Laboratory studies of the diagenesis and mobility of 239,240pu and 137Cs in nearshore sediments

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

The pore water chemistry of 239,240Pu and 137Cs in sediments of Buzzards Bay,Massachusetts

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. SO₄^2?, 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 $\text{0.01 ± 0.02}$ 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.     

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.     

Plutonium, 241Am and 137Cs ratios,inventories and vertical profiles in Washington and Oregon continental shelf sediments

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.     

Transport and accumulation of actinide elements in the near-shore environment: field and modelling studies

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.     

Changes in the sorption capacity of Coastal Plain sediments due to redox alteration of mineral surfaces

Chemical characteristics of grain coatings in a Coastal Plain sandy aquifer on the Eastern Shore of Virginia were investigated where sediments have been exposed to distinct groundwater redox conditions. Dissolved O₂ was 5.0 to 10.6 mg L⁻¹ in the regionally extensive aerobic groundwater, whereas in a narrow leachate plume it was only <0.001 to 0.9 mg L⁻¹. The amount of dissolved Fe in the aerobic groundwater was only 0.005 to 0.01 mg L⁻¹, but it was 12 to 47 mg L⁻¹ in the anaerobic zone. The amount of extractable Fe was an order of magnitude higher for the aerobic sediments than for the anaerobic sediments indicating that reductive dissolution removed the oxide coatings. The capacity for anion sorption on the sediment surfaces, as indicated by the sorption of ³⁵SO₄^2-, was an order of magnitude higher in the aerobic vs. anaerobic sediments. The presence of anaerobic groundwater did not significantly alter the amount of extractable Al oxides on the surface of the sediments, and those coatings helped to maintain a high surface area. The removal of the Fe oxides from the grain surfaces under anaerobic conditions was solely responsible for the significant reduction of SO₄ sorption observed. This loss of capacity for anion sorption could lead to more extensive transport of negatively charged constituents such as some contaminant chemicals or bacteria that may be of concern in groundwater.     

Isotopic fractionation associated with biosynthesis of fatty acids by a marine bacterium under oxic and anoxic conditions

Shewanella putrefaciens (Strain MR-4), a gram negative facultative marine bacterium, was grown to stationary phase under both aerobic and anaerobic conditions using lactate as the sole carbon source. Aerobically-produced cells were slightly enriched in ¹³C (+1.5‰) relative to the lactate carbon source, whereas those from anaerobic growth were depleted in ¹³C (−2.2‰). The distribution of fatty acids produced under aerobic conditions was similar to that resulting from anaerobic growth, being dominated by C_16:1 ω7 and C_16:0 fatty acids with a lesser amount of the C_18:1 ω7 component. Low concentrations of saturated even numbered normal fatty acids in the C₁₄ to C₁₈ range, and iso-C_15:0 were synthesized under both conditions. Fatty acids from anaerobic cultures (average δ¹³C=−37.8‰) were considerably depleted in ¹³C relative to their aerobically-synthesized counterparts (−28.8‰). The distinct differences in isotopic composition of both whole cells and individual fatty acid components result from differences in assimilation pathways. Under aerobic conditions, the primary route of assimilation involves the pyruvate dehydrogenase enzyme complex which produces acetyl-CoA, the precursor to lipid synthesis. In contrast, under anaerobic conditions formate, and not acetate, is the central intermediate in carbon assimilation with the precursors to fatty acid synthesis being produced via the serine pathway. Anaerobically-produced bacterial fatty acids were depleted by up to 12‰ relative to the carbon source. Therefore, detection of isotopically depleted fatty acids in sediments may be falsely attributed to a terrestrial origin, when in fact they are the result of bacterial resynthesis.     

NE8420汽车伽玛能谱仪241Am自稳装置

NE8420汽车伽玛能谱仪因无自稳电路,影响测量精度的提高。本文介绍采用²⁴¹Am为参考源的自稳装置的线路框图、工作原理及性能测试结果。     

The effect of fulvic acid on the sorption of actinides and fission products on granite and selected minerals

Organic material is present at low concentrations, typically 1–2 mg/l in terms of dissolved organic carbon (DOC), in groundwaters deep in granitic rock. Hydrophobic and hydrophilic acids may complex inorganic contaminants and change their sorption behaviour on geological materials. This report describes a series of experiments performed under aerobic conditions to investigate the effects of fulvic acid over a concentration range of 0–5 mg/I DOC on the sorption of⁸⁵Sr,¹³⁷Cs,²³³U,²³⁸Pu and²⁴¹'Am by crushed granite, biotite, goethite, montmorillonite and quartz. In addition, similar solutions were used to study the effects of dissolved fulvic acid on the sorption of⁹⁹Tc and¹²⁵I on each of the above solids except quartz. The fulvic acid was extracted from groundwater collected at a depth of 240 m in the granitic rock of the Underground Research Laboratory near Lac du Bonnet, Manitoba.In all experiments, the sorption of the fulvic acid by the geological materials was in the order goethite montmorillonite > biotite > granite > quartz. No sorption of Tc was observed from any of the solutions on any of the solids. Low sorption of I on montmorillonite occurred in the presence of the dissolved organic material. No sorption of I was observed with the other solids used. Only montmorillonite sorbed any appreciable amount of Sr in this study with the fulvic acid having no effect on this sorption. All the solids except quartz sorbed substantial amounts of Cs, but sorption was not affected by the organic material in solution. Each of the solids sorbed U with no difference in sorption observed due to the dissolved organic. In general, Pu sorption decreased as the concentration of dissolved fulvic acid increased. However, sorption of Pu on quartz remained at approximately the same levels regardless of the concentration of organic in solution. Generally high sorption of Am was found. Lowest sorption of Am on all solids occurred from the solution with the highest concentration of fulvic acid. Sorption of Am on granite decreased as the concentration of the organic in solution increased.This study indicated that, under aerobic conditions, the effect of dissolved organic material on sorption of radioisotopes depends on the radioisotope in question and the concentration of the organic in solution.     

Comparative 210Pb, 137Cs,and pollen geochronologies of sediments from Lakes Ontario and Erie

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.     

Comparisons of 210Pb and pollen methods for determining rates of estuarine sediment accumulation

Comparisons of sedimentation rates obtained by ²¹⁰Pb and pollen analyses of 1-m cores collected throughout the Potomac Estuary show good agreement in the majority of cores that can be analyzed by both methods. Most of the discrepancy between the methods can be explained by the analytical precision of the ²¹⁰Pb method and by the exactness with which time horizons can be identified and dated for the pollen method. X-radiographs of the cores and the distinctness of the pollen horizons preclude significant displacement by reworking and/or mixing of sediments. Differences between the methods are greatest where uncertainties exist in assigning a rate by one or both methods (i.e., ²¹⁰Pb trends and/or “possible” horizon assignments). Both methods show the same relative rates, with greater sediment accumulation more common in the upper and middle estuary and less toward the mouth. The results indicate that geochronologic studies of estuarine sediments should be preceded by careful observation of sedimentary structures, preferably by X-radiography, to evaluate the extent of mixing of the sediments. Time horizons, whether paleontologic or isotopic, are generally blurred where mixing has occurred, precluding precise identification. Whenever possible, two methods should be used for dating sediments because a rate, albeit erroneous, can be obtained isotopically in sediments that are mixed; accurate sedimentation rates are also difficult to determine where the time boundary is a zone rather than a horizon, where the historical record does not provide a precise date for the pollen horizon, or where scouring has removed some of the sediment above a dated pollen horizon.     

Americium interaction with calcite and aragonite surfaces in seawater

Observations of the distribution of ²⁴¹Am in the marine environment indicate that Am has a high affinity for solid surfaces. The adsorption of Am onto calcite and aragonite surfaces from seawater and related solutions has been studied, in order to establish the interaction of Am with a major component of many marine sediments. Results indicate that Am is rapidly and strongly adsorbed. This occurs even when both dissolved Am concentrations and solid to solution ratios are low. The minimum value for $\text{K}{}_{\mathrm{D}}$ determined is 2 × 10⁵. Measurements of reaction kinetics established that Am is adsorbed from seawater at 40 times the rate per unit surface area on synthetic aragonite that it is on synthetic calcite. Approximately 15% of the difference is attributable to epitaxial influences, with the remainder being due to enhanced site competition by Mg on calcite relative to aragonite. The adsorption rate is first order with respect to Am concentration, but follows approximately the square root of the solid surface area to solution volume ratio.Adsorption rate of Am on biogenic aragonite and Mg-calcites are, within a given particle size range, close to equal. It is not possible to normalize these adsorption rates to surface area due to the differing microporous structure of biogenic carbonates. The Am adsorption rates on a shallow water calcium carbonate-rich sediment gave results which were predicted from, its mineralogie mixture of components.     

Association of dissolved radionuclides released by the Chernobyl accident with colloidal materials in surface water

The association of dissolved ⁹⁰Sr, ^239,240Pu and ²⁴¹Am with natural colloids was investigated in surface waters in the Chernobyl nuclear accident area. A 4-step ultrafiltration (UF) study (<1 kilodaltons (Da), 1–10 kDa, 10–100 kDa, 100 kDa<) showed that 49–83% of ^239,240Pu and 76% of ²⁴¹Am are distributed in colloids of the two size fractions larger than 10 kDa (nominal molecular weight limit of the filter, NMWL), while ⁹⁰Sr was found exclusively (85–88%) in the lowest molecular size fraction below 1 kDa (NMWL) for the Sahan River water at the highly contaminated area close to the Chernobyl Nuclear Power Plant (ChNPP). Consistent results were obtained by 2-step fractionation (larger than and smaller than 10 kDa (NMWL)) for river and lake waters including other locations within about 30 km away from ChNPP. It is likely that Pu and Am isotopes were preferentially associated with dissolved organic matter of high molecular size, as suggested by the fact that (i) only a few inorganic elements (Mg, Ca, Sr, Si, Mn, Al) were found in the colloidal size ranges, and (ii) the positive correlation between dissolved organic C (DOC) concentrations and UV absorbance at 280 nm, a broad absorption peak characteristic of humic substances (HS) was found. A model calculation on the complexation of Pu and Am with HS as an organic ligand suggests that the complexed form could be dominant at a low DOC concentration of 1 mgC L⁻¹, that is commonly encountered as a lower limit in fresh surface water. The present results suggest the general importance of natural organic colloids in dictating the chemical form of actinides in the surface aquatic environment.     

Anomalous isotopic concentrations in the sea off Southern California

Measurements are reported of the ¹⁰Be concentrations in 15 sediments from the sea off southern California. The sedimentation patterns are modelled with a two component system, one component having the high ¹⁰Be concentration of pelagic sediment and the other the low concentration of continental runoff. The pelagic component, brought to the region by the California Current with the Pacific Ocean as reservoir, is very likely the source not only of anomalously high ¹⁰Be deposition but also of similar effects with ²¹⁰¹Pb, ^239,240pu and ²⁴¹Pu.     

Mg2+ removal in the system Mg2+—amorphous SiO2—H2O by adsorption and Mg-hydroxysilicate precipitation

Two chemical processes can remove Mg²⁺ from suspensions containing amorphous silica (am-SiO₂) at low temperatures: adsorption and precipitation of a Mg-hydroxysilicate resembling sepiolite. Mg²⁺ removal from am-SiO₂ suspensions was investigated, and the relative role of the two removal processes evaluated, as a function of: pH, ionic strength, Mg²⁺ concentration, and temperature.The extent of Mg²⁺ adsorption onto am-SiO₂ decreases with increasing NaCl concentration due to displacement of Mg²⁺ by Na⁺. At NaCl concentrations of 0.05 M and above, adsorption occurs only at pH values above 8.5, where rapid dissolution of am-SiO₂ gives rise to high concentrations of dissolved silica, resulting in supersaturation with respect to sepiolite. Removal of Mg²⁺, at concentrations of 40 to 650 μM, from am-SiO₂ suspensions in 0.70 M NaCl at 25 °C occurs at pH 9.0 and above. Experiments show that under these conditions adsorption and Mg-hydroxysilicate precipitation remove Mg²⁺ at similar rates. For 0.05 M Mg²⁺, at 0.70 M ionic strength and 25 °C, measurable Mg²⁺ removal occurs down to ca. pH 7.5 but is primarily due to Mg-hydroxysilicate precipitation. For the same solution conditions at 5°C, Mg²⁺ removal occurs above pH 8.0 and is primarily due to adsorption.Assuming that increasing pressure does not greatly enhance adsorption, Mg²⁺ adsorption onto am-SiO₂ is an insignificant process in sea water. The surface charge of pristine am-SiO₂ in sea water is primarily controlled by interactions with Na⁺. The principal reaction between Mg²⁺ and am-SiO₂ in marine sediments is sepiolite precipitation.The age distribution of sepiolite in siliceous pelagic sediments is influenced by temperatures of bottom waters and by geothermal gradients.     

Role of prior exposure on anaerobic degradation of naphthalene and phenanthrene in marine harbor sediments

The anaerobic degradation of the polycyclic aromatic hydrocarbons (PAHs) naphthalene and phenanthrene was investigated in several marine harbor sediments. In sediments from Boston Harbor that were heavily contaminated with petroleum, [¹⁴C]-naphthalene and [¹⁴C]-phenanthrene were oxidized to ¹⁴CO₂ without a lag, suggesting that the microbial community was adapted for anaerobic PAH oxidation in situ. The addition of molybdate, a specific inhibitor of sulfate-reducing microorganisms, inhibited PAH mineralization which suggested that sulfate reducers were involved in the anaerobic oxidation of the PAHs. PAHs were also anaerobically oxidized at another site in Boston Harbor that was less heavily contaminated, but at a slower rate than in the most heavily contaminated sediments. Sediments not contaminated with petroleum did not significantly oxidize the PAHs. A similar correspondence between rates of anaerobic PAH oxidation and the degree of PAH contamination was observed in sediments from Tampa Bay and San Diego Bay. When relatively pristine sediments from San Diego Bay that did not have a significant capacity for anaerobic PAH oxidation were exposed to high concentrations of naphthalene, they developed a potential for naphthalene degradation that was comparable to that in sediments that had a history of PAH contamination. The increase in potential for naphthalene degradation in the sediments exposed to naphthalene was associated with an increase in naphthalene-degrading microorganisms. These results suggest that many marine harbor sediments contain microorganisms capable of anaerobically oxidizing PAHs under sulfate-reducing conditions and that these microorganisms will respond with an increase in their activity when PAHs are introduced into the sediments. Thus, if PAH inputs into harbor sediments from petroleum can be reduced there may be a widespread potential for microorganisms to remove this PAH contamination from the sediments, despite anaerobic conditions.     

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.     

东北四海龙湾玛珥湖沉积物纹层计年与137Cs、210Pb测年

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。}     

Adsorption of Co and selected actinides by Mn and Fe oxides in soils and sediments

Iron and Mn oxides and associated radionuclides in soils and sediments from the radioactive waste burial grounds at Oak Ridge National Laboratory have been selectively extracted using wet chemical techniques. Product-moment-correlation analyses have demonstrated that ⁶⁰Co and various actinides, principally ²⁴⁴Cm, ²⁴¹Am and ²³⁸Pu are dominantly associated with Mn oxides. Correlation coefficients between these radionuclides and Fe oxides and organic C are generally very low. The important role of Mn oxides in radionuclide adsorption is attributed to their unique surface and colloidal properties. The data illustrate the importance of the Mn oxide component of soils and sediments in controlling transition metal and actinide solubility.These results suggest two major implications for the disposal of radioactive waste. First, in order to minimize future ⁶⁰Co and actinide mobilization from disposal sites, a chemical environment in which Mn oxides are least soluble should be maintained. Second, the liberal use of Mn oxides in waste management operations might improve long-term retention of these radionuclides. Deep-sea Mn modules, which may in the future be mined for their trace metal contents, could serve as a ready supply of Mn oxide for waste disposal applications.     

深海沉积物10Be记录研究

DSDP519钻孔¹⁰Be测定结果表明，在B／M，M／G两地磁极性倒转期间，¹⁰Be产生率均约增加20％。DSDP519孔δ¹⁰Be曲线与DSDP502孔δ¹⁸O曲线具有明显的正相关关系。CT85－5钻孔¹⁰Be曲线在34000±3000aB．P存在明显的峰，峰值比正常值高出2．5倍，⁹Be，Zn变化曲线中均未观察到此峰，与Vostok冰芯¹⁰Be峰在时间上属于同期。这进一步说明了此时期内¹⁰Be浓度增加是全球性的，只能归因于¹⁰Be产生率的增加。Raisbeck峰讯号可以成为某些储存库精确时标。