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At least 541 records · Page 30

Compatibility of Type 304H Stainless Steel in Static Molten FLiBe for Inertial Confinement Fusion Reactors: Role of Impurities and Redox Control

Molten fluoride salts, such as FLiBe (LiF-BeF2), are promising candidates for tritium breeding and heat transfer in fusion reactors, but corrosion of structural materials remains a major challenge. This study investigates the corrosion behavior of austenitic stainless steel 304H in purified and NiF2-containing FLiBe at 500°C and 600°C, focusing on the effects of impurities and redox control. Exposure to purified FLiBe resulted in the concurrent depletion of Cr, Mn, and Fe, with corrosion at 500 °C dominated by the combined oxide formation and elemental dissolution, while at 600°C elemental depletion was predominant. The addition of a controlled NiF2 impurity significantly accelerated corrosion at both temperatures, demonstrating the sensitivity of 304H to the salt redox state. Beryllium additions were effective in mitigating corrosion for both baseline and NiF2-containing FLiBe; minimal depletion of Cr, Mn, and Fe occurred with Be additions as low as 2.5 mg (147 wppm), and no NiBe intermetallics formed at 5 mg (294 wppm), indicating that small Be inventories can provide substantial protection without deleterious phase formation. Thermodynamic equilibrium and coupled thermodynamic-kinetic analyses at the salt-alloy interface suggested low corrosion rates in systems with limited hydrogen fluoride (HF) generation, highlighting the importance of salt redox control. Estimates for a Be addition rate were calculated for the HYLIFE-II fusion reactor that can mitigate corrosion-induced degradation, assuming complete conversion of tritium to tritium fluoride (TF). Overall, 304H shows reasonable compatibility with FLiBe under optimized redox conditions. These results provide quantitative guidance for material selection and salt management in fusion blanket and heat exchanger systems and motivate validation under flowing, nonisothermal, and irradiated conditions.

Pillai, Rishi [ORNL] (ORCID:0000000243688197)↗

Dissolution and reduction of magnetite by bacteria

Magnetite (Fe3O4) is an iron oxide of mixed oxidation state [Fe(II), Fe(III)] that contributes largely to geomagnetism and plays a significant role in diagenesis in marine and freshwater sediments. Magnetic data are the primary evidence for ocean floor spreading and accurate interpretation of the sedimentary magnetic record depends on an understanding of the conditions under which magnetite is stable. Though chemical reduction of magnetite by dissolved sulfide is well known, biological reduction has not been considered likely based upon thermodynamic considerations. This study shows that marine and freshwater strains of the bacterium Shewanella putrefaciens are capable of the rapid dissolution and reduction of magnetite, converting millimolar amounts to soluble Fe(II)in a few days at room temperature. Conditions under which magnetite reduction is optimal (pH 5-6, 22-37 degrees C) are consistent with an enzymatic process and not with simple chemical reduction. Magnetite reduction requires viable cells and cell contact, and it appears to be coupled to electron transport and growth. In a minimal medium with formate or lactate as the electron donor, more than 10 times the amount of magnetite was reduced over no carbon controls. These data suggest that magnetite reduction is coupled to carbon metabolism in S. putrefaciens. Bacterial reduction rates of magnetite are of the same order of magnitude as those estimated for reduction by sulfide. If such remobilization of magnetite occurs in nature, it could have a major impact on sediment magnetism and diagenesis.

Non-NASA Center↗

Comprehensive Insights into Nucleation, Autocatalytic Growth, and Stripping Efficiency for Lithium Plating in Full Cells

Synchrotron high-energy X-ray diffraction is used to enable nondestructive detection and quantification of heterogeneous lithium plating in working batteries. In this study a LiNi 0.5 Mn 0.3 Co 0.2 O 2 /graphite pouch cell was operated under 6C fast-charge rate for greater than 1200 cycles. The magnitude and spatial distribution of lithium plating, lithium stripping, and the effect of metallic lithium deposition on lithium intercalation into graphite were quantified. Fully intercalated graphite (LiC 6 ) was detected after discharge with a lateral distribution closely correlated with lithium plating, which can be used as a higher-sensitivity indicator for lithium plating. Over an extended cycle life, the overall metallic lithium concentration followed a sigmoidal curve indicating two-stage continuous nucleation and autocatalytic growth. The lithium stripping efficiency underwent an exponential decay as a function of cycle life as the buildup of metallic lithium hindered the efficient dissolution back into the electrolyte. The findings provide direct insights into the characteristics of lithium plating and stripping under realistic fast-charge conditions.

25 ENERGY STORAGE↗

Beneficiation of coal using supercritical water and carbon dioxide extraction: sulfur removal

Abstract This work explores the use of carbon dioxide, water, and their mixtures as solvent for the precombustion beneficiation of raw coal without using any toxic mineral acids in the temperature range of 200–400 °C. The fluid polarity, ionic constant, and supercritical point can be adjusted by H 2 O/CO 2 ratio and temperature. Adding carbon dioxide to hydrothermal fluid also increases the ionization by forming carbonic acid. Extractions with supercritical fluids have several benefits including enhanced mass transport, ease of separation and recycle, wide range of extractive capability and tunability, better inherent safety, and in the case of carbon dioxide and water–low cost. A semi-continuous extraction system was designed and built in which pressure, temperature and the relative flow rates of CO 2 and H 2 O can be controlled. Coal powder is kept in a packed bed and the extraction is carried out at 143 bar pressure. Using sulfur as a model heteroatom, extractive efficiency is examined as a function of the temperature, fluid composition, fluid flow, and extraction time. The results indicate that carbon dioxide, water, and supercritical water-carbon dioxide (ScWC) all can effectively extract about 50% of total sulfur from bituminous coal in 1 h. Extraction above 350 °C decreased effectiveness, and extraction above the supercritical point of pure water caused hydrothermal carbonization. ScWC extraction may provide necessary control to prevent organic dissolution while removing sulfur.

DeCuir, Matthew J.↗

Seawater Acidification and Bubble Plume Dispersion from Accidental Subsea CO 2 Pipeline Rupture: A Multiphase CFD Study

If a CO 2 reservoir or transmission pipeline were to leak, both the surrounding ecology and maritime traffic safety could be put at risk. To better understand and prepare for this risk, multiphase Computational Fluid Dynamics (CFD) models were built in ANSYS Fluent to capture the behavior of a leak once it enters the water. A 3D Eulerian–Eulerian model was used for validation, while a simplified 2D model was applied to simulate conditions at a 50-m depth. The models integrate bubble dynamics, gas holdup, CO 2 dissolution, dissolved species transport, and seawater acidification into a unified CFD framework. Mass transfer was calculated using the Hughmark correlation, and local seawater temperature and salinity were factored in to determine dissociation behavior and the relevant Henry’s Law constant. To confirm the 3D model’s accuracy, results were checked against two experimental datasets: the QICS field study and the Hauser Tank experiments. The team also modeled a hypothetical release scenario at the High Island 10L site and compared the results with earlier published work. The results show that at a depth of 50 m, the surrounding water column can completely absorb a CO 2 release at a rate of 35 kg/s, since the gas dissolves into the seawater as it rises toward the surface. Beyond confirming this mitigation capacity, the simulations shed light on how a leak would actually unfold in the environment, including the shape and movement of the rising bubble plume, how much CO 2 dissolves along the way, and the resulting shifts in seawater pH and pCO 2 . Together, this provides a practical framework for assessing how CO 2 leaks could affect marine environments in the Gulf of Mexico.

54 ENVIRONMENTAL SCIENCES↗

Path Forward for Groundwater Compliance Strategy at the Tuba City, Arizona, Disposal Site - 19581

The Tuba City, Arizona, Disposal Site is located in the Navajo Nation and near the Hopi Reservation. A uranium mill operated at the site from 1956 to 1966. During the operational period, mill tailings were slurried to an unlined impoundment. Excess slurry water was transferred to unlined evaporation ponds. Groundwater contamination resulting from the infiltration of fluids in the mill tailings impoundment and evaporation ponds was characterized in the 1990's. The site's Groundwater Compliance Action Plan was prepared in 1999, and a groundwater extraction and treatment system was constructed in 2002. Issues with aquifer productivity and treatment plant reliability led to the suspension of operations in 2014. The limitations of the remediation system prompted a realization that the site conceptual model should be reevaluated. An integrated study to better understand the geochemical and hydrologic factors affecting contaminant transport, to support the development of a new groundwater compliance strategy, was initiated in 2017 and is ongoing. In addition to the groundwater science components, the study included the evaluation of enhanced evaporation methods. The integrated evaluation will lead to refinement of the site groundwater flow model and development of a contaminant transport model and subsequent development of remedial alternatives. Remedial alternatives will be evaluated to determine a new groundwater compliance strategy. The objectives of geochemical testing were to confirm and quantify geochemical reactions controlling uranium fate and transport. These reactions are important because they control the distribution of uranium on the solid phase; potential for release from the solid phase; mobility of uranium in the water phase; and potential for uranium redistribution onto the currently uncontaminated solid phase. A key outcome is the change in understanding of the mass of uranium in the subsurface that is potentially soluble. These results contradict the previous basis for remediation: that uranium was almost exclusively present in soluble form, within the boundaries of the contaminant plume. Testing showed that uranium sorption downgradient from the plume was measurable but relatively minimal. The movement of other mill-related constituents (nitrate, sulfate, alkalinity) results in the dissolution of naturally occurring uranium and a higher than background concentration of uranium in groundwater. These constituents are not subject to sorption, and their downgradient concentrations are reduced only by diffusion and dispersion. The geochemical testing provides conceptual and quantitative information on potential plume migration. While the testing revealed the potential availability of uranium contaminant sources, the aquifer buffering capacity, pH, and presence of oxygen in groundwater may, individually or in combination, be controlling factors for plume movement. Evaluation of evaporative treatment alternatives was undertaken to determine one or more sustainable and efficient methods capable of treating 151 liters per minute (L/min) (40 gallons per minute), the annual average flow rate. In addition to establishing the baseline capacity for evaporation using the site's existing pond, prospective methods of enhanced evaporation included preheating water before inflow to the evaporation pond, vertical circulation in the pond, dye addition, and Wind-Aided Intensified Evaporation. Consideration of a 151 L/min evaporative treatment arose from previous analysis of extraction well production rates and contaminant mass removal, which indicated that about 80% contaminant removal, relative to full-scale operation of the site's groundwater treatment plant, could be achieved with a smaller capacity system. The lower-flow evaporative option also represented a potentially more sustainable treatment system in comparison to restarting or reconfiguring the groundwater treatment plant. Aquifer pumping tests were designed to develop or improve estimates of hydraulic properties such as transmissivity, horizontal and vertical hydraulic conductivity, storativity, and storage coefficient. Testing involved pumping from one well at a constant flow rate for up to 5 days while monitoring groundwater drawdown in the pumping well and five surrounding wells and then shutting down the pumping well to observe groundwater recovery. The aquifer pumping test results provide insight regarding the hydraulics of the saturated zone. The saturated zone is in a low-conductivity formation with preferential flow in the horizontal direction. The aquifer exhibits low vertical conductance. The use of AQTESOLV software indicates that the saturated zone is a layered system due to the cross-bedded sand-grain orientation within the Navajo Sandstone. These indicators of limited vertical flow provide a potential justification for the observed depth of the contaminant plume of 15-46 meters (50-150 feet) below ground surface). Given the relatively low vertical conductance, groundwater extraction should be focused on the upper portions of the saturated zone. Aquifer response testing provided an improved understanding of aquifer characteristics. However, the primary objective, to identify optimal groundwater extraction strategies, has not been fully addressed. A list of path forward activities for hydrologic analyses was developed, with an overarching objective of providing input parameters for groundwater flow and contaminant transport modeling. Defensible predictions of contaminant transport, through modeling, are critical to the development of a new site groundwater compliance strategy. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Photocatalyzed electron exchange between organic chromophores and hematite nanoparticles and the role of solid-state charge transport

Understanding photocatalyzed redox interactions between Fe(III)–(oxyhydr)oxide mineral nanoparticles and adsorbed chromophoric organic matter is critical for accurately predicting bioavailable iron fluxes in the euphotic zone of natural aquatic systems, and for improving the effectiveness of nano-iron-based water purification systems. However, the electron transfer processes that underpin photoreductive dissolution at particle/organic/solution interfaces occur on ultrafast timescales and thus remain difficult to probe. In this work, we report an ultrafast transient absorption spectroscopy (TAS) study of suspensions of hematite nanoplatelets (HNPs) sensitized by adsorbed rhodamine B (RhB) dye as a function of solution media and pH. The TAS results indicate a substantially longer fluorescence lifetime of RhB adsorbed on HNPs across a wide range of pH conditions, consistent with transient photoinduced electron transfer to the oxide with recombination kinetics controlled by electron migration back to the interface via small polaron hopping. Normalization of the observed kinetics to the measured surface loading of RhB at different pH values shows that the recombination rates are insensitive to environmental variables, likely controlled instead by particle properties that determine small polaron diffusion behavior.

54 ENVIRONMENTAL SCIENCES↗

Laser-Interference Surface Preparation for Enhanced Coating Adhesion and Adhesive Joining of Multi-Materials (Final Project Report)

This report investigates a laser-interference surface treatment as a non-contact, i.e., without major solid/liquid medium application or abrasion, and non-chemical surface preparation method for aerospace coating systems. It was proposed to use the laser-interference technique to structure surfaces of Al and/or Ti, creating "rough" surfaces with pre-engineered series of ridges and valleys at submicron scale. The science goal of this study was to develop an understanding of the surface microstructure, topology, and physical mechanisms that would improve adhesion and corrosion protection of Al2024-T3. Microstructure analysis indicates that the laser-interference structuring (LIS) was found to reduce the formation of CuMn-rich precipitates in Al 2024-T3 over a 500-800 nm depth from top surface. The X-cut and cross-hatch coating adhesion ratings indicate that the LIS specimens meet the performance requirements in the coating adhesion specifications by having a higher or identical ranking to those specimens prepared with current state-of-the-art chemical conversion or sulfuric acid anodizing. After the ASTM B117 corrosion exposure, it was found that the laser processed specimens exhibited only few blisters. It was found that the corrosion damage was minimized at a laser rastering speed of 4 mm/s, for which only 33% of specimens developed very minor corrosion damage. The ASTM D1654 creepage ratings, used to evaluate corrosion damage along the scribe lines, were found to be at least nine for all coated panels. These results indicate that the laser-interference technique with the additional acetone wiping has the potential to be further developed as a minor chemical surface preparation technique for chromate-containing epoxy primers coatings.

36 MATERIALS SCIENCE↗

Fungal hyphae develop where titanomagnetite inclusions reach the surface of basalt grains

Nutrient foraging by fungi weathers rocks by mechanical and biochemical processes. Distinguishing fungal-driven transformation from abiotic mechanisms in soil remains a challenge due to complexities within natural field environments. We examined the role of fungal hyphae in the incipient weathering of granulated basalt from a three-year field experiment in a mixed hardwood-pine forest (S. Carolina) to identify alteration at the nanometer to micron scales based on microscopy-tomography analyses. Investigations of fungal-grain contacts revealed (i) a hypha-biofilm-basaltic glass interface coinciding with titanomagnetite inclusions exposed on the grain surface and embedded in the glass matrix and (ii) native dendritic and subhedral titanomagnetite inclusions in the upper 1–2 µm of the grain surface that spanned the length of the fungal-grain interface. We provide evidence of submicron basaltic glass dissolution occurring at a fungal-grain contact in a soil field setting. An example of how fungal-mediated weathering can be distinguished from abiotic mechanisms in the field was demonstrated by observing hyphal selective occupation and hydrolysis of glass-titanomagnetite surfaces. We hypothesize that the fungi were drawn to basaltic glass-titanomagnetite boundaries given that titanomagnetite exposed on or very near grain surfaces represents a source of iron to microbes. Furthermore, glass is energetically favorable to weathering in the presence of titanomagnetite. Our observations demonstrate that fungi interact with and transform basaltic substrates over a three-year time scale in field environments, which is central to understanding the rates and pathways of biogeochemical reactions related to nuclear waste disposal, geologic carbon storage, nutrient cycling, cultural artifact preservation, and soil-formation processes.

58 GEOSCIENCES↗

Electrochemical Mitigation of Corrosion in Molten Chloride Salts During CSP Plant Operation

We are designing an electrochemical flow-cell for removal of corrosive impurities from molten chloride salt Gen3 Concentrating Solar Power (CSP) plants during plant operation. Corrosive impurities will inevitably form in molten chloride salts upon exposure to air and moisture. We previously showed that even small amounts of these impurities, especially MgOHCl, will be detrimental in Gen3 CSP plants, necessitating prohibitively expensive containment alloys and frequent replacement of corroded components. Pre-purification of salt with Mg metal at temperatures above 650 degrees C is the current method for removing corrosive impurities from chloride salts before they are introduced to CSP systems. However, this is not a suitable method for impurity removal during plant operation. First, this method will produce MgO particulates which will damage plant components. Second, Mg metal is solid at the low temperature point (500 degrees C), so the purification will not proceed at a fast rate. At the high temperature point, Mg is soluble. In this case, fast purification may proceed, but dissolved metal is likely to precipitate out in cold-temperature point components, causing damage. In contrast, our electrochemically driven method allows fast Mg-based purification to proceed at the low temperature point, without formation of harmful particulates and without the risk of Mg metal precipitation. This novel approach is inspired by electrorefining techniques that are widely employed in industrial metallurgy for removal of impurities from metals. Impurities in the incoming molten salt will be reduced to inert MgO at the cathode, which can be removed by periodically washing the cell with acid. Simultaneously, Mg dissolution at the anode will ensure salt composition is maintained, with no net removal of Mg2+. We have validated this electrochemical approach at lab scale under static conditions with batch rectors. Furthermore, we have performed analytical modeling and technoeconomic analysis to produce a preliminary engineering design for the purification flow cell.

CSP↗

A nitrogen- and carbonyl-rich conjugated small-molecule organic cathode for high-performance sodium-ion batteries

Organic-based cathode materials have attracted considerable attention for sustainable Na-ion batteries due to their great promise to overcome the issues arising from the insertion of large Na + into the rigid structures of conventional transition-metal-containing inorganic electrodes. The structural flexibility as a result of weak intermolecular interactions and simple electron- and ion-storage mechanisms found in organic compounds ensure facile and reversible transport of Na ions. In order to address the general drawbacks of small-molecule organic electrodes such as material dissolution in commonly used organic electrolytes and poor electronic conductivity, we report the use of a nitrogen- and carbonyl-rich highly extended π-conjugated small molecule, hexaazatrianthranylene (HATA) embedded quinone (HATAQ), as a cathode for sodium-ion batteries. The unique hydrogen bonds between highly functionalized conjugated HATAQ molecules allow supramolecular graphite-like 2D layered arrangements in the solid state which help facilitate the structural stability during long-term cycling and promote charge transfer. The compound delivers a capacity as high as 460 mA h g -1 at 500 mA g -1 and an excellent capacity retention of 99% (~138 mA h g -1 ) after 5000 cycles at an extremely high rate of 60 A g -1 . The reaction kinetics and redox mechanism of the material have been elucidated by several characterization techniques together with density functional theory (DFT) studies. The insights gained in this work could pave the way for ultra-high-performance small-molecule organic cathodes for sustainable energy storage.

25 ENERGY STORAGE↗

Durable High-Power Membrane Electrode Assemblies with Low Pt Loading

Recent progress in developing and implementing Pt-alloy cathode catalysts and thin (10-15 micron) low resistance membranes has enabled high performance state of art (SOA) membrane electrode assembly (MEA) with low Pt loading. However, these high performing MEAs do not meet durability requirements, especially at peak power, because of complex degradation mechanisms that are sensitive to the materials, MEA design, and fuel cell operating strategy. Specifically, power degradation of the cathode occurs via Pt and Co dissolution as well as deterioration of O 2 transport properties. Additionally, thin membranes are subject to failure due to manufacturing defects in the adjacent gas diffusion media and electrodes and the formation of membrane-attacking radical species caused by high gas crossover. In this project led by General Motors LLC (GM), the objective was to enhance the durability of SOA MEA through optimization of operating conditions, instead of new materials development. Along with our project partners, we have mapped the impact of operating conditions on the durability of SOA MEA. Output of the project include a low Pt loading SOA MEA that exceeds Department of Energy (DOE) 2020 target of >1 W/cm 2 at rated power and pathway to achieve >5000 h of durability. Durability studies in the project provide a detailed understanding of failure modes and operating condition sensitivity on cathode and membrane failure, critical for defining operating conditions and hybridization strategies that can guide system controls to maximize low-Pt MEA life. The project also generated and validated degradation models that will provide future research direction, critical for guiding future cycles of automotive MEA development.

08 HYDROGEN↗

Development of Corrosion Resistant Coatings for Structural Materials for Liquid Fueled Molten Salts Reactors Applications (Final Report)

Current structural alloys, code certified for the MSRs temperature ranges, contain high levels of chromium, making them highly susceptible to molten halide salt corrosion. One potential solution to circumvent the need for code certification of novel alloys, which is expensive and time consuming, is to design claddings that will protect the underlying code certified materials from corrosion damage during operation. In this work, we examined the corrosion of Ni and Cu electroplated, Ni and CuNi weld overlay, Mo-laser clad, and carburized claddings on SS316H for use in molten salt reactor environments. After characterization of the cladded materials (Task 1), static corrosion tests were used to assess corrosion resistance of the claddings in typical molten fluoride salts (Task 2). The corrosion tests were performed in molten FLiNaK at 700°C up to 1000 hours. Pre- and post-corrosion Scanning Electron Microscopy (SEM), energy-dispersive-spectroscopy (EDS), Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD) and glow-discharge-optical-emission-spectroscopy (GDOES) were performed on cladding cross-sections and surfaces to evaluate degradation. The Cu and Ni electroplated samples, as well as the carburized samples, showed excellent corrosion resistance relative to the bare SS316H. To assess high temperature cladding stability, ageing experiments were performed at temperatures up to 900 C in inert atmosphere for the electroplated and carburized samples and a diffusion model was developed to predict long term cladding behavior (Task 3). It was found that the Cu cladding was basically insensitive to the high temperature ageing, except for small secondary phases forming at the interface. On the other hand, the Ni electroplated cladding experienced significant interdiffusion. Nevertheless, the gain in corrosion resistance for a 100μm Ni electroplated cladding is phenomenal, with more than 50% reduction in chromium dissolution from the substrate material for the first 15 years of salt exposure at 700°C. To assess radiation resistance and phase stability, high-temperature 4MeV Ni heavy ion irradiation was performed across the cladding/substrate interface up to 50 displacement-per-atom (DPA) at 500°C and 700°C to assess the phase stability and irradiation behaviors of the electroplated systems (Task 4). The Ni and Cu electroplated systems did not experience void swelling at the contrary to the SS316H substrate due to their nanocrystalline nature. Some level of recrystallization was observed in the cladding, as well as radiation induced segregation and enhanced diffusion. The interface acted as a potent sink for point defects with the presence of a void denuded zone. The mechanical properties of the claddings were assessed using thermal shock, micro-indentation, nano-indentation, and four-point bend testing experiments (Task 5). These experiments were performed on the claddings in as-received, corroded, irradiated, and thermally aged states to determine the effects of typical molten salt reactor environments on cladding integrity. No significant mass loss was observed after repeated thermal shocks. While the electroplated samples softened after high-temperature ageing, irradiation hardening compensate this effect, such that there is little different with the as-received materials. The results of these experiments suggest that the electroplated (copper/nickel) show the greatest promise for application in molten salt reactor development. These claddings prevented any chromium dissolution from occurring during the static corrosion experiments. Additionally, they demonstrated favorable properties for high temperature diffusion, phase stability, interfacial mechanical properties, and irradiation resistance. Weld-overlay cladding are also of great interest and could reach properties similar to the electroplated samples upon optimization (especially with multiple weld passes). The carburized SS316H showed excellent behavior as well, but more work needs to be done to assess their long-term stability. Finally, the Mo-laser clad system was not pursued further due to the manufacturing challenges. It is also worth noting that the Ni cladding systems should behave relatively well in terms of weldability since the Ni-weld overlay microstructure and associated corrosion rate are sound. While the NiCu weld-overlay has even lower corrosion rates than the Ni-weld overlay, more studies on welding of Cu-electroplated systems are necessary since Cu clusters are known to embrittle steels.

36 MATERIALS SCIENCE↗

Common Ion Effects In Zeoponic Substrates: Dissolution And Cation Exchange Variations Due to Additions of Calcite, Dolomite and Wollastonite

c1inoptilolite-rich tuff-hydroxyapatite mixture (zeoponic substrate) has the potential to serve as a synthetic soil-additive for plant growth. Essential plant macro-nutrients such as calcium, phosphorous, magnesium, ammonium and potassium are released into solution via dissolution of the hydroxyapatite and cation exchange on zeolite charged sites. Plant growth experiments resulting in low yield for wheat have been attributed to a Ca deficiency caused by a high degree of cation exchange by the zeolite. Batch-equilibration experiments were performed in order to determine if the Ca deficiency can be remedied by the addition of a second Ca-bearing, soluble, mineral such as calcite, dolomite or wollastonite. Variations in the amount of calcite, dolomite or wollastonite resulted in systematic changes in the concentrations of Ca and P. The addition of calcite, dolomite or wollastonite to the zeoponic substrate resulted in an exponential decrease in the phosphorous concentration in solution. The exponential rate of decay was greatest for calcite (5.60 wt. % -I), intermediate for wollastonite (2.85 wt.% -I) and least for dolomite (1.58 wt.% -I). Additions of the three minerals resulted in linear increases in the calcium concentration in solution. The rate of increase was greatest for calcite (3.64), intermediate for wollastonite (2.41) and least for dolomite (0.61). The observed changes in P and Ca concentration are consistent with the solubilities of calcite, dolomite and wollastonite and with changes expected from a common ion effect with Ca. Keywords: zeolite, zeoponics, common-ion effect, clinoptilolite, hydroxyapatite

Beiersdorfer, R. E.↗

Evolution of Local Microstructures: Spatial Instabilities of Coarsening Clusters

This work examines the diffusional growth of discrete phase particles dispersed within a matrix. Engineering materials are often microstructurally heterogeneous, and the details of the microstructure determine how well that material performs in a given application. Critical to the development of designing multiphase microstructures with long-term stability is the process of Ostwald ripening. Ripening, or phase coarsening, is diffusion-limited and arises in polydisperse multiphase materials. Growth and dissolution occur because fluxes of solute, driven by chemical potential gradients at the interfaces of the dispersed phase material, depend on particle size. Competitive kinetics of these processes dictates that larger particles grow at the expense of smaller ones, overall leading to an increase of the average particle size. The classical treatment of phase coarsening was done by Todes, Lifshitz, and Slyozov, (TLS) in the limit of zero volume fraction, V(sub V)=0 of the dispersed phase. Since the publication of TLS theory, there have been numerous investigations, many of which sought to describe the kinetic scaling behavior over a range of volume fractions. Some studies in the literature report that the relative increase in coarsening rate at low (but not zero) volume fractions compared to that predicted by TLS is proportional to V(exp 1/2)(sub v) whereas others suggest V(exp 1/3)(sub v).This issue has been addressed recently by simulation studies at low volume fractions in three dimensions by members of the Rensselaer/MSFC team.

Glicksman, Martin E.↗

Li–Mn–O Li-rich cation disordered rock-salt cathode materials do not undergo reversible oxygen redox during cycling

An in-depth study of “Li 4 Mn 2 O 5 ”, a nanocomposite of Li 2 O and Li 4-x Mn 2 O 5 with a disordered rock salt structure (LMO), was conducted to determine the origins of the observed anomalously high charge and discharge capacity in lithium cells, which can exceed 350 mA h g -1 . Using soft and hard X-ray absorption spectroscopy (XAS), mapping of resonant inelastic X-ray scattering (mRIXS), and X-ray Raman spectroscopy (XRS), it was determined that electrochemical decomposition of Li 2 O upon charge and reduction of Mn to below 3+ during discharge is responsible for the capacities that are observed, with no evidence of contributions from reversible oxygen redox. Here, the over-reduction is exacerbated when charging limits of 4.5–4.8 V are used due to side reactions between electrolytic solution and the highly oxidized active material. These side reactions result in dissolution of Mn at room temperature and release of oxygen and other gases during initial cycles, which, in turn, cause rapid capacity fading. This is accompanied by evolution of the voltage profile upon cycling towards one that resembles that of manganese oxide spinels. The cycling behavior can be improved somewhat by reducing the upper voltage limit, although this results in a diminishment of the discharge capacities below 200 mA h g -1 . By adding various amounts of spinel LiMn 2 O 4 during synthesis, it was possible to produce LMOs with rock salt structures having significantly improved cycling behavior but still having capacities in excess of 250 mA h g -1 . An optimized modified material also exhibits better rate capability and much less gas evolution during initial cycles than the unmodified LMO. Interestingly, as-made modified materials generally exhibited lower than expected average Mn oxidation states attributable to oxygen loss during the synthesis process, as well as higher capacities than expected based on their manganese contents. The oxygen loss during processing may reduce the activity of the remaining oxygen and account for the lower reactivity of the spinel-modified material.

25 ENERGY STORAGE↗

Evolution of Local Microstructures (ELMS): Spatial Instabilities of Coarsening

This work examines the diffusional growth of discrete phase particles dispersed within a matrix. Engineering materials are microstructurally heterogeneous, and the details of the microstructure determine how well that material performs in a given application. Critical to the development of designing multiphase microstructures with long-term stability is the process of Ostwald ripening. Ripening, or phase coarsening, is a diffusion-limited process which arises in polydisperse multiphase materials. Growth and dissolution occur because fluxes of solute, driven by chemical potential gradients at the interfaces of the dispersed phase material, depend on particle size. The kinetics of these processes are "competitive," dictating that larger particles grow at the expense of smaller ones, overall leading to an increase of the average particle size. The classical treatment of phase coarsening was done by Todes, Lifshitz, and Slyozov, (TLS) in the limit of zero volume fraction, V(sub v), of the dispersed phase. Since the publication of TLS theory there have been numerous investigations, many of which sought to describe the kinetic scaling behavior over a range of volume fractions. Some studies in the literature report that the relative increase in coarsening rate at low (but not zero) volume fractions compared to that / 2 1/ 3 predicted by TLS is proportional to V(sub v)(exp 1/2), whereas others suggest V(sub v)(exp 1/3). This issue has been resolved recently by simulation studies at low volume fractions in three dimensions by members of the Rensselaer/MSFC team.

Glicksman, Martin E.↗