Mapping the structural trends in zinc aluminosilicate glasses

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

doi:10.1063/5.0157790

DOE OSTI · 2404954

Mapping the structural trends in zinc aluminosilicate glasses

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

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Abstract

The structure of zinc aluminosilicate glasses with the composition (ZnO) x (Al 2 O 3 ) y (SiO 2 ) 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 27 Al 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) Å 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) Å, respectively, for the network-modifying role vs 5.96(10) and 2.08(1) Å, 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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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Amorphous materials Chemical bonding Chemical speciation Glass High-energy X rays Magic angle spinning nuclear magnetic resonance spectroscopy Materials and material systems Particle distribution functions Silicates X-ray diffraction

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Mendes Da Silva, Rita, Zeidler, Anita, Mohammadi, Hesameddin, Gammond, Lawrence D., Girón Lange, Esther, Youngman, Randall E., Aitken, Bruce G., Hannon, Alex C., Benmore, Chris J., Vaughan, Gavin M., Salmon, Philip S.. 2023-08-08. Mapping the structural trends in zinc aluminosilicate glasses. https://doi.org/10.1063/5.0157790

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