JP2015162337A - Nonaqueous electrolyte secondary battery and method for manufacturing the same - Google Patents

Nonaqueous electrolyte secondary battery and method for manufacturing the same Download PDF

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JP2015162337A
JP2015162337A JP2014036506A JP2014036506A JP2015162337A JP 2015162337 A JP2015162337 A JP 2015162337A JP 2014036506 A JP2014036506 A JP 2014036506A JP 2014036506 A JP2014036506 A JP 2014036506A JP 2015162337 A JP2015162337 A JP 2015162337A
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separator
secondary battery
electrolyte secondary
electrode
nonaqueous electrolyte
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JP6404577B2 (en
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松田　和也
Kazuya Matsuda
和也 松田
幸広 畑
Yukihiro Hata
幸広 畑
阿部　敏浩
Toshihiro Abe
敏浩 阿部
隆宏 新井
Takahiro Arai
隆宏 新井
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Maxell Holdings Ltd
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Hitachi Maxell 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

Abstract

PROBLEM TO BE SOLVED: To provide a nonaqueous electrolyte secondary battery superior in load characteristics, etc.SOLUTION: A nonaqueous electrolyte secondary battery of the present invention comprises a multilayer electrode body arranged by laminating a positive electrode, a negative electrode and a separator. One of the positive and negative electrodes is bonded with the separator through an adhesive part. A method for manufacturing the nonaqueous electrolyte secondary battery of the present invention comprises: a coating step of coating a belt-shaped separator with a radiation-curable resin to form an adhesive part; an electrode-putting step of putting an electrode on the adhesive part; and a bonding step of bonding the electrode to the separator by irradiating the adhesive part with radioactive rays and thus hardening the radiation-curable resin.

Description

本発明は、リチウムイオン二次電池等の非水電解質二次電池及びその製造方法に関する。   The present invention relates to a nonaqueous electrolyte secondary battery such as a lithium ion secondary battery and a method for producing the same.

リチウムイオン二次電池に代表される非水電解質二次電池は、エネルギー密度が高いという特徴から、携帯電話やノート型パーソナルコンピューター等の携帯機器の電源として広く用いられている。携帯機器の高性能化に伴ってリチウムイオン二次電池の高容量化及び長寿命化が更に進む傾向にあり、更なる研究・開発が進められている。   Nonaqueous electrolyte secondary batteries represented by lithium ion secondary batteries are widely used as power sources for portable devices such as mobile phones and notebook personal computers because of their high energy density. As mobile devices become more sophisticated, lithium ion secondary batteries tend to have higher capacities and longer lifetimes, and further research and development are underway.

このような状況下で従来から上記非水電解質二次電池の電池特性を向上させるために種々の方策が検討されてきた。その中で、正極と負極とセパレータとを積層して積層電極体を形成し、その積層電極体をラミネートフィルムからなる外装体に収納した積層型ラミネート電池が実用化されている。積層型ラミネート電池は、負荷特性等に優れており、複数の電池を組み合わせて車載用電源や各種蓄電装置用電源等として用いられているほか、薄型軽量が求められるモバイル機器用電池としても用いられている。   Under such circumstances, various measures have been conventionally studied in order to improve the battery characteristics of the non-aqueous electrolyte secondary battery. Among them, a laminated laminate battery in which a positive electrode, a negative electrode, and a separator are laminated to form a laminated electrode body, and the laminated electrode body is housed in an exterior body made of a laminate film has been put into practical use. Multi-layer laminated batteries have excellent load characteristics, etc., and are used as a power source for in-vehicle power supplies and various power storage devices by combining multiple batteries, and also as a battery for mobile devices that require thin and light weight. ing.

しかし、積層型ラミネート電池は、複数の電極とセパレータとを積層して製造するため、電極の位置ずれ等のない正確な積層工程が必要となり、その積層方法について種々の方法が提案されている。   However, since a laminate-type laminate battery is manufactured by laminating a plurality of electrodes and separators, an accurate lamination process without positional displacement of electrodes is required, and various methods for the lamination method have been proposed.

例えば、特許文献１には、セパレータの両面にイオン伝導性接着剤を塗布し、その両面に正極板と負極板とを接着して位置決めし、その後多数回折ることにより積層電極体を形成する方法が提案されている。   For example, Patent Document 1 discloses a method in which an ion conductive adhesive is applied to both sides of a separator, a positive electrode plate and a negative electrode plate are bonded and positioned on both surfaces, and then a multilayer electrode body is formed by diffracting a large number of times. Has been proposed.

特開２００１−２２９９７９号公報（特許第３３５８８０７号公報）JP 2001-229979 A (Patent No. 3358807)

しかし、特許文献１では、セパレータの両面の全面にイオン伝導性接着剤を塗布しており、電極とセパレータとの接着強度を上げるためにある程度の厚さで塗布した場合、たとえイオン伝導性接着剤であっても電池の内部抵抗は上昇する。このような電池の場合、低温充電や急速充電等を行うとセパレータ上に局所的なリチウムの析出が生じる原因となり、短絡の恐れが大きくなる。   However, in Patent Document 1, an ion conductive adhesive is applied to the entire surface of both surfaces of the separator, and when applied to a certain thickness in order to increase the adhesive strength between the electrode and the separator, the ion conductive adhesive is used. Even so, the internal resistance of the battery increases. In the case of such a battery, if low-temperature charging, rapid charging, or the like is performed, it causes local precipitation of lithium on the separator, and the risk of a short circuit increases.

本発明は上記問題を解決したもので、電極の位置ずれをなくすとともに、負荷特性等に優れた積層型の非水電解質二次電池及びその製造方法を提供するものである。   The present invention solves the above-mentioned problems, and provides a laminated nonaqueous electrolyte secondary battery excellent in load characteristics and the like, and a manufacturing method thereof, while eliminating the displacement of electrodes.

本発明の非水電解質二次電池は、正極と、負極と、セパレータとが積層された積層電極体を含む非水電解質二次電池であって、前記正極及び前記負極のいずれか一方の電極と、前記セパレータとは、接着部により接着されていることを特徴とする。   The non-aqueous electrolyte secondary battery of the present invention is a non-aqueous electrolyte secondary battery including a laminated electrode body in which a positive electrode, a negative electrode, and a separator are laminated, and one of the positive electrode and the negative electrode The separator is bonded by an adhesive portion.

また、本発明の非水電解質二次電池の製造方法は、帯状のセパレータに放射線硬化性樹脂を塗布して接着部を形成する塗布工程と、塗布された前記接着部の上に電極を配置する電極配置工程と、前記接着部に放射線を照射して前記放射線硬化性樹脂を硬化して前記電極と前記セパレータとを接着する接着工程とを含むことを特徴とする。   Moreover, the manufacturing method of the nonaqueous electrolyte secondary battery of this invention arrange | positions an electrode on the apply | coating process which apply | coats a radiation curable resin to a strip | belt-shaped separator, and forms an adhesion part, and the said adhesion | attachment part applied. The method includes an electrode arranging step and an adhesion step of irradiating the bonding portion with radiation to cure the radiation curable resin and bond the electrode and the separator.

本発明によると、電極の位置ずれがなく、負荷特性等に優れた非水電解質二次電池及びその製造方法を提供できる。   According to the present invention, it is possible to provide a non-aqueous electrolyte secondary battery excellent in load characteristics and the like without any positional deviation of electrodes and a manufacturing method thereof.

図１は、本発明の非水電解質二次電池の製造工程の一例を示す模式側面図である。FIG. 1 is a schematic side view showing an example of the manufacturing process of the nonaqueous electrolyte secondary battery of the present invention. 図２は、本発明の非水電解質二次電池の製造工程の一例を示す模式平面図である。FIG. 2 is a schematic plan view showing an example of a manufacturing process of the nonaqueous electrolyte secondary battery of the present invention. 図３は、本発明の非水電解質二次電池に用いる積層電極体の一例を示す底面図である。FIG. 3 is a bottom view showing an example of a laminated electrode body used in the nonaqueous electrolyte secondary battery of the present invention. 図４は、本発明の非水電解質二次電池の製造工程の他の一例を示す模式図である。FIG. 4 is a schematic view showing another example of the manufacturing process of the nonaqueous electrolyte secondary battery of the present invention. 図５は、本発明の非水電解質二次電池に用いる積層電極体の他の一例を示す底面図である。FIG. 5 is a bottom view showing another example of the laminated electrode body used in the nonaqueous electrolyte secondary battery of the present invention. 図６は、本発明の非水電解質二次電池の一例を示す平面図である。FIG. 6 is a plan view showing an example of the nonaqueous electrolyte secondary battery of the present invention.

本発明の非水電解質二次電池は、正極と、負極と、セパレータとが積層された積層電極体を備えている。また、上記正極及び上記負極のいずれか一方の電極と、上記セパレータとは、接着部により接着されている。   The nonaqueous electrolyte secondary battery of the present invention includes a laminated electrode body in which a positive electrode, a negative electrode, and a separator are laminated. In addition, one of the positive electrode and the negative electrode is bonded to the separator by an adhesive portion.

上記電極は、上記接着部により上記セパレータに接着して固定されているので、上記セパレータに対する電極のずれをなくすことができる。これにより、負荷特性等に優れた非水電解質二次電池を提供できる。   Since the electrode is bonded and fixed to the separator by the bonding portion, the electrode can be prevented from being displaced with respect to the separator. Thereby, the nonaqueous electrolyte secondary battery excellent in load characteristics etc. can be provided.

また、上記正極と上記セパレータとが、上記接着部により接着されており、上記負極と上記セパレータとは、接着されていないことが好ましい。リチウムイオンを受け入れる側の負極がセパレータと接着していないことにより、セパレータのイオン伝導性が阻害されず、低温充電や急速充電等を行ってもリチウムの析出が抑制されて、短絡の恐れが小さくなる。   Moreover, it is preferable that the said positive electrode and the said separator are adhere | attached by the said adhesion part, and the said negative electrode and the said separator are not adhere | attached. Since the negative electrode that accepts lithium ions is not bonded to the separator, the ion conductivity of the separator is not hindered, and even if low-temperature charging or rapid charging is performed, lithium deposition is suppressed and the risk of short-circuiting is small. Become.

また、上記接着部は放射線硬化性樹脂から形成されていることが好ましい。これにより、放射線硬化性樹脂以外の接着性樹脂を用いる場合に比べて上記接着部の接着強度を高めることができるとともに、放射線を照射するという簡便な工程で樹脂を硬化できるため、製造工程を簡略化できる。   Moreover, it is preferable that the said adhesion part is formed from the radiation curable resin. This makes it possible to increase the adhesive strength of the adhesive portion compared to the case where an adhesive resin other than a radiation curable resin is used, and the resin can be cured by a simple process of irradiating radiation, thus simplifying the manufacturing process. Can be

上記接着部の１箇所当たりの面積は、０．３ｍｍ2以上７．１ｍｍ2以下であることが好ましい。これにより、接着強度を保持しつつ、接着部の面積をできるだけ小さくして、セパレータのイオン伝導性の低下を抑制できる。 Area per one place of the adhesive portion is preferably 0.3 mm 2 or more 7.1 mm 2 or less. Thereby, the area | region of an adhesion part can be made as small as possible, maintaining adhesive strength, and the fall of the ion conductivity of a separator can be suppressed.

上記接着部の１箇所当たりの厚さは、５μｍ以下であることが好ましい。上記接着部の厚さが５μｍあれば接着強度としては十分であり、逆に上記接着部の厚さが５μｍを超えると上記接着部が凸状となり、積層電極体が変形する恐れがあるからである。この観点からは、上記接着部の厚さの下限値は、接着強度を確保できれば０μｍであることが最も好ましい。   It is preferable that the thickness per one part of the said adhesion part is 5 micrometers or less. If the thickness of the adhesive part is 5 μm, the adhesive strength is sufficient, and conversely if the thickness of the adhesive part exceeds 5 μm, the adhesive part becomes convex and the laminated electrode body may be deformed. is there. From this viewpoint, the lower limit value of the thickness of the bonded portion is most preferably 0 μm as long as the bonding strength can be secured.

上記電極と上記セパレータとの接着強度は、０．５Ｎ以上あればよく、これにより工程中の電極のずれの防止が可能となる。   The adhesive strength between the electrode and the separator may be 0.5 N or more, which can prevent the electrode from being displaced during the process.

上記接着部の配置位置は、上記電極毎に異なることが好ましい。これにより、上記接着部に厚さがある場合に、電極の積層方向における上記接着部同士の重なりを防止でき、積層電極体の変形を抑制することができる。   The arrangement position of the adhesive portion is preferably different for each electrode. Thereby, when the said adhesion part has thickness, the overlap of the said adhesion parts in the lamination direction of an electrode can be prevented, and a deformation | transformation of a laminated electrode body can be suppressed.

上記セパレータは、袋状セパレータを形成していることが好ましい。これにより、本発明の非水電解質二次電池では、正極と負極との短絡をより確実に防止できる。上記積層電極体において、上記袋状セパレータは、それぞれ独立していても、それぞれ連結していてもよい。   The separator preferably forms a bag-like separator. Thereby, in the nonaqueous electrolyte secondary battery of this invention, the short circuit with a positive electrode and a negative electrode can be prevented more reliably. In the laminated electrode body, the bag-like separators may be independent or connected to each other.

また、本発明の非水電解質二次電池の製造方法は、帯状のセパレータに放射線硬化性樹脂を塗布して接着部を形成する塗布工程と、塗布された上記接着部の上に電極を配置する電極配置工程と、上記接着部に放射線を照射して上記放射線硬化性樹脂を硬化して上記電極と上記セパレータとを接着する接着工程とを備えている。   Moreover, the manufacturing method of the nonaqueous electrolyte secondary battery according to the present invention includes an application step of applying a radiation curable resin to a strip-shaped separator to form an adhesive portion, and disposing an electrode on the applied adhesive portion. An electrode placement step, and a bonding step of irradiating the bonding portion with radiation to cure the radiation curable resin and bond the electrode and the separator.

上記接着に放射線硬化性樹脂を用いているため、放射線硬化性樹脂以外の接着性樹脂を用いる場合に比べて接着強度を高めることができるとともに、放射線を照射するという簡便な工程で樹脂を硬化できるため、製造工程を簡略化でき、本発明の非水電解質二次電池を効率的に製造できる。   Since a radiation curable resin is used for the adhesion, the adhesive strength can be increased compared to the case where an adhesive resin other than the radiation curable resin is used, and the resin can be cured by a simple process of irradiating radiation. Therefore, the manufacturing process can be simplified, and the nonaqueous electrolyte secondary battery of the present invention can be efficiently manufactured.

上記放射線硬化性樹脂の１箇所当たりの塗布量は、０．００５ｍｇ以上０．１５ｍｇ以下であることが好ましい。これにより、上記接着部の１箇所当たりの面積を０．３ｍｍ2以上７．１ｍｍ2以下とすることができ、前述のとおり、セパレータのイオン伝導性の低下を抑制できる。上記塗布量は、０．０７ｍｇ以下がより好ましい。これにより、上記接着部の１箇所当たりの厚さを５μｍ以下にすることができ、積層電極体の変形を抑制することができる。 The coating amount of the radiation curable resin per location is preferably 0.005 mg or more and 0.15 mg or less. Thus, the area per one place of the adhesive portion can be made 0.3 mm 2 or more 7.1 mm 2 or less, as described above, it is possible to suppress the deterioration of the ion conductivity of the separator. The coating amount is more preferably 0.07 mg or less. Thereby, the thickness per one place of the said adhesion part can be 5 micrometers or less, and a deformation | transformation of a laminated electrode body can be suppressed.

上記放射線硬化性樹脂の塗布粘度は、３０℃において４０ｍＰａ・ｓ以上であることが好ましい。上記粘度が上記範囲にあれば、塗布された放射線硬化性樹脂がセパレータを貫通してしまうことがないため、製造装置の汚染を防止できるとともに、セパレータの表面にある程度の放射線硬化性樹脂を保持できるため、確実にセパレータと電極とを接着できる。また、上記塗布粘度は、上記放射線硬化性樹脂をある程度セパレータ内に浸透させるために、３００ｍＰａ・ｓ以下であることが好ましい。   The coating viscosity of the radiation curable resin is preferably 40 mPa · s or more at 30 ° C. If the viscosity is in the above range, the applied radiation curable resin does not penetrate the separator, so that contamination of the manufacturing apparatus can be prevented and a certain amount of radiation curable resin can be held on the surface of the separator. Therefore, the separator and the electrode can be securely bonded. Further, the coating viscosity is preferably 300 mPa · s or less in order to allow the radiation curable resin to penetrate into the separator to some extent.

上記塗布工程において、上記接着部は上記電極毎に異なる位置に配置されることが好ましい。これにより、上記接着部に厚さがある場合に、電極の積層方法における上記接着部同士の重なりを防止でき、積層電極体の変形を抑制することができる。   In the coating step, it is preferable that the bonding portion is disposed at a different position for each of the electrodes. Thereby, when the said adhesion part has thickness, the overlap of the said adhesion parts in the lamination | stacking method of an electrode can be prevented, and a deformation | transformation of a laminated electrode body can be suppressed.

上記接着工程の後に上記電極の上に別のセパレータを配置するセパレータ積層工程と、対向する上記セパレータ同士を接合して袋状セパレータを形成するセパレータ接合工程とを更に備えることもできる。   It is also possible to further include a separator stacking step in which another separator is disposed on the electrode after the bonding step, and a separator joining step in which the separators facing each other are joined to form a bag-like separator.

上記接着部により上記セパレータと接着される電極としては、正極が好ましい。通常、正極は、負極に比べて大きさが小さいため、負極に比べて位置決めが困難だからである。また、上記接着部はリチウムイオンの受け入れを悪化させるため、負極とセパレータとは上記接着部により接着されていないことが好ましい。   The electrode bonded to the separator by the bonding portion is preferably a positive electrode. This is because the positive electrode is usually smaller in size than the negative electrode and is difficult to position compared to the negative electrode. Moreover, since the said adhesion part worsens acceptance of lithium ion, it is preferable that the negative electrode and the separator are not adhere | attached by the said adhesion part.

以下、本発明の実施形態を図面に基づき説明する。   Hereinafter, embodiments of the present invention will be described with reference to the drawings.

（実施形態１）
先ず、本発明の非水電解質二次電池の製造方法の実施形態を説明する。 (Embodiment 1)
First, an embodiment of a method for producing a nonaqueous electrolyte secondary battery of the present invention will be described.

図１は、本発明の非水電解質二次電池の製造工程の一例を示す模式側面図であり、図２は、図１に対応する本発明の非水電解質二次電池の製造工程の一例を示す模式平面図である。但し、図２では、電極とセパレータのみを図示した。   FIG. 1 is a schematic side view showing an example of the manufacturing process of the nonaqueous electrolyte secondary battery of the present invention, and FIG. 2 shows an example of the manufacturing process of the nonaqueous electrolyte secondary battery of the present invention corresponding to FIG. It is a schematic plan view to show. However, in FIG. 2, only the electrode and the separator are shown.

本実施形態では、先ず、第１の繰り出しロール１０に帯状の第１のセパレータ１を準備し、第２の繰り出しロール２０に帯状の第２のセパレータ２を準備する。   In this embodiment, first, the strip-shaped first separator 1 is prepared for the first feeding roll 10, and the strip-shaped second separator 2 is prepared for the second feeding roll 20.

次に、第１の繰り出しロール１０から第１のセパレータ１を水平に繰り出し、放射線硬化性樹脂塗布機３０から放射線硬化性樹脂３を第１のセパレータ１の上に塗布する。その際、放射線硬化性樹脂３は、正極が配置される予定位置のほぼ中央に３ａ、３ｂとして塗布される。但し、放射線硬化性樹脂３の塗布位置は、上記位置に限定されず、また、それぞれの塗布毎に塗布位置を相違させてもよい。更に、塗布位置の数も、２箇所には限定されず、１箇所でもよく、３箇所以上でもよい。   Next, the first separator 1 is fed horizontally from the first feeding roll 10, and the radiation curable resin 3 is applied onto the first separator 1 from the radiation curable resin coating machine 30. At that time, the radiation curable resin 3 is applied as 3a, 3b in the approximate center of the position where the positive electrode is to be disposed. However, the application position of the radiation curable resin 3 is not limited to the above position, and the application position may be different for each application. Furthermore, the number of application positions is not limited to two, and may be one or three or more.

放射線硬化性樹脂３としては特に限定されないが、硬化性が良好な２官能以上の放射線硬化性樹脂が好ましい。具体的には例えば、アクリル酸、アクリル酸エステル、アクリルアミド類、メタクリル酸エステル、メタクリル酸アミド類、アリル化合物、ビニルエーテル、ビニルエステル類等を使用できる。これらの樹脂は、単独でも使用できるが、複数を組み合わせて使用することもできる。硬化に用いる放射線としては、紫外線、電子線、可視光等を使用できるが、高いエネルギーで安価に照射できる点で紫外線が好ましい。   Although it does not specifically limit as the radiation curable resin 3, The bifunctional or more radiation curable resin with favorable sclerosis | hardenability is preferable. Specifically, for example, acrylic acid, acrylic acid ester, acrylamide, methacrylic acid ester, methacrylic acid amide, allyl compound, vinyl ether, vinyl ester and the like can be used. These resins can be used alone or in combination. As radiation used for curing, ultraviolet rays, electron beams, visible light, and the like can be used, but ultraviolet rays are preferable because they can be irradiated with high energy at low cost.

次に、正極供給機４０により塗布された放射線硬化性樹脂３ａ、３ｂに接するように、端子４ａを備えた正極４を第１のセパレータ１の上に配置した後、放射線照射装置５０から放射線５０ａをセパレータ１側から照射して、放射線硬化性樹脂３ａ、３ｂを硬化して、セパレータ１と正極４とを接着する。この際に正極４は硬化した放射線硬化性樹脂３によりセパレータ１に固定され、その後の工程により正極４がセパレータ１に対してずれることは一切ない。   Next, after the positive electrode 4 provided with the terminal 4a is disposed on the first separator 1 so as to be in contact with the radiation curable resins 3a and 3b applied by the positive electrode feeder 40, the radiation 50a is irradiated with the radiation 50a. Is irradiated from the separator 1 side to cure the radiation curable resins 3a and 3b, and the separator 1 and the positive electrode 4 are bonded. At this time, the positive electrode 4 is fixed to the separator 1 by the cured radiation curable resin 3, and the positive electrode 4 is not displaced from the separator 1 by any subsequent process.

次に、第２の繰り出しロール２０から第２のセパレータ２を繰り出して、第２のセパレータ２を正極４の上に配置する。続いて、台座６０の上で加熱装置７０を用いて、第２のセパレータ２を正極４の外形に沿って密着させるとともに、第１のセパレータ１と第２のセパレータ２とを熱溶着により接合して、正極入り袋状セパレータ５を形成する。この時点では、正極入り袋状セパレータ５は、接合部５ａ及び連結部６ａを有し、正極入り袋状セパレータ連結体６を形成している。   Next, the second separator 2 is fed out from the second feeding roll 20, and the second separator 2 is disposed on the positive electrode 4. Subsequently, using the heating device 70 on the pedestal 60, the second separator 2 is brought into close contact with the outer shape of the positive electrode 4, and the first separator 1 and the second separator 2 are joined by thermal welding. Thus, the positive electrode-containing bag-like separator 5 is formed. At this point, the positive electrode-filled bag-shaped separator 5 has the joining portion 5a and the connecting portion 6a, and forms the positive-electrode-filled bag-shaped separator connector 6.

次に、正極入り袋状セパレータ連結体６の連結部６ａを切断・除去して、正極入り袋状セパレータ５を分離する。続いて、別途準備した負極７と、分離した正極入り袋状セパレータ５とを交互に積層して、図３に示す積層電極体９Ａを作製する。図３は、積層電極体９Ａの底面図である。図３では、負極７を５枚、正極入り袋状セパレータ５を４枚それぞれ積層した例を示したが、電極の枚数はこれらに限定されない。   Next, the connecting portion 6a of the positive electrode bag-like separator connector 6 is cut and removed to separate the positive electrode bag-like separator 5. Subsequently, the separately prepared negative electrode 7 and the separated positive electrode-filled bag-like separator 5 are alternately laminated to produce a laminated electrode body 9A shown in FIG. FIG. 3 is a bottom view of the laminated electrode body 9A. Although FIG. 3 shows an example in which five negative electrodes 7 and four positive electrode-containing bag-like separators 5 are stacked, the number of electrodes is not limited thereto.

最後に、作製した積層電極体９Ａを外装体に挿入し、電解液を注入して、外装体を封止すれば、本発明の非水電解質二次電池が完成する。上記外装体及び電解液については後述する。   Finally, the produced multilayer electrode body 9A is inserted into the exterior body, an electrolytic solution is injected, and the exterior body is sealed. Thus, the nonaqueous electrolyte secondary battery of the present invention is completed. The said exterior body and electrolyte solution are mentioned later.

次に、本発明の非水電解質二次電池の製造方法の他の実施形態を説明する。図４は、本発明の非水電解質二次電池の製造工程の他の一例を示す模式図である。図４では、前述の図１〜３で示した部分と対応する部分には同一の符号を付けて詳細な説明は省略する。   Next, another embodiment of the method for producing a nonaqueous electrolyte secondary battery of the present invention will be described. FIG. 4 is a schematic view showing another example of the manufacturing process of the nonaqueous electrolyte secondary battery of the present invention. In FIG. 4, parts corresponding to those shown in FIGS. 1 to 3 are given the same reference numerals, and detailed description thereof is omitted.

本実施形態でも、正極入り袋状セパレータ連結体６を、前述の図１及び図２を用いて説明した工程と同様にして形成する。本実施形態では、正極入り袋状セパレータ連結体６は４個の正極入り袋状セパレータ５を備えているが、電池の容量に応じて正極入り袋状セパレータ５の数を増減できる。   Also in the present embodiment, the positive electrode-filled bag-like separator connector 6 is formed in the same manner as the steps described with reference to FIGS. In this embodiment, the positive electrode-containing bag-like separator connector 6 includes four positive-electrode-containing bag-like separators 5, but the number of positive-electrode-containing bag-like separators 5 can be increased or decreased according to the capacity of the battery.

次に、図４に示すように、正極入り袋状セパレータ連結体６の正極入り袋状セパレータ５に対応する表側と裏側にそれぞれ負極７を配置し、正極入り袋状セパレータ連結体６の連結部６ａを折り目としてつづら折りして、正極入り袋状セパレータ５と負極７とをそれぞれ交互に積層して、図５に示す積層電極体９Ｂを作製する。   Next, as shown in FIG. 4, the negative electrode 7 is arrange | positioned at the front side and back side corresponding to the positive electrode containing bag-like separator 5 of the positive electrode containing bag-like separator connecting body 6, respectively, and the connection part of the positive electrode containing bag-like separator connecting body 6 6a is folded as a crease, and the positive electrode-filled bag-like separator 5 and the negative electrode 7 are alternately laminated to produce a laminated electrode body 9B shown in FIG.

その後は、前述したように通常の方法で本発明の非水電解質二次電池を製造する。本実施形態では、正極入り袋状セパレータ連結体６の連結部６ａの切断・除去が不要で、連結部６ａの幅を調整するのみで積層電極体９Ｂを連続的に作製できるので、生産効率を向上できる。   Thereafter, as described above, the nonaqueous electrolyte secondary battery of the present invention is manufactured by a normal method. In the present embodiment, it is not necessary to cut and remove the connecting portion 6a of the positive electrode bag-like separator connecting body 6, and the laminated electrode body 9B can be continuously produced simply by adjusting the width of the connecting portion 6a. It can be improved.

（実施形態２）
次に、本発明の非水電解質二次電池の実施形態について代表的な非水電解質二次電池であるリチウムイオン二次電池を例に説明する。 (Embodiment 2)
Next, a non-aqueous electrolyte secondary battery according to an embodiment of the present invention will be described using a lithium ion secondary battery, which is a typical non-aqueous electrolyte secondary battery, as an example.

図６は、本発明のラミネート形リチウムイオン二次電池の一例を示す平面図である。図６において、本実施形態のラミネート形リチウムイオン二次電池１００では、実施形態１で説明した積層電極体９Ａ又は９Ｂ及び非水電解液が、平面視で矩形のラミネートフィルムからなる外装体２００内に収容されている。そして、正極外部端子３００及び負極外部端子４００が、外装体２００の同じ辺から引き出されている。   FIG. 6 is a plan view showing an example of a laminated lithium ion secondary battery of the present invention. 6, in the laminated lithium ion secondary battery 100 of the present embodiment, the laminated electrode body 9A or 9B and the non-aqueous electrolyte described in the first embodiment are inside the outer package 200 made of a rectangular laminated film in plan view. Is housed in. The positive external terminal 300 and the negative external terminal 400 are drawn from the same side of the exterior body 200.

本実施形態に用いる正極は、正極活物質、正極用導電助剤、正極用バインダ等を含む混合物に、溶剤を加えて十分に混練して得た正極合剤ペーストを、正極集電体の両面に塗布して乾燥した後に、その正極合剤層を所定の厚さ及び所定の電極密度に制御することにより形成できる。   The positive electrode used in the present embodiment is a mixture of positive electrode active material, positive electrode conductive additive, positive electrode binder, and the like, and a positive electrode mixture paste obtained by sufficiently kneading the mixture with a solvent. After being applied to and dried, the positive electrode mixture layer can be formed by controlling it to a predetermined thickness and a predetermined electrode density.

上記正極活物質としては、例えば、ＬｉＣｏＯ2等のリチウムコバルト酸化物、ＬｉＭｎ2Ｏ4等のリチウムマンガン酸化物、ＬｉＮｉＯ2等のリチウムニッケル酸化物等が使用できるが、リチウムイオンを吸蔵・放出可能であればこれらに限定はされない。 Examples of the positive electrode active material include lithium cobalt oxides such as LiCoO 2 , lithium manganese oxides such as LiMn 2 O 4 , lithium nickel oxides such as LiNiO 2, etc., and can absorb and release lithium ions. If it is, it will not be limited to these.

上記正極集電体としては、構成された電池において実質的に化学的に安定な電子伝導体であれば特に限定されない。正極集電体としては、例えば、アルミニウム箔等が用いられる。   The positive electrode current collector is not particularly limited as long as it is an electron conductor that is substantially chemically stable in the battery. As the positive electrode current collector, for example, an aluminum foil or the like is used.

本実施形態に用いる負極は、負極活物質、負極用導電助剤、負極用バインダ等を含む混合物に、溶剤を加えて十分に混練して得た負極合剤ペーストを、負極集電体の両面に塗布して乾燥した後に、その負極合剤層を所定の厚さ及び所定の電極密度に制御することにより形成できる。   The negative electrode used in the present embodiment is obtained by adding a negative electrode mixture paste obtained by sufficiently kneading a mixture containing a negative electrode active material, a conductive aid for negative electrode, a binder for negative electrode, and the like, to both surfaces of the negative electrode current collector. After coating and drying, the negative electrode mixture layer can be formed by controlling the thickness to a predetermined thickness and a predetermined electrode density.

上記負極活物質としては、例えば、天然黒鉛、又は塊状黒鉛、鱗片状黒鉛、土状黒鉛等の人造黒鉛等の炭素材料が用いられるが、リチウムイオンを吸蔵・放出可能であればこれらに限定はされない。   As the negative electrode active material, for example, natural graphite, or carbon materials such as artificial graphite such as massive graphite, flake graphite, earthy graphite, etc. are used, but there is no limitation to these as long as lithium ions can be occluded / released. Not.

上記負極集電体としては、構成された電池において実質的に化学的に安定な電子伝導体であれば特に限定されない。負極集電体としては、例えば、銅箔等が用いられる。   The negative electrode current collector is not particularly limited as long as it is an electron conductor that is substantially chemically stable in the constituted battery. For example, a copper foil or the like is used as the negative electrode current collector.

本実施形態に用いるセパレータとしては、大きなイオン透過度及び所定の機械的強度を有する熱可塑性樹脂からなる微多孔性フィルムを用いることができる。   As the separator used in the present embodiment, a microporous film made of a thermoplastic resin having a large ion permeability and a predetermined mechanical strength can be used.

外装体２００としては、アルミニウム等の金属層と熱可塑性樹脂層とが積層されたラミネートフィルムを用いることができる。   As the exterior body 200, a laminate film in which a metal layer such as aluminum and a thermoplastic resin layer are laminated can be used.

上記非水電解液としては、例えば、ビニレンカーボネート（ＶＣ）、プロピレンカーボネート（ＰＣ）、エチレンカーボネート（ＥＣ）、ブチレンカーボネート（ＢＣ）、ジメチルカーボネート（ＤＭＣ）、ジエチルカーボネート（ＤＥＣ）、メチルエチルカーボネート（ＭＥＣ）、γ−ブチロラクトン等の有機溶媒を１種類又は２種類以上混合した溶媒に、例えば、ＬｉＣｌＯ4、ＬｉＰＦ6、ＬｉＢＦ4、ＬｉＡｓＦ6、ＬｉＳｂＦ6、ＬｉＣＦ3ＳＯ3等から選ばれる少なくとも１種類のリチウム塩を溶解させた電解液を用いればよい。この電解液中のＬｉイオンの濃度は、０．５〜１．５ｍｏｌ／Ｌとすればよい。 Examples of the non-aqueous electrolyte include vinylene carbonate (VC), propylene carbonate (PC), ethylene carbonate (EC), butylene carbonate (BC), dimethyl carbonate (DMC), diethyl carbonate (DEC), and methyl ethyl carbonate ( MEC), an organic solvent such as γ- butyrolactone to one or more kinds mixed solvent, for example, at least one selected from LiClO 4, LiPF 6, LiBF 4 , LiAsF 6, LiSbF 6, LiCF 3 SO 3 , etc. An electrolytic solution in which the lithium salt is dissolved may be used. The concentration of Li ions in the electrolytic solution may be 0.5 to 1.5 mol / L.

以下、実施例により本発明を説明する。   Hereinafter, the present invention will be described by way of examples.

先ず、図１及び図２に示す製造方法により正極４とセパレータ１とを放射線硬化性樹脂３により接着した。その際に放射線硬化性樹脂３の１箇所当たりの塗布量を変化させて各種のサンプルを作製した。正極４としては、厚さ１０６μｍ、縦２００ｍｍ、横８４ｍｍの正極を用いた。セパレータ１としては、厚さ２１μｍのポリエチレン製微多孔膜を用いた。放射線硬化性樹脂としては、主剤にＤＰＨＡ（ジペンタエリストールヘキサアクリレート）を６８質量部、希釈剤にＨＤＤＡ（１,６−ヘキサンジオールジアクリレート）を２９質量部、光開始剤に２,４,６−トリメチルベンゾイル−ジフェニルフォスフィンオキサイドを３質量部、それぞれ混合して用いた。この時、３０℃で測定した放射線硬化性樹脂３の粘度は、１６０ｍＰａ・ｓであった。   First, the positive electrode 4 and the separator 1 were bonded with the radiation curable resin 3 by the manufacturing method shown in FIGS. 1 and 2. At that time, various samples were prepared by changing the coating amount per one place of the radiation curable resin 3. As the positive electrode 4, a positive electrode having a thickness of 106 μm, a length of 200 mm, and a width of 84 mm was used. As the separator 1, a polyethylene microporous film having a thickness of 21 μm was used. As the radiation curable resin, 68 parts by mass of DPHA (dipentaerystol hexaacrylate) as a main agent, 29 parts by mass of HDDA (1,6-hexanediol diacrylate) as a diluent, and 2,4,4 as a photoinitiator. Three parts by mass of 6-trimethylbenzoyl-diphenylphosphine oxide were mixed and used. At this time, the viscosity of the radiation curable resin 3 measured at 30 ° C. was 160 mPa · s.

次に、各サンプルの放射線硬化性樹脂３による接着部の１箇所当たりの面積及び厚さを測定した。その後、引張試験機を用いて各サンプルについて、正極４からセパレータ１を、正極４に対して垂直方向に引っ張って接着強度を測定した。引っ張り速度は１００ｍｍ／分とした。接着強度としては、正極４からセパレータ１が剥離するまでの最大引張強度を測定した。   Next, the area and thickness per one part of the adhesion part by the radiation curable resin 3 of each sample were measured. Thereafter, for each sample, the separator 1 was pulled from the positive electrode 4 in a direction perpendicular to the positive electrode 4 using a tensile tester, and the adhesive strength was measured. The pulling speed was 100 mm / min. As the adhesive strength, the maximum tensile strength until the separator 1 was peeled from the positive electrode 4 was measured.

表１に以上の結果を示す。   Table 1 shows the above results.

Figure 2015162337
Figure 2015162337

表１から、接着強度を０．５Ｎ以上にするには、放射線硬化性樹脂の１箇所当たりの塗布量を０．００５ｍｇ以上とする必要があることが分かる。また、放射線硬化性樹脂の１箇所当たりの塗布量が０．１５ｍｇあれば接着強度としては７Ｎ以上あり、接着強度としては十分であることが分かる。また、上記塗布量が０．００５ｍｇ以上０．１５ｍｇ以下であれば、接着部の１箇所当たりの面積を０．３ｍｍ2以上７．１ｍｍ2以下とでき、上記塗布量が０．０７ｍｇ以下であれば接着部の１箇所当たりの厚さを５μｍ以下とできることが分かる。 From Table 1, it can be seen that, in order to increase the adhesive strength to 0.5 N or more, it is necessary to set the application amount of the radiation curable resin per location to 0.005 mg or more. Further, it can be seen that if the coating amount per spot of the radiation curable resin is 0.15 mg, the adhesive strength is 7 N or more, and the adhesive strength is sufficient. Further, if the application amount is 0.005 mg or more and 0.15 mg or less, the area per one part of the bonded portion can be 0.3 mm 2 or more and 7.1 mm 2 or less, and the application amount is 0.07 mg or less. In other words, it can be seen that the thickness of each bonded portion can be 5 μm or less.

次に、上記放射線硬化性樹脂の３０℃での塗布粘度を変化させて、塗布後の上記セパレータに対する上記放射線硬化性樹脂の貫通時間を測定した。その結果を表２に示す。   Next, the coating viscosity at 30 ° C. of the radiation curable resin was changed, and the penetration time of the radiation curable resin with respect to the separator after coating was measured. The results are shown in Table 2.

Figure 2015162337
Figure 2015162337

表２から、上記放射線硬化性樹脂の３０℃での塗布粘度が４０ｍＰａ・ｓ以上であれば、上記貫通時間を１秒以上とすることができ、上記放射線硬化性樹脂の硬化時間は通常１秒以下であるため、塗布された放射線硬化性樹脂がセパレータを貫通してしまうことがない。また、セパレータの内部にある程度の放射線硬化性樹脂を浸透させる必要があるため、上記塗布粘度は３００ｍＰａ・ｓ以下であることが好ましい。   From Table 2, if the coating viscosity at 30 ° C. of the radiation curable resin is 40 mPa · s or more, the penetration time can be set to 1 second or more, and the curing time of the radiation curable resin is usually 1 second. Since it is the following, the applied radiation curable resin does not penetrate the separator. Moreover, since it is necessary to permeate a certain amount of radiation-curable resin into the separator, the coating viscosity is preferably 300 mPa · s or less.

以上説明したように、本発明は、負荷特性等に優れた非水電解質二次電池及びその製造方法を提供できる。   As described above, the present invention can provide a nonaqueous electrolyte secondary battery excellent in load characteristics and the like and a method for manufacturing the same.

１ 第１のセパレータ
２ 第２のセパレータ
３ 放射線硬化性樹脂
４ 正極
５ 正極入り袋状セパレータ
６ 正極入り袋状セパレータ連結体
７ 負極
９Ａ、９Ｂ 積層電極体
１０ 第１の繰り出しロール
２０ 第２の繰り出しロール
３０ 放射線硬化性樹脂塗布機
４０ 正極供給機
５０ 放射線照射装置
５０ａ 放射線
６０ 台座
７０ 加熱装置
１００ ラミネート形リチウムイオン二次電池
２００ 外装体
３００ 正極外部端子
４００ 負極外部端子 DESCRIPTION OF SYMBOLS 1 1st separator 2 2nd separator 3 Radiation curable resin 4 Positive electrode 5 Bag-like separator containing positive electrode 6 Bag-like separator connected with positive electrode 7 Negative electrode 9A, 9B Laminated electrode body 10 First feeding roll 20 Second feeding Roll 30 Radiation curable resin coating machine 40 Positive electrode feeder 50 Radiation irradiation device 50a Radiation 60 Base 70 Heating device 100 Laminated lithium ion secondary battery 200 Exterior body 300 Positive electrode external terminal 400 Negative electrode external terminal

Claims (14)

正極と、負極と、セパレータとが積層された積層電極体を含む非水電解質二次電池であって、
前記正極及び前記負極のいずれか一方の電極と、前記セパレータとは、接着部により接着されていることを特徴とする非水電解質二次電池。 A non-aqueous electrolyte secondary battery including a laminated electrode body in which a positive electrode, a negative electrode, and a separator are laminated,
The nonaqueous electrolyte secondary battery, wherein either the positive electrode or the negative electrode and the separator are bonded by an adhesive portion. 前記正極と前記セパレータとが、前記接着部により接着されており、前記負極と前記セパレータとは、接着されていない請求項１に記載の非水電解質二次電池。   The nonaqueous electrolyte secondary battery according to claim 1, wherein the positive electrode and the separator are bonded by the bonding portion, and the negative electrode and the separator are not bonded. 前記接着部は、放射線硬化性樹脂から形成されている請求項１又は２に記載の非水電解質二次電池。   The non-aqueous electrolyte secondary battery according to claim 1, wherein the adhesion portion is formed of a radiation curable resin. 前記接着部の１箇所当たりの面積が、０．３ｍｍ2以上７．１ｍｍ2以下である請求項１〜３のいずれか１項に記載の非水電解質二次電池。 The nonaqueous electrolyte secondary battery according to any one of claims 1 to 3, wherein an area per one portion of the bonding portion is 0.3 mm 2 or more and 7.1 mm 2 or less. 前記接着部の１箇所当たりの厚さが、５μｍ以下である請求項１〜４のいずれか１項に記載の非水電解質二次電池。   The nonaqueous electrolyte secondary battery according to any one of claims 1 to 4, wherein a thickness per one portion of the adhesion portion is 5 µm or less. 前記電極と前記セパレータとの接着強度が、０．５Ｎ以上である請求項１〜５のいずれか１項に記載の非水電解質二次電池。   The non-aqueous electrolyte secondary battery according to claim 1, wherein an adhesive strength between the electrode and the separator is 0.5 N or more. 前記接着部の配置位置が、前記電極毎に異なる請求項１〜６のいずれか１項に記載の非水電解質二次電池。   The non-aqueous electrolyte secondary battery according to claim 1, wherein an arrangement position of the adhesive portion is different for each of the electrodes. 前記セパレータは、袋状セパレータを形成している請求項１〜７のいずれか１項に記載の非水電解質二次電池。   The non-aqueous electrolyte secondary battery according to claim 1, wherein the separator forms a bag-shaped separator. 請求項１〜８のいずれか１項に記載の非水電解質二次電池を製造する方法であって、
帯状のセパレータに放射線硬化性樹脂を塗布して接着部を形成する塗布工程と、
塗布された前記接着部の上に電極を配置する電極配置工程と、
前記接着部に放射線を照射して前記放射線硬化性樹脂を硬化して前記電極と前記セパレータとを接着する接着工程とを含むことを特徴とする非水電解質二次電池の製造方法。 A method for producing the nonaqueous electrolyte secondary battery according to any one of claims 1 to 8,
An application step of applying a radiation curable resin to a strip-shaped separator to form an adhesive portion;
An electrode placement step of placing an electrode on the applied adhesive portion;
The manufacturing method of the nonaqueous electrolyte secondary battery characterized by including the adhesion | attachment process of irradiating a radiation to the said adhesion part, hardening | curing the said radiation curable resin, and adhere | attaching the said electrode and the said separator. 前記放射線硬化性樹脂の１箇所当たりの塗布量が、０．００５ｍｇ以上０．１５ｍｇ以下である請求項９に記載の非水電解質二次電池の製造方法。   The method for producing a nonaqueous electrolyte secondary battery according to claim 9, wherein an application amount of the radiation curable resin per place is 0.005 mg or more and 0.15 mg or less. 前記放射線硬化性樹脂の塗布粘度が、３０℃において４０ｍＰａ・ｓ以上３００ｍＰａ・ｓ以下である請求項９又は１０に記載の非水電解質二次電池の製造方法。   The method for producing a nonaqueous electrolyte secondary battery according to claim 9 or 10, wherein the coating viscosity of the radiation curable resin is 40 mPa · s or more and 300 mPa · s or less at 30 ° C. 前記塗布工程において、前記接着部を前記電極毎に異なる位置に配置する請求項９〜１１のいずれか１項に記載の非水電解質二次電池の製造方法。   The method for manufacturing a non-aqueous electrolyte secondary battery according to claim 9, wherein in the application step, the adhesive portion is disposed at a different position for each of the electrodes. 前記接着工程の後に前記電極の上に別のセパレータを配置するセパレータ積層工程と、対向する前記セパレータ同士を接合して袋状セパレータを形成するセパレータ接合工程とを更に含む請求項９〜１２のいずれか１項に記載の非水電解質二次電池の製造方法。   Any of Claims 9-12 further including the separator lamination process which arrange | positions another separator on the said electrode after the said adhesion process, and the separator joining process which joins the said separators which oppose and form a bag-shaped separator. A method for producing a non-aqueous electrolyte secondary battery according to claim 1. 前記電極が、正極である請求項９〜１３のいずれか１項に記載の非水電解質二次電池の製造方法。   The method for producing a nonaqueous electrolyte secondary battery according to any one of claims 9 to 13, wherein the electrode is a positive electrode.
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