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Ping, Weiwei, Chengwei Wang, Ruiliu Wang, Qi Dong, Zhiwei Lin, Alexandra H. Brozena, Jiaqi Dai, Jian Luo, and Liangbing Hu. "Printable, high-performance solid-state electrolyte films." Science Advances 6, no. 47 (November 2020): eabc8641. http://dx.doi.org/10.1126/sciadv.abc8641.
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Current ceramic solid-state electrolyte (SSE) films have low ionic conductivities (10−8 to 10−5 S/cm ), attributed to the amorphous structure or volatile Li loss. Herein, we report a solution-based printing process followed by rapid (~3 s) high-temperature (~1500°C) reactive sintering for the fabrication of high-performance ceramic SSE films. The SSEs exhibit a dense, uniform structure and a superior ionic conductivity of up to 1 mS/cm. Furthermore, the fabrication time from precursor to final product is typically ~5 min, 10 to 100 times faster than conventional SSE syntheses. This printing and rapid sintering process also allows the layer-by-layer fabrication of multilayer structures without cross-contamination. As a proof of concept, we demonstrate a printed solid-state battery with conformal interfaces and excellent cycling stability. Our technique can be readily extended to other thin-film SSEs, which open previously unexplores opportunities in developing safe, high-performance solid-state batteries and other thin-film devices.
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Isarraras, Gustavo, Tung Dang, Dirar Mashaleh, Michael Oye, Dahyun Oh, and Santosh KC. "Tuning Ionic Conductivity and Stability of Li10GeP2S12 Solid-State Electrolyte." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 212. http://dx.doi.org/10.1149/ma2022-012212mtgabs.
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All-solid-state Li-ion batteries gained a huge attention because they exhibit higher power density, wider electrochemical stability windows, and overall safety of solid-state electrolytes (SSE) compared to conventional liquid electrolyte-based batteries. Unfortunately, most of the SSE materials have not matched the ionic conductivity of their liquid counterpart. But, recent research and the synthesis of new materials have shown SSE can conduct ions at an equivalent or even higher rate. However, the electrochemical stability needs to be improved. There is a growing research effort in identifying a solid electrolyte that is both electrochemically stable and has a very high ionic conductivity. The Li10GeP2S12 (LGPS) is one of the superionic conductors, is known for its high ionic conductivity that can be deployed as a solid electrolyte in batteries. However, LGPS is not stable as exposed to air and moisture, posing challenges during its manufacturing, and designing process. Thus, in an attempt to optimize the stability and ionic conductivity, the effect of antimony (Sb), tin (Sn), and oxygen (O) substitution on conductivity and stability of LGPS is investigated using Density Functional Theory (DFT). The systematic study of compositional variation, phase stability, defects chemistry, and the impact on electronic properties and ionic conductivity is performed. Thus, this study will provide significant insights on ion conduction mechanisms and strategies that can tune the ionic conductivity and stability of LGPS based electrolytes. This project was supported in part by COE SJSU, DOE NERSC, and XSEDE.
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Hu, Shengyi, and Chun Huang. "Machine-Learning Approaches for the Discovery of Electrolyte Materials for Solid-State Lithium Batteries." Batteries 9, no. 4 (April 17, 2023): 228. http://dx.doi.org/10.3390/batteries9040228.
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Solid-state lithium batteries have attracted considerable research attention for their potential advantages over conventional liquid electrolyte lithium batteries. The discovery of lithium solid-state electrolytes (SSEs) is still undergoing to solve the remaining challenges, and machine learning (ML) approaches could potentially accelerate the process significantly. This review introduces common ML techniques employed in materials discovery and an overview of ML applications in lithium SSE discovery, with perspectives on the key issues and future outlooks.
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Liu, Junlong, Tao Wang, Jinjian Yu, Shuyang Li, Hong Ma, and Xiaolong Liu. "Review of the Developments and Difficulties in Inorganic Solid-State Electrolytes." Materials 16, no. 6 (March 21, 2023): 2510. http://dx.doi.org/10.3390/ma16062510.
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All-solid-state lithium-ion batteries (ASSLIBs), with their exceptional attributes, have captured the attention of researchers. They offer a viable solution to the inherent flaws of traditional lithium-ion batteries. The crux of an ASSLB lies in its solid-state electrolyte (SSE) which shows higher stability and safety compared to liquid electrolyte. Additionally, it holds the promise of being compatible with Li metal anode, thereby realizing higher capacity. Inorganic SSEs have undergone tremendous developments in the last few decades; however, their practical applications still face difficulties such as the electrode–electrolyte interface, air stability, and so on. The structural composition of inorganic electrolytes is inherently linked to the advantages and difficulties they present. This article provides a comprehensive explanation of the development, structure, and Li-ion transport mechanism of representative inorganic SSEs. Moreover, corresponding difficulties such as interface issues and air stability as well as possible solutions are also discussed.
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Bistri, Donald, and Claudio V. Di Leo. "A Thermodynamically Consistent, Phase-Field Electro-Chemo-Mechanical Theory with Account for Damage in Solids: Application to Metal Filament Growth in Solid-State Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 523. http://dx.doi.org/10.1149/ma2022-024523mtgabs.
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Solid-state batteries (SSBs) present a promising technology and have attracted significant research attention owing to their superior properties including increased energy density (3860 mAh), wider electrochemical window (0-5V) and safer electrolyte design. From a safety standpoint, SSBs are particularly appealing in that replacement of flammable conventional organic electrolytes with highly conductive, mechanically stiff inorganic solid-state electrolytes (SSEs) can alleviate failure due to short circuit or ignition. However, operation of SSBs is hampered by numerous chemo-mechanical challenges [1 - 4], the most critical one associated with metal filament growth across the SSE. Filament protrusions can initiate at perturbations of the interface or microstructural heterogeneities and subsequently grow through the SSE, causing the battery to short-circuit. It is critical to understand from both an experimental and modeling perspective the interplay of various mechanisms including morphology of the SSE microstructure, elastic-viscoplastic behavior of Li-metal, critical current density and stack pressure on the morphology of filamentary protrusions across the SSE. While much has been done to understand the interplay of aforementioned mechanisms from an experimental standpoint [5,6], theoretical frameworks on modeling of filaments growth in SSBs are still at their infancy and typically simplify dendrites as pressurized cracks under a linear-elastic fracture mechanics (LEFM) approach [7-8]. In this work, we propose a thermodynamically consistent phase-field reaction-diffusion-damage theory to investigate the morphology of filament growth across the SSE under varying chemo-mechanical operational conditions. The theory is fully coupled with electrodeposition at the Li metal-SSE interface impacting mechanical deformation, stress generation and subsequent fracture of the SSE. Conversely, electrodeposition kinetics are affected by mechanical stresses through a thermodynamically consistent, physically motivated driving force that distinguishes the role of various chemical, electrical and mechanical contributions. Concurrently, the theory captures the interplay between crack propagation and electrodeposition phenomena by tracking the damage and reaction field using separate phase-field variables such that metal growth is preceded by and confined to damaged regions within the SSE accessible by Li-metal. This is a critical feature of the theory and confirms experimental observations that the crack front propagates ahead of Li. We specialize the theory and study the role of variations of chemo-mechanical properties (i.e. applied electric potential, SSE fracture energy) on the morphology of metal filament growth and map operational conditions to distinguish between domains of i) stable vs. unstable growth ii) intergranular vs. transgranular growth mode. In doing so, the proposed framework provides a quantitative understanding on mechanisms dictating metal filament growth in SSEs and identifies mitigation strategies to employ in future SSB designs for successful operation. References: [1] Zhang, Fangzhou, et al. "A review of mechanics-related material damages in all-solid-state batteries: Mechanisms, performance impacts and mitigation strategies." Nano Energy 70 (2020): 104545. [2] Bistri, Donald, Arman Afshar, and Claudio V. Di Leo. "Modeling the chemo-mechanical behavior of all-solid-state batteries: a review." Meccanica 56.6 (2021): 1523-1554. [3] Wang, Peng, et al. "Electro–chemo–mechanical issues at the interfaces in solid‐state lithium metal batteries." Advanced Functional Materials 29.27 (2019): 1900950 [4] Bistri, Donald, and Claudio V. Di Leo. "Modeling of Chemo-Mechanical Multi-Particle Interactions in Composite Electrodes for Liquid and Solid-State Li-Ion Batteries." Journal of The Electrochemical Society 168.3 (2021): 030515. [5] Ren, Yaoyu, et al. "Direct observation of lithium dendrites inside garnet-type lithium-ion solid electrolyte." Electrochemistry Communications 57 (2015): 27-30. [6] Cheng, Eric Jianfeng, Asma Sharafi, and Jeff Sakamoto. "Intergranular Li metal propagation through polycrystalline Li6. 25Al0. 25La3Zr2O12 ceramic electrolyte." Electrochimica Acta 223 (2017): 85-91. [7] Klinsmann, Markus, et al. "Dendritic cracking in solid electrolytes driven by lithium insertion." Journal of Power Sources 442 (2019): 227226. [8] Bucci, Giovanna, and Jake Christensen. "Modeling of lithium electrodeposition at the lithium/ceramic electrolyte interface: the role of interfacial resistance and surface defects." Journal of Power Sources 441 (2019): 227186.
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Kalutara Koralalage, Milinda, Varun Shreyas, William Richard Arnold, Sharmin Akter, Arjun Thapa, Jacek Bogdan Jasinski, Gamini Sumanasekera, Hui Wang, and Badri Narayanan. "Quasi-Solid-State Lithium-Sulfur Batteries Consist of Super P – Sulfur Composite Cathode." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 541. http://dx.doi.org/10.1149/ma2022-024541mtgabs.
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Lithium-Sulfur (Li-S) batteries stand out to be one of the most promising candidates to meet the current energy storage requirement, with its natural abundance of materials, high theoretical capacity of 1672 mAhg-1, high energy density of 2600 Whkg-1, and low cost and lower environmental impact. Sulfur itself (S8), Li2S2 and Li2S formed during the discharge process, are electrical insulators and hence reduce the active material utilization and the electronic conductivity of the cathode affecting the battery performance. Combining of Carbon Super P (SP) with sulfur in cathode formulation is used to overcome these issues. In Liquid electrolyte batteries, polysulfides formed while charging and discharging, easily dissolve in liquid electrolyte and the resulting polysulfide shuttling leads to poor coulombic efficiency and cyclability. Liquid electrolytes used in the conventional Li-S batteries are easy to flow and become flammable. Further, Lithium dendrites piercing through separator causing short circuit paths leads to safety concerns. Replacement of the liquid electrolyte by a solid-state electrolyte (SSE) proves to be a strategy to overcome above mentioned issues. Sulfide based solid electrolytes have received greater attention due to their higher ionic conductivity, compatible interface with sulfur-based cathodes, and lower grain boundary resistance. Novel Li6PS5F0.5Cl0.5 due to its remarkable ionic conductivity of 3.5 x 10-4 S cm-1 makes it an excellent candidate for use in a Li-S solid state battery. However, the interface between SSEs and cathodes has become a challenge to be addressed in all solid-state Li-S batteries due to the rigidity of the participating surfaces. A hybrid electrolyte containing of SSE coupled with a small amount of ionic liquid at the interface, has been employed to improve the interface contact of the SSE with the electrodes. Cathode formulation consisting of sulfur as the active material, Super P as the conductive carbon black, acetylene carbon black as conductive carbon additive, with water based carboxymethyl cellulose (CMC) solution and Styrene butadiene rubber (SBR) as the binder was successfully developed. Thermo gravimetric analysis (TGA) studies of the cathode were carried out by the thermo gravimetric analyzer TA 2050 under N2 gas flow of 100 ml/min. Cathode surface morphology was characterized using the Field emission gun scanning electron microscope (FEI), TESCAN scanning electron microscope with energy dispersive X-ray spectroscopy (EDAX). Using a solvent-based process, Li6PS5F0.5Cl0.5 and Li6PS5F0.5Cl2 SSE were synthesized via the introduction of LiF into the argyrodite crystal structure, which enhances both the ionic conductivity and interface-stabilizing properties of the SSE. Relevant Ionic Liquids (IL) were prepared using Lithium bis(trifluoromethyl sulfonyl)imide (LiTFSI) as salt, with premixed pyrrolidinium bis(trifluoromethyl sulfonyl)imide (PYR) as solvent and 1,3-dioxolane (DOL) as diluent. SP-S cathode with 0.70 mgcm-2 sulfur loading was punched into disks of 2.0 cm2. SSE was pressed into 150 mg pellets using a stainless-steel tank. During the assembly, SSE was wetted with total of 40 μl of IL (LiTFSI dissolved in PYR and DOL solution) from both ends using a micropipette. 2032 type coin cells of Quasi-solid-state Li-S batteries (QSSLSB) consisting of SP-S based composite cathodes, Li anodes and novel Li6PS5F0.5Cl0.5 SSE were tested with an ionic liquid wetting both electrode-SSE interfaces. All the QSSLSB were cycled at 30 °C between 1.0 V and 2.8 V using an 8 channel Arbin battery testing system. Effect of IL dilution, co-solvent amount, LiTFSI concentration and C rate at which the batteries are tested, were systematically studied and optimized to develop a QSSLSB with higher capacity retention and cyclability. Optimum batteries had initial discharge capacity >1100 mAh/g and discharge capacity >400 mAh/g after 100 cycles at the C rate of C/10 with a significant coulombic efficiency. 40 μl of LiTFSI (2M) dissolved in PYR:DOL(1:1) IL was found to be optimum for high performance QSSEBs with low sulfur loading of 0.7 mg/cm2. From the C rate performance study QSSEBs have shown improved stability with the higher current rates. Next, cathodes with higher sulfur loading were studied and for sulfur loading > 4 mgcm-2, initial discharge capacity >950 mAh/g and 400 mAh/g after 60 cycles at C/20 rate were achieved with 40 μl of IL consisting of LiTFSI (3M) dissolved in PYR:DOL(1:3) for the SSE Li6PS5F0.5Cl2. Further testing is underway to improve the performance at high C rate for higher loading by incorporating SSE in the cathode to realize QSSLSB with higher capacity with improved cycle retention.
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Fu, Yao, Dangling Liu, Yongjiang Sun, Genfu Zhao, and Hong Guo. "Epoxy Resin-Reinforced F-Assisted Na3Zr2Si2PO12 Solid Electrolyte for Solid-State Sodium Metal Batteries." Batteries 9, no. 6 (June 19, 2023): 331. http://dx.doi.org/10.3390/batteries9060331.
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Solid sodium ion batteries (SIBs) show a significant amount of potential for development as energy storage systems; therefore, there is an urgent need to explore an efficient solid electrolyte for SIBs. Na3Zr2Si2PO12 (NZSP) is regarded as one of the most potential solid-state electrolytes (SSE) for SIBs, with good thermal stability and mechanical properties. However, NZSP has low room temperature ionic conductivity and large interfacial impedance. F−doped NZSP has a larger grain size and density, which is beneficial for acquiring higher ionic conductivity, and the composite system prepared with epoxy can further improve density and inhibit Na dendrite growth. The composite system exhibits an outstanding Na+ conductivity of 0.67 mS cm−1 at room temperature and an ionic mobility number of 0.79. It also has a wider electrochemical stability window and cycling stability.
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Bock, Robert, Morten Onsrud, Håvard Karoliussen, Bruno Pollet, Frode Seland, and Odne Burheim. "Thermal Gradients with Sintered Solid State Electrolytes in Lithium-Ion Batteries." Energies 13, no. 1 (January 3, 2020): 253. http://dx.doi.org/10.3390/en13010253.
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The electrolyte is one of the three essential constituents of a Lithium-Ion battery (LiB) in addition to the anode and cathode. During increasingly high power and high current charging and discharging, the requirement for the electrolyte becomes more strict. Solid State Electrolyte (SSE) sees its niche for high power applications due to its ability to suppress concentration polarization and otherwise stable properties also related to safety. During high power and high current cycling, heat management becomes more important and thermal conductivity measurements are needed. In this work, thermal conductivity was measured for three types of solid state electrolytes: Li 7 La 3 Zr 2 O 12 (LLZO), Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP), and Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) at different compaction pressures. LAGP and LATP were measured after sintering, and LLZO was measured before and after sintering the sample material. Thermal conductivity for the sintered electrolytes was measured to 0.470 ± 0.009 WK − 1 m − 1 , 0.5 ± 0.2 WK − 1 m − 1 and 0.49 ± 0.02 WK − 1 m − 1 for LLZO, LAGP, and LATP respectively. Before sintering, LLZO showed a thermal conductivity of 0.22 ± 0.02 WK − 1 m − 1 . An analytical temperature distribution model for a battery stack of 24 cells shows temperature differences between battery center and edge of 1–2 K for standard liquid electrolytes and 7–9 K for solid state electrolytes, both at the same C-rate of four.
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Yang, Guang, Yuxuan Zhang, Ethan Self, Teerth Brahmbhatt, Jean-Christophe Bilheux, Hassina Bilheux, and Jagjit Nanda. "(Invited) Initial Capacity Loss Mechanism of All-Solid-State Lithium Sulfide Battery Unraveled By in Situ Neutron Tomography." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 205. http://dx.doi.org/10.1149/ma2022-012205mtgabs.
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All-solid-state lithium metal batteries promise a specific energy >500 Wh/kg. A solid-state electrolyte (SSE) plays an irreplaceable role in reaching such an energy density goal. Among different SSE types, the sulfide and thiophosphate-based SSE has emerged as a prominent class of soft ionic conductors. Compared to their ceramic and oxide SSE counterparts, sulfide SSEs provide several favorable advantages, including a) high room temperature ionic conductivity up to 10 mS/cm that is comparable to liquid-based electrolytes; b) ductile and mechanically soft SSE that enables better processible and intimate contact with electrodes; and c) scalability with solution-based low-temperature synthesis route. However, when paring with a high voltage cathode, such as lithium nickel manganese cobalt oxide (NMC), the (electro)chemical instability of the sulfide SSE at the electrode/SSE interfaces becomes a major challenge to tackle with. The interfacial instability can result in up to 50% initial capacity loss in a Li/sulfide SSE/NMC battery, thereby keeping the sulfide SSEs from commercialization. Herein, by using neutron computed tomography, we trace in situ lithium displacement in an all-solid-state battery composed of a 7Li anode, natLi3PS4(LPS) electrolyte, and a natLiNi0.8Mn0.1Co0.1O2 (NMC811) cathode. We show that after the first galvanostatic charge/discharge cycle, lithium accumulates at the LPS/NMC811 interface and preferably fills in the pre-formed cracks in the cold-pressed LPS SSE pellet. Such irreversible lithium displacement contributes to the initial capacity loss of the Li/LPS/NMC battery. Our findings suggest that to achieve high-capacity retention of an all-solid-state sulfide-based battery using an NMC cathode, the cathode/sulfide interface should be better engineered and the defects of the LPS pellet should be suppressed. Acknowledgment This research was conducted at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) and is supported by Asst. Secretary, Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (VTO) through the Advanced Battery Materials Research (BMR) Program. This research used resources at High Flux Isotope Reactor, a DOE Office of Science User Facilities operated by the Oak Ridge National Laboratory.
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Ryu, Kun, Kyungbin Lee, Hyun Ju, Jinho Park, Ilan Stern, and Seung Woo Lee. "Ceramic/Polymer Hybrid Electrolyte with Enhanced Interfacial Contact for All-Solid-State Lithium Batteries." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2621. http://dx.doi.org/10.1149/ma2022-0272621mtgabs.
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All solid-state lithium batteries (ASSLBs) with a high energy density are challenging, yet desired by the rising energy demands. Its intrinsic safety of solid-state electrolytes (SSEs) compared to flammable liquid electrolytes makes ASSLBs a modern-day necessity. NASICON-type Li1.5Al0.5Ge1.5P3O12 (LAGP) has high ionic conductivity, high stability against air and water, and a wide electrochemical window. However, the application of LAGP is significantly hindered by its slow interfacial kinetics and brittle nature. In addition, the ionic conductivity of LAGP is relatively low at room temperature compared to that obtained at elevated temperatures. In our study, LAGP was incorporated into a polymer matrix to accelerate charge transport at the electrode-electrolyte interface to form LAGP-poly-DOL (LAGP-pDOL) hybrid electrolyte. The in-situ cationic ring-opening polymerization of DOL decreases the interfacial contact impedance and improves the mechanical properties of the SSE. LAGP-pDOL electrolyte exhibits prolonged cycle stability in symmetric cells (> 200 h) and in Li|LiFePO4 full cells (99% retention after 50 cycles) at room temperature. This study demonstrates the effective utilization of conductive polymer matrix into LAGP to enhance mechanical strength, interfacial contact, and room temperature electrochemical performance.
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Stegmaier, Sina, Karsten Reuter, and Christoph Scheurer. "Exploiting Nanoscale Complexion in LATP Solid-State Electrolyte via Interfacial Mg2+ Doping." Nanomaterials 12, no. 17 (August 24, 2022): 2912. http://dx.doi.org/10.3390/nano12172912.
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While great effort has been focused on bulk material design for high-performance All Solid-State Batteries (ASSBs), solid-solid interfaces, which typically extend over a nanometer regime, have been identified to severely impact cell performance. Major challenges are Li dendrite penetration along the grain boundary network of the Solid-State Electrolyte (SSE) and reductive decomposition at the electrolyte/electrode interface. A naturally forming nanoscale complexion encapsulating ceramic Li1+xAlxTi2−x(PO4)3 (LATP) SSE grains has been shown to serve as a thin protective layer against such degradation mechanisms. To further exploit this feature, we study the interfacial doping of divalent Mg2+ into LATP grain boundaries. Molecular Dynamics simulations for a realistic atomistic model of the grain boundary reveal Mg2+ to be an eligible dopant candidate as it rarely passes through the complexion and thus does not degrade the bulk electrolyte performance. Tuning the interphase stoichiometry promotes the suppression of reductive degradation mechanisms by lowering the Ti4+ content while simultaneously increasing the local Li+ conductivity. The Mg2+ doping investigated in this work identifies a promising route towards active interfacial engineering at the nanoscale from a computational perspective.
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Cui, Yufan. "Simulation of Li3HoCl6 Solid-state Lithium Batteries Based on COSMOL Multiphysics." Journal of Physics: Conference Series 2393, no. 1 (December 1, 2022): 012014. http://dx.doi.org/10.1088/1742-6596/2393/1/012014.
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Abstract The rapid development of portable smart devices and electric vehicles is placing greater demands on the energy density and safety of rechargeable secondary batteries. Lithium-ion batteries using the Solid State Electrolyte (SSE) are considered to be the most promising direction to achieve these goals. Among the latest electrolyte developments, chloride solid electrolytes have attracted much attention due to their physicochemical properties such as high ionic conductivity, ease of deformation and oxidative stability. In this paper, a one-dimensional model of a solid-state Li3HoCl6 battery is proposed based on COSMOL Multiphysics multi-physics field simulation software, and the charge-discharge curves and lithium-ion concentration variation curves at different discharge rates are obtained. The results show that the battery has a stable potential and relatively high-capacity density at low C rates (1.8C~14.4C). Therefore, it has application values at low currents and space for improvement at high currents.
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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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Yu, Zhaoxin, and Dongping Lu. "Highly Conductive Sulfide Solid-State Electrolytes for All-Solid-State Li Battery." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2450. http://dx.doi.org/10.1149/ma2022-0272450mtgabs.
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The All-Solid-State Battery (ASSB) Is a Promising Next-Generation Energy Storage Technology for Both Consumer Electronics and Electric Vehicles Because of Its High Energy Density and Improved Safety. Sulfide Solid-State Electrolytes (SSEs) Have Merits of Low Density, High Ionic Conductivity, and Favorable Mechanical Properties Compared to Oxide Ceramic and Polymer Materials. However, Mass Production and Processing of Sulfide SSEs Remain a Grand Challenge Because of Their Poor Moisture Stability. Here We Report a Reversible Surface Coating Strategy for Enhancing the Moisture Stability of Sulfide Sses By Using Amphipathic Organic Molecules. an Ultra-Thin Layer of 1-Bromopentane Is Coated on the Sulfide SSE Surface (e.g., Li7P2S8Br0.5I0.5) Via Van Der Waals Force. 1-Bromopentane Has More Negative Adsorption Energy with SSE Than H2O Based on First-Principles Calculations, Thereby Enhancing the Moisture Stability of SSE Because the Hydrophobic Long-Chain Alkyl Tail of 1-Bromopentane Repels Water Molecules. Moreover, This Amphipathic Molecular Layer Has a Negligible Effect on Ionic Conductivity and Can be Removed Reversibly By Heating at Low Temperatures (e.g., 160°C). This Finding Opens a New Pathway for the Surface Engineering of Moisture-Sensitive SSEs and Other Energy Materials, Thereby Speeding up Their Deployment in ASSBs.
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Yuan, Boheng, Bin Zhao, Zhi Cong, Zhi Cheng, Qi Wang, Yafei Lu, and Xiaogang Han. "A Flexible, Fireproof, Composite Polymer Electrolyte Reinforced by Electrospun Polyimide for Room-Temperature Solid-State Batteries." Polymers 13, no. 21 (October 20, 2021): 3622. http://dx.doi.org/10.3390/polym13213622.
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Solid-state batteries (SSBs) have attracted considerable attention for high-energy-density and high-safety energy storage devices. Many efforts have focused on the thin solid-state-electrolyte (SSE) films with high room-temperature ionic conductivity, flexibility, and mechanical strength. Here, we report a composite polymer electrolyte (CPE) reinforced by electrospun PI nanofiber film, combining with succinonitrile-based solid composite electrolyte. In situ photo-polymerization method is used for the preparation of the CPE. This CPE, with a thickness around 32.5 μm, shows a high ionic conductivity of 2.64 × 10−4 S cm−1 at room temperature. It is also fireproof and mechanically strong, showing great promise for an SSB device with high energy density and high safety.
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Fujishiro, Miki, Ryoichi Tatara, Kazuhide Ueno, Masayoshi Watanabe, and Kaoru Dokko. "Li-Ion Transport in Three-Layer Electrolyte of Ionic Liquid/Solid-State Electrolyte (SSE)/Ionic Liquid." ECS Meeting Abstracts MA2020-02, no. 68 (November 23, 2020): 3444. http://dx.doi.org/10.1149/ma2020-02683444mtgabs.
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Hu, Qianyu, Kunfeng Chen, Fei Liu, Mengying Zhao, Feng Liang, and Dongfeng Xue. "Smart Materials Prediction: Applying Machine Learning to Lithium Solid-State Electrolyte." Materials 15, no. 3 (February 2, 2022): 1157. http://dx.doi.org/10.3390/ma15031157.
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Traditionally, the discovery of new materials has often depended on scholars’ computational and experimental experience. The traditional trial-and-error methods require many resources and computing time. Due to new materials’ properties becoming more complex, it is difficult to predict and identify new materials only by general knowledge and experience. Material prediction tools based on machine learning (ML) have been successfully applied to various materials fields; they are beneficial for modeling and accelerating the prediction process for materials that cannot be accurately predicted. However, the obstacles of disciplinary span led to many scholars in materials not having complete knowledge of data-driven materials science methods. This paper provides an overview of the general process of ML applied to materials prediction and uses solid-state electrolytes (SSE) as an example. Recent approaches and specific applications to ML in the materials field and the requirements for building ML models for predicting lithium SSE are reviewed. Finally, some current obstacles to applying ML in materials prediction and prospects are described with the expectation that more materials scholars will be aware of the application of ML in materials prediction.
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Al-Salih, Hilal, Mohamed Houache, Elena A. Baranova, and Yaser Abu-Lebdeh. "Exploring the Interplay between Composite Cathode Design and Cell Performance for Solid-State Lithium Batteries." ECS Meeting Abstracts MA2022-01, no. 1 (July 7, 2022): 127. http://dx.doi.org/10.1149/ma2022-011127mtgabs.
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To accelerate the mass market adaptation of electric vehicles (EVs), raising the gravimetric energy density of batteries to > 250 Wh/kg while maintaining a cost target of < $ 120/kWh is of critical importance (the ultimate targets of the U.S. Department and the advanced battery consortium).[1] Solid-state batteries are widely recognized as excellent prospects for application in the next generation of EVs and other energy storage devices, with the promise to realize higher energy densities, superior safety and environmentally friendly characteristics. At the cell level, the development of SSBs has been hampered by challenges with the interface originating from the poor interfacial stability between the solid-state electrolytes (SSE) and the electrodes. By eliminating the liquid electrolyte, conductive pathways throughout the whole thickness of the positive electrode and at the solid-solid interface become less efficient causing large polarization and diminished cell performance. This can be exacerbated by the current urge to use thicker electrodes in an attempt to increase the energy density which is a common practice in the currently widely adapted lithium ion batteries employing liquid electrolytes. Notably, increasing cathode thickness beyond a certain limit leads to a point of diminishing returns in terms of energy density. This is mainly attributed to the dominating effect of porosity at higher cathode thickness.[2,3] For instance, it has been found that cells with NMC cathodes thinner than 155 μm (< 6.5 mAh cm-2) showed excellent cycling stability and no capacity losses for C-rates up to 0.5C.[4] To address this challenge, one approach is to formulate the cathode (positive electrode) using a small fraction of ionic conductors (Catholyte) that are mostly derived from the solid electrolyte formulation. In addition, this approach could be complemented with the application of a 10 μm intermediate SSE coating at the cathode surface. The use of catholytes has a second advantage of replacing the non-green polymer polyvinylidene fluoride (PVDF) which is currently the most commonly used binder. Having fluorine in its structure, PVDF is non-recyclable and a potential source of environmentally harmful fluorocarbons.[5] We have begun studying the interfacial stability between composite cathodes using LiFePO4 (LFP), a safe, environmentally-friendly, 3.4 V cathode material, and different SSEs including ceramic electrolytes, polymer electrolytes and polymer-ceramic composite electrolytes. In this work, an optimally designed DOE was planned to study the impact of varying active material mass loading in composite cathodes, and the significance of intermediate coating on SSB electrochemical performance. The SSE used is a plasticized polymer electrolyte with the following optimized formula: 77 % PEO, 13% LiTFSI and 10% Succinonitrile (SN) while the composite cathode was composed of 86% LFP, 4% C65 conductive carbon and 10% of the aforementioned SSE as the catholyte. The active material mass loading was varied between 1 – 12 mg cm-2 in 1 mg cm-2 increments and all composite cathodes were tested with and without the intermediate coating layer. This powerful and contemporary statistical approach aims to provide an enhanced design strategy for a popular and very promising SSB chemistry (Li/PEO/LFP). Finally, our findings shed light on a new approach that can be adopted to explore other battery chemistry with higher voltages such as oxide cathodes, non-oxide solid or semi-solid electrolytes. References: [1] R. Schmuch, R. Wagner, G. Hörpel, T. Placke, M. Winter, Nat. Energy 2018 34 2018, 3, 267. [2] Z. Du, D. L. Wood, C. Daniel, S. Kalnaus, J. Li, J. Appl. Electrochem. 2017, 47, 405. [3] M. Wood, J. Li, Z. Du, C. Daniel, A. R. Dunlop, B. J. Polzin, A. N. Jansen, G. K. Krumdick, D. L. Wood, J. Power Sources 2021, 515, 230429. [4] M. Singh, J. Kaiser, H. Hahn, J. Electroanal. Chem. 2016, 782, 245. [5] O. Rynne, M. Dubarry, C. Molson, E. Nicolas, D. Lepage, A. Prébé, D. Aymé-Perrot, D. Rochefort, M. Dollé, ACS Appl. Energy Mater. 2020, 3, 2935. Figure 1
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Thompson, Simon T., Patricia H. Smith, and Tien Q. Duong. "(Invited) U.S. DOE Lithium Metal Solid-State Battery R&D." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 380. http://dx.doi.org/10.1149/ma2022-024380mtgabs.
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Decarbonizing transportation through electrification requires less expensive, higher energy density batteries made from earth-abundant materials to displace internal combustion engines. Suitable solid-state electrolytes (SSEs) that facilitate lithium metal anodes by blocking Li dendrite formation represent a promising pathway to high-energy density cells. In a similar manner, SSEs that block the polysulfide shuttle could facilitate sulfur cathodes with even higher energy density that avoid issues of critical materials and supply chain constraints coupled to transition metal oxide-based cathodes. Interest in solid-state batteries has increased rapidly in recent years. There are examples of solid-state batteries (SSBs) in commercial automotive applications; however, achieving wider adoption requires SSBs operating without the need for heating or excessive applied cell pressure. Several solid-state electrolyte chemistries (e.g., sulfides, ceramics, polymers, halides) are under development, but key issues remain unresolved in the case of each electrolyte chemistry. The U.S. Department of Energy Vehicle Technologies Office supports R&D encompassing all of these candidate electrolytes for solid-state batteries through the Advanced Battery Materials Research program. The R&D portfolio prioritizes: improving electrolytes through modified composition or synthesis to increase room-temperature Li+ conductivity and mitigate Li dendrite penetration; improving interfaces to address chemical or electrochemical reactivity, to decrease impedance, and to improve Li plating and stripping; and improving suitability for high-volume manufacturing of solid-state lithium metal batteries by improving mechanical properties and demonstrating thin, defect-free, large-area SSE layers. This presentation comprises solid-state lithium metal battery R&D priorities and accomplishments in the context of meeting DOE targets for energy density, cycle life, and cost. It will also emphasize the importance of SSBs to U.S. DOE strategy for increasing domestic lithium-based battery manufacturing and securing the U.S. position in next-generation battery innovation.
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Steinle, Dominik, Fanglin Wu, Guk-Tae Kim, Stefano Passerini, and Dominic Bresser. "PEO-based Interlayers for LAGP-type Solid-State Lithium-Metal Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 375. http://dx.doi.org/10.1149/ma2022-024375mtgabs.
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Solid-state electrolytes (SSEs) are expected to play a decisive role for the realization of safer rechargeable batteries and may, additionally, allow for the employment of lithium-metal anodes, thus, paving the way for significantly higher energy densities. 1, 2 There are essentially two main groups of SSEs: (i) polymer and (ii) inorganic solids. The latter can be divided, e.g., into sulfide and oxide based electrolytes. 3 Among the oxides, the so-called NASICON-type electrolytes such as LAGP (lithium aluminum germanium phosphate) are considered as attractive low-cost alternative compared to sulfides. 4 Nonetheless, the incompatibility of LAGP with lithium metal accompanied by the formation of highly resistive interfacial reaction products, detrimentally affecting cycle life and rate capability, remain a great challenge. 5 To overcome this issue, the introduction of polyether (e.g., polyethylene oxide, PEO) as protective interlayer between the lithium-metal anode and the LAGP SSE was proposed. 6, 7, 8 The successful use of such interlayers, however, requires a fast and efficient charge transfer across this interlayer. Herein, we present a comprehensive investigation of PEO-based interlayers comprising varying amounts of ionic liquid-based electrolytes, which consist ofN-butyl-N-methyl pyrrolidinium-based and lithium cations as well as bis(fluorosulfonyl)imide (FSI-) and bis(trifluoromethanesulfonyl)imide (TFSI-) anions. Optimized compositions and the incorporation of selected additives further enhances the charge transfer across this interlayer and the two interfaces with the LAGP electrolyte and lithium metal, enabling long-term stable cycle life and good rate capability of the resulting lithium-metal battery cells. References 1. Gao, Z. et al. Promises, Challenges, and Recent Progress of Inorganic Solid-State Electrolytes for All-Solid-State Lithium Batteries. Adv. Mater. 30, 1705702 (2018). 2. Famprikis, T., Canepa, P., Dawson, J. A., Islam, M. S. & Masquelier, C. Fundamentals of inorganic solid-state electrolytes for batteries. Nat. Mater. 18, 1278–1291 (2019). 3. Fan, L., Wei, S., Li, S., Li, Q. & Lu, Y. Recent Progress of the Solid-State Electrolytes for High-Energy Metal-Based Batteries. Adv. Energy Mater. 8, 1702657 (2018). 4. Bachman, J. C. et al. Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction. Chem. Rev. 116, 140–62 (2016). 5. Hartmann, P. et al. Degradation of NASICON-Type Materials in Contact with Lithium Metal: Formation of Mixed Conducting Interphases (MCI) on Solid Electrolytes. J. Phys. Chem. C 117, 21064–21074 (2013). 6. Wang, C. et al. Suppression of Lithium Dendrite Formation by Using LAGP-PEO (LiTFSI) Composite Solid Electrolyte and Lithium Metal Anode Modified by PEO (LiTFSI) in All-Solid-State Lithium Batteries. ACS Appl. Mater. Interfaces 9, 13694–13702 (2017). 7. Bosubabu, D., Sivaraj, J., Sampathkumar, R. & Ramesha, K. LAGP|Li Interface Modification through a Wetted Polypropylene Interlayer for Solid State Li-Ion and Li–S batteries. ACS Appl. Energy Mater. 2, 4118–4125 (2019). 8. Wang, L., Liu, D., Huang, T., Geng, Z. & Yu, A. Reducing interfacial resistance of a Li1.5Al0.5Ge1.5(PO4)3 solid electrolyte/electrode interface by polymer interlayer protection. RSC Adv. 10, 10038–10045 (2020).
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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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Bubulinca, Constantin, Natalia E. Kazantseva, Viera Pechancova, Nikhitha Joseph, Haojie Fei, Mariana Venher, Anna Ivanichenko, and Petr Saha. "Development of All-Solid-State Li-Ion Batteries: From Key Technical Areas to Commercial Use." Batteries 9, no. 3 (March 1, 2023): 157. http://dx.doi.org/10.3390/batteries9030157.
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Innovation in the design of Li-ion rechargeable batteries is necessary to overcome safety concerns and meet energy demands. In this regard, a new generation of Li-ion batteries (LIBs) in the form of all-solid-state batteries (ASSBs) has been developed, attracting a great deal of attention for their high-energy density and excellent mechanical-electrochemical stability. This review describes the current state of research and development on ASSB technology. To this end, study of the literature and patents as well as market analysis over the last two decades were carried out, highlighting how scientific achievements have informed the application of commercially profitable ASSBs. Analyzing the patents registered over the past 20 years revealed that the number of them had increased exponentially-from only few per year in early 2000 to more than 342 in 2020. Published literature and patents on the topic declare a solid-state electrolyte (SSE) to be the main component of ASSBs, and most patented examples are referred to as solid inorganic electrolytes (SIEs), followed by solid polymer electrolytes (SPEs) and solid hybrid electrolytes (SHEs) in popularity. Investigation of company websites, social media profiles, reports, and academic publications identified 93 companies associated with ASSBs. A list of leading businesses in the solid-state battery sector was compiled, out of which 36 provided information on the ASSB units in their product portfolio for detailed analysis.
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Sadeghzadeh, Rozita, Mickaël Dollé, David Lepage, Arnaud Prébé, Gabrielle Foran, and David Aymé-Perrot. "(Digital Presentation) Post-Treatment Study on Blended Polymer for Solid-State Lithium Batteries." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2468. http://dx.doi.org/10.1149/ma2022-0272468mtgabs.
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The widely used Li batteries (LiBs) is the most established rechargeable energy storage device. Therefore, the development of new electrode and electrolyte materials is essential for improving battery performance. Solid polymer electrolytes (SPEs) have been presented as safer alternatives for liquid electrolytes as they tend to be non-flammable, have enough mechanical strength to resist dendrite growth, and do not leak. However, these materials tend to be less conductive than liquid electrolytes. This problem can be solved by solid-state gel polymer electrolytes (GPEs), which have lately received more attention. In fact, present a possible solution to this dilemma as they combine the ionic conductivity of liquid electrolytes with the increased safety of SPE to develop of electrolytes with high ionic conductivity and good mechanical stability.1 This work presents a preparation of in-situ GPE from SPE which produce by dry process in order to take advantage of the easy processability of SPE and the higher ionic conductivity of GPE.2, 3 The initial SPE was prepared by combining two polymers with LiTFSI (bis(trifluorormethanesulfonyl)imide) via extrusion mixing. This method of GPE processing was also found to improve other aspects of the electrolyte such as thermal and electrochemical properties which were characterized using cycling voltammetry, electrochemical impedance spectroscopy, and thermal gravimetric analysis. Additionally, the salt-polymer interaction in the GPE was characterized using FTIR, NMR, and the homogeneity of the polymer blend study by SEM-EDX. The cell of LFP/electrolyte/ Li metal showed a high capacity near to the theoretical one at C/20 at temperature 60 C. Additionally, the ionic conductivity of the electrolyte is around 10-5 S/cm. These first results confirmed that this blend of the polymers is a good electrolyte candidate for lithium batteries. Verdier, N.; Lepage, D.; Zidani, R.; Prebe, A.; Ayme-Perrot, D.; Pellerin, C.; Dolle, M.; Rochefort, D., Cross-linked polyacrylonitrile-based elastomer used as gel polymer electrolyte in Li-ion battery. ACS Applied Energy Materials 2019, 3 (1), 1099-1110. Ma, C.; Cui, W.; Liu, X.; Ding, Y.; Wang, Y., In situ preparation of gel polymer electrolyte for lithium batteries: Progress and perspectives. InfoMat 2021. Verdier, N.; Foran, G.; Lepage, D.; Prébé, A.; Aymé-Perrot, D.; Dollé, M., Challenges in Solvent-Free Methods for Manufacturing Electrodes and Electrolytes for Lithium-Based Batteries. Polymers 2021, 13 (3), 323.
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Tao, Tao, Zhijia Zheng, Yuxuan Gao, Baozhi Yu, Ye Fan, Ying Chen, Shaoming Huang, and Shengguo Lu. "Understanding the role of interfaces in solid-state lithium-sulfur batteries." Energy Materials 2, no. 5 (2022): 35. http://dx.doi.org/10.20517/energymater.2022.46.
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All-solid-state lithium-sulfur batteries (ASSLSBs) exhibit huge potential applications in electrical energy storage systems due to their unique advantages, such as low costs, safety and high energy density. However, the issues facing solid-state electrolyte (SSE)/electrode interfaces, including lithium dendrite growth, poor interfacial capability and large interfacial resistance, seriously hinder their commercial development. Furthermore, an insufficient fundamental understanding of the interfacial roles during cycling is also a significant challenge for designing and constructing high-performance ASSLSBs. This article provides an in-depth analysis of the origin and issues of SSE/electrode interfaces, summarizes various strategies for resolving these interfacial issues and highlights advanced analytical characterization techniques to effectively investigate the interfacial properties of these systems. Future possible research directions for developing high-performance ASSLSBs are also suggested. Overall, advanced in-situ characterization techniques, intelligent interfacial engineering and a deeper understanding of the interfacial properties will aid the realization of high-performance ASSLSBs.
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Desta, Gidey Bahre Bahre, and Yao Jane Hsu (b)*. "Using Synchrotron Techniques, Investigation of Electrochemical Interfaces in Ni-Rich NMC and Sulfide Electrolytes in All-Solid-State Lithium Metal Batteries." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2610. http://dx.doi.org/10.1149/ma2022-0272610mtgabs.
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a Nano-electrochemistry Laboratory, Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology, Taipei 106, Taiwan, R.O.C b National Synchrotron Radiation Research Center (NSRRC), Hsinchu, 30076, Taiwan, R.O.C In all-solid-state lithium metal batteries enable long cyclability of high voltage oxides cathode persistent problem for the large scale application as their underprivileged interfacial steadiness in contrast to sulfide solid-state electrolyte. In this context, the interfaces of the solid electrolyte and Ni-rich NMC811 active material are looked upon as interfacial chemical responses induced by delithiation. In this study, we monitor the impedance progress at the unstable electrode|electrolyte interface due to the electrochemical interfacial response and help us understand the complex nature of reactivity and degradation kinetics with the solid-solid interface redox decomposition, which makes decoupling each effect difficult. we investigated the interfacial phenomenon between LPSC and high voltage cathode NMC811. The effects of spontaneous retort by the side of the interface were separated, and the intrinsic electrochemical decomposition of LPSC was quantified. Moreover, we show that the notch of interfacial degradation surges and the presence of oxidation mechanisms. At the higher delithiation stage, the cathode might twitch structural defenselessness and oxygen utter and resulting in further stark degradation. This complex kinetic degradation behavior was investigated at the solid-solid interface in a delithiation NMC811 and SSE based on the local oxidation state of NMC811, and LPSC SE interfacial chemical response. In this work, we used various characterization techniques to investigate the interfacial phenomenon between LPSC|NMC811 combining EIS and advanced synchrotron techniques such as sXAS, XPS, XRF-XANES mapping, and In-situ Raman spectroscopy. Keywords: delithiation, Ni-rich cathode, Sulfide-solid-state electrolyte, interfacial reaction, Synchrotron XPS, XRF.
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Kang, Yeomin, Taekyung Kim, Koo Young Jung, and Ki Tae Park. "Recent Progress in Electrocatalytic CO2 Reduction to Pure Formic Acid Using a Solid-State Electrolyte Device." Catalysts 13, no. 6 (May 31, 2023): 955. http://dx.doi.org/10.3390/catal13060955.
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The electrocatalytic CO2 reduction reaction (CO2RR) to formic acid has gained significant attention as a potential environmentally friendly approach to reducing CO2 emissions and producing carbon-neutral liquid fuels. However, several challenges must be addressed to achieve the production of high-purity and high-concentration formic acid through CO2RR. One major challenge is the formation of a formate mixture instead of pure formic acid in conventional reactors. This requires costly downstream purification and concentration processes to obtain pure formic acid. To overcome this problem, a three-compartment reactor design has been proposed where a solid-state electrolyte (SSE) is inserted between the anode and cathode compartments to recover pure formic acid directly. This reactor design involves the use of an anion exchange membrane (AEM) and a cation exchange membrane (CEM) to separate the anode and cathode compartments, and a center compartment filled with high-conductivity SSE to minimize ohmic resistance. Several studies have implemented this reactor design for continuous CO2RR and have reported remarkable improvements in the concentration and purity of the formic acid product. In this review, we summarize the recent progress of the SSE reactor design for CO2RR to produce pure formic acid (HCOOH) and propose further research to scale up this technology for industrial-scale applications in the future.
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Gao, Jingxiong, Jie Wu, Songyi Han, Jingze Zhang, Lei Zhu, Yongmin Wu, Jinbao Zhao, and Weiping Tang. "A novel solid electrolyte formed by NASICON-type Li3Zr2Si2PO12 and poly(vinylidene fluoride) for solid state batteries." Functional Materials Letters 14, no. 03 (January 27, 2021): 2140001. http://dx.doi.org/10.1142/s1793604721400014.
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Owing to their high ionic conductivity and excellent flexibility, composite polymer electrolytes (CPEs) have been widely studied in solid lithium metal batteries (SLMBs). In this study, a new solid electrolyte of NASICON-type Li3Zr2Si2[Formula: see text] (LZSP) was prepared by the sol–gel method, and then a new type of CPE membrane containing LZSP and Poly(vinylidene fluoride) (PVDF) was synthesized by slurry-casting method. The CPE membrane presented much higher ionic conductivity of 5.66 × 10[Formula: see text] S ⋅ cm[Formula: see text] at 25∘C and stronger electrochemical stability compared to the one without LZSP. In addition, the cells containing the composite electrolyte membrane exhibited considerable rate performance and cycle performance.
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Taormina, Riccardo, and Fabio Di Fonzo. "Amorphous Lithium Aluminate As Solid Electrolyte Produced By Pulsed Laser Deposition." ECS Meeting Abstracts MA2022-01, no. 4 (July 7, 2022): 543. http://dx.doi.org/10.1149/ma2022-014543mtgabs.
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Solid state batteries are deemed to become the cornerstone of the future electric mobility. Nevertheless, research on solid electrolytes is still ongoing due the many limitations of current polycrystalline materials. The isotropic and non-periodic structure of amorphous ceramics have shown to contribute to increase the overall ionic conductivity of the material by decreasing the grain-boundary resistive contribution. At the current state, the most promising amorphous material happened to be lithium phosphate oxynitride LiPON (σLi = 10-6 S/cm, ), which demonstrates that the absence of grain boundaries, allows the formation of lithium small dendrites which can grow inside the material without cracking it, avoiding short life cycle of the battery over high current densities [1]. Gao et al. [2] addressed the limited ionic conductivity of LiPON to the strong bond between the PO 4- group with Li+: for this reason, elements with weaker electronegativity than P, such as Al, can generate an ionic bond with O with weaker electrostatic force, regulating the kinetics of Li+ transport and speeds up the diffusion process [3]. In this scenario, Lithium Aluminate (LiAlO2) and Nitrogen-doped Lithium Aluminate (LiAlON) result in a competitive position for the development of an innovative amorphous-glassy electrolyte: very few studies have been conducted on the development of lithium aluminate based solid electrolytes at the present time, mainly due to its low processability at the amorphous phase and the low ionic conductivity of the crystalline phase, more common in the traditional sintering processes. In this study, we demonstrate for the first time the possibility to obtain with Pulsed Laser Deposition (PLD), a completely amorphous LiAlO2 solid electrolyte with a room temperature ionic conductivity of 10-10 S/cm. Thanks to the PLD processing, the grade of polymorphism can be easily controlled as well as film thickness range (10nm up to 10um) and film porosity. By controlling the deposition atmosphere, different content of nitrogen doping has been achieved, promoting the formation of the highly ionic conductive LiAlON (almost two order of higher conductivity). Electrochemical analysis such as DC polarization and Impedance Spectroscopy, revealed the wide electrochemical voltage stability against lithium metal and the high ionic conductivity of the solid electrolyte. A multi-layer approach for the direct deposition of the solid electrolyte over lithium metal surface is proposed, allowing the realization of symmetric cell test and plating/stripping test. Good protection of Li metal substrate has been observed from the LiAlO2 SSE over 24h, hindering oxidation and degradation of the sample. [1] - Nowak, Berkemeier, and Schmitz, “Ultra-Thin LiPON Films – Fundamental Properties and Application in Solid State Thin Film Model Batteries.” [2] - Gao et al., “Screening Possible Solid Electrolytes by Calculating the Conduction Pathways Using Bond Valence Method.” [3] - Guan et al., “Superior Ionic Conduction in LiAlO 2 Thin-Film Enabled by Triply Coordinated Nitrogen.”
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Au, Benedict Wen-Cheun, Kah-Yoong Chan, Mohd Zainizan Sahdan, Abraham Shiau-Iun Chong, and Dietmar Knipp. "Realisation of Solid-State Electrochromic Devices Based on Gel Electrolyte." F1000Research 11 (June 6, 2022): 380. http://dx.doi.org/10.12688/f1000research.73661.2.
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Background: In the last decade, there has been much interest in the area of solid polymer electrolyte (SPE) to address the issues of electrolyte leakage and evaporation in electrochromic devices (ECD). ECD is a state-of-the-art technology having the ability to change from transparent state to opaque state under the influence of a small applied voltage for energy saving applications. Methods: In this work, tungsten oxide (WO3) films were fabricated via the sol-gel spin-coating method. Subsequently, ECDs were assembled based on SPE and liquid polymer electrolyte (LPE), respectively using indium doped tin oxide (ITO) coated glass as conducting electrodes and WO3 films as working electrode. Results: Cyclic voltammetry (CV) results revealed reduced ionic conductivity of conducting ions in SPE based ECD (SECD) owing to increased viscosity by addition of PMMA. However, lesser time was required for the colouration process. LPE based ECD (LECD) showed higher colouration efficiency (CE) compared to its SECD counterpart. This is attributed to its larger optical modulation. Conclusions: This work presents a comparison between the performance of LECD and SECD in terms of electrochromic (EC) and optical properties. They were analysed through CV, chronoamperometry (CA) and ultraviolet-visible (UV-Vis) spectrophotometer. Furthermore, this work provides an insight on the employment of solid-state electrolytes in ECDs in view of the persistent leakage and evaporation problems in ECD implementation.
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Au, Benedict Wen-Cheun, Kah-Yoong Chan, Mohd Zainizan Sahdan, Abraham Shiau-Iun Chong, and Dietmar Knipp. "Realisation of Solid-State Electrochromic Devices Based on Gel Electrolyte." F1000Research 11 (March 31, 2022): 380. http://dx.doi.org/10.12688/f1000research.73661.1.
Full textAbstract:
Background: In the last decade, there has been much interest in the area of solid polymer electrolyte (SPE) to address the issues of electrolyte leakage and evaporation in electrochromic devices (ECD). ECD is a state-of-the-art technology having the ability to change from transparent state to opaque state under the influence of a small applied voltage for energy saving applications. Methods: In this work, tungsten oxide (WO3) films were fabricated via the sol-gel spin-coating method. Subsequently, ECDs were assembled based on SPE and liquid polymer electrolyte (LPE), respectively using indium doped tin oxide (ITO) coated glass as conducting electrodes and WO3 films as working electrode. Results: Cyclic voltammetry (CV) results revealed reduced ionic conductivity of conducting ions in SPE based ECD (SECD) owing to increased viscosity by addition of PMMA. However, lesser time was required for the colouration process. LPE based ECD (LECD) showed higher colouration efficiency (CE) compared to its SECD counterpart. This is attributed to its larger optical modulation. Conclusions: This work presents a comparison between the performance of LECD and SECD in terms of electrochromic (EC) and optical properties. They were analysed through CV, chronoamperometry (CA) and ultraviolet-visible (UV-Vis) spectrophotometer. Furthermore, this work provides an insight on the employment of solid-state electrolytes in ECDs in view of the persistent leakage and evaporation problems in ECD implementation.
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Murtaza, Imran, Muhammad Umair Ali, Hongtao Yu, Huai Yang, Muhammad Tariq Saeed Chani, Khasan S. Karimov, Hong Meng, Wei Huang, and Abdullah M. Asiri. "Recent Advancements in High-Performance Solid Electrolytes for Li-ion Batteries: Towards a Solid Future." Current Nanoscience 16, no. 4 (August 20, 2020): 507–33. http://dx.doi.org/10.2174/1573413716666191230153257.
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With the emergence of non-conventional energy resources and development of energy storage devices, serious efforts on lithium (Li) based rechargeable solid electrolyte batteries (Li- SEBs) are attaining momentum due to their potential as a safe candidate to replace state-of-the-art conventionally existing flammable organic liquid electrolyte-based Li-ion batteries (LIBs). However, Li-ion conduction in solid electrolytes (SEs) has been one of the major bottlenecks in large scale commercialization of next-generation Li-SEBs. Here, in this review, various challenges in the realization of high-performance Li-SEBs are discussed and recent strategies employed for the development of efficient SEs are reviewed. In addition, special focus is laid on the ionic conductivity enhancement techniques for inorganic (including ceramics, glasses, and glass-ceramics) and polymersbased SEs. The development of novel fabrication routes with controlled parameters and highperformance temperature optimized SEs with stable electrolyte-electrode interfaces are proposed to realize highly efficient Li-SEBs.
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Pham, Quoc-Thai, Badril Azhar, and Chorng-Shyan Chern. "Novel Acrylonitrile-Based Polymers for Solid–State Polymer Electrolyte and Solid-State Lithium Ion Battery." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 160. http://dx.doi.org/10.1149/ma2022-012160mtgabs.
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Rechargeable lithium-ion batteries (LIBs) involving lithium metal oxides, liquid electrolyte and graphite have been widely used in portable electronic devices due to their relatively high energy density and long cycle life. These desirable features make LIBs very attractive as the power source for electronic devices, hybrid electric vehicles (HEVs) and electric vehicles (EVs) applications [1, 2]. For future EV applications, higher energy density of LIBs up to 360 Wh kg-1 is required. Currently, the energy density of the state-of-the-art LIBs using conventional graphite anode, LiFePO4 (denoted as LFP) or LiNi0.5Co0.2Mn0.3O2 (NCM523) cathodes and 1-1.2 M LiPF6 in organic carbonate electrolytes provide practically achievable energy densities of up to around 200-260 Wh kg−1 [3]. When commercial graphite anodes are used, LiNi0.8Co0.15Al0.05O2 (NCA), LiNi0.8Co0.1Mn0.1O2 (NCM811), LiNi0.5Mn1.5O4 (LNMO) and LiNiPO4 (LNP) cathode based batteries with high-voltage provide energy densities of 354, 338, 351 and 414 Wh kg-1, respectively. However, LIBs using these high-voltage cathode materials and the organic carbonate electrolytes exhibit quite low thermal stability and tend to catch fire or even explode when abnormal charge/discharge cycling or accidental penetration of cells occurs, which greatly limits the automotive applications. When replacing graphite with a Li metal anode, the energy densities of all battery systems can be enhanced significantly due to the highest theoretical specific energy density (3860 mAh g-1) among all anode materials for rechargeable LIBs. Nevertheless, commercial LIBs are prone to cause safety problems due to the safety concern arising from Li dendrite growth in liquid organic electrolytes [4-6]. The promising solid-state LIBs offer high thermal stability (i.e., low risk in catching fire), high energy density, wide electrochemical stability window and less environmental impact. A competent electrolyte is the key component of solid-state LIBs. The solid-state electrolyte materials are mainly classified as solid polymer electrolytes (SPEs), inorganic solid electrolytes (ISEs), and organic/inorganic composite electrolytes. ISEs include oxide-based and sulfide-based materials [7, 8], which show very high ionic conductivity (10-2 – 10-3 S cm-1). Furthermore, the lithium ion transference number is close to 1. However, the major limitation factors of practical solid-state LIB applications are the large interfacial impedance between electrode and ISE and the difficulty of processing [9]. Considering processability, mechanical flexibility, interfacial compatibility and electrochemical stability, one prefers SPEs to the inorganic ceramic electrolytes. Nevertheless, SPEs have low ion conductivities (10−7 − 10−5 S cm−1 near room temperature) and most of the Li+ transference numbers are lower than 0.5 [10, 11]. The major requirements for SPEs include high ionic conductivity and transference number at room temperature, wide electrochemical potential window, high mechanical strength and excellent thermal stability. However, the ion conductivity is the most important (> 10-4 S cm-1 at room temperature desired) and should be considered first. The coordinating groups of a good polymeric host are expected to interact with Li+ and facilitate dissociation. In this study, we prepared various novel acrylonitrile-based polymers (e.g., acrylonitrile/acrylate copolymer and polymer with two pendant groups b-cyano ethyl ether (-O-CH2CH2-CN) sulfonate alkyl ether (-O-(CH2)3SO3Li). The corresponding SPEs comprising acrylonitrile-based polymer and ca. 50 wt.% lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) with high ionic conductivity (up to 10-3 S cm-1) at room temperature, high ion transfer number (up to 0.45) and large electrochemical potential window (oxidation stability > 5 V vs. Li+/Li) achieved. The selected SPEs were used as the separator in solid-state batteries with LiFePO4 as the cathode and Li foil as the anode; and long-term cycle stability of solid-state LIB was achieved. The polymers and corresponding SPEs were characterized by using DSC, SEM, XRD and FTIR measurements. Ionic conductivities of SPEs were determined from electrochemical impedance spectroscopy results. The linear sweep voltammetry technique was adopted to measure the oxidation stability window of SPE, and the Evans-Vincent-Bruce method was used to determined ion transfer number. References [1] J.B. Goodenough, Energy Environ. Sci. 7 (2014) 14−18. [2] M. Armand, et al., Nature 451 (2008) 652-657. [3] F. Wu, et al., Chem Soc Rev 49 (2020) 1569-1614. [4] Q. Wang, et at., J Power Sources 208 (2012) 210-224. [5] A.W. Golubkov, et al., RSC Adv 5 (2015) 57171-57186. [6] Z. Wang, et al. Nat Energy 3, (2018) 227–235. [7] L. Fan, et al., Adv. Energy Mater. 2018, 8, 1702657. [8] G. Kim, et al., J Power Sources 282 (2015) 299-322. [9] P. Knauth, Solid State Ion 180 (2009) 911-916. [10] C. Ma, et al., J Power Sources 2016; 317 :103–11. [11] N.K. Karan, et al., Solid State Ion 179 (2008) 689–696. Figure 1
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Houache, Mohamed, Zouina Karkar, Chae-Ho Yim, Gina Filoso, Svetlana Niketic, and Yaser Abu-Lebdeh. "Optimization of Catholyte in Composite Cathodes for Garnet-Structured Llzo Electrolyte in Solid-State Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 233. http://dx.doi.org/10.1149/ma2022-012233mtgabs.
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The application of Li-ion batteries have been expanding at a rapid rate in recent decades due to the tremendous demands in the market for portable electronics, smart grid, and electric vehicles (EVs). All-solid-state lithium metal battery (ASSLB) is the most promising next-generation energy storage device as they can solve the safety issue resulted from liquid electrolytes. Among different types of solid-state electrolytes (SSE), garnet-type structure materials have been shown to be very promising for the development of ASSLBs owing to their high Li-ion conductivity (∼10–3 S cm–1 at RT), wide electrochemical stability window (∼6 V vs Li+/Li), and good chemical stability against Li metal. The high interfacial resistance generated by inadequate contact and interfacial reactions is a substantial impediment to the adaptation of ASSLBs. To address this challenge, a catholyte (a small amount of ionic conductors which are mostly derived from the solid electrolyte formulation) is introduced into the cathode formulation. This necessities a re-design of the cathode into a composite cathode with possibly new components such as carbon additives with high aspect ratio and conductive binders. Understanding their individual and combined impacts on performance is essential in the pursuit of optimized systems. In this work, we designed a series of composite cathode formulations defined with three cathode active materials (LFP, NMC 622 and NMC 811), three carbonaceous additives (carbon black, carbon nanofibers and carbon nanotubes), and a series of organic and inorganic molecular, and polymeric conductors along with LLZO to create a composite cathode with high capacity and stability at high C-rates. A systematic DOE approach has been utilized to evaluate the impact of each component on the electrode and cell performance and the results will be presented.
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Hao, Wei, and Gyeong S. Hwang. "(Digital Presentation) On the Origin of High Resistance at the Interface between Lithium Metal and Sulfide Solid Electrolytes." ECS Meeting Abstracts MA2022-01, no. 1 (July 7, 2022): 92. http://dx.doi.org/10.1149/ma2022-01192mtgabs.
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Sulfide materials have been extensively studied as solid-state electrolytes (SSEs) for all-solid-state lithium metal batteries (ASSLMBs) because of their high ionic conductivity, wide electrochemical window, and appropriate mechanical properties. However, they suffer from the high interfacial resistance with Li metal anode, besides poor stability when exposed to air, hindering the application of sulfide-based SSEs in ASSLMBs. Sulfide materials are well known to undergo reaction with Li metal, leading to solid-electrolyte interphase layer formation at the SSE/Li metal interface. The side reactions could be primarily responsible for the high resistance at the interface between SSE and Li metal anode, but the underlying mechanisms still remain unclear. To better understand the structure and property changes of the sulfide SSE due to the reaction with Li metal, we took β-Li3PS4 (LPS) as a model system and systematically analyzed the structural, electronic, transport, and mechanical properties of lithiated LPS with varying Li contents using first-principles methods. Moreover, we examined the compositional and structural evolution at the LPS/Li metal interface using ab initio molecular dynamics (AIMD) simulations. Our results unequivocally show that Li incorporation leads to decomposition of PS4 3- to Li2S and Li3P when fully lithiated. With lithiation, Li-ion conductivity is predicted to remain in the same order of magnitude despite the significant structural and compositional changes. Both the band gap and density of the lithiated LPS becomes smaller than those of the unlithiated LPS. More importantly, we found the formation of voids at the LPS/Li metal interface. In this talk, based on our results we will discuss the mechanisms responsible for the high interfacial impedance as often observed in previous experimental studies.
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Ebenezer Anitha, Angellina, and Marius Dotter. "A Review on Liquid Electrolyte Stability Issues for Commercialization of Dye-Sensitized Solar Cells (DSSC)." Energies 16, no. 13 (July 3, 2023): 5129. http://dx.doi.org/10.3390/en16135129.
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Dye-sensitized solar cells have been under development for the last three decades but are yet to see the market. This has been attributed to stability issues of the electrolyte in the cell. Electrolytes can be liquid, quasi-solid, or solid. Liquid electrolytes were the first to be developed and, therefore, have been subject to radical revisions in both composition and applicability. They have shown the best power conversion efficiencies but have poor thermal stability. Although quasi-solid and solid-state electrolytes were developed to overcome these stability issues, they too have their limits. The aim of this paper is to explore the development of liquid electrolytes, outlining the current state of the technology and considering their potential in the photovoltaic market.
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Zhao, Feipeng, Jianwen Liang, and Xueliang Andy Sun. "Improved Air Stability of Sulfide Electrolytes for All-Solid-State Li Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 230. http://dx.doi.org/10.1149/ma2022-012230mtgabs.
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Sulfide-based solid electrolytes (SEs) are receiving increasing attention due to their high ionic conductivities (up to 10-2 S cm-1 at room temperature) that can be comparable to the liquid electrolytes.1 However, the air stability of sulfide SEs is very poor.2, 3 Most developed sulfide SEs are prone to turn bad when exposed to the moisture. The generated H2S is dangerous, which places the commercialization of sulfide SEs into a challenging situation. 2, 3 In our work, to improve the air stability of sulfide SEs, we employed element substitution (Sn and Sb) for the problematic element (P) in conventional sulfide SEs (Li3PS4, Li6PS5I, Li10GeP2S12) based on the hard and soft acid and base theory (HSAB).4, 5, 6 Our results suggest that Sn and Sb-substituted sulfide SEs show significantly improved air stability compared with the pristine sulfides. Meanwhile, it is found that the Sn or Sb element substitution effectively enhance the ionic conductivity as well as Li metal compatibility in some cases. Various structural (e.g., X-ray diffraction, X-ray absorption near edge spectroscopy, solid-state nuclear magnetic resonance) and electrochemical characterizations are employed to identify the mechanism of the improvements are related to the Sn/Sb substitution-derived crystal structure, reinforced bonding energy, and the optimized electrode/electrolyte interfaces. Our studies provide a new idea of designing functional sulfide composition to realize improved air stability coupling with other essential properties. Re ferences N. Kamaya, R. Kanno*, et al. A lithium superionic conductor, Nat. Mater. 2011, 10, 682-686. C. Yu, F. Zhao, J. Luo, X. Sun*. Recent Development of lithium argyrodite solid-state electrolytes for solid-state batteries: synthesis, structure, stability and dynamics. Nano Energy 2021, 83, 105858. F. Zhao, S. Zhang, Y. Li*, X. Sun*. Emerging characterization techniques to understand electrode interfaces in all-solid-state lithium batteries. Small Struct. 2021, DOI: 10.1002/sstr.202100146. F. Zhao, J. Liang, X. Sun*, et al. A Versatile Sn-Substituted Argyrodite Sulfide Electrolyte for All-Solid-State Li Metal Batteries, Adv. Energy Mater. 2020, 10, 1903422. F. Zhao, X. Sun*, et al. An Air-Stable and Li-Metal-Compatible Glass-Ceramic Electrolyte enabling High-Performance All-Solid-State Li-Metal Batteries. Adv. Mater. 2021, 33, 2006577. J. Liang, X. Sun*, et al. Li10Ge(P1–xSbx)2S12 Lithium-Ion Conductors with Enhanced Atmospheric Stability, Chem. Mater. 2020, 32, 2664-2672.
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Choi, Sanghyeon, and Woo Young Yoon. "Electrochemical Properties of the Interface Modified Li-Metal All Solid State Battery (Li/LLZO/LVO cell)." ECS Meeting Abstracts MA2022-01, no. 1 (July 7, 2022): 48. http://dx.doi.org/10.1149/ma2022-01148mtgabs.
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As an anode material, Li metal is a most promising because of a low electrochemical potential(−3.045 V vs the standard hydrogen electrode), high theoretical capacity(3860 mAh/g), low density (0.534 g/cm3 ), and high electrical conductivity. However, a Li-metal anode battery is limited to use because of poor safety and electrochemical instability because of dendritic growth and “dead-lithium” outbreak during cycling in a flammable liquid electrolyte system. 1-3 The dendrite growth on the electrode surface is mainly caused by the localization of current due to the heterogeneous SEI film on the surface and the high current rate during cycling. 4 In order to overcome a dendrite growth behavior, there are many trials reported such as, Li metal morphology change(ref), coating the metal surface(ref), or adding a surfactant in the electrolyte. In addition, applying a solid state electrolyte (SSE) instead of a liquid electrolyte, it may overcome the disadvantage of a flammable electrolyte in the Li-metal battery.5 There are two types of solid state electrolyte systems, such as a sulfidic electrolyte (i.e. LGPS(Li10GeP2S12)) and an oxide-based electrolyte(i.e. LLZO(Li7La3Zr2O12)). The former has very high ionic conductivity (12x10-3Scm-1). 6 Also, due to its ductile mechanical properties, it doesn’t require high pressure and temperature to manufacture the efficient solid state electrolyte pellet. 7, but it causes byproduct when exposed to reactive gases, humidity and lithium metal. 8 Otherwise, an oxide-based electrolyte like LLZO has high ionic conductivity and is chemically and electrochemically stable with lithium metal anode. 9,10 However, high energy (1100oC, 300Mpa) is required to fabricate the efficient LLZO electrolyte. 11 and it also has the disadvantage of poor contact with the electrode due to its rigid mechanical properties. To be a true meaning of the Li-metal all solid state battery (ASSB), the Li-anode metal should be an energy (or ion) source. Therefore, non-lithiate materials such as sulfur or O2 should be coupled as a cathode material. Though they are still more works to use in the cell, Sulfur and O2 are attracting attention as a next-generation cathode material for lithium metal batteries due to their high theoratical capacity. 15,16 Instead, the LiV3O8 may be a proper non-lithiated cathode material to test a Li-metal ASSB, because its stability and electrochemical properties are already reported. 17, 18 major obstacles at each constituents are numbered: (1) dendritic growth on the Li metal anode surface, (2) inappropriate contact at the anode/solid electrolyte interface, (3) poor ionic conductivity caused by less compacted solid electrolyte materials, (4) inappropriate contact at the solid electrolyte/ cathode interface, (5) poor ionic and electronic conductivity caused by less compacted cathode materials. Of course, more problems such as by-products due to every reactions, intervention of side reaction, and enhanced mechanical properties of the electrode materials also overcome to be a commercial Li-metal ASSB. The major purpose of the this research, however, builds a Li-metal ASSB system in which Li-metal used as an anode and understands the electrochemical performances of the Li/LLZO/LVO secondary batteries.
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Zhang, Shumin, Feipeng Zhao, and Xueliang Andy Sun. "Interface Engineering Via Fluorinated Solid Electrolytes for All-Solid-State Li Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 159. http://dx.doi.org/10.1149/ma2022-012159mtgabs.
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Solid electrolytes (SEs) are vital for all-solid-state batteries (ASSBs) since they replace the flammable liquid electrolytes to make the ASSBs safer and compacter.1 In order to boost the energy density of ASSBs, a practical SE is not only expected possessing high ionic conductivity, but also good compatibility with both cathode and anode to allow the use of high-voltage cathode and Li metal.2, 3 However, most of the developed SEs show limitations on directly contact with either high-voltage cathode materials or Li metal. As such, SE modification is required to address the interfacial issues between SE and electrodes. In this work, fluorinated sulfide- and halide-based SEs are proposed to stabilize the SE/Li metal and SE/high-voltage cathode interfaces, respectively. Our results firstly show that fluorinated argyrodite Li6PS5Cl (LPSCl) can enhance the interfacial stability toward the Li metal anode.4 The in-situ formed interface between Li and LPSCl1−xFx are of highly fluorinated and condense, which enables ultrastable Li plating/stripping behavior over 250 hrs at a high current density of 6.37 mA cm−2 and a cutoff capacity of 5 mAh cm−2. The Li metal treated by the LPSCl1−xFx SE is then demonstrated to deliver good durability and rate capability in full cells. Other than anode side improvement, F is introduced into a superionic conductor Li3InCl6 to widen the oxidation limit to over 6 V (vs. Li/Li+).5 Both experimental and computational results identify that F-containing passivating interphases are generated to contribute to the enhanced oxidation stability of Li3InCl6-xFx and stabilization the surface of cathodes at high cut-off voltages. The optimized composition Li3InCl4.8F1.2 is directly matched with bare high-voltage LiCoO2, enabling ASSBs to stably operate at room temperature at a cut-off voltage of 4.8 V (vs Li/Li+). Our studies provide a new strategy of interface engineering by introducing F in SEs, realizing the good compatibility between SE and electrodes and opening up the applications of ASSBs. Re ferences Manthiram, A., Yu, X. W., Wang, S. F. Lithium battery chemistries enabled by solid-state electrolytes. Nat. Rev . Mater. 2, 1-16 (2017). Wang, C. H., Liang, J. W., Zhao, Y., Zheng, M. T., Li, X. N., Sun, X. L. All-solid-state lithium batteries enabled by sulfide electrolytes: from fundamental research to practical engineering design. Energy Environ. Sci. 14, 2577-2619 (2021). Li, J. C., Ma, C., Chi, M. F., Liang, C. D., Dudney, N. J. Solid Electrolyte: the Key for High-Voltage Lithium Batteries. Adv. Energy Mater. 5, 1401408 (2015). Zhao, F. P., et al. Ultrastable Anode Interface Achieved by Fluorinating Electrolytes for All-Solid-State Li Metal Batteries. ACS Energy Lett. 5, 1035-1043 (2020). Zhang, S. M., et al. Advanced High-Voltage All-Solid-State Li-Ion Batteries Enabled by a Dual-Halogen Solid Electrolyte. Adv. Energy Mater. 11, 2100836 (2021).
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Dornbusch, Donald, Rocco P. Viggiano, James Wu, Yi Lin, John Connell, and Vadim Lvovich. "Design Considerations for Practical Li-S Battery Components for Electric Aviation." ECS Meeting Abstracts MA2022-01, no. 1 (July 7, 2022): 133. http://dx.doi.org/10.1149/ma2022-011133mtgabs.
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The development of high-energy, high-safety, and high-power batteries beyond electric automobile requirements is vital for future electric aviation applications. The transition to non-volatile solid-state electrolytes (SSE) promises many advantages over traditional flammable liquid electrolytes and may also be an enabling technology for next generation chemistries. However, significant manufacturing challenges must be overcome before the adoption of such technology. This study focuses on advancement of previous electrolyte development to produce sulfide-polymer composites with densified thicknesses between 20-30 microns using a tape-casting technique with an elastomer binder [1]. Parameters such as binder type, binder loading, and filler loading are modified to determine their impact on electrochemical performance and mechanical stability. The composites were determined to retain reasonable ionic conductivity with improved flexibility and scalability critical for practical manufacturing of such cells. Films were produced 10-15 times thinner than comparable bulk powder electrolytes and within the range of commercial polyolefin separators (25 micron) used in commercial liquid containing lithium-ion cells. Composite conductivities were maintained above 0.2mS/cm, which holds promise for future electric aviation applications. Processing techniques are investigated to further improve electrochemical performance. [1] Donald A. Dornbusch, Rocco P. Viggiano, John W. Connell, Yi Lin, Vadim F. Lvovich. Practical considerations in designing solid state Li-S cells for electric aviation, Electrochimica Acta, 2021, 139406, ISSN 0013-4686, https://doi.org/10.1016/j.electacta.2021.139406.
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Sankara Raman, Ashwin, Samik Jhulki, Billy Johnson, Aashray Narla, and Gleb Yushin. "Facile in-Situ Polymerized Polymer Electrolytes in All Solid-State Lithium-Ion Batteries." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 316. http://dx.doi.org/10.1149/ma2022-023316mtgabs.
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With the push towards renewable energy sources and “green” technologies, lithium-ion batteries (LIBs) have proven to be necessary across multiple technological realms, the biggest of which is currently the electric vehicle (EV) and grid storage markets. But the popular choice of liquid organic electrolytes in LIBs suffers from safety concerns, which motivated significant innovations in safer solid-state electrolytes. Among them, solid polymer electrolytes (SPEs) have shown great potential due to their processability, flexibility and tunability of physical properties. The past decade has seen rapid evolution in the development of SPE LIBs, but most of them still stand inadequate. SPEs are typically processed either by using solvents, or by using them in their solid state, to blend with the active electrode materials. While these systems are often subject to additional compression to promote continuous electrolyte-electrode interface, they still suffer from the almost unavoidable formations of voids, and inhomogeneous contact between the active materials and the SPEs. Furthermore, most of these processes require excessive amounts of SPEs, and yet result in a large interfacial resistance. Here we introduce a novel one-step manufacturing strategy for polymer electrolytes in solvent-free SPE LIBs. The process involves in-situ polymerization of a liquid-monomer precursor directly infiltrated into a dry jelly roll or individual electrodes to form SPE cells. Our microscopy and FIB experiments confirmed a near-perfect polymer infiltration in porous cathodes, while electro-chemical tests confirmed excellent characteristics of cathode-electrolyte interfaces. The cycling performance of lithium iron phosphate (LFP) half cells using thus produced and infiltrated SPE showed very good stability and columbic efficiency. In addition to single-ion conductive SPEs, we tested hybrid SPE systems where Li salts were added into the single-ion conductive SPEs to improve rate and capacity utilization.
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Yang, Guang, Ethan Self, Teerth Brahmbhatt, Anna Mills, Wan-Yu Tsai, Daniel Hallinan, Xi Chen, Frank Delnick, and Jagjit Nanda. "Development of Argyrodite-Based Sulfide Electrolytes for Next-Generation Solid-State Li Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 537. http://dx.doi.org/10.1149/ma2022-024537mtgabs.
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Advances in solid electrolytes (SEs) with superionic conductivity and stabilized electrode-electrolyte interfaces are key enablers for all-solid-state batteries (SSBs) to meet the energy density and cost targets for next-generation batteries for electric vehicles. Argyrodite sulfide-based electrolytes with the nominal composition Li6PS5X; where X= Cl and/or Br, I provide several key advantages over other types of SE counterparts, including (i) exceptionally high ionic conductivities up to 10-2 S/cm at room temperature (comparable to nonaqueous liquid electrolytes), (ii) availability of low temperature and inexpensive synthesis routes to produce glass, glass-ceramic, and crystalline structures, and (iii) soft mechanical properties facilitating material processing and solid-state battery (SSB) fabrication. Several key challenges exist for the practical use of the argyrodite sulfide-based electrolyte in an SSB: (i) scale-up synthesis to produce phase-pure materials, (ii) rationale processing method development to produce free-standing thin film SSEs, and (iii) identifying buried interfacial side-reaction products at the electrode/electrolyte interfaces using advanced characterization tools. In this talk, we will present our recent achievements focusing on tackling each of these challenges, including (i) solution-based synthesis of Li6PS5X; (ii) optimizing binder, slurry composition, and processing method to make Li6PS5X thin film (<50 µm) SSEs, and (iii) combining in-situ Raman spectroscopy and microscopy with complementary electrochemical impedance spectroscopy (EIS) to explore electrode/ Li6PS5X interfacial stability. Acknowledgment This research conducted at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) is sponsored by the Office of Energy Efficiency and Renewable Energy (EERE) in the Vehicle Technologies Office (VTO) through the Advanced Battery Materials Research (BMR) Program.
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He, Yaolong, Shufeng Li, Sihao Zhou, and Hongjiu Hu. "Mechanical Integrity Degradation and Control of All-Solid-State Lithium Battery with Physical Aging Poly (Vinyl Alcohol)-Based Electrolyte." Polymers 12, no. 9 (August 21, 2020): 1886. http://dx.doi.org/10.3390/polym12091886.
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Ensuring the material durability of an electrolyte is a prerequisite for the long-term service of all-solid-state batteries (ASSBs). Herein, to investigate the mechanical integrity of a solid polymer electrolyte (SPE) in an ASSB upon electrochemical operation, we have implemented a sequence of quasi-static uniaxial tension and stress relaxation tests on a lithium perchlorate-doped poly (vinyl alcohol) electrolyte, and then discussed the viscoelastic behavior as well as the strength of SPE film during the physical aging process. On this basis, a continuum electrochemical-mechanical model is established to evaluate the stress evolution and mechanical detriment of aging electrolytes in an ASSB at a discharge state. It is found that the measured elastic modulus, yield stress, and characteristic relaxation time boost with the prolonged aging time. Meanwhile, the shape factor for the classical time-decay equation and the tensile rupture strength are independent of the aging history. Accordingly, the momentary relaxation modulus can be predicted in terms of the time–aging time superposition principle. Furthermore, the peak tensile stress in SPE film for the full discharged ASSB will significantly increase as the aging proceeds due to the stiffening of the electrolyte composite. It may result in the structure failure of the cell system. However, this negative effect can be suppressed by the suggested method, which is given by a 2D map under different lithiation rates and relative thicknesses of the electrolyte. These findings can advance the knowledge of SPE degradation and provide insights into reliable all-solid-state electrochemical device applications.
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Gao, Mengmeng, Xiaolei Wu, Jianhang Wang, Caiyan Yu, Dong Yan, Hui Ying Yang, Huiling Zhao, and Ying Bai. "Fabrication of Li1.4Al0.4Ti1.6(PO4)3 quasi-solid electrolyte with high conductivity and compatibility through AAO template." Applied Physics Letters 120, no. 19 (May 9, 2022): 191902. http://dx.doi.org/10.1063/5.0088623.
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Employing inorganic ion conductors as solid electrolytes (SEs) is one promising solution to develop advanced all- and quasi-solid-state batteries with high energy and safety advantages. Among numerous Li+ ion conductors, Li1.4Al0.4Ti1.6(PO4)3 (LATP) has attracted extensive attention due to its preponderances of air stability and superior Li+ conductivity. However, the practical application of the LATP electrolyte is still obsessed by serious side reactions at the Li-electrode/electrolyte interface. In this work, one kind of quasi-solid electrolyte (QSE) is designed combining anodic aluminum oxide (AAO), LATP, and liquid electrolyte [LE, LiPF6/ethylene carbonate-dimethyl carbonate (EC-DMC)], wherein well-ordered LATP arrays are constructed in the AAO framework to facilitate ionic transport, and a certain content of the LE is introduced to reduce the interfacial resistances. The characterization results suggest that the ionic conductivity of as-prepared AAO–LATP–QSE (ALQSE) is boosted up to ∼6.50 × 10−3 S cm−1 with a Li+ transference number of 0.66, especially the interval between the LATP compound and the Li-metal electrode can effectively restrain Ti4+→Ti3+ reduction at the Li-anode/electrolyte interface. Thus, the assembled LiFePO4|ALQSE|Li cell exhibits excellent electrochemical stability, delivering an initial discharge capacity of 153.3 mAh g−1 at 0.1C and remaining 152.4 mAh g−1 after 60 cycles with a fairly mild reduction of 0.028% per cycle. This study not only presents a facile strategy to prepare a robust QSE framework employing an AAO template but also promotes the rational interface design between titanium (Ti)-containing solid-state electrolytes and Li-metal anodes.
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Wang, Kun, Yuechen Gao, Mohamed Mostafa, Thanh Nguyen, Hyang Seol, Volodymyr Koverga, Naveen Dandu, Anh Ngo, Gang Cheng, and Sangil Kim. "Highly Ion-Conductive, Elastic, and Adhesive Zwitterionic Polymer Electrolyte for All-Solid-State Lithium Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 391. http://dx.doi.org/10.1149/ma2022-024391mtgabs.
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Currently, lithium-ion batteries (LIBs) are considered to be one of the most popular energy storage systems for electronic devices supported by high energy density, high operating voltage, and favorable cycling performance. However, commercial LIBs with the organic liquid electrolyte and lithium (Li) salts are associated with critical safety issues such as uncontrollable side reactions, toxic liquid electrolyte leakage, flammability of electrolytes, and poor thermal stability. Therefore, replacing the liquid electrolyte with solid electrolytes is quite necessary. Among several solid ion conductors, solid polymer electrolytes (SPEs) can offer excellent flexibility, interfacial compatibility with electrodes, good processibility, low cost, and light weights that can overcome the limitations of ceramic ion conductors. However, current SPEs often encounter limitations such as poor mechanical strength and dimensional thermal stability, inferior electrochemical stability, and low Li+ ion conductivity at room temperature (~10-5 S cm-1 at 25 ℃). Here we present a multifunctional solid polymer electrolyte based on zwitterionic polyurethanes (zPU-SPE) for all-solid-state LIBs (SLBs). Our zPU-SPE exhibits a great potential to overcome current technical limitations of conventional SPE materials in SLB applications (e.g., low Li+ ion conductivity, inferior electrochemical/mechanical stabilities, unsatisfactory suppression of Li dendrite growth). We designed and synthesized a series of zPU [i.e., poly ((diethanolamine ethyl acetate)-co-poly(tetrahydrofuran)-co-(1,6-diisocyanatohexane))]. Our zPU-SPE can host an equal amount of lithium bis(trifluoromethanesulfonyl) imide (LiTFSI) without phase separation (up to 90 wt% of LiTFSI loading). The Li-ion conductivity value of zPU exponentially increases with the addition of LiTFSI and reaches 7.4 × 10-4 S/cm at 25° C, almost 14 times higher than that of poly(ethylene oxide) (PEO) SPE with ethylene oxide/Li+ ratio = 16. In addition, its superior adhesion energy (487.5 J/m2 of zPU-SPE vs. 150 J/m2 of commercial 3M Scotch Tape) can minimize interfacial resistance between electrode and SPE, and thus cell resistance of 100-µm-thick zPU SPE is as low as 280 W/cm2 compared to 1230 W/cm2 of the cell with a similar thickness of PEO SPE. Our zPU-SPE also showed an excellent elastic property with a tensile break of 1700% owing to its high density of inter- and intra-molecular hydrogen bonding in polymer matrix. The SLB battery performance of PEO and zPU-SPEs was evaluated using a solid-state Li/SPE/LiFePO4 cell; the assembled SLB cell was cycled at a constant current rate of 1 C at 25 °C. After a discharge capacity of the cell with zPU-SPE stabilized at 100 mAh g-1 after 15 cycles, there was a negligible capacity decrease (only 3% capacity decrease after 500 cycles), delivering a discharge capacity of 97 mAh g-1 with stable Coulombic efficiency (100%) over entire cycles. However, the discharge capacity of Li/PEO/LiFePO4 cells drops rapidly to 3 mAh g-1 after 100 cycles. These results demonstrate that the SLB cell assembled with PCB-PTHFU shows high discharge/charge capacity and excellent capacity retention with stable Coulombic efficiency. The good electrochemical performance of the zPU SPE can be attributed to good compatibility with electrodes, low charge transfer resistance at the interface of electrode/electrolyte, and high Li-ion conductivity, strongly suggesting that zPU SPEs are potential candidates for development of high performance of SLBs. Figure 1
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Méry, Adrien, Steeve Rousselot, David Lepage, David Aymé-Perrot, and Mickael Dollé. "Limiting Factors Affecting the Ionic Conductivities of LATP/Polymer Hybrid Electrolytes." Batteries 9, no. 2 (January 28, 2023): 87. http://dx.doi.org/10.3390/batteries9020087.
Full textAbstract:
All-Solid-State Lithium Batteries (ASSLB) are promising candidates for next generation lithium battery systems due to their increased safety, stability, and energy density. Ceramic and solid composite electrolytes (SCE), which consist of dispersed ceramic particles within a polymeric host, are among the preferred technologies for use as electrolytes in ASSLB systems. Synergetic effects between ceramic and polymer electrolyte components are usually reported in SCE. Herein, we report a case study on the lithium conductivity of ceramic and SCE comprised of Li1.4Al0.4Ti1.6(PO4)3 (LATP), a NASICON-type ceramic. An evaluation of the impact of the processing and sintering of the ceramic on the conductive properties of the electrolyte is addressed. The study is then extended to Poly(Ethylene) Oxide (PEO)-LATP SCE. The presence of the ceramic particles conferred limited benefits to the SCE. These findings somewhat contradict commonly held assumptions on the role of ceramic additives in SCE.
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Zhu, Hongli, and Xiao Sun. "High-Performance All-Solid-State Li-S Batteries Enabled by Reaction Kinetics Enhancement and Interface Stabilization." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 468. http://dx.doi.org/10.1149/ma2022-024468mtgabs.
Full textAbstract:
Compared to the conventional lithium-sulfur (Li-S) batteries using liquid electrolytes, all-solid-state lithium-sulfur batteries (ASSLSBs) own the merits of eliminating polysulfide shuttle effects, potentially higher energy density, and superior safety. However, there are challenges of low utilization of sulfur caused by poor ion and electron conductions in the cathode, huge interfacial resistance due to the contact loss caused by huge volume change of sulfur during cycling, and sluggish reaction kinetics and higher thermodynamic barriers because of the one-step reaction from S8 to Li2S reactions. Also, the carbon additive could accelerate the decomposition of sulfide solid-state electrolyte (SSE) resulting newborn impedance. Therefore, it is significant to interface engineering the carbon additive through surface modification and functionalization to improve the electrochemical stability, charge transfer, and reaction kinetics in ASSLSBs. Herein, for the first time, we designed a highly conductive carbon fiber decorated with vertically grown MoS2 nanosheets and applied it in ASSLSBs. The chemical and electrochemical compatibility among MoS2, sulfur, and sulfide SSE can greatly improve the stability of the cathode and therefore maintain pristine interfaces between the different compositions for stable ion and electron transport. The presence of electrical-conductive metallic 1T MoS2 and its uniform distribution on carbon fiber without aggregation benefit the electron transfer between carbon and sulfur. Meanwhile, the unique layered structure of MoS2 can be intercalated by a large amount of Li atoms and therefore facilitate both ionic and electronic conductivity. In consequence, the charge transfer and reaction kinetics were greatly enhanced, and the decomposition of SSEs was successfully relieved. As a result, our ASSLSB delivered an ultrahigh initial discharge capacity of 1456 mAh g-1 with ultrahigh initial coulombic efficiency and maintained high-capacity retention of 78 % at 0.1 C after 220 cycles. The batteries also obtained remarkable rate performance of 1069 mAh g-1 at 1 C. This study pioneered new idea that fabricating the high performance ASSLSBs through developing surface functionalized and stabilized conductive carbon additives with metal sulfides.
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Minnmann, Philip, Anja Bielefeld, Raffael Ruess, Simon Burkhardt, Sören L. Dreyer, Enrico Trevisanello, Philipp Adelhelm, et al. "Evaluating Kinetics of Composite Cathodes of All-Solid-State Batteries." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2496. http://dx.doi.org/10.1149/ma2022-0272496mtgabs.
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ASSBs (all-solid-state batteries) are promoted as an energy dense and safe alternative to current Li-ion batteries (LIBs) and attract great interest from academia and industry. In contrast to LIBs, which employ a liquid organic electrolyte, they utilize a solid electrolyte. This substitution promises to eliminate the flammability of the battery and to simplify the cell design. While recent research efforts have concentrated on miniaturizing and eventually even removing the anode host material in batteries, the relative portion of the cathode needs to be maximized, as cathodes are the only component that can increase energy density by increasing its fraction. In a simplified view, the cathode kinetics are determined by the cathode microstructure, the volume fractions of the constituents and the properties of electrolyte and cathode active material (CAM). Liquid electrolytes can easily penetrate porous composite cathodes, but rigid SEs can not do the same, resulting in residual porosity in the cathode. This porosity can lower active interface area between CAM and SE, and increase tortuosity of ionic and electronic charge transport pathways. Sufficient ionic and electronic transport pathways in composite cathode structures are, however, essential because cathode active material particles that are either electronically or ionically isolated cannot contribute to the charging or discharging process. We analyse the requirements for SSB cathodes and determine charge transport bottlenecks by impedance spectroscopy of a reference system consisting of a thiophosphate based solid electrolyte and a nickel rich layered CAM. Different cathode microstructures are analysed and their charge transport properties are quantified as partial conductivities. From the obtained partial conductivities, we calculated tortuosity factors and correlated them to cell performance with complementary cycling data of all-solid-state batteries in order to determine charge transport bottlenecks. We find, that ionic charge transport and consequently cathode kinetics are highly dependent on the SE particle size distribution In addition, we analyse the requirements for CAMs for SSBs and develop design principles for different CAM types that aim to further increase cathode performance.
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Méry, Adrien, Steeve Rousselot, David Lepage, and Mickaël Dollé. "A Critical Review for an Accurate Electrochemical Stability Window Measurement of Solid Polymer and Composite Electrolytes." Materials 14, no. 14 (July 9, 2021): 3840. http://dx.doi.org/10.3390/ma14143840.
Full textAbstract:
All-solid-state lithium batteries (ASSLB) are very promising for the future development of next generation lithium battery systems due to their increased energy density and improved safety. ASSLB employing Solid Polymer Electrolytes (SPE) and Solid Composite Electrolytes (SCE) in particular have attracted significant attention. Among the several expected requirements for a battery system (high ionic conductivity, safety, mechanical stability), increasing the energy density and the cycle life relies on the electrochemical stability window of the SPE or SCE. Most published works target the importance of ionic conductivity (undoubtedly a crucial parameter) and often identify the Electrochemical Stability Window (ESW) of the electrolyte as a secondary parameter. In this review, we first present a summary of recent publications on SPE and SCE with a particular focus on the analysis of their electrochemical stability. The goal of the second part is to propose a review of optimized and improved electrochemical methods, leading to a better understanding and a better evaluation of the ESW of the SPE and the SCE which is, once again, a critical parameter for high stability and high performance ASSLB applications.
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Liu, Ying, Fang Fu, Chen Sun, Aotian Zhang, Hong Teng, Liqun Sun, and Haiming Xie. "Enabling Stable Interphases via In Situ Two-Step Synthetic Bilayer Polymer Electrolyte for Solid-State Lithium Metal Batteries." Inorganics 10, no. 4 (March 29, 2022): 42. http://dx.doi.org/10.3390/inorganics10040042.
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Poly(ethylene oxide) (PEO)-based electrolyte is considered to be one of the most promising polymer electrolytes for lithium metal batteries. However, a narrow electrochemical stability window and poor compatibility at electrode-electrolyte interfaces restrict the applications of PEO-based electrolyte. An in situ synthetic double-layer polymer electrolyte (DLPE) with polyacrylonitrile (PAN) layer and PEO layer was designed to achieve a stable interface and application in high-energy-density batteries. In this special design, the hydroxy group of PEO-SPE can form an O-H---N hydrogen bond with the cyano group in PAN-SPE, which connects the two layers of DLPE at a microscopic chemical level. A special Li+ conducting mechanism in DLPE provides a uniform Li+ flux and fast Li+ conduction, which achieves a stable electrolyte/electrode interface.LiFePO4/DLPE/Li battery shows superior cycling stability, and the coulombic efficiency remains 99.5% at 0.2 C. Meanwhile, LiNi0.6Co0.2Mn0.2O2/DLPE/Li battery shows high specific discharge capacity of 176.0 mAh g−1 at 0.1 C between 2.8 V to 4.3 V, and the coulombic efficiency remains 95% after 100 cycles. This in situ synthetic strategy represents a big step forward in addressing the interface issues and boosting the development of high-energy-density lithium-metal batteries.
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Zhang, Qiangqiang, Yaxiang Lu, Weichang Guo, Yuanjun Shao, Lilu Liu, Jiaze Lu, Xiaohui Rong, et al. "Hunting Sodium Dendrites in NASICON-Based Solid-State Electrolytes." Energy Material Advances 2021 (May 22, 2021): 1–10. http://dx.doi.org/10.34133/2021/9870879.
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NASICON- (Na superionic conductor-) based solid-state electrolytes (SSEs) are believed to be attracting candidates for solid-state sodium batteries due to their high ionic conductivity and prospectively reliable stability. However, the poor interface compatibility and the formation of Na dendrites inhibit their practical application. Herein, we directly observed the propagation of Na dendrites through NASICON-based Na3.1Zr2Si2.1P0.9O12 SSE for the first time. Moreover, a fluorinated amorphous carbon (FAC) interfacial layer on the ceramic surface was simply developed by in situ carbonization of PVDF to improve the compatibility between Na metal and SSEs. Surprisingly, Na dendrites were effectively suppressed due to the formation of NaF in the interface when molten Na metal contacts with the FAC layer. Benefiting from the optimized interface, both the Na||Na symmetric cells and Na3V2(PO4)3||Na solid-state sodium batteries deliver remarkably electrochemical stability. These results offer benign reference to the maturation of NASICON-based solid-state sodium batteries.