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At least 55 records · Page 3

Advanced Newton methods for geodynamical models of Stokes flow with viscoplastic rheologies

Strain localization and resulting plasticity and failure play an important role in the evolution of the lithosphere. These phenomena are commonly modeled by Stokes flows with viscoplastic rheologies. The nonlinearities of these rheologies make the numerical solution of the resulting systems challenging, and iterative methods often converge slowly or not at all. Yet accurate solutions are critical for representing the physics. Moreover, for some rheology laws, aspects of solvability are still unknown. We study a basic but representative viscoplastic rheology law. The law involves a yield stress that is independent of the dynamic pressure, referred to as von Mises yield criterion. Two commonly used variants, perfect/ideal and composite viscoplasticity, are compared. We derive both variants from energy minimization principles, and we use this perspective to argue when solutions are unique. We propose a new stress-velocity Newton solution algorithm that treats the stress as an independent variable during the Newton linearization but requires solution only of Stokes systems that are of the usual velocity-pressure form. To study different solution algorithms, we implement 2-D and 3-D finite element discretizations, and we generate Stokes problems with up to 7 orders of magnitude viscosity contrasts, in which compression or tension results in significant nonlinear localization effects. Comparing the performance of the proposed Newton method with the standard Newton method and the Picard fixed-point method, we observe a significant reduction in the number of iterations and improved stability with respect to problem nonlinearity, mesh refinement, and the polynomial order of the discretization.

Rudi, Johann↗

Modeling of Chemical Slurry Rheology in DWPF Sludge Batch (SB) 10 Simulants

The Defense Waste Processing Facility (DWPF) treats high-activity radionuclides from sludge through a process called vitrification. This process converts radioactive liquid waste currently stored in tank farms into a solid glass form that is suitable for long-term storage and disposal. Due to the complexities involved in vitrifying this waste within each operation of the Chemical Processing Cell (CPC), waste rheology is studied to characterize the fluid-mechanical properties as it passes through the CPC and into the Melter. To better understand the waste and validate flow behavior, slurry rheology of simulants that represents the waste was studied at various acid stoichiometry percentages and solids concentrations to determine the simulant’s yield stress and viscosity. This research work has been supported by the DOE-FIU Science & Technology Workforce Development Initiative, an innovative program developed by the U.S. Department of Energy’s Office of Environmental Management (DOE-EM) and Florida International University’s Applied Research Center (FIU-ARC). During the spring of 2022, a DOE Fellow intern, Brendon Cintas, spent 10 weeks doing a summer internship at Savannah River National Laboratory (SRS) under the supervision and guidance of Dan Lambert, Chemical Flowsheet Development. The intern’s project was initiated on June 6, 2022, and continued through August 11, 2022 with the objective of assisting scientists at SRNL’s Rheology and Grout Laboratory at Aiken Country Technology Lab (ACTL) better understand the sludge composition on the rheology of a simulant slurry using a HAAKE RheoStress 6000 rheometer and extrapolate the results to the real-waste data.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The role of a pressure-dependent rheology in the dynamics of mantle circulation

A thermomechanical model for upper mantle convection was constructed such that the thickness and the structure of the lithosphere are determined self consistently by the heat transported by convection. In this study of the interaction between the lithosphere and upper mantle, strongly temperature and pressure dependent rheologies for both Newtonian and non-Newtonian creep mechanisms are employed. For a strictly temperature dependent rheology an insignificant amount of heat, less than 12.5 mW/sq m, can be transported convectively for an interior viscosity, 0(10 sup 21 Pas), compatible with post glacial rebound. On the other hand, for similar values of the interior viscosity, steady heat fluxes between 20 and 40 mW/sq m are produced by introducing pressure dependence into the rheology. For the temperature and pressure dependent flow law the horizontally averaged interior temperature displays very little variation with the amount of heat evacuated, once all of the rheological parameters are fixed. This finding may have important ramifications for parameterized convection.

Yuen, D. A.↗

Convection in Ice I with Composite Newtonian/Non-Newtonian Rheology: Application to the Icy Galilean Satellites

Ice I exhibits a complex rheology at temperature and pressure conditions appropriate for the interiors of the outer ice I shells of Europa, Ganymede, and Callisto. We use numerical methods to determine the conditions required to trigger convection in an ice I shell with a stress-, temperature-, and grain-size-dependent rheology measured in laboratory experiments by Goldsby and Kohlstedt [2001] (henceforth GK2001). Triggering convection from an initially conductive ice shell with a non-Newtonian rheology for ice I requires that a finite-amplitude temperature perturbation be issued to the ice shell [2]. Here, we characterize the amplitude and wavelength of temperature perturbation required to initiate convection in the outer ice I shells of Europa, Ganymede, and Callisto using the GK2001 rheology for a range of ice grain sizes.

Barr, Amy C.↗

Convective Instability in Ice I with Non-Newtonian Rheology: Application to the Galilean Satellites

At the temperatures and stresses associated with the onset of convection in an ice I shell of the Galilean satellites, ice behaves as a non-Newtonian fluid with a viscosity that depends on both temperature and strain rate. The convective stability of a non-Newtonian ice shell can be judged by comparing the Rayleigh number of the shell to a critical value. Previous studies suggest that the critical Rayleigh number for a non-Newtonian fluid depends on the initial conditions in the fluid layer, in addition to the thermal, rheological, and physical properties of the fluid. We seek to extend the existing definition of the critical Rayleigh number for a non-Newtonian, basally heated fluid by quantifying the conditions required to initiate convection in an ice I layer initially in conductive equilibrium. We find that the critical Rayleigh number for the onset of convection in ice I varies as a power (-0.6 to -0.5) of the amplitude of the initial temperature perturbation issued to the layer, when the amplitude of perturbation is less than the rheological temperature scale. For larger-amplitude perturbations, the critical Rayleigh number achieves a constant value. We characterize the critical Rayleigh number as a function of surface temperature of the satellite, melting temperature of ice, and rheological parameters so that our results may be extrapolated for use with other rheologies and for a generic large icy satellite. The values of critical Rayleigh number imply that triggering convection from a conductive equilibrium in a pure ice shell less than 100 km thick in Europa, Ganymede, or Callisto requires a large, localized temperature perturbation of a few kelvins to tens of kelvins to soften the ice and therefore may require tidal dissipation in the ice shell.

Barr, A. C.↗

Multi-fidelity modeling to predict the rheological properties of a suspension of fibers using neural networks and Gaussian processes

Unveiling the rheological properties of fiber suspensions is of paramount interest to many industrial applications. There are multiple factors, such as fiber aspect ratio and volume fraction, that play a significant role in altering the rheological behavior of suspensions. Three-dimensional (3D) numerical simulations of coupled differential equations of the suspension of fibers are computationally expensive and time-consuming. Machine learning algorithms can be trained on the available data and make predictions for the cases where no numerical data are available. However, some widely used machine learning surrogates, such as neural networks, require a relatively large training dataset to produce accurate predictions. Multi-fidelity models, which combine high-fidelity data from numerical simulations and less expensive lower fidelity data from resources such as simplified constitutive equations, can pave the way for more accurate predictions. Here, we focus on neural networks and the Gaussian processes with two levels of fidelity, i.e., high and low fidelity networks, to predict the steady-state rheological properties, and compare them to the single-fidelity network. High-fidelity data are obtained from direct numerical simulations based on an immersed boundary method to couple the fluid and solid motion. The low-fidelity data are produced by using constitutive equations. Multiple neural networks and the Gaussian process structures are used for the hyperparameter tuning purpose. Results indicate that with the best choice of hyperparameters, both the multi-fidelity Gaussian processes and neural networks are capable of making predictions with a high level of accuracy with neural networks demonstrating marginally better performance.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Controlling Rheology of Fluid Interfaces through Microblock Length of Sequence-Controlled Amphiphilic Copolymers

Previous studies have demonstrated that films of sequence-controlled amphiphilic copolymers display contact angles that depend on microblock size. This suggests that microblock length may provide a means of tuning surface and interfacial properties. In this work, the interfacial rheology of a series of sequence-controlled copolymers, prepared through the addition of bicyclo[4.2.0]oct-1(8)-ene-8-carboxamide (monomer A) and cyclohexene (monomer B) to generate sequences up to 24 monomeric units composed of (A m B n ) i microblocks, where m, n, and i range from 1 to 6. Interfacial rheometry is used to measure the mechanical properties of an air–water interface with these copolymers. As the microblock size increases, the interfacial storage modulus, G', increases, which may be due to an increase in the size of interfacial hydrophobic domains. Small-angle X-ray scattering shows that the copolymers have a similar conformation in solution, suggesting that any variations in the mechanics of the interface are due to assembly at the interface, and not on solution association or bulk rheological properties. This is the first study demonstrating that microblock size can be used to control interfacial rheology of amphiphilic copolymers. Here, the results provide a new strategy for controlling the dynamics of fluid interfaces through precision sequence-controlled polymers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Rheological and microstructural characterization of aqueous suspensions of carbon black and reduced graphene oxide

Carbon black is often used as a conductivity enhancer in battery electrodes. Reduced graphene oxide is another conducting material, with a high aspect ratio sheet-like morphology, and offers the possibility of generating a conducting network at loadings that are small compared to carbon black. Suspensions of conducting carbon, active materials and binders are typically coated on current collectors during the formation of electrodes. The rheology of these suspensions is an important indicator of the connectivity of particles in the suspension and impacts the electrical conductivity as well as the thickness of the coated layer. In this work, the rheology and microstructures of aqueous suspensions of para-aminobenzoic acid terminated carbon black (CB) with and without reduced graphene oxide (RGO) were investigated. The CB loading varied between 0.05 wt.% -10 wt.%, while the samples containing RGO had an RGO loading of 0.05 wt.%. The pH of the suspension was varied from 7.5 to 3. The carboxyl groups on the CB surface are deprotonated at pH 7.5, making the particles hydrophilic. Protonation of the carboxylate groups at pH 3 makes the particles partially hydrophobic. Suspensions of CB showed Newtonian behavior at all loadings for pH 7.5, and at loadings below 1.5 wt.% for pH 3. They are shear thinning at loadings between 1.5–10 wt.%. Interestingly, the low shear viscosity is non-monotonic with CB loading, rising up to a CB loading of 7.5 wt.%, and then dropping at 10 wt.%. Cryogenic scanning electron microscopy (SEM) showed CB particles forming aggregates at pH 3 for CB loadings greater than 1.5 wt.%. At pH 3, addition of 0.05 wt.% RGO resulted in a viscosity increase for suspensions containing 0.5 wt.% CB, as the RGO formed connections with CB particles that enhanced network formation. Adding RGO had little effect on suspensions that had 1.5 wt.% CB. The combination of SEM imaging and suspension rheology provides insight into the particle connectivity for the carbon-based materials studied here. These insights will be useful in determining coating conditions for slurries used in rechargeable battery electrodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Coarse-grained simulation of colloidal self-assembly, cation exchange, and rheology in Na/Ca smectite clay gels

Knowledge Gap: The aggregation of clay minerals—layered silicate nanoparticles—strongly impacts fluid flow, solute migration, and solid mechanics in soils, sediments, and sedimentary rocks. Experimental and computational characterization of clay aggregation is inhibited by the delicate water-mediated nature of clay colloidal interactions and by the range of spatial scales involved, from 1 nm thick platelets to flocs with dimensions up to micrometers or more. Simulations: Using a new coarse-grained molecular dynamics (CGMD) approach, we predicted the microstructure, dynamics, and rheology of hydrated smectite (more precisely, montmorillonite) clay gels containing up to 2,000 clay platelets on length scales up to 0.1 μm. Further, simulations investigated the impact of simulation time, platelet diameters (6 to 25nm), and the ratio of Na to Ca exchangeable cations on the assembly of tactoids (i.e., stacks of parallel clay platelets) and larger aggregates (i.e., assemblages of tactoids). We analyzed structural features including tactoid size and size distribution, basal spacing, counterion distribution in the electrical double layer, clay association modes, and the rheological properties of smectite gels. Findings: Our results demonstrate new potential to characterize and understand clay aggregation in dilute suspensions and gels on a scale of thousands of particles with explicit representation of counterion clouds and with accuracy approaching that of all-atom molecular dynamics (MD) simulations. For example, our simulations predict the strong impact of Na/Ca ratio on clay tactoid formation and the shear-thinning rheology of clay gels.

42 ENGINEERING↗

Rheological effects of moisture content on the anatomical fractions of loblolly pine (Pinus taeda)

Here, this study focused on assessing the influence of moisture content on the rheological properties of different anatomical fractions of pine residue using the FT4 powder rheometer. Moisture content exhibited some influence on the 2 mm bark and needle fractions, increasing their cohesion, angle of internal friction, unconfined yield strength, and major principal stress. Stem and whole, on the other hand, presented minimal changes upon moisture introduction. All 4 mm fractions did not show many changes in their rheological properties with moisture introduction, which can be due to less particle-particle interactions and consequently reducing any liquid bridging the particles might undergo; however, they were shown to have a more unpredictable behavior compared to the 2 mm analogues (i.e., higher standard deviation) which can be due to a higher degree of particle-interlocking. Out of the three fractions, needle presented the poorest rheological properties for flowability in addition to being susceptible by moisture, unlike other fractions.

36 MATERIALS SCIENCE↗

Mapping Structure and Rheology of pH-Responsive Resins for Low-VOC Coatings

In recent years, the paint and coatings industry has shifted away from traditional resin formulations that require high concentrations of volatile organic compounds (VOCs) to achieve the desired rheological performance and sustainability targets. One approach to eliminate or reduce VOCs in paint and coating formulations while maintaining the final performance is to disperse stimuli-responsive polymer latex particles in water. The chemistry and architecture of these particles have been engineered such that the suspension rheology changes in response to the pH changes. The particles can also be swollen with organic solvents to illicit similar rheological changes. To understand how the particle microstructure influences the observed macroscopic properties, we use small-angle neutron scattering and dynamic light scattering to determine that these particles consist of a cross-linked core with long polymer tails that extend into the dispersing medium. Carboxylic acid groups present on the tails deprotonate with increasing pH, and the extension of the polymer chain due to charge repulsion increases the hydrodynamic drag on the particle. Here we find that adjusting the pH alone has a much more significant effect on the shear dependence of the viscosity of the studied resin than adding organic solvent alone. We also find that this resin architecture is more responsive per mole of pH-responsive group than other architectures of pH-responsive latex particles in the literature.

36 MATERIALS SCIENCE↗

Effects of PLA/PHB Blend Ratio and Wood Flour Loading on the Melt Rheology and Thermomechanical Properties of Biobased Polymer Composites

The development of sustainable, biobased polymer composites is crucial for reducing supply chain dependence on fossil fuels. A major challenge lies in understanding and predicting the processability of these sustainable material alternatives, which directly impacts large-scale manufacturing. Here, this study systematically investigates the effect of poly(lactic acid) (PLA)/polyhydroxybutyrate (PHB) blend ratios and wood flour (WF) loadings on the thermal, rheological, and mechanical properties of the composites. Composites were prepared via melt compounding and characterized by using differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), oscillatory shear melt rheology, tensile testing, and scanning electron microscopy. Results showed that increasing the PHB content lowered the glass transition temperature, while higher PHB and WF loadings decreased thermal stability. Complex viscosity decreased with increasing PHB in 0 and 10% WF, whereas it increased in 20% and 30% WF for PHB-rich blends (80/20 and 70/30 PLA/PHB) due to stronger filler interactions with flexible PHB chains. At 30% WF, PHB-containing composites also showed elastic dominance with G′ higher than G″. This behavior was confirmed by van Gurp–Palmen plots, where the phase angle decreased with increasing PHB and WF loadings. WF addition also shifted Cole–Cole plots away from semicircular terminal relaxation, while time–temperature superposition validity was maintained, confirming that polymer chain dynamics continue to dominate melt behavior. Young’s modulus increased with WF loading, while tensile strength and toughness decreased due to weaker interfacial adhesion between the matrix and the filler. Interestingly, 10% WF systems containing PHB exhibited the highest toughness among all of the filled systems, indicating synergistic reinforcement from WF fillers and PHB-induced ductility. Overall, melt rheology effectively captured the internal structure and stiffness of the composites as the formulation changed, reinforcing the concept that the PLA/PHB ratio and WF content can be tuned to adjust melt elasticity and balance mechanical property trade-offs for targeted applications.

melt rheology↗

Use of Lignin-Based Admixture as Water Reducer (WRA) for Tailoring the Rheological Properties of Mortars for 3D-Printing

Efforts towards decarbonizing construction materials and industrial processes related to cement and concrete can be aided via multifaceted approaches that target alternative admixtures as well as precision control of fabrication. Chemical admixtures for water reduction have played a crucial role in the development of advanced mortar and concrete mixtures. Newer biomass processing techniques developed for aviation fuel production from corn stover biomass produce a highly reactive lignin byproduct that is suitable for chemical modifications to mimic the properties of commonly used polycarboxylate ethers (PCEs) with a smaller carbon footprint. These lignin-based plasticizers developed at NREL can be used in place of petrochemical-derived superplasticizers to tailor the rheological properties of cement-based systems for applications such as additive manufacturing while reducing the carbon intensity of the concrete mix. Lignosulfonates derived from paper pulping were historically used as water reducers only to be displaced with the rise of PCEs. The present study examines the use of a NREL produced lignin-based water reducing admixture (WRA), in cement pastes and mortar mixtures for 3D-printing at small- (mm) scale. The experimental program consisted of different formulations of oxidized lignin-based WRAs added in variable dosages to cement pastes with a fixed water-to-cement ratio. The objective is to achieve an appropriate workability, extrudability and buildability of mortar mixtures to produce 3D-printed specimens. The rheological characterization was performed to compare the initial yield stress and viscosity of the different mixtures with lignin-based admixture with respect to conventional PCE superplasticizers. The rheological characterization shows that the proposed material act as an effective water-reducer in cement systems, affecting the yield stress, plastic viscosity, and structuration rate of the mixtures evaluated. On the other hand, the effect on early hydration process of the cement pastes containing lignin-based admixtures is comparable to conventional superplasticizers.

3D-printing↗

Evaluation of the rheological and electrical percolation of high‐density polyethylene/carbon black composites using mathematical models

Abstract In this work, conductive polymer composites (CPCs) of bio‐based polyethylene (BioPe) containing different concentrations of carbon black (CB) were developed. By using oscillatory rheology analysis, a Newtonian plateau was observed in BioPe, and all BioPe/CB composites had a behavior of a pseudo‐solid and that composites with volume fractions ranging from 0.24 to 0.56 presented higher viscosity, storage, and loss modulus. This suggests the formation of a percolated network and by using the power‐law models, it was observed that the electrical percolation threshold was higher than the rheological percolation threshold. The electrical conductivity was measured using the four‐point probe method and a sigmoid model was used to predict the CPCs' electrical conductivity percolation threshold. The results indicated that the four‐point probe method presented satisfactory results according to the calculated standard deviations and voltage–current characteristics for each round of measurements considering the same ranging as used in rheology analysis. The analytical model used showed a coefficient of determination ( R 2 ) higher than 95%, allowing the prediction of the electrical conductivity of the CPC and the percolation threshold as a function of the volumetric fraction of the CB.

da SiIva, Moacy P.↗

Assessment of asymmetrical rheological behavior of cementitious material for 3D printing application

Among the multiplicity of construction methods based on digital concrete technologies, the most common one remains the extrusion-based process. Two opposed strategies have been developed in order to print a concrete structure using extrusion: the first one emphasizes the ease-of-pumping of material which is massively accelerated to ensure the stability of the structure, when leaving the extruder; the second one uses a firm mortar able to sustain the own weight of the structure during the printing, without requiring any accelerator. Both methods have their pros and cons and don't imply the same rheological requirements. Most of the recent literature assumes that both types of material (fluid and firm) follow the same trend of behavior and obey to the Von Mises plasticity criterion, while it has been demonstrated that firm cement-based materials can exhibit a pressure dependent behavior. Moreover, rheological study is mainly based on shear rheometry, while the extrusion-based printing process requires a description of the rheological behavior in compression to predict the global stability of the structure, and in tension to prevent cracks formation. This paper investigates the fresh behavior of cement paste and mortar under different solicitations (shear, compression, tension) for different water to cement ratios. The analysis of these results allows to describe the transition between a ductile fluid material (symmetrical in tension and compression) that obeys to a Von Mises plasticity criterion, and a brittle and firm material (asymmetrical in tension and compression) that requires a pressure dependent plasticity criterion in order to predict its strength under a given solicitation.

36 MATERIALS SCIENCE↗

Scaling of Shear Rheology of Concentrated Charged Colloidal Suspensions across Glass Transition

Electrostatic interparticle interactions are a key component in controlling and designing rheological characteristics of concentrated charged colloidal suspensions. Herein, we investigate electroviscous effects on shear rheology using highly charged silica particles. By fixing the volume fraction but varying the salinity, the system undergoes a glass transition as evidenced by the evolution of the yield stress and zero-shear viscosity. We show that the steady shear viscosities obey a critical scaling relation that scales the flow curves into a super- and a sub-critical branch with glass transition salinity serving as the bifurcation point; we also demonstrate an isoviscosity scaling that collapses all isoviscosity lines into a single master curve that exhibits no singularity. Based on each scaling relation, in conjunction with common modeling equations, the quantitative relationships between the shear viscosity, stress, and salinity are established. This study demonstrates a new framework to model the steady shear rheology of concentrated charged colloids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Large-Scale Compatibilization of Postconsumer Polyolefins in the Presence of Paraffin Wax as a Rheology Modifier

Postconsumer polyolefins (r-POs) are leading plastic waste contributors today. This study reports, for the first time, the compatibilization of r-POs at a 50 kilogram (kg) scale with a styrene block copolymer compatibilizer in the presence of paraffin waxes as rheology modifiers (RMs). The addition of the rheological modifier (RM) and compatibilizer enhances the melt flow indices (MFIs) and mechanical properties, respectively. One aspect of this study is to compare the effectiveness of low-cost paraffin wax to that of specialized and expensive RMs in r-POs. The mechanical and rheological properties such as the melt flow index (MFI) of r-POs were compared in the presence of two types of RMs. Next, the study explores the challenges encountered when scaling the compatibilization of r-POs in the presence of paraffin wax from a 10-g to a 50-kg scale. The mechanical properties were determined and compared for samples at different scales. The study further investigated the effect of the method used for blending paraffin wax with r-PO and its impact on the value of their MFI and mechanical properties. This at-scale validation could pave the way for the commercialization of r-POs.

crystallinity↗

Fluctuations and power-law scaling of dry, frictionless granular rheology near the hard-particle limit

Here the flow of frictionless granular particles is studied with stress-controlled discrete element modeling simulations for systems varying in size from 300 to 100,000 particles. The volume fraction and shear-stress ratio μ are relatively insensitive to system size for a wide range of inertial numbers I. Second-order effects in strain rate, such as normal stress differences, require large system sizes to accurately extract meaningful results, notably a nonmonotonic dependence in the first normal stress difference with strain rate. The rheological response represented by the μ(I) scalar model works well at describing the lower-order aspects of the rheology, except near the quasistatic limit of these stress-controlled flows. The pressure is varied over five decades, and a pressure dependence of the coordination number is observed, which is not captured by the inertial number. Large fluctuations observed for small systems N≤1000 near the quasistatic limit can lead to the arrest of flow resulting in challenges to fitting the data to rheological relationships. The inertial number is also insufficient for capturing the pressure-dependent behavior of property fluctuations. Fluctuations in the flow and microstructural properties are measured in both the quasistatic and inertial regimes, including shear stress, pressure, strain rate, normal stress differences, volume fraction, coordination number, and contact fabric anisotropy. The fluctuations in flow properties scale self-similarly with pressure and system size. A transition in the scaling of fluctuations of stress properties and contact fabric anisotropy are measured and proposed as a quantitative identification of the transition from inertial to quasistatic flow.

36 MATERIALS SCIENCE↗