Understanding the origin and the consequences of glass alteration regimes is necessary for the prediction of nuclear glass durability. The so-called “stage 3” or “resumption of alteration regime” of glasses used to sequester nuclear waste by vitrification, is characterized by a sudden acceleration of glass alteration rate arising from the precipitation of secondary minerals, mainly zeolites. To study this process, a promising approach is developed, based on seeding by synthesized zeolite seeds. This study quantitatively links the alteration of a six-oxide reference borosilicate glass (ISG) and the precipitation of zeolites that affects concentrations of key species—in particular aluminum—and thus the glass dissolution rate. The characterization of stage 3—easier at alkaline pH—can now be extended to pH conditions more representative of those found in a geological repository thanks to seeding that reduces, or even eliminates, the latency period preceding a resumption of glass alteration. The resumption occurrence and glass dissolution rate are related with temperature and pH. This study shows that the detrimental effect of zeolite precipitation decreases with decreasing pH and temperature, until it is no longer detectable at a pH around 9 imposed by the dissolution of the ISG glass. Even for both high temperature and high pH, the resumption rate is lower than the initial alteration rate, which remains the fastest kinetic regime.

为了预测核玻璃的耐用性，必须了解玻璃蚀变制度的起源和后果。用于通过玻璃化隔离核废料的玻璃的所谓“第3阶段”或“恢复变化状态”，其特征在于，由于次要矿物（主要是沸石）的沉淀而引起的玻璃变化速率的突然加速。为了研究该过程，基于合成沸石种子的播种，开发了一种有前途的方法。这项研究定量地将六氧化物参比硼硅酸盐玻璃（ISG）的变化与沸石的沉淀联系在一起，这影响了关键物质（特别是铝）的浓度，从而影响了玻璃的溶解速度。由于播种减少或什至消除了重新开始玻璃蚀变的潜伏期，现在可以将第3阶段的表征（在碱性pH下更容易）扩展到更能代表地质库中条件的pH条件。恢复发生和玻璃溶解速率与温度和pH有关。这项研究表明，随着pH值和温度的降低，沸石沉淀的有害作用逐渐降低，直到在ISG玻璃溶解所造成的pH值约为9时不再能够检测到。即使对于高温和高pH值，恢复速率也低于初始改变速率，而初始改变速率仍然是最快的动力学机制。恢复发生和玻璃溶解速率与温度和pH有关。这项研究表明，随着pH值和温度的降低，沸石沉淀的有害作用逐渐降低，直到在ISG玻璃溶解所造成的pH值约为9时不再能够检测到。即使对于高温和高pH值，恢复速率也低于初始改变速率，而初始改变速率仍然是最快的动力学机制。恢复发生和玻璃溶解速率与温度和pH有关。这项研究表明，随着pH值和温度的降低，沸石沉淀的有害作用逐渐降低，直到在ISG玻璃溶解所造成的pH值约为9时不再能够检测到。即使对于高温和高pH值，恢复速率也低于初始改变速率，而初始改变速率仍然是最快的动力学机制。