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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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High-Pressure Structural Response of an Insensitive Energetic Crystal: 1,1-Diamino-2,2-dinitroethene (FOX-7)
Abstract not provided
Determination of the Dominant Catalyst Derived from the Classic [RhCp*Cl[subscript 2]][subscript 2] Precatalyst System: Is it Single-Metal Rh[subscript 1]Cp*-Based, Subnanometer Rh4 Cluster-Based, or Rh(0)[subscript n] Nanoparticle-Based Cyclohexene Hydrogenation Catalysis at Room Temperature and Mild Pressures?
Abstract not provided
Raising the Bar: Increased Hydraulic Pressure Allows Unprecedented High Power Densities in Pressure-Retarded Osmosis
Pressure-retarded osmosis (PRO) has the potential to generate sustainable energy from salinity gradients. PRO is typically considered for operation with river water and seawater, but a far greater energy of mixing can be harnessed from hypersaline solutions. This study investigates the power density that can be obtained in PRO from such concentrated solutions. Thin-film composite membranes with an embedded woven mesh were supported by tricot fabric feed spacers in a specially designed crossflow cell to maximize the operating pressure of the system, reaching a stable applied hydraulic pressure of 48 bar (700 psi) for more than 10 h. Operation at this increased hydraulic pressure allowed unprecedented power densities, up to 60 W/m(2) with a 3 M (180 g/L) NaCl draw solution. Experimental power densities demonstrate reasonable agreement with power densities modeled using measured membrane properties, indicating high-pressure operation does not drastically alter membrane performance. Our findings exhibit the promise of the generation of power from high-pressure PRO with concentrated solutions.
High-Pressure Synthesis and Local Structure of Corundum-Type In[subscript 2;#8722;2x]Zn[subscript x]Sn[subscript x]O[subscript 3] (x ;#8804; 0.7)
The corundum-type In{sub 2-2x}Zn{sub x}Sn{sub x}O{sub 3} solid solution (cor-ZITO, x {<=} 0.7) was synthesized at 1000 C under a high pressure of 70 kbar. cor-ZITO is a high-pressure polymorph of the transparent conducting oxide bixbyite-In{sub 2-2x}Zn{sub x}Sn{sub x}O{sub 3} (x {<=} 0.4). Analysis of the extended X-ray absorption fine structure suggests that significant face-sharing of Zn and Sn octahedra occurs, as expected for the corundum structure type. In contrast to the ideal corundum structure, however, Zn and Sn are displaced and form oxygen bonds with lengths that are similar to those observed in high-pressure ZnSnO{sub 3}. Powder X-ray diffraction patterns of cor-ZITO showed the expected unit cell contraction with increased cosubstitution, but no evidence for ilmenite-type ordering of the substituted Zn and Sn. A qualitative second harmonic generation measurement, for the solid solution x = 0.6 and using 1064 nm radiation, showed that Zn and Sn adopt a polar LiNbO{sub 3}-type arrangement.
Pressure-Driven Changes in the Electronic Bonding Environment of GeO 2 Glass above Megabar Pressures
Noncrystalline oxides under pressure undergo gradual structural modifications, highlighted by the formation of a dense noncrystalline network topology. The nature of the densified networks and their electronic structures at high pressures may account for the mechanical hardening and the anomalous changes in electromagnetic properties. Despite its importance, direct probing of the electronic structures in amorphous oxides under compression above the Mbar pressure (>100 GPa) is currently lacking. Here, we report the observation of pressure-driven changes in electronic configurations and their delocalization around oxygen in glasses using inelastic X-ray scattering spectroscopy (IXS). In particular, the first O K-edge IXS spectra for compressed GeO 2 glass up to 148 GPa, the highest pressure ever reached in an experimental study of GeO 2 glass, reveal that the glass densification results from a progressive increase of oxygen proximity. While the triply coordinated oxygen [3] O is dominant below ~50 GPa, the IXS spectra resolve multiple edge features that are unique to topologically disordered [4] O upon densification above 55 GPa. Topological compaction in GeO 2 glass above 100 GPa results in pronounced electronic delocalization, revealing the contribution from Ge d-orbitals to oxide densification. Strong correlations between the glass density and the electronic configurations beyond the Mbar conditions highlight the electronic origins of densification of heavy-metal-bearing oxide glasses. Furthermore, current experimental breakthroughs shed light on the direct probing of the electronic density of states in high-Z oxides above 1 Mbar, offering prospects for studies on the pressure-driven changes in magnetism, superconductivity, and electronic transport properties in heavy-metal-bearing oxides under compression.
Pressure-Induced Phase Transformation, Reversible Amorphization, and Anomalous Visible Light Response in Organolead Bromide Perovskite
Abstract not provided
4D Proxy Imaging of Fracture Dilation and Stress Shadowing Using Electrical Resistivity Tomography During High Pressure Injections into a Dense Rock Formation
Fluid flow through fractured rock systems is governed in large part by the distribution, interconnectivity, and size of fracture apertures. In-situ stress is one of the primary factors controlling fracture aperture, and one that is altered significantly during high-pressure fluid injections or extractions. Interactions between stress, pore pressure, aperture, and fluid flow can result in complex and evolving poroelastic behavior with significant implications regarding the predictability and risk of developing and managing deep subsurface reservoirs (geothermal, fossil energy, and geologic carbon sequestration). In saturated crystalline rocks, bulk electrical conductivity is highly sensitive to porosity, and therefore to fracture aperture size and distribution. We demonstrate the use of time-lapse 3D electrical resistivity tomography for remotely monitoring stress induced changes in aperture distribution during high pressure injections into a fractured rock system at a scale of tens of meters. Results reveal a complex and continuously evolving stress field involving aperture dilations in the natural fracture system and aperture contractions in adjacent zones of shadow stress. Results provide information about the spatiotemporal changes in the system behavior and point to the potential of electrical imaging for autonomously and remotely monitoring evolving stress conditions by proxy through changes in bulk electrical conductivity.
A stable compound of helium and sodium at high pressure
Helium is generally understood to be chemically inert and this is due to its extremely stable closed-shell electronic configuration, zero electron affinity and an unsurpassed ionization potential. It is not known to form thermodynamically stable compounds, except a few inclusion compounds. Here, using the ab initio evolutionary algorithm USPEX and subsequent high-pressure synthesis in a diamond anvil cell, we report the discovery of a thermodynamically stable compound of helium and sodium, Na 2 He, which has a fluorite-type structure and is stable at pressures >113 GPa. We show that the presence of He atoms causes strong electron localization and makes this material insulating. This phase is an electride, with electron pairs localized in interstices, forming eight-centre two-electron bonds within empty Na 8 cubes. As a result, we also predict the existence of Na 2 HeO with a similar structure at pressures above 15 GPa.
Pressure induced polymerization of acetylide anions in CaC 2 and 10 7 fold enhancement of electrical conductivity
Pressure induced polymerization of CaC 2 in the amorphous phase is evidenced for the first time, accompanied by a 10 7 fold enhancement of the electrical conductivity.
Experimental verification of the high pressure crystal structures in NH{sub 3}BH{sub 3}
A detailed high-pressure study on NH{sub 3}BH{sub 3} has been carried out using in situ synchrotron X-ray diffraction (XRD) and Raman scattering with a diamond anvil cell up to 20 and 33 GPa, respectively. The Rietveld refinement based on the XRD pattern and analysis of Raman data indicate two first-order phase transitions from the ambient pressure I4 mm structure (α-NH{sub 3}BH{sub 3}) to a high pressure Cmc2{sub 1} phase (β-NH{sub 3}BH{sub 3}) at 2.14 GPa, and further into a monoclinic P2{sub 1} (Z = 2) phase (γ-NH{sub 3}BH{sub 3}) at 9.67 GPa. Fitting the measured volumetric compression data to the third order Birch-Murnaghan equation of state reveals a bulk modulus of B{sub 0} = 9.9 ± 0.5 and 17.0 ± 3.0 GPa (with fixed B{sub 0}{sup ′} = 4) for the β-NH{sub 3}BH{sub 3} below and above 5 GPa, respectively. Still, with the splitting of the NBH rock mode in Raman experiment, it is concluded that a second-order isostructural phase transition occurs at 5 GPa. By analyzing the dihydrogen bonding framework, the origin of the isostructural phase transition is attributed to the number of dihydrogen bondings per molecule in the Cmc2{sub 1} phase increasing from 12 to 14 at 5 GPa.
High pressure Laue diffraction and its application to study microstructural changes during the α → β phase transition in Si
Here, an approach using polychromatic x-ray Laue diffraction is described for studying pressure induced microstructural changes of materials under pressure. The advantages of this approach with respect to application of monochromatic x-ray diffraction and other techniques are discussed. Experiments to demonstrate the applications of the method have been performed on the α → β phase transition in Si at high pressures using a diamond anvil cell. We present the characterization of microstructures across the α–β phase transition, such as morphology of both the parent and product phases, relative orientation of single-crystals, and deviatoric strains. Subtle inhomogeneous strain of the single-crystal sample caused by lattice rotations becomes detectable with the approach.
Structure of HfO 2 modified with Y, Gd, and Zr at ambient conditions and high pressures
Abstract not provided
High-pressure studies with x-rays using diamond anvil cells
Pressure profoundly alters all states of matter. The symbiotic development of ultrahigh-pressure diamond anvil cells, to compress samples to sustainable multi-megabar pressures; and synchrotron x-ray techniques, to probe materials' properties in situ, has enabled the exploration of rich high-pressure (HP) science. In this article, we first introduce the essential concept of diamond anvil cell technology, together with recent developments and its integration with other extreme environments. We then provide an overview of the latest developments in HP synchrotron techniques, their applications, and current problems, followed by a discussion of HP scientific studies using x-rays in the key multidisciplinary fields. These HP studies include: HP x-ray emission spectroscopy, which provides information on the filled electronic states of HP samples; HP x-ray Raman spectroscopy, which probes the HP chemical bonding changes of light elements; HP electronic inelastic x-ray scattering spectroscopy, which accesses high energy electronic phenomena, including electronic band structure, Fermi surface, excitons, plasmons, and their dispersions; HP resonant inelastic x-ray scattering spectroscopy, which probes shallow core excitations, multiplet structures, and spin-resolved electronic structure; HP nuclear resonant x-ray spectroscopy, which provides phonon densities of state and time-resolved Mössbauer information; HP x-ray imaging, which provides information on hierarchical structures, dynamic processes, and internal strains; HP x-ray diffraction, which determines the fundamental structures and densities of single-crystal, polycrystalline, nanocrystalline, and non-crystalline materials; and HP radial x-ray diffraction, which yields deviatoric, elastic and rheological information. Integrating these tools with hydrostatic or uniaxial pressure media, laser and resistive heating, and cryogenic cooling, has enabled investigations of the structural, vibrational, electronic, and magnetic properties of materials over a wide range of pressure-temperature conditions.
High Voltage Insulation and Gas Absorption of Polymers in High Pressure Argon and Xenon Gases
High pressure gas time projection chambers (HPGTPCs) are made with a variety of materials, many of which have not been well characterized in high pressure noble gas environments. As HPGTPCs are scaled up in size toward ton-scale detectors, assemblies become larger and more complex, creating a need for detailed understanding of how structural supports and high voltage insulators behave. This includes the identification of materials with predictable mechanical properties and without surface charge accumulation that may lead to field deformation or sparking. This paper explores the mechanical and electrical effects of high pressure gas environments on insulating polymers PTFE, HDPE, PEEK, POM and UHMW in Argon and Xenon, including studying absorption, swelling and high voltage insulation strength.
Hybridization and suppression of the superconductivity in CeFeAsO 1-y . Pressure and temperature dependences of the electronic structure
Pressure and temperature dependence of the electronic structure of superconducting (SC) CeFeAsO 1-y and non-SC CeFeAsO 1-y have been investigated using two complementary hard x-ray spectroscopic probes at the Ce L 3 edge, partial fluorescence yield x-ray absorption spectroscopy and resonant x-ray emission spectroscopy. With increasing pressure, the ratio between the intensity of the peak related to the f 0 (Ce 4+ ) state and that of the f 1 (Ce 3+ ) state, I(f 0 )/I(f 1 ), is found to increase continuously for both compounds, indicating a continuous increase in the Ce valence. The valence of non-SC CeFeAsO 1-y is found to be slightly higher than that of SC CeFeAsO 1-y in the entire pressure and temperature ranges of this study. The valence of CeFeAsO 1-y around 6 GPa, where the superconductivity breaks down, is estimated to be ~3.0 , but no change in the valence is observed upon cooling. The dependence of the interatomic distances on the concentration of oxygen vacancies is studied via extended absorption fine structure spectroscopy.
Exploring the high-pressure behavior of superhard tungsten tetraboride
In this work, we examine the high-pressure behavior of superhard material candidate WB{sub 4} using high-pressure synchrotron x-ray diffraction in a diamond anvil cell up to 58.4 GPa. The zero-pressure bulk modulus, K{sub 0}, obtained from fitting the pressure-volume data using the second-order Birch-Murnaghan equation of state is 326 {+-} 3 GPa. A reversible, discontinuous change in slope in the c/a ratio is further observed at {approx}42 GPa, suggesting that lattice softening occurs in the c direction above this pressure. This softening is not observed in other superhard transition metal borides such as ReB{sub 2} compressed to similar pressures. Speculation on the possible relationship between this softening and the orientation of boron-boron bonds in the c direction in the WB{sub 4} structure is included. Finally, the shear and Young's modulus values are calculated using an isotropic model based on the measured bulk modulus and an estimated Poisson's ratio for WB{sub 4}.