All-solid-state battery and manufacturing method therefor

Abstract

The present invention relates to an all-solid-state battery and a manufacturing method therefor and, more specifically, to an all-solid-state battery manufacturing method comprising the steps of: forming a first transfer layer on a first release substrate so as to prepare a first transfer member; slitting one side surface of the first transfer member; transferring, onto a cathode substrate, the first transfer layer on the first release substrate; and slitting the other side surface of the first transfer layer together with the cathode substrate so as to prepare a first electrode.

Description

All-solid-state battery and method for manufacturing the same

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

[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 a method for manufacturing an all-solid-state battery capable of preventing the detachment of the positive electrode active material layer and the resulting short circuit.

[0007] Another problem that the present invention aims to solve is to provide an all-solid-state battery capable of preventing the detachment of the positive active material layer and the resulting short circuit.

[0008]

[0009] A method for manufacturing an all-solid-state battery according to the concept of the present invention may include: preparing a first transfer member by forming a first transfer layer on a first release substrate; slitting one side of the first transfer member; transferring the first transfer layer on the first release substrate onto an anode substrate; and preparing a first electrode by slitting the other side of the first transfer layer together with the anode substrate. The first transfer layer may include at least one of a first solid electrolyte layer and an anode active material layer.

[0010] An all-solid-state battery according to another concept of the present invention may comprise a positive electrode substrate; a first positive electrode active material layer on the positive electrode substrate; and a first transfer layer on the first positive electrode active material layer. The first transfer layer may comprise at least one of a second positive electrode active material layer and a first solid electrolyte layer. One side of the positive electrode substrate may include a first tab portion protruding in a first direction. The first positive electrode active material layer may include a first side adjacent to the first tab portion. The first transfer layer may include a second side adjacent to the first tab portion, wherein the first inclination angle formed between the first side and the lower surface of the positive electrode substrate is 85° to 95°, and the second inclination angle formed between the second side and the lower surface of the first positive electrode active material layer is 85° to 95°.

[0011]

[0012] A method for manufacturing an all-solid-state battery according to the concept of the present invention prevents the formation of a slope at the end of the positive active material layer by forming and slitting the positive active material layer on a separate member and then transferring it onto the positive substrate, without directly coating the positive active material layer onto the positive substrate. Through this, the detachment of the positive active material layer can be prevented, and short circuits can be prevented without a separate insulating film. In addition, the occurrence of defects can be reduced.

[0013] The all-solid-state battery according to the concept of the present invention has excellent lifespan characteristics.

[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 of an all-solid-state battery according to another embodiment of the present invention.

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

[0019] FIG. 5 is a cross-sectional view of an all-solid-state battery according to another embodiment of the present invention.

[0020] FIG. 6 is a cross-sectional view of an all-solid-state battery according to another embodiment of the present invention.

[0021] FIG. 7a is a cross-sectional view of an all-solid-state battery according to another embodiment of the present invention.

[0022] FIG. 7b is a cross-sectional view of an all-solid-state battery according to another embodiment of the present invention. FIG. 7c and FIG. 7d are enlarged views showing region M of FIG. 7b and region N of FIG. 7b.

[0023] FIG. 8a is a plan view illustrating a positive electrode for an all-solid-state battery according to a comparative example. FIG. 8b is a cross-sectional view along the line A-A' of FIG. 8a.

[0024] FIG. 9 is a flowchart for explaining a method for manufacturing an all-solid-state battery according to one embodiment of the present invention.

[0025] FIGS. 10a to 10d are cross-sectional views illustrating the formation of a first transfer layer on a first release substrate. FIG. 10e is a cross-sectional view along line A-A' of FIG. 10d. FIG. 10f is a cross-sectional view along line B-B' of FIG. 10d.

[0026] FIG. 10g is a cross-sectional view illustrating the removal of the first peeling substrate.

[0027] FIG. 10h is a cross-sectional view illustrating slitting the other side of the first electrode.

[0028] FIG. 11 is a flowchart for explaining a method for manufacturing an all-solid-state battery according to another embodiment of the present invention.

[0029] FIG. 12a is a cross-sectional view illustrating the preparation of the first and second transfer members.

[0030] FIGS. 12b and FIGS. 12c are cross-sectional views illustrating slitting one side of the first and second transfer members.

[0031] FIGS. 12d to 12g are cross-sectional views for illustrating the transfer of the transfer layers of the first and second transfer members.

[0032] FIG. 12h is a cross-sectional view illustrating slitting the other side of the first electrode.

[0033] FIG. 13a is a plan view illustrating the first electrode of an all-solid-state battery manufactured by the manufacturing method (S10) described above with reference to FIG. 9. FIG. 13b is a cross-sectional view along the line A-A' of FIG. 13a. FIG. 13c is a cross-sectional view along the line B-B' of FIG. 13a.

[0034] FIG. 14a is a plan view illustrating a first electrode of an all-solid-state battery manufactured by the manufacturing method (S10a) described above with reference to FIG. 11. FIG. 14b is a cross-sectional view along the line A-A' of FIG. 14a. FIG. 14c to 14e are examples of partial modifications of the first electrode of FIG. 14a.

[0035] FIG. 15 is a flowchart for explaining a method for manufacturing an all-solid-state battery according to another embodiment of the present invention.

[0036] FIGS. 16a to 16g are cross-sectional views illustrating the formation of a first electrode comprising a plurality of positive active material layers.

[0037] FIG. 17a is a plan view illustrating the first electrode of an all-solid-state battery manufactured by the manufacturing method (S10) described above with reference to FIG. 15, FIG. 17b is a cross-sectional view along the line A-A' of FIG. 17a, and FIG. 17c is a cross-sectional view along the line B-B' of FIG. 17a.

[0038] FIGS. 18a to 18c are cross-sectional views for explaining the first electrode of an all-solid-state battery manufactured by the manufacturing method (S10) described above with reference to FIG. 15, and FIGS. 18a to 18c are cross-sectional views according to other embodiments of FIG. 17b.

[0039] FIGS. 19 to 21 are conceptual diagrams for explaining a method of manufacturing an all-solid-state battery using a first electrode manufactured by the manufacturing method described above with reference to FIG. 15.

[0040]

[0041] 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.

[0042] 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.

[0043] 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.

[0044] Unless otherwise specified in this specification, the singular form may also include the plural. 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.

[0045] 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.

[0046] 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.

[0047] 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).

[0048] 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.

[0049] 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.

[0050] 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).

[0051] 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.

[0052] 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.

[0053] 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.

[0054] 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.

[0055] 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.

[0056] 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.

[0057] 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).

[0058] 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.

[0059] 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.

[0060] 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.

[0061] 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.

[0062] 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.

[0063] 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.

[0064] 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.

[0065] 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.

[0066] 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.

[0067] 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.

[0068] 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).

[0069] 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.

[0070] 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).

[0071] 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).

[0072] 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).

[0073] 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).

[0074] 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.

[0075] The solid electrolyte in the solid electrolyte layer (300) may have particle shapes such as spheres or ellipsoids.

[0076] 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.

[0077] In one embodiment, the solid electrolyte in the solid electrolyte layer (300) is Li 7-a M a PS 6-c X c It may be an argyrodite-type compound containing. Here, X may be Cl, Br, or a combination thereof. M may be Na, K, Fe, Mg, Ca, Ag, Cu, Zr, Zn, or a combination thereof. a and c may each be real numbers between 0 and 2.

[0078] 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.

[0079] 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).

[0080] 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).

[0081] 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.

[0082] 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.

[0083] 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.

[0084] 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.

[0085] 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.

[0086] 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.

[0087] 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.

[0088] 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.

[0089] 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.

[0090] 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.

[0091] Referring to FIGS. 1 and 2, the area of ​​the anode layer (100) and the area of ​​the cathode layer (200) may differ 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 superimposed within the cathode layer (200).

[0092] In one embodiment of the present invention, the first solid electrolyte layer (310) may have substantially the same area as the anode layer (100). The second solid electrolyte layer (320) may have substantially the same area as the cathode layer (200).

[0093] Referring to FIGS. 1 and 2, 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).

[0094] 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 above numerical range is exceeded, 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 above numerical range is not met, it is difficult to suppress the formation of lithium dendrites in the negative electrode, and there may be a risk of a short circuit.

[0095] 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.

[0096] 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.

[0097] Referring to FIGS. 1 and 2, the first solid electrolyte layer (310) may have a third width (W3) in the second direction (D2). The second solid electrolyte layer (320) may have a fourth width (W4) in the second direction (D2). The third width (W3) may be smaller than the fourth width (W4).

[0098] The difference between the third width (W3) and the fourth width (W4) may be 10 mm or less. Specifically, the difference between the third width (W3) and the fourth width (W4) may be 8 mm or less, 5 mm or less, or 3 mm or less. The difference between the fourth width (W4) and the third width (W3) may be 0.1 mm or more, 0.5 mm or more, or 1 mm or more. If the above numerical range is exceeded, 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 above numerical range is not met, it is difficult to suppress the formation of lithium dendrites in the negative electrode, and there may be a risk of a short circuit.

[0099] The ratio (W4 / W3) of the fourth width (W4) to the third width (W3) may be 1 to 1.6. Specifically, the ratio (W4 / W3) of the fourth width (W4) to the third width (W3) may be 1 to 1.5, 1 to 1.4, 1 to 1.3, 1 to 1.2, or 1 to 1.1.

[0100] If the ratio (W4 / W3) of the fourth width (W4) to the third width (W3) exceeds the numerical range, the energy density of the all-solid-state battery (10) is reduced.

[0101]

[0102] FIG. 3 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 and FIG. 2 are omitted, and differences are described in detail.

[0103] Referring to FIG. 3, 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) serves 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).

[0104] 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.

[0105] The lithium metal layer (400) may have a fifth width (W5) in the first direction (D1). 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).

[0106] FIG. 4 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 to 3 are omitted, and differences are described in detail.

[0107] Referring to FIG. 4, the bi-cell all-solid-state battery (20) may include a first monocell (510) and a second monocell (520).

[0108] Each of the first and second monocells (510, 520) may include an anode layer (100), a cathode layer (200), and a solid electrolyte layer (300) disposed between the anode layer (100) and the cathode layer (200). The solid electrolyte layer (300) of each of the first and second monocells (510, 520) may include a first solid electrolyte layer (310) adjacent to the anode layer (100) and having a first width (W1) and a first thickness (t1), and a second solid electrolyte layer (320) adjacent to the cathode layer (200) and having a second width (W2) and a second thickness (t2). The second monocell (520) may be arranged vertically symmetrically with respect to the first monocell (510). The anode layer (100) of the first monocell (510) and the anode layer (100) of the second monocell (520) can face each other.

[0109] FIG. 5 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 to 4 are omitted, and differences are described in detail.

[0110] Referring to FIG. 5, the bi-cell all-solid-state battery (20) may further include an elastic member (ELP) disposed on one side of the negative electrode layer (200). The elastic member (ELP) is composed of members capable of absorbing volume changes (expansion) of the all-solid-state battery (20) due to charging and discharging, and is capable of elastic deformation; more specifically, it may be composed of a material having a lower elastic modulus than that of the positive current collector and the negative current collector. The material constituting the elastic member (ELP) may have a slope of the stress-displacement curve of 200 MPa or less at a displacement of 80% or less. Specifically, the material constituting the elastic member (ELP) may have a slope of the stress-displacement curve of 50 MPa or less at a displacement of 80% or less, and 10 MPa or less at a displacement of 50% or less.

[0111] Examples of materials for the above elastic member (ELP) include, but are not limited to, epoxy resin, acrylic resin, polyimide resin, polyester resin, polypropylene resin, polyamide resin, polystyrene resin, polyvinyl chloride resin, polycarbonate resin, fluoropolymer resin such as PTFE, silicone rubber, etc. Each elastic member (ELP) may be composed of a single material or may be composed of a combination of several materials. In addition, each elastic member (ELP) may include the same material or may include different materials. Furthermore, the elastic member (ELP) may include an insulating material and may insulate between each bicell all-solid-state battery (20). The insulating material has a surface resistance value of 1.0*10 17 Ω·cm 2 It may be the above, and specifically, it may be a fluoropolymer such as PTFE or silicone rubber, etc.

[0112] Since an elastic member (ELP) is disposed between each bicell all-solid-state battery (20), the pressure generated when the all-solid-state battery (20) is charged and expanded can be dispersed, thereby reducing the uneven distribution of pressure applied to each all-solid-state battery (20) due to charging and discharging. In addition, this can suppress cracking or deformation of the electrolyte layer that may occur as charging and discharging are repeated, and can suppress deterioration of battery characteristics such as cycle characteristics.

[0113] FIG. 6 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 to 5 are omitted, and differences are described in detail.

[0114] Referring to FIG. 6, the all-solid-state battery (20) may further include an inert member (INM) disposed on one side of the positive electrode layer (100) and the first solid electrolyte layer (310). By including the inert member (INM), cracking of the solid electrolyte layer (300) is prevented during manufacturing and / or charging and discharging of the all-solid-state battery (20), and consequently, the cycle characteristics of the all-solid-state battery (20) can be improved.

[0115] The inert member (INM) may include one or more selected from lithium-ion insulators and lithium-ion conductors. The inert member (INM) may be an electronic insulator; that is, the inert member (INM) may not be an electronic conductor. The inert member (INM) may be an ion insulator; that is, the inert member (INM) may not be an ion conductor. The inert member (INM) includes, for example, organic materials, inorganic materials, or organic-inorganic composite materials. Organic materials may be, for example, polymers. Inorganic materials may be ceramics, for example, metal oxides. Organic-inorganic composite materials may be a composite of a polymer and a metal oxide.

[0116] The above inert member (INM) may be disposed between the second solid electrolyte layer (320) of the first monocell (510) and the second solid electrolyte layer (320) of the second monocell (520). By including the inert member (INM), uniform pressure can be applied during the manufacturing process of the all-solid-state battery (20), thereby preventing cracking of the solid electrolyte layer (300) and consequently improving the cycle characteristics of the all-solid-state battery (20).

[0117] The thickness of the inert member (INM) may be equal to or less than the sum of the thickness (t1) of the first solid electrolyte layer (310) of the first monocell (510) and the thickness of the anode layer (100), and the thickness (t1) of the first solid electrolyte layer (310) of the second monocell (520) and the thickness of the anode layer (100). The thickness of the inert member (INM) may be greater than the thickness of the anode layer (100). If the thickness of the inert member (INM) is smaller than the thickness of the anode layer (100), appropriate pressure is not applied to the side of the second solid electrolyte layer (320), and cracks may occur in the solid electrolyte layer (300). If the thickness of the above inert member (INM) is greater than the sum of the thickness (t1) of the first solid electrolyte layer (310) of the first monocell (510) and the thickness of the anode layer (100), and the thickness (t1) of the first solid electrolyte layer (310) of the second monocell (520) and the thickness of the anode layer (100), the anode layer (100) and the first solid electrolyte layer (310) may not be sufficiently pressurized.

[0118] FIG. 7a is a cross-sectional view of an all-solid-state battery according to another embodiment of the present invention.

[0119] Referring to FIG. 7a, the positive current collector (110) may provide a reference surface on which the positive active material layer (120) is placed. The positive current collector (110) may have a portion protruding from the positive active material layer (120) in a first direction (D1). The protruding portion may be a positive non-positive portion. The protruding portion may be a tab of the positive. The negative current collector (210) may provide a reference surface on which the negative coating layer (220) is placed. The negative current collector (210) may have a portion protruding from the negative coating layer (220) in the opposite direction of the first direction (D1). The protruding portion may be a tab of the negative. An inert member (INM) may surround the side of the positive active material layer (120) and the side of the first solid electrolyte layer (310).

[0120]

[0121] FIG. 7b is a cross-sectional view of an all-solid-state battery according to another embodiment of the present invention. FIG. 7c and FIG. 7d are enlarged views showing the M region of FIG. 7b and the N region of FIG. 7b. In these embodiments, detailed descriptions of technical features that overlap with those previously described with reference to FIG. 1 to FIG. 7a are omitted, and differences are described in detail.

[0122] Referring to FIG. 7b, the positive current collector (110) may provide a reference surface on which the positive active material layer (120) is placed. That is, the positive current collector (110) may be a positive substrate. The positive current collector (110) may include an active portion (AAP) and a tab portion (ATP). The positive active material layer (120) may be placed on the active portion (AAP) of the positive current collector (110). The tab portion (ATP) of the positive current collector (110) may be a portion protruding from the active portion (AAP) in the first direction (D1). The tab portion (ATP) of the positive current collector (100) may be a non-positive portion. The negative current collector (210) may provide a reference surface on which the negative coating layer (220) is placed. The negative current collector (210) may have a portion protruding from the negative coating layer (220) in the opposite direction of the first direction (D1). The above protruding part may be a tab of the negative electrode.

[0123] The positive active material layer (120) may include a first positive active material layer (120_1) on the positive current collector (110) and a second positive active material layer (120_2) on the first positive active material layer (120_1). The content of the positive active material included in the first positive active material layer (120_1) may be greater than the content of the positive active material included in the second positive active material layer (120_2). That is, the positive active material layer (120) may have a structure including a double layer or multiple layers. Due to the structure including a double layer or multiple layers, the first positive active material layer (120_1) may be spaced apart from the solid electrolyte layer (300).

[0124] The thickness of the first positive active material layer (120_1) may be greater than the thickness of the second positive active material layer (120_2). As another example, the thickness of the first positive active material layer (120_1) and the thickness of the second positive active material layer (120_2) may be the same. The thickness of the first positive active material layer (120_1) may be greater than the thickness of the solid electrolyte layer (300), and the thickness of the second positive active material layer (120_2) may be smaller than the thickness of the solid electrolyte layer (300).

[0125] For example, the thickness of the positive active material layer (120) may be 120 μm or less. Specifically, the thickness of the positive active material layer (120) may be 110 μm or less and 90 μm or less. The thickness of the positive active material layer (120) may be 50 μm or more. Specifically, the thickness of the positive active material layer (120) may be 60 μm or more, 70 μm or more, and 80 μm or more.

[0126] For example, the thickness of the first positive active material layer (120_1) may be 60 μm or less. Specifically, the thickness of the first positive active material layer (120_1) may be 50 μm or less, 40 μm or less, or 30 μm or less. The thickness of the first positive active material layer (120_1) may be 10 μm or more. Specifically, the thickness of the first positive active material layer (120_1) may be 15 μm or more, 20 μm or more, or 25 μm or more.

[0127] For example, the thickness of the second positive active material layer (120_2) may be 60 μm or less. Specifically, the thickness of the second positive active material layer (120_2) may be 50 μm or less, 40 μm or less, or 30 μm or less. The thickness of the second positive active material layer (120_2) may be 10 μm or more. Specifically, the thickness of the second positive active material layer (120_2) may be 15 μm or more, 20 μm or more, or 25 μm or more.

[0128] If the thickness of the positive active material layer (120) exceeds the aforementioned numerical range, deformation of the edge portion (uneven portion) of the all-solid-state battery (10) may occur, and delamination of the positive active material may occur when pressurized during the manufacturing process of the all-solid-state battery (10).

[0129] The loading level of the positive active material layer (120) on the positive current collector (110) is 10 mg / cm 2 Up to 50 mg / cm² 2 It may be. Specifically, the loading level of the positive active material layer (120) is 15 mg / cm² 2 Up to 45 mg / cm² 2 It may be 20 mg / cm² 2 Up to 40 mg / cm² 2 It may be 20 mg / cm² 2 Up to 30 mg / cm² 2 It may be possible. If the loading level of the positive active material layer (120) exceeds the value mentioned above, the diffusion path of lithium ions may be lengthened, and the charging and discharging performance of the all-solid-state battery (10) may be reduced.

[0130] The inert member (INM) may surround the sides of the first positive active material layer (120_1) and the second positive active material layer (120_2). The inert member (INM) may be placed on the solid electrolyte layer (300).

[0131] Referring to FIGS. 7c and 7d, an air gap (AGP) may be interposed between the first positive active material layer (120_1) and the inert member (INM), and between the second positive active material layer (120_2) and the inert member (INM). An air gap (AGP) may be interposed between the first positive active material layer (120_1) and the inert member (INM), between the second positive active material layer (120_2) and the inert member (INM), and between the positive current collector (110) and the inert member (INM). For example, the air gap (AGP) may be a void or a seam.

[0132] The first positive active material layer (120_1) may include a first side (SID1) adjacent to the tab portion (ATP) of the positive current collector (110). The second positive active material layer (120_2) may include a second side (SID2) adjacent to the tab portion (ATP) of the positive current collector (110). The first positive active material layer (120_1) may include a first inclination angle (θ1) formed by the first side (SID1) and the lower surface of the positive current collector (110). The second positive active material layer (120_2) may include a second inclination angle (θ2) formed by the second side (SID2) and the lower surface of the first positive active material layer (120_1).

[0133] The first positive active material layer (120_1) may include a third side (SID3) that is spaced apart from the tab portion (ATP) of the positive current collector (110) and adjacent to the active portion (AAP). The third side (SID3) may be spaced apart from the aforementioned first side (SID1) in the first direction (D1). The second positive active material layer (120_2) may include a fourth side (SID4) that is spaced apart from the tab portion (ATP) of the positive current collector (110) and adjacent to the active portion (AAP). The fourth side (SID4) may be spaced apart from the aforementioned second side (SID2) in the first direction (D1). The first positive active material layer (120_1) may include a third inclination angle (θ3) formed by the third side (SID3) and the lower surface of the positive current collector (110). The second positive active material layer (120_2) may include a fourth inclination angle (θ4) formed by the fourth side (SID4) and the lower surface of the first positive active material layer (120_1). The positive current collector (110) may include a fifth side (SID5) aligned with the third side (SID3) and the fourth side (SID4). The positive current collector (110) may include a fifth inclination angle (θ5) formed by the fifth side (SID5) and the upper surface of the positive current collector (110).

[0134] The first angle of inclination (θ1) and the second angle of inclination (θ2) may be substantially the same as each other. As another example, the first angle of inclination (θ1) and the second angle of inclination (θ2) may be different from each other. The third angle of inclination (θ3) and the fourth angle of inclination (θ4) may be substantially the same as each other. Also, the fifth angle of inclination (θ5) may be the same as the third angle of inclination (θ3) and the fourth angle of inclination (θ4). As another example, the third angle of inclination (θ3) and the fourth angle of inclination (θ4) may be different from each other.

[0135] If the first inclination angle (θ1) and the second inclination angle (θ2) are the same, the first side (SID1) and the second side (SID2) can be aligned with each other. If the third inclination angle (θ3), the fourth inclination angle (θ4), and the fifth inclination angle (θ5) are the same, the third side (SID3), the fourth side (SID4), and the fifth side (SID5) can be aligned with each other.

[0136] Each of the first to fifth inclination angles (θ1, θ2, θ3, θ4, θ5) may have an angle close to a right angle. Specifically, each of the first to fourth inclination angles (θ1, θ2, θ3, θ4) may be greater than 85° and less than 95°. The fifth inclination angle (θ5) may be greater than 85° and less than 95°. As another example, each of the first to fifth inclination angles (θ1, θ2, θ3, θ4, θ5) may be 90°.

[0137]

[0138] FIG. 8a is a plan view illustrating a positive electrode for an all-solid-state battery according to a comparative example. FIG. 8b is a cross-sectional view along the line A-A' of FIG. 8a.

[0139] Referring to FIGS. 8a and 8b, when a positive active material slurry is directly applied and coated onto a positive current collector (110), a slope may occur at the end portion (EDG) of the positive active material layer (120), and as a result, proper pressure may not be applied to the end portion (EDG). Consequently, delamination may occur at the end portion (EDG), which may act as a cause of short circuit.

[0140] A method for manufacturing an all-solid-state battery according to embodiments of the present invention can prevent the detachment of the positive active material layer and the resulting short circuit by forming a positive active material layer on a separate peeling substrate, slitting it, and then transferring the positive active material layer onto a positive current collector.

[0141] Specifically, in the all-solid-state battery according to FIGS. 8a and 8b, the end portion (EDG) has a slope, so the angle of inclination is less than 80°, which may cause detachment and a short circuit at the end portion of the positive active material layer. In contrast, the first to fourth angles of inclination (θ1, θ2, θ3, θ4) of the all-solid-state battery (10) according to one embodiment of the present invention are each greater than 85° and less than 95°, so appropriate pressurization can be applied during the subsequent manufacturing process. That is, the all-solid-state battery (10) according to one embodiment of the present invention can prevent detachment of the positive active material layer (120) and a short circuit caused thereby. Thus, an all-solid-state battery with improved lifespan characteristics and stability can be provided.

[0142] Hereinafter, a method for manufacturing an all-solid-state battery according to embodiments of the present invention will be described in detail.

[0143]

[0144] FIG. 9 is a flowchart for explaining a method for manufacturing an all-solid-state battery according to one embodiment of the present invention.

[0145] Referring to FIG. 9, a method (S10) for manufacturing an all-solid-state battery according to one embodiment of the present invention may include manufacturing a first electrode. Specifically, manufacturing the first electrode may include: preparing a first transfer member by forming a first transfer layer on a first release substrate (S100); slitting one side of the first transfer member (S200); transferring the first transfer layer on the first release substrate onto an anode substrate (S300); and slitting the other side of the first transfer layer integrally with the anode substrate (S400).

[0146] FIGS. 10a to 10d are cross-sectional views illustrating the formation of a first transfer layer on a first peeling substrate.

[0147] Referring to FIG. 9 and FIG. 10a, in one embodiment, a first transfer layer (TRL1) can be formed on a first peeling substrate (PES1). Through this, a first transfer member (TRM1) can be prepared.

[0148] In one embodiment, the first transfer layer (TRL1) may include at least one of the first solid electrolyte layer (SEL1) and the positive active material layer (CML). In one example, the first transfer layer (TRL1) may include the first solid electrolyte layer (SEL1) and the positive active material layer (CML) on the first solid electrolyte layer (SEL1).

[0149] In one embodiment, forming a first transfer layer (TRL1) on a first peelable substrate (PES1) may include forming a first solid electrolyte layer (SEL1) on the first peelable substrate (PES1); and forming an anode active material layer (CML) on the first solid electrolyte layer (SEL1).

[0150] The material of the first peeling substrate (PES1) is not particularly limited, and a material that can be easily peeled off during a transfer process may be used. In one embodiment, the first peeling substrate (PES1) may have a single-layer or multi-layer structure. In one embodiment, the first peeling substrate (PES1) may include a polymer film or a metal film. For example, the first peeling substrate (PES1) may include at least one of a polyethylene terephthalate (PET) film, a polycarbonate (PC) film, a polyurethane (PU) film, and a polyvinyl alcohol (PVA) film. For example, the first peeling substrate (PES1) may include 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.

[0151] In one embodiment, the material of the first peeling substrate (PES1) may be the same as the material of the anode current collector (110) described above with reference to FIG. 1. As an example, the first peeling substrate (PES1) may be aluminum foil.

[0152] In one embodiment, the first solid electrolyte layer (SEL1) may correspond to the first solid electrolyte layer (310) of the all-solid-state battery (10) described above with reference to FIG. 1. As an example, the first solid electrolyte layer (SEL1) may include the solid electrolyte described above with reference to FIG. 1.

[0153] The method of forming the first solid electrolyte layer (SEL1) on the first peelable substrate (PES1) is not particularly limited. In one embodiment, forming the first solid electrolyte layer (SEL1) on the first peelable substrate (PES1) may include directly coating the first solid electrolyte slurry on the first peelable substrate (PES1).

[0154] In another embodiment, forming a first solid electrolyte layer (SEL1) on a first release substrate (PES1) may include laminating a first solid electrolyte layer (SEL1) in the form of a self-supporting film on the first release substrate (PES1). As an example, the first solid electrolyte layer (SEL1) in the form of a self-supporting film may be manufactured by coating a first solid electrolyte slurry on a release film or a porous film.

[0155] Referring again to FIG. 9 and FIG. 10a, forming a first transfer layer (TRL1) on a first peeling substrate (PES1) may include forming an anode active material layer (CML) on a first solid electrolyte layer (SEL1).

[0156] In one embodiment, forming a positive active material layer (CML) on a first solid electrolyte layer (SEL1) may include directly coating a positive active material slurry on the first solid electrolyte layer (SEL1). By doing so, the interfacial resistance between the positive active material layer (CML) and the first solid electrolyte layer (SEL1) can be improved.

[0157] In another embodiment, forming an anode active material layer (CML) on a first solid electrolyte layer (SEL1) may include forming an anode active material layer (CML) by coating an anode active material slurry on a second peeling substrate; and transferring the anode active material layer (CML) on the second peeling substrate onto the first solid electrolyte layer (SEL1). The anode active material layer (CML) coated on the second peeling substrate may be laminated onto the first solid electrolyte layer (SEL1); laminating; and removing the second peeling substrate (PES2) to transfer the anode active material layer (CML) on the second peeling substrate onto the first solid electrolyte layer (SEL1).

[0158] The positive active material layer (CML) may correspond to the positive active material layer (120) described above with reference to FIG. 1. As an example, the positive active material layer (CML) may include the positive active material and solid electrolyte described above with reference to FIG. 1. The positive active material layer (CML) may include a binder and a conductive material.

[0159] In one embodiment, the material of the second peeling substrate may include at least one of the materials of the first peeling substrate (PES1) described above. For example, the material of the second peeling substrate may be the same as the material of the first peeling substrate.

[0160]

[0161] FIG. 10b are cross-sectional views illustrating slitting one side of a first transfer member.

[0162] Referring to FIG. 9 and FIG. 10b, one side of the first transfer member (TRM1) can be slit.

[0163] In one embodiment, one side of the first transfer member (TRM1) can be slit at an angle within ±5° relative to the vertical direction from the upper surface to the lower surface of the first transfer member (TRM1). The angle within ±5° means an angle rotated within 5° in a clockwise or counterclockwise direction relative to the vertical direction from the upper surface to the lower surface of the first transfer member (TRM1). For example, the first transfer member (TRM1) can be slit in the vertical direction (CD1) from the upper surface to the lower surface of the first transfer member (TRM1). Alternatively, it can be slit along a direction (CD2) rotated within 5° in a counterclockwise direction or a direction (CD3) rotated within 5° in a clockwise direction relative to the vertical direction from the upper surface to the lower surface of the first transfer member (TRM1).

[0164] If the angle range is exceeded, the asymmetry between the positive active material layer (CML) and the first solid electrolyte layer (SEL1) increases, resulting in reduced structural stability and reduced space efficiency during subsequent packaging. In particular, when slitting is performed at an angle of 5° or more counterclockwise with respect to the third direction (D3), the inclined surface formed at the end of the positive active material layer (CML) may act as a cause of short circuit as described above with reference to FIG. 8b.

[0165] FIG. 10c is a cross-sectional view illustrating a side formed after slitting one side of a first transfer member (TRM1). Referring to FIG. 10b, through slitting, one side of each of the first peeling substrate (PES1), the first solid electrolyte layer (SEL1), and the positive active material layer (CML) can be integrally cut and aligned with each other. That is, a single continuous cut surface can be formed.

[0166] FIGS. 10d to 10h are plan or cross-sectional views for explaining a process of transferring a first transfer layer of a first transfer member onto an anode substrate. FIG. 10d is a plan view for explaining the first transfer member laminated onto an anode substrate. FIG. 10e is a cross-sectional view along line A-A' of FIG. 10d. FIG. 10f is a cross-sectional view along line B-B' of FIG. 10d.

[0167] Referring to FIG. 9 and FIG. 10c, a first transfer layer (TRL1) on a first peeling substrate (PES1) can be transferred onto an anode substrate (CUS). In other words, a first transfer layer (TRL1) can be transferred from a first transfer member (TRM1) onto an anode substrate (CUS). Specifically, a first solid electrolyte layer (SEL1) and an anode active material layer (CML) can be transferred onto an anode substrate (CSU).

[0168] In one embodiment, the positive substrate (CUS) may include the positive current collector (110) described above with reference to FIG. 1.

[0169] In one embodiment, the positive substrate (CUS) may further include a carbon layer on the positive current collector (110).

[0170] In one embodiment, as described below with reference to FIG. 13a, the anode substrate (CUS) may include a first tab portion protruding in a first direction (D1). The first tab portion (TAB1) may be an anode tab.

[0171] In one embodiment, with reference to FIGS. 9, 10d to 10f, transferring a first solid electrolyte layer (SEL1) and a positive active material layer (CML) from a first transfer member (TRM1) onto a positive substrate (CSU) may include inverting the first transfer member (TRM1) and stacking it onto the positive substrate (CSU); and removing a first peeling substrate (PES1). By inverting the first transfer member (TRM1) and stacking it onto the positive substrate (CSU), the positive active material layer (CML) can be stacked adjacent to the positive substrate (CSU). As a result, the first peeling substrate (PES1) can be located on the top surface.

[0172] FIG. 10g is a cross-sectional view illustrating the removal of the first peeling substrate (PES1).

[0173] Referring to FIG. 10g, in one embodiment, the first peelable substrate (PES1) can be removed. The method of removing the first peelable substrate (PES1) is not particularly limited. For example, one end of the first peelable substrate (PES1) can be pulled to peel it off. Alternatively, the first peelable substrate (PES1) can be removed using a separate peeling device. By removing the first peelable substrate (PES1), a first electrode can be prepared in which an anode substrate (CSU); an anode electrolyte layer (CML) and a first solid electrolyte layer (SEL1) are sequentially stacked.

[0174] FIG. 10h is a cross-sectional view illustrating slitting the other side of the first electrode.

[0175] Referring to FIG. 9 and FIG. 10h, the other side of the first electrode can be slit. Specifically, the other side of the first transfer layer (TRL1) can be slit integrally with the anode substrate (CSU). Through the slitting, stacking errors between the anode substrate (CSU), the anode active material layer (CML), and the first solid electrolyte layer (SEL1) that may occur during the transfer process (S300) can be eliminated.

[0176] In one embodiment, the method for manufacturing an all-solid-state battery (S10) may further include forming a negative electrode coating layer on a negative electrode substrate; and forming a second solid electrolyte layer on the negative electrode coating layer to prepare a second electrode.

[0177] In one embodiment, the cathode substrate and the cathode coating layer, respectively, may be identical to the cathode current collector (210) and the cathode coating layer (220) described above with reference to FIG. 1. The second solid electrolyte layer may be identical to the second solid electrolyte layer (320) described above with reference to FIG. 1.

[0178] In one embodiment, the method for manufacturing an all-solid-state battery (S10) may include laminating a first electrode and a second electrode. Specifically, the first solid electrolyte layer (SEL1) of the first electrode and the second solid electrolyte layer of the second electrode may be arranged adjacently, and then the first electrode and the second electrode may be laminated.

[0179]

[0180] In the embodiments of the present invention described below, detailed descriptions of technical features that overlap with the manufacturing method of the all-solid-state battery described above are omitted, and differences are described in detail.

[0181] FIG. 11 is a flowchart illustrating a method for manufacturing an all-solid-state battery according to another embodiment of the present invention. FIG. 12a to 12h are cross-sectional views illustrating the method for manufacturing the all-solid-state battery.

[0182] Referring to FIG. 11, a method (S10a) for manufacturing an all-solid-state battery according to one embodiment of the present invention may include manufacturing a first electrode. Specifically, manufacturing the first electrode comprises:

[0183] The method may include preparing a first transfer member by forming a first transfer layer on a first peelable substrate (S100a); preparing a second transfer member by forming a second transfer layer on a second peelable substrate (S100b); slitting one side of the first transfer member (S200a); slitting one side of the second transfer member (S200b); transferring the first transfer layer on the first peelable substrate onto an anode substrate (S300a); transferring the second transfer layer on the second peelable substrate onto the first transfer layer (S300b); and slitting the other side of the first transfer layer and the second transfer layer integrally with the anode substrate (S400a).

[0184] FIG. 12a is a cross-sectional view for explaining preparing a first transfer member by forming a first transfer layer on a first release substrate (S100a); and preparing a second transfer member by forming a second transfer layer on a second release substrate (S100b).

[0185] Referring to FIGS. 11 and FIG. 12a, a first transfer layer (TRL1) can be formed on a first peelable substrate (PES1). A second transfer layer (TRL2) can be formed on a second peelable substrate (PES2).

[0186] Each of the first and second peeling substrates (PES1, PES2) may be identical to the first peeling substrate described above with reference to FIG. 9.

[0187] Forming a first transfer layer (TRL1) on a first peeling substrate (PES1) may include forming an anode active material layer (CML) on the first peeling substrate (PES1). In one embodiment, forming an anode active material layer (CML) on the first peeling substrate (PES1) may include directly coating an anode active material slurry on the first peeling substrate (PES1).

[0188] Forming a second transfer layer (TRL2) on a second peeling substrate (PES1) may include forming a first solid electrolyte layer (SEL1) on a second peeling substrate (PES2). In one embodiment, forming the first solid electrolyte layer (SEL1) on the second peeling substrate (PES2) may include directly coating a solid electrolyte slurry on the second peeling substrate (PES2).

[0189] FIGS. 12b and FIGS. 12c are cross-sectional views illustrating slitting one side of a first transfer member (TRM1) (S200a); and slitting one side of a second transfer member (TRM2) (S200b).

[0190] Referring to FIG. 10 and FIG. 12b, in one embodiment, one side of the first transfer member (TRM1) can be slit at an angle within ±5° with respect to the vertical direction from the upper surface to the lower surface of the first transfer member (TRM1). One side of the second transfer member (TRM2) can be slit at an angle within ±5° with respect to the vertical direction from the upper surface to the lower surface of the second transfer member (TRM2). Through this, one side can be slit as shown in FIG. 12c.

[0191] FIGS. 12d to 12g are cross-sectional views for explaining transferring a first transfer layer (TRL1) on a first peeling substrate (PES1) onto an anode substrate (CSU) (S300a); and transferring a second transfer layer (TRL1) on a second peeling substrate (PES2) onto the first transfer layer (TRL1) (S300b).

[0192] Referring to FIGS. 11 and FIGS. 12d to 12e, a first transfer layer (TRL1) on a first peeling substrate (PES1) can be transferred onto an anode substrate (CUS). In other words, a first transfer layer (TRL1) can be transferred from a first transfer member (TRM1) onto an anode substrate (CUS). Specifically, an anode active material layer (CML) can be transferred onto an anode substrate (CSU).

[0193] In one embodiment, the positive substrate (CUS) may include the positive current collector (110) described above with reference to FIG. 1.

[0194] In one embodiment, the positive substrate (CUS) may further include a carbon layer on the positive current collector (110).

[0195] In one embodiment, the anode substrate (CUS) may include a first tab portion protruding in a first direction (D1).

[0196] In one embodiment, transferring the positive active material layer (CML) from the first transfer member (TRM1) onto the positive substrate (CSU) may include inverting the first transfer member (TRM1) and stacking it onto the positive substrate (CSU); and removing the first peeling substrate (PES1). By inverting the first transfer member (TRM1) and stacking it onto the positive substrate (CSU), the positive active material layer (CML) can be stacked adjacent to the positive substrate (CSU). As a result, the first peeling substrate (PES1) can be located on the top surface.

[0197] Referring to FIG. 12e, the first peelable substrate (PES1) can be removed. The method of removing the first peelable substrate (PES1) is not particularly limited. For example, the first peelable substrate (PES1) can be removed by the method described above with reference to FIG. 10g.

[0198] Referring to FIG. 9, FIG. 12f, and FIG. 12g, a second transfer layer (TRL2) on a second peeling substrate (PES2) can be transferred onto a first transfer layer (TRL1). In other words, a second transfer layer (TRL2) from a second transfer member (TRM2) can be transferred onto a first transfer layer (TRL1). Specifically, a first solid electrolyte layer (SEL1) of a second transfer member (TRM2) can be transferred onto an anode active material layer (CML).

[0199] In one embodiment, transferring the positive active material layer (CML) from the first transfer member (TRM1) onto the positive substrate (CSU) may include inverting the first transfer member (TRM1) and stacking it onto the positive substrate (CSU); and removing the first peeling substrate (PES1). By inverting the first transfer member (TRM1) and stacking it onto the positive substrate (CSU), the positive active material layer (CML) can be stacked adjacent to the positive substrate (CSU). As a result, the first peeling substrate (PES1) can be located on the top surface.

[0200] Referring to FIG. 12g, the second peelable substrate (PES2) can be removed. The method of removing the second peelable substrate (PES2) is not particularly limited. For example, the second peelable substrate (PES2) can be removed by the method described above with reference to FIG. 10g.

[0201] FIG. 12h is a cross-sectional view illustrating slitting the other side of the first electrode.

[0202] Referring to FIG. 11 and FIG. 12h, other sides of the first electrode can be slit. Specifically, other sides of the first transfer layer (TRL1) and the second transfer layer (TRL2) can be slit integrally with the anode substrate (CSU). In one embodiment, other sides of the anode substrate (CSU), other sides of the anode active material layer (CML), and other sides of the first solid electrolyte layer (SEL1) can be slit integrally.

[0203] Through the above slitting, stacking errors between the anode substrate (CSU), the anode active material layer (CML), and the first solid electrolyte layer (SEL1) that may occur during the transfer process (S300) can be eliminated.

[0204] In one embodiment, the method for manufacturing an all-solid-state battery (S10a) may further include forming a negative electrode coating layer on a negative electrode substrate; and forming a second solid electrolyte layer on the negative electrode coating layer to prepare a second electrode.

[0205] In one embodiment, the cathode substrate and the cathode coating layer, respectively, may be identical to the cathode current collector (210) and the cathode coating layer (220) described above with reference to FIG. 1. The second solid electrolyte layer may be identical to the second solid electrolyte layer (320) described above with reference to FIG. 1.

[0206] In one embodiment, the method for manufacturing an all-solid-state battery (S10a) may include laminating a first electrode and a second electrode. Specifically, the first solid electrolyte layer (SEL1) of the first electrode and the second solid electrolyte layer of the second electrode may be arranged adjacently, and then the first electrode and the second electrode may be laminated.

[0207]

[0208] Hereinafter, a positive electrode of an all-solid-state battery manufactured by a manufacturing method according to embodiments of the present invention will be described in detail.

[0209] FIG. 13a is a plan view illustrating the first electrode of an all-solid-state battery manufactured by the manufacturing method (S10) described above with reference to FIG. 9. FIG. 13b is a cross-sectional view along the line A-A' of FIG. 13a. FIG. 13c is a cross-sectional view along the line B-B' of FIG. 13a.

[0210] Referring to FIGS. 13a to 13c, the first electrode (ELT1) may include a positive electrode substrate (CSU), a positive electrode active material layer (CML) on the positive electrode substrate (CSU), and a first solid electrolyte layer (SEL1) on the positive electrode active material layer (CML). The positive electrode substrate (CSU) and the positive electrode active material layer (CML) on the positive electrode substrate (CSU) may constitute the positive electrode layer (100) of the all-solid-state battery described above with reference to FIG. 1.

[0211] In one embodiment, the positive substrate (CUS) may include the positive current collector (110) described above with reference to FIG. 1.

[0212] In one embodiment, the positive substrate (CUS) may further include a carbon layer on the positive current collector (110). The carbon layer can improve the bonding strength between the positive current collector and the positive active material layer, as described above with reference to FIG. 1.

[0213] In one embodiment, the anode substrate (CSU) may include a first tab portion (TAB1) protruding in a first direction (D1).

[0214] Referring to FIG. 13b, in one embodiment, the positive active material layer (CML) may include a first side (SID1) adjacent to a first tab portion (TAB1). The first solid electrolyte layer (SEL1) may include a second side (SID2) adjacent to the first tab portion (TAB1). The positive substrate (CSU) may include a third side (SID3) adjacent to the first side (SID1). The first to third sides (SID1-SID3) may be adjacent to each other.

[0215] In one embodiment, the first side (SID1) and the second side (SID2) can be aligned with each other. As described above with reference to FIG. 9, the first side (SID1) and the second side (SID2) can be aligned with each other by slitting one side of the positive active material layer (CML) and the first solid electrolyte layer (SEL1) together. On the other hand, since one side of the positive substrate (CSU) is not slit together with the positive active material layer (CML), the first side (SID1) and the third side (SID3) may not be aligned.

[0216] Referring to FIG. 13b, in one embodiment, the positive active material layer (CML) may have a first inclination angle (θ1) which is the angle formed between the first side (SID1) and the lower surface of the first electrode (ELT1). The first solid electrolyte layer (SEL1) may have a second inclination angle (θ2) which is the angle formed between the second side (SID2) and the lower surface of the first electrode (ELT1). The positive substrate (CSU) may have a third inclination angle (θ3) which is the angle formed between the third side (SID3) and the lower surface of the first electrode (ELT1). For example, the lower surface of the first electrode (ELT1) may be the lower surface of the positive substrate (CSU).

[0217] In one embodiment, the difference between the first inclination angle (θ1) and the second inclination angle (θ2) may be 3° or less or 1° or less. For example, the first inclination angle (θ1) and the second inclination angle (θ2) may be substantially the same.

[0218] In one embodiment, the first side (SID1) and the second side (SID2) of the anode active material layer (CML) formed by slitting may each have an angle close to a right angle. Specifically, the first inclination angle (θ1) and the second inclination angle (θ2) may each be greater than 85° and less than 90°, or greater than 90° and less than 95°.

[0219] Referring to FIG. 13b, in one embodiment, the positive active material layer (CML) may include a fourth side (SID4) spaced apart from a first side (SID1) in a first direction (D1). The first solid electrolyte layer (SEL1) may include a fifth side (SID5) spaced apart from a second side (SID2) in a first direction (D1). The positive substrate (CSU) may include a sixth side (SID6) spaced apart from a fourth side (SID4) in a first direction (D1). The fourth to sixth sides (SID4-SID6) may be adjacent to each other.

[0220] In one embodiment, the fourth to sixth sides (SID4-SID6) may be aligned with each other. As described above with reference to FIG. 9, the sixth side (SID6) may be formed by slitting together the positive substrate (CSU), the positive active material layer (CML), and the first solid electrolyte layer (SEL1). As a result, unlike the fourth side (SID4), the sixth side (SID6) may be aligned with the fourth and fifth sides (SID4, SID5).

[0221] Referring to FIG. 13b, in one embodiment, the positive active material layer (CML) may have a fourth inclination angle (θ4), which is the angle formed between the fourth side (SID4) and the lower surface of the first electrode (ELT1). The first solid electrolyte layer (SEL1) may have a fifth inclination angle (θ5), which is the angle formed between the fifth side (SID5) and the lower surface of the first electrode (ELT1). The positive substrate (CSU) may have a sixth inclination angle (θ6), which is the angle formed between the sixth side (SID6) and the lower surface of the first electrode (ELT1). For example, the lower surface of the first electrode (ELT1) may be the lower surface of the positive substrate (CSU).

[0222] In one embodiment, the difference between the fourth angle of inclination (θ4) and the fifth angle of inclination (θ5) may be 3° or less or 1° or less. For example, the fourth angle of inclination (θ4) and the fifth angle of inclination (θ5) may be substantially the same.

[0223] In one embodiment, the difference between the fourth angle of inclination (θ4) and the sixth angle of inclination (θ6) may be 3° or less or 1° or less. For example, the fourth angle of inclination (θ4) and the sixth angle of inclination (θ6) may be substantially the same.

[0224] The first electrode may include an anode substrate (CSU), an anode active material layer (CML) on the anode substrate (CSU), and a first solid electrolyte layer (SEL1) on the anode active material layer (CML).

[0225] The positive substrate (CSU) may include the positive current collector (110) described above with reference to FIG. 1, the positive active material layer (CML) may include the positive active material layer (120) described above with reference to FIG. 1, and the first solid electrolyte layer (SEL1) may include the first solid electrolyte layer (310) described above with reference to FIG. 1.

[0226] A solid-state battery according to embodiments of the present invention may further include a second solid electrolyte layer on a first solid electrolyte layer (SEL1) and a negative electrode layer on the second solid electrolyte layer. The second solid electrolyte layer may include the second solid electrolyte layer (320) described above with reference to FIG. 1, and the negative electrode layer may include the negative electrode layer (200) described above with reference to FIG. 1.

[0227]

[0228] FIG. 14a is a plan view illustrating the first electrode of an all-solid-state battery manufactured by the manufacturing method (S10a) described above with reference to FIG. 11. FIG. 14b is a cross-sectional view along the line A-A' of FIG. 14a. FIG. 14c to 14e are examples of partial modifications to the first electrode of FIG. 14a. Detailed descriptions of technical features that overlap with those previously described with reference to FIG. 13a to 13c are omitted, and the differences are described in detail.

[0229] Referring to FIGS. 14a and 14b, as described above with reference to FIGS. 12a through 12h, the first electrode can be manufactured by individually slitting one side of a first transfer member (TRM1) containing a positive active material layer (CML) and one side of a second transfer member (TRM2) containing a first solid electrolyte layer (SEL1), and then sequentially transferring them onto a positive substrate (CSU). As a result, the first side (SID1) of the positive active material layer (CML) and the second side (SID2) of the first solid electrolyte layer (SEL1) may not be aligned with each other. The first side (SID1) and the second side (SID2) may be offset from each other.

[0230] Referring to FIG. 14b and FIG. 14e, in one embodiment, the difference between the first inclination angle (θ1) and the second inclination angle (θ2) may be greater than 3°. For example, the difference between the first inclination angle (θ1) and the second inclination angle (θ2) may be greater than 3° and equal to or less than 20°. Alternatively, the difference between the first inclination angle (θ1) and the second inclination angle (θ2) may be greater than 3° and equal to or less than 10°.

[0231] In one embodiment, the first inclination angle (θ1) and the second inclination angle (θ2) may each be greater than 85° and less than 90°, or greater than 90° and less than 95°. Specifically, referring to FIG. 14b, the first inclination angle (θ1) may be greater than 85° and less than 90°, and the second inclination angle (θ2) may be greater than 90° and less than 95°. Referring to FIG. 14c, the first inclination angle (θ1) and the second inclination angle (θ2) may each be greater than 85° and less than 90°. Referring to FIG. 14d, the first inclination angle (θ1) may be greater than 90° and less than 95°, and the second inclination angle (θ2) may be greater than 85° and less than 90°. Referring to FIG. 14e, the first inclination angle (θ1) and the second inclination angle (θ2) may each be greater than 90° and less than 95°.

[0232]

[0233] Additionally, since one side of the first and second transfer members (TRM1, TRM2) is slit and then transferred onto the anode substrate (CSU), one side (COS) of the anode active material layer (CML) and one side (SOS) of the anode substrate (CSU) may not be aligned at the same angle. In one embodiment, the difference between the first inclination angle (θ1) and the second inclination angle (θ2) may be greater than 3° or 5°. For example, the difference between the first inclination angle (θ1) and the third inclination angle (θ3) may be greater than 3° and equal to or less than 20°. Alternatively, the difference between the first inclination angle (θ1) and the third inclination angle (θ3) may be greater than 5° and equal to or less than 10°.

[0234] On the other hand, as described above with reference to FIG. 13b, after transferring the positive active material layer (CML) and the first solid electrolyte layer (SEL1) onto the positive substrate (CSU), the other side of the first electrode is slit, so the 4th to 6th sides (SID4-SID6) can be aligned with each other.

[0235] In one embodiment, the difference between the fourth angle of inclination (θ4) and the fifth angle of inclination (θ5) may be less than 3° or less than 1°. For example, the fourth angle of inclination (θ4) and the fifth angle of inclination (θ5) may be substantially the same.

[0236] In one embodiment, the fourth inclination angle (θ4) and the sixth inclination angle (θ6) may be less than 3° or less than 1°. For example, the fourth inclination angle (θ4) and the sixth inclination angle (θ6) may be substantially the same.

[0237] In one embodiment, as shown in FIG. 14b and FIG. 14c, the first solid electrolyte layer (SEL1) may protrude further in a first direction (D1) than the positive active material layer (CML). This prevents a short circuit. In another embodiment, although not illustrated, the positive active material layer (CML) may protrude further in a first direction (D1) than the first solid electrolyte layer (SEL1).

[0238]

[0239] FIG. 15 is a flowchart for explaining a method for manufacturing an all-solid-state battery according to another embodiment of the present invention.

[0240] Referring to FIG. 15, a method (S10) for manufacturing an all-solid-state battery according to one embodiment of the present invention may include preparing a first electrode. Specifically, preparing the first electrode may include: preparing a first transfer member by forming a first transfer layer on a first release substrate (S100); preparing a second transfer member by forming a second transfer layer on a second release substrate (S200); forming a laminate by bonding the first transfer member and the second transfer member (S300); integrally slitting a first side of the first transfer member and a second side of the second transfer member (S400); removing the first release substrate and transferring the laminate onto an anode substrate (S500); integrally slitting the other side of each of the second transfer member and the first transfer layer with the anode substrate (S600); and removing the second release substrate from the second transfer layer (S700).

[0241] FIGS. 16a to 16g are cross-sectional views illustrating the formation of a first electrode comprising a plurality of positive active material layers.

[0242] Referring to FIGS. 15 and FIG. 16a, in one embodiment, a first transfer layer (TRL1) can be formed on a first release substrate (PES1). Through this, a first transfer member can be prepared. In one embodiment, a second transfer layer (TRL2) can be formed on a second release substrate (PES2). Through this, a second transfer member can be prepared.

[0243] In one embodiment, the first transfer layer (TRL1) may include the aforementioned first positive active material layer (120_1). The second transfer layer (TRL2) may include the aforementioned second positive active material layer (120_2).

[0244] The material of the first peeling substrate (PES1) is not particularly limited, and a material that can be easily peeled off during a transfer process may be used. In one embodiment, the first peeling substrate (PES1) may have a single-layer or multi-layer structure. In one embodiment, the first peeling substrate (PES1) may include a polymer film or a metal film. For example, the first peeling substrate (PES1) may include at least one of a polyethylene terephthalate (PET) film, a polycarbonate (PC) film, a polyurethane (PU) film, and a polyvinyl alcohol (PVA) film. For example, the first peeling substrate (PES1) may include 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.

[0245] In one embodiment, the material of the first peeling substrate (PES1) may be the same as the material of the anode current collector (110) described above with reference to FIG. 1. As an example, the first peeling substrate (PES1) may be aluminum foil.

[0246] Forming a first transfer layer (TRL1) on a first peeling substrate (PES1) (S100) may involve forming an anode active material layer on the first peeling substrate (PES1), and specifically, may include directly coating an anode active material slurry on the first peeling substrate (PES1).

[0247] The above positive active material layer may correspond to the first positive active material layer (120_1) described above with reference to FIG. 7b. As an example, the above positive active material layer may include the positive active material and solid electrolyte described above with reference to FIG. 1. The above positive active material layer may include a binder and a conductive material.

[0248] In one embodiment, the material of the second peeling substrate (PES2) may include at least one of the materials of the first peeling substrate (PES1) described above. For example, the material of the second peeling substrate may be the same as the material of the first peeling substrate.

[0249] Forming a second transfer layer (TRL2) on a second peeling substrate (PES2) (S200) may involve forming an anode active material layer on the second peeling substrate (PES2), and specifically, may include directly coating an anode active material slurry on the second peeling substrate (PES2).

[0250] The above positive active material layer may correspond to the second positive active material layer (120_2) described above with reference to FIG. 7b. As an example, the above positive active material layer may include the positive active material and solid electrolyte described above with reference to FIG. 1. The above positive active material layer may include a binder and a conductive material.

[0251] Referring to FIG. 15 and FIG. 16b, in one embodiment, forming a laminate by joining the first transfer member and the second transfer member (S300) may include: inverting the second transfer member to laminate a second transfer layer (TRL2) on the first transfer layer (TRL1); and joining the first transfer layer (TRL1) and the second transfer layer (TRL2). After joining the first transfer layer (TRL1) and the second transfer layer (TRL2), the first release substrate (PES1) and the second release substrate (PES2) may be spaced apart in a third direction (D3) with the first and second transfer layers (TRL1, TRL2) in between.

[0252] Referring to FIGS. 15, FIGS. 16c, and FIGS. 16d, the first side of the first transfer member and the second side of the second transfer member can be slit integrally. In one embodiment, the first side of the first transfer member and the second side of the second transfer member can be slit at an angle within ±5° with respect to the vertical direction from the upper surface to the lower surface of the first transfer member. Specifically, the second side of the second release substrate (PES2), the second side of the second transfer layer (TRL2), the first side of the first transfer layer (TRL1), and the first side of the first release substrate (PES1) can be slit integrally at an angle within ±5°.

[0253] The above angle within ±5° means an angle rotated within 5° in a clockwise or counterclockwise direction relative to the vertical direction from the upper surface to the lower surface of the first transfer member. For example, the first transfer member and the second transfer member can be slit in the vertical direction (CD1) from the upper surface to the lower surface of the first transfer member. Alternatively, they can be slit along a direction rotated within 5° in a counterclockwise direction (CD2) or a direction rotated within 5° in a clockwise direction (CD3) relative to the vertical direction from the upper surface to the lower surface of the first transfer member.

[0254] If the angle range is exceeded, the asymmetry between the first transfer layer (TRL1) and the second transfer layer (TRL2) increases, resulting in reduced structural stability and reduced space efficiency during subsequent packaging. In particular, when slitting is performed at an angle of 5° or more in a counterclockwise direction relative to the third direction (D3), the inclined surface formed at the end of the first and second transfer layers (TRL1, TRL2) may act as a cause of short circuits as described above with reference to FIG. 8b.

[0255] FIG. 16d is a cross-sectional view illustrating a side formed after integrally slitting the first side of the first transfer member and the second side of the second transfer member. Referring to FIG. 16d, through slitting, one side of each of the second release substrate (PES2), the second transfer layer (TRL2), the first transfer layer (TRL1), and the first release substrate (PES1) can be integrally cut and aligned with each other. That is, a single continuous cut surface can be formed.

[0256] Referring to FIGS. 15 and FIGS. 16e, in one embodiment, removing the first peeling substrate and transferring the laminate onto the anode substrate (S500) may involve removing the first peeling substrate (PES1) and then transferring the first transfer layer (TRL1) of the laminate onto the anode substrate (CSU). That is, the first transfer layer (TRL1), the second transfer layer (TRL2), and the second peeling substrate (PES2) may be transferred onto the anode substrate (CSU). As a result, the second peeling substrate (PES2) may be located on the top surface.

[0257] In one embodiment, the positive substrate (CSU) may be the same as the material of the positive current collector (110) described above with reference to FIG. 1. As an example, the positive substrate (CSU) may further include a carbon layer on the positive current collector (110).

[0258] In one embodiment, as described below with reference to FIG. 17a, the anode substrate (CSU) may include a first tab portion protruding in a first direction (D1). The first tab portion may be an anode tab, and the first tab portion may correspond to the aforementioned tab portion (ATP).

[0259] Referring to FIGS. 15 and FIGS. 16f, the other side of each of the second transfer member and the first transfer layer can be slit integrally with the anode substrate. In one embodiment, the other side of each of the second transfer member and the first transfer layer can be slit at an angle within ±5° with respect to the vertical direction from the upper surface to the lower surface of the anode substrate. Specifically, the other side of each of the second release substrate (PES2), the second transfer layer (TRL2), the first transfer layer (TRL1), and the anode substrate (CSU) can be slit integrally at an angle within ±5°.

[0260] The above angle within ±5° means an angle rotated within 5° in a clockwise or counterclockwise direction relative to the vertical direction from the upper surface to the lower surface of the first transfer member. For example, the first transfer member and the second transfer member can be slit in the vertical direction (CD1) from the upper surface to the lower surface of the first transfer member. Alternatively, they can be slit along a direction rotated within 5° in a counterclockwise direction (CD2) or a direction rotated within 5° in a clockwise direction (CD3) relative to the vertical direction from the upper surface to the lower surface of the first transfer member.

[0261] If the angle range is exceeded, the asymmetry between the first transfer layer (TRL1) and the second transfer layer (TRL2) increases, resulting in reduced structural stability and reduced space efficiency during subsequent packaging. In particular, when slitting is performed at an angle of 5° or more in a counterclockwise direction relative to the third direction (D3), the inclined surface formed at the other end of the first and second transfer layers (TRL1, TRL2) may act as a cause of short circuits as described above with reference to FIG. 8b.

[0262] Referring to FIG. 15 and FIG. 16g, after slitting the other side of each of the second transfer member and the first transfer layer together with the anode substrate, the second peeling substrate can be removed from the second transfer layer. Through slitting, the other sides of each of the second transfer layer (TRL2), the first transfer layer (TRL1), and the anode substrate (CSU) can be cut together and aligned with each other. That is, a single continuous cut surface can be formed.

[0263] Referring to FIGS. 15 and FIGS. 16a to 16g, according to a method for manufacturing an all-solid-state battery according to one embodiment of the present invention, a first electrode comprising a plurality of positive active material layers can be prepared.

[0264]

[0265] Hereinafter, a positive electrode of an all-solid-state battery manufactured by a manufacturing method according to embodiments of the present invention will be described in detail.

[0266] FIG. 17a is a plan view illustrating the first electrode of an all-solid-state battery manufactured by the manufacturing method (S10) described above with reference to FIG. 15. FIG. 17b is a cross-sectional view along the line A-A' of FIG. 17a. FIG. 17c is a cross-sectional view along the line B-B' of FIG. 17a.

[0267] Referring to FIGS. 17a to 17c, the first electrode (ELT1) may include a positive electrode substrate or a positive electrode current collector (110), a first positive electrode active material layer (120_1) on the positive electrode current collector (110), and a second positive electrode active material layer (120_2) on the first positive electrode active material layer (120_1). The positive electrode current collector (110) and the first and second positive electrode active material layers (120_1, 120_2) on the positive electrode current collector (110) may constitute the positive electrode layer (100) of the all-solid-state battery described above with reference to FIG. 1.

[0268] In one embodiment, the positive current collector (110) may further include a carbon layer. The carbon layer can improve the bonding strength between the positive current collector (110) and the positive active material layer, as described above with reference to FIG. 1.

[0269] In one embodiment, the positive current collector (110) may include a tab portion (ATP) protruding in a first direction (D1).

[0270] Referring to FIG. 17b, in one embodiment, the first positive active material layer (120_1) may include a first side (SID1) adjacent to the tab portion (ATP). The second positive active material layer (120_2) may include a second side (SID2) adjacent to the tab portion (ATP). In one embodiment, the first side (SID1) and the second side (SID2) may be aligned with each other. As described above with reference to FIG. 15, the first side (SID1) and the second side (SID2) may be aligned with each other by slitting one side of the first positive active material layer (120_1) and the second positive active material layer (120_2) together.

[0271] Referring to FIG. 17b, in one embodiment, the first positive active material layer (120_1) may have a first inclination angle (θ1) which is the angle formed between the first side (SID1) and the lower surface of the first electrode (ELT1). The second positive active material layer (120_2) may have a second inclination angle (θ2) which is the angle formed between the second side (SID2) and the lower surface of the first electrode (ELT1). For example, the lower surface of the first electrode (ELT1) may be the lower surface of the positive current collector (110).

[0272] In one embodiment, the difference between the first inclination angle (θ1) and the second inclination angle (θ2) may be 3° or less or 1° or less. For example, the first inclination angle (θ1) and the second inclination angle (θ2) may be substantially the same.

[0273] In one embodiment, the first side (SID1) of the first positive active material layer (120_1) formed by slitting and the second side (SID2) of the second positive active material layer (120_2) may each have an angle close to a right angle. Specifically, the first inclination angle (θ1) and the second inclination angle (θ2) may each be greater than 85° and less than 90°, or greater than 90° and less than 95°.

[0274] Referring again to FIG. 17b, in one embodiment, the first positive active material layer (120_1) may include a third side (SID3) spaced apart from the first side (SID1) in the first direction (D1). The second positive active material layer (120_2) may include a fourth side (SID4) spaced apart from the second side (SID2) in the first direction (D1). The positive current collector (110) may include a fifth side (SID5) adjacent to the third side (SID3). The third to fifth sides (SID3-SID5) may be adjacent to each other.

[0275] In one embodiment, the third side (SID3), the fourth side (SID4), and the fifth side (SID5) can be aligned with each other. As described above with reference to FIG. 15, the third side (SID3) to the fifth side (SID5) can be aligned with each other by slitting together the other side of the first positive active material layer (120_1) and the second positive active material layer (120_2) and the other side of the positive current collector (110).

[0276] The positive current collector (110) may include a sixth side (SID6) adjacent to the first side (SID1) and opposite to the fifth side (SID5). The first side (SID1), the second side (SID2), and the sixth side (SID6) may be adjacent to each other. On the other hand, since the sixth side (SID6) of the positive current collector (100) is not slit together with the first and second positive active material layers (120_1, 120_2), the sixth side (SID6) may not be aligned with the first and second sides (SID1, SID2).

[0277] Referring again to FIG. 17b, in one embodiment, the first positive active material layer (120_1) may have a third inclination angle (θ3), which is the angle formed between the third side (SID3) and the lower surface of the first electrode (ELT1). The second positive active material layer (120_2) may have a fourth inclination angle (θ4), which is the angle formed between the fourth side (SID4) and the lower surface of the first electrode (ELT1). The positive current collector (110) may have a fifth inclination angle (θ5), which is the angle formed between the fifth side (SID5) and the lower surface of the first electrode (ELT1). For example, the lower surface of the first electrode (ELT1) may be the lower surface of the positive current collector (110).

[0278] In one embodiment, the difference between the third inclination angle (θ3) and the fourth inclination angle (θ4), and the difference between the third inclination angle (θ3) and the fifth inclination angle (θ5) may be 3° or less or 1° or less. For example, the third inclination angle (θ3), the fourth inclination angle (θ4), and the fifth inclination angle (θ5) may be substantially the same.

[0279] The first electrode may include a positive current collector (110), a first positive active material layer (120_1) on the positive current collector (110), and a second positive active material layer (120_2) on the first positive active material layer (120_1).

[0280] A solid-state battery according to embodiments of the present invention may further include a solid electrolyte layer on a second positive active material layer and a negative electrode layer on the solid electrolyte layer. The solid electrolyte layer may include the solid electrolyte layer (300) described above with reference to FIG. 1, and the negative electrode layer may include the negative electrode layer (200) described above with reference to FIG. 1.

[0281]

[0282] FIGS. 18a to 18c are cross-sectional views illustrating a first electrode of an all-solid-state battery manufactured by the manufacturing method (S10) described above with reference to FIG. 15, and FIGS. 18a to 18c are examples of partial modifications of the first electrode of FIG. 17b. Detailed descriptions of technical features that overlap with those previously described with reference to FIGS. 17a to 17c are omitted, and the differences are described in detail.

[0283] Referring to FIG. 18a, in one embodiment, the first inclination angle (θ1) and the second inclination angle (θ2) may each be obtuse, and the third inclination angle (θ3), the fourth inclination angle (θ4), and the fifth inclination angle (θ5) may each be acute. For example, the first inclination angle (θ1) and the second inclination angle (θ2) may each be greater than 90° and less than 95°, and the third inclination angle (θ3), the fourth inclination angle (θ4), and the fifth inclination angle (θ5) may each be greater than 85° and less than 90°. The first side (SID1) and the second side (SID2) may be aligned with each other, and the third side (SID3), the fourth side (SID4), and the fifth side (SID5) may be aligned with each other.

[0284] Referring to FIG. 18b, in one embodiment, the first angle of inclination (θ1) may be acute and the second angle of inclination (θ2) may be obtuse. The third angle of inclination (θ3), the fourth angle of inclination (θ4), and the fifth angle of inclination (θ5) may each be acute. For example, the first angle of inclination (θ1) may be greater than 85° and less than 90°, and the second angle of inclination (θ2) may be greater than 90° and less than 95°. The third angle of inclination (θ3), the fourth angle of inclination (θ4), and the fifth angle of inclination (θ5) may each be greater than 85° and less than 90°. The first side (SID1) and the second side (SID2) may be aligned with each other, and the third side (SID3), the fourth side (SID4), and the fifth side (SID5) may be aligned with each other. In this case, the first side (SID1) and the second side (SID2) may be adjacent to each other but not integrally aligned.

[0285] Referring to FIG. 18c, the first inclination angle (θ1) and the second inclination angle (θ2) may each be right angles, and the third inclination angle (θ3), the fourth inclination angle (θ4), and the fifth inclination angle (θ5) may each be acute angles. For example, the first inclination angle (θ1) and the second inclination angle (θ2) may each be 90°, and the third inclination angle (θ3), the fourth inclination angle (θ4), and the fifth inclination angle (θ5) may each be greater than 85° and less than 90°. In this case, the first side (SID1) and the second side (SID2) may be vertically aligned.

[0286] Referring again to FIG. 18a and FIG. 18c, the difference between the first inclination angle (θ1) and the second inclination angle (θ2) may be greater than 3°. For example, the difference between the first inclination angle (θ1) and the second inclination angle (θ2) may be greater than 3° and equal to or less than 20°. Alternatively, the difference between the first inclination angle (θ1) and the second inclination angle (θ2) may be greater than 3° and equal to or less than 10°.

[0287]

[0288] FIGS. 19 to 21 are conceptual diagrams for explaining a method of manufacturing an all-solid-state battery using a first electrode manufactured by the manufacturing method described above with reference to FIG. 15.

[0289] Referring to FIG. 19, a method for manufacturing an all-solid-state battery according to one embodiment of the present invention may include preparing a second electrode; and applying pressure so that the prepared first electrode and the second electrode are joined. Specifically, preparing the second electrode may include forming a negative electrode coating layer on a negative electrode substrate and forming a solid electrolyte layer on the negative electrode coating layer. Specifically, forming the negative electrode coating layer may be formed by directly coating a negative electrode active material slurry onto the negative electrode substrate.

[0290] Pressing to join the first electrode and the second electrode may involve joining the first electrode and the second electrode so that the solid electrolyte layer (310) of the second electrode and the second positive active material layer (120_2) of the first electrode come into contact with each other, and applying a first pressure.

[0291] For example, combining the first electrode and the second electrode may include a pressurization process in which a hydraulic plate press is applied. However, this method is not necessarily limited to this method, and any pressurization process applicable in the relevant technical field may be applied. For example, pressurization processes such as a roll press and a warm isostatic press may be applied.

[0292] When a roll press is applied during the formation process of the all-solid-state battery, the first pressure may be 0.1 ton / cm or more. Specifically, the first pressure may be 0.5 ton / cm or more and 1.0 ton / cm or more. The first pressure may be 2.0 ton / cm or less. Specifically, the first pressure may be 1.5 ton / cm or less.

[0293] FIGS. 20 and 21 are conceptual diagrams for explaining a method for manufacturing an all-solid-state battery according to another embodiment of the present invention.

[0294] FIG. 20 is a conceptual diagram illustrating a method for manufacturing an all-solid-state battery according to another embodiment of the invention. In this embodiment, detailed descriptions of technical features that overlap with those previously described with reference to FIG. 15, FIG. 16a to 16g, and FIG. 19 are omitted, and the differences are described in detail.

[0295] An all-solid-state battery according to another embodiment of the present invention may include first and second monocells (510, 520). The second monocell (520) may be arranged vertically symmetrically with respect to the first monocell (510) and combined by applying pressure. Specifically, the all-solid-state battery may be manufactured by symmetrically arranging and combining the first monocell (510) and the second monocell (520) so that the positive current collectors (110) of each of the first and second monocells (510, 520) come into contact with each other, and by applying pressure. Referring to FIG. 21, an elastic member (ELP) may be further included on the upper and lower portions of the monocells (510, 520) of the all-solid-state battery.

[0296]

[0297] Hereinafter, embodiments and comparative examples of the present invention are described. However, the following embodiments are merely examples of the present invention, and the present invention is not limited to the following embodiments.

[0298] Example 1-1

[0299] (Transfer component manufacturing)

[0300] solid electrolyte layer

[0301] A mixture was prepared by adding 1 part by weight of a polytetrafluoroethylene (PTFE) first binder and 1 part by weight of a polyvinylidene fluoride (PVDF) second binder to an argyrodite-type crystal Li6PS5Cl sulfide-based solid electrolyte (D50 = 3 μm, crystalline) with respect to 98 parts by weight of the solid electrolyte into a grind mixer and mixing. A dough was prepared by adding the prepared mixture to a mortar heated to 80°C and stirring. The prepared dough was passed through a roller and formed into a sheet shape to prepare a solid electrolyte membrane of uniform thickness.

[0302] A solid electrolyte layer was prepared by the above process. The above solid electrolyte layer consisted of a first solid electrolyte layer having substantially the same area as the anode layer and a second solid electrolyte layer having substantially the same area as the cathode layer. The elastic modulus of the sulfide-based solid electrolyte was approximately 15 GPa to 30 GPa.

[0303] Anode slurry

[0304] LiNi coated with Li2O-ZrO2 (LZO) as a positive electrode active material 0.8 Co 0.15 Mn 0.05 O2(NCM) was prepared. The LZO-coated cathode active material was prepared according to the method disclosed in Korean Patent Publication No. 10-2016-0064942.

[0305] Li6PS5Cl, an argyrodite-type crystal (D50 = 0.5 μm, crystalline), was prepared as a solid electrolyte. Polytetrafluoroethylene (PTFE) binder was prepared as a binder. Carbon nanofiber (CNF) was prepared as a conductive agent. These materials were mixed with xylene solvent in a weight ratio of positive active material : solid electrolyte : conductive agent : binder = 84 : 11.5 : 3 : 1.5 to prepare a positive slurry.

[0306] Warrior absence

[0307] A first solid electrolyte layer prepared previously was laminated onto an aluminum substrate. Then, a previously prepared anode slurry was applied onto the first solid electrolyte layer and dried to form an anode active material layer. That is, a transfer member was manufactured in which a transfer layer (first solid electrolyte layer and anode active material layer) was formed on an aluminum substrate (strip substrate). One side of the manufactured transfer member was slit. The angle of inclination of the side of the anode active material layer and the first solid electrolyte layer of the slit transfer member was measured to be approximately 87°.

[0308]

[0309] (Manufacturing of anode semi-finished products)

[0310] A previously manufactured transfer member was laminated so that a positive active material layer was in contact with the cross-section of a positive current collector, which is made of aluminum foil with a carbon coating on its cross-section. The transfer member and the positive current collector were laminated by cold rolling at a pressure of 3.0 ton / cm. Subsequently, the aluminum substrate on the uppermost surface was peeled off to produce a positive semi-finished product comprising a positive layer and a first solid electrolyte layer on the positive layer. Then, the other side opposite to the positive tab was slit. The inclination angle of the other side of the positive current collector, positive active material layer, and first solid electrolyte layer formed by the slitting was measured to be approximately 88°.

[0311] The total thickness of the anode layer was approximately 120 μm. The thickness of the anode active material layer was approximately 107 μm, and the thickness of the carbon-coated (thickness 1 mm) aluminum foil was approximately 13 μm. The area of ​​the anode current collector, excluding the anode active material layer and the anode tab, was the same. The thickness of the first solid electrolyte layer was approximately 10 μm.

[0312] (Manufacture of cathode semi-finished products)

[0313] cathode layer

[0314] A Ni foil with a thickness of 10 μm was prepared as a cathode current collector. Additionally, as the material for the cathode coating layer, carbon black (CB) with a primary particle size of approximately 30 nm and silver (Ag) particles with an average particle size (D50) of approximately 60 nm were prepared. 4 g of a mixed powder, prepared by mixing carbon black (CB) and silver (Ag) particles in a weight ratio of 3:1, was placed in a container, and 4 g of an NMP solution containing 7 wt% of PVDF binder (Kureha # 9300) was added to prepare a mixed solution. Subsequently, a cathode coating slurry was prepared by stirring the mixed solution while gradually adding NMP to it. The prepared slurry was applied to a Ni sheet using a bar coater and dried in air at 80°C for 10 minutes. The resulting laminate was vacuum dried at 40°C for 10 hours. The dried laminate was cold-roll-pressed at a pressure of 1.5 ton / cm to flatten the surface of the cathode coating layer of the laminate. The cathode layer was fabricated by the above process. The thickness of the cathode coating layer included in the cathode layer was approximately 7 μm. The area of ​​the cathode current collector, excluding the cathode coating layer and the cathode tab portion, was the same.

[0315] Cathode semi-finished product

[0316] After stacking the previously manufactured second solid electrolyte layer on the previously manufactured cathode layer, the laminate was laminated by cold rolling at a pressure of 3.0 ton / cm.

[0317] (Manufacture of fixed layer, inert member (gasket))

[0318] A fixed layer was prepared to be disposed on a second solid electrolyte layer adjacent to the cathode layer. An adsorption flame retardant film member was prepared as the material of the fixed layer. For example, pulp fibers, glass fibers, Al(OH)3, binders, and mixtures thereof were prepared as the fixed layer.

[0319] An inert member (gasket) is prepared to surround a first solid electrolyte layer adjacent to an anode layer on a second solid electrolyte layer adjacent to a cathode layer. By providing a fixing layer, the inert member can be fixed without detaching from the fixing layer. The adhesive strength of the fixing layer may be 50gf / 25mm to 300gf / 25mm, and specifically, the adhesive strength of the fixing layer may be 200gf / 25mm.

[0320] (Manufacturing of all-solid-state batteries)

[0321] An all-solid-state battery was manufactured by assembling the previously manufactured positive electrode semi-product, negative electrode semi-product, and inert member. An all-solid-state battery was manufactured by stacking the inert member and the positive electrode semi-product on the negative electrode semi-product and pressing the stack at a pressure of 0.5 ton / cm².

[0322] Referring to FIG. 1, the second width (W2) of the second solid electrolyte layer was manufactured to be 4 mm larger than the first width (W1) of the first solid electrolyte layer. The thickness (t1) of the first solid electrolyte layer was 10 μm, and the thickness (t2) of the second solid electrolyte layer was manufactured to be 60 μm.

[0323]

[0324] Examples 1-2

[0325] A positive electrode semi-product, a negative electrode semi-product, and an all-solid-state battery were manufactured in the same manner as in Example 1-1, except that the thickness (t1) of the first solid electrolyte layer was 30 μm and the thickness (t2) of the second solid electrolyte layer was 30 μm.

[0326]

[0327] Comparative Example 1-1

[0328] A cathode semi-product and an all-solid-state battery were manufactured in the same manner as in Example 1-1, except that the positive electrode semi-product was manufactured as follows. That is, in Comparative Example 1-1, a positive electrode active material layer was formed by directly applying a positive electrode active material slurry onto a positive electrode current collector as follows.

[0329] (Anode semi-finished product)

[0330] anode layer

[0331] An anode layer was prepared by applying and drying the anode slurry prepared according to Example 1-1 onto the cross-section of an anode current collector made of aluminum foil with carbon coating on the cross-section.

[0332] The total thickness of the anode layer was approximately 120 µm. The thickness of the anode active material layer was approximately 107 µm, and the thickness of the carbon-coated (thickness 1 m) aluminum foil was approximately 13 µm. The area of ​​the anode current collector, excluding the anode active material layer and the anode tab, was the same.

[0333] anode semi-finished product

[0334] The previously manufactured anode layer and the first solid electrolyte layer manufactured according to Example 1-1 were laminated and pressed using a roll press method. An anode semi-finished product was manufactured by applying a linear pressure of 3.5 ton / cm at 120 ℃.

[0335] Subsequently, a cathode semi-finished product and an all-solid-state battery were manufactured using the same method as in Example 1-1.

[0336] In the manufactured all-solid-state battery, the angle of inclination of one side of the positive active material layer adjacent to the positive tab and one side of the first solid electrolyte layer was measured. The angle of inclination of the first solid electrolyte layer was measured to be approximately 80°, and the angle of inclination of the positive active material layer was measured to be approximately 62°.

[0337]

[0338] Example 2-1

[0339] (Transfer component manufacturing)

[0340] Anode slurry

[0341] LiNi coated with Li2O-ZrO2 (LZO) as a positive electrode active material 0.8 Co 0.15 Mn 0.05 O2(NCM) was prepared. The LZO-coated cathode active material was prepared according to the method disclosed in Korean Patent Publication No. 10-2016-0064942.

[0342] Li6PS5Cl, an argyrodite-type crystal (D50 = 0.5 μm, crystalline), was prepared as a solid electrolyte. Polytetrafluoroethylene (PTFE) binder was prepared as a binder. Carbon nanofiber (CNF) was prepared as a conductive agent. These materials were mixed with xylene solvent in a weight ratio of positive active material : solid electrolyte : conductive agent : binder = 84 : 11.5 : 3 : 1.5 to prepare a positive slurry.

[0343] Warrior absence

[0344] A first positive active material layer was formed by applying the previously prepared positive slurry onto a first aluminum substrate and drying it. A second positive active material layer was formed by applying the previously prepared positive slurry onto a second aluminum substrate and drying it. That is, a first transfer member was manufactured in which a first transfer layer (first positive active material layer) was formed on a first aluminum substrate (release substrate). A second transfer member was manufactured in which a second transfer layer (second positive active material layer) was formed on a second aluminum substrate (release substrate). After laminating the second transfer layer onto the first transfer layer, the first transfer layer and the second transfer layer were bonded. One side of the bonded first transfer member and second transfer member was slit. The angle of inclination of each side of the slit first transfer layer and the second transfer layer was measured to be approximately 87°.

[0345] (Manufacturing of anode semi-finished products)

[0346] The first aluminum substrate of the previously manufactured first transfer member was peeled off. The previously manufactured first transfer member and second transfer member were laminated so that the first transfer layer was in contact with the cross-section of an anode current collector made of aluminum foil with a carbon coating on one side. The first transfer member, the second transfer member, and the anode current collector were laminated by roll pressing at a pressure of 3.5 ton / cm. Afterward, the second aluminum substrate on the top surface was peeled off to manufacture an anode semi-product including a first anode active material layer and a second anode active material layer. Then, the other side opposite to the anode tab was slit. The inclination angle of the other side of the anode current collector, the first anode active material layer, and the second anode active material layer formed by the slitting was measured to be approximately 87°.

[0347] The total thickness of the anode layer was approximately 190 μm. The thickness of the first anode active material layer was approximately 93 μm, and the thickness of the second anode active material layer was approximately 93 μm. The thickness of the carbon-coated (thickness 1 mm) aluminum foil was approximately 10 μm. The area of ​​the anode current collector, excluding the anode active material layer and the anode tab, was the same.

[0348] (Manufacture of cathode semi-finished products)

[0349] cathode layer

[0350] A Ni foil with a thickness of 10 μm was prepared as a cathode current collector. Additionally, as the material for the cathode coating layer, carbon black (CB) with a primary particle size of approximately 30 nm and silver (Ag) particles with an average particle size (D50) of approximately 60 nm were prepared. 4 g of a mixed powder, prepared by mixing carbon black (CB) and silver (Ag) particles in a weight ratio of 3:1, was placed in a container, and 4 g of an NMP solution containing 7 wt% of PVDF binder (Kureha # 9300) was added to prepare a mixed solution. Subsequently, a cathode coating slurry was prepared by stirring the mixed solution while gradually adding NMP to it. The prepared slurry was applied to a Ni sheet using a bar coater and dried in air at 80°C for 10 minutes. The resulting laminate was vacuum dried at 40°C for 10 hours. The dried laminate was cold-roll-pressed at a pressure of 1.5 ton / cm to flatten the surface of the cathode coating layer of the laminate. The cathode layer was fabricated by the above process. The thickness of the cathode coating layer included in the cathode layer was approximately 7 μm. The area of ​​the cathode current collector, excluding the cathode coating layer and the cathode tab portion, was the same.

[0351] solid electrolyte layer

[0352] A mixture was prepared by adding 1 part by weight of a polytetrafluoroethylene (PTFE) first binder and 1 part by weight of a polyvinylidene fluoride (PVDF) second binder to an argyrodite-type crystal Li6PS5Cl sulfide-based solid electrolyte (D50 = 3 μm, crystalline) with respect to 98 parts by weight of the solid electrolyte into a grind mixer and mixing. A dough was prepared by adding the prepared mixture to a mortar heated to 80°C and stirring. The prepared dough was passed through a roller and formed into a sheet shape to prepare a solid electrolyte membrane of uniform thickness.

[0353] A solid electrolyte layer was prepared by the above process. Each of the above solid electrolyte layers was prepared having a substantially the same area as the cathode layer. The elastic modulus of the sulfide-based solid electrolyte was about 15 GPa to 30 GPa.

[0354] Cathode semi-finished product

[0355] After stacking the previously manufactured solid electrolyte layer on the previously manufactured cathode layer, the laminate was laminated by cold rolling at a pressure of 3.0 ton / cm.

[0356] (Manufacture of fixed layer, inert member (gasket))

[0357] A fixed layer was prepared to be disposed on a solid electrolyte layer adjacent to the cathode layer. An adsorption flame retardant film member was prepared as the material of the fixed layer. For example, pulp fibers, glass fibers, Al(OH)3, binders, and mixtures thereof were prepared as the fixed layer.

[0358] An inert member (gasket) is prepared to surround a first positive active material layer and a second positive active material layer adjacent to an anode layer on a solid electrolyte layer adjacent to a cathode layer. By providing a fixing layer, the inert member can be fixed without detaching from the fixing layer. The adhesive strength of the fixing layer may be 50gf / 25mm to 300gf / 25mm, and specifically, the adhesive strength of the fixing layer may be 200gf / 25mm.

[0359] (Manufacturing of all-solid-state batteries)

[0360] An all-solid-state battery was manufactured by assembling the previously manufactured positive electrode semi-product, negative electrode semi-product, and inert member. An all-solid-state battery was manufactured by stacking the inert member and the positive electrode semi-product on the negative electrode semi-product and pressing the stack at a pressure of 0.5 ton / cm².

[0361]

[0362] Example 2-2

[0363] A solid-state battery was manufactured using the same method as in Example 2-1, except that the thickness of the second positive active material layer was 96 μm and the positive active material in the second positive active material layer was formed to be 83 parts by weight.

[0364]

[0365] Examples 2-3

[0366] A solid-state battery was manufactured using the same method as in Example 2-1, except that the thickness of the second positive active material layer was 99 μm and the positive active material in the second positive active material layer was formed to be 80 parts by weight.

[0367]

[0368] Examples 2-4

[0369] A solid-state battery was manufactured using the same method as in Example 2-1, except that the thickness of the second positive active material layer was 106 μm and the positive active material in the second positive active material layer was formed to be 75 parts by weight.

[0370]

[0371] Examples 2-5

[0372] A solid-state battery was manufactured using the same method as in Example 2-1, except that the thickness of the first positive active material layer was 88 μm and the positive active material in the first positive active material layer was formed to be 90 parts by weight.

[0373]

[0374] Examples 2-6

[0375] A solid-state battery was manufactured using the same method as in Example 2-1, except that when manufacturing the solid-state battery, the thickness of the second positive active material layer was 88 μm and the positive active material in the second positive active material layer was formed to be 90 parts by weight.

[0376]

[0377] Comparative Example 2-1

[0378] An all-solid-state battery identical to the one described above was manufactured, except that the second positive active material layer formed in Example 2-1 above was omitted.

[0379]

[0380] Evaluation Example 1: Good Product Rate (Mass Manufacturability)

[0381] The all-solid-state batteries manufactured according to Examples 1-1, 1-2 and Comparative Example 1-1 were subjected to a yield rate test to verify the mass producibility of the batteries. The yield rate test evaluates the ratio of the number of good samples to the total number of samples produced; specifically, 100 samples were manufactured for each of the examples and comparative examples to conduct the test. The results of the yield rate test were classified as a percentage based on the number of good cells among the 100 samples. The classification results are shown in Table 1 below. Good (or defective) products were determined based on the value of OCV (IM 3590 Impedance Analyzer, Open circuit voltage, 1kHz, 1V). If the OCV value was less than 100mV, it was determined to be defective, and if the OCV value was 100mV or more but less than 300mV, it was determined to be a good product.

[0382]

[0383] Evaluation Example 2: Initial dosage

[0384] The all-solid-state batteries prepared according to Examples 1-1, 1-2 and Comparative Example 1-1 were evaluated by the following charge-discharge test. The charge-discharge test was performed by placing the all-solid-state batteries in a constant temperature bath at 45°C. In the first cycle, the battery was charged at a constant current of 0.1C until the battery voltage reached 4.25V, and upon reaching 4.25V, charging was performed at a constant voltage of 4.25V under a 0.05C cut-off condition. Subsequently, the battery was discharged at a constant current of 0.1C until the battery voltage reached 2.5V. The discharge capacity of the first cycle was set as the initial capacity. The results are shown in Table 1 below. The initial capacity was measured under standard method (first discharge amount) conditions and is shown in Table 1 below.

[0385]

[0386] Evaluation Example 3: Evaluation of Life Characteristics at the Time of Short Circuit Occurrence

[0387] The all-solid-state batteries prepared according to the examples and comparative examples were evaluated by the following charge-discharge test. The charge-discharge test was performed by placing the all-solid-state batteries in a constant temperature bath at 45°C. In the first cycle, the battery was charged with a constant current of 0.33C until the battery voltage reached 4.25V, and upon reaching 4.25V, constant voltage charging was performed at 4.25V under a 0.1C cut-off condition. Subsequently, the battery was discharged with a constant current of 0.33C until the battery voltage reached 2.5V. From the second cycle onwards, charging and discharging were performed up to 350 cycles under the same conditions as the first cycle. This implies that the life characteristics improve as the number of cycles at which a short circuit occurs increases. The results of the charge-discharge test are shown in Table 1 below. A short circuit was confirmed to have occurred using the standard method (charge amount during life = discharge amount * 10%), and the number of times the life had progressed up to that point was recorded and is shown in Table 1 below.

[0388] Evaluation of method for forming a positive active material layer on a positive current collector Quantity of good products (%) Initial capacity (mAh / g) Time of short circuit occurrence Example 1-1 Transfer 92190 > 200 Example 1-2 Transfer 52170 > 150 Comparative Example 1-1 Direct coating 68180 < 50” > n” means that no short circuit occurs even after n cycle tests. <n”은, n회 사이클 시험 동안 단락이 발생함을 의미함.

[0389] Referring to Table 1, it can be seen that the all-solid-state batteries of Examples 1-1 and 1-2, in which a positive active material layer is formed on a positive current collector by a transfer method, have excellent lifespan characteristics related to short circuit occurrence. On the other hand, it can be seen that the all-solid-state battery of Comparative Example 1-1, in which a positive active material layer is directly coated on a positive current collector, has poor lifespan characteristics.

[0390]

[0391] Evaluation Example 4: Initial dosage

[0392] All-solid-state batteries prepared according to Examples 2-1 to 2-6 and Comparative Example 2-1 were evaluated by the following charge-discharge test. The charge-discharge test was performed by placing the all-solid-state batteries in a constant temperature bath at 45°C. In the first cycle, the battery was charged at a constant current of 0.1C until the battery voltage reached 4.25V, and upon reaching 4.25V, charging was performed at a constant voltage of 4.25V under a 0.05C cut-off condition. Subsequently, the battery was discharged at a constant current of 0.1C until the battery voltage reached 2.5V. The discharge capacity of the first cycle was set as the initial capacity. The results are shown in Table 1 below. The initial capacity was measured under standard method (first discharge amount) conditions and is shown in Table 1 below.

[0393]

[0394] Evaluation Example 5: Charge / Discharge Rate

[0395] The charge and discharge levels of the all-solid-state batteries prepared according to Examples 2-1 to 2-6 and Comparative Example 2-1 were verified through a charge-discharge test (duration = 1 hr). Specifically, after preparing samples for each example and comparative example, a charge-discharge test was performed. The results of the charge-discharge rate experiment based on the samples are shown in Table 2 below.

[0396] First positive active material layer Second positive active material layer Initial capacity (mAh) Charge / discharge rate (%) Active material (%) L / L (mg / cm²) 2 )Thickness (㎛) Active Material (%) L / L (mg / cm²) 2 Thickness (㎛) Example 2-185 25.493.485 25.493.479475 Example 2-285 25.493.483 25.495.678580 Example 2-385 25.493.480 25.499.277183 Example 2-485 25.493.475 25.410 5.874885 Example 2-590 25.488.285 25.493.4777.170 Example 2-685 25.493.490 25.488.273 6.265 Comparative Example 2-185 25.493.4---35777

[0397] Referring to Table 2, it can be seen that the all-solid-state batteries of Examples 2-1 to 2-6, which are formed by slitting both sides and have multiple layers of positive active material, have superior initial capacity and charge / discharge rate compared to Comparative Example 2-1. On the other hand, it can be seen that the all-solid-state battery of Comparative Example 2-1, in which a second positive active material layer is not formed, has an initial capacity that is less than half of that of the all-solid-state batteries of Examples 2-1 to 2-6.

Claims

1. Preparing a first transfer member by forming a first transfer layer on a first peelable substrate; Slitting one side of the first transfer member; Transferring the first transfer layer on the first peeling substrate onto the positive substrate; and The method includes preparing a first electrode by slitting the other side of the first transfer layer together with the anode substrate, wherein A method for manufacturing an all-solid-state battery, wherein the first transfer layer comprises at least one of a first solid electrolyte layer and a positive electrode active material layer.

2. In Paragraph 1, The above first transfer layer includes a solid electrolyte layer and an anode active material layer. A method for manufacturing an all-solid-state battery in which the solid electrolyte layer is located between the first peeling substrate and the positive active material layer.

3. In Paragraph 2, Preparing the above-mentioned first transfer member is: Forming the first solid electrolyte layer on the first peelable substrate; and A method for manufacturing an all-solid-state battery, comprising forming a positive active material layer on the first solid electrolyte layer.

4. In Paragraph 3, Forming the positive active material layer on the first solid electrolyte layer is: A method for manufacturing an all-solid-state battery, comprising coating a positive electrode active material slurry on the first solid electrolyte layer.

5. In Paragraph 3, Forming the positive active material layer on the first solid electrolyte layer is: Forming the positive active material layer on the second peelable substrate; and A method for manufacturing an all-solid-state battery, comprising transferring the second positive active material layer onto the first solid electrolyte layer.

6. In Paragraph 1, The first transfer layer comprises the positive active material layer, wherein A method for manufacturing an all-solid-state battery, wherein the positive active material layer comprises a first positive active material layer and a second positive active material layer on the first positive active material layer.

7. In Paragraph 6, Forming the above-mentioned first transfer layer is: Forming the first positive active material layer on the first peelable substrate; Forming the second positive active material layer on the second peelable substrate; and A method for manufacturing an all-solid-state battery, comprising transferring the second positive active material layer onto the first positive active material layer.

8. In Paragraph 1, Slitting the one side of the first transfer member is: Based on the vertical direction from the upper surface to the lower surface of the first transfer member, A method for manufacturing an all-solid-state battery, comprising slitting one side of the first transfer member at an angle within ±5°.

9. In Paragraph 1, One side of the anode substrate includes a first tab portion protruding in a first direction, and A method for manufacturing an all-solid-state battery, wherein one side of the anode substrate is adjacent to the slit one side of the first transfer layer.

10. In Paragraph 1, Preparing a second electrode; and The method further includes laminating the first electrode and the second electrode, A method for manufacturing an all-solid-state battery, wherein the second electrode comprises a negative electrode substrate and a negative electrode coating layer on the negative electrode substrate.

11. Anode material; A first positive active material layer on the above positive substrate; and It includes a first transfer layer on the first positive active material layer, The first transfer layer comprises at least one of the second positive active material layer and the first solid electrolyte layer, and One side of the anode substrate includes a first tab portion protruding in a first direction, and The first positive active material layer includes a first side adjacent to the first tab portion, and The first transfer layer includes a second side adjacent to the first tab portion, and The first inclination angle formed by the first side surface and the lower surface of the anode substrate is 85° to 95°, and An all-solid-state battery in which the second angle of inclination formed by the second side and the lower surface of the first positive active material layer is 85° to 95°.

12. In Paragraph 11, The above anode substrate includes a third side adjacent to the first side, and The first side and the second side are aligned with each other, The above-mentioned first side and the above-mentioned third side are not aligned with each other, in a solid-state battery.

13. In Paragraph 11, A solid-state battery in which the first angle of inclination and the second angle of inclination are substantially the same.

14. In Paragraph 11, The first positive active material layer includes a fourth side spaced apart from the first side in the first direction, and The first transfer layer includes a fifth side spaced apart from the second side and in the first direction, and The above anode substrate includes a sixth side adjacent to the fourth side, and The above-mentioned fourth to sixth sides are aligned with each other, forming an all-solid-state battery.

15. In Paragraph 11, A second solid electrolyte layer on the first transfer layer; and A solid-state battery further comprising a negative electrode layer on the second solid electrolyte layer.

16. In Paragraph 11, An inert member surrounding the first positive active material layer; and A solid-state battery further comprising an air gap between the first positive active material layer and the inert member.

17. In Paragraph 11, Either one of the first and second inclination angles is greater than 85° and less than 90°, and The remaining one of the first and second inclination angles is greater than 90° and less than 95° for an all-solid-state battery.

18. In Paragraph 11, A solid-state battery in which each of the first and second inclination angles is greater than 85° and less than 90°.

19. In Paragraph 11, A solid-state battery in which each of the first and second inclination angles is greater than 90° and less than 95°.

20. In Paragraph 11, The first transfer layer comprises the second positive active material layer, and An all-solid-state battery having a total thickness of 80㎛ to 100㎛ of the first and second positive active material layers.

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