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Pore-scale controls on calcite dissolution rates from flow-through laboratory and numerical experiments.

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This study investigated calcite dissolution under high carbon dioxide (CO2) conditions using experiments and pore-scale modeling. Results show that while reaction rates are key, mass transport limitations also affect dissolution, especially in complex geological formations.

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Area of Science:

  • Geochemistry
  • Geology
  • Chemical Engineering

Background:

  • Calcite dissolution is crucial for geological processes, including carbon sequestration and reservoir integrity.
  • Understanding dissolution under elevated carbon dioxide (CO2) is vital for subsurface applications.
  • Pore-scale transport and surface reactions govern mineral dissolution rates.

Purpose of the Study:

  • To investigate pore-scale transport and surface reaction controls on calcite dissolution.
  • To simulate calcite dissolution under elevated partial pressure of CO2 (pCO2) conditions.
  • To compare experimental results with high-resolution pore-scale numerical modeling.

Main Methods:

  • Laboratory experiments involving injecting a solution at 4 bar pCO2 into a calcite-packed capillary tube.
  • High-resolution pore-scale numerical modeling using computational domains from X-ray microtomography images.
  • Analysis of effluent concentrations and comparison between simulated and measured data.

Main Results:

  • Simulated effluent concentrations exceeded measured values by a factor of 1.8.
  • Discrepancies were primarily attributed to uncertainties in the calcite reaction rate model.
  • Mass transport limitations, particularly diffusive boundary layers and slow-flow zones, contributed to discrepancies.

Conclusions:

  • Pore-scale transport limitations, though minor in this study, are discernible and impact calcite dissolution.
  • The findings highlight the importance of accurate reaction kinetics and transport modeling for subsurface processes.
  • Differences between pore- and continuum-scale models are expected to increase with greater subsurface heterogeneity.