Elemental and isotopic (29Si and 18O) tracing of glass alteration mechanisms

To better understand glass alteration mechanisms, especially alteration layers formation, leaching experiments of a borosilicate glass (SON68) doped with a different rare earth element (La, Ce, or Nd) with solutions rich in 29Si and 18O were carried out. The coupled analyses of glass, alteration products, and solution led to a complete elemental and isotopic (29Si and 18O) budget. They revealed different behaviours of elements that depend not only on their structural role in the glass, but also on their affinity for alteration products (gel, phyllosilicates, phosphates). However, analyses of both glass and solution are not sufficient to describe the real exchanges occurring between glass and solution. The use of 29Si and 18O tracers gives new insights on the formation of alteration layers. During alteration the phyllosilicates records the isotopic variations of the leaching solution. Their isotopic signatures highlight a mechanism of dissolution/precipitation, which implies equilibrium between the secondary phases and the solution. On the other hand the gel isotopic signature, that is intermediate between the glass and the solution, substantiates the hypothesis that the gel is formed by hydrolysis/condensation reactions. This mechanism can thus explain the influence of the gel formation conditions (alteration conditions, solution saturation) on the structure (reorganisation) and texture (porosity) of this layer and on its protective effect. These hydrolysis/condensation reactions are also certainly involved in the aluminosilicate glass alteration and in the formation of palagonite.