KR100439350B1 - Method for Continuously Making Band Type Lithium Metal Anode, Rechargeable Lithium Polymer Battery and Method for Making the Same Using the Lithium Metal Anode - Google Patents

Abstract

In the present invention, the basic assembly process in the glove box is simple in a continuous process so that the cutting and packaging process can be performed in the air when mass production is applied, and thus the productivity is high, and the cross-sectional area of the anode is doubled to double the capacity of the battery. The present invention relates to a lithium polymer secondary battery having a structure that can be improved and a method of manufacturing the same.

The secondary battery of the present invention is disposed to face the first and second negative electrodes formed of lithium metal on both sides using a conductive foil as a negative electrode current collector, respectively, and is not oxidized at high temperature sintering. The first and second positive electrodes formed by using a lithium transition metal oxide as a positive electrode material in a mesh-type positive electrode current collector, and the charge and discharge at the same time while separating between the first and second positive electrode and the first and second negative electrode It is characterized by consisting of a polymer electrolyte capable of the movement of lithium ions.

The secondary battery can be manufactured in the glove box in the glove box without the use of the evaporator continuously by the plating method, the basic assembly process is carried out in a continuous process method using this, and the cutting and packaging process in the air is made Productivity becomes high.

Description

Method for Continuously Making Band Type Lithium Metal Anode, Rechargeable Lithium Polymer Battery and Method for Making the Same Using the Lithium Metal Anode }

The present invention relates to a lithium polymer secondary battery and a method for manufacturing the same, and in particular, the basic assembly process in a glove box is simply performed in a continuous process so that cutting and packaging processes can be performed in the air during mass production. The present invention relates to a lithium polymer secondary battery having a structure capable of increasing productivity and doubling the cross-sectional area of a positive electrode and doubling the capacity of the battery, and a manufacturing method thereof.

Secondary batteries have been widely used in portable electronic devices such as mobile communication terminals since they can be manufactured in a lightweight, thin, rechargeable form. Lithium-ion batteries (LIBs), which improve the shortcomings of nickel-cadmium batteries and nickel-hydrogen batteries, have contributed to the popularization of mobile phones because the energy density is about 2 times by volume and 3 times by weight compared to nickel cadmium batteries. .

The lithium ion battery uses lithium cobalt or lithium manganese composite oxide for the positive electrode, graphite for the negative electrode, and a maintenance electrolyte for the electrolyte, but does not use metal lithium for the negative electrode in consideration of safety during charge and discharge.

On the contrary, lithium metal batteries (LMBs) using lithium aluminum (LiAl) alloys or lithium titanium composite oxides as negative electrodes require a special structure for safety even more than lithium ion batteries.

That is, the lithium secondary battery described above uses lithium as a positive electrode and / or a negative electrode. Lithium is the lightest metal among the metals, has excellent electron retention capability, has an energy density of at least 5 times that of a lead acid battery, and at least 3 times that of an alkaline battery. One cell can deliver 3.0V of drive power, which has advantages in miniaturization and stability.

However, lithium ions, due to their aggressive nature, destroy internal materials or cases, or react violently with oxygen or water in the air to produce hydrogen, causing hydrogen to explode or to increase internal pressure, thereby destroying the battery. Alternatively, lithium melts at a relatively low temperature, with a melting temperature of 179 ° C, which may explode if lithium melts and comes in direct contact with the cathode during a fire.

Moreover, when lithium metal is used as a negative electrode of a secondary battery, it has advantages of high energy density and low self discharge rate, but lithium metal precipitates through needle or dendrite crystal during charging to penetrate the separator. There is a problem such as low temperature stability, low energy density during high load discharge, and commercialization is not possible. Lithium ion batteries using carbon (graphite) as a negative electrode material have been commercialized.

However, commercially available Li-ion batteries employ a triple safety measure, in addition to using a carbon electrode as a negative electrode, an electronic control device to prevent overcharge and overdischarge, and a separator that turns into an insulator when the temperature rises above a dangerous temperature. It is equipped with PTC for the temperature rise and a safety vent to prevent overcharge.

Since the problem of the lithium ion battery is largely due to the use of a liquid electrolyte, a lithium ion polymer battery (LIPB), which has been replaced with a solid electrolyte made of a solid polymer material instead of the liquid electrolyte, has recently been proposed.

Lithium-ion polymer battery has no risk of leakage of electrolyte solution and can be made thinner and slimmer by using plastic's unique plasticity, and it can secure safety by simplifying the manufacturing process and without dendrite phenomenon. It is expected as a battery.

This lithium-ion polymer battery is a technology proposed by Bell Communication Research Co. (Bellcore) in the United States. The positive and negative electrodes are made of films, laminated with positive and negative current collectors, cut into unit cell sizes, and cut into unit cell sizes. The unit cell is obtained through a cell lamination process together with the prepared electrolyte. After that, plasticizer extraction and electrolyte impregnation are completed, followed by packaging and terminal assembly.

The lithium ion polymer battery structure proposed by Belcoa and others uses hard carbon or graphite without using lithium as a negative electrode, and uses Cu foil or Cu-Exmet as a negative electrode current collector and a positive electrode current collector. Al foil or Al-Exmet is used.

Moreover, in recent years, a lithium polymer battery (LPB) structure has been proposed, which allows the movement of lithium ions to a solid polymer electrolyte while employing lithium metal as a negative electrode, and has attempted mass production.

The process of manufacturing such a conventional lithium-ion polymer and lithium polymer battery, the entire process must be carried out inside the glove box of the moisture (free), and a plurality of vapor deposition for Li cathode deposition on Al or Cu foil inside the glove box Since the size of the glove box depends on the overall product yield since it must be installed in the box, there is a problem that continuous process processing is impossible.

In addition, due to the difficulty in manufacturing and the development of a suitable solid polymer electrolyte due to the use of lithium metal, its production method has yet to be proposed which can be competitive in yield and yield during mass production while maintaining ultra-thin thickness. Can not do it.

Therefore, the present invention has been made in view of the problems of the prior art, the object of which is that the basic assembly process in the glove box can be simply made in a continuous process so that the cutting and packaging process in the air can be made in mass production application The present invention provides a lithium polymer secondary battery having a high productivity and having a structure capable of doubling the charge / discharge rate by doubling the cross-sectional area of the positive electrode, and a manufacturing method thereof.

Another object of the present invention is to provide a method for manufacturing a negative electrode sheet sheet for a lithium polymer secondary battery which can manufacture a continuous negative plate sheet by a plating method so that the assembly process can be continuously performed in the glove box.

1 is a schematic plan view of a lithium polymer secondary battery obtained according to the manufacturing method of the present invention,

2 is a cross-sectional view taken along the X-X line in a state in which the exterior material is removed from FIG.

3A to 3C are a manufacturing process diagram, a heat treatment process diagram, and a plan view of a manufactured cathode plate sheet for use in manufacturing a lithium polymer secondary battery according to the present invention;

4 is a process flow diagram illustrating a continuous manufacturing process of a lithium polymer secondary battery according to the present invention;

5A and 5B are plan views of a negative electrode sheet used in the production of a lithium polymer secondary battery according to the present invention, and a sectional view taken along the line Y-Y of FIG. 5A,

6 is a plan view of a cell battery sheet including a plurality of unit cells basically assembled in a glove box;

7 is an explanatory diagram for explaining a cell cutting / packaging process performed outside the glove box.

* Explanation of Signs of Major Parts of Drawings *

One ; Lithium polymer secondary battery 1a-1n; Unit cell

2 ; Negative electrode current collectors 2a, 2b; cathode

4 ; Polymer electrolyte 6; Anode current collector

6a, 6b; Anode 8; Exterior material

10; Cell battery sheet 10a-10n; Cell area

11; Outer crimp sections 12a, 12b; Crimp

13; Cutting line 20; Negative plate

21,60a, 60b; Base material 21a, 601a; Protrusion

22a, 22b; LiAl alloy layer 23a, 23b; Li metal layer

24; Molten Li metal 25,26; Plating bath

31a-38b, 65a, 65b; Guide rollers 39a and 39b; Dipping Device

40; Polymer electrolyte sheet 60; Anodized sheet

61a-61n; Anode 62; Anode Material Slurry

63a, 63b; Hopper 64; Nozzle

66a, 66b; Compression roller 67; heater

80; Exterior material 100; Glove box

In order to achieve the above object, the present invention uses a conductive foil as a negative electrode current collector, the first and second negative electrodes formed of lithium metal on both sides, respectively, facing the first and second negative electrode, respectively, at high temperature sintering The first and second positive electrodes formed by using a lithium transition metal oxide as a positive electrode material in a mesh-type positive electrode current collector which is not oxidized at the same time are separated from the first and second positive electrodes and the first and second negative electrodes. Provided is a lithium polymer secondary battery comprising a polymer electrolyte capable of moving lithium ions during charging / discharging.

The lithium transition metal oxide is made of any one of lithium manganese oxide (LiMn ₂ O ₄ ) and lithium cobalt oxide (LiCoO ₂ ), the positive electrode current collector is made of any one of stainless steel and platinum (Pt), the negative electrode current collector Made of either aluminum or copper foil.

In addition, when the negative electrode current collector is an aluminum foil, it is preferable to further include a LiAl alloy layer for improving the wettability to lithium metal between the aluminum foil and the lithium metal layer.

In the first method of manufacturing the lithium polymer secondary battery, the first and second negative electrode layers in which lithium metal is plated on both sides of the upper and lower surfaces by using a conductive foil as a substrate for negative electrode current collector in an oxygen-free atmosphere glove box are provided. Preparing a band-type negative electrode sheet having a band; and preparing a roll-shaped band-shaped first and second polymer electrolyte sheets by impregnating and drying a polymer electrolyte solution into a separator, respectively, and containing lithium transition metal oxide as a main component. Preparing a roll-shaped band-shaped first and second cathode plate sheets in which a plurality of anodes are formed by sintering a slurry of a cathode material in a thin film form at predetermined intervals on a substrate for cathode current collector; The first polymer electrolyte sheet and the first positive electrode plate sheet are sequentially stacked on the upper surface of the negative electrode sheet in the box, and the second polymer electrolyte is deposited on the lower surface. And sequentially assembling the band-shaped cell battery sheet including the plurality of cell regions by sequentially stacking the sheet and the second positive electrode plate sheet, and pressing and sealing the open part of the cell battery sheet after the assembled cell battery sheet is brought into close contact. And removing the sealed cell battery sheet outside the glove box and separating and packaging a plurality of cell regions into unit cells in the air.

The second method of manufacturing the lithium polymer secondary battery includes the first and second negative electrode layers in which lithium metal is plated on both sides of the upper and lower surfaces by using aluminum foil as a substrate for negative electrode current collector in an oxygen-free atmosphere. Preparing a band-type negative plate sheet having a, and the separation between the positive electrode and the negative electrode, and at the same time made of a material that can move the lithium ion during charging / discharging, the roll-shaped band-shaped first and second polymer electrolyte sheet The first and second roll-shaped band-shaped first and second rolls in which a cathode layer is formed by sintering a cathode material slurry containing lithium transition metal oxide as a main component, respectively, in a thin film form on a substrate for a cathode current collector. Preparing a positive electrode sheet, and sequentially laminating a first polymer electrolyte sheet and a first positive electrode sheet on the upper surface of the negative electrode sheet in the glove box; Sequentially stacking the second polymer electrolyte sheet and the second positive electrode sheet on the lower surface, and assembling a band-shaped cell battery sheet including a plurality of cell regions; And dividing the cell region into unit cells.

The third method of manufacturing the lithium polymer secondary battery includes a first and a second negative electrode layer in which lithium metal is plated on both sides of the upper and lower sides by using aluminum foil as a substrate for negative electrode current collector in an oxygen-free atmosphere. Preparing a band-type negative plate sheet having a, and the separation between the positive electrode and the negative electrode, and at the same time made of a material that can move the lithium ion during charging / discharging, the roll-shaped band-shaped first and second polymer electrolyte sheet The first and second roll-shaped band-shaped first and second rolls in which a cathode layer is formed by sintering a cathode material slurry containing lithium transition metal oxide as a main component, respectively, in a thin film form on a substrate for a cathode current collector. Preparing a positive electrode plate sheet, and preparing a roll-shaped band-shaped first and second exterior sheet sheet, and the upper surface of the negative electrode sheet sheet in the glove box A first polymer electrolyte sheet, a first positive electrode plate sheet and a first outer material sheet is sequentially laminated, and the second polymer electrolyte sheet, a second positive electrode plate sheet and a second outer material sheet is sequentially stacked on the lower surface to include a plurality of cell regions And assembling the band-shaped cell battery sheet, and packaging the separated cell areas by separating the unit cell cells into unit cells.

In the separating and packaging of the unit cell, the cell battery sheet assembled with the close contact is compressed and sealed by pressing the sealed part of the cell battery sheet, and then taken out into or out of the glove box to separate and package a plurality of cell regions into unit cells in the air. It consists of steps.

In the preparing of the band-type negative plate, the first and second LiAl for improving wettability of lithium metal on both sides of the upper and lower sides by using a band-type aluminum foil as a substrate for negative electrode current collector in an oxygen-free atmosphere glove box. Continuously forming an alloy layer, and a substrate having first and second LiAl alloy layers formed on both surfaces thereof continuously passing a plating bath of molten lithium metal to form lithium on the surface of the first and second LiAl alloy layers. And depositing a metal layer to continuously form the first and second cathode layers.

Furthermore, the preparing of the roll-shaped band-shaped first and second positive plate sheets may be performed by extruding a positive electrode material slurry containing lithium transition metal oxide as a main component while transferring the substrate for the positive electrode current collector in the form of a mesh, respectively. Forming a thin film, winding up the cathode material slurry formed on the substrate by heating and drying the roll, and sintering the dried roll substrate in an oxygen atmosphere to form an anode layer. It is preferable.

In this case, the sintering of the cathode material slurry is preferably heat-treated in an oxygen atmosphere between 500 ℃ to 600 ℃.

When the base material for the positive electrode current collector is assembled into a cell battery sheet, a plurality of first protruding regions protruding by the self-aligning method to the outside of the cell area is formed for each cell area, and the base material for the negative electrode current collector is a cell. When assembled with a battery sheet, a plurality of second protrusions protruding outward from the cell area by self-alignment and positioned adjacent to the first protrusion area are formed for each cell area, and the plurality of first protrusions are formed. It is preferable that the positive electrode terminals are connected to the regions after being divided into unit cells, and the negative electrode terminals are respectively connected to the plurality of second protruding regions after being divided into unit cells.

As described above, in the lithium polymer secondary battery (LPB) according to the present invention, a pair of the first and second positive electrodes and the first and second negative electrodes react with each other in a single cell, so that the reaction surface area of the positive electrode has a conventional structure. As compared with the increase of 2 times, the battery capacity can be increased more than 2 times without doubling the thickness of the entire battery.

In addition, the secondary battery uses a negative electrode sheet continuously manufactured in a glove box, so that the assembling process is simply performed in a continuous process manner, and the cutting and packaging processes can be performed in the air, thereby increasing productivity and yield.

(Example)

Hereinafter, the present invention will be described in more detail with reference to the accompanying drawings.

FIG. 1 is a schematic plan view of a lithium polymer secondary battery obtained according to the manufacturing method of the present invention, and FIG. 2 is a cross-sectional view taken along the line X-X of FIG.

1 and 2, a lithium polymer secondary battery (LPB) 1 obtained according to a continuous process of the present invention described below has an anode including a mesh made of stainless steel, aluminum, or platinum (Pt) on the outside thereof. The first and second positive electrodes 6a and 6b formed by using the whole 6 and, for example, aluminum (Al) or copper (Cu) foil are formed on both sides using the negative electrode current collector 2, and Separating the first and second cathodes 2a and 2b disposed between the first and second anodes 6a and 6b, and the first and second anodes 6a and 6b and the cathodes 2a and 2b, respectively. At the same time, the solid polymer electrolyte is composed of the first and second polymer electrolytes 4a and 4b impregnated in the separator to enable the movement of lithium ions at the time of charge / discharge. The exterior material 80 is covered.

In the lithium polymer secondary battery 1, the positive electrodes 6a and 6b use, for example, lithium transition metal oxides such as lithium manganese oxide (LiMn ₂ O ₄ ), lithium cobalt oxide (LiCoO ₂ ), and the like as the positive electrode material. The cathodes 2a and 2b are made of, for example, lithium (Li) metal, and the polymer electrolyte 4 is impregnated / dried with a known electrolyte solution using a porous substrate as a separator.

The lithium polymer secondary battery (LPB) 1 according to the present invention as described above has the first and second negative electrodes 2a and 2b and the first and second positive electrodes formed on the upper and lower portions of the negative electrode current collector 2. 6a) reacts with each other, and as the reaction surface area of the positive electrode reacting with the negative electrode doubles as compared with the conventional structure, the capacity of the battery can be doubled.

Hereinafter, a method of continuously manufacturing a lithium polymer secondary battery having the above structure will be described in detail with reference to FIGS. 3 to 7.

First, Figure 3a is a process chart for explaining the manufacturing method of the band-shaped positive electrode sheet required for manufacturing a lithium polymer secondary battery according to the present invention in a continuous process method.

In the present invention, the band-shaped positive plate sheet 60 used to continuously manufacture the lithium polymer secondary battery has a plurality of positive electrodes 61a-having a constant spacing d and a constant area on the mesh-shaped substrate 60a as shown in FIG. 3C. 61n) is formed.

The distance d between the left and right adjacent anodes 61a-61n is between the pair of crimping portions 12a and the crimping portion 12b required to seal the respective cells 1a-1n as shown in FIG. 7. It is set to the length including the formed cutting | disconnection area | regions 13a-13n.

The band-shaped positive plate sheet 60 first prepares a known positive electrode material containing lithium manganese oxide (LiMn ₂ O ₄ ) or lithium cobalt oxide (LiCoO ₂ ) as a main component in the form of a slurry. Thereafter, the prepared anode material slurry 62 is guided through a pair of guide rollers 65a and 65b by a continuous extrusion coating method, and a pair of hoppers 63a and 63b to a pair of mesh-shaped substrates 60a and 60b. It is sprayed periodically through the nozzle 64 of and apply | coated in a predetermined pattern, respectively, as shown in FIG. 3C.

Subsequently, a drying step of drying the coated positive electrode material slurry after application of the positive electrode material slurry 62 at a temperature of about 200 ° C. by the heater 67, and a pressing step of slimming using a pair of pressing rollers 66a and 66b. It is wound into a roll form in the winder through.

The process may be of a structure or a single structure for obtaining two positive electrode sheets 60 at the same time, the extrusion of the positive electrode material slurry 62 may be continuously ejected to form a whole.

In this case, the substrates 60a and 60b serve as the positive electrode current collector 6 when they are assembled and then divided into unit cells. Therefore, preferably, the protruding region 601a is extended to one side of the substrates 60a and 60b so that the protruding region 601a is formed on the negative electrode sheet sheet 20 as shown in FIG. It may be preset to protrude in a self-aligning manner to the outside of the). The positive electrode terminal is connected to the protruding region 601a during the packaging process.

Thereafter, when the roll-shaped anode plate sheet 60 in which the cathode material sludge is pre-dried is heat-treated in an oxygen atmosphere between 500 ° C. and 600 ° C. as shown in FIG. 3B, the coated cathode material slurry is sintered to obtain a plurality of anodes 61a-61n. The formed band-shaped positive plate sheet 60 is obtained.

The material usable as the substrate 60a is a material that can withstand oxidation without losing electrical properties during heat treatment of the anode material slurry in an oxygen atmosphere between 500 ° C. and 600 ° C., for example, stainless steel and platinum (Pt). Or aluminum. In addition, using a mesh form as the base materials 60a and 60b is a structure for preventing the anode material oxide from being easily broken.

On the other hand, as the polymer electrolyte, it is possible to use a well-known solid polymer electrolyte, and for example, a roll-shaped band-type polymer electrolyte 40 using a hybrid gel medium formed by mixing an organic solvent and a lithium salt in a polymer matrix. Prepare (see FIG. 4).

The hybrid gel-type polymer electrolyte is a form in which an electrolyte solution in which lithium salt is dissolved in an organic solvent is impregnated in the pore portion of the polymer matrix. PAN), polymethyl methacrylate (PMMA), and polyvinylidene fluride (PVDF).

The polymer electrolyte may be one obtained by impregnating a known electrolyte solution on a paper such as a nonwoven fabric and then drying it. Of course, it is possible to use a high ionic conductivity as a fully solid polymer electrolyte.

Meanwhile, when a pair of roll-shaped band-shaped positive plate sheets 60 and 60, polymer electrolyte sheets 40 and 40, and aluminum deposition films 80 which can be used as exterior materials are obtained as described above, the glove as shown in FIG. A process of continuously assembling a cell battery sheet including a plurality of unit cells in the box 100 is performed.

In this case, first, a two-step dipping process (S1, S2) to obtain a band-shaped negative plate sheet 20 as shown in Figure 5a and 5b. The negative electrode sheet 20 has a structure in which LiAl alloy layers 22a and 22b and Li metal layers 23a and 23b are formed on the upper and lower surfaces by using aluminum foil or the like as the base material 21.

Since the LiAl alloy layers 22a and 22b have a high surface tension and poor wettability with the aluminum foil, lithium is not applied to the surface of the aluminum foil by simple dipping. Therefore, the LiAl alloy layers 22a and 22b are films for enhancing the wettability of the molten lithium metal.

First, the aluminum foil substrate 21 is set to 300 ° C. or more, which is the minimum temperature at which the LiAl alloy is formed through the guide rollers 31a, 31b, 32a, and 32b, and the first dipping apparatus 39a in which the lithium metal 24 is melted. LiAl alloy layers 22a and 22b are formed on both surfaces of the aluminum foil base material 21 while passing through the plating bath 25 of the step (S1).

Subsequently, the substrate 21 having the LiAl alloy layers 22a and 22b formed on both surfaces thereof is set to 200 ° C. or less by the guide rollers 33, 34a, 34b, 35a, and 35b, and has a second dipping apparatus in which lithium metal is melted ( Li metal layers 23a and 23b are applied to both surfaces of the LiAl alloy layers 22a and 22b while passing through the plating bath 26 of 39b) (S2).

The plating bath 26 is set to a maximum of 200 ° C. at the lowest temperature capable of maintaining lithium in the molten state because the wettability of lithium is high at the lowest possible temperature.

In this case, the substrate 21 to which the Li metal layers 23a and 23b, which serve as the negative electrode, are applied as the negative electrode current collector 2 when divided into unit cells. Therefore, preferably, the protruding region 21a is extended to one side of the base 21 so that the protruding region 21a of the bipolar plate sheet 60 as shown in FIG. It may be set in advance to protrude to the outside in a self-aligning manner. The negative electrode terminal is connected to the protruding region 21a during the packaging process. In addition, the regions 10a-10n indicated by dotted lines in FIG. 5 are used as a plurality of cell regions when assembled later as shown in FIG. 6.

Then, the negative electrode sheet 20 obtained through the above process is laminated with the polymer electrolyte sheets 40 and 40 on both sides thereof through guide rollers 36a and 36b, and then guide rollers 37a and 37b and guide rollers ( The anode plate sheets 60 and 60 and the aluminum deposition films 80 and 80 for exterior materials are sequentially laminated on both surfaces thereof through 38a and 38b.

The cell battery sheet 10 obtained through the assembling process is sequentially formed on the upper and lower portions of the negative electrode plate sheet 20, the polymer electrolyte sheets 40 and 40, the positive electrode plate sheets 60 and 60, and the aluminum deposition film 80 for the exterior material. 80) has a laminated structure.

In this case, the protruding region 601a of the positive electrode substrate 60a and the protruding region 21a of the negative electrode substrate 21 protrude outwardly in a self-aligning manner for each cell as shown in FIG. 6.

After that, the cell battery sheet 10 is subjected to a slimming process in a pressing roller, and the front end and both sides of the slim cell battery sheet 10 are sequentially pressed by a press device to form the outer press part 11, and finally the rear end part thereof. Squeeze. Therefore, the cell battery sheet 10 that has undergone the above basic assembly process is sealed to prevent air containing oxygen from invading from the outside.

After that, the cutting process is performed as shown in FIG. 7 to take out the cell battery sheet 10 sealed by the outer shell pressing unit 11 to the outside of the glove box 100 and divide the cell battery sheet into unit cells in the air.

In the cell cutting process, first, the cell battery sheet 10 including the plurality of cell regions 10a-10n is sequentially moved by a predetermined distance to the pressing / cutting apparatus, and the adjacent cell regions 10a-10n are pressed in the pressing / cutting apparatus. ) And at the same time form a pair of crimping portions 12a, 12b necessary to seal the cells 1a-1n at predetermined intervals to form a cutting area between the crimping portions 12a, 12b or The cell is cut along the cutting line 13 in the middle of the cutting area with a parallax, and the unit cell 1a positioned at the distal end is separated.

After that, after moving by the unit cell area, the above operation is repeated sequentially to separate the remaining unit cells 1b-1n. Of course, in this case, it is also possible to increase the processing efficiency by forming and cutting the predetermined number of crimping portions 12a and 12b to separate the predetermined number of cells at one time.

In this case, the pair of crimping portions 12a and 12b can be formed by attaching them without forming a cutting region in the middle thereof and cutting the boundary line by setting the cutting line 13.

The unit cell batteries 1a-1n obtained through the above process are sealed by the four-sided pressing parts 11, 11, 12a, and 12b as shown in FIGS. 1 and 7, and the exterior materials 8 and 80 have upper and lower surfaces. The positive electrode collectors 6; 60a connected to the positive electrodes 6a, 6b; 61a-61n and the negative electrode collectors 2; 21 connected to the negative electrodes 2a, 2b; 23a, 23b protrude from one side end thereof. It is.

Therefore, in the present invention, the positive electrode terminal is connected to the protruding positive electrode current collector 6 and the negative electrode terminal is connected to the negative electrode current collector 2, so that the finished product packaging can be made easier than the conventional method, and the positive electrode terminal and the negative electrode terminal There is no need for a separate process for withdrawing.

In addition, in the present invention, only the basic assembly process is simply performed in the glove box 100, and the cutting and packaging process may be performed in the air, thereby increasing the assembly productivity.

In the above-described embodiment, a structure in which the aluminum deposition films 80 and 80 which are exterior materials are integrally laminated when the cell battery sheet 10 is assembled in the glove box 100 is illustrated. It is also possible to proceed in the box 100 and the cell division and packaging process outside the glove box 100.

That is, even when the aluminum deposition films 80 and 80 do not seal the outside of the cell battery sheet 10, the cathodes 2a and 2b of the Li metal layers 23a and 23b positioned at the center portion surround a outside of the cell sheet 10. Since the sealing state is maintained by the polymer electrolytes 4a and 4b and the pair of anodes 6a and 6b; 61a to 61n, the cell division and packaging process can be performed in the air.

In this case, the negative electrode terminal and the positive electrode terminal are respectively connected to the negative electrode current collector 2 and the positive electrode current collector 6 of the unit cell separated from the outside of the glove box 100, and the outside is, for example, heat-bonded water such as epoxy resin. Gina completes the sealing packaging for the battery cell using an aluminum deposition film or the like as an exterior material.

Of course, when the outside of the cell battery sheet 10 is not sealed with the aluminum deposition films 80 and 80, the cell division and packaging processes may be performed in the glove box 100.

As described above, in the present invention, the continuous production of the band-type negative plate sheet 20 essential for continuous production (assembly) is realized by adopting a plating method. As a result, it is possible to obtain a continuous negative plate sheet in a small occupied space, so the space utilization inside the glove box 100 is very efficient.

In addition, the positive electrode sheet 60 and the polymer electrolyte sheet 40 can also be produced continuously, and the cell battery sheet 10 including a plurality of cell regions 10a-10n together with the negative electrode sheet 20 described above. It is possible to make a continuous production of.

As a result, it is possible to significantly reduce the production cost of the product and at the same time increase the production volume, thereby securing the competitiveness of the product.

As described above, in the lithium polymer secondary battery (LPB) according to the present invention, a pair of the first and second positive electrodes and the first and second negative electrodes react with each other in a single cell, so that the reaction surface area of the positive electrode has a conventional structure. As compared with the increase of 2 times, the battery capacity can be increased more than 2 times without doubling the thickness of the entire battery.

In addition, the secondary battery uses a negative electrode sheet continuously manufactured by plating in a glove box, so that the assembling process is simply performed in a continuous process method, and cutting and packaging processes can be performed in the air, thereby increasing productivity and productivity. .

The result is a savings in equipment investment for expensive glove boxes for mass production and multiple evaporators.

In the above, the present invention has been illustrated and described with reference to specific preferred embodiments, but the present invention is not limited to the above-described embodiments and is not limited to the spirit of the present invention. Various changes and modifications can be made by those who have

Claims (16)

First and second negative electrodes formed by sequentially plating LiAl alloy layers and lithium metal layers on both sides to improve wettability to lithium metal using aluminum foil as a negative electrode current collector; It is made of one of stainless steel and platinum (Pt) which are disposed to face the first and second cathodes and are not oxidized at high temperature sintering, respectively, and are formed by using a lithium transition metal oxide as a cathode material in a mesh-shaped cathode current collector. The first and second anodes, A lithium polymer secondary battery comprising a polymer electrolyte capable of moving lithium ions during charge / discharge while separating between the first and second positive electrodes and the first and second negative electrodes. delete delete Preparing a band-type negative plate sheet having first and second negative electrode layers having lithium metal plated on both upper and lower surfaces by using a conductive foil as a substrate for negative electrode current collector in an oxygen-free atmosphere box; Preparing a roll-shaped band-shaped first and second polymer electrolyte sheets by impregnating / drying the polymer electrolyte solution into the separator, respectively; Preparing a roll-shaped band-shaped first and second cathode plate sheets each having a plurality of anodes formed after forming a cathode material slurry containing lithium transition metal oxide as a main component at a predetermined interval on a substrate for a cathode current collector; In the glove box, a first polymer electrolyte sheet and a first positive electrode sheet sheet are sequentially stacked on an upper surface of the negative electrode sheet sheet, and a second polymer electrolyte sheet and a second positive electrode sheet sheet are sequentially stacked on a lower surface thereof, thereby forming a plurality of cell regions. Assembling a band-type cell battery sheet including; Contacting the assembled cell battery sheet and then pressing and sealing the opening of the cell battery sheet; The method of manufacturing a lithium polymer secondary battery comprising the step of taking out the sealed cell battery sheet outside the glove box and separating and packaging a plurality of cell regions into unit cells in the air. Preparing a band-type negative plate sheet having first and second negative electrode layers on which lithium metal is plated on both upper and lower surfaces by using aluminum foil as a substrate for negative electrode current collector in an oxygen-free atmosphere box; Preparing a roll-shaped band-shaped first and second polymer electrolyte sheets, each of which is made of a material capable of moving lithium ions during charge / discharge while separating between the positive and negative electrodes, respectively; Preparing a roll-shaped band-shaped first and second positive electrode plate sheets each having a positive electrode material slurry containing lithium transition metal oxide as a main component on a substrate for a positive electrode current collector in a mesh form; In the glove box, a first polymer electrolyte sheet and a first positive electrode sheet sheet are sequentially stacked on an upper surface of the negative electrode sheet sheet, and a second polymer electrolyte sheet and a second positive electrode sheet sheet are sequentially stacked on a lower surface thereof, thereby forming a plurality of cell regions. Assembling a band-type cell battery sheet including; The method of manufacturing a lithium polymer secondary battery, characterized in that consisting of the step of packaging the cell battery sheet is assembled to the plurality of cells separated into unit cells. Preparing a band-type negative plate sheet having first and second negative electrode layers having lithium metal plated on both upper and lower surfaces by using aluminum foil as a substrate for negative electrode current collector in an oxygen-free atmosphere box; Preparing a roll-shaped band-shaped first and second polymer electrolyte sheets, each of which is made of a material capable of moving lithium ions during charge / discharge while separating between the positive and negative electrodes, respectively; A cathode material slurry containing lithium transition metal oxide as a main component, respectively, is formed in a thin film form on a substrate of a cathode-type positive electrode current collector, and then sintered to prepare roll-shaped band-shaped first and second cathode plate sheets having an anode layer. Steps, Preparing a roll-shaped band-shaped first and second exterior sheet sheets, In the glove box, a first polymer electrolyte sheet, a first positive electrode plate sheet, and a first exterior sheet are sequentially stacked on an upper surface of the negative electrode sheet, and a second polymer electrolyte sheet, a second positive electrode sheet, and a second exterior sheet on a lower surface thereof. Sequentially assembling the band cell battery sheet including a plurality of cell regions, The method of manufacturing a lithium polymer secondary battery, characterized in that consisting of the step of packaging the cell battery sheet is assembled to the plurality of cells separated into unit cells. The method of claim 6, wherein the separating and packaging of the unit cell comprises the steps of pressing and sealing the opening of the cell battery sheet in close contact with the assembled cell battery sheet; The method of manufacturing a lithium polymer secondary battery comprising the step of taking out the sealed cell battery sheet outside the glove box and separating and packaging a plurality of cell regions into unit cells in the air. The method of any one of claims 4 to 6, wherein the preparing of the band type negative plate sheet Continuously forming first and second LiAl alloy layers for improving wettability to lithium metal on both upper and lower sides by using a band-shaped aluminum foil as a substrate for negative electrode current collector in an oxygen-free atmosphere box; First and second cathodes are formed by continuously passing a substrate having first and second LiAl alloy layers on both surfaces through a plating bath of molten lithium metal, and depositing a lithium metal layer on the surfaces of the first and second LiAl alloy layers. Method for producing a lithium polymer secondary battery, characterized in that consisting of a step of forming a layer continuously. The method according to any one of claims 4 to 6, wherein the preparing of the roll-shaped band-shaped first and second bipolar plate sheets is performed respectively. Extruding the cathode material slurry containing lithium transition metal oxide as a main component while transferring the substrate for the cathode current collector in the form of a predetermined thin film; Winding the cathode material slurry formed on the substrate by heat treatment and drying the rolls; And sintering the dried roll substrate in an oxygen atmosphere to form a positive electrode layer. The method of manufacturing a lithium polymer secondary battery according to claim 9, wherein the base for positive electrode current collector is made of one of stainless steel, platinum (Pt), and aluminum. The method of claim 9, wherein the sintering of the cathode material slurry is heat-treated in an oxygen atmosphere between 500 ° C. and 600 ° C. 11. The cell according to any one of claims 4 to 6, wherein the base for positive electrode current collector has a plurality of first protruding regions projecting out of the cell region in a self-aligned manner when assembled into a cell battery sheet. Each of the plurality of second protruding regions, which are formed by regions and protrudes in a self-aligning manner to the outside of the cell region and is positioned adjacent to the first protruding region when assembled into the cell battery sheet, is formed. Extends by the cell area of Fabrication of a lithium polymer secondary battery, characterized in that the positive terminal is connected to each of the plurality of first projection regions after being divided into unit cells, and the negative electrode terminal is connected to each of the plurality of second projection regions after being divided into unit cells. Way. The method of claim 4, wherein the dividing and packaging of the plurality of cell regions into unit cells is performed. The cell battery sheet including the plurality of cell regions is formed between the adjacent cell regions while forming the first and second crimps required to seal the cells while partitioning the adjacent cell regions. Dividing the unit cells sequentially by cutting the cutting region between the portions to separate the unit cells located at the front end portion; And connecting the negative electrode terminal and the positive electrode terminal to the negative electrode current collector and the positive electrode current collector of the divided unit cells, respectively, and packaging the package with an exterior material. The method of any one of claims 4 to 6, wherein the separating of the plurality of cell regions into unit cells is performed. The cell battery sheet including the plurality of cell regions is partitioned between adjacent cell regions, and at the same time, a crimping portion necessary to seal each cell is formed between the plurality of adjacent cell regions, and the middle portion of the crimping portion is cut. A method of manufacturing a lithium polymer secondary battery, comprising dividing a plurality of unit cells at the same time. A lithium polymer secondary battery prepared according to claim 4. In the manufacturing method of the band-type negative plate sheet used for the continuous manufacture of a lithium secondary battery, A band-type aluminum foil is used as a base material for the negative electrode current collector in an oxygen-free atmosphere box to continuously pass a plating bath of lithium metal set at a LiAl alloy formation temperature or higher to improve wettability of lithium metal on both sides. Continuously forming the first and second LiAl alloy layers, The substrate on which the first and second LiAl alloy layers are formed on both surfaces is continuously passed through a plating bath of molten lithium metal set to a temperature capable of maintaining molten lithium, thereby continuously passing the plating bath of molten lithium metal. A method of manufacturing a band-type negative plate sheet for a lithium secondary battery, comprising the step of depositing a lithium metal layer on the surfaces of the first and second LiAl alloy layers to continuously form the first and second negative electrode layers.