Stacking apparatus and method for manufacturing all-solid-state battery using same

Abstract

The present invention relates to a stacking apparatus and a method for manufacturing an all-solid-state battery using same. More specifically, the stacking apparatus comprises: a stacking table comprising a stage and a rotary unit, the rotary unit being configured to rotate to a first position, a second position, a third position, and a fourth position as the stage rotates; a first input unit adjacent to the first position, the first input unit being configured to stack a first sheet on the stage; a second input unit adjacent to the second position, the second input unit being configured to stack a second sheet on the stage; a third input unit adjacent to the third position, the third input unit being configured to stack a third sheet on the stage; a first discharge gripper adjacent to the fourth position; and a pressing unit adjacent to the first discharge gripper.

Description

Laminating device and method for manufacturing an all-solid-state battery using the same

[0001] The present invention relates to a laminating device and a method for manufacturing an all-solid-state battery using the same, and more specifically, to a laminating device and a laminating method capable of continuously laminating sheets on a rotating circulating stage.

[0002]

[0003] Recent industrial demands have led to the active development of batteries with high energy density and safety. For example, lithium-ion batteries are being used not only in information and communication devices, but also in the automotive sector. Safety is particularly important in the automotive sector, as it is directly related to life.

[0004] Meanwhile, lithium-ion batteries currently on the market contain electrolytes containing flammable organic dispersions, which pose a risk of overheating and fire in the event of a short circuit. Considering these issues, all-solid-state batteries, which replace the electrolyte with a solid electrolyte, are being proposed. By eliminating flammable organic dispersions, all-solid-state batteries significantly reduce the risk of fire or explosion in the event of a short circuit. Therefore, these all-solid-state batteries can significantly improve safety compared to lithium-ion batteries that use electrolytes.

[0005]

[0006] The problem to be solved by the present invention is to provide a lamination device capable of continuously laminating sheets constituting an all-solid-state battery.

[0007] Another problem to be solved by the present invention is to provide a method for manufacturing an all-solid-state battery using the above-mentioned stacking device.

[0008]

[0009] According to one embodiment of the present invention, a stacking device may include a stacking table including a stage and a rotation unit, the rotation unit being configured to cycle through a first position, a second position, a third position, and a fourth position while the stage rotates; a first input unit adjacent to the first position, the first input unit being configured to stack a first sheet on the stage; a second input unit adjacent to the second position, the second input unit being configured to stack a second sheet on the stage; a third input unit adjacent to the third position, the third input unit being configured to stack a third sheet on the stage; a first discharge gripper adjacent to the fourth position; and a pressing unit adjacent to the first discharge gripper. The first discharge gripper is configured to transfer a stack including the first to third sheets from the stage to the pressing unit, and the pressing unit may be configured to perform a pressing process on the stack.

[0010] According to another embodiment of the present invention, a method for manufacturing an all-solid-state battery may include: laminating a first sheet on a stage at a first position; laminating a second sheet on the stage at a second position; laminating a third sheet on the stage at a third position; and performing a pressing process on a laminate including the first to third sheets. The stage may rotate and cycle through the first position, the second position, and the third position.

[0011]

[0012] The laminating device according to the present invention can continuously laminate sheets by rotating and circulating the stage. The pressing unit can receive the laminate and form an all-solid-state battery in a single pressurization process. This allows the manufacturing process for all-solid-state batteries to be performed efficiently.

[0013] The laminating device according to the present invention can laminate monocells or cathode / anode layers. That is, the laminating process can be continuously performed without limitation even if the sheet has the form of a monocell or an electrode layer.

[0014]

[0015] FIG. 1 and FIG. 2 are each cross-sectional views illustrating an all-solid-state battery according to embodiments of the present invention.

[0016] FIG. 3 is a plan view illustrating a stacking device of an all-solid-state battery according to embodiments of the present invention.

[0017] FIGS. 4 to 8 are cross-sectional views illustrating a method for manufacturing an all-solid-state battery according to embodiments of the present invention.

[0018] FIG. 9 is a plan view illustrating another embodiment of the first input unit of the stacking device of FIG. 3.

[0019] FIGS. 10 to 15 are cross-sectional views illustrating a method for manufacturing an all-solid-state battery according to embodiments of the present invention.

[0020]

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

[0022] In this specification, when a component is referred to as being on another component, it means that it can be formed directly on the other component, or a third component may be interposed between them. Also, in the drawings, the thickness of the components is exaggerated for the purpose of effectively explaining the technical contents. Parts designated by the same reference numbers throughout the specification represent the same components.

[0023] The embodiments described herein will be described with reference to cross-sectional views, plan views, and / or perspective views, which are ideal illustrations of the present invention. Although terms such as "first," "second," and "third" are used to describe various components in various embodiments of this specification, these components should not be limited by these terms. These terms are used merely to distinguish one component from another. The embodiments described and illustrated herein also include complementary embodiments.

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

[0025]

[0026] FIG. 1 and FIG. 2 are cross-sectional views illustrating an all-solid-state battery according to embodiments of the present invention. Referring to FIG. 1, a mono-cell (MNC) of an all-solid-state battery according to one embodiment of the present invention is illustrated. The mono-cell (MNC) may include a positive electrode layer (100), a negative electrode layer (200) facing the positive electrode layer (100), and a solid electrolyte layer (300) disposed between the positive electrode layer (100) and the negative electrode layer (200). However, the present invention is not limited thereto, and the mono-cell (MNC) 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).

[0027] The positive electrode layer (100) may include a positive electrode current collector (110) and a positive electrode active material layer (120) disposed on the positive electrode current collector (110). The positive electrode active material layer (120) may include a positive electrode active material, a solid electrolyte, a conductive material, and a binder.

[0028] The positive electrode current collector (110) can provide a reference surface on which the positive electrode active material layer (120) is arranged. The positive electrode current collector (110) can have a plate or foil shape. For example, the positive electrode current collector (110) can include 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.

[0029] Unlike that illustrated in FIG. 1, in one embodiment of the present invention, the positive electrode current collector (110) may be omitted. Although not illustrated, a carbon layer having a thickness of 0.1 μm to 4 μm may be additionally disposed between the positive electrode current collector (110) and the positive electrode active material layer (120) to increase the bonding strength between the positive electrode current collector (110) and the positive electrode active material layer (120).

[0030] The cathode active material may be a material that can reversibly absorb and desorb lithium ions. For example, the cathode active material may include, but is not limited to, lithium transition metal oxides such as lithium cobalt oxide (LCO), lithium nickel oxide, lithium nickel cobalt oxide, lithium nickel cobalt aluminum oxide (NCA), lithium nickel cobalt manganese oxide (NCM), lithium manganate, and lithium iron phosphate, nickel sulfide, copper sulfide, lithium sulfide, iron oxide, or vanadium oxide. The cathode active materials may be used alone or as a mixture of two or more thereof.

[0031] Lithium transition metal oxides include, for example, Li a A 1-b B b D2(0.90≤a≤1, 0≤b≤0.5), Li a E 1-b B b O 2-c D c (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05), LiE 2-b B b O 4-c D c (0≤b≤0.5, 0≤c≤0.05), Li a Ni 1-b-c Co b B c D α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α<2), Li a Ni 1-b-c Co b B c O 2-α F α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α<2), Li a Ni 1-b-c Mn b B c D α(0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α≤2), Li a 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 may be a compound represented by any one of Fe2(PO4)3(0≤f≤2), LiFePO4. In these compounds, a capital letter “” is Ni, Co, Mn, or a combination thereof, a capital letter “” is Al, Ni, Co, Mn, Cr, Fe, Mg, Sr, V, a rare earth element, or a combination thereof, a capital letter “” is O, F, S, P, or a combination thereof, a capital letter “” is Co, Mn, or a combination thereof, a capital letter “” is F, S, P, or a combination thereof, a capital letter “” is Al, Cr, Mn, Fe, Mg, La, Ce, Sr, V, or a combination thereof, a capital letter “” is Ti, Mo, Mn, or a combination thereof, a capital letter “” is Cr, V, Fe, Sc, Y, or a combination thereof, and a capital letter “” is V, Cr, Mn, Co, Ni, Cu, or a combination thereof.

[0032] The cathode active material may include, for example, a lithium salt of a transition metal oxide having a layered rock salt type structure among the lithium transition metal oxides described above. The "layered rock salt type structure" is, for example, a cubic rock salt type structure. <111> It is a structure in which oxygen atomic layers and metal atomic layers are arranged alternately and regularly in the direction, and each atomic layer thereby forms a two-dimensional plane. The "cubic rock salt structure" refers to the sodium chloride type (NaCl type) structure, which is a type of crystal structure, and specifically refers to a structure in which the face-centered cubic lattice (fcc) formed by each cation and anion is arranged with a displacement of half of the ridge of the unit lattice. Lithium transition metal oxides having this layered rock salt structure include, for example, LiNi x Co y Al z O2(NCA) or LiNi x Co y Mn 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, 모노셀(MNC)의 에너지 밀도가 커지고 열안정성이 향상될 수 있다.

[0033] The above-described compound included in the positive electrode active material may be covered by a coating layer (not shown). The positive electrode active material may also be a mixture of the above-described compound and a compound to which a coating layer is added. Meanwhile, the coating layer added to the surface of the positive electrode active material may include, for example, an oxide, a hydroxide, an oxyhydroxide, an oxycarbonate, or a hydroxycarbonate of the coating elements below. The compound forming the coating layer may be 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 may be 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 may include, for example, a spray coating method or an immersion method.

[0034] When the positive electrode active material is a ternary lithium transition metal oxide such as NCA or NCM and contains nickel (Ni), it may be possible to increase the capacity density of the monocell (MNC) and reduce metal dissolution of the positive electrode active material in a charged state. As a result, the cycle characteristics of the monocell (MNC) in a charged state may be improved. Meanwhile, the “cycle characteristics” are characteristics indicating the degree to which the monocell (MNC) deteriorates due to charge / discharge of the monocell (MNC). A monocell (MNC) with high cycle characteristics may have a small degree of deterioration due to charge / discharge, and a monocell (MNC) with low cycle characteristics may have a large degree of deterioration due to charge / discharge.

[0035] The shape of the positive electrode active material may include particle shapes such as a sphere or an ellipsoid, for example. The particle size and content of the positive electrode active material are not particularly limited.

[0036] The solid electrolyte may include a sulfide-based solid electrolyte having excellent lithium ion conductivity characteristics. Examples of the sulfide-based solid electrolyte include Li2S-P2S5, Li2S-P2S5-LiX (X is a halogen element), Li2S-P2S5-Li2O, Li2S-P2S5-Li2O-LiI, Li2S-SiS2, Li2S-SiS2-LiI, Li2S-SiS2-LiBr, Li2S-SiS2-LiCl, Li2S-SiS2-B2S3-LiI, Li2S-SiS2-P2S5-LiI, Li2S-B2S3, Li2S-P2S5-Z. m S n (m, n are positive numbers, capital letter “Z” represents Ge, Zn or Ga), Li2S-GeS2, Li2S-SiS2-Li3PO4, Li2S-SiS2-Li p MO q (p, q are positive numbers, capital letter “M” is one of P, Si, Ge, B, Al, Ga In), Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x It may include at least one selected from (0≤x≤2).

[0037] Sulfide-based solid electrolytes include, for example, Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x(0≤x≤2) may be an argyrodite-type compound including at least one selected from. In particular, the sulfide-based solid electrolyte may be an argyrodite-type compound including at least one 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. Since the argyrodite-type solid electrolyte has a density of 1.5 g / cc or more, the internal resistance of the all-solid-state battery is reduced, and the defect of the solid electrolyte membrane being penetrated and short-circuited due to the formation of lithium dendrites can be prevented. The elastic modulus of the solid electrolyte may be, for example, 15 GPa to 35 GPa.

[0038] The solid electrolyte included in the positive electrode active material layer (120) may have a smaller median particle size (D50) than the solid electrolyte included in the solid electrolyte layer (300). For example, the median particle size (D50) of the solid electrolyte included in the positive electrode active material layer (120) may be 90% or less, 80% or less, 70% or less, 60% or less, 50% or less, 40% or less, 30% or less, or 20% or less of the median particle size (D50) of the solid electrolyte included in the solid electrolyte layer (300). Meanwhile, the median particle size (D50) may be a median diameter measured using a laser particle size distribution meter.

[0039] The positive electrode active material layer (120) may include a conductive material. The conductive material may be conductive without causing chemical changes in the mono-cell (MNC), thereby increasing the conductivity of the positive electrode active material and the solid electrolyte. The conductive material may include a carbon-based material. For example, the conductive material may include one or more selected from graphite, carbon black, acetylene black, carbon nanofibers, and carbon nanotubes.

[0040] The positive electrode active material layer (120) may further include a binder. The binder may include a material for binding the positive electrode active material, solid electrolyte, and conductive material included in the positive electrode active material layer (120) and improving bonding strength with the positive electrode current collector (110). For example, the binder may include polyvinylidene fluoride, styrene butadiene rubber (SBR), polytetrafluoroethylene, polyvinylidene fluoride, vinylidene fluoride / hexafluoropropylene copolymer, polyacrylonitrile, or polymethyl methacrylate.

[0041] When the total amount of the positive electrode active material, the solid electrolyte, the conductive material, and the binder is 100 parts by weight, the positive electrode active material layer (120) may include 85 parts by weight to 92 parts by weight of the positive electrode active material. The positive electrode active material layer (120) may include 0.5 parts by weight to 1.5 parts by weight of the binder.

[0042] Within the positive electrode active material layer (120), the conductive material may be present in an amount of 1 to 50 parts by weight relative to 100 parts by weight of the solid electrolyte. If the conductive material is present in an amount less than 1 part by weight relative to 100 parts by weight of the solid electrolyte, the electrical conductivity of the positive electrode active material layer (120) may be reduced. If the conductive material is present in an amount greater than 50 parts by weight relative to 100 parts by weight of the solid electrolyte, the conductive material ratio may be excessively high, and thus a covering layer covering the surface of the solid electrolyte may not be properly formed.

[0043] According to embodiments, the positive electrode active material layer (120) may further include at least one additive selected from the group consisting of a filler, a coating agent, a dispersant, and an ion conductive auxiliary agent in addition to the above-described positive electrode active material, solid electrolyte, conductive agent, and binder.

[0044] The solid electrolyte layer (300) is disposed between the positive electrode layer (100) and the negative electrode layer (200) and may include a sulfide-based solid electrolyte having excellent lithium ion conductivity characteristics. The solid electrolyte included in the solid electrolyte layer (300) may be the same as or different from any one of the materials that may be included in the solid electrolyte included in the positive electrode active material layer (120) described above.

[0045] The solid electrolyte layer (300) of one embodiment may include a sulfide-based solid electrolyte. The sulfide-based solid electrolyte may be manufactured by treating starting materials such as Li2S and P2S5 by a melting rapid cooling method or a mechanical milling method. In addition, a heat treatment may be performed after the treatment. The solid electrolyte may be amorphous, crystalline, or a mixture thereof. In addition, the solid electrolyte may include, for example, at least sulfur (S), phosphorus (P), and lithium (Li) as constituent elements among the above-described sulfide-based solid electrolyte materials. For example, the solid electrolyte may be a material including Li2S-P2S5. When using a sulfide-based solid electrolyte material including Li2S-P2S5 to form the solid electrolyte, the mixing molar ratio of Li2S and P2S5 is, for example, in the range of Li2S:P2S5=50:50 to 90:10.

[0046] Sulfide-based solid electrolytes include, for example, Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x(0≤x≤2) may be an argyrodite-type compound including at least one selected from. In particular, the sulfide-based solid electrolyte may be an argyrodite-type compound including at least one 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. Since the argyrodite-type solid electrolyte has a density of 1.5 g / cc or more, the internal resistance of the all-solid-state battery is reduced, and the defect of the solid electrolyte membrane being penetrated and short-circuited due to the formation of lithium dendrites can be prevented. The elastic modulus of the solid electrolyte is, for example, 15 GPa to 35 GPa.

[0047] The solid electrolyte layer (300) may further include a binder. The binder in the solid electrolyte layer (300) may be, for example, styrene butadiene rubber (SBR), polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, etc., but is not limited thereto. The binder of the 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).

[0048] The negative electrode layer (200) may include a negative electrode current collector (210) and a negative electrode coating layer (220) on the negative electrode current collector (210). The negative electrode current collector (210) may provide a reference surface on which the negative electrode coating layer (220) is disposed. The negative electrode current collector (210) may include, for example, a material that does not react with lithium, i.e., does not form an alloy or a compound with lithium. For example, the negative electrode current collector (210) may include at least one metal selected from the group consisting of copper (Cu), stainless steel, titanium (Ti), iron (Fe), cobalt (Co), and nickel (Ni). The thickness of the negative electrode current collector (210) may be 1 μm to 20 μm, more specifically 5 μm to 15 μm, and more specifically 7 μm to 10 μm.

[0049] The negative electrode current collector (210) may be composed of one of the above-described metals, or may include an alloy or coating material of two or more metals. The negative electrode current collector (210) may have, for example, a plate shape or a foil shape. Meanwhile, in one embodiment, the negative electrode current collector (210) may be omitted.

[0050] The negative electrode coating layer (220) can allow lithium metal to grow between the negative electrode current collector (210) and the monocell (MNC) when charging. The negative electrode coating layer (220) can act as a protective layer for the lithium metal and suppress the precipitation and growth of lithium dendrites.

[0051] The cathode coating layer (220) may include a metal and carbon. For example, the cathode coating layer (220) may include at least one metal selected from the group consisting of gold (Au), platinum (Pt), palladium (Pd), silicon (Si), silver (Ag), aluminum (Al), bismuth (Bi), tin (Sn), and zinc (Zn). The cathode coating layer (220) may include at least one carbon selected from the group consisting of carbon black, acetylene black, furnace black, ketjen black, and graphene. In one embodiment, the cathode coating layer (220) may include a mixture of carbon black and silver (Ag).

[0052] The cathode coating layer (220) may further include additives other than metal and carbon. The cathode coating layer (220) may further include, for example, at least one additive selected from the group consisting of a binder, a filler, a coating agent, a dispersant, and an ion conductive additive.

[0053] The negative electrode coating layer (220) may have a smaller thickness than the positive electrode active material layer (120). The thickness of the negative electrode coating layer (220) may be, for example, 50% or less, 40% or less, 30% or less, 20% or less, 10% or less, or 5% or less of the thickness of the positive electrode active material layer (120). The thickness of the negative electrode coating layer (220) may be, for example, 1 um to 20 um, 2 um to 10 um, or 3 um to 7 um. If the thickness of the negative electrode coating layer (220) is too thin, lithium dendrites formed between the negative electrode coating layer (220) and the negative electrode current collector (210) may collapse the negative electrode coating layer (220), thereby deteriorating the cycle characteristics of the monocell (MNC). If the thickness of the cathode coating layer (220) increases excessively, the energy density of the monocell (MNC) may decrease and the internal resistance of the monocell (MNC) due to the cathode coating layer (220) may increase, thereby deteriorating the cycle characteristics of the monocell (MNC).

[0054] Meanwhile, although not shown, a carbon layer may be further included to improve adhesion between the cathode coating layer (220) and the solid electrolyte layer (300).

[0055] According to embodiments of the present invention, the width (or width) of the anode layer (100) may be smaller than the width (or width) of the cathode layer (200). For example, the anode layer (100) may have a first width (W1) in a first direction (D1), and the cathode layer (200) may have a second width (W2) in the first direction (D1). The first width (W1) may be smaller than the second width (W2).

[0056] According to embodiments of the present invention, the solid electrolyte layer (300) may include a positive electrode electrolyte layer (300a) and a negative electrode electrolyte layer (300b). The positive electrode electrolyte layer (300a) and the negative electrode electrolyte layer (300b) may be laminated to form a single solid electrolyte layer (300). The positive electrode electrolyte layer (300a) may be in contact with the positive electrode active material layer (120), and the negative electrode electrolyte layer (300b) may be in contact with the negative electrode coating layer (220).

[0057] For example, the positive electrode electrolyte layer (300a) and the negative electrode electrolyte layer (300b) may include solid electrolytes having the same composition. As another example, the positive electrode electrolyte layer (300a) and the negative electrode electrolyte layer (300b) may include solid electrolytes having different compositions.

[0058] The positive electrode electrolyte layer (300a) may have a first width (W1), and the negative electrode electrolyte layer (300b) may have a second width (W2). In other words, the width (or width) of the positive electrode electrolyte layer (300a) may be smaller than the width (or width) of the negative electrode electrolyte layer (300b).

[0059] Referring to FIG. 2, a bi-cell (BIC) of an all-solid-state battery according to one embodiment of the present invention is illustrated. The bi-cell (BIC) may include a first cathode layer (201), a second cathode layer (205), and a cathode layer (100) sandwiched between the first and second cathode layers (201, 205).

[0060] Each of the first and second negative electrode layers (201, 205) may include a negative electrode current collector (210), a negative electrode coating layer (220) on the negative electrode current collector (210), and a negative electrode electrolyte layer (300b) on the negative electrode coating layer (220). The negative electrode current collector (210) and the negative electrode coating layer (220) may be the same as the negative electrode current collector (210) and the negative electrode current collector (210), respectively, described above with reference to FIG. 1. The negative electrode electrolyte layer (300b) may be the same as the solid electrolyte layer (300) described above with reference to FIG. 1. The negative electrode electrolyte layer (300b) may be in direct contact with the negative electrode coating layer (220).

[0061] The positive electrode layer (100) may include a first positive electrode active material layer (120a), a second positive electrode active material layer (120b), and a positive electrode current collector (110) interposed between the first and second positive electrode active material layers (120a, 120b). Each of the first and second positive electrode active material layers (120a, 120b) may have the same composition or different compositions.

[0062] The positive electrode layer (100) may further include a positive electrode electrolyte layer (300a) provided on each of the first and second positive electrode active material layers (120a, 120b). In one embodiment, the positive electrode layer (100) may include a pair of positive electrode electrolyte layers (300a). The first and second positive electrode active material layers (120a, 120b) may be sandwiched between the pair of positive electrode electrolyte layers (300a). One of the pair of positive electrode electrolyte layers (300a) may be in contact with the first positive electrode active material layer (120a). The other of the pair of positive electrode electrolyte layers (300a) may be in contact with the second positive electrode active material layer (120b). The positive electrode electrolyte layer (300a) may be the same as the solid electrolyte layer (300) described above with reference to FIG. 1.

[0063] The positive and negative electrolyte layers (300a, 300b) interposed between the first positive active material layer (120a) and the negative coating layer (220) of the first negative electrode layer (201) can constitute a first solid electrolyte layer (301). The positive and negative electrolyte layers (300a, 300b) interposed between the second positive active material layer (120b) and the negative coating layer (220) of the second negative electrode layer (205) can constitute a second solid electrolyte layer (305).

[0064] According to some embodiments, the anode layer (100) may have a first width (W1), and each of the first and second cathode layers (201, 205) may have a second width (W2). The first width (W1) may be smaller than the second width (W2). Since the width of the anode layer (100) is smaller than the width of each of the first and second cathode layers (201, 205), a gasket may be further provided around the periphery of the anode layer (100) to compensate for this.

[0065]

[0066] FIG. 3 is a plan view illustrating a stacking device for an all-solid-state battery according to embodiments of the present invention. Referring to FIG. 3, the stacking device may include a first input unit (ISU1), a second input unit (ISU2), a third input unit (ISU3), and a stacking table (STT). The stacking device may further include a first discharge gripper (EGR1), a pressing unit (SHP), a second discharge gripper (EGR2), a defective discharge unit (NGE), a taping unit (TPU), and a battery discharge unit (ETR).

[0067] The first to third input units (ISU1-ISU3) may be sequentially arranged counterclockwise around the perimeter of the stacking table (STT). The first input unit (ISU1) may include a first magazine unit (MAG1), a first transfer unit (TFU1), and a first alignment unit (ALU1). A plurality of first sheets may be loaded into the first magazine unit (MAG1). The first magazine unit (MAG1) may be configured to sequentially supply the plurality of first sheets.

[0068] The first transfer unit (TFU1) may be configured to transfer the first sheet supplied from the first magazine unit (MAG1) onto the first alignment unit (ALU1). For example, the first transfer unit (TFU1) may have the form of a robot arm capable of gripping and transferring the first sheet.

[0069] The first alignment unit (ALU1) may be configured to measure the alignment of the first sheet transferred via the first transfer unit (TFU1). For example, the first alignment unit (ALU1) may inspect the alignment of the first sheet via vision. Through the first alignment unit (ALU1), the first sheet may be accurately aligned on the stage (STG) of the stacking table (STT) described below.

[0070] The second input unit (ISU2) may include a second magazine unit (MAG2), a second transfer unit (TFU2), and a second alignment unit (ALU2). A plurality of second sheets may be loaded into the second magazine unit (MAG2). The second magazine unit (MAG2) may be configured to sequentially supply the plurality of second sheets. The second transfer unit (TFU2) may be configured to transport the second sheets supplied from the second magazine unit (MAG2) onto the second alignment unit (ALU2). The second alignment unit (ALU2) may be configured to measure the alignment of the second sheets transported through the second transfer unit (TFU2).

[0071] The third input unit (ISU3) may include a third magazine unit (MAG3), a third transfer unit (TFU3), an inversion unit (IVU), and a third alignment unit (ALU3). A plurality of third sheets may be loaded into the third magazine unit (MAG3). The third magazine unit (MAG3) may be configured to sequentially supply the plurality of third sheets. The third transfer unit (TFU3) may be configured to transport the third sheets supplied from the third magazine unit (MAG3) onto the third alignment unit (ALU3). The inversion unit (IVU) may be configured to vertically invert the third sheets transported by the third transfer unit (TFU3). In other words, the third sheets may be flipped over by the inversion unit (IVU). The third alignment unit (ALU3) may be configured to measure the alignment of the inverted third sheets.

[0072] The stacking table (STT) may include a stage (STG) and a rotation unit (DRU). The stage (STG) may be connected to the rotation unit (DRU) and may rotate 360 ​​degrees. For example, the rotation unit (DRU) may be configured to rotate the stage (STG) counterclockwise. The rotation unit (DRU) may have the form of a rotatable index table. For example, the rotation unit (DRU) may include a rotation plate and a motor for driving the rotation plate.

[0073] The stage (STG) can be sequentially moved to first to eighth positions (PO1-PO8) by the rotation unit (DRU). Specifically, a first sheet supplied from the first input unit (ISU1) can be stacked on the stage (STG) at the first position (PO1). An alignment inspection between the first sheet and the stage (STG) can be performed on the stage (STG) that has moved to the second position (PO2).

[0074] The stage (STG) can be moved from the second position (PO2) to the third position (PO3). A second sheet supplied from the second input unit (ISU2) can be stacked on the stage (STG) at the third position (PO3). The second sheet can be stacked on the first sheet. An alignment inspection between the second sheet and the stage (STG) can be performed on the stage (STG) that has moved to the fourth position (PO4).

[0075] The stage (STG) can be moved from the fourth position (PO4) to the fifth position (PO5). On the stage (STG) at the fifth position (PO5), an inverted third sheet supplied from the third input unit (ISU3) can be stacked. The inverted third sheet can be stacked on the second sheet. On the stage (STG) moved to the sixth position (PO6), an alignment inspection between the third sheet and the stage (STG) can be performed.

[0076] The stage (STG) can move from the sixth position (PO6) to the seventh position (PO7). At the seventh position (PO7), the stack on the stage (STG) can move onto the first discharge gripper (EGR1).

[0077] The first discharge gripper (EGR1) may be configured to transfer the laminate received from the stacking table (STT) to the pressing unit (SHP). The first discharge gripper (EGR1) may be configured to transfer the laminate discharged from the pressing unit (SHP) to the second discharge gripper (EGR2). The first discharge gripper (EGR1) may rotate clockwise or counterclockwise while holding the laminate.

[0078] The pressing unit (SHP) can be configured to pressurize the laminate received from the first discharge gripper (EGR1). The pressing unit (SHP) can pressurize the laminate using surface pressure. The pressing unit (SHP) can be configured to perform a heating process simultaneously when pressing the laminate. In other words, the pressing unit (SHP) can perform both a pressing and a heating process. For example, the pressing unit (SHP) can utilize a hydraulic method or a servo motor method. The pressing unit (SHP) can discharge the laminate, after pressing, back to the first discharge gripper (EGR1).

[0079] The second discharge gripper (EGR2) can be configured to transfer the pressurized laminate received from the first discharge gripper (EGR1) to a taping unit (TPU) or a defect discharge unit (NGE). The second discharge gripper (EGR2) can rotate clockwise or counterclockwise while holding the laminate. If there is a defect in the laminate, the second discharge gripper (EGR2) can discharge the laminate to the defect discharge unit (NGE). If there is no defect in the laminate, the second discharge gripper (EGR2) can transfer the laminate to the taping unit (TPU).

[0080] The taping unit (TPU) may be configured to tape the laminate received from the second discharge gripper (EGR2). The taping unit (TPU) may rotate the laminate and wrap the tape around the laminate.

[0081] The taped laminate can be discharged from the taping unit (TPU) to the ejection tray (ETR). The ejection tray (ETR) can include a tray on which the laminate can be loaded. An all-solid-state battery can be manufactured using the laminate loaded into the ejection tray (ETR).

[0082]

[0083] Figures 4 to 8 are cross-sectional views illustrating a method for manufacturing an all-solid-state battery according to embodiments of the present invention. In this embodiment, a method for manufacturing an all-solid-state battery using the laminating device of Figure 3 described above is described.

[0084] Referring to FIGS. 3 and 4, an elastic pad (ELP) may be provided on the stage (STG) at the first position (PO1). The elastic pad (ELP) may correspond to a first sheet supplied through the first input unit (ISU1).

[0085] An elastic pad (ELP) can relieve stress generated due to volume changes in a battery cell during charge and discharge. The elastic pad (ELP) can be composed of elastically deformable members. The elastic pad (ELP) can include a material having a lower elastic modulus than the positive and negative current collectors. The elastic pad (ELP) can include an insulating material. For example, the material of the elastic pad (ELP) can be selected from the group consisting of epoxy resin, acrylic resin, polyimide resin, polyester resin, polypropylene resin, polyamide resin, polystyrene resin, polyvinyl chloride resin, polycarbonate resin, fluororesin such as PTFE, and silicone rubber.

[0086] Referring to FIGS. 3 and 5, a first monocell (MNC1) may be provided on a stage (STG) at a third position (PO3). The first monocell (MNC1) may be aligned and stacked on an elastic pad (ELP). The first monocell (MNC1) may correspond to a second sheet supplied through a second input unit (ISU2). The first monocell (MNC1) may be substantially the same as the monocell (MNC) described above with reference to FIG. 1. The cathode layer (200) of the first monocell (MNC1) may be in direct contact with the elastic pad (ELP). The anode layer (100) of the first monocell (MNC1) may be exposed upward.

[0087] Referring to FIGS. 3 and 6, a second monocell (MNC2) may be provided on the stage (STG) at the fifth position (PO5). The second monocell (MNC2) may be provided in an inverted state with the anode layer (100) facing downward. The second monocell (MNC2) may be aligned and stacked on the first monocell (MNC1). The second monocell (MNC2) may correspond to an inverted third sheet supplied through the third input unit (ISU3). The second monocell (MNC2) may be substantially the same as the monocell (MNC) described above with reference to FIG. 1. The anode layer (100) of the second monocell (MNC2) may be in direct contact with the anode layer (100) of the first monocell (MNC1). The cathode layer (200) of the second monocell (MNC2) may be exposed upward.

[0088] Referring to FIGS. 3 and 7, the lamination process described above with reference to FIGS. 4 to 6 may be repeatedly performed while the stage (STG) rotates by the rotation unit (DRU). The lamination process may be performed n times. n may be an integer greater than or equal to 1. By performing the lamination process n times, a laminate (STS) may be formed on the stage (STG) at the seventh position (PO7).

[0089] In one embodiment, the stack (STS) may include a first monocell (MNC1), a second monocell (MNC2), a third monocell (MNC3), a fourth monocell (MNC4), ... a 2n-1 monocell (MNC2n-1) and a 2n-th monocell (MNC2n). n may be an integer greater than or equal to 3. The stack (STS) may further include a plurality of elastic pads (ELP). Two monocells (MNC) may be sandwiched between adjacent elastic pads (ELP).

[0090] Referring to FIGS. 3 and 8, the laminate (STS) on the stage (STG) at the seventh position (PO7) can be transferred to the pressing unit (SHP) via the first discharge gripper (EGR1). A pressurizing and heating process can be performed on the laminate (STS) within the pressing unit (SHP). In one embodiment, the interface between the positive electrolyte layer (300a) and the negative electrolyte layer (300b) within the laminate (STS) can be activated by the pressurizing and heating process.

[0091] According to embodiments of the present invention, rather than performing the pressurizing and heating processes on each of the monocells (MNC), a single pressurizing and heating process can be performed on a plurality of stacked monocells (MNC). This can improve the efficiency of the manufacturing process of the all-solid-state battery.

[0092] The pressurized laminate (STS) can be transferred to the taping unit (TPU) via the second discharge gripper (EGR2). A taping process can be performed on the laminate (STS) within the taping unit (TPU). The laminate (STS) after taping can be loaded into the battery discharge unit (ETR).

[0093]

[0094] FIG. 9 is a plan view illustrating another embodiment of the first input unit of the stacking device of FIG. 3. Referring to FIGS. 3 and 9, the first input unit (ISU1) may further include a fourth magazine unit (MAG4). A plurality of fourth sheets may be loaded into the fourth magazine unit (MAG4). The fourth magazine unit (MAG4) may be configured to sequentially supply the plurality of fourth sheets. The first transfer unit (TFU1) may be configured to transfer the fourth sheets supplied from the fourth magazine unit (MAG4) onto the first alignment unit (ALU1). The first alignment unit (ALU1) may be configured to measure the alignment of the fourth sheets transferred through the first transfer unit (TFU1).

[0095] The first input unit (ISU1) can sequentially stack the first sheet and the fourth sheet on the stage (STG) at the first position (PO1).

[0096]

[0097] Figures 10 to 15 are cross-sectional views illustrating a method for manufacturing an all-solid-state battery according to embodiments of the present invention. In this embodiment, a method for manufacturing an all-solid-state battery using the laminating device of Figures 3 and 9 described above is described.

[0098] Referring to FIGS. 3, 9, and 10, an elastic pad (ELP) may be provided on the stage (STG) of the first position (PO1). The elastic pad (ELP) may correspond to a first sheet supplied through the first input unit (ISU1). Specifically, the elastic pad (ELP) may be supplied through the first magazine unit (MAG1) of the first input unit (ISU1). The elastic pad (ELP) may alleviate stress generated due to volume change of the battery cell during charging and discharging.

[0099] Referring to FIGS. 3, 9, and 11, a first cathode layer (201) may be provided on a stage (STG) at a first position (PO1). The first cathode layer (201) may be aligned and laminated on an elastic pad (ELP). The first cathode layer (201) may correspond to a fourth sheet supplied through the first input unit (ISU1). Specifically, the first cathode layer (201) may be supplied through the fourth magazine unit (MAG4) of the first input unit (ISU1).

[0100] The first negative electrode layer (201) may be substantially the same as the first negative electrode layer (201) described above with reference to FIG. 2. The first negative electrode layer (201) may include a negative electrode current collector (210), a negative electrode coating layer (220), and a negative electrode electrolyte layer (300b) that are sequentially laminated. In one embodiment of the present invention, the first negative electrode layer (201) prepared in the fourth magazine unit (MAG4) may be prepared by sequentially coating a negative electrode coating layer (220) and a negative electrode electrolyte layer (300b) on the negative electrode current collector (210) and then pressing the same. The pressing process of the first negative electrode layer (201) may be performed at a lower pressure than the pressing process to be performed in the pressing unit (SHP) described later.

[0101] Referring to FIGS. 3 and 12, an anode layer (100) may be provided on a stage (STG) at a third position (PO3). The anode layer (100) may be aligned and laminated on a first cathode layer (201). The anode layer (100) may correspond to a second sheet supplied through a second input unit (ISU2).

[0102] The positive electrode layer (100) may be substantially the same as the positive electrode layer (100) described above with reference to FIG. 2. The positive electrode layer (100) may include a positive electrode electrolyte layer (300a), a first positive electrode active material layer (120a), a positive electrode current collector (110), a second positive electrode active material layer (120b), and a positive electrode electrolyte layer (300a) that are sequentially laminated. In one embodiment of the present invention, the positive electrode layer (100) prepared in the second magazine unit (MAG2) may be prepared by sequentially coating positive electrode active material layers (120a, 120b) and positive electrode electrolyte layers (300a) on both sides of an anode current collector (210), and then pressing them. The pressing process of the positive electrode layer (100) may be performed at a lower pressure than the pressing process to be performed in a pressing unit (SHP) to be described later.

[0103] Referring to FIGS. 3 and 13, a second cathode layer (205) may be provided on the stage (STG) at the fifth position (PO5). The second cathode layer (205) may be provided in an inverted state with the cathode electrolyte layer (300b) facing downward. The second cathode layer (205) may be aligned and laminated on the anode layer (100). The second cathode layer (205) may correspond to an inverted third sheet supplied through the third input unit (ISU3).

[0104] The second negative electrode layer (205) may be substantially the same as the second negative electrode layer (205) described above with reference to FIG. 2. The second negative electrode layer (205) may include a negative electrode electrolyte layer (300b), a negative electrode coating layer (220), and a negative electrode current collector (210) that are sequentially laminated. In one embodiment of the present invention, the second negative electrode layer (205) prepared in the third magazine unit (MAG3) may be prepared by sequentially coating the negative electrode coating layer (220) and the negative electrode electrolyte layer (300b) on the negative electrode current collector (210), and then pressing the same. The pressing process of the second negative electrode layer (205) may be performed at a lower pressure than the pressing process to be performed in the pressing unit (SHP) described later.

[0105] A first cathode layer (201), a positive electrode layer (100), and a second cathode layer (205) sequentially laminated on an elastic pad (ELP) can constitute a first bi-cell (BIC1). The first bi-cell (BIC1) can include a first solid electrolyte layer (301) and a second solid electrolyte layer (305).

[0106] Referring to FIGS. 3 and 14, the lamination process described above with reference to FIGS. 10 to 13 may be repeatedly performed while the stage (STG) rotates by the rotation unit (DRU). The lamination process may be performed n times. n may be an integer greater than or equal to 1. By performing the lamination process n times, a laminate (STS) may be formed on the stage (STG) at the seventh position (PO7).

[0107] In one embodiment, the stack (STS) may include a first bicell (BIC1), a second bicell (BIC2), ..., n-th bicell (BICn). n may be an integer greater than or equal to 3. The stack (STS) may further include a plurality of elastic pads (ELP). A single bicell (BIC) may be sandwiched between adjacent elastic pads (ELP).

[0108] Referring to FIGS. 3 and 15, the laminate (STS) on the stage (STG) at the seventh position (PO7) can be transferred to the pressing unit (SHP) via the first discharge gripper (EGR1). A pressurizing and heating process can be performed on the laminate (STS) within the pressing unit (SHP). In one embodiment, the interface between the positive electrolyte layer (300a) and the negative electrolyte layer (300b) within the laminate (STS) can be activated by the pressurizing and heating process.

[0109] According to embodiments of the present invention, rather than performing the pressurizing and heating processes on each of the bi-cells (BIC), a single pressurizing and heating process can be performed on a plurality of stacked bi-cells (BIC). This can improve the efficiency of the manufacturing process of the all-solid-state battery.

[0110] The pressurized laminate (STS) can be transferred to the taping unit (TPU) via the second discharge gripper (EGR2). A taping process can be performed on the laminate (STS) within the taping unit (TPU). The laminate (STS) after taping can be loaded into the battery discharge unit (ETR).

[0111]

[0112] While embodiments of the present invention have been described with reference to the attached drawings, the present invention may be implemented in other specific forms without altering the technical spirit or essential features thereof. Therefore, it should be understood that the embodiments described above are exemplary in all respects and are not limiting.

Claims

1. A stacking table including a stage and a rotation unit, wherein the rotation unit is configured to cycle through a first position, a second position, a third position, and a fourth position while the stage rotates; A first input unit adjacent to the first position, the first input unit being configured to stack a first sheet on the stage; A second input unit adjacent to the second position, the second input unit being configured to stack a second sheet on the stage; A third input unit adjacent to the third position, the third input unit being configured to stack a third sheet on the stage; a first discharge gripper adjacent to the fourth position; and Including a pressing unit adjacent to the first discharge gripper, The first discharge gripper is configured to transfer a laminate including the first to third sheets from the stage to the pressing unit, The above pressing unit is a laminate device configured to perform a pressing process on the laminate.

2. In paragraph 1, The above first input unit: A first magazine unit configured to supply the first sheet; A first transfer device configured to transfer the first sheet; and A stacking device comprising a first alignment unit for checking the alignment of the first sheet.

3. In paragraph 2, A stacking device wherein the first input unit further comprises a fourth magazine unit configured to supply a fourth sheet.

4. In paragraph 3, The first sheet above includes an elastic pad, The fourth sheet above includes a first cathode layer, The second sheet includes a positive electrode layer, The third sheet is a laminated device including a second cathode layer.

5. In paragraph 1, The above second input unit: A second magazine unit configured to supply the second sheet; A second transfer device configured to transfer the second sheet; and A stacking device comprising a second alignment unit for checking the alignment of the second sheet.

6. In paragraph 1, The above third input unit: A third magazine unit configured to supply the third sheet; A third transfer device configured to transfer the third sheet; A reverser for reversing the third sheet; and A stacking device including a third alignment unit for checking the alignment of the inverted third sheet.

7. In paragraph 1, A second discharge gripper adjacent to the first discharge gripper; A defective discharge unit that receives a defective laminate from the second discharge gripper; and A laminating device further comprising a taping unit for receiving a good laminate from the second discharge gripper.

8. In paragraph 1, The above pressing unit is a laminate device configured to perform a heating process while the pressing process is performed on the laminate.

9. In paragraph 1, The first sheet above includes an elastic pad, The second sheet above includes the first monocell, The third sheet is a laminated device including a second monocell.

10. In paragraph 9, Each of the first and second monocells: A cathode layer comprising a cathode current collector and a cathode coating layer on the cathode current collector; A cathode layer including a cathode current collector and a cathode active material layer on the cathode current collector; and A laminated device comprising a solid electrolyte layer sandwiched between the cathode layer and the anode layer.

11. Stacking the first sheet on the stage at the first position; Laminating a second sheet on the stage at the second position; Laminating a third sheet on the stage at the third position; and Including performing a pressurizing process on a laminate including the first to third sheets, A method for manufacturing an all-solid-state battery, wherein the stage rotates and cycles through the first position, the second position, and the third position.

12. In paragraph 11, The first sheet above includes an elastic pad, The second sheet above includes the first monocell, A method for manufacturing an all-solid-state battery, wherein the third sheet comprises a second monocell.

13. In paragraph 12, Each of the first and second monocells: A cathode layer comprising a cathode current collector and a cathode coating layer on the cathode current collector; A cathode layer including a cathode current collector and a cathode active material layer on the cathode current collector; and A method for manufacturing an all-solid-state battery, comprising a solid electrolyte layer sandwiched between the cathode layer and the anode layer.

14. In paragraph 11, Further comprising laminating a fourth sheet on the stage at the first position, A method for manufacturing an all-solid-state battery, wherein the fourth sheet is laminated on the first sheet.

15. In paragraph 14, The first sheet above includes an elastic pad, The fourth sheet above includes a first cathode layer, The second sheet includes a positive electrode layer, A method for manufacturing an all-solid-state battery, wherein the third sheet includes a second cathode layer.

16. In paragraph 15, Preparing each of the first and second cathode layers: Sequentially coating a cathode coating layer and a cathode electrolyte layer on a cathode current collector; and A method for manufacturing an all-solid-state battery, comprising performing a pressurizing process on the negative electrode current collector, the negative electrode coating layer, and the negative electrode electrolyte layer.

17. In paragraph 15, Preparing the above bipolar layer: Sequentially coating a first positive electrode active material layer and a first positive electrode electrolyte layer on the first surface of the positive electrode current collector; Sequentially coating a second positive electrode active material layer and a second positive electrode electrolyte layer on the second surface of the positive electrode current collector; and A method for manufacturing an all-solid-state battery, comprising performing a pressurizing process on the second positive electrode electrolyte layer, the second positive electrode active material layer, the positive electrode current collector, the first positive electrode active material layer, and the first positive electrode electrolyte layer.

18. In paragraph 11, A method for manufacturing an all-solid-state battery, further comprising performing a heating process while performing a pressurizing process on the laminate.

19. In paragraph 11, The stage is configured such that the first to third sheets are stacked n times while the first to third positions are cycled n times, A method for manufacturing an all-solid-state battery, wherein n is an integer greater than or equal to 3.

20. In paragraph 11, A method for manufacturing an all-solid-state battery, further comprising performing a taping process on the pressurized laminate.

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