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At least 361 records · Page 20
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Gas adsorption/separation properties of metal directed self-assembly of two coordination polymers with 5-nitroisophthalate

Two new coordination polymers, namely, [Co(µ-nip)(µ-bpe)]{sub n} (1) and [Zn(µ-nip)(µ-bpe)]{sub n} (2) (nip: 5-nitroisophthalate, bpe: 1,2-bis(4-pyridyl)ethane) were hydrothermally synthesized and structurally characterized by single crystal X-ray diffraction, IR spectroscopy, elemental analysis and thermal analysis. Moreover, atomically detailed simulation studies of complex 2 for CO{sub 2}/CH{sub 4} adsorption and separation were performed. Complex 1 consists of two dimensional (2D) (4,4) grid networks with the point symbol of 4{sup 4}.6{sup 2}. Complex 2 exhibits a 3-fold interpenetrating 3D framework with 6{sup 5}.8-dmp topology. Thermal properties of the complexes showed that both complexes were stable over 320 °C. Simulation studies demonstrated that complex 2 can separate CO{sub 2} from CH{sub 4} at low pressures at 273 K. - Graphical abstract: In this study, two new coordination polymers, namely, [Co(µ-nip)(µ-bpe)]{sub n} (1) and [Zn(µ-nip)(µ-bpe)]{sub n} (2) (nip: 5-nitroisophthalate, bpe: 1,2-bis(4-pyridyl)ethane) were hydrothermally synthesized and structurally characterized by single crystal X-ray diffraction, IR spectroscopy, elemental analysis and thermal analysis. Moreover, atomically detailed simulation studies of complex 2 for CO{sub 2}/CH{sub 4} adsorption and separation were performed. Complex 1 consists of two dimensional (2D) (4,4) grid networks with the point symbol of 4{sup 4}.6{sup 2}. Complex 2 exhibits a 3-fold interpenetrating 3D framework with 6{sup 5}.8-dmp topology. Simulation studies demonstrated that complex 2 can separate CO{sub 2} from CH{sub 4} at low pressures at 273 K. Display Omitted - Highlights: • Two new coordination polymers with 5-nitroisophthalate and 1,2-bis(4-pyridyl)ethane. • Atomically detailed simulation studies of the complexes. • Complex 2 can be proposed as molecular sieve to separate CO{sub 2} from CH{sub 4} at low pressures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Methane Activation on Cu Containing Zeolite Catalysts (Final Report)

In order to increase the value of the light alkane ethane found in shale gas, we investigated the transformation of ethane into ethylene and aromatic hydrocarbons using zinc-containing microporous catalysts. We investigated the kinetics of the reaction, and identified various active sites for the ethane dehydrogenation and aromatization. In addition, we investigated iron-containing zeolites, as catalysts for the addition of methyl groups to small olefins containing 2, 3 and 4 carbon molecules. We determined the reaction mechanism, the identity of the active site, and details of the reaction kinetics. We concluded that the use of iron zeolites is very promising to upgrade small olefins (2-4 carbon species) into larger olefins (4-7 carbon species) that are more valuable as fuels and as petrochemical products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Microwave catalytic reactor for upgrading stranded shale gas to aromatics

Microwave (MW) catalytic processing has been applied to science discovery in a number of research fields. The potential of MW assisted catalysis in direct ethane dehydroaromatization was explored in this study. Under MW irradiation, significant enhancement in ethane conversion to aromatics was achieved at 400 °C which otherwise would take up to 600 °C in a thermally heated fixed-bed reactor. The role of MW irradiation in activating ethane over the catalyst and the reaction mechanism were elucidated. The results showed that MW could possibly induce the formation of dipoles on catalyst surface, facilitating electron shifting and sharing between catalyst and reaction intermediates. Here, this activation process has significantly lowered activation energy, allowing the reaction to proceed under lower bulk temperature with enhanced aromatic yield.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Phosphine and N-heterocyclic carbene ligands on Pt(II) shift selectivity from ethylene hydrophenylation toward benzene vinylation

In this study, a series of Pt(II) complexes of the type ([(L~L)Pt(L')(Ph)][BAr' 4 ] (L~L = 1,2-bis(dimethylphosphino)ethane, 1,2-bis(diphenylphosphino)ethane, ( N -pyrrolyl) 2 P(CH 2 ) 2 P( N -pyrrolyl) 2 , 1,3-bis(diphenylphosphino)propane, 1,1'-bis(diphenylphosphino)ferrocene, (bis-(diphenylphosphino)methyl)methylamine, 8-(diisopropylphosphino)quinoline, 1,1'-methylene-3,3'-di- tert -butylimidazol-2,2'-diylidine); L' = THF or NCMe) has been synthesized and fully characterized. These complexes were screened as catalysts for ethylene hydrophenylation to yield ethylbenzene. All of the complexes exhibited selectivity for styrene production with low catalytic turnover. DFT calculations have been used to model reactivity of the [(dmpe)Pt(L')(Ph)][BAr' 4 ] (dmpe = 1,2-bis(dimethylphosphino)ethane). It is shown that selective styrene formation is a result of a calculated ΔΔ G ‡ of 5 kcal/mol for the benzene C–H activation step in the catalytic cycles for styrene versus ethylbenzene formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Bimolecular Peroxy Radical (RO 2 ) Reactions and Their Relevance in Radical Initiated Oxidation of Hydrocarbons

The kinetics of peroxy radical (RO 2 ) reactions have been of long-standing interest in atmospheric and combustion chemistry. Nevertheless, the lack of kinetic studies at higher temperatures for their reactions with other radicals such as OH has precluded the inclusion of this class of reactions in detailed kinetics models developed for combustion applications. In this work, guided by the limited room temperature experimental studies on selected alkyl-peroxy radicals and literature theoretical kinetics on the prototypical CH 3 O 2 + OH system, we have performed parametric studies on the effect of uncertainties in the rate coefficients and branching ratios to potential product channels for RO 2 + OH reactions at higher temperatures. Literature kinetics models were used to simulate autoignition delays, laminar flame speeds, and speciation profiles in flow and stirred reactors for a variety of common combustion-relevant fuels. Inclusion of RO 2 + OH reactions was found to retard autoignition in fuel-lean (φ = 0.5) mixtures of ethane and dimethyl ether in air. The observed effects were noticeably more pronounced in ozone-enriched combustion of ethane and dimethyl ether. The simulations also examined the influence of ozone doping levels, pressures, and equivalence ratios for both ethane and dimethyl ether oxidation. Sensitivity and flux analyses revealed that the RO 2 + OH reaction is a significant sink of RO 2 radicals at the early stage of autoignition, affecting fuel oxidation through RO 2 ↔ QOOH, RO 2 ↔ alkene + HO 2 , or RO 2 + HO 2 ↔ ROOH + O 2 . Additionally, the kinetic stability of the trioxide formed from RO 2 + OH reactions was investigated using master equation analyses. Last, we discuss other bimolecular reactions that are missing in literature kinetics models but are relevant to hydrocarbon oxidation initiated by external radical sources (plasma-enhanced, ozone-enriched combustion, etc.). In conclusion, the present simulations provide a strong motivation for better characterizing the bimolecular kinetics of peroxy radicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Adsorption of Natural Gas in Metal–Organic Frameworks: Selectivity, Cyclability, and Comparison to Methane Adsorption

Evaluation of metal–organic frameworks (MOFs) for adsorbed natural gas (ANG) technology employs pure methane as a surrogate for natural gas (NG). This approximation is problematic, as it ignores the impact of other heavier hydrocarbons present in NG, such as ethane and propane, which generally have more favorable adsorption interactions with MOFs compared to methane. Herein, using quantitative Raman spectroscopic analysis and Monte Carlo calculations, we demonstrate the adsorption selectivity of high-performing MOFs, such as MOF-5, MOF-177, and SNU-70, for a methane and ethane mixture (95:5) that mimics the composition of NG. The impact of selectivity on the storage and deliverable capacities of these adsorbents during successive cycles of adsorption and desorption, simulating the filling and emptying of an ANG tank, is also demonstrated. Finally, the study reveals a gradual reduction in the storage performance of MOFs, particularly with smaller pore volumes, due to ethane accumulation over long-term cycling, until a steady state is reached with substantially degraded storage performance.

03 NATURAL GAS↗
DOE OSTI2015

A thermodynamic tank model for studying the effect of higher hydrocarbons on natural gas storage in metal-organic frameworks

Metal-organic frameworks (MOFs) are promising materials for storing natural gas in vehicular applications. Evaluation of these materials has focused on adsorption of pure methane, although commercial natural gas also contains small amounts of higher hydrocarbons such as ethane and propane, which adsorb more strongly than methane. There is, thus, a possibility that these higher hydrocarbons will accumulate in the MOF after multiple operating (adsorption/desorption) cycles, and reduce the storage capacity. To study the net effect of ethane and propane on the performance of an adsorbed natural gas (ANG) tank, we developed a mathematical model based on thermodynamics and mass balance equations that describes the state of the tank at any instant. The required inputs are the pure-component isotherms, and mixture adsorption data are calculated using the Ideal Adsorbed Solution Theory (IAST). We focused on how the "deliverable energy'' provided by the ANG tank to the engine changed over 200 operating cycles for a sample of 120 MOF structures. We found that, with any MOF, the ANG tank performance monotonically declines during early operating cycles until a "cyclic steady state'' is reached. We determined that the best materials when the fuel is 100% methane are not necessarily the best when the fuel includes ethane and propane. Among the materials tested, some top MOFs are MOF-143 > NU-800 > IRMOF-14 > IRMOF-20 > MIL-100 > NU-125 > IRMOF-1 > NU-111. MOF-143 is predicted to deliver 5.43 MJ L-1 of tank to the engine once the cyclic steady state is reached. The model also provided insights that can assist in future work to discover more promising adsorbent materials for natural gas storage.

Zhang, HD↗
DOE OSTI2018

C2 adsorption in zeolites: in silico screening and sensitivity to molecular models

Efficient separation of ethane and ethylene has been a long-standing challenge for the chemical industry. In this work, we use molecular modeling to identify zeolite and zeotype frameworks that have the potential to be the next-generation solution for the separation of these C2 compounds. Using two different united-atom versions of the transferable potentials for phase equilibria (TraPPE) force field, the zeolitic structures in the database of the International Zeolite Association are screened for the separation of ethane and ethylene. A detailed analysis, with regards to accessibility of favorable sites and sensitivity to molecular models (also considering the explicit-hydrogen TraPPE model for ethane), is carried out on the top-performing structures. This study provides insights on the performance and limitations of molecular models for predicting mixture adsorption in zeolites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Low-Energy, Low-Cost Ethylene Production by Low-Temperature Oxidative Coupling of Methane

Ethylene, one of the highest volume production chemicals in the U.S. and globally, is an essential chemical building block that is used to manufacture countless products, from packaging to antifreeze to tires. Most ethylene is produced via a process called steam cracking, where the feedstock (mostly ethane, sometimes naphtha or propane) is heated to high temperatures over a catalyst. The naphtha feedstock typically comes from petroleum refineries, while ethane is becoming increasingly used as a feedstock in the U.S. due to the rise in domestic natural gas production from shale resources. However, steam cracking is energy intensive and occurs in large- scale facilities. Low-temperature oxidative coupling of methane (LT-OCM) is an alternative ethylene production method that converts methane (natural gas) and optionally ethane to ethylene in a single-step, energy-producing conversion system using an innovative process. While OCM has been studied for over 30 years due to its potential to reduce ethylene production cost, past efforts did not result in a viable catalyst with performance needed for commercialization. These catalysts, while at times achieving promising yield and selectivity, were hampered by very high operating temperatures, low activities, and short lifetimes on the order of hours to days. Recognizing this, Siluria applied a combination of new innovations in catalyst development and a thorough definition and understanding of the problem to develop unique catalysts that enable commercialization of OCM. The OCM catalysts operate at significantly lower temperature (several hundreds of degrees lower) and practical operating pressures (5-10 atmospheres), have high activities and standard lifetimes of years under said conditions. In addition, the simple process provides excellent scalability and flexibility, especially when compared to today’s mega-scale steam crackers, thus enabling small- volume “distributed scale” reactors for on-demand ethylene production for applications such as on-site conversion of ethylene to high value polymer derivatives.

02 PETROLEUM↗
DOE OSTI2026

Integrated Direct Air Capture and H₂-Free CO₂ Valorization

This project advances fundamental understanding of a novel integrated direct air capture (DAC) and CO₂ conversion process that valorizes atmospheric CO₂ without external H₂. The research encompasses four critical components: (1) design of task-specific ionic liquids for efficient CO₂ capture under ambient conditions, (2) development of H₂-free tandem catalytic systems using ethane as a reductant, (3) advanced operando characterization to elucidate capture and conversion mechanisms, and (4) data science-driven predictive computation to accelerate material discovery. Over the project period, we developed five high-performance DAC sorbent systems—including CaO/superbase ionic liquid composites, Ni-MOF/Ionic Liquid (IL) hybrids, fluorinated covalent organic frameworks with ion-pair functional groups, defect-engineered UiO-66, and a validated kinetic model for humid-condition operation, achieving CO₂ capacities up to 1.86 mmol/g at 400 ppm with excellent cycling stability. For H₂-free conversion, we constructed atomically synergistic Zn–O–Cr binuclear catalytic sites that achieve 100% ethylene selectivity, ~9.6% ethane conversion, and 99% CO₂ utilization in equimolar co-conversion of ethane and CO₂. We further demonstrated downstream valorization pathways converting CO and C₂H₄ into polyketones and C₃ chemicals. These advances strengthen the scientific foundation for producing value-added materials from ambient CO₂.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Application of Gauss's theorem to quantify localized surface emissions from airborne measurements of wind and trace gases

Airborne estimates of greenhouse gas emissions are becoming more prevalent with the advent of rapid commercial development of trace gas instrumentation featuring increased measurement accuracy, precision, and frequency, and the swelling interest in the verification of current emission inventories. Multiple airborne studies have indicated that emission inventories may underestimate some hydrocarbon emission sources in US oil- and gas-producing basins. Consequently, a proper assessment of the accuracy of these airborne methods is crucial to interpreting the meaning of such discrepancies. We present a new method of sampling surface sources of any trace gas for which fast and precise measurements can be made and apply it to methane, ethane, and carbon dioxide on spatial scales of ~1000 m, where consecutive loops are flown around a targeted source region at multiple altitudes. Using Reynolds decomposition for the scalar concentrations, along with Gauss's theorem, we show that the method accurately accounts for the smaller-scale turbulent dispersion of the local plume, which is often ignored in other average mass balance methods. With the help of large eddy simulations (LES) we further show how the circling radius can be optimized for the micrometeorological conditions encountered during any flight. Furthermore, by sampling controlled releases of methane and ethane on the ground we can ascertain that the accuracy of the method, in appropriate meteorological conditions, is often better than 10 %, with limits of detection below 5 kg h -1 for both methane and ethane. Because of the FAA-mandated minimum flight safe altitude of 150 m, placement of the aircraft is critical to preventing a large portion of the emission plume from flowing underneath the lowest aircraft sampling altitude, which is generally the leading source of uncertainty in these measurements. Finally, we show how the accuracy of the method is strongly dependent on the number of sampling loops and/or time spent sampling the source plume.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1972

Compounds of the organogenic elements in Apollo 11 and 12 lunar samples - A review.

Investigations of low molecular weight compounds of the organogenic elements on lunar samples are reviewed. The three general techniques of vacuum pyrolysis, acid hydrolysis, and crushing have been employed by most investigators. Vacuum pyrolysis of lunar fines produce a variety of gaseous species which are either: (1) indigenous, (2) solar wind products and/or (3) chemical reaction products of mineral phases found in the lunar samples. Acid hydrolysis of lunar fines using deuterium-labeled acids yields evidence for indigenous methane and ethane. Methane and ethane found in the lunar fines are largely derived from the solar wind with only trace amounts indigenous to the samples. Crushing experiments with lunar fines and breccias produce methane, ethane, hydrogen, nitrogen, hydrogen sulfide and the rare gases.

Gibson, E. K., Jr.↗
NASA NTRS1975

Sulfur poisoning of hydrocarbon oxidation by palladium

Using a differential bed recycle reactor the oxidation of ethane and diethyl ketone by a Pd catalyst was studied at the 0-30 ppm level in air. In both cases first order kinetics were observed. The ethane oxidation rate was characterized n the Arrhenius form by a pre-exponential of 1.0 x 10 to the 8th power cm/sec and an E sub a of 27 kcal/mole. The diethyl ketone oxidation rate was characterized by a pre-exponential of 5.7 x -1000 cm/sec and E sub a of 14 kcal/mole. Poisoning of ethan oxidation was also investigated by hydrogen sulfide and to a smaller extent by the refrigerants Freon 22 and Gentron 142-B. Poisoning by Gentron 142-B was much more severe than by hydrogen sulfide. Kinetic experiments indicated that only the pre-exponential was changing.

Baumgartner, A. J.↗
NASA NTRS1985

Evolution of Titan's coupled ocean-atmosphere system and interaction of ocean with bedrock

A recent model for the surface state of Titan proposes a liquid ethane-methane-molecular nitrogen layer of order one kilometer thick which because of stratospheric methane photolysis has become increasingly ethane-rich with time. The interaction of such an ocean with the underlying 'bedrock' of Titan (assumed to be water-ice or ammonia hydrate) and with the primarily nitrogen atmosphere is explored. It is concluded that although modest exchange of oceanic hydrocarbons with enclathrated methane in the bedrock can in principle occur, it is unlikely for reasonable regolith depths. The surprisingly high solubility of water-ice in liquid methane implies that topographic features on Titan of order 100 meters in height can be eroded away on a time scale of one-billion years. The large solubility difference of N2 in methane versus ethane implies that the ocean composition is a strong determinant of atmospheric pressure; a simple radiative model of the Titan atmosphere is employed to demonstrate that significant surface pressure and temperature changes can occur as the oceanic composition evolves with time.

Lunine, J. I.↗
NASA NTRS1994

Effects of biomass burning on summertime nonmethane hydrocarbon concentrations in the Canadian wetlands

Approximately 900 whole air samples were collected and assayed for selected C2-C10 hydrocarbons and seven halocarbons during the 5-week Arctic Boundary Layer Expedition (ABLE) 3B conducted in eastern Canadian wetland areas. In more than half of the 46 vertical profiles flown, enhanced nonmethane hydrocarbon (NMHC) concentrations attributable to plumes from Canadian forest fires were observed. Urban plumes, also enhanced in many NMHCs, were separately identified by their high correlation with elevated levels of perchloroethene. Emission factors relative to ethane were determined for 21 hydrocarbons released from Canadian biomass burning. Using these data for ethane, ethyne, propane, n-butane, and carbon monoxide enhancements from the literature, global emissions of these four NMHCs were estimated. Because of its very short atmospheric lifetime and its below detection limit background mixing ratio, 1,3-butadiene is an excellent indicator of recent combustion. No statistically significant emissions of nitrous oxide, isoprene, or CFC 12 were observed in the biomass-burning plumes encountered during ABLE 3B. The presence of the short-lived biogenically emitted isoprene at altitudes as high as 3000 m implies that mixing within the planetary boundary layer (PBL) was rapid. Although background levels of the longer-lived NMHCs in this Canadian region increase during the fire season, isoprene still dominated local hydroxyl radical photochemistry within the PBL except in the immediate vicinity of active fires. The average biomass-burning emission ratios for hydrocarbons from an active fire sampled within minutes of combustion were, relative to ethane, ethene, 2.45; ethyne 0.57; propane, 0.25; propene, 0.73; propyne, 0.06; n-butane, 0.09; i-butane, 0.01; 1-butene, 0.14; cis-2-butene, 0.02; trans-2-butene, 0.03; i-butylene, 0.07; 1,3-butadiene, 0.12; n-pentane, 0.05; i-pentane, 0.03; 1-pentene, 0.06; n-hexane, 0.05; 1-hexene, 0.07; benzene, 0.37; toluene, 0.16.

Blake, D. R.↗
NASA NTRS2007

Opposed Jet Burner Extinction Limits: Simple Mixed Hydrocarbon Scramjet Fuels vs Air

Opposed Jet Burner tools have been used extensively by the authors to measure Flame Strength (FS) of laminar non-premixed H2 air and simple hydrocarbon (HC) air counterflow diffusion flames at 1-atm. FS represents a strain-induced extinction limit based on air jet velocity. This paper follows AIAA-2006-5223, and provides new HC air FSs for global testing of chemical kinetics, and for characterizing idealized flameholding potentials during early scramjet-like combustion. Previous FS data included six HCs, pure and N2-diluted; and three HC-diluted H2 fuels, where FS decayed very nonlinearly as HC was added to H2, due to H-atom scavenging. This study presents FSs on mixtures of (candidate surrogate) HCs, some with very high FS ethylene. Included are four binary gaseous systems at 300 K, and a hot ternary system at approx. 600 K. The binaries are methane + ethylene, ethane + ethylene, methane + ethane, and methane + propylene. The first three also form two ternary systems. The hot ternary includes both 10.8 and 21.3 mole % vaporized n-heptane and full ranges of methane + ethylene. Normalized FS data provide accurate means of (1) validating, globally, chemical kinetics for extinction of non-premixed flames, and (2) estimating (scaling by HC) the loss of incipient flameholding in scramjet combustors. The n-heptane is part of a proposed baseline simulant (10 mole % with 30% methane + 60% ethylene) that mimics the ignition of endothermically cracked JP-7 like kerosene fuel, as suggested by Colket and Spadaccini in 2001 in their shock tube Scramjet Fuels Autoignition Study. Presently, we use FS to gauge idealized flameholding, and define HC surrogates. First, FS was characterized for hot nheptane + methane + ethylene; then a hot 36 mole % methane + 64% ethylene surrogate was defined that mimics FS of the baseline simulant system. A similar hot ethane + ethylene surrogate can also be defined, but it has lower vapor pressure at 300 K, and thus exhibits reduced gaseous capacity. The new FS results refine our earlier idealized reactivity scale that shows wide ranging (50 x) diameter-normalized FSs for various HCs. These range from JP-10 and methane to H2 air, which produces an exceptionally strong flame that agrees within approx. 1% of recent 2-D numerically simulations. Finally, we continue advocating the FS approach as more direct and fundamental, for assessing idealized scramjet flameholding potentials, than measurements of unstrained laminar burning velocity or blowout in a Perfectly Stirred Reactor.

Pellett, Gerald L.↗
NASA NTRS2009

Strong Solar Control of Infrared Aurora on Jupiter: Correlation Since the Last Solar Maximum

Polar aurorae in Jupiter's atmosphere radiate throughout the electromagnetic spectrum from X ray through mid-infrared (mid-IR, 5 - 20 micron wavelength). Voyager IRIS data and ground-based spectroscopic measurements of Jupiter's northern mid-IR aurora, acquired since 1982, reveal a correlation between auroral brightness and solar activity that has not been observed in Jovian aurora at other wavelengths. Over nearly three solar cycles, Jupiter auroral ethane emission brightness and solar 10.7 cm radio flux and sunspot number are positively correlated with high confidence. Ethane line emission intensity varies over tenfold between low and high solar activity periods. Detailed measurements have been made using the GSFC HIPWAC spectrometer at the NASA IRTF since the last solar maximum, following the mid-IR emission through the declining phase toward solar minimum. An even more convincing correlation with solar activity is evident in these data. Current analyses of these results will be described, including planned measurements on polar ethane line emission scheduled through the rise of the next solar maximum beginning in 2009, with a steep gradient to a maximum in 2012. This work is relevant to the Juno mission and to the development of the Europa Jupiter System Mission. Results of observations at the Infrared Telescope Facility (IRTF) operated by the University of Hawaii under Cooperative Agreement no. NCC5-538 with the National Aeronautics and Space Administration, Science Mission Directorate, Planetary Astronomy Program. This work was supported by the NASA Planetary Astronomy Program.

Kostiuk, T.↗