• Journal of the Korean Society for Marine Environment & Energy
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• v.19 no.1
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• pp.18-24
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• 2016

Mineral carbonation is a technology for permanently storing carbon dioxide by reacting with metal oxides containing calcium and magnesium. In this study, we used sea water and alkaline industrial by-product such as paper sludge ash (PSA) for the storage of carbon dioxide through direct carbonation. We found the optimum conditions of both sea water content (mixing ratio of sea water and PSA) and reaction time required in the direct carbonation through various experiments using sea water and PSA. In addition, we compared the amounts of carbon dioxide storage with the cases when sea water and ultra-pure water were separately used as solvents in the direct carbonation with PSA. The amount of carbon dioxide storage was calculated by using both solid weight increase through the carbonation reaction and the contents of carbonate salts from thermal gravimetric analysis. PSA particle used in this study contained 67.2% of calcium. The optimum sea water content and reaction time in the carbonation reaction using sea water and PSA were 5 mL/g and 2 hours, respectively, under the conditions of 0.05 L/min flow rate of carbon dioxide injected at $25^{\circ}C$ and 1 atm. The amounts of carbon dioxide stored when sea water and ultra-pure water were separately used as solvents in the direct carbonation with PSA were 113 and $101kg\;CO_2/(ton\;PSA)$, respectively. The solid obtained through the carbonation reaction using sea water and PSA was composed of mainly calcium carbonate in the form of calcite and a small amount of magnesium carbonate. The solid obtained by using ultra-pure water, also, was found to be carbonate salt in the form of calcite.

• Proceedings of the Korean Institute of Building Construction Conference
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• 2017.05a
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• pp.13-14
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• 2017

In this paper, research for use possibility as silica source of waste concrete powder discharged from direct and indirect carbonation has progressed. For the research, properties on the extruding panel using waste concrete powder with high silica content is evaluated. As the results, compressive strength of specimen is increased 24% compared to control specimen when waste concrete powder replaced 50%, that is discharged from carbonation process, as silica source.

• Journal of the Mineralogical Society of Korea
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• v.27 no.1
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• pp.17-30
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• 2014

Waste cement generated from recycling processes of waste concrete is a potential raw material for mineral carbonation. For the $CO_2$ sequestration utilizing waste cement, this study was conducted to obtain basic information on the aqueous carbonation methods and the characteristics of carbonate mineral formation. Cement paste was made with W:C= 6:4 and stored for 28 days in water bath. Leaching tests using two additives (NaCl and $MgCl_2$) and two aqueous carbonation experiments (direct and indirect aqueous carbonation) were conducted. The maximum leaching of $Ca^{2+}$ ion was occurred at 1.0 M NaCl and 0.5 M $MgCl_2$ solution rather than higher tested concentration. The concentration of extracted $Ca^{2+}$ ion in $MgCl_2$ solution was more than 10 times greater than in NaCl solution. Portlandite ($Ca(OH)_2$) was completely changed to carbonate minerals in the fine cement paste (< 0.15 mm) within one hour and the carbonation of CSH (calcium silicate hydrate) was also progressed by direct aqueous carbonation method. The both additives, however, were not highly effective in direct aqueous carbonation method. 100% pure calcite minerals were formed by indirect carbonation method with NaCl and $MgCl_2$ additives. pH control using alkaline solution was important for the carbonation in the leaching solution produced from $MgCl_2$ additive and carbonation rate was slow due to the effect of $Mg^{2+}$ ions in solution. The type and crystallinity of calcium carbonate mineral were affected by aqueous carbonation method and additive type.

• Economic and Environmental Geology
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• v.50 no.1
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• pp.27-34
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• 2017

Mineral carbonation for the storage of carbon dioxide is a CCS option that provides an alternative for the more widely advocated method of geological storage in underground formation. Carbonation of magnesium- or calcium-based minerals, especially the carbonation of waste materials and industrial by-products is expanding, even though total amounts of the industrial waste are too small to substantially reduce the $CO_2$ emissions. The mineral carbonation was performed with steelmaking reduction slag as starting material. The steelmaking reduction slag dissolution experiments were conducted in the $H_2SO_4$ and $NH_4NO_3$ solution with concentration range of 0.3 to 1 M at $100^{\circ}C$ and $150^{\circ}C$. The hydrothermal treatment was performed to the starting material via a modified direct aqueous carbonation process at the same leaching temperature. The initial pH of the solution was adjusted to 12 and $CO_2$ partial pressure was 1MPa for the carbonation. The carbonation rate after extracting $Ca^^{2+}$ under $NH_4NO_3$ was higher than that under $H_2SO_4$ and the carbonation rates in 1M $NH_4NO_3$ solution at $150^{\circ}C$ was dramatically enhanced about 93%. In this condition well-faceted rhombohedral calcite, and rod or flower-shaped aragonite were appeared together in products. As the concentration of $H_2SO_4$ increased, the formation of gypsum was predominant and the carbonation rate decreased sharply. Therefore it is considered that the selection of the leaching solution which does not affect the starting material is important in the carbonation reaction.

• Journal of Korean Society of Environmental Engineers
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• v.36 no.5
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• pp.342-351
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• 2014

The present paper investigates the performance of direct wet mineral carbonation technology to fix carbon dioxide ($CO_2$) from relatively high $CO_2$ concentration feeding gas using wollastonite ($CaSiO_3$)-water (and 0.46 M acetic acid) suspension solution. To minimize the energy consumed on the process, the carbonation in this work is carried out at atmospheric pressure and slightly higher room temperature. As a result, carbon fixation is confirmed on the surface of $CaSiO_3$ after carbonation with wollastonite-water suspension solution and its amount is increased according to the $CO_2$ composition in the feeding gas. The leaching and carbonation ratio of wollastonite-water suspension system obtained from the carbonation with 50% of $CO_2$ composition feeding gas is 13.2% and 10.4%, respectively. On the other hand, the performance of wollastonite-acetic acid in the same condition is 63% for leaching and 1.39% for carbonation.

• Journal of the Mineralogical Society of Korea
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• v.28 no.1
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• pp.39-49
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• 2015

Recently, carbon capture and storage (CCS) techniques have been globally studied. This study was conducted to use waste cement powder as an efficient raw material of mineral carbonation for $CO_2$ sequestration. Direct aqueous carbonation experiment was conducted with injecting pure $CO_2$ gas (99.9%) to a reactor containing $200m{\ell}$ reacting solution and the pulverized cement paste (W:C = 6:4) having particle size less than 0.15 mm. The effects of two additives (NaCl, $MgCl_2$) in carbonation were analyzed. The characteristics of carbonate minerals and carbonation process according to the type of additives and pH change were carefully evaluated. pH of reacting solution was gradually decreased with injecting $CO_2$ gas. $Ca^{2+}$ ion concentration in $MgCl_2$ containing solution was continuously decreased. In none $MgCl_2$ solution, however, $Ca^{2+}$ ion concentration was increased again as pH decreased. This is probably due to the dissolution of newly formed carbonate mineral in low pH solution. XRD analysis indicates that calcite is dominant carbonate mineral in none $MgCl_2$ solution whereas aragonite is dominant in $MgCl_2$ containing solution. Unstable vaterite formed in early stage of experiment was transformed to well crystallized calcite with decreasing pH in the absence of $MgCl_2$ additives. In the presence of $MgCl_2$ additives, the content of aragonite was increased with decreasing pH whereas the content of calite was decreased.

• Economic and Environmental Geology
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• v.53 no.1
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• pp.1-9
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• 2020

Magnesium silicate minerals such as serpentine [Mg₃Si₂O₅(OH)₄] have a high potential for the sequestration of CO₂; thus, their reactivity toward dissolution under CO₂-free and CO₂-containing conditions in acidic solvents is a critical process with respect to their carbonation reactions. To examine the carbonation efficiency and dissolution mechanism of serpentine, hydrothermal treatment was performed to the starting material via a modified direct aqueous carbonation process at 100 and 150℃. The serpentine dissolution experiments were conducted in H₂SO₄ solution with concentration range of 0.3-1 M and at a CO₂ partial pressure of 3 MPa. The initial pH of the solution was adjusted to 13 for the carbonation process. Under CO₂-free and CO₂-containing conditions, the carbonation efficiency increased in proportion to the concentration of H₂SO₄ and the reaction temperature. The leaching rate under CO₂-containing conditions was higher than that under CO₂-free conditions. This suggests that shows the presence of CO₂ affects the carbonation reaction. The leaching and carbonation efficiencies at 150℃ in 1 M H₂SO₄ solution under CO₂-containing conditions were 85 and 84%, respectively. The dissolution rate of Mg was higher than that of Si, such that the Mg : Si ratio of the reacted serpentine decreased from the inner part (approximately 1.5) to the outer part (less than 0.1). The resultant silica-rich layer of the reaction product ultimately changed through the Mg-depleted skeletal phase and the pseudo-serpentine phase to the amorphous silica phase. A passivating silica layer was not observed on the outer surface of the reacted serpentine.

• Economic and Environmental Geology
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• v.55 no.4
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• pp.377-388
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• 2022

Laboratory-scale experiments were performed to identify the As removal mechanism of the residual slag generated after the mineral carbonation process. The residual slags were manufactured from the steelmaking slag (blast oxygen furnace slag: BOF) through direct and indirect carbonation process. RDBOF (residual BOF after the direct carbonation) and RIBOF (residual BOF after the indirect carbonation) showed different physicochemical-structural characteristics compared with raw BOF such as chemical-mineralogical properties, the pH level of leachate and forming micropores on the surface of the slag. In batch experiment, 0.1 g of residual slag was added to 10 mL of As-solution (initial concentration: 203.6 mg/L) titrated at various pH levels. The RDBOF showed 99.3% of As removal efficiency at initial pH 1, while it sharply decreased with the increase of initial pH. As the initial pH of solution decreased, the dissolution of carbonate minerals covering the surface was accelerated, increasing the exposed area of Fe-oxide and promoting the adsorption of As-oxyanions on the RDBOF surface. Whereas, the As removal efficiency of RIBOF increased with the increase of initial pH levels, and it reached up to 70% at initial pH 10. Considering the PZC (point of zero charge) of the RIBOF (pH 4.5), it was hardly expected that the electrical adsorption of As-oxyanion on surface of the RIBOF at initial pH of 4-10. Nevertheless it was observed that As-oxyanion was linked to the Fe-oxide on the RIBOF surface by the cation bridge effect of divalent cations such as Ca²⁺, Mn²⁺, and Fe²⁺. The surface of RIBOF became stronger negatively charged, the cation bridge effect was more strictly enforced, and more As can be fixed on the RIBOF surface. However, the Ca-products start to precipitate on the surface at pH 10-11 or higher and they even prevent the surface adsorption of As-oxyanion by Fe-oxide. The TCLP test was performed to evaluate the stability of As fixed on the surface of the residual slag after the batch experiment. Results supported that RDBOF and RIBOF firmly fixed As over the wide pH levels, by considering their As desorption rate of less than 2%. From the results of this study, it was proved that both residual slags can be used as an eco-friendly and low-cost As remover with high As removal efficiency and high stability and they also overcome the pH increase in solution, which is the disadvantage of existing steelmaking slag as an As remover.

• Journal of the Korean Crystal Growth and Crystal Technology
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• v.34 no.3
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• pp.86-91
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• 2024

In this study, the characteristics of mortar using carbondioxide conversion capture materials (CCMs), fabricated by reacting CO₂ with desulfurization gypsum (DG) by-produced from a oil refinery, as a cement mixture. Based on the chemical component and particle size analysis results, it estimated that desulfurized gypsum reacted with carbon dioxide to produce carbonate crystals such as CaCO₃. Using CCMs as a cement mixture, physical property and durability analysis were conducted by measuring such as workability, compressive strength, compressive strength ratio after freezing-thawing and accelerated carbonation depth. The experimental results showed that as the content of the admixture increased, workability and compressive strength characteristics decreased. Compressive strength after freezing-thawing and accelerated carbonation depth also showed similar characteristics to the physical property measurement results. In addition, compared to desulfurized gypsum, using CCMs showed better physical properties and durability. This was assumed to be due to differences in the crystal phases of the mixed materials such as free-CaO and CaCO₃.