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Article

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

by
Mara Iris Lönartz
1,*,
Lars Dohmen
2,
Christoph Lenting
1,
Christina Trautmann
3,
Maik Lang
4 and
Thorsten Geisler
1
1
Institut für Geowissenschaften und Meteorologie, Universität Bonn, Poppelsdorfer Schloss, Meckenheimer Allee 169, 53115 Bonn, Germany
2
SCHOTT AG, Hattenbergstr. 10, 55122 Mainz, Germany
3
GSI Helmholtzzentrum, 64291 Darmstadt and Technische Universität Darmstadt, 64287 Darmstadt, Germany
4
Department of Nuclear Engineering, University of Tennessee, Knoxville, TN 37996, USA
*
Author to whom correspondence should be addressed.
Materials 2019, 12(9), 1480; https://doi.org/10.3390/ma12091480
Submission received: 27 March 2019 / Revised: 29 April 2019 / Accepted: 1 May 2019 / Published: 7 May 2019
(This article belongs to the Special Issue Materials for Nuclear Waste Immobilization)
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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.
Keywords: borosilicate glass corrosion; heavy ion irradiation; in situ fluid-cell Raman spectroscopy; forward dissolution rate borosilicate glass corrosion; heavy ion irradiation; in situ fluid-cell Raman spectroscopy; forward dissolution rate

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MDPI and ACS Style

Lönartz, M.I.; Dohmen, L.; Lenting, C.; Trautmann, C.; Lang, M.; Geisler, T. 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. Materials 2019, 12, 1480. https://doi.org/10.3390/ma12091480

AMA Style

Lönartz MI, Dohmen L, Lenting C, Trautmann C, Lang M, Geisler T. 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. Materials. 2019; 12(9):1480. https://doi.org/10.3390/ma12091480

Chicago/Turabian Style

Lönartz, Mara Iris, Lars Dohmen, Christoph Lenting, Christina Trautmann, Maik Lang, and Thorsten Geisler. 2019. "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" Materials 12, no. 9: 1480. https://doi.org/10.3390/ma12091480

APA Style

Lönartz, M. I., Dohmen, L., Lenting, C., Trautmann, C., Lang, M., & Geisler, T. (2019). 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. Materials, 12(9), 1480. https://doi.org/10.3390/ma12091480

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