Mapping the structural trends in zinc aluminosilicate glasses

Rita Mendes Da Silva; Anita Zeidler; Hesameddin Mohammadi; Lawrence V. D. Gammond; Esther Giron Lange; Randall E. Youngman; Bruce G. Aitken; Alex C Hannon; Chris J Benmore; Gavin Vaughan; Philip Salmon

doi:10.1063/5.0157790

Mapping the structural trends in zinc aluminosilicate glasses

Rita Mendes Da Silva, Anita Zeidler, Hesameddin Mohammadi, Lawrence V. D. Gammond, Esther Giron Lange, Randall E. Youngman, Bruce G. Aitken, Alex C Hannon, Chris J Benmore, Gavin Vaughan, Philip Salmon

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Abstract

The structure of zinc aluminosilicate glasses with the composition (ZnO)x(Al2O3)y(SiO2)1−x−y, where 0 ≤ x < 1, 0 ≤ y < 1 and x+y < 1, was investigated over a wide composition range by combining neutron and high-energy x-ray diffraction with 27Al magic angle spinning nuclear magnetic resonance spectroscopy. The results were interpreted using an analytical model for the composition-dependent structure in which the zinc ions do not act as network formers. Four-coordinated aluminum atoms were found to be in the majority for all the investigated glasses, with five-coordinated aluminum atoms as the main minority species. Mean Al-O bond distances of 1.764(5) and 1.855(5) °A were obtained for the four- and five-coordinated aluminum atoms, respectively. The coordination environment of zinc was not observed to be invariant. Instead, it is dependent on whether zinc plays a predominantly network-modifying or charge-compensating role, and therefore varies systematically with the glass composition. The Zn-O coordination number and bond distance were found to be 4.36(9) and 2.00(1) °A, respectively, for the network-modifying role versus 5.96(10) and 2.08(1) °A, respectively, for the charge-compensating role. The more open coordination environment of the charge-compensator is related to an enhanced probability of zinc finding bridging oxygen atoms as nearest-neighbors, reflecting a change in the connectivity of the glass network comprising four-coordinated silicon and aluminum atoms as the alumina content is increased.

Original language	English
Article number	064501
Number of pages	19
Journal	Journal of Chemical Physics
Volume	159
Issue number	6
Early online date	8 Aug 2023
DOIs	https://doi.org/10.1063/5.0157790
Publication status	Published - 14 Aug 2023

Funding

We thank Gabriel Cuello (Grenoble) for help with the D4c experiment. R.M.D.S. was supported by the Royal Society (Grant No. RGF/EA/180060). A.Z. was supported by a Royal Society-EPSRC Dorothy Hodgkin Research Fellowship. H.M. was supported by Corning, Inc. (Agreement No. CM00002159/SA/01). L.V.D.G. acknowledges the funding and support from the EPSRC Centre for Doctoral Training in Condensed Matter Physics (CDT-CMP), Grant No. EP/L015544/1, and the Science and Technology Facilities Council (STFC) and Diamond Light Source, Ltd. (Reference No. STU0173). E.G.L. was supported by the funding from the European Union’s Horizon 2020 Research and Innovation Program under Marie Skłodowska-Curie Grant Agreement No. 847439 and from Corning Inc. (Agreement No. CM00003814). P.S.S. and A.Z. are grateful to Corning Inc. for the award of Gordon S. Fulcher Distinguished Scholarships during which this work was conceived. We acknowledge use of the Inorganic Crystal Structure Database accessed via the Chemical Database Service funded by the Engineering and Physical Sciences Research Council (EPSRC) and hosted by the Royal Society of Chemistry. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

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10.1063/5.0157790Licence: CC BY

Data sets for "Mapping the structural trends in zinc aluminosilicate glasses"
Salmon, P. (Creator), Zeidler, A. (Creator) & Youngman, R. E. (Work Package Leader), University of Bath, 31 Jul 2023
DOI: 10.15125/BATH-01200
Dataset

Cite this

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title = "Mapping the structural trends in zinc aluminosilicate glasses",

abstract = "The structure of zinc aluminosilicate glasses with the composition (ZnO)x(Al2O3)y(SiO2)1−x−y, where 0 ≤ x < 1, 0 ≤ y < 1 and x+y < 1, was investigated over a wide composition range by combining neutron and high-energy x-ray diffraction with 27Al magic angle spinning nuclear magnetic resonance spectroscopy. The results were interpreted using an analytical model for the composition-dependent structure in which the zinc ions do not act as network formers. Four-coordinated aluminum atoms were found to be in the majority for all the investigated glasses, with five-coordinated aluminum atoms as the main minority species. Mean Al-O bond distances of 1.764(5) and 1.855(5) °A were obtained for the four- and five-coordinated aluminum atoms, respectively. The coordination environment of zinc was not observed to be invariant. Instead, it is dependent on whether zinc plays a predominantly network-modifying or charge-compensating role, and therefore varies systematically with the glass composition. The Zn-O coordination number and bond distance were found to be 4.36(9) and 2.00(1) °A, respectively, for the network-modifying role versus 5.96(10) and 2.08(1) °A, respectively, for the charge-compensating role. The more open coordination environment of the charge-compensator is related to an enhanced probability of zinc finding bridging oxygen atoms as nearest-neighbors, reflecting a change in the connectivity of the glass network comprising four-coordinated silicon and aluminum atoms as the alumina content is increased.",

author = "{Mendes Da Silva}, Rita and Anita Zeidler and Hesameddin Mohammadi and Gammond, {Lawrence V. D.} and {Giron Lange}, Esther and Youngman, {Randall E.} and Aitken, {Bruce G.} and Hannon, {Alex C} and Benmore, {Chris J} and Gavin Vaughan and Philip Salmon",

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AU - Mendes Da Silva, Rita

AU - Zeidler, Anita

AU - Mohammadi, Hesameddin

AU - Gammond, Lawrence V. D.

AU - Giron Lange, Esther

AU - Youngman, Randall E.

AU - Aitken, Bruce G.

AU - Hannon, Alex C

AU - Benmore, Chris J

AU - Vaughan, Gavin

AU - Salmon, Philip

PY - 2023/8/14

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N2 - The structure of zinc aluminosilicate glasses with the composition (ZnO)x(Al2O3)y(SiO2)1−x−y, where 0 ≤ x < 1, 0 ≤ y < 1 and x+y < 1, was investigated over a wide composition range by combining neutron and high-energy x-ray diffraction with 27Al magic angle spinning nuclear magnetic resonance spectroscopy. The results were interpreted using an analytical model for the composition-dependent structure in which the zinc ions do not act as network formers. Four-coordinated aluminum atoms were found to be in the majority for all the investigated glasses, with five-coordinated aluminum atoms as the main minority species. Mean Al-O bond distances of 1.764(5) and 1.855(5) °A were obtained for the four- and five-coordinated aluminum atoms, respectively. The coordination environment of zinc was not observed to be invariant. Instead, it is dependent on whether zinc plays a predominantly network-modifying or charge-compensating role, and therefore varies systematically with the glass composition. The Zn-O coordination number and bond distance were found to be 4.36(9) and 2.00(1) °A, respectively, for the network-modifying role versus 5.96(10) and 2.08(1) °A, respectively, for the charge-compensating role. The more open coordination environment of the charge-compensator is related to an enhanced probability of zinc finding bridging oxygen atoms as nearest-neighbors, reflecting a change in the connectivity of the glass network comprising four-coordinated silicon and aluminum atoms as the alumina content is increased.

AB - The structure of zinc aluminosilicate glasses with the composition (ZnO)x(Al2O3)y(SiO2)1−x−y, where 0 ≤ x < 1, 0 ≤ y < 1 and x+y < 1, was investigated over a wide composition range by combining neutron and high-energy x-ray diffraction with 27Al magic angle spinning nuclear magnetic resonance spectroscopy. The results were interpreted using an analytical model for the composition-dependent structure in which the zinc ions do not act as network formers. Four-coordinated aluminum atoms were found to be in the majority for all the investigated glasses, with five-coordinated aluminum atoms as the main minority species. Mean Al-O bond distances of 1.764(5) and 1.855(5) °A were obtained for the four- and five-coordinated aluminum atoms, respectively. The coordination environment of zinc was not observed to be invariant. Instead, it is dependent on whether zinc plays a predominantly network-modifying or charge-compensating role, and therefore varies systematically with the glass composition. The Zn-O coordination number and bond distance were found to be 4.36(9) and 2.00(1) °A, respectively, for the network-modifying role versus 5.96(10) and 2.08(1) °A, respectively, for the charge-compensating role. The more open coordination environment of the charge-compensator is related to an enhanced probability of zinc finding bridging oxygen atoms as nearest-neighbors, reflecting a change in the connectivity of the glass network comprising four-coordinated silicon and aluminum atoms as the alumina content is increased.

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VL - 159

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

IS - 6

M1 - 064501

ER -

Mapping the structural trends in zinc aluminosilicate glasses

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