title: Origin and consequences of silicate glass passivation by surface layers.
abstract: Silicate glasses are durable materials, but are they sufficiently durable to confine highly radioactive wastes for hundreds of thousands years? Addressing this question requires a thorough understanding of the mechanisms underpinning aqueous corrosion of these materials. Here we show that in silica-saturated solution, a model glass of nuclear interest corrodes but at a rate that dramatically drops as a passivating layer forms. Water ingress into the glass, leading to the congruent release of mobile elements (B, Na and Ca), is followed by in situ repolymerization of the silicate network. This material is at equilibrium with pore and bulk solutions, and acts as a molecular sieve with a cutoff below 1 nm. The low corrosion rate resulting from the formation of this stable passivating layer enables the objective of durability to be met, while progress in the fundamental understanding of corrosion unlocks the potential for optimizing the design of nuclear glass-geological disposal.
authors.affiliation: CEA, DEN, DTCD, SECM, F-30207 Bagnols-sur-Ceze, France.
authors.forename: Stéphane
authors.initials: S
authors.lastname: Gin
authors.affiliation: CEA, DEN, DTCD, SECM, F-30207 Bagnols-sur-Ceze, France.
authors.forename: Patrick
authors.initials: P
authors.lastname: Jollivet
authors.affiliation: CEA, DEN, DTCD, SECM, F-30207 Bagnols-sur-Ceze, France.
authors.forename: Maxime
authors.initials: M
authors.lastname: Fournier
authors.affiliation: CEA, DEN, DTCD, SECM, F-30207 Bagnols-sur-Ceze, France.
authors.forename: Frédéric
authors.initials: F
authors.lastname: Angeli
authors.affiliation: CEA, DEN, DTCD, SECM, F-30207 Bagnols-sur-Ceze, France.
authors.forename: Pierre
authors.initials: P
authors.lastname: Frugier
authors.affiliation: CEA, DSM, IRAMIS, NIMBE, UMR 3299, F-91191 Gif-sur-Yvette, France.
authors.forename: Thibault
authors.initials: T
authors.lastname: Charpentier