Mechanisms of aqueous wollastonite carbonation as a possible CO2 sequestration process

W.J.J. Huijgen, G.J. Witkamp, R.N.J. Comans

Research output: Contribution to journalArticleAcademicpeer-review

186 Citations (Scopus)

Abstract

The mechanisms of aqueous wollastonite carbonation as a possible carbon dioxide sequestration process were investigated experimentally by systematic variation of the reaction temperature, CO2 pressure, particle size, reaction time, liquid to solid ratio and agitation power. The carbonation reaction was observed to occur via the aqueous phase in two steps: (1) Ca leaching from the CaSiO3 matrix and (2) CaCO3 nucleation and growth. Leaching is hindered by a Ca-depleted silicate rim resulting from incongruent Ca-dissolution. Two temperature regimes were identified in the overall carbonation process. At temperatures below an optimum reaction temperature, the overall reaction rate is probably limited by the leaching rate of Ca. At higher temperatures, nucleation and growth of calcium carbonate are probably limiting the conversion, due to a reduced (bi)carbonate activity. The mechanisms for the aqueous carbonation of wollastonite were shown to be similar to those reported previously for an industrial residue and a Mg-silicate. The carbonation of wollastonite proceeds rapidly relative to Mg¿silicates, with a maximum conversion in 15 min of 70% at , 20 bar CO2 partial pressure and particle size of . The obtained insight in the reaction mechanisms enables the energetic and economic assessment of CO2 sequestration by wollastonite carbonation, which forms an essential next step in its further development.
Original languageEnglish
Pages (from-to)4242-4251
JournalChemical Engineering Science
Volume61
Issue number13
DOIs
Publication statusPublished - 2006

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Carbonation
Leaching
Silicates
Carbon dioxide process
Nucleation
Temperature
Particle size
Calcium Carbonate
Carbonates
Calcium carbonate
Partial pressure
Reaction rates
calcium silicate
Dissolution
Economics
Liquids

Keywords

  • dioxide
  • disposal

Cite this

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title = "Mechanisms of aqueous wollastonite carbonation as a possible CO2 sequestration process",
abstract = "The mechanisms of aqueous wollastonite carbonation as a possible carbon dioxide sequestration process were investigated experimentally by systematic variation of the reaction temperature, CO2 pressure, particle size, reaction time, liquid to solid ratio and agitation power. The carbonation reaction was observed to occur via the aqueous phase in two steps: (1) Ca leaching from the CaSiO3 matrix and (2) CaCO3 nucleation and growth. Leaching is hindered by a Ca-depleted silicate rim resulting from incongruent Ca-dissolution. Two temperature regimes were identified in the overall carbonation process. At temperatures below an optimum reaction temperature, the overall reaction rate is probably limited by the leaching rate of Ca. At higher temperatures, nucleation and growth of calcium carbonate are probably limiting the conversion, due to a reduced (bi)carbonate activity. The mechanisms for the aqueous carbonation of wollastonite were shown to be similar to those reported previously for an industrial residue and a Mg-silicate. The carbonation of wollastonite proceeds rapidly relative to Mg¿silicates, with a maximum conversion in 15 min of 70{\%} at , 20 bar CO2 partial pressure and particle size of . The obtained insight in the reaction mechanisms enables the energetic and economic assessment of CO2 sequestration by wollastonite carbonation, which forms an essential next step in its further development.",
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Mechanisms of aqueous wollastonite carbonation as a possible CO2 sequestration process. / Huijgen, W.J.J.; Witkamp, G.J.; Comans, R.N.J.

In: Chemical Engineering Science, Vol. 61, No. 13, 2006, p. 4242-4251.

Research output: Contribution to journalArticleAcademicpeer-review

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AU - Comans, R.N.J.

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N2 - The mechanisms of aqueous wollastonite carbonation as a possible carbon dioxide sequestration process were investigated experimentally by systematic variation of the reaction temperature, CO2 pressure, particle size, reaction time, liquid to solid ratio and agitation power. The carbonation reaction was observed to occur via the aqueous phase in two steps: (1) Ca leaching from the CaSiO3 matrix and (2) CaCO3 nucleation and growth. Leaching is hindered by a Ca-depleted silicate rim resulting from incongruent Ca-dissolution. Two temperature regimes were identified in the overall carbonation process. At temperatures below an optimum reaction temperature, the overall reaction rate is probably limited by the leaching rate of Ca. At higher temperatures, nucleation and growth of calcium carbonate are probably limiting the conversion, due to a reduced (bi)carbonate activity. The mechanisms for the aqueous carbonation of wollastonite were shown to be similar to those reported previously for an industrial residue and a Mg-silicate. The carbonation of wollastonite proceeds rapidly relative to Mg¿silicates, with a maximum conversion in 15 min of 70% at , 20 bar CO2 partial pressure and particle size of . The obtained insight in the reaction mechanisms enables the energetic and economic assessment of CO2 sequestration by wollastonite carbonation, which forms an essential next step in its further development.

AB - The mechanisms of aqueous wollastonite carbonation as a possible carbon dioxide sequestration process were investigated experimentally by systematic variation of the reaction temperature, CO2 pressure, particle size, reaction time, liquid to solid ratio and agitation power. The carbonation reaction was observed to occur via the aqueous phase in two steps: (1) Ca leaching from the CaSiO3 matrix and (2) CaCO3 nucleation and growth. Leaching is hindered by a Ca-depleted silicate rim resulting from incongruent Ca-dissolution. Two temperature regimes were identified in the overall carbonation process. At temperatures below an optimum reaction temperature, the overall reaction rate is probably limited by the leaching rate of Ca. At higher temperatures, nucleation and growth of calcium carbonate are probably limiting the conversion, due to a reduced (bi)carbonate activity. The mechanisms for the aqueous carbonation of wollastonite were shown to be similar to those reported previously for an industrial residue and a Mg-silicate. The carbonation of wollastonite proceeds rapidly relative to Mg¿silicates, with a maximum conversion in 15 min of 70% at , 20 bar CO2 partial pressure and particle size of . The obtained insight in the reaction mechanisms enables the energetic and economic assessment of CO2 sequestration by wollastonite carbonation, which forms an essential next step in its further development.

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