All-solid-state battery

Abstract

An all-solid-state battery includes: an all-solid-state battery element including a laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers, and a plurality of negative electrode layers stacked in a first direction, a first external electrode disposed outside the laminate and connected to the plurality of positive electrode layers, and a second external electrode disposed outside the laminate and connected to the plurality of negative electrode layers; a second external electrode disposed outside the laminate and connected to the plurality of negative electrode layers; and a resin sealing body covering the all-solid-state battery element and exposing a portion of the first external electrode and a portion of the second external electrode. The resin sealing body includes a first resin sealing body and a second resin sealing body, and an elastic modulus of the first resin sealing body is different from an elastic modulus of the second resin sealing body.

Description

TECHNICAL FIELD

[0001] The disclosure relates to an all-solid-state battery. BACKGROUND

[0002] Recently, as portable electronic devices require miniaturization and long-term use, high-capacity batteries are required, and as wearable electronic devices are popularized, the safety of batteries needs to be ensured.

[0003] Lithium ion batteries currently on the market use an electrolyte solution including a flammable organic solvent, and thus can overheat and catch fire at the time of short circuit. Accordingly, an all-solid-state battery using a solid electrolyte instead of an electrolyte solution has been proposed.

[0004] An all-solid-state battery can expand as the volume of an electrode active material layer changes during charging and discharging. Inside the expanded all-solid-state battery, the electrode can be damaged, or the junction of the electrode-solid electrolyte interface can be damaged, thereby causing poor contact, which can deteriorate the battery characteristics, particularly the charge-discharge cycle characteristics. In addition, due to the difference in expansion rates of the electrode and the solid electrolyte, cracks can be generated in the all-solid-state battery, thereby causing moisture penetration. SUMMARY

[0005] TECHNICAL PROBLEM An aspect of an embodiment is to provide an all-solid-state battery in which expansion can be inhibited.

[0006] An aspect of an embodiment is to provide an all-solid-state battery in which moisture penetration can be prevented.

[0007] However, the problems to be solved by embodiments of the disclosure are not limited to the above-mentioned problems, and various extensions can be made within the scope of the technical spirit of the disclosure.

[0008] SOLUTION TO PROBLEM An all-solid-state battery according to an embodiment can include an all-solid-state battery element including a laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers, and a plurality of negative electrode layers stacked in a first direction, a first external electrode disposed outside the laminate and connected to the plurality of positive electrode layers, and a second external electrode disposed outside the laminate and connected to the plurality of negative electrode layers, and a resin sealing body covering the all-solid-state battery element and exposing a portion of the first external electrode and a portion of the second external electrode. The resin sealing body can include a first resin sealing body and a second resin sealing body, and an elastic modulus of the first resin sealing body can be different from an elastic modulus of the second resin sealing body.

[0009] Additionally, the resin seal allows the end surfaces of the first external electrode and the second external electrode in the second direction to be exposed, and the second direction may intersect with the first direction.

[0010] Additionally, the first resin sealant may cover the outer surface of the laminate, and the second resin sealant may cover the first resin sealant, at least a portion of the first external electrode (excluding the stated portion), and at least a portion of the second external electrode (excluding the stated portion).

[0011] Additionally, the first external electrode may include a first strip portion disposed on the outer surface of the laminate in the first direction, the second external electrode may include a second strip portion disposed on the outer surface of the laminate in the first direction, and the two ends of the first resin sealant in the second direction may respectively contact the first strip portion and the second strip portion.

[0012] In addition, the thickness of the first resin seal may be less than the thickness of the first strip and the thickness of the second strip.

[0013] Additionally, the first external electrode may include a first strip portion disposed on the outer surface of the laminate in the first direction, and the second external electrode may include a second strip portion disposed on the outer surface of the laminate in the first direction. The first resin sealant may cover a portion of the first strip portion and a portion of the second strip portion, and the second resin sealant may cover the remaining portion of the first strip portion and the remaining portion of the second strip portion.

[0014] In addition, the thickness of the first resin seal may be greater than the thickness of the first strip and may be greater than the thickness of the second strip.

[0015] In addition, the elastic modulus of the first resin seal may be greater than that of the second resin seal, and the second resin seal may cover the first resin seal.

[0016] In addition, the elastic modulus of the first resin sealant may be less than that of the second resin sealant, and the second resin sealant may cover the first resin sealant.

[0017] Additionally, the first resin sealant may include phenolic epoxy resin, phenolic resin, phenolic varnish epoxy resin, o-cresol resin, acrylic resin, or a combination thereof.

[0018] Additionally, the second resin sealant may include polyimide resin, polyimide silicone resin, silicone resin, polyamide resin, rubber, polyurethane resin, or combinations thereof.

[0019] According to another embodiment, an all-solid-state battery includes: an all-solid-state battery element including a laminate, a first external electrode, and a second external electrode; the laminate includes a plurality of solid electrolyte layers, a plurality of positive electrode layers, and a plurality of negative electrode layers stacked in a first direction; the first external electrode is disposed outside the laminate and connected to the plurality of positive electrode layers; the second external electrode is disposed outside the laminate and connected to the plurality of negative electrode layers; and a resin sealant covering the all-solid-state battery element and exposing a portion of the first external electrode and a portion of the second external electrode. The resin sealant may include a first resin sealant, a second resin sealant, and a third resin sealant stacked in the first direction.

[0020] In addition, the elastic modulus of the first resin seal may be greater than that of the second resin seal, and the elastic modulus of the third resin seal may be greater than that of the second resin seal.

[0021] Additionally, the first external electrode may include a first strip portion disposed on the outer surface of the laminate in the first direction, and the second external electrode may include a second strip portion disposed on the outer surface of the laminate in the first direction. The first resin sealant may cover the outer surface of the laminate and may contact the first strip portion and the second strip portion. The second resin sealant may cover the first resin sealant and may contact the first strip portion and the second strip portion. The third resin sealant may cover the second resin sealant and may expose the end surfaces of the first external electrode and the second external electrode in the second direction, and the second direction may intersect the first direction.

[0022] In addition, the first resin seal can be disposed between the first strip and the second strip, and the thickness of the first resin seal can be less than the thickness of the first strip and less than the thickness of the second strip.

[0023] In addition, the elastic modulus of the first resin seal may be less than that of the second resin seal, and the elastic modulus of the third resin seal may be less than that of the second resin seal.

[0024] Additionally, the first external electrode may include a first strip portion disposed on the outer surface of the laminate in the first direction, and the second external electrode may include a second strip portion disposed on the outer surface of the laminate in the first direction. The first resin sealant may cover the outer surface of the laminate and may contact the first strip portion and the second strip portion. The second resin sealant may cover the first resin sealant and may contact the first strip portion and the second strip portion. The third resin sealant may cover the second resin sealant and may expose the end surfaces of the first external electrode and the second external electrode in the second direction, and the second direction may intersect the first direction.

[0025] In addition, the first resin seal can be disposed between the first strip and the second strip, and the thickness of the first resin seal can be less than the thickness of the first strip and less than the thickness of the second strip.

[0026] According to another embodiment, an all-solid-state battery includes: an all-solid-state battery element, including a laminate, a first external electrode, and a second external electrode, the laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers, and a plurality of negative electrode layers stacked in a first direction, the first external electrode being disposed outside the laminate and connected to the plurality of positive electrode layers, and the second external electrode being disposed outside the laminate and connected to the plurality of negative electrode layers; a substrate including a first electrode pad connected to the first external electrode of the all-solid-state battery element and a second electrode pad connected to the second external electrode of the all-solid-state battery element; a resin sealant covering the all-solid-state battery element and in contact with the substrate; and a housing covering the resin sealant. The resin sealant may include a first resin sealant and a second resin sealant, the first resin sealant covering at least a portion of the all-solid-state battery element, the second resin sealant covering the first resin sealant and in contact with the substrate, and the elastic modulus of the first resin sealant may be different from the elastic modulus of the second resin sealant.

[0027] In addition, the elastic modulus of the first resin sealant may be greater than that of the second resin sealant.

[0028] In addition, the elastic modulus of the first resin sealant may be less than that of the second resin sealant.

[0029] In addition, the resin seal may also include a third resin seal, which covers the second resin seal and contacts the substrate, and the elastic modulus of the third resin seal may be less than that of the second resin seal.

[0030] In addition, the first resin sealant may cover the outer surface of the laminate, the first external electrode may include a first strip portion disposed on the outer surface of the laminate in the first direction, the second external electrode may include a second strip portion disposed on the outer surface of the laminate in the first direction, and the thickness of the first resin sealant may be less than the thickness of the first strip portion and the thickness of the second strip portion.

[0031] Additionally, the outer casing may include metal or alloy.

[0032] Additionally, the housing may include aluminum (Al), aluminum (Al) alloys, steel, stainless steel, or combinations thereof.

[0033] According to another embodiment, an all-solid-state battery includes: an all-solid-state battery element including a stack, a first external electrode, and a second external electrode; the stack includes a plurality of solid electrolyte layers, a plurality of positive electrode layers, and a plurality of negative electrode layers stacked in a first direction; the first external electrode is disposed outside the stack and connected to the plurality of positive electrode layers; the second external electrode is disposed outside the stack and connected to the plurality of negative electrode layers; and a resin sealant extending between the first external electrode and the second external electrode, and covering a portion of the first external electrode and a portion of the second external electrode. The resin sealant may include a plurality of layers and may be spaced apart from the plurality of positive electrode layers and the plurality of negative electrode layers.

[0034] Additionally, the laminate may include multiple surfaces, the first external electrode may be disposed on a first surface among the multiple surfaces to connect to the multiple positive electrode layers, the second external electrode may be disposed on a second surface among the multiple surfaces to connect to the multiple negative electrode layers, the first surface may be opposite to the second surface, and among the multiple surfaces, the resin sealant may cover the surfaces other than the first surface and the second surface.

[0035] In addition, at least two of the plurality of layers of the resin sealant may comprise different materials.

[0036] In addition, at least two of the plurality of layers of the resin sealant may have different elastic moduli.

[0037] In addition, the elastic modulus of one of the plurality of layers of the resin sealant may be greater than the elastic modulus of another layer of the plurality of layers of the resin sealant that covers that layer.

[0038] In addition, the elastic modulus of one of the plurality of layers of the resin sealant may be greater than or equal to 100 MPa, and the elastic modulus of another layer of the plurality of layers of the resin sealant may be less than or equal to 0.15 MPa.

[0039] In addition, at least two of the plurality of layers of the resin seal can contact the first external electrode and the second external electrode.

[0040] According to another embodiment, an all-solid-state battery includes: an all-solid-state battery element including a laminate, a first external electrode, and a second external electrode, the laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers, and a plurality of negative electrode layers stacked in a first direction, the first external electrode being disposed outside the laminate and connected to the plurality of positive electrode layers, and the second external electrode being disposed outside the laminate and connected to the plurality of negative electrode layers; a substrate including a first electrode pad connected to the first external electrode of the all-solid-state battery element and a second electrode pad connected to the second external electrode of the all-solid-state battery element; a first resin sealant covering the all-solid-state battery element and disposed between the all-solid-state battery element and the substrate for contact with the substrate; a second resin sealant covering the first resin sealant and contacting the substrate; and a housing covering the second resin sealant.

[0041] In addition, the elastic modulus of the first resin sealant may be different from that of the second resin sealant.

[0042] In addition, the elastic modulus of the first resin sealant may be greater than that of the second resin sealant.

[0043] In addition, the first resin seal can cover the first external electrode and the second external electrode and can contact the first external electrode and the second external electrode.

[0044] In addition, the second resin seal can be spaced apart from the first external electrode and the second external electrode.

[0045] In addition, the second resin sealant may be spaced apart from the laminate.

[0046] Additionally, on the substrate, the first resin sealant may be disposed between the first electrode pad and the second electrode pad, and the second resin sealant may be disposed in the region outside the first electrode pad and the second electrode.

[0047] Beneficial effects of the invention According to the all-solid-state battery of the embodiment, the expansion of the all-solid-state battery during charging and discharging can be suppressed.

[0048] According to the embodiment of the all-solid-state battery, moisture can be prevented from entering. Attached Figure Description

[0049] Figure 1This is a schematic perspective view of an all-solid-state battery according to an embodiment.

[0050] Figure 2 It is shown schematically. Figure 1 A 3D view of an all-solid-state battery component.

[0051] Figure 3 It is shown schematically. Figure 1 A three-dimensional diagram of a stacked body.

[0052] Figure 4 It is along Figure 1 A cross-sectional view taken from line IV-IV'.

[0053] Figure 5A It is shown schematically. Figure 2 A partial cross-sectional view of the positive electrode layer of an all-solid-state battery element.

[0054] Figure 5B It is shown schematically. Figure 2 A partial cross-sectional view of the negative electrode layer of an all-solid-state battery element.

[0055] Figure 6 This is a schematic cross-sectional view showing an all-solid-state battery according to another embodiment.

[0056] Figure 7 This is a schematic cross-sectional view showing an all-solid-state battery according to yet another embodiment.

[0057] Figure 8 This is a schematic cross-sectional view showing an all-solid-state battery according to another embodiment.

[0058] Figure 9 This is a schematic cross-sectional view showing an all-solid-state battery according to yet another embodiment.

[0059] Figure 10 This is a schematic cross-sectional view showing an all-solid-state battery according to another embodiment.

[0060] Figure 11 This is a graph showing the results of the initial charge / discharge test performed on the all-solid-state battery prepared according to the example at a temperature of 25°C and a humidity of 25%.

[0061] Figure 12 This is a graph showing the results of the initial charge / discharge test performed on the all-solid-state battery prepared according to the comparative example at a temperature of 25°C and a humidity of 25%.

[0062] Figure 13 This is a graph showing the results of the initial charge / discharge test performed on the all-solid-state battery prepared according to the example at a temperature of 25°C and a humidity of 55%.

[0063] Figure 14 This is a graph showing the results of the initial charge / discharge test performed on the all-solid-state battery prepared according to the comparative example at a temperature of 25°C and a humidity of 55%. Detailed Implementation

[0064] In the following detailed description, only specific embodiments of the invention are shown and described by way of illustration only. The drawings and descriptions are to be considered illustrative rather than restrictive in nature. Throughout the specification, the same reference numerals denote the same elements. Furthermore, some components in the drawings may be enlarged, omitted, or shown schematically, and the dimensions of the individual components do not perfectly reflect the actual dimensions.

[0065] The accompanying drawings are provided to help to readily understand the embodiments disclosed in this specification, and the technical spirit disclosed in this specification is not limited to the drawings. It will be understood that the invention includes all variations, equivalents and alternatives included within the spirit and scope of the invention.

[0066] Ordinal terms such as "first" and "second" are used to describe various constituent elements, but these constituent elements are not limited by these terms. These terms are only used to distinguish one constituent element from another.

[0067] 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" a reference portion, the element being located above or below the reference portion does not necessarily mean that the element is located "above" or "on" in a direction opposite to the direction of gravity.

[0068] Throughout this specification, it will be understood that the terms "comprising" and "having" are intended to specify the presence of the features, quantities, steps, operations, constituent elements, components, or combinations thereof described in the specification, without precluding the possibility of the presence or addition of one or more other features, quantities, steps, operations, constituent elements, components, or combinations thereof. Therefore, unless explicitly stated otherwise, the words "comprising" and variations such as "including" or "having" will be understood to imply the inclusion of the stated elements but not the exclusion of any other elements.

[0069] Furthermore, throughout the instruction manual, when referred to as "on a plane," it indicates the view of the target portion from above, and when referred to as "on a cross section," it indicates the view of the cross section obtained by vertically cutting the target portion from the side.

[0070] Furthermore, throughout the specification, when referred to as “connected,” this not only indicates that two or more constituent elements are directly connected, but also that two or more constituent elements are indirectly connected through another constituent element. It can also indicate that two or more constituent elements are physically connected, electrically connected, or that even if two or more constituent elements are called by different names according to their location and function, they are still a single unit.

[0071] Figure 1 This is a schematic perspective view of an all-solid-state battery according to an embodiment. Figure 2 It is shown schematically. Figure 1 A 3D view of an all-solid-state battery component. Figure 3 It is shown schematically. Figure 1 A three-dimensional diagram of the stacked body, and Figure 4 It is along Figure 1 A cross-sectional view taken from line IV-IV'.

[0072] Reference Figure 1 , Figure 2 , Figure 3 and Figure 4 The all-solid-state battery 1000 according to this embodiment includes an all-solid-state battery element 1100 and a resin seal 1200.

[0073] First, when defining directions for the purpose of clearly describing this embodiment, the L-axis, W-axis, and T-axis shown in the accompanying drawings represent the axes representing the length, width, and thickness directions of the all-solid-state battery 1000, respectively.

[0074] 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 of the components in which the stacked laminate 100 is formed.

[0075] The length direction (L-axis direction) is a direction parallel to the wide surface (main surface) of the sheet assembly, and can be a direction intersecting (or orthogonal) to the thickness direction (T-axis direction). For example, the length direction (L-axis direction) can be the direction in which the first external electrode 300 and the second external electrode 400 are opposite each other.

[0076] The width direction (W-axis direction) is the direction parallel to the wide surface (main surface) of the sheet assembly, and can be a direction that intersects (or is orthogonal) both the thickness direction (T-axis direction) and the length direction (L-axis direction).

[0077] The all-solid-state battery element 1100 includes a stack 100, a first external electrode 300, and a second external electrode 400.

[0078] 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 parallelepiped shape, but the portions corresponding to corners or vertices may have a rounded shape.

[0079] In this embodiment, for ease of description, 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, 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, and 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.

[0080] Therefore, the first direction in 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 that are 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), or they can be the width direction (W-axis direction) and the thickness direction (T-axis direction), respectively.

[0081] The length of the laminate 100 can be defined as: the maximum length of a plurality of line segments in an optical microscope or scanning electron microscope (SEM) photograph of a cross-section of the laminate 100 at its central portion in the width direction (W-axis direction) along the length direction (L-axis direction) and thickness direction (T-axis direction), where each line segment connects to the two outermost boundary lines of the laminate 100 shown in the cross-sectional photograph along the length direction (L-axis direction) and parallel to the length direction (L-axis direction). Note that the length of the laminate 100 can also be defined as: the minimum length of a plurality of line segments in a cross-sectional photograph, where each line segment connects to the two outermost boundary lines of the laminate 100 shown in the cross-sectional photograph along the length direction (L-axis direction) and parallel to the length direction (L-axis direction). On the other hand, the length of the laminate 100 can mean the arithmetic mean of the lengths of at least two of the multiple line segments of the laminate 100 shown in the cross-sectional photograph, which are opposite each other in the length direction (L-axis direction) to the two outermost boundary lines and are parallel to the length direction (L-axis direction).

[0082] The thickness of the laminate 100 can be defined as: the maximum value among multiple line segments of the laminate 100 in the thickness direction (T-axis direction) and parallel to the two outermost boundary lines of the laminate 100 in the thickness direction (T-axis direction) shown in the cross-sectional photograph of the central portion of the laminate 100 in the width direction (W-axis direction) and in the length direction (L-axis direction) and thickness direction (T-axis direction). Note that the thickness of the laminate 100 can also be defined as: the minimum value among multiple line segments of the laminate 100 in the thickness direction (T-axis direction) and parallel to the two outermost boundary lines of the laminate 100 in the thickness direction (T-axis direction) shown in the cross-sectional photograph. On the other hand, the thickness of the laminate 100 can mean the arithmetic mean of the lengths of at least two of the multiple line segments of the laminate 100 shown in the cross-sectional photograph, which are opposite to the two outermost boundary lines in the thickness direction (T-axis direction) and parallel to the thickness direction (T-axis direction).

[0083] The width of the laminate 100 can be defined as: the maximum length of each line segment in an optical microscope or scanning electron microscope (SEM) photograph of a cross-section of the laminate 100 at its central portion in the thickness direction (T-axis direction) along the length direction (L-axis direction) and the width direction (W-axis direction), where each line segment connects to the two outermost boundary lines of the laminate 100 shown in the cross-sectional photograph in the width direction (W-axis direction) and is parallel to the width direction (W-axis direction). Note that the width of the laminate 100 can also be defined as: the minimum length of each line segment in the cross-sectional photograph of the laminate 100, where each line segment connects to the two outermost boundary lines of the laminate 100 shown in the cross-sectional photograph in the width direction (W-axis direction) and is parallel to the width direction (W-axis direction). On the other hand, the width of the stack 100 can mean the arithmetic mean of the lengths of at least two of the multiple line segments of the stack 100 shown in the cross-sectional photograph, which are opposite to each other in the width direction (W-axis direction) of the two outermost boundary lines and are parallel to the width direction (W-axis direction).

[0084] The laminate 100 may include a solid electrolyte layer 110, a positive electrode layer 130, a negative electrode layer 150, an upper protective layer 160, a lower protective layer 170, and an edge portion 180.

[0085] There can be multiple solid electrolyte layers 110, positive electrode layers 130, and negative electrode layers 150. The positive electrode layers 130 and negative electrode layers 150 can be stacked alternately in the thickness direction (T-axis direction), with the solid electrolyte layer 110 positioned between the positive electrode layers 130 and negative electrode layers 150. This stacked structure can be repeated within the laminate 100, and the electrode layer closest to the fifth surface S5 of the laminate 100 can be either the positive electrode layer 130 or the negative electrode layer 150, and the electrode layer closest to the sixth surface S6 can be either the negative electrode layer 150 or the positive electrode layer 130.

[0086] The positive electrode layer 130 may be disposed on one surface of the solid electrolyte layer 110, and the negative electrode layer 150 may be disposed on the other surface of the solid electrolyte layer 110.

[0087] The solid electrolyte layer 110 includes a solid electrolyte. The solid electrolyte can be used as a channel for lithium (Li) ions.

[0088] The solid electrolyte included in the solid electrolyte layer 110 may include a glass-ceramic-based electrolyte containing lithium halides (LiX, where X is a halogen element such as F, Br, Cl, I, etc.). Glass-ceramics (or microcrystalline glass) refer to a mixture of crystalline and amorphous materials that exhibit peaks and bulges in X-ray diffraction, electron beam diffraction, etc., and are crystallographically consistent. Therefore, glass-ceramic-based electrolytes are electrolytes that undergo partial crystallization through sintering and contain a mixture of amorphous and crystalline materials.

[0089] Glass-ceramic based electrolytes may include mixtures of amorphous materials and two or more types of crystalline materials. Additionally, the crystalline materials included in the glass-ceramic based electrolyte may include lithium compound crystalline phases containing lithium.

[0090] When a glass-ceramic-based electrolyte is included in the solid electrolyte layer 110, sufficient densification is achieved after sintering, thereby enabling high ionic conductivity.

[0091] Glass-ceramic based electrolytes 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). As a specific example, glass-ceramic based electrolytes may include Li₂O-B₂O₃-SiO₂-P₂O₅-GeO₂-LiCl.

[0092] Optionally, the solid electrolyte included in the solid electrolyte layer 110 may include a lithium borosilicate-based electrolyte (hereinafter, also referred to as an LBSO-based electrolyte). The LBSO-based electrolyte is a glassy electrolyte, and glass refers to a crystallographically amorphous material that exhibits a hump peak in X-ray diffraction, electron beam diffraction, etc.

[0093] When the LBSO-based electrolyte is included in the solid electrolyte layer 110, it can maintain an amorphous state during sintering while reducing the sintering temperature. Therefore, it has the advantages of achieving high ionic conductivity and having low reactivity with the electrodes. The LBSO-based electrolyte may include lithium (Li), boron (B), silicon (Si), aluminum (Al), phosphorus (P), germanium (Ge), and sulfur (S).

[0094] Optionally, the solid electrolyte included in the solid electrolyte layer 110 may be one or more types selected from the group consisting of garnet type, Na superionic conductor (NASICON) type, lithium superionic conductor (LISICON) type, perovskite type, and lithium phosphorus oxynitride (LiPON) type.

[0095] In the region where the edge portion 180 to be described later is provided, a material having low ionic conductivity and low electronic conductivity (i.e., an insulating material) may be present, or a material having an ionic conductivity (or electronic conductivity) approximate to that of the solid electrolyte may be present. For example, when a material having an ionic conductivity (or electronic conductivity) approximate to that of the solid electrolyte is present in the region, the material may be the same as or different from the solid electrolyte in other regions. In another example, a material having an ionic conductivity (or electronic conductivity) approximate to that of the solid electrolyte and an insulating material may coexist in the region.

[0096] The garnet-type solid electrolyte may refer to lithium lanthanum zirconate oxide (LLZO) represented by Li a La b Zr c O 12 (such as Li7La3Zr2O 12 ), and the NASICON-type solid electrolyte may include lithium aluminum titanium phosphate (LATP) (Li 1+x Al x M 2-x (PO4)3 (LAMP) (where 0 < x < 2, and M is Zr, Ti, or Ge) formed by introducing Ti into the compound of 1+x Al x Ti 2-x (PO4)3) (where 0 < x < 1), and lithium-rich 1+xAl x Ge 2-x (PO4)3 (where 0 < x < 1) (such as Li 1.3 Al 0.3 Ge 1.7 (PO4)3) represents lithium aluminum germanium phosphate (LAGP) and / or lithium zirconium phosphate (LZP) (LiZr2(PO4)3).

[0097] In addition, the LISICON-type solid electrolyte may include a solid solution oxide represented by xLi3AO4-(1-x)Li4BO4 (where A is P, As, V, etc., and B is Si, Ge, Ti, etc.), such as Li4Zn(GeO4)4, Li 10 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 etc., and a solid solution sulfide such as Li2S-P2S5, Li2S-SiS2, Li2S-SiS2-P2S5, Li2S-GeS2, etc. represented by Li 4-x M 1-y M' y S4 (where M is Si or Ge, and M' is P, Al, Zn or Ga).

[0098] In addition, the perovskite-type solid electrolyte may include lithium lanthanum titanate oxide (LLTO) represented by Li 3x La 2 / 3-x □ 1 / 3-2x TiO3 (where 0 < x < 0.16, and □ is a vacancy) (such as Li 1 / 8 La 5 / 8 TiO3), and the LiPON-type solid electrolyte may include nitrides such as lithium phosphorus oxynitride (such as Li 2.8 PO 3.3 N 0.46 ).

[0099] The positive electrode layer 130 may be exposed to the outside of the laminate 100 from the first surface S1 of the laminate 100 and may be connected to the first external electrode 300. <00003​​​​​​​For example, the positive electrode current collector 133 can be made using a plate-like component or a thin component. As another example, the positive electrode current collector 133 can be a porous body having a network-like or mesh-like structure.

[0102] The positive current collector 133 may include a first surface 133a and a second surface 133b. The first surface 133a and the second surface 133b are opposite to each other in the thickness direction (T-axis direction).

[0103] For example, the positive current collector 133 may include, but is not limited to, a porous metal plate made of stainless steel, nickel (Ni), copper (Cu), tin (Sn), aluminum (Al), or alloys thereof.

[0104] In addition, the positive current collector 133 may be coated with an antioxidant metal or alloy film to prevent oxidation.

[0105] The positive current collector 133 may also include a carbon substrate-like component, a thin component, or a linear component. The positive current collector 133 may include a conductive carbon material. The conductive carbon material may include graphite, conductive fibers (such as carbon nanotubes (CNTs) or vapor-grown carbon fibers (VGCF)) or conductive carbon (such as carbon black).

[0106] In addition, the positive electrode current collector may also include one or more types of solid electrolytes.

[0107] The first positive electrode active material layer 135 and the second positive electrode active material layer 136 may include positive electrode active material and may be disposed on the surface of the positive electrode current collector 133. The first positive electrode active material layer 135 and the second positive electrode active material layer 136 may be formed by printing positive electrode active material on one or both surfaces of the positive electrode current collector 133. However, the method of forming the positive electrode active material layer is not limited to this.

[0108] The positive electrode active material included in the positive electrode active material layers 135 and 136 may include a material containing lithium (Li) ions. The positive electrode active material can reversibly insert and extract lithium ions. That is, the positive electrode active material may contain lithium ions and be used to provide 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.

[0109] 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 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 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 eO2 (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 represents Ni, Co, or Mn; M represents Al, Ni, Co, Mn, Cr, Fe, Mg, Sr, V, Nb, Ti, or rare earth elements; D represents O, F, S, or P; E represents Co or Mn; X represents F, S, or P; G represents Al, Cr, Mn, Fe, Mg, La, Ce, Sr, or V; Q represents Ti, Mo, or Mn; R represents Cr, V, Fe, Sc, or Y; and J represents V, Cr, Mn, Co, Ni, or Cu.

[0110] 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 and 0 ≤ y ≤ 0.5), LiFePO4, TiS2, FeS2, TiS3 or FeS3, but not limited to these.

[0111] The positive electrode active material may selectively include conductive materials and binders. However, because organic materials such as binders decompose during the sintering process, organic materials may not remain on the positive electrode active material layer of the obtained positive electrode current collector.

[0112] There are no particular restrictions on the conductive materials, as long as they are conductive and do not cause chemical changes in the all-solid-state battery 1000. For example, the following materials can be used: graphite, such as natural or artificial graphite; carbon-based materials, such as carbon black (acetylene black, Ketjen black). ® Carbon black produced by 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), copper (Cu), etc.), oxides of metallic components, nitrides of metallic components, or fluorides of metallic components; conductive whiskers, such as zinc oxide or potassium titanate; conductive metal oxides, such as titanium oxide; conductive materials, such as polyphenylene derivatives.

[0113] Adhesives can be used to improve the bonding strength of active materials, conductive materials, etc. Adhesives may include, but are not limited to, 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 (SBR), fluororubber, and various copolymers.

[0114] Furthermore, the positive electrode layer 130 may also contain a solid electrolyte component. The solid electrolyte component may contain one or more of the components mentioned above and can serve as an ion conduction channel in the positive electrode layer. Therefore, the interfacial resistance can be reduced.

[0115] The negative electrode layer 150 may be exposed to the outside of the laminate 100 from the second surface S2 of the laminate 100 and may be connected to the second external electrode 400.

[0116] Reference Figure 4 and Figure 5B The negative electrode layer 150 may include a negative electrode current collector 153, a first negative electrode active material layer 155, and a second negative electrode active material layer 156.

[0117] For example, the negative electrode current collector 153 may include a plate-like member or a thin member. As another example, the negative electrode current collector 153 may include a porous body having a network-like, mesh-like, or similar structure.

[0118] The negative electrode current collector 153 may include a first surface 153a and a second surface 153b. The first surface 153a and the second surface 153b are opposite to each other in the thickness direction (T-axis direction).

[0119] For example, the negative electrode current collector 153 may include, but is not limited to, a porous metal plate made of stainless steel, nickel (Ni), copper (Cu), tin (Sn), aluminum (Al), or alloys thereof.

[0120] In addition, the negative electrode current collector 153 may be coated with an antioxidant metal or alloy film to prevent oxidation.

[0121] Similar to the positive electrode current collector 133, the negative electrode current collector 153 may include a conductive carbon-based material and may include one or more types of solid electrolytes. The negative electrode current collector 153 may be the same as the negative electrode active material layers 155 and 156.

[0122] The first negative electrode active material layer 155 and the second negative electrode active material layer 156 may include a negative electrode active material and may be provided on the surface of the negative electrode current collector 153. The first negative electrode active material layer 155 and the second negative electrode active material layer 156 may be formed by printing the negative electrode active material on one or both surfaces of the negative electrode current collector 153. However, the method of forming the negative electrode active material layer is not limited thereto.

[0123] The negative electrode active material in the negative electrode active material layers 155 and 156 may store the lithium ions that have moved from the positive electrode and release the lithium ions during the discharge of the all-solid-state battery, thereby generating electric energy. A carbon-based material, silicon, silicon oxide, silicon-based alloy, silicon-carbon-based material composite, tin, tin-based alloy, tin-carbon composite, metal oxide, or a combination thereof may be used as the negative electrode active material. The negative electrode active material may contain lithium metal and / or a lithium metal alloy.

[0124] The lithium metal alloy may contain lithium and a metal / metalloid capable of forming an alloy with lithium. For example, the metal / metalloid capable of forming an alloy with lithium may include Si, Sn, Al, Ge, Pb, Bi, Sb, Si-AM alloy (where AM is an alkali metal, alkaline earth metal, element in Groups 13 to 16, 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, element in Groups 13 to 16, transition metal, transition metal oxide such as lithium titanate (Li4Ti5O 12 ), rare earth element, or a combination thereof, and does not include Sn), MnO x (where 0 < x ≤ 2), etc.

[0125] The element AM may include 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.

[0126] In addition, the metal / metalloid oxides capable of alloying with lithium may include lithium titanium oxides, vanadium oxides, lithium vanadium oxides, SnO2, SiO x (where 0 < x < 2), etc. For example, the negative electrode active material may include one or more elements selected from the group consisting of elements in Groups 13 to 16 of the periodic table. For example, the negative electrode active material may contain one or more elements selected from the group consisting of Si, Ge, and Sn.

[0127] The carbon-based materials may include crystalline carbon, amorphous carbon, or a mixture thereof. The crystalline carbon may be graphite, such as natural graphite or artificial graphite in an amorphous form, disk form, flake form, spherical form, or fiber form. In addition, the amorphous carbon may include, but is not limited to, soft carbon (low-temperature calcined carbon), hard carbon, mesophase pitch carbide, calcined coke, graphene, carbon black, fullerene soot, carbon nanotubes, carbon fibers, etc.

[0128] Silicon may include at least one selected from the group consisting of Si, SiO x (where 0 < x < 2, for example, 0.5 to 1.5), Sn, SnO2, or a silicon-containing metal alloy and their mixtures. For example, the silicon-containing metal alloy may include one or more of Al, Sn, Ag, Fe, Bi, Mg, Zn, In, Ge, Pb, or Ti and silicon.

[0129] The negative electrode active material may selectively include a conductive material and an adhesive.

[0130] The conductive material is not particularly limited as long as it has conductivity and does not cause chemical changes in the all-solid-state battery 1000. For example, the following materials may 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 thermal cracking carbon black); conductive fibers, such as carbon fibers, metal fibers, etc.; carbon fluorides; metal components (such as lithium (Li), tin (Sn), aluminum (Al), nickel (Ni), copper (Cu), etc.), oxides of metal components, nitrides of metal components, or fluorides of metal components); conductive whiskers, such as zinc oxide and potassium titanate; conductive metal oxides, such as titanium oxides; conductive materials, such as polyphenylene derivatives, etc.

[0131] The adhesive can be used to improve the bonding strength of the active material, conductive material, etc. The adhesive may include, but is not limited to, 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 (SBR), fluororubber, various copolymers, etc.

[0132] Furthermore, the negative electrode layer 150 may also contain a solid electrolyte component. The solid electrolyte component may contain one or more of the components mentioned above and can serve as an ion conduction channel in the negative electrode layer. Therefore, the interfacial resistance can be reduced.

[0133] The upper protective layer 160 and the lower protective layer 170 can be the outermost layers respectively disposed on the fifth surface S5 and the sixth surface S6 of the laminate 100. That is, the upper protective layer 160 can be the outermost layer located on the fifth surface S5 of the laminate 100, and the lower protective layer 170 can be the outermost layer located on the sixth surface S6 of the laminate 100. The upper protective layer 160 and the lower protective layer 170 can improve moisture-proof reliability by preventing moisture penetration and can prevent damage caused by physical stress and chemical stress.

[0134] The upper protective layer 160 and the lower protective layer 170 may be insulating layers comprising an insulating material (i.e., a non-conductive (ionic) material).

[0135] The upper protective layer 160 and the lower protective layer 170 may include, but are not limited to, at least one ceramic material selected from the group consisting of, for example, 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 of these materials and / or nitrides of these materials, and any other suitable ceramic material. Additionally, the upper protective layer 160 and the lower protective layer 170 may selectively include the aforementioned solid electrolyte and may include one or more types of solid electrolytes. However, this disclosure is not limited thereto.

[0136] For example, the edge portion 180 may be provided on the solid electrolyte layer 110 and located in a region other than the region where the positive electrode layer 130 or the negative electrode layer 150 is provided. If a positive electrode layer 130 is provided on the solid electrolyte layer 110, the edge portion 180 may be provided in a region other than the region where the positive electrode layer 130 is provided. Similarly, if a negative electrode layer 150 is provided on the solid electrolyte layer 110, the edge portion 180 may be provided in a region other than the region where the negative electrode layer 150 is provided.

[0137] Reference Figure 4 The edge portion 180 may form part of the first surface S1 and part of the second surface S2 of the laminate 100. In addition, although not shown, the edge portion 180 may also form part of the third surface S3 and part of the fourth surface S4 of the laminate 100.

[0138] The edge portion 180 can be configured to compensate for the height difference between the solid electrolyte layer 110 and the positive electrode layer 130, and the height difference between the solid electrolyte layer 110 and the negative electrode layer 150. For example, the edge portion 180 can be disposed on the same surface as the surface of the positive electrode layer 130 and the same surface as the surface of the negative electrode layer 150. The edge portion 180 can compensate for the height difference between the solid electrolyte layer 110 and the positive electrode layer 130, or the height difference between the solid electrolyte layer 110 and the negative electrode layer 150. This increases the density between the solid electrolyte layer 110 and the electrode layers, preventing interlayer delamination or warping caused by sintering during the manufacturing process of all-solid-state batteries.

[0139] Furthermore, the edge portion 180 may include a moisture-resistant material with low lithium (Li) ion conductivity. In this case, the edge portion 180 can protect the active material layers 135, 136, 155, and 156 from moisture penetration or lithium (Li) ion leakage. For example, the edge portion 180 may include an insulating material or an electrolyte material, and may include an ion conductivity of less than or equal to 1.0 × 10⁻⁶. -10 Materials with S / cm.

[0140] The edge portion 180 may include an insulating material (i.e., a material that does not have electrical (ionic) conductivity).

[0141] The edge portion 180 may include, but is not limited to, at least one ceramic material selected from, for example, 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 of these materials and / or nitrides of these materials, or any other suitable ceramic material.

[0142] Furthermore, the edge portion 180 may include a solid electrolyte that is the same as or different from the solid electrolyte included in the solid electrolyte layer described above, and may include one or more types of solid electrolytes. However, this disclosure is not limited thereto.

[0143] Additionally, in the edge portion 180, a material with low ionic conductivity and low electronic conductivity (i.e., an insulating material) may be present, and a material with ionic conductivity (or electronic conductivity) approximating that of the solid electrolyte may also be present. For example, when a material with ionic conductivity (or electronic conductivity) approximating that of the solid electrolyte is present in the edge portion, this material may be the same as or different from the solid electrolyte in other regions. As another example, a material with ionic conductivity (or electronic conductivity) approximating that of the solid electrolyte and an insulating material may coexist in the edge portion.

[0144] The first external electrode 300 and the second external electrode 400 are disposed on the outside of the laminate 100.

[0145] The first external electrode 300 is connected to the positive electrode layer 130 on the first surface S1 of the laminate 100.

[0146] For example, the first external electrode 300 may extend onto the third surface S3, the fourth surface S4, the fifth surface S5 and the sixth surface S6 of the laminate 100 to partially cover the respective surfaces.

[0147] The second external electrode 400 is connected to the negative electrode layer 150 on the second surface S2 of the laminate 100.

[0148] For example, the second external electrode 400 may extend onto the third surface S3, the fourth surface S4, the fifth surface S5 and the sixth surface S6 of the laminate 100 to partially cover the respective surfaces.

[0149] Furthermore, in some embodiments, the first external electrode 300 and the second external electrode 400 may extend onto the fifth surface S5 or the sixth surface S6 to partially cover the respective surfaces.

[0150] The first external electrode 300 may include a first connecting portion 301, a first strip portion 303, and a first edge portion 305.

[0151] The first connecting portion 301 covers the first surface S1 of the laminate 100 and is electrically connected to the positive electrode layer 130.

[0152] In some embodiments, the first connecting portion 301 may cover a portion of the first surface S1 of the laminate 100.

[0153] The first strip 303 extends from the first connecting portion 301 to cover a portion of the fifth surface S5 and a portion of the sixth surface S6 of the laminate 100. The first strip 303 allows the first external electrode 300 to adhere more firmly to the laminate 100.

[0154] The first edge portion 305 may be the portion that connects the first connecting portion 301 and the first belt portion 303.

[0155] The second external electrode 400 may include a second connecting portion 401, a second strip portion 403, and a second edge portion 405.

[0156] The second connecting part 401 covers the second surface S2 of the laminate 100 and is electrically connected to the negative electrode layer 150.

[0157] In some embodiments, the second connection portion 401 may cover a portion of the second surface S2 of the laminate 100.

[0158] The second strip 403 extends from the second connecting portion 401 to cover a portion of the fifth surface S5 and a portion of the sixth surface S6 of the laminate 100. The second strip 403 allows the second external electrode 400 to adhere more firmly to the laminate 100.

[0159] The second edge portion 405 may be the portion that connects the second connecting portion 401 and the second belt portion 403.

[0160] Based on optical microscope or scanning electron microscope (SEM) images of a cross-section taken at the central portion of the all-solid-state battery 1000 in the width direction (W-axis direction) along the length direction (L-axis direction) and thickness direction (T-axis direction), in the all-solid-state battery 1000 shown in the aforementioned cross-sectional images, the first connecting portion 301 and the second connecting portion 401 may have a shape substantially parallel to the thickness direction (T-axis direction), the first strip portion 303 and the second strip portion 403 may have a shape substantially parallel to the length direction (L-axis direction), and the first edge portion 305 and the second edge portion 405 may have a curved shape. The aforementioned curved shape may be a tangent shape, the slope of which changes from a direction parallel to the thickness direction (T-axis direction) to a direction parallel to the length direction (L-axis direction) (or in the opposite direction).

[0161] For example, the first external electrode 300 and the second external electrode 400 can be sintered electrodes comprising a conductive metal and glass. As another example, the first external electrode 300 and the second external electrode 400 can be resin-based electrodes comprising a conductive metal and a matrix resin. In this case, the matrix resin can be epoxy resin.

[0162] For example, the first external electrode 300 and the second external electrode 400 can be made by coating a paste containing a conductive metal onto each of the first surface S1 and the second surface S2 of the laminate 100, or by transferring a dry film generated by drying the conductive paste onto the laminate 100 and then sintering it. However, the method of forming the first external electrode 300 and the second external electrode 400 is not limited thereto. The conductive metal may include, but is not limited to, one or more of, such as copper (Cu), nickel (Ni), tin (Sn), palladium (Pd), platinum (Pt), gold (Au), silver (Ag), tungsten (W), titanium (Ti), lead (Pb), and alloys thereof.

[0163] Furthermore, by forming plating layers on the first external electrode 300 and the second external electrode 400 respectively, the mounting characteristics of the external electrodes can be improved. The plating layers may include at least one 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, but this disclosure is not limited thereto. The plating layers may be formed in one or more layers.

[0164] The resin seal 1200 may partially cover the all-solid-state battery element 1100. The resin seal 1200 may expose a portion of the first external electrode 300 and a portion of the second external electrode 400 of the all-solid-state battery element 1100.

[0165] The resin seal 1200 may include a first resin seal 1210 and a second resin seal 1220.

[0166] The first resin seal 1210 can be a harder material than the second resin seal 1220. That is, the elastic deformation resistance of the first resin seal 1210 can be greater than that of the second resin seal 1220. Therefore, the elastic modulus (or Young's modulus) of the first resin seal 1210 can be greater than that of the second resin seal 1220.

[0167] The first resin sealant 1210 may cover at least a portion of the outer surface of the laminate 100.

[0168] For example, the first resin sealant 1210 may cover a portion of the third surface S3, a portion of the fourth surface S4, a portion of the fifth surface S5, and a portion of the sixth surface S6 of the laminate 100.

[0169] Additionally, the first resin seal 1210 may cover a portion of the first strip 303 and a portion of the second strip 403.

[0170] The region from the end of the first strip portion 303 near the center of the laminate 100 in the longitudinal direction (L-axis direction) to the point spaced apart from the first edge portion 305 can be covered by the first resin sealant 1210. That is, the first resin sealant 1210 may not be provided on the first edge portion 305 of the first external electrode 300. Similarly, the region from the end of the second strip portion 403 near the center of the laminate 100 in the longitudinal direction (L-axis direction) to the point spaced apart from the second edge portion 405 can be covered by the first resin sealant 1210. That is, the first resin sealant 1210 may not be provided on the second edge portion 405 of the second external electrode 400.

[0171] In this way, the first resin seal 1210 can cover the outer surface of the laminate 100 exposed through the first strip 303 and the second strip 403, and can also cover a portion of the first strip 303 and a portion of the second strip 403.

[0172] The first resin sealant 1210 may include phenolic epoxy resin, phenolic resin, phenolic varnish epoxy resin, ortho-cresol resin, acrylic resin, or combinations thereof, but this embodiment is not limited thereto.

[0173] The elastic modulus of the first resin seal 1210 can be greater than or equal to 100 MPa and less than or equal to 300 MPa. If the elastic modulus of the first resin seal 1210 is less than 100 MPa, it may be difficult to effectively prevent the volume expansion of the all-solid-state battery, and if the elastic modulus exceeds 300 MPa, the brittleness may increase, making the all-solid-state battery susceptible to impact.

[0174] The elastic modulus of the first resin seal 1210 can be measured by methods known in the art. For example, the first resin seal can be peeled off from the all-solid-state battery, a sample with dimensions of 10 mm × 2 mm × 4 mm can be cut, and the elastic modulus can be measured by using a dynamic mechanical analyzer (DMA) (RSA-G2 available from TA instruments) while the temperature is increased from 30 °C at a rate of 3 °C / min.

[0175] The tensile strength of the first resin seal 1210 can be greater than or equal to 82 MPa and less than or equal to 85 MPa. If the tensile strength of the first resin seal 1210 is less than 82 MPa, the brittleness may increase, making the all-solid-state battery susceptible to impact. If the tensile strength exceeds 85 MPa, the resistance to elastic deformation will decrease, making it difficult to prevent the volume expansion of the all-solid-state battery.

[0176] The tensile strength of the first resin seal 1210 can be measured by methods known in the art. For example, the first resin seal can be peeled off from the all-solid-state battery, a sample with dimensions of 10 mm × 2 mm × 4 mm can be cut, and the tensile strength can be measured by using a dynamic mechanical analyzer (DMA) (RSA-G2 available from TA instruments) while the temperature is increased from 30 °C at a rate of 3 °C / min.

[0177] The thickness of the first resin seal 1210 can be greater than or equal to 1 μm and less than or equal to 1 mm. If the thickness of the first resin seal 1210 is less than 1 μm, it may be difficult to prevent the volume expansion of the all-solid-state battery, and if the thickness exceeds 1 mm, the overall encapsulation thickness of the all-solid-state battery becomes greater than the required thickness, which may be disadvantageous in terms of energy density.

[0178] In addition, the thickness of the first resin seal 1210 can be greater than or equal to 10 μm and less than or equal to 500 μm.

[0179] In addition, the thickness of the first resin seal 1210 may be greater than the thickness of the first strip 303, and the thickness of the first resin seal 1210 may be greater than the thickness of the second strip 403.

[0180] Here, the thickness of the first resin seal and the thickness of the strip are measured based on scanning electron microscopy (SEM) images at 10,000x magnification of a cross-section taken at the central portion of the all-solid-state battery 1000 along the length direction (L-axis) and thickness direction (T-axis). The thickness of the first resin seal can be the maximum value of the length of the line segment parallel to the thickness direction (T-axis) and connecting the laminate between the first and second strips, as shown in the aforementioned cross-sectional image, and the length of the outer surface of the first resin seal. The thickness of the strip can be the maximum value of the strip thicknesses shown in the aforementioned cross-sectional image.

[0181] The second resin seal 1220 can be a softer material than the first resin seal 1210. That is, the elastic deformation resistance of the second resin seal 1220 can be smaller than that of the first resin seal 1210. Therefore, the elastic modulus (or Young's modulus) of the second resin seal 1220 can be smaller than that of the first resin seal 1210.

[0182] The second resin seal 1220 may cover the first resin seal 1210 and may expose a portion of the first external electrode 300 and a portion of the second external electrode 400.

[0183] The second resin sealant 1220 can cover the portion of the first strip 303 not covered by the first resin sealant 1210 and the portion of the second strip 403 not covered by the first resin sealant 1210. That is, the second resin sealant 1220 can cover the first strip 303 located between the first edge portion 305 and the first resin sealant 1210. Additionally, the second resin sealant 1220 can cover the second strip 403 located between the second edge portion 405 and the first resin sealant 1210.

[0184] For example, the first strip portion 303 can be divided into a portion covered by the first resin sealant 1210, a portion covered by the second resin sealant 1220, and the remaining portion. Similarly, the second strip portion 403 can be divided into a portion covered by the first resin sealant 1210, a portion covered by the second resin sealant 1220, and the remaining portion.

[0185] Furthermore, the second resin seal 1220 can expose the first connection portion 301 of the first external electrode 300 and the second connection portion 401 of the second external electrode 400. That is, the second resin seal 1220 may not be provided on the first connection portion 301 and the second connection portion 401.

[0186] For example, the second resin seal 1220 may include polyimide resin, polyimide silicone resin, silicone resin, polyamide resin, rubber, polyurethane resin, or combinations thereof.

[0187] The elastic modulus of the second resin seal 1220 can be greater than 0 MPa and less than or equal to 0.15 MPa. If the elastic modulus of the second resin seal 1220 exceeds 0.15 MPa, the hardness may increase, thereby reducing the effect of absorbing external impact.

[0188] The elastic modulus of the second resin seal 1220 can be measured by methods known in the art. For example, the second resin seal can be peeled off from the all-solid-state battery, a sample with dimensions of 10 mm × 2 mm × 4 mm can be cut, and the elastic modulus can be measured by using a dynamic mechanical analyzer (DMA) (RSA-G2 available from TA instruments) while the temperature is increased from 30 °C at a rate of 3 °C / min.

[0189] The tensile strength of the second resin seal 1220 can be greater than or equal to 13 MPa and less than or equal to 20 MPa. If the tensile strength of the second resin seal 1220 is less than 13 MPa, its ductility may increase, making it easier to deform under external impact. If the tensile strength exceeds 20 MPa, its hardness may increase, thereby reducing its effectiveness in absorbing external impact.

[0190] The tensile strength of the second resin seal 1220 can be measured by methods known in the art. For example, the second resin seal can be peeled off from the all-solid-state battery, a sample with dimensions of 10 mm × 2 mm × 4 mm can be cut, and the tensile strength can be measured using a dynamic mechanical analyzer (DMA) (RSA-G2 available from TA instruments) while the temperature is increased from 30 °C at a rate of 3 °C / min.

[0191] The thickness of the second resin seal 1220 can be greater than or equal to 1 μm and less than or equal to 1 mm. If the thickness of the second resin seal 1220 is less than 1 μm, it may be difficult to expect the effect of preventing moisture penetration and absorbing external impacts, and if the thickness exceeds 1 mm, the overall encapsulation thickness of the all-solid-state battery becomes greater than the required thickness, which may be disadvantageous in terms of energy density.

[0192] In addition, the thickness of the second resin seal 1220 can be greater than or equal to 10 μm and less than or equal to 500 μm.

[0193] Here, the thickness of the second resin seal is measured based on a scanning electron microscope (SEM) image at 10,000x magnification of a cross-section taken at the central portion of the all-solid-state battery 1000 along the length direction (L-axis) and thickness direction (T-axis). The thickness of the second resin seal can be the maximum value among the thicknesses of the second resin seal measured in the region between the first and second strips shown in the aforementioned cross-sectional image.

[0194] As described above, the elastic modulus of the first resin seal 1210 can be greater than that of the second resin seal 1220. That is, the first resin seal 1210 is a harder material than the second resin seal 1220, and therefore the first resin seal 1210 can undergo smaller elastic deformation.

[0195] When the all-solid-state battery 1000 is in operation, the structures of the positive electrode layer 130 and the negative electrode layer 150 may change, causing the all-solid-state battery 1000 to expand. In this case, the exposed surfaces (i.e., the outer surfaces) of the laminate 100 may primarily expand. According to this embodiment, a first resin sealant 1210 made of a material with a relatively large elastic modulus (i.e., a hard material) contacts the outer surface of the laminate 100, thereby suppressing the expansion of the laminate 100 and preventing moisture penetration by preventing the formation of cracks.

[0196] In addition, a second resin seal 1220 made of a material with a relatively small elastic modulus (i.e., a soft material) covers the first resin seal 1210, thereby protecting the all-solid-state battery 1000 by absorbing externally applied shocks.

[0197] In this way, according to this embodiment, a first resin seal 1210 and a second resin seal 1220 with different elastic moduli are used together to suppress the expansion of the laminate 100 and absorb external impacts, thereby improving the performance of the all-solid-state battery.

[0198] Unlike this embodiment, if the laminate 100 is only covered by the second resin sealant 1220 and not the first resin sealant 1210, then when the laminate 100 expands, the second resin sealant 1220 expands along with the laminate 100, so the effect of preventing crack formation may be insufficient. On the other hand, if the laminate 100 is only covered by the first resin sealant 1210 and not the second resin sealant 1220, the effect of absorbing external impact may be insufficient.

[0199] Furthermore, the second resin seal 1220 can be made of a highly moisture-resistant material. For example, the second resin seal 1220 can be made of a material with a water vapor transfer rate (WVTR) of less than or equal to 1 g / m³. 2 The material is made of a material that provides a moisture absorption rate of less than 0.1 after 24 hours at a temperature of 85°C and a relative humidity of 85%RH. Therefore, in this case, the effect of preventing moisture penetration can be further enhanced.

[0200] Figure 6 This is a schematic cross-sectional view showing an all-solid-state battery according to another embodiment.

[0201] Reference Figure 6 The all-solid-state battery 2000 includes an all-solid-state battery element 1100 and a resin seal 2200.

[0202] The resin seal 2200 may partially cover the all-solid-state battery element 1100. The resin seal 2200 may expose a portion of the first external electrode 300 and a portion of the second external electrode 400 of the all-solid-state battery element 1100.

[0203] The resin seal 2200 may include a first resin seal 2210 and a second resin seal 2220.

[0204] The elastic modulus of the first resin sealant 2210 may be greater than that of the second resin sealant 2220. The first resin sealant 2210 may be a material that is harder than the second resin sealant 2220.

[0205] The first resin sealant 2210 can cover the outer surface of the laminate 100.

[0206] For example, the first resin sealant 2210 may cover a portion of the third surface S3, a portion of the fourth surface S4, a portion of the fifth surface S5, and a portion of the sixth surface S6 of the laminate 100.

[0207] Furthermore, the first resin sealant 2210 can contact the first strip portion 303 and the second strip portion 403. That is, the first resin sealant 2210 can contact the end of the first strip portion 303 near the center of the laminate 100 in the longitudinal direction (L-axis direction). Additionally, the first resin sealant 2210 can contact the end of the second strip portion 403 near the center of the laminate 100 in the longitudinal direction (L-axis direction).

[0208] Therefore, the first resin sealant 2210 can cover the outer surface of the laminate 100 while contacting the first strip 303 and the second strip 403 respectively.

[0209] Furthermore, the thickness of the first resin seal 2210 may be less than the thickness of the first strip 303, and may be less than the thickness of the second strip 403.

[0210] Here, the thickness of the first resin seal and the thickness of the strip are measured based on scanning electron microscopy (SEM) images of a cross-section of the all-solid-state battery 2000 at a magnification of 10,000 times in the length direction (L-axis direction) and thickness direction (T-axis direction) at the central portion in the width direction (W-axis direction) of the cross-section. The thickness of the first resin seal can be the maximum value of the length of the line segment parallel to the thickness direction (T-axis direction) and connecting the laminate between the first and second strips, as shown in the aforementioned cross-sectional image, and the length of the outer surface of the first resin seal. The thickness of the strip can be the maximum value of the thicknesses of the strips shown in the aforementioned cross-sectional image.

[0211] Other material properties of the first resin sealant 2210 not described above can be referred to in [reference needed]. Figure 1 Other material properties of the first resin seal 1210 described in the embodiment shown in Figure 5, and other material properties of the second resin seal 2220 not described above, can be referred to in the following text. Figure 1 Other material properties of the second resin seal 1220 described in the embodiment shown in Figure 5.

[0212] Other components besides the components mentioned above and Figure 1 The other components of the all-solid-state battery shown are the same, so redundant descriptions will be omitted.

[0213] Figure 7 This is a schematic cross-sectional view showing an all-solid-state battery according to yet another embodiment.

[0214] Reference Figure 7The all-solid-state battery 3000 includes an all-solid-state battery element 1100 and a resin seal 3200.

[0215] The resin seal 3200 can partially cover the all-solid-state battery element 1100. The resin seal 3200 can expose a portion of the first external electrode 300 and a portion of the second external electrode 400 of the all-solid-state battery element 1100.

[0216] The resin seal 3200 may include a first resin seal 3210, a second resin seal 3220 and a third resin seal 3230.

[0217] The elastic modulus of the first resin sealant 3210 may be greater than that of the second resin sealant 3220. Furthermore, the elastic modulus of the third resin sealant 3230 may be greater than that of the second resin sealant 3220. In other words, the first resin sealant 3210 and the third resin sealant 3230 may be made of materials harder than the second resin sealant 3220. The first resin sealant 3210 and the third resin sealant 3230 may be made of the same material, but this embodiment is not limited to this.

[0218] The first resin sealant 3210 can cover the outer surface of the laminate 100.

[0219] For example, the first resin sealant 3210 may cover a portion of the third surface S3, a portion of the fourth surface S4, a portion of the fifth surface S5, and a portion of the sixth surface S6 of the laminate 100.

[0220] Furthermore, the first resin sealant 3210 can contact the first tape portion 303 and the second tape portion 403. That is, the first resin sealant 3210 can contact the end of the first tape portion 303 near the center of the laminate 100 in the longitudinal direction (L-axis direction). Additionally, the first resin sealant 3210 can contact the end of the second tape portion 403 near the center of the laminate 100 in the longitudinal direction (L-axis direction).

[0221] Therefore, the first resin seal 3210 can cover the outer surface of the laminate 100 while contacting the first strip 303 and the second strip 403 respectively.

[0222] In addition, the thickness of the first resin seal 3210 may be less than the thickness of the first strip 303, and the thickness of the first resin seal 3210 may be less than the thickness of the second strip 403.

[0223] Here, the thickness of the first resin seal and the thickness of the strip are measured based on scanning electron microscopy (SEM) images of a cross-section of the all-solid-state battery 3000 at 10,000x magnification, taken at the central portion in the width direction (W-axis direction) and in the length direction (L-axis direction) and thickness direction (T-axis direction). The thickness of the first resin seal can be the maximum value of the length of the line segment parallel to the thickness direction (T-axis direction) and connecting the laminate between the first and second strips, as shown in the aforementioned cross-sectional image, and the length of the outer surface of the first resin seal. The thickness of the strip can be the maximum value of the thicknesses of the strips shown in the aforementioned cross-sectional image.

[0224] The second resin seal 3220 may cover the first resin seal 3210. The second resin seal 3220 may be made of a material that is softer than the first resin seal 3210.

[0225] Additionally, the second resin seal 3220 may cover a portion of the first strip 303 and a portion of the second strip 403.

[0226] The region from the end of the first strip portion 303 near the center of the laminate 100 in the longitudinal direction (L-axis direction) to the point spaced apart from the first edge portion 305 can be covered by the second resin sealant 3220. That is, the second resin sealant 3220 may not be provided on the first edge portion 305 of the first external electrode 300. Similarly, the region from the end of the second strip portion 403 near the center of the laminate 100 in the longitudinal direction (L-axis direction) to the point spaced apart from the second edge portion 405 can be covered by the second resin sealant 3220. That is, the second resin sealant 3220 may not be provided on the second edge portion 405 of the second external electrode 400.

[0227] The third resin seal 3230 may cover the second resin seal 3220 and may expose a portion of the first external electrode 300 and a portion of the second external electrode 400. The third resin seal 3230 may be a material harder than the second resin seal 3220.

[0228] The third resin sealant 3230 can cover the portion of the first strip 303 not covered by the second resin sealant 3220 and the portion of the second strip 403 not covered by the second resin sealant 3220. That is, the third resin sealant 3230 can cover the first strip 303 located between the first edge portion 305 and the second resin sealant 3220. Additionally, the third resin sealant 3230 can cover the second strip 403 located between the second edge portion 405 and the second resin sealant 3220. The third resin sealant 3230 may not be provided on the first edge portion 305 and the second edge portion 405.

[0229] For example, the first strip portion 303 can be divided into a portion covered by the second resin sealant 3220, a portion covered by the third resin sealant 3230, and the remaining portion. Similarly, the second strip portion 403 can be divided into a portion covered by the second resin sealant 3220, a portion covered by the third resin sealant 3230, and the remaining portion.

[0230] Other material properties of the first resin sealant 3210 and the third resin sealant 3230 not described above can be referred to in [reference]. Figure 1 Other material properties of the first resin seal 1210 described in the embodiment shown in Figure 5, and other material properties of the second resin seal 3220 not described above, can be referred to in the following text. Figure 1 Other material properties of the second resin seal 1220 described in the embodiment shown in Figure 5.

[0231] Other components besides the components mentioned above and Figure 1 The other components of the all-solid-state battery shown are the same, so redundant descriptions will be omitted.

[0232] Figure 8 This is a schematic cross-sectional view showing an all-solid-state battery according to another embodiment.

[0233] Reference Figure 8 The all-solid-state battery 4000 includes an all-solid-state battery element 1100 and a resin seal 4200.

[0234] The resin seal 4200 may partially cover the all-solid-state battery element 1100. The resin seal 4200 may expose a portion of the first external electrode 300 and a portion of the second external electrode 400 of the all-solid-state battery element 1100.

[0235] The resin seal 4200 may include a first resin seal 4210, a second resin seal 4220 and a third resin seal 4230.

[0236] The elastic modulus of the first resin sealant 4210 may be less than that of the second resin sealant 4220. Furthermore, the elastic modulus of the third resin sealant 4230 may be less than that of the second resin sealant 4220. In other words, the first resin sealant 4210 and the third resin sealant 4230 may be made of materials softer than the second resin sealant 4220. The first resin sealant 4210 and the third resin sealant 4230 may be made of the same material, but this embodiment is not limited to this.

[0237] The first resin sealant 4210 can cover the outer surface of the laminate 100.

[0238] For example, the first resin sealant 4210 may cover a portion of the third surface S3, a portion of the fourth surface S4, a portion of the fifth surface S5, and a portion of the sixth surface S6 of the laminate 100.

[0239] Furthermore, the first resin sealant 4210 can contact the first tape portion 303 and the second tape portion 403. That is, the first resin sealant 4210 can contact the end of the first tape portion 303 near the center of the laminate 100 in the longitudinal direction (L-axis direction). Additionally, the first resin sealant 4210 can contact the end of the second tape portion 403 near the center of the laminate 100 in the longitudinal direction (L-axis direction).

[0240] Therefore, the first resin seal 4210 can cover the outer surface of the laminate 100 while in contact with the first strip 303 and the second strip 403.

[0241] In addition, the thickness of the first resin seal 4210 may be less than the thickness of the first strip 303, and the thickness of the first resin seal 4210 may be less than the thickness of the second strip 403.

[0242] Here, the thickness of the first resin seal and the thickness of the strip are measured based on scanning electron microscopy (SEM) images of a cross-section of the all-solid-state battery 4000 at 10,000x magnification, taken at the central portion in the width direction (W-axis direction) and in the length direction (L-axis direction) and thickness direction (T-axis direction). The thickness of the first resin seal can be the maximum value of the length of the line segment parallel to the thickness direction (T-axis direction) and connecting the laminate between the first and second strips, as shown in the aforementioned cross-sectional image, and the length of the outer surface of the first resin seal. The thickness of the strip can be the maximum value of the thicknesses of the strips shown in the aforementioned cross-sectional image.

[0243] The second resin seal 4220 may cover the first resin seal 4210. The second resin seal 4220 may be a material that is harder than the first resin seal 4210.

[0244] Additionally, the second resin seal 4220 may cover a portion of the first strip 303 and a portion of the second strip 403.

[0245] The area from the end of the first strip portion 303 near the center of the laminate 100 in the longitudinal direction (L-axis direction) to the point spaced apart from the first edge portion 305 can be covered by the second resin sealant 4220. That is, the second resin sealant 4220 may not be provided on the first edge portion 305. Similarly, the area from the end of the second strip portion 403 near the center of the laminate 100 in the longitudinal direction (L-axis direction) to the point spaced apart from the second edge portion 405 can be covered by the second resin sealant 4220. That is, the second resin sealant 4220 may not be provided on the second edge portion 405.

[0246] The third resin seal 4230 may cover the second resin seal 4220 and may expose a portion of the first external electrode 300 and a portion of the second external electrode 400. The third resin seal 4230 may be made of a softer material than the second resin seal 4220.

[0247] The third resin sealant 4230 can cover the portion of the first strip 303 not covered by the second resin sealant 4220, as well as the portion of the second strip 403 not covered by the second resin sealant 4220. That is, the third resin sealant 4230 can cover the first strip 303 located between the first edge portion 305 and the second resin sealant 4220. Additionally, the third resin sealant 4230 can cover the second strip 403 located between the second edge portion 405 and the second resin sealant 4220. The third resin sealant 4230 may not be provided on the first edge portion 305 and the second edge portion 405.

[0248] For example, the first strip portion 303 can be divided into a portion covered by the second resin sealant 4220, a portion covered by the third resin sealant 4230, and the remaining portion. Similarly, the second strip portion 403 can be divided into a portion covered by the second resin sealant 4220, a portion covered by the third resin sealant 4230, and the remaining portion.

[0249] According to this embodiment, a first resin seal 4210, made of a material with a relatively small elastic modulus (i.e., a soft material), contacts the outer surface of the laminate 100, so that the first resin seal 4210 can expand together with the laminate 100 when the all-solid-state battery 4000 is in operation. However, a second resin seal 4220, made of a material with a relatively large elastic modulus (i.e., a hard material), covers the first resin seal 4210, thereby suppressing the expansion of the laminate 100.

[0250] Other material properties of the first resin sealant 4210 and the third resin sealant 4230 not described above can be referred to in [reference]. Figure 1Other material properties of the second resin seal 1220 described in the embodiment shown in Figure 5, and other material properties of the second resin seal 4220 not described above, can be referred to in the following text. Figure 1 Other material properties of the first resin seal 1210 described in the embodiment shown in Figure 5.

[0251] Other components besides the components mentioned above and Figure 1 The other components of the all-solid-state battery shown are the same, so redundant descriptions will be omitted.

[0252] Figure 9 This is a schematic cross-sectional view showing an all-solid-state battery according to yet another embodiment.

[0253] Reference Figure 9 The all-solid-state battery 5000 includes an all-solid-state battery element 1100, a substrate 5100, a resin sealant 5200, and a housing 5300.

[0254] The all-solid-state battery element 1100 includes a stack 100, a first external electrode 300, and a second external electrode 400.

[0255] The all-solid-state battery element 1100 can be mounted on the substrate 5100. The substrate 5100 is a circuit board, which can be a multilayer circuit board, a single-layer double-sided printed circuit board, etc., and there are no specific type restrictions.

[0256] The substrate 5100 may include a first electrode pad 5110 and a second electrode pad 5120.

[0257] The first electrode pad 5110 may be electrically connected to the first external electrode 300 of the all-solid-state battery element 1100. For example, the first external electrode 300 may be electrically connected to the first electrode pad 5110 via a first conductive bonding member 5130. For example, the first conductive bonding member may include solder.

[0258] The second electrode pad 5120 may be electrically connected to the second external electrode 400 of the all-solid-state battery element 1100. For example, the second external electrode 400 may be electrically connected to the second electrode pad 5120 via a second conductive bonding member 5140. For example, the second conductive bonding member may include solder.

[0259] The resin seal 5200 may include a first resin seal 5210 and a second resin seal 5220.

[0260] The elastic modulus of the first resin sealant 5210 can be greater than that of the second resin sealant 5220. In other words, the first resin sealant 5210 can be made of a material that is harder than the second resin sealant 5220.

[0261] The first resin sealant 5210 may cover at least a portion of the all-solid-state battery element 1100 and may contact the substrate 5100.

[0262] For example, the first resin sealant 5210 may cover the entire all-solid-state battery 1100 except for the area between the all-solid-state battery 1100 and the substrate 5100 occupied by the first electrode pad 5110, the second electrode pad 5120, the first conductive bonding member 5130 and the second conductive bonding member 5140.

[0263] The second resin sealant 5220 may cover the first resin sealant 5210 and may contact the substrate 5100. The second resin sealant 5220 may be made of a material that is softer than the first resin sealant 5210.

[0264] The outer casing 5300 can cover the second resin seal 5220 and can contact the substrate 5100.

[0265] The housing 5300 may be made of metal or alloy. For example, the housing 5300 may include aluminum, aluminum alloy, steel, stainless steel, or a combination thereof.

[0266] The outer casing 5300 can be made by processing a plate or by joining plates, but this embodiment is not limited to this.

[0267] Other material properties of the first resin sealant 5210 not described above can be referred to in [reference]. Figure 1 Other material properties of the first resin sealant 1210 described in the embodiment shown in Figure 5, and other material properties of the second resin sealant 5220 not described above, can be referred to in the following text. Figure 1 Other material properties of the second resin seal 1220 described in the embodiment shown in Figure 5.

[0268] Other components besides the components mentioned above and Figure 1 The other components of the all-solid-state battery shown are the same, so redundant descriptions will be omitted.

[0269] Figure 10 This is a schematic cross-sectional view showing an all-solid-state battery according to another embodiment.

[0270] Reference Figure 10 The all-solid-state battery 6000 includes an all-solid-state battery element 1100, a substrate 5100, a resin sealant 6200, and a housing 6300.

[0271] The all-solid-state battery element 1100 includes a stack 100, a first external electrode 300, and a second external electrode 400.

[0272] The all-solid-state battery element 1100 can be mounted on the substrate 5100.

[0273] The substrate 5100 may include a first electrode pad 5110 and a second electrode pad 5120.

[0274] The first electrode pad 5110 may be electrically connected to the first external electrode 300 of the all-solid-state battery element 1100. For example, the first external electrode 300 may be electrically connected to the first electrode pad 5110 via a first conductive bonding member 5130. For example, the first conductive bonding member may include solder.

[0275] The second electrode pad 5120 may be electrically connected to the second external electrode 400 of the all-solid-state battery element 1100. For example, the second external electrode 400 may be electrically connected to the second electrode pad 5120 via a second conductive bonding member 5140. For example, the second conductive bonding member may include solder.

[0276] The resin seal 6200 may include a first resin seal 6210, a second resin seal 6220 and a third resin seal 6230.

[0277] The elastic modulus of the first resin sealant 6210 may be less than that of the second resin sealant 6220. Furthermore, the elastic modulus of the third resin sealant 6230 may be less than that of the second resin sealant 6220. In other words, the first resin sealant 6210 and the third resin sealant 6230 may be made of materials softer than the second resin sealant 6220. The first resin sealant 6210 and the third resin sealant 6230 may be made of the same material, but this embodiment is not limited to this.

[0278] The first resin sealant 6210 can cover the outer surface of the laminate 100.

[0279] For example, the first resin sealant 6210 may cover a portion of the third surface S3, a portion of the fourth surface S4, a portion of the fifth surface S5, and a portion of the sixth surface S6 of the laminate 100.

[0280] Furthermore, the first resin sealant 6210 can contact the first strip portion 303 and the second strip portion 403. That is, the first resin sealant 6210 can contact the end of the first strip portion 303 near the center of the laminate 100 in the longitudinal direction (L-axis direction). Additionally, the first resin sealant 6210 can contact the end of the second strip portion 403 near the center of the laminate 100 in the longitudinal direction (L-axis direction).

[0281] Therefore, the first resin seal 6210 can cover the outer surface of the laminate 100 while in contact with the first strip 303 and the second strip 403.

[0282] In addition, the thickness of the first resin seal 6210 may be less than the thickness of the first strip 303, and the thickness of the first resin seal 6210 may be less than the thickness of the second strip 403.

[0283] Here, the thickness of the first resin seal and the thickness of the strip are measured based on scanning electron microscopy (SEM) images at 10,000x magnification of a cross-section taken at the central portion of the all-solid-state battery 6000 along the length direction (L-axis) and thickness direction (T-axis). The thickness of the first resin seal can be the maximum value of the length of the line segment parallel to the thickness direction (T-axis) and connecting the laminate between the first and second strips, as shown in the aforementioned cross-sectional image, and the length of the outer surface of the first resin seal. The thickness of the strip can be the maximum value of the strip thicknesses shown in the aforementioned cross-sectional image.

[0284] The second resin seal 6220 may cover at least a portion of the all-solid-state battery element 1100 and the first resin seal 6210, and may be in contact with the substrate 5100. The second resin seal 6220 may be a material harder than the first resin seal 6210.

[0285] For example, the second resin seal 6220 may cover the first resin seal 6210 and the entire all-solid-state battery 1100 except for the area occupied by the first electrode pad 5110, the second electrode pad 5120, the first conductive bonding member 5130 and the second conductive bonding member 5140 between the all-solid-state battery 1100 and the first resin seal 6210 and the substrate 5100.

[0286] The third resin sealant 6230 may cover the second resin sealant 6220 and may contact the substrate 5100. The third resin sealant 6230 may be a material softer than the second resin sealant 6220.

[0287] The outer casing 6300 can cover the third resin seal 6230 and can contact the substrate 5100.

[0288] The housing 6300 may be made of metal or alloy. For example, the housing 6300 may include aluminum, aluminum alloy, steel, stainless steel, or a combination thereof.

[0289] The outer casing 6300 can be made by processing a plate or by joining plates, but this embodiment is not limited to this.

[0290] Other material properties of the first resin sealant 6210 and the third resin sealant 6230 not described above can be referred to in [reference]. Figure 1Other material properties of the second resin seal 1220 described in the embodiment shown in Figure 5, and other material properties of the second resin seal 6220 not described above, can be referred to in the following text. Figure 1 Other material properties of the first resin seal 1210 described in the embodiment shown in Figure 5.

[0291] Other components besides the components mentioned above and Figure 9 The other components of the all-solid-state battery shown are the same, so redundant descriptions will be omitted.

[0292] [Preparation Example: Fabrication of All-Solid-State Batteries] (Example) Multiple strip-shaped positive electrode layers are formed by printing positive electrode active material layer, positive electrode current collector and positive electrode active material layer in sequence on solid electrolyte layer (green sheet), and then filling the space between positive electrode layers with insulating material to form positive electrode sheet.

[0293] Multiple strip-shaped negative electrode layers are formed by printing on a solid electrolyte layer (green sheet) in the order of negative electrode active material layer, negative electrode current collector, and negative electrode active material layer, and then filling the space between the negative electrode layers with insulating material to form a negative electrode sheet.

[0294] Positive and negative electrode sheets are stacked alternately to form green sheets.

[0295] Cut the green blanks to form a laminate.

[0296] The laminate is sintered in an air or nitrogen atmosphere within the range of 400°C to 550°C. After applying conductive paste to the surface of the laminate, the laminate is successively held in a curing oven at 50°C, 80°C, and 200°C for 30 minutes each, and then cooled to form the external electrode.

[0297] Epoxy resin is applied to cover a portion of the surface of the laminate and a portion of the external electrode, and then cured.

[0298] All-solid-state batteries are prepared by coating polyimide silicone resin to cover epoxy resin and then curing it.

[0299] (Comparative example) Multiple strip-shaped positive electrode layers are formed by printing positive electrode active material layer, positive electrode current collector and positive electrode active material layer in sequence on solid electrolyte layer (green sheet), and then filling the space between positive electrode layers with insulating material to form positive electrode sheet.

[0300] Multiple strip-shaped negative electrode layers are formed by printing on a solid electrolyte layer (green sheet) in the order of negative electrode active material layer, negative electrode current collector, and negative electrode active material layer, and then filling the space between the negative electrode layers with insulating material to form a negative electrode sheet.

[0301] Positive and negative electrode sheets are stacked alternately to form green sheets.

[0302] Cut the green blanks to form a laminate.

[0303] The laminate is sintered in an air or nitrogen atmosphere at a temperature ranging from 400°C to 550°C.

[0304] An edge portion is provided on the surface of the sintered laminate.

[0305] After applying conductive paste to the surface of the laminate, the laminate was successively kept in a curing oven at 50°C, 80°C and 200°C for 30 minutes each, and then cooled to form an external electrode, thereby preparing an all-solid-state battery.

[0306] [Experimental Example: Evaluation of the Moisture Resistance Reliability of All-Solid-State Batteries] Five all-solid-state batteries, representing both example and comparative examples, were fabricated. Initial charge / discharge tests were performed on each representative sample at 25°C and 25% humidity, and the results are presented below. Figure 11 and Figure 12 In addition, initial charge / discharge tests were performed on each representative sample at 25°C and 55% humidity, and the results are presented below. Figure 13 and Figure 14 middle.

[0307] Reference Figure 11 and Figure 12 Normal discharge capacity variation was observed in both the all-solid-state battery prepared according to the example and the all-solid-state battery prepared according to the comparative example.

[0308] On the other hand, refer to Figure 13 and Figure 14 The all-solid-state battery prepared according to the example exhibited normal discharge capacity variation, while the all-solid-state battery prepared according to the comparative example showed a sharp decrease in discharge capacity. This appears to be because, under conditions where humidity increased from 25% to 55%, the all-solid-state battery prepared according to the comparative example experienced volume expansion, cracking, and moisture penetration.

[0309] While the invention has been described in conjunction with what are now considered practical embodiments, it should be understood that the invention is not limited to the disclosed embodiments. Rather, the invention is intended to cover various variations and equivalents included within the spirit and scope of the appended claims.

[0310] <Explanation of reference numerals in the attached figures> 1000: All-solid-state battery 1100: All-solid-state battery element 1200: Resin sealant 1210: First resin sealant 1220: Second resin sealant 100: Layered body 110: Solid electrolyte layer 130: Positive electrode layer 133: Positive current collector 135, 136: Positive electrode active material layer 150: Negative electrode layer 153: Negative current collector 155, 156: Negative electrode active material layer 160: Upper protective layer 170: Lower protective layer 180: Edge 300: First external electrode 400: Second external electrode 5100: Substrate 5110: First electrode pad 5120: Second electrode pad 5130: First conductive bonding member 5140: Second conductive bonding member 5300: Outer shell.

Claims

1. An all-solid-state battery comprising: an all-solid-state battery element including a laminate, a first external electrode, and a second external electrode, the laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers, and a plurality of negative electrode layers stacked in a first direction, the first external electrode provided outside the laminate and connected to the plurality of positive electrode layers, the second external electrode provided outside the laminate and connected to the plurality of negative electrode layers; and a resin sealing body covering the all-solid-state battery element and exposing a portion of the first external electrode and a portion of the second external electrode, wherein the resin sealing body includes a first resin sealing body and a second resin sealing body, and wherein an elastic modulus of the first resin sealing body is different from an elastic modulus of the second resin sealing body.

2. The all-solid-state battery according to claim 1, the resin sealing body exposing an end surface of the first external electrode in a second direction and an end surface of the second external electrode in the second direction, and wherein wherein the second direction intersects the first direction.

3. The all-solid-state battery according to claim 1, the first resin sealing body covering an outer surface of the laminate, and wherein, wherein the second resin sealing body covers at least a portion of the first resin sealing body, at least a portion of a remaining portion of the first external electrode other than the portion, and at least a portion of a remaining portion of the second external electrode other than the portion.

4. The all-solid-state battery according to claim 3, the first external electrode including a first band portion provided on an outer surface of the laminate in the first direction, wherein wherein the second external electrode includes a second band portion provided on the outer surface of the laminate in the first direction, and wherein both ends of the first resin sealing body in a second direction are in contact with the first band portion and the second band portion, respectively.

5. The all-solid-state battery according to claim 4, a thickness of the first resin sealing body is smaller than a thickness of the first band portion and a thickness of the second band portion. wherein 6. The all-solid-state battery according to claim 3, the first external electrode including a first band portion provided on an outer surface of the laminate in the first direction, wherein wherein the second external electrode includes a second band portion arranged on the outer surface of the laminate in the first direction, wherein the first resin sealing body covers a portion of the first band portion and a portion of the second band portion, and wherein the second resin sealing body covers a remaining portion of the first band portion and a remaining portion of the second band portion.

7. The all-solid-state battery according to claim 6, a thickness of the first resin sealing body is greater than a thickness of the first band portion and greater than a thickness of the second band portion. wherein, 8. The all-solid-state battery according to claim 1, an elastic modulus of the first resin sealing body is greater than an elastic modulus of the second resin sealing body, and the second resin sealing body covers the first resin sealing body. wherein, 9. The all-solid-state battery according to claim 1, ​ wherein The first resin seal has an elastic modulus that is less than an elastic modulus of the second resin seal, and the second resin seal covers the first resin seal.

10. The all-solid-state battery according to claim 1, wherein The first resin seal includes a phenol epoxy resin, a phenol resin, a novolak epoxy resin, an o-cresol resin, an acrylic resin, or a combination thereof.

11. The all-solid-state battery according to claim 1, wherein The second resin seal includes a polyimide resin, a polyimide silicone resin, a silicone resin, a polyamide resin, a rubber, a polyurethane resin, or a combination thereof.

12. An all-solid-state battery comprising: an all-solid-state battery element including a laminate, a first external electrode, and a second external electrode, the laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers, and a plurality of negative electrode layers stacked in a first direction, the first external electrode disposed outside the laminate and connected to the plurality of positive electrode layers, the second external electrode disposed outside the laminate and connected to the plurality of negative electrode layers; and a resin seal covering the all-solid-state battery element and exposing a portion of the first external electrode and a portion of the second external electrode, wherein the resin seal includes a first resin seal, a second resin seal, and a third resin seal stacked in the first direction.

13. The all-solid-state battery according to claim 12, wherein the first resin seal has an elastic modulus that is greater than an elastic modulus of the second resin seal, and wherein the third resin seal has an elastic modulus that is greater than an elastic modulus of the second resin seal.

14. The all-solid-state battery according to claim 13, wherein the first external electrode includes a first tab portion disposed on an outer surface of the laminate in the first direction, wherein the second external electrode includes a second tab portion arranged on the outer surface of the laminate in the first direction, wherein the first resin seal covers the outer surface of the laminate and is in contact with the first tab portion and the second tab portion, wherein the second resin seal covers the first resin seal and is in contact with the first tab portion and the second tab portion, wherein the third resin seal covers the second resin seal and exposes an end surface of the first external electrode in a second direction and an end surface of the second external electrode in the second direction, and wherein the second direction intersects the first direction.

15. The all-solid-state battery according to claim 14, wherein the first resin seal is disposed between the first tab portion and the second tab portion, and wherein a thickness of the first resin seal is less than a thickness of the first tab portion and less than a thickness of the second tab portion.

16. The all-solid-state battery according to claim 12, wherein the first resin seal has an elastic modulus that is less than an elastic modulus of the second resin seal, and wherein the third resin seal has an elastic modulus that is less than an elastic modulus of the second resin seal.

17. The all-solid-state battery according to claim 16, wherein, the first outer electrode includes a first strip portion provided on an outer surface of the laminate in the first direction, the second outer electrode includes a second strip portion arranged on the outer surface of the laminate in the first direction, the first resin seal covers the outer surface of the laminate and is in contact with the first strip portion and the second strip portion, the second resin seal covers the first resin seal and is in contact with the first strip portion and the second strip portion, the third resin seal covers the second resin seal and exposes an end surface of the first outer electrode in a second direction and an end surface of the second outer electrode in the second direction, and the second direction intersects the first direction.

18. The all-solid-state battery according to claim 17, wherein, the first resin seal is provided between the first strip portion and the second strip portion, and a thickness of the first resin seal is smaller than a thickness of the first strip portion and smaller than a thickness of the second strip portion.

19. An all-solid-state battery comprising: an all-solid-state battery element including a laminate, a first outer electrode, and a second outer electrode, the laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers, and a plurality of negative electrode layers stacked in a first direction, the first outer electrode provided outside the laminate and connected to the plurality of positive electrode layers, the second outer electrode provided outside the laminate and connected to the plurality of negative electrode layers; a substrate including a first electrode pad connected to the first outer electrode of the all-solid-state battery element and a second electrode pad connected to the second outer electrode of the all-solid-state battery element; a resin seal covering the all-solid-state battery element and in contact with the substrate; and an outer housing covering the resin seal, the resin seal includes a first resin seal and a second resin seal, and the first resin seal covers at least a portion of the all-solid-state battery element, the second resin seal covers the first resin seal and is in contact with the substrate, and an elastic modulus of the first resin seal is different from an elastic modulus of the second resin seal.

20. The all-solid-state battery according to claim 19, wherein, the elastic modulus of the first resin seal is greater than the elastic modulus of the second resin seal.

21. The all-solid-state battery according to claim 19, wherein, the elastic modulus of the first resin seal is smaller than the elastic modulus of the second resin seal.

22. The all-solid-state battery according to claim 21, wherein, the resin seal further includes a third resin seal covering the second resin seal and in contact with the substrate, and an elastic modulus of the third resin seal is smaller than the elastic modulus of the second resin seal.

23. The all-solid-state battery according to claim 22, wherein the first resin seal covers an outer surface of the laminate, the first outer electrode includes a first strip portion provided on an outer surface of the laminate in the first direction, wherein the second external electrode includes a second strip portion arranged on the outer surface of the laminate in the first direction, and wherein a thickness of the first resin seal is smaller than a thickness of the first strip portion and a thickness of the second strip portion.

24. The all-solid-state battery of claim 19, wherein the outer shell includes a metal or an alloy.

25. The all-solid-state battery of claim 24, wherein the outer shell includes aluminum (Al), an aluminum (Al) alloy, steel, stainless steel, or a combination thereof.

26. An all-solid-state battery, comprising: an all-solid-state battery element including a laminate, a first external electrode, and a second external electrode, the laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers, and a plurality of negative electrode layers stacked in a first direction, the first external electrode disposed outside the laminate and connected to the plurality of positive electrode layers, the second external electrode disposed outside the laminate and connected to the plurality of negative electrode layers; and a resin seal extending between the first external electrode and the second external electrode and covering a portion of the first external electrode and a portion of the second external electrode, wherein the resin seal includes a plurality of layers and is spaced apart from the plurality of positive electrode layers and the plurality of negative electrode layers.

27. The all-solid-state battery of claim 26, wherein the laminate includes a plurality of surfaces, wherein the first external electrode is disposed on a first surface among the plurality of surfaces to be connected to the plurality of positive electrode layers, and the second external electrode is disposed on a second surface among the plurality of surfaces to be connected to the plurality of negative electrode layers, wherein the first surface is opposite the second surface, and wherein, among the plurality of surfaces, the resin seal covers surfaces other than the first surface and the second surface.

28. The all-solid-state battery of claim 26, wherein at least two layers of the plurality of layers of the resin seal include different materials.

29. The all-solid-state battery of claim 28, wherein, the at least two layers of the plurality of layers of the resin seal have different elastic moduli.

30. The all-solid-state battery of claim 26, wherein, an elastic modulus of one layer of the plurality of layers of the resin seal is greater than an elastic modulus of another layer of the plurality of layers of the resin seal that covers the one layer of the plurality of layers of the resin seal.

31. The all-solid-state battery of claim 30, wherein, the elastic modulus of the one layer of the plurality of layers of the resin seal is greater than or equal to 100 MPa, and the elastic modulus of the another layer of the plurality of layers of the resin seal is less than or equal to 0.15 MPa.

32. The all-solid-state battery of claim 26, wherein, at least two layers of the plurality of layers of the resin seal are in contact with the first external electrode and the second external electrode.

33. An all-solid-state battery, comprising: A full solid battery element including a laminate, a first external electrode, and a second external electrode, the laminate including a plurality of solid electrolyte layers, a plurality of positive electrode layers, and a plurality of negative electrode layers stacked in a first direction, the first external electrode provided outside the laminate and connected to the plurality of positive electrode layers, the second external electrode provided outside the laminate and connected to the plurality of negative electrode layers; a substrate including a first electrode pad connected to the first external electrode of the full solid battery element and a second electrode pad connected to the second external electrode of the full solid battery element; a first resin sealing body covering the full solid battery element and provided between the full solid battery element and the substrate to be in contact with the substrate; a second resin sealing body covering the first resin sealing body and in contact with the substrate; and a housing body covering the second resin sealing body.

34. The full solid battery according to claim 33, an elastic modulus of the first resin sealing body is different from an elastic modulus of the second resin sealing body. wherein 35. The full solid battery according to claim 34, an elastic modulus of the first resin sealing body is greater than an elastic modulus of the second resin sealing body. wherein 36. The full solid battery according to claim 33, the first resin sealing body covers and is in contact with the first external electrode and the second external electrode. wherein, 37. The full solid battery according to claim 36, the second resin sealing body is spaced apart from the first external electrode and the second external electrode. wherein 38. The full solid battery according to claim 33, the second resin sealing body is spaced apart from the laminate. wherein 39. The full solid battery according to claim 33, on the substrate, the first resin sealing body is provided between the first electrode pad and the second electrode pad, and the second resin sealing body is provided in a region outside the first electrode pad and the second electrode pad. wherein ​

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