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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 73 records · Page 4

Pressure-induced polyamorphic transition in CaA l 2 O 4 glass

In situ high-pressure ultrasonic velocity measurements of CaAl 2 O 4 glass reveal abrupt irreversible discontinuities in the elastic wave velocities at ~8–10 GPa. Total structure factor and pair distribution functions measured by synchrotron x-ray diffraction show a rapid change in the intermediate range structure attributed to a rearrangement of calcium ions over this narrow pressure region. Atomistic models obtained from molecular dynamics simulations reveal that this intermediate range structure is explained by a transition of Ca–O void radius distribution from a bimodal distribution with peaks at ~2.1 and ~2.4 Å to a single distribution centered at ~2.1 Å. Further, these abrupt structural changes involving the rapid increase in elastic wave velocity are markedly different to the continuous transformations observed in conventional network-forming glasses, such as SiO 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Resolving domain positions of cellobiose dehydrogenase by small angle X–ray scattering

The interdomain electron transfer (IET) between the catalytic flavodehydrogenase domain and the electron-transferring cytochrome domain of cellobiose dehydrogenase (CDH) plays an essential role in biocatalysis, biosensors and biofuel cells, as well as in its natural function as an auxiliary enzyme of lytic polysaccharide monooxygenase. We investigated the mobility of the cytochrome and dehydrogenase domains of CDH, which is hypothesised to limit IET in solution by small angle X-ray scattering (SAXS). CDH from Myriococcum thermophilum (syn. Crassicarpon hotsonii, syn. Thermothelomyces myriococcoides) was probed by SAXS to study the CDH mobility at different pH and in the presence of divalent cations. By comparison of the experimental SAXS data, using pair-distance distribution functions and Kratky plots, we show an increase in CDH mobility at higher pH, indicating alterations of domain mobility. To further visualise CDH movement in solution, we performed SAXS-based multistate modelling. Glycan structures present on CDH partially masked the resulting SAXS shapes, we diminished these effects by deglycosylation and studied the effect of glycoforms by modelling. The modelling shows that with increasing pH, the cytochrome domain adopts a more flexible state with significant separation from the dehydrogenase domain. On the contrary, the presence of calcium ions decreases the mobility of the cytochrome domain. Experimental SAXS data, multistate modelling and previously reported kinetic data show how pH and divalent ions impact the closed state necessary for the IET governed by the movement of the CDH cytochrome domain.

59 BASIC BIOLOGICAL SCIENCES↗

Assembly and Repair of the Photosystem II Reaction Center

This project investigated the biochemical and biophysical mechanisms governing assembly and repair of Photosystem II (PSII), the membrane protein complex responsible for solar-driven water oxidation in oxygenic photosynthesis. The work focused on three integrated areas: (1) protein–protein interactions that facilitate PSII assembly in cyanobacterial biogenesis centers, (2) the chemical mechanism of photo-assembly of the Mn 4 CaO 5 oxygen-evolving complex (OEC), and (3) mechanisms that target PSII reaction centers for degradation and repair in photosynthetic organisms. Using electron paramagnetic resonance spectroscopy, protein biochemistry, molecular genetics, quantitative mass spectrometry, and computational modeling, the project demonstrated that proton release events limit early steps of OEC assembly and that chloride and calcium ions facilitate Mn oxidation and intermediate stabilization. Complementary studies identified chaperone recruitment mechanisms in cyanobacterial PSII biogenesis centers and translation and protease factors involved in PSII turnover in Chlamydomonas. Together, these results establish proton management and coordinated protein quality control as central design principles in PSII assembly and repair and provide mechanistic insight relevant to biological and artificial photosynthetic systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DataSet for Elucidating molecular level interfacial interactions between a de novo protein and nucleated calcite with solid-state NMR

Biomineralization is the process by which organisms use biomolecules to produce hierarchically structured organic-inorganic composites. Using biology as inspiration, a protein construct (FD31) was previously designed to accelerate formation of nano-calcite with an unconventional {110} face. To understand the molecular interactions essential for protein aided calcite nucleation, solid-state nuclear magnetic resonance (ssNMR) spectroscopy was used in this work to characterize the FD31-calcite interface at the atomic level. Glutamic acid side chains designed to interact directly with calcium ions on the surface were found to have dynamics on the sub-millisecond timescale, indicating possible interactions between the protein and surface waters that were not included in the original model. Dipolar ssNMR recoupling techniques also showed that the protein backbone is ~2 Å closer to the surface than in the original docking model. Refined molecular simulations were done in the presence of explicit waters, which resulted in the protein backbone closer to the surface than in the original docking structure, providing better agreement with experiment and highlighting the important role played by water in FD31-calcite interactions. These studies provide the first experimental evidence to confirm that FD31 interactions with calcite are localized to the surface of the protein designed to serve as a template. However, these studies do indicate a more dynamic binding and closer binding mode between FD31 and the nucleated surface than originally proposed. In all, this enhanced molecular insight into the FD31-calcite interface has advanced our fundamental understanding of the atomic interactions at the organic-inorganic interface and will aid in the design of biological templates for the nucleation of inorganic crystals.

Saccuzzo Close, Emily Grace [Pacific Northwest Nat↗

Impact of magnetic and electric fields on the free energy to form a calcium carbonate ion-pair

Electromagnetic fields are used in water treatment and desalination to regulate scale formation and extend the lifetime of membranes. External electric and magnetic fields can promote or suppress mineral nucleation and growth. However, the molecular-scale mechanisms of such processes remain unknown. Computing the free energies needed to form ion pairs under external fields provides important insights into understanding the elemental steps during the initial formation of mineral scales. In this paper, we used molecular dynamics combined with metadynamics simulations to investigate the free energies of forming the [Ca–CO 3 ] 0 ion pair, a fundamental building block of carbonate scales, under a range of magnetic (up to 10 T) and electric (up to 10 V m −1 ) fields in water. The presence of constant magnetic or electric fields favored the ion pairing reaction and lowered the free energies by up to 3% to 6%. The internal energy and entropic components of the free energy showed significant changes and exhibited non-linear behavior with increasing field strength. The [Ca–CO 3 ] 0 ion pairing is an entropy-driven process in the absence of an external field, but the mechanism shifts to an internal energy-driven process under selected external fields, suggesting possible changes in the nucleation pathways.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Design Principles and Routes for Calcium Alkoxyaluminate Electrolytes

Multivalent-ion battery technologies are increasingly attractive options for meeting diverse energy storage needs. Calcium ion batteries (CIB) are particularly appealing candidates for their earthly abundance, high theoretical volumetric energy density, and relative safety advantages. Here, at present, only a few Ca-ion electrolyte systems are reported to reversibly plate at room temperature: for example, aluminates and borates, including Ca[TPFA] 2 , where [TPFA] - = [Al(OC(CF 3 ) 3 ) 4 ] - and Ca[B(hfip) 4 ] 2 , [B(hfip) 4 ] 2 – = [B(OCH(CF 3 ) 2 ) 4 ] - . Analyzing the structure of these salts reveals a common theme: the prevalent use of a weakly coordinating anion (WCA) consisting of a tetracoordinate aluminum/boron (Al/B) center with fluorinated alkoxides. Leveraging the concept of theory-aided design, we report an innovative, one-pot synthesis of two new calcium-ion electrolyte salts (Ca[Al(tftb) 4 ] 2 , Ca[Al(hftb) 4 ] 2 ) and two reported salts (Ca[Al(hfip) 4 ] 2 and Ca[TPFA] 2 ) where hfip = (-OCH(CF 3 ) 2 ), tftb = (-OC(CF 3 )(Me) 2 ), hftb = (-OC(CF 3 ) 2 (Me)), [TPFA] - = [Al(OC(CF 3 ) 3 ) 4 ] - . We also reveal the dependence of Coulombic efficiency on their inherent propensity for cation–anion coordination.

25 ENERGY STORAGE↗

Salts for multivalent ion batteries

Methods for preparing electrolyte salts for alkaline earth metal-ion batteries (e.g., calcium and magnesium ion batteries) are described. The electrolyte salts comprise alkaline earth metal (e.g., Mg or Ca) salts of 3,4-dicyano-2-trifluoromethylimidazole (TDI). The methods comprise contacting TDI with an alkaline earth metal bis(trifluoroacetate) salt in trifluoroacetic acid.

25 ENERGY STORAGE↗

Effect of seawater as mixing water on the hydration behaviour of tricalcium aluminate

This study explored the mechanism of the effect of seawater on tricalcium aluminate (C{sub 3}A) hydration. The results showed that seawater retarded C{sub 3}A hydration and reduced the reaction degree of C{sub 3}A. The co-existence or ion pairing of Ca{sup 2+} and SO{sub 4}{sup 2−} onto the surface of C{sub 3}A poisoning the reactive sites is the main reason for this retardation. Besides, the precipitation of Mg(OH){sub 2} on the surface of C{sub 3}A would prolong the induction period for another 30 min and then consequently decrease the dissolution rate of C{sub 3}A hydration. Trace amounts of MgSO{sub 4}{sup 0} and Mg{sup 2+} present in the alkaline solution had little retardation effect. It was also found that Cl{sup −} would preferentially react with C{sub 3}A to form Friedel's salt, rather than forming hydroxy-AFm as that in the C{sub 3}A-deionized water paste. The direct formation of Friedel's salt resulted in an accumulation of Al{sup 3+} in solution, which would also hinder the subsequent dissolution of C{sub 3}A.

36 MATERIALS SCIENCE↗

Structural analyses of amorphous calcium carbonate before and after removing strontium ions from an aqueous solution

Amorphous calcium carbonate (ACC) is a precursor of crystalline calcium carbonate; hence, its structural information at the atomic level is very important for controlling the morphology of crystalline calcium carbonate. In this study, we attempted to elucidate the process of Sr extraction from aqueous solution by using ACC for the purpose of removal of radioactive Sr from the contaminated water leaked after the Fukushima Daiichi nuclear accident. Here, the pair distribution functions, g(r) obtained by X-ray and neutron diffraction (ND) measurements show that ACC has a structure partially similar to that of monohydrocalcite, suggesting that ACC is transferred to the crystalline calcium carbonate starting from its crystal nucleus. Rietveld analysis of the ND data showed that the ACC that removed Sr was crystallized to calcite. However, the Sr–O coordination analyzed using extended X-ray absorption fine structure (EXAFS) implies that the local environment of O around Sr is similar to that in crystalline calcium carbonate aragonite.

36 MATERIALS SCIENCE↗

Uptake of aqueous heavy metal ions (Co2+, Cu2+ and Zn2+) by calcium-aluminium-silicate-hydrate gels

Highlights: • C-A-S-H gels containing metal ions (Co{sup 2+}, Cu{sup 2+} or Zn{sup 2+}) were precipitated by a sol-gel technique. • Uptake mechanism and immobilization capacity of divalent metal ions by C-A-S-H are elucidated. • Up to ~55–60 mol% of Zn can be incorporated in defective tobermorite-type C-A-S-H. • Metal uptake by C-A-S-H is controlled mainly by isomorphous substitution for Ca ions. • Crystal-chemical features of C-A-S-H gels and implications for practical application are discussed. Calcium-aluminium-silicate-hydrate (C-A-S-H) gels containing heavy metal ions (Me: Co{sup 2+}, Cu{sup 2+} or Zn{sup 2+}) were precipitated at different Me/Si molar ratios to study the uptake mechanism and immobilization capacity. Aqueous solution chemistry and solid-phase characterization using XRD, FTIR, ESEM-EDX, TEM-HAADF and TG-DSC methods reveal threshold values for ion substitution of ~55–60 mol% for Zn, ~30–40 mol% for Co and ~25–30 mol% for Cu in defective tobermorite-type C-A-S-H with (Ca + Me)/(Si + Al) molar ratios from 0.86 to 1.04. At higher aqueous Me concentrations, Me (chloride) hydroxides start to co-precipitate. The uptake mechanism of Me ions by C-A-S-H is based on (i) isomorphous substitution of Me for Ca in the CaO layer, (ii) ion exchange in the interlayer, (iii) tetrahedral substitution (Zn) within the dreierketten chains and (iv) surface adsorption onto the C-A-S-H gel structure. Systematics in crystal-chemistry of Me-bearing C-A-S-H and implications for application and performance in natural and man-made settings are discussed.

36 MATERIALS SCIENCE↗

Cs retention and diffusion in C-S-H at different Ca/Si ratio

Cement and concrete are commonly used in the construction of repository sites for radioactive wastes. The correct isolation of those contaminants requires good adsorption and low diffusion rates. Both parameters are highly affected by many factors, such as pH, temperature or composition. The large variability of experimental conditions and formulations makes it extraordinarily difficult to tackle the influence of each of them independently in experimental samples. To this effect, molecular dynamics simulations have been employed in this study to investigate the role of the composition in the capacity to retain Cs and diffusivity of these ions in calcium silicate hydrate (C-S-H) gel pores. The results indicate that the adsorption of Cs ions is worsened at high Ca/Si ratios due to a lower interaction of the cations with the C-S-H surface, while hydrophilicity of the C-S-H nanopore rises, resulting in higher long-range ordering and lower diffusion coefficients of Cs ions.

36 MATERIALS SCIENCE↗

A Comparison of Groundwater Sampling Technologies, Including Passive Diffusion Sampling, for Radionuclide Contamination - 20205

Using traditional high-flow purge methods for long-term water quality monitoring of deep groundwater wells can be expensive, affect contaminant migration, and produce excessive volumes of discharge water that can be difficult to manage. The use of low-flow pumping methods and depth discrete bailers (DDBs) can reduce the cost of sampling deep groundwater wells. In general, using different pumping methods to obtain reproducible and representative groundwater can be challenging. Passive diffusion samplers (PDSs) have successfully been used in long-term monitoring for volatile organic compounds, major ions, and trace-elements, but application has been limited for stable and radioactive isotopes. Beginning in 2018, the United States Geological Survey (USGS) conducted three sampling events to test the ability of PDSs and DDBs to obtain reproducible and representative groundwater samples. The sampled well is completed in a regional, permeable carbonate aquifer and is one in a set of wells that have historically been used for tritium tracer testing. All samples were obtained at 180 m (590 ft) below land surface (bls) in a 13.97 cm (5.5 inch) uncased well that has a total depth of 202 m (662 ft) bls. The first sampling event deployed a regenerated cellulose dialysis membrane (RCDM) PDS for 14 days with deionized water as the blank. The second sampling event deployed a RCDM for 27 days also with deionized water as the blank. The third sampling event deployed a Dual Membrane (DM) PDS for 65 days using a blank of tritium-dead carbonate water. The DM PDS was used to assess the effect of longer term deployment on tritium concentrations and address whether or not the PDSs reached equilibrium with ambient groundwater. The day after each of the three passive samplers were retrieved a DDB was used to obtain discrete non-integrated groundwater samples. For each DDB sampling day, the bailer was lowered into the well 10 consecutive times to determine if the water chemistry changed from the first to the last bailed sample. Quality assurance samples including blanks and duplicates were obtained during all three sampling events. All blank waters had tritium concentrations less than 21±33 pCi/L. Major ion (e.g. calcium, chloride, sodium, and sulfate) results were compared between all samples obtained with RCDM and DDB. Major ion concentrations showed a coefficient of variation of less than 6% between all RCDM and DDB samples; however, the coefficient of variation between the different deployment times and the two different methods for trace-element concentrations was much larger, particularly for manganese (82%), lead (41%), and zinc (33%). Stable isotope values were compared between the RCDM and DDB samples. The DDB sample results all fell within analytical uncertainty and were considered representative of the formation groundwater. The stable isotope values from the RCDM samples indicated that a longer deployment time was necessary to gain equilibrium and to obtain representative groundwater samples. Tritium results from groundwater samples obtained from the RCDM, DM, and DDB indicate that groundwaters obtained with PDSs produced tritium concentrations 2 to 3 times higher (between 1,426 and 3,060±87 pCi/L) than groundwaters obtained with a DDB (479 to 1,219±51 pCi/L). The longer the passive diffusion samplers were deployed, the higher the tritium concentration, suggesting that equilibrium with tritium was not reached within a 27-day deployment. DDB samples showed tritium results declining from the first to the last bailed sample for all three sampling events. This research suggests that tritium results from groundwater samples obtained from PDSs are more reproducible than samples obtained from DDBs. Also, PDSs likely do not accumulate isotopes of water but rather equilibrate with the ambient groundwater. On the other hand, both PDSs and DDBs were able to provide representative groundwater samples for major ions and have the potential to produce representative groundwater samples for stable isotopes of water (δD and δ{sup 18}O). Utilizing the most effective method for sampling groundwater is important for long-term groundwater monitoring. Quantifying the ability of passive diffusion groundwater samplers to obtain representative radioactive chemistry samples will help determine if these methods can be a useful alternative to pumping and purging wells for long-term monitoring. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Layered Transition Metal Oxides as Ca Intercalation Cathodes: A Systematic First-Principles Evaluation

Finding high-voltage Ca cathode materials is a critical step to unleashing the full potential of high-energy-density Ca-ion batteries. Therefore, first-principles calculations are used to demonstrate that P-type layered calcium transition metal (TM) oxide materials (CaTM 2 O 4 ) with a range of TM substitutions (TM = Ti, V, Cr, Mn, Fe, Co, and Ni) have excellent battery-related properties including thermodynamic stability, average voltage, energy density, synthesizability, ionic mobility, and electronic structure. However, the thermodynamic stability of the charged phase and TM redox activity are shown to be sensitive to TM selection, with CaCo 2 O 4 having the best balance of all considered properties. The utility of combining multiple TMs to expand the chemical search space for TM substitutions is demonstrated by mixing Co and Ni in layered CaTM 2 O 4 .

25 ENERGY STORAGE↗

Adiabatically controlled motional states of a CaO + and Ca + trapped-ion chain cooled to the ground state

Control of the external degree of freedom of trapped molecular ions is essential for their promising applications to spectroscopy, precision measurements of fundamental constants, and quantum information technology. Here, in this study, we demonstrate near ground-state cooling of the axial motional modes of a calcium mono-oxide ion via sympathetic sideband cooling with a cotrapped calcium ion. We also show that the phonon state of the axial out-of-phase mode of the ion chain is maintained while the mode frequency is adiabatically ramped up and/or down. The adiabatic ramping of the motional mode frequency is a prerequisite for searching for the proposed molecular dipole-phonon interaction.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Structural mechanisms of TRPV6 inhibition by ruthenium red and econazole

TRPV6 is a calcium-selective ion channel implicated in epithelial Ca 2+ uptake. TRPV6 inhibitors are needed for the treatment of a broad range of diseases associated with disturbed calcium homeostasis, including cancers. Here we combine cryo-EM, calcium imaging, and mutagenesis to explore molecular bases of human TRPV6 inhibition by the antifungal drug econazole and the universal ion channel blocker ruthenium red (RR). Econazole binds to an allosteric site at the channel’s periphery, where it replaces a lipid. In contrast, RR inhibits TRPV6 by binding in the middle of the ion channel’s selectivity filter and plugging its pore like a bottle cork. Despite different binding site locations, both inhibitors induce similar conformational changes in the channel resulting in closure of the gate formed by S6 helices bundle crossing. The uncovered molecular mechanisms of TRPV6 inhibition can guide the design of a new generation of clinically useful inhibitors.

59 BASIC BIOLOGICAL SCIENCES↗

Computational Predictions of the Stability of Fluorinated Calcium Aluminate and Borate Salts

Energy storage concepts based on multivalent ions, such as calcium, have great potential to become next-generation batteries due to their low cost and comparable cell voltage and energy density to Li-ion batteries. However, the development of Ca batteries is still hindered by the lack of suitable materials that grant a long cycle life. Specific to electrolyte materials, developing a calcium salt that is chemically stable under ambient conditions and enables reversible electrodeposition of Ca is critical. In this work, we use first-principles calculations to study the intrinsic and reductive stability of twelve Ca salts with fluorinated aluminate and borate anions and analyze the decomposition products formed on the metal anode surface that are critical to early-stage solid electrolyte interphase formation. Here we found anions with significant steric hindrance and a high degree of fluorination are intrinsically less stable and deemed unviable designs for Ca salt. Aluminate salts are generally less reactive with the Ca anode than their borate counterparts, and a high degree of fluorination leads to weaker reductive stability. Calcium fluoride is the most prominent decomposition product on the anode surface, and carbide-like motifs were also found from the decomposition of the designed salts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗