GSA Annual Meeting in Denver, Colorado, USA - 2016

Paper No. 119-4
Presentation Time: 2:15 PM

DEPTH DEPENDENT CO2-INDUCED ELEMENTAL MOBILIZATION FROM CARBONATE-RICH ROCKS USING FIELD-RELEVANT PRESSURE AND TEMPERATURE


LAWTER, Amanda R.1, QAFOKU, Nik1, ASMUSSEN, R. Matthew1, KUKKADAPU, Ravi K.2, QAFOKU, Odeta3, BACON, Diana4 and BROWN, Christopher1, (1)Geosciences, Pacific Northwest National Laboratory, 902 Battelle Blvd, P7-54, Richland, WA 99352, (2)Environmental Molecular Sciences Laboratory, 3335 Innovation Boulevard, Richland, WA 99354, (3)Fundamental and Computational Science, Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, WA 99354, (4)Pacific Northwest National Laboratory, 902 Battelle Blvd, P7-54, Richland, WA 99352, amanda.lawter@pnnl.gov

In the past decade, many studies have been conducted to determine changes within the reservoir following CO2 injection as well as effects of CO2 release into overlying groundwater aquifers. There is little or no literature available, however, on the effect of CO2 release on rock between the storage reservoir and the subsurface. To fill this current knowledge gap, this study used relevant rock materials, temperatures and pressures to study solid phase mineralogical changes and measure elements released into or removed from the aqueous phase through mineral dissolution or mineral precipitation. Using a NaCl background solution to represent reservoir brine, and depth dependent pressures ranging from 3,800-14,000 kPa and temperatures from 50-61°C, rocks samples (either <212 µm or larger rock chips) were reacted for 7 days. The liquid samples were then analyzed with IC, ICP-OES and ICP-MS, and the solids were analyzed with SEM/EDS, QXRD, and Mössbauer spectroscopy. A significant increase of major elements (e.g., Ca, Mg, Si, Mn, K) and variable releases of potential contaminants (e.g., Sr, S, Ba, Cs, B, Cu, and Cr) were observed in the liquid phase from CO2 experiments; lower concentrations of these elements were observed in the N2 experiments. SEM and Mössbauer spectroscopy results showed the formation of new minerals and Fe oxides in some CO2-reacted samples. This has important implications for contaminant removal from the aqueous phase due to potential incorporation into precipitated minerals or the strong adsorption properties of Fe oxides. The rock chemistry (determined with extractions), and the mineralogical and physical (particle size) properties were the major controlling factors for elemental release; each of these properties, as well as the calculated pressure and temperature for each experiment are, in some extent, related to the depth of the samples. These experiments show the interactions between the CO2-rich brine and the rock between deep storage reservoirs and overlying groundwater aquifers have the potential to affect the level of risk to overlying groundwater resources, and should be considered during site selection and risk evaluation.