New perspectives on supercritical methane adsorption in shales and associated thermodynamics

Tang, Xu; Ripepi, Nino; Rigby, Sean; Mokaya, Robert; Gilliland, Ellen

doi:10.1016/j.jiec.2019.06.015

New perspectives on supercritical methane adsorption in shales and associated thermodynamics

Journal Article · Tue Oct 01 00:00:00 UTC 2019 · Journal of Industrial and Engineering Chemistry

DOI:https://doi.org/10.1016/j.jiec.2019.06.015· OSTI ID:1799733

^[1]; Ripepi, Nino ^[2]; Rigby, Sean ^[3]; Mokaya, Robert ^[3]; Gilliland, Ellen ^[2]

Univ. of Nottingham (United Kingdom); Chinese Academy of Sciences (CAS), Beijing (China); OSTI
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Univ. of Nottingham (United Kingdom)

Understanding methane adsorption behavior in shales is fundamental for optimizing shale gas development as the adsorbed methane is a large portion of the subsurface shale gas resource. However, the adsorption mechanism of supercritical methane in shales and associated thermodynamics are poorly understood because the equation of state of the adsorbed methane is unmeasurable. This work analyzed adsorption equilibria (up to 32 MPa and 393.15 K) using a rigorous framework that can account for non-ideal gas properties and accurately extrapolate absolute adsorption uptakes from measured adsorption isotherms. The framework also allows a straightforward calculation of thermodynamic potentials relevant to adsorption such as enthalpy and entropy. Modelling results show that methane adsorption isotherms in shale under different pressures and temperatures are represented by a two dimensional adsorption isotherm surface. The density of the adsorbed methane in shales depends on temperature and pressure, which is always lower than the liquid methane density but higher than the corresponding gaseous methane density. The temperature-dependent and pressure-dependent characteristics of adsorbed methane density leads to the corresponding temperature-dependent and pressure-dependent measured/absolute adsorption isotherms. The maximum adsorption uptake of shales is independent of temperature and pressure. The isosteric enthalpy/entropy of adsorption and enthalpy/entropy of adsorbed methane are found to be temperature- and surface coverage-dependent. These new findings not only clarify some historical misunderstandings of methane adsorption in shales for engineering application, but also provide a novel framework for interpreting methane adsorption behavior in shales and for determining the associated thermodynamics.

View Accepted Manuscript (DOE)

Research Organization:: Southern States Energy Board, Peachtree Corners, GA (United States); Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Fossil Energy (FE)

Grant/Contract Number:: FE0006827; FE0026086; FE0029465

OSTI ID:: 1799733

Alternate ID(s):: OSTI ID: 1532785

Journal Information:: Journal of Industrial and Engineering Chemistry, Journal Name: Journal of Industrial and Engineering Chemistry Journal Issue: C Vol. 78; ISSN 1226-086X

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Adsorbed density
Adsorption
Chemistry
Engineering
Enthalpy
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Shale

New perspectives on supercritical methane adsorption in shales and associated thermodynamics

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