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Calculated rate constants for the reaction ClO + O yields Cl + O2 between 220 and 1000 deg K
Classical trajectory calculations are presented for the reaction ClO + O yields Cl + O2, a reaction which is an important step in the chlorine-catalyzed destruction of ozone which is thought to occur in the 220 and 1000 K. The calculated rate constant is 4.36 x 10 to the minus 11th power exp (-191/T)cu cm molecule (-1)s(-1) and its value at 300 K is 2.3 plus or minus 10 to the 11th power cu cm molecule (-1)s(-1), about a factor of 2 lower than recent experimental data. The empirical potential energy surface used in the calculations was constructed to fit experimental data for ClO, O2 and ClOO molecules. Other important features of this potential surface, such as the barrier to reaction, were varied systematically and calculations were performed for a range of conditions to determine the best theoretical rate constants. Results demonstrate the utility of classical trajectory methods for determining activation energies and other kinetic data for important atmospheric reactions.
A simplified reaction mechanism for calculation of emissions in hydrocarbon (Jet-A) combustion
The paper presents a simplified reaction mechanism developed for use in calculations of NO(x) emissions in Jet-A combustion. The rate for the N2 + O2 reaction was selected to match available experimental results, and the reaction rates for other global reactions in the Jet-A are empirical reaction rates adjusted to match species concentrations using the detailed mechanism of Miller and Bowman (1989). The mechanism was validated by comparing the emission of NO(x) calculated using propane as fuel.
Upper limits of the rate constants for the reactions of CFCl3/F-11/, CF2Cl2/F-12/, and N2O with OH - Estimates of corresponding lower limits to their tropospheric lifetimes
A discharge-flow system with resonance fluorescence detection of OH is used to study the reactions of CFCl3, CF2Cl2, and N2O with OH at temperatures up to 480 K. Little, if any reaction was found, with upper limits of 5, 6, and 4 x 10 to the -16th cu cm/s reported at 480 K for the three rate constants. A very simple model is used to calculate removal times exceeding 10,000 years for reaction with tropospheric OH.
Rate Constant for the Reaction CH3 + CH3 Yields C2H6 at T = 155 K and Model Calculation of the CH3 Abundance in the Atmospheres of Saturn and Neptune
The column abundances of CH3 observed by the Infrared Space Observatory (ISO) satellite on Saturn and Neptune were lower than predicted by atmospheric photochemical models, especially for Saturn. It has been suggested that the models underestimated the loss of CH3 due to poor knowledge of the rate constant k of the CH3 + CH3 self-reaction at the low temperatures and pressures of these atmospheres. Motivated by this suggestion, we undertook a combined experimental and photochemical modeling study of the CH3 + CH3 reaction and its role in determining planetary CH3 abundances. In a discharge flow-mass spectrometer system, k was measured at T = 155 K and three pressures of He. The results in units of cu cm/molecule/s are k(0.6 Torr) = 6.82 x 10(exp -11), k(1.0 Torr) = 6.98 x 10(exp -11), and k(1.5 Torr) = 6.91 x 10(exp -11). Analytical expressions for k were derived that (1) are consistent with the present laboratory data at T = 155 K, our previous data at T = 202 K and 298 K, and those of other studies in He at T = 296-298 K and (2) have some theoretical basis to provide justification for extrapolation. The derived analytical expressions were then used in atmospheric photochemical models for both Saturn and Neptune. These model results reduced the disparity with observations of Saturn, but not with observations of Neptune. However, the disparity for Neptune is much smaller. The solution to the remaining excess CH3 prediction in the models relative to the ISO observations lies, to a large extent, elsewhere in the CH3 photochemistry or transport, not in the CH3 + CH3 rate.
Venus volcanism: Rate estimates from laboratory studies of sulfur gas-solid reactions
Thermochemical reactions between sulfur-bearing gases in the atmosphere of Venus and calcium-, iron-, magnesium-, and sulfur-bearing minerals on the surface of Venus are an integral part of a hypothesized cycle of thermochemical and photochemical reactions responsible for the maintenance of the global sulfuric acid cloud cover on Venus. SO2 is continually removed from the Venus atmosphere by reaction with calcium bearing minerals on the planet's surface. The rate of volcanism required to balance SO2 depletion by reactions with calcium bearing minerals on the Venus surface can therefore be deduced from a knowledge of the relevant gas-solid reaction rates combined with reasonable assumptions about the sulfur content of the erupted material (gas + magma). A laboratory program was carried out to measure the rates of reaction between SO2 and possible crustal minerals on Venus. The reaction of CaCO3(calcite) + SO2 yields CaSO4 (anhydrite) + CO was studied. Brief results are given.
The Cassini Reaction Wheels: Drag and Spin-Rate Trends from an Aging Interplanetary Spacecraft at Saturn
The purpose of this paper is to provide a summary of the long-term trends of the estimated drag torque and spin-rates of the Cassini reaction wheel assemblies during eleven years of intensive science operations at Saturn..
Inflight Performance of Cassini Reaction Wheel Bearing Drag in 1997-2013
As the first spacecraft to achieve orbit at Saturn in 2004, Cassini has collected science data throughout its four-year prime mission (2004-08), and has since been approved for a first and second extended missions through September 2017. Cassini is a three-axis stabilized spacecraft. It uses reaction wheels to achieve high level of spacecraft pointing stability that is needed during imaging operations of several science instruments. The Cassini flight software makes in-flight estimates of reaction wheel bearing drag torque and made them available to the mission operations team. These telemetry data are being trended for the purpose of monitoring the long-term health of the reaction wheel bearings. Anomalous drag torque signatures observed over the past 15 years are described in this paper. One of these anomalous drag conditions is bearing cage instability that appeared (and disappeared) spontaneously and unpredictably. Cage instability is an uncontrolled vibratory motion of the bearing cage that can produce high-impact forces internal to the bearing that will cause intermittent and erratic torque transients. Characteristics of the observed cage instabilities and other drag torque "spikes" are described in this paper. In day-to-day operations, the reaction wheels' rates must be neither too high nor too low. To protect against operating the wheels in any undesirable conditions (such as prolonged low spin rate operations), a ground software tool named Reaction Wheel Bias Optimization Tool (RBOT) was developed for the management of the wheels. Disciplined and long-term use of this ground software has led to significant reduction in the daily consumption rate of the wheels' low spin rate dwell time. Flight experience on the use of this ground software tool as well as other lessons learned on the management of Cassini reaction wheels is given in this paper.
Alumina-supported Pd-Ag catalysts for low-temperature CO and methanol oxidation
Pd-Ag bimetallic catalysts, supported on gamma-Al2O3, have been evaluated as exhaust catalysts for methanol-fueled vehicles. Laboratory studies have shown that a 0.01% Pd-5% Ag catalyst has greater CO and CH3OH oxidation activity than either 0.01% Pd or 5% Ag catalysts alone. Moreover, Pd and Ag interact synergistically in the bimetallic catalyst to produce greater CO and CH3OH oxidation rates and lower yields of methanol partial oxidation products than expected from a mixture of the single-component catalysts. The Pd-Ag synergism results from Pd promoting the rate of O2 adsorption and reaction with CO and CH3OH on Ag. Rate enhancement by the bimetallic catalyst is greatest at short reactor residence times where the oxygen adsorption rate limits the overall reaction rate.
Self discharge of nickel-hydrogen cells
Values for the capacity loss with time, naturally on open circuit stand, and information regarding the minimum amount of circuit charge needed to keep the cell charged can be determined from the self-discharge behavior of nickel hydrogen cells. Furthermore, the rate of reaction between hydrogen and a charged nickel electrode is also open for nickel cadmium batteries. In a nickel hydrogen cell, the hydrogen is stored as pressurized gas and the cell stack with the charge that is oxidized nickel-hydroxide electrode is in direct contact with the hydrogen. Therefore, the rate of reaction can be measured easily and precisely by monitoring the charge, the change in hydrogen pressure with time. Measures made on twelve 15 ampere hour nickel hydrogen cells of different stack configurations built for COMSAT are discussed.
GCR Transport in the Brain: Assessment of Self-Shielding, Columnar Damage, and Nuclear Reactions on Cell Inactivation Rates
Radiation shield design is driven by the need to limit radiation risks while optimizing risk reduction with launch mass/expense penalties. Both limitation and optimization objectives require the development of accurate and complete means for evaluating the effectiveness of various shield materials and body-self shielding. For galactic cosmic rays (GCR), biophysical response models indicate that track structure effects lead to substantially different assessments of shielding effectiveness relative to assessments based on LET-dependent quality factors. Methods for assessing risk to the central nervous system (CNS) from heavy ions are poorly understood at this time. High-energy and charge (HZE) ion can produce tissue events resulting in damage to clusters of cells in a columnar fashion, especially for stopping heavy ions. Grahn (1973) and Todd (1986) have discussed a microlesion concept or model of stochastic tissue events in analyzing damage from HZE's. Some tissues, including the CNS, maybe sensitive to microlesion's or stochastic tissue events in a manner not illuminated by either conventional dosimetry or fluence-based risk factors. HZE ions may also produce important lateral damage to adjacent cells. Fluences of high-energy proton and alpha particles in the GCR are many times higher than HZE ions. Behind spacecraft and body self-shielding the ratio of protons, alpha particles, and neutrons to HZE ions increases several-fold from free-space values. Models of GCR damage behind shielding have placed large concern on the role of target fragments produced from tissue atoms. The self-shielding of the brain reduces the number of heavy ions reaching the interior regions by a large amount and the remaining light particle environment (protons, neutrons, deuterons. and alpha particles) may be the greatest concern. Tracks of high-energy proton produce nuclear reactions in tissue, which can deposit doses of more than 1 Gv within 5 - 10 cell layers. Information on rates of cell killing from GCR, including patterns of cell killing from single particle tracks. can provide useful information on expected differences between proton and HZE tracks and clinical experiences with photon irradiation. To model effects on cells in the brain, it is important that transport models accurately describe changes in the GCR due to interactions in the cranium and proximate tissues. We describe calculations of the attenuated GCR particle fluxes at three dose-points in the brain and associated patterns of cell killing using biophysical models. The effects of the brain self-shielding and bone-tissue interface of the skull in modulating the GCR environment are considered. For each brain dose-point, the mass distribution in the surrounding 4(pi) solid angle is characterized using the CAM model to trace 512 rays. The CAM model describes the self-shielding by converting the tissue distribution to mass-equivalent aluminum, and nominal values of spacecraft shielding is considered. Particle transport is performed with the proton, neutron, and heavy-ion transport code HZETRN with the nuclear fragmentation model QMSFRG. The distribution of cells killed along the path of individual GCR ions is modeled using in vitro cell inactivation data for cells with varying sensitivity. Monte Carlo simulations of arrays of inactivated cells are considered for protons and heavy ions and used to describe the absolute number of cell killing events of various magnitude in the brain from the GCR. Included are simulations of positions of inactivated cells from stopping heavy ions and nuclear stars produced by high-energy ions most importantly, protons and neutrons.
Electromagnetic containerless reaction of samarium with cobalt for the formation of samarium-cobalt alloys
The electromagnetic levitation technique has been used to obtain nearly stoichiometric SmCo5, with the reaction temperature controlled by a gas jet. The results of several experiments carried out at a 450 kHz, 25 kw RF power levitation facility using different reaction times and cooling rates are presented. It is shown that reaction rates achieved with the levitation technique are larger than the expected diffusion rate in the system liquid samarium-solid cobalt. It is also shown that substantial mixing occurs in the RF-levitated melt.
Rate constant measurements for the reaction Cl + CH2O yields HCl + CHO Implications regarding the removal of stratospheric chlorine
The flash photolysis resonance fluorescence technique was employed to investigate the rate constant for the reaction Cl + CH2O yields HCl + CHO from 223 to 323 K. An Arrhenius fit of the data gives a rate constant equal to (1.09 + or - 0.40) x 10 to the -10th exp/-(131 + or - 98)/T/ in units of cu cm/molecule per sec. The results are compared to two very recent kinetic studies and are assessed in view of the reaction's role in disrupting the Cl-ClO stratospheric ozone depletion chain.
Rate Constants and Temperature Dependences for the Reactions of Hydroxyl Radicals with Three
Rate constants and temperature dependences for the reactions of OH with CF3OCH3 (HFOC-.
Heterogeneous chemistry on Antarctic polar stratospheric clouds - A microphysical estimate of the extent of chemical processing
A detailed model of polar stratospheric clouds (PSCs), which includes nucleation, condensational growth. and sedimentation processes, has been applied to the study of heterogeneous chemical reactions. For the first time, the extent of chemical processing during a polar winter has been estimated for an idealized air parcel in the Antarctic vortex by calculating in detail the rates of heterogeneous reactions on PSC particles. The resulting active chlorine and NO(x) concentrations at first sunrise are analyzed with respect to their influence upon the Antarctic ozone hole using a photochemical model. It is found that the species present at sunrise are primarily influenced by the relative values of the heterogeneous reaction rate constants and the initial gas concentrations. However, the extent of chlorine activation is also influenced by whether N2O5 is removed by reaction with HCl or H2O. The reaction of N2O5 with HCl, which occurs rapidly on type 1 PSCs, activates the chlorine contained in the reservoir species HCl. Hence the presence and surface area of type 1 PSCs early in the winter are crucial in determining ozone depletion.
Mechanism and rate constant of the reaction between methylene and methyl radicals
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Absolute rate constant for the reaction of atomic hydrogen with acetylene over an extended pressure and temperature range
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