All-solid-state battery and method for manufacturing same
Patent Information
- Authority / Receiving Office
- WO · WO
- Patent Type
- Applications
- Current Assignee / Owner
- SAMSUNG SDI CO LTD
- Filing Date
- 2025-03-10
- Publication Date
- 2026-07-30
Smart Images

Figure KR2025003084_30072026_PF_FP_ABST
Abstract
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] 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.
[0003] Meanwhile, currently commercially available lithium secondary batteries use electrolytes containing flammable organic dispersion media, which can lead to fires or explosions due to overheating caused by external short circuits. To address this problem, interest in all-solid-state batteries, which replace the liquid electrolyte with a solid electrolyte, is growing. Since all-solid-state batteries do not use flammable organic dispersion media, they can reduce the likelihood of fire or explosion compared to lithium-ion batteries that use liquid electrolytes, even if an external short circuit occurs.
[0004] The problem that the present invention aims to solve is to provide an all-solid-state battery having excellent safety.
[0005] A solid-state battery according to one embodiment of the present invention comprises: an electrode assembly including at least one unit cell; a substrate tab extending from the unit cell; a gasket disposed on one side of the electrode assembly and configured to surround the substrate tab; and an outer casing that accommodates the electrode assembly, wherein the substrate tab includes a bending portion A extending at an angle from the unit cell and a tab assembly portion formed by the bending portion A being joined together, and the gasket surrounds the bending portion A, and the corner of the gasket contacts the outer casing.
[0006] A solid-state battery according to another embodiment of the present invention comprises: an electrode assembly including at least one unit cell; a substrate tab extending from the unit cell; a gasket disposed on one side of the electrode assembly and configured to surround the substrate tab; and an outer casing for housing the electrode assembly, wherein the substrate tab includes a connecting portion adjacent to the unit cell and a bending portion B extending at an angle from the connecting portion, and the gasket surrounds the connecting portion.
[0007] A method for manufacturing an all-solid-state battery according to another embodiment of the present invention comprises the steps of: manufacturing an electrode assembly comprising at least one unit cell and a substrate tab extending from the unit cell; manufacturing a gasket having an opening; and placing the gasket on one side of the electrode assembly, wherein the step of bending the substrate tab and forming a tab assembly may be performed before or after the step of placing the gasket.
[0008] An all-solid-state battery according to one embodiment of the present invention has excellent safety because, by placing a gasket on one side of an electrode assembly comprising at least one unit cell, the substrate tab extending from the unit cell and the outer material are separated through the gasket, thereby effectively preventing a short circuit from occurring.
[0009] In addition, an all-solid-state battery according to another embodiment of the present invention has excellent safety because, by placing a gasket on one side of an electrode assembly comprising at least one unit cell, the unit cell can be protected from the outside, and at the same time, internal short circuits or short circuits caused by foreign substances that may occur during the manufacturing process can be effectively prevented.
[0010] FIG. 1 is a cross-sectional view of a unit cell of an all-solid-state battery according to one embodiment of the present invention.
[0011] FIGS. 2 and FIGS. 3 are cross-sectional views of a unit cell according to another embodiment of the present invention.
[0012] FIG. 4 shows a pouch-type all-solid-state battery according to one embodiment of the present invention.
[0013] FIG. 5 is a cross-sectional view along the line AA' of FIG. 4, schematically illustrating a cross-section of a pouch-type all-solid-state battery without a gasket according to one embodiment of the present invention.
[0014] FIG. 6 is a cross-sectional view along the line AA' of FIG. 4, schematically illustrating a cross-section of a pouch-type all-solid-state battery according to one embodiment of the present invention.
[0015] FIG. 7 is a cross-sectional view along the line AA' of FIG. 4, schematically illustrating a cross-section of a pouch-type all-solid-state battery according to another embodiment of the present invention.
[0016] FIG. 8 is a cross-sectional view according to the first direction of a gasket according to one embodiment of the present invention.
[0017] FIG. 9 is a cross-sectional view along the first direction of a gasket according to another embodiment of the present invention.
[0018] FIG. 10 is a cross-sectional view according to a second direction of a gasket according to one embodiment of the present invention.
[0019] FIG. 11 is a cross-sectional view along a second direction of a gasket according to another embodiment of the present invention.
[0020] FIG. 12 shows a schematic flowchart of a method for manufacturing an all-solid-state battery according to another embodiment of the present invention.
[0021] FIG. 13 is a schematic diagram of the steps for manufacturing an all-solid-state battery according to another embodiment of the present invention.
[0022] FIG. 14 is a cross-sectional view along the line AA' of FIG. 4, schematically illustrating a cross-section of a pouch-type all-solid-state battery according to another embodiment of the present invention.
[0023] Figure 15 is a schematic cross-sectional view showing an enlarged view of the M region of Figure 14.
[0024] FIG. 16 is a schematic cross-sectional view illustrating a gasket according to another embodiment of the present invention.
[0025] FIG. 17 is a schematic cross-sectional view illustrating a gasket according to another embodiment of the present invention.
[0026] FIG. 18 is a cross-sectional view of a gasket according to another embodiment of the present invention.
[0027] FIG. 19 is a cross-sectional view of a gasket according to another embodiment of the present invention.
[0028] FIG. 20 shows a schematic flowchart of a method for manufacturing an all-solid-state battery according to another embodiment of the present invention.
[0029] FIG. 21 is a schematic diagram of the steps for manufacturing an all-solid-state battery according to another embodiment of the present invention.
[0030] FIG. 22 confirms the occurrence of a short circuit according to the evaluation example for the all-solid-state batteries of Example 2-1 and Comparative Example 2-1.
[0031] [Explanation of the symbol]
[0032] 1: Unit cell 10: Electrode assembly
[0033] 20: Pouch-type all-solid-state battery 100: Cathode
[0034] 110: Positive current collector 120: Positive active material layer
[0035] 200: Cathode 210: Cathode current collector
[0036] 220: Coating layer 300: Solid electrolyte layer
[0037] 400: Elastic layer 500: Gasket
[0038] 510: Vertical extension 511: First vertical extension
[0039] 512: Second vertical extension 520: Horizontal extension
[0040] 521: 1st horizontal extension 522: 2nd horizontal extension
[0041] 523: 3rd horizontal extension 524: 4th horizontal extension
[0042] 530: Opening 531: First opening
[0043] 532: Second opening 533: Third opening
[0044] 534: 4th opening PCH: Pouch
[0045] TB1: Anode tab TB1a: Connection part
[0046] TB1b: Banding section A or Banding section B TB1c: Positive tab assembly
[0047] TB2: Cathode lead tab LTB1: Anode lead tab
[0048] LTB2: Negative lead tab
[0049] 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.
[0050] 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.
[0051] The embodiments described herein will be explained with reference to cross-sectional and / or plan views, which are exemplary illustrations of the invention. In the drawings, the thicknesses of the films and regions are exaggerated for effective explanation 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.
[0052] In the various embodiments of this specification, terms such as first, second, primary, secondary, etc., have been used to describe various components, but 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.
[0053] All numbers and expressions indicating the amounts of components, reaction conditions, etc. described in this specification should be understood as being modified by the term "about" in all cases unless otherwise specified.
[0054] The terms used herein are for describing the embodiments and are not intended to limit the invention. In this specification, the singular form includes the plural form unless specifically stated otherwise in the text. As used herein, 'comprises' and / or 'comprising' do not exclude the presence or addition of one or more other components to the mentioned components.
[0055] 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.
[0056] In this specification, “metal” includes both metals and metalloids such as silicon and germanium in an elemental or ionic state, and “alloy” means a mixture of two or more metals.
[0057] In this specification, “anode active material” refers to an anode material capable of undergoing lithiation and delithiation, and “anode active material” refers to an anode material capable of undergoing lithiation and delithiation.
[0058] In this specification, “lithiation” and “to lithiate” refer to the process of adding lithium to an electrode active material, and “delithiation” and “to delithiate” refer to the process of removing lithium from an electrode active material.
[0059] In this specification, “charge” and “to charge” refer to the process of providing electrochemical energy to a battery, and “discharge” and “to discharge” refer to the process of removing electrochemical energy from a battery.
[0060] In this specification, “positive electrode” refers to an electrode where electrochemical reduction and lithiation occur during the discharge process, and “negative electrode” refers to an electrode where electrochemical oxidation and delithiation occur during the discharge process.
[0061] All-solid-state batteries are manufactured in various shapes, including cylindrical, prismatic, and pouch types. Recently, interest in pouch-type all-solid-state batteries has been growing due to their excellent flexibility, which allows for diverse design forms and enables reductions in weight and volume. However, pouch-type all-solid-state batteries have a problem with poor durability, as they are relatively vulnerable to external physical impact and are susceptible to damage from pressure or deformation.
[0062] An all-solid-state battery may have a structure comprising an electrode assembly in which unit cells including a negative electrode and a positive electrode are stacked, and a substrate tab extending from said unit cells is electrically connected to a lead tab. In this case, an outer casing may seal them, and said outer casing may generally be composed of multiple layers. For example, a pouch-type outer casing may include an outer layer that protects the battery from the outside and provides mechanical strength and durability, a middle layer that prevents the penetration of oxygen or moisture and has high barrier properties, and an inner layer that contacts the interior of the battery and seals the battery cell through heat sealing.
[0063] A fire may occur due to a short circuit resulting from the internal components of the battery coming into contact with the outer casing. To prevent such short circuits, an insulating layer capable of ensuring battery safety is typically placed in the inner layer that contacts the battery's interior. For example, thermoplastic polymers such as polypropylene and polyethylene, which offer excellent electrical insulation performance and thermal sealing capabilities, are primarily used as the insulating layer for pouch outer casings.
[0064] However, polypropylene and polyethylene, which are currently mainly used as insulating layers, have the problem of low melting points. For example, polypropylene begins to be damaged at temperatures above 140°C and may melt away at temperatures above 170°C. Therefore, if the internal temperature of the battery rises due to repeated charging and discharging, the insulating layer of the outer casing may be damaged or lost, potentially causing a short circuit. Furthermore, as the thickness of the outer casing is reduced to accommodate various designs or to ensure excellent flexibility, the possibility of such damage increases. Consequently, research on all-solid-state batteries that can improve safety while ensuring excellent flexibility is continuing.
[0065] An all-solid-state battery according to one embodiment of the present invention can separate a substrate tab extending from a unit cell and an outer casing through a gasket by placing a gasket on one side of an electrode assembly comprising at least one unit cell. More specifically, the gasket can separate the substrate tab and the outer casing by surrounding the substrate tab and the edges of the gasket contacting the outer casing.
[0066] Therefore, it is possible to effectively prevent short circuits within the internal battery configuration, for example, between the substrate tab and the casing, where thermal deformation is most likely to occur. Furthermore, safety can be ensured regardless of the thickness of the casing through a simple process of placing a gasket; since there are no restrictions on the thickness of the casing required to ensure safety, a wider variety of all-solid-state battery designs can be created.
[0067] Meanwhile, in the process of manufacturing all-solid-state batteries, multiple substrate tabs may be assembled and welded, soldered, or brazed to electrically connect them to lead tabs. During this process, metallic foreign substances may be generated, which can lead to internal short circuits or short circuits. Additionally, lithium within the unit cell may melt and precipitate to form lithium dendrites, and internal short circuits or short circuits may occur when these lithium dendrites come into contact with the substrate tabs. Furthermore, while pouch-type all-solid-state batteries offer excellent flexibility, they are relatively vulnerable to external impacts, making the substrate tabs susceptible to pressure, which can lead to internal short circuits. Therefore, research on all-solid-state batteries capable of preventing internal short circuits or short circuits is ongoing.
[0068] An all-solid-state battery according to another embodiment of the present invention has excellent safety because, by placing a gasket on one side of an electrode assembly including a unit cell, the unit cell can be protected from the outside, and at the same time, internal short circuits or short circuits caused by foreign substances that may occur during the manufacturing process can be effectively prevented. More specifically, in the manufacturing process of an all-solid-state battery according to another embodiment of the present invention, a gasket is placed on one side of an electrode assembly to fix a substrate tab extending from the unit cell, and then the substrate tab is bent to form a tab assembly. Accordingly, short circuits or internal short circuits caused by metallic foreign substances that may occur due to processes such as welding to form the tab assembly, or by substances that may melt and precipitate from the unit cell, can be effectively prevented.
[0069]
[0070] All-solid-state battery
[0071] A solid-state battery according to one embodiment of the present invention comprises: an electrode assembly including at least one unit cell; a substrate tab extending from the unit cell; a gasket disposed on one side of the electrode assembly and configured to surround the substrate tab; and an outer casing that accommodates the electrode assembly, wherein the substrate tab includes a bending portion A extending at an angle from the unit cell and a tab assembly portion formed by the bending portion A being joined together, and the gasket surrounds the bending portion A, and the corner of the gasket contacts the outer casing.
[0072] An all-solid-state battery according to one embodiment of the present invention may be of the cylinder type, prismatic type, or pouch type, but is not limited thereto. As a specific example, the all-solid-state battery may be a pouch-type all-solid-state battery.
[0073] For example, pouch-type solid-state batteries are lightweight and flexible, offering excellent performance in terms of energy density and safety, while the pouch can simultaneously protect and isolate the unit cell from the outside. A pouch-type solid-state battery can be used as a single independent unit, or multiple pouch-type solid-state batteries can be combined to form a battery module, or multiple battery modules can be combined to form a battery pack.
[0074] FIG. 4 illustrates a pouch-type all-solid-state battery according to an embodiment of the present invention. Referring to FIG. 4, the pouch-type all-solid-state battery (20) may be in the form of an electrode assembly (10) in which a plurality of unit cells are stacked and packaged in a pouch (PCH), and may include a positive electrode substrate tab (TB1) protruding from a positive electrode (100), a positive electrode lead tab (LTB1) electrically connected to the positive electrode substrate tab (TB1) and protruding outside the pouch, a negative electrode substrate tab (TB2) protruding from a negative electrode (200), and a negative electrode lead tab (LTB2) electrically connected to the negative electrode substrate tab (TB2) and protruding outside the pouch. At this time, the method of electrical connection is not particularly limited, and methods such as welding, soldering, and brazing may be used.
[0075] More specifically, the all-solid-state battery (20) may include a plurality of unit cells (1) and a plurality of substrate tabs (a plurality of TB1 and a plurality of TB2) extending from the plurality of unit cells (1), and the gasket (500) may surround the plurality of substrate tabs (a plurality of TB1 and a plurality of TB2).
[0076] FIG. 5 is a cross-sectional view along the line AA' of FIG. 4, schematically illustrating a cross-section of a pouch-type all-solid-state battery without a gasket according to an embodiment of the present invention. Specifically, it shows a conventional pouch-type all-solid-state battery having a flexible pouch outer material without a gasket according to an embodiment of the present invention. Referring to FIG. 5, the pouch outer material (PCH) surrounds and seals the electrode assembly (10), the positive and negative substrate tabs (LTB1 and LTB2), and a portion of the positive and negative lead tabs (LTB1 and LTB2), and is located in close proximity to the outermost positive and negative substrate tabs (LTB1 and LTB2). In this case, the pouch outer material, particularly the insulating layer which is the inner layer of the pouch outer material, may be damaged by heat generated during repeated charging and discharging of the all-solid-state battery, and thus a short circuit may occur, leading to a fire.
[0077] FIG. 6 is a cross-sectional view along the line AA' of FIG. 4, schematically illustrating a cross-section of a pouch-type all-solid-state battery according to one embodiment of the present invention. Specifically, FIG. 6 illustrates a cross-section of a pouch-type all-solid-state battery (20) comprising a first gasket (501) disposed on one side of an electrode assembly (10) and a second gasket (502) disposed on the other side of an electrode assembly (10). The gasket (500) may include a first gasket (501) surrounding the positive electrode substrate tab (TB1) and a second gasket (502) surrounding the negative electrode substrate tab (TB2).
[0078] More specifically, a pouch-type all-solid-state battery (20) according to one embodiment of the present invention may include an electrode assembly (10) comprising a plurality of unit cells (1), a plurality of substrate tabs (a plurality of TB1s and a plurality of TB2s) extending from the plurality of unit cells (1), and gaskets (501 and 502) disposed on both sides of the electrode assembly (10) and surrounding the substrate tabs. Additionally, each of the plurality of substrate tabs (a plurality of TB1s and a plurality of TB2s) may include a banding portion A (TB1a or TB2a) and a tab assembly portion (TB1b or TB2b) extending at an angle from the unit cells, and the tab assembly portion may be in a form in which the plurality of substrate tabs are gathered together. At this time, the pouch-type all-solid-state battery (20) may include a positive lead tab (LTB1) and a negative lead tab (LTB2) that are electrically connected to the plurality of positive substrate tabs (TB1) and negative substrate tabs (TB2), respectively, and the tab assembly (TB1b or TB2b) may be in a form that can be electrically connected to the positive lead tab (LTB1) and the negative lead tab (LTB2).
[0079] FIG. 7 is a cross-sectional view along the line AA' of FIG. 4, schematically illustrating a cross-section of a pouch-type all-solid-state battery according to another embodiment of the present invention. Specifically, FIG. 7 also illustrates a cross-section of a pouch-type all-solid-state battery (20) including a first gasket (501) disposed on one side of an electrode assembly (10) and a second gasket (502) disposed on the other side of an electrode assembly (10), in the same manner as FIG. 6.
[0080] More specifically, in FIG. 6, the first and second gaskets (501 and 502) are arranged so that they do not come into contact with the electrode assembly (10), and in FIG. 7, the first and second gaskets (501 and 502) are arranged so that they both come into contact with the electrode assembly (10). When the gasket (500) is arranged so that it does not come into contact with the electrode assembly (10) as in FIG. 6, it may be easier to control the distance between the outer material (PCH) and the substrate tab (TB1 or TB2), and when the gasket (500) comes into contact with the electrode assembly (10) as in FIG. 7, the effect of protecting the electrode assembly from the outside may be superior.
[0081] Additionally, FIGS. 6 and 7 illustrate a structure in which a gasket (500) is placed on both one side and the other side of the electrode assembly (10), but it may be placed on only one side or the other side of the electrode assembly (10). Specifically, a pouch-type all-solid-state battery (20) according to one embodiment of the present invention may include a first gasket (501) or a second gasket (502), and may include both the first gasket (501) and the second gasket (502). At this time, the electrode assembly (10) schematically illustrates a structure in which a plurality of unit cells (1) are stacked, and each of the unit cells (1) illustrates a structure in which an elastic layer (400), a positive electrode (100), a solid electrolyte layer (300), and a negative electrode (200) are stacked. Each configuration will be described in detail below.
[0082]
[0083] electrode assembly
[0084] According to another embodiment of the present invention, the all-solid-state battery may include at least one unit cell. More specifically, the all-solid-state battery may include an electrode assembly in which a plurality of unit cells are stacked.
[0085] The above unit cell may include an anode, a solid electrolyte layer, and a cathode. In this specification, the term "unit cell" may refer to a basic unit containing components that constitute a cell.
[0086] FIG. 1 is a cross-sectional view of a unit cell of an all-solid-state battery according to one embodiment of the present invention. Referring to FIG. 1, the unit cell (1) may be a mono cell composed of a positive electrode (100), a negative electrode (200), and a solid electrolyte layer (300) disposed between the positive electrode (100) and the negative electrode (200). More specifically, the unit cell (1) may be a mono cell having a structure in which a negative electrode current collector (210), a coating layer (220), a solid electrolyte layer (300), a positive electrode active material layer (220), and a positive electrode current collector (210) are stacked in order.
[0087] FIGS. 2 and 3 are cross-sectional views of a unit cell according to another embodiment of the present invention.
[0088] Referring to FIG. 2, the unit cell (1) may be a bi-cell composed of a positive electrode (100), a solid electrolyte layer (300), a negative electrode (200), a solid electrolyte layer (300), and a positive electrode (100). More specifically, the unit cell (1) may be a bi-cell in which a positive electrode current collector (110), a positive electrode active material layer (120), a solid electrolyte layer (300), a coating layer (220), a negative electrode current collector (210), a coating layer (220), a solid electrolyte layer (300), a positive electrode active material layer (120), and a positive electrode current collector (110) are stacked in order.
[0089] Referring to FIG. 3, the unit cell (1) may be a bicell composed of a negative electrode (200), a solid electrolyte layer (300), a positive electrode (100), a solid electrolyte layer (300), and a negative electrode (200). More specifically, the unit cell (1) may be a bicell in which a negative electrode current collector (210), a coating layer (220), a solid electrolyte layer (300), a positive electrode active material layer (120), a positive electrode current collector (110), a positive electrode active material layer (120), a solid electrolyte layer (300), a coating layer (220), and a negative electrode current collector (210) are stacked in order.
[0090] The multiple anodes, solid electrolyte layers, and cathodes arranged in Figures 2 and 3 above may each be the same or different.
[0091] The above unit cell (1) may further include an additional functional layer between the anode (100) and the solid electrolyte layer (300), and / or between the cathode (200) and the solid electrolyte layer (300). For example, the above unit cell (1) may further include an additional functional layer, such as an adhesion enhancing layer, between the anode (100) and the solid electrolyte layer (300), and / or between the cathode (200) and the solid electrolyte layer (300), but is not limited thereto.
[0092] Additionally, according to another embodiment of the present invention, the unit cell (1) may further include a lithium metal layer disposed between the negative electrode current collector (210) and the coating layer (220). More specifically, the unit cell (1) may have a structure in which a negative electrode current collector (210), a lithium metal layer, a coating layer (220), a solid electrolyte layer (300), a positive active material layer (120), and a positive current collector (110) are stacked in order.
[0093] The lithium metal layer may include lithium or a lithium alloy. The lithium metal layer is a metal layer containing lithium and can function as a lithium reservoir. For example, the lithium alloy may be a 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., but is not limited thereto. The lithium alloy may be composed of one of the metals described above or may include an alloy of two or more metals.
[0094] Additionally, the lithium metal layer may be a plated layer formed by precipitation between the coating layer (220) and the negative current collector (210) during the charging process.
[0095] For example, the thickness of the lithium metal layer may be 1 μm to 500 μm, 1 μm to 200 μm, 1 μm to 150 μm, 1 μm to 100 μm, or 1 μm to 50 μm. By satisfying the above range, the cycle characteristics of the battery containing the lithium metal layer can be improved without degrading the performance. If the thickness of the lithium metal layer is less than the above range, it cannot sufficiently perform the role of a lithium reservoir, and if it exceeds the above range, the mass and volume of the battery may increase, leading to a decrease in performance and a decrease in cycle characteristics.
[0096] According to another embodiment of the present invention, the lithium metal layer may be provided between the negative current collector (210) and the coating layer (220) before assembly of the unit cell (1). As a specific example, the lithium metal layer may be disposed as a lithium foil between the negative current collector (210) and the coating layer (220) before assembly of the unit cell (1).
[0097] According to another embodiment of the present invention, the lithium metal layer may be formed by precipitation through charging after the assembly of the battery. In this case, since the lithium metal layer is not included during the assembly of the battery, the energy density of the battery may be increased, and charging may be performed beyond the charging capacity of the coating layer. That is, the coating layer (220) may be overcharged. Specifically, lithium may be absorbed in the coating layer (220) during the initial charging phase, but when charged beyond the capacity of the coating layer, lithium may be precipitated between the coating layer (220) and the negative current collector (210) to form a lithium metal layer.
[0098] Since the above lithium metal layer can be composed mainly of lithium, the lithium in the lithium metal layer can be ionized and move to the positive electrode during discharge. That is, the lithium in the lithium metal layer can be used as a negative electrode active material.
[0099] In addition, since the coating layer (220) can be disposed on the lithium metal layer, the coating layer (220) can cover and protect the lithium metal layer and suppress the precipitation growth of lithium dendrites. Therefore, external short circuits and capacity degradation of the battery can be suppressed, and the cycle characteristics of the battery can be improved.
[0100] When a lithium metal layer is formed by charging after assembly of the unit cell (1), the negative current collector (210), the coating layer (220), and the region between them may be a Li-free region that does not contain lithium (Li) in the initial state or after complete discharge of the battery.
[0101] Additionally, according to another embodiment of the present invention, the all-solid-state battery may further include a plurality of elastic layers (400) interposed between each of the plurality of unit cells (1) (see FIG. 5). Additionally, according to another embodiment of the present invention, the all-solid-state battery may include the plurality of unit cells (1) and may include an elastic layer (400) at the bottom and / or top of the unit cell (1) (see FIG. 5).
[0102] The elastic layer (400) may include an insulating resin. For example, the elastic layer may include an epoxy resin, an acrylic resin, a polyimide resin, a polyester resin, a polypropylene resin, a polyamide resin, a polystyrene resin, a polyvinyl chloride resin, a polycarbonate resin, a fluoropolymer resin, silicone rubber, or a combination thereof.
[0103] By including the above elastic layer (400), the elastic layer can absorb external vibrations or shocks to prevent physical damage between unit cells (1), thereby improving the safety of the all-solid-state battery and reducing contact failures or damage between unit cells. Additionally, the elastic layer (400) can effectively dissipate heat generated within the battery to prevent overheating and can mitigate volume changes of the electrode that may occur during charging and discharging, thereby improving cycle characteristics.
[0104]
[0105] <Bipolar>
[0106] The anode (100) may include an anode active material layer (120). Additionally, the anode (100) may not include an anode current collector (110). That is, the anode current collector (110) may be omitted.
[0107] Additionally, the anode (100) may include an anode current collector (110) and an anode active material layer (120) disposed on one surface of the anode current collector (see FIGS. 1 to 3).
[0108] The positive current collector (110) can provide a reference surface on which the positive active material layer (120) is placed. For example, the positive current collector (110) may include a plate or foil comprising indium (In), copper (Cu), magnesium (Mg), stainless steel (SUS), titanium (Ti), iron (Fe), cobalt (Co), nickel (Ni), zinc (Zn), aluminum (Al), germanium (Ge), lithium (Li), or an alloy thereof. As a specific example, the positive current collector (110) may be an aluminum foil.
[0109] The thickness of the anode current collector (110) may be, for example, 1 μm to 100 μm, 1 μm to 50 μm, 5 μm to 35 μm, or 8 μm to 30 μm.
[0110] According to another embodiment of the present invention, the anode (100) may further include a carbon layer between the anode current collector (110) and the anode active material layer (120). For example, the carbon layer may include amorphous carbon, crystalline carbon, etc., and its thickness may be 20 nm to 1 μm, 50 nm to 1 μm, or 1 μm to 4 μm. By including the carbon layer, the bonding strength between the anode current collector (110) and the anode active material layer (120) can be improved.
[0111] The positive electrode active material is a material capable of reversibly absorbing and desorbing lithium ions. 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, as well as nickel sulfide, copper sulfide, lithium sulfide, iron oxide, or vanadium oxide, but is not limited thereto. The positive electrode active material may consist of one type or be a mixture of two or more types.
[0112] 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 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 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.
[0113] 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. 양극활물질이 층상암염형 구조를 갖는 삼원계 리튬전이금속산화물을 포함하는 경우, 전고체 전지(10)의 에너지 밀도가 커지고 열안정성이 향상될 수 있다.
[0114] 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.
[0115] 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.
[0116] The shape of the positive electrode active material may include particle shapes such as spheres or ellipsoids. The particle size and content of the positive electrode active material are not particularly limited.
[0117] The solid electrolyte may include a sulfide-based solid electrolyte with excellent lithium ion conductivity characteristics. Sulfide-based solid electrolytes include, 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 x It may include at least one selected from (0≤x≤2).
[0118] 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 xIt 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.
[0119] Alternatively, sulfide-based solid electrolytes are Li 7-a-c M a PS 6-c X c It may be an argyrodite-type compound containing (0≤a≤2, (0≤c≤2)). Here, X may be F, Br, Cl, or a combination thereof. M can be candium (Sc), yttrium (Y), titanium (Ti), zirconium (Zr), hafnium (Hf), vanadium (V), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo), tungsten (W), manganese (Mn), technetium (Tc), rhenium (Re), iron (Fe), ruthenium (Ru), osmium (Os), cobalt (Co), rhodium (Rh), iridium (Ir), nickel (Ni), palladium (Pd), platinum (Pt), copper (Cu), silver (Ag), gold (Au), zinc (Zn), cadmium (Cd), mercury (Hg), aluminum (Al), gallium (Ga), indium (In), thallium (Tl), silicon (Si), germanium (Ge), tin (Sn), lead (Pb), arsenic (As), antimony (Sb), bismuth (Bi), or a combination thereof. there is.
[0120] 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 circuits 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.
[0121] The solid electrolyte included in the positive electrode active material layer (120) may have a smaller average particle size (D50) compared to the solid electrolyte included in the solid electrolyte layer (300). For example, the average 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 average particle size (D50) of the solid electrolyte included in the solid electrolyte layer (300). Meanwhile, the average particle size (D50) may be the median diameter measured using a laser particle size distribution meter.
[0122] 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 (20), thereby increasing the conductivity of the positive 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.
[0123] The positive active material layer (120) may further include a binder. The binder may include a material for bonding the positive active material, solid electrolyte, and conductive material included in the positive active material layer (120), and for improving the bonding strength with the positive current collector (110). For example, the binder may include polyvinylidene fluoride, styrene butadiene rubber (SBR), polytetrafluoroethylene, polyvinylidene fluoride, vinylidene fluoride / hexafluoropropylene copolymer, polyacrylonitrile, and polymethyl methacrylate.
[0124] The content of the positive active material in the positive active material layer may be 80 to 95 parts by weight, and the content of the binder may be 0.1 to 2 parts by weight. For example, when the positive active material layer comprises the positive active material, the solid electrolyte, the conductive material, and the binder, the positive active material layer may comprise 80 to 92 parts by weight or 85 to 95 parts by weight of the positive active material and 0.2 to 1.5 parts by weight or 0.5 to 1.5 parts by weight of the binder, based on the total weight of the positive active material, the solid electrolyte, the conductive material, and the binder.
[0125] In addition, the content of the conductive material in the positive active material layer may be 1 to 50 parts by weight. For example, the positive active material layer may contain 1.5 to 40 parts by weight or 2 to 30 parts by weight of conductive material per 100 parts by weight of the solid electrolyte. If the content of the conductive material is less than the above range, it may be difficult to secure sufficient electrical conductivity in the positive active material layer, and if the content of the conductive material exceeds the above range, a coating layer covering the surface of the solid electrolyte may not be properly formed.
[0126] In addition, 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.
[0127]
[0128] <Cathode>
[0129] The above cathode (200) may include a cathode current collector (210) and a coating layer (220). The cathode current collector (210) may provide a reference surface on which the coating layer (220) is placed (see FIGS. 1 to 3).
[0130] The above-mentioned negative electrode current collector (210) may include a material that does not react with lithium, that is, does not form an alloy or compound with lithium. For example, the above-mentioned negative electrode current collector (210) may include at least one metal selected from the group consisting of copper (Cu), stainless steel (SUS), titanium (Ti), iron (Fe), cobalt (Co), and nickel (Ni). The above-mentioned negative electrode current collector (210) may be composed of one of the metals described above, or may include an alloy or coating material of two or more metals.
[0131] Additionally, the negative current collector (210) may be in the form of a plate or a foil, and the thickness of the negative current collector (210) may be 1 μm to 20 μm, 5 μm to 15 μm, or 7 μm to 10 μm.
[0132] According to another embodiment of the present invention, the all-solid-state battery may not include a negative electrode current collector (210). That is, the negative electrode current collector (210) may be omitted.
[0133] The coating layer (220) can be configured to allow lithium metal to grow between the solid electrolyte layer (300) and the negative current collector (210). The coating layer (220) can serve as a protective layer for the lithium metal and simultaneously suppress the precipitation and growth of lithium dendrites.
[0134] The coating layer (220) may be a single-layer structure or a multi-layer structure including a plurality of layers. For example, the coating layer (220) may be a single layer or a structure of two, three, or four layers.
[0135] The coating layer (220) may include a metal-carbon composite. More specifically, the coating layer (220) may include a composite of metal particles and a carbon-based material.
[0136] Specifically, the coating layer (220) may be a metal-carbon composite having a particle shape as a composite of metal particles and a carbon-based material. For example, the average particle size of the metal-carbon composite may be 4 μm or less, 3 μm or less, 2 μm or less, 1 μm or less, or 900 nm or less, and may be 10 nm to 4 μm, 10 nm to 3 μm, 10 nm to 2 μm, 10 nm to 1 μm, or 10 nm to 900 nm. By satisfying the above ranges for the average particle size of the metal-carbon composite, reversible absorption and / or desorption of lithium during charging and discharging may be easier. The average particle size of the metal-carbon composite is the median diameter (D50) measured using a laser particle size distribution meter.
[0137] The metal particles in the metal-carbon composite may comprise at least one metal or metalloid 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). Additionally, the carbon-based material in the metal-carbon composite may comprise at least one selected from the group consisting of carbon black, acetylene black, furnace black, Kettjen black, and graphene. As a specific example, the carbon-based material in the metal-carbon composite may be amorphous carbon. The amorphous carbon may be carbon that does not have crystallinity or has very low crystallinity.
[0138] The weight ratio of the metal particles and the carbon-based material in the coating layer (220) may be 10:1 to 1:2. For example, the mixing ratio of the metal particles and the carbon-based material may be 5:1 to 1:1 or 4:1 to 2:1.
[0139] In addition, the content of the metal particles may be 8% to 60% by weight, 10% to 50% by weight, 15% to 40% by weight, or 20% to 30% by weight with respect to the total weight of the metal-carbon composite. By satisfying the above ranges for the content of the metal particles, the cycle characteristics of the battery can be further improved.
[0140] According to another embodiment of the present invention, the coating layer (220) may further include other additives in addition to the metal-carbon composite. For example, the coating layer (220) may further include at least one additive selected from the group consisting of binders, fillers, coating agents, dispersants, and ion-conducting aids.
[0141] Additionally, the thickness of the coating layer (220) may be smaller than the thickness of the positive active material layer. For example, the thickness of the coating layer (220) may be 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 active material layer (120), and may be 1 μm to 20 μm, 2 μm to 10 μm, or 3 μm to 7 μm. By satisfying the above range, the cycle characteristics of the battery can be further improved. If the thickness of the coating layer (220) exceeds the above range, the energy density of the battery containing it may decrease, and the internal resistance may increase, thereby degrading the cycle characteristics.
[0142] According to another embodiment of the present invention, the cathode (200) may further include a thin film between the cathode current collector (210) and the coating layer (220). The thin film may be disposed on one surface of the cathode current collector (210) and may form an alloy with lithium.
[0143] The thin film may include elements capable of forming an alloy with lithium. For example, the thin film may include gold, silver, zinc, tin, indium, silicon, aluminum, bismuth, etc., capable of forming an alloy with lithium, but is not limited thereto; any element capable of forming an alloy with lithium in the relevant technical field is possible. The thin film may be composed of one of these metals, or may be composed of an alloy of various types of metals.
[0144] By including the above thin film, the deposition pattern of the lithium metal layer deposited between the thin film and the coating layer (220) can be further flattened, and the cycle characteristics of the battery can be further improved.
[0145] For example, the thickness of the thin film may be 1 nm to 800 nm, 10 nm to 700 nm, 50 nm to 600 nm, or 100 nm to 500 nm. If the thickness of the thin film is less than the above range, it may be difficult to perform the function of the thin film, and if it exceeds the above range, the thin film may absorb lithium, which may reduce the amount of lithium precipitated at the negative electrode, thereby degrading the energy density and cycle characteristics of the battery.
[0146] The above thin film may be formed by vacuum deposition, sputtering, plating, etc., but is not limited thereto.
[0147] According to another embodiment of the present invention, the cathode (200) may further include a carbon layer between the cathode current collector (210) and the solid electrolyte layer (300). The description of the carbon layer is the same as previously described.
[0148] According to another embodiment of the present invention, the cathode (200) may include a cathode active material layer corresponding to the coating layer (220).
[0149] The negative electrode active material in the above negative electrode active material layer may include a material capable of reversibly intercalating / deintercalating lithium ions, lithium metal, an alloy of lithium metal, a material capable of doping and dedoping lithium, or a transition metal oxide.
[0150] A material capable of reversibly intercalating / deintercalating the above lithium ions may be a carbon-based negative electrode active material, such as crystalline carbon, amorphous carbon, or a combination thereof. Examples of the crystalline carbon include graphite such as amorphous, plate-like, flake-like, spherical, or fibrous natural graphite or artificial graphite, and examples of the amorphous carbon include soft carbon or hard carbon, mesophase pitch carbide, calcined coke, etc.
[0151] As the above lithium metal alloy, an alloy of lithium and a metal selected from Na, K, Rb, Cs, Fr, Be, Mg, Ca, Sr, Si, Sb, Pb, In, Zn, Ba, Ra, Ge, Al, and Sn may be used.
[0152] As a material capable of doping and undoping the above lithium, a Si-based negative electrode active material or a Sn-based negative electrode active material may be used. The above Si-based negative electrode active material may be silicon, a silicon-carbon composite, SiOx (0 < x ≤ 2), a Si-Q alloy (wherein Q is selected from alkali metals, alkaline earth metals, group 13 elements, group 14 elements (excluding Si), group 15 elements, group 16 elements, transition metals, rare earth elements, and combinations thereof), or a combination thereof. The above Sn-based negative electrode active material may be Sn, SnO2, a Sn-based alloy, or a combination thereof.
[0153] The silicon-carbon composite may be a composite of silicon and amorphous carbon. As a specific example, the silicon-carbon composite may be in the form of silicon particles and amorphous carbon coated on the surface of the silicon particles. For example, it may include a secondary particle (core) assembled from silicon primary particles and an amorphous carbon coating layer (shell) located on the surface of the secondary particle. The amorphous carbon may also be located between the silicon primary particles, for example, the silicon primary particles may be coated with the amorphous carbon. Additionally, the secondary particles may be dispersed within an amorphous carbon matrix.
[0154] The silicon-carbon composite may further include crystalline carbon. For example, the silicon-carbon composite may include a core comprising crystalline carbon and silicon particles and an amorphous carbon coating layer located on the surface of the core.
[0155] The above Si-based or Sn-based negative electrode active material can be used in combination with a carbon-based negative electrode active material.
[0156] In addition, the content of the negative electrode active material in the negative electrode active material layer may be 90% to 99% by weight with respect to the total weight of the negative electrode active material layer. For example, the content of the negative electrode active material may be 93% to 99% by weight or 96% to 98.5% by weight with respect to the total weight of the negative electrode active material layer.
[0157] As a specific example, the above-mentioned negative electrode active material may include at least one of graphite and Si composites.
[0158] When the above-mentioned cathode active material includes a Si composite and graphite together, the Si composite and graphite may be included in the form of a mixture, in which case the weight ratio of the Si composite and graphite may be 1:99 to 50:50. For example, the weight ratio of the Si composite and graphite may be 3:97 to 20:80 or 5:95 to 20:80.
[0159] The above Si composite may include a core containing Si-based particles and an amorphous carbon coating layer, for example, the Si-based particles may be a Si-C composite, SiO x It may include one or more of (0 < x ≤ 2) and Si alloys. For example, the Si-C composite may include a core containing Si particles and crystalline carbon and an amorphous carbon coating layer located on the surface of the core.
[0160] The above crystalline carbon may include, for example, graphite, and more specifically, may include natural graphite, artificial graphite, or a mixture thereof.
[0161] The above-mentioned cathode may include a binder. The cathode binder can effectively bond the cathode active material particles to each other and can serve to effectively bond the cathode active material to the current collector. As the binder, a non-aqueous binder, an aqueous binder, a dry binder, or a combination thereof may be used.
[0162] The above-mentioned non-aqueous binder may be polyvinyl chloride, carboxylated polyvinyl chloride, polyvinyl fluoride, ethylene propylene copolymer, polystyrene, polyurethane, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, polypropylene, polyamide imide, polyimide, or a combination thereof.
[0163] The above-mentioned water-based binder may be selected from styrene-butadiene rubber, (meth)acrylated styrene-butadiene rubber, (meth)acrylonitrile-butadiene rubber, (meth)acrylic rubber, butyl rubber, fluororubber, polyethylene oxide, polyvinylpyrrolidone, polyepichlorohydrin, polyphosphazene, poly(meth)acrylonitrile, ethylene propylene diene copolymer, polyvinylpyridine, chlorosulfonated polyethylene, latex, polyester resin, (meth)acrylic resin, phenolic resin, epoxy resin, polyvinyl alcohol, and combinations thereof.
[0164] When a water-based binder is used as the above-mentioned cathode binder, a cellulose-based compound capable of imparting viscosity may be further included. As the cellulose-based compound, one or more types such as carboxymethyl cellulose, hydroxypropylmethyl cellulose, methyl cellulose, or alkali metal salts thereof may be mixed and used. The alkali metal salt may include Na, K, or Li.
[0165] The above dry binder is a polymer material capable of fiberization, and may be, for example, polytetrafluoroethylene, polyvinylidene fluoride, polyvinylidene fluoride-hexafluoropropylene copolymer, polyethylene oxide, or a combination thereof.
[0166] In addition, the content of the binder may be 0.5% to 5% by weight with respect to the total weight of the cathode. For example, the content of the cathode binder may be 0.5% to 3.5% by weight or 0.5% to 2% by weight with respect to the total weight of the cathode.
[0167] The above-mentioned cathode may include a conductive material. The description of the conductive material is the same as previously described.
[0168]
[0169] Solid electrolyte layer
[0170] The above solid electrolyte layer (300) may include a solid electrolyte.
[0171] The above solid electrolyte may include a sulfide-based solid electrolyte, an oxide-based solid electrolyte, or a combination thereof. As a specific example, the solid electrolyte included in the solid electrolyte layer (300) may be the same as or different from the solid electrolyte included in the positive electrode active material layer (110).
[0172] The description of the solid electrolyte above is the same as previously stated.
[0173]
[0174] gasket
[0175] An all-solid-state battery according to one embodiment of the present invention includes a gasket disposed on one side of an electrode assembly comprising at least one unit cell.
[0176] An anode substrate tab (TB1) extending from a plurality of unit cells (1) may include a bending portion A (TB1a) extending at an angle from the unit cells (1) and a tab assembly portion (TB1b) formed by the bending portion A (TB1a) being gathered together. At this time, a first gasket (501) surrounds the bending portion A (TB1a) and is positioned so that the corner of the first gasket (501) contacts the outer material (PCH), thereby allowing the anode substrate tab (TB1) to be separated from the outer material (PCH) by the first gasket (501) (see FIGS. 6 and 7).
[0177] Additionally, a cathode substrate tab (TB2) extending from a plurality of unit cells (1) may include a bending portion A (TB2a) extending at an angle from the unit cell (1) and a tab assembly portion (TB2b) formed by the bending portion A (TB2a) being gathered together. At this time, the second gasket (502) surrounds the bending portion A (TB2a) and is positioned so that the corner of the second gasket (502) contacts the outer material (PCH), thereby allowing the cathode substrate tab (TB2) to be separated from the outer material (PCH) by the second gasket (502) (see FIGS. 6 and 7).
[0178] The separation distance between the above-mentioned base tab and the above-mentioned exterior material may be 100 μm or more. For example, the separation distance between the above-mentioned base tab (TB1 or TB2) and the above-mentioned exterior material may be 200 μm or more, 500 μm or more, or 1 mm or more, and may be 3 mm or less, 2 mm or less, or 1.5 mm or less. By satisfying the above ranges for the separation distance between the base tab and the exterior material, excellent flexibility of the exterior material can be secured while safety can be improved. The above separation distance refers to the shortest distance between the base tab and the exterior material.
[0179] Additionally, the angle (α1) formed by the upper surface of the gasket with the exterior material may be 20° to 70°, and the angle (α3) formed by the lower surface of the gasket with the exterior material may be 20° to 70° (see FIG. 6 and 7). For example, the corners of each of the first and second gaskets (501 and 502) may come into contact with the exterior material (PCH), and the angle (α1) formed by the upper surface of each of the first and second gaskets (501 and 502) with the exterior material may be 25° to 75°, 25° to 70°, or 30° to 60°. Additionally, the angle (α3) formed by the lower surface of each of the first and second gaskets (501 and 502) with the exterior material (PCH) may be 25° to 75°, 25° to 70°, or 30° to 60°. The angle (α1) formed by the upper surface of the first and second gaskets (501 and 502) with the exterior material and the angle (α2) formed by the lower surface of the first and second gaskets (501 and 502) with the exterior material may be the same or different from each other.
[0180] Additionally, the angle (α2) formed by the front surface of the gasket with the exterior material may be 10° to 60° (see FIG. 6 and 7). For example, the corners of each of the first and second gaskets (501 and 502) are in contact with the exterior material (PCH), and the angle (α2) formed by the front surface (second direction (D2)) of each of the first and second gaskets (501 and 501) with the exterior material may be 10° to 50°, 15° to 45°, or 20° to 35°.
[0181] Additionally, the substrate tab may have the same thickness as the positive current collector or the negative current collector. More specifically, the positive substrate tab (TB1) may have the same thickness as the positive current collector (110), and the negative substrate tab (TB2) may have the same thickness as the negative current collector (210).
[0182] According to one embodiment of the present invention, the gasket may include a vertical extension portion extending vertically along the stacking direction of the electrode assembly; a first horizontal extension portion and a second horizontal extension portion extending horizontally from the vertical extension portion; and an opening formed between the first horizontal extension portion and the second horizontal extension portion. At this time, the banding portion A of the substrate tab may be inserted into the opening.
[0183] FIG. 8 is a cross-sectional view according to a first direction of a gasket according to an embodiment of the present invention. Specifically, the gasket (500) may include a vertical extension (510) comprising a first vertical extension (511) and a second vertical extension (512) that extend vertically along a third direction (D3), which is the stacking direction of the electrode assembly (10); a horizontal extension (520) comprising a first horizontal extension (521) and a second horizontal extension (522) that extend horizontally from the vertical extension (510); and an opening (530) formed between the first horizontal extension (521) and the second horizontal extension (522). More specifically, the first vertical extension (511) and the second vertical extension (512) may be in a shape facing each other.
[0184] FIG. 9 is a cross-sectional view according to a first direction of a gasket according to another embodiment of the present invention. Specifically, the gasket (500) may include a vertical extension (510, first vertical extension (511)) that extends vertically along a third direction (D3) which is the stacking direction of the electrode assembly (10), a horizontal extension (520) that includes a first horizontal extension (521) and a second horizontal extension (522) that extend horizontally from the vertical extension (510), and an opening (530) formed between the first horizontal extension (521) and the second horizontal extension (522).
[0185] As shown in FIG. 8, the vertical extension (510) of the gasket (500) may include a first vertical extension (511) connecting one end of the first horizontal extension (521) and one end of the second horizontal extension (522), and a second vertical extension (512) connecting the other end of the first horizontal extension (521) and the other end of the second horizontal extension (522). Additionally, as shown in FIG. 9, the vertical extension (510) of the gasket (500) may be composed only of the first vertical extension (511) that contacts one surface of the first and second horizontal extensions (521 and 522).
[0186] When the gasket (500) is composed only of the first vertical extension (511), installation may be easy as the gasket (500) can also be fitted in the first direction (D1) when placed on one side of the electrode assembly (10) (see FIG. 9). In addition, when the gasket (500) is composed of the first and second vertical extensions (511 and 512), the effect of protecting the electrode assembly (10) from external foreign substances and the effect of relieving the pressure received by the substrate tab due to external stimuli can be further enhanced (see FIG. 8).
[0187] FIG. 10 is a cross-sectional view according to a second direction of a gasket according to one embodiment of the present invention, and FIG. 11 is a cross-sectional view according to a second direction of a gasket according to another embodiment of the present invention. Specifically, the opening (530) of the gasket (500) may be formed between a first horizontal extension (521) and a second horizontal extension (522), and the width (b) of the opening (530) in the vertical direction may be constant as seen in FIG. 10, and as seen in FIG. 11, the width (b) of the opening (530) in the vertical direction may decrease as it approaches the tab collection (TB1b or TB2b). As seen in FIG. 11, when the width (b) of the opening (530) in the vertical direction decreases and forms a slope as it approaches the tab collection part (TB1b or TB2b), that is, as it goes toward the second direction (D2), it may be easier to insert the bending part A (TB1a or TB2a) into the opening (530).
[0188] Additionally, the thickness (a) of the gasket (500) may be 30 µm to 300 µm. For example, the thickness of the gasket (500) may be 100 µm to 300 µm, 120 µm to 300 µm, 150 µm to 280 µm, or 160 µm to 250 µm. The thickness (a1) of the first gasket may be the same as or different from the thickness (a2) of the second gasket.
[0189] Additionally, with respect to the vertical direction in which the unit cell (1) is stacked, the length (L2) of the gasket (500) may be equal to or smaller than the length (L1) of the electrode assembly (10) (see FIG. 6 to 9). For example, with respect to the third direction (D3) in which the unit cell (1) is stacked, the length (L2) of the gasket (500) may be 99.5% to 60%, 95% to 70%, or 90% to 80% of the length (L1) of the electrode assembly (10).
[0190] According to one embodiment of the present invention, the gasket (500) may include a polymer having a melting point of 200°C or higher. For example, the melting point of the polymer may be 210°C or higher, 225°C or higher, or 250°C or higher.
[0191] In addition, the gasket (500) is 1.0 × 10 -10 It may include a polymer having an electrical conductivity of S / m or less. For example, the electrical conductivity of the polymer is 0.5 × 10⁻⁶ -10 S / m or less, 1.0 × 10 -9 S / m or less or 1.0 × 10 -8 It may be less than S / m. The gasket (500) has a melting point of 200°C or higher and / or 1.0 × 10 -10 By including a polymer having an electrical conductivity of S / m or less, short circuits can be prevented more effectively, thereby maximizing the safety of the battery.
[0192] The above polymer may include polytetrafluoroethylene (PTFE), polyimide (PI), polyetheretherketone (PEEK), polyphenylene sulfide (PPS), polyethylene terephthalate (PET), nylon 46 (Nylon 46), polycarbonate (PC), polyphenylsulfone (PPSU), or a combination thereof.
[0193]
[0194] Exterior materials
[0195] According to one embodiment of the present invention, the all-solid-state battery may include an outer casing. Additionally, the outer casing may include an insulating layer. As a specific example, the all-solid-state battery may be a pouch-type all-solid-state battery including a pouch outer casing.
[0196] For example, the insulating layer may include polypropylene, polyethylene, polyester, polyamide, polyimide, polyvinyl chloride, polycarbonate, polystyrene, ethylene-vinyl acetate, or a combination thereof.
[0197] In addition, the thickness of the insulating layer may be 5 μm to 100 μm, 5 μm to 70 μm, 8 μm to 50 μm, or 10 μm to 35 μm.
[0198] In addition, the exterior material may further include a functional layer in addition to the insulating layer. For example, the exterior material may further include a functional layer such as a metal layer such as Al in addition to the insulating layer, but is not limited thereto.
[0199] The thickness of the exterior material may be 60 µm to 300 µm, 80 µm to 250 µm, or 100 µm to 250 µm.
[0200]
[0201] Meanwhile, an all-solid-state battery according to another embodiment of the present invention comprises an electrode assembly including at least one unit cell; a substrate tab extending from the unit cell; a gasket disposed on one side of the electrode assembly and configured to surround the substrate tab; and an outer casing that accommodates the electrode assembly, wherein the substrate tab includes a connecting portion adjacent to the unit cell and a bending portion B extending at an angle from the connecting portion, and the gasket surrounds the connecting portion.
[0202] FIG. 14 is a cross-sectional view along the line AA' of FIG. 4, schematically illustrating a cross-section of a pouch-type all-solid-state battery according to another embodiment of the present invention. Specifically, FIG. 14 illustrates a cross-section of a pouch-type all-solid-state battery (20) in which a gasket (500) is disposed on one side of an electrode assembly (10), more specifically on the side where a positive electrode substrate tab (TB1) is provided.
[0203] More specifically, the all-solid-state battery (20) may include a plurality of unit cells (1) and a plurality of substrate tabs (a plurality of TB1 and a plurality of TB2) extending from the plurality of unit cells (1), and each of the plurality of substrate tabs may include a tab assembly (TB1c or TB2c). The tab assembly may be in the form where the plurality of substrate tabs are gathered together.
[0204] That is, as shown in FIG. 14, the pouch-type all-solid-state battery (20) includes an electrode assembly (10) comprising a plurality of unit cells (1), and includes a gasket (500) disposed on one side of the electrode assembly (10), more specifically on the side where a positive electrode substrate tab (TB1) is provided, and each of the plurality of positive electrode substrate tabs (TB1) may include a connecting portion (TB1a) adjacent to the unit cell (1), a bending portion B (TB1b) extending at an angle from the connecting portion, and a tab assembly portion (TB1c) in which the plurality of substrate tabs are gathered together. At this time, the pouch-type all-solid-state battery (20) may include a positive lead tab (LTB1) and a negative lead tab (LTB2) that are electrically connected to the plurality of positive substrate tabs (TB1) and negative substrate tabs (TB2), respectively, and the tab assembly (TB1c or TB2c) may be in a form that can be electrically connected to the positive lead tab (LTB1) and the negative lead tab (LTB2), respectively.
[0205] Additionally, FIG. 14 illustrates a structure in which a gasket (500) is placed only on one side equipped with an anode substrate tab (TB1) and an anode lead tab (LTB1), but a gasket (500) may also be placed on one side equipped with a cathode substrate tab (TB2) and a cathode lead tab (LTB2). That is, a gasket (500) may be placed on both sides of the electrode assembly (10). At this time, the electrode assembly (10) schematically illustrates a structure in which a plurality of unit cells (1) are stacked, and each of the unit cells (1) illustrates a structure in which an elastic layer (400), an anode (100), a solid electrolyte layer (300), and a cathode (200) are stacked.
[0206]
[0207] electrode assembly
[0208] The description of the electrode assembly is the same as previously stated.
[0209]
[0210] gasket
[0211] A solid-state battery according to another embodiment of the present invention includes a gasket disposed on one side of an electrode assembly comprising at least one unit cell.
[0212] FIG. 15 is a schematic cross-sectional view illustrating an enlarged view of the M region of FIG. 14. Referring to FIG. 14 and 15, an anode substrate tab (TB1) may be extended from an anode current collector (110) toward a second direction (D2). The anode substrate tab (TB1) may include a connecting portion (TB1a) adjacent to the anode and a bending portion B (TB1b) extending at an angle from the connecting portion. A gasket (500) may be positioned on one side of the electrode assembly (10) and arranged to surround the connecting portion (TB1a) of the anode substrate tab (TB1).
[0213] Additionally, the substrate tab may have the same thickness as the positive current collector or the negative current collector. More specifically, the positive substrate tab (TB1) may have the same thickness as the positive current collector (110), and the negative substrate tab (TB2) may have the same thickness as the negative current collector (210).
[0214] According to another embodiment of the present invention, the substrate tab may be secured by a gasket. The substrate tab may be an anode substrate tab (TB1) and a cathode substrate tab (TB2). The gasket (500) may surround and secure at least one of the connecting portions (TB1a or TB2a) of the anode substrate tab (TB1) and the cathode substrate tab (TB2).
[0215] More specifically, as shown in FIG. 14, the positive electrode substrate tab (TB1) may include a connecting portion (TB1a) adjacent to the unit cell (1) and a bending portion B (TB1b) extending at an angle from the connecting portion (TB1a), and the gasket (500) may serve to fix the connecting portion (TB1a) of the positive electrode substrate tab (TB1). That is, the gasket (500) can protect the unit cell (1) from the outside on one side of the electrode assembly (10), and at the same time, by fixing the positive electrode substrate tab (TB1), it can relieve pressure on the positive electrode substrate tab (TB1) caused by external stimuli, thereby preventing short circuits or internal short circuits from occurring.
[0216] FIG. 14 illustrates a structure in which a gasket (500) is disposed only on one side equipped with an anode substrate tab (TB1) and an anode lead tab (LTB1), but a gasket (500) may also be disposed on one side equipped with a cathode substrate tab (TB2) and a cathode lead tab (LTB2). Specifically, the cathode substrate tab (TB2) may also include a connecting portion (TB2a) adjacent to the unit cell (1) and a bending portion B (TB2b) extending from the connecting portion (TB2a) with an incline, and the gasket (500) may serve to fix the connecting portion (TB2a) of the cathode substrate tab (TB2).
[0217] According to another embodiment of the present invention, the gasket may include a vertical extension portion extending vertically along the stacking direction of the electrode assembly; a first horizontal extension portion and a second horizontal extension portion extending horizontally from the vertical extension portion; and an opening formed between the first horizontal extension portion and the second horizontal extension portion.
[0218] FIG. 16 is a schematic cross-sectional view illustrating a gasket according to another embodiment of the present invention. Specifically, the gasket (500) may include a vertical extension (510) comprising a first vertical extension (511) and a second vertical extension (512) that extend vertically along a third direction (D3), which is the stacking direction of the electrode assembly (10); a horizontal extension (520) comprising a first horizontal extension (521) and a second horizontal extension (522) that extend horizontally from the vertical extension (510); and an opening (530) formed between the first horizontal extension (521) and the second horizontal extension (522). More specifically, the first vertical extension (511) and the second vertical extension (512) may be in a form facing each other.
[0219] FIG. 17 is a schematic cross-sectional view illustrating a gasket according to another embodiment of the present invention. Specifically, the gasket (500) may include a vertical extension (510, first vertical extension (511)) that extends vertically along a third direction (D3) which is the stacking direction of the electrode assembly (10), a horizontal extension (520) that includes a first horizontal extension (521) and a second horizontal extension (522) that extend horizontally from the vertical extension (510), and an opening (530) formed between the first horizontal extension (521) and the second horizontal extension (522).
[0220] As shown in FIG. 16, the vertical extension (510) of the gasket (500) may include a first vertical extension (511) in contact with one side of the first and second horizontal extensions (521 and 522) and a second vertical extension (512) in contact with the other side of the first and second horizontal extensions (521 and 522). Additionally, as shown in FIG. 17, the vertical extension (510) of the gasket (500) may be composed only of the first vertical extension (511) in contact with one side of the first and second horizontal extensions (521 and 522).
[0221] When the gasket (500) is composed only of the first vertical extension (511), installation may be easy because the gasket (500) can be inserted in the first direction (D1) when placed on one side of the electrode assembly (10) (see FIG. 17). In addition, when the gasket (500) is composed of the first and second vertical extensions (511 and 512), the effect of protecting the electrode assembly (10) from external foreign substances and the effect of relieving the pressure received by the substrate tab due to external stimuli can be further enhanced (see FIG. 16).
[0222] FIG. 18 is a cross-sectional view of a gasket according to another embodiment of the present invention. Specifically, the gasket (500) may include four openings (530, first to fourth openings (531 to 534), a vertical extension (510, including a first vertical extension (511) and a second vertical extension (512)) that extends vertically along a third direction (D3) which is the stacking direction of the electrode assembly (10), and first to fourth horizontal extensions (521 to 525) that extend horizontally from the vertical extension.
[0223] FIG. 19 is a cross-sectional view of a gasket according to another embodiment of the present invention. Specifically, the gasket (500) may include four openings (530, first opening to fourth openings (531 to 534)), a vertical extension (500, first vertical extension (511)) that extends vertically along a third direction (D3) which is the stacking direction of the electrode assembly (10), and first to fourth horizontal extensions (521 to 524) that extend horizontally from the vertical extension.
[0224] The gasket (500) may include at least one opening (530). Specifically, the gasket (500) may include a plurality of openings (530), and each of the plurality of openings may have a different shape.
[0225] For example, the shape of the opening (530) may be a polygon such as a square, or a shape including curves such as a circle, a semicircle, or an ellipse. As a specific example, the gasket (500) may include a square opening, or a shape in which one or more square openings are surrounded by a vertical extension and a horizontal extension. Additionally, the gasket (500) may include a circular, semicircular, or elliptical opening, and may be in the shape of the letters E, B, P, or D.
[0226] Additionally, the connecting portion (TB1a or TB2a) of the substrate tab (TB1 or TB2) may be inserted into the opening (530), and the opening (530) may have the same shape as the substrate tab (TB1 or TB2) (see FIG. 16 and 17). More specifically, the shape of the cross-sectional area in the first direction (D1) of the opening (530) may be the same as the cross-sectional area in the first direction (D1) of the substrate tab (TB1 or TB2), that is, the shape of the cross-sectional area of the connecting portion (TB1a or TB2a) of the substrate tab (TB1 or TB2).
[0227] Additionally, the opening (530) may have a larger cross-sectional area than the substrate tab (TB1 or TB2). Specifically, the cross-sectional area of the opening (530) may be larger than the cross-sectional area of the substrate tab (TB1 or TB2) so that the substrate tab (TB1 or TB2) can be easily inserted through the opening (530). For example, the cross-sectional area of the opening (530) may be 102% to 135% or 105% to 120% of the cross-sectional area of the substrate tab (TB1 or TB2). If the cross-sectional area of the opening (530) is below the above range, it may not be easy to insert the substrate tab (TB1 or TB2), and if it exceeds the above range, the effect of preventing short circuits or internal short circuits may be reduced.
[0228] The number of openings (530) may be equal to the number of substrate tabs (TB1 or TB2) on which the gasket (500) is placed. For example, if the number of positive substrate tabs (TB1) that are mutually gathered in the positive tab collection section (TB1c) is 4, the number of openings (530) of the gasket (500) surrounding the connection section (TB1a) of the positive substrate tabs (TB1) may be 4.
[0229] The thickness (a) of the gasket (500) may be 30 µm to 300 µm. For example, the thickness of the gasket (500) may be 30 µm to 200 µm, 30 µm to 180 µm, 40 µm to 160 µm, or 50 µm to 150 µm.
[0230] Additionally, with respect to the vertical direction in which the unit cell (1) is stacked, the length (L2) of the gasket (500) may be equal to or smaller than the length (L1) of the electrode assembly (10) (see FIG. 14, 18 and 19). For example, with respect to the third direction (D3) in which the unit cell (1) is stacked, the length (L2) of the gasket (500) may be equal to the length (L1) of the electrode assembly (10), and the length (L2) of the gasket (500) may be 99.5% to 85% or 99% to 95% of the length (L1) of the electrode assembly (10).
[0231] According to another embodiment of the present invention, the gasket (500) may include a polymer having a heat deflection temperature (HDT) of 200°C or higher. For example, the heat deflection temperature of the polymer may be 210°C or higher, 230°C or higher, 250°C or higher, or 270°C or higher. Since the gasket (500) includes a polymer having a heat deflection temperature of 200°C or higher, thermal runaway caused by a short circuit or internal short circuit can be prevented more effectively, thereby maximizing the safety of the battery.
[0232] The above polymer may include polyimide (PI), polysulfone (PSU), polyetherimide (PEI), polyphenylene sulfide (PPS), polyetheretherketone (PEEK), or a combination thereof.
[0233] In addition, the angle (α) formed by the connecting part (TB1a or TB2a) of the outermost material tab among the plurality of material tabs (multiple TB1s and multiple TB2s) and the bending part B (TB1b or TB2b) may be 120° to 150°, 123° to 145°, or 125° to 135°. Since the angle (α) formed by the connecting part (TB1a or TB2a) of the outermost material tab among the plurality of material tabs (multiple TB1s and multiple TB2s) and the bending part B (TB1b or TB2b) satisfies the above range, the external force received by the outermost material tab can be reduced, thereby further improving safety.
[0234]
[0235] Method for manufacturing all-solid-state batteries
[0236] A method for manufacturing an all-solid-state battery according to another embodiment of the present invention comprises the steps of: manufacturing an electrode assembly comprising at least one unit cell and a substrate tab extending from the unit cell; manufacturing a gasket having an opening; and placing the gasket on one side of the electrode assembly, wherein the step of bending the substrate tab and forming a tab assembly may be performed before or after the step of placing the gasket.
[0237]
[0238] A method for manufacturing an all-solid-state battery according to another embodiment of the present invention may include the steps of: manufacturing an electrode assembly comprising at least one unit cell; bending a substrate tab extending from the unit cell and forming a tab assembly; manufacturing a gasket having an opening; inserting the substrate tab into the opening of the gasket to place the gasket on one side of the electrode assembly; and sealing with an outer casing.
[0239] FIG. 12 shows a schematic flowchart of a method for manufacturing an all-solid-state battery according to another embodiment of the present invention. With reference to FIG. 12, a method (S100) for manufacturing an all-solid-state battery will be described in detail below.
[0240] First, an electrode assembly (10) comprising at least one unit cell (1) is manufactured. Specifically, a plurality of unit cells (1) may be manufactured and stacked to manufacture the electrode assembly (10). The description of the unit cell (1) is the same as previously described.
[0241] Specifically, the unit cell (1) may include an anode (100), a solid electrolyte layer (300), and a cathode (200). The unit cell (1) may be a monocell or a bicell stacked in the order shown in FIGS. 1 to 3, but the stacking order is not limited thereto. The description of the anode (100), the solid electrolyte layer (300), and the cathode (200) is the same as described above.
[0242] Afterwards, the recording tab (TB1 or TB2) extending from the unit cell (1) is bent to form a tab collection part (TB1b or TB2b).
[0243] The above-mentioned tab may include a banding portion A extending at an angle from the unit cell and a tab collection portion in which the banding portions A are gathered together.
[0244] In addition, after bending the above-mentioned tab and forming a tab assembly, the above-mentioned tab can be inserted into the opening of the above-mentioned gasket to place the gasket on one side of the electrode assembly.
[0245] More specifically, a plurality of material tabs (a plurality of TB1s and a plurality of TB2s) extending from the unit cell (1) can each be bent to form a bending portion A (TB1a or TB2a), and the bent plurality of material tabs can be gathered together to form a tab gathering portion (TB1b or TB2b).
[0246] Subsequently, a gasket (500) having an opening is manufactured. The description of the gasket (500) is the same as previously described.
[0247] The process of manufacturing the above gasket (500) may be performed by processes such as injection molding, extrusion molding, and blow molding, but is not limited thereto.
[0248] Afterwards, the material tab (TB1 or TB2) is inserted into the opening (530) of the gasket (500), and the gasket (500) is placed on one side of the electrode assembly (10).
[0249] Specifically, the gasket (500) can be placed on one side of the electrode assembly (10) by inserting the bending portion A (TB1a or TB2a) through the tab collection portion (TB1b or TB2b) of the material tab (TB1 or TB2) into the opening (530) of the gasket (500). At this time, the gasket (500) may also be placed on both sides of the electrode assembly (10).
[0250] Subsequently, it is sealed with an exterior material (PCH). Specifically, it may include a step of sealing with an exterior material (PCH).
[0251] The above gasket can surround the above-mentioned substrate tab, thereby separating the above-mentioned substrate tab from the above-mentioned outer material. More specifically, a solid-state battery (20) can be manufactured by surrounding the above-mentioned electrode assembly (10) and the above-mentioned substrate tab (TB1 or TB2), with a part of the lead tab (LTB1 or LTB2) protruding outside the outer material (PCH), and then sealing. At this time, since the corner of the placed gasket (500) comes into contact with the outer material (PCH) and the above-mentioned substrate tab (TB1 or TB2) and the outer material (PCH) can be separated from each other, a short circuit can be effectively prevented.
[0252] FIG. 13 illustrates the steps for manufacturing an all-solid-state battery according to another embodiment of the present invention. Referring to FIG. 13, a plurality of positive electrode substrate tabs (TB1) extending from a plurality of unit cells (1) of the electrode assembly (10) can be bent to form a bending portion A (TB1a), and then the tabs can be gathered together to form a tab gathering portion (TB1b). Subsequently, the bending portion A (TB1a) can be inserted through the tab gathering portion (TB1b) of the positive electrode substrate tabs (TB1) into the opening (530) of the gasket (500), and the gasket (500) can be placed on one side of the electrode assembly (10).
[0253] In addition, according to another embodiment of the present invention, the step of placing the gasket (500) can be performed after the step of forming the tab assembly (TB1b or TB2b). Accordingly, the gasket (500) can be appropriately placed so that the outer material (PCH) and the base tab (TB1 or TB2) can be spaced apart from each other according to conditions such as the bending angle of the bending portion A (TB1a or TB2a) of the base tab (TB1 or TB2). Therefore, not only can a short circuit between the base tab (TB1 or TB2) and the outer material (PCH) be effectively prevented, but safety can also be ensured with only a simple process of placing the gasket (500) regardless of conditions such as the thickness of the outer material (PCH).
[0254]
[0255] In addition, a method for manufacturing an all-solid-state battery according to another embodiment of the present invention may include the steps of: manufacturing an electrode assembly comprising at least one unit cell; manufacturing a gasket; placing the gasket on one side of the electrode assembly to fix a substrate tab extending from the unit cell; and bending the substrate tab and forming a tab assembly.
[0256] FIG. 20 shows a schematic flowchart of a method for manufacturing an all-solid-state battery according to another embodiment of the present invention. With reference to FIG. 20, a method (S100) for manufacturing an all-solid-state battery will be described in detail below.
[0257] First, an electrode assembly (10) comprising at least one unit cell (1) is manufactured. Specifically, a plurality of unit cells (1) may be manufactured and stacked to manufacture the electrode assembly (10). The description of the unit cell (1) is the same as previously described.
[0258] Specifically, the unit cell (1) may include an anode (100), a solid electrolyte layer (300), and a cathode (200). The unit cell (1) may be a monocell or a bicell stacked in the order shown in FIGS. 1 to 3, but the stacking order is not limited thereto. The description of the anode (100), the solid electrolyte layer (300), and the cathode (200) is the same as described above.
[0259] Afterwards, a gasket (500) is manufactured. The description of the gasket (500) is the same as previously described.
[0260] The process of manufacturing the above gasket (500) may be performed by processes such as injection molding, extrusion molding, and blow molding, but is not limited thereto.
[0261] Afterward, a gasket (500) may be placed on one side of the electrode assembly (10) to fix the substrate tab (TB1 or TB2) extending from the unit cell (1), and then the substrate tab (TB1 or TB2) may be bent to form a tab assembly (TB1c or TB2c). At this time, gaskets (500) may also be placed on both sides of the electrode assembly (10).
[0262] Specifically, the above-mentioned material tab (TB1 or TB2) may include a connecting portion (TB1a or TB2a) adjacent to the unit cell and a bending portion B (TB1b or TB2b) extending at an angle from the connecting portion (TB1a or TB2a), and after fixing the above-mentioned material tab (TB1 or TB2) by placing the gasket (500), the above-mentioned material tab (TB1 or TB2) may be bent to form a tab assembly portion (TB1c or TB2c).
[0263] FIG. 21 illustrates the steps for manufacturing an all-solid-state battery according to another embodiment of the present invention. Referring to FIG. 21, for a plurality of positive electrode substrate tabs (TB1) extending from a plurality of unit cells (1) of the electrode assembly (10), a gasket (500) is placed on one side of the electrode assembly (10) to surround the connecting portion (TB1a) of the plurality of positive electrode substrate tabs (TB1), and then the plurality of positive electrode substrate tabs (TB1) are bent to form a plurality of bending portions B (TB1b), and then the tabs are gathered together to form a tab gathering portion (TB1c).
[0264] The above gasket can surround the connection portion of the above-mentioned tab to secure the above-mentioned tab. Specifically, the step of securing the above-mentioned tab (TB1 or TB2) can be performed by the gasket (500) surrounding the connection portion (TB1a or TB2a) of the above-mentioned tab (TB1 or TB2). More specifically, the above-mentioned tab (TB1 or TB2) can be inserted into the opening (530) of the gasket (500) so that the gasket (500) surrounds the connection portion (TB1a or TB2a) of the above-mentioned tab (TB1 or TB2).
[0265] In addition, according to another embodiment of the present invention, a step of forming a tab assembly (TB1c or TB2c) can be performed after a step of fixing the substrate tab (TB1 or TB2). Accordingly, internal short circuits or short circuits caused by metal foreign substances or substances that may be melted and precipitated from the unit cell (1) that may occur due to a process such as welding to form the tab assembly (TB1c or TB2c) can be effectively prevented, thereby improving safety against fire or thermal runaway.
[0266] Examples and comparative examples of the present invention are described below. However, the following examples are merely one example of the present invention, and the present invention is not limited to the following examples.
[0267]
[0268] [Example]
[0269] Manufacturing of all-solid-state batteries (1)
[0270] Example 1-1
[0271] (1) Manufacturing of the anode
[0272] LiNi0.8Co0 as positive active material. 15 Mn0. 05O2(NCM) powder was prepared. A crystalline azirodite-based solid electrolyte (Li6PS5Cl) was prepared as the solid electrolyte, polytetrafluoroethylene (PTFE, DuPont’s Teflon binder) was prepared as the binder, and carbon nanofiber (CNF) was prepared as the conductive material. The above positive active material : above solid electrolyte : above conductive material : above binder were mixed in a weight ratio of 84.2 : 11.5 : 2.9 : 1.4, and the mixture was molded into a sheet shape to produce a positive sheet. The prepared positive sheet was pressed onto a positive current collector made of carbon-coated aluminum foil with a thickness of 18 μm to produce a positive electrode.
[0273] (2) Preparation of a solid electrolyte layer
[0274] An azirodite-type solid electrolyte Li6PS5Cl was mixed with an isobutylyl isobutylate binder to which an acrylate-based polymer was added. At this time, the mixing weight ratio of the solid electrolyte to the binder was 98.7:1.3, and the solid content of the mixture was 50 wt%. Subsequently, the mixture was applied to a release polytetrafluoroethylene film and dried at 60°C for 2 hours to produce a solid electrolyte layer with a thickness of 100 μm.
[0275] (3) Preparation of the cathode
[0276] A stainless steel (SUS) foil was prepared as the negative current collector. A nickel / copper alloy was prepared as the negative lead tab. As the negative active material, carbon black (CB) with a primary particle size of about 30 nm and silver (Ag) particles with an average particle diameter of about 60 nm were prepared.
[0277] 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 a PVDF binder (Kureha # 9300) was added to prepare a mixed solution. A cathode slurry was prepared by stirring the mixed solution while gradually adding NMP to the prepared mixed solution. The prepared cathode slurry was applied to a SUS sheet using a bar coater, dried at 80°C for 10 minutes, and then vacuum dried at 40°C for 10 hours to produce a cathode laminate. The cathode was manufactured by applying pressure to the prepared cathode laminate.
[0278] (4) Manufacturing of electrode assembly
[0279] A unit cell was manufactured by stacking the cathode manufactured in step (3), the solid electrolyte layer manufactured in step (2), and the anode manufactured in step (1) in order. A total of 10 unit cells were manufactured with the same configuration as the unit cell, and an electrode assembly was manufactured by stacking the 10 unit cells.
[0280] (5) Manufacturing of gaskets
[0281] A gasket was manufactured by injection molding using polyimide (PI) pellets. Specifically, PI pellets were heated at 350°C and injected into a mold to form the shape of a gasket, and then dried at 200°C to manufacture the gasket. At this time, the shape of the gasket was manufactured to be the same as that shown in Figures 8 and 10.
[0282] (6) Manufacturing of pouch-type solid-state batteries
[0283] In the above-manufactured electrode assembly, ten cathode substrate tabs (SUS foil) protruding from the cathode current collector of the cathode are pressed to form a cathode tab assembly, and the cathode and the cathode lead tabs (Cu / Ni alloy) are welded to electrically connect the cathode and the cathode lead tabs. Subsequently, ten anode substrate tabs (Al foil) protruding from the anode current collector of the anode are pressed to form an anode tab assembly, and the anode and the anode lead tabs (Al foil) are welded to electrically connect the anode and the anode lead tabs.
[0284] Subsequently, the positive electrode substrate tab and the negative electrode substrate tab were inserted respectively through the opening of the gasket, and gaskets were placed on both sides of the electrode assembly (see FIG. 7).
[0285] Subsequently, an electrode assembly in which the substrate tabs and lead tabs of the cathode and anode are respectively connected is sealed inside an aluminum pouch, which is an outer material, and the positive lead tab and the negative lead tab are protruded out of the aluminum pouch and subjected to a warm isostatic press (WIP) at 80°C at 500 MPa for 30 minutes to manufacture a pouch-type all-solid-state battery. The outer material included a polypropylene insulating layer with a thickness of 10 μm on the inside.
[0286]
[0287] Examples 1-2
[0288] A pouch-type all-solid-state battery was manufactured in the same manner as in Example 1-1, except that in step (4), the shape of the gasket was manufactured as shown in FIGS. 9 and 11.
[0289]
[0290] Comparative Example 1-1
[0291] A pouch-type all-solid-state battery was manufactured in the same manner as in Example 1-1, except that the gasket of step (4) was not used.
[0292]
[0293] Evaluation Example: Safety Evaluation
[0294] Safety was evaluated for the pouch-type all-solid-state batteries of Example 1-1 and Comparative Example 1-1 by checking for short circuits and heat generation.
[0295] Specifically, a pouch-type all-solid-state battery was placed in a chamber and heated from room temperature to 300°C. At this time, there was a temperature maintenance period of 30 minutes at 15°C intervals from room temperature to 300°C, and whether a short circuit or heat generation occurred was indicated as ○ (short circuit or heat generation occurred) or Χ (short circuit or heat generation did not occur).
[0296]
[0297] Separation Paragraph Occurrence Heat Generation Example 1-1XX Comparative Example 1-1OO
[0298]
[0299] As shown in Table 1 above, the pouch-type all-solid-state battery of Comparative Example 1-1 was damaged in the polypropylene insulation layer of the outer material at 150°C to 170°C, causing a short circuit, which resulted in a rapid rise in temperature, causing the cell to overheat and ignite. On the other hand, the pouch-type all-solid-state battery of Example 1-1 according to one embodiment of the present invention did not experience a short circuit and did not overheat or ignite, confirming that it possesses excellent safety.
[0300] Specifically, the pouch-type all-solid-state battery of Example 1-1 includes gaskets on both sides of an electrode assembly comprising at least one unit cell, thereby separating the pouch outer material and the substrate tab; thus, no short circuit or heat generation occurred even at high temperatures above the melting point (approx. 150°C to 170°C) of the polypropylene insulating layer. That is, in the pouch-type all-solid-state battery according to one embodiment of the present invention, even if the polypropylene insulating layer is lost at high temperatures, a short circuit does not occur because the pouch outer material and the substrate tab are separated. However, in Comparative Example 1-1, which does not include a gasket on one side of the electrode assembly, a short circuit and heat generation occurred as the polypropylene insulating layer was lost at high temperatures.
[0301]
[0302] Manufacturing of all-solid-state batteries (2)
[0303] Example 2-1
[0304] (1) Manufacturing of the anode
[0305] LiNi0.8Co0 as positive active material. 15 Mn0. 05 O2(NCM) powder was prepared. A crystalline azirodite-based solid electrolyte (Li6PS5Cl) was prepared as the solid electrolyte, polytetrafluoroethylene (PTFE, DuPont’s Teflon binder) was prepared as the binder, and carbon nanofiber (CNF) was prepared as the conductive material. The above positive active material : above solid electrolyte : above conductive material : above binder were mixed in a weight ratio of 84.2 : 11.5 : 2.9 : 1.4, and the mixture was molded into a sheet shape to produce a positive sheet. The prepared positive sheet was pressed onto a positive current collector made of carbon-coated aluminum foil with a thickness of 18 μm to produce a positive electrode.
[0306] (2) Preparation of a solid electrolyte layer
[0307] An azirodite-type solid electrolyte Li6PS5Cl was mixed with an isobutylyl isobutylate binder to which an acrylate-based polymer was added. At this time, the mixing weight ratio of the solid electrolyte to the binder was 98.7:1.3, and the solid content of the mixture was 50 wt%. Subsequently, the mixture was applied to a release polytetrafluoroethylene film and dried at 60°C for 2 hours to produce a solid electrolyte layer with a thickness of 100 μm.
[0308] (3) Preparation of the cathode
[0309] A stainless steel (SUS) foil was prepared as the negative current collector. A nickel / copper alloy was prepared as the negative lead tab. As the negative active material, carbon black (CB) with a primary particle size of about 30 nm and silver (Ag) particles with an average particle diameter of about 60 nm were prepared.
[0310] 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 a PVDF binder (Kureha #9300) was added to prepare a mixed solution. A cathode slurry was prepared by stirring the mixed solution while gradually adding NMP to the prepared mixed solution. The prepared cathode slurry was applied to a SUS foil using a bar coater, dried at 80°C for 10 minutes, and then vacuum dried at 40°C for 10 hours to produce a cathode laminate. The cathode was manufactured by applying pressure to the prepared cathode laminate.
[0311] (4) Manufacturing of electrode assembly
[0312] A unit cell was manufactured by stacking the cathode manufactured in step (3), the solid electrolyte layer manufactured in step (2), and the anode manufactured in step (1) in order. A total of 10 unit cells were manufactured with the same configuration as the unit cell, and an electrode assembly was manufactured by stacking the 10 unit cells.
[0313] (5) Manufacturing of gaskets
[0314] A gasket was manufactured by injection molding using polyimide (PI) pellets. Specifically, PI pellets were heated at 350°C and injected into a mold to form the shape of a gasket, and then dried at 200°C to manufacture the gasket. At this time, the shape of the gasket was manufactured to be the same as that shown in Fig. 18.
[0315] (6) Manufacturing of pouch-type solid-state batteries
[0316] The gasket manufactured above was placed on one side (the anode substrate tab side) of the electrode assembly manufactured above. At this time, the anode substrate tab was inserted through the opening.
[0317] Subsequently, ten positive substrate tabs (Al foil) protruding from the positive current collector of the positive electrode were bent and pressed to form a positive tab assembly, and the positive lead tabs (Al foil) were welded to electrically connect the positive electrode and the positive lead tabs. Subsequently, ten negative substrate tabs (SUS foil) protruding from the negative current collector of the negative electrode were bent and pressed to form a negative tab assembly, and the negative lead tabs (Cu / Ni alloy) were welded to electrically connect the negative electrode and the negative lead tabs.
[0318] Subsequently, an electrode assembly in which the substrate tabs and lead tabs of the cathode and anode are respectively connected is sealed inside an aluminum pouch which is an outer material, and the positive lead tab and the negative lead tab are protruded out of the aluminum pouch and subjected to a warm isostatic press (WIP) at 80°C at 500 MPa for 30 minutes to manufacture a pouch-type all-solid-state battery.
[0319]
[0320] Example 2-2
[0321] A pouch-type all-solid-state battery was manufactured in the same manner as in Example 2-1, except that in step (4), the shape of the gasket was manufactured as shown in Fig. 19.
[0322]
[0323] Comparative Example 2-1
[0324] A pouch-type all-solid-state battery was manufactured in the same manner as in Example 2-1, except that the gasket of step (4) was not used.
[0325]
[0326] Evaluation Example: Safety Evaluation
[0327] Safety was evaluated for the pouch-type all-solid-state batteries of Example 2-1 and Comparative Example 2-1 by checking for short circuits and heat generation.
[0328] Specifically, a pouch-type all-solid-state battery was placed in a chamber and heated from room temperature to 300°C. At this time, whether a short circuit or heat generation occurred was indicated as ○ (short circuit or heat generation occurred) or Χ (short circuit or heat generation did not occur).
[0329]
[0330] Separation Paragraph Occurrence Heat Generation Example 2-1XX Comparative Example 2-1OO
[0331]
[0332] As shown in Table 2 above, the pouch-type all-solid-state battery of Comparative Example 2-1 experienced a short circuit, causing the temperature at the positive and negative electrodes to rise rapidly, resulting in heat generation and ignition of the cell. On the other hand, the pouch-type all-solid-state battery of Example 2-1 according to one embodiment of the present invention did not experience a short circuit and did not generate heat or ignite, confirming that it possesses excellent safety.
[0333] FIG. 22 confirms the occurrence of a short circuit according to the evaluation example for the pouch-type all-solid-state batteries of Example 2-1 and Comparative Example 2-1. Referring to FIG. 22, the pouch-type all-solid-state battery of Example 2-1 did not experience a short circuit when exposed to heat from room temperature to 300°C, whereas the pouch-type all-solid-state battery of Comparative Example 2-1 experienced a short circuit (approx. 1,100 seconds) in which the Open Circuit Voltage (OCV) dropped rapidly to 0V when exposed to heat from room temperature to 300°C.
[0334] Specifically, in Example 2-1, by including a gasket on one side of the electrode assembly, no foreign substances were present inside the all-solid-state battery, so no short circuit or heat generation occurred even at high temperatures above the melting point of lithium (180°C). However, in Comparative Example 2-1, which did not include a gasket on one side of the electrode assembly, lithium melted and precipitated around foreign substances inside the all-solid-state battery, and lithium dendrites were formed. As a result, a short circuit and heat generation occurred.
[0335] Although preferred embodiments of the present invention have been described above, the present invention is not limited thereto and can be implemented with various modifications within the scope of the claims, the detailed description of the invention, and the attached drawings, and it is obvious that such modifications also fall within the scope of the present invention.
Claims
An electrode assembly comprising at least one unit cell; A recording tab extending from the above unit cell; A gasket disposed on one side of the electrode assembly and configured to surround the substrate tab; and It includes an outer casing that accommodates the above electrode assembly, and The above-mentioned tab includes a banding portion A extending at an angle from the unit cell and a tab assembly portion in which the banding portions A are gathered together. A solid-state battery in which the above gasket surrounds the above banding portion A, and the corner of the above gasket contacts the above exterior material. In Article 1, The above-mentioned tab is separated from the exterior material by the above-mentioned gasket, and An all-solid-state battery in which the separation distance between the above-mentioned material tab and the above-mentioned outer material is 100 μm or more. In Article 1, An all-solid-state battery in which the angle (α1) formed by the upper surface of the gasket with the exterior material is 20° to 70°, the angle (α3) formed by the lower surface of the gasket with the exterior material is 20° to 70°, and the angle (α2) formed by the front surface of the gasket with the exterior material is 10° to 60°. In Article 1, The above gasket is, A vertical extension extending vertically along the stacking direction of the electrode assembly; A first horizontal extension and a second horizontal extension extending horizontally from the above vertical extension; and It includes an opening formed between the first horizontal extension and the second horizontal extension, and A solid-state battery in which the bending portion A of the above-mentioned tab is inserted into the above-mentioned opening. In Article 4, The above vertical extension is, A first vertical extension connecting one end of the first horizontal extension and one end of the second horizontal extension; and It includes a second vertical extension connecting the other end of the first horizontal extension and the other end of the second horizontal extension, and A solid-state battery in which the width (b) in the vertical direction of the above opening decreases as it approaches the above tab collection part. In Article 1, The thickness (a) of the above gasket is 30 μm to 300 μm, and With respect to the vertical direction in which the above unit cells are stacked, the length (L2) of the gasket is equal to or smaller than the length (L1) of the electrode assembly, and The above gasket has a melting point of 200°C or higher and 1.0 × 10 -10 It includes a polymer having an electrical conductivity of S / m or less, and The above polymer comprises polytetrafluoroethylene (PTFE), polyimide (PI), polyetheretherketone (PEEK), polyphenylene sulfide (PPS), polyethylene terephthalate (PET), nylon 46 (Nylon 46), polycarbonate (PC), polyphenylsulfone (PPSU), or a combination thereof, in an all-solid-state battery. In Article 1, The above unit cell includes an anode, a solid electrolyte layer, and a cathode, and The above-mentioned substrate tab comprises an anode substrate tab protruding from the anode and a cathode substrate tab protruding from the cathode, in an all-solid-state battery. In Article 7, The above gasket includes a first gasket surrounding the anode substrate tab and a second gasket surrounding the cathode substrate tab, and A solid-state battery in which the thickness (a1) of the first gasket is the same as or different from the thickness (a2) of the second gasket. In Article 1, The above exterior material includes an insulating layer, and The insulating layer comprises polypropylene, polyethylene, polyester, polyamide, polyimide, polyvinyl chloride, polycarbonate, polystyrene, ethylene-vinyl acetate, or a combination thereof, in an all-solid-state battery. In Article 1, The above-described all-solid-state battery comprises a plurality of unit cells and a plurality of substrate tabs extending from the plurality of unit cells, and The above gasket surrounds the plurality of substrate tabs, an all-solid-state battery. An electrode assembly comprising at least one unit cell; A recording tab extending from the above unit cell; A gasket disposed on one side of the electrode assembly and configured to surround the substrate tab; and It includes an outer casing that accommodates the above electrode assembly, and The above-mentioned tab includes a connecting portion adjacent to the unit cell and a bending portion B extending at an angle from the connecting portion, and The above gasket is a solid-state battery that surrounds the above connection. In Article 11, The above gasket is, A vertical extension extending vertically along the stacking direction of the electrode assembly; A first horizontal extension and a second horizontal extension extending horizontally from the above vertical extension; and It includes an opening formed between the first horizontal extension and the second horizontal extension, and A solid-state battery in which the connecting portion of the above-mentioned tab is inserted into the above-mentioned opening. In Article 12, The above vertical extension includes a first vertical extension that contacts one side of the first and second horizontal extensions and a second vertical extension that contacts the other side of the first and second horizontal extensions, and The above gasket includes at least one opening, and The above-mentioned opening has a larger cross-sectional area than the above-mentioned substrate tab and has the same shape as the above-mentioned substrate tab, an all-solid-state battery. In Article 11, The above-mentioned tab is fixed by the above-mentioned gasket, and The above gasket comprises a polymer having a heat deflection temperature (HDT) of 200°C or higher, and The above polymer comprises polyimide (PI), polysulfone (PSU), polyetherimide (PEI), polyphenylene sulfide (PPS), polyetheretherketone (PEEK), or a combination thereof, in an all-solid-state battery. In Article 11, The above unit cell includes an anode, a solid electrolyte layer, and a cathode, and The above-mentioned substrate tab includes an anode substrate tab protruding from the anode and a cathode substrate tab protruding from the cathode, and The above gasket surrounds the connection portion of at least one of the positive electrode substrate tab and the negative electrode substrate tab, in an all-solid-state battery. A step of manufacturing an electrode assembly comprising at least one unit cell and a substrate tab extending from the unit cell; Step of manufacturing a gasket having an opening; and The method includes the step of placing the gasket on one side of the electrode assembly, A method for manufacturing an all-solid-state battery, comprising the step of bending the substrate tab and forming a tab assembly portion before or after the step of placing the gasket. In Article 16, The above-mentioned tab includes a banding portion A extending at an angle from the unit cell and a tab assembly portion in which the banding portions A are gathered together. A method for manufacturing an all-solid-state battery, wherein, after bending the above-mentioned base tab and forming a tab assembly portion, the above-mentioned base tab is inserted into the opening of the above-mentioned gasket and the above-mentioned gasket is placed on one side of the electrode assembly. In Article 17, It includes a step of sealing with exterior materials, A method for manufacturing an all-solid-state battery, wherein the above gasket surrounds the above-mentioned substrate tab and separates the above-mentioned substrate tab from the above-mentioned outer material. In Article 16, The above-mentioned tab includes a connecting portion adjacent to the unit cell and a bending portion B extending at an angle from the connecting portion, and A method for manufacturing an all-solid-state battery, wherein the above gasket is placed to fix the above-mentioned substrate tab, and then the above-mentioned substrate tab is bent to form a tab assembly. In Article 19, A method for manufacturing an all-solid-state battery in which the above gasket surrounds the connecting portion of the above-mentioned substrate tab to secure the above-mentioned substrate tab.