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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 901 records · Page 50
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Structural disordering of de-alloyed Pt bimetallic nanocatalysts: the effect on oxygen reduction reaction activity and stability

Platinum bimetallic alloys are well-known for their ability to catalyze the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). In this work, Pt x Co 1-x colloidal nanoparticles were synthesized with varying initial Pt : Co ratios, but constant size to investigate how the initial metal composition affects their electrocatalytic performance. The results show that upon contact with acid environment the Co leaches out of the particles leading to almost identical compositions, independent of the initial differences. Surprisingly the data show a clear trend in ORR activity, although the Pt x Co 1-x nanoparticles almost completely de-alloy during acid leaching, i.e. under reaction conditions in a fuel cell. To scrutinize the resulting particle structure after de-alloying we used pair distribution function (PDF) analysis and X-ray diffraction (XRD) gaining insight into the structural disorder and its dependence on the initial metal composition. Our results suggest that not only the ORR activity, but also the corrosion resistance of the synthesized NPs, are dependent on the structural disorder resulting from the de-alloying process.

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

Spectral features of colloidal solutions of elongated gold nanoparticles produced by laser ablation in aqueous solutions

The extinction spectra of colloidal solutions of gold nanoparticles produced by laser ablation in water and aqueous solutions of salts using two near-IR lasers with pulse durations of 200 ns and 1 ps are experimentally investigated. The extinction spectrum of the particles formed by ablation in aqueous solutions is characterised by enhanced optical density in the red and IR regions. This feature is due to the formation of elongated gold nanoparticles, as confirmed by transmission electron microscopy. The surface images of a gold target subjected to multipulse laser ablation exhibit micron and submicron structures. (nanophotonics)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS1994

Electrokinetic transport of heterogeneous particles in suspension

The Smoluchowski equation for electrophoresis predicts that the electrophoretic velocity of a particle is proportional to its zeta potential but not its size, shape, or orientation. Furthermore, the equation predicts that the rotation rate is identically zero. The Smoluchowski equation fails for heterogeneous particles (i.e., those with nonuniform zeta potentials). Recent theories and experiments show that particles with a dipole moment of zeta potential rotate into alignment with an externally applied electric field. For doublets (particles composed of two spheres) the rotation rate depends on (1) whether the spheres are rigidly rocked or freely rotating, and (2) the gap distance between the spheres. The relative configuration of two coagulated spheres is determined by the colloidal forces of the system. The goal of our research is to use measurements of electrophoretic rotation to determine the gap between two spheres of a colloidal doublet and also to determine whether or not the doublet is rigid.

Velegol, D.↗
DOE OSTI2014

How does a thermal binary crystal break under shear?

When exposed to strong shearing, the particles in a crystal will rearrange and ultimately, the crystal will break by forming large nonaffine defects. Even for the initial stage of this process, only little effort has been devoted to the understanding of the breaking process on the scale of the individual particle size for thermalized mixed crystals. Here, we explore the shear-induced breaking for an equimolar two-dimensional binary model crystal with a high interaction asymmetry between the two different species such that the initial crystal has an intersecting square sublattice of the two constituents. Using Brownian dynamics computer simulations, we show that the combination of shear and thermal fluctuations leads to a characteristic hierarchical breaking scenario where initially, the more strongly coupled particles are thermally distorted, paving the way for the weakly coupled particles to escape from their cage. This in turn leads to mobile defects which may finally merge, proliferating a cascade of defects, which triggers the final breakage of the crystal. This scenario is in marked contrast to the breakage of one-component crystals close to melting. Moreover, we explore the orientational dependence of the initial shear direction relative to the crystal orientation and compare this to the usual melting scenario without shear. Our results are verifiable in real-space experiments of superparamagnetic colloidal mixtures at a pending air-water interface in an external magnetic field where the shear can be induced by an external laser field.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1996

Dynamics of Disorder-Order Transitions in Hard Sphere Colloidal Dispersions in micro-g

We performed a series of experiments on 0.518 millimeter PMMA spheres suspended in an index matching mixture of decalin and tetralin the microgravity environment provided by the Shuttle Columbia on mission STS-73. The samples ranged in concentration from 0.49 to 0.62. volume fraction (phi) of spheres, which covers the range in which liquid, coexistence, solid and glass phases are expected from Earth bound experiments. Light scattering was used to probe the static structure, and the particle dynamics. Digital and 35 mm photos provided information on the morphology of the crystals. In general, the crystallites grew considerably larger (roughly an order of magnitude larger) than the same samples with identical treatment in 1 g. The dynamic light scattering shows the typical short time diffusion and long time caging effects found in 1 g. The surprises that were encountered in microgravity include the preponderance of random hexagonal close packed (RHCP) structures and the complete absence of the expected face centered cubic (FCC) structure, existence of large dendritic crystals floating in the coexistence samples (where liquid and solid phases coexist) and the rapid crystallization of samples which exist only in glass phase under the influence of one g. These results suggest that colloidal crystal growth is profoundly effected by gravity in yet unrecognized ways. We suspect that the RCHP structure is related to the nonequilibrium growth that is evident from the presence of dendrites. An analysis of the dendritic growth instabilities is presented within the framework of the Ackerson-Schatzel equation.

Zhu, J. X.↗
DOE OSTI2015

Multiple dynamic regimes in colloid-polymer dispersions: New insight using X-ray photon correlation spectroscopy

We present an X-ray photon correlation spectros- copy (XPCS) study of dynamic transitions in an anisotropic colloid-polymer dispersion with multiple arrested states. The results provide insight into the mechanism for formation of repulsive glasses, attractive glasses, and networked gels of col- loids with weakly adsorbing polymer chains. In the presence of adsorbing polymer chains, we observe three distinct regimes: a state with slow dynamics consisting of finite particles and clusters, for which interparticle interactions are predominantly repulsive; a second dynamic regime occurring above the satu- ration concentration of added polymer, in which small clusters of nanoparticles form via a short-range depletion attraction; and a third regime above the overlap concentration in which dynamics of clusters are independent of polymer chain length. The observed complex dynamic state diagram is primarily gov- erned by the structural reorganization of a nanoparticle cluster and polymer chains at the nanoparticle-polymer surface and in the concentrated medium, which in turn controls the dynamics of the dispersion

36 MATERIALS SCIENCE↗
DOE OSTI2013

Light-emitting nanocomposite particles

A method of making an inorganic light emitting layer includes combining a solvent for semiconductor nanoparticle growth, a solution of core/shell quantum dots, and semiconductor nanoparticle precursor(s); growing semiconductor nanoparticles to form a crude solution of core/shell quantum dots, semiconductor nanoparticles, and semiconductor nanoparticles that are connected to the core/shell quantum dots; forming a single colloidal dispersion of core/shell quantum dots, semiconductor nanoparticles, and semiconductor nanoparticles that are connected to the core/shell quantum dots; depositing the colloidal dispersion to form a film; and annealing the film to form the inorganic light emitting layer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Multivalent Electrochemistry of Spinel Mg x Mn 3– x O 4 Nanocrystals

Oxides undergoing reversible electrochemical cycling of Mg 2+ ions would enable novel battery concepts beyond Li + , capable of storing large amounts of energy. However, materials showing this chemical reactivity are scarce. Suitable candidates require small particles to shorten transport lengths, together with chemically complex structures that promote cation mobility, such as spinel. These goals pose a challenge for materials chemists. Here, nanocrystals of spinel-type Mg 0.5 Mn 2.5 O 4 were prepared using colloidal synthesis, and their electrochemical activity is presented. Cycling in an aqueous Mg 2+ electrolyte led to a reversible transformation between a reduced spinel and an oxidized layered framework. This reaction involves large amounts of capacity because of the full oxidation to Mn 4+ , through the extraction of both Mg 2+ and, in the first cycle, Mn 2+ ions. Re-formation of the spinel upon reduction resulted in enrichment with Mg 2+ , indicating that its insertion is more favorable than that of Mn 2+ . Incorporation of water into the structure was not indispensable for the transformation, as revealed by experiments in non-aqueous electrolytes and infrared spectroscopy. Lastly, the findings open the door for the use of similar nanocrystals in Mg batteries provided that electrolytes with suitable anodic stability are discovered, thereby identifying novel routes toward electrode materials for batteries with high energy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Aluminosilicate colloidal gels: from the early age to the precipitation of zeolites

Aluminosilicate hydrogels are often considered to be precursors for the crystallisation of zeolites carried out under hydrothermal conditions. The preparation of mechanically homogeneous aluminosilicate gels enables the study of these materials through bulk rheology and observation of the aging dynamics until the precipitation of crystalline zeolites. The first part of this study deals with the establishment of ternary state diagrams, in order to identify the range of chemical formulations that enable preparation of single-phase homogeneous gels. Then, by studying the viscoelastic moduli during the gelation reaction, and by yielding the gel under large deformation, we propose an empirical law considering the partial order of reaction on each chemical element, to predict the gelation time according to the chemical formulation. The scaling behavior of the elastic properties of this colloidal gel shows a transition from a strong link behavior to a weak link regime. Long term aging results in the shrinkage of the gel, accompanied by syneresis of interstitial liquid at the surface. Zeolites precipitate through crystallisation by a particle attachment mechanism, when thermodynamic equilibrium is reached. The stoichiometry of the precipitated zeolites is not only consistent with the concentration of the remaining species in the supernatant but, surprisingly, it is also very close to the partial order of the reaction of the chemical elements involved in the determination of the critical gel point. This indicates a strong correlation between the morphology of the soft amorphous gel network that is formed at an early age and those of the final solid precipitated crystals.

36 MATERIALS SCIENCE↗
DOE OSTI2020

A collective elastic fluctuation mechanism for decoupling and stretched relaxation in glassy colloidal and molecular liquids

We propose a microscopic theory for the decoupling of self-diffusion and structural relaxation in glass-forming liquids within the Elastically Collective Nonlinear Langevin Equation (ECNLE) activated dynamics framework. Our central hypothesis is that the heterogeneity relevant to this problem is static fluctuations of local density on the scale of 3–4 particle diameters and how this changes local packing correlations. These fluctuations modify the degree of dynamical cage expansion that mechanistically couples intracage large amplitude hopping and longer range collective elasticity in ECNLE theory. Decoupling only emerges in the deeply supercooled regime where the strongly temperature dependent elastic barrier becomes non-negligible relative to its noncooperative local analog. The theory makes predictions for various aspects of the decoupling phenomenon, including apparent fractional power law Stokes-Einstein behavior, that appear to be consistent with experiments and simulations on hard sphere fluids and molecular liquids. Of central importance is a microscopic connection between the barrier fluctuation variance and most probable barrier height. Sensible results are also obtained for the nonexponential stretching of a generic relaxation time correlation function and its temperature evolution. Nonuniversality can arise from the relative importance of the local and collective barriers (related to fragility) and the precise magnitude of the length scale that defines the transition from local cage to elastic physics. Comparison is made with a traplike model based on a Gaussian distribution of barriers.

Xie, Shi-Jie (ORCID:0000000333174720)↗
DOE OSTI2022

Aerosol-Assisted Deposition for TiO 2 Immobilization on Photocatalytic Fibrous Filters for VOC Degradation

Atomization and spraying are well-established methods for the production of submicrometer- and micrometer- sized powders. In addition, they could be of interest to the immobilization of photocatalytic nanoparticles onto supports because they enable the formation of microporous films with photocatalytic activity. Here, we provide a comparison of aerosol-assisted immobilization methods, such as spray-drying (SD), spray atomization (SA), and spray gun (SG), which were used for the deposition of TiO 2 dispersions onto fibrous filter media. The morphology, microstructure, and electronic properties of the structures with deposited TiO 2 were characterized by SEM and TEM, BET and USAXS, and UV-Vis spectrometry, respectively. The photocatalytic performances of the functionalized filters were evaluated and compared to the benchmark dip-coating method. Our results showed that the SG and SA immobilization methods led to the best photocatalytic and operational performance for the degradation of toluene, whereas the SD method showed the lowest degradation efficiency and poor stability of coating. We demonstrated that TiO2 sprays using the SG and SA methods with direct deposition onto filter media involving dispersed colloidal droplets revealed to be promising alternatives to the dip-coating method owing to the ability to uniformly cover the filter fibers. In addition, the SA method allowed for fast and simple control of the coating thickness as the dispersed particles were continuously directed onto the filter media without the need for repetitive coatings, which is common for the SG and dip-coating methods. Our study highlighted the importance of the proper immobilization method for the efficient photocatalytic degradation of VOCs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1979

Formation of metallic and metal hydrous oxide dispersions

The formation, via hydrothermally induced precipitation from homogeneous solution, of a variety of well-defined dispersions of metallic and hydrous metal in the conditions under which the particles are produced (e.g., pH and composition of the growth medium, aging temperature, rate of heating, or degree of agitation) can be readily discerned by following changes in the mass, composition, and morphology of the final solid phase. The generation of colloidal dispersions in the absence of gravity convection or sedimentation effects may result in the appearance of morphological modifications not previously observed in terrestrially formed hydrosols.

Matijevic, E.↗
DOE OSTI2015

PVA and PEG functionalised LSMO nanoparticles for magnetic fluid hyperthermia application

La{sub 0.7}Sr{sub 0.3}MnO{sub 3} magnetic nanoparticles are synthesized by a solution combustion method and functionalised with polyvinyl alcohol and polyethylene glycol. The induction heating characteristics of coated magnetic nanoparticles (42 °C) were observed at a reasonably low concentration (5 mg/mL). Remarkably, coated magnetic nanoparticles exhibited a promisingly high specific absorption rate with varying magnetic field and constant frequency. The surface analysis is carried out by X-ray photoelectron spectroscopy. A reduction in the agglomeration of the particles was observed when the magnetic nanoparticles were functionalised with polyvinyl alcohol or polyethylene glycol and can be confirmed by transmission electron microscopy and dynamic light scattering studies. Vibrating sample magnetometer measurements indicate superparamagnetic behaviour at room temperature before and after coating. Colloidal stability revealed a considerably higher zeta potential value for coated system. In vitro cytotoxicity test of the magnetic nanoparticles indicates that coated nanoparticles have no significant effect on cell viability within the tested concentrations (1–5 mg mL{sup -1}) as compared to uncoated La{sub 0.7}Sr{sub 0.3}MnO{sub 3}. All these findings explore the potentiality of La{sub 0.7}Sr{sub 0.3}MnO{sub 3} nanoparticles for magnetic fluid hyperthermia. - Highlights: • Surface functionalization of LSMO nanoparticles — first time with PVA • Surface functionalization of LSMO nanoparticles — first time with PEG • BSA protein — first time used as dispersion medium for stability of LSMO nanoparticles • The heating ability observed at low concentration • Improved efficiency of magnetic fluid hyperthermia treatment with surfactants.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Coherent Phonon Dynamics in Plasmonic Gold Tetrahedral Nanoparticle Ensembles

Coherent phonon modes supported by plasmonic nanoparticles offer prospective applications in chemical and biological sensing. Whereas characterization of these phonon modes often requires single particle measurements, synthetic routes to narrow size distributions of nanoparticles permit ensemble investigations. Recently, the synthesis of highly monodisperse gold tetrahedral nanoparticles with tunable edge length and corner sharpness has been developed. Herein, we characterize a size series of these nanoparticles in colloidal dispersion via transient absorption spectroscopy to examine their mechanical and plasmonic responses upon photoexcitation. Oscillations of transient absorption signals are observed in the plasmon resonance and correspond to the lowest order radial breathing modes of the nanoparticles, the frequencies of which are affected by edge length and truncation of the corners. Furthermore, quality factor values ranging from 10 to 15 are observed for the oscillations that convey potential utility in mass-sensing and plasmon-exciton coupling photonics schemes. Finite-difference time domain and finite element analysis calculations establish the specific optically-relevant phonon modes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Colloidal Stability of PFSA-Ionomer Dispersions Part II: Determination of Suspension pH Using Single-Ion Potential Energies

Perfluorosulfonic acid (PFSA) ionomers serve a vital role in the performance and stability of fuel-cell catalyst layers. These properties, in turn, depend on the colloidal processing of precursor inks. Here, to understand the colloidal structure of fuel-cell catalyst layers, we explore the aggregation of PFSA ionomers dissolved in water/alcohol solutions and relate the predicted aggregation to experimental measurements of solution pH. Not all side chains contribute to measured pH because of burying inside particle aggregates. To account for the measured degree of dissociation, a new description is developed for how PFSA aggregates interact with each other. The developed single-counterion electrostatic repulsive pair potential from Part I is incorporated into the Smoluchowski collision-based kinetics of interacting aggregates with buried side chains. We demonstrate that the surrounding solvent mixture affects the degree of aggregation as well as the pH of the system primarily through the solution dielectric permittivity, which drives the strength of the interparticle repulsive energies. Successful pH prediction of Nafion ionomer dispersions in water/n-propanol solutions validates the numerical calculations. Nafion-dispersion pH measurements serve as a surrogate for Nafion particle-size distributions. The model and framework can be leveraged to explore different ink formulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Connectivity and free-surface effects in polymer glasses

The glass transition is one of the few unsolved problems in condensed matter physics: agreement on the cause of the slowing down of structural relaxation in glass-forming liquids is lacking. Glasses are amorphous solids, which do not possess the long-range crystalline order, yet display arrested dynamics and the shear elastic modulus characteristic of equilibrium elasticity. It has been suggested that due to the influence of intramolecular interactions and chain connectivity, the nature of the glass transition in polymers and in standard glass-formers is fundamentally different. Here, we discuss the role of connectivity in polymer glasses, demonstrating that although covalent bonding promotes glass formation, bonding sequentiality that defines a polymer chain is not critical in the bulk: glassy dynamics is purely a result of the number of connections per particle, independently of how these connections are formed, agreeing with the classical Phillips-Thorpe topological constraint theory. We show that bonding sequentiality does play an important role in the surface effects of the glass, highlighting a major difference between polymeric and colloidal glasses. Further, we identify the heterogenous dynamics of model coarse-grained polymer chains both in ‘bulk’ and near the free surface, and demonstrate characteristic domain patterns in local displacement and connectivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Freezing lines of colloidal Yukawa spheres. II. Local structure and characteristic lengths

Using the Rogers-Young (RY) integral equation scheme for the static pair correlation functions combined with the liquid-phase Hansen-Verlet freezing rule, we study the generic behavior of the radial distribution function and static structure factor of monodisperse charge-stabilized suspensions with Yukawa-type repulsive particle interactions at freezing. In a related article, labeled Paper I [J. Gapinski, G. Nägele, and A. Patkowski, J. Chem. Phys. 136, 024507 (2012)], this hybrid method was used to determine two-parameter freezing lines for experimentally controllable parameters, characteristic of suspensions of charged silica spheres in dimethylformamide. A universal scaling of the RY radial distribution function maximum is shown to apply to the liquid-bcc and liquid-fcc segments of the universal freezing line. A thorough analysis is made of the behavior of characteristic distances and wavenumbers, next-neighbor particle coordination numbers, osmotic compressibility factor, and the Ravaché-Mountain-Streett minimum-maximum radial distribution function ratio.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Analysis of the static magnetic field-dependent optical transmission of Ni nanorod colloidal suspensions

The magnetic field-dependent optical transmission of dilute Ni nanorod aqueous suspensions was investigated. A series of four samples of nanorods were synthesized using the AAO template method and processed to stable colloids. The distributions of their length and diameter were characterized by analysis of TEM images and revealed average diameters of ∼25 nm and different lengths in the range of 60 nm–1100 nm. The collinear magnetic and optical anisotropy was studied by static field-dependent transmission measurements of linearly polarized light parallel and perpendicular to the magnetic field direction. The experimental results were modelled assuming the field-dependent orientation distribution function of a superparamagnetic ensemble for the uniaxial ferromagnetic nanorods in liquid dispersion and extinction cross sections for longitudinal and transversal optical polarization derived from different approaches, including the electrostatic approximation and the separation of variables method, both applied to spheroidal particles, as well as finite element method simulations of spheroids and capped cylindrical particles. The extinction cross sections were compared to reveal the differences associated with the approximations of homogeneous polarization and/or particle shape. The consequences of these approximations for the quantitative analysis of magnetic field-dependent optical transmission measurements were investigated and a reliable protocol derived. Furthermore, the changes in optical cross sections induced by electromagnetic interaction between two nanorods in parallel end-to-end and side-by-side configuration as a function of their separation were studied.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗