Search

Understanding flow, transport, chemical reactions, and hydromechanical processes in fractured geologic materials is key for optimizing a range of subsurface processes including carbon dioxide and hydrogen storage, unconventional energy resource extraction, and geothermal energy recovery. Flow and transport processes in naturally fractured shale rocks have been challenging to characterize due to experimental complexity and the multiscale nature of quantifying continuum scale descriptions of mass exchange between micrometer-scale fractures and nanometer-scale pores. In this study, we use positron emission tomography (PET) to image the transport of a conservative tracer in a naturally fractured Wolfcamp shale core before and after the core was exposed to low pH brine conditions. Image-based experimental observations are interpreted by fitting an analytical transport model to fracture-containing voxels in the core. Results of this analysis indicate subtle increases in matrix diffusivity and a slightly more uniform fracture velocity distribution following exposure to low pH conditions. These observations are compared with a multicomponent one-dimensional reactive transport model that indicates the capacity for a 10% increase in porosity at the fracture-matrix interface as a result of the low pH brine exposure. This porosity change is the result of the dissolution of carbonate minerals in the shale matrix to low pH conditions. This image-based workflow represents a new approach for quantifying spatially resolved fracture-matrix transport processes and provides a foundation for future work to better understand the role of coupled transport, reaction, and mechanical processes in naturally fractured rocks.

The transport of chemical species in rocks is affected by their structural heterogeneity to yield a wide spectrum of local solute concentrations. To quantify such imperfect mixing, advanced methodologies are needed that augment the traditional breakthrough curve analysis by probing solute concentration within the fluids locally. Here, we demonstrate the application of asynchronous, multimodality imaging by X‐ray computed tomography (XCT) and positron emission tomography (PET) to the study of passive tracer experiments in laboratory rock cores. The four‐dimensional concentration maps measured by PET reveal specific signatures of the transport process, which we have quantified using fundamental measures of mixing and spreading. We observe that the extent of solute spreading correlate strongly with the strength of subcore‐scale porosity heterogeneity measured by XCT, while dilution is enhanced in rocks containing substantial sub‐micron porosity. We observe that the analysis of different metrics is necessary, as they can differ in their sensitivity to the strength and forms of heterogeneity. The multimodality imaging approach is uniquely suited to probe the fundamental difference between spreading and mixing in heterogeneous media. We propose that when multi‐dimensional data is available, mixing and spreading can be independently quantified using the same metric. We also demonstrate that one‐dimensional transport models have limited predictive ability toward the internal evolution of the solute concentration, when the model is solely calibrated against the effluent breakthrough curves. The data set generated in this study can be used to build realistic digital rock models and to benchmark transport simulations that account deterministically for rock property heterogeneity. X‐ray computed tomography and positron emission tomography applied in a multimodal imaging approach to study transport in rock coresSpreading and mixing are independently quantified from pulse tracer tests and correlated to distinct forms of subcore‐scale heterogeneityWhen solely calibrated against the breakthrough curve, 1D transport models cannot accurately describe internal concentration profiles X‐ray computed tomography and positron emission tomography applied in a multimodal imaging approach to study transport in rock cores Spreading and mixing are independently quantified from pulse tracer tests and correlated to distinct forms of subcore‐scale heterogeneity When solely calibrated against the breakthrough curve, 1D transport models cannot accurately describe internal concentration profiles

Dissolution trapping is one of the primary mechanisms of carbon dioxide (CO2) storage in deep saline aquifers. The determination of the realized rates of CO2dissolution requires an understanding of the mixing process that takes place following the emplacement of CO2into the formation. Owing to the difficulty of reproducing the time-dependent convective process in porous media, experiments so far have largely focused on 2D systems (e.g., Hele-Shaw cells) and used analogue fluid pairs with properties that differ from the subsurface CO2/brine system. Here, we present a novel experimental approach to investigate the evolution of the convective mixing process in 3D porous media (homogeneous packings of glass beads) using X-ray computed tomography (CT). We explore a range of Rayleigh numbers (Ra= 3000–55000) and observe directly the mixing structures that arise upon dissolution. We compute from the images the temporal evolution of the spatial moments of the concentration distribution, including the cumulative dissolved mass, the location of the center of mass, and the standard deviation of the concentration field. The scalings of the spatial moments suggest an impact of hydrodynamic dispersion on the longitudinal mixing. We propose a simplified representation of the mixing process by analogy with the 1D advection–dispersion model. This enables the estimation of the bulk advective velocity and the effective longitudinal dispersion coefficient for each bead packing. These estimates suggest that the presence of the finger pattern and the counter-current flow structure enhance the longitudinal spreading of the solute by roughly 1 order of magnitude compared to unidirectional dispersion of a single-solute plume.