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1.
Among the risks of CO2 storage is the potential of CO2 leakage into overlaying formations and near-surface potable aquifers. Through a leakage, the CO2 can intrude into protected groundwater resources, which can lead to groundwater acidification followed by potential mobilisation of heavy metals and other trace metals through mineral dissolution or ion exchange processes. The prediction of pH buffer reactions in the formations overlaying a CO2 storage site is essential for assessing the impact of CO2 leakages in terms of trace metal mobilisation. For buffering the pH-value, calcite dissolution is one of the most important mechanisms. Although calcite dissolution has been studied for decades, experiments conducted under elevated CO2 partial pressures are rare. Here, the first study for column experiments is presented applying CO2 partial pressures from 6 to 43 bars and realising a near-natural flow regime. Geochemical calculations of calcite dissolution kinetics were conducted using PHREEQC together with different thermodynamic databases. Applying calcite surface areas, which were previously acquired by N2-BET or calculated based on grain diameters, respectively, to the rate laws according to Plummer et al. (Am J Sci 278:179–216, doi:10.2475/ajs.278.2.179, 1978) or Palandri and Kharaka (US Geol Surv Open file Rep 2004–1068:71, 2004) in the numerical simulations led to an overestimation of the calcite dissolution rate by up to three orders of magnitude compared to the results of the column experiments. Only reduction of the calcite surface area in the simulations as a fitting procedure allowed reproducing the experimental results. A reason may be that the diffusion boundary layer (DBL), which depends on the groundwater flow velocity and develops at the calcite grain surface separating it from the bulk of the solution, has to be regarded: The DBL leads to a decrease in the calcite dissolution rate under natural laminar flow conditions compared to turbulent mixing in traditional batch experiments. However, varying the rate constants by three orders of magnitudes in a field scale PHREEQC model simulating a CO2 leakage produced minor variations in the pH buffering through calcite dissolution. This justifies the use of equilibrium models when calculating the calcite dissolution in CO2 leakage scenarios for porous aquifers and slow or moderate groundwater flow velocities. However, the selection of the thermodynamic database has an impact on the dissolved calcium concentration, leading to an uncertainty in the simulation results. The resulting uncertainty, which applies also to the calculated propagation of an aquifer zone depleted in calcite through dissolution, seems negligible for shallow aquifers of approximately 60 m depth, but amounts to 35 % of the calcium concentration for aquifers at a depth of approximately 400 m.  相似文献   

2.
Hydrogeochemical processes that accompany seawater intrusion in coastal aquifers can alter the resulting water quality and are important ingredients in coastal aquifer management. The presence of dissolution–precipitation reactions and ion exchange in the mixing zone of the Biscayne aquifer (FL, USA) are suggested based on changes in major ion concentrations and mineral saturation indices (SI). Major ion concentrations from 11 groundwater samples are compared with theoretical mixing between freshwater and seawater. PHREEQC code was used to calculate saturation indices of the samples with respect to common phases in the Biscayne aquifer. High Ca2+ and HCO3 ? content of the samples is typical of waters in contact with carbonate aquifers. Water quality of the samples is mainly attributed to mixing and precipitation–dissolution reactions with calcite and dolomite. The samples were saturated with calcite (SI ~ 0) and undersaturated for dolomite (SI < 0), while a few samples showed dolomite saturation. Because gypsum and halite SI could be predicted by theoretical mixing, reactions with those minerals, if present, are thought to be insignificant. In the active intrusion areas, cation exchange also appears to modify water quality leading to excess Ca2+, but depleted Na+, Mg2+ and K+ concentrations. On the other hand, samples from previous intrusion areas plotted very close to the theoretical mixing line and approached equilibrium with the seawater.  相似文献   

3.
The injection of CO2 into deep saline aquifers is being considered as an option for greenhouse gas mitigation. However, the response of an aquifer to the injected CO2 is largely unknown. Experiments involving the reaction of Navajo Sandstone with acidic brine were conducted at 200°C and 25 or 30 MPa to evaluate the extent of fluid–rock interactions. The first experiment examined sandstone interaction with CO2-impregnated brine; the second experiment examined sandstone dissolution in CO2-free acidic brine; the third one is carried out in a mixed-flow reactor and designed to measure sandstone dissolution rates based on time-series Si concentrations. The solution chemistry data indicate that the SiO2(aq) increases gradually and pH increases slowly with reaction progress. Silicate minerals in the sandstone display textures (dissolution features, secondary mineralization), indicating that these phases are reacting strongly with the fluid. Dissolution of feldspars and conversion of smectite to illite are likely to be the two reactions that contribute to the release of SiO2(aq). The product minerals present at the end of the experiments are illite, illite/smectite, allophane, and carbonate minerals (for the CO2-charged system). Dissolved CO2 is likely to acidify the brine and to provide a source of carbon for the precipitation of carbonate minerals. Mineral trapping through the precipitation of carbonate minerals is favored thermodynamically and was observed in the experiments. The chemical reactions likely increase the bulk porosity of the sandstone due to dissolution of silicate minerals. However, allophane and illite/smectite fill voids in sandstone grains. There is no evidence for the removal of clay coatings due to chemical reactions. It is uncertain whether the mechanical forces near an injection well would mobilize the smectite and allophane and clog pore throats. Trace amounts of metals, including Cu, Zn, and Ba, were mobilized.  相似文献   

4.
The systematic sampling of the chemical composition of the groundwater from five karst springs (including an overflow spring) and one outflowing borehole have permitted to determine distinctive chemical changes in the waters that reflect the geochemical processes occurring in a carbonate aquifer system from southern Spain. The analysis of the dissolution parameters revealed that geochemical evolution of the karst waters basically depends on the availability of the minerals forming aquifer rocks and the residence time within the aquifers. In the three proposed scenarios in the aquifers, which include the preferential flow routines, the more important geochemical processes taking place during the groundwater flow from the recharge to the discharge zones are: CO2 dissolution and exsolution (outgassing), calcite net dissolution, calcite and dolomite sequential dissolution, gypsum/anhydrite and halite dissolution, de-dolomitization and calcite precipitation. A detailed analysis of the hydrochemical data set, saturation indices of the minerals and partial pressure of CO2 in the waters joined to the application of geochemical modelling methods allowed the elaboration of a hydrogeochemical model of the studied aquifers. The developed approach contributes to a better understanding of the karstification processes and the hydrogeological functioning of carbonate aquifers, the latter being a crucial aspect for the suitable management of the water resources.  相似文献   

5.
There are 59 springs at the Gevas–Gurp?nar–Güzelsu basins, 38 of these springs emerge from the fractured karst aquifers (recrystallized limestone and travertine) and 21 emerge from the Yuksekova ophiolites, K?rkgeçit formation and alluvium. The groundwater samples collected from 38 out of the total of 59 springs, two streams, one lake and 12 wells were analyzed physico-chemically in the year 2002. EC and TDS values of groundwater increased from the marble (high altitude) to the ophiolites and alluvium (toward Lake Van) as a result of carbonate dissolution and connate seawater. Five chemical types of groundwater are identified: Ca–Mg–HCO3, Mg–Ca–HCO3, Mg–Na–HCO3, Na–Ca–HCO3 and Mg–Ca–Na–HCO3. The calculations and hydrochemical interpretations show that the high concentrations of Ca2+, Mg2+ and HCO3 ? as predominant ions in the waters are mainly attributed to carbonate rocks and high pCO2 in soil. Most of the karst springs are oversaturated in calcite, aragonite and dolomite and undersaturated in gypsum, halite and anhydrite. The water–rock interaction processes that singly or in combination influence the chemical composition of each water type include dissolution of carbonate (calcite and dolomite), calcite precipitation, cation exchange and freshening of connate seawater. These processes contribute considerably to the concentration of major ions in the groundwater. Stable isotope contents of the groundwater suggest mainly direct integrative recharge.  相似文献   

6.
Geochemistry of soil, soil water, and soil gas was characterized in representative soil profiles of three Michigan watersheds. Because of differences in source regions, parent materials in the Upper Peninsula of Michigan (the Tahquamenon watershed) contain only silicates, while those in the Lower Peninsula (the Cheboygan and the Huron watersheds) have significant mixtures of silicate and carbonate minerals. These differences in soil mineralogy and climate conditions permit us to examine controls on carbonate and silicate mineral weathering rates and to better define the importance of silicate versus carbonate dissolution in the early stage of soil-water cation acquisition.Soil waters of the Tahquamenon watershed are the most dilute; solutes reflect amphibole and plagioclase dissolution along with significant contributions from atmospheric precipitation sources. Soil waters in the Cheboygan and the Huron watersheds begin their evolution as relatively dilute solutions dominated by silicate weathering in shallow carbonate-free soil horizons. Here, silicate dissolution is rapid and reaction rates dominantly are controlled by mineral abundances. In the deeper soil horizons, silicate dissolution slows down and soil-water chemistry is dominated by calcite and dolomite weathering, where solutions reach equilibrium with carbonate minerals within the soil profile. Thus, carbonate weathering intensities are dominantly controlled by annual precipitation, temperature and soil pCO2. Results of a conceptual model support these field observations, implying that dolomite and calcite are dissolving at a similar rate, and further dissolution of more soluble dolomite after calcite equilibrium produces higher dissolved inorganic carbon concentrations and a Mg2+/Ca2+ ratio of 0.4.Mass balance calculations show that overall, silicate minerals and atmospheric inputs generally contribute <10% of Ca2+ and Mg2+ in natural waters. Dolomite dissolution appears to be a major process, rivaling calcite dissolution as a control on divalent cation and inorganic carbon contents of soil waters. Furthermore, the fraction of Mg2+ derived from silicate mineral weathering is much smaller than most of the values previously estimated from riverine chemistry.  相似文献   

7.
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8.
The hydrogeochemistry and isotope geochemistry of groundwater from 85 wells in fractured dolomite aquifers of Central Slovenia were investigated. This groundwater represents waters strongly influenced by chemical weathering of dolomite with an average of δ13CCARB value of +2.2 ‰. The major groundwater geochemical composition is HCO3 ? > Ca2+ > Mg2+. Several differences in hydrogeochemical properties among the classes of dolomites were observed when they were divided based on their age and sedimentological properties, with a clear distinction of pure dolomites exhibiting high Mg2+/Ca2+ ratios and low Na+, K+ and Si values. Trace element and nutrient concentrations (SO4 2?, NO3 ?) were low, implying that karstic and fractured dolomite aquifers are of good quality to be used as tap water. Groundwater was generally slightly oversaturated with respect to calcite and dolomite, and dissolved CO2 was up to 46 times supersaturated relative to the atmosphere. The isotopic composition of oxygen (δ18OH2O), hydrogen (δDH2O) and tritium ranged from ?10.3 to ?8.4 ‰, from ?68.5 to ?52.7 ‰ and from 3.5 TU to 10.5 TU, respectively. δ18O and δD values fell between the GMWL (Global Meteoric Water Line) and the MMWL (Mediterranean Meteoric Water Line) and indicate recharge from precipitation with little evaporation. The tritium activity in groundwater suggests that groundwater is generally younger than 50 years. δ13CDIC values ranged from ?14.6 to ?9.3 ‰ and indicated groundwater with a contribution of degraded organic matter/dissolved inorganic carbon in the aquifer. The mass balances for groundwater interacting with carbonate rocks suggested that carbonate dissolution contributes from 43.7 to 65.4 % and degradation of organic matter from 34.6 to 56.3 %.  相似文献   

9.
The hydrogeochemical and carbon isotope characteristics of the Krka River, Slovenia, were investigated to estimate the carbon transfer from the land ecosystem in the watershed. During the 3-year sampling period (2008–2010), temperature, pH, electrical conductivity, major ion content, dissolved inorganic carbon (DIC) and dissolved organic carbon content, and the isotopic composition of DIC (δ13CDIC) were monitored in the main stream of the Krka River and its tributaries. The major solute composition of analysed waters is dominated by an input of HCO3 ?, Ca2+ and Mg2+ originating from carbonate dissolution. The Mg2+/Ca2+ and Mg2+/HCO3 ? molar ratio values ranging from 0.24 to 0.71 and 0.05 to 0.30, respectively, indicate a high degree of dolomite dissolution relative to calcite. Dissolved CO2 concentrations in the river were up to tenfold supersaturated relative to the atmosphere, resulting in supersaturation with respect to calcite and degassing of CO2 downstream. The δ13C values in river water range from ?15.6 to ?9.4 ‰ and are controlled by the input of tributaries, exchange with atmospheric CO2, degradation of organic matter, and dissolution of carbonates. The mass balance calculations for riverine DIC suggest that the contribution from carbonate dissolution and degradation of organic matter have major influence, whereas the exchange with atmospheric CO2 has minor influence on the inorganic carbon pool in the Krka River.  相似文献   

10.
The geochemical and isotopic composition of surface waters and groundwater in the Velenje Basin, Slovenia, was investigated seasonally to determine the relationship between major aquifers and surface waters, water–rock reactions, relative ages of groundwater, and biogeochemical processes. Groundwater in the Triassic aquifer is dominated by HCO3 –, Ca2+, Mg2+ and δ13CDIC indicating degradation of soil organic matter and dissolution of carbonate minerals, similar to surface waters. In addition, groundwater in the Triassic aquifer has δ18O and δD values that plot near surface waters on the local and global meteoric water lines, and detectable tritium, likely reflecting recent (<50 years) recharge. In contrast, groundwater in the Pliocene aquifers is enriched in Mg2+, Na+, Ca2+, K+, and Si, and has high alkalinity and δ13CDIC values, with low SO4 2– and NO3 – concentrations. These waters have likely been influenced by sulfate reduction and microbial methanogenesis associated with coal seams and dissolution of feldspars and Mg-rich clay minerals. Pliocene aquifer waters are also depleted in 18O and 2H, and have 3H concentrations near the detection limit, suggesting these waters are older, had a different recharge source, and have not mixed extensively with groundwater in the Triassic aquifer.  相似文献   

11.
《Geochimica et cosmochimica acta》1999,63(19-20):3133-3143
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12.
In assessing the feasibility of widespread deployment of CO2 geological storage, it is prudent to first assess potential consequences of an error or accident that could lead to CO2 leakage into groundwater resources above a sequestration interval. Information about the sensitivity of the groundwater system to introduction of CO2 is needed in order to design groundwater monitoring program. A laboratory-batch experiment was conducted to explore the range of CO2 impact on groundwater quality of a spectrum of representative aquifers, in the Gulf Coast region, USA. Results show that CO2 elevated concentrations of many cations within hours or days. Two types of cations were recognized according to their concentration trends. Type I cations—Ca, Mg, Si, K, Sr, Mn, Ba, Co, B, Zn—rapidly increased following initial CO2 flux and reached stable concentrations before the end of the experiment. Type II cations—Fe, Al, Mo, U, V, As, Cr, Cs, Rb, Ni and Cu—increased at the start of CO2 flux, but declined, in most cases, to levels lower than pre-CO2 concentrations. Dissolution of dolomite and calcite caused the largest increase in concentrations for Ca, Mg, Mn, Ba and Sr. Cation release rates decreased linearly as pH increased during mineral buffering. Experiment results suggest that carbonate minerals are the dominant contributor of changes in groundwater quality. Risk assessments of potential degradation of groundwater and monitoring strategies should focus on these fast-reacting minerals. Mobilization risk of Type II cations, however, may be self-mitigated because adsorption occurs when pH rebounds.  相似文献   

13.
An approach is presented to investigate the regional evolution of groundwater in the basin of the Amacuzac River in Central Mexico. The approach is based on groundwater flow cross-sectional modeling in combination with major ion chemistry and geochemical modeling, complemented with principal component and cluster analyses. The hydrogeologic units composing the basin, which combine aquifers and aquitards both in granular, fractured and karstic rocks, were represented in sections parallel to the regional groundwater flow. Steady-state cross-section numerical simulations aided in the conceptualization of the groundwater flow system through the basin and permitted estimation of bulk hydraulic conductivity values, recharge rates and residence times. Forty-five water locations (springs, groundwater wells and rivers) were sampled throughout the basin for chemical analysis of major ions. The modeled gravity-driven groundwater flow system satisfactorily reproduced field observations, whereas the main geochemical processes of groundwater in the basin are associated to the order and reactions in which the igneous and sedimentary rocks are encountered along the groundwater flow. Recharge water in the volcanic and volcano-sedimentary aquifers increases the concentration of HCO3 –, Mg2+ and Ca2+ from dissolution of plagioclase and olivine. Deeper groundwater flow encounters carbonate rocks, under closed CO2 conditions, and dissolves calcite and dolomite. When groundwater encounters gypsum lenses in the shallow Balsas Group or the deeper Huitzuco anhydrite, gypsum dissolution produces proportional increased concentration of Ca2+ and SO4 2–; two samples reflected the influence of hydrothermal fluids and probably halite dissolution. These geochemical trends are consistent with the principal component and cluster analyses.  相似文献   

14.
The assessment of the environmental impacts of CO2 geological storage requires the investigation of potential CO2 leakages into fresh groundwater, particularly with respect to protected groundwater resources. The geochemical processes and perturbations associated with a CO2 leak into fresh groundwater could alter groundwater quality: indeed, some of the reacting minerals may contain hazardous constituents, which might be released into groundwater. Since the geochemical reactions may occult direct evidence of intruding CO2, it is necessary to characterize these processes and identify possible indirect indicators for monitoring CO2 intrusion. The present study focuses on open questions: Can changes in water quality provide evidence of CO2 leakage? Which parameters can be used to assess impact on freshwater aquifers? What is the time scale of water chemistry degradation in the presence of CO2? The results of an experimental approach allow selecting pertinent isotope tracers as possible indirect indicators of CO2 presence, opening the way to devise an isotopic tracing tool.The study area is located in the Paris Basin (France), which contains deep saline formations identified as targets by French national programs for CO2 geological storage. The study focuses on the multi-layered Albian fresh water aquifer, confined in the central part of the Paris Basin a major strategic potable groundwater overlying the potential CO2 storage formations. An experimental approach (batch reactors) was carried out in order to better understand the rock–water–CO2 interactions with two main objectives. The first was to assess the evolution of the formation water chemistry and mineralogy of the solid phase over time during the interaction. The second concerned the design of an isotopic monitoring program for freshwater resources potentially affected by CO2 leakage. The main focus was to select suitable environmental isotope tracers to track water rock interaction associated with small quantities of CO2 leaking into freshwater aquifers.In order to improve knowledge on the Albian aquifer, and to provide representative samples for the experiments, solid and fluid sampling campaigns were performed throughout the Paris Basin. Albian groundwater is anoxic with high concentrations of Fe, a pH around 7 and a mineral content of 0.3 g L−1. Macroscopic and microscopic solid analyses showed a quartz-rich sand with the presence of illite/smectite, microcline, apatite and glauconite. A water–mineral–CO2 interaction batch experiment was used to investigate the geochemical evolution of the groundwater and the potential release of hazardous trace elements. It was complemented by a multi-isotope approach including δ13CDIC and 87Sr/86Sr. Here the evolution of the concentrations of major and trace elements and isotopic ratios over batch durations from 1 day to 1 month are discussed. Three types of ion behavior are observed: Type I features Ca, SiO2, HCO3, F, PO4, Na, Al, B, Co, K, Li, Mg, Mn, Ni, Pb, Sr, Zn which increased after initial CO2 influx. Type II comprises Be and Fe declining at the start of CO2 injection. Then, type III groups element with no variation during the experiments like Cl and SO4. The results of the multi-isotope approach show significant changes in isotopic ratios with time. The contribution of isotope and chemical data helps in understanding geochemical processes involved in the system. The isotopic systems used in this study are potential indirect indicators of CO2–water–rock interaction and could serve as monitoring tools of CO2 leakage into an aquifer overlying deep saline formations used for C sequestration and storage.  相似文献   

15.
In a mid-continental North American grassland, solute concentrations in shallow, limestone-hosted groundwater and adjacent surface water cycle annually and have increased steadily over the 15-year study period, 1991-2005, inclusive. Modeled groundwater CO2, verified by measurements of recent samples, increased from 10−2.05 atm to 10−1.94 atm, about a 20% increase, from 1991 to 2005. The measured groundwater alkalinity and alkaline-earth element concentrations also increased over that time period. We propose that carbonate minerals dissolve in response to lowered pH that occurs during an annual carbonate-mineral saturation cycle. The cycle starts with low saturation during late summer and autumn when dissolved CO2 is high. As dissolved CO2 decreases in the spring and early summer, carbonates become oversaturated, but oversaturation does not exceed the threshold for precipitation. We propose that groundwater is a CO2 sink through weathering of limestone: soil-generated CO2 is transformed to alkalinity through dissolution of calcite or dolomite. The annual cycle and long-term increase in shallow groundwater CO2 is similar to, but greater than, atmospheric CO2.  相似文献   

16.
A suite of terrestrial-marine transitional carbonate beds occur in the Lower Tertiary of the Kuqa Basin, Xinjiang. The pebbly coquina, Paleocene in age, is distributed along the southern pediment of the Tianshan Mountains north of Baicheng, where Pb-mineralization has been observed for the first time. The pebbly coquina consists of well-rounded quartzitic pebbles, quartz sands, shell fossils, shell fragments and equigranular fecal pellets. Four types of carbonate minerals have been revealed: 1) euhedral dolomite (Mg60Ca40)CO3, 2) anhedral dolomite (Mg57Ca43)CO3, 3) dolomitic calcite (Mg20Ca80)CO3 and magnesitic dolomite with a trace amount of Pb(Mg73Ca27)CO3. Five types of galena filling the pebbly coquina have been found: 1) in the shell tower end, 2) on the inner shell wall, 3) on the outer shell wall, 4) around the shell wall, and 5) among shell fragments. The galena replacement took place mainly in the early stage of diagenesis. Stable isotope analyses show (δ13C values range from −0.8 to +2.3 and δ18O values from −0.1 to +0.5, indicating a marine environment under the influence of fresh water, which is consistent with the result of megascopic facies analysis in paleogeography. It is concluded that the discovery of galena in the Tertiary pebbly coquina in the north of Baicheng, Xinjiang may provide new clues to the searching for strata-bound Pb-Zn deposits in the vast area of northern Tarim Basin.  相似文献   

17.
《Applied Geochemistry》2000,15(8):1085-1095
The pore space of deep saline aquifers in the Alberta (sedimentary) Basin offers a significant volume for waste storage by “hydrodynamic trapping”. Furthermore, given the slow regional fluid flow in these deep saline aquifers, ample time exists for waste-water/rock chemical reactions to take place. A geochemical computer model (PATHARC) was used to compute the interaction of industrial waste streams comprising CO2, H2SO4 and H2S with the minerals in typical carbonate and sandstone aquifers from the Alberta Basin. The results support the idea that these acids can be neutralized by such reactions and that new mineral products are formed, such as calcite, siderite, anhydrite/gypsum and pyrrhotite, thereby trapping the CO3, SO4 and S ions that are formed when the acid gases dissolve in the formation water. Siliciclastic aquifers appear to be a better host for “mineral trapping” than carbonate aquifers, especially with regard to CO2. Carbonate aquifers may be more prone to leakage due to high CO2 pressures generated by reaction with H2SO4 and H2S. Even though permeability decreases are expected due to this “mineral trapping”, they can be partially controlled so that plugging of the aquifer does not occur.  相似文献   

18.
 The Sanggok mine used to be one of the largest lead-zinc mines in the Hwanggangri mining district, Republic of Korea. The present study characterizes the heavy metal contamination in the abandoned Sanggok mine creek on the basis of physico-chemical properties of various kinds of water samples (mine, surface and groundwater). Hydrochemistry of the water samples is characterized by the relatively significant enrichment of Ca2+, HCO3 –, NO3 – and Cl– in the surface and groundwaters, whereas the mine water is relatively enriched in Ca2+, Mg2+, heavy metals, and HCO3 – and SO4 2–. The more polluted mine water has a lower pH and higher Eh, conductivity and TDS values. The concentrations of some toxic elements (Al, As, Cd, Cu, Fe, Mn, Pb, Se, Sr, Pb and Zn) are tens to hundreds of times higher in the mine water than in the unpolluted surface and groundwaters. However, most immobile toxic pollutants from the mine drainage were quickly removed from the surface water by the precipitation of Al and Fe oxyhydroxides. Geochemical modeling showed that potentially toxic heavy metals might exist largely in the forms of MSO4 2– and M2+ in the mine water. These metals in the surface and groundwaters could form M2+, CO3 2– and OH– complex ions. Computer simulation indicates that the saturation indices of albite, alunite, anhydrite, chlorite, fluorite, gypsum, halloysite and strontianite in the water samples are undersaturated and have progressively evolved toward the saturation condition. However, barite, calcite, chalcedony, dolomite, gibbsite, illite and quartz were in equilibrium, and only clay minerals were supersaturated. Ground and mine waters seemed to be in equilibrium with kaolinite field, but some surface water were in equilibrium with gibbsite and seceded from the stability field of quartz. This indicates that surface water samples in reaction with carbonate rocks would first equilibrate with carbonate minerals, then gibbsite to kaolinite. Investigations on water quality and environmental improvement of the severely polluted Sanggok creek, as well as remediation methods on the possible future pollution of the groundwater by the acid mine drainage from the abandoned metal mines, are urgently required. Received: 4 February 2000 · Accepted: 9 May 2000  相似文献   

19.
Acid mine drainage is a major source of water pollution in the Sarcheshmeh porphyry copper mine area. The concentrations of heavy metals and rare earth elements (REEs) in the host rocks, natural waters and acid mine drainage (AMD) associated with mining and tailing impoundments are determined. Contrary to the solid samples, AMDs and impacted stream waters are enriched in middle rare earth elements (MREEs) and heavy rare earth elements (HREEs) relative to light rare earth elements (LREEs). This behavior suggests that REE probably fractionate during sulfide oxidation and acid generation and subsequent transport, so that MREE and HREE are preferentially enriched. Speciation modeling predict that the dominant dissolved REE inorganic species are Ln3+, Ln(SO4)2−, LnSO4+, LnHCO32+, Ln(CO3)2− and LnCO3+. Compared to natural waters, Sarcheshmeh AMD is enriched in REEs and SO42−. High concentrations of SO42− lead to the formation of stable LnSO4+, thereby resulting in higher concentrations of REEs in AMD samples. The model indicates that LnSO4+ is the dissolved form of REE in acid waters, while carbonate and dicarbonate complexes are the most abundant dissolved REE species in alkaline waters. The speciation calculations indicate that other factors besides complexation of the REE's, such as release of MREE from dissolution and/or desorption processes in soluble salts and poorly crystalline iron oxyhydroxy sulfates as well as dissolution of host rock MREE-bearing minerals control the dissolved REE concentrations and, hence, the MREE-enriched patterns of acid mine waters.  相似文献   

20.
Compactional deformation facilitated replacement of dolomite and calcite by siderite and its subsequent oxidation in carbonate cemented red beds of the Triassic Buntsandstein in the Iberian Chain. Locally, the sedimentary clasts were cemented by carbonate that was derived from dissolution of locally exposed dolomite in the basement. Microstructures indicate that during sedimentation of the rocks, oxidizing conditions prevailed in the sediments and the basement was reddened by impregnation of hematite. Reducing conditions prevailed during deformation of the sediments. Ferric iron was reduced to Fe2+, that reacted with deformed dolomite and calcite cement to produce fine grained siderite. At a later stage, siderite crystallites were (partly) oxidized to form a secondary phase of brown ferric oxide (goethite). Locally, goethite transformed to fine grained hematite that caused secondary reddening of the sediments. The reactions are associated with a combined volume loss of the solid phases of c. 50% per reaction mol; this was accommodated by the formation of pores. Oxidation of siderite was associated with release of CO2; localized dissolution took place of feldspar and concurrently growth of kaolinite occurred by acidifying condition during release of CO2. The relation of redox reactions and deformation is comparable to those in red bed conglomerates in the region. Reductive dissolution occurred at sites of stress concentration, particularly at contact points of pebbles. Late stage precipitation of ferric oxides and pyrolusite took place at oxidizing conditions in association with uplift.  相似文献   

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