Insights into structure-composition-capacity relationship of ultrastable metal halide absorbents for ammonia separation and storage
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Mahtab, S. M. Tanveer↗
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First-Principles Molecular Dynamics Simulations of Ammonia Adsorption onto MFI Zeolite Nanosheets
MFI zeolite nanosheet membranes are promising candidates for ammonia separation from nitrogen and hydrogen gases, yet questions remain on the origin of their high selectivity. Silanols, Si–OH, are present in high concentration at the surface of zeolite nanosheets, and force-field-based simulations indicate that surface adsorption at the silanols contributes to selectivity. Acidic silanol groups can chemically react with ammonia via transfer of a proton to form ammonium ions, which may further contribute to the ability of zeolite nanosheet membranes to separate ammonia from other gases. In this work, we used first-principles molecular dynamics techniques to simulate ammonia’s behavior within stacked MFI zeolite nanosheets. We found that at 523 K and a loading corresponding to 35 bar, conditions desired for the ammonia separation, about 30% of ammonia reacts with surface silanols. Our work explored H-bonding and proton transfer within this system.
ammonia↗
First Principles Molecular Dynamics Simulations of Ammonia Adsorption onto MFI Zeolite Nanosheets
MFI zeolite nanosheets membranes are promising candidates for ammonia separation from nitrogen and hydrogen, yet questions remain on the origin of their high selectivity. Silanols, Si-OH, are present in high concentration at the surface of zeolite nanosheets, and force-field-based simulations indicate that surface adsorption at the silanols contributes to selectivity. Silanols can chemically react with ammonia, which may further contribute to the ability of zeolite nanosheet membranes to separate it from other gases. In this work, we use first-principles molecular dynamics techniques to simulate ammonia’s behavior within stacked MFI zeolite nanosheets. We find that at 523 K and a loading corresponding to 35 bar, conditions desired for the ammonia separation, about 30% of ammonia reacts with surface silanols. Our work explores H-bonding and proton transfer within this system.
36 MATERIALS SCIENCE↗
Ion mobility spectrometry of hydrazine, monomethylhydrazine, and ammonia in air with 5-nonanone reagent gas
Hydrazine (HZ) and monomethylhydrazine (MMH) in air were monitored continuously using a hand-held ion mobility spectrometer equipped with membrane inlet, 63Ni ion source, acetone reagent gas, and ambient temperature drift tube. Response characteristics included detection limit, 6 ppb; linear range, 10-600 ppb; saturated response, >2 ppm; and stable response after 15-30 min. Ammonia interfered in hydrazines detection through a product ion with the same drift time as that for MMH and HZ. Acetone reagent gas was replaced with 5-nonanone to alter drift times of product ions and separate ammonia from MMH and HZ. Patterns in mobility spectra, ion identifications from mass spectra, and fragmentation cross-sections from collisional-induced dissociations suggest that drift times are governed by ion-cluster equilibria in the drift region of the mobility spectrometer. Practical aspects including calibration, stability, and reproducibility are reported from the use of a hand-held mobility spectrometer on the space shuttle Atlantis during mission STS-37.
Flight Experiment↗
"Reagentless" flow injection determination of ammonia and urea using membrane separation and solid phase basification
Flow injection analysis instrumentation and methodology for the determination of ammonia and ammonium ions in an aqueous solution are described. Using in-line solid phase basification beds containing crystalline media. the speciation of ammoniacal nitrogen is shifted toward the un-ionized form. which diffuses in the gas phase across a hydrophobic microporous hollow fiber membrane into a pure-water-containing analytical stream. The two streams flow in a countercurrent configuration on opposite sides of the membrane. The neutral pH of the analytical stream promotes the formation of ammonium cations, which are detected using specific conductance. The methodology provides a lower limit of detection of 10 microgram/L and a dynamic concentration range spanning three orders of magnitude using a 315-microliters sample injection volume. Using immobilized urease to enzymatically promote the hydrolysis of urea to produce ammonia and carbon dioxide, the technique has been extended to the determination of urea.
NASA Center JSC↗
Development of a nitrogen generation system
An eight-stage nitrogen generation module was developed. The design integrated a hydrazine catalytic dissociator, three ammonia dissociation stages and four palladium/silver hydrogen separator stages. Alternating ammonia dissociation and hydrogen separation stages are used to remove hydrogen and ammonia formed in the dissociation of hydrazine which results in negligible ammonia and hydrogen concentrations in the product nitrogen stream. An engineering breadboard nitrogen supply subsystem was also developed. It was developed as an integratable subsystem for a central spacecraft air revitalization system. The subsystem consists of the hydrazine storage and feed mechanism, the nitrogen generation module, the peripheral mechanical and electrical components required to control and monitor subsystem performance, and the instrumentation required to interface with other subsystems of an air revitalization system. The breadboard nitrogen supply subsystem was integrated and tested with a one-person capacity experimental air revitalization system. The integration, checkout and testing was successfully accomplished.
Heppner, D. B.↗
US Navy Submarine Sea Trial of the NASA Air Quality Monitor
For the past four years, the Air Quality Monitor (AQM) has been the operational instrument for measuring trace volatile organic compounds on the International Space Station (ISS). The key components of the AQM are the inlet preconcentrator, the gas chromatograph (GC), and the differential mobility spectrometer. Most importantly, the AQM operates at atmospheric pressure and uses air as the GC carrier gas, which translates into a small reliable instrument. Onboard ISS there are two AQMs, with different GC columns that detect and quantify 22 compounds. The AQM data contributes valuable information to the assessment of air quality aboard ISS for each crew increment. The U.S. Navy is looking to update its submarine air monitoring suite of instruments, and the success of the AQM on ISS has led to a jointly planned submarine sea trial of a NASA AQM. In addition to the AQM, the Navy is also interested in the Multi-Gas Monitor (MGM), which was successfully flown on ISS as a technology demonstration to measure major constituent gases (oxygen, carbon dioxide, water vapor, and ammonia). A separate paper will present the MGM sea trial results. A prototype AQM, which is virtually identical to the operational AQM, has been readied for the sea trial. Only one AQM will be deployed during the sea trial, but it is sufficient to detect the compounds of interest to the Navy for the purposes of this trial. A significant benefit of the AQM is that runs can be scripted for pre-determined intervals and no crew intervention is required. The data from the sea trial will be compared to archival samples collected prior to and during the trial period. This paper will give a brief overview of the AQM technology and protocols for the submarine trial. After a quick review of the AQM preparation, the main focus of the paper will be on the results of the submarine trial. Of particular interest will be the comparison of the contaminants found in the ISS and submarine atmospheres, as both represent closed environments. In U.K. submarine trials in the early 2000s, the submarine and ISS atmospheres were found to be remarkably similar.
Limero, Thomas↗
Preparation of the NASA Air Quality Monitor for a U.S. Navy Submarine Sea Trial
For the past 4 years, the Air Quality Monitor (AQM) has been the operational instrument for measuring trace volatile organic compounds on the International Space Station (ISS). The key components of the AQM are the inlet preconcentrator, the gas chromatograph (GC), and the differential mobility spectrometer. Onboard the ISS are two AQMs with different GC columns that detect and quantify 22 compounds. The AQM data contributes valuable information to the assessment of air quality aboard ISS for each crew increment. The US Navy is looking to update its submarine air monitoring suite of instruments and the success of the AQM on ISS has led to a jointly planned submarine sea trial of a NASA AQM. In addition to the AQM, the Navy is also interested in the Multi-Gas Monitor (MGM), which measures major constituent gases (oxygen, carbon dioxide, water vapor, and ammonia). A separate paper will present the MGM sea trial preparation and the analysis of most recent ISS data. A prototype AQM, which is virtually identical to the operational AQM, has been readied for the sea trial. Only one AQM will be deployed during the sea trial, but this is sufficient for NASA purposes and to detect the compounds of interest to the US Navy for this trial. The data from the sea trial will be compared to data from archival samples collected before, during, and after the trial period. This paper will start with a brief history of past collaborations between NASA and the U.S. and U.K. navies for trials of air monitoring equipment. An overview of the AQM technology and protocols for the submarine trial will be presented. The majority of the presentation will focus on the AQM preparation and a summary of available data from the trial.
Limero, Thomas↗
Mobility Spectrometer Studies on Hydrazine and Ammonia Detection
An airborne vapor analyzer for detecting sub- to low- parts-per-million (ppm) hydrazine in the presence of higher concentration levels of ammonia has been under development for the Orion program. The detector is based on ambient pressure ionization and ion mobility characterization. The detector encompasses: 1) a membrane inlet to exclude particulate and aerosols from the analyzer inlet; 2) a method to separate hydrazine from ammonia which would otherwise lead to loss of calibration and quantitative accuracy for the hydrazine determination; and 3) response and quantitative determinations for both hydrazine and ammonia. Laboratory studies were made to explore some of these features including mobility measurements mindful of power, size, and weight issues. The study recommended the use of a mobility spectrometer of traditional design with a reagent gas and equipped with an inlet transfer line of bonded phase fused silica tube. The inlet transfer line provided gas phase separation of neutrals of ammonia from hydrazine at 50 C simplifying significantly the ionization chemistry that underlies response in a mobility spectrometer. Performance of the analyzer was acceptable between ranges of 30 to 80 C for both the pre-fractionation column and the drift tube. An inlet comprised of a combined membrane with valve-less injector allowed high speed quantitative determination of ammonia and hydrazine without cross reactivity from common metabolites such as alcohols, esters, and aldehydes. Preliminary test results and some of the design features are discussed.
Niu, William↗
Isotopic analyses of nitrogenous compounds from the Murchison meteorite: ammonia, amines, amino acids, and polar hydrocarbons
The combined volatile bases (ammonia, aliphatic amines, and possibly other bases), ammonia, amino acids, and polar hydrocarbons were prepared from the Murchison meteorite for isotopic analyses. The volatile bases were obtained by cryogenic transfer after acid-hydrolysis of a hot-water extract and analyzed by combined gas chromatography-mass spectrometry of pentafluoropropionyl derivatives. The aliphatic amines present in this preparation comprise a mixture that includes both primary and secondary isomers through C5 at a total concentration of > or = 100 nmoles g-1. As commonly observed for meteoritic organic compounds, almost all isomers through C5 are present, and the concentrations within homologous series decrease with increasing chain length. Ammonia was chromatographically separated from the other volatile bases and found at a concentration of 1.1-1.3 micromoles g-1 meteorite. The ammonia analyzed includes contributions from ammonium salts and the hydrolysis of extractable organic compounds, e.g., carboxamides. Stable isotope analyses showed the volatile bases to be substantially enriched in the heavier isotopes, relative to comparable terrestrial compounds delta D < or = +1221%; delta 13C = +22%; delta 15N = +93%). Ammonia, per se, was found to have a somewhat lower delta 15N value (+69%) than the total volatile bases; consequently, a higher delta 15N (>93%) can be inferred for the other bases, which include the amines. Solvent-extractable polar hydrocarbons obtained separately were found to be enriched in 15N (delta 15N = +104%). Total amino acids, prepared from a hydrolyzed hot-water extract by cation exchange chromatography, gave a delta 15N of +94%, a value in good agreement with that obtained previously. Nitrogen isotopic data are also given for amino acid fractions separated chromatographically. The delta 15N values of the Murchison soluble organic compounds analyzed to date fall within a rather narrow range (delta 15N = +94 +/- 8%), an observation consistent with their formation, or formation of their precursors, by interstellar chemistry.
Non-NASA Center↗
In-situ polymerized PLOT columns III: divinylbenzene copolymers and dimethacrylate homopolymers
Studies of divinylbenzene copolymers and dimethacrylate homopolymers indicate that the polymer pore size controls the separation of water and ammonia on porous-layer-open-tubular (PLOT) columns. To a lesser degree, the polarity of the polymers also affects the separation of a water-ammonia gas mixture. Our results demonstrate that the pore size can be regulated by controlling the cross-linking density or the chain length between the cross-linking functional groups. An optimum pore size will provide the best separation of water and ammonia.
NASA Discipline Exobiology↗
Artemis II Mission Performance of the Orion Active Thermal Control System
The Orion spacecraft has recently completed Artemis II, the first crewed mission around the moon in 54 years. This test flight demonstrated vehicle capability as the foundation for all future missions under the Artemis program. As a major system of Orion, the Active Thermal Control System (ATCS) successfully managed crew and vehicle heat loads to provide adequate cooling and thermal comfort for the duration of the Artemis II mission. Thermal control on the Orion vehicle is managed through two redundant cooling loops in the Crew Module (CM) that absorb heat loads from the cabin and Air Revitalization System (ARS) heat exchangers, the Liquid Cooling Garment (LCG) heat exchanger, and the avionics cold plates, and then transfer those heat loads to the Service Module (SM) radiator loops and/or the Phase Change Material (PCM) and ammonia boilers when required through thermal configuration or mission phase. During Artemis II, Orion did not necessitate any supplemental cooling from ammonia boilers until service module separation, allowing the maximum availability of ammonia cooling prior to entry. This presentation will provide an overview of the Orion ATCS major subsystems, highlight the performance during key mission phases, and comment on the applicability of the observed thermal response to future Artemis missions.
Ellie Thurston↗
High Ph, Ammonia Toxicity, and the Search for Life on the Jovian Planets
The effects of pH and ammonia concentration were studied separately, where possible, on a variety of organisms, including some isolated from natural environments of high pH and/or ammonia concentration. Escherichia coli and Bacillus subtilis are both extremely sensitive to ammonia. An aerobic organism (growth up to pH 11.4) from an alkaline spring is more resistant, but exhibits a toxic response to ammonia at a pH much lower than its maximum for growth. The greatest ammonia resistance has been found in an unidentified organism growing at near neutral pH. Even in this case, however, urvival at ammonia concentrations reasonably expected on the Jovian planets is measured in hours. This is two to three orders of magnitude longer than for E. coli. Results support the tentative conclusion that contamination of the Jovian planets with terrestrial organisms that can grow is unlikely. However, the range of toxic response noted, coupled with the observation that terrestrial life has not been exposed to high ammonia concentrations for millions of years, suggests that adaptation to greater ammonia tolerance may be possible.
Deal, P. H.↗
Preprototype nitrogen supply subsystem development
A nitrogen supply subsystem based on the dissociation of hydrazine into a mixture of hydrogen and nitrogen is developed. The latter is separated to provide makeup nitrogen to control the composition of spacecraft atmospheres. Specific hardware developments resulted in the design and fabrication of a nominal 3.6 kg/d nitrogen generation module. The design integrates a hydrazine catalytic dissociator, three ammonia dissociation stages and four hydrogen separation stages into a 33 kg, 14 cu dm module. A technique was devised to alternate the ammonia dissociation and hydrogen separation stages to give high nitrogen purity in the end product stream. Tests show the product stream to contain less than 0.5 percent hydrogen and 10 parts per million ammonia. The design and development of a test stand for the nitrogen generation module and a series of tests which verified its operation and performance capability are described.
Heppner, D. B.↗
Performance testing of a two-phase interface heat exchanger
This paper describes the design and performance testing of a heat exchanger which interfaces separate two-phase ammonia thermal loops. The basic design involves a tube-in-tube concept, with boiling occurring in the inner tube and condensation in the outer tube. Eight such tubes are arranged in parallel. Testing has demonstrated that up to 8.2 kW of heat may be transferred across the heat exchanger when the saturation temperature difference between the systems is 5 C. Performance of the heat exchanger is affected primarily by the mass flow rate of ammonia in the liquid supply loop.
Mccabe, M. E., Jr.↗
Fluorescence Excitation Models of Ammonia and Amidogen Radical (NH2) in Comets: Application to Comet C/2004 Q2 (Machholz)
Ammonia is a major reservoir of nitrogen atoms in cometary materials. However, detections of ammonia in comets are rare, with several achieved at radio wavelengths. A few more detections were obtained through near-infrared observations (around the 3 m wavelength region), but moderate relative velocity shifts are required to separate emission lines of cometary ammonia from telluric absorption lines in the 3 micron wavelength region. On the other hand, the amidogen radical (NH2 -- a photodissociation product of ammonia in the coma) also shows rovibrational emission lines in the 3 micron wavelength region. Thus, gas production rates for ammonia can be determined from the rovibrational emission lines of ammonia (directly) and amidogen radical (indirectly) simultaneously in the near-infrared. In this article, we present new fluorescence excitation models for cometary ammonia and amidogen radical in the near-infrared, and we apply these models to the near-infrared high-dispersion spectra of comet C/2004 Q2 (Machholz) to determine the mixing ratio of ammonia to water in the comet. Based on direct detection of NH3 lines, the mixing ratio of NH3/H2O is 0.46% +/- 0.03% in C/2004 Q2 (Machholz), in agreement with other results. The mixing ratio of ammonia determined from the NH2 observations (0.31% -- 0.79%) is consistent but has relatively larger error, owing to uncertainty in the photodissociation rates of ammonia. At the present level of accuracy, we confirm that NH3 could be the sole parent of NH2 in this comet.
Kawakita, Hideyo↗