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NASA NTRS2002

Assembly of Colloidal Materials Using Bioadhesive Interactions

We have pursued the use of biological crosslinking molecules of several types to make colloidal materials at relatively low volume fraction of colloidal particles. The objective is to make binary alloys of colloidal particles, made of two different colloidal particles coated with complementary biological lock-and-key binding molecules, which assemble due to the biological specificity. The long-term goal is to use low affinity lock-and-key biological interactions, so that the can anneal to form crystalline states. We have used a variety of different surface chemistries in order to make colloidal materials. Our first system involved using selectin-carbohydrate (sialyl-Lewis) interactions; this chemistry is derived from immune system. This chemical interaction is of relatively low affinity, with timescales for dissociation of several seconds. Furthermore, the adhesion mediated by these molecules can be reversed by the chelation of calcium atoms; thus assembled structures can be disassembled reversibly. Our second system employed avidin-biotin chemistry. This well-studied system is of high affinity, and is generally irreversible on a laboratory time-scale. Thus, we would expect selectin-carbohydrate interactions at high molecular density and avidin-biotin interactions to give kinetically-trapped structures; however, at low densities, we would expect significant differences in the structure and dynamics of the two materials, owing to their very different release rates. We have also begun to use a third chemistry - DNA hybridization. By attaching single stranded DNA oligonucleotide chains to beads, we can drive the assembly of colloidal materials by hybridization of complementary DNA chains. It is well known that DNA adenosine-thymine (A-T) and guanine-cytosine (G-C) bases hybridize pairwise with a Gibbs free energy change of 1.7 kcal/mol per base; thus, the energy of the assembly can be modulated by altering the number of complementary bases in the DNA chains. Using these different crosslinking molecules, we have assembled colloidal materials from different-sized colloidal particles, A and B. In the first sets of experiment, we used high densities of adhesion molecules, and 0.96 micron (A) and 5.5 micron (B) diameter particles. The high density of adhesion molecules means that the structures are kinetically trapped in nonequilibrium configurations. The structure of the suspension can be varied by changing the number ratio of the two types of colloidal particles, NA and NB, where A is the smaller particle. With carbohydrate-selectin or avidin-biotin interactions, large NA/NB leads to the formation of colloidal micelles, with the large center B particle surrounded by many smaller A particles. As the ratio NA/NB decreases, the structures become more extended, approaching the formation of macro-Rouse polymers - extended linear chains where A beads are connected with intervening small B linkers.

Hammer, Daniel A.↗

NASA NTRS2002

Nanoscale and Microscale Iron Emulsions for Treating DNAPL

This study demonstrated the feasibility of using emulsified nanoscale and microscale iron particles to enhance dehalogenation of (Dense Non-Aqueous Phase Liquid) DNAPL free-phase. The emulsified system consisted of a surfactant-stabilized, biodegradable oil-in-water emulsion with nanoscale or microscale iron particles contained within the emulsion droplets. It was demonstrated that DNAPLs, such as trichloroethene (TCE), diffuse through the oil membrane of the emulsion particle whereupon they reach an aqueous interior and the surface of an iron particle where dehalogenation takes place. The hydrocarbon reaction by-products of the dehalogenation reaction, primarily ethene (no chlorinated products detected), diffuse out of the emulsion droplet. This study also demonstrated that an iron-emulsion system could be delivered in-situ to the DNAPL pool in a soil matrix by using a simulated push well technique. Iron emulsions degraded pure TCE at a rate comparable to the degradation of dissolved phase TCE by iron particles, while pure iron had a very low degradation rate for free-phase TCE. The iron-emulsion systems can be injected into a sand matrix where they become immobilized and are not moved by flowing water. It has been documented that surfactant micelles possess the ability to pull pooled TCE into emulsion droplets where degradation of TCE takes place.

Geiger, Cherie L.↗

NASA NTRS2003

Metal Nanoparticle Catalysts for Carbon Nanotube Growth

Work this summer involved and new and unique process for producing the metal nanoparticle catalysts needed for carbon nanotube (CNT) growth. There are many applications attributed to CNT's, and their properties have deemed them to be a hot spot in research today. Many groups have demonstrated the versatility in CNT's by exploring a wide spectrum of roles that these nanotubes are able to fill. A short list of such promising applications are: nanoscaled electronic circuitry, storage media, chemical sensors, microscope enhancement, and coating reinforcement. Different methods have been used to grow these CNT's. Some examples are laser ablation, flame synthesis, or furnace synthesis. Every single approach requires the presence of a metal catalyst (Fe, Co, and Ni are among the best) that is small enough to produce a CNT. Herein lies the uniqueness of this work. Microemulsions (containing inverse micelles) were used to generate these metal particles for subsequent CNT growth. The goal of this summer work was basically to accomplish as much preliminary work as possible. I strived to pinpoint which variable (experimental process, metal product, substrate, method of application, CVD conditions, etc.) was the determining factor in the results. The resulting SEM images were sufficient for the appropriate comparisons to be made. The future work of this project consists of the optimization of the more promising experimental procedures and further exploration onto what exactly dictated the results.

Pierce, Benjamin F.↗

NASA NTRS1998

Helicity, membrane incorporation, orientation and thermal stability of the large conductance mechanosensitive ion channel from E. coli

In this report, we present structural studies on the large conductance mechanosensitive ion channel (MscL) from E. coli in detergent micelles and lipid vesicles. Both transmission Fourier transform infrared spectroscopy and circular dichroism (CD) spectra indicate that the protein is highly helical in detergents as well as liposomes. The secondary structure of the proteins was shown to be highly resistant towards denaturation (25-95 degrees C) based on an ellipticity thermal profile. Amide H+/D+ exchange was shown to be extensive (ca. 66%), implying that two thirds of the protein are water accessible. MscL, reconstituted in oriented lipid bilayers, was shown to possess a net bilayer orientation using dichroic ratios measured by attenuated total-reflection Fourier transform infrared spectroscopy. Here, we present and discuss this initial set of structural data on this new family of ion-channel proteins.

NASA Discipline Cell Biology↗

NASA NTRS2005

Pre-biotic stage of life origin under non-photosynthetic conditions

Spontaneous assembling of a simplest bacterial cell even if all necessary molecules are present in a solution seems to be extremely rare event and from the scientific standpoint has to be considered as impossible. Therefore, a predecessor of a living cell has to be very simple for providing its self-assembling and at the same time it should be able of progressive increase in complexity. Now phase-separated particles, first of all micelles, are put forward as possible predecessors of living cell. According to the offered working concept only phase-separated particles possessing autocatalytic properties can be considered as predecessors of living cells. The first stage of evolution of these phase-separated autocatalytic systems is the appearance of pre-biotic metabolism providing synthesis of amphiphiles for formation of capsules of these systems. This synthesis is maintained by the energy of a base reaction being a component of a planet-chemical cycle. Catalytic system providing functioning of pre-biotic metabolism is based on multivariate oligomeric autocatalyst, which reproduces itself from monomers, penetrating the particles from the outside. Since the autocatalyst realizes random polymerization then a collection of other oligomers possessing different catalytic functions is produced. In the paper the functioning of multivariate oligomeric autocatalyst in flow reactor is analyzed. c2005 Published by Elsevier Ltd on behalf of COSPAR.

Biogenesis↗

NASA NTRS2007

Strain Dependence of Photoluminescense of Individual Carbon Nanotubes

We have investigated strain dependence of photoluminescense (PL) spectra of single wall carbon nanotubes (SWNT). Nanotubes were sparsely dispersed in a thin PMMA film applied to acrylic bar, and strained in both compression and extension by bending this bar in either direction in a homebuilt four-point bending rig. The average surface strain was measured with high accuracy by a resistive strain gage applied on top of the film. The near infrared imaging and spectroscopy were performed on the inverted microscope equipped with high numerical aperture reflective objective lens and InGaAs CCD cameras. PL was excited with a diode laser at either 658, 730 or 785 nm, linearly polarized in the direction of the strain. We were able to measure (n,m) types and orientation of individual nanotubes with respect to strain direction and strain dependence of their PL maxima. It was found that PL peak shifts with respect to the values measured in SDS micelles are a sum of three components. First, a small environmental shift due to difference in the dielectric constant of the surrounding media, that is constant and independent of the nanotube type. Second, shift due to isotropic compression of the film during drying. Third, shifts produced by the uniaxial loading of the film in the experiment. Second and third shifts follow expression based on the first-order expansion of the TB hamiltonian. Their magnitude is proportional to the nanotube chiral angle and strain, and direction is determined by the nanotube quantum number. PL strain dependence measured for a number of various nanotube types allows to estimate TB carbon-carbon transfer integral.

Nikolaev, Pavel N.↗

NASA NTRS1981

Functional magnetic microspheres

Functional magnetic particles are formed by dissolving a mucopolysaccharide such as chitosan in acidified aqueous solution containing a mixture of ferrous chloride and ferric chloride. As the pH of the solution is raised magnetite is formed in situ in the solution by raising the pH. The dissolved chitosan is a polyelectrolyte and forms micelles surrounding the granules at pH of 8-9. The chitosan precipitates on the granules to form microspheres containing the magnetic granules. On addition of the microspheres to waste aqueous streams containing dissolved ions, the hydroxyl and amine functionality of the chitosan forms chelates binding heavy metal cations such as lead, copper, and mercury and the chelates in turn bind anions such as nitrate, fluoride, phosphate and borate.

Yen, Shiao-Ping S.↗

NASA NTRS2003

Treatment to Destroy Chlorohydrocarbon Liquids in the Ground

A relatively simple chemical treatment that involves the use of emulsified iron has been found to be effective in remediating groundwater contaminated with trichloroethylene and other dense chlorohydrocarbon liquids. These liquids are members of the class of dense, nonaqueous phase liquids (DNAPLs), which are commonly recognized to be particularly troublesome as environmental contaminants. The treatment converts these liquids into less-harmful products. As a means of remediation of contaminated groundwater, this treatment takes less time and costs less than do traditional pump-and-treat processes. At some sites, long-term leakage and/or dissolution of chlorohydrocarbon liquids from pools and/or sorbed concentrations in rock and soil gives rise to a need to continue pumpand- treat processes for times as long as decades in order to maintain protection of human health and the environment. In contrast, the effects of the emulsified-iron treatment are more lasting, decreasing the need for long-term treatment and monitoring of contaminated areas. The material used in this treatment consists of iron particles with sizes of the order of nanometers to micrometers contained within the micelles of a surfactant-stabilized, biodegradable, oil-in-water emulsion. The emulsion is simple to prepare and consists of relatively inexpensive and environmentally acceptable ingredients: One typical formulation consists of 1.3 weight percent of a food-grade surfactant, 17.5 weight percent of iron particles, 23.2 weight percent of vegetable oil, and 58.0 weight percent of water.

Quinn, Jacqueline↗

NASA NTRS2017

Coupling Between Metabolism and Compartmentalization: Vesicle Growth in the Presence of Dipeptides

A fundamental unresolved question in studies on the origin of life is: how different, ubiquitous protocellular functions begun to work in concert setting the stage for Darwinian evolution of nascent life? From this perspective, of particular significance is coupling between growth of protocellular compartments and the encapsulated, primordial metabolism, which is one of the focal topics of the current ISSOL meeting. Specifically, growth and division of cells facilitated by the products of a metabolic reaction would confer an evolutionary advantage on protocells encapsulating this reaction, as their population would increase at the expense of other protocells. Along these lines, Adamala and Szostak have recently demonstrated that a dipeptide captured inside fatty acid vesicles catalyzes the formation of other dipeptides from activated monomers. Some of the newly synthesized dipeptides, in turn, are capable to promote competitive growth of vesicles in the presence of fatty acid micelles. As vesicles become larger, they adapt filamentous shape, which has been shown to promote their division. On the basis of computer simulations, we provide a molecularly detailed explanation of this process and draw conclusions about its generality.

Wei, C.↗

NASA NTRSDate not supplied

Optimization of Aerogels for High Temperature Applications

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 drastic densification and decrease in surface area is often exhibited after high-temperature exposure. Current research investigates yttria-stabilized zirconia (YSZ) aerogels, which have low thermal conductivity and are expected to be used between 600°C and 1000°C. We anticipate that new sol-gel chemistries and processing will yield YSZ aerogels that display retained mesoporous structure, increased surface area, and minimized shrinkage upon exposure to higher temperatures in the projected use range. This work investigates the cationic surfactant, cetrimonium bromide (CTAB), as a templating agent to prevent the collapse of the aerogel pore structure upon gelation and drying. It was determined that adding one-half times the critical micelle concentration (CMC) of CTAB increased the surface area and pore volume of the aerogels, as compared to aerogels without CTAB or with twice the CMC of CTAB, following high-temperature exposure. By optimizing CTAB, the thermal stability of YSZ aerogels can be enhanced to make these materials more efficient when used as thermal management systems.

Rebecca C Walker↗