CALENDAR-PROCESSED CATHODE COMPOSITION AND METHOD FOR MANUFACTURING SAME - Patent application

Abstract

Provided herein are compositions and methods for calendaring cathode materials for lithium battery construction.

Description

[Technical field]

[0001] CROSS-REFERENCE TO RELATED APPLICATIONS

[0001] This application claims the benefit of U.S. Provisional Patent Application Nos. 63 / 483,238, filed February 3, 2023, 63 / 521,297, filed June 15, 2023, and 63 / 546,173, filed October 27, 2023, which are incorporated by reference in their entireties for all purposes.

[0002] Field SUMMARY OF THE DISCLOSURE

[0002] Provided herein are compositions and methods for calendaring materials such as, but not limited to, cathode electrodes for lithium battery construction. [Background technology]

[0003] background

[0003] Currently, there is an unmet need in the field of rechargeable lithium batteries for better methods of calendering materials for manufacturing electrodes (e.g., cathodes). Calendering is a common method to tailor the surface properties of a material, such as its smoothness, and its porosity and / or density. Because cathode materials and their current collectors have different physical properties, calendering, which may also involve the application of heat and pressure, can cause edge defects in the product that make it unsuitable for use in electrodes.

[0004]

[0004] Thus, there is a continuing need for improved methods of calendering that can reduce or eliminate the amount of edge defects in bilayer compositions (eg, cathodes and their current collectors).

[0005]

[0005] Presented herein is a solution to this problem and other problems in the related art. Summary of the Invention [Means for solving the problem]

[0006] overview

[0006] In this specification, for example, lithium ion (Li + Provided are bilayer compositions and methods for making the bilayer compositions having superior properties that are useful as cathodes (i.e., positive electrodes) in rechargeable lithium batteries for reversibly storing lithium ions.

[0007]

[0007] In one aspect, the present specification provides a metal substrate having at least two longitudinal ends and at least two lateral ends; a cathode material disposed on a metal substrate; A bilayer comprising: the cathode material covers at least about 50% of the surface of the metal substrate but not the longitudinal ends; A bilayer is provided.

[0008]

[0008] In one aspect, the present specification provides a metal substrate having at least two longitudinal ends and at least two lateral ends; a cathode material disposed on a metal substrate; A bilayer comprising: the cathode material covers at least about 50% of the surface of the metal substrate but not the longitudinal ends; the longitudinal end includes one or more cuts extending from the longitudinal end to the cathode material; A bilayer is provided.

[0009] In certain embodiments, the bilayer cathode material is disposed on the metal substrate as two lanes (eg, two continuous or discontinuous cathode material lanes parallel to the longitudinal edges).

[0010] In certain embodiments, the bilayer cathode material is arranged in three lanes on the metal substrate (e.g., two wide outer cathode material lanes and a narrow central cathode material lane, each parallel to a longitudinal edge). In certain embodiments, the bilayer cathode material is arranged in four or more lanes on the metal substrate.

[0011] In a second aspect, the present specification provides a method for producing a compound comprising the steps of: a metal substrate having at least two longitudinal ends and at least two lateral ends; a cathode material disposed on a metal substrate; A green bilayer comprising: the cathode material covers at least about 50% of the surface of the metal substrate but not the longitudinal ends; the longitudinal end includes one or more cuts extending from the longitudinal end to the cathode material; A green bilayer is provided.

[0012]

[0012] In certain embodiments taught elsewhere in this specification, the green bilayer includes at least three lanes of coating material disposed on a metal substrate, the first and second lanes of coating material including a cathode material.

[0013]

[0013] In certain embodiments, the cathode material of the green bilayer is disposed on the metal substrate in two lanes as otherwise disclosed herein. In certain embodiments, the cathode material of the green bilayer is disposed on the metal substrate in three lanes as otherwise disclosed herein. In certain embodiments, the cathode material of the green bilayer is disposed on the metal substrate in four or more lanes as otherwise disclosed herein.

[0014] In a third aspect, the present specification provides a method for producing a compound comprising the steps of: a metal substrate having at least two longitudinal ends and at least two lateral ends; a cathode material disposed on a metal substrate; Providing a green bilayer comprising: the cathode material covers at least about 50% of the surface of the metal substrate but not the longitudinal ends; the longitudinal end including one or more cuts extending from the longitudinal end to a cathode material disposed on the metal substrate; and calendering the green bilayer; A method for manufacturing a cathode is provided, comprising:

[0015] In a fourth aspect, the present specification provides a method for producing a compound comprising the steps of: coating a metal substrate with a cathode slurry to provide a green bilayer comprising a cathode material disposed on the metal substrate; the metal substrate having at least two longitudinal edges and at least two lateral edges; the cathode material covers at least about 50% of the surface of the metal substrate but not the longitudinal ends; calendering the green bilayer; and die punching the green bilaminate to produce a cathode; A method for manufacturing a cathode is provided, comprising:

[0016] In certain embodiments, the method further includes creating a green bilayer using a laser pattern for subsequent die punch processing.

[0017]

[0017] In certain embodiments, the method further includes cutting the metal substrate, the cuts including one or more cuts at a longitudinal end, the one or more cuts extending from the longitudinal end to the cathode material disposed on the metal substrate.

[0018] In certain embodiments, the calendaring of the green bilayer occurs at a temperature less than 100° C. In certain embodiments, the green bilayer is calendared at a temperature less than 75° C. In certain embodiments, the green bilayer is calendared at a temperature less than 50° C. In certain embodiments, the green bilayer is calendared at a temperature between 30° C. and 100° C., between 40° C. and 90° C., or between 50° C. and 75° C.

[0019] In a fifth aspect, the present specification provides a method for producing a compound comprising the steps of: a metal substrate having at least two longitudinal ends and at least two lateral ends; at least three lanes of coating material disposed on the metal substrate; A green bilayer comprising: the first and second lanes of coating material include a cathodic material; the coating material covers at least about 50% of the surface of the metal substrate but does not cover the longitudinal edges; the longitudinal end includes one or more cuts extending from the longitudinal end toward the coating material; A green bilayer is provided.

[0020]

[0020] In a sixth aspect, there is provided a metal foil having two longitudinal ends and two transverse ends, coated with a coating material, wherein the coating material does not coat the longitudinal ends and the coating material is separated by parallel or nearly parallel exposed metal foil, and the longitudinal ends include one or more cuts extending from the longitudinal ends towards the coating material.

[0021]

[0021] These and other aspects and embodiments are described by the present invention. [Brief description of the drawings]

[0022] BRIEF DESCRIPTION OF THE DRAWINGS [Figure 1A]

[0022] One of several exemplary cathode comparisons showing a continuous cathode. [Figure 1B]

[0022] One of several exemplary cathode comparisons shows the calendering of FIG. 1A. [Figure 1C]

[0022] One of several exemplary cathode comparisons showing an intermittent (ie, patch coated) cathode. [Figure 1D]

[0022] A comparison of several exemplary cathodes, one of which shows the calendering of FIG. 1C. [Figure 1E]

[0022] One of several exemplary cathode comparisons showing a continuous cathode with tab cuts. [Figure 1F]

[0022] One of several exemplary cathode comparisons shows the calendering of FIG. 1E. [Figure 2A]

[0023] FIG. 1 is a diagram of a standard calendering process to 25% volume porosity (excluding active material porosity). [Figure 2B]

[0023] Photograph of a calendered cathode with noticeable wrinkles and edge defects. [Diagram 3]

[0024] FIG. 1 is a flow diagram of an exemplary calendering process having cathode slits and cut gaps at the longitudinal ends. [Figure 4]

[0025] FIG. 13 illustrates the effect of tab configuration on the amount of wrinkles and burrs. [Figure 5A]

[0026] This is one of several embodiments of different cut patterns, showing a pattern that is a slit (or shape) running the entire length on both sides. [Figure 5B]

[0026] This is one of several embodiments of different cut patterns, where the shapes (or slits) on both sides are different. [Figure 5C]

[0026] This is one of several embodiments of different cut patterns, where the shapes (or slits) on both sides are different. [Figure 5D]

[0026] This is one of several embodiments of different cut patterns, with different slits on one side and different shapes on the other side. [Figure 6]

[0027] 1 shows an embodiment of a cathode without offset (left) and with offset (right). [Figure 7A]

[0028] FIG. 1 is an embodiment of the method of the present invention including laser notching (i.e., the center lane process) showing coating a foil to form a coated foil having two center lanes of uncoated foil. [Figure 7B]

[0028] FIG. 1 is an embodiment of the method of the present invention involving laser notching (ie, a center lane process), showing laser notching of the center lane of a coated foil. [Figure 7C]

[0028] An embodiment of the method of the present invention including laser notching (ie, the center lane process) and calendering the notched foil is shown. [Figure 7D]

[0028] FIG. 1 is an embodiment of the method of the present invention involving laser notching (ie, center lane process), showing a center cut (herein "cut") in the foil between the notched areas. [Figure 7E]

[0028] An embodiment of the method of the present invention including laser notching (ie, center lane process) is shown for die punch processing of a foil. [Figure 8A]

[0029] FIG. 2 is a second embodiment of the method of the present invention including laser notching (i.e., the end lane process) showing coating a foil to form a coated foil having two end lanes. [Figure 8B] FIG. 2 is a second embodiment of the method of the present invention involving laser notching (ie, the end lane process), showing laser notching of an end lane of a coated foil. [Figure 8C]

[0029] FIG. 2 is a second embodiment of the method of the present invention including laser notching (ie, the end lane process) and showing calendering of the notched foil. [Figure 8D]

[0029] FIG. 2 is a second embodiment of the method of the present invention involving laser notching (ie, the end lane process), showing a center cut (herein "cut") in the foil between the notched areas. [Figure 8E]

[0029] A second embodiment of the method of the present invention involving laser notching (ie, the end lane process) is shown for die punch processing of a foil. [Figure 9]

[0030] A photograph of the coated and calendered cathode roll is shown, in which the side lanes are about 90 mm wide, the center lane is about 20 mm wide, and the uncoated foil section is about 30 mm wide. [Figure 10]

[0031] A photograph of the coated and calendered cathode roll is shown, in which the width of the central coated lane is about 180 mm, the width of the side coated lane is about 10 mm, and the width of the uncoated area of ​​the foil is about 30 mm. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0023] Detailed Description Description of exemplary embodiments

[0032] Provided herein are compositions and methods for calendaring bilayer electrode (i.e., cathode) materials useful in the construction of lithium ion and lithium metal batteries.

[0024]

[0033] Also provided herein are compositions and methods for calendaring bilayer electrode materials useful in lithium ion and lithium metal batteries that include a solid separator.

[0025]

[0034] In certain aspects and embodiments disclosed elsewhere herein, the compositions and methods provide improved edge effect after calendering, in certain embodiments, improved edge effect includes elimination or reduction of edge effect.

[0026] definition

[0035] When referring to the compositions and methods provided herein, the following terms have the following meanings unless otherwise indicated. 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. In the event that there are multiple definitions for a term herein, those in this section prevail unless expressly stated otherwise.

[0027]

[0036] As used herein, the terms "a," "an," and "the" include aspects including one element as well as aspects including multiple elements. For example, an embodiment including "a cathode active material and a binder" should be understood to represent a particular aspect including at least a second cathode active material, at least a second binder, or both.

[0028]

[0037] The term "about" as used herein, when modifying a numerical value, such as about 15% w / w, refers to a numerical value that falls within a range including the modified numerical value, and optionally about ±10% of the modified numerical value. For example, about 15% w / w includes not only 15% w / w, but also 13.5% w / w, 14% w / w, 14.5% w / w, 15.5% w / w, 16% w / w, or 16.5% w / w. For example, "about 75°C" includes not only 75°C, but also 68°C, 69°C, 70°C, 71°C, 72°C, 73°C, 74°C, 75°C, 76°C, 77°C, 78°C, 79°C, 80°C, 81°C, 82°C, or 83°C.

[0029]

[0038] As used herein, the phrase "selected from the group consisting of" refers to a single element from the group, two or more elements from the group, or a combination of elements from the group. An element selected from the group consisting of A, B, and C includes, for example, A and B, A and C, B and C, and A, B and C, as well as A alone, B alone, or C.

[0030]

[0039] As used herein, the term "or" refers to a single element from a group, multiple elements from a group, or a combination of multiple elements from a group. An element selected from the group consisting of A, B, and C includes, for example, A and B, A and C, B and C, and A, B and C, as well as A alone, B alone, or C.

[0031]

[0040] As used herein, the term "dry air" refers to air that has a reduced amount of moisture. Dry air may be provided to clean rooms. Dry air is characterized by having a dew point of less than -10°C.

[0032]

[0041] As used herein, the term "cathode active material" refers to a material capable of intercalating or reversibly reacting with lithium ions. Examples include LiMPO4 (M=Fe, Ni, Co, Mn); Li x Ti y O z (x is 0-8, y is 1-12, z is 1-24);LiMn 2a Ni a O4 (a is 0~2); Nickel cobalt aluminum oxide, LiNi x Mn y Co z O2(x+y+z=1, 0≦x≦1, 0≦y≦1, 0≦z≦1); and LiNi x Co y Al z O2 (x+y+z=1, 0≦x≦1, 0≦y≦1, 0≦z≦1), where x, y, and z are selected such that the formula is charge neutral.

[0033]

[0042] As used herein, the term "solid-state cathode" refers to a cathode that does not contain a liquid phase electrolyte.

[0034]

[0043] The terms "cathode" and "anode" as used herein refer to the electrodes of a battery. Cathode and anode are often referred to in related art as positive and negative electrodes, respectively. In some applications, the cathode is used instead of the positive electrode, and the anode is used instead of the negative electrode. During the charge cycle of a Li secondary battery, Li ions move from the cathode through the electrolyte to the anode. During the charge cycle, electrons move from the cathode through an external circuit to the anode. During the discharge cycle of a Li secondary battery, Li ions move from the anode to the cathode through the electrolyte. During the discharge cycle, electrons move from the anode to the cathode through an external circuit.

[0035]

[0044] As used herein, the term "positive electrode" refers to the electrode in a secondary battery that carries positive ions (e.g., Li + As used herein, the term "negative electrode" refers to an electrode in a secondary battery through which positive ions (e.g., Li) conduct, flow, or move during the discharge of the battery. + ) flows or moves from the Li metal electrode and an electrode that contains a conversion chemistry, an intercalation chemistry, or a combination of conversion / intercalation chemistry (i.e., a cathode active material, such as NiF x , LiNi x Mn y Co z O2(NMC), LiNi x Al y Co z In a battery composed of LiCoO2 (NCA) (x+y+z=1); or doped LiCoO2, e.g., La-doped LiCoO2, Al-doped LiCoO2, or a combination thereof), the electrode with the conversion chemistry, intercalation chemistry, or combination of conversion / intercalation chemistry is called the positive electrode. In some applications, "cathode" is used instead of "positive electrode" and "anode" is used instead of "negative electrode". When a Li secondary battery is charged, the Li + The ions are positively charged (e.g. NiF x, NMC, NCA) toward the negative electrode (e.g. Li metal). When a Li secondary battery is discharged, Li + Ions migrate from the negative electrode towards the positive electrode.

[0036]

[0045] As used herein, the term "cathode material" refers to a mixture of components that form a positive electrode. Typically, the cathode material includes at least one cathode active material and at least one binder.

[0037]

[0046] As used herein, the term "solid separator" refers to a separator that is substantially insulating to electrons (e.g., the lithium ion conductivity is at least 10 times that of the electronic conductivity). 3 times, often 10 6 times larger), which acts as a physical barrier or spacer between the positive and negative electrodes in an electrochemical cell. + Refers to ionically conductive materials.

[0038]

[0047] As used herein, the term "edge defect" refers to bends, bubbles, cracks, chips, delaminations, warping, wrinkles, and the like, and combinations thereof (i.e., anything that prevents or reduces the conformability of the cathode to the current conductor). Typically, edge defects are defects in shape or contact rather than in chemical composition, and are typically visible without a microscope.

[0039]

[0048] As used herein, the term "substantial edge defects" refers to edge defects that render at least about 5% of the current collector or cathode unusable in subsequent steps in battery manufacturing, either due to physical deformation, poor physical contact with the cathode current collector, or a combination thereof.

[0040]

[0049] As used herein, the term "calendering" refers to the process of using metal rolls (typically hardened steel) to apply pressure to a surface (e.g., the surface of the cathode and its current collector) to alter its properties (e.g., to change the porosity of the material or to smooth its surface).

[0041]

[0050] As used herein, the term "cut" refers to an intentional discontinuity or break in a surface (e.g., the surface of a cathode current collector). A cut can be a gap where the ends of the cut do not touch (e.g., FIG. 3 or FIG. 4) or a slit where the ends of the cut are in close proximity (e.g., FIG. 2).

[0042]

[0051] The term "longitudinal edge" as used herein refers to the edge of the cathode / current collector that is parallel (or more nearly parallel, in the case of irregular edge shapes) to the direction in which the calendaring process takes place.

[0043]

[0052] The term "lateral edge" as used herein refers to the edge of the cathode / current collector that is perpendicular (or closer to perpendicular in the case of irregular edge shapes) to the direction in which the calendering process takes place.

[0044]

[0053] As used herein, the term "center cut" refers to a cut parallel to the longitudinal ends. In a preferred embodiment, the center cut bisects the lateral ends. For example, Figure 2 shows an example of such a center cut.

[0045]

[0054] As used herein, the terms "periodic" or "periodically" refer to a feature or effect that is repeated at regular intervals. For electrodes, this is usually a spatial interval, such as a set of periodic parallel cuts, each spaced 2.0 cm apart.

[0046]

[0055] As used herein, the term "patch coating" refers to gaps of cathode material on the surface of a current collector. Typically, the gaps are periodic.

[0047]

[0056] As used herein, the term "lane" refers to a region of a metal substrate (e.g., a cathode or cathode precursor) that is coated with a cathode material, either continuously or in patch coatings, whether near the midpoint of the metal substrate (the "center lane") or near a longitudinal end of the metal substrate (the "outer lane"). In certain preferred embodiments, a lane is separated from a second lane by a region of the metal substrate that is not coated with cathode material, and its longest dimension is parallel to the lateral end.

[0048]

[0057] The term "center lane" refers to the uncoated area between two coated lanes, the uncoated area being the area of ​​the metal substrate whose longest dimension is parallel to the lateral edges. The term "end lane" refers to the uncoated areas at the ends (e.g., longitudinal edges) of the coated areas.

[0049]

[0058] The term "coating material" as used herein refers to either a composition that includes active material or a dummy cathode material (e.g., one that does not include active material). In certain embodiments, the dummy cathode material has physical properties (e.g., viscosity, coating material height) similar to the cathode material during application or processing of the green bilayer, but the dummy cathode material does not include the active material included in the cathode material. In certain embodiments, the dummy cathode material includes an inexpensive carbon material with similar physical properties instead of the active material. In certain embodiments, the coating material is deposited on the metal foil by casting a slurry. Casting can be done using a drawdown table or doctor blade coating device. The slurry is dried, optionally with heating, before being calendered.

[0050]

[0059] As used herein, "binder" refers to a polymer that has the ability to enhance the adhesion and / or cohesion of materials, such as solids, in the green tape. "Binder" refers to a material that aids in the adhesion of another material.

[0051]

[0060] As used herein, "d 50 The phrase "diameter" refers to the median size in a size distribution as measured by microscopy or other particle size analysis techniques, such as, but not limited to, scanning electron microscopy and dynamic light scattering. 50 " includes the characteristic dimension below which 50% of the particles are smaller than the stated size.

[0052]

[0061] As used herein, "d 90 The phrase "diameter" refers to a size in a size distribution as measured by microscopy or other particle size analysis techniques, such as, but not limited to, scanning electron microscopy and dynamic light scattering. 90 " includes the characteristic dimension below which 90% of the particles are smaller than the stated size.

[0053]

[0062] As used herein, the phrase "film" or "thin film" refers to a thin film less than about 10 mm thick and greater than about 0.5 nm thick. A thin film also has a lateral dimension greater than 5 mm. A "film" or "thin film" can be manufactured by a continuous process such as tape casting, slip casting, or screen printing.

[0054]

[0063] As used herein, the phrase "film thickness" refers to the distance between the top and bottom surfaces of the film, or the median of the measured distances. As used herein, top and bottom refer to the surfaces of the film having the largest surface area. As used herein, thickness is measured by cross-sectional scanning electron microscopy.

[0055]

[0064] A "bi-laminate" as described herein is a composite material that includes a green body (e.g., cathode material) deposited on a metal layer. In some examples, the green body is continuous, and in other examples, the green body is deposited in a patch coating format. In some examples, the green body is produced by casting a slurry and then drying. In some examples, one layer of the bi-laminate is a metal foil. The metal foil may be produced from nickel (Ni), copper (Cu), aluminum (Al), iron (Fe), alloys thereof, and combinations thereof. In some embodiments, the bi-laminate is calendared. In some embodiments, the bi-laminate is sintered, fired, or calcined.

[0056]

[0065] "Green" as used herein refers to a bilayer that has not (or has not yet) been calendered. A "green bilayer" as described herein is a composite material that includes a green body deposited on a metal layer. In some examples, the green body is continuous, and in other examples, the green body is deposited in a patch coating format. The green body is produced by casting a slurry and then drying. In some examples, the green bilayer is an undried or undried bilayer. In some examples, one layer of the bilayer is a metal foil. The metal foil can be produced from nickel (Ni), copper (Cu), aluminum (Al), iron (Fe), alloys thereof, and combinations thereof.

[0057] bilayer composition

[0066] Provided herein are bilayer compositions useful as electrode (i.e., cathode) materials in solid-state lithium battery constructions.

[0058]

[0067] In certain aspects and embodiments, the present disclosure provides a metal substrate having longitudinal ends and lateral ends; a cathode material disposed on a metal substrate; A bilayer comprising: the longitudinal end includes one or more cuts extending from the longitudinal end to the cathode material; A bilayer is provided.

[0059]

[0068] In certain embodiments taught elsewhere herein, the cathode material covers at least about 50% of the surface of the metal substrate but does not cover the longitudinal edges.

[0060]

[0069] In certain embodiments taught elsewhere herein, the bilayer includes at least three lanes of coating material disposed on a metal substrate, with a first and second lane of coating material including a cathodic material.

[0061]

[0070] Suitable binders may include, but are not limited to, polyvinylidene fluoride (PVDF), polyvinylidene hexafluoropropylene (PVDF-HFP), styrene butadiene rubber (SBR), and ethylene alpha-olefin copolymers. For example, polyvinyl butyral, as used herein, is a binder because it is useful for adhering, for example, garnet materials. Other binders may include polycarbonates. Other binders may include polyacrylates and polymethacrylates. These examples of binders are not intended to limit the overall scope of binders contemplated herein, but rather serve merely as examples. Binders useful in the present disclosure include, but are not limited to, polypropylene (PP), polyethylene, atactic polypropylene (aPP), isotactic polypropylene (iPP), ethylene propylene rubber (EPR), ethylene pentene copolymer (EPC), polyisobutylene (PIB), styrene butadiene rubber (SBR), polyolefins, polyethylene-co-poly-1-octene (PE-co-PO), polyethylene-co-poly(methylenecyclopentane) (PE-co-PMCP), poly(methyl methacrylate) (and other acrylics), acrylics, polyvinyl acetacetal resins, polyvinyl butyral resins, PVB, polyvinyl acetal resins, stereoblock polypropylene, polypropylene polymethylpentene copolymers, polyethylene oxide (PEO), PEO block copolymers, silicones, and the like.In certain embodiments, including any of those previously described, the binder is selected from the group consisting of polyacrylonitrile (PAN), polypropylene, polyethylene, polyethylene oxide (PEO), polymethyl methacrylate (PMMA), polyvinyl chloride (PVC), polyvinylpyrrolidone (PVP), polyethylene oxide poly(allyl glycidyl ether) PEO-AGE, polyethylene oxide 2-methoxyethoxyethyl glycidyl ether (PEO-MEEGE), polyethylene oxide 2-methoxyethoxyethyl glycidyl poly(allyl glycidyl ether) (PEO-MEEGE-AGE), The binder is a polymer selected from the group consisting of polysiloxane, polyvinylidene fluoride (PVDF), polyvinylidene hexafluoropropylene fluoride (PVDF-HFP), ethylene propylene (EPR), nitrile rubber (NPR), styrene butadiene rubber (SBR), polybutadiene polymer, polybutadiene rubber (PB), polyisobutadiene rubber (PIB), polyolefin, α-polyolefin, ethylene α-polyolefin, polyisoprene rubber (PI), polychloroprene rubber (CR), acrylonitrile butadiene rubber (NBR), and polyethyl acrylate (PEA). In some examples, the binder may be a monopolymer or a copolymer. In some examples, the binder may be a PVdF-based polymer, a PVdF-based copolymer, or a combination thereof.

[0062]

[0071] In certain embodiments disclosed elsewhere herein, the cathode slurry includes a carbon source, such as carbon black, acetylene black, graphite, graphene, furnace black, ketjen black, single-walled carbon nanotubes, multi-walled carbon nanotubes, or combinations thereof. The carbon source may be added to the cathode slurry at about 1-3 w / w%.

[0063]

[0072] In certain embodiments disclosed elsewhere herein, the cathode slurry includes a surfactant, hi certain embodiments, the surfactant is a hyperbranched polyamine copolymer or a polyacrylonitrile copolymer.

[0064]

[0073] In certain embodiments disclosed elsewhere herein, the cathode slurry includes a binder. In certain embodiments, the binder may be a functionalized PVDF polymer, polyvinyl alcohol, polyamine, polyacrylate, polyurethane, polystyrene, or any combination thereof. In certain embodiments disclosed elsewhere herein, the cathode slurry includes a cathode active material and a carbon source, as well as an optional surfactant and an optional binder. In certain embodiments, a dummy slurry is used, applied to the foil substrate at the same height as the cathode slurry. The dummy slurry may not include a cathode active material.

[0065]

[0074] In certain embodiments as otherwise taught herein, the cut has a T-shape (e.g., FIG. 2). In certain embodiments, the cut has an L-shape. In certain embodiments, the cut has an I-shape. In certain embodiments, the cut has a cross-shape. In certain embodiments, the cut has a U-shape (e.g., FIG. 3). In certain embodiments, the cut has a V-shape.

[0066]

[0075] In certain embodiments as otherwise taught herein, one or more of the cuts is a gap. In certain embodiments, one or more of the cuts is a slit.

[0067]

[0076] In certain embodiments taught elsewhere herein, one or more of the longitudinal edges between the cuts are shaped as one or more battery tabs.

[0068]

[0077] In certain embodiments as otherwise taught herein, the metal substrate has one or more perforations or depressions shaped as one or more battery tabs. In certain embodiments, the one or more perforations or depressions are located along a longitudinal edge. In certain embodiments, the one or more perforations or depressions are located proximate to a longitudinal edge.

[0069]

[0078] In certain embodiments as otherwise taught herein, the cuts are periodically spaced. In certain embodiments, the cuts are periodically spaced at intervals of 1-20 cm (e.g., about 1, 1.5, 2, 2.5, 3, 3.5, 4, 4.5, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, or 20). In certain embodiments, the cuts are periodically spaced at intervals of 3-10 cm (e.g., about 3, 3.5, 4, 4.5, 5, 5.5, 6, 6.5, 7, 7.5, 8, 8.5, 9, 9.5, or 10). In certain embodiments, provided herein are bilayers as otherwise taught herein in which the cuts are not periodically spaced.

[0070]

[0079] In certain embodiments as otherwise taught herein, cuts are present on both longitudinal ends. In some embodiments, the cut on one longitudinal end is the same as the cut on the other longitudinal end. In other embodiments, the cut on one longitudinal end is different from the cut on the other longitudinal end. In certain embodiments, one longitudinal end has a T-shaped slit cut and the other longitudinal end has a rectangular cut.

[0071]

[0080] In certain embodiments taught elsewhere herein, the cathode material is coated onto the substrate as a patch (ie, patch coated).

[0072]

[0081] In certain embodiments taught elsewhere herein, the cathode material coats at least one or more lateral edges.

[0073]

[0082] In certain embodiments taught elsewhere herein, the cathode further comprises a center cut (i.e., a cut parallel to the longitudinal ends). In certain embodiments, cuts are present at both longitudinal ends and the cathode further comprises a center cut (e.g., FIG. 2).

[0074]

[0083] In certain embodiments as otherwise taught herein, the cathode further comprises one or more slits. In certain embodiments, the slits comprise an I-shape, an L-shape, a T-shape, or a combination thereof. In certain embodiments, the slits have an I-shape. In certain embodiments, the slits have an L-shape. In certain embodiments, the slits have a T-shape.

[0075]

[0084] In certain embodiments as otherwise taught herein, the cuts include one or more geometric shapes. In certain embodiments, the geometric shapes include a triangle, a semicircle, an arch, a trapezoid, a parallelogram, or combinations thereof. In certain embodiments, the geometric shapes include a triangle. In certain embodiments, the geometric shapes include a semicircle. In certain embodiments, the geometric shapes include an arch. In certain embodiments, the geometric shapes include a trapezoid. In certain embodiments, the geometric shapes include a parallelogram, such as a rectangle (e.g., a square).

[0076]

[0085] In certain embodiments as otherwise taught herein, the cuts include one or more slits and one or more geometric shapes (e.g., alternating T-shaped slits and rectangles). The pattern may be a periodic or non-periodic sequence, combining different slits and different geometric shapes, such as, but not limited to, the embodiment depicted in FIG. 5. In certain embodiments, the electrodes may have either slits or shapes, or both, on each side over the entire length or a certain length of the roll. In certain embodiments, the electrodes may have various combinations of different slits and shapes (e.g., L-shaped, square, L-shaped, or square) even on the same end.

[0077]

[0086] In certain embodiments taught elsewhere herein, the end of the cut is about 0-6 mm (e.g., about 0, 0.25, 0.5, 0.75, 1.0, 1.25, 1.5, 1.75, 2.0, 2.5, 3.0, 3.5, 4.0, 4.5, 5.0, 5.5, or 6.0 mm) from the end of the cathode material. In certain embodiments, the edge of the cut is about 0-0.2 mm (e.g., about 0.01, 0.02, 0.025, 0.03, 0.04, 0.05, 0.06, 0.07, 0.075, 0.08, 0.09, 0.10, 0.11, 0.12, 0.125, 0.13, 0.14, 0.15, 0.16, 0.17, 0.175, 0.18, 0.19, or 0.20 mm) from the edge of the cathode material.

[0078]

[0087] In certain embodiments taught elsewhere herein, the distance between an end of a first cut and an end of a second adjacent cut is between about 5 mm and 75 mm (e.g., about 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 49, 50, 51, 52, 53, 54, 55, 56, 57, 58, 59, 60, 61, 62, 63, 64, 65, 66, 67, 68, 69, 70, 71, 72, 73, 74, 75, 75, 76, 77, 78, 79, 80, 81, 82, 83, 84, 85, 86, 87, 88, 89, 90, 91, 92, 93, 94, 95, 96, 97, 98, 99, 100, 101, 102, 103, 104, 105, 106, 107, 108, 109, 110, 111, 112, 113, 114, 115, 116, 117, , 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 49, 50, 51, 52, 53, 54, 55, 56, 57, 58, 59, 60, 61, 62, 63, 64, 65, 66, 67, 68, 69, 70, 71, 72, 73, 74, or 75 mm).

[0079]

[0088] In certain embodiments taught elsewhere herein, the cathode has a surface area of ​​at least about 29 mg / cm 2 (i.e., at least about 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 49, or 50 mg / cm 2 In certain embodiments, the cathode has an active material loading of at least about 5-50 mg / cm. 2(i.e., about 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 49, or 50 mg / cm 2 ) of the active material carried thereon.

[0080]

[0089] In certain embodiments taught elsewhere herein, the cathode has a thickness of about 190 μm to about 240 μm (e.g., about 150 to about 300 μm, about 175 to about 275 μm, about 190 to about 240 μm, or about 200 to about 250 μm). In certain embodiments, the cathode has a thickness of less than about 250 μm (e.g., 5, 10, 25, 50, 75, or 100 to about 250 μm). In certain embodiments, the cathode has a thickness of less than about 200 μm (e.g., 5, 10, 25, 50, 75, or 100 to about 200 μm). In certain embodiments, the cathode has a thickness of less than about 150 μm (e.g., 5, 10, 25, 50, 75, or 100 to about 150 μm). In certain embodiments, the cathode has a thickness of about 100 to about 250 μm.

[0081]

[0090] In certain embodiments taught elsewhere herein, the porosity of the cathode is about 25% by volume or less (e.g., about 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, or 10% by volume or less).

[0082]

[0091] In certain embodiments taught elsewhere herein, the cathode porosity after calendaring is between about 40% and 7% porosity (e.g., about 40, 39, 38, 37, 36, 35, 34, 33, 32, 31, 30, 29, 28, 27, 26, 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, or 7% by volume).

[0083]

[0092] In certain embodiments taught elsewhere herein, the cathode porosity before calendering is between about 30% and 60% porosity (e.g., about 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 49, 50, 51, 52, 53, 54, 55, 56, 57, 58, 59, or 60% by volume).

[0084]

[0093] In certain embodiments as otherwise taught herein, the metal substrate is free of edge defects.In certain embodiments, provided herein are bilayers as otherwise taught herein, in which the cathode is free of edge defects.

[0085]

[0094] In certain embodiments as taught elsewhere herein, the metal substrate is substantially free of edge defects.In certain embodiments, provided herein are bilayers as taught elsewhere herein, in which the cathode is substantially free of edge defects.

[0086]

[0095] In certain embodiments taught elsewhere herein, the cathode has a surface flatness variation (e.g., less than 1 cm) of about 50 μm or less (e.g., about 50, 45, 40, 35, 30, 25, 20, 15, 10, or 5 μm). 2 In certain embodiments, the variation in surface flatness is about 50-5 μm (e.g., about 50, 45, 40, 35, 30, 25, 20, 15, 10, or 5 μm). In certain embodiments, the variation in surface flatness is about 40-10 μm (e.g., about 40, 35, 30, 25, 20, 15, or 10 μm).

[0087]

[0096] In certain embodiments taught elsewhere herein, the cathode is 1 cm 2 In certain embodiments, the cathode has a surface flatness of about 1 to 50 μm (e.g., about 50, 45, 40, 35, 30, 25, 20, 15, 10, or 5 μm) per cm. 2 The surface has a surface flatness of about 50 μm or less (e.g., about 50, 45, 40, 35, 30, 25, 20, 15, 10, or 5 μm) per

[0088]

[0097] In certain embodiments as otherwise taught herein, the metal substrate is an aluminum or aluminum alloy metal substrate. In certain embodiments, the metal substrate is aluminum. In certain embodiments, the metal substrate is an aluminum alloy metal substrate.

[0089]

[0098] In certain embodiments as otherwise taught herein, the metal substrate is a copper or copper alloy metal substrate. In certain embodiments, the metal substrate is copper. In certain embodiments, the metal substrate is a copper alloy metal substrate.

[0090]

[0099] In certain embodiments as otherwise taught herein, the metal substrate is a nickel or nickel alloy metal substrate. In certain embodiments, the metal substrate is nickel. In certain embodiments, the metal substrate is a nickel alloy metal substrate.

[0091]

[0100] In certain embodiments taught elsewhere herein, the metal substrate has a thickness of about 8.0 μm to 35 μm (i.e., about 8.0, 8.5, 9.0, 9.5, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, or 35 μm).

[0092]

[0101] In certain embodiments as otherwise taught herein, the metal substrate may be between about 5.0 mm and 400 mm (i.e., about 5.0, 5.25, 5.5, 5.75, 6, 6.5, 7, 7.5, 8, 8.5, 9, 9.5, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 27.5, 30, 32.5, 35, 37.5, 40, 42.5, 45, 47.5, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 100, 105, 110, 115, 120, 125, 130, 140, 150, 160, 170, 175, 180, 190, 200, 210, 220, 225, 230, 240, 250, 260, 270, 275, 280, 290, 300, 310, 320, 325, 330, 340, 350, 360, 370, 375, 380, 390, or 400 mm.

[0093]

[0102] In certain embodiments as otherwise taught herein, the metal substrate may have a thickness of about 12 cm to 1000 cm (i.e., about 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 27.5, 30, 32.5, 35, 37.5, 40, 42.5, 45, 47.5, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 100, 105, 110, 115, 120, 125, 130, 140, 150, 160, 170, 175, 180, 190, 200, 210, 220, 230, 240, 250, 27.5, 30, 32.5, 35, 37.5, 40, 42.5, 45, 47.5, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 100, 105, 110, 115, 120, 125, 130, 140, 150, 160, 170, 175, 180, 190, 210, 220, 230, 240, 250, 260, 270, 280, 290, 300, 310, 320, 330, 340, 350, 36 , 200, 210, 220, 225, 230, 240, 250, 260, 270, 275, 280, 290, 300, 310, 320, 325, 330, 340, 350, 360, 370, 375, 380, 390, 400, 425, 450, 475, 500, 525, 550, 575, 600, 625, 650, 675, 700, 725, 750, 775, 800, 825, 850, 875, 900, 925, 950, 975, or 1000 cm). In certain embodiments, the metal substrate is between about 1.0 m and 1000 m (i.e., about 1.0, 1.5, 2.0, 2.5, 3.0, 3.5, 4.0, 4.5, 5.0, 5.5, 6.0, 6.5, 7.0, 7.5, 8.0, 8.5, 9.0, 9.5, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 27.5, 30, 32.5, 35, 37.5, 40, 42.5, 45, 47.5, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 100, 105, 110, 115, 120, 125, 130, 135, 140, 145, 150, 160, 170, 185, 190, 195, 200, 205, 206, 207, 208, 209, 210, 211, 212, 213, 214, 215, 216, 217, 218, 219, 220, 221, 222, 230, 231, 232, 233, 234, 235, 240, 241, 242, 243, 244, 245, 245, 2 5, 130, 140, 150, 160, 170, 175, 180, 190, 200, 210, 220, 225, 230, 240, 250, 260, 270, 275, 280, 290, 300, 310, 320, 325, 330, 340, 350, 360, 370, 375, 380, 390, 400, 425, 450, 475, 500, 525, 550, 575, 600, 625, 650, 675, 700, 725, 750, 775, 800, 825, 850, 875, 900, 925, 950, 975, or 1000 m).

[0094]

[0103] In certain embodiments as otherwise taught herein, the metal substrate is bare (i.e., uncoated). In certain embodiments, the metal substrate has a carbon coating on one side. In certain embodiments, the metal substrate has a carbon coating on both sides.

[0095]

[0104] In certain embodiments taught elsewhere herein, the carbon coating includes carbon black, graphite, graphene, acetylene black, furnace black, ketjen black, single-walled carbon nanotubes, multi-walled carbon nanotubes, or combinations thereof.

[0096]

[0105] In certain embodiments taught elsewhere herein, the carbon coating has a thickness of about 5 to 4000 mm. 2 / g (e.g., about 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 22.5, 25, 27.5, 30, 32.5, 35, 37.5, 40, 42.5, 45, 47.5, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 1 00, 105, 110, 115, 120, 125, 130, 140, 150, 160, 170, 175, 180, 190, 200, 210, 220, 225, 230, 240, 250, 275, 300, 325, 350, 375, 400, 425, 450, 475, 500, 525 , 550, 575, 600, 625, 650, 675, 750, 800, 850, 900, 950, 1000, 1050, 1100, 1150, 1200, 1250, 1300, 1350, 1400, 1450, 1500, 1600, 1700, 1750, 1800, 1900, 2 000, 2100, 2200, 2250, 2300, 2400, 2500, 2600, 2700, 2750, 2800, 2900, 3000, 3100, 3200, 3250, 3300, 3400, 3500, 3600, 3700, 3750, 3800, 3900, or 4000m 2 / g) surface area.

[0097]

[0106] In certain embodiments taught elsewhere herein, the carbon coating on the metal substrate has a thickness of about 0.5 μm to 7.0 μm (i.e., about 0.5, 0.6, 0.7, 0.75, 0.8, 0.9, 1.0, 1.1, 1.2, 1.25, 1.3, 1.4, 1.5, 1.6, 1.75, 1.8, 1.9, 2.0, 2.25, 2.5, 2.75, 3.0, 3.25, 3.5, 3.75, 4.0, 4.25, 4.5, 4.75, 5.0, 5.25, 5.5, 5.75, 6.0, 6.25, 6.5, 6.75, or 7 μm).

[0098]

[0107] In certain embodiments as otherwise taught herein, the carbon coating of the metal substrate is the same on both sides. In certain embodiments, the carbon coating of the metal substrate is different on each side.

[0099]

[0108] The carbon coating of the metal substrate can be of any width and any length up to and including the width and length of the metal substrate. In certain embodiments as otherwise taught herein, the carbon coating is the same width as the metal substrate. In certain embodiments, the width of the carbon coating is less than the width of the metal substrate. In certain embodiments, the carbon coating is the same length as the metal substrate. In certain embodiments, the length of the carbon coating is less than the length of the metal substrate.

[0100]

[0109] In certain embodiments taught elsewhere herein, the metal substrate having a carbon coating has a thickness of about 8.0 μm to 40 μm (i.e., about 8.0, 8.5, 9.0, 9.5, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, or 40 μm).

[0101]

[0110] In certain embodiments taught elsewhere herein, the positive electrode active material layer can include a sulfide solid electrolyte, an oxide solid electrolyte, etc. For example, the sulfide solid electrolyte can include a mixture of Li2S:P2S5.

[0102]

[0111] In certain embodiments taught elsewhere herein, the surface of the positive electrode active material may be coated with a solid electrolyte, such as a conductive material (e.g., acetylene black, etc.), a binder (e.g., polyvinylidene fluoride, etc.), etc.

[0103]

[0112] In certain embodiments taught elsewhere herein, the material for the cathode is prepared by mixing (e.g., kneading) the components of the cathode with a solvent to form a paste, and then spreading the paste onto a positive current collector, after which the paste is dried and the material in the positive electrode is densified by pressing (e.g., by calendaring).

[0104]

[0113] In certain embodiments taught elsewhere herein, the thickness of the positive electrode active material layer after pressing is, for example, about 5 to 250 μm, preferably about 10 to 100 μm or about 20 to 50 μm, for example, about 20, 25, 30, 35, 40, 45, or 50 μm.

[0105]

[0114] In certain aspects and embodiments, the present disclosure provides a metal substrate having at least two longitudinal ends and at least two lateral ends; a cathode material disposed on a metal substrate; A green bilayer comprising: the longitudinal end includes one or more cuts extending from the longitudinal end to the cathode material; A green bilayer is provided.

[0106]

[0115] In certain embodiments taught elsewhere herein, the cathode material covers at least about 50% of the surface of the metal substrate but does not cover the longitudinal edges.

[0107]

[0116] In certain embodiments taught elsewhere herein, the green bilayer includes at least three lanes of coating material disposed on a metal substrate, with a first and second lane of coating material including a cathode material.

[0108]

[0117] In certain aspects and embodiments disclosed elsewhere herein, the cuts are periodically spaced.

[0109]

[0118] In certain aspects and embodiments disclosed elsewhere herein, the cathode material coats at least one or more lateral edges.

[0110]

[0119] In certain aspects and embodiments disclosed elsewhere herein, the cut has a T-shape.

[0111]

[0120] In certain embodiments disclosed elsewhere herein, the metal substrate has one or more perforations or depressions shaped as one or more battery tabs.

[0112]

[0121] In certain embodiments disclosed elsewhere herein, the cathode further comprises one or more slits. In certain embodiments, the slits comprise an I-shape, an L-shape, a T-shape, or a combination thereof. In certain embodiments, the slits have an I-shape. In certain embodiments, the slits have an L-shape. In certain embodiments, the slits have a T-shape.

[0113]

[0122] In certain embodiments as otherwise taught herein, the cuts include one or more geometric shapes. In certain embodiments, the geometric shapes include a triangle, a semicircle, an arch, a trapezoid, a parallelogram, or combinations thereof. In certain embodiments, the geometric shapes include a triangle. In certain embodiments, the geometric shapes include a semicircle. In certain embodiments, the geometric shapes include an arch. In certain embodiments, the geometric shapes include a trapezoid. In certain embodiments, the geometric shapes include a parallelogram, such as a rectangle (e.g., a square).

[0114]

[0123] In certain embodiments taught elsewhere herein, the cuts include one or more slits and one or more geometric shapes (eg, alternating T-shaped slits and rectangles).

[0115]

[0124] In certain embodiments, the cuts at the two ends do not have an offset.In certain embodiments, the cuts at the two ends have an offset.

[0116]

[0125] In certain embodiments disclosed elsewhere herein, the cathode material has a thickness of about 100 μm to about 250 μm (e.g., about 150 to about 275 μm, about 175 to about 250 μm, about 190 to about 240 μm, or about 200 to about 250 μm). In certain embodiments, the cathode material has a thickness of less than about 250 μm. In certain embodiments, the cathode material has a thickness of less than about 200 μm. In certain embodiments, the cathode material has a thickness of less than about 150 μm.

[0117]

[0126] In certain embodiments taught elsewhere herein, the cathode is substantially free of edge defects.

[0118]

[0127] In certain aspects and embodiments disclosed elsewhere herein, the edge defect is selected from the group consisting of a crack, a bend, a warp, a wrinkle, a delamination, and combinations thereof.

[0119]

[0128] In certain embodiments, the bilayer cathodic material is disposed in two lanes on the metal substrate. In certain embodiments, the bilayer cathodic material is disposed in three lanes on the metal substrate. In certain embodiments, the bilayer cathodic material is disposed in four or more lanes on the metal substrate.

[0120]

[0129] In certain embodiments, the lanes are continuous. In certain embodiments, the lanes are discontinuous (e.g., patch coating). In certain embodiments, the lanes are parallel to the longitudinal edges. In certain embodiments, the cathode material of the bilayer is arranged as two wide outer lanes and a narrow central lane.

[0121]

[0130] In certain embodiments taught elsewhere herein, the cathode material covers at least about 50% of the surface of the metal substrate but does not cover the longitudinal edges.

[0122]

[0131] In certain embodiments taught elsewhere herein, the green bilayer includes at least three lanes of coating material disposed on a metal substrate, with a first and second lane of coating material including a cathode material.

[0123]

[0132] In certain aspects and embodiments as otherwise taught herein, a metal substrate having at least two longitudinal ends and at least two lateral ends; at least three lanes of coating material disposed on the metal substrate; A bilayer comprising: the first and second lanes of coating material comprise a cathode material; A bilayer is provided.

[0124]

[0133] In certain aspects and embodiments as otherwise taught herein, a metal substrate having at least two longitudinal ends and at least two lateral ends; at least three lanes of coating material disposed on the metal substrate; A bilayer comprising: the first and second lanes of coating material include a cathodic material; the longitudinal end includes one or more cuts extending from the longitudinal end toward the coating material; A bilayer is provided.

[0125]

[0134] In certain embodiments taught elsewhere herein, the cathode material covers at least about 50% of the surface of the metal substrate, but does not cover the longitudinal edges.

[0126]

[0135] In certain embodiments taught elsewhere herein, the bilayer includes at least three lanes of coating material disposed on a metal substrate, with a first and second lane of coating material including a cathodic material.

[0127]

[0136] In certain aspects and embodiments as otherwise taught herein, a metal substrate having at least two longitudinal ends and at least two lateral ends; at least three lanes of coating material disposed on the metal substrate; A green bilayer comprising: the first and second lanes of coating material comprise a cathode material; A green bilayer is provided.

[0128]

[0137] In certain aspects and embodiments as otherwise taught herein, a metal substrate having at least two longitudinal ends and at least two lateral ends; at least three lanes of coating material disposed on the metal substrate; A green bilayer comprising: the first and second lanes of coating material include a cathodic material; the longitudinal end includes one or more cuts extending from the longitudinal end toward the coating material; A green bilayer is provided.

[0129]

[0138] In certain embodiments taught elsewhere herein, the cathode material covers at least about 50% of the surface of the metal substrate, but does not cover the longitudinal edges.

[0130]

[0139] In certain embodiments taught elsewhere herein, the green bilayer includes at least three lanes of coating material disposed on a metal substrate, with a first and second lane of coating material including a cathode material.

[0131]

[0140] In certain embodiments, provided herein is a bilayer or green bilayer as otherwise disclosed herein, wherein the third lane of coating material comprises a cathode material. In certain embodiments, the third lane of coating material does not comprise a cathode material. In certain embodiments, the three coating material lanes are identical in composition. In certain embodiments, the three coating material lanes are not identical in composition.

[0132]

[0141] In a particular embodiment, a metal foil is provided that includes two longitudinal ends and two lateral ends, the metal foil being coated with a coating material, where the coating material does not coat the longitudinal ends and is separated by parallel or nearly parallel exposed metal foil portions, and the longitudinal ends include one or more cuts extending from the longitudinal ends toward the coating material.

[0133]

[0142] In certain embodiments, at least 50% of the surface of the metal foil is coated with the coating material.

[0134]

[0143] In certain embodiments, the first and third lanes are positioned 1-5 mm (e.g., about 0.5, 0.75, 1.0, 1.5, 2.0, 2.5, 3.0, 3.5, 4.0, 4.5, or 5.0 mm) from the longitudinal end, excluding any tab features on the longitudinal end.

[0135]

[0144] In certain embodiments, the material is coated to have a uniform average thickness of 150 μm to 500 μm (e.g., about 150, 175, 200, 225, 250, 275, 300, 325, 350, 375, 400, 425, 450, 475, or 500 μm) before calendaring. In certain embodiments, after calendaring, the material has a uniform average thickness of 100 μm to 500 μm, 150 μm to 400 μm, 150 μm to 300 μm, or 150 μm to 250 μm.

[0136]

[0145] In certain embodiments, the coating material has a uniform average thickness.

[0137]

[0146] In certain embodiments, at least three lanes of material disposed on a metal substrate have average thicknesses within 10-20% (e.g., 5%, 7.5%, 10%, 12.5%, 15%, 17.5%, or 20%) of each other.

[0138] Manufacturing method

[0147] Provided herein are methods (ie, processes) for making the bilayer compositions described in this application.

[0139]

[0148] In certain embodiments, the bilayer compositions can be formed as described herein and used in the manufacture of lithium ion batteries, lithium batteries, solid-state lithium batteries, and components thereof. Examples of such batteries and their component parts are described, for example, in PCT Applications PCT / US2021 / 049528 and PCT / US2022 / 053080.

[0140]

[0149] In certain aspects, the present disclosure provides Providing a bilayer, the bilayer comprising: a metal substrate having longitudinal ends and lateral ends; a cathode material disposed on a metal substrate; Including, the longitudinal end includes one or more cuts extending from the longitudinal end to a cathode material disposed on the metal substrate; and calendering the bilayer; A method for making a cathode is provided, comprising:

[0141]

[0150] In certain embodiments taught elsewhere herein, the cathode material covers at least about 50% of the surface of the metal substrate but does not cover the longitudinal edges.

[0142]

[0151] In certain embodiments taught elsewhere herein, the green bilayer includes at least three lanes of coating material disposed on a metal substrate, with a first and second lane of coating material including a cathode material.

[0143]

[0152] In certain embodiments, the bilayer is not calendered ("green"). As used herein, green refers to the bilayer before it is calendered. In certain embodiments, the green bilayer is not (or has not yet been) fired, calcined, or sintered.

[0144]

[0153] In certain embodiments, provided herein is a method as taught elsewhere herein, further comprising die punching the bilayer.

[0145]

[0154] In certain embodiments, provided herein are methods as taught elsewhere herein, further comprising heating the bilayer. High temperatures are used in the industry to achieve high density and low porosity cathodes. For example, Current and future lithium-ion battery manufacturing(cell.com)(https: / / www.cell.com / iscience / pdf / S2589-0042(21)00300-X.pdf); Investigation of the Adhesion Strength along the Electrode Manufacturing Process for Improved Lithium-Ion Anodes-Billot-2020-Energy Technology-Wiley Online Library(https: / / onlinelibrary.wiley.com / doi / 10.1002 / ente.201801136); Calendar of Li(Ni 0.33 Mn 0.33 Co 0.33)O2-Based Cathodes: Analyzing the Link Between Process Parameters and Electrode Properties by Advanced Statistics-Primo-2021-Batteries&Supercaps-Wiley Online Library(https: / / chemistry-europe.onlinelibrary.wiley.com / doi / 10.1002 / batt.202000324) Please refer to.

[0146]

[0155] In certain embodiments, the present disclosure provides a method for producing a cathode at a temperature lower than that typically used in the art. In certain embodiments, the green bilayer of the present disclosure is calendered at a temperature less than 100° C. (e.g., about 100, 95, 90, 85, 80, 75, 70, 65, 60, 55, 50, 45, 40, 35, 30, 25, or 20° C.). In certain embodiments, the green bilayer is calendered at a temperature less than 75° C. (e.g., about 75, 70, 65, 60, 55, 50, 45, 40, 35, 30, 25, or 20° C.). In certain embodiments, the green bilayer is calendered at a temperature less than 50° C. (e.g., about 50, 45, 40, 35, 30, 25, or 20° C.). In certain embodiments, the green bilayer is calendered at a temperature of 30° C. to 100° C. (e.g., about 100, 95, 90, 85, 80, 75, 70, 65, 60, 55, 50, 45, 40, 35, or 30° C.), 40° C. to 90° C. (e.g., about 90, 85, 80, 75, 70, 65, 60, 55, 50, 45, or 40° C.), or 50° C. to 75° C. (e.g., about 75, 70, 65, 60, 55, or 50° C.).

[0147]

[0156] In certain embodiments of the methods taught elsewhere herein, two active rollers are used to calender the bilayer. In certain embodiments, one active roller is used to calender the bilayer.

[0148]

[0157] In certain embodiments of the methods taught elsewhere herein, calendering of the bilayer is done sheet by sheet, hi certain embodiments, calendering of the bilayer is done in a roll-to-roll manner (e.g., using a winder / rewinder).

[0149]

[0158] In certain embodiments of the methods taught elsewhere herein, the calendering of the bilayer is at a pressure of at least about 50 MPa (eg, at least about 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, or 100 MPa).

[0150]

[0159] In certain embodiments of the methods taught elsewhere herein, the calendering of the bilayer is at a pressure of about 150 MPa to 2000 MPa (e.g., about 150, 160, 175, 200, 225, 250, 275, 300, 325, 350, 375, 400, 450, 500, 550, 600, 650, 700, 750, 800, 850, 900, 950, 1000, 1100, 1200, 1250, 1300, 1400, 1500, 1600, 1700, 1750, 1800, 1900, or 2000 MPa).

[0151]

[0160] In certain embodiments of the methods taught elsewhere herein, the calendering of the bilayer is performed at a speed between about 0.1 m / s and 50 m / s (e.g., about 0.1, 0.15, 0.2, 0.25, 0.3, 0.35, 0.4, 0.45, 0.5, 0.6, 0.7, 0.8, 0.9, 1.0, 1.25, 1.5, 1.75, 2.0, 2.25, 2.5, 2.75, 3.0, 3.25, 3.5, 3.75, 4.0, 4.25, 4. ... , 4.5, 4.75, 5, 5.5, 6, 6.5, 7, 7.5, 8, 8.5, 9, 9.5, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 49, or 50 m / s).

[0152]

[0161] In certain embodiments of the methods taught elsewhere herein, the bilayer is subjected to a single calendering. In certain embodiments of the methods taught elsewhere herein, the bilayer is subjected to more than one calendering (e.g., two times). In certain embodiments, the calendering conditions are the same. In certain embodiments, the calendering conditions are different.

[0153]

[0162] In certain embodiments of the methods taught elsewhere herein, the cathode has a thickness of at least about 25 mg / cm 2 In some embodiments, the cathode has an active material loading of at least about 26 mg / cm 2 , 27 mg / cm 2 , 28 mg / cm 2 , 29 mg / cm 2 , or 30 mg / cm 2 The amount of the active material carried is 100%.

[0154]

[0163] In certain embodiments of the methods taught elsewhere herein, the thickness of the cathode is reduced to about 240 μm to about 190 μm (e.g., about 300 to 240, about 275 to 220, about 250 to 200 μm, about 200 to 160 μm, about 175 to 140 μm, or about 200 to 250 μm).

[0155]

[0164] In certain embodiments of the methods taught elsewhere herein, the porosity of the cathode is reduced to about 25% or less (e.g., about 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, or 10% or less).

[0156]

[0165] In certain embodiments as taught elsewhere herein, the cathode after calendering has a surface flatness variation of about 50 μm or less (e.g., about 50, 45, 40, 35, 30, 25, 20, 15, 10, or 5 μm). In certain embodiments, the surface flatness variation is about 50-5 μm (e.g., about 50, 45, 40, 35, 30, 25, 20, 15, 10, or 5 μm). In certain embodiments, the surface flatness variation is about 40-10 μm (e.g., about 40, 35, 30, 25, 20, 15, or 10 μm).

[0157]

[0166] In certain embodiments taught elsewhere herein, the cathode active material is a material described in International Patent Application Publication No. PCT / US2021 / 049528, entitled "CATHODE COATING," filed September 8, 2021, the entire contents of which are incorporated herein by reference in their entirety for all purposes.

[0158]

[0167] In certain embodiments taught elsewhere herein, the cathode comprises a cathode active material selected from manganese oxide, iron oxide, copper oxide, nickel oxide, lithium-manganese composite oxide, lithium-nickel composite oxide, lithium-cobalt composite oxide, lithium-cobalt-nickel oxide, lithium-manganese-cobalt composite oxide, spinel phase lithium-manganese-nickel composite oxide, lithium phosphate having an olivine structure, lithium phosphate having a NASICON type structure, iron (III) sulfate, vanadium oxide, and combinations thereof.

[0159]

[0168] In certain embodiments taught elsewhere herein, the cathode active material is MnO, Li x Mn2O4, Li x MnO2, Li x NiO2, Li x CoO2, LiNi (1-y) Co y O2, LiMn y Co (1-y) O2, Li x Mn (2-y) Ni y O4, Li x FePO4, Li x Fe (1-y) Mn y PO4, Li x and selected from CoPO4, Li7V2(PO4)3, Fe2(SO4)3, V2O5, and combinations thereof, where 1≦x≦5 and 0≦y≦1.

[0160]

[0169] In certain embodiments taught elsewhere herein, the cathode active material is LiMPO4 (M=Fe, Ni, Co, Mn); x Ti y O z (x is 0 to 8, y is 1 to 12, and z is 1 to 24);LiMn 2a Ni a O4 (where a is 0 to 2); Nickel cobalt aluminum oxide; LiNi x Mn y Co z O2(x+y+z=1, 0≦x≦1, 0≦y≦1, 0≦z≦1); and LiNi x Co y Al z O2(x+y+z=1, 0≦x≦1, 0≦y≦1, 0≦z≦1).

[0161]

[0170] In certain embodiments taught elsewhere herein, the cathode active material is LiNi x Mn y Co z O2(NMC)(x+y+z=1, 0≦x≦1, 0≦y≦1, 0≦z≦1, x+y+z=1).

[0162]

[0171] In certain embodiments taught elsewhere herein, the cathode active material is LiNi x Mn y Co z O2 (x is 0.8, y is 0.1, and z is 0.1).

[0163]

[0172] In certain embodiments taught elsewhere herein, the cathode active material is LiNi x Mn y Co z O2 (x is 0.6, y is 0.2, and z is 0.2).

[0164]

[0173] In certain embodiments taught elsewhere herein, the cathode active material is LiNi x Mn y Co z O2 (x is 0.5, y is 0.3, and z is 0.2).

[0165]

[0174] In certain embodiments taught elsewhere herein, the cathode active material is LiNi x Mn y Co z O2 (x is 1 / 3, y is 1 / 3, and z is 1 / 3).

[0166]

[0175] In certain embodiments taught elsewhere herein, the cathode active material is Li(NiCoMn)O2. In certain embodiments taught elsewhere herein, the cathode active material is NMC, NCA, NMO, LCO, LFP, or a combination thereof.

[0167]

[0176] In certain embodiments taught elsewhere herein, the cathode active material is LiFePO4.

[0168]

[0177] In certain embodiments taught elsewhere herein, the NMC is 0.1 μm <S<50μmのd 50 In a particular embodiment, the NMC has a particle size S of 0.5 μm. <S<30μmのd 50 In a particular embodiment, the NMC has a particle size S of 1 μm <S<20μmのd 50 It has a particle size S.

[0169]

[0178] In certain embodiments, including any of the foregoing, the present specification provides a thin sheet comprising a cathode bilayer as described herein.

[0170]

[0179] In certain embodiments, including any of the above, the present specification provides a thin sheet comprising the cathode bilayer described herein. In certain embodiments, the cathode material is cast onto an aluminum foil (e.g., Armor) that is 100 m long x 260 mm wide x 18 μm thick. In certain embodiments, the length, width, and thickness are modified as needed. In certain embodiments, the thickness can also be modified to accommodate different substrates or different aluminum foils.

[0171]

[0180] In certain embodiments taught elsewhere herein, the cathode active loading in the cathode is about 1-15 mAh / cm 2 (e.g. 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, or 15 mAh / cm 2 In certain embodiments, including any of the foregoing, the cathode active loading is at least about 5 mAh / cm 2 It is.

[0172]

[0181] In certain embodiments taught elsewhere herein, the cathode has a thickness of 120 μm. In certain embodiments, including any of the above, the cathode has a thickness of 150 μm.

[0173]

[0182] In certain embodiments taught elsewhere herein, the cathode has a width of at least 5 centimeters (cm). In certain embodiments, the cathode has a width of at least 1 meter (m).

[0174]

[0183] In certain embodiments as otherwise taught herein, the length of the cathode is at least 10 cm. In certain embodiments, including any of the above, the length of the cathode is at least 70 cm. In certain embodiments, including any of the above, the length of the cathode is at least about 1 m.

[0175]

[0184] In a particular embodiment taught elsewhere herein, the cathode is about 100 mm by 2,000 mm.

[0176]

[0185] In a particular embodiment taught elsewhere herein, the cathode is about 150 mm by 100 mm.

[0177]

[0186] In certain embodiments taught elsewhere herein, the cathode is about 300 mm by a continuous roll.

[0178]

[0187] In certain embodiments taught elsewhere herein, the metal layer is a layer of Al.

[0179]

[0188] In certain embodiments taught elsewhere herein, the metal layer is a layer of Ni.

[0180]

[0189] In certain embodiments, the solid-state positive electrodes described elsewhere in this disclosure may be part of a solid-state battery, hi certain embodiments, such batteries are useful as power sources for electronic devices or vehicle batteries.

[0181]

[0190] In certain aspects and embodiments, the present disclosure provides a metal substrate having at least two longitudinal ends and at least two lateral ends; a cathode material disposed on a metal substrate; Providing a green bilayer comprising: the cathode material covers at least about 50% of the surface of the metal substrate but not the longitudinal ends; the longitudinal end includes one or more cuts extending from the longitudinal end to a cathode material disposed on the metal substrate; and calendering the green bilayer; A method for making a cathode is provided, comprising:

[0182]

[0191] In certain aspects and embodiments, the present disclosure provides coating a metal substrate with a cathode slurry to provide a green bilayer comprising a cathode material disposed on the metal substrate; the metal substrate having at least two longitudinal edges and at least two lateral edges; the cathode material covers at least about 50% of the surface of the metal substrate but not the longitudinal ends; calendering the green bilayer; die punching the green bilaminate to produce a cathode; A method for manufacturing a cathode is provided, comprising:

[0183]

[0192] In certain embodiments of the methods described elsewhere herein, the method further includes creating a green bilayer using a laser pattern for subsequent die punch processing.

[0184]

[0193] In certain embodiments, the use of the laser pattern is done simultaneously on both sides so that there is no offset in the resulting cuts or tabs, hi certain embodiments, the use of the laser pattern is not done simultaneously on both sides.

[0185]

[0194] In certain embodiments of the methods described elsewhere herein, the method further includes cutting the metal substrate, wherein the longitudinal end includes one or more cuts extending from the longitudinal end to the cathode material disposed on the metal substrate.

[0186]

[0195] In certain embodiments of the methods described elsewhere herein, the method further includes cutting the metal substrate, the cutting including one or more cuts at a longitudinal end, the one or more cuts extending from the longitudinal end to the cathode material disposed on the metal substrate.

[0187]

[0196] In certain embodiments of the methods described elsewhere herein, the method further includes cutting the metal substrate, the cutting including one or more cuts at the lateral edge. In certain embodiments described elsewhere herein, the one or more cuts extend from the lateral edge to the second lateral edge (e.g., FIGS. 7D and 8D). In certain embodiments, the one or more cuts are substantially parallel to the longitudinal edge.

[0188]

[0197] In certain embodiments of the methods described elsewhere herein, cutting of the metal substrate may be performed at a speed of about 0.1 m / s to 100 m / s (e.g., about 0.1, 0.15, 0.2, 0.25, 0.3, 0.35, 0.4, 0.45, 0.5, 0.6, 0.7, 0.8, 0.9, 1.0, 1.25, 1.5, 1.75, 2.0, 2.25, 2.5, 2.75, 3.0, 3.25, 3.5, 3.75, 4.0, 4.25, 4.5, 4.75, 5, 5.5, 6, 6.5, 7, 7.5, 8, 8.5, 9, 9.5, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 49, 50, 51, 52, 53, 54, 55, 56, 57, 58, 59, 60, 61, 62, 63, 64, 65, 66, 67, 68, 69, 70, 71, 72, 73, 74, 75, 76, 1, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 49, 50, 51, 52, 53, 54, 55, 56, 57, 58, 59, 60, 61, 62, 6 3, 64, 65, 66, 67, 68, 69, 70, 71, 72, 73, 74, 75, 76, 77, 78, 79, 80, 81, 82, 83, 84, 85, 86, 87, 88, 89, 90, 91, 92, 93, 94, 95, 96, 97, 98, 99, or 100 m / s).

[0189]

[0198] In certain embodiments of the methods described elsewhere herein, the use of the laser pattern occurs prior to calendaring the bilayer. In certain embodiments, the use of the laser pattern occurs prior to cutting the metal substrate. In certain embodiments, the use of the laser pattern occurs prior to cutting the metal substrate and calendaring the bilayer.

[0190]

[0199] In certain embodiments of the methods described elsewhere herein, cutting of the metal substrate occurs prior to the use of the laser pattern. In certain embodiments, cutting of the metal substrate occurs prior to calendaring of the bilayer. In certain embodiments, cutting of the metal substrate occurs prior to the use of the laser pattern and calendaring of the bilayer.

[0191]

[0200] In certain embodiments of the methods described elsewhere herein, cutting of the metal substrate occurs prior to calendering of the bilayer. In certain embodiments, calendering of the bilayer occurs prior to cutting of the metal substrate.

[0192] Exemplary embodiments

[0201] Embodiment 1. A metal foil including two longitudinal ends and two transverse ends, coated with a coating material, where the coating material does not coat the longitudinal ends and the coating material is separated by parallel or nearly parallel exposed metal foil, and the longitudinal ends include one or more cuts extending from the longitudinal ends toward the coating material.

[0193]

[0202] Embodiment 2. The metal foil of embodiment 1, wherein at least 50% of the surface of the metal foil is coated with the coating material.

[0194]

[0203] Embodiment 3. The metal foil of embodiment 1 or 2, wherein the first and third lanes are located 1 mm, 2 mm, 3 mm, 4 mm, or 5 mm from the longitudinal ends, excluding any tab features on the longitudinal ends.

[0195]

[0204] Embodiment 4. The metal foil according to any one of embodiments 1 to 3, wherein the material is coated to have a uniform average thickness of 150 μm to 250 μm after calendaring.

[0196]

[0205] Embodiment 5. The metal foil of any one of embodiments 1 to 4, wherein the coating material has a uniform average thickness.

[0197]

[0206] Embodiment 6. The metal foil of any one of embodiments 1-5, wherein at least three lanes of material disposed on the metal substrate have average thicknesses within 10-20% of each other.

[0198]

[0207] Embodiment 7. A metal substrate having at least two longitudinal ends and at least two lateral ends; at least three lanes of coating material disposed on the metal substrate; A bilayer comprising: the first and second lanes of coating material include a cathodic material; the coating material covers at least about 50% of the surface of the metal substrate but does not cover the longitudinal edges; the longitudinal end includes one or more cuts extending from the longitudinal end toward the coating material; Two-layered body.

[0199]

[0208] Embodiment 8. The bilayer of embodiment 7, wherein the at least three lanes of material disposed on the metal substrate have a uniform average thickness.

[0200]

[0209] Embodiment 9. The bilayer of embodiment 7 or 8, wherein the metal substrate having at least two longitudinal edges and at least two lateral edges is a metal foil.

[0201]

[0210] Embodiment 10. The bilayer of any one of embodiments 7-9, wherein at least three lanes of material disposed on the metal substrate have average thicknesses within 10-20% of each other.

[0202]

[0211] Embodiment 11. The bilayer of any one of embodiments 7-10, wherein the third lane of coating material comprises a cathodic material.

[0203]

[0212] Embodiment 12. The bilayer of any one of embodiments 7-10, wherein the third lane of coating material does not include a cathode material.

[0204]

[0213] Embodiment 13. A bilayer according to any one of embodiments 7 to 11, wherein the composition of the three coating material lanes is identical.

[0205]

[0214] Embodiment 14. A bilayer according to any one of embodiments 7 to 12, wherein the compositions of the three coating material lanes are not identical.

[0206]

[0215] Embodiment 15. A bilayer according to any one of embodiments 7 to 14, wherein the first and third lanes are positioned 1 to 5 mm from the longitudinal ends, excluding any tab features.

[0207]

[0216] Embodiment 16. The bilayer of any one of embodiments 7 to 15, wherein the cuts are periodically spaced.

[0208]

[0217] Embodiment 17. The bilayer of any one of embodiments 7 to 15, wherein the cuts are not periodically spaced.

[0209]

[0218] Embodiment 18. A bilayer according to any one of embodiments 7 to 17, wherein cuts are present on both longitudinal ends.

[0210]

[0219] Embodiment 19. The bilayer of any one of embodiments 7-18, wherein the cathode material coats the substrate as a patch.

[0211]

[0220] Embodiment 20. The bilayer of any one of embodiments 7 to 19, wherein the cathode material coats at least one or more lateral edges.

[0212]

[0221] Embodiment 21. The bilayer of any one of embodiments 7 to 20, wherein the cathode material further comprises a center cut parallel to the longitudinal ends.

[0213]

[0222] Embodiment 22. The bilayer of any one of embodiments 7 to 21, wherein the cut comprises one or more slits.

[0214]

[0223] Embodiment 23. The bilayer of embodiment 22, wherein the slit comprises an I-shape, an L-shape, a T-shape, or a combination thereof.

[0215]

[0224] Embodiment 24. The bilayer of embodiment 22, wherein the slit is T-shaped.

[0216]

[0225] Embodiment 25. The bilayer of any one of embodiments 7 to 21, wherein the cuts include one or more geometric shapes.

[0217]

[0226] Embodiment 26. The bilayer of embodiment 25, wherein the geometric shape comprises a triangle, a semicircle, an arch, a trapezoid, a parallelogram, or a combination thereof.

[0218]

[0227] Embodiment 27. The bilayer of embodiment 25, wherein the geometric shape comprises a trapezoid, and the trapezoid is a rectangle.

[0219]

[0228] Embodiment 28. A bilayer according to any one of embodiments 7 to 27, wherein the cuts include one or more slits and one or more geometric shapes.

[0220]

[0229] Embodiment 29. The bilayer of any one of embodiments 7-28, wherein the metal substrate has one or more perforations or depressions shaped as one or more battery tabs.

[0221]

[0230] Embodiment 30. The cathode material is at least 27 mg / cm 2 30. The bi-layer body of any one of embodiments 7 to 29, having a cathode active material loading of

[0222]

[0231] Embodiment 31. The cathode material is at least 28 mg / cm 2 31. The bilayer of embodiment 30 having a cathode active material loading of

[0223]

[0232] Embodiment 32. The cathode material is at least 29 mg / cm 2 32. The bilayer of embodiment 31 having a cathode active material loading of

[0224]

[0233] Embodiment 33. The cathode material is at least 30 mg / cm2 33. The bilayer of embodiment 32 having a cathode active material loading of

[0225]

[0234] Embodiment 34. The bilayer of any one of embodiments 7 to 33, wherein the thickness of the cathode material is less than 250 μm.

[0226]

[0235] Embodiment 35. The bilayer of embodiment 34, wherein the thickness of the cathode material is about 100 μm to 250 μm.

[0227]

[0236] Embodiment 36. The bilayer of embodiment 35, wherein the thickness of the cathode material is about 190 μm to 240 μm.

[0228]

[0237] Embodiment 37. The bilayer of embodiment 34, wherein the thickness of the cathode material is less than about 200 μm.

[0229]

[0238] Embodiment 38. The bilayer of embodiment 37, wherein the thickness of the cathode material is less than about 150 μm.

[0230]

[0239] Embodiment 39. The bilayer of embodiment 38, wherein the thickness of the cathode material is less than about 100 μm.

[0231]

[0240] Embodiment 40. The bilayer of any one of embodiments 7 to 39, wherein the cathode material has a porosity of about 25 volume percent or less.

[0232]

[0241] Embodiment 41. The bilayer of any one of embodiments 7-40, wherein the metal substrate is substantially free of edge defects.

[0233]

[0242] Embodiment 42. The bilayer of any one of embodiments 7-41, wherein the cathode is substantially free of edge defects.

[0234]

[0243] Embodiment 43. The bilayer of embodiment 41 or 42, wherein the edge defects are selected from the group consisting of cracks, bends, warping, wrinkling, peeling, and combinations thereof.

[0235]

[0244] Embodiment 44. The cathode is about 50 μm / cm 2 The bilayer body according to any one of embodiments 7 to 43, having a surface flatness of:

[0236]

[0245] Embodiment 45. The cathode is about 1 to 50 μm 2 45. The bilayer of embodiment 44, having a surface flatness of

[0237]

[0246] Embodiment 46. The bilayer body of any one of embodiments 7 to 45, wherein the metal substrate is an aluminum or aluminum alloy metal substrate.

[0238]

[0247] Embodiment 47. The bilayer of embodiment 46, wherein the metal substrate is aluminum foil.

[0239]

[0248] Embodiment 48. The bilayer body of any one of embodiments 7 to 45, wherein the metal substrate is a copper or copper alloy metal substrate.

[0240]

[0249] Embodiment 49. The bilayer body of any one of embodiments 7 to 45, wherein the metal substrate is a nickel or nickel alloy metal substrate.

[0241]

[0250] Embodiment 50. The bilayer body of any one of embodiments 7 to 49, wherein the cathode comprises a cathode active material selected from the group consisting of manganese oxide, iron oxide, copper oxide, nickel oxide, lithium-manganese composite oxide, lithium-nickel composite oxide, lithium-cobalt composite oxide, lithium-cobalt-nickel oxide, lithium-manganese-cobalt composite oxide, spinel phase lithium-manganese-nickel composite oxide, lithium phosphate having an olivine structure, lithium phosphate having a NASICON type structure, iron(III) sulfate, vanadium oxide, and combinations thereof.

[0242]

[0251] Embodiment 51. The cathode is MnO, Li x Mn2O4, Lix MnO2, Li x NiO2, Li x CoO2, LiNi (1-y) Co y O2, LiMn y Co (1-y) O2, Li x Mn (2-y) Ni y O4, Li x FePO4, Li x Fe (1-y) Mn y PO4, Li x 51. The bi-layer of embodiment 50, comprising a cathode active material selected from the group consisting of CoPO4, Li7V2(PO4)3, Fe2(SO4)3, V2O5, and combinations thereof, where 1≦x≦5 and 0≦y≦1.

[0243]

[0252] Embodiment 52. The cathode is LiMPO4 (M=Fe, Ni, Co, Mn); Li x Ti y O z (x is 0 to 8, y is 1 to 12, and z is 1 to 24);LiMn 2a Ni a O4 (where a is 0 to 2); Nickel cobalt aluminum oxide; LiNi x Mn y Co z O2(x+y+z=1, 0≦x≦1, 0≦y≦1, 0≦z≦1); and LiNi x Co y Al z 52. The bilayer of any one of embodiments 7-51, comprising a cathode active material selected from the group consisting of O2(x+y+z=1, 0≦x≦1, 0≦y≦1, 0≦z≦1).

[0244]

[0253] Embodiment 53. The cathode is a cathode active material LiNi x Mn y Co z 51. The bilayer of embodiment 50, comprising O2(NMC)(0≦x≦1, 0≦y≦1, 0≦z≦1, x+y+z=1).

[0245]

[0254] Embodiment 54. The bilayer of embodiment 53, wherein x is 0.8, y is 0.1, and z is 0.1.

[0246]

[0255] Embodiment 55. The bilayer of embodiment 53, wherein x is 0.6, y is 0.2, and z is 0.2.

[0247]

[0256] Embodiment 56. The bilayer of embodiment 53, wherein x is 0.5, y is 0.3, and z is 0.2.

[0248]

[0257] Embodiment 57. The bilayer of embodiment 53, wherein x is 1 / 3, y is 1 / 3, and z is 1 / 3.

[0249]

[0258] Embodiment 58. NMC is 0.1 μm <S<50μmのd 50 58. The bilayer of any one of embodiments 53 to 57, having a particle size S.

[0250]

[0259] Embodiment 59. NMC is 0.5 μm <S<30μmのd 50 59. The bilayer of embodiment 58 having a particle size S.

[0251]

[0260] Embodiment 60. NMC is 1 μm <S<20μmのd 50 60. The bilayer of embodiment 59 having a particle size S.

[0252]

[0261] Embodiment 61. The bilayer of any one of embodiments 7 to 60, wherein the edge of the cut is about 0 to 6 mm from the edge of the cathode material.

[0253]

[0262] Embodiment 62. The bilayer of any one of embodiments 7 to 61, wherein the distance between the end of the first cut and the end of the second adjacent cut is about 5 mm to 75 mm from the end of the cathode material.

[0254]

[0263] Embodiment 63. A metal substrate having at least two longitudinal ends and at least two lateral ends; a cathode material disposed on a metal substrate; A green bilayer comprising: the cathode material covers at least about 50% of the surface of the metal substrate but not the longitudinal ends; the longitudinal end includes one or more cuts extending from the longitudinal end to the cathode material; Green double layer.

[0255]

[0264] Embodiment 64. The green bilayer of embodiment 63, wherein the cuts are periodically spaced.

[0256]

[0265] Embodiment 65. The green bilayer of embodiment 63 or 64, wherein the cathode material covers at least one or more lateral edges.

[0257]

[0266] Embodiment 66. The green bilayer of any one of embodiments 63-65, wherein the cuts include one or more slits.

[0258]

[0267] Embodiment 67. The green bilayer of embodiment 66, wherein the slit comprises an I-shape, an L-shape, a T-shape, or a combination thereof.

[0259]

[0268] Embodiment 68. A green bilayer according to any one of embodiments 63 to 67, wherein the slit is T-shaped.

[0260]

[0269] Embodiment 69. The green bilayer of any one of embodiments 63-65, wherein the cuts include one or more geometric shapes.

[0261]

[0270] Embodiment 70. The green bilayer of embodiment 69, wherein the geometric shape comprises a triangle, a semicircle, an arch, a trapezoid, a parallelogram, or a combination thereof.

[0262]

[0271] Embodiment 71. The green bilayer of embodiment 70, wherein the geometric shape comprises a trapezoid, and the trapezoid is a rectangle.

[0263]

[0272] Embodiment 72. A bilayer according to any one of embodiments 66 to 71, wherein the cuts include one or more slits and one or more geometric shapes.

[0264]

[0273] Embodiment 73. The green bilayer of any one of embodiments 63-72, wherein the metal substrate has one or more perforations or depressions shaped as one or more battery tabs.

[0265]

[0274] Embodiment 74. The green bilayer of any one of embodiments 63 to 73, wherein the thickness of the cathode material is about 100 μm to 250 μm.

[0266]

[0275] Embodiment 75. The green bilayer of any one of embodiments 63-74, wherein the cathode is substantially free of edge defects.

[0267]

[0276] Embodiment 76. The green bilayer of any one of embodiments 63-74, wherein the edge defects are selected from the group consisting of cracks, bends, warping, wrinkling, peeling, and combinations thereof.

[0268]

[0277] Embodiment 77. The green bilayer of any one of embodiments 63-76, wherein at least three lanes of coating material are disposed on the metal substrate, and a first and second lane of coating material comprises a cathode material.

[0269]

[0278] Embodiment 78. A metal substrate having at least two longitudinal ends and at least two lateral ends; a cathode material disposed on a metal substrate; Providing a green bilayer comprising: the longitudinal end including one or more cuts extending from the longitudinal end to a cathode material disposed on the metal substrate; and calendering the green bilayer at a temperature of less than 100°C; A method for manufacturing a cathode, comprising:

[0270]

[0279] Embodiment 79 The method of embodiment 78, further comprising heating the bilayer.

[0271]

[0280] Embodiment 80 The method of embodiment 78 or 79, further comprising heating the bilayer to a temperature less than 75° C.

[0272]

[0281] Embodiment 81. The method of any one of embodiments 78 to 80, further comprising calendering the cathode at a pressure of at least about 50 MPa.

[0273]

[0282] Embodiment 82. The method of any one of embodiments 78-81, further comprising die punching the bilayer.

[0274]

[0283] Embodiment 83. The cathode material has a cathode active material loading of at least 29 mg / cm 2 The method of any one of embodiments 78 to 82, wherein

[0275]

[0284] Embodiment 84. The method of any one of embodiments 78 to 83, wherein the thickness of the cathode material is reduced to between about 240 μm and 190 μm.

[0276]

[0285] Embodiment 85. The method of any one of embodiments 78-84, wherein the porosity of the cathode material is reduced to about 25% or less.

[0277]

[0286] Embodiment 86 The method of any one of embodiments 78 to 85, wherein the variation in surface flatness of the cathode after calendaring is about 50 μm or less.

[0278]

[0287] Embodiment 87. The method of any one of embodiments 78 to 86, wherein the calendaring step has two active rollers.

[0279]

[0288] Embodiment 88. The method of any one of embodiments 78-87, further comprising die punching the green bilayer to produce a cathode.

[0280]

[0289] Embodiment 89. The method of any one of embodiments 78-88, further comprising using a laser pattern to create a green bilayer for subsequent die punch processing.

[0281]

[0290] Embodiment 90. The method of any one of embodiments 78-89, further comprising cutting the metal substrate, the cutting comprising one or more cuts at a longitudinal end, the one or more cuts extending from the longitudinal end to the cathode material disposed on the metal substrate.

[0282]

[0291] Embodiment 91. The method of any one of embodiments 78 to 90, wherein the calendaring step has two active rollers.

[0283]

[0292] Embodiment 92. The method of any one of embodiments 78-91, wherein the cathode material covers at least about 50% of the surface of the metal substrate but does not cover the longitudinal ends.

[0284]

[0293] Embodiment 93. The method of any one of embodiments 78-92, wherein the green bilayer comprises at least three lanes of coating material disposed on the metal substrate, and a first and second lane of coating material comprises a cathode material. EXAMPLES

[0285] Working Example

[0294] The symbols and conventions employed in the methods, schemes, and examples used herein are consistent with those used in the current scientific literature, regardless of whether a particular abbreviation is specifically defined.

[0286] Example 1A - Basic Preparation of Cathode and Current Collector

[0295] For the fabrication of an exemplary high energy density cathode / current collector useful in the present invention, the cathode is cast onto aluminum foil (Armor) measuring 100 mm long by 260 mm wide by 18 μm thick.

[0287]

[0296] Solids: (a) 90-98% w / w of active material (e.g. high nickel content NMC, NCA, NMO, LCO, or LFP; 95-96 high nickel content NMC, etc.); (b) 0.1-3% w / w of binder (e.g. PVDF-based polymer or PVDF-based copolymer, e.g. Kurcha 9700); (c) 1-3% w / w of carbon (with a surface area of ​​30-2000 m 2 / g, e.g., C65); and (d) a surfactant (e.g., a functionalized PVDF polymer, polyvinyl alcohol, polyamine, polyacrylate, polyurethane, polystyrene, or any combination thereof, e.g., Zeon BM-740H). The sum of a+b+c+d is 100%. The solvent for the slurry is NMP.

[0288]

[0297] The slurry is mixed in a multi-step process and cast using a die coating system and doctor blade casting with a roll-to-roll casting method. In one embodiment, the target loading is about 29 mg / cm 2 The initial thickness of the electrode after casting the slurry was about 245 μm to about 280 μm.

[0289]

[0298] After coating, the electrode is dried by a multi-stage drying process. In some embodiments, the temperatures of each stage are 80° C., 100° C., and 110° C., and the cathode passes through each stage at a speed of 1 m / min. The electrode is held at 110° C. for 8 hours. After these stages, the entire roll is dried again in an oven at 110° C. under a N2 purge for 8 hours.

[0290]

[0299] After drying, the electrodes are calendered (e.g., using an ONO calendering tool) from their initial thickness to a final thickness of approximately 180-200 µm, based on the final desired porosity.

[0291] Example 1B - Preparation of Exemplary Cathode 1

[0300] A slurry containing solids of (a) 91% w / w NMC active material, (b) 5.0% w / w PVDF-based functionalized binder, (c) 3.0% w / w carbon black, and (d) 1.0% w / w Ketjen black was prepared in NMP solvent and then cast onto a carbon-coated aluminum foil measuring 100 mm long by 260 mm wide and approximately 18-21 μm thick.

[0292]

[0301] After coating, the electrodes were dried by a multi-stage drying process, where the temperatures for each stage were 80°C, 100°C, and 110°C, and the cathode passed through each stage at a speed of 1 m / min. The electrodes were held at 110°C for 8 hours. After these stages, the entire roll was dried again in an oven at 110°C for 8 hours under a N2 purge.

[0293]

[0302] After drying, the electrodes were calendered (e.g., using an ONO calendering tool) from the initial thickness to a final thickness of approximately 180-200 μm, based on the final porosity required.

[0294]

[0303] The cathode was cast onto an aluminum foil (Armor) measuring 100 mm long x 260 mm wide x 18 μm thick.

[0295]

[0304] Slurries were prepared containing solids of (a) 95-96% w / w active material (i.e., high nickel content NMC), (b) 1-3% w / w binder (Kureha 9700), (c) 1-3% w / w carbon (C65), and (d) surfactant (Zeon BM-740H). The sum of a+b+c+d was 100%. The slurry solvent was NMP.

[0296]

[0305] The slurry was mixed in a multi-step process and cast using a die coating system and doctor blade casting with a roll-to-roll casting method. The target loading was about 29 mg / cm. 2 The initial thickness of the electrode after casting the slurry was about 245 μm to about 280 μm.

[0297]

[0306] After coating, the electrodes were dried by a multi-stage drying process, where the temperatures for each stage were 80°C, 100°C, and 110°C, and the cathode passed through each stage at a speed of 1 m / min. The electrodes were held at 110°C for 8 hours. After these stages, the entire roll was dried again in an oven at 110°C for 8 hours under a N2 purge.

[0298]

[0307] After drying, the electrodes were calendered from their initial thickness to a final thickness of approximately 180–200 μm using an ONO calendering tool, based on the final desired porosity.

[0299] Example 2 - Preparation of Exemplary Cathode 2

[0308] A slurry containing solids of (a) 95% w / w NMC active material, (b) 2.3% w / w PVDF-based functionalized binder, and (c) 2.7% w / w carbon black was prepared in NMP solvent. The slurry was then cast onto an aluminum foil measuring 100 mm long x 260 mm wide x 18 μm thick. The coated electrode was then dried and calendered according to the method described in Example 1A.

[0300] Example 3 - Preparation of Exemplary Cathode 3

[0309] A slurry containing solids of (a) 96% w / w NMC active material, (b) 2.3% w / w PVDF-based non-functionalized binder, and (c) 2.7% w / w carbon black was prepared in NMP solvent. The slurry was then cast onto an aluminum foil measuring 100 mm long x 260 mm wide x 18 μm thick. The coated electrode was then dried and calendered according to the method described in Example 1A.

[0301] Example 4 - Preparation of Exemplary Cathode 4

[0310] A slurry containing solids of (a) 96% w / w NMC active material, (b) 2.0% w / w PVdF-based functionalized binder, and (c) 2.0% w / w carbon black was prepared in NMP solvent. The slurry was then cast onto an aluminum foil measuring 100 mm long x 260 mm wide x 18 μm thick. The coated electrode was then dried and calendered according to the method described in Example 1A.

[0302] Example 5 - Preparation of Exemplary Cathode 5

[0311] A slurry containing solids of (a) 96% w / w NMC active material, (b) 2.0% w / w PVdF-based functionalized binder, and (c) 2.0% w / w carbon black was prepared in NMP solvent. The slurry was then cast onto a carbon-coated aluminum foil measuring 100 mm long x 260 mm wide x 18-21 μm thick. The coated electrode was then dried and calendered according to the method described in Example 1A.

[0303] Example 6 - Fabrication of a wrinkle-free cathode

[0312] To produce wrinkle-free cathodes, the cathode slurries of Examples 1B-5 were used to coat foils to form coated foils with three cathode slurry lanes. The bilayer was then laser notched and then calendered at a speed of about 2 m / min and a temperature of less than 100° C. The pressure during calendering was 2-10 tons per side. A slitter was then used to cut the foil between the notch areas of the calendered cathode, and a die punch was used to punch out wrinkle-free cathodes.

[0304]

[0313] When less than 3 lanes of coating were used, wrinkling was evident. When 3 lanes of coating were used, wrinkling was absent / reduced. By maintaining a consistent average height across the aluminum foil using 3 lanes, no wrinkling was observed.

[0305] Example 7 - Procedure for reducing burrs

[0314] To investigate the effect of edge width on wrinkling and burrs, comparative experiments were prepared with different cathodes (Figure 4). Cathodes with 5 mm, 2 mm, 1 mm, and 0.5 mm metal edges on the lateral edges of the cathode coating material were prepared, and the metal edges were removed. The results showed that larger metal edges resulted in more wrinkling of the cathode material, and smaller metal edges resulted in more burrs. However, the effect of burrs at 0.5 mm was not as severe as the effect of wrinkling at 5 mm.

[0306]

[0315] The above-described embodiments and examples are intended to be illustrative and not limiting. Those skilled in the art will recognize, or be able to ascertain using no more than routine experimentation, numerous equivalents to the specific compounds, materials, and procedures. All such equivalents are within the scope of the appended claims and are considered to be encompassed by the claims.

[0307]

[0316] All publications, patents, and applications cited in this specification are incorporated by reference herein as if each individual publication or patent application was specifically and individually indicated to be incorporated by reference. Although the claimed subject matter has been described in terms of various embodiments, those skilled in the art will understand that various modifications, substitutions, omissions, and changes can be made therein without departing from the spirit thereof. Accordingly, it is intended that the scope of the subject matter be limited only by the scope of the following claims, including equivalents thereof.

Claims

1. a metal substrate having at least two longitudinal ends and at least two lateral ends; at least three lanes of coating material disposed on said metal substrate; A bilayer comprising: the first and second lanes of coating material include a cathodic material; the longitudinal end includes one or more cuts extending from the longitudinal end toward the coating material; Two-layered body.

2. 10. The bilayer of claim 1, wherein the coating material covers at least about 50% of the surface of the metal substrate but does not cover the longitudinal edges.

3. 3. The bilayer of claim 1 or 2, wherein the third lane of slurry material comprises a cathode material.

4. 3. The bilayer of claim 1 or 2, wherein the third lane of coating material does not include a cathode material.

5. The bilayer of any one of claims 1 to 4, wherein the composition of the three coating material lanes is the same.

6. The bilayer of any one of claims 1 to 4, wherein the compositions of the three coating material lanes are not the same.

7. 7. The bilayer of any one of claims 1 to 6, wherein the first and third lanes are located 1 to 5 mm from the longitudinal ends, excluding any tab features.

8. The bilayer of any one of claims 1 to 7, wherein the cuts are periodically spaced.

9. The bilayer of any one of claims 1 to 7, wherein the cuts are not periodically spaced.

10. The bilayer according to any one of claims 1 to 9, wherein the cuts are present on both longitudinal ends.

11. The bilayer of any one of claims 1 to 10, wherein the cathode material coats the substrate as a patch.

12. The bilayer of any one of claims 1 to 11, wherein the cathode material further comprises a center cut parallel to the longitudinal ends.

13. The bilayer of any one of claims 1 to 12, wherein the cut comprises one or more slits.

14. 14. The bilayer of claim 13, wherein the slit comprises an I-shape, an L-shape, a T-shape, or a combination thereof.

15. The bilayer of any one of claims 1 to 12, wherein the cuts comprise one or more geometric shapes.

16. 16. The bilayer of claim 15, wherein the geometric shape comprises a triangle, a semicircle, an arch, a trapezoid, a parallelogram, or a combination thereof.

17. The bilayer of any one of claims 1 to 16, wherein the metal substrate has one or more perforations or depressions shaped as one or more battery tabs.

18. The cathode material has a thickness of at least 27 mg / cm ２ The bilayer body of any one of claims 1 to 17, having a cathode active material loading of

19. The bilayer of any one of claims 1 to 18, wherein the cathode material has a thickness of less than 250 μm.

20. 20. The bilayer of claim 19, wherein the cathode material has a thickness of less than about 150 μm.

21. The bilayer of any one of claims 1 to 20, wherein the cathode material has a porosity of about 25% by volume or less.

22. The bilayer of any one of claims 1 to 21, wherein the cathode is substantially free of edge defects.

23. The cathode is about 50 μm / cm ２ The bilayer body according to any one of claims 1 to 22, having a surface flatness of:

24. The bilayer body according to any one of claims 1 to 23, wherein the metal substrate is an aluminum or aluminum alloy metal substrate.

25. 25. The bilayer of claim 24, wherein the metal substrate is an aluminum foil.

26. The bilayer body according to any one of claims 1 to 25, wherein the cathode comprises a cathode active material selected from the group consisting of manganese oxide, iron oxide, copper oxide, nickel oxide, lithium-manganese composite oxide, lithium-nickel composite oxide, lithium-cobalt composite oxide, lithium-cobalt-nickel oxide, lithium-manganese-cobalt composite oxide, spinel phase lithium-manganese-nickel composite oxide, lithium phosphate having an olivine structure, lithium phosphate having a NASICON structure, iron (III) sulfate, vanadium oxide, and combinations thereof.

27. The cathode is LiMPO ４ (M=Fe, Ni, Co, Mn); Li ｘ Ti ｙ O ｚ (x is 0 to 8, y is 1 to 12, and z is 1 to 24); LiMn ２ａ Ni ａ O ４ (where a is 0 to 2); nickel cobalt aluminum oxide; LiNi ｘ Mn ｙ Co ｚ O ２ (x+y+z=1, 0≦x≦1, 0≦y≦1, 0≦z≦1); and LiNi ｘ Co ｙ A ｚ O ２ 27. The bilayer of any one of claims 1 to 26 comprising a cathode active material selected from the group consisting of: (x+y+z=1, 0≦x≦1, 0≦y≦1, 0≦z≦1).

28. The cathode is the cathode active material LiNi ｘ Mn ｙ Co ｚ O ２ 28. The bilayer of claim 27 comprising (NMC)(0≦x≦1, 0≦y≦1, 0≦z≦1, x+y+z=1).

29. The NMC is 0.1 μm<S<50 μm. ５０ 30. The bilayer of claim 28 having a particle size S.

30. 30. The bilayer of any one of claims 1 to 29, wherein the end of the cut is about 0-6 mm from the end of the cathode material.

31. a metal substrate having at least two longitudinal ends and at least two lateral ends; a cathode material disposed on the metal substrate; A green bilayer comprising: the cathode material covers at least about 50% of a surface of the metal substrate but not the longitudinal ends; the longitudinal end includes one or more cuts extending from the longitudinal end to the cathode material; Green double layer.

32. 32. The green bilayer of claim 31 , wherein the cut comprises one or more slits.

33. 33. The green bilayer of claim 32, wherein the slit comprises an I-shape, an L-shape, a T-shape, or a combination thereof.

34. 32. The green bilayer of claim 31 , wherein the cuts include one or more geometric shapes.

35. 35. The green bilayer of claim 34, wherein the geometric shape comprises a triangle, a semicircle, an arch, a trapezoid, a parallelogram, or a combination thereof.

36. 36. The green bilayer of any one of claims 31 to 35, wherein the metal substrate has one or more perforations or depressions shaped as one or more battery tabs.

37. 37. The green bilayer of any one of claims 31 to 36, wherein the cathode material has a thickness of about 100 μm to 250 μm.

38. 38. The green bilayer of any one of claims 31 to 37, wherein at least three lanes of coating material are disposed on the metal substrate, a first and second lane of coating material comprising a cathodic material.

39. a metal substrate having at least two longitudinal ends and at least two lateral ends; a cathode material disposed on the metal substrate; Providing a green bilayer comprising: the longitudinal end including one or more cuts extending from the longitudinal end to the cathode material disposed on the metal substrate; and calendering said green bilayer at a temperature of less than 100°C; A method for manufacturing a cathode, comprising:

40. 40. The method of claim 39, further comprising heating the bilayer.

41. 41. The method of claim 39 or 40, further comprising heating the bilayer to a temperature less than 75°C.

42. The method of any one of claims 39 to 41, further comprising calendering the cathode at a pressure of at least about 50 MPa.

43. The method of any one of claims 39 to 42, further comprising die punching the bilayer.

44. A method according to any one of claims 39 to 43, wherein the thickness of the cathode material is reduced to between about 240 μm and 190 μm.

45. The method of any one of claims 39 to 44, wherein the porosity of the cathode material is reduced to about 25% or less.

46. The method of any one of claims 39 to 45, further comprising die punching the green bilaminate to produce the cathode.

47. 47. The method of any one of claims 39 to 46, further comprising preparing the green bilayer using a laser pattern for subsequent die punch processing.

48. 48. The method of any one of claims 39 to 47, further comprising cutting the metal substrate, the cutting comprising one or more cuts at a longitudinal end, the one or more cuts extending from a longitudinal end to the cathode material disposed on the metal substrate.

49. The method of any one of claims 39 to 48, wherein the cathode material covers at least about 50% of the surface of the metal substrate but does not cover the longitudinal ends.

50. 50. The method of any one of claims 39-49, wherein the green bilayer comprises at least three lanes of coating material disposed on the metal substrate, a first and second lane of coating material comprising the cathode material.

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