Predicting Q-Speciation in Binary Phosphate Glasses using Statistical Mechanics

Mikkel Sandfeld Bødker, John C. Mauro, Sushmit Goyal, Randall E. Youngman, Morten Mattrup Smedskjær

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

4 Citationer (Scopus)

Resumé

Predicting the compositional evolution of the atomic-scale structure of oxide glasses is important for developing quantitative composition-property models. In binary phosphate glasses, the addition of network modifiers generally leads to depolymerization of the networks as described by the Q-speciation, where Q n denotes PO 4 tetrahedra with n number (between 0 and 3) of bridging P-O-P linkages per tetrahedron. Upon the initial creation of nonbridging oxygens and thus partly depolymerized Q species, a variety of network former-modifier interactions exist. Here, on the basis of 31P magic angle spinning nuclear magnetic resonance spectroscopy data from the literature, we present a statistical description of the compositional evolution of Q-speciation in these glasses by accounting for the relative enthalpic and entropic contributions to the bonding preferences. We show that the entire glass structure evolution can be predicted based on experimental structural information for only a few glass compositions in each series. The model also captures the differences in bonding preferences in glasses with different field strengths (charge-to-size ratio) of the modifier cations.

OriginalsprogEngelsk
TidsskriftJournal of Physical Chemistry Part B: Condensed Matter, Materials, Surfaces, Interfaces & Biophysical
Vol/bind122
Udgave nummer30
Sider (fra-til)7609-7615
Antal sider7
ISSN1520-6106
DOI
StatusUdgivet - 2 aug. 2018

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Statistical mechanics
statistical mechanics
phosphates
Phosphates
Glass
glass
tetrahedrons
depolymerization
Depolymerization
Magic angle spinning
magnetic resonance spectroscopy
Chemical analysis
linkages
Oxides
metal spinning
Nuclear magnetic resonance spectroscopy
Cations
field strength
Positive ions
Oxygen

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title = "Predicting Q-Speciation in Binary Phosphate Glasses using Statistical Mechanics",
abstract = "Predicting the compositional evolution of the atomic-scale structure of oxide glasses is important for developing quantitative composition-property models. In binary phosphate glasses, the addition of network modifiers generally leads to depolymerization of the networks as described by the Q-speciation, where Q n denotes PO 4 tetrahedra with n number (between 0 and 3) of bridging P-O-P linkages per tetrahedron. Upon the initial creation of nonbridging oxygens and thus partly depolymerized Q species, a variety of network former-modifier interactions exist. Here, on the basis of 31P magic angle spinning nuclear magnetic resonance spectroscopy data from the literature, we present a statistical description of the compositional evolution of Q-speciation in these glasses by accounting for the relative enthalpic and entropic contributions to the bonding preferences. We show that the entire glass structure evolution can be predicted based on experimental structural information for only a few glass compositions in each series. The model also captures the differences in bonding preferences in glasses with different field strengths (charge-to-size ratio) of the modifier cations.",
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Predicting Q-Speciation in Binary Phosphate Glasses using Statistical Mechanics. / Bødker, Mikkel Sandfeld; Mauro, John C.; Goyal, Sushmit; Youngman, Randall E.; Smedskjær, Morten Mattrup.

I: Journal of Physical Chemistry Part B: Condensed Matter, Materials, Surfaces, Interfaces & Biophysical, Bind 122, Nr. 30, 02.08.2018, s. 7609-7615.

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

TY - JOUR

T1 - Predicting Q-Speciation in Binary Phosphate Glasses using Statistical Mechanics

AU - Bødker, Mikkel Sandfeld

AU - Mauro, John C.

AU - Goyal, Sushmit

AU - Youngman, Randall E.

AU - Smedskjær, Morten Mattrup

PY - 2018/8/2

Y1 - 2018/8/2

N2 - Predicting the compositional evolution of the atomic-scale structure of oxide glasses is important for developing quantitative composition-property models. In binary phosphate glasses, the addition of network modifiers generally leads to depolymerization of the networks as described by the Q-speciation, where Q n denotes PO 4 tetrahedra with n number (between 0 and 3) of bridging P-O-P linkages per tetrahedron. Upon the initial creation of nonbridging oxygens and thus partly depolymerized Q species, a variety of network former-modifier interactions exist. Here, on the basis of 31P magic angle spinning nuclear magnetic resonance spectroscopy data from the literature, we present a statistical description of the compositional evolution of Q-speciation in these glasses by accounting for the relative enthalpic and entropic contributions to the bonding preferences. We show that the entire glass structure evolution can be predicted based on experimental structural information for only a few glass compositions in each series. The model also captures the differences in bonding preferences in glasses with different field strengths (charge-to-size ratio) of the modifier cations.

AB - Predicting the compositional evolution of the atomic-scale structure of oxide glasses is important for developing quantitative composition-property models. In binary phosphate glasses, the addition of network modifiers generally leads to depolymerization of the networks as described by the Q-speciation, where Q n denotes PO 4 tetrahedra with n number (between 0 and 3) of bridging P-O-P linkages per tetrahedron. Upon the initial creation of nonbridging oxygens and thus partly depolymerized Q species, a variety of network former-modifier interactions exist. Here, on the basis of 31P magic angle spinning nuclear magnetic resonance spectroscopy data from the literature, we present a statistical description of the compositional evolution of Q-speciation in these glasses by accounting for the relative enthalpic and entropic contributions to the bonding preferences. We show that the entire glass structure evolution can be predicted based on experimental structural information for only a few glass compositions in each series. The model also captures the differences in bonding preferences in glasses with different field strengths (charge-to-size ratio) of the modifier cations.

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DO - 10.1021/acs.jpcb.8b04604

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VL - 122

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EP - 7615

JO - Journal of Physical Chemistry Part B: Condensed Matter, Materials, Surfaces, Interfaces & Biophysical

JF - Journal of Physical Chemistry Part B: Condensed Matter, Materials, Surfaces, Interfaces & Biophysical

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