ABSTRACT
Potential leakages of CO2 from storage sites to shallow aquifers could have adverse impacts on the quality of potable groundwater. The mineralogy of well-sorted silica sand is modified by the pH-controlled precipitation of eight metals (Cr, Mn, Fe, Co, Ni, Cu, Zn, Cd). Continuous flow tests are performed in two fixed-bed columns packed with the modified sand by coinjecting gas CO2/distilled water (2-phase column) and distilled water (1-phase column/control test) at constant influx rates for a period of two months. The concentration of dissolved metals is measured in the effluents of columns with atomic absorption spectroscopy (AAS). Mineralogical analysis of the surface of sand grains is done before and after the flow tests with scanning electron microscopy-X-ray energy dispersive spectroscopy (SEM-EDS) and X-ray photoelectron spectroscopy (XPS), whereas the precise quantitative measurement of the metal content in the sand is done with AAS. A dynamic numerical model that couples the flow and mass-transfer processes in porous media with the equilibrium and kinetically driven metal desorption processes is developed. Inverse modeling of the continuous flow test enables us to quantify and rank the selectivity of metal mobility in terms of equilibrium and kinetic desorption parameters. The continuous CO2 dissolution and water acidification causes significant mobilization and dissolution of several metals (Mn, Ni, Cu, Zn, Co), moderate mobilization of Cr, acceleration of Cd dissolution, whereas Fe remains strongly bonded on the sand grains as goethite. The parameters estimated from lab-scale column tests might be helpful for interpreting field-scale CO2 leakage scenarios and installing relevant early warning monitoring systems.
