Nanometre-scale evidence for interfacial dissolution-reprecipitation control of silicate glass corrosion

被引:245
作者
Hellmann, Roland [1 ,2 ]
Cotte, Stephane [1 ,2 ]
Cadel, Emmanuel [3 ]
Malladi, Sairam [4 ]
Karlsson, Lisa S. [5 ]
Lozano-Perez, Sergio [5 ]
Cabie, Martiane [6 ]
Seyeux, Antoine [7 ]
机构
[1] Univ Grenoble Alpes, ISTerre, F-38041 Grenoble 9, France
[2] CNRS, ISTerre, F-38041 Grenoble, France
[3] Univ Rouen, CNRS, INSA, GPM, F-76821 St Etienne, France
[4] Delft Univ Technol, Kavli Inst Nanosci Delft, NL-2628 CJ Delft, Netherlands
[5] Univ Oxford, Dept Mat, Oxford OX1 3PH, England
[6] Aix Marseille Univ, CP2M, F-13397 Marseille, France
[7] CNRS Chim ParisTech, Inst Rech Chim Paris, F-75005 Paris, France
关键词
NUCLEAR GLASS; AQUEOUS DISSOLUTION; LAYER FORMATION; BASALTIC GLASS; SURFACE-LAYERS; MECHANISM; WATER; CHEMISTRY; 50-DEGREES-C; MINERALS;
D O I
10.1038/nmat4172
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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(1), or the biogeochemical weathering of volcanic glasses in seawater(2). The aqueous dissolution of synthetic and natural glasses results in the formation of a hydrated, cation-depleted near-surface alteration zone(1,3-8) and, depending on alteration conditions, secondary crystalline phases on the surface(1,2,4-7). The long-standing accepted model of glass corrosion is based on diffusion-coupled hydration and selective cation release, producing a surface-altered zone(2,5-8). 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(9-13).
引用
收藏
页码:307 / 311
页数:5
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