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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 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

In-situ magnetic alignment model for additive manufacturing of anisotropic bonded magnets

In this work, we report a mathematical framework which predicts the degree of alignment (DoA) in an in-situ aligned additively manufactured 3D printed bonded magnets. A multiphysics model is developed which couples the harmonious interactions of magnetic particles in a viscous flowing polymer under the presence of an external magnetic field. The hydrodynamic fluid-particle interaction is paired with the magnetophoretic force to predict the particle trajectory and distribution during extrusion through a 3D printer nozzle. Succeeding the force balance, a magnetohydrodynamic torque equilibrium analysis is performed to predict the net-orientation of the magnetic particles as a function of the applied field strength, viscous forces, and particle-to-particle interactions (P2P). Experimental validation of the DoA predictions is performed using 65 vol% Nd-Fe-B+Sm-Fe-N in Nylon12 (DoA exp = 0.620 and DoA theory = 0.686) and 15 vol% Sm-Co in PLA (DoA exp = 0.830 and DoA theory = 0.863). A parametric analysis is performed to analyze the effect of operating and design parameters like alignment field strength, magnetic loading fraction, extrusion load, and particle size. The model predicts a competing behavior between particle-fluid and particle-particle interactions under the presence of an applied field. Lastly, the model provides a framework to efficiently predict the DoA in tandem with a functionalized-magnetic 3D printer and allows the user to adjust the operating parameters according to the desired DoA.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Yor022c protein is a phospholipase A{sub 1} that localizes to the mitochondrial matrix

In mammals, three types of intracellular phospholipase A{sub 1} (iPLA{sub 1}) enzymes have been characterized and are thought to be involved in various cellular processes such as phospholipid metabolism, organelle biogenesis, and membrane trafficking. In this study we analyzed the unique iPLA{sub 1}-like protein, Yor022c, in the budding yeast Saccharomyces cerevisiae. By the mass spectrometry analysis, we demonstrate that Yor022c is actually a phospholipase displaying sn-1-specific activity toward phosphatidylcholine, phosphatidylethanolamine, and phosphatidic acid, generating 2-acyl lysophospholipids. GFP-fused Yor022c co-stained with the mitochondrial dye MitoTracker, indicating that, unlike its mammalian counterparts, it is a mitochondrial protein. Further biochemical fractionation experiment combined with protease sensitivity assay showed that Yor022c localizes to the mitochondrial matrix. Thus Yor022c is the first PLA{sub 1} putatively involved in the maintenance of sn-1 acyl chains of phospholipids in the mitochondrial inner membrane. - Highlights: • Yeast Yor022c protein displays phospholipase A{sub 1} activity to various phospholipids. • Yor022c-GFP fusion protein localizes to mitochondria. • Biochemical fractionation showed that Yor022c localizes to the mitochondrial matrix.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2018

Rbfox family proteins make the homo- and hetero-oligomeric complexes

Rbfox family of proteins that consists of Rbfox1, Rbfox2, and Rbfox3 in mammals regulates alternative pre-mRNA splicing in various tissues via direct binding to their RNA binding element. Although many studies have indicated the splicing activity of each member of the Rbfox family, the interactions of Rbfox family proteins are largely unknown. Here, we have investigated interactions among Rbfox family proteins. Co-immunoprecipitation (Co-IP) and GST-pull down assays confirmed that Rbfox proteins form homo and hetero complexes. Moreover, in vivo crosslinking using disuccinimidyl suberate treatment indicated that the Rbfox proteins form a dimer which then assembles with other proteins to form a large multiprotein complex. Duolink in situ proximity ligation (PLA) assay revealed that neuron specific Rbfox3 protein interacts with other Rbfox family proteins. This study is the first to provide an evidence that Rbfox family proteins form homo- and hetero-oligomeric complexes in vivo.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2018

Shape memory behavior and recovery force of 4D printed textile functional composites

Four-dimensional (4D) printing of multi-directionally reinforced preforms has tremendous potential for the development of next generation functional composites by using the capabilities of 3D printing technology, 3D textile preform design, and polymer shape memory behavior. This paper demonstrates the shape memory behavior and recovery force of 4D printed circular braided tube preforms and their silicone elastomer matrix composites. The preforms were printed by fused deposition modeling using the shape memory polymer (SMP), polylactic acid (PLA). The effects of braiding angle, tube wall thickness, and shape recovery temperature on the shape memory behavior of 4D printed tube preforms and their silicone elastomer matrix composites have been characterized. Measurements of shape recovery forces of the preform and composite were conducted using dynamic mechanical analysis (DMA). The braided microstructural parameters and shape recovery temperature have a significant effect on the preform shape memory behavior. The introduction of the silicone elastomer matrix greatly enhances the shape recovery force, shape recovery ratio, as well as radial compressive failure load of the 4D printed preform/silicone elastomer matrix composite. Finally, building on these results, a potential application for 4D printed textile functional composites is presented.

42 ENGINEERING↗
DOE OSTI2022

Application of the core shell model for strengthening polymer filament interfaces

While surface segregation has been intensively studied in thin films, relatively little has been investigated in filament geometries. In contrast to thin films, the filament surface forms a continuum, with interactions both at the free air and internal filament interface, which makes it difficult to achieve an equilibrium configuration. This asymmetry has become particularly apparent with the increasing use of additive manufacturing where entire structures are constructed via layered deposition of filamentous layers from a moving thermal nozzle. In addition, this process is highly non-equilibrated with poor thermal retention and is responsible for insufficient filament–filament interfacial fusion and internal pore formation along the printing direction. These features all contribute to poor mechanical and structural properties, which are exacerbated in semi-crystalline polymers, such as Polylactic Acid (PLA), where the melting point, T m , is much higher than the glass transition, T g . Even though system is liquid the molecules become ordered within the crystal structure and this ordering interferes with interdiffusion, which in turn prevents proper interfacial fusion. Capitalizing on the differential in surface tension, we show that addition of less than 1%, or trace amounts, of longer chain polymers, an oriented core shell structure, will be formed with a self-limiting thickness of three time the radius of gyration, R g , of the tracer chains. The lower T g of the tracers and their orientation makes them poised for interdiffusion when subsequent layers are deposited producing structures with significant improvement of the mechanical properties and internal structural integrity.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Creep suppression and fatigue in bio-based composites manufactured via conventional and large format additive manufacturing processes

The emergence of novel extrusion-based additive manufacturing (AM) processes has prompted the development of new thermoplastic composite feedstocks, and broadening sustainability initiatives have driven the development of bio-based and recyclable material for AM feedstocks. Poly(lactic acid) (PLA) with wood flour (WF) is one composite system that has been demonstrated in numerous AM applications, as well as traditional processing methods (i.e., compression and injection molding); however, there has been a need to understand how the variation in processing methodology impacts the material performance of these bio-based feedstocks from a fundamental perspective, with particular emphasis on creep for an extended application use-life. Herein, PLA/WF is explored as a feedstock material for large format additive manufacturing (LFAM) and the performance of additively manufactured materials is compared to those produced via more traditional processing methods. It is also demonstrated that the addition of WF decreases the material’s coefficient of thermal expansion (CTE) while increasing its Young’s modulus, susceptibility to water uptake, and creep fatigue resistance. Essentially, the addition of 20 wt% WF results in a 92 % decrease in rubbery regime CTE while simultaneously resulting in a 14 % increase in modulus, 190 % increase in water uptake, and a 31 % decrease in residual strain after cyclic creep tests. The processing method was also found to play a large role in the final part performance, with the printed material increasing the crystallinity by 183 % and 214 % compared to its compression and injection molded counterparts. Furthermore, the porosity of printed samples increased by two orders of magnitude compared to samples prepared via traditional processing methods.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Mixed polyester recycling can enable a circular plastic economy with environmental benefits

The mixed and varied nature of fossil-based and bio-based plastic waste requires complex and costly separations to enable compatibility with recycling technologies. A circular plastic economy based on mixed polyesters through cleaving ester bonds to produce monomers, while re-utilizing bio-based monomers to produce high-quality sustainable plastics, charts an exciting solution. However, the feasibility of such a circular economy solution remains underexplored. Here, in this study, we conducted a techno-economic analysis and life-cycle assessment of three polyester depolymerization recycling processes-methanolysis, glycolysis, and acid hydrolysis-for a mixed feedstock (polyethylene terephthalate [PET], polylactic acid [PLA], and polybutylene adipate terephthalate [PBAT]). Methanolysis outperforms glycolysis and hydrolysis economically and environmentally due to more efficient downstream separations, generating products with a 31% decrease in selling price and 21%-46% reduction in acidification, carcinogenic toxicity, fossil-fuel depletion, global warming potential, particulate formation, and smog formation compared to conventional polyester manufacturing. This study highlights the viability of a circular plastic economy for mixed polyesters via a single chemical recycling process.

09 BIOMASS FUELS↗
DOE OSTI2017

Development of a new approach based on midwave infrared spectroscopy for post-consumer black plastic waste sorting in the recycling industry

Highlights: • MWIR reflectance contact measurements were performed on post-consumer waste. • MWIR absorptions are found to be potentially suitable for black plastic resin classification. • MWIR is also potentially suitable for separation of coloured plastic and wood based products. • Atmospheric transmittance simulations suggest feasibility of stand-off measurements. - Abstract: Waste sorting is key to the process of waste recycling. Exact identification of plastic resin and wood products using Near Infrared (NIR, 1–1.7 µm) sensing is currently in use. Yet, dark targets characterized by low reflectance, such as black plastics, are hard to identify by this method. Following the recent success of Midwave Infrared (MWIR, 3–12 µm) measurements to identify coloured plastic polymers, the aim of this study was to assess whether this technique is applicable to sorting black plastic polymers and wood products. We performed infrared reflectance contact measurements of 234 plastic samples and 29 samples of wood and paper products. Plastic samples included black, coloured and transparent Polyethylene Terephthalate (PET), Polyethylene (PE), Polyvinyl Chloride (PVC), Polypropylene (PP), Polylactic acid (PLA) and Polystyrene (PS). The spectral signatures of the black and coloured plastic samples were compared with clear plastic samples and signatures documented in the literature to identify the polymer spectral features in the presence of coloured material. This information was used to determine the spectral bands that best suit the sorting of black plastic polymers. The main NIR-MWIR absorption features of wood, cardboard and paper were identified as well according to the spectral measurements. Good agreement was found between our measurements and the absorption features documented in the literature. The new approach using MWIR spectral features appears to be useful for black plastics as it overcomes some of the limitations in the NIR region to identify them. The main limitation of this technique for industrial applications is the trade-off between the signal-to-noise ratio of the sensor operating in standoff mode and the speed at which waste is moved under the sensor. This limitation can be resolved by reducing the system’s spectral resolution to 16 cm{sup −1}, which allows for faster spectra acquisition while maintaining a reasonable signal-to-noise ratio.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Formation of Disordered Cocontinuous Phases by Randomly Linked Star Copolymers

Cocontinuous polymeric nanostructures have garnered significant interest due to their ability to combine different properties of two separate polymer domains. Randomly linked copolymer networks have proven to be especially robust for formation of disordered cocontinuous phases across wide composition ranges (≈30 wt % or more). While theoretical treatments of microphase-separated networks have focused primarily on the role of random elastic forces imposed on the self-assembled nanostructures by virtue of the network architecture, experimental studies seeking to disentangle these contributions from other potential effects, such as dispersity in preferred interfacial curvatures, have been scarce. To provide insight into this matter, we here study the self-assembly of randomly linked star copolymers (RSCs), constructed by linking premade polymer arms of polystyrene (PS) and poly(d,l-lactide) (PLA) using 3, 4, and 6-functional connectors. This architecture yields similar distributions of preferred curvature as networks made using corresponding difunctional strands, but lacks the elastic forces imposed by a network architecture. Gravimetry and small-angle X-ray scattering, coupled with scanning electron microscopy, were performed to identify the percolation of PS/PLA RSCs. Remarkably, the 4-arm RSC system exhibited a disordered cocontinuous window of ≈25 wt %, indicating that dispersity in preferred curvature can in some cases be sufficient to robustly drive formation of this morphology. However, the other RSC architectures showed smaller cocontinuous ranges, which we interpret in terms of the influence of homopolymer stars in the 3-arm case and the narrower distribution of preferred interfacial curvatures in the 6-arm case. Finally, thin layers of interconnected porous PS were achieved by solution-processing, suggesting that RSCs have the potential to serve as a robust and easily processable cocontinuous polymeric nanomaterials in both bulk and membrane geometries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Microphase Separation of Randomly Linked Branched Polystyrene/Polylactic Acid for Formation of Cocontinuous Nanostructures

Cocontinuous polymeric nanomaterials have gained attention for their ability to preserve distinct properties of constituent microphases within a single material. Randomly linked copolymer networks have shown very wide stability windows for disordered cocontinuous phases (extending over ≈ 30 wt % in composition), but the reliance on a network architecture prevents subsequent solution- or melt-processing. Furthermore, the key factors contributing to cocontinuity have remained unclear. We recently found that randomly linked star copolymers (RSCs) can exhibit a cocontinuous window as wide as 25 wt % in the case of 4-arm stars, suggesting that while a network architecture is not essential for the formation of disordered cocontinuous phases, the presence of random elastic forces in such architectures may indeed facilitate their formation. In addition, the behavior was found to be highly sensitive to arm number, with 6-arm RSCs exhibiting almost no cocontinuous phase. These results raised a key mechanistic question regarding the contribution of random elastic forces, originating from strands that bridge between junctions, in stabilizing disordered cocontinuous phases. In the current study, we synthesized randomly linked branched copolymers (RBCs) of polystyrene (PS) and poly(D,L-lactic acid) (PLA), which represent an intermediate architecture between networks and stars. This approach allows for the introduction of elastic contributions from strands bridging between different junctions, while still maintaining the processability advantages of a non-network architecture. The cocontinuous regions of the PS/PLA RBCs, with varying polymer and linker functionalities (f p and f l , respectively), were characterized by small-angle X-ray scattering, gravimetry, and scanning electron microscopy. We found that the cocontinuous windows of RBCs typically expanded with increasing elastic contributions and exhibited reduced sensitivity to junction-functionality compared to RSCs. Notably, RBCs with f p = 1.50 and f l = 3, which had large molecular weights due to proximity to the gel point, achieved a cocontinuous window of ≈ 34 wt %, which is almost twice as wide as analogous 3-arm RSCs and comparable to randomly linked networks. Leveraging this robust cocontinuity and solution-processability, we fabricated a film of interconnected nanoporous PS.

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

Poly(lactic acid)-Based Ink for Biodegradable Printed Electronics With Conductivity Enhanced through Solvent Aging

Biodegradable electronics is a rapidly growing field, and the development of controllably biodegradable, high-conductivity materials suitable for additive manufacturing under ambient conditions remains a challenge. Here, printable conductive pastes that employ poly(lactic acid) (PLA) as a binder and tungsten as a conductor are demonstrated. These composite conductors can provide enhanced stability in applications where moisture may be present, such as environmental monitoring or agriculture. Post-processing the printed traces using a solvent-aging technique increases their conductivity by up to 2 orders of magnitude, with final conductivities approaching 5000 S/m. Such techniques could prove useful when thermal processes including heating or laser sintering are limited by the temperature constraints of typical biodegradable substrates. Finally, both accelerated oxidative and hydrolytic degradation of the printed composite conductors are examined, and a fully biodegradable capacitive soil moisture sensor is fabricated and tested.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Assembly of Disordered Cocontinuous Morphologies by Multiblock Copolymers with Random Block Sequence and Length Dispersity

Among the wide variety of nanostructures accessible by self-assembly of block copolymers, cocontinuous morphologies are of great interest for separations, catalysis, sensing, and energy storage due to their ability to integrate distinct properties of the constituent polymers. Furthermore, we investigate the tendency to form disordered cocontinuous phases of multiblock copolymers (MBCs) with random block sequence and length dispersity prepared by step-growth polymerization of pre-made telechelic polymers, specifically using thiol-Michael addition between diacrylate functionalized polystyrene (PS) and poly (D,L - lactide) (PLA) chains and a small molecule dithiol. In the phase diagram so established, disordered cocontinuous nanostructures occupy a wide window (≈ 25 % vol) at a modest segregation strength of χN = 15, close to the critical value for microphase separation. At a higher segregation strength of χN = 30, only a moderately wide (≈ 10 vol %) cocontinuous window is found, with MBCs instead tending to form ordered nanostructures. Although the breadth of the cocontinuous widow is less than that found in prior work on analogous randomly end-linked copolymer networks (RECNs), the MBC architecture offers offsetting advantages in terms of solution and melt processability.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Regio- and Stereoselective Lactone Polymerization: Divergent Effect of Catalyst Modification and Monomer Structure

Selective ring-opening polymerization (ROP) of chiral lactones enables access to biodegradable polyesters with precisely controlled microstructures. Here, combined DFT modeling and experimental validation elucidate how fine-tuning of enantiopure SalBinam aluminum catalysts (through introduction of bromine atoms and tert-butyl groups, respectively, in ortho- and para-positions) modulates regio- and stereocontrol in the ROP of methyl glycolide (MeG) and lactide (LA). Computations reveal that regioselectivity in MeG polymerization arises mainly from steric repulsion, with a small contribution from weak stabilizing C-H···Br interactions that favor ring-opening at the glycolic site, consistent with the experimentally enhanced regioselectivity for (R)-MeG. In contrast, the same steric congestion at the ligand’s ortho positions destabilizes the key transition states in rac-LA polymerization, reducing the calculated stereoselectivity. Experiments confirm the predicted loss of stereocontrol, yielding nearly atactic PLA under standard conditions. Extension of the computational framework to rac-MeG polymerization promoted by racemic catalyst identified a low-barrier, stepwise polymer chain exchange pathway that rationalizes the experimentally observed syndiotacticity of poly(lactic-co-glycolic acid).

DFT calculations↗
DOE OSTI2017

Effects of Grafting Density on Block Polymer Self-Assembly: From Linear to Bottlebrush

Grafting density is an important structural parameter that imparts significant influences over the physical properties of architecturally complex polymers. In this paper, the physical consequences of varying the grafting density (z) were studied in the context of block polymer self-assembly. Well-defined block polymers spanning the linear, comb, and bottlebrush regimes (0 ≤ z ≤ 1) were prepared via grafting-through ring-opening-metathesis polymerization (ROMP). ω-norbornenyl poly(D,L-lactide) (PLA) and polystyrene (PS) macromonomers were copolymerized with discrete co-monomers in different feed ratios, enabling precise control over the grafting density. Small-angle X-ray scattering (SAXS) experiments demonstrate that these graft block polymers can self-assemble into long-range-ordered lamellar structures. For seventeen series of block polymers with variable z, the scaling of the lamellar period with the total backbone degree of polymerization (d* ~ N bb α ) was studied. The scaling exponent α monotonically decreases with decreasing z and exhibits an apparent transition at z ≈ 0.2, suggesting significant changes in the chain conformations. Comparison of two block polymer systems, one that is strongly segregated for all z (System I) and one that experiences weak segregation at low z (System II), indicates that the observed trends are primarily caused by the polymer architectures, instead of segregation strengths. A model is pro-posed in which the characteristic ratio (C ∞ ), a proxy for the backbone stiffness, scales with N bb as a function of the grafting density: C ∞ ~ N bb f(z) . To the best of our knowledge, this report represents the first study of scaling behavior for the self-assembly of block polymers with variable grafting density. Lastly, the relationships disclosed herein provide valuable insights into conformational changes with grafting density, thus introducing new opportunities for future block polymer design.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Design, Synthesis, and Self-Assembly of Polymers with Tailored Graft Distributions

Grafting density and graft distribution impact the chain dimensions and physical properties of polymers. However, achieving precise control over these structural parameters presents long-standing synthetic challenges. In this report, we introduce a versatile strategy to synthesize polymers with tailored architectures via grafting-through ring-opening metathesis polymerization (ROMP). One-pot copolymerization of an ω-norbornenyl macromonomer and a discrete norbornenyl co-monomer (diluent) provides opportunities to control the backbone sequence and therefore the side chain distribution. Toward sequence control, the homopolymerization kinetics of 23 diluents were studied, representing diverse variations in the stereochemistry, anchor groups, and substituents. These modifications tuned the homopolymerization rate constants over two orders of magnitude (0.36 M -1 s -1 < k homo < 82 M -1 s -1 ). Rate trends were identified and elucidated by complementary mechanistic and density functional theory (DFT) studies. Building on this foundation, complex architectures were achieved through copolymerizations of selected diluents with a poly (D,L-lactide) (PLA), polydimethylsiloxane (PDMS), or polystyrene (PS) macromonomer. The cross-propagation rate constants were obtained by non-linear least squares fitting of the instantaneous co-monomer concentrations according to the Mayo-Lewis terminal model. Indepth kinetic analyses indicate a wide range of accessible macromonomer/diluent reactivity ratios (0.08 < r 1 /r 2 < 20), corresponding to blocky, gradient, or random backbone sequences. We further demonstrated the versatility of this copolymerization approach by synthesizing AB graft diblock polymers with tapered, uniform, and inverse-tapered molecular “shapes.” Small-angle X-ray scattering analysis of the self-assembled structures illustrates effects of the graft distribution on the domain spacing and backbone conformation. Collectively, the insights provided herein into the ROMP mechanism, monomer design, and homo- and copolymerization rate trends offer a general strategy for the design and synthesis of graft polymers with arbitrary architectures. Lastly, controlled copolymerization therefore expands the parameter space for molecular and materials design.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Depolymerization of polyesters by a binuclear catalyst for plastic recycling

Plastics play an essential role in modern society, however, the relentless growth of their production is threatening both human health and ecosystems. As a result, there are intensive efforts in developing recycling technologies to repurpose waste plastics into the building blocks for valuable materials. Here we show a binuclear complex that can catalyze the degradation of polyethylene terephthalate (PET)-the most widely used polyester globally-and a wide spectrum of other plastics including polylactic acid (PLA), polybutylene adipate terephthalate (PBAT), polycaprolactone (PCL), polyurethane (PU) and Nylon 66. Inspired by hydrolases, the group of enzymes that catalyze bond cleavages with water, the present catalyst design features biomimetic Zn-Zn sites which activate the plastic, stabilize the key intermediate, and enable intramolecular hydrolysis. This synthetic catalyst delivers activities of 36 mg PET d -1 g catal -1 toward PET depolymerization at pH 8 and 40 oC, and of 577 g PET d -1 g catal -1 at pH 13 and 90 oC for scalable PET recycling. We further demonstrate the closed-loop production of a bottle-grade PET. This work presents a practical and viable solution to the sustainable management of plastics waste.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Structure-guided functional studies of plasmid-encoded dihydrofolate reductases reveal a common mechanism of trimethoprim resistance in Gram-negative pathogens

Two plasmid-encoded dihydrofolate reductase (DHFR) isoforms, DfrA1 and DfrA5, that give rise to high levels of resistance in Gram-negative bacteria were structurally and biochemically characterized to reveal the mechanism of TMP resistance and to support phylogenic groupings for drug development against antibiotic resistant pathogens. Preliminary screening of novel antifolates revealed related chemotypes that showed high levels of inhibitory potency against Escherichia coli chromosomal DHFR (EcDHFR), DfrA1, and DfrA5. Kinetics and biophysical analysis, coupled with crystal structures of trimethoprim bound to EcDHFR, DfrA1 and DfrA5, and two propargyl-linked antifolates (PLA) complexed with EcDHFR, DfrA1 and DfrA5, were determined to define structural features of the substrate binding pocket and guide synthesis of pan-DHFR inhibitors.

59 BASIC BIOLOGICAL SCIENCES↗