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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 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Enhanced Carbon Capture Behavior of Carbon Fibers via Ionic Liquid Modification

Carbon-based materials are widely deployed in carbon capture but are only limited to physisorption procedures. Further extending functionalized carbon materials to CO 2 chemisorption under low CO 2 concentration is highly desirable yet challenging. In this study, a carbon fiber composed of solely ultra-micropores (~0.45 nm) was deployed as the precursor to avoid the pore blocking effect, which was modified by superbase-derived ionic liquids (ILs) containing strong interaction sites with CO 2 . By forming a thin coating layer on the surface, the as-afforded surface-functionalized fiber materials demonstrated enhanced CO 2 uptake capacity and improved CO 2 sorption kinetics, as evaluated by both the volumetric method and thermogravimetric analysis, as well as the calculated energy distribution curves. The achievements made in this work provide guidance on the functionalization of carbon-based materials towards enhanced CO 2 chemisorption by forming a thin layer of selected IL coating.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Counterintuitive Catalytic Reactivity of the Aluminum Oxide “Passivation” Shell of Aluminum Nanoparticles Facilitating the Thermal Decomposition of exo -Tetrahydrodicyclopentadiene (JP-10)

High energy density aluminum nanoparticles (AlNP) have been at the center of attention as additives to hydrocarbon jet fuels like exo-tetrahydrodicyclopentadiene (JP-10, C 10 H 16 ) aiming at a superior performance of volume-limited air-breathing propulsion systems. However, a fundamental understanding of the ignition and combustion chemistry of JP-10 in presence of AlNPs has been elusive. Exploiting an isomer-selective comprehensive identification of the decomposition products in a newly designed high temperature chemical microreactor coupled to vacuum ultraviolet photoionization, we reveal an active low temperature heterogeneous surface chemistry commencing at 650 K involving the alumina (Al 2 O 3 ) shell. Contrary to textbook knowledge of an “inactive alumina surface”, this unconventional reactivity, where oxygen is transferred from alumina to JP-10, leads to generating cyclic, oxygenated organics like phenol (C 6 H 5 OH) and 2,4-cyclopentadiene-1-one (C 5 H 4 O) - key tracers of an alumina-mediated interfacial chemistry. Furthermore, this counterintuitive reactivity transforms our knowledge on the (catalytic) processes of alumina-coated AlNPs on the molecular level.

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

Command of active and responsive elastomers by topological defects and patterns

The project resulted in the development of stimuli-responsive elastomer coatings formed by photopolymerized liquid crystal molecules. The molecular orientation of the liquid crystal elastomers is coupled to rubber-like elasticity. The project developed an approach to produce complex patterns of molecular orientation in elastomers by employing photopatterning technique based on plasmonic metamasks that convert unpolarized incoming light into a transmitted light beam with spatially-varying linear polarization. The polarization-modulated light beam aligns the film of azodye molecules, which serves as the substrate for liquid crystal elastomer coating. The alignment of the azodye molecules follows the polarization pattern with a phase shift of the alignment direction by 90 degrees. The azodye substrate imposes orientation of molecules in the adjacent liquid crystal layer which is preserved after the monomers are polymerized into a liquid crystal elastomer. By using differently aligned substrates one could produce various patterns of molecular orientation in the elastomer, which dictate the mechanical properties of the elastomers and their response to external stimuli such as temperature, humidity, and ultraviolet irradiation. In particular, the predesigned molecular orientation produces deterministically defined topography response of the liquid crystal coatings, in which their free surface changes from flat to either locally elevated or locally compressed, depending on whether the pre-inscribed molecular orientation is predesigned with a splay or bend deformation. The research established that the mechanism of this deterministic relation between the dynamic topography and pre-inscribed molecular orientation is rooted in the change of the tensorial order parameter that characterizes the degree of orientational order, and in the contraction/expansion of polymer molecules in response to the order parameter changes. In particular, lowering the order causes contraction of polymer globules. The work demonstrated that the dynamic topography of elastomer coatings with three-dimensional pattern of orientational order includes up and down motion of the material (along the normal to the coating) and also shifts in lateral directions. We demonstrate that the deterministic relationship between the orientational patterns and variations of coatings’ profile is caused by forces that are mathematically equivalent to active forces in the system of “pullers” or “pushers” in active matter, demonstrating universality of the out-of-equilibrium behavior. The project resulted in theoretical models that predictively describe the dynamic response of coatings. The topography of liquid crystal elastomers is sensitive to stimuli such as temperature, ultraviolet irradiation, and humidity. The applicability of the patterned approach to produce dynamic coatings was expanded from nematic elastomers to their smectic counterparts. The project combined a battery of imaging techniques to unveil the dynamic properties of the coatings, ranging from the state-of-the-art dynamic holographic microscopy to fluorescent confocal polarizing microscopy and polscope microscopy. The research uncovered potential applications of dynamic elastomer coatings, such as control placement of colloidal particles, engineering of living tissues with alignment patterns of cells that follow the orientational order of elastomer coatings. The approach developed in the project can be used to design programmable dynamic coatings with functionalities that mimic biological tissues such as skin.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Lithium battery cathode

A novel lithium battery cathode, a lithium ion battery using the same and processes and preparation thereof are disclosed. The battery cathode is formed by force spinning. Fiber spinning allows for the formation of core-shell materials using material chemistries that would be incompatible with prior spinning techniques. A fiber spinning apparatus for forming a coated fiber and a method of forming a coated fiber are also disclosed.

25 ENERGY STORAGE↗
DOE OSTI2020

Elastic gas barrier coating compositions

An elastic gas barrier coating composition includes a barrier material dispersed in an aqueous media, a polysulfide, and a curing agent reactive with the polysulfide. When applied to a substrate and cured to form a coating, the barrier material forms a continuous phase and a polysulfide elastomer forms a discontinuous phase. An elastic gas coating is also disclosed that includes a continuous phase with a barrier material and a discontinuous phase with a polysulfide elastomer. Substrates at least partially coated with elastic gas barrier coating compositions are further disclosed.

36 MATERIALS SCIENCE↗
NASA NTRS2014

Characterization of Encapsulated Corrosion Inhibitors for Environmentally Friendly Smart Coatings

Research efforts are under way to replace current corrosion inhibitors with more environmentally friendly alternatives. However, problems with corrosion inhibition efficiency, coating compatibility and solubility have hindered the use of many of these materials as simple pigment additives.This paper will present technical details on how the Corrosion Technology Lab at NASAs Kennedy Space Center (KSC) has addressed these issues by encapsulating environmentally friendly inhibitors into organic and inorganic microparticles and microcapsules. The synthetic process for polymer particles was characterized and post-synthesis analysis was performed to determine the interactions between the inhibitors and the encapsulation material. The pH-controlled release of inhibitors from various particle formulations in aqueous base was monitored and compared to both electrochemical and salt immersion accelerated corrosion experiment. Furthermore, synergistic corrosion inhibition effects observed during the corrosion testing of several inhibitor combinations will be presented.

Environmentally Friendly↗
DOE OSTI2022

Flash Recycling of Graphite Anodes

The ever-increasing production of commercial lithium-ion batteries (LIBs) will result in a staggering accumulation of waste when they reach their end of life. A closed-loop solution, with effective recycling of spent LIBs, will lessen both the environmental impacts and economic cost of their use. Presently, <5% of spent LIBs are recycled and the regeneration of graphite anodes has, unfortunately, been mostly overlooked despite the considerable cost of battery-grade graphite. Here, in this work, an ultrafast flash recycling method to regenerate the graphite anode is developed and valuable battery metal resources are recovered. Selective Joule heating is applied for only seconds to efficiently decompose the resistive impurities. The generated inorganic salts, including lithium, cobalt, nickel, and manganese, can be easily recollected from the flashed anode waste using diluted acid, specifically 0.1 M HCl. The flash-recycled anode preserves the graphite structure and is coated with a solid-electrolyte-interphase-derived carbon shell, contributing to high initial specific capacity, superior rate performance, and cycling stability, when compared to anode materials recycled using a high-temperature-calcination method. Life-cycle-analysis relative to current graphite production and recycling methods indicate that flash recycling can significantly reduce the total energy consumption and greenhouse gas emission while turning anode recycling into an economically advantageous process.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Hybrid nanocapsules for in situ TEM imaging of gas evolution reactions in confined liquids

Liquid cell transmission electron microscopy (TEM) enables the direct observation of dynamic physical and chemical processes in liquids at the nanoscale. Quantitative investigations into reactions with fast kinetics and/or multiple reagents will benefit from further advances in liquid cell design that facilitate rapid in situ mixing and precise control over reagent volumes and concentrations. This work reports the development of inorganic–organic nanocapsules for high-resolution TEM imaging of nanoscale reactions in liquids with well-defined zeptoliter volumes. These hybrid nanocapsules, with 48 nm average diameter, consist of a thin layer of gold coating a lipid vesicle. As a model reaction, the nucleation, growth, and diffusion of nanobubbles generated by the radiolysis of water is investigated inside the nanocapsules. When the nanobubbles are sufficiently small (10–25 nm diameter), they are mobile in the nanocapsules, but their movement deviates from Brownian motion, which may result from geometric confinement by the nanocapsules. Gases and fluids can be transported between two nanocapsules when they fuse, demonstrating in situ mixing without using complex microfluidic schemes. The ability to synthesize nanocapsules with controlled sizes and to monitor dynamics simultaneously inside multiple nanocapsules provides opportunities to investigate nanoscale processes such as single nanoparticle synthesis in confined volumes and biological processes such as biomineralization and membrane dynamics.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Revealing in-plane movement of platinum in polymer electrolyte fuel cells after heavy-duty vehicle lifetime

Fuel cell heavy-duty vehicles (HDVs) require increased durability of oxygen-reduction-reaction electrocatalysts, making knowledge of realistic degradation mechanisms critical. Here identical-location micro-X-ray fluorescence spectroscopy was performed on membrane electrode assemblies. The results exposed heavy in-plane movement of electrocatalyst after HDV lifetime, suggesting that electrochemical Ostwald ripening may not be a local effect. Development of local loading hotspots and preferential movement of electrocatalyst away from cathode catalyst layer cracks was observed. The heterogeneous degradation exhibited by a modified cathode gas diffusion layer membrane electrode assembly after HDV lifetime was successfully quantified by the identical-location approach. Further synchrotron micro-X-ray diffraction and micro-X-ray fluorescence experiments were performed to obtain the currently unknown correlation between electrocatalyst nanoparticle size increase and loading change. A direct correlation was discovered which developed only after HDV lifetime. Finally, the work provides a route to engineer immediate system-level mitigation strategies and to develop structured cathode catalyst layers with durable electrocatalysts.

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

The nanocaterpillar's random walk: diffusion with ligand–receptor contacts

Particles with ligand–receptor contacts bind and unbind fluctuating “legs” to surfaces, whose fluctuations cause the particle to diffuse. Quantifying the diffusion of such “nanoscale caterpillars” is a challenge, since binding events often occur on very short time and length scales. Here, in this work, we derive an analytical formula, validated by simulations, for the long time translational diffusion coefficient of an overdamped nanocaterpillar, under a range of modeling assumptions. We demonstrate that the effective diffusion coefficient, which depends on the microscopic parameters governing the legs, can be orders of magnitude smaller than the background diffusion coefficient. Furthermore it varies rapidly with temperature, and reproduces the striking variations seen in existing data and our own measurements of the diffusion of DNA-coated colloids. Our model gives insight into the mechanism of motion, and allows us to ask: when does a nanocaterpillar prefer to move by sliding, where one leg is always linked to the surface, and when does it prefer to move by hopping, which requires all legs to unbind simultaneously? We compare a range of systems (viruses, molecular motors, white blood cells, protein cargos in the nuclear pore complex, bacteria such as Escherichia coli, and DNA-coated colloids) and present guidelines to control the mode of motion for materials design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

In situ study of Crystal Surface Interactions Guided by Biomolecules or Ligands

Ligands or biomolecules commonly exist and play a key role in particle-mediated materials growth, leading to a wide variety of structures. However, it is not fully understood how these organic molecules control forces interacting between particles and thus the dynamics of particle assembly. Herein, the overall goal of this project is to gain an understanding of the role of surface-coating materials (ligands and biomolecules) in particle assembly processes; that is, how surface-coating materials determine the interfacial structures of solvent/ligand (biomolecule)/crystal surface and thus the interaction forces.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Chemical properties and single-particle mixing state of soot aerosol in Houston during the TRACER campaign

Abstract. A high-resolution soot particle aerosol mass spectrometer (SP-AMS) was used to selectively measure refractory black carbon (rBC) and its associated coating material using both the ensemble size-resolved mass spectral mode and the event trigger single particle (ETSP) mode in Houston, Texas, in summer 2022. This study was conducted as part of the Department of Energy Atmospheric Radiation Measurement (ARM) program's TRacking Aerosol Convection interactions ExpeRiment (TRACER) field campaign. The study revealed an average (±1σ) rBC concentration of 103 ± 176 ng m−3. Additionally, the coatings on the BC particles were primarily composed of organics (59 %; 219 ± 260 ng m−3) and sulfate (26 %; 94 ± 55 ng m−3). Positive matrix factorization (PMF) analysis of the ensemble mass spectra of BC-containing particles resolved four distinct types of soot aerosol, including an oxidized organic aerosol (OOABC,PMF) factor associated with processed primary organic aerosol, an inorganic sulfate factor (SO4,BC,PMF), an oxidized rBC factor (O-BCPMF), and a mixed mineral dust–biomass burning aerosol factor with significant contribution from potassium (K-BBBC,PMF). Additionally, K-means clustering analysis of the single-particle mass spectra identified eight different clusters, including soot particles enriched in hydrocarbon-like organic aerosol (HOABC,ETSP), sulfate (SO4,BC,ETSP), two types of rBC, OOA (OOABC,ETSP), chloride (ClBC,ETSP), and nitrate (NO3,BC,ETSP). The single-particle measurements demonstrate substantial variation in BC coating thickness with coating-to-rBC mass ratios ranging from 0.1 to 100. The mixing state index (χ), which denotes the degree of homogeneity of the soot aerosol, varied from 4 % to 94 % with a median of 40 %, indicating that the aerosol population lies in between internal and external mixing but has large temporal and source type variability. In addition, a significant fraction of BC-containing particles, a majority enriched with oxidized organics and sulfate, exhibit sufficiently high κ values and diameters conducive to activation as cloud nuclei under atmospherically relevant supersaturation conditions. This finding bears significance in comprehending the aging processes of rBC-containing particles and their activation into cloud droplets. Our analysis highlights the complex nature of soot aerosol and underscores the need to comprehend its variability across different environments for accurate assessment of climate change.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

SI-PET-RAFT Polymerization via Electrodeposited Macroinitiator Thin Films: Toward Biomedical and Sensing Applications

Surface-initiated photoinduced electron transfer-reversible addition–fragmentation chain transfer (SI-PET-RAFT) polymerization has been preferentially used for preparing thin polymeric film coatings due to its simple execution under ambient conditions (e.g., in air) and visible light requirement. In this study, we demonstrate the preparation of polymer brushes by SI-PET-RAFT polymerization on a thin macroinitiator film electrodeposited on electrically conductive indium tin oxide and gold surfaces. An electrochemically active carbazole-containing chain transfer agent as macroinitiator was shown to be not only effective in mediating SI-PET-RAFT polymerization for various monomers but also capable of forming block copolymers. Additionally, the fabricated polymer brush films were able to encapsulate colloidal gold nanoparticles, thereby demonstrating potential use for biomedical and sensing applications.

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

Printing 2D Conjugated Polymer Monolayers and Their Distinct Electronic Properties

Abstract Recently, 2D monolayer films of conjugated polymers have gained increasing attention owing to the preeminence of 2D inorganic films that exhibit unique optoelectronic and mechanical properties compared to their bulk analogs. Despite numerous efforts, crystallization of semiconducting polymers into highly ordered 2D monolayer films still remains challenging. Herein, a dynamic‐template‐assisted meniscus‐guided coating is utilized to fabricate continuous, highly ordered 2D monolayer films of conjugated polymers over a centimeter scale with enhanced backbone π–π stacking. In contrast, monolayer films printed on solid substrates confer upon the 1D fiber networks strong alkyl side‐chain stacking at the expense of backbone packing. From single‐layers to multilayers, the polymer π‐stacks change from edge‐on to bimodal orientation as the film thickness reaches ≈20 nm. Spectroscopic and cyclic voltammetry analysis reveals an abrupt increase in J‐aggregation and absorption coefficient and a decrease in bandgap and highest occupied molecular orbital level until critical thickness, possibly arising from the straightened polymer backbone. This is corroborated by an abrupt increase in hole mobility with film thickness, reaching a maximum of 0.7 cm 2 V −1 s −1 near the critical thickness. Finally, fabrication of chemical sensors incorporating polymer films of various thicknesses is demonstrated, and an ultrahigh sensitivity of the ≈7 nm thick ultrathin film (bilayers) to 1 ppb ammonia is shown.

Kafle, Prapti↗
NASA NTRS2001

The Combined Detection of Morphological and Molecular Biomarkers: Implications for Astrobiology

Experience gathered by previous researchers during their hunt for evidence of early Earth life has shown the complexity in interpreting observations of possible microfossils and to establish the evidence to be positive. Similarly, the stillsimmering controversy on the nature of the nano-structures in Martian meteorite ALH84001 described by McKay et al. (1996) emphasizes the difficulties of conclusively identifying those structures as (a) fossilized bacterial cells and (b) establish their indigeneity. A better understanding of biological signatures in rocks is needed in order to identify traces of microbial life, which include morphological, mineralogical and chemical traces. It is thus considered crucial to tackle the problems emerging in the search for evidence of early life on Earth and in exopaleontological research with a multidisciplinary approach. With this is mind we applied surface sensitive Time of Flight-Secondary Ion Mass Spectroscopy (ToF-SIMS) to a previously described 25 m.y. old fossil bacterial biofilm. This technique allows in situ analysis with high mass resolution as well as molecular imaging of micron sized structures. As no extraction or derivatisation of the sample is required for ToF-SIMS analysis, electron microscopical investigation of the same samples subsequent to analysis is possible, thus allowing the combination of molecular and morphological biomarkers. The analysed fossil bacterial biofilms were associated with macrofossils from volcanoclastic lacustrine sediments from the Upper Oligocene Enspel formation (Germany). Preliminary scanning electron microscopy (SEM) studies have shown that a fossil structure interpreted as a coprolite purely consisted of fossilized bacterial biofilm. For ToF-SIMS investigation small particles were taken from the fossil biofilm and mounted onto Au-coated In-foil and analysed in a Phi Evans T-2000 TRIFT system. The ToF-SIMS analysed samples were Au/Pd-sputter coated and imaged using a Philips XL40 Field Emission Gun SEM (FEG-SEM). ToF-SIMS analysis of the organic rich fossil biofilm (TOC 29%) in the 0-100 Dalton (Da) range showed significant amounts of inorganic species, confirming the results obtained previously by EDX analysis, clearly showing the bacterial fossils to be mineralised. ToF-SIMS furthermore revealed the presence of a variety of low- and high-mass organic molecules and fragments thereof. These include peaks indicative of alkenes and alkanes, aromatic organic species and the polycyclic aromatic hydrocarbon naphthalene. More tentatively, peaks indicative of alkyl pyrroles and pyridyl-CH2 were identified. Other peaks of interest include peaks indicative of C(n)H(2n)O2 and C(n)H(2n-2)O2, which according to their general formula would suggest the presence of both saturated and unsaturated fatty acids although further in situ derivatisation experiments and GC-MS (Gas Chromatography MS) need to be applied to verify this beyond doubt. Furthermore, peaks at m/z 370, 384, 398, 412, 426, 440, 454 and 468 were identified, which indicate the potential presence of bacterial hopanes, a class of biomarkers indicative of bacteria. The main diagnostic peak for this group of chemicals is the fragment at m/z 191.18. Our studies conducted on purified hopane standards have shown that in the high-mass resolution mode differentiation of this diagnostic hopane peak and polyethylene at m/z 191.05 is possible. However, the spectra discussed here were collected in the lower resolution mapping mode, therefore this differentiation was not possible. The centroids of the possible hopane peaks obtained on the fossil biofilms are well within the range associated with bacterial hopanes. There is a strong possibility therefore that hopanoids may be associated with the fossil bacterial cells. Due to the non-destructive nature of ToF-SIMS, analysed samples can be studied using SEM, thus allowing the combination of morphological and molecular biomarkers. Subsequent SEM analysis of the ToF-SIMS analysed samples confirmed that the analysed material purely consists of fossil bacterial cells. This is thus the first successful effort to demonstrate the combination of spectral and morphological biomarkers. The advantages of highly sensitive non-destructive in situ analysis techniques for biomarker detection are invaluable, particularly with respect to envisaged Mars sample return missions, as it may allow us to identify remains and traces of former microbial life in both ancient terrestrial and extraterrestrial materials. This technique may prove particularly useful in the quest for extraterrestrial life with respect to precious extraterrestrial materials, as minute quantities are sufficient to conduct analysis.

Toporski, J.↗
NASA NTRS1996

Protective Coatings

Ameron International Protective Coatings Group developed a special coating for NASA that would withstand the high temperatures generated by the Space Shuttle rocket engines. The coating remains intact for at least 10 minutes, and insulates the launch pad so that it does not exceed 150 degrees and buckle. The NASA formulation was from Ameron's Engineered Siloxane (PSX) chemistry, which employs an inorganic silicon-oxygen structure which the company states is stronger and more reliable than organic polymers. Some of Ameron's PSX product line is based on the NASA technology, used for everything from industrial equipment to bridges.

Source record↗
DOE OSTI2023

Surface-Modified Pd/CeO 2 Single-Atom Catalyst Shows Increased Activity for Suzuki Cross-Coupling

Single-atom catalysts (SACs) comprise catalytically active atoms dispersed on supports; they combine the high activity and site uniformity of homogeneous catalysts with the ease of separability of heterogeneous catalysts. However, SACs lack fine control over the active site, provided by ligands in homogeneous catalysts. In this work, we demonstrate that modification of the support with an organic monolayer is a viable approach to improving the catalytic performance. Here, the addition of catechol-type monolayers to a Pd/CeO 2 SAC increases its catalytic activity for Suzuki cross-coupling, a central reaction in the synthesis of fine chemicals and pharmaceuticals. Kinetic trials reveal that the coating reduces the activation energy from 49 ± 9 to 22 ± 5 kJ/mol and produces a 4-fold rate enhancement at 25 °C, an effect we attribute to π-π interactions between the reactant and the catechol coating. Further development of this approach could vastly increase the utility of SACs in organic synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗