General Motors Developments in Solid-State Battery Technology

Reducing interfacial impedance between solid electrolytes and solid electrodes in solid-state batteries by incorporating thin layers of liquid metal between them. The liquid metal composition, containing gallium, is applied to the solid electrode and electrolyte surfaces in a controlled environment with oxygen to form oxide coatings that reduce surface tension and improve wetting. The liquid metal fills in surface voids and forms continuous interfacial layers between the solids, improving contact and charge transfer.

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Semi-solid electrolyte system for solid-state lithium-ion and lithium metal batteries that provides improved stability and ionic conductivity. The system uses a combination of oxysulfide solid electrolyte and a solvated ionic liquid as the electrolyte. The oxysulfide solid electrolyte facilitates ion transfer between the electrodes and also acts as a separator. The solvated ionic liquid fills some of the pores in the separator to further enhance ionic conductivity. This allows high ionic conductivity and current density at lower stack pressures compared to just using the solid electrolyte. It also provides chemical stability and longer cell life compared to just using the solvated ionic liquid.

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Battery cell design with functionalized separators to improve performance and safety. The separator between the anode and cathode contains a lithium-ion conductive solid electrolyte and an active capacitor material. This functionalized separator allows high current density, reduces internal resistance, and mitigates thermal runaway compared to regular separators. It also provides capacitive energy storage to smooth out current peaks during charging and discharging.

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A solid-state battery design using an elastomer layer between the solid electrolyte and silicon anode to mitigate volume expansion and cracking of the anode during charging. The elastomer layer contains a plasticizer and a lithium ion conductive medium. The elastomer absorbs the anode expansion and contracts during charging/discharging to prevent cracking and pulverization. It also improves ionic interface between the solid electrolyte and anode. The elastomer layer is sandwiched between the solid electrolyte and silicon anode in the battery cell.

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Anode electrode for all-solid-state batteries with patterned silicon to improve performance and lifetime. The anode has arrays of silicon pillars arranged in a pattern with empty spaces between. This allows Si expansion during charging without cracking, as the pillars compress and the spaces accommodate volume change. The pillars also provide high lithium ion conductivity to the solid electrolyte. The pattern is created by selectively removing silicon or masking before deposition.

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All-solid-state battery (ASSB) cells with patterned silicon anodes that improve cycle life and performance compared to traditional solid-state batteries. The anodes have silicon columns arranged in a predetermined pattern with voids between them. The voids allow the silicon to expand during charging without cracking or pulverization like solid silicon anodes do. This reduces stress and extends cycle life. The voids also help relieve stress caused by lithium ion diffusion. The patterned silicon anodes also promote lithium ion conduction between the silicon and solid electrolyte to improve battery performance. The voids are created by laser patterning or masking before depositing the silicon columns.

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Reducing impedance and improving cycle life in solid-state lithium metal batteries by forming an interfacial layer between the lithium metal anode and the solid electrolyte. The interfacial layer is formed by coating the lithium metal with a mixture of lithium nitrate, trimethyl phosphate, and dimethoxyethane. This coating reduces side reactions between the lithium and the electrolyte, improves contact, and lowers interfacial impedance compared to bare lithium. The coated lithium metal is then assembled into a solid-state battery cell with the electrolyte.

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Bicontinuous solid-state battery separators that address issues like limited energy density and lithium plating in solid electrolytes. The separators have a porous matrix filled with a solid electrolyte powder. The solid electrolyte is dispersed in the matrix pore structure. This allows efficient ionic conduction through the solid electrolyte filled pores while preventing lithium metal deposition in the porous matrix. The porous separator with dispersed solid electrolyte provides a continuous pathway for ionic transport with reduced resistance compared to solid electrolytes alone. The porous matrix also limits lithium metal plating compared to solid electrolytes.

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Solid-state battery design with uniformly distributed solid-state electrolyte for improved performance. The batteries have solid electrodes with apertures through them that are filled with a solid-state electrolyte precursor solution. The stack is then heated to solidify the electrolyte and form a homogeneous distribution throughout the battery. This improves contact between electrode particles and electrolyte compared to non-uniform electrolyte distribution. The apertures allow the electrolyte to fill voids and pores in the electrodes.

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A high-speed manufacturing method for all-solid-state batteries with improved flexibility and efficiency compared to conventional stacking methods. The method involves continuously fabricating expandable anode electrodes or zigzag stacking continuous cathode electrodes. The expandable anode has a continuous anode current collector with anode material on both sides. The continuous cathode electrodes have cathode material on both sides. The expandable anodes or zigzag stacked cathodes are arranged in an alternating pattern to form the battery cell. This allows faster, more efficient production compared to individually punched electrodes and reduces positioning errors. The use of expandable anodes and zigzag stacking enables higher flexibility in the battery design. The anode and cathode electrodes can be made using roll-to-roll manufacturing techniques. Sulfide-based electrolytes are also used in the battery

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Solid state lithium ion batteries with improved cycle life and rate performance by using a fibrillated polymer network in the electrode instead of a binder. The electrode active material, electrolyte, and conductive particles are mixed with fibrillated polymer particles and a processing additive like activated carbon. The mixture is consolidated into a film without solvents, forming a fibrous network with distributed particles. This provides a structurally reinforced electrode without separate binders that can degrade during cycling. The fibrillated polymer network improves cycle life and rate performance compared to conventional binders.

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Solid-state lithium-ion battery electrodes with improved cycling performance and capacity retention compared to conventional solid-state batteries. The electrodes have a porous active layer made of a fibrillated polymer network with dispersed solid particles. The fibrillated polymer is a fibrous network with an average fiber diameter of 20-300 nm. The particles include electroactive material, solid electrolyte, and porous fibrillation particles. The fibrous network provides mechanical stability and a high surface area for the solid particles. The solventless fabrication process uses heat and avoids solvents to form the electrode. The fibrillated polymer electrode shows improved cycling performance compared to conventional solid-state electrodes.

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Scalable manufacturing process for solid-state batteries using continuous high-speed zigzag stacking of bendable anode and cathode electrodes. The process allows large-scale production of solid-state batteries with improved safety and performance compared to liquid electrolyte batteries like lithium-ion. The process involves continuously bending and stacking the anode and cathode electrodes in a zigzag pattern to form the battery stack. This allows continuous production of solid-state battery cells without the need for cutting and joining of separate electrodes. The bendable electrodes can contain individual anode or cathode layers. The process can use sulfide-based electrolytes for improved safety compared to traditional organic electrolytes.

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Tabless solid-state battery design with integrated cell structure and housing for improved energy density and simplified manufacturing compared to conventional tabbed solid-state batteries. The tabless battery has parallel-connected anode and cathode electrodes arranged as a cell core. Multiple cell cores are stacked between plated sheets in the housing. The plated sheets have channels for receiving and positioning the electrodes. Terminals are integrated into the housing end walls. This eliminates the need for external tab connections. The simplified cell structure reduces parts count and improves consistency compared to separate tabbed cells. The integrated design also simplifies cooling and assembly.

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Method for manufacturing sulfide impregnated solid state batteries with improved performance and reduced cost compared to conventional methods. The method involves impregnating a sulfide-based solid electrolyte into a partially sealed battery cell instead of mixing it with the active material slurry. This is done by introducing a sulfide electrolyte precursor solution into the cell, evaporating the solvent, curing the electrolyte in situ, densifying it under pressure, and sealing the cell. The impregnated electrolyte forms a tight interface with the electrodes without moisture exposure, improving battery performance.

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Free-standing thin electrolyte layer for solid-state batteries with high conductivity and reduced thickness, as well as improved mechanical properties. The electrolyte layer has a porous scaffold and a solution processable solid electrolyte filling the pores. The scaffold provides mechanical support while allowing the electrolyte to penetrate and form a homogenous layer. The scaffold has high porosity (50-90%) to enable easy impregnation of the electrolyte. The electrolyte can be a sulfide-based solid or a mixture of solid and liquid phases. The scaffold can be made of fibers with diameters of 0.01-10 microns and lengths of 1-20 microns. The layer is formed by contacting the scaffold with a precursor solution containing the electrolyte, allowing it to penetrate,

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Thin, porous electrolyte layers for solid-state batteries that improve performance and safety. The electrolyte layers contain a solution-processable solid electrolyte material that partially fills the pores of a porous framework. The layers can be made by depositing the electrolyte precursor solution into the framework pores. This allows thin, flexible, and conformable electrolyte layers with high porosity (50-90%) for solid-state batteries. The solid electrolyte material fills the framework pores to provide a conductive pathway for lithium ion movement. The thin, porous electrolyte layers enable better interfacial contact with the battery electrodes and reduce the risk of internal short circuits compared to solid electrolyte layers.

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An all-solid-state battery design with improved power capability and energy density. The battery uses a negative electrode made of columnar silicon with in-situ formed sulfide electrolyte. The columnar silicon structure with voids between the pillars allows the sulfide electrolyte to fill the voids. This provides high electrolyte volume filling, reducing interfacial resistance compared to solid electrolyte only. The columnar silicon anode with sulfide electrolyte is formed by contacting a columnar silicon film with a sulfide precursor electrolyte, then removing the solvent to infiltrate the voids.

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Solid-state batteries with reduced porosity electrolytes, and methods to make them. The solid electrolyte is represented by Li3AB6 where A is Yttrium, Indium, Scandium, Erbium, or combinations, and B is Chloride, Bromide, ClxBr(x-1), with 0 < x < 1. The battery structure has a separator between the positive and negative electrodes. The positive electrode contains the electroactive material and solid electrolyte. The negative electrode may also have electroactive material. The solid electrolyte layer can be formed simultaneously with the positive electrode. This reduces porosity compared to separate layers. The reduced porosity improves battery performance by reducing electrolyte degradation and preventing short circuits.

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<|assistant|> Solid-state batteries for electric vehicles that use sulfide electrolytes inside columnar silicon anodes. The batteries have an electrode structure with a void space filled by a solid sulfide electrolyte. The electrode comprises a stack of hierarchical silicon columns with openings between them. The electrolyte is formed by infiltrating a precursor solution into the silicon stack and then removing the solvent. This avoids the need for liquid electrolytes and separators in all-solid-state batteries. The columnar silicon anodes enable higher capacity compared to planar silicon anodes. The sulfide electrolyte provides stable cycling and intercalation between the silicon and electrode active materials.

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A solid-state battery design that eliminates the need for a separate anode by using a bare current collector and a gel electrolyte. The battery has a cathode layer with a host cathode material containing transient anode elements. During charging, the gel electrolyte extracts anode elements from the cathode and deposits them on the bare collector. During discharging, the gel returns the anode elements back to the cathode. This allows the battery to operate without a separate anode by using the gel electrolyte to diffuse anode elements between the cathode and collector.

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Anode-less lithium metal battery with a three-dimensional porous negative electrode current collector to prevent dendrite formation and minimize volume changes during cycling. The battery has a solid electrolyte sandwiched between a positive electrode and a negative electrode current collector that has a porous structure with interconnected openings. During charging, lithium metal deposits inside the pores instead of plating on the collector surfaces. This prevents dendrite growth and volume changes compared to plating on flat surfaces.

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Battery cell with improved power capability and durability at low temperatures using a combination of reduction-resistant and oxidation-resistant solid electrolytes. The reduction-resistant electrolyte is used in contact with the anode and the oxidation-resistant electrolyte is used in contact with the cathode. This prevents electrolyte decomposition during charge/discharge cycles at low temperatures. The reduction-resistant electrolyte can be a Li-rich LLZO and the oxidation-resistant electrolyte can be Li-containing LATP. The amounts of these electrolytes in the anode and cathode layers are optimized to balance performance and stability.

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Solid state battery with graphite anode for improved performance and longevity. The graphite anode contains a mixture of high and low surface area graphite particles. The low surface area graphite reduces excessive SEI (solid electrolyte interface) formation during charging and discharging, preventing active lithium loss and resistance buildup. The high surface area graphite provides good electrical contact. This interface design strategy reduces total ion contact area between the gel electrolyte and graphite.

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Solid-state batteries with improved power and energy density by forming a continuous solid-state electrolyte network using a polymeric gel electrolyte. The polymeric precursor is contacted with the electrodes, filling voids between the active particles and reacting to form the continuous electrolyte layer. The precursor contains a crosslinkable polymer, plasticizer, and lithium salt. This provides enhanced interfacial contact and reduces resistance compared to separate electrode and electrolyte layers. The continuous electrolyte network enables higher power solid-state batteries.

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A solid-state lithium-ion battery cell design that provides high performance and durability at both low and high temperatures. The cell has a solid electrolyte sandwiched between the anode and cathode instead of the traditional liquid electrolyte. The solid electrolytes are reduction tolerant on the anode side and oxidation tolerant on the cathode side. This allows using the same solid electrolyte material on both sides, which improves compatibility and reduces interfacial reactions compared to using different solid electrolytes. The design improves battery performance at low temperatures, like winter conditions, and durability at high temperatures, like charging and discharging cycles.

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Solid state battery design with improved energy density and safety by impregnating sulfide-based solid electrolytes into the pore structure of the battery cells. The impregnation process involves dissolving the sulfide electrolyte in a solvent, filling the battery cells with the solution, evaporating the solvent to leave the impregnated electrolyte, and densifying it by pressure. This eliminates the need for large amounts of external electrolyte and reduces the risk of moisture reactions. The uniformly distributed impregnated electrolyte also improves the electrode-electrolyte interface and reduces the overall electrolyte content for higher energy density.

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Sulfide-based solid-state electrolytes for lithium-ion batteries that have improved conductivity and cost compared to conventional sulfide electrolytes. The method involves mixing a sulfate precursor with carbonaceous materials like activated carbon, graphene, or carbon nanotubes, then calcining to form an electrolyte precursor containing lithium sulfide. This precursor is further mixed with additional sulfide-containing electrolyte materials to form the final solid-state electrolyte. The carbonaceous materials enhance the electrolyte conductivity and power response compared to pure sulfides.

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Micro-sized secondary particles for solid-state lithium-ion batteries with enhanced ionic conductivity. The particles have a core of electrode material surrounded by a solid-state electrolyte. The electrode material can be a cathode or anode active material. The solid-state electrolyte penetrates the electrode material, improving ionic conductivity compared to traditional micro-sized particles with just a solid electrolyte coating. This allows solid-state batteries to have higher power, energy density, and thermal tolerance.

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Solid state battery electrolyte composition and preparation method that enables high ionic conductivity and stability for solid state batteries. The electrolyte composition is an argyrodite compound containing Li3PS4, which provides high ionic conductivity. The preparation method involves simultaneously or sequentially preparing suspensions of Li3PS4 and Li2S-LiX (where X is a halide) and mixing them to form a precursor liquid. The precursor liquid is then dried to obtain the solid argyrodite electrolyte. The simultaneous suspension preparation ensures homogenous mixing of the components. The drying step removes the solvent to form the solid electrolyte.

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Scalable manufacturing method for solid-state batteries with high-performance digermorite electrolytes. The method involves simultaneously preparing a digermorite electrolyte precursor by mixing a LiPS4 suspension with a Li2S:LiX solution containing alcohol and ester solvents. This precursor is then dried to form the digermorite electrolyte. This enables efficient and scalable production of the digermorite electrolyte compared to ball milling methods. The digermorite electrolyte has a composition Li6PS5X where X is Cl, Br, or I. It has high ionic conductivity (10^-3 - 10^-10 S/cm) and operates over a wide temperature range.

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Method to manufacture high performance solid state batteries with improved productivity. The method involves stacking multiple battery cells on a continuous bipolar current collector that is simultaneously wound into a stack. The stack is then compressed and cut to form the final solid state battery. This eliminates the need for separate cell assembly and stacking steps. The continuous winding allows efficient cell insertion and stacking. The compression improves battery performance by densifying the stack. The cut edges expose the battery electrodes for external connections. The method allows high throughput production of solid state batteries.

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Sulfide-impregnated solid-state battery design with uniformly distributed sulfide-based solid electrolyte (S-SSE) in the pore structures of the battery core. This provides intimate electrode-electrolyte interfaces and reduces S-SSE content while boosting power density compared to conventional S-SSBs. The battery design involves stacking cell units with cathode, anode, oxide electrolyte layers, and separators to form the core. The core is then impregnated with a sulfide precursor solution that solidifies and densifies inside the pore structure. This replaces the need for excess S-SSE in the electrodes. The impregnated core is sealed for the battery.

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A composite interlayer for lithium metal anode solid state batteries to improve performance and reduce degradation compared to using a solid electrolyte directly on the lithium metal. The interlayer contains an ionic conductor dispersed in an organic matrix. It is sandwiched between the lithium metal anode and solid electrolyte in the battery. The interlayer suppresses unwanted reactions between the lithium metal and solid electrolyte, reduces interfacial impedance, and improves contact compared to direct contact between the lithium metal and solid electrolyte. The organic matrix helps prevent voids and delamination between the electrolyte and anode.

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Method to restore solid state battery electrolyte layers that have formed passivation layers on their surfaces. The passivation layers can degrade battery performance. The restoration method involves removing the passivation layers using laser or plasma surface treatment. This improves battery characteristics like impedance and wettability.

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Ionically conductive polymer composite interlayer for use in solid state batteries. The interlayer is made by pressing an electroactive material layer, containing lithium metal, between two electrolyte layers. The applied pressure exceeds the yield strength of the lithium metal. This compresses the lithium metal to prevent dendrite growth and short circuits in the solid state battery. The ionically conductive polymer composite interlayer sandwiched between the electrodes improves battery performance and cycle life by suppressing lithium plating and dendrite formation in solid state batteries.

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Forming ion-conducting polymer composite interlayers between electrodes and solid-state electrolytes in solid-state batteries. The interlayers are formed by converting precursor layers into conductive polymer composites through heat and/or pressure. This improves electrical contact and reduces voids between the electrodes and electrolyte compared to using only solid materials. The precursor layers can contain fluoropolymers like PVDF to facilitate conversion. The interlayers have thicknesses of 10-1000 S/cm and contain lithium fluoride intercalated into carbonaceous matrices. The interlayers are formed on the electrode surfaces that align with the solid-state electrolyte surfaces.

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Solid state batteries with improved interfacial contact between the electrodes and electrolyte for better performance. The batteries have a solid electrolyte layer formed by reacting a polymer precursor containing crosslinkable polymer, plasticizer, and lithium salt. The precursor can be applied to the electrode or a separate layer, then cured to form the solid electrolyte. This provides better adhesion and contact between the electrodes and electrolyte compared to liquid electrolytes. The solid electrolyte can also be formed between electrodes by filling pores in a nonwoven mat or by filling voids between solid electrolyte particles. Alternatively, the solid electrolyte layer can be formed separately and then attached to the electrodes.

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Reducing interfacial impedance in solid-state lithium batteries by forming thin interfacial layers between the electrodes and solid electrolyte using liquid metal. The liquid metal composition is applied to the electrode or electrolyte surfaces in the presence of oxygen to form oxides that reduce surface tension. This allows the metal to wet and fill surface voids, improving contact and charge transfer. The liquid metal coating is then solidified between the electrodes and electrolyte to create thin interfacial layers. The liquid metal used is gallium, which melts at temperatures around 20-30°C, enabling room temperature application.

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Solid-state battery electrolyte made by a process that involves mixing a sulfide precursor with carbonaceous materials, calcining to form an electrolyte precursor containing Li2S, then mixing in additional components to create the solid electrolyte. The electrolyte has a composite structure with a carbon capacitor cluster coated in sulfide. This enables high sulfur content and solid-state separation without a separate separator. The composite structure improves electrolyte stability, conductivity, and cycling compared to homogeneous solid electrolytes.

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Solid-state battery electrolyte with improved interfacial contact between the electrodes and the electrolyte to enable better battery performance. The electrolyte is a softened version of a conventional oxide or sulfide-based solid electrolyte. It is softened by replacing some of the anions with larger radius anions. This reduces the elastic modulus of the electrolyte to make it more flexible. The softened electrolyte has better interfacial contact with the electrodes compared to the unsoftened electrolyte, especially with the positive electrode.

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Solid state batteries with thick electrodes and improved energy density for applications like electric vehicles. The batteries have electrodes with thicknesses of 100-3000 microns instead of the typical 50-200 microns. The thicker electrodes are made possible by embedding the active material particles in a porous metal foam that acts as a current collector. This allows higher loading of active material for more capacity. The foam also provides more contact area between the solid electrolyte and electrode particles. The thicker electrodes enable higher energy densities compared to thin electrodes. The thicker electrodes also have higher power capability due to the increased contact between the particles. The batteries also use thicker solid electrolyte layers and current collector foils.

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Solid-state battery with improved capacity and cycle life by using thicker electrodes and a solid electrolyte. The battery has a thicker first and second electrode, both over 100 microns thick, sandwiched around a solid electrolyte layer. The thicker electrodes contain embedded electroactive particles. This design reduces electrode resistance and improves capacity and cycle life compared to thin film electrodes used in most solid-state batteries. The thicker electrodes also allow for easier manufacturing and scaling of the batteries.

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Bipolar capacitor-assisted solid-state lithium ion battery with improved cold-cranking performance. The battery has solid-state electrolyte cells with capacitor material incorporated into the electrodes. The capacitor material, like supercapacitors, stores charge electrostatically and absorbs/de-absorbs ions quickly compared to the active electrode material. This enhances power density. However, the lower capacity of the capacitor material restricts energy density. The bipolar battery architecture mitigates energy density losses by stacking cells with capacitor-assisted electrodes.

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All-solid-state batteries with high-energy-density electrodes that can accommodate the volumetric expansion and contraction of high-capacity electroactive materials like silicon, sulfur, and tin during cycling. The electrodes have a controlled internal porosity in the electroactive material particles to allow inward expansion/contraction rather than outward expansion. This prevents micro-cracking and delamination compared to dense electrodes. The composite electrodes also have interparticle porosity between the electroactive material and electrolyte. This reduces overall electrode density but allows higher loading of the solid-state electrolyte.

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Fiber reinforced separator/solid electrolyte for lithium and sodium metal anode batteries to improve resistance to dendrite penetration. The separator/electrolyte is made by reinforcing the brittle glassy electrolyte with fibers like silica glass, mica, or clay. The fibers are dispersed throughout the electrolyte during processing to create a composite separator/electrolyte. The fibers prevent crack propagation and fracture when loaded, preventing dendrite growth. The fiber concentration is optimized to enhance toughness without significantly reducing ionic conductivity.

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Low-cost, sulfide-impregnated solid-state batteries that do not require tightly controlled moisture environments during manufacturing. The method involves making a solid-state battery core using conventional lithium-ion battery components, then impregnating it with a sulfide-based solid-state electrolyte precursor solution. The solvent is evaporated to solidify the electrolyte inside the battery core. This in-situ solidification step avoids direct contact between the electrolyte precursor and moisture, allowing the battery to be made using conventional lithium-ion processes without strict moisture control. The densified electrolyte-impregnated core is then sealed to complete the solid-state battery.

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