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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 NTRS1977

Simplified methods for calculating photodissociation rates

Simplified methods for calculating the transmission of solar UV radiation and the dissociation coefficients of various molecules are compared. A significant difference sometimes appears in calculations of the individual band, but the total transmission and the total dissociation coefficients integrated over the entire SR (solar radiation) band region agree well between the methods. The ambiguities in the solar flux data affect the calculated dissociation coefficients more strongly than does the method. A simpler method is developed for the purpose of reducing the computation time and computer memory size necessary for storing coefficients of the equations. The new method can reduce the computation time by a factor of more than 3 and the memory size by a factor of more than 50 compared with the Hudson-Mahle method, and yet the result agrees within 10 percent (in most cases much less) with the original Hudson-Mahle results, except for H2O and CO2. A revised method is necessary for these two molecules, whose absorption cross sections change very rapidly over the SR band spectral range.

Shimazaki, T.↗

NASA NTRS1983

Modelling atmospheric aerosol backscatter at CO2 laser wavelengths. I - Aerosol properties, modeling techniques, and associated problems. II - Modeled values in the atmosphere. III - Effects of changes in wavelength and ambient conditions

The various methods of calculating the atmospheric aerosol backscattering function, beta(CO2), both from measured aerosol characteristics and from optical measurements made at other wavelengths, are discussed in detail, with limits placed on their accuracy. The most significant factor in determining beta(CO2) is found to be the aerosol size distribution and concentration; this should be known accurately for particle radii up to at least 1 micron for stratospheric particles and 5 microns for tropospheric particles. Results are then presented from the modeling of the aerosol backscattering function at a wavelength of 10.6 microns in the lowest 20 km of the atmosphere. It is found that beta(CO2) varies from 10 to the -6th per m per sr in the planetary boundary layer to less than 10 to the -11th per m per sr in the stratosphere. It is next shown that, with the exception of (NH4)2SO4-containing aerosols, whose size distributions have relatively large numbers of small particles, the variation of backscattering with CO2 wavelength is less than a factor of approximately 3. For such (NH4)2SO4 aerosol distributions, however, the variation of backscatter function with CO2 wavelengths between 9.1 and 11.1 microns may reach one order of magnitude.

Kent, G.S.↗

NASA NTRS1985

Results from the UCSD magnetic monopole search

The energy loss mechanism for slowly moving magnetic monopoles in helium provides a means of extending the search for such particles by ionization techniques to velocities approximately 3 X 1 million cm/sec (beta approximately equals 0.0001). Other gases (e.g., CH2 or CO2) mixed with helium will be ionized with high efficiency by collisions with excited helium atoms, thus allowing the use of large proportional chamber systems for the detection of the monopoles. The first reported results utilizing this mechanism was the experiment of Kajino, et al., using a detector with an area-solid angle product alpha time delta alpha of 24.7 square meters sr. They set a limit on the flux of monopoles of 7.2 x 10 to the 13th power cm(-2) sr(-1) sec(-1) at a 90% confidence level for beta 3x 0.0001. Here, the results of a He:CH2 proportional tube array designed to extend the velocity limit down to beta approximately 0.0001 are reported. The detector which has been operating at the University of California, San Diego (UCSD) since last summer, is a prototype for a larger array currently under construction at UCSD. The data presented here is from 200 days of live time with the prototype detector.

Masek, G. E.↗

NASA NTRS1991

Aerosol backscatter measurements at 10.6 microns with airborne and ground-based CO2 Doppler lidars over the Colorado High Plains. II - Backscatter structure

Measurements of tropospheric aerosol volume backscatter coefficients at 10.6-microns wavelength were obtained with airborne continuous wave and ground-based pulsed CO2 Doppler lidars over the Colorado High Plains during a 20-day period in summer 1982. A persistent 'background' layer was found between 6- and 10-km altitude, with a generally uniform backscatter mixing ratio of about 10 to the -10th sq m/kg per sr. The upper boundary of this background layer varied with the tropopause height; the lower boundary varied with the strength and diurnal cycle of convective mixing in the planetary boundary layer (PBL). For quiescent meteorological conditions, the transition from the PBL to the background layer was usually very sharp, with backscatter decreases sometimes as large as 3 decades in about 70 m. Sharp gradients were also found at the boundaries of shallow (tens of meters) subvisible cirrus clouds. For less stable conditions, associated with vertical aerosol transport by deep cumuliform clouds, backscatter tended to decrease exponentially with altitude.

Bowdle, David A.↗

NASA NTRS1999

Investigating the Martian Environment with the Mars Global Surveyor Thermal Emission Spectrometer

The Thermal Emission Spectrometer (TES) onboard Mars Global Surveyor (MGS) is being used to investigate the surface and atmosphere of Mars and the martian moons Phobos and Deimos. As such, it builds upon infrared observations obtained by previous spacecraft, e.g.. Mariner 9 and Viking Orbiters. The objectives of the TES experiment are: (1) determine and map surface minerals. rocks. and ices; (2) study the atmospheric dust composition. particle size, and spatial and temporal distribution; (3) investigate condensate clouds, CO2 and H2O, location. temperature, and height; (4) investigate polar cap deposits, e.g., growth, retreat, and energy balance; (5) measure the thermo-physical properties of surface materials; and (6) characterize the atmospheric structure and dynamics. The TES instrument is based upon a Michelson interferometer and collects data in the 1700-200 per cm region (about 6-50 micron at 5 or 10 per cm resolution. There are also broad-band bolometric (4.5100 microns and solar reflectance (0.3-2.7 microns) channels. The TES was designed to have a noise equivalent spectral radiance of 1.2 x l0(exp -8) per W per square cm per sr per cm corresponding to a signal-to-noise ratio of 490 at 1000 per cm (10 mm) for a 270 K scene and preflight data suggest a radiometric accuracy of about 1.2 x 10(exp -8) per W per square cm per sr per cm. In-flight observations indicate a small systematic calibration offset of about 1.2 x 10(exp -7) per W per square cm per sr per cm is present in the TES data. MGS achieved Mars orbital insertion September 11, 1997, and entered the initial aerobraking phase. MGS should have reached a circular orbit by early 1998. However, structural damage to one solar panel occurred during its deployment in the cruise phase and ultimately required an assessment of the extent of the damage and a much slower aerobraking period. This has delayed reaching the final circular orbit until March 1999. TES and the other MGS science instruments began operating just after orbital insertion and continued to obtain data until November 1998 when the TES was turned off to reduce power consumption on the spacecraft. TES data obtained during orbits 2 to 53 have previously been published and clearly illustrate the variety of scientific questions that can be addressed with them.

Roush, T. L.↗

NASA NTRS1988

Deccan volcanism at the Cretaceous-Tertiary boundary

The accuracy with which one can claim that Deccan trap volcanism occurred at the Cretaceous-Tertiary boundary (KTB) over a very short time interval is of key importance in deciding whether a volcanic origin of the KTB events should be taken seriously. In the two years since paleomagnetic, paleontological and geodynamic evidence was published, further data have become available and the case now appears to be well constrained. The Ar-40/Ar-39 results from six labs have yielded some 24 reliable plateau ages that narrow the age range to 65 to 69 Ma. Moreover, it appears that a significant part of this range results from inter-lab spread and possible minor alteration. Paleontology demonstrates that volcanism started in the Maestrichtian, more precisely in the A. mayaroensis zone. Paleomagnetism shows that volcanism spanned only 3 chrons and only one correlation remains possible, that of the main central reversed chron with 29R. Therefore, whereas Ar-40/Ar-39 is able only to restrict the duration of volcanism to some 4 Ma, paleomagnetism restricts it to 0.5 Ma. Using some geochemical indicators such as C-13 as proxy, it is suggested that volcanism actually consists of a few shorter events of unequal magnitude. Extrusion rates may be as high as 100 cu km/yr and fissure lengths as long as several 100 km. Such a scenario appears to be at least as successful as others in accounting for most anomalies observed at the KTB. Particularly important are Iridium and other platinum group elements (PGE) profiles, Sr-87/Sr-86, C-13, 0-18, other exotic geochemical signatures, spherules, soot, shocked minerals, selective and stepwise extinctions. The environmental impact of CO2 possibly released during explosive phases of volcanism, and SO2 released during effusive phases, and the ability of volcanism to ensure worldwide distribution of KTB products are now all addressed. In conclusion, the case for a causal link between internal hotspot activity, birth of the Reunion hotspot itself as the Deccan and KTB events appears to rest on an increasingly stronger basis.

Courtillot, V.↗

NASA NTRS1980

The thermal decomposition of 1,3,5-trinitrohexahydro-1,3,5-triazine (RDX) and RDXd6 at high temperatures

The ballistics behavior of nitramine propellants containing RDX in an inert binder was examined. It is shown that at 2000 to 5000 psi, depending on the particle size, a slope break or discontinuity in the log burning rate versus log pressure curve occurs. It is shown that at higher pressures the nitramine decomposition proceeds predominately by C-N bond rupture and gives CH2 and N20. At still higher pressures (after the slope break) the decomposition proceeds by N-N rupture. The decomposition of RDX was investigated from 170 to 800 C at atmospheric pressure. The major decomposition products were CH2, CO, CO2, N20, N2, and H20. The ratio of the products varied with the pyrolysis rate and temperature.

Miller, P. J.↗