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1.
Horizontal drilling and hydraulic fracturing have enhanced unconventional hydrocarbon recovery but raised environmental concerns related to water quality. Because most basins targeted for shale‐gas development in the USA have histories of both active and legacy petroleum extraction, confusion about the hydrogeological context of naturally occurring methane in shallow aquifers overlying shales remains. The Karoo Basin, located in South Africa, provides a near‐pristine setting to evaluate these processes, without a history of conventional or unconventional energy extraction. We conducted a comprehensive pre‐industrial evaluation of water quality and gas geochemistry in 22 groundwater samples across the Karoo Basin, including dissolved ions, water isotopes, hydrocarbon molecular and isotopic composition, and noble gases. Methane‐rich samples were associated with high‐salinity, NaCl‐type groundwater and elevated levels of ethane, 4He, and other noble gases produced by radioactive decay. This endmember displayed less negative δ13C‐CH4 and evidence of mixing between thermogenic natural gases and hydrogenotrophic methane. Atmospheric noble gases in the methane‐rich samples record a history of fractionation during gas‐phase migration from source rocks to shallow aquifers. Conversely, methane‐poor samples have a paucity of ethane and 4He, near saturation levels of atmospheric noble gases, and more negative δ13C‐CH4; methane in these samples is biogenic and produced by a mixture of hydrogenotrophic and acetoclastic sources. These geochemical observations are consistent with other basins targeted for unconventional energy extraction in the USA and contribute to a growing data base of naturally occurring methane in shallow aquifers globally, which provide a framework for evaluating environmental concerns related to unconventional energy development (e.g., stray gas).  相似文献   

2.
Fifteen submarine glasses from the East Pacific Rise (CYAMEX), the Kyushu-Palau Ridge (DSDP Leg 59) and the Nauru Basin (DSDP Leg 61) were analysed for noble gas contents and isotopic ratios. Both the East Pacific Rise and Kyushu-Palau Ridge samples showed Ne excess relative to Ar and a monotonic decrease from Xe to Ar when compared with air noble gas abundance. This characteristic noble gas abundance pattern (type 2, classified by Ozima and Alexander) is interpreted to be due to a two-stage degassing from a noble gas reservoir with originally atmospheric abundance. In the Kyushu-Palau Ridge sample, noble gases are nearly ten times more abundant than in the East Pacific Rise samples. This may be attributed to an oceanic crust contamination in the former mantle source.There is no correlation between the He content and that of the other noble gas in the CYAMEX samples. This suggests that He was derived from a larger region, independent from the other noble gases.Except where radiogenic isotopes are involved, all other noble gas isotopic ratios were indistinguishable from air noble gas isotopic ratios. The3He/4He in the East Pacific Rise shows a remarkably uniform ratio of (1.21±0.07)×10?5, while the40Ar/36Ar ranges from 700 to 5600.  相似文献   

3.
Gas‐saturated groundwater forms bubbles when brought to atmospheric pressure, preventing precise determination of its in situ dissolved gas concentrations. To overcome this problem, a modeling approach called the atmospheric sampling method is suggested here to recover the in situ dissolved gas concentrations of groundwater collected ex situ under atmospheric conditions at the Horonobe Underground Research Laboratory, Japan. The results from this method were compared with results measured at the same locations using two special techniques, the sealed sampler and pre‐evacuated vial methods, that have been developed to collect groundwater under its in situ conditions. In gas‐saturated groundwater cases, dissolved methane and inorganic carbon concentrations derived using the atmospheric sampling method were mostly within ±4 and ±10%, respectively, of values from the sealed sampler and pre‐evacuated vial methods. In gas‐unsaturated groundwater, however, the atmospheric sampling method overestimated the in situ dissolved methane concentrations, because the groundwater pressure at which bubbles appear (Pcritical) was overestimated. The atmospheric sampling method is recommended for use where gas‐saturated groundwater can be collected only ex situ under atmospheric conditions.  相似文献   

4.
Noble gas isotopes (3He, 4He, Ne, Ar, Kr, Xe), tritium (3H), chlorofluorocarbons (CFCs) and dissolved oxygen (O2) were seasonally measured in a small groundwater system recharged by infiltration of river water at Linsental, northeastern Switzerland. All Groundwater samples contained an excess of atmospheric noble gases (‘excess air’) usually with an elemental composition equal to air. The concentrations of atmospheric noble gases in the groundwater were used to calculate the excess air component and the water temperature at recharge. The noble gas temperatures (NGTs) in the boreholes close to the river vary seasonally, however, the average NGT of all samples lies close to the mean annual temperature of the river water. Groundwater ages were calculated using the tritium/helium-3 (3H/3He) dating method. The water ages of the samples obtained near the river depend on the amount of recently infiltrated river water and are young during times of active river discharge. In contrast, the mean water age of about 3 years of the deep aquifer remained nearly constant over the sampling period. The observed CFC-11 (CFCl3) and CFC-12 (CF2Cl2) concentrations are significantly higher than the atmospheric equilibrium concentrations and therefore CFCs do not provide any direct information on the residence time of the groundwater. Nevertheless, the CFC excess in the groundwater shows a linear increase with the 3H/3He age. Additionally, both accumulation of radiogenic He (4Herad) and O2 consumption are strongly correlated with residence time. All these correlations can be interpreted either in terms of mixing of recently infiltrated river water with older groundwater or in terms of accumulation/consumption rates.  相似文献   

5.
Atmospheric noble gases (e.g., 22Ne, 36Ar, 84Kr, 130Xe) in crustal fluids are only sensitive to subsurface physical processes. In particular, depletion of atmospheric noble gases in groundwater due to boiling and steam separation is indicative of the occurrence of a thermal event and can thus be used to trace the thermal history of stable tectonic regions. We present noble gas concentrations of 38 deep brines (~ 0.5–3.6 km) from the Michigan Basin. The atmospheric noble gas component shows a strong depletion pattern with respect to air saturated water. Depletion of lighter gases (22Ne and 36Ar) is stronger compared to the heavier ones (84Kr and 130Xe). To understand the mechanisms responsible for this overall atmospheric noble gas depletion, phase interaction models were tested. We show that this atmospheric noble gas depletion pattern is best explained by a model involving subsurface boiling and steam separation, and thus, consistent with the occurrence of a past thermal event of mantle origin as previously indicated by both high 4He/heat flux ratios and the presence of primordial mantle He and Ne signatures in the basin. Such a conceptual model is also consistent with the presence of past elevated temperatures in the Michigan Basin (e.g., ~ 80–260 °C) at shallow depths as suggested by previous thermal studies in the basin. We suggest that recent reactivation of the ancient mid-continent rift system underneath the Michigan Basin is likely responsible for the release of both heat and mantle noble gases into the basin via deep-seated faults and fracture zones. Relative enrichment of atmospheric Kr and Xe with respect to Ar is also observed, and is interpreted as reflecting the addition of sedimentary Kr and Xe from associated hydrocarbons, following the hydrothermal event. This study pioneers the use of atmospheric noble gases in subsurface fluids to trace the thermal history of stable tectonic regions.  相似文献   

6.
A number of processes may modify the noble gas composition of silicate liquids so that the composition of noble gases observed in glassy margins of deep-sea basalts is not that of the upper mantle. Differential solubility enhances the light noble gases relative to the heavier gases; however, we demonstrate that the observed abundance pattern cannot be attributed to solubility of noble gases with atmospheric proportions. Partial melting and fractional crystallization increase the noble gas content of all species relative to mantle concentrations, but do not fractionate their relative abundances. Noble gases may be lost from an ascending magma in various ways, the most important, however, may be exclusion of gas from crystals forming at the time of solidification, which is shown to result in marked loss of gas from the basalt. Small amounts of low-temperature alteration of solidified basalt can produce dramatic changes in the noble gas abundance pattern, since the adsorption coefficients for the different noble gas favor uptake of heavy species relative to the light species. Atmospheric contamination can account for observed variations in the 40Ar/36Ar ratio of oceanic basalts. The degree of crystallinity of glassy margins of deep-sea basalts may control the helium abundance of these samples; however, the uniform 3He/4He values reported apparently reflect a relatively constant proportion of radiogenic and primordial helium in the mantle.  相似文献   

7.
Peter G. Cook 《水文研究》2013,27(25):3694-3707
Environmental tracer methods have been used to quantify groundwater discharge to rivers for the past few decades. A number of different tracers have been used in these studies, including individual ion concentrations, electrical conductivity, stable isotopes 2H and 18O, and the dissolved gases helium, chlorofluorocarbons and radon. This paper discusses the assumptions of the method, as well as its resolution and accuracy. The method will be most accurate when the tracer concentration in groundwater is very distinct from that in the river. On the basis of typical parameters, groundwater inflow rates as low as 5 mm/day can usually be estimated with electrical conductivity and ion tracers. A lower limit of resolution of approximately 2 mm/day is usually possible with radon, principally because the ratio of the river concentration to the groundwater concentration will be higher. However, hyporheic exchange can also contribute radon to the river. Where this process is significant, it is more difficult to estimate groundwater inflow from radon activities in the river, thus reducing the accuracy of the method. For CFCs, the lower limit of resolution is approximately 30 mm/day. Helium has not been widely used but can potentially be very accurate if the groundwater is old. The method assumes steady‐state conditions and so can only be applied when river flows are stable. Sampling resolution is also particularly important for dissolved gases, and uncertainty in where groundwater inflow occurs between sampling points can cause large uncertainty in inflow rates if the distance between sample locations is large. Poor mixing of solutes within the river can limit the method if the river is wide and shallow. When correctly applied, however, the environmental tracer method is able to provide robust estimates of groundwater discharge at a scale and accuracy that is not possible with most other methods. Copyright © 2012 John Wiley & Sons, Ltd.  相似文献   

8.
Noble gas elemental and isotopic abundances were measured in seven deep-sea water samples from five different sampling sites in the Nankai Trough, the Japan Trench and the Kuril Trench. The samples were obtained by the manned submersible “Nautile”. Most of the sampling sites are associated with clam colonies and/or fluid venting. Excesses both in3He/4He ratio and He concentration are observed in a seawater sample collected a few kilometers off the clam colonies which were found at a depth of 3830 m at the mouth of the Tenryu Canyon. Concentrations of noble gases (Ne, Ar, Kr and Xe) in this sample show progressive depletion from Ne to Xe relative to those in 1°C air-saturated seawater, which can be attributed to mixing of hot water ( 15°C) with cold ambient water ( 1°C). Isotopic compositions of Ne, Ar, Kr and Xe in this sample are atmospheric. These observations may reflect venting of hot pore water around the Tenryu Canyon. All the other samples show a significant excess in concentration of all noble gases relative to 1°C air-saturated seawater and the isotopic compositions are atmospheric. This excess of noble gas concentrations may appear to be air contamination in the samples. However, results of hydrocarbon analyses of the Kaiko samples imply that such large amount of air contamination is improbable. Decomposition of gas hydrate in deep-sea sediments is a more likely explanation for the observed excess of noble gas concentration.  相似文献   

9.
Few studies have investigated large reaches of rivers in which multiple sources of groundwater are responsible for maintaining baseflow. This paper builds upon previous work undertaken along the Fitzroy River, one of the largest perennial river systems in north‐western Australia. Synoptic regional‐scale sampling of both river water and groundwater for a suite of environmental tracers (4He, 87Sr/86Sr, 222Rn and major ions), and subsequent modeling of tracer behavior in the river, has enabled definition and quantification of groundwater input from at least three different sources. We show unambiguous evidence of both shallow “local” groundwater, possibly recharged to alluvial aquifers beneath the adjacent floodplain during recent high‐flow events, and old “regional” groundwater introduced via artesian flow from deep confined aquifers. We also invoke hyporheic exchange and either bank return flow or parafluvial flow to account for background 222Rn activities and anomalous chloride trends along river reaches where there is no evidence of the local or regional groundwater inputs. Vertical conductivity sections acquired through an airborne electromagnetic (AEM) survey provide insights to the architecture of the aquifers associated with these sources and general groundwater quality characteristics. These data indicate fresh groundwater from about 300 m below ground preferentially discharging to the river, at locations consistent with those inferred from tracer data. The results demonstrate how sampling rivers for multiple environmental tracers of different types—including stable and radioactive isotopes, dissolved gases and major ions—can significantly improve conceptualization of groundwater—surface water interaction processes, particularly when coupled with geophysical techniques in complex hydrogeological settings.  相似文献   

10.
Stepwise heating experiments on separated graphite-diamond-kamacite aggregates have revealed a pronounced difference in the release patterns of spallogenic3He and trapped gases. About half the3He is released at T ? 920°C, without being accompanied by significant amounts of primordial gases; the latter, together with the remaining3He, is given off only at T ? 1200°C. Acid treatment of an aliquant dissolved about 2/3 of the total Fe in the sample but did not cause a significant change in the gas concentrations. It is concluded that (a) there is no evidence for a loss of spallogenic3He from the graphite-diamond-kamacite aggregates, (b) one major constituent of the aggregates - graphite - is almost void of trapped gases, (c) kamacite is not a main carrier of the gases. This leaves diamond as the most probable site of the primordial gases.The elemental abundance pattern in the noble gases is essentially as reported previously. In particular, the excellent correlation between relative depletion factors, normalized to the cosmic abundance ratios, and the respective ionisation energies is confirmed. Other important features of the trapped gases are a20Ne/22Ne ratio of 12.3 ± 0.6, intermediate between solar wind and solar flare implanted Ne,36Ar/38Ar = 5.20 ± 0.06 and a measured40Ar/36Ar ratio (before blank correction) of 0.0076.Possible modes of trapping of the noble gases are discussed.  相似文献   

11.
Environmental concerns regarding the potential for drinking water contamination in shallow aquifers have accompanied unconventional energy development in the northern Appalachian Basin. These activities have also raised several critical questions about the hydrogeological parameters that control the naturally occurring presence and migration of hydrocarbon gases in shallow aquifers within petroliferous basins. To interrogate these factors, we analyzed the noble gas, dissolved ion, and hydrocarbon gas (molecular and isotopic composition) geochemistry of 98 groundwater samples from south‐central New York. All samples were collected ?1km from unconventional drilling activities and sample locations were intentionally targeted based on their proximity to various types of documented fault systems. In agreement with studies from other petroliferous basins, our results show significant correlations between elevated levels of radiogenic [4He], thermogenic [CH4], and dissolved ions (e.g., Cl, Br, Sr, Ba). In combination, our data suggest that faults have facilitated the transport of exogenous hydrocarbon‐rich brines from Devonian source rocks into overlying Upper Devonian aquifer lithologies over geologic time. These data conflict with previous reports, which conclude that hydrodynamic focusing regulates the occurrence of methane and salt in shallow aquifers and leads to elevated levels of these species in restricted flow zones within valley bottoms. Instead, our data suggest that faults in Paleozoic rocks play a fundamental role in gas and brine transport from depth, regulate the distribution of their occurrence in shallow aquifers, and influence the geochemistry of shallow groundwater in this petroliferous basin.  相似文献   

12.
The Earth's mantle contains a mixture of primordial noble gases, in particular solar-type helium and neon, and radiogenic rare gases from long-lived U, 232Th, 40K and short-lived 129I, 244Pu. Rocks derived from deep mantle plume magmatism like on Hawaii or Iceland contain a higher proportion of primordial nuclides than rocks from the shallow upper mantle, e.g. mid ocean ridge basalts (MORBs). This is widely regarded as the key evidence for survival of a less degassed and more “primitive” reservoir within the lower mantle. We present an evaluation of noble gas composition showing the shallow mantle to have about five times more radiogenic (relative to primordial) isotopes than Hawaii/Iceland-type plume reservoirs, no matter if short- or long-lived decay systems are considered. This fundamental property suggests that both MORB and plume-type noble gases are mixtures of: (1) a homogeneous radiogenic component present throughout most of the mantle and (2) a uniform primordial noble gas component with very minor radiogenic ingrowth. This conclusion depends crucially on the observed excess of radiogenic Xe in plume-derived rocks, and is only valid if this Xe excess is inherent to the plume sources.Possible sources of the primordial component of mantle plume reservoirs—and possibly also the MORB mantle—could be mantle reservoirs that remained relatively isolated over most of Earth's history (“blobs”, a deep abyssal layer, or the D” layer), but these need a considerable concentration of primordial gases to compensate U, Th, K decay over 4.5 Ga. Earth's core is evaluated as an alternative viable source feeding primordial nuclides into mantle reservoirs: even low metal-silicate partitioning coefficients allow sufficient primordial noble gases to be incorporated into the early forming core, as the undifferentiated proto-Earth was initially gas-rich. Massive mantle degassing soon after core formation then provides the opposite concentration gradient that allows primordial noble gases reentering the mantle at the core-mantle boundary, probably via partial mantle melts. Another possible source of primordial noble gases in Earth's mantle are subducted sediments containing extraterrestrial dust with solar He and Ne, but this supply mechanism crucially depends on largely unconstrained parameters. The latter two scenarios do not require the preservation of a “primitive” mantle reservoir over 4.5 Ga, and can potentially better reconcile increasing geochemical evidence of recycled lithospheric components in mantle plumes and seismic evidence for whole mantle convection.  相似文献   

13.
Karst spring measurements assess biogeochemical processes occurring within groundwater contributing areas to springs (springsheds) but can only provide aggregated information. To better understand spatially distributed processes that comprise these aggregated measures, we investigated aquifer denitrification evidence in groundwater wells (n = 16) distributed throughout a springshed in the Upper Floridan aquifer in northern Florida. Aquifer geochemistry, nitrate isotopes, and dissolved gases were compared against similar measurements at the spring outlet to evaluate spatial heterogeneity of denitrification evidence in relation to land surface–aquifer connectivity. Sample locations spanned spatial variation in recharge processes (i.e., diffuse vs. focused recharge) and proximity to sources of denitrification reactants (e.g., wetlands). Although no distinct spatial pattern in denitrification was uncovered, excess dissolved N2 gas measurements were only above detection in the unconfined springshed, with some evidence of a wetland proximity effect. Measured oxidation–reduction potential and dissolved oxygen poorly predicted denitrification, indicating that measured denitrification may be occurring upgradient from sampled wells. Despite dramatic spatial chemical heterogeneity across wells, mean values for recharge nitrate concentrations (0.02 to 5.56 mg N L?1) and excess N2 from aquifer denitrification (below detection to 1.37 mg N L?1) corresponded reasonably with mean spring outlet measurements for initial nitrate (0.78 to 1.36 mg N L?1) and excess N2 (0.15 to 1.04 mg N L?1). Congruence between groundwater and spring measurements indicates that combining sampling at the spring outlet and across the springshed is useful for understanding spatial aquifer denitrification. However, this approach would be improved with a high‐density sampling network with transects of wells along distinct groundwater flow paths.  相似文献   

14.
The abundances and isotopic compositions of noble gases in two samples from ultramafic xenoliths in alkali basalt, a young kaersutitic amphibole separated from a peridotite xenolith from Dish Hill, California and an ancient whole-rock lherzolite xenolith from Baja California, are reported and compared with the results of analyses on other mantle samples. In addition to previously recognized excesses of 3He and 129Xe, our results indicate that ambient gases in the mantle show a general enrichment of the lighter-mass nonradiogenic isotopes of Ar, Kr and Xe, and Ar with 40Ar/36Ar = 3 · 102.  相似文献   

15.
Oldoinyo Lengai is the world's only active carbonatite volcano and considerable debate still surrounds the genesis of its magmas. Gases were collected from two fumaroles discharging close to the then active vent in October 2003. Measured fumarole temperatures were ≤ 195°C, despite the nearby, vigorous eruptive activity. Gases were sampled and analysed for noble gas isotopes. Freshly erupted natrocarbonatite lavas, a 1917 nephelinite and a sub-recent wollastonite bearing rock were also collected and analysed for noble gas isotopes using vacuum crushing techniques. In all the lava samples the neon, argon, krypton and xenon isotope ratio data are indistinguishable from air implying atmospheric contamination of the hygroscopic rocks. In the fumaroles, measured 3He/4He ratios are between 4 and 7 R/Ra. This range is similar to published values for silicate xenoliths of the East African Rift implying a local lithospheric mantle source for the volatile component of the Lengai magmas. It is still unclear if the natrocarbonatites themselves come from this region, or if fractionation and/or liquid immiscibility generate the carbonate magmas from a silicate melt within the crust itself.  相似文献   

16.
Noble gas isotopes including 3He/4He, 40Ar/36Ar and Xe isotope ratios were determined for coexisting glass and olivine crystals in tholeiitic and alkalic basalts and dunite xenoliths from Loihi Seamount.Glass and coexisting olivine crystals have similar 3He/4He ratios (2.8–3.4) × 10?5, 20 to 24 times the atmospheric ratio (RA), but different 40Ar/36Ar ratios (400–1000). Based on the results of noble gas isotope ratios and microscopic observation, some olivine crystals are xenocrysts. We conclude that He is equilibrated between glass and olivine xenocrysts, but Ar is not.The apparent high 3He/4He ratio (3 × 10?5; = 21 RA) coupled with a relatively high 40Ar/36Ar ratio (4200) for dunite xenoliths (KK 17-5) may be explained by equilibration of He between MORB-type cumulates and the host magma.Except for the dunite xenoliths, noble gas data for these Loihi samples are compatible with a model in which samples from hot spot areas may be explained by mixing between P (plume)-type and M (MORB)-type components with the addition of A (atmosphere)-type component.Excess 129Xe has not been observed due to apparent large mass fractionation among Xe isotopes.  相似文献   

17.
springerlink.com Studies of mantle fluids are currently one of the hot topics in the earth science, greatly contributing to re-vealing origins and evolutions of fluids. In general, the concept of mantle fluids refers to their active compo-nents, such as CO2, H2O, N2, etc., while the noble gases inert in chemical properties belong to another research system. Due to their marked differences in various fluid sources of the Earth[1], the isotopic sig-natures of He and Ar have been widely used a…  相似文献   

18.
All twenty-three stable rare gas isotopes have been measured in a mantle-derived amphibole, kaersutite. The elemental abundance pattern of the rare gases is similar to the “planetary” rare gas pattern as defined by carbonaceous chondrites. The3He/4He ratio, (4.9 ± 0.6) × 10?5, is suggestive of primordial He degassing from the mantle. Excess21Ne is present. The measured40Ar/36Ar ratio,400 ± 5, may represent a mantle40Ar/36Ar ratio <240 when corrected for radiogenic40Ar. The heavy isotopes of Kr and t0he Xe isotopes are within error of the atmosphere values.  相似文献   

19.
Groundwater is not a sustainable resource, unless abstraction is balanced by recharge. Identifying the sources of recharge in a groundwater basin is critical for sustainable groundwater management. We studied the importance of river water recharge to groundwater in the south‐eastern San Joaquin Valley (24,000 km2, population 4 million). We combined dissolved noble gas concentrations, stable isotopes, tritium, and carbon‐14 analyses to analyse the sources, mechanisms, and timescales of groundwater recharge. Area‐representative groundwater sampling and numerical model input data enabled a stable isotope mass balance and quantitative estimates of river and local recharge. River recharge, identified by a lighter stable isotope signature, represents 47 ± 4% of modern groundwater in the San Joaquin Valley (recharged after 1950) but only 26 ± 4% of premodern groundwater (recharged before 1950). This implies that the importance of river water recharge in the San Joaquin valley has nearly doubled and is likely the result of a 40% increase in total recharge, caused by river water irrigation return flows and increased stream depletion and river recharge due to groundwater pumping. Compared with the large and long‐duration capacity for water storage in the subsurface, storage of water in rivers is limited in time and volume, as evidenced by cold river recharge temperatures resulting from fast infiltration and recharge. Groundwater banking of seasonal surface water flows and expansion of managed aquifer recharge practices therefore appear to be a natural and promising method for increasing the resilience of the San Joaquin Valley water supply system.  相似文献   

20.
The isotopic composition and abundances of He, Ne and Ar have been measured in a sequence of vertically stacked gas reservoirs at Hajduszoboszlo and Ebes, in the Pannonian Basin of Hungary. The gas reservoirs occur at depths ranging from 727 to 1331 m, are CH4 dominated and occupy a total rock volume of approximately 1.5 km3. There are systematic variations in both major species abundances and rare gas isotopic composition with depth: CO2 and N2 both increase from 0.47 and 1.76% to 14.1 and 30.5%, respectively, and 40Ar/36Ar and 21Ne/22Ne increase systematically from 340 and 0.02990 at 727 m to 1680 and 0.04290 at 1331 m. A mantle-derived He component between 2 and 5% is present in all samples, the remainder is crustal-radiogenic He. The Ar and Ne isotope variations arise from mixing between atmosphere-derived components in groundwater, and crustally produced radiogenic Ar and Ne. The atmosphere-derived 40Ar and 21Ne decreases from 85 and 97% of the total 40Ar and 21Ne at 727 m to 18 and 68% at 1331 m. The deepest samples are shown to have both atmosphere-derived and radiogenic components close to the air-saturated water and radiogenic production ratios. The shallowest samples show significant fractionation of He/Ar and Ne/Ar ratios in atmosphere-derived and radiogenic rare gas components, but little or no fractionation of He/Ne ratios. This suggests that diffusive fractionation of rare gases is relatively unimportant and that rare gas solubility partitioning between CH4 and H2O phases controls the observed rare gas elemental abundances.The total abundance of atmosphere-derived and radiogenic rare gas components in the Hajduszoboszlo gas field place limits on the minimum volume of groundwater that has interacted with the natural gas, and the amount of crust that has degassed and supplied radiogenic rare gases. The radiogenic mass balance cannot be accounted for by steady state production either within the basin sediments or the basement complex since basin formation. The results require that radiogenic rare gases are stored at their production ratios on a regional scale and transported to the near surface with minimal fractionation. The minimum volume of groundwater required to supply the atmosphere-derived rare gases would occupy a rock volume of some 1000 km3 (assuming an average basin porosity of 5%), a factor of 670 greater than the reservoir volume. Interactions between groundwater and the Hajduszoboszlo hydrocarbons has been on a greater scale than often envisaged in models of hydrocarbon formation and migration.  相似文献   

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