Browsing by Author "Pearce, JK"

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    Cooper Basin REM gas shales after CO2 storage or acid reactions: metal mobilisation and methane accessible pore changes
    (Elsevier, 2023-05-15) Pearce, JK; Blach, T; Dawson, GKW; Southam, G; Paterson, DJ; Golding, SD; Bahadur, J; Melnichenko, YB; Rudolph, V
    Shale - 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.
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    Core characterisation and predicted CO2 reactivity of sandstones and mudstones from an Australian oil field
    (Elsevier, 2022-02-01) Pearce, JK; Brink, F; Dawson, GW; Poitras, J; Southam, G; Paterson, DJ; Wolhuter, A; Underschultz, JR
    CO2 geological storage has been proposed as one method to mitigate climate change. Storage of CO2 in depleted oil or gas fields is one option, potentially following enhanced recovery. Understanding the potential impacts of CO2 water rock reactions is an important aspect of storage feasibility studies. Drill core samples of sandstones and mudstones from the Jurassic Moonie oil field, Australia, were characterised. In the Precipice Sandstone reservoir samples pore throats had broad size distributions, with mercury intrusion porosities 6.2 to 14.6%. Evergreen Formation samples were more variable with 1.2 to 16.1% porosity. Porosities measured by QEMSCAN were in reasonable agreement at 8.6 to 15.3% for Precipice Sandstones, and 0.6 to 21.5 for the Evergreen Formation. Sandstones had larger pore throat sizes and lower threshold pressures indicative of good reservoir rocks. Calcite cemented sandstones had truncated pore throat distributions, and the coal and clay rich mudstones had pore throats <0.1 μm with higher threshold pressures likely to seal or baffle CO2. Quartz grains were naturally fractured, with silica, apatite, rutile, calcite, and siderite cements filling porosity in some samples. Feldspars had been weathered producing secondary porosity but also resulting in kaolinite and illite filling intergranular porosity. Pyrite and barite were mainly associated with coals. Synchrotron X-ray fluorescence mapping showed Sr was mainly hosted in calcite cement, apatite and barite; with Rb in both plagioclase and K-feldspars. Calcite mainly hosted Mn; while Zn and Cu were mainly in sulphides. Sulphide minerals in coal also hosted As in one core. Kinetic geochemical CO2-water-rock modelling using the characterisation data over 30 or 1000 years indicated reaction of carbonate minerals where present, and alteration of mainly plagioclase, K-feldspar and chlorite. Net precipitation of ankerite, calcite or siderite mineral trapped 0.23 to 1.28 kg/m3 of CO2 after 1000 years in the different rock packages and was highest in Evergreen Formation rocks. The predicted pH was in the range 5.0 to 5.4 after 1000 years, or higher at 5.2 to 7.1 in lower CO2 fugacity models. Sandstone reactivity was overall low over 30 years indicating a low likelihood of reservoir scaling which would be favourable, with mineral trapping likely in the overlying Evergreen Formation. © 2021 Elsevier B.V.
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    Impure CO2 storage reactions of sandstone, mudstone and carbonate cemented cores: xxperimental CO2 SO2 NOX O2 reaction metal mobilisation and fate
    (Elsevier, 2023-09-01) Pearce, JK; Dawson, GW; Brink, F; Southam, G; Paterson, DJ; Hall, N; Heath, R; Greer, D; Kirste, D; Golding, SD
    CO2 geological storage can be part of the solution to reduce carbon emissions to the atmosphere. An understanding of the geochemical processes occurring during CO2 storage is needed to reduce risk. Drill cores from a low salinity reservoir site proposed for CO2 storage, and the overlying and underlying formations, were characterised for minerals by QEMSCAN, total metals and porosity. Elements including Li, Ba, Sr, K, Mg, V, Zn, REE, Fe, Pb, P, and S were relatively elevated in the Moolayember Formation underlying the reservoir. Synchrotron XFM showed the main host of Mn was siderite, with Rb in K-feldspar, Zn and Cu in sphalerite and chalcopyrite, and As in pyrite in coal pores associated with coal laminations. Drill cores are reacted at reservoir conditions with synthetic formation water and an impure CO2 stream composition of CO2-SOx-NOx-O2 expected to be injected at the site. Elements released were dependant on mineral content, with quartz rich reservoir, lower Precipice Sandstone core reactions resulting in dissolution of trace carbonates, alteration of sulphides and monazite, and variable elevated dissolved Pb, and U. Dissolved Co, Ni, Ca, Zn, Li, Rb, and U were released at relatively elevated concentrations from the mudstone. For carbonate cemented upper Precipice Sandstone or Moolayember Formation core strong dissolution of calcite and ankerite, with corrosion of siderite, Fe-rich chlorite, and sulphides or monazite were observed after reaction. Dissolved elements including Ca, Mg, Mn, Sr, and Ba increased in experiments from the reaction of calcite, siderite, and ankerite. Generally dissolved Fe, Pb, Cr, Cu, Co etc. increased from dissolution, and subsequently decreased in concentration with adsorption and precipitation processes. The fast mobilisation of elements including Fe and Pb are consistent with the release of metals from carbonate dissolution and desorption. The presence of O2 and NOX in the gas stream results in Fe-(oxyhydr)oxide precipitation especially where Fe has been rapidly mobilised from dissolution of siderite and Fe-chlorite. This acts as a sink for Fe and provides new adsorption sites for sequestering a proportion of the trace metals. These processes are applicable to other CO2 storage sites and potential leakage indicators in overlying drinking water aquifers. The findings are also more broadly applicable to subsurface energy storage such as compressed air renewable energy storage, CO2 enhanced recovery, geothermal, natural gas or hydrogen storage. © 2023 The Authors. Published by Elsevier B.V. - Open Access CC-BY.
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    Multiple tracers for dis-connectivity of shallow aquifers, alluvium, and coal seam gas wells in the Great Artesian Basin
    (CSIRO Publishing, 2022-05-13) Pearce, JK; Golding, SD; Baublys, KA; Hofmann, H; Cendón, DI; Herbert, SJ; Hayes, PJ
    The potential for connectivity between water supply aquifers and gas reservoirs raises community, government, and scientific concerns. Methane can occur naturally, making it difficult to determine whether water bore methane levels are being influenced by nearby gas operations. This poses a challenge in the Surat Basin, where coal seam gas production operates alongside groundwater using industries (including feedlots, agriculture, mines). Water and gas samples were taken from water bores and coal seam gas (CSG) wells in the Walloon Coal Measures and from overlying aquifers (nominally, the Springbok, Gubberamunda, Orallo, and Mooga sandstones) and the Condamine Alluvium, for stable isotopes of gases, groundwater and dissolved inorganic carbon, as well as strontium isotopes. Most of the sampled water bores had isotopic signatures distinct from CSG wells, though a minority from gassy Springbok Sandstone and Walloon Coal Measure water bores could not be distinguished from CSG wells. In those few cases, neither connectivity or dis-connectivity could be confirmed. Alluvium and shallow aquifer samples have higher R36Cl values distinct from the older CSG production waters, as is the case with most 14C measurements. Waters from the Condamine River indicate potential surface water connectivity with the alluvium. The use of multiple tracers has shown that groundwater in some aquifers can be differentiated from groundwater in the coal seam gas reservoir and hence are useful tools in identifying where groundwater connectivity occurs. Understanding this connectivity forms another line of evidence to improve impact prediction models on a regional scale as well as providing information on connectivity in local groundwater investigations. © 2022 The Author(s) (or their employer(s)). Published by CSIRO Publishing on behalf of APPEA.
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    Predicted CO2 water rock reactions in naturally altered CO2 storage reservoir sandstones, with interbedded cemented and coaly mudstone seals
    (Elsevier, 2022-03-15) Pearce, JK; Dawson, GW; Golding, SD; Southam, G; Paterson, DJ; Brink, F; Underschultz, JR
    Geological storage of CO2 captured from industrial processes such as coal combustion or from direct air capture is part of the transition to low emissions. The Jurassic Precipice Sandstone of the southern Surat Basin, Queensland, Australia, is undergoing feasibility studies for industrial scale CO2 geological storage, however regional data has so far been lacking. Precipice Sandstone reservoir drill core samples from the Southwood 1 and Tipton 153 wells in the southern Surat Basin include favourably quartz rich sandstone regions with quartz grain fracturing. A mudstone layer is also present in the reservoir. The overlying lower section of the Evergreen Formation seals consist of clay rich sandstones, interbedded mudstones, coal layers, Fe-Mg-Mn siderite, and Mg-calcite cemented sandstones. K-feldspars are weathered creating localised secondary porosity and pore filling kaolinite and illite. Layers of coal, pore filling cements, and framework grain compaction introduce vertical heterogeneity. Heavy minerals including pyrite, mixed composition sulphides, and barite are associated with disseminated coals in mudstones. Precipice Sandstone mercury intrusion porosities (MIP) ranged from 9 to 22% with favourably low reservoir injection threshold pressures, and the QEMSCAN measured open porosity between 2 and 22%. Evergreen Formation seal porosities were 7.5 to 16% by MIP or 1 to 19% by QEMSCAN, with the smallest pore throat distribution associated with the low permeability coal rich mudstone. Synchrotron XFM shows Rb mainly hosted in K-feldspars and muscovite, with metals including Mn mainly hosted in siderite. Zn and As are present in sulphides; and calcite and apatite cements mainly hosted Sr. Twenty kinetic geochemical CO2-water-rock models were run for 30 and 1000 years with Geochemist Workbench, with calcite and siderite initially dissolving. In the Precipice Sandstone reservoir variable alteration of carbonates, feldspars and chlorite to kaolinite, silica, siderite and smectite were predicted with the pH remaining below 5.5. CO2 was mineral trapped through alteration of chlorite to siderite in three of the four cases, with −0.02 to 1.43 kg/m3 CO2 trapped after 1000 years. In the calcite and siderite cemented Evergreen Formation seal, plagioclase conversion to ankerite trapped the most CO2 with 2.6 kg/m3 trapped after 1000 years. The Precipice Sandstone in both wells appears to be generally suitable as a storage reservoir, with mineral trapping predicted to mainly occur in the overlying lower Evergreen Formation and in interbedded mudstones. Heterogeneity in interbedded sandstone, mudstone, and coal layers are likely to act as baffles to CO2 and encourage mineral trapping. Quartz grain fractures may influence preferential migration pathways in the reservoir but this would need future experimental investigation. Experimental CO2 water rock reactions to understand porosity and permeability changes were out of scope here but are recommended in future validation, along with investigating the potential for CO2 adsorption trapping in coal and mudstone layers. © 2022 Elsevier B.V. All rights reserved.