Effect of Lithium Concentration on the Network Connectivity of Nuclear Waste Glasses

BLACK, Aine, SCRIMSHIRE, Alex, IUGA, Dinu, LAVALLEE, Yan, MORRISON, Kate, BINGHAM, Paul, TAYLOR, Tracey, LEAY, Laura, HARRISON, Mike, BLANC, Frederick and PATEL, Maulik (2024). Effect of Lithium Concentration on the Network Connectivity of Nuclear Waste Glasses. Journal of Non-Crystalline Solids, 646: 123234. [Article]

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Abstract
Structure of borosilicate glasses with varying Li2O contents were investigated using Magic Angle Spinning (MAS) Nuclear Magnetic Resonance (NMR), employing 6Li, 11B, 23Na, 27Al and 29Si nuclei. 11B MAS NMR revealed that increasing Li2O contents result in formation of [BO4]- sites at the expense of BO3. 11B{6Li} and 27Al{6Li} dipolar heteronuclear multiple quantum correlation (D-HMQC) NMR revealed Li as a charge compensator for anionic tetrahedral sites with increased Li. 11B{6Li} J-coupling mediated HMQC NMR highlighted the possible association of Li with non-bridging oxygens on Q2 and Q3 sites, indicating its dual role in the glass network. 29Si and 23Na MAS NMR spectra showed depolymerisation of the silicate network and shortening of Na-O bond lengths with increased Li. NMR results are supported by Raman spectroscopy and thermal analysis that indicate depolymerisation of the silicate network and a reduction in glass transition temperature at higher Li content.
Plain Language Summary

The Role of Lithium in Enhancing Nuclear Waste Glass Structures

What is it about?

This research investigates how lithium concentration affects the structure of borosilicate glasses used for storing high-level nuclear waste. These glasses immobilize radioactive materials, ensuring safe, long-term containment. The study focuses on two glass types—Mixture Windscale (MW) and Calcium Zinc (CaZn)—with varying lithium levels. The goal is to understand how lithium influences the glass network’s durability and ability to contain waste. Using advanced techniques like Nuclear Magnetic Resonance (NMR) and Raman spectroscopy, researchers analyzed the interaction of lithium with other elements like boron and silicon. Lithium modifies the glass network by depolymerizing silicate structures and stabilizing tetrahedral boron units, which are critical for the glass’s durability. Findings show that higher lithium levels reduce the glass transition temperature but increase its adaptability for incorporating complex waste elements.

Why is it important?

Nuclear waste management is a critical challenge, with long-term storage requiring materials that remain stable for thousands of years. Borosilicate glasses are the preferred choice for immobilizing high-level waste due to their durability and capacity to incorporate multiple elements. However, their performance can vary based on the chemical composition. Lithium’s dual role in modifying and stabilizing glass networks enhances their ability to adapt to different waste compositions. By understanding lithium’s effects, this study provides insights for designing glasses that are more efficient and cost-effective for nuclear waste storage. Optimizing these materials ensures safer storage, reduces environmental risks, and supports sustainable nuclear energy. This work is particularly relevant as the UK prepares to dispose of vitrified nuclear waste in deep geological facilities. The findings could lead to improved glass formulations capable of withstanding extreme conditions like radiation and groundwater exposure.

Key Takeaways:

1. Lithium improves glass structure by modifying silicate and borate networks.

2. Higher lithium levels enhance adaptability but lower transition temperatures.

3. Calcium Zinc glasses handle complex waste better than simpler formulations.

4. Optimized lithium content ensures long-term stability of nuclear waste glass.

5. Insights aid in safer and more efficient nuclear waste management globally.

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