JP2002279974A - Method of manufacturing electrode for secondary battery - Google Patents

Method of manufacturing electrode for secondary battery

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Publication number
JP2002279974A
JP2002279974A JP2001078203A JP2001078203A JP2002279974A JP 2002279974 A JP2002279974 A JP 2002279974A JP 2001078203 A JP2001078203 A JP 2001078203A JP 2001078203 A JP2001078203 A JP 2001078203A JP 2002279974 A JP2002279974 A JP 2002279974A
Authority
JP
Japan
Prior art keywords
thin film
electrode
active material
current collector
secondary battery
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Withdrawn
Application number
JP2001078203A
Other languages
Japanese (ja)
Inventor
Koichi Nishimura
Hisaki Tarui
Hiromasa Yagi
弘雅 八木
久樹 樽井
康一 西村
Original Assignee
Sanyo Electric Co Ltd
三洋電機株式会社
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Sanyo Electric Co Ltd, 三洋電機株式会社 filed Critical Sanyo Electric Co Ltd
Priority to JP2001078203A priority Critical patent/JP2002279974A/en
Publication of JP2002279974A publication Critical patent/JP2002279974A/en
Withdrawn legal-status Critical Current

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Classifications

    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50Manufacturing or production processes characterised by the final manufactured product
    • Y02P70/54Manufacturing of lithium-ion, lead-acid or alkaline secondary batteries

Abstract

(57) Abstract: An object of the present invention is to produce a secondary battery electrode having a high discharge capacity, excellent charge / discharge cycle life characteristics, and less wrinkling due to charge / discharge on a current collector. SOLUTION: In a method for manufacturing a secondary battery electrode formed by depositing an active material thin film 4 on a current collector 1, a method for manufacturing the current collector
, A mesh 3 is disposed above the active material layer 3, and an active material thin film 4 is deposited through the mesh 3.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for manufacturing an electrode for a secondary battery such as a lithium secondary battery and an electrode for a secondary battery manufactured by this method.

[0002]

2. Description of the Related Art In recent years, lithium secondary batteries have been actively developed. In a lithium secondary battery, battery characteristics such as charge / discharge voltage, charge / discharge cycle life characteristics, and storage characteristics greatly depend on the electrode active material used.

[0003] Among the electrode active materials capable of inserting and extracting lithium, silicon is a material capable of inserting lithium by alloying with lithium, and has been studied variously because of its large theoretical capacity. I have. However, since silicon absorbs lithium by alloying, volume expansion and contraction associated with charge / discharge reactions are large. For this reason, electrodes for lithium secondary batteries using silicon particles as an active material have poor charge / discharge cycle characteristics due to the fact that the active material is pulverized and peeled off from the current collector, and thus are not put into practical use. Not reached.

[0004]

SUMMARY OF THE INVENTION The present applicant uses an electrode made of a silicon thin film formed on a copper foil such as an electrolytic copper foil by a CVD method or a sputtering method as an electrode for a lithium secondary battery. It has been found that a lithium secondary battery having a high discharge capacity and excellent charge-discharge cycle life characteristics can be obtained (Japanese Patent Application No. 2000-32120).
No. 1). In these electrodes, a cut is formed in the thickness direction of the thin film by the charge / discharge reaction, whereby the thin film is separated into a columnar shape, and a void is formed around the columnar portion. It is thought that such voids can reduce expansion and contraction of the volume of the active material during the charge / discharge reaction.

[0005] However, in such an electrode, stress due to expansion and contraction of the volume of the active material due to a charge / discharge reaction acts on the current collector, and wrinkles may occur in the current collector. When wrinkles occur in the current collector, the energy density per volume when stored in the battery can is reduced.

An object of the present invention is to provide a method for producing an electrode for a secondary battery having a high discharge capacity, excellent charge-discharge cycle life characteristics, and in which wrinkles due to a charge-discharge reaction are unlikely to occur on a current collector. .

[0007]

SUMMARY OF THE INVENTION The present invention is a method of manufacturing an electrode for a secondary battery formed by depositing an active material thin film on a current collector, wherein a mesh is arranged above the current collector, and It is characterized in that an active material thin film is deposited through a mesh.

According to the present invention, an active material thin film is formed in a region of the current collector corresponding to the hole of the mesh so as to be relatively thick. Also, a relatively thin active material thin film is formed in a region corresponding to the mesh frame,
Alternatively, no active material thin film is formed. Generally, by arranging a mesh near the current collector, the thickness of a thin film formed in a region corresponding to a frame portion of the mesh tends to be thin, and an active material thin film is formed in a region corresponding to a mesh frame. To avoid this, the mesh is placed as close as possible to the current collector. Preferably, a mesh is arranged so as to be in close contact with the current collector.

According to the present invention, it is possible to form an active material thin film in which thick regions of the active material thin film are dispersed in an island shape corresponding to the holes of the mesh. In the active material thin film formed according to the present invention, the expansion and contraction of the volume in the thick island-like region can be absorbed in the surrounding thin region or the region where the thin film does not exist. It is possible to alleviate the stress due to the expansion and contraction of the volume acting on the current collector, and to suppress the occurrence of wrinkles in the current collector.

In a preferred embodiment according to the present invention, the active material thin film is deposited and formed only in the region corresponding to the holes of the mesh. In the active material thin film formed in this way, since the active material thin film does not exist around the island-shaped portion of the active material thin film, the volume expansion of the active material thin film can be sufficiently reduced, and the It is possible to more effectively prevent the current collector from wrinkling due to the stress.

In the present invention, a continuous thin film of the active material may be formed on the current collector in advance, and the active material thin film may be deposited on the thin film through a mesh. The continuous thin film serving as the underlayer can be formed, for example, by depositing an active material thin film without disposing a mesh above the current collector. After forming the continuous active material thin film in this manner, a mesh is arranged above the current collector, and the active material thin film can be formed by the same thin film forming method as when the continuous thin film is formed. According to such a method, a continuous thin film serving as a base layer and an active material thin film formed thereon can be formed in the same thin film forming apparatus. The thickness of the continuous active material thin film serving as an underlayer is not particularly limited,
It is preferably 10 μm or less per side.

In the case where the active material thin film is deposited only on the portion corresponding to the hole of the mesh and the active material thin film is not deposited on the portion corresponding to the frame of the mesh, the above-mentioned current collector or the above-mentioned current collector may be used. It is preferable to deposit the active material thin film in a state where the mesh is in close contact with the continuous thin film. As described above, the active material thin film formed as described above does not have a thin film around the island portion, so that the stress due to the volume expansion and contraction of the island portion can be sufficiently relaxed, and the current collector The generation of wrinkles can be more effectively prevented.

When the electrode for a secondary battery manufactured according to the present invention is used as an electrode for a lithium secondary battery, the active material thin film is formed of a thin film made of an active material that absorbs and releases lithium. Examples of the active material that stores and releases lithium include an active material that stores and absorbs lithium by alloying. Examples of such an active material include thin films of silicon, germanium, aluminum, tin, and the like. Among these, silicon has a high charge / discharge capacity, and therefore, a silicon thin film or a thin film containing silicon is preferably used. As the thin film containing silicon, a thin film containing 50 atomic% or more of silicon is preferable. Further, the silicon thin film or the thin film containing silicon is preferably an amorphous or microcrystalline thin film.

The method for forming an active material thin film in the present invention includes a method for forming a thin film from a gas phase and a method for forming a thin film from a liquid phase. As a method of depositing and forming a thin film from a gas phase, a sputtering method, a vacuum deposition method,
CVD method, thermal spraying method and the like can be mentioned. Examples of the method for depositing a thin film from a liquid phase include an electrolytic plating method and an electroless plating method.

In the mesh used in the present invention, the active material thin film is formed so as to be thicker in a region corresponding to the hole of the mesh. It is appropriately selected and used. For example, the size of the hole is 2 μm to 1 μm.
mm range.

As the mesh used in the present invention,
A mesh called an electroformed screen is preferably used. This is also called an electric sieve, and is a screen produced by an electrochemical method.

The current collector used in the present invention preferably has a small thickness, and is preferably a metal foil. In the case of a lithium secondary battery electrode, a current collector formed of a material that does not alloy with lithium is preferably used. Specific examples of such a current collector include at least one selected from copper, nickel, stainless steel, molybdenum, tungsten, and tantalum. As a particularly preferred current collector, a copper foil is used. As the copper foil, a copper foil whose surface is roughened is preferable. An electrolytic copper foil is mentioned as such a copper foil. Alternatively, a metal foil whose surface is roughened by depositing copper on another metal foil such as a nickel foil by an electrolytic method may be used.

FIG. 1 is a schematic perspective view for explaining the manufacturing method of the present invention. Referring to FIG. 1, a mesh 3 is arranged between a current collector 1 and an evaporation source 2 such as a target. The active species for forming a thin film generated from the evaporation source 2 reach the current collector 1 through the mesh 3 and reach the thin film 4.
Is formed. By providing the mesh 3 between the evaporation source 2 and the current collector 1, as shown in FIG. 1, a thin film 4 separated into islands corresponding to the holes of the mesh 3 is formed on the current collector 1. You. By bringing the mesh 3 closer to the current collector 1, an island-shaped active material thin film 4 having a pattern shape corresponding to the pattern of the holes of the mesh 3 can be formed.
By separating the mesh 3 from the current collector 1, the unevenness of the active material thin film 4 gradually becomes gentle, and the active material thin film has a smooth uneven surface.

The secondary battery electrode of the present invention is characterized in that it is a secondary battery electrode manufactured by the above-described manufacturing method of the present invention. The electrode for a secondary battery according to a more limited aspect of the present invention is characterized in that an active material thin film is selectively formed on a plurality of isolated island regions on a current collector.

[0020]

BEST MODE FOR CARRYING OUT THE INVENTION The present invention will be described below in detail with reference to examples, but the present invention is not limited to the following examples at all, and may be carried out by appropriately changing the scope of the present invention. It is possible.

(Examples 1 and 2) [Preparation of electrode] 4 inch (about 100 mm) single crystal Si
Was used as a target, and an active material thin film was formed on the current collector by a sputtering method using an RF magnetron sputtering apparatus. As the current collector, an electrolytic copper foil (18 μm in thickness) was used. This current collector was fixed to the cylindrical outer peripheral surface of the rotary drum, and affixed to the current collector in a state where the mesh was in close contact with the current collector. Electroformed screen (mesh made by electrochemical method) as mesh
Was used. Two types of electroformed screens were used, 250 LPI (thickness 34 μm, porosity 3).
8%) and 400 LPI (thickness 20 μm, porosity 34%)
Was used. LPI is 1 inch (2.54 cm)
The number of mesh lines per mesh, 250 LPI
Indicates that the mesh has 250 lines per inch (2.54 cm).

After the inside of the vacuum chamber was evacuated to 8 × 10 −4 Pa or less, sputtering was performed while introducing an argon gas at a flow rate of 50 sccm to deposit an amorphous silicon thin film on the current collector. The deposition amount of the silicon thin film is 10 μm when no mesh is arranged.
And the amount of deposition. The RF power was 350 W.

FIG. 2 shows a 200 LP used as a mesh.
1 is an optical micrograph showing an electroformed screen of I. FIG. 3 is an optical micrograph showing an electrode formed by depositing a silicon thin film on a copper foil as a current collector using the mesh shown in FIG.

FIG. 4 shows 400 LP used as a mesh.
1 is an optical micrograph showing an electroformed screen of I. FIG. 5 is an optical microscope photograph showing an electrode formed by depositing a silicon thin film on a copper foil as a current collector using the mesh shown in FIG.

As is apparent from FIGS. 2 to 5, an island-like silicon thin film having a pattern corresponding to the holes (voids) of the mesh is formed on the current collector. No silicon thin film is formed in a region corresponding to the mesh frame, and the surface of the copper foil is exposed.

An electrode having a silicon thin film formed on one side of the current collector as described above was cut into a size of 2 cm × 2 cm, and a monopolar test cell was prepared using the electrode as a working electrode. Note that an electrode manufactured using a 250 LPI mesh was referred to as Example 1, and an electrode manufactured using a 400 LPI mesh was referred to as Example 2.

[Preparation of Single Electrode Test Cell] As described above, a test cell was prepared using the electrodes of Examples 1 and 2 as a working electrode and metallic lithium as a counter electrode and a reference electrode. As the electrolytic solution, one obtained by dissolving 1 mol / liter of LiPF 6 in a mixed solvent of ethylene carbonate and diethyl carbonate at a volume ratio of 1: 1 was used. In the unipolar test cell, the reduction of the working electrode is charged and the oxidation is discharge.

Comparative Example 1 As a comparison, a copper foil as a current collector was prepared in the same manner as in the above example except that a silicon thin film was deposited on the current collector without disposing a mesh on the current collector. A silicon thin film was formed thereon, and this was used as an electrode of Comparative Example 1. Using this electrode, a monopolar test cell was produced in the same manner as described above.

[Charge / Discharge Test] With respect to the test cells of Examples 1 and 2 and Comparative Example 1 produced as described above,
A charge / discharge test was performed at 5 ° C. The test cells of Examples 1 and 2 had a constant current of 4 mA, the test cell of Comparative Example 1 had a constant current of 2 mA, and the potential with respect to the reference electrode was 0.
After charging until the voltage reached V, the battery was discharged until the voltage reached 2.0 V. This was defined as one cycle of charge and discharge, and charge and discharge were performed up to 10 cycles.

The maximum discharge capacity per 1 cm 2 of the electrode area of each test cell up to 10 cycles is shown in Table 1 as the maximum capacity. The thickness of the electrode after 10 cycles was measured with a micrometer, and the change in electrode thickness was determined from the thickness of the electrode before charging and the thickness of the electrode after 10 cycles. Since a slight variation was observed in the maximum capacity depending on the electrode, the change in electrode thickness was divided by the maximum capacity, and the change in thickness per 1 mAh is shown in Table 1 as “change in electrode thickness”.

[0031]

[Table 1] As is clear from Table 1, the electrodes of Examples 1 and 2 manufactured according to the present invention have a smaller change in electrode thickness than the electrode of Comparative Example 1. Examples 1 and 2
It has been observed with the naked eye that the wrinkle generated on the current collector of the electrode of Comparative Example 1 was significantly smaller than that of the electrode of Comparative Example 1. The reason why the change in the electrode thickness in Examples 1 and 2 is smaller than the change in the electrode thickness in Comparative Example 1 is that in the electrodes of Examples 1 and 2, the generation of wrinkles in the current collector due to charging and discharging is suppressed. Because it is.

Therefore, when the electrodes of Examples 1 and 2 are housed in a battery can, the energy density per volume can be increased as compared with the electrode of Comparative Example 1. (Example 3) [Preparation of electrode] Using the same current collector, target and apparatus as in Example 1, about 2 μm was formed on the current collector without using a mesh.
m amorphous silicon thin films were formed. Next, an electroformed screen of 250 LPI was attached on the silicon thin film formed on the current collector, and an amorphous silicon thin film was deposited again under the same conditions as in Example 1. An approximately 6 μm silicon thin film was deposited with the mesh arranged.

Observation of the fabricated electrode with an optical microscope confirmed that an island-shaped silicon thin film was formed on the silicon thin film serving as a base layer in a pattern corresponding to the holes of the mesh.

[0034]

According to the present invention, an electrode for a secondary battery having a high discharge capacity, excellent charge / discharge cycle life characteristics, and less wrinkling due to charge / discharge on a current collector can be obtained.

[Brief description of the drawings]

FIG. 1 is a schematic perspective view for explaining a manufacturing method of the present invention.

FIG. 2 is a plan view showing a 250 LPI electroformed screen used as a mesh in the embodiment of the present invention.

FIG. 3 is a plan view showing a surface state of an electrode manufactured using the mesh shown in FIG. 2 in the example of the present invention.

FIG. 4 is a plan view showing a 400 LPI electroformed screen used as a mesh in the embodiment of the present invention.

FIG. 5 is a plan view showing a surface state of an electrode manufactured using the mesh shown in FIG. 4 in the example of the present invention.

[Explanation of symbols]

 DESCRIPTION OF SYMBOLS 1 ... Current collector 2 ... Evaporation source 3 ... Mesh 4 ... Active material thin film

 ────────────────────────────────────────────────── ─── Continued on the front page (72) Inventor Hisaki Tarui 2-5-5 Keihanhondori, Moriguchi-shi, Osaka Sanyo Electric Co., Ltd. F-term (reference) 5H029 AJ03 AJ05 AL12 AM03 AM07 CJ24 5H050 AA07 AA08 BA16 CB12 DA03 DA04 GA24

Claims (10)

[Claims]
1. A method for manufacturing an electrode for a secondary battery in which an active material thin film is formed by depositing an active material thin film on a current collector, wherein a mesh is arranged above the current collector, and the active material thin film is deposited through the mesh. A method for producing an electrode for a secondary battery, comprising:
2. The active material thin film according to claim 1, wherein the active material thin film is formed on an isolated island region on the current collector corresponding to the hole of the mesh. A method for manufacturing an electrode for a secondary battery.
3. The active material thin film according to claim 1, wherein a continuous thin film of the active material is previously formed on the current collector, and the active material thin film is deposited on the thin film through the mesh. Method for producing an electrode for a secondary battery.
4. The continuous thin film is a thin film formed without disposing a mesh above the current collector. After the thin film is formed, a mesh is disposed above the current collector, and the continuous thin film is formed. The method for manufacturing an electrode for a secondary battery according to claim 3, wherein the active material thin film is formed by a similar thin film forming method.
5. The method for manufacturing an electrode for a secondary battery according to claim 1, wherein the mesh is disposed in close contact with the current collector or the continuous thin film. .
6. The electrode according to claim 1, wherein the active material thin film is a thin film for inserting and extracting lithium, and the electrode for a secondary battery is an electrode for a lithium secondary battery.
13. The method for producing an electrode for a secondary battery according to the above item.
7. The thin film of the active material is a silicon thin film or a thin film containing silicon.
The method for producing an electrode for a secondary battery according to any one of the above.
8. The method according to claim 1, wherein the active material thin film is formed by a sputtering method,
The method for producing an electrode for a secondary battery according to any one of claims 1 to 7, wherein the electrode is formed by a vacuum deposition method or a CVD method.
9. An electrode for a secondary battery, manufactured by the method according to claim 1. Description:
10. An electrode for a secondary battery, wherein an active material thin film is selectively formed on a plurality of isolated island regions on a current collector.
JP2001078203A 2001-03-19 2001-03-19 Method of manufacturing electrode for secondary battery Withdrawn JP2002279974A (en)

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