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1.
Abstract— We have analyzed an important fraction of the free carboxylic acids present in water extracts of the CM2 chondrite Murchison and the CI1 chondrite Orgueil using gas chromatographymass spectrometry (GC‐MS). The free nature of the carboxylic acids analyzed was ensured by employing a single‐step water extraction. Analyses revealed the presence of a structurally diverse suite of both aliphatic and aromatic acids in Murchison, while Orgueil exhibits a simpler distribution of exclusively aromatic acids. Within the Murchison aromatic acids, there are previously unreported phthalic acids, methyl phthalic acids, and hydroxybenzoic acids. In Orgueil, benzoic acid and very small amounts of methylbenzoic acids and methylhydroxybenzoic acids were detected. For the aromatic acids in both Murchison and Orgueil, most structural isomers were identified, suggesting an origin by abiotic processes. Quantitative differences are evident between acids in the two meteorites; carboxylic acids are much more abundant in Murchison than in Orgueil. The data suggest that differing levels of aqueous alteration on the meteorite parent body(ies) has produced dissimilar distributions of carboxylic acids.  相似文献   

2.
Aromatic compounds have been considered a likely candidate for enhanced aerosol formation in the polar region of Jupiter. We develop a new chemical model for aromatic compounds in the Jovian auroral thermosphere/ionosphere. The model is based on a previous model for hydrocarbon chemistry in the Jovian atmosphere and is constrained by observations from Voyager, Galileo, and the Infrared Space Observatory. Precipitation of energetic electrons provides the major energy source for the production of benzene and other heavier aromatic hydrocarbons. The maximum mixing ratio of benzene in the polar model is 2x10-9, a value that can be compared with the observed value of 2+2-1x10-9 in the north polar auroral region. Sufficient quantities of the higher ring species are produced so that their saturated vapor pressures are exceeded. Condensation of these molecules is expected to lead to aerosol formation.  相似文献   

3.
Haze particles exert a significant influence over the thermodynamics and radiation absorption properties of the Titan haze, as well as its complex organic chemistry. Characterization of both the molecular and the submicrometer components of the haze is therefore vital for understanding the global properties of Titan. We have carried out a Titan tholin synthesis experiment and measured the time variation of the infrared spectrum of the product as a thin film developed. Also, to examine the possibility of oxygen contamination, we compared the infrared spectrum of the tholin film with that of a tholin film exposed to dry air and laboratory air. The objective of this study is to understand the chemical processes related to how simple organic molecules are processed into more complex haze particles. The progressive development of features characteristic of amines, aromatic and aliphatic hydrocarbons, and nitriles in the experimental mixture is clear. Of particular interest is the formation of aromatic rings after only a few seconds of glow discharge, indicating that these compounds appear to be intermediates between simple haze molecules and microphysical aerosols. The early dominance of aromatic ring structures is accompanied during the later stages of the experiment by the appearance of nitrile and amine compounds. This time-dependent succession of chemical structures provides vital clues to the possible chemical formation pathways of Titan haze aerosols.  相似文献   

4.
Titan, the largest satellite of Saturn, has a thick nitrogen/methane atmosphere with a thick global organic haze. A laboratory analogue of Titan's haze, called tholin, was formed in an inductively coupled plasma from nitrogen/methane=90/10 gas mixture at various pressures ranging from 13 to 2300 Pa. Chemical and optical properties of the resulting tholin depend on the deposition pressure in cold plasma. Structural analyses by IR and UV/VIS spectroscopy, microprobe laser desorption/ionization mass spectrometry, and Raman spectroscopy suggest that larger amounts of aromatic ring structures with larger cluster size are formed at lower pressures (13 and 26 Pa) than at higher pressures (160 and 2300 Pa). Nitrogen is more likely to incorporate into carbon networks in tholins formed at lower pressures, while nitrogen is bonded as terminal groups at higher pressures. Elemental analysis reveals that the carbon/nitrogen ratio in tholins increases from 1.5-2 at lower pressures to 3 at 2300 Pa. The increase in the aromatic compounds and the decrease in C/N ratio in tholin formed at low pressures indicate the presence of the nitrogen-containing polycyclic aromatic compounds in tholin formed at low pressures. Tholin formed at high pressure (2300 Pa) consists of a polymer-like branched chain structure terminated with CH3, NH2, and CN with few aromatic compounds. Reddish-brown tholin films formed at low pressures (13-26 Pa) shows stronger absorptions (almost 10 times larger k-value) in the UV/VIS range than the yellowish tholin films formed at high pressures (160 and 2300 Pa). The tholins formed at low pressures may be better representations of Titan's haze than those formed at high pressures, because the optical properties of tholin formed at low pressures agree well with that of Khare et al. (1984a, Icarus 60, 127-137), which have been shown to account for Titan's observed geometric albedo. Thus, the nitrogen-containing polycyclic aromatic compounds we find in tholin formed at low pressure may be present in Titan's haze. These aromatic compounds may have a significant influence on the thermal structure and complex organic chemistry in Titan's atmosphere, because they are efficient absorbers of UV radiation and efficient charge exchange intermediaries. Our results also indicate that the haze layers at various altitudes might have different chemical and optical properties.  相似文献   

5.
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   

6.
Abstract— The polycyclic aromatic hydrocarbon (PAH) naphthalene was exposed to ultraviolet radiation in H2O ice under astrophysical conditions, and the products were analyzed using infrared spectroscopy and high‐performance liquid chromatography. As we found in our earlier studies on the photoprocessing of coronene in H2O ice, aromatic alcohols and ketones (quinones) were formed. The regiochemistry of the reactions is described and leads to specific predictions of the relative abundances of various oxidized naphthalenes that should exist in meteorites if interstellar ice photochemistry influenced their aromatic inventory. Since oxidized PAHs are present in carbon‐rich meteorites and interplanetary dust particles (IDPs), and ubiquitous in and fundamental to biochemistry, the delivery of such extraterrestrial molecules to the early Earth may have played a role in the origin and evolution of life.  相似文献   

7.
The morphology, molecular composition, and distribution of organic matter (OM) were investigated in a suite of CR chondrites to better constrain its hydrothermal evolution. Multiple focused ion beam sections were extracted from the matrices of seven CR chondrites. Scanning transmission X-ray microscopy and transmission electron microscopy reveal OM ubiquitously distributed across the CR matrices. OM mainly occurs as either discrete submicron rounded or irregularly shaped vein-like particles. Two spectral populations of organic particles were identified by carbon K-edge X-ray absorption near edge structure (XANES): the most abundant one, similar to insoluble organic matter (IOM) residues, contains aromatic, carbonyl, and carboxylic groups. The second population is more aromatic-rich and lacks a distinctive carbonyl peak. An additional, ubiquitous organic component occurs associated with amorphous silicates and phyllosilicates. Less aromatic but aliphatic- and carboxylic-rich, this diffuse OM is interpreted as the result of the redistribution of organic compounds by aqueous fluids. The most altered CR1 GRO 95577 contains a more mature OM and highly aliphatic- and carboxylic-rich diffuse OM. This evolution, from the CR2s to the CR1, is comparable to that of terrestrial gas shale maturation involving cracking reactions, releasing bitumen-like, aliphatic-, and carboxylic-rich compounds, and aromatic residues. Our observations support the accretion of soluble OM and its later polymerization to IOM, as well as the maturation of IOM and its partial oxidation, releasing mobile compounds. The differences in GRO 95577 are clearly attributable to the hydrothermal episode(s), but the relative role of water and temperature on the evolution of OM remains elusive.  相似文献   

8.
In this second paper on the 3.2–3.5 μm region, we report the results of a theoretical study of the possible contributions of hydrogenated compounds to the observed infrared emission. We consider small aromatic species to which hydrogens have been added directly on the polycyclic frame, in both neutral and ionized forms, to mimic typical structural situations expected for larger polycyclic aromatic hydrocarbons (PAHs). The evolution of the infrared spectra for PAHs having increasingly higher excess H coverage is investigated up to saturation. The present study shows that hydrogenated PAHs produce series of bands that may be at the origin of the broad plateau observed below the 3.4- and 3.5-μm features, together with the features themselves. Ionization produces the usual collapse of the aromatic CH intensities, but it also affects the alicyclic CH intensities, although less drastically, in contrast to the CH intensities of aliphatic substituents.  相似文献   

9.
Abstract– The successful return of the Stardust spacecraft provides a unique opportunity to investigate the nature and distribution of organic matter in cometary dust particles collected from comet 81P/Wild 2. Analysis of individual cometary impact tracks in silica aerogel using the technique of two‐step laser mass spectrometry demonstrates the presence of complex aromatic organic matter. While concerns remain as to the organic purity of the aerogel collection medium and the thermal effects associated with hypervelocity capture, the majority of the observed organic species appear indigenous to the impacting particles and are hence of cometary origin. While the aromatic fraction of the total organic matter present is believed to be small, it is notable in that it appears to be N rich. Spectral analysis in combination with instrumental detection sensitivies suggest that N is incorporated predominantly in the form of aromatic nitriles (R–C≡N). While organic species in the Stardust samples do share some similarities with those present in the matrices of carbonaceous chondrites, the closest match is found with stratospherically collected interplanetary dust particles. These findings are consistent with the notion that a fraction of interplanetary dust is of cometary origin. The presence of complex organic N containing species in comets has astrobiological implications as comets are likely to have contributed to the prebiotic chemical inventory of both the Earth and Mars.  相似文献   

10.
Material of low geometric albedo (pV?0.1) is found on many objects in the outer Solar System, but its distribution in the saturnian satellite system is of special interest because of its juxtaposition with high-albedo ice. In the absence of clear, diagnostic spectral features, the composition of this low-albedo (or “dark”) material is generally inferred to be carbon-rich, but the form(s) of the carbon is unknown. Near-infrared spectra of the low-albedo hemisphere of Saturn's satellite Iapetus were obtained with the Visible-Infrared Mapping Spectrometer (VIMS) on the Cassini spacecraft at the fly-by of that satellite of 31 December 2004, yielding a maximum spatial resolution on the satellite's surface of ∼65 km. The spectral region 3-3.6 μm reveals a broad absorption band, centered at 3.29 μm, and concentrated in a region comprising about 15% of the low-albedo surface area. This is identified as the CH stretching mode vibration in polycyclic aromatic hydrocarbon (PAH) molecules. Two weaker bands attributed to CH2 stretching modes in aliphatic hydrocarbons are found in association with the aromatic band. The bands most likely arise from aromatic and aliphatic units in complex macromolecular carbonaceous material with a kerogen- or coal-like structure, similar to that in carbonaceous meteorites. VIMS spectra of Phoebe, encountered by Cassini on 11 June 2004, also show the aromatic hydrocarbon band, although somewhat weaker than on Iapetus. The origin of the PAH molecular material on these two satellites is unknown, but PAHs are found in carbonaceous meteorites, cometary dust particles, circumstellar dust, and interstellar dust.  相似文献   

11.
Deuterium abundance measurements and the 13C NMR spectrum of the HF/HCl insoluble residue of the Orgueil carbonaceous chondrite indicate the presence of an extensive component of polycyclic aromatic hydrocarbons (PAH) that is of possible interstellar origin or is similar to PAH hypothesized to exist in interstellar space. Infrared spectra have been obtained using an FTIR spectrometer of the acid insoluble residue, the residue after heating in vacuum, and condensate. Bulk acid insoluble residue was pressed into KBr pellets and also heated under high vacuum to sublimate a volatile component onto KBr disks. The remaining non-volatile organic component of the Orgueil meteorite from such evaporations pressed into KBr pellets exhibits a spectral signature similar to that observed in emission from the Orion Nebula and found in Raman spectra of interplanetary dust particles (IDPs). In addition it has an 11.3 microns (885 cm-1) band indicating PAH having single hydrogens per peripheral aromatic ring. We conclude the nonvolatile material is similar to interstellar PAH because the observed 11.3 microns (885 cm-1) unidentified infrared (UIR) emission suggests interstellar PAH have single hydrogens per peripheral aromatic ring. The volatile fraction of the Orgueil shows an aliphatic CH stretch feature and its spectrum in the 2-25 microns range is similar to that of the bulk residue.  相似文献   

12.
We report the results of an experiment that produced a residue which closely matches the hydrocarbon component of the Murchison carbonaceous chondrite. This experiment suggests that the parent material of the meteoritic component originated as polycyclic aromatic hydrocarbon species in carbon stars during their later stages of evolution. The experiments also indicate that the pathway from those formation sites to eventual incorporation into the meteorite parent body involved hydrogenation in a plasma in the solar nebula or in H II regions prior to the solar nebula. This model is consistent with what is known about the meteoritic hydrocarbon component including deuterium abundance, the observation of cosmic infrared emission bands best attributed to polycyclic aromatic hydrocarbon molecules, and the inherent stability of these molecules that allows their formation in stars and subsequent survival in the interstellar medium.  相似文献   

13.
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   

14.
Aromatic hydrocarbons account for a significant portion of the organic matter in carbonaceous chondrite meteorites, as a component of both the low molecular weight, solvent-extractable compounds and the insoluble organic macromolecular material. Previous work has suggested that the aromatic compounds in carbonaceous chondrites may have originated in the radiation-processed icy mantles of interstellar dust grains. Here we report new studies of the organic residue made from benzene irradiated at 19 K by 0.8 MeV protons. Polyphenyls with up to four rings were unambiguously identified in the residue by gas chromatography–mass spectrometry. Atmospheric pressure photoionization Fourier transform mass spectrometry was used to determine molecular composition, and accurate mass measurements suggested the presence of polyphenyls, partially hydrogenated polyphenyls, and other complex aromatic compounds. The profile of low molecular weight compounds in the residue compared well with extracts from the Murchison and Orgueil meteorites. These results are consistent with the possibility that solid phase radiation chemistry of benzene produced some of the complex aromatics found in meteorites.  相似文献   

15.
We have developed antibodies and a multi-array competitive immunoassay (MACIA) for the detection of a wide range of molecular size compounds, from single aromatic ring derivatives or polycyclic aromatic hydrocarbons (PAHs), through small peptides, proteins or whole cells (spores). Multiple microarrays containing target molecules are used simultaneously to run several competitive immunoassays. The sensitivity of the MACIA for small organic compounds like naphthalene, 4-phenilphenol or 4-tertbutilphenol is in the range of 100–500 ppb (ng ml−1), for others like the insecticide terbutryn it is at the ppt (ng l−1) level, while for small peptides, as well as for more complex molecules like the protein thioredoxin, the sensitivity is approximately 1–2 ppb, or 104–105 spores of Bacillus subtilis per milliliter. For organic compounds, a water–methanol solution was used in order to achieve a better dissolution of the organics without compromising the antibody–antigen interaction. The above-mentioned compounds were detected by MACIA in water–(10%) methanol extracts from spiked pyrite and hematite-containing rock powder samples, as well as from a spiked-sand sample subjected to organic extraction with dichloromethane–methanol (1/1).  相似文献   

16.
Polycyclic aromatic hydrocarbons (PAHs) are important components of the interstellar medium and carbonaceous chondrites, but have never been identified in the reducing atmospheres of the outer solar system. Incompletely characterized complex organic solids (tholins) produced by irradiating simulated Titan atmospheres reproduce well the observed UV/visible/IR optical constants of the Titan stratospheric haze. Titan tholin and a tholin generated in a crude simulation of the atmosphere of Jupiter are examined by two-step laser desorption/multiphoton ionization mass spectrometry. A range of two- to four-ring PAHs, some with one to four alkylation sites are identified, with net abundance approximately 10(-4) g g-1 (grams per gram) of tholins produced. Synchronous fluorescence techniques confirm this detection. Titan tholins have proportionately more one- and two-ring PAHs than do Jupiter tholins, which in turn have more four-ring and larger PAHs. The four-ringed PAH chrysene, prominent in some discussions of interstellar grains, is found in Jupiter tholins. Solid state 13C NMR spectroscopy suggests approximately equal to 25% of the total C in both tholins is tied up in aromatic and/or aliphatic alkenes. IR spectra indicate an upper limit in both tholins of approximately equal to 6% by mass in benzenes, heterocyclics, and PAHs with more than four rings. Condensed PAHs may contribute at most approximately 10% to the observed detached limb haze layers on Titan. As with interstellar PAHs, the synthesis route of planetary PAHs is likely to be via acetylene addition reactions.  相似文献   

17.
Abstract– Even in the absence of any biosphere on Mars, organic molecules, including polycyclic aromatic hydrocarbons (PAHs), are expected on its surface due to delivery by comets and meteorites of extraterrestrial organics synthesized by astrochemistry, or perhaps in situ synthesis in ancient prebiotic chemistry. Any organic compounds exposed to the unfiltered solar ultraviolet spectrum or oxidizing surface conditions would have been readily destroyed, but discoverable caches of Martian organics may remain shielded in the subsurface or within surface rocks. We have studied the stability of three representative polycyclic aromatic hydrocarbons (PAHs) in a Mars chamber, emulating the ultraviolet spectrum of unfiltered sunlight under temperature and pressure conditions of the Martian surface. Fluorescence spectroscopy is used as a sensitive indicator of remaining PAH concentration for laboratory quantification of molecular degradation rates once exposed on the Martian surface. Fluorescence‐based instrumentation has also been proposed as an effective surveying method for prebiotic organics on the Martian surface. We find the representative PAHs, anthracene, pyrene, and perylene, to have persistence half‐lives once exposed on the Martian surface of between 25 and 60 h of noontime summer UV irradiation, as measured by fluorescence at their peak excitation wavelength. This equates to between 4 and 9.6 sols when the diurnal cycle of UV light intensity on the Martian surface is taken into account, giving a substantial window of opportunity for detection of organic fluorescence before photodegradation. This study thus supports the use of fluorescence‐based instrumentation for surveying recently exposed material (such as from cores or drill tailings) for native Martian organic molecules in rover missions.  相似文献   

18.
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   

19.
We recorded one‐ and two‐dimensional solid‐state nuclear magnetic resonance spectra of meteoric insoluble organic matter with unprecedented sensitivity and resolution permitting us to reveal unambiguous spectroscopic fingerprints relevant to its molecular and isotopic features. Two‐dimensional 1H‐1H and 1H‐13C correlation experiments have unveiled the spatial proximity between aliphatic and aromatic groups proving a highly branched character of a rigid macromolecular network composed of short aliphatic chains linking together small aromatic units. One‐dimensional 2H and two‐dimensional 1H‐2H correlation spectroscopy delivered evidence of significant reduction in the deuterium enrichment of aromatic species relevant to interstellar processes, proto‐planetary disk chemistry, and to determining the origin of the meteoritic insoluble organic matter. The experimental approach developed in this work opens new perspectives for systematic and nondestructive analysis at the molecular level of meteoritic insoluble organic matter even with a very small amount of sample from some particularly rare chondrites.  相似文献   

20.
M.L. Delitsky  C.P. McKay 《Icarus》2010,207(1):477-484
The Cassini spacecraft detected benzene high in Titan’s atmosphere as well as the presence of large mass positive and negative ions. Previous work has suggested that these large mass ions could be composed of fused-ring polycyclic aromatic hydrocarbon compounds. These fused-ring PAHs, such as naphthalene and anthracene, are usually the result of high temperature processes that may not occur in Titan’s thin, cold, upper thermosphere. Here we suggest that a different class of aromatic compounds, polyphenyls, may be a better explanation of the data. Polyphenyls can grow to be large polymeric structures and could condense to form the aerosols seen in Titan’s cloud and hazes. They have similar properties to fused-ring PAHs (for example, electron affinity, ionization potential) and could be the negative ion species seen in the CAPS instrument data from the Cassini spacecraft.  相似文献   

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