The reactive crystallization kinetics of hydromagnesite in the MgCl 2 −CO 2 −NH 3 −H 2 O system, which plays an important role in a new approach to sequester CO 2 with saline sea/lake brines, was systematically investigated by the MSMPR (mixed-suspension-mixed-product removal) crystallization method. The temperature effect on the crystallization of magnesium carbonate hydrates in the system was first investigated batchwise. The optimum temperature of 353.2 K for precipitation of the regular spherical hydromagnesite with good filterability was selected for kinetic study. The supersaturation of hydromagnesite was experimentally tested, and the activity coefficients of aqueous species were strictly calculated by the Pitzer model embedded in the Aspen Plus platform. The nucleation and growth rate and agglomeration kernel were determined by moments analysis based on the PSD (particle size distribution) of crystals in volume coordinates. The corresponding kinetic parameters in three empirical equations were then estimated by linear regression. The resulting volume growth rate order of 2.30 means that surface integration is dominant in the volume growth of hydromagnesite. A simplified process for the new sequestration approach was finally constructed. The value of hydromagnesite as carbonated product was assessed considering the scale-up and costs of such a process.
INTRODUCTIONThe rising level of CO 2 in the atmosphere, mainly resulting from the combustion of fossil fuels, and its deleterious impact on the climate continues to raise concerns. Since alternative energy sources are not likely to replace fossil fuels soon, and since the atmospheric concentration of CO 2 is expected to triple by the end of 21st century with the continued growth of emerging densely populated developing countries, it is necessary to develop effective methods of sequestering CO 2 . 1−3 Numerous approaches to CO 2 sequestration, including ocean, terrestrial, geological, chemical, and biological options, are currently being studied, and some commercial scale processes have been demonstrated. 1,3−12 However, the implementation of these methods is limited because of either their extensive energy cost or unsteady behavior of CO 2 . 10 Mineral sequestration via reaction of CO 2 with Mg−Ca silicate rocks in aqueous solutions 11,12 offers an attractive option for the permanent and safe storage of CO 2 in a solid form because the resulting neoformations are thermodynamically stable at ambient temperature. 13 This method, first proposed by Seifritz, 14 requires cations, i.e. Mg and Ca in silicates as olivine and serpentine-group minerals, to neutralize CO 2 through formation of carbonates. Unfortunately, the industrial extraction of Ca and Mg from silicate minerals requires expensiveprocessing, which contributes to the problem rather than to the solution. 15 Furthermore, this option is not at all practical in many countries owing to the paucity of exposed basic and ultrabasic rocks. 3 An attractive alternative involves the interaction of ions in aqueo...