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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Dissolution and reprecipitation of amorphous silica in silica Rich shales induces Non-Monotonic evolution of porosity in acidic reactive environments

Advances in sustainable subsurface energy technologies are crucial for meeting our energy and resource needs for a climate-resilient future. Novel strategies to harness subsurface shale reservoirs for recovering valuable metals and for enabling CO 2 storage are influenced by the morphological and mineralogical heterogeneities of these materials. In this context, delineating the interactions of highly acidic solutions such as wet supercritical CO 2 on shales with varying mineralogy is crucial to inform the stability of caprock seal for CO 2 storage and enhancements in permeability for fluid transport, reactivity, and storage. The feedback chemical effects associated with the interactions of acidic solutions on the morphologies and mineralogies of shales have not been extensively investigated. These insights are crucial for assessing temporal changes in the reactivity and the fate of the fluids in subsurface environments. In this study, we investigate the effect of 1M HCl solution on the chemistry and morphology of three different shale samples with varying carbonate, clay and silica contents. An increase in the amorphous content, from 37% to 41.3%, of silica-rich and carbonate/clay lean shale is noted due to reactions with an acidic solution which is attributed to the dissolution of Si-bearing phases such as clays, accompanied by SiO 2 precipitation. In shales bearing high content of clays and carbonates, significant increase in the pore volumes and surface areas are noted. Non-monotonic changes in the micron-scale porosity of silica rich–carbonate/clay lean (e.g., Mowry shale) are noted using in-situ X-ray microtomography experiments. Due to the initial mobilization of silica and dissolution of carbonate/clay phases, the total porosity slightly increases from 6.7% to 10.7% followed by a decrease to similar to 4% caused by SiO 2 reprecipitation. In conclusion, these findings suggest that even though silica is less reactive in acidic environments, the changes in the amorphous and crystalline content due to dissolution and reprecipitation alter the porosity and fluid flow paths.

04 OIL SHALES AND TAR SANDS↗
DOE OSTI2020

29 Si solid state MAS NMR study on leaching behaviors and chemical stability of different Mg-silicate structures for CO 2 sequestration

Silicon is one of the most earth abundant elements, and thus, the fate and reactivity of silicate materials are often important for various energy and environmental technologies including carbon sequestration, where CO 2 is captured and stored as a thermodynamically stable solid carbonate phase. Thus, understanding the structures and chemistries of different silicate phases has become an important research aim. Here in this study, the changes in the silicate structures (Q 0 –Q 4 ) of heat-treated Mg-bearing mineral (serpentine) exposed to a CO 2 -water system (carbonic acid) was investigated using 29 Si MAS NMR, XRPD and ICP-OES and the identified structures were employed to explain complex leaching behaviors of silicate materials. The 29 Si MAS NMR and XRPD analysis indicated that the heat-treated serpentine is a mixture of amorphous (Q 1 : dehydroxylate I, Q 2 : enstatite, Q 4 : silica) and crystalline (Q 0 : forsterite, Q 3 : dehydroxylate II and serpentine) phase, while natural serpentine mineral has single crystalline Q 3 silicate structure. The leaching experiments showed that both Mg and Si in the amorphous silicate structures (Q 1 : dehydroxylate I, Q 2 : enstatite) are more soluble than those in crystalline phase (Q 0 : forsterite, Q 3 : dehydroxylate II and serpentine). Therefore, tuning the silicate structure towards Q 1 and Q 2 would significantly improve carbon sequestration potential of silicate minerals, whereas silicate materials with Q 3 structure would provide great chemical stabilities in acidic conditions. The solubilities of silicate structures were in the order of Q 1 (dehydroxylate I) > Q2 (enstatite) >> Q0 (forsterite) > Q3 (dehydroxylate II) > Q 3 (serpentine) and this finding can be used to better design a wide range of energy and environmental materials and reaction systems.

25 ENERGY STORAGE↗
DOE OSTI2023

E-beam-enhanced solid-state mechanical amorphization of α-quartz: Reduced deformation barrier via localized excess electrons as network modifiers

Under hydrostatic pressure, α-quartz (α-SiO 2 ) undergoes solid-state mechanical amorphization wherein the interpenetration of [SiO 4 ] 2- tetrahedra occurs and the material loses crystallinity. This phase transformation requires a high hydrostatic pressure of 14GPa because the repulsive forces resulting from the ionic nature of the Si–O bonds prevent the severe distortion of the atomic configuration. Herein, we experimentally and computationally demonstrate that e-beam irradiation changes the nature of the interatomic bonds in α-quartz and enhances the solid-state mechanical amorphization at nanoscale. Specifically, during in situ uniaxial compression, a larger permanent deformation occurs in α-quartz submicron pillars compressed during e-beam irradiation than in those without e-beam irradiation. Microstructural analysis reveals that the large permanent deformation under e-beam irradiation originates from the enhanced mechanical amorphization of α-quartz and the subsequent viscoplastic deformation of the amorphized region. Further, atomic-scale simulations suggest that the delocalized excess electrons introduced by e-beam irradiation move to highly distorted atomic configurations and alleviate the repulsive force, thus reducing the barrier to the solid-state mechanical amorphization. In conclusion, these findings deepen our understanding of electron–matter interactions and can be extended to new glass forming and processing technologies at nano- and microscale.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Dynamic Interconversion of Metal Active Site Ensembles in Zeolite Catalysis

Catalysis science is founded on understanding the structure, number, and reactivity of active sites. Kinetic models that consider active sites to be static and noninteracting entities are routinely successful in describing the behavior of heterogeneous catalysts. Yet, active site ensembles often restructure in response to their external environment and even during steady-state catalytic turnover, sometimes requiring non-mean-field kinetic treatments to describe distance-dependent interactions among sites. Such behavior is being recognized more frequently in modern catalysis research, with the advent of experimental methods to quantify turnover rates with increasing precision, an expanding arsenal of operando characterization tools, and computational descriptions of atomic structure and motion at chemical potentials and timescales increasingly relevant to reaction conditions. This review focuses on dynamic changes to metal active site ensembles on zeolite supports, which are silica-based crystalline materials substituted with Al that generate binding sites for isolated and low-nuclearity metal site ensembles. Metal sites can become solvated and mobilized during reaction, facilitating interactions among sites that change their nuclearity and function. Such intersite communication can be regulated by the zeolite support, resulting in non-single-site and potentially non-mean-field kinetic behavior arising from mechanisms of catalytic action that combine elements of those canonically associated with homogeneous and heterogeneous catalysis. Here, we discuss recent literature examples that document dynamic active site behavior in metal-zeolites and outline methodologies to identify and interpret such behavior. We conclude with our outlook on future research directions to develop this evolving branch of catalysis science and harness it for practical applications.

operando characterization↗
NASA NTRS1983

Transmittance and reflectance of crystalline quartz and highand low-water content fused silica from 2 microns to 1 mm

The transmittances and reflectances of cultured crystalline quartz, Suprasil, Suprasil W, and Infrasil were compared over the wavelength region from 2 to 1000 microns. The high-water content of Suprasil and the low-water content of cultured crystalline quartz, Suprasil W, and Infrasil were determined by their transmittances measured at 2.73 microns where water content causes high absorption in optical materials. The fact that the fused silicas, both with high- and low-water content, had identical far-IR transmittances and that their transmittances were greatly inferior to that of crystalline quartz led to the conclusion that their inferior transmittance is due to their amorphous structure and not to their water content.

Heaney, J. B.↗
NASA NTRS1995

The Spreading of Variable-Viscosity Axisymmetric Radial Gravity Currents: Applications to the Emplacement of Venusian 'Pancake' Domes

The Magellan images of Venus have revealed a number of intriguing volcanic features, including the steep-sided or 'pancake' domes. These volcanic domes or flows have morphologies that suggest formation by a single continuous emplacement of lava with a higher viscosity than that of the surrounding basaltic plains. Numerous investigators have suggested that such high viscosity is due to high silica content, leading to the conclusion that the domes are evidence of evolved magmatic products on Venus. However, viscosity depends on crystallinity as well as on silica content: high viscosity could therefore also be due to a cooler (and therefore higher crystal content) lava. Models of dome emplacement which include both cooling and composition factors are thus necessary in order to determine the ranges of crystallinity and silica content which might lead to the observed gross dome morphologies. Accordingly, in this study domes are modelled as radial viscous gravity currents with an assumed cooling-induced viscosity increase to include both effects. Analytical and numerical results indicate that pancake dome formation is feasible with compositions ranging from basaltic to rhyolitic. Therefore, observations of gross dome morphology alone are insufficient for determining composition and the domes do not necessarily represent strong evidence for evolved magmatism on Venus.

Sakimoto, S. E. H.↗
DOE OSTI2020

Phase transformation of hydrous ringwoodite to the lower-mantle phases and the formation of dense hydrous silica

In order to understand the effects of H 2 O on the mineral phases forming under the pressure-temperature conditions of the lower mantle, we have conducted laser-heated diamond-anvil cell experiments on hydrous ringwoodite (Mg 2 SiO 4 with 1.1wt% H 2 O) at pressures between 29 and 59 GPa and temperatures between 1200 and 2400 K. Our experimental results show that hydrous ringwoodite (hRw) converts to crystalline dense hydrous silica, stishovite (Stv) or CaCl 2 -type SiO 2 (mStv), containing 1 wt% H 2 O together with Brd and MgO at the pressure-temperature conditions expected for shallow lower-mantle depths between approximately 660 to 1600 km. Considering lack of sign for melting in our experiments, our preferred interpretation of the observation is that Brd partially breaks down to dense hydrous silica and periclase (Pc), forming Brd + Pc + Stv mineralogy. Our experiments may provide an explanation for the enigmatic coexistence of Stv and Fp inclusions in lower-mantle diamonds

58 GEOSCIENCES↗
NASA NTRS1977

Improved ceramic heat exchange material

Improved corrosion resistant ceramic materials that are suitable for use as regenerative heat exchangers for vehicular gas turbines is reported. Two glass-ceramic materials, C-144 and C-145, have superior durability towards sulfuric acid and sodium sulfate compared to lithium aluminosilicate (LAS) Corning heat exchange material 9455. Material C-144 is a leached LAS material whose major crystalline phase is silica keatite plus mullite, and C-145 is a LAS keatite solid solution (S.S.) material. In comparison to material 9455, material C-144 is two orders of magnitude better in dimensional stability to sulfuric acid at 300 C, and one order of magnitude better in stability to sodium sulfate at 1000 C. Material C-145 is initially two times better in stability to sulfuric acid, and about one order of magnitude better in stability to sodium sulfate. Both C-144 and C-145 have less than 300 ppm delta L/L thermal expansion from ambient to 1000 C, and good dimensional stability of less than approximately 100 ppm delta L/L after exposure to 1000 C for 100 hours. The glass-ceramic fabrication process produced a hexagonal honeycomb matrix having an 85% open frontal area, 50 micrometer wall thickness, and less than 5% porosity.

Mccollister, H. L.↗
NASA NTRS1986

Complex dielectric constants for selected near-millimeter-wave materials at 245 GHz

A double-beam instrument developed in this laboratory has been used to measure the complex dielectric constant of selected materials at 245 GHz. It is reported here the results for crystalline quartz, fused silica (Spectrosil WF and Dynasil 4000), beryllia (iso-pressed), boron nitride (hot-pressed), and a nickel ferrite (Trans-Tech 2-111). Results are compared with the data obtained by other researchers.

Dutta, J. M.↗
NASA NTRS1988

Gossans on Mars

The appearance of rusty iron-rich oxidized cappings over sulfide-bearing rocks on earth indicates that similar gossans may have formed on the surface of Mars. Electrochemical processes and thermodynamic relationships linking acidity to oxidation-reduction reactions between primary sulfide minerals and their oxidative weathering products present in the regolith of Mars are discussed. Remote-sensed visible spectra of the Martian surface are in keeping with the presence of poorly-crystalline FeOOH, jarosite, silica, and clay silicates found in gossans, while incompletely weathered pyrrhotite may represent the magnetic material observed in Martian regolith.

Burns, Roger G.↗
NASA NTRS1993

Venus pancake dome formation: Morphologic effects of a cooling-induced variable viscosity during emplacement

The distinctive steep-sided 'pancake' domes discovered in the Magellan images of Venus have morphologies that suggest formation by a single continuous emplacement of a high viscosity magma. A resemblance of the venusian domes to much smaller terrestrial rhyolite and dacite volcanic domes has prompted some authors to suggest that the domes on Venus also have high silica compositions and thus, high viscosities. However, viscosity is a function of crystallinity as well as silica content in a magma, and thus increases as a result of magmatic cooling. To investigate the effect of a cooling-induced viscosity increase on dome morphology, we have modeled the domes as radial viscous gravity currents that cool during emplacement. Various aspects of the investigation are discussed.

Sakimoto, S. E. H.↗
NASA NTRSDate not supplied

Mineralogy of the Greenheugh Pediment and Underlying Murray Formation from the Mars Science Laboratory CheMin Instrument

The Mars Science Laboratory Curiosity rover has been investigating a sequence of ancient fluvio-lacustrine and eolian units in Gale crater. For much of the mission, Curiosity has studied the fluvio-lacustrine deposits of the Murray formation. Curiosity has also studied the ancient eolian Stimson formation in a few locations, which unconformably overlies the Murray fm. The Stimson formation was previously studied at the Naukluft and Emerson Plateaus and recently studied at the Greenheugh pediment capping unit. The Curiosity science team also investigated the Murray formation directly underlying the pediment. Curiosity drilled the “Edinburgh” target within the pediment capping unit and the “Hutton” target in the Murray formation near the contact with the pediment and delivered these materials to the CheMin X-ray diffractometer to characterize bulk mineralogy. Edinburgh contains abundant plagioclase, pyroxene, magnetite, olivine, and X-ray amorphous materials, with 10 wt.% smectite and minor sanidine. The mineralogy of the Stimson at Greenheugh is distinct from the mineralogy of the Stimson at Naukluft and Emerson because previous Stimson targets did not contain olivine or clay minerals. This suggests sediments in the pediment may have a different source and/or different aqueous alteration history than those from Naukluft and Emerson. Hutton contains abundant plagioclase, pyroxene, magnetite, and X-ray amorphous materials, 6 wt.% smectite, and minor cristobalite, opal-CT, sanidine, hematite, fluorapatite, and anhydrite. Other Murray targets in the surrounding Glen Torridon region that are farther from the pediment contact contain ~30 wt.% smectite and lack cristobalite and opal-CT. Cristobalite and/or opal-CT are present in a few other targets elsewhere along the traverse, including the top of the nearby Vera Rubin ridge and the top of the Pahrump Hills outcrop. Stimson overlies the Pahrump Hills, and, based on projections of the pediment slope, the Stimson may have overlain Vera Rubin ridge. The proximity of the low-smectite and cristobalite- and/or opal-CT-bearing outcrops to the contact between the Murray and Stimson suggests the contact provided a conduit for diagenetic fluids that altered clay minerals and formed crystalline and paracrystalline silica.

E. B. Rampe↗
DOE OSTI2024

Highly cascaded first-order fiber Bragg gratings in highly multimode optical fibers for distributed temperature sensing under harsh environment conditions

This study presents a pioneering technique for fabricating highly cascaded first-order fiber Bragg gratings (FBGs) using a femtosecond laser-assisted point-by-point inscription method in highly multimode optical fibers, specifically Sapphire crystalline fiber, and pure silica coreless fiber. Notably, it marks the first successful demonstration of a distributed array comprising 10 FBGs within highly multimode fibers. This achievement is facilitated by a high-power laser technique that yields larger reflectors characterized by a Gaussian intensity profile. These first-order FBGs offer various advantages, including enhanced reflectivity, reduced fabrication time, and simplified spectral characteristics, enhancing their accessibility for interpretation when contrasted with higher-order FBGs. In addition to that it encompasses a comprehensive analysis of the robustness and efficacy of these FBGs, with particular emphasis on their ability to endure extreme temperatures. These FBGs demonstrate an advantageous capability for localized multi-point temperature monitoring, reaching temperatures up to 1500°C with sapphire crystalline fiber and 1100°C with pure silica coreless fiber. This resilience makes them suitable for deployment in harsh environmental conditions. This innovative approach substantially broadens the potential applications of highly multimode optical fibers, particularly in the arena of sensing and communication, where challenges related to thermal gradients and harsh environments prevail. Furthermore, these groundbreaking first-order FBGs signify a substantial advancement in the realm of distributed temperature sensing, offering supreme capabilities for temperature monitoring and signal stability. As such, our work holds the promise of a substantial impact on industries and applications that demand unwavering reliability under extreme conditions.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Vitreous silica formation within shear bands in a dynamically compacted granular crystalline α‐quartz

A shear band is a heterogeneous, narrow seam within a solid material whose formation is caused by intense localized shearing when a sufficiently large amount of deformation occurs. If that deformation occurs at a sufficiently rapid rate, with operative friction, then co‐located ephemeral heating will occur in the shear band. In this study, shear bands were produced from dynamic shear‐induced compaction of a granular form of crystalline α‐quartz (SiO 2 ). The produced shear bands were approximately 25‐µm thick and were examined with scanning electron microscopy/electron backscatter diffraction, transmission electron microscopy, Raman spectroscopy, and nanoindentation. Further, they were found to contain a mixture of vitreous silica and small‐sized crystallites. This finding is significant because the presence of the vitreous silica within the shear band is a postmortem indicator that the localized temperature had reached or exceeded the melting temperature (∼1723°C) of crystalline SiO 2 during the rapid shear and compaction and then sufficiently rapid cooling quenched in that vitreous state.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Crystalline Mesoporous Complex Oxides: Porosity-Controlled Electromagnetic Response

A colloidal--amphiphile--templated growth is developed to synthesize mesoporous complex oxides with highly crystalline frameworks. Organosilane-containing colloidal templates can convert into thermally stable silica that prevents the overgrowth of crystalline grains and the collapse of the mesoporosity. Using ilmenite CoTiO 3 as an example, the high crystallinity and the extraordinary thermal stability of its mesoporosity are demonstrated at 800 °C for 48 h under air. This synthetic approach is general and applicable to a series of complex oxides that are not reported with mesoporosity and high crystallinity, such as NiTiO 3 , FeTiO 3 , ZnTiO 3 , Co 2 TiO 4 , Zn 2 TiO 4 , MgTi 2 O 5 , and FeTi 2 O 5 . Those novel materials make it possible to build up correlations between mesoscale porosity and surface-sensitive physicochemical properties, e.g., electromagnetic response. For mesoporous CoTiO 3 , there is a 3 K increase of its antiferromagnetic ordering temperature, compared with that of nonporous one. Lastly, this finding provides a general guideline to design mesoporous complex oxides that allow exploring their unique properties different from bulk materials.

36 MATERIALS SCIENCE↗
DOE OSTI2021

A constitutive model for glass–ceramic materials

Glass–ceramics have received recent attention for use in glass–ceramic to metal hermetic seals. Due to their heterogeneous microstructure, these materials exhibit a number of advantageous responses over conventional glass based seals. Key amongst them is the possibility of a controllable thermal strain response and apparent coefficient of thermal expansion which may be used to minimize thermally induced residual stresses for aforementioned seals. Furthermore, these behaviors result from an inorganic glass matrix and variety of crystalline ceramic phases including silica polymorph(s) that may undergo reversible solid-to-solid transformations with associated inelastic strain. Correspondingly, these materials exhibit complex thermomechanical responses associated with multiple inelastic mechanisms (viscoelasticity and phase transformation). While modeling these behaviors is essential for developing and analyzing the corresponding applications, no such model exists. Therefore, in this work a three-dimensional continuum constitutive model for glass–ceramic materials combining these various inelastic mechanisms is developed via an internal state variable approach. A corresponding fully implicit three dimensional numerical formulation is also proposed and implemented. The model is used to simulate existing experiments and validate the proposed formalism. As an example, the simple seal problem of a glass–ceramic seal inside a concentric metal shell is explored. Finally, the impact of the cooling rates, viscoelastic shift factors, and inelastic strain on final residual stress state are all investigated and the differing contributions highlighted.

36 MATERIALS SCIENCE↗
NASA NTRS2018

Weathering in the Forelands of Two Rapidly Retreating Alpine Glaciers of Volcanic Bedrock in the Three Sisters, Oregon, USA

The glaciers of the Three Sisters volcanoes in Cascadia have retreated dramatically over the past century. In order to understand ongoing chemical weathering and solute transport in the proglacial valleys, waters were sampled from glacier outwash streams, local snowmelt, and proglacial springs and lakes at Collier and Diller Glaciers. To understand weathering and transport processes in the proglacial plains, infrared orbital remote sensing data was used to map compositional variability and highlight weathering products, which were then ground-truthed with laboratory mineralogical and chemical analyses of sediments. The hydrochemistry is significantly affected by a sub- and proglacial mafic weathering system lacking carbonate minerals. Here we report major ion concentrations in meltwaters for the summer 2016 and 2017 melt seasons. Total cation concentrations range from 3 to 250 μeq/l and dissolved bicarbonate concentrations range from 2 to 200 μeq/l. Other dissolved anions are negligible compared to bicarbonate. Dissolved silica concentrations range from 2 to 260 μmol/l, comparable to total dissolved cation concentrations. The highest cation and silica concentrations were measured in moraine-sourced springs. Compositional remote sensing analysis identified alteration zones in the proglacial plains at both Collier and Diller indicating potential hydrated silica. This analysis is consistent with laboratory analysis of sediment samples, which indicate the presence of poorly crystalline phases weathering products, including hydrated silica. Weathered materials are preferentially deposited on moraines due to aeolian and glacial transport, as well as intra-moraine alteration, and at abandoned stream terraces due to fluvial transport. Geochemical measurements indicate that the predominant form of chemical weathering in these periglacial mafic systems is the carbonation of feldspar as well as reactive volcanic glass. The presence of poorly crystalline silicates, as indicated by remote sensing datasets and laboratory analysis, is consistent with rapid weathering of feldspars and glass and formation of Fe-Al-Si-bearing mineraloids in these proglacial valleys. This weathering regime has wide-ranging implications for atmospheric CO2 drawdown due to cold-climate volcanic rock weathering.

Rutledge, Alicia M.↗