Silicate Carbonation in Supercritical CO2 Containing Dissolved H2O: An in situ High Pressure X-Ray Diffraction and Infrared Spectroscopy Study

Schaef, H. Todd; Miller, Quin R. S.; Cj, Thompson; Loring, John S.; Bowden, M. D.; Arey, B. W.; McGrail, B. Peter; Rosso, K. M.

doi:10.1016/j.egypro.2013.06.514

Cited by 16 publications

(21 citation statements)

References 5 publications

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“…These results indicate that nesquehonite is a metastable precursor to magnesite, exemplified in the reactions: and which illustrates the precipitation of nesquehonite and amorphous silica, followed by the conversion of nesquehonite to magnesite. This is consistent with work that demonstrates magnesite is the most thermodynamically stable magnesium carbonate phase at 50 °C [39,51,52] and hydrated carbonate phases are metastable precursors [25,41,53]. The coupled forsterite dissolution and carbonate precipitation reactions likely occurred in nanometer-sized thin water films on the forsterite surface.…”

Section: H 2 O Control Hxrd Experiments (Exp 1 and Exp 2)supporting

confidence: 87%

Experimental Study of Organic Ligand Transport in Supercritical CO2 Fluids and Impacts to Silicate Reactivity

et al. 2014

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The interactions between water-saturated supercritical carbon dioxide, organics, and minerals are relatively unknown despite being important to carbon sequestration and enhanced hydrocarbon recovery activities. The goals of this study include verification of organic transport through scCO 2 and exploration of whether organic ligands can impact carbonate formation. An in situ near-infrared spectroscopic technique was used to probe supercritical CO 2 (scCO 2 )-organic mixtures at 35 °C and 100 bar. Observation of C-H bands in the spectra collected from scCO 2 equilibrated with a Ca-acetate solution (1.7 m) provided direct evidence of organic partitioning into the scCO 2 phase. A series of high pressure X-ray diffraction experiments at 50 °C and 90 bar were performed to investigate how citrate (0.01-0.5 m) affected the coupled dissolution of forsterite and precipitation of magnesium carbonates in scCO 2 . In control experiments where no citrate was present, nesquehonite (MgCO 3 •3H 2 O) was initially produced as a metastable intermediate that was then converted to magnesite (MgCO 3 ). However, experiments with citrate promoted magnesite, rather than nesquehonite, precipitation, and at the highest concentrations reduced the extent of the carbonation reaction. This paper discusses these unique findings on organic and scCO 2 interactions that are not currently being considered in the fate and transport of CO 2 in the subsurface.

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Section: H 2 O Control Hxrd Experiments (Exp 1 and Exp 2)supporting

confidence: 87%

Experimental Study of Organic Ligand Transport in Supercritical CO2 Fluids and Impacts to Silicate Reactivity

et al. 2014

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“…Two of the low-temperature (<150 °C) studies , shown in Figure A examined carbonation when olivine was exposed to H 2 O-saturated scCO 2 (wet scCO 2 ), a non-aqueous reactive phase . Dissolution and carbonate precipitation in wet scCO 2 are facilitated by the formation of angstrom- to nanometer-scale water films on hydrophilic mineral surfaces. ,,, Work in this area, including studies of olivine carbonation, ,,,,,,,,− has revealed unique reaction mechanisms and pathways for mineral carbonation that cannot be attained in aqueous media. For instance, the properties of Si-rich surface precipitates on carbonating silicates in wet scCO 2 are distinct from those that develop in aqueous experiments, and their development is remarkably sensitive to pressure–temperature conditions of the CO 2 . ,− Also, critical water film thicknesses are required for continuous coupled dissolution and precipitation. ,, Lastly, nucleation and growth of magnesite at low temperatures (≲65 °C) is promoted in wet scCO 2 , ,, likely due to the reduced level of hydration of Mg 2+ in nanoscale interfacial water films. , …”

Section: Knowledge Gaps and Research Frontiersmentioning

confidence: 99%

“…Red plotted points denote the P – T conditions of compiled studies that evaluated interactions of minerals, rocks, cement, or steel with water-bearing scCO 2 . Blue points denote wet scCO 2 experiments conducted with olivine. ,,,,,,− Dashed drop-down lines are a visual reference for interpreting the location of the points in three-dimensional space, and they illustrate the full range of solubility of water in CO 2 for the specified P – T conditions. (B) Phase relationships of CO 2 and H 2 O determined experimentally by Takenouchi and Kennedy .…”

Section: Knowledge Gaps and Research Frontiersmentioning

confidence: 99%

Quantitative Review of Olivine Carbonation Kinetics: Reactivity Trends, Mechanistic Insights, and Research Frontiers

Miller

Schaef

Kaszuba

et al. 2019

Environ. Sci. Technol. Lett.

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Magnesium-dominant olivine (Mg2SiO4) has received considerable attention for geologic and ex situ carbon mineralization due to its reaction potential with CO2 and its abundance in mafic and ultramafic rocks. To enable better predictions and optimization of its carbonation rate, here we compile the results of 15 separate studies into an internally consistent kinetic framework. Time-dependent transformation curves were determined, analyzed, and used to calculate temperature-dependent carbonation rate constants between 50 and 300 °C. The unified results clearly show that olivine carbonation is optimized at 185–200 °C and indicate a change in the carbonation reaction mechanism above 90 °C. Additional outcomes include the identification of important knowledge gaps and research frontiers for carbon mineralization, including those related to unraveling competitive serpentinization reactions, H2O-saturated supercritical CO2 (wet scCO2) reactivity, and the formation and impacts of secondary surface coatings. In addition to supporting the deployment of carbon storage technologies in a climate-responding world, the findings may help improve understanding of how carbonation and serpentinization processes influence critical geochemical cycles.

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“…We also note that interactions with surface groups are highly responsible for the formation of these species and that probing clay edge site chemistry is a growing challenge in the community given the importance of these interactions. were targeted host rocks for geological storage [251][252][253][254][255][256]. The interest in phyllosilicates [101,248,257,258], especially expandable clays, was also motivated by their ability to intercalate and thus lock CO 2 species into their bulk structure.…”

Section: Sulfidesmentioning

confidence: 99%

Surface chemistry of carbon dioxide revisited

Taifan

Boily

Baltrušaitis

2016

Surface Science Reports

145

129

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This review discusses modern developments in CO 2 surface chemistry by focusing on the work published since the original review by H. J. Freund and M.W. Roberts two decades ago (Surface Science Reports 25 (1996) 225-273). It includes relevant fundamentals pertaining to the topics covered in that earlier review, such as conventional metal and metal oxide surfaces and CO 2 interactions thereon. While UHV spectroscopy has routinely been applied for CO 2 gas-solid interface analysis, the present work goes further by describing surface-CO 2 interactions under elevated CO 2 pressure on non-oxide surfaces, such as zeolites, sulfides, carbides and nitrides. Furthermore, it describes salient in situ techniques relevant to the resolution of the interfacial chemistry of CO 2 , notably infrared spectroscopy and state-of-the-art theoretical methods, currently used in the resolution of solid and soluble carbonate species in liquid-water vapor, liquid-solid and liquid-liquid interfaces. These techniques are directly relevant to fundamental, natural and technological settings, such as heterogeneous and environmental catalysis and CO 2 sequestration.

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Silicate Carbonation in Supercritical CO2 Containing Dissolved H2O: An in situ High Pressure X-Ray Diffraction and Infrared Spectroscopy Study

Cited by 16 publications

References 5 publications

Experimental Study of Organic Ligand Transport in Supercritical CO2 Fluids and Impacts to Silicate Reactivity

Experimental Study of Organic Ligand Transport in Supercritical CO2 Fluids and Impacts to Silicate Reactivity

Quantitative Review of Olivine Carbonation Kinetics: Reactivity Trends, Mechanistic Insights, and Research Frontiers

Surface chemistry of carbon dioxide revisited

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