to promote interfacial reactions through hydrogen bonds between adjacent particles. Upon heating/dehydration under vacuum above 250 C, nanoparticles start to grow with low activation energies, rapid increase of nanoparticle size, and a reduction in the a lattice dimension. This study underscores the value of neutron diffraction and prompt-gamma analysis, coupled with molecular modeling, in elucidating the influence of surface hydration on the structure and metastable persistence of oxide nanomaterials.

Authors:

Wang, Hsiu-Wen ^[1]; Wesolowski, David J ^[1]; Proffen, Thomas E ^[1]; Vlcek, Lukas ^[1]; Wang, Wei ^[1]; Allard, Jr, Lawrence Frederick ^[1]; Kolesnikov, Alexander I ^[1]; Feygenson, Mikhail ^[1]; Paul, Dr. Rick L. ^[2]

ORNL
National Institute of Standards and Technology (NIST), Gaithersburg, MD

Publication Date:: Tue Jan 01 00:00:00 EST 2013

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1079854

DOE Contract Number:: DE-AC05-00OR22725

Resource Type:: Journal Article

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 135; Journal Issue: 18; Journal ID: ISSN 0002--7863

Country of Publication:: United States

Language:: English

Citation Formats


                    Wang, Hsiu-Wen, Wesolowski, David J, Proffen, Thomas E, Vlcek, Lukas, Wang, Wei, Allard, Jr, Lawrence Frederick, Kolesnikov, Alexander I, Feygenson, Mikhail, Anovitz, Lawrence, and Paul, Dr. Rick L. Structure and Stability of SnO2 Nanocrystals and Surface-Bound.  United States: N. p., 2013. 
        Web.  doi:10.1021/ja312030e.

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                    Wang, Hsiu-Wen, Wesolowski, David J, Proffen, Thomas E, Vlcek, Lukas, Wang, Wei, Allard, Jr, Lawrence Frederick, Kolesnikov, Alexander I, Feygenson, Mikhail, Anovitz, Lawrence, & Paul, Dr. Rick L. Structure and Stability of SnO2 Nanocrystals and Surface-Bound.  United States.  https://doi.org/10.1021/ja312030e

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                    Wang, Hsiu-Wen, Wesolowski, David J, Proffen, Thomas E, Vlcek, Lukas, Wang, Wei, Allard, Jr, Lawrence Frederick, Kolesnikov, Alexander I, Feygenson, Mikhail, Anovitz, Lawrence, and Paul, Dr. Rick L. 2013.  
        "Structure and Stability of SnO2 Nanocrystals and Surface-Bound".  United States.  https://doi.org/10.1021/ja312030e.

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@article{osti_1079854,

  title        = {Structure and Stability of SnO2 Nanocrystals and Surface-Bound},

  author       = {Wang, Hsiu-Wen and Wesolowski, David J and Proffen, Thomas E and Vlcek, Lukas and Wang, Wei and Allard, Jr, Lawrence Frederick and Kolesnikov, Alexander I and Feygenson, Mikhail and Anovitz, Lawrence and Paul, Dr. Rick L.},

  abstractNote = {ABSTRACT: The structure of SnO2 nanoparticles (avg. 5 nm) with a few layers of water on the surface has been elucidated by atomic pair distribution function (PDF) methods using in situ neutron total scattering data and molecular dynamics (MD) simulations. Analysis of PDF, neutron prompt gamma, and thermogravimetric data, coupled with MD-generated surface D2O/OD configurations demonstrates that the minimum concentration of OD groups required to prevent rapid growth of nanoparticles during thermal dehydration corresponds to 0.7 monolayer coverage. Surface hydration layers not only stabilize the SnO2 nanoparticles but also induce particle-size-dependent structural modifications and are likely to promote interfacial reactions through hydrogen bonds between adjacent particles. Upon heating/dehydration under vacuum above 250 C, nanoparticles start to grow with low activation energies, rapid increase of nanoparticle size, and a reduction in the a lattice dimension. This study underscores the value of neutron diffraction and prompt-gamma analysis, coupled with molecular modeling, in elucidating the influence of surface hydration on the structure and metastable persistence of oxide nanomaterials.},

  doi          = {10.1021/ja312030e},

  url          = {https://www.osti.gov/biblio/1079854},
  journal      = {Journal of the American Chemical Society},

  issn         = {0002--7863},

  number       = 18,

  volume       = 135,

  place        = {United States},

  year         = {Tue Jan 01 00:00:00 EST 2013},

  month        = {Tue Jan 01 00:00:00 EST 2013}

}

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