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1.
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   

2.
Here we report the elemental and isotopic compositions of the insoluble organic material (IOM) isolated from several previously unanalyzed meteorites, as well as the reanalyses of H isotopic compositions of some previously measured samples (Alexander et al., 2007). The IOM in ordinary chondrites (OCs) has very large D enrichments that increase with increasing metamorphism and decreasing H/C, the most extreme δD value measured being almost 12,000‰. We propose that such large isotopic fractionations could be produced in the OC parent bodies through the loss of isotopically very light H2 generated when Fe was oxidized by water at low temperatures (<200 °C). We suggest that similar isotopic fractionations were not generated in the IOM of CV and CO chondrites with similar metamorphic grades and IOM H/C ratios because proportionately less water was consumed during metamorphism, and the remaining water buffered the H isotopic composition of the IOM even a H was being lost from it.Hydrogen would also have been generated during the alteration of CI, CM and CR carbonaceous chondrites. The IOM in these meteorites exhibit a considerable range in isotopic compositions, but all are enriched in D, as well as 15N, relative to terrestrial values. We explore whether these enrichments could also have been produced by the loss of H2, but conclude that the most isotopically anomalous IOM compositions in meteorites from these groups are probably closest to their primordial values. The less isotopically anomalous IOM has probably been modified by parent body processes. The response of IOM to these processes was complex and varied, presumably reflecting differences in conditions within and between parent bodies.The D enrichments associated with H2 generation, along with exchange between D-rich IOM and water in the parent bodies, means that it is unlikely that any chondrites retain the primordial H isotopic composition of the water ice that they accreted. The H isotopic compositions of the most water-rich chondrites, the CMs and CIs, are probably the least modified and their compositions (δD ? −25‰) suggest that their water did not form at large radial distances from the Sun where ice is predicted to be very D-rich. Yet models to explain the O isotopic composition of inner Solar System bodies require that large amounts of ice were transported from the outer to the inner Solar System.  相似文献   

3.
We have conducted the first systematic analyses of molecular distribution and δD values of individual compounds in pyrolysates of insoluble organic matter (IOM) from different carbonaceous chondrite groups, using flash pyrolysis coupled to gas chromatography-mass spectrometry and compound-specific D/H analysis. IOM samples from six meteorites of different classifications, Elephant Moraine (EET) 92042 (CR2), Orgueil (CI1), Allan Hills (ALH) 83100 (CM1/2), Murchison (CM2), ALH 85013 (CM2), and Tagish Lake (C2) were isolated and studied. Except for the pyrolysate of Tagish Lake IOM, pyrolysates of all five meteorite IOM samples were dominated by an extensive series of aromatic (C1 to C7 alkyl-substituted benzenes, C0 to C2 alkyl-substituted naphthalenes), with aliphatic (straight chain and branched C10 to C15 alkanes) hydrocarbons and several S- and O- containing compounds (C1 to C2 alkylthiophenes, benzothiophene, benzaldehyde) being also present. The strong similarity in the pyrolysates of different carbonaceous chondrites suggests certain common characteristics in the formation mechanisms of IOM from different meteorites. The Tagish Lake IOM sample is unique in that its pyrolysate lacks most of the alkyl-substituted aromatic hydrocarbons detected in other meteorite IOM samples, suggesting distinctively different formation processes. Both bulk δD values of meteorite IOMs and weighted-average δD values of individual compounds in pyrolysates show a decreasing trend: CR2 > CI1 > CM2 > C2 (Tagish Lake), with the EET 92042 (CR2) IOM having the highest δD values (∼2000‰ higher than other samples). We attribute the high D contents in the IOM to primitive interstellar organic sources.  相似文献   

4.
All chondrites accreted ∼3.5 wt.% C in their matrices, the bulk of which was in a macromolecular solvent and acid insoluble organic material (IOM). Similar material to IOM is found in interplanetary dust particles (IDPs) and comets. The IOM accounts for almost all of the C and N in chondrites, and a significant fraction of the H. Chondrites and, to a lesser extent, comets were probably the major sources of volatiles for the Earth and the other terrestrial planets. Hence, IOM was both the major source of Earth’s volatiles and a potential source of complex prebiotic molecules.Large enrichments in D and 15N, relative to the bulk solar isotopic compositions, suggest that IOM or its precursors formed in very cold, radiation-rich environments. Whether these environments were in the interstellar medium (ISM) or the outer Solar System is unresolved. Nevertheless, the elemental and isotopic compositions and functional group chemistry of IOM provide important clues to the origin(s) of organic matter in protoplanetary disks. IOM is modified relatively easily by thermal and aqueous processes, so that it can also be used to constrain the conditions in the solar nebula prior to chondrite accretion and the conditions in the chondrite parent bodies after accretion.Here we review what is known about the abundances, compositions and physical nature of IOM in the most primitive chondrites. We also discuss how the IOM has been modified by thermal metamorphism and aqueous alteration in the chondrite parent bodies, and how these changes may be used both as petrologic indicators of the intensity of parent body processing and as tools for classification. Finally, we critically assess the various proposed mechanisms for the formation of IOM in the ISM or Solar System.  相似文献   

5.
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   

6.
Nanoglobules are a form of organic matter found in interplanetary dust particles and primitive meteorites and are commonly associated with 15N and D isotopic anomalies that are suggestive of interstellar processes. We report the discovery of two isotopically-anomalous organic globules from the Stardust collection of particles from Comet 81P/Wild 2 and compare them with nanoglobules from the Murchison CM2 meteorite. One globule from Stardust Cometary Track 80 contains highly aromatic organic matter and a large 15N anomaly (δ15N = 1120‰). Associated, non-globular, organic matter from this track is less enriched in 15N and contains a mixture of aromatic and oxidized carbon similar to bulk insoluble organic material (IOM) from primitive meteorites. The second globule, from Cometary Track 2, contains non-aromatic organic matter with abundant nitrile (CN) and carboxyl (COOH) functional groups. It is significantly enriched in D (δD = 1000‰) but has a terrestrial 15N/14N ratio. Experiments indicate that similar D enrichments, unaccompanied by 15N fractionation, can be reproduced in the laboratory by electron irradiation of epoxy or cyanoacrylate. Thus, a terrestrial origin for this globule cannot be ruled out, and, conversely, exposure to high-energy electron irradiation in space may be an important factor in producing D anomalies in organic materials. For comparison, we report two Murchison globules: one with a large 15N enrichment and highly aromatic chemistry analogous to the Track 80 globule and the other only moderately enriched in 15N with IOM-like chemistry. The observation of organic globules in Comet 81P/Wild 2 indicates that comets likely sampled the same reservoirs of organic matter as did the chondrite parent bodies. The observed isotopic anomalies in the globules are most likely preserved signatures of low temperature (<10 K) chemistry in the interstellar medium or perhaps the outer regions of the solar nebula. In other extraterrestrial samples, D isotopic anomalies, but not those of 15N, may be explained in part by exposure to ionizing electron radiation.  相似文献   

7.
Low molecular weight monocarboxylic acids are the most abundant water soluble organic compounds in the Murchison and many other CM type carbonaceous chondrites. In this study, we examined the monocarboxylic acids in Murchison and EET96029.20 carbonaceous meteorites using a new sample preparation and introduction technique for gas chromatograph recently developed for volatile, water-soluble organic compounds: solid phase micro-extraction (SPME). We identified more than 50 monocarboxylic acids from Murchison compared with the 18 compounds reported previously. Formic acid, a known interstellar molecule, has been fully analyzed in these carbonaceous meteorites, with its δD value suggesting an interstellar origin. We determined both carbon and hydrogen isotopic ratios of individual monocarboxylic acids in Murchison, to better define the origins and genetic relationships of these compounds. The compound-specific isotopic data reveal a large enrichment in 13C (δ13C up to + 32.5‰) and particularly D (δD up to + 2024‰). The branched acids are substantially enriched in both 13C and D relative to the straight chain acids, with those branched acids containing a quaternary carbon showing the greatest isotopic enrichment. The isotopic difference may be attributed to variations in the different synthetic regimes or terrestrial input of straight chain acids.  相似文献   

8.
《Comptes Rendus Geoscience》2007,339(14-15):895-906
Carbonaceous chondrites are characterized by their enrichment in organic matter, mainly represented by insoluble organic matter (IOM), which consists of small aromatic units linked by short-branched aliphatic chains. Furthermore, IOM contains organic radicals heterogeneously distributed along with diradicaloids. These chemical features discriminate IOM from terrestrial counterparts. Isotopic compositions, especially the D/H isotopic ratio, are also distinct. IOM is highly enriched in D (D/H > 350 × 10−6), and the D/H isotopic ratio is heterogeneous. The isotopic composition is the result of interstellar-like processes that could have taken place during the first ages of the protosolar nebula. Chemical structure and isotopic composition clearly show that IOM is synthesized by an abiotic process and is subsequently affected by aqueous alteration or high-temperature metamorphism on the parent body.  相似文献   

9.
Organic carbon (OC) and total nitrogen (TN) concentrations and stable isotope ratios (δ13C, δ15N) of fine (<50 μm) size fractions of deep-sea sediments from the central North Atlantic were employed to identify changes in sources of organic matter over the past 50 ka BP. Ambient glacial sediments are characterised by values that reflect mixtures of marine and terrestrial inputs (averages ± 1σ: OC/TN = 7.6 ± 0.8; δ13C = −22.8 ± 1.0‰; δ15N = 5.5 ± 0.6‰). δ13C, OC, and TN concentrations shift to higher values during the Holocene, indicating a gradual decrease of fine terrigenous supply to the North Atlantic. The unchanged δ15N record between last glacial and Holocene stages indicates that the central North Atlantic region remained oligotrophic at least during the past 50 ka BP, but additional studies are required to support this result in terms of nitrogen oceanic budget. During the phases of enhanced ice-rafted detrital supply corresponding to prominent Heinrich events (HL1, HL2, HL4, and HL5), fine-sized sedimentary organic matter has lower OC and TN concentrations, contrasting sharply with those of ambient glacial sediments. Lower δ13C (down to −28‰) and δ15N (down to 1.6‰) values and high OC:TN ratios (up to 14.7 ± 1.1) are found for HL1, HL2, and with lesser extent for HL4. These values reflect enhanced detrital supply originating from poorly differentiated soil horizons that characterise periglacial climate conditions and from organic matter-bearing rock sources of the underlying geological basement. During HL5, only the δ13C offset records the input of fine size ice-rafted organic matter. Gradually changing soil development conditions during the time interval covering HL5 to HL1 (marine isotope stages 5 to 2), as well as varying erosion levels, have been hypothesized on the basis of constant δ13C, increasing OC/TN and decreasing δ15N values.  相似文献   

10.
The carbon and nitrogen isotope composition of organic matter has been widely used to trace biogeochemical processes in marine and lacustrine environments. In order to reconstruct past environmental changes from sedimentary organic matter, it is crucial to consider potential alteration of the primary isotopic signal by bacterial degradation in the water column and during early diagenesis in the sediments.In a series of oxic and anoxic incubation experiments, we examined the fate of organic matter and the alteration of its carbon and nitrogen isotopic composition during microbial degradation. The decomposition rates determined with a double-exponential decay model show that the more reactive fraction of organic matter degrades at similar rates under oxic and anoxic conditions. However, under oxic conditions the proportion of organic matter resistent to degradation is much lower than under anoxic conditions. Within three months of incubation the δ13C of bulk organic matter decreased by 1.6‰ with respect to the initial value. The depletion can be attributed to the selective preservation of 13C-depleted organic compounds. During anoxic decay, the δ15N values continuously decreased to about 3‰ below the initial value. The decrease probably results from bacterial growth adding 15N-depleted biomass to the residual material. In the oxic experiment, δ15N values increased by more then 3‰ before decreasing to a value indistinguishable from the initial isotopic composition. The dissimilarity between oxic and anoxic conditions may be attributed to differences in the type, timing and degree of microbial activity and preferential degradation. In agreement with the anoxic incubation experiments, sediments from eutrophic Lake Lugano are, on average, depleted in 13C (−1.5‰) and 15N (−1.2‰) with respect to sinking particulate organic matter collected during a long-term sediment trap study.  相似文献   

11.
Ion microprobe measurements of D/H ratios in individual fragments of eight stratospheric dust particles give δD values ranging from ?386 to +2534‰ relative to SMOW. The δD values in five particles far exceed those in terrestrial samples and prove that the samples are interplanetary dust particles (IDPs). The hydrogen isotopic composition is heterogeneous on a scale of a few microns demonstrating that the dust is unequilibrated. Measurements of D/H ratios in conjunction with elemental and molecular ion signals in different fragments of individual IDPs show that a carbonaceous phase, not water, is the carrier of the D enrichments. Previous infrared transmission measurements have shown that IDPs fall into three main spectral classes. Particles from two of those three IR classes show large D/H ratios. Two particles studied from the third class do not. However, one of these contains solar flare tracks and is extraterrestrial. Thus, most, but not all, IDPs contain hydrogen with a non-terrestrial isotopic composition.Carbon isotopic measurements on fragments of three IDPs give ratios similar to terrestrial values and show a largely uniform isotopic composition for a given particle. Small, but significant, differences in δ13C of ~40‰ between particles are seen. No correlations between the hydrogen and carbon isotopic compositions are observed.The magnesium and silicon isotopic compositions of fragments of three IDPs are found to be normal within measurement errors.  相似文献   

12.
Large shifts in the isotopic compositions of organic matter (OM) in lake sediments, over the last few hundred years, are commonly interpreted as representing changes in photosynthetic productivity corresponding to eutrophication or in the input of terrestrial OM due to human disturbances. Based on multiple-proxy data (C:N ratio, δ13C and δ15N of OM, δ13C of calcite, lithology and fossil pollen) from a 700-year sediment core at White Lake, New Jersey (USA), we propose a new explanation that relates these large shifts in OM δ13C and δ15N to human-induced changes in aquatic OM producers. Combined records of geochronology, fossil pollen and lithology from White Lake reveal that the upland forest was cleared by European settlers for farmland beginning around 1745 A.D. and has gradually reforested since 1930 after the abandonment of the farmlands. For the pre-agricultural period, OM had relatively constant but extremely low δ13CVPDB (−35.8 to −34.5‰) and δ15NAir (−3.5 to −2.5‰) and high atomic C:N ratios (13.7 to 16.7), indicating a stable anoxic lake environment with prominent microbial producers. Following the human disturbance (since 1745), high OM mass accumulation rates and abundances of the green alga Pediastrum indicate an increase in aquatic photosynthetic productivity due to enhanced nutrient input from disturbed uplands. However, carbonate δ13C remains constant or even decreases during this period, implying that increasing productivity did not elevate the δ13C of dissolved inorganic carbon and thus cannot explain the observed large increase in OM δ13C (7.4‰) and δ15N (5.8‰) over this period. Instead, δ13C, δ15N and C:N ratios of OM and differences in δ13C between calcite and OM suggest that the large increase in OM δ13C and δ15N can be attributed to a human-induced ecological shift in the predominant organic source from anaerobic bacteria to autotrophic phytoplankton. During the post-agricultural period, mass accumulation rates of OM, carbonate and silicate, and the δ13C of OM and calcite all decreased significantly, corresponding to stabilization of the uplands. However, over the last 70 years, an intensifying aquatic stress from the deposition of 15N-enriched industrial pollutants has resulted in a steady increase of 1.9‰ in δ15N. Proxy records for lake (δ13C and δ15N of OM) and upland conditions (pollen and silicates) at White Lake show complex trajectories of the aquatic and terrestrial ecosystems in response to past human disturbances.  相似文献   

13.
The problems involved with the interpretation of carbon isotopes as indicators for early life in highly metamorphosed early Archean rocks have prompted the search for additional chemical and isotopic biomarkers. Here we report an attempt to identify the origin of carbonaceous matter in the 3.8 Ga old Isua Supracrustal Belt in southern West Greenland by measuring the concentration and isotopic composition of a trapped nitrogen component. Stepped-combustion/pyrolysis-mass spectrometry of carbonaceous matter in several rock samples revealed three different reservoirs of trapped nitrogen: (1) nitrogen associated with a very small amount of reactive carbonaceous material, (2) nitrogen intercalated in graphite, correlated with intercalated radiogenic argon, (3) nitrogen strongly retained at defects or chemically bound in the graphite structure. The δ15N of nitrogen associated with reactive carbonaceous matter (ca. +6‰) overlaps with that of average Phanerozoic sedimentary organic matter, and is believed to be part of nonindigenous postmetamorphic biologic material. In situ Raman spectroscopy confirmed the high degree of crystallinity of the metamorphosed indigenous carbonaceous material, and this material is further referred to as graphite. Graphite interpreted as epigenetic (associated with Mg,Mn-siderite in metacarbonates) contains a very small strongly retained nitrogen component with a low δ15N ratio (−3 to −1‰). This range overlaps with values that are typically found in Archean kerogens, but also those of a metamorphically emplaced inorganic basaltic source. Geological constraints suggest that this graphite incorporated nitrogen from surrounding metabasaltic rocks. Graphite interpreted as syngenetic and biogenic found in a turbidite deposit is relatively similar to this Mg,Mn-siderite-derived graphite, based on degree of graphite crystallinity, amount of trapped radiogenic argon, low nitrogen concentration and δ15N signature. We conclude that nitrogen concentration and its isotope ratio in graphite cannot be used conclusively as a biomarker in these rocks from the highly metamorphosed Isua Supracrustal Belt.  相似文献   

14.
The metal-rich carbonaceous chondrites (CB and CH) have the highest whole-rock 15N-enrichments (δ15N up to 1500‰) among planetary materials. They are also characterized by the absence of interchondrule fine-grained matrix. The only fine-grained material is present as lithic clasts, which experienced extensive aqueous alteration in contrast to the surrounding high-temperature components (chondrules, refractory inclusions, metal grains). Hence, the clasts are foreign objects that were incorporated at a late stage into the final parent body of Isheyevo. Their origin is poorly constrained. Based on mineralogy, petrography, and thermal processing of the aromatic carbonaceous component, different types of clasts have been previously identified in the CB/CH-like chondrite Isheyevo. Here, we focus on the rare lithic clasts characterized by the presence of anhydrous silicates (chondrules, chondrule fragments, and CAIs). Their mineralogy and oxygen isotopic compositions reveal them to be micro-chondrules, fragments of chondrules, and refractory inclusions related to those in the Isheyevo host, suggesting accretion in the same region. In contrast to previously studied IDPs or primitive chondritic matrices, the fine-grained material in the clasts we studied is highly and rather uniformly enriched in heavy nitrogen, with bulk δ15N values ranging between 1000‰ and 1300‰. It is also characterized by the presence of numerous 15N hotspots (δ15N ranging from 1400‰ to 4000‰). No bulk (δD <-240‰) or localized deuterium enrichments were observed. These clasts have the highest bulk enrichment in heavy nitrogen measured to date in a fine-grained material. They represent a unique material, of asteroidal or cometary origin, in our collection of cosmomaterials. We show that they were 15N-enriched before their incorporation in the final parent body of Isheyevo. They experienced an extensive aqueous alteration that most likely played a role in redistributing 15N over the whole fine-grained material and may have significantly modified its initial hydrogen isotopic composition. Based on a review of isotopic fractionation models, we conclude that the nitrogen isotopic fractionation process, its timing, and its location are still poorly constrained. The 15N-rich clasts may represent the surviving original carrier of the 15N anomaly in Isheyevo whole-rock.  相似文献   

15.
Carbonaceous matter occurring in chert deposits of the 3.4-3.2 Ga old Barberton Greenstone Belt (BGB), South Africa, has experienced low grade regional metamorphism and variable degrees of local hydrothermal alteration. Here a detailed study is presented of in situ analysis of carbonaceous particles by LRS (laser Raman spectroscopy) and SIMS (secondary ion mass spectrometry), reporting degree of structural disorder, carbon isotope ratio and nitrogen-to-carbon ratio. This combination of in situ analytical tools is used to interpret the δ13C values of only the best preserved carbonaceous remains, enabling the rejection of non-indigenous (unmetamorphosed) material as well as the exclusion of strongly hydrothermally altered carbonaceous particles. Raman spectroscopy confirmed that all carbonaceous cherts studied here have experienced a regional sub- to lower-greenschist facies metamorphic event. Although this identifies these organics as indigenous to the cherts, it is inferred from petrographic observations that hydrothermal alteration has caused small scale migration and re-deposition of organics. This suggest that morphological interpretation of these carbonaceous particles, and in general of putative microfossils or microlaminae in hydrothermally altered early Archean cherts, should be made with caution. A chert in the Hooggenoeg Formation, which is older than and has been hydrothermally altered by a volcanic event 3445 Ma ago, contains strongly altered carbonaceous particles with a uniform N/C-ratio of 0.001 and a range of δ13C that is shifted from its original value. Cherts of the Kromberg Formation post-date this volcanic event, and contain carbonaceous particles with a N/C-ratio between 0.002 and 0.006. Both the Buck Reef Chert and the Footbridge Chert of the Kromberg Formation have retained fairly well-preserved δ13C values, with ranges from −34‰ to −24‰ and −40‰ to −32 ‰, respectively. Abiologic reactions associated with hydrothermal serpentinization of ultramafic crust (such as Fischer-Tropsch synthesis) were an unlikely source for carbonaceous material in these cherts. The carbonaceous matter in these cherts has all the characteristics of metamorphosed biologic material.  相似文献   

16.
High molecular weight dissolved organic matter (HMW-DOM) represents an important component of dissolved organic carbon (DOC) in seawater and fresh-waters. In this paper, we report measurements of stable carbon (δ13C) isotopic compositions in total lipid, total hydrolyzable amino acid (THAA), total carbohydrate (TCHO) and acid-insoluble “uncharacterized” organic fractions separated from fourteen HMW-DOM samples collected from four U.S. estuaries. In addition, C/N ratio, δ13C and stable nitrogen (δ15N) isotopic compositions were also measured for the bulk HMW-DOM samples. Our results indicate that TCHO and THAA are the dominant organic compound classes, contributing 33-46% and 13-20% of the organic carbon in HMW-DOM while total lipid accounts for only <2% of the organic carbon in the samples. In all samples, a significant fraction (35-49%) of HMW-DOM was included in the acid-insoluble fraction. Distinct differences in isotopic compositions exist among bulk samples, the compound classes and the acid-insoluble fractions. Values of δ13C and δ15N measured for bulk HMW-DOM varied from −22.1 to −30.1‰ and 2.8 to 8.9‰, respectively and varied among the four estuaries studied as well. Among the compound classes, TCHO was more enriched in 13C (δ13C = −18.5 to −22.8‰) compared with THAA (δ13C = −20.0 to −29.6‰) and total lipid (δ13C = −25.7 to −30.7‰). The acid-insoluble organic fractions, in general, had depleted 13C values (δ13C = −23.0 to −34.4‰). Our results indicate that the observed differences in both δ13C and δ15N were mainly due to the differences in sources of organic matter and nitrogen inputs to these estuaries in addition to the microbial processes responsible for isotopic fractionation among the compound classes. Both terrestrial sources and local sewage inputs contribute significantly to the HMW-DOM pool in the estuaries studied and thus had a strong influence on its isotopic signatures.  相似文献   

17.
The detailed examination of meteorites and interplanetary dust particles provides an opportunity to infer the origin of the organic matter found in primitive Solar System materials. If this organic matter were produced by aqueous alteration of elemental (graphitic or amorphous) carbon on an asteroid, then we would expect to see the organic matter occurring preferentially in interplanetary materials that exhibit evidence of aqueous activity, such as the presence of hydrated silicates. On the other hand, if the organic matter were produced either during the nebula phase of Solar System evolution or in the interstellar medium, we might expect this organic matter to be incorporated into the dust as it formed. In that case pre-biotic organic matter would be present in both the anhydrous and the hydrated interplanetary materials. We have performed carbon X-ray absorption near-edge structure spectroscopy and infrared spectroscopy on primitive anhydrous and hydrated interplanetary dust particles (IDPs) collected by NASA from the Earth's stratosphere. We find that organic matter is present in similar types and abundances in both the anhydrous and the hydrated IDPs, and, in the anhydrous IDPs some of this organic matter is the “glue” that holds grains together. These measurements provide the first direct, experimental evidence from the comparison of extraterrestrial samples that the bulk of the pre-biotic organic matter occurs in similar types and abundances in both hydrated and anhydrous samples. This indicates that the bulk of the pre-biotic organic matter in the Solar System did not form by aqueous processing, but, instead, had already formed at the time that primitive, anhydrous dust was being assembled. Thus, the bulk of the pre-biotic organic matter in the Solar System was formed by non-aqueous processing, occurring in either the Solar nebula or in an interstellar environment. Aqueous processing on asteroids may have altered this pre-existing organic matter, but such processing did not affect in any substantial way the C=O content of the organic matter, the aliphatic C-H abundance, or the mean aliphatic chain length.  相似文献   

18.
We measured molecular distributions and compound-specific hydrogen (δD) and stable carbon isotopic ratios (δ13C) of mid- and long-chain n-alkanes in forest soils, wetland peats and lake sediments within the Dorokawa watershed, Hokkaido, Japan, to better understand sources and processes associate with delivery of terrestrial organic matter into the lake sediments. δ13C values of odd carbon numbered C23-C33n-alkanes ranged from −37.2‰ to −31.5‰, while δD values of these alkanes showed a large degree of variability that ranged from −244‰ to −180‰. Molecular distributions in combination with stable carbon isotopic compositions indicate a large contribution of C3 trees as the main source of n-alkanes in forested soils whereas n-alkanes in wetland soil are exclusively derived from marsh grass and/or moss. We found that the n-alkane δD values are much higher in forest soils than wetland peat. The higher δD values in forest samples could be explained by the enrichment of deuterium in leaf and soil waters due to increased evapotranspiration in the forest or differences in physiology of source plants between wetland and forest. A δ13C vs. δD diagram of n-alkanes among forest, wetland and lake samples showed that C25-C31n-alkanes deposited in lake sediments are mainly derived from tree leaves due to the preferential transport of the forest soil organic matter over the wetland or an increased contribution of atmospheric input of tree leaf wax in the offshore sites. This study demonstrates that compound-specific δD analysis provides a useful approach for better understanding source and transport of terrestrial biomarkers in a C3 plant-dominated catchment.  相似文献   

19.
The carbonaceous chondrites contain significant amounts of carbon- and nitrogen-bearing components, the most abundant of which is organic matter. Stepped combustion data of whole rock and HF/HCl residues of carbonaceous chondrites reveal that the organic material can be subdivided operationally into three components: (1) free organic matter (FOM), which is readily extractable from whole-rock meteorites and is enriched in 13C and 15N; (2) labile organic matter (LOM), which has a macromolecular structure but is liberated by hydrous pyrolysis; LOM is the parent structure for some FOM and is also enriched in 13C and 15N; and (3) refractory organic matter (ROM), which is also macromolecular but is virtually unaffected by hydrous pyrolysis and is relatively depleted in 13C and 15N. The macromolecular entities (LOM and ROM) are by far the most abundant organic components present, and as such, the relative abundances of the 13C- and 15N-enriched LOM and the 13C- and 15N-depleted ROM will have a major influence on the overall isotopic composition of the whole-rock meteorite. Laboratory experiments designed to simulate the effects of parent body aqueous alteration indicate that this form of processing removes LOM from the macromolecular material, allowing ROM to exert a stronger influence on the overall isotopic compositions. Hence, aqueous alteration of macromolecular materials on the meteorite parent body may have a significant control on the stable isotopic compositions of whole-rock carbonaceous chondrites. The enstatite chondrites are also carbon rich but have been subjected to high levels of thermal metamorphism on their parent body. Stepped combustion data of HF/HCl residues of enstatite chondrites indicate, that if they and carbonaceous chondrites inherited a common organic progenitor, metamorphism under reducing conditions appears to incorporate and preserve some of the 13C enrichments in LOM during graphitisation. However, when metamorphism is at its most extreme, the 15N enrichments in LOM are lost.  相似文献   

20.
The δD values of over 40 amino acids and two pyridine carboxylic acids of the Murchison and Murray meteorites have been obtained by compound-specific isotopic analyses. For compounds with no known terrestrial distribution, these values range from approximately +330‰ (for cyclic leucine) to +3600‰ (for 2-amino-2,3-dimethylbutyric acid). The latter value is the highest ever recorded for a soluble organic compound in meteorites and nears deuterium to hydrogen ratios observed remotely in interstellar molecules. Deuterium content varies significantly between molecular species and is markedly higher for amino acids having a branched alkyl chain. The δD value of Murray l-isovaline, with an enantiomeric excess of ∼ 6% in the meteorite, was within experimental error of that determined for the combined dl-isovaline enantiomers. Overall, the hydrogen isotope composition of meteoritic amino acids is relatively simple and their δD values appear to vary more with the structure of their carbon chains than with the number and relative distribution of their functionalities or 13C content. The magnitude and extent of deuterium enrichment shared by many and varied amino acids in meteorites indicate that cosmic regimes such as those found in the interstellar medium were capable of producing, if not all the amino acids directly, at least a suite of their direct precursors that was abundant, varied, and considerably saturated.  相似文献   

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