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1.
In situ measured microprofiles of Ca2+, pCO2, pH and O2 were performed to quantify the CaCO3 dissolution and organic matter mineralization in marine sediments in the eastern South Atlantic. A numerical model simulating the organic matter decay with oxygen was used to estimate the calcite dissolution rate. From the oxygen microprofiles measured at four stations along a 1300-m isobath of the eastern African margin and one in front of the river Niger at a water depth of 2200 m the diffusive oxygen uptake (DOU) and oxygen penetration depth (OPD) was calculated. DOU rates were in the range of 0.3 to 3 mmol m−2 d−1 and showed a decrease with increasing water depth, corresponding to an increase in OPD. The calculated amount of degradated organic matter is in the range of 1 to 8.5 gC m−2 a−1. The metabolic CO2, released from mineralization of the organic matter drives calcite dissolution in these sediments overlain by calcite-supersaturated water. Fluxes across the sediment water interface calculated from the in situ Ca2+ microprofiles were 0.6 mmol m−2 d−1 for two stations at a water depth of 1300 m. The ratio of calcite dissolution flux and organic C degradation is 0.53 and 0.97, respectively. The microprofiles indicate that CO2 produced within the upper oxic sediment layer dissolves up to 85% of the calcite rain to the seafloor. Modeling our O2, pH and Ca2+ profiles from one station predicted a calcite dissolution rate constant for this calcite-poor site of 1000 mol kgw−1 a−1 (mol per kg water and year), which equals 95% d−1. This rate constant is at the upper end of reported in situ values.  相似文献   

2.
The biomarker composition and stable isotope (C, O) ratio values of organic matter (OM) and carbonate from sediment cores from the oligotrophic Lake Brienz and the eutrophic Lake Lugano (both in Switzerland) are compared, in order to obtain information about OM sources and transformation processes. Eutrophic conditions at Lake Lugano are reflected in elevated total organic carbon (TOC) content and hydrogen index (HI) values, as well as higher lipid concentrations. Parallel down core trends in δ13C values of TOC and calcite in the Lake Lugano sediments reflect bioproductivity cycles. Variations in δ18O values of calcite are consistent with changes in mean summer temperature over the time interval covered by the core. In contrast, such a correlation does not exist for Lake Brienz and there the stable isotope composition of calcite reflects its allochthonous origin. In the sediments of both lakes, fatty acid (FA) distributions and the composition of n-alkanols and n-alkanes indicate highly variable proportions of autochthonous OM sources (algae, zooplankton, bacteria) and OM from land plants. Enhanced in situ microbial synthesis during sediment deposition in Lake Lugano is suggested by the higher TOC-normalised concentrations of branched chain FAs (C15–C17), hopanoic acids and triterpenoid alcohols (i.e. tetrahymanol, diplopterol). Variations in the concentrations of cholesterol are related to contributions from zooplankton and/or green algae, while sitosterol concentrations reflect the input of vascular plants. Periods of increased input of OM from diatoms are evidenced by high 24-methylcholesta-5,22-dien-3β-ol (either epibrassicasterol or brassicasterol) and/or highly branched isoprenoid (HBI) alkenes concentrations. High relative concentrations of diplopterol in Lake Lugano sediments are consistent with the predominance of cyanobacteria commonly observed in eutrophic lakes. The presence of archeol and hydroxyarcheol in very low concentrations in the Lugano sediments argues for the activity of methanogens and/or anaerobic methanotrophs.Differences in OM degradation processes are reflected in higher chlorin index values in the Brienz sediments but higher saturated vs. unsaturated n-FAs in the core from Lugano. Higher concentrations of branched chain FAs and 16:1ω7 n-FA, as well as enhanced 18:1ω7/18:1ω9 n-FA, are consistent with enhanced bacterial biomass in the Lugano water column or sediments. The preservation of phytol seems to be enhanced in sediments with a high relative contribution of land plant OM. Major factors affecting OM accumulation in the lakes are differences in OM sources (i.e. terrestrial OM vs. autochthonous production), extent of bacterial activity and most likely oxygen availability in the water column.  相似文献   

3.
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   

4.
Methane produced in anoxic organic-rich sediments of Cape Lookout Bight, North Carolina, enters the water column via two seasonally dependent mechanisms: diffusion and bubble ebullition. Diffusive transport measured in situ with benthic chambers averages 49 and 163 μmol · m ?2 · hr ?1 during November–May and June–October respectively. High summer sediment methane production causes saturation concentrations and formation of bubbles near the sediment-water interface. Subsequent bubble ebullition is triggered by low-tide hydrostatic pressure release. June–October sediment-water gas fluxes at the surface average 411 ml (377 ml STP: 16.8 mmol) · m?2 per low tide. Bubbling maintains open bubble tubes which apparently enhance diffusive transport. When tubes are present, apparent sediment diffusivities are 1.2–3.1-fold higher than theoretical molecular values reaching a peak value of 5.2 × 10?5 cm2 · sec?1. Dissolution of 15% of the rising bubble flux containing 86% methane supplies 170μmol · m?2 · hr?1 of methane to the bight water column during summer months; the remainder is lost to the troposphere. Bottom water methane concentration increases observed during bubbling can be predicted using a 5–15 μm stagnant boundary layer dissolution model. Advective transport to surrounding waters is the major dissolved methane sink: aerobic oxidation and diffusive atmospheric evasion losses are minor within the bight.  相似文献   

5.
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   

6.
《Applied Geochemistry》2000,15(4):425-438
The dissolution of silica and diffusion of reactive dissolved Si in the porewaters of river sediments are investigated using sediments of different physical and chemical properties. Three sediments are considered: (a) from sectioned cores taken from a river-bed, (b) fine organic-rich surface sediment (<5 cm depth) installed in a fluvarium channel and, (c) coarse river sediment of low organic matter content also installed in a fluvarium channel. Dissolution rates of silica are measured at 10°C using batches of suspended material. The derived dissolution rate constants show large differences between the sediments. The river bed-sediment cores had vertical concentration profiles of dissolved Si that are consistent with the diffusion and dissolution of biogenic silica. Experiments in a fluvarium channel enabled Si fluxes to be calculated from a mass-balance of the overlying solution. The results are consistent with the attainment of a steady-state concentration profile of dissolved Si in the sediment. There are no discernible effects of water velocity over the sediment between 5 and 11 cm s−1. However, at 20 cm s−1, the flux increases as a result of either entrainment of fine particles at the surface or advective effects in the surface sediment. A fluvarium experiment with the fine sediment (<125 μm) over 61 days, produced a concentration profile with the highest concentration of 1025 μmol dm−3 at a depth of 4–5 cm in the sediment. A FORTRAN program is used to model the results of the increase in dissolved Si in the overlying water and development of a concentration profile in the porewater. This leads to a sediment diffusion coefficient of 1.21×10−9 m2 s−1 at 8.8°C at the beginning of the experiment and rate constant k=13.1×10−7 s−1 at pH=7.82 and average temperature of 7.6°C for the entire experiment. Fluxes measured at the sediment–surface interface and calculated assuming steady-state profiles had developed are typically 0.01–0.04 μmol m−2 (of river bed) s−1. The approach enables the efflux of dissolved Si from bottom-sediments to be estimated from dissolution rates measured using suspensions of bed-sediment.  相似文献   

7.
A 2-year (October 2003–October 2005) high-resolution sediment trap study was conducted in Sacrower See, a dimictic hardwater lake in northeastern Germany. Geochemical and diatom data from sediment trap samples were compared with a broad range of limnological and meteorological parameters to quantify the impact of single parameters on biochemical calcite precipitation and organic matter production. Our goals were to disentangle how carbonaceous varves and their sublaminae form during the annual cycle to better understand the palaeorecords and to detect influences of dissolution, resuspension as well as of global radiation and stratification on lake internal particle formation. Total particle fluxes in both investigated years were highest during spring and summer. Sedimentation was dominated by autochthonous organic matter and biochemically precipitated calcite. Main calcite precipitation occurred between April and July and was preceded and followed by smaller flux peaks caused by resuspension during winter and blooms of the calcified green algae Phacotus lenticularis during summer. In some of the trap intervals during summer up to 100% of the precipitated calcite was dissolved in the hypolimnion. High primary production due to stable insolation conditions in epilimnic waters began with stratification of the water column. Start and development of stratification is closely related to air and water surface temperatures. It is assumed that global radiation influences the onset and stability of water column stratification and thereby determining the intensity of primary production and consequently of timing and amount of calcite precipitation which is triggered by phytoplanktonic CO2 consumption. Sediment fluxes of organic matter and calcite are also related to the winter NAO-Index. Therefore these fluxes will be used as a proxy for ongoing reconstruction of Holocene climate conditions.  相似文献   

8.
Physiochemical controls on the carbonate geochemistry of large river systems are important regulators of carbon exchange between terrestrial and marine reservoirs on human time scales. Although many studies have focused on large-scale river carbon fluxes, there are few investigations of mechanistic aspects of carbonate mass balance and transport at the catchment scale. We determined elemental and carbonate geochemistry and mass balances for net carbonate dissolution fluxes from the forested, mid-latitude Huron River watershed, established on carbonate-rich unconfined glacial drift aquifers. Shallow groundwaters are near equilibrium with respect to calcite at pCO2 values up to 25 times atmospheric values. Surface waters are largely groundwater fed and exhibit chemical evolution due to CO2 degassing, carbonate precipitation in lakes and wetlands, and anthropogenic introduction of road salts (NaCl and CaCl2). Because the source groundwater Mg2+/HCO3 ? ratio is fairly constant, this parameter permits mass balances to be made between carbonate dissolution and back precipitation after groundwater discharge. Typically, precipitation does not occur until IAP/K calcite values exceed 10 times supersaturation. Stream chemistry changes little thereafter even though streams remain highly supersaturated for calcite. Our data taken together with historical United States Geological Survey (USGS) data show that alkalinity losses to carbonate precipitation are most significant during periods of lowest discharge. Thus, on an annual basis, the large carbon flux from carbonate dissolution in soil zones is only decreased by a relatively small amount by the back precipitation of calcium carbonate.  相似文献   

9.
《Applied Geochemistry》1998,13(2):257-268
We report the hydrogeochemical modeling of a complicated suite of reactions that take place during the oxidation of pyrite in a marine sediment. The sediment was equilibrated in a column with MgCl2 solution and subsequently oxidized with H2O2. The oxidation of pyrite triggers dissolution of calcite, cation and proton exchange, and CO2 sorption. The composition of the column effluent was modeled with PHREEQC, a hydrogeochemical transport model. The model was extended with a formal ID transport module which includes dispersion and diffusion. The algorithm solves the advection-reaction-dispersion equation with explicit finite differences in a split-operator scheme. Also, kinetic reactions for pyrite oxidation, calcite dissolution and precipitation, and organic C oxidation were included. Kinetic relations for pyrite oxidation and calcite dissolution were taken from the literature, and a coefficient equivalent to the ratio A/V (surface over volume), was adjusted to fit the experimental data. The comparison of model and experiment shows that ion exchange and sorption are dominant chemical processes in regulating and buffering water quality changes upon the oxidation of pyrite. Cation exchange was assigned to the colloidal fraction ( < 2 μm) and deprotonated organic matter, proton buffering to organic matter, and CO2 sorption to amorphous Fe-oxyhydroxide. These processes have been neglected in earlier modeling studies of pyrite oxidation in natural sediments.  相似文献   

10.
At burial depths of 800-1000 m, within the epicontinental Queensland Trough of north-east Australia (ODP Site 823), microcrystalline inter- and intraskeletal mosaics of anhedral (loaf-shaped, rounded) calcite have Sr2+ values ranging from below microprobe detection limits (<150 ppm) to 8100 ppm. Host rocks are well lithified, fine-grained mixed sediment to clayey wackestone and packstone of Middle and Late Miocene age. Petrography demonstrates that calcite precipitation has spanned shallow to deep burial, overlapping formation of framboidal pyrite in the upper 50 m; shallow-burial dolomitization (<300 m); and dedolomitization during sediment consolidation and incipient chemical compaction at greater (>400–500 m) depths. Petrographic observations illustrate that the calcite microfabric formed through coalescing crystal growth resulting from one or a combination of displacive growth in clay, porphyroid neomorphism of aragonite/vaterite, and clay replacement by calcite. Sr2+ mean concentrations in calcite between depths of 800 and 1000 m are similar to an expected equilibrium pore-water concentration, using a Dsr of 0.06, and may indicate active calcite precipitation. However, Sr2+ variation (2000–5000 ppm) within and among crystals, and concentrations that range well above predicted equilibrium values for a given depth, illustrate either variable Sr2+ retention during recrystallization of shelf-derived aragonite (and authigenic local vaterite) or relative uptake of Sr2+ during calcite precipitation with burial. Within the context of calcite formation during burial to 1 km, diagenetic attributes that affect the latter process include increased concentrations of pore-water Sr2+ with depth associated with aragonite recrystallization/dissolution; upward migration of Sr-rich pore water; and increased DSr related to local variation in precipitation/recrystallization rates, differential crystal sector growth rates and/or microvariation in aragonite distribution.  相似文献   

11.
《Applied Geochemistry》2003,18(9):1497-1506
Sedimentation and benthic release of As was determined in Baldeggersee, a eutrophic lake in central Switzerland. Sediment traps recorded As sedimentation during 1994, including a flood event in spring. Diagenetic processes were studied using porewater profiles at the sediment–water interface and in deeper sediment strata deposited in the mesotrophic lake (before 1885). Sediment cores were used to calculate the accumulation and to construct the balance of sedimentation and remobilisation. The results showed that the lake sediment acts as an efficient sink for As. Only 22% of the particulate As flux reaching the sediment surface was remobilised at the sediment–water interface. The As accumulation in the recent varved section of the eutrophic lake was 40 mg As m−2 a−1. Iron reduction in older sediment caused a remobilisation of 1.2 mg As m−2 a−1. This upward flux from the deeper sediment was quantitatively immobilised in the recent sulfidic sediments. The flood event in spring contributed about 34% of the yearly sediment load and led to distinct peak profiles of dissolved As in the porewater. This evidence for rapid remobilisation disappeared within months.  相似文献   

12.
发生在沉积物-水界面的剧烈生物地球化学作用对沉积物和上覆水体具重要的环境效应，然而此方面研究很少。本文通过云贵高原四个湖泊湖水和孔隙水NH和NO剖面，沉积物柱芯不同结合态氮含量剖面分布，界面扩散通量，影响氮循环的因素及它们季节性变化规律等的对比研究，初步揭示了湖泊沉积物一水界面的氮循环及其环境效应。  相似文献   

13.
During the anaerobic decomposition of organic matter in sediments iodine is released into solution. Three techniques have been applied to independently estimate the resulting flux of soluble I from the sediments to the overlying water of Mud Bay, Georgetown, South Carolina. Flux estimates (summer) range between ~ 5 and 41 μmol/m2/day. The estimates predicted from either the pore water I concentration gradient across the sediment-water interface or the dissolved I production rate are higher than the apparent flux measured directly at the same site. This suggests that I which is released to the pore water under the anoxic conditions below the sediment surface reacts with a sedimentary component at or near the sediment water interface and is lost from solution.  相似文献   

14.
We present a numerical model to quantify calcite dissolution in the guts of deposit feeding invertebrates. Deposit feeder guts were modeled as constantly stirred reactors (CSTRs) following terminology from digestion theory. Saturation state and dissolution of calcium carbonate were calculated from changes in total dissolved carbon dioxide and alkalinity resulting from sediment passage through the digestive tract, while accounting for dissolution of calcite and respiration of organic carbon. Typical dissolution rates for a gut volume of 1 ml ranged between 0.5-4 mg calcite d−1. Sensitivity analysis revealed gut pH, sediment organic matter (OM) content and OM reactivity to be the critical parameters determining calcite dissolution rate. Carbonate dissolution rate was inversely related to gut pH. However, calcite dissolution was found to be possible even at alkaline gut pH due to respiration by intestinal microbes. The kinetics of calcite dissolution had only marginal influence on daily calcite dissolution rates: Varying the calcite dissolution rate constant κ by six orders of magnitude affected calcite dissolution rates by less than a factor of 10. Calcite dissolution rates were calculated for 4 different hydrographic regimes that differed in their content of sedimentary calcite and OM and furthermore in their OM reactivity. Highest dissolution rates were calculated for the shallow water setting, where relatively high OM content facilitated high microbial respiration rates depressing gut pH. However, dissolution rates for the deep sea setting were only slightly lower, due to greatly elevated ingestion rates resulting from low OM content. As a consequence of much higher faunal abundances, shallow-water benthos is likely to contribute the vast majority of gut-mediated carbonate dissolution. Nevertheless, the fraction of sedimentary calcite that dissolves during one gut passage is probably too small to be observable by simple gravimetric analysis. This may explain the notable scarcity of evidence for gut-mediated carbonate dissolution in the literature to date. Assuming depth-dependent calcite dissolution rates and deposit feeder abundances, we estimate gut-mediated carbonate dissolution to contribute approximately 5% of the annual global sedimentary carbonate dissolution rate, which corresponds to an average calcite dissolution rate of approximately 0.5 mg m−2 d−1 for the entire ocean floor.  相似文献   

15.
The biogeochemistry of iron sulfide minerals in the water column of the Cariaco Basin was investigated in November 2007 (non-upwelling season) and May 2008 (upwelling season) as part of the on-going CARIACO (CArbon Retention In A Colored Ocean) time series project. The concentrations of particulate sulfur species, specifically acid volatile sulfur (AVS), greigite, pyrite, and particulate elemental sulfur, were determined at high resolution near the O2/H2S interface. In November 2007, AVS was low throughout the water column, with the highest concentration at the depth where sulfide was first detected (260 m) and with a second peak at 500 m. Greigite, pyrite, and particulate elemental sulfur showed distinct concentration maxima near the interface. In May 2008, AVS was not detected in the water column. Maxima for greigite, pyrite, and particulate elemental sulfur were again observed near the interface. We also studied the iron sulfide flux using sediment trap materials collected at the Cariaco station. Pyrite comprised 0.2-0.4% of the total particulate flux in the anoxic water column, with a flux of 0.5-1.6 mg S m−2 d−1.Consistent with the water column concentration profiles for iron sulfide minerals, the sulfur isotope composition of particulate sulfur found in deep anoxic traps was similar to that of dissolved sulfide near the O2/H2S interface. We conclude that pyrite is formed mainly within the redoxcline where sulfur cycling imparts a distinct isotopic signature compared to dissolved sulfide in the deep anoxic water. This conclusion is consistent with our previous study of sulfur species and chemoautotrophic production, which suggests that reaction of sulfide with reactive iron is an important pathway for sulfide oxidation and sulfur intermediate formation near the interface. Pyrite and elemental sulfur distributions favor a pathway of pyrite formation via the reaction of FeS with polysulfides or particulate elemental sulfur near the interface. A comparison of thermodynamic predictions with actual concentration profiles for iron sulfides leads us to argue that microbes may mediate this precipitation.  相似文献   

16.
The coastal upwelling system off central Namibia is one of the most productive regions of the oceans and is characterized by frequently occurring shelf anoxia with severe effects for the benthic life and fisheries. We present data on water column dissolved oxygen, sulfide, nitrate and nitrite, pore water profiles for dissolved sulfide and sulfate,35S-sulfate reduction rates, as well as bacterial counts of large sulfur bacteria from 20 stations across the continental shelf and slope. The stations covered two transects and included the inner shelf with its anoxic and extremely oxygen-depleted bottom waters, the oxygen minimum zone on the continental slope, and the lower continental slope below the oxygen minimum zone. High concentrations of dissolved sulfide, up to 22 mM, in the near-surface sediments of the inner shelf result from extremely high rates of bacterial sulfate reduction and the low capacity to oxidize and trap sulfide. The inner shelf break marks the seaward border of sulfidic bottom waters, and separates two different regimes of bacterial sulfate reduction. In the sulfidic bottom waters on the shelf, up to 55% of sulfide oxidation is mediated by the large nitrate-storing sulfur bacteria, Thiomargarita spp. The filamentous relatives Beggiatoa spp. occupy low-O2 bottom waters on the outer shelf. Sulfide oxidation on the slope is apparently not mediated by the large sulfur bacteria. The data demonstrate the importance of large sulfur bacteria, which live close to the sediment-water interface and reduce the hydrogen sulfide flux to the water column. Modeling of pore water sulfide concentration profiles indicates that sulfide produced by bacterial sulfate reduction in the uppermost 16 cm of sediment is sufficient to account for the total flux of hydrogen sulfide to the water column. However, the total pool of hydrogen sulfide in the water column is too large to be explained by steady state diffusion across the sediment-water interface. Episodic advection of hydrogen sulfide, possibly triggered by methane eruptions, may contribute to hydrogen sulfide in the water column.  相似文献   

17.
Geochemical controls on a calcite precipitating spring   总被引：2，自引：0，他引：2  
A small spring fed stream was found to precipitate calcite by mainly inorganic processes and in a nonuniform manner. The spring water originated by rainwater falling in a 0.8 km2 basin, infiltrating, and dissolving calcite and dolomite followed by dissolution of gypsum or anhydrite. The Ca2+/Mg2+ indicates that calcite is probably precipitated in the subsurface from a supersaturated solution. This water emerges from the spring still about 5 times supersaturated with respect to calcite and continues calcite precipitation. When 10 times supersaturation is reached, due to CO2 degassing the precipitation is more rapid. The calcite accumulation from the stream with a flow of 5 l/s is calculated to be 12600 kg/yr with the highest rates in areas where CO2 degassing is the greatest. The non-equilibrium, as shown by the high calcite supersaturation, is also reflected in a variable partitioning pattern for Sr2+ between the water and calcite.  相似文献   

18.
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   

19.
Biomarker compositions of particulate organic matter (POM) from the oligotrophic Lake Brienz and the eutrophic Lake Lugano (both Switzerland) are compared, in order to obtain information about organic matter (OM) production and transformation processes in relation to water column stratification. Eutrophic conditions in Lake Lugano are reflected by enhanced alkalinity, elevated total organic carbon (TOC) and chlorin contents compared with Lake Brienz. Lower δ13C values of dissolved inorganic carbon (DIC) in Lake Lugano reflect enhanced OM respiration in the water column.Differences in OM dynamics between both lakes, as well as seasonal variations, are evidenced by TOC-normalised concentration profiles of total fatty acids (FAs) and total neutrals. In Lake Brienz, the results reflect the relative contributions of primary productivity and refractory, allochthonous OM to POM, governed by particle load and interflows due to density stratification. The depth trends at Lake Lugano are a result of high primary productivity, water column stratification and associated particle load in the upper layers, as well as microbially induced degradation close to the chemocline and greater preservation under anoxic conditions. Minor differences exist with regard to the OM composition. In both lakes, FA distributions and the composition of n-alkanols indicate a predominant autochthonous OM source (algae, zooplankton, bacteria). Inputs of OM from diatoms are reflected in highly-branched isoprenoid (HBI) alkenes, 16:1 n-FAs and 24-methylcholesta-5,22-dien-3β-ol (either epibrassicasterol or brassicasterol). Differences in relative proportions of n-C16 vs. n-C18 FAs and alkanols, respectively, as well as in the percentages of C27, C28 and C29 sterols relative to the sum of sterols are related to differences in the abundances of chrysophytes, diatoms and green algae within the euphotic zone of both lakes as well as in bacterial activity and soil in-wash. High relative proportions of cholesterol in the autumn samples, most pronounced at Lake Lugano, were attributed to an increased input from zooplankton grazing in the water column.Differences in OM degradation processes are reflected in slightly higher chlorin index values and higher relative proportions of saturated vs. unsaturated n-FAs in Lake Lugano. Higher contents of branched chain FAs, 16:1ω7 n-FA, and enhanced 18:1ω7/18:1ω9 n-FA ratios suggest enhanced bacterial biomass in the water column of Lake Lugano close to the chemocline. Increasing proportions of saturated n-FAs and n-alkanols with increasing water depth, most distinct in the autumn for both lakes, argue for intensified bacterial activity and degradation of OM during autumn. High relative contents of sterols and low n-alkanol concentrations in POM close to the chemocline at Lake Lugano during spring are interpreted to reflect higher primary productivity in the photic zone, OM export to the deeper parts and enhanced degradation rates of more labile constituents (i.e. C13–C20 n-alkanols), as compared to Lake Brienz.  相似文献   

20.
The release of remineralized N and P from the organic-rich anoxic sediments of Cape Lookout Bight is controlled by processes occurring within the sediment column and at the sediment-water interface. The relatively rapid rates of temperature dependent microbial degradation of organic matter support seasonally varying nutrient fluxes ranging from 20 to 1200 μmol·m?2·hr?1 for dissolved ammonium and from ? 20 to 120 μmol·m?2·hr?1 for total dissolved phosphate (measured in situ over the period October, 1976 to October, 1978). Molecular diffusion along steep vertical pore water concentration gradients measured simultaneously cannot explain the high fluxes observed during warmer months. Gradients for ammonium and phosphate ranged from 0.33 to 1.10 and from 0 to 0.29 μmol·cm?3pw·cm?1s respectively. These high summertime fluxes appear to result from increased sediment-water transport associated with bubble tubes created and maintained by low-tide methane gas bubble ebullition. When these tubes are present, apparent bulk sediment diffusivities calculated from concurrent studies of methane and radon-222 sediment-water exchange are 1.0–3.1 times greater than molecular diffusivities. Nutrient fluxes calculated via Fick's first law taking into account this enhanced transport and the differential diffusive mobilities of dissolved ammonium, phosphate and phosphate ion pairs indicate that removal by aerobic adsorption and/or biological uptake at the sediment-water interface plays an important role in controlling nutrient exchange in these sediments.  相似文献   

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