Carbon dioxide sequestration by direct mineral carbonation with carbonic acid

O'Connor, William K.; Dahlin, David C.; Nilsen, David N.; Walters, Richard P.; Turner, Paul C.
USDOE - Office of Fossil Energy

The Albany Research Center (ARC) of the U.S. Dept. of Energy (DOE) has been conducting a series of mineral carbonation tests at its Albany, Oregon, facility over the past 2 years as part of a Mineral Carbonation Study Program within the DOE. Other participants in this Program include the Los Alamos National Laboratory, Arizona State University, Science Applications International Corporation, and the DOE National Energy Technology Laboratory. The ARC tests have focused on ex-situ mineral carbonation in an aqueous system. The process developed at ARC utilizes a slurry of water mixed with a magnesium silicate mineral, olivine [forsterite end member (Mg2SiO4)], or serpentine [Mg3Si2O5(OH)4]. This slurry is reacted with supercritical carbon dioxide (CO2) to produce magnesite (MgCO3). The CO2 is dissolved in water to form carbonic acid (H2CO3), which dissociates to H+ and HCO3 -. The H+ reacts with the mineral, liberating Mg2+ cations which react with the bicarbonate to form the solid carbonate. The process is designed to simulate the natural serpentinization reaction of ultramafic minerals, and for this reason, these results may also be applicable to in-situ geological sequestration regimes. Results of the baseline tests, conducted on ground products of the natural minerals, have been encouraging. Tests conducted at ambient temperature (22 C) and subcritical CO2 pressures (below 73 atm) resulted in very slow conversion to the carbonate. However, when elevated temperatures and pressures are utilized, coupled with continuous stirring of the slurry and gas dispersion within the water column, significant reaction occurs within much shorter reaction times. Extent of reaction, as measured by the stoichiometric conversion of the silicate mineral (olivine) to the carbonate, is roughly 90% within 24 hours, using distilled water, and a reaction temperature of 185?C and a partial pressure of CO2 (PCO2) of 115 atm. Recent tests using a bicarbonate solution, under identical reaction conditions, have achieved roughly 83% conversion of heat treated serpentine and 84% conversion of olivine to the carbonate in 6 hours. The results from the current studies suggest that reaction kinetics can be improved by pretreatment of the mineral, catalysis of the reaction, or some combination of the two. Future tests are intended to examine a broader pressure/temperature regime, various pretreatment options, as well as other mineral groups.