Solid-State Electrolytes in EV Battery Design

Solid-state lithium metal batteries (SSLMBs) are regarded as the next-generation energy storage systems, offering enhanced safety and higher density. Polyethylene oxide-based solid-state electrolytes (SSEs) have garnered significant attention due to their advantages, including superior safety, straightforward fabrication processes, high However, low ionic conductivity has hindered commercialization of SSLMBs. In this study, we developed a modified grafting PEG onto material COF-5-6 SSE slurry, which was coated surface LiFePO4 cathode construct an integrated for The B atoms in COF-5-6-PEG serve Lewis acid sites, adsorbing anchoring anions from salts, thereby promoting dissociation salts releasing more Li+. Additionally, S O polar complex with Li+, facilitating solvation Li+ within flexible segments enabling rapid transport through interconnected channels. As result, membrane demonstrates 1.41 103 cm1 transference number 0.47, along stable polarization behavior over 400 h Li electrodes at 80 C. Moreover, Li||COF-5-6-PEG SSE||LiFePO4 cells exhibit dendrite-free surface, promi... Read More

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High-capacity lithium-rich manganese-based materials Li1.20Mn0.54Ni0.13Co0.13O2 (LRMs) are potential cathodes for solid-state lithium batteries with high energy density. However, there challenges of low initial Coulomb efficiency (ICE) and interfacial degradation the cathode caused by irreversible oxygen release. Here, oxygen-deficient ceria (CeO2-x) abundant vacancies was used to scavenge excess species manipulate evolution LRM in battery. CeO2-x realizes reversible storage release anion vacancies, doping Ce3+/4+ into lattice stabilizes structure enhances Li+ transport kinetics. Therefore, cell a NASICON-type F-doped Li1.3Al0.3Ti1.7(PO3.93F0.07)3 (F-LATP) solid electrolyte shows ICE 86.74%, an outstanding rate performance 70.0 mAh g-1 at 1 C, remarkable cyclability lower capacity decay 0.27% per cycle. It is believed that this work provides valuable guidance design redox high-capacity LRMs batteries.

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Bipolar lithium battery packs for high energy density applications like electric vehicles with reduced flammability and improved safety compared to conventional liquid electrolyte batteries. The packs use bipolar electrodes with solid electrolytes sandwiched between the electrode layers instead of liquid electrolytes. The electrodes have a current collector, cathode, and optionally an anode. The solid electrolyte is a hybrid of an inorganic solid electrolyte and a solid polymer electrolyte. The packs are made by stacking the bipolar electrodes with separators between them to form modules.

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Abstract Sulfide solid electrolytes (SSEs) exhibit exceptional ionic conductivity and processing advantages for allsolidstate lithium metal batteries (ASSLBs), but their commercialization is constrained by ambient hydrolysisinduced H 2 S generation dendrite formation at electrolyte/anode interfaces. Herein, a Ce/O cosubstitution strategy employed to synthesize argyroditetype Li 5.4+x P 1x Ce x 4.42x O 2x Cl 1.6 (0 0.05) electrolytes. The substitution of 5+ with 4+ 2 2 in the PS 4 3 structure forms stable CeS 4 3 groups enhances structural integrity. Simultaneously, incorporation expands lattice spacing facilitates + transport. Optimized 5.42 0.98 0.02 4.36 0.04 electrolyte exhibits superior (7.13 mS cm 1 ) excellent air stability (H emission: 0.36 g after 30 min 30% RH). demonstrates an enhanced critical current density 1.3 mA 2 plating/stripping over 5000 h 0.1 . ASSLBs LiNbO @NCM622 cathodes deliver initial discharge capacity 128.19 mAh 99.49% retention 300 cycles. This work provides designing highperformance SSEs toward practical batte... Read More

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Synthesizing high-performance lithium lanthanum zirconate (LLZO) solid electrolyte for lithium-ion batteries by starting with lanthanum zirconate (LZO) nanocrystals. The LLZO is formed by dispersing LZO nanocrystals in a slurry with lithium and lanthanum compounds, drying and calcining the slurry to transform the LZO nanocrystals into LLZO. This allows direct synthesis of LLZO using LZO nanocrystals as precursors instead of starting from scratch.

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A solid electrolyte material for solid-state lithium batteries that provides improved properties like purity, crystalline structure, ionic conductivity, electronic conductivity, mechanical properties, electro-chemical stability, etc. The electrolyte is a quaternary halide material containing alkali, other metal, and halide ions. It has reduced contents of binary, oxyhalide, and water-insoluble impurity phases compared to conventional halides. The quaternary halide can have mixed crystalline interphases with nearest atomic distances <0.5 nm and larger nanometric domains.

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Abstract The fundamental interactions and the as-derived microstructures among electrolyte components play a pivotal role in determining bulk interfacial properties of electrolytes. However, complex structure-property relationships remain elusive, leading to uncontrollable physicochemical characteristics electrolytes unsatisfied battery performance. Herein, we propose two interaction motif descriptors quantify ion-solvent spanning electrostatic dispersion regimes. These are highly relevant salt dissolution, phase miscibility, electrode-electrolyte interface chemistries. Guided by principle minimizing solvent-solvent while ensuring sufficient dissociation, representative electrolyte, i.e ., lithium bis(fluorosulfonyl)imide dissolved trimethyl methoxysilane 1,3,5-trifluorobenzene with molar ratio 1:2.5:3.0, is designed, which achieves ~99.7% (0.2%) Li plating/stripping Coulombic efficiency endows 4.5 V Li||LiCoO 2 90% capacity retention after 600 cycles at 0.2 C/0.5 C charge/discharge rate. Notably, Cu||LiNi 0.5 Co Mn 0.3 O pouch cells this sustain over 100 stable cycles. By establis... Read More

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Synthesizing lithium lanthanum zirconate (LLZO), a fast ion conducting solid electrolyte for lithium-ion batteries, using molten salt synthesis to produce pure cubic LLZO without the need for high temperatures or dopants. The synthesis involves combining metal oxide precursors like lithium nitrate, lanthanum nitrate, and zirconium oxynitrate with a molten salt medium like eutectic lithium chloride-potassium chloride. The molten salt is heated to yield pure cubic LLZO that can be washed to obtain powder. The molten salt composition and precursor ratios can be tuned to achieve phase pure LLZO synthesis.

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Abstract The highvoltage reactivity and flammability of electrolytes remain critical challenges for highsafety highenergydensity lithium metal batteries (LMBs). Here, a novel ceramicether coupling electrolyte (CCE) is reported, in which thin liquid layer the ether immobilized on particle surface Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) matrix through coordination interactions. With an LLZTO content exceeding 82%, it demonstrates high plasticity, nonflammability, oxidation voltage threshold above 5.0 V. strong interactions between solvent molecules or anions are revealed, generate cohesive forces that impart highplastic rheological behavior to matrix, ensuring conformal contact at solid/solid interfaces. These also lead loose + solvation sheath electrolyte, not only accelerates transport, achieving ionic conductivity 2.7 10 4 S cm 1 , but promotes anion decomposition form inorganicrich cathode interphase (CEI). This enables Li/LiNi 0.8 Co 0.1 Mn 2 (NCM811) cells operate stably cutoff 4.5 work can open up new insights into design safety LMBs.

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All-solid-state lithium-metal batteries (ASSLMBs) are promising for transportation electrification due to their superior safety and high energy density. Lithium halide electrolytes provide excellent processing flexibility, ionic conductivity, anodic stability (>4.1 V), making them highly compatible with high-voltage cathodes, surpassing sulfide (<2.1 V). Nevertheless, suffer from low cathodic form an electronically conductive interphase lithium, resulting in a critical current density (CCD) of nearly zero. Herein, Li3YbCl6 synthesized that kinetically stable lithium by forming electronic insulating solid electrolyte interphase. Guided overpotential criteria, PI3 interlayer is designed transforms into Li6PI3 upon contact substantially reducing the interfacial resistance against 34 achieving 114 mV. By substituting Yb Lu, Li3LuCl6 interlayers reach CCD 1.0 mA cm-2 at capacity mAh cm-2, comparable but higher oxidation stability. Additionally, enables cycling Li//Li cells 0.5 400 cycles maintains 86.5% Li//LiCoO2 after 220 30 C, paving way high-performance ASSLMBs.

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Standalone solid electrolyte sheets for lithium batteries that are freestanding, amorphous, and highly lithium ion conductive to enable high performance lithium batteries without the need for a liquid electrolyte. The solid electrolyte sheets are made from continuous sulfide glasses with intrinsic room temperature lithium ion conductivity above 10^-4 S/cm. The glass sheets have parallel edges, battery size, and are self-supporting. The sulfide glass composition and processing are optimized for interfacial stability with lithium metal. The continuous glass sheets can be cut into separators for battery cells or used as substrates for electrode assemblies.

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Abstract Polyethylene oxide (PEO) electrolytes hold significant potential for the nextgeneration allsolidstate lithium metal batteries. However, their practical application is limited by low ionic conductivity, unstable solid electrolyte interphase (SEI) and, especially, poor oxidative stability under high voltages. Herein, a fillermodified PEO proposed to address these challenges. The filler, TIO (SnO 2 doped with In O 3 ), rich in oxygen vacancies, acting as Lewis acids interact TFSI , which releases more Li + and achieves higher conductivity transference number. Moreover, Sn 4+ /In 3+ can form alloy phases facilitate deposition transport across SEI. Consequently, Li//LiFePO 4 cells using exhibit reversible capacity of 140 mAh g 1 excellent retention 92% over 800 cycles at 0.2 C. Importantly, interacts hydroxy groups H atom on C PEO, reducing PEO's reactivity extending its decomposition 4.75 V. Owing inhibited upon highvoltage cycling, enables Li//LiNi 0.8 Co 0.1 Mn achieve an outstanding initial 170 maintain 70% 200 0.5 C cutoff voltage 4.3

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ABSTRACT With the advancement of global dualcarbon goal, green technology has become a priority in energy field. Among storage technologies, allsolidstate batteries attract significant attention due to their high density, enhanced safety, and long cycle life. Poly(ethylene oxide) (PEO)based polymer solidstate electrolytes are research hotspot for nextgeneration lithiummetal because flexibility, filmforming capabilities, compatibility with lithium salts. In this study, cyclodextrin (CD) is employed as filler combined highmodulus polyacrylonitrile (PAN) fibers plastic crystalline succinonitrile (SN) synergistically enhance electrochemical mechanical properties PEObased electrolytes. The PAN/PEO/LiClO 4 /CD/SN electrolyte achieves an ionic conductivity 6.5 10 5 S cm 1 at 30C ion transference number 0.33 80C. PAN fiber significantly improves properties, achieving tensile strength exceeding eight times that PEO/LiClO membrane. Li/Li symmetric batteries, demonstrates excellent interfacial stability over 1100 h 0.1 mA 2 . Additionally,... Read More

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Ceramic material for solid-state batteries with improved lithium ion conductivity, lower manufacturing energy requirements, and better moisture resistance compared to traditional ceramic electrolytes. The ceramic contains a lithium ion conductor like LLZO or LATP along with a lithium metal halide like lithium indium chloride. The halide allows preparing the ceramic at lower temperatures and pressures instead of sintering at high temps for hours. It also improves moisture tolerance as the halide absorbs water instead of the main conductor. The ceramic can be used as a solid-state electrolyte in batteries.

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Abstract Lithium argyrodite sulfide electrolytes show great potential in allsolidstate lithium metal batteries (ASSLMBs) due to their high ionic conductivity and ductile feature, among which Li 6 PS 5 I presents the most promising stability with metals but a low (10 6 S cm 1 ). It is because of absence 2 /I disorder thus forbidden + ion intercage migrations. Herein, particles iodinegradientdisordered interphase were designed that opened up proscribed jumps synergistically blocked interfacial electron leakage for ultrastable ASSLMBs. Density functional theory calculations 7 spinlattice relaxation NMR experiments prove activated even accelerated conduction reduced migration barrier. Electrostatic profiles also certify transitionshielding as origin parasiticreactionfree interface. Gathered evidence of, other characterizations demonstrated combination conductivities (cold press 5.7 mS ), (1.510 8 improved critical current density (1.65 mA 2 excellent (over 1,500 h) prominent cycling rate performance. This study provides insights on novel de... Read More

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Abstract Polymer in ceramic (PIC) electrolytes have garnered significant attention due to their advantages over individual inorganic and organic polymer electrolytes. However, the slow movement of Li + on chain segments hard contact among particles with irregular surface severely impede smooth transport lithium ions. The bipolar character Nmethyl2,2,2trifluoroacetamide (MFA) makes it significantly enriched surface, accordingly converting between into a soft mode, opening up ion multiple phases. structure fluorine substitution further disperses negative charge density carbonyl group from MFA accelerates ligand removal . Accordingly, interconnected PIC electrolyte (MPIC) exhibits an ionic conductivity 1.13 mS cm 1 transfer number 0.81 at 30 C, also delivering remarkable critical current 2.6 mA 2 corresponding full cell can achieve stable cycling high 1.2 even 20 still retains 94% its capacity after 100 cycles, overcoming temperature limitations. This work paves way for designing commercial viability by interphase regulation.

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The uncontrollable growth of lithium dendrites and the unstable interface metal anode/electrolyte inhibit potential large-scale applications batteries. polymer artificial solid-electrolyte layer shows for homogeneity ion flux toward a electrode. Herein, we design an ionic conductive stretchable organogel as protective via in situ polymerization on active anode, which can accommodate volume changes maintain enhanced interfacial contact with propylene carbonate long alkyl ether contribute to inducing uniform Li deposition enhance transport. In addition, membrane adheres tightly effectively eliminate barriers transport at heterogeneous interfaces has strength tending suppress dendrites. As result, Li/Li symmetric cell this polymeric protect stably cycle over 800 h under 1 mA cm-2 without increased polarization voltage, while corresponding metal/LiFePO4 full battery delivers high-capacity retention 102.6, 127.7, 136.7% after 244, 862, 976 cycles 0.3, 1, 2 C. Furthermore, equipped also longer cycling life higher reversible specific capacity (130.24 mAh g-1) C rate performance than bare ba... Read More

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An all-solid-state battery with improved charge/discharge efficiency and lifespan compared to conventional solid-state batteries. The battery uses a coating layer made of a porous network of intertwined fibrous carbon that is coated with an inorganic electrolyte. This coating layer is sandwiched between the anode current collector and the solid electrolyte. The coating provides balanced ionic and electronic conductivity, eliminating the need for a separate anode active material. The coated porous carbon network allows lithium intercalation/deintercalation without internal short circuits, improving cycling stability.

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High-ionic-conductivity solid electrolyte for lithium-ion batteries that can be produced by sintering at low temperatures. The solid electrolyte contains an oxide with the general formula Li6-xR1-y-aAy-bMx(BO3)3, where R is a rare earth element, A is an alkali or transition metal, M is a tetravalent element, and x, y, a, and b are real numbers. The electrolyte exhibits specific X-ray diffraction peaks with a certain angular separation. This composition and structure allows high ionic conductivity when sintered at low temperatures compared to traditional sulfide-based electrolytes.

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Improving electrical contact between the anode and solid-state electrolyte in all-solid-state batteries using a chemical connection process. The process involves adding a small amount of a chemical compound to the solid-state electrolyte surface before adding the anode. This forms a specialized solid electrolyte interphase layer that enables better electrical connection between the anode and electrolyte compared to unmodified electrolytes. The chemical connection process allows using phthalocyanine solid-state electrolytes, which are not ductile and cannot flow under high pressure like some other electrolytes, in solid-state batteries.

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