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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.
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3.
《Applied Geochemistry》2001,16(7-8):745-758
The physical–chemical characteristics of the groundwater in the Baza–Caniles detrital aquifer system indicate that a wide diversity of hydrochemical conditions exists in this semiarid region, defining geochemical zones with distinct groundwater types. The least mineralized water is found closest to the main recharge zones, and the salinity of the water increases significantly with depth towards the center of the basin. Geochemical reaction models have been constructed using water chemistry data along flow paths that characterize the different sectors of the aquifer system, namely: Quaternary aquifer, unconfined sector and shallow and deep confined sectors of the Mio–Pliocene aquifer. Geochemical mass–balance calculations indicate that the dominant groundwater reaction throughout the detrital system is dedolomitisation (dolomite dissolution and calcite precipitation driven by gypsum dissolution); this process is highly developed in the central part of the basin due to the abundance of evaporites. Apart from this process, there are others which influence the geochemical zoning of the system. In the Quaternary aquifer, which behaves as a system open to gases and which receives inputs of CO2 gas derived from the intensive farming in the area, the interaction of the CO2 with the carbonate matrix of the aquifer produces an increase in the alkalinity of the water. In the shallow confined sector of the Mio–Pliocene aquifer, the process of dedolomitisation evolves in a system closed to CO2 gas. Ca2+/Na+ cation exchange and halite dissolution processes are locally important, which gives rise to a relatively saline water. Finally, in the deep confined sector, a strongly reducing environment exists, in which the presence of H2S and NH+4 in the highly mineralized groundwater can be detected. In this geochemical zone, the groundwater system is considered to be closed to CO2 gas proceeding from external sources, but open to CO2 from oxidation of organic matter. The geochemical modeling indicates that the chemical characteristics of this saline water are mainly due to SO4 dissolution, dedolomitisation and SO4 reduction, coupled with microbial degradation of lignite.  相似文献   

4.
In a natural analog study of risks associated with carbon sequestration, impacts of CO2 on shallow groundwater quality have been measured in a sandstone aquifer in New Mexico, USA. Despite relatively high levels of dissolved CO2, originating from depth and producing geysering at one well, pH depression and consequent trace element mobility are relatively minor effects due to the buffering capacity of the aquifer. However, local contamination due to influx of brackish waters in a subset of wells is significant. Geochemical modeling of major ion concentrations suggests that high alkalinity and carbonate mineral dissolution buffers pH changes due to CO2 influx. Analysis of trends in dissolved trace elements, chloride, and CO2 reveal no evidence of in situ trace element mobilization. There is clear evidence, however, that As, U, and Pb are locally co-transported into the aquifer with CO2-rich brackish water. This study illustrates the role that local geochemical conditions will play in determining the effectiveness of monitoring strategies for CO2 leakage. For example, if buffering is significant, pH monitoring may not effectively detect CO2 leakage. This study also highlights potential complications that CO2 carrier fluids, such as brackish waters, pose in monitoring impacts of geologic sequestration.  相似文献   

5.
Evaluation of major ion chemistry and solute acquisition process controlling water chemical composition were studied by collecting a total of fifty-one groundwater samples in shallow (<25 m) and deep aquifer (>25 m) in the Varanasi area. Hydrochemical facies, Mg-HCO3 dominated in the largest part of shallow groundwater followed by Na-HCO3 and Ca-HCO3 whereas Ca-HCO3 is dominated in deep groundwater followed by Mg-HCO3 and Na-HCO3. High As concentration (>50 μg/l) is found in some of the villages situated in northeastern parts (i.e. adjacent to the concave part of the meandering Ganga river) of the Varanasi area. Arsenic contamination is confined mostly in tube wells (hand pump) within the Holocene newer alluvium deposits, whereas older alluvial aquifers are having arsenic free groundwater. Geochemical modeling using WATEQ4F enabled prediction of saturation state of minerals and indicated dissolution and precipitation reactions occurring in groundwater. Majority of shallow and deep groundwater samples of the study area are oversaturated with carbonate bearing minerals and under-saturated with respect to sulfur and amorphous silica bearing minerals. Sluggish hydraulic conductivity in shallow aquifer results in higher mineralization of groundwater than in deep aquifer. But the major processes in deep aquifer are leakage of shallow aquifer followed by dominant ion-exchange and weathering of silicate minerals.  相似文献   

6.
The unconfined High Plains (Ogallala) aquifer is the largest aquifer in the USA and the primary water supply for the semiarid southern High Plains of Texas and New Mexico. Analyses of water and soils northeast of Amarillo, Texas, together with data from other regional studies, indicate that processes during recharge control the composition of unconfined groundwater in the northern half of the southern High Plains. Solute and isotopic data are consistent with a sequence of episodic precipitation, concentration of solutes in upland soils by evapotranspiration, runoff, and infiltration beneath playas and ditches (modified locally by return flow of wastewater and irrigation tailwater). Plausible reactions during recharge include oxidation of organic matter, dissolution and exsolution of CO2, dissolution of CaCO3, silicate weathering, and cation exchange. Si and 14C data suggest leakage from perched aquifers to the High Plains aquifer. Plausible mass-balance models for the High Plains aquifer include scenarios of flow with leakage but not reactions, flow with reactions but not leakage, and flow with neither reactions nor leakage. Mechanisms of recharge and chemical evolution delineated in this study agree with those noted for other aquifers in the south-central and southwestern USA. Electronic Publication  相似文献   

7.
Two sediment cores retrieved at the northern slope of Sakhalin Island, Sea of Okhotsk, were analyzed for biogenic opal, organic carbon, carbonate, sulfur, major element concentrations, mineral contents, and dissolved substances including nutrients, sulfate, methane, major cations, humic substances, and total alkalinity. Down-core trends in mineral abundance suggest that plagioclase feldspars and other reactive silicate phases (olivine, pyroxene, volcanic ash) are transformed into smectite in the methanogenic sediment sections. The element ratios Na/Al, Mg/Al, and Ca/Al in the solid phase decrease with sediment depth indicating a loss of mobile cations with depth and producing a significant down-core increase in the chemical index of alteration. Pore waters separated from the sediment cores are highly enriched in dissolved magnesium, total alkalinity, humic substances, and boron. The high contents of dissolved organic carbon in the deeper methanogenic sediment sections (50-150 mg dm−3) may promote the dissolution of silicate phases through complexation of Al3+ and other structure-building cations. A non-steady state transport-reaction model was developed and applied to evaluate the down-core trends observed in the solid and dissolved phases. Dissolved Mg and total alkalinity were used to track the in-situ rates of marine silicate weathering since thermodynamic equilibrium calculations showed that these tracers are not affected by ion exchange processes with sediment surfaces. The modeling showed that silicate weathering is limited to the deeper methanogenic sediment section whereas reverse weathering was the dominant process in the overlying surface sediments. Depth-integrated rates of marine silicate weathering in methanogenic sediments derived from the model (81.4-99.2 mmol CO2 m−2 year−1) are lower than the marine weathering rates calculated from the solid phase data (198-245 mmol CO2 m−2 year−1) suggesting a decrease in marine weathering over time. The production of CO2 through reverse weathering in surface sediments (4.22-15.0 mmol CO2 m−2 year−1) is about one order of magnitude smaller than the weathering-induced CO2 consumption in the underlying sediments. The evaluation of pore water data from other continental margin sites shows that silicate weathering is a common process in methanogenic sediments. The global rate of CO2 consumption through marine silicate weathering estimated here as 5-20 Tmol CO2 year−1 is as high as the global rate of continental silicate weathering.  相似文献   

8.
It is challenging to predict the degree to which shallow groundwater might be affected by leaks from a CO2 sequestration reservoir, particularly over long time scales and large spatial scales. In this study observations at a CO2 enriched shallow aquifer natural analog were used to develop a predictive model which is then used to simulate leakage scenarios. This natural analog provides the opportunity to make direct field observations of groundwater chemistry in the presence of elevated CO2, to collect aquifer samples and expose them to CO2 under controlled conditions in the laboratory, and to test the ability of multi-phase reactive transport models to reproduce measured geochemical trends at the field-scale. The field observations suggest that brackish water entrained with the upwelling CO2 are a more significant source of trace metals than in situ mobilization of metals due to exposure to CO2. The study focuses on a single trace metal of concern at this site: U. Experimental results indicate that cation exchange/adsorption and dissolution/precipitation of calcite containing trace amounts of U are important reactions controlling U in groundwater at this site, and that the amount of U associated with calcite is fairly well constrained. Simulations incorporating these results into a 3-D multi-phase reactive transport model are able to reproduce the measured ranges and trends between pH, pCO2, Ca, total C, U and Cl− at the field site. Although the true fluxes at the natural analog site are unknown, the cumulative CO2 flux inferred from these simulations are approximately equivalent to 37.8E−3 MT, approximately corresponding to a .001% leak rate for injection at a large (750 MW) power plant. The leakage scenario simulations suggest that if the leak only persists for a short time the volume of aquifer contaminated by CO2-induced mobilization of U will be relatively small, yet persistent over 100 a.  相似文献   

9.
Patchy occurrences of elevated As are often encountered in groundwater from the shallow aquifers (<50 m) of the Bengal Delta Plain (BDP). A clear understanding of various biogeochemical processes, responsible for As mobilization, is very important to explain this patchy occurrence and thus to mitigate the problem. The present study deals with the periodical monitoring of groundwater quality of five nested piezometeric wells between December 2008 and July 2009 to investigate the temporal changes in groundwater chemistry vis-a-vis the prevalent redox processes in the aquifer. Geochemical modeling has been carried out to identify key phases present in groundwater. A correlation study among different aqueous redox parameters has also been performed to evaluate prevailing redox processes in the aquifer. The long term monitoring of hydrochemical parameters in the multilevel wells together with hydrogeochemical equilibrium modeling has shown more subtle differences in the geochemical environment of the aquifer, which control the occurrence of high dissolved As in BDP groundwater. The groundwater is generally of Ca-HCO3 type. The dissolved As concentration in groundwater exceeded both WHO and National drinking water standard (Bureau of Indian Standards; BIS, 10 μg L−1) throughout the sampling period. The speciation of As and Fe indicate persistent reducing conditions within the aquifer [As(III): 87-97% of AsT and Fe(II): 76-96% of FeT]. The concentration of major aqueous solutes is relatively high in the shallow aquifer (wells A and B) and gradually decreases with increasing depth in most cases. The calculation of SI indicates that groundwater in the shallow aquifer is also relatively more saturated with carbonate minerals. This suggests that carbonate mineral dissolution is possibly influencing the groundwater chemistry and thereby controlling the mobilization of As in the monitored shallow aquifer. Hydrogeochemical investigation further suggests that Fe and/or Mn oxyhydroxide reduction is the principal process of As release in groundwater from deeper screened piezometric wells. The positive correlations of U and V with As, Fe and Mn indicate redox processes responsible for mobilization of As in the deeper screened piezometric wells are possibly microbially mediated. Thus, the study advocates that mobilization of As is depth dependent and concentrations of As in groundwater depends on single/combined release mechanisms.  相似文献   

10.
《Applied Geochemistry》2002,17(8):1047-1060
Due to the scarcity of water resources in semiarid sedimentary basins, hill reservoirs are often constructed to recharge groundwater and limit runoff induced water loss. The impact of such reservoirs on groundwater chemistry is investigated in the aquifers of the El Gouazine watershed, Central Tunisia. Three groundwater types are recognised, Ca–HCO3, Na–Cl and Ca–SO4. The strong similarity between host rock and groundwater chemistries indicates significant rock–water interaction. A flowpath, along which the chemical composition of the groundwater evolves, can be identified using the contrast in stable isotope signature between upstream and downstream groundwater. Shallow upstream groundwater is recharged by the infiltration of rainwater with the rate of recharge strongly linked to the permeability of the host lithology. Calcium and HCO3 are supplied to an alluvial aquifer from a more rapidly recharged limestone aquifer with the concentration of Ca and HCO3 ions decreasing by dilution. The alluvial aquifer is also enriched in Ca and SO4 during the downstream flow of groundwater through gypsiferous materials. There is evidence of mixing between meteoric groundwater and evaporated reservoir water. Below the reservoir and partly responsible for reservoir leakage is a sandy aquifer, formed by weathering and erosion of a sandstone host which also supplies water to the alluvial aquifer.  相似文献   

11.

Tamborine Mountain, Queensland (Australia), is a prime example of a basalt fractured-rock aquifer. Yet very little is known about the hydrochemistry of this groundwater system. Both analytical (major ions and stable isotopes) and multivariate (hierarchical cluster analysis, principal component analysis and factor analysis) analyses were used in this study to investigate the factors that interact within this aquifer system, in order to determine groundwater hydrogeochemistry. A new approach was applied to the data by classifying hydrographs by water type to clearly identify differing aquifer zones. Three distinct groundwater chemistry types were identified, and they were differentiated by variations in depth. Shallow bores were dominated by Na–Cl waters, deep bores were dominated by Na–HCO3 and Ca–HCO3 waters, and the two deepest bores were dominated by mixed water types. The evaluation of hydrogeochemical data has determined that both mineral weathering processes and groundwater/surface-water interaction had a strong influence on the hydrogeochemistry. Seasonal effects were minimal in the study area based on physicochemical parameters and ion chemistry. However, stable isotopic data show temporal trends. Increased rainfall events during the wet season produced a depletion in δ18O and increased d-excess values. The opposite is found during the dry season as a result of higher evaporation rates that are not hindered by intense rainfall events.

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12.
Fifty-seven shallow groundwater samples were collected from Guiyang karst basin, China, to analyze the aqueous rare-earth elements in low-water seasons and it is shown that the total amount of rare-earth elements (ΣREE) in karst groundwater is exceedingly low compared with that in carbonate rocks or weathering crusts of carbonate rocks, and ranges from 0.01 to 0.43, from 0.03 to 0.27, from 0.03 to 0.19 and from 0.05 to 1.38 μg·L-1 for dolomite, dolomitic & limestone, limestone and clastic rock aquifer, respectively. Both distributions and contents of rare-earth elements (REE) in karst groundwater reflect the lithology of host rocks or weathering crusts of carbonate rocks through which groundwater flows. The chondrite-normalized patterns show a non-flat profile with higher enrichment of slightly light rare-earth elements (LREE) than heavy rare-earth elements (HREE), prominent fractionation between LREE and HREE, negative Ce anomalies and negative or positive Eu anomalies. There is more obvious fractionation between LREE and HREE in groundwater than that in carbonate rocks and their weathering crusts due to high contents of HCO3? and PH in groundwater. In shallow karst groundwater, REE(CO3)n2n-3 (n=1 and 2) is the main inorganic species of REE. But for a clastic rock aquifer, both REESO4+ and REECO3+ are the main inorganic species of REE. Species of REE in groundwater is closely associated with the hydrochemical type of groundwater which is predominated by the lithology of host rocks, groundwater-rock interaction and weathering-pedogenesis of carbonate rocks.  相似文献   

13.
The Lower Triassic Buntsandstein in Central Germany comprises one of the major clastic, lithified hydrocarbon reservoirs, it is a major groundwater aquifer and it is considered as a potential underground gas storage lithology. Thus, sandstones of the Buntsandstein from Thuringia and NE Hesse were used to analyse their geochemical composition combined with mineralogical data in order to investigate the origin of several bleaching phenomena in primary red beds, since these give a hint for mineral alteration, mineral formation and mineral reactivity in the course of fluid-rock-interactions. This is relevant for e.g. recent Carbon Capture and Storage (CCS) efforts. The origin of the observed bleaching phenomena is diverse and it is linked to certain stages of diagenesis and different episodes of fluid flow: (1) eodiagenetic bleaching coupled with palaeosoil formation and iron mobilisation, (2) mesodiagenetic bleaching as a result of hydrocarbon migration, (3) Tertiary bleaching due to CO2 degassing from Miocene volcanism, (4) Tertiary telodiagenetic bleaching due to weathering under humid climate conditions, and (5) weathering processes related to recent telodiagenesis/pedogenesis. This study emphasizes the multiple nature of fluids, which can induce iron mobilisation and bleaching of red beds.  相似文献   

14.
Potential pathways in the subsurface may allow upwardly migrating gaseous CO2 from deep geological storage formations to be released into near surface aquifers. Consequently, the availability of adequate methods for monitoring potential CO2 releases in both deep geological formations and the shallow subsurface is a prerequisite for the deployment of Carbon Capture and Storage technology. Geoelectrical surveys are carried out for monitoring a small-scale and temporally limited CO2 injection experiment in a pristine shallow aquifer system. Additionally, the feasibility of multiphase modeling was tested in order to describe both complex non-linear multiphase flow processes and the electrical behavior of partially saturated heterogeneous porous media. The suitability of geoelectrical methods for monitoring injected CO2 and geochemically altered groundwater was proven. At the test site, geoelectrical measurements reveal significant variations in electrical conductivity in the order of 15?C30?%. However, site-specific conditions (e.g., geological settings, groundwater composition) significantly influence variations in subsurface electrical conductivity and consequently, the feasibility of geoelectrical monitoring. The monitoring results provided initial information concerning gaseous CO2 migration and accumulation processes. Geoelectrical monitoring, in combination with multiphase modeling, was identified as a useful tool for understanding gas phase migration and mass transfer processes that occur due to CO2 intrusions in shallow aquifer systems.  相似文献   

15.

The Biscayne Aquifer (Florida, USA) is a coastal, shallow, unconfined, and heterogeneous aquifer with high water tables, composed of less-permeable sand to highly permeable karstic limestone. These properties make the Biscayne Aquifer one of the world’s most productive groundwater resources. The aquifer’s high yield and non-Darcian flow cause challenges for estimating aquifer parameters, which are essential for understanding groundwater processes and managing and protecting the groundwater resources. Water-table fluctuations in the Biscayne Aquifer are associated with astronomical tidal forces and gate operations on canal water-control structures. Analysis of observed groundwater level fluctuations can provide an understanding of the connectivity between the aquifer, Biscayne Bay, and the water level in the canals. Further, groundwater level fluctuations can be used for aquifer parameter estimation. In this research, observed ocean water levels measured at tidal stations and groundwater levels are fitted to Jacob’s analytical solution, where the amplitude of the groundwater head fluctuation decreases exponentially, and the time lag increases with distance from the shore. Observed groundwater levels were obtained from monitoring wells along the Miami-Dade shore and the barrier island of Miami Beach. Results indicate that Jacob’s solution is effective for aquifer parameter estimation in Miami Beach, where monitoring wells are closer to the shore. Estimated hydraulic conductivity appears to increase by four orders of magnitude to approximately 1 m s–1 as the distance from shore increases. Constructing monitoring wells closer to the shore in Miami-Dade County and elsewhere would permit improved aquifer parameter estimation and support enhanced groundwater modeling efforts.

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16.
Elevated As concentrations in groundwater of the Huhhot basin (HB), Inner Mongolia, China, and the western Bengal basin (WBB), India, have been known for decades. However, few studies have been performed to comprehend the processes controlling overall groundwater chemistry in the HB. In this study, the controls on solute chemistry in the HB have been interpreted and compared with the well-studied WBB, which has a very different climate, physiography, lithology, and aquifer characteristics than the HB. In general, there are marked differences in solute chemistry between HB and WBB groundwaters. Stable isotopic signatures indicate meteoric recharge in the HB in a colder climate, distant from the source of moisture, in comparison to the warm, humid WBB. The major-ion composition of the moderately reducing HB groundwater is dominated by a mixed-ion (Ca–Na–HCO3–Cl) hydrochemical facies with an evolutionary trend along the regional hydraulic gradient. Molar ratios and thermodynamic calculations show that HB groundwater has not been affected by cation exchange, but is dominated by weathering of feldspars (allitization) and equilibrium with gibbsite and anorthite. Mineral weathering and mobilization of As could occur as recharging water flows through fractured, argillaceous, metamorphic or volcanic rocks in the adjoining mountain-front areas, and deposits solutes near the center of the basin. In contrast, WBB groundwater is Ca–HCO3-dominated, indicative of calcite weathering, with some cation exchange and silicate weathering (monosiallitization).  相似文献   

17.
A regional scale hydrogeochemical study of a ∼21,000-km2 area in the western Bengal basin shows the presence of hydrochemically distinct water bodies in the main semiconfined aquifer and deeper isolated aquifers. Spatial trends of solutes and geochemical modeling indicate that carbonate dissolution, silicate weathering, and cation exchange control the major-ion chemistry of groundwater and river water. The main aquifer water has also evolved by mixing with seawater from the Bay of Bengal and connate water. The isolated aquifers contain diagenetically altered water of probable marine origin. The postoxic main aquifer water exhibits overlapping redox zones (metal-reducing, sulfidic and methanogenic), indicative of partial redox equilibrium, with the possibility of oxidation in micro-scale environments. The redox processes are depth-dependent and hydrostratigraphically variable. Elevated dissolved As in the groundwater is possibly related to Fe(III) reduction, but is strongly influenced by coupled Fe–S–C redox cycles. Arsenic does not show good correlations with most solutes, suggesting involvement of multiple processes in As mobilization. The main river in the area, the Bhagirathi–Hoogly, is chemically distinctive from other streams in the vicinity and probably has little or no influence on deep groundwater chemistry. Arsenic in water of smaller streams (Jalangi and Ichamati) is probably introduced by groundwater discharge during the dry season.  相似文献   

18.
Kinmen Island is principally composed of low permeable granitoid and covered by a very thin sedimentary layer. Both surface and groundwater resources are limited and water demand is increasing with time. The groundwater in the granitoid has been surveyed as an alternative water source for daily use. Two to five highly fractured zones in the granitoid aquifer for each site were first determined by geochemical well logging. Accordingly, ten samples were collected from three sites. Using environmental isotopes and geochemical modeling, geochemical processes occurring due to water–rock interaction in the granitoid aquifer can be quantitatively interpreted. The stable isotopes of oxygen and hydrogen in groundwaters cluster along Taiwan’s local meteoric waterline, indicating evaporation does not have considerable effect on groundwaters. Given such a high evaporation rate for Kinmen Island, this result implies that infiltration rate of groundwater is high enough to reduce retention time through a well-developed fracture zone. NetpathXL is employed for inverse geochemical modeling. Results determine gypsum as being the major source of sulfate for deep groundwaters. The contribution from pyrite is minor. In addition, the weathering of albite to kaolinite is the dominant water–rock interaction characterizing geochemical compositions of deep groundwater in Kinmen Island.  相似文献   

19.
The Northern Basque Country (Southwestern France) is subject to a constant need of increasing water due to a rising population. The fissured aquifer of the Ursuya Mount is one of the main water supplies able to meet these needs. Unfortunately, there is a lack of knowledge on the residence time of groundwater and flow pattern in this strategic resource. Geochemical monitoring of groundwater was carried out from 2009 to 2011 in conjunction with CFC–SF6 measurement and with a detailed geological field characterization. It appears that groundwater flows and water geochemistry are conditioned by the development of a weathered layer overlying the fissured aquifer. When the weathered layer is absent, groundwater flows take place in unconfined conditions along fractures and fissures. The rapid circulation (mean residence time between 11 and 15 a) and the low solubility of the matrix generates low mineralization (mean about 61 μS cm−1). When a weathered layer is present, the flow depends on the degree of weathering, with groundwater circulating in the deep fissured zone in the case of a high degree of weathering. The apparent age is then between 10 and 42 a and the mineralization tends to increase concomitantly with the residence time, and particularly terrigenic element concentrations. In the case of a lesser degree of weathering, mixing between recent water from the shallow weathered layer and the oldest water (25 to >50 a) from the underlying fissured aquifer is observed. These results allow the definition of a conceptual model of flow characteristics in the study area which is also applicable to other weathered–fractured systems worldwide.  相似文献   

20.
The major ionic and dissolved inorganic carbon (DIC) concentrations and the stable carbon isotope composition of DIC (δ13CDIC) were measured in a freshwater aquifer contaminated by produced water brine with petroleum hydrocarbons. Our aim was to determine the effects of produced water brine contamination on the carbonate evolution of groundwater. The groundwater was characterized by three distinct anion facies: HCO3−-rich, SO42−-rich and Cl−-rich. The HCO3−-rich groundwater is undergoing closed system carbonate evolution from soil CO2(g) and weathering of aquifer carbonates. The SO42−-rich groundwater evolves from gypsum induced dedolomitization and pyrite oxidation. The Cl−-rich groundwater is contaminated by produced water brine and undergoes common ion induced carbonate precipitation. The δ13CDIC of the HCO3−-rich groundwater was controlled by nearly equal contribution of carbon from soil CO2(g) and the aquifer carbonates, such that the δ13C of carbon added to the groundwater was −11.6‰. In the SO42−-rich groundwater, gypsum induced dedolomitization increased the 13C such that the δ13C of carbon added to the groundwater was −9.4‰. In the produced water brine contaminated Cl−-rich groundwater, common ion induced precipitation of calcite depleted the 13C such that the δ13C of carbon added to the groundwater was −12.7‰. The results of this study demonstrate that produced water brine contamination of fresh groundwater in carbonate aquifers alters the carbonate and carbon isotopic evolution.  相似文献   

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