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1.
Groundwater is an important and often exclusive water resource in arid and semi-arid regions. The aim of the present paper was to gain insight into the processes and conditions that control the deterioration of groundwater quality in the semi-arid Kalahari of Botswana. Measurements of 3He, 4He, 20Ne, 22Ne, and of 14C of dissolved inorganic carbon (DIC) were combined with existing isotopic and hydrochemical data to investigate groundwater from the Ntane Sandstone Aquifer, which is affected by high nitrate concentrations of non-anthropogenic origin. All groundwater samples revealed neon concentrations in excess to air-saturated water, which we attributed to the addition of excess air during recharge. Neon concentrations ranged from values close to air saturation for 14C DIC rich samples (up to 80.5%MC) up to values of 90% in excess to air-saturated water for lower 14C DIC contents (2.6-61.3%MC). A strong linear correlation of excess Ne with nitrate concentrations suggests an intimate connection between groundwater quality and the processes and conditions during groundwater recharge. Low groundwater recharge rates under present-day semi-arid conditions are associated with low amounts of excess Ne and elevated nitrate concentrations. In contrast to this, higher excess Ne values in groundwater of lower 14C DIC and nitrate contents indicate that the high quality groundwater end-member presumably is related to higher groundwater table fluctuations during wetter climatic conditions in the past. We attribute the decline in groundwater quality with respect to nitrate to a decreasing rate and temporal variability of groundwater recharge, and to concurrent changes in biogeochemical activities following a transition to a drier climate during the Holocene. Under such conditions, a much stronger decrease in groundwater recharge compared to the release of nitrate from soil organic matter may result in elevated nitrate concentrations in the vadose zone and groundwater. This implies a strong impact of climate change on the transport of solutes like nitrate through the vadose zone which needs to be considered in predictions of future groundwater quality.  相似文献   

2.
《Applied Geochemistry》1993,8(5):483-493
Information regarding the origin, composition and transport of natural dissolved organic carbon (DOC) in groundwater is necessary to understand the transport of metals and organic pollutants, as well as for the use of14C in DOC as an isotopic groundwater dating method. Previous research in several groundwater systems has suggested soil organic C is the predominant source of high molecular weight DOC to the subsurface. Through the use of stable isotopes,14C and geochemical analyses, this study shows that significant concentrations of DOC and CH4 in a regional confined aquifer can be generated in situ from subsurface sedimentary organic sources. The DOC and CH4 produced is a combined result of degradation of buried peats and bacterial action, resulting in high DOC concentrations and strongly methanogenic conditions in the aquifer. The DOC and CH4 comprise, on average, nearly 50% of the total dissolved C pool in the central part of the aquifer. Methanogenic conditions complicate isotopic groundwater dating by the conventional dissolved inorganic carbon (DIC) method. Estimates of isotopic groundwater residence time using DOC14C data are proposed by the application of14C isotope and mass balance corrections.  相似文献   

3.
This study uses 3H concentrations, 14C activities (a14C), 87Sr/86Sr ratios, and δ13C values to constrain calcite dissolution in groundwater from the Ovens catchment SE Australia. Taken in isolation, the δ13C values of dissolved organic C (DIC) and 87Sr/86Sr ratios in the Ovens groundwater imply that there has been significant calcite dissolution. However, the covariance of 3H and 14C and the calculated initial 14C activities (a014C) imply that most groundwater cannot have dissolved more than 20% of 14C-free calcite under closed-system conditions. Rather, calcite dissolution must have been partially an open-system process allowing 13C and 14C to re-equilibrate with CO2 in the unsaturated zone. Recognising that open-system calcite dissolution has occurred is important for dating deeper groundwater that is removed from its recharge area in this and other basins. The study is one of the first to use 14C and 3H to constrain the degree of calcite dissolution and illustrates that it is a valuable tool for assessing geochemical processes in recharge areas.  相似文献   

4.
The Bohemian Cretaceous Basin represents a complex hydrogeological system composed of several aquifers with very favourable hydrogeological properties. These aquifers have been exploited for many years. The sustainability of such resources might be guaranteed by well organised water management, which requires a detailed knowledge about the functioning of the hydrogeological system. Although many efforts have previously been made to evaluate groundwater residence time, the many intricate geochemical processes complicate groundwater dating. The current study clarifies the functioning of this complex hydrogeological basin using hydrogeochemical and isotopic investigations. Chemical data and a combination of 13C and 14C isotopes within the Cenomanian and the Turonian layers indicate groundwater interactions with deep-seated CO2, rock matrix, surface waters and fossil organic matter. Very depleted δ13C values (average δ13C ∼ −13.4‰) suggest interactions with fossil organic matter, whereas enriched values account for the interaction with deep CO2 gas ascending from the upper mantle via the numerous faults and fractures, and also, to a lesser extent, from calcite dissolution. Geochemical processes that take place in the system cause a clear depletion in 14C that greatly complicates groundwater residence time evaluation. Different dilution correction models have been applied considering the different C origins. The stable isotope content, mainly 18O values, indicates both the contribution of modern precipitation and the partial infiltration of palaeowaters during colder climatic conditions from the end of the Pleistocene. The apparent 14C groundwater ages range from modern to 11.1 ka BP, which suggests some post glacial infiltration from melting ice sheets. Finally, all the acquired information was used to propose a conceptual model of C origin within the basin.  相似文献   

5.
地下水14C年龄校正一直是地下水年代学研究中的一个热点问题,将反向地球化学路径模型与同位素质量传输模型耦合起来,在综合考虑不同碳源、不同水文地球化学反应对14C质量传输影响的基础上,提出了一种新的综合性的校正方法,从而使地下水14C定年技术得到了进一步发展。识别深层地下水演化过程中影响14C浓度变化的主要因素并定量确定其对地下水14C浓度的影响程度是地下水14C校正的精度和可信度的重要考虑因素;在应用水文地球化学路径模拟技术进行地下水14C年龄校正时,必须要充分考虑地下水补给环境特点以及反向地球化学模拟模型中的非可行解的排除。  相似文献   

6.
The continuous abstraction of groundwater from Arusha aquifers in northern Tanzania has resulted in a decline in water levels and subsequent yield reduction in most production wells. The situation is threatening sustainability of the aquifers and concise knowledge on the existing groundwater challenge is of utmost importance. To gain such knowledge, stable isotopes of hydrogen and oxygen, and radiocarbon dating on dissolved inorganic carbon (DIC), were employed to establish groundwater mean residence time and recharge mechanism.14C activity of DIC was measured in groundwater samples and corrected using a δ13C mixing method prior to groundwater age dating. The results indicated that groundwater ranging from 1,400 years BP to modern is being abstracted from deeper aquifers that are under intensive development. This implies that the groundwater system is continuously depleted due to over-pumping, as most of the sampled wells and springs revealed recently recharged groundwater. High 14C activities observed in spring water (98.1?±?7.9 pMC) correspond with modern groundwater in the study area. The presence of modern groundwater suggests that shallow aquifers are actively recharged and respond positively to seasonal variations.  相似文献   

7.
《Applied Geochemistry》2001,16(7-8):849-859
Isotopic investigations using 14C of groundwater were carried out to understand the hydraulic conditions in the sedimentary rocks at the Tono study site, central Japan. 14C activities of groundwater observed range from 2 to 32 % Modern Carbon (pMC). Measured 14C activities of groundwater are corrected by the isotopic mass balance model based on 14C activities, δ13C values, concentrations of the dissolved inorganic carbon (DIC) and δ13C values of non-active carbon dissolved into the groundwater from carbonate minerals and organics. Assuming that the groundwater reservoir is comparable to the piston flow situation, the relative 14C ages of groundwaters were calculated from the corrected 14C activity. The relative 14C age suggests that the groundwater infiltration from the upper part of the sedimentary rocks to the lower part takes several thousands of years, or that the groundwater in the lower part of sedimentary rocks is derived from long distance flow from the surface through the unconformity between the sedimentary rocks and basement granite. The flow rate calculated by relative 14C ages shows similar values to those estimated by computer simulation using hydraulic pressure and conductivity data. Hydraulic conditions at the Tono study site inferred from 14C activity agree with those suggested from hydrogeological analyses. Isotopic approaches using 14C activity can be applied as geochemical evaluation for interpretations from the hydraulic study.  相似文献   

8.
The objective of this paper is to build a general correction model that takes into account all the different radiocarbon-dilution reactions and resolving the processes that are geochemically “aging” the groundwater in the Neogene Aquifer. For this, δ13C and radiocarbon in groundwater are investigated with their relationship to other chemical components in groundwater. The δ13C values in the Neogene Aquifer are influenced by various geochemical reactions like calcite dissolution, oxidation of organic matter and methanogenesis. Calcite dissolution and CH4 production increase δ13C while the oxidation of organic matter decreases δ13C in the groundwater. The reactions that modify δ13C also influence the 14C activity. Due to the complex geochemical environment, existing correction models are not applicable to this situation. A correction model for initial 14C activity is formulated in which the different C sources that influence 14C activity are taken into account. It is observed that recent dissolved organic matter plays an important role in redox reactions. The corrected 14C ages lie between −0.792 and 6.425 ka representing the maximum age. If a part of the organic matter that oxidises is fossil, the determined age will represent an overestimated age.  相似文献   

9.
The study place is in the Barreirinhas region, Maranhão State, northeastern Brazil. A vegetation transect of 78 km was studied among four vegetation types: Restinga (coastal vegetation), Cerrado (woody savanna), Cerradão (dense woody savanna), and Forest, as well as three forested sites around Lagoa do Caçó, located approximately 10 km of the transect. Soil profiles in this transect were sampled for δ13C analysis, as well as buried charcoal fragments were used for 14C dating. The data interpretation indicated that approximately between 15,000 and ∼9000 14C yr B.P., arboreal vegetation prevailed in the whole transect, probably due to the presence of a humid climate. Approximately between ∼9000 and 4000-3000 14C yr B.P., there was the expansion of the savanna, probably related to the presence of drier climate. From ∼4000-3000 14C yr B.P. to the present, the results indicated an increase in the arboreal density in the area, due to the return to a more humid and probably similar climate to the present. The presence of buried charcoal fragments in several soil depths suggested the occurrence of palaeofires during the Holocene. The vegetation dynamic inferred in this study for northeastern Brazil is in agreement with the results obtained in areas of Amazon region, based on pollen analysis of lake sediments and carbon isotope analysis of soil organic matter (SOM), implying than similar climatic conditions have affected these areas during the late Pleistocene until the present.  相似文献   

10.
The speciation and mobility of a variety of chemical species in groundwater are strongly influenced by redox and pH conditions. Dissolved O2 (DO) and dissolved inorganic C (DIC) concentrations are significant controls of these conditions, respectively. It is not always clear what the major processes are that influence changes in the concentration of DO and DIC across a groundwater flowpath. The combined use of the stable isotope compositions of DO (δ18O–DO) and DIC (δ13C–DIC) has the potential to help investigators discriminate between sources and sinks of DO and DIC in groundwater systems.  相似文献   

11.
《Applied Geochemistry》1998,13(5):593-606
The comparative geochemical and isotopic study of confined and unconfined Chalk groundwaters of the Paris Basin and the N German Basin proves a significant chemical evolution during groundwater flow from the recharge zones to the deep confined aquifer. Different time dependent geochemical parameters have been tested as dating tools: Cation ratios (Sr2+/Ca2+, Mg2+/Ca2+), N–NO−3, noble gas contents as paleotemperature indicators (Ne, Ar, Kr, Xe), radiogenic He, 13C, 14C, 18O, 2H, 3H. Cation ratios and 13C show the importance of incongruent dissolution processes in the Chalk aquifer. Water–rock interactions were taken into account in a multi-step dissolution model to determine radiocarbon groundwater ages. The oldest waters in the confined part of the Paris basin Chalk with maximum 14C ages of 14,000 a B.P. contain pleistocene recharge components as can be shown by a stable isotope depletion and noble gas temperatures significantly lower than in recent groundwaters. Chalk waters at the Lägerdorf site in Northern Germany show a distinct stratification with respect to residence times and hydrochemistry.  相似文献   

12.
The northern section of the Bohemian Cretaceous Basin has been the site of intensive U exploitation with harmful impacts on groundwater quality. The understanding of groundwater flow and age distribution is crucial for the prediction of the future dispersion and impact of the contamination. State of the art tracer methods (3H, 3He, 4He, 85Kr, 39Ar and 14C) were, therefore, used to obtain insights to ageing and mixing processes of groundwater along a north–south flow line in the centre of the two most important aquifers of Cenomanian and middle Turonian age. Dating of groundwater is particularly complex in this area as: (i) groundwater in the Cenomanian aquifer is locally affected by fluxes of geogenic and biogenic gases (e.g. CO2, CH4, He) and by fossil brines in basement rocks rich in Cl and SO4; (ii) a thick unsaturated zone overlays the Turonian aquifer; (iii) a periglacial climate and permafrost conditions prevailed during the Last Glacial Maximum (LGM), and iv) the wells are mostly screened over large depth intervals.Large disagreements in 85Kr and 3H/3He ages indicate that processes other than ageing have affected the tracer data in the Turonian aquifer. Mixing with older waters (>50 a) was confirmed by 39Ar activities. An inverse modelling approach, which included time lags for tracer transport throughout the unsaturated zone and degassing of 3He, was used to estimate the age of groundwater. Best fits between model and field results were obtained for mean residence times varying from modern up to a few hundred years. The presence of modern water in this aquifer is correlated with the occurrence of elevated pollution (e.g. nitrates).An increase of reactive geochemical indicators (e.g. Na) and radiogenic 4He, and a decrease in 14C along the flow direction confirmed groundwater ageing in the deeper confined Cenomanian aquifer. Radiocarbon ages varied from a few hundred years to more than 20 ka. Initial 14C activity for radiocarbon dating was calibrated by means of 39Ar measurements. The 14C age of a sample recharged during the LGM was further confirmed by depleted stable isotope signatures and near freezing point noble gas temperature. Radiogenic 4He accumulated in groundwater with concentrations increasing linearly with 14C ages. This enabled the use of 4He to validate the dating range of 14C and extend it to other parts of this aquifer. In the proximity of faults, 39Ar in excess of modern concentrations and 14C dead CO2 sources, elevated 3He/4He ratios and volcanic activity in Oligocene to Quaternary demonstrate the influence of gas of deeper origin and impeded the application of 4He, 39Ar and 14C for groundwater dating.  相似文献   

13.
A comprehensive hydrogeochemical study was carried out in the Paleozoic Basses-Laurentides sedimentary rock aquifer system in Québec over a 1500 km2 study area. Groundwater samples were collected at 153 sites, characterizing all geological and hydrogeological units to a maximum depth of 140 m. Groundwater was analyzed for major, minor and trace inorganic constituents, stable isotopes δ 2H, δ 18O, and δ 13C of dissolved inorganic carbon (DIC), and some samples were analyzed for 3H, and 14C of DIC. The regional distribution of groundwater types shows that the hydrogeological conditions exert a dominant control on the major ions chemistry of groundwater. Preferential recharge areas are characterized by tritiated Ca-Mg-HCO3 groundwater, and confined conditions by submodern Na-HCO3 and Na-Cl groundwater types. Two groundwater end-members are identified in the aquifer system, modern meteoric water and Pleistocene Champlain Sea water. The region displays significant variations of groundwater geochemistry and quality controlled by glaciation, Champlain Sea invasion, lithological rock diversity, and flow system scales. This situation leads to varied groundwater types and origins within a restricted area.  相似文献   

14.
3H, δ13C and hydrochemical data were used to estimate the corrected groundwater age derived from conventional 14C age of dissolved inorganic carbon (DIC). The Middle-Upper Devonian aquifer system from the Baltic upland recharge area in eastern Lithuania towards the discharge area on the Baltic Sea coast in the west was considered. The concentration of total dissolved solids (TDS) in groundwater changes from 300 to 24,000  mg/L and increases downgradient towards the coast. The other major constituents have the same trend as the TDS. The hydrochemical facies of groundwater vary from an alkali-earth carbonates facies at the eastern upland area to an alkali-earth carbonate-sulfate and chloride facies at transit and discharge areas. Meteoric water percolating through the Quaternary and Devonian aquifers regulate the initial 14C activities of groundwater involving two main members of DIC: soil CO2 with modern 14C activity uptake and dissolution of 14C-free aquifer carbonates. Other sources of DIC are less common. 14C activity of DIC in the groundwater ranged from 60 to 108 pMC at the shallow depths. With an increase of the aquifers depth the dolomitization of aqueous solution and leakage of the “old” groundwater from lower aquifers take place, traced by lower activities (7–30 pMC).  相似文献   

15.
The particular objective of the present work is the development of a new radiocarbon correction approach accounting for palaeoclimate conditions at recharge and hydrochemical evolution. Relevant climate conditions at recharge are atmospheric pCO2 and infiltration temperatures, influencing C isotope concentrations in recharge waters. The new method is applied to the Ledo-Paniselian Aquifer in Belgium. This is a typical freshening aquifer where recharge takes place through the semi-confining cover of the Bartonian Clay. Besides cation exchange which is the major influencing process for the evolution of groundwater chemistry (particularly in the Bartonian Clay), also mixing with the original porewater solution (fossil seawater) occurs in the aquifer. Recharge temperatures were based on noble gas measurements. Potential infiltration water compositions, for a range of possible pCO2, temperature and calcite dissolution system conditions, were calculated by means of PHREEQC. Then the sampled groundwaters were modelled starting from these infiltration waters, using the computer code NETPATH and considering a wide range of geochemical processes. Fitting models were selected on the basis of correspondence of calculated δ13C with measured δ13C. The 14C modelling resulted in residence times ranging from Holocene to Pleistocene (few hundred years to over 40 ka) and yielded consistent results within the uncertainty estimation. Comparison was made with the δ13C and Fontes and Garnier correction models, that do not take climate conditions at recharge into account. To date these are considered as the most representative process-oriented existing models, yet differences in calculated residence times of mostly several thousands of years (up to 19 ka) are revealed with the newly calculated ages being mostly (though not always) younger. Not accounting for climate conditions at recharge (pCO2 and temperature) is thus producing substantial error on deduced residence times. The derived 14C model ages are correlated with He concentrations measured in the groundwater of the aquifer. The obtained residence times show a gap between about 14 and 21 ka indicating possible permafrost conditions which inhibited any groundwater recharge.  相似文献   

16.
The purpose of this report is to explain geochemical and stable isotopes trends in the Brazilian unit of the Guarani Aquifer System (Botucatu and Piramboia aquifers) in S?o Paulo State, Brazil. Trends of dissolved species concentrations and geochemical modeling indicated a significant role of cation exchange and dissolution of carbonates in downgradient evolution of groundwater chemistry. Loss of calcium by the exchange for sodium drives dissolution of carbonates and results in Na–HCO3 type of groundwater. The cation-exchange front moves downgradient at probably much slower rate compared to the velocity of groundwater flow and at present is located near to the cities of Sert?ozinho and águas de Santa Barbara (wells PZ-34 and PZ-148, respectively) in a shallow confined area, 50–70 km from the recharge zone. Part of the sodium probably enters the Guarani Aquifer System. together with chloride and sulfate from the underlying Piramboia Formation by diffusion related to the dissolution of evaporates like halite and gypsum. High concentrations of fluorine (up to 13.3 mg/L) can be explained by dissolution of mineral fluoride also driven by cation exchange. However, it is unclear if the dissolution takes place directly in the Guarani Aquifer System or in the overlying basaltic Serra Geral Formation. There is depletion in δ 2H and δ 18O values in groundwater downgradient. Values of δ 13C(DIC) are enriched downgradient, indicating dissolution of calcite under closed system conditions. Values of δ 13C(DIC) in deep geothermal wells are very high (>–6.0‰) and probably indicate isotopic exchange with carbonates with δ 13C about –3.0‰. Future work should be based on evaluation of vertical fluxes and potential for penetration of contamination to the Guarani Aquifer System. Electronic Publication  相似文献   

17.
Environmental stable and radioactive isotopes (δ2H, δ13C, δ18O; 3H and 14C), together with physical and geochemical data, were used in the determination of the origins of groundwater salinization and geochemical evolution processes in coastal regions. Two case studies on the Atlantic Coast are discussed, one located in the Essaouira sedimentary basin, western Morocco, and the second, in the Lower Tagus–Sado sedimentary basin, southwest Portugal. In both regions, groundwater degradation occurs by salinization increase to different concentrations and in relation to different origins. The main quality issues for the groundwater resources are related to seawater intrusion, dissolution of diapiric structures intruding the aquifer layers, brine dissolution at depth, and/or evaporation of irrigation water. Anthropogenic pollution ascribed to agricultural activities is another source for groundwater degradation, affecting mainly the shallow aquifers. The apparent 14C age of the analysed samples ranges from 2.9?±?0.3 up to 45.6?±?0.6 pmC in the Miocene groundwater samples from the basin in Portugal; at the Essaouira basin in Morocco, the 14C content varies from 60 to 86 pmC. In most of the water samples, the 3H concentration is below the detection limit. In both basins, the isotopic results together with the geochemical data provided an effective label for tracing the mineralization origin and groundwater degradation processes. Further, the isotopic signatures were used in the identification of a paleoclimate (colder period), recorded in the stable isotopic composition and corroborated with the 14C data.  相似文献   

18.
The geochemical processes, water–rock interactions and stable isotopes distribution (δ13C of DIC and δ18O and δ34S of \({\text{SO}}^{{{\text{2 - }}}}_{{\text{4}}} \)) were investigated in the gasoline-contaminated aquifer at the Hnevice site, 50  km northwest of Prague, Czech Republic. Diesel, gasoline and oil leaks originate from a large fuel storage area causing heavy contamination of the saturated and unsaturated zones in an area of about 0.7  km2. Groundwater investigations were conducted using five multilevel sampler wells with emphasis on redox parameters and degradation by-products and a solid-phase study focused on iron speciation and determination of principal and secondary minerals. Based on the study of groundwater and solid-phase geochemistry, four different geochemical zones were described. Zone I is thought to be background consisting of an aerobic aquifer and the absence of reduced species in significant concentrations. Zone II is situated in the plume core with methanogenic, sulphate and iron-reducing conditions accompanied by ankerite and kutnahorite precipitates and significant depletion of the oxidation capacity of the aquifer. Zone III is a mixing (corona) zone, situated at the fringe of the plume with high biodegradation rates and Fe(III)-precipitants. In zone IV, reoxidation of Fe(II) minerals (with e.g. the occurrence of psilomelane and cornelite) is typical.  相似文献   

19.
This research aims to evaluate the groundwater resources of Paleogene aquifer in the Upper Jazireh area (Syria), in terms of chemical water type, recharge zones and water ages. The results show that the main recharge zones for the Paleogene aquifer range between 650 and 900 m a.s.l., which coincide with the outcrop of the karstified limestone in the Mardin uplift. The chemical and isotopic behaviors of groundwater, together with radiometric 14C reflect the existence of three different groundwater groups: (1) the fresh and cold water, percolating in short and shallow flow paths, for which the main replenishment processes are recent; (2) the brackish and thermal water containing certain amounts of H2S gas, that percolate in longer and deeper flow paths, for which the main replenishment processes occurred during the palaeoclimatic humid conditions of Pleistocene time, placed at 10–18 Ka BP; (3) the brackish and admixed thermal groundwater with intermediate 14C age, which seems to be formed as a result of mixing between the previous two groups.  相似文献   

20.
Geochemical reaction models were evaluated to improve radiocarbon dating of dissolved inorganic carbon (DIC) in groundwater from confined parts of the Upper Floridan aquifer in central and northeastern Florida, USA. The predominant geochemical reactions affecting the 14C activity of DIC include (1) dissolution of dolomite and anhydrite with calcite precipitation (dedolomitization), (2) sulfate reduction accompanying microbial degradation of organic carbon, (3) recrystallization of calcite (isotopic exchange), and (4) mixing of fresh water with as much as 7% saline water in some coastal areas. The calculated cumulative net mineral transfers are negligibly small in upgradient parts of the aquifer and increase significantly in downgradient parts of the aquifer, reflecting, at least in part, upward leakage from the Lower Floridan aquifer and circulation that contacted middle confining units in the Floridan aquifer system. The adjusted radiocarbon ages are independent of flow path and represent travel times of water from the recharge area to the sample point in the aquifer. Downgradient from Polk City (adjusted age 1.7 ka) and Keystone Heights (adjusted age 0.4 ka), 14 of the 22 waters have adjusted 14C ages of 20–30 ka, indicating that most of the fresh-water resource in the Upper Floridan aquifer today was recharged during the last glacial period. All of the paleowaters are enriched in 18O and 2H relative to modern infiltration, with maximum enrichment in δ18O of approximately 2.0‰. Electronic Publication  相似文献   

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