in particular the leached layer theory. Most importantly, our data provide critical evidence for 51 a single mechanism based on interfacial dissolution-reprecipitation. This concept not only 52 unifies weathering processes for the first time, but we also suggest that nanoscale-surface 53 processes can have a potentially negative impact on CO 2 uptake associated with chemical 54 weathering. The results in this study, when combined with recently published research on 55 fluid-assisted mineral replacement reactions, supports the idea that dissolution-reprecipitation 56 is a universal mechanism controlling fluid-mineral interactions . 57Based on this we propose the existence of a chemical weathering continuum based solely on 58 the interfacial dissolution-reprecipitation mechanism. 59 3

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.

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[1] Geological repositories subject to the injection of large amounts of anthropogenic carbon dioxide will undergo chemical and mechanical instabilities for which there are currently little experimental data. This study reports on experiments where low and high P co 2 (8 MPa) aqueous fluids were injected into natural rock samples. The experiments were performed in flow-through triaxial cells, where the vertical and confining stresses, temperature, and pressure and composition of the fluid were separately controlled and monitored. The axial vertical strains of two limestones and one sandstone were continuously measured during separate experiments for several months, with a strain rate resolution of 10 À11 s À1. Fluids exiting the triaxial cells were continuously collected and their compositions analyzed. The high P co 2 fluids induced an increase in strain rates of the limestones by up to a factor of 5, compared to the low P co 2 fluids. Injection of high P co 2 fluids into the sandstone resulted in deformation rates one order of magnitude smaller than the limestones. The creep accelerating effect of high P co 2 fluids with respect to the limestones was mainly due to the acidification of the injected fluids, resulting in a significant increase in solubility and reaction kinetics of calcite. Compared to the limestones, the much weaker response of the sandstone was due to the much lower solubility and reactivity of quartz in high P co 2 fluids. In general, all samples showed a positive correlation between fluid flow rate and strain rate. X-ray tomography results revealed significant increases in porosity at the inlet portion of each core; the porosity increases were dependent on the original lithological structure and composition. The overall deformation of the samples is interpreted in terms of simultaneous dissolution reactions in pore spaces and intergranular pressure solution creep.

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