JP2008270004A - Lithium ion secondary battery, its manufacturing method, and coating device - Google Patents

Lithium ion secondary battery, its manufacturing method, and coating device Download PDF

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JP2008270004A
JP2008270004A JP2007112547A JP2007112547A JP2008270004A JP 2008270004 A JP2008270004 A JP 2008270004A JP 2007112547 A JP2007112547 A JP 2007112547A JP 2007112547 A JP2007112547 A JP 2007112547A JP 2008270004 A JP2008270004 A JP 2008270004A
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metal foil
coating film
coating
surface treatment
lithium ion
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JP5369385B2 (en
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Takao Kuromiya
孝雄 黒宮
Tatsuya Hashimoto
達也 橋本
Masaya Okochi
正也 大河内
Yuji Iwagami
祐司 岩上
Kazunori Kubota
和典 久保田
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Panasonic Holdings Corp
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Matsushita Electric Industrial Co Ltd
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    • Y—GENERAL 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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Abstract

<P>PROBLEM TO BE SOLVED: To provide the manufacturing method of a lithium ion secondary battery capable of obtaining an electrode plate having a coating start end part having no bent or no swelling. <P>SOLUTION: The manufacturing method of the lithium ion secondary battery has at least a process continuously feeding metal foil from a hoop on which a belt-like metal foil is wound; a process intermittently conducting physical surface treatment on either one surface of the fed metal foil; a process forming a coating film by applying coating material on a part or the whole of the physically treated surface of the metal foil; a process removing volatile components in the coating film; and a process continuously winding metal foil having on its surface the coating film from which volatile components are removed on the hoop. <P>COPYRIGHT: (C)2009,JPO&INPIT

Description

本発明は、リチウムイオン二次電池の製造方法に関し、さらにこの方法により製造されたリチウムイオン二次電池、および塗布装置に関する。   The present invention relates to a method for manufacturing a lithium ion secondary battery, and further relates to a lithium ion secondary battery manufactured by this method and a coating apparatus.

近年、携帯電話、ノートパソコン等の携帯用電子・通信機器等に用いられる非水電解液二次電池の代表として、リチウムイオンの吸蔵・放出が可能な炭素材料等を負極活物質とし、リチウム遷移金属複合酸化物を正極活物質とするリチウムイオン二次電池が実用化されている。   In recent years, as a representative of non-aqueous electrolyte secondary batteries used in portable electronic and communication devices such as mobile phones and laptop computers, carbon transition materials that can occlude and release lithium ions are used as negative electrode active materials, and lithium transitions A lithium ion secondary battery using a metal composite oxide as a positive electrode active material has been put into practical use.

リチウム遷移金属複合酸化物のような正極活物質、導電材、結着剤、及び増粘剤を溶媒に加えて混練分散し、流動性を有する正極用の電極合剤塗料を作製する。このように作製した電極合剤塗料を、例えば図１に示すように、集電体１であるアルミニウム箔の長手方向Ａ（塗布方向）に沿って間欠的に塗布し、塗工部２と未塗工部３とを交互に形成する。このようにしてアルミニウム箔の両面に塗布された電極合剤塗料中の揮発成分である溶媒を除去した後、所定の密度になるように圧延し、幅方向Ｂにおいて必要な幅に裁断する。このようにして正極板を作製する。   A positive electrode active material such as a lithium transition metal composite oxide, a conductive material, a binder, and a thickener are added to a solvent and kneaded and dispersed to prepare an electrode mixture paint for a positive electrode having fluidity. For example, as shown in FIG. 1, the electrode mixture paint produced in this way is intermittently applied along the longitudinal direction A (application direction) of the aluminum foil that is the current collector 1, and the coating part 2 and the uncoated part 2 are not applied. The coating parts 3 are formed alternately. Thus, after removing the solvent which is a volatile component in the electrode mixture coating material applied to both surfaces of the aluminum foil, it is rolled to a predetermined density and cut to a required width in the width direction B. In this way, a positive electrode plate is produced.

この正極に用いられるアルミニウム箔のような金属箔は、一般に、圧延のような製造工程を経るため、表面に油分が付着しているものが多い。このような油分が残存した金属箔の表面に塗料を塗布すると、図２に示すように塗工部２と未塗工部３の境界部４が湾曲したり、図３に示すように塗工開始端部５において盛り上がりが生じたりすることで、圧延工程における過剰な応力集中による金属箔の切れや、合材脱落が発生し、ひいては電池性能を低下させるという問題が生じる。   In general, a metal foil such as an aluminum foil used for the positive electrode undergoes a manufacturing process such as rolling, so that many oils adhere to the surface. When a paint is applied to the surface of the metal foil in which such oil remains, the boundary 4 between the coated portion 2 and the uncoated portion 3 is curved as shown in FIG. 2, or the coating is applied as shown in FIG. When the starting end portion 5 is raised, the metal foil is cut off due to excessive stress concentration in the rolling process, or the composite material is dropped, resulting in a problem that the battery performance is lowered.

従って、電極用集電体として用いられる金属箔は、表面の残油量の少ないものが必要とされる。   Therefore, the metal foil used as the electrode current collector is required to have a small amount of residual oil on the surface.

一般に、金属箔の表面の脱脂方法に関しては、有機系溶剤、酸、アルカリ等の洗浄液による洗浄、焼鈍による油の焼失等が知られている（特許文献１、２、３、４または５参照）。
特開平５−２００４０６号公報 特開平１１−８７１８９号公報 特開平１１−２２９１００号公報 特開２００５−２２２９３６号公報 特開平７−１３５０２３号公報 In general, as for the method of degreasing the surface of a metal foil, cleaning with a cleaning liquid such as an organic solvent, acid, alkali, etc., oil burning by annealing, etc. are known (see Patent Documents 1, 2, 3, 4 or 5). .
JP-A-5-200406 JP 11-87189 A JP-A-11-229100 JP 2005-222936 A JP 7-1335023 A

しかしながら、従来の脱脂方法は、金属箔の表面に電極合剤塗料を塗布する前に、別の工程において脱脂処理を施しており、また、脱脂の効果を高めるために、脱脂するための手段を備えた装置で脱脂処理を複数回繰り返して施しており、金属箔の強度や生産性が低くなるという問題を有していた。   However, in the conventional degreasing method, before applying the electrode mixture paint to the surface of the metal foil, degreasing treatment is performed in a separate step, and in order to enhance the degreasing effect, a means for degreasing is provided. The degreasing treatment was repeated a plurality of times with the provided apparatus, and the strength and productivity of the metal foil were low.

さらに、脱脂処理によって油分が除去された表面は非常に濡れ性が高くなるため、この金属箔の表面には、工程内に存在または発生する異物も非常に付着しやすくなる。このような異物が除去されずに電池内に混入した場合、電池性能が低下し、さらには異物が導電
性を有する場合、正負極間が短絡し発熱および発火が生じるという問題も有していた。 Furthermore, since the surface from which the oil has been removed by the degreasing treatment has very high wettability, foreign matter present or generated in the process is very likely to adhere to the surface of the metal foil. When such foreign matter is mixed in the battery without being removed, the battery performance deteriorates. Further, when the foreign matter has conductivity, there is a problem that the positive and negative electrodes are short-circuited to generate heat and fire. .

前記従来の課題を解決するために、本発明のリチウムイオン二次電池の製造方法は、少なくとも、帯状の金属箔を連続的に送り出す工程と、送り出された金属箔のいずれか一方の表面に物理的表面処理を間欠的に施す工程と、金属箔の物理的表面処理された部分の一部また全部の表面に塗料を塗布して塗膜を形成する工程と、前記塗膜中の揮発成分を除去する工程と、揮発成分が除去された塗膜が表面に形成された金属箔を連続的にフープに巻き取る工程を有することを特徴とするものである。   In order to solve the above-mentioned conventional problems, the method of manufacturing a lithium ion secondary battery of the present invention includes at least a step of continuously feeding a strip-shaped metal foil and a physical surface on one surface of the fed metal foil. A step of intermittently applying a surface treatment, a step of applying a paint on a part or all of the surface of the metal foil that has been physically surface-treated to form a coating film, and a volatile component in the coating film. It has the process of removing, and the process of winding up the metal foil in which the coating film from which the volatile component was removed was formed in the hoop continuously.

本発明のリチウムイオン二次電池の製造方法によって、良好な塗布開始端部を有する電極合剤塗膜を形成することができる。   By the method for producing a lithium ion secondary battery of the present invention, an electrode mixture coating film having a good coating start end can be formed.

また、この金属箔の物理的表面処理が施された部分の２５℃における表面張力が、ＪＩＳ Ｋ６７６８に記載された試験方法によって測定されたぬれ張力値で３５ｍＮ／ｍ以上であるのが好ましい。   Moreover, it is preferable that the surface tension in 25 degreeC of the part to which the physical surface treatment of this metal foil was performed is 35 mN / m or more by the wetting tension value measured by the test method described in JISK6768.

本発明のリチウムイオン二次電池は、上記の方法で製造されたリチウムイオン二次電池である。   The lithium ion secondary battery of this invention is a lithium ion secondary battery manufactured by said method.

さらに、本発明の塗布装置は、少なくとも、帯状の金属箔を連続的に送り出す手段と、前記金属箔のいずれか一方の表面に物理的表面処理を間欠的に施すことができる手段と、金属箔の物理的表面処理された部分の一部または全部の表面に塗料を塗布して塗膜を形成する手段と、前記塗膜中の揮発成分を除去する手段と、揮発成分が除去された塗膜が表面に形成された金属箔を連続的にフープに巻き取る手段を少なくとも、備えたものであり、本発明のリチウムイオン二次電池の製造方法に適した塗布装置である。   Furthermore, the coating apparatus of the present invention includes at least means for continuously feeding a strip-shaped metal foil, means for intermittently performing physical surface treatment on one surface of the metal foil, and metal foil. Means for applying a paint to a part or all of the surface of the part subjected to the physical surface treatment to form a coating film, means for removing volatile components in the coating film, and coating film from which volatile components have been removed Is a coating apparatus suitable for the method for producing a lithium ion secondary battery of the present invention, comprising at least means for continuously winding the metal foil formed on the surface of the metal foil into a hoop.

この塗布装置における隣接する金属箔の搬送用ロール間の最も短い距離が、前記物理的表面処理が間欠的に施された金属箔の物理的表面処理がされていない部分の長さより短いことが好ましい。   The shortest distance between adjacent metal foil transport rolls in this coating apparatus is preferably shorter than the length of the portion of the metal foil that has been subjected to the physical surface treatment that has not been subjected to physical surface treatment. .

本発明によると、金属箔の強度や生産性の低下や、金属箔の表面への異物の付着を生じさせることなく、良好な塗布開始端部の形状を実現させることができ、その後の圧延工程においても電極合剤塗膜の局所的な応力集中による金属箔の切れ、塗膜の脱落を生じさせることなく、良好な電池性能を有するリチウムイオン二次電池を実現できるとともに、電池内への異物の混入を抑制することができ、電池性能や安全性の低下も抑制することができる。   According to the present invention, it is possible to realize a good shape of the coating start end without causing a decrease in strength and productivity of the metal foil and adhesion of foreign matter to the surface of the metal foil, and a subsequent rolling step In addition, it is possible to realize a lithium ion secondary battery having good battery performance without causing the metal foil to be cut off or the coating film to fall off due to local stress concentration of the electrode mixture coating film, and to prevent foreign matter from entering the battery. Can be suppressed, and battery performance and safety can also be prevented from deteriorating.

以下に本発明を実施するための最良の形態について、図面を参照しながら説明する。   The best mode for carrying out the present invention will be described below with reference to the drawings.

（実施の形態）
図４は、本発明の実施の形態における電極合剤塗料の塗布装置の模式図である。図４において、巻き出し部６のフープ１１から送り出された金属箔からなる集電体１の表面は、物理的表面処理装置７によって、脱脂処理が施される。この脱脂処理された方の集電体１の表面に、塗布器８によって電極合剤塗料を間欠的に塗布することで、電極合剤塗膜からなる塗工部２と塗膜が形成されていない未塗工部３が形成され、塗工部２の電極合剤塗膜に含まれる揮発成分を乾燥器９によって除去した後に、巻き取り部１０で電極合剤塗膜が形成された集電体１がフープ１２に巻き取られる。 (Embodiment)
FIG. 4 is a schematic diagram of an electrode mixture paint coating apparatus according to an embodiment of the present invention. In FIG. 4, the surface of the current collector 1 made of a metal foil sent out from the hoop 11 of the unwinding unit 6 is degreased by a physical surface treatment device 7. By applying the electrode mixture paint intermittently with the applicator 8 on the surface of the current collector 1 subjected to the degreasing treatment, the coating part 2 and the coating film made of the electrode mixture coating film are formed. A current collector in which an uncoated part 3 is formed and a volatile component contained in the electrode mixture coating film of the coating part 2 is removed by the dryer 9 and then an electrode mixture coating film is formed in the winding unit 10 The body 1 is wound on the hoop 12.

ここで、物理的表面処理装置７は、物理的表面処理を施した金属箔の表面のぬれ性が向上させることができるものであれば、特に限定されるものではなく、例えば、コロナ放電処理、プラズマ処理、紫外線照射処理、レーザー処理が挙げられる。また、物理的表面処理装置の能力については、塗布速度、塗膜厚み、金属箔の表面に存在する油分の種類および量、電極合剤塗料の粘度および表面張力などによって異なるため、一義に定義することはできないが、例えば、塗布速度２０ｍ／ｍｉｎで、粘度５０００ｍＰａ・ｓ、表面張力４０ｍＮ／ｍの電極合剤塗料を０．１５ｍｍの厚みでアルミニウム圧延箔上へ塗布する場合に、１本の電極を備えたコロナ放電処理装置を１ｋＷの出力で用いることで、十分にぬれ性を高めることが可能であった。   Here, the physical surface treatment apparatus 7 is not particularly limited as long as the wettability of the surface of the metal foil subjected to the physical surface treatment can be improved. For example, the corona discharge treatment, Plasma treatment, ultraviolet irradiation treatment, and laser treatment are exemplified. In addition, the ability of the physical surface treatment apparatus is uniquely defined because it varies depending on the coating speed, the coating thickness, the type and amount of oil present on the surface of the metal foil, the viscosity and surface tension of the electrode mixture paint, etc. For example, when an electrode mixture paint having a coating speed of 20 m / min, a viscosity of 5000 mPa · s, and a surface tension of 40 mN / m is applied to an aluminum rolled foil with a thickness of 0.15 mm, one electrode By using a corona discharge treatment apparatus equipped with an output of 1 kW, it was possible to sufficiently improve the wettability.

また、塗布器８についても、塗膜を所望の厚みに塗布することが可能なものであれば本発明では特に限定されるものではなく、例えば、ダイ、グラビア、コンマ、バーなどの一般的な塗布方式を用いることができる。同様に、乾燥器９についても、本発明では、電極合剤塗料中の揮発成分を除去できるものであれば特に限定されるものではなく、例えば、遠赤外線または中赤外線ヒーターなどの輻射伝熱によるもの、ジェットノズル、カウンターフローなどの熱風の対流伝熱によるもの、電磁誘導加熱によるものなどを用いることができる。   Further, the applicator 8 is not particularly limited in the present invention as long as it can apply the coating film to a desired thickness. For example, a common die, gravure, comma, bar, etc. A coating method can be used. Similarly, the dryer 9 is not particularly limited in the present invention as long as it can remove the volatile components in the electrode mixture paint. For example, the dryer 9 is based on radiant heat transfer such as far infrared or mid infrared heaters. The thing by the convection heat transfer of hot air, such as a thing, a jet nozzle, and a counter flow, the thing by electromagnetic induction heating, etc. can be used.

次に、物理的表面処理が施され、かつ電極合剤塗料が形成されていない部分３の長さが、塗布装置内の隣接する搬送ロール間の最小距離よりも長く、このような部分を含む集電体を塗布装置で搬送した場合には、一般的に塗布装置に用いられている蛇行矯正手段や張力調整手段の動作によって、集電体に皺が発生したり、破断したりすることがある。これは、搬送ロールの表面と物理的表面処理が施された集電体の表面の密着性が高いために、適度に必要な搬送ロール表面における集電体の滑りが抑制されてしまうためであり、この問題は、集電体表面の電極合剤塗膜を形成しない部分に物理的表面処理を施さないことで解決できる。また、物理的表面処理が施されてぬれ性の高められた集電体の表面は、異物も非常に付着し易く、特にリチウムイオン二次電池では、異物による電池性能や安全性の低下が顕著なため、この点からも、集電体表面の電極合剤塗膜を形成しない部分には物理的表面処理を施さないことが望ましい。   Next, the length of the portion 3 where the physical surface treatment is performed and the electrode mixture coating material is not formed is longer than the minimum distance between adjacent transport rolls in the coating apparatus, and includes such a portion. When the current collector is transported by a coating device, wrinkles may occur on the current collector or may break due to the operation of the meandering correction means and tension adjusting means generally used in the coating device. is there. This is because, due to the high adhesion between the surface of the transport roll and the surface of the current collector that has been subjected to physical surface treatment, slipping of the current collector on the surface of the transport roll that is necessary is suppressed. This problem can be solved by not applying a physical surface treatment to the portion of the current collector surface where the electrode mixture coating film is not formed. In addition, the surface of the current collector that has been subjected to physical surface treatment and has improved wettability is very susceptible to foreign matter, and particularly in lithium ion secondary batteries, the battery performance and safety are significantly reduced due to foreign matter. Therefore, also from this point, it is desirable not to perform physical surface treatment on the portion of the current collector surface where the electrode mixture coating film is not formed.

ここで、本発明における脱脂とは、油分が揮発して除去されることのみならず、油分が物理的表面処理によって分解または変化して表面張力が低下した状態をも含むものである。従って、脱脂の度合いは、残油量あるいは油分の分解物または変化物の残留量ではなく、コーティング材の塗工性の良否、即ち箔表面のぬれ性によって判断される。前記ぬれ性は、ＪＩＳ Ｋ６７６８に記載された試験方法によって測定された値をぬれ張力値として定義する。本発明のアルミニウム硬箔は、箔用途や前記ぬれ性試験液による接触角を限定するものではないが、リチウムイオン二次電池の電極用基材として用いる場合は、コーティング材の塗工性を確保するために前記ぬれ張力値が３５ｍＮ／ｍ以上となされたものを用いることが好ましく、特に４０ｍＮ／ｍ以上が好ましい。また、上述したぬれ性試験液として、エチレングリコールモノエチルエーテルとホルムアミドの混合液を例示できる。本発明は、上述した以外のぬれ性試験やそのようなぬれ性試験で規定されたぬれ性を有する金属箔を排除するものではない。   Here, the degreasing in the present invention includes not only that the oil is volatilized and removed, but also includes a state where the oil is decomposed or changed by physical surface treatment and the surface tension is lowered. Therefore, the degree of degreasing is determined not by the residual oil amount or the residual amount of decomposed or changed oil components but by the quality of the coating material, that is, the wettability of the foil surface. The wettability is defined as a wet tension value measured by a test method described in JIS K6768. The aluminum hard foil of the present invention does not limit the contact angle with the foil application or the wettability test solution, but when used as a base material for an electrode of a lithium ion secondary battery, the coating property of the coating material is ensured. In order to achieve this, it is preferable to use one having a wetting tension value of 35 mN / m or more, particularly 40 mN / m or more. Examples of the wettability test solution described above include a mixed solution of ethylene glycol monoethyl ether and formamide. The present invention does not exclude wettability tests other than those described above and metal foils having wettability defined by such wettability tests.

本発明の脱脂処理は、洗浄液による脱脂のように洗浄液を除去するといった別の工程も不要で、単一の塗布装置内で金属箔の表面処理から塗布、乾燥までを連続して行うため、生産性に優れるとともに、塗膜を形成する部分のみを選択して表面処理を施すことも容易に実現できる。   The degreasing process of the present invention does not require another process such as removing the cleaning liquid like degreasing with a cleaning liquid, and since the process from surface treatment to coating and drying of the metal foil is continuously performed in a single coating apparatus, production In addition to being excellent in properties, it is also possible to easily perform surface treatment by selecting only the portion where the coating film is formed.

従来のリチウムイオン二次電池と、本発明の製造方法によるリチウムイオン二次電池との比較を表１のデータをもとに説明する。   A comparison between a conventional lithium ion secondary battery and a lithium ion secondary battery produced by the production method of the present invention will be described based on the data in Table 1.

（実施例１）
本発明の製造方法による実施例１の電池には、集電体として、ＪＩＳ Ｈ４１６０に記載された合金番号１０８５、厚み０．０２ｍｍのアルミニウム箔を用いた。前記アルミニウム箔は、圧延により製造されたものであり、その製造過程で用いられた油分が表面に残存しており、何らの表面処理を施さない状態での前記アルミニウム箔表面のぬれ性はＪＩＳ Ｋ６７６８に記載された試験方法にて２８ｍＮ／ｍのぬれ張力値であった。 Example 1
In the battery of Example 1 according to the manufacturing method of the present invention, an aluminum foil having an alloy number of 1085 and a thickness of 0.02 mm described in JIS H4160 was used as a current collector. The aluminum foil is manufactured by rolling, the oil used in the manufacturing process remains on the surface, and the wettability of the surface of the aluminum foil without any surface treatment is JIS K6768. The wetting tension value was 28 mN / m according to the test method described in 1).

塗布装置の巻き出し部と塗布器との間に配置された物理的表面処理装置によって、巻き出し部から送り出された前記アルミニウム箔の塗膜を形成する側の表面に物理的表面処理を施し、物理的表面処理が施された表面に正極合剤塗料をダイ方式で間欠的に所定量塗布し、揮発分を乾燥除去することによって正極合剤塗膜を形成した。同様にしてアルミニウム箔のもう一方の表面に正極合剤塗膜を形成した後、ロールプレスにより所定の厚みとし、さらに所定の寸法に裁断することで、正極板を作製した。   By applying a physical surface treatment to the surface on which the coating film of the aluminum foil fed from the unwinding part is formed by a physical surface treatment device arranged between the unwinding part and the applicator of the coating apparatus, A predetermined amount of positive electrode mixture paint was intermittently applied to the surface that had been subjected to physical surface treatment by a die method, and volatile components were removed by drying to form a positive electrode mixture coating film. In the same manner, after forming a positive electrode mixture coating film on the other surface of the aluminum foil, the positive electrode plate was prepared by making a predetermined thickness by a roll press and further cutting into a predetermined dimension.

正極合剤塗料には、正極活物質であるコバルト酸リチウム１００重量部に、導電材であるアセチレンブラック４重量部および結着剤であるポリフッ化ビニリデン５重量部を分散媒であるｎ−メチル−２−ピロリドン中に分散させスラリー化したものを用いた。   In the positive electrode mixture paint, 100 parts by weight of lithium cobaltate as a positive electrode active material, 4 parts by weight of acetylene black as a conductive material and 5 parts by weight of polyvinylidene fluoride as a binder are n-methyl-as a dispersion medium. What was dispersed and slurried in 2-pyrrolidone was used.

本実施例で用いた物理的表面装置は、コロナ放電によるものであり、コロナ放電電極と、前記コロナ放電電極に対向した接地ロールに巻き掛けられたアルミニウム箔表面との距離を０．５ｍｍとし、走行速度２０ｍ／ｍｉｎにて、塗布器により正極合剤塗膜を塗布する直前に、アルミニウム箔表面に０．２ｋＷの出力でコロナ放電処理を行った。また、コロナ放電は、正極合剤塗膜を形成する部分のみに行った。   The physical surface device used in this example is by corona discharge, and the distance between the corona discharge electrode and the surface of the aluminum foil wound around the grounding roll facing the corona discharge electrode is 0.5 mm, Immediately before applying the positive electrode mixture coating film with an applicator at a running speed of 20 m / min, a corona discharge treatment was performed on the aluminum foil surface with an output of 0.2 kW. Moreover, corona discharge was performed only to the part which forms a positive mix film.

前記コロナ放電処理によって、アルミニウム箔表面のぬれ性は、ＪＩＳ Ｋ６７６８に記載された試験方法にて３４ｍＮ／ｍのぬれ張力値となった。前記アルミニウム箔上に間欠塗布された正極合剤塗膜の塗工部と未塗工部の境界部４の湾曲は小さく、図２に示したＬの値は０．２ｍｍとなった。塗布開始端部５の厚みは平均厚みに対して０．０１ｍｍの盛り上がりであった。   By the corona discharge treatment, the wettability of the aluminum foil surface became a wet tension value of 34 mN / m by the test method described in JIS K6768. The curvature of the boundary portion 4 between the coated portion and the uncoated portion of the positive electrode mixture coating film intermittently applied on the aluminum foil was small, and the value of L shown in FIG. 2 was 0.2 mm. The thickness of the coating start end 5 was a swell of 0.01 mm with respect to the average thickness.

また、塗布装置、ロールプレス装置、裁断装置のいずれにおいても、アルミニウム箔の皺、切れは発生することはなかった。   Moreover, no flaws or breakage of the aluminum foil occurred in any of the coating device, roll press device, and cutting device.

（実施例２）
アルミニウム箔表面のコロナ放電処理における出力を０．５ｋＷとした以外は、実施例１と全く同じにして正極板を作製した。 (Example 2)
A positive electrode plate was produced in the same manner as in Example 1 except that the output in the corona discharge treatment on the aluminum foil surface was 0.5 kW.

アルミニウム箔表面のぬれ性は、ＪＩＳ Ｋ６７６８に記載された試験方法にて４２ｍＮ／ｍのぬれ張力値となった。前記アルミニウム箔上に間欠塗布された正極合剤塗膜の塗工部と未塗工部の境界部４の湾曲はＬ＝０．０ｍｍ、塗布開始端部５の厚みは平均厚みに対して０．００４ｍｍの盛り上がりとなり、塗布装置、ロールプレス装置、裁断装置のいずれにおいても、アルミニウム箔の皺、切れが発生することはなかった。   The wettability of the aluminum foil surface was a wet tension value of 42 mN / m by the test method described in JIS K6768. The curvature of the boundary portion 4 between the coated portion and the uncoated portion of the positive electrode mixture coating film intermittently applied on the aluminum foil is L = 0.0 mm, and the thickness of the coating start end portion 5 is 0 with respect to the average thickness. The swell was 0.004 mm, and no flaws or breakage of the aluminum foil occurred in any of the coating apparatus, roll press apparatus, and cutting apparatus.

（実施例３）
アルミニウム箔表面のコロナ放電処理における出力を２．０ｋＷとした以外は、実施例１と全く同じにして正極板を作製した。 (Example 3)
A positive electrode plate was produced in exactly the same manner as in Example 1 except that the output in the corona discharge treatment on the aluminum foil surface was 2.0 kW.

アルミニウム箔表面のぬれ性は、ＪＩＳ Ｋ６７６８に記載された試験方法にて５１ｍＮ／ｍのぬれ張力値となった。前記アルミニウム箔上に間欠塗布された正極合剤塗膜の塗工部と未塗工部の境界部４の湾曲はＬ＝０．０ｍｍ、塗布開始端部５の厚みは平均厚みに対して０．００３ｍｍの盛り上がりとなり、塗布装置、ロールプレス装置、裁断装置のいずれにおいても、アルミニウム箔の皺、切れが発生することはなかった。   The wettability of the aluminum foil surface was a wet tension value of 51 mN / m by the test method described in JIS K6768. The curvature of the boundary portion 4 between the coated portion and the uncoated portion of the positive electrode mixture coating film intermittently applied on the aluminum foil is L = 0.0 mm, and the thickness of the coating start end portion 5 is 0 with respect to the average thickness. The swell was 0.003 mm, and no flaws or breakage of the aluminum foil occurred in any of the coating apparatus, roll press apparatus, and cutting apparatus.

（比較例１）
アルミニウム箔表面に何らの表面処理を施していないこと以外は、実施例１と全く同じにして正極板を作製した。アルミニウム箔表面のぬれ性はＪＩＳ Ｋ６７６８に記載された試験方法にて２８ｍＮ／ｍのぬれ張力値であった。 (Comparative Example 1)
A positive electrode plate was produced in the same manner as in Example 1 except that no surface treatment was applied to the surface of the aluminum foil. The wettability of the aluminum foil surface was a wet tension value of 28 mN / m according to the test method described in JIS K6768.

間欠塗布した前記正極合剤塗膜の塗工部と未塗工部の境界部４は大きく湾曲しており、Ｌ＝２．０ｍｍであった。さらに、湾曲の最も凹んだ部分での塗布開始端部５の厚みは、平均厚みに対して０．０４ｍｍと大きく盛り上がった形状となっていた。   The boundary portion 4 between the coated portion and the uncoated portion of the positive electrode mixture coating film applied intermittently was greatly curved, and L = 2.0 mm. Furthermore, the thickness of the coating start end portion 5 at the most concave portion of the curve was a shape that greatly increased to 0.04 mm with respect to the average thickness.

塗布装置および裁断装置ではアルミニウム箔の皺、切れが発生することはなかったが、ロールプレス装置にて、塗布開始端部５を起点としたアルミニウム箔の切れが発生した。塗布開始端部５の盛り上がりが０．０４ｍｍと大きいことによるロールプレスによる応力集中が原因と考えられる。   In the coating device and the cutting device, the aluminum foil did not wrinkle or break, but in the roll press device, the aluminum foil started from the coating start end 5. It is considered that the stress concentration due to the roll press due to the large bulge of the coating start end 5 is 0.04 mm.

（比較例２）
アルミニウム箔の物理的表面処理を、塗布装置とは別の表面処理専用装置を用いて行った。表面処理専用装置は、巻き出し部、コロナ放電装置および巻き取り部からなり、コロナ放電電極と、前記コロナ放電電極と対向する接地ロールに巻き掛けられたアルミニウム箔表面との距離は、実施例の場合と同様に０．５ｍｍとした。アルミニウム箔表面へのコロナ放電処理は、前記表面処理専用装置にて、コロナ放電の出力を０．５ｋＷ、走行速度を２０ｍ／ｍｉｎとして行った。一方のアルミニウム箔表面の全面にコロナ放電処理を行い、処理されたアルミニウム箔を巻き取り部で巻き取った後、巻き取ったアルミニウム箔を裏返して、巻き出し部から再度送り出して反対側の表面の全面を処理した。 (Comparative Example 2)
The physical surface treatment of the aluminum foil was performed using a dedicated surface treatment apparatus different from the coating apparatus. The surface treatment dedicated device is composed of an unwinding portion, a corona discharge device, and a winding portion. The distance between the corona discharge electrode and the surface of the aluminum foil wound on the grounding roll facing the corona discharge electrode is the same as in the embodiment. It was set to 0.5 mm as in the case. The corona discharge treatment on the surface of the aluminum foil was carried out with the surface treatment dedicated apparatus at a corona discharge output of 0.5 kW and a traveling speed of 20 m / min. One surface of the aluminum foil is subjected to corona discharge treatment, and the treated aluminum foil is taken up by the take-up portion, and then the wound aluminum foil is turned over and sent out from the unwind portion again. The whole surface was processed.

上記のようにして表面処理専用装置でアルミニウム箔の表面処理を行った以外は、実施例１と全く同じにして正極板を作製した。   A positive electrode plate was produced in exactly the same manner as in Example 1 except that the surface treatment of the aluminum foil was performed by the surface treatment apparatus as described above.

アルミニウム箔表面のぬれ性は、表面処理の直後では、ＪＩＳ Ｋ６７６８に記載された試験方法にて４２ｍＮ／ｍのぬれ張力値があったが、処理から２４時間後に塗布装置にて正極合剤塗膜の塗布を行った直前には３１Ｎ／ｍまで低下していた。この結果、アルミニウム箔上に塗布された正極合剤塗膜の塗工部と未塗工部の境界部４はＬ＝０．８ｍｍの湾曲が生じ、また、塗布開始端部５の厚みも０．０２ｍｍの盛り上がりとなった。また、塗布装置、ロールプレス装置および裁断装置に設置された走行位置矯正装置が動作する度にアルミニウム箔に皺が発生し、幾度もアルミニウム箔の切れが発生した。また、ロールプレス装置では、塗布開始端部５の盛り上がりへの応力集中によるアルミニウム箔の切れも発生した。   As for the wettability of the aluminum foil surface, immediately after the surface treatment, there was a wet tension value of 42 mN / m by the test method described in JIS K6768. Immediately before the application of was reduced to 31 N / m. As a result, the boundary portion 4 between the coated portion and the uncoated portion of the positive electrode mixture coating film coated on the aluminum foil is curved with L = 0.8 mm, and the thickness of the coating start end portion 5 is also 0. The climax was .02mm. In addition, wrinkles were generated in the aluminum foil every time the running position correction device installed in the coating device, roll press device, and cutting device was operated, and the aluminum foil was cut several times. Further, in the roll press apparatus, the aluminum foil was cut due to stress concentration on the rising of the coating start end 5.

（比較例３）
正極合剤塗膜が形成される塗工部、正極合剤塗膜が形成されない未塗工部に関わらず、アルミニウム箔の表面全体にコロナ放電処理を行った以外は、実施例２と全く同じにして、正極板を作製した。 (Comparative Example 3)
Except for the coated part where the positive electrode mixture coating film is formed and the uncoated part where the positive electrode mixture coating film is not formed, the same as Example 2 except that the entire surface of the aluminum foil was subjected to corona discharge treatment. Thus, a positive electrode plate was produced.

アルミニウム箔表面のぬれ性は、ＪＩＳ Ｋ６７６８に記載された試験方法にて４２ｍＮ／ｍのぬれ張力値となった。このアルミニウム箔上に塗布された正極合剤塗膜の塗工部
と未塗工部の境界部の湾曲は生じず、また、塗布開始端部の厚みも０．００４ｍｍの盛り上がりしか発生しなかった。 The wettability of the aluminum foil surface was a wet tension value of 42 mN / m by the test method described in JIS K6768. No bending occurred at the boundary between the coated portion and the uncoated portion of the positive electrode mixture coating film coated on the aluminum foil, and the thickness of the coating start end portion was raised only by 0.004 mm. .

しかし、実施例２とは異なり、塗布装置、ロールプレス装置および裁断装置において、アルミニウム箔の皺が発生し、幾度もアルミニウム箔の切れが発生した。   However, unlike Example 2, in the coating apparatus, roll press apparatus, and cutting apparatus, aluminum foil wrinkles occurred and the aluminum foil was cut several times.

以上のように作製した実施例１、実施例２、実施例３および比較例１、比較例２、比較例３の正極板にセパレータを介在させて負極板とともに捲回した電極群を、ケースに電解液とともに挿入、封止してリチウムイオン二次電池を作製し、その電池性能を評価した。電池性能の評価は、最大電流１４００ｍＡ、上限電圧４．２Ｖまでの定電流充電を行った後、さらに４．２Ｖの定電圧で１００ｍＡまでの充電、および２０００ｍＡ、放電終止電圧３．０Ｖとした定電流放電を繰り返して行った。３サイクル目の放電容量を１００％として、１００サイクルを経過した電池の容量維持率を算出し、容量維持率とした。   An electrode group wound together with a negative electrode plate with a separator interposed in the positive electrode plate of Examples 1, Example 2, Example 3, Comparative Example 1, Comparative Example 2, and Comparative Example 3 produced as described above is used as a case. A lithium ion secondary battery was prepared by inserting and sealing together with the electrolytic solution, and the battery performance was evaluated. The battery performance was evaluated by performing constant current charging up to a maximum current of 1400 mA and an upper limit voltage of 4.2 V, then charging up to 100 mA with a constant voltage of 4.2 V, and 2000 mA and a discharge end voltage of 3.0 V. The current discharge was repeated. The discharge capacity at the third cycle was assumed to be 100%, and the capacity retention rate of the battery after 100 cycles was calculated and used as the capacity retention rate.

Figure 2008270004
Figure 2008270004

表１に示されるように、比較例１および比較例２の電池では、他に比べて顕著に電池性能が劣っていた。評価後の電池を分解したところ、比較例１および比較例２のリチウムイオン二次電池では、正極合剤塗膜の塗布開始端部近傍がアルミニウム箔から浮き上がっていたのに対し、他の電池では塗布開始端部はアルミニウム箔と密着した状態を保持しており、これが比較例１および比較例２の電池性能低下の原因であったものと考えられる。   As shown in Table 1, the batteries of Comparative Example 1 and Comparative Example 2 were significantly inferior in battery performance as compared with others. When the battery after evaluation was disassembled, in the lithium ion secondary batteries of Comparative Example 1 and Comparative Example 2, the vicinity of the coating start end of the positive electrode mixture coating film was lifted from the aluminum foil, whereas in other batteries, The application start end portion is kept in close contact with the aluminum foil, and this is considered to be the cause of the battery performance deterioration in Comparative Examples 1 and 2.

また、比較例２の電池では、電池性能の評価中に発熱が生じ、評価を中断した電池が多数含まれ、発火に至るものもあった。発熱を生じた電池を分解したところ、セパレータを
貫通する導電性の異物の存在が認められた。これは、比較例２の電池は、塗布装置とは別の装置にてコロナ放電処理を施しており、表裏両面を処理するために表面処理装置にてアルミニウム箔を２回走行させる必要があったため、処理装置の搬送ロール表面に存在した異物等がコロナ放電処理されて、ぬれ性が高められたアルミニウム箔表面に多量に付着したことが原因と考えられる。 In addition, the battery of Comparative Example 2 generated heat during the evaluation of battery performance, and included many batteries whose evaluation was interrupted, leading to ignition. When the battery that generated heat was disassembled, the presence of conductive foreign matter penetrating the separator was observed. This is because the battery of Comparative Example 2 was subjected to corona discharge treatment by a device different from the coating device, and it was necessary to run the aluminum foil twice by the surface treatment device in order to treat both the front and back surfaces. It is thought that the cause is that a large amount of foreign matter or the like present on the surface of the transport roll of the processing apparatus has been subjected to corona discharge treatment and adhered to the aluminum foil surface with improved wettability.

実施例１〜実施例３の電池は、いずれも電池性能に優れ、発熱・発火を生じることなく安全性も優れていた。その中でも、アルミニウム箔表面のぬれ張力値が３５Ｎ／ｍ以上であった実施例２および実施例３の電池が特に優れた結果を示した。   The batteries of Examples 1 to 3 were all excellent in battery performance, and were excellent in safety without generating heat and ignition. Among them, the batteries of Example 2 and Example 3 in which the wetting tension value on the surface of the aluminum foil was 35 N / m or more showed particularly excellent results.

本実施例では、物理的放電処理を施す方法として、コロナ放電によるアルミニウム箔の表面処理およびコロナ放電により処理されたアルミニウム箔を集電体として用いた正極板による例を示したが、本発明は本実施例に限定されるものではない。   In this example, as a method of performing physical discharge treatment, an example of a surface treatment of an aluminum foil by corona discharge and a positive electrode plate using an aluminum foil treated by corona discharge as a current collector was shown. The present invention is not limited to this embodiment.

表面処理を施す対象については、アルミニウム箔以外の他の金属箔であってもよく、特に、その製造過程で圧延工程が含まれている金属箔については効果が顕著である。   The object to be subjected to the surface treatment may be a metal foil other than the aluminum foil, and the effect is particularly remarkable for the metal foil in which the rolling process is included in the manufacturing process.

表面処理された金属箔を集電体として用いるのは、正極板および負極板のいずれであっても効果に変わりはない。   The use of the surface-treated metal foil as the current collector is the same regardless of whether the positive electrode plate or the negative electrode plate is used.

物理的表面処理の方法については、金属箔表面のぬれ性を高められるものであればその方法を限定されるものではなく、本実施例で示したコロナ放電処理以外にも、コロナプラズマ処理、紫外線照射処理、レーザー処理等を用いても同様の効果が期待できることは言うまでもない。   The method of physical surface treatment is not limited as long as the wettability of the surface of the metal foil can be improved. Besides the corona discharge treatment shown in this embodiment, corona plasma treatment, ultraviolet ray It goes without saying that the same effect can be expected even when irradiation treatment, laser treatment, or the like is used.

本発明にかかるリチウムイオン二次電池の製造方法によると、アルミニウム箔表面の合剤塗膜を形成する部分に物理的表面処理を施し、合剤塗膜が形成されない部分の一部または全部には前記物理的表面処理を施さないことによって、湾曲や盛り上がりのない良好な塗布開始端部を形成することができ、優れた電池性能のリチウムイオン二次電池が得られるとともに、製造過程におけるアルミニウム箔の切れや皺の発生が生じることなく、高い歩留まりおよび生産性でリチウムイオン二次電池を製造することが可能となる。   According to the method for producing a lithium ion secondary battery according to the present invention, a physical surface treatment is applied to a portion of the aluminum foil surface where the mixture coating film is formed, and a part or all of the portion where the mixture coating film is not formed is applied. By not performing the physical surface treatment, it is possible to form a good coating start end without bending or bulging, and to obtain a lithium ion secondary battery with excellent battery performance, and the aluminum foil in the manufacturing process It is possible to manufacture a lithium ion secondary battery with high yield and productivity without occurrence of cutting or wrinkles.

金属箔に合剤塗膜を塗布した状態を示す模式図Schematic diagram showing a state in which a mixture coating film is applied to a metal foil 脱脂が不十分なアルミニウム箔に合剤塗膜を塗布した状態を示す模式図Schematic diagram showing a state in which a mixture coating film is applied to an aluminum foil with insufficient degreasing 図２のＡ−Ａ線断面図AA line sectional view of FIG. 本発明のリチウムイオン二次電池の製造方法に用いる塗布装置の一実施の形態を示す模式図The schematic diagram which shows one Embodiment of the coating device used for the manufacturing method of the lithium ion secondary battery of this invention

符号の説明Explanation of symbols

１ 集電体
２ 塗工部
３ 未塗工部
４ 境界部
５ 塗工開始端部
６ 巻き出し部
７ 物理的表面処理装置
８ 塗布器
９ 乾燥器
１０巻き取り部
１１フープ
１２フープ
Ａ 長手方向
Ｂ 幅方向 DESCRIPTION OF SYMBOLS 1 Current collector 2 Coating part 3 Uncoated part 4 Boundary part 5 Coating start edge part 6 Unwinding part 7 Physical surface treatment apparatus 8 Applicator 9 Dryer 10 Winding part 11 Hoop 12 Hoop A Longitudinal direction B Width direction

Claims (5)

帯状の金属箔が巻き取られたフープから前記金属箔を連続的に送り出す工程と、送り出された金属箔のいずれか一方の表面に物理的表面処理を間欠的に施す工程と、金属箔の物理的表面処理された部分の一部または全部の表面に塗料を塗布して塗膜を形成する工程と、前記塗膜中の揮発成分を除去する工程と、揮発成分が除去された塗膜が表面に形成された金属箔を連続的にフープに巻き取る工程を少なくとも有するリチウムイオン二次電池の製造方法。   A step of continuously feeding out the metal foil from a hoop in which a band-shaped metal foil is wound up, a step of intermittently performing a physical surface treatment on the surface of any one of the fed metal foils, A step of forming a coating film by applying a paint to a part or all of the surface of the part subjected to a surface treatment, a step of removing volatile components in the coating film, and a coating film from which volatile components have been removed A method for producing a lithium ion secondary battery comprising at least a step of continuously winding a metal foil formed on a hoop. 前記金属箔の物理的表面処理が施された部分の２５℃における表面張力が、ＪＩＳ Ｋ６７６８に記載された試験方法によって測定されたぬれ張力値で３５ｍＮ／ｍ以上である請求１に記載のリチウムイオン二次電池の製造方法。   2. The lithium ion according to claim 1, wherein a surface tension at 25 ° C. of a portion of the metal foil subjected to a physical surface treatment is 35 mN / m or more in terms of a wetting tension value measured by a test method described in JIS K6768. A method for manufacturing a secondary battery. 請求項１または２のいずれかの方法によって、製造されたリチウムイオン二次電池。   A lithium ion secondary battery produced by the method according to claim 1. 少なくとも、帯状の金属箔を連続的に送り出す手段と、前記金属箔のいずれか一方の表面に物理的表面処理を間欠的に施すことができる手段と、金属箔の物理的表面処理された部分の一部または全部の表面に塗料を塗布して塗膜を形成する手段と、前記塗膜中の揮発成分を除去する手段と、揮発成分が除去された塗膜が表面に形成された金属箔を連続的にフープに巻き取る手段を少なくとも、備えた塗布装置。   At least means for continuously feeding a strip-shaped metal foil, means for intermittently applying a physical surface treatment to one of the surfaces of the metal foil, and a physical surface-treated portion of the metal foil. Means for applying a paint to a part or all of the surface to form a coating film; means for removing volatile components in the coating film; and a metal foil having a coating film from which volatile components have been removed formed on the surface. An applicator comprising at least means for continuously winding on a hoop. 前記塗布装置における隣接する金属箔の搬送用ロール間の最も短い距離が、前記物理的表面処理が間欠的に施された金属箔の物理的表面処理がされていない部分の長さより短いことを特徴とする請求項４に記載の塗布装置。   The shortest distance between adjacent metal foil transport rolls in the coating apparatus is shorter than the length of the portion of the metal foil that has been subjected to the physical surface treatment that has not been subjected to physical surface treatment. The coating apparatus according to claim 4.
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