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1.
Abstract— A new insight into carbon and hydrogen isotope variations of insoluble organic matter (IOM) is provided from seven CM chondrites, including Murchison and six Antarctic meteorites (Y‐791198, Y‐793321, A‐881280, A‐881334, A‐881458 and B‐7904) as well as Murchison IOM residues after hydrous pyrolysis at 270–330 °C for 72 h. Isotopic compositions of bulk carbon (δ13Cbulk) and hydrogen (δD) of the seven IOMs vary widely, ranging from ?15.1 to ?7.6%0 and +133 to +986%0, respectively. Intramolecular carboxyl carbon (δ13CCOOH) is more enriched in 13C by 7.5. 11%0 than bulk carbon. After hydrous pyrolysis of Murchison IOM at 330 °C, H/C ratio, δ13Cbulk, δ13CCOOH, and δD values decrease by up to 0.31, 3.5%0, 5.5%0, and 961%0, respectively. The O/C ratio increases from 0.22 to 0.46 at 270 °C and to 0.25 at 300 °C, and decreases to 0.10 at 330 °C. δ13Cbulk‐δD cross plot of Murchison IOM and its pyrolysis residues shows an isotopic sequence. Of the six Antarctic IOMs, A‐881280, A‐881458, Y‐791198 and B‐7904 lie on or near the isotopic sequence depending on the degree of hydrous and/or thermal alteration, while A‐881334 and Y‐793321 consist of another distinct isotope group. A δ13Cbulk‐δ13CCOOH cross‐plot of IOMs, including Murchison pyrolysis residues, has a positive correlation between them, implying that the oxidation process to produce carboxyls is similar among all IOMs. These isotope distributions reflect various degree of alteration on the meteorite parent bodies and/or difference in original isotopic compositions before the parent body processes.  相似文献   

2.
Two petrographic settings of carbonaceous components, mainly filling open fractures and occasionally enclosed in shock‐melt veins, were found in the recently fallen Tissint Martian meteorite. The presence in shock‐melt veins and the deuterium enrichments (δD up to +1183‰) of these components clearly indicate a pristine Martian origin. The carbonaceous components are kerogen‐like, based on micro‐Raman spectra and multielemental ratios, and were probably deposited from fluids in shock‐induced fractures in the parent rock of Tissint. After precipitation of the organic matter, the rock experienced another severe shock event, producing the melt veins that encapsulated a part of the organic matter. The C isotopic compositions of the organic matter (δ13C = ?12.8 to ?33.1‰) are significantly lighter than Martian atmospheric CO2 and carbonate, providing a tantalizing hint for a possible biotic process. Alternatively, the organic matter could be derived from carbonaceous chondrites, as insoluble organic matter from the latter has similar chemical and isotopic compositions. The presence of organic‐rich fluids that infiltrated rocks near the surface of Mars has significant implications for the study of Martian paleoenvironment and perhaps to search for possible ancient biological activities on Mars.  相似文献   

3.
Planetary noble gases in chondrites are concentrated in an unidentified carrier phase, called “Q.” Phase Q oxidized at relatively low temperature in pure oxygen is a very minor part of insoluble organic matter (IOM), but has not been separated in a pure form. High‐pressure (HP) experiments have been used to test the effects of thermal metamorphism on IOM from the Orgueil (CI1) meteorite, at conditions up to 10 GPa and 700 °C. The effect of the treatment on carbon structural order was characterized by Raman spectroscopy of the carbon D and G bands. The Raman results show that the IOM becomes progressively more graphite‐like with increasing intensity and duration of the HP treatment. The carbon structural transformations are accompanied by an increase in the release temperatures for IOM carbon and 36Ar during stepped combustion (the former to a greater extent than the latter for the most HP treated sample) when compared with the original untreated Orgueil (CI1) sample. The 36Ar/C ratio also appears to vary in response to HP treatment. Since 36Ar is a part of Q, its release temperature corresponds to that for Q oxidation. Thus, the structural transformations of Q and IOM upon HP treatment are not equal. These results correspond to observations of thermal metamorphism in the meteorite parent bodies, in particular those of type 4 enstatite chondrites, e.g., Indarch (EH4), where graphitized IOM oxidized at significantly higher temperatures than Q (Verchovsky et al. 2002 ). Our findings imply that Q is less graphitized than most of the macromolecular carbonaceous material present during parent body metamorphism and is thus a carbonaceous phase distinct from other meteoritic IOM.  相似文献   

4.
Abstract– The insoluble organic matter (IOM) of an unequilibrated enstatite chondrite Sahara (SAH) 97096 has been investigated using a battery of analytical techniques. As the enstatite chondrites are thought to have formed in a reduced environment at higher temperatures than carbonaceous chondrites, they constitute an interesting comparative material to test the heterogeneities of the IOM in the solar system and to constrain the processes that could affect IOM during solar system evolution. The SAH 97096 IOM is found in situ: as submicrometer grains in the network of fine‐grained matrix occurring mostly around chondrules and as inclusions in metallic nodules, where the carbonaceous matter appears to be more graphitized. IOM in these two settings has very similar δ15N and δ13C; this supports the idea that graphitized inclusions in metal could be formed by metal catalytic graphitization of matrix IOM. A detailed comparison between the IOM extracted from a fresh part and a terrestrially weathered part of SAH 97096 shows the similarity between both IOM samples in spite of the high degree of mineral alteration in the latter. The isolated IOM exhibits a heterogeneous polyaromatic macromolecular structure, sometimes highly graphitized, without any detectable free radicals and deuterium‐heterogeneity and having mean H‐ and N‐isotopic compositions in the range of values observed for carbonaceous chondrites. It contains some submicrometer‐sized areas highly enriched in 15N (δ15N up to 1600‰). These observations reinforce the idea that the IOM found in carbonaceous chondrites is a common component widespread in the solar system. Most of the features of SAH 97096 IOM could be explained by the thermal modification of this main component.  相似文献   

5.
Insoluble organic matter (IOM) and hydrothermally treated IOM extracted from two carbonaceous chondrites, Murchison and Allende, was studied using sulfur K‐edge XANES (X‐ray absorption near edge structure) and μ‐Raman spectroscopy, with the aim to understand their IOM's sulfur speciation and structural order, and how aqueous alteration or thermal metamorphism may have transformed these materials. We found that the sulfur‐functional group chemistry of both the Murchison IOM and hydrothermally treated IOM samples have a large chemical variability ranging from oxidation states of S?2 to S+6, and exhibit a transformation in their oxidation state after the hydrothermal treatment (HT) to produce thiophenes and thiol compounds. Sulfoxide and sulfite peaks are also present in Murchison. Sulfates considered intrinsic to Murchison are most likely preaccretionary in nature, and not a result of reactions with water at high temperatures on the asteroid parent body. We argue that the reduced sulfides may have formed in the CM parent body, while the thiophenes and thiol compounds are a result of the HT. Micro‐Raman spectra show the presence of aliphatic and aromatic moieties in Murchison's material as observed previously, which exhibits no change after HT. Because the Murchison IOM was modified, as seen by XANES analysis, absence of a change observed using micro‐Raman indicated that although the alkyl carbons of IOM were cleaved, the aromatic network was not largely modified after HT. By contrast, Allende IOM contains primarily disulfide and elemental sulfur, no organic sulfur, and shows no transformation after HT. This nontransformation of Allende IOM after HT would indicate that parent body alteration of sulfide to sulfate is not feasible up to temperatures of 300°C. The reduced sulfur products indicate extreme secondary chemical processing from the precursor compounds in its parent body at temperatures as high as 624°C, as estimated from μ‐Raman D band parameters. The Raman parameters in Allende IOM that was interpreted in terms of amorphous carbon with regions of large clusters of benzene rings, was transformed after the HT to those with fewer benzene rings.  相似文献   

6.
Abstract— We report on the molecular analyses of the water‐ and solvent‐soluble organic compounds released from the insoluble organic material (IOM) of the Murray meteorite upon treatment with weight‐equivalent amounts of water and under conditions of elevated temperature and pressure. A varied suite of compounds was identified by gas chromatography‐mass spectrometry (GC‐MS). C3‐C17 alkyl dicarboxylic acids and N‐ and O‐containing hydroaromatic and aromatic compounds were found in the water extracts. The solvent extracts contained N‐, O‐, and S‐containing aromatic compounds, a large number of their isomers and homologs, and a series of polycyclic aromatic hydrocarbons (PAHs) of up to five rings, together with noncondensed aromatic species such as substituted benzenes, biphenyl, and terphenyls as well as their substituted homologs, and hydrated PAHs. Isotopic analyses showed that residue IOMs after hydrothermal treatment had lower deuterium and 15N content than the untreated material (ΔD = ?833‰ and Δ15N = ?24.1) but did not differ from it in 13C composition. The effect of the hydrothermolytic release was recorded in significant differences between the NMR spectra of untreated and residue IOM. A possible relation to common precursors for the dicarboxylic acids found in the IOM and bulk extracts is discussed.  相似文献   

7.
Abstract– Insight into the chemical history of an ungrouped type 2 carbonaceous chondrite meteorite, Wisconsin Range (WIS) 91600, is gained through molecular analyses of insoluble organic matter (IOM) using solid‐state 13C nuclear magnetic resonance (NMR) spectroscopy, X‐ray absorption near edge structure spectroscopy (XANES), and pyrolysis‐gas chromatography coupled with mass spectrometry (pyr‐GC/MS), and our previous bulk elemental and isotopic data. The IOM from WIS 91600 exhibits similarities in its abundance and bulk δ15N value with IOM from another ungrouped carbonaceous chondrite Tagish Lake, while it exhibits H/C, δ13C, and δD values that are more similar to IOM from the heated CM, Pecora Escarpment (PCA) 91008. The 13C NMR spectra of IOM of WIS 91600 and Tagish Lake are similar, except for a greater abundance of CHxO species in the latter and sharper carbonyl absorption in the former. Unusual cross‐polarization (CP) dynamics is observed for WIS 91600 that indicate the presence of two physically distinct organic domains, in which the degrees of aromatic condensation are distinctly different. The presence of two different organic domains in WIS 91600 is consistent with its brecciated nature. The formation of more condensed aromatics is the likely result of short duration thermal excursions during impacts. The fact that both WIS 91600 and PCA 91008 were subjected to short duration heating that is distinct from the thermal history of type 3 chondrites is confirmed by Carbon‐XANES. Finally, after being briefly heated (400 °C for 10 s), the pyrolysis behavior of Tagish Lake IOM is similar to that of WIS 91600 and PCA 91008. We conclude that WIS 91600 experienced very moderate, short duration heating at low temperatures (<500 °C) after an episode of aqueous alteration under conditions that were similar to those experienced by Tagish Lake.  相似文献   

8.
Abstract– To evaluate kinetic parameters for thermal degradation of organic matter, in situ heating experiments of insoluble organic matter (IOM) and bulk of Murchison (CM2) meteorite were conducted under Fourier transform infrared micro‐spectroscopy combined with a heating stage. Decreases of aliphatic C–H band area under Ar flow were well fitted with Ginstling‐Brounshtein three‐dimensional diffusion model, and the rate constants for decreases of aliphatic C–H were determined. Activation energies Ea and frequency factors A obtained from these rate constants at different temperatures using the Arrhenius equation were Ea = 109 ± 3 kJ mol?1 and A = 8.7 × 104 s?1 for IOM, and Ea = 61 ± 6 kJ mol?1 and A = 3.8 s?1 for bulk, respectively. Activation energy values of aliphatic C–H decrease are larger for IOM than bulk. Hence, the mineral assemblage of the Murchison meteorite might have catalytic effects for the organic matter degradation. Using obtained kinetic expressions, the time scale for metamorphism can be estimated for a given temperature with aliphatic C–H band area, or the temperature of metamorphism can be estimated for a given time scale. For example, using the obtained kinetic parameters of IOM, aliphatic C–H is lost approximately within 200 years at 100 °C and 100 Myr at 0 °C. Assuming alteration period of 7.5 Myr, alteration temperatures could be calculated to be <15 ± 12 °C. Aliphatic C–H decrease profiles in a parent body can be estimated using time–temperature history model. The kinetic expression obtained by the infrared spectral band of aliphatic C–H could be used as an alternative method to evaluate thermal processes of organic matter in carbonaceous chondrites.  相似文献   

9.
Abstract— Chemical structures of the insoluble organic matter (IOM) from the Antarctic CM2 chondrites (Yamato [Y‐] 791198, 793321; Belgica [B‐] 7904; Asuka [A‐] 881280, 881334) and the Murchison meteorite were analyzed by solid‐state 13C nuclear magnetic resonance (NMR) spectroscopy. Different types of carbons were characterized, such as aliphatic carbon (Ali‐C), aliphatic carbon linked to hetero atom (Hetero‐Ali‐C), aromatic carbon (Aro‐C), carboxyls (COOR), and carbonyls (C=O). The spectra of the IOM from Murchison and Y‐791198 showed two major peaks: Ali‐C and Aro‐C, while the spectra from the other meteorites showed only one major peak of Aro‐C. Carbon distribution was determined both by manual integration and deconvolution. For most IOM, the Aro‐C was the most abundant (49.8–67.8%) of all carbon types. When the ratios of Ali‐C to Aro‐C (Ali/Aro) were plotted with the atomic hydrogen to carbon ratio (H/C), a correlation was observed. If we use the H/C as a parameter for the thermal alteration event on the meteorite parent body, this result shows a different extent of thermal alteration. In addition, IOM with a lower Ali/Aro showed a lower ratio of Ali‐C to COOR plus C=O (Ali / (COOR + C=O)). This result suggests that the ratio of CO moieties to aliphatic carbon in IOM might reflect chemical oxidation that was involved in hydrothermal alteration.  相似文献   

10.
Past studies of the various separable carbonaceous fractions have been unable to account for all of C in primitive chondrites. In particular, up to 20–50% of the C is lost during acid leaching of bulk samples even after the C in carbonates and soluble organic matter is accounted for. To try to better characterize the nature of this “missing C,” we have compared the bulk infrared (IR) absorption spectra of a number of primitive chondrites with those of their previously reported insoluble organic matter (IOM). The aliphatic C–H stretching bands, in particular, allow us to compare the molecular structures of bulk C with that of IOM. The spectral differences between bulk C and IOM reflect “missing C” phases that were lost during acid leaching, although we cannot completely exclude the possibility that the OM was modified after demineralization. Comparing IR spectra of bulk meteorite powder and IOM suggests that the missing C varies in its molecular structure, and that mildly thermally metamorphosed type 3 chondrites tend to be richer in an aliphatic fraction with lower CH2/CH3 ratios, relative to IOM, compared to aqueously altered carbonaceous chondrites (CI/CM/CR). The missing C is most likely released from acid‐labile functional groups, such as esters, acetals, and amides, during demineralization, although it cannot be ruled out that some fraction of the missing C is in small grains that are difficult to recover from suspension, or in water‐soluble compounds trapped in phyllosilicates.  相似文献   

11.
Effects of aqueous alteration on primordial noble gas carriers were investigated by analyzing noble gases and determining presolar SiC abundances in insoluble organic matter (IOM) from four Tagish Lake meteorite (C2‐ung.) samples that experienced different degrees of aqueous alteration. The samples contained a mixture of primordial noble gases from phase Q and presolar nanodiamonds (HL, P3), SiC (Ne‐E[H]), and graphite (Ne‐E[L]). The second most altered sample (11i) had a ~2–3 times higher Ne‐E concentration than the other samples. The presolar SiC abundances in the samples were determined from NanoSIMS ion images and 11i had a SiC abundance twice that of the other samples. The heterogeneous distribution of SiC grains could be inherited from heterogeneous accretion or parent body alteration could have redistributed SiC grains. Closed system step etching (CSSE) was used to study noble gases in HNO3‐susceptible phases in the most and least altered samples. All Ne‐E carried by presolar SiC grains in the most altered sample was released during CSSE, while only a fraction of the Ne‐E was released from the least altered sample. This increased susceptibility to HNO3 likely represents a step toward degassing. Presolar graphite appears to have been partially degassed during aqueous alteration. Differences in the 4He/36Ar and 20Ne/36Ar ratios in gases released during CSSE could be due to gas release from presolar nanodiamonds, with more He and Ne being released in the more aqueously altered sample. Aqueous alteration changes the properties of presolar grains so that they react similar to phase Q in the laboratory, thereby altering the perceived composition of Q.  相似文献   

12.
Organic nanoglobules are microscopic spherical carbon‐rich objects present in chondritic meteorites and other astromaterials. We performed a survey of the morphology, organic functional chemistry, and isotopic composition of 184 nanoglobules in insoluble organic matter (IOM) residues from seven primitive carbonaceous chondrites. Hollow and solid nanoglobules occur in each IOM residue, as well as globules with unusual shapes and structures. Most nanoglobules have an organic functional chemistry similar to, but slightly more carboxyl‐rich than, the surrounding IOM, while a subset of nanoglobules have a distinct, highly aromatic functionality. The range of nanoglobule N isotopic compositions was similar to that of nonglobular 15N‐rich hotspots in each IOM residue, but nanoglobules account for only about one third of the total 15N‐rich hotspots in each sample. Furthermore, many nanoglobules in each residue contained no 15N enrichment above that of bulk IOM. No morphological indicators were found to robustly distinguish the highly aromatic nanoglobules from those that have a more IOM‐like functional chemistry, or to distinguish 15N‐rich nanoglobules from those that are isotopically normal. The relative abundance of aromatic nanoglobules was lower, and nanoglobule diameters were greater, in more altered meteorites, suggesting the creation/modification of IOM‐like nanoglobules during parent‐body processing. However, 15N‐rich nanoglobules, including many with highly aromatic functional chemistry, likely reflect preaccretionary isotopic fractionation in cold molecular cloud or protostellar environments. These data indicate that no single formation mechanism can explain all of the observed characteristics of nanoglobules, and their properties are likely a result of multiple processes occurring in a variety of environments.  相似文献   

13.
Abstract— Low molecular weight monocarboxylic acids, including acetic acid, are some of the most abundant organic compounds in carbonaceous chondrites. So far, the 13C‐ and D‐enriched signature of water‐extractable carboxylic acids has implied an interstellar contribution to their origin. However, it also has been proposed that monocarboxylic acids could be formed by aqueous reaction on the meteorite parent body. In this study, we conducted hydrous pyrolysis of macromolecular organic matter purified from the Murchison meteorite (CM2) to examine the generation of monocarboxylic acids with their stable carbon isotope measurement. During hydrous pyrolysis of macromolecular organic matter at 270–330 °C, monocarboxylic acids with carbon numbers ranging from 2 (C2) to 5 (C5) were detected, acetic acid (CH3COOH; C2) being the most abundant. The concentration of the generated acetic acid increased with increasing reaction temperature; up to 0.48 mmol acetic acid/g macromolecular organic matter at 330 °C. This result indicates that the Murchison macromolecule has a potential to generate at least ?0.4 mg acetic acid/g meteorite, which is about four times higher than the amount of water‐extractable acetic acid reported from Murchison. The carbon isotopic composition of acetic acid generated by hydrous pyrolysis of macromolecular organic matter is ?‐27‰ (versus PDB), which is much more depleted in 13C than the water‐extractable acetic acid reported from Murchison. Intramolecular carbon isotope distribution shows that methyl (CH3‐)‐C is more enriched in 13C relative to carboxyl (‐COOH)‐C, indicating a kinetic process for this formation. Although the experimental condition of this study (i.e., 270–330 °C for 72 h) may not simulate a reaction condition on parent bodies of carbonaceous chondrite, it may be possible to generate monocarboxylic acids at lower temperatures for a longer period of time.  相似文献   

14.
Raman spectroscopy was used to investigate insoluble organic matter (IOM) from a range of chondritic meteorites, and a suite of interplanetary dust particles (IDPs). Three monochromatic excitation wavelengths (473 nm, 514 nm, 632 nm) were applied sequentially to assess variations in meteorite and IDP Raman peak parameters (carbon D and G bands) as a function of excitation wavelength (i.e., dispersion). Greatest dispersion occurs in CVs > OCs > CMs > CRs with type 3 chondrites compared at different excitation wavelengths displaying conformable relationships, in contrast to type 2 chondrites. These findings indicate homogeneity in the structural nature of type 3 chondrite IOM, while organic matter (OM) in type 2 chondrites appears to be inherently more heterogeneous. If type 2 and type 3 chondrite IOM shares a common source, then thermal metamorphism may have a homogenizing effect on the originally more heterogeneous OM. IDP Raman G bands fall on an extension of the trend displayed by chondrite IOM, with all IDPs having Raman parameters indicative of very disordered carbon, with almost no overlap with IOM. The dispersion effect displayed by IDPs is most similar to CMs for the G band, but intermediate between CMs and CRs for the D band. The existence of some overlapping Raman features in the IDPs and IOM indicates that their OM may share a common origin, but the IDPs preserve more pristine OM that may have been further disordered by ion irradiation. H, C, and N isotopic data for the IDPs reveal that the disordered carbon in IDPs corresponds with higher δ15N and lower δ13C.  相似文献   

15.
Abstract— We have analyzed the chemically and isotopically well‐characterized insoluble organic matter (IOM) extracted from 51 unequilibrated chondrites (8 CR, 9 CM, 1 CI, 3 ungrouped C, 9 CO, 9 CV, 10 ordinary, 1 CB and 1 E chondrites) using confocal imaging Raman spectroscopy. The average Raman properties of the IOM, as parameterized by the peak characteristics of the so‐called D and G bands, which originate from aromatic C rings, show systematic trends that are correlated with meteorite (sub‐) classification and IOM chemical compositions. Processes that affect the Raman and chemical properties of the IOM, such as thermal metamorphism experienced on the parent bodies, terrestrial weathering and amorphization due to irradiation in space, have been identified. We established separate sequences of metamorphism for ordinary, CO, oxidized, and reduced CV chondrites. Several spectra from the most primitive chondrites reveal the presence of organic matter that has been amorphized. This amorphization, usually the result of sputtering processes or UV or particle irradiation, could have occurred during the formation of the organic material in interstellar or protoplanetary ices or, less likely, on the surface of the parent bodies or during the transport of the meteorites to Earth. D band widths and peak metamorphic temperatures are strongly correlated, allowing for a straightforward estimation of these temperatures.  相似文献   

16.
Compound‐specific carbon isotope analysis (δ13C) of meteoritic organic compounds can be used to elucidate the abiotic chemical reactions involved in their synthesis. The soluble organic content of the Murchison carbonaceous chondrite has been extensively investigated over the years, with a focus on the origins of amino acids and the potential role of Strecker‐cyanohydrin synthesis in the early solar system. Previous δ13C investigations have targeted α‐amino acid and α‐hydroxy acid Strecker products and reactant HCN; however, δ13C values for meteoritic aldehydes and ketones (Strecker precursors) have not yet been reported. As such, the distribution of aldehydes and ketones in the cosmos and their role in prebiotic reactions have not been fully investigated. Here, we have applied an optimized O‐(2,3,4,5,6‐pentafluorobenzyl)hydroxylamine (PFBHA) derivatization procedure to the extraction, identification, and δ13C analysis of carbonyl compounds in the Murchison meteorite. A suite of aldehydes and ketones, dominated by acetaldehyde, propionaldehyde, and acetone, were detected in the sample. δ13C values, ranging from ?10.0‰ to +66.4‰, were more 13C‐depleted than would be expected for aldehydes and ketones derived from the interstellar medium, based on interstellar 12C/13C ratios. These relatively 13C‐depleted values suggest that chemical processes taking place in asteroid parent bodies (e.g., oxidation of the IOM) may provide a secondary source of aldehydes and ketones in the solar system. Comparisons between δ13C compositions of meteoritic aldehydes and ketones and other organic compound classes were used to evaluate potential structural relationships and associated reactions, including Strecker synthesis and alteration‐driven chemical pathways.  相似文献   

17.
Abstract— Kainsaz CO3 insoluble organic matter (IOM) was studied using Curie point pyrolysis, electronic paramagnetic resonance (EPR), and high‐resolution transmission electron microscopy (HRTEM) to determine the effect of thermal metamorphism on molecular chondritic fingerprints. Pyrolysis released a very low amount of products that consist of one‐ and two‐ring aromatic units with methyl, dimethyl, and ethyl substituents. Moreover, Kainsaz IOM contains two orders of magnitude fewer radicals than Orgueil, Murchison, and Tagish Lake IOM. In addition, no diradicaloids were found in Kainsaz, although they are thought to constitute a specific signature for weakly organized extraterrestrial organic compounds in contrast to terrestrial ones. HRTEM reveals a very heterogeneous structure, with microporous disordered carbon, mesoporous graphitic carbons and graphite. Graphitization likely occurs and explains the differences between Kainsaz and CI or CM IOM. Heating stress experienced by Kainsaz IOM, on the parent body and/or prior its accretion, is likely responsible for the differences in molecular and structural organizations compared with those of CI and CM IOM.  相似文献   

18.
Here, we present the results of a multitechnique study of the bulk properties of insoluble organic material (IOM) from the Tagish Lake meteorite, including four lithologies that have undergone different degrees of aqueous alteration. The IOM C contents of all four lithologies are very uniform and comprise about half the bulk C and N contents of the lithologies. However, the bulk IOM elemental and isotopic compositions vary significantly. In particular, there is a correlated decrease in bulk IOM H/C ratios and δD values with increasing degree of alteration—the IOM in the least altered lithology is intermediate between CM and CR IOM, while that in the more altered lithologies resembles the very aromatic IOM in mildly metamorphosed CV and CO chondrites, and heated CMs. Nuclear magnetic resonance (NMR) spectroscopy, C X‐ray absorption near‐edge (XANES), and Fourier transform infrared (FTIR) spectroscopy confirm and quantitate this transformation from CR‐like, relatively aliphatic IOM functional group chemistry to a highly aromatic one. The transformation is almost certainly thermally driven, and probably occurred under hydrothermal conditions. The lack of a paramagnetic shift in 13C NMR spectra and 1s‐σ* exciton in the C‐XANES spectra, both typically seen in metamorphosed chondrites, shows that the temperatures were lower and/or the timescales were shorter than experienced by even the least metamorphosed type 3 chondrites. Two endmember models were considered to quantitatively account for the changes in IOM functional group chemistry, but the one in which the transformations involved quantitative conversion of aliphatic material to aromatic material was the more successful. It seems likely that similar processes were involved in producing the diversity of IOM compositions and functional group chemistries among CR, CM, and CI chondrites. If correct, CRs experienced the lowest temperatures, while CM and CI chondrites experienced similar more elevated temperatures. This ordering is inconsistent with alteration temperatures based on mineralogy and O isotopes.  相似文献   

19.
Based on the statistical model proposed for the molecular structure of the insoluble organic matter (IOM) isolated from the Murchison meteorite, it was recently proposed that, in the solar T‐Tauri disk regions where (photo)dissociation of gaseous molecules takes place, aromatics result from the cyclization/aromatization of short aliphatics. This hypothesis is tested in this study, with n‐alkanes being submitted to high‐frequency discharge at low pressure. The contamination issue was eliminated using deuterated precursor. IOM was formed and studied using solid‐state nuclear magnetic resonance, pyrolysis coupled to gas chromatography and mass spectrometry, RuO4 oxidation, and high‐resolution transmission electron microscopy. It exhibits numerous similarities at the molecular level with the hydrocarbon backbone of the natural IOM, reinforcing the idea that the initial precursors of the IOM were originally chains in the gas. Moreover, a fine comparison between the chemical structure of several meteorite IOM suggests either that (i) the meteorite IOMs share a common precursor standing for the synthetic IOM or that (ii) the slight differences between the meteorite IOMs reflect differences in their environment at the time of their formation i.e., related to plasma temperature that, in turn, dictates the dissociation–recombination rates of organic fragments.  相似文献   

20.
Abstract— Hydrogen isotope ratios of organic compounds in carbonaceous chondrites provide critical information about their origins and evolutionary history. However, because many of these compounds are obtained by aqueous extraction, the degree of hydrogen‐deuterium (H/D) exchange that occurs during the process needs to be quantitatively evaluated. This study uses compound‐specific hydrogen isotopic analysis to quantify the H/D exchange during aqueous extraction. Three common meteoritic dicarboxylic acids (succinic, glutaric, and 2‐methyl glutaric acids) were refluxed under conditions simulating the extraction process. Changes in δD values of the dicarboxylic acids were measured following the reflux experiments. A pseudo‐first order rate law was used to model the H/D exchange rates which were then used to calculate the isotope exchange resulting from aqueous extraction. The degree of H/D exchange varies as a result of differences in molecular structure, the alkalinity of the extraction solution and presence/absence of meteorite powder. However, our model indicates that succinic, glutaric, and 2‐methyl glutaric acids with a δD of 1800%***o would experience isotope changes of 38o, 10o, and 6o, respectively during the extraction process. Therefore, the overall change in δD values of the dicarboxylic acids during the aqueous extraction process is negligible. We also demonstrate that H/D exchange occurs on the chiral α‐carbon in 2‐methyl glutaric acid. The results suggest that the racemic mixture of 2‐methyl glutaric acid in the Tagish Lake meteorite could result from post‐synthesis aqueous alteration. The approach employed in this study can also be used to quantify H/D exchange for other important meteoritic compounds such as amino acids.  相似文献   

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