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首页> 美国卫生研究院文献>Materials >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
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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

机译：重离子辐照对液硅拉曼光谱法原位和实时研究硼硅酸盐玻璃正向溶解速率的影响

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摘要

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.
机译：硼硅酸盐玻璃是用于固定核电站中乏燃料的后处理中高水平核废料（HLW）固定的首选材料。要评估核废玻璃的长期稳定性，了解自辐照如何影响玻璃的结构状态并影响其溶解行为至关重要。在这项研究中，我们专注于重离子辐照对非放射性三元硼硅酸盐玻璃正向溶解速率的影响。为了产生更大的辐射缺陷，使用 197 Au离子对玻璃进行重离子辐照，该离子穿透玻璃的深度约为50 µm。用拉曼光谱法表征了结构破坏，揭示了在辐照玻璃中硅酸盐和硼酸盐网络的显着解聚和平均硼配位数的降低。在80至85°C（初始pH = 7.1）的温度下，用辐照过的玻璃在不饱和二氧化硅，0.5 M NaHCO3溶液中进行了实时原位流式细胞拉曼光谱腐蚀实验。在时间和空间上解析的原位拉曼数据显示，与未辐照玻璃相比，辐照玻璃的正向溶解速率提高了3.7±0.5倍，表明辐照引起的结构破坏对溶解动力学具有显着影响。

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