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Toward a Structural Model for the Aluminum Tellurite Glass System

Barney, Emma; Laorodphan, Nattapol; Mohd-Noor, Faizani; Holland, Diane; Kemp, Tom; Iuga, Dinu; Dupree, Ray

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Authors

Nattapol Laorodphan

Faizani Mohd-Noor

Diane Holland

Tom Kemp

Dinu Iuga

Ray Dupree



Abstract

Neutron diffraction, 27Al MAS NMR, and 27Al Double Quantum MAS NMR results are presented and analyzed to determine the local environments of the cations in a series of aluminum tellurite glasses. Total scattering results show that, within a maximum Te–O distance of 2.36 Å, tellurium exhibits a mix of [TeO3E] and [TeO4E] environments (E = electron lone-pair), with a linear reduction in the average tellurium–oxygen coordination number as Al2O3 is added to the glass. This is accompanied by a linear decrease in the average aluminum–oxygen coordination number as [AlO4] units form at the expense of [AlO6] units, while the fraction of [AlO5] units remains roughly constant. A consideration of the bonding requirements of the five structural units in the glass, [TeO3E], [TeO4E], [AlO4], [AlO5], and [AlO6], has allowed a direct quantitative relationship between tellurium–oxygen and aluminum–oxygen coordination numbers to be derived for the first time, and this has been successfully extended to the boron tellurite system. Double Quantum 27Al MAS NMR indicates that, in contrast to previous reports, the shortest Al...Al separations are significantly smaller (∼3.2 Å) than expected for a uniform distribution and there is a preference for [AlO6]–[AlO6] and [AlO4]–[AlO4] corner sharing polyhedra. These associations support a new structural model which successfully applies the principle of charge balance to describe the interaction of tellurium and aluminum and identifies and explains the clustering of [AlOn] polyhedra in the glass and their preferred associations. [AlO6] and [TeO4E] units dominate the network in TeO2-rich glasses and [AlO4]− units form to stabilize the [TeO3E]+ units as alumina is added to the glass.

Citation

Barney, E., Laorodphan, N., Mohd-Noor, F., Holland, D., Kemp, T., Iuga, D., & Dupree, R. (2020). Toward a Structural Model for the Aluminum Tellurite Glass System. Journal of Physical Chemistry C, 124(37), 20516–20529. https://doi.org/10.1021/acs.jpcc.0c04342

Journal Article Type Article
Acceptance Date Aug 19, 2020
Online Publication Date Aug 21, 2020
Publication Date Sep 17, 2020
Deposit Date Sep 24, 2020
Publicly Available Date Aug 22, 2021
Journal The Journal of Physical Chemistry C
Print ISSN 1932-7447
Electronic ISSN 1932-7455
Peer Reviewed Peer Reviewed
Volume 124
Issue 37
Pages 20516–20529
DOI https://doi.org/10.1021/acs.jpcc.0c04342
Keywords General Energy; Physical and Theoretical Chemistry; Electronic, Optical and Magnetic Materials; Surfaces, Coatings and Films
Public URL https://nottingham-repository.worktribe.com/output/4901745
Publisher URL https://pubs.acs.org/doi/pdf/10.1021/acs.jpcc.0c04342
Additional Information This document is the Accepted Manuscript version of a Published Work that appeared in final form in [JournalTitle], copyright © 2020 American Chemical Society after peer review and technical editing by t he publisher. To access the final edited and published work see https://pubs.acs.org/doi/pdf/10.1021/acs.jpcc.0c04342

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