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1.
A detailed geochemical and microbiological study of a ∼2 m sediment core from the inactive Alvin mounds within the TAG hydrothermal field was conducted to examine, for the first time, the role of prokaryotes in subsurface weathering of hydrothermal sediments. Results show that there has been substantial post-depositional remobilisation of metal species and diagenetic overprinting of the original high-temperature hydrothermal minerals, and aspects have involved prokaryotic processes. Prokaryotic enumeration demonstrates the presence of a population smaller than the average for deep sea sediments, probably due to the low organic carbon content, but not inhibited by (and hence adapted to) the metal rich environment. There was a small but significant increase in population size associated with the active redox boundary in an upper metal sulphide layer (50-70 cm) around which active metal remobilisation was concentrated (Cu, Au, Cd, Ag, U, Zn and Zn). Hence, subsurface prokaryotes were potentially obtaining energy from metal metabolism in this near surface zone. Close association of numbers of culturable Mn and Fe reducing prokaryotes with subsurface Fe2+ and Mn2+ pore water profiles suggested active prokaryotic metal reduction at depth in core CD102/43 (to ∼175 cm). In addition, a prokaryotic mechanism, which is associated with bacterial sulphate reduction, is invoked to explain the U enrichment on pyrite surfaces and Zn and Pb remobilisation in the upper sediment. Although prokaryotic populations are present throughout this metalliferous sediment, thermodynamic calculations indicated that the inferred low pH of pore waters and the suboxic/anoxic conditions limits the potential energy available from Fe(II) oxidation, which may restrict prokaryotic chemolithotrophic biomass. This suggests that intense prokaryotic Fe oxidation and weathering of seafloor massive sulphide deposits may be restricted to the upper portion of the deposit that is influenced by near neutral pH and oxic seawater unless there is significant subsurface fluid flow.  相似文献   

2.
Raman analysis of the vapor phase formed after heating pure water to near critical (355-374 °C) temperatures in a hydrothermal diamond-anvil cell (HDAC) reveals the synthesis of abiogenic methane. This unexpected result demonstrates the chemical reactivity of diamond at relatively low temperatures. The rate of methane production from the reaction between water and diamond increases with increasing temperature and is enhanced by the presence of a metal gasket (Re, Ir, or Inconel) which is compressed between the diamond anvils to seal the aqueous sample. The minimum detection limit for methane using Raman spectroscopy was determined to be ca. 0.047 MPa, indicating that more than 1.4 nanograms (or 8.6 × 10−11 mol) of methane were produced in the HDAC at 355 °C and 30 MPa over a period of ten minutes. At temperatures of 650 °C and greater, hydrogen and carbon dioxide were detected in addition to methane. The production of abiogenic methane, observed in all HDAC experiments where a gasket was used, necessitates a reexamination of the assumed chemical systems and intensive parameters reported in previous hydrothermal investigations employing diamonds. The results also demonstrate the need to minimize or eliminate the production of methane and other carbonic species in experiments by containing the sample within a HDAC without using a metal gasket.  相似文献   

3.
Comparative study of genesis and structure of dispersed organic matter (DOM) from background pelagic bottom sediments and sediments inside an active hydrothermal field Ashadze-1 collected during the cruise of the R/V “Professor Logachev” in 2003 was carried out. The received results allow to speak about an essential originality of structure and distribution of DOM in bottom sediments of the field Ashadze-1, according to unique physical and chemical conditions and facial specificity of sedimentation in hydrothermal zones. At the same time, attributes of petroleum hydrocarbons abiogenic synthesis hasn’t been fixed. Opposite, the received data allow to consider the process of fast maturing of biogenic OM in hydrothermal systems as a major factor of HC formation.  相似文献   

4.
The first building blocks of life could be produced in ultramafic-hosted hydrothermal systems considering the large amounts of hydrogen and methane generated by serpentinisation and Fischer–Tropsch-Type synthesis, respectively, in those systems. The purpose of this study was to detect and characterise organic molecules in hydrothermal fluids from ultramafic-hosted hydrothermal systems in the Mid-Atlantic Ridge (MAR) region. During the EXOMAR cruise 2005, fluids from the Rainbow (36°14′N) and the Lost City (30°N) hydrothermal fields were collected and treated by Stir Bar Sorptive Extraction (SBSE) and Solid Phase Extraction (SPE). The extracts were analysed by Thermal Desorption–Gas Chromatography–Mass Spectrometry (TD–GC–MS) and GC–MS, respectively. Compared to nearby deep seawater, hydrothermal fluids were clearly enriched in organic compounds, with a more diverse spectrum of molecules. We observed a very similar range of organic compounds in fluids from both sites, with a dominance of aliphatic hydrocarbons (C9–C14), aromatic compounds (C6–C16) and carboxylic acids (C8–C18). The occurrence of these compounds is supported by other field studies on serpentinites and sulfide deposits. Literature on thermodynamic data and experimental work has suggested the possible abiogenic origin of hydrocarbons and organic acids. In addition, it has been shown elsewhere that catalytic reactions producing hydrocarbons likely occur at both Lost City and Rainbow hydrothermal fields as suggested by the evolution of δ13C with increasing C number for methane, ethane, propane and butane. In order to investigate the origin of the organic molecules in the fluids, compound-specific carbon isotope ratio measurements were performed on n-alkanes and carboxylic acids, for which the δ13C values were in the range of ? 46 to ? 20‰ (vs. V-PDB). These preliminary data did not allow conclusive support or rejection of an abiogenic origin of the compounds. Indeed, predicting δ13C signatures in hydrothermal systems is likely to be complicated, due to differences in source δ13C signatures (i.e., of the C building blocks), and a variety of, mostly unknown, fractionation steps which may occur along the synthesis pathways. In addition, even though a fraction of the compounds detected in the fluids is likely abiotically produced, a dominance of biogenic sources and/or processes might hide their characteristic signature.  相似文献   

5.
Natural evidence for rapid abiogenic hydrothermal generation of CH4   总被引：1，自引：0，他引：1  
Although recent hydrothermal experiments imply that abiogenic methane (CH4) generation from hydrothermal reduction of CO2 can occur, evidence from natural systems was still lacking. Based on the chemical and isotopic equilibrium signatures of low-temperature fumarolic gas discharges, we are able to provide hard evidence for its natural occurrence, namely in three subduction-related bi-phase hydrothermal systems of the Mediterranean, whose temperatures range from 260 to 470 °C. The attainment of equilibrium and the time spans of recent volcanic dormancy allowed us to calculate minimum rates for chemical and isotopic equilibration. These are significantly higher than those previously reported and might be due to the presence of a saturated water vapor phase in the investigated systems. The fact that nature provides conditions enabling relatively fast production of hydrocarbons from CO2 strongly supports the concerns that were recently raised from laboratory experiments. These address the use of the carbon isotope composition of reduced carbon in Archean sediments as a tracer of early life and the occurrence of CH4 on extraterrestrial planets as a bioindicator. In view of the potential role of abiogenic CH4 as a precursor of life, we also present an estimate of abiogenic hydrothermal CH4 fluxes throughout the Archean. It is not expected that these fluxes exceeded 80 Mt/yr during the past 4.0 Ga. This, however, would have been enough to facilitate HCN production on the prebiotic Earth.  相似文献   

6.
We present first data on the geochemistry, mineralogy and morphology of near-vent sediments (35 and 200 m from active vent) and ridge flank sediments (approximately 3 km from the vent field) as well as oxyhydroxide deposits from the Endeavour segment, Juan de Fuca Ridge. The purpose of the study was to understand better the origin and characteristic features of metalliferous sediments associated with base and precious metal massive sulfides in volcanic terrains. Hydrothermal components in sediments are Fe-Si ± S-rich and Mn-Fe-Si-rich phases, sulfides and barite, which were exclusively derived from plume fallout. Sulfides are only a minor constituent of near-vent sediments (2-4 wt%) and were not detected in ridge flank sediments. The study suggests that the distribution of hydrothermal phases and associated elements in near-vent and ridge flank sediments is affected mainly by processes of agglomeration, dissolution, absorption and settling that take place within a plume and to a lesser extent post-depositional processes. Rapid deposition of sulfides in the vicinity of the vents is reflected in a sharp drop of the Cu concentrations in sediments with increasing distance from the vents. Besides sulfides, important carriers of Pb, Cu, Zn and Co in near-vent sediments are Fe-Mn oxyhydroxides that occur together with silica as aggregates of gel-like material and flaky particles and as coatings on filaments. Away from the vents, trace metals are mostly in Fe-Mn oxyhydroxides and authigenic Fe-rich montmorillonite. Oxyhydroxides at the Main Endeavour field are interpreted to have originated from oxidation of mound sulfides accompanied by precipitation of primary Fe-oxyhydroxide + silica from low-temperature fluids. At the Mothra field, seafloor deposits and chimney crusts composed of Fe-oxyhydroxide ± Mn + silica are considered to be direct precipitates from hydrothermal fluids that have been less diluted with seawater. Oxyhydroxide deposits exhibit unique microtextures that resemble mineralized microorganisms and may indicate existence of diverse microbial communities.  相似文献   

7.
Overbank sediments contaminated with metalliferous minerals are a source of toxic metals that pose risks to living organisms. The overbank sediments from the Geul river in Belgium contain 4000-69,000 mg/kg Zn as a result of mining and smelting activities, principally during the 19th century. Three main Zn species were identified by powder Zn K-edge EXAFS spectroscopy: smithsonite (ZnCO3), tetrahedrally coordinated sorbed Zn (sorbed IVZn) and Zn-containing trioctahedral phyllosilicate. Smithsonite is a primary mineral, which accounts for approximately 20-60% of the Zn in sediments affected by mining and smelting of oxidized Zn ores (mostly carbonates and silicates). This species is almost absent in sediments affected by mining and smelting of both sulphidic (ZnS, PbS) and oxidized ores, presumably because of acidic dissolution associated with the oxidation of sulphides, as suggested by the lower pH of this second type of sediment (pH(CaCl2) <7.0 vs. pH(CaCl2) >7.0 for the first type). Thus, sulphide minerals in sediment deposits can act as a secondary source of dissolved metals by a chemical process analogous to acid mine drainage. The sorbed IVZn component ranges up to approximately 30%, with the highest proportion occurring at pH(CaCl2) <7.0 as a result of the readsorption of dissolved Zn2+ on sediments constituents. Kerolite-like Zn-rich phyllosilicate is the major secondary species in all samples, and in some the only detected species, thus providing the first evidence for pervasive sequestration of Zn into this newly formed precipitate at the field scale.  相似文献   

8.
Short-wave infrared (SWIR) spectral reflectance of hydrothermally altered volcanic rocks in the footwall of the Hellyer massive sulfide deposit was measured with a portable PIMA-II infrared spectrometer. The Al–OH band was used to derive information on the octahedral Al content and the abundance of white mica (sericite) in the hydrothermal alteration and mineralization system. The range of the Al–OH band wavelength from 2192 nm to 2222 nm corresponds to the number of octahedral Al (Alvi) in white mica approximately from 3.9 to 3.0 (based on 4 octahedral cations per formula). This Alvi range represents a significant compositional variation, covering most of the compositional region between muscovite (Alvi = 4.0) and phengite (Alvi = 3.0). Furthermore, the spectral reflectance data show that the compositional variation of white mica is spatially related to hydrothermal alteration zoning, such that phengitic white mica tends to occur in 1) main upflow fluid channel, 2) intensely altered volcanic rocks, and 3) Pb–Zn mineralization, whereas muscovitic white mica was formed preferentially distal to massive sulfide mineralization on the margin of the footwall alteration system. The results suggest that the Al–OH band wavelength, and therefore the octahedral Al content, of white mica can be used as vectors to mineralization to map the hydrothermal system at Hellyer.  相似文献   

9.
The analysis of gaseous compositions from Solfatara (Campi Flegrei, South Italy) fumaroles since the early 1980s, clearly reveals a double thermobarometric signature. A first signature at temperatures of about 360 °C was inferred by methane-based chemical-isotopic geoindicators and by the H2/Ar geothermometer. These high temperatures, close to the critical point of water, are representative of a deep zone where magmatic gases flash the hydrothermal liquid, forming a gas plume. A second signature was found to be at around 200-240 °C. At these temperatures, the kinetically fast reactive species (H2 and CO) re-equilibrate in a pure vapor phase during the rise of the plume. A combination of these observations with an original interpretation of the oxygen isotopic composition of the two dominant species, i.e. H2O and CO2, shed light on the origin of fumarolic fluids by showing that effluents are mixture between fluids degassed from a magma body and the vapor generated at about 360 °C by the vaporization of hydrothermal liquids. A typical ‘andesitic’ water type (δD ∼ −20‰, δ18O ∼10‰) and a CO2-rich composition (XCO2∼0.4) has been inferred for the magmatic fluids, while for the hydrothermal component a meteoric origin and a CO2 fugacity fixed by fluid-rock reaction at high temperatures have been estimated. In the time the fraction of magmatic fluids in the fumaroles increased (up to ∼0.5) at each seismic and ground uplift crisis (bradyseism) which occurred at Campi Flegrei, suggesting that bradyseismic crises are triggered by periodic injections of CO2-rich magmatic fluids at the bottom of the hydrothermal system.  相似文献   

10.
The chemical and isotopic composition of pore fluids is presented for five deep-rooted mud volcanoes aligned on a transect across the Gulf of Cadiz continental margin at water depths between 350 and 3860 m. Generally decreasing interstitial Li concentrations and 87Sr/86Sr ratios with increasing distance from shore are attributed to systematically changing fluid sources across the continental margin. Although highest Li concentrations at the near-shore mud volcanoes coincide with high salinities derived from dissolution of halite and late-stage evaporites, clayey, terrigenous sediments are identified as the ultimate Li source to all pore fluids investigated. Light δ7Li values, partly close to those of hydrothermal vent fluids (δ7Li: +11.9‰), indicate that Li has been mobilized during high-temperature fluid/sediment or fluid/rock interactions in the deep sub-surface. Intense leaching of terrigenous clay has led to radiogenic 87Sr/86Sr ratios (∼0.7106) in pore fluids of the near-shore mud volcanoes. In contrast, non-radiogenic 87Sr/86Sr ratios (∼0.7075) at the distal locations are attributed to admixing of a basement-derived fluid component, carrying an isotopic signature from interaction with the basaltic crust. This inference is substantiated by temperature constraints from Li isotope equilibrium calculations suggesting exchange processes at particularly high temperatures (>200 °C) for the least radiogenic pore fluids of the most distal location.Advective pore fluids in the off-shore reaches of the Gulf of Cadiz are influenced by successive exchange processes with both oceanic crust and terrigenous, fine-grained sediments, resulting in a chemical and isotopic signature similar to that of fluids in near-shore ridge flank hydrothermal systems. This suggests that deep-rooted mud volcanoes in the Gulf of Cadiz represent a fluid pathway intermediate between mid-ocean ridge hydrothermal vent and shallow, marginal cold seep. Due to the thicker sediment coverage and slower fluid advection rates, the overall geochemical signature is shifted towards the sediment-diagenetic signal compared to ridge flank hydrothermal environments.  相似文献   

11.
This work is devoted to characterization of zinc interaction in aqueous solution with two marine planktonic (Thalassiosira weissflogii = TW, Skeletonema costatum = SC) and two freshwater periphytic species (Achnanthidium minutissimum = AMIN, Navicula minima = NMIN) by combining adsorption and electrophoretic measurements with surface complexation modeling and by assessing Zn isotopes fractionation during both long term uptake and short term adsorption on diatom cells and their frustules. Reversible adsorption experiments were performed at 25 and 5 °C as a function of exposure time (5 min to 140 h), pH (2 to 10), zinc concentration in solution (10 nM to 1 mM), ionic strength (I = 0.001 to 1.0 M) and the presence of light. While the shape of pH-dependent adsorption edge is almost the same for all four species, the constant-pH adsorption isotherm and maximal Zn binding capacities differ by an order of magnitude. The extent of adsorption increases with temperature from 5 to 25 °C and does not depend on light intensity. Zinc adsorption decreases with increase of ionic strength suggesting competition with sodium for surface sites. Cell number-normalized concentrations of sorbed zinc on whole cells and their silica frustules demonstrated only weak contribution of the latter (10-20%) to overall zinc binding by diatom cell wall. Measurements of electrophoretic mobilities (μ) revealed negative diatoms surface potential in the full range of zinc concentrations investigated (0.15-760 μmol/L), however, the absolute value of μ decreases at [Zn] > 15 μmol/L suggesting a change in surface speciation. These observations allowed us to construct a surface complexation model for Zn binding by diatom surfaces that postulates the constant capacitance of the electric double layer and considers Zn complexation with carboxylate and silanol groups. Thermodynamic and structural parameters of this model are based on previous acid-base titration and spectroscopic results and allow quantitative reproduction of all adsorption experiments. Although Zn adsorption constants on carboxylate groups are almost the same, Zn surface adsorption capacities are very different among diatom species which is related to the systematic differences in their cell wall composition and thickness. Measurements of Zn isotopic composition (66Zn/(64Zn)) performed using a multicollector ICP MS demonstrated that irreversible incorporation of Zn in cultured diatom cells produces enrichment in heavy isotope compared to growth media (Δ66Zn(solid-solution) = 0.27 ± 0.05, 0.08 ± 0.05, 0.21 ± 0.05, and 0.19 ± 0.05‰ for TW, SC, NMIN, and AMIN species, respectively). Accordingly, an enrichment of cells in heavy isotopes (Δ66Zn(solid-solution) = 0.43 ± 0.1 and 0.27 ± 0.1‰ for NMIN and AMIN, respectively) is observed following short-term Zn sorption on freshwater cells in nutrient media at pH ∼ 7.8. Finally, diatoms frustules are enriched in heavy isotopes compared to solution during Zn adsorption on silica shells at pH ∼ 5.5 (Δ66Zn(solid-solution) = 0.35 ± 0.10‰). Measured isotopes fractionation can be related to the structure and stability of Zn complexes formed and they provide a firm basis for using Zn isotopes for biogeochemical tracing.  相似文献   

12.
The concentrations of mercury (Hg) and other trace metals (Ni, Cu, Zn, Mo, Ba, Re, U) and the Hg isotopic composition were examined across a dramatic redox and productivity transition in a mid-Pleistocene Mediterranean Sea sapropel sequence. Characteristic trace metal enrichment in organic-rich layers was observed, with organic-rich sapropel layers ranging in Hg concentration from 314 to 488 ng/g (avg = 385), with an average enrichment in Hg by a factor of 5.9 compared to organic-poor background sediments, which range from 39 to 94 ng/g Hg (avg = 66). Comparison of seawater concentrations and sapropel accumulations of trace metals suggests that organic matter quantitatively delivers Hg to the seafloor. Near complete scavenging of Hg from the water column renders the sapropel Hg isotopic composition representative of mid-Pleistocene Mediterranean seawater. Sapropels have an average δ202Hg value of −0.91‰ ± 0.15‰ (n = 5, 1 SD) and Δ199Hg value of 0.11‰ ± 0.03‰ (n = 5, 1 SD). Background sediments have an average δ202Hg of −0.76‰ ± 0.16‰ (n = 5, 1 SD) and Δ199Hg of 0.05‰ ± 0.01‰ (n = 5, 1 SD), which is indistinguishable from the sapropel values. We suggest that the sapropel isotopic composition is most representative of the mid-Pleistocene Tyrrhenian Sea.  相似文献   

13.
Geochemical methods (major elements and Sr, Nd isotopes) have been used to (1) characterize Lake Le Bourget sediments in the French Alps, (2) identify the current sources of the clastic sediments and estimate the source variability over the last 600 years. Major element results indicate that Lake Le Bourget sediments consist of 45% clastic component and 55% endogenic calcite. In addition, several individual flood levels have been identified during the Little Ice Age (LIA) on the basis of their higher clastic content (> 70%).Potential sources of Lake Le Bourget clastic sediments have been investigated from Sr and Nd isotope compositions. The sediments from the Sierroz River and Leysse River which are mainly derived from the Mesozoic Calcareous Massifs are characterised by lower 87Sr/86Sr ratios and slightly lower ?Nd(0) ratios than the Arve River sediments which are derived from the Palaeozoic Mont-Blanc External Crystalline Massifs. The Rhône River appears to have been the main source of clastic sediments into the lake for the last 600 years, as evidenced by a similar Sr and Nd isotopic compositions analyzed in core B16 sediments (87Sr/86Sr = 0.719, ?Nd(0) = − 10) and in the sediments of the Rhône River (87Sr/86Sr = 0.719, ?Nd(0) = − 9.6).The isotopic signatures of flood events and background samples from core B16 in Lake Le Bourget are also similar. This indicates that prior to ∼ 1800, the inputs into the lake have remained relatively homogeneous with the proportion of clastic component mainly being a function of the palaeohydrology of the Rhone River. Early human modification (deforestation and agriculture) of the lake catchment before the 1800s appears to have had little influence on the source of clastic sediments.  相似文献   

14.
Joint application of the Mo isotope paleoredox proxy and Re-Os deposition-age geochronometer to euxinic black shales has potential for tracing the evolution of ocean redox chemistry over geological time. Here, we report new Re-Os and Mo isotope data for the Mesoproterozoic Velkerri Formation (Roper Group) and Paleoproterozoic Wollogorang Formation (Tawallah Group), McArthur Basin, northern Australia. New Re-Os ages of 1361 ± 21 Ma (2σ, n = 14, mean square of weighted deviates [MSWD] = 1.3, Model 1) and 1417 ± 29 Ma (2σ, n = 12, MSWD = 1.3, Model 1) constrain the depositional age of the Velkerri Formation and its contained biomarkers, as well as acritarchs and microfossils from the Roper Group. Black shales from the upper Velkerri Formation have high Mo abundances (105-119 ppm) and degree of pyritization [DOP] values (0.90-0.92) implying quantitative conversion of molybdate (MoO42−) to thiomolybdate (MoS42−) in overlying bottom waters. The average δ97/95Mo (0.72 ± 0.10‰, 2σ, n = 6) of these shales is consistent with previous data, but represents a significantly more precise determination for global seawater δ97/95Mo at 1.4 Ga. This value is lighter than present-day seawater by ∼0.85‰ and reflects expanded strongly euxinic deep ocean conditions ([H2S]aq > 11 μM) relative to oxic, suboxic, and weakly/intermittently euxinic ([H2S]aq < 11 μM) marine deposition in the 1.4 Ga oceans. Mass-balance modelling suggests Mo removal into strongly euxinic and oxic sediments may have comprised 30-70% and less than 15%, respectively, of the oceanic Mo sink at 1.4 Ga as opposed to 5% and 35% today, respectively.The Re-Os radioisotope system in organic-rich shales serves as a test for post-depositional alteration that could affect the usefulness of paleoredox tracers such as Mo stable isotopes. Re-Os isotope data for the Wollogorang Formation black shales are scattered and yield a highly imprecise date of 1359 ± 150 Ma (2σ, n = 21, MSWD = 85, Model 3). This age is younger than U-Pb zircon ages from interbedded tuffs that constrain the age of deposition at ca. 1730 Ma. In conjunction with previous petrological, geochemical, and paleomagnetic data, the Re-Os isotope data suggest hydrothermal fluid flow through the Wollogorang Formation, possibly associated with formation of the ca. 1640 Ma McArthur River Pb-Zn-Ag sedimentary exhalative deposit, resulted in post-depositional mobilization of Re and Os. Based on the degree of deviation of the Re-Os data from a 1730 Ma reference line, open-system behavior of Re and Os was greatest near the base of the black shale unit. Wollogorang Formation black shales are enriched in Mo (41-58 ppm), but are characterized by variable δ97/95Mo (0.3-0.8‰) and DOP (0.57-0.92). The lightest δ97/95Mo values occur near the base of the black shale unit. Based on the Re-Os systematics, hydrothermal fluids have probably overprinted the authigenic δ97/95Mo signature in those shales. However, the heaviest δ97/95Mo values in the Wollogorang Formation come from stratigraphically higher shales, and are similar to those observed for the Velkerri Formation, and thus may reflect seawater δ97/95Mo at 1.73 Ga.  相似文献   

15.
Knowledge of the subduction input flux of nitrogen (N) in altered oceanic crust (AOC) is critical in any attempt to mass-balance N across arc-trench systems on a global or individual-margin basis. We have employed sealed-tube, carrier-gas-based methods to examine the N concentrations and isotopic compositions of AOC. Analyses of 53 AOC samples recovered on DSDP/ODP legs from the North and South Pacific, the North Atlantic, and the Antarctic oceans (with larger numbers of samples from Site 801 outboard of the Mariana trench and Site 1149 outboard of the Izu trench), and 14 composites for the AOC sections at Site 801, give N concentrations of 1.3 to 18.2 ppm and δ15NAir of −11.6‰ to +8.3‰, indicating significant N enrichment probably during the early stages of hydrothermal alteration of the oceanic basalts. The N-δ15N modeling for samples from Sites 801 and 1149 (n = 39) shows that the secondary N may come from (1) the sedimentary N in the intercalated sediments and possibly overlying sediments via fluid-sediment/rock interaction, and (2) degassed mantle N2 in seawater via alteration-related abiotic reduction processes. For all Site 801 samples, weak correlation of N and K2O contents indicates that the siting of N in potassic alteration phases strongly depends on N availability and is possibly influenced by highly heterogeneous temperature and redox conditions during hydrothermal alteration.The upper 470-m AOC recovered by ODP Legs 129 and 185 delivers approximately 8 × 105 g/km N annually into the Mariana margin. If the remaining less-altered oceanic crust (assuming 6.5 km, mostly dikes and gabbros) has MORB-like N of 1.5 ppm, the entire oceanic crust transfers 5.1 × 106 g/km N annually into that trench. This N input flux is twice as large as the annual N input of 2.5 × 106 g/km in seafloor sediments subducting into the same margin, demonstrating that the N input in oceanic crust, and its isotopic consequences, must be considered in any assessment of convergent margin N flux.  相似文献   

16.
The origin of Zn isotope fractionation in sulfides   总被引：2，自引：0，他引：2  
Isotope fractionation of Zn between aqueous sulfide, chloride, and carbonate species (Zn2+, Zn(HS)2, , , ZnS(HS)−, ZnCl+, ZnCl2, , and ZnCO3) was investigated using ab initio methods. Only little fractionation is found between the sulfide species, whereas carbonates are up to 1‰ heavier than the parent solution. At pH > 3 and under atmospheric-like CO2 pressures, isotope fractionation of Zn sulfides precipitated from sulfidic solutions is affected by aqueous sulfide species and the δ66Zn of sulfides reflect these in the parent solutions. Under high PCO2 conditions, carbonate species become abundant. In high PCO2 conditions of hydrothermal solutions, Zn precipitated as sulfides is isotopically nearly unfractionated with respect to a low-pH parent fluid. In contrast, negative δ66Zn down to at least −0.6‰ can be expected in sulfides precipitated from solutions with pH > 9. Zinc isotopes in sulfides and rocks therefore represent a potential indicator of mid to high pH in ancient hydrothermal fluids.  相似文献   

17.
Contaminated fluvial sediments represent both temporary sinks for river-borne pollutants and potential sources in case of natural and/or anthropogenic resuspension. Reservoir lakes play a very important role in sediment dynamics of watersheds and may offer great opportunities to study historical records of river-borne particles and associated elements transported in the past. The fate and potential environmental impact of Hg depends on its abundance, its carrier phases and its chemical speciation. Historical Hg records and solid state Hg speciation were compared in sediments from two contrasting reservoirs of the Lot River (France) upstream and downstream from a major polymetallic pollution (e.g. Cd, Zn) source. Natural (geochemical background) and anthropogenic Hg concentrations and their relationships with predominant carrier phases were determined. The results reveal important historical Hg contamination (up to 35 mg kg−1) of the downstream sediment, reflecting the historical evolution of industrial activity at the point source, i.e. former coal mining, Zn ore treatment and post-industrial remediation work. Single chemical extractions (ascorbate, H2O2, KOH) suggest that at both sites most (∼75%) of the Hg is bound to organic and/or reactive sulphide phases. Organo-chelated (KOH-extracted) Hg, representing an important fraction in the uncontaminated sediment, shows similar concentrations (∼0.02 mg kg−1) at both sites and may be mainly attributed to natural inputs and/or processes. Although, total Hg concentrations in recent surface sediments at both sites are still very different, similar mono-methylmercury concentrations (up to 4 μg kg−1) and vertical distributions were observed, suggesting comparable methylation-demethylation processes. High mono-methylmercury concentrations (4–15 μg kg−1) in 10–40 a-old, sulphide-rich, contaminated sediment suggest long-term persistence of mono-methylmercury. Beyond historical records of total concentrations, the studied reservoir sediments provided new insights in solid state speciation and carrier phases of natural and anthropogenic Hg. In case of sediment resuspension, the major part of the Hg historically stored in the Lot River sediments will be accessible to biogeochemical recycling in the downstream fluvial-estuarine environment.  相似文献   

18.
Zinc isotopes have been studied along two smelter-impacted soil profiles sampled near one of the largest Pb and Zn processing plants in Europe located in northern France, about 50 km south of Lille. Mean δ66Zn values along these two soil profiles range from +0.22 ± 0.17‰ (2σ) to +0.34 ± 0.17‰ (2σ) at the lowest horizons and from +0.38 ± 0.45‰ (2σ) to +0.76 ± 0.14‰ (2σ) near the surface. The δ66Zn values in the lowest horizons of the soils are interpreted as being representative of the local geochemical background (mean value +0.31 ± 0.38‰), whereas heavier δ66Zn values near the surface of the two soils are related to anthropogenic Zn. This anthropogenic Zn occurs in the form of franklinite (ZnFe2O4)-bearing slag grains originating from processing wastes at the smelter site and exhibiting δ66Zn values of +0.81 ± 0.20‰ (2σ). The presence of franklinite is indicated by EXAFS analysis of the topsoil samples from both soil profiles as well as by micro-XANES analysis of the surface horizon of a third smelter-impacted soil from a distant site. These results indicate that naturally occurring Zn and smelter-derived Zn exhibit significantly different δ66Zn values, which suggests that zinc isotopes can be used to distinguish between geogenic and anthropogenic sources of Zn in smelter-impacted soils. In addition to a possible influence of additional past sources of light Zn (likely Zn-sulfides and Zn-sulfates directly emitted by the smelter), the light δ66Zn values in the surface horizons compared to smelter-derived slag materials are interpreted as resulting mainly from fractionation processes associated with biotic and/or abiotic pedological processes (Zn-bearing mineral precipitation, Zn complexation by organic matter, and plant uptake of Zn). This conclusion emphasizes the need for additional Zn isotopic studies before being able to use Zn isotopes to trace sources and pathways of this element in surface environments.  相似文献   

19.
Enstatite meteorites include the undifferentiated enstatite chondrites and the differentiated enstatite achondrites (aubrites). They are the most reduced group of all meteorites. The oxygen isotope compositions of both enstatite chondrites and aubrites plot along the terrestrial mass fractionation line, which suggests some genetic links between these meteorites and the Earth as well.For this study, we measured the Zn isotopic composition of 25 samples from the following groups: aubrites (main group and Shallowater), EL chondrites, EH chondrites and Happy Canyon (impact-melt breccia). We also analyzed the Zn isotopic composition and elemental abundance in separated phases (metal, silicates, and sulfides) of the EH4, EL3, and EL6 chondrites. The different groups of meteorites are isotopically distinct and give the following values (‰): aubrite main group (−7.08 < δ66Zn < −0.37); EH3 chondrites (0.15 < δ66Zn < 0.31); EH4 chondrites (0.15 < δ66Zn < 0.27); EH5 chondrites (δ66Zn = 0.27 ± 0.09; n = 1); EL3 chondrites (0.01 < δ66Zn < 0.63); the Shallowater aubrite (1.48 < δ66Zn < 2.36); EL6 chondrites (2.26 < δ66Zn < 7.35); and the impact-melt enstatite chondrite Happy Canyon (δ66Zn = 0.37).The aubrite Peña Blanca Spring (δ66Zn = −7.04‰) and the EL6 North West Forrest (δ66Zn = 7.35‰) are the isotopically lightest and heaviest samples, respectively, known so far in the Solar System. In comparison, the range of Zn isotopic composition of chondrites and terrestrial samples (−1.5 < δ66Zn < 1‰) is much smaller ( [Luck et al., 2005] and [Herzog et al., 2009]).EH and EL3 chondrites have the same Zn isotopic composition as the Earth, which is another example of the isotopic similarity between Earth and enstatite chondrites. The Zn isotopic composition and abundance strongly support that the origin of the volatile element depletion between EL3 and EL6 chondrites is due to volatilization, probably during thermal metamorphism. Aubrites show strong elemental depletion in Zn compared to both EH and EL chondrites and they are enriched in light isotopes (δ66Zn down to −7.04‰). This is the opposite of what would be expected if Zn elemental depletion was due to evaporation, assuming the aubrites started with an enstatite chondrite-like Zn isotopic composition. Evaporation is therefore not responsible for volatile loss from aubrites. On Earth, Zn isotopes fractionate very little during igneous processes, while differentiated meteorites show only minimal Zn isotopic variability. It is therefore very unlikely that igneous processes can account for the large isotopic fractionation of Zn in aubrites. Condensation of an isotopically light vapor best explains Zn depletion and isotopically light Zn in these puzzling rocks. Mass balance suggests that this isotopically light vapor carries Zn lost by the EL6 parent body during thermal metamorphism and that aubrites evolved from an EL6-like parent body. Finally, Zn isotopes suggest that Shallowater and aubrites originate from distinct parent bodies.  相似文献   

20.
Zinc smelting and chlor-alkali production are major sources of Hg contamination to the environment, potentially leading to serious impacts on the health of the local population. Huludao, NE China has been heavily contaminated by Hg due to long-term Zn smelting and chlor-alkali production. The aim of this work was to determine Hg accumulation in the aquatic and terrestrial environment, as well as in the human population of Huludao. The investigation included: (a) Hg accumulation in sediments, Spirogyra algae, crucian carp and shrimp, (b) Hg distribution in soil, vegetables and corn, and (c) assessment of potential health effects of Hg exposure associated with total Hg (T-Hg) concentrations in human hair. Measured T-Hg concentrations in sediments of Wuli River ranged from 0.15 to 15.4 mg kg−1, with the maximum Hg concentration in sediment exceeding the background levels in Liaoning Province by 438 times. The maximum T-Hg levels in Spirogyra, crucian carp and shrimp were 13.6, 0.36, and 0.44 mg kg−1, respectively. Total-Hg concentrations in hair of the human population varied from 0.05 to 3.25 mg kg−1 (average 0.43 mg kg−1). However, the frequency of paraesthesia to most inhabitants in Huludao was estimated to be lower than 5%, with only one person rated at 50%. The results indicated minimal adverse health effects of Hg exposure to the inhabitants of Huludao, despite the serious Hg contamination of the environment.  相似文献   

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