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Acceleration of glass alteration rates induced by zeolite seeds at controlled pH
Applied Geochemistry ( IF 3.4 ) Pub Date : 2020-02-01 , DOI: 10.1016/j.apgeochem.2019.104515
James J. Neeway , Benjamin P. Parruzot , Jeffrey F. Bonnett , Joelle T. Reiser , Sebastien N. Kerisit , Joseph V. Ryan , Jarrod V. Crum

Abstract As the glass-water reaction proceeds, certain glass compositions undergo a delayed acceleration in the alteration rate – a phenomenon that is commonly referred to as Stage III behavior – which generally coincides with zeolite formation. However, studying Stage III in the laboratory is difficult because the time scale required to observe Stage III behavior can vary from months to several years, and the solution conditions that initiate this acceleration remain poorly understood. Consequently, the development of a corrosion test method capable of quantifying Stage III rates in a timely manner would be of great benefit to both the scientific community and policy makers concerned with nuclear waste disposal. In this work, we induced and measured the acceleration in the corrosion rate of the AFCI glass by seeding static corrosion tests with zeolite Na–P2 at imposed pH90°C values ranging from 9.5 to 11.5. The log10 induced Stage III rates increased linearly with increasing pH and were measured to be between the forward and residual rates of AFCI. Tests designed to compare induced Stage III rates obtained for different seeding times showed that the induced Stage III rates were faster in the absence of an alteration layer. In summary, the use of the seeded test method allows for a quantification of induced Stage III rates in a relatively short, one-month time period.

中文翻译:

沸石晶种在受控 pH 值下加速玻璃化变率

摘要 随着玻璃-水反应的进行,某些玻璃成分的变质速率会延迟加速——这种现象通常被称为第三阶段行为——通常与沸石的形成同时发生。然而,在实验室研究第三阶段是困难的,因为观察第三阶段行为所需的时间尺度可能从几个月到几年不等,而且引发这种加速的解决方案条件仍然知之甚少。因此,开发能够及时量化第三阶段速率的腐蚀测试方法将对科学界和关注核废料处理的政策制定者都大有裨益。在这项工作中,我们通过在 9.5 到 11.5 的 pH90°C 值范围内用沸石 Na-P2 进行种子静态腐蚀试验来诱导和测量 AFCI 玻璃腐蚀速率的加速。log10 诱导的 III 期速率随着 pH 值的增加而线性增加,并被测量为介于 AFCI 的正向和残留速率之间。旨在比较不同播种时间获得的诱导阶段 III 速率的测试表明,在没有蚀变层的情况下,诱导阶段 III 速率更快。总之,使用种子测试方法可以在相对较短的一个月的时间内量化诱导的 III 期发病率。旨在比较不同播种时间获得的诱导阶段 III 速率的测试表明,在没有蚀变层的情况下,诱导阶段 III 速率更快。总之,使用种子测试方法可以在相对较短的一个月的时间内量化诱导的 III 期发病率。旨在比较不同播种时间获得的诱导阶段 III 速率的测试表明,在没有蚀变层的情况下,诱导阶段 III 速率更快。总之,使用种子测试方法可以在相对较短的一个月的时间内量化诱导的 III 期发病率。
更新日期:2020-02-01
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