Direct Observations of the Coupling between Quartz Dissolution and Mg-Silicate Formation

Abstract

Although quartz is a stable mineral at Earth surface conditions, field samples have shown its rapid dissolution in combination with the precipitation of Mg-silicate phases. Atomic force microscopy (AFM) experiments were performed to investigate the dissolution of quartz and the precipitation of secondary phases in high-pH, Mg-rich solutions both in situ and ex situ. Experiments were conducted at room temperature with varying MgCl 2 or MgSO 4 concentrations (0.1-100 mM), pH (8.9-12) and ionic strength (<1-530 mM). The results suggest that quartz dissolves by the removal of nanoparticles on the time scale of minutes, and that a nanometer-scale gel-like layer of amorphous silica forms on the quartz surface and is thicker at higher pH. During the in situ experiments, soft and poorly attached precipitates form on the surface when the Mg concentration is high (100 mM). After 20 h in a high-pH, Mg-rich solution, solid Mg-rich precipitates can be observed at places on the surface where the gel-like silica layer is present, predominantly near surface edges where dissolution is enhanced. This suggests a coupling between the dissolution of quartz, that resulted in the gel-like layer, and the formation of secondary phases, indicating an interface-coupled dissolution-precipitation mechanism. The precipitates could not be precisely identified but evidence suggests they are likely to be amorphous Mg-silicate phases. Such a coupled reaction may provide a pathway for Mg-Si phase formation suitable as a new environmentally friendly cement.