Uranium-series chronology for sediments of Lake Hovsgol, Mongolia, and the 1-Ma records of uranium and thorium isotopes from the HDP-04 drill core

Uranium and thorium isotopes in an 81-m long sediment core (HDP-04) of Lake Hovsgol, Mongolia, were measured to investigate their downcore distributions and to explore potential linkage to paleoenvironmental changes. Three-dimensional isochron techniques using isotope-ratio diagrams in ²³⁸U–²³⁴U–²³⁰Th–²³²Th system presented by Ludwig and Titterington were applied to age date the lake sediments at the depths of 11.42, 14.71 and 14.83 m in the HDP-04 section, the estimated ages of these horizons are 66 ± 8, 122 ± 11 and 128 ± 22 ka, respectively. The ²³⁸U concentration throughout the entire section fluctuated by a factor of 12, ranging from 19.9 to 232.1 mBq/g with anomalously high ²³⁸U peak at 23.8 m in depth, while the ²³²Th concentration varied only by a factor of about two between 24.3 and 54.0 mBq/g. The discrimination of the bulk ²³⁸U into authigenic and terrigenous ²³⁸U fractions was attempted, based on the measured ²³²Th as a correction index for terrigenous materials. In the upper 24 m corresponding to the last 250 ka, the authigenic ²³⁸U was higher in interglacials and lower in glacials. This depth profile of authigenic ²³⁸U contents was almost identical pattern with that found in a sediment core (VER98-1-6) from the Academician Ridge, Lake Baikal. Further, this profile can be correlated well with that of photosynthetic pigment contents, one of proxies of paleoproductivity, suggesting that the variation of authigenic ²³⁸U contents were associated with the environmental change around Lake Hovsgol.     

U-Pb systems and U isotopic composition of the sandstone-hosted paleovalley Dybryn uranium deposit, Vitim uranium district, Russia

The isotopic (U-Pb, ²³⁸U-²³⁵U, ²³⁴U-²³⁸U) and chemical study of whole-rock samples and finegrained fractions of rocks in a vertical section of the terrigenous sequence at the Dybryn uranium deposit in the Khiagda ore field shows that a wide U-Pb isotopic age range (26.9-6.5 Ma) is caused by oxidation and disturbance of the U-Pb isotopic system in combination with protracted uranium ore deposition. The oxidation of rocks resulted in the loss of uranium relative to lead and eventually to an overestimated ²⁰⁶Pb/²³⁸U age at sites with a low U content. The ²³⁸U/²³⁵U ratios in the studied samples are within the range of 137.74–137.88. Samples with a high uranium content are characterized by a decreasing ²³⁸U/²³⁵U ratio with a decrease in ²⁰⁷Pb/²³⁵U and ²⁰⁶Pb/²³⁸U ages. A nonequilibrium ²³⁴U/²³⁸U ratio in most studied samples furnishes evidence for young (<1.5 Ma) transformation of the Miocene uranium ore, which is responsible for uranium migration and its redeposition.     

Distribution of natural uranium,thorium, lead,and polonium radionuclides in tidal phases of a Delaware salt marsh

Natural radionuclides in the uranium and thorium series were measured in solid tidal phases (suspended particles, bottom sediment, surface microlayer colloids) of a salt marsh in lower Delaware. The purpose was to identify potential processes responsible for trace element cycling (sources, redistribution and exchange) in salt water marshes and with their coastal waters. Generally, concentrations of U, Th,²¹⁰Pb, and²¹⁰Po on the tidal solid phases suggest a general mechanism by which tidal marshes appear to be trapping the nuclides into their interiors. The processes may include transport of enriched fine particles into the marsh, capture by salt marsh grass and chemical fixation by redox processes at the sediment surface. Specifically, the uranium contents of most of the samples are similar with activity ratios²³⁴U²³⁸U≧1, indicating a mixture of detrital and nondetrital (authigenic) uranium inputs such as seawater or ground water. Since the²³⁰Th daughter is generally deficient by about 50%, the authigenic enrichment process appears to favor uranium and is potentially linked to the extensive diagenetic sulfur redox cycle of salt marsh sediments. The²¹⁰Po/²¹⁰Pb activity ratio is less than one on Spartina adsorbed solids, and could suggest a general process in salt marshes which favors²¹⁰Pb enrichment by atmospheric fallout over enrichment of²¹⁰Po on time scales of weeks which correspond to complete tide marsh exchange. A²²⁸Th/²³²Th activity ratio of less than unity on the solids adsorbed onto marsh grass suggests a net process whereby diffusive loss of the intermediate daughter²²⁸Ra from the adsorbed solids to tidal waters dominates over potential²²⁸Th scavenging by suspended sediment.     

Behavior of isotope (<Superscript>18</Superscript>O/<Superscript>16</Superscript>O, <Superscript>234</Superscript>U/<Superscript>238</Superscript>U) systems during the formation of uranium deposits of the “sandstone” type

The uneven character of the distribution of ¹⁸O/¹⁶O and ²³⁴U/²³⁸U values was established in the vertical cross section of the productive sequence of the Dybryn uranium deposit (Vitim uranium-ore region, Buryatia). Both a deficiency and an excess of ²³⁴U in relation to the equilibrium ²³⁴U/²³⁸U ratio in the vertical sequence may provide evidence for the extremely low rate of the infiltration water flow. The behavior of oxygen isotope characteristics for different size fractions of terrigenous rocks provides evidence for active uranium redistribution and openness of the isotope system of this element during interaction of terrigenous–sedimentary rocks with infiltration waters.     

U-series isotopic composition of kasolite associated with aplite-pegmatite at Jabal Sayid,Hijaz region,Kingdom of Saudi Arabia

Uranium and thorium isotopic composition of kasolite [Pb(UO₂)SiO₄-(H₂O)] from Jabal Sayid area was determined by thermal ionization mass spectrometry. Secondary electron imaging, back-scattered electron imaging, and energy dispersive spectral scans were used to investigate the mineralogical characteristics of this uranyl mineral phase. Distinct crystal faces and crystal growth of kasolite from the study area confirm mineral precipitation near the surface from the circulating groundwater. The obtained data were used to interpret the mechanism of uranium mobility in Jabal Sayid weathering profile and to construct a tentative model to explain the isotopic evolution of uranium and thorium. This model indicates that (1) uranium was leached at depth, (2) uranyl mineralization was precipitated along fractures and cavities in the host rocks during humid conditions and pluvial periods, (3) preferential leaching of ²³⁴U from uranyl mineralization by recoil processes was continuous indicative of a weakly circulating groundwater, and (4) ²³⁴U-deficiency resulted in isotopic signatures characterized by low ²³⁴U/²³⁸U and high ²³⁰Th/²³⁴U ratios. The modification pattern of these activity ratios suggests that uranyl mineralization of Jabal Sayid, most probably, has been precipitated during the same Late Quaternary pluvial periods responsible for the formation of the corresponding mineralizations in the Eastern Desert of Egypt.     

水－岩反应的铀系不平衡判别

天然体系中水－岩反应的铀系不平衡判别,是基于水－岩反应使岩石中天然铀衰变系子体核素＾２３４Ｕ,＾２２６Ｒｂ和六价铀的选择性溶失,造成原始放射性平衡遭到不同程度破坏,因而可利用现今测得的岩石中３组核素放射性活度比值Ａ（＾２３４Ｕ）／Ａ（＾２３８Ｕ）,Ａ（＾２３０Ｔｈ）／Ａ（＾２３４Ｕ）和Ａ（＾２２６Ｒａ）／Ａ（＾２３０Ｔｈ）反演判别该岩石曾经历了近代水－岩反应的大致强度和出现,持续时间,这是近十余年     

Distribution of radioactive isotopes in rock and ore of Arkhangelskaya pipe from the Arkhangelsk diamond province

The contents of radioactive elements and the uranium isotopic composition of kimberlite in the Arkhangelskaya pipe at the M.V. Lomonosov deposit and of nearby country rocks have been studied. A surplus of ²³⁴U isotope has been established in rocks from the near-pipe space. The high γ = ²³⁴U/²³⁸U ratio is controlled by the geological structure of the near-pipe space. A nonequilibrium uranium halo reaches two pipe diameters in size and can be regarded as a local ore guide for kimberlite discovery. The rocks in the nearpipe space are also characterized by elevated or anomalous U, Th, and K contents with respect to the background.     

Factors controlling the groundwater transport of U, Th, Ra, and Rn

A model for the groundwater transport of naturally occurring U, Th, Ra, and Rn nuclides in the²³⁸U and²³²Th decay series is discussed. The model developed here takes into account transport by advection and the physico-chemical processes of weathering, decay, α-recoil, and sorption at the water-rock interface. It describes the evolution along a flowline of the activities of the²³⁸U and²³²Th decay series nuclides in groundwater. Simple sets of relationships governing the activities of the various species in solution are derived, and these can be used both to calculate effective retardation factors and to interpret groundwater data. For the activities of each nuclide, a general solution to the transport equation has been obtained, which shows that the activities reach a constant value after a distance ϰ_i, characteristic of each nuclide. Where ϰ_i is much longer than the aquifer length, (for²³⁸U,²³⁴U, and²³²Th), the activities grow linearly with distance. Where gKⁱ is short compared to the aquifer length, (for²³⁴Th,²³⁰Th,²²⁸Th,²²⁸Ra, and²²⁴Ra), the activities rapidly reach a constant or quasi-constant activity value. For²²⁶Ra and²²²Rn, the limiting activity is reached after 1 km. High δ²³⁴U values (proportional to the ratio^ɛ234Th/^W238U) can be obtained through high recoil fraction and/or low weathering rates. The activity ratios²³⁰Th/²³²Th,²²⁸Ra/²²⁶Ra and²²⁴Ra/²²⁶Ra have been considered in the cases where either weathering or recoil is the predominant process of input from the mineral grain. Typical values for weathering rates and recoil fractions for a sandy aquifer indicate that recoil is the dominant process for Th isotopic ratios in the water. Measured data for Ra isotope activity ratios indicate that recoil is the process generally controlling the Ra isotopic composition in water. Higher isotopic ratios can be explained by different desorption kinetics of Ra. However, the model does not provide an explanation for²²⁸Ra/²²⁶Ra and²²⁴Ra/²²⁶Ra activity ratios less than unity. From the model, the highest²²²Rn emanation equals 2ɛ. This is in agreement with the hypothesis that²²²Rn activity can be used as a first approximation for input by recoil (Krishnaswamiet al 1982). However, high²²²Rn emanation cannot be explained by production from the surface layer as formulated in the model. Other possibilities involve models including surface precipitation, where the surface layer is not in steady-state.     

确定砂岩型铀矿矿化地段的铀、钍同位素证据

根据铀、钍同位素地球化学基本原理,对新疆伊梨盆地５１２矿床含矿砂岩的Ｕ、Ｔｈ含量及其＾２３４Ｕ／＾２３８Ｕ、＾２３０Ｔｈ／＾２３２Ｔｈ进行了测试,并在此基础上对含矿砂岩的氧化带、还原带和氧化还原过渡带特征进行了研究。研究表明,与氧化带、还原带相比,氧化－还原过渡带具有较高Ｕ含量和＾２３４Ｕ／＾２３８Ｕ比值,较低Ｔｈ／Ｕ比值;矿石样品中的＾２３４Ｕ／＾２３８Ｕ、＾２３０Ｔｈ／＾２３８Ｕ比值位于过渡带     

Th/U/U and Pa/U ages from a single fossil coral fragment by multi-collector magnetic-sector inductively coupled plasma mass spectrometry

The ²³⁰Th/²³⁴U/²³⁸U age dating of corals via alpha counting or mass spectrometry has significantly contributed to our understanding of sea level, radiocarbon calibration, rates of ocean and climate change, and timing of El Nino, among many applications. Age dating of corals by mass spectrometry is remarkably precise, but many samples exposed to freshwater yield inaccurate ages. The first indication of open-system ²³⁰Th/²³⁴U/²³⁸U ages is elevated ²³⁴U/²³⁸U_initial values, very common in samples older than 100,000 yr. For samples younger than 100,000 yr that have ²³⁴U/²³⁸U_initial values close to seawater, there is a need for age validation. Redundant ²³⁰Th/²³⁴U/²³⁸U and ²³¹Pa/²³⁵U ages in a single fossil coral fragment are possible by Multi-Collector Magnetic Sector Inductively Coupled Plasma Mass Spectrometry (MC-MS-ICPMS) and standard anion exchange column chemistry, modified to permit the separation of uranium, thorium, and protactinium isotopes from a single solution. A high-efficiency nebulizer employed for sample introduction permits the determination of both ²³⁰Th/²³⁴U/²³⁸U and ²³¹Pa/²³⁵U ages in fragments as small as 500 mg. We have obtained excellent agreement between ²³⁰Th/²³⁴U/²³⁸U and ²³¹Pa/²³⁵U ages in Barbados corals (30 ka) and suggest that the methods described in this paper can be used to test the ²³⁰Th/²³⁴U/²³⁸U age accuracy.Separate fractions of U, Th, and Pa are measured by employing a multi-dynamic procedure, whereby ²³⁸U is measured on a Faraday cup simultaneously with all minor isotopes measured with a Daly ion counting detector. The multi-dynamic procedure also permits correcting for both the Daly to Faraday gain and for mass discrimination during sample analyses. The analytical precision of ²³⁰Th/²³⁴U/²³⁸U and ²³¹Pa/²³⁵U dates is generally better than ±0.3% and ±1.5%, respectively (2 Relative Standard deviation [RSD]). Additional errors resulting from uncertainties in the decay constant for ²³¹Pa and from undetermined sources currently limit the ²³¹Pa/²³⁵U age uncertainty to about ±2.5%. U isotope data and ²³⁰Th/²³⁴U/²³⁸U ages agree with National Institute of Standards and Technology (NIST) reference materials and with measurements made by Thermal Ionization Mass Spectrometry (TIMS) in our laboratory.     

Use of 234U/238U disequilibrium in measuring chemical weathering rate of rocks

The rate of chemical weathering of rocks has been determined by using uranium as a natural isotopic tracer. The concentration of uranium and ²³⁴U/²³⁸U ratio in natural waters, rocks, and soils of the Preto river basin (Bahia State, Brazil) was measured by alpha-ray spectroscopy.The activity ratio U234/U238 measured in the various samples indicates the uranium fraction which is dissolved from rocks during the weathering process. The results obtained show that 1 m of rock needs 25,000 yr to be weathered in this region under present climatic conditions.     

Processes controlling 234U and 238U isotope fractionation and helium in the groundwater of the St. Lawrence Lowlands,Quebec: The potential role of natural rock fracturing

The goal of this study is to explain the origin of ²³⁴U–²³⁸U fractionation in groundwater from sedimentary aquifers of the St. Lawrence Lowlands (Quebec, Canada), and its relationship with ³He/⁴He ratios, to gain insight regarding the evolution of groundwater in the region. (²³⁴U/²³⁸U) activity ratios, or (²³⁴U/²³⁸U)_act, were measured in 23 groundwater samples from shallow Quaternary unconsolidated sediments and from the deeper fractured regional aquifer of the Becancour River watershed. The lowest (²³⁴U/²³⁸U)_act, 1.14 ± 0.01, was measured in Ca–HCO₃-type freshwater from the Quaternary Shallower Aquifer, where bulk dissolution of the carbonate allows U to migrate into water with little ²³⁴U–²³⁸U isotopic fractionation. The (²³⁴U/²³⁸U)_act increases to 6.07 ± 0.14 in Na–HCO₃–Cl-type groundwater. Preferential migration of ²³⁴U into water by α-recoil is the underlying process responsible for this isotopic fractionation. An inverse relationship between (²³⁴U/²³⁸U)_act and ³He/⁴He ratios has been observed. This relationship reflects the mixing of newly recharged water, with (²³⁴U/²³⁸U)_act close to the secular equilibrium and containing atmospheric/tritiogenic helium, and mildly-mineralized older water (¹⁴C ages of 6.6 kyrs), with (²³⁴U/²³⁸U)_act of ≥6.07 and large amounts of radiogenic ⁴He, in excess of the steady-state amount produced in situ. The simultaneous fractionation of (²³⁴U/²³⁸U)_act and the addition of excess ⁴He could be locally controlled by stress-induced rock fracturing. This process increases the surface area of the aquifer matrix exposed to pore water, from which produced ⁴He and ²³⁴U can be released by α-recoil and diffusion. This process would also facilitate the release of radiogenic helium at rates greater than those supported by steady-state U–Th production in the rock. Consequently, sources internal to the aquifers could cause the radiogenic ⁴He excesses measured in groundwater.     

Uranium series disequilibrium in young lacustrine sediments from an arid environment at Henkries,Republic of South Africa

Uranium adsorbed on to carbonaceous material and clays, and in minerals (boltwoodite, carnotite, zippeite), is present in a lacustrine deposit from an arid environment of southern Africa. Granites in the area, which may contain up to 50 ppm U₃O₈, are believed to be the original source for the U mineralization. The U is concentrated selectively in certain strata which are characterized by high diatomaceous earth and carbonaceous contents, high moisture contents, low densities, and considerable porosity.Activities of the ²³⁸U series nuclides (²³⁸U, ²³⁴U, ²³⁰Th and ²²⁶Ra) were determined by alpha spectrometry and indicate: (1) the deposit is geologically young; and (2) disequilibrium among nuclides in the U series is prevalent at present. Because of this disequilibrium between U and its daughter products, there is no correlation between U₃O₈ determined by chemical analysis and that inferred from radiometric methods based on gamma ray spectrometry (eU₃O₈); in some cases chemical U₃O₈ is higher than eU₃O₈ inferred from gamma ray spectrometry whereas in other cases the reverse is true. In order to evaluate the deposit, all drill core, and trench and pit samples were analysed by X-ray fluorescence. At this time, movement of U and its daughter elements appears to be an active process, particularly in those layers which are porous and have a high moisture content. Paleoclimatic studies have shown that alternating pluvial and arid periods existed in the last 40 000 yr in southern Africa. These would result in fluctuations in the water table sufficient to cause selective relative migrations of ²³⁸U series nuclides thus accounting for at least some of the observed disequilibrium.     

Budgets and behaviors of uranium and thorium series isotopes in Santa Monica Basin sediments

Nine natural decay-series isotopes were measured in six box cores collected from a transect across the Santa Monica Basin. The ²¹⁰Pb-derived sedimentation rate decreases from ~80 mg/cm²-yr at the slope to ~20 mg/cm²-yr in the deep central basin. Sediment mixing prevails in sites underlying oxic waters, but is subdued in the anoxic deep basin below the sill depth. Uranium contents in sediments are controlled by levels of authigenic U, which are higher in the more reduced condition in the deep basin. Most of the authigenic U results from precipitation within the sediments.The ²³²Th-²²⁸Th disequilibrium in sediments indicates that ²²⁸Ra is lost from the sediments from a depth of ~ 10 cm upward. Modelling the distribution of excess ²²⁸Th and ²³⁴Th in the surficial layers of the deep basin sediments results in a mean sediment mixing coefficient of 0.2 cm²/yr and a sedimentation rate close to that based on ²¹⁰Pb. There is no evidence of changing sedimentation rate in the central basin during the past century. Fluxes of excess ²¹⁰Pb, ²³⁰Th and ²³¹Pa to the central Santa Monica Basin sediments are much higher than what can be predicted from local supply. Advective input of open ocean waters coupled with enhanced scavenging of these reactive nuclides at the ocean margin is considered to be the primary cause.     

高分辨电感耦合等离子体质谱法测定铀矿石样品中234U/238U、230Th/232Th和228Ra/226Ra同位素比值 

采用氢氟酸-硝酸-盐酸混合酸密闭消解含铀矿石样品,用阴离子交换树脂、阳离子交换树脂和锶特效树脂逐级分离富集铀、钍和镭。使用高分辨电感耦合等离子体质谱(HR-ICPMS)测定分离纯化液中234U/238U2、30Th/232Th和228Ra/226Ra同位素。比值的测量精密度取决于比值的大小和对应核素浓度的大小。对质量浓度为10 ng/mL天然铀测量液,234U/238U的测量精密度优于1.2%;对230Th质量浓度为0.6ng/mL且230Th和232Th质量浓度接近的测量液,230Th/232Th的测量精密度为1.2%;对228Ra质量浓度为0.48 pg/mL且228Ra和226Ra质量浓度接近的测量液,228Ra/226Ra的测量精密度为4.0%。     

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.     

Uranium geochemistry and dating of Pacific island apatite

Uranium-series disequilibrium dating of island phosphate deposits is evaluated in terms of known associated coral ages, uranium geochemistry, and stratigraphic sequences as well as the concordance between the geochronometers ²³⁴U/²³⁸U, ²³⁰Th/²³⁴U and ²²⁶Ra/²³⁸U. U(VI) is the predominant oxidation state of uranium in island phosphorites and by analogy to the youngest surficial deposits, most of the uranium initially bound is in the form of U(VI) sorbed by surfaces from seawater. Insular deposits contain more organic matter than even very young ocean floor samples and this leads to a greater probability of reduction of available recoil uranium than occurs in marine deposits. As a consequence, R(VI) ? R(T) ? R(VI), where R represents the ²³⁴U/²³⁸U activity ratio. This situation is completely opposite from that observed for marine-origin phosphorites. We determined that a fraction of U(VI) in ancient insular phosphorites is very labile and lost to alkaline carbonate solutions with a uranium activity ratio even more depleted in ²³⁴U than the bulk R(VI).Most younger samples appear to have no more discordance between ²³⁴U/²³⁸U, ²³⁰Th/²³⁴U and ²²⁶Ra/²³⁸U than marine phosphorites of similar apparent age. Young, surficial atoll-rim apatite cements and unconsolidated phosphorites date in the range of 1500–8000 years B.P., consistent with the concept of partial submergence of low-lying coral islands prior to 2000 years B.P. Sub-surficial samples in the same environment date older at about 20,000 years B.P. Violation of the closed system assumption occurs in at least 6 out of 13 ancient (> 800,000 year) samples. Uranium-series disequilibrium dating of insular apatite shows some promise as a recorder of climatic/sea level events, but the assumptions necessary for valid ages must be carefully evaluated for each occurrence.     

Uranium series disequilibrium in a young surficial uranium deposit,northeastern Washington,U.S.A.

A recently discovered ore-grade accumulation of U in organic-rich sediments of late Quaternary age provides an opportunity for studying the early association of U, U-daughters, and organic matter in a natural setting. The U occurs in valley-fill sediments of peat, peaty clay, silt, and sand along the north fork of Flodelle Creek, Stevens County, Washington. Radiometric techniques (delayed neutron, high-resolution gamma-ray spectrometry, thin-source alpha spectrometry) were employed to determine the abundance and distribution of U-series nuclides, the extent of secular equilibrium within the U decay series, and the apparent U-series ages of U incorporation.Sixteen lithologically distinct intervals were sampled from a 292 cm core. Uranium contents range from 140 to 2790 ppm and are positively correlated with organic contents. Measured alpha activity ratios of ²³⁴U/²³⁸U (1.31–1.38) are very similar to those reported in coexisting waters, suggesting a rather constant isotopic composition of introduced U. Much lower Th contents of <10–40 ppm are controlled by the type and abundance of silicate detritus. The youth of the host sediments (<15 000 a) and the paucity of associated radioactivity suggested large excesses of U relative to radioactive daughters and such excesses were observed, particularly in the shallowest intervals. Apparent ages of U emplacement determined by the (alpha) activity ratio of ²³⁰Th daughter to ²³⁴U parent show a general increase with depth and fair agreement with estimated depositional ages. This observation suggests dominantly syndepositional or early post depositional emplacement of U followed by decay-generated buildup of ²³⁰Th daughter with time. However, interval by interval comparisons of the relative abundances of other daughters, particularly ²²⁶Ra and ²¹⁰Pb, indicate variability caused by processes other than closed-system growth and decay, probably because chemically diverse daughters that are decay-generated in situ have differing mobilities and because upwelling ground water continuously adds more U and minor amounts of daughters. If ²³⁰Th is considered the least susceptible to these modifications, the data suggest some addition of ²³⁴U in the deepest intervals and some loss of ²²⁶Ra and/or gain of ²²²Rn throughout the studied core.     

Variability in the uranium isotopic composition of the oceans over glacial-interglacial timescales

Uranium-series mass spectrometric analyses of corals from the uplifted last glacial terraces at Huon Peninsula, Papua New Guinea, that grew from 50,000 years ago to 30,000 years ago show systematically low values of ²³⁴U/²³⁸U, at the time of coral growth, compared with modern corals. When combined with coral data from other studies a systematic trend emerges indicating shifts in the ²³⁴U/²³⁸U ratio at times of major glacial-interglacial transitions that involve large variations in sea-levels. From last glacial to Holocene, the rate of change in δ²³⁴U is approximately 1‰ per thousand years. The variations in the U budget of the oceans appear to be due to accumulation of excess ²³⁴U in near shore areas in anoxic and suboxic sediments, in salt marshes and mangroves, in estuaries, and in continental margins during periods of warm climate and high sea-levels. These near-shore areas are exposed during periods of low sea level resulting in rapid oxidation of U into highly soluble phases. The subsequent release of ²³⁴U-enriched uranium into the oceans occurs over a sustained period, in step with rising sea-levels.     

TIMS测定铀矿石样品中^234U/^238U、^230Th/^232Th、^228Ra/^226Ra的方法研究

研究了TIMS测定铀矿石样品中234U/238U、230Th/232Th、228Ra/226Ra的方法。建立了铀矿石密闭混酸一次溶样的方法和采用阴离子、阳离子和Sr特效树脂逐级离子交换分离纯化U、Th和Ra的流程,满足了TIMS测量要求。测定结果表明：100～1000 ng的天然铀中234U/238U,其测量精密度从静态多接收的2.34%提高到动态多接收的0.47%;对230Th与232Th丰度接近、质量为1μg左右的钍,采用三带点样技术和法拉第多接收技术测定230Th/232Th,其内精度平均值为0.0048%,外精度为0.028%;采用单带加钽发射剂,ETP跳峰测定50～100 fg镭-228稀释剂中的228Ra/226Ra,其内精度小于0.10%,外精度小于0.20%。比较TIMS和HR-ICP-MS、α能谱法测定234U/238U、230Th/232Th、228Ra/226Ra结果,三者结果相吻合。TIMS测量法样品用量少、快速、准确、精密度高,是U、Th、Ra同位素比值测定方法的又一补充。