Journal articles on the topic 'Solid state electrolyte'
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1
Liu, Liyu, Kai Chen, Liguo Zhang, and Bong-Ki Ryu. "Prospects of Sulfide-Based Solid-State Electrolytes Modified by Organic Thin Films." International Journal of Energy Research 2023 (February 6, 2023): 1–7. http://dx.doi.org/10.1155/2023/2601098.
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Lithium-ion batteries are key to tackling today’s energy crisis. In recent years, compared with the research on other components of lithium-ion batteries, the research on solid-state electrolytes is particularly hot. Among various solid-state electrolyte modification measures, we found that the material design of organic/inorganic composite flexible solid-state electrolytes can achieve the best all-solid-state battery cycling performance. Based on the study of sulfide-based organic/inorganic composite solid-state electrolytes, this article firstly introduces the classification of inorganic solid electrolytes and the advantages and disadvantages of each type of materials. At the same time, the research progress of various oxide solid electrolyte materials and sulfide solid electrolyte materials in recent years is introduced as well as the advantages of organic/inorganic composite solid-state electrolyte materials. Then the influencing factors that affect the performance of solid-state electrolytes, such as material lattice, lattice defects, electrolyte interface problems, and electrolyte microcracks, are introduced. Finally, the superiority of the industrial electrochemical performance of the organic/inorganic composite solid electrolyte material and its future prospects are introduced.
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Carmona, Eric A., and Paul Albertus. "Solid-State Electrolyte Fracture in Lithium Metal Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 396. http://dx.doi.org/10.1149/ma2022-024396mtgabs.
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Next generation batteries utilizing solid-state electrolytes to enable use of lithium metal electrodes are of significant interest due to increased energy density and the potential safety enhancements. Despite their high yield strength, high room temperature ionic conductivity, and lack of reactivity with metallic lithium, these ceramic solid electrolytes are still prone to dendrite formation and subsequent cell failure above critical current densities. One experimentally observed dendrite formation and propagation mechanism requires mechanical failure of the electrolyte via fracture. Ceramic solid electrolyte’s do not undergo ductile deformation, leaving fracture as the primary means of stress relaxation. The electrolyte’s propensity to fracture is dependent on its material properties (i.e. fracture toughness), electrode mechanical properties, and the cell operating conditions (e.g. applied current density, stack pressure, temperature). This talk will focus on electrochemical-mechanical coupling (including thermodynamic and kinetic couplings of mechanical forces with electrochemical behavior) and the relationship between the current distribution, developed stresses, and solid-electrolyte fracture initiation at Li protrusions. The effect of current focusing on stress-driven fracture, plastic deformation of lithium, and the influence of mechanical boundary conditions will be described.
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Bhardwaj, Ravindra Kumar, and David Zitoun. "Recent Progress in Solid Electrolytes for All-Solid-State Metal(Li/Na)–Sulfur Batteries." Batteries 9, no. 2 (February 3, 2023): 110. http://dx.doi.org/10.3390/batteries9020110.
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Metal–sulfur batteries, especially lithium/sodium–sulfur (Li/Na-S) batteries, have attracted widespread attention for large-scale energy application due to their superior theoretical energy density, low cost of sulfur compared to conventional lithium-ion battery (LIBs) cathodes and environmental sustainability. Despite these advantages, metal–sulfur batteries face many fundamental challenges which have put them on the back foot. The use of ether-based liquid electrolyte has brought metal–sulfur batteries to a critical stage by causing intermediate polysulfide dissolution which results in poor cycling life and safety concerns. Replacement of the ether-based liquid electrolyte by a solid electrolyte (SEs) has overcome these challenges to a large extent. This review describes the recent development and progress of solid electrolytes for all-solid-state Li/Na-S batteries. This article begins with a basic introduction to metal–sulfur batteries and explains their challenges. We will discuss the drawbacks of the using liquid organic electrolytes and the advantages of replacing liquid electrolytes with solid electrolytes. This article will also explain the fundamental requirements of solid electrolytes in meeting the practical applications of all solid-state metal–sulfur batteries, as well as the electrode–electrolyte interfaces of all solid-state Li/Na-S batteries.
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Kim, A.-yeon, Hun-Gi Jung, Hyeon-Ji Shin, and Jun tae Kim. "Binderless Sheet-Type Oxide-Sulfide Composite Solid Electrolyte for All-Solid-State Batteries." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 745. http://dx.doi.org/10.1149/ma2023-024745mtgabs.
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Lithium-ion batteries have been used as energy sources not only for small electronic devices but also for high-capacity and high-energy-density applications such as electric vehicles. However, the use of flammable organic liquid electrolytes in lithium-ion batteries has raised safety concerns in various applications. Therefore, solid-state batteries using flame-retardant inorganic materials are considered a more reasonable direction for future energy sources due to their high safety and high energy density. Solid electrolytes(SEs) are divided into oxide-based, sulfide-based, and polymer-based. Each solid electrolyte has its own advantages and disadvantages. Oxide-based solid electrolytes (e.g., Li7La3Zr2O12 (LLZO), Li3xLa2/3-xTiO3 (LLTO), Li1.3Al0.3Ti1.7(PO4)3 (LATP)) are air-stable and exhibit excellent electrochemical properties over a wide potential range. However, their high interfacial resistance may limit their practical application as batteries. Sulfide-based solid electrolytes (e.g., Li6PS5X (X=Cl, Br, I), Li10GeP2S12, (100-x)Li2S-xP2S5)) have high ionic conductivity, ductile properties, low interfacial resistance, and good room temperature workability. However, they are vulnerable to atmospheric instability, which can produce toxic gases such as H2S, and are relatively electrochemically unstable with Li metal. Polymer-based solid electrolytes, such as those made from polymers like PEO, PVDF, PAN, etc. that are compounded with other solid electrolytes (oxides, sulfides, etc.), offer the advantage of being able to form solid electrolyte membranes over large areas. But they have low ionic conductivity and weak mechanical properties of the polymer itself, limiting their practical application. To apply solid-state batteries to practical high-energy density energy storage devices such as electric vehicles, high ion conductivity, electrochemical stability, high mechanical properties, and large area formation of the electrolyte layer are essential. Solid electrolytes are mainly formed in powder form, and without a polymer binder, it is limited to apply as a film for large-capacity storage devices. Here, we fabricated a freestanding sheet-type Al-LLZO oxide-based solid electrolyte that forms a 3D network without a polymer material using an electrospinning method. In addition, we prepared a oxide-sulfide composite solid electrolyte membrane by impregnating LPSCl sulfide-based solid electrolyte into the Al-LLZO solid electrolyte sheet. As a result, This process removed the polymer and improved both the ionic conductivity and mechanical properties. Furthermore, it was possible to achieve both large-area and film characteristics without the need for a polymer.
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Won, Eun-Seo, and Jong-Won Lee. "Biphasic Solid Electrolytes with Homogeneous Li-Ion Transport Pathway Enabled By Metal-Organic Frameworks." ECS Meeting Abstracts MA2022-01, no. 55 (July 7, 2022): 2248. http://dx.doi.org/10.1149/ma2022-01552248mtgabs.
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Solid-state batteries based on nonflammable inorganic solid electrolytes provide a promising technical solution that can resolve the safety issues of current lithium-ion batteries. Biphasic solid electrolytes comprising Li7La3Zr2O12 (LLZO) garnet and polymer have been attracting significant interest for solid-state Li batteries because of their mechanical robustness and enhanced Li+ conductivity, compared to conventional polymer electrolytes. Furthermore, the hybridization allows for the fabrication of thin and large-area electrolyte membranes without the need for high-temperature sintering of LLZO. However, the non-uniform distribution of LLZO particles and polymer species in biphasic electrolytes may cause uneven Li+ conduction, which results in poor interfacial stability with electrodes during repeated charge–discharge cycling. In this study, we report a biphasic solid electrolyte with homogeneous Li+ transport pathway achieved by a metal–organic framework (MOF) layer. To regulate and homogenize the Li+ flux across the interface between the electrolyte and electrode, a free-standing, biphasic solid electrolyte membrane is integrated with the MOF nanoparticle layer. A mixture of plastic crystal (PC) and polymeric phase is infused into porous networks of the MOF-integrated electrolyte membrane, producing the percolating Li+ conduction pathways. The MOF-integrated electrolyte membrane is found to form the smooth and uniform interface with nanoporous channels in contact with the electrodes, effectively facilitating homogeneous Li+ transport. A solid-state battery with the MOF-integrated electrolyte membrane shows the enhanced rate-capability and cycling stability in comparison to the battery with the unmodified biphasic electrolyte. This study demonstrates that the proposed electrolyte design provides an effective approach to improving the interfacial stability of biphasic electrolytes with electrodes for long-cycling solid-state batteries. [1] H.-S. Shin, W. Jeong, M.-H. Ryu, S.W. Lee, K.-N. Jung, J.-W. Lee, Electrode-to-electrode monolithic integration for high-voltage bipolar solid-state batteries based on plastic-crystal polymer electrolyte, Chem. Eng. J, published online. [2] T. Jiang, P. He, G. Wang, Y. Shen, C.-W. Nan, L.-Z. Fan, Solvent-free synthesis of thin, flexible, nonflammable garnet-based composite solid electrolyte for all-solid-state lithium batteries, Adv. Energy Mater. 10 (2020) 1903376.
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Tron, Artur, Andrea Paolella, and Alexander Beutl. "New Insights of Infiltration Process of Argyrodite Li6PS5Cl Solid Electrolyte into Conventional Lithium-Ion Electrodes for Solid-State Batteries." Batteries 9, no. 10 (October 4, 2023): 503. http://dx.doi.org/10.3390/batteries9100503.
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All-solid-state lithium-ion batteries based on solid electrolytes are attractive for electric applications due to their potential high energy density and safety. The sulfide solid electrolyte (e.g., argyrodite) shows a high ionic conductivity (10−3 S cm−1). There is an open question related to the sulfide electrode’s fabrication by simply infiltrating methods applied for conventional lithium-ion battery electrodes via homogeneous solid electrolyte solutions, the structure of electrolytes after drying, chemical stability of binders and electrolyte, the surface morphology of electrolyte, and the deepening of the infiltrated electrolyte into the active materials to provide better contact between the active material and electrolyte and favorable lithium ionic conduction. However, due to the high reactivity of sulfide-based solid electrolytes, unwanted side reactions between sulfide electrolytes and polar solvents may occur. In this work, we explore the chemical and electrochemical properties of the argyrodite-based film produced by infiltration mode by combining electrochemical and structural characterizations.
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Cai, Jinhai, Yingjie Liu, Yingying Tan, Wanying Chang, Jingyi Wu, Tong Wu, and Chunyan Lai. "Constructing Enhanced Composite Solid-State Electrolytes with Sb/Nb Co-Doped LLZO and PVDF-HFP." Applied Sciences 14, no. 7 (April 8, 2024): 3115. http://dx.doi.org/10.3390/app14073115.
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Composite solid-state electrolytes are viewed as promising materials for solid-state lithium-ion batteries due to their combined advantages of inorganic solid-state electrolytes and solid-state polymer electrolytes. In this study, the solid electrolytes Li6.7−xLa3Zr1.7−xSb0.3NbxO12 (LLZSNO) with Sb and Nb co-doping were prepared by a high-temperature solid-phase method. Results indicate that Sb/Nb co-doping causes lattice deformation in LLZO and increases the lithium vacancy concentration and conductivity of LLZO. Then, with the co-doped LLZSNO as an inorganic filler, a composite solid electrolyte of polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) was prepared with a casting method. The obtained composite solid electrolyte exhibits a high ionic conductivity of 1.76 × 10−4 S/cm at room temperature, a wide electrochemical stable window of 5.2 V, and a lithium-ion transfer number of 0.32. The Li|LiFePO4 coin battery with the composite solid electrolyte shows a high specific capacity of 161.2 mAh/g and a Coulombic efficiency close to 100% at 1 C. In addition, the symmetrical lithium battery Li|Li with the composite electrolyte could cycle stably for about 1500 h without failure at room temperature.
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Jean-Fulcrand, Annelise, Eun Ju Jeon, Schahrous Karimpour, and Georg Garnweitner. "Cross-Linked Solid Polymer-Based Catholyte for Solid-State Lithium-Sulfur Batteries." Batteries 9, no. 7 (June 23, 2023): 341. http://dx.doi.org/10.3390/batteries9070341.
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All-solid-state lithium-sulfur batteries (ASSLSBs) are a promising next-generation battery technology. They exhibit high energy density, while mitigating intrinsic problems such as polysulfide shuttling and lithium dendrite growth that are common to liquid electrolyte-based batteries. Among the various types of solid electrolytes, solid polymer electrolytes (SPE) are attractive due to their superior flexibility and high safety. In this work, cross-linkable polymers composed of pentaerythritol tetraacrylate (PETEA) and tri(ethylene glycol) divinyl ether (PEG), are incorporated into sulfur–carbon composite cathodes to serve a dual function as both a binder and electrolyte, as a so-called catholyte. The influence of key parameters, including the sulfur–carbon ratio, catholyte content, and ionic conductivity of the electrolyte within the cathode on the electrochemical performance, was investigated. Notably, the sulfur composite cathode containing 30 wt% of the PETEA-PEG copolymer catholyte achieved a high initial discharge capacity of 1236 mAh gS−1 at a C-rate of 0.1 and 80 °C.
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Liu, Zhantao, Jue Liu, Yifei Mo, and Hailong Chen. "Design of High-Performance Solid Electrolytes Guided By Crystal Structure Characterization and Understanding." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 225. http://dx.doi.org/10.1149/ma2022-023225mtgabs.
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Solid electrolyte is the key component in all-solid-state-batteries that is currently limiting the commercialization of this technology. An ideal solid electrolyte should have high room temperature ionic conductivity, low electronic conductivity, good compatibility with both cathode and anode, good mechanical properties, high air and moisture stability and low manufacture cost. Among these requirements, the improvement of ionic conductivity is prioritized as the conductivity of most existing solid electrolyte is still much lower than that of conventional liquid electrolyte. The improvement of ionic conductivity and design and development of solid electrolyte materials are closely related to our understanding on the ionic diffusion mechanism in solids and the structure-property relationship. We believe that rational design of high-performance solid electrolyte should start from careful characterization and good understanding of the crystal structure. Here we report the crystal structure characterization on sulfides and halide solid electrolytes and the design and development of novel solid electrolytes based on our findings in structural characterizations. Ex situ high resolution synchrotron X-ray and neutron diffraction and pair distribution function analysis are used to understand the crystal structures in great details. In situ X-ray diffraction for different synthesis methods is coupled with variable temperature electrochemical impedance spectroscopy to understand the structure-property relationship in the solid electrolytes. The design, synthesis and electrochemical evaluation of several solid electrolytes will be presented and discussed.
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Lee, Kyoung-Jin, Eun-Jeong Yi, Gangsanin Kim, and Haejin Hwang. "Synthesis of Ceramic/Polymer Nanocomposite Electrolytes for All-Solid-State Batteries." Journal of Nanoscience and Nanotechnology 20, no. 7 (July 1, 2020): 4494–97. http://dx.doi.org/10.1166/jnn.2020.17562.
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Lithium-ion conducting nanocomposite solid electrolytes were synthesized from polyethylene oxide (PEO), poly(methyl methacrylate) (PMMA), LiClO4, and Li1.3Al0.3Ti1.7(PO4)3 (LATP) ceramic particles. The synthesized nanocomposite electrolyte consisted of LATP particles and an amorphous polymer. LATP particles were homogeneously distributed in the polymer matrix. The nanocomposite electrolytes were flexible and self-standing. The lithium-ion conductivity of the nanocomposite electrolyte was almost an order of magnitude higher than that of the PEO/PMMA solid polymer electrolyte.
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Lv, Wenjing, Kaidong Zhan, Xuecheng Ren, Lu Chen, and Fan Wu. "Comparing Charge Dynamics in Organo-Inorganic Halide Perovskite: Solid-State versus Solid-Liquid Junctions." Journal of Nanoelectronics and Optoelectronics 19, no. 2 (February 1, 2024): 121–28. http://dx.doi.org/10.1166/jno.2024.3556.
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In this study, we explore the dynamics of a perovskite-electrolyte photoelectrochemical cell, pivotal for advancing electrolyte-gated field effect transistors, water-splitting photoelectrochemical and photocatalytic cells, supercapacitors, and CO2 capture and reduction technologies. The instability of hybrid perovskite materials in aqueous electrolytes presents a significant challenge, yet recent breakthroughs have been achieved in stabilizing organo-inorganic halide perovskite films. This stabilization is facilitated by employing liquid electrolytes, specifically those formed by dissolving tetrabutylammoniumperchlorate in dichloromethane. A critical aspect of this research is the comparative analysis of charge and ion kinetics at the perovskite/liquid electrolyte interface versus the perovskite/solid charge transport layer interface. Employing Intensity Modulated Photocurrent Spectroscopy (IMPS), Open-Circuit Voltage Decay (OCVD), and Capacitance-Frequency (C-F) methods, the study scrutinizes charge dynamics in both perovskite/electrolyte and perovskite/solid interfaces. Furthermore, the investigation extends to contrasting the properties of solid–liquid and solid-state junctions, focusing on mobile ions, electric field impacts, and electron-hole transport. The research also examines variations in recombination resistance and ionic double layer charging in perovskite-based devices, aiming to elucidate the operational mechanisms and kinetic complexities at the hybrid perovskite/electrolyte interface.
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Choi, Kyoung Hwan, Eunjeong Yi, Kyeong Joon Kim, Seunghwan Lee, Myung-Soo Park, Hansol Lee, and Pilwon Heo. "(Invited) Pragmatic Approach and Challenges of All Solid State Batteries: Hybrid Solid Electrolyte for Technical Innovation." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 988. http://dx.doi.org/10.1149/ma2023-016988mtgabs.
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For the growth of electric vehicle market, lithium-ion batteries (LIBS) used in the EVs still requires safety and reliability. Unfortunately, large-scale application of the LIBs is being challenged due to the fact that the use of flammable liquid electrolytes has caused safety issues such as leakage and fire explosion. In this respect, all-solid-state batteries (ASSBs) have been intensively studied to ensure the safety and mileage that are superior to the current LIBs. In terms of solid electrolytes, oxide electrolytes not only shows high ionic conductivity (10-4 ~ 10-3 S/cm) but also high mechanical strength to suppress surface dendrite formation. In addition, the oxide electrolytes possess advantages such as non-flammability, high thermal stability, and excellent electrochemical stability (~ 6 V), enabling high temperature/high voltage operations of oxide-based ASSBs. However, most of oxide materials require a sintering process at high temperatures to form a planar solid electrolyte. And a lack of flexibility results in non-uniform electrolyte/electrode contact in the battery, which makes it difficult to apply the rigid oxide electrolyte directly. On the other hand, solid polymer electrolytes have also been actively investigated due to no leakage, good electrolyte/electrode contact, easy processing, flexibility, and good film formability. However, the solid polymer electrolytes have critical disadvantages such as low ionic conductivity at room temperature and low thermal/mechanical stability, which precludes commercialization of solid polymer-based ASSBs despite their advantages. To overcome each disadvantages of oxide and polymer electrolytes, we developed hybrid electrolytes for improved ionic conductivity, easy processing, and formation of continuous electrolyte/electrode interface. In this presentation, pragmatic approach and current challenges related to solid batteries will be discussed including innovative manufacturing process. Hybrid electrolytes and their synergistic effect on the battery performance as a promissing solution will be presented [Fig. 1]
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Kim, Jun tae, Hyeon-ji Shin, and Hun-Gi Jung. "Solid Electrolyte Coated NCM523 for Composite Cathode in All-Solid-State Batteries." ECS Meeting Abstracts MA2023-02, no. 65 (December 22, 2023): 3067. http://dx.doi.org/10.1149/ma2023-02653067mtgabs.
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All-solid-state battery using sulfide solid electrolyte has advantages such as high lithium ionic conductivity and wide electrochemical stability window. Although it is attracting great attention in that it is capable of high power and high energy density, there are problems to be improved. Organic liquid electrolytes in conventional lithium ion batteries have excellent wettability and can form uniform lithium ion transfer channels in electrodes. However, in the case of all-solid-state battery, the formation of a solid-solid interface is limited due to the solid characteristics. In addition, the degradation of the interfacial contact between the active material and solid electrolyte in the composite electrode due to the volume change of the active material with (de)-intercalation of lithium ion during cycling causes loss of the lithium ionic pathway and deterioration of cell performance. This study focuses on improving battery performance by coating the surface of active material with solid electrolyte to maintain an even lithium ion transfer path in the composite electrode. The solid electrolyte coating of the active material has a decisive effect on the electrochemical behavior of the cell because it affects the formation of smooth lithium ionic pathway and suppression of voids in the composite electrode. Therefore, the focus of this study is to confirm the formation of uniform solid electrolyte coating layer according to the size of the solid electrolyte. Therefore, the particle size of the solid electrolyte was diversified using a liquid-phase process and a dispersant, and the solid electrolyte coating was performed using a dispersion process. It was confirmed that an even solid electrolyte coating layer was formed as the particles size of the solid electrolyte decreased, and the electrochemical performance was improved due to the solid electrolyte coating layer. In addition, it was confirmed that the lithium ionic pathway was maintained even after long cycling with the solid electrolyte coating layer, and also the side reactions occurred less according to the homogeneous electrochemical reaction.
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Ashraf, Juveiriah M., Myriam Ghodhbane, and Chiara Busa. "The Effect of Ionic Carriers and Degree of Solidification on the Solid-State Electrolyte Performance for Free-Standing Carbon Nanotube Supercapacitor." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2490. http://dx.doi.org/10.1149/ma2022-0272490mtgabs.
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To eliminate electrolyte leakage, the development of safe and flexible supercapacitors necessitates solid-state electrolytes which integrate both high mechanical and electrochemical capabilities. Quasi-solid-state electrolytes, which constitute a polymer matrix along with an aqueous electrolytic phase, are a viable answer to this problem. Recently, gel electrolytes have gained a lot of attention in flexible and wearable electronic devices due to their remarkable advancements. However, the limitation in the multi-functional abilities and high-performance in such gels hinders the practical usage of such devices. On the electrochemical perspective, the performance of the gel electrolyte depends on the type of ionic carrier (acidic, alkaline, or salt-based), size of the ion, solvent concentration, type of polymer, as well as the interaction between the polymer and other components. Moreover, the performance of the electrolyte differs with the electrode-electrolyte interface and thus is highly dependent on the electrode material. For this reason, it is vital to carry a parametric study to evaluate the effect of the above stated. The aim of this study is to investigate the effect of changing the ionic carrier (namely H3PO4, KOH and LiCl) as well as the solvent concentration on architecturally engineered PVA-based electrolytes’ performance in free-standing CNT supercapacitor using a bio-based compound, cellulose as a binder. The dependence of the electrolyte’s mechanical structure for long term stability is further evaluated by using the optimized concentration of each (H3PO4, KOH and LiCl) by freezing and de-freezing the gel to form membrane-like films, as a result of the increased physical cross-linking. The supercapacitors are studied for their capacitance, charge/discharge capabilities as well their long-term stability and also compared with aqueous electrolyte for the three aforementioned ionic carriers.
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Liang, Xinghua, Yuying Wang, Zhida Liang, Ge Yan, Lingxiao Lan, Yujiang Wang, Xueli Shi, Shuhong Yun, and Meihong Huang. "Long-Cycle Stability of In Situ Ultraviolet Curable Organic/Inorganic Composite Electrolyte for Solid-State Batteries." Polymers 16, no. 1 (December 23, 2023): 55. http://dx.doi.org/10.3390/polym16010055.
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Lithium-ion solid-state batteries with spinel Li4Ti5O12 (LTO) electrodes have significant advantages, such as stability, long life, and good multiplication performance. In this work, the LTO electrode was obtained by the atmospheric plasma spraying method, and a composite solid electrolyte was prepared by in situ ultraviolet (UV) curing on the LTO electrode. The composite solid electrolyte was designed using a soft–hard combination strategy, and the electrolyte was prepared into a composite of a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) flexible structure and high-conductivity Li1.3Al0.3Ti1.7(PO4)3 (LATP) hard particles. The composite electrolyte exhibited a good ionic conductivity up to 0.35 mS cm−1 at 30 °C and an electrochemical window above 4.0 V. In situ and ex situ electrolytes were assembled into LTO//electrolyte//Li solid-state batteries to investigate their impact on the electrochemical performance of the batteries. As a result, the assembled Li4Ti5O12//in situ electrolytes//Li batteries exhibited excellent rate of performance, and their capacity retention rate was 90% at 0.2 mA/cm2 after 300 cycles. This work provides a new method for the fabrication of novel advanced solid-state electrolytes and electrodes for applications in solid-state batteries.
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Raj, Hari, Audric Neveu, and Valerie Pralong. "New Low Cost Sulfide Electrolytes for All Solid State Batteries." ECS Meeting Abstracts MA2023-02, no. 8 (December 22, 2023): 3251. http://dx.doi.org/10.1149/ma2023-0283251mtgabs.
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The low cost, safe and high energy storage technology is needed to ensure a continuous energy supply from renewal energy sources. However, current Li-ion batteries (LiBs) are facing challenges to fulfil the safety and high energy and power demands of fast-growing market of electric vehicles (EVs). In particular, liquid organic electrolytes used in conventional LIBs have raised the safety issues due to serious fire risk. Solid state batteries (SSBs) are considered to provide better safety as compared to LIBs because of solid electrolytes (SEs) are used in SSBs instead of flammable organic liquid based electrolytes [1-4]. The various types of solid electrolytes have already been reported for SSBs which can be divided into oxides, sulfides, halides and polymers based on their properties, advantages and disadvantages [5]. Among these solid electrolytes, sulfide solid electrolytes have advantages over other due to high conductivity and ductile nature of sulfides [6]. The discovery of Li10GeP2S12 solid electrolyte called LGPS structured sulfide electrolyte have shown great potential to replace liquid electrolyte as ionic conductivity of LGPS was found 1.2×10-2 S cm-1 at room temperature comparable to the conductivity of organic liquid electrolyte [7]. However, Li10GeP2S12 electrolyte suffers with poor cyclability in solid state batteries due to reduction of Ge+4 ions to Ge0, and instable against lithium metal anode. Moreover, germanium (Ge) is a rare and expensive element, which limits the industrial application of Li10GeP2S12 [8, 9]. Therefore, in the present work, we have developed LGPS structured based new Ge free solid electrolytes with high conductivity and better electrochemical stability. The phase identification of newly synthesized solid electrolytes is done by X-ray diffractometer technique along with Rietveld refinement analysis. The conductivity of prepared solid electrolytes is determined by electrochemical impedance spectroscopy. The ionic conductivity of newly synthesised electrolytes has reached upto 0.67 mS cm-1 at room temperature. The electrochemical analysis of prepared solid electrolytes is done using Li-metal in both side (in symmetric cell) as well as using standard cathode and anode materials (full cell). References: Janek et al., Energy 1, 2016, 16141. Xu et al., Joule 2, 2018, 1991. Li et al., RSC Adv. 5, 2015, 52382. Scrosati et al., Power Sources 195, 2010, 2419. Zhang et al., Energy Storage Mater. 10, 2018, 139-159. Jiang et al., ACS Appl Mater Interfaces 12, 2020, 54662-70. Kamaya et al., Mater., 10, 2011, 682–686. Neveu et al., Power Sources 467, 2020, 228250. Wan et al., ACS Energy Lett., 6, 2021, 862–868.
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Liang, Xinghua, Dongxue Huang, Linxiao Lan, Guanhua Yang, and Jianling Huang. "Enhancement of the Electrochemical Performances of Composite Solid-State Electrolytes by Doping with Graphene." Nanomaterials 12, no. 18 (September 16, 2022): 3216. http://dx.doi.org/10.3390/nano12183216.
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With high safety and good flexibility, polymer-based composite solid electrolytes are considered to be promising electrolytes and are widely investigated in solid lithium batteries. However, the low conductivity and high interfacial impedance of polymer-based solid electrolytes hinder their industrial applications. Herein, a composite solid-state electrolyte containing graphene (PVDF-LATP-LiClO4-Graphene) with structurally stable and good electrochemical performance is explored and enables excellent electrochemical properties for lithium-ion batteries. The ionic conductivity of the composite electrolyte membrane containing 5 wt% graphene reaches 2.00 × 10−3 S cm−1 at 25 °C, which is higher than that of the composite electrolyte membrane without graphene (2.67 × 10−4 S cm−1). The electrochemical window of the composite electrolyte membrane containing 5 wt% graphene reaches 4.6 V, and its Li+ transference numbers reach 0.84. Assembling this electrolyte into the battery, the LFP/PVDF-LATP-LiClO4-Graphene /Li battery has a specific discharge capacity of 107 mAh g−1 at 0.2 C, and the capacity retention rate was 91.58% after 100 cycles, higher than that of the LiFePO4/PVDF-LATP-LiClO4/Li (LFP/PLL/Li) battery, being 94 mAh g−1 and 89.36%, respectively. This work provides a feasible solution for the potential application of composite solid electrolytes.
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Chang, Kang-Feng, Pradeep Kumar Panda, Chien-Te Hsieh, Po-Chih Yang, Navish Kataria, and Kuan Shiong Khoo. "Solid-State Lithium Batteries with Cathode-Supported Composite Solid Electrolytes Enabling High-Rate Capability and Excellent Cyclic Performance." Batteries 9, no. 10 (September 26, 2023): 490. http://dx.doi.org/10.3390/batteries9100490.
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In this study, robust composite solid electrolytes were developed and employed to enhance the performance of Li-metal batteries significantly. The robust composite solid electrolytes are composed of a soft polymer, poly(ethylene oxide), a Li salt, bis(trifluoromethanesulfonyl)imide (LiTFSI), and super ionic conductive ceramic fillers such as Li1.5Al0.5Ti1.5(PO4)3 (LATP), and Li6.4La3Zr1.4Ta0.6O12 (LLZTO). The main goal of this study is to enhance the electrochemical stability and ionic conductivity. The ionic conductivities of the composite solid electrolytes were found to be 2.08 × 10−4 and 1.64 × 10−4 S cm−1 with the introduction of LATP and LLZTO fillers, respectively. The results prove that the fabricated solid electrolyte was electrochemical stable at voltage exceeding 4.25 V vs. Li/Li+. The internal resistance of the solid electrolyte significantly reduced compared to gel electrolyte. This reduction can be attributed to the alleviation of bulk electrolyte, charge-transfer, and interfacial electrolyte/electrode impedance. When LiFePO4 cathode sheets are coated with a composite solid electrolyte containing LATP powders, the resulting Li-metal battery displays high capacity at 5 C (with a capacity retention of 65.2% compared to the original capacity at 0.2 C) as well as superior cyclic stability and excellent Coulombic efficiency (>99.5%, 200 cycles). These results confirm that the composite solid electrolyte acts as a protective layer which has the ability to prevent the growth of Li dendrites. Consequently, the fabricated electrolyte configuration can be engineered to enable high energy/power density and electrochemical stable cyclability in Li-metal batteries.
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Chen, Feiyang, and Zheng-Long Xu. "Mg(TFSI)2-Based Solid-State Eutectic Electrolyte Towards Safer Magnesium Batteries." ECS Meeting Abstracts MA2023-01, no. 7 (August 28, 2023): 2776. http://dx.doi.org/10.1149/ma2023-0172776mtgabs.
Full textAbstract:
Magnesium (Mg) batteries are regarded as safer alternatives for Li+-dominated batteries by virtue of the unique dendrite-free property of Mg element. However, traditional liquid electrolytes applied in Mg batteries are mainly based on chloride salts and highly flammable organic solvents, which might cause numerous safety issues such as fire, electrochemical corrosion, and leakage of hazardous chemicals. These kinds of electrolytes seriously violate the original purpose of developing Mg-based batteries. Therefore, exploring non-flammable chloride-free solid-state electrolytes is of significant importance for realizing safer Mg batteries. Here in this work, a novel non-flammable eutectic electrolyte based on chloride-free Mg(TFSI)2 salt is first proposed as a solid electrolyte for safer Mg metal batteries. Our recent results demonstrate that compared with traditional Mg(TFSI)2-based electrolytes which dissolve in flammable organic solvents such as EC, PC, and THF solvent, this Mg(TFSI)2-based eutectic solid electrolyte is non-flammable with robust mechanical structures. When applied in Mg//Mg symmetric batteries, this novel eutectic solid electrolyte could greatly suppress the overpotential phenomenon that occurs in traditional Mg-based electrolytes and achieves stable Mg plating/stripping reversibility with more than 150 h. Furthermore, the practical feasibility of this eutectic solid electrolyte is also demonstrated in Mg//V2O5 full cell, which shows competitive electrochemical performance. We believe that the research on such new electrolytes could provide a new strategy for developing safe and sustainable Mg-based batteries.
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Yao, Wangbing, Zhuoyuan Zheng, Jie Zhou, Dongming Liu, Jinbao Song, and Yusong Zhu. "A Minireview of the Solid-State Electrolytes for Zinc Batteries." Polymers 15, no. 20 (October 10, 2023): 4047. http://dx.doi.org/10.3390/polym15204047.
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Aqueous zinc-ion batteries (ZIBs) have gained significant recognition as highly promising rechargeable batteries for the future due to their exceptional safety, low operating costs, and environmental advantages. Nevertheless, the widespread utilization of ZIBs for energy storage has been hindered by inherent challenges associated with aqueous electrolytes, including water decomposition reactions, evaporation, and liquid leakage. Fortunately, recent advances in solid-state electrolyte research have demonstrated great potential in resolving these challenges. Moreover, the flexibility and new chemistry of solid-state electrolytes offer further opportunities for their applications in wearable electronic devices and multifunctional settings. Nonetheless, despite the growing popularity of solid-state electrolyte-based-ZIBs in recent years, the development of solid-state electrolytes is still in its early stages. Bridging the substantial gap that exists is crucial before solid-state ZIBs become a practical reality. This review presents the advancements in various types of solid-state electrolytes for ZIBs, including film separators, inorganic additives, and organic polymers. Furthermore, it discusses the performance and impact of solid-state electrolytes. Finally, it outlines future directions for the development of solid-state ZIBs.
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Wu, Xinsheng, and Jay Whitacre. "Reevaluating the Stability of the PEO-Based Solid-State Electrolytes for High Voltage Solid-State Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 402. http://dx.doi.org/10.1149/ma2022-024402mtgabs.
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Poly(ethylene oxide) (PEO) is a very popular polymer-based solid electrolyte material with relatively high ionic conductivity and dielectric constant1. However, many previous works mentioned that it could not be used in high voltage cells for its low oxidation potential (~3.9V vs. Li/Li+)2. However, only a handful of prior investigations evaluated the stability of the PEO-based solid-state electrolyte considering the contribution of the cathode surface chemistry to electrolyte oxidation and decomposition. Since most of the previous research exploring high voltage cathodes with PEO used LiCoO2, it could be possible the other cathode compositions will erode the PEO-based solid electrolyte in different and less extreme ways. Our work revisits the high voltage electrochemical stability of PEO-based solid state-electrolyte materials. Potentiodynamic and galvanostatic tests were performed in test cells using PEO electrolyte layers with either LiNixMnyCozO2 or LiCoO2 cathode materials. We found that the high voltage instability of PEO-based solid-state cells is profoundly affected by the instability of the cathode material used. Specifically, the LiCoO2 electrodes were observed to undergo an irreversible oxidation process where they shattered into small pieces, which then led to a rapid irreversible loss in capacity. In contrast, we found that the PEO-based solid-state electrolytes could be stably cycled with high-nickel content cathodes stably at a voltage up to 4.5V vs. Li/Li+ over many cycles with minimal capacity deterioration. K. Chrissopoulou, K. S. Andrikopoulos, S. Fotiadou, S. Bollas, C. Karageorgaki, D. Christofilos, G. A. Voyiatzis, and S. H. Anastasiadis, 44, 9710–9722 (2011). J. Qiu, X. Liu, R. Chen, Q. Li, Y. Wang, P. Chen, L. Gan, S.-J. Lee, D. Nordlund, Y. Liu, X. Yu, X. Bai, H. Li, and L. Chen, Adv. Funct. Mater., 30, 1909392 (2020).
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Gorai, Prashun, Hai Long, Eric Jones, Shriram Santhanagopalan, and Vladan Stevanović. "Defect chemistry of disordered solid-state electrolyte Li10GeP2S12." Journal of Materials Chemistry A 8, no. 7 (2020): 3851–58. http://dx.doi.org/10.1039/c9ta10964a.
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Most solid-state electrolytes exhibit significant structural disorder, which requires careful consideration when modeling the defect energetics. Here, we model the native defect chemistry of a disordered solid electrolyte, Li10GeP2S12.
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Li, Gang, Shuo Wang, Jipeng Fu, Yuan Liu, and Zehua Chen. "Manufacturing High-Energy-Density Sulfidic Solid-State Batteries." Batteries 9, no. 7 (June 28, 2023): 347. http://dx.doi.org/10.3390/batteries9070347.
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All-solid-state batteries (ASSBs) using sulfide solid electrolytes with high room-temperature ionic conductivity are expected as promising next-generation batteries, which might solve the safety issues and enable the utilization of lithium metal as the anode to further increase the energy density of cells. Most researchers in the academic community currently focus on developing novel sulfide solid electrolytes, clarifying the interface issues between sulfide electrolytes and solid electrodes and mechanism of lithium dendrite growth in ASSB. However, there is a lacking in the technical route analysis about the commercialization of ASSBs based on sulfide solid electrolytes. This review mainly introduces the specific preparation methods of various parts in sulfide-based ASSBs, including the preparation methods of sulfide solid electrolyte particles, sulfide-based composite electrolyte membranes, composite cathodes and anodes, and analyzes the advantages and disadvantages of these methods. In addition, several schemes of ASSB assembly are also introduced. Finally, a perspective of large-scale production of sulfide-based ASSBs is provided, which is expected to accelerate the commercialization of sulfide-based ASSBs.
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Wang, Wei Min. "Study on All Solid-State Composite Polymer Electrolyte." Advanced Materials Research 571 (September 2012): 13–16. http://dx.doi.org/10.4028/www.scientific.net/amr.571.13.
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So far, there has been a large number of high conductivity of solid materials to replace the liquid electrolyte. All solid-state composite polymer electrolyte materials have not yet fully realized industrial production, but many areas are moving in the direction of practical development. With the deepening of the study, the ionic conductivity mechanism and constantly improve, but the ionic conductivity of composite electrolytes should be improved, need to conduct groundbreaking research in the preparation process, structure and properties of the composite electrolyte materials have many problems. The composite polymer electrolyte materials has become an intersection of many disciplines including materials science, chemistry, physics, and the content may lead to the field of new energy materials, in particular, is a new technological revolution in the field of battery materials, which study of the problem will continue and in-depth.
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Park, Sangbaek. "Recent Advances in Interface Engineering for All-Solid-State Batteries." Ceramist 25, no. 1 (March 31, 2022): 104–21. http://dx.doi.org/10.31613/ceramist.2022.25.1.03.
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All-solid-state batteries are attractive energy storage devices with high stability and energy density due to their non-flammable solid electrolytes that can utilize lithium and allow cells to be stacked directly in series. It is essential to develop superior solid interfaces for its commercialization by improving the interfacial stability and kinetics. However, complex interfacial phenomena in both solid electrolyte/cathode and solid electrolyte/anode make the interfacial problem of all-solid-state batteries difficult to solve. To overcome this issue, the origins of high resistance and low stability at solid interfaces have been widely explored and alternatives have been proposed accordingly. In this paper, the main methodologies and recent advances for solving the solid electrolyte/electrode interface problems will be reviewed in the chemical, electrochemical, and mechanical aspects.
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Suci, Windhu Griyasti, Harry Kasuma (Kiwi) Aliwarga, Yazid Rijal Azinuddin, Rosana Budi Setyawati, Khikmah Nur Rikhy Stulasti, and Agus Purwanto. "Review of various sulfide electrolyte types for solid-state lithium-ion batteries." Open Engineering 12, no. 1 (January 1, 2022): 409–23. http://dx.doi.org/10.1515/eng-2022-0043.
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Abstract The high sulfide ion polarization is known to cause increased ionic conductivity in the solid sulfide-type electrolytes. Three groups of sulfide-based solid-state electrolytes, namely, Li-P-S, Li6PS5X (X: Cl, Br, and I), and Li x MP x S x (M: Sn, Si, and Al) were reviewed systematically from several aspects, such as conductivity, stability, and crystal structure. The advantages and disadvantages of each electrolyte were briefly considered and compared. The method of the preparation was presented with experimental and theoretical studies. The analysis that has been carried out showed that the solid electrolyte Li10GeP2S12 is superior to others with an ionic conductivity of 12 × 10−2 S cm−1. This conductivity is comparable to that of conventional liquid electrolytes. However, the availability and high price of Ge are the problems encountered. Furthermore, because sulfide-based solid electrolytes have low chemical stability in ambient humidity, their handling is restricted to inert gas environments. When solid sulfide electrolytes are hydrolyzed, structural changes occur and H2S gas is produced. The review’s objective includes presenting a complete knowledge of sulfide-solid electrolyte synthesis method, characteristics, such as conductivity, structure, and stability, as well as generating more efficient and targeted research in enhancing the performance of the chemical substance.
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Reddy, Mogalahalli V., Christian M. Julien, Alain Mauger, and Karim Zaghib. "Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review." Nanomaterials 10, no. 8 (August 15, 2020): 1606. http://dx.doi.org/10.3390/nano10081606.
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Energy storage materials are finding increasing applications in our daily lives, for devices such as mobile phones and electric vehicles. Current commercial batteries use flammable liquid electrolytes, which are unsafe, toxic, and environmentally unfriendly with low chemical stability. Recently, solid electrolytes have been extensively studied as alternative electrolytes to address these shortcomings. Herein, we report the early history, synthesis and characterization, mechanical properties, and Li+ ion transport mechanisms of inorganic sulfide and oxide electrolytes. Furthermore, we highlight the importance of the fabrication technology and experimental conditions, such as the effects of pressure and operating parameters, on the electrochemical performance of all-solid-state Li batteries. In particular, we emphasize promising electrolyte systems based on sulfides and argyrodites, such as LiPS5Cl and β-Li3PS4, oxide electrolytes, bare and doped Li7La3Zr2O12 garnet, NASICON-type structures, and perovskite electrolyte materials. Moreover, we discuss the present and future challenges that all-solid-state batteries face for large-scale industrial applications.
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Bae, Youngjoon, Sungjin Lim, Ryounghee Kim, and Tae Young Kim. "The Effect of Pressure during Sintering on the Interface between Oxide Solid Electrolyte and Cathode in Solid State Lithium Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 410. http://dx.doi.org/10.1149/ma2022-024410mtgabs.
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Conventional Li-ion batteries (LIBs), which have been widely used as main power sources for various electronic devices, are facing huge challenges with the explosive growth of electric vehicles (EVs) market. The safety problems of LIBs in EVs causing fire incident mainly result from the use of liquid electrolytes which provide fuel for combustion. Therefore, solid state lithium batteries using a solid electrolyte are widely accepted as promising candidates for next generation energy storage devices with superior safety performances. However, solid state batteries have limitations that originate from solid-solid interfaces between electrode and solid electrolyte, hindering practical development of solid state batteries. Especially, compared to sulfide based solid electrolyte, oxide based solid electrolyte is rigid, resulting in difficulty in forming intimate contact between solid electrolyte and electrode materials. In this study, using lithium vanadium phosphate (Li3V2(PO4)3, LVP) and lithium aluminum germanium phosphate (Li1.5Al0.5Ge1.5(PO4)3, LAGP) as cathode material and oxide solid electrolyte model system, we demonstrate the effect of pressure during sintering on the contact between LVP and LAGP, and concomitant cell performance. In addition, we found that the crystallinity of solid electrolyte and the content of carbon conducting agent critically affect the contact. Without any complicated interfacial modification, we successfully made decent cathode-solid electrolyte interface with simple method for superior solid state lithium batteries.
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Touidjine, Amina, Vincent Calmes, Mélanie Dendary, Philippe Borel, Paulin Truche, and Thibaut Dussart. "Solid-State Polymer Battery: Manufacturing Process and Characterization." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 720. http://dx.doi.org/10.1149/ma2023-024720mtgabs.
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Solid-state batteries are a promising technology that could provide higher energy density, better safety, longer cycle life and a wider operating temperature range than current commercial LiBs [1] . The solid electrolyte is the main component of all-solid-state batteries. It can be ceramic, glass, polymer, or a mixture. Solid Polymer Electrolyte (SPEs) have received distinctive attention, especially by industry, owing to their potential advantages such as safety, lightweight, high flexibility, and realistic processability. However, despite fast growing interest in solid-state technology, reports on the scalable production of all-solid-state lithium-ion batteries using electrodes with meaningful areal capacities are rather scarce [2] . Moreover, chemical, and mechanical challenges remain. The intimate contact between the electrode and the solid electrolyte is difficult due its non-infiltrative nature. This lack of intimate contact severely limits the cycling properties [3] . The development of effective strategies to alleviate the issue of physical contact is imperative in the engineering of solid-state batteries [4] . In the frame of SAFELiMOVE (Advanced all Solid stAte saFE Lithium Metal technology tOwards Vehicle Electrification) project, we assemble a solid-state pouch based on lithium metal anode, a solid polymer electrolyte layer and a compatible cathode. In work, we report on a reliable fabrication process of large-scale all-solid-state lithium-ion batteries using cathodes prepared by CIDETEC, lithium anode provided by Hydro-Quebec, polymers provided by CICe, inorganic filler provided by SCHOTT and a solid polymer electrolyte manufactured at SAFT. All-solid-state lithium-ion battery pouch cells have been successfully built with consistent electrochemical performance. Cycling that shows the good performance of those cells and the lesson learned regarding their cycling conditions will be presented. [1] J. Motalli, “A solid future Nature, 526, S96 (2015) [2] Ningxin Zhang et al “Scalable preparation of practical 1Ah all-solid-state lithium-ion batteries cells and their abuse tests”, Journal of Energy Storage 59 (2023) 106547 [3] Li et al.“Atomically Intimate Contact between Solid Electrolytes and Electrodes for Li Batteries” Mater 1, 1001-1016, October 2, 2019. [4] Theodosios Famprikis, Pieremanuele Canepa, James A. Dawson, M. Saiful Islam and Christian Masquelier“Fundamentals of inorganic solid-state electrolytes for batteries” Nature Materials-August 2019. Figure 1
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Li, Yutao, Weidong Zhou, Xi Chen, Xujie Lü, Zhiming Cui, Sen Xin, Leigang Xue, Quanxi Jia, and John B. Goodenough. "Mastering the interface for advanced all-solid-state lithium rechargeable batteries." Proceedings of the National Academy of Sciences 113, no. 47 (November 7, 2016): 13313–17. http://dx.doi.org/10.1073/pnas.1615912113.
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A solid electrolyte with a high Li-ion conductivity and a small interfacial resistance against a Li metal anode is a key component in all-solid-state Li metal batteries, but there is no ceramic oxide electrolyte available for this application except the thin-film Li-P oxynitride electrolyte; ceramic electrolytes are either easily reduced by Li metal or penetrated by Li dendrites in a short time. Here, we introduce a solid electrolyte LiZr2(PO4)3 with rhombohedral structure at room temperature that has a bulk Li-ion conductivity σLi = 2 × 10−4 S⋅cm−1 at 25 °C, a high electrochemical stability up to 5.5 V versus Li+/Li, and a small interfacial resistance for Li+ transfer. It reacts with a metallic lithium anode to form a Li+-conducting passivation layer (solid-electrolyte interphase) containing Li3P and Li8ZrO6 that is wet by the lithium anode and also wets the LiZr2(PO4)3 electrolyte. An all-solid-state Li/LiFePO4 cell with a polymer catholyte shows good cyclability and a long cycle life.
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Choi, Gyo, Jaehyeong Park, Sungjun Bae, and Jung Park. "Quasi-Solid-State SiO2 Electrolyte Prepared from Raw Fly Ash for Enhanced Solar Energy Conversion." Materials 15, no. 10 (May 17, 2022): 3576. http://dx.doi.org/10.3390/ma15103576.
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Quasi-solid-state electrolytes in dye-sensitized solar cells (DSSCs) prevent solvent leakage or evaporation and stability issues that conventional electrolytes cannot; however, there are no known reports that use such an electrolyte based on fly ash SiO2 (FA_SiO2) from raw fly ash (RFA) for solar energy conversion applications. Hence, in this study, quasi-solid-state electrolytes based on FA_SiO2 are prepared from RFA and poly(ethylene glycol) (PEG) for solar energy conversion. The structural, morphological, chemical, and electrochemical properties of the DSSCs using this electrolyte are characterized by X-ray diffraction (XRD), high-resolution field-emission scanning electron microscopy (HR-FESEM), X-ray fluorescence (XRF), diffuse reflectance spectroscopy, electrochemical impedance spectroscopy (EIS), and incident photon-to-electron conversion efficiency (IPCE) measurements. The DSSCs based on the quasi-solid-state electrolyte (SiO2) show a cell efficiency of 5.5%, which is higher than those of nanogel electrolytes (5.0%). The enhancement of the cell efficiency is primarily due to the increase in the open circuit voltage and fill factor caused by the reduced electron recombination and improved electron transfer properties. The findings confirm that the RFA-based quasi-solid-state (SiO2) electrolyte is an alternative to conventional liquid-state electrolytes, making this approach among the most promising strategies for use in low-cost solar energy conversion devices.
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Giffin, Guinevere A., Mara Goettlinger, Hendrik Bohn, Simone Peters, Mario Weller, Alexander Naßmacher, Timo Brändel, and Alex Friesen. "Development of a Polymer-Based Silicon-NMC Solid-State Cell." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 373. http://dx.doi.org/10.1149/ma2023-022373mtgabs.
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Solid-state batteries are seen as the next generation of battery technology with the promise of high energy density and improved safety as compared to conventional lithium-ion batteries. To achieve these goals, high-capacity negative electrodes, e.g., silicon or lithium, need to be combined with high capacity and high voltage positive electrodes, e.g., Ni-rich NMC. This combination of active materials provides a number of significant challenges for the solid-state electrolyte. If silicon is used as the anode active material, significant volume changes during lithiation/delithiation occur. These volume changes lead to a variety of problems including irreversible loss of lithium and eventual disintegration of the electrodes, resulting in capacity fade. Therefore, the electrolyte must be sufficiently elastic to buffer these changes. If Ni-rich NMC is used as a cathode active material, then the electrolyte must be stable at voltages up to at least 4.2 V. There are currently few, if any, electrolyte solutions that can address these challenges simultaneously. In the ASTRABAT project, a silicon-NMC solid-state cell has been developed based on two tailored polymer electrolytes, which allows the specific challenges of each cell compartment to be addressed separately. A vinylidene fluoride copolymer-based electrolyte has been developed for use as a catholyte and a hybrid inorganic-organic polymer electrolyte as the anolyte. This work will report a characterization of both electrolytes, along with their electrochemical performance in solid-state half-cells and full-cells.
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Bera, Bapi, Anirban Roy, Douglas Aaron, and Matthew M. Mench. "Understanding the Transport Phenomena in Solid State Battery (SSB)." ECS Meeting Abstracts MA2022-01, no. 1 (July 7, 2022): 45. http://dx.doi.org/10.1149/ma2022-01145mtgabs.
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The state-of-the-art Li-ion battery has energy density plateauing at ~300 Wh/kg. Replacing the graphite-based anode with Li metal is the easiest way to increase energy density. However, a lithium metal anode is prone to non-uniform plating/striping that leads to capacity decay and dendrite formation. Dendrites trigger short-circuiting and possible explosions as the liquid electrolytes that are used in Li-ion batteries are flammable. Solid-state batteries (SSBs) have the potential to enable Li-metal anodes as they are typically less reactive and nonflammable. Additionally, SSBs exhibit greater mechanical stability and can prevent dendritic growth [1,2]. Furthermore, solid electrolytes show much higher thermal stability, are non-toxic, and have high energy density, making the solid-state battery one of the best choices for the next generation of energy storage devices. Solid polymer electrolytes are an important class of materials for making solid-state batteries commercially viable. These have the potential to increase energy density and decrease contact resistance between anode and separator by formation of a suitable solid-electrolyte-interphase (SEI) [1]. However, this technology still has major hurdles to overcome, like lower Li-ion conductivity when compared to state-of-art ceramic separators. In recent years, garnet-type lithium oxide perovskites have gained attractiveness as state-of-art ceramic separators for SSBs. LLZTO is one such ceramic electrolyte that is being thoroughly investigated by researchers as it shows very high Li-ion conductivity at room temperature [2]. However, these materials suffer from poor interfacial contact. Recently, Yang, et al., [3] combined the best of both worlds with a new type of solid polymer separator which has better physical contact between separator and lithium and good li-ion conductivity at room temperature. In this work, we investigate the transport of Li-ions across both a solid polymer electrolyte and LLZTO solid electrolyte using a symmetric Li-cell configuration. Fig. 1 (a) and (c) show the Li plating/stripping cycling performance in a symmetric cell. The cell voltage measured during plating and stripping is to be very high for LLZTO compared to polymer electrolyte. A possible explanation may be due to high interfacial resistance arising between solid ceramic and lithium metal. Impedance spectroscopy was performed on both LLZTO and polymer separators after each current density step (24 h) and shown in Fig. 1 (b) and (d) respectively. The impedance increased with cycling for the LLZTO separator but decreased with cycling for polymer electrolyte. This may indicate that better interfacial contact between Li and polymer exists and that these connections may become more established while cycling. Furthermore, the transport of Li-ions across the separators will be analyzed using the transference number calculated using the Bruce-Vincent method. The influence of temperature and separator thickness on the transference number will also be used to characterize the nature of ion transport across such solid electrolyte separators. Such deep understanding of the transport mechanism is needed to minimize the different losses in SSBs and make it commercially viable. Figure 1: Li plating/stripping cycling performance of the (a) LLZTO electrolyte, and (c) PEO polymer electrolyte at different current density, with 12 minutes for each plating/stripping half cycle, for a total of 72 h at 70 ℃ temperature and their corresponding impedance are shown in (b) and (d) respectively. References R. Sahore, Z. Du, X. C. Chen, W. B. Hawley, A. S. Westover, and N. J. Dudney, Practical considerations for testing polymer electrolytes for high-energy solid-state batteries, ACS Energy Lett. 2021, 6, 2240-2247. A. Parejiya, R. Amin, M. B. Dixit, R. Essehli, C. J. Jafta, D. L. Wood, III, and I. Belharouak, Improving contact impedance via electrochemical pulses applied to lithium−solid electrolyte interface in solid-state batteries, ACS Energy Lett. 2021, 6, 3669−3675. Yang at al, Copper-coordinated cellulose ion conductors for solid-state batteries, Nature, 2021, 598, 590−596. Figure 1
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Sing Liow, Kai, Coswald Stephen Sipaut, Rachel Fran Mansa, Mee Ching Ung, and Shamsi Ebrahimi. "Effect of PEG Molecular Weight on the Polyurethane-Based Quasi-Solid-State Electrolyte for Dye-Sensitized Solar Cells." Polymers 14, no. 17 (September 1, 2022): 3603. http://dx.doi.org/10.3390/polym14173603.
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Nanosilica was surface modified with polyaniline and incorporated into polyurethane to form a polymer matrix capable of entrapping a liquid electrolyte and functioning as quasi-solid-state electrolyte in the dye-sensitized solar cells. The effect on the S−PANi distribution, surface morphology, thermal stability, gel content, and structural change after varying the PEG molecular weight of the polyurethane matrix was analyzed. Quasi-solid-state electrolytes were prepared by immersing the polyurethane matrix into a liquid electrolyte and the polymer matrix absorbency, conductivity, and ion diffusion were investigated. The formulated quasi-solid-state electrolytes were applied in dye-sensitized solar cells and their charge recombination, photovoltaic performance, and lifespan were measured. The quasi-solid-state electrolyte with a PEG molecular weight of 2000 gmol−1 (PU−PEG 2000) demonstrated the highest light-to-energy conversion efficiency, namely, 3.41%, with an open-circuit voltage of 720 mV, a short-circuit current of 4.52 mA cm−2, and a fill factor of 0.63.
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Sun, Zhouting, Mingyi Liu, Yong Zhu, Ruochen Xu, Zhiqiang Chen, Peng Zhang, Zeyu Lu, Pengcheng Wang, and Chengrui Wang. "Issues Concerning Interfaces with Inorganic Solid Electrolytes in All-Solid-State Lithium Metal Batteries." Sustainability 14, no. 15 (July 25, 2022): 9090. http://dx.doi.org/10.3390/su14159090.
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All-solid-state batteries have attracted wide attention for high-performance and safe batteries. The combination of solid electrolytes and lithium metal anodes makes high-energy batteries practical for next-generation high-performance devices. However, when a solid electrolyte replaces the liquid electrolyte, many different interface/interphase issues have arisen from the contact with electrodes. Poor wettability and unstable chemical/electrochemical reaction at the interfaces with lithium metal anodes will lead to poor lithium diffusion kinetics and combustion of fresh lithium and active materials in the electrolyte. Element cross-diffusion and charge layer formation at the interfaces with cathodes also impede the lithium ionic conductivity and increase the charge transfer resistance. The abovementioned interface issues hinder the electrochemical performance of all-solid-state lithium metal batteries. This review demonstrates the formation and mechanism of these interface issues between solid electrolytes and anodes/cathodes. Aiming to address the problems, we review and propose modification strategies to weaken interface resistance and improve the electrochemical performance of all-solid-state lithium metal batteries.
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Gao, Hongcai, Nicholas S. Grundish, Yongjie Zhao, Aijun Zhou, and John B. Goodenough. "Formation of Stable Interphase of Polymer-in-Salt Electrolyte in All-Solid-State Lithium Batteries." Energy Material Advances 2020 (December 23, 2020): 1–10. http://dx.doi.org/10.34133/2020/1932952.
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The integration of solid-polymer electrolytes into all-solid-state lithium batteries is highly desirable to overcome the limitations of current battery configurations that have a low energy density and severe safety concerns. Polyacrylonitrile is an appealing matrix for solid-polymer electrolytes; however, the practical utilization of such polymer electrolytes in all-solid-state cells is impeded by inferior ionic conductivity and instability against a lithium-metal anode. In this work, we show that a polymer-in-salt electrolyte based on polyacrylonitrile with a lithium salt as the major component exhibits a wide electrochemically stable window, a high ionic conductivity, and an increased lithium-ion transference number. The growth of dendrites from the lithium-metal anode was suppressed effectively by the polymer-in-salt electrolyte to increase the safety features of the batteries. In addition, we found that a stable interphase was formed between the lithium-metal anode and the polymer-in-salt electrolyte to restrain the uncontrolled parasitic reactions, and we demonstrated an all-solid-state battery configuration with a LiFePO4 cathode and the polymer-in-salt electrolyte, which exhibited a superior cycling stability and rate capability.
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Gao, Hongcai, Nicholas S. Grundish, Yongjie Zhao, Aijun Zhou, and John B. Goodenough. "Formation of Stable Interphase of Polymer-in-Salt Electrolyte in All-Solid-State Lithium Batteries." Energy Material Advances 2021 (January 7, 2021): 1–10. http://dx.doi.org/10.34133/2021/1932952.
Full textAbstract:
The integration of solid-polymer electrolytes into all-solid-state lithium batteries is highly desirable to overcome the limitations of current battery configurations that have a low energy density and severe safety concerns. Polyacrylonitrile is an appealing matrix for solid-polymer electrolytes; however, the practical utilization of such polymer electrolytes in all-solid-state cells is impeded by inferior ionic conductivity and instability against a lithium-metal anode. In this work, we show that a polymer-in-salt electrolyte based on polyacrylonitrile with a lithium salt as the major component exhibits a wide electrochemically stable window, a high ionic conductivity, and an increased lithium-ion transference number. The growth of dendrites from the lithium-metal anode was suppressed effectively by the polymer-in-salt electrolyte to increase the safety features of the batteries. In addition, we found that a stable interphase was formed between the lithium-metal anode and the polymer-in-salt electrolyte to restrain the uncontrolled parasitic reactions, and we demonstrated an all-solid-state battery configuration with a LiFePO4 cathode and the polymer-in-salt electrolyte, which exhibited a superior cycling stability and rate capability.
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Zahiri, Beniamin, Chadd Kiggins, Dijo Damien, Michael Caple, Arghya Patra, Carlos Juarez Yescaz, John B. Cook, and Paul V. Braun. "Hybrid Halide Solid Electrolytes and Bottom-up Cell Assembly Enable High Voltage Solid-State Lithium Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 327. http://dx.doi.org/10.1149/ma2022-012327mtgabs.
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Interface between halide based solid electrolytes and layered transition metal oxide cathodes has been found to be electro-chemically stable due to stability of chloride compounds, in particular, at >4V range. The extent of interfacial stability is correlated with the type of cationic and anionic species in the solid electrolyte compound, a fact supported by theoretical prediction and yet, not accurately measured in composite cathode mixtures. By altering the architecture of cathode into a dense additive-free structure, we have identified differences in interfacial stability of chloride compounds which are hidden in composite cathode formats. In this work, we report the use of dense cathode to track the electrochemical evolution of interface between a hybrid halide solid electrolyte composed of chloride and fluoride species. Introducing fluoride compounds is known to be a promising method to expand the oxidation stability while the nature of such expansion is found to be related to kinetics rather than thermodynamics, we report. Furthermore, fluorination of solid electrolyte is generally accompanied with loss of ionic conductivity due to strong electronegative fluoride ions. We demonstrate a fundamental change of solid-state battery assembly from conventional electrolyte pelletizing followed by electrode placement, to a bottom-up assembly route starting with dense cathode, thin (<20µm) layer of SE and anode addition, which compensates for the suppressed conductivity of fluorinated halide solid electrolytes. Through extensive characterization, compositional optimization, and electrochemical interfacial analysis, we demonstrate stable cycling of LiCoO2/hybrid halide solid electrolyte up to 4.4V vs. Li. Our findings pave the way for expanding the voltage stability of solid electrolytes without compromising the cell performance due to ionic conductivity overpotential issues.
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Wu, Ming, Gaozhan Liu, and Xiayin Yao. "Oxygen doped argyrodite electrolyte for all-solid-state lithium batteries." Applied Physics Letters 121, no. 20 (November 14, 2022): 203904. http://dx.doi.org/10.1063/5.0114275.
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Highly conductive argyrodite electrolytes are considered to be one of the most prospective solid electrolytes for all-solid-state batteries. However, poor electrochemical compatibility with a Li anode restrains their application. Herein, oxygen doping is adopted to improve the chemical and electrochemical performance of the argyrodite electrolyte. Meanwhile, the Cl−/S2− ratio is increased to enhance the lithium ionic conductivity. The resultant Li6.05PS4.9O0.1Cl1.05 electrolyte exhibits a high conductivity of 7.49 mS cm−1. Benefitting from the stable Li3OCl formed at the electrolyte/Li interface and the low electronic conductivity arising from the oxygen doping, a Li6.05PS4.9O0.1Cl1.05 electrolyte shows excellent interfacial stability and lithium dendrites suppression capability. A Li/Li6.05PS4.9O0.1Cl1.05/Li cell can maintain stable Li plating/stripping for 13 000 h at 0.1 mA cm−2. Moreover, a high critical current density up to 1.3 mA cm−2 of Li6.05PS4.9O0.1Cl1.05 is realized. Consequently, the LiCoO2/Li6.05PS4.9O0.1Cl1.05/Li batteries achieve remarkable better cycling stability than that using pristine Li6PS5Cl, possessing a reversible capacity of 104.6 mAh g−1 at 1C with a capacity retention of 86.7% after 300 cycles.
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Hou, Wangshu, Yanfang Zhai, Zongyuan Chen, Chengyong Liu, Chuying Ouyang, Ning Hu, Xiao Liang, Peerasak Paoprasert, and Shufeng Song. "Fluorine-regulated cathode electrolyte interphase enables high-energy quasi-solid-state lithium metal batteries." Applied Physics Letters 122, no. 4 (January 23, 2023): 043903. http://dx.doi.org/10.1063/5.0134474.
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Lithium metal batteries (LMBs) enabled by quasi-solid electrolytes are under consideration for their prospect of reliable safety and high energy density. The limited oxidative stabilization and inferior chemical compatibility of quasi-solid electrolytes toward high-voltage cathodes are a long-standing challenge. Herein, we report that an additive level (0.05 M) of LiPF6 is introduced to a polymeric concentrated quasi-solid electrolyte (10 M LiFSI in poly-1,3-dioxolane [poly-DOL], ethylene carbonate [EC], and ethyl methyl carbonate [EMC]) to build in situ a fluorine-regulated cathode electrolyte interphase (CEI) on a highly catalytic LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode. The CEI with a conformal thickness of ∼7 nm features a fluorine-rich outer layer and manipulative LiF/organofluorine species, which mitigates the detrimental side reactions between the quasi-solid electrolyte and NCM cathode and maintains the structure of cycled NCM, as demonstrated by the characterizations of SEM, TEM, XRD, Raman spectroscopy, AFM, EDS, and XPS. As a result, the LiPF6-contained polymeric concentrated quasi-solid electrolyte not only provides a superior ionic conductivity of 3.1 × 10−4 S cm−1 at 25 °C and a remarkable electrochemical stability window of 5.5 V vs Li/Li+, but also achieves an excellent capacity retention of 74% after 100 cycles for LiǁNCM811 quasi-solid-state LMB, bringing a quasi-solid electrolyte design strategy of engineered CEI chemistry for LMBs.
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Yan, Yingchun, Zheng Liu, Xinhou Yang, and Zhuangjun Fan. "Multilayer composite nanofibrous film accelerates the Li+ diffusion for quasi-solid-state lithium-ion batteries." IOP Conference Series: Earth and Environmental Science 1171, no. 1 (April 1, 2023): 012034. http://dx.doi.org/10.1088/1755-1315/1171/1/012034.
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Abstract The rational design of dense and flexible solid-state electrolytes (SSEs) with interface compatibility is still challenging. Here, we report a three-layer dense 3D nanofibrous matrix (PCOF) by constructing a nanofiber framework combining polyacrylonitrile (PAN) and fast Li-ion conductor covalent organic frameworks (COFs) by electrospinning method. PCOF film can maintain an extraordinary electrolyte/electrode interface and an interconnected ion-conduction pathway, accelerating Li+ diffusion. The PCOF quasi-solid-state electrolyte (QSSE) has high oxidative stability (4.70 V, versus Li+/Li) and ion conductivity of 2.94×10−4 S cm−1 at room temperature. Lithium-ion battery based on PCOF QSSE with LiFPO4 (LFP) cathode exhibits outstanding rate characteristics and cycling stability. This multi-layer composite strategy will start a new area of QSSEs lithium-ion electrolytic devices, and simultaneously accelerate the design of electrolytes featuring a wide range of properties.
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Park, Haeseok, Jiwhan Lee, Da Young Ko, and Hansu Kim. "Stable Anodeless Solid-State Batteries Enabled by Carbon-Metal Based Artificial Interface." ECS Meeting Abstracts MA2023-01, no. 4 (August 28, 2023): 861. http://dx.doi.org/10.1149/ma2023-014861mtgabs.
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Anodeless system maximizes all-solid-state batteries’ advantages of energy density and stability. Sulfide-based solid electrolytes exhibit high ionic conductivity and processability, but the narrow electrochemical stability window causes electrolyte decomposition. A preferential strategy to suppress electrolyte decomposition is limiting contact area between lithium metal and electrolyte by the introduction of protective layer, such as carbon-metal layer, between the current collector and the sulfide-based electrolyte layer is one example. In this presentation, we report protective capability of carbon only layer and carbon-metal layer using various electrochemical and analytical characterization technics. Cross sectional images of charged, discharged state of these two anodeless systems demonstrate carbon-metal layer could regulate the site for lithium plating and spatially separate the solid state electrolyte and lithium deposited layer. From these results, we will discuss the key parameters for stable operation of Li metal free anode for all solid-state battery systems.
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Park, Habin, Anthony Engler, Nian Liu, and Paul Kohl. "Dynamic Anion Delocalization of Single-Ion Conducting Polymer Electrolyte for High-Performance of Solid-State Lithium Metal Batteries." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 227. http://dx.doi.org/10.1149/ma2022-023227mtgabs.
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Lithium metal batteries (LMBs) have been considered as next-generation energy storages due to their extremely high theoretical specific capacity (3860 mAh g-1). However, current LMBs, using conventional liquid electrolytes, still could not fulfill the demand of soaring expansion of energy era, such as electrical vehicles, because of their safety issues, originated by uncontrollable electrolytic side reaction on the lithium, resulting unstable solid-electrolyte interphase (SEI) and vicious lithium dendritic growth [1]. Also, carbonate-based liquid electrolytes have an intrinsic flammability, and the lithium dendrite, which short-circuits a cell, can lead to severe safety hazard with the unfavorable flammability of current liquid system when they are ignited. Therefore, solid-state electrolytes have been spotlighted recently for a pathway for safe, and high energy and power LMBs, due to their superior thermal stability and low vapor pressure, while maintaining suitable electrolytic performances. In this study, solid-state single-ion conducting polymer electrolytes (SICPEs), utilizing dynamic anion delocalization (DAD), realizing high ionic conductivity and dimensional stability for high-performance LMB, are studied. The SICPEs enable superior lithium transference number, resulting in highly reduced concentration gradient of lithium cation along the electrolyte to suppress the undesirable lithium dendritic growth. However, SICPEs have prominently lower ionic conductivity than dual-ion conducting polymer electrolyte (DICPEs), which is a critical issue to make a slower charge/discharge for SICPEs [2]. Although an approach utilizing gel polymer electrolyte (GPE), using a liquid solvent as a plasticizer, has been exploited to increase the ionic conductivity of SICPEs, GPEs have struggled with lower mechanical stability, compared to solid state, and still existing flammability issue with the plasticizer. The novel plasticizer, which is described here, can interact with bulky anionic polymer matrix, so that the negative charge can be dispersed onto the whole complex by DAD. Once the bulky complex is formed by DAD, the dissociation of lithium cation from anionic matrix can be easier with the decreased activation energy and higher ionic conduction. While increasing the ionic conductivity with DAD, the nature of polymeric plasticizer will highly suppress flammability. DAD allows the membrane endure more tensile strength due to the dynamic structural change in crosslinking state, so that the polymer electrolyte can tolerate dendritic growth of lithium by morphological change on an electrode surface. The obvious advantages of DAD-induced solid polymer electrolytes in this study for a high energy and power, and ultra-safe LMB can present a novel approach of polymer electrolyte design to the astronomical demand of energy storages. [1] F. Ahmed, I. Choi, M.M. Rahman, H. Jang, T. Ryu, S. Yoon, L. Jin, Y. Jin, W. Kim, ACS Appl. Mater. Interfaces 2019, 11, 34930-34938. [2] D.-M. Shin, J.E. Bachman, M.K. Taylor, J. Kamcev, J.G. Park, M.E. Ziebel, E. Velasquez, N.N. Jarenwattananon, G.K. Sethi, Y. Cui, J.R. Long, Adv. Mater. 2020, 32, 1905771.
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Burazer, Sanja, and Jasminka Popović. "Mechanochemical Synthesis of Solid-State Electrolytes." Inorganics 12, no. 2 (February 6, 2024): 54. http://dx.doi.org/10.3390/inorganics12020054.
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In recent decades, the field of materials research has put significant emphasis on developing innovative platforms that have the potential to address the increasing global energy demand. Batteries have demonstrated their enormous effectiveness in the context of energy storage and consumption. However, safety issues associated with liquid electrolytes combined with a low abundance of lithium in the Earth’s crust gave rise to the development of solid-state electrolytes and cations other than lithium. The commercial production of solid-state batteries demands the scaling up of solid-state electrolyte syntheses as well as the mixing of electrode composites containing solid electrolytes. This review is motivated by the recent literature, and it gives a thorough overview of solid-state electrolytes and highlights the significance of the employed milling and dispersing procedures for the resulting ionic transport properties.
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Tron, Artur, Raad Hamid, Ningxin Zhang, and Alexander Beutl. "Rational Optimization of Cathode Composites for Sulfide-Based All-Solid-State Batteries." Nanomaterials 13, no. 2 (January 12, 2023): 327. http://dx.doi.org/10.3390/nano13020327.
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All-solid-state lithium-ion batteries with argyrodite solid electrolytes have been developed to attain high conductivities of 10−3 S cm−1 in studies aiming at fast ionic conductivity of electrolytes. However, no matter how high the ionic conductivity of the electrolyte, the design of the cathode composite is often the bottleneck for high performance. Thus, optimization of the composite cathode formulation is of utmost importance. Unfortunately, many reports limit their studies to only a few parameters of the whole electrode formulation. In addition, different measurement setups and testing conditions employed for all-solid-state batteries make a comparison of results from mutually independent studies quite difficult. Therefore, a detailed investigation on different key parameters for preparation of cathodes employed in all-solid-state batteries is presented here. Employing a rational approach for optimization of composite cathodes using solid sulfide electrolytes elucidated the influence of different parameters on the cycling performance. First, powder electrodes made without binders are investigated to optimize several parameters, including the active materials’ particle morphology, the nature and amount of the conductive additive, the particle size of the solid electrolyte, as well as the active material-to-solid electrolyte ratio. Finally, cast electrodes are examined to determine the influence of a binder on cycling performance.
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Ozdogru, Bertan, and Omer Ozgur Özgür Capraz. "In Situ Strain Measurements on LAGP Solid Electrolyte in Symmetrical Li/LAGP/Li Battery during Li Plating and Stripping." ECS Meeting Abstracts MA2022-01, no. 37 (July 7, 2022): 1631. http://dx.doi.org/10.1149/ma2022-01371631mtgabs.
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Solid electrolytes have potential to dramatically improve energy density of batteries for demanding applications such as electrical vehicles by allowing the utilization of high energy density-Li metal anodes. However, harvesting the benefits of the solid electrolytes for Li-metal batteries is limited to due to interfacial instabilities, dendrite formation and large impedance. Chemo-mechanical deformations in the electrode- solid electrolyte interface are still the bottleneck to improve performance of solid-state batteries. Investigation of the solid electrolyte - electrode interface during battery cycling is must to elucidate the governing forces behind the deformations and associated electrochemical performance loss in all-solid-state batteries. Various in situ characterization techniques such as Micro CT, XPS, and TEM have provided crucial information about the deformation mechanisms in the solid electrolyte1. In this study, we utilized digital image correlation (DIC) to monitor chemo-mechanical deformations in solid-state batteries during battery cycling. DIC computes strains with spatial and temporal resolution by tracking the changes in the speckle patterns in small neighborhoods called subsets during deformation2. In situ strain measurements previously utilized to investigate the driving forces behind the structural and interfacial instabilities in alkali metal-ion battery electrodes3,4. A custom cell was designed to operate in operando strain measurements on solid electrolytes while cycling the all-solid-state battery. Shortly, symmetrical Li | LAGP | Li cells were fabricated, and stainless-steel disks were used as a current collector. Li1.5,Al0.5Ge1.5P3O12 (LAGP) powder was used to prepare LAGP solid electrolyte. In order to obtain a flat surface for the DIC measurements, the solid electrolyte was cut in half to obtain a semi-circle. Carbon black was used to decorate the flat side of the solid electrolyte as speckle pattern. In situ strain measurements demonstrated the impact of the early non-uniform deformations on the spatial distribution of Li plating and stripping on the solid electrolyte – electrode interface. The strain measurements provided quantitative analysis of the mechanical deformations and its coupling with the electrochemical behavior of the symmetrical battery cell. The measurements demonstrated the correlation between mechanical deformation in Li anode – LAGP interphase and the overpotential. Large amount of deformations in the center of the LAGP electrolyte was recorded at higher current densities and the fracture in the solid electrolyte was verified with ex-situ Micro-CT measurement. In this talk, we will present the spatial and temporal distribution of the strains in the LAGP solid electrolyte during battery cycling and we will discuss its coupling with the electrochemical performance. Acknowledgement: This work was supported by the NASA EPSCoR Research Initiation Grant. We are grateful for the valuable discussions with Dr. Behrad Koohbor and Dr. James Wu. References: Lewis, J. A., Tippens, J., Cortes, F. J. Q. & McDowell, M. T. Chemo-Mechanical Challenges in Solid-State Batteries. Trends Chem. 1, 845–857 (2019). Sutton, M., Mingqi, C., Peters, W., Chao, Y. & McNeill, S. Application of an optimized digital correlation method to planar deformation analysis. Image Vis. Comput. 4, 143–150 (1986). Jones, E. M. C., Çapraz, Ö. Ö., White, S. R. & Sottos, N. R. Reversible and Irreversible Deformation Mechanisms of Composite Graphite Electrodes in Lithium-Ion Batteries. J. Electrochem. Soc. 163, A1965–A1974 (2016). Özdogru, B. et al. In Situ Probing Potassium-Ion Intercalation-Induced Amorphization in Crystalline Iron Phosphate Cathode Materials. Nano Lett. (2021). doi:10.1021/acs.nanolett.1c02095
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Dolle, Mickael, Lea Caradant, Nina Verdier, Gabrielle Foran, Paul Nicolle, David Lepage, Arnaud Prébé, and David Aymé-Perrot. "(Invited) Polymer Blends As Electrolytes in All-Solid-State Batteries." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 994. http://dx.doi.org/10.1149/ma2023-016994mtgabs.
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Advantages of polymer electrolytes include material flexibility, good interfacial compatibility and easy processability. However, these materials typically possess room temperature ionic conductivities, oxidation stability windows and mechanical strengths that are too low for them to be useful electrolyte materials in all-solid-state batteries (ASSB). One reason for this is that polymer properties that favor improved ionic conductivity such as high polymer chain mobility are generally not compatible with good mechanical strength making these properties difficult to optimize simultaneously. One strategy that has been investigated to this effect is polymer blending. The idea is that polymers with good ionic conductivity can be blended with thermoplastic or elastomeric materials that have high mechanical resistance to create a new electrolyte material with the properties of its combined parts. In this work, polymers with good ionic conductivity were combined with thermoplastic materials with high mechanical strength via melt processing methods to yield solid polymer electrolytes. The resultant electrolyte materials show promising results when implemented in composite electrodes and electrolytes for use in ASSB which will be discussed in this talk.
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Tan, Feihu, Hua An, Ning Li, Jun Du, and Zhengchun Peng. "Stabilization of Li0.33La0.55TiO3 Solid Electrolyte Interphase Layer and Enhancement of Cycling Performance of LiNi0.5Co0.3Mn0.2O2 Battery Cathode with Buffer Layer." Nanomaterials 11, no. 4 (April 12, 2021): 989. http://dx.doi.org/10.3390/nano11040989.
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All-solid-state batteries (ASSBs) are attractive for energy storage, mainly because introducing solid-state electrolytes significantly improves the battery performance in terms of safety, energy density, process compatibility, etc., compared with liquid electrolytes. However, the ionic conductivity of the solid-state electrolyte and the interface between the electrolyte and the electrode are two key factors that limit the performance of ASSBs. In this work, we investigated the structure of a Li0.33La0.55TiO3 (LLTO) thin-film solid electrolyte and the influence of different interfaces between LLTO electrolytes and electrodes on battery performance. The maximum ionic conductivity of the LLTO was 7.78 × 10−5 S/cm. Introducing a buffer layer could drastically improve the battery charging and discharging performance and cycle stability. Amorphous SiO2 allowed good physical contact with the electrode and the electrolyte, reduced the interface resistance, and improved the rate characteristics of the battery. The battery with the optimized interface could achieve 30C current output, and its capacity was 27.7% of the initial state after 1000 cycles. We achieved excellent performance and high stability by applying the dense amorphous SiO2 buffer layer, which indicates a promising strategy for the development of ASSBs.
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Mukhan, Orynbassar, Ji-Su Yun, and Sung-soo Kim. "Investigation of Interfacial Behavior of Ni-Rich NCM Cathode Particles in Sulfide-Based Solid-State Electrolyte." ECS Meeting Abstracts MA2023-02, no. 60 (December 22, 2023): 2892. http://dx.doi.org/10.1149/ma2023-02602892mtgabs.
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All-solid-state batteries (ASSBs) are currently investigated as a future battery technology with conventional layered cathode materials because they can offer benefits in the gravimetric and volumetric energy densities compared to flammable liquid electrolyte lithium-ion batteries with graphite intercalation anode. The solid electrolyte is believed to suppress dendritic growth and low Coulombic efficiency on the lithium metal anode side, which are the key issues for the use of a lithium metal electrode in conventional batteries with liquid electrolyte. Moreover, layered transition metal oxides such as LiNixCoyMnzO2 (NCM, 0 < x, y, z < 1) are one of the most promising positive electrode active material candidates being developed to increase the energy density. In particular, recent studies have shown a tendency to decrease the cobalt content and increase the nickel content to increase energy density and price competitiveness, so high-nickel NCM can be the optimal material suitable for this purpose. However, the remaining interfacial challenges of the cathode / solid electrolyte interface still need to be solved. Herein, we investigated the kinetics such as charge transfer resistance at the interface between high nickel (Ni0.94) NCM particles and argyrodite (Li6PS5Cl) solid electrolytes using the microcavity electrode with the negative and positive pulsed current measurement technique and compared with liquid electrolytes using the same manner measurement technique. The cavity-electrode system is adopted to analyze the electrochemical properties of active particles and electrolytes confined in the cavity to exclude the effects of surrounding interfaces, barriers, and side reactions caused by battery components around the electrodes and the impact of loading and current collectors of the composite electrode. Therefore, understanding the electrode-electrolyte interface between cathode active particles and solid electrolytes is crucial for theoretical studies on the interfacial phenomenon in solid electrolyte batteries.
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Li, Qinghui, Xiaofen Wang, Linlin Wang, Shyuan Zhu, Qingdong Zhong, Yuanyuan Li, and Qiongyu Zhou. "Li+ Conduction in a Polymer/Li1.5Al0.5Ge1.5(PO4)3 Solid Electrolyte and Li-Metal/Electrolyte Interface." Molecules 28, no. 24 (December 10, 2023): 8029. http://dx.doi.org/10.3390/molecules28248029.
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The solid oxide electrolyte Li1.5Al0.5Ge1.5(PO4)3 (LAGP) with a NASICON structure has a high bulk ionic conductivity of 10−4 S cm−1 at room temperature and good stability in the air because of the strong P5+-O2− covalence bonding. However, the Ge4+ ions in LAGP are quickly reduced to Ge3+ on contact with the metallic lithium anode, and the LAGP ceramic has insufficient physical contact with the electrodes in all-solid-state batteries, which limits the large-scale application of the LAGP electrolyte in all-solid-state Li-metal batteries. Here, we prepared flexible PEO/LiTFSI/LAGP composite electrolytes, and the introduction of LAGP as a ceramic filler in polymer electrolytes increases the total ionic conductivity and the electrochemical stability of the composite electrolyte. Moreover, the flexible polymer shows good contact with the electrodes, resulting in a small interfacial resistance and stable cycling of all-solid-state Li-metal batteries. The influence of the external pressure and temperature on Li+ transfer across the Li/electrolyte interface is also investigated.