All-solid-state batteries and their manufacturing methods

Abstract

The disclosed all-solid-state battery includes: a solid electrolyte layer; a first electrode unit layer and a second electrode unit layer, which are opposite to each other and the solid electrolyte layer is located between the first electrode unit layer and the second electrode unit layer; a first external electrode connected to the second electrode unit layer; and a first edge portion disposed between the first electrode unit layer and the first external electrode, wherein the first electrode unit layer includes a first current collector and a first boundary portion, the first boundary portion being disposed between the first current collector and the first edge portion and including a first active material.

Description

Technical Field

[0001] This disclosure relates to an all-solid-state battery and a method for manufacturing the same. Background Technology

[0002] With the increasing prevalence of portable electronic devices used for extended periods, there is a growing need for batteries with higher capacity, and with the proliferation of wearable devices, ensuring battery safety is paramount. Therefore, the development of all-solid-state batteries, which use solid electrolytes instead of liquid electrolytes, is actively underway.

[0003] All-solid-state batteries use a solid electrolyte instead of the conventional liquid electrolyte, which greatly reduces the risk of explosion caused by the flammability of liquid electrolytes. Furthermore, because all-solid-state batteries do not use a liquid electrolyte, they can operate stably even in harsh environments with relatively high temperatures and pressures. Additionally, since the batteries can be stacked without separate cooling, high energy density can be achieved within the same volume, making them promising for future applications. Moreover, small all-solid-state batteries are being developed in board-mountable forms and have great potential in areas where miniaturization is important, such as wearable devices.

[0004] Traditionally, in the manufacture of all-solid-state batteries, active materials are printed between the current collectors to enhance electrode performance.

[0005] Due to the difference in physical properties between the active material and the current-collecting conductive material, the above structure may cause the current-collecting layer to be exposed outside the positive electrode layer after sintering. The current-collecting layer exposed after sintering has a high risk of contact with the surrounding electrodes, which could lead to a short circuit. Summary of the Invention

[0006] Technical issues One aspect of this embodiment aims to provide an all-solid-state battery capable of preventing short-circuit defects.

[0007] Solution to the problem An all-solid-state battery according to some embodiments of the present disclosure may include: a solid electrolyte layer; a first electrode unit layer and a second electrode unit layer, opposite to each other and the solid electrolyte layer being located between the first electrode unit layer and the second electrode unit layer; a first external electrode connected to the second electrode unit layer; and a first edge portion disposed between the first electrode unit layer and the first external electrode, wherein the first electrode unit layer includes a first current collector and a first boundary portion, the first boundary portion being disposed between the first current collector and the first edge portion and including a first active material.

[0008] In addition, the first boundary portion can prevent the first current collector from contacting the first edge portion.

[0009] In addition, the first electrode unit layer may be disposed on the first current collector and on the first boundary portion.

[0010] In addition, the first active material layer can be made of the same material as the first boundary portion.

[0011] Furthermore, the first active material layer and the first boundary portion can satisfy the following conditional expression: [Conditional Expression] 0.01%≤L2 / L1≤0.1%, in, L1: The length of the first active material layer L2: The length of the first boundary portion.

[0012] In addition, the first active material can be a positive electrode active material.

[0013] In addition, the first boundary portion may also include aluminum oxide (Al2O3) and an electrolyte.

[0014] In addition, the first boundary portion may also include insulating material.

[0015] In addition, the all-solid-state battery may also include: a second external electrode connected to the first electrode unit layer; and a second edge portion disposed between the second electrode unit layer and the second external electrode, wherein the second electrode unit layer may include a second current collector and a second boundary portion disposed between the second current collector and the second edge portion.

[0016] In addition, the second boundary portion may include a negative electrode active material.

[0017] In addition, the second boundary portion can prevent the second current collector from contacting the second edge portion.

[0018] In addition, the second electrode unit layer may also include a second active material layer disposed on the second current collector and the second boundary portion, and the second active material layer is made of the same material as the second boundary portion.

[0019] According to another embodiment, an all-solid-state battery may include: a laminate including a solid electrolyte layer, a positive electrode layer and a negative electrode layer, wherein the solid electrolyte layer is disposed between the positive electrode layer and the negative electrode layer; a first external electrode disposed outside the laminate; and a first edge portion disposed between the positive electrode layer and the first external electrode, wherein the positive electrode layer includes a positive electrode active material layer, a positive electrode current collector and a first boundary portion, the positive electrode current collector is disposed on the positive electrode active material layer, and the first boundary portion is disposed between the positive electrode current collector and the first edge portion and includes the positive electrode active material.

[0020] In addition, the first boundary portion can prevent the positive current collector from contacting the first edge portion.

[0021] In addition, the positive electrode active material layer and the first boundary portion can be made of the same material.

[0022] Additionally, the all-solid-state battery may include: a second external electrode, opposite to the first external electrode and the laminated body is located between the first external electrode and the second external electrode; and a second edge portion, disposed between the negative electrode layer and the second external electrode, wherein the negative electrode layer may include a negative electrode active material layer, a negative electrode current collector and a second boundary portion, the negative electrode current collector being disposed on the negative electrode active material layer, and the second boundary portion being disposed between the negative electrode current collector and the second edge portion.

[0023] In addition, the second boundary portion can be made of the same material as the negative electrode active material layer.

[0024] A method for manufacturing an all-solid-state battery according to an embodiment includes: coating an active material paste onto a solid electrolyte layer to form an active material layer; coating an insulating paste onto the solid electrolyte layer to form a first edge portion; coating a conductive paste onto the active material layer to form a current collector; and forming a boundary portion by coating a paste for a boundary portion onto a portion of the active material layer where the current collector is not formed.

[0025] The method of manufacturing the all-solid-state battery may further include forming a second edge layer by applying insulating paste to the edge layer of the first layer, wherein the entire second edge layer may be formed to be spaced apart from the entire current collector by the boundary portion.

[0026] In addition, the paste used for the boundary portion can be made from the same material as the active material paste.

[0027] Beneficial effects of the invention According to at least one of the embodiments, a boundary portion is formed between the current collector and the edge portion, thereby preventing short-circuit defects caused by the current collector being exposed to the outside of the positive electrode layer.

[0028] However, the embodiments of this disclosure are not limited to the above, and various extensions can be made within the scope of the technical concepts included in this disclosure. Attached Figure Description

[0029] Figure 1 This is a perspective view showing an all-solid-state battery according to an embodiment.

[0030] Figure 2 It is shown Figure 1 A three-dimensional diagram of the stacked structure of an all-solid-state battery.

[0031] Figure 3 It is along Figure 1 The cross-sectional view taken from line III-III' in the diagram.

[0032] Figure 4 It is shown Figure 3 A partial 3D view of part A.

[0033] Figure 5 This is a partial perspective view showing a portion of the positive electrode layer according to an embodiment.

[0034] Figure 6 yes Figure 5 An exploded 3D diagram.

[0035] Figure 7 It is along Figure 4 A partial cross-sectional view taken from line VII-VII'.

[0036] Figure 8 This is a cross-sectional view showing the length of the positive electrode active material layer and the first boundary portion.

[0037] Figure 9 It is shown Figure 3 A partial 3D view of part B.

[0038] Figure 10 It is along Figure 9 A cross-sectional view taken by line X-X'.

[0039] Figures 11 to 17 A method for manufacturing the positive electrode cell layer of an all-solid-state battery according to an embodiment is shown.

[0040] Figure 18 This is a partial perspective view showing a portion of the negative electrode layer of an all-solid-state battery according to another embodiment.

[0041] Figure 19 yes Figure 18 An exploded 3D diagram.

[0042] Figure 20 It is along Figure 18 A partial cross-sectional view taken from line XX-XX' in the diagram. Detailed Implementation

[0043] The present disclosure will now be described in detail with reference to the accompanying drawings, in which embodiments of the disclosure are illustrated. The drawings and description are to be considered illustrative rather than restrictive in nature. Throughout the specification, the same reference numerals denote the same elements. In the drawings, some components are shown enlarged, omitted, or schematically, and the dimensions of the individual components do not perfectly reflect their actual dimensions.

[0044] The accompanying drawings are intended only to facilitate understanding of the embodiments disclosed in this specification, and it should be understood that the technical concepts disclosed herein are not limited to the drawings, but include all variations, equivalents and alternatives within the scope of the concepts and techniques disclosed herein.

[0045] Although terms such as "first" and "second" are used to explain various constituent elements, the constituent elements are not limited to these terms. These terms are only used to distinguish one constituent element from another.

[0046] Furthermore, it will be understood that when an element such as a layer, film, region, or substrate is referred to as being "on" another element, the element may be directly on the other element, or there may be an intermediate element present. In contrast, when an element is referred to as being "directly on" another element, there is no intermediate element present. Additionally, when an element is referred to as being "on" or "above" a reference element, the element may be located above or below the reference element, and is not necessarily referred to as being "on" or "above" in a direction opposite to the direction of gravity.

[0047] Throughout this specification, the terms “comprising” or “having” are intended to specify the presence of the stated features, integers, steps, operations, constituent elements, components, or combinations thereof, without excluding the presence or addition of one or more other features, integers, steps, operations, constituent elements, components, and / or groups thereof. Therefore, unless explicitly stated otherwise, the words “comprising” and variations such as “including” or “having” will be understood to imply inclusion of the stated constituent elements but not exclusion of any other constituent elements.

[0048] Furthermore, throughout the specification, the phrase "in a plan view" or "on a plane" indicates the target portion as viewed from the top, and the phrase "in a cross-sectional view" or "on a cross-section" describes the cross-section formed by vertically cutting the target portion as viewed from the side.

[0049] Throughout the specification, the term "connection" may refer not only to a direct connection between two or more constituent components, but also to an indirect connection between two or more constituent components through another constituent component, to an electrical connection and a physical connection between two or more components, or to two or more constituent components represented by different names but combined by position or function.

[0050] When describing the all-solid-state battery in this specification, the direction along which the main components of the all-solid-state battery are stacked is defined as the "stack direction," but this can also be the "thickness direction." In addition, a direction parallel to a plane perpendicular to the stack direction can be defined as a "planar direction," and the planar direction can include a "first direction" and a "second direction" that are orthogonal to each other.

[0051] Figure 1This is a perspective view showing an all-solid-state battery according to an embodiment. Figure 2 It is shown Figure 1 A three-dimensional diagram of the stacked structure of an all-solid-state battery, and Figure 3 It is along Figure 1 The cross-sectional view taken from line III-III' in the diagram.

[0052] Reference Figure 1 , Figure 2 and Figure 3 According to an embodiment, the all-solid-state battery 10 includes a stack 100, a first external electrode 300, and a second external electrode 400.

[0053] First, in order to clearly describe this embodiment, directions are defined. The L-axis, W-axis and T-axis shown in the figures refer to the axes representing the length direction, width direction and thickness direction of the all-solid-state battery 10, respectively.

[0054] The thickness direction (T-axis direction) can be a direction perpendicular to the wide surface (main surface) of the sheet component. For example, the thickness direction (T-axis direction) can be used as the same concept as the direction along which the components of the stacked laminate 100 are located.

[0055] The length direction (L-axis direction) is parallel to the wide surface (main surface) of the sheet assembly and can be a direction that intersects (or is perpendicular to) the thickness direction (T-axis direction). For example, the length direction (L-axis direction) can be the direction along which the first external electrode 300 and the second external electrode 400 are opposite each other.

[0056] The width direction (W-axis direction) is parallel to the wide surface (main surface) of the sheet component, and can be a direction that intersects (or is perpendicular to) the thickness direction (T-axis direction) and the length direction (L-axis direction).

[0057] The laminate 100 may have a generally hexahedral shape, but this embodiment is not limited to this. Due to shrinkage during sintering, the laminate 100 may not have a perfectly hexahedral shape, but may have a generally hexahedral shape. For example, the laminate 100 may have a generally cuboid shape, but the portions corresponding to the corners or vertices may have a rounded shape.

[0058] For better understanding and ease of description, in this embodiment, surfaces that are opposite to each other in the length direction (L-axis direction) are defined as the first surface S1 and the second surface S2, and surfaces that are opposite to each other in the width direction (W-axis direction) and connect the first surface S1 and the second surface S2 are defined as the third surface S3 and the fourth surface S4. Surfaces that are opposite to each other in the thickness direction (T-axis direction) and connect the first surface S1 and the second surface S2 are defined as the fifth surface S5 and the sixth surface S6.

[0059] Therefore, the first direction along which the first surface S1 and the second surface S2 are opposite to each other can be the length direction (L-axis direction), and the second and third directions perpendicular to the first direction and perpendicular to each other can be the thickness direction (T-axis direction) and the width direction (W-axis direction), respectively, or they can be the width direction (W-axis direction) and the thickness direction (T-axis direction), respectively. In this embodiment, for better understanding and ease of description, the length direction (L-axis direction), the width direction (W-axis direction), and the thickness direction (T-axis direction) are defined as the first direction, the second direction, and the third direction, respectively. However, this is only for better understanding and ease of description, and the first direction, the second direction, and the third direction are not limited thereto. The first direction, the second direction, and the third direction intersect each other (or are perpendicular to each other).

[0060] The length of the laminate 100 can refer to the maximum length of a plurality of line segments parallel to the length direction (L-axis direction) and thickness direction (T-axis direction) of the laminate 100 at its central portion in the width direction (W-axis direction), as shown in the cross-sectional photographs of the central portion in the width direction (W-axis direction). In the following text, the length direction (L-axis direction) - thickness direction (T-axis direction) cross-section refers to a cross-section where the length direction (L-axis direction) and thickness direction (T-axis direction) intersect (or are perpendicular to each other). Furthermore, the length of the laminate 100 can also refer to the minimum length of a plurality of line segments parallel to the length direction (L-axis direction) and connecting the two outermost boundary lines parallel to the length direction (L-axis direction) as shown in the cross-sectional photographs of the laminate 100. Furthermore, the length of the laminate 100 can refer to the arithmetic mean of the lengths of at least two line segments among the two outermost boundary lines that are opposite each other in the length direction (L-axis direction) and parallel to the length direction (L-axis direction) of the laminate 100 shown in the above cross-sectional photograph.

[0061] The thickness of the laminate 100 can refer to the maximum value among the lengths of multiple line segments that are opposite to the two outermost boundary lines in the thickness direction (T-axis direction) of the laminate 100 at the central part in the width direction (W-axis direction) and the thickness direction (T-axis direction).

[0062] Furthermore, the thickness of the laminate 100 can refer to the minimum length of a plurality of line segments that connect the laminate 100 shown in the above cross-sectional photograph, are opposite to the two outermost boundary lines in the thickness direction (T-axis direction), and are parallel to the thickness direction (T-axis direction). Alternatively, the thickness of the laminate 100 can refer to the arithmetic mean of the lengths of at least two line segments that connect the laminate 100 shown in the above cross-sectional photograph, are opposite to the two outermost boundary lines in the thickness direction (T-axis direction), and are parallel to the thickness direction (T-axis direction).

[0063] The thickness of the laminate 100 can refer to the maximum length of a cross-section (length direction - width direction - W direction) at the central portion of the ceramic body 10 in the thickness direction (T-axis direction) compared to the length direction (L-axis direction) - width direction (W-axis direction). This thickness is determined by an optical microscope or SEM image of the cross-section, which connects the two outermost boundary lines of the laminate 100 shown in the cross-section and is parallel to the width direction (W-axis direction). In the following text, the length direction (L-axis direction) - width direction (W-axis direction) cross-section refers to a cross-section where the length direction (L-axis direction) and the width direction (W-axis direction) intersect (or are perpendicular to each other). Furthermore, the width of the laminate 100 can refer to the minimum length of a cross-section, which connects the two outermost boundary lines of the laminate 100 shown in the cross-section and is parallel to the width direction (W-axis direction). Furthermore, the width of the laminate 100 can refer to the arithmetic mean of the lengths of at least two line segments among the two outermost boundary lines that are opposite each other in the width direction (W-axis direction) and parallel to the width direction (W-axis direction) of the laminate 100 shown in the above cross-sectional photograph.

[0064] The laminate 100 may include a solid electrolyte layer 110, a positive electrode unit layer 130, a negative electrode unit layer 150, an upper protective layer 180, and a lower protective layer 190. The positive electrode unit layer 130 and the negative electrode unit layer 150 may be defined as a first unit layer and a second unit layer, or they may be defined as a second unit layer and a first unit layer.

[0065] Multiple solid electrolyte layers 110, multiple positive electrode unit layers 130, and multiple negative electrode unit layers 150 may exist respectively. The positive electrode unit layers 130 and negative electrode unit layers 150 may be stacked alternately in the thickness direction (T-axis direction), with the solid electrolyte layer 110 situated between the positive electrode unit layers 130 and the negative electrode unit layers 150. The laminate 100 may have a stacked structure of solid electrolyte layer 110 / negative electrode unit layer 150 / solid electrolyte layer 110 / positive electrode unit layer 130. That is, the positive electrode unit layers 130 and negative electrode unit layers 150 may be opposite each other, with the solid electrolyte layer 110 situated between the positive electrode unit layers 130 and the negative electrode unit layers 150. Based on the solid electrolyte layer 110, the positive electrode unit layer 130 may be disposed on one surface of the solid electrolyte layer 110, and the negative electrode unit layer 150 may be disposed on the other surface of the solid electrolyte layer 110.

[0066] Solid electrolyte layer 110 includes a solid electrolyte. The solid electrolyte can serve as a channel for lithium (Li) ions. The solid electrolyte included in solid electrolyte layer 110 may include a glass-ceramic electrolyte containing lithium halides (such as halogens like LiX, where X is F, Br, Cl, or I). Glass-ceramic (or microcrystalline glass) indicates the crystallographic coexistence of amorphous and crystalline elements. For example, it can indicate the crystallographic coexistence of amorphous and crystalline substances when peaks and halo peaks are observed in X-ray diffraction or electron beam diffraction. Therefore, a glass-ceramic electrolyte is an electrolyte in which amorphous and crystalline elements are mixed due to partial crystallization through sintering.

[0067] Glass-ceramic electrolytes may contain a mixture of amorphous and two or more types of crystalline materials. Additionally, the crystalline material included in the glass-ceramic electrolyte may include a lithium compound crystalline phase containing lithium.

[0068] When a glass-ceramic electrolyte is included, high ionic conductivity can be achieved after sufficient densification is achieved through sintering.

[0069] The glass-ceramic electrolyte may include at least one selected from the group consisting of lithium (Li) oxide, boron (B) oxide, silicon (Si) oxide, aluminum (Al) oxide, gallium (Ga) oxide, phosphorus (P) oxide, germanium (Ge) oxide, magnesium (Mg) oxide, and lithium chloride (LiCl). According to some embodiments, the glass-ceramic electrolyte may include lithium (Li) oxide, boron (B) oxide, silicon (Si) oxide, aluminum (Al) oxide, gallium (Ga) oxide, phosphorus (P) oxide, germanium (Ge) oxide, magnesium (Mg) oxide, and lithium chloride (LiCl). As a specific example, the glass-ceramic electrolyte may include Li₂O-B₂O₃-SiO₂-P₂O₅-GeO₂-LiCl.

[0070] The solid electrolyte included in the solid electrolyte layer 110 may include a lithium borosilicate-based electrolyte (hereinafter, referred to as an LBSO-based electrolyte). The LBSO-based electrolyte is an electrolyte in a glassy state. Glass is amorphous crystallographically and may exhibit a hump peak in X-ray diffraction or electron beam diffraction. When the solid electrolyte layer 110 includes the LBSO-based electrolyte, the sintering temperature can be reduced and the amorphous state can be maintained during sintering. Therefore, high ionic conductivity can be achieved, and the advantage of not reacting highly with the electrode can be ensured. The LBSO-based electrolyte may include at least one selected from the group consisting of lithium (Li), boron (B), silicon (Si), aluminum (Al), phosphorus (P), germanium (Ge), and sulfur (S). According to some embodiments, the LBSO-based electrolyte may include lithium (Li), boron (B), silicon (Si), aluminum (Al), phosphorus (P), germanium (Ge), and sulfur (S).

[0071] In addition, the solid electrolyte included in the solid electrolyte layer 110 may be one or more types selected from the group consisting of garnet type, NASICON type, LISICON type, perovskite type, and LiPON type.

[0072] The garnet-type solid electrolyte may be represented by Li 1+x , 2-x , 0.3 , 1.7 , 2-x , 1.3 , 1+x , x , x , 2-x La b Zr c O 12 such as lithium lanthanum zirconium oxide (LLZO) represented by Li7La3Zr2O 12 (. The NASICON-type solid electrolyte may be represented by Ti introduced into Li 1+x Al x M 2-x (PO4)3 (LAMP) (0 < x < 2, where M is Zr, Ti, or Ge) type compound by Li 1+x Al x Ti 2-x (PO4)3 (0 < x < 1) represented by lithium aluminum titanium phosphate (LATP), lithium aluminum germanium phosphate (LAGP) represented by Li 1+x Al x Ge 2-x (PO4)3 (0 < x < 1) (such as Li 1.3 Al 0.3 Ti 1.7 (PO4)3, etc.) and / or lithium zirconium phosphate (LZP) (LiZr2(PO4)3).

[0073] In addition, the LISICON-type solid electrolyte may be represented by xLi3AO4-(1-x)Li4BO4 (where A is P, As, or V, etc., and B is Si, Ge, or Ti, etc.) and includes Li4Zn(GeO4)4, Li10 GeP2O 12 (LGPO), Li 3.5 Si 0.5 P 0.5 O4, Li 10.42 Si(Ge) 1.5 P 1.5 Cl 0.08 O 11.92 and other solid - solution oxides such as those of Li 4-x M 1-y M' y solid - solution sulfides such as Li2S - P2S5, Li2S - SiS2, Li2S - SiS2 - P2S5, Li2S - GeS2, etc., represented by Li2S - M'2S5 (where M is Si, Ge, and M' is P, Al, Zn, Ga).

[0074] The perovskite - type solid electrolyte can be represented by lithium lanthanum titanium oxide (LLTO) such as Li 3x La 2 / 3-x □ 1 / 3-2x TiO3 (0 < x < 0.16, □ is a vacancy) (such as Li 1 / 8 La 5 / 8 TiO3, etc.), and the LiPON - type solid electrolyte can refer to nitrides such as lithium phosphorus oxynitride (such as Li 2.8 PO 3.3 N 0.46 etc.).

[0075] For example, the minimum length of the solid - electrolyte layer 110 in the thickness direction (T - axis direction) can be greater than or equal to 28 μm.

[0076] The upper protective layer 180 and the lower protective layer 190 can be the outermost layers provided on the fifth surface S5 and the sixth surface S6 of the laminate 100, respectively. That is, the upper protective layer 180 can be the outermost layer on the fifth surface S5 of the laminate 100, and the lower protective layer 190 can be the outermost layer on the sixth surface S6 of the laminate 100. The upper protective layer 180 and the lower protective layer 190 can improve the moisture - proof reliability by preventing moisture from penetrating into the laminate 100. In addition, the upper protective layer 180 and the lower protective layer 190 can prevent damage to the laminate 100 caused by physical impact or chemical impact.

[0077] Both the upper protective layer 180 and the lower protective layer 190 can be insulating layers made of insulating materials (materials that do not have electronic conductivity (or ionic conductivity)).

[0078] The upper protective layer 180 and the lower protective layer 190 may comprise, but are not limited to, ceramic materials (such as alumina (Al2O3), aluminum nitride (AlN), beryllium oxide (BeO), boron nitride (BN), silicon (Si), silicon carbide (SiC), silicon dioxide (SiO2), silicon nitride (Si3N4), gallium arsenide (GaAs), gallium nitride (GaN), barium titanate (BaTiO3), zirconium dioxide (ZrO2), mixtures thereof, oxides and / or nitrides thereof) or any other suitable ceramic material. Additionally, the upper protective layer 180 and the lower protective layer 190 may optionally comprise the aforementioned solid electrolyte, and may comprise one or more types of solid electrolytes, but are not limited to these.

[0079] The first external electrode 300 and the second external electrode 400 are disposed on the outer surface of the laminate 100. For example, the first external electrode 300 may be an external positive electrode, and the second external electrode 400 may be an external negative electrode. However, the first external electrode 300 and the second external electrode 400 are not limited thereto.

[0080] A first external electrode 300 is disposed on a first surface S1, and a second external electrode 400 is disposed on a second surface S2. The first external electrode 300 is in contact with the positive electrode layer 131 on the first surface S1 of the laminate 100, and the second external electrode 400 is in contact with the negative electrode layer 151 on the second surface S2 of the laminate 100. The first external electrode 300 may cover the first surface S1 of the laminate 100 and be connected to the positive electrode layer 131. The second external electrode 400 may cover the second surface S2 of the laminate 100 and be connected to the negative electrode layer 151.

[0081] For example, the first external electrode 300 may extend from the first surface S1 of the laminate 100 to the third surface S3, the fourth surface S4, the fifth surface S5, and the sixth surface S6 to partially cover each surface. Similarly, the second external electrode 400 may extend from the second surface S2 of the laminate 100 to the third surface S3, the fourth surface S4, the fifth surface S5, and the sixth surface S6 to partially cover each surface.

[0082] As another example, the first external electrode 300 may extend from the first surface S1 to the fifth surface S5 or the sixth surface S6 to partially cover the respective surface, and the second external electrode 400 may extend from the second surface S2 to the fifth surface S5 or the sixth surface S6 to partially cover the respective surface.

[0083] The first external electrode 300 may include a first electrode unit layer 310 and a first plating layer 320, and the second external electrode 400 may include a second electrode layer 410 and a second plating layer 420.

[0084] The above reference Figure 1 and Figure 3The first external electrode 300 and the second external electrode 400 are described for distinction purposes only, and their construction is not limited by terminology. For example, in another description, the first external electrode may contact the second surface S2, and the second external electrode may contact the first surface S1.

[0085] In the following text, reference will be made to Figure 3 and Figure 4 A first unit layer is described. The first unit layer includes a first electrode unit layer and a first edge portion. The first electrode unit layer may include a first active material layer, a first current collector, and a first boundary layer. For better understanding and ease of description, the first unit layer will be described as a positive electrode unit layer 130, and the first electrode unit layer will be described as a positive electrode layer 131.

[0086] Figure 4 It is shown Figure 3 A partial 3D view of part A.

[0087] Reference Figure 3 and Figure 4 The positive electrode unit layer 130 may be formed on one surface of the solid electrolyte layer 110. The positive electrode unit layer 130 may include a positive electrode layer 131 and a first edge portion 133. The positive electrode layer 131 is the portion responsible for electron conduction, and one end is exposed to the first surface S1 of the laminate 100 and in contact with the first external electrode 300.

[0088] The first edge portion 133 is the region of the positive electrode unit layer 130 excluding the positive electrode layer 131. The first edge portion 133 may be disposed on the second surface S2, the third surface S3, and the fourth surface S4. That is, the first edge portion 133 is the portion parallel to the positive electrode layer 131 in both the length direction (L-axis direction) and the width direction (W-axis direction). The first edge portion 133 may be formed to contact two surfaces of the positive electrode layer 131 along the length direction (L-axis direction) and to contact one surface of the positive electrode layer 131 along the width direction (W-axis direction). Therefore, the first edge portion 133 may be exposed to the second surface S2, the third surface S3, and the fourth surface S4 of the laminate 100. In other words, the first edge portion 133 may be formed to surround the positive electrode layer 131 in three directions. For example, the first edge portion 133 may have a hyperbolic shape.

[0089] The first edge portion 133 may be formed using an insulating material that is not electronically conductive (or ionicly conductive).

[0090] The first edge portion 133 may include a ceramic material. For example, the first edge portion 133 may include at least one selected from the group consisting of alumina (Al2O3), aluminum nitride (AlN), beryllium oxide (BeO), boron nitride (BN), silicon (Si), silicon carbide (SiC), silicon dioxide (SiO2), silicon nitride (Si3N4), gallium arsenide (GaAs), gallium nitride (GaN), barium titanate (BaTiO3), zirconium dioxide (ZrO2), mixtures thereof, oxides and / or nitrides thereof, or any other suitable ceramic material.

[0091] Additionally, the first edge portion 133 may include one or more types of solid electrolytes, and may optionally include the aforementioned solid electrolytes.

[0092] The first edge portion 133 may include a material with low ionic conductivity and low electronic conductivity (such as an insulating material). Additionally, a material with an ionic conductivity (or electronic conductivity) approximating that of the solid electrolyte may be present in the first edge portion 133. For example, if the first edge portion 133 includes a material with an ionic conductivity (or electronic conductivity) approximating that of the solid electrolyte, this material may be the same as or a different material from the solid electrolyte in other regions.

[0093] As another example, the first edge portion 133 may simultaneously include an insulating material and a material having an ionic conductivity (or electronic conductivity) similar to that of a solid electrolyte.

[0094] The height difference between the solid electrolyte layer 110 and the positive electrode layer 131 can be resolved by forming a portion of the side surface of the positive electrode unit layer 130 that is parallel to the positive electrode layer 131 in both the length direction (L-axis direction) and the width direction (W-axis direction). Therefore, the occurrence of interlayer delamination or bending due to sintering can be suppressed.

[0095] The first edge portion 133 can be formed by coating an insulating paste onto the solid electrolyte layer 110. Figure 3 The boundary between the first edge portion 133 and the solid electrolyte layer 110 is clearly shown in the figure. However, when the first edge portion 133 and the solid electrolyte layer 110 are formed using the same material, it may be difficult to distinguish the boundary in the laminate after sintering.

[0096] Figure 5 This is a partial perspective view showing a portion of the positive electrode layer 131 of an all-solid-state battery 10 according to some embodiments. Figure 6 yes Figure 5 The exploded stereoscopic view, and Figure 7 It is along Figure 4A partial cross-sectional view taken from line VII-VII'.

[0097] Reference Figure 4 , Figure 5 , Figure 6 and Figure 7 The positive electrode layer 131 may include a positive electrode current collector 1313, a positive electrode active material layer 1311, and a first boundary portion 1314.

[0098] One end of the positive current collector 1313 may be exposed along the direction of the first surface S1. For example, the positive current collector 1313 may be formed as a plate-like member or a thin member. As another example, the positive current collector 1313 may be formed using a porous material such as a network or mesh.

[0099] The positive current collector 1313 may be a porous metal plate made of stainless steel, and may include at least one selected from the group consisting of nickel (Ni), copper (Cu), tin (Sn), aluminum (Al) and alloys thereof. Additionally, the positive current collector 1313 may be coated with an oxidation-resistant metal or alloy film to prevent oxidation.

[0100] The positive electrode current collector 1313 can be formed as a carbon substrate-like component, a carbon-based thin component, a carbon-based linear component, or a carbon-based circular component. The positive electrode current collector 1313 may include a conductive carbon-based material. For example, the conductive carbon material may include conductive fibers (such as graphite, carbon nanotubes (CNTs) or vapor-grown carbon fibers (VGCF)) or conductive carbon (such as carbon black).

[0101] The positive current collector 1313 may include one or more types of solid electrolytes.

[0102] The first boundary portion 1314 may be provided on the side surface of the positive current collector 1313 in the length direction (L-axis direction) and width direction (W-axis direction). The first boundary portion 1314 may be provided between the positive current collector 1313 and the first edge portion 133. The first boundary portion 1314 may contact the two ends of the positive current collector 1313 in the width direction (W-axis direction). In addition, the first boundary portion 1314 may contact the end of the positive current collector 1313 near the second surface S2 among the two ends in the length direction (L-axis direction). The first boundary portion 1314 may be configured to surround the ends of the positive current collector 1313 in the length direction (L-axis direction) and width direction (W-axis direction) other than the end exposed to the first surface S1. That is, the first boundary portion 1314 may be configured to contact one of the two ends of the positive current collector 1313 provided in the length direction (L-axis direction) and the two ends provided in the width direction (W-axis direction). At the end of the positive current collector 1313, the end that does not contact the first boundary portion 1314 may be exposed to the first surface S1 of the laminate 100 and may contact the first external electrode 300. Since the first boundary portion 1314 is disposed between the positive current collector 1313 and the first edge portion 133, the positive current collector 1313 and the first edge portion 133 are spaced apart from each other. In other words, the first boundary portion 1314 prevents the positive current collector 1313 from contacting the first edge portion 133.

[0103] Based on the first edge portion 133, the first boundary portion 1314 can be configured to contact the inner surface of the first edge portion 133 along both the length direction (L-axis direction) and the width direction (W-axis direction). Therefore, the first boundary portion 1314 can be formed to surround the positive electrode current collector 1313 in three directions. Since the positive electrode current collector 1313 contacts and surrounds the positive electrode current collector 1313 on the third surface S3, the second surface S2, and the fourth surface S4, the entire positive electrode current collector 1313 and the entire first edge portion 133 can be separated by the first boundary portion 1314. In other words, the first boundary portion 1314 can prevent the positive electrode current collector 1313 from contacting the first edge portion 133.

[0104] The first boundary portion 1314 includes a positive electrode active material. The first boundary portion 1314 may be made of the same material as the positive electrode active material layer 1311. For example, the first boundary portion 1314 may be formed using a material that includes lithium (Li) ions. In this case, the first boundary portion 1314 can reversibly insert and extract lithium ions.

[0105] For example, the first boundary portion 1314 may include at least one selected from the group consisting of compounds represented by the following chemical formulas: Li a A 1-b Mb D2 (where 0.90≤a≤1.8, 0≤b≤0.5); Li a E 1-b M b O 2-c D c (Where, 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05); LiE 2-b M b O 4-c D c (Where, 0 ≤ b ≤ 0.5, 0 ≤ c ≤ 0.05); Li a Ni 1-b- c Co b M c D α (Where, 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α≤2); Li a Ni 1-b-c Co b M c O 2-α X α (Where, 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α<2); Li a Ni 1-b-c Co b M c O 2-α X2 (where 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α<2); Li a Ni 1-b-c Mn b M c D α (Where, 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α≤2); Li a Ni 1-b-c Mn b M c O 2-α X α (Where, 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α<2); Li a Ni 1-b-c Mn b M c O 2-α X2 (where 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α<2); Li a Ni b E c G dO2 (where 0.90≤a≤1.8, 0≤b≤0.9, 0≤c≤0.5, 0.001≤d≤0.1); Li a Ni b Co c Mn d G e O2 (where 0.90≤a≤1.8, 0≤b≤0.9, 0≤c≤0.5, 0≤d≤0.5, 0.001≤e≤0.1); Li a NiG b O2 (where 0.90≤a≤1.8, 0.001≤b≤0.1); Li a CoG b O2 (where 0.90≤a≤1.8, 0.001≤b≤0.1); Li a MnG b O2 (where 0.90≤a≤1.8, 0.001≤b≤0.1); Li a Mn2G b O4 (where 0.90≤a≤1.8, 0.001≤b≤0.1); QO2; QS2; LiQS2; V2O5; LiV2O2; LiRO2; LiNiVO4; Li (3-f) J2(PO4)3 (0≤f≤2); Li (3-f) Fe2(PO4)3 (where 0≤f≤2) and LiFePO4. In the above chemical formulas, A is Ni, Co or Mn; M is Al, Ni, Co, Mn, Cr, Fe, Mg, Sr, V, Nb, Ti or a rare earth element; D is O, F, S or P; E is Co or Mn; X is F, S or P; G is Al, Cr, Mn, Fe, Mg, La, Ce, Sr or V; Q is Ti, Mo or Mn; R is Cr, V, Fe, Sc or Y; and J is V, Cr, Mn, Co, Ni or Cu.

[0106] The first boundary portion 1314 may also include aluminum oxide (Al2O3) and an electrolyte. In this case, the first boundary portion 1314 may also include an insulating material to reduce lithium (Li) leakage.

[0107] Due to the difference in shrinkage rates between the positive electrode active material and the current collector, if the current collector protrudes further than the positive electrode active material layer 1311 in the length direction (L-axis direction) or width direction (W-axis direction), it may increase the risk of contact with surrounding electrodes, thereby leading to short-circuit defects. The first boundary portion 1314 can prevent short-circuit defects caused by the protrusion of the current collector. That is, as described above, the first boundary portion 1314 can prevent short-circuit defects in the all-solid-state battery 10 by preventing the current collector from protruding.

[0108] The positive electrode active material layer 1311 includes a positive electrode active material. The positive electrode active material layer 1311 may be disposed on the positive electrode current collector 1313 and the first boundary portion 1314. The positive electrode active material layer 1311 can be formed by printing the positive electrode active material on one or both surfaces of the positive electrode current collector 1313 and the first boundary portion 1314. However, the method of forming the positive electrode active material layer 1311 is not limited to this.

[0109] The positive electrode active material included in the positive electrode active material layer 1311 can be a material containing lithium (Li) ions. The positive electrode active material can reversibly insert and extract lithium ions. In other words, the positive electrode active material contains lithium ions and can be used to supply lithium ions to the negative electrode during charging of the all-solid-state battery. The positive electrode active material can affect the capacity and output of the all-solid-state battery.

[0110] For example, the positive electrode active material may include at least one selected from the group consisting of compounds represented by the following chemical formulas: Li a A 1-b M b D2 (where 0.90≤a≤1.8, 0≤b≤0.5); Li a E 1-b M b O 2-c D c (Where, 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05); LiE 2-b M b O 4-c D c (Where, 0 ≤ b ≤ 0.5, 0 ≤ c ≤ 0.05); Li a Ni 1-b-c Co b M c D α (Where, 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α≤2); Li a Ni 1-b-c Co b M c O 2-α X α (Where, 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α<2); Li a Ni 1-b-c Co b M c O 2-α X2 (where 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α<2); Li a Ni 1-b-c Mn b Mc D α (Where, 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α≤2); Li a Ni 1-b-c Mn b M c O 2-α X α (Where, 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α<2); Li a Ni 1-b-c Mn b M c O 2-α X2 (where 0.90≤a≤1.8, 0≤b≤0.5, 0≤c≤0.05, 0<α<2); Li a Ni b E c G d O2 (where 0.90≤a≤1.8, 0≤b≤0.9, 0≤c≤0.5, 0.001≤d≤0.1); Li a Ni b Co c Mn d G e O2 (where 0.90≤a≤1.8, 0≤b≤0.9, 0≤c≤0.5, 0≤d≤0.5, 0.001≤e≤0.1); Li a NiG b O2 (where 0.90≤a≤1.8, 0.001≤b≤0.1); Li a CoG b O2 (where 0.90≤a≤1.8, 0.001≤b≤0.1); Li a MnG b O2 (where 0.90≤a≤1.8, 0.001≤b≤0.1); Li a Mn2G b O4 (where 0.90≤a≤1.8, 0.001≤b≤0.1); QO2; QS2; LiQS2; V2O5; LiV2O2; LiRO2; LiNiVO4; Li (3-f) J2(PO4)3 (0≤f≤2); Li (3-f)Fe2(PO4)3 (where 0≤f≤2) and LiFePO4. In the above chemical formulas, A is Ni, Co or Mn; M is Al, Ni, Co, Mn, Cr, Fe, Mg, Sr, V, Nb, Ti or a rare earth element; D is O, F, S or P; E is Co or Mn; X is F, S or P; G is Al, Cr, Mn, Fe, Mg, La, Ce, Sr or V; Q is Ti, Mo or Mn; R is Cr, V, Fe, Sc or Y; and J is V, Cr, Mn, Co, Ni or Cu.

[0111] Positive electrode active materials may also include LiCoO2 and LiMn. x O 2x (where x is 1 or 2), LiNi 1-x Mn x O 2x (where 0) <x<1)、LiNi 1-x-y Co x Mn y O2 (where 0≤x≤0.5, 0≤y≤0.5), LiFePO4, TiS2, FeS2, TiS3 or FeS3, but not limited to these.

[0112] The positive electrode active material may optionally include a conductive material and a binder. However, since organic materials such as binders decompose during sintering, organic materials may not remain in the positive electrode active material layer 1311 located on the obtained positive electrode current collector 1313.

[0113] There are no particular limitations on the conductive materials, as long as they are conductive and do not cause chemical changes in the all-solid-state battery 10. For example, the following materials can be used: graphite, such as natural graphite or artificial graphite; carbon-based materials, such as carbon black, acetylene black, Ketjen black, channel black, furnace black, lamp black, and pyrolysis black; conductive fibers, such as carbon fibers and metal fibers; fluorides; metallic components (such as lithium (Li), tin (Sn), aluminum (Al), nickel (Ni), and copper (Cu)) and oxides, nitrides, or fluorides of said metallic components; conductive whiskers, such as zinc oxide or potassium titanate; conductive metal oxides, such as titanium oxide; and conductive materials, such as polyphenylene derivatives.

[0114] Adhesives can be used to improve the bonding strength between active and conductive materials. Materials that can be used as adhesives may include at least one selected from the group consisting of: polyvinylidene fluoride, polyvinyl alcohol, carboxymethyl cellulose (CMC), starch, hydroxypropyl cellulose, regenerated cellulose, polyvinylpyrrolidone, polytetrafluoroethylene, polyethylene, polypropylene, ethylene propylene diene monomer (EPDM), sulfonated EPDM, styrene-butadiene rubber, fluororubber, various copolymers, etc., but are not limited thereto.

[0115] The positive electrode active material layer 1311 may additionally include a solid electrolyte component. The solid electrolyte component may be one or more of the components described above. The solid electrolyte component included in the positive electrode active material layer 1311 can serve as an ion conduction channel in the positive electrode active material layer 1311. This reduces the interfacial resistance.

[0116] For example, the first boundary portion 1314 and the positive electrode active material layer 1311 may comprise the same material. Alternatively, the first boundary portion 1314 and the positive electrode active material layer 1311 may be formed using the same paste.

[0117] Figure 8 This is a cross-sectional view showing the length of the positive electrode active material layer and the first boundary portion.

[0118] exist Figure 8 In the figure, L1 represents the length of the positive electrode active material layer 1311 in the length direction (L-axis direction), L2 represents the length of the first boundary portion 1314 in the length direction (L-axis direction), and L3 represents the length of the positive electrode current collector 1313 in the length direction (L-axis direction).

[0119] The ratio of the length L2 of the first boundary portion 1314 in the longitudinal direction (L-axis direction) to the length L1 of the positive electrode active material layer 1311 in the longitudinal direction (L-axis direction) can be greater than or equal to 0.01% and less than or equal to 0.1%. That is, the positive electrode active material layer 1311 and the first boundary portion 1314 can satisfy the following conditional expression: [Conditional Expression] 0.01%≤L2 / L1≤0.1%, in, L1: The length of the positive electrode active material layer in the longitudinal direction. L2: The length of the first boundary part in the longitudinal direction.

[0120] If the ratio of the length L2 of the first boundary portion 1314 in the longitudinal direction (L-axis direction) to the length L1 of the positive electrode active material layer 1311 in the longitudinal direction (L-axis direction) exceeds 0.1%, the battery capacity may be significantly reduced. Conversely, if the ratio of the length L2 of the first boundary portion 1314 to the length L1 of the positive electrode active material layer 1311 is less than 0.01%, a short circuit may occur. For example, the minimum length of the solid electrolyte layer 110 in the thickness direction (T-axis direction) may be greater than or equal to 28 μm.

[0121] For example, the length of the positive electrode active material layer 1311 in the length direction (L-axis direction) can refer to: the maximum value of multiple line segments parallel to the length direction (L-axis direction) and connecting the two outermost boundary lines of the positive electrode active material layer 1311 shown in the cross-section photograph taken at the central portion of the width direction (W-axis direction) of the laminate 100, in the length direction (L-axis direction) and thickness direction (T-axis direction). As another example, the length of the positive electrode active material layer 1311 in the length direction (L-axis direction) can refer to the minimum value among the lengths of the aforementioned multiple line segments. As yet another example, the length of the positive electrode active material layer 1311 in the length direction (L-axis direction) can refer to the arithmetic mean of at least two of the lengths of the aforementioned multiple line segments.

[0122] The length L2 of the first boundary portion 1314 in the longitudinal direction (L-axis direction) can refer to the difference between the length L1 of the positive electrode active material layer 1311 in the longitudinal direction (L-axis direction) and the length L3 of the positive electrode current collector 1313. That is, when measuring the length L1 of the positive electrode active material layer 1311 and the length L3 of the first boundary portion 1313, the difference L3-L1 can be the length L2 of the first boundary portion 1314.

[0123] For example, the length of the positive current collector 1313 in the length direction (L-axis direction) can refer to: the maximum value of multiple line segments parallel to the length direction (L-axis direction) and connecting the two outermost boundary lines of the positive current collector 1313 shown in the cross-section photograph taken at the central portion of the width direction (W-axis direction) of the laminate 100, in the length direction (L-axis direction) - thickness direction (T-axis direction). As another example, the length of the positive current collector 1313 in the length direction (L-axis direction) can refer to the minimum value among the lengths of the aforementioned multiple line segments. As yet another example, the length of the positive current collector 1313 in the length direction (L-axis direction) can refer to the arithmetic mean of at least two of the lengths of the aforementioned multiple line segments.

[0124] If a boundary portion satisfying the above-described conditional expression is formed, short-circuit defects can be prevented even when the thickness of the solid electrolyte layer 110 is reduced, and the battery capacity can be maintained at the same level. Therefore, while reducing the thickness of the laminate 100, almost the same battery capacity can be maintained without short-circuit defects. Furthermore, if the thickness of the laminate 100 remains constant, more positive electrode unit layers 130 and negative electrode unit layers 150 can be formed in the laminate 100, thereby increasing the battery capacity.

[0125] In the following text, reference will be made to Figure 9 and Figure 10 The second unit layer is described. The second unit layer includes a second electrode unit layer and a second edge portion. For better understanding and ease of description, it is assumed that the second unit layer is a negative electrode unit layer 150.

[0126] Figure 9 It is shown Figure 3 A partial 3D view of part B. Figure 10 It is along Figure 9 A cross-sectional view taken by line X-X'.

[0127] Reference Figure 3 , Figure 9 and Figure 10 The negative electrode unit layer 150 may be formed on one surface of the solid electrolyte layer 110. The negative electrode unit layer 150 includes a negative electrode layer 151 and a second edge portion 153. One end of the negative electrode layer 151 is exposed to the second surface S2 of the laminate 100 and is in contact with the second external electrode 400. The second edge portion 153 is disposed between the negative electrode layer 151 and the first external electrode 300.

[0128] The second edge portion 153 constitutes the region of the negative electrode unit layer 150 other than the negative electrode layer 131. That is, the second edge portion 153 may be disposed on the first surface S1, the third surface S3, and the fourth surface S4. Specifically, the second edge portion 153 is the portion parallel to the negative electrode layer 151 in both the length direction (L-axis direction) and the width direction (W-axis direction). The second edge portion 153 may be formed to contact two surfaces of the negative electrode layer 151 along the length direction (L-axis direction) and one surface of the negative electrode layer 151 along the width direction (W-axis direction). Therefore, the second edge portion 153 may be exposed to the second surface S2, the third surface S3, and the fourth surface S4 of the laminate 100. For example, the second edge portion 153 may have a hyperbolic shape.

[0129] The second edge portion 153 may be formed using an insulating material (i.e., a material that does not have electronic conductivity (or ionic conductivity)).

[0130] The second edge portion 153 may include a ceramic material. For example, the second edge portion 153 may include at least one selected from the group consisting of alumina (Al2O3), aluminum nitride (AlN), beryllium oxide (BeO), boron nitride (BN), silicon (Si), silicon carbide (SiC), silicon dioxide (SiO2), silicon nitride (Si3N4), gallium arsenide (GaAs), gallium nitride (GaN), barium titanate (BaTiO3), zirconium dioxide (ZrO2), mixtures thereof, oxides and / or nitrides thereof, or any other suitable ceramic material.

[0131] Additionally, the second edge portion 153 may include one or more types of solid electrolytes, and may optionally include the aforementioned solid electrolytes.

[0132] The second edge portion 153 may include a material having low ionic conductivity and low electronic conductivity (i.e., an insulating material). Additionally, a material having an ionic conductivity (or electronic conductivity) approximating that of the solid electrolyte and an insulating material may coexist in the second edge portion 153. For example, if the second edge portion 153 includes a material having an ionic conductivity (or electronic conductivity) approximating that of the solid electrolyte, this material may be the same material as or different from the solid electrolyte in other regions. As another example, the second edge portion 153 may simultaneously include an insulating material and a material having an ionic conductivity (or electronic conductivity) approximating that of the solid electrolyte.

[0133] The first edge portion 133 and the second edge portion 153 can be formed using the same material. Alternatively, the solid electrolyte, the first edge portion 133, and the second edge portion 153 can be formed using the same material.

[0134] The second edge portion 153 can be formed by coating an insulating paste onto the solid electrolyte layer 110. Figure 3 The boundary between the second edge portion 153 and the solid electrolyte layer 110 is clearly shown in the figure. However, when the second edge portion 153 and the solid electrolyte layer 110 are formed using the same material, it may be difficult to distinguish the boundary in the laminate after sintering.

[0135] The negative electrode layer 151 includes a negative electrode active material. The negative electrode active material included in the negative electrode layer 151 can generate electrical energy by storing and releasing lithium ions that have moved from the positive electrode layer 131 during the discharge of the all-solid-state battery 10. Carbon-based materials, silicon, silicon oxides, silicon-based alloys, silicon-carbon composites, tin, tin-based alloys, tin-carbon composites, metal oxides, or combinations thereof can be used as the negative electrode active material, and lithium metal and / or lithium metal alloys may be included.

[0136] The lithium metal alloy may include lithium and a metal / metalloid capable of alloying with lithium. For example, the metal / metalloid capable of alloying with lithium may include Si, Sn, Al, Ge, Pb, Bi, Sb, Si-AM alloy (where AM is an alkali metal, alkaline earth metal, group 13 to group 16 element, transition metal, rare earth element or a combination thereof, and does not include Si), Sn-AM alloy (where AM is an alkali metal, alkaline earth metal, group 13 to group 16 element, transition metal, transition metal oxide (such as lithium titanium oxide (Li4Ti5O 12 etc.), rare earth element or a combination thereof, and does not include Sn), MnO x (0 < x ≤ 2) etc.

[0137] The element AM may be Mg, Ca, Sr, Ba, Ra, Sc, Y, Ti, Zr, Hf, Rf, V, Nb, Ta, Db, Cr, Mo, W, Sg, Tc, Re, Bh, Fe, Pb, Ru, Os, Hs, Rh, Ir, Pd, Pt, Cu, Ag, Au, Zn, Cd, B, Al, Ga, Sn, In, Tl, Ge, P, As, Sb, Bi, S, Se, Te, Po or a combination thereof.

[0138] In addition, the oxide of the metal / metalloid capable of alloying with lithium may be lithium titanium oxide, vanadium oxide, lithium vanadium oxide, SnO2, SiO x (0 < x < 2) etc. For example, the negative electrode active material may include one or more elements selected from the group consisting of group 13 to group 16 elements of the periodic table. For example, the negative electrode active material may include one or more elements selected from the group consisting of Si, Ge and Sn.

[0139] The carbon-based material may be crystalline carbon, amorphous carbon or a mixture thereof. The crystalline carbon may be graphite, such as natural graphite or artificial graphite in amorphous, plate-like, flaky, spherical or fibrous form. Additionally, the amorphous carbon may be soft carbon (low-temperature sintered carbon) or hard carbon, mesophase pitch carbide, sintered coke, graphene, carbon black, fullerene soot, carbon nanotubes, carbon fibers, etc., but is not limited thereto.

[0140] Silicon may include at least one selected from the group consisting of Si, SiO x (0 < x < 2, for example, 0.5 to 1.5), Sn, SnO2 or a silicon-containing metal alloy and mixtures thereof. The silicon-containing metal alloy may include, for example, at least one selected from the group consisting of Al, Sn, Ag, Fe, Bi, Mg, Zn, In, Ge, Pb and Ti and silicon.

[0141] The negative electrode active material may optionally include a conductive material and an adhesive.

[0142] There are no particular limitations on the conductive materials, as long as they are conductive and do not cause chemical changes in the all-solid-state battery 10. For example, the following materials can be used: graphite, such as natural graphite or artificial graphite; carbon-based materials, such as carbon black, acetylene black, Ketjen black, channel black, furnace black, lamp black, and pyrolysis black; conductive fibers, such as carbon fibers and metal fibers; fluorides; metallic components (such as lithium (Li), tin (Sn), aluminum (Al), nickel (Ni), and copper (Cu)) and oxides, nitrides, or fluorides of said metallic components; conductive whiskers, such as zinc oxide or potassium titanate; conductive metal oxides, such as titanium oxide; and conductive materials, such as polyphenylene derivatives.

[0143] Adhesives can be used to improve the bonding strength between active and conductive materials. For example, adhesives may include polyvinylidene fluoride, polyvinyl alcohol, carboxymethyl cellulose (CMC), starch, hydroxypropyl cellulose, regenerated cellulose, polyvinylpyrrolidone, polytetrafluoroethylene, polyethylene, polypropylene, ethylene propylene diene monomer (EPDM), sulfonated EPDM, styrene-butadiene rubber, fluororubber, and various copolymers.

[0144] The first electrode layer 310 of the first external electrode 300 can be electrically connected to the positive electrode layer 131, and the second electrode layer 410 of the second external electrode 400 can be electrically connected to the negative electrode layer 151.

[0145] For example, the first electrode layer 310 and the second electrode layer 410 can be sintered electrodes containing conductive metal and glass, or they can be resin-based electrodes containing conductive metal and resin.

[0146] For example, the first electrode layer 310 and the second electrode layer 410 can be formed, respectively, by applying a terminal electrode paste containing a conductive metal to the first surface S1 and the second surface S2 of the laminate 100. As another example, the first electrode layer 310 and the second electrode layer 410 can be formed by transferring a dry film of conductive paste onto the laminate 100 and then sintering the dry film. However, the method of forming the first electrode layer 310 and the second electrode layer 410 is not limited to these methods. The conductive metal may include one or more selected from the group consisting of copper (Cu), nickel (Ni), tin (Sn), palladium (Pd), platinum (Pt), gold (Au), silver (Ag), tungsten (W), titanium (Ti), lead (Pb), and alloys thereof.

[0147] A first plating layer 320 covers a first electrode layer 310, and a second plating layer 420 covers a second electrode layer 410. The first plating layer 320 and the second plating layer 420 can be used to improve the mounting characteristics of the external electrode. The first plating layer 320 and the second plating layer 420 may comprise at least one type selected from the group consisting of copper (Cu), nickel (Ni), tin (Sn), palladium (Pd), platinum (Pt), gold (Au), silver (Ag), tungsten (W), titanium (Ti), lead (Pb), and alloys thereof. Both the first plating layer 320 and the second plating layer 420 can be formed using one or more layers.

[0148] Next, the manufacturing method of the positive electrode cell layer 130 in the all-solid-state battery 10 constructed above will be described.

[0149] Figures 11 to 17 A method for manufacturing the positive electrode cell layer 130 of an all-solid-state battery according to an embodiment is shown.

[0150] Reference Figure 11 Prepare a solid electrolyte layer 110, and form a first positive electrode active material layer 1311a by printing an active material paste onto the solid electrolyte layer 110 and then drying it.

[0151] Reference Figure 12 Next, an insulating paste can be applied to the solid electrolyte layer 110 by printing, followed by drying, to form the first edge portion 133a. The insulating paste can be applied to the remaining portions of the solid electrolyte where the first edge portion 133a is not formed. The first edge portion 133a can contact the edge of the first positive electrode active material layer 1311a in a planar manner. The first edge portion 133a can contact three of the four edge surfaces of the first positive electrode active material layer 1311a in the length direction (L-axis direction) and width direction (W-axis direction). The first edge portion 133a can be formed to contact two of the four edge surfaces of the first positive electrode active material layer 1311a arranged along the length direction (L-axis direction). Among the edges of the first positive electrode active material layer 1311a, the edges that do not contact the first edge portion 133a can be exposed to the first surface S1 after sintering the laminate 100.

[0152] Reference Figure 13 The positive current collector 1313 can be formed by printing conductive paste onto the first positive active material layer 1311a and then drying it.

[0153] Reference Figure 14The first boundary portion 1314 can be formed by printing a paste for the first boundary portion onto the first positive electrode active material layer 1311a and then drying it. The paste for the first boundary portion can be applied to the portion of the first positive electrode active material layer 1311a where the positive electrode current collector 1313 is not formed. The first boundary portion 1314 can contact the edge surface of the positive electrode current collector 1313 in a plane. That is, the first boundary portion 1314 can be provided along the edge of the positive electrode current collector 1313 in the length direction (L-axis direction). In addition, the first boundary portion 1314 can be provided along one of the two opposing edges of the positive electrode current collector 1313 in the length direction (L-axis direction). At this time, the edge of the positive electrode current collector 1313 that contacts the first boundary portion 1314 is set to be the edge closer to the second surface S2. The edge of the positive electrode current collector 1313 that does not contact the first boundary portion 1314 can be exposed to the first surface S1 of the laminate 100. In other words, the positive electrode current collector 1313 may have a generally hexahedral shape with two edge surfaces along the length direction (L-axis direction) and two edge surfaces along the width direction (W-axis direction), and the first boundary portion 1314 may be formed to contact one of the two edge surfaces of the positive electrode current collector 1313 arranged along the length direction (L-axis direction) and one of the two edge surfaces arranged along the width direction (W-axis direction). That is, the first boundary portion 1314 may be formed to surround three of the four surfaces of the positive electrode current collector 1313 in the planar direction. The paste for the first boundary portion includes a positive electrode active material. The paste for the first boundary portion coated when forming the first boundary portion 1314 may include lithium (Li) ions. For example, the paste for the first boundary portion may include alumina (Al2O3) and an electrolyte, and may also include an insulating material. For example, the paste for the first boundary portion may be the same as the active material paste for forming the positive electrode active material layer.

[0154] Reference Figure 15 The second edge portion 133b can be formed by printing insulating paste onto the first edge portion 133a and then drying it. The second edge portion 133b can contact the edge of the first boundary portion 1314 on a plane. The direction in which the second edge portion 133b contacts the edge of the first boundary portion 1314 can be the same as the direction in which the first boundary portion 1314 contacts the edge of the positive current collector 1313.

[0155] Reference Figure 16 The second positive electrode active material layer 1311b can be formed by printing an active material paste onto the positive electrode current collector 1313 and the first boundary portion 1314 and then drying it.

[0156] Reference Figure 17The third edge portion 133c can be formed by printing insulating paste on the second edge portion 133b and drying it. The third edge portion 133c can contact the edge of the second positive electrode active material layer 1311b in a planar manner. That is, the third edge portion 133c can contact three of the four edges of the second positive electrode active material layer 1311b in the length direction (L-axis direction) and width direction (W-axis direction). Among the edges of the first positive electrode active material layer 1311a, the edges that do not contact the first edge portion 133a can be exposed on the first surface S1 after sintering the laminate 100. In this way, the first edge 133 can be formed by coating the first edge portion 133a, the second edge portion 133b, and the third edge portion 133c respectively and drying them.

[0157] [Experimental Example 1] Twenty all-solid-state batteries of Examples 1 to 9 and Comparative Examples 1 to 3 were fabricated by varying the thickness of the solid electrolyte layer (the length of the solid electrolyte layer in the thickness direction (T-axis direction)) and the length of the positive electrode current collector. The length of the positive electrode active material layer of the all-solid-state batteries of Examples 1 to 9 and Comparative Examples 1 to 3 was measured in the length direction, and was 8 mm in all cases. The length of the positive electrode current collector was also measured in the length direction.

[0158] A paste containing 65 wt% (by weight) lithium cobalt oxide (LOC) and 35 wt% solid electrolyte is used to form the positive electrode active material layer. A conductive paste for forming the positive electrode current collector contains 60 wt% flake graphite and 40 wt% solid electrolyte. A paste containing 60 wt% spherical natural graphite and 40 wt% solid electrolyte is used to form the negative electrode active material layer. The same material as the positive electrode active material layer is used to form the boundary of the all-solid-state batteries of Examples 1 to 9. To form the positive electrode layer, a first positive electrode active material layer with a thickness of 50 μm, a positive electrode current collector with a thickness of 10 μm, and a second positive electrode active material layer with a thickness of 50 μm are printed on the solid electrolyte sheet, respectively. Additionally, to form the negative electrode layer, a negative electrode active material layer with a thickness of 50 μm is printed on the solid electrolyte sheet.

[0159] A laminate was manufactured such that the positive electrode unit layer and the negative electrode unit layer formed as described above each consisted of 25 layers, for a total of 50 layers. The results of measuring the average capacity and short-circuit defect rate of the all-solid-state batteries of Examples 1 to 7 and Comparative Examples 1 to 4 are shown in Table 1. In Table 1, the ratio of the first boundary portion represents the ratio of the length of the first boundary portion to the length of the positive electrode active material layer.

[0160] [Table 1]

[0161] As shown in Table 1, it is confirmed that when the thickness of the solid electrolyte layer is the same, the capacity increases with the increase of the ratio of the first boundary portion. Furthermore, as the ratio of the first boundary portion increases, the short-circuit defect rate also decreases.

[0162] However, when the thickness of the solid electrolyte layer is less than or equal to 25 μm, short-circuit defects occur even when the ratio of the first boundary portion increases to 1%. When the thickness of the solid electrolyte layer is 30 μm, 20% of short-circuit defects occur in Comparative Example 3, which does not have a first boundary portion, while no short-circuit defects occur in Examples 7, 8, and 9, where the ratio of the first boundary portion is greater than or equal to 0.25%.

[0163] Therefore, it is confirmed that in order to prevent short-circuit defects, the thickness of the solid electrolyte layer must be greater than 25 μm, and a first boundary portion must be formed.

[0164] [Experimental Example 2] One hundred all-solid-state batteries of Examples 10 to 14 and Comparative Examples 4 to 7 were fabricated by varying the length of the positive electrode active material layer (measured in the length direction) and the length of the positive electrode current collector. Since it was confirmed in Experimental Example 1 that the thickness of the solid electrolyte layer must be greater than 25 μm to prevent short-circuit defects, each of the all-solid-state batteries of Examples 10 to 14 and Comparative Examples 4 to 7 was fabricated with a solid electrolyte layer having a thickness of 28 μm.

[0165] A paste containing 65 wt% (by weight) lithium cobalt oxide (LOC) and 35 wt% solid electrolyte is used to form the positive electrode active material layer. A conductive paste for forming the positive electrode current collector contains 60 wt% flake graphite and 40 wt% solid electrolyte. A paste containing 60 wt% spherical natural graphite and 40 wt% solid electrolyte is used to form the negative electrode active material layer. The same material as the positive electrode active material layer is used to form the boundary of the all-solid-state batteries of Examples 10 to 14. To form the positive electrode layer, a first positive electrode active material layer with a thickness of 50 μm, a positive electrode current collector with a thickness of 10 μm, and a second positive electrode active material layer with a thickness of 50 μm are printed on the solid electrolyte sheet, respectively. Additionally, to form the negative electrode layer, a negative electrode active material layer with a thickness of 50 μm is printed on the solid electrolyte sheet.

[0166] A laminate was manufactured such that there were 25 positive electrode unit layers and 25 negative electrode unit layers, for a total of 50 layers. The results of measuring the average capacity and short-circuit defect rate are shown in Table 2. In Table 2, the ratio of the first boundary portion represents the ratio of the length of the first boundary portion to the length of the positive electrode active material layer.

[0167] [Table 2]

[0168] As shown in Table 2, short-circuit defects occurred in all-solid-state batteries where the positive electrode current collector was longer than the positive electrode active material layer (Comparative Example 4) and in all-solid-state batteries where the ratio of the first boundary portion was less than 0.01%. Therefore, it is confirmed that the ratio of the first boundary portion must be greater than or equal to 0.01% to prevent short-circuit defects.

[0169] Furthermore, as the ratio of the first boundary portion increases, the battery capacity tends to decrease. Specifically, it was confirmed that the battery capacity decreases significantly when the ratio of the first boundary portion is 0.1%. Observing the measurement results of Examples 10 to 13 (14.12mAh and 14.22mAh) with similar lengths of the positive electrode active material layers, the battery capacity decreased from 16.17mAh to 16.13mAh as the ratio of the first boundary portion increased from 0.01% to 0.1%. On the other hand, observing the measurement results of Examples 14 and Comparative Example 6 (13.96mAh and 13.99mAh) with similar lengths of the positive electrode active material layers, although the difference was small, the capacity was significantly reduced compared to the results of Examples 10 to 13 (15.98mAh and 15.70mAh, respectively), with first boundary portion ratios of 0.10% and 0.11%, respectively. As described above, compared to blocks with a ratio exceeding 0.1%, blocks with a first boundary portion ratio greater than or equal to 0.01% and less than or equal to 0.1% exhibit a lower reduction in battery capacity. In other words, it is confirmed that when the ratio of the first boundary portion exceeds 0.1%, the efficiency in terms of battery capacity decreases significantly.

[0170] In the following text, reference will be made to Figures 18 to 20 Describes an all-solid-state battery according to another embodiment.

[0171] Figure 18 This is a partial perspective view showing a portion of the negative electrode layer 155 of an all-solid-state battery according to another embodiment. Figure 19 yes Figure 18 The exploded stereoscopic view, and Figure 20 It is along Figure 18 A partial cross-sectional view taken from line XX-XX' in the diagram. Figures 18 to 20 The all-solid-state battery of the embodiment shown is compared with the reference. Figures 1 to 10 The description is similar to that of an all-solid-state battery. Detailed descriptions of identical components have been omitted.

[0172] Reference Figures 18 to 20 According to this embodiment, the negative electrode layer 155 of the all-solid-state battery may include a negative electrode active material layer 1551, a negative electrode current collector 1553, and a second boundary portion 1554.

[0173] For example, the negative electrode current collector 1553 can be made of stainless steel, nickel (Ni), copper (Cu), tin (Sn), aluminum (Al), or alloys thereof. Additionally, the negative electrode current collector 1553 can be coated with an antioxidant metal or alloy film to prevent oxidation.

[0174] The negative electrode current collector 1553 can be formed using the same conductive carbon-based material as the positive electrode current collector 1313. Additionally, the negative electrode current collector 1553 can contain one or more types of solid electrolytes. For example, the negative electrode current collector 1553 may include a sintered oxide glass electrolyte.

[0175] The second boundary portion 1554 may be provided on the side surface of the negative electrode current collector 1553 in the length direction (L-axis direction) and width direction (W-axis direction). The second boundary portion 1554 may be provided between the negative electrode current collector 1553 and the second edge portion 153. The second boundary portion 1554 may contact the two ends of the negative electrode current collector 1553 in the width direction (W-axis direction). In addition, the second boundary portion 1554 may contact the end of the two ends of the negative electrode current collector 1553 in the length direction (L-axis direction) that is closer to the first surface S1. The second boundary portion 1554 may be configured to surround the ends of the negative electrode current collector 1553 in the length direction (L-axis direction) and width direction (W-axis direction) other than the end exposed to the first surface S1. That is, the second boundary portion 1554 may be configured to contact one of the two ends of the positive electrode current collector 1553 provided in the length direction (L-axis direction) and the two ends provided in the width direction (W-axis direction). At the end of the negative electrode current collector 1553, the end that does not contact the second boundary portion 1554 can be exposed to the second surface S2 of the laminate 100 and can contact the second external electrode 400. Since the second boundary portion 1554 is disposed between the negative electrode current collector 1553 and the second edge portion 153, the negative electrode current collector 1553 and the second edge portion 153 are spaced apart from each other. That is, the second boundary portion 1554 can prevent the negative electrode current collector 1553 from contacting the second edge portion 153.

[0176] Based on the second edge portion 153, the second boundary portion 1554 can be configured to contact the inner surface of the second edge portion 153 along the length direction (L-axis direction) and the width direction (W-axis direction). Therefore, the second boundary portion 1554 can be formed to surround the negative electrode current collector 1553 in three directions. Since the negative electrode current collector 1553 contacts the negative electrode current collector 1553 on the third surface S3, the first surface S1, and the fourth surface S4 while surrounding the negative electrode current collector 1553, the entire negative electrode current collector 1553 and the entire second edge portion 153 can be separated by the second boundary portion 1554.

[0177] For example, the second boundary portion 1554 may use carbon-based materials, silicon, silicon oxide, silicon-based alloys, silicon-carbon composites, tin, tin-based alloys, tin-carbon composites, metal oxides, or combinations thereof, and may include lithium metal and / or lithium metal alloys. The second boundary portion 1554 may be formed using the same material as the negative electrode active material layer 1551.

[0178] Since the length and measurement method of the second boundary portion 1554 are the same as those of the first boundary portion 1314, repeated descriptions will be omitted.

[0179] The negative electrode active material layer 1551 includes a negative electrode active material. The negative electrode active material layer 1551 may be disposed on the negative electrode current collector 1553 and the second boundary portion 1554. The negative electrode active material layer 1551 can be formed by printing negative electrode active material on one or both surfaces of the negative electrode current collector 1553 and the second boundary portion 1554. That is, the negative electrode active material layer 1551 may include a first negative electrode active material layer 1551a disposed on one surface of the negative electrode current collector 1553 and the second boundary portion 1554, and may also include a second negative electrode active material layer 1551b disposed on the other surface of the negative electrode current collector 1553 and the second boundary portion 1554. However, the method of forming the negative electrode active material layer 1551 is not limited thereto. Because the negative electrode active material included in the negative electrode active material layer 1551 is similar to a reference... Figures 1 to 10 The negative electrode active material described is the same, so repeated descriptions will be omitted.

[0180] While this disclosure has been described in conjunction with what is now considered to be actual embodiments, it should be understood that this disclosure is not limited to the disclosed embodiments, but rather is intended to cover various variations and equivalents included within the spirit and scope of the appended claims.

[0181] <Explanation of reference numerals in the attached figures> 10: All-solid-state batteries 100: Layered body 110: Solid electrolyte layer 130: Positive electrode unit layer 131: Positive electrode layer 1311: Positive electrode active material layer 1313: Positive current collector 1314: First Boundary Section 133: First edge 150: Negative electrode unit layer 151: Negative electrode layer 153: Second edge 1551: Negative electrode active material layer 1553: Negative electrode current collector 1554: Second Boundary Section 180: Upper protective layer 190: Lower protective layer 300: First external electrode 310: First electrode layer 320: First coating 400: Second external electrode 410: Second electrode layer 420: Second coating.

Claims

1. An all-solid-state battery, comprising: Solid electrolyte layer; The first electrode unit layer and the second electrode unit layer are opposite to each other, and the solid electrolyte layer is located between the first electrode unit layer and the second electrode unit layer; A first external electrode is disposed on the outer surface of the all-solid-state battery and connected to the second electrode unit layer; and The first edge portion is disposed between the first electrode unit layer and the first outer electrode. The first electrode unit layer includes a first current collector and a first boundary portion, wherein the first boundary portion is disposed between the first current collector and the first boundary portion and includes a first active material.

2. The all-solid-state battery according to claim 1, wherein, The first boundary portion prevents the first current collector from contacting the first edge portion.

3. The all-solid-state battery according to claim 1, wherein, The first electrode unit layer further includes a first active material layer disposed on the first current collector and on the first boundary portion.

4. The all-solid-state battery according to claim 3, wherein, The first active material layer comprises the same material as the first boundary portion.

5. The all-solid-state battery according to claim 3, wherein, The first active material layer and the first boundary portion satisfy the following conditional expression: [Conditional Expression] 0.01%≤L2 / L1≤0.1%, in, L1: The length of the first active material layer L2: The length of the first boundary portion.

6. The all-solid-state battery according to claim 1, wherein, The first active material is a positive electrode active material.

7. The all-solid-state battery according to claim 1, wherein, The first boundary portion also includes aluminum oxide (Al2O3) and an electrolyte.

8. The all-solid-state battery according to claim 7, wherein, The first boundary portion also includes insulating material.

9. The all-solid-state battery according to claim 1, further comprising: The second external electrode is disposed on the outer surface of the all-solid-state battery and connected to the first electrode unit layer; as well as The second edge portion is disposed between the second electrode unit layer and the second outer electrode. The second electrode unit layer includes a second current collector and a second boundary portion disposed between the second current collector and the second edge portion.

10. The all-solid-state battery according to claim 9, wherein, The second boundary portion includes a negative electrode active material.

11. The all-solid-state battery according to claim 9, wherein, The second boundary portion prevents the second current collector from contacting the second edge portion.

12. The all-solid-state battery according to claim 9, wherein, The second electrode unit layer further includes a second active material layer disposed on the second current collector and the second boundary portion, and The second active material layer comprises the same material as the second boundary portion.

13. An all-solid-state battery, comprising: A laminate includes a solid electrolyte layer and a positive electrode layer and a negative electrode layer disposed therebetween, wherein the solid electrolyte layer is disposed between the positive electrode layer and the negative electrode layer; A first external electrode is disposed on the outer side of the laminate; and The first edge portion is disposed between the positive electrode layer and the first external electrode. The positive electrode layer includes a positive electrode active material layer, a positive electrode current collector, and a first boundary portion. The positive electrode current collector is disposed on the positive electrode active material layer, and the first boundary portion is disposed between the positive electrode current collector and the first boundary portion and includes positive electrode active material.

14. The all-solid-state battery according to claim 13, wherein, The first boundary portion prevents the positive current collector from contacting the first edge portion.

15. The all-solid-state battery according to claim 13, wherein, The positive electrode active material layer and the first boundary portion comprise the same material.

16. The all-solid-state battery according to claim 13, wherein the all-solid-state battery comprises: The second external electrode is opposite to the first external electrode and the laminate is located between the first external electrode and the second external electrode; as well as The second edge portion is disposed between the negative electrode layer and the second external electrode. The negative electrode layer includes a negative electrode active material layer, a negative electrode current collector, and a second boundary portion. The negative electrode current collector is disposed on the negative electrode active material layer, and the second boundary portion is disposed between the negative electrode current collector and the second boundary portion.

17. The all-solid-state battery according to claim 16, wherein, The second boundary portion is made of the same material as the negative electrode active material layer.

18. A method for manufacturing an all-solid-state battery, comprising: An active material paste is coated onto a solid electrolyte layer to form an active material layer; An insulating paste is applied to the solid electrolyte layer to form the first edge layer; A conductive paste is coated onto the active material layer to form a current collector; as well as A boundary portion is formed by applying a paste for the boundary portion to the portion of the active material layer where the current collector is not formed.

19. The method for an all-solid-state battery according to claim 18, the method further comprising: The second edge layer is formed by applying insulating paste to the edge of the first layer. The entire edge portion of the second layer is formed to be spaced apart from the entire current collector by the boundary portion.

20. The method for an all-solid-state battery according to claim 18, wherein, The paste used for the boundary portion comprises the same material as the active material paste.

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