Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “micelles”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 127 records · Page 7

Remobilizing the Interface of Thermocapillary Driven Bubbles Retarded By the Adsorption of a Surfactant Impurity on the Bubble Surface

Thermocapillary migration is a method for moving bubbles in space in the absence of buoyancy. A temperature gradient is the continuous phase in which a bubble is situated, and the applied gradient impressed on the bubble surface causes one pole of the drop to be cooler than the opposite pole. As the surface tension is a decreasing function of temperature, the cooler pole pulls at the warmer pole, creating a flow that propels the bubble in the direction of the warmer fluid. A major impediment to the practical use of thermocapillary to direct the movement of bubbles in space is the fact that surfactant impurities, which are unavoidably present in the continuous phase, can significantly reduce the migration velocity. A surfactant impurity adsorbed onto the bubble interface is swept to the trailing end of the bubble. When bulk concentrations are low (which is the case with an impurity), diffusion of surfactant to the front end is slow relative to convection, and surfactant collects at the back end of the bubble. Collection at the back lowers the surface tension relative to the front end setting up a reverse tension gradient. (This can also be the case if kinetic desorption of surfactant at the back end of the bubble is much slower than convection.) For buoyancy driven bubble motions in the absence of a thermocapillarity, the tension gradient opposes the surface flow, and reduces the surface and terminal velocities (the interface becomes more solid-like and bubbles translate as solid particles). When thermocapillary forces are present, the reverse tension gradient set up by the surfactant accumulation reduces the temperature-induced tension gradient, and can decrease to near zero the bubble's thermocapillary velocity. The objective of our research is to develop a method for enhancing the thermocapillary migration of bubbles which have be retarded by the adsorption onto the bubble surface of a surfactant impurity. Our remobilization theory proposes to use surfactant molecules which kinetically rapidly exchange between the bulk and the surface and are at high bulk concentrations. Because the remobilizing surfactant is present at much higher concentrations than the impurity, it adsorbs to the bubble surface much faster than the impurity when the bubble is formed, and thereby prevents the impurity from adsorbing onto the surface. In addition, the rapid kinetic exchange and high bulk concentration maintain a saturated surface with uniform surface concentrations. This prevents retarding surface tension gradients and keeps the thermocapillary velocity high. In our reports over the first 2 years, we presented numerical simulations of the bubble motion and surfactant transport which verified theoretically the concept of remobilization, and the development of an apparatus to track and measure the velocity of rising bubbles in a glycerol/water surfactant solution. This year, we detail experimental observations of remobilization. Two polyethylene oxide surfactants were studied, C12E6 (CH3(CH2)11(OCH2)6OH) and C10E8 (CH3(CH2)4(OCH2CH2)8OH). Measurements of the kinetic exchange for these surfactants show that the one with the longer hydrophobe chain C12E6 has a lower rate of kinetic exchange. In addition, this surfactant is much less soluble in the glycerol/water mixture because of the shorter ethoxylate chain. As a result, we found that C12E6 had only a very limited ability to remobilize rising bubbles because of the limited kinetic exchange and reduced solubility. However, C10E8, with its higher solubility and more rapid exchange was found to dramatically remobilize rising bubbles. We also compared our theoretical calculations to the experimental measurements of velocity for both the non-remobilizing and remobilizing surfactants and found excellent agreement. We further observed that for C10E8 at high concentrations, which exceeded the critical micelle concentrations, additional remobilization was measured. In this case the rapid exchange of monomer between micelle and surfactant provides an additional mechanism for maintaining a uniform surface concentrations.

Palaparthi, Ravi↗

[Results of Simulation Studies]

Lattice Monte Carlo and off-lattice molecular dynamics simulations of h(sub 1)t(sub 4) and h(sub 4)t(sub l) (head/tail) amphiphile solutions have been performed as a function of surfactant concentration and temperature. The lattice and off-lattice systems exhibit quite different self-assembly behavior at equivalent thermodynamic conditions. We found that in the weakly aggregating regime (no preferred-size micelles), all models yield similar micelle size distributions at the same average aggregation number, albeit at different thermodynamic conditions (temperatures). In the strongly aggregating regime, this mapping between models (through temperature adjustment) fails, and the models exhibit qualitatively different micellization behavior. Incipient micellization in a model self-associating telechelic polymer solution results in a network with a transient elastic response that decays by a two-step relaxation: the first is due to a heterogeneous jump-diffusion process involving entrapment of end-groups within well-defined clusters and this is followed by rapid diffusion to neighboring clusters and a decay (terminal relaxation) due to cluster disintegration. The viscoelastic response of the solution manifests characteristics of a glass transition and entangled polymer network.

Source record↗

Optimizing Surfactant Templating of Yttria-Stabilized Zirconia Aerogels for High-Temperature Applications: Effect of Cationic Surfactant

Aerogels can be used in spaceflight applications as thermal insulators due to their low density, low thermal conductivity, and tortuous path for solid conduction. However, the aerogel formulation must be optimized to increase the thermal stability of the aerogels, as a drastic densification and decrease in surface area often is exhibited after high-temperature exposure. This work considers yttria-stabilized zirconia (YSZ) aerogels, whichhave low thermal conductivity and are expected to be used for temperatures between 600°C and 1000°C. It is anticipated that new sol-gel chemistries will yield YSZ aerogels that exhibit retained mesoporous structure, increased surface area, and minimized shrinkage upon exposure to higher temperatures in the expected use range. This work investigates the addition of surfactant to 20 mol% YSZ aerogels. The cationic surfactant, cetrimonium bromide (CTAB), was used as the templating agent, preventing the collapse of the mesoporous structure upon gelation and drying. It was determined that adding one-half times the critical micelle concentration of CTAB increased the surface area of the aerogels by 72% and 41% and increased the pore volume following exposure to 600°C and1000°C, respectively. This level of CTAB had the greatest increase in surface area and pore volume as compared to aerogels without CTAB or with twice the critical micelle concentration of CTAB. By optimizing the concentration of CTAB, the thermal stability ofYSZ aerogels can be enhanced to make these materials more efficient when used as thermal management systems.

Yttria-stabilized zirconia aerogel↗

Method of forming inorganic nanocages

Nanocages are formed by etching nancubes. The nanocubes are added to an aqueous system having an amphiphilic lipid dissolved in an organic solvent (e.g. a hydrophobic alcohol) to form reverse micelles. As the water evaporates the micelles shrink as etching of the flat surface of the nanocubes occurs. In this fashion hollow nanocages are produced. In one embodiment, the nanocage is covalently attached to a polymer shell (e.g. a dextran shell).

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Method of forming inorganic nanocages

Nanocages are formed by etching nanocubes. The nanocubes are added to an aqueous system having an amphiphilic lipid dissolved in an organic solvent (e.g. a hydrophobic alcohol) to form reverse micelles. As the water evaporates the micelles shrink as etching of the flat surface of the nanocubes occurs. In this fashion hollow nanocages are produced. In one embodiment, the nanocage is covalently attached to a polymer shell (e.g. a dextran shell).

Matsui, Hiroshi↗

Breast tumor-targeted drug delivery via polymer nanocarriers: Endogenous and exogenous strategies

Breast cancer, one of the most common types of cancer worldwide, has a high degree of malignancy while lacking efficient treatments. The off-target events frequently occurring in drug administration have been a major obstacle, which causes severe side effects to patients and reduces the therapeutic efficacy. An ideal medication should precisely target the specific site with precise control over concentration and duration. In recent years, there has been immense progress in polymer nanocarriers that demonstrate great potential in the targeted delivery. These nanocarriers are constructed from materials sensitive to a wide range of endogenous (e.g., pH, enzyme, redox) and exogenous stimuli (e.g., light, ultrasound, magnetic waves), driving cargo release to the targeted tissue or cells. Here, we elucidate the mechanism of current targeting strategies and the engineering methods to construct these targeting systems or to improve their targeting efficiency. Here we capture the recent progress in the targeted nanocarriers derived from polymers which span hydrogels and micelles, demonstrating their design and applications in chemo, hyperthermia, immuno, and gene therapies.

36 MATERIALS SCIENCE↗

Nanostructural and rheological transitions of pH-responsive supramolecular systems involving a zwitterionic amphiphile and a triamine

Supramolecular aqueous complexes of a synthesized zwitterionic surfactant, 2-(dimethyl(octadecyl)ammonio)acetate (stearyl betaine) and diethylenetriamine, have been found to display pH-tunable rheological properties without the need for a co-surfactant. For this supramolecular system, the dynamically changing interplay among the constituents is responsible for the rich phase behavior including hollow nanotubules, bilayers, and vesicles. A further hypothesis is that hollow nanotubular structure is highly desirable for achieving chain entanglement geometries with reduced mesh size. The rheological properties of the suspension were measured using a rotational rheometer. An analysis using zero-shear viscosities at various temperatures as well as differential scanning calorimetry(DSC) helped shed light on thermodynamic and phase transitions taking place. The morphology of the suspension was analyzed by using a combination of small angle x-ray scattering(SAXS) and atomic force microscopy(AFM). Large steady-shear viscosities (up to ~160 Pa.s) and viscoelastic behavior was observed in acidic conditions which diminished upon increasing the pH. A novel analysis consisting of measured thermodynamic quantities such as activation energy(E a ) and enthalpy of transition(ΔH T ) further allude to the rich pH-sensitive nanoarchitecture of the system. Rather than commonly observed wormlike micelles, hollow nanotubules, as long as 1.6 µm were observed at pH 4 which disintegrated to bilayer sheets and vesicles upon increasing pH. Finally, gaining a comprehensive understanding from all the results, a transition mechanism between different suspension architectures was proposed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Phase diagrams and microstructures of aqueous short alkyl chain polyethylene glycol ether carboxylate and carboxylic acid triblock surfactant solutions

The surfactant C 8 Eo 8 CH 2 COOH (Akypo LF2) and its salts have a small hydrophobic and a significantly longer hydrophilic part. As a consequence, there must be a significant steric constraint, once these surfactant molecules form micelles. In addition, the partially charged headgroups should bring some additional fine-tuning via electrostatic interactions to this "essentially non-ionic" surfactant. Experiments: Phase diagrams of binary mixtures of water and C 8 Eo 8 CH 2 COOH are established over large concentration and temperature ranges, also at different pHs and in the presence of sodium and calcium ions. Surface tensions and osmotic pressures are measured to understand the systems. To evaluate the microstructures, also Dynamic Light Scattering and Small-Angle X-ray Scattering are performed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Key Intermediate Nanostructures in the Self-Assembly of Amphiphilic Polypeptoids Revealed by Cryo-TEM

Amphiphilic copolypeptoids are known to form a variety of nanostructures (fibers, tubes, sheets, etc.), but the assembly mechanisms and key intermediates remain underexplored. This study investigates the intermediate structures formed during the early stages of self-assembly in diblock copolypeptoids using cryo-transmission electron microscopy (cryo-TEM). Here we focused on two diblock copolypeptoids, one with a free N-terminus and the other with a capped N-terminus, which ultimately form less-ordered nanofibers and well-ordered nanosheets, respectively. Through cryo-TEM imaging of vitrified solutions at various time points during the self-assembly process, the study identified micelles and vesicles as key intermediate structures. Notably, the formation of vesicles as intermediates is unusual in crystallization-driven self-assembly and suggests a unique pathway in polypeptoid self-assembly. The study provides direct imaging evidence of key intermediates in polypeptoid self-assembly, advancing the understanding of their self-assembly mechanisms.

59 BASIC BIOLOGICAL SCIENCES↗

Mechanisms of Metal Additive-Induced Ordering During SNIPS Membrane Formation

Isoporous membranes can be fabricated by combining self-assembly with nonsolvent induced phase separation (SNIPS) using an amphiphilic block copolymer like polystyrene-b-poly(4-vinylpyridine) (SV). Poly(4-vinylpyridine) (V) is known to complex with metal salts, which are hypothesized to stabilize solution ordering and preserve structure during casting. We explored how the molar ratio of metal additive to the poly(4-vinylpyridine) block affected the final membrane morphology via scanning electron microscopy (SEM). Dynamic light scattering (DLS), small-angle X-ray scattering (SAXS), and in situ grazing-incidence SAXS were used to track changes in solution ordering and chain conformation as a function of the molar ratio of the additive to the V block. Additives induced aggregation, promoted the formation of more compact conformations in solution, and facilitated micelle ordering onto lattices at optimal ratios. Furthermore, these experimental results were supported by random phase approximation calculations, which helped explain how the thermodynamic order–disorder transition shifts with additive binding strength. Stronger additive–polymer interactions reduced the block copolymer volume fraction required for ordering in solution, allowing ordered domains to form at lower polymer concentrations.

Additives↗

Conductive Thin Films over Large Areas by Supramolecular Self-Assembly

We report a “one-step” method for preparing conductive thin films with cylindrical microdomains oriented normal to the surface over large areas using the supramolecular assembly of poly(styrene-block-4-vinylpyridine) (PS19-b-P4VP 5 ) and 5,10,15,20-tetrakis(4-hydroxyphenyl)-21H,23H-porphine (HOTPP). HOTPP interacts with the P4VP block by hydrogen bonding between the hydroxyl group of HOTPP and pyridine ring of PS 19 -b-P4VP 5 , forming cylindrical P4VP(HOTPP) domains having an average diameter of ~17 nm in a PS matrix. Here, dynamic light scattering, contact angle, and in situ grazing incidence small-angle X-ray scattering measurements show a morphological transition from spherical micelles in solution to cylindrical microdomains oriented normal to the substrate surface during the drying process. From the dependence of current on voltage, an average current of ~4.0 nA is found to pass through a single microdomain, pointing to a promising route for organic semiconductor device applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

How Does the Rate of Chain Exchange Relate to Stress Relaxation in Triblock Copolymer Networks?

The relationship between macroscopic stress relaxation and molecular-level chain exchange in triblock copolymer micelles has been explored using rheology and time-resolved small-angle neutron scattering (TR-SANS), marking the first measurements of chain exchange in concentrated triblock networks. It has long been assumed in models of transient or thermoreversible networks that the time scales for these two processes are equal. Experimentally, we find that stress relaxation occurs many orders-of-magnitude faster than chain exchange. This difference is quantitatively explained by modest dispersity in the core block that results in a slight asymmetry within any given nominally symmetric triblock. For stress relaxation to occur, only the shorter chain must pull out, while chain exchange is slowed due to the requirement of the eventual pullout of the longer block. The pullout time is extremely sensitive to the length of the core block. This mechanism is supported by measurements with an intentionally asymmetric triblock copolymer, which displays an even larger difference between the stress relaxation and chain exchange rates. These results establish a quantitative molecular-level picture of the chain dynamics associated with stress relaxation in triblock copolymer networks.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Harnessing Peptide Binding to Capture and Reclaim Phosphate

With rising consumer demands, society is tapping into wastewater as an innovative source to recycle depleting resources. Novel reclamation technologies have been recently explored for this purpose, including several that optimize natural biological processes for targeted reclamation. However, this emerging field has a noticeable dearth of synthetic material technologies that are programmed to capture, release, and recycle specified targets; and of the novel materials that do exist, synthetic platforms incorporating biologically inspired mechanisms are rare. We present here a prototype of a materials platform utilizing peptide amphiphiles that has been molecularly engineered to sequester, release, and reclaim phosphate through a stimuli-responsive pH trigger, exploiting a protein-inspired binding mechanism that is incorporated directly into the self-assembled material network. This material is able to harvest and controllably release phosphate for multiple cycles of reuse, and it is selective over nitrate and nitrite. We have determined by simulations that the binding conformation of the peptide becomes constrained in the dense micelle corona at high pH such that phosphate is expelled when it otherwise would be preferentially bound. However, at neutral pH, this dense structure conversely employs multichain binding to further stabilize phosphate when it would otherwise be unbound, opening opportunities for higher-order conformational binding design to be engineered into this controllably packed corona. With this work, we are pioneering a new platform to be readily altered to capture other valuable targets, presenting a new class of capture and release materials for recycling resources on the nanoscale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DNA-caged nanoparticles via electrostatic self-assembly

DNA-modified nanoparticles enable DNA sensing and therapeutics in nanomedicine and are also crucial for nanoparticle self-assembly with DNA-based materials. However, methods to conjugate DNA to nanoparticle surfaces are limited, inefficient, and lack control. Inspired by DNA tile nanotechnology, we demonstrate a new approach to nanoparticle modification based on electrostatic attraction between negatively charged DNA tiles and positively charged nanoparticles. This approach does not disrupt nanoparticle surfaces and leverages the programmability of DNA nanotechnology to control DNA presentation. We demonstrated this approach using a variety of nanoparticles, including polymeric micelles, polystyrene beads, gold nanoparticles, and superparamagnetic iron oxide nanoparticles with sizes ranging from 5–20 nm in diameter. DNA cage formation was confirmed through transmission electron microscopy (TEM), neutralization of zeta potential, and a series of fluorescence experiments. DNA cages present “handle” sequences that can be used for reversible target attachment or self-assembly. Handle functionality was verified in solution, at the solid–liquid interface, and inside fixed cells, corresponding to applications in biosensing, DNA microarrays, and erasable immunocytochemistry. Finally, these experiments demonstrate the versatility of the electrostatic DNA caging approach and provide a new pathway to nanoparticle modification with DNA that will empower further applications of these materials in medicine and materials science.

60 APPLIED LIFE SCIENCES↗

Investigating microstructure evolution in block copolymer membranes

Block copolymer self-assembly in conjunction with nonsolvent-induced phase separation (SNIPS) has been increasingly leveraged to fabricate integral-asymmetric membranes. The large number of formulation and processing parameters associated with SNIPS, however, has prevented the reliable construction of high performance membranes. In this study, we apply dynamical self-consistent field theory to model the SNIPS process and investigate the effect of various parameters on the membrane morphology: solvent selectivity, nonsolvent selectivity, initial film composition, and glass transition composition. We examine how solvent selectivity and concentration of polymers in the film impact the structure of micelles that connect to form the membrane matrix. In particular, we find that preserving the order in the surface layer and forming a connection between the supporting and surface layer are nontrivial and sensitive to each parameter studied. Furthermore, the effect of each parameter is discussed, and suggestions are made for successfully fabricating viable block copolymer membranes.

36 MATERIALS SCIENCE↗

Synthesis and characterization of N-parinaroyl analogs of ganglioside GM3 and de-N-acetyl GM3. Interactions with the EGF receptor kinase

A specific plasma membrane glycosphingolipid, known as ganglioside GM3, can regulate the intrinsic tyrosyl kinase activity of the epidermal growth factor (EGF) receptor; this modulation is not associated with alterations in hormone binding to the receptor. GM3 inhibits EGF receptor tyrosyl kinase activity in detergent micelles, in plasma membrane vesicles, and in whole cells. In addition, immunoaffinity-purified EGF receptor preparations contain ganglioside GM3 (Hanai et al. (1988) J. Biol. Chem. 263, 10915-10921), implying that the glycosphingolipid is intimately associated with the receptor kinase in cell membranes. Both the nature of this association and the molecular mechanism of kinase inhibition remain to be elucidated. In this report, we describe the synthesis of a fluorescent analog of ganglioside GM3, in which the native fatty acid was replaced with trans-parinaric acid. This glycosphingolipid inhibited the receptor kinase activity in a manner similar to that of the native ganglioside. A modified fluorescent glycosphingolipid, N-trans-parinaroyl de-N-acetyl ganglioside GM3, was also prepared. This analog, like the nonfluorescent de-N-acetyl ganglioside GM3, had no effect on receptor kinase activity. Results from tryptophan fluorescence quenching and steady-state anisotropy measurements in membranes containing these fluorescent probes and the human EGF receptor were consistent with the notion that GM3, but not de-N-acetyl GM3, interacts specifically with the receptor in intact membranes.

NASA Discipline Cell Biology↗

Thermoplastic Elastomers and Their Physical Gels Electrospun into Tunable Microfibrous Nonwoven Mats: Structure Formation and Property Enhancement

Abstract Thermoplastic elastomers (TPEs) based on styrenic block copolymers constitute excellent examples of self‐networking macromolecules that are employed in a wide range of contemporary technologies as molded parts. In such applications, these TPEs exist as dense (nonporous) films or other shapes. Here, it is first demonstrated that a series of commercial TPEs possessing comparable compositions can be electrospun from solution to form microfibers that are arranged into nonwoven mats that are breathable. An important consideration for microfiber formation is the copolymer molecular weight, which regulates i) the viscosity of the parent solution prior to electrospinning, ii) the ability of these copolymers to self‐assemble during electrospinning, iii) the microfiber morphology, and iv) the mechanical properties of the resultant microfibers. The addition of a midblock‐selective aliphatic oil to these TPEs yields thermoplastic elastomer gels (TPEGs), wherein the copolymer morphology and mechanical properties become highly composition‐tunable. Electrospinning TPEGs from a binary oil+solvent solution introduces a micelle inversion mechanism that begins with an oil‐rich micellar core and ends with a styrene‐rich micellar core, required for network stabilization, as the solvent dries during microfiber solidification. This work has implications for the production of controllably low‐modulus microfibrous materials possessing modestly improved toughness but exceptional extensibility and enhanced optical transparency.

Shamsi, Mohammad↗

Two‐Dimensional Superstructures of Silica Cages

Abstract Despite extensive studies on mesoporous silica since the early 1990s, the synthesis of two‐dimensional (2D) silica nanostructures remains challenging. Here, mesoporous silica is synthesized at an interface between two immiscible solvents under conditions leading to the formation of 2D superstructures of silica cages, the thinnest mesoporous silica films synthesized to date. Orientational correlations between cage units increase with increasing layer number controlled via pH, while swelling with oil and mixed surfactants increase micelle size dispersity, leading to complex clathrate type structures in multilayer superstructures. The results suggest that a three‐dimensional (3D) crystallographic registry within cage‐like superstructures emerges as a result of the concerted 3D co‐assembly of the organic and inorganic components. Mesoporous 2D superstructures can be fabricated over macroscopic film dimensions and stacked on top of each other. The realization of previously inaccessible mesoporous silica heterostructures with separation or catalytic properties unachievable via conventional bulk syntheses is envisioned.

Aubert, Tangi↗