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Title: GEOCHEMICAL ASPECTS OF THE CARBONATION OF MAGNESIUM SILICATES IN AN AQUEOUS MEDIUM

Abstract

No abstract prepared.

Authors:
;
Publication Date:
Research Org.:
Los Alamos National Lab., NM (US)
Sponsoring Org.:
US Department of Energy (US)
OSTI Identifier:
776170
Report Number(s):
LA-UR-01-1429
TRN: AH200137%%112
DOE Contract Number:
W-7405-ENG-36
Resource Type:
Conference
Resource Relation:
Conference: Conference title not supplied, Conference location not supplied, Conference dates not supplied; Other Information: PBD: 1 Mar 2001
Country of Publication:
United States
Language:
English
Subject:
29 ENERGY PLANNING, POLICY AND ECONOMY; MAGNESIUM SILICATES; CARBONATES; LANL

Citation Formats

G. GUTHRIE, and ET AL. GEOCHEMICAL ASPECTS OF THE CARBONATION OF MAGNESIUM SILICATES IN AN AQUEOUS MEDIUM. United States: N. p., 2001. Web.
G. GUTHRIE, & ET AL. GEOCHEMICAL ASPECTS OF THE CARBONATION OF MAGNESIUM SILICATES IN AN AQUEOUS MEDIUM. United States.
G. GUTHRIE, and ET AL. Thu . "GEOCHEMICAL ASPECTS OF THE CARBONATION OF MAGNESIUM SILICATES IN AN AQUEOUS MEDIUM". United States. doi:. https://www.osti.gov/servlets/purl/776170.
@article{osti_776170,
title = {GEOCHEMICAL ASPECTS OF THE CARBONATION OF MAGNESIUM SILICATES IN AN AQUEOUS MEDIUM},
author = {G. GUTHRIE and ET AL},
abstractNote = {No abstract prepared.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Thu Mar 01 00:00:00 EST 2001},
month = {Thu Mar 01 00:00:00 EST 2001}
}

Conference:
Other availability
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  • 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.
  • The dramatic increase in atmospheric carbon dioxide since the Industrial Revolution has caused concerns about global warming. Fossil-fuel-fired power plants contribute approximately one third of the total human-caused emissions of carbon dioxide. Increased efficiency of these power plants will have a large impact on carbon dioxide emissions, but additional measures will be needed to slow or stop the projected increase in the concentration of atmospheric carbon dioxide. By accelerating the naturally occurring carbonation of magnesium silicate minerals it is possible to sequester carbon dioxide in the geologically stable mineral magnesite (MgCO3). The carbonation of two classes of magnesium silicate minerals,more » olivine (Mg2SiO4) and serpentine (Mg3Si2O5(OH)4), was investigated in an aqueous process. The slow natural geologic process that converts both of these minerals to magnesite can be accelerated by increasing the surface area, increasing the activity of carbon dioxide in the solution, introducing imperfections into the crystal lattice by high-energy attrition grinding, and in the case of serpentine, by thermally activating the mineral by removing the chemically bound water. The effect of temperature is complex because it affects both the solubility of carbon dioxide and the rate of mineral dissolution in opposing fashions. Thus an optimum temperature for carbonation of olivine is approximately 185 degrees C and 155 degrees C for serpentine. This paper will elucidate the interaction of these variables and use kinetic studies to propose a process for the sequestration of the carbon dioxide.« less
  • Direct aqueous mineral carbonation has been investigated as a process to convert gaseous CO{sub 2} into a geologically stable, solid final form. The process utilizes a solution of sodium bicarbonate (NaHCO{sub 3}), sodium chloride (NaCl), and water, mixed with a mineral reactant, such as olivine (Mg{sub 2}SiO{sub 4}) or serpentine [Mg{sub 3}Si{sub 2}O{sub 5}(OH){sub 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 (MgCO{sub 3}) in a single unit operation. Activation of the silicatemore » 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 CO{sub 2} (P{sub CO2}). However, optimum results have been achieved using the bicarbonate-bearing solution, and high P{sub CO2}. Specific conditions include: 185 C; P{sub CO2}=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.« less
  • 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 acceleratedmore » 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.« less
  • Carbon dioxide sequestration by an ex-situ, direct aqueous mineral carbonation process has been investigated over the past two years. This process was conceived to minimize the steps in the conversion of gaseous CO2 to a stable solid. This meant combining two separate reactions, mineral dissolution and carbonate precipitation, into a single unit operation. It was recognized that the conditions favorable for one of these reactions could be detrimental to the other. However, the benefits for a combined aqueous process, in process efficiency and ultimately economics, justified the investigation. The process utilizes a slurry of water, dissolved CO2, and a magnesiummore » silicate mineral, such as olivine [forsterite end member (Mg2SiO4)], or serpentine [Mg3Si2O5(OH)4]. These minerals were selected as the reactants of choice for two reasons: (1) significant abundance in nature; and (2) high molar ratio of the alkaline earth oxides (CaO, MgO) within the minerals. Because it is the alkaline earth oxide that combines with CO2 to form the solid carbonate, those minerals with the highest ratio of these oxides are most favored. Optimum results have been achieved using heat pretreated serpentine feed material, sodium bicarbonate and sodium chloride additions to the solution, and high partial pressure of CO2 (PCO2). Specific conditions include: 155?C; PCO2=185 atm; 15% solids. Under these conditions, 78% conversion of the silicate to the carbonate was achieved in 30 minutes. Future studies are intended to investigate various mineral pretreatment options, the carbonation solution characteristics, alternative reactants, scale-up to a continuous process, geochemical modeling, and process economics.« less