JP2021005457A - Electrochemical cell and manufacturing method of the same - Google Patents

Electrochemical cell and manufacturing method of the same Download PDF

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JP2021005457A
JP2021005457A JP2019117495A JP2019117495A JP2021005457A JP 2021005457 A JP2021005457 A JP 2021005457A JP 2019117495 A JP2019117495 A JP 2019117495A JP 2019117495 A JP2019117495 A JP 2019117495A JP 2021005457 A JP2021005457 A JP 2021005457A
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negative electrode
electrode body
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peripheral wall
electrochemical cell
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JP7288816B2 (en
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恒昭 玉地
Tsuneaki Tamachi
恒昭 玉地
渡邊 俊二
Shunji Watanabe
俊二 渡邊
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Seiko Instruments Inc
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    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10Energy storage using batteries
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/13Energy storage using capacitors
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50Manufacturing or production processes characterised by the final manufactured product

Abstract

To provide an electrochemical cell in the present invention.SOLUTION: An electrochemical cell of the present invention, comprises an electrode lamination body which is formed by wounding an arbitrary winding center axis so as to be circulated via a separator layer formed by a coating hardening layer in which at least one surface is coated in at least of a band-shaped positive electrode body and a band-shaped negative electrode body, is provided with an inner side container having an outer peripheral wall and an outer side container having the outer peripheral wall, and is characterized in that the electrode lamination body is housed in an outer casing body in which the outer peripheral wall of the inner side container is overlapped with the outer peripheral wall of the outer side container, is folded and fused, and is integrated.SELECTED DRAWING: Figure 1

Description

本発明は、電解化学セルとその製造方法に関する。 The present invention relates to an electrolytic chemical cell and a method for producing the same.

従来、スマートフォン、ウエアラブル機器、補聴器などの小型機器の電源として、リチウムイオン二次電池、電気化学キャパシタ等の電気化学セルが広く活用されている。
このような電気化学セルにおいて、電池容量並びに充電電流および放電電流を大きくする観点から、電気化学セル内で対向している電極どうしの面積を可能な限り大きくすることが必要とされている。電気化学セルの構造として、一対の帯状の正極電極と負極電極を帯状のセパレータを介し巻回してケースに収め、電解液をケースに封入した構造が知られている。
Conventionally, electrochemical cells such as lithium ion secondary batteries and electrochemical capacitors have been widely used as a power source for small devices such as smartphones, wearable devices, and hearing aids.
In such an electrochemical cell, it is necessary to increase the area of the electrodes facing each other in the electrochemical cell as much as possible from the viewpoint of increasing the battery capacity and the charging current and the discharging current. As a structure of an electrochemical cell, a structure in which a pair of strip-shaped positive electrodes and negative electrodes are wound around a band-shaped separator and housed in a case, and an electrolytic solution is sealed in the case is known.

例えば、電池用の多孔性セパレータとして、以下の特許文献1には、電極上にセパレータ前駆体の薄い層を印刷する工程とこの薄い層を加硫して微孔性複合セパレータ構造に変化させる工程を備える製造方法が開示されている。
以下の特許文献2には、高分子固体電解質樹脂溶液を延伸多孔質PTFE(ポリテトラフルオロエチレン)に含浸した後、溶媒を除去して得られた高分子固体電解質と、延伸多孔質PTFEの空隙中に電極触媒と高分子固体電解質を含む電極成分を充填した電極とを一体成形した複合高分子固体電解質膜/電極一体成形体が記載されている。
また、以下の特許文献3に記載のように、帯状の正極および負極とシート状のセパレータを介し巻回して電極を構成し、この電極を正極側容器と負極側容器からなる外装体の内部に収容したボタン型の電気化学セルが知られている。
For example, as a porous separator for a battery, Patent Document 1 below describes a step of printing a thin layer of a separator precursor on an electrode and a step of vulcanizing this thin layer to change it into a microporous composite separator structure. A manufacturing method comprising the above is disclosed.
In Patent Document 2 below, the voids between the polymer solid electrolyte obtained by impregnating the stretched porous PTFE (polytetrafluoroethylene) with a polymer solid electrolyte resin solution and then removing the solvent, and the stretched porous PTFE. A composite polymer solid electrolyte membrane / electrode integrally molded body in which an electrode catalyst and an electrode filled with an electrode component containing a polymer solid electrolyte are integrally molded is described.
Further, as described in Patent Document 3 below, an electrode is formed by winding a band-shaped positive electrode and a negative electrode via a sheet-shaped separator, and this electrode is placed inside an exterior body composed of a positive electrode side container and a negative electrode side container. The housed button-type electrochemical cell is known.

特開平10−334877号公報Japanese Unexamined Patent Publication No. 10-334877 特開平08−329962号公報Japanese Unexamined Patent Publication No. 08-329962 特開2016−100122号公報Japanese Unexamined Patent Publication No. 2016-100122

特許文献3に記載の構成において、帯状の正極と負極を巻回した電極を収容する外装体は、アルミニウムなどの金属箔の両面に樹脂層を積層したラミネート構造の正極側容器と負極側容器からなる外装体を用いている。また、正極側容器と負極側容器の接合部は、内側の容器の外周壁と外側の容器の外周壁を重ね合わせて折り曲げつつ重ね合わせるようにプレス加工することで形成されている。 In the configuration described in Patent Document 3, the outer body accommodating the electrode wound around the strip-shaped positive electrode and the negative electrode is composed of a positive electrode side container and a negative electrode side container having a laminated structure in which resin layers are laminated on both sides of a metal foil such as aluminum. The exterior body is used. Further, the joint portion between the positive electrode side container and the negative electrode side container is formed by press working so that the outer peripheral wall of the inner container and the outer peripheral wall of the outer container are overlapped and bent while being overlapped.

しかし、ラミネート構造の容器の外周壁をプレス加工により折り曲げ加工した場合、金属箔とともに樹脂層が引き伸ばされるので、樹脂層に欠陥が生じていた場合、樹脂層にピンホールや亀裂、筋などの欠陥部分を生じるおそれがある。
内側の容器の外周壁にこれらの欠陥部分を生じると、容器内に封入した電解液が金属箔に接触するおそれを生じる。前述の電気化学セルがリチウムイオン電池であって、金属箔がアルミニウムの場合、アルミニウムはリチウムと負極側電位で合金化する可能性があるので、負極電位によってアルミニウムの劣化が加速されるおそれがあった。
However, when the outer peripheral wall of the container having a laminated structure is bent by press working, the resin layer is stretched together with the metal foil. Therefore, if the resin layer has defects, the resin layer has defects such as pinholes, cracks, and streaks. May cause parts.
If these defective portions are formed on the outer peripheral wall of the inner container, the electrolytic solution sealed in the container may come into contact with the metal foil. When the above-mentioned electrochemical cell is a lithium ion battery and the metal foil is aluminum, aluminum may be alloyed with lithium at the negative electrode side potential, so that the negative electrode potential may accelerate the deterioration of aluminum. It was.

また、ラミネート構造の容器において外側の樹脂層は強靱であり、融点の高いナイロンなどの樹脂が適用されているが、ナイロンは親水性が高く、水分を含有すると膨潤する性質がある。外側の樹脂層に膨潤に伴う体積変化に負けてクラックを生じると、封止部分が劣化するおそれを有していた。
特に、コイン型電気化学セルの場合、内容積が小さいため、電極を構成する集電体箔と容器外周壁の間隔が狭く、構造的に内部ショートを発生しやすいという問題がある。例えば、帯状の正極および負極をシート状のセパレータを介し巻回して電極を構成する場合、少しでも巻ずれを生じると、セパレータの外側に電極がはみ出し、内部ショートが発生するおそれがある。
Further, in a container having a laminated structure, the outer resin layer is tough and a resin such as nylon having a high melting point is applied. Nylon has a high hydrophilicity and has a property of swelling when it contains water. If the outer resin layer loses the volume change due to swelling and cracks occur, the sealed portion may deteriorate.
In particular, in the case of a coin-type electrochemical cell, since the internal volume is small, the distance between the current collector foil constituting the electrode and the outer peripheral wall of the container is narrow, and there is a problem that an internal short circuit is structurally likely to occur. For example, when a band-shaped positive electrode and a negative electrode are wound around a sheet-shaped separator to form an electrode, if any winding deviation occurs, the electrode may protrude to the outside of the separator and an internal short circuit may occur.

本発明は、以上説明のような従来の実情に鑑みなされたものであり、帯状の正極と負極を巻回して電極を構成する電気化学セルの場合、ショートリスクの発生を抑制し、製造時の歩留まり向上を図ることのできる電気化学セルとその製造方法の提供を目的とする。 The present invention has been made in view of the conventional circumstances as described above, and in the case of an electrochemical cell in which a band-shaped positive electrode and a negative electrode are wound to form an electrode, the occurrence of a short-circuit risk is suppressed and the manufacturing process is performed. An object of the present invention is to provide an electrochemical cell capable of improving the yield and a method for manufacturing the same.

(1)本発明は、帯状の正極体と帯状の負極体の少なくとも一方において少なくとも一方の面を被覆した塗膜硬化層からなるセパレータ層を介し、前記正極体と前記負極体を任意の巻き中心軸を周回するように巻回してなる電極積層体を備え、外周壁を有する内側容器と外周壁を有する外側容器からなり、前記内側容器の外周壁と前記外側容器の外周壁を重ね合わせて折り曲げ融着一体化した外装体に、前記電極積層体が収容されたことを特徴とする。 (1) In the present invention, the positive electrode body and the negative electrode body are wound at an arbitrary center via a separator layer composed of a coating film curing layer covering at least one surface of at least one of the band-shaped positive electrode body and the band-shaped negative electrode body. It is provided with an electrode laminate formed by winding around a shaft, and is composed of an inner container having an outer peripheral wall and an outer container having an outer peripheral wall, and the outer peripheral wall of the inner container and the outer peripheral wall of the outer container are overlapped and bent. The electrode laminate is housed in a fused and integrated exterior body.

(2)本発明は、帯状の正極体と帯状の負極体の少なくとも一方において少なくとも一方の面を被覆した塗膜硬化層からなるセパレータ層を介し、前記正極体と前記負極体を任意の巻き中心軸を周回するように巻回してなる電極積層体を備え、正極缶と負極缶をガスケットを介し一体化した外装体に、前記電極積層体が収容されたことを特徴とする。 (2) In the present invention, the positive electrode body and the negative electrode body are wound at an arbitrary center via a separator layer composed of a coating film cured layer covering at least one surface of at least one of the band-shaped positive electrode body and the band-shaped negative electrode body. The electrode laminate is provided by winding it around a shaft, and the electrode laminate is housed in an exterior body in which a positive electrode can and a negative electrode can are integrated via a gasket.

塗膜硬化層からなるセパレータ層を備えた正極体と負極体を巻回した構造の電極積層体であれば、セパレータ層が確実に正極体と負極体を絶縁分離するので、仮に正極体と負極体に巻ずれを生じてもショートリスク発生の少ない電解化学セルを提供できる。
これに対し、テープ状のセパレータを正極体と負極体とともに巻回した構造であると、正極体または負極体に巻ずれを生じた場合、電極体の一部がセパレータ層からはみ出すので、内部ショートリスクを引き起こすおそれがある。内部ショートのリスクを回避するため、セパレータを単純に大きくすると、電気学セルとして、体積当たりの電池容量密度が低下する。このため、塗膜硬化層からなるセパレータ層を備えた正極体と負極体が巻回された電気化学セルであれば、体積当たりの電池容量密度低下を引き起こすことのない電気化学セルを提供できる。
In the case of an electrode laminate having a structure in which a positive electrode body and a negative electrode body having a separator layer composed of a coating film cured layer are wound, the separator layer reliably insulates and separates the positive electrode body and the negative electrode body. It is possible to provide an electrolytic chemical cell with less risk of short circuit even if the body is miswound.
On the other hand, in the structure in which the tape-shaped separator is wound together with the positive electrode body and the negative electrode body, when the positive electrode body or the negative electrode body is unwound, a part of the electrode body protrudes from the separator layer, so that an internal short circuit occurs. May pose a risk. Simply increasing the separator to avoid the risk of internal shorts reduces the battery capacity density per volume as an electrical cell. Therefore, an electrochemical cell in which a positive electrode body and a negative electrode body provided with a separator layer made of a coating film cured layer are wound can provide an electrochemical cell that does not cause a decrease in battery capacity density per volume.

(3)本発明の一形態に係る電気化学セルにおいて、前記帯状の正極体と前記帯状の負極体の表裏両面及び側面を含む周面に設けた塗膜硬化層が前記巻回状態で融合一体化されたセパレータ層が設けられたことが好ましい。 (3) In the electrochemical cell according to one embodiment of the present invention, the coating film cured layer provided on both the front and back surfaces of the band-shaped positive electrode body and the peripheral surface including the front and back surfaces and the side surface of the band-shaped negative electrode body is fused and integrated in the wound state. It is preferable that a modified separator layer is provided.

正極体の周面と負極体の周面を個別に覆った塗膜硬化層を一体化してなるセパレータ層であるならば、正極体と負極体の巻回時に正極体と負極体の一部に巻乱れなどを生じていても、正極体と負極体は確実にセパレータ層で覆われる。また、正極体と負極体を巻回した電極積層体の外周面も確実にセパレータ層で覆われる。この結果、内部ショートのおそれを生じない電気化学セルを提供できる。 If the separator layer is formed by integrating a coating film curing layer that individually covers the peripheral surface of the positive electrode body and the peripheral surface of the negative electrode body, it may be part of the positive electrode body and the negative electrode body when the positive electrode body and the negative electrode body are wound. Even if the winding is disturbed, the positive electrode body and the negative electrode body are surely covered with the separator layer. Further, the outer peripheral surface of the electrode laminate around which the positive electrode body and the negative electrode body are wound is also surely covered with the separator layer. As a result, it is possible to provide an electrochemical cell that does not cause an internal short circuit.

(4)本発明の一形態に係る電気化学セルにおいて、前記正極体と前記負極体の一部に延出部が形成され、前記正極側の延出部の先端側と前記負極側の延出部の先端側に前記塗膜硬化層からなるセパレータ層が形成されていない接続タブが形成されたことが好ましい。 (4) In the electrochemical cell according to one embodiment of the present invention, an extension portion is formed on the positive electrode body and a part of the negative electrode body, and the extension portion on the positive electrode side and the extension portion on the negative electrode side are extended. It is preferable that a connection tab is formed on the tip end side of the portion so that the separator layer made of the coating film curing layer is not formed.

正極側の接続タブを一方の容器側の正極端子に接続し、負極側の接続タブを他方の容器側の負極端子に接続することで、導通用のタブなどを別途用いることなく容器側の端子に正極体と負極体を接続できる。このため、導通用のタブを略することができ、導通用のタブを設けていたスペースに電極を配置できるので、体積当たりの電池容量密度の高い電気化学セルを提供できる。 By connecting the connection tab on the positive electrode side to the positive electrode terminal on one container side and the connection tab on the negative electrode side to the negative electrode terminal on the other container side, the terminal on the container side does not use a separate tab for conduction. The positive electrode body and the negative electrode body can be connected to. Therefore, the tab for conduction can be omitted, and the electrode can be arranged in the space where the tab for conduction is provided, so that an electrochemical cell having a high battery capacity density per volume can be provided.

(5)本発明の一形態に係る電気化学セルにおいて、前記内側容器の外周壁と前記外側容器の外周壁が金属箔の両面に樹脂層を設けたラミネート構造体からなることが好ましい。 (5) In the electrochemical cell according to one embodiment of the present invention, it is preferable that the outer peripheral wall of the inner container and the outer peripheral wall of the outer container are made of a laminated structure in which resin layers are provided on both sides of the metal foil.

金属箔を含むラミネート構造体からなる外装体であれば、金属箔の部分で水分の侵入を阻止することができ、外装体の内部側に外部から水分浸入のおそれのない電気化学セルを提供できる。
また、仮に、樹脂層にピンホールや裂け、筋などの欠陥が発生し、外装体の金属箔が電解液に接触し、更に、電極積層体側に接触するおそれを生じても、電極積層体と金属箔との間に塗膜硬化層からなるセパレータ層を確実に介在できるので、金属箔に電位を作用させるおそれがなく、金属箔の劣化促進を生じ難い構造を提供できる。
In the case of an exterior body made of a laminated structure containing a metal foil, the metal foil portion can prevent the intrusion of moisture, and an electrochemical cell without a risk of moisture intrusion from the outside can be provided on the inner side of the exterior body. ..
Further, even if defects such as pinholes, tears, and streaks occur in the resin layer, the metal foil of the exterior body may come into contact with the electrolytic solution, and further, even if there is a risk of contact with the electrode laminate side, the electrode laminate and the electrode laminate Since a separator layer made of a coating film curing layer can be reliably interposed between the metal foil and the metal foil, there is no risk of applying an electric potential to the metal foil, and it is possible to provide a structure in which deterioration of the metal foil is unlikely to occur.

(6)本発明の一形態に係る電気化学セルにおいて、前記帯状の正極体と前記帯状の負極体が、いずれも、前記外装体の平面視形状に類似する平面視形状の複数の電極本体と、これら複数の電極本体を接続する電極接続部を有し、前記正極体と前記負極体が前記塗膜硬化層を介し互いに渦巻き状に巻回されて一体化され、前記正極体の前記電極本体および前記電極接続部と、前記負極体の前記電極本体および前記電極接続部が、いずれも前記塗膜硬化層からなるセパレータ層に覆われたことが好ましい。 (6) In the electrochemical cell according to one embodiment of the present invention, the band-shaped positive electrode body and the band-shaped negative electrode body are both a plurality of electrode bodies having a plan view shape similar to the plan view shape of the exterior body. , The electrode connecting portion for connecting the plurality of electrode bodies is provided, and the positive electrode body and the negative electrode body are spirally wound and integrated with each other via the coating film curing layer, and the electrode body of the positive electrode body is integrated. It is preferable that the electrode connecting portion, the electrode main body of the negative electrode body, and the electrode connecting portion are all covered with a separator layer made of the coating film cured layer.

正極体と負極体が外装体の平面視形状に類似する平面視形状の複数の電極本体を備え、複数の電極本体を複数の電極接続部を介し接続した構造ならば、正極側の電極本体と負極側の電極本体を重ね合わせつつ互いに渦巻き状に巻回することで、外装体の内部に隙間無く高密度で収容できる外装体の外形に見合った形状の電極積層体を備えた電気化学セルを提供できる。そして、電極本体と電極接続部の両方をセパレータ層で覆うことにより、電極積層体全体をセパレータ層で覆った構造であり、ショートリスクの少ない電気化学セルを提供できる。 If the positive electrode body and the negative electrode body are provided with a plurality of electrode bodies having a plan view shape similar to the plan view shape of the exterior body, and the plurality of electrode bodies are connected via a plurality of electrode connection portions, the electrode body on the positive electrode side and the electrode body are connected. By winding the electrode bodies on the negative electrode side in a spiral shape while overlapping them, an electrochemical cell equipped with an electrode laminate having a shape that matches the outer shape of the exterior body can be accommodated at high density without gaps inside the exterior body. Can be provided. By covering both the electrode body and the electrode connection portion with the separator layer, the entire electrode laminate is covered with the separator layer, and an electrochemical cell with less risk of short circuit can be provided.

(7)本発明の一形態に係る電気化学セルにおいて、前記電極本体と前記電極接続部が、いずれも、金属箔からなる集電体層の表裏両面に活物質層を備えたことが好ましい。 (7) In the electrochemical cell according to one embodiment of the present invention, it is preferable that both the electrode body and the electrode connecting portion are provided with active material layers on both the front and back surfaces of a current collector layer made of a metal foil.

正極体と負極体の具体構造として、金属箔からなる集電体層の表裏両面に活物質層を備えた構造の正極体あるいは負極体を適用できる。塗布硬化層からなるセパレータ層であるならば、集電体層とその上に設けられた活物質層との積層構造であっても、正極体と負極体の全体を確実に覆うことができる。このため、例えば、巻回時に正極体と負極体に巻ずれなどを生じていても、セパレータ層で正極体と負極体を確実に覆った構造の電気化学セルを提供できる。 As a specific structure of the positive electrode body and the negative electrode body, a positive electrode body or a negative electrode body having a structure in which active material layers are provided on both the front and back surfaces of a current collector layer made of a metal foil can be applied. If the separator layer is composed of a coating and curing layer, the entire positive electrode body and negative electrode body can be reliably covered even with a laminated structure of the current collector layer and the active material layer provided on the current collector layer. Therefore, for example, it is possible to provide an electrochemical cell having a structure in which the positive electrode body and the negative electrode body are surely covered with a separator layer even if the positive electrode body and the negative electrode body are unwound during winding.

(8)本発明の一形態に係る電気化学セルは、正極体と負極体の少なくとも一方において少なくとも一方の面を被覆した塗膜硬化層からなるセパレータ層を介し、前記正極体と前記負極体を積層してなる電極積層体を備え、外周壁を有する内側容器と外周壁を有する外側容器からなり、前記内側容器の外周壁と前記外側容器の外周壁を重ね合わせて折り曲げ融着一体化した外装体に、前記電極積層体が収容されたことを特徴とする。 (8) In the electrochemical cell according to one embodiment of the present invention, the positive electrode body and the negative electrode body are connected to each other via a separator layer composed of a coating film curing layer covering at least one surface of at least one of the positive electrode body and the negative electrode body. The exterior is provided with an electrode laminate formed by laminating, and is composed of an inner container having an outer peripheral wall and an outer container having an outer peripheral wall, and the outer peripheral wall of the inner container and the outer peripheral wall of the outer container are overlapped and bent, fused and integrated. It is characterized in that the electrode laminate is housed in the body.

内側容器の外周壁と外側容器の外周壁を重ねて折り曲げつつ融着一体化した外装体であるならば、内側容器と外側容器を融着した接合部の密着性が良好で、封止性に優れた外装体を提供できる。 If the outer body is fused and integrated by overlapping and bending the outer peripheral wall of the inner container and the outer peripheral wall of the outer container, the adhesion of the joint where the inner container and the outer container are fused is good, and the sealing property is improved. It can provide an excellent exterior body.

(9)本発明に係る一形態の電気化学セルの製造方法は、(1)、(3)〜(7)のいずれかに記載の電気化学セルを製造する方法において、帯状の正極体と帯状の負極体の少なくとも一方において、少なくとも一面に硬化型の塗膜を形成した後、前記塗膜が半硬化の状態で前記正極体と前記負極体を巻回して電極積層体を構成し、この電極積層体を外装体の内部に収容して外装体の形を整えた後、前記半硬化塗膜を硬化させることを特徴とする。 (9) The method for producing an electrochemical cell according to the present invention is the method for producing an electrochemical cell according to any one of (1), (3) to (7), wherein a strip-shaped positive electrode body and a strip-shaped positive electrode are formed. After forming a curable coating film on at least one surface of at least one of the negative electrode bodies, the positive electrode body and the negative electrode body are wound around the positive electrode body in a semi-cured state to form an electrode laminate, and the electrodes are formed. It is characterized in that the semi-cured coating film is cured after the laminated body is housed inside the exterior body and the shape of the exterior body is adjusted.

半硬化状態の塗膜を周面に備えた正極体と負極体を巻回して電極積層体を構成することで正極体と負極体の互いに接する部分に存在する半硬化状態の塗膜どうしを接触させて一体化しながら巻回することができる。このように密着させた半硬化状態の塗膜を備える電極積層体を外装体の内部に収容し、外装体の形を整えた状態から半硬化状態の塗膜を完全硬化させることで、全体として形の整った状態であり、セパレータ層で電極積層体の全体を覆った構造の電気化学セルを得ることができる。
特に、外装体が金属箔と樹脂層のラミネート構造体である場合、電極積層体を収容した状態で外装体は柔軟性があり、半硬化状態の塗膜の存在も相俟って、電気化学セルとして全体形状が固まっていないが、外装体の形を整えた後、塗膜を完全硬化させることで、形の整った強固な構造の電気化学セルを提供できる。
By winding a positive electrode body and a negative electrode body having a semi-cured coating film on the peripheral surface to form an electrode laminate, the semi-cured coating films existing in the portions where the positive electrode body and the negative electrode body are in contact with each other are brought into contact with each other. It can be wound while being integrated. By accommodating the electrode laminate having the semi-cured coating film adhered in this way inside the exterior body and completely curing the semi-cured coating film from the state in which the shape of the exterior body is adjusted, as a whole. It is possible to obtain an electrochemical cell having a well-shaped state and a structure in which the entire electrode laminate is covered with a separator layer.
In particular, when the exterior body is a laminated structure of a metal foil and a resin layer, the exterior body is flexible in a state where the electrode laminate is housed, and the presence of a semi-cured coating film is also present, so that electrochemical is used. Although the overall shape of the cell is not solidified, it is possible to provide an electrochemical cell having a well-shaped and strong structure by completely curing the coating film after adjusting the shape of the exterior body.

本発明による、塗膜硬化層からなるセパレータ層を備えた正極体と負極体を巻回した構造の電極積層体であるならば、セパレータ層により確実に正極と負極を絶縁分離できるので、正極体と負極体に仮に巻ずれを生じていてもショートリスク発生の少ない電解化学セルを提供できる。 According to the present invention, if the electrode laminate has a structure in which a positive electrode body and a negative electrode body having a separator layer composed of a coating film cured layer are wound, the positive electrode body and the negative electrode body can be reliably separated by insulation by the separator layer. It is possible to provide an electrolytic chemical cell with less risk of short circuit even if the negative electrode body is miswound.

本発明に係る第1実施形態の二次電池(電気化学セル)の一部を断面とした斜視図である。It is a perspective view which made a part of the secondary battery (electrochemical cell) of 1st Embodiment which concerns on this invention a cross section. セパレータ層付きの正極体と負極体を巻回してなる電極積層体を示す斜視図である。It is a perspective view which shows the electrode laminated body formed by winding a positive electrode body and a negative electrode body with a separator layer. 同電極積層体を構成する正極体と負極体を展開した状態を示す平面図である。It is a top view which shows the developed state of the positive electrode body and the negative electrode body which make up the electrode laminated body. 図3に示す正極体と負極体からセパレータ層を除いた状態を示す平面図である。It is a top view which shows the state which removed the separator layer from the positive electrode body and the negative electrode body shown in FIG. 本発明に係る第2実施形態の二次電池(電気化学セル)の一部を断面とした斜視図である。It is a perspective view which made a part of the secondary battery (electrochemical cell) of 2nd Embodiment which concerns on this invention a cross section. 同第2実施形態の二次電池に収容される電極積層体について示すもので、(A)は負極側集電体層の一例を示す正面図、(B)は同集電体層にセパレータ層を被覆した状態を示す平面図、(C)は正極側集電体層の一例を示す正面図、(D)は同集電体層にセパレータ層を被覆した状態を示す平面図、(E)は電極積層体を示す斜視図である。The electrode laminate housed in the secondary battery of the second embodiment is shown, (A) is a front view showing an example of a negative electrode side current collector layer, and (B) is a separator layer on the current collector layer. (C) is a front view showing an example of a positive electrode side current collector layer, (D) is a plan view showing a state in which the current collector layer is covered with a separator layer, (E). Is a perspective view showing an electrode laminate. 本発明に係る第3実施形態の二次電池(電気化学セル)の断面図である。It is sectional drawing of the secondary battery (electrochemical cell) of 3rd Embodiment which concerns on this invention. 同第3実施形態の二次電池の一部を断面とした斜視図である。It is a perspective view which made a part of the secondary battery of the 3rd Embodiment as a cross section.

以下、本発明に係る電極の実施形態について図面を参照して説明する。以下の実施形態では、電気化学セルの一例として、コイン型のリチウムイオン二次電池(以下、単に「電池」という。)を挙げ、この電池に搭載される電極について説明する。
なお、以下の説明に用いる図面では、各部材を認識可能な大きさとするため、各部材の縮尺を適宜変更している。
Hereinafter, embodiments of the electrodes according to the present invention will be described with reference to the drawings. In the following embodiment, a coin-type lithium ion secondary battery (hereinafter, simply referred to as “battery”) is given as an example of an electrochemical cell, and an electrode mounted on the battery will be described.
In the drawings used in the following description, the scale of each member is appropriately changed in order to make each member recognizable.

<第1実施形態>
図1は、本発明に係る電解化学セルを二次電池に適用した第1実施形態を示す部分断面図である。
本実施形態の電池1は、平面視円形状のボタン型の電池である。この電池1は、容器状の外装体2と外装体2の内部に収容された電極積層体3を備えている。なお、図1では略されているが、外装体2の内部に電解液が充填されている。この電解液は支持塩を非水溶媒に溶解した電解液などが好適に用いられる。
<First Embodiment>
FIG. 1 is a partial cross-sectional view showing a first embodiment in which the electrolytic chemical cell according to the present invention is applied to a secondary battery.
The battery 1 of the present embodiment is a button-type battery having a circular shape in a plan view. The battery 1 includes a container-shaped exterior body 2 and an electrode laminate 3 housed inside the exterior body 2. Although omitted in FIG. 1, the outer body 2 is filled with an electrolytic solution. As the electrolytic solution, an electrolytic solution in which a supporting salt is dissolved in a non-aqueous solvent is preferably used.

(外装体)
外装体2は、電極積層体3を収容する収容部4と、収容部4の外周4aに沿って折り曲げられた封止部5と、を備える。封止部5は、例えば絞り成形によって、収容部4の外周4aに沿って折り曲げられて形成されている。
外装体2は、電極積層体3を間に挟む第1容器(外側容器)10および第2容器(内側容器)20を備える。第1容器10および第2容器20は、それぞれラミネート構造体(ラミネートフィルム)により形成されている。ラミネート構造体は、金属箔(金属層)と、重ね合わせ面(内側面)に設けられ金属箔を被覆する融着層(樹脂層)と、外側面に設けられ金属箔を被覆する保護層(樹脂層)とを有する。金属層は、例えばアルミニウムやステンレス鋼等からなり、外気や水蒸気を遮断する金属箔により形成されている。重ね合わせ面の融着層は、例えば、ポリオレフィンのポリエチレンやポリプロピレン等の熱可塑性樹脂の単体やコポリマーから形成されている。外側面の保護層は、例えば、上述のポリオレフィンや、ポリエチレンテレフタレート等のポリエステル、ナイロン等から形成される。
(Exterior body)
The exterior body 2 includes an accommodating portion 4 for accommodating the electrode laminate 3, and a sealing portion 5 bent along the outer circumference 4a of the accommodating portion 4. The sealing portion 5 is formed by being bent along the outer peripheral 4a of the accommodating portion 4 by, for example, drawing.
The outer body 2 includes a first container (outer container) 10 and a second container (inner container) 20 that sandwich the electrode laminate 3 in between. The first container 10 and the second container 20 are each formed of a laminated structure (laminated film). The laminated structure includes a metal foil (metal layer), a fusion layer (resin layer) provided on the overlapping surface (inner side surface) and covering the metal foil, and a protective layer provided on the outer surface and covering the metal foil (the protective layer). It has a resin layer). The metal layer is made of, for example, aluminum or stainless steel, and is formed of a metal foil that blocks outside air and water vapor. The fused layer of the overlapping surface is formed of, for example, a simple substance or a copolymer of a thermoplastic resin such as polyethylene or polypropylene of polyolefin. The protective layer on the outer side surface is formed of, for example, the above-mentioned polyolefin, polyester such as polyethylene terephthalate, nylon, or the like.

第1容器10は、円形状の第1底壁部11と、第1底壁部11の外周から筒状に延びる第1周壁部12を備える。第1底壁部11の中心には第1貫通孔13が形成されている。
第1底壁部11の内面には、第1シーラントリング14を介して銅板または銅板にニッケルプレートなどを一体化した負極プレート15が熱融着されている。第1シーラントリング14は、ポリオレフィンのポリエチレンやポリプロピレンなどの熱可塑性樹脂を用いて形成された、シーラントフィルムをリング状に成形したものである。
The first container 10 includes a circular first bottom wall portion 11 and a first peripheral wall portion 12 extending in a tubular shape from the outer periphery of the first bottom wall portion 11. A first through hole 13 is formed in the center of the first bottom wall portion 11.
On the inner surface of the first bottom wall portion 11, a negative electrode plate 15 in which a copper plate or a nickel plate or the like is integrated with the copper plate is heat-sealed via a first sealant ring 14. The first sealant ring 14 is a ring-shaped sealant film formed by using a thermoplastic resin such as polyolefin polyethylene or polypropylene.

負極プレート15の内面は、電極積層体3の後述する負極体30の接続タブ35(図2参照)に接続されている。負極プレート15の外面の中央には、ニッケルプレートなどの耐摩耗性プレートが溶接されていることが好ましい。負極プレート15は、第1貫通孔13を貫通して外部に露出され、電池1の負極端子として機能する。また、負極プレート15をニッケルまたはニッケル合金製とするならば、ニッケルプレートは省略してもよい。 The inner surface of the negative electrode plate 15 is connected to a connection tab 35 (see FIG. 2) of the negative electrode body 30 described later in the electrode laminate 3. A wear-resistant plate such as a nickel plate is preferably welded to the center of the outer surface of the negative electrode plate 15. The negative electrode plate 15 penetrates the first through hole 13 and is exposed to the outside, and functions as a negative electrode terminal of the battery 1. If the negative electrode plate 15 is made of nickel or a nickel alloy, the nickel plate may be omitted.

第2容器20は、円形状の第2底壁部21と、第2底壁部21の外周縁から筒状に延びる第2周壁部22と、第2周壁部22の開口縁から第2周壁部22の外側に向けて断面U字状になるように折り曲げられて第2底壁部21側に延びる折曲部23を備えている。
第2底壁部21は、電極積層体3を挟んで第1容器10の第1底壁部11と反対側に配置されている。第2底壁部21は、第1容器10の第1底壁部11と同等の外径に形成されている。第2底壁部21の中心には、第2貫通孔24が形成されている。
The second container 20 has a circular second bottom wall portion 21, a second peripheral wall portion 22 extending in a tubular shape from the outer peripheral edge of the second bottom wall portion 21, and a second peripheral wall from the opening edge of the second peripheral wall portion 22. A bent portion 23 that is bent toward the outside of the portion 22 so as to have a U-shaped cross section and extends toward the second bottom wall portion 21 is provided.
The second bottom wall portion 21 is arranged on the opposite side of the first container 10 from the first bottom wall portion 11 with the electrode laminate 3 interposed therebetween. The second bottom wall portion 21 is formed to have an outer diameter equivalent to that of the first bottom wall portion 11 of the first container 10. A second through hole 24 is formed in the center of the second bottom wall portion 21.

図1の構造では、第1周壁部12と第2周壁部22の外径が同一であるため、第1周壁部12において第2周壁部12側の端部に段部12aを介し径を若干大きくした接続周壁12bが形成され、この接続周壁12bが第2周壁部22の外側に接合されている。
なお、第1周壁部12の外径を接続周壁12bの外径と同一に形成した場合は、段部12aと接続周壁12bを省略し、第1周壁部12の開口側を直に第2周壁部22に外挿しても良い。
In the structure of FIG. 1, since the outer diameters of the first peripheral wall portion 12 and the second peripheral wall portion 22 are the same, the diameter of the first peripheral wall portion 12 is slightly smaller than that of the end portion on the second peripheral wall portion 12 side via the step portion 12a. An enlarged connecting peripheral wall 12b is formed, and the connecting peripheral wall 12b is joined to the outside of the second peripheral wall portion 22.
When the outer diameter of the first peripheral wall portion 12 is formed to be the same as the outer diameter of the connecting peripheral wall portion 12b, the step portion 12a and the connecting peripheral wall portion 12b are omitted, and the opening side of the first peripheral wall portion 12 is directly connected to the second peripheral wall portion. It may be externally attached to the portion 22.

第2底壁部21の内面には、第2シーラントリング25を介してアルミニウムなどからなる正極プレート26が熱融着されている。第2シーラントリング25は、第1シーラントリング14と同様に、熱可塑性樹脂により形成されている。
正極プレート26の内面は、電極積層体2の後述する正極体40の接続タブ45(図2参照)に接続されている。正極プレート26の外面の中央には、ニッケルプレートなどの低接触抵抗のプレートが溶接されていることが好ましい。この場合のニッケルプレートは、第2貫通孔24を貫通して外部に露出され、電池1の正極端子として機能する。なお、例えば、アルミニウムからなる正極プレート26に代えて、ステンレス鋼などからなる正極プレートを用いることもできる。
A positive electrode plate 26 made of aluminum or the like is heat-sealed on the inner surface of the second bottom wall portion 21 via a second sealant ring 25. The second sealant ring 25 is made of a thermoplastic resin like the first sealant ring 14.
The inner surface of the positive electrode plate 26 is connected to a connection tab 45 (see FIG. 2) of the positive electrode body 40, which will be described later, of the electrode laminate 2. It is preferable that a plate having low contact resistance such as a nickel plate is welded to the center of the outer surface of the positive electrode plate 26. The nickel plate in this case penetrates the second through hole 24 and is exposed to the outside, and functions as a positive electrode terminal of the battery 1. For example, instead of the positive electrode plate 26 made of aluminum, a positive electrode plate made of stainless steel or the like can be used.

第2周壁部22は、第2底壁部21の外周から第1容器10の第1底壁部11に向けて筒状に延びている。第2周壁部22は、収容部4の外周4aを形成する。折曲部23は、第2周壁部22のうち、第1底壁部11側の端部から第2周壁部22に沿って第2底壁部21側へ筒状になるように折り曲げられている。折曲部23は、第2周壁部22に対して外側に間隔をおいて配置されている。
第2周壁部22は、第1周壁部12の接続壁12bの内側で、かつ、折曲部23の内側に配置されている。また、折曲部23は、第1周壁部12の接続壁12bの内側に配置され、折曲部23の融着層と接続壁12bの融着層とが熱融着されている。
The second peripheral wall portion 22 extends in a tubular shape from the outer periphery of the second bottom wall portion 21 toward the first bottom wall portion 11 of the first container 10. The second peripheral wall portion 22 forms the outer circumference 4a of the accommodating portion 4. The bent portion 23 is bent so as to form a tubular shape from the end portion on the first bottom wall portion 11 side of the second peripheral wall portion 22 toward the second bottom wall portion 21 along the second peripheral wall portion 22. There is. The bent portions 23 are arranged at intervals on the outside with respect to the second peripheral wall portion 22.
The second peripheral wall portion 22 is arranged inside the connecting wall 12b of the first peripheral wall portion 12 and inside the bent portion 23. Further, the bent portion 23 is arranged inside the connecting wall 12b of the first peripheral wall portion 12, and the fusion layer of the bent portion 23 and the fusion layer of the connecting wall 12b are heat-sealed.

折曲部23の融着層と接続壁12bの融着層とが超音波又は加熱等により融着されることにより、封止部5が形成されている。よって、収容部4の外周が封止部5で封止されている。以上の構造により、第1容器10および第2容器20が重ね合わされて接合され、外装体2が形成されている。封止部5は、収容部4の外側に筒状に形成され、かつ、収容部4の外周4aに沿って折り曲げられている。
収容部4には、第1容器10と第2容器20とが重ね合されることにより密封空間が形成されている。具体的に、収容部4は、第1底壁部11、第2底壁部21、および第2周壁部22により画成され、平面視で円形に形成されている。
The sealing portion 5 is formed by fusing the fusion layer of the bent portion 23 and the fusion layer of the connecting wall 12b by ultrasonic waves, heating, or the like. Therefore, the outer circumference of the accommodating portion 4 is sealed by the sealing portion 5. With the above structure, the first container 10 and the second container 20 are overlapped and joined to form the exterior body 2. The sealing portion 5 is formed in a tubular shape on the outside of the accommodating portion 4, and is bent along the outer circumference 4a of the accommodating portion 4.
A sealed space is formed in the accommodating portion 4 by superimposing the first container 10 and the second container 20. Specifically, the accommodating portion 4 is defined by the first bottom wall portion 11, the second bottom wall portion 21, and the second peripheral wall portion 22, and is formed in a circular shape in a plan view.

(電極積層体)
図2は、第1実施形態の電極積層体3を示す斜視図であり、この電極積層体3は、図3に示すように負極側セパレータ層36で被覆された負極体30と正極側セパレータ層46で被覆された正極体40からなる。
電極積層体3は、負極体30および正極体40を互い違いに積層するように折り畳まれた電極積層体である。具体的に、電極積層体3は、セパレータ層36、46を介して負極体30と正極体40とを図2に示すように重ね合わせて扁平状に巻回することにより形成されている。負極体30は、上述した負極プレート15に接続され、正極体40は、上述した正極プレート26に接続されている。
(Electrode laminate)
FIG. 2 is a perspective view showing the electrode laminate 3 of the first embodiment, and the electrode laminate 3 is a negative electrode body 30 and a positive electrode side separator layer coated with a negative electrode side separator layer 36 as shown in FIG. It is composed of a positive electrode body 40 coated with 46.
The electrode laminate 3 is an electrode laminate that is folded so that the negative electrode body 30 and the positive electrode body 40 are alternately laminated. Specifically, the electrode laminate 3 is formed by superimposing the negative electrode body 30 and the positive electrode body 40 via the separator layers 36 and 46 and winding them in a flat shape as shown in FIG. The negative electrode body 30 is connected to the negative electrode plate 15 described above, and the positive electrode body 40 is connected to the positive electrode plate 26 described above.

負極側セパレータ層36は負極体30において後述する接続タブ35の先端部を除く全体を覆うように形成されている。正極側セパレータ層46は負極体40において後述する接続タブ45の先端部を除く全体を覆うように形成されている。
このため、セパレータ層36、46は、負極体30と正極体40を巻回した状態において負極体30および正極体40の周囲およびこれらの層間に配置され、負極体30と正極体40とが絶縁分離される。なお、図2においては層厚を無視して負極側セパレータ層36の存在位置のみを表示し、正極側セパレータ46の図示を省略しているが、セパレータ36、46は少なくとも負極体30と正極体40とが対向する領域の全体で負極体30と正極体40との間に介在するように、かつ、負極側セパレータ層36が負極体30を覆うように、正極側セパレータ層46が正極体40を覆うように配置されている。
以下、負極体30および正極体40が巻回されて積層された方向を積層方向と称する。なお、巻回とは、特定の巻回中心軸の周囲を周回するように巻かれることである。
The negative electrode side separator layer 36 is formed so as to cover the entire negative electrode body 30 except for the tip end portion of the connection tab 35 described later. The positive electrode side separator layer 46 is formed so as to cover the entire negative electrode body 40 except for the tip end portion of the connection tab 45 described later.
Therefore, the separator layers 36 and 46 are arranged around the negative electrode body 30 and the positive electrode body 40 and between these layers in a state where the negative electrode body 30 and the positive electrode body 40 are wound around, and the negative electrode body 30 and the positive electrode body 40 are insulated from each other. Be separated. In FIG. 2, only the position where the negative electrode side separator layer 36 exists is shown ignoring the layer thickness, and the positive electrode side separator 46 is not shown. However, the separators 36 and 46 are at least the negative electrode body 30 and the positive electrode body. The positive electrode side separator layer 46 is the positive electrode body 40 so as to be interposed between the negative electrode body 30 and the positive electrode body 40 in the entire region facing the 40, and so that the negative electrode side separator layer 36 covers the negative electrode body 30. It is arranged so as to cover.
Hereinafter, the direction in which the negative electrode body 30 and the positive electrode body 40 are wound and laminated is referred to as a lamination direction. In addition, winding means winding so as to orbit around a specific winding central axis.

負極体30は、金属材料により形成された箔状の負極集電体と、負極集電体の片面または両面に塗工された負極活物質層とを備えたシート状の部材である。負極集電体は、例えば銅やステンレス等の金属箔により形成されている。金属箔の厚さは一例として数μm程度である。負極活物質は、例えば、シリコンやシリコン酸化物、グラファイト、ハードカーボン、チタン酸リチウム等の単体又は混合物である。
負極活物質層の形成材料として、負極活物質に加え、導電助剤(例えば、グラファイト等)、バインダ(例えば、ポリフッ化ビニリデンやスチレンブタジエンゴム(SBR)のディスパージョン等)、増粘剤(例えば、カルボキシメチルセルロース(CMC)等)、溶剤(例えば、N−メチルピロリドン等の任意の溶媒)を混合して負極用スラリーを作製することができる。負極活物質層を形成するための構成材料を含む塗布液を「負極用スラリー」ということができる。この負極用スラリーを負極側集電体に塗布し、乾燥させることにより負極活物質層を形成できる。
The negative electrode body 30 is a sheet-like member including a foil-shaped negative electrode current collector formed of a metal material and a negative electrode active material layer coated on one or both sides of the negative electrode current collector. The negative electrode current collector is formed of, for example, a metal foil such as copper or stainless steel. The thickness of the metal foil is, for example, about several μm. The negative electrode active material is, for example, a simple substance or a mixture of silicon, silicon oxide, graphite, hard carbon, lithium titanate and the like.
As a material for forming the negative electrode active material layer, in addition to the negative electrode active material, a conductive auxiliary agent (for example, graphite), a binder (for example, a dispersion of polyvinylidene fluoride or styrene-butadiene rubber (SBR)), and a thickener (for example, a thickener). , Carboxymethyl cellulose (CMC), etc.) and a solvent (for example, any solvent such as N-methylpyrrolidone) can be mixed to prepare a slurry for a negative electrode. A coating liquid containing a constituent material for forming the negative electrode active material layer can be referred to as a “negative electrode slurry”. The negative electrode active material layer can be formed by applying this negative electrode slurry to the negative electrode side current collector and drying it.

正極体40は、金属材料により形成された箔状の正極集電体と、正極集電体の片面または両面に塗工された正極活物質層と、を備えた1枚のシート状の部材である。正極集電体は、例えばアルミニウムやステンレス等の金属箔により形成されている。金属箔の厚さは一例として10数μm程度である。正極活物質は、例えば、コバルト酸リチウムやチタン酸リチウム、マンガン酸リチウム等のように、リチウムと遷移金属とを含む複合酸化物である。
正極活物質層の形成材料として、上述の正極活物質に加え、導電助剤(例えば、グラファイト等)、バインダ(例えば、ポリフッ化ビニリデン等)、溶剤(例えばN−メチルピロリドン等の任意の溶媒)を混合して正極用スラリーを作製することができる。正極活物質層を形成するための構成材料を含む塗布液を「正極用スラリー」ということができる。この正極用スラリーを正極側集電体に塗布し、乾燥させることにより正極活物質層を形成できる。
The positive electrode body 40 is a single sheet-like member including a foil-shaped positive electrode current collector formed of a metal material and a positive electrode active material layer coated on one or both sides of the positive electrode current collector. is there. The positive electrode current collector is formed of, for example, a metal foil such as aluminum or stainless steel. The thickness of the metal foil is, for example, about 10 μm. The positive electrode active material is a composite oxide containing lithium and a transition metal, such as lithium cobalt oxide, lithium titanate, and lithium manganate.
As a material for forming the positive electrode active material layer, in addition to the above-mentioned positive electrode active material, a conductive additive (for example, graphite, etc.), a binder (for example, polyvinylidene fluoride, etc.), a solvent (for example, any solvent such as N-methylpyrrolidone). Can be mixed to prepare a slurry for a positive electrode. A coating liquid containing a constituent material for forming a positive electrode active material layer can be referred to as a “positive electrode slurry”. The positive electrode active material layer can be formed by applying this positive electrode slurry to the positive electrode side current collector and drying it.

セパレータ層36、46は、一例としてリチウムイオン導電性を有する樹脂層である。
セパレータ層36、46は、以下の塗料を負極体30と正極体40の必要箇所に塗布して塗膜を形成し、この塗膜を硬化させて形成した樹脂層からなる。
The separator layers 36 and 46 are resin layers having lithium ion conductivity as an example.
The separator layers 36 and 46 are composed of a resin layer formed by applying the following paints to necessary parts of the negative electrode body 30 and the positive electrode body 40 to form a coating film and curing the coating film.

セパレータ層36、46を構成するための塗料としては、例えば、ポリエチレンオキシド(PEO)、ポリプロピレンオキシド(PPO)、もしくはそれらの共重合体と電解液に支持塩として加えたリチウム塩をアセトニトリル等の溶媒に溶かした塗料を用いることができる。また、塗料自体にリチウムイオン導電性が無くとも、電解液を湿潤することで、イオン導電性を付与できる材料を用いても良く、例えば、ポリフッ化ビニリデン(PVDF)やポリフッ化ビニリデン−ヘキサフルオロプロピレン(PVDF−HFP)と電解液に支持塩として加えたリチウム塩をアセトンやN-メチル-2-ピロリドン (NMP)等の溶媒に溶かした溶液を用いても良い。
さらに、塗料に含まれる樹脂に無機物を混合することで、イオン導電性を付与しても良い。その場合、無機物自身がイオン導電性を有していても良いが、無機物と樹脂の界面に形成された層がイオン導電性を発現することでも良い。
添加する無機物としては、酸化アルミニウム粉末、酸化チタニウム粉末、酸化ケイ素粉末、酸化亜鉛粉末、酸化マグネシウム粉末の単体、又は、混合物を種々の配合で混和し利用することが出来る。この時、無機物の粒子径は、5nm〜1μmの物が好ましい。
これら塗料を塗布して塗膜を形成した後に、加熱や光照射、乾燥等の手段で溶媒を飛ばし、塗膜を硬化することで、セパレータ層36、46を形成できる。また、セパレータ層36、46としての強度を補強するために、無機または有機の粒状やフィラー状の粉末を同時に塗料中に溶かし込むことも効果的である。
As the coating material for forming the separator layers 36 and 46, for example, polyethylene oxide (PEO), polypropylene oxide (PPO), or a copolymer thereof and a lithium salt added as a supporting salt to the electrolytic solution are added to a solvent such as acetonitrile. A paint dissolved in is used. Further, even if the coating material itself does not have lithium ion conductivity, a material that can impart ion conductivity by moistening the electrolytic solution may be used. For example, polyvinylidene fluoride (PVDF) or polyvinylidene fluoride-hexafluoropropylene may be used. A solution obtained by dissolving (PVDF-HFP) and a lithium salt added as a supporting salt to the electrolytic solution in a solvent such as acetone or N-methyl-2-pyrrolidone (NMP) may be used.
Further, ionic conductivity may be imparted by mixing an inorganic substance with the resin contained in the paint. In that case, the inorganic substance itself may have ionic conductivity, but the layer formed at the interface between the inorganic substance and the resin may exhibit ionic conductivity.
As the inorganic substance to be added, a simple substance or a mixture of aluminum oxide powder, titanium oxide powder, silicon oxide powder, zinc oxide powder and magnesium oxide powder can be mixed and used in various formulations. At this time, the particle size of the inorganic substance is preferably 5 nm to 1 μm.
After applying these paints to form a coating film, the solvent is blown off by means such as heating, light irradiation, and drying to cure the coating film, whereby the separator layers 36 and 46 can be formed. Further, in order to reinforce the strength of the separator layers 36 and 46, it is also effective to simultaneously dissolve inorganic or organic granular or filler-like powder in the paint.

図1に示すように、電極積層体3は、外装体2の収容部4内に高密度で配置されるように、収容部4内の密封空間の形状に対応する形状に形成されている(図1参照)。すなわち、電極積層体3は、積層方向から見て、円形状に形成されている。なお、電極積層体3を積層方向から見た形状を基本形状と定義する。 As shown in FIG. 1, the electrode laminate 3 is formed in a shape corresponding to the shape of the sealed space in the housing portion 4 so as to be arranged at a high density in the housing portion 4 of the exterior body 2 ( (See FIG. 1). That is, the electrode laminate 3 is formed in a circular shape when viewed from the stacking direction. The shape of the electrode laminate 3 viewed from the stacking direction is defined as the basic shape.

ここで、電極積層体3の展開状態における負極体30と正極体40の形状について説明する。
図3は、セパレータ層を備えた第1実施形態の負極体30および正極体40の展開状態を示す平面図であり、図4は、セパレータ層を除いた負極体30および正極体40の展開状態を示す平面図である。
図3、図4に示すように、負極体30は、一列に並んで配置された複数(図示の例では8個)の略円形状の負極本体31と、隣り合う一対の負極本体31を接続する少なくとも1つ(図示の例では7個)の電極接続部32と、負極本体31から延出する負極タブ35を備える。負極本体31は、電極積層体3において積層方向に直交する面に沿って平坦に延びる部分である(図2参照)。
電極接続部32は、積層時に複数の負極本体31が互いに重なるように、積層電極体2の側部において折り返される部分である(図2参照)。負極タブ35は、上述した負極プレート15に接続される部分である。負極本体31および電極接続部32のそれぞれの表裏面には、負極活物質を塗布した負極活物質層が形成されている。負極タブ35の先端部の表裏面には、負極活物質層が塗布されておらず、負極集電体が露出されている。
Here, the shapes of the negative electrode body 30 and the positive electrode body 40 in the deployed state of the electrode laminate 3 will be described.
FIG. 3 is a plan view showing the expanded state of the negative electrode body 30 and the positive electrode body 40 of the first embodiment provided with the separator layer, and FIG. 4 is the expanded state of the negative electrode body 30 and the positive electrode body 40 excluding the separator layer. It is a top view which shows.
As shown in FIGS. 3 and 4, the negative electrode body 30 connects a plurality of (8 in the illustrated example) substantially circular negative electrode bodies 31 arranged side by side in a row and a pair of adjacent negative electrode bodies 31. It is provided with at least one electrode connecting portion (7 in the illustrated example) and a negative electrode tab 35 extending from the negative electrode main body 31. The negative electrode body 31 is a portion of the electrode laminate 3 that extends flat along a plane orthogonal to the lamination direction (see FIG. 2).
The electrode connecting portion 32 is a portion that is folded back at the side portion of the laminated electrode body 2 so that the plurality of negative electrode bodies 31 overlap each other during lamination (see FIG. 2). The negative electrode tab 35 is a portion connected to the negative electrode plate 15 described above. A negative electrode active material layer coated with a negative electrode active material is formed on the front and back surfaces of the negative electrode main body 31 and the electrode connecting portion 32, respectively. The negative electrode active material layer is not applied to the front and back surfaces of the tip of the negative electrode tab 35, and the negative electrode current collector is exposed.

以下、複数の負極本体31が並ぶ方向を負極連結方向(第1方向)と称し、負極連結方向に直交する方向を負極幅方向と称する。また、負極連結方向において、複数の負極本体31のうち電極積層体3の最も巻回中心側に配置される負極本体31に対し、電極積層体3の外周側に配置される負極本体31側を「外周側」と定義し、その反対方向を「内周側」と定義する。また、以下では、複数の負極本体31について、最内周の負極本体31から外周側に順に序数を付して説明する。換言すると、Nを自然数とし、最内周の負極本体31から外周側に数えてN番目の負極本体を第N負極本体と称する。例えば、最内周の負極本体31は、第1負極本体である。複数の電極接続部32についても同様である。 Hereinafter, the direction in which the plurality of negative electrode bodies 31 are lined up is referred to as a negative electrode connecting direction (first direction), and the direction orthogonal to the negative electrode connecting direction is referred to as a negative electrode width direction. Further, in the negative electrode connecting direction, the negative electrode main body 31 side arranged on the outer peripheral side of the electrode laminated body 3 is opposed to the negative electrode main body 31 arranged on the most winding center side of the electrode laminated body 3 among the plurality of negative electrode main bodies 31. It is defined as "outer circumference side", and the opposite direction is defined as "inner circumference side". Further, in the following, the plurality of negative electrode main bodies 31 will be described with ordinal numbers in order from the innermost peripheral negative electrode main body 31 to the outer peripheral side. In other words, N is a natural number, and the Nth negative electrode body counted from the innermost negative electrode body 31 to the outer peripheral side is referred to as the Nth negative electrode body. For example, the innermost peripheral negative electrode body 31 is the first negative electrode body. The same applies to the plurality of electrode connection portions 32.

複数の負極本体31は、負極連結方向から見て負極幅方向の中心が互いに重なるように配置されている。複数の負極本体31は、円の一部が欠けた形状に形成されている。負極本体31のうち最外周に配置される第8負極本体31Hを除く負極本体31は、上記基本形状に対して負極連結方向の寸法を徐々に小さくするように、負極連結方向の直線部33全体が上記基本形状に対して中心軸寄りに設けられている。 The plurality of negative electrode bodies 31 are arranged so that the centers in the negative electrode width direction are overlapped with each other when viewed from the negative electrode connecting direction. The plurality of negative electrode bodies 31 are formed in a shape in which a part of a circle is missing. The negative electrode body 31 excluding the eighth negative electrode body 31H arranged on the outermost periphery of the negative electrode body 31 has the entire straight portion 33 in the negative electrode connecting direction so as to gradually reduce the dimension in the negative electrode connecting direction with respect to the above basic shape. Is provided closer to the central axis with respect to the above basic shape.

複数の電極接続部32は、負極連結方向で隣り合う一対の負極本体31の間に設けられている。各電極接続部32は、負極連結方向の中間部が最も幅狭になるように形成されている。なお、中間部とは、対象の両端間の中央のみならず、対象の両端間の内側の範囲を含む意とする。電極接続部32の負極幅方向の両側の外縁は、負極幅方向に窪む円弧状に延びている。複数の電極接続部32において負極連結方向における寸法は、最内周に配置される第1電極接続部32Aから離れるに従い大きくなっている。換言すると、複数の電極接続部32は、内周側に隣り合う電極接続部32よりも負極連結方向に徐々に大きくなるように形成されている。 The plurality of electrode connecting portions 32 are provided between a pair of negative electrode main bodies 31 adjacent to each other in the negative electrode connecting direction. Each electrode connecting portion 32 is formed so that the intermediate portion in the negative electrode connecting direction has the narrowest width. The intermediate portion means not only the center between both ends of the target but also the inner range between both ends of the target. The outer edges of the electrode connecting portion 32 on both sides in the negative electrode width direction extend in an arc shape recessed in the negative electrode width direction. The dimensions of the plurality of electrode connecting portions 32 in the negative electrode connecting direction increase as the distance from the first electrode connecting portion 32A arranged on the innermost circumference increases. In other words, the plurality of electrode connecting portions 32 are formed so as to be gradually larger in the negative electrode connecting direction than the electrode connecting portions 32 adjacent to the inner peripheral side.

負極タブ35は、第8負極本体31Hから第1負極本体31Aと反対側に延出されている。負極タブ35は、複数の電極接続部32よりも狭い幅で負極連結方向に延びている。
以上構成の負極体30において、負極タブ35の先端側を除く部分の全体が負極側セパレータ層36で覆われている(図3参照)。すなわち、負極本体31の表裏面に加えて周面(側面)と電極接続部32の表裏面に加えて側面が負極側セパレータ層36により覆われている。
The negative electrode tab 35 extends from the eighth negative electrode body 31H to the side opposite to the first negative electrode body 31A. The negative electrode tab 35 extends in the negative electrode connecting direction with a width narrower than that of the plurality of electrode connecting portions 32.
In the negative electrode body 30 having the above configuration, the entire portion of the negative electrode tab 35 except the tip end side is covered with the negative electrode side separator layer 36 (see FIG. 3). That is, in addition to the front and back surfaces of the negative electrode body 31, the peripheral surface (side surface) and the front and back surfaces of the electrode connecting portion 32 and the side surface are covered with the negative electrode side separator layer 36.

先に説明したように負極側セパレータ層36は塗膜を硬化させて形成したものである。図4に示す負極体30に対し、負極タブ先端側を除く部分の表裏面に塗料を塗布すると、負極体30の周面側(周端面側)にも塗料の回り込みを生じさせることができるので、負極タブ35の先端部分を除いて負極体30のほぼ全体を覆う負極側セパレータ層36を形成できる。
塗料については塗膜形成後、熱により硬化する塗料を用いた場合は硬化温度まで加熱し、紫外線等の光照射により硬化する塗料を用いた場合は硬化のために必要な波長の光を必要な強度で照射し、乾燥により硬化する塗料の場合は適切な温度で乾燥することにより、塗料を硬化できる。塗料の硬化により、図3に示すようにセパレータ層36で覆った構造の負極体30を得ることができる。
As described above, the negative electrode side separator layer 36 is formed by curing the coating film. When the paint is applied to the front and back surfaces of the negative electrode body 30 shown in FIG. 4 except for the tip end side of the negative electrode tab, the paint can wrap around on the peripheral surface side (peripheral end surface side) of the negative electrode body 30. The negative electrode side separator layer 36 can be formed so as to cover almost the entire negative electrode body 30 except for the tip portion of the negative electrode tab 35.
As for the paint, after forming the coating film, if a paint that cures by heat is used, it is heated to the curing temperature, and if a paint that cures by irradiation with light such as ultraviolet rays is used, light of the wavelength required for curing is required. In the case of a paint that is irradiated with intensity and cured by drying, the paint can be cured by drying at an appropriate temperature. By curing the paint, a negative electrode body 30 having a structure covered with the separator layer 36 can be obtained as shown in FIG.

次に、電極積層体3の展開状態における正極体40の形状について説明する。
図3、図4に示すように正極体40は、一列に並んで配置された複数(図示の例では8個)の正極本体41と、隣り合う一対の正極本体41を接続する少なくとも1つ(図示の例では7個)の電極接続部42と、正極本体41から延出する正極タブ45を有する。
正極本体41は、電極積層体3において積層方向の垂直面に沿って平坦に延びる部分である。電極接続部42は、複数の正極本体41が負極本体31に重なるように、積層電極体2の側部において折り返される部分である。正極タブ45は、上述した正極プレート26に接続される部分である。正極本体41および電極接続部42それぞれの全体の表面には、正極活物質を塗布した正極活物質層が形成されている。正極タブ45の先端部の表面には、正極集電体が露出されている。
Next, the shape of the positive electrode body 40 in the expanded state of the electrode laminate 3 will be described.
As shown in FIGS. 3 and 4, the positive electrode body 40 is at least one (8) connected to a plurality of (8 in the illustrated example) positive electrode bodies 41 arranged side by side in a row and a pair of adjacent positive electrode bodies 41. In the illustrated example, it has 7) electrode connection portions 42 and a positive electrode tab 45 extending from the positive electrode body 41.
The positive electrode body 41 is a portion of the electrode laminate 3 that extends flat along a vertical plane in the stacking direction. The electrode connecting portion 42 is a portion that is folded back at the side portion of the laminated electrode body 2 so that the plurality of positive electrode main bodies 41 overlap the negative electrode main body 31. The positive electrode tab 45 is a portion connected to the positive electrode plate 26 described above. A positive electrode active material layer coated with the positive electrode active material is formed on the entire surface of each of the positive electrode main body 41 and the electrode connecting portion 42. A positive electrode current collector is exposed on the surface of the tip of the positive electrode tab 45.

以下、複数の正極本体41が並ぶ方向を正極連結方向(第2方向)と称し、正極連結方向に直交する方向を正極幅方向と称する。また、正極連結方向において、複数の正極本体41のうち積層電極体の最も巻回中心側に配置される正極本体41に対し、電極積層体3の外周側に配置される正極本体41側を「外周側」と定義し、その反対方向を「内周側」と定義する。また、以下では、複数の正極本体41および複数の電極接続部42について、負極本体31および電極接続部32と同様に序数を付して説明する。 Hereinafter, the direction in which the plurality of positive electrode bodies 41 are lined up is referred to as the positive electrode connecting direction (second direction), and the direction orthogonal to the positive electrode connecting direction is referred to as the positive electrode width direction. Further, in the positive electrode connecting direction, the positive electrode main body 41 arranged on the outer peripheral side of the electrode laminated body 3 is "" with respect to the positive electrode main body 41 arranged on the most winding center side of the laminated electrode body among the plurality of positive electrode main bodies 41. It is defined as "outer circumference side", and the opposite direction is defined as "inner circumference side". Further, in the following, the plurality of positive electrode main bodies 41 and the plurality of electrode connecting portions 42 will be described with ordinal numbers in the same manner as the negative electrode main body 31 and the electrode connecting portions 32.

複数の正極本体41は、負極本体31と同数設けられている。複数の正極本体41は、正極連結方向から見て正極幅方向の中心が互いに重なるように配置されている。複数の正極本体41のうち最内周に配置される第1正極本体41Aを除く正極本体41は、電極積層体3においてセパレータ層36、46を介して対向する負極本体31の外形よりも小さく形成されている。例えば、第7正極本体41Gの外形は、セパレータ層36、46を介して対向する第8負極本体31Hおよび第6負極本体31Fの外形よりも小さい。第8正極本体41Hの外形は、正極側セパレータ層46を介して対向する第7負極本体31Gの外形よりも小さい。 The plurality of positive electrode main bodies 41 are provided in the same number as the negative electrode main bodies 31. The plurality of positive electrode bodies 41 are arranged so that the centers in the positive electrode width direction are overlapped with each other when viewed from the positive electrode connecting direction. The positive electrode main body 41 other than the first positive electrode main body 41A arranged on the innermost circumference of the plurality of positive electrode main bodies 41 is formed smaller than the outer shape of the negative electrode main body 31 facing each other via the separator layers 36 and 46 in the electrode laminate 3. Has been done. For example, the outer shape of the seventh positive electrode body 41G is smaller than the outer shape of the eighth negative electrode body 31H and the sixth negative electrode body 31F facing each other via the separator layers 36 and 46. The outer shape of the eighth positive electrode body 41H is smaller than the outer shape of the seventh negative electrode body 31G facing each other via the positive electrode side separator layer 46.

図3、図4に示すように、複数の電極接続部42は、正極連結方向で隣り合う一対の正極本体41の間に設けられている。各電極接続部42は、正極連結方向の中間部が最も幅狭になるように形成されている。 As shown in FIGS. 3 and 4, the plurality of electrode connecting portions 42 are provided between a pair of positive electrode main bodies 41 adjacent to each other in the positive electrode connecting direction. Each electrode connecting portion 42 is formed so that the intermediate portion in the positive electrode connecting direction is the narrowest.

正極タブ45は、第8正極本体41Hから第1正極本体41Aとは反対側に延出している。正極タブ45は、複数の電極接続部42よりも狭い幅で正極連結方向に延びている。
以上構成の正極体40において、正極タブ45の先端側を除く部分の全体が正極側セパレータ層46で覆われている(図3参照)。すなわち、正極本体41の表裏面に加えて周面(側面)と電極接続部42の表裏面に加えて側面が正極側セパレータ層46により覆われている。
The positive electrode tab 45 extends from the eighth positive electrode main body 41H to the side opposite to the first positive electrode main body 41A. The positive electrode tab 45 extends in the positive electrode connecting direction with a width narrower than that of the plurality of electrode connecting portions 42.
In the positive electrode body 40 having the above configuration, the entire portion except the tip end side of the positive electrode tab 45 is covered with the positive electrode side separator layer 46 (see FIG. 3). That is, in addition to the front and back surfaces of the positive electrode body 41, the peripheral surface (side surface) and the front and back surfaces of the electrode connecting portion 42 and the side surface are covered with the positive electrode side separator layer 46.

先に説明したように正極側セパレータ層46は塗膜を硬化させて形成したものである。図4に示す正極体40に対し、正極タブ先端側を除く部分の表裏面に塗料を塗布すると、正極体40の周面側(周端面側)にも塗料の回り込みを生じさせることができるので、正極タブ45の先端部分を除いて正極体40のほぼ全体を覆う負極側セパレータ層46を形成できる。
塗料については塗膜形成後、熱により硬化する塗料を用いた場合は硬化温度まで加熱し、紫外線等の光照射により硬化する塗料を用いた場合は硬化のために必要な波長の光を必要な強度で照射し、乾燥により硬化する塗料の場合は適切な温度で乾燥することにより、塗料を硬化できる。塗料の硬化により、図3に示すようにセパレータ層46で覆った構造の正極体40を得ることができる。
As described above, the positive electrode side separator layer 46 is formed by curing the coating film. When the paint is applied to the front and back surfaces of the positive electrode body 40 shown in FIG. 4 except for the tip end side of the positive electrode tab, the paint can wrap around on the peripheral surface side (peripheral end surface side) of the positive electrode body 40. The negative electrode side separator layer 46 can be formed so as to cover almost the entire positive electrode body 40 except for the tip portion of the positive electrode tab 45.
For paint, after forming the coating film, if a paint that cures by heat is used, it is heated to the curing temperature, and if a paint that cures by irradiation with light such as ultraviolet rays is used, light of the wavelength required for curing is required. In the case of a paint that is irradiated with intensity and cured by drying, the paint can be cured by drying at an appropriate temperature. By curing the paint, a positive electrode body 40 having a structure covered with a separator layer 46 can be obtained as shown in FIG.

次に、負極体30および正極体40の巻回構造について説明する。
負極体30と正極体40を巻回する場合、最初に、負極体30の第1負極本体31Aと正極体40の第1正極本体41Aとを互いに重ねる。この際、負極体30と正極体40を互いに一直線状になるように、接続タブ35、45が互いに反対方向を向くように配置する。この状態から順次負極体30と正極体40を同じ方向に順次渦巻き状に巻回することで図2に示す電極積層体3を形成できる。
Next, the winding structure of the negative electrode body 30 and the positive electrode body 40 will be described.
When winding the negative electrode body 30 and the positive electrode body 40, first, the first negative electrode body 31A of the negative electrode body 30 and the first positive electrode body 41A of the positive electrode body 40 are overlapped with each other. At this time, the connection tabs 35 and 45 are arranged so as to face each other so that the negative electrode body 30 and the positive electrode body 40 are in a straight line with each other. From this state, the electrode laminate 3 shown in FIG. 2 can be formed by sequentially winding the negative electrode body 30 and the positive electrode body 40 in the same direction in a spiral shape.

例えば、最初に第1電極接続部32Aを折り曲げて、第1負極本体31Aと第2負極本体31Bとの層間に第1正極本体41Aを挿入して、巻回を開始してもよい。この場合には、第1正極本体41Aの直線部43aを第1電極接続部32Aに突き当てるように、第1負極本体31Aと第2負極本体31Bとの層間に第1正極本体41Aを挿入することができる。
上述のいずれの巻回構造としても、巻回中心軸の方向は図1に示すように電池1を描いた場合、第1底壁部11あるいは第2底壁部21と平行な向きとされている。
For example, the first electrode connecting portion 32A may be first bent, the first positive electrode body 41A may be inserted between the first negative electrode body 31A and the second negative electrode body 31B, and the winding may be started. In this case, the first positive electrode body 41A is inserted between the first negative electrode body 31A and the second negative electrode body 31B so that the straight portion 43a of the first positive electrode body 41A abuts against the first electrode connecting portion 32A. be able to.
In any of the above-mentioned winding structures, the direction of the winding central axis is parallel to the first bottom wall portion 11 or the second bottom wall portion 21 when the battery 1 is drawn as shown in FIG. There is.

また、電極接続部32それぞれの負極連結方向の寸法は、第1負極本体31Aから離れるに従い大きくなっている。
ここで、複数の負極本体31のうち第8負極本体31Hを除き、展開状態で隣り合う一対の負極本体31に着目する。一対の負極本体31の巻回状態における間隔は、一対の負極本体31が外周側に位置する負極本体31の対であるほど、一対の負極本体31の間に配置される負極本体31等の層数が増える分、大きくなる。本実施形態によれば、電極接続部32の第1方向の寸法が第1電極接続部32Aから離れるに従い大きくなることで、一対の負極本体31の間隔を確保でき、一対の負極本体31の巻回状態における互いの位置ずれを抑制できる。よって、積層方向から見て、複数の負極本体31の位置ずれが抑制され、負極体30を所望の扁平形状に巻回できる。
Further, the dimensions of each of the electrode connecting portions 32 in the negative electrode connecting direction increase as the distance from the first negative electrode main body 31A increases.
Here, attention is paid to a pair of negative electrode bodies 31 that are adjacent to each other in the expanded state, except for the eighth negative electrode body 31H among the plurality of negative electrode bodies 31. The distance between the pair of negative electrode bodies 31 in the wound state is such that the pair of negative electrode bodies 31 is paired with the negative electrode bodies 31 located on the outer peripheral side, the layers such as the negative electrode bodies 31 arranged between the pair of negative electrode bodies 31. As the number increases, it becomes larger. According to the present embodiment, the dimension of the electrode connecting portion 32 in the first direction increases as the distance from the first electrode connecting portion 32A increases, so that the distance between the pair of negative electrode main bodies 31 can be secured, and the winding of the pair of negative electrode main bodies 31 can be secured. It is possible to suppress the displacement of each other in the rotating state. Therefore, when viewed from the stacking direction, the positional deviation of the plurality of negative electrode bodies 31 is suppressed, and the negative electrode body 30 can be wound into a desired flat shape.

しかも、少なくとも1つの電極接続部32それぞれの負極連結方向の寸法は、第1電極接続部32Aから離れるに従い大きくなる。この構成によれば、一対の負極本体31のうち外周側の負極本体31は、内周側の負極本体31よりも負極連結方向に大きく形成される。このため、複数の負極本体31が互いに重なった状態で、積層方向から見て、外周側の負極本体31には内周側の負極本体31が重ならない非重畳領域が設けられる。
内周側の負極本体31に接続して積層方向に延びる電極接続部32を、積層方向から見て外周側の負極本体31における非重畳領域に配置することで、積層方向から見て電極接続部32が外周側の負極本体31から突出することを抑制できる。よって、電極積層体3を突出部のない所望の扁平形状に巻回して外装体3内に高密度で配置することが可能となる。
以上により、積層方向から見て、複数の負極本体31の位置ずれ、および電極接続部32の突出が抑制される。したがって、負極体30を所望の扁平形状に巻回でき、形状の自由度の向上、および容量の確保が図られた電池(電気化学セル)1を提供できる。
Moreover, the dimensions of each of the at least one electrode connecting portion 32 in the negative electrode connecting direction increase as the distance from the first electrode connecting portion 32A increases. According to this configuration, the negative electrode main body 31 on the outer peripheral side of the pair of negative electrode main bodies 31 is formed larger in the negative electrode connecting direction than the negative electrode main body 31 on the inner peripheral side. Therefore, in a state where the plurality of negative electrode bodies 31 overlap each other, the negative electrode body 31 on the outer peripheral side is provided with a non-overlapping region in which the negative electrode bodies 31 on the inner peripheral side do not overlap when viewed from the stacking direction.
By arranging the electrode connecting portion 32 connected to the negative electrode body 31 on the inner peripheral side and extending in the stacking direction in the non-superimposed region of the negative electrode body 31 on the outer peripheral side when viewed from the stacking direction, the electrode connecting portion is viewed from the stacking direction. It is possible to prevent the 32 from protruding from the negative electrode body 31 on the outer peripheral side. Therefore, the electrode laminate 3 can be wound into a desired flat shape without protrusions and arranged in the exterior body 3 at a high density.
As described above, the positional deviation of the plurality of negative electrode bodies 31 and the protrusion of the electrode connecting portions 32 are suppressed when viewed from the stacking direction. Therefore, it is possible to provide the battery (electrochemical cell) 1 in which the negative electrode body 30 can be wound into a desired flat shape, the degree of freedom in the shape is improved, and the capacity is secured.

図4に示す帯状の負極体30と正極体40を渦巻き状に巻回して電極積層体3を形成する場合、負極体30または正極体40と同一平面視形状のフィルム状のセパレータを用いて巻回することも考えられる。しかし、フィルム状のセパレータとともに負極体30と正極体40を巻回すると、これらのいずれかに巻ずれが発生することがある。負極体30または正極体40とセパレータのいずれかに巻ずれを生じると、電極積層体の外周部のどこかにおいて電極本体がセパレータの外側に突出した部分を生じ、これが内部ショート発生のリスクを高める。
この点において、塗膜を硬化させて形成したセパレータ層36、46を備えた負極体30、正極体40の巻回構造であるならば、負極体30、正極体40に巻ずれを生じたとしてもセパレータ層36、46が負極体30、正極体40を覆っていることに変わりは無い。このため、負極側セパレータ層36を備えた負極体30と正極側セパレータ層46を備えた正極体40との巻回である限り、内部ショート発生のリスクは生じない。即ち、塗膜硬化層からなるセパレータ層36、46を備えた負極体30、正極体40からなる巻回構造の電極積層体3であるならば、内部ショートのリスクの発生しない電池(電気化学セル)1を提供できる。
When the strip-shaped negative electrode body 30 and the positive electrode body 40 shown in FIG. 4 are spirally wound to form the electrode laminate 3, the negative electrode body 30 or the positive electrode body 40 is wound using a film-shaped separator having the same plan view shape as the negative electrode body 30 or the positive electrode body 40. It is also possible to turn it. However, when the negative electrode body 30 and the positive electrode body 40 are wound together with the film-shaped separator, winding misalignment may occur in any of these. When either the negative electrode body 30 or the positive electrode body 40 and the separator are unwound, a portion where the electrode body protrudes to the outside of the separator is formed somewhere on the outer peripheral portion of the electrode laminate, which increases the risk of internal short circuit. ..
In this respect, if the negative electrode body 30 and the positive electrode body 40 having the separator layers 36 and 46 formed by curing the coating film have a wound structure, it is assumed that the negative electrode body 30 and the positive electrode body 40 are miswound. However, the separator layers 36 and 46 still cover the negative electrode body 30 and the positive electrode body 40. Therefore, as long as the negative electrode body 30 having the negative electrode side separator layer 36 and the positive electrode body 40 having the positive electrode side separator layer 46 are wound, there is no risk of internal short circuit. That is, if the electrode laminate 3 has a wound structure composed of a negative electrode body 30 and a positive electrode body 40 having separator layers 36 and 46 made of a cured coating film, a battery (electrochemical cell) in which the risk of internal short circuit does not occur. ) 1 can be provided.

また、第1実施形態の構造において、電極積層体3を収容している外装体2は、アルミニウム箔などの金属箔の両面を樹脂層で覆ったラミネート構造体からなり、第2周壁部22と折曲部23と接続壁12bを折り曲げつつプレス成形して熱融着し、封止部5を形成している。
この構造であると、第2周壁部22と折曲部23と接続壁12bの内側に位置している樹脂層に欠陥があった場合、プレス加工に伴い樹脂層にピンホールや亀裂あるいは筋などの欠陥部分を生じるおそれがある。
Further, in the structure of the first embodiment, the exterior body 2 accommodating the electrode laminate 3 is composed of a laminate structure in which both sides of a metal foil such as an aluminum foil are covered with a resin layer, and the second peripheral wall portion 22 The bent portion 23 and the connecting wall 12b are press-molded while being bent and heat-sealed to form the sealing portion 5.
With this structure, if there is a defect in the resin layer located inside the second peripheral wall portion 22, the bent portion 23, and the connecting wall 12b, pinholes, cracks, streaks, etc. are formed in the resin layer due to press working. May cause defective parts.

これら欠陥部分を生じていると、収容部4に充填されている電解液が外装体2内のアルミニウム箔に接触するおそれがある。ここで、例えば負極体30の一部が電極積層体3の外周部に露出する部分があり、この部分が外装体2内のアルミニウム箔に近接するか接触して負極電位がアルミニウム箔に印加された場合、金属リチウムとアルミニウムとの接触に伴うアルミニウム箔の負極劣化が進行するおそれがある。しかし、第1実施形態の電極積層体3であるならば、セパレータ層36、46が確実に負極体30、正極体40を覆うので、外装体2の内面側に欠陥部分を生じてアルミニウム箔が露出していたとしても、アルミニウム箔の劣化を進行させることがない。また、セパレータ層36、46が確実に負極体30、正極体40を覆うので、内部ショート発生のリスクを低減した電池(電気化学セル)1を提供できる。 If these defective portions are generated, the electrolytic solution filled in the accommodating portion 4 may come into contact with the aluminum foil in the exterior body 2. Here, for example, there is a portion where a part of the negative electrode body 30 is exposed on the outer peripheral portion of the electrode laminate 3, and the negative electrode potential is applied to the aluminum foil when this portion is close to or in contact with the aluminum foil in the exterior body 2. In that case, the negative electrode deterioration of the aluminum foil due to the contact between the metallic lithium and the aluminum may progress. However, in the case of the electrode laminate 3 of the first embodiment, since the separator layers 36 and 46 surely cover the negative electrode body 30 and the positive electrode body 40, a defective portion is generated on the inner surface side of the exterior body 2 and the aluminum foil is formed. Even if it is exposed, the deterioration of the aluminum foil does not proceed. Further, since the separator layers 36 and 46 surely cover the negative electrode body 30 and the positive electrode body 40, the battery (electrochemical cell) 1 with reduced risk of internal short circuit can be provided.

なお、本実施形態では、負極体30と正極体40を巻回して電極積層体3を製造するに際し、塗料を硬化させた後のセパレータ層36、46を備えた負極体30、正極体40を巻回した。
これに対し、セパレータ層36、46を形成するために塗布した塗膜を完全に硬化させるのではなく、半硬化状態とした段階で負極体30と正極体40を巻回して電極積層体3を構成し、その後必要な硬化条件でセパレータ層36、46を完全硬化させても良い。
In the present embodiment, when the negative electrode body 30 and the positive electrode body 40 are wound around the electrode laminated body 3, the negative electrode body 30 and the positive electrode body 40 provided with the separator layers 36 and 46 after the paint is cured are used. I wound it.
On the other hand, the coating film applied to form the separator layers 36 and 46 is not completely cured, but the negative electrode body 30 and the positive electrode body 40 are wound around the electrode laminate 3 at the stage of being in a semi-cured state. After that, the separator layers 36 and 46 may be completely cured under the required curing conditions.

半硬化状態のセパレータ層36、46を備えた負極体30と正極体40を巻回すると、巻回時に負極体30の周囲に存在する半硬化状態の塗料と正極体40の周囲に存在する半硬化状態の塗料の接触部分どうしを密着させて互いに融合した一体化状態とすることができる。
この融合一体化した状態から、セパレータ層36、46を完全に硬化する条件で加熱処理などを施すと、負極体30のセパレータ層36と正極体40のセパレータ層46を融合一体化させた状態のまま硬化させた電極積層体3を得ることができる。
この構造の電極積層体3であれば、負極体30と正極体40の周囲をより完全にセパレータ層36、46で覆った構造の電極積層体3を得ることができる。
When the negative electrode body 30 and the positive electrode body 40 having the separator layers 36 and 46 in the semi-cured state are wound, the semi-cured paint existing around the negative electrode body 30 and the half existing around the positive electrode body 40 at the time of winding are wound. The contact portions of the cured paint can be brought into close contact with each other to form an integrated state in which they are fused with each other.
When heat treatment or the like is performed under the condition that the separator layers 36 and 46 are completely cured from this fused and integrated state, the separator layer 36 of the negative electrode body 30 and the separator layer 46 of the positive electrode body 40 are fused and integrated. The electrode laminate 3 cured as it is can be obtained.
With the electrode laminate 3 having this structure, it is possible to obtain the electrode laminate 3 having a structure in which the negative electrode body 30 and the positive electrode body 40 are more completely covered with the separator layers 36 and 46.

図1に示す外装体2を構成する場合、1つの例として、第1容器10において第1周壁部12の上部側にプレス加工により折曲部23を形成する以前の状態は折曲部23をリング板状のフランジ部としておく。また、第2容器20において第2底壁部21の外周側にプレス加工により第2周壁部22と折曲部23を形成する以前の状態ではこれらをリング板状のフランジ部としておく。
第2容器20の内部に前述の電極積層体3を電解液とともに収容し、第2容器のフランジ部の上に第1容器10のフランジ部を重ねた後、2つのフランジ部に対しリング状の突部を有するパンチでもってプレス加工することにより第2周壁部22と折曲部23と接続壁12bを図1に示す形状に加工することで図1に示す構造を得ることができる。なお、このフランジ部をプレス加工する技術の詳細については、特開2018−85214号公報(特許第6284248号公報)に記載されている。
When the exterior body 2 shown in FIG. 1 is configured, as an example, the bent portion 23 is formed in the first container 10 before the bent portion 23 is formed on the upper side of the first peripheral wall portion 12 by press working. It is a ring plate-shaped flange. Further, in the state before forming the second peripheral wall portion 22 and the bent portion 23 by press working on the outer peripheral side of the second bottom wall portion 21 in the second container 20, these are set as ring plate-shaped flange portions.
The above-mentioned electrode laminate 3 is housed inside the second container 20 together with the electrolytic solution, and after the flange portion of the first container 10 is placed on the flange portion of the second container, a ring shape is formed with respect to the two flange portions. The structure shown in FIG. 1 can be obtained by processing the second peripheral wall portion 22, the bent portion 23, and the connecting wall 12b into the shape shown in FIG. 1 by press working with a punch having a protrusion. Details of the technique for pressing the flange portion are described in JP-A-2018-852214 (Patent No. 6284248).

第1容器10と第2容器20を前述のラミネート構造体から構成した場合、フランジ部をプレス加工して第1容器10と第2容器20を成形した状態において、外装体2は形が固定された状態ではなく、内部に封入した電極積層体3が多少膨らんだ状態である場合などはそれに応じて外装体2も多少膨らんだ状態となっている。
この状態を回避するためには、前述のプレス加工時、あるいは、プレス加工後に別途成形用のプレスを行った状態において、セパレータ層36、46を構成する塗膜が完全硬化する温度に加熱して所定時間保持する加熱処理を行う。この加熱処理により、セパレータ層36、46を構成する塗膜を完全に硬化できるので、図1に示す形の整った電池1を得ることができる。
When the first container 10 and the second container 20 are composed of the above-mentioned laminated structure, the shape of the exterior body 2 is fixed in a state where the flange portion is pressed to form the first container 10 and the second container 20. When the electrode laminate 3 enclosed inside is in a slightly inflated state instead of in a state of being slightly inflated, the exterior body 2 is also in a slightly inflated state accordingly.
In order to avoid this state, the coating films constituting the separator layers 36 and 46 are heated to a temperature at which the coating films constituting the separator layers 36 and 46 are completely cured during the above-mentioned press working or in a state where a separate pressing for molding is performed after the press working. Perform heat treatment to hold for a predetermined time. By this heat treatment, the coating films constituting the separator layers 36 and 46 can be completely cured, so that the well-shaped battery 1 shown in FIG. 1 can be obtained.

外装体2の形を整えた状態から半硬化状態の塗膜を完全硬化させることで、全体として形の整った状態であり、セパレータ層36、46で全体を覆った電極積層体3を備えた電池1を得ることができる。
特に、外装体2が金属箔と樹脂層のラミネート構造体である場合、電極積層体3を収容した状態で外装体2は柔軟性があり、半硬化状態の塗膜の存在も相俟って、全体形状が固まっていないが、外装体2の形を整えるとともに塗膜を完全硬化させることで、電池1として全体形状を形の整った強固な形状に形成できる。
By completely curing the coating film in the semi-cured state from the state in which the shape of the exterior body 2 is adjusted, the overall shape is in a well-formed state, and the electrode laminate 3 covered entirely with the separator layers 36 and 46 is provided. Battery 1 can be obtained.
In particular, when the exterior body 2 is a laminated structure of a metal foil and a resin layer, the exterior body 2 is flexible in a state where the electrode laminate 3 is housed, and the presence of a coating film in a semi-cured state is also present. Although the overall shape is not solidified, the overall shape of the battery 1 can be formed into a well-shaped and strong shape by adjusting the shape of the exterior body 2 and completely curing the coating film.

また、負極体30の周面と正極体40の周面を個別に覆った塗膜硬化層を一体化してなるセパレータ層であるならば、負極体30と正極体40の巻回時に負極体30と正極体40の一部に巻乱れなどを生じていても、負極体30と正極体40は確実にセパレータ層で覆われる。また、負極体30と正極体40を巻回した電極積層体3の外周面も確実にセパレータ層で覆うことができる。この結果、内部ショートのおそれを生じない電気化学セルを提供できる。 Further, if the separator layer is formed by integrating the coating film curing layer that individually covers the peripheral surface of the negative electrode body 30 and the peripheral surface of the positive electrode body 40, the negative electrode body 30 is wound when the negative electrode body 30 and the positive electrode body 40 are wound. Even if a part of the positive electrode body 40 is disturbed, the negative electrode body 30 and the positive electrode body 40 are surely covered with the separator layer. Further, the outer peripheral surface of the electrode laminate 3 around which the negative electrode body 30 and the positive electrode body 40 are wound can be reliably covered with the separator layer. As a result, it is possible to provide an electrochemical cell that does not cause an internal short circuit.

「第2実施形態」
図5は本発明に係る電気化学セルを二次電池に適用した第2実施形態の電池50の断面構造を示すもので、この電池50は、平面視円形状のボタン形の電池である。この第2実施形態の電池50は、容器状の外装体2と外装体2の内部に収容された電極積層体53を備えている。
第2実施形態に用いられている外装体2は、先の第1実施形態において採用されていた外装体2と同等構成である。このため、外装体2の構成について、第1実施形態と同等の構成には同一の符号を付し、同一構成の詳細説明は省略する。
第2実施形態の外装体2において、第1容器10と第2容器20がラミネート構造体からなり、収容部4を有し、封止部5において第1容器10と第2容器20が接合されている構造は同等である。また、接合部5に第2周壁部22と折曲部23と接続壁12bが形成され、折曲部23と接続壁12bがプレス加工により熱融着された構造も同等である。
"Second embodiment"
FIG. 5 shows a cross-sectional structure of the battery 50 of the second embodiment in which the electrochemical cell according to the present invention is applied to a secondary battery, and the battery 50 is a button-shaped battery having a circular shape in a plan view. The battery 50 of the second embodiment includes a container-shaped exterior body 2 and an electrode laminate 53 housed inside the exterior body 2.
The exterior body 2 used in the second embodiment has the same configuration as the exterior body 2 used in the first embodiment. Therefore, regarding the configuration of the exterior body 2, the same reference numerals are given to the configurations equivalent to those of the first embodiment, and detailed description of the same configuration will be omitted.
In the exterior body 2 of the second embodiment, the first container 10 and the second container 20 are made of a laminated structure, have an accommodating portion 4, and the first container 10 and the second container 20 are joined at the sealing portion 5. The structures are equivalent. Further, the structure in which the second peripheral wall portion 22, the bent portion 23, and the connecting wall 12b are formed at the joint portion 5 and the bent portion 23 and the connecting wall 12b are heat-sealed by press working is also the same.

第2実施形態の電池50にあっては、電極積層体53の構造が第1実施形態の電極積層体3と異なっている。
第2実施形態において電極積層体53は、図6(A)に示す負極体55に塗膜硬化層からなる図6(B)に示す負極側セパレータ層56を形成したものと、図6(C)に示す正極体57に図6(D)に示す正極側セパレータ層58を形成したものを渦巻き状に巻回した構造を有する。
負極体55は、先の第1実施形態で用いた負極体30と平面視形状は異なるが、積層構造は同等であり、正極体57は先の第1実施形態で用いた正極体40と平面視形状は異なるが、積層構造は同等である。
In the battery 50 of the second embodiment, the structure of the electrode laminate 53 is different from that of the electrode laminate 3 of the first embodiment.
In the second embodiment, the electrode laminate 53 has a negative electrode body 55 shown in FIG. 6 (A) formed of a coating film cured layer and a negative electrode side separator layer 56 shown in FIG. 6 (B), and FIG. 6 (C). ) Is formed with the positive electrode side separator layer 58 shown in FIG. 6 (D) and wound in a spiral shape.
The negative electrode body 55 has a different plan view shape from the negative electrode body 30 used in the first embodiment, but has the same laminated structure, and the positive electrode body 57 is flat with the positive electrode body 40 used in the first embodiment. The visual shape is different, but the laminated structure is the same.

負極体55は、銅などの金属箔からなる帯状の負極集電体の片面または表裏面に負極活物質を塗布した負極活物質層を備えている。正極体57は、アルミニウムなどの金属箔からなる帯状の正極集電体の片面または表裏面に正極活物質を塗布した正極活物質層を備えている。負極集電体と正極集電体を構成する金属材料と、正極活物質層と負極活物質層を構成する材料は先の第1実施形態において説明したものを用いることができる。
帯状の負極集電体の両面に負極活物質層を形成し、それらを覆うセパレータ層56を形成するには、先の第1実施形態においてセパレータ層36、46の形成用に用いたものと同等の塗料を用いることができる。
負極集電体と負極活物質層を覆うように塗料を塗布する場合、負極集電体の長さ方向一端側に未塗工部を設けて負極集電体の端部を露出させておき、この露出部分を接続タブ55aとすることができる。正極集電体と正極活物質層を覆うように塗料を塗布する場合、正極集電体の長さ方向一端側に未塗工部を設けて正極集電体の端部を露出させておき、この露出部分を接続タブ57aとすることができる。
The negative electrode body 55 includes a negative electrode active material layer in which a negative electrode active material is applied to one side or the front and back surfaces of a band-shaped negative electrode current collector made of a metal foil such as copper. The positive electrode body 57 includes a positive electrode active material layer in which a positive electrode active material is applied to one side or the front and back surfaces of a band-shaped positive electrode current collector made of a metal foil such as aluminum. As the metal material constituting the negative electrode current collector and the positive electrode current collector and the material constituting the positive electrode active material layer and the negative electrode active material layer, those described in the first embodiment can be used.
In order to form the negative electrode active material layers on both sides of the strip-shaped negative electrode current collector and to form the separator layer 56 covering them, it is equivalent to the one used for forming the separator layers 36 and 46 in the first embodiment. Paint can be used.
When the paint is applied so as to cover the negative electrode current collector and the negative electrode active material layer, an uncoated portion is provided on one end side in the length direction of the negative electrode current collector to expose the end portion of the negative electrode current collector. This exposed portion can be a connection tab 55a. When the paint is applied so as to cover the positive electrode current collector and the positive electrode active material layer, an uncoated portion is provided on one end side in the length direction of the positive electrode current collector to expose the end portion of the positive electrode current collector. This exposed portion can be a connection tab 57a.

セパレータ層形成用の塗料を塗布後、第1実施形態において説明したように塗膜の硬化条件あるいは半硬化条件となるように熱処理などを施し、負極体56、正極体57を形成し、それらを用いて円環状に巻回することで図6(F)に示す電極積層体59を得ることができる。
積層体59を得たならば、これをプレス加工による融着前の第1容器10と第2容器20からなる収容部4に電解液とともに収容し、プレス加工により第2周壁部22、折曲部23、接続壁12bを形成し、折曲部23の外面側の樹脂層と接続壁12bの内周側の樹脂層を熱融着することにより図5に示す構造の電池50を得ることができる。
After applying the paint for forming the separator layer, heat treatment or the like is performed so as to satisfy the curing condition or the semi-curing condition of the coating film as described in the first embodiment to form the negative electrode body 56 and the positive electrode body 57, and these are formed. The electrode laminate 59 shown in FIG. 6 (F) can be obtained by winding it in an annular shape.
When the laminate 59 is obtained, it is stored together with the electrolytic solution in the accommodating portion 4 composed of the first container 10 and the second container 20 before fusion by press working, and the second peripheral wall portion 22 is bent by press working. The battery 50 having the structure shown in FIG. 5 can be obtained by forming the portion 23 and the connecting wall 12b and heat-sealing the resin layer on the outer surface side of the bent portion 23 and the resin layer on the inner peripheral side of the connecting wall 12b. it can.

図5に示す電池50にあっても、第1実施形態の電池1と同様に、塗膜を硬化させたセパレータ層56、58を備えた負極体55、正極体57の巻回構造であるならば、負極体55、正極体57に巻ずれを生じたとしてもセパレータ層56、58が負極体55、正極体57を覆っていることに変わりは無い。このため、負極側セパレータ層56を備えた負極体55と正極側セパレータ層58を備えた正極体57との巻回である限り、内部ショート発生のリスクは生じない。即ち、塗膜硬化層からなるセパレータ層56、58を備えた負極体55、正極体57からなる巻回構造の電極積層体59であるならば、内部ショートリスクの発生しない電池(電気化学セル)50を提供できる。 The battery 50 shown in FIG. 5 also has a wound structure of the negative electrode body 55 and the positive electrode body 57 provided with the separator layers 56 and 58 having the cured coating film, as in the battery 1 of the first embodiment. For example, even if the negative electrode body 55 and the positive electrode body 57 are miswound, the separator layers 56 and 58 still cover the negative electrode body 55 and the positive electrode body 57. Therefore, as long as the negative electrode body 55 having the negative electrode side separator layer 56 and the positive electrode body 57 having the positive electrode side separator layer 58 are wound, there is no risk of internal short circuit. That is, if the electrode laminate 59 has a wound structure composed of a negative electrode body 55 and a positive electrode body 57 having separator layers 56 and 58 made of a cured coating film, a battery (electrochemical cell) in which an internal short-circuit risk does not occur. 50 can be provided.

また、図5に示す電池50において、半硬化状態の塗膜を備えた電極積層体53を外装体2に収容し、プレス加工による融着後に加熱処理を行ってセパレータ層56、58を完全硬化させても良い。この場合、先に示した第1実施形態において半硬化状態の塗膜を用いた場合と同様の作用効果を得ることができる。
以上説明した第2実施形態では、上述のいずれの巻回構造としても、負極体55と正極体57の巻回中心軸の方向は図5に示すように電池50を描いた場合、第1底壁部11あるいは第2底壁部21と垂直な向きとされる。
Further, in the battery 50 shown in FIG. 5, an electrode laminate 53 having a semi-cured coating film is housed in the exterior body 2, and heat treatment is performed after fusion by press working to completely cure the separator layers 56 and 58. You may let me. In this case, the same effect as when the semi-cured coating film is used in the first embodiment shown above can be obtained.
In the second embodiment described above, in any of the above-described winding structures, the direction of the winding central axis of the negative electrode body 55 and the positive electrode body 57 is the first bottom when the battery 50 is drawn as shown in FIG. The orientation is perpendicular to the wall portion 11 or the second bottom wall portion 21.

「第3実施形態」
図7、図8は本発明に係る電気化学セルを二次電池に適用した第3実施形態の電池60の断面構造を示すもので、この電池60は円形のボタン型電池である。この第3実施形態の電池60は、偏平な容器状の外装体62と外装体62の内部に図示略の電解液とともに収容された電極積層体63を備えている。なお、電解液は支持塩を非水溶媒に溶解した電解液などが好適に用いられる。
"Third embodiment"
7 and 8 show a cross-sectional structure of the battery 60 of the third embodiment in which the electrochemical cell according to the present invention is applied to a secondary battery, and the battery 60 is a circular button type battery. The battery 60 of the third embodiment includes a flat container-shaped exterior body 62 and an electrode laminate 63 housed inside the exterior body 62 together with an electrolytic solution (not shown). As the electrolytic solution, an electrolytic solution in which a supporting salt is dissolved in a non-aqueous solvent is preferably used.

外装体62は、平面視で円形状を呈している。具体的に、外装体62は、有底筒状の正極側容器65と、この正極側容器65にガスケット66を介し組み付けられ、正極側容器65との間に収納空間Sを画成する有頂筒型の負極側容器67を有している。
図7、図8に示す第3実施形態において、正極側容器65および負極側容器67のそれぞれの中心軸線が共通軸上に配置されている。以下、この共通軸を軸線Oと称し、軸線O方向に沿う負極側容器67側を上側と称し、正極側容器65側を下側と称し、軸線O方向から見た平面視で軸線Oに直交する方向を径方向と称し、軸線O回りに周回する方向を周方向と称する。
The exterior body 62 has a circular shape in a plan view. Specifically, the exterior body 62 is assembled to the bottomed tubular positive electrode side container 65 via a gasket 66, and forms a storage space S between the positive electrode side container 65 and the positive electrode side container 65. It has a tubular negative electrode side container 67.
In the third embodiment shown in FIGS. 7 and 8, the central axes of the positive electrode side container 65 and the negative electrode side container 67 are arranged on a common axis. Hereinafter, this common axis is referred to as the axis O, the negative electrode side container 67 side along the axis O direction is referred to as the upper side, the positive electrode side container 65 side is referred to as the lower side, and is orthogonal to the axis O in a plan view from the axis O direction. The direction of rotation is referred to as the radial direction, and the direction of orbiting around the axis O is referred to as the circumferential direction.

正極側容器65および負極側容器67は、例えばステンレス鋼板等の金属板材を絞り加工等して形成されている。図示の例において、正極側容器65の内径は、負極側容器67の外径よりも大きくされている。
ガスケット66は、軸線Oと同軸状に配置された環状とされ、正極側容器65の周壁部65a内に嵌合されている。ガスケット66には、負極側容器67の周壁部67aを保持する溝部69が全周に渡り形成されている。負極側容器67は、周壁部67aをガスケット66の溝部69内に保持した状態で、正極側容器65の周壁部65aの上端側を径方向の内側にカシメることで正極側容器65に固定される。
ガスケット66は、樹脂材料(例えば、ポリプロピレン(PP)、ポリフェニレンサルファイド(PPS)、ポリエーテルエーテルケトン(PEEK))等の絶縁性を有する材料により形成されている。
The positive electrode side container 65 and the negative electrode side container 67 are formed by drawing, for example, a metal plate material such as a stainless steel plate. In the illustrated example, the inner diameter of the positive electrode side container 65 is larger than the outer diameter of the negative electrode side container 67.
The gasket 66 has an annular shape arranged coaxially with the axis O, and is fitted in the peripheral wall portion 65a of the positive electrode side container 65. The gasket 66 is formed with a groove portion 69 that holds the peripheral wall portion 67a of the negative electrode side container 67 over the entire circumference. The negative electrode side container 67 is fixed to the positive electrode side container 65 by caulking the upper end side of the peripheral wall portion 65a of the positive electrode side container 65 inward in the radial direction while the peripheral wall portion 67a is held in the groove portion 69 of the gasket 66. To.
The gasket 66 is formed of an insulating material such as a resin material (for example, polypropylene (PP), polyphenylene sulfide (PPS), polyetheretherketone (PEEK)).

電極積層体63は以下に説明する円板状の負極体70と正極体71を複数枚積層した構造を有する。
負極体70は、円板状の負極集電体72とその上面に塗布された負極活物質層73を有し、負極活物質層73が塗布硬化層からなる負極側セパレータ層75によって覆われている。
正極体71は、円板状の正極集電体76とその上面に塗布された正極活物質層77を有し、正極活物質層77が塗布硬化層からなる正極側セパレータ層78によって覆われている。
The electrode laminated body 63 has a structure in which a plurality of disc-shaped negative electrode bodies 70 and positive electrode bodies 71 described below are laminated.
The negative electrode body 70 has a disc-shaped negative electrode current collector 72 and a negative electrode active material layer 73 coated on the upper surface thereof, and the negative electrode active material layer 73 is covered with a negative electrode side separator layer 75 made of a coated cured layer. There is.
The positive electrode body 71 has a disk-shaped positive electrode current collector 76 and a positive electrode active material layer 77 coated on the upper surface thereof, and the positive electrode active material layer 77 is covered with a positive electrode side separator layer 78 made of a coated cured layer. There is.

負極集電体72は第1実施形態の電池1において負極体30の負極集電体を構成した材料と同等材料、例えば銅箔からなり、正極集電体72は第1実施形態の電池1において正極体40の正極集電体を構成した材料と同等材料、例えばアルミニウム箔からなる。
負極活物質層73は第1実施形態の電池1において負極体30の負極活物質層を構成した材料と同等材料からなり、正極活物質層77は第1実施形態の電池1において正極体40の正極活物質層を構成した材料と同等材料からなる。
The negative electrode current collector 72 is made of a material equivalent to the material constituting the negative electrode current collector of the negative electrode body 30 in the battery 1 of the first embodiment, for example, copper foil, and the positive electrode current collector 72 is the battery 1 of the first embodiment. It is made of a material equivalent to the material constituting the positive electrode current collector of the positive electrode body 40, for example, an aluminum foil.
The negative electrode active material layer 73 is made of the same material as the material constituting the negative electrode active material layer of the negative electrode body 30 in the battery 1 of the first embodiment, and the positive electrode active material layer 77 is made of the positive electrode body 40 in the battery 1 of the first embodiment. It is made of the same material as the material constituting the positive electrode active material layer.

負極側セパレータ層75と正極側セパレータ層78を構成する材料は第1実施形態の電池1において、負極側セパレータ層50、正極側セパレータ層60を形成した材料と同等材料からなる。
第3実施形態の電極積層体63は、負極活物質層73を負極側セパレータ層75により覆った構造の複数の負極体70と、正極活物質層77を正極側セパレータ層78で覆った構造の複数の正極体71を交互にそれらの厚さ方向に積層してなる。
電極積層体63において、各負極体70の外周部には負極集電体72の外周部が配置され、各正極体71の外周部には正極集電体76の外周部が配置されている。正極活物質層77の外径は、負極活物質層73の外径より小さく形成されている。
The material constituting the negative electrode side separator layer 75 and the positive electrode side separator layer 78 is made of the same material as the material forming the negative electrode side separator layer 50 and the positive electrode side separator layer 60 in the battery 1 of the first embodiment.
The electrode laminate 63 of the third embodiment has a structure in which a plurality of negative electrode bodies 70 having a structure in which the negative electrode active material layer 73 is covered with a negative electrode side separator layer 75 and a structure in which the positive electrode active material layer 77 is covered with a positive electrode side separator layer 78. A plurality of positive electrode bodies 71 are alternately laminated in the thickness direction thereof.
In the electrode laminate 63, the outer peripheral portion of the negative electrode current collector 72 is arranged on the outer peripheral portion of each negative electrode body 70, and the outer peripheral portion of the positive electrode current collector 76 is arranged on the outer peripheral portion of each positive electrode body 71. The outer diameter of the positive electrode active material layer 77 is formed to be smaller than the outer diameter of the negative electrode active material layer 73.

なお、図7、図8では記載を略したが、外装体62の内部には電極積層体63に設けられている全ての負極集電体72に接続されて負極側容器67に導通した接続導体が設けられ、電極積層体63に設けられている全ての正極集電体76に接続されて正極側容器63に導通した接続導体が設けられている。 Although the description is omitted in FIGS. 7 and 8, a connecting conductor inside the exterior body 62 is connected to all the negative electrode current collectors 72 provided in the electrode laminate 63 and conducted to the negative electrode side container 67. Is provided, and a connecting conductor that is connected to all the positive electrode current collectors 76 provided in the electrode laminate 63 and conducts to the positive electrode side container 63 is provided.

以上説明の電池60は、負極活物質層73を負極側セパレータ層75により覆い、正極活物質層77を正極側セパレータ層78で覆った構造である。このため、負極側セパレータ層75と正極側セパレータ層78による絶縁分離が十分になされた構造を提供できる。
塗膜硬化型の負極側セパレータ層75と正極側セパレータ層78を用いることで、必要な位置にセパレータ層75、78を配することができ、内部ショートリスクが発生し難い構造を提供できる。
The battery 60 described above has a structure in which the negative electrode active material layer 73 is covered with the negative electrode side separator layer 75, and the positive electrode active material layer 77 is covered with the positive electrode side separator layer 78. Therefore, it is possible to provide a structure in which the negative electrode side separator layer 75 and the positive electrode side separator layer 78 are sufficiently insulated and separated.
By using the coating film curing type negative electrode side separator layer 75 and positive electrode side separator layer 78, the separator layers 75 and 78 can be arranged at necessary positions, and a structure in which the risk of internal short circuit is unlikely to occur can be provided.

1…電池(電気化学セル)、2…外装体、3…電極積層体、4…収容部、5…封止部、10…第1容器(外側容器)、11…第1底壁部、12…第1周壁部、12b…接続壁、15…負極プレート、20…第2容器(内側容器)、21…第2底壁部、22…第2周壁部、23…折曲部、30…負極体、31…電極本体、32…電極接続部、35…接続タブ、36…負極側セパレータ層、40…正極体、41…電極本体、42…電極接続部、45…接続タブ、46…正極側セパレータ層、50…電池(電気化学セル)、55…負極体、56…負極側セパレータ層、57…正極体、58…正極側セパレータ層、59…電極積層体、60…電池(電気化学セル)、62…外装体、63…電極積層体、65…正極側容器、66…ガスケット、67…負極側容器、70…負極体、71…正極体、72…負極集電体、73…負極活物質層、75…負極側セパレータ層、76…正極集電体、77…正極活物質層、78…正極側セパレータ層。 1 ... Battery (electrochemical cell), 2 ... Exterior body, 3 ... Electrode laminate, 4 ... Storage part, 5 ... Sealing part, 10 ... First container (outer container), 11 ... First bottom wall part, 12 ... 1st peripheral wall part, 12b ... connection wall, 15 ... negative electrode plate, 20 ... second container (inner container), 21 ... second bottom wall part, 22 ... second peripheral wall part, 23 ... bent part, 30 ... negative electrode Body, 31 ... Electrode body, 32 ... Electrode connection, 35 ... Connection tab, 36 ... Negative electrode side separator layer, 40 ... Positive electrode body, 41 ... Electrode body, 42 ... Electrode connection, 45 ... Connection tab, 46 ... Positive electrode side Separator layer, 50 ... Battery (electrochemical cell), 55 ... Negative electrode body, 56 ... Negative electrode side separator layer, 57 ... Positive electrode body, 58 ... Positive electrode side separator layer, 59 ... Electrode laminate, 60 ... Battery (electrochemical cell) , 62 ... exterior body, 63 ... electrode laminate, 65 ... positive electrode side container, 66 ... gasket, 67 ... negative electrode side container, 70 ... negative electrode body, 71 ... positive electrode body, 72 ... negative electrode current collector, 73 ... negative electrode active material Layers, 75 ... Negative electrode side separator layer, 76 ... Positive electrode current collector, 77 ... Positive electrode active material layer, 78 ... Positive electrode side separator layer.

Claims (9)

帯状の正極体と帯状の負極体の少なくとも一方において少なくとも一方の面を被覆した塗膜硬化層からなるセパレータ層を介し、前記正極体と前記負極体を任意の巻き中心軸を周回するように巻回してなる電極積層体を備え、
外周壁を有する内側容器と外周壁を有する外側容器からなり、前記内側容器の外周壁と前記外側容器の外周壁を重ね合わせて折り曲げ融着一体化した外装体に、前記電極積層体が収容されたことを特徴とする電気化学セル。
The positive electrode body and the negative electrode body are wound around an arbitrary winding central axis via a separator layer composed of a coating film curing layer covering at least one surface of at least one of the band-shaped positive electrode body and the band-shaped negative electrode body. Equipped with a rotating electrode laminate
The electrode laminate is housed in an outer body composed of an inner container having an outer peripheral wall and an outer container having an outer peripheral wall, and the outer peripheral wall of the inner container and the outer peripheral wall of the outer container are overlapped and bent and fused and integrated. An electrochemical cell characterized by that.
帯状の正極体と帯状の負極体の少なくとも一方において少なくとも一方の面を被覆した塗膜硬化層からなるセパレータ層を介し、前記正極体と前記負極体を任意の巻き中心軸を周回するように巻回してなる電極積層体を備え、
正極缶と負極缶をガスケットを介し一体化した外装体に、前記電極積層体が収容されたことを特徴とする電気化学セル。
The positive electrode body and the negative electrode body are wound around an arbitrary winding central axis via a separator layer composed of a coating film curing layer covering at least one surface of at least one of the band-shaped positive electrode body and the band-shaped negative electrode body. Equipped with a rotating electrode laminate
An electrochemical cell characterized in that the electrode laminate is housed in an exterior body in which a positive electrode can and a negative electrode can are integrated via a gasket.
前記帯状の正極体と前記帯状の負極体の表裏両面及び側面を含む周面に設けた塗膜硬化層が前記巻回状態で融合一体化されたセパレータ層が設けられたことを特徴とする請求項1または請求項2に記載の電気化学セル。 A claim characterized in that a separator layer is provided in which a coating film cured layer provided on both front and back surfaces of the band-shaped positive electrode body and the peripheral surface including the side surfaces of the band-shaped negative electrode body is fused and integrated in the wound state. The electrochemical cell according to claim 1 or 2. 前記正極体と前記負極体の一部に延出部が形成され、前記延出部の先端側に前記塗膜硬化層からなるセパレータ層が形成されていない接続タブが形成されたことを特徴とする請求項1〜請求項3のいずれか一項に記載の電気化学セル。 An extension portion is formed on the positive electrode body and a part of the negative electrode body, and a connection tab is formed on the tip end side of the extension portion without a separator layer made of the coating film cured layer. The electrochemical cell according to any one of claims 1 to 3. 前記内側容器の外周壁と前記外側容器の外周壁が金属箔の両面に樹脂層を設けたラミネート構造体からなることを特徴とする請求項1〜請求項4のいずれか一項に記載の電気化学セル。 The electricity according to any one of claims 1 to 4, wherein the outer peripheral wall of the inner container and the outer peripheral wall of the outer container are made of a laminated structure in which resin layers are provided on both sides of a metal foil. Chemical cell. 前記帯状の正極体と前記帯状の負極体が、いずれも、前記外装体の平面視形状に類似する平面視形状の複数の電極本体と、これら複数の電極本体を接続する電極接続部を有し、前記正極体と前記負極体が前記塗膜硬化層を介し互いに渦巻き状に巻回されて一体化され、
前記正極体の前記電極本体および前記電極接続部と、前記負極体の前記電極本体および前記電極接続部が、いずれも前記塗膜硬化層からなるセパレータ層に覆われたことを特徴とする請求項1〜請求項5のいずれか一項に記載の電気化学セル。
Both the band-shaped positive electrode body and the band-shaped negative electrode body have a plurality of electrode bodies having a plan view shape similar to the plan view shape of the exterior body, and an electrode connecting portion for connecting the plurality of electrode bodies. , The positive electrode body and the negative electrode body are spirally wound around each other via the coating film cured layer and integrated.
The claim is characterized in that the electrode body and the electrode connecting portion of the positive electrode body, and the electrode body and the electrode connecting portion of the negative electrode body are all covered with a separator layer made of the coating film cured layer. The electrochemical cell according to any one of 1 to 5.
前記電極本体と前記電極接続部が、いずれも、金属箔からなる集電体層の表裏両面に活物質層を備えたことを特徴とする請求項1〜請求項6のいずれか一項に記載の電気化学セル。 The invention according to any one of claims 1 to 6, wherein both the electrode body and the electrode connecting portion are provided with active material layers on both the front and back surfaces of a current collector layer made of a metal foil. Electrochemical cell. 正極体と負極体の少なくとも一方において少なくとも一方の面を被覆した塗膜硬化層からなるセパレータ層を介し、前記正極体と前記負極体を積層してなる電極積層体を備え、
外周壁を有する内側容器と外周壁を有する外側容器からなり、前記内側容器の外周壁と前記外側容器の外周壁を重ね合わせて折り曲げ融着一体化した外装体に、前記電極積層体が収容されたことを特徴とする電気化学セル。
An electrode laminate formed by laminating the positive electrode body and the negative electrode body is provided via a separator layer composed of a coating film curing layer covering at least one surface of at least one of the positive electrode body and the negative electrode body.
The electrode laminate is housed in an outer body composed of an inner container having an outer peripheral wall and an outer container having an outer peripheral wall, and the outer peripheral wall of the inner container and the outer peripheral wall of the outer container are overlapped and bent and fused and integrated. An electrochemical cell characterized by that.
請求項1、請求項3〜請求項7のいずれか一項に記載の電気化学セルの製造方法において、帯状の正極体と帯状の負極体の少なくとも一方において、少なくとも一面に硬化型の塗膜を形成した後、前記塗膜が半硬化の状態で前記正極体と前記負極体を巻回して電極積層体を構成し、この電極積層体を外装体の内部に収容して外装体の形を整えた後、前記半硬化塗膜を硬化させることを特徴とする電気化学セルの製造方法。 In the method for producing an electrochemical cell according to any one of claims 1 and 3 to 7, a curable coating film is applied to at least one surface of at least one of a band-shaped positive electrode body and a band-shaped negative electrode body. After the formation, the positive electrode body and the negative electrode body are wound around the positive electrode body and the negative electrode body in a semi-cured state to form an electrode laminate, and the electrode laminate is housed inside the exterior body to shape the exterior body. After that, a method for producing an electrochemical cell, which comprises curing the semi-cured coating film.
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