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1.
Monocarboxylic acids (MCAs) are important astrobiologically because they are often the most abundant soluble compounds in carbonaceous chondrites (CCs) and are potential synthetic end products for many biologically important compounds. However, there has been no systematic study on the effect of parent body alteration on molecular and isotopic variability of MCAs. Since MCAs in meteorites are dominated by low molecular weight (C1-C8), highly volatile compounds, their distributions are likely to be particularly sensitive to secondary alteration processes. In contrast, the aliphatic side chains of insoluble organic matter (IOM) in CCs, whose composition has been shown to be closely related to the MCAs, may be far more resistant to secondary alteration. In the present study, we determined the distributions and isotopic ratios of free and IOM-derived MCAs in six carbonaceous chondrites with a range of classifications: Murchison (CM2), EET 87770 (CR2), ALH 83034 (CM1), ALH 83033 (CM2), MET 00430 (CV3) and WIS 91600 (C2). We compare mineralogical and petrological characteristics to the MCAs distributions to better define the processes leading to the synthesis and alteration of meteoritic MCAs. Our results show that aqueous and especially thermal alteration in the parent bodies led to major loss of free MCAs and depletion of straight relative to branched chain compounds. However, the MCAs derived from aliphatic side chains of IOM are well preserved despite of secondary alterations. The molecular and isotopic similarities of IOM-derived MCAs in different chondrite samples indicate very similar synthetic histories for organic matter in different meteorites.  相似文献   

2.
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   

3.
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   

4.
α-Amino acids and α-hydroxy acids are well known constituents of several carbonaceous meteorites. One proposed mechanism of their formation is the reactions of CN−, NH3, aldehydes and ketones in aqueous solution, a Strecker-like synthesis. Iminodicarboxylic acids, relatively unusual in molecular structure, are significant by-products of laboratory Strecker syntheses of α-amino acids. It is therefore notable that an analogous suite of imino acids has not been reported in CM2 chondrites where amino and hydroxy acids are abundant. In this work, aqueous extracts of the Murchison meteorite were examined for the presence of imino acids; GC-MS and HPLC molecular analyses revealed a complex suite of such acids. With the exception of one of the seven-carbon members, all of the C4 through C7 imino acids were observed in Murchison. These observations suggest that the Strecker synthesis made, at least, some contribution to the formation of extraterrestrial amino acids.  相似文献   

5.
Deuterium-enriched amino acids occur in the Murchison carbonaceous chondrite. Synthesis from D-enriched interstellar precursors by Strecker reactions during aqueous alteration of the parent body has been proposed. To test this hypothesis, we have measured the retention of deuterium in amino acids produced from HCN, NH3, and formaldehyde-D2, acetaldehyde-D4, and acetone-D6 in H2O. The isotopic label is 50% to 98% retained, with variations in retentivity depending on the amino acid and the reaction conditions. If amino acids, once formed on the parent body by the Strecker synthesis, lose no deuterium by subsequent exchange with water or H-bearing minerals, then the observed deuterium isotopic composition of Murchison amino acids represents as much as 50% or more of the enrichments inherited from their interstellar precursors. Imino diacids are prominent side products of the Strecker synthesis which have not been reported in carbonaceous chondrites. Under the conditions of the Strecker reaction using deuterium labeled aldehydes and ketones, unlabeled amino acids are also formed by an HCN polymerization route indicating multiple pathways for the synthesis of amino acids in meteorites.  相似文献   

6.
地外有机化合物   总被引：1，自引：0，他引：1  
球粒陨石中的有机化合物起源于星际介质,是构成太阳星云的初始组分,并与其他物质一起吸积形成小行星和行星。在小行星内,有机质经历了不同程度的水蚀变和热变质作用。球粒陨石中的有机化合物尽管是非生命成因,但组成极为复杂,主要是类似于干酪根的大分子物质,以及少量可溶性有机物。大部分可溶有机分子也发现于地球生物圈,但前者可具有完全不同的H、C、N等同位素组成,这也是它们来源于地球之外的重要证据。星云中宇宙线和紫外线（UV）的辐射、小行星的热变质和水蚀变,是地外有机质演化的主要过程。球粒陨石中的有机质是地球生命起源的物质基础,是生命起源不可或缺的重要环节。同样重要的是,大量的火星探测表明,火星历史上有过满足生命存在的基本条件,而在火星陨石中还发现了一些生物活动相关的线索。未来很可能首先在火星上发现地外生命存在的证据。  相似文献   

7.
The δ13C values of thirty-four individual amino acids and two pyridine carboxylic acids have been obtained fromthe Murchison meteorite. They were found to range from +4.9 to +52.8‰, with statistically significant differences observed both within and between amino acid subgroups. The 13C content of α-amino acids declines with increasing chain length, a trend similar to the ones previously observed for carboxylic acids and alkanes. Also 2-methyl-2-amino acids were found to be heavier in 13C than the corresponding 2-H homologues. The3-, 4-, and 5-amino acids do not show a comparable declining trend in δ13C values and neither do the amino dicarboxylic acids. This variability in δ 13C values can be interpreted as to indicate that the synthetic histories of soluble organics in meteorites may have been diverse even within groups of compounds with very similar functional group composition.  相似文献   

8.
The hydroxy acid suites extracted from the Murchison (MN), GRA 95229 (GRA) and LAP 02342 (LAP) meteorites have been investigated for their molecular, chiral and isotopic composition. Substantial amounts of the compounds have been detected in all three meteorites, with a total abundance that is lower than that of the amino acids in the same stones. Overall, their molecular distributions mirror closely that of the corresponding amino acids and most evidently so for the LAP meteorite. A surprising l-lactic acid enantiomeric excess was found present in all three stones, which cannot be easily accounted by terrestrial contamination; all other compounds of the three hydroxy acid suites were found racemic. The branched-chain five carbon and the diastereomer six-carbon hydroxy acids were also studied vis-a-vis the corresponding amino acids and calculated ab initio thermodynamic data, with the comparison allowing the suggestion that meteoritic hydroxyacid at these chain lengths formed under thermodynamic control and, possibly, at a later stage than the corresponding amino acids. 13C and D isotopic enrichments were detected for many of the meteoritic hydroxy acids and found to vary between molecular species with trends that also appear to correlate to those of amino acids; the highest δD value (+3450‰) was displayed by GRA 2-OH-2-methylbutyric acid. The data suggest that, while the amino- and hydroxy acids likely relate to common presolar precursor, their final distribution in meteorites was determined to large extent by the overall composition of the environments that saw their formation, with ammonia being the determining factor in their final abundance ratios.  相似文献   

9.
Deuterium-enriched amino acids occur in the Murchison carbonaceous chrondrite. This meteorite underwent a period of aqueous alteration with isotopically light water. With the objective of setting limits on the conditions of aqueous alteration, the exchange of the carbon-bonded hydrogen atoms of amino acids with D2O has been studied from 295 to 380 K as a function of time and meteorite/heavy water ratio. The amount of Murchison or Allende dust present has a significant effect on the rate and amount of hydrogen-deuterium exchange observed. At elevated temperatures, the alpha-hydrogens of all the amino acids studied were found to exchange with deuterium. In glycine and aspartic acid, this process resulted in total exchange of the carbon-bonded hydrogen. A completely deuterated isotopomer of alanine was produced in significant quantities only when the rock/water ratio was greater than 0.5. No exchange of carbon-bonded hydrogens was observed in the case of amino acids which do not possess an alpha-hydrogen atom. The rates of H/D exchange for amino acids observed here did not correspond to deuterium enrichment of the amino acids in the Murchison meteorite. These results suggest that H/D exchange with water had a negligible effect on the observed deuterium enrichment of amino acids found in Murchison and that the temperature at which the amino acids were exposed to liquid water was close to 273 K.  相似文献   

10.
The hydroxymonocarboxylic acids, dicarboxylic acids, and hydroxydicarboxylic acids of the Murchison meteorite were analyzed as their tert-butyldimethylsilyl derivatives using combined gas chromatography-mass spectrometry. The hydroxydicarboxylic acids have not been found previously in meteorites. Each class of compounds is numerous with carbon chains up to C8 or C9 and many, if not all, chain and substitution position isomers represented at each carbon number. The alpha-hydroxycarboxylic acids and alpha-hydroxydicarboxylic acids correspond structurally to many of the known meteoritic alpha-aminocarboxylic acids and alpha-aminodicarboxylic acids, a fact that supports the proposal that a Strecker synthesis was involved in the formation of both classes of compounds. Isotopic analyses show these acids to be D-rich relative to terrestrial organic compounds as expected; however, the hydroxy acids appear to be isotopically lighter than the amino acids with respect to both carbon and hydrogen. The latter finding would not be expected if both classes of compounds came exclusively from common precursors as would have been the case for a Strecker synthesis.  相似文献   

11.
Mineralogical, chemical, textural, and isotopic studies of the abundant carbonaceous inclusions in the Jodzie howardite are consistent with CM characteristics. These CM xenoliths show regolith alteration on a level comparable to the Murray and Murchison meteorites but less than Nogoya, flow-oriented development of phyllosilicates and ‘poorly characterized phases’, and partial oxidation of sulfides. Temperature-programmed pyrolysis mass spectrometry (25°–1400°C) indicates that gas release patterns of volatiles and hydrocarbon components and percent contents of N(0.15), C(2.3) and S(2.4) are typical of CM meteorites. Release of significant amounts of SO2 is attributed to the thermal breakdown of ‘poorly characterized phases’ (Fe-Ni-C-S-O) that formed during low temperature aqueous alteration in the CM parent body.Noble gas abundances are well within the reported range of CM meteorites. The fact that the Ne composition is typical for ‘solar’ values and the isotopic structure of Xe is ‘planetary’ argues that these gases were entrapped by different mechanisms. Cosmic ray exposure ages for the xenoliths (3He, 5 × 106; 21Ne, 6.7 × 106; 38Ar, 6.9 × 106 yr) agree with the reported exposure age for the eucritic host. Volatile abundances, presence of intact organic molecules, and phyllosilicates in the CM xenoliths preclude regolith temperatures in excess of 200°C after CM incorporation. Mixing of the host and xenoliths probably occurred during a low-velocity collision of main belt asteroids.  相似文献   

12.
Analyses of fractionated aqueous extracts of the Murchison meteorite by gas chromatography-mass spectrometry after silylation with N-methyl-N (tert-butyldimethylsilyl) trifluoroacetamide have revealed an extensive series of linear and cyclic aliphatic amides. These include monocarboxylic acid amides, dicarboxylic acid monoamides, hydroxy acid amides, lactams, carboxy lactams, lactims, N-acetyl amino acids, and substituted hydantoins. Numerous isomers and homologues through at least C8 were observed in all cases, except for the N-acetyl amino acids and hydantoins. Carboxy lactams, lactams, hydantoins, and N-acetyl amino acids are converted to amino acids by acid hydrolysis, thus, these compounds qualitatively account for the earlier observation of acid-labile amino acid precursors in meteoritic extracts. Laboratory studies of the spontaneous decomposition of N-carbamyl-alpha-amino acids and their dehydration products, the 5-substituted hydantoins, have led to the recognition of a series of aqueous phase reactions by which amino acids and cyanic acid/cyanate ion in the primitive parent body might have given rise to several of the observed classes of amides, as well as to monocarboxylic acids, dicarboxylic acids, and hydroxy acids. A previously undescribed reaction of 5-substituted hydantoins with cyanic acid/cyanate ion to give carboxamides of the 5-substituent groups was observed in the course of these studies. The presence of an extensive suite of amides in a CM chondrite appears to be consistent with the interstellar-parent body formation hypothesis for the organic compounds of these meteorites. The presence of carboxy lactams and lactams along with free amino acids suggests the possibility of further chemical evolution of meteorite amino acids by thermal polymerization. The cyclic amides, given their potential for hydrogen-bonded pair formation, might be considered candidate bases for a primitive sequence coding system.  相似文献   

13.
The enantiomeric excesses determined for eight amino acids and one hydroxy acid of carbonaceous chondrite meteorites represent to date the only case of molecular asymmetry measured outside the biosphere. Because of the chiral homogeneity of life’s structures and functions, the findings have been debated for the possible relevance that a-biotic chiral symmetry-breaking might have had in the origin of terrestrial homochirality. While the many unknowns surrounding the origin of life have inevitably hindered the inquiries raised in this discourse, the hypotheses put forward in regard to the origin of extraterrestrial chiral asymmetry, which is a defined physico-chemical phenomenon, have been approached analytically and their scrutiny has aided the understanding of pre-biotic chemical evolution. We report here on our current knowledge of the asymmetric effects that could have influenced the chiral symmetry breaking of molecules in cosmochemical environments and how they correlate with the data obtained from meteorite analyses. We also address recent proposals that aqueous processes might have influenced the chirality of amino acids in meteorites and show that the crystallization behavior of isovaline, the most abundant non-racemic amino acid in the Murchison meteorite, excludes its attainment of enantiomeric excesses via phase changes such as crystallization or sublimation.  相似文献   

14.
To better understand the role of aqueous alteration on the CI1 parent body, we have analyzed the texture, composition and mineral associations of iron nickel sulfides in four of the five known CI1 chondrites.The most commonly-occurring sulfide present in the CI1 chondrites is the iron-deficient Fe,Ni sulfide pyrrhotite ([Fe,Ni]1−xS), that has a composition close to that of stoichiometric troilite (FeS). Three of the CI1s (Alais, Ivuna and Tonk) also contain pentlandite ([Fe,Ni]9S8), although pentlandite is a rare phase in Ivuna. Cubanite (CuFe2S3) was found in both Alais and Ivuna in this study, although it has also been reported in Orgueil (MacDougall and Kerridge, 1977). The pyrrhotite grains in all four chondrites form hexagonal, rectangular or irregular shapes, and show no evidence of Ni or Co zoning. The pyrrhotite grains in Orgueil and Ivuna are, in general, smaller, and show more “corrosions,” or “embayments,” than those in Alais or Tonk.We suggest that the precursor sulfide present in the CI1 chondrites was troilite which, during brecciation and oxidation on the parent body at a temperature of 100°C or less, converted the troilite to magnetite and pyrrhotite with pentlandite inclusions. Subsequently, continued alteration on the parent body removed pentlandite—partially from Alais, Tonk and Ivuna, completely from Orgueil—leaving behind pyrrhotite with spaces (“corrosions”) where the pentlandite had been. Ni derived from the pentlandite was incorporated into ferrihydrite, onto the surface of which the Ni,Na sulfate Ni-bloedite formed.Based on the size and abundant “corrosions” within pyrrhotite grains, combined with observations from other authors, we conclude that Orgueil and Ivuna have undergone a greater degree of alteration than Alais and Tonk. Further work is needed to assess the conditions under which pentlandite would be dissolved preferentially to pyrrhotite, as the study of terrestrial literature indicates that the latter mineral is preferentially removed.  相似文献   

15.
Petrographic observations and analyses of CM matrices are consistent with their origin as in situ low temperature (<400°K) aqueous alteration products in a parent body regolith. At least four different phyllosilicates were tentatively characterized in Murray and Murchison meteorites, in addition to Fe- and Mg-serpentines in Nogoya. In comparison with bulk meteorite compositions, all phyllosilicates and bulk matrices show enrichment of K relative to Na. Possible loss of Na and possibly some Cl, with addition of H2O and CO2 and water-soluble organic compounds during alteration, indicates a partially open system during alteration. Poorly characterized phases (PCP) are fine-grained (< 1 μm) admixtures of variable proportions of phyllosilicates, carbonaceous matter and opaque oxides of sulfur with high Fe, Ni and Cr contents. Calcite and some magnetite show paragenetic overlap with PCP and phyllosilicates. Carbonaceous matter is largely associated with PCP in altered CM matrices. In the unaltered CV Allende, carbonaceous matter is concentrated on olivine surfaces as a micromounded coating, particularly in the dark haloes that surround some chondrules and aggregates. Precursive alteration material may have been analogous to similarly coated olivine mixed with smaller amounts of metal and sulfides.Synthesis of the water soluble organic compounds found in CM matrices may have occurred prior to or in the same environment as did aqueous alteration of the precursive phases. Preservation or partial preservation of this organic matter may reflect the degree of overlap in episodes of synthesis and alteration.Nogoya is 95% altered and has a bulk carbon content of 5.2 wt%, which is higher than any meteorite. In addition, it has the lowest measured 13C12C ratio of any other carbonaceous chondrite, except for Karoonda.  相似文献   

16.
Using microprobe laser-desorption, laser-ionization mass spectrometry (μL2MS), we measured the distributions of alkylated and unalkylated polycyclic aromatic hydrocarbons (PAHs) in the free organic material of 20 carbonaceous chondrites. These meteorites represent a variety of meteorite classes and alteration histories, including CI, CK, CM, CO, CR, CV, and Tagish Lake. This work provides information on free organic compounds that is complementary to studies of the structure and composition of meteoritic macromolecular content.For the nine CM2 meteorites analyzed, we observe that higher relative abundances of alkylated PAHs correlate with more intense aqueous activity. We attribute this correlation to the differences in solubility and volatility between unalkylated and alkylated PAHs. Naphthalene and its alkylation series are more susceptible to the effects of aqueous exposure than the less-soluble PAH phenanthrene and its alkylated derivatives. These observations are consistent with the possibility of chromatographic separations on the meteorite parent bodies. We identify six CM2 meteorites with similar PAH distributions that may represent the original, unaltered organic composition of the parent body.Increased metamorphic intensity reduces the abundance of all PAHs. The thermally metamorphosed CK chondrites had no detectable levels of typical meteoritic PAHs. This observation might be explained either by a loss of PAHs caused by volatilization or by a significantly different organic content of the CK parent body.  相似文献   

17.
All ten of the possible five-carbon acyclic primary β-, γ-, and δ-amino alkanoic acids (amino position isomers of the valines) have been positively identified in hot-water extracts of the Murchison meteorite using combined gas chromatography-mass spectrometry (GC-MS) and ion exchange chromatography. With the exception of δ-aminovaleric acid, none of these amino acids has been previously reported to occur in meteorites or in any other natural material. The γ-amino acids (4-aminopentanoic acid, 4-aminc-2-meth-ylbutanoic acid, and 4-amino-3-methylbutanoic acid) are present at higher concentrations (about 5 nmol g?1) than are the β-amino isomers (3-aminopentanoic acid, 3-amino-2-methylbutanoic acid, allo-3-amino-2-methylbutanoic acid, 3-amino-3-methylbutanoic acid, 3-amino-2-ethylpropanoic acid, and 3-amino-2,2-dimethylpropanoic acid) which are present at concentrations of 1–2 nmol g?1. These amino acids are less abundant in the meteorite than either the corresponding α-amino acids or the four-carbon homologues. Thirty-six amino acids have now been positively identified in the Murchison meteorite, 17 of which are apparently unique to carbonaceous chondrites. The fact that the meteorite contains all possible five-carbon acyclic primary α-, β-, γ-, and δ-amino alkanoic acids is consistent with a synthetic process involving random combination of single-carbon precursors.  相似文献   

18.
Amino acids, amines and aldehydes were obtained from the water extracts of two CR2 carbonaceous chondrites from Antarctica and analyzed for their molecular and 15N isotopic content. These compounds were found to differ significantly from those of CM chondrites in both overall abundances and molecular distribution. The amino acids suites comprise a preponderant abundance of linear, 2-H amino acids, show rapid non-linear decrease with the compounds’ increasing chain length and include protein amino acids never identified in meteorites before, such as threonine, tyrosine and phenylalanine. The presence of tertiary amines as well as a diverse, large abundance of aldehydes and ketones also distinguishes both CR2 organic suites. The δ15N values determined for CR2 amino acids have a distribution between molecular subgroups that is opposite to the one of their δD values, with 2-H amino acids having higher δ15N and lower δD values than 2-methyl amino acids, while the opposite is true for 2-methyl amino acids. Based on theoretical data, these isotopic findings would place the formation of the two amino acid groups or their direct precursors at different ISM stages of star formation.  相似文献   

19.
Aqueous alteration of primitive meteorites was among the earliest geological processes during the evolution of our solar system. ‘Clumped-isotope’ thermometry of carbonates in the CM chondrites, Cold Bokkeveld, Murray, and Murchison, demonstrates that they underwent aqueous alteration at 20-71 °C from a fluid with δ18OVSMOW of 2.0‰ to 8.1‰ and δ17OVSMOW of −0.1‰ to 3.0‰. The δ13CVPDB values of these carbonates exhibit a negative correlation with the δ18OVSMOW of their formation waters, consistent with formation and escape of 13C-depleted CH4 during aqueous alteration. Methane generation under these conditions implies that the alteration fluid was characterized by an Eh ? −0.67 and pH ? 12.5 (or lower at the highest alteration temperatures). Our findings suggest that methane generation may have been a widespread consequence of planetesimal and planetary aqueous alteration, perhaps explaining the occurrence of methane on Titan, Triton, Pluto, and other Kuiper-belt objects.  相似文献   

20.
The enantiomeric and carbon-isotopic composition of the amino acid isovaline have been analyzed in several samples of the Murchison meteorite and one sample of the Murray meteorite. l-Enantiomeric excesses of the amino acid were found to range from 0 to 15.2%, varying significantly both between meteorite stones and at short distances within a single stone. The upper limit of this range is the largest enantiomeric excess measured to date for a biologically rare meteoritic amino acid and raises doubts that circularly polarized light irradiation could have been the sole cause of amino acids chiral asymmetry in meteorites. Individual d- and l-isovaline δ13C values ware found to be about +18‰, with no significant differences between the two enantiomers to suggest terrestrial contamination. The amino acid relative abundance also varied between samples, with isovaline/alanine ratios of 0.5 to 6.5. X-ray diffraction analyses of contiguous meteorite fragments suggest a possible correlation between isovaline and hydrous silicates abundances.  相似文献   

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