All-solid-state battery manufacturing apparatus and all-solid-state battery manufacturing method using same

Abstract

The present invention relates to an all-solid-state battery manufacturing apparatus and manufacturing method, and an all-solid-state battery manufactured using same, and more specifically, the all-solid-state battery manufacturing apparatus according to the present invention comprises: an electrode supply unit; a moving cutting unit which cuts a traveling second electrode to form a second electrode sheet and transfers the second electrode sheet onto a traveling first electrode; a pressing unit which laminates the traveling first electrode and the second electrode sheet to each other to form an electrode stack; and a cell cutting unit which cuts the electrode stack at predetermined intervals to form unit cells.

Description

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

[0001] The present invention relates to an all-solid-state battery manufacturing device and an all-solid-state battery manufacturing method using the same.

[0002] 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.

[0003] 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.

[0004] 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.

[0005] 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.

[0006]

[0007] An all-solid-state battery manufacturing device according to the concept of the present invention may include an electrode supply unit including a first electrode supply roll on which a first electrode is wound and a second electrode supply roll on which a second electrode is wound; a moving cutting unit configured to cut the moving second electrode to form a second electrode sheet and transfer the second electrode sheet onto the moving first electrode; a pressing unit configured to laminate the moving first electrode and the second electrode sheet to each other to form an electrode laminate; and a cell cutting unit configured to cut the electrode laminate at predetermined intervals to form a unit cell.

[0008] A method for manufacturing an all-solid-state battery according to another concept of the present invention may include: unwinding wound first and second electrodes to travel in a first direction; cutting the second electrode to form a second electrode sheet; transferring the second electrode sheet onto the first electrode; pressing the first electrode and the second electrode sheet on the first electrode with a first pressure to form an electrode laminate; and cutting the electrode laminate at predetermined intervals to manufacture a unit cell.

[0009] 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 may be greater than 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 includes a first electrode tab protruding in a direction opposite to the second direction, and the second electrode sheet includes a second electrode tab protruding in the second direction, and the first electrode tab may not overlap the second electrode sheet. A portion of the second electrode tab may vertically overlap the first electrode sheet.

[0010]

[0011] 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, enabling the process to be performed without separate driving auxiliary materials.

[0012] FIG. 1 is a cross-sectional view of an all-solid-state battery manufacturing device according to embodiments of the present invention.

[0013] FIG. 2 is a schematic diagram illustrating a moving cutting unit according to one embodiment of the present invention.

[0014] Figure 3 is a flowchart for explaining a method for manufacturing an all-solid-state battery according to embodiments of the present invention.

[0015] FIGS. 4a, 4b, 4c, 5a, 5b, 6a, 6b, and 7 to 11 are conceptual diagrams illustrating a method for manufacturing an all-solid-state battery according to embodiments of the present invention.

[0016] Fig. 12a is a plan view of an all-solid-state battery according to one embodiment of the present invention. Fig. 12b is a cross-sectional view taken along line AA' of Fig. 12a.

[0017] Figure 13 is a plan view of an all-solid-state battery according to another embodiment of the present invention.

[0018] Figure 14 is a plan view of a gasket according to one embodiment of the present invention.

[0019]

[0020] 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.

[0021] 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.

[0022] 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.

[0023] 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.

[0024] In this specification, the term “connected” includes not only a case where member A and member B are directly connected, but also a case where member C is interposed between member A and member B, so that member A and member B are indirectly connected.

[0025]

[0026] All-solid-state battery manufacturing device (10)

[0027] The all-solid-state battery manufacturing device according to embodiments of the present invention can manufacture an all-solid-state battery without separate driving auxiliary materials by providing roll-type electrodes.

[0028] Furthermore, by continuously cutting and providing a notched second electrode on the moving first electrode, cells can be assembled continuously without stopping the equipment. In other words, all-solid-state batteries can be manufactured through continuous operation, rather than through go-and-stop operation, thereby improving productivity.

[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 (ESU); a moving cut unit (MCU); a film supply unit (FSU); a pressurizing unit (PRU); and a cell cutting unit (CTU).

[0030] An electrode supply unit (ESU) can be configured to unwind and drive the wound first and second electrodes.

[0031] A moving cutting unit (MCU) may be configured to cut a moving second electrode to form a second electrode sheet. In addition, the moving cutting unit (MCU) may be configured to align and place the second electrode sheet on the moving first electrode. When aligning the second electrode sheet, the first electrode tab of the first electrode and the second electrode tab of the second electrode sheet may be set as alignment reference points.

[0032] A film supply unit (FLU) may be configured to supply an upper film and a lower film. The upper film and the lower film may protect the first electrode and the second electrode sheet on the first electrode. The upper film and the lower film may be detached after the pressing process.

[0033] The pressurizing unit (PRU) can be configured to laminate a first electrode and a second electrode sheet on the first electrode, thereby forming an electrode laminate.

[0034] A cutting unit (CTU) can be configured to cut the electrode stack into a predetermined size. Through this, an all-solid-state unit cell can be formed.

[0035] Below, each component of the all-solid-state battery manufacturing device (10) is described in more detail.

[0036] An electrode supply unit (ESU) may be configured to supply a first electrode (ELT1) and a second electrode (ELT2). The first electrode (ELT1) and the second electrode (ELT2) may each be a wound roll type electrode.

[0037] In one embodiment, the electrode supply unit (ESU) may include a first electrode supply roll (ESR1) on which a first electrode (ELT1) is wound and a second electrode supply roll (ESR2) on which a second electrode (ELT2) is wound. The first electrode (ELT1) may be unwound on the first electrode supply roll (ESR1). The second electrode (ELT2) may be unwound on the second supply roll (ESR2).

[0038] In one embodiment, the first electrode (ELT1) and the second electrode (ELT2) may each be notched. Specifically, the first electrode (ELT1) may include a plurality of first electrode tabs. The second electrode (ELT2) may include a plurality of second electrode tabs.

[0039] In one embodiment, a plurality of first electrode tabs may be spaced apart from each other in the longitudinal direction of the first electrode (ELT1). The longitudinal direction of the first electrode (ELT1) may be the first direction (D1).

[0040] In one embodiment, a plurality of second electrode tabs may be spaced apart from each other in the longitudinal direction of the second electrode (ELT2). The longitudinal direction of the second electrode (ELT2) may be the first direction (D1).

[0041] 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).

[0042] The electrode supply unit (ESU) 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). In one embodiment, the plurality of first guide rollers (GUR1) may adjust a driving path so that the first electrode (ELT1) unwound from the first electrode 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 electrode supply roll (ESR2) travels in the first direction (D1).

[0043] Although not shown, in one embodiment, the electrode supply unit (ESU) 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 travel path of the object. The skew correction unit may further include a servo motor to precisely adjust the travel path of the object.

[0044] Figure 2 is a schematic diagram showing the configuration of a moving cutting unit (MCU).

[0045] Referring to FIGS. 1 and 2, the moving cutting unit (MCU) can be configured to cut the second electrode (ELT2) and provide it on the first electrode (ELT1). Specifically, the moving cutting unit (MCU) can cut the second electrode (ELT2) to form a second electrode sheet (ELS2) of a predetermined size. In addition, the moving cutting unit (MCU) can align and transfer the second electrode sheet (ELS2) on the upper surface of the first electrode (ELT1). For example, the moving cutting unit (MCU) can align and then stack the second electrode sheet (ELS2) on the upper surface of the first electrode (ELT1). Alternatively, the moving cutting unit (MCU) can transfer the second electrode sheet (ELS2) to the nip roll (NIP) so that the second electrode sheet (ELS2) is aligned on the upper surface of the first electrode (ELT1). By passing the first electrode (ELT1) and the second electrode sheet (ELS2) through the nip roll together, the second electrode sheet (ELS2) can be laminated on the first electrode (ELT1). The second electrode sheet (ELS2) can include one or more second electrode tabs. For example, the second electrode sheet (ELS2) can include one second electrode tab.

[0046] As an example, referring to FIG. 2, a moving cutting unit (MCU) may include a main frame (MFR), a vertical frame (VFR) connected to the main frame (MFR), a driving part (DRP), a moving cutter (MOC), a gripper (GRP), and a feeding part (FDP).

[0047] The driving unit (DRP) may include a horizontal driving unit (HDP) configured to horizontally move the moving cutter (MOC) and the gripper (GRP) and a vertical driving unit (VDP) configured to vertically move the moving cutter (MOC) and the gripper (GRP). The driving unit (DRP) may further include a servo motor to precisely control the movement of the moving cutter (MOC) and the gripper (GRP).

[0048] Referring back to FIG. 2, the moving cutter (MOC) may include an upper layer (UBL) and a lower layer (LBL). The upper layer (UBL) may be fixed to an upper layer holder (UBH). The upper layer holder (UBH) may be connected to a vertical driving unit (VDP). The lower layer (LBL) may be fixed to an lower layer support (LBS). The lower layer support (LBS) may be connected to a vertical frame (VFR). The moving cutter (MOC) may cut a second electrode (ELT2) to form a second electrode sheet (ELS2). In one embodiment, the horizontal driving unit (HDP) may adjust a cutting interval of the second electrode by horizontally moving the moving cutter (MOC) in a first direction (D1) and a direction opposite to the first direction (D1). Through this, the width of the second electrode sheet (ELS2) formed by cutting the second electrode (ELT2) may be adjusted.

[0049] Referring again to FIG. 2, the gripper (GRP) may include an upper grip (UGR) and a lower grip (LGR). The upper grip (UGR) may be connected to a vertical drive unit (VDP). The lower grip (LGR) may be fixed to a lower support (LBS). The gripper (GRP) may transfer and align the cut second electrode sheet (ELS2) onto the upper surface of the first electrode (ELT1). Specifically, the gripper (GRP) may grip the second electrode sheet (ELS2) and align it on the upper surface of the first electrode (ELT1).

[0050] Referring again to FIG. 2, the feeding unit (FDP) can drive the second electrode (ELT2) with the moving cutter (MOC). The feeding unit (FDP) can control the driving speed of the second electrode (ELT2). The feeding unit (FDP) can contribute to the unwinding of the second electrode (ELT2) from the second electrode supply roll (ESR2).

[0051] In one embodiment, the feeding part (FDP) can cause the remaining portion of the second electrode (ELT2) to travel along the moving cutter (MOC) when the moving cutter (MOC) cuts the second electrode (ELT2) to form the second electrode sheet (ELS2). This allows the tension of the second electrode (ELT2) to be maintained.

[0052] In one embodiment, when the moving cutting unit (MCU) directly laminates the second electrode sheet (ELS2) on the first electrode (ELT1), the lamination speed of the second electrode sheet (ELS2) can be synchronized with the pressing speed of the pressing unit (PRU) described later. For example, the rotation speed of the pressing roller (PRR) and the speed at which the moving cutting unit (MCU) provides the second electrode sheet (ELS2) on the first electrode (ELT1) can be synchronized. Through this, the process can be performed continuously without stopping the moving first electrode (ELT1) and second electrode (ELT2).

[0053] In another embodiment, referring back to FIG. 1, the moving cutting unit (MCU) can transfer the second electrode sheet (ELS2) to the nip roll (NIR) through which the first electrode (ELS1) passes. Through this, the second electrode sheet (ELS2) can be laminated and adhered to the first electrode (ELT1). When the moving cutting unit (MCU) transfers the second electrode to the nip roll, the speed at which the moving cutting unit (MCU) transfers the second electrode sheet (ELS2) to the nip roll (NIP) can be synchronized with the pressing speed of the pressurizing unit (PRU). For example, the rotational speed and speed of the pressurizing roller (PRR) and the speed at which the moving cutting unit (MCU) transfers the second electrode sheet (ELS2) to the nip roll (NIP) can be synchronized. Through this, the process can be performed continuously without stopping the moving first electrode (ELT1) and second electrode (ELT2).

[0054] Referring back to FIG. 1, the all-solid-state battery manufacturing device (10) may further include a sensing unit (ADU). The sensing unit (ADU) may be configured to measure the positions or spacings of a plurality of first electrode tabs of the first electrode (ELT1). The moving cutting unit (MCU) may transfer the second electrode sheet (ELS2) onto the first electrode (ELT1) based on the positions or spacings of the first electrode tabs measured as described above. For example, the moving cutting unit (MCU) may transfer and align the second electrode sheet (ELS2) onto the upper surface of the first electrode (ELT2) such that the second electrode tabs are aligned with the first electrode tabs (TAR1) in the second direction (D2).

[0055] In one embodiment, the sensing unit (ADU) may include a vision sensor, an ultrasonic sensor, an infrared sensor, a laser sensor, or a combination thereof.

[0056] Referring back to FIG. 1, the all-solid-state battery manufacturing device (10) may include a film supply unit (FSU). The film supply unit (FSU) may be configured to supply an upper film (UFM). The film supply unit (FSU) may further be configured to supply a lower film (LFM). Each of the upper film (UFM) and the lower film (LFM) may be a wound roll-type film.

[0057] In one embodiment, the film supply unit (FSU) may include a first film supply roll (FSR1) on which an upper film (UFM) is wound and a second film supply roll (FSR2) on which a lower film (LFM) is wound. The upper film (UFM) may be unwound from the first film supply roll (FSR1). The lower film (LFM) may be unwound from the second film supply roll (FSR2).

[0058] The upper film (UMF) may be provided on the upper surface of the driving second electrode sheet (ELS2). The lower film (LFM) may be provided on the lower surface of the driving first electrode (ELT1).

[0059] Referring back to FIG. 1, in one embodiment, a first electrode (ELT1), a second electrode sheet (ELS2) on the first electrode (ELT1), and an upper film (UFM) on the second electrode sheet (ELS2) can pass through a nip roll (NIR). As a result, the first electrode (ELT1), the second electrode sheet (ELS2), and the upper film (UFM) can be brought into close contact.

[0060] The film supply unit (FSU) may further include a plurality of second guide rollers (GUR2). The plurality of second guide rollers (GUR1) may adjust the running directions of the upper film (UFM) and the lower film (LFM). In one embodiment, the plurality of second guide rollers (GUR2) may adjust a running path so that the upper film (UFM) unwound from the first film supply roll (FSR1) runs in the first direction (D1). In addition, the plurality of second guide rollers (GUR2) may adjust a running path so that the lower film (LFM) unwound from the second film supply roll (FSR2) runs in the first direction (D1).

[0061] 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 one or more feeding belts or feeding rolls.

[0062] In one embodiment, the first feeding unit (FDU1) may be driven by a power source to contribute to unwinding of the first electrode (ELT1) from the first electrode supply roll (ESR1). In addition, the first feeding unit (FDU1) may contribute to unwinding of the upper film (UFM) from the first film supply roll (FSR1) and unwinding of the lower film (LFM) from the second film supply roll (FSR2).

[0063] Referring back to FIG. 1, the all-solid-state battery manufacturing device (10) may include a pressurizing unit (PRU). 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 sheet (ELS2) on the first electrode (ELT1) with each other. When a lower film (LFM) is provided on a lower surface of the first electrode (ELT1), the lower film (LFM) serves to protect a lower surface of the electrode stack (ETS). When the upper film (UFM) is provided on the second electrode sheet (ELS2), the upper film (UFM) protects the electrode laminate and serves to maintain the alignment of the second electrode sheet (ELS2) laminated on the upper surface of the first electrode (ELT1).

[0064] In one embodiment, the pressurization unit (PRU) may further include a heater (HEA) configured to heat the object. Through this, the pressurization unit (PRU) may heat and pressurize the object.

[0065] Referring back to FIG. 1, the all-solid-state battery manufacturing device (10) may include a film recovery unit (FRU). The film recovery unit (FRU) may be configured to recover upper and lower films provided on the upper and lower surfaces of the electrode stack (ETS) that have passed through the pressurizing unit (PRU).

[0066] The film recovery unit (FRU) may include a first film recovery roll (FRR1) on which the upper film (UFM) is rewound and a second film recovery roll (FRR2) on which the lower film (LFM) is rewound. The first film recovery roll (FRR1) rewinds the upper film (UFM) so that the upper film (UFM) can be detached from the electrode stack (ETS). The second film recovery roll (FRR2) rewinds the lower film (LFM) so that the lower film (LFM) can be detached from the electrode stack (ETS).

[0067] Referring back to FIG. 1, the all-solid-state battery manufacturing device (10) may include a cell cutting unit (CTU). The cell cutting unit (CTU) may be configured to cut an electrode stack (ETS) running in a lengthwise direction in a widthwise direction. For example, an all-solid-state battery may be manufactured by cutting an electrode stack (ETS) running in a first direction (D1) in a second direction (D2) intersecting the first direction (D1). Specifically, an all-solid-state unit cell (UCL) may be manufactured. Hereinafter, in the present specification, “unit cell (UCL)” is used with the same meaning as “the above-described all-solid-state unit cell (UCL).”

[0068] Referring back to FIG. 1, the all-solid-state battery manufacturing device (10) may further include a cell transport unit (TRU) and a magazine unit (MAU).

[0069] 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).

[0070] A cell transfer unit (TRU) may be configured to transfer unit cells (UCLs) from a cell 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.

[0071] 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).

[0072] Referring back to FIG. 1, the all-solid-state battery manufacturing device (10) may further include a gasket supply unit (GSU). The gasket supply unit (GSU) may be configured to provide gaskets to the unit cells (UCL). By not continuously providing the second electrode sheet (ELS2) and the gasket on the moving first electrode (ELT1), but by providing the gasket at the unit cell (UCL) stage where lamination and pressurization are completed, incorrect attachment of the gasket can be prevented and process efficiency can be improved.

[0073] In one embodiment, a gasket supply unit (GSU) may provide a gasket to a unit cell (UCL). The gasket may be laminated on a first electrode sheet formed by cutting a first electrode (ELT1). The gasket may have a shape that surrounds a side surface of a second electrode sheet. The gasket may compensate for the area difference between the first electrode sheet and the second electrode sheet. The gasket may prevent damage to the unit cell (UCL) during transport. In addition, the gasket may prevent short circuits due to lithium precipitation during charging and discharging, and may prevent deformation of the cell. The specific structure of the gasket (GSK) will be described later.

[0074]

[0075] All-solid-state battery manufacturing method (S10)

[0076] Figure 3 is a flowchart for explaining a method for manufacturing an all-solid-state battery according to embodiments of the present invention. Figures 4a, 4b, 4c, 5a, 5b, 6a, 6b, and 7 to 11 are conceptual diagrams for explaining a method for manufacturing an all-solid-state battery according to embodiments of the present invention.

[0077] Referring to FIG. 3, the all-solid-state battery manufacturing method (S10) may include an electrode supply process (S100); a second electrode cutting process (S200); a second electrode sheet transfer process (S300); a film supply process (S400); a pressurizing process (S500), and a cell cutting process (S600).

[0078] Referring to FIG. 4A, the electrode supply process (S100) may include unwinding and driving a wound first electrode (ELT1); and unwinding and driving a wound second electrode (ELT2). In one embodiment, each of the first electrode (ELT1) and the second electrode (ELT2) may drive in a first direction (D1).

[0079] In one embodiment, the first electrode (ELT1) may be wound on the first electrode supply roll (ESR1) described with reference to Fig. 1. The second electrode (ELT2) may be wound on the second electrode 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 (ESU) described with reference to Fig. 1.

[0080] Fig. 4b is a plan view illustrating a first electrode (ELT1) according to one embodiment. Fig. 4c is a plan view illustrating a second electrode (ELT2) according to one embodiment.

[0081] Referring to FIG. 4B, the first electrode (ELT1) may be notched. Specifically, the first electrode (ELT1) extending in the longitudinal direction may include a plurality of first electrode tabs (TAR1). The plurality of first electrode tabs (TAR1) may be arranged to be spaced apart from each other in the longitudinal direction. The plurality of first electrode tabs (TAR1) may protrude in the width direction. In one embodiment, the length direction may be a first direction (D1), and the width direction may be a second direction (D2).

[0082] Referring to FIG. 4C, the second electrode (ELT2) may be notched. Specifically, the second electrode (ELT2) extending in the longitudinal direction may include a plurality of second electrode tabs (TAR2). The plurality of second electrode tabs (TAR2) may be arranged to be spaced apart from each other in the longitudinal direction. The plurality of second electrode tabs (TAR2) may protrude in the width direction. In one embodiment, the length direction may be the first direction (D1), and the width direction may be the second direction (D2).

[0083] Referring to FIGS. 4b and 4c, the first electrode tabs (TAR1) and the second electrode tabs (TAR2) may protrude in opposite directions. For example, the first electrode tabs (TAR1) may protrude in a direction opposite to the second direction (D2), and the second electrode tabs (TAR2) may protrude in the second direction (D2).

[0084] Fig. 5a is a cross-sectional view for explaining the second electrode cutting process (S200). Fig. 5b is a plan view for explaining the second electrode cutting process (S200).

[0085] Referring to FIG. 3 and FIG. 5a, the second electrode cutting process (S200) may include cutting the running second electrode (ELT2) to form a second electrode sheet (ELS2).

[0086] In one embodiment, the second electrode cutting process (S200) may be performed by a moving cutting unit (MCU) described with reference to FIG. 1.

[0087] Specifically, referring to FIGS. 5A and 5B, the vertical drive unit (HDP) of the moving cutting unit (MCU) can vertically move the upper surface (UBL) of the moving cutter (MOC) and the upper grip (UGR) of the gripper (GRP). The vertical drive unit (HDP) can lower the upper surface (UBL), thereby cutting the second electrode (ELT2) to form the second electrode sheet (ELS2). In addition, the vertical drive unit (HDP) can lower the upper grip (UGR) to allow the gripper (GRP) to grip the second electrode sheet (ELS2).

[0088] The second electrode sheet transfer process (S300) may include transferring the second electrode sheet (ELS2) onto the first electrode (ELT2). In one embodiment, the second electrode sheet transfer process (S300) may be performed by a moving cutting unit (MCU) described with reference to FIG. 1.

[0089] The horizontal driving part (HDP) of the moving cutting unit (MCU) can move the moving cutter (MOC) and the gripper (GRP) in the horizontal direction by moving the vertical frame (VFR) in the horizontal direction. For example, referring to FIG. 6A, the horizontal driving part (HDP) can reciprocate the moving cutter (MOC) and the gripper (GRP) in the first direction (D1) and the opposite direction. Through this, the gripper (GRP) holding the second electrode sheet (ELS2) can move horizontally to transfer and align the second electrode sheet (ELS2) onto the upper surface of the first electrode (ELT1) moving in the first direction (D1).

[0090] For example, the gripper (GRP) can align the second electrode sheet (ELS2) on the upper surface of the first electrode (ELT1) and then directly laminate the second electrode sheet (ELS2) on the first electrode (ELT1). As another example, the gripper (GRP) can transfer the second electrode sheet (ELS2) to the nip roll (NIP) so that the second electrode sheet (ELS2) is aligned on the upper surface of the first electrode (ELT1). The electrode sheet (ELS2) can be transferred to the nip roll (NIP) at a speed at which the moving first electrode (ELT1) passes through the nip roll (NIP). Through this, the second electrode sheet (ELS2) can be laminated and adhered to the first electrode (ELT1).

[0091] After the second electrode sheet (ELS2) is laminated on the upper surface of the first electrode (ELT1), the horizontal drive unit (HDP) and the vertical drive unit (VDP) can move the moving cutter (MOC) and the gripper (GRP) vertically or horizontally so that they return to their original positions.

[0092] Figure 6b is a plan view illustrating a plurality of second electrode sheets (ELS2) mounted on a first electrode (ELT1).

[0093] Referring to FIG. 6b, by repeating the above operations, second electrode sheets (ELS2) can be spaced apart from each other at a predetermined interval and placed on the first electrode (ELT1) that is moving. In one embodiment, a plurality of second electrode sheets (ELS2) can be spaced apart from each other in the first direction (D1) and placed on the first electrode (ELT1) that is moving in the first direction (D1). As a result, the area of ​​the first electrode sheet (ELS1) of the all-solid-state unit cell (UCL) manufactured in the cell cutting process (S600) described below becomes larger than the area of ​​the second electrode sheet (ELS2).

[0094] In one embodiment, the second electrode sheet transfer process (S300) may include measuring the positions or spacings of a plurality of first electrode tabs (TAR1) of a first electrode (ELT1); and stacking a second electrode sheet (ELS2) on the first electrode (ELT1) based on the positions or spacings. After measuring the positions or spacings of the plurality of first electrode tabs (TAR1) of the first electrode (ELT1), the second electrode sheet (ELS2) may be aligned on the first electrode (ELT1) based on the positions or spacings of the first electrode tabs (TAR1). In other words, the second electrode sheet (ELS2) may be placed on the first electrode (ELT1) using the positions or spacings of the first electrode tabs (TAR1) as reference points. For example, referring to FIG. 6b, the second electrode sheet (ELS2) may be placed on the first electrode (ELT1) at a position where the first electrode tab (TAR1) of the first electrode (ELT1) and the second electrode tab (TAR2) of the second electrode sheet (ELS2) are aligned in the width direction. In one embodiment, the width direction may be a second direction (D2) intersecting the first direction (D1). The first electrode tab (TAR1) and the second electrode tab (TAR2) may protrude in opposite directions. For example, the first electrode tab (TAR1) may protrude in a direction opposite to the second direction (D2), and the second electrode tab (TAR2) may protrude in the second direction (D2).

[0095] In one embodiment, measuring the positions or spacings of the first electrode tabs (TAR1) can be performed by the sensing unit (ADU) described with reference to FIG. 1.

[0096] Referring again to FIGS. 3 and 6A and 7, the film supply process (S400) may include providing an upper film (UFM) on the upper surface of the running second electrode sheet (ELS2). The film supply process (S400) may further include providing a lower film (LFM) on the lower surface of the running first electrode sheet (ELT1).

[0097] In one embodiment, each of the upper film (UFM) and the lower film (LFM) may have relasing properties. For example, each of the upper film (UFM) and the lower film (LFM) may have relasing properties such that they can be detached from the object. In one embodiment, each of the upper film (UFM) and the lower film (LFM) may include at least one selected from the group consisting of polyethylene terephthalate, polypropylene, polymethylpentene, and copolymers thereof.

[0098] The upper film (UFM) serves to protect the first electrode (ELT1) and the second electrode sheet (ELS2), and at the same time, protects the alignment of the second electrode sheet (ELS2) mounted on the first electrode (ELT1) from being disturbed. The lower film (LFM) serves to protect the first electrode (ELT1) and the second electrode sheet (ELS2).

[0099] Referring to FIGS. 3 and 8, the pressurizing process (S500) may include pressurizing a first electrode (ELT1) that runs and a second electrode sheet (ELS2) on the first electrode (ELT1). In one embodiment, the pressurizing may be line pressing with a first pressure.

[0100] Through the pressurization process (S500), an electrode laminate (ETS) in which a first electrode (ELT1) and a second electrode sheet (ELS2) are bonded can be formed. The electrode laminate (ETS) can be continuously driven.

[0101] In one embodiment, the pressurization process (S500) may be accompanied by heating. Through pressurization and heating, the interface between the first electrode (ELT1) and the second electrode sheet (ELS2) may be activated.

[0102] In one embodiment, the pressurization process (S500) may be performed by a pressurization unit (PRU) as described with reference to FIG. 1.

[0103] Referring to FIG. 9, the upper film (UFM) and the lower film (LFM) can be recovered after the pressurization process (S500). In one embodiment, the recovery of the upper film (UFM) and the lower film (LFM) can be performed by the film recovery unit (FRU) described with reference to FIG. 1.

[0104] Referring to FIGS. 3 and 10, the cell cutting process (S600) may include cutting the electrode stack (ETS) that runs in the longitudinal direction at predetermined intervals. In one embodiment, the cell cutting process (S600) may be cutting the electrode stack (ETS) that runs in the longitudinal direction in the width direction. For example, the longitudinal direction may be a first direction (D1), and the width direction may be 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.

[0105] In one embodiment, the cell cutting process (S600) may be performed by a cell cutting unit (CTU) described with reference to FIG. 1.

[0106] Referring again to FIG. 10, the all-solid-state unit cell (UCL) to be manufactured may include a first electrode sheet (ELS1) and a second electrode sheet (ELS2) on the first electrode sheet (ELS1). The first electrode sheet (ELS1) is formed by cutting the first electrode (ELT1), and the second electrode sheet (ELS2) is formed by cutting the second electrode (ELT2).

[0107] In one embodiment, the length of the first electrode sheet (ELS1) in the first direction (D1) may be greater than the length of the second electrode sheet (ELS2) in the first direction (D1). In addition, the width of the first electrode sheet (ELS1) in the second direction (D2) may be greater than the width of the second electrode sheet (ELS2) in the second direction (D2). In other words, the area of ​​the first electrode sheet (ELS1) formed by the length in the first direction (D1) and the width in the second direction (D2) may be greater than the area of ​​the second electrode sheet (ELS2).

[0108] In one embodiment, the all-solid-state battery manufacturing method (S10) may further include a gasket supply process of providing a gasket (GSK) on a first electrode sheet (ELS1) of an all-solid-state unit cell (UCL). Referring to FIG. 11, the gasket (GSK) may be laminated on an upper surface of the first electrode sheet (ELS1). The gasket (GSK) may be laminated on a portion of the upper surface of the first electrode sheet (ELS1) where the second electrode sheet (ELS2) is not present. The gasket (GSK) may have a structure capable of compensating for the area difference between the first electrode sheet and the second electrode sheet. For example, the gasket (GSK) may have a structure that wraps around a side surface of the second electrode sheet (ELS2). The gasket (GSK) may have an opening formed on one surface so as not to vertically overlap with a portion of the second electrode tab (TAR2). The specific structure of the gasket (GSK) will be described later.

[0109] 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).

[0110] 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.

[0111] 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.

[0112] 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.

[0113] 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.

[0114] Forming the above positive electrode laminate and negative electrode laminate may include a pressing process using a roll press.

[0115] 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.

[0116] 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.

[0117] 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.

[0118] 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.

[0119] Each of the manufactured positive electrode laminate and negative electrode laminate can be wound.

[0120] 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 an elastic pad and the all-solid-state bi-cell or the all-solid-state unit cell (UCL). An elastic pad may be provided on each of the lowermost and uppermost surfaces of the all-solid-state stack cell.

[0121] 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.

[0122]

[0123] All-solid-state batteries

[0124] Fig. 12a is a plan view of an all-solid-state battery according to embodiments of the present invention. Fig. 12b is a cross-sectional view taken along line AA' of Fig. 12a.

[0125] Referring to FIGS. 12A and 12B, 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 cell 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 moving cutting unit (MCU).

[0126] 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).

[0127] Referring again to FIG. 12A, 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).

[0128] In one embodiment, the first electrode tab (TAR1) and the second electrode tab (TAR2) may protrude in opposite directions. For example, the first electrode tab (TAR1) may protrude in the b direction (D2b) of the second direction (D2), and the second electrode tab (TAR2) may protrude in the a direction (D2a) of the second direction (D2).

[0129] A portion of the second electrode tab (TAR2) may be positioned on the first electrode (ELT1). In other words, a portion of the second electrode tab (TAR2) may vertically overlap the first electrode (ELT1).

[0130] Referring again to FIG. 12A, 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 may be greater than L2.

[0131] 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.

[0132] For example, the unit cell (UCL) may be manufactured using the above-described all-solid-state battery manufacturing device (10) or manufacturing method (S10).

[0133] Referring to FIG. 13, in one embodiment, the all-solid-state unit cell (UCL) may further include a gasket (GSK) on the first electrode sheet (ELS1). The gasket (GSK) may be placed on a portion of the upper surface of the first electrode sheet (ELS1) where the second electrode sheet (ELS2) is not present. Specifically, the gasket (GSK) may be placed on a portion of the second electrode sheet (ELS2) excluding the second electrode tab (TAR2).

[0134] In one embodiment, the thickness of the gasket (GSK) in the third direction (D3) may be less than or equal to the thickness of the second electrode sheet (ELS2) in the third direction (D3).

[0135] Fig. 13 is a plan view illustrating a gasket (GSK). Referring to Fig. 13, the gasket (GSK) may include an opening (OPP) formed on one surface. The second electrode tab (TAR2) of the second electrode sheet (ELS2) described above protrudes through the opening (OPP), and thus, the gasket (GSK) and the second electrode sheet (ELS2) may not vertically overlap.

[0136] Referring again to FIG. 12b, 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.

[0137] 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.

[0138] Meanwhile, unlike as illustrated in FIG. 12b, 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).

[0139] 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.

[0140] 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.

[0141] 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.

[0142] 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.

[0143] 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.

[0144] 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.

[0145] 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).

[0146] 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.

[0147] 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.

[0148] 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.

[0149] 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.

[0150] 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.

[0151] 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.

[0152] 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 70 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.

[0153] 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. If 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). If 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.

[0154] 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.

[0155] 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.

[0156] 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.

[0157] 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.

[0158] 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).

[0159] 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.

[0160] 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.

[0161] 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).

[0162] 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.

[0163] 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).

[0164] 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.

[0165] 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.

[0166] 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.

[0167] 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.

[0168] 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.

[0169] 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).

[0170] 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).

[0171] 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).

[0172] 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.

[0173] 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.

[0174] 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.

[0175] 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 or all-solid-state unit cells. 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 bi-cells and elastic pads are alternately stacked. For example, the all-solid-state stack cell may have a structure in which elastic pads, bi-cells, elastic pads, bi-cells, and elastic pads are stacked in that order.

[0176] 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 patent 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 electrode supply roll on which a first electrode is wound and a second electrode supply roll on which a second electrode is wound; A moving cutting unit configured to cut the second electrode while driving to form a second electrode sheet and transfer the second electrode sheet onto the first electrode while driving; A pressing unit configured to laminate the first electrode and the second electrode sheet to each other to form an electrode laminate; and An all-solid-state battery manufacturing device comprising a cell cutting unit configured to cut the electrode laminate at predetermined intervals to form a unit cell.

2. In paragraph 1, Including more sensing units, The first electrode includes a plurality of first electrode tabs, and the second electrode sheet includes a second electrode tab. An all-solid-state battery manufacturing device, wherein the sensing unit is configured to measure the position or spacing of the plurality of first electrode tabs.

3. In paragraph 2, 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, The above moving cutting unit: A moving cutter configured to cut the second electrode to form a second electrode sheet; A gripper configured to align the second electrode sheet onto the upper surface of the first electrode; and An all-solid-state battery manufacturing device comprising a driving unit configured to move the moving cutter and gripper horizontally or vertically.

5. In paragraph 1, The plurality of first electrode tabs are arranged spaced apart from each other in the first direction and protrude in a second direction intersecting the first direction, An all-solid-state battery manufacturing device, wherein the second electrode tab protrudes in a direction opposite to the second direction.

6. In paragraph 1, The above pressurizing unit includes a pressurizing roller, An all-solid-state battery manufacturing device, wherein the rotation speed of the pressure roller is synchronized with the speed at which the moving cutting unit transfers the second electrode sheet onto the first electrode.

7. In paragraph 1, Further comprising a film supply unit configured to provide an upper film on the second electrode sheet, An all-solid-state battery manufacturing device, wherein the upper film maintains the alignment of the second electrode sheet positioned on the first electrode.

8. In paragraph 1, An all-solid-state battery manufacturing device further comprising a gasket supply unit configured to provide a gasket to the unit cell.

9. 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.

10. Unwinding the wound first and second electrodes and driving them in the first direction; Cutting the second electrode that runs above to form a second electrode sheet; Transferring the second electrode sheet onto the driving first electrode, Forming an electrode laminate by pressing the first electrode and the second electrode sheet on the first electrode with a first pressure; and A method for manufacturing an all-solid-state battery, comprising cutting the electrode laminate at predetermined intervals to manufacture a unit cell.

11. In paragraph 10, The first electrode includes a plurality of first electrode tabs, and the second electrode sheet includes a second electrode tab. Transferring the above second electrode sheet: Measuring the position or spacing of the plurality of first electrode tabs; and A method for manufacturing an all-solid-state battery, comprising aligning the second electrode sheet on the first electrode based on the position or the gap.

12. In paragraph 10, Cutting the above second electrode is performed by a moving cutting unit, The above moving cutting unit: A moving cutter that cuts the second electrode to form a second electrode sheet; A gripper for transferring the second electrode sheet onto the upper surface of the first electrode; and A method for manufacturing an all-solid-state battery, comprising a driving unit that moves the moving cutter and gripper horizontally or vertically.

13. In paragraph 11, Laminating the second electrode sheet on the first electrode comprises: A method for manufacturing an all-solid-state battery, wherein the second electrode sheet is laminated in a second direction intersecting the first direction so that the first electrode tab and the second electrode tab are aligned.

14. In paragraph 11, The plurality of first electrode tabs are arranged spaced apart from each other in the first direction and protrude in a second direction intersecting the first direction, A method for manufacturing an all-solid-state battery, wherein the second electrode tab protrudes in a direction opposite to the second direction.

15. In paragraph 10, Further comprising providing an upper film on the second electrode sheet, A method for manufacturing an all-solid-state battery, wherein the upper film has a detachable release property from the second electrode sheet.

16. In paragraph 10. Further comprising laminating a gasket on the first electrode sheet of the above unit cell, The above first electrode sheet is formed by cutting the first electrode, The length of the first electrode sheet in the first direction is greater than 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, A method for manufacturing an all-solid-state battery, wherein the gasket is laminated on a portion of the upper surface of the first electrode sheet exposed by the second electrode sheet, thereby compensating for the difference in area between the first electrode sheet and the second electrode sheet.

17. 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.

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 greater than 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 a direction opposite to the second direction, The second electrode sheet includes a second electrode tab protruding in 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 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, Further comprising a gasket laminated on the first electrode sheet, The above gasket surrounds the side of the second electrode sheet, An all-solid-state battery, wherein the gasket includes an opening configured to protrude the second electrode tab.

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