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1.
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2.
We have used in-situ pumps which filter large volumes of sea water through a 1 μm cartridge prefilter and two MnO2-coated cartridges to obtain information on dissolved and particulate radionuclide distributions in the oceans. Two sites in the northwest Atlantic show subsurface maxima of the fallout radionuclides137Cs,239,240Pu and241Am. Although the processes of scavenging onto sinking particles and release at depth may contribute to the tracer distributions, comparison of predicted and measured water column inventories suggests that at least 35–50% of the Pu and241Am are supplied to the deep water by advection.The depth distributions of the naturally occurring radionuclides232Th,228Th and230Th reflect their sources to the oceans.232Th shows high dissolved concentrations in surface waters, presumably as a result of atmospheric or riverine supply. Activities of232Th decrease with depth to values 0.01 dpm/1000 l.228Th shows high activities in near surface and near bottom water, due to the distribution of its parent,228Ra. Dissolved230Th, produced throughout the water column from234U decay, increases with depth to 3000 m. Values in the deep water (> 3000 m) are nearly constant ( 0.6–0.7 dpm/1000 l), and the distribution of this tracer (and perhaps other long-lived particle-reactive tracers as well) may be affected by the advection inferred from Pu and241Am data.The ratio of particulate to dissolved activity for both230Th and228Th is 0.15–0.20. This similarity precludes the calculation of sorption rate constants using a simple model of reversible sorption equilibrium. Moreover, in mid-depths228Th tends to have a higher particulate/dissolved ratio than230Th, suggesting uptake and release of230Th and228Th by different processes. This could occur if228Th, produced in surface water, were incorporated into biogenic particles formed there and released as those particles dissolved or decomposed during sinking.230Th, produced throughout the water column, may more closely approach a sorption equilibrium at all depths.230Th,241Am and239,240Pu are partitioned onto particles in the sequence Th > Am > Pu with 15% of the230Th on particles compared with 7% for Am and 1% for Pu. Distribution coefficients (Kd) are 1.3–1.6 × 107 for Th, 5–6 × 106 for Am and 7–10 × 105 for Pu. The lower reactivity for Pu is consistent with analyses of Pu oxidation states which show 85% oxidized (V + VI) Pu. However, theKd value for Pu may be an upper limit because Pu, like228Th, may be incorporated into particles in surface waters and released at depth only by destruction of the carrier phase.  相似文献   

3.
The distribution of “ash” (the non-combustible fraction of marine suspended matter) and concentrations of particulate Al, Ca, Fe, Cr, Ni, Cu, Sr and234Th in surface waters and of210Pb,230Th and234Th in two vertical profiles (385–4400 m) of the Indian Ocean are reported.The ash concentrations in surface waters follow the primary productivity pattern, with higher abundances in samples south of 40°S and lower concentrations in the equatorial and subtropical regions. Opaline silica and CaCO3 are the dominant components of the ash in samples from >40°S and from 7°N to 39°S, respectively. Aluminosilicates are only a minor constituent of the surface particulate matter. The metal/Al ratios in the surface particles are significantly higher compared to their corresponding crustal ratios for all the metals analyzed in this work. Comparison of enrichment factors between marine aerosols, plankton and surface oceanic particles, seem to indicate that this high metal/Al ratio in surface particles most likely arises from their involvement in marine biogeochemical cycles. Particulate234Th activity in surface waters parallels the ash abundance implying that its scavenging efficiency from surface waters depends on the particulate concentration.The particulate230Th and210Pb concentration profiles increase monotonously with depth. It is difficult to ascribe this increase to a process other than the in-situ vertical scavenging of230Th and210Pb from the water column by settling particles. The mean settling velocities of particles calculated from the particulate230Th data using a one-dimensional settling model is about 2 × 10?3 cm/s. The settling velocity computed from the particulate230Th profiles does not appear to be compatible with the particulate210Pb depth profiles; one possible explanation to account for the disparity would be that230Th and210Pb are scavenged by different size populations of particles.On the whole, the geographic distribution of particulate matter, their composition and settling velocities in the Atlantic, Pacific and Indian Oceans are similar indicating that they are controlled by quite similar processes in the marine hydrosphere.  相似文献   

4.
The concentrations of214Pb (half-life=26.4minutes) and22Rn (half-life=3.84days) have been measured in deep groundwaters of Gujarat, India. The results show that the abundance of214Pb in the water is only ～25% of that expected from its production through the radioactive decay of dissolved222Rn. This deficiency if modelled in terms of a first-order removal, yields a residence time of ～10 minutes for214Pb in these waters. The estimated residence time for214Pb is the shortest observed for any nuclide in natural water systems and suggests that reactive nuclides lead like could be removed from aqueous phases to adjoining solid surfaces on extremely short time scales. Results of laboratory experiments using the212Pb-224Ra pair are compatible with the observed fast removal of214Pb from groundwaters.Re-evaluation of234Th residence times in these waters using a model with a recoil flux of234Th into aqueous phase, the same as that of222Rn, yields values in the range of 23 to<176 minutes, very similar to that of214Pb. This “concordancy” in the residence times seems to suggest that the geochemical behaviour of234Th and214Pb in these waters is quite similar.  相似文献   

5.
The concentrations of radionuclides of the U-Th series (238U,234Th,234U,230Th,226Ra,210Pb,210Po, and232Th,228Ra,228Th) in the water of Narragansett Bay are reported. Analysis of the total, particulate, dissolved and colloidal forms of Th isotopes reveal a consistent removal behavior which is controlled mainly by the particulate matter concentration and the sediment resuspension rate. Half-removal times of Th from solution onto particles range from 1.5 to 15 days, and settling velocities of Th containing particles range generally between 1 and 11 m/day.210Pb and210Po concentrations are seasonally dependent, with higher concentrations and slower removal during the early summer (half-removal times from solution onto particles of 1–5 days in winter and up to 2 months in early summer).  相似文献   

6.
Four vertical profiles of230Th and228Th were determined using large volume water samples in the western North Pacific. An almost linear increase of230Th with depth was observed for all of the profiles for which the unidirectional first order scavenging model was difficult to explain. We developed a model which included a dissolved-particulate transformation as well as parameters of the scavenging model. Application of the model to the vertical distributions of total and the GEOSECS particulate Th isotopes (230Th and234Th) yielded the residence time of dissolved Th with respect to adsorption to particles and the turnover time of particulate Th to be 235 days and 57 days, respectively. The Th isotopes appeared to be carried down the water column by fine particles with a mean settling velocity of 1 m/day which continually release Th into sea water as well as pick up Th from the water along their journey to the bottom.For228Th, a large excess over232Th was observed throughout the water column with pronounced high concentrations in surface and bottom waters, suggesting that the228Th was derived from228Ra diffused out of sediments. The vertical distributions of228Th seemed to be significantly influenced by lateral mixing along isopycnals.  相似文献   

7.
An experiment was designed to assess the relative importance of sediment accumulation and bioturbation in determining the vertical distribution of nuclides in estuarine sediments. A diver-collected core, 120 cm long, was raised from central Long Island Sound and analyzed down its length for:210Pb and226Ra;239, 240Pu; and Mn, Zn, Cu, and Pb. Sampling for chemical analysis was guided by X-radiography of the core. Excess210Pb (relative to226Ra) is roughly homogeneous in the top 2–4 cm of the core, then decreases quasi-exponentially to zero at (or above) 15 cm.239, 240Pu and excess Zn, Cu, and Pb, relative to background values at greater depths in the core, are distributed like excess210Pb in the top 10–15 cm. The absence of Mn enrichment at the top of the core, in contrast to other cores raised from this station, suggests that 1–3 cm of sediment was lost by erosion at the site of this core sometime prior to sampling. Below 15 cm excess210Pb and excess Zn, Cu, and Pb are found only in the bulk sample from 25 to 30 cm and in clearly identifiable burrow fillings dissected from 70 cm and 115 cm depth. Infilling of large burrows, excavated and then abandoned by crustaceans, is therefore a mechanism for transfer of surficial material to depth in these sediments.The bioturbation rate in the top several centimeters at this station has been determined previously using234Th (24-day half-life). The distribution of239, 240Pu can be used to estimate a bioturbation rate for the underlying layer (to ～10 cm depth); this rate is found to be 1–3% of the maximum mixing rate for the top 2–3 cm. Using these two mixing rates in a composite-layer, mixing + sedimentation model, the distribution of excess210Pb in the top 15 cm was used to constrain the sediment accumulation rate, ω. While the apparent rate of sediment accumulation (assuming no mixing below 2–4 cm) is 0.11 cm/yr, the model requires ω < 0.05 cm/yr. Thus in an area of slow sediment accumulation, a low rate of bioturbation below the surficial zone of rapid mixing causes an increase of at least a factor of two in apparent accumulation rate.  相似文献   

8.
Anthropogenic radionuclides have reached the Hudson estuary as global fallout from nuclear weapons testing and through local releases from commercial nuclear reactors. Significant activities of238Pu and239,240Pu (fallout-derived),134Cs and60Co (reactor-released), and137Cs (derived from both sources), have accumulated in the sediments throughout the estuary, with the primary zone of accumulation near the downstream end of the system in New York harbor. The estuary appears to have trapped nearly all of the239,240Pu delivered as fallout, and consequently, ocean dumping of dredged harbor sediment is currently the primary means for the net transport of these nuclides to coastal waters. In contrast, only 10–30% of the137Cs,134Cs and60Co delivered to the estuary have been retained on the fine particles which accumulate at a rapid rate in the harbor.The primary factors which have governed the distribution of anthropogenic radionuclides in Hudson sediments are: (1) spread of fine particles labeled with both fallout and reactor nuclides throughout the axis of the estuary, (2) differences in timing of the peak fallout years (1962–1964) and years of maximum reactor releases (1971–1972), (3) large variations in sediment accumulation rates, ranging from a few millimeters per year or less to many tens of centimeters per year, (4) appreciable desorption of137Cs and134Cs from particles at higher salinities, and (5) possible enhanced desorption of60Co at higher salinities (relative to134Cs and137Cs) which may be associated with the release of reduced manganese from the harbor sediments.  相似文献   

9.
The mean residence time (τ) of thorium with respect to non-radioactive removal from water was determined as a function of location in three traverses of the New York Bight using both234Th/238U and228Th/228Ra. τ correlates well with salinity increasing from about ten days near shore to 70 days at the shelf break. It shows a much weaker correlation with suspended matter concentrations both because suspended matter varies in its scavenging efficiency and because salinity is a longer-term integrator of scavenging potential.τ's computed from228Th/228Ra were often higher than those computed from234Th/238U either because of the detrital matter present as reflected in the232Th concentrations or because the water parcels had recently arrived from environments of lower scavenging efficiency.Anomalous isotopic concentrations found in three adjacent samples can best be explained as the result of an episodic release of228Ra from bottom sediments at a rate 200 times the normal one.  相似文献   

10.
The thorium isotope content of ocean water   总被引：1，自引：0，他引：1  
232Th concentrations of surface and deep Pacific Ocean waters are 0.01–0.02 dpm/1000 kg (60 pgm/kg). The230Th activity is 0.03–0.13 dpm/1000 kg in surface waters and 0.3–2.7 dpm/1000 kg in deep waters. Chemical residence times based on in situ production from parent isotopes are about the same for230Th and228Th in surface waters (1–5 years) but are ten times greater for230Th in deep waters (10–100 years). Apparently there are additional sources of230Th into deep waters. At MANOP site S manganese nodule tops are enriched in Th isotopes by adsorption of Th from seawater and not by incorporation of Th-rich particulates.  相似文献   

11.
The first224Ra (t1/2 = 3.64days) measurements from mixing zones of estuarine systems are presented for the Pee Dee River-Winyah Bay and Delaware Bay Estuaries. High-resolution gamma-ray spectrometry was used to determine224Ra,228Ra (t1/2 = 5.7years), and226Ra (t1/2 = 1622years) activity ratios. Desorption and diffusion from suspended and bottom sediments contributes to the non-conservative increases of the three isotopes in each systems. In Delaware Bay224Ra concentrations were nearly constant over the 2.5‰ to 15‰ salinity range where two turbidity maximum zones are located.228Th scavenging onto the suspended particles in the turbid zones may supply a regenerative source of224Ra in this system. Samples collected on the ebb and flood tide from a salt marsh along Delaware Bay have a 5-fold increase in224Ra from flood to ebb and 3- and 2-fold increases for228Ra and226Ra respectively, indicating salt marshes are another source of radium to estuarine waters.  相似文献   

12.
Unsupported226Ra (t12 = 1620years) in marine sediments can provide a basis for measuring rates of accumulation of the order of centimeters per thousand years. The excess radium apparently enters the sediments incorporated in phytoplankton. The sensitivity of the method depends upon the initial value of the unsupported226Ra and of the value of230Th, a parent of226Ra, in the sedimentary components.226Ra dating was applied to a sediment taken from the slope of the San Clemente Basin in the Southern California coastal region. Rates of sedimentation over two half-lives of the nuclide were found to be either 5.2 or 5.3 cm/1000 years depending upon which of two models for the geochronology is used. One model assumes that the230Th brings to the deposit an amount of226Ra in equilibrium with it. The other is based upon the growth of the226Ra from the230Th in the sedimentary components.238+239Pu and210Pb levels in the upper strata indicated sedimentation rates of the order of 100–500 cm/1000 years, i.e. much faster accumulations. We suggest these derived rates are spurious and reflect bioturbative activities of surface-living organisms.  相似文献   

13.
Hydrothermal waters collected by “Alvin” from the Galapagos Spreading Center are enriched in222Rn by factors of 50–200 over bottom waters. The226Ra in the same samples, however, is enriched by less than a factor of four over bottom waters. Enrichments of222Rn result primarily from α-recoil from rock surfaces while226Ra enrichments are dominantly produced by high-temperature alteration of cooling ridge volcanics. The abundances of both nuclides exhibit positive correlations with temperature. The data extrapolate to bottom water temperatures and compositions, demonstrating the importance of seawater mixing. Different vents, however, have different mixing lines, and vents with high222Rn have low226Ra. We propose these patterns result from variations in the extent of low-temperature crustal interaction with the hydrothermal fluids. Low-temperature crustal waters can maintain high steady state222Rn contents due to the α-recoil additions to the fluids. The226Ra, however, is strongly adsorbed at low-temperatures resulting in low concentrations of this nuclide in low-temperature crustal waters. Thus, physical mixing of a crustal water component with hydrothermal waters or variable crustal path lengths of the hydrothermal fluids can account for the variable mixing lines and222Rn/226Ra values of the hot springs.The222Rn/226Ra value appears to be a sensitive indicator of low-temperature crustal interaction. Values > 100 have experienced extensive crustal interaction and are indicative of diffuse hydrothermal flow. Values between 1 and 10 are indicative of primary hydrothermal fluids which have not experienced significant interaction with the crust. Values of222Rn/226Ra between 103 and 104 are indicative of interaction of the hydrothermal fluids with sediments. Such values are observed in water samples from the Galapagos hydrothermal mounds.  相似文献   

14.
The234Th/238U activity ratios in the near-bottom waters at a station in the South Pacific have been measured. The activity ratios are close to the secular equilibrium value, ranging between 0.9 and 1.13 (± 8%), suggesting that the rate of removal of234Th by bottom-water scavenging processes at this station is slow compared to its rate of radioactive decay. The mean234U/238U activity ratios in these waters is 1.14 ± 0.02, the same as the reported values for the world oceans.  相似文献   

15.
A fiber extraction technique is used to concentrate Ra and Th isotopes from 1000 liters or more of seawater. Natural226Ra and234Th are used as yield tracers. In the equatorial Pacific the228Ra activity of surface water varies from 20 to 1 dpm/1000 kg and generally decreases away from continental shelf areas. Across the Peru Current System, this decrease is modeled as one-dimensional diffusion and indicates the possibility of two flow regimes with distinct characteristic mixing lengths and apparent eddy diffusivities of 105 and 107 cm2/s. The perturbing effects of advection and equatorial upwelling west of the Galapagos Islands are noted. Off the coast of Southern California a vertical228Ra distribution gives an apparent diffusivity of 1.6 cm2/s for the upper thermocline.226Ra concentrations near the coast appear to be higher than the open ocean values at comparable depths, which may reflect supply of this isotope from continental shelf sediments and/or upwelling. The insoluble daughter/soluble parent activity ratios228Th/228Ra and234Th/238U in the equatorial Pacific surface water display latitudinal trends which may be correlated with productivity variations. Near the coast of California these ratios reflect the differing oceanographic conditions north and south of Pt. Conception indicating a mean chemical removal time constant on the order of 4 months for Th and other highly reactive elements within the Southern California Bight. The232Th content of seawater sampled is less than 0.1 μg/1000 1; most of the published values for seawater232Th could well be too high. A comparison of the two methods of determining228Ra (via228Ac and via228Th) made on 64 seawater samples shows that the time delay required by the228Th method is more than compensated by its better analytical simplicity and precision.  相似文献   

16.
Two expeditions (October 1989 and May 1992) were carried out to two points of the main Amazon River channel and four tributaries. The Solimões and Madeira rivers, taking their origin in the Andes, are whitewater rivers. The Negro River is a typical acid, blackwater river. The Trombetas River flows through bauxite‐rich areas, and is characterized by low concentrations of dissolved humic substances. The 238U, 234U, 232Th and 230Th activities were recorded from dissolved, suspended particulate phases and river bank sediments. The latter were analysed for their 226Ra, 228Ra and 210Pb contents, and also subjected to leaching with 0·2 M hydroxylamine–hydrochloride solution to determine the concentrations of radionuclides bound to amorphous Fe hydroxides and Mn oxides and hydroxides. The dissolved U average concentration in the Amazon system is ten times lower than the mean world river concentration. The uranium concentration observed at Óbidos in the lower Amazon (0·095 µg L?1), where the U content in the river bank sediments and suspended matter is lowest, suggests U release from the solid phase during river transport. About 485 t of U are transported annually to the Amazon delta area in dissolved form, and 1943 t bound to suspended particulate matter. Total U and Th concentrations in the river bank sediments ranged from 1·59 to 7·14 µg g?1 and from 6·74 to 32 µg g?1, respectively. The highest concentrations were observed in the Trombetas River. The proportion extracted by means of the hydroxylamine solution (HL) was relatively high for U in the Trombetas river bank sediment (31%) and for Th in the Solimões sediment (30%). According to the alpha recoil effects, the 234U/238U activity ratios of the Andean river waters and downstream Amazon water (Óbidos) were >1, but were <1 in the Negro River (at Manaus). The activity ratios of dissolved U correlate with pH and also with the U activity ratios in the river bank sediment hydroxylamine extracts. As expected, the 234U/238U activity ratios in river bank sediments were <1 in the Andean rivers and in the downstream Amazon, but they were >1 in the Trombetas and Negro rivers. Such ratios probably result from the binding of dissolved uranium to solid sediment. The 228Th/232Th ratios of river bank sediments were close to unity (except for the Negro River, where it is lower), suggesting no significant Th exchanges between the river water and the sediment. The 226Ra/232Th activity ratios were <1, and the 226Ra/228Ra activity ratios generally were significantly higher than the activity ratios of their respective parents. This perhaps is the result of easier leaching of the 226Ra parent, 230Th, from solid material (owing to the alpha recoil effect) than of the 228Ra parent. Uranium and thorium isotopes were used as tools to evaluate the chemical weathering rate of rocks in the Amazon system, which was estimated to be 2·7 cm 1000 year?1 s?1. Copyright © 2002 John Wiley & Sons, Ltd.  相似文献   

17.
238Pu,239Pu and137Cs in rain and dry fallout and90Sr in rain samples were measured at Woods Hole, Massachusetts, from June 1976 through December 1977. The dry fallout was estimated to be about 7.8% of the total deposition of239Pu and137Cs.239Pu/137Cs ratios, almost constant at about 0.011 in rain or dry fallout, February through December 1977, suggested that fractionation between the refractory and volatile radionuclides is insignificant in stratospheric fallout. This supports the idea of regional homogeneity of radionuclide ratios in fallout.  相似文献   

18.
The228Ra concentrations of the Dead Sea waters range from 0.13 to 1.48 dpm kg−1, two to three orders of magnitude higher than those of ocean waters and lake waters. However, the228Ra/226Ra activity ratios, (0.12–1.29) × 10−2, are in the range reported for the hydrosphere.The surface waters of the Dead Sea are enriched in228Ra by a factor of about three over the near-bottom waters. There is a factor of about two spatial variability in the mid-depth Ra concentrations at the two profile stations. The near-bottom228Ra gradients yield vertical eddy diffusivity coefficient (K) of 2.0 and 0.4 cm2 s−1 at profile locations 1 and 2 respectively. These values are comparable to those measured in oceans and lakes.  相似文献   

19.
In Funka Bay of Hokkaido, Japan, seawater, suspended matter and settling matter were collected once every month in the summer of 1974. These samples were analyzed for234Th, a short-lived daughter of dissolved238U. A pronounced disequilibrium between234Th and238U, and a highly variable concentration of234Th were found. Positive correlation, however, exist among the deficiency of234Th relative to238U in seawater, the concentration of particulate234Th, the fraction of particulate234Th to total234Th in seawater, the total dry weight of suspended matter, and the primary productivity during the month previous to sampling. The specific activity of234Th for the settling particles (620 ± 170 dpm/g) was nearly equal to that for suspended particles (720 ± 600 dpm/g) but much greater than that for plankton (47 ± 24 dpm/g). These facts suggest that suspended particles are somehow closely related to the removal of heavy metals from seawater, in spite of the negligibly small settling flux of suspended matter. The residence time of thorium in Funka Bay (mean depth: 60 m) is found to be about 60 days, which is nearly equal to those of210Pb and210Po.  相似文献   

20.
Strong isotopic fractionation between234U and238U has been noted in deep oil-well brines. The waters are stratigraphically and structurally isolated from fresh-water inflow and have remained stagnant for more than five half-lifes of234U. Excess234U is explained by the234Th alpha-recoil nucleus event.  相似文献   

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