241Pu/239+240Pu ratios in polar glaciers

The analyses of plutonium isotopes in dated strata of polar ice sheets indicate that the²⁴¹Pu/^239+240Pu activity ratio produced in the U.S.-dominated nuclear tests during the 1950s was about 26, while that in the U.S.S.R.-dominated weapons tests in the early 1960s was between 12 and 14. This difference provides time horizons for sedimentary deposits. Further, the²³⁹Pu/²⁴⁰Pu ratio may show a similar difference in fallout values from these two periods of weapons testing and may provide an additional, and perhaps more sensitive, chronology for sediments.     

241Pu and241Am in sediments from coastal basins off California and Mexico

In sediments deposited in the coastal basins off the western North American continent since the early 1960's, there is more²⁴¹Am activity than one would predict if its presence was solely due to the decay of²⁴¹Pu that was produced during the testing of weapons in 1961–1962 (taken as July 1, 1962 for calculations). This excess can be accounted for by the decay of²⁴¹Pu, if pre-1962 fallout (fallout from the pre-moratorium testing) has been continuously introduced into the recent sediments along with fallout from post-moratorium testing. This hypothesis is supported by the plutonium depth profiles which do not reflect direct fallout from the atmosphere, as characterized by two peaks corresponding to the two major weapons testing periods, but continuously increasing plutonium and americium concentrations from 1954 to 1974. Thus, the nuclides may be coming from a large reservoir that has accumulated and mixed fallout since 1952. Such a concentration gradient for all of the nuclides requires their immobilization in the sediment after deposition.     

The coagulation of dissolved239, 240Pu in estuaries as determined from a mixing experiment

A mixing experiment, using large volumes (100 l) of filtered (< 1 μm) freshwater and seawater end-members, was performed to simulate and investigate the chemical reactivity of^{239, 240}Pu during estuarine mixing. An organic-rich freshwater with a relatively high concentration (0.8 dpm/100 l) of dissolved^{239, 240}Pu was used as one end-member; Buzzards Bay seawater (dissolved^{239, 240}Pu= 0.04dpm/100l) was the other. The results demonstrate that dissolved^{239, 240}Pu in the freshwater undergoes extensive and rapid coagulation under simulated estuarine conditions. There is a strong correlation between the amount of coagulation of dissolved^{239, 240}Pu, humic acids (HA), and Fe. The extent of coagulation of all three constituents increases with increasing salinity and the net extent of their removal is 53%, 57%, and 100% for Pu, HA, and Fe respectively. As has been documented for Fe in freshwater, dissolved^{239, 240}Pu appears to be stabilized by naturally occurring humic substances to form negatively charged colloids which are then coagulated by seawater cations. The extrapolation of these experimental results to real estuaries will require additional research.     

Transport and deposition of plutonium in the ocean: evidence from Gulf of Mexico sediments

A study of sediments in the Gulf of Mexico shows dramatic gradients in Pu content and isotope ratios from the continental shelf to the Sigsbee Abyssal Plain. In terms of predicted direct fallout inventory of Pu, one shelf core contains 745% of the predicted inventory, while abyssal plain sediments contain only 15–20% of the predicted value. Absolute Pu concentrations of shelf sediments are also conspicuously high, up to 110 dpm/kg, compared to 13.5 dpm/kg in Mississippi River suspended sediment. There is no evidence of Pu remobilization in Gulf of Mexico shelf sediments, based on comparison of Pu profiles with Mn/Al and Fe/Al profiles. Horizontal transport of fallout nuclides from the open ocean to removal sites in ocean margin sediments is concluded to be the source of both the high concentrations and high inventories of Pu reported here.The shelf sediments show²⁴⁰Pu/²³⁹Pu ratios close to 0.179, the average stratospheric fallout value, but the ratios decrease progressively across the Gulf to low values of 0.06 in abyssal plain sediments. The source of low-ratio Pu in deep-water sediments may be debris from low yield tests transported in the troposphere. Alternatively, it may represent a fraction of the Pu from global stratospheric fallout which has been separated in the water column from the remainder of the Pu in the ocean. In either case, the low-ratio material must have been removed rapidly to the sea floor where it composes a major fraction of the Pu in abyssal plain sediments. Pu delivered by global atmospheric fallout from the stratosphere has apparently remained for the most part in the water or has been transported horizontally and removed into shallow-water sediments.     

Radionuclide ratios in wet and dry deposition samples from June 1976 through December 1977

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.     

239+240Pu and 137Cs concentrations for zooplankton and nekton in the Northwest Pacific and Antarctic Oceans (1993-1996)

The concentrations of 239+240Pu and 137Cs in zooplankton and nekton in the Northwest Pacific and Southern Oceans were measured during the period 1993-1996. The object of the sampling was to assess the potential impacts of existing submerged anthropogenic-radioactive materials in the western North Pacific as well as the East China Sea. Samples from the Bransfield Strait of the Antarctic Ocean provided a control source impacted by only atmospheric bomb fallout. No particularly elevated levels of 239+240Pu were found in zooplankton samples from the Northwest Pacific, although significantly lower levels of 239+240Pu were found in three mixed zooplankton samples from the Bransfield Strait. The body burden of 239+240Pu in zooplankton appears to reflect concentrations in ambient seawater with some variation. Some additional measurements of 137Cs in fish are also reported here to complement existing databases and for future reference in the regional marine environmental radioactivity monitoring effort.     

Routes of plutonium uptake and their relation to biomagnification in starfish

The distribution of ^{239 + 240}Pu and ²³⁸Pu in environmental samples of starfish tissues is identical to the tissue distribution observed in experimental animals following uptake of plutonium directly from water. Plutonium in sea water has a strong affinity for the mucus-rich epidermal layer of starfish which contributes substantially to the relatively high levels of this transuranium nuclide measured in these invertebrates. Transfer of plutonium to starfish via food also occurs; however, the resultant tissue distribution is not consistent with that found in the natural environment where plutonium is available from both contaminated food and water. These data suggest that food chain biomagnification of plutonium by starfish does not occur in nature as has been previously hypothesized.     

Pu and137Cs in coastal sediments

Analyses are presented of¹³⁷Cs,²³⁸Pu, and^239,240Pu, in relation to depth in sediment, in 21 gravity cores. These cores span the ranges of times 1964–1975, and of water depths 12–2000 m; they come from three distinct sedimentation areas off the northeast coast of the United States. Although the ranges of total sediment inventories of^239,240Pu and of¹³⁷Cs from the various areas hardly overlap, the range of ratios of the inventories of these two nuclides is probably the same in all the areas. In the shallow-water cores the^239,240Pu/¹³⁷Cs ratio regularly diminishes with depth in the core, and a tendency is seen for curves of this function to have similar slopes in each area; ratios of²³⁸Pu/^239,240Pu show no change with depth in these shallow-water cores. In the deeper-water cores, the^239,240Pu/¹³⁷Cs ratio shows no systematic change with depth, but sometimes the²³⁸Pu/^239,240Pu ratio shows a minimum at the sediment surface, and is much higher deeper in the cores. We believe that these phenomena can be explained in terms of a complicated bioturbational process moving the nuclides, together, down into the sediments, of chemical resolubilization, at depth, of plutonium only, and of its subsequent upward translocation in the interstitial solution. Some re-immobilization of plutonium near the sediment surface is implied, and a mechanism is suggested for this, based on displacement of plutonium from organic complexes by the increasing concentrations, in upper layers of the sediment, of re-oxidized dissolved iron.     

Concentrations of 137Cs, 90Sr, 108m Ag, 239+240 Pu and atom ratio of 240Pu/239Pu in tanner crabs, Chionoecetes japonicus and Chionoecetes opilio collected around Japan

The anthropogenic radionuclides, ¹³⁷Cs, ⁹⁰Sr, ^108mAg, ^239+240Pu, were measured in two Chionoecetes species, red queen crab (Chionoecetes japonicus) and snow crab (Chionoecetes opilio) collected around Japan during 1996–2007. There was no increase in the concentrations of these radionuclides and no large variation of the atom ratio of ²⁴⁰Pu/²³⁹Pu during this research period. These results indicated that the source of the radionuclides was not the radioactive wastes dumped by the former USSR and Russia and originated from past nuclear weapon tests. The higher atom ratio in the crab species than that from global fallout would be contributed by the Pacific Proving Grounds close-in fallout. The variability of the concentration of radionuclides in the crab species would result from the variability of the composition and quantity in the diet. However, the decrease in the concentration of radionuclides with sampling depth would depend on the concentration in the seawater and diet.     

Atmospherically-derived radionuclides as tracers of sediment mixing and accumulation in near-shore marine and lake sediments: Evidence from7Be,210Pb,and239,240Pu

Cosmogenic⁷Be(t_1/2 = 53.3days) has been used to estimate particle-mixing rates in the upper layers of lacustrine and near-shore marine sediments. Excess²¹⁰Pb and/or^239,240Pu have provided limits on rates of sediment accumulation in these environments and indices of the efficiency of the sediments as collectors of reactive nuclides over longer time scale.In sediment cores from Long Island Sound (marine) and Lake Whitney (fresh-water)⁷Be was measurable in the top 2–3 cm. Diffusion-analog particle-mixing coefficients calculated from these data are in the range of 10^?7 cm²/s. For Long Island Sound the coefficients are lower by factors of 3–6 than those estimated from the depth distributions of excess²³⁴Th at the same stations [14]. For Lake Whitney the calculated mixing coefficient is an upper limit because of the possibility of a sampling artifact.Measurements of total (wet + dry) atmospheric deposition of⁷Be in New Haven give an average flux of 0.07 dpm/cm² day during March-November, 1977; this is equivalent to a steady-state inventory of 5.4 dpm/cm² in a perfect collector. Sediment cores from Long Island Sound contain about half this⁷Be inventory, consistent with either a mean residence time for⁷Be in the water column of about one half-life or with post-depositional loss of⁷Be from Long Island Sound sediments. The Lake Whitney cores contain about 5 dpm/cm², much nearer the atmospheric delivery. A higher inventory of⁷Be in fresh-water, as compared to marine, sediments could be due either to a shorter mean residence time for⁷Be in fresh water or to lateral transport processes in the lake or its catchment. High inventories of excess²¹⁰Pb and^239,240Pu in Lake Whitney sediments demonstrate the importance of lateral transport on longer time scales at least.     

Investigations of gram quantities of Atlantic and Pacific surface particulates

Particulates amounting to 0.1–2.0 g efficiently collected from large volumes of Atlantic and Pacific surface waters have been analyzed for carbonate, opal, quartz and several natural and man-made radioisotopes.The concentrations of particles range between 10 and 600 μg/kg. In the equatorial regions particle concentrations are low and similar in both the oceans. At higher latitudes (>30°N or S), the Atlantic waters, however, have higher concentrations of particles compared to those in the Pacific. The latitudinal distribution exhibits a north-south symmetry with higher concentrations in the 30°–60° belt. Based on the particulate abundance for CaCO₃ and opal and their sedimentation, we have estimated their production and in-situ integrated dissolution rates for a few regions.Radioisotopes having different source functions, namely¹⁴C and²³⁹Pu injected due to nuclear weapon tests,²³⁴Th,²³⁰Th and²²⁸Th produced in-situ in seawater,²³²Th which derives primarily from land,²¹⁰Pb introduced via wet precipitations and²²⁶Ra introduced through diffusion from deep-sea sediments have been measured in the particulates. The relative enrichment factors for these nuclides in particles vary as Th ? Pu > Pb > Ra. The atmospheric bomb fallout pattern is discernible in the surface particulates; the²³⁹Pu concentration increases with latitude in both the hemispheres; however, the values are about a factor of two lower in the southern hemisphere.The distribution pattern of radioisotopes is found to be complex, even for²³⁴Th whose source function in the oceans is uniform. In view of the differences in the source functions it becomes possible to delineate the principal geochemical/geophysical processes which determine the concentrations of these nuclides in surface waters.     

Sedimentary processes in the inner New York Bight: Evidence from excess210Pb and239,240Pu

Particle-reactive radionuclides were determined in sediments from the inner New York Bight to trace transport and storage of fine-grained sediments and associated reactive materials. Seven sediment ? cores 20–50 cm in length were analyzed for water content, loss on ignition (LOI) and excess²¹⁰Pb; three of these were also analyzed for^239,240Pu. Excepting some depth horizons in a core from a dredge-spoil dumpsite, every sample analyzed contained excess²¹⁰Pb. Variations in the concentration of excess²¹⁰Pb with depth in the sediment at all stations correlated strongly with LOI, which apparently traces that fraction of the sediment which is active in removing reactive elements from the water column. In the cores analyzed for^239,240Pu, every sample contained finite Pu, and Pu concentrations correlated strongly with excess²¹⁰Pb.The radionuclide distributions may be simply viewed as products of steady-state sediment accumulation or of mixing. Geochemically reasonable accumulation rates are very high (0.5–2.6 g/cm² y) and could probably only be sustained by offshore transport of dumped materials. At the other extreme the relationships between excess²¹⁰Pb and LOI are compatible with rapid mixing of a²¹⁰Pb carrier phase (traced by LOI) into the pre-existing substrate with little or no actual accumulation. Other non-steady-state processes, such as sediment gravity flow, could also explain the observed distributions.Measured sediment inventories (dpm/cm²) of excess²¹⁰Pb and Pu at these stations are greatly in excess of those supportable by direct atmospheric deposition: lateral supply is required. Incorporation of sedimentary fines into the sand substrate could make the inner New York Bight an important repository of reactive materials.     

Evidence for244Pu fission tracks in hibonites from Murchison carbonaceous chondrite

We have developed a technique for revealing nuclear tracks in the mineral hibonite (CaAl₁₂O₁₉), found in the refractory inclusions from carbonaceous chondrites. The tracks in hibonitesfrom Murchison carbonaous chondrite are dominated by fission tracks from²⁴⁴Pu (constituting more than 90% of the total). The measured uranium contents in these crystals range from 1.2 to 62 ppb. We deduce that the average value for the²⁴⁴Pu/²³⁸U ratio in most of the Murchison hibonites at the time of track retention is0.022 ± 0.011.     

Depositional history of artificial radionuclides in the Ross Ice Shelf,Antarctica

The annual fluxes of artificial radionuclides (²³⁸Pu,^239+240Pu,²⁴¹Am,¹³⁷Cs,⁹⁰Sr and³H) from the atmosphere to the Ross Ice Shelf in Antarctica were determined from measurements in strata dated by²¹⁰Pb. Recognizable sources include the U.S. tests (Mike-Ivy and Castle Hill) in the early 1950s, the U.S.S.R. tests of the early 1960s, the SNAP-9A burnup of 1964 and the French and Chinese tests in the late 1960s and 1970s. There are several problems still awaiting resolution: the differences in atmospheric chemistries of fission products and of transuranics produced in weapons tests and the anomalous fluxes of²³⁸Pu to the ice shelf which do not appear to reflect a one-year stratospheric residence. There is no evidence for a smearing of the fallout record as a consequence of diffusion of these radionuclides in the glacial column.     

The case for an unfractionated244Pu/238U ratio in high-temperature condensates

The coarse-grained, Ca-rich inclusions in the Allende meteorite are the highest-temperature condensates from the cooling solar nebula and, as such, the oldest solid objects in the solar system. All refractory elements with condensation points above the accretion temperature of the inclusions whose concentrations in them have been measured are seen to be present in the inclusions in unfractionated proportion to one another relative to C1 chondrites when data are averaged for a large number of inclusions. Observational data for U and theoretical data for both U and Pu suggest that these elements exhibited refractory behavior in the solar nebula. An experiment is proposed in which fissiogenic Xe and U contents are measured in a suite of these inclusions to obtain the²⁴⁴Pu/²³⁸U ratio of the solar system at the time of initial condensation with an uncertainty of ±15%.     

Spatial variability in sedimentation rates and artificial radionuclide storage in alluvial banks of the lower Rh?ne River

This paper analyzes the relationship between bank sediment storage and radionuclide content in six alluvial sites located in different geomorphic contexts along the lower Rh?ne River. The ¹³⁷Cs, ²³⁸Pu, ^239+240Pu, ²⁴¹Am and ²¹⁰Pb profiles show different patterns, which indicates a differential storage of contaminated sediment in the banks. Three sites record historical nuclear releases in the river and give evidence for long-term retention of particle-reactive long-lived radionuclides. Two sites record only atmospheric global fallout. Only one site, connected to the river groundwater, provides some evidence for desorption of particle-bound contaminants, with a low and constant ¹³⁷Cs activity profile. The history of the releases from the Marcoule spent-fuel reprocessing plant—the main source of artificial radioactivity—provides a reliable chronology of the last 50?years. Sediment grain size and bank topography are important factors in determining where artificial radionuclides are stored, but these two parameters cannot be used alone to determine variations in high concentrations of radionuclides. The chronology of fluvial geomorphic “metamorphosis” during the twentieth Century, especially after 1960, is also a critical factor affecting the spatial variability in sedimentation rates and artificial radionuclide storage; the timing of channel deepening and bank sedimentary accretion interfere with the chronology of major floods and the short period of low discharge during the height of contamination from nuclear liquid effluents. The reach-scale adjustment described in this paper can contribute to determining what the local history may have been. This result has important implications for river management decisions.     

Correlations between13C and ΣCO2 in surface waters and atmospheric CO2

¹³C and ΣCO₂ data from the North and South Atlantic, the Antarctic, and the North and South Pacific are given. The δ¹³C of the ΣCO₂ in the deep water (～3000m) decreases from 1.7‰ in the North Atlantic to ?0.10‰ in the North Pacific. This change is attributed to the addition of about 158 μmoles of CO₂ per kg of seawater. The in-situ oxidation of organic matter accounts for 83% of this increase in ΣCO₂, while the remainder is attributed to dissolution of calcium carbonate.The δ¹³C of the dissolved CO₂ in mid-latitude surface water samples is controlled by a quasi-steady-state equilibrium with atmospheric CO₂ at a mean temperature of 16°C. The δ¹³C and ΣCO₂ values of Antarctic surface water samples suggest that these waters are derived from a mixture of North Atlantic deep water and equilibrated surface water.     

Effects of biological sediment mixing on the210Pb chronology and trace metal distribution in a Long Island Sound sediment core

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, 240}Pu; 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, 240}Pu 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 of^{239, 240}Pu 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.     

Natural and anthropogenic radionuclide distributions in the northwest Atlantic Ocean

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 and^239,240Pu 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 (K_d) 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, theK_d 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.     

137Cs湖泊沉积年代学方法应用的局限——以Crawford湖为例

＾１３７Ｃｓ湖泊沉积年代学方法是测定现代湖泊沉积物沉积年代和沉积速率的重要同位素年代学方法之一。对加拿大Ｃｒａｗｆｏｒｄ湖采集的沉积孔柱内＾１３７Ｃｓ垂直分布的研究发现,该方法给出时的标有明显偏差。比较＾２１０Ｐｂ和纹层等年代方法的结果,其１９６３年时标蓄积峰值所在位置明显移向表层,而作为１９５４年时标的该核素出现蓄积的层位则远早于该年沉积物蓄积层位。研究还表明,孔柱中较高的间隙水含量、缺少足以吸