Apparatus and method for manufacturing all-solid-state battery

Abstract

The present invention relates to a method and an apparatus for manufacturing an all-solid-state battery. By using the method and apparatus for manufacturing an all-solid-state battery according to the present invention, a roll-type electrode laminate can be cut and continuously stacked on a pressing plate, thereby manufacturing an all-solid-state battery in the form of a stack cell.

Description

Manufacturing apparatus and method for all-solid-state batteries

[0001] The present invention relates to an apparatus and method for manufacturing an all-solid-state battery.

[0002]

[0003] Recently, driven by industrial demands, the development of batteries with high energy density and safety is actively underway. For example, lithium-ion batteries are being commercialized not only in the fields of information and communication devices but also in the automotive sector. In the automotive sector, safety is considered particularly important because it is directly related to human life.

[0004] Recently, all-solid-state batteries have been proposed in which the liquid electrolyte of lithium-ion batteries is replaced with a solid electrolyte. By not using flammable organic dispersion media, all-solid-state batteries can significantly reduce the likelihood of fire or explosion in the event of a short circuit. Therefore, such all-solid-state batteries can possess excellent safety.

[0005]

[0006] The problem that the present invention aims to solve is to provide an apparatus capable of manufacturing an all-solid-state battery by cutting and continuously stacking a roll-type electrode laminate on a pressure plate.

[0007] Another problem that the present invention aims to solve is to provide a method for manufacturing an all-solid-state battery by cutting and continuously stacking a roll-type electrode laminate on a pressure plate.

[0008]

[0009] A method for manufacturing an all-solid-state battery according to the concept of the present invention may include: driving a first laminated body extended in a first direction in the first direction; placing a first front portion, which is a front region of the first laminated body, on a first pressure plate; cutting the first front portion to form a first unit electrode, wherein the first laminated body is formed with a second front portion, which is a new front region, by the cutting; adjusting the position of the first pressure plate on which the first unit electrode is placed; driving the first laminated body in the first direction to place the second front portion on the first unit electrode; cutting the second front portion to form a second unit electrode; and laminating a second laminated body comprising the first and second unit electrodes that are sequentially stacked.

[0010] A method for manufacturing an all-solid-state battery according to another concept of the present invention may include: driving a first laminated body extended in a first direction in the first direction; the first laminated body comprising a first end, a middle portion, and a second end; cutting the first end, which is a front region of the first laminated body, to form a first end electrode on a first pressure plate of a pressure unit; cutting the middle portion, which is a new front region of the first laminated body, to form a unit electrode on the first end electrode; cutting the second end, which is a new front region of the first laminated body, to form a second end electrode on the unit electrode; and integrally laminating a second laminated body comprising the first end electrode, the unit electrode, and the second end electrode, which are sequentially stacked.

[0011] An all-solid-state battery manufacturing apparatus according to another concept of the present invention may include: a feeding unit configured to deliver a first laminate to a pressurizing unit; a cutting unit configured to cut the first laminate; and a pressurizing unit configured to stack and laminate unit electrodes formed by cutting the first laminate. The pressurizing unit may include: a first pressurizing plate and a second pressurizing plate facing each other; and a first control unit configured to adjust the position of the first pressurizing plate.

[0012]

[0013] The present invention provides a method and apparatus for manufacturing an all-solid-state stack cell including a bipolar electrode. By manufacturing a stack cell using the method and apparatus of the present invention, process efficiency can be improved. A stack cell manufactured according to the embodiments of the present invention has a structure in which a plurality of bipolar electrodes are connected in series, and has excellent energy density.

[0014]

[0015] FIG. 1 is a cross-sectional view of an all-solid-state battery according to one embodiment of the present invention.

[0016] FIG. 2 is a plan view of an all-solid-state battery according to one embodiment of the present invention.

[0017] FIG. 3 is a cross-sectional view illustrating an all-solid-state battery according to another embodiment of the present invention.

[0018] FIG. 4 is a cross-sectional view illustrating an all-solid-state battery according to another embodiment.

[0019] FIG. 5 is a configuration diagram for explaining an all-solid-state battery manufacturing apparatus according to one embodiment.

[0020] FIG. 6 is a configuration diagram for explaining a stack cell forming unit according to one embodiment.

[0021] FIG. 7 is a flowchart for explaining a method for manufacturing an all-solid-state battery according to one embodiment of the present invention.

[0022] FIGS. 8a to 15 are cross-sectional and exploded perspective views for explaining a method for manufacturing an all-solid-state battery according to one embodiment.

[0023] FIGS. 16a to 19 are cross-sectional and exploded perspective views illustrating a method for manufacturing an all-solid-state battery according to another embodiment.

[0024]

[0025] In order to fully understand the structure and effects of the present invention, preferred embodiments of the present invention are described with reference to the attached drawings. However, the present invention is not limited to the embodiments disclosed below, but can be implemented in various forms and various modifications can be made. The description of these embodiments is provided merely to ensure that the disclosure of the present invention is complete and to fully inform those skilled in the art of the scope of the invention.

[0026] In this specification, when a component is described as being on another component, it means that it may be formed directly on the other component or that a third component may be interposed between them. Additionally, in the drawings, the thicknesses of the components are exaggerated for the effective description of the technical content. Throughout the specification, parts indicated by the same reference numeral represent the same components.

[0027] The embodiments described herein will be described with reference to cross-sectional and / or plan views, which are exemplary illustrations of the invention. In the drawings, the thicknesses of films and regions are exaggerated for effective description of the technical content. Accordingly, the regions illustrated in the drawings are schematic in nature, and the shapes of the regions illustrated in the drawings are intended to illustrate specific forms of regions of the device and are not intended to limit the scope of the invention. Although terms such as first, second, third, etc., have been used to describe various components in the various embodiments of this specification, these components should not be limited by such terms. These terms are used merely to distinguish one component from another. The embodiments described and illustrated herein also include their complementary embodiments.

[0028] Unless otherwise specified in this specification, singular forms may also include plural forms. Additionally, unless otherwise specified, "A or B" may mean "comprising A, comprising B, or comprising A and B." As used herein, "comprises" and / or "comprising" do not exclude the presence or addition of one or more other components to the mentioned components.

[0029] In this specification, "combination of these" may mean a mixture of components, a laminate, a composite, a copolymer, an alloy, a blend, and a reaction product, etc.

[0030] FIG. 1 is a cross-sectional view of an all-solid-state battery according to one embodiment of the present invention. FIG. 2 is a plan view of an all-solid-state battery according to one embodiment of the present invention.

[0031] 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, not limited thereto, 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).

[0032] In one embodiment, the anode layer (100) may include an anode current collector (110) and an anode active material layer (120) disposed on the anode current collector (110). Although not illustrated, the anode active material layer (120) may include an anode active material, a solid electrolyte, a conductive material, and a binder.

[0033] The positive current collector (110) can provide a reference surface on which the positive active material layer (120) is placed. The positive current collector (110) may include, for example, a plate or foil comprising 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.

[0034] Meanwhile, unlike as illustrated in FIG. 1, the positive current collector (110) may be omitted in one embodiment of the present invention. Although not illustrated, a carbon layer with a thickness of 0.1 μm to 4 μm may be further disposed between the positive current collector (110) and the positive active material layer (120) to increase the bonding strength between the positive current collector (110) and the positive active material layer (120).

[0035] The positive electrode active material may include a material capable of reversibly absorbing and desorbing lithium ions. The positive electrode active material may include a plurality of particles. The positive electrode active material may include, for example, 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, but is not necessarily limited to these. Each positive electrode active material may be a single material or a mixture of two or more materials.

[0036] Lithium transition metal oxides are, 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 bB c D α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α≤2), Li a Nor 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 Nor 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 Nor 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 b O2(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-fIt is a compound represented by any one of Fe2(PO4)3 (0≤f≤2) or LiFePO4. In such compounds, the uppercase "A" is Ni, Co, Mn, or a combination thereof; the uppercase "B" is Al, Ni, Co, Mn, Cr, Fe, Mg, Sr, V, a rare earth element, or a combination thereof; the uppercase "D" is O, F, S, P, or a combination thereof; the uppercase "E" is Co, Mn, or a combination thereof; the uppercase "F" is F, S, P, or a combination thereof; the uppercase "G" is Al, Cr, Mn, Fe, Mg, La, Ce, Sr, V, or a combination thereof; the uppercase "Q" is Ti, Mo, Mn, or a combination thereof; the uppercase "I" is Cr, V, Fe, Sc, Y, or a combination thereof; and the uppercase "J" is V, Cr, Mn, Co, Ni, Cu, or a combination thereof.

[0037] The positive electrode 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 and metal atomic layers are alternately and regularly arranged in a specific direction, thereby forming a two-dimensional plane for each atomic layer. The "cubic rock salt type structure" represents a sodium chloride (NaCl) type structure, which is a type of crystal structure; specifically, it exhibits a structure in which face-centered cubic lattices (fcc) formed by cations and anions, respectively, are offset from each other by half the ridge of the unit lattice. Lithium transition metal oxides having such a layered rock salt type structure are, for example, LiNi x Co y Al z O2(NCA) or LiNi x Co y Mn zO2(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.

[0038] The aforementioned compound contained 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 aforementioned compound and the compound to which the coating layer is added. Meanwhile, the coating layer added to the surface of the positive electrode active material may include, for example, oxides, hydroxides, oxyhydroxides, oxycarbonates, or hydroxycarbonates of the following coating elements. The compounds forming this coating layer are 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. The method for forming the coating layer is, for example, spray coating or immersion.

[0039] When the positive electrode active material contains 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) is increased, and the metal leaching of the positive electrode active material in the charged state can be reduced. As a result, the cycle characteristics of the all-solid-state battery (10) in the charged state are improved. Meanwhile, "cycle characteristics" is a characteristic that indicates the degree of deterioration of the all-solid-state battery (10) due to charging and discharging of the all-solid-state battery (10). An all-solid-state battery (10) with high cycle characteristics has a small degree of deterioration due to charging and discharging, while an all-solid-state battery (10) with low cycle characteristics may have a large degree of deterioration due to charging and discharging.

[0040] The positive active material may have a particle shape such as a sphere or an ellipsoid. The particle size and content of the positive active material are not particularly limited. In one embodiment, the positive active material is in the form of a polycrystalline structure and may include secondary particles formed by the aggregation of at least two primary particles. In other words, a single first particle may include a plurality of primary particles (NNP) aggregated together. The first particle may have a spherical or elliptical shape.

[0041] A solid electrolyte may be dispersed between the cathode active materials. The solid electrolyte dispersed between the cathode active materials may have a particulate form. The solid electrolyte dispersed between the cathode active materials may include a sulfide-based solid electrolyte with excellent lithium ion conductivity characteristics. Sulfide-based solid electrolytes are, for example, Li2S-P2S5, Li2S-P2S5-LiX (where 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, and Li2S-P2S5-Z m S n (m, n are positive numbers, uppercase “Z” is one of Ge, Zn, or Ga), Li2S-GeS2, Li2S-SiS2-Li3PO4, Li2S-SiS2-Li p MO q (p, q are positive numbers, uppercase “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 xIt may include at least one selected from (0≤x≤2).

[0042] Sulfide-based solid electrolytes are, 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 comprising one or more selected from (0≤x≤2). In particular, the sulfide-based solid electrolyte may be an argyrodite-type compound comprising one or more selected from Li6PS5Cl, Li6PS5Br, and Li6PS5I. The density of the argyrodite-type solid electrolyte may be 1.5 g / cc to 2.0 g / cc. By having a density of 1.5 g / cc or higher for the argyrodite-type solid electrolyte, the internal resistance of the all-solid-state battery is reduced, and defects such as penetration and short circuit of the solid electrolyte film due to lithium dendrite formation can be prevented. The elastic modulus of the solid electrolyte may be, for example, 15 GPa to 35 GPa.

[0043] A sulfide-based solid electrolyte according to one embodiment is Li x M a PS y X zIt may include an argyrodite-type compound represented by (5.0≤x≤9.0, 0≤a≤1.0, 4.0≤y≤7.0, 0≤z≤3.0). Here, M is silicon (Si), germanium (Ge), tin (Sn), antimony (Sb), bismuth (Bi), aluminum (Al), tungsten (W), molybdenum (Mo), gallium (Ga), or a combination thereof, and X may be F, Cl, Br, I, or a combination thereof. However, the value of x may be determined such that the total charge of all cations (Li, M, P) and the total charge of all anions (S, X) in the compound are in equilibrium to satisfy electrical neutrality.

[0044] The solid electrolyte in the positive active material layer (120) may have a smaller average particle size (D50) of intermediate particle size compared to the solid electrolyte in the solid electrolyte layer (300) described later. For example, the average particle size (D50) of the solid electrolyte included in the positive 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 average particle size (D50) of the solid electrolyte included in the solid electrolyte layer (300). Meanwhile, the average particle size (D50) may be a median diameter measured using a laser particle size distribution meter.

[0045] The positive active material layer (120) may include a conductive material. The conductive material may have conductivity without causing chemical changes in the all-solid-state battery (10), thereby increasing the conductivity of the positive 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 active material layer (120) may further include a binder. The binder may bind the positive active material, solid electrolyte, and conductive material within the positive active material layer (120) together. The binder may include a material to improve the bonding strength between the positive active material layer (120) and the positive 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 positive active material, solid electrolyte, conductive material, and binder, the positive active material layer (120) may contain 70 parts by weight or more and 92 parts by weight or less of the positive active material. Based on 100 parts by weight of the total positive active material, solid electrolyte, conductive material, and binder, the positive active material layer (120) may contain 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 solid electrolyte within the positive active material layer (120), the positive active material layer (120) may contain 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 active material layer (120) in an amount less than 1 part by weight based on 100 parts by weight of solid electrolyte within the positive active material layer (120), the proportion of the conductive material decreases, and the electrical conductivity of the positive active material layer (120) may decrease. If the conductive material is included in the positive active material layer (120) in an amount exceeding 50 parts by weight based on 100 parts by weight of solid electrolyte within the positive active material layer (120), the proportion of the conductive material is excessively high, and a coating layer covering the surface of the solid electrolyte may not be properly formed.

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

[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 placed. The negative electrode current collector (210) may include, for example, a material that does not react with lithium, that is, does not form any alloys or compounds 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 current collector (210) may be composed of one of the metals described above, or may include an alloy of two or more metals or a coating material. The negative current collector (210) may, for example, have a plate-like or foil-like shape. Meanwhile, in one embodiment, the negative current collector (210) may be omitted.

[0052] The negative electrode coating layer (220) can allow lithium metal to grow between the all-solid-state battery (10) and the negative electrode current collector (210) during charging. The negative electrode coating layer (220) can serve 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 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 other additives in addition to metal and carbon. The cathode coating layer (220) may further include at least one additive selected from the group consisting of, for example, binders, fillers, coating agents, dispersants, and ion-conducting aids.

[0055] The negative electrode coating layer (220) may have a smaller thickness compared to 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 µm to 20 µm, 2 µm to 10 µm, or 3 µm to 7 µm. If the thickness of the negative electrode coating layer (220) is excessively 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 degrading the cycle characteristics of the all-solid-state battery (10). If the thickness of the negative electrode coating layer (220) increases excessively, the energy density of the all-solid-state battery (10) decreases, and the internal resistance of the all-solid-state battery (10) due to the negative electrode coating layer (220) increases, which may degrade the cycle characteristics of the all-solid-state battery (10).

[0056] Meanwhile, although not illustrated, 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 anode layer (100) and the cathode layer (200). The solid electrolyte layer (300) may include a sulfide-based solid electrolyte with 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 aforementioned anode active material layer (120).

[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 anode layer (100), and the second solid electrolyte layer (320) may be adjacent to the cathode layer (200).

[0059] The second solid electrolyte layer (320) can be in direct contact with the negative electrode coating layer (220). By doing so, the second solid electrolyte layer (320) can suppress lithium dendrites formed between the negative electrode coating layer (220) and the negative electrode current collector (210). The second solid electrolyte layer (320) can effectively suppress negative side reactions. By doing so, the cell performance of the all-solid-state battery (10) according to the present invention can be improved.

[0060] The solid electrolyte in the solid electrolyte layer (300) may have particle shapes such as spheres or ellipsoids.

[0061] The solid electrolyte in the solid electrolyte layer (300) may include a sulfide-based solid electrolyte. The solid electrolyte in the solid electrolyte layer (300) may be amorphous, crystalline, or a mixture thereof. Additionally, the solid electrolyte may include sulfur (S), phosphorus (P), and lithium (Li) as at least constituent elements among the sulfide-based solid electrolyte materials described above, for example. For example, the solid electrolyte may be a material containing Li2S-P2S5. When using a sulfide-based solid electrolyte material containing Li2S-P2S5 to form the solid electrolyte, the molar ratio of Li2S and P2S5 is, for example, in the range of Li2S : P2S5 = 50 : 50 to 90 : 10.

[0062] In one embodiment, the solid electrolyte in the solid electrolyte layer (300) is Li x M a PS y X zIt may be an argyrodite-type compound represented by (5.0≤x≤9.0, 0≤a≤1.0, 4.0≤y≤7.0, 0≤z≤3.0). Here, M is silicon (Si), germanium (Ge), tin (Sn), antimony (Sb), bismuth (Bi), aluminum (Al), tungsten (W), molybdenum (Mo), gallium (Ga), or a combination thereof, and X may be F, Cl, Br, I, or a combination thereof. However, the value of x may be determined such that the total charge of all cations (Li, M, P) and the total charge of all anions (S, X) in the compound are in equilibrium to satisfy electrical neutrality.

[0063] The density of the azyrodite-type solid electrolyte may be 1.5 g / cc to 2.0 g / cc. By having a density of 1.5 g / cc or higher for the azyrodite-type solid electrolyte, the internal resistance of the all-solid-state battery is reduced, and defects such as penetration and short circuit of the solid electrolyte film due to lithium dendrite formation can be prevented. The elastic modulus of the solid electrolyte in the solid electrolyte layer (300) is, for example, 15 GPa to 35 GPa.

[0064] The solid electrolyte layer (300) may further include a binder. The binder included in the solid electrolyte layer (300) is, for example, styrene butadiene rubber (SBR), polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, etc., but is not limited to these. The binder of the solid electrolyte layer (300) 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 again to FIG. 1, the first solid electrolyte layer (310) may have a first thickness (t1), and the second solid electrolyte layer (320) may have a second thickness (t2). The solid electrolyte layer (300) may have a third thickness (t3). The first thickness (t1) The second thickness (t2) may have different thicknesses. The second thickness (t2) may be larger than the first thickness (t1).

[0066] The thinner the thickness of the solid electrolyte layer (300), the higher the energy density, but on the other hand, it is difficult to suppress the formation of lithium dendrites in the negative electrode, so there is a possibility of a short circuit.

[0067] In solid electrolytes, voids can form at the interface between the electrode and the electrolyte, which act as interfacial resistance and can lead to battery performance degradation.

[0068] Interfacial resistance can be reduced by applying pressure to the electrode and the solid electrolyte layer together. In one embodiment, since the sulfide-based solid electrolyte has high ionic conductivity and is mechanically soft, an all-solid-state battery with improved interfacial resistance can be fabricated through pressure application.

[0069] In one embodiment of the present invention, the anode layer (120) and the cathode layer (220) may include a pressurization process in the manufacturing process. In one embodiment of the present invention, the pressurization process may be performed by applying different pressures to each of the anode layer (120) and the cathode layer (220). In one embodiment of the present invention, the anode layer (120) may be manufactured by applying a relatively higher pressure compared to the cathode layer (220). For example, applying nanoscale particles to the anode and cathode active materials can increase the contact area with the solid electrolyte and improve interfacial resistance. In one embodiment, the anode active material may be in a polycrystalline form for reasons such as improved adhesion to the electrode plate, capacity characteristics, and lifespan characteristics, and may include secondary particles formed by the aggregation of at least two primary particles. In this case, the interface resistance between the anode layer (120) and the first solid electrolyte layer (310) is observed to be greater than the interface resistance between the cathode layer (220) and the second solid electrolyte layer (320), so the anode laminate can be manufactured by applying a relatively higher pressure compared to the cathode laminate. However, this is not limited thereto, and the anode layer (120) and the cathode layer (220) can be manufactured through a pressurization process in which different pressures are applied to each for various reasons.

[0070] One embodiment of the present invention can solve process problems that may occur when the interfacial resistance between the anode layer (120) and the first solid electrolyte layer (310) is different from the interfacial resistance between the cathode layer (220) and the second solid electrolyte layer (320) by dividing the solid electrolyte (300) into a first solid electrolyte layer (310) and a second solid electrolyte layer (320). For example, an all-solid-state battery manufactured according to the all-solid-state battery manufacturing method described below can provide an all-solid-state battery manufactured by applying different pressures to the anode stack and the cathode stack, respectively.

[0071] One embodiment of the present invention divides the solid electrolyte layer (300) into a first solid electrolyte layer (310) and a second solid electrolyte layer (320) and adjusts the thickness of each differently, thereby increasing energy density while suppressing the formation of lithium dendrites in the negative electrode. This allows for the provision of an all-solid-state battery (10) with improved stability against short-circuit risk and shock and high energy density.

[0072] The ratio (t2 / t1) of the second thickness t2 to the first thickness t1 may be 1 to 20. Specifically, the ratio (t2 / t1) of the second thickness t2 to the first thickness t1 may be 2 to 15, 4 to 11, or 4.5 to 5.5. When the ratio (t2 / t1) of the second thickness t2 to the first thickness t1 is within the aforementioned numerical range, the formation of lithium dendrites in the negative electrode is suppressed while increasing energy density, thereby improving stability against short-circuit risk and shock, and providing an all-solid-state battery (10) with high energy density.

[0073] The first thickness (t1) may be 30 μm or less. Specifically, the first thickness (t1) may be 25 μm or less, 20 μm or less, 14 μm or less, or 10 μm or less. The first thickness (t1) may be 0.1 μm or more. Specifically, the first thickness (t1) may be 1 μm or more, 2 μm or more, 4 μm or more, or 5 μm or more. If the first thickness (t1) exceeds the numerical range mentioned above, the energy density of the all-solid-state battery (10) may decrease. If the first thickness (t1) does not fall within the numerical range mentioned above, the first thickness (t1) may not be sufficient to form an interface with respect to the diameter of the active material powder within the positive electrode.

[0074] The second thickness (t2) may be 30 μm or more. Specifically, it may be 35 μm or more, 40 μm or more, 45 μm or more, 50 μm or more, 55 μm or more, and 60 μm or more. The second thickness (t2) may be 120 μm or less. Specifically, the second thickness (t2) may be 90 μm or less and 60 μm or less. If the second thickness (t2) does not fall within the aforementioned numerical range, it may be difficult to suppress the formation of lithium dendrites within the negative electrode, and there may be a risk of a short circuit. If the second thickness (t2) exceeds the aforementioned numerical range, the energy density of the all-solid-state battery (10) may decrease.

[0075] The third thickness (t3) may be 120 μm or less. Specifically, the third thickness (t3) may be 90 μm or less and 60 μm or less. The third thickness (t3) may be 10 μm or more. Specifically, the third thickness (t3) may be 30 μm or more and 50 μm or more. If the third thickness (t3) exceeds the above numerical range, the energy density of the all-solid-state battery (10) may decrease.

[0076] Referring to FIG. 1, the first solid electrolyte layer (310) may have a first width (W1) in the first direction (D1). The second solid electrolyte layer (320) may have a second width (W2) in the first direction (D1). The first width (W1) may be smaller than the second width (W2).

[0077] The difference between the second width (W2) and the first width (W1) may be 10 mm or less. Specifically, the difference between the second width (W2) and the first width (W1) may be 8 mm or less, 5 mm or less, or 3 mm or less. The difference between the second width (W2) and the first width (W1) may be 0.1 mm or more, 0.5 mm or more, or 1 mm or more. If the value exceeds the above numerical range, the size of the anode layer (100) becomes relatively smaller, so the discharge capacity is lowered and the energy density of the all-solid-state battery (10) may decrease. If the value does not fall within the above numerical range, it is difficult to suppress the formation of lithium dendrites in the negative electrode, and there may be a risk of a short circuit.

[0078] The ratio (W2 / W1) of the second width (W2) to the first width (W1) may be 1 to 1.6. Specifically, the ratio (W2 / W1) of the second width (W2) to the first width (W1) may be 1 to 1.5, 1 to 1.4, 1 to 1.3, 1 to 1.2, or 1 to 1.1.

[0079] If the ratio (W2 / W1) of the second width (W2) to the first width (W1) exceeds the numerical range, the energy density of the all-solid-state battery (10) is reduced.

[0080] In another embodiment, although not illustrated, the first width (W1) may be substantially the same as the second width (W2).

[0081]

[0082] FIG. 2 is a cross-sectional view illustrating an all-solid-state battery according to another embodiment of the present invention. In this embodiment, detailed descriptions of technical features that overlap with those previously described with reference to FIG. 1 are omitted, and differences are described in detail.

[0083] Referring to FIG. 2, the negative electrode layer (200) of the all-solid-state battery (10) may further include a lithium metal layer (400) between the negative electrode current collector (210) and the negative electrode coating layer (220). The thickness of the lithium metal layer (400) may increase further during charging of the all-solid-state battery (10). The negative electrode coating layer (220) acts as a protective layer for the lithium metal layer (400) and, at the same time, can suppress the growth of lithium dendrites from the lithium metal layer (400).

[0084] The lithium metal layer (400) may be a thin metal film containing lithium or a lithium alloy. The lithium alloy is not limited to, for example, Li-Al alloy, Li-Sn alloy, Li-In alloy, Li-Ag alloy, Li-Au alloy, Li-Zn alloy, Li-Ge alloy, Li-Si alloy, etc., and any alloy used as a lithium alloy is possible. The lithium metal layer (400) may contain one of these alloys or lithium. Alternatively, the lithium metal layer (400) may contain various types of alloys.

[0085] The lithium metal layer (400) may have a fifth width (W5) in the first direction (D1).

[0086] In one embodiment, the fifth width (W5) may be equal to or greater than the first width (W1). The fifth width (W5) may be equal to or smaller than the second width (W2). For example, the fifth width (W5) may be greater than the first width (W1) and smaller than the second width (W2).

[0087] In another embodiment, although not illustrated, the first width (W1) and the second width (W2) may be substantially the same. The fifth width (W5) may be smaller than the first width (W5).

[0088]

[0089] FIG. 3 is a cross-sectional view illustrating an all-solid-state battery according to another embodiment of the present invention. Detailed descriptions of technical features that overlap with those previously described with reference to FIG. 1 and FIG. 2 are omitted, and the differences are described in detail.

[0090] Referring to FIG. 3, an all-solid-state battery (CEL) according to one embodiment may be in the form of a stack cell in which at least one unit electrode (UEL) is stacked.

[0091] Referring to FIG. 3, the all-solid-state battery (CEL) may include at least one unit electrode (UEL). The unit electrode (UEL) may be a bipolar electrode in which one side acts as a positive electrode and the opposite side acts as a negative electrode. Specifically, the all-solid-state battery (CEL) may include a first unit electrode (UEL1), a second unit electrode (UEL2) on the first unit electrode (UEL), and a third unit electrode (UEL3) on the second unit electrode (UEL2). The all-solid-state battery (CEL) may include additional unit electrodes (UEL) in addition to the first to third unit electrodes (UEL1, UEL2, UEL3).

[0092] Each of the first to third unit electrodes (UEL1, UEL2, UEL3) may comprise a bipolar substrate (BPS); a first electrode composite layer (EML1) on one side of the bipolar substrate (BPS); a first gasket (GSK1) surrounding the first electrode composite layer (EML1); a first electrolyte layer (SEL1) on the first electrode composite layer (EML1); a second electrode composite layer (EML2) on the other side of the bipolar substrate (BPS); a second gasket (GSK2) surrounding the second electrode composite layer (EML2); and a second electrolyte layer (SEL2) on the second electrode composite layer (EML2).

[0093] In one embodiment, the length of the bipolar substrate (BPS) in the first direction (D1) may be substantially the same as the length of the first electrolyte layer (SEL1) in the first direction (D1). Additionally, the length of the bipolar substrate (BPS) in the first direction (D1) may be substantially the same as the length of the second electrolyte layer (SEL2) in the first direction (D1). This may be because the lengths in the first direction (D1) become substantially the same as the bipolar substrate (BPS) and the first and second electrolyte layers (SEL1, SEL2) are cut integrally.

[0094] In one embodiment, each of the first and second gaskets (GSK1, GSK2) may comprise one or more selected from lithium-ion insulators and lithium-ion conductors. Each of the first and second gaskets (GSK1, GSK2) may be an electronic insulator. That is, each of the first and second gaskets (GSK1, GSK2) may not be an electronic conductor. Each of the first and second gaskets (GSK1, GSK2) may be an ion insulator. That is, each of the first and second gaskets (GSK1, GSK2) may not be an ion conductor. Each of the first and second gaskets (GSK1, GSK2) comprises, for example, an organic material, an inorganic material, or an organic-inorganic composite material. The organic material may be, for example, a polymer. The inorganic material may be, for example, a ceramic such as a metal oxide. The organic-inorganic composite material may be a composite of a polymer and a metal oxide.

[0095] In one embodiment, each of the first and second gaskets (GSK1, GSK2) may include at least one of polyimide, polyetherimide, and polypropylene as a polymer. By including said polymer, they can be stretched in a lamination process.

[0096] Referring to FIG. 3, in one embodiment, the first and second gaskets (GSK1, GSK2) may each protrude outward beyond the first and second electrolyte layers (SEL1, SEL2). The bipolar substrate and the first and second gaskets (GSK1, GSK2) are cut integrally, but the first and second gaskets (GSK1, GSK2) may be extended and protrude outward due to the lamination process described later.

[0097] In one embodiment, the bipolar substrate (BPS) is composed of a material that does not react with, for example, lithium. That is, the bipolar substrate (BPS) is composed of a material that does not form any alloys or compounds with lithium. The material constituting the bipolar substrate (BPS) may be, for example, stainless steel, aluminum (Al), copper (Cu), titanium (Ti), iron (Fe), cobalt (Co), nickel (Ni), alloys thereof, and clads thereof, but is not necessarily limited to these; any material used as an electrode current collector for a bipolar battery in the relevant technical field is acceptable.

[0098] In one embodiment, the first electrode composite layer (EML1) may be either the anode layer (100) or the cathode layer (200) described above with reference to FIG. 1, and the second electrode composite layer (EML2) may be the other one of the anode active material layer (120) and the cathode coating layer (220) described above. As an example, the first electrode composite layer (EML1) may be the anode active material layer (120), and the second electrode composite layer (EML2) may be the cathode coating layer (220).

[0099] In one embodiment, the first electrolyte layer (SEL1) may be either the first solid electrolyte layer (310) and the second solid electrolyte layer (320) described above with reference to FIG. 1, and the second electrolyte layer (SEL2) may be the other one of the first solid electrolyte layer (310) and the second solid electrolyte layer (320). For example, the first electrolyte layer (SEL1) may be the first solid electrolyte layer (310), and the second electrolyte layer (SEL2) may be the second solid electrolyte layer (320). That is, each of the first and second electrolyte layers (SEL1, SEL2) may be a solid electrolyte layer containing a solid electrolyte.

[0100] Referring again to FIG. 3, in one embodiment, the all-solid-state battery (CEL) may further include a first end electrode (EEL1) and a second end electrode (EEL2) at both ends. As an example, the all-solid-state battery (CEL) may include a first end electrode (EEL1) on the lower surface of a first unit electrode (UEL1) and a second end electrode (EEL2) on the upper surface of a third unit electrode (UEL3). Each of the first and second end electrodes (EEL1, EEL2) is a monopolar electrode comprising one electrode composite layer and may include a current collector (COL) and an electrode composite layer (EML) on the current collector (COL). The current collector (COL) may be either the positive current collector (110) and the negative current collector (210) described above with reference to FIG. 1. The electrode composite layer (EML) may be the first electrode composite layer (EML1) or the second electrode composite layer (EML2) described above with reference to FIG. 3.

[0101] For example, the first end electrode (EEL1) may include a positive current collector (110), and the second end electrode (EEL2) may include a negative current collector (120).

[0102]

[0103] Referring to FIG. 3, the all-solid-state battery (CEL) may have a structure in which first to third unit electrodes (UEL1, UEL2, UEL3) are connected in series. By connecting the unit electrodes in series within the all-solid-state battery (CEL), the structure can be simplified and energy transfer efficiency can be improved. In addition, a high output voltage can be achieved through the series connection.

[0104] FIG. 4 is a cross-sectional view illustrating an all-solid-state battery according to another embodiment.

[0105] Referring to FIG. 4, the all-solid-state battery (CEL) may include a first end electrode (EEL1), a second end electrode (EEL2), and at least one unit electrode (UEL) disposed between the first end electrode (EEL1) and the second end electrode (EEL2). As an example, the all-solid-state battery (CEL) may include a first end electrode (EEL1), a first unit electrode (UEL1) on the first end electrode, a second unit electrode (UEL2) on the first unit electrode (UEL1), and a second end electrode (EEL2) on the second unit electrode (UEL2).

[0106] Each of the first and second end electrodes (EEL1, EEL2) is a monopolar electrode comprising one electrode composite layer and may include a current collector (COL), an electrode composite layer (EML) on the current collector (COL), and an electrolyte layer (EML) on the electrode composite layer (EML). The current collector (COL) may be either the positive current collector (110) and the negative current collector (210) described above with reference to FIG. 1. The electrode composite layer (EML) may be the first electrode composite layer (EML1) or the second electrode composite layer (EML2) described above with reference to FIG. 3. The electrolyte layer (EML) may be the first electrolyte layer (EML1) or the second electrolyte layer (EML2) described above with reference to FIG. 3.

[0107] For example, the first end electrode (EEL1) may include a positive current collector (110), and the second end electrode (EEL2) may include a negative current collector (120).

[0108]

[0109] Hereinafter, an all-solid-state battery manufacturing apparatus according to embodiments of the present invention will be described with reference to FIGS. 5 and FIGS. 5 is a configuration diagram for describing an all-solid-state battery manufacturing apparatus according to one embodiment. FIGS. 6 is a configuration diagram for describing a stack cell forming unit (SMU) among the all-solid-state battery manufacturing apparatus.

[0110] Referring to FIG. 5, the all-solid-state battery manufacturing apparatus may include a stack supply unit (SSU); a stack cell forming unit (SMU); and a loading unit (TRU).

[0111] Referring to FIG. 5, the laminate supply unit (SSU) can be configured to supply the first laminate (STK1).

[0112] In one embodiment, the laminate supply unit (SSU) may include a first laminate (STK1) in a wound state. The laminate supply unit (SSU) may be configured to unwind.

[0113] The laminate supply unit (SSU) can be configured to drive the unwinded first laminate (STK1) in the first direction (D1).

[0114] FIG. 6 is a configuration diagram for explaining a stack cell forming unit (SMU) according to one embodiment. Referring to FIG. 6, the stack cell forming unit (SMU) may include a feeding unit (FDU), a cutting unit (CTU), and a pressurizing unit (PRU).

[0115] In one embodiment, the feeding unit (FDU) may be configured to transfer a first laminate (STK1) from a laminate supply unit (SSU) to a pressurizing unit (PRU). Specifically, the feeding unit (FDU) may be configured to transfer the first laminate (STK1) traveling in a first direction (D1) onto a first pressurizing plate (PPL1). As an example, the feeding unit (FDU) may include a feeding roller or a feeding belt. Although not illustrated, the feeding unit (FDU) may further include a feeding control unit. The feeding control unit may be configured to control the driving speed of the feeding roller, i.e., the rotational speed of the feeding roller. The driving speed of the feeding roller may be synchronized with the cutting speed of the cutting unit (CTU) described later.

[0116] In one embodiment, the cutting unit (CTU) may be configured to cut an object. Specifically, the cutting unit (CTU) may be configured to cut a first laminate (STK1) placed within a pressurizing unit (PRU) described later. As an example, the cutting unit (CTU) may include a cutter. The cutting unit (CTU) may further include a cutter control unit. The cutter control unit may be configured to control the movement of the cutter. As an example, the cutter control unit may control the movement of the cutter using a hydraulic method, a gear method, a screw method, a cam method, etc.

[0117] In one embodiment, the pressurizing unit (PRU) may be configured to pressurize an object. Specifically, the pressurizing unit (PRU) may be configured to pressurize the objects as a whole after stacking them on a first pressurizing plate (PPL1). As an example, the pressurizing unit (PRU) may be configured to pressurize a second laminate (STK2) formed by sequentially stacking a first laminate (STK1) after cutting it.

[0118] In one embodiment, the pressure unit (PRU) may include a first pressure plate (PPL1) and a second pressure plate (PPL2) facing each other. A first laminate (STK1) may be placed on the first pressure plate (PPL1). The pressure unit (PRU) may further include a first control unit (MCU1) configured to adjust the position of the first pressure plate (PPL1). The first control unit (MCU1) may move the first pressure plate (PPL1) up and down in a third direction (D3). The first control unit (MCU1) may move the first pressure plate (PPL1) up and down according to the thickness of an object located on the first pressure plate (PPL1).

[0119] In one embodiment, the pressurizing unit (CTU) may further include a positioning plate (POP). The positioning plate (POP) may be located between the first and second pressurizing plates (PPL1, PPL2). The positioning plate (POP) may be configured to align the front area of ​​the first laminate (STK1) onto the first pressurizing plate (PPL1). The positioning plate (POP) may provide a reference point for the first laminate (STK1) placed on the first pressurizing plate (PPL1). The positioning plate (POP) may block the advance of the first laminate (STK1) so that the first laminate (STK1) is cut to a predetermined size.

[0120] In one embodiment, the positioning plate (POP) may be configured to move horizontally. By moving the positioning plate horizontally to adjust its position, the size of the portion of the first laminate (STK1) that is cut can be adjusted.

[0121] The pressurizing unit (CTU) may further include a second control unit (MCU2) configured to control the positioning plate (POP). The second control unit (MCU2) may be configured to control the horizontal movement of the positioning plate (POP).

[0122] The pressurizing unit (CTU) may further include a third control unit (MCU3). The third control unit (MCU3) may be configured to control the first and second pressurizing plates (PPL1, PPL2) pressing the object. Specifically, the third control unit (MCU) may be configured to control the vertical movement of at least one of the first and second pressurizing plates (PPL1, PPL2) in a third direction (D3). The third control unit (MCU3) may control the movement of at least one of the first and second pressurizing plates (PPL1, PPL2) using a hydraulic method, a gear method, a screw method, a cam method, etc. By controlling the movement of at least one of the first and second pressurizing plates (PPL1, PPL2), the object can be pressed.

[0123] In one embodiment, the third control unit (MCU3) may be configured to control the pressure applied by the pressurizing unit (PRU) to the target body.

[0124] For example, a pressurizing unit (CTU) can manufacture a stack cell (STC) by laminating the second laminate (STK2) described below.

[0125] In one embodiment, the loading unit (TRU) may be configured to load a stack cell (STC) formed in a pressurizing unit (CTU) into a case. As an example, the loading unit (TRU) may be configured to seal the case after loading the stack cell (STC) into the case.

[0126]

[0127] Hereinafter, with reference to FIGS. 7 to 15, a method for manufacturing an all-solid-state battery according to an embodiment of the present invention will be described.

[0128] FIG. 7 is a flowchart for explaining a method for manufacturing an all-solid-state battery according to an embodiment of the present invention. Referring to FIG. 7, the method for manufacturing an all-solid-state battery (S10) may include: driving a first stacked body including a bipolar electrode (S100); placing and cutting the front portion of the first stacked body onto a first pressure plate to form a first unit electrode (S200); adjusting the position of the first pressure plate on which the first unit electrode is placed (S300); continuing to drive the first stacked body to place and cut the front portion onto the first unit electrode to form a second unit electrode (S400); and integrally forming a second stacked body including a first terminal cell and a second unit electrode (S500).

[0129] In one embodiment, driving a first laminate including a bipolar electrode (S100) may include preparing a first laminate (STK1).

[0130] In one embodiment, the first laminate (STK1) can be extended in a first direction (D1).

[0131] FIG. 8a is a cross-sectional view illustrating a first laminate (STK1) according to one embodiment. FIG. 8b is an exploded perspective view of the bipolar electrode (BIE) of FIG. 8a.

[0132] Referring to FIGS. 8a and 8b, the first laminate (STK1) may include a bipolar electrode (BIE). The bipolar electrode (BIE) may include a bipolar substrate (BPS); a first electrode composite layer (EML1) on one side of the bipolar substrate (BPS); a first gasket (GSK1) surrounding the first electrode composite layer (EML1); a second electrode composite layer (EML2) on the other side of the bipolar substrate (BPS); and a second gasket (GSK2) surrounding the second electrode composite layer (EML2).

[0133] Referring to FIGS. 6a and 6b, the first laminate (STK1) may further include a first electrolyte layer (SEL1) on one side of the bipolar electrode (BIE); and a second electrolyte layer (SEL2) on the other side of the bipolar electrode (BIE).

[0134] Each of the first gasket (GSK1) and the second gasket (GSK2) may include an opening (HH). A first electrode composite layer (EML1) may be disposed within the opening (HH) of the first gasket (GSK1), and a second electrode composite layer (EML2) may be disposed within the opening (HH) of the second gasket (GSK2). For example, the first electrode composite layer (EML1) may be formed by applying and drying an electrode slurry inside the first gasket (GSK1) on a bipolar substrate (BPS). Similarly, the second electrode composite layer (EML2) may be formed by applying and drying an electrode slurry inside the second gasket (GSK2).

[0135] In one embodiment, the first gasket (GSK1) and the second gasket (GSK2) may each include two or more openings (HH). By forming an electrode composite layer (EML) in each of the multiple openings (HH), the first laminate (STK1) can then be cut to form multiple unit electrodes (UEL).

[0136] A method for manufacturing an all-solid-state battery (S10) may include placing a first front portion, which is a front region in the first direction (D1) of a first laminate (STK1), on a first pressure plate (PPL1). Then, it may include cutting the first front portion of the first laminate (STK1) to form a first unit electrode (UEL1) (S200).

[0137] Referring to FIG. 9, in one embodiment, a first laminate (STK1) can be placed on a first pressure plate (PPL1) using the feeding unit (FDU) described above with reference to FIG. 6.

[0138] In one embodiment, the first laminate (STK1) traveling in the first direction (D1) may be stopped in front of the positioning plate (POP) described above with reference to FIG. 6. At this time, the first front portion of the first laminate (STK1) may be placed on the first pressure plate (PPL1).

[0139] Referring to FIG. 10, a first front portion of a first laminate (STK1) can be placed on a pressure plate (PPL1), and then the first laminate (STK1) can be cut to form a first unit electrode (ULE1). As a result, a second front portion, which is a new front region, can be formed in the first laminate (STK1). For example, the cutting can be performed by a cutting unit (CTU) described above with reference to FIG. 5. In one embodiment, the delivery speed of the first laminate (STK1) of the feeding unit and the cutting speed of the cutting unit can be synchronized.

[0140] Referring to FIG. 11, the method for manufacturing an all-solid-state battery (S10) may include adjusting the position of the first pressure plate (PPL1) on which the first unit electrode (UEL1) is placed (S300).

[0141] In one embodiment, the first pressure plate (PPL1) on which the first unit electrode (UEL1) is placed can be lowered so that the first unit electrode (UEL1) is positioned below the first laminate (STK1). As a result, the first laminate (STK1) traveling in the first direction (D1) can be placed on the first unit electrode (UEL1).

[0142] Referring to FIGS. 12 and 13, a method for manufacturing an all-solid-state battery (S10) may include placing and cutting a first laminate on a first unit electrode to form a second unit electrode (S400).

[0143] In one embodiment, a second front portion, which is a new front region of a first laminate (STK1), is driven in a first direction (D1) and placed on a first unit electrode, and then the first laminate (STK1) is cut to form a second unit electrode (ULE2) on a first unit electrode (UEL1).

[0144] In one embodiment, unit electrodes (UEL) can be further formed on the second unit electrode (UEL2) in the same manner as the first and second unit electrodes (UEL1, UEL2) were formed.

[0145] Referring to FIG. 14a, a method for manufacturing an all-solid-state battery (S10) may include integrally laminating a second laminate (STK2) comprising a first unit electrode (UEL1) and a second unit electrode (UEL2) (S500). The second laminate (STK2) may include first and second unit electrodes (UEL1, UEL2) stacked sequentially. In one embodiment, the second laminate (SKT2) may further include at least one unit electrode (UELn).

[0146] Referring to FIG. 14a, a stack cell (STC) can be manufactured by integrally laminating a second laminate (STK2) located between a first pressure plate (PPL1) and a second pressure plate (PPL2).

[0147] In one embodiment, laminating the second laminate (STK2) may involve applying a pressure of 1 MPa to 10 MPa to the second laminate (STK2), and for example, the pressure may be 1 MPa to 8 MPa, or 2 MPa to 6 MPa.

[0148] In one embodiment, in a stack cell (STSC) manufactured after lamination, as described above with reference to FIG. 3, the first and second gaskets (GSK1, GSK2) of the unit electrodes (UEL1, UEL2) have excellent elongation and can protrude outward from the bipolar substrate (BPS). That is, each of the first and second gaskets (GSK1, GSK2) can have a length in the first direction (D1) and a width in the second direction (D2) greater than the bipolar substrate (BPS).

[0149] FIG. 14b is a modified embodiment of the second laminate (STK2) of FIG. 14a. Referring to FIG. 14b, the second laminate (STK2) may further include first and second end electrodes (EEL1, EEL2). Specifically, it may include a first end electrode (EEL1) at the bottom and a second end electrode (EEL2) at the top.

[0150] The first and second end electrodes (EEL1, EEL2) are the same as those described above with reference to FIG. 3.

[0151] Although not illustrated, the first end electrode (EEL1) can be positioned at the bottom by first placing the first end electrode (EEL1) on the first pressure plate (PPL1) before placing the first laminate (STK1) on the first pressure plate (PPL1). That is, the first end electrode (EEL1) can be positioned at the bottom by forming the first unit electrode (UEL1) on the first end electrode (EEL1) during the first unit electrode (UEL1) formation process (S200).

[0152] In addition, by stacking unit electrodes (UELn) on the first pressure plate (PPL1) and then stacking the second end electrode (EEL2), the second end electrode (EEL2) can be positioned at the top.

[0153] In one embodiment, the first and second end electrodes (EEL1, EEL2) each can be supplied from the end electrode supply unit (EU) described above with reference to FIG. 5.

[0154] Referring to FIG. 15, the manufactured stack cell (STC) may further be loaded into a case (CSE). As described above, the first and second gaskets (GSK1, GSK2) protrude in the first direction (D1) and the second direction (D2) relative to the bipolar substrate (BPS), thereby preventing the bipolar substrate (BPS) from coming into direct contact with the side of the case (CSE), and consequently preventing a short circuit.

[0155]

[0156] FIGS. 16a to 19 are cross-sectional views illustrating a method for manufacturing an all-solid-state battery according to another embodiment. Descriptions of the same content as those described with reference to FIGS. 8a to 15 will be omitted, and the explanation will focus on the differences.

[0157] Referring again to FIG. 7, the method for manufacturing an all-solid-state battery (S10) may include driving a first laminate including a bipolar electrode (S100).

[0158] FIG. 16a is a cross-sectional view illustrating a first laminate (STK1) according to one embodiment. FIG. 16b is an exploded perspective view of the bipolar electrode (BIE) of FIG. 16a.

[0159] Referring to FIG. 16a and FIG. 16b, the first laminate (STK1) may include a bipolar substrate (BPS); a first electrode composite layer (EML1) on one side of the bipolar substrate (BPS); a first gasket (GSK1) surrounding the first electrode composite layer (EML1); a second electrode composite layer (EML2) on the other side of the bipolar substrate (BPS); and a second gasket (GSK2) surrounding the second electrode composite layer (EML2). The bipolar substrate (BPS), the first electrode composite layer (EML1), the first gasket (GSK1), the second electrode composite layer (EML2), and the second gasket (GSK2) may constitute a bipolar electrode (BIE).

[0160] The first laminate (STK1) may further include a first electrolyte layer (SEL1) on one side of the bipolar electrode (BIE); and a second electrolyte layer (SEL2) on the other side of the bipolar electrode (BIE).

[0161] Referring again to FIG. 16, the first laminate (STK1) may include a first end (ENP1); an intermediate part (MEP); and a second end (ENP2). The first end (ENP1) may not include a second electrode composite layer (EML2), a second gasket (GSK2), and a second electrolyte layer (SEL2) on the lower surface of the bipolar substrate (BPS). The first end (ENP1) may subsequently be cut to become the first end electrode (EEL1) described above with reference to FIG. 4.

[0162] By using the first stack (STK1) with the above structure, a stack cell (STC) can be manufactured without separately supplying the first end electrode (EEL1) and the second end electrode (EEL2).

[0163]

[0164] The second end (ENP2) may not include the first electrode composite layer (EML1), the first gasket (GSK1), and the first electrolyte layer (SEL1) on the upper surface of the bipolar substrate (BPS). The second end (ENP2) may then be cut to become the second end electrode (EEL2) described above with reference to FIG. 4.

[0165] As described above, the intermediate portion (MEP) may include a bipolar substrate (BPS); a first electrode composite layer (EML1) on one side of the bipolar substrate (BPS); a first gasket (GSK1) surrounding the first electrode composite layer (EML1); a second electrode composite layer (EML2) on the other side of the bipolar substrate (BPS); and a second gasket (GSK2) surrounding the second electrode composite layer (EML2). The intermediate portion (MEP) may further include a first electrolyte layer (SEL1) on one side of the bipolar electrode (BIE); and a second electrolyte layer (SEL2) on the other side of the bipolar electrode (BIE). The intermediate portion (MEP) may subsequently be cut to become the first and second unit electrodes (UEL1, UEL2) described above with reference to FIG. 4.

[0166] Referring to FIG. 17, a method for manufacturing an all-solid-state battery may include placing and cutting a first end (ENP1), which is a front region of a first laminate (STK1), on a first pressure plate (PPL1) to form a first end electrode (EEL1).

[0167] Referring to FIG. 17, a first end (ENP1), which is a front region of a first laminate (STK1), is placed on a pressure plate (PPL1), and then the first laminate (STK1) is cut to form a first end electrode (EEL1). As a result, a second front region, which is a new front region, can be formed in the middle portion (MEP) of the first laminate (STK1).

[0168] Referring to FIG. 17, the method for manufacturing an all-solid-state battery may further include adjusting the position of a first pressure plate (PPL1) on which a first end electrode (EEL1) is placed.

[0169] In one embodiment, the first pressure plate (PPL1) on which the first end electrode (EEL1) is placed can be lowered so that the first end electrode (EEL1) is positioned below the first laminate (STK1). As a result, the first laminate (STK1) traveling in the first direction (D1) can be placed on the first end electrode (EEL1).

[0170]

[0171] Referring to FIGS. 7 and FIGS. 18, a method for manufacturing an all-solid-state battery may include placing and cutting the front portion of a first laminate (STK1) on a first pressure plate to form a first unit electrode (S200).

[0172] In one embodiment, the intermediate portion (MEP) of the first laminate (STK1) can be placed on the first end electrode (EEL1) using the feeding unit (FDU) described above with reference to FIG. 6. That is, the intermediate portion (MEP) of the first laminate (STK1) can be laminated on the first end electrode (EEL1) placed on the first pressure plate (PPL1). Then, by cutting the intermediate portion (MEP) of the first laminate (STK1), a first unit electrode (ULE1) can be formed on the first end electrode (EEL1).

[0173] A second unit electrode (UEL2) can be formed on the first unit electrode (UEL1) in the same manner as the first unit electrode (ULE1) was formed. Additionally, at least one unit electrode (UELn) can be further formed on the second unit electrode (UEL2).

[0174] In one embodiment, a second end electrode (EEL2) may be located at the top of the unit electrodes (UELn). The second end electrode (EEL2) may be formed by cutting the second end (ENP2) of the first laminate (STK1).

[0175] Referring to FIG. 19, the method for manufacturing an all-solid-state battery (S10) may include laminating a second laminate (STK2) including a first unit electrode (UEL1) and a second unit electrode (UEL2) as a whole (S500).

[0176] In one embodiment, the pressure for laminating the second laminate (STK2) may be 1 MPa to 10 MPa, and for example, 1 MPa to 8 MPa, or 2 MPa to 6 MPa.

[0177] In one embodiment, in a stack cell (STSC) manufactured after lamination, as described above with reference to FIG. 4, the first and second gaskets (GSK1, GSK2) of the unit electrodes (UEL1, UEL2) have excellent elasticity and can protrude outward from the bipolar substrate (BPS). That is, each of the first and second gaskets (GSK1, GSK2) can have a length in the first direction (D1) and a width in the second direction (D2) greater than the bipolar substrate (BPS).

[0178] A method for manufacturing an all-solid-state battery may further include loading a stack cell (STC) into a case (CSE) as described above with reference to FIG. 15. As described above, the first and second gaskets (GSK1, GSK2) protrude in the first direction (D1) and the second direction (D2) relative to the bipolar substrate (BPS), thereby preventing the bipolar substrate (BPS) from coming into direct contact with the side of the case (CSE), and consequently preventing a short circuit.

[0179]

[0180] Although preferred embodiments of the present invention have been described above, the present invention is not limited thereto and can be implemented with various modifications within the scope of the claims, the detailed description of the invention, and the attached drawings, and it is obvious that such modifications also fall within the scope of the present invention.

Claims

1. Driving a first laminated body extended in a first direction in the first direction; Placing a first front portion, which is the front region of the first laminate, on a first pressure plate; The first front portion is cut to form a first unit electrode, and by the cutting, the first laminate is formed with a second front portion, which is a new front region; Adjusting the position of the first pressure plate on which the first unit electrode is placed; Driving the first laminated body in the first direction to place the second front portion on the first unit electrode; Cutting the second front portion to form a second unit electrode; and A method for manufacturing an all-solid-state battery comprising laminating a second laminate including the first and second unit electrodes stacked sequentially.

2. In Paragraph 1, The first unit electrode above is: Bipolar electrode; A first electrolyte layer on one surface of the above-mentioned bipolar electrode; and A method for manufacturing an all-solid-state battery comprising a second electrolyte layer on the other side of the above-mentioned bipolar electrode.

3. In Paragraph 2, The above bipolar electrode is: Current collector; A first electrode composite layer on one side of the above current collector; A second electrode composite layer on the other side of the above current collector; A first gasket surrounding the side of the first electrode composite layer; and It includes a second gasket surrounding the side of the second electrode composite layer, and A method for manufacturing an all-solid-state battery in which the first electrode composite layer and the first electrolyte layer are in contact.

4. In Paragraph 3, The first electrode composite layer includes a positive active material layer, and A method for manufacturing an all-solid-state battery, wherein the positive active material layer comprises a positive active material and a solid electrolyte.

5. In Paragraph 2, A method for manufacturing an all-solid-state battery, wherein at least one of the first and second electrolyte layers comprises a sulfide-based solid electrolyte.

6. In Paragraph 1, Adjusting the position of the first pressure plate is: A method for manufacturing an all-solid-state battery, comprising lowering the first pressure plate so that the first unit electrode is positioned below the first laminate.

7. In Paragraph 1, Laminating the above-mentioned second laminate as a whole is: A method for manufacturing an all-solid-state battery, comprising applying a pressure of 1 MPa to 10 MPa to the second laminate.

8. In Paragraph 1, It further includes placing a first end electrode on a first pressure plate, and A method for manufacturing an all-solid-state battery, wherein the first front portion of the first laminate is disposed on the first end electrode.

9. In Paragraph 8, A method for manufacturing an all-solid-state battery, wherein the first end electrode comprises a monopolar electrode and a solid electrolyte layer on the monopolar electrode.

10. In Paragraph 1, A stack cell is formed by laminating the above second laminated body, and A method for manufacturing an all-solid-state battery, wherein the above manufacturing method further comprises loading the stack cell into a case.

11. Driving a first laminated body extended in a first direction in said first direction, said first laminated body comprising a first end, an intermediate part, and a second end; Cutting the first end portion, which is the front region of the first laminate, to form a first end electrode on the first pressure plate of the pressure unit; Cutting the intermediate portion, which is a new front region of the first laminate, to form a unit electrode on the first end electrode; Cutting the second end, which is a new front region of the first laminate, to form a second end electrode on the unit electrode; and A method for manufacturing an all-solid-state battery comprising integrally laminating a second laminate comprising the first end electrode, the unit electrode, and the second end electrode, which are sequentially stacked.

12. In Paragraph 11, The first end electrode comprises a monopolar electrode and a solid electrolyte layer on the monopolar electrode, wherein A method for manufacturing an all-solid-state battery, wherein the monopolar electrode comprises either a positive electrode layer or a negative electrode layer.

13. In Paragraph 11, The first unit electrode above is: Bipolar electrode; A first electrolyte layer on one surface of the above-mentioned bipolar electrode; and A method for manufacturing an all-solid-state battery comprising a second electrolyte layer on the other side of the above-mentioned bipolar electrode.

14. In Paragraph 13, The above bipolar electrode is: Current collector; A first electrode composite layer on one side of the above current collector; A second electrode composite layer on the other side of the above current collector; A first gasket surrounding the side of the first electrode composite layer; and It includes a second gasket surrounding the side of the second electrode composite layer, and A method for manufacturing an all-solid-state battery in which the first electrode composite layer and the first electrolyte layer are in contact.

15. In Paragraph 11, Laminating the above-mentioned second laminate as a whole is: A method for manufacturing an all-solid-state battery, comprising applying a pressure of 1 MPa to 10 MPa to the second laminate.

16. In Paragraph 11, A stack cell is formed by laminating the above second laminated body, and A method for manufacturing an all-solid-state battery, wherein the above manufacturing method further comprises loading the stack cell into a case.

17. A feeding unit configured to deliver the first laminate to a pressurizing unit; A cutting unit configured to cut the first laminate; and A pressurizing unit configured to stack and laminate unit electrodes formed by cutting the first laminate, wherein The above pressurization unit is: A first pressure plate and a second pressure plate facing each other; and A solid-state battery manufacturing apparatus comprising a first control unit configured to adjust the position of the first pressure plate.

18. In Paragraph 17, The above feeding unit is configured to deliver the first laminate onto the first pressure plate, and The above cutting unit is configured to cut the front region of the first laminate disposed on the first pressure plate, an all-solid-state battery manufacturing apparatus.

19. In Paragraph 17, The above-mentioned pressure unit further includes a positioning plate configured to align the front region of the first laminated body onto the first pressure plate, wherein The above positioning plate is disposed between the first and second pressure plates, forming an all-solid-state battery manufacturing device.

20. In Paragraph 19, The above-mentioned pressurizing unit further comprises a second control unit configured to control the movement of the positioning plate, an all-solid-state battery manufacturing apparatus.

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