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1.
The accumulation and mobility of Fe, Mn, Al, Cu, Ni and Pb in the sediments of two lakes (Clearwater, pH 4.5; and McFarlane, pH 7.5) near Sudbury, Ontario have been investigated. The Al, Cu and Ni concentrations are expectedly relatively high in the overlying waters of Clearwater Lake and much lower for Al and Cu in McFarlane Lake. The low trace metal concentrations found in the anoxic porewaters of Clearwater Lake could be explained by a sharp increase in porewater pH concomitant with SO42 reduction and H2S production within the first 1–2 cm of the sediments, which has conceivably led to the precipitation of mineral phases such as AL(OH)3, NiS, and CuS. In both lakes, Fe concentrations in anoxic porewaters appear to be controlled by FeS and/or FeCO3 formation. Solubility calculations also indicate MnCO3 precipitation in McFarlane Lake. In Clearwater Lake, however, both porewater and total Mn were relatively low, a possible result of the continuous loss of Mn(II) through the acidic interface. It is suggested that upwardly decreasing total Mn profiles resulting from the removal of Mn from the top sediment layers under acidic conditions may constitute a reliable symptom of recent lake acidification.The downward diffusion of AI, Cu and Ni from the overlying water to the sediments has been estimated from their concentration gradients at the interface and compared to their total accumulation rates in the sediments. In both lakes the diffusion of Al is negligible compared to its accumulation rate. However, diffusion accounts for 24–52% of the accumulation of Cu in the sediments of Clearwater Lake, but appears negligible in McFarlane Lake. The downward diffusive flux of Ni is important and may explain 76–161% of the estimated Ni accumulation rate in Clearwater Lake, and 59% in McFarlane Lake. The porewater Cu and Ni profiles suggest that the subsurface sedimentary trace metal peaks observed in Clearwater Lake (as in other acid lakes) may not be caused by sediment leaching or by a recent reduction in sedimentation but may have a diagenetic origin instead. Diffusion to the sediments thus appears to be an important and previously overlooked trace metal deposition mechanism, particularly in acid lakes.  相似文献   

2.
Arsenic species including arsenite, arsenate, and organic arsenic were measured in the porewaters collected from Poyang Lake, the largest freshwater lake of China. The vertical distributions of dissolved arsenic species and some diagenetic constituents [Fe(II), Mn(II), S(−II)] were also obtained in the same porewater samples in summer and winter. In sediments the concentration profiles of total As and As species bound to Fe–Mn oxyhydroxides and to organic matter were also determined along with the concentrations of Fe, Mn and S in different extractable fractions. Results indicate that, in the summer season, the concentrations of total dissolved As varying from 3.9 to 55.8 μg/L in sediments were higher than those (5.3–15.7 μg/L) measured in the winter season, while the concentrations of total As species in the solid phase varied between 10.97 and 25.32 mg/kg and between 7.84 and 30.52 mg/kg on a dry weight basis in summer and winter, respectively. Seasonal profiles of dissolved As suggest downward and upward diffusion, and the flux of dissolved As across the sediment–water interface (SWI) in summer and winter were estimated at 3.88 mg/m2 a and 0.79 mg/m2 a, respectively. Based on porewater profiles and sediment phase data, the main geochemical behavior of As was controlled by adsorption/desorption, precipitation and molecular diffusion. The solubility and migration of inorganic As are controlled by Fe–Mn oxyhydroxides in summer whereas they appear to be more likely controlled by both amorphous Fe–Mn oxyhydroxides and sulfides in winter. A better knowledge of the cycle of As in Poyang Lake is essential to a better management of its hydrology and for the environmental protection of biota in the lake.  相似文献   

3.
Analytical methods of dissolved Se species in river water and seawater were established and applied to study dissolved Se speciation in the Kaoping and Erhjen rivers and estuaries, southwestern Taiwan. The Kaoping and Erhjen rivers and estuaries were respectively in relatively oxygenated and oxygen-deficient conditions as revealed from the distributions of dissolved oxygen, DOC, nutrients, and dissolved Mn. Concentrations of dissolved total Se increased downstream in the riverine sections, ranging from 0.6 nM to 1.2 nM for the Kaoping River and from 0.8 nM to 1.05 nM for the Erhjen River. The dissolved total Se was only slightly higher in the Erhjen middle estuary than in the Kaoping middle estuary in spite of heavier pollution in the former. The dissolved total Se behaved rather conservatively in the Kaoping estuary but nonconservatively in the Erhjen estuary resulting from anthropogenic inputs, and in this respect showed similarities with the behavior of redox-sensitive Mn. The predominant species of selenium were Se(VI) and organic Se in the Kaoping River and Se(VI) in the Kaoping estuary. The elevated concentration of Se(VI) in the Kaoping estuary may stem from the degradation of organic Se and oxidation of Se(IV). On the other hand, Se(IV) and organic Se were equally dominant in the Erhjen River, and Se(IV) was predominant through most of the Erhjen estuary. The elevated distribution of Se(IV) in the Erhjen middle estuary may result mostly from partial decomposition of organic Se, but further oxidation of Se(IV) was inhibited in reducing waters. However, Se(VI) became dominant at Erhjen outer estuary where water was oxygenated by the replacement of intruded coastal seawater. Apparently, the speciation of dissolved Se was mainly controlled by the biological and redox processes in the Kaoping and Erhjen rivers and estuaries.  相似文献   

4.
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   

5.
Geochemistry of Rare Earth Elements in the Ocean   总被引：4，自引：0，他引：4  
This work briefly outlines modern ideas on geochemistry of rare earth elements (REE) in the ocean. Sources of REE and chemical properties of these elements, which govern their migration ability in natural processes, are considered. The REE behavior in the river water–seawater mixing zone is analyzed. The fractionation of dissolved and suspended REE in oceanic water in both aerobic and anaerobic conditions is also considered. It is shown that the variability of REE composition in pelagic sediments reflects the fractionation of these elements in the oceanic water as a consequence of material differentiation in the ocean. The REE distribution in terrigenous, authigenic, hydrothermal, and biogenic constituents of sediments, such as clay, bone debris, barite, phillipsite, Fe–Mn oxyhydroxides (ferromanganese nodules and micronodules), Fe–Ca hydroxo-phosphate, diatoms, and foraminifers, is considered.  相似文献   

6.
We measured the vertical distributions of Mo, Fe, Mn, sulfide, sulfate, organic carbon, major ions, and pH in sediment porewater from one perennially oxic and three seasonally anoxic lacustrine basins in Eastern Canada, as well as those of Mo, acid volatile sulfide, Fe, Mn, Al, organic C, 210Pb and 137Cs in sediment cores from the same sites. The only input of anthropogenic Mo to these lakes comes from atmospheric deposition.The relatively monotonous distribution of Mo in the porewater of three seasonally anoxic basins suggests that Mo is not redistributed in the sedimentary column during periods of anoxia. In contrast, porewater Mo profiles obtained at three sampling dates in a perennially oxic basin display sharp Mo peaks below the sediment-water interface, indicating redistribution subsequent to deposition. Modeling of these latter porewater Mo profiles with a diagenetic reaction-transport equation coupled to comparisons among the various porewater and solid phase profiles reveal that Mo is released at 1-2 cm depth as a consequence of the reductive dissolution of Fe oxyhydroxides and scavenged both at the vicinity of the sediment-water interface, by re-adsorption onto authigenic Fe oxyhydroxides, and deeper in the sediments where dissolved sulfide concentrations are higher. The estimated rate constant for the adsorption of Mo onto Fe oxyhydroxides is 36 ± 45 cm3 mol−1 s−1.Diagenetic modeling indicates that authigenic Mo in sediments of the perennially oxic basin represents about one-third of the total solid phase Mo in the first cm below the sediment-water interface and only one tenth below this horizon. If we assume that no authigenic Mo is accumulated in the seasonally anoxic lake sediments we conclude that the sediment Mo concentrations, which are up to 3-16 times higher than the average lithogenic composition, depending on the lake, are mainly due to atmospheric deposition of anthropogenic Mo and not to the formation of authigenic Mo phases. Reconstructed historical records of the atmospheric Mo deposition indicate maximum values in the 1970s and 1980s and significant decreases since then. Emissions to the atmosphere associated with the smelting of non-ferrous ores and coal combustion appear to be the most important sources of anthropogenic Mo.  相似文献   

7.
为探析长江口沉积物-水界面砷的迁移转化机制,本文分析了2019年夏季长江口4个站位上覆水和间隙水中总As浓度及形态的剖面变化特征,耦合氧化还原敏感元素(Fe、Mn和S)的剖面变化剖析了沉积物-水界面砷循环的Fe-Mn-S控制机制,同时结合砷相关功能基因探讨了沉积物-水界面砷迁移转化的微生物调控过程,估算了沉积物-水界面总As的扩散通量。结果表明,除A7-4站位外,长江口其他3个站位间隙水总As以As3+为主要存在形态,且总As浓度均在上覆水中为最低值(0.748~1.57 μg·L-1),而在间隙水中随着深度增加而逐渐增加并在6~9 cm深度达到峰值(7.14~26.9 μg·L-1)。间隙水总As及As3+浓度的剖面变化趋势与溶解态Fe2+、Mn2+相似,其均在中间层出现高值,说明沉积物Fe/Mn还原带砷的释放可能是随固相Fe(Ⅲ)或Mn(Ⅳ)的还原而转移到间隙水中的。氧化层和Fe/Mn还原带过渡区间隙水砷浓度与砷异化还原菌功能基因arrA和arsC丰度存在对应关系(除A1-3站外),说明砷异化还原菌将溶解As5+或固相As5+还原为溶解As3+可能是该过渡层砷迁移转化的另一重要过程。硫酸盐还原带的间隙水总As和As3+浓度降低,但由于间隙水的低S2-浓度不利于砷硫化物生成,因此深层间隙水砷可能与铁硫矿物结合而被移除。底层环境氧化还原条件是影响沉积物-水界面砷迁移转化的重要因素,随底层水DO浓度的降低,砷迁移转化更倾向于微生物还原控制。长江口沉积物-水界面总As的扩散通量为1.18×10-7~2.07×10-7 μmol·cm-2·s-1,均表现为沉积物间隙水中总As向上覆水释放,即沉积物是研究区域水体总As的来源之一。  相似文献   

8.
Mn, Sr, Ba, Rb, Cu, Zn, Pb and Cd concentrations have been measured seasonally in the water and deposited sediments of the system comprising: Zala river (main input) — Lakes Kis-Balaton 1 and 2 (small artificial lakes created in a former bay of Lake Balaton) — Keszthely bay (hypertrophic part of Lake Balaton). The concentrations of the trace elements together with pH, alkalinity, dissolved cations (Ca2+, Mg2+, Na+, and K+), dissolved inorganic ligands (Cl–, SO4 2–), particulate Al, Ca, inorganic and organic carbon are used to assess the contamination of the study area and biogeochemical processes controlling trace element concentrations. Thermodynamic speciation calculations have also been utilized to enhance our understanding of the system. In the sediments Rb, Ba, Cu and Zn concentrations were mainly controlled by the abundance of the aluminosilicate fraction. Strontium was mainly associated with the calcium carbonate fraction. The aluminosilicate fraction constitutes a major sink for Mn and Cd but the concentration of these elements are also strongly related to calcite precipitation. The main processes that control the dissolved distribution of trace elements in the Balaton system were: solid phase formation (carbonate) for Mn; coprecipitation with calcite for Sr, Ba, Rb and possibly Mn and Cd; adsorption/desorption processes (pH dependent) for Zn and Pb; solubilization of Mn and precipitation of Cd and Cu in reed covered wetland areas where anoxic conditions were probably existing during the warm season. A preliminary budget of atmospheric and river input to Lake Balaton has also been outlined. Although Lake Balaton, is subjected to anthropogenic inputs mainly from agricultural and domestic activities, their impact on trace element concentrations in the Balaton system is very limited due to the efficiency of removal processes (i.e. adsorption and co-precipitation) and to high sedimentation rates and strong sediment re-suspension. Anthropogenic inputs are only detected for Pb.  相似文献   

9.
This paper presents results from the numerical modelling of the transport of atmospheric noble gases (He, Ne, Ar, Kr, Xe), tritiated water and 3He produced by radioactive decay of 3H, in unconsolidated lacustrine sediment. Two case studies are discussed: (1) the evolution of 3H and 3He concentrations in the sediment porewater of Lake Zug (Switzerland) from 1953 up to the present; and (2) the response of dissolved atmospheric noble gas concentrations in the sediment porewater of a subtropical lake to an abrupt climatic change that occurred some 10 kyr before the present. (1) Modelled 3H and 3He porewater concentrations are compared with recent data from Lake Zug. An estimate of the effective diffusion coefficients in the sediment porewater is derived using an original approach which is also applicable also to lakes for which the historical 3H and 3He concentrations in the water column are unknown. (2) The air/water partitioning of atmospheric noble gases is sensitive to water temperature and salinity, and thus provides a mechanism by which these environmental variables are recorded in the concentrations of atmospheric noble gases in lakes. We investigate the feasibility of using noble gas concentrations in the porewater of lacustrine sediments as a proxy for palaeoenvironmental conditions in lakes. Numerical modelling shows that heavy noble gases in sediment porewater, because of their comparatively small diffusion coefficients and the strong temperature sensitivity of their equilibrium concentrations, can preserve concentrations corresponding to past lake temperatures over times on the order of 10 kyr. Noble gas analysis of sediment porewaters therefore promises to yield valuable quantitative information on the past environmental states of lakes.  相似文献   

10.
The Integrated Lake Watershed Acidification Study (ILWAS) model was used to simulate the recovery of the highly acidified Clearwater Lake, Ontario. Recovery started in the mid-1970s and continued through the 1980s in response to an estimated 30–50% decrease in S deposition from smelter emissions in nearby Sudbury, Ontario. Appreciable recovery of Clearwater Lake between the mid-1970s and 1987 is simulated by the ILWAS model, as indicated by a 50% decrease in SO−4 concentration, an 80% decrease in total Al concentration, an increase in acid-neutralizing capacity (ANC) from −60 to −17 μeq/l, and an increase in pH from 4.2 to 4.8. These decreases in acidic constituents are in good agreement with monitoring data. Long-term simulations indicate that deacidification may continue until 2020, if S deposition rates remain at or less than the 1987 level. Simulations for years beyond 2020 yield yearly average ANC values of 18–40 μeq/l and pH values of 6.2–6.6, which are comparable to the estimated pre-smelter pH of 6.0–6.5 for Clearwater Lake. The agreement between simulated and monitoring data for the first 10 a of recovery and the simulated long-term recovery of the lake to its presmelter level of acidity lend confidence in the capability of numerical models to simulate the reversibility of watershed acidification and suggest that some highly acidic watersheds may eventually recover, given substantial decreases in acid deposition.  相似文献   

11.
A study of the water and sediment chemistry of the Nainital, Bhimtal, Naukuchiyatal and Sattal Lakes of Kumaun, has shown that the water of these lakes are alkaline and that electrical conductivity, total dissolved solid and bicarbonate HCO 3 − are much higher in Nainital than in the other three lakes. The weathering of limestone lithology and anthropogenic pollution, the latter due to the very high density of population in the Nainital valley, are the primary sources of enhanced parameters. The low pH of Nainital Lake water is due to low photosynthesis and enhanced respiration, increasing CO2 in the water and the consequent enhancement of Ca2+ and HCO 3 − . The dissolved oxygen in Nainital Lake is less compared to other lakes, indicating anoxic conditions developing at the mud–water interface at depth. The PO 4 3− content in Nainital is higher (124 μg/l), showing an increasing trend over time leading to eutrophic conditions. The trace metals (Cu, Co, Zn, Ni, Mn, and Sr) are present in greater amounts in the water of Nainital Lake than in the other three lakes, though Fe and Cr are high in Bhimtal and Fe in Naukuchiyatal. The higher abundance is derived from the leaching of Fe–Mg from metavolcanic and metabasic rocks. Most of the heavy metals (Cr, Ni, Cu, Mn, Fe, Sr, and Zn) significantly enrich the suspended sediments of the lakes compared to the bed sediments which due to their adsorption on finer particles and owing to multiple hydroxide coating and organic content, except for Fe, which is enriched in the bed sediments. The high rate of sedimentation, 11.5 mm/year in Nainital, compared to Bhimtal with 4.70 mm/year, Naukuchiyatal with 3.72 mm/year, and Sattal with 2.99 mm/year, has resulted in shorter residence time, poor sorting of grains, and lesser adsorption of heavy metals, leading consequently, their depletion in the bed sediments of Nainital Lake.  相似文献   

12.
The accumulation of selenium in evaporation basins (or ponds) in the San Joaquin Valley, California is of a great concern due to its potential hazards to environments. In this study, the accumulation, speciation and concentrations of Se were examined in waters as well as sediments in a system of the evaporation ponds. A significant decrease in the total dissolved Se concentration in Cell 1 in which drainage water with higher Se concentration was pumped from Inlet Channels indicated that the immobilization of Se was active in the Cell 1 and resulted in the higher Se concentration in sediments compared to the terminal cell such as Cell 9. The percentage of reduced Se species such as selenite [Se(IV)] and org-Se of total Se in drainage waters was also found increased in Cell 1 compared to Inlet Channels. The total dissolved Se concentrations in water along flow paths from Cell 1 were relatively constant except for terminal cells such as Cells 9 and 10, which showed higher total dissolved Se concentrations due to evapoconcentration. The percentage of reduced Se forms of total Se was inversely proportional to the percentage of Se(VI) depending on the redox condition of evaporation ponds along the flow paths. Sequential extractions of Se species in sediments indicated that organic associated Se and elemental Se were prevalent forms in sediments in the ponds system. The higher concentrations of elemental Se and organic associated Se in sediments in Cell 1 indicated that the immobilization of Se was active in the sediments compared to Cell 9, while the percentage of both fractions of total Se in sediments in Cells 1 and 9 was relatively constant. The organic materials from algae might provide carbon sources for Se reduction and Se sink in sediments in its elemental and organic associated forms.  相似文献   

13.
The distribution and speciation of Se within aerobic Burkholderia cepacia biofilms formed on α-Al2O3 (1-102) surfaces have been examined using grazing-angle X-ray spectroscopic techniques. We present quantitative information on the partitioning of 10−6 M to 10−3 M selenate and selenite between the biofilms and underlying alumina surfaces derived from long-period X-ray standing wave (XSW) data. Changes in the Se partitioning behavior over time are correlated with microbially induced reduction of Se(VI) and Se(IV) to Se(0), as observed from X-ray absorption near edge structure (XANES) spectroscopy.Selenite preferentially binds to the alumina surfaces, particularly at low [Se], and is increasingly partitioned into the biofilms at higher [Se]. When B. cepacia is metabolically active, B. cepacia rapidly reduces a fraction of the SeO32− to red elemental Se(0). In contrast, selenate is preferentially partitioned into the B. cepacia biofilms at all [Se] tested due to a lower affinity for binding to the alumina surface. Rapid reduction of SeO42− by B. cepacia to Se(IV) and Se(0) subsequently results in a vertical segregation of Se species at the B. cepacia/α-Al2O3 interface. Elemental Se(0) accumulates within the biofilm with Se(VI), whereas Se(IV) intermediates preferentially sorb to the alumina surface.B. cepacia/α-Al2O3 samples incubated with SeO42− and SeO32− when the bacteria were metabolically active result in a significant reduction in the mobility of Se vs. X-ray treated biofilms. Remobilization experiments show that a large fraction of the insoluble Se(0) produced within the biofilm is retained during exchange with Se-free solutions. In addition, Se(IV) intermediates generated during Se(VI) reduction are preferentially bound to the alumina surface and do not fully desorb. In contrast, Se(VI) is rapidly and extensively remobilized.  相似文献   

14.
The vertical distributions of Se (IV), Se (VI) and dissolved organic Se have been determined in the oxic and non-sulfide-bearing anoxic zones of the Orca Basin. In the oxic waters, the concentration of Se (IV) increases with depth gradually from 0.25 nmole/kg at the surface to a maximum of 0.46 nmole/kg at 750 m and then decreases with depth to a relatively constant concentration of 0.39 nmole/ kg below 1,230 m. The concentration of Se (VI) is rather uniform in the top 250 m at about 0.24 nmole/ kg. Below 250 m it increases with depth to 0.50 nmole/kg at 1.230 m, and it stays relatively constant below this depth. The concentration of organic Se increases from 0.50 nmole/kg at the surface to 1.39 nmole/kg at 78 m. A pronounced broad maximum of organic Se exists between 78 and 250 m. The concentration decreases with depth below 250 m, dropping sharply between 250 and 380 m and more gradually at greater depths. It becomes undetectable at 1,230 m. Organic Se is the dominant species above 250 m. Se (IV) is the most abundant between 250 and 1,000 m while Se (VI) becomes the dominant species below 1,000 m. The distributions of these three species can be explained by the biological uptake of Se in the surface waters and the multi-step regeneration of Se from biogenic particles at greater depths. In suboxic waters at the oxic-anoxic interface, the concentration of Se (IV) increases while that of Se (VI) decreases reflecting a change in redox conditions in the environment. In the anoxic brine, the concentration of Se (IV) is around 0.25 nmole/kg while Se (VI) is undetectable. The concentration of organic Se increases sharply in the suboxic waters and reaches 2.6 nmole/kg in the anoxic brines probably as a result of the decomposition of organic matter and/or a diffusive flux from the underlying sediment.  相似文献   

15.
Samples of authigenic material, sediment overlying water and oxic surface sediment (0–0.5-cm depth) from a perennially oxygenated lacustrine basin were analysed to investigate which solid phases are important for binding a suite of trace elements (Ag, As, Ca, Cd, Cu, Hg, In, methylmercury (MeHg), Mg, Mo, Pb, Sb and Zn). The authigenic material, which was collected with inert Teflon sheets deployed for several years across the sediment–water interface, contained mainly poorly crystallized Fe oxyhydroxides and natural organic matter, presumably humic substances derived from the watershed. Manganese oxyhydroxides were not present in the collected authigenic material due to the slightly acidic condition (pH = 5.6) of the lake that prevents the formation and recycling of these compounds. Conditional equilibrium constants for the adsorption of cationic (KFe–M) and anionic (KFe–A) trace elements onto the authigenic Fe oxyhydroxides were estimated from their concentrations in the authigenic material and in bottom water samples. These field-derived values of KFe–M and KFe–A were compared with those predicted by the surface complexation model, using laboratory-derived intrinsic adsorption constants and the water composition at the study site. Equilibrium constants (KPOM–M) were also calculated for the adsorption of the cationic trace elements onto the humic substances contained in the diagenetic material. The field-derived values of KPOM–M were compared to those predicted by the speciation code WHAM 6 for the complexation of the trace elements by dissolved humic substances in the lake. Combining the results of the present study with those on the distributions of trace elements in the porewater and solid-phase sediments reported in previous studies at the same site, it was determined whether the trace elements bind preferentially to Fe oxyhydroxides or natural organic matter in oxic sediments. The main inferences are that the anionic trace elements As, Mo and Sb, as well as the cationic metal Pb are preferentially bound to the authigenic Fe oxyhydroxides whereas the other trace elements, and especially Hg and MeHg, are preferentially bound to the humic substances.  相似文献   

16.
Xuanwu Lake (3.7 km2) is a shallow (mean depth 1.4 m) hypereutrophic lake (annual productivity greater than 600 g cm–2) located in East China's flood plain near the N end of Nanjing, China's ninth largest city. Paleolimnological data based on a 16 cm long sediment core removed from near the center of the lake indicated that nutrient pollution tolerant diatoms have replaced pollution intolerant taxa which were common near the base of the core (approximately 35 years before present). These paleolimnological observations support the hypothesis that progressive eutrophication is occurring in Xuanwu Lake. This conclusion is corroborated by direct comparisons of the present day phytoplankton and zooplankton species composition within the lake and published accounts of its species composition during the mid 1970's.During the last decade, zooplankton density has increased 153% and zooplankton species' richness has declined by 33%. Phytoplankton biomass has increased over 10-fold and the lake's photic zone has decreased to its current (1987) condition (1% surface light intensity at 0.7 m).Xuanwu Lake, like many similar shallow polymictic lakes in E China, has not been depleted of dissolved oxygen near its bottom. This is due to frequent wind mixing, of the entire lake. Thus its progressive hypereutrophication does not result in the same suite of problems experienced by lakes whose hypolimnion is stagnant for long periods of time.  相似文献   

17.
The geochemistry of Se is largely controlled by that of iron, with which Se is closely affiliated in both oxidizing and reducing environments. In aerated waters the Se(IV) oxyanions, HSeO?3 and SeO2?3, are strongly adsorbed by hydrated surfaces of ferric oxides over the pH range 2–8; above pH8 adsorption decreases to complete desorption at pH 11. This adsorption immobilizes Se(IV) in neutral-to-acid waters and increases the range of oxidation potential over which Se(IV) is stable. During experimental aeration of aqueous Fe-S-Se systems, the stability field of Se(IV) is attained and elemental Se is slowly oxidized to this higher valence; oxidation potentials of the Se(VI) stability field were never reached, however, even by continued aeration of an alkaline system. Under reducing conditions, elemental Se either is incorporated within pyrite or forms the mineral ferroselite (FeSe2.Selenium geochemistry is summarized on an Eh-pH diagram, synthesized from equilibrium calculations, experimental work and reported geologic occurrences. A stability field for ferroselite, constructed for a Gibbs free-energy value of ?23.2 kcal/mole, is in accord both with its geologic occurrence and behavior and with conditions under which ferroselite has been synthesized. Traces on this diagram of Eh-pH variation show the behavior of selenium during oxidation of associated iron-sulfide minerals. Such considerations also demonstrate the manner in which selenium migrates, is deposited and is increasingly concentrated in roll-type sandstone uranium deposits, as well as the relative positions of the several forms of selenium within the deposit.  相似文献   

18.
Iron–manganese oxide coatings form on a wide range of geologic samples where they have the ability to adsorb elements and potentially act as a mineral exploration/environmental monitoring tool. In this study, Fe–Mn oxide coatings on stream pebbles were collected from streams in four study areas located across the province of Newfoundland and Labrador, Canada. The study locations were in areas of former copper mines (Tilt Cove and Betts Cove), carbonate geology (Robinsons River), and a metropolitan area (Rennies River). Collected pebbles underwent a simple sample preparation procedure and were then analyzed for a wide range of elements by LA-ICP-MS after optimization of the operating conditions. Water samples accompanied the pebbles, and these were analyzed for pH, dissolved oxygen, conductivity, and a large selection of elements by ICP-MS. Multivariate statistics, in the form of Principal Component Factor Analysis (PCFA) was performed on both data sets. Graphs of the factor scores from the PCFA produced groupings of the samples that were related to geologic/environmental inputs. The loading of variables in each factor was related to the adsorption of the element either to the MnO2 or Fe2O3 phase with most elements except Cr and Cu displaying preferential adsorption to MnO2. Elemental Fe–Mn oxide coating concentrations were a result of the element's affinity (chalcophile, lithophile, or siderophile), pH of the environment, stream water concentration, and amount of each oxide phase present. Even with these complications, LA-ICP-MS analysis of Fe–Mn oxides was able to identify areas of heavy metal pollution and locate geologic inputs.  相似文献   

19.
《Applied Geochemistry》1998,13(2):213-233
Porewater concentration profiles were determined for Fe, trace elements (As, Cd, Co, Cu, Mn, Ni, Pb, Zn), sulfide, SO4 and pH in two Canadian Shield lakes (Chevreuil and Clearwater). Profiles of pyrite, sedimentary trace elements associated with pyrite and AVS were also obtained at the same sites. Thermodynamic calculations are used, for the anoxic porewaters where sulfide was measured, to characterize diagenetic processes involving sulfide and trace elements and to illustrate the importance of sulfide, and possibly polysulfides and thiols, in binding trace elements. The ion activity products (IAP) of Fe sulfide agree with the solubility products (Ks) of greigite or mackinawite. For Co, Ni and Zn, IAP values are close to the KS values of their sulfide precipitates; for Cu and Pb, IAP/Ks indicate large oversaturations, which can be explained by the presence of other ligands (not measured) such as polysulfides (Cu) and thiols (Pb). Cobalt, Cu, Ni and Zn porewater profiles generally display a decrease in concentration with increasing ΣH2S, as expected for transition metals, whereas Cd, Pb and Zn show an increase (mobilisation). The results suggest that removal of trace elements from anoxic porewaters occurs by coprecipitation (As and Mn) with FeS(s) and/or adsorption (As and Mn) on FeS(s), and by formation of discrete solid sulfides (Cd, Cu, Ni, Pb, Zn and Co). Reactive Fe is extensively sulfidized (51–65%) in both lakes, mostly as pyrite, but also as AVS. Similarities between As, Co, Cu and Ni to Fe ratios in pyrite and their corresponding mean diffusive flux ratios suggest that pyrite is an important sink at depth for these trace elements. High molar ratios of trace elements to Fe in pyrite from Clearwater Lake correspond chronologically to the onset of smelting activities. AVS can be an important reservoir of reactive As, Cd and Ni and, to a lesser extent, of Co, Cu and Pb. Overall, the trace elements most extensively sulfidized were Ni, Cd and As (maximum of 100%, 81% and 49% of the reactive fraction, respectively), whereas Co, Cu, Mn, Pb and Zn were only moderately sulfidized (11–16%).  相似文献   

20.
Polonium, like other elements in the Group VI Oxygen series (S, Se, Te), has the potential to form volatile alkyl derivatives. This may be evident in its pervasive radioactive excesses in the atmosphere and coastal waters, and its deficiency in surface open ocean waters. We present evidence for the formation of volatile polonium species. The first evidence comes from duplicating experiments that proved the existence of volatile tellurium, its Group VI congener. Cultures of bread mold at room temperature spiked with polonium tracers showed a significant and reproducible loss of about 0.5% per day of volatile polonium species. In another set of experiments, between 30–50% loss of210Po was observed from Floridan groundwater when nitrogen was bubbled through it over durations of 5–30 minutes. Polonium volatility is highly relevant for biogeochemical studies because it may provide a natural radiochemical tracer for recycling of similar volatile sulfur and other Group VI metal species between the geosphere, atmosphere, and hydrosphere.  相似文献   

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