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Title: Understanding the structural origin of crystalline phase transformations in nepheline (NaAlSiO 4 )‐based glass‐ceramics

Abstract

Abstract Nepheline (Na 6 K 2 Al 8 Si 8 O 32 ) is a rock‐forming tectosilicate mineral which is by far the most abundant of the feldspathoids. The crystallization in nepheline‐based glass‐ceramics proceeds through several polymorphic transformations — mainly orthorhombic, hexagonal, cubic — depending on their thermochemistry. However, the fundamental science governing these transformations is poorly understood. In this article, an attempt has been made to elucidate the structural drivers controlling these polymorphic transformations in nepheline‐based glass‐ceramics. Accordingly, two different sets of glasses (meta‐aluminous and per‐alkaline) have been designed in the system Na 2 O–CaO–Al 2 O 3 –SiO 2 in the crystallization field of nepheline and synthesized by the melt‐quench technique. The detailed structural analysis of glasses has been performed by 29 Si, 27 Al, and 23 Na magic‐angle spinning — nuclear magnetic resonance ( MAS NMR ), and multiple‐quantum MAS NMR spectroscopy, while the crystalline phase transformations in these glasses have been studied under isothermal and non‐isothermal conditions using differential scanning calorimetry ( DSC ), X‐ray diffraction ( XRD ), and MQMAS NMR . Results indicate that the sequence of polymorphic phase transformations in these glass‐ceramics is dictated by the compositional chemistry of the parent glasses andmore » the local environments of different species in the glass structure; for example, the sodium environment in glasses became highly ordered with decreasing Na 2 O/CaO ratio, thus favoring the formation of hexagonal nepheline, while the cubic polymorph was the stable phase in SiO 2 –poor glass‐ceramics with (Na 2 O+CaO)/Al 2 O 3 > 1. The structural origins of these crystalline phase transformations have been discussed in the paper.« less

Authors:
 [1];  [2];  [3];  [3];  [3]; ORCiD logo [2]; ORCiD logo [1]
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  1. Department of Materials Science and Engineering Rutgers‐The State University of New Jersey Piscataway New Jersey
  2. School of Mechanical &, Materials Engineering and Materials Science &, Engineering Program Washington State University Pullman Washington
  3. Department of Chemistry and Biomolecular Sciences University of Ottawa Ottawa ON Canada
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1401780
Grant/Contract Number:  
DE‐EM0003207
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: 100 Journal Issue: 7; Journal ID: ISSN 0002-7820
Publisher:
Wiley-Blackwell
Country of Publication:
United States
Language:
English

Citation Formats

Deshkar, Ambar, Marcial, José, Southern, Scott A., Kobera, Libor, Bryce, David L., McCloy, John S., and Goel, Ashutosh. Understanding the structural origin of crystalline phase transformations in nepheline (NaAlSiO 4 )‐based glass‐ceramics. United States: N. p., 2017. Web. doi:10.1111/jace.14845.
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Deshkar, Ambar, Marcial, José, Southern, Scott A., Kobera, Libor, Bryce, David L., McCloy, John S., & Goel, Ashutosh. Understanding the structural origin of crystalline phase transformations in nepheline (NaAlSiO 4 )‐based glass‐ceramics. United States. https://doi.org/10.1111/jace.14845
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Deshkar, Ambar, Marcial, José, Southern, Scott A., Kobera, Libor, Bryce, David L., McCloy, John S., and Goel, Ashutosh. Sun . "Understanding the structural origin of crystalline phase transformations in nepheline (NaAlSiO 4 )‐based glass‐ceramics". United States. https://doi.org/10.1111/jace.14845.
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@article{osti_1401780,
title = {Understanding the structural origin of crystalline phase transformations in nepheline (NaAlSiO 4 )‐based glass‐ceramics},
author = {Deshkar, Ambar and Marcial, José and Southern, Scott A. and Kobera, Libor and Bryce, David L. and McCloy, John S. and Goel, Ashutosh},
abstractNote = {Abstract Nepheline (Na 6 K 2 Al 8 Si 8 O 32 ) is a rock‐forming tectosilicate mineral which is by far the most abundant of the feldspathoids. The crystallization in nepheline‐based glass‐ceramics proceeds through several polymorphic transformations — mainly orthorhombic, hexagonal, cubic — depending on their thermochemistry. However, the fundamental science governing these transformations is poorly understood. In this article, an attempt has been made to elucidate the structural drivers controlling these polymorphic transformations in nepheline‐based glass‐ceramics. Accordingly, two different sets of glasses (meta‐aluminous and per‐alkaline) have been designed in the system Na 2 O–CaO–Al 2 O 3 –SiO 2 in the crystallization field of nepheline and synthesized by the melt‐quench technique. The detailed structural analysis of glasses has been performed by 29 Si, 27 Al, and 23 Na magic‐angle spinning — nuclear magnetic resonance ( MAS NMR ), and multiple‐quantum MAS NMR spectroscopy, while the crystalline phase transformations in these glasses have been studied under isothermal and non‐isothermal conditions using differential scanning calorimetry ( DSC ), X‐ray diffraction ( XRD ), and MQMAS NMR . Results indicate that the sequence of polymorphic phase transformations in these glass‐ceramics is dictated by the compositional chemistry of the parent glasses and the local environments of different species in the glass structure; for example, the sodium environment in glasses became highly ordered with decreasing Na 2 O/CaO ratio, thus favoring the formation of hexagonal nepheline, while the cubic polymorph was the stable phase in SiO 2 –poor glass‐ceramics with (Na 2 O+CaO)/Al 2 O 3 > 1. The structural origins of these crystalline phase transformations have been discussed in the paper.},
doi = {10.1111/jace.14845},
journal = {Journal of the American Ceramic Society},
number = 7,
volume = 100,
place = {United States},
year = {Sun Apr 09 00:00:00 EDT 2017},
month = {Sun Apr 09 00:00:00 EDT 2017}
}
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