• Nagel, T. J.
• Grange, M. L.
• Nemchin, A. A.
• Kilburn, Matthew
• Janßen, A. C.
• Icenhower, J. P.
• Geisler, T.
• Fonseca, R. O. C.

Abstract

© 2015 Elsevier Ltd. Currently accepted mechanistic models describing aqueous corrosion of borosilicate glasses are based on diffusion-controlled hydrolysis, hydration, ion exchange reactions, and subsequent re-condensation of the hydrolyzed glass network, leaving behind a residual hydrated glass or gel layer. Here, we report results of novel oxygen and silicon isotope tracer experiments with ternary Na borosilicate glasses that can be better explained by a process that involves the congruent dissolution of the glass, which is spatially and temporally coupled to the precipitation and growth of an amorphous silica layer at an inwardly moving reaction interface. Such a process is thermodynamically driven by the solubility difference between the glass and amorphous silica, and kinetically controlled by glass dissolution reactions at the reaction front, which, in turn, are controlled by the transport of water and solute elements through the growing corrosion zone. Understanding the coupling of these reactions is the key to understand the formation of laminar or more complex structural and chemical patterns observed in natural corrosion zones of ancient glasses. We suggest that these coupled processes also have to be considered to realistically model the long-term performance of silicate glasses in aqueous environments.

Topics

• impedance spectroscopy
• amorphous
• corrosion
• experiment
• Oxygen
• glass
• glass
• Silicon
• precipitation