Abstract Alteration of widespread interfaces between cements and clays in geological time scales is essential to the safety assessment of radioactive waste repositories but not well understood partly due to the low reliability of thermodynamic data for zeolites. Here, we collected and full-scale characterized Ca-based zeolites with six types of frameworks that could possibly form in the interfaces. Besides, chemical interactions between degraded cementitious phases and rock forming minerals after equilibrating for ~6 years were investigated. By using the currently generated thermodynamic data of selected zeolites, chemical interactions in the cement/rock systems were studied, showing that no equilibrium was reached after 6 years and zeolites favored in thermodynamics, such as chabazite and gismondine rather than faujasite, can be expected to form at even longer timescale. The experimentally derived thermodynamic data was verified preliminarily by establishing consistent predominance diagrams of cement-zeolite-clay minerals, helping to predict zeolite stability domains in large timescales.

中文翻译：

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使用实验产生的沸石溶解度数据对水泥/岩石相互作用进行热力学研究

摘要 地质时间尺度上水泥和粘土之间广泛界面的改变对于放射性废物处置库的安全评估至关重要，但部分原因是沸石热力学数据的可靠性低。在这里，我们收集并全面表征了具有六种可能在界面中形成的骨架的钙基沸石。此外，还研究了平衡约 6 年后降解胶结相与造岩矿物之间的化学相互作用。通过使用当前生成的选定沸石的热力学数据，研究了水泥/岩石系统中的化学相互作用，表明 6 年后未达到平衡，沸石在热力学方面更受青睐，例如菱沸石和吉士蒙菱，而不是八面沸石，预计会在更长的时间范围内形成。通过建立水泥-沸石-粘土矿物的一致性优势图，初步验证了实验得出的热力学数据，有助于预测大时间尺度的沸石稳定性域。