Sherwood Chang

Carbonaceous chondrites. II - Carbonaceous chondrite phyllosilicates and light element geochemistry as indicators of parent body processes and surface conditions

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.

Organic Matter in Meteorites: Molecular and Isotopic Analyses of the Murchison Meteorite

Carbonaceous chondrites comprise a unique subset of meteorites. Two classes of carbonaceous chondrites, the so-called CI1 and CM2 chondrites, are particularly interesting, in part because of their relatively high carbon content and the fact that most of this carbon is present as organic matter. This material is largely macromolecular but also contains a complex mixture of organic compounds that include carboxylic acids, dicarboxylic acids, amino acids, hydroxy acids, sulfonic acids, phosphonic acids, amines, amides, nitrogen heterocycles including purines and a pyrimidine, alcohols, carbonyl compounds, and aliphatic, aromatic, and polar hydrocarbons. The organic-rich CI1 and CM2 chondrites also contain an extensive clay mineralogy and other minerals that are believed to be indicative of an early episode of hydrous activity in the meteorite parent body. Recent stable isotope measurements have shown the organic matter in general, to be substantially enriched in deuterium and the discrete organic compounds to be enriched in 15N and somewhat enriched in 13C relative to terrestrial matter. These findings suggest that the organic matter is comprised of, or is closely related to, interstellar organic compounds. The organic chemistry of these meteorites is consistent with a formation scheme in which (1) a parent body was formed from volatile-rich icy planetesimals containing interstellar organic matter, (2) warming of the parent body led to an extensive aqueous phase in which the interstellar organics underwent various reactions, and (3) residual volatiles were largely lost leaving behind the suite of nonvolatile compounds that now characterize these meteorites.

Isotopic characterisation of kerogen-like material in the Murchison carbonaceous chondrite☆

Isotopic data for C, H and N in acid-resistant residues from carbonaceous chondrites show substantial variability during stepwise pyrolysis and/or combustion. After subtraction of contributions due apparently to inorganic C grains, of probably circumstellar origin, considerable isotopic variability remains, attributable to the kerogen-like organic fraction. That variability may be interpreted in terms of three or four distinct components, based on C, H and N isotopes. The relative proportions of those components vary significantly from sample to sample. The different isotopic components are tentatively identified in terms of specific chemical/structural moieties within the kerogen-like material. This combination of chemical, structural and isotopic information suggests a complex for meteoritic organic matter. At least three components within the organic populations as a whole still carry a signature of apparently interstellar D-enrichment. Part, at least, of the interstellar carrier consisted of reactive entities, not solely polymers.

The possible role of solid surface area in condensation reactions during chemical evolution - Reevaluation

SummaryPublished data on adsorption and condensation of amino acids, purine and pyrimidine bases, sugars, nucleosides, and nucleotides are analyzed in connection with Bernals hypothesis that clays and other minerals may have provided the most likely surface for adsorption and condensation of these molecules in prebiotic times. Using surface concentration and reaction rate as the main criteria for the feasibility of condensation reactions, four types of prebiotic environments were analyzed: (1) an ocean-sediment system, (2) a dehydrated lagoon bed produced by evaporation, (3) the surface of a frozen sediment, and (4) a fluctuating system where hydration (rainstorms, tidal variations, flooding) and dehydration (evaporation) take place in a cyclic manner. With the possible exception of nucleotides, low adsorption of organomonomers on sediment surfaces of a prebiotic ocean (pH 8) is expected, and significant condensation is considered unlikely. In dehydrated and frozen systems, high surface concentrations are probable and condensation is more likely. In fluctuating environments, condensation rates will be enhanced and the size distribution of the oligomers formed during dehydration may be influenced by a “redistribution mechanism” in which adsorbed oligomers and monomers are desorbed and redistributed on the solid surface during the next hydration-dehydration cycle.

A SEARCH FOR C60 IN CARBONACEOUS CHONDRITES

Analysis of interior samples of the Murchison meteorite by two routes yielded an upper limit of 2 ppb for its C60 content, as compared to parts per million levels for individual polycyclic aromatic hydrocarbons (PAHs). Provided the samples contain an interstellar component, which is probable since Murchison hydrocarbons contain excess deuterium, this result argues against the ubiquitous presence of C60 in the interstellar medium. A possible explanation for the absence of C60 was found in experiments showing how PAHs replace fullerenes as stable end products when hydrogen is present during carbon condensation. As a secondary result we found high molecular weight PAHs in the Murchison and Allende meteorites. Coronene and its methyl derivatives are especially interesting since features in the coronene spectrum have been shown to match some of the unidentified interstellar infrared emission bands.

Carbonaceous components in the comet Halley dust

Cometary grains containing large amounts of carbon and/or organic matter (CHON) were discovered by in situ measurements of comet Halley dust composition during VEGA and GIOTTO flyby missions. In this paper, we report the classification of these cometary grains by means of cluster analysis, discuss the resulting compositional groups, and compare them with substances observed or hypothesized in meteorites, interplanetary dust particles, and the interstellar medium. Grains dominated by carbon and/or organic matter (CHON grains) represent approximately 22% of the total population of measured cometary dust particles. They usually contain a minor abundance of rock-forming elements as well. Grains having organic material are relatively more abundant in the vicinity of the nucleus than in the outer regions of the coma, which suggests decomposition of the organics in the coma environment. The majority of comet Halley organic particles are multicomponent mixtures of carbon phases and organic compounds. Possibly, the cometary CHON grains may be related to kerogen material of an interstellar origin in carbonaceous meteorites. Pure carbon grains, hydrocarbons and polymers of cyanopolyynes, and multi-carbon monoxides are present in cometary dust as compositionally simple and distinctive components among a variety of others. There is no clear evidence of significant presence of pure formaldehyde or HCN polymers in Halley dust particles. The diversity of types of cometary organic compounds is consistent with the interstellar dust model of comets and probably reflects differences in composition of precursor dust. Preservation of this heterogeneity among submicron particles suggests the gentle formation of cometary nucleus by aggregation of interstellar dust in the protosolar nebula without complete mixing or chemical homogenization at the submicron level.

Carbonaceous chondrites. I - Characterization and significance of carbonaceous chondrite /CM/ xenoliths in the Jodzie howardite

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.

Modification of amino acids at shock pressures of 3.5 to 32 GPa.

Amino acids were subjected to shock impact over a pressure range of 3.5 to 32 GPa both within and without meteoritic mineral matrices. The extent of amino acid destruction, racemization, and conversion to secondary amino acids was examined. Abundances of parent compounds decreased by a factor of 10(3) over this pressure range. Racemization also occurred, but some residual optical activity remained in the amino acids surviving shocks up to 32 GPa. Secondary amino acids formed in the high peak pressure range; those identified were beta-alanine, glycine, alanine, gamma-aminobutyric acid, and beta-aminoisobutyric acid. At 30 GPa, the abundances of these daughter compounds exceeded those of the remaining initial amino acids. As the concomitant effects of high mechanical stress and temperature accompanying shocks cannot be separated in this work, their relative contribution to the observed transformations cannot be estimated. The survival of amino acids in shock experiments suggests that, after formation or emplacement of amino acids in carbonaceous chondrite parent bodies, these objects never experienced impact velocities greater than 5 km/s, which suffices to generate 30 GPa for typical silicate/silicate impacts. These results also provide guidelines for choosing appropriate capture media for interplanetary dust particles on Earth-orbiting platforms.

The Strecker synthesis as a source of amino acids in carbonaceous chondrites: Deuterium retention during synthesis

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.

Phosphorylation by way of inorganic phosphate as a potential prebiotic process.

Conditions can be created in which inorganic phosphates act as phosphorylating agents. Such reactions may have occurred in prebiotic chemical processes.