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1.
239 + 240Pu activities of 100–450dpm/kg are found down to 15–18 cm in anoxic Saanich Inlet sediments, with a subsurface maximum in undisturbed deposits. Integrated 239 + 240Pu inventories which overlap delivery estimates are present both in two cores of anoxic sediments from Saanich Inlet and in one core of oxic sediments 65 km away in Dabob Bay, Washington. 241Am239 + 240Pu ratios in Saanich Inlet sediments overlap ratios in unfractionated midnorthern latitude fallout, in oxic sediments from the Washington continental shelf, and in anoxic sediments from two basins off southern California and Mexico. The 239 + 240Pu137Cs ratios in three intervals of Saanich Inlet sediments are also in agreement with ratios previously reported for oxic coastal marine sediments. The Pu inventories, the AmPu and PuCs ratios, and the Saanich Inlet Dabob Bay comparison all argue that Pu is not rapidly remobilized in anoxic sediments.The subsurface 239 + 240Pu activity maximum is not in agreement with the historical record of peak Pu fallout in 1963–1964 unless our 210Pb-derived sedimentation rates are incorrectly high. However, they are in good agreement with previous 210Pb and varve chronologies in Saanich Inlet, and also give reasonable dates for times when 239 + 240Pu and SNAP-9A supplied 238Pu first appear in the sediments. We conclude they properly date the maximum in sedimentary 239 + 240Pu activity at 1970–1973, and seek explanations for the 7–10yr time lag after peak fallout.239 + 240Pu inventories in one core from the eastern basin of the Cariaco Trench and in two cores from Golfo Dulce. an anoxic basin off the Pacific coast of Costa Rica, are also in reasonable agreement with fallout delivery to these latitudes when excess 210Pb inventories and fluxes are used to verify recovery of at least a major fraction of the most recently deposited sediments.  相似文献   

2.
The collection of large volumes of pore water (1–2 liters per 2 cm horizon of sediment) and low level radiochemical measurements of 239,240Pu and 137Cs have been combined to produce the first study of these fallout artificial radionuclides in marine pore waters. Profiles from box cores taken in June and September 1982 from Buzzards Bay, Mass., are reported along with profiles of many diagenetic constituents (i.e. SO42?, alkalinity, Fe, Mn, DOC, and nutrients).The 239,240Pu pore water profile is characterized by a subsurface maximum of about 0.28 dpm/100 kg lying between 3–11 cm. Overlying seawater, in contrast, has an activity of 0.01 ± 0.02 dpm/100 kg. Below about 11 cm, the pore water 239,240Pu distribution follows that of the solid phase which decreases rapidly with depth. The pore water profiles of 137Cs are characterized by a broad and deeply penetrating maximum where activities of about 35–40 dpm/100 kg extend from 3 to 20 cm. Overlying seawater, in contrast, has an activity of 17–24 dpm/100 kg. The 137Cs and 239,240Pu pore water data show that there is preferential downward transport of 137Cs and that 239,240Pu does not have an active diagenetic chemistry and is not significantly mobile in these coastal sediments.  相似文献   

3.
The concentrations of 238Pu, 239 + 240Pu, 241Am and 137Cs were determined in rain samples collected at Monaco in the course of 1978–1979. Based on these data, the annual deliveries of these radionuclides to the Mediterranean by rain are computed to be 0.18 ± 0.01 pCim?2 for 238Pu, 8.1 ± 0.1 pCim?2 for 239 + 240Pu, 0.58 ± 0.02 pCim?2 for 241Am and 351 ± 4 pCim?2 for 137Cs.Comparing the delivery data with the mixed layer inventories of 239 + 240Pu and 241Am in the Mediterranean, the upper limits of the mean residence time of these radionuclides in the mixed layer were estimated to be 12.3 yr for 239 + 240pu and 2.9 yr for 241Am. These values are consistent with the conclusion deduced from the vertical distribution pattern of these transuranic elements in the Mediterranean.Based on delivery values, the annual activity ratios for 238pu239 + 240Pu, 241Am239 + 240Pu and 239 + 240pu137Cs are found to be 0,022, 0.072 and 0.023 respectively. The 238pu239 + 240pu and 239 + 240Pu137Cs activity ratios vary within relatively narrow ranges with time, while a much wider variation was observed for the 241Am239 + 240Pu activity ratio. The cause of the wider variation of the 241Am239 + 240Pu ratio may be related to the difference in the mean age of fallout brought down in different seasons.  相似文献   

4.
Continental shelf sediments from nine locations off Washington and Oregon have 239,240Pu inventories which average 8.0 ± 2.6 mCi/km2. The Columbia River and seawaters advecting over the shelf supply Pu which is removed to underlying sediments, principally through scavenging by inorganic paniculate matter. Mass balance calculations argue that less than 20 percent of the advected Pu need be scavenged from the water column to balance river input and total shelf sediment inventories. The percentage of the Pu removed through scavenging is consistent with observed participate concentrations in shelf waters and published sediment/water distribution coefficients.No marked separation of Pu from 137Cs is observed with depth in Pacific shelf sediments as has been reported in Atlantic coastal sediments. This interocean distinctness can be explained by differences in particle mixing and downward diffusion of Cs in sediments of varying porosities. The transuranic inventories and Pu/Cs ratios in the Pacific sediments do not support the hypothesis of Livingston and Bowen that Pu is remobilized within the sediment column by ‘complexone’ formation with (principally) organic substances.Excess 210Pb/239,240Pu inventory ratios in eight representative cores from the Washington shelf average 100 ± 19, even though absolute values of both inventories vary by much larger factors. This reasonably constant ratio, for a given water depth, permits estimation of total Pu inventories and prediction of sites of unusual Pu accumulation from data on the more easily measured natural radionuclide.  相似文献   

5.
Two very different sets of 244Pu238U ratios have been reported for early solar system materials. One group of samples yields high (0.015–0.016) ratios (Podosek, 1970a, 1972; Drozd et al., 1977) and calculations based on another group of analyses yield low ratios (~0.004) (Marti et al., 1977). Recently measured partition coefficients for Pu and Sm are used to evaluate the data of Marti et al. and sol244Pu238U ratios from other sources are also considered. A low sol244Pu238U ratio (~0.005) is favored, and some implications of this low ratio to galactic nucleosynthesis and meteorite age dating are briefly discussed.  相似文献   

6.
228Ra, 226Ra, and 222Rn activities were determined on over 150 ground water samples collected from drilled, public water supply wells throughout South Carolina. A wide range of aquifer lithologies were sampled including the crystalline rocks of the Piedmont and sedimentary deposits of the Coastal Plain. A significant linear relationship between log 228Ra and log 226Ra (n = 182, r = 0.83) was indistinguishable between Piedmont and Coastal Plain ground water. Median 228Ra226Ra activity ratios for the Piedmont, 1.2, and Coastal Plain, 1.3, ground water are close to estimated average crustal 232Th238U activity ratios of 1.2 to 1.5 corresponding to Th/U weight ratios of 3.5 to 4.5. A linear correlation was also found between log 222Rn and log 226Ra for Piedmont (n = 68, r = 0.62) and Coastal Plain (n = 89, r = 0.64) ground water. However, the median 222Rn226Ra activity ratio for Piedmont ground water, 6100, was much higher than for Coastal Plain ground water, 230. Higher excess 222Rn activities may be due to greater retention of 226Ra by the chemically active Piedmont aquifers compared to the more inert sand aquifers sampled in the Coastal Plain. The relationship between log 228Ra and log 226Ra was used to predict total Ra (228Ra + 226Ra) distributions in Appalachian and Atlantic and Gulf Coastal Plain ground water. Predictions estimate that 2.4% of Appalachian and 5.3% of Atlantic and Gulf Coastal Plain ground water supplies contain total Ra activities in excess of the 5 pCi/l limit established by the U.S. Environmental Protection Agency. These predictions also indicate that 40–50% of these ground water wells may be overlooked using the presently suggested screening activity of 3.0 pCi/l of 226Ra for 228Ra analysis.  相似文献   

7.
The 10Be contents of 28 stony meteorites with known 21Ne contents range from 0.97 to 23 dpm/kg and give an average 21Ne production rate (P21) of (0.28 ± 0.02) × 108 cm3 STP/g-Myr for shielding conditions corresponding to 22Ne21Ne = 1.114 in an H-chondrite. Our P21(10Be) agrees with others' P21 based on 22Na, 81Kr and 53Mn but not on 26A1. Temporal variations in the cosmic ray flux do not explain the disagreement satisfactorily; major errors in the radionuclide half-lives are not indicated. The discrepancy seems rooted in the data selection and the difficulties of making accurate corrections for shielding, chemical composition and other sources of variability.  相似文献   

8.
Approximately one thousand drilled wells were investigated for their natural radioactivity. The determinations of 238U, 234U, 226Ra and 222Rn from 310 samples showed a high state of radioactive disequilibrium between the members of the uranium series present in water. The 238U226Ra activity ratio usually fell in the range 1–20 and the 238U222Rn activity ratio in the range 1–20 × 10?4, the highest activity ratios being from samples with an elevated uranium content. The 234U238U activity ratio varied between 0.76 and 4.67, the most frequent values showing a 60% excess of 234U in the samples. Most of the 234U238U activity ratios near unity were found in samples with a high uranium content. Several drilled wells with anomalously high uranium contents were found in southern Finland. The average 226Ra and 222Rn contents of these wells were not exceptionally high, which suggests high mobility of uranium in groundwater from the areas involved.  相似文献   

9.
The concentrations of noble gas isotopes of He, Ne and Ar have been measured in eight mineral separates of the Bruderheim chondrite. The cosmic-ray-produced nuclides 21Ne and 38Ar were correlated by a computer least-squares fitting program with the elemental composition in each separate of potential targets for nuclear production yielding the following production equations: [21Ne, 10?8 cm3/g] = k(0.45[Mg] + 0.085[Si] + 0.060[S] + 0.017[Ca] + 0.0044[Fe + Ni]); [38Ar, 10?8 cm3/g] = k(2.6[K] + 0.37[Ca] + 0.08[Ti + Cr + Mn] + 0.021[Fe + Ni]) with elemental concentrations in weight per cent and k equal to the reciprocal of the cosmic-ray exposure age of Bruderheim. The P(S)/P(Cr + Mn + Fe + Ni) weight production ratio for 3He was determined to be 1.53; relative productions of 3He from O, Mg and Si and 21Ne from Al proved to be incalculable.  相似文献   

10.
A detailed study of the U distribution of the St. Severin chondrite has been made by fission track radiography in order to clarify the interpretation of fission Xe thermal release data in terms of the mineralogical location of the fission Xe within the meteorite. This is of importance because the 244Pu238U ratio for St. Severin has been widely adopted as the average solar system value. The U contents of the constituent minerals cannot account for the total rock U which, instead, appears to be primarily localized on grain boundaries. The greatest localizations of U are in olivine-poor, orthopyroxene-rich ‘clasts’. Our data coupled with those of Podosek (1970a) show that 244Pu in St. Severin was also located on grain boundaries and that the bulk of Pu and U are unfractionated within this meteorite. Due to recoil, the 244Pu fission Xe is found in 10 micron surface layers on major phases. Assuming that the grain boundaries (on which the Pu was located) was formed during metamorphism, the 244Pu238U ratio for St. Severin applies to a time subsequent to the textural recrystallization of the meteorite. Our data support the interpretation of Podosek and our best estimate of the solar system 244Pu238U is 0.015.  相似文献   

11.
The Rameka Gabbro, emplaced 367 Ma ago, experienced a well documented reheating on intrusion of the Separation Point Batholith 114 Ma ago. 40Ar39Ar age spectrum analyses of hornblende from the Rameka Gabbro show diffusion gradients which provide information on the 40Ar boundary concentration during reheating.Three samples of hornblende exhibit age spectra that conform to a model of 40Ar loss by diffusion, implying a zero 40Ar boundary concentration during heating. The calculated 40Ar loss from these samples, together with a model of heat flow in the aureole, provide estimates of diffusion coefficients of 40Ar in Mg-rich hornblende which correspond to an activation energy, E, of ~60 kcal-mol?1 and a frequency factor. D0, of ~ 10?3 cm2-sec?1. When combined with laboratory diffusion results, these data yield a well defined diffusion law (E = 63.3 ± 1.7 kcal-mol?1, D0 = 0.022 +0.048?0.010cm2-sec?1).The age spectra of the eight other samples record steep gradients of excess 40Ar over the first few percent of gas release. Although this effect causes high apparent conventional K-Ar ages, the plateau segments of many sampes still record the crystallization age of 367 ± 5 Ma. These measurements show that the excess 40Ar phase developed locally in the intergranular regions of the gabbro, following intrusion of the batholith. on time scales that varied from 104 to 106years. The minimum average 40Ar36Ar ratio of this component was found to be 1300 ± 400. The partial pressure of Ar was at least 10?2 bars in some places.A single 40Ar39Ar age spectrum analysis of plagioclase reveals a ‘saddle-shaped” release pattern with a minimum at 140 Ma.In conjunction with theoretical diffusion models and a diffusion law, 40Ar39Ar age spectrum analysis of hornblende that has experienced a post-crystallization heating can provide close estimates of the maximum temperature of the thermal event as well as both age of crystallization and reheating.  相似文献   

12.
Diffusion of ions in sea water and in deep-sea sediments   总被引:3,自引:0,他引:3  
The tracer-diffusion coefficient of ions in water, Dj0, and in sea water, Dj1, differ by no more than zero to 8 per cent. When sea water diffuses into a dilute solution of water, in order to maintain the electro-neutrality, the average diffusion coefficients of major cations become greater but of major anions smaller than their respective Dj1 or Dj0 values. The tracer diffusion coefficients of ions in deep-sea sediments, Dj,sed., can be related to Dj1 by Dj,sed. = Dj1 · αθ2, where θ is the tortuosity of the bulk sediment and a a constant close to one.  相似文献   

13.
87Sr86Sr measurements of 108 sedimentary carbonate rocks have been used to trace variations in the strontium isotopic composition of seawater during the Phanerozoic. The lowest 87Sr/86Sr observed for any suite of carbonates is taken as the best approximation to the value in well-mixed contemporary seawater. Our data support the existence of low 87Sr86Sr in the Cretaceous and Late Jurassic but they do not support further structure beyond a general trend through the Phanerozoic, which may correlate with the continental denudation rate.  相似文献   

14.
The decay constant 87Rb has been redetermined by measuring the amount of radiogenic 87Sr produced over a period of 19 years, in 20 g samples of purified RbClO4, using isotope dilution techniques. The rubidium sample was spiked with 84Sr and the nanogram quantities of strontium separated by coprecipitation with Ba(NO3)2. Analyses were carried out on a 25cm, 90° sector mass spectrometer equipped with a Spiraltron electron multiplier. Measurement of three independent ratios permitted continuous monitoring of the ion beam fractionation. The average of nine determinations gives a value for the decay constant of 1.419(±0.012) × 10?11 yr?1 (2σ). [τ12 = 4.89(±0.04) × 1010yr.]  相似文献   

15.
Isotopes of plutonium (Pu), cesium (Cs), and cobalt (Co) introduced into the Hudson River Estuary from fallout deposition, the erosion of fallout-contaminated surface soils, and nuclear reactor effluent (isotopes of Cs and Co only) have been measured in water column samples collected from 1975 to 1980 Isotopic measurements conducted independently by two research groups utilizing different sampling and analytical techniques have been summarized. The major conclusions drawn from the work are that for water samples collected by the two laboratories over similar time periods, the mean concentrations of nonfilterable239,240Pu (<0.45 μm) were identical at 0.13 fCi/l, mean concentrations of both137Cs and239,240Pu in suspended particulates were more divergent at 2,270±920 pCi/kg (±1 SD) and 1,430±430 pCi/kg for137Cs, and 19±8 pCi/kg and 12±4 pCi/kg for239,240Pu The behavior of239,240Pu and137Cs within the water column is shown to diverge within brackish waters Specifically, the magnitude of the137Cs distribution coefficient (K d ) can be expressed as an inverse power function of the chloride ion concentrations for chlorinities between 0.1 and 4 g Cl/l No difference in the239,240PuK d has been observed between fresh and brackish waters Based on the expected inventories of239,240Pu and137Cs within watershed soils, the current downstream transport of these radionuclides represents fractional mobilization rates on the order of 1–4 (×10−4) per year  相似文献   

16.
Al26 and noble gas contents of 6 ordinary chondrites with He3Ne21 ratios above 6.0 or below 4.0 are used to infer the variability of the production rates of He3 and Ne21 (PHe3 and PNe21). The ratio of the observed Al26 content to a calculated, normal value is taken as a measure of the change of PNe21 from its normal value. The corresponding change in PHe3 is then computed from the observed He3Ne21 ratio and an average value of PHe3.According to these calculations which exclude orbital effects, PHe3 will be near the average value in meteorites with high He3Ne21 ratios, while PNe21 will be about 30 per cent below normal. In meteorites with low He3Ne21 ratios, PHe3 may be depressed by as much as 25 per cent from normal while PNe21 may be 15–20 per cent above the average.  相似文献   

17.
HD Fractionation factors between epidote minerals and water, and between the AlO(OH) dimorphs boehmite and diaspore and water, have been determined between 150 and 650°C. Small water mineral ratios were used to minimise the effect of incongruent dissolution of epidote minerals. Waters were extracted and analysed directly by puncturing capsules under vacuum. Hydrogen diffusion effects were eliminated by using thick-walled capsules.HD Exchange rates are very fast between epidote and water (and between boehmite and water), complete exchange taking only minutes above 450°C but several months at 250°C. Exchange between zoisite and water (and between diaspore and water) is very much slower, and an interpolation method was necessary to determine fractionation factors at 450 and below.For the temperature range 300–650°C, the HD equilibrium fractionation factor (αe) between epidote and water is independent of temperature and Fe content of the epidote, and is given by 1000 In αepidote-H2Oe = ?35.9 ± 2.5, while below 300°C 1000 In αepidote-H2Oe = 29.2(106T2) ? 138.8, with a ‘cross-over’ estimated to occur at around 185°C. By contrast, zoisite-water fractionations fit the relationship 1000 In αzoisite-H2Oe = ? 15.07 (106T2) ? 27.73.All studied minerals have hydrogen bonding. Fractionations are consistent with the general relationship: the shorter the O-H -- O bridge, the more depleted is the mineral in D.On account of rapid exchange rates, natural epidotes probably acquired their H-isotope compositions at or below 200°C, where fractionations are near or above 0%.; this is in accord with the observation that natural epidotes tend to concentrate D relative to other coexisting hydrous minerals.  相似文献   

18.
The distribution of 210Pb, 137Cs, and Ambrosia (ragweed) pollen in two sediment cores from Lake Ontario and in three cores from Lake Erie provides independent estimates of sediment accumulation rates. Geochronology with 210Pb is based on radioactive decay of the isotope following burial in sediments. The method can reveal with precision changes in sedimentation occurring over the past 100 yr or so. Geochronologies with 137Cs and Ambrosia are based on the occurrence of a horizon corresponding, respectively, to the onset of nuclear testing 25 yr ago and to regional forest clearance in the middle 1800s. These methods provide estimates of long-term average sediment accumulation rates. In all but one core, the distributions of 137Cs and 210Pb indicate no physical mixing of near-surface sediments. In two cores, including one from central Lake Erie collected by diver, all three estimates of sedimentation rates are in excellent agreement. In two other cores, rates based on 210Pb are significantly higher than those inferred from Ambrosia pollen profiles. Lower average rates appear to result from occasional massive losses of sediments. Such events, apparent in the distribution of 210Pb but not in pollen records, correlate with the occurrence of major storm surges on the lakes during this century. In one core from western Lake Erie, exponential distributions of both 210Pb and Ambrosia appear to be artifacts which may result from extensive biological or physical reworking of sediments in shallow water (11 m). Previous indications of increased sedimentation in Lake Erie since about 1935 based on Castanea (chestnut) pollen data are not substantiated.  相似文献   

19.
The 26Al, light rare gas and major and minor element contents of Al-rich and poor samples separated from Allende. Bereba and Junivas have been measured. The production rate of 21Ne from Al (21PAl) is (1.9 ± 0.6) × 21PSi and 2221PAl = 1.4 ± 0.4. The 3He, 21Ne and 38Ar exposure ages of the eucritic pyroxenes agree suggesting complete cosmogenic gas retention. The eucritic feldspars have lost virtually all 3He and most radiogenic 4He. The equation 26Al = 0.42 ± 0.41 Mg + 2.74 ± 0.21 Si + 4.92 ± 0.51 Al + 1.33 S + 0.24 Ca + 0.03 Fe reproduces within 15% our 26Al measurements and the average values measured in ordinary chondrites without recourse to unusual cosmic-ray effects.  相似文献   

20.
Controlled laboratory experiments have been used to study the diagenetic chemistry of 239,240Pu 137Cs, and 55Fe. Experiments using Buzzards Bay sediments in small tanks show that sulfate reduction is accompanied by the production of large pore water concentration gradients of alkalinity, phosphate, ammonia and dissolved organic carbon and the formation of subsurface maxima in Fe and Mn. These pore water profiles demonstrate that bacterially-mediated processes of organic matter degradation and redox reactions can be simulated in the laboratory.A vertical profile of 55Fe in pore waters is reported for the first time: it follows the profile of stable Fe and as such has a large (200 dpm/100 kg) subsurface maximum between 2–4 cm depth. Comparison of 55Fe/Fe ratios in sediments and pore waters shows that there is preferential solubilization of 55Fe over stable Fe.The pore water activities of 239,240Pu show no gradients within the large uncertainties of the counting statistics, but are two to four times higher than Buzzards Bay seawater (0.05 dpm/100 kg).The activity of 137Cs in the pore water profile is constant (40 dpm/100 kg) within the large counting uncertainties and is twice that of Buzzards Bay seawater. Cs-137 does not appear to be involved in diagenetic chemistry but may increase in pore waters as a result of ion exchange reactions.Flux estimates based on the pore water data show that remobilization and transport of 239,240 Pu in coastal sediments are not significant processes while the transport of l37Cs may be.  相似文献   

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