Trace metals and radionuclides reveal sediment sources and accumulation rates in Jordan Cove, Connecticut

Many small estuaries are influenced by flow restrictions resulting from transportation rights-of-way and other causes. The biogeochemical functioning and history of such systems can be evaluated through study of their sediments. Ten long and six short cores were collected from the length of Jordan Cove, Connecticut, a Long Island Sound subestuary, and analyzed for stratigraphy, radionuclides (¹⁴C, ²¹⁰Pb, ²²⁶Ra, ¹³⁷Cs, and ⁶⁰Co), and metals (Ag, Cd, Cu, Pb, Zn, Fe, and Al). For at least 3,800 yr, rising sea level has gradually inundated Jordan Cove, filling it with mud similar to that currently being deposited there. Long-term sediment accumulation in the cove averaged close to 0.1 cm yr⁻¹ over the last three millennia. Recent sediment accumulation rates decrease inland from 0.84 cm yr⁻¹ to 0.40 cm yr⁻¹, and are slightly faster than relative sea-level rise at this site (0.3 cm yr⁻¹). Similarity of depth distributions of trace metals was used to confirm relative sediment accumulation rates. ⁶⁰Co and Ag are derived from sources outside the cove and its watershed, presumably the Millstone nuclear power plant and regional contaminated sediments, respectively. The combined data suggest that Long Island Sound is an important source of sediment to the cove; a minor part of total sediment is supplied from the local watershed. Trace metal levels are strongly correlated with Fe but not with either organic matter or Al. Sediment quality has declined in the cove over the past 60 yr, but only slightly. Cu, Pb, and Zn data correlate strongly with Fe but not with either organic matter or aluminum. Ratios of Ag to Fe and to trace metals suggest that Ag in the cove is derived almost entirely from Long Island Sound. This result supports the notion that Fenormalized Ag can serve as a better tracer of some kinds of contamination than more common and abundant metals, like Cu, Pb, and Zn. *** DIRECT SUPPORT *** A01BY085 00008     

The relationship of soil 210Po and 210Pb geochemical dispersion patterns to uranium mineralization

²¹⁰Po and ²¹⁰Pb measurements of soils delineated uranium anomalies at three out of four test sites in Ontario, Canada. Measurements were made of ²¹⁰Po in solutions produced by both complete digestion and partial leaching of soil samples. Direct plating of ²¹⁰Po onto metal plates was followed by measuring the alpha activity. Subsequent plating of ²¹⁰Po in-grown from ²¹⁰Pb in solution several months later confirmed the anomalies.The ²¹⁰Po and ²¹⁰Pb anomalies at three of the test sites coincided with ²²⁶Ra and ²²²Rn anomalies. Samples from the fourth uranium occurrence associated with a known ²²²Rn anomaly failed to show either a ²²⁶Ra anomaly on the one hand, or ²¹⁰Po or ²¹⁰Pb anomalies on the other. This suggests that the ²¹⁰Po and ²¹⁰Pb anomalies were probably produced by the decay of ²²⁶Ra contained within secondary dispersion haloes.Although anomalies due to the ²¹⁰Po and ²¹⁰Pb products of ²²²Rn have now been documented, prospecting methods based on their use as direct tracers of the migration paths of ²²²Rn require much further development.     

The relationship of soil Po and Pb geochemical dispersion patterns to uranium mineralization

²¹⁰Po and ²¹⁰Pb measurements of soils delineated uranium anomalies at three out of four test sites in Ontario, Canada. Measurements were made of ²¹⁰Po in solutions produced by both complete digestion and partial leaching of soil samples. Direct plating of ²¹⁰Po onto metal plates was followed by measuring the alpha activity. Subsequent plating of ²¹⁰Po in-grown from ²¹⁰Pb in solution several months later confirmed the anomalies.The ²¹⁰Po and ²¹⁰Pb anomalies at three of the test sites coincided with ²²⁶Ra and ²²²Rn anomalies. Samples from the fourth uranium occurrence associated with a known ²²²Rn anomaly failed to show either a ²²⁶Ra anomaly on the one hand, or ²¹⁰Po or ²¹⁰Pb anomalies on the other. This suggests that the ²¹⁰Po and ²¹⁰Pb anomalies were probably produced by the decay of ²²⁶Ra contained within secondary dispersion haloes.Although anomalies due to the ²¹⁰Po and ²¹⁰Pb products of ²²²Rn have now been documented, prospecting methods based on their use as direct tracers of the migration paths of ²²²Rn require much further development.     

Mixing and cycling of uranium,thorium and 210Pb in Puget Sound sediments

Activity profiles of excess ²³⁴Th, excess ²¹⁰Pb, ²³²Th, ²³⁰Th, ²³⁴U and ²³⁸U, and ^228/232Th ratios determined in eight box cores of sediment from six sites in central Puget Sound provide new insights into the dynamic nature of solid phase mixing in surface sediments, the exchange of ²²⁸Ra and other soluble species across the sediment-water interface, and the cycling of U, Th and ²¹⁰Pb in this coastal zone.Comparison of excess ²³⁴Th inventories in sediments with its production rate in the overlying water column indicates a mean residence time of at most 14 days for particles in the central Puget Sound water column.Surface sediment horizons with excess ²³⁴Th have no excess ²²⁸Th which might be used to ascertain sediment accumulation rates over the past decade. Instead, deficiencies of ²²⁸Th due to loss of soluble ²²⁸Ra from pore water to the overlying water persist to 20–30 cm, revealing that exchange of soluble chemicals between pore and overlying waters reaches these depths in the extensively bioturbated sediments of Puget Sound.Solid phase U isotope concentrations tend to increase by up to a factor of two with depth in sediments, as a result of dissolved U being biologically pumped down into sediments where it is partially removed when conditions become mildly reducing. ²³²Th and ²³⁰Th activities and ^230/232Th ratios are constant with depth in sediments, indicating constant detrital phase compositions and essentially no authigenic ²³⁰Th. Steady state ²¹⁰Pb depositional activities in and fluxes to Puget Sound sediments average only about onehalf those for sediments of the open Washington coast north of the Columbia River mouth, primarily because of a much lower supply of dissolved ²¹⁰Pb in sea waters adverting into Puget Sound.Excess ²³⁴Th profiles in sediments reveal much more detail about the depth dependency, dynamic nature and recent history of solid phase mixing processes than excess ²¹⁰Pb profiles. At least six of eight ²³⁴Th profiles show that mixing within the ²¹⁰Pb-defined surface mixed layer is depth dependent. In three profiles, ²³⁴Th-derived mixing rates are fastest several centimeters below the sediment-water interface, indicating greater macro-benthic activity at these depths. Depth dependent mixing coefficients derived from the best fit of a four layer, advection-diffusion-decay model to the ²³⁴Th data are consistent with ²¹⁰Pb profiles determined for the same sediments, strongly suggesting that ²³⁴Th and ²¹⁰Pb are mixed equivalently and in a multilayered manner.     

Particle mixing rates in sediments of the eastern equatorial Pacific: Evidence from 210Pb, 239,240Pu and 137Cs distributions at MANOP sites

Particle mixing rates (D_B) 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 (D_B = 0.03?0.4 cm²/y) than for continuous input at a constant rate (D_B = 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 ${}^{\mathrm{239,240}}\text{Pu}{}^{137}\text{Cs}$ 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 ${}^{\mathrm{239,240}}\text{Pu}{}^{137}\text{Cs}$ 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.     

210Pb, 226Ra and 32Si in Pavin lake (Massif Central,France)

Measurements of cosmogenic ³²Si and the U-decay series' nuclides ²¹⁰Pb and ²²⁶Ra in waters and sediments of lake Pavin are reported. Both ²¹⁰Pb and ²²⁶Ra are enriched in the anoxic deep waters compared to the oxic surface waters, respectively by a factor of 4 and 10, whereas ³²Si is depleted by a factor of2. Redox conditions in the lake appear to have no marked effect on the ³²Si. Using a steady-state box model it is shown that the deep-water ³²Si concentration is controlled by the underground lacustrine springs. The residence times of ²¹⁰Pb, ³²Si and ²²⁶Ra are1,10 and80 a, respectively. In the case of ³²Si, where more data are available, the assessed inventory data from the overhead atmospheric fallout and that measured in the sediments agree very well as expected. The ²¹⁰Pb- and ³²Si-based deposition rates during the past100 a ranged from 0.8 to 1.9 mm a⁻¹, earlier these were a factor of3–5 faster. The geochemistry of ³²Si and ²¹⁰Pb in lake Pavin in many ways resembles that in the ocean, only the time scales of the processes involved are faster.     

Determination of 210Pb, 226Ra and 137Cs in sediments

A method is described for bringing a sediment sample into solution and subsequently carrying out analysis for ²¹⁰Pb, ²²⁶Ra and ¹³⁷Cs. Silica is removed from the sample by cyclic HNO₃HF treatments. ¹³⁷Cs is separated from ²¹⁰Ra in a carbonate fusion, extracted by absorption on ammonium molybdophosphate, precipitated directly with BiI₃ in presence of citric acid, and β-counted. ²¹⁰Pb and ²²⁶Ra are separated out by 70–75% HNO³ precipitation. Further purification and mutual separation of the two radionuclides is achieved by solvent extraction and anion-exchange techniques. ²¹⁰Pb and ²²⁶Ra are determined by β- and α- counting of their chromate precipitates, respectively, after allowing suitable ingrowth periods for their daughters. The procedural steps effectively eliminate possible interference from other natural or fall-out radioactivities.     

U-238 series radioactive disequilibrium in groundwaters: implications to the origin of excess U-234 and fate of reactive pollutants

The concentrations of ²³⁸U, ²³⁴Th, ²²⁶Ra, ²²²Rn and ²¹⁰Pb and ${}^{234}\text{U}{}^{238}\text{U}$ activity ratios have been measured in several groundwater samples from Gujarat, India. In the aqueous phase the abundances of ²³⁴Th and ²¹⁰Pb are grossly deficient relative to their parents, ²³⁸U and ²²²Rn respectively. The deficiency is ascribable to the impact adsorption of ²³⁴Th and ²¹⁰Pb atoms onto particle surfaces which are very abundant in the groundwater regimes. The scavenging residence times for both these nuclides is about a day, suggesting that irreversible removal of ‘reactive’ metals and pollutants in groundwaters can occur on very short time scales. The fast removal of ²³⁴Th onto particles necessitates that in these groundwaters ²³⁴U ‘excess’ has to originate through leaching of soil grains rather than through in situ decay of dissolved ²³⁴Th in the water.     

Determination of recent sedimentation rates in Lake Michigan using Pb-210 and Cs-137

This paper describes the use of ²¹⁰Pb and ¹³⁷Cs radioactivity measurements to determine the rates of sedimentation in the Great Lakes. Cores from eight locations in Lake Michigan were chosen for examination to cover as wide as possible a range of sedimentation rates and representative sedimentary environments. The surficial ²¹⁰Pb activity in the sediments varies between 7 and 23 pCi/g dry wt and its profile in each core shows the expected exponential decrease with depth consistent with the assumption of uniform sedimentation rate over the last hundred years and secular equilibrium between supported ²¹⁰Pb and ²²⁶Ra (0.5-1.0 pCi/g dry wt). Companion measurements of ¹³⁷Cs indicate that the coring technique satisfactorily recovered the uppermost levels of the deposit and that the mobility of both radionuclides within the sediment is probably small.Based on the limited number of cores analyzed to date, it appears that modern sedimentation rates are not very different from average rates for the last 7000 yr. The excess ²¹⁰Pb appears to originate primarily from atmospheric fallout, but a further inventory of the ²¹⁰Pb distribution over the lake bottom must be made to properly assess the significance of other sources. The spatial distributions of both ¹³⁷Cs and ²¹⁰Pb at certain stations suggest that the mode of transport of these radionuclides are comparable and involve attachment to settling particles. A mathematical model is developed which accounts for the observed limited mobility of both ²¹⁰Pb and ¹³⁷Cs in several of the cores in terms of post-depositional redistribution by physical or biological mixing processes.     

放射性同位素定年技术在崇明岛潮滩沉积速率上的应用研究

选取崇明岛北侧由东至西4个潮滩沉积柱,分析137Cs、226Ra和210Pb放射性比活度,应用210Pb和137Cs放射性同位素定年方法计算崇明岛潮滩沉积物沉积速率。对于东西两端,210Pb方法测得速率分别为3.08cm/a和2.34 cm/a,而137Cs测得速率分别为6.19 cm/a和2.06 cm/a。结果表明,137Cs定年方法计算出的潮滩沉积速率普遍大于210Pb方法结果;但两者反映了相同的速率规律。崇明岛主力生长方向为东和东北,西侧沉积作用相对较弱,表现出"东快西慢"的特点。沉积纵向上,1954年以来,自下而上沉积速率逐渐减缓。     

Accretion rates and sediment accumulation in Rhode Island salt marshes

In order to test the assumption that accretion rates of intertidal salt marshes are approximately equal to rates of sea-level rise along the Rhode Island coast,²¹⁰Pb analyses were carried out and accretion rates calculated using constant flux and constant activity models applied to sediment cores collected from lowSpartina alterniflora marshes at four sites from the head to the mouth of Narragansett Bay. A core was also collected from a highSpartina patens marsh at one site. Additional low marsh cores from a tidal river entering the bay and a coastal lagoon on Block Island Sound were also analyzed. Accretion rates for all cores were also calculated from copper concentration data assuming that anthropogenic copper increases began at all sites between 1865 and 1885. Bulk density and weight-loss-on-ignition of the sediments were measured in order to assess the relative importance of inorganic and organic accumulation. During the past 60 yr, accretion rates at the eight low marsh sites averaged 0.43±0.13 cm yr^?1 (0.25 to 0.60 cm yr^?1) based on the constant flux model, 0.40±0.15 cm yr^?1 (0.15 to 0.58 cm yr^?1) based on the constant activity model, and 0.44±0.11 cm yr^?1 (0.30 to 0.59 cm yr^?1) based on copper concentration data, with no apparent trend down-bay. High marsh rates were 0.24±0.02 (constant flux), 0.25±0.01 (constant activity), and 0.47±0.04 (copper concentration data). The cores showing closest agreement between the three methods are those for which the excess²¹⁰Pb inventories are consistent with atmospheric inputs. These rates compare to a tide gauge record from the mouth of the bay that shows an average sea-level rise of 0.26±0.02 cm yr^?1 from 1931 to 1986. Low marshes in this area appear to accrete at rates 1.5–1.7 times greater than local relative sea-level rise, while the high marsh accretion rate is equal to the rise in sea level. The variability among the low marsh sites suggests that marshes may not be poised at mean water level to within better than ±several cm on time scales of decades. Inorganic and organic dry solids each contributed about 9% by volume to low marsh accretion, while organic dry solids contributed 11% and inorganic 4% to high marsh accretion. Water/pore space accounted for the majority of accretion in both low and high marshes. If water associated with the organic component is considered, organic matter accounts for an average of 91% of low marsh and 96% of high marsh accretion. A dramatic increase in the organic content at a depth of 60 to 90 cm in the cores from Narragansett Bay appears to mark the start of marsh development on prograding sand flats.     

Precise two chronometer dating of Pleistocene travertine: The Th/U and Raex/Ra(0) approach

In order to determine the geochemical evolution of a freshwater limestone cave system located in central Switzerland (Hell Grottoes at Baar/Zug,) young postglacial tufaceous limestone and travertine precipitates were investigated using the ²³⁰Th/²³⁴U ingrowth system. Additional analyses of further radionuclides within the ²³⁸U decay chain, i.e. ²²⁶Ra and ²¹⁰Pb, showed that the Th/U chronometer started with insignificant inherited ²³⁰Th over the entire formation period of the travertine setting (i.e. ²³⁰Th(0)=0). A contribution from detrital impurities with ²³⁰Th/²³⁴U in secular equilibrium could be precisely subtracted by applying isochron dating of cogenetic phases and recently formed travertine. The resulting precise ²³⁰Th/²³⁴U formation ages were found to be consistent with the geological stratigraphy and were furthermore used to demonstrate the applicability of the next geologically important chronometer in the ²³⁸U-decay series, based on decay of excess ²²⁶Ra normalized to the initial, i.e.²²⁶Ra_ex/²²⁶Ra(0). This system is suitable for dating phases younger than 7000 yr when the correction of a detritus component increasingly limits the precision of the ²³⁰Th/²³⁴U chronometer. Analytical solutions of the coupled ²³⁴U/²³⁰Th/²²⁶Ra radionuclide system predicted that the ²²⁶Ra_ex/²²⁶Ra(0) chronometer is independent of the actual ²³⁰Th activity build up from decay of ²³⁴U, if the systems starts with zero inherited ²³⁰Th(0). The data set confirmed this hypothesis and showed furthermore that the initially incorporated ²²⁶Ra excess must have remained almost uniform in all limestone over a period of at least 7000 yr, i.e. 4–5 half-lives of ²²⁶Ra. This is concluded because (i) the ²²⁶Ra_ex/²²⁶Ra(0) ages agreed well with those derived from ²³⁰Th/²³⁴U, (ii) all data plot within uncertainty on the ²²⁶Ra_ex/²²⁶Ra(0) decay curve and (iii) the atomic Ba/Ca ratio was found to be constant in the travertine material independent of the sample ages. Provided that such boundary conditions hold, ²²⁶Ra_ex/²²⁶Ra(0) should be applicable to materials which are suitable for ²³⁰Th/²³⁴U dating in sedimentology and oceanography, i.e. travertine, corals, phosphorites, etc., and should strongly support ²³⁰Th/²³⁴U for samples that have been formed a few thousand years ago.     

Evaluation of lead isotopic methods for uranium exploration, Koongarra Area, Northern Territory, Australia

Analysis of radioactive (²¹⁰Pb) and stable lead isotopes in near-surface samples has been tested as a method of uranium exploration in the Pine Creek Geosyncline, Northern Territory, Australia. The lead isotopes were extracted from the samples by a mild leaching agent and were measured by alpha spectrometry for ²¹⁰Pb and by mass spectrometry for stable lead isotopes. The results are compared with those obtained by conventional methods utilizing measurements of radioactivity and radon (Track Etch) in situ and ²²⁶Ra, ²²⁸Ra and U contents of soils. The major problems addressed were whether the lead isotopic methods are more sensitive than the conventional methods and whether they can discriminate “real” anomalies from the common barren anomalies found in black soils and swamps which contain radium in excess of the uranium present.Four test areas, representing a range of exploration problems, were chosen in the vicinity of the Koongarra uranium deposits and 25 samples from each area were analyzed. Most samples have more ²²⁶Ra than uranium. Radium analyses of several water samples show the source of this radium to be non-uraniferous rocks within the Kombolgie sandstone. The results for soil ²²⁶Ra, radon, scintillometry and ²¹⁹Pb were generally closely correlated, and as a result, the ²¹⁰Pb method was not considered to have any advantages over the conventional methods.At the Koongarra X prospect, which has a weak surface expression, the ratio gave the strongest indication of the underlying uranium mineralization with an anomaly to background ratio of 12.5. However, this ratio is correlated with uranium content and does not offer any particular advantages over uranium analyses alone. More subtle indications of uranium mineralization were found by relating the radiogenic lead (²⁰⁶Pb) and the thorium-derived lead (²⁰⁸Pb) to the common lead content (²⁰⁴Pb). A plot of versus (horizontal axis) is linear for country rock samples, irrespective of the amount of more recently introduced ²²⁶Ra. Samples above uranium mineralization lie off this trend, along a line of near-zero slope. By the use of this plot, indications were found of the Koongarra No. 2 orebody, which is concealed by about 40 m of barren overburden; none of the other techniques detected this mineralization.     

Consequences of diffuse and channelled porous melt migration on uranium series disequilibria

Magmas erupted at mid-ocean ridges (MORB) result from decompression melting of upwelling mantle. However, the mechanism of melt transport from the source region to the surface is poorly understood. It is debated whether melt is transported through melt-filled conduits or cracks on short time scales (<∼ 10³ yrs), or whether there is a significant component of slow, equilibrium porous flow on much longer time scales (>∼ 10³-10⁴ yrs). Radiogenic excess ²²⁶Ra in MORB indicates that melt is transported from the melting region on time scales less than the half life of ²²⁶Ra (∼1600 yrs), and has been used to argue for fast melt transport from the base of the melting column. However, excess ²²⁶Ra can be generated at the bottom of the melt column, during the onset of melting, and at the top of the melt column by reactive porous flow. Determining the depth at which ²²⁶Ra is generated is critical to interpreting the rate and mechanism of magma migration. A recent compilation of high quality U-series isotope data show that in many young basalts, ²²⁶Ra excess in MORB is negatively correlated with ²³⁰Th excess. The data suggest that ²²⁶Ra excess is generated independently of ²³⁰Th excess, and cannot be explained by “dynamic” or fractional melting, where observed radiogenic excesses are all generated at the base of the melt column. One explanation is that the negative correlation of activity ratios is a result of mixing of slow moving melt that has travelled through reactive, low-porosity pathways and relatively fast moving melt that has been transported in unreactive high-porosity channels. We investigate this possibility by calculating U-series disequilibria in a melting column in which high-porosity, unreactive channels form within a low-porosity matrix that is undergoing melting. The results show that the negative correlation of ²²⁶Ra and ²³⁰Th excesses observed in MORB can be produced if ∼60% of the total melt flux travels through the low-porosity matrix. This melt maintains ²²⁶Ra excesses via chromatographic fractionation of Ra and Th during equilibrium transport. Melt that travels through the unreactive, high-porosity channels is not able to maintain significant ²²⁶Ra excesses because Ra and Th are not fractionated from each other during transport and the transport time for melt in the channels to reach the top of the melt column is longer than the time scale for ²²⁶Ra excesses to decay. Mixing of melt from the high porosity channels with melt from the low-porosity matrix at the top of the melting column can produce a negative correlation of ²²⁶Ra and ²³⁰Th excesses with the slope and magnitude observed in MORB. This transport process can also account for other aspects of the geochemistry of MORB, such as correlations between La/Yb, α_Sm/Nd, and Th/U and ²²⁶Ra and ²³⁰Th excess.     

Flow of metals into the global atmosphere

Concentrations of ¹³⁷Cs, ²¹⁰Pb, ²²⁶Ra, U, V, Pb, Cd and Hg have been measured in firn and ice deposited during the past three decades in accumulation zones of glaciers and also in pre-industrial glacier ice collected in Spitsbergen, Northern Norway, Alaska, Southern Norway, Alps, Himalayas, Ruwenzori, Peruvian Andes, and at King George Island in Antarctica. Except for Hg, the geographical distribution of mean concentrations of ²²⁶Ra, U and stable heavy metals in contemporary ice is not uniform, with the lowest concentrations found in Northern Norway, Alaska and Antarctica, and the highest in continental locations at equatorial and middle latitudes. We did not find evidence of changes in rate of metal deposition during the last three decades, as compared with pre-industrial period, however, our samples of pre-industrial ice might be contaminated in part by contemporary fallout migrating from the exposed surface of old parts of glaciers into the deeper ice layers. Using the data on annual injections of ¹³⁷Cs into the global atmosphere and mean global concentrations of radionuclides and heavy metals found in contemporary ice the global annual flows of ²²⁶Ra, ²¹⁰Pb, U,V, Pb, Cd and Hg were estimated as 6.6 kCi, 485 kCi, 12kt, 4870kt, 590 kt, 180 kt and 190 kt, respectively. These estimates are 1–2 orders of magnitude higher than estimates based on primary paniculate emissions. The anthropogenic contribution is a small fraction of the flows, which are dominated by natural processes leading to enrichment of metals in airborne dust.     

The use of 210Pb as a heavy metal tracer in the Susquehanna River system

Analysis of soil profiles and shallow ground water in the Susquehanna River basin, northeastern U.S.A., indicates that the atmospheric flux of ²¹⁰Pb is efficiently scavenged by the organic-rich horizons of the soils. This atmospherically supplied ²¹⁰Pb in soil profiles can only be lost from the system by soil erosion. Based on the annual sediment yield of the Susquehanna River and the excess ²¹⁰Pb concentration in particulate matter, a mean residence time of 2000 yr is calculated for metals similar to Pb in soil profiles.The West Branch of the Susquehanna River (WBSR) is strongly affected by acid mine drainage and is low in pH and high in dissolved ( <0.4 μm) ²¹⁰Pb, Fe and Mn. Along its course iron hydroxide is precipitating at a pH of between 4 and 4.5 and the ²¹⁰Pb supplied by the acid mine water is diminished by about 25% as a result of dilution. As the WBSR enters the Valley and Ridge Province of the Appalachians it has a ²¹⁰Pb concentration of ~ 0.2 dpm/l. At this juncture it receives a considerable influx of alkalinity from tributaries draining carbonate terranes, resulting in neutralization of the sulfuric acid and increase of the river pH to around 6.5–7. This pH adjustment is accompanied by the precipitation of Fe and Mn. Due to the slow rate of Mn removal from solution, the Mn precipitation extends a considerable distance down river from the point of acid neutralization. Analyses for ²¹⁰Pb in the river at points in or below the region of Mn precipitation show that ²¹⁰Pb is rapidly scavenged from solution onto suspended particles. From the data it is possible to calculate the removal rate of Pb from water in the presence of Fe and Mn hydroxides and other particles. At a pH of 4–4.5 Pb removal is nonexistent relative to the river flow rate, but at a pH of 6.5–7 the ²¹⁰Pb data indicate a residence time of <0.7 day for dissolved Pb.     

Differential behavior of components of the <Superscript>238</Superscript>U-<Superscript>206</Superscript>Pb and <Superscript>235</Superscript>U-<Superscript>207</Superscript>Pb isotopic systems in polymineralic U ores

U-Pb systems were examined in samples (ranging from 4 to 10 cm³ in volume) of ore material taken from along a 3.5-m profile across a zone of U mineralization exposed in an underground mine at the Strel’tsovskoe U deposit in eastern Transbaikalia. The behaviors of two isotopic U-Pb systems (²³⁸U-²⁰⁶Pb and ²³⁵U-²⁰⁷Pb) are principally different in all samples from our profile. While the individual samples are characterized by a vast scatter of their T(²⁰⁶Pb/²³⁸U) age values (from 112 to 717 Ma), the corresponding T(²⁰⁷Pb/²³⁵U) values vary much less significantly (from 127 to 142 Ma) and are generally close to the true age of the U mineralization. The main reason for the distortion of the U-Pb system is the long-lasting (for tens of million years) migration of intermediate decay products in the ²³⁸U-²⁰⁶Pb(RD²³⁸U) in the samples. This process resulted in the loss of RD²³⁸U from domains with high U concentrations and the subsequent accommodation of RD²³⁸U at sites with low U concentrations. The long-term effect of these opposite processes resulted in a deficit or excess of ²⁰⁶Pb as the final product of ²³⁸U decay. The loss or migration of RD²³⁸U are explained by the occurrence of pitchblende in association with U oxides that have higher Si and OH concentrations than those in the pitchblende and a higher ⁺⁶U/⁺⁴U ratio. The finely dispersed character of the mineralization and the loose or metamict texture of the material are the principal prerequisites for RD²³⁸U loss and an excess of ²⁰⁶Pb in adjacent domains with low U concentrations. Domains with low U contents in the zone with U mineralization serve as geochemical barriers (because of sulfides contained in them) at which long-lived RD²³⁸U(²²⁶Ra, ²¹⁰Po, ²¹⁰Bi, and ²¹⁰Pb) were accommodated and subsequently caused an excess of ²⁰⁶Pb. The ²³⁵U-²⁰⁷Pb system remained closed because of the much briefer lifetime of the ²³⁵U decay products. This may account for the significant discrepancies between the T(²⁰⁶Pb/²³⁸U) and T(²⁰⁷Pb/²³⁵U) age values. RD²³⁸U was most probably lost via the migration of radioisotopes at the middle part and end of the ²³⁸U family (starting with ²²⁶Ra). The heavy Th, Pa, and U radioisotopes (²³⁴Th, ²³⁴Pa, ²³⁴U, and ²³⁰Th) that occur closer to the beginning of ²³⁸U decay, before ²²⁶Ra, only relatively insignificantly participated in the process. Our results show that the loss and migration of RD²³⁸U are, under certain conditions, the main (or even the only) process responsible for the distortion of the U-Pb system.     

Temporal dynamics of airborne lead-210 in Missouri (USA): implications for geochronological methods

 Lead-210 (²¹⁰Pb) deposited from the atmosphere is used in the dating of certain geological materials such as glacial ice and lacustrine sediments, but its long-term atmospheric behavior has been little studied. The present investigation reports measurements of airborne ²¹⁰Pb at 21 monitoring stations in Springfield, Missouri, during 1975–1995. Seasonal and diurnal patterns of atmospheric concentrations are established, and the mean annual concentrations of ²¹⁰Pb in ground level air during the 20-year period are examined. Although airborne ²¹⁰Pb concentrations are found to vary diurnally and seasonally, mean annual concentrations in southwest Missouri have remained relatively constant during this time period. This finding is important for geochronological methods that assume a constant ²¹⁰Pb flux from the atmosphere. Received: 8 September 1998 · Accepted: 12 October 1998     

Suspended sediment sources and tributary effects in the lower reaches of a coastal plain stream as indicated by radionuclides, Loco Bayou, Texas

Characterizing the dynamics of fluvial sediment sources over space and time is often critical in identifying human impacts on fluvial systems. Upland interfluve and subsoil sources of suspended sediment at Loco Bayou, Texas, were distinguished using ²²⁶Ra/²³²Th, ²²⁶Ra/²³⁰Th and, ²²⁸Ra/²³²Th. Source contributions were apportioned at three stations during within-bank and flood flows. ¹³⁷Cs and ²¹⁰Pb_xs (excess ²¹⁰Pb) were used to determine floodplain sedimentation; suspended sediment ²¹⁰Pb_xs/¹³⁷Cs data mirrored results of Ra/Th, showing dominance of subsoil sources during within-bank flows, changing to interfluve sources during flood. This trend corresponds spatially to influx of sediment from ephemeral tributaries, reflecting mobilization of stored interfluvial sediments during flood stage. Upper basin sedimentation was similar but markedly less at the lowermost station. These results indicate (1) modified ephemeral tributaries store sediment derived from sheet wash, discharging them during flood, and (2) southernmost Loco Bayou is episodically re-worked, resulting in significantly reduced local rates of sedimentation.     

210Pb activities in and fluxes to sediments of the Washington continental slope and shelf

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.