Research on carbon capture and storage has been focused on CO 2 storage in geologic formations, with many potential risks. An alternative to conventional geologic storage is carbon mineralization, where CO 2 is reacted with metal cations to form carbonate minerals. Mineralization methods can be broadly divided into two categories: in situ and ex situ. In situ mineralization, or mineral trapping, is a component of underground geologic sequestration, in which a portion of the injected CO 2 reacts with alkaline rock present in the target formation to form solid carbonate species. In ex situ mineralization, the carbonation reaction occurs above ground, within a separate reactor or industrial process. This literature review is meant to provide an update on the current status of research on CO 2 mineralization.

Geological sequestration of CO2, whether by enhanced oil recovery (EOR), coal-bed methane (CBM) recovery, or saline aquifer injection is a promising near-term sequestration methodology. While tremendous experience exists for EOR, and CBM recovery has been demonstrated in existing fields, saline aquifer injection studies have only recently been initiated. Studies evaluating the availability of saline aquifers suitable for CO2 injection show great potential, however, the long-term fate of the CO2 injected into these ancient aqueous systems is still uncertain. For the subject study, a series of laboratory-scale CO2 flood tests were conducted on whole core samples of the Mt. Simon sandstone from the Illinois Basin. By conducting these tests on whole core samples rather than crushed core, an evaluation of the impact of the CO2 flood on the rock mechanics properties as well as the geochemistry of the core and brine solution has been possible. This empirical data could provide a valuable resource for the validation of reservoir models under development for these engineered CO2 systems.

The Albany Research Center (ARC) conducted studies of mechanical activation by conventional and ultra fine grinding techniques to enhance olivine reactivity in mineral carbonation reactions. Activated olivine is one of several solid feed materials used at ARC in reactions with carbon dioxide to form carbonate minerals. This paper compares grinding techniques via energy demand data and product characteristics, including particle size distributions, surface areas, full-width-at-half-maximum (FWHM) XRD analyses, and particle morphology by SEM analyses, Reactivity was calculated by percent conversion to carbonate in subsequent carbonation tests. Particle size reduction has the greatest impact on reactivity, and wet grinding is more energy efficient than dry grinding. Large additional inputs of energy to increase surface area or reduce crystallinity do not result in proportional improvements in reactivity.

Carbonation of magnesium- and calcium-silicate minerals to form their respective carbonates is one method to sequester carbon dioxide. Process development studies have identified reactor design as a key component affecting both the capital and operating costs of ex-situ mineral sequestration. Results from mineral carbonation studies conducted in a batch autoclave were utilized to design and construct a unique continuous pipe reactor with 100% recycle (flow-loop reactor). Results from the flow-loop reactor are consistent with batch autoclave tests, and are being used to derive engineering data necessary to design a bench-scale continuous pipeline reactor.

Due to the scale and breadth of carbon dioxide emissions, and speculation regarding their impact on global climate, sequestration of some portion of these emissions has been under increased study. A practical approach to carbon sequestration will likely include several options, which will be driven largely by the energy demand and economics of operation. Aqueous mineral carbonation of calcium and magnesium silicate minerals has been studied as one potential method to sequester carbon dioxide. Although these carbonation reactions are all thermodynamically favored, they occur at geologic rates of reaction. Laboratory studies have demonstrated that these rates of reaction are accelerated with increasing temperature, pressure, and particle surface area. Mineral-specific activation methods were identified, however, each of these techniques incurs energy as well as economic costs. An overview of the mineral availability, pretreatment options and energy demands, and process economics is provided.

Sequestration of carbon as a stable mineral carbonate has been proposed to mitigate environmental concerns that carbon dioxide may with time escape from its sequestered matrix using alternative sequestration technologies. A method has been developed to prepare stable carbonate products by reacting CO2 with magnesium silicate minerals in aqueous bicarbonate/chloride media at high temperature and pressure. Because this approach is inherently expensive due to slow reaction rates and high capital costs, studies were conducted to improve the reaction rates through mineral pretreatment steps and to cut expenses through improved reactor technology. An overview is given for the estimated cost of the process including sensitivity to grinding and heating as pretreatment options for several mineral feedstocks. The energy costs are evaluated for each pretreatment in terms of net carbon avoided. New studies with a high-temperature, high-pressure flow-loop reactor have yielded information on overcoming kinetic barriers experienced with processing in stirred autoclave reactors. Repeated tests with the flow-loop reactor have yielded insights on wear and failure of system components, on challenges to maintain and measure flow, and for better understanding of the reaction mechanism.

Direct mineral carbonation was investigated as a process to convert gaseous CO2 into a geologically stable final form. The process utilizes a slurry of water, with bicarbonate and salt additions, mixed with a mineral reactant, such as olivine (Mg2SiO4) or serpentine [Mg3Si2O5(OH)4]. Carbon dioxide is dissolved into this slurry, resulting in dissolution of the mineral and precipitation of magnesium carbonate (MgCO3). Optimum results were achieved using heat-pretreated serpentine feed material and a high partial pressure of CO2 (PCO2). Specific conditions include 155°C, PCO2 = 185 atm and 15% solids. Under these conditions, a 78% conversion of the silicate to the carbonate was achieved in 30 minutes. Process mineralogy was utilized to investigate the appropriate feed characteristics, identify the process products and interpret the mineral dissolution and carbonate precipitation reaction paths.

Direct aqueous mineral carbonation has been investigated as a process to convert gaseous CO2 into a geologically stable, solid final form. The process utilizes a solution of sodium bicarbonate (NaHCO3), sodium chloride (NaCl), and water, mixed with a mineral reactant, such as olivine (Mg2SiO4) or serpentine [Mg3Si2O5(OH)4]. Carbon dioxide is dissolved into this slurry, by diffusion through the surface and gas dispersion within the aqueous phase. The process includes dissolution of the mineral and precipitation of the magnesium carbonate mineral magnesite (MgCO3) in a single unit operation. Activation of the silicate minerals has been achieved by thermal and mechanical means, resulting in up to 80% stoichiometric conversion of the silicate to the carbonate within 30 minutes. Heat treatment of the serpentine, or attrition grinding of the olivine and/or serpentine, appear to activate the minerals by the generation of a non-crystalline phase. Successful conversion to the carbonate has been demonstrated at ambient temperature and relatively low (10 atm) partial pressure of CO2 (PCO2). However, optimum results have been achieved using the bicarbonate-bearing solution, and high PCO2. Specific conditions include: 185°C; PCO2=150 atm; 30% solids. Studies suggest that the mineral dissolution rate is not solely surface controlled, while the carbonate precipitation rate is primarily dependent on the bicarbonate concentration of the slurry. Current and future activities include further examination of the reaction pathways and pretreatment options, the development of a continuous flow reactor, and an evaluation of the economic feasibility of the process.

Direct mineral carbonation has been investigated as a process to convert gaseous CO2 into a geologically stable, solid final form. The process utilizes a solution of sodium bicarbonate (NaHCO3), sodium chloride (NaCl), and water, mixed with a mineral reactant, such as olivine (Mg2SiO4) or serpentine [Mg3Si2O5(OH)4]. Carbon dioxide is dissolved into this slurry, by diffusion through the surface and gas dispersion within the aqueous phase. The process includes dissolution of the mineral and precipitation of magnesium carbonate (MgCO3) in a single unit operation. Optimum results have been achieved using heat pretreated serpentine feed material, with a surface area of roughly 19 m2 per gram, and high partial pressure of CO2 (PCO2). Specific conditions include: 155?C; PCO2=185 atm; 15% solids. Under these conditions, 78% stoichiometric conversion of the silicate to the carbonate was achieved in 30 minutes. Studies suggest that the mineral dissolution rate is primarily surface controlled, while the carbonate precipitation rate is primarily dependent on the bicarbonate concentration of the slurry. Current studies include further examination of the reaction pathways, and an evaluation of the resource potential for the magnesium silicate reactant, particularly olivine. Additional studies include the examination of various pretreatment options, the development of a continuous flowmore » reactor, and an evaluation of the economic feasibility of the process.« less