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1.
The carbon geochemistry of serpentinized peridotites and gabbroic rocks recovered at the Lost City Hydrothermal Field (LCHF) and drilled at IODP Hole 1309D at the central dome of the Atlantis Massif (Mid-Atlantic Ridge, 30°N) was examined to characterize carbon sources and speciation in oceanic basement rocks affected by long-lived hydrothermal alteration. Our study presents new data on the geochemistry of organic carbon in the oceanic lithosphere and provides constraints on the fate of dissolved organic carbon in seawater during serpentinization. The basement rocks of the Atlantis Massif are characterized by total carbon (TC) contents of 59 ppm to 1.6 wt% and δ13CTC values ranging from −28.7‰ to +2.3‰. In contrast, total organic carbon (TOC) concentrations and isotopic compositions are relatively constant (δ13CTOC: −28.9‰ to −21.5‰) and variations in δ13CTC reflect mixing of organic carbon with carbonates of marine origin. Saturated hydrocarbons extracted from serpentinites beneath the LCHF consist of n-alkanes ranging from C15 to C30. Longer-chain hydrocarbons (up to C40) are observed in olivine-rich samples from the central dome (IODP Hole 1309D). Occurrences of isoprenoids (pristane, phytane and squalane), polycyclic compounds (hopanes and steranes) and higher relative abundances of n-C16 to n-C20 alkanes in the serpentinites of the southern wall suggest a marine organic input. The vent fluids are characterized by high concentrations of methane and hydrogen, with a putative abiotic origin of hydrocarbons; however, evidence for an inorganic source of n-alkanes in the basement rocks remains equivocal. We propose that high seawater fluxes in the southern part of the Atlantis Massif likely favor the transport and incorporation of marine dissolved organic carbon and overprints possible abiotic geochemical signatures. The presence of pristane, phytane and squalane biomarkers in olivine-rich samples associated with local faults at the central dome implies fracture-controlled seawater circulation deep into the gabbroic core of the massif. Thus, our study indicates that hydrocarbons account for an important proportion of the total carbon stored in the Atlantis Massif basement and suggests that serpentinites may represent an important—as yet unidentified—reservoir for dissolved organic carbon (DOC) from seawater.  相似文献   

2.
Variations in sulfur mineralogy and chemistry of serpentinized peridotites and gabbros beneath the Lost City Hydrothermal Field at the southern face of the Atlantis Massif (Mid-Atlantic Ridge, 30°N) were examined to better understand serpentinization and alteration processes and to study fluid fluxes, redox conditions, and the influence of microbial activity in this active, peridotite-hosted hydrothermal system. The serpentinized peridotites are characterized by low total sulfur contents and high bulk δ34S values close to seawater composition. Low concentrations of 34S-enriched sulfide phases and the predominance of sulfate with seawater-like δ34S values indicate oxidation, loss of sulfide minerals and incorporation of seawater sulfate into the serpentinites. The predominance of pyrite in both serpentinites and gabbros indicates relatively high fO2 conditions during progressive serpentinization and alteration, which likely result from high fluid fluxes during hydrothermal circulation and evolution of the Lost City system from temperatures of ∼250 to 150 °C. Sulfate and sulfide minerals in samples from near the base of hydrothermal carbonate towers at Lost City show δ34S values that reflect the influence of microbial activity. Our study highlights the variations in sulfur chemistry of serpentinized peridotites in different marine environments and the influence of long-lived, moderate temperature peridotite-hosted hydrothermal system and high seawater fluxes on the global sulfur cycle.  相似文献   

3.
The opaque mineralogy and the contents and isotope compositions of sulfur in serpentinized peridotites from the MARK (Mid-Atlantic Ridge, Kane Fracture Zone) area were examined to understand the conditions of serpentinization and evaluate this process as a sink for seawater sulfur. The serpentinites contain a sulfur-rich secondary mineral assemblage and have high sulfur contents (up to 1 wt.%) and elevated δ34Ssulfide (3.7 to 12.7‰). Geochemical reaction modeling indicates that seawater-peridotite interaction at 300 to 400°C alone cannot account for both the high sulfur contents and high δ34Ssulfide. These require a multistage reaction with leaching of sulfide from subjacent gabbro during higher temperature (∼400°C) reactions with seawater and subsequent deposition of sulfide during serpentinization of peridotite at ∼300°C. Serpentinization produces highly reducing conditions and significant amounts of H2 and results in the partial reduction of seawater carbonate to methane. The latter is documented by formation of carbonate veins enriched in 13C (up to 4.5‰) at temperatures above 250°C. Although different processes produce variable sulfur isotope effects in other oceanic serpentinites, sulfur is consistently added to abyssal peridotites during serpentinization. Data for serpentinites drilled and dredged from oceanic crust and from ophiolites indicate that oceanic peridotites are a sink for up to 0.4 to 6.0 × 1012 g seawater S yr−1. This is comparable to sulfur exchange that occurs in hydrothermal systems in mafic oceanic crust at midocean ridges and on ridge flanks and amounts to 2 to 30% of the riverine sulfate source and sedimentary sulfide sink in the oceans. The high concentrations and modified isotope compositions of sulfur in serpentinites could be important for mantle metasomatism during subduction of crust generated at slow spreading rates.  相似文献   

4.
In-situ uplifted portions of oceanic crust at the central dome of the Atlantis Massif (Mid-Atlantic Ridge, 30°N) were drilled during Expeditions 304 and 305 of the Integrated Ocean Drilling Program (IODP) and a 1.4 km section of predominantly gabbroic rocks with minor intercalated ultramafic rocks were recovered. Here we characterize variations in sulfur mineralogy and geochemistry of selected samples of serpentinized peridotites, olivine-rich troctolites and diverse gabbroic rocks recovered from Hole 1309D. These data are used to constrain alteration processes and redox conditions and are compared with the basement rocks of the southern wall of the Atlantis Massif, which hosts the Lost City Hydrothermal Field, 5 km to the south. The oceanic crust at the central dome is characterized by Ni-rich sulfides reflecting reducing conditions and limited seawater circulation. During uplift and exhumation, seawater interaction in gabbroic-dominated domains was limited, as indicated by homogeneous mantle-like sulfur contents and isotope compositions of gabbroic rocks and olivine-rich troctolites. Local variations from mantle compositions are related to magmatic variability or to interaction with seawater-derived fluids channeled along fault zones. The concomitant occurrence of mackinawite in olivine-rich troctolites and an anhydrite vein in a gabbro provide temperature constraints of 150-200 °C for late circulating fluids along local brittle faults below 700 m depth. In contrast, the ultramafic lithologies at the central dome represent domains with higher seawater fluxes and higher degrees of alteration and show distinct changes in sulfur geochemistry. The serpentinites in the upper part of the hole are characterized by high total sulfide contents, high δ34Ssulfide values and low δ34Ssulfate values, which reflect a multistage history primarily controlled by seawater-gabbro interaction and subsequent serpentinization. The basement rocks at the central dome record lower oxygen fugacities and more limited fluid fluxes compared with the serpentinites and gabbros of the Lost City hydrothermal system. Our studies are consistent with previous results and indicate that sulfur speciation and sulfur isotope compositions of altered oceanic mantle sequences commonly evolve over time. Heterogeneities in sulfur geochemistry reflect the fact that serpentinites are highly sensitive to local variations in fluid fluxes, temperature, oxygen and sulfur fugacities, and microbial activity.  相似文献   

5.
Low temperature vent fluids (<91 °C) issuing from the ultramafic-hosted hydrothermal system at Lost City, 30°N Mid-Atlantic Ridge, are enriched in dissolved volatiles (H2,CH4) while attaining elevated pH values, indicative of the serpentization processes that govern water/rock interactions deep in the oceanic crust. Here, we present a series of theoretical models to evaluate the extent of hydrothermal alteration and assess the effect of cooling on the systematics of pH-controlled B aqueous species. Peridotite-seawater equilibria calculations indicate that the mineral assemblage composed of diopside, brucite and chrysotile likely dictates fluid pH at moderate temperature serpentinization processes (<300 °C), by imposing constraints on the aCa++/a2H+ ratios and the activity of dissolved SiO2. Based on Sr abundances and the 87Sr/86Sr isotope ratios of vent fluids reported from Lost City, estimated water/rock mass ratios (w/r = 2-4) are consistent with published models involving dissolved CO2 and alkane concentrations. Combining the reported δ18O values of vent fluids (0.7‰) with such w/r mass ratios, allows us to bracket subseafloor reaction temperatures in the vicinity of 250 °C. These estimates are in agreement with previous theoretical studies supporting extensive conductive heat loss within the upflow zones. Experimental studies on peridotite-seawater alteration suggest that fluid pH increases during cooling which then rapidly enhances boron removal from solution and incorporation into secondary phases, providing an explanation for the highly depleted dissolved boron concentrations measured in the low temperature but alkaline Lost City vent fluids. Finally, to account for the depleted 11B composition (δ11B ∼25-30‰) of vent fluids relative to seawater, isotopic fractionation between tetrahedrally coordinated aqueous boron species with BO3-bearing mineral sites (e.g. in calcite, brucite) is proposed.  相似文献   

6.
The estimation of the fluid/rock (W/R) ratio during serpentinization on the basis of oxygen isotope characteristics is peculiar, because this process is accompanied by not only changes in the stoichiometric proportions of oxygen in fluid and rock, but also by the formation of associated minerals. These factors should be taken into account for environments when the volume of aqueous fluid is limited, for instance, for serpentinization of the deep-seated rocks of oceanic lithosphere under low spreading rates. We studied isotope characteristics of samples collected in dives of submersible MIR during Cruise 50 of the R/V Akademik Mstislav Keldysh along vertical profile on the southern slope of the Atlantis Massif, which hosts the Lost City hydrothermal field. Almost all studied serpentinites have homogenous strontium isotope composition corresponding to the composition of the modern seawater. Oxygen isotope composition of these serpentinites shows systematic variations from 2. 6 to 6.1‰ with sampling depth, which indicates the preservation of stratigraphic position of samples in the sequence of the Atlantis Massif and the global serpentinization of the entire plutonic sequence. The value of the fluid–rock ratio during serpentinization in a system closed to fluid was estimated using the dissolution–crystallization model. This model takes into account the variable stoichiometry of oxygen and the effect of the simultaneous crystallization of brucite on the oxygen isotope composition of newly formed serpentine. The results show that at moderately elevated temperatures (≈300°C) and 0.1 < W/R < 5, fluid, crystallizing serpentine, and brucite are characterized by sharp variations in oxygen isotope composition: 1.3–7.8, 2.5–8.9, and 4.5–1.9‰, respectively. The model explains the observed range of δ18O in the serpentinized harzburgites of the Atlantis Massif. According to our estimates, the rocks of the studied sequence of the Atlantis Massif were serpentinized at 270–350°C and W/R = 0.7–3. For lower temperature serpentinization, for instance, at T = 250°C, the W/R ratio can be as high as 6. The present-day serpentinization of the deepseated zones of the Atlantis Massif with the Lost City fluid participance proceeds at T > 270°C and W/R ratio <1. These conditions are similar to those of serpentinization of harzburgites from the lower parts of the studied sequence of the Atlantis Massif.  相似文献   

7.
Bulk-rock chlorine content and isotopic composition (δ37Cl) were determined in oceanic serpentinites, high-pressure metaperidotites and metasediments in order to gain constraints on the global chlorine cycle associated with hydrothermal alteration and subduction of oceanic lithosphere. The distribution of insoluble chlorine in oceanic serpentinites was also investigated by electron microprobe. The hydrothermally-altered ultramafic samples were dredged along the South West Indian Ridge and the Mid-Atlantic Ridge. The high-pressure metamorphic samples were collected in the Western Alps: metaperidotites in the Erro-Tobbio unit and metasediments in the Schistes Lustrés nappe.Oceanic serpentinites show relatively large variations of bulk-rock Cl contents and δ37Cl values with mean values of 1105 ± 596 ppm and −0.7 ± 0.4‰, respectively (n = 8; 1σ). Serpentines formed after olivine (meshes) show lower Cl content than those formed after orthopyroxene (bastites). In bastites of two different samples, Cl is positively correlated with Al2O3 and negatively correlated with SiO2. These relationships are interpreted as reflecting preferential Cl-incorporation into the bastite structure distorted by Al (substituted for Si) rather than different alteration conditions between olivine and orthopyroxene minerals. High-pressure metaperidotites display relatively homogeneous Cl contents and δ37Cl values with mean values of 467 ± 88 ppm and −1.4 ± 0.1‰, respectively (n = 7; 1σ). A macroscopic high-pressure olivine-bearing vein, formed from partial devolatilization of serpentinites at ∼2.5 GPa and 500-600 °C, shows a Cl content and a δ37Cl value of 603 ppm and −1.6‰, respectively. Metasediments (n = 2) show low whole-rock Cl contents (<15 ppm Cl) that did not allow Cl isotope analyses to be obtained.The range of negative δ37Cl values observed in oceanic serpentinites is likely to result from water-rock interaction with fluids that have negative δ37Cl values. The homogeneity of δ37Cl values from the high-pressure olivine-bearing vein and the metaperidotite samples implies that progressive loss of Cl inherited from oceanic alteration throughout subduction did not significantly fractionate Cl isotopes. Chlorine recycled in subduction zones via metaperidotites should thus show a range of δ37Cl values similar to the range found in oceanic serpentinized peridotites.  相似文献   

8.
We experimentally determined the boron partitioning and boron isotope fractionation between coexisting liquid and vapor in the system H2O−NaCl−B2O3. Experiments were performed along the 400 and 450°C isotherms. Pressure conditions ranged from 23 to 28 MPa at 400°C and from 38 to 42 MPa at 450°C. Boron partitions preferentially into the liquid. Its overall liquid-vapor fractionation is, however, weak: Calculated boron distribution coefficients DBliquid-vapor are < 2.5 at all run conditions. With decreasing pressure (i.e. increasing opening of the solvus) DBliquid-vapor increases along the individual isotherms. Extrapolation to salt saturated conditions yields maximum boron liquid-vapor fractionations of DBliquid-vapor = 1.8 at 450°C and DBliquid-vapor = 2.7 at 400°C. 11B preferentially fractionates into the vapor. Calculated Δ11Bvapor-liquid = {[(11B/10B)vapor - (11B/10B)liquid]/(11B/10B)NBS 951}*1000 are small and range from 0.2 (± 0.7) to 0.9 (± 0.5) ‰ at 450°C and from 0.1 (± 0.6) to 0.7 (± 0.6) ‰ at 400°C. The data indicate increasing isotopic fractionation with decreasing pressure (i.e. increasing opening of the solvus). Extrapolation to salt saturated conditions yields maximum boron isotope liquid-vapor fractionations of Δ11Bvapor-liquid = 1.5 (± 0.7) ‰ at 450°C and Δ11Bvapor-liquid = 1.3 (± 0.6) ‰ at 400°C. The weak boron isotope fractionation suggests similar trigonal speciation in liquid and vapor. Although the boron and boron isotope fractionation between liquid and vapor is only weak, mass balance calculations indicate that for high degrees of fractionation liquid-vapor phase separation in an open system can significantly alter the boron and boron isotope signature of low-salinity hydrous fluids in hydrothermal systems. Comparing the model calculations with natural oceanic hydrothermal fluids, however, indicate that other processes than fluid phase separation dominate the boron geochemistry in oceanic hydrothermal fluids.  相似文献   

9.
The isotopic (δD, δ18O, δ13C, and 87Sr/86Sr) and geochemical characteristics of hydrothermal solutions from the Mid-Atlantic Ridge and the material of brucite-carbonate chimneys at the Lost City hydrothermal field at 30°N, MAR, were examined to assay the role of the major factors controlling the genesis of the fluid and hydrothermal chimneys of the Lost City field. The values of δD and δ18O in fluid samples indicates that solutions at the Lost City field were produced during the serpentinization of basement ultramafic rocks at temperatures higher than 200°C and at relatively low fluid/rock ratios (<1). The active role of serpentinization processes in the genesis of the Lost City fluid also follows from the results of the electron-microscopic studying of the material of hydrothermal chimneys at this field. The isotopic (δ18O, δ13C, and 87Sr/86Sr) and geochemical (Sr/Ca and REE) signatures indicate that, before its submarine discharging at the Lost City field, the fluid filtered through already cold altered outer zones of the Atlantis Massif and cooled via conductive heat loss. During this stage, the fluid could partly dissolve previously deposited carbonates in veins cutting serpentinite at the upper levels of the Atlantis Massif and the carbonate cement of sedimentary breccias underlying the hydrothermal chimneys. Because of this, the age of modern hydrothermal activity at the Lost City field can be much younger than 25 ka.  相似文献   

10.
Boron isotope compositions (δ11B) and B concentrations of rains and snows were studied in order to characterize the sources and fractionation processes during the boron atmospheric cycle. The 11B/10B ratios of instantaneous and cumulative rains and snows from coastal and continental sites show a large range of variations, from −1.5 ± 0.4 to +26.0 ± 0.5‰ and from −10.2 ± 0.5 to +34.4 ± 0.2‰, respectively. Boron concentrations in rains and snows vary between 0.1 and 3.0 ppb. All these precipitation samples are enriched in 10B compared to the ocean value (δ11B = +39.5‰). An empirical rain-vapour isotopic fractionation of +31‰ is estimated from three largely independent methods. The deduced seawater-vapour fractionation is +25.5‰, with the difference between the rain and seawater fractionations principally reflecting changes in the speciation of boron in the liquid with ∼100% B(OH)3 present in precipitations. A boron meteoric water line, δD = 2.6δ11B − 133, is proposed which describes the relationship between δD and δ11B in many, but not all, precipitations. Boron isotopic compositions of precipitations can be related to that of the seawater reservoir by the seawater-vapour fractionation and one or more of (1) the rain-vapour isotopic fractionation, (2) evolution of the δ11B value of the atmospheric vapour reservoir via condensation-precipitation processes (Rayleigh distillation process), (3) any contribution of vapour from the evaporation of seawater aerosols, and (4) any contribution from particulate matter, principally sea salt, continental dust and, perhaps more regionally, anthropogenic sources (burning of biomass and fossil fuels). From the δ11B values of continental precipitations, a sea salt contribution cannot be more than a percent or so of the total B in precipitation over these areas.  相似文献   

11.
Boron isotope composition of marine carbonates has been proposed as a paleo-pH proxy and potential tool to reconstruct atmospheric pCO2. The precise knowledge of the boron isotopic composition of ancient seawater represents the fundamental prerequisite for any paleo-pH reconstruction. This contribution presents boron isotope values for Silurian to Permian brachiopod calcite that might be used to reconstruct pH or boron isotope composition of past oceans. All brachiopod shells were screened for diagenetic recrystallization by means of cathodoluminescence microscopy, trace element geochemistry (B, Fe, Mn, Sr) as well as SEM. Only nonluminescent shells revealing well-preserved microstructures, high strontium and boron concentrations as well as low iron and manganese contents were accepted for boron isotope analysis. The boron isotope ratios of Silurian, Devonian, Pennsylvanian and Permian brachiopod calcite range from 6.8 to 11.0‰, 7.3 to 14.9‰, 12.4 to 15.8‰ and 10.1 to 11.7‰, respectively. These δ11B values are significantly lower in comparison to δ11B values of modern biogenic carbonates and indicate that the Paleozoic oceans were depleted in 11B by up to 10‰. Box modeling of the boron geochemical cycle suggests that the significant depletion of 11B in the oceanic reservoir may have been initiated by an enhanced continental boron discharge. Our data support the earlier made conclusion that boron isotopes may not be used in the geological past as reliable paleo-pH proxy unless the boron isotopic composition of ancient oceans can be constrained by further studies.  相似文献   

12.
We investigate the Logatchev Hydrothermal Field at the Mid-Atlantic Ridge, 14°45′N to constrain the calcium isotope hydrothermal flux into the ocean. During the transformation of seawater to a hydrothermal solution, the Ca concentration of pristine seawater ([Ca]SW) increases from about 10 mM to about 32 mM in the hydrothermal fluid endmember ([Ca]HydEnd) and thereby adopts a δ44/40CaHydEnd of −0.95 ± 0.07‰ relative to seawater (SW) and a 87Sr/86Sr isotope ratio of 0.7034(4). We demonstrate that δ44/40CaHydEnd is higher than that of the bedrock at the Logatchev field. From mass balance calculations, we deduce a δ44/40Ca of −1.17 ± 0.04‰ (SW) for the host-rocks in the reaction zone and −1.45 ± 0.05‰ (SW) for the isotopic composition of the entire hydrothermal cell of the Logatchev field. The values are isotopically lighter than the currently assumed δ44/40Ca for Bulk Earth of −0.92 ± 0.18‰ (SW) [Skulan J., DePaolo D. J. and Owens T. L. (1997) Biological control of calcium isotopic abundances in the global calcium cycle. Geochim. Cosmochim. Acta61,(12) 2505-2510] and challenge previous assumptions of no Ca isotope fractionation between hydrothermal fluid and the oceanic crust [Zhu P. and Macdougall J. D. (1998) Calcium isotopes in the marine environment and the oceanic calcium cycle. Geochim. Cosmochim. Acta62,(10) 1691-1698; Schmitt A. -D., Chabeaux F. and Stille P. (2003) The calcium riverine and hydrothermal isotopic fluxes and the oceanic calcium mass balance. Earth Planet. Sci. Lett. 6731, 1-16]. Here we propose that Ca isotope fractionation along the fluid flow pathway of the Logatchev field occurs during the precipitation of anhydrite. Two anhydrite samples from the Logatchev Hydrothermal Field show an average fractionation of about Δ44/40Ca = −0.5‰ relative to their assumed parental solutions. Ca isotope ratios in aragonites from carbonate veins from ODP drill cores indicate aragonite precipitation directly from seawater at low temperatures with an average δ44/40Ca of −1.54 ± 0.08‰ (SW). The relatively large fractionation between the aragonite precipitates and seawater in combination with their frequent abundance in weathered mafic and ultramafic rocks suggest a reconsideration of the marine Ca isotope budget, in particular with regard to ocean crust alteration.  相似文献   

13.
Carbon and hydrogen concentrations and isotopic compositions were measured in 19 samples from altered oceanic crust cored in ODP/IODP Hole 1256D through lavas, dikes down to the gabbroic rocks. Bulk water content varies from 0.32 to 2.14 wt% with δD values from −64‰ to −25‰. All samples are enriched in water relative to fresh basalts. The δD values are interpreted in terms of mixing between magmatic water and another source that can be either secondary hydrous minerals and/or H contained in organic compounds such as hydrocarbons. Total CO2, extracted by step-heating technique, ranges between 564 and 2823 ppm with δ13C values from −14.9‰ to −26.6‰. As for water, these altered samples are enriched in carbon relative to fresh basalts. The carbon isotope compositions are interpreted in terms of a mixing between two components: (1) a carbonate with δ13C = −4.5‰ and (2) an organic compound with δ13C = −26.6‰. A mixing model calculation indicates that, for most samples (17 of 19), more than 75% of the total C occurs as organic compounds while carbonates represent less than 25%. This result is also supported by independent estimates of carbonate content from CO2 yield after H3PO4 attack. A comparison between the carbon concentration in our samples, seawater DIC (Dissolved Inorganic Carbon) and DOC (Dissolved Organic Carbon), and hydrothermal fluids suggests that CO2 degassed from magmatic reservoirs is the main source of organic C addition to the crust during the alteration process. A reduction step of dissolved CO2 is thus required, and can be either biologically mediated or not. Abiotic processes are necessary for the deeper part of the crust (>1000 mbsf) because alteration temperatures are greater than any hyperthermophilic living organism (i.e. T > 110 °C). Even if not required, we cannot rule out the contribution of microbial activity in the low-temperature alteration zones. We propose a two-step model for carbon cycling during crustal alteration: (1) when “fresh” oceanic crust forms at or close to ridge axis, alteration starts with hot hydrothermal fluids enriched in magmatic CO2, leading to the formation of organic compounds during Fischer-Tropsch-type reactions; (2) when the crust moves away from the ridge axis, these interactions with hot hydrothermal fluids decrease and are replaced by seawater interactions with carbonate precipitation in fractures. Taking into account this organic carbon, we estimate C isotope composition of mean altered oceanic crust at ∼ −4.7‰, similar to the δ13C of the C degassed from the mantle at ridge axis, and discuss the global carbon budget. The total flux of C stored in the altered oceanic crust, as carbonate and organic compound, is 2.9 ± 0.4 × 1012 molC/yr.  相似文献   

14.
Although commonly utilized in continental geothermal work, the water-hydrogen and methane-hydrogen isotope geothermometers have been neglected in hydrothermal studies. Here we report δD-CH4 and δD-H2 values from high-temperature, black smoker-type hydrothermal vents and low-temperature carbonate-hosted samples from the recently discovered Lost City Hydrothermal Field. Methane deuterium content is uniform across the dataset at − 120 ± 12‰. Hydrogen δD values vary from − 420‰ to − 330‰ at high-temperature vents to − 700‰ to − 600‰ at Lost City. The application of several geothermometer equations to a suite of hydrothermal vent volatile samples reveals that predicted temperatures are similar to measured vent temperatures at high-temperature vents, and 20-60 °C higher than those measured at the Lost City vents. We conclude that the overestimation of temperature at Lost City reflects 1) that methane and hydrogen are produced by serpentinization at > 110 °C, and 2) that isotopic equilibrium at temperatures < 70 °C is mediated by microbial sulfate reduction. The successful application of hydrogen isotope geothermometers to low-temperature Lost City hydrothermal samples encourages its employment with low-temperature diffuse hydrothermal fluids.  相似文献   

15.
Eight DSDP/ODP cores were analyzed for major ion concentrations and δ37Cl values of water-soluble chloride (δ37ClWSC) and structurally bound chloride (δ37ClSBC) in serpentinized ultramafic rocks. This diverse set of cores spans a wide range in age, temperature of serpentinization, tectonic setting, and geographic location of drilled serpentinized oceanic crust. Three of the cores were sampled at closely spaced intervals to investigate downhole variation in Cl concentration and chlorine isotope composition.The average total Cl content of all 86 samples is 0.26 ± 0.16 wt.% (0.19 ± 0.10 wt.% as water-soluble Cl (XWSC) and 0.09 ± 0.09 wt.% as structurally bound Cl (XSBC)). Structurally bound Cl concentration nearly doubles with depth in all cores; there is no consistent trend in water-soluble Cl content among the cores. Chlorine isotope fractionation between the structurally bound Cl− site and the water-soluble Cl− site varies from − 1.08‰ to + 1.16‰, averaging to + 0.21‰. Samples with negative fractionations may be related to reequilibration of the water-soluble chloride with seawater post-serpentinite formation. Six of the cores have positive bulk δ37Cl values (+ 0.05‰ to + 0.36‰); the other two cores (173-1068A (Leg-Hole) and 84-570) have negative bulk δ37Cl values (− 1.26‰ and − 0.54‰). The cores with negative δ37Cl values also have variable Cl− / SO42 ratios, in contrast to all other cores. The isotopically positive cores (153-920D and 147-895E) show no isotopic variation with depth; the isotopically negative core (173-1068A) decreases by ∼1‰ with depth for both the water-soluble and structurally bound Cl fractions.Non-zero bulk δ37Cl values indicate Cl in serpentinites was incorporated during original hydration and is not an artifact of seawater infiltration during drilling. Cores with positive δ37Cl values are most likely explained by open system fractionation during hydrothermal alteration, with preferential incorporation of 37Cl from seawater into the serpentinite and loss of residual light Cl back to the ocean. Fluid / rock ratios were probably low as evidenced by the presence of water-soluble salts. The two isotopically negative cores are characterized by a thick overlying sedimentary package that was in place prior to serpentinization. We believe the low δ37Cl values of these cores are a result of hydration of ultramafic rock by infiltrating aqueous pore fluids from the overlying sediments. The resulting serpentinites inherit the characteristic negative δ37Cl values of the pore waters. Chlorine stable isotopes can be used to identify the source of the serpentinizing fluid and ultimately discern chemical and tectonic processes involved in serpentinization.  相似文献   

16.
The Lost City Hydrothermal Field (LCHF) is a serpentinite-hosted vent field located 15 km west of the spreading axis of the Mid-Atlantic Ridge. In this study, uranium-thorium (U-Th) geochronological techniques have been used to examine the U-Th systematics of hydrothermal fluids and the 230Th ages of hydrothermally-precipitated carbonate chimneys at the LCHF. Fluid sample analyses indicate that endmember fluids likely contain only 0.0073 ng/g U or less compared to 3.28 ± 0.03 ng/g of U in ambient seawater. For fluid samples containing only 2-21% ambient seawater (1.1-11 mmol/kg Mg), Th concentration is 0.11-0.13 pg/g and surrounding seawater concentrations average 0.133 ± 0.016 pg/g. The 230Th/232Th atomic ratios of the vent fluids range from 1 (±10) × 10−6 to 11 (±5) × 10−6, are less than those of seawater, and indicate that the vent fluids may contribute a minor amount of non-radiogenic 230Th to the LCHF carbonate chimney deposits. Chimney 238U concentrations range from 1 to 10 μg/g and the average chimney corrected initial δ234U is 147.2 ± 0.8, which is not significantly different from the ambient seawater value of 146.5 ± 0.6. Carbonate 232Th concentrations range broadly from 0.0038 ± 0.0003 to 125 ± 16 ng/g and 230Th/232Th atomic ratios vary from near seawater values of 43 (±8) × 10−6 up to 530 (±25) × 10−3. Chimney ages, corrected for initial 230Th, range from 17 ± 6 yrs to 120 ± 13 kyrs. The youngest chimneys are at the intersection of two active, steeply-dipping normal faults that cut the Atlantis Massif; the oldest chimneys are located in the southwest portion of the field. Vent deposits on a steep, fault-bounded wall on the east side of the field are all <4 kyrs old, indicating that mass wasting in this region is relatively recent. Comparison of results to prior age-dating investigations of submarine hydrothermal systems shows that the LCHF is the most long-lived hydrothermal system known to date. It is likely that seismic activity and active faulting within the Atlantis Massif and the Atlantis Fracture Zone, coupled with volumetric expansion of the underlying serpentinized host rocks play major roles in sustaining hydrothermal activity at this site. The longevity of venting at the LCHF may have implications for ecological succession of microorganisms within serpentinite-hosted vent environments.  相似文献   

17.
Sulfide sulfur in mid-oceanic ridge hydrothermal vents is derived from leaching of basaltic-sulfide and seawater-derived sulfate that is reduced during high temperature water rock interaction. Conventional sulfur isotope studies, however, are inconclusive about the mass-balance between the two sources because 34S/32S ratios of vent fluid H2S and chimney sulfide minerals may reflect not only the mixing ratio but also isotope exchange between sulfate and sulfide. Here, we show that high-precision analysis of S-33 can provide a unique constraint because isotope mixing and isotope exchange result in different Δ33S (≡δ33S-0.515 δ34S) values of up to 0.04‰ even if δ34S values are identical. Detection of such small Δ33S differences is technically feasible by using the SF6 dual-inlet mass-spectrometry protocol that has been improved to achieve a precision as good as 0.006‰ (2σ).Sulfide minerals (marcasite, pyrite, chalcopyrite, and sphalerite) and vent H2S collected from four active seafloor hydrothermal vent sites, East Pacific Rise (EPR) 9-10°N, 13°N, and 21°S and Mid-Atlantic Ridge (MAR) 37°N yield Δ33S values ranging from −0.002 to 0.033 and δ34S from −0.5‰ to 5.3‰. The combined δ34S and Δ33S systematics reveal that 73 to 89% of vent sulfides are derived from leaching from basaltic sulfide and only 11 to 27% from seawater-derived sulfate. Pyrite from EPR 13°N and marcasite from MAR 37°N are in isotope disequilibrium not only in δ34S but also in Δ33S with respect to associated sphalerite and chalcopyrite, suggesting non-equilibrium sulfur isotope exchange between seawater sulfate and sulfide during pyrite precipitation. Seafloor hydrothermal vent sulfides are characterized by low Δ33S values compared with biogenic sulfides, suggesting little or no contribution of sulfide from microbial sulfate reduction into hydrothermal sulfides at sediment-free mid-oceanic ridge systems. We conclude that 33S is an effective new tracer for interplay among seawater, oceanic crust and microbes in subseafloor hydrothermal sulfur cycles.  相似文献   

18.
Xixi Zhao  Masako Tominaga   《Tectonophysics》2009,474(3-4):435-448
Integrated Ocean Drilling Program (IODP) Expeditions 304/305 recovered a total of 1.4 km sequence of lower crustal gabbroic and minor ultramafic rocks from the Atlantis Massif oceanic core complex on the western flank of the Mid Atlantic Ridge (MAR) at 30°N. We conducted an integrated paleomagnetic and rock magnetic study on this sequence to help address the interplay between magmatism and detachment faulting. Detailed thermal and alternating-field demagnetization results demonstrate that stable components of magnetization of mainly reversed polarity with unblocking temperatures below the Curie temperature of magnetite are retained in gabbroic rocks at IODP Site U1309. Several samples also contain multicomponent remanences of both normal and reversed polarities that were acquired over sharply defined blocking temperature intervals, providing evidence for localized reheating of some intervals during both normal and reversed polarity periods. Results from a series of rock magnetic measurements corroborate the demagnetization behavior and show that titanomagnetites are the main magnetic carrier rocks recovered at Site U1309D. The overall magnetic inclination of Hole U1309D is -35°, implying significant (up to ~ 50° counterclockwise, viewed to the north) rotation of the footwall around a horizontal axis parallel to the rift axis (010°) may have occurred. The tectonic rotations inferred by the paleomagnetic data suggest that the original fault orientation dipped relative steeply toward the spreading axis and subsequently rotated to a shallower angle. Coupled with the newly published U–Pb zircon ages for Hole U1309D rocks [Grimes, C.B., John, B.E., Wooden, J.L., 2008. Protracted construction of gabbroic crust at a slow-spreading ridge: Constraints from 206Pb/238U zircon ages from Atlantis Massif and IODP Hole 1309D, (30°N, MAR). Geochem. Geophys. Geosyst. 9, Q08012. doi:1029/2008GC002063], the new paleomagnetic data provide temporal and thermal constraints on the accretion history of the Atlantis Massif.  相似文献   

19.
This paper provides the first measurements of the nitrogen (N) concentrations and isotopic compositions of high- and ultrahigh-pressure mafic eclogites, aimed at characterizing the subduction input flux of N in deeply subducting altered oceanic crust (AOC). The samples that were studied are from the Raspas Complex (Ecuador), Lago di Cignana (Italy), the Zambezi Belt (Zambia) and Cabo Ortegal (Spain), together representing subduction to 50-90 km depths. The eclogites contain 2-20 ppm N with δ15Nair values ranging from −1 to +8‰. These values overlap those of altered oceanic crust, but are distinct from values for fresh MORB (for the latter, ∼1.1 ppm N and δ15Nair ∼ −4‰). Based on N data in combination with other trace element data, the eclogite suites can be subdivided into those that are indistinguishable from their likely protolith, AOC, with or without superimposed effects of devolatilization (Lago di Cignana, Cabo Ortegal), and those that have experienced metasomatic additions during subduction-zone metamorphism (Zambezi Belt, Raspas). For the former group, the lack of a detectable loss of N in the eclogites, compared to various altered MORB compositions, suggests the retention of N in deeply subducted oceanic crust. The metasomatic effects affecting the latter group can be best explained by mixing with a (meta)sedimentary component, resulting in correlated enrichments of N and other trace elements (in particular, Ba and Pb) thought to be mobilized during HP/UHP metamorphism. Serpentinized and high-pressure metamorphosed peridotites, associated with the eclogites at Raspas and Cabo Ortegal, contain 3-15 ppm N with δ15Nair values ranging from +3 to +6‰, significantly higher than the generally accepted values for the MORB mantle (δ15Nair ∼ −5‰). Based on their relatively high N contents and their homogeneous and positive δ15N values, admixing of sedimentary N is also indicated for the serpentinized peridotites.One possible pathway for the addition of sediment-derived N into eclogites and peridotites involves mixing with fluids along the slab-mantle wedge interface. Alternatively, sedimentary N could be incorporated into peridotites during serpentinization at bending-related faults at the outer rise and, during later deserpentinization, released into fluids that then infiltrate overlying rocks. Deep retention of N in subducting oceanic crust should be considered in any attempt to balance subduction inputs with outputs in the form of arc volcanic gases. If materials such as these eclogites and serpentinized peridotites are eventually subducted to beyond sub-arc depths into the deeper mantle, containing some fraction of their forearc-subarc N inventory (documented here), they could deliver isotopically heavy N into the mantle to potentially be sampled by plume-related magmas.  相似文献   

20.
Nitrogen and carbon isotopic compositions, together with mineralogy and trace element geochemistry, were studied in a few kerogen-rich Paleoarchean cherts, a barite and a dolomitic stromatolite belonging to the eastern (Dixon Island Formation) and western (Dresser and Strelley Pool Chert Formations; North Pole Dome and Marble Bar) terranes of Pilbara Craton, Western Australia. The aim of the study was to search for 15N-depleted isotopic signatures, often found in kerogens of this period, and explain the origin of these anomalies. Trace elements suggest silica precipitation by hydrothermal fluids as the main process of chert formation with a contamination from volcanoclastic detritus. This is supported by the occurrence of hydrothermal-derived minerals in the studied samples indicating precipitation temperatures up to 350 °C. Only a dolomitic stromatolite from Strelley Pool shows a superchondritic Y/Ho ratio of 72 and a positive Eu/Eu* anomaly of 1.8, characteristic of chemical precipitates from the Archean seawater. The bulk δ13C vs. δ15N values measured in the cherts show a roughly positive co-variation, except for one sample from the North Pole (PI-85-00). The progressive enrichment in 15N and 13C from a pristine source having δ13C ? −36‰ and δ15N ? −4‰ is correlated with a progressive depletion in N content and to variations in Ba/La and Co/As ratios. These trends have been interpreted as a progressive hydrothermal alteration of the cherts by metamorphic fluids. Isotopic exchange at 350 °C between NH4+(rock) and N2(fluid) may explain the isotopic and elemental composition of N in the studied cherts. However, we need to assume isotopic exchange at 350 °C between carbonate C and graphite to explain the large 13C enrichment recorded. Only sample PI-85-00 shows a large N loss (90%) with a positive δ15N value (+11‰), while C (up to 120 ppm and δ13C −38‰) seems to be unaffected. This pattern has been interpreted as the result of devolatilization and alteration (oxidation) of graphite by low-temperature fluids. The 15N-13C-depleted pristine source has δ 15N values from −7‰ to −4‰ and 40Ar/36Ar ratios from 30,000 to 60,000, compatible with an inorganic mantle N source, although the elemental abundance ratios N/C and 40Ar/C are not exactly the same with the mantle source. The component alternatively could be explained by elemental fractionation from metabolic activity of chemolithoautotrophs and methanogens at the proximity to the hydrothermal vents. However, ambiguities between mantle vs organic sources of N subsist and need further experimental work to be fully elucidated.  相似文献   

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