Stable, durable immobilization of radioactive wastes requires robust understanding of the sub-surface geochemical processes that occur in repository environments. For example, the accelerated dissolution (corrosion) of nuclear waste immobilization glasses (i.e., the so-called “Stage III” corrosion) following the precipitation of zeolitic phases is a significant issue that could result in radionuclide release. However, current uncertainties in establishing the tendency for the persistence of zeolites results in difficulties in estimating the chemical environments and state variables that favor zeolite precipitation. To assess the tendency for Stage III corrosion, we compiled a unified, internally-consistent thermodynamic database to estimate zeolite stability under conditions relevant to nuclear waste repositories (namely, p = 1 bar and T < 95 °C), i.e., for compounds including: analcime, clinoptilolite, mordenite, erionite, thomsonite, bikitaite, brewsterite, dachiardite, epistilbite, ferrierite, gonnardite, harmotome, leonhardite, paranatrolite, tetranatrolite, yugawaralite zeolite X, and zeolite P(Ca). The database, which features both existing and/or newly-derived thermodynamic properties, is integrated with a Gibbs (free) energy minimization (GEM) solver to estimate stable zeolite phase equilibria and their partitioning at equilibrium. The database offers favorable predictions of the solubility of the zeolite phases as a function of temperature. The validity of the database is ascertained by comparing newly-constructed equilibrium activity diagrams with experimental observations of zeolite formation during glass dissolution across conditions encompassing diverse solution chemistries, pH’s, and temperatures.

稳定，持久地固定放射性废物需要深入了解储存环境中发生的地下地球化学过程。例如，沸石相沉淀后核废料固定玻璃的加速溶解（腐蚀）（即所谓的“ III期”腐蚀）是一个重要问题，可能导致放射性核素释放。然而，目前在确定沸石持久性趋势方面的不确定性导致难以估计有利于沸石沉淀的化学环境和状态变量。为了评估III期腐蚀的趋势，我们编译了一个统一的内部一致的热力学数据库，以估算在与核废料库相关的条件下的沸石稳定性（即，p  = 1 bar和T <95°C），即用于以下化合物：芳族金属，斜发沸石，丝光沸石，毛沸石，硫磺铝石，方钠铁矿，碳酸钙镁石，da石辉石，硬石辉石，镁碱沸石，针铁矿，扁榴石，Harmotome，莱onhardite，方钠石，方钠石，Yugawaralite沸石（X， Ca）。该数据库同时具有现有和/或新衍生的热力学特性，并与吉布斯（自由）能量最小化（GEM）求解器集成在一起，以估算稳定的沸石相平衡及其在平衡状态下的分配。该数据库提供了沸石相的溶解度随温度变化的有利预测。