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Structure and Crystallization Behavi...

Zhang, Yingcheng,

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Structure and Crystallization Behavior of Sodium- and Alumina-Rich Model High-Level Nuclear Waste Glasses /

Record Type:	Electronic resources : Monograph/item
Title/Author:	Structure and Crystallization Behavior of Sodium- and Alumina-Rich Model High-Level Nuclear Waste Glasses // Yingcheng Zhang.
Author:	Zhang, Yingcheng,
Description:	1 electronic resource (323 pages)
Notes:	Source: Dissertations Abstracts International, Volume: 86-10, Section: B.
Contained By:	Dissertations Abstracts International86-10B.
Subject:	Engineering. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31767651
ISBN:	9798310167377

Structure and Crystallization Behavior of Sodium- and Alumina-Rich Model High-Level Nuclear Waste Glasses /
Zhang, Yingcheng,

Structure and Crystallization Behavior of Sodium- and Alumina-Rich Model High-Level Nuclear Waste Glasses /Yingcheng Zhang. - 1 electronic resource (323 pages)

Source: Dissertations Abstracts International, Volume: 86-10, Section: B.

The United States Department of Energy (DOE) is planning to vitrify around 56 million gallons of radioactive waste stored underground at Hanford site in Washington State into borosilicate glasses. During the vitrification process, due to the thermal gradient in the steel canister, the melt is prone to the crystallization of nepheline phase, which has been reported to significantly decrease the long-term chemical durability of the final waste form. Deeper understanding of the nepheline crystallization problem will facilitate advanced composition design with increased waste loadings, and hence can directly reduce the overall cost. In this pursuit, efforts have been made to predict the propensity of nepheline crystallization in the nuclear waste glasses by investigating composition - property relationships, and several empirical models have been proposed based on large volumes of experimental data. Due to the statistical nature of these models, they are only applicable or valid within the composition domain encompassed by the utilized dataset. Hence, they are demonstrated to fail or are over conservative in certain circumstances. Furthermore, due to their non-scientific basis, which simply predicts whether or not a melt is expected to crystallize nepheline upon cooling into the final vitrified form based on the chemical composition, these models do not facilitate the design of novel glass composition with increased waste loadings. In light of the discussed rationale, the overarching goal of this research is to unearth the structural descriptors governing the crystallization behavior of the nepheline phase in simplified High-Level waste (HLW) glasses, and to establish composition - structure - property relationships in multicomponent silicate glasses, eventually pushing the boundaries of our understanding in glass science.A set of studies are conducted in nepheline-based Na2O-Al2O3-B2O3-SiO2 system to systematically investigate the effect of various structure scripters on the propensity of nepheline crystallization. In general, it has been found that the Al/Si mixing degree, in other words, the formation/depletion of Al-O-Si linkages, is critically important in determining the nepheline crystallization tendency. In terms of the network modifier environment, the alkali coordination in the glass network should exhibit similar values as those found in synthetic nepheline for the phase to crystallize. In details, the structural arrangements and short-medium structural variations of the glass network with the change in chemical composition have been investigated by state-of-art structural characterization techniques including Mossbauer, Raman and advanced NMR spectroscopy along with molecular dynamic (MD) simulations. It has been found that in aluminoborosilicate-based glasses, the addition of Fe2O3 and P2O5 induces significant structural rearrangements of the overall glass network, which is considered as the origins of the suppression of nepheline crystallization observed in the investigated system. Furthermore, the introduction of Ca2+, a high cation field strength cation, leads to a change in (1) network former mixing degree and (2) modifier, particularly Na+ , coordination in the glass network. Both of these two structural scripters are shown to effectively alter the nepheline crystallization propensity. In the end, attempts have been made to establish quantitative composition-structure-property relationships in alkali aluminoborosilicate glasses, and the structure origin of the mixed alkali effect (MAE) is discussed.

English

ISBN: 9798310167377Subjects--Topical Terms:

586835
Engineering.
Subjects--Index Terms:

Composition-structure-property relationships

Structure and Crystallization Behavior of Sodium- and Alumina-Rich Model High-Level Nuclear Waste Glasses /
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520 $a The United States Department of Energy (DOE) is planning to vitrify around 56 million gallons of radioactive waste stored underground at Hanford site in Washington State into borosilicate glasses. During the vitrification process, due to the thermal gradient in the steel canister, the melt is prone to the crystallization of nepheline phase, which has been reported to significantly decrease the long-term chemical durability of the final waste form. Deeper understanding of the nepheline crystallization problem will facilitate advanced composition design with increased waste loadings, and hence can directly reduce the overall cost. In this pursuit, efforts have been made to predict the propensity of nepheline crystallization in the nuclear waste glasses by investigating composition - property relationships, and several empirical models have been proposed based on large volumes of experimental data. Due to the statistical nature of these models, they are only applicable or valid within the composition domain encompassed by the utilized dataset. Hence, they are demonstrated to fail or are over conservative in certain circumstances. Furthermore, due to their non-scientific basis, which simply predicts whether or not a melt is expected to crystallize nepheline upon cooling into the final vitrified form based on the chemical composition, these models do not facilitate the design of novel glass composition with increased waste loadings. In light of the discussed rationale, the overarching goal of this research is to unearth the structural descriptors governing the crystallization behavior of the nepheline phase in simplified High-Level waste (HLW) glasses, and to establish composition - structure - property relationships in multicomponent silicate glasses, eventually pushing the boundaries of our understanding in glass science.A set of studies are conducted in nepheline-based Na2O-Al2O3-B2O3-SiO2 system to systematically investigate the effect of various structure scripters on the propensity of nepheline crystallization. In general, it has been found that the Al/Si mixing degree, in other words, the formation/depletion of Al-O-Si linkages, is critically important in determining the nepheline crystallization tendency. In terms of the network modifier environment, the alkali coordination in the glass network should exhibit similar values as those found in synthetic nepheline for the phase to crystallize. In details, the structural arrangements and short-medium structural variations of the glass network with the change in chemical composition have been investigated by state-of-art structural characterization techniques including Mossbauer, Raman and advanced NMR spectroscopy along with molecular dynamic (MD) simulations. It has been found that in aluminoborosilicate-based glasses, the addition of Fe2O3 and P2O5 induces significant structural rearrangements of the overall glass network, which is considered as the origins of the suppression of nepheline crystallization observed in the investigated system. Furthermore, the introduction of Ca2+, a high cation field strength cation, leads to a change in (1) network former mixing degree and (2) modifier, particularly Na+ , coordination in the glass network. Both of these two structural scripters are shown to effectively alter the nepheline crystallization propensity. In the end, attempts have been made to establish quantitative composition-structure-property relationships in alkali aluminoborosilicate glasses, and the structure origin of the mixed alkali effect (MAE) is discussed.
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