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Decreasing membrane thickness reduces the reaction time for the competing amine-H 2 S and amine-CO 2 reactions, thus enhancing the selectivity for the “faster”, kinetically favored product, i.e. , hydrosulfide.
Procedure for the formation of aminoacyl esters of monoribonucleotides with aminoacyl imidazolides were first reported by Gottikh et al. (1970) and summarized in 1970. This reaction has been widely used by us and numbers of other workers as a convenient means of preparing aminoacyl esters of nucleotides. We have previously reported that, under conditions of excess imidazolide, large amounts of bis 2', 3' esters are formed in addition to the monoesters. However, to our knowledge, no one has reported that in addition to the esters, relatively large amounts of the mixed anhydride, with the amino acid carboxyl attached to the phosphate, are also formed at short reaction times. We report here on the relative amounts of anhydride and esters formed in this reaction of racemic mixtures of eleven N-acetyl amino acid imidazolides with 5'-AMP and discuss the relevance of the findings to the origin of protein synthesis.
Lunar regolith will be used for a variety of purposes such as oxygen and propellant production and manufacture of various materials. The design and development of chemical conversion reactors for processing lunar regolith will require an understanding of the coupling among the chemical, mass and energy transport processes occurring at the length and time scales of the overall reactor with those occurring at the corresponding scales of the regolith particles. To this end, a coupled transport model is developed using, as an example, the reduction of ilmenite-containing regolith by a continuous flow of hydrogen in a flow-through reactor. The ilmenite conversion occurs on the surface and within the regolith particles. As the ilmenite reduction proceeds, the hydrogen in the reactor is consumed, and this, in turn, affects the conversion rate of the ilmenite in the particles. Several important quantities are identified as a result of the analysis. Reactor scale parameters include the void fraction (i.e., the fraction of the reactor volume not occupied by the regolith particles) and the residence time of hydrogen in the reactor. Particle scale quantities include the time for hydrogen to diffuse into the pores of the regolith particles and the chemical reaction time. The paper investigates the relationships between these quantities and their impact on the regolith conversion. Application of the model to various chemical reactor types, such as fluidized-bed, packed-bed, and rotary-bed configurations, are discussed.
Lunar regolith will be used for a variety of purposes such as oxygen and propellant production and manufacture of various materials. The design and development of chemical conversion reactors for processing lunar regolith will require an understanding of the coupling among the chemical, mass and energy transport processes occurring at the length and time scales of the overall reactor with those occurring at the corresponding scales of the regolith particles. To this end, a coupled transport model is developed using, as an example, the reduction of ilmenite-containing regolith by a continuous flow of hydrogen in a flow-through reactor. The ilmenite conversion occurs on the surface and within the regolith particles. As the ilmenite reduction proceeds, the hydrogen in the reactor is consumed, and this, in turn, affects the conversion rate of the ilmenite in the particles. Several important quantities are identified as a result of the analysis. Reactor scale parameters include the void fraction (i.e., the fraction of the reactor volume not occupied by the regolith particles) and the residence time of hydrogen in the reactor. Particle scale quantities include the time for hydrogen to diffuse into the pores of the regolith particles and the chemical reaction time. The paper investigates the relationships between these quantities and their impact on the regolith conversion. Application of the model to various chemical reactor types, such as fluidized-bed, packed-bed, and rotary-bed configurations, are discussed.
Man's reactions to vibration are emphasized rather than his reactions to the vibrational characteristics of vehicles. Vibrational effects studies include: performance effects reflected in tracking proficiency, reaction time, visual impairment, and other measures related to man's ability to control a system; physiological reactions; biodynamic responses; subjective reactions; and human tolerance limits. Technological refinements in shaker systems and improved experimental designs are used to validate the data.
The Psychomotor Vigilance Task (PVT) is considered the gold standard fatigue detection device and is used frequently in fatigue research. The purpose of this study was to compare a psychomotor vigilance task developed for use on touchscreen devices with the original PVT-192 in conditions of acute sleep loss and circadian desynchronization. Participants arrived in the lab approximately two hours after their habitual time and were asked to stay awake for up to 24 hrs and take 5-minute reaction time tests every 2 hours on two different devices: the original PVT-192 and NASA-PVT on an iPod. We found that the NASA-PVT and PVT-192 were sensitive to the 24 hrs of extended wakefulness.
BACKGROUND Manual control during exploration spaceflight consists of both planned automated supervisory control and unplanned crew override. This crew override capability is critical to enable overall mission success during landing contingencies. However, the introduction of manual override capabilities must be implemented to enable crews to mitigate risks introduced by human error. Adaptive changes in the sensorimotor system can manifest during g-transitions as spatial disorientation. While training and landing aids enable successful landing through disorientation, these adaptive changes may increase cognitive demand that needs to be accounted for in the manual control strategy. It is important to characterize these effects as soon as possible following the G-transition to develop appropriate countermeasures. METHODS The following study seeks to inform the risk associated with altered sensorimotor and vestibular function impacting critical mission tasks. We aim to characterize the effects of short and long-duration weightlessness on manual control following G-transitions using simulated lunar landing on a six-degree-of-freedom (6DOF) motion base, a fixed base simulation, and a supervisory control tablet task. The primary goal is to understand the impact of spaceflight on crew ability to perform manual crew override and supervisory control. This aim will be assessed by comparing pre- versus postflight simulation performance in crewmembers assigned to either short duration (< 30 day) or long duration (~6- month) missions to the International Space Station (ISS). We hypothesize there will be postflight increases in the percent time that pilots are outside of the acceptable range for recommended vehicle state parameters and the reaction time for secondary cognitive tasks. Ground-based control subjects, who are demographically matched to the crew considering age (± 5 years) and gender, will undergo the same testing schedule as the crew to examine the effects of flight phase independent of microgravity exposure. The second aim is to examine how adaptive changes in vestibular and cognitive function relate to changes in manual crew override proficiency. Crew performance for a sensorimotor perceptual test battery will evaluate motion perception tracking, roll nulling, and/or vection sensitivity using the 6DOF motion base. We hypothesize that a higher severity of vestibular alterations will be associated with increased percent time outside of guidance limits. Motion sickness severity and sleepiness will also be evaluated. To determine the impact of “just-in-time” training, the third aim seeks to compare performance during on-board lunar landing tasks conducted late in-flight to early postflight. We hypothesize that proficiency on the “just-in-time” laptop trainer late in mission will be positively correlated with early postflight proficiency on the same task. The final aim will establish assessments of performance, training protocols, and the learning progression in a ground-control cohort of first-time users. RESULTS The assessment of the learning progression associated with the piloting task on the motion base system with thirty ground subjects will be reported. Learning curves will be established across four distinct sessions and within session considering trial difficulty. The difficulty of the landing task can be modulated with the landing divert distance and cross or downrange difficulty. Results may include changes in performance across multiple trials of a multi-attribute lunar tablet supervisory control task. Preliminary investigations of eighteen subjects who completed vestibular threshold and motion perception tasks offer expected performance ranges for upcoming preflight crew evaluations. The results yielded an average roll threshold of 0.46 ± 0.30 deg/s and an average roll nulling root mean square error performance of 2.52 ± 0.52 deg/s. RELEVANCE This project will deliver an operational demonstration of crew monitoring capability following spaceflight and identify potential deficits that may require remediation. Comparison of individual vestibular and cognitive changes with crew performance will help better characterize the manual control risks associated with sensorimotor alterations. Ground testing will evaluate learning progression, refine training protocols, and serve as a control cohort for comparisons to crew performance. ACKNOWLEDGEMENTS: The authors acknowledge contributions from Draper, the Dynamic Skills Trainer (DST) Lab, and the Software, Robotics, and Simulation Division toward the development of the lunar landing simulation platforms. This project is funded by the Human Health Countermeasures Element.
A one dimensional compensatory tracking task and a digit processing reaction time task were combined in a three phase experiment designed to investigate tracking performance in time sharing. Adaptive techniques, elaborate feedback devices, and on line standardization procedures were used to adjust task difficulty to the ability of each individual subject and manipulate time sharing demands. Feedback control analysis techniques were employed in the description of tracking performance. The experimental results show that when the dynamics of a system are constrained, in such a manner that man machine system stability is no longer a major concern of the operator, he tends to adopt a first order control describing function, even with tracking systems of higher order. Attention diversion to a concurrent task leads to an increase in remnant level, or nonlinear power. This decrease in linearity is reflected both in the output magnitude spectra of the subjects, and in the linear fit of the amplitude ratio functions.
The temporal dynamics of the spatial scaling of attention during visual search were examined by recording event-related potentials (ERPs). A total of 16 young participants performed a search task in which the search array was preceded by valid cues that varied in size and hence in precision of target localization. The effects of cue size on short-latency (P1 and N1) ERP components, and the time course of these effects with variation in cue-target stimulus onset asynchrony (SOA), were examined. Reaction time (RT) to discriminate a target was prolonged as cue size increased. The amplitudes of the posterior P1 and N1 components of the ERP evoked by the search array were affected in opposite ways by the size of the precue: P1 amplitude increased whereas N1 amplitude decreased as cue size increased, particularly following the shortest SOA. The results show that when top-down information about the region to be searched is less precise (larger cues), RT is slowed and the neural generators of P1 become more active, reflecting the additional computations required in changing the spatial scale of attention to the appropriate element size to facilitate target discrimination. In contrast, the decrease in N1 amplitude with cue size may reflect a broadening of the spatial gradient of attention. The results provide electrophysiological evidence that changes in the spatial scale of attention modulate neural activity in early visual cortical areas and activate at least two temporally overlapping component processes during visual search.
Binary pnictogen chalcogen compounds, primarily bismuth tellurides and selenides, are of great interest due to their applications in emerging quantum devices, as well as thermoelectric generators. The performance of bismuth telluride in these roles depends on its structure at the nanoscale, particularly the size, shape, and crystallinity of its nanocrystalline forms. However, current methods for controlling these features are often slow, inconsistent, or difficult to scale. Here, we demonstrate that through a solvothermal synthesis and hot injection process, precise control over the morphology of bismuth telluride nanoplates is possible with independent tuning of process variables, such as temperature and reaction time. We find that the nanoplate shape and internal porosity vary systematically with synthesis temperature and that the same morphological outcomes can be rapidly achieved at a fixed temperature by adjusting reaction duration. These results reveal that both the temperature and time can independently direct bismuth telluride morphological features, allowing for rapid, tunable synthesis strategies. Our approach offers a scalable framework, not only for bismuth telluride but also for related layered chalcogenides used in energy harvesting and quantum technologies.
Deconstruction of polyolefins into functionalized macromonomers presents a compelling strategy for polyolefin upcycling by creating macromonomers through dehydrogenation/depolymerization. We show that nitrous oxide (N 2 O), a greenhouse gas waste product from the production of nylon, mediates the deconstruction of polycyclooctene (PCOE) and generates carbonyl-functionalized macromonomers. Carbonyl incorporation and macromonomer molar mass were well controlled by reaction time, and subsequent hydrogenation readily removed residual carbon-carbon double bonds. Here, we also demonstrated that the reaction could progress efficiently with substrates of moderate levels of unsaturation, closely mimicking partially dehydrogenated polyethylene. Such carbonyl-functionalized macromonomers could serve as feedstock for preparing vitrimers and other functional polymers.
Limited proteolysis promotes aggregation/gelation of plant proteins, but its relationship with the molecular characteristics of hydrolysates remains poorly understood. In here, response surface methodology was employed to evaluate the effects of protein concentration, Alcalase level, and hydrolysis time on the storage modulus (G′) of pea protein hydrolysates (PPH). 7.5% protein, 1.65% Alcalase, and a 6-min reaction time resulted in the highest relative increase in G′ upon heating PPH, whereas both higher (3.55%) and lower (0.3%) Alcalase levels led to less increment. Increasing the Alcalase level increased the degree of hydrolysis while decreasing the molecular weight, surface hydrophobicity, and total sulfhydryl and disulfide bond contents of PPH. Confocal laser scanning microscopy and X-ray scattering analyses found PPH produced with 1.65% Alcalase formed interconnected aggregates with dual structural domains, but not at other Alcalase conditions. These results demonstrate the role of controlled proteolysis in governing the aggregation/gelation behavior of PPH.
The objective of this contrast was to optimize and scale-up the synthesis of 2,2-bis(4-aminophenyl)-hexafluoropropane and 1,3-bis(4-aminophenyl)hexafluoropropane, as well as to explore avenues to other perfluoroalkyl-bridged dianilines. Routes other than Friedel-Crafts reaction leading to 2,2-bis(4-aminophenyl)hexafluoropropane were investigated. The processes utilizing bisphenol-AF were all unsuccessful; reactions aimed at the production of 4-(hexafluoro-2-halo-isopropyl)aniline from the hydroxyl intermediate failed to yield the desired products. Tailoring the conditions of the Friedel-Crafts reaction of 4-(hexafluoro-2-hydroxyisopropyl)aniline, aniline, and aluminum chloride by using hydrochloride salts and selecting optimum reagent ratios, reaction times, and temperature resulted in approx. 20% yield of pure crystallized 2,2-bis(4-aminophenyl)hexafluoropropane in 0.2 mole reaction batches. Yields up to approx. 40% were realized in small, approx. 0.01 mole, batches. The synthesis of 1,3-bis(4-aminophenyl)hexafluoropropane starting with perfluoroglutarimidine was reinvestigated. The yield of the 4-step reaction sequence giving 1,3-bis(4-acetamidophenyl)hexafluoropropane was raised to 44%. The yield of the subsequent hydrolysis process was improved by a factor of approx. 2. Approaches to prepare other perfluoroalkyl-bridged dianilines were unsuccessful. Reactions reported to proceed readily with trifluoromethyl substituents failed when longer chain perfluoroalkyl groups were employed.
A chemical kinetic mechanism is proposed for the combustion of silane-hydrogen-oxygen-nitrogen mixtures in the initial temperature range from 800K to 1250K and pressure range from 0.5 to 1.35 atm. The mechanism yields results which are in agreement with published ignition delay times obtained from shock tube experiments. Comparisons between the results obtained using the proposed mechanism and that of an alternative mechanism reveal that the former predicts appreciably shorter ignition delay times, but a flame blowout envelope which is shifted so as to decrease the stable flame region. Over much of the thermodynamic range examined, the mechanism predicts long reaction times. A three step global mechanism is proposed which closely models the ignition phase of SiH4 - H2 - air combustion; however, the reaction phase is less well reproduced by the global model. The necessity for additional experimental data to further assess the proposed models is stressed.
The electrochemical CO 2 reduction reaction (CO 2 RR) holds enormous potential as a carbon-neutral route to the sustainable production of fuels and platform chemicals. The durability for long-term operation is currently inadequate for commercialization, however, and the underlying deactivation process remains elusive. A fundamental understanding of the degradation mechanism of electrocatalysts, which can dictate the overall device performance, is needed. In this work, we report the structural dynamics and degradation pathway of Cu oxide nanoparticles (CuO x NPs) during the CO 2 RR by using in situ small-angle X-ray scattering (SAXS) and X-ray absorption spectroscopy (XAS). The in situ SAXS reveals a reduction in the size of NPs when subjected to a potential at which no reaction products are detected. At potentials where the CO 2 RR starts to occur, CuO x NPs are agglomerated through a particle migration and coalescence process in the early stage of the reaction, followed by Ostwald ripening (OR) as the dominant degradation mechanism for the remainder of the reaction. As the applied potential becomes more negative, the OR process becomes more dominant, and for the most negative applied potential, OR dominates for the entire reaction time. The morphological changes are linked to a gradual decrease in the formation rate for multicarbon products (C 2 H 4 and ethanol). Other reaction parameters, including reaction intermediates and local high pH, induce changes in the agglomeration process and final morphology of the CuO x NPs electrode, supported by post-mortem ex situ microscopic analysis. The in situ XAS analysis suggests that the CuO x NPs reduced into the metallic state before the structural transformation was observed. The introduction of high surface area carbon supports with ionomer coating mitigates the degree of structural transformation and detachment of the CuO x NPs electrode. These findings show the dynamic nature of Cu nanocatalysts during the CO 2 RR and can serve as a rational guideline toward a stable catalyst system under electrochemical conditions.
The independence of information load (Hick's Law) and movement precision (Fitts' Law) was tested using additive factors methodology. Subjects were required to classify stimuli according to a decision rule with a variable entropy. The stimuli were presented in the center of the CRT screen. In response, subjects had to move a cursor from a starting point near the stimulus to the appropriate target. The precision of the response movement was varied by manipulating the ratio of the radius of the annulus to the width of the target area. The dependent measure was elapsed time between onset of the stimulus and completion of the response movement. Independence of the Hick's Law and Fitts' Law components of the reaction time was tested with an analysis of variance. Presence of an interaction would suggest that a decision stage and a response stage are dependent, and cannot be considered discrete steps in a serial process.
Chemical and mechanical processes are coupled in many geological and geochemical environments. Reactive processes anneal defects and restructure grain boundaries, modifying their elastic properties, levels of internal friction, wave propagation rates and fracture behaviors. The nature of these changes is, however, contingent on the initial state of the rock. Here, in this study, impulse excitation was used to measure changes in mechanical properties as a function of dry and steam heating time at 300 °C for three carbonate rocks: Carrara marble, Carthage marble (Burlington Limestone), and Texas Cream limestone (Edwards limestone), with initial porosities of about 1 %, 3 %, and 27 %, respectively. Frequency-dependent phenomena along with mineral recrystallization were observed. This was coupled with small-angle X-ray and neutron scattering analysis to determine the relationship between changes in bulk mechanical and microstructural properties. An observed decrease in both the Young's and shear moduli in the experimental limestones as a function of heating time reflects and quantifies a reduction in the stiffness of the rock due to annealing. The internal friction of the samples first increases then decreases with reaction time, reflecting defect annealing, but this was balanced against grain boundary dissolution apparently driven by condensation of steam in the confined grain-boundary environment. This suggests an increase in the boiling point under confinement leading to dissolution, increased porosity and widening of the grain boundaries. In addition, comparison of small-angle X-ray and neutron scattering results suggests that it is inappropriate to assume that pores are empty for quantitative analysis of typical small-angle scattering samples.
This paper is part of an integrated study by NASA and the NNSA to quantitatively understand the response timeframe should a threatening Earth-impacting near-Earth object (NEO) be identified. The two realistic responses considered are the use of a spacecraft functioning as either a kinetic impactor or a nuclear explosive carrier to deflect the approaching NEO. The choice depends on the NEO size and mass, the available response time prior to Earth impact, and the various uncertainties. Whenever practical, the kinetic impactor is the preferred approach, but various factors, such as large uncertainties or short available response time, reduce the kinetic impactor's suitability and, ultimately, eliminate its sufficiency. Herein we examine response time and the activities that occur between the time when an NEO is recognized as being a sufficient threat to require a deflection and the time when the deflection impulse is applied to the NEO. To use a kinetic impactor for successful deflection of an NEO, it is essential to minimize the reaction time and maximize the time available for the impulse delivered to the NEO by the kinetic impactor to integrate forward in time to the eventual deflection of the NEO away from Earth impact. To shorten the response time, we develop tools to survey the profile of needed spacecraft launches and the possible mission payloads. We further present a vehicle design capable of either serving as a kinetic impactor, or, if the need arises, serving as a system to transport a nuclear explosive to the NEO. These results are generated by analyzing a specific case study in which the simulated Earth-impacting NEO is modeled very closely after the real NEO known as 101955 Bennu (1999 RQ36). Bennu was selected for our case study in part because it is the best-studied of the known NEOs. It is also the destination of NASA's OSIRIS-REx sample return mission, which is, at the time of this writing, enroute to Bennu following a September 2016 launch.