Structure including solid electrolyte materials and organic materials and method of forming

Abstract

The structure may include particles comprising an electrolyte material attached to fibers comprising a polymer. The electrolyte material may include an inorganic material. In one embodiment, the structure may include a fiber concentration of 0.15 / μm2 or higher.

Description

Technology Field

[0001] The following relates to a structure comprising a solid electrolyte material and an organic material and a method for forming the same, and in particular, to a structure comprising a solid electrolyte material and a fiber comprising a polymer and a method for forming the same. Background Technology

[0002] The electrolyte layer for all-solid-state Li batteries (ASSLB) can be formed via a tape-casting method. Solvents are typically used as carriers for the electrolyte material and binder in the system. Since the solvent must be removed by drying, this process can increase manufacturing costs and environmental impact. The industry continues to demand improved electrolytes and all-solid-state batteries. Brief explanation of the drawing

[0003] By referring to the attached drawings, those skilled in the art can better understand the present disclosure and clearly recognize numerous features and advantages. FIG. 1 includes an SEM image illustrating a part of a structure according to one embodiment. FIG. 2 includes an SEM image illustrating a part of a structure according to another embodiment. FIGS. 3a to 3c include SEM images illustrating a part of a structure according to another embodiment. Figure 4 includes XRD patterns of Li3YBr6 and decomposed Li3YBr6. FIG. 5 includes a cross-sectional view of a structure comprising a plurality of layers according to one embodiment. FIG. 6 includes a flowchart illustrating a method for forming a structure according to one embodiment. FIGS. 7a to 7d include SEM images showing the microstructures of different samples. Figure 8 includes a diagram showing the fiber concentrations of different samples. Those skilled in the art understand that elements in the drawings are depicted for simplicity and clarity and are not necessarily drawn to scale. For example, the dimensions of some elements in the drawings may be exaggerated relative to others to help improve understanding of embodiments of the invention. The use of the same reference numerals in different drawings indicates similar or identical items. Specific details for implementing the invention

[0004] The following description, in combination with the drawings, is provided to aid in understanding the teachings disclosed herein. The following discussion will focus on specific implementations and embodiments of the teachings. This focus is provided to aid in explaining the teachings and should not be construed as a limitation on the scope or availability of the teachings.

[0005] As used herein, the terms “comprising,” “comprising,” “having,” “having,” “having,” “having,” or any other variation thereof are intended to include non-exclusive inclusions. For example, a process, method, article, or apparatus comprising a list of features is not necessarily limited to such features but may include other features not explicitly listed or not unique to such process, method, article, or apparatus. Also, unless explicitly stated otherwise, “or” refers to inclusive or rather than exclusive or. For example, condition A or B is satisfied by any one of the following: A is true (or exists) and B is false (or does not exist); A is false (or does not exist) and B is true (or exists); and A and B are both true (or exist).

[0006] The use of the singular (“a” or “an”) is intended to describe the elements and components described herein. This is done merely for convenience and to provide a general meaning of the scope of the invention. Such descriptions should be interpreted as including one or at least one, unless it is evident that they are meant otherwise, and the singular form includes the plural, and vice versa.

[0007] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by those skilled in the art to which the present invention pertains. Materials, methods, and examples are merely illustrative and not intended to be limiting.

[0008] Embodiments of the present invention relate to a structure that may comprise a solid electrolyte material and an organic material. In certain embodiments, the structure may comprise particles comprising a solid electrolyte material and particles attached to fibers comprising an organic material, such as a polymer. In more specific embodiments, the structure may comprise a specific fiber density, fiber aspect ratio, solid electrolyte content, average particle size, particle size distribution, or any combination thereof. The structure may have improved properties, such as improved ionic conductivity, mechanical strength, electrochemical stability, or any combination thereof.

[0009] The embodiments relate to a process for forming a structure. In particular, the process may include a dry process. For example, a solvent may not be used in the process. In certain embodiments, one or more parameters of the process may be carefully controlled to form a structure having an improved microstructure, solid loading amount, uniformity, properties, or any combination thereof.

[0010] In one embodiment, the structure may comprise a solid electrolyte material comprising an organic material and an inorganic material, wherein the organic material may comprise a polymer in the form of fibers. In another embodiment, the structure may comprise fibers comprising a polymer and a solid electrolyte material directly attached to the fibers, wherein the solid electrolyte material may be in the form of particles. In one example, the particles comprising the solid electrolyte material may comprise various shapes and / or forms such as coarse particles, aggregates, granules, pellets, sheets, plates, rods, solid masses of other shapes, or any combination thereof. In a specific embodiment, the structure may comprise particles of the electrolyte material attached to fibers comprising a polymer. In a specific example, the fibers may essentially consist of one or more polymers. In another embodiment, the structure may comprise a network comprising particles of the electrolyte material and fibers extending in three dimensions. For example, the fibers may extend through at least a portion of the volume of the structure. In another example, the fibers may be attached to each other, to one or more particles, or to any combination thereof. In a specific example, the fiber can form a three-dimensional fiber structure. In another specific example, particles containing an electrolyte material can be uniformly dispersed within the three-dimensional fiber structure.

[0011] FIG. 1 includes a scanning electron microscope image of a cross-section of a structure (100) according to one embodiment. The structure (100) comprises particles (104) containing an electrolyte material and fibers (106). One or more fibers (106) may be attached to the particles (104) and / or other fibers (106). In one embodiment, the fibers (106) may be made of an organic material. In a specific embodiment, the fibers (106) may be made of one or more polymers.

[0012] As illustrated, the fiber (106) may have a random orientation. For example, the fiber (106) may include fibers extending in intersecting directions, substantially parallel directions, or any combination thereof.

[0013] In one embodiment, the organic material may include a specific melt flow rate (also referred to as "MFR") that can promote the formation of a structure and / or the improvement of properties. For example, the structure may include a polymer having a specific melt flow rate that can promote the formation of a structure and / or the improvement of properties. In the present invention, the melt flow rate of the organic material may be measured at 150°C to 200°C according to ASTM D1238, procedure A. In one example, the organic material may include a material having a melt flow rate greater than 10 g / 10 min or greater than 12 g / 10 min, e.g., 13 g / 10 min or more, 14 g / 10 min or more, 15 g / 10 min or more, 17 g / 10 min or more, 20 g / 10 min or more, 22 g / 10 min or more, 25 g / 10 min or more, 27 g / 10 min or more, 30 g / 10 min or more, 33 g / 10 min or more, 35 g / 10 min or more, 38 g / 10 min or more, or 40 g / 10 min or more. In a specific example, the organic material may include a material having a melt flow rate greater than 40 g / 10 min, e.g., 55 g / 10 min or more, 70 g / 10 min or more, 85 g / 10 min or more, 90 g / 10 min or more, or greater than 90 g / 10 min. In other examples, the organic material may include a material having a melt flow rate of 200 g / 10 min or less, 180 g / 10 min or less, 150 g / 10 min or less, 130 g / 10 min or less, 120 g / 10 min or less, 110 g / 10 min or less, 100 g / 10 min or less, 90 g / 10 min or less, 80 g / 10 min or less, 70 g / 10 min or less, 60 g / 10 min or less, 55 g / 10 min or less, or 50 g / 10 min or less. Furthermore, the organic material may include a material having a melt flow rate in a range including the minimum and maximum values ​​mentioned herein.For example, the organic material may include a material having an MFR in a range including greater than 10 g / 10 min and less than or equal to 200 g / 10 min, or greater than or equal to 25 g / 10 min and less than or equal to 200 g / 10 min, or greater than or equal to 55 g / 10 min and less than or equal to 200 g / 10 min, or greater than or equal to 90 g / 10 min and less than or equal to 200 g / 10 min. In a specific embodiment, the fiber may include a polymer having a melt flow rate in a range including any minimum and maximum values ​​mentioned herein. In one embodiment, the structure and / or fiber may include a blend of organic materials, and the blend may have any of the MFRs mentioned in the embodiments of this specification. For example, the blend may contain an MFR greater than 10 g / 10 min, greater than 20 g / 10 min, greater than 30 g / 10 min, greater than 40 g / 10 min, greater than 55 g / 10 min, greater than 70 g / 10 min, greater than 85 g / 10 min, greater than 90 g / 10 min, or greater than 90 g / 10 min. In other examples, the blend may contain an MFR less than or equal to 200 g / 10 min, less than or equal to 180 g / 10 min, less than or equal to 150 g / 10 min, less than or equal to 130 g / 10 min, less than or equal to 120 g / 10 min, or less than or equal to 110 g / 10 min. Furthermore, the blend may contain an MFR within a range that includes any minimum and maximum values ​​mentioned herein. For example, the blend may have an MFR in the range including greater than 10 g / 10 min and less than or equal to 200 g / 10 min, or greater than or equal to 50 g / 10 min and less than or equal to 200 g / 10 min, or greater than or equal to 90 g / 10 min and less than or equal to 200 g / 10 min. The MFR of the blend of organic materials may be measured in the same manner as described above. The blend may be prepared by mixing the organic materials in equal weight percent relative to the total weight of the blend. For example, a blend of two organic materials may have a weight ratio of 50:50 between them.After reading the present disclosure, those skilled in the art understand that MFR may affect the formation and / or properties of the structures of the embodiments of this specification. For example, MFR may affect the solid loading amount, strength, or a combination thereof of the structures. For example, an MFR that is too high may have adverse effects, such as resulting in a structure having insufficient strength to maintain a proper shape during the molding process. In another example, an MFR that is too low may have an adverse effect on the solid loading amount. For example, if the MFR is too low, the solid loading amount may be too low.

[0014] In one embodiment, the structure may include an organic material that may be more lipophilic / hydrophobic than hydrophilic / hydrophobic. In one example, the organic material is formula HLB = 20×M h / M(here, M h It may have a predetermined hydrophilic-lipophilic balance determined according to Griffin's mathematical method using (where is the molecular weight of the hydrophilic portion of the organic material and M is the molecular weight of the entire organic material). For illustrative purposes, using an exemplary HLB scale from 0 to 20, an HLB value of 0 may correspond to a molecule that is completely lipophilic / hydrophobic, and a value of 20 may correspond to a molecule that is completely hydrophilic / lipophilic. In certain embodiments, the structure may comprise an organic material that may have an HLB value of 10 or less, 5 or less, 4 or less, 3 or less, 2 or less, 1 or less, or 0.5 or less. In more specific embodiments, the organic material may be lipophilic / hydrophobic, such as having an HLB value of 0.

[0015] In further embodiments, the organic material may have limited reactivity to the solid electrolyte material during the process of forming the structure. In further embodiments, the reactivity of the organic material may be tested and quantified using X-ray diffraction analysis as follows. The organic material and the solid electrolyte material may be mixed for 1 to 3 minutes in a weight percentage ratio of organic material to solid electrolyte material of 50:50. The mixture may be stored in a Kapton tube at a temperature for forming the structure, e.g., 150°C to 200°C, under an inert atmosphere for at least 12 hours and no more than 2 to 4 days prior to further analysis. Subsequently, the mixture may be sealed in an airtight sample holder having a Kapton film window to perform X-ray diffraction (XRD) analysis at 2 theta of 25 to 80°C with a step size of 7.5°C and a step duration of 120 seconds. The entire test may be performed in a dry environment with an H2O content of less than 1 ppm. Changes in the XRD pattern of the solid electrolyte material can be evaluated by comparing the XRD pattern of the mixture with the XRD of the solid electrolyte material. After reading the present disclosure, those skilled in the art understand that degradation or decomposition of the solid electrolyte material may cause changes in the XRD pattern of the solid electrolyte material. Changes may include the disappearance of one or more characteristic peaks of the solid electrolyte material, a change in the intensity of one or more characteristic peaks of the solid electrolyte material, the appearance of new peaks, the disappearance of other peaks, or any combination thereof.

[0016] In one embodiment, the organic material may have a specific reactivity value that can promote the formation of a structure and the improvement of properties. For example, the organic material may have a reactivity value of 20% or less or less than 20%, e.g., 18% or less, 15% or less, 12% or less, or 10% or less. In a specific example, the organic material may have a reactivity value of less than 10%, e.g., 9% or less, 8% or less, 7% or less, 6% or less, 5% or less, 4% or less, 3% or less, or 2% or less. In another example, the organic material may have a reactivity value of 0% or more than 0%, e.g., 0.01% or more, 0.1% or more, 0.2% or more, 0.3% or more, 0.5% or more, 0.8% or more, or 1% or more. Furthermore, the reactivity value may be within a range including any minimum and maximum percentages mentioned herein. For example, organic materials can have a reactivity value of 2% or less.

[0017] The reactivity value of the organic material can be determined based on the XRD pattern of the mixture using the formula RV=[B / A]×100%, where A represents the intensity of a characteristic peak of the solid electrolyte material and B represents the intensity of a characteristic peak of a representative decomposition product of the solid electrolyte material. The representative decomposition product may include a binary compound containing the major anionic and cation atoms of the solid electrolyte material. For example, the solid electrolyte material may include a halide material, and lithium halide may be a representative decomposition product of the halide material. Thus, A may be a characteristic peak of the halide material, and B may be a characteristic peak of lithium halide. Referring to FIG. 4, the XRD pattern of Li3YBr6 typically includes a characteristic peak A appearing between 31 and 32.2, and 2 theta. The XRD pattern of the decomposed Li3YBr6 includes peak B, a characteristic peak of the decomposition product LiBr, which typically appears at 27.9 to 28.5 degrees 2 theta. If the XRD pattern of the mixture does not include the characteristic peak of the decomposition product but contains peak A, a characteristic peak of the solid electrolyte material (i.e., A is not zero), the reactivity value of the organic material may be zero. If the XRD pattern of the mixture does not include the characteristic peak of the solid electrolyte material, the reactivity value of the organic material may not be defined.

[0018] In one embodiment, the organic material may comprise a specific binder material, a coupling agent, a plasticizer, or a combination thereof. In further embodiments, any of the binder material, the coupling agent, the plasticizer, or any combination thereof may have the MFR, HLB values, and / or reactivity values ​​mentioned in the embodiments of this specification.

[0019] In one embodiment, the structure may comprise a specific total content of organic material capable of promoting improved properties of the structure. In exemplary cases, the total content of the organic material may be 55 volume% or less with respect to the total volume of the structure, for example, 50 volume% or less or less than 50 volume% with respect to the total volume of the structure. In specific examples, the structure may comprise 45 volume% or less with respect to the total volume of the structure, for example, 40 volume% or less, 35 volume% or less, 30 volume% or less, 28 volume% or less, or 25 volume% or less with respect to the total volume of the structure. In another example, the total content of the organic material may be 5 volume% or more with respect to the total volume of the structure, for example, 8 volume% or more, 10 volume% or more, 12 volume% or more, 15 volume% or more, 18 volume% or more, 20 volume% or more, 25 volume% or more, 30 volume% or more, 35 volume% or more, 38 volume% or more, 40 volume% or more, 45 volume% or more, or 49 volume% or more with respect to the total volume of the structure. Furthermore, the structure may contain a total content of organic material within a range including any minimum and maximum percentages mentioned herein.

[0020] In one embodiment, the organic material may comprise a specific binder material capable of promoting the formation of a structure and / or the improvement of properties. In one example, the binder material may comprise a thermoplastic material, a thermosetting material, or a combination thereof. In another example, the binder material may comprise one or more thermoplastic polymers. A specific exemplary binder material may comprise one or more of high-density polyethylene (HDPE), polypropylene (PP), low-density polyethylene (LDPE), ethylene tetrafluoroethylene, ethylene chlorotrifluoroethylene, or any combination thereof. In a further embodiment, the organic material may comprise a coupling agent, a plasticizer, or a combination thereof. In a specific embodiment, the coupling agent may comprise a wax, a derivative thereof, or any combination thereof. An exemplary wax may comprise an animal wax, a vegetable wax, a petroleum wax, a derivative thereof, or any combination thereof. In another embodiment, the organic material may not contain a solvent. In another embodiment, the organic material may not contain an elastomer.

[0021] In one embodiment, the structure may comprise one or more polymers comprising high-density polyethylene (HDPE), polypropylene (PP), low-density polyethylene (LDPE), or any combination thereof. In a further embodiment, the structure may comprise a wax comprising animal wax, vegetable wax, petroleum wax, derivatives thereof, or any combination thereof. In another embodiment, the structure may not contain a solvent.

[0022] In certain embodiments, the structure may comprise one or more of high-density polyethylene (HDPE), polypropylene (PP), low-density polyethylene (LDPE), ozokerite wax, paraffin wax, or any combination thereof. In other embodiments, the structure may not contain an elastomer.

[0023] In one embodiment, the fiber may comprise one or more polymers. In another embodiment, the fiber may comprise a polymer having a specific melt flow rate that can promote the formation of a structure and / or the improvement of properties. In a specific example, the MFR of the polymer may be related to the temperature at which the structure is formed. In another example, the melt flow rate may be greater than 10 g / 10 min at 150°C to 200°C, e.g., greater than 15 g / 10 min, greater than 20 g / 10 min, greater than 25 g / 10 min, greater than 30 g / 10 min, or greater than 40 g / 10 min. In another example, the melt flow rate may be 200 g / 10 min or less, 180 g / 10 min or less, 150 g / 10 min or less, 130 g / 10 min or less, 120 g / 10 min or less, 100 g / 10 min or less, 90 g / 10 min or less, 80 g / 10 min or less, 70 g / 10 min or less, 55 g / 10 min or less, or 50 g / 10 min or less at 150°C to 180°C. Furthermore, the fiber may comprise a polymer having a melt flow rate in a range including the minimum and maximum values ​​mentioned herein.

[0024] In other embodiments, the fiber may comprise a polymer having a specific melting temperature that can promote the formation of a structure and / or improvement of properties. In one example, the melting temperature may be less than 300°C, e.g., 280°C or less, 260°C or less, 240°C or less, 220°C or less, 205°C or less, 200°C or less, 190°C or less, 180°C or less, 170°C or less, 160°C or less, 150°C or less, 140°C or less, or 130°C or less. In other examples, the melting temperature may be greater than 100°C, greater than 105°C, greater than 110°C, greater than 115°C, greater than 120°C, greater than 125°C, greater than 130°C, or greater than 135°C. Furthermore, the fiber may comprise a polymer having a melting temperature in a range including the minimum and maximum values ​​mentioned herein.

[0025] In another embodiment, the fiber may comprise a polymer having a specific elongation at break that can promote the formation of a structure and / or improvement of properties. In one example, the polymer may have a machine direction elongation at break of 5% or more, 10% or more, 30% or more, 50% or more, 70% or more, 100% or more, 200% or more, 350% or more, 400% or more, 500% or more, 600% or more, 700% or more, 800% or more, or 900% or more. In another example, the polymer may have a machine direction elongation at break of 1000% or less, e.g., 900% or less, 800% or less, 700% or less, 600% or less, 500% or less, 400% or less, 300% or less, 200% or less, 100% or less, or 55% or less. Furthermore, the fiber may comprise a polymer having a mechanical direction elongation at break within a range including the minimum and maximum values ​​mentioned in this specification.

[0026] In additional examples, the fiber may comprise a polymer having a transverse elongation at break of 5% or more, 10% or more, 30% or more, 50% or more, 70% or more, 100% or more, 200% or more, 350% or more, 400% or more, 500% or more, 600% or more, 650% or more, 700% or more, 800% or more, or 900% or more. In other examples, the polymer may have a transverse elongation at break of 1000% or less, e.g., 900% or less, 800% or less, 700% or less, 600% or less, 500% or less, 400% or less, 300% or less, 200% or less, 100% or less, or 55% or less. Furthermore, the fiber may include a polymer having a transverse elongation at break within a range including the minimum and maximum values ​​mentioned in this specification.

[0027] In additional embodiments, the fiber may comprise most of the total content of the organic material, for example, 55 volume% or more, 60 volume% or more, 70 volume% or more, 80 volume% or more, 90 volume% or more, or 95 volume% or more of the total content of the organic material. Additionally or alternatively, the fiber may comprise 99 volume% or less of the total content of the organic material, for example, 97 volume% or less, 95 volume% or less, 92 volume% or less, 90 volume% or less, 86 volume% or less, 84 volume% or less, 82 volume% or less, 80 volume% or less, 75 volume% or less, 73 volume% or less, 70 volume% or less, 65 volume% or less, 63 volume% or less, 60 volume% or less, or 58 volume% or less. In certain embodiments, the fiber may comprise essentially all of the total content of the organic material. Furthermore, the fiber may contain an organic material in an amount including any minimum and maximum percentages mentioned in this specification.

[0028] In other embodiments, the fiber may comprise a polymer, and the polymer may be included in a specific amount that can promote the formation of the structure and / or improvement of properties. In one example, the polymer may be in an amount of 55 volume% or less, 50 volume% or less, or even less than 50 volume% with respect to the total volume of the structure. In a specific example, the polymer may be 45 volume% or less with respect to the total volume of the structure, e.g., 40 volume% or less, 35 volume% or less, 30 volume% or less, 28 volume% or less, or 25 volume% or less with respect to the total volume of the structure. In other examples, the polymer content may be 5 volume% or more with respect to the total volume of the structure, for example, 8 volume% or more, 10 volume% or more, 12 volume% or more, 15 volume% or more, 18 volume% or more, 20 volume% or more, 25 volume% or more, 30 volume% or more, 35 volume% or more, 38 volume% or more, 40 volume% or more, 45 volume% or more, or 49 volume% or more with respect to the total volume of the structure. Furthermore, the fiber may contain a polymer, and the polymer may be in an amount including any minimum and maximum percentages mentioned herein.

[0029] In other embodiments, the fiber may comprise high-density polyethylene (HDPE), polypropylene (PP), low-density polyethylene (LDPE), or any combination thereof. In further embodiments, the fiber may comprise a wax comprising animal wax, vegetable wax, petroleum wax, derivatives thereof, or any combination thereof. In certain embodiments, the fiber may comprise an organic material essentially composed of high-density polyethylene (HDPE), a wax, for example, ozokerite wax and / or paraffin wax, or any combination thereof. For example, the fiber may comprise an organic material essentially composed of high-density polyethylene (HDPE) and a wax. In other more specific embodiments, the fiber may comprise an organic material essentially composed of polypropylene (PP), high-density polyethylene (HDPE), low-density polyethylene (LDPE), a wax, or any combination thereof. For example, the fiber may comprise an organic material essentially composed of a wax and one or more of polypropylene (PP), high-density polyethylene (HDPE), and low-density polyethylene (LDPE). In certain embodiments, the fiber may not contain an elastomer.

[0030] In other embodiments, the structure may comprise a specific amount of solid electrolyte material and / or organic material capable of promoting improvement of the properties of the structure. In one embodiment, the structure may comprise a specific weight% or volume% content of solid electrolyte material or organic material, respectively, with respect to the weight or volume of the structure. The content (weight%) may be determined using inductively coupled plasma (ICP) and elemental analysis to analyze a sample of the structure acidified using nitric acid. Those skilled in the art understand that the volume% content can be calculated based on the weight% and density of the components of the structure. In other embodiments, the structure may comprise a specific amount of solid electrolyte material. In one example, the content of the solid electrolyte material may be 55 weight% or more with respect to the total volume of the structure, for example, 60 weight% or more, 63 weight% or more, 68 weight% or more, 50 weight% or more, 72 weight% or more, 75 weight% or more, or 78 weight% or more with respect to the total volume of the structure. In other cases, the structure may comprise a solid electrolyte material of 95 volume% or less with respect to the total volume of the structure, for example, 93 volume% or less, 91 volume% or less, 89 volume% or less, 86 volume% or less, 83 volume% or less, 80 volume% or less, 76 volume% or less, 73 volume% or less, 70 volume% or less, 67 volume% or less, 65 volume% or less, 62 volume% or less, 60 volume% or less, 58 volume% or less, 55 volume% or less, 53 volume% or less, or 51 volume% or less with respect to the total volume of the structure. Furthermore, the content of the solid electrolyte material may be within a range including any minimum and maximum percentages mentioned herein.

[0031] In one embodiment, the structure may include a specific amount of particles comprising an electrolyte material capable of promoting improvement of the properties of the structure. In one example, the content of the particles may be 55 wt% or more with respect to the total volume of the structure, for example, 60 wt% or more, 63 wt% or more, 68 wt% or more, 50 wt% or more, 72 wt% or more, 75 wt% or more, or 78 wt% or more with respect to the total volume of the structure. In additional examples, the particle content may be 95 weight% or less with respect to the total volume of the structure, for example, 93 volume% or less, 91 volume% or less, 89 volume% or less, 86 volume% or less, 83 volume% or less, 80 volume% or less, 76 volume% or less, 73 volume% or less, 70 volume% or less, 67 volume% or less, 65 volume% or less, 62 volume% or less, 60 volume% or less, 58 volume% or less, 55 volume% or less, 53 volume% or less, or 51 volume% or less with respect to the total volume of the structure. Furthermore, the particle content may be within a range including any minimum and maximum percentages mentioned herein.

[0032] In one embodiment, most of the particles (i.e., more than 50%) may be in contact with one another, for example, more than 55%, more than 60%, more than 70%, more than 80%, more than 90%, or more than 95% of the particles may be in contact with one another. The particles in contact may be quantified by examining different SEM images of one or more cross-sections of the sample. The number of images indicates statistical significance. As used herein, the percentage of particles in contact with one another may be based on the total number or content (volume%) of particles calculated based on the SEM images.

[0033] FIG. 2 includes an SEM image of a cross-section of an exemplary structure (200) comprising fibers (204) that may be taut and fibers (202) that may not be taut. As demonstrated, the fibers (202) may be loose, curly, and / or wavy. FIG. 3a includes an SEM image of a cross-section of an exemplary structure (300) comprising taut fibers (302) and non-taut fibers (304).

[0034] In other embodiments, the fiber may include a length, a width, and an aspect ratio of width to length. In certain embodiments, a single taut fiber (e.g., fiber (202) in FIG. 2 and fiber (302) in FIG. 3a) may have a predetermined length. As disclosed herein, a single fiber may start or end at another fiber or particle. This length may be a linear distance between opposite ends of the fiber. As illustrated in FIG. 3a and FIG. 3b, the fiber (302) may be attached to fiber (306) and fiber (308), and thus may start at one of fiber (306) and (308) and end at the other. The length (3022) of the fiber (302) may extend between the point (306) where the fiber (302) contacts and the point (308) where the fiber (302) contacts. As illustrated in FIGS. 3a through 3c, the fiber (302) may include a width that varies along the length (3022) and may include a maximum width (3026). It should be understood that the structure of an embodiment of this specification may include a fiber having a substantially constant width, and that the width of such fiber may be the maximum width. The fiber (302) may further include an aspect ratio (APmw / l) of the maximum width (3026) to the length (3022). As used herein, the aspect ratio of the maximum width to the length is intended for a taut fiber.

[0035] In another embodiment, the structure (e.g., the structure (100, 200, 300) of FIGS. 1 to 3a) may include fibers having a specific aspect ratio (APmw / l) of maximum width to length that can promote improvement of the characteristics of the structure. For example, the structure may include fibers having an aspect ratio (APmw / l) of maximum width to length of 0.2 or less. In additional examples, the structure may include fibers having an aspect ratio (APmw / l) of 0.0001 or more, 0.001 or more, 0.002 or more, 0.003 or more, 0.004 or more, 0.005 or more, 0.006 or more, 0.007 or more, 0.008 or more, 0.009 or more, 0.01 or more, 0.02 or more, 0.03 or more, 0.04 or more, or 0.05 or more. Furthermore, the structure may include fibers having an aspect ratio (APmw / l) in a range including any minimum and maximum values ​​mentioned in this specification.

[0036] In certain embodiments, most of the fibers (i.e., more than 50%) may have a maximum width-to-length aspect ratio (APmw / l) of 0.2 or less, and, for example, more than 60%, more than 70%, more than 80%, or more than 90% of the fibers may have a maximum width-to-length aspect ratio of 0.2 or less. Furthermore, the content of fibers having an aspect ratio (APmw / l) of 0.2 or less may be within a range including any minimum and maximum percentages mentioned herein. In certain examples, essentially all fibers may have a maximum width-to-length aspect ratio (APmw / l) of 0.2 or less. As used herein, the percentage of fibers may be based on the total number of fibers or the total content (volume%) of organic material that can be analyzed for the aspect ratio (APmw / l).

[0037] In further embodiments, the structure may include a specific fiber concentration capable of promoting the formation of the structure and / or improvement of its properties. For example, the structure may be 0.15 / μm 2The fiber concentration may include the above. In another example, the fiber concentration may not be too high to hinder contact between particles containing solid electrolyte material, which could adversely affect the properties of the structure.

[0038] In certain embodiments, the structure may comprise fibers having an aspect ratio (APmw / l) of 0.2 or less at a specific fiber concentration capable of promoting the formation and / or improvement of properties of the structure. For example, the fiber concentration of fibers having an aspect ratio (APmw / l) of 0.2 or less is 0.15 / μm 2 Above, 0.18 / μm 2 Above, 0.20 / μm 2 Above, 0.22 / μm 2 Above, 0.25 / μm 2 Above, 0.30 / μm 2 Above, 0.33 / μm 2 Above, 0.35 / μm 2 Above, 0.38 / μm 2 Above, 0.40 / μm 2 Above, 0.45 / μm 2 Above, 0.50 / μm 2 Above, 0.55 / μm 2 Above, 0.60 / μm 2 Above, 0.62 / μm 2 Above, 0.65 / μm 2 Above, 0.70 / μm 2 Above, 0.73 / μm 2 Above, 0.75 / μm 2 Above, 0.78 / μm 2 Above, 0.80 / μm 2 Above, or 0.82 / μm 2 It may be more than that. In another example, the fiber concentration of a fiber having an aspect ratio (APmw / l) of 0.2 or less is 150 / μm 2 Below, for example, 130 / μm 2 Below, 110 / μm 2 Below, 85 / μm 2 ≤ 60 / μm 2 Less than 40 / μm 2 Less than 20 / μm2 Less than 10 / μm 2 Below, 7.5 / μm 2 Below, 4.6 / μm 2 Below, 2.2 / μm 2 Below, 1.3 / μm 2 Less than or equal to 0.9 / μm 2 It may be less than or equal to. In another example, the fiber concentration of a fiber having an aspect ratio (APmw / l) of 0.2 or less may be within a range including any minimum and maximum values ​​mentioned in this specification.

[0039] As described herein, the fiber concentration can be determined as follows. A sample of the structure can be broken by hand to expose the cross-section. Scanning electron microscope images with a width of 25 μm are acquired at random locations along the entire thickness of the cross-section of the structure. 10 μm 2 to 180 μm 2 A 2D rectangular region is randomly selected across the entire SEM image. Regions containing particles larger than 5 μm, regions with voids larger than 5 μm (cavities where particles may have detached), and regions that may be out of focus should be excluded from the analysis. The number of clearly distinguishable taut fibers with an aspect ratio (maximum width / length) of 0.2 or less can be counted. Fibers that start in the designated region but end outside the region may be included. It should be understood that a single fiber may start and end in another fiber or particle. Fiber concentration may be the number of fibers counted across the entire 2D region being analyzed.

[0040] In one embodiment, the particle (e.g., particle (104) of FIG. 1) may comprise a solid electrolyte material comprising a halide-based material, a sulfide-based material, an oxyhalide, a halide hydroxide, an oxide, or any combination thereof. In another embodiment, the particle may comprise a hygroscopic solid electrolyte material.

[0041] In one embodiment, the halide material is formula M 3-δ (Me k+ ) f X 3-δ+k*f (In the above formula, -3≤δ<3, 0≤f≤1, k is the valence of Me, 2≤k<6, M may be one or more alkali metals including Li, Me may include a metal element different from M, and X may include a halogen), and the halide material may include at least two metal elements. Specific examples of Me may include rare earth elements, Y, In, Sn, Fe, Bi, Zr, Ti, Hf, Sb, alkaline earth metal elements, or any combination thereof. In other specific examples, X may include at least two halides including Cl, F, Br, I, or any combination thereof.

[0042] Exemplary sulfide-based materials may include an amorphous phase, a crystalline phase, or any combination thereof. Specific examples of sulfide-based materials include xLi2S-yP2S5 (LPS), e.g., 0.67Li2S-0.33P2S5, 80Li2S-20P2S5, 75Li2S-25P2S5, 70Li2S-30P2S5, etc., Li2S-X (where X represents at least one sulfide of SiS2, GeS2, and B2S3), e.g., 0.50Li2S-0.50GeS2, LiI-Li2S-SiS2, e.g., 0.40LiI-0.36Li2S-0.24SiS2, etc., 0.05Li4SiO4-0.57Li2S-0.38SiS2, Li3PO4-Li2S-SiS2, e.g., 0.01Li3PO4-0.63Li2S-0.36SiS2, etc. LiI-Li2S-B2S3, e.g., 0.44LiI-0.30Li2S-0.26B2S3, etc., LiI-Li2S-P2S5, e.g., 0.45LiI-0.37Li2S-0.18P2S5, etc., a-Li3PS4, LGPS(e.g., Li 10 GeP2S 12), LPSCl (e.g., Li6PS5Cl), LPSBr (e.g., Li6PS5Br), LSPSCl (e.g., Li 9.54 Si 1.74 P 1.44 S 11.7 Cl 0.3 ), Li 10.35 [Sn 0.27 Si 1.08 ]P 1.65 S 12 , or any combination thereof may be included, but is not limited thereto.

[0043] In additional examples, the solid electrolyte is a lithium oxyhalide, a lithium halide hydroxide, or any combination thereof, e.g., Li3OCl, Li3OBr, Li3O(Cl, Br), Li3OCl0.5Br0.5, Li2OHX, Li2OHCl, Li2OHBr, Li7O2(Br 3-x F x ), Li7O2(Br d Cl (1-d) )3, Li7O2(Br d F e Cl (1-d-e) It may include )3, Li4(OH)3X (where X is Cl, Br, and / or F), or a combination thereof.

[0044] Exemplary oxides include NASICON-type solid electrolytes represented by LiTi2(PO4)3 or their elemental substituents; (LaLi)TiO3-based perovskite solid electrolytes; Li 14 ZnGe4O 16 LISICON-type solid electrolytes represented by , Li4SiO4, and LiGeO4, or elemental substituents thereof; Li7La3Zr2O 12 It may include a garnet-type solid electrolyte or an elemental substituent thereof represented by; Li3N or its H substituent; or Li3PO4 or its N substituent.

[0045] In one embodiment, the structure may be in the form of a tape, sheet, block, film, disk, or any combination thereof. In one embodiment, the structure may be a standalone type, a single-layer structure, or both.

[0046] In one embodiment, the structure may be formed using a process comprising mixing, pressing, compounding, casting, molding, extrusion, shaping, cutting, or any combination thereof. In certain embodiments, this process may not involve the use of a solvent.

[0047] Referring to FIG. 6, a process for forming a structure is illustrated. The process (500) may begin in a block (502) comprising forming a mixture comprising an organic material and a solid electrolyte material. In one embodiment, the mixture may be a dry mixture. For example, the organic material may not contain liquid. In another embodiment, the solid electrolyte material may be mixed with the organic material at a specific weight content ratio that can facilitate formation and / or improvement of properties. The weight content may be based on the total weight of the solid electrolyte material and the organic material. For example, the weight ratio of solid electrolyte material to organic material may be 60:40 or greater, e.g. 65:35 or greater, 68:32 or greater, 70:30 or greater, 72:38 or greater, 75:25 or greater, 78:22 or greater, 80:20 or greater, 82:18 or greater, 84:16 or greater, 86:14 or greater, 88:12 or greater, or 90:10 or greater. In one example, the weight ratio of solid electrolyte material to organic material may be 96:4 or less, e.g. 94:6 or less, 92:8 or less, 90:10 or less, 88:12 or less, 86:14 or less, 84:16 or less, or 82:18 or less. Furthermore, the weight ratio of solid electrolyte material to organic material may be within a range including any minimum and maximum values ​​mentioned herein.

[0048] In additional embodiments, the organic material may comprise a binder material and one or more of a coupling agent, a plasticizer, or any combination thereof. The materials may be mixed using a mixing device to promote the formation of a homogeneous mixture.

[0049] In additional embodiments, mixing may include blending. For example, a material comprising a solid electrolyte and an organic material may be loaded into a blender to form a homogeneous mixture suitable for further processing to form a structure. In other embodiments, the solid electrolyte material and the organic material may be loaded separately into a blending device or an extruder and mixed.

[0050] In another embodiment, the process (500) may include a step of pretreating a solid electrolyte material and / or an organic material to have a specific particle size that can facilitate material mixing and / or structure formation and / or property improvement. In one example, the material may be cut, crushed, milled, ground, sieved, or otherwise processed by techniques known to those skilled in the art, or processed by any combination thereof. In a specific example, the solid electrolyte material may be mechanically milled, for example using a mortar and pestle, jet milled, or a combination thereof. In another example, pellets of a binder material, such as HDPE, may be ground and / or milled to have a specific particle size. In a specific example, cryogenic grinding may be used to form particles of the organic material having a specific particle size.

[0051] The process (500) continues to a block (504) that forms a structure from a mixture. In a specific embodiment, one or more parameters of the process (500) may be carefully controlled to form a structure from a dry mixture. In one embodiment, forming the structure may include blending, extrusion, or a combination thereof. In another embodiment, a suitable device may be used to perform the formation of the structure. In one example, the process (500) may include using an extruder or a device capable of having an equivalent function. An exemplary extruder may include a screw extruder, such as a single-screw extruder / blender, a twin-screw extruder, etc. In another specific embodiment, the extruder may include a die extruder.

[0052] In one embodiment, a suitable device may be used to perform the mixing of the mixture. For example, an extruder or a separate device having a mixing function may be used. In another embodiment, the process may include the step of dividing the mixture into batches and feeding them into the barrel of an extruder, wherein the barrel may include a mixing section. For example, the mixture may be divided into batches having similar weights of solid electrolytes and fed into the barrel one at a time. In another embodiment, the step of adding a second batch may be performed when at least a portion of the first batch can pass through the mixing section. In a specific embodiment, the barrel may include a plurality of mixing sections, and a second batch may be fed when at least a portion of the first batch can pass through the first mixing section.

[0053] In additional embodiments, adding a second batch or a subsequent batch may be performed at a specific torque. In certain embodiments, the next batch may be added after the torque has increased and then decreased again. After reading the present disclosure, those skilled in the art will understand that the torque may increase when a load is applied to the mixing section and may decrease when the load begins to move out of the mixing section. In certain exemplary applications, the torque may increase to a maximum torque (e.g., 15 Nm) when the batch is loaded, and may decrease (e.g., to 2 to 3 Nm) when the batch begins to move out of the mixing section and before the batch reaches the end of the barrel. After reading the present disclosure, those skilled in the art will understand that the maximum torque may vary depending on the solid loading amount (i.e., weight% or volume% of the solid electrolyte material) and that the maximum torque may be adjusted to suit various solid loading amounts. In one example, for a solid loading amount of 90 weight% or less, the torque may be as high as 15 Nm. In other specific embodiments, subsequent batches may be added at a torque in the range of 2 to 6 Nm. Those skilled in the art understand that various devices can be used to adjust the torque value so that the mixture can be divided into batches, properly loaded, and extruded.

[0054] In other embodiments, a subsequent batch may be added at a specific timing. In certain examples, the timing for adding the subsequent batch may be 0.6 to 2 minutes after adding the previous batch. In other specific examples, the subsequent batch may be added at 20 rpm or less. It should be noted that adding the material into the barrel at 20 rpm or less may improve the mixability of the organic material, facilitate the blending of the solid electrolyte material and the organic material, or promote a combination thereof. In certain exemplary applications, the subsequent batch may be added at 2 or more, 5 or more, 10 or more, or 15 or more rpm. After reading this disclosure, those skilled in the art understand that the screw may be operated at a low rpm to allow the new batch to be incorporated into the barrel, and that the rpm value may be adjusted for the use of different equipment. In other embodiments, the timing for adding the batch to the barrel may be controlled from seconds up to minutes.

[0055] In one embodiment, extrusion may be performed at 300 rpm or less, which may help reduce the formation of bubbles, edge defects, or both within the extruded product. Bubbles can be observed using SEM imaging. In one example, the screw rpm may be less than 300, e.g., 280 or less, 250 or less, 200 or less, 170 or less, 150 or less, 120 or less, 100 or less, 70 or less, 60 or less, 40 or less, 30 or less, 20 or less, or 10 or less. For mixtures having a higher solid loading amount (e.g., 85 wt% or more), rpm of 5 to 10 may be particularly helpful in preventing edge defects. For example, the screw rpm may be 1 or more, e.g. 10 or more, 20 or more, 30 or more, 50 or more, 70 or more, 90 or more, 100 or more, 110 or more, or 130 or more, which may help prevent deformation of the extruded product. Deformation may include bulging, warping, or other misshapes. Furthermore, the process (500) may include a screw rpm range including any minimum and maximum values ​​mentioned herein.

[0056] In another embodiment, the extruder may include a conveyor, wherein the belt speed may be controlled to facilitate the formation of the structure. In a further embodiment, the belt speed may be controlled to match the extrusion speed. In a specific embodiment, the belt speed may include any rpm mentioned for the screw rpm in the embodiments of this specification. In a further embodiment, the extruded structure may be shaped to form the finally formed structure. In one example, the structure may be shaped using a roller after extrusion, which includes compression, flattening, and making the tape more uniform.

[0057] In an additional embodiment, the process (500) may include the step of passing the extruded material through a barrel in the manner described in the embodiments of this specification, which may help improve the uniformity of the finally formed structure.

[0058] In further embodiments, compounding and / or extrusion may be performed at a temperature that may be above the melting temperature of the organic material. For example, the compounding and / or extrusion temperature may be above the melting temperature of the coupling agent and / or plasticizer, if present. In further examples, the compounding and / or extrusion temperature may be above the melting temperature of the binder material. In further embodiments, the compounding and / or extrusion temperature may be above the melting temperature of the binder material.

[0059] In certain embodiments, blending and / or extrusion may be performed at a specific temperature of 120°C or higher, e.g., 140°C or higher, 150°C or higher, 160°C or higher, or 180°C or higher. Alternatively or additionally, blending and / or extrusion may be performed at a temperature of less than 300°C, 280°C or lower, 280°C or lower, 250°C or lower, 230°C or lower, 210°C or lower, 200°C or lower, or less than 200°C. In certain examples, blending and / or extrusion may be performed at a temperature of 190°C or lower, 180°C or lower, 170°C or lower, 160°C or lower, or 150°C or lower. Furthermore, blending and / or extrusion may be performed at a temperature range including any minimum and maximum values ​​mentioned herein. In one example, the blending and / or extrusion temperature may be a range including 120°C or higher and 250°C or lower, e.g., a range including 130°C or higher and 210°C or lower, or a range including 140°C or higher and 170°C or lower, or a range including 160°C or higher and 200°C or lower. In other specific embodiments, blending and / or extrusion may be performed at a specific barrel temperature. In further embodiments, the barrel temperature may include any minimum and / or maximum blending and / or extrusion temperatures mentioned herein.

[0060] In a specific embodiment, the process (500) may be performed in a dry environment to promote the improvement of the formation of the structure. For example, a certain solid electrolyte material may be hygroscopic, and using a dry environment may help reduce the degradation of the material. In one example, the dry environment may contain an H2O content of less than 1 ppm. In another example, the process (500) may be performed inside a glove box.

[0061] In a specific embodiment, the process (500) may be a dry process and may be particularly suitable for forming a structure comprising a halide-based solid electrolyte material. Halide-based materials are more susceptible to moisture than sulfide-based materials or other hygroscopic electrolyte materials (e.g., hydroxyl halides) and are prone to decomposition due to moisture trapped in organic materials or the environment. In a specific example, the process (500) may include using a strictly controlled dry environment (i.e., H2O content is less than 0.01 ppm) which may help further prevent the decomposition of the halide-based material.

[0062] In one embodiment, the structure may include particles having a specific maximum particle size that can promote improvement of the performance and / or characteristics of the structure. In one example, the maximum particle size may be 0.5 μm or more, e.g., 1 μm or more, 2 μm or more, 3 μm or more, 5 μm or more, 8 μm or more, 10 μm or more, or 12 μm or more. In another example, the maximum particle size may be 20 μm or less, e.g., 18 μm or less, 15 μm or less, 13 μm or less, 11 μm or less, 8 μm or less, or 5 μm or less. Furthermore, the structure may include particles having a specific maximum particle size within a range including any minimum and maximum values ​​mentioned herein.

[0063] In one embodiment, the structure may include particles having a specific minimum particle size that can promote improvement of the performance and / or properties of the structure. For example, the structure may include particles having a minimum particle size of 100 nm or more, e.g. 200 nm or more, 300 nm or more, 400 nm or more, 500 nm or more, 600 nm or more, 700 nm or more, 800 nm or more, 900 nm or more, or 1 μm or more. In another example, the minimum particle size may be 5 μm or less, 4 μm or less, 3 μm or less, 2 μm or less, 1 μm or less, 800 nm or less, or 600 nm or less. Furthermore, the structure may include particles having a specific minimum particle size within a range including any minimum and maximum values ​​mentioned herein.

[0064] In one embodiment, the structure may include particles having a specific average particle size that can promote improvement of the performance and / or properties of the structure. In one embodiment, the average particle size may be 100 nm or more, e.g. 200 nm or more, 300 nm or more, 400 nm or more, 500 nm or more, 600 nm or more, 700 nm or more, 800 nm or more, 900 nm or more, or 1 μm or more. In another example, the average particle size may be 10 μm or less, 9 μm or less, 8 μm or less, 7 μm or less, 6 μm or less, 5 μm or less, 4 μm or less, 3 μm or less, 2 μm or less, or 1 μm or less. Furthermore, the particles may have an average particle size in a range including any minimum and maximum values ​​mentioned herein.

[0065] In one embodiment, the structure may comprise particles having a bimodal particle size distribution comprising fine particles and coarse particles having a specific particle size that can promote the formation of the structure and / or the improvement of performance and / or properties. In a further embodiment, the fine particles may have an average particle size of 2 μm or less, e.g. 1.5 μm or less, 1 μm or less, 800 nm or less, 600 nm or less, 500 nm or less, 400 nm or less, 300 nm or less, 200 nm or less, 100 nm or less, or 800 nm or less. Alternatively or additionally, the fine particles may have an average particle size of 100 nm or more, 200 nm or more, 300 nm or more, 400 nm or more, 500 nm or more, 600 nm or more, 700 nm or more, 800 nm or more, 900 nm or more, or 1 μm or more. Furthermore, the particle may have an average particle size in a range including any minimum and maximum values ​​mentioned in this specification.

[0066] In additional embodiments, the structure may comprise a specific amount of fine particles capable of promoting improvement of the performance and / or properties of the structure. In one example, the structure may comprise fine particles in an amount of 30% or less of the total amount of particles by volume, e.g., 25% or less, 20% or less, 15% or less, or 10% or less of the total amount of particles. In another example, the structure may comprise fine particles in an amount of 2% or more of the total amount of particles, e.g., 4% or more, 6% or more, 5% or more, 9% or more, 11% or more, 15% or more, 17% or more, or 20% or more of the total amount of particles. Furthermore, the content of fine particles may be within a range including any minimum and maximum percentages mentioned herein. The total amount of particles may be based on the total number of particles within the structure or the total volume percentage of the particles.

[0067] In other embodiments, the coarse particles may have an average particle size of 20 μm or less, 15 μm or less, 13 μm or less, 11 μm or less, 8 μm or less, or 5 μm or less. Alternatively or additionally, the coarse particles may have an average particle size of 400 nm or more, 500 nm or more, 600 nm or more, 700 nm or more, 800 nm or more, 900 nm or more, 1 μm or more, or 2 μm or more. Furthermore, the structure may comprise coarse particles having an average particle size within a range including any minimum and maximum values ​​mentioned herein.

[0068] In additional embodiments, the structure may comprise a specific amount of coarse particles that can promote improvement of the performance and / or properties of the structure. In one example, the structure may comprise coarse particles in an amount of 80% or less of the total amount of particles by volume, e.g., 70% or less, 60% or less, 50% or less, or 40% or less of the total amount of particles. In another example, the structure may comprise coarse particles in an amount of 20% or more of the total amount of particles, e.g., 30% or more, 35% or more, 40% or more, 45% or more, 50% or more, 60% or more, 85% or more, or 70% or more of the total amount of particles. Furthermore, the content of coarse particles may be within a range including any minimum and maximum percentages mentioned herein. The total amount of particles may be based on the total number of particles in the structure or the total volume percentage of the particles. In another embodiment, the structure may comprise 90% or less, 95% or less, or 98% or less of coarse particles based on volume with respect to the total amount of particles. In a specific embodiment, the structure may essentially consist of coarse particles.

[0069] In one embodiment, the structure may have a thickness t (shown in FIG. 4) of 0.1 μm or more, 1 μm or more, 5 μm or more, 6 μm or more, 7 μm or more, 8 μm or more, 9 μm or more, 10 μm or more, 12 μm or more, 14 μm or more, 17 μm or more, or 20 μm or more. Alternatively or additionally, the structure may have a thickness of 500 μm or less, 400 μm or less, 200 μm or less, 100 μm or less, 80 μm or less, 60 μm or less, 40 μm or less, 30 μm or less, 20 μm or less, 10 μm or less, or 8 μm or less. Furthermore, the thickness may be within a range including any minimum and maximum percentages mentioned herein.

[0070] In one embodiment, the structure may comprise a specific porosity, such as 20 volume% or less, 15 volume% or less, 10 volume% or less, 9 volume% or less, 8 volume% or less, 7 volume% or less, 6 volume% or less, 5 volume% or less, 4 volume% or less, 3 volume% or less, 2 volume% or less, or 1 volume% or less, based on the total volume of the structure. Alternatively or additionally, the structure may comprise a porosity of 0.05 volume% or more, 0.1 volume% or more, 0.5 volume% or more, or 1 volume% or more based on the total volume of the structure. Furthermore, the porosity may be within a range including any minimum and maximum percentages mentioned herein.

[0071] In one embodiment, the structure may have improved ionic conductivity. In another embodiment, the structure is 0.02 mS / cm or more, e.g. 0.03 mS / cm or more, 0.04 mS / cm or more, 0.05 mS / cm or more, 0.06 mS / cm or more, 0.07 mS / cm or more, 0.08 mS / cm or more, 0.09 mS / cm or more, or 0.10 mS / cm or more, 0.11 mS / cm or more, 0.12 mS / cm or more, 0.13 mS / cm or more, 0.14 mS / cm or more, 0.16 mS / cm or more, 0.20 mS / cm or more, 0.30 mS / cm or more, 0.40 mS / cm or more, 0.50 mS / cm or more, 0.60 mS / cm or more, 0.70 mS / cm or more, 0.80 mS / cm or more, 0.90 It can have an ionic conductivity of at least mS / cm, at least 1 mS / cm, at least 2 mS / cm, at least 3 mS / cm, at least 4 mS / cm, or at least 5 mS / cm. Additionally or alternatively, the structure may have an ionic conductivity of 10 mS / cm or less, 8 mS / cm or less, 6 mS / cm or less, 5 mS / cm or less, 4 mS / cm or less, 3 mS / cm or less, 2 mS / cm or less, 1.5 mS / cm or less, 1 mS / cm or less, 0.8 mS / cm or less, 0.7 mS / cm or less, 0.5 mS / cm or less, 0.4 mS / cm or less, 0.25 mS / cm or less, 0.22 mS / cm or less, 0.20 mS / cm or less, 0.19 mS / cm or less, 0.18 mS / cm or less, 0.17 mS / cm or less, 0.16 mS / cm or less, or 0.15 mS / cm or less. Furthermore, the structure may have an ionic conductivity in a range including any minimum and maximum values ​​mentioned herein. In the present disclosure, ionic conductivity can be measured at room temperature (i.e., 20 to 25°C) and activation energy in the range of 0.2 eV to 0.5 eV. In one embodiment, the structure may be an electrolyte, a separator, or both.In certain examples, the structure may be a solid-state electrolyte, a solid-state separator, or both.

[0072] In one embodiment, the electrochemical device may include such a structure. An exemplary electrochemical device may include a battery. Specific examples may include a solid-state battery, e.g., an all-solid-state lithium battery, an all-solid-state Li / Na battery, etc., or any combination thereof. For example, the electrochemical device may include a cathode, an anode, or both, wherein the structure may be in contact with either or both of the cathode and the anode. In a specific embodiment, the electrochemical device may include a structure adjacent to the anode. For example, the structure may be in direct contact with an anode which may include lithium, indium, aluminum, or any combination thereof. In further embodiments, the structure may serve as an electrolyte, a separator, or both.

[0073] Referring to FIG. 5, a multilayer structure (400) comprising a structure (406) between layers (402) and layers (404) is illustrated. In a particular example, the structure (406) may be an electrolyte or a separator comprising any feature described in embodiments of this specification. One of layers (402) or layers (404) may be an anode. In a particular example, the anode may comprise one or more metals including lithium, and more specifically, an electrolyte material, a polymeric fiber, or both may be in direct contact with the anode.

[0074] In other embodiments, the structure may comprise an electronically conductive material, such as comprising a conductive additive, an active electrode material, or a combination thereof. An exemplary electrode material may comprise an anode active material or a cathode active material. In one example, the anode active material may comprise lithium, indium, aluminum, or any combination thereof. In a specific example, the anode active material may comprise one or more metals including lithium. In another example, the cathode material may comprise a lithium-containing oxide, a transition metal fluoride, a polyanionic material, a fluorinated polyanionic material, a transition metal sulfide, a transition metal oxyfluoride, a transition metal oxysulfide, a transition metal oxynitride, or any combination thereof. Certain exemplary cathode materials include LiCoO2, LiFePO4, Li(NiCoAl)O2, LiCoO2, LiMnPO4, LiMn2O4, and LiNi 1 / 3 Co 1 / 3 Mn 1 / 3 O2, NMC622, NMC 811, other NMCs, etc., or any combination thereof may be included.

[0075] In one embodiment, the structure may have improved thickness variability, uniformity, or any combination thereof.

[0076] Many different aspects and embodiments are possible. Some of these aspects and embodiments are described herein. After reading this specification, those skilled in the art will understand that these aspects and embodiments are merely illustrative and do not limit the scope of the invention. Embodiments may follow any one or more of the embodiments listed below.

[0077] Implementation form

[0078] Embodiment 1. As a structure, it comprises particles of a solid electrolyte material attached to polymeric fibers, wherein the fiber concentration of the polymeric fibers is 0.15 / μm 2 Lee Sang-in, structure.

[0079] Embodiment 2. A structure comprising particles of a solid electrolyte material attached to a polymeric fiber, wherein the polymeric fiber comprises a polymer having a melt flow rate greater than 10 g / 10 min.

[0080] Embodiment 3. A structure comprising particles of a solid electrolyte material attached to a polymeric fiber, wherein the polymeric fiber comprises high-density polyethylene (HDPE), low-density polyethylene (LDPE), polypropylene (PP), or a combination thereof.

[0081] Embodiment 4. In any one of Embodiments 1 to 3, the aspect ratio of the maximum width to length is 0.2 or less and 0.15 / μm2 or more, 0.18 / μm2 or more, 0.20 / μm2 or more, 0.22 / μm2 or more, 0.25 / μm2 or more, 0.30 / μm2 or more, 0.33 / μm2 or more, 0.35 / μm2 or more, 0.38 / μm2 or more, 0.40 / μm2 or more, 0.45 / μm2 or more, 0.50 / μm2 or more, 0.55 / μm2 or more, 0.60 / μm2 or more, 0.62 / μm2 or more, 0.65 / μm2 or more, 0.70 / μm2 or more, 0.73 / μm2 or more, 0.75 / μm2 or more, A structure comprising polymeric fibers having a fiber concentration of 0.78 / μm2 or higher, 0.80 / μm2 or higher, or 0.82 / μm2 or higher.

[0082] Embodiment 5. In any one of Embodiments 1 to 4, the polymeric fiber comprises a polymer having a melt flow rate greater than 10 g / 10 min, 20 g / 10 min or more, 30 g / 10 min or more, or 40 g / 10 min or more; and the structure wherein the melt flow rate is 200 g / 10 min or less, 180 g / 10 min or less, 150 g / 10 min or less, 130 g / 10 min or less, 120 g / 10 min or less, 100 g / 10 min or less, 90 g / 10 min or less, 80 g / 10 min or less, 70 g / 10 min or less, 55 g / 10 min or less, or 50 g / 10 min or less.

[0083] Embodiment 6. In any one of Embodiments 1 to 5, the structure comprises a polymer having a melting temperature of less than 300 degrees and greater than 100 degrees.

[0084] Embodiment 7. In any one of Embodiments 1 to 6, the polymeric fiber comprises a polymer having a breaking elongation of 10 to 1000%.

[0085] Embodiment 8. A structure comprising, in any one of Embodiments 1 to 7, particles comprising 55 volume% or more of the total volume of the structure, 60 volume% or more, 63 volume% or more, 68 volume% or more, 50 volume% or more, 72 volume% or more, 75 volume% or more, or 78 volume% or more of the total volume of the structure, or 98 volume% or less, 95 volume% or less, 93 volume% or less, 91 volume% or less, 89 volume% or less, 86 volume% or less, 83 volume% or less, 80 volume% or less, 76 volume% or less, 73 volume% or less, 70 volume% or less, 67 volume% or less, 65 volume% or less, 62 volume% or less, 60 volume% or less, 58 volume% or less, 55 volume% or less, 53 volume% or less, or 51 volume% or less of the total volume of the structure.

[0086] Embodiment 9. A structure in any one of Embodiments 1 to 8, wherein most of the particles are in contact with each other, and more than 50%, 55% or more, 60% or more, 70% or more, 80% or more, 90% or more, or 95% or more of the particles are in contact with each other.

[0087] Embodiment 10. In any one of Embodiments 1 to 9, the structure comprises a solid electrolyte material comprising 55 volume% or more, 60 volume% or more, 63 volume% or more, 68 volume% or more, 50 volume% or more, 72 volume% or more, 75 volume% or more, or 78 volume% or more, based on the total volume of the structure; A structure comprising a solid electrolyte material comprising 98 volume% or less of the total volume of the structure, or 97 volume% or less, 95 volume% or less, 93 volume% or less, 91 volume% or less, 89 volume% or less, 86 volume% or less, 83 volume% or less, 80 volume% or less, 76 volume% or less, 73 volume% or less, 70 volume% or less, 67 volume% or less, 65 volume% or less, 62 volume% or less, 60 volume% or less, 58 volume% or less, 55 volume% or less, 53 volume% or less, or 51 volume% or less of the total volume of the structure.

[0088] Embodiment 11. A structure in any one of Embodiments 1 to 10, wherein the polymeric fiber comprises high-density polyethylene (HDPE), polypropylene (PP), or both, and the polymeric fiber comprises high-density polyethylene (HDPE).

[0089] Embodiment 12. An embodiment of any one of Embodiments 1 to 11, further comprising animal wax, vegetable wax, petroleum wax, derivatives thereof, or combinations thereof, wherein the structure comprises ozokerite wax, paraffin wax, or any combination thereof, and the polymeric fiber comprises ozokerite wax, paraffin wax, or any combination thereof.

[0090] Embodiment 13. A structure in any one of Embodiments 1 to 12, wherein the particles comprise a maximum particle size of 0.5 μm or more and 20 μm or less, a minimum particle size of 100 nm or more and 5 μm or less, or a combination thereof; and the particles comprise an average particle size of 0.1 μm or more and 10 μm or less.

[0091] Embodiment 14. In any one of Embodiments 1 to 13, the structure comprises a bimodal particle size distribution comprising 20% ​​or less of particles based on the volume of the particles, wherein the particles have a particle size of less than 2 μm.

[0092] Embodiment 15. In any one of Embodiments 1 to 14, the particles comprise a hygroscopic material; and the solid electrolyte material is of the formula M 3-δ (Me k+ ) f X 3-δ+k*f A structure comprising a halide-based material represented by the above formula (wherein -3≤δ<3, 0≤f≤1, k is the valence of Me, 2≤k<6, M includes Li, Me includes a metal element different from M, and X includes a halogen), wherein the halide-based material comprises at least two metal elements.

[0093] Embodiment 16. The structure of Embodiment 15, wherein Me comprises Y, In, Sn, Fe, rare earth elements, Bi, Zr, Ti, Hf, Sb, alkaline earth metal elements, or any combination thereof.

[0094] Embodiment 17. In any one of Embodiments 1 to 16, the particle comprises a sulfide-based material, an oxyhalide, a halide hydroxide, an oxide, or any combination thereof, forming a structure.

[0095] Embodiment 18. A structure comprising a thickness of 0.1 μm or more, 1 μm or more, 5 μm or more, 6 μm or more, 7 μm or more, 8 μm or more, 9 μm or more, 10 μm or more, 12 μm or more, 14 μm or more, 17 μm or more, or 20 μm or more in any one of Embodiments 1 to 17.

[0096] Embodiment 19. A structure comprising, in any one of Embodiments 1 to 18, a thickness of 500 μm or less, 400 μm or less, 200 μm or less, 100 μm or less, 80 μm or less, 60 μm or less, 40 μm or less, 30 μm or less, 20 μm or less, 10 μm or less, or 8 μm or less.

[0097] Embodiment 20. A structure comprising, in any one of embodiments 1 to 19, a porosity of 20 volume% or less, 15 volume% or less, 10 volume% or less, 9 volume% or less, 8 volume% or less, 7 volume% or less, 6 volume% or less, 5 volume% or less, 4 volume% or less, 3 volume% or less, 2 volume% or less, or 1 volume% or less, based on the total volume of the structure.

[0098] Embodiment 21. A structure comprising, in any one of embodiments 1 to 20, a porosity of 0.05 volume% or more, 0.1 volume% or more, 0.5 volume% or more, or 1 volume% or more with respect to the total volume of the structure.

[0099] Embodiment 22. A structure in any one of Embodiments 1 to 21, wherein the polymeric fiber does not contain an elastomer.

[0100] Embodiment 23. An embodiment of any one of Embodiments 1 to 22, wherein the structure does not contain a solvent.

[0101] Embodiment 24. In any one of Embodiments 1 to 23, 0.02 mS / cm or more, e.g. 0.03 mS / cm or more, 0.04 mS / cm or more, 0.05 mS / cm or more, 0.06 mS / cm or more, 0.07 mS / cm or more, 0.08 mS / cm or more, 0.09 mS / cm or more, or 0.10 mS / cm or more, 0.11 mS / cm or more, 0.12 mS / cm or more, 0.13 mS / cm or more, 0.14 mS / cm or more, 0.16 mS / cm or more, 0.20 mS / cm or more, 0.30 mS / cm or more, 0.40 mS / cm or more, 0.50 mS / cm or more, 0.60 mS / cm or more, 0.70 mS / cm or more, A structure comprising an ionic conductivity of 0.80 mS / cm or more, 0.90 mS / cm or more, 1 mS / cm or more, 2 mS / cm or more, 3 mS / cm or more, 4 mS / cm or more, or 5 mS / cm or more.

[0102] Embodiment 25. A structure comprising, in any one of Embodiments 1 to 24, an ionic conductivity of 10 mS / cm or less, 8 mS / cm or less, 6 mS / cm or less, 5 mS / cm or less, 4 mS / cm or less, 3 mS / cm or less, 2 mS / cm or less, 1.5 mS / cm or less, 1 mS / cm or less, 0.8 mS / cm or less, 0.7 mS / cm or less, 0.5 mS / cm or less, 0.4 mS / cm or less, 0.25 mS / cm or less, 0.22 mS / cm or less, 0.20 mS / cm or less, 0.19 mS / cm or less, 0.18 mS / cm or less, 0.17 mS / cm or less, 0.16 mS / cm or less, or 0.15 mS / cm or less.

[0103] Embodiment 26. In any one of Embodiments 1 to 25,

[0104] Polymeric fibers have random orientation or;

[0105] At least most polymeric fibers extend in intersecting directions;

[0106] The length of the polymeric fiber forms an angle with respect to the thickness direction of the structure, and the angle includes an acute angle, an obtuse angle, or any combination thereof; or

[0107] A structure that is any combination of these.

[0108] Embodiment 27. In any one of Embodiments 1 to 26, the polymeric fiber forms a three-dimensional fiber structure, the structure.

[0109] Embodiment 28. A structure in any one of Embodiments 1 to 27, wherein the polymeric fibers are connected to extend three-dimensionally over at least a portion of the volume of the structure.

[0110] Embodiment 29. A structure in any one of Embodiments 1 to 28, wherein most of the polymeric fibers have a maximum width-to-length aspect ratio of 0.2 or less, of which 60% or more, 70% or more, 80% or more, or 90% or more; or wherein essentially all of the polymeric fibers have a maximum width-to-length aspect ratio of 0.2 or less.

[0111] Embodiment 30. In any one of Embodiments 1 to 29, the total content of an organic material is less than 50 volume%, 45 volume% or less, 40 volume% or less, 35 volume% or less, 30 volume% or less, 28 volume% or less, 25 volume% or less, 22 volume% or less, 20 volume% or less, 17 volume% or less, 14 volume% or less, 11 volume% or less, 8 volume% or less, 5 volume% or less, or 3 volume% or less, based on the total volume of the structure; A structure comprising a total content of organic material of 2 volume% or more, 3 volume% or more, 5 volume% or more, 8 volume% or more, 10 volume% or more, 12 volume% or more, 15 volume% or more, 18 volume% or more, 20 volume% or more, 25 volume% or more, 30 volume% or more, 35 volume% or more, 38 volume% or more, 40 volume% or more, 45 volume% or more, or 49 volume% or more, based on the total volume of the structure.

[0112] Embodiment 31. A structure in any one of embodiments 1 to 30, wherein the polymeric fiber comprises a majority of the total content of the organic material, 55 volume% or more, 60 volume% or more, 70 volume% or more, 80 volume% or more, 90 volume% or more, or 95 volume% or more of the total content of the organic material; or the polymeric fiber comprises essentially the entire total content of the organic material, 99 volume% or less of the total content of the organic material, for example 97 volume% or less, 95 volume% or less, 92 volume% or less, 90 volume% or less, 86 volume% or less, 84 volume% or less, 82 volume% or less, 80 volume% or less, 75 volume% or less, 73 volume% or less, 70 volume% or less, 65 volume% or less, 63 volume% or less, 60 volume% or less, or 58 volume% or less.

[0113] Embodiment 32. In any one of embodiments 1 to 31, the polymeric fiber comprises a polymer, and the polymer is present in an amount of less than 50 volume%, 45 volume% or less, 40 volume% or less, 35 volume% or less, 30 volume% or less, 28 volume% or less, or 25 volume% or less with respect to the total volume of the structure.

[0114] Embodiment 33. In any one of Embodiments 1 to 32, the structure is in the form of a tape, sheet, block, film, disk, or any combination thereof.

[0115] Embodiment 34. In any one of Embodiments 1 to 33, the structure is a freestanding type, a single-layer structure, or both.

[0116] Embodiment 35. A structure comprising, in any one of Embodiments 1 to 34, an electronically conductive material comprising a conductive additive, an anode active material, or a combination thereof.

[0117] Embodiment 36. A structure comprising, in any one of Embodiments 1 to 34, an electronically conductive material comprising a conductive additive, a cathode active material, or a combination thereof.

[0118] Embodiment 37. A multilayer structure comprising an anode in direct contact with a structure of any one of Embodiments 1 to 34.

[0119] Embodiment 38. An electrolyte comprising a structure of any one of Embodiments 1 to 34.

[0120] Embodiment 39. A separator comprising a structure of any one of Embodiments 1 to 34.

[0121] Examples

[0122] Example 1

[0123] Representative sample S1 is formed using a tabletop mixer / extruder placed inside a glove box. A die with a thickness of 0.3 mm is used. Li3YBr 1.2 Cl 4.8A mixture of powder, high-density polyethylene (having an MFR of 35.7 g / 10 min under a load of 2.16 kg at 180°C), and ozokerite wax is prepared, containing 86 wt% of halide relative to the total sum of the halide and organic materials. The weight ratio of HDPE to ozokerite wax is 1:1. The blend of HDPE and ozokerite wax has an MFR greater than 90 g / 10 min at 150°C. The mixture is added, blended, and extruded in 5 to 6 batches, each containing 4 g of halide. The screw is set to 20 rpm. The timing for adding subsequent batches is 1 to 1.5 minutes, during which the torque reading increases from approximately 2 Nm to 8 Nm and then begins to decrease again. When adding the material to the barrel, care must be taken to use less than 20 rpm to avoid poor mixing of the organic materials and halide. To avoid air bubbles being incorporated into the tape, the RPM is controlled so that it does not reach 200 to 300 during extrusion. During extrusion, the belt speed is matched to an extrusion speed of a low RPM of 5 to 10, which helps prevent edge defects. Subsequently, the tape is fed onto a conveyor and cooled.

[0124] The process of forming S1 is repeated with the changes mentioned below. When adding the same mixture of S1 in batches, if the rpm exceeds 20, the second batch is added to the funnel and fed to the screw. HDPE pellets are observed to pop out of the funnel.

[0125] The process of forming S1 is repeated with the changes mentioned below. When adding the same mixture of S1 in batches, the next batch is added before the torque begins to decrease, causing the torque to reach its maximum and the screw to stop moving. If an additional attempt is made to operate the screw again, the torque reaches its maximum. The barrel is disassembled to completely remove the blockage.

[0126] The process of forming S1 is repeated with the changes mentioned below. A first batch containing 4 g of halide powder is fed into the extruder. The rpm is maintained at 20 and the batch is allowed to reach the die without adding additional batches. The batch is not extruded because there is insufficient back pressure to push it through the die.

[0127] The process of forming S1 is repeated with the changes mentioned below. A first batch containing 4 g of halide powder is fed into the extruder. The screw RPM is set to 20, and the batch is allowed to move through the entire barrel. A second batch is added when it is observed that some material is approaching, but before it passes through the die. Since the second batch does not appear to apply sufficient pressure to extrude the first batch, the addition at this point is observed to be too late. The material accumulates and densifies behind the die and can therefore exit the die. Before proceeding, the die is separated and the material is removed.

[0128] In the present disclosure, halide-based materials having different halogens, metal elements, and / or molar ratios between the halogens may be used and may be collectively referred to by the elements of the components. For example, Li3YBr 1.2 Cl 4.8 It can be referred to as LYBC, and Li3YBr6 can be referred to as LYB.

[0129] Example 2

[0130] The organic material is mixed with LYBC in a weight ratio of 1:1, and XRD analysis is performed on the mixture to determine the electrolyte decomposition of the halide-based material. The organic material is heated to its melting point and then mixed with the halide. The mixture is flattened and cooled for XRD analysis. The organic material is considered compatible when minimal or no decomposition is observed (when the reactivity value is 2% or less).

[0131] Test data and specified characteristics of organic materials are included in Table 1.

[0132] [Table 1]

[0133]

[0134] Example 3

[0135] Separator tape samples S5 to S8 are formed by extrusion. Tape samples S5 to S8 are formed using the same LYBC used to form S1. Sample S5 is prepared using PS. Sample S6 is prepared using PP and ozokerite wax. The blend of PP and ozokerite wax has an MRF greater than 90 g / 10 min at 180°C. Samples S7 and S8 are prepared using HDPE and ozokerite wax. The blend of HDPE and ozokerite wax has an MRF greater than 90 g / 10 min at 180°C. Mixing and extrusion are performed according to the method for forming S1 as described in Example 1, except that different amounts of LYBC and organic materials are used. The weight ratio of each binder to ozokerite wax is maintained at 1:1. Ozokerite wax is not used to form sample S5 because the extrusion temperature is higher than the decomposition temperature of the wax. The content (volume %) of solid electrolyte material relative to the total volume of the tape is shown in Table 2.

[0136] The average particle size of coarse LYBC particles is 10 μm. The average particle size of fine LYBC particles is 2 μm.

[0137] [Table 2]

[0138]

[0139] Note that it is difficult to reach a solid loading amount of more than 53 volume% using PS as a binder material.

[0140] It can be observed that samples S7 and S8 have higher ionic conductivity compared to samples S5 and S6. At lower solid loading amounts, sample S7 exhibits improved ionic conductivity compared to sample S8.

[0141] Sample C10, a separator tape sample, is formed using polyisobutylene (PIB) as a binder material as follows. PIB is tested to be compatible with LYBC.

[0142] PIB was pre-dissolved in toluene, a chemically compatible solvent material, and then mixed with the same LYBC powder material used to form samples S6 and S8. The composition of the mixture is included in Table 3. Tape casting of the mixture was performed on a thin aluminum foil using a doctor blade. The tape was allowed to dry without applying heat. The composition and ionic conductivity of the tape are included in Table 4.

[0143] [Table 3]

[0144]

[0145] [Table 4]

[0146]

[0147] It can be seen that sample C10 has a higher solid loading amount than sample S8 but has similar ionic conductivity to sample S8.

[0148] FIGS. 7a through 7d each include SEM images of samples S8, S6, C10, and S5. Sample S8 comprises fibers (602) and particles (604) attached to the fibers (602) and each other. Sample S6 comprises fibers (606) and particles (608) attached to the fibers (606) and each other. Sample C10 comprises particles (610) attached to each other, and no fibers are observed. Sample S5 comprises particles (612) attached to a binder material (614), and no fibers are observed. It can be observed that sample S8 has a higher fiber concentration than S6.

[0149] Example 4

[0150] Separator tape samples S12 and S13 are formed using PP and HDPE, respectively, as binders according to the method of forming sample S1. Samples S12 and S13 have the same LYBC content of 86 wt% relative to the total weight of the tape, and the polymer-to-wax weight ratio is 1:1. The fiber concentration of the samples is measured as described in the embodiments of this specification. The fiber concentration of the two sample groups is analyzed for each binder type. The fiber concentrations with a maximum width-to-length aspect ratio of 0.2 or less are shown in FIG. 8. Sample S13 has a significantly higher fiber concentration than sample S12. The average ionic conductivity of the samples is included in Table 5 below. Sample S13 exhibits improved ionic conductivity compared to sample S12.

[0151] [Table 5]

[0152]

[0153] The foregoing embodiments indicate that they are out of the latest technology. The embodiments relate to a structure comprising particles comprising a solid electrolyte material attached to fibers comprising a polymer. The structure may have improved microstructure, e.g., fiber concentration, fiber aspect ratio, or any combination thereof, and / or properties including ionic conductivity, uniformity, flexibility, toughness, or a combination thereof. The structure may be formed using a solvent-free process and by carefully controlling certain parameters.

[0154] Advantages, other advantages, and solutions to problems have been described above in relation to specific embodiments. However, any advantage, advantage, solution to problem, and any feature(s) that may give rise to or further highlight any advantage, advantage, or solution should not be interpreted as important, necessary, or essential features of any or all claims. References to a material comprising one or more components in this specification may be interpreted to include at least one embodiment in which the material is essentially composed of one or more identified components. The term “essentially composed of” will be interpreted to include a composition comprising the identified material and excluding all other materials except that they are present in a small amount (e.g., impurity content) that does not significantly alter the properties of the material. Additionally or alternatively, in certain non-limiting embodiments, any composition identified in this specification may essentially not contain any materials not explicitly disclosed. It will be understood that embodiments in this specification include a specified range of amounts for certain components within a material, and that the total amount of the components within a given material is 100%.

[0155] The specifications and examples of the embodiments described herein are intended to provide a general understanding of the structures of various embodiments. The specifications and examples are not intended to serve as a complete and comprehensive description of all elements and features of devices and systems using the structures or methods described herein. Distinct embodiments may also be provided in combination with a single embodiment, and conversely, for brevity, various features described in the context of a single embodiment may also be provided separately or in any sub-combination. Additionally, references to values ​​presented within a range include each and all values ​​within that range. Many other embodiments may be apparent to those skilled in the art only after reading this specification. Other embodiments may be used and derived from this disclosure so that structural substitutions, logical substitutions, or other modifications may be made without departing from the scope of this disclosure. Accordingly, this disclosure should be considered illustrative rather than restrictive.

Claims

Claim 1 As a structure, it comprises particles of a solid electrolyte material attached to a polymeric fiber, wherein the fiber concentration of the polymeric fiber is 0.15 / μm 2 Lee Sang-in, structure. Claim 2 A structure comprising particles of a solid electrolyte material attached to a polymeric fiber, wherein the polymeric fiber comprises a polymer having a melt flow rate greater than 10 g / 10 min. Claim 3 A structure comprising particles of a solid electrolyte material attached to a polymeric fiber, wherein the polymeric fiber comprises high-density polyethylene (HDPE), low-density polyethylene (LDPE), polypropylene (PP), or a combination thereof. Claim 4 A structure comprising a polymeric fiber having a maximum width-to-length aspect ratio of 0.2 or less, in any one of claims 1 to 3. Claim 5 In paragraph 2 or 3, 0.15 / μm 2 A structure comprising the above-mentioned fiber concentration of the polymeric fiber. Claim 6 A structure according to claim 1 or 3, wherein the polymeric fiber comprises a polymer having a melt flow rate of more than 10 g / 10 min. Claim 7 A structure according to any one of claims 1 to 6, wherein the polymeric fiber comprises a polymer having a melting temperature of less than 300 degrees and greater than 100 degrees. Claim 8 A structure according to any one of claims 1 to 7, wherein the structure comprises at least 55 volume% of the solid electrolyte material with respect to the total volume of the structure. Claim 9 In claim 8, the structure in which most of the particles of the solid electrolyte material are in contact with each other. Claim 10 A structure according to any one of claims 1 to 9, wherein the polymeric fiber comprises high-density polyethylene (HDPE), polypropylene (PP), or both. Claim 11 A structure according to any one of claims 1 to 10, further comprising animal wax, vegetable wax, petroleum wax, derivatives thereof, or combinations thereof, wherein the structure comprises ozokerite wax, paraffin wax, or any combination thereof, and the polymeric fiber comprises ozokerite wax, paraffin wax, or any combination thereof. Claim 12 A structure according to any one of claims 1 to 11, wherein the particle comprises a maximum particle size of 0.5 μm or more and 20 μm or less, a minimum particle size of 100 nm or more and 5 μm or less, or a combination thereof. Claim 13 A structure according to any one of claims 1 to 12, wherein the particle comprises a bimodal particle size distribution. Claim 14 In any one of claims 1 to 13, the particles comprise a hygroscopic material; and the solid electrolyte material is of the formula M 3-δ (Me k+ ) f X 3-δ+k*f A structure comprising a halide-based material represented by the above formula (wherein -3≤δ<3, 0≤f≤1, k is the valence of Me, 2≤k<6, M includes Li, Me includes a metal element different from M, and X includes a halogen), wherein the halide-based material comprises at least two metal elements. Claim 15 A structure according to any one of claims 1 to 14, wherein the polymeric fibers have a random orientation; at least most of the polymeric fibers extend in an intersecting direction; the length of the polymeric fibers forms an angle with respect to the thickness direction of the structure, said angle including an acute angle, an obtuse angle, or any combination thereof; or any combination thereof.

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