Using stable isotopes in water to trace brine source and mobilization at WIPP: Preliminary results from halite fluid inclusions
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Eldridge, Daniel Lee↗
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Re-187 Os-187 Isotopic and Highly Siderophile Element Systematics of Group IVB Irons
Study of the magmatic iron meteorite groups permits constraints to be placed on the chemical and isotopic composition of parent bodies, and the timing of, and crystal-liquid fractionation processes involved in the crystallization of asteroidal cores. Here we examine Re-Os isotopic and trace elemental systematics of group IVB irons. Compared to most irons, the irons comprising this group are enriched in some of the most refractory siderophile elements, yet highly-depleted in most volatile siderophile elements. These characteristics have been attributed to processes such as high temperature condensation of precursor materials and oxidation in the parent body. Most recently it has been suggested that both processes may be involved in the chemical complexity of the group. Here, high precision isotopic and highly siderophile element (HSE) concentrations are used to further examine these possible origins, and the crystallization history of the group. In addition, we have begun to assess the possibility of relating certain ungrouped irons with major groups via multi-element, trace element modeling. In a companion abstract, the isotopic and trace element systematics of the ungrouped iron Tishomingo are compared with the IVB irons.
Honesto, J.↗
The Meteoritic Component in Impact Deposits
An important part of the history of impacts on Earth, and their influence on the terrestrial environment and biotic evolution, is the provenance of the impacting bolides. This will reflect the history of the large-body object flux in the inner solar system. The physical and chemical properties of projectiles, as well as their orbital evolution, has influenced the dynamics and the relative timing of impact events. Possible impact scenarios include random impacts by individual asteroids or comets, or clusters of impacts due to major collisions in the asteroid or Kuiper belts, or large perturbations of the Oort cloud of comets. Over the last several years, a combination of trace element, isotopic, and petrologic data have yielded significant insights into this impact history. The trace element chemistry of sediments, in particular the concentration of siderophiles (e.g., Ir), is a useful tool to detect impacts and provides supporting evidence for suspected impact deposits. However, siderophiles are not especially useful in distinguishing between types of projectiles. Interelement abundances of PGEs can distinguish a chondritic signature, but since most asteroids, and probably all comets are chondritic, these data do little to distinguish between chondritic source materials. Perhaps the most significant chemical argument used to constrain provenance, is that the total amount of Ir in the global Cretaceous-Tertiary (KT) boundary ejecta layer is considerably less than that expected by a low-velocity, 10 km asteroid impact and is most consistent with the impact of a high-velocity, low-Ir comet. Alternatively, much of the Ir may have been buried in the Chicxulub crater and/or ejected to escape velocity.
Kyte, Frank T.↗
Re-187-Os-187, Pt-190-Os-186 Isotopic and Highly Siderophile Element Systematics of Group IVA Irons
We have recently completed Re-187-Os-187 and Pt-190-Os-186 isotopic and elemental studies of the two largest magmatic iron meteorite groups, IIAB and IIIAB [1]. These studies revealed closed-system behavior of both isotopic systems, but complex trace element behavior for Re, Pt and Os in group IIIAB. Here we examine isotopic and trace elemental systematics of group IVA irons. The IVA irons are not as extensively fractionated as IIAB and IIIAB and their apparently less complex crystallization history may make for more robust interpretation of the relative partitioning behavior of Re, Pt and Os, as well as the other highly siderophile elements (HSE) measured here; Pd, Ru and Ir [e.g. 2]. An additional goal of our continuing research plan for iron meteorites is to assess the possibility of relating certain ungrouped irons with major groups via trace element modeling. Here, the isotopic and trace element systematics of the ungrouped irons Nedagolla and EET 83230 are compared with the IVA irons.
Walker, R. J.↗
The Effects of Experimentally Induced Zircon Annealing on Melt Inclusion-Zircon Geochemistry: A Case Study of Archean Zircon From the Barberton Complex
Crystalline melt inclusions (MIs) in Archean zircons can potentially constrain the evolution of magmatic processes. However, to obtain a homogeneous glassy MI representative of the parent melt, devitrified MIs must be heated at temperatures above the liquidus. Although, it is well known that radiation damaged domains in MI-host zircon undergo temperature-time dependent annealing, the effects of annealing on zircon stable isotope and trace element compositions has received less attention. In this study, we heated multiple aliquots of low-magnetism zircons with relatively low levels of radiation damage (Deff<9.6x1014 α-events/mg) from a 3.304 Ga tonalite gneiss xenolith from the Barberton greenstone belt (sample B87-18; Kamo and Davis, 1994) in an internally-heated pressure vessel at 0.4GPa and 1000–1200°C. Zircons were imaged by SEM (CL, BSE) to determine the zoning patterns around the MIs. The radiation damage preserved in the heated and unheated zircons was determined by measuring broadening of the 3(SiO4) Raman stretching band of zircon (FWHM). Oxygen isotope ratios (δ18O), OH/O ratios, and trace and rare earth element (TREE) concentrations were measured in the zircons and MIs using SIMS. The FWHM and Raman shift of the zircon 3(SiO4) band show a systematic increase of zircon crystallinity with increasing experimental temperature. Despite increasing crystallinity, the 3(SiO4) FWHM is not correlated with δ18O(Zrn) values in the heated or unheated zircons, suggesting that δ18O was not altered by laboratory heating in these low initial radiation damage zircons. FWHM and OH/O are positively correlated in both heated and unheated zircons. The unheated zircons have the largest FWHM and OH/O (OH/OMAX=3.5×10-4) suggesting that H2O was lost during experimental heating due to the progressive annealing of radiation-damaged domains in the zircons. Zircon TREE concentrations and FWHM values are not correlated despite the presence of TREE altered domains in both the heated and unheated zircons. Our results demonstrate that pre-experimental zircon TREE concentrations and δ18O(Zrn) remain intact during laboratory heating of crystalline MIs in zircon, while secondary H2O hosted in radiation damaged domains is partially lost. Thus, MIs in low initial radiation damage Archean zircon are a potentially viable tool for constraining melt compositions.
Joseph P. Gonzalez↗
Formation and Preservation of the Depleted and Enriched Shergottite Isotopic Reservoirs in a Convecting Martian Mantle
There is compelling isotopic and crater density evidence for geologically recent volcanism on Mars, in the last 100-200 million years and possibly in the last 50 million years. This volcanism is due to adiabatic decompression melting and thus requires some type of present-day convective upwelling in the martian mantle. On the other hand, martian meteorites preserve evidence for at least 3 distinct radiogenic isotopic reservoirs. Anomalies in short-lived isotopic systems (Sm-146, Nd-142, Hf-182, W-182) require that these reservoirs must have developed in the first 50 to 100 million years of Solar System history. The long-term preservation of chemically distinct reservoirs has sometimes been interpreted as evidence for the absence of mantle convection and convective mixing on Mars for most of martian history, a conclusion which is at odds with the evidence for young volcanism. This apparent paradox can be resolved by recognizing that a variety of processes, including both inefficient mantle mixing and geographic separation of isotopic reservoirs, may preserve isotopic heterogeneity on Mars in an actively convecting mantle. Here, we focus on the formation and preservation of the depleted and enriched isotopic and trace element reservoirs in the shergottites. In particular, we explore the possible roles of processes such as chemical diffusion and metasomatism in dikes and magma chambers for creating the isotopically enriched shergottites. We also consider processes that may preserve the enriched reservoir against convective mixing for most of martian history.
Kiefer, Walter S.↗
Processes involved in the formation of magnesian-suite plutonic rocks from the highlands of the Earth's Moon
The earliest evolution of the Moon likely included the formation of a magma ocean and the subsequent development of anorthositic flotation cumulates. This primary anorthositic crust was then intruded by mafic magmas which crystallized to form the lunar highlands magnesian suite. The present study is a compilation of petrologic, mineral-chemical, and geochemical information on all pristine magnesian-suite plutonic rocks and the interpretation of this data in light of 18 'new' samples. Of these 18 clasts taken from Apollo 14 breccias, 12 are probably pristine and include four dunites, two norites, four troctolites, and two anorthosites. Radiogenic isotopic whole rock data also are reported for one of the 'probably pristine' anorthositic troctolites, sample 14303,347. The relatively low Rb content and high Sm and Nd abundances of 14303,347 suggest that this cumulate rock was derived from a parental magma which had these chemical characteristics. Trace element, isotopic, and mineral-chemical data are used to interpret the total highlands magnesian suite as crustal precipitates of a primitive KREEP (possessing a K-, rare earth element (REE)-, and P-enriched chemical signature) basalt magma. This KREEP basalt was created by the mixing of ascending ultramafic melts from the lunar interior with urKREEP (the late, K-, REE-, and P-enriched residuum of the lunar magma ocean). A few samples of the magnesian suite with extremely elevated large-ion lithophile elements (5-10x other magnesian-suite rocks) cannot be explained by this model or any other model of autometasomatism, equilibrium crystallization, or 'local melt-pocket equilibrium' without recourse to an extremely large-ion lithophile element-enriched parent liquid. It is difficult to generate parental liquids which are 2-4 x higher in the REE than average lunar KREEP, unless the liquids are the basic complement of a liquid-liquid pair, i.e., the so-called 'REEP-fraction,' from the silicate liquid immiscibility of urKREEP. Scarce age information on lunar rocks suggests that magnesian-suite magmatism was initiated at progressively more recent time from the northeast to the southwest on the lunar nearside from 4.45 to 4.25 Ga.
Snyder, Gregory A.↗
Constraints on the development of the early continental crust from isotopic data
Aspects of the origin and development of the early (AE) continential crust are addressed by radiogenic isotope and trace element studies. The most important ones are: (1) at what time did the earliest continental crust form; (2) what was its composition; (3) by what processes did it grow and by what processes was it destroyed; (4) what were the rates of production and destruction as a function of time during this time period? Nd is isotopic data on the oldest terrestrial rocks indicate that the mantle at this time had already suffered substantial depletion in incompatible elements due to earlier continent forming events. Isotopic data on young volcanic rocks derived from the depleted mantle show no evidence of this early history. The observed isotopic patterns of Nd, Sr, Hf and Pb through time together with the presently observed age spectrum of crustal rocks are considered. These patterns can be modelled by a transport model in which the continental growth and destruction rates are allowed to vary as a function of time. It is suggest that the mass of the continents at 3.8 AE ago was about 25% of the current continental mass. However, due to the very high recycling rates obtained in the early Archean only a few percent of this crust has been preserved up to the present.
Jacobson, S. B.↗
New Martian Meteorite Is One of the Most Oxidized Found to Date
As of 2013, about 60 meteorites from the planet Mars have been found and are being studied. Each time a new Martian meteorite is found, a wealth of new information comes forward about the red planet. The most abundant type of Martian meteorite is a shergottite; its lithologies are broadly similar to those of Earth basalts and gabbros; i.e., crustal igneous rocks. The entire suite of shergottites is characterized by a range of trace element, isotopic ratio, and oxygen fugacity values that mainly reflect compositional variations of the Martian mantle from which these magmas came. A newly found shergottite, NWA 5298, was the focus of a study performed by scientists within the Astromaterials Research and Exploration Science (ARES) Directorate at the Johnson Space Center (JSC) in 2012. This sample was found in Morocco in 2008. Major element analyses were performed in the electron microprobe (EMP) laboratory of ARES at JSC, while the trace elements were measured at the University of Houston by laser inductively coupled plasma mass spectrometry (ICPMS). A detailed analysis of this stone revealed that this meteorite is a crystallized magma that comes from the enriched end of the shergottite spectrum; i.e., trace element enriched and oxidized. Its oxidation comes in part from its mantle source and from oxidation during the magma ascent. It represents a pristine magma that did not mix with any other magma or see crystal accumulation or crustal contamination on its way up to the Martian surface. NWA 5298 is therefore a direct, albeit evolved, melt from the Martian mantle and, for its lithology (basaltic shergottite), it represents the oxidized end of the shergottite suite. It is thus a unique sample that has provided an end-member composition for Martian magmas.
Hui, Hejiu↗
Molecular and Higher Precision Isotopic Measurements of the Mars Atmosphere and Subsurface Volatiles
In response to the question 'what to do next' at Mars we explore the value of a high precision in situ measurement of isotopic and trace gas constituents in the atmosphere combined with a similar analysis of gas extracted from near surface rocks and soils. The scientific goals are to advance our understanding of the evolution of the Martian atmosphere and to search for fossils of past geochemical conditions. One element of this program that ties directly to the goals of the Astrobiology Program will be a sensitive search for simple or complex organic molecules contained in the atmosphere and in the solid phase. The broad chemical and isotopic analysis planned insures that a highly successful program will be carried out even if no organics are detected. We will demonstrate that the technology to carry out this Program is presently in hand.
Mahaffy, P. R.↗
Magnesian anorthosites from the western highlands of the Moon: Isotope geochemistry and petrogenesis
Breccias from the Apollo 14 landing site have provided a wealth of information on the genesis of the lunar highlands. Various pristine rock-types have been discovered in relative abundance including rare ferroan anorthosites and alkali-suite and magnesian-suite rocks. Mineral-chemical and radiogenic isotopic data are reported here for a newly discovered Mg-suite anorthosite from Apollo 14, sample 14303,347. Meyer et al. reported U-Pb zircon analyses of Mg-suite highlands rocks from the western limb of the Moon. We have compiled these ages and generated a weighted average age of 4211 = 6 Ma; some 200 Ma younger than ferroan anorthosites. Utilizing this age for Mg-anorthosite 14303,347, our data results in an initial epsilon(sub Nd) value of -1.0 and initial Sr-87/Sr-86 of 0.69915. Based on trace-element, isotopic, and mineral-chemical data, the western highlands Mg-suite is interpreted to be crustal precipitates of a picritic magma, which assimilated KREEPy trapped liquid from upper-mantle cumulates during its transport to the crust.
Snyder, Gregory A.↗
Not So Rare Earth? New Developments in Understanding the Origin of the Earth and Moon
A widely accepted model for the origin of the Earth and Moon has been a somewhat specific giant impact scenario involving an impactor to proto-Earth mass ratio of 3:7, occurring 50-60 Ma after T(sub 0), when the Earth was only half accreted, with the majority of Earth's water then accreted after the main stage of growth, perhaps from comets. There have been many changes to this specific scenario, due to advances in isotopic and trace element geochemistry, more detailed, improved, and realistic giant impact and terrestrial planet accretion modeling, and consideration of terrestrial water sources other than high D/H comets. The current scenario is that the Earth accreted faster and differentiated quickly, the Moon-forming impact could have been mid to late in the accretion process, and water may have been present during accretion. These new developments have broadened the range of conditions required to make an Earth-Moon system, and suggests there may be many new fruitful avenues of research. There are also some classic and unresolved problems such as the significance of the identical O isotopic composition of the Earth and Moon, the depletion of volatiles on the lunar mantle relative to Earth's, the relative contribution of the impactor and proto-Earth to the Moon's mass, and the timing of Earth's possible atmospheric loss relative to the giant impact.
Righter, Kevin↗
Lipid accumulation in nitrogen and phosphorus-limited yeast is caused by less growth-related dilution
Oleaginous yeasts are used commercially to produce oleochemicals and hold potential also for biodiesel production. In response to nitrogen or phosphorous limitation, oleaginous yeasts accumulate lipids in the form of triacylglycerols. Previous work has investigated potential mechanisms by which nutrient limitation induces lipid biosynthesis without verifying whether lipid biosynthesis flux is actually enhanced. Here, in this work, we show, using 13C-glucose tracing, that in nitrogen or phosphorous limitation, lipid accumulation occurs without consistent increases in biosynthetic flux. Instead, the main driver of increased lipid pools is decreased growth-related dilution. This conclusion holds across two divergent oleaginous yeasts: Rhodotorula toruloides and Yarrowia lipolytica . Quantitative proteomics shows a substantial proteome reallocation in response to nitrogen and phosphorous limitation, with ribosomal proteins strongly downregulated, while lipid enzymes are preserved but not consistently upregulated in absolute quantity. Thus, nutrient limitation, rather than triggering greatly enhanced lipid synthesis, results in roughly sustained lipid enzyme levels and biosynthetic flux. Due to slower lipid dilution by cell division, this suffices to drive marked lipid accumulation.
09 BIOMASS FUELS↗
Maternal and embryonic trace element concentrations and stable isotope fractionation in the smalleye smooth-hound (Mustelus higmani)
Not Available
de Souza-Araujo, Juliana↗
Cu-, Co-, and Zn-Based Metal–Organic Framework-Derived Nanoporous Ion Emitters for Picogram Level Analysis of Actinides
Thermal ionization mass spectrometry (TIMS) is often regarded as the preferred technique for trace-level isotopic analysis of actinides owing to its high sensitivity and absence of carry-over effects. However, actinide sample utilization efficiency (SUE) is typically low (<0.05%) without the use of activators or specialized loading approaches which can yield SUEs of >5%. To this effect, we investigate a series of metal–organic framework (MOF)-based nanoporous ion emitters (nano-PIEs) that show enhanced ionization of actinides when used in TIMS loading. We study the impact of physical and chemical properties of MOFs on TIMS SUEs using two families of MOFs that can be synthesized under similar reaction conditions. The structural and chemical properties of these MOFs can be systematically modified one at a time while keeping other features the same. This allows us to strategically investigate their impact on SUEs. The first family of MOFs considered in this study is Zeolitic Imidazole Frameworks (ZIFs) which are made using 2 methyl-imidazole as an organic linker with zinc (ZIF-8) and cobalt (ZIF-67) as metal centers. Additionally, the effect of morphology was also studied using Zn-based ZIF-L with a 2-dimensional structure. The second family of MOFs was synthesized using benzene-1,3,5-tricarboxylate (BTC) with copper (Cu-BTC) and zinc (Zn-BTC) as the metal center. Among the MOFs tested, Cu-BTC showed the highest SUE with an average SUE of 0.27 ± 0.15%, followed closely by Zn-BTC (0.24 ± 0.10%), ZIF-8 (0.17 ± 0.10%), and trailed by the other MOFs. When the MOFs were pyrolyzed in N 2 before loading, an apparent increase in the SUE was observed with ZIF-8 and Cu-BTC showing average SUEs of 0.25 ± 0.08% and 0.34 ± 0.13%, respectively, with the highest measured SUE of 0.53% for pyrolyzed Cu-BTC. In conclusion, this observed increase in SUE by up to an order of magnitude compared to bare filaments demonstrates the efficacy and potential of MOF-derived nano-PIEs for TIMS application.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Rates and Reversibilities in Interconnected Reaction Networks
Mathematical relations prescribing unidirectional forward and reverse rates originally derived based on single-path reaction sequences do not apply to interconnected reaction networks. The presence of branches in reaction networks, leading to alternative stable products, decreases unidirectional rates in reference to those calculated by single-path functional forms, as shown by simulated isotopic exchange rates, but impacts the unidirectional forward and reverse rates equally such that the functional form of effective reversibility remains unchanged. Regardless of stoichiometric numbers and network connectivity, the application of the pseudo-steady-state hypothesis on reactive intermediates in conjunction with consideration of unidirectional rates toward the product of interest and all alternative stable products results in mathematical expressions that accurately reflect simulated isotopic exchange rates. Further analyses based on kinetic resistance, a property akin to electrical resistance, illustrate the manifestation of nodal resistances in addition to the single-path kinetic resistance for interconnected reaction networks. The generalized formalism for assessing rates and reversibilities in interconnected networks derived herein enables us to demonstrate that unidirectional rates cannot be assessed solely from effective reversibilities and net rates of generation of stable species in such networks. Furthermore, isotopic exchange rates, under the condition that each elementary step in the overall reaction sequence forms a unique reactive intermediate that is consumed solely by the subsequent step, can be utilized to determine unidirectional rates and can serve to validate postulated reaction pathways in highly interconnected reaction networks (e.g., CO x hydrogenation).
42 ENGINEERING↗
Isotopic and REE studies of lunar basalt 12038 - Implications for petrogenesis of aluminous mare basalts
Sr, Nd, and Sm isotopic studies of lunar basalt 12038, one of the so-called aluminous mare basalts, are reported. The evolution of the Sr and Nd isotopic compositions and the rare earth element (REE) abundances is successfully modeled within the framework of the model developed by Nyquist et al. (1977, 1979) for Apollo 12 olivine-pigeonite and ilmenite basalts. It is pointed out that the isotopic and trace element features of 12038 can by modeled as produced by partial melting of a cumulate mantle source which crystallized from a lunar magma ocean with a chondrite-normalized REE pattern of constant negative slope. Chondrite-normalized La/Yb is equal to 2.2 for this hypothetical magma ocean pattern.
Nyquist, L. E.↗
Trace element concentrations in the isotopically unique Allende inclusion, EK 1-4-1
The bulk sample and mineral separates of the isotopically unique Allende inclusion, EK 1-4-1, are analyzed by instrumental neutron activation for the concentrations of REE, Sc, Fe, Co, Cr, Na, and Ir, and REE concentrations were also determined by mass spectrometric isotope dilution for two density separates. Results show that the inclusion is enriched in light REE compared to heavy REE with a positive Yb anomaly, and has a high Cr concentration, both of which indicate group II affinity, although EK 1-4-1 is a coarse-grained group I inclusion. On the other hand, high Ir, and Sc, and low FeO and Co concentrations were found in the bulk inclusion, and low Na concentrations were found in mineral separates, which indicate an affinity to group I. In addition, for melilite and pyroxene fractions REE, Sc, Co, and Fe were determined to have distributions that were substantially different from those observed for normal Allende type B inclusions.
Nagasawa, H.↗