首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献，搜索用时 343 毫秒
1.
Sediments are an excellent archive for evaluation of time-series environmental contamination of water systems. Measurements of ultra-trace radioactive species, such as 129I, provide information for both chronologic calibration and anthropogenic emissions during the nuclear era. Here data are presented on 129I and other chemical parameters from two sediment cores collected in the Baltic Sea during 1997. The sediment sections have a relatively uniform grain size (clay–mud) and cover a period of about 50 a. Distribution of 129I in the sediment strongly relates to the liquid release records from the nuclear reprocessing facilities at Sellafield and La Hague. However, syn- and post-depositional alteration of organic matter at the sediment–water interface and within the sediment column may have contributed to slightly obliterating the anthropogenic 129I signals. Indication of Chernobyl-derived 129I occurs in the sediment profile, but is apparently overridden by the overwhelming flux from the nuclear reprocessing facilities. Although the record did not cover the pre-nuclear era (before 1945) sections, the ultra sensitive 129I profile provides a potential tool for relative dating and monitoring sources of water and sediment to the region.  相似文献   

2.
《Geochimica et cosmochimica acta》1999,63(13-14):1927-1938
Large quantities of iodine-129 have been released during nuclear weapons testing, and from nuclear power and fuel reprocessing plants. The distribution of this isotope was investigated in 110 surface water and soil samples from western New York (where several potential point sources are located) and other areas of North America, to evaluate its sources, transport pathways, and reservoirs. Elevated 129I concentrations associated with a former reprocessing facility at West Valley, NY, can be tracked to Lakes Erie and Ontario via site drainage, and for over 200 km via atmospheric transport, while only a negligible signal is associated with active power plants in the area. The results point to local reprocessing as the major source of 129I in western New York, while bomb fallout constitutes less than 0.5% of the signal. Surface soil is the dominant reservoir for anthropogenic 129I in this region. Across North America, 129I concentrations are lower than in western New York, although still significantly higher than expected weapons fallout. Reprocessing releases are currently seen to be the major source for elevated 129I concentrations on a global scale, in contrast to previous suggestions that most anthropogenic 129I was still derived from weapons fallout. Concentrations of 129I and iodine in surface reservoirs are generally found to be uncorrelated, implying that natural iodine and anthropogenic 129I are not yet in equilibrium. The results suggest that anthropogenic 129I is cycled between the atmosphere-soil-vegetation systems more rapidly than natural, pre-anthropogenic iodine.  相似文献   

3.
This work constitutes the first survey of I isotope ratios for Scottish sea water including the first data for the west of Scotland. These data are of importance because of the proximity to the world’s second largest emission source of 129I to the sea, the Sellafield nuclear reprocessing plant, because of the increasing importance of the sea to land transfer of 129I and also as input data for dose estimates based on this pathway of 129I. 129I/127I ratios in SW Scotland reached 3 × 10−6 in 2004. No strong variation of I isotope ratios was found from 2003 to 2005 in Scottish sea waters. Iodine isotope ratios increased by about a factor of 6 from 1992 to 2003 in NE Scotland, in agreement with the increase of liquid 129I emissions from Sellafield over that time period. It is demonstrated that 129I/127I ratios agree better than 129I concentrations for samples from similar locations taken in very close temporal proximity, indicating that this ratio is more appropriate to interpret than the radionuclide concentration.  相似文献   

4.
Iodine-129 and 238Pu, 239Pu and 240Pu are radionuclides posing a long-term safety concern due to their potential integration in bio and geo-chemical cycles and their significant half-lives. They are present throughout the environment at very low levels, and more particularly, nuclear fuel reprocessing plants (NRP) have been identified as local sources of these radionuclides. However, due to measurement difficulties, published data concerning their activity levels in terrestrial environments around NRP facilities remain scarce. The aim of the present paper is to communicate 129I, 238Pu and 239+240Pu measurements results from the area surrounding the Marcoule NRP, which is situated in SE France. Several vegetation samples were collected around the nuclear installation in 1999 and 2000, in order to examine the possible impacts of its atmospheric I and Pu discharges. Based on 238Pu/239+240Pu activity ratios and 129I/127I isotopic ratios, local increases in Pu and 129I were detected and related to industrial activity.  相似文献   

5.
Tracer technology has been used to understand water circulation in marine systems where the tracer dose is commonly injected into the marine waters through controlled experiments, accidental releases or waste discharges. Anthropogenic discharges of 129I have been used to trace water circulation in the Arctic and North Atlantic Ocean. Here, 129I, together with 127I, is utilized as a tracer of water pathways and circulation in the Baltic Sea through collection of seawater depth profiles. The results indicate the presence of 129I signatures which are distinct for each water mass and provide evidence for: (1) inflow water masses through the Drogden Sill that may reach as far as the SW of the Arkona Sea, (2) a portion of North Atlantic water in the bottom of Arkona basin, (3) cyclonic upwelling which breaks through the halocline in a pattern similar to the Baltic haline conveyor belt and (4) more influx of fresher water from the Gulf of Finland and Bothnian Sea in August relative to April. These findings provide advances in labeling and understanding water pathways in the Baltic Sea.  相似文献   

6.
《Applied Geochemistry》2005,20(8):1461-1472
Iodine is a biophilic element, with one stable isotope, 127I, and one long-lived radioisotope, 129I. Radioiodine originates in the surface environment almost entirely from anthropogenic activities such as nuclear fuel reprocessing in Europe and thus provides a unique point source tracer. Very few studies have evaluated the geochemical behavior of I isotopes in the subsurface. In this study, the concentrations of 129I and 127I were measured in wells fed by a series of artificial recharge ponds in the Forebay Area of the Orange County ground water basin (California, USA) to evaluate their potential use as hydrological tracers. To substantiate interpretation of 129I and 127I concentration data, the aquifer system was evaluated using the literature values of aquifer water mass age based on 3H/3He, Xe and δ18O tracer data. The aquifer data demonstrate the nearly conservative behavior of 129I with 129I/127I ratios likely reflecting variations in source functions as well as climatic conditions, and with inferred particle-water partition coefficients (Kd) of 0.1 cm3 g−1 or less.  相似文献   

7.
Accelerator Mass Spectrometry (AMS) was used to measure 129I/127I ratios in surface sea, lake, and river water samples collected in 2004 and 2005 from the English Lake District and from SW Scotland, areas which are in relatively close proximity to the Sellafield nuclear fuel reprocessing plant in NW England. The 129I/127I ratios in surface water collected from the shore of the Irish Sea were in the range 2.8 × 10−6 to 8.2 × 10−6. These ratios are one order of magnitude higher than that of seawater collected from the Irish Sea in 1992, correlating with the increase in 129I content of the Sellafield liquid effluent discharge over the last decade. The 129I/127I ratios in lakes in the Lake District were in the range 0.7 × 10−6 to 6.4 × 10−6 and decreased exponentially as a function of distance from Sellafield. Consideration of the relative variation of stable I concentrations and 129I/127I ratios suggests that Sellafield gaseous discharges may be the dominant source of 129I to the lakes.  相似文献   

8.
The stable nitrogen and carbon isotope ratios of bone collagen prepared from more than 100 animals representing 66 species of birds, fish, and mammals are presented. The δ15N values of bone collagen from animals that fed exclusively in the marine environment are, on average, 9%. more positive than those from animals that fed exclusively in the terrestrial environment; ranges for the two groups overlap by less than 1%. Bone collagen δ15N values also serve to separate marine fish from the small number of freshwater fish we analyzed. The bone collagen δ15N values of birds and fish that spent part of their life cycles feeding in the marine environment and part in the freshwater environment are intermediate between those of animals that fed exclusively in one or the other system. Further, animals that fed at successive trophic levels in the marine and terrestrial environment are separated, on average, by a 3%. difference in the δ15N values of their bone collagen. Specifically, carnivorous and herbivorous terrestrial animals have mean δ15N values for bone collagen of + 8.0 and + 5.3%., respectively. Among marine animals, those that fed on fish have a mean δ15N value for bone collagen of + 16.5%., whereas those that fed on invertebrates have a mean δ15N value of + 13.3%. These results support previous suggestions of a 3%. enrichment in δ15N values at each successively higher trophic level. In contrast to the results for δ15N values, the ranges of bone collagen δ13C values from marine and terrestrial feeders overlap to a great extent. Additionally, bone collagen δ13C values do not reflect the trophic levels at which the animals fed. These results indicate that bone collagen δ15N values will be useful in determining relative dependence on marine and terrestrial food sources and in investigating trophic level relationships among different animal species within an ecosystem. This approach should be applicable to animals represented by prehistoric or fossilized bone in which collagen is preserved.  相似文献   

9.
Analyses were made of a mollusc‐based meta dataset of 859 δ13C and δ18O data of Miocene nearshore settings in the European Paratethys Sea and its descendant Lake Pannon. The observed trends document a strong tie to geodynamics, which are largely decoupled from Miocene open ocean isotope curves. Semi‐ to fully enclosed, initially marine water bodies such as the Paratethys Sea are prone to switching seawater isotope signatures because they respond rapidly to changes in the evaporation/precipitation ratio. Two phases of positive deviations of oxygen isotope values of water (relative to the modern ocean value, SMOW) occurred during the Middle Miocene; both were initiated by tectonic constrictions of the seaways and became amplified by global warming and regionally decreasing precipitation. With the final disintegration of the Paratethys, the marine isotope signatures vanish. Instead, the observed isotope trends suggest a comparably simple system of an alkaline lake with steadily declining salinity. The ‘ocean‐derived’ Paratethys Sea may thus act as a key for understanding isotope trends in epicontinental seas.  相似文献   

10.
The C and N stable isotope compositions of some flora of East Africa from coastal Tanzania and Amboseli National Park (Kenya) are used to assess if they can be used as a terrestrial end member during the estimation of terrestrial fraction in coastal marine sediments. The results of C isotope composition of various tree leaves, which average −29.3 ± 1.4%, indicate that these tropical higher land plant species follow a Calvin-Benson or non-Kranz (C3) type of metabolism. The results for grass species, which average −13.2 ± 2.4%, indicate that most of them follow a Hatch-Slack or Kranz (C4) type of metabolism. However, some of the succulent plants from the Amboseli National Park have δ13C values that average −14.7%, an indication that they follow a CAM (Crassulacean Acid Metabolism) type of metabolism. The N isotope values are relatively higher than expected for the terrestrial organic material. The average δ15N values for both tree and grass samples are higher than 5% and fall within the range normally considered to be marine. The high enrichment in 15N may be related to the environmental conditions in which plants thrive. Plants growing in sandy, dry and overgrazed environments are expected to be enriched in 15N owing to full utilisation of all available N species, regardless of their isotopic compositions. Other processes which may cause an enrichment in 15N include adsorption by various types of clay minerals, supply of 15N-enriched nitrate through sea-spray, and local denitrification, especially in swampy and lake margins where the input of organic matter may be higher than the rate of decomposition.The stable isotopic composition of organic C and N for surficial organic matter for the coastal marine sediments averages −17.0 ± 0.9% and 5.4 ± 1.1%, respectively. These values indicate a substantial contribution of C4 plants and sea grasses. However, contribution of C4 relative to that of sea grasses can not be evaluated owing to the fact that there is no significant difference in the isotopic compositions between the two groups.In the savannah environment, where a contribution from the C4 types of plants might be substantial, the δ13C value for a terrestrial end member needs to be established prior to evaluation of the terrestrially derived organic matter in the marine environment. Owing to a significant contribution of sea grasses to the total organic matter preserved in coastal marine sediments, the stable isotopes of organic C seem to have a limited applicability as source indicators in the East African coastal waters. Furthermore, the results indicate that N stable isotopes seem to have a limited applicability as source indicators in coastal waters of East Africa. However, more work needs to be conducted to determine the terrestrial and sea grass end member values for the coastal areas.  相似文献   

11.
Fifty-three samples, including brines associated with oil and natural gas reservoirs and groundwater samples from deep boreholes, were collected from the Pacific and Japan Sea coastal regions in Japan. The 129I/127I and 36Cl/Cl ratios, and stable isotopes (δD and δ18O) are compared to investigate differences related to the geotectonic settings of the two regions. The δD and δ18O data indicate that brine and groundwater from the Pacific coastal region reflect mixing of meteoric water with connate seawater in the pores of sedimentary rocks. On the other hand, brine and groundwater from the Japan Sea coastal region have been hydrothermally altered. In particular, brines associated with petroleum accumulations at Niigata and Akita showed the same isotopic characteristics as fluids found in the Kuroko deposits of the Green Tuff region in northeastern Japan. There is little difference in the 36Cl/Cl ratios in brine and groundwater from the Pacific and Japan Sea coasts. Most brine and some deep groundwater, except those from the Pleistocene Kazusa Group, have already reached the average secular equilibrium ratio of 9.9 ± 2.7 × 10−15 for their mudstone and sandstone reservoirs. There was no correlation between the 36Cl/Cl ratios and differences in geotectonic setting between the Pacific and the Japan Sea coast. The molar I/Br ratio suggests that the I in all of water samples was of biogenic origin. The average 129I/127I ratio was 290 ± 130 × 10−15 to 294 ± 105 × 10−15 in both regions, showing no relationship to the different geotectonic settings. The uncontaminated brine and groundwater samples are likely to have retained the original 129I/127I ratios of marine I released from the old organic matter stored in sedimentary rock.  相似文献   

12.
Microbial dissimilatory iron reduction (DIR) has been identified as a mechanism for production of aqueous Fe(II) that has low 56Fe/54Fe ratios in modern and ancient suboxic environments that contain ferric oxides or hydroxides. These studies suggest that DIR could have played an important role in producing distinct Fe isotope compositions in Precambrian banded iron formations or other marine sedimentary rocks. However, the applicability of experimental studies of Fe isotope fractionation produced by DIR in geochemically simple systems to ancient marine environments remains unclear. Here we report Fe isotope fractionations produced during dissimilatory microbial reduction of hematite by Geobacter sulfurreducens in the presence and absence of dissolved Si at neutral and alkaline pH. Hematite reduction was significantly decreased by Si at alkaline (but not neutral) pH, presumably due to Si polymerization at the hematite surface. The presence of Si altered Fe isotope fractionation factors between aqueous Fe(II) or sorbed Fe(II) and reactive Fe(III), reflecting changes in bonding environment of the reactive Fe(III) component at the oxide surface. Despite these changes in isotopic fractionations, our results demonstrate that microbial Fe(III) oxide reduction produces Fe(II) with negative δ56Fe values under conditions of variable pH and dissolved Si, similar to the large inventory of negative δ56Fe in Neoarchean and Paleoproterozoic age marine sedimentary rocks.  相似文献   

13.
Iodine-129 (t12, 16 My) is a naturally-occurring tracer which can be used to study hydrologic and geologic processes on time scales up to 100 My. The pre-bomb atmospheric ratio 129II should have been constant in time and space and is the starting value in ground-water recharge. Subsequent ratio changes in ground water should be determined by isotope contributions from three sources: recharge water, iodine leached from the formation, and in situ uranium fission. The mathematical expression of these time-dependent processes forms the basis for dating and tracing applications.The expected behavior of natural 129I in ground water is compared to results from field studies. Ground-water samples from the Great Artesian Basin, Australia, provide an estimate of the atmospheric equilibrium ratio, 6 × 10?13. Down-gradient changes in water up to 1 My old suggest that subsurface production can be significant. The usefulness of 129I as an indicator of brine source and age is verified in brines collected in and around Louisiana salt domes. The method leads to ages of 7 and 9 My for two brine pockets trapped within Jurassic salt, and 32 to >40 My for oil-field brines in Miocene sands adjacent to the domes.The results demonstrate the capability of tandem accelerator mass spectrometry to measure as few as 107 atoms of 129I in 10 mg I with 10% precision. Although such atom sensitivity can be achieved otherwise, the accelerator technique is necessary to measure naturally low pre-1945 cosmogenic isotope ratios.  相似文献   

14.
Representative samples of crude oils from Cusiana, Cupiagua, Apiay, Castilla and Chichimene fields in the Eastern Llanos Basin of Colombia were analyzed to determine its compound-specific stable carbon isotope composition (CSIA) using gas chromatography–isotopic ratio–mass spectrometry (GC–IRMS). GC–IRMS analyses of n-alkanes allowed differentiating between Cretaceous and Cretaceous/Tertiary oil samples. Cretaceous sourced samples have δ13C-enriched values than Cretaceous/Tertiary sourced samples; the heavier isotope composition of these samples is due to their major terrigenous organic matter input. Their isotope distribution patterns suggest significant algal and/or bacterial contribution (marine origin). The analysis of the n-alkane fractions by GC–IRMS confirms that the organic matter has marine origin in those samples from Cusiana, Cupiagua and Apiay while Castilla and Chichimene have marine origin with terrestrial inputs. The results were confirmed by gas chromatography/FID and gas chromatography/mass spectrometry (GC/MS). Basic geochemical composition show that samples from Cupiagua/Cusiana fields and Apiay/Castilla/Chichimene fields in the Llanos basin, Colombia present different characteristics reflecting a specific for each depositional environment.  相似文献   

15.
Determining sources of sediment to coastal systems is an important and complex problem that figures prominently in a myriad of geological, geomorphological, geochemical, and biological processes. Lithogenic (226Ra,228Ra,228Th,230Th,232Th) and fallout (137Cs,210Pb) isotopes were employed in conjunction with sedimentological methods to determine rates of sedimentation in the Nueces Delta and Nueces-Corpus Christi Estuary and to assess the relative importance of marine versus terrestrial sediment sources to the estuary. Similarity of lithogenic isotope ratios in surface sediments throughout the system precluded a numeric approach to discerning the importance of each of the two large scale sediment sources (terrestrial and marine). A stepwise, graphical examination of discrete lithogenic isotope activity concentrations shows more promise. Terrestrial, marine, and bay sediment means for226Ra versus232Th,226Ra versus230Th, and228Ra versus232Th show that terrestrial and marine sediment sources have different signatures, despite having similar grain size distributions (sands), and that sediment deposited in Nueces and Corpus Christi Bays are indistinguishable from the terrestrial component. Supporting evidence is provided by thorium isotopes,230Th versus232Th,228Th versus232Th, and228Th versus230Th. Nueces Delta sedimentation (0.09–0.53 g cm−2 yr−1) shows a subtle gradient, with rates generally lower in the west and progressively higher moving east, likely reflecting contrasts in land use and topography. Nueces Bay cores differ from those in Corpus Christi Bay in that sands comprise a larger percentage of their composition, and they are mixed over greater depth, most likely due to geographic and physiographic effects. Sediment accumulation rates consistently decrease over the first 20 km from the Nueces River and become constant after that, implying that the river is the most significant source of sediment to the estuary. The interpretation of sediment supply to this estuary as dominated by terrestrial inputs is based on three complimentary sets of data: sediment grain size distributions, discrete lithogenic isotope data (Ra versus Th and Th versus Th), and sediment accumulation rates for both Nueces and Corpus Christi Bays.  相似文献   

16.
Iodine enrichment in the Atacama Desert of northern Chile is widespread and varies significantly between reservoirs, including nitrate-rich “caliche” soils, supergene Cu deposits and marine sedimentary rocks. Recent studies have suggested that groundwater has played a key role in the remobilization, transport and deposition of iodine in Atacama over scales of millions-of-years. However, and considering that natural waters are also anomalously enriched in iodine in the region, the relative source contributions of iodine in the waters and its extent of mixing remain unconstrained. In this study we provide new halogen data and isotopic ratios of iodine (129I/I) in shallow seawater, rivers, salt lakes, cold and thermal spring water, rainwater and groundwater that help to constrain the relative influence of meteoric, marine and crustal sources in the Atacama waters. Iodine concentrations in surface and ground waters range between 0.35 μM and 26 μM in the Tarapacá region and between 0.25 μM and 48 μM in the Antofagasta region, and show strong enrichment when compared with seawater concentrations (I = ∼0.4 μM). In contrast, no bromine enrichment is detected (1.3–45.7 μM for Tarapacá and 1.7–87.4 μM for Antofagasta) relative to seawater (Br = ∼600 μM). These data, coupled to the high I/Cl and low Br/Cl ratios are indicative of an organic-rich sedimentary source (related with an “initial” fluid) that interacted with meteoric water to produce a mixed fluid, and preclude an exclusively seawater origin for iodine in Atacama natural waters. Iodine isotopic ratios (129I/I) are consistent with halogen chemistry and confirm that most of the iodine present in natural waters derives from a deep initial fluid source (i.e., groundwater which has interacted with Jurassic marine basement), with variable influence of at least one atmospheric or meteoric source. Samples with the lowest isotopic ratios (129I/I from ∼215 to ∼1000 × 10−15) strongly suggest mixing between the groundwater and iodine storage in organic-rich rocks (with variable influence of volcanic fluids) and pre-anthropogenic meteoric water, while samples with higher values (∼2000–93,700 × 10−15) indicate the input of anthropogenic meteoric fluid. Taking into account the geological, hydrologic and climatic features of the Atacama region, we propose that the mean contribution of anthropogenic 129I is associated with 129I releases during nuclear weapon tests carried out in the central Pacific Ocean until the mid 1990's (129I/I = ∼12,000 × 10−15). This source reflects rapid redistribution of this radioisotope on a global scale. Our results support the notion of a long-lived continental iodine cycle in the hyperarid margin of western South America, which is driven by local hydrological and climate conditions, and confirm that groundwater was a key agent for iodine remobilization and formation of the extensive iodine-rich soils of Atacama.  相似文献   

17.
The Fruitland Formation of the San Juan Basin was deposited during the late Cretaceous and is associated with significant reservoirs of coalbed methane (CBM). The purpose of this study is to determine the origin and history of waters associated with the formation, using long-lived cosmogenic and stable isotope systems. Ratios of 129I/I and stable isotope values (δD and δ18O) were determined in waters from close to 100 wells, 36Cl/Cl ratios for a subset of these samples. A significant group of samples has 129I/I ratios between 100 × 10−15 and 200 × 10−15, indicating minimum iodine ages close to 60 Ma. If these ages are corrected for the addition of fissiogenic 129I, they are compatible with the depositional age of the Fruitland Formation (Late Cretaceous).Several sets of waters are clearly present within the data. A group dominated by infiltration of recent surface waters is restricted to the uplifted basin margins, with a lateral extent of less than 5 km from outcrop, and is characterized by 129I/I ratios in excess of 1500 × 10−15 and meteoric δD, δ18O, and 36Cl/Cl signatures. The rest of the basin is characterized by several subsets of formation waters which have undergone variable degrees of iodine enrichment through diagenesis as well as variable degrees of dilution. The first subgroup is found in coals of relatively low vitrinite reflectance and moderate enrichment of iodine. This subgroup predominantly consists of entrapped pore fluids, although it may also contain waters which infiltrated the coals at the time of the Laramide uplift, between 25 and 30 Ma. A second subgroup consists of formation waters associated with coals of high vitrinite reflectance. Despite subsequent uplift, the high iodine concentrations and low 129I/I ratios of this subgroup, as well as a moderate depletion of deuterium relative to 18O, suggest that these waters were not significantly altered since the time when diagenetic reactions occurred in the deepest portion of the basin. A third subgroup, with higher δD and δ18O values as well as higher 129I/I ratios, extends roughly west to east at the New Mexico-Colorado state line and corresponds to a region of extensive fracturing of the coalbeds. In this case, the higher 129I/I ratios are probably due to contributions of fissiogenic 129I through fracture flow, perhaps from deeper formation waters. Our results do not support models of subsequent basin-wide groundwater migration in the Fruitland Formation. The combined use of 129I and 36Cl with stable isotope studies provides valuable information as to the hydrologic history of coalbed methane deposits, as well as their potential for commercial exploitation.  相似文献   

18.
129I is one of the three major radiation risk contributors to the public as a consequence of past nuclear processing activities at Department of Energy (DOE) facilities. Elevated levels of 129I are present in the surface soils of F-Area of Savannah River Site, which used to be an isotope separation facility for the production of nuclear weapons components. The 129I in soils is thought to be bound predominantly to soil organic matter (SOM). Measurements of stable 127I and radioactive 129I in humic acids (HAs) and fulvic acids (FAs) obtained by five successive alkaline, two glycerol and one citric acid-alkaline extraction, demonstrated that these extractable humic substances (HS) together account for 54-56% and 46% of the total 127I and 129I in the soil, respectively. The remainder was likely bound to residual SOM. The iodine content (μg-I/g-C) generally decreased with each subsequent extract, while 129I/127I increased concurrently. The coincident variations in chemical compositions, aromaticity (estimated by UV spectroscopy), functional groups (e.g., aliphatic), degree of humification, relative migration in the hydrophobic interaction column, and molecular weight indicated that: (1) iodine in different HAs was bound to a small-size aromatic subunit (∼10 kDa); (2) the large-size subunit (∼90 kDa), which likely linked the small-size unit through some weak chemical forces (hydrogen bonds, hydrophobic or electrostatic interactions), determined the relative mobility of iodine bound to organic matter; (3) from the strong correlation between iodine content and aromaticity in the HAs, we suggested that iodine incorporation into the SOM via covalent aromatic C-I bond is the key mechanism controlling iodine behavior in this system. However, this relationship is not universal for all fractions of organic matter as evidenced from the different slopes of this relationship at the two sampling sites, as well as from the different relationships for HAs and FAs, respectively. These differences in iodination are due to different SOM molecular sizes, compositions, and availability of preferred iodination sites. 129I in the soil downstream from the contaminated site and near a wetland abruptly dropped below our detection limit (0.5 pCi-129I/g-soil), which suggests that the high SOM in the plume soil around the 129I-contaminated F-Area might be a natural barrier to scavenge radioiodine released from the nuclear waste repository by forming organo-iodine compounds. Soil resuspension experiments showed that mobile 129I was mostly associated with a low average molecular weight amphiphilic organic carrier (13.5-15 kDa). SOM clearly behaves as a sink for iodine at the Savannah River Site F-Area. However, this work demonstrates that a small fraction of the SOM can also behave as a source, namely that a small fraction that may be readily dispersible under some environmental conditions and presumably release iodine in the organic-colloidal form. This radioiodinated organo-colloid likely can get into the groundwater through infiltration or surface runoff where it might migrate further into the wetlands. Results from this study provide the geochemical basis for future 129I migration controls, remediation, and/or land-groundwater management strategies.  相似文献   

19.
Large rounded pyrite grains (>1 mm), commonly referred to as “buckshot” pyrite grains, are a characteristic feature of the auriferous conglomerates (reefs) in the Witwatersrand and Ventersdorp supergroups, Kaapvaal Craton, South Africa. Detailed petrographic analyses of the reefs indicated that the vast majority of the buckshot pyrite grains are of reworked sedimentary origin, i.e., that the pyrite grains originally formed in the sedimentary environment during sedimentation and diagenesis. Forty-one of these reworked sedimentary pyrite grains from the Main, Vaal, Basal, Kalkoenkrans, Beatrix, and Ventersdorp Contact reefs were analyzed for their multiple sulfur isotope compositions (δ34S, Δ33S, and Δ36S) to determine the source of the pyrite sulfur. In addition, five epigenetic pyrite samples (pyrite formed after sedimentation and lithification) from the Middelvlei and the Ventersdorp Contact reefs were measured for comparison. The δ34S, Δ33S, and Δ36S values of all 41 reworked sedimentary pyrite grains indicate clear signatures of mass-dependent and mass-independent fractionation and range from ?6.8 to +13.8?‰, ?1.7 to +1.7?‰, and ?3.9 to +0.9?‰, respectively. In contrast, the five epigenetic pyrite samples display a very limited range of δ34S, Δ33S, and Δ36S values (+0.7 to +4.0?‰, ?0.3 to +0.0?‰. and ?0.3 to +0.1?‰, respectively). Despite the clear signatures of mass-independent sulfur isotope fractionation, very few data points plot along the primary Archean photochemical array suggesting a weak photolytic control over the data set. Instead, other factors command a greater degree of influence such as pyrite paragenesis, the prevailing depositional environment, and non-photolytic sulfur sources. In relation to pyrite paragenesis, reworked syngenetic sedimentary pyrite grains (pyrite originally precipitated along the sediment-water interface) are characterized by negative δ34S and Δ33S values, suggesting open system conditions with respect to sulfate supply and the presence of microbial sulfate reducers. On the contrary, most reworked diagenetic sedimentary pyrite grains (pyrite originally precipitated below the sediment-water interface) show positive δ34S and negative Δ33S values, suggesting closed system conditions. Negligible Δ33S anomalies from epigenetic pyrite suggest that the sulfur was sourced from a mass-dependent or isotopically homogenous metamorphic/hydrothermal fluid. Contrasting sulfur isotope compositions were also observed from different depositional environments, namely fluvial conglomerates and marine-modified fluvial conglomerates. The bulk of the pyrite grains from fluvial conglomerates are characterized by a wide range of δ34S values (?6.2 to +4.8?‰) and small Δ33S values (±0.3?‰). This signature likely represents a crustal sulfate reservoir derived from either volcanic degassing or from weathering of sulfide minerals in the hinterland. Reworked sedimentary pyrite grains from marine-modified fluvial conglomerates share similar isotope compositions, but also produce a positive Δ33S/δ34S array that overlaps with the composition of Archean barite, suggesting the introduction of marine sulfur. These results demonstrate the presence of multiple sources of sulfur, which include atmospheric, crustal, and marine reservoirs. The prevalence of the mass-dependent crustal sulfur isotope signature in fluvial conglomerates suggests that sulfate concentrations were probably much higher in terrestrial settings in comparison to marine environments, which were sulfate-deficient. However, the optimum conditions for forming terrestrial sedimentary pyrite were probably not during fluvial progradation but rather during the early phases of flooding of low angle unconformities, i.e., during retrogradational fluvial deposition, coupled in some cases with marine transgressions, immediately following inflection points of maximum rate of relative sea level fall.  相似文献   

20.
A variety of approaches have previously been developed to estimate the fraction of terrestrial or marine organic carbon present in aquatic sediments. The task of quantifying each component is especially important for the Arctic due to the regions’ sensitivity to global climate change and the potential for enhanced terrestrial organic carbon inputs with continued Arctic warming to alter carbon sequestration. Yet it is unclear how each approach compares in defining organic carbon sources in sediments as well as their impact on regional or pan-Arctic carbon budgets. Here, we investigated multiple methods: (1) two end-member mixing models utilizing bulk stable carbon isotopes; (2) the relationship between long-chain n-alkanes and organic carbon (ALKOC); (3) principal components analysis (PCA) combined with scaling of a large suite of lipid biomarkers; and (4) ratios of branched and isoprenoid glycerol dialkyl glycerol tetraether lipids (the BIT index) to calculate the fraction of terrestrial organic matter components preserved in Arctic marine sediments.Estimated terrestrial organic carbon content among approaches showed considerable variation for identical sediment samples. For a majority of the samples, the BIT index resulted in the lowest estimates for terrestrial organic carbon, corroborating recent suggestions that this proxy may represent a distinct fraction of terrestrial organic matter; i.e., peat or soil organic matter, as opposed to markers such as n-alkanes or long-chain fatty acids which measure higher plant wax inputs. Because of the patchy inputs of n-alkanes to this region from coastal erosion in the western Arctic, the ALKOC approach was not as effective as when applied to river-dominated margins found in the eastern Arctic. The difficulties in constraining a marine δ13C end-member limit the applicability of stable isotope mixing models in polar regions. Estimates of terrestrial organic carbon using the lipid-based PCA method and the bulk δ13C mixing model approach varied drastically at each site, suggesting that organic matter fractions such as amino acids or carbohydrates may affect bulk organic matter composition in a manner that is not captured in the lipid-based analysis. Overall, terrestrial organic matter inputs to the Chukchi and western Beaufort Seas using the average of the methods at each site ranged from 11% to 44%, indicating that land-derived organic matter plays a substantial role in carbon dynamics in the western Arctic Ocean.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号