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Trace element abundances in L-chondrites determined by neutron activation analysis, and implications cosmothermometry
Chondrites elements fractionation in solar nebula starting from carbonaceous material
Eighteen achondrites and 4 terrestrial basalts (3 ocean ridge, 1 continental) were analyzed by radiochemical neutron activation analysis for Ag, Au, Bi, Br, Cd, Co, Cs, Cu, Ga, In, Ir, Rb, Se, Tl and Zn. Samples included 7 eucrites, 5 howardites, 2 nakhlites, 2 shergottites, an angrite, and an aubrite. Light and dark portions of the gas-rich meteorites Kapoeta and Pesyanoe were analyzed separately. Nakhlites and shergottites have volatile element abundances similar to those in ocean ridge basalts; eucrites, howardites, and angrites show greater depletions by an order of magnitude and less similar abundance patterns. In terms of a two-component model of planetary accretion, the parent planets contained the following percentages of low-temperature material: eucrites 0.8, nakhlites 38, shergottites 28. Shergottites may be genetically related to L-chondrites. The siderophile element pattern of achondrites resembles that of the moon, but with less extreme depletions.
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Radiochemical neutron activation is applied to the analysis of four C3V chondrites and three C3O chondrites for 17 trace elements (U, Re, Ir, Ni, Au, Sb, Ge, Ag, Rb, Cs, Bi, Tl, Br, Se, Te, In, and Cd). It is shown that both classes exhibit a typical chondritic step pattern, reflecting loss of volatiles during chondrule formation. It appears that the H2S/H2 ratio is the key variable to account for the condensation of chalcophile elements as a function of H2S. C3O's seem to have condensed in a region where enough metallic Fe was present to buffer the H2S pressure, whereas C3V's condensed in a more oxidized region where H2S was in excess. Accretion temperatures for both subclasses is determined. Sb and Au show variable depletion, presumably reflecting variable loss during chondrule formation.
An investigation involving the measurement of 17 trace elements in 4 ureilites was conducted with the objective to obtain information for the characterization of the two components of the ureilites. The groundmass of the mineral is an olivine-clinopyroxene rock which is presumably the residue left after partial melting of a more primitive precursor. This ultramafic rock is permeated by a network of veins containing diamond, graphite, nickel-iron, and primordial noble gases. Attention is given to the vein material, the origin of the vein material, the 'constant' siderophile component and ultramafic rock, and questions concerning the origin of ureilites.
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An investigation was conducted involving the determination of Os in 53 highland samples from the Apollo 14-17 missions. The Os/Ir ratio was found to remain essentially constant at 1.05 as Os and Ir abundances vary over four orders of magnitude. The Os-Au and the Os-Ni correlation in highland samples is presented in graphs. The graphs show that the majority of highland samples have Os/Au and Os/Ni ratios somewhat below the cosmic value. But there is no reason to attribute this trend to a loss of Os by local processes, because two other refractory siderophiles, Ir and Re, show exactly the same trend. Results on more than 150 analyzed highland samples show that meteoritic groups of low (Ir, Re, Os)/Au ratio are much more common at the Apollo landing sites than are groups of high ratio.
The cosmochemical and geochemical history of planetary material is reflected in relative and absolute abundances of two groups of trace elements; siderophiles and volatiles. Many of these elements can be determined at the required levels only by radiochemical neutron activation analysis. The abundance patterns of elements in chondritic meteorites result from condensation processes in the solar nebula. The composition of planetisimals which bombarded the moon is characterized from trace elements in lunar breccias, and is also related to nebula processes. Trace elements in anorthosites and basalts from earth and moon suggest that the moon is refractory-rich and volatile-poor relative to the earth.
Measurements of the compositions of 20 trace elements in the representative C2 chondrites Boriskino, Cold Bokkeveld, Erakot, Essebi, Haripura, Santa Cruz and Al Rais are reported. The contents of Ag, Au, Bi, Cd, Cs, Ge, In, Ir, Ni, Os, Pd, Rb, Re, Sb, Se, Sn, Te, Tl, U, and Zn were determined by radiochemical neutron activation analysis. The siderophile abundances of the C2 chondrites are found to be less uniform than those of other carbonaceous chondrites, while the C2R chondrite Al Rais is systematically lower in 12 volatiles than the C2M chondrites. Enrichment of Bi and Tl found in Erakot and Haripura indicate the possible presence of the late condensate mysterite. Volatile abundances are shown to agree with matrix contents for meteorites that have suffered little aqueous alteration, however to be 20-30% lower for the more altered meteorites. Finally, the decline of element abundance with volatility is shown to be consistent with the sigmoid curve explained by the two-component model.
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Predicting, responding to, or interpreting the chemical record preserved in debris derived from nuclear events can be challenging due to chemical fractionation. Chemical fractionation is where different species of the evolving radionuclide inventory segregate and/or are lost from the system over the timescales of debris formation. Both historic data and recent research suggest that the interaction and character of the local environment may exert controls on chemical fractionation by influencing the cooling and evolution of the associated fireball as well as the composition of the vapor term and resultant speciation. Prior to this work, an integrated platform permitting dynamic and concurrent consideration of physical and chemical evolution of early time post-detonation event environments did not exist. Our work merged historic data and experimental approaches to support development of a computational framework able to simulate fundamental processes (e.g., entrainment of local environment, oxidation chemistry, and cooling time scales) that may perturb the radionuclide inventory captured in post-detonation debris. Work with historic debris confirmed that entrained environmental material affect debris composition, structure, and radionuclide incorporation. Complementary work utilizing a readily controllable and tunable benchtop setup (a plasma flow reactor) simulated the late cooling of a nuclear fireball (e.g., T < 6000 K) and bounded the sensitivity of actinide speciation and particle size distribution to variations in oxygen concentration and cooling rates. Concurrent laser ablation and laser heating experiments were used to investigate the chemistry and physics of processes occurring in vaporized and/or rapidly heated actinides and other elements in the presence of oxygen. A more computationally efficient microphysical model was developed for predicting and evolving size distributions of particles forming from mixed vapor terms and simulating particle formation processes under a variety of extreme conditions. Continued study of historic nuclear event film confirmed that shockwave data and physics codes agree to within the uncertainty of the data. Good agreement was achieved for thermal emission from an airburst, however the paucity of low-temperature molecular opacity data for mixtures of air, bomb debris, entrained dirt, and water vapor complicate agreement for more elaborate scenarios. A multiphysics code (ALE3D) was modified to bring the necessary physics and chemistry, including these new data and insights, onto a single platform. Code development included improved initialization of large physical systems, modernization of chemistry capabilities, and modifications to enable inclusion of particle transport.
Chemical and physical heterogeneity in biomass feedstocks such as agricultural or forestry residues is due to substantial differences in plant tissue types. These differences can contribute significant challenges to handling, preprocessing, and conversion in biorefining processes. An understanding of this chemical and physical heterogeneity can be used to inform fractionation technologies that could facilitate more streamlined processing and potentially be employed to yield multiple co-product streams for a single feedstock. In this chapter, the motivation and scope of biomass fractionation is first outlined. Physical and chemical properties of biomass feedstocks, along with their distribution and diversity within plants, are next discussed with respect to how these differences can be exploited in a fractionation process. A summary of some of the key physical principles that allow for fractionation is next covered along with how these physical principles are exploited in equipment designs. Examples from the literature are briefly discussed that highlight how these approaches can be employed to achieve processing objectives. Several case studies on physical fractionation of corn stover and forestry residues are presented that illustrate how integrated fractionation processes could be employed. Lastly, prospects and potential economic drivers for adoption of biomass fractionation technologies are discussed.
Chemical data obtained by instrumental neutron activation analysis are reported for 30 elements in eight lunar soil size fractions from 370 to less than 2 microns, as well as petrology for five size fractions down to 40-10 microns in two Luna 24 soils. While the compositions of coarser fractions are similar to each other, they differ from the fractions smaller than 10 microns; these become increasingly feldspathic and enriched in large ion lithophile elements (LILE) with decreasing grain size. The high concentrations of the Ni, Au and Ir meteoritic indicator elements in these finer fractions are consistent with comminution by meteoritic impact. Size distributions, petrology and LILE patterns indicate that Luna 24 soils are less reworked than most lunar soils.
The reported chemical fractionation of a single isotope O-16 under simulated space conditions provides the first experimental proof for the hypothesis that the oxygen isotopic anomaly (and other similar anomalies) seen in meteorites is a product of chemical fractionation in interstellar or circumstellar space. Work proposed on this subject was discontinued because a peer review determined that such effects could not possibly exist and that continued support of this project would be a wasted effort. A bibliography is included of articles generated during research in this area.
Chemical fractionation processes are investigated with emphasis on selective single isotope fractionation in polyisotopic systems, particularly in oxygen. The related temperature parameters of meteoritic condensates and of their source medium are investigated by a thermometric method that is independent of assumptions regarding temperatures and pressures in the solar nebula. The crucial nonlinear chemical fractionation of O-16 was demonstrated experimentally. The effect was achieved in condensed CO2 formed from CO with C-12 O-16 selectively excited by H Ly alpha. The effect was verified by mass spectrometric measurements. The meteorite paleotemperature estimates were advanced from defining only thermal exposure to evaluating time and temperature independently. Grain temperatures at condensation of refractory inclusion materials are indicated to be less than 900 K in agreement with radiation temperature considerations and observations in circumstellar dust shells.
Zirconium and hafnium, a geochemically coherent pair of elements, are strongly fractionated in lunar rocks, as evidenced by a wide range of Zr/Hf mass ratios from 12 for the anorthosite 60015,65A to 50 for the KREEP breccia 14321. This may be explained in part by selective reduction of Zr(4+) to Zr(3+) and exclusion of the Zr(3+) from early crystallized Fe-Ti minerals.
A few unusual chondrules in the Mezoe-Madaras L3 chondrite contain the peralkaline mineral merrihueite, (K, Na)2(Fe, Mg)5Si12O30, formed by reaction of free silica in the chondrules with K, Na, Fe-rich nebular gas. Vapor fractionation was required to create chondrules poor in Al and rich in Si, and the fractionated condensate produced had to aggregate into protochondrules very promptly (on the order of hours or less) to prevent it from mixing with dust of more generalized composition in the nebula. The traditional paradigm for chondrule formation, involving a series of unrelated events (chemical fractionation of precursor dust; clumping of the dust; melting of the dust-clumps), is inadequate for making these chondrules. A rapid process, all stages of which are related, is required. We propose that this occurred during the cooling and contraction of the volume of hot gas created by a small transient high-energy event in the nebula, of unspecified nature. Microdroplets of silicate melt created by condensation from the cooling, contracting gas had velocity vectors directed toward the center of the volume. Coalescence occurred in the crowded central zone where the microdroplets converged. The Mezoe-Madaras merriihueite-bearing chondrules may have been formed by an atypically low-energy nebular event, which achieved the needed chemical fractionations by only partially vaporizing precursor dust. More commonplace chondrule types may have been created by the same basic process, but involving higher-energy events in which precursor dust was completely vaporized and recondensed.