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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Size-Controlled Nanoparticles Embedded in a Mesoporous Architecture Leading to Efficient and Selective Hydrogenolysis of Polyolefins

A catalytic architecture, comprising a mesoporous silica shell surrounding platinum nanoparticles (NPs) supported on a solid silica sphere (mSiO2/Pt-X/SiO2; X is the mean NP diameter), catalyzes hydrogenolysis of melt-phase polyethylene (PE) into a narrow C23-centered distribution of hydrocarbons in high yield using very low Pt loadings (~10 -5 g Pt/g PE). During catalysis, a polymer chain enters a pore and contacts a Pt NP where the C–C bond cleavage occurs and then the smaller fragment exits the pore. mSiO 2 /Pt/SiO 2 resists sintering or leaching of Pt and provides high yields of liquids; however, many structural and chemical effects on catalysis are not yet resolved. Here, we report the effects of Pt NP size on activity and selectivity in PE hydrogenolysis. Time-dependent conversion and yields and a lumped kinetics model based on the competitive adsorption of long vs short chains reveal that the activity of catalytic material is highest with the smallest NPs, consistent with a structure-sensitive reaction. Remarkably, the three mSiO 2 /Pt-X/SiO 2 catalysts give equivalent selectivity. We propose that mesoscale pores in the catalytic architecture template the C 23 -centered distribution, whereas the active Pt sites influence the carbon–carbon bond cleavage rate. This conclusion provides a framework for catalyst design by separating the C–C bond cleavage activity at catalytic sites from selectivity for chain lengths of the products influenced by the structure of the catalytic architecture. The increased activity, selectivity, efficiency, and lifetime obtained using this architecture highlight the benefits of localized and confined environments for isolated catalytic particles under condensed-phase reaction conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1994

Exobiology experiments for Earth-orbital platforms

Low-gravity (microgravity) studies relevant to prebiotic evolution and the history of the biogenic elements (C, H, N, O, P, S) are particularly suited to orbital platforms. Relevant to these topics are phenomena such as gas-particle interactions (e.g., formation of organic aerosols via photolytic reactions) including nucleation, condensation, evaporation, adsorption, and catalytic reactions on surfaces; and, small-particle or grain interactions (e.g., growth of interstellar dust particles and planetesimals) including processes such as aggregation (or coagulation), scavenging, and collisions. Both gas-particle and grain (i.e., dust, crystals, organic aerosols, etc.) interactions studies can benefit from microgravity and are pertinent to studies in the areas of chemical evolution in the solar nebula, the interstellar medium, and planetary atmospheres; growth of planetesimals; and prebiotic evolution. In general, the microgravity environment allows for long duration and controlled simulations of processes occurring in exobiologically significant systems such as Titan's atmosphere, interstellar dust clouds, and the solar nebula in which gas-particle or particle-particle interactions play a significant role.

Huntington, J. L.↗
DOE OSTI2025

Probing Condensed-Phase Structure and Dynamics in Hierarchical Zeolites and Nanosheets for Catalytic Upgradation of Biomass (Final Report)

Understanding complex reaction pathways in systems governed by multi-scale collective interactions across time and length scales remains a central scientific challenge. This project was guided by the hypothesis that the interplay among oligomers, solvents, and active sites can be tuned by a suitable choice of solvation environment and pore architecture in solid-acid catalysts to direct chemical transformations relevant to biomass conversion. Zeolites and zeolite nanosheets were used as model platforms, allowing for the interaction of macromolecules with the surface of the zeolite nanosheets and with smaller pores that host catalytically active sites. To investigate these coupled phenomena, we employ a multi-scale computational framework that integrates molecular-level descriptions with advanced sampling approaches to capture key physical and chemical interactions. Our work through this project improved fundamental understanding of how reactants and solid-acid catalysts interact in solvent-rich environments, thereby enabling the rational design of catalytic systems that upgrade biomass with enhanced selectivity and energy efficiency. In addition, the project developed advanced sampling methodologies critical for disentangling complex, reactive processes in multi-component catalytic environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1985

Role of minerals in the thermal alteration of organic matter. I - Generation of gases and condensates under dry condition

Pyrolysis experiments conducted at 200 and 300 C on kerogen and bitumen from the Monterey formation and on the Green River Formation kerogen with montmorillonite, illite, and calcite added are described. The pyrolysis products are identified and gas and condensate analyses are performed. A catalytic effect is detected in the pyrolysis of kerogen with montmorillonite; however, illite and calcite display no catalytic activity. The increased production of C1-C6 hydrocarbons and the dominance of branched hydrocarbons in the C4-C6 range reveals a catalytic influence. It is observed that the catalysis of montmorillonite is greater during bitumen pyrolysis than for kerogen, and catalysis with minerals affects the production of CO2. It is concluded that a mineral matrix is important in determining the type and amount of gases and condensates forming from organic matter under thermal stress.

Tannenbaum, E.↗
DOE OSTI2025

Effects of Water Vapor on the Reactivity of Aluminosilicates in Vapor-Phase Propanal Aldol Condensation

Aluminosilicate materials have been extensively studied as efficient aldol catalysts for C-C coupling reactions due to their acidic nature, high surface area, thermal stability, and porous structure. This work investigated the impact of water vapor pressure on the catalytic reactivity of aluminosilicates for the aldol condensation of propanal to 2-methyl-2-pentenal (MP). The catalytic performance of amorphous SiO2-Al2O3 (A-Si-Al) and aluminated MCM-41 (Al-MCM-41) for the vapor-phase aldol condensation of propanal was evaluated at 200 degrees C as a function of vapor-phase water content at atmospheric pressure. Our findings demonstrate that co-feeding low water vapor pressures (1-18 kPa) with propanal enhances the rates of MP production at 200 degrees C on A-Si-Al. Conversely, water vapor pressures of 25 kPa result in a decrease in aldol dimer formation rates. The rate of MP production evaluated on Al-MCM-41 also increased in the presence of 5 kPa water compared to anhydrous conditions. Propylamine temperature-programmed desorption analyses revealed an increase in Bronsted acid site density when both catalysts were exposed to water, which likely accounts for the observed enhancement in aldol condensation reactivity under hydrous conditions. Reversibility testing of the water vapor effect under reaction conditions, combined with X-ray diffraction analysis of fresh, spent, and regenerated catalysts, revealed no structural changes in either aluminosilicate upon exposure to water or reaction conditions. The rates of aldol condensation and the impact of water vapor were highly consistent across both materials, suggesting that zeolite crystallinity has minimal influence on the catalytic performance.

acid catalysts↗
NASA NTRS1993

Fuel-rich catalytic combustion of a high density fuel

Fuel-rich catalytic combustion (ER is greater than 4) of the high density fuel exo-tetrahydrocyclopentadiene (JP-10) was studied over the equivalence ratio range 5.0 to 7.6, which yielded combustion temperatures of 1220 to 1120 K. The process produced soot-free gaseous products similar to those obtained with iso-octane and jet-A in previous studies. The measured combustion temperature agreed well with that calculated assuming soot was not a combustion product. The process raised the effective hydrogen/carbon (H/C) ratio from 1.6 to over 2.0, thus significantly improving the combustion properties of the fuel. At an equivalence ratio near 5.0, about 80 percent of the initial fuel carbon was in light gaseous products and about 20 percent in larger condensable molecules. Fuel-rich catalytic combustion has now been studied for three fuels with H/C ratios of 2.25 (iso-octane), 1.92 (jet-A), and 1.6 (JP-10). A comparison of the product distribution of these fuels shows that, in general, the measured concentrations of the combustion products were monotonic functions of the H/C ratio with the exception of hydrogen and ethylene. In these cases, data for JP-10 fell between iso-octane and jet-A rather than beyond jet-A. It is suggested that the ring cross-linking structure of JP-10 may be responsible for this behavior. All the fuels studied showed that the largest amounts of small hydrocarbon molecules and the smallest amounts of large condensable molecules occurred at the lower equivalence ratios. This corresponds to the highest combustion temperatures used in these studies. Although higher temperatures may improve this mix, the temperature is limited. First, the life of the present catalyst would be greatly shortened when operated at temperatures of 1300 K or greater. Second, fuel-rich catalytic combustion does not produce soot because the combustion temperatures used in the experiments were well below the threshold temperature (1350 K) for the formation of soot. Increasing the temperature above this value would remove the soot-free nature of the process. Since all the fuels studied show a similar breakdown of the primary fuel into smaller molecular combustion products, this technique can be applied to all hydrocarbon fuels.

Brabbs, Theodore A.↗
NASA NTRS1983

Development of a condenser for the dual catalyst water recovery system

Conceptual evaporation/condensation systems suitable for integration with the catalytic water recovery method were evaluated. The primary requirements for each concept were its capability to operate under zero-gravity conditions, condense recovered water from a vapor-noncondensable gas mixture, and integrate with the catalytic system. Specific energy requirements were estimated for concepts meeting the primary requirements, and the concept most suitable for integration with the catalytic system was proposed. A three-man rate condenser capable of integration with the proposed system, condensing water vapor in presence of noncondensables and transferring the heat of condensation to feed urine was designed, fabricated, and tested. It was treated with steam/air mixtures at atmospheric and elevated pressures and integrated with an actual catalytic water recovery system. The condenser has a condensation efficiency exceeding 90% and heat transfer rate of approximately 85% of theoretical value at coolant temperature ranging from 7 to 80 deg C.

Budinikas, P.↗
DOE OSTI2023

Reaction process involving capillary condensation within a microporous catalyst

Described herein is a catalytic reaction process including introducing one or more gas-phase reactants into a reactor comprising a microporous catalyst having a pore size less than or equal to 2 nm and adjusting the temperature and/or the pressure of the reactor such that one or more of the gas-phase reactants condense within the micropores of the catalyst thereby causing the catalytic reaction to take place in a liquid phase. Additionally, a process for engineering defects on a carboxylate-based metal organic framework (MOF) catalyst is described. The process includes providing a carboxylate-based MOF catalyst; and heating the carboxylate-based MOF catalyst in an inert gas atmosphere at temperatures between about 150° C. and about 900° C.

Aguirrezabal, Iker↗
NASA NTRS1988

Appendices to the model description document for a computer program for the emulation/simulation of a space station environmental control and life support system

A Model Description Document for the Emulation Simulation Computer Model was already published. The model consisted of a detailed model (emulation) of a SAWD CO2 removal subsystem which operated with much less detailed (simulation) models of a cabin, crew, and condensing and sensible heat exchangers. The purpose was to explore the utility of such an emulation simulation combination in the design, development, and test of a piece of ARS hardware, SAWD. Extensions to this original effort are presented. The first extension is an update of the model to reflect changes in the SAWD control logic which resulted from test. Also, slight changes were also made to the SAWD model to permit restarting and to improve the iteration technique. The second extension is the development of simulation models for more pieces of air and water processing equipment. Models are presented for: EDC, Molecular Sieve, Bosch, Sabatier, a new condensing heat exchanger, SPE, SFWES, Catalytic Oxidizer, and multifiltration. The third extension is to create two system simulations using these models. The first system presented consists of one air and one water processing system. The second consists of a potential air revitalization system.

Yanosy, James L.↗
NASA NTRS1988

Appendices to the user's manual for a computer program for the emulation/simulation of a space station environmental control and life support system

A user's Manual for the Emulation Simulation Computer Model was published previously. The model consisted of a detailed model (emulation) of a SAWD CO2 removal subsystem which operated with much less detailed (simulation) models of a cabin, crew, and condensing and sensible heat exchangers. The purpose was to explore the utility of such an emulation/simulation combination in the design, development, and test of a piece of ARS hardware - SAWD. Extensions to this original effort are presented. The first extension is an update of the model to reflect changes in the SAWD control logic which resulted from the test. In addition, slight changes were also made to the SAWD model to permit restarting and to improve the iteration technique. The second extension is the development of simulation models for more pieces of air and water processing equipment. Models are presented for: EDC, Molecular Sieve, Bosch, Sabatier, a new condensing heat exchanger, SPE, SFWES, Catalytic Oxidizer, and multifiltration. The third extension is to create two system simulations using these models. The first system presented consists of one air and one water processing system, the second a potential Space Station air revitalization system.

Yanosy, James L.↗
DOE OSTI2026

Lignin Extraction and Condensation as a Function of Temperature, Residence Time, and Solvent System in Flow-through Reactors

Solvolytic extraction of lignin from biomass is a critical step in lignin-first biorefining, including the reductive catalytic fractionation (RCF) process. Key to optimal RCF processing is the ability to rapidly extract lignin from biomass at high delignification extents and transfer the lignin molecules to a catalyst surface in a time frame that minimizes lignin condensation reactions. Here, we use a flow-through reactor to study the effects of temperature (175–250 °C), residence time (9 to 36 min), and solvent composition (methanol and methanol–water) on lignin extraction and condensation. We evaluated three metrics at each condition: total delignification, delignification rate, and extent of condensation, the latter measured by a decrease in monomer yield for batch hydrogenolysis reactions of solvolysis liquor compared to batch RCF reactions. We observe that delignification is predominantly determined by temperature, while residence time dictates the lignin condensation extent. Moreover, the extent of both extraction and condensation increased in the methanol–water solvent system compared to that in the methanol system. Lignin extracted in methanol is stable up to 18-min residence times at or below 225 °C, while a majority of the lignin extracted in methanol–water is condensed with a 9-min residence time at 200 °C. These results can inform reactor designs and solvent selection for lignin-first biorefining processes that aim to physically separate the biomass and catalyst.

biorefining↗
NASA NTRS1971

Vacuum distillation: vapor filtered-catalytic oxidation water reclamation system utilizing radioisotopes

The development of a functional model water reclamation system is discussed. The system produces potable water by distillation from the urine and respiration-perspiration condensate at the normal rate generated by four men. Basic processes employed are vacuum distillation, vapor filtration, vapor phase catalytic oxidation, and condensation. The system is designed to use four 75-watt isotope heaters for distillation thermal input, and one 45-watt isotope for the catalytic oxidation unit. The system is capable of collecting and storing urine, and provides for stabilizing the urine by chemical pretreatment. The functional model system is designed for operation in a weightless condition with liquid-vapor phase separators for the evaporator still, and centrifugal separators for urine collection and vapor condensation. The system provides for storing and dispensing reclaimed potable water. The system operates in a batch mode for 40 days, with urine residues accumulating in the evaporator. The evaporator still and residue are removed to storage and replaced with a fresh still for the next 40-day period.

Honegger, R. J.↗
DOE OSTI2021

Catalytic Activity and Water Stability of the MgO(111) Surface for 2-Pentanone Condensation

Nanomaterials derived from earth-abundant metal oxides have gained tremendous interest as catalysts; although, water stability remains a challenge. This study examines MgO(111) surfaces for 2-pentanone condensation and their evolution during D2O hydration. Catalyst screening confirmed the high activity of fresh MgO(111) for 2-pentanone condensation relative to conventionally prepared MgO(100). Computational modeling suggests that the (111) surface is readily hydroxylated, and that surface hydroxyls help stabilize the surface and reduce the barrier for 2-pentanone condensation. Vapor-phase D2O hydration after 3 min increased MgO(111) hydroxyls and retained surface area and activity; however, after 1 h, deuteroxide formation reduced the surface area and activity by >30 %. After 24 h, deuteroxide growth slowed down, and surface area and activity remained stable. This suggests MgO(111)-derived hydroxide may be the dominant surface responsible for 2-pentanone condensation following water exposure. Thermal regeneration of the 24-h sample restored 86 % of the surface area and 94 % of the activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1980

A possible role of fluctuating clay-water systems in the production of ordered prebiotic oligomers

A model is proposed for the intermediate stages of prebiotic evolution, based on the characteristics of the adsorption and condensation of amino acids and nucleotides on the surface area of clay minerals in a fluctuating environment. Template replication and translation of adsorbed oligonucleotides and catalytic effects by peptide products on further condensation are proposed, due to specific properties of hypohydrous clay surfaces as well as the biomolecules themselves. Experimental evidence supports some of the proposed interactions, and all of them can be tested experimentally.

Lahav, N.↗
DOE OSTI2021

A bifunctional zeolitic porous liquid with incompatible Lewis pairs for antagonistic cascade catalysis

The emergence of porous liquids (PLs) opened opportunities to form unique antagonistic systems capable of fulfilling cascade reactions promoted by incompatible active sites in one pot, which is a long-term challenging subject in catalysis. Herein, unique bifunctional type III PL-based systems were facilely fabricated via assembly of zeolite nanosheets with ionic liquids. Rational structural design afforded PLs that feature high zeolite concentration, stable dispersion after 2 years, abundant cavity distribution, and involvement of antagonistic groups (acid and base sites) in separated and active form via steric hindrance control and electronic repulsion regulation. These unique properties worked cooperatively to fulfill the cascade deacetalization-Knoevenagel/Aldol condensation in one pot with superior catalytic efficiency outperforming the traditional systems. The key to success lies in the formation of bifunctional composites, transformation of zeolite from heterogeneous to homogeneous via surface modification, as well as rapid mass transfer ensured by the rigid porous architecture.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Cross-aldol condensation on missing linker sites of metal–organic framework UiO-66

Missing linkers induce coordinatively unsaturated Lewis acid-base pair sites in metal–organic frameworks such as UiO-66 (Zr). The Lewis acid-base pair is induced by replacing the benzene dicarboxylic acid linker with formic acid, which subsequently is thermally decomposed. The concentration of coordinatively unsaturated Zr 4+ cations was titrated with acetone. In parallel to their concentration, the catalytic activity increased while the selectivity for aldol condensation between furfural and acetone remained constant. The missing linkers generate a complex ensemble consisting of an (at least partly) accessible Zr 4+ cation surrounded by oxygen, catalyzing the cross-aldol condensation. As a result, density functional theory calculations, matching the experimental findings provide a more detailed understanding of the elementary steps during the condensation reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1994

Trace contaminant control simulation computer program, version 8.1

The Trace Contaminant Control Simulation computer program is a tool for assessing the performance of various process technologies for removing trace chemical contamination from a spacecraft cabin atmosphere. Included in the simulation are chemical and physical adsorption by activated charcoal, chemical adsorption by lithium hydroxide, absorption by humidity condensate, and low- and high-temperature catalytic oxidation. Means are provided for simulating regenerable as well as nonregenerable systems. The program provides an overall mass balance of chemical contaminants in a spacecraft cabin given specified generation rates. Removal rates are based on device flow rates specified by the user and calculated removal efficiencies based on cabin concentration and removal technology experimental data. Versions 1.0 through 8.0 are documented in NASA TM-108409. TM-108409 also contains a source file listing for version 8.0. Changes to version 8.0 are documented in this technical memorandum and a source file listing for the modified version, version 8.1, is provided. Detailed descriptions for the computer program subprograms are extracted from TM-108409 and modified as necessary to reflect version 8.1. Version 8.1 supersedes version 8.0. Information on a separate user's guide is available from the author.

Perry, J. L.↗