4.7 Article

Capillary pressure and saturation relations for supercritical CO2 and brine in sand: High-pressure Pc(Sw) controller/meter measurements and capillary scaling predictions

Journal

WATER RESOURCES RESEARCH
Volume 49, Issue 8, Pages 4566-4579

Publisher

AMER GEOPHYSICAL UNION
DOI: 10.1002/wrcr.20316

Keywords

capillary pressure; geologic carbon sequestration; capillary scaling; wettability

Funding

  1. ZERT
  2. NCGC
  3. NRAP
  4. Office of Sequestration, Hydrogen, and Clean Coal Fuels, through the National Energy Technology Laboratory (NETL), U.S. Department of Energy [DE-AC02-05CH11231]
  5. Center for Nanoscale Control of Geologic CO2, an Energy Frontier Research Center
  6. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-05CH11231]
  7. DOE Office of Fossil Energy's Cross Cutting Research program
  8. NRAP under U.S. Department of Energy [DE-AC02-05CH11231]

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In geologic carbon sequestration, reliable predictions of CO2 storage require understanding the capillary behavior of supercritical (sc) CO2. Given the limited availability of measurements of the capillary pressure (P-c) dependence on water saturation (S-w) with scCO(2) as the displacing fluid, simulations of CO2 sequestration commonly rely on modifying more familiar air/H2O and oil/H2O P-c(S-w) relations, adjusted to account for differences in interfacial tensions. In order to test such capillary scaling-based predictions, we developed a high-pressure P-c(S-w) controller/meter, allowing accurate P-c and S-w measurements. Drainage and imbibition processes were measured on quartz sand with scCO(2)-brine at pressures of 8.5 and 12.0MPa (45 degrees C), and air-brine at 21 degrees C and 0.1MPa. Drainage and rewetting at intermediate S-w levels shifted to P-c values that were from 30% to 90% lower than predicted based on interfacial tension changes. Augmenting interfacial tension-based predictions with differences in independently measured contact angles from different sources led to more similar scaled P-c(S-w) relations but still did not converge onto universal drainage and imbibition curves. Equilibrium capillary trapping of the nonwetting phases was determined for P-c=0 during rewetting. The capillary-trapped volumes for scCO(2) were significantly greater than for air. Given that the experiments were all conducted on a system with well-defined pore geometry (homogeneous sand), and that scCO(2)-brine interfacial tensions are fairly well constrained, we conclude that the observed deviations from scaling predictions resulted from scCO(2)-induced decreased wettability. Wettability alteration by scCO(2) makes predicting hydraulic behavior more challenging than for less reactive fluids.

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