Insights into silicate carbonation processes in water-bearing supercritical CO2 fluids

[Display omitted] ► Pressurized XRD tracked carbonation of wollastonite in wet supercritical CO2. ► Thin water films formed on the wollastonite surface during exposure to wet supercritical CO2. ► Hydrated amorphous calcium carbonate was identified as a reaction product. Subsurface injection of CO2 i...

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Published in:International journal of greenhouse gas control Vol. 15; pp. 104 - 118
Main Authors: Miller, Q.R.S., Thompson, C.J., Loring, J.S., Windisch, C.F., Bowden, M.E., Hoyt, D.W., Hu, J.Z., Arey, B.W., Rosso, K.M., Schaef, H.T.
Format: Journal Article
Language:English
Published: Elsevier Ltd 01-07-2013
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Abstract [Display omitted] ► Pressurized XRD tracked carbonation of wollastonite in wet supercritical CO2. ► Thin water films formed on the wollastonite surface during exposure to wet supercritical CO2. ► Hydrated amorphous calcium carbonate was identified as a reaction product. Subsurface injection of CO2 is commonplace in certain industries, yet deployment at the scale required for emission reduction is unprecedented and therefore requires a high degree of predictability. Accurate modeling of subsurface geochemical processes related to geologic carbon sequestration requires experimentally derived data for mineral reactions. Most work in this area has focused on aqueous-dominated systems in which dissolved CO2 reacts to form crystalline carbonate minerals. Comparatively little laboratory research has been conducted on reactions occurring between minerals in the host rock and the wet supercritical fluid phase. We studied the carbonation of wollastonite [CaSiO3] exposed to variably hydrated supercritical CO2 (scCO2) at 50, 55 and 70°C and 90, 120 and 160bar. Reactions were followed by three novel in situ high pressure techniques, which demonstrated increased dissolved water concentrations in the scCO2 resulted in increased wollastonite carbonation approaching ∼50wt.%. Overall, the X-ray diffraction and infrared and magic angle nuclear magnetic resonance spectroscopies experiments conducted in this study allow detailed examination of mechanisms impacting carbonation rates. These include the development of amorphous passivating layers, thin liquid water films, and amorphous hydrated carbonate phases. Collectively, these results emphasize the importance of understanding geochemical processes occurring in wet scCO2 fluids.
AbstractList Subsurface injection of CO2 is commonplace in certain industries, yet deployment at the scale required for emission reduction is unprecedented and therefore requires a high degree of predictability. Accurate modeling of subsurface geochemical processes related to geologic carbon sequestration requires experimentally derived data for mineral reactions. Most work in this area has focused on aqueous-dominated systems in which dissolved CO2 reacts to form crystalline carbonate minerals. Comparatively little laboratory research has been conducted on reactions occurring between minerals in the host rock and the wet supercritical fluid phase. We studied the carbonation of wollastonite [CaSiO3] exposed to variably hydrated supercritical CO2 (scCO2) at 50, 55 and 70 degree C and 90, 120 and 160 bar. Reactions were followed by three novel in situ high pressure techniques, which demonstrated increased dissolved water concentrations in the scCO2 resulted in increased wollastonite carbonation approaching a1450 wt.%. Overall, the X-ray diffraction and infrared and magic angle nuclear magnetic resonance spectroscopies experiments conducted in this study allow detailed examination of mechanisms impacting carbonation rates. These include the development of amorphous passivating layers, thin liquid water films, and amorphous hydrated carbonate phases. Collectively, these results emphasize the importance of understanding geochemical processes occurring in wet scCO2 fluids.
[Display omitted] ► Pressurized XRD tracked carbonation of wollastonite in wet supercritical CO2. ► Thin water films formed on the wollastonite surface during exposure to wet supercritical CO2. ► Hydrated amorphous calcium carbonate was identified as a reaction product. Subsurface injection of CO2 is commonplace in certain industries, yet deployment at the scale required for emission reduction is unprecedented and therefore requires a high degree of predictability. Accurate modeling of subsurface geochemical processes related to geologic carbon sequestration requires experimentally derived data for mineral reactions. Most work in this area has focused on aqueous-dominated systems in which dissolved CO2 reacts to form crystalline carbonate minerals. Comparatively little laboratory research has been conducted on reactions occurring between minerals in the host rock and the wet supercritical fluid phase. We studied the carbonation of wollastonite [CaSiO3] exposed to variably hydrated supercritical CO2 (scCO2) at 50, 55 and 70°C and 90, 120 and 160bar. Reactions were followed by three novel in situ high pressure techniques, which demonstrated increased dissolved water concentrations in the scCO2 resulted in increased wollastonite carbonation approaching ∼50wt.%. Overall, the X-ray diffraction and infrared and magic angle nuclear magnetic resonance spectroscopies experiments conducted in this study allow detailed examination of mechanisms impacting carbonation rates. These include the development of amorphous passivating layers, thin liquid water films, and amorphous hydrated carbonate phases. Collectively, these results emphasize the importance of understanding geochemical processes occurring in wet scCO2 fluids.
Author Hu, J.Z.
Arey, B.W.
Miller, Q.R.S.
Bowden, M.E.
Rosso, K.M.
Windisch, C.F.
Schaef, H.T.
Thompson, C.J.
Hoyt, D.W.
Loring, J.S.
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  organization: Pacific Northwest National Laboratory, P. O. Box 999, MS K8-98, Richland, WA 99352, USA
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  givenname: J.S.
  surname: Loring
  fullname: Loring, J.S.
  organization: Pacific Northwest National Laboratory, P. O. Box 999, MS K8-98, Richland, WA 99352, USA
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  surname: Windisch
  fullname: Windisch, C.F.
  organization: Department of Chemistry and Physics, S. Holden Street, University of Central Missouri, Warrensburg, MO 64093, USA
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  givenname: M.E.
  surname: Bowden
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  givenname: D.W.
  surname: Hoyt
  fullname: Hoyt, D.W.
  organization: Pacific Northwest National Laboratory, P. O. Box 999, MS K8-98, Richland, WA 99352, USA
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  surname: Rosso
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  givenname: H.T.
  surname: Schaef
  fullname: Schaef, H.T.
  email: todd.schaef@pnnl.gov
  organization: Pacific Northwest National Laboratory, P. O. Box 999, MS K8-98, Richland, WA 99352, USA
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Snippet [Display omitted] ► Pressurized XRD tracked carbonation of wollastonite in wet supercritical CO2. ► Thin water films formed on the wollastonite surface during...
Subsurface injection of CO2 is commonplace in certain industries, yet deployment at the scale required for emission reduction is unprecedented and therefore...
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SubjectTerms Calcite
Carbon sequestration
Silicate carbonation
Supercritical CO2
Title Insights into silicate carbonation processes in water-bearing supercritical CO2 fluids
URI https://dx.doi.org/10.1016/j.ijggc.2013.02.005
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