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<p>Carbon capture, utilization, and storage (CCUS) technologies are central to mitigating greenhouse gas emissions and achieving net-zero emission goals. Among these, CO<sub>2</sub> mineralization in mafic and ultramafic rocks offers a permanent storage mechanism by converting CO<sub>2</sub> into stable carbonates through reactions with Ca-, Mg-, and Fe-rich minerals. This study examines the effects of depth-pressure-temperature (P-T), CO<sub>2</sub> fugacity (pCO<sub>2</sub>), CO<sub>2</sub> saturation, reactive surface area (SA), and fracture surface roughness on mineral carbonation potential in mafic deposits, utilizing reactive-transport modeling. Using a 1 m<sup>3</sup> mixed-flow homogeneous reactor with parallel-plate fractures, we conducted 4400 single-mineral simulations (forsterite, diopside, anorthite, and magnetite) over 1000 years, with variable depth, pCO<sub>2</sub>, and SA. Additional simulations examined carbonation in synthetic heterogeneous mixtures representing mafic intrusions from the Duluth Complex, Minnesota. </p><p>Response surface analysis of carbonation potential (<InlineEquation ID="IEq1"> <EquationSource Format="TEX">\({\alpha _{mineral}}\)</EquationSource> </InlineEquation>=g CO<sub>2</sub> mineralized/g initial mineral) showed higher sensitivity to SA than pCO<sub>2</sub> at the surface, with rougher surfaces yielding higher <InlineEquation ID="IEq2"> <EquationSource Format="TEX">\({\alpha _{mineral}}\)</EquationSource> </InlineEquation>. At constant SA, the <InlineEquation ID="IEq3"> <EquationSource Format="TEX">\({\alpha _{mineral}}\)</EquationSource> </InlineEquation> sensitivity to pCO<sub>2</sub> increases with depth due to enhanced CO<sub>2</sub> solubility at higher P-T, promoting more carbonation. Thus, under subcritical pCO<sub>2</sub> (&lt; 500&#xa0;m), highly fractured mafic rocks exhibited the greatest <InlineEquation ID="IEq4"> <EquationSource Format="TEX">\({\alpha _{mineral}}\)</EquationSource> </InlineEquation>. Forsterite and magnetite showed the highest carbonation (0.1–0.65 and 0.05–0.45), while diopside and anorthite showed intermediate (0.006–0.13) and low values (0.0012–0.0046), respectively. Comparison showed that forsterite and magnetite drove rapid carbonation initially, while diopside and anorthite sustained long-term mineralization in complex rocks. These insights advance predictive frameworks for quantifying carbonation potential and optimizing CO<sub>2</sub> mineralization conditions in mafic and ultramafic deposits and mine tailings.</p>

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Optimizing CO2 mineralization potential under in situ and ex situ conditions using reactive transport simulation

  • 期刊论文

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  • 发表日期：

    2026年4月24日

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  • Piyali Chanda,
  • John Ogunleye,
  • Emran Chowdhury,
  • Thomas Monecke,
  • Ryan M. Pollyea

摘要

Carbon capture, utilization, and storage (CCUS) technologies are central to mitigating greenhouse gas emissions and achieving net-zero emission goals. Among these, CO2 mineralization in mafic and ultramafic rocks offers a permanent storage mechanism by converting CO2 into stable carbonates through reactions with Ca-, Mg-, and Fe-rich minerals. This study examines the effects of depth-pressure-temperature (P-T), CO2 fugacity (pCO2), CO2 saturation, reactive surface area (SA), and fracture surface roughness on mineral carbonation potential in mafic deposits, utilizing reactive-transport modeling. Using a 1 m3 mixed-flow homogeneous reactor with parallel-plate fractures, we conducted 4400 single-mineral simulations (forsterite, diopside, anorthite, and magnetite) over 1000 years, with variable depth, pCO2, and SA. Additional simulations examined carbonation in synthetic heterogeneous mixtures representing mafic intrusions from the Duluth Complex, Minnesota.

Response surface analysis of carbonation potential ( \({\alpha _{mineral}}\) =g CO2 mineralized/g initial mineral) showed higher sensitivity to SA than pCO2 at the surface, with rougher surfaces yielding higher \({\alpha _{mineral}}\) . At constant SA, the \({\alpha _{mineral}}\) sensitivity to pCO2 increases with depth due to enhanced CO2 solubility at higher P-T, promoting more carbonation. Thus, under subcritical pCO2 (< 500 m), highly fractured mafic rocks exhibited the greatest \({\alpha _{mineral}}\) . Forsterite and magnetite showed the highest carbonation (0.1–0.65 and 0.05–0.45), while diopside and anorthite showed intermediate (0.006–0.13) and low values (0.0012–0.0046), respectively. Comparison showed that forsterite and magnetite drove rapid carbonation initially, while diopside and anorthite sustained long-term mineralization in complex rocks. These insights advance predictive frameworks for quantifying carbonation potential and optimizing CO2 mineralization conditions in mafic and ultramafic deposits and mine tailings.