Nitrogen-rich La-Si-Al-O-N oxynitride glass structures probed by solid state NMR

Ekaterina Leonova; Abbas S. Hakeem; Kjell Jansson; Baltzar Stevensson; Zhijian Shen; Jekabs Grins; Saeid Esmaeilzadeh; Mattias Edén

doi:10.1016/j.jnoncrysol.2007.07.027

Nitrogen-rich La-Si-Al-O-N oxynitride glass structures probed by solid state NMR

Ekaterina Leonova, Abbas S. Hakeem, Kjell Jansson, Baltzar Stevensson, Zhijian Shen, Jekabs Grins, Saeid Esmaeilzadeh, Mattias Edén^*

^*Corresponding author for this work

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

65 Scopus citations

Abstract

We investigate the local structures of oxynitride La-Si-(Al)-O-N glasses by ²⁹Si and ²⁷Al magic-angle spinning (MAS) solid state Nuclear Magnetic Resonance (NMR). The glasses studied span an unprecedented range of compositions, up to >50 at.% lanthanum and nitrogen out of the cations and anions, respectively, and achievable through a recently introduced glass preparation route. Transmission as well as scanning electron microscopy verified homogeneous samples over length-scales down to 20 nm. As the nitrogen content of the glasses increased, ²⁹Si NMR evidenced a progressive formation of Si-N bonds, with SiO₂N₂ tetrahedra dominating in the nitrogen-rich glass networks. In the oxygen-rich end of the series, aluminum is predominantly present in tetrahedral coordination as AlO₄, whereas the glasses with highest nitrogen contents have a major fraction of AlO₃N structural units. Trends in isotropic ²⁹Si and ²⁷Al chemical shifts and ²⁷Al quadrupolar couplings are compared with results of La-Si-Al-O glasses and are discussed in relation to the glass compositions and their proposed structures.

Original language	English
Pages (from-to)	49-60
Number of pages	12
Journal	Journal of Non-Crystalline Solids
Volume	354
Issue number	1
DOIs	https://doi.org/10.1016/j.jnoncrysol.2007.07.027
State	Published - 1 Jan 2008
Externally published	Yes

Bibliographical note

Funding Information:
This work was supported by the Swedish Research Council (VR) and the foundations of Carl Trygger, Magn. Bergvall and Lars Hierta’s minne. S. Esmaeilzadeh possesses a research fellowship from the Royal Academy of Sciences financed by the Knut and Alice Wallenberg Foundation. We thank A. Rosenflanz at the 3M central research laboratory for providing the aluminate glass, Z. Weng for instrumental NMR support and L. Göthe for XRD powder diffraction measurements.

Keywords

Al NMR
Cation distributions
Cross-polarization
Glass structure
La-Si-Al-O glass
Oxynitride glass
Rare-earth Silicate
Si NMR
TEM

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Ceramics and Composites
Condensed Matter Physics
Materials Chemistry

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10.1016/j.jnoncrysol.2007.07.027

Cite this

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title = "Nitrogen-rich La-Si-Al-O-N oxynitride glass structures probed by solid state NMR",

abstract = "We investigate the local structures of oxynitride La-Si-(Al)-O-N glasses by 29Si and 27Al magic-angle spinning (MAS) solid state Nuclear Magnetic Resonance (NMR). The glasses studied span an unprecedented range of compositions, up to >50 at.% lanthanum and nitrogen out of the cations and anions, respectively, and achievable through a recently introduced glass preparation route. Transmission as well as scanning electron microscopy verified homogeneous samples over length-scales down to 20 nm. As the nitrogen content of the glasses increased, 29Si NMR evidenced a progressive formation of Si-N bonds, with SiO2N2 tetrahedra dominating in the nitrogen-rich glass networks. In the oxygen-rich end of the series, aluminum is predominantly present in tetrahedral coordination as AlO4, whereas the glasses with highest nitrogen contents have a major fraction of AlO3N structural units. Trends in isotropic 29Si and 27Al chemical shifts and 27Al quadrupolar couplings are compared with results of La-Si-Al-O glasses and are discussed in relation to the glass compositions and their proposed structures.",

keywords = "Al NMR, Cation distributions, Cross-polarization, Glass structure, La-Si-Al-O glass, Oxynitride glass, Rare-earth Silicate, Si NMR, TEM",

author = "Ekaterina Leonova and Hakeem, {Abbas S.} and Kjell Jansson and Baltzar Stevensson and Zhijian Shen and Jekabs Grins and Saeid Esmaeilzadeh and Mattias Ed{\'e}n",

note = "Funding Information: This work was supported by the Swedish Research Council (VR) and the foundations of Carl Trygger, Magn. Bergvall and Lars Hierta{\textquoteright}s minne. S. Esmaeilzadeh possesses a research fellowship from the Royal Academy of Sciences financed by the Knut and Alice Wallenberg Foundation. We thank A. Rosenflanz at the 3M central research laboratory for providing the aluminate glass, Z. Weng for instrumental NMR support and L. G{\"o}the for XRD powder diffraction measurements.",

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doi = "10.1016/j.jnoncrysol.2007.07.027",

language = "English",

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T1 - Nitrogen-rich La-Si-Al-O-N oxynitride glass structures probed by solid state NMR

AU - Leonova, Ekaterina

AU - Hakeem, Abbas S.

AU - Jansson, Kjell

AU - Stevensson, Baltzar

AU - Shen, Zhijian

AU - Grins, Jekabs

AU - Esmaeilzadeh, Saeid

AU - Edén, Mattias

N1 - Funding Information: This work was supported by the Swedish Research Council (VR) and the foundations of Carl Trygger, Magn. Bergvall and Lars Hierta’s minne. S. Esmaeilzadeh possesses a research fellowship from the Royal Academy of Sciences financed by the Knut and Alice Wallenberg Foundation. We thank A. Rosenflanz at the 3M central research laboratory for providing the aluminate glass, Z. Weng for instrumental NMR support and L. Göthe for XRD powder diffraction measurements.

PY - 2008/1/1

Y1 - 2008/1/1

N2 - We investigate the local structures of oxynitride La-Si-(Al)-O-N glasses by 29Si and 27Al magic-angle spinning (MAS) solid state Nuclear Magnetic Resonance (NMR). The glasses studied span an unprecedented range of compositions, up to >50 at.% lanthanum and nitrogen out of the cations and anions, respectively, and achievable through a recently introduced glass preparation route. Transmission as well as scanning electron microscopy verified homogeneous samples over length-scales down to 20 nm. As the nitrogen content of the glasses increased, 29Si NMR evidenced a progressive formation of Si-N bonds, with SiO2N2 tetrahedra dominating in the nitrogen-rich glass networks. In the oxygen-rich end of the series, aluminum is predominantly present in tetrahedral coordination as AlO4, whereas the glasses with highest nitrogen contents have a major fraction of AlO3N structural units. Trends in isotropic 29Si and 27Al chemical shifts and 27Al quadrupolar couplings are compared with results of La-Si-Al-O glasses and are discussed in relation to the glass compositions and their proposed structures.

AB - We investigate the local structures of oxynitride La-Si-(Al)-O-N glasses by 29Si and 27Al magic-angle spinning (MAS) solid state Nuclear Magnetic Resonance (NMR). The glasses studied span an unprecedented range of compositions, up to >50 at.% lanthanum and nitrogen out of the cations and anions, respectively, and achievable through a recently introduced glass preparation route. Transmission as well as scanning electron microscopy verified homogeneous samples over length-scales down to 20 nm. As the nitrogen content of the glasses increased, 29Si NMR evidenced a progressive formation of Si-N bonds, with SiO2N2 tetrahedra dominating in the nitrogen-rich glass networks. In the oxygen-rich end of the series, aluminum is predominantly present in tetrahedral coordination as AlO4, whereas the glasses with highest nitrogen contents have a major fraction of AlO3N structural units. Trends in isotropic 29Si and 27Al chemical shifts and 27Al quadrupolar couplings are compared with results of La-Si-Al-O glasses and are discussed in relation to the glass compositions and their proposed structures.

KW - Al NMR

KW - Cation distributions

KW - Cross-polarization

KW - Glass structure

KW - La-Si-Al-O glass

KW - Oxynitride glass

KW - Rare-earth Silicate

KW - Si NMR

KW - TEM

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DO - 10.1016/j.jnoncrysol.2007.07.027

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AN - SCOPUS:36549048012

SN - 0022-3093

VL - 354

SP - 49

EP - 60

JO - Journal of Non-Crystalline Solids

JF - Journal of Non-Crystalline Solids

IS - 1

ER -

Nitrogen-rich La-Si-Al-O-N oxynitride glass structures probed by solid state NMR

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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