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1.
Recent Lake Tanganyika Hg deposition records were derived using 14C and excess 210Pb geochronometers in sediment cores collected from two contrasting depositional environments: the Kalya Platform, located mid-lake and more removed from watershed impacts, and the Nyasanga/Kahama River delta region, located close to the lake’s shoreline north of Kigoma. At the Kalya Platform area, pre-industrial Hg concentrations are 23 ± 0.2 ng/g, increasing to 74 ng/g in modern surface sediment, and the Hg accumulation rate has increased from 1.0 to 7.2 μg/m2/a from pre-industrial to present, which overall represents a 6-fold increase in Hg concentration and accumulation. At the Nyasanga/Kahama delta region, pre-industrial Hg concentrations are 20 ± 3 ng/g, increasing to 46 ng/g in surface sediment. Mercury accumulation rate has increased from 30 to 70 μg/m2/a at this site, representing a 2–3-fold increase in Hg concentration and accumulation. There is a lack of correlation between charcoal abundance and Hg accumulation rate in the sediment cores, demonstrating that local biomass burning has little relationship with the observed Hg concentration or Hg accumulation rates. Examined using a sediment focusing-corrected mass accumulation rate approach, the cores have similar anthropogenic atmospheric Hg deposition profiles, suggesting that after accounting for background sediment concentrations the source of accumulating Hg is predominantly atmospheric in origin. In summary, the data document an increase of Hg flux to the Lake Tanganyika ecosystem that is consistent with increasing watershed sediment delivery with background-level Hg contamination, and regional as well as global increases in atmospheric Hg deposition.  相似文献   

2.
Several Gigantopithecus faunas associated with taxonomically undetermined hominoid fossils and/or stone artifacts are known from southern China. These faunas are particularly important for the study of the evolution of humans and other mammals in Asia. However, the geochronology of the Gigantopithecus faunas remains uncertain. In order to solve this problem, a program of geochronological studies of Gigantopithecus faunas in Guangxi Province was recently initiated. Chuifeng Cave is the first studied site, which yielded 92 Gigantopithecus blacki teeth associated with numerous other mammalian fossils. We carried out combined ESR/U-series dating of fossil teeth and sediment paleomagnetic studies. Our ESR results suggest that the lower layers at this cave can be dated to 1.92 ± 0.14 Ma and the upper layers can be dated to older than 1.38 ± 0.17 Ma. Correlation of the recognized magnetozones to the geomagnetic polarity timescale was achieved by combining magnetostratigraphic, biostratigraphic and ESR data. The combined chronologies establish an Olduvai subchron (1.945–1.778 Ma) for the lowermost Chuifeng Cave sediments. We also analyzed the enamel δ13C values of the Gigantopithecus faunas. Our results show that southern China was dominated by C3 plants during the early Pleistocene and that the Gigantopithecus faunas lived in a woodland-forest ecosystem.  相似文献   

3.
Speciation of Hg and conversion to methyl-Hg were evaluated in stream sediment, stream water, and aquatic snails collected downstream from the Bonanza Hg mine, Oregon. Total production from the Bonanza mine was >1360 t of Hg, during mining from the late 1800s to 1960, ranking it as an intermediate sized Hg mine on an international scale. The primary objective of this study was to evaluate the distribution, transport, and methylation of Hg downstream from a Hg mine in a coastal temperate climatic zone. Data shown here for methyl-Hg, a neurotoxin hazardous to humans, are the first reported for sediment and water from this area. Stream sediment collected from Foster Creek flowing downstream from the Bonanza mine contained elevated Hg concentrations that ranged from 590 to 71,000 ng/g, all of which (except the most distal sample) exceeded the probable effect concentration (PEC) of 1060 ng/g, the Hg concentration above which harmful effects are likely to be observed in sediment-dwelling organisms. Concentrations of methyl-Hg in stream sediment collected from Foster Creek varied from 11 to 62 ng/g and were highly elevated compared to regional baseline concentrations (0.11–0.82 ng/g) established in this study. Methyl-Hg concentrations in stream sediment collected in this study showed a significant correlation with total organic C (TOC, R2 = 0.62), generally indicating increased methyl-Hg formation with increasing TOC in sediment. Isotopic-tracer methods indicated that several samples of Foster Creek sediment exhibited high rates of Hg-methylation. Concentrations of Hg in water collected downstream from the mine varied from 17 to 270 ng/L and were also elevated compared to baselines, but all were below the 770 ng/L Hg standard recommended by the USEPA to protect against chronic effects to aquatic wildlife. Concentrations of methyl-Hg in the water collected from Foster Creek ranged from 0.17 to 1.8 ng/L, which were elevated compared to regional baseline sites upstream and downstream from the mine that varied from <0.02 to 0.22 ng/L. Aquatic snails collected downstream from the mine were elevated in Hg indicating significant bioavailability and uptake of Hg by these snails. Results for sediment and water indicated significant methyl-Hg formation in the ecosystem downstream from the Bonanza mine, which is enhanced by the temperate climate, high precipitation in the area, and high organic matter.  相似文献   

4.
The distribution of Cu, Co, As and Fe was studied downstream from mines and deposits in the Idaho Cobalt Belt (ICB), the largest Co resource in the USA. To evaluate potential contamination in ecosystems in the ICB, mine waste, stream sediment, soil, and water were collected and analyzed for Cu, Co, As and Fe in this area. Concentrations of Cu in mine waste and stream sediment collected proximal to mines in the ICB ranged from 390 to 19,000 μg/g, exceeding the USEPA target clean-up level and the probable effect concentration (PEC) for Cu of 149 μg/g in sediment; PEC is the concentration above which harmful effects are likely in sediment dwelling organisms. In addition concentrations of Cu in mine runoff and stream water collected proximal to mines were highly elevated in the ICB and exceeded the USEPA chronic criterion for aquatic organisms of 6.3 μg/L (at a water hardness of 50 mg/L) and an LC50 concentration for rainbow trout of 14 μg/L for Cu in water. Concentrations of Co in mine waste and stream sediment collected proximal to mines varied from 14 to 7400 μg/g and were highly elevated above regional background concentrations, and generally exceeded the USEPA target clean-up level of 80 μg/g for Co in sediment. Concentrations of Co in water were as high as in 75,000 μg/L in the ICB, exceeding an LC50 of 346 μg/L for rainbow trout for Co in water by as much as two orders of magnitude, likely indicating an adverse effect on trout. Mine waste and stream sediment collected in the ICB also contained highly elevated As concentrations that varied from 26 to 17,000 μg/g, most of which exceeded the PEC of 33 μg/g and the USEPA target clean-up level of 35 μg/g for As in sediment. Conversely, most water samples had As concentrations that were below the 150 μg/L chronic criterion for protection of aquatic organisms and the USEPA target clean-up level of 14 μg/L. There is abundant Fe oxide in streams in the ICB and several samples of mine runoff and stream water exceeded the chronic criterion for protection of aquatic organisms of 1000 μg/L for Fe. There has been extensive remediation of mined areas in the ICB, but because some mine waste remaining in the area contains highly elevated Cu, Co, As and Fe, inhalation or ingestion of mine waste particulates may lead to human exposure to these elements.  相似文献   

5.
The “type” DeKalb mounds of northeastern Illinois, USA (42.0°N, −88.7°W), are formed of basal sand and gravel overlain by rhythmically bedded fines, and weathered sand and gravel. Generally from 2 to 7 m thick, the fines include abundant fossils of ostracodes and uncommon leaves and stems of tundra plants. Rare chironomid head capsules, pillclam shells, and aquatic plant macrofossils also have been observed.Radiocarbon ages on the tundra plant fossils from the “type” region range from 20,420 to 18,560 cal yr BP. Comparison of radiocarbon ages of terrestrial plants from type area ice-walled lake plains and adjacent kettle basins indicate that the topographic inversion to ice-free conditions occurred from 18,560 and 16,650 cal yr BP. Outside the “type” area, the oldest reliable age of tundra plant fossils in DeKalb mound sediment is 21,680 cal yr BP; the mound occurs on the northern arm of the Ransom Moraine (−88.5436°W, 41.5028°N). The youngest age, 16,250 cal yr BP, is associated with a mound on the Deerfield Moraine (−87.9102°W, 42.4260°N) located about 9 km east of Lake Michigan. The chronology of individual successions indicates the lakes persisted on the periglacial landscape for about 300 to 1500 yr.  相似文献   

6.
The natural abundance of radiocarbon (14C) provides unique insight into the source and cycling of sedimentary organic matter. Radiocarbon analysis of bacterial phospholipid lipid fatty acids (PLFAs) in salt-marsh sediments of southeast Georgia (USA)—one heavily contaminated by petroleum residues—was used to assess the fate of petroleum-derived carbon in sediments and incorporation of fossil carbon into microbial biomass. PLFAs that are common components of eubacterial cell membranes (e.g., branched C15 and C17, 10-methyl-C16) were depleted in 14C in the contaminated sediment (mean Δ14C value of +25 ± 19‰ for bacterial PLFAs) relative to PLFAs in uncontaminated “control” sediment (Δ14C = +101 ± 12‰). We suggest that the 14C-depletion in bacterial PLFAs at the contaminated site results from microbial metabolism of petroleum and subsequent incorporation of petroleum-derived carbon into bacterial membrane lipids. A mass balance calculation indicates that 6-10% of the carbon in bacterial PLFAs at the oiled site could derive from petroleum residues. These results demonstrate that even weathered petroleum may contain components of sufficient lability to be a carbon source for biomass production by marsh sediment microorganisms. Furthermore, a small but significant fraction of fossil carbon is assimilated even in the presence of a much larger pool of presumably more-labile and faster-cycling carbon substrates.  相似文献   

7.
To establish a natural background and its temporal and spatial variability for the area around Casey Station in the Windmill Islands, East Antarctica, the authors studied major and trace element concentrations and the distribution of organic matter in marine and lacustrine sediments. A wide range of natural variability in trace metal concentrations was identified between sites and within a time scale of 9 ka (e.g., Ni 5–37 mg kg−1, Cu 20–190 mg kg−1, Zn 50–300 mg kg−1, Pb 4.5–34 mg kg−1). TOC concentrations are as high as 3 wt.% at the marine sites and 20 wt.% at the lacustrine sites, and indicate highly productive ecosystems. These data provide a background upon which the extent of human impact can be established, and existing data indicate negligible levels of disturbance. Geochemical and lithological data for a lacustrine sediment core from Beall Lake confirm earlier interpretation of recent climatic changes based on diatom distribution, and the onset of deglaciation in the northern part of the Windmill Islands between 8.6 and 8.0 ka BP. The results demonstrate that geochemical and lithological data can not only be used to define natural background values, but also to assess long-term climatic changes of a specific environment. Other sites, however, preserve a completely different sedimentary record. Therefore, inferred climatic record, and differences between sites, can be ascribed to differences in elevation, distance from the shore, water depth, and local catchment features. The extreme level of spatial variability seems to be a feature of Antarctic coastal areas, and demonstrates that results obtained from a specific site cannot be easily generalized to a larger area.  相似文献   

8.
Diatom frustule-bound organic compounds presumably play an important role in biomineralization and constitute an important pool of organic matter preserved in diatom frustule-rich sediments. In this study, detailed analysis of diatom frustule-bound organic matter in opal-rich Southern Ocean plankton and sediments revealed for the first time the presence of low molecular weight, UV light absorbing compounds called mycosporine-like amino acids (MAAs). Chemically cleaned diatom frustule-derived biosilica was dissolved in HF, releasing bound or entrapped organic compounds that were subsequently characterized using liquid chromatography with UV-Vis and electrospray ionization mass spectrometry (LC/PDA/ESI-MS). Palythine ([M+H]+ = 245), porphyra-334 ([M+H]+ = 347) and shinorine ([M+H]+ = 333) were the most abundant MAAs detected in HF digests of plankton and sediment. Traces of asterina ([M+H]+ = 289), palythinol ([M+H]+ = 303) and palythinic acid ([M+H]+ = 329) were also detected. MAAs in cleaned HF digested frustules were up to two orders of magnitude more abundant than methanol extractable MAAs. MAAs are substituted with acid hydrolysable amino acid residues. Our results suggest that MAAs, and not proteins, could be responsible for the high proportion of the amino acids glycine and threonine found in hydrolysates of HF digested diatom-rich environmental samples. Total MAAs accounted for 3-27% of the carbon and 2-18% of total nitrogen in the frustules undergoing various chemical cleaning treatments. This is the first report of MAAs in close association with a mineral phase and we hypothesize that the mineral matrix could stabilize these compounds, thereby enhancing photoprotection against the harmful effects of UV light. The presence of frustule-bound MAAs in sediment cores further suggests the possibility that they could be used in compound-specific isotope analysis of diatom-bound organic matter and as indicators of past solar irradiance.  相似文献   

9.
To improve the usefulness and accuracy of modeling Earth's anthrobiogeochemical metal cycles, global maps at approximately 1° × 1° are produced of the concentrations and masses of Fe, Al, Cu, and Zn contained in continental sediments and soils. The maps generated utilize inverse distance weighting (IDW) and cokriging to generate new estimates for geospatially weighted mean global concentrations for these metallic micronutrients. Sediment metal concentration maps are generated from IDW of sediment samples; global soil maps are produced via cokriging upon an underlying parent rock dataset composed of both surface bedrock and sediment samples. Derived are independent estimates for the global mean concentrations in continental sediments (Fe = 3.1 wt.%, Al = 6.1 wt.%, Cu = 45 μg/g, Zn = 86 μg/g) and soils (Fe = 2.5 wt.%, Al = 3.9 wt.%, Cu = 17 μg/g, Zn = 50 μg/g). While continental sediment concentrations for Cu are within the range of previous estimates, Zn concentrations are relatively higher, ~ 20 μg/g above previous estimates. Fe and Al are slightly depleted (~ 1 wt.%) in continental sediments relative to previous estimates, likely ascribable to sampling bias and error inherent in the comparative methodologies. Besides an estimated global mean, metal concentrations in soils are also broken down by FAO soil group. Metal masses in sediments and soils remain within 30% of previous, non-spatial estimates. These maps also illustrate the discernable spatial variability across the Earth's surface. Despite data gaps, maps of metal mass show regional patterns such as the high quantities of Al in the soils and biomass of the Amazonia and Congo regions. Concentrations of metals are relatively high in the anthrosols of China. Finally, this analysis highlights those areas for which generating and providing publically available geochemical data should be prioritized. For instance, gypsisols, lixisols, and nitisols have little to no analytical data available on metal contents. A sensitivity analysis suggests that the most poorly constrained soil metal concentrations occur in the thick, old tropical soils of central Africa and the anthrosols of eastern China.  相似文献   

10.
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   

11.
Sediment supply: The main driver of shelf-margin growth   总被引：1，自引：0，他引：1  
Despite the obvious importance of sediment supply to shelf-margin architecture and to the potential of margins to contain and bypass deep-water sands, the role of supply in shelf-margin growth has received limited attention. High cross-shelf sediment flux is critically important for the occurrence of deep-water sands, not least on Greenhouse or rapidly subsiding margins where the impact of eustatic sea-level fall may be insufficient to drive sediment delivery out across the shelf into deep-water areas. To draw greater attention to the supply parameter we review a number of shelf margins that have grown chiefly through supply by shelf-edge deltas and associated sediment-gravity flows. Based on structural style and water depth, we recognize two broad types of shelf-margin. Moderately deep-water margins produce clinoforms < 1000 m high and show rates of shelf-edge progradation < 60 km/My and aggradation < 270 m/My, and consequently, infill their basins relatively rapidly, and develop more progradational architectures with morphologically smooth and relatively undeformed slopes. Very deep-water margins produce clinoforms > 1000 m high and generally show rates of shelf-edge progradation < 40 km/My and aggradation < 2500 m/My, and therefore infill their basins more slowly and develop more aggradational architectures with much gravity-driven slope deformation, proneness to failure and ponded architectures (salt or shale driven). On both margin types, long-term (> 1 My) rates of shelf-edge progradation of several tens of km/My tend to be linked to the delivery of relatively large volumes of sand into the deep-water basin. Delivery of this sand beyond the shelf-edge happens despite Greenhouse conditions and is likely recurrent and periodic (delivery cycles in the order of 100′s ky). Such prominent margin growth is a strong indication that sediment influx was relatively high and we refer to these margins as “supply-dominated” shelf margins. The Gulf of Mexico margin is a well-known and data-rich example of a “supply-dominated” shelf-margin during certain times (e.g., Paleocene). In contrast, on both margin types, low rates of shelf-edge progradation are linked to diminished (or even non-existent) and less frequently recurrent deep-water sediment delivery suggestive of relatively low sediment influx. Occurrence of deep-water sand delivery under low sediment influx probably requires fall of relative sea level. The differences between rapidly and slowly prograding margins indicate that sediment supply (and not sea level) is likely to be the key limiting factor on the growth of shelf margins and that sediment supply, as interpreted through progradation rate, can therefore be used to make a first-order prediction of relative amounts of sand passed to deep-water areas.  相似文献   

12.
Sediments from the Aquia aquifer in coastal Maryland were collected as part of a larger study of As in the Aquia groundwater flow system where As concentration are reported to reach levels as high as 1072 nmol kg−1, (i.e., ∼80 μg/L). To test whether As release is microbially mediated by reductive dissolution of Fe(III) oxides/oxyhydroxides within the aquifer sediments, the Aquia aquifer sediment samples were employed in a series of microcosm experiments. The microcosm experiments consisted of sterilized serum bottles prepared with aquifer sediments and sterilized (i.e., autoclaved), artificial groundwater using four experimental conditions and one control condition. The four experimental conditions included the following scenarios: (1) aerobic; (2) anaerobic; (3) anaerobic + acetate; and (4) anaerobic + acetate + AQDS (anthraquinone-2,6-disulfonic acid). AQDS acts as an electron shuttle. The control condition contained sterilized aquifer sediments kept under anaerobic conditions with an addition of AQDS. Over the course of the 27 day microcosm experiments, dissolved As in the unamended (aerobic and anaerobic) microcosms remained constant at around ∼28 nmol kg−1 (2 μg/L). With the addition of acetate, the amount of As released to the solution approximately doubled reaching ∼51 nmol kg−1 (3.8 μg/L). For microcosm experiments amended with acetate and AQDS, the dissolved As concentrations exceeded 75 nmol kg−1 (5.6 μg/L). The As concentrations in the acetate and acetate + AQDS amended microcosms are of similar orders of magnitude to As concentrations in groundwaters from the aquifer sediment sampling site (127-170 nmol kg−1). Arsenic concentrations in the sterilized control experiments were generally less than 15 nmol kg−1 (1.1 μg/L), which is interpreted to be the amount of As released from Aquia aquifer sediments owing to abiotic, surface exchange processes. Iron concentrations released to solution in each of the microcosm experiments were higher and more variable than the As concentrations, but generally exhibited similar trends to the As concentrations. Specifically, the acetate and acetate + AQDS amended microcosm typically exhibited the highest Fe concentrations (up to 1725 and 6566 nmol kg−1, respectively). The increase in both As and Fe in the artificial groundwater solutions in these amended microcosm experiments strongly suggests that microbes within the Aquia aquifer sediments mobilize As from the sediment substrate to the groundwaters via Fe(III) reduction.  相似文献   

13.
The fractionation of P in Pandoh Lake surface sediments has been investigated for the first time in order to understand its environmental availability and sources, and the eutrophication status of this lake. Inorganic-P is present mainly as authigenic-P (step-III). The authigenic P concentration is higher in winter relative to the summer and monsoon seasons and ranged from 35.9 to 46.9 μg/g. The loosely sorbed or exchangeable-P (step-I), Fe(III)-bound-P (step-II) and detrital inorganic-P (step-IV) were higher in the monsoon season and varied from 3.70 to 11.1 μg/g, 16.9 to 32.0 μg/g and 9.89 to 17.0 μg/g, respectively. Organic-P reached a maximum in the summer season and ranged from 8.00 to 14.9 μg/g. Authigenic-P and detrital inorganic-P show seasonal changes, as pH influences the interaction between P and CaCO3 in the water column. In the winter season, phosphate is precipitated out of the water column and fixed in the sediments as a result of an increase in pH. Calcite-bound-P in the sediments may be redissolved by decreasing pH in the summer season. Relatively high rates of mineralization during the monsoon results in the seasonal pattern of organic-P fractionation to sediment as follows: monsoon = winter < summer. Iron, Ca, organic matter and silt and clay contents seem to play a significant role in regulating the seasonal P budget. Principal component analysis (PCA) was used to identify the factors which influence sedimentary P in the different seasons.  相似文献   

14.
Sediment capping is a remedial option for managing contaminated sediments that involves the artificial placement of a layer of material over a contaminated area. Sorbent materials such as activated C and coke can be used to amend sand caps to improve cap performance. In this study, analytical and numerical modelling approaches were compared for predicting contaminant fate and transport in sediment caps using several diffusion-controlled and advection-dominated contaminant transport scenarios. An analytical tool was used to predict cap performance at steady-state. These results were compared with the results from the numerical CoReTranS model in which the effective diffusivity and degradation rates were modelled as discontinuous functions at a prescribed bioturbation depth. The numerical approach was also applied to modelling a sorptive cap. It was shown that, while the analytical approach can be used to predict steady-state contaminant transport, the numerical approach is needed to evaluate multiple sediment layers with different transport and sorption characteristics and to examine the transient performance between the time that the single layer transient is applicable (i.e., before penetration of the cap containment layer) and until steady-state in the upper layer. For the 30 cm thick sand cap that was considered in this study, the predicted time to reach steady-state conditions for a diffusion-controlled scenario is 1 ka. For an advection-dominated transport, the time to reach steady-state conditions is reduced to 100 a. The activated C-amended sand cap was more effective in isolating the contaminant within the sorbent layer for a sustained period of time (∼100 a). Results from both modelling approaches showed that capping can effectively reduce contaminant flux to the overlying water with critical variables being cap thickness, groundwater velocity, and sediment sorptivity.  相似文献   

15.
Late Cretaceous terrestrial ecosystems in southern Europe are relatively poorly known, although much progress has been made during the past decade, principally with regard to the microvertebrate components of these ecosystems. The Maastrichtian terrestrial deposits of the Haeg Basin, at the easternmost end of the South European archipelago and well known for reptilian fossils (e.g., turtles, crocodilians, pterosaurs and dinosaurs), have been thoroughly screened during the past five years. Important microvertebrate assemblages, both quantitatively and qualitatively speaking, were found at Pui (Sînpetru Formation), Tutea and, particularly, Vlioara (Densu-Ciula Formation). Several new taxa are noted here for the first time for the Haeg Basin, including gars, discoglossids, albanerpetontids, scincomorphan and anguimorphan lizards; dromaeosaurids and multituberculates are confirmed. Most of the microvertebrate remains are poorly preserved and precise systematic assignment has proved difficult. The Haeg fauna appears to be primitive and endemic, with a Neopangean core composition, and suggests a composite palaeobiogeographic origin for the Late Cretaceous European ecosystems, confirming conclusions reached in studies of the larger vertebrates.  相似文献   

16.
A multisite surface complexation (MUSIC) model for ferrihydrite (Fh) has been developed. The surface structure and composition of Fh nanoparticles are described in relation to ion binding and surface charge development. The site densities of the various reactive surface groups, the molar mass, the mass density, the specific surface area, and the particle size are quantified. As derived theoretically, molecular mass and mass density of nanoparticles will depend on the types of surface groups and the corresponding site densities and will vary with particle size and surface area because of a relatively large contribution of the surface groups in comparison to the mineral core of nanoparticles. The nano-sized (∼2.6 nm) particles of freshly prepared 2-line Fh as a whole have an increased molar mass of M ∼ 101 ± 2 g/mol Fe, a reduced mass density of ∼3.5 ± 0.1 g/cm3, both relatively to the mineral core. The specific surface area is ∼650 m2/g. Six-line Fh (5-6 nm) has a molar mass of M ∼ 94 ± 2 g/mol, a mass density of ∼3.9 ± 0.1 g/cm3, and a surface area of ∼280 ± 30 m2/g. Data analysis shows that the mineral core of Fh has an average chemical composition very close to FeOOH with M ∼ 89 g/mol. The mineral core has a mass density around ∼4.15 ± 0.1 g/cm3, which is between that of feroxyhyte, goethite, and lepidocrocite. These results can be used to constrain structural models for Fh. Singly-coordinated surface groups dominate the surface of ferrihydrite (∼6.0 ± 0.5 nm−2). These groups can be present in two structural configurations. In pairs, the groups either form the edge of a single Fe-octahedron (∼2.5 nm−2) or are present at a single corner (∼3.5 nm−2) of two adjacent Fe octahedra. These configurations can form bidentate surface complexes by edge- and double-corner sharing, respectively, and may therefore respond differently to the binding of ions such as uranyl, carbonate, arsenite, phosphate, and others. The relatively low PZC of ferrihydrite can be rationalized based on the estimated proton affinity constant for singly-coordinated surface groups. Nanoparticles have an enhanced surface charge. The charging behavior of Fh nanoparticles can be described satisfactory using the capacitance of a spherical Stern layer condenser in combination with a diffuse double layer for flat plates.  相似文献   

17.
Located at the midpoint of the Asian “airborne dust corridor”, Lake Qinghai receives substantial dust annually, which may impact the biogeochemical cycles of the system. In order to determine quantitatively the flux and chemical contributions of dust to Lake Qinghai sediment, dust samples were collected monthly at two sites surrounding the lake from June 2009 to May 2011. The results demonstrate similar chemical compositions of dust samples to the local loess, implying strong representativeness of regional dust. The average dust deposition flux is 265.7 ± 55.0 g/m2/a, constituting 56.6 ± 11.7% of the modern sediment, approximating to previous estimates (∼65%). Contributions of dust-derived elements in the sediment differ substantially, with a minimum of 16.7% for Sr and a maximum of 83.9% for Cu. Among these elements, the contribution of lithophile elements (Na, Al, K, Ti, Mn, Fe and Rb) is close to that of the bulk dust; the contributions of mobile elements (Mg, Ca and Sr) are low, only 16.7% (Sr)–26.1% (Mg), whereas potentially harmful metals (Cu, Zn and Pb) have high contributions (70.3–83.9%). Seasonal variations of elemental inputs indicate that springtime contributions dominate the annual dust fluxes for all elements into the sediment, in agreement with the high dust flux in spring. These observations not only quantify the contribution of dust to the sediment of Lake Qinghai, but also highlight the important role of dust in the accumulation of various elements in the sediment, especially for potentially harmful metals.  相似文献   

18.
The Drenchwater shale-hosted Zn–Pb–Ag deposit and the immediate vicinity, on the northern flank of the Brooks Range in north-central Alaska, is an ideal example of a naturally low pH system. The two drainages, Drenchwater and False Wager Creeks, which bound the deposit, differ in their acidity and metal contents. Moderately acidic waters with elevated concentrations of metals (pH ? 4.3, Zn ? 1400 μg/L) in the Drenchwater Creek drainage basin are attributed to weathering of an exposed base-metal-rich massive sulfide occurrence. Stream sediment and water chemistry data collected from False Wager Creek suggest that an unexposed base-metal sulfide occurrence may account for the lower pH (2.7–3.1) and very metal-rich waters (up to 2600 μg/L Zn, ? 260 μg/L Cu and ?89 μg/L Tl) collected at least 2 km upstream of known mineralized exposures. These more acidic conditions produce jarosite, schwertmannite and Fe-hydroxides commonly associated with acid-mine drainage. The high metal concentrations in some water samples from both streams naturally exceed Alaska state regulatory limits for freshwater aquatic life, affirming the importance of establishing base-line conditions in the event of human land development. The studies at the Drenchwater deposit demonstrate that poor water quality can be generated through entirely natural weathering of base-metal occurrences, and, possibly unmineralized black shale.  相似文献   

19.
Lacustrine sediments, submerged tailings, and their pore waters have been collected at several sites in Yellowknife Bay, Great Slave Lake, Canada, in order to investigate the biogeochemical controls on the remobilization of As from mining-impacted materials under different depositional conditions. Radiometric dating confirms that a mid-core enrichment of Pb, Zn, Cu and Sb corresponds to the opening of a large Au mine 60 a ago. This was evident even in a relatively remote site. Arsenic was enriched at mid-core, coincident with mining activity, but clearly exhibited post-depositional mobility, migrating upwards towards the sediment water interface (SWI) as well as down-core. Deep-water (15 m) Yellowknife Bay sediments that contain buried mine waste are suboxic, relatively organic-rich and abundant in microbes with As in pore waters and sediments reaching 585 μg/L and 1310 mg/kg, respectively. Late summer pore waters show equal proportions of As(III) and As(V) (16–415 μg/L) whereas late winter pore waters are dominated by As(III) (284–947 μg/L). This can be explained by As(III) desorption mechanisms associated with the conversion of FeS to FeS2 and the reduction of As(V) to As(III) through the oxidation of dissolved sulfide, both microbially-mediated processes. Processes affecting As cycling involve the attenuating efficiency of the oxic zone at the SWI, sediment redox heterogeneity and the reductive dissolution of Fe(hydr)oxides by labile organic matter, temporarily and spatially variable.  相似文献   

20.
Two samples of produced-water collected from a storage tank at US Geological Survey research site B, near Skiatook Lake in northeastern Oklahoma, have activity concentrations of dissolved 226Ra and 228Ra that are about 1500 disintegrations/min/L (dpm/L). Produced-water also contains minor amounts of small (5–50 μm) suspended grains of Ra-bearing BaSO4 (barite). Precipitation of radioactive barite scale in the storage tank is probably hindered by low concentrations of dissolved SO4 (2.5 mg/L) in the produced-water. Sediments in a storage pit used to temporarily collect releases of produced-water have marginally elevated concentrations of “excess” Ra (several dpm/g), that are 15–65% above natural background values. Tank and pit waters are chemically oversaturated with barite, and some small (2–20 μm) barite grains observed in the pit sediments could be transferred from the tank or formed in place. Measurements of the concentrations of Ba and excess Ra isotopes in the pit sediments show variations with depth that are consistent with relatively uniform deposition and progressive burial of an insoluble Ra-bearing host (barite?). The short-lived 228Ra isotope (half-life = 5.76 a) shows greater reductions with depth than 226Ra (half-life = 1600 a), that are likely explained by radioactive decay. The 228Ra/226Ra activity ratio of excess Ra in uppermost pit sediments (1.13–1.17) is close to the ratio measured in the samples of produced-water (0.97, 1.14). Declines in Ra activity ratio (excess) with sediment depth can be used to estimate an average rate of burial of 4 cm/a for the Ra-bearing contaminant. Local shallow ground waters contaminated with NaCl from produced-water have low dissolved Ra (<20 dpm/L) and also are oversaturated with barite. Barite is a highly insoluble Ra host that probably limits the environmental mobility of Ra at site B.  相似文献   

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