Lönartz, Mara Iris ; Dohmen, Lars ; Lenting, Christoph ; Trautmann, Christina ; Lang, Maik ; Geisler, Thorsten (2024)
The Effect of Heavy Ion Irradiation on the Forward Dissolution Rate of Borosilicate Glasses Studied In Situ and Real Time by Fluid-Cell Raman Spectroscopy.
In: Materials, 2019, 12 (9)
doi: 10.26083/tuprints-00015662
Artikel, Zweitveröffentlichung, Verlagsversion
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Kurzbeschreibung (Abstract)
Borosilicate glasses are the favored material for immobilization of high-level nuclear waste (HLW) from the reprocessing of spent fuel used in nuclear power plants. To assess the long-term stability of nuclear waste glasses, it is crucial to understand how self-irradiation affects the structural state of the glass and influences its dissolution behavior. In this study, we focus on the effect of heavy ion irradiation on the forward dissolution rate of a non-radioactive ternary borosilicate glass. To create extended radiation defects, the glass was subjected to heavy ion irradiation using ¹⁹⁷Au ions that penetrated ~50 µm deep into the glass. The structural damage was characterized by Raman spectroscopy, revealing a significant depolymerization of the silicate and borate network in the irradiated glass and a reduction of the average boron coordination number. Real time, in situ fluid-cell Raman spectroscopic corrosion experiments were performed with the irradiated glass in a silica-undersaturated, 0.5 M NaHCO₃ solution at temperatures between 80 and 85 °C (initial pH = 7.1). The time- and space-resolved in situ Raman data revealed a 3.7 ± 0.5 times increased forward dissolution rate for the irradiated glass compared to the non-irradiated glass, demonstrating a significant impact of irradiation-induced structural damage on the dissolution kinetics.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2024 |
| Autor(en): | Lönartz, Mara Iris ; Dohmen, Lars ; Lenting, Christoph ; Trautmann, Christina ; Lang, Maik ; Geisler, Thorsten |
| Art des Eintrags: | Zweitveröffentlichung |
| Titel: | The Effect of Heavy Ion Irradiation on the Forward Dissolution Rate of Borosilicate Glasses Studied In Situ and Real Time by Fluid-Cell Raman Spectroscopy |
| Sprache: | Englisch |
| Publikationsjahr: | 19 Januar 2024 |
| Ort: | Darmstadt |
| Publikationsdatum der Erstveröffentlichung: | 2019 |
| Ort der Erstveröffentlichung: | Basel |
| Verlag: | MDPI |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Materials |
| Jahrgang/Volume einer Zeitschrift: | 12 |
| (Heft-)Nummer: | 9 |
| Kollation: | 13 Seiten |
| DOI: | 10.26083/tuprints-00015662 |
| URL / URN: | https://tuprints.ulb.tu-darmstadt.de/15662 |
| Zugehörige Links: | |
| Herkunft: | Zweitveröffentlichung DeepGreen |
| Kurzbeschreibung (Abstract): | Borosilicate glasses are the favored material for immobilization of high-level nuclear waste (HLW) from the reprocessing of spent fuel used in nuclear power plants. To assess the long-term stability of nuclear waste glasses, it is crucial to understand how self-irradiation affects the structural state of the glass and influences its dissolution behavior. In this study, we focus on the effect of heavy ion irradiation on the forward dissolution rate of a non-radioactive ternary borosilicate glass. To create extended radiation defects, the glass was subjected to heavy ion irradiation using ¹⁹⁷Au ions that penetrated ~50 µm deep into the glass. The structural damage was characterized by Raman spectroscopy, revealing a significant depolymerization of the silicate and borate network in the irradiated glass and a reduction of the average boron coordination number. Real time, in situ fluid-cell Raman spectroscopic corrosion experiments were performed with the irradiated glass in a silica-undersaturated, 0.5 M NaHCO₃ solution at temperatures between 80 and 85 °C (initial pH = 7.1). The time- and space-resolved in situ Raman data revealed a 3.7 ± 0.5 times increased forward dissolution rate for the irradiated glass compared to the non-irradiated glass, demonstrating a significant impact of irradiation-induced structural damage on the dissolution kinetics. |
| Freie Schlagworte: | borosilicate glass corrosion, heavy ion irradiation, in situ fluid-cell Raman spectroscopy, forward dissolution rate |
| Status: | Verlagsversion |
| URN: | urn:nbn:de:tuda-tuprints-156625 |
| Zusätzliche Informationen: | This article belongs to the Special Issue Materials for Nuclear Waste Immobilization |
| Sachgruppe der Dewey Dezimalklassifikatin (DDC): | 500 Naturwissenschaften und Mathematik > 530 Physik 600 Technik, Medizin, angewandte Wissenschaften > 660 Technische Chemie |
| Fachbereich(e)/-gebiet(e): | 11 Fachbereich Material- und Geowissenschaften 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft |
| Hinterlegungsdatum: | 19 Jan 2024 14:26 |
| Letzte Änderung: | 22 Jan 2024 09:20 |
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- The Effect of Heavy Ion Irradiation on the Forward Dissolution Rate of Borosilicate Glasses Studied In Situ and Real Time by Fluid-Cell Raman Spectroscopy. (deposited 19 Jan 2024 14:26) [Gegenwärtig angezeigt]
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