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Thomas Headen

Publications and source records attributed to Thomas Headen.

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Neutron scattering reveals fractionation of natural gas mixtures in unconventional petroleum reservoir pores: Perspectives on energy resource recovery and storage

In unconventional petroleum reservoirs hydrocarbon fluids are hosted by both mineral and organic matter pores. These pores can have diameters that range from microns to less than a single nanometer and, for unconventional reservoirs, there is evidence that small pores ( <20 nm diameter) may constitute a large proportion of the available space. Understanding subsurface volumes and how fluids behave in them can be helpful for predicting hydrocarbon production and storage in the subsurface. One area with knowledge gaps regarding hydrocarbon behavior in small pores is the possibility for mixtures to fractionate (i.e., unmix) based on pore size or pore type. Mixture fractionation as a function of pore size could impact recovery of hydrocarbons, drive compositional shifts during production, and limit fluid storage within candidate reservoirs. To investigate natural gas fractionation in small geologic pores, we applied total neutron scattering to probe methane-ethane mixtures at reservoir pressures (up to ≈30 MPa) and temperature (60°C) within a sample from the Upper Cretaceous Niobrara Formation. Neutron scattering data reveal only minor fractionation occurs between methane and ethane in 20-nm diameter sample mesopores. Increased fractionation is observed for sample micropores, with up to 72% (±1% at 1-sigma) methane found in 2 nm diameter pores following injection of a 50%-50% methane-ethane mixture. These data provide rarely available direct experimental observations of hydrocarbon mixture behavior under nanoconfinement in a sample from an important unconventional petroleum reservoir. Our results are discussed in the context of evaluating hydrocarbon resources in unconventional reservoir meso- and micropores, reconciling observed gas composition changes during production, and more broadly, understanding subsurface pore volumes within an energy storage framework.

Fuel↗

Exploring methane behavior in Marcellus Shale micropores via contrast matching neutron scattering

Petroleum in shale reservoirs is hosted in organic matter and mineral pores as well as in natural fractures and voids. For thermally mature plays, e.g., the Marcellus Shale, methane and other light alkane gases are thought to be primarily contained in organic matter pores with radii ≦50 nm. Thus, in order to understand natural gas occurrence, transport, storage, and recoverability within unconventional reservoirs at the dry-gas stage of thermal maturity, it is critical to characterize the associated organic matter porosity across length scales from 50 nm down to the angstrom level. We utilized wide Q-range neutron total scattering to characterize deuterated methane (CD 4 ) adsorption at 60ºC up to the zero average contrast (ZAC) pressure (~60 MPa) within two mineralogically different samples collected from the same producing interval from the Middle Devonian Marcellus Shale. The neutron scattering approach used here provides structural information from the inter-atomic regime up to a nominal pore radius of ~12.5 nm and, by reaching the CD 4 ZAC pressure (~60 MPa), it is possible to examine the distribution of open versus closed pores within this pore size range in the samples. Our results indicate that ~10% of the largest pores measured are closed to CD 4 for a quartz-rich sample whereas up to 25% of pores with a nominal radius of ~12.5 nm are inaccessible within a sample with an equivalent proportion of quartz, carbonate, and clay. As pore size decreases, accessibility also decreases; all pores with radii ~0.5 nm are effectively closed to CD 4 in both samples. Additionally, up to ~4.5× more CD 4 is adsorbed within the quartz-rich sample at 60 MPa and we see no evidence for densification of CD 4 within the shale pores. These findings suggest that, for shale samples within the dry-gas window, (i) nanometer-scale porosity is primarily located within organic matter, (ii) the amount of available nano-porosity can vary widely over meter scales, and (iii) mineralogy plays a secondary role in dictating methane behavior within these systems.

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