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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Elucidating the mechanisms of enhanced lignin bioconversion by an alkali sterilization strategy

Biological lignin valorization represents an emerging green approach to upgrade lignin for sustainable and economic biorefineries. However, lignin generally exhibits poor water solubility and inhomogeneous distribution in an aqueous medium, significantly limiting its bioconversion efficiency. Herein, we develop a novel alkali sterilization strategy to effectively enhance the dispersion and fermentation performance of lignin substrates. The colloidal particle size and molecular structure variations of lignin during the sterilization were thoroughly investigated to reveal the mechanisms of enhanced fermentation performance. Results showed that alkali sterilization achieved a completely aseptic effect when mixing lignin medium at an initial pH of 12.7 for 24 h. Dynamic light scattering (DLS) analysis demonstrated that the hydrodynamic volume of colloidal lignin particles decreased by 96.3% by alkali sterilization compared with the conventional thermal sterilization. Moreover, lignin characterizations by nuclear magnetic resonance (NMR) spectroscopy and gel permeation chromatography (GPC) suggested that alkali sterilization modified the lignin molecular structure by generating 50% more hydrophilic carboxyl groups, reducing the weight-average molecular weight (M w ) by 23.0%, and narrowing the molar-mass dispersity (D M ) by 23.8%. The generation of lignin substrates with more uniform distribution and lower molecular weight improved Rhodococcus opacus PD630 cell growth and metabolism. Microbial cell amount, lignin degradation, and lipid production in alkali sterilized medium increased by 309%, 30.3%, and 48.3%, respectively, compared to those in thermally sterilized medium. These results clearly demonstrated that alkali sterilization dramatically improved the lignin bioconversion performance. Furthermore, this work presents a facile and effective sterilization strategy to overcome inhomogeneous lignin distribution in aqueous fermentation media, showing great potentials as a platform technique for promoting biological lignin valorization.

59 BASIC BIOLOGICAL SCIENCES↗
NASA NTRS1999

Chain Dynamics in Magnetorheological Suspensions

Magnetorheological (MR) suspensions are composed of colloidal particles which acquire dipole moments when subjected to an external magnetic field. At sufficient field strengths and concentrations, the dipolar particles rapidly aggregate to form long chains. Subsequent lateral cross-linking of the dipolar chains is responsible for a rapid liquid-to-solid-like rheological transition. The unique, magnetically-activated rheological properties of MR suspensions make them ideal for interfacing mechanical systems to electronic controls. Additionally, the ability to experimentally probe colloidal suspensions interacting through tunable anisotropic potentials is of fundamental interest. Our current experimental work has focused on understanding the fluctuations of dipolar chains. It has been proposed by Halsey and Toor (HT) that the strong Landau-Peierls thermal fluctuations of dipolar chains could be responsible for long-range attractions between chains. Such interactions will govern the long-time relaxation of MR suspensions. We have synthesized monodisperse neutrally buoyant MR suspensions by density matching stabilized ferrofluid emulsion droplets with D2O. This allows us to probe the dynamics of the dipolar chains using light scattering without gravitational, interfacial, and polydispersity effects to resolve the short-wavelength dynamics of the dipolar chains. We used diffusing wave spectroscopy to measure these dynamics. The particle displacements at short times that show an independence to the field strength, but at long times exhibit a constrained, sub-diffusive motion that slows as the dipole strength is increased. The experiments are in good qualitative agreement with Brownian dynamics simulations of dipolar chains. Although there have been several important and detailed studies of the structure and interactions in MR suspensions, there has not been conclusive evidence that supports or contradicts the HT model prediction that long-range interactions exist between fluctuating chains of dipolar particles. Resolving this issue would contribute greatly to the understanding of these interesting and important materials. We have begun to test the predictions of the HT model by both examining the dynamics of individual chains and by measuring the forces between dipolar chains directly to accurately and quantitatively assess the interactions that they experience. To do so, we employ optical trapping techniques and video-microscopy to manipulate and observe our samples on the microscopic level. With these techniques, it is possible to observe chains that are fluctuating freely in three-dimensions, independent of interfacial effects. More importantly, we are able to controllably observe the interactions of two chains at various separations to measure the force-distance profile. The techniques also allow us to study the mechanical properties of individual chains and chain clusters. Our work to this point has focused on reversibly-formed dipolar chains due to field induced dipoles where the combination of this chaining, the dipolar forces, and the hydrodynamic interactions that dictate the rheology of the suspensions. One can envision, however, many situations where optical, electronic, or rheological behavior may be optimized with magneto-responsive anisotropic particles. Chains of polarizable particles may have the best properties as they can coil and flex in the absence of a field and stiffen and orient when a field is applied. We have recently demonstrated a synthesis of stable, permanent paramagnetic chains by both covalently and physically linking paramagnetic colloidal particles. The method employed allows us to create monodisperse chains of controlled length. We observed the stability, field-alignment, and rigidity of this new class of materials. The chains may exhibit unique rheological properties in an applied magnetic field over isotropic suspensions of paramagnetic particles. They are also useful rheological models as bead-spring systems. These chains form the basis for our current experiments with optical traps.

Gast, A. P.↗
DOE OSTI2024

Emergent biaxiality in chiral hybrid liquid crystals

Biaxial nematic liquid crystals are fascinating systems sometimes referred to as the Higgs boson of soft matter because of experimental observation challenges. Here we describe unexpected states of matter that feature biaxial orientational order of colloidal supercritical fluids and gases formed by sparse rodlike particles. Colloidal rods with perpendicular surface boundary conditions exhibit a strong biaxial symmetry breaking when doped into conventional chiral nematic fluids. Minimization of free energy prompts these particles to orient perpendicular to the local molecular director and the helical axis, thereby imparting biaxiality on the hybrid molecular-colloidal system. The ensuing phase diagram features colloidal gas and liquid and supercritical colloidal fluid states with long-range biaxial orientational symmetry, as supported by analytical and numerical modeling at all hierarchical levels of ordering. Unlike for nonchiral hybrid systems, dispersions in chiral nematic hosts display biaxial orientational order at vanishing colloid volume fractions, promising both technological and fundamental research utility.

Colloids↗
DOE OSTI2024

Colloidal Stability of PFSA-Ionomer Dispersions. Part I. Single-Ion Electrostatic Interaction Potential Energies

Charged colloidal particles neutralized by a single counterion are increasingly important for many emerging technologies. Attention here is paid specifically to hydrogen fuel cells and water electrolyzers whose catalyst layers are manufactured from a perfluorinated sulfonic acid polymer (PFSA) suspended in aqueous/alcohol solutions. Partially dissolved PFSA aggregates, known collectively as ionomers, are stabilized by the electrostatic repulsion of overlapping diffuse double layers consisting of only protons dissociated from the suspended polymer. We denote such double layers containing no added electrolyte as "single ion". Size-distribution predictions build upon interparticle interaction potential energies from the Derjaguin-Landau-Verwey-Overbeek (DLVO) formalism. However, when only a single counterion is present in solution, classical DLVO electrostatic potential energies no longer apply. Accordingly, here a new formulation is proposed to describe how single-counterion diffuse double layers interact in colloidal suspensions. Part II (Srivastav, H.; Weber, A. Z.; Radke, C. J. Langmuir 2024 DOI: 10.1021/acs.langmuir.3c03904) of this contribution uses the new single-ion interaction energies to predict aggregated size distributions and the resulting solution pH of PFSA in mixtures of n-propanol and water. A single-counterion diffuse layer cannot reach an electrically neutral concentration far from a charged particle. Consequently, nowhere in the dispersion is the solvent neutral, and the diffuse layer emanating from one particle always experiences the presence of other particles (or walls). Thus, in addition to an intervening interparticle repulsive force, a backside osmotic force is always present. With this new construction, we establish that single-ion repulsive pair interaction energies are much larger than those of classical DLVO electrostatic potentials. The proposed single-ion electrostatic pair potential governs dramatic new dispersion behavior, including dispersions that are stable at a low volume fraction but unstable at a high volume fraction and finite volume-fraction dispersions that are unstable with fine particles but stable with coarse particles. Finally, the proposed single-counterion electrostatic pair potential provides a general expression for predicting colloidal behavior for any charged particle dispersion in ionizing solvents with no added electrolyte.

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

Tunable assembly of hybrid colloids induced by regioselective depletion

Assembling colloidal particles using site-selective directional interactions into predetermined colloidal superlattices with desired properties is broadly sought-after, but challenging to achieve. Here in this paper, we exploit regioselective depletion interactions to engineer the directional bonding and assembly of non-spherical colloidal hybrid microparticles. We report that the crystallization of a binary colloidal mixture can be regulated by tuning the depletion conditions. Subsequently, we fabricate triblock biphasic colloids with controlled aspect ratios to achieve regioselective bonding. Without any surface treatment, these biphasic colloids assemble into various colloidal superstructures and superlattices featuring optimized pole-to-pole or center-to-center interactions. Additionally, we observe polymorphic crystallization, quantify the abundancy of each form using algorithms we developed, and investigate the crystallization process in real time. We demonstrate selective control of attractive interactions between specific regions on an anisotropic colloid with no need of site-specific surface functionalization, leading to a general method for achieving colloidal structures with yet unforeseen arrangements and properties.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Skyrmion dynamics and topological sorting on periodic obstacle arrays

Abstract We examine skyrmions under a dc drive interacting with a square array of obstacles for varied obstacle size and damping. When the drive is applied in a fixed direction, we find that the skyrmions are initially guided in the drive direction but also move transverse to the drive due to the Magnus force. The skyrmion Hall angle, which indicates the difference between the skyrmion direction of motion and the drive direction, increases with drive in a series of quantized steps as a result of the locking of the skyrmion motion to specific symmetry directions of the obstacle array. On these steps, the skyrmions collide with an integer number of obstacles to create a periodic motion. The transitions between the different locking steps are associated with jumps or dips in the velocity–force curves. In some regimes, the skyrmion Hall angle is actually higher than the intrinsic skyrmion Hall angle that would appear in the absence of obstacles. In the limit of zero damping, the skyrmion Hall angle is 90°, and we find that it decreases as the damping increases. For multiple interacting skyrmion species in the collective regime, we find jammed behavior at low drives where the different skyrmion species are strongly coupled and move in the same direction. As the drive increases, the species decouple and each can lock to a different symmetry direction of the obstacle lattice, making it possible to perform topological sorting in analogy to the particle sorting methods used to fractionate different species of colloidal particles moving over two-dimensional obstacle arrays.

36 MATERIALS SCIENCE↗
NASA NTRS2020

CHAP Enhances Versatility in Colloidal Probe Fabrication

A colloidal probe, comprising a colloidal particle attached to an atomic force microscope cantilever, is employed to measure directly interaction forces between the particle and a surface. It is possible to change or even destroy a particle while attaching it to a cantilever, thus limiting the types of systems to which the colloidal probe technique may be applied. Here we present the Controlled Heating and Alignment Platform (CHAP) for fabricating colloidal probes without altering the original characteristics of the attached particle. The CHAP applies heat directly to the atomic force microscope chip to rapidly and precisely control cantilever temperature. This minimizes particle heating and enables control over the viscosity of thermoplastic adhesive, to prevent it from contaminating the particle surface. 3D-printed components made the CHAP compatible with standard optical microscopes and streamlined the fabrication process while increasing the platform’s versatility. Using the CHAP with a thermoplastic wax adhesive, colloidal probes were fabricated using polystyrene and silica particles between 0.7 and 40 μm in diameter. We characterized the properties and interactions of the adhesive and particles, as well as the properties of the completed probes, to demonstrate the retention of particle features throughout fabrication. Pull-off tests with CHAP’s probes measured adhesive force values in the expected ranges and demonstrated that particles were firmly attached to the cantilevers.

Schmitz, Russell C.↗
DOE OSTI2020

Photo-printing of faceted DNA patchy particles

Patchy particles with shape complementarity can serve as building blocks for assembling colloidal superstructures. Alternatively, encoding information on patches using DNA can direct assembly into a variety of crystalline or other preprogrammed structures. Here, we present a tool where DNA is used both to engineer shape and to encode information on colloidal particles. Two reactive oil emulsions with different but complementary DNA (cDNA) brushes are assembled into CsCl-like crystalline lattices. The DNA brushes are recruited to and ultimately localized at the junctions between neighboring droplets, which gives rise to DNA-encoded faceted patches. The emulsions are then solidified by ultraviolet (UV) polymerization, producing faceted patchy particles. The facet size and DNA distribution are determined by the balance between the DNA binding energy and the elastic deformation energy of droplets. This method leads to a variety of new patchy particles with directional interactions in scalable quantities.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Size and shape fluctuations of ultrasoft colloids

An ultrasoft colloidal particle fluctuates due to its flexibility. Such fluctuation is essential for colloidal structure and dynamics, but is challenging to quantify experimentally. We use dendrimers as a model system to study the fluctuation of ultrasoft colloids. By considering the dynamic polydispersity in the small-angle neutron scattering (SANS) model and introducing the fluctuation of invasive water into the contrast in SANS, we reveal the fluctuating amplitudes of the size and shape of the dendrimer of generation 6 at finite concentrations. The size fluctuation is suppressed while the shape fluctuation increases as the weight fraction of dendrimers passes 11%. With neutron spin echo data, we suggest that such a crossover originates from the competition between the inter- and intraparticle dynamics. Further investigation on lower-generation samples shows a contrary result, which suggests a structural basis for these dynamic phenomena.

42 ENGINEERING↗
DOE OSTI2025

Machine-learning-informed scattering correlation analysis of sheared colloids

We have carried out theoretical analysis, Monte Carlo simulations and machine-learning analysis to quantify microscopic rearrangements of dilute dispersions of spherical colloidal particles from coherent scattering intensity. Both monodisperse and polydisperse dispersions of colloids were created and underwent a rearrangement consisting of an affine simple shear and non-affine rearrangement using the Monte Carlo method. We calculated the coherent scattering intensity of the dispersions and the correlation function of intensity before and after the rearrangement and generated a large data set of angular correlation functions for varying system parameters, including number density, polydispersity, shear strain and non-affine rearrangement. Singular value decomposition of the data set shows the feasibility of machine-learning inversion from the correlation function for the polydispersity, shear strain and non-affine rearrangement using only three parameters. A Gaussian process regressor is then trained on the data set and can retrieve the affine shear strain, non-affine rearrangement and polydispersity with relative errors of 3%, 1% and 6%, respectively. Altogether, our model provides a framework for quantitative studies of both steady and non-steady microscopic dynamics of colloidal dispersions using coherent scattering methods.

Gaussian process regression↗
NASA NTRS2001

Light Microscopy Module: An On-Orbit Microscope Planned for the Fluids and Combustion Facility on the International Space Station

The Light Microscopy Module (LMM) is planned as a fully remotely controllable on-orbit microscope subrack facility, allowing flexible scheduling and control of fluids and biology experiments within NASA Glenn Research Center's Fluids and Combustion Facility on the International Space Station. Within the Fluids and Combustion Facility, four fluids physics experiments will utilize an instrument built around a light microscope. These experiments are the Constrained Vapor Bubble experiment (Peter C. Wayner of Rensselaer Polytechnic Institute), the Physics of Hard Spheres Experiment-2 (Paul M. Chaikin of Princeton University), the Physics of Colloids in Space-2 experiment (David A. Weitz of Harvard University), and the Low Volume Fraction Colloidal Assembly experiment (Arjun G. Yodh of the University of Pennsylvania). The first experiment investigates heat conductance in microgravity as a function of liquid volume and heat flow rate to determine, in detail, the transport process characteristics in a curved liquid film. The other three experiments investigate various complementary aspects of the nucleation, growth, structure, and properties of colloidal crystals in microgravity and the effects of micromanipulation upon their properties. Key diagnostic capabilities for meeting the science requirements of the four experiments include video microscopy to observe sample features including basic structures and dynamics, interferometry to measure vapor bubble thin film thickness, laser tweezers for colloidal particle manipulation and patterning, confocal microscopy to provide enhanced three-dimensional visualization of colloidal structures, and spectrophotometry to measure colloidal crystal photonic properties.

Doherty, Michael P.↗
NASA NTRS1990

Particle migration in suspensions by thermocapillary or electrophoretic motion

Two problems of similar mathematical structure are presented: the thermocapillary motion of bubbles and the electrophoresis of colloidal particles. For both problems, it is shown that in a cloud of n particles surrounded by an infinite expanse of fluid, the velocity of each sphere under creeping flow conditions is equal to the velocity of an isolated particle, unchanged by interactions between the particles. However, when the cloud fills a container, conservation of mass shows that this result cannot continue to hold, and the average translational velocity must be calculated subject to a constraint on the mass flux. It is concluded that the average thermocapillary or electrophoretic translational velocity of a particle in the cloud is related to the effective conductivity of the cloud over the whole range of particle volume fractions, provided that the particles are identical, non-conducting and, for the thermocapillary problem, inviscid.

Acrivos, A.↗
NASA NTRS2000

Glass/Jamming Transition in Colloidal Aggregation

We have studied colloidal aggregation in a model colloid plus polymer system with short-range attractive interactions. By varying the colloid concentration and the strength of the attraction, we explored regions where the equilibrium phase is expected to consist of colloidal crystallites in coexistance with colloidal gas (i.e. monomers). This occurs for moderate values of the potential depth, U approximately equal to 2-5 kT. Crystallization was not always observed. Rather, over an extended sub-region two new metastable phases appear, one fluid-like and one solid-like. These were examined in detail with light scattering and microscopy techniques. Both phases consist of a near uniform distribution of small irregular shaped clusters of colloidal particles. The dynamical and structural characteristics of the ergodic-nonergodic transition between the two phases share much in common with the colloidal hard sphere glass transition.

Segre, Philip N.↗
DOE OSTI2025

Blockage effects in the chemotaxis of diffusiophoretic particles

Transport mechanisms at the micro- and nano-scale play an essential role in regulating intracellular organization. Recent work indicates that directed motion of constituents inside cells can emerge through diffusiophoretic transport, in which colloidal particles move under the influence of chemical gradients. Here, we examine how blockers—passive or actively consuming—reshape those gradients and thereby influence the motion of diffusiophoretic particles. By combining analytical solutions with finite element simulations, we first show that a single blocker can distort a background gradient enough to create or eliminate stagnation points, significantly modifying particle transport. We then introduce a second, explicitly sized blocker at one of these stagnation points and measure how its finite radius alters the diffusiophoretic velocity field for a test particle. Even moderate changes in the second blockers size can cause noticeable shifts in the substrate distribution, highlighting the importance of accounting for explicit particle radii under crowded or consumption-driven conditions. Our findings underscore that subtle geometric variations—such as the radii and positions of two or more blockers—can profoundly affect diffusiophoretic motion, providing a more complete picture of how blocking and crowding phenomena shape intracellular transport.

Song, Zehao [Northwestern Univ., Evanston, IL (Uni↗
DOE OSTI2023

Environmental impact of solution pH on the formation and migration of iron colloids in deep subsurface energy systems

Deep subsurface stimulation processes often promote fluid-rock interactions that can lead to the formation of small colloidal particles that are suspected to migrate through the rock matrix, partially or fully clog pores and microfractures, and promote the mobilization of contaminants. Thus, the goal of this work is to understand the geochemical changes of the host rock in response to reservoir stimulation that promote the formation and migration of colloids. Two different carbonate-rich shales were exposed to different solution pHs (pH = 2 and 7). In this study, iron and other mineral transformations at the shale-fluid interface were first characterized by synchrotron-based XRF mapping. Then, colloids that were able to migrate from the shale into the bulk fluid were characterized by synchrotron-based extended X-ray absorption structure (EXAFS), scanning electron microscopy (SEM), and single-particle inductively coupled plasma time-of-flight mass spectrometry (sp-icpTOF-MS). When exposed to the pH = 2 solution, extensive mineral dissolution and secondary precipitation was observed; iron-(oxyhydr)oxide colloids colocated with silicates were observed by SEM at the fluid-shale interfaces, and the mobilization of chromium and nickel with these iron colloids into the bulk fluid was detected by sp-icpTOF-MS. Iron EXAFS spectra of the solution at the shale-fluid interface suggests the rapid (within minutes) formation of ferrihydrite-like nanoparticles. Thus, we demonstrate that the pH neutralization promotes the mobilization of existing silicate minerals and the rapid formation of new iron colloids. These Fe colloids have the potential to migrate through the shale matrix and mobilize other heavy metals (such as Cr and Ni, in this study) and impacting groundwater quality, as well produced waters from these hydraulic fracturing operations.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2000

Diffusing Wave Spectroscopy Used to Study Foams

The white appearance of familiar objects such as clouds, snow, milk, or foam is due to the random scattering of light by the sample. As we all know, pure water is clear and easily passes a beam of light. However, tiny water droplets, such as those in a cloud, scatter light because the air and water droplet have different indexes of refraction. When many droplets, or scattering sites, are present, the incident light is scattered in random directions and the sample takes on a milky white appearance. In a glass of milk, the scattering is due to small colloidal particles. The white appearance of shaving cream, or foam, is due to the scattering of light at the water-bubble interface. Diffusing wave spectroscopy (DWS) is a laser light-scattering technique used to noninvasively probe the particle dynamics in systems that strongly scatter light. The technique takes advantage of the diffuse nature of light, which is reflected or transmitted from samples such as foams, dense colloidal suspensions (such as paint and milk), emulsions, liquid crystals, sandpiles, and even biological tissues.

Zimmerli, Gregory A.↗
DOE OSTI2022

Plutonium reactive transport in fractured granite: Multi-species experiments and simulations

Plutonium (Pu) in the subsurface environment can transport in different oxidation states as an aqueous solute or as colloidal particles. The transport behavior of Pu is affected by the relative abundances of these species and can be difficult to predict when they simultaneously exist. This study investigates the concurrent transport of Pu intrinsic colloids, Pu(IV) (aq) and Pu(V-VI) (aq) through a combination of controlled experiments and semi-analytical dual-porosity transport modeling. Pu transport experiments were conducted in a fractured granite at high and low flow rates to elucidate sorption processes and their scaling behavior. In the experiments, Pu(IV) (aq) was the least mobile of the Pu species, Pu(V-VI) (aq) had intermediate mobility, and the colloidal Pu, which consisted mainly of precipitated and/or hydrolyzed Pu(IV), was the most mobile. The semi-analytical modeling revealed that the sorption of each Pu species was rate-limited, as the sorption could not be described by assuming local equilibrium in the experiments. The model was able to describe the sorption of the different Pu species that occurring either on fracture surfaces, in the pores of the rock matrix, or simultaneously in both locations. While equally good fits to the data could be achieved using any of these assumptions, a fracture-dominated process was considered to be the most plausible because it provided the most reasonable estimates of sorption rate constants. Importantly, a key result of this work is that the sorption rate constant of all Pu species tends to decrease with increasing time scales, which implies that Pu will tend to be more mobile at longer time scales than observations at shorter time scales suggest. This result has important implications for predicting the environmental impacts of Pu in the safety assessments of geologic repositories for radioactive waste disposal, and we explore potential mechanistic bases for upscaling the sorption rate constants to time and distance scales that cannot be practically evaluated in experiments.

58 GEOSCIENCES↗