Device for manufacturing all-solid-state battery, and method for manufacturing all-solid-state battery using same

Abstract

The present invention relates to a device and method for manufacturing an all-solid-state battery, and an all-solid-state battery manufactured using same. More specifically, the device for manufacturing an all-solid-state battery comprises: an electrode supply unit including a first supply roll around which a first electrode is wound and a second supply roll around which a second electrode is wound, the second electrode comprising a plurality of second electrode tabs; a pressing unit for laminating the first electrode, which travels in a first direction, and the second electrode, which travels in the first direction, together to form an electrode laminate; and a notching unit for notching a first side of the first electrode to form a plurality of first electrode tabs.

Description

All-solid-state battery manufacturing device and all-solid-state battery manufacturing method using the same

[0001] The recent rapid proliferation of battery-powered electronic devices, such as mobile phones, laptops, and electric vehicles, has led to a rapid increase in demand for high-energy density, high-capacity secondary batteries. Accordingly, active research and development is underway to improve the performance of lithium secondary batteries.

[0002] A lithium secondary battery is a battery that includes a positive electrode and a negative electrode that contain active materials capable of intercalating and deintercalating lithium ions, and an electrolyte, and produces electrical energy through oxidation and reduction reactions when lithium ions are intercalated / deintercalated from the positive electrode and negative electrode.

[0003] The problem to be solved by the present invention is to provide a device for manufacturing an all-solid-state battery cut to a predetermined size from roll-type electrodes.

[0004] Another problem to be solved by the present invention is to provide a method for manufacturing an all-solid-state battery cut to a predetermined size from roll-type electrodes.

[0005]

[0006] The problem to be solved by the present invention is to provide a device for manufacturing an all-solid-state battery cut to a predetermined size from roll-type electrodes.

[0007] Another problem to be solved by the present invention is to provide a method for manufacturing an all-solid-state battery cut to a predetermined size from roll-type electrodes.

[0008] An all-solid-state battery manufacturing device according to the concept of the present invention may include an electrode supply unit including a first supply roll on which a first electrode is wound and a second supply roll on which a second electrode is wound, the second electrode including a plurality of second electrode tabs; a pressing unit configured to laminate the first electrode traveling in a first direction and the second electrode traveling in the first direction to each other to form an electrode laminate; and a notching unit configured to notch a first side of the first electrode to form a plurality of first electrode tabs. The notching unit may include: a sensing unit configured to measure positions or intervals of the plurality of second electrode tabs; and a tab forming unit configured to notch the first electrode based on the positions or the intervals.

[0009] A method for manufacturing an all-solid-state battery according to another concept of the present invention may include an electrode supply process for unwinding wound first and second electrodes and causing them to travel in a first direction, the second electrode including a plurality of second electrode tabs protruding in the second direction; a pressing process for laminating the first electrode traveling in the first direction and the second electrode traveling in the first direction to each other to form an electrode laminate; and a notching process for notching the first electrode of the electrode laminate to form a plurality of first electrode tabs. The notching process may include: measuring positions or intervals between the plurality of second electrode tabs; and notching a first side of the first electrode based on the positions or intervals.

[0010] According to another concept of the present invention, an all-solid-state battery includes a first electrode sheet and a second electrode sheet laminated on the first electrode sheet, wherein a length of the first electrode sheet in a first direction is substantially the same as a length of the second electrode sheet in the first direction, and a width of the first electrode sheet in a second direction may be greater than a width of the second electrode sheet in the second direction. The first electrode sheet may include a first electrode tab protruding in the second direction, and the second electrode sheet may include a second electrode tab protruding in a direction opposite to the second direction. The first electrode tab may not overlap the second electrode sheet, and a portion of the second electrode tab may vertically overlap the first electrode sheet.

[0011]

[0012] By utilizing the all-solid-state battery manufacturing apparatus and method of the present invention, all-solid-state unit cells cut to a predetermined size can be manufactured through a series of continuous processes without equipment interruption. Furthermore, the all-solid-state battery manufacturing method of the present invention utilizes a roll-type electrode sheet, enabling the process to be performed without separate driving auxiliary materials.

[0013] FIG. 1 is a cross-sectional view of an all-solid-state battery manufacturing device according to embodiments of the present invention.

[0014] Fig. 2a is a schematic diagram illustrating a notching unit according to one embodiment of the present invention. Fig. 2b is a conceptual diagram illustrating an operating principle of a notching unit according to one embodiment of the present invention to form a first electrode tab on a first electrode sheet.

[0015] Figure 3 is a flowchart for explaining a method for manufacturing an all-solid-state battery according to embodiments of the present invention.

[0016] Figures 4 to 9 are conceptual diagrams for explaining a method for manufacturing an all-solid-state battery according to embodiments of the present invention.

[0017] Figure 10 is a plan view of an all-solid-state battery according to one embodiment of the present invention.

[0018] Fig. 11 is a cross-sectional view taken along line AA' of the all-solid-state battery of Fig. 10.

[0019] Fig. 12 is a BB' cross-sectional view of the all-solid-state battery of Fig. 10.

[0020] Figure 13 is a cross-sectional view of an all-solid-state battery according to another embodiment.

[0021]

[0022]

[0023] To fully understand the structure and effects of the present invention, preferred embodiments of the present invention will be described with reference to the accompanying drawings. However, the present invention is not limited to the embodiments disclosed below, but can be implemented in various forms and subject to various modifications. However, the description of these embodiments is provided solely to ensure a complete disclosure of the present invention and to fully inform those skilled in the art of the invention of the scope of the invention.

[0024] In this specification, when a component is referred to as being on another component, it means that it can be formed directly on the other component, or a third component may be interposed between them. Furthermore, in the drawings, the thicknesses of the components are exaggerated for the sake of clarity. Parts designated by the same reference numerals throughout the specification represent the same components.

[0025] Embodiments described herein will be described with reference to cross-sectional and / or plan views, which are ideal illustrations of the present invention. In the drawings, the thicknesses of films and regions are exaggerated for the purpose of effectively explaining the technical contents. Accordingly, the regions illustrated in the drawings have a schematic nature, and the shapes of the regions illustrated in the drawings are intended to illustrate specific shapes of regions of the device and are not intended to limit the scope of the invention. Although terms such as first, second, and third are used to describe various components in various embodiments of the present specification, these components should not be limited by such terms. These terms are used only to distinguish one component from another. The embodiments described and illustrated herein also include complementary embodiments thereof.

[0026] The terminology used herein is for the purpose of describing embodiments and is not intended to limit the present invention. In this specification, the singular also includes the plural unless specifically stated otherwise. As used herein, the words "comprises" and / or "comprising" do not exclude the presence or addition of one or more other components.

[0027]

[0028] All-solid-state battery manufacturing device (10)

[0029] FIG. 1 is a cross-sectional view illustrating an all-solid-state battery manufacturing device according to embodiments of the present invention. Referring to FIG. 1, the all-solid-state battery manufacturing device (10) may include an electrode supply unit (ECU); a gasket supply unit (GCU); a pressurizing unit (PRU); a notching unit (NOU); and a cutting unit (CTU).

[0030] An electrode supply unit (ECU) may be configured to supply a first electrode (ELT1) and a second electrode (ELT2). Each of the first electrode (ELT1) and the second electrode (ELT2) may be a wound roll type electrode.

[0031] In one embodiment, the electrode supply unit (ECU) may include a first supply roll (ESR1) on which a first electrode (ELT1) is wound and a second supply roll (ESR2) on which a second electrode (ELT2) is wound. The first electrode (ELT1) may be unwound on the first supply roll (ESR1). The second electrode (ELT2) may be unwound on the second supply roll (ESR2). The second electrode (ELT2) to be unwound may be provided on the first electrode (ELT1) to be unwound.

[0032] In one embodiment, the first electrode (ELT1) may include a cathode layer (200) and a cathode solid electrolyte layer (320) on the cathode layer (200). An adhesion enhancing layer may further be included between the cathode layer (200) and the cathode solid electrolyte layer (320). The second electrode (ELT2) may include a cathode layer (100) and a cathode solid electrolyte layer (310) on the cathode layer (100). An adhesion enhancing layer may further be included between the cathode layer (100) and the cathode solid electrolyte layer (310).

[0033] The electrode supply unit (ECU) may further include a plurality of first guide rollers (GUR1). The plurality of first guide rollers (GUR1) may adjust the driving directions of the first electrode (ELT1) and the second electrode (ELT2). The plurality of first guide rollers (GUR1) may adjust a driving path so that the first electrode (ELT1) unwound from the first supply roll (ESR1) travels in the first direction (D1). In addition, the plurality of first guide rollers (GUR1) may adjust a driving path so that the second electrode (ELT2) unwound from the second supply roll (ESR2) travels in the first direction (D1).

[0034] Although not shown, in one embodiment, the electrode supply unit (ECU) may further include a skew correction unit. The skew correction unit may be configured to correct skew of the first electrode (ELT1) and the second electrode (ELT2). As an example, the skew correction unit may include a sensor for detecting skew of the object; and an adjustment roller for adjusting the driving path of the object. The skew correction unit may further include a servo motor to precisely adjust the driving path of the object.

[0035] Referring back to FIG. 1, the gasket supply unit (GCU) may be configured to supply a first gasket (GSK1) and a second gasket (GSK2). The first gasket (GSK1) and the second gasket (GSK2) may each be a wound roll type gasket.

[0036] In one embodiment, the gasket supply unit (GCU) may include a first gasket roll (GSR1) having a first gasket (GSK1) wound around it and a second gasket roll (GSR2) having a second gasket (GSK2) wound around it. The first gasket (GSK1) may be unwound on the first gasket roll (GSR1). The second gasket (GSK2) may be unwound on the second gasket roll (GSR2). The unwound first gasket (GSK1) and second gasket (GSK2) may be provided on a first electrode (ELT1).

[0037] The first gasket (GSK1) and the second gasket (GSK2) may be spaced apart from each other in the second direction (D2) of the first electrode (ELT1). The second electrode (ELT2) may be placed between the first gasket (GSK1) and the second gasket (GSK2). The first gasket (GSK1) and the second gasket (GSK2) may prevent damage caused by a step difference between the first electrode (ELT1) and the second electrode (ELT2) during the pressurizing process.

[0038] In one embodiment, the thickness of the second gasket (GSK2) in the third direction (D3) may be smaller than the thickness of the first gasket (GSK1) in the third direction (D3). The thickness of the second gasket (GSK2) in the third direction (D3) may be smaller than the thickness of the second electrode sheet (ELS2) in the third direction (D3).

[0039] The gasket supply unit (GCU) may further include a plurality of second guide rollers (GUR2). The plurality of second guide rollers (GUR2) may adjust the running directions of the first gasket (GSK1) and the second gasket (GSK2). The plurality of second guide rollers (GUR2) may adjust the running path so that the first gasket (GSK1) unwound from the first gasket roll (GSR1) runs in the first direction (D1). In addition, the plurality of second guide rollers (GUR2) may adjust the running path so that the second gasket (GSK2) unwound from the second gasket roll (GSR2) runs in the first direction (D1).

[0040] Although not shown, in one embodiment, the gasket supply unit (GSU) may further include a skew correction unit. The skew correction unit may be configured to correct skew of the first gasket (GSK1) and the second gasket (GSK2).

[0041] Referring back to FIG. 1, the all-solid-state battery manufacturing device (10) may further include a first feeding unit (FDU1) configured to transfer the object to the pressurizing unit (PRU). In one embodiment, the first feeding unit (FDU1) may include a feeding belt or a feeding roll. The first feeding unit (FDU) may be driven by a power source to contribute to unwinding of the first and second electrodes (ELT1, ELT2) from the first and second supply rolls (ESR1, ESR2). The first feeding unit (FDU) may be driven by a power source to contribute to unwinding of the first and second gaskets (GSK1, GSK2) from the first and second gasket rolls (GSR1, GSR2).

[0042] The pressurizing unit (PRU) may be configured to laminate an object. For example, the pressurizing unit (PRU) may include a pressurizing roller (PRR). In one embodiment, the pressurizing unit (PRU) may form an electrode stack (ETS) by laminating a first electrode (ELT1) traveling in a first direction (D1) and a second electrode (ELT2) traveling in the first direction (D1) to each other.

[0043] In one embodiment, the pressurization unit (PRU) may further include a heater configured to heat the object. Through this, the pressurization unit (PRU) may heat and pressurize the object.

[0044] The notching unit (NOU) can be configured to notch the first side (ENR1) of the first electrode (ELT1) in the second direction (D2). For example, the notching unit (NOU) can form a plurality of first electrode tabs (TAR1) spaced apart in the first direction (D1) by notching the first side (ENR1) of the first electrode (ELT1).

[0045] Fig. 2a is a schematic diagram illustrating a notching unit according to one embodiment of the present invention. Fig. 2b is a conceptual diagram illustrating an operating principle of a notching unit according to one embodiment of the present invention to form a first electrode tab on a first electrode sheet.

[0046] Referring to FIG. 2A, in one embodiment, the notching unit (NOU) may include a sensing unit (ADU) and a tab forming unit (CUU). The notching unit (NOU) may further include a control unit (CTU).

[0047] Referring to FIG. 2B, the sensing unit (ADU) can recognize notched reference points within the detection area (SR) and measure the positions of the reference points or the spacing between the reference points. In one embodiment, the sensing unit (ADU) can include a vision sensor, an ultrasonic sensor, an infrared sensor, a laser sensor, or a combination thereof.

[0048] In one embodiment, the second electrode tabs (TAR2) of the second electrode sheet (ETS2) described below may be reference points detected or measured by the sensing unit (ADU). For example, the sensing unit (ADU) may be configured to detect and measure the position of the second electrode tabs (TAR2) of the second electrode (ELT2) or the gap between adjacent second electrode tabs (TAR2).

[0049] The control unit (CTU) may be configured to control the tab forming unit (CUU). Specifically, the control unit (CTU) may control the tab forming unit (CUU) to notch a notching region (NR). The notching region (NR) may be selected based on position and spacing information of the reference points measured by the sensing unit (ADU). For example, the notching region (NR) may be selected so as to have the same spacing as the second electrode tabs (TAR2) formed on the second electrode (ELT2).

[0050] The tab forming unit (CUU) may be configured to cut a selected notching region (NR). In one embodiment, the tab forming unit (CUU) may be a laser or a die cutting machine. For example, the tab forming unit (CUU) may form a plurality of first electrode tabs (TAR1) by cutting a portion of the first side (ENR1) of the first electrode (ELT1).

[0051] The electrode stack (ETS) having the first electrode tabs (TAR1) formed thereon can travel in the first direction (D1).

[0052] The cutting unit (CTU) may be configured to cut the electrode stack (ETS) extending in the first direction (D1) in the second direction (D2). For example, by cutting the electrode stack (ETS) extending in the first direction (D1) at predetermined intervals, an all-solid-state battery may be manufactured. Specifically, an all-solid-state unit cell (UCL) may be manufactured. Hereinafter, in the present specification, the term "unit cell (UCL)" is used with the same meaning as "the above-described all-solid-state unit cell (UCL)."

[0053] The all-solid-state battery manufacturing device (10) may further include a cell transfer unit (TRU) and a magazine unit (MAU).

[0054] A plurality of all-solid-state batteries may be loaded into a magazine unit (MAU). In one embodiment, a plurality of unit cells (UCL) may be loaded into the magazine unit (MAU).

[0055] A cell transfer unit (TRU) may be configured to transfer unit cells (UCL) from a cutting unit (CTU) to a magazine unit (MAU). For example, the cell transfer unit (CTU) may include a second feeding unit (FDU2), a transfer belt, and an adsorption belt.

[0056] The second feeding unit (FDU2) may include a feeding belt or a feeding roll. The second feeding unit (FDU2) may transfer the cut unit cells (UCL) onto a conveying belt. The conveying belt may transfer the unit cells (UCL) in a first direction (D1). A suction belt may be positioned above the conveying belt. The suction belt may suction the unit cells (UCL) on the conveying belt and transfer them onto a magazine unit (MAU).

[0057] The all-solid-state battery manufacturing device (10) may further include a side coating unit (SCU).

[0058] In one embodiment, the side coating unit (SCU) may be configured to coat a protective layer on both sides of the unit cell (UCL). Specifically, the side coating unit (SCU) may be configured to coat a protective layer on both sides of the unit cell (UCL) in the longitudinal direction. The longitudinal direction of the unit cell (UCL) may correspond to the first direction (D1). Accordingly, a protective layer may be coated on two sides of the unit cell (UCL) on which the first and second electrode tabs (TAR1, TAR2) are not formed among the four sides.

[0059] In one embodiment, the side coating unit (SCU) may include a sprayer capable of spraying a coating composition onto both sides of the unit cell (UCL). The side coating unit (SCU) may further include a curing unit capable of curing the sprayed coating composition. For example, the curing unit may be, but is not limited to, an IR heater or a UV lamp.

[0060] In one embodiment, the side coating unit (SDU) may be located on the cell transport unit (RTU).

[0061]

[0062] All-solid-state battery manufacturing method (S10)

[0063] Figure 3 is a flowchart illustrating a method for manufacturing an all-solid-state battery according to embodiments of the present invention. Figures 4 to 9 are conceptual diagrams illustrating a method for manufacturing an all-solid-state battery according to embodiments of the present invention.

[0064] Referring to FIG. 3, the all-solid-state battery manufacturing method (S10) may include an electrode supply process (S100); a pressurizing process (S200); a notching process (S300); a cutting process (S400); and a side coating process (S500).

[0065] The electrode supply process (S100) may include unwinding a wound first electrode (ELT1) and causing it to travel in a first direction; unwinding a wound second electrode (ELT2) and causing it to travel in the first direction; and positioning the second electrode (ELT2) on the first electrode (ELT1).

[0066] In one embodiment, the first electrode (ELT1) may be wound on the first supply roll (ESR1) described with reference to FIG. 1. The second electrode (ELT2) may be wound on the second supply roll (ESR2) described with reference to FIG. 1. As an example, the electrode supply process (S100) may be performed by the electrode supply unit (ECU) described with reference to FIG. 1.

[0067] In one embodiment, the electrode supply process (S100) may include unwinding each of the wound first gasket (GSK1) and second gasket (GSK2) and running them in a first direction (D1); and positioning each of the first gasket (GSK1) and the second gasket (GSK2) on a first electrode sheet (ELS1). The first gasket (GSK1) and the second gasket (GSK2) may be spaced apart from each other in a second direction (D2). The second direction (D2) may intersect the first direction (D1). Each of the first gasket (GSK1) and the second gasket (GSK2) may be positioned so as not to overlap a first side (ENR1) of a first electrode (ELT1) described below.

[0068] Referring to FIGS. 3 and 4, a first electrode (ELT1) running in a first direction (D1) may include a first side (ENR1). The first side (ENR1) may then be notched to form a plurality of first electrode tabs (TAR1).

[0069] Referring to FIGS. 3 and 6, a second electrode (ELT2) may be provided on a first electrode (ELT1) traveling in a first direction (D2).

[0070] In one embodiment, the width of the first electrode (ELT1) in the second direction (D2) may be greater than the width of the second electrode (ELT2) in the second direction (D2). A first gasket (GSK1) and a second gasket (GSK2) may be provided on a portion of the upper surface of the first electrode (ELT2) where the second electrode (ELT2) is not present. For example, a portion of the second electrode (ELT2) excluding the second electrode tabs (TAR2) may be provided between the first gasket (GSK1) and the second gasket (GSK2).

[0071] The first gasket (GSK1) and the second gasket (GSK2) can prevent damage caused by the step between the first electrode (ELT1) and the second electrode (ELT2) during the pressurizing process (S200).

[0072] The second electrode (ELT2) may be pre-notched. Specifically, the second electrode (ELT2) may include a plurality of second electrode tabs (TAR2) protruding in the second direction (D2). The plurality of second electrode tabs (TAR2) may be arranged to be spaced apart from each other in the first direction (D1). When the second electrode (ELT2) is arranged on the first electrode (ELT1) and then a tab is formed on the second electrode, the first electrode (ELT1) having a larger width in the second direction (D2) may be damaged. On the other hand, the method for manufacturing an all-solid-state battery (S10) of the present invention can prevent damage to the first electrode (ELT1) by providing the second electrode (ELT2) on which the second electrode tabs (TAR2) are formed in advance.

[0073] Referring to FIGS. 3 and 7, the pressurizing process (S200) may include pressurizing a first electrode (ELT1) traveling in a first direction (D1) and a second electrode (ELT2) on the first electrode (ELT1). In one embodiment, the pressurizing may be line pressing with a first pressure.

[0074] Through the pressurizing process (S200), an electrode stack (ETS) in which a first electrode (ELT1) and a second electrode (ELT2) are joined can be formed. The electrode stack (S200) can continue to move in the first direction (D1).

[0075] In one embodiment, the pressurization process (S200) may be accompanied by heating. Through pressurization and heating, the interface between the first electrode (ELT1) and the second electrode (ELT2) may be activated.

[0076] For example, the pressurization process (S200) can be performed by the pressurization unit (PRU) described with reference to FIG. 1.

[0077] Referring to FIGS. 3 and 8, the notching process (S300) may include notching the first electrode (ELT1) of the electrode laminate (S200) running in the first direction (D1). Specifically, the notching may be performed on the first side (ENR) of the first electrode (ELT1). Through this, a plurality of first electrode tabs (TAR1) may be formed on the first side (ENR) of the first electrode (ELT1).

[0078] In one embodiment, the notching process (S300) may include measuring a position of a second electrode tab (TAR2) of a second electrode (ELT2) or a gap between adjacent second electrode tabs (TAR2) of the second electrode (ELT2); and notching a first end portion of the first electrode (ELT1) based on the position of the second electrode tab (TAR2) or the gap. Through this, a notching tolerance can be prevented, and consequently, product defects due to tolerance accumulation can be prevented.

[0079] Referring again to FIG. 8, the first electrode tabs (TAR1) of the first electrode (ELT1) can be formed to face the second electrode tabs (TAR2) of the second electrode (ELT2) in the second direction (D2).

[0080] In one embodiment, the first electrode tabs (TAR1) may be formed spaced apart in the first direction (D1).

[0081] In one embodiment, the first electrode tabs (TAR1) may be formed to be aligned with the second electrode tabs (TAR2) in a second direction (D2). The second direction (D2) may intersect the first direction (D1).

[0082] As an example, the notching process (S300) can be performed by the notching unit (NOU) described with reference to FIGS. 2a and 2b.

[0083] Referring to FIGS. 3 and 9, the cutting process (S400) may include cutting the electrode stack (ETS) at predetermined intervals. In one embodiment, the cutting process (S400) may be cutting the electrode stack (ETS) traveling in a first direction (D1) in a second direction (D2). Through this, an all-solid-state unit cell (UCL) may be manufactured. The all-solid-state unit cell (UCL) will be described later.

[0084] For example, the cutting process (S400) can be performed by the cutting unit (CTU) described with reference to FIG. 1.

[0085] Referring to FIGS. 3 and 13, the side coating process (S500) may include coating both sides of an all-solid unit cell (UCL) to form a protective layer. Specifically, the side coating process (S500) may be coating a coating composition on both sides of the all-solid unit cell (UCL) in the first direction (D1).

[0086] The type of coating composition is not limited as long as it has insulating properties.

[0087] The coating composition may include at least one selected from the group consisting of a UV-curable resin composition, a thermosetting resin, and a thermoplastic resin. The UV-curable resin composition may include a UV-curable resin, a solvent, and a photopolymerization initiator.

[0088] The UV curable resin may include urethane acrylate, unsaturated polyester, epoxy acrylate, oxetane, vinyl ether, polyester acrylate, silicone acrylate, cycloaliphatic epoxy resin, glycidyl ether epoxy resin, or a combination thereof.

[0089] In one embodiment, the solvent may be water or an organic solvent. For example, the organic solvent may be NMP or acetone.

[0090] In one embodiment, the photopolymerization initiator may be an alkylphenone compound, an acylphosphine oxide compound, a titanocene compound, an oxime ester compound, a benzoin compound, an acetophenone compound, a benzophenone compound, a thioxanthone compound, an α-acyl oxime ester compound, a phenylglyoxylate compound, a benzyl compound, an azo compound, a diphenyl sulfide compound, an organic pigment compound, an iron-phthalocyanine compound, a benzoin ether compound, an anthraquinone compound, a diazonium salt, an iodonium salt, a sulfonium salt, a metalnocene compound, or a combination thereof.

[0091] In one embodiment, the thermosetting resin may be an epoxy resin, a phenol resin, a melamine resin, a urea resin, an unsaturated polyester resin, an alkyd resin, a silicon resin, a polyurethane resin, a polyimide resin, or a combination thereof.

[0092] In one embodiment, the thermoplastic resin may be polytetrafluoroethylene, polyethylene, polypropylene, polystyrene, vinyl chloride, vinylidene chloride, fluororesin, acrylic resin, polyvinyl acetate resin, polyamide resin, polycarbonate, acetal resin, polyphenylene oxide, polyester, polysulfone, or a combination thereof.

[0093] By coating both sides of the all-solid-state unit cell (UCL) in the first direction (D1) with the coating composition to form a protective layer, a short circuit can be prevented.

[0094] In one embodiment, the method for manufacturing an all-solid-state battery (S10) may further include manufacturing an all-solid-state bi-cell by stacking two all-solid-state unit cells (UCL) facing each other. The method for manufacturing an all-solid-state battery (S10) may further include manufacturing an all-solid-state stack cell by alternately stacking the all-solid-state bi-cell or the all-solid-state unit cells (UCL) with elastic pads. Elastic pads may be provided on the lowermost and uppermost surfaces of the all-solid-state stack cell, respectively.

[0095] In one embodiment, when the all-solid-state unit cells (UCL) constituting the all-solid-state stack cell do not include a protective layer (PRL), the method may further include forming a protective layer on both sides of the all-solid-state stack cell. Forming the protective layer may be performed using the same process as forming the protective layer on the all-solid-state unit cell (UCL). Through this, the protective layer may be formed up to the side of the elastic pad.

[0096] In one embodiment, the method for manufacturing an all-solid-state battery (S10) may further include manufacturing a first electrode (ELT1) and a second electrode (ELT2).

[0097] In one embodiment, the first electrode (ELT1) may be a roll-type cathode laminate. The second electrode (ELT2) may be a roll-type anode laminate.

[0098] In one embodiment, a positive electrode laminate may be formed by stacking a positive electrode electrolyte layer on a positive electrode layer and then applying a second pressure. A negative electrode laminate may be formed by stacking a negative electrode electrolyte layer on a negative electrode layer and then applying a third pressure.

[0099] Since the positive and negative electrode laminates are manufactured using separate pressurization methods, the second and third pressures can be controlled differently. This allows for a relatively low pressure to be applied to the positive and negative electrode laminates, which may be damaged when pressurized at high pressure due to their low mechanical strength or severe structural imbalance.

[0100] The second pressure may be greater than the third pressure. For example, the second pressure may be defined as a pressure applied from the upper and lower surfaces of the positive electrode laminate toward the interior of the positive electrode laminate. The third pressure may be defined as a pressure applied from the upper and lower surfaces of the negative electrode laminate toward the interior of the negative electrode laminate.

[0101] Forming the above positive electrode laminate and negative electrode laminate may include a pressing process using a roll press.

[0102] When roll press is applied during the formation process of the above-mentioned positive electrode laminate, the linear pressure of the second pressure may be 1 ton / cm to 5 ton / cm. Specifically, the linear pressure of the second pressure may be 1 ton / cm to 4 ton / cm, 1 ton / cm to 3 ton / cm, or 1 ton / cm to 2.5 ton / cm.

[0103] When roll press is applied during the formation process of the above-mentioned negative electrode laminate, the linear pressure of the third pressure may be 1 ton / cm to 4 ton / cm. Specifically, the linear pressure of the third pressure may be 1 ton / cm to 3 ton / cm, 1 ton / cm to 2.5 ton / cm, or 1 ton / cm to 2 ton / cm.

[0104] The above pressurization process can be carried out at a relatively high temperature. Specifically, the pressurization process can be carried out at 60 to 150°C, 80 to 130°C, or 100 to 125°C.

[0105] Forming the above positive electrode laminate and negative electrode laminate may include a preheating process prior to the pressurizing process. Specifically, the positive electrode laminate and negative electrode laminate may be preheated to ±10°C and ±5°C, respectively, of the temperature at which the pressurizing process is performed. The preheating process may prevent damage to the positive electrode laminate and negative electrode laminate due to rapid temperature changes during the high-temperature pressurizing process.

[0106] Each of the manufactured positive electrode laminate and negative electrode laminate can be wound.

[0107] Hereinafter, the solid-state battery manufactured using the solid-state battery manufacturing device (10) and manufacturing method (S10) described above will be described in detail.

[0108] All-solid-state batteries

[0109] Fig. 10 is a plan view of an all-solid-state battery according to embodiments of the present invention. Fig. 11 is a cross-sectional view taken along line A-A' of Fig. 10. Fig. 12 is a cross-sectional view taken along line B-B' of Fig. 10.

[0110] Referring to Fig. 10, an all-solid-state battery according to one embodiment may be in the form of an all-solid-state unit cell (UCL). The all-solid-state unit cell (UCL) may include a first electrode sheet (ELS1) and a second electrode sheet (ELS2) on the first electrode sheet (ELS1). The first electrode sheet (ELS1) may be formed by cutting a first electrode (ELT1) extending in a first direction (D1) by a cutting unit (CTU). The second electrode sheet (ELS2) may be formed by cutting a second electrode (ELT2) extending in the first direction (D1) by a cutting unit (CTU).

[0111] In one embodiment, the first electrode sheet (ELS1) may include a cathode layer (200) and a cathode solid electrolyte layer (320) on the cathode layer (200). The second electrode sheet (ELS2) may include a cathode layer (100) and a cathode solid electrolyte layer (310) on the cathode layer (100). The cathode solid electrolyte layer (320) and the cathode solid electrolyte layer (310) may constitute a solid electrolyte layer (300). However, the present invention is not limited thereto, and the all-solid-state unit cell (UCL) may further include an additional functional layer, such as an adhesion enhancing layer, disposed between the cathode layer (100) and the solid electrolyte layer (300) or between the cathode layer (200) and the solid electrolyte layer (300).

[0112] Referring again to FIG. 10, the first electrode sheet (ELS1) may include a first electrode tab (TAR1) protruding in the second direction (D2). The second electrode sheet (ELS2) may include a second electrode tab (TAR2) protruding in the second direction (D2). A portion of the second electrode tab (TAR2) may be positioned on the first electrode (ELT1).

[0113] Referring to FIGS. 10 and 11, in one embodiment, the first electrode sheet (ELS1) may have a length L1 in the first direction (D1). The second electrode sheet (ELS2) may have a length L2 in the first direction (D1). L1 and L2 may be substantially the same.

[0114] In one embodiment, the first electrode sheet (ELS1) may have a width W1 in the second direction (D2). The second electrode sheet (ELS2) may have a width W2 in the second direction (D2). W1 may be greater than W2.

[0115] For example, the unit cell (UCL) may be manufactured by the above-described all-solid-state battery manufacturing device (10) or manufacturing method (S10). Specifically, the unit cell (UCL) may include a first electrode sheet, ESL1) and a second electrode sheet (ESL2) laminated on the first electrode sheet (ESL1). The length of the first electrode sheet (ESL1) in the first direction (D1) may be substantially the same as the length of the second electrode sheet (ELS2) in the first direction (D1). The width of the first electrode sheet (ESL1) in the second direction (D2) may be greater than the width of the second electrode sheet (ELS2) in the second direction (D2). Again, referring to FIG. 10, the first electrode sheet (ELS1) may include a first electrode tab (TAR1) protruding in the a direction (D2a) of the second direction (D2). The first electrode tab (TAR1) may not overlap with the second electrode sheet (ELS2). The second electrode sheet (ELS2) may include a second electrode tab (TAR2) protruding in the b direction (D2b) among the second directions (D2). The a direction (D2a) and the b direction (D2b) may be opposite directions. That is, the first electrode tab (TAR1) and the second electrode tab (TAR2) may protrude in opposite directions.

[0116] A portion of the second electrode tab (TAR2) may vertically overlap with the first electrode sheet (ELS1). For example, the second electrode tab (TAR2) may protrude so that a portion thereof overlaps with the first electrode sheet (ELS1) in the third direction (D3).

[0117] Referring to FIGS. 10 and 12, in one embodiment, the all-solid-state unit cell (UCL) may further include a first gasket (GSK1) and a second gasket (GSK2) on the first electrode sheet (ELS1). The first gasket (GSK1) and the second gasket (GSK2) may be positioned such that the second electrode sheet (ELS2) is positioned between the first gasket (GSK1) and the second gasket (GSK2). Specifically, a portion of the second electrode sheet (ELS2) excluding the second electrode tab (TAR2) may be positioned between the first gasket (GSK1) and the second gasket (GSK2). A portion of the second electrode tab (TAR2) may overlap the second gasket (GSK2) in a third direction (D3).

[0118] In one embodiment, the thickness of the second gasket (GSK2) in the third direction (D3) may be smaller than the thickness of the first gasket (GSK1) in the third direction (D3). The thickness of the second gasket (GSK2) in the third direction (D3) may be smaller than the thickness of the second electrode sheet (ELS2) in the third direction (D3).

[0119] The first gasket (GSK1) and the second gasket (GSK2) can prevent damage caused by the step difference between the first electrode sheet (ELS1) and the second electrode sheet (ELS2) during the pressurizing process (S200).

[0120] In another embodiment, the unit cell (UCL) may not include the first gasket (GSK1) and the second gasket (GSK2).

[0121] Fig. 13 is a cross-sectional view of an all-solid-state battery according to another embodiment of the present invention compared to Fig. 11. Referring to Fig. 13, the unit cell (UCL) may further include protective layers (PRL) arranged on both sides in the first direction (D1). This may prevent short circuiting of the first electrode sheet (ELS1) and the second electrode sheet (ELS2).

[0122] The positive electrode layer (100) of one embodiment may include a positive electrode current collector (110) and a positive electrode active material layer (120) disposed on the positive electrode current collector (110). The positive electrode active material layer (120) may include a positive electrode active material, a solid electrolyte, a conductive material, and a binder.

[0123] The positive electrode current collector (110) can provide a reference surface on which the positive electrode active material layer (120) is arranged. The positive electrode current collector (110) can include a plate or foil including, for example, indium (In), copper (Cu), magnesium (Mg), stainless steel, titanium (Ti), iron (Fe), cobalt (Co), nickel (Ni), zinc (Zn), aluminum (Al), germanium (Ge), lithium (Li), or an alloy thereof.

[0124] Meanwhile, unlike that illustrated in FIG. 10, in one embodiment of the present invention, the positive electrode current collector (110) may be omitted. Although not illustrated, a carbon layer having a thickness of 0.1 μm to 4 μm may be additionally disposed between the positive electrode current collector (110) and the positive electrode active material layer (120) to increase the bonding strength between the positive electrode current collector (110) and the positive electrode active material layer (120).

[0125] The cathode active material may include a material that can reversibly absorb and desorb lithium ions. The cathode active material may include a plurality of particles. The cathode active material may include, but is not necessarily limited to, lithium transition metal oxides such as lithium cobalt oxide (LCO), lithium nickel oxide, lithium nickel cobalt oxide, lithium nickel cobalt aluminum oxide (NCA), lithium nickel cobalt manganese oxide (NCM), lithium manganate, and lithium iron phosphate, nickel sulfide, copper sulfide, lithium sulfide, iron oxide, or vanadium oxide. The cathode active materials may be used alone or as a mixture of two or more.

[0126] Lithium transition metal oxides include, for example, Li a A 1-b B b D2(0.90≤a≤1, 0≤b≤0.5), Li a E 1-b B b O 2-c D c (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05), LiE 2-b B b O 4-c D c (0≤b≤0.5, 0≤c≤0.05), Li a Ni 1-b-c Co b B c D α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α<2), Li a Ni 1-b-c Co b B c O 2-α F α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α<2), Li a Ni 1-b-c Mn bB c D α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α≤2), Li a Nor 1-b-c Mn b B c O 2-α F α (0.90≤a≤1, 0≤b≤0.5, 0≤c≤0.05, 0<α<2), Li a Nor b E c G d O2(0.90≤a≤1, 0≤b≤0.9, 0≤c≤0.5, 0.001≤d≤0.1), Li a Nor b Co c Mn d GeO2(0.90≤a≤1, 0≤b≤0.9, 0≤c≤0.5, 0≤d≤0.5, 0.001≤e≤0.1), Li a NiG b O2(0.9≤a≤1, 0.001≤b≤0.1), Li a CoG b O2(0.90≤a≤1, 0.001≤b≤0.1), Li a MnG b O2(0.90≤a≤1, 0.001≤b≤0.1), Li a Mn2GbO4(0.90≤a≤1, 0.001≤b≤0.1), QO2, QS2, LiQS2, V2O5, LiV2O5, LiIO2, LiNiVO4, Li 3-f J2(PO4)3(0≤f≤2), Li 3-fA compound represented by any one of Fe2(PO4)3(0≤f≤2), LiFePO4. In these compounds, the capital letter “A” is Ni, Co, Mn, or a combination thereof, the capital letter “B” is Al, Ni, Co, Mn, Cr, Fe, Mg, Sr, V, a rare earth element, or a combination thereof, the capital letter “D” is O, F, S, P, or a combination thereof, the capital letter “E” is Co, Mn, or a combination thereof, the capital letter “F” is F, S, P, or a combination thereof, the capital letter “G” is Al, Cr, Mn, Fe, Mg, La, Ce, Sr, V, or a combination thereof, the capital letter “Q” is Ti, Mo, Mn, or a combination thereof, the capital letter “I” is Cr, V, Fe, Sc, Y, or a combination thereof, and the capital letter “J” is V, Cr, Mn, Co, Ni, Cu, or a combination thereof.

[0127] The cathode active material may include, for example, a lithium salt of a transition metal oxide having a layered rock salt type structure among the lithium transition metal oxides described above. The "layered rock salt type structure" is, for example, a cubic rock salt type structure. <111> It is a structure in which oxygen atomic layers and metal atomic layers are alternately and regularly arranged in a direction, and thereby each atomic layer forms a two-dimensional plane. The "cubic rock salt structure" refers to the sodium chloride type (NaCl type) structure, which is a type of crystal structure, and specifically refers to a structure in which the face-centered cubic lattice (fcc) formed by each cation and anion is arranged with a displacement of half of the ridge of the unit lattice. Lithium transition metal oxides having this layered rock salt structure include, for example, LiNi x Co y Al z O2(NCA) or LiNi x Co y Mn zO2(NCM) (0 <x<1,0<y<1, 0<z<1, x+y+z=1) 등의 삼원계 리튬전이금속산화물일 수 있다. 양극 활물질이 층상암염형 구조를 갖는 삼원계 리튬전이금속산화물을 포함하는 경우, 전고체 단위셀(UCL)의 에너지 밀도가 커지고 열안정성이 향상될 수 있다.

[0128] The above-described compound included in the positive electrode active material may be covered by a coating layer (not shown). The positive electrode active material may also be a mixture of the above-described compound and a compound to which a coating layer is added. Meanwhile, the coating layer added to the surface of the positive electrode active material may include, for example, an oxide, a hydroxide, an oxyhydroxide, an oxycarbonate, or a hydroxycarbonate of the coating elements below. The compound forming the coating layer is amorphous or crystalline. The coating elements included in the coating layer may include Mg, Al, Co, K, Na, Ca, Si, Ti, V, Sn, Ge, Ga, B, As, Zr, or mixtures thereof. The coating layer may include, for example, Li2O-ZrO2 (LZO). The method for forming the coating layer is selected within a range that does not adversely affect the physical properties of the positive electrode active material (PAM). The method for forming the coating layer includes, for example, spray coating, dipping, etc.

[0129] When the positive electrode active material is a ternary lithium transition metal oxide such as NCA or NCM and contains nickel (Ni), it is possible to increase the capacity density of the all-solid-state unit cell (UCL) and reduce metal dissolution of the positive electrode active material (PAM) in a charged state. As a result, the cycle characteristics of the all-solid-state unit cell (UCL) in a charged state are improved. Meanwhile, the "cycle characteristics" are characteristics indicating the degree to which the all-solid-state unit cell (UCL) is deteriorated by charge / discharge of the all-solid-state unit cell (UCL). An all-solid-state unit cell (UCL) with high cycle characteristics may have a small degree of deterioration of the all-solid-state unit cell (UCL) due to charge / discharge, and an all-solid-state unit cell (UCL) with low cycle characteristics may have a large degree of deterioration of the all-solid-state unit cell (UCL) due to charge / discharge.

[0130] The positive electrode active material may have a particle shape such as a sphere or an ellipsoid, for example. The particle size and content of the positive electrode active material are not particularly limited.

[0131] The solid electrolyte may have a particle shape. The solid electrolyte may be dispersed between the positive electrode active materials. The solid electrolyte may include a sulfide-based solid electrolyte having excellent lithium ion conductivity characteristics. Examples of the sulfide-based solid electrolyte include Li2S-P2S5, Li2S-P2S5-LiX (X is a halogen element), Li2S-P2S5-Li2O, Li2S-P2S5-Li2O-LiI, Li2S-SiS2, Li2S-SiS2-LiI, Li2S-SiS2-LiBr, Li2S-SiS2-LiCl, Li2S-SiS2-B2S3-LiI, Li2S-SiS2-P2S5-LiI, Li2S-B2S3, Li2S-P2S5-Z m S n (m, n are positive numbers, capital letter “Z” represents Ge, Zn or Ga), Li2S-GeS2, Li2S-SiS2-Li3PO4, Li2S-SiS2-Li p MO q(p, q are positive numbers, capital letter “M” is one of P, Si, Ge, B, Al, Ga In), Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x It may include at least one selected from (0≤x≤2).

[0132] Sulfide-based solid electrolytes include, for example, Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x It may be an argyrodite-type compound including at least one selected from (0≤x≤2). In particular, the sulfide-based solid electrolyte may be an argyrodite-type compound including at least one selected from Li6PS5Cl, Li6PS5Br, and Li6PS5I.

[0133] Alternatively, the sulfide-based solid electrolyte is Li 7-a M a PS 6-c X cIt may be an argyrodite-type compound containing (0≤a≤2, (0≤c≤2)), where X may be F, Br, Cl, or a combination thereof. M is candium (Sc), yttrium (Y), titanium (Ti), zirconium (Zr), hafnium (Hf), vanadium (V), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo), tungsten (W), manganese (Mn), technetium (Tc), rhenium (Re), iron (Fe), ruthenium (Ru), osmium (Os), cobalt (Co), rhodium (Rh), iridium (Ir), nickel (Ni), palladium (Pd), platinum (Pt), copper (Cu), silver (Ag), gold (Au), zinc (Zn), cadmium (Cd), mercury (Hg), aluminum (Al), gallium (Ga), indium (In), thallium (Tl), silicon (Si), germanium (Ge), tin (Sn), lead (Pb), arsenic (As), antimony (Sb), bismuth (Bi), or a combination thereof. Can be.

[0134] The density of the argyrodite-type solid electrolyte may be 1.5 g / cc to 2.0 g / cc. Since the argyrodite-type solid electrolyte has a density of 1.5 g / cc or more, the internal resistance of the all-solid-state battery is reduced, and the defect of the solid electrolyte membrane being penetrated and short-circuited due to the formation of lithium dendrites can be prevented. The elastic modulus of the solid electrolyte may be, for example, 15 GPa to 35 GPa.

[0135] The solid electrolyte in the positive electrode active material layer (120) may have a smaller median particle size average particle diameter (D50) than the first and second solid electrolytes (SE1, SE2) in the solid electrolyte layer (300) to be described later. For example, the median particle size average particle diameter (D50) of the solid electrolyte included in the positive electrode active material layer (120) may be 90% or less, 80% or less, 70% or less, 60% or less, 50% or less, 40% or less, 30% or less, or 20% or less of the median particle size average particle diameter (D50) of the solid electrolyte included in the solid electrolyte layer (300). Meanwhile, the median particle size average particle diameter (D50) may be a median diameter measured using a laser particle size distribution meter.

[0136] The positive electrode active material layer (120) may include a conductive material. The conductive material may have conductivity without causing chemical changes in the all-solid-state unit cell (UCL), thereby increasing the conductivity of the positive electrode active material and the solid electrolyte. The conductive material may include a carbon-based material. For example, the conductive material may include one or more selected from graphite, carbon black, acetylene black, carbon nanofibers, and carbon nanotubes.

[0137] The positive electrode active material layer (120) may further include a binder. The binder may bind the positive electrode active material, the solid electrolyte, and the conductive material within the positive electrode active material layer (120) to each other. The binder may include a material for improving the bonding strength between the positive electrode active material layer (120) and the positive electrode current collector (110). The binder may include, for example, polyvinylidene fluoride, styrene butadiene rubber (SBR), polytetrafluoroethylene, polyvinylidene fluoride, vinylidene fluoride / hexafluoropropylene copolymer, polyacrylonitrile, and polymethyl methacrylate.

[0138] Based on 100 parts by weight of the total of the positive electrode active material, the solid electrolyte, the conductive agent, and the binder, the positive electrode active material layer (120) may include 85 parts by weight or more and 92 parts by weight or less of the positive electrode active material. Based on 100 parts by weight of the total of the positive electrode active material (PAM), the solid electrolyte, the conductive agent, and the binder, the positive electrode active material layer (120) may include 0.5 parts by weight or more and 1.5 parts by weight or less of the binder.

[0139] Based on 100 parts by weight of the solid electrolyte, the positive electrode active material layer (120) may include 1 part by weight or more and 50 parts by weight or less of a conductive material. When the conductive material is included in the positive electrode active material layer (120) in an amount of less than 1 part by weight based on 100 parts by weight of the solid electrolyte, the proportion of the conductive material may decrease, thereby lowering the electrical conductivity of the positive electrode active material layer (120). When the conductive material is included in the positive electrode active material layer (120) in an amount of more than 50 parts by weight based on 100 parts by weight of the solid electrolyte, the proportion of the conductive material may be excessively high, so that a covering layer covering the surface of the solid electrolyte may not be properly formed.

[0140] The positive electrode active material layer (120) may further include additives such as fillers, coating agents, dispersants, and ion conductive aids in addition to the above-described positive electrode active material, solid electrolyte, conductive agent, and binder.

[0141] The negative electrode layer (200) may include a negative electrode current collector (210) and a negative electrode coating layer (220) on the negative electrode current collector (210). The negative electrode current collector (210) may provide a reference surface on which the negative electrode coating layer (220) is disposed. The negative electrode current collector (210) may include, for example, a material that does not react with lithium, i.e., does not form an alloy or a compound with lithium. For example, the negative electrode current collector (210) may include at least one metal selected from the group consisting of copper (Cu), stainless steel, titanium (Ti), iron (Fe), cobalt (Co), and nickel (Ni). The thickness of the negative electrode current collector (210) may be 1 μm to 20 μm, more specifically 5 μm to 15 μm, and more specifically 7 μm to 10 μm.

[0142] The negative electrode current collector (210) may be composed of one of the above-described metals, or may include an alloy or coating material of two or more metals. The negative electrode current collector (210) may have, for example, a plate shape or a foil shape. Meanwhile, in one embodiment, the negative electrode current collector (210) may be omitted.

[0143] The cathode coating layer (220) can allow lithium metal to grow between the cathode current collector (210) and the all-solid-state unit cell (UCL) when charging. The cathode coating layer (220) can act as a protective layer for the lithium metal and simultaneously suppress the precipitation and growth of lithium dendrites.

[0144] The cathode coating layer (220) may include a metal and carbon. For example, the cathode coating layer (220) may include at least one metal selected from the group consisting of gold (Au), platinum (Pt), palladium (Pd), silicon (Si), silver (Ag), aluminum (Al), bismuth (Bi), tin (Sn), and zinc (Zn). The cathode coating layer (220) may include at least one carbon selected from the group consisting of carbon black, acetylene black, furnace black, ketjen black, and graphene. In one embodiment, the cathode coating layer (220) may include a mixture of carbon black and silver (Ag).

[0145] The cathode coating layer (220) may further include additives other than metal and carbon. The cathode coating layer (220) may further include, for example, at least one additive selected from the group consisting of a binder, a filler, a coating agent, a dispersant, and an ion conductive additive.

[0146] The negative electrode coating layer (220) may have a smaller thickness than the positive electrode active material layer (120). The thickness of the negative electrode coating layer (220) may be, for example, 50% or less, 40% or less, 30% or less, 20% or less, 10% or less, or 5% or less of the thickness of the positive electrode active material layer (120). The thickness of the negative electrode coating layer (220) may be, for example, 1 um to 20 um, 2 um to 10 um, or 3 um to 7 um. If the thickness of the negative electrode coating layer (220) is too thin, lithium dendrites formed between the negative electrode coating layer (220) and the negative electrode current collector (210) may collapse the negative electrode coating layer (220), thereby deteriorating the cycle characteristics of the all-solid-state unit cell (UCL). If the thickness of the cathode coating layer (220) increases excessively, the energy density of the all-solid-state unit cell (UCL) may decrease and the internal resistance of the all-solid-state unit cell (UCL) due to the cathode coating layer (220) may increase, thereby deteriorating the cycle characteristics of the cell.

[0147] Meanwhile, although not shown, a carbon layer may be further included to improve adhesion between the cathode coating layer (220) and the solid electrolyte layer (300).

[0148] A solid electrolyte layer (300) may be provided between the positive electrode layer (100) and the negative electrode layer (200). The solid electrolyte layer (300) may include a sulfide-based solid electrolyte having excellent lithium ion conductivity characteristics. The solid electrolyte in the solid electrolyte layer (300) may be the same as or different from any one of the materials included in the solid electrolyte in the positive electrode active material layer (120) described above.

[0149] The solid electrolyte layer (300) may include an anode solid electrolyte layer (310) and a cathode solid electrolyte layer (320). The anode solid electrolyte layer (310) may be adjacent to the anode layer (100), and the cathode solid electrolyte layer (320) may be adjacent to the cathode layer (200).

[0150] The positive electrode solid electrolyte layer (310) may include a first solid electrolyte (SE1), and the negative electrode solid electrolyte layer (320) may include a second solid electrolyte (SE2). Each of the first and second solid electrolytes (SE1, SE2) may have a particle shape such as a sphere or an ellipsoid.

[0151] Each of the first and second solid electrolytes (SE1, SE2) may include a sulfide-based solid electrolyte. The first and second solid electrolytes (SE1, SE2) may be the same or different. Each of the first and second solid electrolytes (SE1, SE2) may be amorphous, crystalline, or a mixture thereof. In addition, the solid electrolyte may include, for example, at least sulfur (S), phosphorus (P), and lithium (Li) as constituent elements among the above-described sulfide-based solid electrolyte materials. For example, the solid electrolyte may be a material including Li2S-P2S5. When using a sulfide-based solid electrolyte material including Li2S-P2S5 to form the solid electrolyte, the mixing molar ratio of Li2S and P2S5 is, for example, in the range of Li2S:P2S5=50:50 to 90:10.

[0152] Sulfide-based solid electrolytes include, for example, Li 7-x PS 6-x Cl x (0≤x≤2), Li 7-x PS 6-x Br x (0≤x≤2), and Li 7-x PS 6-x I x It may be an argyrodite-type compound including at least one selected from (0≤x≤2). In particular, the sulfide-based solid electrolyte may be an argyrodite-type compound including at least one selected from Li6PS5Cl, Li6PS5Br, and Li6PS5I.

[0153] Alternatively, the sulfide-based solid electrolyte is Li 7-a Ma PS 6-c X c It may be an argyrodite-type compound containing (0≤a≤2, (0≤c≤2)), where X may be F, Br, Cl, or a combination thereof. M is candium (Sc), yttrium (Y), titanium (Ti), zirconium (Zr), hafnium (Hf), vanadium (V), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo), tungsten (W), manganese (Mn), technetium (Tc), rhenium (Re), iron (Fe), ruthenium (Ru), osmium (Os), cobalt (Co), rhodium (Rh), iridium (Ir), nickel (Ni), palladium (Pd), platinum (Pt), copper (Cu), silver (Ag), gold (Au), zinc (Zn), cadmium (Cd), mercury (Hg), aluminum (Al), gallium (Ga), indium (In), thallium (Tl), silicon (Si), germanium (Ge), tin (Sn), lead (Pb), arsenic (As), antimony (Sb), bismuth (Bi), or a combination thereof. Can be.

[0154] The density of the argyrodite-type solid electrolyte may be 1.5 g / cc to 2.0 g / cc. Since the argyrodite-type solid electrolyte has a density of 1.5 g / cc or more, the internal resistance of the all-solid-state battery is reduced, and the defect of the solid electrolyte membrane being penetrated and short-circuited due to the formation of lithium dendrites can be prevented. The elastic modulus of the first solid electrolyte (SE1) is, for example, 15 GPa to 35 GPa.

[0155] Each of the positive and negative electrode solid electrolyte layers (310, 320) may further include a binder. The binder included in the solid electrolyte layer (300) may be, for example, styrene butadiene rubber (SBR), polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, or the like, but is not limited thereto. The binder of the positive and negative electrode solid electrolyte layers (310, 320) may be the same as or different from the binder included in the positive electrode active material layer (120) or the binder included in the negative electrode coating layer (220).

[0156] Referring back to FIG. 11, the positive electrode solid electrolyte layer (310) and the negative electrode solid electrolyte layer (320) may have the same or different thicknesses. The positive electrode solid electrolyte layer (310) may have a first thickness (TK1), and the negative electrode solid electrolyte layer (320) may have a second thickness (TK2). For example, the first thickness (TK1) may be greater than the second thickness (TK2). For example, the first thickness (TK1) may be 2 to 100 times greater than the second thickness (TK2). For example, the second thickness (TK2) may be greater than the first thickness (TK1). For example, the second thickness (TK2) may be 2 to 100 times greater than the first thickness (TK2).

[0157] In one embodiment, the positive electrode solid electrolyte layer (310) may have substantially the same area as the positive electrode layer (100). The negative electrode solid electrolyte layer (320) may have substantially the same area as the negative electrode layer (200).

[0158] The all-solid-state unit cell (UCL) according to the present embodiment can be manufactured by forming a positive electrode laminate of a positive electrode layer (100) and a positive electrode solid electrolyte layer (310), forming a negative electrode laminate of a negative electrode layer (200) and a negative electrode solid electrolyte layer (320), and then laminating the positive electrode laminate and the negative electrode laminate.

[0159] In one embodiment, the all-solid-state unit cell (UCL) may be in the form of a mono-cell including an anode layer, a cathode layer, and a solid electrolyte layer disposed between the anode layer and the cathode layer as described above.

[0160] In another embodiment, the all-solid-state battery may be an all-solid-state bi-cell. For example, the all-solid-state bi-cell may include two unit cells (UCL) as described above. That is, the all-solid-state bi-cell may include a first unit cell and a second unit cell. Each of the first and second unit cells may include a positive electrode layer, a negative electrode layer, and a solid electrolyte layer disposed between the positive electrode layer and the negative electrode layer. The solid electrolyte layer of each of the first and second unit cells may include the positive electrode solid electrolyte layer and the negative electrode solid electrolyte layer as described above. Each of the first and second unit cells may further include a protective layer formed on both side surfaces. The positive electrode layer of the first unit cell and the positive electrode layer of the second unit cell may face each other.

[0161] In another embodiment, the all-solid-state battery may be an all-solid-state stack cell. The all-solid-state stack cell may include a plurality of all-solid-state unit cells (UCLs) as described above. The all-solid-state stack cell may further include elastic pads. The all-solid-state stack cell may have a structure in which unit cells or bicells and elastic pads are alternately stacked. For example, the all-solid-state stack cell may have a structure in which elastic pads, bicells, elastic pads, bicells, and elastic pads are stacked in that order.

[0162] In one embodiment, the all-solid-state stack cell may further include a protective layer on both sides. The protective layer may be identical to the protective layer of the unit cell (UCL) described with reference to FIG. 13. The protective layer may cover the sides of the elastic pad of the all-solid-state stack cell.

[0163]

[0164] Although the preferred embodiments of the present invention have been described above, the present invention is not limited thereto, and various modifications can be made within the scope of the claims, the detailed description of the invention, and the attached drawings, and it is obvious that this also falls within the scope of the present invention.

Claims

1. An electrode supply unit including a first supply roll on which a first electrode is wound and a second supply roll on which a second electrode is wound, the second electrode including a plurality of second electrode tabs; A pressing unit configured to laminate the first electrode traveling in the first direction and the second electrode traveling in the first direction to each other to form an electrode laminate; and Including a notching unit configured to form a plurality of first electrode tabs by notching the first side of the first electrode, The above notching unit: A sensing unit configured to measure the position or spacing of the plurality of second electrode tabs; and An all-solid-state battery manufacturing device comprising a tab forming unit configured to notch the first electrode based on the position or the gap.

2. In paragraph 1, Further comprising a gasket supply unit configured to supply a first gasket and a second gasket, The first gasket and the second gasket are arranged to be spaced apart from each other in a second direction on the first electrode, the second direction intersecting the first direction, An all-solid-state battery manufacturing device, wherein the second electrode is disposed between the first gasket and the second gasket.

3. In paragraph 1, An all-solid-state battery manufacturing device, wherein the sensing unit includes a vision sensor, an ultrasonic sensor, an infrared sensor, a laser sensor, or a combination thereof.

4. In paragraph 1, It further includes a cutting unit configured to cut the electrode laminate on which the first electrode tabs are formed at a predetermined interval, An all-solid-state battery manufacturing device in which a unit cell is formed by the above cutting.

5. In paragraph 4, Further comprising a cell transfer unit and a magazine unit, An all-solid-state battery manufacturing device, wherein the cell transfer unit is configured to transfer the unit cell from the cutting unit to the magazine unit.

6. In paragraph 4, Including a side coating unit, An all-solid-state battery manufacturing device, wherein the side coating unit is configured to form a protective layer by coating both sides of the unit cell.

7. In paragraph 6, The above side coating unit An all-solid-state battery manufacturing device comprising a sprayer configured to spray a coating composition.

8. In paragraph 1, The above first electrode: It comprises a negative electrode current collector, a negative electrode coating layer on the negative electrode current collector, and a negative electrode solid electrolyte layer on the negative electrode coating layer. The second electrode is: An all-solid-state battery manufacturing device comprising a positive electrode current collector, a positive electrode active material layer on the positive electrode current collector, and a positive electrode solid electrolyte layer on the positive electrode active material layer.

9. In paragraph 1, The plurality of first electrode tabs are formed to be aligned with the plurality of second electrode tabs in the second direction, respectively, An all-solid-state battery manufacturing device, wherein the second direction intersects the first direction.

10. An electrode supply process for unwinding the wound first and second electrodes and driving them in a first direction, wherein the second electrode includes a plurality of second electrode tabs protruding in a second direction; A pressing process for forming an electrode laminate by laminating the first electrode traveling in the first direction and the second electrode traveling in the first direction with each other; and Including a notching process for forming a plurality of first electrode tabs by notching the first electrode of the electrode laminate, The above notching process is: Measuring the position or spacing of the plurality of second electrode tabs; and A method for manufacturing an all-solid-state battery, comprising notching a first side of the first electrode based on the position or the gap.

11. In paragraph 10, The above electrode supply process: Unwinding the wound first and second gaskets and causing them to travel in the first direction; and Further comprising placing the second electrode, the first gasket and the second gasket on the first electrode, A method for manufacturing an all-solid-state battery, wherein the first gasket and the second gasket are arranged to be spaced apart from each other in a second direction.

12. In paragraph 10, A method for manufacturing an all-solid-state battery, wherein the first electrode tabs and the second electrode tabs are formed to face each other in a second direction.

13. In paragraph 10, After the above notching process, A method for manufacturing an all-solid-state battery, further comprising a process of manufacturing an all-solid-state unit cell by cutting the electrode laminate.

14. In paragraph 13. A method for manufacturing an all-solid-state battery, further comprising forming a protective layer by coating both sides of the all-solid-state unit cell with a coating composition.

15. In paragraph 14, A method for manufacturing an all-solid-state battery, wherein the coating composition comprises at least one selected from the group consisting of a UV-curable resin composition, a thermosetting resin, and a thermoplastic resin.

16. In paragraph 10, The above first electrode: It comprises a negative electrode current collector, a negative electrode coating layer on the negative electrode current collector, and a negative electrode solid electrolyte layer on the negative electrode coating layer. The second electrode is: A method for manufacturing an all-solid-state battery, comprising: a positive electrode current collector, a positive electrode active material layer on the positive electrode current collector, and a positive electrode solid electrolyte layer on the positive electrode active material layer.

17. In paragraph 10, The plurality of first electrode tabs are formed to be aligned with the plurality of second electrode tabs in the second direction, respectively, A method for manufacturing an all-solid-state battery, wherein the second direction intersects the first direction.

18. Including a first electrode sheet and a second electrode sheet laminated on the first electrode sheet, The length of the first electrode sheet in the first direction is substantially the same as the length of the second electrode sheet in the first direction, The width of the first electrode sheet in the second direction is greater than the width of the second electrode sheet in the second direction, The first electrode sheet includes a first electrode tab protruding in the second direction, The second electrode sheet includes a second electrode tab protruding in the opposite direction to the second direction, The above first electrode tab does not overlap with the above second electrode sheet, An all-solid-state battery, wherein a portion of the second electrode tab vertically overlaps the first electrode sheet.

19. In paragraph 18, The first electrode sheet includes a negative electrode current collector, a negative electrode coating layer on the negative electrode current collector, and a negative electrode solid electrolyte layer on the negative electrode coating layer, The above second electrode sheet includes a positive electrode current collector, a positive electrode active material layer on the positive electrode current collector, and a positive electrode solid electrolyte layer on the positive electrode active material layer. An all-solid-state battery, wherein the second electrode sheet is disposed on the first electrode sheet so that the negative electrode solid electrolyte layer and the positive electrode solid electrolyte layer face each other.

20. In paragraph 18, An all-solid-state battery further comprising a protective layer disposed on both sides of the all-solid-state battery.

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