JP2006260892A - Electrode plate for nonaqueous electrolyte secondary battery and its manufacturing method, and nonaqueous electrolyte secondary battery using the above electrode plate - Google Patents
Electrode plate for nonaqueous electrolyte secondary battery and its manufacturing method, and nonaqueous electrolyte secondary battery using the above electrode plate Download PDFInfo
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Abstract
Description
本発明は、リチウムイオン二次電池に代表される非水電解液二次電池用の電極、当該電極の製造方法、及び、それらを用いた非水電解液二次電池に関する。 The present invention relates to an electrode for a non-aqueous electrolyte secondary battery represented by a lithium ion secondary battery, a method for producing the electrode, and a non-aqueous electrolyte secondary battery using them.
非水電解液二次電池、代表的にはリチウムイオン二次電池は、高エネルギー密度で高電圧を有し、且つ軽量性に優れることから、駆動機器、携帯電子機器、電気自動車等、種々の分野で用いられている。 Non-aqueous electrolyte secondary batteries, typically lithium ion secondary batteries, have high energy density, high voltage, and excellent lightness. Used in the field.
有機電解液を主成分とする非水電解質を用いる非水電解液二次電池では、非水電解質の電気伝導度が水系電解質に比べて低いので、電極板を薄くする必要がある。また、大電流を取り出すには反応面積を大きくする必要があるため、正、負の電極板をシート状にし、これらの電極板をセパレータを介してロール状に捲回した構造等が採用されている。 In a non-aqueous electrolyte secondary battery using a non-aqueous electrolyte containing an organic electrolyte as a main component, the electric conductivity of the non-aqueous electrolyte is lower than that of an aqueous electrolyte, so that the electrode plate needs to be thin. Also, since it is necessary to increase the reaction area in order to extract a large current, a structure in which the positive and negative electrode plates are formed into a sheet shape and these electrode plates are wound in a roll shape through a separator is adopted. Yes.
電気自動車等に用いられる大型の非水電解液二次電池では、高出力かつ充放電時の発熱を抑えるため、電極を積層した電池、または電極を捲回し、捲回の周回ごとにリード線をとった電池がある。積層型の電池では電極を切り抜くか又は打ち抜いて、セパレータを挟んで積層させる。一方、捲回型電池では、電極の片側に未塗工部を作り、その未塗工部にリード線をタブ付け溶接して集電する方法が開示されている（特許文献１、２）。しかし、この方法では作業中に未塗工部が変形し易く、作業性が悪かった。
For large non-aqueous electrolyte secondary batteries used in electric vehicles, etc., in order to suppress heat generation during high output and charge / discharge, a battery with stacked electrodes or electrodes is wound and a lead wire is provided for each turn. There is a battery that I took. In a stacked battery, electrodes are cut out or punched out and stacked with a separator interposed therebetween. On the other hand, in a wound battery, a method is disclosed in which an uncoated portion is formed on one side of an electrode and a lead wire is tabbed and welded to the uncoated portion to collect current (
また、電極板にリード線をタブ付けするための方法としては、導電性基材の生地部を形成するために、従来から、活物質層用塗工組成物の塗布、乾燥により形成された活物質層を除去することが行なわれている。除去する方法として、一対のナイフ材で筋入れを行なうとともに筋間の活物質層をスリ割フライスにより削り落とす方法（特許文献３）や、両面に塗布された活物質層の上下両方向から刃状体を当接し、活物質層を剥離除去する方法（特許文献４）が提案されている。しかしこれらの方法では、活物質層の剥離除去という余分な作業工程を必要とするだけでなく、除去しきれなかった活物質層があった場合、その影響でリード線のタブ付け溶接が困難であった。 In addition, as a method for attaching a lead wire to an electrode plate, an active material layer formed by applying and drying an active material layer coating composition has been conventionally used to form a fabric portion of a conductive substrate. The material layer is removed. As a method of removing, a method of scoring the active material layer between the muscles with a pair of knife materials and scraping off the active material layer with a slit mill (Patent Document 3), or an edge shape from both the upper and lower directions of the active material layer applied on both sides There has been proposed a method (Patent Document 4) in which a body is brought into contact with and an active material layer is peeled and removed. However, these methods not only require an extra work step of stripping and removing the active material layer, but also when there is an active material layer that could not be removed, it is difficult to perform tab welding of the lead wire due to the effect. there were.
導電性基材の生地部を形成するための方法としては、特許文献５には、特定の粘性を有する電極材料塗布液を、塗布液供給システムに接続されたダイノズルによって吐出させ、走行する導電性基材上に、長手方向の一定間隔ごとに未塗布部を設けながら前記塗布液を塗布することを特徴とするシート状電極板の製造方法が開示されている。
As a method for forming a fabric portion of a conductive base material,
本発明は上記の実状に鑑みて成し遂げられたものであり、その第一の目的は、電極板が変形することなく捲回する時に重なるようにリード線をとることが可能で、電池反応の効率がよいため、体積あたりのエネルギー量が高く、且つリード線の取り付けが容易で効率的に生産可能な非水電解液二次電池用の正極板と負極板の組み合わせを提供することにある。 The present invention has been accomplished in view of the above circumstances, and the first object of the present invention is to allow lead wires to overlap when the electrode plate is wound without being deformed, and the efficiency of the battery reaction. Therefore, an object of the present invention is to provide a combination of a positive electrode plate and a negative electrode plate for a non-aqueous electrolyte secondary battery that has a high energy amount per volume, can be easily attached to a lead wire, and can be produced efficiently.
また、本発明の第二の目的は、電極板が変形することなく捲回する時に重なるようにリード線をとることが可能で、電池反応の効率がよいため、体積あたりのエネルギー量が高く、且つリード線の取り付けが容易で効率的に生産可能な非水電解液二次電池用電極板の正極板と負極板の製造方法を提供することにある。 In addition, the second object of the present invention is that it is possible to take lead wires so as to overlap when the electrode plate is wound without being deformed, and since the efficiency of the battery reaction is good, the energy amount per volume is high, Another object of the present invention is to provide a method for producing a positive electrode plate and a negative electrode plate of an electrode plate for a non-aqueous electrolyte secondary battery that can be easily and efficiently produced by attaching lead wires.
また、本発明の第三の目的は、上記電極板を用いて、電池反応の効率がよく、高出力且つ充放電時の発熱を抑えることが可能な非水電解液二次電池を提供することにある。 A third object of the present invention is to provide a non-aqueous electrolyte secondary battery that uses the above electrode plate and has a high battery reaction efficiency, high output, and can suppress heat generation during charging and discharging. It is in.
本発明に係る非水電解液二次電池用の正極板と負極板の組み合わせは、該正極板と該負極板とが集電体と該集電体の少なくとも一面へ所定パターン状に設けられた電極活物質層を備え、該パターン形状は少なくとも集電体の長手方向へ電極活物質層が間欠的に配置されてなり、該正極板と該負極板の間にセパレータを挟んで重ねて捲回する時に正負両極の活物質層の非塗布部同士及び正負両極の活物質層の塗布部同士が同位置に重なるように、集電体の長手方向の各電極活物質層のピッチが異なることを特徴とする。 In the combination of the positive electrode plate and the negative electrode plate for the non-aqueous electrolyte secondary battery according to the present invention, the positive electrode plate and the negative electrode plate are provided in a predetermined pattern on at least one surface of the current collector and the current collector. An electrode active material layer is provided, and the pattern shape is such that at least the electrode active material layer is intermittently arranged in the longitudinal direction of the current collector, and the separator is sandwiched between the positive electrode plate and the negative electrode plate and wound The pitch of the electrode active material layers in the longitudinal direction of the current collector is different so that the non-coated portions of the positive and negative active material layers and the coated portions of the positive and negative active material layers overlap at the same position. To do.
また、本発明に係る非水電解液二次電池用電極板の正極板と負極板の製造方法は、集電体へ電極活物質層用塗工組成物を塗布する塗布部と塗布しない非塗布部とを、当該各塗布部のピッチが異なるように、集電体の塗布流れ方向へ設けることにより、該正極板と該負極板の間にセパレータを挟んで重ねて捲回する時に正負両極の活物質層の非塗布部同士及び正負両極の活物質層の塗布部同士が同位置に重なるような所定パターン状に電極活物質層を形成する工程を少なくとも有することを特徴とする。 In addition, the method for producing the positive electrode plate and the negative electrode plate of the electrode plate for a non-aqueous electrolyte secondary battery according to the present invention includes an application part for applying the coating composition for the electrode active material layer to the current collector and an unapplied non-application Are provided in the application flow direction of the current collector so that the pitches of the respective application parts are different, so that a positive and negative electrode active material is wound when the positive electrode plate and the negative electrode plate are sandwiched and wound. It has at least a step of forming the electrode active material layer in a predetermined pattern so that the non-coated portions of the layers and the coated portions of the positive and negative active material layers overlap at the same position.
また、本発明に係る非水電解液二次電池は、上記本発明に係る非水電解液二次電池用の正極板と負極板の組み合わせを備えることを特徴とする。 The non-aqueous electrolyte secondary battery according to the present invention includes a combination of a positive electrode plate and a negative electrode plate for the non-aqueous electrolyte secondary battery according to the present invention.
本発明においては、前記各電極活物質層のピッチが、正極板と負極板を重ね合わせて捲回する時に、正負両極の活物質層の塗布部が同位置に重なるように設定されているため、電池反応の効率がよく、体積あたりのエネルギー量が高い。従って、この正極板と負極板の組み合わせを二次電池に用いることにより、高出力が得られ、且つ、充放電時の発熱を抑えることが可能である。 In the present invention, the pitch of the electrode active material layers is set so that the application portions of the positive and negative active material layers overlap at the same position when the positive electrode plate and the negative electrode plate are wound together. Battery reaction efficiency is good and energy per volume is high. Therefore, by using the combination of the positive electrode plate and the negative electrode plate for the secondary battery, high output can be obtained and heat generation during charging / discharging can be suppressed.
また、本発明においては、少なくとも集電体の長手方向へ電極活物質層が間欠的に配置されてなる正極板と負極板を捲回する時に、正負両極の活物質層の非塗布部が同位置に重なるように、集電体の長手方向の各電極活物質層のピッチが異なるため、当該ピッチに含まれる非塗布部にリード線を取り付けることにより、電極板が変形することなく、捲回する時に正極板のリード線同士および負極板のリード線同士が、それぞれ重なるようにリード線をとることが可能である。
従って、非塗布部にリード線を取り付けるためリード線の取り付けが容易で、且つ効率的に生産可能である。また、正極板のリード線群の配置と負極板のリード線群の配置をそれぞれまとめるため、異極間のリード線の接触を確実に防止することが出来る。
Further, in the present invention, when winding the positive electrode plate and the negative electrode plate in which the electrode active material layer is intermittently arranged at least in the longitudinal direction of the current collector, the non-coated portions of the positive and negative active material layers are the same. Since the pitch of each electrode active material layer in the longitudinal direction of the current collector is different so as to overlap the position, by attaching a lead wire to the non-coated part included in the pitch, the electrode plate is not deformed and wound. In this case, the lead wires can be taken so that the lead wires of the positive electrode plate and the lead wires of the negative electrode plate overlap each other.
Therefore, since the lead wire is attached to the non-application portion, the lead wire can be easily attached and can be produced efficiently. In addition, since the arrangement of the lead wire group of the positive electrode plate and the arrangement of the lead wire group of the negative electrode plate are combined, it is possible to reliably prevent the contact of the lead wires between the different electrodes.
本発明に係る非水電解液二次電池用電極板は、集電体と該集電体の少なくとも一面へ所定パターン状に設けられた電極活物質層を備えた非水電解液二次電池用の正極板と負極板の組み合わせにおいて、該パターン形状は少なくとも集電体の長手方向へ電極活物質層が間欠的に配置されてなり、該正極板と該負極板の間にセパレータを挟んで重ねて捲回する時に正負両極の活物質層の非塗布部同士及び正負両極の活物質層の塗布部同士が、それぞれ同位置にぴったりと重なるように、集電体の長手方向の各電極活物質層のピッチが異なることを特徴とする。 An electrode plate for a non-aqueous electrolyte secondary battery according to the present invention is for a non-aqueous electrolyte secondary battery including a current collector and an electrode active material layer provided in a predetermined pattern on at least one surface of the current collector. In the combination of the positive electrode plate and the negative electrode plate, the pattern shape is such that at least the electrode active material layer is intermittently disposed in the longitudinal direction of the current collector, and a separator is sandwiched between the positive electrode plate and the negative electrode plate. When rotating, the non-coated portions of the positive and negative active material layers and the coated portions of the positive and negative active material layers overlap each other exactly at the same position. The pitch is different.
また、本発明に係る非水電解液二次電池用の正極板と負極板の製造方法は、集電体へ電極活物質層用塗工組成物を塗布する塗布部と塗布しない非塗布部とを、当該各塗布部のピッチが異なるように、集電体の塗布流れ方向へ設けることにより、正極板と負極板の間にセパレータを挟んで重ねて捲回する時に正負両極の活物質層の非塗布部同士及び正負両極の活物質層の塗布部が同位置にぴったりと重なるような所定パターン状に電極活物質層を形成する工程を少なくとも有することを特徴とするものである。 In addition, a method for producing a positive electrode plate and a negative electrode plate for a non-aqueous electrolyte secondary battery according to the present invention includes an application part for applying a coating composition for an electrode active material layer to a current collector, and a non-application part not applied. Is provided in the direction of application of the current collector so that the pitch of each application part is different, so that the positive and negative electrode active material layers are not applied when winding with the separator sandwiched between the positive electrode plate and the negative electrode plate. It has at least a step of forming the electrode active material layer in a predetermined pattern so that the portions and the application portions of the positive and negative active material layers exactly overlap at the same position.
本発明に用いる正極板は、少なくとも正極活物質及び結着材を含有する正極用活物質層塗工組成物を集電体の少なくとも一面に塗布して、正極活物質層を形成することによって作製される。
一方、負極板は、少なくとも負極活物質及び結着材を含有する負極用活物質層塗工組成物を集電体の少なくとも一面に塗布して、負極活物質層を形成することによって作製される。
The positive electrode plate used in the present invention is prepared by applying a positive electrode active material layer coating composition containing at least a positive electrode active material and a binder to at least one surface of a current collector to form a positive electrode active material layer. Is done.
On the other hand, the negative electrode plate is produced by applying a negative electrode active material layer coating composition containing at least a negative electrode active material and a binder to at least one surface of a current collector to form a negative electrode active material layer. .
正極活物質としては、従来から非水電解液二次電池の正極活物質として用いられている材料を用いることができ、例えば、ＬｉＭｎ2Ｏ4（マンガン酸リチウム）、ＬｉＣｏＯ2（コバルト酸リチウム）若しくはＬｉＮｉＯ2（ニッケル酸リチウム）等のリチウム酸化物、または、ＴｉＳ2、ＭｎＯ2、ＭｏＯ3もしくはＶ2Ｏ5等のカルコゲン化合物を例示することができる。 As the positive electrode active material, it is possible to use a material used as a positive electrode active material of nonaqueous electrolyte secondary batteries conventionally, for example, LiMn 2 O 4 (lithium manganate), LiCoO 2 (lithium cobaltate) Alternatively, a lithium oxide such as LiNiO 2 (lithium nickelate) or a chalcogen compound such as TiS 2 , MnO 2 , MoO 3, or V 2 O 5 can be exemplified.
正極活物質は、塗工層中に均一に分散させるために、１〜１００μｍの範囲の粒径を有し、且つ平均粒径が約１０μｍの粉体であることが好ましい。これらの正極用活物質は単独で用いてもよいし、２種以上を組み合わせて用いてもよい。 The positive electrode active material is preferably a powder having a particle size in the range of 1 to 100 μm and an average particle size of about 10 μm so as to be uniformly dispersed in the coating layer. These positive electrode active materials may be used alone or in combination of two or more.
一方、負極活物質としては、従来から非水電解液二次電池の負極活物質として用いられている材料を用いることができ、例えば、天然グラファイト、人造グラファイト、アモルファス炭素、カーボンブラック、または、これらの成分に異種元素を添加したもののような炭素質材料が好んで用いられる。溶媒が有機系の場合には金属リチウムまたはリチウム合金のようなリチウム含有金属が好適に用いられる。 On the other hand, as the negative electrode active material, materials conventionally used as the negative electrode active material of non-aqueous electrolyte secondary batteries can be used. For example, natural graphite, artificial graphite, amorphous carbon, carbon black, or these Carbonaceous materials such as those obtained by adding different elements to these components are preferably used. When the solvent is organic, a lithium-containing metal such as lithium metal or a lithium alloy is preferably used.
負極活物質の粒子形状は特に限定されないが、例えば、鱗片状、塊状、繊維状、球状のものが使用可能である。負極活物質は、塗工層中に均一に分散させるために、１〜１００μｍの範囲の粒径を有し、且つ平均粒径が約１０μｍの粉体であることが好ましい。これらの負極用活物質は単独で用いてもよいし、２種以上を組み合わせて用いてもよい。 Although the particle shape of a negative electrode active material is not specifically limited, For example, a flaky shape, a lump shape, a fiber shape, and a spherical shape can be used. The negative electrode active material is preferably a powder having a particle size in the range of 1 to 100 μm and an average particle size of about 10 μm so as to be uniformly dispersed in the coating layer. These negative electrode active materials may be used alone or in combination of two or more.
塗工組成物中の正極又は負極活物質の配合割合は、溶剤を除く配合成分を基準（固形分基準）とした時に通常は９０〜９８．５重量％とする。 The blending ratio of the positive electrode or negative electrode active material in the coating composition is usually 90 to 98.5% by weight, based on the blending components excluding the solvent (solid content basis).
結着材としては従来から用いられているもの、例えば、熱可塑性樹脂、より具体的にはポリエステル樹脂、ポリアミド樹脂、ポリアクリル酸エステル樹脂、ポリカーボネート樹脂、ポリウレタン樹脂、セルロース樹脂、ポリオレフィン樹脂、ポリビニル樹脂、フッ素系樹脂またはポリイミド樹脂等を使用することができる。この際、反応性官能基を導入したアクリレートモノマーまたはオリゴマーを結着材中に混入させることも可能である。そのほかにも、ゴム系の樹脂や、アクリル樹脂、ウレタン樹脂等の熱硬化性樹脂、アクリレートモノマー、アクリレートオリゴマー或いはそれらの混合物からなる電離放射線硬化性樹脂、上記各種の樹脂の混合物を使用することもできる。 Conventionally used binders such as thermoplastic resins, more specifically polyester resins, polyamide resins, polyacrylate resins, polycarbonate resins, polyurethane resins, cellulose resins, polyolefin resins, polyvinyl resins Fluorine resin or polyimide resin can be used. At this time, an acrylate monomer or oligomer into which a reactive functional group is introduced can be mixed in the binder. In addition, rubber-based resins, thermosetting resins such as acrylic resins and urethane resins, ionizing radiation curable resins composed of acrylate monomers, acrylate oligomers or mixtures thereof, and mixtures of the above various resins may be used. it can.
塗工組成物中の結着材の配合割合は、固形分基準で通常は０．５〜１０重量％、好ましくは３〜６重量％とする。 The blending ratio of the binder in the coating composition is usually 0.5 to 10% by weight, preferably 3 to 6% by weight, based on the solid content.
正極又は負極用活物質層塗工組成物には、導電剤を添加しても良い。導電剤としては、例えば、グラファイト、カーボンブラックまたはアセチレンブラック等の炭素質材料が必要に応じて用いられる。塗工組成物中の導電剤の配合割合は、通常、固形分基準で１．５〜１０．０重量％とする。 A conductive agent may be added to the positive electrode or negative electrode active material layer coating composition. As the conductive agent, for example, a carbonaceous material such as graphite, carbon black, or acetylene black is used as necessary. The blending ratio of the conductive agent in the coating composition is usually 1.5 to 10.0% by weight based on the solid content.
正極又は負極用活物質層塗工組成物を調製する溶剤としては、トルエン、メチルエチルケトン、Ｎ−メチル−２−ピロリドン或いはこれらの混合物のような有機溶剤を用いることができる。塗工組成物中の溶剤の割合は、通常は３０〜６０重量％、好ましくは４５〜５５重量％とし、塗工液をスラリー状に調製する。 As a solvent for preparing the positive electrode or negative electrode active material layer coating composition, an organic solvent such as toluene, methyl ethyl ketone, N-methyl-2-pyrrolidone, or a mixture thereof can be used. The ratio of the solvent in the coating composition is usually 30 to 60% by weight, preferably 45 to 55% by weight, and the coating liquid is prepared in a slurry form.
正極又は負極活物質層用塗工組成物は、適宜選択した正極又は負極活物質、結着材、及び他の配合成分を適切な溶剤中にいれ、ホモジナイザー、ボールミル、サンドミル、ロールミルまたはプラネタリーミキサー等の分散機により混合分散して、スラリー状に調製できる。 The coating composition for the positive electrode or negative electrode active material layer is prepared by adding a suitably selected positive electrode or negative electrode active material, binder, and other compounding components in an appropriate solvent, and homogenizer, ball mill, sand mill, roll mill or planetary mixer. It can be mixed and dispersed by a dispersing machine such as a slurry to prepare a slurry.
このようにして調製された正極又は負極活物質層用塗工組成物を、基体である集電体の少なくとも一面に塗布・乾燥して正極又は負極活物質層を形成する。正極板の集電体としては通常、アルミニウム箔が好ましく用いられる。一方、負極板の集電体としては、電解銅箔や圧延銅箔等の銅箔が好ましく用いられる。集電体の厚さは通常、５〜５０μｍ程度とする。 The positive electrode or negative electrode active material layer coating composition thus prepared is applied to and dried on at least one surface of a current collector as a substrate to form a positive electrode or negative electrode active material layer. In general, an aluminum foil is preferably used as the current collector of the positive electrode plate. On the other hand, as the current collector of the negative electrode plate, a copper foil such as an electrolytic copper foil or a rolled copper foil is preferably used. The thickness of the current collector is usually about 5 to 50 μm.
特に、本発明においては、集電体へ電極活物質層用塗工組成物を塗布する塗布部と塗布しない非塗布部とを、当該各塗布部のピッチが異なるように、集電体の塗布流れ方向へ設けることにより、正極板と負極板の間にセパレータを挟んで捲回する時に正極活物質層と負極活物質層の非塗布部同士、及び、正極活物質層と負極活物質層の塗布部同士が、それぞれ同位置にぴったりと重なるような所定パターン状に電極活物質層を形成する。
図１は、本発明の非水電解液二次電池用電極板１の一例を模式的に示した図であり、集電体２の少なくとも一面に、集電体２の長手方向へ電極活物質層３が間欠的に、すなわち電極活物質層３と非塗布部４が交互に配置されてなり、集電体２の長手方向の各電極活物質層３のピッチ（５（１）、５（２）、・・・５（ｎ））が異なっている。上記電極活物質層（塗布部）のピッチとは、各電極活物質層（塗布部）の集電体の長手方向（塗布流れ方向）の一辺の長さの起点（又は終点）６と、当該電極活物質層（塗布部）に隣接する電極活物質層（塗布部）の集電体の長手方向（塗布流れ方向）の同じ側の一辺の長さの起点（又は終点）６との間の距離をいう。
In particular, in the present invention, the application of the current collector is performed so that the application part for applying the electrode active material layer coating composition to the current collector and the non-application part not applied are different in pitch of the application parts. By providing in the flow direction, when the separator is sandwiched between the positive electrode plate and the negative electrode plate, the non-coated portions of the positive electrode active material layer and the negative electrode active material layer, and the coated portions of the positive electrode active material layer and the negative electrode active material layer The electrode active material layers are formed in a predetermined pattern so that they overlap each other exactly at the same position.
FIG. 1 is a diagram schematically showing an example of an
各塗布部のピッチが異なるとは、ランダムに異なることも、所定の規則性を持って異なることも含まれる。 That the pitch of each application part is different includes different randomly and differently with a predetermined regularity.
前記各電極活物質層のピッチは、電池１セル分全体で、又は電池１セル分の中で２以上に分けられた領域の少なくとも１つの領域で、集電体の長手方向に向かって次第に大きくなるか又は次第に小さくなることが、捲回する時に重なるようにリード線をとることが可能になる点から好ましい。なお、電池１セル分９とは、電池１セルに使用する電極板の部分をいう。本発明の電極板は、電池１セル分９が複数個提供できるような長尺の電極板であっても良く、例えば図１に示されるように、電池１セル分９毎の間には、電池作製に使用されない電極活物質層や非塗布部を含んでいても良い。
The pitch of each electrode active material layer is gradually increased in the longitudinal direction of the current collector in the whole battery cell or in at least one region divided into two or more in one battery cell. It is preferable that the lead wire can be taken so as to overlap when winding. The
前記各電極活物質層のピッチが、電池１セル分全体で、集電体の長手方向に向かって次第に大きくなるか又は次第に小さくなる場合の一例としては、図１のような場合が挙げられる。また、電池１セル分の中で２以上に分けられた領域の少なくとも１つの領域で、集電体の長手方向に向かって次第に大きくなるか又は次第に小さくなる場合の一例としては、図２（ａ）のように、電池１セル分の中で３つに分けられた領域１０（１）、１０（２）、１０（３）のうち、１０（２）において、各電極活物質層のピッチが集電体の長手方向に向かって次第に大きくなるか又は次第に小さくなっている場合が挙げられる。また別の一例としては、図２（ｂ）のように、電池１セル分の中で４つに分けられた領域１０（１）、１０（２）、１０（３）、１０（４）のうち、１０（２）及び１０（３）において各々別のピッチで次第に大きくなるか又は次第に小さくなる場合等が挙げられる。
例えば、図２（ｂ）のような、電池１セル分の中で２以上に分けられた領域の２以上において、各電極活物質層のピッチが集電体の長手方向に向かって次第に大きくなるか又は次第に小さくなっている場合には、捲回時に、巻きの内側部におけるリード線を付ける周回数と、巻きの外側部におけるリード線を付ける周回数とを変えていくことが可能になる。例えば、捲回時に、巻きの内側部においては４周回ごとにリード線を付け、巻きの外側部においては３周回ごとにリード線を付けること等ができるようになる。捲回時に、リード線を付ける周回数を適宜調節することにより、非塗布部を最小限に減らして電池容量を上げながら良好に充放電時の発熱を抑える等が可能になる。なお、電池１セル分の中で２以上に分けられた領域には、非塗布部のみからなる領域があっても良い。このような非塗布部のみからなる領域は、例えば、小型電池等において電極板を捲き回した時に最外周に用いられる。
An example of the case where the pitch of each electrode active material layer gradually increases or gradually decreases in the longitudinal direction of the current collector in the entire battery cell is as shown in FIG. In addition, as an example in which at least one region divided into two or more in one battery cell gradually increases or decreases gradually in the longitudinal direction of the current collector, FIG. ), The pitch of each electrode active material layer is 10 (2) among the regions 10 (1), 10 (2), 10 (3) divided into three in one battery cell. Examples include a case where the current collector gradually increases or decreases gradually in the longitudinal direction of the current collector. As another example, as shown in FIG. 2 (b), the regions 10 (1), 10 (2), 10 (3), 10 (4) divided into four in one battery cell. Among them, there are cases where 10 (2) and 10 (3) gradually increase or decrease gradually at different pitches.
For example, the pitch of each electrode active material layer gradually increases in the longitudinal direction of the current collector in two or more regions divided into two or more in one battery cell as shown in FIG. When the winding is gradually reduced, it is possible to change the number of turns for attaching the lead wire on the inner side of the winding and the number of turns for attaching the lead wire on the outer side of the winding during winding. For example, at the time of winding, a lead wire can be attached every four turns in the inner part of the winding, and a lead wire can be attached every three turns in the outer part of the winding. By appropriately adjusting the number of turns to which the lead wire is attached at the time of winding, it becomes possible to suppress heat generation during charging and discharging well while reducing the non-coated portion to the minimum and increasing the battery capacity. In addition, in the area | region divided into 2 or more in 1 battery part, the area | region which consists only of a non-application part may be sufficient. Such a region consisting only of the non-coated portion is used, for example, on the outermost periphery when the electrode plate is rolled around in a small battery or the like.
前記各電極活物質層のピッチが、電池１セル分全体でランダムである場合であっても、捲回時に、リード線を付ける周回数を適宜ランダムに取れば、捲回する時に重なるようにリード線をとることが可能になる。 Even if the pitch of each electrode active material layer is random for the entire battery cell, if the number of rounds to which the lead wire is attached is appropriately random at the time of winding, the leads are overlapped at the time of winding. It becomes possible to draw a line.
塗布部のピッチを変える方法としては、電極活物質層の長手方向の長さと非塗布部の長手方向の長さの両方を変える方法、電極活物質層の長手方向の長さは一定にして非塗布部の長手方向の長さを変える方法、非塗布部の長手方向の長さはそれぞれ一定にして電極活物質層の長手方向の長さを変える方法等が挙げられるが、単位面積当りの電極活物質量を増加する点からは、電極活物質層の長手方向の長さはなるべく長くすることが好ましい。 As a method of changing the pitch of the coating part, a method of changing both the length of the electrode active material layer in the longitudinal direction and the length of the non-coating part in the longitudinal direction, and the length of the electrode active material layer in the longitudinal direction are made constant. Examples include a method of changing the length in the longitudinal direction of the coating portion and a method of changing the length in the longitudinal direction of the electrode active material layer while keeping the length of the non-application portion in the longitudinal direction constant. From the viewpoint of increasing the amount of active material, the length of the electrode active material layer in the longitudinal direction is preferably as long as possible.
従って、前記各電極活物質層のピッチに含まれる電極活物質層の集電体の長手方向の長さは、ピッチの長さが長い程それよりも短いピッチに含まれる電極活物質層の集電体の長手方向の長さと同じか又はそれよりも長いことが、単位面積当りの電極活物質量を増加することができ、電池容量の点から好ましい。 Therefore, the length in the longitudinal direction of the current collector of the electrode active material layer included in the pitch of each of the electrode active material layers is such that the longer the pitch length, the more the electrode active material layer included in the shorter pitch. A length equal to or longer than the length in the longitudinal direction of the electric body can increase the amount of electrode active material per unit area, which is preferable from the viewpoint of battery capacity.
更に、リード線を良好に取り付ける目的から非塗布部の長手方向の長さをリード線が良好に取り付けられる最低限の長さに一定に確保して、電極活物質層の長さをピッチの長さに合わせて調節することが、単位面積当りの電極活物質量を増加することができ、電池容量の点から好ましい。
尚、本発明のように集電体へ電極活物質層用塗工組成物を塗布する時に、塗布部と非塗布部とを、集電体の塗布流れ方向へ間歇的に設けることにより以下の効果が得られる。
すなわち、従来、集電体へ電極活物質層用塗工組成物を塗布する時は、集電体の幅方向における少なくとも一方の側縁部に所定の幅で集電体の非塗布部を残し、集電体の長手方向へ切れ間なく塗工組成物を塗布して塗布部を設けることにより、該塗布部と長手方向に平行して非塗布部を形成していた。そして、活物質層を高密度化するために電極板を圧延した後、該非塗布部にリード線が取り付けられていた。しかし、このような電極板を圧延する際には、塗布部と非塗布部の長手方向の伸び率が異なるため、電極板が変形し、歪んでシワが生じてしまう。
これに対して、本発明においては、集電体へ電極活物質層用塗工組成物を塗布する時は、集電体の長手方向へ間歇的に塗工組成物を塗布して塗布部と非塗布部を交互に設ける。そして、集電体の幅方向における側縁部に長手方法と平行にのびた非塗布部がある場合には、該非塗布部を裁断して切り離した後、電極板を圧延し、前記非塗布部にリード線を取り付ける。このため、電極板の圧延の際には、塗布部が長手方向に均一に伸び、電極板が変形したり、歪んでシワを生じさせることなく、電極活物質層を高密度化することができる。
Furthermore, for the purpose of mounting the lead wires well, the length of the non-coated portion in the longitudinal direction is kept constant to the minimum length that allows the lead wires to be mounted well, and the length of the electrode active material layer is set to the length of the pitch. It is preferable from the viewpoint of battery capacity that the amount of electrode active material per unit area can be increased.
When applying the electrode active material layer coating composition to the current collector as in the present invention, the application part and the non-application part are intermittently provided in the current application direction of the current collector as follows. An effect is obtained.
That is, conventionally, when the electrode active material layer coating composition is applied to the current collector, at least one side edge in the width direction of the current collector is left with a non-coated portion of the current collector with a predetermined width. By applying the coating composition in the longitudinal direction of the current collector and providing an application part, a non-application part was formed in parallel with the application part and in the longitudinal direction. And after rolling an electrode plate in order to make an active material layer into high density, the lead wire was attached to this non-application part. However, when rolling such an electrode plate, since the elongation ratio in the longitudinal direction of the coated portion and the non-coated portion is different, the electrode plate is deformed and distorted to cause wrinkles.
On the other hand, in the present invention, when the electrode active material layer coating composition is applied to the current collector, the coating composition is applied intermittently in the longitudinal direction of the current collector, Non-application parts are provided alternately. And, when there is a non-applied part extending in parallel with the longitudinal method at the side edge in the width direction of the current collector, after cutting and separating the non-applied part, the electrode plate is rolled, Attach the lead wire. For this reason, when the electrode plate is rolled, the application portion extends uniformly in the longitudinal direction, and the electrode active material layer can be densified without causing deformation or warping of the electrode plate. .
集電体へ電極活物質層用塗工組成物を塗布する塗布部と塗布しない非塗布部とを、当該各塗布部のピッチが異なるように、集電体の塗布流れ方向へ設けることにより、所定パターン状に電極活物質層を形成する工程における塗布方法としては、電極活物質層用塗工組成物をダイヘッドで間欠的に供給するダイコート法を用いて、該電極活物質層用塗工組成物を集電体に塗布する方法や、電極活物質層用塗工組成物をダイヘッドへ連続的に供給し、ダイヘッド及び／又は集電体を離間、接近させて、該電極活物質層用塗工組成物を該集電体に塗布することで、集電体へ塗布する塗布部と塗布しない非塗布部とを集電体の塗布流れ方向へ設ける方法や、電極活物質層用塗工組成物を第１のロール上へ供給しコンマヘッドで掻き取って所定量とし、該所定量の電極活物質組成物をコンマリバース法により第２ロール上に沿って走行する集電体へ転移させる際に、第２ロールを第１ロールから離間、接近させることで、前記集電体へ前記電極活物質組成物の塗布部と非塗布部とを設ける方法等が挙げられる。なお、活物質層は、複数回塗布、乾燥を繰り返すことにより形成してもよい。 By providing the application part for applying the electrode active material layer coating composition to the current collector and the non-application part not applied in the application flow direction of the current collector so that the pitch of each application part is different, As a coating method in the step of forming the electrode active material layer in a predetermined pattern, the electrode active material layer coating composition is formed by using a die coating method in which the electrode active material layer coating composition is intermittently supplied by a die head. The electrode active material layer coating method and the electrode active material layer coating composition are continuously supplied to the die head, and the die head and / or the current collector are separated and brought close to each other. A method of applying a coating composition to the current collector to provide an application portion to be applied to the current collector and a non-application portion not to be applied in the application flow direction of the current collector, or a coating composition for an electrode active material layer The product is fed onto the first roll and scraped with a comma head to a predetermined amount, When transferring a predetermined amount of the electrode active material composition to the current collector running along the second roll by the comma reverse method, the current collector is separated from and approached the first roll. And a method of providing an application part and a non-application part of the electrode active material composition. The active material layer may be formed by repeating application and drying a plurality of times.
塗布された電極活物質層用塗工組成物は、組成物中に含まれる溶剤を除去するために、通常乾燥される。乾燥工程における熱源としては、熱風、赤外線、マイクロ波、高周波、或いはそれらを組み合わせて利用できる。乾燥工程において集電体をサポート又はプレスする金属ローラーや金属シートを加熱して放出させた熱によって乾燥してもよい。また、乾燥後、電子線または放射線を照射することにより、結着材を架橋反応させて活物質層を得ることもできる。 The applied electrode active material layer coating composition is usually dried in order to remove the solvent contained in the composition. As a heat source in the drying process, hot air, infrared rays, microwaves, high frequencies, or a combination thereof can be used. You may dry with the heat which discharge | released the metal roller and metal sheet which support or press a collector in a drying process. In addition, after drying, the active material layer can also be obtained by irradiating an electron beam or radiation to cause a crosslinking reaction of the binder.
更に、得られた電極活物質層をプレス加工することにより、電極活物質層の密度、集電体に対する密着性、均質性を向上させることができる。 Furthermore, the density of the electrode active material layer, the adhesion to the current collector, and the homogeneity can be improved by pressing the obtained electrode active material layer.
プレス加工は、例えば、金属ロール、弾性ロール、加熱ロールまたはシートプレス機等を用いて行う。本発明においてプレス温度は、活物質層の塗工膜を乾燥させる温度よりも低い温度とする限り、室温で行っても良いし又は加温して行っても良いが、通常は室温（室温の目安としては１５〜３５℃である。）で行う。 The press working is performed using, for example, a metal roll, an elastic roll, a heating roll, a sheet press machine, or the like. In the present invention, the pressing temperature may be performed at room temperature or may be performed as long as the temperature is lower than the temperature for drying the coating film of the active material layer. As a guide, it is 15 to 35 ° C.).
ロールプレスは、ロングシート状の負極板を連続的にプレス加工できるので好ましい。ロールプレスを行う場合には定位プレス、定圧プレスのいずれを行っても良い。プレスのライン速度は通常、５〜５０ｍ／ｍｉｎ．とする。ロールプレスの圧力を線圧で管理する場合、加圧ロールの直径に応じて調節するが、通常は線圧を０．５ｋｇｆ／ｃｍ〜１ｔｆ／ｃｍとする。 The roll press is preferable because a long sheet-like negative electrode plate can be continuously pressed. When performing a roll press, either a stereotaxic press or a constant pressure press may be performed. The line speed of the press is usually 5 to 50 m / min. And When the pressure of the roll press is managed by linear pressure, the pressure is adjusted according to the diameter of the pressure roll, but the linear pressure is usually 0.5 kgf / cm to 1 tf / cm.
また、シートプレスを行う場合には通常、４９０３〜７３５５０Ｎ／ｃｍ２（５００〜７５００ｋｇｆ／ｃｍ２）、好ましくは２９４２０〜４９０３３Ｎ／ｃｍ２（３０００〜５０００ｋｇｆ／ｃｍ２）の範囲に圧力を調節する。プレス圧力が小さすぎると活物質層の均質性が得られにくく、プレス圧力が大きすぎると集電体を含めて電極板自体が破損してしまう場合がある。活物質層は、一回のプレスで所定の厚さにしてもよく、均質性を向上させる目的で数回に分けてプレスしてもよい。 Also, normally when performing sheet pressing, 4903~73550N / cm 2 (500~7500kgf / cm 2), preferably to adjust the pressure in the range of 29420~49033N / cm 2 (3000~5000kgf / cm 2). If the pressing pressure is too low, it is difficult to obtain the homogeneity of the active material layer. If the pressing pressure is too high, the electrode plate itself including the current collector may be damaged. The active material layer may have a predetermined thickness by a single press, or may be pressed several times for the purpose of improving homogeneity.
電極活物質層の塗工量は通常、２０〜２５０ｇ／ｍ2とし、その厚さは、乾燥、プレス後に通常１０〜２００μｍ、好ましくは５０〜１７０μｍの範囲にする。負極活物質層の密度は、塗工後は１．０ｇ／ｃｃ程度であるが、プレス後は１．５ｇ／ｃｃ以上（通常は１．５〜１．７５ｇ／ｃｃ程度）まで増大する。従って、プレス加工を支障なく行って体積エネルギー密度を向上させることにより、電池の高容量化を図ることが出来る。 The coating amount of the electrode active material layer is usually 20 to 250 g / m 2 , and the thickness is usually 10 to 200 μm, preferably 50 to 170 μm after drying and pressing. The density of the negative electrode active material layer is about 1.0 g / cc after coating, but increases to 1.5 g / cc or more (usually about 1.5 to 1.75 g / cc) after pressing. Therefore, the capacity of the battery can be increased by improving the volume energy density by performing the pressing without hindrance.
このようにして得られる電極板の活物質層は、少なくとも正極又は負極活物質及び結着材を含有し、さらに必要に応じて導電剤やその他の成分を含有してなるものであり、乾燥後の活物質層に含有される各成分の配合割合は、活物質層用塗工組成物の固形分基準での配合割合と同じである。 The active material layer of the electrode plate thus obtained contains at least a positive electrode or negative electrode active material and a binder, and further contains a conductive agent and other components as necessary, and after drying The blending ratio of each component contained in the active material layer is the same as the blending ratio on the basis of the solid content of the active material layer coating composition.
図３に模式的に示すように、本発明において用いられる正極板と負極板は、該正極板１ａと該負極板１ｂの間にセパレータ２を挟んで重ねて捲回すると、正負両極の活物質層の非塗布部同士４ａ、４ｂが同位置にぴったりと重なり、且つ、正負両極の活物質層の塗布部３ａ、３ｂが同位置にぴったりと重なる。
正極板と負極板を捲回した状態で、正負両極の活物質層の非塗布部同士及び正負両極の活物質層の塗布部を、それぞれ同位置に重ねるためには、本発明のように、巻きの周回距離に合わせて、塗工部と非塗工部を含む活物質層のピッチを調節する必要がある。展開状態の集電体の長手方向に等間隔に塗工部と非塗工部を設ける場合には、捲回した状態で塗布部同士及び非塗布部同士を同位置に重ねることが出来ない。
As schematically shown in FIG. 3, when the positive electrode plate and the negative electrode plate used in the present invention are wound with the
In a state where the positive electrode plate and the negative electrode plate are wound, in order to overlap the non-coated portions of the positive and negative active material layers and the coated portions of the positive and negative active material layers, respectively, at the same position, as in the present invention, It is necessary to adjust the pitch of the active material layer including the coated portion and the non-coated portion in accordance with the winding distance. When the coating part and the non-coating part are provided at equal intervals in the longitudinal direction of the current collector in the developed state, the coating part and the non-coating part cannot be overlapped at the same position in a wound state.
本発明においては、正極板と負極板を捲回した状態で、正負両極の活物質層の塗布部同士がセパレータを間に介して同位置にぴったりと重なるため、正極活物質層塗布部と負極活物質層塗布部がセパレータを介してぴったりと重ならない場合よりも、電池反応の効率を向上させ、体積あたりのエネルギー量を増大させることができる。 In the present invention, since the positive electrode plate and the negative electrode plate are wound, the application portions of the positive and negative electrode active material layers are exactly overlapped at the same position with the separator interposed therebetween, so that the positive electrode active material layer application portion and the negative electrode The efficiency of the battery reaction can be improved and the amount of energy per volume can be increased as compared with the case where the active material layer application portion does not overlap exactly through the separator.
また、本発明においては、電極板を捲回する時に正極活物質層の非塗布部と負極活物質層の非塗布部が同位置に重なるように、集電体の長手方向の各電極活物質層のピッチが異なるため、当該ピッチに含まれる非塗布部にリード線を取り付けることにより、電極板が変形することなく捲回の周回ごとに、同極のリード線同士がそれぞれ重なり、且つ、異極リード線と接触しないようにリード線をとることが可能である。その結果、高出力が得られ、且つ、充放電時の発熱を抑えることが可能である。
図４には、非塗布部にリード線７ａが取り付けられた正極板１ａと、非塗布部にリード線７ｂが取り付けられた負極板１ｂの組み合わせが、正極活物質層の各非塗布部のリード線７ａ同士及び負極活物質層の各非塗布部のリード線７ｂ同士が、それぞれ同極ごとに同位置に重なるように捲回されて、テープ８で固定されている一例の概略図を示す。
例えば、図５（ａ）と図５（ｂ）に示すように、正極活物質層非塗布部に溶接されるリード線と負極活物質層非塗布部に溶接されるリード線が、集電体の異なる端側から外部へ突出するように溶接されていると、正極のリード線と負極のリード線との間に距離が保たれ、上記効果を得ることができる。
Further, in the present invention, each electrode active material in the longitudinal direction of the current collector is so arranged that the non-coated portion of the positive electrode active material layer and the non-coated portion of the negative electrode active material layer overlap at the same position when winding the electrode plate. Since the pitches of the layers are different, by attaching lead wires to the non-applied part included in the pitches, the same-polarity lead wires overlap each other in each round of winding without deformation of the electrode plate. It is possible to take the lead wire so as not to contact the polar lead wire. As a result, high output can be obtained and heat generation during charging / discharging can be suppressed.
In FIG. 4, the combination of the
For example, as shown in FIGS. 5A and 5B, the lead wire welded to the positive electrode active material layer non-applied portion and the lead wire welded to the negative electrode active material layer non-applied portion are current collectors. If they are welded so as to protrude from the different end sides to the outside, a distance is maintained between the positive lead wire and the negative lead wire, and the above effect can be obtained.
リード線は公知のリード線でよく、例えば集電体に溶接すること等により固定することができる。リード線は、電極板を捲回する１回ごとに同位置に重ならなくてもよく、電極板を捲回する複数回ごとにリード線が同位置に重なるようにしても良い。
本発明においては、非塗布部にリード線を取り付けるためリード線の取り付けが容易で、且つ効率的に生産可能である。さらに、集電体の長手方向へ電極活物質層が間欠的に配置されていることから、高密度化するための圧延プレス時の高圧でもシワが発生しないというメリットも有する。
The lead wire may be a known lead wire and can be fixed, for example, by welding to a current collector. The lead wire does not have to overlap at the same position every time the electrode plate is wound, and the lead wire may overlap at the same position every time the electrode plate is wound.
In the present invention, since the lead wire is attached to the non-coated portion, the lead wire can be easily attached and can be produced efficiently. Furthermore, since the electrode active material layer is intermittently arranged in the longitudinal direction of the current collector, there is an advantage that wrinkles are not generated even at a high pressure during rolling press for increasing the density.
電極板を捲回する時に正極または負極活物質層の非塗布部は、捲回の毎周回ごとに出現する必要はなく、電極板を捲回する複数回ごとに非塗布部が同位置に重なるようにしても良い。
また、本発明に用いる非水電解液二次電池用の正極板及び負極板電極板において、上記のように間欠的に配置された電極活物質層は、集電体の少なくとも一方の面にあればよい。
なお、各塗布部のピッチ、非塗布部の集電体の長手方向の長さ、電極活物質層の集電体の長手方向の長さ等は、製造する非水電解液二次電池の設計によりそれぞれ適宜調節されるものであり、特に制限されない。
When the electrode plate is wound, the non-coated portion of the positive electrode or negative electrode active material layer does not need to appear every winding, and the non-coated portion overlaps at the same position every time the electrode plate is wound. You may do it.
In the positive electrode plate and the negative electrode plate electrode plate for the non-aqueous electrolyte secondary battery used in the present invention, the electrode active material layer arranged intermittently as described above should be on at least one surface of the current collector. That's fine.
In addition, the pitch of each application part, the length in the longitudinal direction of the current collector of the non-application part, the length in the longitudinal direction of the current collector of the electrode active material layer, etc. are designed for the nonaqueous electrolyte secondary battery to be manufactured. Are appropriately adjusted, and are not particularly limited.
以上のようにして本発明に係る非水電解液二次電池用の正極板と負極板の組み合わせが得られ、この正極板と負極板を用いて非水電解液二次電池を作製することができる。 As described above, a combination of a positive electrode plate and a negative electrode plate for a non-aqueous electrolyte secondary battery according to the present invention is obtained, and a non-aqueous electrolyte secondary battery can be produced using the positive electrode plate and the negative electrode plate. it can.
通常、正極板及び負極板を、ポリエチレン製多孔質フィルムのようなセパレータを介して渦巻状に捲き回し、外装容器に挿入する。挿入後、正極板に取り付けられたリード線を外装容器に設けた正極端子に接続し、一方、負極板に取り付けられたリード線を外装容器に設けた負極端子に接続し、外装容器に非水電解液を充填し、密封することによって、本発明に係る電極板を備えた非水電解液二次電池が完成する。 Usually, a positive electrode plate and a negative electrode plate are spirally wound through a separator such as a polyethylene porous film and inserted into an outer container. After the insertion, the lead wire attached to the positive electrode plate is connected to the positive electrode terminal provided in the outer container, while the lead wire attached to the negative electrode plate is connected to the negative electrode terminal provided in the outer container, By filling and sealing the electrolyte, a non-aqueous electrolyte secondary battery equipped with the electrode plate according to the present invention is completed.
リチウム系二次電池を作製する場合には、溶質であるリチウム塩を有機溶媒に溶かした非水電解液が用いられる。リチウム塩としては、例えば、ＬｉＣｌＯ４、ＬｉＢＦ４、ＬｉＰＦ６、ＬｉＡｓＦ６、ＬｉＣｌ、ＬｉＢｒ等の無機リチウム塩、または、ＬｉＢ（Ｃ６Ｈ５）４、ＬｉＮ（ＳＯ２ＣＦ３）２、ＬｉＣ（ＳＯ２ＣＦ３）３、ＬｉＯＳＯ２ＣＦ３、ＬｉＯＳＯ２Ｃ２Ｆ５、ＬｉＯＳＯ２Ｃ３Ｆ７、ＬｉＯＳＯ２Ｃ４Ｆ９、ＬｉＯＳＯ２Ｃ５Ｆ１１、ＬｉＯＳＯ２Ｃ６Ｆ１３、ＬｉＯＳＯ２Ｃ７Ｆ１５等の有機リチウム塩等が用いられる。
When producing a lithium secondary battery, a nonaqueous electrolytic solution in which a lithium salt as a solute is dissolved in an organic solvent is used. Examples of the lithium salt include inorganic lithium salts such as LiClO 4 , LiBF 4 , LiPF 6 , LiAsF 6 , LiCl, and LiBr, or LiB (C 6 H 5 ) 4 , LiN (SO 2 CF 3 ) 2 , LiC ( SO 2 CF 3) 3, LiOSO 2
リチウム塩を溶解するための有機溶媒としては、環状エステル類、鎖状エステル類、環状エーテル類、鎖状エーテル類等を例示できる。より具体的には、環状エステル類としては、プロピレンカーボネート、ブチレンカーボネート、γ−ブチロラクトン、ビニレンカーボネート、２−メチル−γ−ブチロラクトン、アセチル−γ−ブチロラクトン、γ−バレロラクトン等を例示できる。 Examples of the organic solvent for dissolving the lithium salt include cyclic esters, chain esters, cyclic ethers, chain ethers and the like. More specifically, examples of cyclic esters include propylene carbonate, butylene carbonate, γ-butyrolactone, vinylene carbonate, 2-methyl-γ-butyrolactone, acetyl-γ-butyrolactone, γ-valerolactone, and the like.
鎖状エステル類としては、ジメチルカーボネート、ジエチルカーボネート、ジブチルカーボネート、ジプロピルカーボネート、メチルエチルカーボネート、メチルブチルカーボネート、メチルプロピルカーボネート、エチルブチルカーボネート、エチルプロピルカーボネート、ブチルプロピルカーボネート、プロピオン酸アルキルエステル、マロン酸ジアルキルエステル、酢酸アルキルエステル等を例示できる。 Chain esters include dimethyl carbonate, diethyl carbonate, dibutyl carbonate, dipropyl carbonate, methyl ethyl carbonate, methyl butyl carbonate, methyl propyl carbonate, ethyl butyl carbonate, ethyl propyl carbonate, butyl propyl carbonate, propionic acid alkyl ester, malon Examples thereof include acid dialkyl esters and acetic acid alkyl esters.
環状エーテル類としては、テトラヒドロフラン、アルキルテトラヒドロフラン、ジアルキルテトラヒドロフラン、アルコキシテトラヒドロフラン、ジアルコキシテトラヒドロフラン、１，３−ジオキソラン、アルキル−１，３−ジオキソラン、１，４−ジオキソラン等を例示できる。 Examples of cyclic ethers include tetrahydrofuran, alkyltetrahydrofuran, dialkyltetrahydrofuran, alkoxytetrahydrofuran, dialkoxytetrahydrofuran, 1,3-dioxolane, alkyl-1,3-dioxolane, 1,4-dioxolane and the like.
鎖状エーテル類としては、１，２−ジメトキシエタン、１，２−ジエトキシエタン、ジエチルエーテル、エチレングリコールジアルキルエーテル、ジエチレングリコールジアルキルエーテル、トリエチレングリコールジアルキルエーテル、テトラエチレングリコールジアルキルエーテル等を例示することができる。 Examples of chain ethers include 1,2-dimethoxyethane, 1,2-diethoxyethane, diethyl ether, ethylene glycol dialkyl ether, diethylene glycol dialkyl ether, triethylene glycol dialkyl ether, and tetraethylene glycol dialkyl ether. Can do.
（実施例１）
正極用活物質としてＬｉＭｎ2Ｏ4（粉末を９０重量部と、正極用導電剤としてアセチレンブラックを５重量部と、正極用結着材としてポリフッ化ビニリデンを５重量部と、固形分が組成物中６０重量％になるように溶剤としてＮ−メチル−ピロリドンを用いて、これらをプラネタリーミキサーで混合することにより、正極活物質層用塗工組成物の調製を行った。集電体として厚さ１５μｍのアルミ箔に、捲回時に１周ごとに非塗布部が重なるように、ダイヘッドで間欠的に供給するダイコート法を用いて、正極活物質層用塗工組成物を塗工した。一面あたりの塗工量は約１５０ｇ／ｍ2となるようにし、両面に同じパターンで塗工した。電池１セル分において、非塗布部は２０ｍｍに固定し、最初に塗布した塗布部の集電体の長手方向の長さが１８０ｍｍで、塗布部は各ピッチごとに２０ｍｍずつ長手方向に長くなるように１５回塗布した。また、各電池１セル分の間は、非塗布部を４０ｍｍ、塗布部を１００ｍｍ設けた。
Example 1
LiMn 2 O 4 as active material for positive electrode (90 parts by weight of powder, 5 parts by weight of acetylene black as conductive agent for positive electrode, 5 parts by weight of polyvinylidene fluoride as binder for positive electrode, solid content A coating composition for a positive electrode active material layer was prepared by mixing these with a planetary mixer using N-methyl-pyrrolidone as a solvent so that the content of the mixture was 60% by weight. A positive electrode active material layer coating composition was applied to a 15 μm thick aluminum foil by using a die coating method in which a non-coated portion is intermittently supplied by a die head so that a non-coated portion overlaps every turn during winding. The coating amount was about 150 g / m 2, and the both sides were coated with the same pattern, and the non-coated part was fixed at 20 mm for 1 cell, and the current collector of the coated part applied first Length in the longitudinal direction The application part was applied 15 times so as to be longer in the longitudinal direction by 20 mm for each pitch, and 40 mm for the non-application part and 100 mm for the application part were provided for each cell.
また、負極用活物質として人造黒鉛を９７重量部と、増粘剤としてカルボキシメチルセルロースを１重量部と、負極用結着材としてスチレン−ブタジエンゴムを２重量部と、固形分が組成物中４５重量％になるように溶剤としてイオン交換水を用いて、これらをプラネタリーミキサーで混合することにより、負極活物質層用塗工組成物の調製を行った。集電体として厚さ１０μｍの銅箔に、捲回時に１周ごとに非塗布部が重なるように、ダイヘッドで間欠的に供給するダイコート法を用いて、負極活物質層用塗工組成物を塗工した。一面あたりの塗工量は約５０ｇ／ｍ2となるようにし、両面に同じパターンで塗工した。電池１セル分において、非塗布部は１８ｍｍに固定し、最初に塗布した塗布部の集電体の長手方向の長さが１９０ｍｍで、塗布部は各ピッチごとに２０ｍｍずつ長手方向に長くなるように１５回塗布した。また、各電池１セル分の間は、非塗布部を４０ｍｍ、塗布部を１００ｍｍ設けた。 In addition, 97 parts by weight of artificial graphite as the active material for the negative electrode, 1 part by weight of carboxymethyl cellulose as the thickener, 2 parts by weight of styrene-butadiene rubber as the binder for the negative electrode, and a solid content of 45 parts in the composition A negative electrode active material layer coating composition was prepared by mixing these with a planetary mixer using ion-exchanged water as a solvent so as to be in% by weight. A negative electrode active material layer coating composition is applied to a copper foil having a thickness of 10 μm as a current collector by using a die coating method in which a non-coated portion is intermittently supplied by a die head so that a non-coated portion is overlapped every round during winding. Coated. The coating amount per side was set to about 50 g / m 2, and coating was performed on both sides with the same pattern. In one battery cell, the non-applied part is fixed at 18 mm, the length of the collector applied in the longitudinal direction is 190 mm in the longitudinal direction, and the coated part is elongated in the longitudinal direction by 20 mm for each pitch. Was applied 15 times. Moreover, between 1 cell of each battery, the non-application part was provided 40 mm and the application part 100 mm was provided.
塗工乾燥後、ロールプレス機にて、正極は塗工部が３．２０ｇ／ｃｃ、負極は塗工部が１．２０ｇ／ｃｃになるように圧延加工を行った。
その後、正極は１００ｍｍ幅、負極は１０５ｍｍ幅になるようにスリットを行い、各電極板を作製した。
After coating and drying, a roll press machine was used to perform rolling so that the coating part of the positive electrode was 3.20 g / cc and the coating part of the negative electrode was 1.20 g / cc.
Thereafter, slitting was performed so that the positive electrode had a width of 100 mm and the negative electrode had a width of 105 mm, thereby producing each electrode plate.
得られた正極板と負極板の各非塗布部にリード線をタブ付けした。当該正極板と負極板を外装容器に挿入できるように、セパレータを介して、両極の非塗布部同士及び両極の塗布部同士がぴったりと重なるように捲き回した。捲き回した電極板を外装容器に挿入し、電解液として１Ｍ ＬｉＰＦ6のエチレンカーボネート／メチルエチルカーボネート（１／１）溶液を注入した。 The lead wire was tabbed to each non-coated part of the obtained positive electrode plate and negative electrode plate. The positive electrode plate and the negative electrode plate were rolled so that the non-applied parts of both electrodes and the applied parts of both electrodes were exactly overlapped with each other via a separator so that the positive electrode plate and the negative electrode plate could be inserted into the outer container. The rolled electrode plate was inserted into an outer container, and a 1M LiPF 6 ethylene carbonate / methyl ethyl carbonate (1/1) solution was injected as an electrolytic solution.
１…非水電解液二次電池用電極板
１ａ…正極板
１ｂ…負極板
２…集電体
３（３ａ、３ｂ）…電極活物質層
４（４ａ、４ｂ）…電極活物質層非塗布部
５（１）、５（２）、・・・５（ｎ）…各電極活物質層のピッチ
６…各電極活物質層の集電体の長手方向の一辺の長さの起点又は終点
７（７ａ、７ｂ）…リード線
８…テープ
９…電池１セル分
１０（１）、１０（２）、・・１０（ｎ）…電池１セル分で２以上に分けられた領域
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