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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 775 records · Page 43
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Quantitative 3D evolution of colloidal nanoparticle oxidation in solution

Watching nanomaterials transform in time Real-time analysis of chemical transformations of nanoparticles is usually done with electron microscopy of a few particles. One limitation is interference by the electron beam. Sun et al. monitored the oxidation of iron nanoparticles in solution by using small- and wide-angle x-ray scattering and molecular dynamics simulations (see the Perspective by Cadavid and Cabot). These methods revealed the formation of voids within the nanoparticles, diffusion of material into and out of the nanoparticles, and ultimately the coalescence of the voids. Science , this issue p. 303 ; see also p. 245

36 MATERIALS SCIENCE↗
NASA NTRS2005

Characterization of colloid thruster beams

In this article we use retarding potential, time of flight, and a Faraday cup, to measure the energy and specific charge distributions of the electrospray particles as a function of the position within the beam, as well as beam profiles. This information is then used, together with a model of the beam, to calculate its spreading.

electric propulsion↗
DOE OSTI2022

Tuning Stoichiometry to Promote Formation of Binary Colloidal Superlattices

The self-assembly of binary nanoparticle superlattices from colloidal mixtures is a promising method for the fabrication of complex colloidal cocrystal structures. However, binary mixtures often form amorphous or metastable phases instead of the thermodynamically stable phase. Here we show that in binary mixtures of differently sized spherical particles, an excess of the smaller component can promote—and, in some cases, may be necessary for—the self-assembly of a binary cocrystal. Using computer simulations, we identify two mechanisms responsible for this phenomenon. First, excess small particles act like plasticizers and enable systems to reach a greater supersaturation before kinetic arrest occurs. Second, they can disfavor competing structures that may interfere with the growth of the target structure. We find the phase behavior of simulated mixtures of nearly hard spheres closely matches published experimental results. We demonstrate the generality of our findings for mixtures of particles of arbitrary shape by presenting a binary mixture of hard shapes that only self-assembles with an excess of the smaller component.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Aqueous aggregation behavior of citric acid coated magnetite nanoparticles: Effects of pH, cations, anions, and humic acid

Highlights: • Citric acid (CA) coatings greatly enhanced the stability of MNPs at pH = 5–9. • Stability of CA-MNPs increased with pH increase due to CA deprotonation. • The valence and adsorption of ions affected the surface charge of CA-MNPs. • The aggregation behaviors of CA-MNPs agreed with DLVO predictions. Improving the colloidal stability of magnetite nanoparticles (MNPs) is essential for their successful applications. In this study, the surface zeta potential and particle size evolutions of citric acid coated magnetite nanoparticles (CA-MNPs) were measured under varied aqueous conditions using dynamic light scattering (DLS). The effects of pH (5.0–9.0), ionic strength (IS), cations (Na{sup +} and Ca{sup 2+}), anions (phosphate, sulfate, and chloride) and humic acid on the aggregation behaviors of CA-MNPs were explored. Compared with bare MNPs, the stability of CA-MNPs were greatly improved over the typical pH range of natural aquatic environments (pH = 5.0–9.0), as the coated CA-MNPs were highly negatively charged over the pH range due to the low pK{sub a1} value (3.13) of citrate acid. CA-MNPs were more stable in the presence of monovalent cation (Na{sup +}) compared with divalent cation (Ca{sup 2+}), as Ca{sup 2+} could neutralize the surface charge of MNPs more significantly than Na{sup +}. In the presence of anions, the surface charges of CA-MNPs became more negative, and the stability of CA-MNPs followed the order: in phosphate > sulfate > chloride. The observed aggregation trend could be explained by the differences in the valences of the anions and their adsorption behaviors onto CA-MNPs, which altered the surface charges of CA-MNPs. The measured critical coagulation concentrations (CCC) values of CA-MNPs in these electrolyte solutions agreed well with Derjaguin–Landau–Verwey–Overbeek (DLVO) calculations. With the addition of Humic acid (HA), the aggregation of CA-MNPs was inhibited in all electrolyte solutions even with the critical coagulation concentrations. This is due to the adsorption of HA onto CA-MNPs, which enhanced the electrostatic and steric repulsive forces between CA-MNPs. Considering the good stability of CA-MNPs in solutions with varied pH and electrolyte compositions, as well as with the easy synthesis of CA-MNPs and their non-toxicity, this study suggested CA coating as a good strategy to increase the stability of MNPs.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Confusion-Driven Machine Learning of Structural Phases of a Flexible, Magnetic Stockmayer Polymer

We use a semisupervised, neural-network-based machine learning technique, the confusion method, to investigate structural transitions in magnetic polymers, which we model as chains of magnetic colloidal nanoparticles characterized by dipole–dipole and Lennard-Jones interactions. As input for the neural network, we use the particle positions and magnetic dipole moments of equilibrium polymer configurations, which we generate via replica-exchange Wang–Landau simulations. We demonstrate that by measuring the classification accuracy of neural networks, we can effectively identify transition points between multiple structural phases without any prior knowledge of their existence or location. We corroborate our findings by investigating relevant conventional order parameters. Our study furthermore examines previously unexplored low-temperature regions of the phase diagram, where we find new structural transitions between highly ordered helicoidal polymer configurations.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Rheological Properties of Aqueous Colloidal Silica Suspensions Related to Amendment Delivery for Subsurface Remediation

Colloidal silica (fumed silica) suspensions are being tested as carriers for remedial amendment delivery in subsurface remediation and as media for underground contamination containment. The knowledge of the rheological behavior of the silica suspensions is lack in the literature while it is essential for the preparation and field injection of the suspensions. This contribution is focused on the rheological characteristics of colloidal silica suspensions under various environmental conditions relevant to amendment delivery for subsurface remediation. We investigated the influence of silica particle concentration, water source, ionic strength, pH, aging, amendment type and concentration, and subsurface sediment on the rheological behavior of the suspensions. All tested suspension formulations exhibited shear thinning before gelation. Higher silica particle concentration and salinity (Na+ and K+) increased suspensions’ viscosity and the degree of shear thinning. The viscosity of suspensions increased with aging. The suspensions at natural pH exhibited the highest viscosity compared to the acidic and alkaline suspensions with the same silica concentration. Addition of KMnO4 amendment to aqueous silica suspensions increased viscosity, while addition of alcohol amendment decreased suspensions’ viscosity. The presence of amendment did not reduce shear thinning. The gelation rate of silica suspensions was increased with silica concentration and with the addition of sediments. The rheological characteristics of shear thinning aqueous fumed silica suspensions were compared to that of shear thinning solutions formed with organic polymer xanthan gum, which was applied for amendment delivery in subsurface remediation.

Yang, Shuo↗
DOE OSTI2014

Colloid Rates of Radionuclides in Cooling Water of the 120-GeV Proton Accelerator Facilities at Fermilab - Paper 58

Cooling water systems for high-energy accelerators are typically equipped with a deionizer to keep water pure for accelerator materials and to remove radionuclides for radioactivity control. Although the deionizers are expected to collect the entire radionuclides, more radioactivity than expected remains in the cooling water in typical cooling water operations at J-PARC and the Tsukuba Campus of High Energy Accelerator Research Organization (KEK), Japan. For example, specific activity of {sup 7}Be in the cooling water for magnetic horns at the J-PARC Neutrino Experimental Facility was observed to be comparable to the limit of {sup 7}Be activity for drain (30 Bq/mL) after enough deionization duration. Removing this activity from the cooling water is an important problem that must be solved before the water can be released into the environment. In our previous study, it was found that some radionuclides had weak retention on ion-exchange resins in the cooling water deionizer system for the K2K target and magnetic horns at the 12-GeV proton accelerator in KEK, Japan. Incomplete adsorption in the deionizer was attributed to colloid formation. Therefore, understanding the colloid formation of radionuclides in cooling water is important for understanding the activity remaining in the cooling water. Colloid formation in water under high-intensity radiation fields has been investigated by previous irradiation experiments. Under 120-GeV proton irradiation of Cu foils in water, it was found that the colloid formation rates of Mg, Mn, Co, Ni, and Cu isotopes and those of {sup 7}Be, {sup 24}Na, {sup 42}K, and {sup 43}K were approximately 30% and 1.8-3.9%, respectively. Sc, Cr, and Fe isotopes were missing from the water. In the photon irradiation of water in a Cu tube using Bremsstrahlung from an electron linear accelerator and a {sup 60}Co γ-ray source at Kyoto University Research Reactor Institute, we observed Cu colloid formation in consequence of the corrosion of Cu. It is possible that radionuclides attach to the colloids formed by the corrosion of accelerator materials and pass through the deionizer. To enhance the understanding of the behavior of radionuclides in cooling water in a high-energy accelerator environment, we investigated the colloid formation of radionuclides in cooling waters at the 120-GeV proton accelerator facilities at Fermilab, USA. We have already reported the previous results of specific activities of γemitting radionuclides and {sup 3}H in water samples collected from eight cooling water systems. Following the previous study, this paper is concerned with the measurement of colloid formation rates of radionuclides in cooling waters. (authors)

43 PARTICLE ACCELERATORS↗
DOE OSTI2021

Multimodal imaging of oil-in-water bilgewater emulsion and biofilms

Bilgewater emulsions, consisting of oil and surfactant mixtures in water, affect many aquatic species. Thus development of methods and techniques to treat or mitigate the formation and undesired consequences of shipboard emulsions are urgently needed. This work presents new results of the evolution of the bilgewaer chemical and physical properties using in situ imaging. A Navy O/W emulsion consisting of three oils and a detergent mixture was used as the synthetic bilgewater model [1, 2]. Synthetic oil-in-water (O/W) emulsion droplets were seled in a vacuum compatible microfluidic sample holder and imaged using a suite of tools including scanning electron microscopy (SEM), time-of-flight secondary ion mass spectrometry (ToF-SIMS), confocal laser scanning microscopy, and optical microscopy, highlighting the advantage of multiscale analysis and its applications in waste reduction and treatment in the environment. The transferrable and vacuum compatible microfluidic interface, System for Analysis at the Liquid Vacuum Interface (SALVI), was used in this study. SALVI enabled surface analysis of liquids and liquid-solid interactions using ToF-SIMS and SEM [3, 4]. Its detection window is an aperture of 2 ?m in diameter open to vacuum, permitting direct detection of the liquid surface. Liquid is withheld by surface tension within the aperture. The interface is composed of a silicon nitride membrane and polydimethylsiloxane microchannel [3, 4]. A variety of samples including complex liquid mixtures, ionic liquids, single mammalian cells, live biofilms, and solid-electrolyte interface have been analyzed using in situ imaging [5, 6]. The feasibility of using SALVI for in situ SEM imaging of nanoparticles and colloids in liquid was recently demonstrated [7]. This paper shows new findings of multimodal imaging and analysis of synthesized emulsion particles in water. Figure 1 depicts a schematic of multimodal in situ imaging of bilgewater emulsion using SEM and ToF-SIMS. Furthermore, we study the interactions of microbes and bilgewater emulsion. Microbes play an important role in the ocean. We hypothesize that microbes release organics that can act as surfactants that affect bilgewater formation or weakening. We present the first systematic study of emulsions and biofilms and investigate the effects of biofilms on bilgewater emulsions. Pseudomonas was selected as a model strain. Biofilms were cultured in a microchannel to allow culture [8]. Once a thick layer of biofilms was formed, the medium solution was changed to a mixture consisting of 50 % bilgewater emulsion. Dispersed biofilms were collected at 24 hrs. and 48 hrs. after emulsions were introduced into the channel. Bilgewater emulsions, biofilms, and mixtures of bilgewater emulsions and biofilms were analyzed using multiple in situ and ex situ techniques as described earlier. Our findings indicate that biofilms change the chemical makeup of the emulsion surface compositions and emulsion droplet size distribution, confirming the hypothesis that extracellular polymeric substance (EPS) related components released from biofilms can function as surfactants and change the oil-in-water interfaces.

bilgewater, multimodal imaging, biofilms↗
DOE OSTI2017

Dynamic Scaling of Colloidal Gel Formation at Intermediate Concentrations

Here, we have examined the formation and dissolution of gels composed of intermediate volume-fraction nanoparticles with temperature-dependent short-range attractions using small-angle x-ray scatter- ing (SAXS), x-ray photon correlation spectroscopy (XPCS), and rheology to obtain nanoscale and macroscale sensitivity to structure and dynamics. Gel formation after temperature quenches to the vicinity of the rheologically-determined gel temperature, T gel , was characterized via the slow-down of dynamics and changes in microstructure observed in the intensity autocorrelation functions and structure factor, respectively, as a function of quench depth (ΔT = T quench - T gel ), wave vector, and formation time (t f ). We find similar patterns in the slow-down of dynamics that maps the wave-vector-dependent dynamics at a particular ΔT and t f to that at other ΔTs and t f s via an effective scaling temperature, Ts. A single Ts applies to a broad range of ΔT and tf but does depend on the particle size. The rate of formation implied by the scaling is a far stronger function of ΔT than that of the attraction strength between colloids. Finally, we interpret this strong temperature de- pendence in terms of changes in cooperative bonding required to form stable, energetically favored, local structures.

42 ENGINEERING↗
DOE OSTI2014

Even hard-sphere colloidal suspensions display Fickian yet non-Gaussian diffusion

In this study, we scrutinize three decades of probability density displacement distribution in a simple colloidal suspension with hard-sphere interactions. In this index-matched and density-matched solvent, fluorescent tracer nanoparticles diffuse among matrix particles that are eight times larger, at concentrations from dilute to concentrated, over times up to when the tracer diffuses a few times its size. Displacement distributions of tracers, Gaussian in pure solvent, broaden systematically with increasing obstacle density. The onset of non-Gaussian dynamics is seen in even modestly dilute suspensions, which traditionally would be assumed to follow classic Gaussian expectation. The findings underscore, in agreement with recent studies of more esoteric soft matter systems, the prevalence of non-Gaussian yet Fickian diffusion.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Enhancing nanoscale charged colloid crystallization near a metastable liquid binodal

Achieving predictive control over crystallization using non-classical nucleation while avoiding kinetic traps would be a step towards designing materials with new functionalities. We address these challenges by inducing the bottom-up assembly of nanocrystals into ordered arrays, or superlattices. Using electrostatics—rather than density—to tune the interactions between particles, we watch self-assembly proceed through a metastable liquid phase. Here, we systematically investigate the phase behaviour as a function of quench conditions in situ and in real time using small-angle X-ray scattering. By fitting to colloid, liquid and superlattice models, we extract the time evolution of each phase and the system phase diagram, which we find to be consistent with short-range attractive interactions. Using the predictive power of the phase diagram, we establish control of the self-assembly rate over three orders of magnitude, and we identify one- and two-step self-assembly regimes, with only the latter implicating the metastable liquid as an intermediate. The presence of the metastable liquid increases the superlattice formation rate relative to the equivalent one-step pathway, and the superlattice order increases with the rate, revealing a generalizable kinetic strategy for promoting and enhancing ordered assembly.

Tanner, Christian P. N. [University of California,↗
DOE OSTI2019

Ion exchange selectivity in clay is controlled by nanoscale chemical–mechanical coupling

Ion exchange in nanoporous clay-rich media plays an integral role in water, nutrient, and contaminant storage and transport. In montmorillonite (MMT), a common clay mineral in soils, sediments, and muds, the swelling and collapse of clay particles through the addition or removal of discrete molecular layers of water alters cation exchange selectivities in a poorly understood way. Here, we show that ion exchange is coupled to the dynamic delamination and restacking of clay layers, which creates a feedback between the hydration state of the exchanging cation and the composition of the clay interlayer. Particles with different hydration states are distinct phases with unique binding selectivities. Surprisingly, equilibrium achieved through thermal fluctuations in cation concentration and hydration state leads to the exchange of both ions and individual MMT layers between particles, a process we image directly with high-resolution transmission electron microscopy at cryogenic conditions (cryo-TEM). We introduce an exchange model that accounts for the binding selectivities of different phases, which is likely applicable to many charged colloidal or macromolecular systems in which the structural conformation is correlated with the activities of water and counterions within spatially confined compartments.

Whittaker, Michael L.↗
DOE OSTI2020

Characterization of Iron and Organic Carbon Colloids in Boreal Rivers and Their Fate at High Salinity

Riverine colloids are important carriers of macronutrients, trace metals, and pollutants into marine waters. The aim of the current study was to extend the understanding of iron (Fe) and organic carbon (OC) colloids in boreal rivers and their fate at higher salinities. X-ray absorbance spectroscopy (XAS) and dynamic light scattering (DLS) were combined to explore Fe speciation and colloidal characteristics such as size and surface charge and how these are affected at increasing salinity. XAS confirmed the presence of two Fe phases in the river waters—Fe-organic matter (OM) complexes and Fe(oxy)hydroxides. From DLS measurements on filtered and unfiltered samples, three particle size distributions were identified. The smallest particles (10–40 nm) were positively charged and suggested to consist of essentially bare Fe (oxy)hydroxide nanoparticles. The largest particles (300–900 nm) were dominated by Fe(oxy)hydroxides associated with chromophoric molecular matter. An intermediate size distribution (100–200 nm) with a negative surface charge was presumably dominated by OM and containing Fe-OM complexes. Increasing the salinity resulted in a removal of the smallest distribution. Unexpectedly, both the intermediate and largest size distributions were still detected at high salinity. The collective results suggest that Fe(oxy) hydroxides and Fe-OM complexes are both found across the wide size range studied and that colloidal size does not necessarily reflect either Fe speciation or stability toward salinity-induced aggregation. The findings further demonstrate that also particles beyond the typically studied <0.45-μm size range should be considered to fully understand the riverine transport and fate of macronutrients, trace metals, and pollutants.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Diffusive ferromagnetic roller gas

An ensemble of actively rotating ferromagnetic particles is used to realize an active roller gas. Here, we investigate the diffusive properties of such a gas in experiments and simulations. We reveal that ferromagnetic rollers demonstrate a normal (Fickian) diffusion with a characteristic linear growth of the mean-squared displacement, while statistics of displacements stay non-Gaussian. At short times the system has a bimodal distribution of the displacements that transitions with time to a quasi-Gaussian distribution (Gaussian core with overpopulated tails) for a range of studied particle number densities. Inert particles introduced into the active roller gas exhibit similar diffusive behavior. Here, the results provide insights into diffusive properties of active colloidal systems with activity originating from spinning degrees of freedom.

36 MATERIALS SCIENCE↗
DOE OSTI2016

A Brownian dynamics study on ferrofluid colloidal dispersions using an iterative constraint method to satisfy Maxwell’s equations

Ferrofluids are often favored for their ability to be remotely positioned via external magnetic fields. The behavior of particles in ferromagnetic clusters under uniformly applied magnetic fields has been computationally simulated using the Brownian dynamics, Stokesian dynamics, and Monte Carlo methods. However, few methods have been established that effectively handle the basic principles of magnetic materials, namely, Maxwell’s equations. An iterative constraint method was developed to satisfy Maxwell’s equations when a uniform magnetic field is imposed on ferrofluids in a heterogeneous Brownian dynamics simulation that examines the impact of ferromagnetic clusters in a mesoscale particle collection. This was accomplished by allowing a particulate system in a simple shear flow to advance by a time step under a uniformly applied magnetic field, then adjusting the ferroparticles via an iterative constraint method applied over sub-volume length scales until Maxwell’s equations were satisfied. The resultant ferrofluid model with constraints demonstrates that the magnetoviscosity contribution is not as substantial when compared to homogeneous simulations that assume the material’s magnetism is a direct response to the external magnetic field. This was detected across varying intensities of particle-particle interaction, Brownian motion, and shear flow. Ferroparticle aggregation was still extensively present but less so than typically observed.

42 ENGINEERING↗
DOE OSTI2016

Depinning and nonequilibrium dynamic phases of particle assemblies driven over random and ordered substrates: A review

Here, we review the depinning and nonequilibrium phases of collectively interacting particle systems driven over random or periodic substrates. This type of system is relevant to vortices in type-II superconductors, sliding charge density waves, electron crystals, colloids, stripe and pattern forming systems, and skyrmions, and could also have connections to jamming, glassy behaviors, and active matter. These systems are also ideal for exploring the broader issues of characterizing transient and steady state nonequilibrium flow phases as well as nonequilibrium phase transitions between distinct dynamical phases, analogous to phase transitions between different equilibrium states. We discuss the differences between elastic and plastic depinning on random substrates and the different types of nonequilibrium phases which are associated with specific features in the velocity-force curves, fluctuation spectra, scaling relations, and local or global particle ordering. We describe how these quantities can change depending on the dimension, anisotropy, disorder strength, and the presence of hysteresis. Within the moving phase we discuss how there can be a transition from a liquid-like state to dynamically ordered moving crystal, smectic, or nematic states. Systems with periodic or quasiperiodic substrates can have multiple nonequilibrium second or first order transitions in the moving state between chaotic and coherent phases, and can exhibit hysteresis. We also discuss systems with competing repulsive and attractive interactions, which undergo dynamical transitions into stripes and other complex morphologies when driven over random substrates. Throughout this work we highlight open issues and future directions such as absorbing phase transitions, nonequilibrium work relations, inertia, the role of non-dissipative dynamics such as Magnus effects, and how these results could be extended to the broader issues of plasticity in crystals, amorphous solids, and jamming phenomena.

36 MATERIALS SCIENCE↗