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

Deshkar, Ambar; Marcial, José; Southern, Scott A.; Kobera, Libor; Bryce, David L.; McCloy, John S.; Goel, Ashutosh

doi:10.1111/jace.14845

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

Journal Article · Sun Apr 09 00:00:00 EDT 2017 · Journal of the American Ceramic Society

DOI:https://doi.org/10.1111/jace.14845· OSTI ID:1401780

Deshkar, Ambar ^[1]; Marcial, José ^[2]; Southern, Scott A. ^[3]; Kobera, Libor ^[3]; Bryce, David L. ^[3]; ^[2]; ^[1]

Department of Materials Science and Engineering Rutgers‐The State University of New Jersey Piscataway New Jersey
School of Mechanical &, Materials Engineering and Materials Science &, Engineering Program Washington State University Pullman Washington
Department of Chemistry and Biomolecular Sciences University of Ottawa Ottawa ON Canada

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.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: EM0002904; EM0003207

OSTI ID:: 1401780

Journal Information:: Journal of the American Ceramic Society, Journal Name: Journal of the American Ceramic Society Journal Issue: 7 Vol. 100; ISSN 0002-7820

Publisher:: Wiley-BlackwellCopyright Statement

Country of Publication:: United States

Language:: English

References (62)

ZFiltering in MQMAS NMR Amoureux, Jean-Paul; Fernandez, Christian; Steuernagel, Stefan Journal of Magnetic Resonance, Series A, Vol. 123, Issue 1 https://doi.org/10.1006/jmra.1996.0221	journal	November 1996
A Reinvestigation of Low-Carnegieite by XRD, NMR, and TEM Thompson, John G.; Withers, Ray L.; Whittaker, Andrew K. Journal of Solid State Chemistry, Vol. 104, Issue 1 https://doi.org/10.1006/jssc.1993.1141	journal	May 1993
An XRD and Electron Diffraction Study of Cristobalite-Related Phases in the NaAlO2–NaAlSiO4System Thompson, John G.; Melnitchenko, Alexandra; Palethorpe, Stephen R. Journal of Solid State Chemistry, Vol. 131, Issue 1 https://doi.org/10.1006/jssc.1997.7295	journal	June 1997
Magic angle spinning NMR observation of sodium site exchange in nepheline at 500° C Stebbins, Jonathan F.; Farnan, Ian; Williams, Evan H. Physics and Chemistry of Minerals, Vol. 16, Issue 8 https://doi.org/10.1007/BF00209699	journal	November 1989
Thermodynamics of open networks: Ordering and entropy in NaAlSiO4 glass, liquid, and polymorphs Richet, Pascal; Robie, RichardA.; Rogez, Jacques Physics and Chemistry of Minerals, Vol. 17, Issue 5 https://doi.org/10.1007/BF00212206	journal	December 1990
23Na NMR chemical shifts and local Na coordination environments in silicate crystals, melts and glasses Xue, Xianyu; Stebbins, JonathanF. Physics and Chemistry of Minerals, Vol. 20, Issue 5 https://doi.org/10.1007/BF00215100	journal	October 1993
The tetrahedral framework in glasses and melts ? inferences from molecular orbital calculations and implications for structure, thermodynamics, and physical properties Navrotsky, A.; Geisinger, K. L.; McMillan, P. Physics and Chemistry of Minerals, Vol. 11, Issue 6 https://doi.org/10.1007/BF00307406	journal	January 1985
Defects and short-range order in nepheline group minerals: a silicon-29 nuclear magnetic resonance study Stebbins, J. F.; Murdoch, J. B.; Carmichael, I. S. E. Physics and Chemistry of Minerals, Vol. 13, Issue 6 https://doi.org/10.1007/BF00309182	journal	November 1986
Inversions in sub-potassic nephelines Henderson, C. M. B.; Roux, J. Contributions to Mineralogy and Petrology, Vol. 61, Issue 3 https://doi.org/10.1007/BF00376702	journal	January 1977
Glass transitions and thermodynamic properties of amorphous SiO2, NaAlSinO2n+2 and KAlSi3O8 Richet, Pascal; Bottinga, Yan Geochimica et Cosmochimica Acta, Vol. 48, Issue 3 https://doi.org/10.1016/0016-7037(84)90274-6	journal	March 1984
Polymerization of silicate and aluminate tetrahedra in glasses, melts, and aqueous solutions—V. The polymeric structure of silica in albite and anorthite composition glass and the devitrification of amorphous anorthite de Jong, B. H. W. S.; Schramm, Charles M.; Parziale, Victor E. Geochimica et Cosmochimica Acta, Vol. 48, Issue 12 https://doi.org/10.1016/0016-7037(84)90310-7	journal	December 1984
High-resolution 23Na, 27Al and 29Si NMR spectroscopy of framework Aluminosilicate glasses Oestrike, Richard; Yang, Wang-hong; Kirkpatrick, R. James Geochimica et Cosmochimica Acta, Vol. 51, Issue 8 https://doi.org/10.1016/0016-7037(87)90269-9	journal	August 1987
Kinetics of crystal nucleation in silicate glasses James, P. F. Journal of Non-Crystalline Solids, Vol. 73, Issue 1-3 https://doi.org/10.1016/0022-3093(85)90372-2	journal	August 1985
Preparation of nepheline glass-ceramics and their application as dental porcelain Moo-Chin, Wang; Nan-Chung, Wu; Min-Hsiung, Hon Materials Chemistry and Physics, Vol. 37, Issue 4 https://doi.org/10.1016/0254-0584(94)90177-5	journal	May 1994
Investigation of Al–O–Si bond angle in glass by 3Q-MAS NMR and molecular dynamics Angeli, F.; Delaye, J. -M; Charpentier, T. Chemical Physics Letters, Vol. 320, Issue 5-6 https://doi.org/10.1016/S0009-2614(00)00277-3	journal	April 2000
The distribution of sodium ions in aluminosilicate glasses: a high-field Na-23 MAS and 3Q MAS NMR study Lee, Sung Keun; Stebbins, Jonathan F. Geochimica et Cosmochimica Acta, Vol. 67, Issue 9 https://doi.org/10.1016/S0016-7037(03)00026-7	journal	May 2003
FTIR spectroscopy of framework aluminosilicate structures: carnegieite and pure sodium nepheline Markovic, Smilja; Dondur, Vera; Dimitrijevic, Radovan Journal of Molecular Structure, Vol. 654, Issue 1-3 https://doi.org/10.1016/S0022-2860(03)00249-7	journal	June 2003
Al–O–Al and Si–O–Si sites in framework aluminosilicate glasses with Si/Al=1: quantification of framework disorder Lee, Sung Keun; Stebbins, Jonathan F. Journal of Non-Crystalline Solids, Vol. 270, Issue 1-3 https://doi.org/10.1016/S0022-3093(00)00089-2	journal	May 2000
29Si MAS–NMR studies of Qn structural units in metasilicate glasses and their nucleating ability Schneider, J.; Mastelaro, V. R.; Panepucci, H. Journal of Non-Crystalline Solids, Vol. 273, Issue 1-3 https://doi.org/10.1016/S0022-3093(00)00139-3	journal	August 2000
Isothermal and adiabatic nucleation in glass Zanotto, Edgar Dutra Journal of Non-Crystalline Solids, Vol. 89, Issue 3 https://doi.org/10.1016/S0022-3093(87)80278-8	journal	March 1987
Heating of samples induced by fast magic-angle spinning Brus, Jiri Solid State Nuclear Magnetic Resonance, Vol. 16, Issue 3 https://doi.org/10.1016/S0926-2040(00)00061-8	journal	June 2000
Characterization of white Portland cement hydration and the C-S-H structure in the presence of sodium aluminate by 27Al and 29Si MAS NMR spectroscopy Andersen, Morten Daugaard; Jakobsen, Hans J.; Skibsted, Jørgen Cement and Concrete Research, Vol. 34, Issue 5 https://doi.org/10.1016/j.cemconres.2003.10.009	journal	May 2004
Ca and Na environments in Na2O–CaO–Al2O3–SiO2 glasses: influence of cation mixing and cation-network interactions Cormier, L.; Neuville, D. R. Chemical Geology, Vol. 213, Issue 1-3 https://doi.org/10.1016/j.chemgeo.2004.08.049	journal	December 2004
The effect of Na/Si on the structure of sodium silicate and aluminosilicate glasses quenched from melts at high pressure: A multi-nuclear (Al-27, Na-23, O-17) 1D and 2D solid-state NMR study Lee, Sung Keun; Cody, George D.; Fei, Yingwei Chemical Geology, Vol. 229, Issue 1-3 https://doi.org/10.1016/j.chemgeo.2006.01.018	journal	May 2006
Al coordination and speciation in calcium aluminosilicate glasses: Effects of composition determined by 27Al MQ-MAS NMR and Raman spectroscopy Neuville, Daniel R.; Cormier, Laurent; Massiot, Dominique Chemical Geology, Vol. 229, Issue 1-3 https://doi.org/10.1016/j.chemgeo.2006.01.019	journal	May 2006
The effect of network-modifying cations on the structure and disorder in peralkaline Ca–Na aluminosilicate glasses: O-17 3QMAS NMR study Lee, Sung Keun; Sung, Soyoung Chemical Geology, Vol. 256, Issue 3-4 https://doi.org/10.1016/j.chemgeo.2008.07.019	journal	November 2008
Probing silicon and aluminium chemical environments in silicate and aluminosilicate glasses by solid state NMR spectroscopy and accurate first-principles calculations Gambuzzi, Elisa; Pedone, Alfonso; Menziani, Maria Cristina Geochimica et Cosmochimica Acta, Vol. 125 https://doi.org/10.1016/j.gca.2013.10.025	journal	January 2014
Characterization of the structure of calcium alumino-silicate and calcium fluoro-alumino-silicate glasses by magic angle spinning nuclear magnetic resonance (MAS-NMR) Stamboulis, Artemis; Hill, Robert G.; Law, Robert V. Journal of Non-Crystalline Solids, Vol. 333, Issue 1 https://doi.org/10.1016/j.jnoncrysol.2003.09.049	journal	January 2004
Correlation between maximum crystal growth rate and glass transition temperature of silicate glasses Fokin, Vladimir M.; Nascimento, Marcio L. F.; Zanotto, Edgar D. Journal of Non-Crystalline Solids, Vol. 351, Issue 10-11 https://doi.org/10.1016/j.jnoncrysol.2005.02.005	journal	April 2005
Effects of cation field strength on the structure of aluminoborosilicate glasses: High-resolution 11B, 27Al and 23Na MAS NMR Wu, Jingshi; Stebbins, Jonathan F. Journal of Non-Crystalline Solids, Vol. 355, Issue 9 https://doi.org/10.1016/j.jnoncrysol.2009.01.025	journal	April 2009
Nepheline crystallization in boron-rich alumino-silicate glasses as investigated by multi-nuclear NMR, Raman, & Mössbauer spectroscopies McCloy, John; Washton, Nancy; Gassman, Paul Journal of Non-Crystalline Solids, Vol. 409 https://doi.org/10.1016/j.jnoncrysol.2014.11.013	journal	February 2015
Structural characterization of pure Na-nephelines synthesized by zeolite conversion route Dimitrijevic, Radovan; Dondur, Vera; Vulic, Predrag Journal of Physics and Chemistry of Solids, Vol. 65, Issue 10 https://doi.org/10.1016/j.jpcs.2004.03.005	journal	October 2004
Preparation of nepheline glass–ceramics for dental applications Hamzawy, Esmat M. A.; El-Meliegy, Emad A. M. Materials Chemistry and Physics, Vol. 112, Issue 2 https://doi.org/10.1016/j.matchemphys.2008.05.079	journal	December 2008
Calcium environment in silicate and aluminosilicate glasses probed by 43Ca MQMAS NMR experiments and MD-GIPAW calculations Gambuzzi, Elisa; Pedone, Alfonso; Menziani, Maria Cristina Solid State Nuclear Magnetic Resonance, Vol. 68-69 https://doi.org/10.1016/j.ssnmr.2015.04.003	journal	June 2015
Effect of Alkali Cations on Aluminum Incorporation in Geopolymeric Gels Duxson, P.; Lukey, G. C.; Separovic, F. Industrial & Engineering Chemistry Research, Vol. 44, Issue 4 https://doi.org/10.1021/ie0494216	journal	February 2005
High-resolution aluminum-27 NMR of aluminosilicates Lippmaa, E.; Samoson, A.; Magi, M. Journal of the American Chemical Society, Vol. 108, Issue 8 https://doi.org/10.1021/ja00268a002	journal	April 1986
High-Resolution Multinuclear NMR Structural Study of Binary Aluminosilicate and Other Related Glasses Sen, S.; Youngman, R. E. The Journal of Physical Chemistry B, Vol. 108, Issue 23 https://doi.org/10.1021/jp031348u	journal	June 2004
Local Order of Amorphous Zeolite Precursors from ²⁹ Si{ ¹ H} CPMAS and ²⁷ Al and ²³ Na MQMAS NMR and Evidence for the Nature of Medium-Range Order from Neutron Diffraction Yang, Huaixin; Walton, Richard I.; Antonijevic, Sasa The Journal of Physical Chemistry B, Vol. 108, Issue 24 https://doi.org/10.1021/jp037887g	journal	June 2004
Site Populations and Short Range Order in Aluminosilicates Investigated by ²⁷ Al Solid-State NMR Larsen, Flemming H.; Farnan, Ian The Journal of Physical Chemistry B, Vol. 108, Issue 28 https://doi.org/10.1021/jp049603d	journal	July 2004
Unambiguous Description of the Oxygen Environment in Multicomponent Aluminosilicate Glasses from ¹⁷ O Solid State NMR Computational Spectroscopy Pedone, Alfonso; Gambuzzi, Elisa; Menziani, Maria Cristina The Journal of Physical Chemistry C, Vol. 116, Issue 27 https://doi.org/10.1021/jp304802y	journal	June 2012
The Structure of Aluminosilicate Glasses: High-Resolution ¹⁷ O and ²⁷ Al MAS and 3QMAS NMR Study Lee, Sung Keun; Stebbins, Jonathan F. The Journal of Physical Chemistry B, Vol. 104, Issue 17 https://doi.org/10.1021/jp994273w	journal	May 2000
NMR evidence for excess non-bridging oxygen in an aluminosilicate glass Stebbins, Jonathan F.; Xu, Zhi Nature, Vol. 390, Issue 6655 https://doi.org/10.1038/36312	journal	November 1997
Scaling and labeling the high-resolution isotropic axis of two-dimensional multiple-quantum magic-angle-spinning spectra of half-integer quadrupole spins Man, Pascal P. Physical Review B, Vol. 58, Issue 5 https://doi.org/10.1103/PhysRevB.58.2764	journal	August 1998
Crystal data for the low-temperature form of carnegieite NaAlSiO ₄ Klingenberg, R.; Felsche, J.; Miehe, G. Journal of Applied Crystallography, Vol. 14, Issue 1 https://doi.org/10.1107/S0021889881008728	journal	February 1981
Cristobalite-Related Phases in the NaAlO2–NaAlSiO4 System. I. Two Tetragonal and Two Orthorhombic Structures Thompson, J. G.; Withers, R. L.; Melnitchenko, A. Acta Crystallographica Section B Structural Science, Vol. 54, Issue 5 https://doi.org/10.1107/S0108768197019927	journal	October 1998
Cristobalite-Related Phases in the NaAlO2–NaAlSiO4 System. II. A Commensurately Modulated Cubic Structure Withers, R. L.; Thompson, J. G.; Melnitchenko, A. Acta Crystallographica Section B Structural Science, Vol. 54, Issue 5 https://doi.org/10.1107/S0108768197019939	journal	October 1998
Crystallization and Chemical Strengthening of Nepheline Glass-Ceramics Duke, D. A.; MacDowell, J. F.; Karstetter, B. R. Journal of the American Ceramic Society, Vol. 50, Issue 2 https://doi.org/10.1111/j.1151-2916.1967.tb15041.x	journal	February 1967
Formation of Nepheline Glass-Ceramics Using Nb2O5 as a Nucleation Catalyst Kivlighn, H. D.; Russak, M. A. Journal of the American Ceramic Society, Vol. 57, Issue 9 https://doi.org/10.1111/j.1151-2916.1974.tb11417.x	journal	September 1974
Nepheline and Carnegieite Ceramics from A-Type Zeolites by Microwave Heating Ohgushi, Tatsuo; Ishimaru, Kazushi; Komarneni, Sridhar Journal of the American Ceramic Society, Vol. 84, Issue 2 https://doi.org/10.1111/j.1151-2916.2001.tb00657.x	journal	February 2001
Elucidating the Effect of Iron Speciation (Fe ²⁺ /Fe ³⁺ ) on Crystallization Kinetics of Sodium Aluminosilicate Glasses Shaharyar, Yaqoot; Cheng, Justin Y.; Han, Edmund Journal of the American Ceramic Society, Vol. 99, Issue 7 https://doi.org/10.1111/jace.14239	journal	April 2016
Nepheline solid solutions Donnay, Gabrielle; Schairer, J. F.; Donnay, J. D. H. Mineralogical Magazine and Journal of the Mineralogical Society, Vol. 32, Issue 245 https://doi.org/10.1180/minmag.1959.32.245.02	journal	June 1959
Structural Characterisation of Kaolinite:NaCl Intercalate and its Derivatives Thompson, John G. Clays and Clay Minerals, Vol. 40, Issue 4 https://doi.org/10.1346/CCMN.1992.0400401	journal	January 1992
Nepheline Precipitation in High-Level Waste Glasses : Compositional Effects and Impact on the Waste Form Acceptability Li, H.; Vienna, J. D.; Hrma, P. MRS Proceedings, Vol. 465 https://doi.org/10.1557/PROC-465-261	journal	January 1996
The Crystal Chemistry of Nepheline Tait, K. T.; Sokolova, E.; Hawthorne, F. C. The Canadian Mineralogist, Vol. 41, Issue 1 https://doi.org/10.2113/gscanmin.41.1.61	journal	February 2003
Si-Al ordering in leucite group minerals and ion-exchanged analogues; an MAS NMR study Kohn, Simon C.; Henderson, C. Michael; Dupree, Raymond American Mineralogist, Vol. 82, Issue 11-12 https://doi.org/10.2138/am-1997-11-1211	journal	December 1997
The degree of aluminum avoidance in aluminosilicate glasses Lee, Sung Keun; Stebbins, Jonathan F. American Mineralogist, Vol. 84, Issue 5-6 https://doi.org/10.2138/am-1999-5-630	journal	June 1999
Fivefold-coordinated aluminum in tectosilicate glasses observed by triple quantum MAS NMR Toplis, Michael J.; Kohn, Simon C.; Smith, Mark E. American Mineralogist, Vol. 85, Issue 10 https://doi.org/10.2138/am-2000-1031	journal	October 2000
Temperature-induced amorphization of Na-zeolite A: A view from multi-nuclear high-resolution solid-state NMR Kim, H. N.; Lee, S. K. American Mineralogist, Vol. 99, Issue 10 https://doi.org/10.2138/am-2014-4928	journal	October 2014
Nepheline structural and chemical dependence on melt composition Marcial, José; Crum, Jarrod; Neill, Owen American Mineralogist, Vol. 101, Issue 2 https://doi.org/10.2138/am-2016-5370	journal	February 2016
Reaction Processes to form Nephelinecarnegieite Minerals from Various Starting Materials Kubo, Yasushi; Yamaguchi, Goro; Kasahara, Komei Mineralogical Journal, Vol. 5, Issue 3 https://doi.org/10.2465/minerj1953.5.213	journal	January 1967
The nepheline-kalsilite system; Part I, X-ray data for the crystalline phases Smith, J. V.; Tuttle, O. F. American Journal of Science, Vol. 255, Issue 4 https://doi.org/10.2475/ajs.255.4.282	journal	April 1957
The binary system; na 2 Al 2 Si 2 O 8 (nephelite, carnegieite); CaAl 2 Si 2 O 8 (anorthite) Bowen, N. L. American Journal of Science, Vol. s4-33, Issue 198 https://doi.org/10.2475/ajs.s4-33.198.551	journal	June 1912

Similar Records

Submixture model to predict nepheline precipitation in waste glasses

Journal Article · Tue May 10 20:00:00 EDT 2016 · International Journal of Applied Glass Science · OSTI ID:1400970

Structural dependence of crystallization in glasses along the nepheline (NaAlSiO ₄ ) ‐ eucryptite (LiAlSiO ₄ ) join

Journal Article · Wed Jan 31 19:00:00 EST 2018 · Journal of the American Ceramic Society · OSTI ID:1419091

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

Citation Formats

References (62)

Similar Records

Related Subjects

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