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At least 559 records · Page 31
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Explicit Monotone Stable Super-Time-stepping Methods for Finite Time Singularities

We explore a novel way to numerically resolve the scaling behavior of finite-time singularities in solutions of nonlinear parabolic PDEs. The Runge–Kutta–Legendre (RKL) and Runge–Kutta–Gegenbauer (RKG) super-time-stepping methods were originally developed for nonlinear complex physics problems with diffusion. These are multistage single step second-order, forward-in-time methods with no implicit solves. The advantage is that the time-step size for stability scales with stage number 𝑠 as $\mathcal{O}$⁡(𝑠 2 ). Many interesting nonlinear PDEs have finite-time singularities, and the presence of diffusion often limits one to using implicit or semi-implicit time-step methods for stability constraints. Finite-time singularities are particularly challenging due to the large range of scales that one desires to resolve, often with adaptive spatial grids and adaptive time steps. Here, in this study, we show two examples of nonlinear PDEs for which the self-similar singularity structure has time and space scales that are resolvable using the RKL and RKG methods, without forcing even smaller time steps. Compared to commonly used implicit numerical methods, we achieve a significantly smaller run time while maintaining comparable accuracy. We also prove numerical monotonicity for both the RKL and RKG methods under their linear stability conditions for the constant coefficient heat equation, in the case of infinite domain and periodic boundary condition, leading to a theoretical guarantee of the superiority of the RKL and RKG methods over traditional super-time-stepping methods, such as the Runge-Kutta-Chebyshev and the orthogonal Runge-Kutta-Chebyshev methods. Code can be found at https://github.com/ZT220501/SRK-Singularity.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2024

Overview of ASDEX upgrade results in view of ITER and DEMO

Experiments on ASDEX Upgrade (AUG) in 2021 and 2022 have addressed a number of critical issues for ITER and EU DEMO. A major objective of the AUG programme is to shed light on the underlying physics of confinement, stability, and plasma exhaust in order to allow reliable extrapolation of results obtained on present day machines to these reactor-grade devices. Concerning pedestal physics, the mitigation of edge localised modes (ELMs) using resonant magnetic perturbations (RMPs) was found to be consistent with a reduction of the linear peeling-ballooning stability threshold due to the helical deformation of the plasma. Conversely, ELM suppression by RMPs is ascribed to an increased pedestal transport that keeps the plasma away from this boundary. Candidates for this increased transport are locally enhanced turbulence and a locked magnetic island in the pedestal. The enhanced D-alpha (EDA) and quasi-continuous exhaust (QCE) regimes have been established as promising ELM-free scenarios. Here, the pressure gradient at the foot of the H-mode pedestal is reduced by a quasi-coherent mode, consistent with violation of the high-n ballooning mode stability limit there. This is suggestive that the EDA and QCE regimes have a common underlying physics origin. In the area of transport physics, full radius models for both L- and H-modes have been developed. These models predict energy confinement in AUG better than the commonly used global scaling laws, representing a large step towards the goal of predictive capability. A new momentum transport analysis framework has been developed that provides access to the intrinsic torque in the plasma core. In the field of exhaust, the X-Point Radiator (XPR), a cold and dense plasma region on closed flux surfaces close to the X-point, was described by an analytical model that provides an understanding of its formation as well as its stability, i.e., the conditions under which it transitions into a deleterious MARFE with the potential to result in a disruptive termination. With the XPR close to the divertor target, a new detached divertor concept, the compact radiative divertor, was developed. Here, the exhaust power is radiated before reaching the target, allowing close proximity of the X-point to the target. No limitations by the shallow field line angle due to the large flux expansion were observed, and sufficient compression of neutral density was demonstrated. With respect to the pumping of non-recycling impurities, the divertor enrichment was found to mainly depend on the ionisation energy of the impurity under consideration. In the area of MHD physics, analysis of the hot plasma core motion in sawtooth crashes showed good agreement with nonlinear 2-fluid simulations. This indicates that the fast reconnection observed in these events is adequately described including the pressure gradient and the electron inertia in the parallel Ohm’s law. Concerning disruption physics, a shattered pellet injection system was installed in collaboration with the ITER International Organisation. Thanks to the ability to vary the shard size distribution independently of the injection velocity, as well as its impurity admixture, it was possible to tailor the current quench rate, which is an important requirement for future large devices such as ITER. Progress was also made modelling the force reduction of VDEs induced by massive gas injection on AUG. The H-mode density limit was characterised in terms of safe operational space with a newly developed active feedback control method that allowed the stability boundary to be probed several times within a single discharge without inducing a disruptive termination. Regarding integrated operation scenarios, the role of density peaking in the confinement of the ITER baseline scenario (high plasma current) was clarified. The usual energy confinement scaling ITER98(p,y) does not capture this effect, but the more recent H20 scaling does, highlighting again the importance of developing adequate physics based models. Advanced tokamak scenarios, aiming at large non-inductive current fraction due to non-standard profiles of the safety factor in combination with high normalised plasma pressure were studied with a focus on their access conditions. A method to guide the approach of the targeted safety factor profiles was developed, and the conditions for achieving good confinement were clarified. Based on this, two types of advanced scenarios (‘hybrid’ and ‘elevated’

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2019

Three-dimensional flow model development for thermal mixing and stratification modeling in reactor system transients analyses

Mixing, thermal-stratification, and mass transport phenomena in large pools or enclosures play major roles for the safety of reactor systems. Depending on the fidelity requirement and computational resources, various modeling methods, from the 0-D perfect mixing model to 3-D Computational Fluid Dynamics (CFD) models, are available. Each is associated with its own advantages and shortcomings. It is very desirable to develop an advanced and efficient thermal mixing and stratification modeling capability embedded in a modern system analysis code to improve the accuracy of reactor safety analyses and to reduce modeling uncertainties. An advanced system analysis tool, SAM, is being developed at Argonne National Laboratory for advanced non-LWR reactor safety analysis. While SAM is being developed as a system-level modeling and simulation tool, a reduced-order three-dimensional module is under development to model the mull-dimensional flow and thermal mixing and stratification in large enclosures of reactor systems. This paper provides an overview of the three-dimensional finite element flow model in SAM, including the governing equations, stabilization scheme, and solution methods. Additionally, several verification and validation tests are presented, including lid-driven cavity flow, natural convection inside a cavity, laminar flow in a channel of parallel plates. Here, based on the comparisons with the analytical solutions and experimental results, it is demonstrated that the developed 3-D fluid model can perform very well for a wide range of flow problems.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2017

Development of a Reduced-Order Three-Dimensional Flow Model for Thermal Mixing and Stratification Simulation during Reactor Transients

Mixing, thermal-stratification, and mass transport phenomena in large pools or enclosures play major roles for the safety of reactor systems. Depending on the fidelity requirement and computational resources, various modeling methods, from the 0-D perfect mixing model to 3-D Computational Fluid Dynamics (CFD) models, are available. Each is associated with its own advantages and shortcomings. It is very desirable to develop an advanced and efficient thermal mixing and stratification modeling capability embedded in a modern system analysis code to improve the accuracy of reactor safety analyses and to reduce modeling uncertainties. An advanced system analysis tool, SAM, is being developed at Argonne National Laboratory for advanced non-LWR reactor safety analysis. While SAM is being developed as a system-level modeling and simulation tool, a reduced-order three-dimensional module is under development to model the multi-dimensional flow and thermal mixing and stratification in large enclosures of reactor systems. This paper provides an overview of the three-dimensional finite element flow model in SAM, including the governing equations, stabilization scheme, and solution methods. Additionally, several verification and validation tests are presented, including lid-driven cavity flow, natural convection inside a cavity, laminar flow in a channel of parallel plates. Based on the comparisons with the analytical solutions and experimental results, it is demonstrated that the developed 3-D fluid model can perform very well for a wide range of flow problems.

Hu, Rui↗
DOE OSTI2024

Dynamic flux surrogate-based partitioned methods for interface problems

Loosely coupled partitioned methods for multiphysics problems treat each subproblem as a separate entity and advance them independently in time. In so doing these methods enable code reuse, increase concurrency and provide a convenient framework for plug-and-play multiphysics simulations. However, mathematically loosely coupled schemes are equivalent to a single step of an iterative solution method, which can compromise their accuracy and stability. We present a new data-driven partitioned method for coupled parametric PDEs that can improve upon the accuracy of traditional loosely coupled methods without incurring a performance penalty. To that end, we replace conventional field transfers across the interface by a surrogate for the dynamics of the interface flux exchanged between the subdomains. To develop this surrogate we apply dynamic mode decomposition to a non-standard staggered-in-time state, comprising the interface flux and small solution patches near the interface. The new approach shifts the main computational burden to an offline training phase, whereas application of the surrogate in the online phase amounts to a single matrix–vector multiplication. In conclusion, we provide stability analysis of the surrogate-based partitioned scheme and include numerical results that demonstrate its potential.

Dynamic mode decomposition (DMD)↗
DOE OSTI2016

The mechanism of the emergence of distinct overstretched DNA states

Although multiple overstretched DNA states were identified in experiments, the mechanism of the emergence of distinct states is still unclear. Molecular dynamics simulation is an ideal tool to clarify the mechanism, but the force loading rates in stretching achieved by conventional all-atom DNA models are much faster, which essentially affect overstretching states. We employed a modified coarse-grained DNA model with an unprecedented low loading rate in simulations to study the overstretching transitions of end-opened double-stranded DNA. We observed two-strand peeling off for DNA with low stability and the S-DNA with high stability under tension. By introducing a melting-forbidden model which prevents base-pair breaking, we still observed the overstretching transition induced by the formation of S-DNA due to the change of dihedral angle. Hence, we confirmed that the competition between the two strain-softening manners, i.e., base-pair breaking and dihedral angle variation, results in the emergence of distinct overstretched DNA states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Lithium decoration of three dimensional boron-doped graphene frameworks for high-capacity hydrogen storage

Based on density functional theory and the first principles molecular dynamics simulations, a three-dimensional B-doped graphene-interconnected framework has been constructed that shows good thermal stability even after metal loading. The average binding energy of adsorbed Li atoms on the proposed material (2.64 eV) is considerably larger than the cohesive energy per atom of bulk Li metal (1.60 eV). This value is ideal for atomically dispersed Li doping in experiments. From grand canonical Monte Carlo simulations, high hydrogen storage capacities of 5.9 wt% and 52.6 g/L in the Li-decorated material are attained at 298 K and 100 bars.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Adaptive generalized combination complex synchronization of uncertain real and complex nonlinear systems

With comprehensive consideration of generalized synchronization, combination synchronization and adaptive control, this paper investigates a novel adaptive generalized combination complex synchronization (AGCCS) scheme for different real and complex nonlinear systems with unknown parameters. On the basis of Lyapunov stability theory and adaptive control, an AGCCS controller and parameter update laws are derived to achieve synchronization and parameter identification of two real drive systems and a complex response system, as well as two complex drive systems and a real response system. Two simulation examples, namely, ACGCS for chaotic real Lorenz and Chen systems driving a hyperchaotic complex Lü system, and hyperchaotic complex Lorenz and Chen systems driving a real chaotic Lü system, are presented to verify the feasibility and effectiveness of the proposed scheme.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Development and Stability Analysis of Representative Future High Renewable Penetration Power Grid Models for California

The power grid in California is now experiencing a significant increase in renewable generation to achieve 100% clean energy by 2040. This paper discusses a method for developing the transient stability (TS) model of the future high renewable penetration in the power grid in California. The method consists of utilizing an existing future Western Electricity Coordinating Council (WECC) grid model in the database and locating the conventional plants in the base model that will potentially retire in the next few years in California. Next, the dynamic models of those identified conventional plants and controls in the existing model are modified to replicate the future power generation in the California region. Different scenarios of future power grid in California are developed for various renewable penetration levels and control strategies in renewable power plants. The effect of the control strategies on the stability of the power grid under events like loss of generation are evaluated. Based on these evaluations, certain control features in power plants are identified as necessary for stability of future power grids.

Samanta, Sayan↗
DOE OSTI2015

Time-dependent projected Hartree-Fock

Projected Hartree-Fock (PHF) has recently emerged as an alternative approach to describing degenerate systems where static correlation is abundant, when the spin-symmetry is projected. Here, we derive a set of linearized time-dependent equations for PHF in order to be able to access excited states. The close connection of such linear-response time-dependent PHF (TDPHF) to the stability condition of a PHF wave function is discussed. Expanding this analysis also makes it possible to give analytical expressions for the projected coupling terms of Hamiltonian and overlaps between excited Slater determinants. TDPHF with spin-projection (TDSUHF) and its Tamm-Dancoff approximation are benchmarked for several electronically degenerate molecules including the dissociating H{sub 2}, F{sub 2} and O{sub 3} at equilibrium, and the distorted ethylene. It is shown that they give consistently better descriptions of excited states than does time-dependent HF (TDHF). Furthermore, we demonstrate that they offer not only singly but also doubly excited states, which naturally arise upon spin-projection. We also address the thermodynamic limit of TDSUHF, using non-interacting He gas. While TDPHF singly excited states tend to converge to those of HF with the size of the system due to the lack of size-extensivity of PHF, doubly excited states remain reasonable even at the thermodynamic limit. We find that the overall performance of our method is systematically better than the regular TDHF in many cases at the same computational scaling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Cu impurity in insulators and in metal-insulator-metal structures: Implications for resistance-switching random access memories

We present numerical results from atomistic simulations of Cu in SiO{sub 2} and Al{sub 2}O{sub 3}, with an emphasis on the thermodynamic, kinetic, and electronic properties. The calculated properties of Cu impurity at various concentrations (9.91 × 10{sup 20 }cm{sup −3} and 3.41 × 10{sup 22 }cm{sup −3}) in bulk oxides are presented. The metal-insulator interfaces result in up to a ∼4 eV reduction in the formation energies relative to the crystalline bulk. Additionally, the importance of Cu-Cu interaction in lowering the chemical potential is introduced. These concepts are then discussed in the context of formation and stability of localized conductive paths in resistance-switching Random Access Memories (RRAM-M). The electronic density of states and non-equilibrium transmission through these localized paths are studied, confirming conduction by showing three orders of magnitude increase in the electron transmission. The dynamic behavior of the conductive paths is investigated with atomistic drift-diffusion calculations. Finally, the paper concludes with a molecular dynamics simulation of a RRAM-M cell that attempts to combine the aforementioned phenomena in one self-consistent model.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

A stochastic perturbation method to generate inflow turbulence in large-eddy simulation models: Application to neutrally stratified atmospheric boundary layers

Despite the variety of existing methods, efficient generation of turbulent inflow conditions for large-eddy simulation (LES) models remains a challenging and active research area. Herein, we extend our previous research on the cell perturbation method, which uses a novel stochastic approach based upon finite amplitude perturbations of the potential temperature field applied within a region near the inflow boundaries of the LES domain [Muñoz-Esparza et al., “Bridging the transition from mesoscale to microscale turbulence in numerical weather prediction models,” Boundary-Layer Meteorol., 153, 409–440 (2014)]. The objective was twofold: (i) to identify the governing parameters of the method and their optimum values and (ii) to generalize the results over a broad range of atmospheric large-scale forcing conditions, U{sub g} = 5 − 25 m s{sup −1}, where U{sub g} is the geostrophic wind. We identified the perturbation Eckert number, Ec=U{sub g}{sup 2}/ρc{sub p}θ{sup ~}{sub pm}, to be the parameter governing the flow transition to turbulence in neutrally stratified boundary layers. Here, θ{sup ~}{sub pm} is the maximum perturbation amplitude applied, c{sub p} is the specific heat capacity at constant pressure, and ρ is the density. The optimal Eckert number was found for nonlinear perturbations allowed by Ec ≈ 0.16, which instigate formation of hairpin-like vortices that most rapidly transition to a developed turbulent state. Larger Ec numbers (linear small-amplitude perturbations) result in streaky structures requiring larger fetches to reach the quasi-equilibrium solution, while smaller Ec numbers lead to buoyancy dominated perturbations exhibiting difficulties for hairpin-like vortices to emerge. Cell perturbations with wavelengths within the inertial range of three-dimensional turbulence achieved identical quasi-equilibrium values of resolved turbulent kinetic energy, q, and Reynolds-shear stress, . In contrast, large-scale perturbations acting at the production range exhibited reduced levels of , due to the formation of coherent streamwise structures, while q was maintained, requiring larger fetches for the turbulent solution to stabilize. Additionally, the cell perturbation method was compared to a synthetic turbulence generator. The proposed stochastic approach provided at least the same efficiency in developing realistic turbulence, while accelerating the formation of large-scales associated with production of turbulent kinetic energy. Also, it is computationally inexpensive and does not require any turbulent information.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Electronic structures and magnetic stabilities of 2D Mn-doped GaAs nanosheets: The role of long-range exchange interactions and doping strategies

We investigate the structural, electronic and magnetic properties of Mn atoms doped two-dimensional (2D) hexagonal GaAs nanosheets (GaAsNSs) using both first-principle calculations and Monte Carlo simulations. The first-principle molecular dynamics is first used to test the structural stability of Mn-doped GaAsNS ((Ga,Mn)AsNS). The analysis of spin-resolved electronic structures and determination of magnetic exchange interactions based on density functional theory (DFT) calculations reveals the existence of long-range exchange interaction in the system. Finally, Metropolis Monte Carlo simulation is employed to estimate Curie temperatures (T{sub C}s) of (Ga,Mn)AsNSs with different doping concentrations by different doping strategies. The results indicate that a T{sub C} up to 82 K can be obtained in regularly-doped (Ga,Mn)AsNSs and doping strategies have prominent impact on T{sub C}s of the systems, which emphasizes the importance of both long-range interactions and doping strategies in reduced dimensional diluted magnetic semiconductors (DMSs)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

A positive and entropy-satisfying finite volume scheme for the Baer–Nunziato model

We present a relaxation scheme for approximating the entropy dissipating weak solutions of the Baer–Nunziato two-phase flow model. This relaxation scheme is straightforwardly obtained as an extension of the relaxation scheme designed in for the isentropic Baer–Nunziato model and consequently inherits its main properties. To our knowledge, this is the only existing scheme for which the approximated phase fractions, phase densities and phase internal energies are proven to remain positive without any restrictive condition other than a classical fully computable CFL condition. For ideal gas and stiffened gas equations of state, real values of the phasic speeds of sound are also proven to be maintained by the numerical scheme. It is also the only scheme for which a discrete entropy inequality is proven, under a CFL condition derived from the natural sub-characteristic condition associated with the relaxation approximation. This last property, which ensures the non-linear stability of the numerical method, is satisfied for any admissible equation of state. We provide a numerical study for the convergence of the approximate solutions towards some exact Riemann solutions. The numerical simulations show that the relaxation scheme compares well with two of the most popular existing schemes available for the Baer–Nunziato model, namely Schwendeman–Wahle–Kapila's Godunov-type scheme and Tokareva–Toro's HLLC scheme . The relaxation scheme also shows a higher precision and a lower computational cost (for comparable accuracy) than a standard numerical scheme used in the nuclear industry, namely Rusanov's scheme. Finally, we assess the good behavior of the scheme when approximating vanishing phase solutions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Excipient screening by lyophilization provides insights into spray drying formulations for nanoparticle vaccines

Nanoparticles have shown great promise as delivery platforms in the development of tunable and safe vaccines. Nanolipoprotein particles (NLPs), also known as nanodiscs, are discoidal nanoparticles composed of a lipid bilayer stabilized at their periphery by apolipoproteins. Under the right conditions, the NLP self-assembly process is highly customizable in terms of lipids and apolipoprotein constituents, allowing for tunable physical and chemical characteristics. This flexibility allows a wide range of vaccine antigens and adjuvants to be incorporated onto the NLP platform for tailored vaccine design. The stability of NLPs during long term storage is a very important factor in developing a vaccine delivery platform suitable for widespread global use. When stored in a solution for extended periods of time, NLPs dissociate into their corresponding lipids and protein constituents, leading to particle degradation. Proper stabilization of NLPs can often be achieved by lyophilization (i.e. freeze-drying), a method widely used for various applications including pharmaceuticals. This process, however, can be damaging to particles without the presence of lyoprotectants or excipients that help maintain particle stability during lyophilization. Another method used to stabilize vaccines and pharmaceuticals is spray drying, a process that converts liquid formulations into dry powders through controlled heating and airflow. While spray drying is rapid, scalable, and cost-effective, lyophilization is typically a gentler process that better retains biomolecule structure and function. Both processes use excipients for particle stabilization, so lyophilization can be used as a surrogate to test stability of NLPs, to down-select formulations that may withstand the harsher conditions of spray drying. To screen different formulations, NLPs were synthesized and purified to homogeneity by size exclusion chromatography (SEC) and samples were prepared with a wide range of lyoprotectants and/or excipients. To assess the protective effects of excipients on NLPs upon spray drying, both pre- and post-lyophilized samples were analyzed by SEC. To assess the protective effects upon heating (encountered during the spray drying process), NLP samples were incubated at elevated temperatures prior to SEC analysis. The lyoprotectants and excipients evaluated in this study had different efficiencies in protecting NLPs during lyophilization and heating tests. Trehalose, for example, exhibits stabilization on NLPs both upon lyophilization and heating whereas leucine accelerated NLP dissociation. Although some lyoprotectants are effective by themselves, different combinations can decrease the stabilization of NLPs. Shelf-stable vaccines that do not require cold-chain storage are essential for global accessibility and our findings provide fundamental insight into how to advance NLP-based vaccines for these applications.

Serrano, Litzay J [Lawrence Livermore National Lab↗
DOE OSTI2021

Reactive Flows in Porous Media: Challenges in Theoretical and Numerical Methods

We review theoretical and computational research, primarily from the past 10 years, addressing the flow of reactive fluids in porous media. The focus is on systems where chemical reactions at the solid–fluid interface cause dissolution of the surrounding porous matrix, creating nonlinear feedback mechanisms that can often lead to greatly enhanced permeability. Here, we discuss insights into the evolution of geological forms that can be inferred from these feedback mechanisms, as well as some geotechnical applications such as enhanced oil recovery, hydraulic fracturing, and carbon sequestration. Until recently, most practical applications of reactive transport have been based on Darcy-scale modeling, where averaged equations for the flow and reactant transport are solved. We summarize the successes and limitations of volume averaging, which leads to Darcy-scale equations, as an introduction to pore-scale modeling. Pore-scale modeling is computationally intensive but offers new insights as well as tests of averaging theories and pore-network models. We include recent research devoted to validation of pore-scale simulations, particularly the use of visual observations from microfluidic experiments.

wormhole formation↗
DOE OSTI2022

Stabilization and control of persistent current magnets using variable inductance

Ultra-stable, tunable magnetic fields are desirable for a wide range of applications in medical imaging, electron microscopy, quantum science, and atomic physics. Superconducting magnets operated in persistent current mode, with device current flowing in a closed superconducting loop disconnected from a power source, are a common approach for applications with the most stringent requirements on temporal field stability. In this work, we present a method for active control of this persistent current by means of dynamic inductance change within the superconducting circuit. For a first realization of this general technique, we consider a variable superconducting inductor placed in series with the main magnet. The inductor acts as a dynamic flux storage device capable of transferring flux to or from the main magnet through inductance change. This allows for fine and fast adjustments of the persistent current without the use of thermal switches that limit the speed and accuracy of many present-day methods. With first experiments employing this technique, we demonstrate stabilization of a 1.95 T Nb–Ti round lens for electron microscopy against decay resulting from residual losses in the superconducting circuit, and more generally show flexibility for precise control over the magnitude and waveform of the persistent current.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Shear Thickening Electrolyte Built from Sterically Stabilized Colloidal Particles

We present a method to prepare shear thickening electrolytes consisting of silica nanoparticles in conventional liquid electrolytes with limited flocculation. These electrolytes rapidly and reversibly stiffen to solidlike behaviors in the presence of external shear or high impact, which is promising for improved lithium ion battery safety, especially in electric vehicles. However, in initial chemistries the silica nanoparticles aggregate and/or sediment in solution over time. Here, we demonstrate steric stabilization of silica colloids in conventional liquid electrolyte via surface-tethered PMMA brushes, synthesized via surface-initiated atom transfer radical polymerization. The PMMA increases the magnitude of the shear thickening response, compared to the uncoated particles, from 0.311 to 2.25 Pa s. Ultrasmall-angle neutron scattering revealed a reduction in aggregation of PMMA-coated silica nanoparticles compared to bare silica nanoparticles in solution under shear and at rest, suggesting good stabilization. Conductivity tests of shear thickening electrolytes (30 wt % solids in electrolyte) at rest were performed with interdigitated electrodes positioned near the meniscus of electrolytes over the course of 24 h to track supernatant formation. Conductivity of electrolytes with bare silica increased from 10.1 to 11.6 mS cm –1 over 24 h due to flocculation. In contrast, conductivity of electrolytes with PMMA-coated silica remained stable at 6.1 mS cm –1 over the same time period, suggesting good colloid stability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗