CN114824503A - Cylindrical solid battery and method for manufacturing same - Google Patents
Cylindrical solid battery and method for manufacturing same Download PDFInfo
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- CN114824503A CN114824503A CN202210048595.2A CN202210048595A CN114824503A CN 114824503 A CN114824503 A CN 114824503A CN 202210048595 A CN202210048595 A CN 202210048595A CN 114824503 A CN114824503 A CN 114824503A
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- electrode
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- state battery
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
- H01M10/0587—Construction or manufacture of accumulators having only wound construction elements, i.e. wound positive electrodes, wound negative electrodes and wound separators
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- General Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Secondary Cells (AREA)
- Sealing Battery Cases Or Jackets (AREA)
- Cell Electrode Carriers And Collectors (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
The present invention addresses the problem of preventing a decrease in ion conductivity by improving the adhesion between a solid electrolyte layer and an electrode even in a cylindrical solid-state battery having a wound group. In order to solve the above-described problems, a cylindrical solid-state battery is provided with a winding group in which a sheet-like electrode laminate in which a positive electrode and a negative electrode are laminated via a solid electrolyte layer is wound, wherein a sheet-like exterior material is joined to or extended to an outer peripheral end of the electrode laminate, and the exterior material is continuously wound from the electrode laminate and fixed at an end portion thereof, thereby constituting an outermost periphery of the cylindrical solid-state battery.
Description
Technical Field
The present invention relates to a wound cylindrical solid-state battery and a method for manufacturing the same.
Background
A wound cylindrical solid-state battery is configured such that current collectors extending from positive and negative electrodes are respectively collected by cover members at upper and lower sides of a cylindrical wound group, and the wound cylindrical solid-state battery includes a wound group formed by winding a sheet-like electrode laminate in which the positive electrode and the negative electrode are laminated with a solid electrolyte layer interposed therebetween.
All solid-state batteries such as lithium ion batteries have a positive electrode and a negative electrode laminated via a solid electrolyte layer, and conduct ions such as lithium ions via the solid electrolyte layer. Therefore, if the adhesion between the solid electrolyte layer and both electrodes is reduced, the ion conductivity is reduced, and therefore, when a module is configured from a single cell, it is necessary to restrain and apply pressure to maintain the adhesion.
However, since the conventional wound cylindrical solid-state battery is configured such that the wound assembly is inserted into an outer packaging container such as an outer can, a gap is formed between the wound assembly and the outer can. Therefore, it is difficult to apply pressure for restraint. In contrast, a technique of closely adhering the winding group to the outer can is disclosed (see patent document 1), but the outer can is still used, and it is required to maintain the pressure by more easily performing the restraint.
[ Prior Art document ]
(patent document)
Patent document 1: japanese patent laid-open publication No. 2014-082105
Disclosure of Invention
[ problems to be solved by the invention ]
The present invention has been made in view of the above problems, and an object of the present invention is to provide, with a simple configuration, the following means: in a cylindrical solid-state battery having a wound group, the adhesion between the solid electrolyte layer and the electrode is improved, and the reduction in ion conductivity is prevented.
[ means for solving problems ]
The present inventors have found that the above problems can be solved by joining or extending a sheet-like outer covering material to the outer peripheral end of the electrode laminate of the winding group to integrate the outer covering material in advance and winding the outer covering material while applying tension, and have completed the present invention. Namely, the present invention provides the following.
(1) A cylindrical solid-state battery comprising a winding group in which a sheet-like electrode laminate is wound, the sheet-like electrode laminate having a positive electrode and a negative electrode laminated via a solid electrolyte layer, wherein,
a sheet-like exterior material is joined to or extends to the outer peripheral end of the electrode laminate,
the outer material is continuously wound around the electrode laminate and fixed at the end, thereby constituting the outermost periphery of the cylindrical solid-state battery.
According to the invention of (1), the outer peripheral end of the electrode laminate is integrated with the sheet-like exterior material in advance by bonding or stretching, and the exterior material is wound while applying tension thereto, whereby the restrained state between the solid electrolyte layer and the two electrodes can be maintained. Further, since the outer package material directly serves as the outer package container, the outer package container is not required and the winding set does not need to be inserted into the container, which results in a simple structure.
(2) The cylindrical solid-state battery according to (1), wherein the negative electrode is composed of an electrode collector composed of a porous metal body and an electrode composite material filled in pores of the porous metal body.
According to the invention (2), even when an active material that is easily expanded, such as graphite, is used for the negative electrode, the expansion can be effectively absorbed by the three-dimensional network structure of the porous metal body.
(3) The cylindrical solid-state battery according to (2), wherein the electrode composite material of the negative electrode contains an expanding agent.
According to the invention of (3), not only the pressing effect from the outside of the winding group but also the pressing effect from the inside of the winding group can be obtained by utilizing the expansion of the negative electrode.
(4) The cylindrical solid-state battery according to any one of (1) to (3), wherein the exterior material is a current collector extending from the electrode stacked body.
According to the invention of (4), for example, the current collector of the negative electrode is made of stainless steel, and the current collector is directly extended without forming an electrode composite material, whereby the current collector can be used as an outer covering material for stainless steel.
(5) The cylindrical solid-state battery according to any one of (1) to (4), wherein the width of the exterior material in the cylindrical height direction is smaller than the width of the electrode laminate and is larger than the width of the electrode composite layers of the electrode laminate, and a portion of at least one electrode current collector protrudes from an end of the exterior material in the width direction.
According to the invention of (5), the joining property with the lid member connected to the external terminal is improved, and the manufacturing process can be further shortened.
(6) A method for manufacturing a cylindrical solid-state battery including a winding group in which a sheet-like electrode laminate is wound, the sheet-like electrode laminate having a positive electrode and a negative electrode laminated via a solid electrolyte layer, the method comprising:
a first step of bonding or extending a sheet-like outer covering material to an outer peripheral end of the electrode laminate; and (c) a second step of,
a second step of winding the electrode laminate and the exterior material with a predetermined tension to fix the ends, thereby forming the outermost periphery of the cylindrical solid-state battery.
According to the invention (6), the same effects as those of the invention (1) can be obtained. Further, since the electrode laminate is wound and fixed with a predetermined tension, a so-called wound state is obtained, and therefore a sufficient pressure can be maintained between the layers of the electrode laminate.
(7) The method for manufacturing a cylindrical solid-state battery according to item (6), wherein in the second step, the winding is performed while pressing the winding group from the outside.
According to the invention of (7), by pressing the electrode laminate also from the outside by a roll press or the like, a sufficient pressure can be further maintained between the layers of the electrode laminate.
(8) The method for manufacturing a cylindrical solid-state battery according to item (6) or (7), wherein in the second step, the outer diameter of the cylindrical solid-state battery is made substantially constant by adjusting a winding length of the exterior material.
According to the invention as recited in the aforementioned item (8), the outer diameters of the cylindrical solid-state batteries can be made substantially the same even when the layer structure, layer thickness, and the like of the electrode laminate change.
Drawings
Fig. 1 is a schematic perspective view showing one embodiment of a cylindrical solid battery of the present invention.
Fig. 2 is a sectional view showing an embodiment of a layer structure of an electrode collector.
Fig. 3 is a schematic perspective view showing a state in which the electrode collector of fig. 2 is formed by a roll press in the first step.
Fig. 4 is a side view showing an example of joining the winding group and the outer package material in the second step.
Fig. 5 is a side view showing another example of joining the winding group and the outer package material in the second step.
Fig. 6 is a side view showing a state in which pressing is performed by a roll press from the outside of the winding group in the second step.
Fig. 7 is a schematic perspective view showing a modification of the winding group.
Detailed Description
Hereinafter, an embodiment of the present invention will be described with reference to the drawings. The present invention is not limited to the description of the embodiments below. In the following embodiments, a lithium ion battery as a solid-state battery is described as an example, but the present invention can also be applied to solid-state batteries other than lithium ion batteries.
Overall structure of cylindrical solid battery
As shown in fig. 1, the cylindrical solid-state battery 100 of fig. 1 of the present embodiment is a wound-type lithium-ion secondary battery, and is composed of a cylindrical winding group 110, a negative electrode lid member 140 and a positive electrode lid member 150 that are electrically joined to the upper surface and the bottom surface of the winding group 110, respectively. The winding group 110 includes a sheet-like electrode laminate 120 wound around a core member not shown, and an outer cover 130 wound continuously around the outer peripheral end of the electrode laminate 120.
< Structure of electrode laminate >
As shown in fig. 2, the electrode laminate 120 of this embodiment is a counter electrode that constitutes the basic structure of positive electrode/solid electrolyte layer/negative electrode/solid electrolyte layer/positive electrode. A current collector is formed on each electrode, and in this embodiment, is a layer structure of positive electrode current collector 122/positive electrode composite material 122 a/solid electrolyte layer 160/negative electrode composite material 121 a/negative electrode current collector 121/negative electrode composite material 121 a/solid electrolyte layer 160/positive electrode composite material 122 a/positive electrode current collector 122. An insulating layer 170 is formed on the extended surface (both cross-sectional surfaces in fig. 2) of each current collector.
The electrode laminate in the present invention may have any structure as long as the positive electrode and the negative electrode are laminated with the solid electrolyte layer interposed therebetween, and may have, for example, a structure of negative electrode/solid electrolyte layer/positive electrode/solid electrolyte layer/negative electrode.
As shown in fig. 3, the electrode laminate 120 is obtained by press-laminating a first laminate 120A, a second laminate 120B, and a third laminate 120C by using a roll press P or the like (first step), the first laminate 120A being a positive electrode collector 122/positive electrode composite 122 a/solid electrolyte layer 160, the second laminate 120B being a negative electrode composite 121 a/negative electrode collector 121/negative electrode composite 121a, and the third laminate 120C being a solid electrolyte layer 160/positive electrode composite 122 a/positive electrode collector 122.
As a result, as shown in fig. 2 and 3, the electrode laminate 120 extends beyond the negative electrode current collector 121 and the positive electrode current collector 122 toward the respective end edges in the width direction of the wound group 110. In the state where the coil 110 is wound, the negative electrode current collector 121 is electrically joined to the negative electrode lid member 140 to form a negative electrode, and the positive electrode current collector 122 is electrically joined to the positive electrode lid member 150 to form a positive electrode (see fig. 1).
< Structure of Current collector >
In the present invention, the current collector may be a conventionally known current collector foil made of a metal foil of nickel, aluminum, stainless steel, titanium, copper, silver, or the like, but it is preferable that at least the electrode current collector (negative electrode current collector 121 in fig. 2) disposed at the center of fig. 2 is made of a metal porous body having pores (communicating pores) continuous with each other, and the inside is filled with an electrode composite material.
In this case, the hole of the current collector is filled with a composite material-filled region in which an electrode composite material containing an electrode active material is disposed to form an electrode layer, and the composite material-unfilled region in which the electrode composite material is not disposed to form the current collector.
The current collector is made of a porous metal body having pores continuous with each other. By having the continuous pores, the inside of the pores can be filled with the positive electrode composite material and the negative electrode composite material containing the electrode active material, and the amount of the electrode active material per unit area of the electrode layer can be increased. The metal porous body is not particularly limited as long as it has continuous pores, and examples thereof include foamed metals having pores formed by foaming, expanded metals, punched metals, metal nonwoven fabrics, and the like.
The metal used for the porous metal body is not particularly limited as long as it has conductivity, and examples thereof include nickel, aluminum, stainless steel, titanium, copper, and silver. Among them, foamed aluminum, foamed nickel, and foamed stainless steel are preferable as the current collector constituting the positive electrode, and foamed copper and foamed stainless steel are preferable as the current collector constituting the negative electrode.
By using the current collector of the metal porous body, the amount of active material per unit area of the electrode can be increased, and as a result, the volumetric energy density of the lithium ion secondary battery can be increased. Further, since the positive electrode composite material and the negative electrode composite material are easily fixed, unlike the conventional electrode using a metal foil as a current collector, it is not necessary to thicken the coating slurry for forming the electrode composite material layer when the electrode composite material layer is formed into a film having a thick layer. Therefore, the amount of a binder such as an organic polymer compound required for thickening can be reduced. Therefore, the capacity per unit area of the electrode can be increased, and the capacity of the lithium ion secondary battery can be increased.
In particular, in the present invention, even when an active material that is easily expanded, such as graphite, is used for the negative electrode, the expansion can be effectively absorbed by the three-dimensional network structure of the metal porous body.
< Structure of electrode composite >
The positive electrode composite material and the negative electrode composite material are respectively coated and formed on the current collector foil, or are filled and arranged in the hole when the current collector is a metal porous body. The positive electrode composite material and the negative electrode composite material contain a positive electrode active material and a negative electrode active material as essential components, respectively.
(electrode active Material)
The positive electrode active material is not particularly limited as long as it can absorb and release lithium ions, and examples thereof include LiCoO 2 、Li(Ni 5/10 Co 2/10 Mn 3/10 )O 2 、Li(Ni 6/10 Co 2/10 Mn 2/10 )O 2 、Li(Ni 8/10 Co 1/10 Mn 1/10 )O 2 、Li(Ni 0.8 Co 0.15 Al 0.05 )O 2 、Li(Ni 1/6 Co 4/6 Mn 1/6 )O 2 、Li(Ni 1/3 Co 1/3 Mn 1/3 )O 2 、LiCoO 4 、LiMn 2 O 4 、LiNiO 2 、LiFePO 4 Lithium sulfide, sulfur, and the like.
The negative electrode active material is not particularly limited as long as it can absorb and release lithium ions, and examples thereof include metallic lithium, lithium alloys, metal oxides, metal sulfides, metal nitrides, Si, SiO, and carbon materials such as artificial graphite, natural graphite, hard carbon, and soft carbon.
(other Components)
The electrode composite material may optionally contain other components than the electrode active material and the ion conductive particles. The other component is not particularly limited as long as it can be used in the production of a lithium ion secondary battery. Examples thereof include a conductive aid and a binder. The conductive assistant for the positive electrode may be acetylene black, and the binder for the positive electrode may be polyvinylidene fluoride. Examples of the binder for the negative electrode include sodium carboxymethylcellulose, styrene-butadiene rubber, and sodium polyacrylate.
In the present invention, SiO or Si may be intentionally contained as an expanding agent in the negative electrode composite material. In this case, the positive electrode composite material may contain a Li aluminum alloy or olivine iron Li that releases Li at a lower potential than an active material such as NCM. This structure may be operated outside the range of the State of Charge (SOC) of the battery, and the solid electrolyte layer and the electrode composite layer may be maintained in contact by generating a pressure from the inside of the wound group by the negative electrode swelling agent.
< solid electrolyte layer >
The solid electrolyte constituting the solid electrolyte layer is not particularly limited, and examples thereof include a sulfide-based solid electrolyte material, an oxide-based solid electrolyte material, a nitride-based solid electrolyte material, and a halide-based solid electrolyte material. Examples of the sulfide-based solid electrolyte material include LPS-based halogens (Cl, Br, I) and Li in the case of a lithium ion battery 2 S-P 2 S 5 、Li 2 S-P 2 S 5 LiI, etc. In addition, the above-mentioned "Li 2 S-P 2 S 5 "the description means that the composition contains Li 2 S and P 2 S 5 The sulfide-based solid electrolyte material obtained from the raw material composition of (1) is also described in other documents. Examples of the oxide-based solid electrolyte material include a lithium ion battery, which is a NASICON-type oxide, a garnet-type oxide, and a perovskite-type oxide. Examples of the NASICON (sodium super ion conductor) type oxide include oxides containing Li, Al, Ti, P, and O (for example, Li 1.5 Al 0.5 Ti 1.5 (PO 4 ) 3 ). Examples of garnet-type oxides include oxides containing Li, La, Zr, and O (e.g., Li) 7 La 3 Zr 2 O 12 ). Examples of the perovskite-type oxide include oxides containing Li, La, Ti and O (for example, LiLaTiO) 3 )。
< coil group and outer packaging Material >
Next, the outer package material 130, which is a feature of the present invention, will be specifically described with reference to fig. 4 to 6. The same components as those in fig. 1 to 3 are denoted by the same reference numerals, and the description thereof is omitted.
As shown in fig. 4, the winding group 110 forms a joint 180 with the outer cover 130 via a joint member 190 in a region including the end edge portion 120e of the wound electrode laminate 120. The longitudinal (MD) end edges of the outer cover 130 are fixed by welding or the like. The width of the exterior material 130 is substantially the same as the width of the electrode laminate 120 (excluding the extended portion of the current collector). The length of the outer cover 130 in the longitudinal direction (MD direction) may be formed so as to cover at least the entire circumference of the winding group 110, and may be wound in a plurality of turns. The diameter of the cylindrical solid-state battery can be adjusted by adjusting the number of windings (winding length) of the outer material.
The outer package material 130 is a sheet-like member, and is preferably composed of a thin plate of metal or the like. The joining member 190 is an insulating member such as a double-sided tape.
As shown in fig. 5, the outer cover 130 may be formed so as not to be involved between the electrode laminates 120 by the joining member. The term "joined" in the present invention includes a state of being laminated by such entanglement.
The outer material in the present invention does not need to be a member different from the electrode laminate. For example, the current collector extending from the electrode laminate may constitute the exterior material. For example, the negative electrode current collector 121 of the electrode laminate 120 in fig. 2 may be made of stainless steel, the coating of the negative electrode composite material 121a formed on both surfaces thereof may be completed in the longitudinal direction (MD direction) to form an end edge portion of the negative electrode composite material 121a, and only the negative electrode current collector 121 may be extended from the end edge portion to form the outer covering material. That is, the outer cover in the present invention includes not only the "joint" with the electrode laminate but also the outer cover "protruding" from the electrode laminate.
As shown in fig. 6, the electrode laminate 120 and the exterior material 130 continuous therewith are wound with a predetermined tension to form a wound form, thereby obtaining a wound coil 110 (second step). In this case, in addition to the tension adjustment, the winding may be performed while performing pressing by the roll pressure P or the like from the outside of the winding group 110 (from 3 in fig. 6).
According to the present invention, the outer peripheral end of the electrode laminate and the sheet-like outer covering material are integrated in advance by bonding or stretching, and the end portions are wound while applying tension to the outer covering material to fix the end portions. Accordingly, since the solid electrolyte layer and the electrodes can be maintained in a restrained state without forming a gap with the outer casing, the adhesion between the solid electrolyte layer and the electrodes can be improved, and the reduction in ion conductivity can be prevented. Further, since the outer package material directly serves as the outer package container, the outer package container is not required, and the winding group does not need to be inserted into the container.
< modification of winding group >
As shown in fig. 7, the width of the exterior material 130a in the cylindrical height direction in the wound group 110a is smaller than the width of the electrode laminate 120 and is larger than the width of the electrode composites (121a, 122 a). As a result, the electrode collectors 121 and 122 partially protrude from both ends in the width direction of the outer casing 130a, which is different from the winding group 110 in fig. 1, and the configuration is the same as that of the above embodiment except for this point.
According to this embodiment, since the electrode current collector extends from the exterior material while maintaining the constraint of the exterior material within the range of expansion and contraction of the electrode composite material, the bondability to the lid members 140 and 150 connected to the external terminals can be improved (for example, the bonded portions such as ultrasonic bonding, resistance welding, and laser welding are secured), and the manufacturing steps can be further shortened.
In addition, a part of either one of the electrode collectors 121 and 122 may protrude from an end of the exterior material 130 a. Further, any one of the electrodes may be connected to the exterior material so as to have the same potential. However, since the potential of the positive electrode is high, the negative electrode is preferable when the outer package material holds the electrode potential.
Although the preferred embodiments of the present invention have been described above, the contents of the present invention are not limited to the above embodiments and can be appropriately modified.
Reference numerals
100: cylindrical solid battery
110: winding group
120: electrode laminate
130: outer packaging material
140: negative electrode cover member
150: positive electrode cover member
160: solid electrolyte layer
170: insulating layer
180: joint part
190: joining member
Claims (8)
1. A cylindrical solid-state battery comprising a winding group in which a sheet-like electrode laminate is wound, the sheet-like electrode laminate having a positive electrode and a negative electrode laminated via a solid electrolyte layer, wherein,
a sheet-like exterior material is joined to or extends to the outer peripheral end of the electrode laminate,
the outer material is continuously wound around the electrode laminate and fixed at the end, thereby constituting the outermost periphery of the cylindrical solid-state battery.
2. The cylindrical solid-state battery according to claim 1, wherein,
the negative electrode is composed of an electrode collector composed of a porous metal body and an electrode composite material filled in pores of the porous metal body.
3. The cylindrical solid-state battery according to claim 2, wherein,
the electrode composite material of the negative electrode contains an expanding agent.
4. The cylindrical solid-state battery according to claim 1, wherein,
the exterior material is a current collector extending from the electrode laminate.
5. The cylindrical solid-state battery according to claim 1, wherein,
the width of the outer cover in the cylindrical height direction is narrower than the width of the electrode stack and wider than the width of the electrode composite layers of the electrode stack, and a portion of at least one electrode collector protrudes from an end of the outer cover in the width direction.
6. A method for manufacturing a cylindrical solid-state battery including a winding group in which a sheet-like electrode laminate is wound, the sheet-like electrode laminate having a positive electrode and a negative electrode laminated via a solid electrolyte layer, the method comprising:
a first step of bonding or extending a sheet-like outer covering material to an outer peripheral end of the electrode laminate; and the number of the first and second groups,
a second step of winding the electrode laminate and the exterior material with a predetermined tension to fix the ends, thereby forming the outermost periphery of the cylindrical solid-state battery.
7. The manufacturing method of a cylindrical solid battery according to claim 6,
in the second step, the winding is performed while being pressed from the outside of the winding group.
8. The manufacturing method of a cylindrical solid battery according to claim 6 or 7,
in the second step, the outer diameter of the cylindrical solid-state battery is made substantially constant by adjusting the winding length of the exterior material.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2021006215A JP7190516B2 (en) | 2021-01-19 | 2021-01-19 | Cylindrical solid-state battery and manufacturing method thereof |
| JP2021-006215 | 2021-01-19 |
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| Publication Number | Publication Date |
|---|---|
| CN114824503A true CN114824503A (en) | 2022-07-29 |
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| CN202210048595.2A Pending CN114824503A (en) | 2021-01-19 | 2022-01-17 | Cylindrical solid battery and method for manufacturing same |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS60249264A (en) * | 1984-05-24 | 1985-12-09 | Furukawa Battery Co Ltd:The | Manufacture of alkaline storage battery |
| JP4518583B2 (en) * | 1998-08-19 | 2010-08-04 | ソニー株式会社 | Solid electrolyte battery |
| JP4055345B2 (en) * | 1999-09-30 | 2008-03-05 | ソニー株式会社 | Solid electrolyte battery |
| JP2011113718A (en) * | 2009-11-25 | 2011-06-09 | Toyota Motor Corp | Winding-type all-solid battery, and manufacturing method of winding-type all-solid battery |
| WO2013140942A1 (en) * | 2012-03-22 | 2013-09-26 | 住友電気工業株式会社 | All-solid-state lithium secondary battery |
| CN111512490A (en) * | 2017-12-01 | 2020-08-07 | 宁德新能源科技有限公司 | Winding type battery cell |
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| JP7190516B2 (en) | 2022-12-15 |
| JP2022110670A (en) | 2022-07-29 |
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