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1.
We have carried out a comprehensive survey of the isotopic compositions (H, B, C, N, O, and S) of a suite of interplanetary dust particles (IDPs), including both cluster and individual particles. Isotopic imaging with the NanoSIMS shows the presence of numerous discrete hotspots that are strongly enriched in 15N, up to ∼1300‰. A number of the IDPs also contain larger regions with more modest enrichments in 15N, leading to average bulk N isotopic compositions that are 15N-enriched in these IDPs. Although C isotopic compositions are normal in most of the IDPs, two 15N-rich hotspots have correlated 13C anomalies. CN/C ratios suggest that most of the 15N-rich hotspots are associated with relatively N-poor carbonaceous matter, although specific carriers have not been determined. H isotopic distributions are similar to those of N: D anomalies are present both as distinct D-rich hotspots and as larger regions with more modest enrichments. Nevertheless, H and N isotopic anomalies are not directly correlated, consistent with results from previous studies. Oxygen isotopic imaging shows the presence of abundant presolar silicate grains in some of the IDPs. The O isotopic compositions of the grains are similar to those of presolar oxide and silicate grains from primitive meteorites. Most of the silicate grains in the IDPs have isotopic ratios consistent with meteoritic Group 1 oxide grains, indicating origins in oxygen-rich red giant and asymptotic giant branch stars, but several presolar silicates exhibit the 17O and 18O enrichments of Group 4 oxide grains, whose origin is less well understood. Based on their N isotopic compositions, the IDPs studied here can be divided into two groups. One group is characterized as being “isotopically primitive” and consists of those IDPs that have anomalous bulk N isotopic compositions. These particles typically also contain numerous 15N-rich hotspots, occasional C isotopic anomalies, and abundant presolar silicate grains. In contrast, the other “isotopically normal” IDPs have normal bulk N isotopic compositions and, although some contain 15N-rich hotspots, none exhibit C isotopic anomalies and none contain presolar silicate or oxide grains. Thus, isotopically interesting IDPs can be identified and selected on the basis of their bulk N isotopic compositions for further study. However, this distinction does not appear to extend to H isotopic compositions. Although both H and N anomalies are frequently attributed to the survival of molecular cloud material in IDPs and, thus, should be more common in IDPs with anomalous bulk N compositions, D anomalies are as common in normal IDPs as they are in those characterized as isotopically primitive, based on their N isotopes.  相似文献   

2.
Eight interplanetary dust particles (IDPs) exhibiting a wide range of H and N isotopic anomalies have been studied by transmission electron microscopy, x-ray absorption near-edge structure spectroscopy, and Fourier-transform infrared spectroscopy. These anomalies are believed to have originated during chemical reactions in a cold molecular cloud that was the precursor to the Solar System. The chemical and mineralogical studies reported here thus constitute direct studies of preserved molecular cloud materials. The H and N isotopic anomalies are hosted by different hydrocarbons that reside in the abundant carbonaceous matrix of the IDPs. Infrared measurements constrain the major deuterium (D) host in the D-enriched IDPs to thermally labile aliphatic hydrocarbon groups attached to macromolecular material. Much of the large variation observed in D/H in this suite of IDPs reflects the variable loss of this labile component during atmospheric entry heating. IDPs with elevated 15N/14N ratios contain N in the form of amine (-NH2) functional groups that are likely attached to other molecules such as aromatic hydrocarbons. The host of the N isotopic anomalies is not as readily lost during entry heating as the D-rich material. Infrared analysis shows that while the organic matter in primitive anhydrous IDPs is similar to that observed in acid residues of primitive chondritic meteorites, the measured aromatic:aliphatic ratio is markedly lower in the IDPs.  相似文献   

3.
The Patom Complex is characterized by a unique association of carbonate rocks with ultralow (≤8‰) and ultrahigh (>6‰) δ13C values. The thickness, stable isotopic composition along the strike, and lithological and geochemical parameters suggest that these rocks could not form as a result of short-term local events or epigenetic processes. Ultralow δ13C values (less than ?8‰) in carbonate rocks of the Zhuya Group, which substantially exceed all the known negative C isotope anomalies in thickness (up to 1000 m) and amplitude (δ13C = ?10 ± 2‰), point to sedimentation under conditions of extreme “contamination” of water column by oxidized isotopically light organic (hereafter, light) carbon. The decisive role in this contamination belonged to melting and oxidation of huge volumes of methane hydrates accumulated in sediments during the powerful and prolonged Early Vendian glacial epoch. The accumulation of δ13C-depleted carbonates was preceded by the deposition of carbonates with anomalously high δ13C values. These carbonates formed at high rates of the burial of organic matter and methane in sediments during periods when the sedimentation basin consumed carbon dioxide from the atmosphere and organic carbon was conserved in sediments.  相似文献   

4.
To assess settling particulate organic matter (POM) seasonality and its availability to the benthic community, settling particulate matter was studied in terms of mass fluxes and main biogeochemical characteristics (including organic carbon (OC), nitrogen, and stable carbon and nitrogen isotopic values) at two Lake Superior offshore sites over the course of a year. Fourier transform infrared spectroscopy (FTIR) and hydrolysis, extraction, and derivatization were used to provide further compositional information. Carbon and nitrogen content, isotopic and wet chemical data, and FTIR spectra show that summer particulate material is mainly autochthonous, with higher proportions of amide and carbohydrate. FTIR shows that spring particulate material contains relatively high proportions of clay minerals, indicating major sources from sediment resuspension and/or spring runoff. Distinct amino acid distributions at the two sites, revealed by principal component analysis (PCA) based on amino acid mol% composition, possibly result from differences in OM sources and the degree of degradation occurring at the two sites. Carbohydrate (PCHO), total hydrolyzable amino acid (THAA) and FTIR data suggest that the nutritional value of bulk POM to benthic heterotrophs should be lower in spring than summer-fall, although both periods exhibited high sinking fluxes of total mass and OC. Due to sediment resuspension events and an oxic water column, organic matter eventually buried in Lake Superior’s sediments has probably experienced extensive alteration due to several cycles through the water column and the bacterially-active sediment-water interface.  相似文献   

5.
This work presents geochemical characterization of isolated kerogen out of clay fraction using petrography studies, infrared absorption and solid state 13C nuclear magnetic resonance (NMR) spectroscopy, with N‐alkane distributions of saturated hydrocarbon. Mineralogical study of clay mineral associations was carried out using X‐ray diffraction (XRD), on Ypresian phosphatic series from Gafsa‐Metlaoui basin, Tunisia. The XRD data indicate that smectite, palygorskite and sepiolite are the prevalent clay minerals in the selected samples. In this clay mineral association, the N‐alkane (m/z = 57) distribution indicates that the marine organic matter is plankton and bacterial in origin. The kerogens observed on transmitted light microscopy, however, appear to be totally amorphous organic matter, without any appearance of biological form. The orange gel‐like amorphous organic matter with distinct edges and homogenous texture is consistent with a high degree of aliphaticity. This material has relatively intense CH2 and CH3 infrared bands in 13C NMR peaks. This aliphatic character is related to bacterial origin. Brown amorphous organic matter with diffuse edges has a lower aliphatic character than the previous kerogen, deduced from relatively low CH2 and CH3 infrared and 13C NMR band intensities.  相似文献   

6.
X-ray absorption near-edge structure (XANES) and nuclear magnetic resonance (NMR) spectroscopy were used in combination to characterize organic carbon structures in a series of wetland soils in Saskatchewan, and XANES spectroscopy was also used to examine sulphur speciation in the soils. The organic C contents of most of the wetland soils are consistently higher by a factor of two to five times compared to adjacent well-drained soils. NMR analyses indicate that the organic matter in the wetland soils consists of predominantly aliphatic structures such as carbohydrates and long chain poly(methylene) units which are refractory structures found in plant waxes. The poly(methylene) structures have a significant capacity to sorb nonpolar organic molecules. The phenolic OH and carboxyl group content of the wetland soils studied is an additional significant factor in their sequestering ability for heavy metals or pesticides. Carbon XANES spectroscopy shows that the surface (∼10 nm) layer of particulate organic matter has a structure dominated by aromatic, carbohydrate and carboxylic acid-like material apparently derived from partially degraded lignin and cellulose polymers which are adsorbed onto clay minerals. The aliphatic structures remaining in this surface layer are probably recalcitrant (poly)methylene units. At a depth of ∼100 nm, the aliphatic content significantly increases suggesting the presence of more labile structures. The presence of these more labile aliphatic compounds may be due to slow decomposition rates in the wet, often cool environments present and to the protective action of the more refractory components in the surface ∼10 nm of the organic matter. Drying of the wetlands, either by draining or as a result of climate change, is likely to result in the rapid decomposition of these labile organic structures releasing carbon dioxide. Our data indicate that the preservation of the organic carbon compounds in these soils is a result of their presence as surface adsorbed layers on the soil mineral particles. The soils contain three different classes of sulphur compounds: reduced organic sulphur such as sulphides, low valent oxidized sulphur such as sulphoxides, and high valent oxidized sulphur such as sulphonate and sulphate. Of these, reduced sulphur species constitute between one-third and two-thirds of the total. Sulphonate structures comprise between a fifth and a third of the total. Sulphates exhibit a wide variation in content, and sulphoxides are either not detected or are present to a lesser extent (<5%). Drying of the wetlands would cause oxidation of sulphides to sulphates.  相似文献   

7.
Crystallization of authigenic carbonates in mud volcanoes at Lake Baikal   总被引:1,自引:0,他引:1  
This paper presents data on authigenic siderite first found in surface sediments from mud volcanoes in the Central (K-2) and Southern (Malen’kii) basins of Lake Baikal. Ca is the predominant cation, which substitutes Fe in the crystalline lattice of siderite. The enrichment of the carbonates in the 13C isotope (from +3.3 to +6.8‰ for the Malen’kii volcano and from +17.7 to +21.9‰ for K-2) results from the crystallization of the carbonates during methane generation via the bacterial destruction of organic matter (acetate). The overall depletion of the carbonates in 18O is mainly inherited from the isotopic composition of Baikal water.  相似文献   

8.
三水盆地古近系莘庄组顶部至土布心组红岗段的全岩碳酸盐稳定同位素分析结果表明其形成期间经历了多次环境变迁。根据碳酸盐氧、碳同位素比值及其相互关系的变化,可识别三次海水入侵期。其时δ18O值大幅度向正值漂移。而由于受有机质降解的影响,相应时期的δ13 C均表现为低值。在不直接受海洋影响的湖相沉积阶段,δ18O与δ13 C的相关程度虽然未达到典型的封闭型湖泊水平,但仍呈现一定的正相关变化 (r =0.6 5 ),表明其湖水滞留时间较长。而频繁出现的石膏薄层沉积也指示湖盆的封闭性较好。这些均表明这一时期的三水盆地可能是一周期性封闭型湖泊。其稳定同位素组成主要受制于蒸发量/降雨量平衡的变化。而δ13 C比值往往还受有机质活动的控制,更多的是反映有机质生产力、埋藏与降解率。  相似文献   

9.
This review of the literature from 2004 and 2005 concerning secondary ion mass spectrometry (SIMS) highlights the contribution the technique has made in the fields of petrology, geochronology, cosmochemistry and material sciences. In petrology, much research was devoted to the measurement of stable isotopes and trace elements by developments in multicollection acquisition, with emphasis on low atomic mass number elements. Elements studied in particular were S (in sulfides), O (in garnets), C (in sedimentary organic matter), Cl (in glasses) and Si. Novel applications of SIMS to geochronology have included the measurement of young zircon grains by the U-Pb and U-Th decay methods. An increasing number of studies have combined U-Pb geochronology with the measurement of trace elements or stable isotopes in zircon.  相似文献   

10.
The natural isotopic composition of suspended particulate organic nitrogen was determined in the Southern Bight of the North Sea and in the Scheldt estuary. These data show that δ15N constitutes a convenient tracer of the origin of the suspended matter.In the winter, in the absence of intensive primary production, the suspended organic matter of the Scheldt estuary is a mixture of two components: a continental detrital component characterized by a low δ value of 1.5%. and a marine component with a mean δ value of 8%..During the phytoplankton flowering period, lasting from early May to October, intensive primary production occurs throughout the estuary giving rise to a third source of organic matter. This material is characterized by high δ values reflecting the isotopic composition of ammonia, the nitrogenous nutrient assimilated by phytoplankton in the estuary.The nitrification process occuring in the mixing area of the Scheldt estuary leads to higher downstream δ values of ammonia (>20%.) which permits the distinction between estuarine from fresh-water phytoplankton. Simple isotopic budget calculations show that, both in the upstream part and in the downstream part, autochthonous phytoplanktonic material contributes a major part of the total suspended matter in the Scheldt estuary during summer.  相似文献   

11.
Nodular, cryptocrystalline, weathering-derived magnesite deposits in the New England Orogen, Australia, provide a significant source of high-purity magnesite. Common textural features and related isotopic fingerprints indicate a close genetic relationship between weathering-derived magnesite deposits hosted by ultramafic rocks at Attunga and by sediments at Kunwarara while silica-carbonate rock alteration and rare hydrothermal magnesite vein deposits reflect contrasting conditions of formation. Localised weathering of carbonates in a soil environment shifts stable isotopic composition towards low δ 13C and high δ 18O typical for weathering-derived magnesites while intrusion-related fluids do not significantly change the isotopic composition of affected carbonates. At Attunga, magnesite consists of irregular, nodular veins and masses filling faults and cracks in the weathered serpentinite host rock as well as soft powdery magnesite in pervasive serpentinite alteration zones. The high-grade magnesite at Attunga can be contaminated by amorphous silica and serpentine relicts but does not contain dolomite or ferroan magnesite as observed for its hydrothermal equivalent, the Piedmont magnesite deposit, or other widespread deposits of silica-carbonate rock in the Great Serpentinite Belt. Heavy δ 18O values are compatible with a supergene formation from meteoric waters while low δ 13C suggests C3-photosynthetic plants as the predominant source of carbon for the Attunga magnesites. We infer that weathering-derived, nodular magnesite deposits hosted in ultramafic rocks like the Attunga magnesite deposit have formed in a two-step process involving the hypogene formation of a pre-cursor magnesite deposit and complete supergene overprinting by meteoric waters that acquired carbon from percolation through soil.  相似文献   

12.
The ore-forming material sources of the Baiyangping copper-cobalt-silver polymetallic deposit have been studied in view of the S, Pb, C, O and H isotopic characteristics and the ratio of Co/Ni of cobaltite. The results showed that sulfur in metallic sulfides may have come from a mixed sulfur-source consisting of the sulfur-source from metamorphic rocks in the basin basement with basic volcanic rocks and the sulfur-source from basin sulfates; lead in the ores was provided by the sedimentary rocks and basement rocks; CO2 in ore-forming fluids was derived from thermolysis of altered and normal marine facies carbonates and decarboxylation of sedimentary organic matter respectively; the ore-forming fluids belong to the SO4-Cl-Na-Ca-type basin thermal brines derived from paleo-meteoric waters; cobalt in the deposit may also be derived from the metamorphic rocks in the basin basement with basic volcanic rocks.  相似文献   

13.
古海洋生产力指标研究进展   总被引:20,自引:1,他引:19  
寻求反映古海洋生产力变化的指标是古海洋学研究的重要内容。生物沉积物、营养元素、微量元素和同位素、古生物资料等与古海洋生产力具有一定的关系,常用于古海洋生产力的重建工作:(1)生物沉积物主要包括有机碳、生物碳酸盐和生物硅质沉积等,其埋藏速率在很大程度上受到古海洋生产力的控制,常常用作古海洋生产力的替代性指标;(2)在地质时间尺度上,古海洋生产力主要受到大洋中营养元素可利用程度的控制,因此营养元素的相关记录可以提供古海洋生产力状况的重要信息;(3)海洋中某些微量元素的地球化学行为或者与有机质的改造有关,或者受到氧化还原条件变化的控制,或者受到某种浮游生物的生长的影响,从而能够直接或者间接地指示古海洋生产力的变化;(4)海相碳酸盐和有机质的碳同位素记录,海相有机物的氮同位素比值也用以再造古生产率等古海洋学参数;(5)可以利用对微体化石丰度值及其组合反映古生产力的变化。  相似文献   

14.
介绍了扫描电镜能谱、透射电镜、二次离子质谱、激光微探针质谱、显微傅立叶红外光谱等几种微束分析技术的性能特点,系统地论述了其在有机岩石学在应用现状与进展,并较详细地阐述了利用上述技术研究塔里木盆地烃源岩显微组分的结果。  相似文献   

15.
Late Devonian (Famennian) marine successions globally are typified by organic-rich black shales deposited in anoxic and euxinic waters and the cessation of shelf carbonate sedimentation. This global ‘carbonate crisis’, known as the Hangenberg Event, coincides with a major extinction of reef-building metazoans and perturbations to the global carbon cycle, evidenced by positive carbon-isotope excursions of up to 4‰. It has been suggested that authigenic carbonate, formed as cements in sedimentary pore spaces during early burial diagenesis, is a significant mass fraction of the total global carbon burial flux, particularly during periods of low oxygen concentration. Because some authigenic carbonate could have originated from remineralization of organic carbon in sediments, it is possible for this reservoir to be isotopically depleted and thereby drive changes in the carbon isotopic composition of seawater. This study presents bulk isotopic and elemental analyses from fine-grained siliciclastics of the Late Devonian–Early Mississippian Bakken Formation (Williston Basin, USA) to assess the volume and isotopic composition of carbonates in these sediments. Carbonate in the Bakken black shales occurs primarily as microscopic disseminated dolomite rhombs and calcite cements that, together, comprise a significant mass-fraction (ca 9%). The elemental composition of the shales is indicative of a dynamic anoxic to sulphidic palaeoenvironment, likely supported by a fluctuating chemocline. Despite forming in an environment favourable to remineralization of organic matter and the precipitation of isotopically depleted authigenic carbonates, the majority of carbon isotope measurements of disseminated carbonate fall between −3‰ and +3‰, with systematically more depleted carbonates in the deeper-water portions of the basin. Thus, although there is evidence for a significant total mass-fraction of carbonate with contribution from remineralized organic matter, Bakken authigenic carbonates suggest that Famennian black shales are unlikely to be sufficiently 13C-depleted relative to water column dissolved inorganic carbon to serve as a major lever on seawater isotopic composition.  相似文献   

16.
Abundance, bulk chemical composition and sources of the organic matter in the surface horizon of the permanently water-covered part of an intermittently water-covered marsh were investigated. Lipids, insoluble non-hydrolysable macromolecular organic matter and black carbon fractions were isolated and examined via Rock-Eval pyrolysis, elemental analysis, Fourier transform infrared spectroscopy, isotopic (δ13C, δ15N) methods and high resolution transmission electron microscopy. Integration of bulk Rock-Eval data, elemental and isotopic composition, together with spectroscopic features, suggested immature Type III organic matter derived mainly from C3 vascular plants. The distribution of n-alkanes from the non-aromatic lipid fraction exhibited the importance of emergent macrophytes and terrestrial plants, as well as a moderate input of submerged/floating macrophytes to the source biomass. Mathematical deconvolution of a Rock-Eval pyrogram revealed highly heterogeneous organic matter composed of a mixture of thermally labile biopolymers (36%) at various stages of decomposition, as well as humic substances and highly refractory organic matter (64%) in the whole sample. Markedly lower heterogeneity and aliphaticity, together with a higher proportion of humic substances and highly refractory organic matter (ca. 84%) were observed in the macromolecular fraction. An abundant contribution of black carbon to the macromolecular fraction was indicated by mathematical deconvolution of the Rock-Eval pyrogram and was clearly shown by the isolation of this fraction and chemical oxidation. The black carbon fraction appeared to account for ca. half of the macromolecular fraction, the carbon in these two fractions representing 30% and 14% of the initial carbon, respectively. The electron microscopy observations directly evidenced the presence of black carbon, which was comprised of both amorphous poorly organized particles and highly ordered onion-shaped particles.  相似文献   

17.
通过对南海北部神狐海域Site5B和Site4B站位岩心柱沉积物中自生矿物的类型、形貌特点、丰度和稳定同位素特征的研究,探讨了自生矿物的成因机制。研究表明,沉积物中主要发育黄铁矿和碳酸盐类自生矿物。两个站位中发育的自生矿物的丰度、分布位置、晶体形貌和个体大小等存在明显差异,可能与不同站位中甲烷通量和深部构造有关。自生黄铁矿可能是硫酸盐与甲烷等烃类气体或有机质的厌氧氧化作用的产物,极低负值的硫同位素值可能与硫酸盐还原菌和单质硫歧化菌共同参与有关。自生碳酸盐矿物的成因则相对复杂,其形成过程受多种因素的综合影响。碳同位素值未表现出极低负值,可能是甲烷、有机质和正常海水等碳源混合的结果。  相似文献   

18.
沉积有机质中稳定碳同位素逆转现象初探   总被引:7,自引:3,他引:7  
本文研究了沉积有机质的可溶部分(抽提物)和不溶部分(干酪根)及抽提物的族组分(饱和烃、芳烃、非烃、沥青质)的碳同位素组成特征。通过其δ13C的分布为:干酪根>抽提物;沥青质 >非烃 >芳烃 >饱和烃。研究表明由于生源物质的不同,沉积环境的差异可构沉积有机质碳同位素组成异常。如非烃 >沥青质 >芳烃 >非烃、本文称为沉积有机质碳同位素局部逆转。当沉积有机质可溶部分>干酪根时,称之为总体逆转。湖沼相或河间湖相高等植物来源常为正常组或型;经细菌强烈改造生源以高等植物为主有低等生物为类脂组分加入常形成局部逆转的碳同位素组成。总体逆转则常现于有机质演化程度很高的海相沉积岩中。  相似文献   

19.
The Parnok deposit is made up of stratiform lodes of iron (magnetite) and manganese (oxide-carbonate, carbonate, and carbonate-silicate) ores localized among terrigenous-carbonate sediments (black shales) on the western slope of the Polar Urals. The lithological study showed that ore-bearing sediments were accumulated in a calm hydrodynamic setting within a relatively closed seafloor area (trap depressions). Periodic development of anaerobic conditions in the near-bottom seawater was favorable for the accumulation of dispersed organic matter in the terrigenous-carbonate sediments. Carbon required to form calcium carbonates in the ore-bearing sediments was derived from carbon dioxide dissolved in seawater. In the organic-rich sediments, carbonates were formed with the participation of carbon dioxide released by the destruction of organic matter. However, δ13C values (from 0.5 to ?4.4‰ PDB) suggest a relatively low fraction of the isotopically light biogenic carbon in the host calcite. The most probable sources of Fe and Mn were hydrothermal seepages at the seafloor. The Eh-pH conditions during stagnation were favorable for the precipitation of Fe and accumulation of Mn in a dissolved state. Transition from the stagnation regime to the concentration of oxygen in near-bottom waters was accompanied by oxidation of the dissolved Mn and its precipitation. Thus, fluctuations in Eh-pH parameters of water led to the differentiation of Fe and Mn. Initially, these elements were likely precipitated as oxides and hydroxides. During the subsequent lithification, Fe and Mn were reduced to form magnetite and rhodochrosite. The texture and structure of rhodochrosite aggregates indicate that manganese carbonates already began to form at the diagenetic stage and were recrystallized during the subsequent lithogenetic stages. Isotope data (δ13C from ?8.9 to ?17.1‰ PDB) definitely indicate that the oxidized organic matter of sediment served as the main source of carbon dioxide required to form manganese carbonates. Carbonates from host rocks and manganese ores have principally different carbon isotopic compositions. Unlike carbonates of host rocks, manganese carbonates were formed with an active participation of biogeochemical processes. Further processes of metagenesis (T ≈ 250–300°C, P ≈ 2 kbar) resulted in the transformation of textures, structures, and mineral composition of all rocks of the deposit. In particular, increase in temperature and pressure provided the formation of numerous silicates in manganese ores.  相似文献   

20.
High positive C isotopic ratios in many carbonates coincide with high organic carbon contents. Nahcolites in the Green River oil shales have carbon isotopic ratios up to +20%. Some samples of organic rich Monterey and Pismo Formation dolomites also are 13C-rich (δ13C to +14%.). Combining the observations of unusual isotopic ratios and organic richness has led to proposed mechanisms of formation of nahcolites and dolomites. Bacterial fermentation produces 13C-rich carbon dioxide which in the organic rich sediments is formed in large amounts. This leads to chemical reasons for the occurrence of dolomite rather than calcite and nahcolite rather than trona in some shallow burials.  相似文献   

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