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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Spatiotemporal Control over Polynucleotide Brush Growth on DNA Origami Nanostructures

DNA nanotechnology provides an approach to create precise, tunable, and biocompatible nanostructures for biomedical applications. However, the stability of these structures is severely compromised in biological milieu due to their fast degradation by nucleases. Recently, we showed how enzymatic polymerization could be harnessed to grow polynucleotide brushes of tunable length and location on the surface of DNA origami nanostructures, which greatly enhances their nuclease stability. Here, in this study, we report on strategies that allow for both spatial and temporal control over polymerization through activatable initiation, cleavage, and regeneration of polynucleotide brushes using restriction enzymes. The ability to site‐specifically decorate DNA origami nanostructures with polynucleotide brushes in a spatiotemporally controlled way provides access to “smart” functionalized DNA architectures with potential applications in drug delivery and supramolecular assembly.

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

Highly tunable structure-by-design polymer brush membranes for organic solvent nanofiltration

Synthetic polymeric nanofiltration membrane processes offer an alternate low-energy option to energy-intensive distillation to fractionate similar size organic solvents for chemical, petroleum, food and biotechnology industries. Here, in this study, we synthesize and test a new class of structure-by-design hydrophilic polymeric brush membranes, that address the limitations of commercial polymer membranes, are tunable and exhibit commercially relevant filtration performance. Because these brush membranes are grafted by Single Electron Transfer-Living Radical Polymerization (SET-LRP) and replace statistically random phase inversion or interfacial polymerization used for synthesizing commercial polymer membranes, their porous structure can be remodeled by varying their morphology and chemistry. We graft hydroxyethyl methacrylate (HEMA) brush structures with short and long crosslinkers, demonstrate two competing phenomena - pore stiffening and opening - and obtain high selectivity at reasonable permeability for commercially relevant methanol/toluene separation. This new class of stable, tunable, and scalable membranes offers exciting opportunities to reduce energy for separation of organic solvents.

42 ENGINEERING↗
DOE OSTI2024

Copper–Carbon Nanotube Composites Enabled by Brush Coating for Advanced Conductors

There is a growing demand for advanced conductors with enhanced electrical properties to increase the energy efficiency in various applications. A promising strategy to achieve this involves the use of ultraconductive copper (UCC) composites that incorporate highly conductive carbon materials, such as carbon nanotubes (CNTs), into the copper matrix. In this study, we present a scalable brush coating technique to incorporate CNTs onto Cu substrates to produce Cu–CNT–Cu composites. The process involves brush coating the CNT solution on Cu tape substrates, followed by vacuum-assisted thermal removal of organic moieties (e.g., surfactant/polymer). This step ensures the creation of a uniformly distributed CNT network within the Cu matrix. By addition of a thin film Cu overlayer, the fabricated Cu–CNT–Cu composite architecture demonstrates similar electrical conductivity, increased current carrying capacity, and enhanced mechanical properties compared to pure Cu reference tapes. Finally, the performance characteristics of these UCC tapes along with the scalability of the brush coating approach hold great promise for the fabrication of advanced conductors for wide-ranging energy applications.

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

Spatiotemporal Control over Polynucleotide Brush Growth on DNA Origami Nanostructures

Abstract DNA nanotechnology provides an approach to create precise, tunable, and biocompatible nanostructures for biomedical applications. However, the stability of these structures is severely compromised in biological milieu due to their fast degradation by nucleases. Recently, we showed how enzymatic polymerization could be harnessed to grow polynucleotide brushes of tunable length and location on the surface of DNA origami nanostructures, which greatly enhances their nuclease stability. Here, we report on strategies that allow for both spatial and temporal control over polymerization through activatable initiation, cleavage, and regeneration of polynucleotide brushes using restriction enzymes. The ability to site‐specifically decorate DNA origami nanostructures with polynucleotide brushes in a spatiotemporally controlled way provides access to “smart” functionalized DNA architectures with potential applications in drug delivery and supramolecular assembly.

Yang, Yunqi↗
DOE OSTI2022

Grafted polythiophene pendent polymer brushes and their electronanopatterning

Here electrochemical nanolithography using grafted polymer brushes with terthiophene (3T) pendent was investigated. The film was fabricated by surface electropolymerization of a reversible addition-fragmentation chain-transfer agent macroinitiator containing a 3T pendant molecule and the subsequent polymer brush growth from a 3T functionalized methacrylate monomer (3T-Methacrylate). Electrochemical nanolithography and patterning were done using conducting atomic force microscopy (C-AFM) enabling precise nanopattern fabrication. In contrast to direct nanowriting, dip pen nanolithography, and nanolithographic additive manufacturing, the electrochemical nanolithography can be readily facilitated by applying a bias voltage between a conductive AFM tip and the grafted polymer brush film at ambient conditions and without ink transfer. The height and electrical resistance of the nanopatterns were dependent on the writing parameters (i.e. applied bias voltage and scan rate).

36 MATERIALS SCIENCE↗
DOE OSTI2021

Self-Assembled Thermoresponsive Molecular Brushes as Nanoreactors for Asymmetric Aldol Addition in Water

The manipulation and tunability of self-assembled block copolymers through external stimuli presents an attractive strategy to develop smart polymer-based nanoreactors as supports for non-orthogonal tandem catalysis. We report on thermoresponsive core-shell micelles based on poly[norbornene-poly(2-methyl-2-oxazoline-block-2-propyl-2-oxazoline)]-graft-poly[norbornene L-proline] (P[NB-P(MeOx-b-PropOx)]-graft-P[NB-L-proline]) as catalyst supports for L-proline. These molecular brushes exhibit large differences in lower critical solution temperature behavior and nanostructure size in water depending on the chain-lengths and proline connectivity. L-Proline-mediated aldol reactions expose the efficiency by which the molecular brushes self-assemble into micelles. Molecular brushes with an extended backbone show higher activity and selectivity, suggesting better core-shell segregation of the micelles and exclusion of water from the catalytic site. Catalytic efficiencies are not improved above the cloud point temperature, the catalytic be-havior is rather sensitive to conformational changes of the polymer chains.

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

Crosslinking and Gelation of Polymer Brushes and Free Polymer Chains in a Confined Space during Controlled Radical Polymerization-A Computer Simulation Study

The confinement effect on crosslinking and gelation during controlled/living copolymerization of a monovinyl and a divinyl monomer was studied by Monte Carlo computer simulation using the dynamic lattice liquid method. The simulated reactions took place in plane-parallel slits of various widths for various grafting densities (GDs) and various initial initiator/crosslinker ratios ([X] 0 /[Ini] 0 ). Monomers and crosslinkers were initially randomly distributed in the slit, but initiators were either anchored to one solid plane (polymer brushes) or randomly distributed (free chains). For brushes, the gel point (GP) depended on GD and [X] 0 /[Ini] 0 . The higher these parameters, the lower was the gel point. The gel point was also affected by the slit width. For free, nongrafted chains, the dependence of GP on slit width was negligible. For brushes, a nonuniform density of crosslinks was found, the highest density was close to the wall. This asymmetry was high at the gel point and decreased at higher conversions.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Molecular Dynamics Study of the Effect of Grafting Density on Ion Diffusivity in a MARTINI Coarse-Grained Strong Polyelectrolyte Brush

Because surface-grafted polyelectrolyte brushes (PEBs) are responsive to external stimuli, such as electric fields and ionic strength, PEBs are attractive for applications ranging from drug delivery to separation technologies. Essential to PEB utilization is understanding how critical parameters like grafting density (σ) impact the PEB structure and the dynamics of the PEB and counterions. To study the effect of σ on PEB and the counterion structure and dynamics, we fine-tune a coarse-grained model that retains the chemical specificity of a strong polyelectrolyte, poly[(2-(methacryloyloxy)ethyl) trimethylammonium chloride] (PMETAC), using the MARTINI force field. Using “salt-free” conditions where the counterion concentration balances the charge on the brush, we build coarse-grained (CG) molecular dynamics simulations for MARTINI PMETAC brushes (N = 150 monomers; M W = 31.2 kg/mol) at experimentally relevant values of σ = 0.05, 0.10, 0.20, and 0.40 chains/nm 2 . Using 5 μs simulations, we investigate the effects of grafting density on the PEB structure, ion dissociation dynamics, polymer mobility, and counterion diffusivity. Results show that competition between electrostatic interactions, steric hindrance, and polymer mobility controls counterion diffusivity. Finally, the interplay of these factors leads to diffusivity that depends non-monotonically on σ, with counterion diffusivity peaking at an intermediate σ = 0.10 chains/nm 2 .

36 MATERIALS SCIENCE↗
DOE OSTI2026

Microscopic Dynamics Controls Coupling and Cluster Formation in Brush Particle Solids

Thermodynamics-based models predict the structure of polymer-grafted nanoparticles (PGNs) as well as their assembly behavior based on geometric parameters such as particle size, degree of polymerization, and density of grafted chains. The role of microscopic polymer dynamics, such as the mobility of repeat units in the melt state, in the evolution of the structure and properties remains unknown. Brillouin light spectroscopy (BLS), due to its capability to concurrently discern the local and global elastic properties of PGN assemblies, enables the probing of microscopic processes, such as brush interdigitation, sensitive to the annealing of the assembly. For poly(methyl methacrylate) (PMMA)-grafted silica (SiO 2 ) PGNs in the dry powder state and annealed above the glass transition temperature, BLS revealed fully reversible local elasticity, indicative of limited interdigitation between adjacent PGNs. This contrasts with polystyrene (PS)−SiO 2 analogs that displayed ready (and irreversible) fusion of brush layers during annealing. The retardation of brush interdigitation in PMMA-grafted systems is surprising, given the similar thermomechanical properties of both polymers, and is rationalized as the consequence of higher friction between PMMA repeats compared to PS. Microscopic dynamics thus has a profound impact on the kinetic path of structure (and property) evolution and thus should be considered during the processing of PGNs into functional hybrid materials.

chemical structure↗
DOE OSTI2023

Electroresponse of weak polyelectrolyte brushes

Abstract End-tethered polyelectrolytes are widely used to modify substrate properties, particularly for lubrication or wetting. External stimuli, such as pH, salt concentration, or an electric field, can induce profound structural responses in weak polyelectrolyte brushes, which can be utilized to further tune substrate properties. We study the structure and electroresponsiveness of weak polyacid brushes using an inhomogeneous theory that incorporates both electrostatic and chain connectivity correlations at the Debye–Hückel level. Our calculation shows that a weak polyacid brush swells under the application of a negative applied potential, in agreement with recent experimental observation. We rationalize this behavior using a scaling argument that accounts for the effect of the surface charge. We also show that the swelling behavior has a direct influence on the differential capacitance, which can be modulated by the solvent quality, pH, and salt concentration. Graphical Abstract

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1970

Motor brush wear measured with strain gages

Balanced bridge circuit, supplied with low-voltage direct current and connected to a readout device, measures remaining brush material, rate of brush wear, armature runout, and brush signature.

Farrell, W. T.↗
NASA NTRS1990

Flow visualization and motion analysis for a series of four sequential brush seals

Applying the Full Flow Field Tracking (FFFT) method, the flow patterns and the accompanying fluid velocities inside a series of brushes were nonintrusively determined and graphically reconstructed. The visualized flow field revealed regions that are characteristically river-jetting, vortical, and crossflow, and exist upstream, downstream, or within the seal. These flows are especially engendered by variations in fiber void that are spatial and temporal and affect changes in seal leakage and stability. The deformation of the upper half of each of the four sequential brushes as a function of upstream pressure and mass flow was determined. The axial pressure variation across the set of four brushes and the mass flow as a function of the pressure drops are also presented.

Braun, M. J.↗
NASA NTRS1991

Some preliminary results of brush seal/rotor interference effects on leakage at zero and low RPM using a tapered-plug rotor

Some preliminary brush seal leakage results for ambient temperature air are presented. Data for four nominal brush rotor radial clearances of -0.09, -0.048, -0.008, and 0.035 mm were taken by using a tapered plug rotor at 0 and 400 rpm with rotor runout of 0.127 mm peak to peak. The brush seal nominal bore diameter was 38 mm with 0.05 mm bristles at 200 bristles/mm of circumference and a 0.61 mm fence height. Leakages were greater than predicted, but agreement was reasonable. Leakage rates were not significantly altered by hysteresis or inlet flow variations. Visualization studies showed that the bristles followed the 400 rpm excitation, and loading studies indicated that bristles slid relative to one another.

Hendricks, R. C.↗
NASA NTRS1991

Some preliminary results of brush seal/rotor interference effects on leakage at zero and low rpm using a tapered-plug rotor

Some preliminary brush seal leakage results for ambient-temperature air are presented. Data for four nominal brush-rotor radial clearances of -0.09, -0.048, -0.008, and 0.035 mm were taken by using a tapered plug rotor at 0 and 400 rpm with rotor runout of 0.127 mm peak to peak. The brush seal nominal bore diameter was 38 mm with 0.05-mm bristles at 200 bristles/mm of circumference and a 0.61-mm fence height. Leakages were greater than predicted, but agreement was reasonable. Leakage rates were not significantly altered by hysteresis or inlet flow variations. Visualization studies showed that the bristles followed the 400-rpm excitation, and loading studies indicated that bristles slid relative to one another.

Hendricks, R. C.↗
NASA NTRS1991

A bulk flow model of a brush seal system

Fibers can be readily fabricated into a variety of seal configurations that are compliant and responsive to high speed or lightly loaded systems. A linear, circular, or contoured brush seal system is a contact seal consisting of the bristle pattern and hardened interface. When compared to a labyrinth seal, the brush seal system is superior and features low leakage, dynamic stability, and permits compliant structures. But in turn, the system usually requires a hardened smooth interface and permits only limited pressure drops. Wear life and wear debris for operations with static or dynamic excitation are largely undetermined. A seal system involves control of fluid within specific boundaries. The brush and rub ring (or rub surface) form a seal system. Design similitudes, a bulk flow model, and rub ring (interface) coatings are discussed. The bulk flow model calculations are based on flows in porous media and filters. The coatings work is based on experience and expanded to include current practice.

Hendricks, R. C.↗
NASA NTRS1993

High-Temperature, Flexible, Pressure-Assisted Brush Seal

Ceramic-fibers brush and integral spring clip block hot, engine flows. High-temperature, pressure-assisted brush seal installed in movable panel in advanced hypersonic engine. Seal prevents flow of hot engine gas from penetrating gap between movable panel and adjacent stationary panel. Potential applications include sealing gaps in variable-geometry two-dimensional turbojet exhaust nozzles or sealing control surface gaps of hypersonic vehicles. Ceramic brush seals also used as structural seals in high-temperature furnaces or advanced ceramic heat exchangers.

Steinetz, Bruce M.↗
NASA NTRS1992

Integrity testing of brush seal in shroud ring of T-700 engine

A split-ring brush seal was fabricated, installed between two labyrinth-honeycomb shroud seals, and tested in the fourth-stage turbine of a T-700 engine. The annealed Haynes 25 bristles rubbed directly against the nonconditioned, irregular Rene 80 turbine blade shroud surface. A total of 30 hr of cyclic and steady-state data were taken with surface speeds to 335 m/s (1100 ft/s) and shroud temperatures to 620 C (1150 F). Wear appeared to be rapid initially, with an orange flash of hot brush fragments during the first engine startup, to minimal after 10 hr of operation. The brush survived the testing but experienced some bristle pullouts and severe bristle wear; some turbine interface wear and possible material transfer was noted. Future design concerns center on tribological behavior at the interface with or without lubricants.

Hendricks, Robert C.↗
NASA NTRS1992

Flow visualization in a single simulated brush seal

A method to visualize and characterize the complex flow fields in brush seals is presented. A configuration characteristic of the brush seal confined in a two-dimensional tunnel with water as the working fluid was studied. Visualization of the flow field revealed regions that are characteristically jetting, vortical, and crossflow and exist upstream, downstream or within the seal. Such flows are engendered by variations in fiber void that are spatial and temporal and affect changes in seal leakage and stability. While the effects of interface motion and cylindrical configuration have not been considered herein, it is believed that the observed flow fields characterize flow phenomenology in brush seals.

Braun, M. J.↗