DOE OSTI2013
The most effective mechanism to limit CO 2 release from underground Geologic Carbon Sequestration (GCS) sites over multi-century time scales will be to convert the CO 2 into solid carbonate minerals. This report describes the results from four independent research investigations on carbonate mineralization: 1) Colloidal calcite particles forming in Maramec Spring, Missouri, provide a natural analog to evaluate reactions that may occur in a leaking GCS site. The calcite crystals form as a result of physiochemical changes that occur as the spring water rises from a depth of more than 190'. The resultant pressure decrease induces a loss of CO 2 from the water, rise in pH, lowering of the solubility of Ca 2+ and CO 3 2- , and calcite precipitation. Equilibrium modelling of the spring water resulted in a calculated undersaturated state with respect to calcite. The discontinuity between the observed occurrence of calcite and the model result predicting undersaturated conditions can be explained if bicarbonate ions (HCO 3 - ) are directly involved in precipitation process rather than just carbonate ions (CO 3 2- ). 2) Sedimentary rocks in the Oronto Group of the Midcontinent Rift (MCR) system contain an abundance of labile Ca-, Mg-, and Fe-silicate minerals that will neutralize carbonic acid and provide alkaline earth ions for carbonate mineralization. One of the challenges in using MCR rocks for GCS results from their low porosity and permeability. Oronto Group samples were reacted with both CO 2 -saturated deionized water at 90°C, and a mildly acidic leachant solution in flow-through core-flooding reactor vessels at room temperature. Resulting leachate solutions often exceeded the saturation limit for calcite. Carbonate crystals were also detected in as little as six days of reaction with Oronto Group rocks at 90oC, as well as experiments with forsterite-olivine and augite, both being common minerals this sequence. The Oronto Group samples have poor reservoir rock characteristics, none ever exceeded a permeability value of 2.0 mD even after extensive dissolution of calcite cement during the experiments. The overlying Bayfield Group – Jacobsville Formation sandstones averaged 13.4 ± 4.3% porosity and a single sample tested by core-flooding revealed a permeability of ~340 mD. The high porosity-permeability characteristics of these sandstones will allow them to be used for GCS as a continuous aquifer unit with the overlying Mt. Simon Formation. 3) Anaerobic sulfate reducing bacteria (SRB) can enhance the conversion rate of CO 2 into solid minerals and thereby improve long-term storage. SRB accelerated carbonate mineralization reactions between pCO 2 values of 0.0059 and 14.7 psi. Hydrogen, lactate and formate served as suitable electron donors for SRB metabolism. The use of a 13 CO 2 spiked gas source also produced carbonate minerals with ~53% of the carbon being derived from the gas phase. The sulfate reducing activity of the microbial community was limited, however, at 20 psi pCO 2 and carbonate mineralization did not occur. Inhibition of bacterial metabolism may have resulted from the acidic conditions or CO 2 toxicity. 4) Microbialite communities forming in the high turbidity and hypersaline water of Storrs’ Lake, San Salvador Island, The Bahamas, were investigated for their distribution, mineralogy and microbial diversity. Molecular analysis of the organic mats on the microbialites indicate only a trace amount of cyanobacteria, while anaerobic and photosynthetic non-sulfur bacteria of the phyla Chloroflexi and purple sulfur bacteria of class Gammaproteobacteria were abundant.
54 ENVIRONMENTAL SCIENCES↗