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1.
Composite Portland cement–basalt caprock cores with fractures, as well as neat Portland cement columns, were prepared to understand the geochemical and geomechanical effects on the integrity of wellbores with defects during geologic carbon sequestration. The samples were reacted with CO2–saturated groundwater at 50 °C and 10 MPa for 3 months under static conditions, while one cement–basalt core was subjected to mechanical stress at 2.7 MPa before the CO2 reaction. Micro-XRD and SEM–EDS data collected along the cement–basalt interface after 3-month reaction with CO2–saturated groundwater indicate that carbonation of cement matrix was extensive with the precipitation of calcite, aragonite, and vaterite, whereas the alteration of basalt caprock was minor. X-ray microtomography (XMT) provided three-dimensional (3-D) visualization of the opening and interconnection of cement fractures due to mechanical stress. Computational fluid dynamics (CFD) modeling further revealed that this stress led to the increase in fluid flow and hence permeability. After the CO2-reaction, XMT images displayed that calcium carbonate precipitation occurred extensively within the fractures in the cement matrix, but only partially along the fracture located at the cement–basalt interface. The 3-D visualization and CFD modeling also showed that the precipitation of calcium carbonate within the cement fractures after the CO2-reaction resulted in the disconnection of cement fractures and permeability decrease. The permeability calculated based on CFD modeling was in agreement with the experimentally determined permeability. This study demonstrates that XMT imaging coupled with CFD modeling represent a powerful tool to visualize and quantify fracture evolution and permeability change in geologic materials and to predict their behavior during geologic carbon sequestration or hydraulic fracturing for shale gas production and enhanced geothermal systems.  相似文献   

2.
The objective of this study is to understand cement alteration processes with the evolution of porosity and hardness under geologic CO2 storage conditions. For this study, the cylindrical cement cores (class G) were reacted with CO2–saturated water in a vessel (40 °C and 8 MPa) for 10 and 100 days. After the experiment, the CO2 concentration and Vickers hardness were measured in the hydrated cement core to estimate the carbonation depth and to identify the change in hardness, respectively. Diffusive-reactive transport modeling was also performed to trace the alteration processes and subsequent porosity changes. The results show that cement alteration mainly results from carbonation. With alteration processes, four different reaction zones are developed: degradation zone, carbonation zone, portlandite depletion zone, and unreacted zone. In the degradation zone, the re-dissolution of calcite formed in the carbonation zone leads to the increase of porosity. In contrast, the carbonation zone is characterized by calcite formation resulting mainly from the dissolution of portlandite. The carbonation zone acts as a barrier to CO2 intrusion by consuming dissolved CO2. Especially in this zone, although the porosity decreases, the Vickers hardness increases. Our results show that cement alteration processes can affect the physical and hydrological properties of the hydrated cement under CO2-saturated conditions. Further long-term observation is required to confirm our results under in-situ fluid chemistry of a CO2 storage reservoir. Nonetheless, this study would be helpful to understand alteration processes of wellbore cements under CO2 storage conditions.  相似文献   

3.
The interaction of groundwater with cement in a geological disposal facility (GDF) for intermediate level radioactive waste will produce a high pH leachate plume. Such a plume may alter the physical and chemical properties of the GDF host rock. However, the geochemical and mineralogical processes which may occur in such systems over timescales relevant for geological disposal remain unclear. This study has extended the timescale for laboratory experiments and shown that, after 15 years two distinct phases of reaction may occur during alteration of a dolomite-rich rock at high pH. In these experiments the dissolution of primary silicate minerals and the formation of secondary calcium silicate hydrate (C–S–H) phases containing varying amounts of aluminium and potassium (C–(A)–(K)–S–H) during the early stages of reaction (up to 15 months) have been superseded as the systems have evolved. After 15 years significant dedolomitisation (MgCa(CO3)2 + 2OH− → Mg(OH)2 + CaCO3 + CO32−(aq)) has led to the formation of magnesium silicates, such as saponite and talc, containing variable amounts of aluminium and potassium (Mg–(Al)–(K)–silicates), and calcite at the expense of the early-formed C–(A)–(K)–S–H phases. This occured in high pH solutions representative of two different periods of cement leachate evolution with little difference in the alteration processes in either a KOH and NaOH or a Ca(OH)2 dominated solution but a greater extent of alteration in the higher pH KOH/NaOH leachate. The high pH alteration of the rock over 15 years also increased the rock’s sorption capacity for U(VI). The results of this study provide a detailed insight into the longer term reactions occurring during the interaction of cement leachate and dolomite-rich rock in the geosphere. These processes have the potential to impact on radionuclide transport from a geodisposal facility and are therefore important in underpinning any safety case for geological disposal.  相似文献   

4.
Between March 2008 and August 2009, 65,445 tonnes of ∼75 mol% CO2 gas were injected in a depleted natural gas reservoir approximately 2000 m below surface at the Otway project site in Victoria, Australia. Groundwater flow and composition were monitored biannually in two overlying aquifers between June 2006 and March 2011, spanning the pre-, syn- and post-injection periods. The shallower (∼0–100 m), unconfined, porous and karstic aquifer of the Port Campbell Limestone and the deeper (∼600–900 m), confined and porous aquifer of the Dilwyn Formation contain valuable fresh to brackish water resources. Groundwater levels in either aquifer have not been affected by the drilling, pumping and injection activities that were taking place, or by the rainfall increase during the project. In terms of groundwater composition, the Port Campbell Limestone groundwater is brackish (electrical conductivity = 801–3900 μS cm−1), cool (temperature = 12.9–22.5 °C), and near-neutral (pH = 6.62–7.45), whilst the Dilwyn Aquifer groundwater is fresher (electrical conductivity = 505–1473 μS cm−1), warmer (temperature = 42.5–48.5 °C), and more alkaline (pH = 7.43–9.35). Carbonate dissolution, evapotranspiration and cation exchange control the composition of the groundwaters. Comparing the chemical and isotopic composition of the groundwaters collected before, during and after injection shows no statistically significant changes; even if they were statistically significant, they are mostly not consistent with those expected if CO2 addition had taken place. The monitoring program reveals no impact on the groundwater resources attributable to the C storage demonstration project.  相似文献   

5.
Residual waste is expected to be left in 177 underground storage tanks after closure at the US Department of Energy’s Hanford Site in Washington State, USA. In the long term, the residual wastes may represent a potential source of contamination to the subsurface environment. Residual materials that cannot be completely removed during the tank closure process are being studied to identify and characterize the solid phases and estimate the release of contaminants from these solids to water that might enter the closed tanks in the future. As of the end of 2009, residual waste from five tanks has been evaluated. Residual wastes from adjacent tanks C-202 and C-203 have high U concentrations of 24 and 59 wt.%, respectively, while residual wastes from nearby tanks C-103 and C-106 have low U concentrations of 0.4 and 0.03 wt.%, respectively. Aluminum concentrations are high (8.2–29.1 wt.%) in some tanks (C-103, C-106, and S-112) and relatively low (<1.5 wt.%) in other tanks (C-202 and C-203). Gibbsite is a common mineral in tanks with high Al concentrations, while non-crystalline U–Na–C–O–P ± H phases are common in the U-rich residual wastes from tanks C-202 and C-203. Iron oxides/hydroxides have been identified in all residual waste samples studied to date. Contaminant release from the residual wastes was studied by conducting batch leach tests using distilled deionized water, a Ca(OH)2-saturated solution, or a CaCO3-saturated water. Uranium release concentrations are highly dependent on waste and leachant compositions with dissolved U concentrations one or two orders of magnitude higher in the tests with high U residual wastes, and also higher when leached with the CaCO3-saturated solution than with the Ca(OH)2-saturated solution. Technetium leachability is not as strongly dependent on the concentration of Tc in the waste, and it appears to be slightly more leachable by the Ca(OH)2-saturated solution than by the CaCO3-saturated solution. In general, Tc is much less leachable (<10 wt.% of the available mass in the waste) than previously predicted. This may be due to the coprecipitation of trace concentrations of Tc in relatively insoluble phases such as Fe oxide/hydroxide solids.  相似文献   

6.
The Dongping gold deposit hosted in syenites is one of the largest hydrothermal gold deposits in China and composed of ore veins in the upper parts and altered zones in the lower parts of the ore bodies. Pervasive potassic alteration and silicification overprint the wall rocks of the ore deposit. The alteration minerals include orthoclase, microcline, perthite, quartz, sericite, epidote, calcite, hematite and pyrite, with the quartz, pyrite and hematite assemblages closely associated with gold mineralization. The phases of hydrothermal alteration include: (i) potassic alteration, (ii) potassic alteration - silicification, (iii) silicification - epidotization - hematitization, (iv) silicification - sericitization - pyritization and (v) carbonation. Mass-balance calculations in potassic altered and silicified rocks reveal the gain of K2O, Na2O, SiO2, HFSEs and transition elements (TEs) and the loss of REEs. Most major elements were affected by intense mineral reactions, and the REE patterns of the ore are consistent with those of the syenites. Gold, silver and tellurium show positive correlation and close association with silicification. Fluid inclusion homogenization temperatures in quartz veins range from 154 °C to 382 °C (peak at 275 °C–325 °C), with salinities of 4–9 wt.% NaCl equiv. At temperatures of 325 °C the fluid is estimated to have pH = 3.70–5.86, log fO2 = − 32.4 to − 28.1, with Au and Te transported as Au (HS)2− and Te22 − complexes. The ore forming fluids evolved from high pH and fO2 at moderate temperatures into moderate-low pH, low fO2 and low temperature conditions. The fineness of the precipitated native gold and the contents of the oxide minerals (e.g., magnetite and hematite) decreased, followed by precipitation of Au- and Ag-bearing tellurides. The hydrothermal system was derived from an alkaline magma and the deposit is defined as an alkaline rock-hosted hydrothermal gold deposit.  相似文献   

7.
A sedimentary formation perturbated by supercritical CO2 reacts by dissolving primary minerals and forming new secondary phases. In this process CO2 may be trapped in stable carbonate minerals and may thereby be immobilized for long time spans. The potential for mineral trapping can be estimated by solving kinetic expressions for the reservoir minerals and possible secondary phases. This is, however, not trivial as kinetic data are uncertain or even lacking for the minerals of interest. Here, the rate equations most commonly used for CO2 storage simulations have been solved, and the rate parameters varied, to obtain sensitivity on the total amount of CO2 stored as mineral carbonate. As various expressions are in use to estimate growth rates of secondary carbonates, three formulations were compared, including one taking into account mineral nucleation preceding growth. The sensitivity studies were done on two systems, the Utsira Sand being representative for a cold quartz-rich sand (37 °C, 100 bar CO2), and the Gulf Coast Sediment, being representative for a medium temperature quartz–plagioclase-rich system (75 °C, 300 bar CO2).The simulations showed that the total predicted CO2 mineral storage is especially sensitive to the choice of growth rate model and the reactive surface area. The largest sensitivity was found on α, fraction of total surface area available for reactions, with a reduction of one order of magnitude for all reacting phases leading to 3–4 times lower predicted CO2 mineral storage. Because the reactive surface area is highly uncertain for natural systems, the range in predicted results may be even larger. The short-term predictions (<100–1000 a), such as the onset of carbonate growth, were highly sensitive to nucleation and growth rates. Moreover, the type of carbonate minerals formed was shown to be model dependent, with the simplest model predicting an unlikely carbonate assemblage at low temperature (i.e., formation of dolomite at 37 °C). Therefore, to use kinetic models to upscale short-term (<months) laboratory experiments in time, to identify the past reactions and physical conditions of natural CO2 storage analogues, and finally to predict the potential for CO2 trapping in existing and future storage projects, more knowledge has to be collected, especially on the reactive surface area of CO2 storage reservoirs, and on the rate of secondary carbonate nucleation and growth.  相似文献   

8.
The Yuchiling Mo deposit, East Qinling, China, belongs to a typical porphyry Mo system associated with high-K calc-alkaline intrusions. The pure CO2 (PC), CO2-bearing (C), aqueous H2O-NaCl (W), and daughter mineral-bearing (S) fluid inclusions were observed in the hydrothermal quartz. Based on field investigations, petrographic, microthermometric and LA-ICP-MS studies of fluid inclusions, we develop a five-stage fluid evolution model to understand the ore-forming processes of the Yuchiling deposit. The earliest barren quartz ± potassic feldspar veins, developed in intensively potassic alteration, were crystallized from carbonic-dominant fluids at high temperature (> 416 °C) and high pressure (> 133 MPa). Following the barren quartz ± potassic feldspar veins are quartz-pyrite veins occasionally containing minor K-feldspar and molybdenite, which were formed by immiscible fluids at pressures of 47–159 MPa and temperatures of 360–400 °C. The fluids were characterized by high CO2 contents (approximately 8 mol%) and variable salinities, as well as the highest Mo contents that resulted in the development of quartz-molybdenite veins. The quartz-molybdenite veins, accounting for > 90% Mo in the orebody, were also formed by immiscible fluids with lower salinity and lower CO2 content of 7 mol%, at temperatures of 340–380 °C and pressures of 39–137 MPa, as constrained by fluid inclusion assemblages. After the main Mo-mineralization, the uneconomic Cu-Pb-Zn mineralization occurred, as represented by quartz-polymetallic sulfides veins consisting of pyrite, molybdenite, chalcopyrite, digenite, galena, sphalerite and quartz. The quartz-polymetallic sulfide veins were formed by fluids containing 5 mol% CO2, with minimum pressures of 32–110 MPa and temperatures of 260–300 °C. Finally, the fluids became dilute (5 wt.% NaCl equiv) and CO2-poor, which caused the formation of late barren quartz ± carbonate ± fluorite veins at 140–180 °C and 18–82 MPa.It is clear that the fluids became more dilute, CO2-poor, and less fertile, with decreasing temperature and pressure from quartz-pyrite to late barren veins. Molybdenite and other sulfides can only be observed in the middle three stages, i.e., quartz-pyrite, quartz-molybdenite and quartz-polymetallic sulfide veins. These three kinds of veins are generally hosted in potassic altered rocks with remarkable K-feldspathization, but always partly overprinted by phyllic alteration. The traditional porphyry-style potassic–phyllic–propylitic alteration zoning is not conspicuous at Yuchiling, which may be related to, and characteristic of, the CO2-rich fluids derived from the magmas generated in intercontinental collision orogens.Among the fluid inclusions at Yuchiling, only the C-type contains maximum detectable Mo that gradationally decreases from 73 ppm in quartz-pyrite veins, through 19 ppm in quartz-molybdenite veins, and to 13 ppm in quartz-polymetallic sulfide veins, coinciding well with the decreasing CO2 contents from 8 mol%, through 7 mol%, to 5 mol%, respectively. Hence it is suggested that decreasing CO2 possibly results in decreasing Mo concentration in the fluids, as well as the precipitation of molybdenite from the fluids. This direct relationship might be a common characteristic for other porphyry Mo systems in the world.The Yuchiling Mo deposit represents a new type Mo mineralization, with features of collision-related setting, high-K calc-alkaline intrusion, CO2-rich fluid, and unique wall-rock alterations characterized by strong K-feldspathization and fluoritization.  相似文献   

9.
The Ulu Sokor gold deposit is one of the most famous and largest gold deposits in Malaysia and is located in the Central Gold Belt. This deposit consists of three major orebodies that are related to NS- and NE-striking fractures within fault zones in Permian-Triassic meta-sedimentary and volcanic rocks of the East Malaya Block. The faulting events represent different episodes that are related to each orebody and are correlated well with the mineralogy and paragenesis. The gold mineralization consists of quartz-dominant vein systems with sulfides and carbonates. The hydrothermal alteration and mineralization occurred during three stages that were characterized by (I) silicification and brecciation; (II) carbonatization, sericitization, and chloritization; and (III) quartz–carbonate veins.Fluid inclusions in the hydrothermal quartz and calcite of the three stages were studied. The primary CO2–CH4–H2O–NaCl fluid inclusions in stage I are mostly related to gold mineralization and display homogenization temperatures of 269–389 °C, salinities of 2.77–11.89 wt.% NaCl equivalent, variable CO2 contents (typically 5–29 mol%), and up to 15 mol% CH4. In stage II, gold was deposited at 235–398 °C from a CO2 ± CH4–H2O–NaCl fluid with a salinity of 0.83–9.28 wt.% NaCl equivalent, variable CO2 contents (typically 5–63 mol%), and up to 4 mol% CH4. The δ18OH2O and δD values of the ore-forming fluids from the stage II quartz veins are 4.5 to 4.8‰ and − 44 to − 42‰, respectively, and indicate a metamorphic–hydrothermal origin. Oxygen fugacities calculated for the entire range of T-P-XCO2 conditions yielded log fO2 values between − 28.95 and − 36.73 for stage I and between − 28.32 and − 39.18 for stage II. These values indicate reduced conditions for these fluids, which are consistent with the mineral paragenesis, fluid inclusion compositions, and isotope values.The presence of daughter mineral-bearing aqueous inclusions is interpreted to be a magmatic signature of stage IIIa. Combined with the oxygen and hydrogen isotopic compositions (δ18OH2O = 6.8 to 11.9‰, δD = − 77 to − 62‰), these inclusions indicate that the initial fluid was likely derived from a magmatic source. In stage IIIb, the gold was deposited at 263° to 347 °C from a CO2–CH4–H2O–NaCl fluid with a salinity of 5.33 to 11.05 wt.% NaCl equivalent, variable CO2 contents (typically 9–15 mol%), and little CH4. The oxygen and hydrogen isotopic compositions of this fluid (δ18OH2O = 8.1 to 8.8‰, δD = − 44 to − 32‰) indicate that it was mainly derived from a metamorphic–hydrothermal source. The CO2–H2O ± CH4–NaCl fluids that were responsible for gold deposition in the stage IIIc veins had a wide range of temperatures (214–483 °C), salinities of 1.02 to 21.34 wt.% NaCl equivalent, variable CO2 contents (typically 4–53 mol%), and up to 7 mol% CH4. The oxygen and hydrogen isotopic compositions (δ18OH2O = 8.5 to 9.8‰, δD = − 70 to − 58‰) were probably acquired at the site of deposition by mixing of the metamorphic–hydrothermal fluid with deep-seated magmatic water and then evolved by degassing at the site of deposition during mineralization. The log fO2 values from − 28.26 to − 35.51 also indicate reduced conditions for this fluid in stage IIIc. Moreover, this fluid had a near-neutral pH and δ34S values of H2S of − 2.32 to 0.83‰, which may reflect the derivation of sulfur from the subducted oceanic lithospheric materials.The three orebodies represent different gold transportation and precipitation models, and the conditions of ore formation are related to distinct events of hydrothermal alteration and gold mineralization. The gold mineralization of the Ulu Sokor deposit occurred in response to complex and concurrent processes involving fluid immiscibility, fluid–rock reactions, and fluid mixing. However, fluid immiscibility was the most important mechanism for gold deposition and occurred in these orebodies, which have corresponding fluid properties, structural controls, geologic characteristics, tectonic settings, and origins of the ore-forming matter. These characteristics of the Ulu Sokor deposit are consistent with its classification as an orogenic gold deposit, while some of the veins are genetically related to intrusions.  相似文献   

10.
The critical issue in the study of kimberlites, known as principal host rocks of diamonds, is the reconstruction of their primary melt composition, which is poorly constrained due to contamination by xenogenic materials, significant loss of volatiles during eruption, and post-magmatic alteration. It is generally accepted that the last equilibration of primary kimberlite melt with surrounding mantle (garnet lherzolite) occurred beneath cratons at 5–7 GPa (150–230 km depths). However, the subliquidus mineral assemblages obtained in kimberlite melting experiments at mantle pressures differ from lherzolite, probably owing to unaccounted loss of CO2. Here we present experiments at 6.5 GPa and 1200–1600 °C on unaltered kimberlite with an addition of 2–22 mol% CO2 over its natural abundance in the rock (13 mol%), but keeping proportions of other components identical to those in an exceptionally fresh anhydrous kimberlite from Udachnaya-East pipe in Siberia. We found that the partial melt achieves equilibrium with garnet lherzolite at 1500 °C and 19–23 mol% CO2 in the system. Under these conditions this melt contains (mol%): SiO2 = 9, FeO = 6–7, MgO = 23–26, CaO = 16, Na2O = 4, K2O = 1, and CO2 = 30–35. We propose, therefore, the alkali-rich carbonatitic composition of primary kimberlite melt and loss of 34–45 mol% (34–46 wt%) CO2 during ascent of the kimberlite magma to the surface.  相似文献   

11.
The main aim of this study was to assess the natural and anthropogenic contributions of CO2 in the urban atmosphere of Wrocław City (SW Poland) using combined quantitative (CO2 concentrations) and qualitative analysis (δ13C of CO2). Between 21 January 2011 and 22 December 2011, 17 sampling campaigns were performed at 3-week intervals and in total 255 samples were collected. The mean CO2 concentration was 469 ± 71 ppm and the mean δ13C(CO2) was −10.8 ± 1‰.The measured δ13C(CO2) values of major end-members for two winter heating seasons (−25.7‰ in January–March of 2011 and −27.6 ‰ in October–December of 2011) and for one vegetative season (−20.4‰ in April–September of 2011) suggest soil respiration as a main source of atmospheric CO2 during the vegetative season, and a very significant impact of fossil fuel combustion during the winter heating seasons. There were significant increases of CO2 concentrations at many sampling locations after the opening of a new motorway on 31 August 2011. The authors hypothesise that the new motorway contributes to the increase of CO2 across the city.  相似文献   

12.
The Shapinggou porphyry Mo deposit, one of the largest Mo deposits in Asia, is located in the Dabie Orogen, Central China. Hydrothermal alteration and mineralization at Shapinggou can be divided into four stages, i.e., stage 1 ore-barren quartz veins with intense silicification, followed by stage 2 quartz-molybdenite veins associated with potassic alteration, stage 3 quartz-polymetallic sulfide veins related to phyllic alteration, and stage 4 ore-barren quartz ± calcite ± pyrite veins with weak propylitization. Hydrothermal quartz mainly contains three types of fluid inclusions, namely, two-phase liquid-rich (type I), two- or three-phase gas-rich CO2-bearing (type II) and halite-bearing (type III) inclusions. The last two types of fluid inclusions are absent in stages 1 and 4. Type I inclusions in the silicic zone (stage 1) display homogenization temperatures of 340 to 550 °C, with salinities of 7.9–16.9 wt.% NaCl equivalent. Type II and coexisting type III inclusions in the potassic zone (stage 2), which hosts the main Mo orebodies, have homogenization temperatures of 240–440 °C and 240–450 °C, with salinities of 34.1–50.9 and 0.1–7.4 wt.% NaCl equivalent, respectively. Type II and coexisting type III inclusions in the phyllic zone (stage 3) display homogenization temperatures of 250–345 °C and 220–315 °C, with salinities of 0.2–6.5 and 32.9–39.3 wt.% NaCl equivalent, respectively. Type I inclusions in the propylitization zone (stage 4) display homogenization temperatures of 170 to 330 °C, with salinities lower than 6.5 wt.% NaCl equivalent. The abundant CO2-rich and coexisting halite-bearing fluid inclusion assemblages in the potassic and phyllic zones highlight the significance of intensive fluid boiling of a NaCl–CO2–H2O system in deep environments (up to 2.3 kbar) for giant porphyry Mo mineralization. Hydrogen and oxygen isotopic compositions indicate that ore-fluids were gradually evolved from magmatic to meteoric in origin. Sulfur and lead isotopes suggest that the ore-forming materials at Shapinggou are magmatic in origin. Re–Os dating of molybdenite gives a well-defined 187Re/187Os isochron with an age of 112.7 ± 1.8 Ma, suggesting a post-collisional setting.  相似文献   

13.
This paper contributes to the understanding of the genesis of epigenetic, hypogene BIF-hosted iron deposits situated in the eastern part of Ukrainian Shield. It presents new data from the Krivoy Rog iron mining district (Skelevatske–Magnetitove deposit, Frunze underground mine and Balka Severnaya Krasnaya outcrop) and focuses on the investigation of ore genesis through application of fluid inclusion petrography, microthermometry, Raman spectroscopy and baro-acoustic decrepitation of fluid inclusions. The study investigates inclusions preserved in quartz and magnetite associated with the low-grade iron ores (31–37% Fe) and iron-rich quartzites (38–45% Fe) of the Saksaganskaya Suite, as well as magnetite from the locally named high-grade iron ores (52–56% Fe). These high-grade ores resulted from alteration of iron quartzites in the Saksaganskiy thrust footwall (Saksaganskiy tectonic block) and were a precursor to supergene martite, high-grade ores (60–70% Fe). Based on the new data two stages of iron ore formation (metamorphic and metasomatic) are proposed.The metamorphic stage, resulting in formation of quartz veins within the low-grade iron ore and iron-rich quartzites, involved fluids of four different compositions: CO2-rich, H2O, H2O–CO2(± N2–CH4)–NaCl(± NaHCO3) and H2O–CO2(± N2–CH4)–NaCl. The salinities of these fluids were relatively low (up to 7 mass% NaCl equiv.) as these fluids were derived from dehydration and decarbonation of the BIF rocks, however the origin of the nahcolite (NaHCO3) remains unresolved. The minimum P–T conditions for the formation of these veins, inferred from microthermometry are Tmin = 219–246 °C and Pmin = 130–158 MPa. The baro-acoustic decrepitation analyses of magnetite bands indicated that the low-grade iron ore from the Skelevatske–Magnetitove deposit was metamorphosed at T = ~ 530 °C.The metasomatic stage post-dated and partially overlapped the metamorphic stage and led to the upgrade of iron quartzites to the high-grade iron ores. The genesis of these ores, which are located in the Saksaganskiy tectonic block (Saksaganskiy ore field), and the factors controlling iron ore-forming processes are highly controversial. According to the study of quartz-hosted fluid inclusions from the thrust zone the metasomatic stage involved at least three different episodes of the fluid flow, simultaneous with thrusting and deformation. During the 1st episode three types of fluids were introduced: CO2–CH4–N2(± C), CO2(± N2–CH4) and low salinity H2O–N2–CH4–NaCl (6.38–7.1 mass% NaCl equiv.). The 2nd episode included expulsion of the aqueous fluids H2O–N2–CH4–NaCl(± CO2, ± C) of moderate salinities (15.22–16.76 mass% NaCl equiv.), whereas the 3rd event involved high salinity fluids H2O–NaCl(± C) (20–35 mass% NaCl equiv.). The fluids most probably interacted with country rocks (e.g. schists) supplying them with CH4 and N2. The high salinity fluids were most likely either magmatic–hydrothermal fluids derived from the Saksaganskiy igneous body or heated basinal brines, and they may have caused pervasive leaching of Fe from metavolcanic and/or the BIF rocks. The baro-acoustic decrepitation analyses of magnetite comprising the high-grade iron ore showed formation T = ~ 430–500 °C. The fluid inclusion data suggest that the upgrade to high-grade Fe ores might be a result of the Krivoy Rog BIF alteration by multiple flows of structurally controlled, metamorphic and magmatic–hydrothermal fluids or heated basinal brines.  相似文献   

14.
We determined the rock types, the authigenic minerals, the paragenetic sequence, and the origin of dawsonite in pyroclastic rocks from the Yimin Formation of Beier Sag in the Hailar Basin, China. Dawsonite, a diagenetic mineral, is thought to result from a large influx of CO2 and, therefore, this system represents a natural analogue for in-situ mineral carbon storage. The studied host rocks are mainly tuffs/tuffaceous sandstones which now contain up to 70 vol% authigenic carbonates, including dawsonite, ankerite, and siderite. The initial alteration of the tuffs yielded minor siderite. Kaolinite, illite and mixed illite/smectite then formed as product phases. Dawsonite and quartz subsequently precipitated in response to CO2 influx apparently coupled to feldspar and perhaps kaolinte dissolution. Dawsonite reaches a maximum 25 vol% of the bulk rock. Mass balance suggests that this CO2 influx was coupled to the external import of sodium and export of SiO2. Ankerite and additional siderite precipitated during the late-stage alkaline diagenesis. The carbon isotope values of the dawsonite are in the range −4.1‰ to −2.2‰, indicating the magmatic origin of the CO2. Vitrinite reflectance and thermal gradient constraints suggest that the dawsonite at this location formed at a temperature of ∼75 °C.  相似文献   

15.
The Eastern Qinling, Central China, containing more than 20 Mesozoic porphyry ± skarn systems, is the most important Mo province in the world. The Shangfanggou giant Mo deposit, Luanchuan County, Henan Province, is a porphyry-skarn system hosted in a lithologic association comprising carbonaceous sandstone, shale, carbonate and chert within the Neoproterozoic Luanchuan Group. Mo ores are mainly altered porphyry, skarn and hornfels, with minor altered gabbro. The mineralization process includes four stages, potassic alteration of the porphyry and skarnization of dolomite marble in stage 1, stockworks of quartz + molybdenite ± sulfide (stage 2), pyrite + quartz ± sulfides (stage 3), and carbonate ± quartz ± fluorite (stage 4), respectively. Mo mineralization was generally associated with strong silicification and/or phyllic alteration. The fluid inclusions in minerals include three compositional types, i.e., CO2-bearing (C-type), aqueous (W-type) and daughter mineral-bearing (S-type). Minerals formed in stages 1 to 3 contain all the three types of FIs, but the stage 4 minerals only contain the W-type FIs. Oxides and Cu-phosphate are recognized as daughter minerals in S-type inclusions in minerals of stage 1, whereas the daughter sulfide and reducing gases such as CO, CH4, H2S and C2H6 can be observed in quartz of stages 2 and 3, suggesting that the ore-forming fluids were initially oxidizing and then evolved to reducing. Boiling fluid inclusion assemblages can be observed in minerals formed in stage 2 or earlier, but not in stage 3 or later. Fluid boiling caused CO2 escape, oxygen fugacity decrease and rapid precipitation of ore minerals, and was a key factor causing Mo-mineralization at Shangfanggou. Data and interpretations presented in this contribution show that the fluids forming the Shangfanggou Mo deposit evolved from CO2-rich, high-salinity hypothermal, to CO2-poor, low-salinity epithermal (low-T). The Mo mineralization at the Shangfanggou deposit mainly occurred at depth of 6.6–7.0 km, deeper than the majority of porphyry systems in volcanic arcs, which resulted from a CO2-rich magma–fluid system originating from partial melting of thickened lower crust. The Shangfanggou mineral system developed during 158–134 Ma when the Yangtze–North China continental collision began to evolve from compression to extension. Magmatic hydrothermal deposits developed in a continental collision regime are generally formed by CO2-rich, high-salinity fluids.  相似文献   

16.
Pristine diorite drill cores, obtained from the Äspö Hard Rock Laboratory (HRL, Sweden), were used to study the retention properties of fresh, anoxic crystalline rock material towards the redox-sensitive uranium. Batch sorption experiments and spectroscopic methods were applied for this study. The impact of various parameters, such as solid-to-liquid ratio (2–200 g/L), grain size (0.063–0.2 mm, 0.5–1 mm, 1–2 mm), temperature (room temperature and 10 °C), contact time (5–108 days), initial U(VI) concentration (3 × 10−9 to 6 × 10−5 M), and background electrolyte (synthetic Äspö groundwater and 0.1 M NaClO4) on the U(VI) sorption onto anoxic diorite was studied under anoxic conditions (N2). Comparatively, U(VI) sorption onto oxidized diorite material was studied under ambient atmosphere (pCO2 = 10−3.5 atm). Conventional distribution coefficients, Kd, and surface area normalized distribution coefficients, Ka, were determined. The Kd value for the U(VI) sorption onto anoxic diorite in synthetic Äspö groundwater under anoxic conditions by investigating the sorption isotherm amounts to 3.8 ± 0.6 L/kg which corresponds to Ka = 0.0030 ± 0.0005 cm (grain size 1–2 mm). This indicates a weak U sorption onto diorite which can be attributed to the occurrence of the neutral complex Ca2UO2(CO3)3(aq) in solution. This complex was verified as predominating U species in synthetic Äspö groundwater by time-resolved laser-induced fluorescence spectroscopy (TRLFS). Compared to U sorption at room temperature under anoxic conditions, U sorption is further reduced at decreased temperature (10 °C) and under ambient atmosphere. The U species in aqueous solution as well as sorbed on diorite were studied by in situ time-resolved attenuated total reflection Fourier-transform infrared (ATR FT-IR) spectroscopy. A predominant sorbing species containing a UO2(CO3)34− moiety was identified. The extent of U sorption onto diorite was found to depend more on the low sorption affinity of the Ca2UO2(CO3)3(aq) complex than on reduction processes of uranium.  相似文献   

17.
The Tongjing Cu–Au deposit is a medium-sized deposit within the Ningwu volcanic basin, east China, and is hosted by Cretaceous volcanic rocks of the Dawangshan and Niangniangshan Formations. The veined and lenticular Cu–Au orebodies are spatially and temporally related to the volcanic and subvolcanic rocks of the Niangniangshan Formation in the ore district. The wall-rock alteration is dominated by silicification, siderite alteration, carbonation, sericitization, chloritization, and kaolinization. On the basis of field evidence and petrographic observations, two stages of mineralization are recognized: (1) a siderite–quartz–sulfide stage (Stage 1) associated with the formation of chalcopyrite and pyrite in a quartz and siderite gangue; and (2) a quartz–bornite stage (Stage 2) cutting the Stage 1 phases. Stage 1 is the main mineralization stage. Quartz that formed in Stage 1 has δ18OH2O values of − 4.3‰ to 3.5‰ with δD values of fluid inclusion waters of − 97.1‰ to − 49.9‰, indicating that the ore-forming fluids were derived from early magmatic fluids and may have experienced oxygen isotopic exchange with meteoric water during Stage 1 mineralization.LA–MC–ICP–MS zircon U–Pb dating of the mineralization-related nosean-bearing phonolite and nosean-bearing phonolitic brecciated tuff at Tongjing yields ages of 129.8 ± 0.5 Ma and 128.9 ± 1.1 Ma, respectively. These results are interpreted as the crystallization age of the volcanic rocks of the Niangniangshan Formation. A hydrothermal sericite sample associated with Cu–Au mineralization at Tongjing yields a plateau 40Ar–39Ar age of 131.3 ± 1.3 Ma. These results confirm a genetic link between the volcanism and associated Cu–Au mineralization. The Tongjing Cu–Au deposit in the Ningwu basin is genetically and possibly tectonically similar to alkaline intrusion-related gold deposits elsewhere in the world.  相似文献   

18.
Small angle neutron scattering techniques have been applied to investigate the phase behavior of CO2 injected into coal and possible changes in the coal pore structure that may result from this injection. Three coals were selected for this study: the Seelyville coal from the Illinois Basin (Ro = 0.53%), Baralaba coal from the Bowen Basin (Ro = 0.67%), and Bulli 4 coal from the Sydney Basin (Ro = 1.42%). The coals were selected from different depths to represent the range of the underground CO2 conditions (from subcritical to supercritical) which may be realized in the deep subsurface environment. The experiments were conducted in a high pressure cell and CO2 was injected under a range of pressure conditions, including those corresponding to in-situ hydrostatic subsurface conditions for each coal. Our experiments indicate that the porous matrix of all coals remains essentially unchanged after exposure to CO2 at pressures up to 200 bar (1 bar = 105 Pa). Each coal responds differently to the CO2 exposure and this response appears to be different in pores of various sizes within the same coal. For the Seelyville coal at reservoir conditions (16 °C, 50 bar), CO2 condenses from a gas into liquid, which leads to increased average fluid density in the pores (ρpore) with sizes (r) 1 × 105 ≥ r ≥ 1 × 104 Å (ρpore ≈ 0.489 g/cm3) as well as in small pores with size between 30 and 300 Å (ρpore ≈ 0.671 g/cm3). These values are by a factor of three to four higher than the density of bulk CO2 (ρCO2) under similar thermodynamic conditions (ρCO2 ≈ 0.15 g/cm3). At the same time, in the intermediate size pores with r ≈ 1000 Å the average fluid density is similar to the density of bulk fluid, which indicates that adsorption does not occur in these pores. At in situ conditions for the Baralaba coal (35 OC, 100 bar), the average fluid density of CO2 in all pores is lower than that of the bulk fluid (ρpore / ρCO2 ≈ 0.6). Neutron scattering from the Bulli 4 coal did not show any significant variation with pressure, a phenomenon which we assign to the extremely small amount of porosity of this coal in the pore size range between 35 and 100,000 Å.  相似文献   

19.
The Wangfeng gold deposit is located in Western Tian Shan and the central section of the Central Asian Orogenic Belt (CAOB). The deposit is mainly hosted in Precambrian metamorphic rocks and Caledonian granites and is structurally controlled by the Shenglidaban ductile shear zone. The gold orebodies consist of gold-bearing quartz veins and altered mylonite. The mineralization can be divided into three stages: quartz–pyrite veins in the early stage, sulfide–quartz veins in the middle stage, and quartz–carbonate veins or veinlets in the late stage. Ore minerals and native gold mainly formed in the middle stage. Four types of fluid inclusions were identified based on petrography and laser Raman spectroscopy: CO2–H2O inclusions (C-type), pure CO2 inclusions (PC-type), NaCl–H2O inclusions (W-type), and daughter mineral-bearing inclusions (S-type). The early-stage quartz contains only primary CO2–H2O fluid inclusions with salinities of 1.62 to 8.03 wt.% NaCl equivalent, bulk densities of 0.73 to 0.89 g/cm3, and homogenization temperatures of 256 °C–390 °C. Vapor bubbles are composed of CO2. The middle-stage quartz contains all four types of fluid inclusions, of which the CO2–H2O and NaCl–H2O types yield homogenization temperatures of 210 °C–340 °C and 230 °C–300 °C, respectively. The CO2–H2O fluid inclusions have salinities of 0.83 to 9.59 wt.% NaCl equivalent and bulk densities of 0.77 to 0.95 g/cm3, with vapor bubbles composed of CO2, CH4, and N2. Fluid inclusions in the late-stage quartz are NaCl–H2O solution with low salinities (0.35–3.87 wt.% NaCl equivalent) and low homogenization temperatures (122 °C–214 °C). The coexistence of inclusions of these four types in middle-stage quartz suggests that fluid boiling occurred in the middle-stage mineralization. Trapping pressures estimated from CO2–H2O inclusions are 110–300 MPa and 90–250 MPa for the early and middle stages, respectively, suggesting that gold mineralization mainly occurred at depths of about 10 km. In general, the Wangfeng gold deposit originated from a metamorphic fluid system characterized by low salinity, low density, and enrichment of CO2. Depressurized fluid boiling caused gold precipitation. Given the regional geology, ore geology, fluid-inclusion features, and ore-forming age, the Wangfeng gold deposit can be classified as a hypozonal orogenic gold deposit.  相似文献   

20.
The Wang'ershan gold deposit, located in the southern Jiaojia goldfield, is currently the largest gold deposit hosted within the subsidiary faults in Jiaodong Peninsula, with a gold reserve of > 60 t gold at a grade of 4.07 g/t Au. It is hosted in the Late Jurassic Linglong biotite granites and controlled by the second-order, N- to NNE-trending Wang'ershan Fault (and its subsidiary faults) which is broadly parallel to the first-order Jiaojia Fault in the goldfield. Gold mineralization occurs as both disseminated- and stockwork-style and quartz–sulfide vein-style ores, mainly within altered cataclasites and breccias, and sericite–quartz and potassic alteration zones, respectively. Mineralization stages can be divided into (1) the pyrite–quartz–sericite stage, (2) the quartz–pyrite stage, (3) the quartz–sulfide stage, and (4) the quartz–carbonate stage.Two sericite samples associated with the main ore-stage pyrites from pyritic phyllic ores of the deposit with weighted mean plateau 40Ar/39Ar age of 120.7 ± 0.6 Ma and 119.2 ± 0.5 Ma, respectively, were selected for 40Ar/39Ar geochronology. On the basis of petrography and microthermometry, three types of primary fluid inclusions related to the ore forming event were identified: type 1 H2O–CO2–NaCl, type 2 aqueous, and type 3 CO2 fluid inclusions (in decreasing abundance). Stage 1 quartz contains all three primary fluid inclusions, while stages 2 and 3 quartz contain both type 1 and 2 inclusions, and stage 4 quartz contains only type 2 inclusions. The contemporaneous trapping, similar salinities and total homogenization temperature ranges, and different homogenization phases of type 1 and type 2 inclusions indicate that fluid immiscibility did take place in stages 1, 2 and 3 ores, with P–T conditions of 190 to 85 MPa and 334 to 300 °C for stage 1 and 200 to 40 MPa and 288 to 230 °C for stages 2 and 3. Combined with the H–O–C–S–Pb isotopic compositions, ore-forming fluids may have a metamorphic-dominant mixed source, which could be associated with the dehydration and decarbonisation of a subducting paleo-Pacific plate and characterized by medium–high temperature (285–350 °C), CO2-bearing (~ 8 mol%) with minor CH4 (1–4% in carbonic phase), and low salinity (3.38–8.45 eq. wt.% NaCl). During mineralization, the fluid finally evolved into a medium–low temperature NaCl–H2O system. Au(HS)2− was the most probable gold-transporting complex at Wang'ershan, due to the low temperature (157–350 °C) and near-neutral to weakly acidic ore fluids. The reaction between gold-bearing fluids and iron-bearing wall-rocks, and fluid-immiscibility processes caused via fluid–pressure cycling during seismic movement along fault zones that host lode-gold orebodies, which led to breakdown of Au(HS)2−, are interpreted as the two main precipitation mechanisms of gold deposition.In general, the Wang'ershan deposit and other deposits in the Jiaojia camp have concordant structural system and wall-rock alteration assemblages, nature of orebodies and gold occurrence conditions, as well as the similar geochronology, ore-forming fluids system and stable isotope compositions. Thus gold mineralization in the Jiaojia goldfield was a large-scale unified event, with consistent timing, origin, process and mechanism.  相似文献   

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