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All sourcesNASA NTRSDOE OSTI
NASA NTRS1988

Perovskite-type oxides - Oxygen electrocatalysis and bulk structure

Perovskite type oxides were considered for use as oxygen reduction and generation electrocatalysts in alkaline electrolytes. Perovskite stability and electrocatalytic activity are studied along with possible relationships of the latter with the bulk solid state properties. A series of compounds of the type LaFe(x)Ni1(-x)O3 was used as a model system to gain information on the possible relationships between surface catalytic activity and bulk structure. Hydrogen peroxide decomposition rate constants were measured for these compounds. Ex situ Mossbauer effect spectroscopy (MES), and magnetic susceptibility measurements were used to study the solid state properties. X ray photoelectron spectroscopy (XPS) was used to examine the surface. MES has indicated the presence of a paramagnetic to magnetically ordered phase transition for values of x between 0.4 and 0.5. A correlation was found between the values of the MES isomer shift and the catalytic activity for peroxide decomposition. Thus, the catalytic activity can be correlated to the d-electron density for the transition metal cations.

Carbonio, R. E.↗
NASA NTRS1992

Moessbauer spectroscopy of Mg(0.9)Fe(0.1)SiO3 perovskite

Ambient pressure Moessbauer spectra of Mg(0.9)Fe-57(0.1)SiO3 perovskite synthesized at pressure-temperature conditions of about 50 GPa and 1700 K show that the iron is entirely high-spin Fe(2+) and appears to be primarily located in the octahedral site within the crystal structure. We observe broad Moessbauer lines, suggesting a distribution of electric-field gradients caused by disorder associated with the Fe ions. Also, the perovskite exhibits magnetic ordering at temperatures lower than 5 K, implying that there is a magnetic contribution to the absolute ('third-law') entropy of this phase.

Jeanloz, Raymond↗
NASA NTRS2001

Rare-Earth Garnets and Perovskites for Space-Based ADR Cooling at High T and Low H

Future NASA satellite detector systems must be cooled to the 0.1 K temperature range to meet the stringent energy resolution and sensitivity requirements demanded by mid-term astronomy missions. The development of adiabatic demagnetization refrigeration (ADR) materials that can efficiently cool from the passive radiative cooling limit of approx. 30 K down to sub-Kelvin under low magnetic fields (H less than or equal to 3 T) would represent a significant improvement in space-based cooling technology. Governed by these engineering goals, our efforts have focused on quantifying the change in magnetic entropy of rare-earth garnets and perovskites. Various compositions within the gadolinium gallium iron garnet solid solution series (GGIG, Gd3Ga(5-x)Fe(x)O12, 0.00 less than or equal to X less than or equal to 5.00) and gadolinium aluminum perovskite (GAP, GdAlO3) have been synthesized via an organometallic complex approach and confirmed with powder x-ray diffraction. The magnetization of the GGIG and GAP materials has been measured as a function of composition (0.00 less than or equal to X less than or equal to 5.00), temperature (2 K less than or equal to T less than or equal to 30 K) and applied magnetic field (0 T less than or equal to H less than or equal to 3 T). The magnetic entropy change (DeltaS(sub mag)) between 0 T and 3 T was determined from the magnetization data. In the GGIG system, DeltaS(sub mag) was compositionally dependent; Fe(sup 3+) additions up to X less than or equal to 2.44 increased DeltaS(sub mag) at T > 5 K. For GAP, DeltaS(sub mag) was similar to that of GGIG, X = 0.00, both in terms of magnitude and temperature dependence at T > 10 K. However, the DeltaS(sub mag) of GAP at T < 10 K was less than the endmember GGIG composition, X = 0.00, and exhibited maximum approx. 5 K.

King, T. T.↗
NASA NTRS2010

Electrical Switching of Perovskite Thin-Film Resistors

Electronic devices that exploit electrical switching of physical properties of thin films of perovskite materials (especially colossal magnetoresistive materials) have been invented. Unlike some related prior devices, these devices function at room temperature and do not depend on externally applied magnetic fields. Devices of this type can be designed to function as sensors (exhibiting varying electrical resistance in response to varying temperature, magnetic field, electric field, and/or mechanical pressure) and as elements of electronic memories. The underlying principle is that the application of one or more short electrical pulse(s) can induce a reversible, irreversible, or partly reversible change in the electrical, thermal, mechanical, and magnetic properties of a thin perovskite film. The energy in the pulse must be large enough to induce the desired change but not so large as to destroy the film. Depending on the requirements of a specific application, the pulse(s) can have any of a large variety of waveforms (e.g., square, triangular, or sine) and be of positive, negative, or alternating polarity. In some applications, it could be necessary to use multiple pulses to induce successive incremental physical changes. In one class of applications, electrical pulses of suitable shapes, sizes, and polarities are applied to vary the detection sensitivities of sensors. Another class of applications arises in electronic circuits in which certain resistance values are required to be variable: Incorporating the affected resistors into devices of the present type makes it possible to control their resistances electrically over wide ranges, and the lifetimes of electrically variable resistors exceed those of conventional mechanically variable resistors. Another and potentially the most important class of applications is that of resistance-based nonvolatile-memory devices, such as a resistance random access memory (RRAM) described in the immediately following article, Electrically Variable Resistive Memory Devices (MFS-32511-1).

Liu, Shangqing↗
NASA NTRS2020

Oxygen Isotopic Imaging of Refractory Inclusions from the Miller Range (MIL) 090019 CO3 Chondrite: A Perovskite Perspective

Calcium-Aluminum-rich Inclusions (CAIs) in primitive meteorites are the first solids to condense in the Solar System. The oxygen isotopic compositions recorded in various mineral components of CAIs provide clues about their origins and post-formation histories, recording processes such as condensation, melting, nebular alteration, and fluidrock reactions on the parent body. MIL 090019 is similar to some rare carbonaceous chondrites such as Acfer 094, DOM 08004/6 and ALH 77303 that contain high abundances of a variety of refractory inclusions. This provides an opportunity to study the oxygen isotopic record of different types of refractory inclusions within the same meteorite. We analyzed CAIs specifically targeting primary minerals that are direct nebular condensates, such as corundum and perovskite, with the goal of gaining insights into the O isotopic composition of the nebular gas(es) from which these CAIs condensed. As MIL 090019 is a classified as CO3.1, it shows some signs of thermal metamorphism, compared to the more primitive CO3 meteorites (e.g., DOM 08004/06). A second goal of this study is to search for evidence of nebular processes in phases such as perovskite and melilite that are susceptible to parent body alteration to varying degrees. We analyzed the oxygen isotopic compositions of various CAIs from the MIL 090019 CO3 carbonaceous chondrite by ion imaging using the NanoSIMS 50L (Nano Secondary Ion Mass Spectrometer) at JSC following methods described in. An advantage of ion imaging over traditional spot analyses is that it provides spatial context to the oxygen isotopic data. This work builds on previously reported oxygen isotopic composition of two other CAIs (CAI-44 and CAI-E2) from the same meteorite thin section.

Mane, P.↗
NASA NTRS1988

Advantages of barium peroxide in the powder synthesis of perovskite superconductors

This paper compares reaction chemistry, material processing, and material characteristics for the solid state reaction using BaCO3 or BaO2 in the synthesis of perovskite superconductors. Results are presented for weight loss and X-ray diffraction, sample morphology and homogeneity as monitored by SEM and EDS, and the superconductivity critical temperature and ac susceptibility. Greater mass density, increased sample homogeneity, lower resistance, and improved reproducibility for material are found when BaO32 is used.

Hepp, A. F.↗
NASA NTRS1992

Mg-perovskite/silicate melt partition coefficients in the CMS system at 2430 C and 226 Kbars

The partitioning of elements among lower mantle phases and silicate melts is of interest in unraveling the early thermal history of the Earth. Because of the technical difficulty in carrying out such measurements, only one direct set of measurements has been reported, and these results as well as interpretations based on them have generated controversy. The first set of direct measurements on a synthetic system in the CaO-MgO-SiO2 (CMS) is reported. An experiment was conducted at Stony Brook, using the USSA-2000 split sphere anvil apparatus. An experiment in the CMS system doped with oxides of Al, Ti, Sc, and Sm and run at a nominal temperature of 2380 C and pressure of 226 kbars is reported. Nominal temperatures were measured with a W 3 percent Re/W 25 percent Re thermocouple. The hot spot temperature, where the liquidus is located, is estimated to be at 2430 C. A 10 mm MgO octahedron was used in concert with 4 mm truncation edge lengths on the WC cubes. The sample was contained in a Re capsule which was inserted into a LaCrO3 furnace. Pressure was calibrated at 2000 C. Run duration was approximately 3 minutes. The charge was mounted in epoxy and analyzed using a CAMECA SX-50 electron microprobe. Standard operating conditions were employed, although counting time for the less abundant elements was increased to improved counting statistics. The melt is unquenchable, and forms a dendritic intergrowth of quench crystals and residual melt. It was analyzed using a 30 micron raster. The structural identity of the Mg-perovskite phase was confirmed using x ray microdiffractometry. The results of the investigation are presented.

Mcfarlane, Elisabeth A.↗
NASA NTRS1993

Experimental partitioning of Zr, Ti, and Nb between silicate liquid and a complex noble metal alloy and the partitioning of Ti between perovskite and platinum metal

El Goresy et al.'s observation of Nb, Zr, and Ta in refractory platinum metal nuggets (RPMN's) from Ca-Al-rich inclusions (CAI's) in the Allende meteorite led them to propose that these lithophile elements alloyed in the metallic state with noble metals in the early solar nebula. However, Grossman pointed out that the thermodynamic stability of Zr in the oxide phase is vastly greater than metallic Zr at estimated solar nebula conditions. Jones and Burnett suggested this discrepancy may be explained by the very non-ideal behavior of some lithophile transition elements in noble metal solutions and/or intermetallic compounds. Subsequently, Fegley and Kornacki used thermodynamic data taken from the literature to predict the stability of several of these intermetallic compounds at estimated solar nebula conditions. Palme and Schmitt and Treiman et al. conducted experiments to quantify the partitioning behavior of certain lithophile elements between silicate liquid and Pt-metal. Although their results were somewhat variable, they did suggest that Zr partition coefficients were too small to explain the observed 'percent' levels in some RPMN's. Palme and Schmitt also observed large partition coefficients for Nb and Ta. No intermetallic phases were identified. Following the work of Treiman et al., Jurewicz and Jones performed experiments to examine Zr, Nb, and Ti partitioning near solar nebula conditions. Their results showed that Zr, Nb, and Ti all have an affinity for the platinum metal, with Nb and Ti having a very strong preference for the metal. The intermetallic phases (Zr,Fe)Pt3, (Nb,Fe)Pt3, and (Ti,Fe)Pt3 were identified. Curiously, although both experiments and calculations indicate that Ti should partition strongly into Pt-metal (possibly as TiPt3), no Ti has ever been observed in any RPMN's. Fegley and Kornacki also noticed this discrepancy and hypothesized that the Ti was stabilized in perovskite which is a common phase in Allende CAI's.

Jurewicz, Stephen R.↗
NASA NTRS1999

Non-Equilibrium Superconductivity and Magnetic Pair Breaking in Perovskite Half-Metallic Ferromagnet-Insulator-Superconductor (F-I-S) Heterostructures

The effect of spin-polarized quasiparticle currents on the critical current density (J-c) of cuprate superconductors is studied in perovskite F-I-S heterostructures as a function of insulator thickness and of underlying magnetic materials. A pulsed current technique is employed to minimize extraneous Joule heating on the superconductor. At temperatures near T-c, F-I-S samples with insulator thicknesses\1e2nm show precipitous decrease in J_c as current injection (I_m) is increased. In contrast, J_c in a controlled sample with a substituted non-magnetic material (N-I-S) exhibit no dependence on I_m. Similarly, a F-I-S sample with a 10 mn insulating barrier also show little J_c effect versus I_m. At low temperatures with I_m = 0, significant suppression of J-c is observed only in the thin barrier F-I-S samples, although T_c and the normal-state resistivity of all samples are comparable. These phenomena can be attributed to the Cooper pair breaking induced by externally-injected and internally-reflected spin-polarized quasiparticle currents. We estimate an order of magnitude range for the spin diffusion length of 100 nm to 100\ mum.

Fu, C.-C.↗
NASA NTRS2012

Mineralogy and Oxygen Isotope Compositions of an Unusual Hibonite-Perovskite Refractory Inclusion from Allende

Hibonite-rich Ca- and Al-rich inclusions (CAIs) are among the earliest formed solids that condensed in the early nebula. We discovered an unusual refractory inclusion from the Allende CV3 chondrite (SHAL) containing an approx 500 micron long single crystal of hibonite and co-existing coarse-grained perovskite. The mineralogy and petrography of SHAL show strong similarities to some FUN inclusions, especially HAL. Here we report on the mineralogy, petrography, mineral chemistry and oxygen isotopic compositions in SHAL.

Keller, L. P.↗
NASA NTRS2013

Trace Element Abundances in an Unusual Hibonite-Perovskite Refractory Inclusion from Allende

Calcium-aluminum-rich refractory inclusions (CAIs) are thought to be the first-formed solids in the Solar protoplanetary disk and can provide information about the earliest Solar System processes (e.g., [1]). A hibonite-perovskitebearing CAI from the Allende CV3 chondrite (SHAL, [2]) contains a single of 500 micrometers hibonite grain and coarse-grained perovskite. The mineralogy and oxygen isotopic composition of this CAI shows similarities with FUN inclusions, especially HAL [2]. Here we present trace element abundances in SHAL.

Mane, Prajkta↗
NASA NTRS2014

Temperature and Pressure Sensors Based on Spin-Allowed Broadband Luminescence of Doped Orthorhombic Perovskite Structures

Systems and methods that are capable of measuring pressure or temperature based on luminescence are discussed herein. These systems and methods are based on spin-allowed broadband luminescence of sensors with orthorhombic perovskite structures of rare earth aluminates doped with chromium or similar transition metals, such as chromium-doped gadolinium aluminate. Luminescence from these sensors can be measured to determine at least one of temperature or pressure, based on either the intense luminescence of these sensors, even at high temperatures, or low temperature techniques discussed herein.

Eldridge, Jeffrey I.↗
NASA NTRS2017

The Beryllium-10 Abundance in an Unusual Hibonite-Perovskite Refractory Inclusion from Allende: Implications for the Origin of Be-10

Beryllium-10 (decays to B-10, t1/2 = t(sub 1/2) = 1.3 Myr) 1.3 Myr) is a radionuclide that exclusively requires a is a radionuclide that exclusively requires a spallation origin. Therefore, one could obtain important insights into the irradiation environment in the solar nebula by understanding the distribution and abundance of this radionuclide in meteoritic inclusions. Most previous data are derived from B isotopic analysis of coarse-grained CV3 Ca-Al-rich Inclusions (CAIs) that have AL-26.Al-27 Al close to the canonical level of 5 x 10 (exp -5) and inferred Be-10/Be-9 ratios between 4 x 10(exp -4) and 1 x 10 (exp -2=3) [1-5]. Al-26-depleted FUN (Fractionaed and Unknown Nuclear anomalies) CAIs are less studied due to their rarity. FUN CAIs are thought to have formed prior to homogenization of Al-26/Al-27 Al and stable isotope anomalies (e.g., Ti-50) in the solar nebula, and thus represent one of the oldest Solar System solids [6]. So far, only three FUN CAIs (Axtell 2771, KT-1 and HAL) from CV3 chondrites have been measured for Be-10. They are characterized by variable Be-10/Be-9 ratios between (2.7−4.4) × 10(exp -4) [4,7]. Another group of rare, Al-26-free and and isotopically more anomalous inclusions, namely platy hibonite crystals (PLACs) from CM2 chondrites, have well-defined Be-10/Be-9 = (5.3 +/- 1.0) x 10 (exp -4) [9]. Al-26-free CAIs appear to have lower Be-1-/Be-9 than Al-26-bearing CAIs, although large analytical errors associated with some data would allow for an apparent overlap. It has been argued that the observed Be-10 variation resulted from the in-situ production of this radionuclide in CAIs (or their precursors) by irradiation, and the ratio difference simply reflects the fluctuation in projectile fluences [e.g., 9]. Another observation in support of this explanation comes from these CAIs' initial B-10/B-11 ratios, most of which are higher than the chondritic value 0.2478 [10]. This has been interpreted as a result of mixing between spallogenic B (B-10/B-11 = 0.4, co-produced with Be-10 in the irradiated solids) and a chondritic component [5,8]. Alternatively, given that all the inferred ratios, most of which are higher than chondritic value 0.2478 [10]. This has been interpreted as a result of mixing between spallogenic B (B-10/B-11 = 0.4, co-produced with Be-10 in the irradiated solics) and a chondritic component [5,8], Alternatively, given that all the inferred ratios in CAIs never fall below 3x10(exp -4), it has been proposed that the Solar System formed with baseline Be-10/Be-9 at this level, which originated from cosmic ray irradiation of the parental molecular cloud, and any value higher than this is a result of additional in-situ spallation [4,11]. Although not explicitly stated in this model, one would expect that inclusions that incorporated the background Be-10 abundance should form with the chondritic B isotopic ratio. However, the three FUN CAIs all have supra-chondritic B-10/B-11 indicative of the presence of a spallogenic component. To test whether some Be-10 did come into the solar nebula by inheritance,a better understanding of Be-10/Be-9 and initial B-10/B-11 in Al-26-free isotopically anomalous samples is needed. Here we present the result of Be10−B-10 system in an unsual hibonite-perovskite inclusion SHAL (son of HAL) from Allende.

Liu, M-C.↗
NASA NTRS2019

Distorted Perovskites for High Voltage Dielectric Capacitors

There are several mechanisms which have been proposed for the existence of colossal dielectric constant in the class of perovskite calcium copper titanate (CaCu3Ti4O12 or CCTO) materials. Researches indicate that existence of twinning parallel to (100) (001) and (010) planes causes planar defects and causes changes in local electronic structure. This change can cause insulating barriers locally which contribute to the large dielectric values irrespective of processing. The combination of insulating barriers, defects and displacements caused by twinning have been attributed to the generation of large dielectric constant in CCTO. To examine some of these arguments some researchers replaced Ca with other elements and evaluated this concept. In this study we present the synthesis and characterization of Ga2/3Cu3Ti4O12-xNx (GCTON) material. This provides both distortion due to atomic size difference and defects due to insertion of nitrogen. The morphology of the compound was determined to show that processing has tremendous effect on the dielectric values. The resistivity of GCTON was several order higher than CCTO and dielectric constant was higher than 10,000.

Gill, Puneet↗
NASA NTRS2020

Structural evolution, electrochemical kinetic properties, and stability of A-site doped perovskite Sr(1-x)Yb(x)CoO(3-δ)

Mixed ionic and electronic conducting (MIEC) perovskite SrCoO(3-δ) is a widely studied (electro)catalyst for the oxygen reduction reaction (ORR) and possesses different crystal structures at different temperatures. These temperature dependent phase transitions significantly impact the ordering of oxygen vacancies and electrochemical kinetic properties as well as the reliability of the related devices. Some of the crystal structures formed, e.g. hexagonal phases, turn out to be almost impermeable to oxygen gas. Therefore, it is important to stabilize the crystal structure of SrCoO(3-δ) that favors the ORR over a wide temperature range. Herein, the partial substitution of the A-site Sr with Yb is systematically studied, including synthesis, characterization and analysis of structural evolution, electrochemical kinetic properties, thermal stability, and stability in a CO2-containing atmosphere. The results indicate that Sr(0.90)Yb(0.10)CoO(3-δ) is able to stabilize the tetragonal crystal structure with less ordered oxygen vacancies, leading to polarization resistances of 0.051, 0.115 and 0.272 U sq.cm at 750, 700 and 650 °C, respectively, on symmetrical cells. Sr(0.90)Yb(0.10)CoO(3-δ) demonstrates a very stable surface oxygen vacancy distribution and electronic structure near oxygen vacancies but dissociation of adsorbed oxygen molecules into atomic oxygen is affected by surface Sr segregation, and polarization resistance degradation is mainly induced by surface Sr segregation. Furthermore, Sr(0.90)Yb(0.10)CoO(3-δ) exhibits excellent thermal stability as well as excellent recovery stability and improved polarization performance after a few pure air/CO2-containing air treatment cycles at 700 °C. However, a hysteresis behavior of polarization performance is observed at 650 °C during gas cycling treatment, which may cause long-term degradation of the Sr(0.90)Yb(0.10)CoO(3-δ) electrode. The different polarization behaviors during gas cycling treatment are induced by different sensitivities of the formed surface strontium carbonate and chemisorbed surface oxo-carbonaceous species to different operating temperatures.

electrochemical kinetic↗
NASA NTRSDate not supplied

Compositional Clues to the Origin of Refractory Metal Nuggets, Perovskite, and Zr-Rich Oxides in Hibonite from the Paris Cm Chondrite

Rare Ca-Al-rich inclusions (CAIs) in carbonaceous chondrites are dominated by Zr-, Sc-, Ti-,and/or Y-rich oxides and silicates, and often contain refractory metal nuggets (RMNs)[1-3]. These phases have ultra refractory (UR) rare earth element (REE)patterns that are complementary to Group II patterns[4]. Therefore, studies of such UR CAIs likely decipher a record of nebular conditions and processes at higher temperatures than other CAIs consisting mainly of spinel and melilite. Our previous TEM analyses reported a discovery of the assemblages of RMNs, perovskite, and Zr-rich oxides in hibonite from the Paris CM chondrite[5]. Here we present TEM results of a detailed chemical study of these UR phases to provide clues to their formation conditions in the early solar nebula.

J Han↗