Gasket structure and method for manufacturing all-solid-state batteries using same

Abstract

The present invention relates to a gasket structure and a method for manufacturing all-solid-state batteries using same. More specifically, the gasket structure comprises: a removable film; an adhesive layer disposed on the removable film and having a first line that separates along a first direction; and a gasket disposed on the adhesive layer and having a second line that separates along the first direction, wherein the adhesive layer comprises first openings, the gasket comprises second openings, the removable film comprises thirds openings, and the first, second, and third openings overlap on top of each other.

Description

Gasket structure and method for manufacturing an all-solid-state battery using the same

[0001] The present invention relates to a gasket structure and a method for manufacturing an all-solid-state battery using the same, and more specifically, to a gasket structure for manufacturing an all-solid-state battery and a method for manufacturing an all-solid-state battery using the same.

[0002] Recent industrial demands have led to the active development of batteries with high energy density and safety. For example, lithium-ion batteries are being used not only in information and communication devices, but also in the automotive sector. Safety is particularly important in the automotive sector, as it is directly related to life.

[0003] Recently, all-solid-state batteries, which replace the electrolyte with a solid electrolyte, have been proposed. By eliminating the use of flammable organic dispersion media, all-solid-state batteries significantly reduce the risk of fire or explosion in the event of a short circuit. Therefore, these all-solid-state batteries can significantly improve safety compared to lithium-ion batteries that use electrolytes.

[0004] The problem to be solved by the present invention is to provide a gasket structure that can easily transport a gasket having a thin thickness and increase the productivity of a cell.

[0005] Another problem to be solved by the present invention is to provide a method for manufacturing an all-solid-state battery that can improve the problem of the steps on the side of an all-solid-state battery being easily damaged when manufacturing an all-solid-state battery by laminating and pressing a positive electrode laminate and a negative electrode laminate having different areas.

[0006] A gasket structure according to one embodiment of the present invention comprises: a removable film; an adhesive layer positioned on the removable film and having a first line separated in a first direction; and a gasket positioned on the adhesive layer and having a second line separated in the first direction; wherein the adhesive layer includes a first opening, the gasket includes a second opening, and the removable film includes a third opening, and in a plan view, the first opening, the second opening, and the third opening can overlap each other.

[0007] According to another embodiment of the present invention, a gasket structure comprises: a removable film; an adhesive layer positioned on the removable film and having a first line separated in a first direction; a gasket positioned on the adhesive layer and having a second line separated in the first direction; and a carrier film positioned on the gasket; wherein the adhesive layer includes a first opening, the gasket includes a second opening, and in a plan view, the first opening and the second opening overlap each other, and the adhesive layer can have an adhesive strength at 15°C to 35°C.

[0008] According to another embodiment of the present invention, a method for manufacturing an all-solid-state battery comprises: forming a positive electrode laminate by stacking a first solid electrolyte layer on a positive electrode layer and then applying a first pressure; forming a negative electrode laminate by stacking a second solid electrolyte layer on a negative electrode layer and then applying a second pressure; bonding a gasket structure on the negative electrode laminate; providing the positive electrode laminate on the gasket structure; and joining the positive electrode laminate and the negative electrode laminate so that the first solid electrolyte layer and the second solid electrolyte layer are in contact with each other; wherein the gasket structure comprises: a removable film; an adhesive layer positioned on the removable film and having a first line separated in a first direction; and a gasket positioned on the adhesive layer and having a second line separated in the first direction; wherein the adhesive layer includes a first opening, and the gasket includes a second opening, and in a plan view, the first opening and the second opening can overlap each other.

[0009] A gasket structure according to one embodiment of the present invention can easily transport a gasket having a thin thickness. Furthermore, the gasket structure can transport multiple gaskets simultaneously. As a result, the gasket structure can increase cell productivity.

[0010] A method for manufacturing an all-solid-state battery according to one embodiment of the present invention can prevent damage to an all-solid-state battery when manufacturing an all-solid-state battery by laminating a positive electrode laminate and a negative electrode laminate having different areas by using the above-described gasket structure.

[0011] FIG. 1 is a plan view of an all-solid-state battery according to embodiments of the present invention.

[0012] Fig. 2 is a cross-sectional view of an all-solid-state battery according to embodiments of the present invention. Fig. 2 is a cross-sectional view taken along line A-A' of Fig. 1.

[0013] FIG. 3 is a cross-sectional view of an all-solid-state battery including a gasket structure according to embodiments of the present invention.

[0014] FIG. 4 is a perspective view of a gasket structure according to embodiments of the present invention.

[0015] FIGS. 5 and 6 are cross-sectional views and bottom views of a gasket structure according to one embodiment of the present invention.

[0016] Figures 7 to 10 are cross-sectional views of a gasket structure according to another embodiment of the present invention.

[0017] Figure 11 is a flowchart of a method for manufacturing an all-solid-state battery according to embodiments of the present invention.

[0018] FIG. 12a, FIG. 12b, FIG. 13a, FIG. 13b, FIG. 13c, and FIG. 13d are cross-sectional views illustrating a method for manufacturing an all-solid-state battery according to one embodiment of the present invention.

[0019] FIGS. 14a, 14b, 14c, 15a, 15b, and 15c are cross-sectional views illustrating a method for manufacturing an all-solid-state battery according to another embodiment of the present invention.

[0020] FIG. 16 is a cross-sectional view illustrating a method for manufacturing a bi-cell and stack cell all-solid-state battery according to embodiments of the present invention.

[0021] To fully understand the structure and effects of the present invention, preferred embodiments of the present invention will be described with reference to the accompanying drawings. However, the present invention is not limited to the embodiments disclosed below, but can be implemented in various forms and subject to various modifications. However, the description of these embodiments is provided solely to ensure a complete disclosure of the present invention and to fully inform those skilled in the art of the invention of the scope of the invention.

[0022] In this specification, when a component is referred to as being on another component, it means that it can be formed directly on the other component, or a third component may be interposed between them. Furthermore, in the drawings, the thicknesses of the components are exaggerated for the sake of clarity. Parts designated by the same reference numerals throughout the specification represent the same components.

[0023] Embodiments described herein will be described with reference to cross-sectional and / or plan views, which are ideal illustrations of the present invention. In the drawings, the thicknesses of films and regions are exaggerated for the purpose of effectively explaining the technical contents. Accordingly, the regions illustrated in the drawings have a schematic nature, and the shapes of the regions illustrated in the drawings are intended to illustrate specific shapes of regions of the device and are not intended to limit the scope of the invention. Although terms such as first, second, and third are used to describe various components in various embodiments of the present specification, these components should not be limited by such terms. These terms are used only to distinguish one component from another. The embodiments described and illustrated herein also include complementary embodiments thereof.

[0024] The terminology used herein is for the purpose of describing embodiments and is not intended to limit the present invention. In this specification, the singular also includes the plural unless specifically stated otherwise. As used herein, the words "comprises" and / or "comprising" do not exclude the presence or addition of one or more other components.

[0025] In this specification, "adhesion" may refer to a state in which different materials are held together by a bonding force between their interfaces. Through adhesion, two materials can adhere to each other and achieve a holding force that prevents them from separating. Adhesion, in a broad sense, may include tackiness.

[0026] In this specification, 'pressure-sensitive adhesion' may refer to a phenomenon (tendency) in which two different objects (excluding gases) attract each other after they come into proximity or contact. In other words, adhesion may refer to a phenomenon in which some force (or work) is required to separate two different objects (excluding gases) after they come into proximity or contact. Adhesion may be continuously releasable.

[0027] In this specification, 'viscoelasticity' may refer to a phenomenon in which, when a force is applied to an object, both a non-restoring flow and a restoring elastic deformation occur simultaneously. A material with viscoelasticity can simultaneously exhibit the properties of both a solid and a liquid.

[0028]

[0029] Fig. 1 is a plan view of an all-solid-state battery according to embodiments of the present invention. Fig. 2 is a cross-sectional view taken along line A-A' of Fig. 1.

[0030] Referring to FIG. 1, an all-solid-state battery (10) according to one embodiment may include a positive electrode layer (100), a negative electrode layer (200) facing the positive electrode layer (100), and a solid electrolyte layer (300) disposed between the positive electrode layer (100) and the negative electrode layer (200). However, the present invention is not limited thereto, and the all-solid-state battery (10) may further include an additional functional layer, such as an adhesion enhancing layer, disposed between the positive electrode layer (100) and the solid electrolyte layer (300) or between the negative electrode layer (200) and the solid electrolyte layer (300).

[0031] The positive electrode layer (100) of one embodiment may include a positive electrode current collector (110) and a positive electrode active material layer (120) disposed on the positive electrode current collector (110). The positive electrode active material layer (120) may include a positive electrode active material, a solid electrolyte, a conductive material, and a binder.

[0032] The positive electrode current collector (110) can provide a reference surface on which the positive electrode active material layer (120) is arranged. The positive electrode current collector (110) can include a plate or foil including, for example, indium (In), copper (Cu), magnesium (Mg), stainless steel, titanium (Ti), iron (Fe), cobalt (Co), nickel (Ni), zinc (Zn), aluminum (Al), germanium (Ge), lithium (Li), or an alloy thereof.

[0033] Meanwhile, although not shown, a carbon layer having a thickness of 0.1 μm to 4 μm may be additionally placed between the positive electrode current collector (110) and the positive electrode active material layer (120) to increase the bonding strength between the positive electrode current collector (110) and the positive electrode active material layer (120).

[0034] The cathode active material may include a material that can reversibly absorb and desorb lithium ions. The cathode active material may include a plurality of particles. The cathode active material may include, but is not necessarily limited to, lithium transition metal oxides such as lithium cobalt oxide (LCO), lithium nickel oxide, lithium nickel cobalt oxide, lithium nickel cobalt aluminum oxide (NCA), lithium nickel cobalt manganese oxide (NCM), lithium manganate, and lithium iron phosphate, nickel sulfide, copper sulfide, lithium sulfide, iron oxide, or vanadium oxide. The cathode active materials may be used alone or as a mixture of two or more.

[0035] Lithium transition metal oxides include, for example, Li a A 1-b B b D2(0.90≤a≤1, 0≤b≤0.5), Li a E 1-b B b O 2-c D c (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05), LiE 2-b B b O 4-c D c (0≤b≤0.5, 0≤c≤0.05), Li a Ni 1-b-c Co b B c D α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α<2), Li a Ni 1-b-c Co b B c O 2-α F α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α<2), Li a Ni 1-b-c Mn b B c D α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α≤2), Li a Ni 1-b-c Mn b B c O 2-α F α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α<2), Li a Ni b E c G d O2(0.90≤a≤1, 0≤b≤0.9, 0≤c≤0.5, 0.001≤d≤0.1), Li a Ni b Co c Mn d GeO2(0.90≤a≤1, 0≤b≤0.9, 0≤c≤0.5, 0≤d≤0.5, 0.001≤e≤0.1), Li a NiG bO2(0.9≤a≤1, 0.001≤b≤0.1), Li a CoG b O2(0.90≤a≤1, 0.001≤b≤0.1), Li a MnG b O2(0.90≤a≤1, 0.001≤b≤0.1), Li a Mn2GbO4(0.90≤a≤1, 0.001≤b≤0.1), QO2, QS2, LiQS2, V2O5, LiV2O5, LiIO2, LiNiVO4, Li 3-f J2(PO4)3(0≤f≤2), Li 3-f A compound represented by any one of Fe2(PO4)3(0≤f≤2), LiFePO4. In these compounds, the capital letter “A” is Ni, Co, Mn, or a combination thereof, the capital letter “B” is Al, Ni, Co, Mn, Cr, Fe, Mg, Sr, V, a rare earth element, or a combination thereof, the capital letter “D” is O, F, S, P, or a combination thereof, the capital letter “E” is Co, Mn, or a combination thereof, the capital letter “F” is F, S, P, or a combination thereof, the capital letter “G” is Al, Cr, Mn, Fe, Mg, La, Ce, Sr, V, or a combination thereof, the capital letter “Q” is Ti, Mo, Mn, or a combination thereof, the capital letter “I” is Cr, V, Fe, Sc, Y, or a combination thereof, and the capital letter “J” is V, Cr, Mn, Co, Ni, Cu, or a combination thereof.

[0036] The cathode active material may include, for example, a lithium salt of a transition metal oxide having a layered rock salt type structure among the lithium transition metal oxides described above. The "layered rock salt type structure" is, for example, a cubic rock salt type structure. <111> It is a structure in which oxygen atomic layers and metal atomic layers are alternately and regularly arranged in a direction, and thereby each atomic layer forms a two-dimensional plane. The "cubic rock salt structure" refers to the sodium chloride type (NaCl type) structure, which is a type of crystal structure, and specifically refers to a structure in which the face-centered cubic lattice (fcc) formed by each cation and anion is arranged with a displacement of half of the ridge of the unit lattice. Lithium transition metal oxides having this layered rock salt structure include, for example, LiNi x Co y Al z O2(NCA) or LiNi x Co y Mn z O2(NCM) (0 <x<1,0<y<1, 0<z<1, x+y+z=1) 등의 삼원계 리튬전이금속산화물일 수 있다. 양극 활물질이 층상암염형 구조를 갖는 삼원계 리튬전이금속산화물을 포함하는 경우, 전고체 전지(10)의 에너지 밀도가 커지고 열안정성이 향상될 수 있다.

[0037] The above-described compound included in the positive electrode active material may be covered by a coating layer (not shown). The positive electrode active material may also be a mixture of the above-described compound and a compound to which a coating layer is added. Meanwhile, the coating layer added to the surface of the positive electrode active material may include, for example, an oxide, a hydroxide, an oxyhydroxide, an oxycarbonate, or a hydroxycarbonate of the coating elements below. The compound forming the coating layer is amorphous or crystalline. The coating elements included in the coating layer may include Mg, Al, Co, K, Na, Ca, Si, Ti, V, Sn, Ge, Ga, B, As, Zr, or mixtures thereof. The coating layer may include, for example, Li2O-ZrO2 (LZO). The method for forming the coating layer is selected within a range that does not adversely affect the physical properties of the positive electrode active material (PAM). The method for forming the coating layer includes, for example, spray coating, dipping, etc.

[0038] When the positive electrode active material includes nickel (Ni) as a ternary lithium transition metal oxide such as NCA or NCM, for example, the capacity density of the all-solid-state battery (10) can be increased, thereby reducing metal dissolution of the positive electrode active material (PAM) in a charged state. As a result, the cycle characteristics of the all-solid-state battery (10) in a charged state are improved. Meanwhile, the "cycle characteristics" are characteristics indicating the degree to which the all-solid-state battery (10) is deteriorated by charge / discharge of the all-solid-state battery (10). An all-solid-state battery (10) with high cycle characteristics may have a small degree of deterioration of the all-solid-state battery (10) due to charge / discharge, and an all-solid-state battery (10) with low cycle characteristics may have a large degree of deterioration of the all-solid-state battery (10) due to charge / discharge.

[0039] The positive electrode active material may have a particle shape such as a sphere or an ellipsoid, for example. The particle size and content of the positive electrode active material are not particularly limited.

[0040] The solid electrolyte may have a particle shape. The solid electrolyte may be dispersed between the positive electrode active materials. The solid electrolyte may include a sulfide-based solid electrolyte having excellent lithium ion conductivity characteristics. Examples of the sulfide-based solid electrolyte include Li2S-P2S5, Li2S-P2S5-LiX (X is a halogen element), Li2S-P2S5-Li2O, Li2S-P2S5-Li2O-LiI, Li2S-SiS2, Li2S-SiS2-LiI, Li2S-SiS2-LiBr, Li2S-SiS2-LiCl, Li2S-SiS2-B2S3-LiI, Li2S-SiS2-P2S5-LiI, Li2S-B2S3, Li2S-P2S5-Z m S n (m, n are positive numbers, capital letter “Z” represents Ge, Zn or Ga), Li2S-GeS2, Li2S-SiS2-Li3PO4, Li2S-SiS2-Li p MO q (p, q are positive numbers, capital letter “M” is one of P, Si, Ge, B, Al, Ga In), Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x It may include at least one selected from (0≤x≤2).

[0041] Sulfide-based solid electrolytes include, for example, Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I xIt may be an argyrodite-type compound including at least one selected from (0≤x≤2). In particular, the sulfide-based solid electrolyte may be an argyrodite-type compound including at least one selected from Li6PS5Cl, Li6PS5Br, and Li6PS5I.

[0042] Alternatively, the sulfide-based solid electrolyte is Li 7-a M a PS 6-c X c It may be an argyrodite-type compound containing (0≤a≤2, (0≤c≤2)), where X may be F, Br, Cl, or a combination thereof. M is candium (Sc), yttrium (Y), titanium (Ti), zirconium (Zr), hafnium (Hf), vanadium (V), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo), tungsten (W), manganese (Mn), technetium (Tc), rhenium (Re), iron (Fe), ruthenium (Ru), osmium (Os), cobalt (Co), rhodium (Rh), iridium (Ir), nickel (Ni), palladium (Pd), platinum (Pt), copper (Cu), silver (Ag), gold (Au), zinc (Zn), cadmium (Cd), mercury (Hg), aluminum (Al), gallium (Ga), indium (In), thallium (Tl), silicon (Si), germanium (Ge), tin (Sn), lead (Pb), arsenic (As), antimony (Sb), bismuth (Bi), or a combination thereof. Can be.

[0043] The density of the argyrodite-type solid electrolyte may be 1.5 g / cc to 2.0 g / cc. Since the argyrodite-type solid electrolyte has a density of 1.5 g / cc or more, the internal resistance of the all-solid-state battery is reduced, and the defect of the solid electrolyte membrane being penetrated and short-circuited due to the formation of lithium dendrites can be prevented. The elastic modulus of the solid electrolyte may be, for example, 15 GPa to 35 GPa.

[0044] The solid electrolyte in the positive electrode active material layer (120) may have a smaller median particle size average particle diameter (D50) than the first and second solid electrolytes (SE1, SE2) in the solid electrolyte layer (300) to be described later. For example, the median particle size average particle diameter (D50) of the solid electrolyte included in the positive electrode active material layer (120) may be 90% or less, 80% or less, 70% or less, 60% or less, 50% or less, 40% or less, 30% or less, or 20% or less of the median particle size average particle diameter (D50) of the solid electrolyte included in the solid electrolyte layer (300). Meanwhile, the median particle size average particle diameter (D50) may be a median diameter measured using a laser particle size distribution meter.

[0045] The positive electrode active material layer (120) may include a conductive material. The conductive material may have conductivity without causing a chemical change in the all-solid-state battery (10), thereby increasing the conductivity of the positive electrode active material and the solid electrolyte. The conductive material may include a carbon-based material. The conductive material may include, for example, one or more selected from graphite, carbon black, acetylene black, carbon nanofibers, and carbon nanotubes.

[0046] The positive electrode active material layer (120) may further include a binder. The binder may bind the positive electrode active material, the solid electrolyte, and the conductive material within the positive electrode active material layer (120) to each other. The binder may include a material for improving the bonding strength between the positive electrode active material layer (120) and the positive electrode current collector (110). The binder may include, for example, polyvinylidene fluoride, styrene butadiene rubber (SBR), polytetrafluoroethylene, polyvinylidene fluoride, vinylidene fluoride / hexafluoropropylene copolymer, polyacrylonitrile, and polymethyl methacrylate.

[0047] Based on 100 parts by weight of the total of the positive electrode active material, the solid electrolyte, the conductive agent, and the binder, the positive electrode active material layer (120) may include 85 parts by weight or more and 92 parts by weight or less of the positive electrode active material. Based on 100 parts by weight of the total of the positive electrode active material (PAM), the solid electrolyte, the conductive agent, and the binder, the positive electrode active material layer (120) may include 0.5 parts by weight or more and 1.5 parts by weight or less of the binder.

[0048] Based on 100 parts by weight of the solid electrolyte, the positive electrode active material layer (120) may include 1 part by weight or more and 50 parts by weight or less of a conductive material. If the conductive material is included in the positive electrode active material layer (120) in an amount of less than 1 part by weight based on 100 parts by weight of the solid electrolyte, the proportion of the conductive material may decrease, thereby lowering the electrical conductivity of the positive electrode active material layer (120). If the conductive material is included in the positive electrode active material layer (120) in an amount of more than 50 parts by weight based on 100 parts by weight of the solid electrolyte, the proportion of the conductive material may be excessively high, so that a covering layer covering the surface of the solid electrolyte may not be properly formed.

[0049] The positive electrode active material layer (120) may further include additives such as fillers, coating agents, dispersants, and ion conductive aids in addition to the above-described positive electrode active material, solid electrolyte, conductive agent, and binder.

[0050] The negative electrode layer (200) may include a negative electrode current collector (210) and a negative electrode coating layer (220) on the negative electrode current collector (210). The negative electrode current collector (210) may provide a reference surface on which the negative electrode coating layer (220) is disposed. The negative electrode current collector (210) may include, for example, a material that does not react with lithium, i.e., does not form an alloy or a compound with lithium. For example, the negative electrode current collector (210) may include at least one metal selected from the group consisting of copper (Cu), stainless steel, titanium (Ti), iron (Fe), cobalt (Co), and nickel (Ni). The thickness of the negative electrode current collector (210) may be 1 μm to 20 μm, more specifically 5 μm to 15 μm, and more specifically 7 μm to 10 μm.

[0051] The negative electrode current collector (210) may be composed of one of the above-described metals, or may include an alloy or coating material of two or more metals. The negative electrode current collector (210) may have, for example, a plate shape or a foil shape. Meanwhile, in one embodiment, the negative electrode current collector (210) may be omitted.

[0052] The negative electrode coating layer (220) can allow lithium metal to grow between it and the negative electrode current collector (210) when the all-solid-state battery (10) is charged. The negative electrode coating layer (220) can act as a protective layer for the lithium metal and simultaneously suppress the precipitation and growth of lithium dendrites.

[0053] The cathode coating layer (220) may include a metal and carbon. For example, the cathode coating layer (220) may include at least one metal selected from the group consisting of gold (Au), platinum (Pt), palladium (Pd), silicon (Si), silver (Ag), aluminum (Al), bismuth (Bi), tin (Sn), and zinc (Zn). The cathode coating layer (220) may include at least one carbon selected from the group consisting of carbon black, acetylene black, furnace black, ketjen black, and graphene. In one embodiment, the cathode coating layer (220) may include a mixture of carbon black and silver (Ag).

[0054] The cathode coating layer (220) may further include additives other than metal and carbon. The cathode coating layer (220) may further include, for example, at least one additive selected from the group consisting of a binder, a filler, a coating agent, a dispersant, and an ion conductive additive.

[0055] The negative electrode coating layer (220) may have a smaller thickness than the positive electrode active material layer (120). The thickness of the negative electrode coating layer (220) may be, for example, 50% or less, 40% or less, 30% or less, 20% or less, 10% or less, or 5% or less of the thickness of the positive electrode active material layer (120). The thickness of the negative electrode coating layer (220) may be, for example, 1 um to 20 um, 2 um to 10 um, or 3 um to 7 um. If the thickness of the negative electrode coating layer (220) is too thin, lithium dendrites formed between the negative electrode coating layer (220) and the negative electrode current collector (210) may cause the negative electrode coating layer (220) to collapse, thereby deteriorating the cycle characteristics of the all-solid-state battery (10). If the thickness of the cathode coating layer (220) increases excessively, the energy density of the all-solid-state battery (10) may decrease and the internal resistance of the all-solid-state battery (10) due to the cathode coating layer (220) may increase, thereby deteriorating the cycle characteristics of the cell.

[0056] Meanwhile, although not shown, a carbon layer may be further included to improve adhesion between the cathode coating layer (220) and the solid electrolyte layer (300).

[0057] A solid electrolyte layer (300) may be provided between the positive electrode layer (100) and the negative electrode layer (200). The solid electrolyte layer (300) may include a sulfide-based solid electrolyte having excellent lithium ion conductivity characteristics. The solid electrolyte in the solid electrolyte layer (300) may be the same as or different from any one of the materials included in the solid electrolyte in the positive electrode active material layer (120) described above.

[0058] The solid electrolyte layer (300) may include a first solid electrolyte layer (310) and a second solid electrolyte layer (320). The first solid electrolyte layer (310) may be adjacent to the positive electrode layer (100), and the second solid electrolyte layer (320) may be adjacent to the negative electrode layer (200).

[0059] Referring to FIG. 2, the first solid electrolyte layer (310) may include a first solid electrolyte (SE1), and the second solid electrolyte layer (320) may include a second solid electrolyte (SE2). Each of the first and second solid electrolytes (SE1, SE2) may have a particle shape such as a sphere or an ellipsoid.

[0060] Each of the first and second solid electrolytes (SE1, SE2) may include a sulfide-based solid electrolyte. The first and second solid electrolytes (SE1, SE2) may be the same or different. Each of the first and second solid electrolytes (SE1, SE2) may be amorphous, crystalline, or a mixture thereof. In addition, the solid electrolyte may include, for example, at least sulfur (S), phosphorus (P), and lithium (Li) as constituent elements among the above-described sulfide-based solid electrolyte materials. For example, the solid electrolyte may be a material including Li2S-P2S5. When using a sulfide-based solid electrolyte material including Li2S-P2S5 to form the solid electrolyte, the mixing molar ratio of Li2S and P2S5 is, for example, in the range of Li2S:P2S5=50:50 to 90:10.

[0061] Sulfide-based solid electrolytes include, for example, Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x It may be an argyrodite-type compound including at least one selected from (0≤x≤2). In particular, the sulfide-based solid electrolyte may be an argyrodite-type compound including at least one selected from Li6PS5Cl, Li6PS5Br, and Li6PS5I.

[0062] Alternatively, the sulfide-based solid electrolyte is Li 7-a M a PS 6-c X cIt may be an argyrodite-type compound containing (0≤a≤2, (0≤c≤2)), where X may be F, Br, Cl, or a combination thereof. M is candium (Sc), yttrium (Y), titanium (Ti), zirconium (Zr), hafnium (Hf), vanadium (V), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo), tungsten (W), manganese (Mn), technetium (Tc), rhenium (Re), iron (Fe), ruthenium (Ru), osmium (Os), cobalt (Co), rhodium (Rh), iridium (Ir), nickel (Ni), palladium (Pd), platinum (Pt), copper (Cu), silver (Ag), gold (Au), zinc (Zn), cadmium (Cd), mercury (Hg), aluminum (Al), gallium (Ga), indium (In), thallium (Tl), silicon (Si), germanium (Ge), tin (Sn), lead (Pb), arsenic (As), antimony (Sb), bismuth (Bi), or a combination thereof. Can be.

[0063] The density of the argyrodite-type solid electrolyte may be 1.5 g / cc to 2.0 g / cc. Since the argyrodite-type solid electrolyte has a density of 1.5 g / cc or more, the internal resistance of the all-solid-state battery is reduced, and the defect of the solid electrolyte membrane being penetrated and short-circuited due to the formation of lithium dendrites can be prevented. The elastic modulus of the first solid electrolyte (SE1) is, for example, 15 GPa to 35 GPa.

[0064] The first and second solid electrolyte layers (310, 320) may further include a binder. The binder included in the solid electrolyte layer (300) may be, for example, styrene butadiene rubber (SBR), polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, etc., but is not limited thereto. The binder of the first and second solid electrolyte layers (310, 320) may be the same as or different from the binder included in the positive electrode active material layer (120) or the binder included in the negative electrode coating layer (220).

[0065] Referring back to FIG. 2, the first solid electrolyte layer (310) and the second solid electrolyte layer (320) may have the same or different thicknesses. The first solid electrolyte layer (310) may have a first thickness (TK1), and the second solid electrolyte layer (320) may have a second thickness (TK2). For example, the first thickness (TK1) may be greater than the second thickness (TK2). For example, the first thickness (TK1) may be 2 to 100 times greater than the second thickness (TK2). For example, the second thickness (TK2) may be greater than the first thickness (TK1). For example, the second thickness (TK2) may be 2 to 100 times greater than the first thickness (TK2).

[0066] Referring back to FIGS. 1 and 2, the area of ​​the anode layer (100) and the area of ​​the cathode layer (200) may be different from each other. Specifically, the area of ​​the cathode layer (200) may be larger than the area of ​​the anode layer (100). The anode layer (100) may be completely overlapped within the cathode layer (200).

[0067] In one embodiment of the present invention, the first solid electrolyte layer (310) may have substantially the same area as the positive electrode layer (100). The second solid electrolyte layer (320) may have substantially the same area as the negative electrode layer (200).

[0068] Specifically, the first solid electrolyte layer (310) may have a first width (WI1) in a first direction (D1). The second solid electrolyte layer (320) may have a second width (WI2) in the first direction (D1). The first width (WI1) may be smaller than the second width (WI2). The first solid electrolyte layer (310) may have a third width (WI3) in the second direction (D2). The second solid electrolyte layer (320) may have a fourth width (WI4) in the second direction (D2). The third width (WI3) may be smaller than the fourth width (WI4).

[0069] The all-solid-state battery (10) according to the present embodiment can be manufactured by forming a positive electrode laminate of a positive electrode layer (100) and a first solid electrolyte layer (310), forming a negative electrode laminate of a negative electrode layer (200) and a second solid electrolyte layer (320), and then laminating the positive electrode laminate and the negative electrode laminate.

[0070]

[0071] The all-solid-state battery (10) according to the present invention may be a mono-cell all-solid-state battery, a bi-cell all-solid-state battery, or a stack-cell all-solid-state battery.

[0072] A mono-cell all-solid-state battery may include a cathode layer, a cathode layer, and a solid electrolyte layer disposed between the cathode layer and the anode layer. The solid electrolyte layer may include the first solid electrolyte layer and the second solid electrolyte layer described above.

[0073] A bi-cell all-solid-state battery may have a structure in which a negative electrode current collector, a negative electrode coating layer, a solid electrolyte layer, a positive electrode active material layer, a positive electrode current collector, a positive electrode active material layer, a solid electrolyte layer, a negative electrode coating layer, and a negative electrode current collector are laminated in that order. The solid electrolyte layer may include the first solid electrolyte layer and the second solid electrolyte layer described above. For example, the bi-cell all-solid-state battery may include two monocells (a first monocell and a second monocell). Each of the first and second monocells may include a positive electrode layer, an negative electrode layer, and a solid electrolyte layer disposed between the positive electrode layer and the negative electrode layer. The solid electrolyte layer of each of the first and second monocells may include the first solid electrolyte layer and the second solid electrolyte layer described above. The positive electrode layer of the first monocell and the positive electrode layer of the second monocell may face each other.

[0074] A stack-cell solid-state battery may include a plurality of bicells. The stack-cell solid-state battery may further include elastic pads. The stack-cell solid-state battery may have a structure in which bicells and elastic pads are alternately stacked. For example, the stack-cell solid-state battery may have a structure in which elastic pads, bicells, elastic pads, bicells, and elastic pads are stacked in that order.

[0075]

[0076] FIG. 3 is a cross-sectional view of an all-solid-state battery including a gasket structure according to one embodiment of the present invention. For convenience of explanation, the description of the same details as those described with reference to FIGS. 1 and 2 will be omitted below, and the differences will be described in detail.

[0077] The all-solid-state battery (10) may include a gasket structure (400). The gasket structure (400) may fill in the step difference in the side surface of the all-solid-state battery (10) caused by the difference in the area of ​​the negative electrode laminate and the positive electrode laminate. The gasket structure (400) may surround the side surfaces of the positive electrode laminate of the all-solid-state battery (10) along the first and second directions (D1, D2). For example, the thickness of the gasket structure (400) may be substantially the same as the thickness of the positive electrode laminate. Accordingly, even when the negative electrode laminate and the positive electrode laminate having different areas are laminated and pressed, damage to the step difference in the side surface of the all-solid-state battery can be prevented. The all-solid-state battery (10) including the gasket structure (400) may be manufactured according to the method for manufacturing an all-solid-state battery according to FIGS. 11 to 16, which will be described later.

[0078] Below, the gasket structure (400) is described in detail.

[0079]

[0080] gasket structure

[0081] Fig. 4 is a perspective view of a gasket structure according to embodiments of the present invention. Figs. 5 and 6 are a cross-sectional view and a bottom view, respectively, of a gasket structure according to one embodiment of the present invention. Figs. 7 to 10 are cross-sectional views of a gasket structure according to other embodiments of the present invention. Figs. 5, 7 to 10 are cross-sectional views taken along line B-B' of Fig. 4.

[0082] Referring to FIG. 4, the gasket structure (400) may include a removable film (430), an adhesive layer (410), and a gasket (420).

[0083] The removable film (430) can protect the adhesive layer (410). The removable film (430) can transport the gasket (420).

[0084] The removable film (430) can be placed on a plane defined by a first direction (D1) and a second direction (D2). The second direction (D2) can be perpendicular to the first direction (D1).

[0085] The removable film (430) may be peeled off later. For example, the removable film (430) may be separated from the adhesive layer (410) and the gasket (420). Accordingly, the removable film (430) may include a material that is separable from the adhesive layer (410) and the gasket (420). For example, the removable film (430) may include at least one selected from the group consisting of polyethylene terephthalate, polypropylene, polymethylpentene, and copolymers thereof. As an example, the removable film (430) may include polyethylene terephthalate and a silicone release coating.

[0086] The removable film (430) may have a smooth surface. For example, the surface of the removable film (430) may be smoother than the surface of the adhesive layer (410).

[0087] The adhesive layer (410) may be positioned on the removable film (430). That is, the adhesive layer (410) may be laminated along a third direction (D3). The third direction (D3) may be perpendicular to the first direction (D1) and the second direction (D2).

[0088] The adhesive layer (410) may be positioned on the lower surface of the gasket (420) described below. The adhesive layer (410) may be completely bonded to the gasket (420). For example, if the adhesive layer (410) is to be separated from the gasket (420), it may cause irreversible physical destruction.

[0089] The adhesive layer (410) may have adhesive strength at 15°C to 200°C. 'Adhesion' may be defined as a property of the adhesive layer (410) with respect to each of the removable film (430), the negative electrode laminate, and the positive electrode laminate.

[0090] For example, the adhesive layer (410) may have adhesive strength at room temperature. For example, the adhesive layer (410) may have adhesive strength at 15°C to 35°C. The adhesive layer (410) may adhere the gasket (420) and the removable film (430) by applying pressure at room temperature. In this case, the 'adhesion' may include 'pressure-sensitive adhesion'. The adhesive layer (410) having pressure-sensitive adhesion may have viscoelasticity.

[0091] When a removable film (430) comes into contact with an adhesive layer (410) having viscoelasticity, a certain amount of force may be required to separate the removable film (430) from the adhesive layer (410). The adhesive layer (410) having viscoelasticity can reversibly attach and detach the removable film (430). By applying a certain amount of force to the adhesive layer (410) having viscoelasticity, the adhesive layer (410) can be adhered to the negative electrode laminate and the positive electrode laminate. For example, the adhesive layer (410) may include at least one of acrylate and silicone.

[0092] As another example, the adhesive layer (410) may have adhesive strength upon heating. For example, the adhesive layer (410) may have adhesive strength at temperatures ranging from 40°C to 200°C, or from 80°C to 180°C. That is, the adhesive layer (410) does not have adhesive strength at room temperature, but may only have adhesive strength upon heating. By applying heat to the adhesive layer (410), the removable film (430) can be reversibly attached and detached. By contacting the adhesive layer (410) with the negative electrode laminate and the positive electrode laminate, and applying heat and pressure, the adhesive layer (410) can be adhered to the negative electrode laminate and the positive electrode laminate. Thereafter, when the heat is cooled, the adhesive layer (410) can be completely bonded to the negative electrode laminate and the positive electrode laminate. As an example, the adhesive layer (410) may include paper that has absorbed a surfactant such as polyethylene glycol.

[0093] Referring to FIGS. 4 and 5, the adhesive layer (410) may include a first opening (OP1). For example, the first opening (OP1) may include a plurality of first openings. The plurality of first openings may be spaced apart from each other in a first direction (D1). The first opening (OP1) may have a first width (W1).

[0094] The adhesive layer (410) may have a first line (LN1). The first line (LN1) may be configured to separate the adhesive layer (410) into two parts along the first direction (D1). That is, the adhesive layer (410) may have a first line (LN1) configured to separate it in the first direction (D1). For example, the first line (LN1) may be at least one of a cut line or a precut line. For example, the first line (LN1) may be located between adjacent ones of the plurality of first openings.

[0095] The gasket (420) may have a thin thickness. The thickness of the gasket (420) may be adjusted so that the thickness of the gasket structure (400) is substantially the same as the thickness of the anode laminate. The thickness of the gasket (420) may be adjusted so that, when the gasket structure (400) and the anode laminate are pressurized with a third pressure as described below, substantially the same pressure is applied to the gasket structure (400) and the anode laminate. However, when the pressure applied to the anode laminate is different, the thickness of the gasket (420) may be adjusted. For example, the thickness of the gasket (420) may be 5 μm to 20 μm. As an example, the gasket (420) may be a non-woven sheet.

[0096] The gasket (420) may be positioned on the adhesive layer (410). That is, the gasket (420) may be laminated along the third direction (D3).

[0097] The gasket (420) may include a second opening (OP2). For example, the second opening (OP2) may include a plurality of second openings. The plurality of second openings may be spaced apart from each other in the first direction (D1). The second opening (OP2) may have a second width (W2).

[0098] From a planar perspective, the first opening (OP1) and the second opening (OP2) may overlap each other. For example, the first width (W1) and the second width (W2) may be substantially equal to each other.

[0099] The gasket (420) may have a second line (LN2). The second line (LN2) may be configured to separate the gasket (420) into two parts along the first direction (D1). That is, the gasket (420) may have a second line (LN2) configured to separate it in the first direction (D1). For example, the second line (LN2) may be at least one of a cut line or a pre-cut line. For example, the second line (LN2) may be located between adjacent ones of the plurality of second openings.

[0100] The gasket structure (400) according to embodiments of the present invention can easily transport a gasket (420) having a thin thickness. The thickness of the gasket structure (400) may be substantially the same as the thickness of the positive electrode laminate. By using the gasket structure (400), when manufacturing an all-solid-state battery by stacking positive electrode laminates and negative electrode laminates having different areas, damage to the all-solid-state battery can be prevented. In particular, when providing and pressurizing a positive electrode laminate having a narrower area on a negative electrode laminate having a wider area, the step on the side of the all-solid-state battery can be prevented from being easily damaged. In addition, the gasket structure (400) can simultaneously transport a plurality of gaskets (420).

[0101]

[0102] Hereinafter, embodiments of the present invention will be described in detail.

[0103] In one embodiment of the present invention, referring to FIGS. 4 to 6, the removable film (430a) may include a third opening (OP3). In a plan view, the third opening (OP3) may overlap the first and second openings (OP1, OP2). The third opening (OP3) may include a plurality of third openings. The plurality of third openings may be spaced apart from each other in the first direction (D1). The third opening (OP3) may have a third width (W3). For example, the third width (W3) may be greater than the first width (W1). For example, the third width (W3) may be greater than the second width (W2). That is, at least a portion of the lower surface of the adhesive layer (410a) may be exposed.

[0104] The adhesive layer (410a) may have adhesive strength at a temperature of 15°C to 200°C. For example, the adhesive layer (410a) may have adhesive strength at a temperature of 40°C to 200°C, or at a temperature of 80°C to 180°C. Since the adhesive layer (410a) does not have adhesive strength at room temperature, contamination and damage of the exposed portion of the adhesive layer (410a) may be prevented during transport of the gasket structure (400). As another example, the adhesive layer (410a) may have adhesive strength at a temperature of 15°C to 35°C. In this case, a separate member or equipment may be included to prevent contamination or damage of the exposed portion of the adhesive layer (410a).

[0105] In other embodiments of the present invention, referring to FIGS. 7 to 10, the gasket structure (400) may further include a carrier film (440a, 440b). The carrier film (440a, 440b) may be positioned on the gasket (420). The carrier film (440a, 440b) may transport the gasket (420). The carrier film (440a, 440b) may protect the gasket (420). The carrier film (440a, 440b) may include polyethylene terephthalate or the like.

[0106] For example, the carrier film (440a, 440b) may have adhesive properties. The adhesive properties may include tackiness. For example, the carrier film (440a, 440b) may have adhesive properties that allow the gasket (420) to be removed later.

[0107] As another example, the carrier films (440a, 440b) may have releasability. For example, the carrier films (440a, 440b) may not have adhesive properties but may have releasability. For example, the carrier films (440a, 440b) may have releasability to a degree that allows the gasket (420) to be removed later.

[0108]

[0109] Referring back to FIG. 7, both the carrier film (440a) and the removable film (430b) may not include openings. That is, the carrier film (440a) may be positioned on top of both the gasket (420) and the second opening (OP2). The removable film (430b) may be positioned on the bottom of both the adhesive layer (410b) and the first opening (OP1). The carrier film (440a) and the removable film (430b) may be advantageous for protecting and transporting the gasket (420).

[0110] In another embodiment of the present invention, referring to FIG. 8, the carrier film (440a) may not include an opening. The carrier film (440a) may be advantageous for protecting and transporting the gasket (420). The removable film (430c) may include a third opening (OP3). In a plan view, the third opening (OP3) may overlap the first and second openings (OP1, OP2). The third opening (OP3) may include a plurality of third openings. Each of the first, second, and third openings (OP1, OP2, OP3) may have a first width (W1'), a second width (W2), and a third width (W3'). The first, second, and third widths (W1', W2, W3') may be substantially the same as each other.

[0111] In another embodiment of the present invention, referring to FIG. 9, the carrier film (440b) may include a fourth opening (OP4). The removable film (430c) may include a third opening (OP3). In a plan view, each of the third and fourth openings (OP3, OP4) may overlap with the first and second openings (OP1, OP2). The third opening (OP3) may include a plurality of third openings. The fourth opening (OP4) may include a plurality of fourth openings (OP4). Each of the first, second, third, and fourth openings (OP1, OP2, OP3, OP4) may have a first width (W1'), a second width (W2), a third width (W3'), and a fourth width (W'). The first, second, third and fourth widths (W1', W2, W3', W4') may be substantially equal to each other.

[0112] In another embodiment of the present invention, referring to FIG. 10, the carrier film (440b) may include a fourth opening (OP4). The removable film (430b) may not include any opening at all. The removable film (430b) may be advantageous for protecting and transporting the gasket (420).

[0113] In the embodiments according to FIGS. 7 to 10, when the removable film (430a, 430b) is peeled off, the lower surface of the adhesive layer (410a, 410b) can be exposed. This prevents contamination and damage to the adhesive layer (410a, 410b) during transport of the gasket structure (400). For example, the adhesive layer (410a) can have adhesive strength at temperatures ranging from 15°C to 35°C. This not only facilitates transport of the gasket structure (400), but also eliminates the need for a separate heating process to activate the adhesive strength.

[0114]

[0115] Method for manufacturing an all-solid-state battery

[0116] FIG. 11 is a flowchart of a method for manufacturing an all-solid-state battery according to embodiments of the present invention. FIGS. 12a to 15c are cross-sectional views illustrating steps S500 and S700 of a method for manufacturing an all-solid-state battery according to embodiments of the present invention, respectively. FIGS. 12a to 13d are cross-sectional views illustrating a method for manufacturing an all-solid-state battery using a gasket structure (see FIG. 5) according to one embodiment of the present invention. FIGS. 14a to 15c are cross-sectional views illustrating a method for manufacturing an all-solid-state battery using a gasket structure (see FIG. 7) according to another embodiment of the present invention.

[0117] Referring to FIG. 11, a method for manufacturing an all-solid-state battery may include forming a positive electrode laminate (S100), forming a negative electrode laminate (S300), bonding a gasket structure onto the negative electrode laminate (S500), providing the positive electrode laminate on the gasket structure, and combining the laminates (S700).

[0118] Each of the positive electrode laminate and the negative electrode laminate can be formed by the following methods (S100, S300). The all-solid-state battery (10) according to one embodiment of the present invention can form the positive electrode laminate by laminating the first solid electrolyte layer (310) on the positive electrode layer (100) and then applying a first pressure, and can form the negative electrode laminate by laminating the negative electrode layer (200) and the second solid electrolyte layer (320) and then applying a second pressure.

[0119] The present invention manufactures the positive electrode laminate and the negative electrode laminate by applying separate pressurization methods, thereby enabling the first pressure and the second pressure to be controlled differently. This allows for a relatively lower pressure to be applied to the positive electrode laminate and the negative electrode laminate, which have weak mechanical strength or are structurally unbalanced and thus are susceptible to damage when pressurized at high pressure.

[0120] The first pressure may be greater than the second pressure. For example, the first pressure may be defined as a pressure applied from the upper and lower surfaces of the positive electrode laminate toward the interior of the positive electrode laminate. The second pressure may be defined as a pressure applied from the upper and lower surfaces of the negative electrode laminate toward the interior of the negative electrode laminate.

[0121] The formation of the above-described positive and negative electrode laminates may include a pressing process using a roll press. However, this method is not necessarily limited to this method, and any pressing process applicable in the relevant technical field may be applied. For example, pressing processes such as a hydraulic plate press and a warm isostatic press may be applied.

[0122] When roll press is applied during the formation process of the above-mentioned positive electrode laminate, the linear pressure of the first pressure may be 1 ton / cm to 5 ton / cm. Specifically, the linear pressure of the first pressure may be 1 ton / cm to 4 ton / cm, 1 ton / cm to 3 ton / cm, or 1 ton / cm to 2.5 ton / cm.

[0123] When roll press is applied during the formation process of the above-mentioned negative electrode laminate, the linear pressure of the second pressure may be 1 ton / cm to 4 ton / cm. Specifically, the linear pressure of the first pressure may be 1 ton / cm to 3 ton / cm, 1 ton / cm to 2.5 ton / cm, or 1 ton / cm to 2 ton / cm.

[0124] The above pressurization process can be carried out at a relatively high temperature. Specifically, the pressurization process can be carried out at 60 to 150°C, 80 to 130°C, or 100 to 125°C.

[0125] Forming the above positive electrode laminate and negative electrode laminate may include a preheating process prior to the pressurizing process. Specifically, the positive electrode laminate and negative electrode laminate may be preheated to ±10°C and ±5°C, respectively, of the temperature at which the pressurizing process is performed. The preheating process may prevent damage to the positive electrode laminate and negative electrode laminate due to rapid temperature changes during the high-temperature pressurizing process.

[0126]

[0127] A gasket structure may be bonded onto a cathode laminate (S500). This step may specifically include providing cathode laminates onto a first film, and bonding a gasket structure onto the cathode laminate on the first film.

[0128] The cathode laminates may be provided on a first film (F1) (see FIGS. 12A and 14B ). The first film (F1) may carry the cathode laminates. For example, the first film (F1) may be a release film. For example, the first film (F1) may have adhesive and relasing properties. For example, the adhesive may include adhesion. Adhesion may be defined as being tightly and tightly attached without gaps.

[0129] The gasket structure (400) can be transported onto the cathode laminate on the first film (F1). For example, it can be transported by holding at least a portion of the upper surface of the gasket structure (400).

[0130] A gasket structure (400) may be adhered to a cathode laminate on a first film (F1) (see FIGS. 12b and 14b). For example, the cathode laminate may be adhered to an adhesive layer (410) of the gasket structure (400). For example, a removable film (430a) of the gasket structure (400) may be adhered to the first film (F1).

[0131]

[0132] An anode laminate may be provided on the gasket structure (400). That is, the anode laminate may be provided within the first and second openings (OP1, OP2) of the gasket structure (400). This step may specifically include providing anode laminates on a second film, and providing anode laminates on the second film on the cathode laminates and the gasket structure.

[0133] The positive electrode laminates may be provided on a second film (F2). The second film (F2) may carry the positive electrode laminates. For example, the second film (F2) may be a release film. For example, the second film (F2) may have adhesive and relasing properties. For example, the adhesive may include adhesion.

[0134] Meanwhile, the order in which the negative electrode laminate is provided on the first film (F1) and the positive electrode laminate is provided on the second film (F2) is not limited. For example, the negative electrode laminate may be provided on the first film (F1) and then the positive electrode laminate may be provided on the second film (F2). In another example, the positive electrode laminate may be provided on the second film (F2) and then the negative electrode laminate may be provided on the first film (F1).

[0135] Anode laminates may be provided on the cathode laminates and the gasket structure (see FIGS. 13A and 15A). For example, the first solid electrolyte layer (310) of the cathode laminate may be in contact with the second solid electrolyte layer (320) of the cathode laminate. Each of the side surfaces of the cathode laminate along the first and second directions (D1, D2) may be adjacent to the adhesive layer (410) and the gasket (420) of the gasket structure (400).

[0136]

[0137] The positive electrode laminate and the negative electrode laminate can be combined so that the first solid electrolyte layer and the second solid electrolyte layer are in contact with each other (S700). This step may specifically include bonding the positive electrode laminate, the negative electrode laminate, and the gasket structure, pressurizing the positive electrode laminate, the negative electrode laminate, and the gasket structure, and separating the gasket structure in the first direction along the first line and the second line.

[0138] The anode laminate, the cathode laminate, and the gasket structure can be bonded. That is, the anode laminate, the cathode laminate, and the gasket structure (400) can be bonded by the adhesive layer (410). This step can be performed under a temperature condition of 15°C to 200°C. The temperature can be controlled depending on the characteristics of the adhesive layer (410). As an example, this step can be performed under a temperature condition of 15°C to 35°C. As another example, this step can be performed under a temperature condition of 40°C to 200°C.

[0139] The positive electrode laminate, the negative electrode laminate, and the gasket structure can be pressurized with a third pressure. As a result, the first solid electrolyte layer and the second solid electrolyte layer can be adhered to each other. As a result, the positive electrode laminate, the negative electrode laminate, and the gasket structure can be combined with each other. This step may include a pressurizing process using a hydraulic plate press. However, it is not necessarily limited to this method, and any pressurizing process applicable in the art can be applied. For example, pressurizing processes such as roll press and warm isostatic press can be applied. For example, the third pressure can be defined as a pressure applied toward the inside from the upper and lower surfaces of the positive electrode laminate, the negative electrode laminate, and the gasket structure. By using the gasket structure, when stacking the positive electrode laminate and the negative electrode laminate having different areas, it is possible to prevent the steps on the sides of the all-solid-state battery from being easily damaged in this step.

[0140] The third pressure may be 2 MPa or more. Specifically, the third pressure may be 2.5 MPa or more, 3 MPa or more, or 3.5 MPa or more. The third pressure may be 100 MPa or less. Specifically, the third pressure may be 20 MPa or less, 10 MPa or less, 5 MPa or less, or 4 MPa or less.

[0141] For example, the first and second films (F1, F2) may be removed from the negative electrode laminate and the positive electrode laminate, respectively (see FIGS. 13b, 13c, and 15b). For example, the first and second films (F1, F2) may be removed sequentially. For example, the first film (F1) may be removed from the negative electrode laminate and then the second film (F2) may be removed from the positive electrode laminate. Alternatively, the second film (F2) may be removed from the positive electrode laminate and then the first film (F1) may be removed from the negative electrode laminate. When the first and second films (F1, F2) are removed, only the gasket (420) and the adhesive layer (410) of the gasket structure (400) may remain bonded to the negative electrode laminate and the positive electrode laminate.

[0142] A method for manufacturing an all-solid-state battery according to one embodiment of the present invention may include separating a gasket structure in a first direction (D1) (see FIGS. 13d and 15c ). That is, the remaining gasket structure (400) includes only an adhesive layer (410) and a gasket (420), and the adhesive layer (410) and the gasket (420) have a first line (LN1) and a second line (LN2), respectively, and the adhesive layer (410) and the gasket (420) can be separated in the first direction (D1) along the first line (LN1) and the second line (LN2). As a result, an assembly of independent positive electrode laminates, negative electrode laminates, and gasket structures can be provided.

[0143] For example, when the first line (LN1) and the second line (LN2) are cut lines, the adhesive layer (410) and the gasket (420) can be separated in the first direction (D1) by applying an external force to the gasket structure. For example, the gasket structure can be separated into two parts along the first line (LN1) and the second line (LN2) by using a relative external force difference.

[0144] As another example, if the first line (LN1) and the second line (LN2) are pre-cut lines, after removing the first and second films (F1, F2), the adhesive layer (410) and the gasket (420) can be separated in the first direction (D1).

[0145]

[0146] Hereinafter, steps S500 and S700 will be described in detail according to embodiments of the gasket structure described above. For convenience of explanation, descriptions of the same details as those described with reference to FIG. 11 will be omitted, and differences will be described in detail.

[0147] As one embodiment of the present invention, a case in which the gasket structure (400) has the cross-section shown in FIG. 5 will be described with reference to FIGS. 12a to 13d.

[0148] That is, the gasket structure (400) includes: a removable film; an adhesive layer positioned on the removable film and having a first line separated in a first direction; and a gasket positioned on the adhesive layer and having a second line separated in the first direction, wherein the adhesive layer includes a first opening and the gasket may include a second opening. In a planar view, the first opening and the second opening may overlap each other.

[0149] In addition, the removable film includes a third opening, wherein, in a planar view, the third opening can overlap the first and second openings. In addition, the first opening has a first width, the second opening has a second width, and the third opening has a third width, wherein the third width is greater than the first width, and the third width can be greater than the second width.

[0150] Referring to FIG. 12a, the cathode laminates can be provided on the first film (F1) (S510a).

[0151] Referring to FIG. 12b, the gasket structure (400) according to FIG. 5 can be transferred and provided on the negative electrode laminates on the first film (F1) (S530a). The negative electrode laminates can be provided within the third opening (OP3) of the gasket structure (400). As a result, a portion of the upper surface of the negative electrode laminate can be adjacent to the exposed portion of the lower surface of the adhesive layer (410a) of the gasket structure (400).

[0152] Referring to FIG. 13a, positive electrode laminates may be bonded to negative electrode laminates and a gasket structure (S710a). The positive electrode laminates may be provided on a second film (F2). The first solid electrolyte layer (310) of the positive electrode laminate may be in contact with the second solid electrolyte layer (320) of the negative electrode laminate. For example, each of the side surfaces of the positive electrode laminate along the first and second directions (D1, D2) may be adjacent to the adhesive layer (410a) of the gasket structure (400) and the gasket (420).

[0153] Among the gasket structures (400), the adhesive layer (410a) can be bonded to the anode laminate and the cathode laminate. This step can be performed at a temperature of 15°C to 200°C. For bonding, this step can include applying pressure with a constant force.

[0154] For example, the adhesive layer (410a) may be manufactured by absorbing a surfactant such as polyethylene glycol into paper, and this step may be performed under conditions of temperature and pressure of 40°C to 200°C. Under the above conditions, the adhesive layer (410a) is activated to have adhesive force, and by cooling the heat, the gasket structure (400) can be completely bonded to the positive electrode laminate and the negative electrode laminate.

[0155] As another example, the adhesive layer (410a) may include at least one of acrylate or silicone, and this step may be performed under conditions of temperature and pressure of 15°C to 35°C. Under these conditions, the gasket structure (400) may be bonded to the anode laminate and the cathode laminate. This allows for the elimination of a separate heating process. In this case, separate components or equipment may be included to prevent the exposed adhesive layer (410a) from being contaminated or damaged.

[0156] Referring to FIG. 13b, the first film (F1) can be removed (S730a). For example, the first film (F1) can be peeled off. At this time, the adhesive force between the negative electrode laminate and the adhesive layer (410a) may be stronger than the adhesive force between the first film (F1) and the negative electrode laminate. The adhesive force between the negative electrode laminate and the positive electrode laminate may be stronger than the adhesive force between the first film (F1) and the negative electrode laminate. Accordingly, even if the first film (F1) is removed, the negative electrode laminate may not be removed together.

[0157] Meanwhile, the adhesive force between the first film (F1) and the removable film (430a) may be stronger than the adhesive force between the removable film (430a) and the adhesive layer (410a). Since the removable film (430a) has a smooth surface, the removable film (430a) may have a substantially wide adhesive area and excellent adhesive force with respect to the first film (F1). That is, the adhesive force between the first film (F1) and the removable film (430a) may be stronger than the adhesive force between the removable film (430a) and the adhesive layer (410a). Accordingly, when the first film (F1) is peeled, the removable film (430a) may be peeled together with the first film (F1).

[0158] Referring to FIG. 13c, the second film (F2) can be removed (S750a). For example, the second film (F2) can be peeled off. At this time, the adhesive force between the positive electrode laminate and the negative electrode laminate may be stronger than the adhesive force between the second film (F2) and the positive electrode laminate. The adhesive force between the gasket (420) and the adhesive layer (410a) may be weaker than the adhesive force between the second film (F2) and the gasket (420). Accordingly, the gasket (420) and the adhesive layer (410a) may remain bonded to the negative electrode laminate and the positive electrode laminate.

[0159] Referring to FIG. 13d, the gasket structure can be separated in the first direction (D1) (S770a). This allows for the provision of combinations of independent positive electrode laminates, negative electrode laminates, and gasket structures.

[0160] In another embodiment of the present invention, a case in which a gasket structure (400) has a cross-section as shown in FIG. 7 will be described with reference to FIGS. 14a to 15c. The description of the steps described below can also be applied to cases in which a gasket structure (400) according to FIGS. 8 to 10 is used.

[0161] That is, the gasket structure (400) includes: a removable film; an adhesive layer positioned on the removable film and having a first line separated in a first direction; and a gasket positioned on the adhesive layer and having a second line separated in the first direction, wherein the adhesive layer includes a first opening, and the gasket includes a second opening, and in a plan view, the first opening and the second opening can overlap each other. In addition, the gasket structure (400) may further include a carrier film on the gasket.

[0162] Referring to Fig. 14a, the removable film (430b) of the gasket structure (400) can be removed (S510b). As a result, the lower surface of the adhesive layer (410b) of the gasket structure (400) can be exposed.

[0163]

[0164] Referring to FIG. 14b, the negative electrode laminates may be provided on the first film (F1). The gasket structure (400) according to S510b may be transported and adhered to the negative electrode laminates on the first film (F1) (S530b). A portion of the upper surface of the negative electrode laminate may be adjacent to a portion of the lower surface of the adhesive layer (410b) of the gasket structure (400).

[0165] The cathode laminate may be bonded to an adhesive layer (410b). For example, the adhesive layer (410b) may include at least one of acrylate and silicone, and this step may be performed at a temperature of 15°C to 35°C. For bonding, this step may include applying pressure with a constant force.

[0166] Referring to FIG. 14c, the carrier film (440a) of the gasket structure (400) can be removed (S550b). At this time, the adhesive force between the adhesive layer (410b) and the negative electrode laminate may be stronger than the adhesive force between the gasket (420) and the carrier film (440a). Accordingly, even if the carrier film (440a) is removed, the adhesive layer (410b) and the gasket (420) may remain adhered to the negative electrode laminate.

[0167] Referring to FIG. 15a, positive electrode laminates may be bonded to negative electrode laminates and a gasket structure (S710b). The positive electrode laminates may be provided on a second film (F2). The first solid electrolyte layer (310) of the positive electrode laminate may be in contact with the second solid electrolyte layer (320) of the negative electrode laminate. For example, each of the side surfaces of the positive electrode laminate along the first and second directions (D1, D2) may be adjacent to the adhesive layer (410b) of the gasket structure (400) and the gasket (420).

[0168] The adhesive layer (410b) of the gasket structure (400) can be bonded to the anode laminate and the cathode laminate. For example, this step can be performed under temperature conditions of 15°C to 35°C. For bonding, this step can include applying pressure with a constant force. Under the above conditions, the gasket structure (400) can be bonded to the anode laminate and the cathode laminate. As a result, a separate heating process can be omitted.

[0169] Referring to FIG. 15b, each of the first and second films (F1, F2) can be removed (S730b). For example, each of the first and second films (F1, F2) can be peeled off. For example, the first and second films (F1, F2) can be removed sequentially. For example, the first film (F1) can be removed from the negative electrode laminate, and then the second film (F2) can be removed from the positive electrode laminate. At this time, the adhesive force between the positive electrode laminate and the negative electrode laminate may be stronger than the adhesive force between the first film (F1) and the negative electrode laminate. The adhesive force between the positive electrode laminate and the negative electrode laminate may be stronger than the adhesive force between the second film (F2) and the positive electrode laminate. Accordingly, even if the first film (F1) and the second film (F2) are removed, the negative electrode laminate and the positive electrode laminate may not be removed together.

[0170] Referring to FIG. 15c, the gasket structure can be separated in the first direction (D1) (S750b). This allows for providing combinations of independent anode laminates, cathode laminates, and gasket structures, respectively.

[0171]

[0172] FIG. 16 is a cross-sectional view illustrating a method for manufacturing a bi-cell and stack-cell all-solid-state battery according to embodiments of the present invention.

[0173] Referring to FIG. 16, a bi-cell solid-state battery can be manufactured by stacking mono-cell solid-state batteries manufactured according to the above-described manufacturing method.

[0174] A stack-cell solid-state battery can be manufactured using a plurality of bi-cell solid-state batteries manufactured according to the above-described manufacturing method. For example, a plurality of bi-cell solid-state batteries can be stacked, and an elastic pad can be placed between the negative electrode current collectors of adjacent bi-cells.

[0175] By using the above-described gasket structure (400), when manufacturing a bi-cell or stack-cell all-solid-state battery in which positive and negative electrode laminates having different areas are laminated, it is possible to prevent the steps on the side of the all-solid-state battery from being easily damaged even when pressure is applied from the upper and lower surfaces.

[0176]

[0177] While embodiments of the present invention have been described with reference to the attached drawings, the present invention may be implemented in other specific forms without altering the technical spirit or essential features thereof. Therefore, it should be understood that the embodiments described above are exemplary in all respects and are not limiting.

Claims

1. Removable film; An adhesive layer positioned on the removable film and having a first line separated in a first direction; and A gasket positioned on the adhesive layer and having a second line separated in the first direction; The adhesive layer includes a first opening, The above gasket includes a second opening, The above removable film includes a third opening, From a planar perspective, the first opening, the second opening and the third opening overlap each other. Gasket structure.

2. In paragraph 1, The above adhesive layer has adhesive strength at 15°C to 200°C, Gasket structure.

3. In paragraph 1, The above adhesive layer comprises paper that has absorbed polyethylene glycol. Gasket structure.

4. In paragraph 1, The adhesive layer comprises at least one of acrylate and silicone. Gasket structure.

5. In paragraph 1, The first opening includes a plurality of first openings, and the plurality of first openings are spaced apart from each other in the first direction, The second opening includes a plurality of second openings, and the plurality of second openings are spaced apart from each other in the first direction, The third opening includes a plurality of third openings, and the plurality of third openings are spaced apart from each other in the first direction. Gasket structure.

6. In paragraph 1, The above first line is at least one of a cutting line or a pre-cut line, The second line is at least one of a cutting line or a pre-cut line, Gasket structure.

7. In paragraph 1, From a planar perspective, the first line and the second line overlap each other, Gasket structure.

8. In paragraph 1, The above first opening has a first width, The second opening has a second width, The third opening has a third width, The above third width is larger than the above first width, The third width is larger than the second width, Gasket structure.

9. Removable film; An adhesive layer positioned on the removable film and having a first line separated in a first direction; A gasket positioned on the adhesive layer and having a second line separated in the first direction; and A carrier film positioned on the gasket; including: The adhesive layer includes a first opening, The above gasket includes a second opening, From a planar perspective, the first opening and the second opening overlap each other, The above adhesive layer has adhesive strength at 15°C to 35°C, Gasket structure.

10. In paragraph 9, The adhesive layer comprises at least one of acrylate and silicone. Gasket structure.

11. In paragraph 9, The first opening includes a plurality of first openings, and the plurality of first openings are spaced apart from each other in the first direction, The second opening includes a plurality of second openings, and the plurality of second openings are spaced apart from each other in the first direction. Gasket structure.

12. In paragraph 9, The above first line is at least one of a cutting line or a pre-cut line, The second line is at least one of a cutting line or a pre-cut line, Gasket structure.

13. In paragraph 9, From a planar perspective, the first line and the second line overlap each other, Gasket structure.

14. In paragraph 9, The above removable film includes a third opening, In plan view, the third opening overlaps the first and second openings, The above first opening has a first width, The second opening has a second width, The third opening has a third width, The first width, the second width, and the third width are substantially the same as each other, Gasket structure.

15. In paragraph 9, The carrier film includes a fourth opening, In plan view, the fourth opening overlaps the first and second openings. Gasket structure.

16. Laminating a first solid electrolyte layer on a positive electrode layer and then applying a first pressure to form a positive electrode laminate; Laminating a second solid electrolyte layer on a cathode layer and then applying a second pressure to form a cathode laminate; Bonding a gasket structure on the above cathode laminate; Providing the anode laminate on the gasket structure; and Combining the positive electrode laminate and the negative electrode laminate so that the first solid electrolyte layer and the second solid electrolyte layer are in contact with each other; including, The above gasket structure: removable film; An adhesive layer positioned on the removable film and having a first line separated in a first direction; and A gasket positioned on the adhesive layer and having a second line separated in the first direction; The adhesive layer includes a first opening, The above gasket includes a second opening, From a planar perspective, the first opening and the second opening overlap each other. Method for manufacturing an all-solid-state battery.

17. In paragraph 16, The above gasket structure: The above removable film includes a third opening, In plan view, the third opening overlaps the first and second openings, The above first opening has a first width, The second opening has a second width, The third opening has a third width, The above third width is larger than the above first width, The third width is greater than the second width, Providing the gasket structure on the cathode laminate comprises providing the cathode laminate within the third opening. Method for manufacturing an all-solid-state battery.

18. In paragraph 16, The above gasket structure further includes a carrier film on the gasket, Providing the gasket structure on the above cathode laminate: Removing the above removable film; Adhering the adhesive layer on the cathode laminate; and Removing the carrier film; including; Method for manufacturing an all-solid-state battery.

19. In paragraph 16, Combining the above positive electrode laminate and the above negative electrode laminate: Bonding the positive electrode laminate, the negative electrode laminate, and the gasket structure; Pressurizing the anode laminate, the cathode laminate, and the gasket structure; and Separating the gasket structure in the first direction along the first line and the second line; Method for manufacturing an all-solid-state battery.

20. In paragraph 19, The bonding of the positive electrode laminate, the negative electrode laminate, and the gasket structure is performed under temperature conditions of 15°C to 200°C. Method for manufacturing an all-solid-state battery.

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