Development of MLIPs for Interfaces in solid state batteries
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Energy - Storage↗
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Results for “Interface state”
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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Interface morphogenesis with a deformable secondary phase in solid-state lithium batteries
Here, the complex morphological evolution of lithium metal at the solid-state electrolyte interface limits performance of solid-state batteries, leading to inhomogeneous reactions and contact loss. Inspired by biological morphogenesis, we developed an interfacial self-regulation concept in which a deformable secondary phase dynamically aggregates at the interface in response to local electro-chemo-mechanical stimuli, enhancing contact. The stripping of a lithium electrode that contains 5 to 20 mole % electrochemically inactive sodium domains causes spontaneous sodium accumulation across the interface, with the sodium deforming to attain intimate electrical contact without blocking lithium transport. This process, characterized with operando x-ray tomography and electron microscopy, mitigates voiding and improves cycling at low stack pressures. The counterintuitive strategy of adding electrochemically inactive alkali metal to improve performance demonstrates the utility of interfacial self-regulation for solid-state batteries.
Yoon, Sun Geun [Georgia Institute of Technology, A↗
Solid-Solid Interfaces in Solid-State Batteries
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solid interface↗
Design Through Manufacturing: The Solid Model - Finite Element Analysis Interface
State-of-the-art computer aided design (CAD) presently affords engineers the opportunity to create solid models of machine parts which reflect every detail of the finished product. Ideally, these models should fulfill two very important functions: (1) they must provide numerical control information for automated manufacturing of precision parts, and (2) they must enable analysts to easily evaluate the stress levels (using finite element analysis - FEA) for all structurally significant parts used in space missions. Today's state-of-the-art CAD programs perform function (1) very well, providing an excellent model for precision manufacturing. But they do not provide a straightforward and simple means of automating the translation from CAD to FEA models, especially for aircraft-type structures. The research performed during the fellowship period investigated the transition process from the solid CAD model to the FEA stress analysis model with the final goal of creating an automatic interface between the two. During the period of the fellowship a detailed multi-year program for the development of such an interface was created. The ultimate goal of this program will be the development of a fully parameterized automatic ProE/FEA translator for parts and assemblies, with the incorporation of data base management into the solution, and ultimately including computational fluid dynamics and thermal modeling in the interface.
Rubin, Carol↗
Characterizing Electrode Materials and Interfaces in Solid-State Batteries
Solid-state batteries (SSBs) could offer improved energy density and safety, but the evolution and degradation of electrode materials and interfaces within SSBs are distinct from conventional batteries with liquid electrolytes and represent a barrier to performance improvement. Over the past decade, a variety of imaging, scattering, and spectroscopic characterization methods has been developed or used for characterizing the unique aspects of materials in SSBs. These characterization efforts have yielded new understanding of the behavior of lithium metal anodes, alloy anodes, composite cathodes, and the interfaces of these various electrode materials with solid-state electrolytes (SSEs). This review provides a comprehensive overview of the characterization methods and strategies applied to SSBs, and it presents the mechanistic understanding of SSB materials and interfaces that has been derived from these methods. This knowledge has been critical for advancing SSB technology and will continue to guide the engineering of materials and interfaces toward practical performance.
25 ENERGY STORAGE↗
Design Through Manufacturing: The Solid Model-Finite Element Analysis Interface
State-of-the-art computer aided design (CAD) presently affords engineers the opportunity to create solid models of machine parts reflecting every detail of the finished product. Ideally, in the aerospace industry, these models should fulfill two very important functions: (1) provide numerical. control information for automated manufacturing of precision parts, and (2) enable analysts to easily evaluate the stress levels (using finite element analysis - FEA) for all structurally significant parts used in aircraft and space vehicles. Today's state-of-the-art CAD programs perform function (1) very well, providing an excellent model for precision manufacturing. But they do not provide a straightforward and simple means of automating the translation from CAD to FEA models, especially for aircraft-type structures. Presently, the process of preparing CAD models for FEA consumes a great deal of the analyst's time.
Rubin, Carol↗
All‐Solid‐State Batteries With Mechanically Stable Interfaces Consisting of a Zero‐Strain Cation‐Disordered Rocksalt Cathode
Interface stabilization is critical to the development of working all‐solid‐state batteries. Rigid cathode/solid electrolyte interfaces often disintegrate due to anisotropic volume change of cathode‐active materials, resulting in irreversible capacity loss. Herein, we demonstrate that Li 1.211 Mo 0.467 Cr 0.3 O 2 (LMCO), a pioneering cation‐disordered rocksalt oxide (DRX) cathode that has intrinsically small volume change upon lithium intercalation, can be integrated with a thiophosphate‐based solid electrolyte for all‐solid‐state batteries. Interface stability of the all‐solid LMCO cell was investigated by electrochemical impedance spectroscopy, X‐ray micro‐computed tomography, and electron microscopy. Since LMCO was initially synthesized as a layered phase exhibiting a large volume change, interface disintegration can be observable in the early cycles. As layered LMCO phase‐transformed into DRX LMCO in subsequent cycles, reintegration of the interfaces occurs within a pressurized cell as a result of its zero‐stain behavior. Consequently, the DRX LMCO cathode maintains interface integrity, and thus electrical wiring, over an extended number of cycles, leading to improved capacity retention with small internal cell resistance.
DRX↗
Machine-learning interatomic potentials for interfaces in all-solid-state batteries: Perspectives on training data, model selection, and validation
Interfaces play a pivotal role in dictating the performance and reliability of all-solid-state batteries (ASSBs), where complex electro-chemo-mechanical phenomena at grain boundaries (GBs) and interfaces can lead to degradation and failure. Traditional atomistic simulation methods, such as first-principles calculations and classical molecular dynamics, face limitations in modeling these interfaces due to either high computational cost or insufficient transferability to the diverse atomic environments evolving at interfaces. Machine-learning interatomic potentials (MLIPs) have emerged as a transformative approach, enabling large-scale, high-accuracy simulations of disordered and chemically complex systems by leveraging the predictability of machine learning models trained on first-principles data. Recent applications of MLIPs have demonstrated their ability to capture intricate behaviors at ASSB interfaces, including ion transport, interfacial evolution, and degradation mechanisms, with accuracy and efficiency unattainable by conventional methods. This prospective paper presents comprehensive analysis and practical guidance for MLIP development for GBs and interfaces in ASSBs, with a focus on three key pillars: data generation, model selection, and validation. Here, we review the current state of MLIP applications for GBs and interfaces in both general and ASSB-specific materials, highlighting best practices and challenges in constructing diverse and representative datasets, choosing appropriate machine learning architectures, and rigorously validating model performance. We also discuss emerging strategies and opportunities for improved reliability and efficiency of MLIPs to simulate realistic interfaces in ASSBs.
Energy - Storage↗
Comparative Analysis of Reactivity of Al and Ga Doped Garnet Solid State Electrolyte at the Interface with Li Metal
Lithium garnet (Li 7 La 3 Zr 2 O 12 , LLZO) based solid electrolytes are leading candidate materials for all-solid-state batteries with lithium metal anodes because of their high ionic conductivity, high mechanical toughness, and superior electrochemical stability. While doping LLZO with Al and Ga increases its ionic conductivity by stabilizing the cubic phase, the impact of dopants on its (electro)chemical stability at the interfaces with Li metal is critical. Here, our study of differences between Al- and Ga-doped LLZO when interfaced with lithium metal using X-ray photoelectron spectroscopy and density functional theory shows a higher propensity of Ga to move across LLZO interface with Li metal and form Ga-Li alloy. Additionally, neutron diffraction reveals loss of cubic phase resulting from the loss of dopant that explains electrochemical behavior differences between Ga- and Al-doped LLZO. Overall, our study reveals the key role of dopant chemistry in enabling stable solid electrolyte materials for all-solid-state batteries.
Klenk, Matthew↗
Unveiling the Role of Lithium Iodide in Stabilizing Solid Interfaces in All-Solid-State Li Metal Batteries
A critical challenge in all-solid-state lithium metal batteries (ASSLMBs) is achieving a stable interface between the lithium metal anode and the solid electrolyte. Leveraging its success in Li/I 2 batteries, lithium iodide has garnered significant attentions for its potential to enhance interfacial stability and overall cell performance in ASSLMBs. Here, we elucidate the role of lithium iodide in stabilizing the solid interface in all-solid-state Li metal batteries with a Li argyrodite electrolyte, particularly focusing on its influence on lithium deposition behavior and interfacial evolution. Through in situ optical imaging, we demonstrate more uniform lithium deposition on an iodide-contained argyrodite electrolyte compared to a chloride-based counterpart. Complementary density functional theory calculations attribute improved lithium plating behavior to the enhanced lithiophilicity and better ionic conductivity of lithium iodide at the solid interface, effectively reducing localized current density. In conclusion, these findings provide useful insights into the mechanisms through which lithium iodide enhances the interfacial stability in ASSLMBs.
Anions↗
Understanding LIB Battery Electrodes Through Classical Electrochemical Interface Theory
Classical models of the electrochemical interface can be applied to complex and dynamic electrodes to understand important mechanisms that are relevant to device-level phenomena like calendar aging or cycle life. Here, we show that negative alloy electrodes with wide electrochemical windows cannot be assumed to have static interfaces throughout all states of charge. Under high states of charge, the interface -including the solid electrolyte interphase - has characteristics that resemble a highly polarized electrode far from the point of zero charge. Under these conditions, the interface can be understood through the Helmholtz model. At lower states of charge, the interface capacitance decreases and the space charge layer length increases. This transformation resembles a metal electrode approaching the point of zero charge which is understood through the Gouy-Chapman-Stern-Grahame model of the electrochemical interface. This transformation happens at both silicon and carbon-coated silicon interfaces. From voltage-limited cycling experiments, in the limit of the diffuse double layer, the silicon electrode impedance rises significantly in the first few cycles. This rise is related to the continuous electrochemical reduction of electrolyte components from an interface that is not electronically screened from the electrolyte. In other words, an electrode interface for batteries should resemble a 'Helmholtz-like' structure.
anode↗
Soil microbial ecology and microbiome-metabolite linkages improve understanding of ecosystem states along terrestrial-aquatic interfaces
These data are from Bandopadhyay et al., "Soil microbial ecology and microbiome-metabolite linkages improve understanding of ecosystem states along terrestrial-aquatic interfaces". This study aims to understand the soil microbial ecology along terrestrial-aquatic interfaces of a freshwater and estuarine region and how it relates to organic matter. We analyzed soil microbial (16S rRNA gene) and organic matter (Fourier-transform ion cyclotron resonance mass spectrometry, FTICR-MS) composition from upland (forested), transition (stressed forest), and wetland positions at three sites in each of the Lake Erie (freshwater) and Chesapeake Bay (estuarine) regions. This dataset includes 16S rRNA gene amplicon data (only processed file types included here) and organic matter composition from FTICR-MS data (raw and processed files included here) from upland (forested), transition (stressed forest), and wetland positions at three sites in each of the Lake Erie and Chesapeake Bay regions. These sites are part of the COMPASS-FME project (https://compass.pnnl.gov/FME/COMPASSFME). File formats and software needed to access files: 16S rRNA gene amplicon data: These files follow the format reported here https://ess-dive.gitbook.io/amplicon-sequencing-reporting-format#updates-in-v1.0.1. As per this format, there are four file types reported: 1. Taxon tables (also called sequence-by-sample or OTU (operational taxonomic unit)/ESV (exact sequence variant) tables) : available in a .txt file format and accessible using TextEdit or MS Excel. 2. Representative sequences (also called consensus sequences) : available in a .fasta format and accessible using TextEdit. 3. Sequencing metadata : available in a MS Excel workbook file format and CSV file format 4. Bioinformatic metadata : available in a MS Excel workbook file format and CSV file format FTICR-MS data: 1. Raw data converted to a processed file with intensities of the peaks in the given samples : available in a MS Excel CSV file format 2. Processed file used in analyses and visualizations (appended as icr_long_) : available in a MS Excel CSV file format 3. Metadata file for ICR features (appended as icr_meta) : available in a MS Excel CSV file format
54 ENVIRONMENTAL SCIENCES↗
Cauchy integral method for two-dimensional solidification interface shapes
A method is developed to determine the shape of steady state solidification interfaces formed when liquid above its freezing point circulates over a cold surface. The solidification interface, which is at uniform temperature, will form in a shape such that the non-uniform energy convected to it is locally balanced by conduction into the solid. The interface shape is of interest relative to the crystal structure formed during solidification; regulating the crystal structure has application in casting naturally strengthened metallic composites. The results also pertain to phase-change energy storage devices, where the solidified configuration and overall heat transfer are needed. The analysis uses a conformal mapping technique to relate the desired interface coordinates to the components of the temperature gradient at the interface. These components are unknown because the interface shape is unknown. A Cauchy integral formulation provides a second relation involving the components, and a simultaneous solution yields the interface shape.
Siegel, R.↗
A Steady State and Quasi-Steady Interface Between the Generalized Fluid System Simulation Program and the SINDA/G Thermal Analysis Program
A general purpose, one dimensional fluid flow code is currently being interfaced with the thermal analysis program SINDA/G. The flow code, GFSSP, is capable of analyzing steady state and transient flow in a complex network. The flow code is capable of modeling several physical phenomena including compressibility effects, phase changes, body forces (such as gravity and centrifugal) and mixture thermodynamics for multiple species. The addition of GFSSP to SINDA/G provides a significant improvement in convective heat transfer modeling for SINDA/G. The interface development is conducted in multiple phases. This paper describes the first phase of the interface which allows for steady and quasisteady (unsteady solid, steady fluid) conjugate heat transfer modeling.
Schallhorn, Paul↗
Use of the Burton-prim-slichter Equation at High Growth Rates
The following must be assumed in order to derive the classic Burton-Prim-Slichter equation for segregation during crystal growth: isobaric, isothermal, isopotential or uncharged species, binary, planar interface, steady state, constant diffusion coefficient in fluid, no diffusion in crystal, no lateral convection within fluid film at interface with complete mixing beyond (stagnant film model), and either density, total concentration or partial molar volumes constant in the fluid phase. In addition, the effective distribution coefficient and the interfacial distribution coefficient must be defined properly. The velocity in the equation is the growth rate times a factor correcting for the difference in volumetric properties between crystal and fluid. The stagnant film thickness is found to be a function of freezing rate, with the precise functionality depending on the type of stirring occurring in the growth fluid.
Wilcox, W. R.↗
Interface Design for High‐Performance All‐Solid‐State Lithium Batteries
All‐solid‐state batteries suffer from high interface resistance and lithium dendrite growth leading to low Li plating/stripping Coulombic efficiency (CE) of <90% and low critical current density at high capacity. Here, in this work, both challenges are simultaneously addressed and the Li plating/stripping CE is significantly increased to 99.6% at 0.2 mA cm −2 /0.2 mAh cm −2 , and critical current density (CCD) of > 3.0 mA cm −2 /3.0 mAh cm −2 by inserting a mixed ionic‐electronic conductive (MIEC) and lithiophobic LiF‐C‐Li 3 N‐Bi nanocomposite interlayer between Li 6 PS 5 Cl electrolyte and Li anode. The highly lithiophobic LiF‐C‐Li 3 N‐Bi interlayer with high ionic conductivity (10 −5 S cm −1 ) and low electronic conductivity (3.4×10 −7 S cm −1 ) enables Li to plate on the current collector (CC) surface rather than on Li 6 PS 5 Cl surface avoiding Li 6 PS 5 Cl electrolyte reduction. During initial Li plating on CC, Li penetrates into porous LiF‐C‐Li 3 N‐Bi interlayer and lithiates Bi nanoparticles into Li 3 Bi. The lithiophilic Li 3 Bi and Li 3 N nanoparticles in LiF‐C‐Li 3 N‐Li 3 Bi sub‐interlayer will move to CC along with plated Li, forming LiF‐C/Li 3 N‐Li 3 Bi lithiophobic/lithiophilic sublayer during the following Li stripping. This interlayer enables Co 0.1 Fe 0.9 S 2 /Li 6 PS 5 Cl/Li cell with an areal capacity of 1.4 mAh cm −2 to achieve a cycle life of >850 cycles at 150 mA g −1 . The lithiophobic/lithiophilic interlayer enables solid‐state metal batteries to simultaneously achieve high energy and long cycle life.
25 ENERGY STORAGE↗
Ultrafast Terahertz Field Control of the Emergent Magnetic and Electronic Interactions at Oxide Interfaces
Ultrafast electric-field control of emergent electronic and magnetic states at oxide interfaces offers exciting prospects for the development of the next generation of energy-efficient devices. Here, it is demonstrated that the electronic structure and emergent ferromagnetic interfacial state in epitaxial LaNiO3/CaMnO3 superlattices can be effectively controlled using intense, single-cycle THz electric-field pulses. A suite of advanced X-ray spectroscopic techniques is employed to measure a detailed magneto-optical profile and the thickness of the ferromagnetic interfacial layer. Then, a combination of time-resolved and temperature-dependent optical measurements is used to disentangle several correlated electronic and magnetic processes driven by ultrafast, high-field THz pulses. Sub-picosecond non-equilibrium Joule heating of the electronic system is observed, ultrafast demagnetization of the ferromagnetic interfacial layer, and slower dynamics indicative of a change in the magnetic state of the superlattice due to the transfer of spin-angular momentum to the lattice. These findings suggest a promising avenue for the efficient control of 2D ferromagnetic states at oxide interfaces using ultrafast electric-field pulses.
X-ray spectroscopy and scattering↗
Novel Superionic Na Conductors for Solid‐State Na batteries: Materials and Interface
This project aims to advance the fundamental understanding on how the cation or anion doping influence on the crystal structure, phase stability and ion transport of novel Na superionic conductors. Specifically, we focus on the Na 3-x A x SbS 4-y X y family solid electrolytes (A: cation dopant, X: anion dopant), a class of promising materials for all-solid-state sodium batteries owing to their high ionic conductivity and compositional tunability. By integrating materials synthesis, neutron scattering, and electrochemical characterization and theoretical simulations, this project sees to elucidate 1) how does the synthesis approaches (solid-state reaction, low-temperature reaction) on the phase purity and doping process; 2) how chemical doping (A: cation dopants such as Sn; X: anion dopants such as Se, F) modulate lattice dynamics and Na+ migration as well as interface stability toward Na metal. Specifically, this project’s proposed technology involves three objectives: (1) synthesize novel Na-ion conductors (anion or cation doped Na 3 SbS 4 ) with high phase purity and examine their structural features (e.g., phase stability); (2) understand Na-ion conductive properties of new Na-ion conductors through a combination of experimental characterizations and theoretical simulations; (3) investigate the interface stability of novel Na superionic conductors with electrode materials in solid-state Na batteries. These objectives will be achieved through combined experimental synthesis/characterizations and computational approaches. The obtained knowledge will provide a comprehensive synthesis-structure-property correlation, enabling the rational design of novel solid-state conductors with excellent conductivity and stability.
25 ENERGY STORAGE↗