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DOE OSTI2017

Viscous regularization of the full set of nonequilibrium-diffusion Grey Radiation-Hydrodynamic equations

A viscous regularization technique, based on the local entropy residual, was proposed by Delchini et al. (2015) to stabilize the nonequilibrium-diffusion Grey Radiation-Hydrodynamic equations using an artificial viscosity technique. This viscous regularization is modulated by the local entropy production and is consistent with the entropy minimum principle. However, Delchini et al. (2015) only based their work on the hyperbolic parts of the Grey Radiation-Hydrodynamic equations and thus omitted the relaxation and diffusion terms present in the material energy and radiation energy equations. Here in this paper, we extend the theoretical grounds for the method and derive an entropy minimum principle for the full set of nonequilibrium-diffusion Grey Radiation-Hydrodynamic equations. This further strengthens the applicability of the entropy viscosity method as a stabilization technique for radiation-hydrodynamic shock simulations. Radiative shock calculations using constant and temperature-dependent opacities are compared against semi-analytical reference solutions, and we present a procedure to perform spatial convergence studies of such simulations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Revisiting Bayesian constraints on the transport coefficients of QCD

Multistage models based on relativistic viscous hydrodynamics have proven successful in describing hadron measurements from relativistic nuclear collisions. These measurements are sensitive to the shear and the bulk viscosities of QCD and provide a unique opportunity to constrain these transport coefficients. Bayesian analyses can be used to obtain systematic constraints on the viscosities of QCD, through methodical model-to-data comparisons. In this manuscript, we discuss recent developments in Bayesian analyses of heavy ion collision data. Furthermore, we highlight the essential role of closure tests in validating a Bayesian analysis before comparison with measurements. We discuss the role of the emulator that is used as proxy for the multistage theoretical model. We use an ongoing Bayesian analysis of soft hadron measurements by the JETSCAPE Collaboration as context for the discussion.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

Langmuir adsorption model to assess the impact of silane coupling on nano-dispersion of silica in SBR

Surface active agents are often used to improve dispersion of nanoparticles. Quantitative correlation between these surface-active molecules and nanoscale dispersion is absent from the literature partly because a quantitative measure of nanoscale dispersion does not exist. Recently, we have developed the Virial-van der Waals method to quantify dispersion in nanocomposites using virial coefficients. In this paper, the Langmuir adsorption model is used to quantify the influence of surface-active agents on nano-scale dispersion in terms of the effective second virial coefficient B 2 *. The impact of silane coupling agent on the nano-dispersion and silica aggregate structure in precipitated silica/SBR nanocomposites is demonstrated. It is shown that the higher viscosity SBR matrix led to a greater silica aggregate structural breakup, while lower viscosity matrix improved surface silanization. The isomeric content of the SBR, which impacts the dielectric behavior, impacted whether the system could be modeled through a mean-field or specific interactions. We earlier showed that larger aggregates improve dispersion, and this is reaffirmed in these results. After account is made for aggregate size, nano-scale dispersion improves with the addition of silane coupling agent. The behavior is well modeled using Langmuir monolayer adsorption.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Versatile Liquid Crystal Elastomer Formulations Using Amine-Acrylate Chemistry and Processing for Advanced Manufacturing

This study aims to tune rheological properties of liquid crystal elastomers (LCEs) through a strategic approach, leveraging the differing reaction rates of thiols and primary and secondary amines with acrylate monomers or the inclusion of processing additives to enable amenability to advanced manufacturing. We found that varying the time of oligomerization at elevated temperatures of amine-functional monomers with acrylate-functional monomers enabled simple control of rheological properties. Additionally, we could also control rheological properties by introducing reinforcing fillers or organic solvents. By varying the oligomerization conditions, we achieved a broad range of viscosities, from 1.1 Pa s to 560 Pa s as measured at 60 °C. When the rheological properties were varied through the incorporation of various solid and liquid inclusions, viscosities could range from less than 1 Pa s to nearly 1000 Pa s when measured at 60 °C. The shape morphing capabilities that are intrinsic to LCEs and the mechanical properties were also characterized. Here, we find that the oligomerization conditions and the addition of fillers influence shape morphing and energy absorption, as characterized by the stress–strain characteristics, further suggesting their potential to be used in energy dissipation applications where performance can be turned. Last, we demonstrate how the range of accessible rheological properties grants formulations amenable to various advanced manufacturing techniques.

Liquid chromatography↗

DOE OSTI2023

Modeling the Impact of the Organic Aerosol Phase State on Multiphase OH Reactive Uptake Kinetics and the Resultant Heterogeneous Oxidation Timescale of Organic Aerosol in the Amazon Rainforest

Accurate predictions of chemical lifetime, i.e., oxidation timescale and change in the mass of organic aerosols (OAs) in atmospheric models, are critical to quantify the impacts of OA on aerosol–cloud interactions, radiative forcing, and air quality. The heterogeneous oxidation of OA by hydroxyl (OH) radicals is a key process governing OA mass changes during their oxidation. Recently, laboratory observations of the OH uptake coefficient (γ OH ) and heterogeneous reaction rate (k het,OH ) for different OA systems with varying phase states have been combined to develop a new parameterization of γ OH and k het,OH as a function of the OA phase state, i.e., viscosity (η OA ). Here, in this work, we use a recently published viscosity prediction framework to analyze the new γ OH and k het,OH parameterization with a box model. Subsequently, we implement this box model to predict γ OH and k het,OH over the Amazon rainforest in the dry-to-wet transition season with both significant biomass burning and biogenic influences. Relevant parameters within our box model are specified based on detailed regional model simulations over the Amazon using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). η OA is predicted as a function of species volatility, OA composition (including water uptake) along with ambient relative humidity (RH), and temperature. Based on ambient conditions simulated by WRF-Chem over the entire atmospheric column, we use the box model to predict the upper bounds of the heterogeneous oxidation timescale of OA. Based on previous laboratory measurements, we assume that this heterogeneous OH oxidation causes fragmentation (carbon loss) of OA, followed by the evaporation of the fragmented molecules that results in the exponential decay of OA. We predict that the oxidation timescale of OA is ~1 month near the Earth’s surface in the pristine Amazonian background because of low OH concentrations. But OA is oxidized more rapidly within urban and wildfire plumes near the Earth’s surface with an order of magnitude higher OH concentrations compared to the pristine background, causing the simulated oxidation timescale of OA to be much shorter, ~3–4 days. At 3–5 km altitudes where biomass burning OA is predicted to be semisolid, the heterogeneous oxidation timescale is estimated as ~6 days to 3 weeks and decreases with increasing OH concentrations within plumes. We show that the simulated mass loss of OA is strongly size-dependent, where smaller particles oxidize more rapidly compared to larger particles due to their greater per-particle surface area-to-volume ratio. Increasing urbanization and deforestation in the Amazon in the future might increase OH concentrations in the background Amazon, causing faster oxidation of OA. At higher altitudes above liquid clouds, especially in the upper troposphere where temperatures approach ~250 K, future measurements are needed to reduce the uncertainties related to the mass loss of OA at colder temperatures and low relative humidity conditions due to its heterogeneous OH oxidation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Investigation of Shear-Thinning Behavior on Film Thickness and Friction Coefficient of Polyalphaolefin Base Fluids With Varying Olefin Copolymer Content

This study investigates the rheological properties, elastohydrodynamic (EHD) film-forming capability, and friction coefficients of low molecular mass poly-alpha-olefin (PAO) base stocks with varying contents of high molecular mass olefin copolymers (OCPs) to assess their shear stability and their potential for energy-efficient lubrication. Several PAO-OCP mixtures were blended in order to examine the relationship between their additive content and tribological performance. Gel permeation chromatography (GPC) and nuclear magnetic resonance (NMR) spectroscopy were used to characterize the molecular masses and structures, respectively. Density, viscosity, EHD film thickness, and friction were measured at 303 K, 348 K, and 398 K. Film thickness and friction were studied at entrainment speeds relevant to the boundary, mixed, and full-film lubrication regimes. The PAO-OCP mixtures underwent temporary shear-thinning resulting in decreases in film thickness and hydrodynamic friction. These results demonstrate that the shear characteristics of PAO-OCP mixtures can be tuned with the OCP content and provide insight into the effects of additives on EHD characteristics.

Elastohydrodynamic lubrication↗

DOE OSTI2023

Shear and combustion characterization of printable ammonium perchlorate composite propellant formulations

Seven formulations of ammonium perchlorate composite propellant (APCP) are developed and their properties relevant for successful additive manufacture are characterized. Extrusion in a custom-built 3D printing system and spindle viscometry are used to collect viscosity measurements of curing primary and non-curing secondary versions of the formulations. The formulations that behave similarly to a Bingham plastic, with apparent viscosities between 4 and 8 thousand Pa*s at 30 minutes post-mix, are determined to be most suitable for printing applications. Measurements of one material show a yield stress of 1 kPa. Ambient pressure burn rates of 2.0–2.9 mm/s were measured for the compositions tested. All measured burn rates were comparable to the lower end of typical burn rates for APCP. In conclusion, the results of the characterization demonstrate a propellant suitable for use in a 3D printing system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

A Piecewise Deterministic Markov Toy Model for Traffic/Maintenance and Associated Hamilton–Jacobi Integrodifferential Systems on Networks

We study optimal control problems in infinite horizon whxen the dynamics belong to a specific class of piecewise deterministic Markov processes constrained to star-shaped networks (corresponding to a toy traffic model). We adapt the results in Soner (SIAM J Control Optim 24(6):1110–1122, 1986) to prove the regularity of the value function and the dynamic programming principle. Extending the networks and Krylov’s “shaking the coefficients” method, we prove that the value function can be seen as the solution to a linearized optimization problem set on a convenient set of probability measures. The approach relies entirely on viscosity arguments. As a by-product, the dual formulation guarantees that the value function is the pointwise supremum over regular subsolutions of the associated Hamilton–Jacobi integrodifferential system. This ensures that the value function satisfies Perron’s preconization for the (unique) candidate to viscosity solution.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2017

Influence of Contrast Agent Dilution on Ballon Deflation Time and Visibility During Tracheal Balloon Dilation: A 3D Printed Phantom Study

PurposeTo determine the effect of contrast medium dilution during tracheal balloon dilation on balloon deflation time and visibility using a 3-dimensional (3D) printed airway phantom.Materials and MethodsA comparison study to investigate balloon deflation times and image quality was performed using two contrast agents with different viscosities, i.e., iohexol and ioxithalamate, and six contrast dilutions with a 3D printed airway phantom.ResultsCompared to 1:0 concentration, 3:1, 2:1, 1:1, 1:2, and 1:3, contrast/saline ratios resulted in a 46% (56.2 s), 59.8% (73.1 s), 74.9% (91.6 s), 81.7% (99.8 s), and 83.5% (102 s) reduction for iohexol, respectively, and a 51.8% (54.7 s), 63.8% (67.6 s), 74.7% (79.2 s), 80.5% (85.3 s), and 82.4% (87.4 s) reduction for ioxithalamate, respectively, in the mean balloon deflation time, although at the expense of decreased balloon opacity (3.5, 6.9, 11.1, 12.4, and 13.9%, for iohexol, respectively, and 3.2, 6, 9.6, 10.8, and 12.4%, for ioxithalamate, respectively).ConclusionsUse of a lower viscosity contrast agent and higher contrast dilution is considered to be able to reduce balloon deflation times and then simultaneously decrease visualization of balloons. The rapid balloon deflation time is likely to improve the safe performance of interventional procedures.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

DOE OSTI2017

Simplified Pore Network Model for Analysis of Flow Capacity and Residual Oil Saturation Distribution Based on Computerized Tomography

The pore network (connected tunnels) can be used not only to describe pore geometry inside a rock but also to calculate various fluid flow properties on a micro scale. Based on a “digital core” extracted from micro computerized tomography (μ-CT), we have developed a simplified pore network model. This study simplifies the pore structure as a lattice of cubes. Pore size, pore distribution, tunnel connectivity, fluid viscosity, interfacial tension, and the external driving pressure gradient are considered for each adjacent cube to evaluate the flow capacity of the pore network. We calculated the permeability, effective permeability, and effective sweep efficiency. The results show that fluid flow initially starts in the largest tunnel, which corresponds to the threshold pressure of the rock sample (fluid flow onset pressure). Permeability changes nonlinearly before all the tunnels are involved in the flow. Changes in the microscopic residual oil saturation and the sweep efficiency were visualized based on the three-dimensional pore distribution. Visualization shows that more oil remains in the formation, the heterogeneity is greater, and the oil viscosity is higher.

58 GEOSCIENCES↗

DOE OSTI2017

Effects of Diisocyanate and Polymeric Epoxidized Chain Extenders on the Properties of Recycled Poly(Lactic Acid)

Increasing demand in the use of poly(lactic acid) (PLA) leads to a debate about using potential foodstuffs for plastic production and a moral issue when starvation problem is taken into account. One of the solutions is recycling of PLA; however, recycling results in property losses during melt processing due to low thermal stability of PLA. This study focuses on using chain extenders to offset thermal degradation of recycled PLA. The effects of a diisocyanate and a polymeric epoxidized chain extender on the properties of the recycled poly(lactic acid) were investigated. In order to mimic the recycling process, PLA was subjected to thermo-mechanical degradation using a laboratory scale compounder. Chain extender type, loading and mixing time were investigated. On-line rheology and intrinsic viscosity measurements of PLA before and after chain extension confirmed that the molecular weight increased. Dynamic mechanical analysis, rheology and tensile tests revealed that the chain extenders led to a significant increase in modulus, strength and melt-viscosity. It was found that diisocyanate had slightly higher and faster chain extension reactivity than polymeric extender. Differential scanning calorimetry results showed an increase in the crystallization temperature due to the branched and extended chain structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Melt Flow Behavior and Processability of Polylactic Acid/Polystyrene (PLA/PS) Polymer Blends

The present investigation dealt with the flow behavior and processability of polylactic acid/polystyrene (PLA/PS) polymer blends using a capillary rheometer. For this purpose, PLA/PS blends with different ratios of the concentrations were prepared using a single screw extruder. The shear viscosity, shear stress, shear rate, power-law index, viscous activation energy at a constant shear stress, and elongational stress were determined. PLA/PS blends exhibited a typical shear-thinning behavior over the entire range of shear rates tested, and the viscosity values of the blends would tend to decrease with increasing amount of PLA. In addition, the polymer blend of 70 % PLA and 30 % PS was found to be relatively less sensitive to the processing temperature, implying that the extrusion process was more desirable for fabrication of PLA/PS polymer blend than the injection process.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Enhancing the Melt Strength of Poly(Lactic Acid) via Micro-Crosslinking and Blending with Poly(Butylene Adipate-co-Butylene Terephthalate)for the Preparation of Foams

The melt strength of poly(lactic acid) (PLA) is an important factor in preparing foams and blowing films. Aiming to endow PLA with a suitable melt strength via a slight crosslink, a superficial micro-crosslinking method was introduced in which the PLA feed was mixed with benzoyl peroxide (BPO) and crosslinked in a 100 °C oven for 1 h. Additionally, poly(butyleneadipate-co-terephthalate) (PBAT) was blended with the crosslinked PLA (C-PLA) to further improve melt strength and viscosity. The blend foams were prepared using a single-screw extruder and azodicarbonamide as a foaming agent. The properties were characterized by gel fraction, melt flow rate (MFR), rheometry, DSC and SEM. The rheological results showed that the complex viscosity and storage modulus of C-PLA and C-PLA/PBAT blends increased, attributed to the micro-crosslinking and addition of PBAT and indicating an improvement in melt strength. Furthermore, the crystallization of modified PLA was also enhanced. Compared with pure PLA foams, the C-PLA/PBAT blend foams showed larger cells with more uniform shapes and homogenous distribution. This approach to improve the melt strength of polymers with micro-crosslinking and blending with PBAT represents an attractive method for preparing foams with regular cells.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Cetyltrimethyl Ammonium Bromide Modified Kaolin as a Reinforcing Filler for Natural Rubber

Cure characteristics, Mooney viscosity and physico-mechanical properties of natural rubber (NR) containing CTAB modified kaolin have been studied. NR mix containing 6 phr (parts per hundred part rubber) of CTAB modified kaolin showed significant increases in cure rate and state of cure as compared to gum NR compound and a mix containing the same amount of unmodified kaolin. Lower Mooney viscosity of the NR mix containing CTAB modified kaolin suggested improved processability. Reinforcing effect of CTAB modified kaolin in NR was evident from higher chemical crosslink density index, tensile modulus, hardness, tensile strength and tear strength. Besides, the NR vulcanizate containing 6 phr of CTAB modified kaolin showed lower abrasion loss and heat build-up which could be beneficial for applications such as tire treads.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Dispersion and Rheological Properties of Aqueous Graphene Suspensions in Presence of Nanocrystalline Cellulose

The possibility and feasibility of nanocrystalline cellulose (NCC) for dispersing hydrophobic graphene in aqueous solutions were studied in the present work. The dispersion properties of graphene particles in aqueous media as a function of various amounts of NCC were investigated. The rheological behavior of NCC-dispersed graphene suspensions was studied, and a polynomial model was proposed and employed to simulate the obtained shear flow of graphene suspensions. The results of UV–Vis analysis and sedimentation test suggested that the increased NCC addition significantly led to the improved dispersion properties of graphene suspensions. Rheological behavior measurements demonstrated that graphene suspensions exhibited a reduction trend in the shear viscosity, shear stress, and viscoelasticity with the increased amount of NCC addition. Meanwhile, the shear viscosity and shear stress of graphene suspensions were found to show a dependency on the process temperature. The above results supported the conclusion that NCC is a promising candidate for improving the dispersion and flowability of graphene in aqueous media.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2019

Synthesis and Performance Evaluation of Unsaturated Polyester Blends of Resins and Its Application on Non-woven/Fabric Jute Fibers Reinforced Composites

The present study focuses on the generation of eco-friendly value added product by utilizing bio-based material as reinforced and matrix phase. Processing of soy and alkyd resin as matrix was carried out by utilization of soy flour and Ricinodendron heudelotii oil, followed essential modification in few inferior properties of soy flour resin by blending with alkyd resin. Separate sets of resin were prepared by maintaining 0%, 5% and 10% of alkyd resin in 100 g of soy flour resin respectively in each set to attain a comparative study on performance of prepared sets of resin blend. Subsequently, performance evaluation of polyester blends was evaluated by processing with non-woven/fabric jute fibers reinforced composites. The blend of R. heudelotii oil based alkyd and soy-flour resin in processing of composites was the noval approach of the study. The resins blend were characterized by FT–IR, viscosity and zeta potential measurements while thermo-mechanical analyses, water absorbancy and surface analyses were performed in composites. Significant increases noticed in the viscosity of blend, the blend containing 10% alkyd resin is two times more viscous compared to soy-flour resin. Furthermore, improvement in properties including water absorption, thermo-mechanical properties and better fiber-matrix interfacial adhesion of the composite could be observed. Higher glass transition temperature T{sub g} value i.e. 126.8 °C obtained for composites with 10% blend as matrix might emphasizes on increase of the degree of cross linking provided by the α-eleostearic fatty acid chain moiety. The enhancements in properties indicate extending opportunities for fiber-reinforced composites in several industries including building material, furniture, aerospace, nano etc.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Effect of Initial FeO Content and CaO:SiO{sub 2} Ratio on the Reduction Smelting Kinetics of the CaO-SiO{sub 2}-MgO{sub satd.}-FeO Slag System

The effect of the initial FeO content and CaO:SiO{sub 2} ratio (CaO mass pct/SiO{sub 2} mass pct) on the reduction smelting of FeO with carbon flake addition is investigated in the CaO-MgO{sub satd.}-SiO{sub 2}-FeO slag system at 1823 K (1550 °C). Carbon rapidly reacted with FeO in the molten slag, causing both foaming and compositional changes in the slag. As FeO is reduced, the MgO saturation is modified, and solid precipitants, including MgO and other complex oxides, were observed, which significantly affected the slag properties, including the viscosity and foaming behavior. The solid-phase fraction and viscosity were estimated from changes in the measured FeO content over time using the thermochemical software FactSage. The iron recovery, which is distinguished from the amount of reduced Fe droplets, showed opposite behavior to the measured maximum foaming height and modified foaming index. According to the FeO mass transfer coefficient considering slag foaming at various initial FeO contents and CaO:SiO{sub 2} ratios, the reduction rate was optimal at higher initial FeO contents and a CaO:SiO{sub 2} ratio of 2.0, which did not correspond to the optimal iron recovery at an initial FeO content of 44 mass pct and above and a CaO:SiO{sub 2} ratio of 1.2. The results showed that slag foaming may increase the reduction kinetics, but the slag composition needs to be optimized for greater iron recovery.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Influence of Melt Superheating Treatment on Solidification Characteristics and Rupture Life of a Third-Generation Ni-Based Single-Crystal Superalloy

The influence of melt superheating treatment on the melt properties, solidification characteristics, and rupture life of a third-generation Ni-based single-crystal superalloy was investigated to reveal the critical temperature range of melt structure evolution and its effect on rupture life. The results showed that the viscosity of superalloy decreased but the surface tension increased with increasing superheating temperature. Two characteristic temperature points where the melt viscosity and undercooling degree suddenly change were determined to be 1600 °C and 1700 °C, respectively. Similarly, the stability of the solidification interface firstly improved and then weakened with increasing superheating temperature. The dendrite arms were well refined and the segregation was reduced at 1700 °C. In addition, the rupture life obtained at 1100 °C and 137 MPa increased by approximately 30 pct, approaching the rupture life of the corresponding superalloy containing 2 pct Ru, with increasing superheating temperature from 1500 °C to 1700 °C. When the melt was further heated to 1800 °C, the rupture life decreased. The evolutions of solidification characteristics and rupture life with increasing melt superheating temperature were attributed to changes in the melt structure.

36 MATERIALS SCIENCE↗