Journal
ACS EARTH AND SPACE CHEMISTRY
Volume 2, Issue 7, Pages 640-652Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsearthspacechem.8b00039
Keywords
shale gas; tight gas; methane; hydrofracking; carbon capture and utilization; smectite
Funding
- United States Department of Energy, Office of Science, Office of Basic Energy Science, Chemical science, Biosciences, and Geo-sciences division [DE-FG02-08ER15929]
- U.S. Department of Energy, Office of Fossil Energy
- United States Department of Energy, Office of Science, Office of Workforce Development
- Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory [48812, 49782]
- DOE [DE-AC05-76RL01830]
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The results from novel in situ high-pressure nuclear magnetic resonance (NMR) spectroscopy, infrared (IR) spectroscopy, and X-ray diffraction (XRD) investigation of the interaction of the smectite hectorite with variably wet supercritical methane (scCH(4)) at 90 bar and 323 K (hydrostatic conditions equivalent to similar to 1 km depth) show that CH4 occurs in the clay interlayers, in pores external to the individual clay particles, and as bulk fluid. The occupancy of each environment depends on the relative humidity (RH) of the CH4-rich fluid and the hydration energy and size of the charge-balancing cation. As RH increases, the fraction of interlayer and interparticle CH4 decreases, although with Cs+, addition of a small amount of H2O initially increases CH4 uptake. Maximum interlayer CH4 adsorption occurs when the mean basal spacing just permits methane intercalation (similar to 11.5 angstrom) and never below this basal spacing. It is also higher with divalent cations than with monovalent cations. The data show that CH4 adsorption occurs predominantly via a weak dispersion interaction with the clay and that its intercalation occurs via a passive space-filling hydrophobic mechanism. The results suggest that, under reservoir conditions, smectite interlayers may provide a reservoir for CH4 under low-water conditions.
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