Major element composition of Georgia tektites.
Major element analysis of chemical composition of Georgia tektite
TEKTITE↗
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Present status of the icy conglomerate model
A brief history of the ice comglomerate model (ICM) of the nuclei of comets is presented. Emphasis is given to the usefulness if the ICM in describing cometary behavior despite its vagueness with respect to the chemical composition and physical structure of cometry nuclei. Alternative theories concerning the relationship between the chemical composition of cometary ices and comet behavior are briefly discussed.
Whipple, F. L.↗
Effect of Thermal Oxidation on the Structure, Surface Texturing, and Microstructure Evolution in Nanocrystalline Ga-O-N Films
An extensive examination of the nanoscale, crystallographic growth dynamics of the system, which is impacted by the thermal energy given to the GaN, is carried out to derive a deeper understanding of the growth kinetics, morphology and microstructure evolution, chemical bonding, and optical properties of Ga-O-N films. Thermal annealing of GaN films is performed in the temperature range of 900–1200 °C. Crystal structure, phase formation, chemical composition, surface morphology, and microstructure evolution of Ga-O-N films are investigated as a function of temperature. Increasing temperature induces surface oxidation, which results in the formation of stable β-Ga2O3 phase in the GaN matrix, where the overall film composition evolves from nitride (GaN) to oxynitride (Ga-O-N). While GaN surfaces are smooth, planar, and featureless, oxidation induced granular-to-rod shaped morphology evolution is seen with increasing temperature to 1200 °C. The considerable texturing and stability of the nanocrystalline Ga-O-N on Si substrates can be attributed to the surface and interface driven modification because of thermal treatment. Corroborating with structure and chemical changes, Raman spectroscopic analyses also indicate that the chemical bonding evolution progresses from fully Ga-N bonds to Ga-O-N. While the GaN oxidation process starts with the formation of β-Ga 2 O 3 at an annealing temperature of 1000 °C, higher annealing temperatures induce structural distortion with the potential formation of Ga-O-N bonds. The structure-phase-chemical composition correlation, which will be useful for nanocrystalline materials for selective optoelectronic applications, is established in Ga-O-N films made by thermal treatment of GaN.
36 MATERIALS SCIENCE↗
Electrochemical Reactivity and Passivation of Silicon Thin-Film Electrodes in Organic Carbonate Electrolytes
This work focuses on the mechanisms of interfacial processes at the surface of amorphous silicon thin-film electrodes in organic carbonate electrolytes to unveil the origins of the inherent nonpassivating behavior of silicon anodes in Li-ion batteries. Attenuated total reflection Fourier-transform infrared spectroscopy, X-ray absorption spectroscopy, and infrared near-field scanning optical microscopy were used to investigate the formation, evolution, and chemical composition of the surface layer formed on Si upon cycling. Herein, we found that the chemical composition and thickness of the solid/electrolyte interphase (SEI) layer continuously change during the charging/discharging cycles. This SEI layer “breathing” effect is directly related to the formation of lithium ethylene dicarbonate (LiEDC) and LiPF6 salt decomposition products during silicon lithiation and their subsequent disappearance upon delithiation. Furthermore, the detected appearance and disappearance of LiEDC and LiPF6 decomposition compounds in the SEI layer are directly linked with the observed interfacial instability and poor passivating behavior of the silicon anode.
25 ENERGY STORAGE↗
Two- and three-layer models of Uranus
Simple two-layer models of Uranus with rocky core and polytropic envelope satisfying exactly the observed mass, radius and the gravitational moments are presented. The models show that the value of the fourth order zonal harmonic is less than about -38 x 10 to the -6th, while J(6) is roughly 10 to the -6th. More elaborate three-layer models fail to satisfy the observational constraints of the ice/rock ratio and/or of the rotation period. It is concluded that three-layer models with uniform chemical composition in each layer may be too restrictive. More realistic models should account for variable chemical composition within each layer.
Horedt, G. P.↗
Buried Porous Silicon-Germanium Layers in Monocrystalline Silicon Lattices
Monocrystalline semiconductor lattices with a buried porous semiconductor layer having different chemical composition is discussed and monocrystalline semiconductor superlattices with a buried porous semiconductor layers having different chemical composition than that of its monocrystalline semiconductor superlattice are discussed. Lattices of alternating layers of monocrystalline silicon and porous silicon-germanium have been produced. These single crystal lattices have been fabricated by epitaxial growth of Si and Si-Ge layers followed by patterning into mesa structures. The mesa structures are strain etched resulting in porosification of the Si-Ge layers with a minor amount of porosification of the monocrystalline Si layers. Thicker Si-Ge layers produced in a similar manner emitted visible light at room temperature.
Fathauer, Robert W.↗
Chemical evolution in spiral and irregular galaxies
A brief review of models of chemical evolution of the interstellar medium in our galaxy and other galaxies is presented. These models predict the time variation and radial dependence of chemical composition in the gas as function of the input parameters; initial mass function, stellar birth rate, chemical composition of mass lost by stars during their evolution (yields), and the existence of large scale mass flows, like infall from the halo, outflow to the intergalactic medium or radial flows within a galaxy. At present there is a considerable wealth of observational data on the composition of HII regions in spiral and irregular galaxies to constrain the models. Comparisons are made between theory and the observed physical conditions. In particular, studies of helium, carbon, nitrogen and oxygen abundances are reviewed. In many molecular clouds the information we have on the amount of H2 is derived from the observed CO column density, and a standard CO/H2 ratio derived for the solar neighborhood. Chemical evolution models and the observed variations in O/H and N/O values, point out the need to include these results in a CO/H2 relation that should be, at least, a function of the O/H ratio. This aspect is also discussed.
Torres-Peimbert, S.↗
Melting of the Primitive Mercurian Mantle, Insights into the Origin of Its Surface Composition
Recent findings of the MESSENGER mission on Mercury have brought new evidence for its reducing nature, widespread volcanism and surface compositional heteregeneity. MESSENGER also provided major elemental ratios of its surface that can be used to infer large-scale differentiation processes and the thermal history of the planet. Mercury is known as being very reduced, with very low Fe-content and high S and alkali contents on its surface. Its bulk composition is therefore likely close to EH enstatite chondrites. In order to elucidate the origin of the chemical diversity of Mercury's surface, we determined the melting properties of EH enstatite chondrites, at pressures between 1 bar and 3 GPa and oxygen fugacity of IW-3 to IW-5, using piston-cylinder experiments, combined with a previous study on EH4 melting at 1 bar. We found that the presence of Ca-rich sulfide melts induces significant decrease of Ca-content in silicate melts at low pressure and low degree of melting (F). Also at pressures lower than 3 GPa, the SiO2-content decreases with F, while it increases at 3 GPa. This is likely due to the chemical composition of the bulk silicate which has a (Mg+Fe+Ca)/Si ratio very close to 1 and to the change from incongruent to congruent melting of enstatite. We then tested whether the various chemical compositions of Mercury's surface can result from mixing between two melting products of EH chondrites. We found that the majority of the geochemical provinces of Mercury's surface can be explained by mixing of two melts, with the exception of the High-Al plains that require an Al-rich source. Our findings indicate that Mercury's surface could have been produced by polybaric melting of a relatively primitive mantle.
Boujibar, A.↗
Characterization of Tank 11H Samples from Tank Closure Cesium Removal (TCCR) Batch 3 - Intermediate and Final Samples
Savannah River Remediation (SRR) is currently operating the Tank Closure Cesium Removal (TCCR) process to remove 137 Cs from tank waste supernate using an ion exchange process. The TCCR unit processes dissolved salt from Tank 10H through a series of ion exchange columns containing crystalline silicotitanate (CST) and the effluent is then discharged to Tank 11H. Four interim samples pulled from Tank 11H during and just after the completion of processing of Batch 3 through the TCCR process have been analyzed for 137 Cs activity and density. The 137 Cs activity was found to decrease with each subsequent sample, which is consistent with the addition of decontaminated solution to Tank 11H. When compared to the expected composition from mixing the Tank 10H Batch 3 feed with the material already present in Tank 11H, the bulk chemical composition was as expected. A corrosion control sample collected from Tank 11H in June 2020 showed changes in the chemical composition and 137 Cs activity when compared to the composition measured at the end of Batch 2 processing. As there were no additions made to the tank during this period, these changes were attributed to leaching of the solids present in Tank 11H. Additional analyses of the 4 th interim sample are pending and will be documented in a revision to this report.
11H↗
Characterization of Tank 11H samples from tank closure cesium removal (TCCR) Batch 3 - intermediate and final samples
Savannah River Remediation (SRR) is currently operating the Tank Closure Cesium Removal (TCCR) process to remove 137 Cs from tank waste supernate using an ion exchange process. The TCCR unit processes dissolved salt from Tank 10H through a series of ion exchange columns containing crystalline silicotitanate (CST) and the effluent is then discharged to Tank 11H. Four interim samples pulled from Tank 11H during and just after the completion of processing of Batch 3 through the TCCR process have been analyzed for 137 Cs activity and density. The 137 Cs activity was found to decrease with each subsequent sample, which is consistent with the addition of decontaminated solution to Tank 11H. When compared to the expected composition from mixing the Tank 10H Batch 3 feed with the material already present in Tank 11H, the bulk chemical composition was as expected. A corrosion control sample collected from Tank 11H in June 2020 showed changes in the chemical composition and 137 Cs activity when compared to the composition measured at the end of Batch 2 processing. As there were no additions made to the tank during this period, these changes were attributed to leaching of the solids present in Tank 11H. Revision 1 of this report contains additional analyses of the fourth interim sample including inductively coupled plasma – mass spectrometry (ICP-MS) results and activities of other radionuclides. These results are consistent with the previously reported results, showing leaching from the Tank 11H heel. Notably, the 90 Sr activity was about 2.7x higher than calculated from a mixture of the original Tank 11H supernate and the Tank 10H supernate as treated by TCCR, suggesting additional leaching of Sr from the Tank 11H heel solids. In addition, Revision 1 includes analysis results for the Batch 3 Post-Production surface and variable depth samples collected in October of 2020. The Post-Production surface sample was similar in composition to the fourth interim surface sample, except for the increased Cs-137 and oxalate concentrations that were presumably associated with leaching of the Tank 11H heel solids.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Investigation of Magmatic Activities on Early Mars Using Igneous Mineral Chemistry in Gale Crater, Mars
One objective of rover missions is exploring the geological context of the surroundings. Over the years, igneous petrology and sedimentology have been disconnected, the first investigating magmatic processes and volcanic activities, and the second seeking environmental conditions in the past and assessing the habitability of the planet. Although different, one is related to the other: igneous rocks are altered and broken down, leading to the formation of sedimentary rocks, which can in turn be used to back out the nature of their magmatic source. The Curiosity rover that landed in the 3.7 Gyr old impact crater Gale is traveling through sedimentary rocks. About fifty float rocks have been observed, and several of them with ambiguous texture and composition have been classified as igneous or sedimentary depending on studies such as Jake_M. The composition of several unambiguous igneous rocks has been analyzed [4- 6] but their heterogeneity at a larger instrumental (measurement size < 2 cm) scale prevents the measurement of a bulk composition as performed on Earth. An original approach avoiding these two last issues is to consider igneous mineral chemistry analyzed within igneous and sedimentary rocks to assess magmatic processes that could have formed them. Most Curiosity data are used to explore ancient environmental conditions, and a significant number of compositional analyses are under-explored for constraining magmatic activities. We will present how we can make use of sedimentary data for investigating igneous processes in the vicinity of Gale crater. Geological Context: We focus on the first 750 martian days, corresponding to measurements in a coherent lacustrine sedimentary unit called Bradbury, because all sedimentary rocks were sourced from the same watershed and appear to have a consistent source with minimal alteration [2-3]. Igneous detrital minerals including feldspar and pyroxene, are observed in sedimentary rocks. Monte Carlo models showed that minimal cation loss is observed based on the composition of all Bradbury rocks, implying negligible weathering [3]. Although clay minerals are detected in few rocks [7], chemical compositions of rocks can be explained by a mixture of primary igneous minerals [3]. Variation of composition within Bradbury rocks can be explained by mineral sorting and one distinct source component. While a common magmatic source is suggested, Bradbury sediments likely come from several volcanic eruptions from a single magmatic chamber [9- 10]. The occurrence of alkali minerals like sanidine and K-rich rocks throughout Bradbury supports the presence of a potassic component, likely trachytic, while plagioclase and a mafic composition suggest a basaltic component [8-9]. Instruments: Mineral chemistry can be estimated by three instruments onboard Curiosity. The CheMin instrument enables detection of mineral assemblages using X-ray diffraction (XRD). Using Rietveld refinement, each mineral is identified according to their 1D XRD pattern [11]. Note that distinction between pyroxene minerals is challenging with the CheMin instrument due to overlapping peaks on XRD patterns and low angular resolution of the instrument [12]. Then, using least square regression and optimization algorithms based on unit-cell parameters, mineral chemistry has been estimated by [11]. Plagioclase composition has been estimated using the NaAlSi3O8- CaAl2Si2O8 system and alkali feldspar is based on the NaAlSi3O8-KAlSi3O8 system (stars in Fig.1). Two mudstone samples (John Klein and Cumberland) and one sandstone sample (Windjana) were analyzed by CheMin at Yellowknife Bay and Kimberley, respectively. Figure 1. Ternary diagrams of feldspars (top) and pyroxene (bottom) quadrilateral. Stars correspond to CheMin composition and the gray patches to ChemCam composition. The colored dots are the composition of feldspar and pyroxene that crystallized during fractional crystallization at FMQ+1 of a melt extracted at distinct melting degree during the adiabatic ascent of a primitive mantle composition, without any water (left panels) and with 0.5 wt.% of water (right panels) at distinct pressure. The ChemCam instrument enables the analysis of the chemical compositions of rocks at hundreds of micrometer scale (350-550 μm) using laser induced breakdown spectroscopy (LIBS), which may provide the composition of minerals when they are larger than the beam spot (>550 μm) [13]. Within >5000 LIBS points, we performed a typical stoichiometric filtering allowing us to distinguish 56 feldspar and 10 pyroxene mineral compositions (grey patches in Fig. 1). Finally, the Alpha Particle X-ray Spectrometer (APXS) analyzes the composition of rocks with a 1.6 cm diameter spot size. Monte Carlo mass balance modeling allowed [3] to decipher a feldspar range varying between An30 and An40 (Fig. 1). Discussion: Although there could be a more complex history and other ways to form the whole compositional range of igneous minerals analyzed within the Bradbury formation, we are presenting here simple magmatic pathways commonly occurring on Earth using the thermodynamical softwares pMELTS and rhyoliteMELTS [14]. The objective is to find reasonable igneous processes that produce minerals that parallel the compositions of feldspar and pyroxene analyzed by the Curiosity rover. As commonly observed for mid-ocean ridge basalts, the adiabatic ascent of a primitive mantle composition [15] partially melting at 2 GPa has been modeled, followed by the extraction of a liquid at distinct degrees of partial melting, which undergoes fractional crystallization at an oxygen fugacity +1 log unit above the fayalite-magnetite-quartz (FMQ) buffer within the crust (0.02-0.4 GPa) with H2O = 0- 0.5 wt. %. These latter conditions correspond to those recorded within igneous clasts from the Noachian martian breccia NWA 7034 and paired and within Gale igneous rocks (colored dots in Fig. 1) [16-17]. To check the reliability of these 2-step models, we also tested fractional crystallization at similar conditions (FMQ+1; P=0.02-0.4 GPa; H2O = 0-0.5 wt. %) of starting compositions corresponding to that of magmas with distinct melting degrees obtained from isobaric experiments at 2 GPa [18]. Mineral compositions obtained from both models are similar. As shown on Fig. 1, the whole range of observed feldspar compositions cannot be reproduced by fractionation of one magma only. Indeed, while alkali feldspar and Na-plagioclase likely crystallized from fractional crystallization of a low-degree melt (here <15%), plagioclase and pyroxene can only be formed by fractional crystallization of a higher degree melt (here >19%). The corresponding liquid descent lines are broadly in agreement with compositions estimated by ChemCam corresponding to float igneous rocks (Fig. 2) [4-6]. Figure 2. Silica versus alkali content. Lines show the liquid lines of descent from magmas with distinct degrees of melting. Gray patches represents the composition of Gale igneous rocks [4-6]. Trachytic to rhyolitic magmas crystallize alkali feldspar, and andesite to dacite magmas likely form plagioclase. Therefore, at least two starting magmas at distinct melting degrees, which could easily come from a single mantle source, are necessary to explain the whole compositional range of feldspar and pyroxene analyzed within Bradbury rocks. Conclusion: Because rocks from the Bradbury formation are likely originating from the same magmatic source with minimal weathering as supported by several studies using different approaches, igneous mineral chemistry analyzed by CheMin and ChemCam allows us to back out reasonable magmatic pathways that could have crystallized them. Fractional crystallization of at least two starting magmas originating from distinct melting degrees of a single mantle source can explain the whole range of feldspar and pyroxene composition. Both alkaline and sub-alkaline liquids can be produced, with compositions corresponding to those of the igneous rocks analyzed by ChemCam within the Bradbury formation, highlighting the complexity of Mars magmatism.
Payre, V.↗
The Post‐Perovskite Transition in Fe‐ and Al‐Bearing Bridgmanite: Effects on Seismic Observables
Abstract The primary phase of the Earth’s lower mantle, (Al, Fe)‐bearing bridgmanite, transitions to the post‐perovskite (PPv) phase at Earth’s deep mantle conditions. Despite extensive experimental and ab initio investigations, there are still important aspects of this transformation that need clarification. Here, we address this transition in (Al 3+ , Fe 3+ )‐, (Al 3+ )‐, (Fe 2+ )‐, and (Fe 3+ )‐bearing bridgmanite using ab initio calculations and validate our results against experiments on similar compositions. Consistent with experiments, our results show that the onset transition pressure and the width of the two‐phase region depend distinctly on the chemical composition: (a) Fe 3+ ‐, Al 3+ ‐, or (Al 3+ , Fe 3+ )‐alloying increases the transition pressure, while Fe 2+ ‐alloying has the opposite effect; (b) in the absence of coexisting phases, the pressure‐depth range of the Pv‐PPv transition is likely too broad to cause a sharp D” discontinuity (<30 km); (c) the average Clapeyron slope of the two‐phase regions are consistent with previous measurements, calculations in MgSiO 3 , and inferences from seismic data. In addition, (d) we observe a softening of the bulk modulus in the two‐phase region. The consistency between our results and experiments gives us the confidence to proceed and examine this transition in aggregates with different compositions computationally, which will be fundamental for resolving the most likely chemical composition of the D" region by analyses of tomographic images.
Geochemistry & Geophysics↗
New insights into the mechanism governing the elasticity of calcium silicate hydrate gels exposed to high temperature: A molecular dynamics study
When exposed to fire, the integrity of cement-based materials is governed by thermally-induced changes in the mechanical properties of their binding phase, i.e., the calcium–silicate–hydrate (C–S–H) gel. However, the effect of temperature on the structure, density, and mechanical properties of C–S–H remains only partially known. Here, based on reactive molecular dynamics simulations, we reveal the nature of thermally-induced damage in C–S–H gels. In general, we show that, at the atomic scale, exposure to high temperature results in partial dehydration, volumetric shrinkage, disordering, and stiffening in the C–S–H grains. However, we show that the thermal response of C–S–H strongly depends on its chemical composition, wherein C–S–H systems associated with lower Ca/Si molar ratios are able to undergo higher temperatures before amorphization. Based on these results, we demonstrate that the stiffness of C–S–H gels (i.e., including porosity—as probed by nanoindentation) is governed by a competition between the stiffening of the grains and the decrease in packing density—wherein the latter eventually become predominant.
36 MATERIALS SCIENCE↗
Computer Program for Calculation of Complex Chemical Equilibrium Compositions, Rocket Performance, Incident and Reflected Shocks, and Chapman-Jouguet Detonations. Interim Revision, March 1976
A detailed description of the equations and computer program for computations involving chemical equilibria in complex systems is given. A free-energy minimization technique is used. The program permits calculations such as (1) chemical equilibrium for assigned thermodynamic states (T,P), (H,P), (S,P), (T,V), (U,V), or (S,V), (2) theoretical rocket performance for both equilibrium and frozen compositions during expansion, (3) incident and reflected shock properties, and (4) Chapman-Jouguet detonation properties. The program considers condensed species as well as gaseous species.
Sanford Gordon↗
Systematic characterization of unknown compounds via dimensionality reduction of time series
Analysis of ambient aerosols provides valuable insight into particle sources and formation chemistry. However, due to the complexity of atmospheric data and the dynamic nature of aerosol composition, a substantial fraction of data often become discarded by conventional analysis methods. Furthermore, a large fraction of chemical species within those data are unidentifiable due to a lack of matching spectral information, resulting in suboptimal characterization of chemical composition. Previous work has demonstrated techniques for cataloging analytes in a chromatographic dataset by deconvolution of mass spectra, but integration of these analytes throughout a large dataset remains time consuming. Here, we present a method to automatically identify an ion for quantitation for single-ion chromatogram based peak fitting and integration, enabling comprehensive integration of analytes with minimal user interaction. The resulting time series are clustered with a machine-learning based dimensionality reduction technique to systematically investigate the underlying characteristics of the categorized analytes and gain new insights into the chemical composition and physicochemical properties of the unidentifiable analytes. We apply these methods to existing atmospheric datasets collected in Manacapuru, Brazil during the GoAmazon2014/5 campaign to identify new analytes and interpret their variability and transformations in the atmosphere. The analysis results generate 408 time series from cataloged analytes of interest, and the clustering of those time series with spherical k-means results in 8 distinct clusters. We find the analytes form clusters based on their distinct physicochemical properties, demonstrating the method’s ability to systematically identify and selectively filter contaminants and instrumental analytes and characterize the unidentifiable analytes.
54 ENVIRONMENTAL SCIENCES↗
A Comparison of Solid Electrolyte Interphase Formation and Evolution on Highly Oriented Pyrolytic and Disordered Graphite Negative Electrodes in Lithium–Ion Batteries
The presence and stability of solid electrolyte interphase (SEI) on graphitic electrodes is vital to the performance of lithium-ion batteries (LIBs). However, the formation and evolution of SEI remain the least understood area in LIBs due to its dynamic nature, complexity in chemical composition, heterogeneity in morphology, as well as lack of reliable in situ/operando techniques for accurate characterization. In addition, chemical composition and morphology of SEI are not only affected by the choice of electrolyte, but also by the nature of the electrode surface. While introduction of defects into graphitic electrodes has promoted their electrochemical properties, how such structural defects influence SEI formation and evolution remains an open question. In this work, utilizing nondestructive operando electrochemical atomic force microscopy (EChem-AFM) the dynamic SEI formation and evolution on a pair of representative graphitic materials with and without defects, namely, highly oriented pyrolytic and disordered graphite electrodes, are systematically monitored and compared. Complementary to the characterization of SEI topographical and mechanical changes during electrochemical cycling by EChem-AFM, chemical analysis and theoretical calculations are conducted to provide mechanistic insights underlying SEI formation and evolution. The results provide guidance to engineer functional SEIs through design of carbon materials with defects for LIBs and beyond.
25 ENERGY STORAGE↗
PM2.5 Active Aerosol Collection Field Campaign Report
The long-range transport of aerosols can affect local air quality as well as contribute elements and constituents to mountain watersheds that have potentially positive (e.g., nitrate) and negative (e.g., heavy metals) effects to the local ecosystem. Isotopic analysis of aerosols can be a powerful tool for deconvolving the relative contributions of far-distant and local sources to the composition of collected aerosols. Our field campaign involved the week-long collection of PM2.5 (i.e., particulate matter with an aerodynamic diameter of about 2.5 microns) aerosols on filters, which were returned to the laboratories at Lawrence Berkeley National Laboratory (LBNL) for analysis. The sampling sites were located at the Gothic, Colorado Surface Atmosphere Integrated Field Laboratory (SAIL) Atmospheric Radiation Measurement (ARM) and the Mt. Crested Butte, Colorado SAIL ARM sites. The original intention was to measure the lead (Pb) and strontium (Sr) isotopic compositions of the collected aerosols at high precision to provide constraints on source portioning and attribution, as well as analyze the chemical compositions and nitrogen and carbon isotopic compositions. However, severe blank issues arose that prevented the planned isotopic analyses of Sr, Pb, C, and N and severely affected the analyses of the bulk chemical compositions of the collected aerosols, resulting in the failure of the study. The issue is described in Section 2.0.
54 ENVIRONMENTAL SCIENCES↗
LABQ3: Bayesian method for quantification of mineral compositions and nano-scale elemental mapping of 3D synchrotron XCT data
Quantitative analysis of mineral compositions is essential in understanding geochemical, mineralogical and environmental processes. Fine-resolution 3D imaging is widely done using synchrotron X-ray computed tomography (XCT), but existing analyses are limited to visualization and segmentation. This paper presents a new method, Linear Attenuation Bayesian Quantitative 3D-mapper (LABQ3), based on the linearity of X-ray attenuation with respect to elemental concentrations. To address the random variability in attenuation measurements, LABQ3 employs Bayesian decision theory to minimize classification error, using reference attenuation distributions from scans of pure mineral standards. To demonstrate LABQ3 and test its performance, we studied precipitated carbonate samples. XCT scans were done at multiple energies using the transmission X-ray microscope (TXM) at beamline 32-ID-C of the Advanced Photon Source at Argonne National Laboratory. The reconstructed 3D images have a voxel size of 20 nm. Analyses revealed rich nano-scale compositional heterogeneity within individual particles. A mixture of calcium and cadmium produced an overall stoichiometric composition of (Ca 0.78 ,Cd 0.22 )CO 3 , with some voxels containing nearly pure CdCO 3 . The addition of zinc led to an overall stoichiometric composition of 33% Ca, 28% Cd, 39% Zn, with a nearly pure CaCO 3 core and compositional zonation through the rim. These compositional gradients are related to temporal sequences of carbonate mineral formation where Cd precipitated at the beginning in (Ca,Cd)CO 3 , while Cd and Zn precipitated at the end in (Ca, Cd,Zn)CO 3 . Results differ from bulk analyses using Inductively Coupled Plasma-Mass Spectrometry (ICP-MS), showing that LABQ3 provides particle-specific insights. LABQ3 distinguishes itself by quantifying chemical compositions along a continuum, making it different from XCT analyses based on segmentation. LABQ3 allows simultaneous acquisition of morphology and chemical composition in 3D, facilitating the interpretation of chemical gradients of trace elements, quantification of solid solution compositions, inferences about temporal sequences of mineral precipitation, and addressing other concerns about solid-phase chemistry.
58 GEOSCIENCES↗