Hydrothermal alteration of silicate minerals: effects of crystallographic orientation and fluid saturation state

Abstract:

Prediction of reaction kinetics of fluid/rock interactions represents a critical issue for several geological and engineering concerns. In the specific context of geothermal energy, the relative intensities of primary mineral leaching and secondary phase formation significantly affect porosity and permeability of the reservoir, thereby influencing its hydraulic performance and the efficiency of a geothermal site. Moreover, it is noteworthy that in general, the circulation of aqueous fluids induces only modest modifications of their chemical composition, which slightly deviate from an equilibrium state. Therefore, fluid rock interactions take place at close-to-equilibrium conditions, where the rate-affinity relations are poorly known and intensively debated [1].

To unravel these points, in the context of the geothermal power station of Soultz-sous-Forêts (Alsace, France), our strategy consists in (1) investigating the dissolution of the main cleavages of K-spar, one of the prevalent primary minerals in the reservoir, in order to decipher the impact of crystallographic orientation and microstructural surface modifications on the dissolution kinetics and (2) proposing a relation between K-spar dissolution rate and the Gibbs free energy of reaction (∆G) over a wide range of ∆G conditions.

Our experimental work relies on a coupled approach which combines classical experiments of K-spar dissolution monitored by aqueous chemical analyses (ICPAES) and innovative techniques of nm to μm-scale characterization of solid surface (FIB-TEM, AFM, VSI) [2].

Our ongoing experiments evidence that K-spar dissolution is an anisotropic process, with faces (-1-1 1) dissolving up to ten times faster than the slowest (001) faces. The complex evolution of surface topography with the occurrence of etch pits is at odds with the shrinking core model implemented in most of reactive-transport codes, representing a possible cause of an apparent modification of silicate dissolution rate over time. In addition, the relation between K-spar dissolution rate and ∆G seems to differ from the transition state theory currently implemented into geochemical codes. Taken together, these new findings show promise as a means for modifying reactive transport codes and improving the predictive ability of geochemical simulations.