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1.
Acid leaching of the primitive C-chondrite Murchison and O-chondrite QUE 97008 reveal nucleosynthetic anomalies in Cr, Sr, Ba, Nd, Sm and Hf. The anomalies in all but Cr and Sm are best explained by variable additions of pure s-process nuclides to a background nebular composition slightly enriched in r-process isotopes compared to average Solar System material. Leaching leaves a residue in Murchison that is strongly enriched in s-process nuclides with depletions of over 0.1% in 135Ba and seven parts in 10,000 in 84Sr. If there are p-process anomalies in these two elements, they are lost in the variability caused by different r-, s-process contributions to the normalizing isotopes. The concentration and isotope systematics are consistent with the Ba and Sr isotopic composition in the Murchison residue being strongly influenced by s-process-rich presolar SiC. In general, the nucleosynthetic isotope anomalies are 2- to 5-fold smaller in QUE 97008 than in Murchison. The different magnitudes of isotope anomalies are similar to the difference in matrix abundance between CM and O chondrites consistent with the suggestion that the carriers of nucleosynthetically anomalous material preferentially reside in the matrix and that some of this material has been distributed throughout the O-chondrite minerals as a result of thermal metamorphism.Neodymium, Sm and Hf display variable s-, r-process nuclide abundances as in Ba and Sr, but the anomalies are much smaller (e.g. ε148Nd, ε148Sm = −5.7, 2.1, respectively, in Murchison and −0.43, 0.16, respectively in QUE 97008 residues). After correcting Nd and Sm for s-, r-process variability, Sm in whole rock chondrites shows variable relative abundances of the p-process isotope 144Sm that correlate weakly with 142Nd suggesting that the direct p-process contribution to 142Nd is small (∼7-9%). Nucleosynthetic variability in Nd explains the range in 142Nd/144Nd seen between C and O, E-chondrites, but not the difference between chondrites and all modern Earth rocks, leaving decay of 146Sm and a superchondritic Sm/Nd ratio as the likely explanation for Earth’s high 142Nd/144Nd.  相似文献   

2.
New precise Te isotope data acquired by multiple collector inductively coupled plasma mass spectrometry (MC-ICPMS) are presented for selected extraterrestrial and terrestrial materials. Bulk samples of carbonaceous, ordinary and enstatite chondrites as well as the metal and sulfide phases of iron meteorites were analyzed to search for nucleosynthetic isotope anomalies and to find evidence of formerly live 126Sn, which decays to 126Te with a half-life of 234,500 yr. None of the meteorites show evidence of mass dependent Te isotope fractionations larger than 2‰ for δ126/128Te. Following internal normalization of the data to 125Te/128Te, the Te isotope ratios of all analyzed meteorites were found to be identical to a terrestrial standard, within uncertainties. This provides evidence that the regions of the solar disk that were sampled during accretion of the meteorite parent bodies were well mixed and homogeneous on a large scale, with respect to Te isotopes. The data acquired for bulk carbonaceous chondrites indicate that the initial 126Sn/118Sn ratio of the solar system was <4 × 10−5, but this is dependent on the assumption that no redistribution of Sn and Te occurred since the start of the solar system. Five Archean sedimentary sulfides that display both mass dependent and mass-independent isotope effects for S yield internally normalized Te isotope data, which indicate that mass-independent Te isotope effects are absent. The mass dependent fractionations in these samples are constrained to be less than ∼1‰ for δ126/128Te.  相似文献   

3.
Stepwise dissolutions of the carbonaceous chondrites Orgueil (CI), Murchison (CM) and Allende (CV) reveal large nucleosynthetic anomalies for Zr isotopes that contrast with the uniform compositions found in bulk meteorites. Two complementary nucleosynthetic components are observed: one enriched and one depleted in s-process nuclides. The latter component, characterized by excess 96Zr, is most distinctive in the acetic acid leachate (up to ε96Zr ≈ 50). The excess decreases with increasing acid strength and the final leaching steps of the experiment are depleted in 96Zr and thus enriched in s-process nuclides. Presolar silicon carbide grains are likely host phases for part of the anomalous Zr released during these later stages. However, by mass balance they cannot account for the 96Zr excesses observed in the early leaching steps and this therefore hints at the presence of at least one additional carrier phase with significant amounts of anomalous Zr. The data provide evidence that average solar system material consists of a homogenized mixture of different nucleosynthetic components, which can be partly resolved by leaching experiments of carbonaceous chondrites.  相似文献   

4.
We discuss the possible stellar sources of short-lived radionuclides (SLRs) known to have been present in the early solar system (26Al, 36Cl, 41Ca, 53Mn, 60Fe, 107Pd, 129I, 182Hf, 244Pu). SLRs produced primarily by irradiation (7Be, 10Be) are not discussed in this paper. We evaluate the role of the galactic background in explaining the inventory of SLRs in the early solar system. We review the nucleosynthetic processes that produce the different SLRs and place the processes in the context of stellar evolution of stars from 1 to 120 M⊙. The ejection of newly synthesized SLRs from these stars is also discussed. We then examine the extent to which each stellar source can, by itself, explain the relative abundances of the different SLRs in the early solar system, and the probability that each source would have been in the right place at the right time to provide the SLRs. We conclude that intermediate-mass AGB stars and massive stars in the range from ∼20 to ∼60 M⊙ are the most plausible sources. Low-mass AGB stars fail to produce enough 60Fe. Core-collapse Type II supernovae from stars with initial masses of <20 M⊙ produce too much 60Fe and 53Mn. Sources such as novae, Type Ia supernovae, and core-collapse supernovae of O-Ne-Mg white dwarfs do not appear to provide the SLRs in the correct proportions. However, intermediate-mass AGB stars cannot provide 53Mn or the r-process elements, so if an AGB star provided the 41Ca, 36Cl, 26Al, 60Fe, and 107Pd, and if a late stellar source is required for 53Mn and the r-process elements, then two types of sources would be required. A separate discussion of the production of r-process elements highlights the difficulties in modeling their production. There appear to be two sources of r-process elements, one that produces the heavy r-process elements, including the actinides, and one that produces the elements from N to Ge and the elements ∼110 < A < ∼130. These can be assigned to SNII explosions of stars of ?11 M⊙ and stars of 12-25 M⊙, respectively. More-massive stars, which leave black holes as supernova remnants, apparently do not produce r-process elements.  相似文献   

5.
Barium isotopic compositions of chemical leachates from six carbonaceous chondrites, Orgueil (CI), Mighei (CM2), Murray (CM2), Efremovka (CV3), Kainsaz (CO3), and Karoonda (CK4), were determined using thermal ionization mass spectrometry in order to assess the chemical evolution in the early solar system.The Ba isotopic data from most of the leachates show variable 135Ba excesses correlated with 137Ba excesses, suggesting the presence and heterogeneity of additional nucleosynthetic components for s- and r-processes in the solar system. The isotopic deviations observed in this study were generally small (−1 < ε < +1) except in the case of the acid residues of CI and CM meteorites. Large deviations of 135Ba (ε = −13.5 to −5.0) and 137Ba (ε = −6.2∼−1.2) observed in the acid residues from one CI and two CM meteorites show significant evidence for the enrichment of s-process isotopes derived from presolar grains. Two models were proposed to estimate the 135Cs isotopic abundances by subtraction of the s- and r-isotopic components from the total Ba isotopic abundances in the three CM meteorites, Mighei, Murchison (measured in a previous study), and Murray. The data points show individual linear trends between 135Cs/136Ba ratios and 135Ba isotopic deviations for the three samples. Considering the different trends observed in the three CM meteorites, the Ba isotopic composition of the CM meteorite parent body was heterogeneous at its formation. Chronological information is unclear in the data for Murchison and Murray because of large analytical uncertainties imposed by error propagation. Only the Mighei meteorite data indicate the possible existence of presently extinct 135Cs (135Cs/133Cs = (2.7 ± 1.6) × 10−4) in the early solar system. Another explanation of the data for the three CM meteorite is mixing of at least three components with different Ba isotopic compositions, although this is model-dependent.  相似文献   

6.
The r-process only nuclide 247Cm decays to 235U with a characteristic half-life of ∼16 million years. 247Cm is presently extinct, but offers considerable potential as a short-lived r-process chronometer, providing constraints on the time interval between the last r-process nucleo-synthetic event and the formation of the solar system. The existence of “live” 247Cm in the early solar system should be manifested today as variations in 235U/238U, provided Cm was chemically fractionated from U when solids formed in the early solar system. Using multiple-collector ICPMS and a high-purity mixed 233U-236U spike to monitor instrumental mass fractionation, we are able to resolve variations in 235U/238U at the 1-2 epsilon level (2σM; 1 epsilon = 1 part in 10,000) on sample sizes consisting of 20 ng of uranium. Data can be acquired on smaller (<10 ng) samples with ±2-3 epsilon 2σ uncertainties. Uranium isotopic measurements and U, Nd and Sm concentrations were acquired on bulk samples of a suite of carbonaceous chondrites, unequilibrated and equilibrated ordinary chondrites and eucrites, for which conflicting results had previously been obtained. Our results show no well-resolved excursions in 235U/238U away from the terrestrial value at the ∼2 epsilon level, and constrain the amount of 247Cm-produced excess 235U atoms to less than ∼1 × 108 atoms per gram of chondritic meteorite, with respect to terrestrial 235U/238U. Large (permil- level) anomalies in 235U/238U could, however, be artificially generated in the ordinary chondrites during laboratory processing. Therefore, U may be more susceptible to isotopic fractionation during chemical processing than previously recognized, and may reconcile some of the highly conflicting ε235U results reported by previous workers for chondritic meteorites. Our results indicate that a timescale of ∼1-2 × 108 years between the last actinide producing r-process event and the formation of the solar system may not be unreasonable based on the 247Cm-235U system. However, this conclusion is far from robust at this stage because the only bulk meteorites analysed that display strong Nd/U fractionation are highly metamorphosed chondrites that may have experienced a protracted history of redistribution and re-equilibration. The search for “live” 247Cm in the early solar system can now be extended to early-formed condensates and mineral phases displaying strong Cm-U fractionations.  相似文献   

7.
Barium isotopic compositions of single 2.3-5.3 μm presolar SiC grains from the Murchison meteorite were measured by resonant ionization mass spectrometry. Mainstream SiC grains are enriched in s-process barium and show a spread in isotopic composition from solar to dominantly s-process. In the relatively coarse grain size fraction analyzed, there are large grain-to-grain variations of barium isotopic composition. Comparison of single grain data with models of nucleosynthesis in asymptotic giant branch (AGB) stars indicates that the grains most likely come from low mass carbon-rich AGB stars (1.5 to 3 solar masses) of about solar metallicity and with approximately solar initial proportions of r- and s-process isotopes. Measurements of single grains imply a wide variety of neutron-to-seed ratios, in agreement with previous measurements of strontium, zirconium and molybdenum isotopic compositions of single presolar SiC grains.  相似文献   

8.
We have analyzed the Pb isotopic compositions of whole-rocks and various components (CAIs, chondrules, and/or mineral separates) of two carbonaceous chondrites, Allende (CV3) and Murchison (CM2), and nine ordinary chondrites, Sainte Marguerite (H4), Nadiabondi and Forest City (H5), Kernouvé (H6), Bjurböle (L/LL4), Elenovka and Ausson (L5), Tuxtuac (LL5), and Saint-Séverin (LL6) by MC-ICP-MS. Three CAI fractions from Allende define an isochron with an age of 4568.1 ± 9.4 Ma (MSWD = 0.08) and plot on the same isochron as fragments of the Efremovka inclusion E60 analyzed by Amelin et al. [Amelin, Y., Krot, A. N., Hutcheon, I. D., and Ulyanov, A. A. (2002a). Lead isotopic ages of chondrules and calcium-aluminum-rich inclusions. Science297, 1679-1683]. When these two groups of samples are combined, the isochron yields an age of 4568.5 ± 0.5 (MSWD = 0.90), which is our best estimate of the age of the Solar System. Chondrules and pyroxene-olivine fractions from the ordinary chondrites yield ages that reflect the blocking of Pb isotope equilibration with the nebular gas. The combination of these ages with the corresponding metamorphic phosphate ages provides constraints on the thermal history of the different chondrite parent bodies. Among the H chondrites, Sainte Marguerite cooled to below ∼1100 K within a few My at 4565 Ma and to ∼800 K at 4563 Ma. Nadiabondi appears to have experienced a slightly more protracted cooling history with the corresponding interval lasting from 4559 to 4556 Ma. The data from Forest City and Kernouvé show evidence of late-stage perturbation with resulting U/Pb fractionation. Likewise, Pb isotopes in Tuxtuac (LL5) record a cooling history lasting from ∼4555 to 4544 Ma, which may indicate that the cooling history for the LL parent body was more prolonged than for the H parent body. We suggest a thermal evolution model for the growth of the planetary bodies based on the release of radiogenic heat from 26Al and 60Fe. This model incorporates the accretion rate, which determines the time at which the radiogenic heat becomes efficiently trapped, and the terminal size of the parent body, which controls its overall thermal inertia. The parent bodies of carbonaceous chondrites, which show little indication of metamorphic transformation, collect cooler nebular material at a relatively late stage. Small asteroids of ∼10-50 km radius accreting within 1-3 My could be the parent bodies of H and LL chondrites. The parent body of the L chondrites is likely to be a larger asteroid (r > 100 km) or possibly the product of collisions of smaller planetary bodies.  相似文献   

9.
We report the isotopic composition of molybdenum in twenty-three presolar SiC grains from the Murchison meteorite which have been measured by resonant ionization mass spectrometry (RIMS). Relative to terrestrial abundance (and normalized to s-process-only 96Mo), the majority of the analyzed grains show strong depletions in the p-process isotopes 92Mo and 94Mo and the r-process isotope 100Mo. Sixteen of these grains have δ-values <−600% for these three isotopes. The observed isotopic patterns of Mo from mainstream SiC grains clearly reveal the signature of s-process nucleosynthesis. Three-isotope plots of all grain data (δiMo vs. δ92Mo) show strong linear correlations with characteristic slopes. This finding suggests mixing of solar-like material and pure s-process material in the parent stars. Comparison with evolutionary calculations of nucleosynthesis and mixing in red giants suggests that low-mass thermally-pulsed symptotic giant branch (TP-AGB) stars are the most likely site for the observed s-process nucleosynthesis.  相似文献   

10.
Seventeen trace elements (Ag, Au, Bi, Br, Cd, Cs, Ge, In, Ir, Rb, Re, Sb, Se, Te, Tl, U and Zn) were measured by neutron activation analysis in 8 C1 samples (1 Alais, 3 Ivuna, 4 Orgueil) and in 3 C2 samples (one each of Mighei, Murchison, Murray). The results show far less scatter than earlier literature data. The standard deviation of a single measurement from the mean of 8 C1 samples lies between 2 and 14 per cent, except for the following 4 elements: Au ±18 per cent, Ag ±22 per cent, Rb ±19 per cent and Br ±33 per cent. The first two probably reflect contamination and sample heterogeneity, the last two, analytical error. Apparently C1 chondrites have a far more uniform composition than some authors have claimed.The new data suggest significant revisions in cosmic abundance for the following elements (old values in parentheses): Zn 1250 (1500), Cd 1.51 (2.12), Ir 0.72 (0.43) atoms/106 Si atoms. The Br value is also lower, 6.8 vs 20.6, but may be affected by analytical error.Relative to C1 chondrites, the C2 chondrites Mighei, Murchison and Murray are depleted in volatile elements by a factor of 0.508 ± 0.038, much more constant than indicated by oldor data. Ordinary chondrites also show a more uniform depletion relative to the new C1 data. The mean depletion factor of Sb, F, Cu, Ga, Ge, Sn, S, Se, Te and Ag is 0.227 ± 0.027 in H-chondrites. This constancy further strengthens the case for the two-component model of chondrite formation.  相似文献   

11.
When recent geological calibrations of the 176Lu decay constant are used, the 176Lu-176Hf ages of chondrites are consistently 4% too old (∼4.75 Ga). Here, we suggest that this discrepancy reflects the photoexcitation of the long-lived 176Lu ground state to the short-lived isomeric state (T1/2 = 3.7 h) by γ-rays irradiating early condensates. Irradiation may have been of solar origin and taking place at the inner edge of the nebular disk. Alternatively, the source of γ-rays could have been one or more supernova(e) exploding in the vicinity of the solar nebula. Such photoexcitation has been experimentally observed, but requires γ-ray photons that have energies in excess of 838 keV. At this stage, we cannot assess whether the Hf isotope composition of the Bulk Silicate Earth differs from that of chondrites, eucrites, and the 4.56 Ga old Martian meteorite ALH84001, and therefore, whether the precursor material for these different planetary bodies received comparable fluences of γ-rays.  相似文献   

12.
We have investigated the distribution and isotopic composition of nitrogen and noble gases, and the Ar-Ar chronology of the Bencubbin meteorite. Gases were extracted from different lithologies by both stepwise heating and vacuum crushing. Significant amounts of gases were found to be trapped within vesicles present in silicate clasts. Results indicate a global redistribution of volatile elements during a shock event caused by an impactor that collided with a planetary regolith. A transient atmosphere was created that interacted with partially or totally melted silicates and metal clasts. This atmosphere contained 15N-rich nitrogen with a pressure ?3 × 105 hPa, noble gases, and probably, although not analyzed here, other volatile species. Nitrogen and noble gases were re-distributed among bubbles, metal, and partly or totally melted silicates, according to their partition coefficients among these different phases. The occurrence of N2 trapped in vesicles and dissolved in silicates indicates that the oxygen fugacity (fO2) was greater than the iron-wüstite buffer during the shock event. Ar-Ar dating of Bencubbin glass gives an age of 4.20 ± 0.05 Ga, which probably dates this impact event. The cosmic-ray exposure age is estimated at ∼40 Ma with two different methods. Noble gases present isotopic signatures similar to those of “phase Q” (the major host of noble gases trapped in chondrites) but elemental patterns enriched in light noble gases (He, Ne and Ar) relative to Kr and Xe, normalized to the phase Q composition. Nitrogen isotopic data together with 40Ar/36Ar ratios indicate mixing between a 15N-rich component (δ15N = +1000‰), terrestrial N, and an isotopically normal, chondritic N.Bencubbin and related 15N-rich meteorites of the CR clan do not show stable isotope (H and C) anomalies, precluding contribution of a nucleosynthetic component as the source of 15N enrichments. This leaves two possibilities, trapping of an ancient, highly fractionated atmosphere, or degassing of a primitive, isotopically unequilibrated, nitrogen component. Although the first possibility cannot be excluded, we favor the contribution of primitive material in the light of the recent finding of extremely 15N-rich anhydrous clasts in the CB/CH Isheyevo meteorite. This unequilibrated material, probably carried by the impactor, could have been insoluble organic matter extremely rich in 15N and hosting isotopically Q-like noble gases, possibly from the outer solar system.  相似文献   

13.
Application of 182Hf-182W chronometry to constrain the duration of early solar system processes requires the precise knowledge of the initial Hf and W isotope compositions of the solar system. To determine these values, we investigated the Hf-W isotopic systematics of bulk samples and mineral separates from several Ca,Al-rich inclusions (CAIs) from the CV3 chondrites Allende and NWA 2364. Most of the investigated CAIs have relative proportions of 183W, 184W, and 186W that are indistinguishable from those of bulk chondrites and the terrestrial standard. In contrast, one of the investigated Allende CAIs has a lower 184W/183W ratio, most likely reflecting an overabundance of r-process relative to s-process isotopes of W. All other bulk CAIs have similar 180Hf/184W and 182W/184W ratios that are elevated relative to average carbonaceous chondrites, probably reflecting Hf-W fractionation in the solar nebula within the first ∼3 Myr. The limited spread in 180Hf/184W ratios among the bulk CAIs precludes determination of a CAI whole-rock isochron but the fassaites have high 180Hf/184W and radiogenic 182W/184W ratios up to ∼14 ε units higher than the bulk rock. This makes it possible to obtain precise internal Hf-W isochrons for CAIs. There is evidence of disturbed Hf-W systematics in one of the CAIs but all other investigated CAIs show no detectable effects of parent body processes such as alteration and thermal metamorphism. Except for two fractions from one Allende CAI, all fractions from the investigated CAIs plot on a single well-defined isochron, which defines the initial ε182W = −3.28 ± 0.12 and 182Hf/180Hf = (9.72 ± 0.44) × 10−5 at the time of CAI formation. The initial 182Hf/180Hf and 26Al/27Al ratios of the angrites D’Orbigny and Sahara 99555 are consistent with the decay from initial abundances of 182Hf and 26Al as measured in CAIs, suggesting that these two nuclides were homogeneously distributed throughout the solar system. However, the uncertainties on the initial 182Hf/180Hf and 26Al/27Al ratios are too large to exclude that some 26Al in CAIs was produced locally by particle irradiation close to an early active Sun. The initial 182Hf/180Hf of CAIs corresponds to an absolute age of 4568.3 ± 0.7 Ma, which may be defined as the age of the solar system. This age is 0.5-2 Myr older than the most precise 207Pb-206Pb age of Efremovka CAI 60, which does not seem to date CAI formation. Tungsten model ages for magmatic iron meteorites, calculated relative to the newly and more precisely defined initial ε182W of CAIs, indicate that core formation in their parent bodies occurred in less than ∼1 Myr after CAI formation. This confirms earlier conclusions that the accretion of the parent bodies of magmatic iron meteorites predated chondrule formation and that their differentiation was triggered by heating from decay of abundant 26Al. A more precise dating of core formation in iron meteorite parent bodies requires precise quantification of cosmic-ray effects on W isotopes but this has not been established yet.  相似文献   

14.
Nanoglobules are a form of organic matter found in interplanetary dust particles and primitive meteorites and are commonly associated with 15N and D isotopic anomalies that are suggestive of interstellar processes. We report the discovery of two isotopically-anomalous organic globules from the Stardust collection of particles from Comet 81P/Wild 2 and compare them with nanoglobules from the Murchison CM2 meteorite. One globule from Stardust Cometary Track 80 contains highly aromatic organic matter and a large 15N anomaly (δ15N = 1120‰). Associated, non-globular, organic matter from this track is less enriched in 15N and contains a mixture of aromatic and oxidized carbon similar to bulk insoluble organic material (IOM) from primitive meteorites. The second globule, from Cometary Track 2, contains non-aromatic organic matter with abundant nitrile (CN) and carboxyl (COOH) functional groups. It is significantly enriched in D (δD = 1000‰) but has a terrestrial 15N/14N ratio. Experiments indicate that similar D enrichments, unaccompanied by 15N fractionation, can be reproduced in the laboratory by electron irradiation of epoxy or cyanoacrylate. Thus, a terrestrial origin for this globule cannot be ruled out, and, conversely, exposure to high-energy electron irradiation in space may be an important factor in producing D anomalies in organic materials. For comparison, we report two Murchison globules: one with a large 15N enrichment and highly aromatic chemistry analogous to the Track 80 globule and the other only moderately enriched in 15N with IOM-like chemistry. The observation of organic globules in Comet 81P/Wild 2 indicates that comets likely sampled the same reservoirs of organic matter as did the chondrite parent bodies. The observed isotopic anomalies in the globules are most likely preserved signatures of low temperature (<10 K) chemistry in the interstellar medium or perhaps the outer regions of the solar nebula. In other extraterrestrial samples, D isotopic anomalies, but not those of 15N, may be explained in part by exposure to ionizing electron radiation.  相似文献   

15.
The re-vegetation of soils contaminated by potentially harmful metals is generally considered a suitable option to reduce the metal dispersion in surrounding environments. A continuous flow experiment was conducted to quantitatively assess the effect of Italian ryegrass (Lolium multiflorum Lam.) root activity on the weathering of smithsonite (ZnCO3), a common Zn mineral. At the end of the experiment (10 days), the total amount of Zn released by smithsonite was increased by a factor of 2.25 in the presence of plants. This increase was due not only to plant uptake but also to the enhancement of the Zn release into leachates. The rate of Zn release from smithsonite to leachates was 2.9 × 10−4 μg g−1 s−1 and 1.5 × 10−4 μg g−1 s−1 in the presence and the absence of plants, respectively. The strong correlation (r = 0.95; p < 0.001) between concentrations of Zn and dissolved organic C (DOC) produced by the rhizosphere activity in leachates indicated that organic root exudates and secretions were closely involved in smithsonite weathering. Although the results are derived from laboratory study, and further in situ investigations over the long term are needed, they clearly highlighted that plants can enhance metal release into the environment by accelerating mineral weathering. Therefore, it is suggested that the ability of plants to alter metal phases in soils should be further taken into account when re-vegetation strategies are proposed for the rehabilitation of metal-polluted soils.  相似文献   

16.
We have reinvestigated the Mn-Cr systematics in a number of primitive meteorites, differentiated planetesimals and terrestrial planets in order to address the chronology of the early stages of protoplanetary disk evolution and planetary formation. Our analytical procedure is based on the assumption of terrestrial abundances for 50Cr and 52Cr only; recognizing that a data reduction scheme based on Earth-like 54Cr/52Cr abundances in all meteorites is not tenable. Here we show that initial ε53Cr compositions of 54Cr-rich and 54Cr-poor acid leach fractions in the primitive carbonaceous chondrite Orgueil differ by 0.9ε, reflecting primordial mineral-scale heterogeneity. However, asteroidal processing effectively homogenized any ε53Cr variations on the planetesimal scale, providing a uniform present-day solar ε53Cr=0.20±0.10. Thus, our 53Mn-53Cr data argue against the previously suggested 53Mn heliocentric gradient. Instead, we suggest that inner Solar System objects possessed an initially homogeneous 53Mn/55Mn composition, which determined by two independent means is estimated at (6.28 ± 0.66) × 10−6. Our revised Mn-Cr age for Ste. Marguerite (SM) metamorphism of 4562.9 ± 1.0 Ma is identical to the Pb-Pb age of SM phosphates. Using this age, we confirm that mantle differentiation of the eucrite parent body occurred 4564.9 ± 1.1 Ma ago, and revise the time interval between this event and CAI formation to 2.2 ± 1.1 Ma. We also constrain metamorphism in carbonaceous chondrites of type 2 and 3 to have occurred between 1 and 6 Ma after CAI formation. The 53Mn-53Cr correlation among chondrites, planetesimals and terrestrial planets (the eucrite parent body, Mars and Earth) provides evidence for Mn/Cr fractionation within the protoplanetary disk recorded by all precursor materials of the terrestrial planets and primitive asteroids. This fractionation appears to have occurred within 2 Ma of CAI formation.  相似文献   

17.
Measurements of the dissolution rate of diopside (r) were carried out as a function of the Gibbs free energy of the dissolution reaction (ΔGr) in a continuously stirred flow-through reactor at 90 °C and pH90 °C = 5.05. The overall relation between r and ΔGr was determined over a free energy range of −130.9 < ΔGr < −47.0 kJ mo1−1. The data define a highly non-linear, sigmoidal relation between r and ΔGr. At far-from-equilibrium conditions (ΔGr ? −76.2 kJ mo1−1), a rate plateau is observed. In this free energy range, the rates of dissolution are constant, independent of [Ca], [Mg] and [Si] concentrations, and independent of ΔGr. A sharp decrease of the dissolution rate (∼1 order of magnitude) occurs in the transition ΔGr region defined by −76.2 < ΔGr ? −61.5 kJ mo1−1. Dissolution closer to equilibrium (ΔGr > −61.5 kJ mo1−1) is characterised by a much weaker inverse dependence of the rates on ΔGr. Modeling the experimental r-ΔGr data with a simple classical transition state theory (TST) law as implemented in most available geochemical codes is found inappropriate. An evaluation of the consequences of the use of geochemical codes where the r-ΔGr relation is based on basic TST was carried out and applied to carbonation reactions of diopside, which, among other reactions with Ca- and Mg-bearing minerals, are considered as a promising process for the solid state sequestration of CO2 over long time spans. In order to take into account the actual experimental r-ΔGr relation in the geochemical code that we used, a new module has been developed. It reveals a dramatic overestimation of the carbonation rate when using a TST-based geochemical code. This points out that simulations of water-rock-CO2 interactions performed with classical geochemical codes should be evaluated with great caution.  相似文献   

18.
Cadmium stable isotope cosmochemistry   总被引：2，自引：0，他引：2  
Cadmium stable isotope compositions are reported for a comprehensive suite of carbonaceous, ordinary, enstatite, and Rumuruti chondrites as well as achondrites and lunar samples (soils, breccias, pristine anorthosite). The Cd isotope analyses were performed by multiple collector ICP-MS with an external reproducibility of ±0.43‰ (2 sd) for δ114/110Cd. None of the samples shows evidence of nucleosynthetic anomalies and cosmogenic isotope effects from neutron-capture by 113Cd were only observed for two lunar samples.The Cd stable isotope compositions of type 1, 2, and some type 3 carbonaceous chondrites, EH4 enstatite chondrites, eucrites, and the Earth are essentially identical at δ114/110Cd ≈ 0.0 ± 0.4. This suggests that the portion of the solar nebula from which the inner solar system bodies accreted was homogeneous with respect to its Cd isotope composition. It also indicates that the primary volatile element depletion of the inner solar system did not involve partial kinetic Rayleigh evaporation or condensation. Furthermore no resolvable Cd isotope effects were generated during the accretion and initial differentiation of the planetary bodies.In contrast, the analyses reveal large Cd isotope effects for ordinary and some enstatite chondrites, which display δ114/110Cd values between about −8 and +16. Smaller fractionations are observed for the Rumuruti and some type 3 to 5 carbonaceous chondrites. These Cd isotope variations are thought to reflect secondary depletion or redistribution of Cd, due to open system thermal metamorphism on the meteorite parent bodies.One CAI and chondrule separates from the Allende meteorite have unexpectedly high Cd concentrations and fractionated light Cd isotope compositions with δ114/110Cd ≈ −1 to −4. These characteristics may have been established by the interaction of originally Cd-poor materials with a volatile-rich gas prior to the final accretion of the Allende parent body. The general Cd enrichment of the lunar soil and regolith mainly reflects early volcanic activity. However, decreasing Cd abundances in lunar soils correlate well with an enrichment of the heavy Cd isotopes. This relationship is best explained by suppressed Rayleigh fractionation in response to space weathering.  相似文献   

19.
An excellent 53Mn-53Cr isochron for bulk CI, CM, CO, CV, CB, and ungrouped C3 chondrites seems to suggest that each carbonaceous chondrite group acquired its Mn/Cr ratio 4568 ± 1 Myr ago. This age is indistinguishable from the age of Ca-Al-rich inclusions (CAIs), which is considered to be the start of the solar system (t0). However, carbonaceous chondrites were not assembled until at least 1.5-5 Myr after t0, to judge by the 207Pb-206Pb and 26Al-26Mg ages of the chondrules within them, and by the fact that they were not melted by heat from the decay of 26Al. Presumably, therefore, these meteorites inherited their bulk Mn-Cr isochron from precursor materials which experienced Mn-Cr fractionation at t0. As a possible physical mechanism for how the isochron was established initially, and later inherited by the carbonaceous chondrites, we propose the rapid formation at t0 of planetesimals that were variably depleted in moderately volatile elements, and hence had variably low Mn/Cr. The planetesimals and the undepleted (high Mn/Cr) primitive dust from which they were made shared the same initial ε53Cr, and therefore evolved on an isochron. We suggest that later impact-disruption of the planetesimals produced dusty debris, which became mixed, in various proportions, with unprocessed (high Mn/Cr) dust before accreting to the carbonaceous chondrite parent bodies. With mixing in a closed system, the isochron was unchanged. We infer that some debris-rich material was converted to chondrules prior to accretion. The chondrules could have been formed by flash melting of the mixed dust, or could instead have been made directly by the impact splashing of molten planetesimals, or by condensation from impact-generated vapor plumes.  相似文献   

20.
Age-dated sediment cores from 4 remote lakes across California were analyzed for total Hg (HgT) concentration as a function of pre- and post-industrialization. Particle size, magnetic susceptibility and organic C and N, were measured to determine if the Hg concentration in sediment cores could be related to atmospheric deposition and/or watershed processes. Results indicate that (a) for each lake modern (1970–2004) HgT lake sediment concentrations have increased by an average factor of 5 times more than historic (pre-1850) HgT concentrations; (b) the ratio of modern to pre-industrial lake sediment HgT for these lakes are higher than estimated for other locations where atmospheric deposition is presumed to be the main source of Hg; (c) 2 of the 4 studied lakes demonstrated significant relationships between HgT concentrations and percentage organic material (r2 = 0.68 and p < 0.01; r2 = 0.67 and p < 0.01) whereas the other two indicated no significant relationship (r2 = 0.05 and p = 0.51; r2 = 0.12 and p = 0.36).  相似文献   

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