Cooper Basin REM gas shales after CO2 storage or acid reactions: metal mobilisation and methane accessible pore changes

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dc.contributor.authorPearce, JKen_AU
dc.contributor.authorBlach, Ten_AU
dc.contributor.authorDawson, GKWen_AU
dc.contributor.authorSoutham, Gen_AU
dc.contributor.authorPaterson, DJen_AU
dc.contributor.authorGolding, SDen_AU
dc.contributor.authorBahadur, Jen_AU
dc.contributor.authorMelnichenko, YBen_AU
dc.contributor.authorRudolph, Ven_AU
dc.date.accessioned2024-11-15T02:49:08Zen_AU
dc.date.available2024-11-15T02:49:08Zen_AU
dc.date.issued2023-05-15en_AU
dc.date.statistics2024-11-08en_AU
dc.description.abstractShale - water - CO2 reactions may occur during CO2 geological storage, enhanced gas recovery, enhanced oil recovery, or supercritical CO2 fracturing. Shale-acid reactions occur during fracturing or acid stimulation. The mobilisation of metals from these processes can be an environmental concern if production water leaks or is released at surface. In addition, reactions may cause changes at the pore scale and affect gas or fluid flow. Three gas shales from the Australian Cooper Basin REM sequence were characterised for metals in minerals by synchrotron X-ray fluorescence microscopy. Metals including Zn, As, Ni, Cr were hosted in sphalerite associated with organic matter, Pb was in pyrite cement, and Mn was hosted in siderite. The shales were separately reacted with brine and supercritical CO2, with CO2-SO2, with dilute HCl, or with N2 at 100 °C and 20 MPa in batch reactors. The solution pH decreased during mineral reactions releasing metals to solution with the general concentrations from reaction with HCl > CO2-SO2 > CO2 > N2 and brine. Of the total available Pb, As, Li, and Zn in the shales, from 0 to 17%, 0.3 to 23%, 3 to 13%, and 0.4 to 28% was released to solution respectively. Corrosion of siderite and ankerite was observed after the CO2 reactions, with precipitation of Fe-oxides. After CO2-SO2 reaction siderite and ankerite were dissolved with pyrite, barite, and Fe-rich precipitates. HCl reactions resulted in complete dissolution of carbonates, with dissolution pits and no mineral precipitation observed. The changes to the fractions of gas accessible mesopores were characterised by small angle neutron scattering (SANS). The Epsilon Formation had the greatest fraction of open accessible pores in the SANS range of 10 to 150 nm, followed by the Murteree and Roseneath shale samples. After CO2 or CO2-SO2 reactions a small decrease in pore accessibility was more pronounced in the Murteree and Roseneath shales, consistent with mineral precipitation. HCl reaction resulted in opening of pores at 150 nm and closing of the smallest measured pores at 10 nm. Metals were mobilised from siderite, ankerite and sulphide minerals mainly, and were dependent on the mineral and metal content but also on the injected gas stream or fluid composition. CO2 based fluids may result in cleaner flow back water, than HCl based fluids. Geochemical reactions during CO2 storage or acid treatment in reactive shales cause pore changes that can affect gas migration. Mineral precipitation during CO2 and CO2-SO2 reactions can result in favourable self-sealing. © 2023 The Authors. Published by Elsevier B.V. Open Access - CC-BY.en_AU
dc.description.sponsorshipLuc Turner, Dean Biddle, and Lei Ge are thanked for assistance with experiments and characterisation. Part of this work was funded by a UQ CEIF Firstlink grant. The UQ SEES Environmental Geochemistry Laboratory (EGL) is thanked for assistance with analyses. The research at Oak Ridge National Laboratory‘s High Flux Isotope Reactor was sponsored by the Laboratory Directed Research and Development Program and the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy, grant IPTS-10582. Part of this research was undertaken on the XFM beamline at the Australian Synchrotron, ANSTO. This relates to grant no. AS193/XFM/15296 “Regulated metals in oil and gas shale and associated flow back fluids”. We acknowledge travel funding provided by the International Synchrotron Access Program (ISAP) managed by the Australian Synchrotron, part of ANSTO, and funded by the Australian Government. Daryl Howard and Martin de Jonge are thanked for assistance at the XFM beamline. The authors acknowledge the facilities, and the scientific and technical assistance, of the Australian Microscopy & Microanalysis Research Facility at the Centre for Microscopy and Microanalysis, The University of Queensland. The anonymous reviewers and editors are thanked for their comments that have improved this manuscript.en_AU
dc.identifier.articlenumber104271en_AU
dc.identifier.citationPearce, J. K., Blach, T., Dawson, G. K. W., Southam, G., Paterson, D. J., Golding, S. D., Bahadur, J., Melnichenko, Y. B., & Rudolph, V. (2023). Cooper Basin REM gas shales after CO2 storage or acid reactions: metal mobilisation and methane accessible pore changes. International Journal of Coal Geology, 273, 104271. doi:10.1016/j.coal.2023.104271en_AU
dc.identifier.issn0166-5162en_AU
dc.identifier.journaltitleInternational Journal of Coal Geologyen_AU
dc.identifier.urihttps://doi.org/10.1016/j.coal.2023.104271en_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/15752en_AU
dc.identifier.volume273en_AU
dc.languageEnglishen_AU
dc.language.isoenen_AU
dc.publisherElsevieren_AU
dc.subjectGasesen_AU
dc.subjectShalesen_AU
dc.subjectCarbon dioxideen_AU
dc.subjectStorageen_AU
dc.subjectMetalsen_AU
dc.subjectMethaneen_AU
dc.subjectOrganic matteren_AU
dc.subjectPyriteen_AU
dc.subjectNickelen_AU
dc.subjectCopperen_AU
dc.subjectZincen_AU
dc.subjectSmall angle scatteringen_AU
dc.subjectSynchrotronsen_AU
dc.subjectWateren_AU
dc.subjectRocksen_AU
dc.titleCooper Basin REM gas shales after CO2 storage or acid reactions: metal mobilisation and methane accessible pore changesen_AU
dc.typeJournal Articleen_AU
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