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1.
Preservation of particulate non-lithogenic uranium in marine sediments   总被引：1，自引：0，他引：1  
Particulate non-lithogenic uranium (PNU), excess U above detrital background levels found in marine particulate matter, is formed in surface waters throughout the ocean. Previous studies have shown that PNU is regenerated completely prior to burial of particles in sediments within well-oxygenated open-ocean regions. However, the fate of PNU has never been examined in ocean margin regions or in anoxic basins. Here we evaluate the preservation of PNU in ocean margin sediments and within semi-enclosed basins using samples from sediment traps deployed at multiple depths and surface sediments. Organic carbon fluxes at the sediment trap locations ranged from 0.1 to 4.3 g/cm2 kyr, while the dissolved oxygen concentration in the water column ranged from <3 μM to ∼ 270 μM. Preservation of PNU increases with decreasing dissolved oxygen concentration, approaching 100% preservation at oxygen concentration < 25 μM. PNU contributes as much as 40 to 70% of the total authigenic U in sediments in the Santa Barbara Basin and seasonally anoxic Saanich Inlet, and some 10% to 50% of the total authigenic U in sediments off the central California Margin.  相似文献   

2.
Pore water and solid phase data for redox-sensitive metals (Mn, Fe, V, Mo and U) were collected on a transect across the Peru upwelling area (11°S) at water depths between 78 and 2025 m and bottom water oxygen concentrations ranging from ∼0 to 93 μM. By comparing authigenic mass accumulation rates and diffusive benthic fluxes, we evaluate the respective mechanisms of trace metal accumulation, retention and remobilization across the oxygen minimum zone (OMZ) and with respect to oxygen fluctuations in the water column related to the El Niño Southern Oscillation (ENSO).Sediments within the permanent OMZ are characterized by diffusive uptake and authigenic fixation of U, V and Mo as well as diffusive loss of Mn and Fe across the benthic boundary. Some of the dissolved Mn and Fe in the water column re-precipitate at the oxycline and shuttle particle-reactive trace metals to the sediment surface at the lower and upper boundary of the OMZ. At the lower boundary, pore waters are not sufficiently sulfidic as to enable an efficient authigenic V and Mo fixation. As a consequence, sediments below the OMZ are preferentially enriched in U which is delivered via both in situ precipitation and lateral supply of U-rich phosphorites from further upslope. Trace metal cycling on the Peruvian shelf is strongly affected by ENSO-related oxygen fluctuations in bottom water. During periods of shelf oxygenation, surface sediments receive particulate V and Mo with metal (oxyhydr)oxides that derive from both terrigenous sources and precipitation at the retreating oxycline. After the recurrence of anoxic conditions, metal (oxyhydr)oxides are reductively dissolved and the hereby liberated V and Mo are authigenically removed. This alternation between supply of particle-reactive trace metals during oxic periods and fixation during anoxic periods leads to a preferential accumulation of V and Mo compared to U on the Peruvian shelf. The decoupling of V, Mo and U accumulation is further accentuated by the varying susceptibility to re-oxidation of the different authigenic metal phases. While authigenic U and V are readily re-oxidized and recycled during periods of shelf oxygenation, the sequestration of Mo by authigenic pyrite is favored by the transient occurrence of oxidizing conditions.Our findings reveal that redox-sensitive trace metals respond in specific manner to short-term oxygen fluctuations in the water column. The relative enrichment patterns identified might be useful for the reconstruction of past OMZ extension and large-scale redox oscillations in the geological record.  相似文献   

3.
Solid phase P speciation has been determined in sediments from a transect across the central section of the continental shelf and slope of the Great Barrier Reef (GBR) lagoon. This region is characterized by a gradient of riverine aluminosilicate clay and silt nearshore, seawards of which biogenic carbonate sediment predominates. Phosphorus speciation results show large variations along this transect. Organic P and authigenic (apatite) P are the major chemical forms of phosphorus in the central GBR continental shelf sediments. Post-depositional reorganization of P was also observed, converting organic P and iron bound P (Fe-P) to authigenic (apatite) P. Phosphorus burial rate was estimated from measurements of total P concentration and excess 210Pb sediment mass accumulation rates. Burial efficiency varies significantly over the shelf. Inshore areas showed significant P remobilization from sediments to the water column (up to ∼50%). The mid and the outer shelf showed little evidence for remobilization (except for coral reef platform sediments), with more of the sediment P being in the less reactive authigenic apatite phases. An appreciable fraction of this non-labile authigenic apatite phase was identified as fish bone. P sources and sinks over the central part of the GBR shelf were quantified using a mass balance approach. This showed that Coral Sea shelf edge upwelling events are essential to satisfy the large P nutrient demand of the whole GBR lagoon. P inputs due to upwelling events were greater than those contributed by local rivers over an average year.  相似文献   

4.
Iodometric titration of deep sea sediment from cores at MANOP sites M and H indicate a particulate Mn oxidation state between 3.3 and 3.9 in the top 5 cm. Results from site H show a minimum in the Mn oxidation state at 1.5 cm depth indicating Mn reduction is occurring above the zone of pore water Mn oxidation. Using a simple box model, the rate of reduction is calculated to be 19 mg/cm2 kyr ? 77 mg/cm2 kyr, at least 5 times the flux of Mn to nodules in this region. Although no Mn oxidation state minimum is observed in site M sediments, oxic reduction is inferred from a particulate mass balance, indicating that a large fraction of the Mn rain to this site is not preserved in the sediments and must be remobilized. We suggest that the process of reduction in oxic or suboxic environments near the sediment-water interface may be an important mechanism controlling the concentration of Mn in sediments and provides a mechanism for supplying diagenetic Mn to the nodules at site H.  相似文献   

5.
This research tests the hypothesis that trace metals respond to the extent of reducing conditions in a predictable way. We describe pore water and sediment measurements of iron (Fe), manganese (Mn), vanadium (V), uranium (U), rhenium (Re), and molybdenum (Mo) along a transect off Washington State (USA). Sediments become less reducing away from the continent, and the stations have a range of oxygen penetration depths (depth to unmeasurable O2 concentration) varying from a few millimeters to five centimeters. When oxygen penetrates ∼1 cm or less, Fe is reduced in the pore waters but reoxidized near the sediment-water interface, preventing a flux of Fe2+ to overlying waters, whereas Mn oxides are reduced and Mn2+ diffuses to overlying waters. Both Re and U authigenically accumulate in sediments. Only at the most reducing location, where the oxygen penetrates 0.3 cm below the sediment-water interface, does the surface 30 cm of sediments become reducing enough to authigenically accumulate Mo.Stations in close proximity to the Juan de Fuca Ridge crest are enriched in Mn and Fe from hydrothermal plume processes. Both V and Mo clearly associate with Mn cycling, whereas U may be associating with either Mn oxides and/or Fe oxyhydroxides. Rhenium is uncomplicated by adsorption to Mn oxides and/or Fe oxyhydroxides, and Re accumulation in sediments appears to be due solely to the extent of reducing conditions. Therefore, authigenic sediment Re enrichment appears to be the best indicator for intermediate reducing conditions, where oxygen penetrates less than ∼1 cm below the sediment-water interface, when coupled with negligible authigenic Mo enrichment.  相似文献   

6.
We have measured U in benthic incubation chambers, sediment pore waters, and in sediments along the California continental margin. Sedimentary U uptake rates, based on a combination of sediment pore water profiles and benthic incubation chambers, generally agree with those predicted from sediment accumulation rate data. This agreement supports the view that most of the continental margin sedimentary U is delivered by diffusion across the seawater-sediment boundary. The average rate of authigenic U accumulation for all the sites examined here is ∼−0.2 nmol cm-2 y-1, which is consistent with published global estimates of sedimentary U uptake. In addition, the accumulation rate of U in sediments exhibits a nonlinear relationship with the oxygen penetration depth and a linear relationship with the organic carbon rain rate. These relationships highlight the potential utility for the U accumulation rate as a proxy for these processes.  相似文献   

7.
We measured U in sediments (both pore waters and solid phase) from three locations on the middle Atlantic Bight (MAB) from the eastern margin of the United States: a northern location on the continental shelf off Massachusetts (OC426, 75 m water depth), and two southern locations off North Carolina (EN433-1, 647 m water depth and EN433-2, 2648 m water depth). These sediments underlie high oxygen bottom waters (250-270 μM), but become reducing below the sediment-water interface due to the relatively high organic carbon oxidation rates in sediments (EN433-1: 212 μmol C/cm2/y; OC426: 120 ± 10 μmol C/cm2/y; EN433-2: 33 μmol C/cm2/y). Pore water oxygen goes to zero by 1.4-1.5 cm at EN433-1 and OC426 and slightly deeper oxygen penetration depths were measured at EN433-2 (∼4 cm).All of the pore water profiles show removal of U from pore waters. Calculated pore water fluxes are greatest at EN433-1 (0.66 ± 0.08 nmol/cm2/y) and less at EN433-2 and OC426 (0.24 ± 0.05 and 0.13 ± 0.05 nmol/cm2/y, respectively). Solid phase profiles show authigenic U enrichment in sediments from all three locations. The average authigenic U concentrations are greater at EN433-1 and OC426 (5.8 ± 0.7 nmol/g and 5.4 ± 0.2 nmol/g, respectively) relative to EN433-2 (4.1 ± 0.8 nmol/g). This progression is consistent with their relative ordering of ‘reduction intensity’, with greatest reducing conditions in sediments from EN433-1, less at OC426 and least at EN433-2. The authigenic U accumulation rate is largest at EN433-1 (0.47 ± 0.05 nmol/cm2/y), but the average among the three sites on the MAB is ∼0.2 nmol/cm2/y. Pore water profiles suggest diffusive fluxes across the sediment-water interface that are 1.4-1.7 times greater than authigenic accumulation rates at EN433-1 and EN433-2. These differences are consistent with oxidation and loss of U from the solid phase via irrigation and/or bioturbation, which may compromise the sequestration of U in continental margin sediments that underlie bottom waters with high oxygen concentrations.Previous literature compilations that include data exclusively from locations where [O2]bw < 150 μM suggest compelling correlations between authigenic U accumulation and organic carbon flux to sediments or organic carbon burial rate. Sediments that underlie waters with high [O2]bw have lower authigenic U accumulation rates than would be predicted from relationships developed from results that include locations where [O2]bw < 150 μM.  相似文献   

8.
Deltaic environments are commonly assumed to be relatively minor sites of biogenic silica burial because of the small quantities of opaline silica detected by most operational analytical techniques. Rapid conversion of biogenic silica into authigenic silicates is also often discounted as a significant control on oceanic silica budgets. A variety of evidence for extensive early diagenetic alteration of biogenic silica in rapidly accumulating Amazon delta sediments indicates that both of these general assumptions are unjustified. Apparent lack of significant biogenic silica storage in deltaic environments, particularly in the tropics, may be largely an artifact of operational definitions that do not include early diagenetic products of biogenic silica. Biogenic silica particles buried in suboxic Amazon delta deposits can be unaltered, partially dissolved, covered with aluminosilicate or metal-rich coatings, or completely reconstituted into authigenic K-Fe-rich aluminosilicate minerals. Pore water (K, Mg, F, Si) and solid-phase distributions, direct observations of particles, laboratory experiments, and depositional context indicate that authigenic clays form rapidly (<1 yr) in the seasonally reworked surface layer (∼ 0.5-2 m) of the delta topset and are disseminated during sediment remobilization. Fe, Al-oxide rich debris derived from the tropical drainage basin is an abundant reactant, and thus the supply of biogenic silica is a major control on the amount of clay formed.The mild 1% Na2CO3 alkaline leach procedure commonly used to estimate biogenic silica was modified to include an initial mild leach step with 0.1N HCl to remove metal oxide coatings and to activate poorly crystalline authigenic phases for alkaline dissolution. Well-crystallized clays are not significantly affected by this modification nor is bulk Amazon River bed sediment. The two-step procedure indicates that ∼90% of the biogenic silica originally present in deposits is converted to clay or otherwise altered, raising the effective quantity of biogenic silica stored from ∼33 to ∼296 μmol Si g−1 (∼1.8% SiO2). Biogenic Si stored in the delta increases away from the river mouth, across shelf and along the dispersal system where primary production is highest. The K/Si ratio of labile authigenic material is ∼0.19 mol mol−1, far higher than Amazon River suspended matter (∼0.07 mol mol−1). Diagenetic models indicate formation rates in the mobile sediment layer of ∼2.8 μmol K g−1 yr−1 (∼16 μmol Si g−1 yr−1). Inclusion of authigenic alteration products of biogenic silica in estimates of reactive Si burial increases the deltaic storage of riverine Si to ∼22% of the Amazon River input. The rapid formation of aluminosilicates from biogenic SiO2, seawater solutes, and remobilized Fe, Al-oxides represents a form of reverse weathering. Rapid reverse weathering reactions in tropical muds and deltaic deposits, the largest sediment depocenters on Earth, confirms the general importance of these processes in oceanic elemental cycles.  相似文献   

9.
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10.
Late Weichselian and Holocene sediment flux and sedimentation rates in a continental‐shelf trough, Andfjord, and its inshore continuation, Vågsfjord, North Norway, have been analysed. The study is based on sediment cores and high‐resolution acoustic data. Andfjord was deglaciated between 14.6 and 13 14C kyr BP (17.5 and 15.6 calibrated (cal.) kyr BP), the Vågsfjord basin before 12.5 14C kyr BP (14.7 cal. kyr BP), and the heads of the inner tributary fjords about 9.7 14C kyr BP (11.2 cal. kyr BP). In Andfjord, five seismostratigraphical units are correlated to a radiocarbon dated lithostratigraphy. Three seismostratigraphical units are recognised in Vågsfjord. A total volume of 23 km3 post‐glacial glacimarine and marine sediments was mapped in the study area, of which 80% are of Late Weichselian origin. Sedimentation rates in outer Andfjord indicate reduced sediment accumulation with increasing distance from the ice margin. The Late Weichselian sediment flux and sedimentation rates are significantly higher in Vågsfjord than Andfjord. Basin morphology, the position of the ice front and the timing of deglaciation are assumed to be the reasons for this. Late Weichselian sedimentation rates in Andfjord and Vågsfjord are comparable to modern subpolar glacimarine environments of Greenland, Baffin Island and Spitsbergen. Downwasting of the Fennoscandian Ice Sheet, and winnowing of the banks owing to the full introduction of the Norwegian Current, caused very high sedimentation rates in parts of the Andfjord trough at the Late Weichselian–Holocene boundary. Holocene sediment flux and sedimentation rates in Andfjord are about half the amount found in Vågsfjord, and about one‐tenth the amount of Late Weichselian values. A strong bottom current system, established at the Late Weichselian–Holocene boundary, caused erosion of the Late Weichselian sediments and an asymmetric Holocene sediment distribution. Copyright © 2002 John Wiley & Sons, Ltd.  相似文献   

11.
Sediments in Lake Qinghai archive important information about past environmental changes. In order to faithfully interpret the sediment records and constrain the elemental cycles, it is critical to trace various sources of sediments in the lake. The results show that the elemental input–output budgets are imbalanced for most major elements between riverine fluxes and mass accumulation rate (MAR) of Lake Qinghai sediments. A realistic model must include contributions of dry/wet atmospheric deposition that allow the major element mass balance for the lake to be defined. The budget estimation is based on mass balances of Si and Al, which are relatively immobile and carried to the lake via particulate forms. Estimated annual budget of dry atmospheric deposition is ∼1.3 ± 0.3 × 103 kt/a (accounting for ∼65% of the total inputs) to the lake sediments, assuming local loess within the catchment as a candidate for dry atmospheric deposition to the lake. The resultant flux of 300 ± 45 g/m2/a falls within the flux average of the desert area (400 g/m2/a) and the loess plateau (250 g/m2/a), consistent with the geographical setting of Lake Qinghai. The role of atmospheric deposition would be more significant if wet deposition via rainfall and snow were taken into account. This highlights the potential importance of dust as a significant source for sediment preservation flux for other catchments worldwide. The results also indicate that nearly all Ca input was preserved in the lake sediments under modern conditions, consistent with Ca2+ supersaturation of the lake water.  相似文献   

12.
Late Cenozoic sedimentation and metal deposition in the North Pacific   总被引：1，自引：0，他引：1  
Similar major chemical variations in cores from three sites across a wide area of the North Pacific are modeled by coupling the vertical and horizontal motions of the Pacific plate with a constant authigenic flux of elements into the sediments. Superimposed over this flux is an input of detrital material of relatively constant chemical composition. The major features of sediment chemistry of cores from the North Pacific apparently vary in a fairly uniform and systematic manner, and these variations are consistent with Cenozoic plate movement. Elements with a significant authigenic component (e.g., Mn, Co, Cu, Ni) display high concentrations at depth in cores that correspond to the period when the seafloor, while under the low-productivity, subtropical gyre of the N. Pacific, accumulated sediment at an extremely slow rate (~1 mm/kyr). These concentrations were diluted when the sites experienced an increase in the eolian mass accumulation rate first brought about by migration into the influence of the westerlies and then, dominantly, by the huge input of wind-blown detritus which corresponded to the onset of Northern Hemisphere glaciation. A comparison of 10Be profiles to the profiles of metal concentrations is used to reveal the occurrence of haituses in the sediment column over the past 8 m.y.  相似文献   

13.
Many (bio)geochemical processes that bring about changes in sediment chemistry normally begin at the sediment-water interface, continue at depth within the sediment column and may persist throughout the lifetime of sediments. Because of the differential reactivity of sedimentary phosphate phases in response to diagenesis, dissolution/precipitation and biological cycling, the oxygen isotope ratios of phosphate (δ18OP) can carry a distinct signature of these processes, as well as inform on the origin of specific P phases. Here, we present results of sequential sediment extraction (SEDEX) analyses combined with δ18OP measurements, aimed at characterizing authigenic and detrital phosphate phases in continental margin sediments from three sites (Sites 1227, 1228 and 1229) along the Peru Margin collected during ODP Leg 201. Our results show that the amount of P in different reservoirs varies significantly in the upper 50 m of the sediment column, but with a consistent pattern, for example, detrital P is highest in siliciclastic-rich layers. The δ18OP values of authigenic phosphate vary between 20.2‰ and 24.8‰ and can be classified into at least two major groups: authigenic phosphate precipitated at/near the sediment-water interface in equilibrium with paleo-water oxygen isotope ratios (δ18Ow) and temperature, and phosphate derived from hydrolysis of organic matter (Porg) with subsequent incomplete to complete re-equlibration and precipitated deeper in the sediments column. The δ18OP values of detrital phosphate, which vary from 7.7-15.4‰, suggest two possible terrigenous sources and their mixtures in different proportions: phosphate from igneous/metamorphic rocks and phosphate precipitated in source regions in equilibrium with δ18Ow of meteoric water. More importantly, original isotopic compositions of at least one phase of authigenic phosphates and all detrital phosphates are not altered by diagenesis and other biogeochemical changes within the sediment column. These findings help to understand the origin and provenance of P phases and paleoenvironmental conditions at/near the sediment-water interface, and to infer post-depositional activities within the sediment column.  相似文献   

14.
Seep‐carbonates (13C‐depleted) are present at different levels within the Miocene terrigenous succession of Deruta (Marnoso‐arenacea Formation, central Italy); they are associated with pebbly sandstones and conglomerates in a tectonically active fan‐delta slope depositional system. Most of these seep‐carbonates are included in slide/slump horizons as scattered blocks. The occurrence of seep‐carbonates is clear evidence of the flow of methane‐rich fluids pervading the sediments. Fluids, probably of biogenic origin, may have reached the sea‐bottom through thrust faults and selectively infiltrated the more permeable coarse‐grained horizons deposited along the slope. Different stages of fluid emissions are documented: slow flux stage, corresponding to the development of large carbonate bodies and dense chemosynthetic communities; and fast fluid flow associated with intense carbonate brecciation, pipes and veins. Large amounts of authigenic carbonates are reworked by slope failures triggered by tectonics and fluids reducing sediment strength; in situ cementation of slide blocks may also have occurred due to remobilization of methane‐rich fluids by mass‐wasting processes.  相似文献   

15.
The sediments of the Madeira Abyssal Plain, east of Great Meteor Seamount, are dominated by distal turbidite deposition. While the turbidites exhibit a wide compositional range (25–80% CaCO3), individual examples can be correlated over a wide area and are relatively homogenous. Organic C oxidation, by bottom water oxygen, proceeds from the turbidite tops downwards after emplacement in pelagic conditions, and the progress of this oxidation front is marked by a sharp colour contrast in the sediments (Wilsonet al., 1985). In turbidites with Corg ? 0.5%, redistribution of authigenic U occurs to form a concentration peak (4–9 ppm U), just below the oxidation front or colour change. Several tens μg U/cm2 may be mobilised, and in all examples studied ?60% of the remobilised U is relocated into the peak. Following burial by subsequent turbidites, such U concentration peaks are persistent as relict indicators of their extinct oxidation fronts for at least 2 × 105 years. In the case of thin turbidites where labile Corg is almost exhausted, the U peaks may be located in underlying sedimentary units because of their relationship to the oxidation front. A redox mechanism for U peak formation is suggested from these data rather than a complexation with organic matter.  相似文献   

16.
A new technique for the determination of uranium and thorium in lacustrine sediments is based on non-destructive synchrotron radiation X-ray fluorescence analysis (SR-XRF) of sediment samples using monochromatic beams of different energies as excitation sources, with the recording and subsequent iterative processing of the X-ray fluorescence spectra. The technique has a multielement capability and enables fast, simultaneous analysis of a few tens of elements. The proposed SR-XRF technique was tested against INAA and ICP-MS methods and showed a number of advantages with a generally good correlation of results by the three methods. Uranium and Th profiles have been measured at a time resolution of 2 kyr in a drill core (BDP-96) from Lake Baikal bottom sediments deposited between 780 and 40 kyr B P. During this time span, peaks in the U and U/Th concentration marked warm climates. Oscillations of U and U/Th in Baikal bottom sediments during the Brunhes chron reflect climate-induced global change in the volume of polar ice, controlled by long-term cyclicity of the Earths orbital parameters. The response of these warm periods is similar to that observed earlier in shorter cores that span the two last interglacials (220-0 kyr BP).  相似文献   

17.
Time-resolved U(VI) laser fluorescence spectra (TRLFS) were recorded for a series of natural uranium-silicate minerals including boltwoodite, uranophane, soddyite, kasolite, sklodowskite, cuprosklodowskite, haiweeite, and weeksite, a synthetic boltwoodite, and four U(VI)-contaminated Hanford vadose zone sediments. Lowering the sample temperature from RT to ∼ 5.5 K significantly enhanced the fluorescence intensity and spectral resolution of both the minerals and sediments, offering improved possibilities for identifying uranyl species in environmental samples. At 5.5 K, all of the uranyl silicates showed unique, well-resolved fluorescence spectra. The symmetric O = U = O stretching frequency, as determined from the peak spacing of the vibronic bands in the emission spectra, were between 705 to 823 cm−1 for the uranyl silicates. These were lower than those reported for uranyl phosphate, carbonate, or oxy-hydroxides. The fluorescence emission spectra of all four sediment samples were similar to each other. Their spectra shifted minimally at different time delays or upon contact with basic Na/Ca-carbonate electrolyte solutions that dissolved up to 60% of the precipitated U(VI) pool. The well-resolved vibronic peaks in the fluorescence spectra of the sediments indicated that the major fluorescence species was a crystalline uranyl mineral phase, while the peak spacing of the vibronic bands pointed to the likely presence of uranyl silicate. Although an exact match was not found between the U(VI) fluorescence spectra of the sediments with that of any individual uranyl silicates, the major spectral characteristics indicated that the sediment U(VI) was a uranophane-type solid (uranophane, boltwoodite) or soddyite, as was concluded from microprobe, EXAFS, and solubility analyses.  相似文献   

18.
Analyses for silica in the interstitial water of five cores from the southeast Pacific are presented. Silica is enriched in these interstitial waters resulting in a vertical flux of silica of between 10 and 50 μmol cm?2 yr?1 from the sediment into the overlaying seawater. This flux is generated by the dissolution of biogenic silica, the dissolution of which is increased in areas of bottom water turbulence. The Si, Al and calculated opal (Leinen, 1977) contents of the bulk sediment of these cores are also presented. Small scale variations over depth intervals of tens of centimetres are present as a result of chaning conditions of sedimentation.  相似文献   

19.
《Geochimica et cosmochimica acta》1999,63(11-12):1735-1750
We analyzed the redox sensitive elements V, Mo, U, Re and Cd in surface sediments from the Northwest African margin, the U.S. Northwest margin and the Arabian Sea to determine their response under a range of redox conditions. Where oxygen penetrates 1 cm or less into the sediments, Mo and V diffuse to the overlying water as Mn is reduced and remobilized. Authigenic enrichments of U, Re and Cd are evident under these redox conditions. With the onset of sulfate reduction, all of the metals accumulate authigenically with Re being by far the most enriched. General trends in authigenic metal accumulation are described by calculating authigenic fluxes for the 3 main redox regimes: oxic, reducing where oxygen penetrates ≤1 cm, and anoxic conditions. Using a simple diagenesis model and global estimates of organic carbon rain rate and bottom water oxygen concentrations, we calculate the area of sediments below 1000 m water depth in which oxygen penetration is ≤1 cm to be 4% of the ocean floor. We conclude that sediments where oxygen penetrates ≤1 cm release Mn, V and Mo to seawater at rates of 140%–260%, 60%–150% and 5%–10% of their respective riverine fluxes, using the authigenic metal concentrations and accumulation rates from this work and other literature. These sediments are sinks for Re, Cd and U, with burial fluxes of 70%–140%, 30%–80% and 20%–40%, respectively, of their dissolved riverine inputs. We modeled the sensitivity of the response of seawater Re, Cd and V concentrations to changes in the area of reducing sediments where oxygen penetrates ≤1 cm. Our analysis suggests a negligible change in seawater Re concentration, whereas seawater concentrations of Cd and V could have decreased and increased, respectively, by 5%–10% over 20 kyr if the area of reducing sediments increased by a factor of 2 and by 10%–20% if the area increased by a factor of 3. The concentration variations for a factor of 2 increase in the area of reducing sediments are at about the level of uncertainty of Cd/Ca and V/Ca ratios observed in foraminifera shells over the last 40 kyr. This implies that the area of reducing sediments in the ocean deeper than 1000 m (4%) has not been greater than twice the present value in the recent past.  相似文献   

20.
Uranium geochemistry has been investigated in three acid lakes located on the Canadian Shield and one circumneutral lake in the Appalachian Region of Eastern Canada. In all Shield lakes, dissolved U concentrations were higher in the porewater than in the overlying water. In one of them, whose hypolimnion is perennially oxic, U released to porewater at depths of Fe remobilization was removed from the porewater at depths of Fe oxyhydroxides precipitation; these similarities in the U and Fe profiles indicate that part of the U becomes associated to Fe oxyhydroxides. The dissolved U and Fe profiles in the other two Shield lakes, whose hypolimnions were anoxic when sampled, did not show any significant recycling of these elements in the vicinity of the sediment-water interface and both elements diffused from the sediment to the overlying water. In contrast, in the Appalachian Lake, dissolved U concentrations were higher in the overlying water than in porewater, strongly decreased at the vicinity of the sediment-water interface and then remained relatively constant with sediment depth. Diagenetic modeling of the porewater U profiles, assuming steady-state, reveals that authigenic U always represented ?3% of the total U concentration in the sediments of all lakes. This observation indicates that diagenetic reactions involving U are not quantitatively important and that most of the U was delivered to the sediments at our study sites as particulate U and not through diffusion across the sediment-water interface, as is seen in continental margin sediments. Comparison of the U:Corg and U:Fe molar ratios in diagenetic material collected across the sediment-water interface with Teflon sheets and in surface sediments (0-0.5 cm) of the lake having a perennially oxic hypolimnion suggest that solid phase U was mainly bound to organic matter originating from the watershed; a strong statistical correlation between sediment non-lithogenic U and Corg in the Appalachian Lake supports this contention. Thermodynamic calculations of saturation states suggest that dissolved U was not removed from porewater through precipitation of UO2(s), U3O7(s) and U3O8(s) as previously proposed in the literature.  相似文献   

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