Iron-induced structural rearrangements and their impact on sulfur solubility in borosilicate-based nuclear waste glasses

The work presented in the article combines the strength of experimental and computational materials science to understand the iron (Fe 2 O 3 ≤ 3 mol.%) -induced structural rearrangements in peralkaline aluminoborosilicate glasses and their impact on the solubility of sulfur (as SO 4 2-) in the model nuclear waste glasses. The majority (>95%) of iron exists as tetrahedrally coordinated Fe 3+ (both isolated and clustered) in the investigated glasses, thus acting as a network former being charge compensated by Na + , while the remaining exists as tetrahedrally (distorted) coordinated Fe 2+ . The addition of iron induces re-polymerization in the glass network, thus lowering the sulfur solubility in the glassy matrix. Mössbauer spectroscopy reveals an insignificant impact of sulfur on the redox behavior or environment of iron in the glass structure.

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Planète et Univers [physics]

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Format du dépôt	Fichier
Type de dépôt	Article dans une revue
Titre	en Iron-induced structural rearrangements and their impact on sulfur solubility in borosilicate-based nuclear waste glasses
Résumé	en <div><p>The work presented in the article combines the strength of experimental and computational materials science to understand the iron (Fe 2 O 3 ≤ 3 mol.%) -induced structural rearrangements in peralkaline aluminoborosilicate glasses and their impact on the solubility of sulfur (as SO 4 2-) in the model nuclear waste glasses. The majority (>95%) of iron exists as tetrahedrally coordinated Fe 3+ (both isolated and clustered) in the investigated glasses, thus acting as a network former being charge compensated by Na + , while the remaining exists as tetrahedrally (distorted) coordinated Fe 2+ . The addition of iron induces re-polymerization in the glass network, thus lowering the sulfur solubility in the glassy matrix. Mössbauer spectroscopy reveals an insignificant impact of sulfur on the redox behavior or environment of iron in the glass structure.</p></div>
Auteur(s)	Xinyi Xu ¹ , Marco Bertani ² , Rajan Saini ³ , Saeed Kamali ⁴ , Daniel R. Neuville ^{5, 6, 7} , Randall Youngman ⁸ , Alfonso Pedone ² , Ashutosh Goel ³ 1 MSSM - Icahn School of Medicine at Mount Sinai [New York] ( 354552 ) - 1 Gustave L. Levy Place New York, NY 10029-5674 - États-Unis 2 UNIMORE - Università degli Studi di Modena e Reggio Emilia = University of Modena and Reggio Emilia ( 203954 ) - 41121 Modena / 42121 Reggio Emilia - Italie 3 RU - Rutgers, The State University of New Jersey [New Brunswick] ( 36051 ) - 57 US Highway 1, New Brunswick, NJ 08901-8554 - États-Unis Rutgers University System ( 566577 ) 4 UTSI - University of Tennessee Space Institute ( 563043 ) - 411 B H Goethert Parkway, Tullahoma, TN 37388 - États-Unis 5 C2RMF - Centre de recherche et de restauration des musées de France ( 510 ) - Palais du Louvre 14 quai François Mitterand 75001 PARIS - France Ministère de la Culture et de la Communication ( 300125 ) ; Centre National de la Recherche Scientifique UMR171 ( 441569 ) 6 IPGP (UMR_7154) - Institut de Physique du Globe de Paris ( 1005035 ) - 1 rue Jussieu, 75238 Paris cedex 05 et Bât. Lamarck A case postale 7011, 75205 Paris CEDEX 13 - France Institut national des sciences de l'Univers UMR_7154 ( 300045 ) ; Université de La Réunion UMR_7154 ( 300316 ) ; Institut de Physique du Globe de Paris UMR_7154 ( 300354 ) ; Centre National de la Recherche Scientifique UMR_7154 ( 441569 ) ; Université Paris Cité UMR_7154 ( 557826 ) 7 new AGLAE - New AGLAE - CNRS/Ministère de la Culture/ENSCP ( 1007422 ) - C2RMF - Palais du Louvre 14 quai François Mitterrand 75001 Paris - France Institut de Chimie - CNRS Chimie ( 341038 ) ; Centre National de la Recherche Scientifique FR3506 ( 441569 ) 8 Corning Incorporated ( 1150773 ) - Corning, New York 14831 - États-Unis
Vulgarisation	Non
Comité de lecture	Oui
Audience	Internationale
Langue du document	Anglais
Nom de la revue	J Phys Chem C - Journal of Physical Chemistry C (ISSN : 1932-7447, ISSN électronique : 1932-7455) American Chemical Society Publié par American Chemical Society https://pubs.acs.org/journal/jpccck
Date de publication	2024-07-02
Volume	128
Numéro	28
Page/Identifiant	11870-11887
Domaine(s)	Planète et Univers [physics]
DOI	10.1021/acs.jpcc.4c02085

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2023-12-29-manuscript-iron-sulfur.pdf ( 872.22 Ko )

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https://hal.science/hal-04786838

Soumis le : samedi 16 novembre 2024 à 14:48:21

Dernière modification le : jeudi 21 novembre 2024 à 03:29:23

Dates et versions

hal-04786838, version 1 (16-11-2024)

Identifiants

HAL Id : hal-04786838 , version 1
DOI : 10.1021/acs.jpcc.4c02085

Citer

Xinyi Xu, Marco Bertani, Rajan Saini, Saeed Kamali, Daniel R. Neuville, et al.. Iron-induced structural rearrangements and their impact on sulfur solubility in borosilicate-based nuclear waste glasses. Journal of Physical Chemistry C, 2024, 128 (28), pp.11870-11887. ⟨10.1021/acs.jpcc.4c02085⟩. ⟨hal-04786838⟩

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