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1.
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   

2.
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   

3.
Particle mixing rates (DB) calculated from excess 210Pb gradients in sediments of the east equatorial Pacific range from 0.04 to 0.5 cm2/y, with variation of a factor of 3–4 at a single site. Diffusion of the 236Ra daughter 222Rn may affect 210Pb distributions under conditions of slow mixing and low 210Pb flux to the seafloor, as shown by a siliceous ooze-clay core which contained the fallout radionuclides 239,240Pu and 137Cs but no excess 210Pb (relative to 226Ra). There is no clear relationship between 210Pbderived mixing rates and sediment type, accumulation rate or organic carbon flux to the sediments. Comparison of 210Pb mixing rates with those calculated from 239,240Pu and 137Cs distributions reveals better agreement for a pulse input of the fallout radionuclides (DB = 0.03?0.4 cm2/y) than for continuous input at a constant rate (DB = 0.1?1.6 cm2/y), although the Pu and 137Cs data are better fit by the latter model. The agreement may be fortuitous because 239,240Pu and 137Cs appear significantly deeper than 210Pb in at least one core. Tracer separation could be caused by particle size-selective mixing by the benthic fauna or by chemical mobilization. If the fallout radionuclides are scavenged from surface waters by large, organic-rich particles such as fecal pellets, their release and migration may result from decomposition of the carrier in surface sediments. Either a relatively unreactive form of Pu (e.g. oxidized Pu) has been released by this process or a one-dimensional model is inadequate to explain its observed penetration into the sediments. Activity ratios of 239,240Pu137Cs in the sediments decrease with increasing north latitude, and the trend reflects higher fluxes of 239,240Pu near the weapons test site at Christmas Island (2°N). The 239,240Pu137Cs ratios and fluxes to the sediment (assuming constant input) at the siliceous ooze-red clay site are consistent with published sediment trap data from a nearby site. Thus if fallout radionuclide fluxes to the sea floor were higher in the past, both 239,240Pu and 137Cs have been released from sinking particles.  相似文献   

4.
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   

5.
6.
Laboratory extraction experiments and field observations were employed to determine the relative mobility of 239,240pu and 241Am from lake sediments under aerobic and anaerobic conditions. Laboratory investigations show that under aerobic conditions 241Am is more readily extracted from Lake Michigan sediments than is 239,240Pu. Under anaerobic conditions, the extractability of plutonium and americium does not increase significantly relative to aerobic conditions. Field studies indicate that neither element is recycled from the sediment to the overlying water column during anaerobic conditions attendant with thermal stratification. The adsorption of these elements onto sediments does not appear to be correlated with extractable iron, manganese, and organic compounds such as humic and fulvic acids.  相似文献   

7.
东北四海龙湾玛珥湖沉积物纹层计年与137Cs、210Pb测年   总被引:15,自引:6,他引:15       下载免费PDF全文
对东北四海龙湾玛珥湖SHLF6孔纹层沉积物的137Cs放射性测量表明:137Cs比活度的最大值出现在55cm处,对应于1963年世界原子弹试爆高峰期。纹层计年表明0~6cm共有35个纹层层偶。从75cm到65cm,137Cs比活度从256±009dpm/g急剧增加到1868±017dpm/g,可能65cm对应于1954年。通过测量226Ra子核214Pb和214Bi(能量为295keV,352keV和609keV)放射的光子数获得226Ra比活度数据,然后求得过剩210Pb比活度(210Pbuns)。210Pbuns比活度随深度增加而呈指数衰减,其异常波动可能与人类活动以及沉积速率变化有关,例如55cm处210Pb比活度较高,与137Cs的峰值对应,这可能与1963年前后人工核实验的高峰有关,因为核试验不仅产生137Cs,而且可以产生208Pb和210Pb;45cm处210Pb比活度较低,而226Ra较高,可能与人类活动加剧,导致沉积速率增加有关。根据210PbunsCRS模式,SHLF6孔0~19cm的平均沉积速率为20mg/cm2·a,或约为011cm/a。210Pb测年数据与137Cs时标及纹层计年均有很好的一致性。四海龙湾玛珥湖发育的纹层为年纹层,可以建立高分辨率时间序列。  相似文献   

8.
Nuclear facilities in coastal locations often discharge low‐level liquid wastes into the sea and the radioisotopes in these discharges are of interest both in assessing possible environmental impacts and as tracers for coastal processes. The distributions of a range of artificial radionuclides, derived from the authorized discharges from British Nuclear Fuels (BNFL) Sellafield, have been determined in the sediments of an intertidal salt marsh in the Esk Estuary, Cumbria, UK. Where published discharge histories exist (for 137Cs, 238Pu, 239,240Pu and 241Am), the sediment core‐profile distributions of these radionuclides have been compared with the releases from Sellafield, and consistent values of the accumulation rate (0·226 ± 0·007 g cm?2 yr?1) are obtained. A quantitative model has been developed, describing association of radionuclides with suspended particulate material, which is then accumulated and mixed in an offshore mud patch before resuspension and deposition in the salt marsh. The model has been used to describe radionuclide distributions observed in both the mud patch and the salt marsh, and to identify isotopes for which post‐depositional remobilization or solution transport from the discharge point are important. The behaviour of the commonly studied isotopes (137Cs, 238Pu, 239,240Pu and 241Am) is similar to that observed at this and other nearby locations. The activation product isotope 236U is enhanced in these sediments over the natural baseline by four to eight orders of magnitude, and the results suggest that Sellafield‐derived uranium is comparably mobile to 137Cs in these sediments although the processes governing the behaviour of these two elements may be different. In situ production of 241Am by decay of its 241Pu parent has generated only 17% of the current sediment inventory of this isotope, insufficient to account for the increase over the last 20–25 years, and suggesting that the input material for these sediments is preferentially enriched in Am relative to Pu during transport from the offshore mud patch. The discharge history of 244Cm, which is unknown, has also been reconstructed from the sediment profile and the model.  相似文献   

9.
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   

10.
Five sediment cores were collected on the shelf of the inner Mississippi Bight in June 2003 for a suite of radionuclides to establish geochronologies and trace elements to examine patterns of contaminant deposition and accumulation. Core sites were chosen to reflect a matrix of variable water depths, proximity to the Mississippi River mouth as the primary source for terrigenous particles, and extent and duration of summertime water column hypoxia. The vertical distribution of239,240Pu and210Pbxs(=210Pbtotal226Ra) provided reliable geochronological age constraints to develop models for mass accumulation rates and historic trace element inputs and variations. Mass accumulation rates ranged from 0.27 to 0.87 g cm−2yr−1 and were internally consistent using either210Pbxs or239,240Pu. Measured inventories of137Cs,239,240Pu, and210Pbxs were compared to atmospheric deposition rates to quantify potential sediment focusing or winnowing. Observed variability in calculated mass accumulation rates may be attributed foremost to site-specific proximity to the river mouth (i.e., sediment source), variability in water depth, and enhanced sediment focusing at the Mississippi River canyon site. Trace element concentrations were first normalized to Al, and then Al-normalized enrichment factors (ANEF) were calculated based on preanthropogenic and crustal trace element abundances. These ANEFs were typically >1 for V and Ba, while for most other elements studied, either no enrichment or depletion was observed. The enrichment of Ba may be related, in part, to the seasonal occurrence of oxygen-depleted subsurface waters off the Mississippi River delta, as well as being an ubiquitous byproduct of the petroleum industry.  相似文献   

11.
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   

12.
Vertical profiles of 137Cs and 239,240Pu were measured in soils collected from two sites in southern Sweden and three sites in southern Poland and were modeled using both a solute transport model and a bioturbation model to better understand their downward migration. A time series of measured 137Cs profiles indicates that 137Cs from Chernobyl was found at the soil surface in 1986 but it has migrated progressively downward into the soil 4.5-25.5 cm since. However, because of dispersion during the migration and mixing following Chernobyl deposition and the much higher activities of 137Cs from Chernobyl, stratospheric fallout of 137Cs from the 1960s cannot be identified as a second 137Cs activity maximum lower in the soil column at any of the sites. Conversely, the 240Pu/239Pu ratio indicates that no Chernobyl-derived Pu is present in any of the cores with the exception of one sample in Sweden. This difference may be attributed to the nature of the release from Chernobyl. Cesium volatilized at the reactor temperature during the accident, and was released as a vapor whereas Pu was not volatile and was only released in the form of minute fuel particles that traveled regionally. Both the solute diffusion and the bioturbation models accurately simulate the downward migration of the radionuclides at some sites but poorly describe the distributions at other sites. The distribution coefficients required by the solute transport model are about 100 times lower than reported values from the literature indicating that even though the solute transport model can simulate the profile shapes, transport as a solute is not the primary mechanism governing the downward migration of either Cs or Pu. The bioturbation model uses reported values from the literature of the distribution coefficients and can simulate the downward migration because that model buries the fallout by placing soil from depth on top and mixing it slightly throughout the mixing zone (0.6-2% per year of mixing). However, mixing in that model predicts concentrations in the top parts of the soil profiles which are too high in many cases. Future progress at understanding the downward migration of radionuclides and other tracers will require a more comprehensive approach, combining solute transport with bioturbation and including other important soil processes.  相似文献   

13.
14.
Surface sediments of the Washington coast have 210Pb activites which average 104 ± 48dpm/g for submarine canyon and slope regimes and 18 ± 12dpm/g for the continental shelf regime. 210Pb sedimentary fluxes are also higher in canyons, averaging 18 ± 13dpm/cm2 per yr, compared to 5.2 ± 3.1 dpm/cm2 per yr for slope and 4.8 ± 1.8dpm/cm2 per year for shelf regions. These 210Pb activities and fluxes are 2–7 times greater than those reported for other coastal regions. Inputs from the atmosphere and the Columbia River are not sufficient to supply the 210Pb, but advection of seawater containing dissolved 210Pb produced in situ from 226Ra provides an input several times larger than the sedimentary fluxes. The sedimentary 210Pb flux is limited by scavenging reactions rather than by supply of dissolved 210Pb.Calculations of maximum biological uptake and fluxes of 210Pb and ‘selective’ chemical leaching experiments all show that the primary scavenging processes are due to hydrous Mn and Fe oxides rather than biological phases. The pattern of higher 210Pb depositional fluxes in canyons than in nearby open slope areas of comparable water depth is most reasonably explained by enhanced scavenging of dissolved 210Pb near the sea floor, rather than by processes operating throughout the water column. Relatively rapid removal of dissolved 210Pb from the near bottom nepheloid layer to slope and canyon sediments is shown by its mean residence time of less than two years in this layer.  相似文献   

15.
The relative mobility of nuclides of Pb, Th, Pu, and Cs, which are widely used as geochemical tracers for sedimentation and bioturbation. was investigated in artificial microcosm tanks (MERL) and in Narragansett Bay. Their mobility was characterized by their removal rates from the water column, their affinity toward particles and their degree of penetration into the surface sediments. Pb, Th, and Pu transport was controlled predominantly by the affinity of these elements to particles, and the transport parameters of the particles themselves (i.e. sediment resuspension and mixing rates). Because of its low distribution coefficient, transport of Cs was controlled by molecular diffusion through pore water in the winter, while in summer, Cs transport was enhanced due to bioturbation. The increase with depth of the CsPu ratio in core profiles of MERL and Narragansett Bay sediments is thus caused primarily by the higher mobility of Cs.  相似文献   

16.
The radionuclide burden of vegetation comprising a tide-washed pasture at Ince Marsh in the Mersey Estuary, U.K., derives mainly from adhered external particulates originating as suspended sediments in estuarine water. Radionuclide concentrations are dominated by the growth cycle of the vegetation, with the highest winter levels of contamination activity an order of magnitude greater than the lowest levels in mid-summer. A secondary effect due to sediment transfer during periods of severe flooding produces subsidiary features on this dominant seasonal profile. Radionuclide concentrations on vegetation are in the range137Cs=8–191,134Cs=0.3–0.9,241Am=0.6–46,238Pu=0.1–1.5, and239/240Pu=0.8–44 Bq kg−1. These ranges reflect the relative concentrations of radionuclides in estuarine sediment (137Cs=615,241Am=202, and239/240Pu=104 Bq kg−1) rather than the values in filtered estuary water (137Cs=0.4,241Am=0.001, and239/240Pu=0.001 Bq 1−1). Median Kd values for these radionuclide species are Cs=1,400, Am=200,000, and Pu=80,000 1 kg−1).  相似文献   

17.
The diagenesis and geochemical evolution of deep-sea sediments are controlled by the interaction between sediments and their associated pore waters. With increasing depth, the pore water of Hole 149 (DSDP) exhibits a strong depletion in Mg and a corresponding enrichment in Ca, while the alkalinity remains relatively constant. Dissolved SiO2 is nearly constant in the upper 100 m of sediment, but is highly enriched in the deepest pore waters. The pore waters exhibit a depletion in K with increasing depth, and O18O16 pore water ratios also decrease.The sediment section has three zones of sedimentary regimes with increasing depth in the drill hole: an upper 100 m section of detrital clays, a middle section enriched in calc-akalic volcanics which have undergone submarine weathering to a smectite phase, and a lower section of siliceous ooze which still has a diagenetic smectite phase. The quartz-feldspar ratios and O18O16 composition of the silicate phases are in agreement with these interpretations.The submarine weathering of volcanics to a smectite can account for the observed pore water gradients. Volcanics release Ca and Mg to the pore waters causing the alkalinity values to increase. Smectite is formed, depletes the pore waters in Mg and O18 and causes the alkalinity to decrease. The net reaction allows for the observed relationship between pore water Ca and Mg gradients with little net change in alkalinity. Given the abundance of volcanics in many deep-sea sediments, especially in lower sections which often form near ridge crests, the submarine formation of smectite may be an additional oceanic Mg sink which has not yet been fully considered.  相似文献   

18.
The annual balance of radionuclides inflow/outflow was assessed for 137Cs and 90Sr isotopes in the Barents Sea, taking into account the atmospheric precipitation, inflow from the Norwegian and the White seas, as well as riverine discharge, liquid radioactive waste disposal (LRWD), and outflow to the adjacent seas. The original and published data for the period of 1950–2009 were analyzed. According to the multiyear dynamics (1960–2009), the inflow of 137Cs and 90Sr into the Barents Sea was significantly preconditioned by the Norwegian Sea currents; and precipitation played a major role in the 1950s, 1960s, and in 1986. Currently, the trans-border redeposition of 90Sr prevails over 137Cs redeposition in the Barents Sea, and constitutes about 99% of inflow of each element.  相似文献   

19.
Matishov  G. G.  Matishov  D. G.  Solatie  D.  Kasatkina  N. E.  Leppanen  A. 《Doklady Earth Sciences》2009,427(2):1006-1011
The results of radioecological investigations carried out within the framework of the Russian-Finnish high-latitude expedition in 2007 are presented. The characteristics of the present-day accumulation level of the significant radioecological isotopes 137Cs, 90Sr and 239,240Pu in the Barents Sea are described. The comparative analysis is performed for the radiation pollution of the environment in the 1980s and 1990s and in the first decade of the 21st century. Natural purification processes in the marine environment are the main factors of the decrease in the intensity level of artificial radioactive isotopes. These processes include repeated dilution, nuclear decay, occlusion by sediments and suspended solid material, and accumulation by aquatic inhabitants. A stable decreasing trend is observed for the intensity level of artificial radioactive isotopes in the Barents Sea.  相似文献   

20.
Vertical profiles of137Cs and210Pb have been determined in a 9 m column of ice from accumulation zone of Changme-Khangpu glacier in north Sikkim valley.137Cs activity varies from 4 to 22 dpm/ L. In many samples210Pb occurs at a level of 20 to 65 dpm/ L which is much higher than the expected fallout value.137Cs and210Pb activities correlate well with each other but not with the dust content. Possibility of210Pb production in the nuclear explosions is discussed. Several peaks appear in the depth profile of137Cs and210Pb which can be matched with Chinese atmospheric nuclear explosions with some phase difference if a uniform ice accumulation rate of 0.7 m per year is assumed since 1969.  相似文献   

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