Dissolution and Sorption Processes on the Surface of Calcite in the Presence of High Co2+ Concentration

Abstract

The interaction of the calcite surface with Co2+-rich aqueous solutions ([Co2+aq]initial = 1000 ppm, i.e., ca. 17 mM) was investigated by means of macroscopic experiments and surface spectroscopic techniques. In the case of the macroscopic experiments, calcite powder and monocrystals were immersed into solutions for different time periods (from 1 min to one month). The Ca concentrations in the filtrates was measured by means of atomic absorption spectrometry (AAS) while the interacted solids were studied using a combination of X-ray photoelectron spectroscopy (XPS) and 12C-rutherford backscattering spectrometry (12C-RBS). The macroscopic data showed a characteristic surface dissolution process, in parallel to the surface sorption processes. Adsorption and co-precipitation were seen for almost the entire immersion period for both calcite powder and monocrystals. The surface study by XPS (analyzed at a depth of approximately 12 nm) suggested that adsorption takes place in the first hour of the interaction, followed by incorporation of Co2+ into calcite surface layers, leading to the formation of a Co2+-bearing surface (co)precipitate, which occurs over a period of hours and days. The 12C-RBS measurements on calcite { 10 1 ¯ 4 } indicated that the thickness of this surface co-precipitate was 270 nm after one day and then stabilized at 320 nm after more than a week.

Keywords

• calcite
• surface
• cobalt
• dissolution
• adsorption
• surface co-precipitation
• photoelectron spectroscopy
• Rutherford backscattering