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1.
Lake Constance is one of Europe’s largest oligotrophic lakes and provides a water source for more than 4.5 million people in Germany and Switzerland. We present here a 12 month study on iodine concentrations, speciation and fluxes to and from the lake to gain a quantitative understanding of the limnic iodine cycle. Monthly water samples were obtained from all major tributaries (14) and the outflow to construct a mass-balance model. Sediment traps were also deployed in the lake for two years at two different stations. Total soluble iodine (TSI) in aqueous samples were analysed by ICP-MS and speciation (iodide, iodate and soluble organically bound iodine, SOI) by ion chromatography-ICP-MS. Iodine concentrations in the Alpine tributaries (1-2 μg l−1) decreased over the summer months due to increasing proportions of snow and glacial melt water from the Alps, while iodine levels in the lowland rivers (∼2-10 μg l−1) increased over the summer. Deposition of TSI to the catchment (16,340 kg I yr−1) was similar to the TSI out-flux by rivers (16,000 kg I yr−1). By also including the particulate riverine iodine flux out of the catchment (∼12,350 kg I yr−1) it is shown that the catchment is a net source of iodine, with the highest particulate fluxes coming from the Alpine rivers. The total TSI flux to the lake was 16,770 kg I yr−1, the largest proportion coming from the Alpenrhein (43%), followed by the Schussen (8%) and Bregenzer Ach (7.7%). Overall the mass-balance for TSI in the lake was negative, with more iodine flowing out of the lake than in (−2050 kg I yr−1; 12% of TSI in-flux). To maintain mass-balance, 8.8 μg I m−2 d−1 from the Obersee and 23 μg I m−2 d−1 from the Untersee must be released from the sediments into the water column. Thus, in comparison with the total iodine flux to the sediments measured by the sediment traps (4762-8075 kg I yr−1), up to 39% of the deposited iodine may be mobilised back into the lake. SOI was the dominant iodine fraction entering the lake, with a total flux of 10,290 kg I yr−1 (64% of TSI input), followed by iodate (3120 kg I yr−1) and iodide (2760 kg I yr−1). Net formation of SOI from iodide and iodate was also noted within the lake, with an estimated production of 6560 kg I yr−1, suggesting a strong role for biology in iodine cycling. In conclusion, organically bound iodine was the dominant iodine species in aqueous and solid phases in Lake Constance, despite low DOC concentrations (<2 mg l−1), and thus is expected to play an important role in iodine cycling in most freshwater environments.  相似文献   

2.
Numerous studies of weathering fluxes have been carried out on major world rivers during the last decade, to estimate CO2 consumption rates, landscape evolution and global erosion rates. For obvious logistical reasons, most of these studies were based on large scale investigations carried out on short timescales. By comparison, much less effort has been devoted to long term monitoring, as a means to verify the temporal variability of the average characteristics, their trends, and the representativeness of short-term investigations. Here we report the results of a three-year survey (November 2000 to December 2003) of the major and trace element composition of dissolved and suspended matter in the lower Rhone River (France), the largest river of the Mediterranean area. Subsurface water samples were collected in Arles, about 48 km upstream of the estuary, twice a month routinely, and at higher frequency during flood events.During each flood event, the suspended particulate matter (SPM) show the usual trend of clockwise hysteresis with higher SPM concentrations on the rising limb of the flood than at the same discharge on the falling limb. We show that the annual average SPM flux of the Rhone River to the Mediterranean Sea (7.3 ± 0.6 × 106 tons yr−1) was largely controlled by the flood events (83% of the solid discharge occurred in less than 12% of the time), and that the precision on the total output flux depends strongly on the precise monitoring of SPM variations during the floods.The chemical composition of water and SPM are characterized by the predominance of Ca2+ due to the abundance of carbonate rocks in the Rhone watershed. Chemical budgets have been calculated to derive the contributions of atmospheric deposition, carbonate, silicate and evaporite weathering, and anthropogenic inputs. The chemical weathering rate of carbonates is estimated to be 89 ± 5 t km−2 yr−1 compared to 14.4 ± 3 t km−2 yr−1 from silicates. By contrast, the physical erosion rate of silicates is about 51 t km−2 yr−1 against 19 t km−2 yr−1 for carbonates.The steady-state model of Gaillardet et al. (1995) has been applied to the chemical composition of dissolved and solid products. The results show that the Rhone River currently exports much less material than produced at steady-state by weathering in its watershed. The sediment flux inferred from the steady-state calculation (21-56 × 106 t yr−1) is on the same order as that estimated in literature for the 19th and the beginning of the 20th centuries. This imbalance may suggest that the Rhone is under a transient erosion regime following climate change (i.e. significant decrease of the flooding frequency since the beginning of the 19th century). On the other hand, the imbalance may also be due to the trapping of alluvion by the numerous dams on the river and its tributaries.Our data corroborate with previous studies that suggest a strong coupling between chemical and physical erosion fluxes, during the hydrological seasonal cycle of the Rhone River. The correlation between physical and chemical transport rates is, however, clearly different from that reported for global annual averages in large world rivers.  相似文献   

3.
In this study we evaluate the dynamics of the biophile element phosphorus (P) in the catchment and proglacial areas of the Rhône and Oberaar glaciers (central Switzerland). We analysed erosion and dissolution rates of P-containing minerals in the subglacial environment by sampling water and suspended sediment in glacier outlets during three ablation and two accumulation seasons. We also quantified biogeochemical weathering rates of detrital P in proglacial sedimentary deposits using two chronosequences of samples of fresh, suspended, material obtained from the Oberaar and Rhône water outlets, Little-Ice-Age (LIA) moraines and Younger Dryas (YD) tills in each catchment. Subglacial P weathering is mainly a physical process and detrital P represents more than 99% of the precipitation-corrected total P denudation flux (234 and 540 kg km−2 yr−1 for the Rhône and Oberaar catchments, respectively). The calculated detrital P flux rates are three to almost five times higher than the world average flux. The precipitation-corrected soluble reactive P (SRP) flux corresponds to 1.88-1.99 kg km−2 yr−1 (Rhône) and 2.12-2.44 kg km−2 yr−1 (Oberaar), respectively. These fluxes are comparable to those of tropical rivers draining transport-limited, tectonically inactive weathering areas.In order to evaluate the efficiency of detrital P weathering in the Rhône and Oberaar proglacial areas, we systematically graded apatite grains extracted from the chronosequence in each catchment relative to weathering-induced changes in their surface morphologies (grades 1-4). Fresh apatite grains are heavily indented and dissolution rounded (grade 1). LIA grains from two 0-10 cm deep moraine samples show extensive dissolution etching, similar to surface grains from the YD profile (mean grades 2.7, 3.5 and 3.5, respectively). In these proglacial deposits, the weathering front deepens progressively as a function of time due to biocorrosion in the evolving acidic pedosphere, with mechanical indentations on grains acting as sites of preferential dissolution. We also measured iron-bound, organic and detrital P concentrations in the chronosequence and show that organic and iron-bound P has almost completely replaced detrital P in the top layers of the YD profiles. Detrital P weathering rates are calculated as 310 and 280 kg km−2 yr−1 for LIA moraines and 10 kg km−2 yr−1 for YD tills. During the first 300 years of glacial sediment exposure P dissolution rates are shown to be approximately 70 times higher than the mean global dissolved P flux from ice-free continents. After 11.6 kyr the flux is 2.5 times the global mean. These data strengthen the argument for substantial changes in the global dissolved P flux on glacial-interglacial timescales. A crude extrapolation from the data described here suggests that the global dissolved P flux may increase by 40-45% during the first few hundred years of a deglaciation phase.  相似文献   

4.
Estimates of glacial sediment delivery to the oceans have been derived from fluxes of meltwater runoff and iceberg calving, and their sediment loads. The combined total (2900 Tg yr−1) of the suspended sediment load in meltwaters (1400 Tg yr−1) and the sediment delivered by icebergs (1500 Tg yr−1) are within the range of earlier estimates. High-resolution microscopic observations show that suspended sediments from glacial meltwaters, supraglacial, and proglacial sediments, and sediments in basal ice, from Arctic, Alpine, and Antarctic locations all contain iron (oxyhydr)oxide nanoparticles, which are poorly crystalline, typically ∼5 nm in diameter, and which occur as single grains or aggregates that may be isolated or attached to sediment grains. Nanoparticles with these characteristics are potentially bioavailable. A global model comparing the sources and sinks of iron present as (oxyhydr)oxides indicates that sediment delivered by icebergs is a significant source of iron to the open oceans, beyond the continental shelf. Iceberg delivery of sediment containing iron as (oxyhydr)oxides during the Last Glacial Maximum may have been sufficient to fertilise the increase in oceanic productivity required to drawdown atmospheric CO2 to the levels observed in ice cores.  相似文献   

5.
The distribution and speciation of mercury (Hg) in the water column, the inputs (wet deposition and tributaries) and the outputs (atmospheric evasion and outlet) of an artificial partially anoxic tropical lake (Petit-Saut reservoir, French Guiana) were investigated on a seasonal basis in order to appraise the cycling and transformations of this metal. The total mercury (HgT) concentrations in the oxygenated epilimnetic waters averaged 5 ± 3 pmol L−1 in the unfiltered samples (HgTUNF) and 4 ± 2 pmol L−1 in the dissolved (HgTD) phase (<0.45 μm). On average, the monomethylmercury (MMHg) constituted 8%, 40% and 18% of the HgT in the dissolved phase, the particulate suspended matter and in the unfiltered samples, respectively. Covariant elevated concentrations of particulate MMHg and chlorophyll a in the epilimnion suggest that phytoplankton is an active component for the MMHg transfer in the lake. In the anoxic hypolimnion the HgTUNF averages 13 ± 6 pmol L−1 and the HgTD 8 ± 4 pmol L−1. The averages of MMHgP and MMHgD in hypolimnetic waters were two and three times the corresponding values of the epilimnion, 170 ± 90 pmol g−1 and 0.9 ± 0.5 pmol L−1, respectively. In the long dry and wet seasons, at the flooded forest and upstream dam sampling stations, the vertical profiles of MMHgD concentrations accounted for two distinct maxima: one just below the oxycline and the other near the benthic interface. Direct wet atmospheric deposition accounted for 14 moles yr−1 HgTUNF, with 0.7 moles yr−1 as MMHgUNF, while circa 76 moles yr−1 of HgTUNF, with 4.7 moles yr−1 as MMHgUNF, coming from tributaries. Circa 78 moles (∼17% as MMHg) are annually exported through the dam, while 23 moles yr−1 of Hg0 evolve in the atmosphere. A mass balance calculation suggests that the endogenic production of MMHgUNF attained 8.1 moles yr−1, corresponding to a methylation rate of 0.06% d−1. As a result, the Petit-Saut reservoir is a large man-made reactor that has extensively altered mercury speciation in favor of methylated species.  相似文献   

6.
A mass balance has been calculated for the elements Li, B, and Sr in the Gulf of Papua from sampling undertaken during 1993 to 1999. Parameters measured included Fly, Kikori, and Purari River inputs of dissolved and particulate phases, removal flux to sediment traps at the base of the continental shelf slope, and century-scale accumulation rates in shelf and slope sediments (derived from excess 210Pb profiles in sediment cores). About 91% of river input Li was in particulate form, and there was conservative behavior of dissolved Li in the salinity gradient of the estuaries. Li accumulation rate in inner-shelf sediments was slightly less than river inputs, suggesting that more than 90% of Li river inputs were trapped in rapid aluminosilicate mud accumulation zones of the inner shelf (<50-m depth). Li removal rate to sediment traps at the base of the slope at ∼1000-m water depth was an order of magnitude smaller than the inner-shelf sedimentation. Export of Li to deep water Coral Sea was estimated to be 1.2 × 108 mol yr−1, and this amount is equivalent to the riverine dissolved Li annual supply rate. About 66% of river input of B was in the particulate phase, and low dissolved B concentrations in freshwater were conservatively mixed with higher concentrations of B in seawater across the salinity gradient. Removal of B to inner-shelf sediments was about 83% of the total river input, indicating a small export of B (1.2 × 108 mol yr−1) to the Coral Sea. About half of the dissolved B input from rivers is sorbed to particles and trapped in inner-shelf sediments. Only 24% of river input of Sr was in particulate form, and low freshwater concentrations of dissolved Sr were conservatively mixed with higher concentrations of Sr in seawater across the salinity gradient. Only 20% of total river inputs of Sr were buried in shelf sediments, and there was a large export (7.3 × 108 mol yr−1) of Sr off the shelf to the Coral Sea. A sediment core from a rapidly accumulating mud deposition zone of the inner shelf shows twofold sympathetic variations in Li, B, and Sr/Ca supply rates over 200- to 1000-yr time intervals.  相似文献   

7.
To understand the geochemical cycle of Hg in hypereutrophic freshwater lake, two sampling campaigns were conducted in Lake Taihu in China during May and September of 2009. The concentrations of unfiltered total Hg (unfTHg) were in the range of 6.8–83 ng L−1 (28 ± 18 ng L−1) in the lake water and total Hg in the sediment was 12–470 ng g−1, both of which are higher than in other background lakes. The concentration of unfTHg in ∼11% of the lake water samples exceeded the second class of the Chinese environmental standards for surface water of 50 ng L−1 (GB 3838-2002), indicating that a high ecological risk is posed by the Hg in Lake Taihu. However, the concentrations of unfiltered total MeHg (unfMeHg) were relatively low in the lake water (0.14 ± 0.05 ng L−1, excluding two samples with 0.81 and 1.0 ng L−1). Lake sediment MeHg varied from 0.2–0.96 ng g−1, with generally low ratios of MeHg/THg of <1%. The low concentrations of TMeHg in the lake water may have resulted from a strong uptake by the high primary productivity and the demethylation of MeHg in oxic conditions. In addition, contrary to the results of previous research conducted in deep-water lakes and reservoirs, the low concentrations of MeHg and low ratio of MeHg/THg in the lake sediment indicates that the net methylation of Hg was not accelerated by the elevated organic matter load created by the eutrophication of Lake Taihu. The results also showed that sediments were a source of THg and MeHg in the water. Higher diffusion fluxes of THg and MeHg may be partly responsible for the higher concentrations of THg in the lake water in May, 2009.  相似文献   

8.
The Yarlung Tsangpo-Brahmaputra river drains a large portion of the Himalaya and southern Tibetan plateau, including the eastern Himalayan syntaxis, one of the most tectonically active regions on the globe. We measured the solute chemistry of 161 streams and major tributaries of the Tsangpo-Brahmaputra to examine the effect of tectonic, climatic, and geologic factors on chemical weathering rates. Specifically, we quantify chemical weathering fluxes and CO2 consumption by silicate weathering in southern Tibet and the eastern syntaxis of the Himalaya, examine the major chemical weathering reactions in the tributaries of the Tsangpo-Brahmaputra, and determine the total weathering flux from carbonate and silicate weathering processes in this region. We show that high precipitation, rapid tectonic uplift, steep channel slopes, and high stream power generate high rates of chemical weathering in the eastern syntaxis. The total dissolved solids (TDS) flux from the this area is greater than 520 tons km−2 yr−1 and the silicate cation flux more than 34 tons km−2 yr−1. In total, chemical weathering in this area consumes 15.2 × 105 mol CO2 km−2 yr−1, which is twice the Brahmaputra average. These data show that 15-20% of the total CO2 consumption by silicate weathering in the Brahmaputra catchment is derived from only 4% of the total land area of the basin. Hot springs and evaporite weathering provide significant contributions to dissolved Na+ and Cl− fluxes throughout southern Tibet, comprising more than 50% of all Na+ in some stream systems. Carbonate weathering generates 80-90% of all dissolved Ca2+ and Mg2+ cations in much of the Yarlung Tsangpo catchment.  相似文献   

9.
The watershed in the southern Jiangxi Province (Jiangxi Province is called simply Gan) (SGW) and the watershed in the central Guizhou Province (Guizhou Province is called simply Qian) (CQW) are two subtropical watersheds of the Yangtze River in China. Both watersheds have similar latitudes and climate, but distinct differences in basin lithology. These similarities and differences provide a good natural laboratory in which to investigate weathering processes and Sr end-members in river waters. This work aims to identify and contrast the sources, fluxes and controls on Sr isotopic composition in the river waters of these two areas. Results showed that the 87Sr/86Sr in the SGW waters ranged from 0.716501 to 0.724931, with dissolved Sr averaging 27 μg l− 1. Rhyolites and granites are two major sources for the dissolved Sr. The SGW waters receive 42% of their Sr from silicates weathering, 32% from carbonates and 3.2% from evaporites. 87Sr/86Sr in the CQW waters has a lesser variation from 0.707694 to 0.710039, but higher Sr contents (average of 208 μg l− 1). Dolomite, limestone and dolomitic limestone are major sources of Sr in the waters. The CQW waters receive 69% of their Sr from carbonates, 1.7% from silicates and 0.9% from evaporites. The chemical erosion rate and Sr flux in the CQW are 122 t km− 2 a− 1 and 0.079 t km− 2 a− 1, respectively, which are higher than those of the SGW (56 t km− 2 a− 1 and 0.021 t km− 2 a− 1, respectively). These data suggest that the intensive carbonates weathering occurred in the karstic area in the upper-reach of the Yangtze River exert great influence on the high Sr concentration and low Sr isotopic ratios in the River.  相似文献   

10.
Two sediment cores retrieved at the northern slope of Sakhalin Island, Sea of Okhotsk, were analyzed for biogenic opal, organic carbon, carbonate, sulfur, major element concentrations, mineral contents, and dissolved substances including nutrients, sulfate, methane, major cations, humic substances, and total alkalinity. Down-core trends in mineral abundance suggest that plagioclase feldspars and other reactive silicate phases (olivine, pyroxene, volcanic ash) are transformed into smectite in the methanogenic sediment sections. The element ratios Na/Al, Mg/Al, and Ca/Al in the solid phase decrease with sediment depth indicating a loss of mobile cations with depth and producing a significant down-core increase in the chemical index of alteration. Pore waters separated from the sediment cores are highly enriched in dissolved magnesium, total alkalinity, humic substances, and boron. The high contents of dissolved organic carbon in the deeper methanogenic sediment sections (50-150 mg dm−3) may promote the dissolution of silicate phases through complexation of Al3+ and other structure-building cations. A non-steady state transport-reaction model was developed and applied to evaluate the down-core trends observed in the solid and dissolved phases. Dissolved Mg and total alkalinity were used to track the in-situ rates of marine silicate weathering since thermodynamic equilibrium calculations showed that these tracers are not affected by ion exchange processes with sediment surfaces. The modeling showed that silicate weathering is limited to the deeper methanogenic sediment section whereas reverse weathering was the dominant process in the overlying surface sediments. Depth-integrated rates of marine silicate weathering in methanogenic sediments derived from the model (81.4-99.2 mmol CO2 m−2 year−1) are lower than the marine weathering rates calculated from the solid phase data (198-245 mmol CO2 m−2 year−1) suggesting a decrease in marine weathering over time. The production of CO2 through reverse weathering in surface sediments (4.22-15.0 mmol CO2 m−2 year−1) is about one order of magnitude smaller than the weathering-induced CO2 consumption in the underlying sediments. The evaluation of pore water data from other continental margin sites shows that silicate weathering is a common process in methanogenic sediments. The global rate of CO2 consumption through marine silicate weathering estimated here as 5-20 Tmol CO2 year−1 is as high as the global rate of continental silicate weathering.  相似文献   

11.
From June 2004 to October 2005, particle size distributions (PSD) and the mineralogy of inorganic colloids in Lake Brienz, a glacial flour-rich Swiss lake, and in its tributaries (the Aare and Lütschine rivers), were quantified by single particle counting based on light scattering (0.1-2 μm) combined with transmission electronic microscopy coupled with energy dispersive spectroscopy and selected area electron diffraction. The two lake tributaries differ in terms of the geology of their catchment area and in their hydrology: the River Lütschine’s glacial regime is unperturbed, while the River Aare has been significantly modified by hydroelectric installations. The dependence of the colloid concentration numbers on colloid diameters can be described by a power-law distribution in all cases. The power-law slopes in the River Aare were consistently smaller, and the total colloid number concentrations consistently higher, (mean values: −3.89 and 6.2 × 108 mL−1, respectively) than in the River Lütschine (−3.61 and 1.7 × 108 mL−1). The measured PSD in the lake were dependent on season and depth: homogenous in the whole epilimnion in winter and modified by river intrusions in summer. In this season, the presence of a river turbid plume above the thermocline is a significant source of colloids in the epilimnion, where their concentration was high (mean value: 5.1 × 107 mL−1). The same main mineral types were found in the different systems: 2:1 minerals, feldspars, chlorite and quartz; with a few particles of oxides. Differences in their relative concentrations in the rivers, essentially reflecting the geological differences of the respective catchment areas, made it possible to trace the origin of the mineral colloids present in lake surface waters throughout the year. The relationship between colloid size and mineralogy was assessed, showing that different minerals have distinct size distributions. In the rivers, where almost no aggregates were observed, PSD would essentially be the result of the nature (particle formation and mineralogy) of the colloids, whereas in the lake, aggregation and sedimentation processes would also play a role, particularly in summer.  相似文献   

12.
Lakes worldwide are commonly oversaturated with CO2, however the source of this CO2 oversaturation is not well understood. To examine the magnitude of the C flux to the atmosphere and determine if an excess of respiration (R) over gross primary production (GPP) is sufficient to account for this C flux, metabolic parameters and stable isotopes of dissolved O2 and C were measured in 23 Québec lakes. All of the lakes sampled were oversaturated with CO2 over the sampling period, on average 221 ± 25%. However, little evidence was found to conclude that this CO2 oversaturation was the result of an excess of pelagic R over GPP. In lakes Croche and à l’Ours, where CO2 flux, R and GPP were measured weekly, the annual difference between pelagic GPP and R, or net primary production (NPP), was not sufficient to account for the size of the CO2 flux to the atmosphere. In Lac Croche average annual NPP was 14.4 mg C m−2 d−1 while the average annual flux of CO2 to the atmosphere was 34 mg C m−2 d−1. In Lac à l’Ours average annual NPP was −9.1 mg C m−2 d−1 while the average annual flux of CO2 to the atmosphere was 55 mg C m−2 d−1. In all of the lakes sampled, O2 saturation averaged 104.0 ± 1.7% during the ice-free season and the isotopic composition of dissolved O2 (δ18ODO) was 22.9 ± 0.3‰, lower than atmospheric values and indicative of net autotrophy. Carbon evasion was not a function of R, nor did the isotopic signature of dissolved CO2 in the lakes present evidence of excess R over GPP. External inputs of C must therefore subsidize the lake to explain the continued CO2 oversaturation. The isotopic composition of dissolved inorganic C (δ13CDIC) indicates that the CO2 oversaturation cannot be attributed to in situ aerobic respiration. δ13CDIC reveals a source of excess C enriched in 13C, which may be accounted for by anaerobic sediment respiration or groundwater inputs followed by kinetic isotope fractionation during degassing under open system conditions.  相似文献   

13.
We present here new measurements of sulfur dioxide and hydrogen sulfide emissions from Vulcano, Etna, and Stromboli (Italy), made by direct sampling at vents and by filter pack and ultraviolet spectroscopy in downwind plumes. Measurements at the F0 and FA fumaroles on Vulcano yielded SO2/H2S molar ratios of ≈0.38 and ≈1.4, respectively, from which we estimate an H2S flux of 6 to 9 t · d−1 for the summit crater. For Mt. Etna and Stromboli, we found SO2/H2S molar ratios of ≈20 and ≈15, respectively, which combined with SO2 flux measurements, suggest H2S emission rates of 50 to 113 t · d−1 and 4 to 8 t · d−1, respectively. We observe that “source” and plume SO2/H2S ratios at Vulcano are similar, suggesting that hydrogen sulfide is essentially inert on timescales of seconds to minutes. This finding has important implications for estimates of volcanic total sulfur budget at volcanoes since most existing measurements do not account for H2S emission.  相似文献   

14.
In this study, we examined the temporal changes of terrestrially-derived particulate organic carbon (POC) in the lower Mississippi River (MR) and in a very limited account, the upper tributaries (Upper MR, Ohio River, and Missouri River). We used for the first time a combination of lignin-phenols, bulk stable carbon isotopes, and compound-specific isotope analyses (CSIA) to examine POC in the lower MR and upper tributaries.A lack of correlation between POC and lignin phenol abundances (Λ8) was likely due to dilution effects from autochthonous production in the river, which has been shown to be considerably higher than previously expected. The range of δ13C values for p-hydroxycinnamic and ferulic acids in POC in the lower river do support that POM in the lower river does have a significant component of C4 in addition to C3 source materials. A strong correlation between δ13C values of p-hydroxycinnamic, ferulic, and vanillyl phenols suggests a consistent input of C3 and C4 carbon to POC lignin while a lack of correlation between these same phenols and POC bulk δ13C further indicates the considerable role of autochthonous carbon in the lower MR POC budget. Our estimates indicate an annual flux of POC of 9.3 × 108 kg y−1 to the Gulf of Mexico. Total lignin fluxes, based on Λ8 values of POC, were estimated to be 1.2 × 105 kg y−1. If we include the total dissolved organic carbon (DOC) flux (3.1 × 109 kg y−1) reported by [Bianchi T. S., Filley T., Dria K. and Hatcher, P. (2004) Temporal variability in sources of dissolved organic carbon in the lower Mississippi River. Geochim. Cosmochim. Acta68, 959-967.], we get a total organic carbon flux of 4.0 × 109 kg y−1. This represents 0.82% of the annual total organic carbon supplied to the oceans by rivers (4.9 × 1011 kg).  相似文献   

15.
Halogen diffusion in a basaltic melt   总被引：2，自引：0，他引：2  
The diffusion of the halogens fluorine, chlorine and bromine was measured in a hawaiitic melt from Mt. Etna at 500 MPa and 1.0 GPa, 1250 to 1450 °C at anhydrous conditions; the diffusion of F and Cl in the melt was also studied with about 3 wt% of dissolved water. Experiments were performed using the diffusion-couple technique in a piston cylinder. Most experiments were performed with only one halogen diffusing between the halogen-enriched and halogen-poor halves of the diffusion couple, but a few experiments with a mixture of halogens (F, Cl and Br) were also performed in order to investigate the possibility of interactions between the halogens during diffusion. Fluorine and chlorine diffusivity show a very similar behavior, slightly diverging at low temperature. Bromine diffusion is a factor of about 2-5 lower than the other halogens in this study. Diffusion coefficients for fluorine range between 2.3 × 10−11 and 1.4 × 10−10 m2 s−1, for chlorine between 1.1 × 10−11 and 1.3 × 10−10 and for bromine between 9.4 × 10−12 and 6.8 × 10−11 m2 s−1. No pressure effect was detected at the conditions investigated. In experiments involving mixed halogens, the diffusivities appear to decrease slightly (by a factor of ∼3), and are more uniform among the three elements. However, activation energies for diffusion do not appear to differ between experiments with individual halogens or when they are all mixed together. The effect of water increases the diffusion coefficients of F and Cl by no more than a factor of 3 compared to the anhydrous melt (DF = 4.0 × 10−11 to 1.6 × 10−10 m2 s−1; DCl = 3.0 × 10−11 to 1.9 × 10−10 m2 s−1). Comparing our results to the diffusion coefficients of other volatiles in nominally dry basaltic melts, halogen diffusivities are about one order of magnitude lower than H2O, similar to CO2, and a factor of ∼5 higher than S. The contrasting volatile diffusivities may affect the variable extent of volatile degassing upon melt depressurization and vesiculation, and can help our understanding of the compositions of rapidly grown magmatic bubbles.  相似文献   

16.
Vegetation assemblages and associated disturbance regimes are spatially heterogeneous in mountain ecosystems throughout the world due to the complex terrain and strong environmental gradients. Given this complexity, numerous sites describing postglacial vegetation and fire histories are needed to adequately understand forest development and ecosystem responses to varying climate and disturbance regimes. To gain insight into long-term historical climate–fire–vegetation interactions in southeastern British Columbia, Canada, sedimentological and paleoecological analyses were performed on a sediment core recovered from a small subalpine lake. The pollen assemblages, stomata, and macroremains indicate that from 9500 to 7500 cal yr BP, Pinus-dominated forests occurred within the catchment and Alnus was also present. Climate was an important control of fire and fire frequency was highest at this time, peaking at 8 fires 1000 yr− 1, yet charcoal accumulation rates were low, indicative of low terrestrial biomass abundance. From 7500 to 4600 cal yr BP, Pinus decreased as Picea, Abies and Larix increased and fire frequencies decreased to 3–6 fires 1000 yr− 1. Since 7500 cal yr BP the fire regime varied at a millennial scale, driven by forest biomass abundance and fuel accumulation changes. Local scale (bottom-up) controls of fire increased in relative importance since at least 6000 cal yr BP.  相似文献   

17.
Recent studies of chemical weathering of andesitic-dacitic material on high-standing islands (HSIs) have shown these terrains have some of the highest observed rates of chemical weathering and associated CO2 consumption yet reported. However, the paucity of stream gauge data in many of these terrains has limited determination of chemical weathering product fluxes. In July 2006 and March 2008, stream water samples were collected and manual stream gauging was performed in watersheds throughout the volcanic island of Dominica in the Lesser Antilles. Distinct wet and dry season solute concentrations reveal the importance of seasonal variations on the weathering signal. A cluster analysis of the stream geochemical data shows the importance of parent material age on the overall delivery of solutes. Observed Ca:Na, HCO3:Na and Mg:Na ratios suggest crystallinity of the parent material may also play an important role in determining weathering fluxes. From total dissolved solids concentrations and mean annual discharge calculations we calculate chemical weathering yields of (6-106 t km−2 a−1), which are similar to those previously determined for basalt terrains. Silicate fluxes (3.1-55.4 t km−2 a−1) and associated CO2 consumption (190-1575 × 103 mol km−2 a−1) determined from our study are among the highest determined to date. The calculated chemical fluxes from our study confirm the weathering potential of andesitic-dacitic terrains and that additional studies of these terrains are warranted.  相似文献   

18.
The continental shelf benthic iron flux and its isotope composition   总被引：1，自引：0，他引：1  
Benthic iron fluxes from sites along the Oregon-California continental shelf determined using in situ benthic chambers, range from less than 10 μmol m−2 d−1 to values in excess of ∼300 μmol m−2 d−1. These fluxes are generally greater than previously published iron fluxes for continental shelves contiguous with the open ocean (as opposed to marginal seas, bays, or estuaries) with the highest fluxes measured in the regions around the high-sediment discharge Eel River and the Umpqua River. These benthic iron fluxes do not covary with organic carbon oxidation rates in any systematic fashion, but rather seem to respond to variations in bottom water oxygen and benthic oxygen demand. We hypothesize that the highest rates of benthic iron efflux are driven, in part, by the greater availability of reactive iron deposited along these river systems as compared to other more typical continental margin settings. Bioirrigation likely plays an important role in the benthic Fe flux in these systems as well. However, the influence of bottom water oxygen concentrations on the iron flux is significant, and there appears to be a threshold in dissolved oxygen (∼60-80 μM), below which sediment-ocean iron exchange is enhanced. The isotope composition of this shelf-derived benthic iron is enriched in the lighter isotopes, and appears to change by ∼3‰ (δ56Fe) during the course of a benthic chamber experiment with a mean isotope composition of −2.7 ± 1.1‰ (2 SD, n = 9) by the end of the experiment. This average value is slightly heavier than those from two high benthic Fe flux restricted basins from the California Borderland region where δ56Fe is −3.4 ± 0.4‰ (2 SD, n = 3). These light iron isotope compositions support previous ideas, based on sediment porewater analyses, suggesting that sedimentary iron reduction fractionates iron isotopes and produces an isotopically light iron pool that is transferred to the ocean water column. In sum, our data suggest that continental shelves may export a higher efflux of iron than previously hypothesized, with the likelihood that along river-dominated margins, the benthic iron flux could well be orders of magnitude larger than non-river dominated shelves. The close proximity of the continental shelf benthos to the productive surface ocean means that this flux is likely to be essential for maintaining ecosystem micronutrient supply.  相似文献   

19.
This study combines sediment geochemical analysis, in situ benthic lander deployments and numerical modeling to quantify the biogeochemical cycles of carbon and sulfur and the associated rates of Gibbs energy production at a novel methane seep. The benthic ecosystem is dominated by a dense population of tube-building ampharetid polychaetes and conspicuous microbial mats were unusually absent. A 1D numerical reaction-transport model, which allows for the explicit growth of sulfide and methane oxidizing microorganisms, was tuned to the geochemical data using a fluid advection velocity of 14 cm yr−1. The fluids provide a deep source of dissolved hydrogen sulfide and methane to the sediment with fluxes equal to 4.1 and 18.2 mmol m−2 d−1, respectively. Chemosynthetic biomass production in the subsurface sediment is estimated to be 2.8 mmol m−2 d−1 of C biomass. However, carbon and oxygen budgets indicate that chemosynthetic organisms living directly above or on the surface sediment have the potential to produce 12.3 mmol m−2 d−1 of C biomass. This autochthonous carbon source meets the ampharetid respiratory carbon demand of 23.2 mmol m−2 d−1 to within a factor of 2. By contrast, the contribution of photosynthetically-fixed carbon sources to ampharetid nutrition is minor (3.3 mmol m−2 d−1 of C). The data strongly suggest that mixing of labile autochthonous microbial detritus below the oxic layer sustains high measured rates of sulfate reduction in the uppermost 2 cm of the sulfidic sediment (100-200 nmol cm−3 d−1). Similar rates have been reported in the literature for other seeps, from which we conclude that autochthonous organic matter is an important substrate for sulfate reducing bacteria in these sediment layers. A system-scale energy budget based on the chemosynthetic reaction pathways reveals that up to 8.3 kJ m−2 d−1 or 96 mW m−2 of catabolic (Gibbs) energy is dissipated at the seep through oxidation reactions. The microorganisms mediating sulfide oxidation and anaerobic oxidation of methane (AOM) produce 95% and 2% of this energy flux, respectively. The low power output by AOM is due to strong bioenergetic constraints imposed on the reaction rate by the composition of the chemical environment. These constraints provide a high potential for dissolved methane efflux from the sediment (12.0 mmol m−2 d−1) and indicates a much lower efficiency of (dissolved) methane sequestration by AOM at seeps than considered previously. Nonetheless, AOM is able to consume a third of the ascending methane flux (5.9 mmol m−2 d−1 of CH4) with a high efficiency of energy expenditure (35 mmol CH4 kJ−1). It is further proposed that bioenergetic limitation of AOM provides an explanation for the non-zero sulfate concentrations below the AOM zone observed here and in other active and passive margin sediments.  相似文献   

20.
In a comprehensive study, we compared depositional conditions, organic matter (OM) composition, and organic carbon turnover in sediments from two different depositional systems along the Chilean continental margin: at ∼23° S off Antofagasta and at ∼36° S off Concepción. Both sites lie within the Chilean coastal upwelling system and have an extended oxygen minimum zone in the water column. However, the northern site (23° S) borders the Atacama Desert, while the southern site (36° S) has a humid hinterland. Eight surface sediment cores (up to 30 cm long) from water depths of 126-1350 m were investigated for excess 210Pb (210Pbxs) activity, total organic and total inorganic carbon concentrations (TOC and TIC, respectively), C/N-ratios, organic carbon isotopic compositions (δ13C), chlorin concentrations, Chlorin Indices (CI), and sulfate reduction rates (SRR). Sediment accumulation rates obtained from 210Pb-analysis were similar in both regions (0.04-0.15 cm yr−1 at 23° S, 0.10-0.19 cm yr−1 at 36° S), although total 210Pbxs fluxes indicated that the vertical particle flux was higher at 36° S than at 23° S. We propose that sediment focusing in isolated deposition centers led to high sediment accumulation rates at 23° S. Furthermore, there were no indications for sediment mixing at 23° S, while bioturbation was intense at 36° S. δ13C-values (−24.5‰ to −20.1‰ vs. VPDB) and C/N-ratios (molar, 8.6-12.8) were characteristic of a predominantly marine origin of the sedimentary OM in both investigated areas. The extent of OM alteration in the water column was partly reflected in the surface sediments as chlorin concentrations decreased and C/N-ratios and CI increased with increasing water depth of the sampling site. SRR were lower at 23° S (areal SRR 0.12-0.60 mmol m−2 d−1) than at 36° S (areal SRR 0.82-1.18 mmol m−2 d−1), which was partly due to the greater water depth of most of the sediments investigated in the northern region and consistent with a lower quality of the sedimentary OM at 23° S. Reaction rate constants for TOC degradation that were obtained from measured SRR (kSRR; 0.0004-0.0022 yr−1) showed a good correspondence to kTOC that were derived from the depth profiles of TOC (0.0003-0.0014 yr−1). Both, kSRR and kTOC, reflect differences in OM composition. At 36° S they were related to the degradation state of bulk OM (represented by C/N-ratios), whereas near 23° S they were related to the freshness of a small fraction of labile OM (represented by CI). Our study shows that although rates of organic carbon accumulation were similar in both investigated sites, the extent and kinetics of organic carbon degradation were closely linked to differing depositional conditions.  相似文献   

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