Type Of Solid Electrolyte Research Articles

Evaluation of Oxide|Sulfide Heteroionic Interface Stability for Developing Solid-State Batteries with a Lithium-Metal Electrode: The Case of LLZO|Li6PS5Cl and LLZO|Li7P3S11.

Developing solid-state batteries (SSB) with a lithium metal electrode (LME) using only one type of solid electrolyte (SE) is a significant challenge since no SE fits all the requirements imposed by both electrodes. A possible solution is using multilayer SSBs with an LME where the drawbacks of each SE are overcome by using layers of different SEs. However, research on inorganic SE1|SE2 heteroionic interfaces is still quite preliminary, especially regarding oxide|sulfide heteroionic interfaces. This work reports the electrochemical investigation of the heteroionic interface between Li6.25Al0.25La3Zr2O12 (Al-LLZO) and two representative materials for sulfide-based SEs: argyrodite-based Li6PS5Cl (LPSCl) and glass-like Li7P3S11 (LPS711). Through in-depth temperature- and pressure-dependent impedance analyses of multilayer symmetric cells at equilibrium (i.e., no current load), the electrical properties of the heteroionic interfaces are assessed. The pressure-dependent kinetic of the Al-LLZO|LPSCl pair is interpreted with the concept of geometric constriction resistance and show that its resistance is lower than for the Al-LLZO|LPS711 pair. Furthermore, the effect of Al-LLZO surface treatment on the electrical properties of the Al-LLZO|LPSCl heteroionic interface is evaluated. Such investigation shows that the value of the interface activation energy decreases when the Al-LLZO surface is heat treated, revealing a significant influence of the carbonate/hydroxide passivation layer on the heteroionic interface. Additionally, by cycling the symmetric cell for 900 h at 1.0 mAh·cm-2, it is revealed that the Al-LLZO|LPSCl interface has a lower impedance increase than the Al-LLZO|LPS711 interface, especially if the Al-LLZO is heat treated. With this work, we highlight that the oxide|argyrodite combination can be a promising candidate for multilayer SSBs with an LME. However, we show that an optimized LLZO surface treatment and chemical analysis of the interface are recommended for future research.

Investigating the Influence of Sintering Temperature and Ascertaining Hopping Path in Sodium Superionic Conducting Electrolytes for Sodium-Ion Batteries

Recently, sodium super-ionic conducting (NASICON) type solid electrolytes have gained significant interest as potential candidates for next-generation batteries due to their exceptional properties such as high ionic conductivity, affordability, and remarkable chemical and electrochemical stability. Therefore, NASICON type solid electrolyte (Na3Zr2Si2PO12) is synthesized by solution assisted-solid state reaction (SA-SSR) method and sintered at three different temperatures, 1200 ℃, 1250 ℃ and 1300 ℃. Various experimental techniques are used to characterize and optimize the sintered electrolytes. The Rietveld refinement of X-ray diffraction pattern of prepared electrolytes revealed the monoclinic crystal structure having 3-dimension hopping channel for sodium ion migration through triangular bottleneck area. Complex impedance spectroscopy revealed, the highest bulk and grain boundary conductivity are found, 4.05 mS cm-1 and 0.31 mS cm-1, respectively, for the sample sintered at 1250 ℃. Using optimized electrolyte, sodium half-cell is demonstrated with Na3V2P3O12 (NVP) as cathode. The assembled cell delivers maximum discharge capacity 101.6 and 84.45 mAh g-1 at the current density 10 and 40 mA g-1, respectively with good capacity retention (~95.02%) upto 50 cycles. Figure 1

Structure and ionic conductivity of NASICON-type LATP solid electrolyte synthesized by the solid-state method

The area of commercial battery innovation to replace safer batteries in widely used secondary batteries offers promising research into solid-state electrolytes (SSEs). Compared to lithium-ion electrolytes, solid-state electrolytes are inherently safer because they replace solvents with non-flammable materials. One of the promising materials for electrolytes today is based on inorganic materials, especially ceramics. Ceramics with superior mechanical, chemical and electrochemical stability and stability against high temperatures are of great interest. NASICON structured Li1.3 Al0.3 Ti1.7 (PO4)3 (LATP) is the most studied type of solid electrolyte due to its stability against air and humidity and high ionic conductivity.In this study, LATP samples were synthesized by solid-state synthesis method. The structural, morphological and charge transport properties (ionic conductivities) of the synthesized samples were characterized by X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM) and electrochemical impedance spectroscopy (EIS). Since the modifications applied during the sample preparation process can change the crystal structure and size of the target material, in this study, in order to minimize the formation of impurity phases and to achieve high ionic conductivity it was applied the different synthesis steps (temperature, time, grinding speed, etc.) from the literature. While the ionic conductivity value obtained is among the best values obtained by LATP synthesis methods in the literature, it is the best ionic conductivity value (1.3 × 10−3 S cm−1) obtained by the solid state synthesis method.

Merits and Demerits of Machine Learning of Ferroelectric, Flexoelectric, and Electrolytic Properties of Ceramic Materials.

In the present review, the merits and demerits of machine learning (ML) in materials science are discussed, compared with first principles calculations (PDE (partial differential equations) model) and physical or phenomenological ODE (ordinary differential equations) model calculations. ML is basically a fitting procedure of pre-existing (experimental) data as a function of various factors called descriptors. If excellent descriptors can be selected and the training data contain negligible error, the predictive power of a ML model is relatively high. However, it is currently very difficult for a ML model to predict experimental results beyond the parameter space of the training experimental data. For example, it is pointed out that all-dislocation-ceramics, which could be a new type of solid electrolyte filled with appropriate dislocations for high ionic conductivity without dendrite formation, could not be predicted by ML. The merits and demerits of first principles calculations and physical or phenomenological ODE model calculations are also discussed with some examples of the flexoelectric effect, dielectric constant, and ionic conductivity in solid electrolytes.

Improved interfacial stability of all-solid-state batteries using cation-anion co-doped glass electrolytes

The electrochemical performance of all-solid-state batteries needs to be improved by addressing the poor stability against the lithium metal anode and the high interfacial resistance at the cathode–solid electrolyte interface. Here, metal halide-doped Li7P2S8I–type (LPSI) solid electrolytes are synthesized that improve the electrochemical performance of all-solid-state batteries. The solid electrolytes exhibit a higher ionic conductivity value of 7.77 mS cm−1 than bare LPSI solid electrolytes of 3.96 mS cm−1, at room temperature. The metal halide-doped LPSI solid electrolyte is also stable against the lithium metal anode, with a calculated critical current density value of 1 mA cm−2. The fabricated all-solid-state battery shows high electrochemical performance with 99.2% specific capacity retention after 250 cycles at a 0.5 C rate. The results of post galvanostatic charge–discharge analysis confirms that the proposed metal halide-doped LPSI solid electrolyte exhibits improved interfacial stability compared to bare LPSI solid electrolytes.

Temperature Impact on Lithium Metal Morphology in Lithium Reservoir-Free Solid-State Batteries

Lithium reservoir-free solid-state batteries can offer exceedingly high energy densities for a range of emerging applications related to aviation and electric vehicles. However, reversible operation of reservoir-free cells is plagued by a range of degradation mechanisms. The morphology of lithium metal film and subsequent evolution during operation can be highly variable and is dependent on the type of solid electrolyte, current collector, and operating conditions (current density, temperature, pressure, etc.). Here we evaluate lithium metal vertical and horizontal growth mechanisms at an argyrodite solid electrolyte–stainless steel interface at various temperatures from 25 to 80∘C. Combining confocal imaging and mesoscale modeling, we demonstrate how lithium metal island agglomeration is accelerated at elevated temperatures and facilitates greater horizontal growth of lithium metal. Maintaining high active material contact (e.g., horizontal growth) is critical for the formation of reversible lithium metal anodes in reservoir-free cells. Published by the American Physical Society 2024

Influence of mixing technique on properties of Li1.3Al0.3Ti1.7(PO4)3 solid electrolyte prepared by the solid-state reaction - A comparison of dry 3D mixing technique with wet ball-milling

Li1.3Al0.3Ti1.7(PO4)3 (LATP) NASICON(Na Super Ion Conductive)-type solid electrolyte is prepared using conventional wet ball-milling and dry 3D mixing techniques to investigate the influence of mixing technique on properties of LATP. The mixing techniques influence impurity formation of calcined LATP powder. Thus, sintering behavior of the calcined powders is also affected by the mixing technique, i.e. LiTiPO5 formation is confirmed in the ball-milling samples and Li-ion conductive Li4P2O7 is main impurity in the 3D mixing samples. The influence is not limited to impurity formation. Uniform grains are observed in the 3D mixing pellet, contrarily, non-uniform sintering occurs in the ball-milling sample. As a result, the 3D mixing pellets demonstrate higher Li-ion conductivity than the ball-mill samples. The dry 3D mixing technique, which can omit drying process, is promising for LATP preparation owing to simplification of preparation process and a formation of high Li-ion conductive LATP pellets. Also, this study clearly shows that the mixing techniques affect ionic conductivity of the sintered LATP significantly, emphasizing importance of mixing procedure in the solid-state reaction.

Round‐robin test of all‐solid‐state battery with sulfide electrolyte assembly in coin‐type cell configuration

AbstractThe replacement of conventional lithium‐ion batteries with solid‐state batteries is currently under investigation by many players both from academia and industry. Sulfide‐based electrolytes are among the materials that are regarded as most promising, especially for application in the transport sector. The performance of anode, cathode, and solid electrolyte materials of this type of solid electrolyte is typically evaluated using manually assembled cells such as Swagelok cells, EL‐CELLs, and in‐house built pressure devices. Coin cells, however, are often disregarded. Though coin cells cannot accurately predict how a material will perform in an end‐use application battery cell format, they are easy to assemble and can provide reproducible data compared to the other cell types, which make them an interesting option for testing the materials under conditions more relevant for their envisioned application. The coin cell preparation method presented in this work has been evaluated interlaboratory for reproducibility and, in addition, can be modified depending on the optimization parameters of the solid electrolyte, cathode material, bilayer comprised on cathode and solid electrolyte, lithium metal anode, and cell in general. Besides, an interlab round‐robin test (RRT) is carried out between four laboratories, measuring defined electrochemical tests of sulfide solid‐state batteries in coin cell configuration. This RRT for the preparation of coin cell solid‐state batteries with sulfide solid electrolyte, lithium nickel manganese cobalt oxides cathode, and lithium metal anode is intended for academic researchers and provides guidelines of research in this field.

Effect of partial substitution of Ta2O5 by ZrO2 on the structure and ionic conductivity of Li2O-Ta2O5-2 SiO2 glass and glass-ceramics

LiTaSiO5 system is considered as type of solid electrolyte with great potential for application as ionic conductor. It is well-known that it is difficult to obtain pure dense LiTaSiO5 phase by traditional synthesis methods, because dielectric LiTaO3 phase easily precipitates during synthesis, which affects ionic conductivity. In this work, a glass-ceramic electrolyte with main LiTaSiO5 phase was obtained by controlled crystallization of Li2OTa 2O5-2 SiO2 glass without porosity. The precipitation of LiTaO3 phase at the grain boundary was effectively inhibited by adding an appropriate amount of ZrO2. Among all the glass-ceramic samples, the glass containing 4.76mol% ZrO2 had the maximum ionic conductivity of 8.40 ? 10?6 S/cm at 25?C, which is two order of magnitude greater than the ionic conductivity of the matrix glass. These glass-ceramic samples have the potential to be used as solid electrolytes in electrochemical applications.

(Invited) Electrolytes for Next-Generation Sodium Metal Batteries

Developing reliable and cost-effective electrical energy storage systems (EESs) for portable electronics, electric vehicles, and grid storage applications is vital. Na-ion batteries are the most promising alternative technology owing to their natural abundance and low sodium cost.[1] Solid-state batteries (SSBs) have garnered extensive attention for their ability to suppress the safety hazards of organic liquid electrolytes by replacing them with solid electrolytes.[2] Among the various solid electrolytes being explored, our group mainly focuses on NASICON (Sodium superionic conductor) type silicate and solid polymer electrolytes. Sodium silicates are a class of materials with composition, NaxMxSixOx (M = rare-earth metals, x = integer (1-10)).[3] They have the advantage of low sintering temperature (~1050 °C) and 3D framework structure containing MO6 octahedra and SiO4 tetrahedra providing facile ionic movement.[4] Solid polymer electrolytes (SPE) are known for their flexibility and electrode compatibility. Highly conductive, filler-free composite solid polymer electrolyte films were prepared using poly(vinylidene fluoride), poly(vinyl pyrrolidone) (PVP), and NaPF6.[5] PVP binder played an essential role in improving Na ion conductivity and excellent plating−stripping performance. This talk will present an overview of these solid electrolytes for next-generation sodium metal batteries.

Organic Modification of Silica-Based Ionogels Improves the Electrolyte/Electrode Contact and Influences Their Functional Properties

The energy transition necessitates sustainable energy storage to address the mismatch between the production and consumption of renewable electricity. Sodium-ion batteries (SIBs) are a promising candidate for stationary energy storage as an alternative for lithium-ion batteries (LIBs). In spite of their lower energy density, SIBs have advantages over LIBs.1 Sodium is considerably more abundant than lithium (2.83% versus 0.01%) and, evenly distributed across the Earth, implying that SIBs may be less expensive and more sustainable than LIBs.1,2 Conventional LIBs contain flammable organic liquid electrolytes (e.g. alkyl carbonates) with limited thermal stability. Thermal runaway can therefore lead to cell ignition, causing a significant safety hazard. Non-flammable electrolytes can be based on ionic liquids, which are molten salts with flame retarding properties and negligible vapor pressures. However, the possibility of leakage and related environmental hazards remains a concern.3 This risk can be mitigated by the use of solid electrolytes. Apart from circumventing safety issues, solid electrolytes may allow a significant increase in energy density. After all, they take up less dead volume than liquid electrolytes and can allow the use of alkali metals as negative electrodes.An attractive type of solid electrolyte is the class of silica-based ionogels, owing to their high ionic conductivity, thermal stability, and broad electrochemical window.4 They comprise an ionic liquid electrolyte (ILE, a salt dissolved in ionic liquid) confined in the pores of a solid silica matrix. The silica matrix is electrochemically inactive but influences the functional properties of the resulting solid material. Ionogels based on solely silica (SiO2) as matrix tend to crack easily when subjected to pressure as the rigid Si-O-Si bonds result in high Young’s modulus materials. Furthermore, materials with high Young’s moduli cannot adapt easily to electrode surfaces, resulting in higher charge-transfer resistances (Rct) between the solid electrolyte and electrode. One way to reduce the stiffness of silica-based ionogels is to modify the silica matrix with e.g. organic groups. Ormosils® are a class of materials completely consisting of organically modified silica and show mechanical properties from glassy to rubbery depending on the amount of organic modification.5 Here, the concepts of ionogels and Ormosils® are combined to produce sodium-ion conducting organically modified ionogels. Two different phenyl-bearing silanes (phenyltrimethoxysilane, PhTMS, or diphenyldimethoxysilane, DPhDMS) are for the first time used as organic modifiers in silica-based ionogels. A non-aqueous sol-gel route with formic acid (FA) is used to synthesize the monoliths. Incorporating phenyl groups allow to reduce the Young’s modulus from 29 MPa down to 6 MPa. The charge-transfer resistances (Rct) of Na|ionogel|Na2Ti3O7 half cells, determined with electrochemical impedance spectroscopy (EIS), followed the trend of the ionogels’ Young’s modulus. Through NMR spectroscopy, pi-stacking was observed between the matrix phenyl moieties and IL imidazolium cations. Furthermore, the organic modification diminished the formation of hydrogen bonds between IL anions and matrix silanol groups. This shows that the organic modification of the matrix can have a pronounced effect on the coordination of the ILE components, which ultimately determine the solid electrolyte’s functional properties. In summary, incorporating phenyl groups in the silica matrix of ionogels improves the mechanical properties and charge transfer resistances, but impairs ionic conductivity. Acknowledgments: This research is made possible by the Research Foundation Flanders (FWO, project G053519N and 1S08921N) and the Special Research Fund (BOF) of Hasselt University (BOF20INCENT19). This work is further supported by Hasselt University and FWO Vlaanderen via the Hercules project AUHL/15/2 - GOH3816N.

Atomic-Resolution Electron Microscopy Unravelling the Role of Unusual Asymmetric Twin Boundaries in the Electron-Beam-Sensitive NASICON-Type Solid Electrolyte.

An atomic-scale understanding of the role of nonperiodic features is essential to the rational design of highly Li-ion-conductive solid electrolytes. Unfortunately, most solid electrolytes are easily damaged by the intense electron beam needed for atomic-resolution electron microscopy observation, so the reported in-depth atomic-scale studies are limited to Li0.33La0.56TiO3- and Li7La3Zr2O12-based materials. Here, we observe on an atomic scale a third type of solid electrolyte, Li1.3Al0.3Ti1.7(PO4)3 (LATP), through minimization of damage induced by specimen preparation. With this capability, LATP is found to contain large amounts of twin boundaries with an unusual asymmetric atomic configuration. On the basis of the experimentally determined structure, the theoretical calculations suggest that such asymmetric twin boundaries may considerably promote Li-ion transport. This discovery identifies a new entry point for optimizing ionic conductivity, and the method presented here will also greatly benefit the mechanistic study of solid electrolytes.

Viscoelastic inorganic glass as solid-state electrolyte for batteries

A most recent exciting research result in the area of solid-state batteries that has been accepted for publication by the journal Nature Energy is highlighted. The research designed a new type of inorganic solid electrolyte named “viscoelastic inorganic glass (VIGLAS)” electrolyte with the compositions of LiAlCl2.5O0.75 and NaAlCl2.5O0.75. The newly developed solid electrolyte material showcases an exceptional degree of deformability at room temperature, high ionic conductivity (>1 mS/cm at room temperature) and high oxidation stability (up to 4.3 V vs. Li+/Li or Na+/Na). Using it as a catholyte enables a facile fabrication and a stable operation under practical stack pressure (＜0.1 MPa) of all-solid-state batteries. VIGLAS represents a new path in the design of promising solid electrolytes for realizing high performance all-solid-state batteries.

The study of ionic conductivity of the Li10GeP2S12 type Solid State Electrolyte by an extrapolation method and a deep-learning method

An extrapolation method is usually applied when Ab initio molecular dynamics (AIMD) is applied to studying ionic conductivity in solid-state electrolytes in lithium-ion batteries. As the ions move slowly in solid-state electrolytes, the first-principles method typically involves computationally intensive calculations, and it can take significant time to obtain accurate results. First-principles method is too expensive for the time scale required at room temperature. The classical molecular dynamics method is typically applied to systems containing thousands of atoms and can simulate the system’s behavior over nanoseconds. During the simulation, the positions and velocities of the atoms are updated at discrete time intervals, allowing the system’s behavior to be studied over time. However, its accuracy depends on the empirical force-field libraries. Limited by the computational resource, the previous studies applied the extrapolation method to obtain the room temperature ionic conductivity, which was not accurate because the linear relationship in the Arrhenius equation was not valid in a wide range of temperatures. Deepmd-Kit is a tool that integrates these two different computational approaches. The extrapolation and Deepmd methods were applied to the materials Li10GeP2S12, Li10SiP2S12, Li10GePS12Cl, and Li10SiPS12Cl, respectively. Both methods showed that the lithium ions favor the c direction when diffusing in the LGPS-type solid-state electrolytes. The ionic conductivity is more accurate with the dependent method compared with experiments.

Impact of sintering temperature and ascertaining hopping bottlenecks for ions in sodium superionic conducting electrolyte for sodium-ion batteries

Recently, sodium super-ionic conducting (NASICON) type solid electrolytes have gained attention for next generation batteries because of their high ionic conductivity, low cost, excellent chemical and electrochemical stability. Therefore, in the present study, NASICON-type solid electrolyte Na3Zr2Si2PO12 is synthesized by solution assisted-solid state reaction (SA-SSR) route. The electrolytes are sintered at three different temperatures, 1200 °C, 1250 °C and 1300 °C. The sintered electrolytes are characterized by various experimental techniques. The Rietveld refinement of X-ray diffraction pattern of prepared electrolytes revealed the monoclinic crystal structure. The 3-dimension hopping channel for sodium ion migration through triangular bottleneck area is identified. From complex impedance spectroscopy measurement, the highest bulk and grain boundary conductivity are found, ∼4.05mScm−1 and ∼0.31mScm−1, respectively, for the sample sintered at 1250 °C. The optimized electrolyte shows wide electrochemical stability (∼6.5 V) which is suitable for high voltage battery application. Using optimized electrolyte, sodium half-cell is fabricated with sodium metal as anode, and Na3V2P3O12 (NVP) as cathode. The assembled cell delivers maximum discharge capacity ∼101.6 and ∼84.5mAhg−1 at the current density 10 and 40mAg−1, respectively with good capacity retention (∼95.02%) upto 50 cycles.

Progress in Sodium Silicates for All‐Solid‐State Sodium Batteries—a Review

All solid‐state sodium batteries (ASSSBs) are considered a promising alternative to lithium‐ion batteries due to increased safety in employing solid‐state components and the widespread availability and low cost of sodium. As one of the indispensable components in the battery system, organic liquid electrolytes are the currently used electrolytes due to their high‐ionic conductivity (10−2 S cm−1) and good wettability; however, their low‐thermal stability, flammability, and leakage tendency pose safety concerns. The growing sodium‐ion battery technology with solid electrolytes is a viable solution due to their improved safety. However, solid electrolytes suffer from insufficient ionic conductivity at room temperature (10−4–10−3 S cm−1), poor interface stability, high charge‐transfer resistance, and low wettability, yielding inferior battery performance. Sodium rare‐earth silicates are a new class of materials with a 3D structure framework similar to sodium‐superionic conductors (NASICONs). These silicates can be used as a solid electrolyte for solid‐state sodium batteries due to their high‐ionic conduction (10−3 S cm−1) at 25 °C. Herein, the sodium rare‐earth silicate synthesis, crystal structure, ion‐conduction mechanism, doping, and electrochemical properties are discussed. This emerging type of inorganic solid electrolyte can pave the way to building next‐generation ASSSBs.

Inorganic–organic hybrid solid electrolytes in the tetramethylammonium iodide–LiI–Li2S–P2S5 system for all-solid-state lithium batteries

A new type of glassy solid electrolyte was prepared by doping tetramethylammonium iodide (TMAI) in Li7P2S8I. TMAI can suppress the large volume change of a Si electrode during cycling.

The Application of Deep Learning on Room Temperature Conductivity of Li10GeP2S12 Type Solid State Electrolyte

Room temperature ionic conductivity of the solid-state electrolyte is the essencial element of the commercialization of solid-state lithium-ion batteries. First-principles method is a good tool as it simulates the atomic level dynamics, and provides accurate insides of the ion moving velocity, path, and the microscopic environment. However, the first-principles method is time and computational resources-consuming. It is usually applied to systems with hundreds of atoms and the simulation time is less than 100 picoseconds. The classical molecular dynamics method applies to systems containing thousands of atoms and the simulation time can reach the scale of nanoseconds. However, it is based on the experimental force-field parameters and can only be applied to limited systems with experimentally-proofed good parameters. The method used in this paper is a combination of the first-principles simulation and classical dynamics. Deep-learning tool Deepmd-kit is used to train the first-principles simulation data of the targeted system into a tailor-made force-field model. The verified model for the specific system will then be used in the classical molecular dynamics simulation. With the first-principles precise and classical efficiency, the molecular dynamics simulation of ion movement at room temperature is achieved. The results of Li10GeP2S12 and Li10SiP2S12 showed good agreement with the experiments.

Silver Doped Lithium Metal Thin Films for Solid-State Batteries

Potential use of lithium metal anode is a primary factor behind the high-energy density promise of solid-state batteries. However, large anodic loads lead to void formation and contact loss at the lithium/solid electrolyte interface which, in turn, lead to much higher effective local current densities during the subsequent lithium plating, causing dendrite formation and cell shorting.1, 2 This is due to the slow self-diffusion of Li atoms/vacancies, which is an inherent limitation of lithium metal.3 Modifying the bulk physiochemical properties of lithium metal via doping/alloying (<10 at% dopant) is an attractive approach, as such a small concentration of dopants can alter lithium metal’s bulk properties, without lowering its energy density. As an example, pore formation was effectively eliminated by alloying Li with 10 at% Mg, although chemical diffusion of Li within the alloy still restricted its rate performance.4 In this work, we report the effects of Ag as a dopant on the morphological stability and rate capability of Li-Ag alloy anodes during electrochemical cycling, as its concentration is varied in Li from 0-10 at.%. The alloy samples are prepared as 10 μm thick films, a practical form factor for solid-state batteries, via a combination of sputtering and thermal evaporation. Comparison of performance as a function of Ag content will be presented for both polymeric and inorganic solid-state electrolytes. Structural characterization of the alloy anodes via complementary techniques will also be presented. This research was sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL). This abstract has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). References Kasemchainan, J.; Zekoll, S.; Spencer Jolly, D.; Ning, Z.; Hartley, G. O.; Marrow, J.; Bruce, P. G., Critical stripping current leads to dendrite formation on plating in lithium anode solid electrolyte cells. Nature Materials 2019, 18 (10), 1105-1111.Krauskopf, T.; Hartmann, H.; Zeier, W. G.; Janek, J., Toward a Fundamental Understanding of the Lithium Metal Anode in Solid-State Batteries—An Electrochemo-Mechanical Study on the Garnet-Type Solid Electrolyte Li6.25Al0.25La3Zr2O12. ACS Applied Materials & Interfaces 2019, 11 (15), 14463-14477.Jow, T. R.; Liang, C. C., Interface Between Solid Electrode and Solid Electrolyte—A Study of the Li / LiI ( Al2 O 3 ) Solid‐Electrolyte System. Journal of The Electrochemical Society 1983, 130 (4), 737-740.Krauskopf, T.; Mogwitz, B.; Rosenbach, C.; Zeier, W. G.; Janek, J., Diffusion Limitation of Lithium Metal and Li–Mg Alloy Anodes on LLZO Type Solid Electrolytes as a Function of Temperature and Pressure. Advanced Energy Materials 2019, 9 (44), 1902568.

Differences in the Interfacial Mechanical Properties of Thiophosphate and Argyrodite Solid Electrolytes and Their Composites.

Interfacial mechanics are a significant contributor to the performance and degradation of solid-state batteries. Spatially resolved measurements of interfacial properties are extremely important to effectively model and understand the electrochemical behavior. Herein, we report the interfacial properties of thiophosphate (Li3PS4)- and argyrodite (Li6PS5Cl)-type solid electrolytes. Using atomic force microscopy, we showcase the differences in the surface morphology as well as adhesion of these materials. We also investigate solvent-less processing of hybrid electrolytes using UV-assisted curing. Physical, chemical, and structural characterizations of the materials highlight the differences in the surface morphology, chemical makeup, and distribution of the inorganic phases between the argyrodite and thiophosphate solid electrolytes.