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PubMed1990

Impact-induced devolatilization and hydrogen isotopic fractionation of serpentine: implications for planetary accretion.

The degree of impact-induced devolatilization of nonporous serpentine, porous serpentine, and deuterium-enriched serpentine was investigated using two independent experimental methods, the gas recovery method and the solid recovery method, yielding consistent results. The gas recovery method enables determination of the chemical and hydrogen isotopic composition of the recovered gases. Experiments on deuterium-enriched serpentine unambiguously identify the samples as the source of the recovered gases, as opposed to other possible contaminants. For shock pressures near incipient devolatilization (Pinitial = 5.0 GPa), the hydrogen isotopic composition of the evolved gas is similar to that of the starting material. For higher shock pressures the bulk evolved gas is significantly lower in deuterium than the starting material. There is also significant reduction of H2O to H2 in gases recovered at higher shock pressures, probably caused by reaction of evolved H2O with the metal gas recovery fixture. The hydrogen isotopic fractionation between the evolved gas and the residual solid indicates nonequilibrium, kinetic control of gas-solid isotopic ratios. In contrast, gaseous H2O-H2 isotopic fractionation suggests high temperature (800-1300 K) isotopic equilibrium between the gaseous species, indicating initiation of devolatilization at sites of greater than average energy deposition (i.e., shear bands). Impact-induced hydrogen isotopic fractionation of hydrous silicates during accretion can affect the distribution of hydrogen isotopes of planetary bodies during accretion, leaving the interiors enriched in deuterium. The significance of this process for planetary development depends on the models used for extrapolation of the observed isotopic fractionation to devolatilizations greater than those investigated experimentally and assumptions about timing and rates of protoatmosphere loss, frequency of multiple impacts, and rates of gas-solid or gas-melt isotopic re-equilibration. A simple model indicates that substantial planetary interior enrichments of D/H relative to that of the incident material can result from impact-induced hydrogen fractionation during accretion.

Asbestos, Serpentine↗

PubMed1991

Correlated Si isotope anomalies and large 13C enrichments in a family of exotic SiC grains.

A suite of morphologically distinctive silicon carbide (SiC) grains from the Orgueil and Murchison carbonaceous chondrite meteorites contains Si and C of highly anomalous isotopic composition. All of the SiC grains in this suite are characterized by a distinctive platy morphology and roughly developed hexagonal crystal forms that allow them to be distinguished from other types of SiC found in the host meteorites. The delta 29Si and delta 30Si values of individual SiC crystals deviate from those of normal solar material by more than 100%, while the delta 13C values range from 150 to 5200%. Isotopically normal C and Si are not found in any of these SiC crystals. The SiC grains belonging to this morphological suite are isotopically distinct from fine-grained SiC aggregates and other morphological types of SiC in unequilibrated meteorites. The 29Si/28Si and 30Si/28Si ratios of these platy grains are well correlated and define a linear array that does not pass through the composition of normal, solar Si. This behavior contrasts sharply with the diverse and poorly correlated Si isotopic compositions shown by the total SiC population. We suggest that the distinctive morphological characteristics and comparatively simple Si isotope systematics identify the platy SiC crystals as a genetically related family, formed around a single, isotopically heterogeneous presolar star or an association of related stars. The enrichments in 13C and the Si isotope systematics of the platy SiC are broadly consistent with theoretical models of nucleosynthesis in low-mass, carbon stars on the asymptotic giant branch. The Si isotope array most plausibly reflects mixing between 28Si-rich material, inherited from a previous generation of stars, and material enriched in 29Si and 30Si, produced in intershell regions by neutron capture during He-burning. 13C is also produced in intershell regions by proton reactions on 12C seed nuclei and is carried with s-process nuclei to the stellar envelope by convection which penetrates down to the He shell. The absence of a correlation between the Si and C isotopic compositions of the SiC suggests either episodic condensation of SiC, extending over several thermal pulses, in the atmosphere of a single star, or derivation of the SiC from several stars characterized by different rates of 13C production. In the multiple star scenario, the linear correlation of the 29Si/28Si and 30Si/28Si ratios among the platy SiC indicates that these stars evolved from a common Si seed composition under similar conditions of neutron-capture nucleosynthesis. The 29Si/30Si ratio of the SiC, inferred by us to be produced by neutron capture in the stellar interior, is distinct from values calculated from models of nucleosynthesis in AGB stars.

Astronomical Phenomena↗

PubMed1991

Chronology of early Archaean granite-greenstone evolution in the Barberton Mountain Land, South Africa, based on precise dating by single zircon evaporation.

We report precise 207Pb/206Pb single zircon evaporation ages for low-grade felsic metavolcanic rocks within the Onverwacht and Fig Tree Groups of the Barberton Greenstone Belt (BGB), South Africa, and from granitoid plutons bordering the belt. Dacitic tuffs of the Hooggenoeg Formation in the upper part of the Onverwacht Group yield ages between 3445 +/- 3 and 3416 +/- 5 Ma and contain older crustal components represented by a 3504 +/- 4 Ma old zircon xenocryst. Fig Tree dacitic tuffs and agglomerates have euhedral zircons between 3259 +/- 5 and 3225 +/- 3 Ma in age which we interpret to reflect the time of crystallization. A surprisingly complex xenocryst population in one sample documents ages from 3323 +/- 4 to 3522 +/- 4 Ma. We suspect that these xenocrysts were inherited, during the passage of the felsic melts to the surface, from various sources such as greenstones and granitoid rocks now exposed in the form of tonalite-trondhjemite plutons along the southern and western margins of the BGB, and units predating any of the exposed greenstone or intrusive rocks. Several of the granitoids along the southern margin of the belt have zircon populations with ages between 3490 and 3440 Ma. coeval with or slightly older than Onverwacht felsic volcanism, while the Kaap Valley pluton along the northwestern margin of the belt is coeval with Fig Tree dacitic volcanism. These results emphasize the comagmatic relationships between greenstone felsic volcanic units and the surrounding plutonic suites. Some of the volcanic plutonic units contain zircon xenocrysts older than any exposed rocks. These indicate the existence of still older units, possibly stratigraphically lower and older portions of the greenstone sequence itself, older granitoid intrusive rocks, or bodies of older, unrelated crustal material. Our data show that the Onverwacht and Fig Tree felsic units have distinctly different ages and therefore do not represent a single, tectonically repeated unit as proposed by others. Unlike the late Archaean Abitibi greenstone belt in Canada, which formed over about 30 Ma. exposed rocks in the BGB formed over a period of at least 220 Ma. The complex zircon populations encountered in this study imply that conventional multigrain zircon dating may not accurately identify the time of felsic volcanic activity in ancient greenstones. A surprising similarity in rock types, tectonic evolution, and ages of the BGB in the Kaapvaal craton of southern Africa and greenstones in the Pilbara Block of Western Australia suggests that these two terrains may have been part of a larger crustal unit in early Archaean times.

Crystallization↗

PubMed1991

Diffusion of a multi-species component and its role in oxygen and water transport in silicates.

An important but poorly understood factor that affects diffusion rates is the role of speciation during diffusion of a multi-species component. The diffusion of such a component is complicated by the different diffusion coefficient of each species and the interconversion reactions among the species. These complexities can be treated by a diffusion equation that incorporates the diffusive fluxes of all species contributing to the concentration of the component. The effects of speciation on the diffusion of the component can be investigated experimentally in some simple cases by measuring concentration profiles of all species developed during diffusion experiments or by studying some of their other consequences. Experimental data on water diffusion in rhyolitic glasses indicate that although dissolved water is present as two species, H2O molecules and OH groups, molecular H2O is the dominant diffusing species at very low to high water concentrations. This explains the apparently complex behavior of water diffusion. Experimental data on oxygen diffusion in some silicates using 18O tracers in the form of H2(18O) are consistent with the idea that 18O transport is dominated by diffusion of H2O molecules even at lower water contents (ppm or less). This explains why oxygen transport depends on the presence of water and generally depends on water fugacity linearly. For this mode of oxygen transport, there is a simple theoretical relationship between the effective total oxygen diffusion coefficient and the total water diffusion coefficient that is a function of only the water concentration of the silicate at low water content. This relationship appears to describe quantitatively the existing data over a wide range in water contents and diffusion coefficients in several phases.

Diffusion↗

PubMed1992

What determines the volume of the oceans?

The volume of Earth's oceans may be determined by a dynamic mechanism involving exchange of water between the crust and the mantle. Fast-spreading mid-ocean ridges are currently submerged to a depth at which the pressure is close to the critical pressure for seawater. This ensures optimal convective heat transport and, hence, maximal penetration of hydrothermal circulation along the ridge axes. The oceanic crust is hydrated to a depth of a kilometer or more and can therefore carry a substantial flux of water to the upper mantle when it is subducted. The current ingassing rate of water by this process is probably at least sufficient to balance the outgassing rate. If the oceans were shallower, as they may have been in the distant past, convective heat transport would be reduced and the depth of hydrothermal penetration and crustal hydration would decrease. Outgassing would exceed ingassing and ocean volume would increase. The system is self-stabilizing as long as the depth of the oceans does not exceed its present value. This mechanism could explain why continental freeboard has remained approximately constant since the Archean despite probable increases in continental area.

Climate↗

PubMed1993

Time-resolved tryptophan fluorescence in photosynthetic reaction centers from Rhodobacter sphaeroides.

Tryptophan fluorescence of reaction centers isolated from Rhodobacter sphaeroides, both stationary and time-resolved, was studied. Fluorescence kinetics were found to fit best a sum of four discrete exponential components. Half of the initial amplitude was due to a component with a lifetime of congruent to 60 ps, belonging to Trp residues, capable of efficient transfer of excitation energy to bacteriochlorophyll molecules of the reaction center. The three other components seem to be emitted by Trp ground-state conformers, unable to participate in such a transfer. Under the influence of intense actinic light, photooxidizing the reaction centers, the yield of stationary fluorescence diminished by congruent to 1.5 times, while the number of the kinetic components and their life times remained practically unchanged. Possible implications of the observed effects for the primary photosynthesis events are considered.

Amino Acid Sequence↗

PubMed1988

Deuterium exchange during acid-demineralisation.

Isotopic analyses of residues prepared by demineralisation of the Murchison meteorite using D-labelled reagents provide evidence for measurable exchange of H-isotopes between residue and reagents. Precise quantification of this effect is precluded by substantial inhomogeneity of the meteoritic organic matter. A conservative estimate of the degree of exchange is 3 to 5% of the H pyrolysable as H2O. This could affect the shape of the curve defining D-release as a function of temperature, but does not change conclusions previously drawn concerning the nature of the bulk D-enrichment of insoluble organic matter in meteorites.

Astronomical Phenomena↗

PubMed1989

Origins of etioporphyrins in sediments: evidence from stable carbon isotopes.

In samples of the Julia Creek and Condor oil shales (Australia, Albian, and early Tertiary, respectively) etioporphyrin III is significantly depleted in 13C (4%) relative to porphyrins derived from chlorophylls. This isotopic difference suggests a large contribution from some independent source. The haem group found in cytochromes derived from microbial sources is the most likely candidate.

Australia↗

PubMed1990

Aliphatic hydrocarbons of the Murchison meteorite.

The indigenous organic compounds of carbonaceous chondrites have been difficult to characterize because of problems arising from terrestrial contamination. The fall of the Murchison meteorite (CM2) provided pristine samples which allowed the resolution of some prior ambiguities as, for example, in the case of the amino acids. However, the nature of the aliphatic hydrocarbons has remained unclear. Shortly after the Murchison fall, one laboratory found them to be mainly cycloalkanes; another found, in order of abundance, branched alkanes, olefins, and cycloalkanes; while a third reported predominantly n-alkanes followed by methyl alkanes and olefins. We have reinvestigated this question using benzene-methanol as the extraction solvent, silica-gel chromatography for fractionation of the extract, and GC-MS, and IR and NMR spectroscopic techniques for the analyses. When interior samples were obtained and the analyses carried out under conditions that minimized environmental contaminants, we have found the principal aliphatic components of the Murchison meteorite to be a structurally diverse suite of C15 to C30 branched alkyl-substituted mono-, di-, and tricyclic alkanes. Comparative analyses were carried out on the Murray (CM2), Allende (CV3), and New Concord (L6) chondrites that illustrate the nature of the contamination problem encountered with carbonaceous chondrites.

Alkanes↗

PubMed1990

Xenon fractionation in porous planetesimals.

The distinctively fractionated Xe on Mars and Earth may have its root in a common source from which both planets accreted. We begin with Ozima and Nakazawa's hypothesis that terrestrial Xe fractionation was caused by gravitational separation of adsorbed solar nebular gases inside large porous planetesimals. We point out that Xe would have been trapped as the planetesimal grew and pores were squeezed shut by lithostatic pressure. We show that enough fractionated Xe to supply the Earth could have been trapped this way. The degree of fractionation is controlled by the lithostatic pressure at the pore-closing front and so would have been roughly the same for all large planetesimals. The predicted degree of fractionation agrees well with that preserved in terrestrial and martian Xe. Relative to Xe, this source is strongly depleted in other noble gases. In contrast to the original Ozima and Nakazawa hypothesis, our hypothesis predicts the observed fractionation, and it allows planetary accretion to occur after the dissipation of the solar nebula. The required planetesimals are large, representing a class of object now extinct in the solar system.

Atmosphere↗

PubMed1990

Primary and diagenetic controls of isotopic compositions of iron-formation carbonates.

Mineralogic, chemical, and isotopic compositions have been determined for 97 carbonate microbands in five core segments from the early Proterozoic (2.5 Ga) Dales Gorge Member of the Brockman Iron Formation, Hamersley Basin, Western Australia. Samples were obtained both from banded iron-formation (BIF) macrobands 9-12 at Paraburdoo, on the southern margin of the basin, and from BIF macroband 13 at Wittenoom, 130 km NW. At Paraburdoo, oxygen-isotopic compositions of coexisting chert and magnetite microbands were measured and indicated final equilibration temperatures ranging from 60-160 degrees C. This range is consistent with observed mineral assemblages and indicates a considerable temperature gradient across the basin (cf. T approximately 300 degrees C at Wittenoom; BECKER and CLAYTON, 1976). Carbon-isotopic compositions of carbonates are near -7% vs. PDB at Paraburdoo and -10.5% at Wittenoom, but the greater isotopic depletion at Wittenoom appears related to primary or diagenetic processes, not metamorphism. Contents of organic carbon are consistently low. Isotopic depletion is roughly correlated with iron abundance and, together with petrographic observations and chemical balances, is consistent with the model of BIF deposition introduced by BEUKES et al. (1990): primary siderite (delta approximately -5%) precipitated from an anoxic water column depleted in 13C; additional depletion of 13C is associated with coprecipitation of iron oxides and organic carbon. Oxygen-isotopic abundances of microbanded carbonates are similar to those under- and overlying massive marine carbonates, ranging from 17.6 to 21.0% vs. SMOW (-9.6 to -12.9% vs. PDB). Millimeter-scale variations in abundances of 13C and 18O are associated with diagenetic replacement of primary siderite by secondary ankerite and/or magnetite. It is shown that these isotopic variations cannot result from mineral-dependent fractionations, metamorphism, or the influence of large volumes of water in an open system.

Carbon↗

PubMed1991

The composition of Permian seawater.

Forty-nine brine inclusions in marine halite from the Ochoan Salado Formation in the Delaware Basin and fifteen inclusions in halite from the Leonardian Wellington Formation in the Kansas Basin were extracted, and their chemical compositions were determined. The brines are of the Na-K-Mg-Cl-SO4 type; their compositions resemble those of evaporated modern seawater. The values of (mCl(-) - mNa+)/mBr- and (mMg(2+) + mCa(2+) - mSO4(2-) - 1/2mHCO3-)/mBr- of the inclusion brine from the two formations are equal to or slightly higher than those of modern seawater. The original mNa+/mBr- and mCl-/mBr- ratios of the inclusion brines were probably equal to or slightly larger than those of modern seawater. The values of mMg2+/mBr- of the inclusion brines from the Salado Formation are very close to that of modern seawater; the ratios of inclusion brines from the Wellington Formation are slightly lower, probably due to the formation of dolomite/magnesite. The mMg2+/mBr- ratio in the initial seawater was probably close to the parent seawater of the Salado brines. The values of (mSO4(2-) - mCa(2+) + 1/2mHCO3-)/mBr- of the inclusion brines appear to be reduced by the formation of dolomite/magnesite, and the value of this ratio in Permian seawater was probably similar to that of modern seawater. The mK+/mBr- ratios of the inclusion brines are variable, but the original ratios are probably close to or slightly larger than that of modern seawater. If the Br- concentration of Permian seawater was equal to that of modern seawater, the composition of Permian seawater can be narrowly constrained; in mmol/kg H2O, 460 < or = mNa+ < 630, 550 < or = mCl- < 730, mMg2+ = 54 +/- 6, mK+ approximately equal to 11, (mSO4(2-) - mCa(2+) + 1/2mHCO3-) > or = 17, 20 < mSO4(2-) < 45, 5 < mCa2+ < 20, and 0.15 < mHCO3- < 5. The composition of Permian seawater was therefore quite similar to that of modern seawater.

Bicarbonates↗

PubMed1991

Diffusion of water in rhyolitic glasses.

Water dehydration experiments on rhyolitic glasses have been carried out at 400-550 degrees C under a N2 atmosphere. Concentration profiles of both H2O molecules and OH groups were measured by Fourier transform infrared spectroscopy. As found in previous studies of water diffusion in rhyolitic melts, the measured total water concentration profiles do not match expectations based on a single constant diffusion coefficient for total water. The diffusion of total water is described by considering the diffusion of both H2O molecules and OH groups and the reaction between them. The concentration relationship between the two species has been obtained from direct infrared measurement on quenched experimental charges. The quench is inferred to be rapid enough to preserve concentrations of both species at experimental temperature based on experimental results designed to examine reaction kinetics. The measured species concentrations along diffusion profiles show that local equilibrium between H2O and OH is approximately reached at high temperatures and high water contents. However, at lower water content or lower temperature, local equilibrium is not reached. In treating the diffusion problem, this disequilibrium effect is partially compensated by using empirical relationships between H2O and OH concentrations based on measurements, instead of using an equilibrium relationship. It is thus possible to obtain diffusion coefficients for both species from their concentration profiles. The diffusion coefficient of OH is found to be negligible compared to that of H2O at 403-530 degrees C (DOH < 0.02 DH2O and could be much smaller); i.e., H2O is the dominant diffusing species even at total water concentration as low as 0.2 wt%. The variation of OH concentration along the diffusion profile is inferred to be due to the local interconversion between OH groups and H2O molecules; the reaction also provides the diffusing H2O species. DH20 values are found to vary by less than a factor of 2 over a total water concentration range of 0.2 to 1.7 wt%. This simple model, coupled with the assumption of local equilibrium between H2O and OH, yields a very good fit to the data from diffusion-couple experiments of LAPHAM et al. (1984) at 850 degrees C. When our data are combined with DH2O obtained from that fit, DH2O (in m2/s) is given by: ln DH2O = (-14.59 +/- 1.59) - (103000 +/- 5000) / RT; 673 K < or = T < or = 1123 K, where T is temperature in K and R is the gas constant in J K-1 mol-1. This equation also approximates well DH2O values calculated from previous measurements of concentration-dependent bulk water diffusion coefficients of KARSTEN et al. (1982). The diffusion of H2O is also compared to the diffusion of the noble gas elements. The activation energy for diffusion in rhyolitic glasses is well correlated with neutral species radii of He, Ne, H2O, and Ar. This supports the contention that the diffusing species for "water" is neutral molecular H2O. The role of speciation may also be important in understanding the diffusion of many other multi-species components, and the effect can be treated in a similar fashion as that during water diffusion.

Diffusion↗

PubMed1991

Implanted 3He, 4He, and Xe in further studies of diamonds from Western Australia.

In measurements of the noble gases in additional samples of diamonds from the Argyle and Ellendale lamproites in Western Australia we have failed to encounter any neon-rich stones such as showed solar-like isotopic compositions in earlier work. No neon was detected above the relatively high blank levels in our glass apparatus. White and brown diamonds showed no differences in noble gas content, nor did samples segregated by the color of long-wave UF fluorescence. The rare gas patterns in the 1.2 Ga Argyle pipe are largely consistent with implanted 3He, 4He, and fissiogenic Xe from U/Th in the matrix rock in which the diamonds have been stored for so long. These implanted species are absent in diamonds from the much younger (approximately 20 Ma) Ellendale pipe. We give implantation formulae for several models of inhomogeneously distributed U/Th. Differences in 3He content between pipe and alluvial Argyle samples are consistent with expected cosmogenic production in the latter. An expanded data base for helium and carbon isotopic data on the same samples supports a negative [4He]-delta 13C correlation seen earlier in work from our group, but if the Argyle samples, which contain light carbon, are corrected for implanted 4He, the correlation is considerably weakened. We no longer see an earlier 3He/4He-delta 13C correlation.

Carbon Isotopes↗

PubMed1991

Isotopic analyses of amino acids from the Murchison meteorite.

Previous isotopic analyses of the total amino acids of the Murchison meteorite showed these compounds to be substantially enriched in 2H, 13C, and 15N relative to terrestrial organic matter. These analyses have been repeated (2H, 13C) with inclusion of an ultrafiltration step to exclude the possibility that a fine particulate contaminant carried the isotopic excesses observed in the previous work. In addition, the meteorite amino acids were chromatographically separated to rule out the possibility that the isotopic enrichment of the meteorite extract could reside in basic compounds other than amino acids. The results indicate that the Murchison amino acids are truly isotopically unusual, that the isotopic excesses reside in at least several different amino acids, and that the isotopic contents of some of these amino acids reach values of about +40% (delta 13C) and +2500% (delta D). If it is assumed that the high deuterium content of the meteorite alpha-amino acids is a result of the synthesis of their molecular precursors by low temperature ion-molecule reactions in an interstellar cloud, their formation by aqueous phase Strecker reactions in the parent body is consistent with their general characteristics and with known parent body processes.

Amino Acids↗

PubMed1991

Strontium isotopic variations of Neoproterozoic seawater: implications for crustal evolution.

We report high precision Sr isotopic data on carbonates from the Neoproterozoic Shaler Group, Victoria Island, Northwest Territories, Canada. Lithostratigraphic correlations with the relatively well-dated Mackenzie Mountains Supergroup constrain Shaler deposition to approximately 770-880 Ma, a range corroborated by 723 +/- 3 Ma lavas that disconformably overlie Shaler carbonates and by Late Riphean microfossils within the section. Samples with low 87Rb/86Sr ratios (<0.01) were selected for Sr isotopic analysis. Delta 18O, Mn, Ca, Mg, and Sr data were used to recognize altered samples. The altered samples are characterized by high Mn/Sr (> or = 2) and variable delta 18O; most are dolomites. The data indicate that between ca. 790-850 Ma the 87Sr/86Sr ratio of seawater varied between 0.70676 and 0.70561. The samples show smooth and systematic variation, with the lowest 87Sr/86Sr value of 0.70561 at ca. 830 Ma. The low 87Sr/86Sr ratio of carbonates from the lower parts of our section is similar to a value reported for one sample from the Adrar of Mauritania (approximately 900 Ma), West African Craton. Isotopic ratios from the upper part of the Shaler section are identical to values from the lower part of the Neoproterozoic Akademikerbreen Group, Spitsbergen. Although a paucity of absolute age determinations hinders attempts at the precise correlation of Neoproterozoic successions, it is possible to draw a broad outline of the Sr isotopic composition of seawater for this period. Indeed, the Sr isotope data themselves provide a stratigraphic tool of considerable potential. Data from this study and the literature are used to construct a curve of the 87Sr/86Sr ratio of Neoproterozoic seawater. The new data reported in this study substantially improve the isotopic record of Sr in seawater for the period 790-850 Ma. The Sr isotope composition of seawater reflects primarily the balance between continental Sr input through river input and mantle input via hydrothermal circulation of seawater through mid-ocean ridges. Coupling of Nd and Sr isotopic systems allows us to model changes in seafloor spreading rates (or hydrothermal flux) and continental erosion. The Sr hydrothermal flux and the erosion rate (relative to present-day value) are modeled for the period 500-900 Ma. The results indicate that the hydrothermal flux reached a maximum value at ca. 830 Ma. In contrast, a large peak in erosion rate is indicated at ca. 570 Ma. The peaks in hydrothermal flux and erosion rate are most likely related to developments in the Pan-African and related orogenic events, whose initial development is characterized by production of juvenile crust during supercontinental break up and rifting. The time ca. 570 Ma is characterized by continent-continent collision and production of recycled crust. Sr isotope data from Proterozoic carbonates offer a valuable resource for understanding large-scale crust dynamics.

Africa, Western↗

PubMed1991

Isotopic composition of hydrogen in insoluble organic matter from cherts.

Robert (1989) reported the presence of unusually enriched hydrogen in the insoluble HF-HCl residue extracted from two chert samples of Eocene and Pliocene ages. Since the presence of heavy hydrogen might be due to the incorporation of extraterrestrial materials, we desired to reexamine the same samples to isolate the D-rich components. Our experiments did not reveal any D-rich components, but the hydrogen isotope composition of the insoluble residue of the two chert samples was well within the range expected for terrestrial organic matter. We also describe a protocol that needs to be followed in the hydrogen isotope analysis of any insoluble organic matter.

Deuterium↗

PubMed1992

Isotopic and molecular analyses of hydrocarbons and monocarboxylic acids of the Murchison meteorite.

The monocarboxylic acids and hydrocarbons of the Murchison meteorite (CM2) were isolated for isotopic analysis. The nonvolatile hydrocarbons were analyzed as crude methanol and benzene-methanol extracts and also after separation by silica gel chromatography into predominantly aliphatic, aromatic, and polar hydrocarbon fractions. The volatile hydrocarbons were obtained after progressive decomposition of the meteorite matrix by freeze-thaw, hot water, and acid treatment. Molecular analyses of the aromatic hydrocarbons showed them to comprise a complex suite of compounds in which pyrene, fluoranthene, phenanthrene, and acenaphthene were the most abundant components, a result similar to earlier analyses. The polar hydrocarbons also comprise a very complex mixture in which aromatic ketones, nitrogen, and sulfur heterocycles were identified. Both delta 13C and delta D values were obtained for all preparations. The monocarboxylic acids, aliphatic, aromatic, and polar hydrocarbons, and the indigenous volatile hydrocarbons were found to be D-rich with delta D values ranging from about +100 to +1000. The delta 13C values ranged overall from -13 to +17. The deuterium enrichment observed in these compounds is suggestive of a relationship to interstellar organic compounds. In two separate analyses, the delta D values of the nonvolatile hydrocarbons were observed to increase in the following order: aliphatic < aromatic < polar. This finding is consistent with an early solar system or parent body conversion of aromatic to aliphatic compounds as well as the earlier suggestion of pyrolytic formation of aromatic from aliphatic compounds.

Benzene↗