title: Nanometre-scale evidence for interfacial dissolution-reprecipitation control of silicate glass corrosion.
abstract: Silicate glasses are durable solids, and yet they are chemically unstable in contact with aqueous fluids-this has important implications for numerous industrial applications related to the corrosion resistance of glasses, or the biogeochemical weathering of volcanic glasses in seawater. The aqueous dissolution of synthetic and natural glasses results in the formation of a hydrated, cation-depleted near-surface alteration zone and, depending on alteration conditions, secondary crystalline phases on the surface. The long-standing accepted model of glass corrosion is based on diffusion-coupled hydration and selective cation release, producing a surface-altered zone. However, using a combination of advanced atomic-resolution analytical techniques, our data for the first time reveal that the structural and chemical interface between the pristine glass and altered zone is always extremely sharp, with gradients in the nanometre to sub-nanometre range. These findings support a new corrosion mechanism, interfacial dissolution-reprecipitation. Moreover, they also highlight the importance of using analytical methods with very high spatial and mass resolution for deciphering the nanometre-scale processes controlling corrosion. Our findings provide evidence that interfacial dissolution-reprecipitation may be a universal reaction mechanism that controls both silicate glass corrosion and mineral weathering.
authors.affiliation: 1] Université Grenoble Alpes, ISTerre, F-38041 Grenoble cedex 9, France [2] CNRS, ISTerre, F-38041 Grenoble, France.
authors.forename: Roland
authors.initials: R
authors.lastname: Hellmann
authors.affiliation: 1] Université Grenoble Alpes, ISTerre, F-38041 Grenoble cedex 9, France [2] CNRS, ISTerre, F-38041 Grenoble, France.
authors.forename: Stéphane
authors.initials: S
authors.lastname: Cotte
authors.affiliation: CNRS, Université de Rouen, INSA, GPM, F-76801 Saint Etienne du Rouvray, France.
authors.forename: Emmanuel
authors.initials: E
authors.lastname: Cadel
authors.affiliation: Kavli Institute of Nanoscience Delft, Delft University of Technology, 2628 CJ Delft, The Netherlands.
authors.forename: Sairam
authors.initials: S
authors.lastname: Malladi
authors.affiliation: Department of Materials, Oxford University, Oxford OX1 3PH, UK.
authors.forename: Lisa S
authors.initials: LS
authors.lastname: Karlsson
authors.affiliation: Department of Materials, Oxford University, Oxford OX1 3PH, UK.
authors.forename: Sergio
authors.initials: S
authors.lastname: Lozano-Perez
authors.affiliation: Aix-Marseille Université, CP2M, F-13397 Marseille, France.
authors.forename: Martiane
authors.initials: M
authors.lastname: Cabié
authors.affiliation: Institut de Recherche de Chimie Paris, CNRS-Chimie ParisTech, 11 rue Pierre et Marie Curie 75005 Paris, France.
authors.forename: Antoine
authors.initials: A
authors.lastname: Seyeux
mesh_terms: D003343:Corrosion; D005898:Glass / Q000737:chemistry*; D008422:Materials Testing; D049329:Nanostructures / Q000737:chemistry* / Q000648:ultrastructure*; D010316:Particle Size; D017640:Silicates / Q000737:chemistry*; D012997:Solvents / Q000737:chemistry*; D013499:Surface Properties; D014867:Water / Q000737:chemistry*
chemical_list: D017640:Silicates; D012997:Solvents; D014867:Water