Dynamic development of geochemical reaction fronts during hydraulic stimulation of shale. (January 2023)

• Record Type: Journal Article
• Authors: Noël, Vincent; Druhan, Jennifer L.; Gundogar, Asli; Kovscek, Anthony R.; Brown, Gordon E.; Bargar, John R.
• Is Part Of: Applied geochemistry. Volume 148(2023)
• Publication Date: 2023-01
• Subjects: Geochemical reaction front -- Mineral dissolution -- Matrix alteration -- Reactive transport -- Hydraulic stimulation -- Unconventional shale -- Synchrotron-based X-ray fluorescence microprobe; Br Bromide -- XFM X-ray Fluorescence Microprobe -- CT Computed Tomography -- XRF X-ray Fluorescence -- NETL National Energy Technology Laboratory -- HFF Hydraulic Fracturing Fluid -- SSRL Stanford Synchrotron Radiation Lightsource -- TST Transition State Theory -- SEM Scanning Electron Microscopy -- DOE Department of Energy -- CMC-UF Center for Mechanistic Control of Water-Hydrocarbon-Rock Interactions in Unconventional and Tight Oil Formations; Environmental geochemistry -- Periodicals; Water chemistry -- Periodicals; Geochemistry -- Social aspects -- Periodicals; Geochemistry -- Periodicals; 551.9
• DOI: 10.1016/j.apgeochem.2022.105542
• Languages: English
• ISSNs: 0883-2927

Abstract

Abstract: Injection of acidic hydraulic fracture fluid (HFF) into shale formations for unconventional oil/gas production results in chemical reactions in the shale matrix that can alter fluid transport. Here, we report the results of set of experiments designed to evaluate the impact of calcite dissolution as a function of carbonate mineral content on matrix chemical reactivity and pore-space modification concomitant with imbibition. We tracked acidic HFF transport in four samples of Wolfcamp shale with calcite contents varying from 4% to 59% by monitoring the rate and spatial extent of bromide tracer transport using synchrotron-based X-ray fluorescence microprobe (XFM) imaging. Concurrently, we also carried out XFM imaging of the spatial distribution of Ca in the Wolfcamp shale cores (as a proxy of calcite distribution). Our approach thus yields a direct record of time-resolved selective ion transport resulting from the penetration of acidic HFF and the associated mineral transformations in the shale cores. We show that the variability in calcite content of Wolfcamp shale samples can directly affect the rate and spatial extent of imbibition. Although reaction of the acidic HFF with carbonates in shales enhances calcite dissolution and increases porosity, the spatial extent of calcite dissolution in the shale matrix is limited due to a rapid neutralization of pH. The relative abundance and spatial distribution of calcite control the chemical saturation state of the HFF progressing into the matrix. As a result, calcite has a major impact on the spatial extent and rate of matrix alteration and thus on HFF transport during subsurface reservoir stimulation. Consequently, increased calcite content in the shale matrix inhibits the spatial extent of the pore-volume increase and, by extension, the spatial extent and rate of imbibition. Our results thus show that the overall rates of calcite dissolution approach the rates of acidic HFF transport ( i.e., Damköhler number ∼1), which could contribute to the efficiency of subsurface reservoir stimulation. A better understanding of HFF-calcite reaction rates is crucial for improving the prediction and optimization of fluid transport across HFF-shale interfaces during hydraulic fracturing. Graphical abstract: Image 1 Highlights: Development of an experimental approach providing qualitative dataset into shale. Spatially and temporally resolved mapping of reactions fronts during hydraulic fracturing. The overall rates of calcite dissolution approach the rates of acidic HFF transport. The increased calcite content in the shale matrix inhibits the imbibition efficiency.