Structure including solid electrolyte material and organic material and methods of forming

Abstract

A structure can include particles including an electrolyte material attached to fibers including a polymer. The electrolyte material can include an inorganic material. In an embodiment, the structure can include a fiber concentration of at least 0.15 / µm2.

Description

[0001] STRUCTURE INCLUDING SOLID ELECTROLYTE MATERIAL AND ORGANIC

[0002] MATERIAL AND METHODS OF FORMING

[0003] TECHNICAL FIELD

[0004] The following is directed to a structure including a solid electrolyte material and an organic material and methods of forming the same, and to, in particular, a structure including a solid electrolyte material and fibers including a polymer and methods of forming the same. BACKGROUND ART

[0005] The electrolyte layer for all solid-state Li batteries (ASSLB) can be formed via a tapecasting method. Solvent is generally used as the carrier for the electrolyte material and binders in the system. As solvent must be dried off, the process can increase manufacturing costs and environmental impact. The industry continues to demand improved electrolyte and all solid-state batteries.

[0006] BRIEF DESCRIPTION OF THE DRAWINGS

[0007] The present disclosure may be better understood, and its numerous features and advantages made apparent to those skilled in the art by referencing the accompanying drawings.

[0008] FIG. 1 includes an SEM image illustrating a portion of a structure in accordance with an embodiment herein.

[0009] FIG. 2 includes an SEM image illustrating a portion of a structure in accordance with another embodiment herein.

[0010] FIGs. 3 A to 3C include an SEM image illustrating a portion of a structure in accordance with another embodiment herein.

[0011] FIG. 4 includes XRD patterns of LEYBn, and decomposed LisYBre.

[0012] FIG. 5 includes a cross-sectional illustration of a structure including a plurality of layers in accordance with an embodiment.

[0013] FIG. 6 includes a flow chart illustrating a process of forming a structure in accordance with an embodiment herein.

[0014] FIGs. 7A to 7D include SEM images demonstrating microstructures of different samples.

[0015] FIG. 8 includes an illustration of fiber concentrations of different samples.

[0016] Skilled artisans appreciate that elements in the figures are illustrated for simplicity and clarity and have not necessarily been drawn to scale. For example, the dimensions of some of the elements in the figures can be exaggerated relative to other elements to help improve understanding of embodiments of the invention. The use of the same reference symbols in different drawings indicates similar or identical items.

[0017] DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENT(S)

[0018] The following description, in combination with the figures, is provided to assist in understanding the teachings disclosed herein. The following discussion will focus on specific implementations and embodiments of the teachings. This focus is provided to assist in describing the teachings and should not be interpreted as a limitation on the scope or applicability of the teachings.

[0019] As used herein, the terms “comprises,” “comprising,” “includes,” “including,” “has,” “having,” or any other variation thereof, are intended to cover a non-exclusive inclusion. For example, a process, method, article, or apparatus that comprises a list of features is not necessarily limited only to those features but can include other features not expressly listed or inherent to such process, method, article, or apparatus. Further, unless expressly stated to the contrary, “or” refers to an inclusive-or and not to an exclusive-or. For example, a condition A or B is satisfied by any one of the following: A is true (or present) and B is false (or not present), A is false (or not present) and B is true (or present), and both A and B are true (or present).

[0020] The use of “a” or “an” is employed to describe elements and components described herein. This is done merely for convenience and to give a general sense of the scope of the invention. This description should be read to include one or at least one and the singular also includes the plural, or vice versa, unless it is clear that it is meant otherwise.

[0021] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The materials, methods, and examples are illustrative only and not intended to be limiting.

[0022] Embodiments herein relate to structures that can include a solid electrolyte material and an organic material. In particular embodiments, the structures can include particles including a solid electrolyte material and attached to fibers including an organic material, such as a polymer. In more particular embodiments, the structures may include particular fiber density, aspect ratios of fibers, content of solid electrolyte, average particle size, particle size distributions, or any combination thereof. The structures may have improved properties, such as improved ionic conductivity, mechanical strength, electrochemical stability, or any combination thereof. Embodiments relate to a process of forming the structures. In particular, the process may include a dry process. For example, a solvent may not be utilized in the process. In particular embodiments, one or more parameters of the process may be carefully controlled to form structures having improved microstructure, solid loadings, uniformity, properties, or any combination thereof.

[0023] In an embodiment, the structure may include an organic material and a solid electrolyte material including an inorganic material, wherein the organic material may include a polymer in the form of fibers. In another embodiment, the structure may include fibers including a polymer and a solid electrolyte material directly attached to fibers, wherein the solid electrolyte material may be in the form of particles. In an example, the particles including the solid electrolyte material may include different shapes and / or forms, such as loose particles, aggregates, granules, pellets, sheets, platelets, rods, another shape of a solid mass, or any combination thereof. In a particular embodiment, the structure may include particles of the electrolyte material attached to fibers including a polymer. In a particular example, the fibers may consist essentially of one or more polymers. In another embodiment, the structure may include a network including fibers extending 3 -dimensionally and particles of an electrolyte material. For example, fibers may extend through at least a portion of the volume of the structure. In another example, fibers may be attached to one another, one or more particles, or any combination thereof. In a particular example, fibers may form a 3- dimensional fibrous structure. In another particular example, particles including an electrolyte material may be dispersed uniformly in the 3-dimensional fibrous structure.

[0024] FIG. 1 includes a scanning electron microscope image of a cross section of the structure 100 according to an embodiment. The structure 100 includes particles 104 including an electrolyte material and fibers 106. A fiber 106 may be attached to one or more particles 104 and / or another fiber 106. In an embodiment, fibers 106 can consist of an organic material. In a particular embodiment, fibers 106 can consist of one or more polymers.

[0025] As illustrated, fibers 106 may have random orientations. For example, fibers 106 may include fibers that extend in directions that may intersect, substantially in parallel, or any combinations thereof.

[0026] In an embodiment, the organic material may include a particular Melt Flow Rate (also referred to as “MFR”) that may facilitate improved formation and / or properties of the structure. For example, the structure may include a polymer having a particular Melt Flow Rate that may facilitate improved formation and / or properties of the structure. In this disclosure, Melt Flow Rate of an organic material may be measured at 150 °C to 200 °C according to ASTM DI 238, Procedure A. In an 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, such as at least 13 g / 10 min, at least 14 g / 10 min, at least 15 g / 10 min, at least 17 g / 10 min, at least 20 g / 10 min, at least 22 g / 10 min, at least 25 g / 10 min, at least 27 g / 10 min, at least 30 g / 10 min, at least 33 g / 10 min, at least 35 g / 10 min, at least 38 g / 10 min, or at least 40 g / 10 min. In a particular example, the organic material may include a material having a Melt Flow Rate greater than 40 g / 10 min, such as at least 55 g / 10 min, at least 70 g / 10 min, at least 85 g / 10 min, at least 90 g / 10 min, or greater than 90 g / 10 min. In another example, the organic material may include a material having the Melt Flow Rate of at most 200 g / 10 min, at most 180 g / 10 min, at most 150 g / 10 min, at most 130 g / 10 min, at most 120 g / 10 min, at most 110 g / 10 min, at most 100 g / 10 min, at most 90 g / 10 min, at most 80 g / 10 min, at most 70 g / 10 min, at most 60 g / 10 min, at most 55 g / 10 min, or at most 50 g / 10 min. Moreover, the organic material may include a material having the Melt Flow Rate in a range including a minimum and maximum values noted herein. For example, the organic material may include a material having an MFR in a range including greater than 10 g / 10 min and at most 200 g / 10 min or in a range including at least 25 g / lOmin and at most 200 g / lOmin or in a range including at least 55 g / lOmin and at most 200 g / lOmin or in a range including at least 90 g / lOmin and at most 200 g / lOmin. In a particular embodiment, the fibers may include a polymer having the Melt Flow Rate in a range including any of the minimum and maximum values noted herein. In an embodiment, the structure and / or fibers may include a blend of organic materials, wherein the blend may have any of the MFR noted in embodiments herein. For example, the blend may include an MFR of greater thanlO g / 10 min, at least 20 g / 10 min, at least 30 g / 10 min, at least 40 g / 10 min, at least 55 g / 10 min, at least 70 g / 10 min, at least 85 g / 10 min, at least 90 g / 10 min, or greater than 90 g / 10 min. In another example, the blend may include an MFR of at most 200 g / 10 min, at most 180 g / 10 min, at most 150 g / 10 min, at most 130 g / 10 min, at most 120 g / 10 min, or at most 110 g / 10 min. Moreover, the blend may include an MFR in a range including any of the minimum and maximum values noted herein. For example, the blend may include an MFR in a range including greater than 10 g / 10 min and at most 200 g / 10 min or in a range including at least 50 g / lOmin and at most 200 g / lOmin or in a range including at least 90 g / lOmin and at most 200 g / lOmin. MFR of a blend of organic materials may be measured in the same manner as described above. The blend may be prepared by mixing organic materials in the same wt% for the total weight of the blend. For example, a blend of two organic materials may have a weight ratio therebetween of 50:50. After reading this disclosure, a skilled artisan appreciates that MFR may affect formation and / or properties of the structures of embodiments herein. For example, MFR may have impact on solid loading, strength, or a combination thereof of the structure. For example, too high an MFR may have an adverse effect, such as, resulting in structures with insufficient strength to hold appropriate shapes during the forming process. In another example, too low an MFR may have adverse effect on solid loading. For example, too low a MFR may result in too low a solid loading.

[0027] In an embodiment, the structure may include an organic material that may be more lipophilic / hydrophobic than hydrophilic / lipophobic. In an example, the organic material may have certain hydrophile-lipophile balance determined according to Grifin’s Mathematical method using the formula, HLB = 20*Mh / M, wherein Mh is the molecular mass of the hydrophilic portion of the organic material, and M is the molecular mass of the whole organic material. To aid understanding, using an exemplary scale of HLB of 0 to 20, an HLB value of 0 can correspond to a completely lipophilic / hydrophobic molecule, and a value of 20 can correspond to a completely hydrophilic / lipophobic molecule. In a particular embodiment, the structure may include an organic material that may have an HLB value of at most 10, at most 5, at most 4, at most 3, at most 2, at most 1, or at most 0.5. In a more particular embodiment, the organic material may be lipophilic / hydrophobic, such as having the HLB value of 0.

[0028] In a further embodiment, the organic material may have limited reactivity to the solid electrolyte material during the process of forming the structure. In a further embodiment, reactivity of the organic material may be tested and quantified by using X-ray diffraction analysis as follows. The organic material and the solid electrolyte material may be mixed at a weight percentage ratio of the organic material to the solid electrolyte material of 50:50 for 1- 3 minutes. The mixture may be kept in a Kapton tube at temperatures for forming the structure, such as from 150 °C to 200 °C, in an inert atmosphere for at least 12 hours and up to 2 to 4 days before further analyzed. The mixture can then be sealed in a gas-tight sample holder having a Kapton film window for performing X-ray diffraction (XRD) analysis from 25 to 80 degrees two-theta with the step size of 7.5 degree and step duration of 120 seconds. The entire testing can be performed in a dry environment with H2O content <1 ppm. The XRD pattern of the mixture may be compared to the XRD pattern of the solid electrolyte material to evaluate changes to the XRD pattern of the solid electrolyte material. After reading this disclosure, a skilled artisan appreciates degradation or decomposition of the solid electrolyte material may cause changes to the XRD pattern of the solid electrolyte material. Changes may include disappearance of one or more characteristic peaks of the solid electrolyte material, changes to intensity of one or more characteristic peaks of the solid electrolyte material, appearance of new peaks, disappearance of other peaks, or any combination thereof.

[0029] In an embodiment, the organic material may include a particular Reactivity Value that may facilitate improved formation and property of the structure. For example, the organic material may have a Reactivity Value of at most 20% or less than 20%, such as at most 18%, at most 15%, at most 12%, or at most 10%. In a particular example, the organic material may have a Reactivity Value of less than 10%, such as at most 9%, at most 8%, at most 7%, at most 6%, at most 5%, at most 4%, at most 3%, or at most 2%. In another example, the organic material can have a Reactivity Value of 0% or greater than 0%, such as at least 0.01%, at least 0.1%, at least 0.2%, at least 0.3%, at least 0.5%, at least 0.8%, or at least 1%. Moreover, the Reactivity Value can be in a range including any of the minimum and maximum percentages noted herein. For example, the organic material can have Reactivity Value of up to at most 2%.

[0030] The Reactivity Value of the organic material may be determined using the formula, RV=[B / A]x 100% based on the XRD pattern of the mixture, wherein A represents the intensity of the characteristic peak of the solid electrolyte material and B represents the intensity of the characteristic peak of a representative decomposition product of the solid electrolyte material. A representative decomposition product may include a binary compound including the major anion and cation atoms of the solid electrolyte material. For example, the solid electrolyte material may include a halide-based material, and lithium halide may be a representative decomposition product of the halide-based material. Accordingly, A can be a characteristic peak of the halide-based material, and B can be the characteristic peak of lithium halide. Referring to FIG. 4, the XRD pattern of LAYBR, includes the characteristic peak A that typically appears between 31 and 32.2 degrees two theta. The XRD pattern of decomposed LisYBre includes the characteristic peak B of the decomposition product, LiBr, that typically appears between 27.9 and 28.5 degrees two theta. In the instance that the XRD pattern of the mixture does not include the characteristic peak of the decomposition product and A the characteristic peak of the solid electrolyte material is present (i.e., A is not 0), the Reactivity Value of the organic material can be 0. In the instances that the XRD pattern of the mixture does not include the characteristic peak of the solid electrolyte material, the Reactivity Value of the organic material can be indefinite.

[0031] In an embodiment, the organic material may include a particular binder material, a coupling agent, a plasticizer, or a combination thereof. In a further embodiment, any of the binder material, a coupling agent, a plasticizer, or any combination thereof may have the MFR, HLB value, and / or Reactivity Value noted in embodiments herein.

[0032] In an embodiment, the structure may include a particular total content of the organic material that may facilitate improved properties of the structure. In an example, the total content of the organic material may be at most 55 vol% for the total volume of the structure, such as at most 50 vol% or less than 50 vol% for the total volume of the structure. In a particular example, the structure may include not greater than 45 vol% of the organic material for the total volume of the structure, such as not greater than 40 vol%, not greater than 35 vol%, not greater than 30 vol%, not greater 28 vol%, or not greater than 25 vol% for the total volume of the structure. In another example, the total content of the organic material may be at least 5 vol% for the total volume of the structure, such as at least 8 vol%, at least 10 vol%, at least 12 vol%, at least 15 vol%, at least 18 vol%, at least 20 vol%, at least 25 vol%, at least 30 vol%, at least 35 vol%, at least 38 vol%, at least 40 vol%, at least 45 vol%, or at least 49 vol% for the total volume of the structure. Moreover, the structure may include the total content of the organic material in a range including any of the minimum and maximum percentages noted herein.

[0033] In an embodiment, the organic material may include a particular binder material that may facilitate improved formation and / or properties of the structure. In an example, the binder material may include a thermoplastic, a thermoset, or a combination thereof. In another example, the binder material may include one or more thermoplastic polymers. A particular exemplary binder material may include 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 include a coupling agent, a plasticizer, or a combination thereof. In a particular embodiment, the coupling agent may include wax, derivatives thereof, or the like, or any combination thereof. Exemplary wax may include animal waxes, plant waxes, petroleum waxes, derivatives thereof, or any combination thereof. In another embodiment, the organic material may be free of a solvent. In another embodiment, the organic material may be free of an elastomer.

[0034] In an embodiment, the structure may include one or more polymers including high density polyethylene (HDPE), polypropylene (PP), low density polyethylene (LDPE), or any combination thereof. In a further embodiment, the structure may include wax including animal waxes, plant waxes, petroleum waxes, derivatives thereof, or any combination thereof. In another embodiment, the structure may be free of a solvent. In a particular embodiment, the structure may include one or more of high density polyethylene (HDPE), polypropylene (PP), low density polyethylene (LDPE), ozokerite wax, paraffin wax, or any combination thereof. In another embodiment, the structure may be free of an elastomer.

[0035] In an embodiment, the fibers may include one or more polymers. In another embodiment, the fibers may include a polymer having a particular Melt Flow Rate that may facilitate improved formation and / or properties of the structure. In a particular example, the MFR of the polymer may be in reference to the forming temperatures of the structure. In another example, the Melt Flow Rate may be greater than 10 g / 10 min at 150 °C to 200 °C, such as at least 15 g / 10 min, at least 20 g / 10 min, at least 25 g / 10 min, at least 30 g / 10 min, or at least 40 g / 10 min. In another example, the Melt Flow Rate may be at most 200 g / 10 min at 150 °C to 180 °C, at most 180 g / 10 min, at most 150 g / 10 min, at most 130 g / 10 min, at most 120 g / 10 min, at most 100 g / 10 min, at most 90 g / 10 min, at most 80 g / 10 min, at most 70 g / 10 min, at most 55 g / 10 min, or at most 50 g / 10 min. Moreover, the fibers may include a polymer having the Melt Flow Rate in a range including a minimum and maximum values noted herein.

[0036] In another embodiment, the fibers may include a polymer having a particular melt temperature that may facilitate improved formation and / or properties of the structure. In an example, the melt temperature may be less than 300 °C, such as at most 280 °C, at most 260 °C, at most 240 °C, at most 220 °C, at most 205 °C, at most 200 °C, at most 190 °C, at most 180 °C, at most 170 °C, at most 160 °C, at most 150 °C, at most 140 °C, or at most 130 °C. In another example, the melt temperature may be greater than 100 °C, at least 105 °C, at least 110 °C, at least 115 °C, at least 120 °C, at least 125 °C, at least 130 °C, or at least 135 °C. Moreover, the fibers may include a polymer having the melt temperature in a range including a minimum and maximum values noted herein.

[0037] In another embodiment, the fibers may include a polymer having a particular elongation-at-break that may facilitate improved formation and / or properties of the structure. In an example, the polymer may have elongation-at-break in the machine direction of at least 5%, at least 10%, at least 30%, at least 50%, at least 70%, at least 100%, at least 200%, at least 350%, at least 400%, at least 500%, at least 600%, at least 700%, at least 800%, or at least 900%. In another example, the polymer may have elongation-at-break in the machine direction of at most 1000%, such as at most 900%, at most 800%, at most 700%, at most 600%, at most 500%, at most 400%, at most 300%, at most 200%, at most 100%, or at most 55%. Moreover, the fibers may include a polymer having elongation-at-break in the machine direction in a range including a minimum and maximum values noted herein.

[0038] In a further example, the fibers may include a polymer having elongation-at-break in the transverse direction of at least 5%, at least 10%, at least 30%, at least 50%, at least 70%, at least 100%, at least 200%, at least 350%, at least 400%, at least 500%, at least 600%, at least 650%, at least 700%, at least 800%, or at least 900%. In another example, the polymer may have elongation-at-break in the transverse direction of at most 1000%, such as at most 900%, at most 800%, at most 700%, at most 600%, at most 500%, at most 400%, at most 300%, at most 200%, at most 100%, or at most 55%. Moreover, the fibers may include a polymer having elongation-at-break in the transverse direction in a range including a minimum and maximum values noted herein.

[0039] In a further embodiment, the fibers may include a majority of the total content of the organic materials, such as at least 55 vol%, at least 60 vol%, at least 70 vol%, at least 80 vol%, at least 90 vol%, or at least 95 vol% of the total content of the organic material. Additionally or alternatively, the fibers may include at most 99 vol% of the total content of the organic material, such as at most 97 vol%, at most 95 vol%, at most 92 vol%, at most 90 vol%, at most 86 vol%, at most 84 vol%, at most 82 vol%, at most 80 vol%, at most 75 vol%, at most 73 vol%, at most 70 vol%, at most 65 vol%, at most 63 vol%, at most 60 vol%, or at most 58 vol% of the total content of the organic material. In a particular embodiment, the fibers may include essentially all of the total content of the organic material. Moreover, the fibers may include the organic material at a content including any of the minimum and maximum percentages noted herein.

[0040] In another embodiment, the fibers may include a polymer, wherein the polymer may include a particular content that may facilitate improved formation and / or properties of the structure. In an example, the polymer may be in a content of at most 55 vol% or at most 50 vol% or even less than 50 vol% for the total volume of the structure. In a particular example, the polymer may be at most 45 vol% for the total volume of the structure, such as at most 40 vol%, at most 35 vol%, at most 30 vol%, at most 28 vol%, or at most 25 vol% for a total volume of the structure. In another example, the content of the polymer may be at least 5 vol% for the total volume of the structure, such as at least 8 vol%, at least 10 vol%, at least 12 vol%, at least 15 vol%, at least 18 vol%, at least 20 vol%, at least 25 vol%, at least 30 vol%, at least 35 vol%, at least 38 vol%, at least 40 vol%, at least 45 vol%, or at least 49 vol% for the total volume of the structure. Moreover, the fibers may include a polymer, wherein the polymer may be in the content including any of the minimum and maximum percentages noted herein.

[0041] In another embodiment, the fibers may include high density polyethylene (HDPE), polypropylene (PP), low density polyethylene (LDPE), or any combination thereof. In a further embodiment, the fibers may include wax including animal waxes, plant waxes, petroleum waxes, derivatives thereof, or any combination thereof. In a particular embodiment, the fibers may include an organic material consisting essentially of high density polyethylene (HDPE), wax, such as ozokerite wax and / or paraffin wax, or any combination thereof. For example, the fibers may include an organic material consisting essentially of high density polyethylene (HDPE) and wax. In another more particular embodiment, the fibers may include an organic material consisting essentially of polypropylene (PP), high density polyethylene (HDPE), low density polyethylene (LDPE), wax, or any combination thereof. For example, the fibers may include an organic material consisting essentially of wax and one or more of polypropylene (PP), high density polyethylene (HDPE), and low density polyethylene (LDPE). In a particular embodiment, the fibers may be free of an elastomer.

[0042] In another embodiment, the structure may include a particular content of the solid electrolyte material and / or the organic material that may facilitate improved properties of the structure. In an embodiment, the structure may include a particular wt% content or vol% content of the solid electrolyte material or the organic material relative to the weight or volume of the structure, respectively. The content (wt%) may be determined using Inductively Coupled Plasma (ICP) to analyze a structure sample acidified by using nitric acid and elemental analysis. A skilled artisan appreciates that the vol% content can be calculated based on the wt% and density of the component of the structure. In another embodiment, the structure may include a particular content of the solid electrolyte material. In an example, the content of the solid electrolyte material may be at least 55 vol% for the total volume of the structure, such as at least 60 vol%, at least 63 vol%, at least 68 vol%, at least 50 vol%, at least 72 vol%, at least 75 vol%, or at least 78 vol% for the total volume of the structure. In another instance, the structure may include at most 95 vol% of the solid electrolyte material for the total volume of the structure, such as at most 93 vol%, at most 91 vol%, at most 89 vol%, at most 86 vol%, at most 83 vol%, at most 80 vol%, at most 76 vol%, at most 73 vol%, at most 70 vol%, at most 67 vol%, at most 65 vol%, at most 62 vol%, at most 60 vol%, at most 58 vol%, at most 55 vol%, at most 53 vol%, or at most 51 vol% of the solid electrolyte material for the total volume of the structure. Moreover, the content of the solid electrolyte material may be in a range including any of the minimum and maximum percentages noted herein.

[0043] In an embodiment, the structure may include a particular content of the particles including an electrolyte material that may facilitate improved properties of the structure. In an example, the content of the particles may be at least 55 vol% for a total volume of the structure, such as at least 60 vol%, at least 63 vol%, at least 68 vol%, at least 50 vol%, at least 72 vol%, at least 75 vol%, or at least 78 vol% for the total volume of the structure. In a further example, the content of the particles may be at most 95 vol% for the total volume of the structure, such as at most 93 vol%, at most 91 vol%, at most 89 vol%, at most 86 vol%, at most 83 vol%, at most 80 vol%, at most 76 vol%, at most 73 vol%, at most 70 vol%, at most 67 vol%, at most 65 vol%, at most 62 vol%, at most 60 vol%, at most 58 vol%, at most 55 vol%, at most 53 vol%, or at most 51 vol% for the total volume of the structure. Moreover, the content of the particles may be in a range including any of the minimum and maximum percentages noted herein.

[0044] In an embodiment, a majority (i.e., greater than 50%) of the particles may be in contact with one another, such as at least 55%, at least 60%, at least 70%, at least 80%, at least 90%, or at least 95% of the particles may be in contact with one another. Particles in contact may be quantified by examining different SEM images of one or more cross sections of a sample. The number of images is representative of a statistical significance. As used herein, the percentages of particles that may be in contact with one another can be in reference to the total number or content (vol%) of the particles calculated based on the SEM images.

[0045] FIG. 2 includes an SEM image of a cross section of an exemplary structure 200 including fibers 204 that may be taut and fibers 202 that may be not taut. As demonstrated, fibers 202 may be loose, curled, and / or wavy. FIG. 3A includes an SEM image of a cross section of an exemplary structure 300 including a taut fiber 302 and not-taut fiber 304.

[0046] In another embodiment, fibers may include a length, a width, and an aspect ratio of width to length. In a particular embodiment, a single taut fiber (e.g., fibers 202 in FIG. 2 and 302 in FIG. 3A) may have a length. A single fiber, as disclosed herein, can start and end at either another fiber or a particle. The length may be the linear distance between the opposite ends of the fiber. As illustrated in FIGs. 3A and 3B, the fiber 302 may be attached to the fibers 306 and 308 and may thus start at one of fibers 306 and 308 and end at the other. The length 3022 of the fiber 302 may extend between where the fiber 302 contacts 306 and where the fiber 302 contacts 308. As illustrated in FIGs. 3 A-3C, the fiber 302 may include a width that may vary along the length 3022 and may include a maximum width 3026. It is to be appreciated that the structure of embodiments herein may include fibers having a substantially constant width, and width for those fibers may be the maximum width. The fiber 302 may further include an aspect ratio of the maximum width 3026 to length 3022 (APmw / 1). As used herein, an aspect ratio of maximum width to length is intended for taut fibers.

[0047] In another embodiment, the structure (e.g., structures 100, 200 and 300 in FIGs. 1 to 3 A) may include fibers having a particular aspect ratio of maximum width to length (APmw / 1) that may facilitate improved properties of the structure. For example, the structure may include fibers having the aspect ratio of maximum width to length (APmw / 1) of at most 0.2. In a further example, the structure may include fibers having the aspect ratio (APmw / 1) of at least 0.0001, at least 0.001, at least 0.002, at least 0.003, at least 0.004, at least 0.005, at least 0.006, at least 0.007, at least 0.008, at least 0.009, at least 0.01, at least 0.02, at least 0.03, at least 0.04, or at least 0.05. Moreover, the structure may include fibers having the aspect ratio (APmw / 1) in a range including any of the minimum and maximum values noted herein.

[0048] In a particular embodiment, a majority of the fibers (i.e., greater than 50%) may have the aspect ratio of maximum width to length (APmw / 1) of at most 0.2, such as at least 60%, at least 70%, at least 80%, or at least 90% of the fibers may have the aspect ratio of maximum width to length of at most 0.2. Moreover, the content of fibers having the aspect ratio (APmw / 1) of at most 0.2 may be in a range including any of the minimum and maximum percentages noted herein. In a particular example, essentially all of the fibers may have the aspect ratio of maximum width to length (APmw / 1) of at most 0.2. As used herein, the percentages of the fibers can be in reference to the total number of fibers that may be analyzed for the aspect ratio (APmw / 1) or a total content (vol%) of the organic material.

[0049] In a further embodiment, the structure may include a particular fibers concentration that may facilitate improved formation and / or properties of the structure. For example, the structure may include a fiber concentration of at least 0.15 / pm2. In another example, the fiber concentration may not be too high to interfere with contact between particles including the solid electrolyte material, which may have adverse impact on properties of the structure.

[0050] In a particular embodiment, the structure may include a particular fiber concentration of fibers having the aspect ratio (APmw / 1) of at most 0.2 that may facilitate improved formation and / or properties of the structure. For example, the fiber concentration of fibers having the aspect ratio (APmw / 1) of at most 0.2 may be at least 0.15 / pm2, at least 0.18 / pm2, at least 0.20 / pm2, at least 0.22 / pm2, at least 0.25 / pm2, at least 0.30 / pm2, at least 0.33 / pm2, at least 0.35 / pm2, at least 0.38 / pm2, at least 0.40 / pm2, at least 0.45 / pm2, at least 0.50 / pm2, at least 0.55 / pm2, at least 0.60 / pm2, at least 0.62 / pm2, at least 0.65 / pm2, at least 0.70 / pm2, at least 0.73 / pm2, at least 0.75 / pm2, at least 0.78 / pm2, at least 0.80 / pm2, or at least 0.82 / pm2. In another example, the fiber concentration of fibers having the aspect ratio (APmw / 1) of at most 0.2 may be at most 150 / pm2, such as at most 130 / pm2, at most 110 / pm2, most 85 / pm2, at most 60 / pm2, at most 40 / pm2, at most 20 / pm2, most 10 / pm2, at most 7.5 / pm2, at most 4.6 / pm2, at most 2.2 / pm2, most 1.3 / pm2, or at most 0.9 / pm2. In another example, the fiber concentration of fibers having the aspect ratio (APmw / 1) of at most 0.2 may be in a range including any of the minimum and maximum values noted herein.

[0051] As described herein, fiber concertation can be determined as follows. A structure sample may be broken by hand to expose a cross section. Scanning electron microscope images with a width of 25 pm are acquired at random locations throughout the thickness of the cross section of the structure. 2D rectangular areas between 10 pm2and 180 pm2are randomly chosen throughout the SEM images. Areas with particles larger than 5 pm, areas with voids (cavities where particles may have been dislodged) larger than 5 pm, and areas that may be out of focus should be excluded from analysis. The number of clearly distinguishable, taut fibers with an aspect ratio (maximum width / length) of at most 0.2 can be counted. Fibers that may start but end outside of the designated area can be included. It is to be appreciated that a single fiber can start and end at either another fiber or a particle. Fiber concentration can be the number of counted fibers over the total of the 2D areas that are analyzed.

[0052] In an embodiment, the particles (e.g., particles 104 in FIG. 1) may include a solid electrolyte material including a halide-based material, a sulfide-based material, an oxyhalide, a halide hydroxide, an oxide, or any combination thereof. In another embodiment, the particles may include a hygroscopic solid electrolyte material.

[0053] In an embodiment, the halide-based material may be represented by formula M3.5(Mek+)fX3. s+k*f, wherein -3< 5<3, 0<f<l, k is the valence of Me, 2<k<6, M may be one or more alkali metal including Li, Me may include a metal element that is different from M, and X includes a halogen, wherein the halide-based material may include at least two metal elements. A particular example of Me may include a rare earth element, Y, In, Sn, Fe, Bi, Zr, Ti, Hf, Sb, an alkaline earth metal element, , or any combination thereof. In another particular example, X may include at least two halogens including Cl, F, Br, I, or any combination thereof. An exemplary sulfide-based material may include an amorphous phase, a crystalline phase, or any combination thereof. A particular example of the sulfide-based material can include, but not limited to, xLi2S-yP2S5 (LPS), such as 0.67Li2S-0.33P2Ss, 80Li2S-20P2Ss, 75Li2S-25P2Ss, 70Li2S-30P2Ss, and the like, IJ2S-X, wherein X represents at least one sulfide of SiS2, GeS2, and B2S3, such as 0.50Li2S-0.50GeS2, LiI-Li2S-SiS2, such as 0.40LH- 0.36Li2S-0.24SiS2and the like, 0.05Li4Si04-0.57Li2S-0.38SiS2, Li3PO4-Li2S-SiS2, such as 0.01Li3P04-0.63Li2S-0.36SiS2and the like, LiI-Li2S-B2S3, such as 0.44LiI-0.30Li2S- 0.26B2S3and the like, LiI-Li2S-P2S5, such as 0.45LiI-0.37Li2S-0.18P2S5 and the like, a- Li3PS4, LGPS (e g., LiioGeP2Si2), LPSC1 (e g., Li6PS5Cl), LPSBr (e g., Li6PS5Br), LSPSC1 (e.g., Li9.54Sii.74Pi.44Sn.7Clo.3), Liio.35[Sno.27Sii.o8]Pi.65Si2, or any combination thereof.

[0054] In a further example, the solid electrolyte may include a lithium oxyhalide, a lithium halide hydroxide, or any combination thereof, such as Li3OCl, Li3OBr, Li3O(Cl, Br), Li30C10.5Br0.5, Li20HX, Li2OHCl, Li2OHBr, Li7O2(Br3.xFx), Li7O2(BrdCl(i-d))3, Li7O2(BrdFeCl(i-d-e))3, Li4(OH)3X (X is Cl, Br, and / or F), or a combination thereof.

[0055] An exemplary oxide may include an NASICON-type solid electrolyte represented by LiTi2(PO4)3or an element substitute thereof; a (LaLi)TiO3-based perovskite solid electrolyte; an LISICON-type solid electrolyte represented by Lii4ZnGe40i6, Li4SiO4, and LiGeO4, or element substitutes thereof; a garnet-type solid electrolyte represented by Li7La3Zr20i2 or an element substitute thereof; a Li3N or an H substitute thereof; or Li3PO4or an N substitute thereof can be used.

[0056] In an embodiment, the structure may be in a form of a tape, a sheet, a block, a film, a disc, or any combination thereof. In an embodiment, the structure may be free-standing, a single-layer structure, or both.

[0057] In an embodiment, the structure may be formed using a process including mixing, pressing, compounding, casting, molding, extruding, shaping, cutting, or any combination thereof. In a particular embodiment, the process may not involve using a solvent.

[0058] Referring to FIG. 6, a process of forming the structure is illustrated. The process 500 may start at block 502 including forming a mixture including the organic material and solid electrolyte material. In an embodiment, the mixture may be a dry mixture. For example, the organic material may be free of a liquid. In another embodiment, the solid electrolyte material may be mixed with the organic material at a particular weight content ratio that may facilitate improved formation and / or properties. The weight content may be relative to the total weight of the solid electrolyte material and the organic material. In an example, the weight content ratio of the solid electrolyte material to the organic material may be at least 60:40, such as at least 65:35, at least 68:32, at least 70:30, at least 72:38, at least 75:25, at least 78:22, at least 80:20, at least 82: 18, at least 84: 16, at least 86: 14, at least 88: 12, or at least 90: 10. In an example, the weight content ratio of the solid electrolyte material to the organic material may be at most 96:4, such as at most 94:6, at most 92:8, at most 90: 10, at most 88: 12, at most 86: 14, at most 84: 16, or at most 82: 18. Moreover, the weight content ratio of the solid electrolyte material to the organic material may be in a range including any of the minimum and maximum values noted herein.

[0059] In a further embodiment, the organic material may include 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 facilitate formation of a uniform mixture.

[0060] In a further embodiment, mixing may include compounding. For example, materials including the solid electrolyte and organic material may be loaded to a compounder for forming a uniform mixture that may be suitable for further processing to form the structure. In another embodiment, the solid electrolyte material and the organic material may be loaded separately and mixed in a compounding device or an extruder.

[0061] In another embodiment, the process 500 may include pretreating the solid electrolyte material and / or the organic material to have particular particles sizes that may facilitate improved mixing of materials and / or formation and / or properties of the structure. In an example, the material may be cut, broken, milled, ground, sieved, or otherwise treated with techniques known to a skilled artisan, or treated in any combination thereof. In a particular example, the solid electrolyte material may be mechanically milled, e.g., using mortar and pestle, or 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 particular particle size. In a particular example, cryogenic grinding may be used to form particles of the organic material having particular particle sizes.

[0062] The process 500 may continue to block 504, forming the structure from the mixture. In a particular embodiment, one or more parameters of the process 500 may be carefully controlled to allow formation of the structure from a dry mixture. In an embodiment, forming the structure may include compounding, extruding, or a combination thereof. In another embodiment, a suitable apparatus may be used to perform formation of the structure. In an example, the process 500 may include using an extruder or an apparatus that may have equivalent function. An exemplary extruder may include screw extruder, such as single screw extruder / compounder, twin screw extruder, or the like. In another particular embodiment, the extruder may include a die extruder. In an embodiment, a suitable device may be used to perform compounding of the mixture. For example, an extruder or a separate device with compounding functionality may be used. In another embodiment, the process may include feeding the mixture to a barrel of an extruder in batches, wherein the barrel may include a compounding section. For example, the mixture may be divided into batches that may have the similar weight of the solid electrolyte material and fed one at a time to the barrel. In another embodiment, adding a second batch may be performed when at least a portion of the first batch can pass through the compounding section. In a particular embodiment, the barrel may include a plurality of compounding sections, wherein a second batch may be fed when at a least a portion of the first batch can pass through the first compounding section.

[0063] In a further embodiment, adding a second or a subsequent batch may be performed at a particular torque. In a particular embodiment, the next batch may be added after torque goes up and then back down. After reading this disclosure, a skilled artisan can appreciate torque may increase when a load is added to the compounding section and decrease when the load starts to move out of the compounding section. In a particular exemplary application, torque may go up to the maximum torque (e.g., 15 Nm) when a batch is loaded and may drop (e.g., to 2-3 Nm) when the batch starts to move out of the compounding section and before the batch reaches the end of the barrel. After reading this disclosure, a skilled artisan appreciates that the maximum torque may depend on the solid loading (i.e., wt% or vol% of the solid electrolyte material), and the maximum torque may be adjusted to suit different solids loading. In an example, for the solid loading of up to 90 wt%, the torque may be as high as 15 Nm. In another particular embodiment, a subsequent batch may be added at a torque in a range from 2 to 6 Nm. A skilled artisan appreciates that the values of torque may be adjusted for using different instruments so that mixtures can be properly loaded in batches and extruded.

[0064] In another embodiment, a subsequent batch may be added at a particular timing. In a particular example, the timing to add a subsequent batch may be from 0.6 minutes to 2 minutes from adding the earlier batch. In another particular example, a subsequent batch may be added at an rpm of at most 20. It is noted adding materials into the barrel at an rpm of at most 20 may facilitate improved mixability of the organic material, compounding of the solid electrolyte material and organic material, or a combination thereof. In a particular exemplary application, a subsequent batch may be added at an rpm of at least 2, at least 5, at least 10, or at least 15. After reading this disclosure, a skilled artisan appreciates that the screws may be at a low rpm so that a new batch can be incorporated into the barrel and that the values of rpm may be adjusted for using different instruments. In another embodiment, the timing for adding batches to the barrel may be controlled in seconds and up to a few minutes.

[0065] In an embodiment, extrusion may be performed at an rpm of at most 300, which may help reduce formation of gas bubbles, edge defects, or both within the extruded product. Gas bubbles may be observed using SEM imaging. In an example, the rpm of the screw may be less than 300, such as at most 280, at most 250, at most 200, at most 170, at most 150, at most 120, at most 100, at most 70, at most 60, at most 40, at most 30, at most 20, or at most 10. For a mixture with a higher solid loading (e.g., 85wt% or higher), a rpm of 5 to 10 may be particularly helpful to prevent edge defects. In another example, the rpm of the screw may be at least 1, which may help avoid deformation of the extruded product, such as at least 10, at least 20, at least 30, at least 50, at least 70, at least 90, at least 100, at least 110, or at least 130. Deformation may include bulging, warp, or other misshapes. Moreover, the process 500 may include a screw rpm in a range including any of the minimum and maximum values noted herein.

[0066] In another embodiment, the extruder may include a conveyor, wherein the belt speed may be controlled to facilitate improved formation of the structure. In a further embodiment, the belt speed may be controlled to match the extrusion speed. In a particular embodiment, the belt speed may include any of the rpms noted with respect to the screw rpm in embodiments herein. In a further embodiment, the extruded structure may be shaped to form the finally formed structure. In an example, a roller may be used after extrusion to shape the structure, including compressing, flattening, making the tape more uniform.

[0067] In a further embodiment, the process 500 may include running the extruded materials through the barrel in the manner as discussed in embodiments herein, which may help improve uniformity of the finally formed structure.

[0068] In a further embodiment, compounding and / or extrusion may be performed at a temperature that may be at least the melting temperature of the organic material. For example, the compounding and / or extrusion temperature may be greater than the melting temperature of the coupling agent and / or the plasticizer if present. In a further example, the compounding and / or extrusion temperature may be at least the melting temperature of the binder material. In a further embodiment, the compounding and / or extrusion temperature may be greater than the melting temperature of the binder material.

[0069] In a particular embodiment, compounding and / or extrusion may be performed at a particular temperature of at least 120 °C, such as at least 140 °C, at least 150 °C, at least 160 °C, or at least 180 °C. Alternatively or additionally, compounding and / or extrusion may be performed at a temperature of such as less than 300 °C, at most 280 °C, at most 280 °C, at most 250 °C, at most 230 °C, at most 210 °C, at most 200 °C or below 200 °C. In certain examples, compounding and / or extrusion may be performed at a temperature of at most 190 °C, at most 180 °C, at most 170 °C, at most 160 °C, or at most 150 °C. Moreover, compounding and / or extrusion may be performed at a temperature in a range including any of the minimum and maximum values noted herein. In an example, the compounding and / or extrusion temperature may be in a range including at least 120 °C and at most 250 °C, such as in a range including at least 130 °C and at most 210 °C or in a range including at least 140 °C and at most 170 °C or in a range including at least 160 °C and at most 200 °C. In another particular embodiment, compounding and / or extrusion may be performed at a particular barrel temperature. In a further embodiment, the barrel temperature may include any of the minimum and / or maximum compounding and / or extrusion temperatures noted herein.

[0070] In a particular embodiment, the process 500 may be performed in a dry environment to facilitate improved formation of the structure. For example, certain solid electrolyte materials may be hygroscopic, and using a dry environment may help reduce degradation of the materials. In an example, dry environment may include H2O content <1 ppm. In another example, the process 500 may be performed in a glove box.

[0071] In a particular embodiment, the process 500 may be a dry process and particularly suited for forming the structure including the halide-based solid electrolyte material. As the halide-based materials are more prone to humidity compared to sulfide-based materials or other hygroscopic electrolyte materials (e.g., hydroxyl halides) and to decomposition due to moistures trapped in organic materials or environment. In a particular example, the process 500 may include using a strictly-controlled dry environment (i.e., H2O content <0.01 ppm) that may further help prevent degradation of the halide-based material.

[0072] In an embodiment, the structure may include particles having a particular maximum particle size that may facilitate improved performance and / or property of the structure. In an example, the maximum particle size may be at least 0.5 pm, such as at least 1 pm, at least 2 pm, at least 3 pm, at least 5 pm, at least 8 pm, at least 10 pm, or at least 12 pm. In another example, the maximum particle size may be at most 20 pm, such as at most 18 pm, at most 15 pm, at most 13 pm, at most 11 pm, at most 8 pm, or at most 5 pm. Moreover, the structure may include particles having a particular maximum particle size in a range including any of the minimum and maximum values noted herein.

[0073] In an embodiment, the structure may include particles having a particular minimum particle size that may facilitate improved performance and / or property of the structure. For example, the structures may include particles having a minimum particle size of at least 100 nm, such as at least 200 nm, at least 300 nm, at least 400 nm, at least 500 nm, at least 600 nm, at least 700 nm, at least 800 nm, at least 900 nm, or at least 1 pm. In another example, the minimum particle size may be at most 5 pm, at most 4 pm, at most 3 pm, at most 2 pm, at most 1 pm, at most 800 nm, or at most 600 nm. Moreover, the structure may include particles having a particular minimum particle size in a range including any of the minimum and maximum values noted herein.

[0074] In an embodiment, the structure may include particles having a particular average particle size that may facilitate improved performance and / or property of the structure. In an embodiment, the average particle size may be at least 100 nm, such as at least 200 nm, at least 300 nm, at least 400 nm, at least 500 nm, at least 600 nm, at least 700 nm, at least 800 nm, at least 900 nm, or at least 1 pm. In another example, the average particle size may be at most 10 pm, at most 9 pm, at most 8 pm, at most 7 pm, at most 6 pm, at most 5 pm, at most 4 pm, at most 3 pm, at most 2 pm, or at most 1 pm. Moreover, the particles may have the average particle size in a range including any of the minimum and maximum values noted herein.

[0075] In an embodiment, the structure may include particles having a bimodal particle size distribution including fine particles and coarse particles having particular particle sizes that may facilitate improved formation and / or performance and / or property of the structure. In a further embodiment, fine particles may have an average particle size of at most 2 pm, such as at most 1.5 pm, at most 1 pm, at most 800 nm, at most 600 nm, at most 500 nm, at most 400 nm, at most 300 nm, at most 200 nm, at most 100 nm, or at most 800 nm. Alternatively or additionally, fine particles may have an average particle size of at least 100 nm, at least 200 nm, at least 300 nm, at least 400 nm, at least 500 nm, at least 600 nm, at least 700 nm, at least 800 nm, at least 900 nm, or at least 1 pm. Moreover, fine particles may have an average particle size in a range including any of the minimum and maximum values noted herein.

[0076] In a further embodiment, the structure may include a particular content of fine particles that may facilitate improved performance and / or property of the structure. In an example, the structure may include at most 30% of fine particles for a total amount of particles by volume, such as at most 25%, at most 20%, at most 15%, or at most 10% for the total amount of the particles. In another example, the structure may include at least 2% of fine particles for the total amount of the particles, such as at least 4%, at least 6%, at least 5%, at least 9%, at least 11%, at least 15%, at least 17%, or at least 20% of fine particles for the total amount of the particles. Moreover, the content of the fine particles may be in a range including any of the minimum and maximum percentages noted herein. The total amount of the particles may be in reference to the total number of particles or a total vol% of the particles in the structure.

[0077] In another embodiment, coarse particles may have an average particle size of at most 20 pm, at most 15 pm, at most 13 pm, at most 11 pm, at most 8 pm, or at most 5 pm. Alternatively or additionally, coarse particles may have an average particle size of at least 400 nm, at least 500 nm, at least 600 nm, at least 700 nm, at least 800 nm, at least 900 nm, at least 1 pm, or at least 2 pm. Moreover, the structure may include coarse particles having the average particle size in a range including any of the minimum and maximum values noted herein.

[0078] In a further embodiment, the structure may include a particular content of coarse particles that may facilitate improved performance and / or property of the structure. In an example, the structure may include at most 80% of coarse particles for a total amount of particles by volume, such as at most 70%, at most 60%, at most 50%, or at most 40% for the total amount of the particles. In another example, the structure may include at least 20% of coarse particles for the total amount of the particles, such as at least 30%, at least 35%, at least 40%, at least 45%, at least 50%, at least 60%, at least 85%, or at least 70% of coarse particles for the total amount of the particles. Moreover, the content of the coarse particles may be in a range including any of the minimum and maximum percentages noted herein. The total amount of the particles may be in reference to the total number of particles or a total vol% of the particles in the structure. In another embodiment, the structure may include up to 90%, up to 95%, or up to 98% of coarse particles for a total amount of particles by volume. In a particular embodiment, the structure may consist essentially of coarse particles.

[0079] In an embodiment, the structure may include a thickness, t (illustrated in FIG. 4), of at least 0.1 pm, at least 1 pm, at least 5 pm, at least 6 pm, at least 7 pm, at least 8 pm, at least 9 pm, at least 10 pm, at least 12 pm, at least 14 pm, at least 17 pm, or at least 20 pm. Alternatively or additionally, the structure may include a thickness of at most 500 pm, at most 400 pm, at most 200 pm, at most 100 pm, at most 80 pm, at most 60 pm, at most 40 pm, at most 30 pm, at most 20 pm, at most 10 pm, or at most 8 pm. Moreover, the thickness may be in a range including any of the minimum and maximum percentages noted herein.

[0080] In an embodiment, the structure may include a particular porosity, such as a porosity of at most 20 vol% for a total volume of the structure, at most 15 vol%, at most 10 vol%, at most 9 vol%, at most 8 vol%, at most 7 vol%, at most 6 vol%, at most 5 vol%, at most 4 vol%, at most 3 vol%, at most 2 vol%, or at most 1 vol% of porosity for the total volume of the structure. Alternatively or additionally, the structure may include a porosity of at least 0.05 vol%, at least 0.1 vol%, at least 0.5 vol%, or at least 1 vol% for the total volume of the structure. Moreover, the porosity may be in a range including any of the minimum and maximum percentages noted herein.

[0081] In an embodiment, the structure may have improved ionic conductivity. In another embodiment, the structure may have ionic conductivity of at least 0.02 mS / cm, such as at least 0.03 mS / cm, at least 0.04 mS / cm, at least 0.05 mS / cm, at least 0.06 mS / cm, at least 0.07 mS / cm, at least 0.08 mS / cm, at least 0.09 mS / cm, or at least 0.10 mS / cm, at least 0.11 mS / cm, at least 0.12 mS / cm, at least 0.13 mS / cm, at least 0.14 mS / cm, at least 0.16 mS / cm, at least 0.20 mS / cm, at least 0.30 mS / cm, at least 0.40 mS / cm, at least 0.50 mS / cm, at least 0.60 mS / cm, at least 0.70 mS / cm, at least 0.80 mS / cm, at least 0.90 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 ionic conductivity of at most 10 mS / cm, at most 8 mS / cm, at most 6 mS / cm, at most 5 mS / cm, at most 4 mS / cm, at most 3 mS / cm, at most 2 mS / cm, at most 1.5 mS / cm, at most 1 mS / cm, at most 0.8 mS / cm, at most 0.7 mS / cm, at most 0.5 mS / cm, at most 0.4 mS / cm, at most 0.25 mS / cm, at most 0.22 mS / cm, at most 0.20 mS / cm, at most 0.19 mS / cm, at most 0.18 mS / cm, at most 0.17 mS / cm, at most 0.16 mS / cm, or at most 0.15 mS / cm. Moreover, the structure may have ionic conductivity in a range including any of the minimum and maximum values noted herein. In this disclosure ionic conductivity can be measured at room temperature (i.e., 20-25 °C) and at activation energy in the range of 0.2 eV and 0.5 eV. In an embodiment, the structure may be an electrolyte, a separator, or both. In a particular example, the structure may be a solid-state electrolyte, a solid-state separator, or both.

[0082] In an embodiment, an electrochemical device may include the structure. An exemplary electrochemical device may include a battery. A particular example may include, a solid state battery, such as an all solid state lithium battery, an all solid state Li / Na battery, or like, 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 any or both of the cathode and anode. In a particular embodiment, an electrochemical device may include the structure abutting an anode. For example, the structure may be in direct contact with an anode that may include lithium, indium, aluminum, or any combination thereof. In a further embodiment, the structure may serve as an electrolyte, separator, or both.

[0083] Referring to FIG. 5, a multilayer structure 400 is illustrated including the structure 406 between layers 402 and 404. In a particular example, the structure 406 may be electrolyte or separator including any features described in embodiments herein. One of the layers 402 or 404 may be an anode. In a particular example, the anode may include one or more metals including lithium, and more particularly, the electrolyte material, polymeric fibers, or both may be in direct contact with the anode.

[0084] In another embodiment, the structure may include an electron conductive material, such as comprising a conductive additive, an active electrode material, or a combination thereof. An exemplary electrode material may include an anode active material or a cathode active material. In an example, the anode active material may include lithium, indium, aluminum, or any combination thereof. In a particular example, the anode active material may include one or more metals including lithium. In another example, the cathode material may include lithium-containing oxide, transition metal fluorides, polyanion materials, fluorinated polyanion materials, transition metal sulfides, transition metal oxyfluorides, transition metal oxysulfides, transition metal oxynitrides, or any combination thereof. Particular exemplary cathode material may include LiCoCh, LiFePC , Li(NiCoAl)O2, LiCoCh, LiMnPCU, LiMn2O4, LiNii / sCoi / sM / sCh, NMC622, NMC 811, another NMC, or the like, or any combination thereof.

[0085] In an embodiment, the structure may have improved thickness variation, uniformity, or any combination thereof.

[0086] Many different aspects and embodiments are possible. Some of those aspects and embodiments are described herein. After reading this specification, skilled artisans will appreciate that those aspects and embodiments are only illustrative and do not limit the scope of the present invention. Embodiments may be in accordance with any one or more of the embodiments as listed below.

[0087] EMBODIMENTS

[0088] Embodiment 1. A structure, comprising particles of a solid electrolyte material attached to polymeric fibers, wherein the structure comprises a fiber concentration of the polymeric fibers of at least 0.15 / pm2.

[0089] Embodiment 2. A structure, comprising particles of a solid electrolyte material attached to polymeric fibers, wherein the polymeric fibers comprise a polymer having a Melt Flow Rate of greater than 10 g / 10 min.

[0090] Embodiment 3. A structure, comprising particles of a solid electrolyte material attached to polymeric fibers, wherein the polymeric fibers comprise high density polyethylene (HDPE), low density polyethylene (LDPE), polypropylene (PP), or a combination.

[0091] Embodiment 4. The structure of any one of embodiments 1 to 3, comprising polymeric fibers having an aspect ratio of maximum width to length of at most 0.2 and a fiber concentration of at least 0.15 / pm2, at least 0.18 / pm2, at least 0.20 / pm2, at least 0.22 / pm2, at least 0.25 / pm2, at least 0.30 / pm2, at least 0.33 / pm2, at least 0.35 / pm2, at least 0.38 / pm2, at least 0.40 / pm2, at least 0.45 / pm2, at least 0.50 / pm2, at least 0.55 / pm2, at least 0.60 / pm2, at least 0.62 / pm2, at least 0.65 / pm2, at least 0.70 / pm2, at least 0.73 / pm2, at least 0.75 / pm2, at least 0.78 / pm2, at least 0.80 / pm2, or at least 0.82 / pm2.

[0092] Embodiment 5. The structure of any one of embodiments 1 to 4, wherein the polymeric fibers comprise a polymer comprising a melt flow Rate of greater than 10 g / 10 min, at least 20 g / 10 min, at least 30 g / 10 min, or at least 40 g / 10 min; and / or wherein the melt flow rate is at most 200 g / 10 min, at most 180 g / 10 min, at most 150 g / 10 min, at most 130 g / 10 min, at most 120 g / 10 min, at most 100 g / 10 min, at most 90 g / 10 min, at most 80 g / 10 min, at most 70 g / 10 min, at most 55 g / 10 min, or at most 50 g / 10 min.

[0093] Embodiment 6. The structure of any one of embodiments 1 to 5, wherein the polymeric fibers comprise a polymer having a melt temperature less than 300 degrees and greater than 100 degrees.

[0094] Embodiment 7. The structure of any one of embodiments 1 to 6, wherein the polymeric fibers comprise a polymer having an elongation at break from 10 - 1000 %.

[0095] Embodiment 8. The structure of any one of embodiments 1 to 7, comprising at least 55 vol% of the particles for a total volume of the structure, at least 60 vol%, at least 63 vol%, at least 68 vol%, at least 50 vol%, at least 72 vol%, at least 75 vol%, or at least 78 vol% for the total volume of the structure; and / or at most 98 vol% of the particles for the total volume of the structure, at most 95 vol%, at most 93 vol%, at most 91 vol%, at most 89 vol%, at most 86 vol%, at most 83 vol%, at most 80 vol%, at most 76 vol%, at most 73 vol%, at most 70 vol%, at most 67 vol%, at most 65 vol%, at most 62 vol%, at most 60 vol%, at most 58 vol%, at most 55 vol%, at most 53 vol%, or at most 51 vol% for the total volume of the structure.

[0096] Embodiment 9. The structure of any one of embodiments 1 to 8, wherein a majority of the particles are in contact with one another, wherein greater than 50%, at least 55%, at least 60%, at least 70%, at least 80%, at least 90%, or at least 95% of the particles are in contact with one another.

[0097] Embodiment 10. The structure of any one of embodiments 1 to 9, wherein the structure comprises at least 55 vol% of the solid electrolyte material for the total volume of the structure, at least 60 vol%, at least 63 vol%, at least 68 vol%, at least 50 vol%, at least 72 vol%, at least 75 vol%, or at least 78 vol% for the total volume of the structure; and / or wherein the structure comprises at most 98 vol% of the solid electrolyte material for the total volume of the structure, at most 97 vol%, at most 95 vol%, at most 93 vol%, at most 91 vol%, at most 89 vol%, at most 86 vol%, at most 83 vol%, at most 80 vol%, at most 76 vol%, at most 73 vol%, at most 70 vol%, at most 67 vol%, at most 65 vol%, at most 62 vol%, at most 60 vol%, at most 58 vol%, at most 55 vol%, at most 53 vol%, or at most 51 vol% of the solid electrolyte material for the total volume of the structure.

[0098] Embodiment 11. The structure of any one of embodiments 1 to 10, wherein the polymeric fibers comprise high density polyethylene (HDPE), polypropylene (PP), or both, wherein the polymeric fibers comprise high density polyethylene (HDPE).

[0099] Embodiment 12. The structure of any one of embodiments 1 to 11, further comprising animal waxes, plant waxes, petroleum waxes, derivatives thereof, or combination thereof, wherein the structure comprises ozokerite wax, paraffin wax, or any combination thereof, wherein the polymeric fibers comprise ozokerite wax, paraffin wax, or any combination thereof.

[0100] Embodiment 13. The structure of any one of embodiments 1 to 12, wherein the particles comprise a maximum particle size of at least 0.5 pm and not greater than 20 pm, a minimum particle size of at least 100 nm and not greater than 5 pm, or a combination thereof; and / or wherein the particles comprise an average particle size of at least 0.1 pm and not greater than 10 pm.

[0101] Embodiment 14. The structure of any one of embodiments 1 to 13, wherein the particles comprise a bimodal particle size distribution including at most 20% of particles by volume of particle phase having a particle size less than 2 pm. Embodiment 15. The structure of any one of embodiments 1 to 14, wherein the particles comprise a hygroscopic material; wherein the solid electrolyte material ; comprise a halide-based material represented by formula M3- g(Mek+)fX3- s+k*f, wherein -3< 5<3, 0<f<l, k is the valence of Me, 2<k<6, M includes Li, Me includes a metal element that is different from M, and X includes a halogen, wherein the halide-based material includes at least two metal elements.

[0102] Embodiment 16. The structure of embodiment 15, wherein Me includes Y, In, Sn, Fe, a rare earth element, Bi, Zr, Ti, Hf, Sb, an alkaline earth metal element, or any combination thereof.

[0103] Embodiment 17. The structure of any one of embodiments 1 to 16, wherein the particles comprise a sulfide-based material, an oxyhalide, a halide hydroxide, an oxide, or any combination thereof.

[0104] Embodiment 18. The structure of any one of embodiments 1 to 17, comprising a thickness of at least 0.1 pm, at least 1 pm, at least 5 pm, at least 6 pm, at least 7 pm, at least 8 pm, at least 9 pm, at least 10 pm, at least 12 pm, at least 14 pm, at least 17 pm, or at least 20 pm.

[0105] Embodiment 19. The structure of any one of embodiments 1 to 18, comprising a thickness of at most 500 pm, at most 400 pm, at most 200 pm, at most 100 pm, at most 80 pm, at most 60 pm, at most 40 pm, at most 30 pm, at most 20 pm, at most 10 pm, or at most 8 pm.

[0106] Embodiment 20. The structure of any one of embodiments 1 to 19, comprising a porosity of at most 20 vol% for a total volume of the structure, at most 15 vol%, at most 10 vol%, at most 9 vol%, at most 8 vol%, at most 7 vol%, at most 6 vol%, at most 5 vol%, at most 4 vol%, at most 3 vol%, at most 2 vol%, or at most 1 vol% of porosity for the total volume of the structure.

[0107] Embodiment 21. The structure of any one of embodiments 1 to 20, comprising a porosity of at least 0.05 vol%, at least 0.1 vol%, at least 0.5 vol%, or at least 1 vol% for the total volume of the structure.

[0108] Embodiment 22. The structure of any one of embodiments 1 to 21, wherein the polymeric fibers are free of an elastomer.

[0109] Embodiment 23. The structure of any one of embodiments 1 to 22, wherein the structure is free of a solvent.

[0110] Embodiment 24. The structure of any one of embodiments 1 to 23, comprising ionic conductivity of at least 0.02 mS / cm, such as at least 0.03 mS / cm, at least 0.04 mS / cm, at least 0.05 mS / cm, at least 0.06 mS / cm, at least 0.07 mS / cm, at least 0.08 mS / cm, at least 0.09 mS / cm, or at least 0.10 mS / cm, at least 0.11 mS / cm, at least 0.12 mS / cm, at least 0.13 mS / cm, at least 0.14 mS / cm, at least 0.16 mS / cm, at least 0.20 mS / cm, at least 0.30 mS / cm, at least 0.40 mS / cm, at least 0.50 mS / cm, at least 0.60 mS / cm, at least 0.70 mS / cm, at least 0.80 mS / cm, at least 0.90 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.

[0111] Embodiment 25. The structure of any one of embodiments 1 to 24, comprising ion conductivity of at most 10 mS / cm, at most 8 mS / cm, at most 6 mS / cm, at most 5 mS / cm, at most 4 mS / cm, at most 3 mS / cm, at most 2 mS / cm, at most 1.5 mS / cm, at most 1 mS / cm, at most 0.8 mS / cm, at most 0.7 mS / cm, at most 0.5 mS / cm, at most 0.4 mS / cm, at most 0.25 mS / cm, at most 0.22 mS / cm, at most 0.20 mS / cm, at most 0.19 mS / cm, at most 0.18 mS / cm, at most 0.17 mS / cm, at most 0.16 mS / cm, or at most 0.15 mS / cm.

[0112] Embodiment 26. The structure of any one of embodiments 1 to 25, wherein: the polymeric fibers have a random orientation; at least a majority of the polymeric fibers extend in directions that intersect; lengths of the polymeric fibers form angles with respect to a thickness direction of the structure, wherein the angles comprise acute angles, obtuse angles, or any combination thereof; or any combination thereof.

[0113] Embodiment 27. The structure of any one of embodiments 1 to 26, wherein the polymeric fibers form a 3 -dimensional fibrous structure.

[0114] Embodiment 28. The structure of any one of embodiments 1 to 27, wherein the polymeric fibers are connected thereby extending 3 -dimensionally throughout at least a portion of a volume of the structure.

[0115] Embodiment 29. The structure of any one of embodiments 1 to 28, wherein a majority, at least 60%, at least 70%, at least 80%, or at least 90% of the polymeric fibers have an aspect ratio of maximum width to length of at most 0.2; or wherein essentially all of the polymeric fibers have an aspect ratio of maximum width to length of at most 0.2.

[0116] Embodiment 30. The structure of any one of embodiments 1 to 29, comprising a total content of an organic material of less than 50 vol%, not greater than 45 vol%, not greater than 40 vol%, not greater than 35 vol%, not greater than 30 vol%, not greater 28 vol%, not greater than 25 vol%, not greater than 22 vol%, not greater than 20 vol%, not greater than 17 vol%, not greater than 14 vol%, not greater than 11 vol%, not greater than 8 vol%, not greater than 5 vol%, or not greater than 3 vol% for a total volume of the structure; and / or the total content of the organic material of at least 2 vol% for the total volume of the structure, at least 3 vol%, at least 5 vol%, at least 8 vol%, at least 10 vol%, at least 12 vol%, at least 15 vol%, at least 18 vol%, at least 20 vol%, at least 25 vol%, at least 30 vol%, at least 35 vol%, at least 38 vol%, at least 40 vol%, at least 45 vol%, or at least 49 vol% for the total volume of the structure.

[0117] Embodiment 31. The structure of any one of embodiments 1 to 30, wherein the polymeric fibers comprise a majority of the total content of the organic materials, at least 55 vol%, at least 60 vol%, at least 70 vol%, at least 80 vol%, at least 90 vol%, or at least 95 vol% of the total content of the organic material; or wherein the polymeric fibers comprise essentially all of the total content of the organic material, at most 99 vol% of the total content of the organic material, such as at most 97 vol%, at most 95 vol%, at most 92 vol%, at most 90 vol%, at most 86 vol%, at most 84 vol%, at most 82 vol%, at most 80 vol%, at most 75 vol%, at most 73 vol%, at most 70 vol%, at most 65 vol%, at most 63 vol%, at most 60 vol%, or at most 58 vol% of the total content of the organic material.

[0118] Embodiment 32. The structure of any one of embodiments 1 to 31, wherein the polymeric fibers comprises a polymer, wherein the polymer is in a content of less than 50 vol%, not greater than 45 vol%, not greater than 40 vol%, not greater than 35 vol%, not greater than 30 vol%, not greater 28 vol%, or not greater than 25 vol% for a total volume of the structure.

[0119] Embodiment 33. The structure of any one of embodiments 1 to 32, wherein the structure is in a form of a tape, a sheet, a block, a film, a disc, or any combination thereof.

[0120] Embodiment 34. The structure of any one of embodiments 1 to 33, wherein the structure is free-standing, a single-layer structure, or both.

[0121] Embodiment 35. The structure of any one of embodiments 1 to 34, further comprising an electron conductive material comprising a conductive additive, an anode active material, or a combination thereof.

[0122] Embodiment 36. The structure of any one of embodiments 1 to 34, further comprising an electronic conductive material comprising a conductive additive, a cathode active material, or a combination thereof.

[0123] Embodiment 37. A multilayer structure, comprising an anode in direct contact with the structure of any one of embodiments 1 to 34.

[0124] Embodiment 38. An electrolyte, comprising the structure of any one of embodiments 1 to 34. Embodiment 39. A separator, comprising the structure of any one of embodiments 1 to 34.

[0125] EXAMPLES

[0126] Example 1

[0127] A representative sample S 1 is formed using a tabletop compounder / extruder that is put inside the glove box. A die having the thickness of 0.3 mm is used. A mixture of LisYBri^CL.s powder, high density polyethylene (having the MFR of 35.7 g / lOmin under load of 2.16kg at 180 °C) and ozokerite wax is made including 86 wt% of the halide for the total of the halide and the organic materials. The weight content ratio of HDPE to ozokerite wax is 1 : 1. The blend of HDPE and ozokerite wax has a MFR greater than 90 g / lOmin at 150 °C. The mixture is added in 5-6 batches each including 4g of the halide, compounded, and extruded. The screws are set to an rpm of 20. The timing to add the subsequent batch is 1 to 1.5 minutes during which the torque reading increases from ~2 Nm up to 8 Nm and starts to decrease again. Care should be taken so that when adding the materials into the barrel an rpm of less than 20 is used to avoid poor mixing of the organic materials and the halide. The rpm is controlled to not reach 200-300 during extrusion to avoid incorporation of gas bubbles within the tape. When extruding, the belt speed is matched with the extrusion speed that is at a low rpm of 5-10, which helps prevent edge defects. The tape is then fed onto the conveyor to cool.

[0128] The process for forming SI is repeated with changes noted below. When adding the same mixture of SI in batches, a second batch is added into the funnel feeding onto the screws when rpm is above 20. It is observed HDPE pellets pop out of the funnel.

[0129] The process for forming SI is repeated with changes noted below. When adding the same mixture of SI in batches, the next batch is added before torque starts to decrease, which causes the torque to max out and the screws stop moving. Additional attempts to restart the screws maxes out the torque. The barrel is disassembled to clear the blockage completely.

[0130] The process for forming SI is repeated with changes noted below. The first batch including 4g of the halide powder is fed to the extruder. The rpm is kept at 20 and the batch is allowed to reach the die without adding a further batch. The batch is not extruded because there is not enough back pressure to push it through the die.

[0131] The process for forming SI is repeated with changes noted below. The first batch including 4g of the halide powder is fed to the extruder. The screw rpm is set to 20 and the batch is allowed to travel through the entire barrel. When some materials are observed to approach but before going through the die the second batch is added. It is observed addition at this point is too late, as it appears that the second batch does not apply enough pressure to extrude out the first batch. Materials build up and densify behind the die, and thus are able to come out of the die. The die is taken off and material removed before continuing.

[0132] In this disclosure, halide-based materials having different halogens, metal elements, and / or molar ratios between halogens may be used and may be collectively referred by using constituents’ elements. For example, LisYBn^Cks may be referred to as LYBC, and LisYBre may be referred to as LYB.

[0133] Example 2

[0134] Organic materials are mixed with LYBC at the weight content ratio of 1 : 1, and XRD analysis is performed on the mixtures to determine electrolyte decomposition the halide- based materials. Organic materials are heated until their melting point and then mixed with the halide. Mixtures are pressed flat and cooled for XRD analysis. The organic material is considered compatible when minimum or no decomposition (Reactivity Value of at most 2%) was observed. Test data and certain characteristics of the organic materials are included in Table 1.

[0135] Table 1 Example 3

[0136] Separator tape Samples S5 to S8 are formed by extrusion. The same LYBC used to form SI is used to form tape Samples S5 to S8. Sample S5 is made using PS. Sample S6 is made using PP and ozokerite wax. The blend of PP and ozokerite wax has the MRF greater than 90 g / lOmin at 180 °C. Samples S7 and S8 are made using HDPE and ozokerite wax. The blend of HDPE and ozokerite wax has the MRF greater than 90 g / lOmin at 180 °C. Mixing and extrusion is performed following the method for forming SI as described in Example 1, except that different contents of LYBC and organic materials are used. The weight content ratios of each binder to Ozokerite wax is kept at 1 : 1. Ozokerite wax is not used for forming Sample S5 due to the extrusion temperature being above the decomposition temperature of the wax. The content (vol%) of the solid electrolyte material for the total volume of the tapes are noted in Table 2.

[0137] Coarse LYBC particles have the average particle size of 10 pm. Fine LYBC particles have the average particle size of 2 pm.

[0138] Table 2

[0139] PS as the binder material.

[0140] It can be observed Samples S7 and S8 have higher ionic conductivity compared to samples S5 and S6. At a lower solid loading, Sample S7 demonstrates improved ionic conductivity compared to samples S8.

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

[0142] PIB is pre-dissolved in a chemically compatible solvent material, toluene, 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 is performed on thin aluminum foil using a doctor blade. The tape is allowed to dry without heat. The composition and ionic conductivity of the tape is included in Table 4. Table 3

[0143] Table 4 conductivity to samples S8.

[0144] FIGs. 7A-7D include SEM images of Samples S8, S6, CIO, and S5, respectively.

[0145] Sample S8 includes fibers 602 and particles 604 attached to fibers 602 and one another. Sample S6 includes fibers 606 and particles 608 attached to fibers 606 and one another. Sample CIO includes particles 610 attached to one another, and fibers are not observed. Sample S5 includes particles 612 attached to the binder material 614, and fibers are not observed. It can be observed that Sample S8 has a higher fiber concentration than S6.

[0146] Example 4

[0147] Separator tape samples, S12 and SI 3, are formed using PP and HDPE as binders, respectively, following the method of forming Sample SI. Samples S12 and S13 have the same content of LYBC, 86 wt%, for the total weight of the tape and weight ratio of polymer to wax of 1 : 1. Fiber concentrations of the samples are analyzed as described in embodiments herein. Fiber concentrations of a group of 2 samples are analyzed for each type of binder. Concentrations of fibers having the aspect ratio of maximum width to length of at most 0.2 are illustrated in FIG. 8. Samples S13 have significantly higher fiber concentrations than Sample S12. Average ionic conductivity of the samples is included in Table 5 below. Samples S13 demonstrates improved ionic conductivity than Samples S12. Table 5

[0148] The foregoing embodiments represent a departure from the state-of-the-art. Embodiments are directed to a structure including particles including a solid electrolyte material attached to fibers including a polymer. The structure may have improved microstructures, such as fiber concentrations, fiber aspect ratios, or any combination thereof and / or properties including ionic conductivity, uniformity, flexibility, toughness, or a combination thereof. The structure may be formed utilizing a process that does not involve a solvent and carefully controlling certain parameters.

[0149] Benefits, other advantages, and solutions to problems have been described above with regard to specific embodiments. However, the benefits, advantages, solutions to problems, and any feature(s) that may cause any benefit, advantage, or solution to occur or become more pronounced are not to be construed as a critical, required, or essential feature of any or all the claims. Reference herein to a material including one or more components may be interpreted to include at least one embodiment wherein the material consists essentially of the one or more components identified. The term “consisting essentially” will be interpreted to include a composition including those materials identified and excluding all other materials except in minority contents (e.g., impurity contents), which do not significantly alter the properties of the material. Additionally, or in the alternative, in certain non -limiting embodiments, any of the compositions identified herein may be essentially free of materials that are not expressly disclosed. The embodiments herein include a range of contents for certain components within a material, and it will be appreciated that the contents of the components within a given material total 100%.

[0150] The specification and illustrations of the embodiments described herein are intended to provide a general understanding of the structure of the various embodiments. The specification and illustrations are not intended to serve as an exhaustive and comprehensive description of all of the elements and features of apparatus and systems that use the structures or methods described herein. Separate embodiments may also be provided in combination in a single embodiment, and conversely, various features that are, for brevity, described in the context of a single embodiment, may also be provided separately or in any subcombination. Further, reference to values stated in ranges includes each and every value within that range. Many other embodiments may be apparent to skilled artisans only after reading this specification. Other embodiments may be used and derived from the disclosure, such that a structural substitution, logical substitution, or another change may be made without departing from the scope of the disclosure. Accordingly, the disclosure is to be regarded as illustrative rather than restrictive.

Claims

WHAT IS CLAIMED IS:

1. A structure, comprising particles of a solid electrolyte material attached to polymeric fibers, wherein the structure comprises a fiber concentration of the polymeric fibers of at least 0.15 / pm2.

2. A structure, comprising particles of a solid electrolyte material attached to polymeric fibers, wherein the polymeric fibers comprise a polymer having a Melt Flow Rate of greater than 10 g / 10 min.

3. A structure, comprising particles of a solid electrolyte material attached to polymeric fibers, wherein the polymeric fibers comprise high density polyethylene (HDPE), low density polyethylene (LDPE), polypropylene (PP), or a combination.

4. The structure of any one of claims 1 to 3, comprising polymeric fibers having an aspect ratio of maximum width to length of at most 0.2.

5. The structure of claim 2 or 3, comprising a fiber concentration of the polymeric fibers of at least 0.15 / pm2.

6. The structure of claim 1 or 3, wherein the polymeric fibers comprise a polymer comprising a Melt Flow Rate of greater than 10 g / 10 min.

7. The structure of any one of claims 1 to 6, wherein the polymeric fibers comprise a polymer having a melt temperature less than 300 degrees and greater than 100 degrees.

8. The structure of any one of claims 1 to 7, wherein the structure comprises at least 55 vol% of the solid electrolyte material for the total volume of the structure.

9. The structure of claim 8, wherein majority of the particles of the solid electrolyte material are in contact with one another.

10. The structure of any one of claims 1 to 9, wherein the polymeric fibers comprise high density polyethylene (HDPE), polypropylene (PP), or both.

11. The structure of any one of claims 1 to 10, further comprising animal waxes, plant waxes, petroleum waxes, derivatives thereof, or combination thereof, wherein the structure comprises ozokerite wax, paraffin wax, or any combination thereof, wherein the polymeric fibers comprise ozokerite wax, paraffin wax, or any combination thereof.

12. The structure of any one of claims 1 to 11, wherein the particles comprise a maximum particle size of at least 0.5 pm and not greater than 20 pm, a minimum particle size of at least 100 nm and not greater than 5 pm, or a combination thereof.

13. The structure of any one of claims 1 to 12, wherein the particles comprise a bimodal particle size distribution.

14. The structure of any one of claims 1 to 13, wherein the particles comprise a hygroscopic material; wherein the solid electrolyte material ; comprise a halide-based material represented by formula M3- g(Mek+)fX3- s+k*f, wherein -3< 5<3, 0<f<l, k is the valence of Me, 2<k<6, M includes Li, Me includes a metal element that is different from M, and X includes a halogen, wherein the halide-based material includes at least two metal elements.

15. The structure of any one of claims 1 to 14, wherein: the polymeric fibers have a random orientation; at least a majority of the polymeric fibers extend in directions that intersect; lengths of the polymeric fibers form angles with respect to a thickness direction of the structure, wherein the angles comprise acute angles, obtuse angles, or any combination thereof; or any combination thereof.

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