JP2020177751A - Secondary cell - Google Patents

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JP2020177751A
JP2020177751A JP2019077665A JP2019077665A JP2020177751A JP 2020177751 A JP2020177751 A JP 2020177751A JP 2019077665 A JP2019077665 A JP 2019077665A JP 2019077665 A JP2019077665 A JP 2019077665A JP 2020177751 A JP2020177751 A JP 2020177751A
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current collector
laminated
positive electrode
negative electrode
electrode current
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JP7212845B2 (en
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巖 新田
Gen Nitta
巖 新田
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Toyota Motor Corp
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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  • Cell Electrode Carriers And Collectors (AREA)
  • Connection Of Batteries Or Terminals (AREA)

Abstract

To provide a secondary cell having a structure where impregnation of a wound electrode body with electrolyte is improved.SOLUTION: A secondary cell includes: a wound electrode body of such structure as a positive electrode where a positive electrode active material layer is formed on a long sheet-like positive electrode collector, and a negative electrode where a negative electrode active material layer is formed on a long sheet-like negative electrode collector, are laminated with a separator in between, and wound in the longer direction; a battery case; and collector terminals of positive and negative electrodes connected with the positive and negative electrodes of the wound electrode body, respectively. On one end of the wound electrode body in the width direction orthogonal to the longer direction of the sheet, a collector exposure part not having the active material layer and exposing the collector is laminated. In a portion of the laminated part, a collector terminal juncture where the collector terminals are joined is formed and, in a region including at least the collector terminal juncture of a portion where the collector exposure part on at least one side of the positive and negative electrodes is laminated, a conductive material is filled between the collectors thus laminated.SELECTED DRAWING: Figure 3

Description

本発明は、二次電池に関する。詳しくは、二次電池の捲回電極体の集電体露出部と集電端子との接合部位を含む領域の構造に関する。 The present invention relates to a secondary battery. More specifically, the present invention relates to the structure of a region including a joint portion between the exposed portion of the current collector and the current collector terminal of the wound electrode body of the secondary battery.

リチウムイオン二次電池、ニッケル水素電池等の二次電池は、軽量かつエネルギー密度が高いことから、近年、パソコンや携帯端末等のいわゆるポータブル電源さらには車両駆動用電源として好ましく用いられている。なかでもリチウムイオン二次電池は、電流密度や単位質量あたりの電池容量が高いことから、特に、電気自動車（ＥＶ）、ハイブリッド自動車（ＨＶ）、プラグインハイブリッド自動車（ＰＨＶ）等の車両の駆動用高出力電源として、益々の普及が期待されている。 Secondary batteries such as lithium ion secondary batteries and nickel-metal hydride batteries are lightweight and have a high energy density, and are therefore preferably used as so-called portable power sources for personal computers and mobile terminals and as power sources for driving vehicles in recent years. Among them, lithium-ion secondary batteries have high current density and battery capacity per unit mass, so they are especially used for driving vehicles such as electric vehicles (EV), hybrid vehicles (HV), and plug-in hybrid vehicles (PHV). It is expected to become more and more popular as a high-output power source.

リチウムイオン二次電池、ナトリウムイオン二次電池等を構成する電極体の一形態として、例えば、長尺なシート状の正極集電体に正極活物質層が形成された長尺なシート状の正極および長尺なシート状の負極集電体に負極活物質層が形成された長尺なシート状の負極が、セパレータを介在させつつ積層され、長手方向に捲回された構造の捲回電極体が挙げられる。
このような捲回電極体は、該捲回電極体の長手方向に直交する幅方向における端部において、集電体露出部が積層されている。そして、捲回電極体は、積層された集電体露出部の一部に、集電端子が接合された状態で、電解液とともに電池ケース内に収容されている。例えば特許文献１および特許文献２では、活物質層非形成部分（集電体露出部）と端子との接合形態、および、電池ケース内への収容形態に関する技術が開示されている。 As one form of the electrode body constituting the lithium ion secondary battery, the sodium ion secondary battery, etc., for example, a long sheet-shaped positive electrode in which a positive electrode active material layer is formed on a long sheet-shaped positive electrode current collector. A wound electrode body having a structure in which a long sheet-shaped negative electrode having a negative electrode active material layer formed on a long sheet-shaped negative electrode current collector is laminated with a separator interposed therebetween and wound in the longitudinal direction. Can be mentioned.
In such a wound electrode body, a current collector exposed portion is laminated at an end portion in the width direction orthogonal to the longitudinal direction of the wound electrode body. The wound electrode body is housed in the battery case together with the electrolytic solution in a state where the current collector terminal is joined to a part of the laminated current collector exposed portion. For example, Patent Document 1 and Patent Document 2 disclose techniques relating to a bonding form between an active material layer non-forming portion (current collector exposed portion) and a terminal, and a housing mode in a battery case.

特開２０１５−４１５８９号公報JP-A-2015-41589 特開２０１４−１４９９９６号公報Japanese Unexamined Patent Publication No. 2014-149996

ところで、電池反応においては、捲回電極体の内部に電解液が含浸し、これが活物質等と接触する必要がある。この際、電解液は上述のような集電体露出部が積層された部分を介して捲回電極体の内部に含浸するため、当該部位が電解液の含浸に対する開口部となっている。即ち、電解液が捲回電極体の内部に含浸する効率は、開口部としての上記集電体露出部が積層された部分の積層厚み等によって調整されている。 By the way, in the battery reaction, the inside of the wound electrode body is impregnated with the electrolytic solution, which needs to come into contact with the active material or the like. At this time, since the electrolytic solution is impregnated inside the wound electrode body through the portion where the current collector exposed portion is laminated as described above, the portion is an opening for impregnation of the electrolytic solution. That is, the efficiency of impregnating the inside of the wound electrode body with the electrolytic solution is adjusted by the stacking thickness of the portion where the current collector exposed portion as the opening is laminated.

しかし、例えば、上記特許文献１で開示されるような接合形態では、接合部に近い部位と遠い部位とで、上記積層厚みに差が生じている。そのため、このような捲回電極体の内部への電解液の含浸量については、部位によってムラが生じることがある。具体的には、例えば、接合部および接合部に近い部位は局所的に積層厚みが小さくなる。そのため、このような部位における電解液の含浸量は少なくなる。したがって、このような部位においては、局所的に抵抗が増大し、電荷担体（例えば、リチウムイオン二次電池においてはリチウムイオン）に由来する物質が析出する虞がある。これは、電池の信頼性および安全性を低下させる要因となるため好ましくない。 However, for example, in the joint form disclosed in Patent Document 1, there is a difference in the laminated thickness between the portion near the joint portion and the portion far from the joint portion. Therefore, the amount of the electrolytic solution impregnated inside the wound electrode body may be uneven depending on the site. Specifically, for example, the laminated thickness is locally reduced in the joint portion and the portion close to the joint portion. Therefore, the amount of the electrolytic solution impregnated in such a portion is reduced. Therefore, at such a site, the resistance may increase locally, and a substance derived from a charge carrier (for example, lithium ion in a lithium ion secondary battery) may be precipitated. This is not preferable because it causes a decrease in the reliability and safety of the battery.

そこで、本発明はかかる課題を解決すべく創出されたものであり、捲回電極体の集電端子接合部における上記積層厚みの不均一さの発生を抑制することによって、該捲回電極体内部への電解液の含浸が向上された構造を有する二次電池の提供を目的とする。 Therefore, the present invention has been created to solve such a problem, and by suppressing the occurrence of the non-uniformity of the laminated thickness at the current collecting terminal joint portion of the wound electrode body, the inside of the wound electrode body. It is an object of the present invention to provide a secondary battery having a structure in which impregnation of an electrolytic solution is improved.

本発明者は、捲回電極体の集電体露出部が積層された部分の少なくとも集電端子を接合する部分を含む領域における各集電体間を導電性物質で充填することに着目した。これによって、集電端子接合後も、当該部位の積層厚みが局所的に小さくなるのを防止することができ、集電端子露出部の積層厚みの不均一さ発生を抑制し得ることを見出し、本発明を完成するに至った。 The present inventor has focused on filling the space between each current collector in the region including at least the portion where the current collector exposed portion of the wound electrode body is laminated and at least the portion where the current collector terminals are joined with a conductive substance. As a result, it has been found that it is possible to prevent the laminated thickness of the relevant portion from being locally reduced even after joining the current collecting terminals, and it is possible to suppress the occurrence of non-uniformity of the laminated thickness of the exposed portion of the current collecting terminal. The present invention has been completed.

即ち、上記目的を実現するべく、本発明は、長尺なシート状の正極集電体に正極活物質層が形成された長尺なシート状の正極および長尺なシート状の負極集電体に負極活物質層が形成された長尺なシート状の負極が、セパレータを介在させつつ積層され、長手方向に捲回された構造の捲回電極体と、上記捲回電極体を電解液とともに収容する電池ケースと、上記電池ケース内に少なくとも一部が配置され、上記捲回電極体の正極および負極にそれぞれ接続された正極集電端子および負極集電端子と、を備えた二次電池である。
上記捲回電極体のシート長手方向に直交する幅方向における一方の端部には、上記正極活物質層を有しないで上記正極集電体が露出した正極集電体露出部が積層されている。該積層された部分の一部には、上記正極集電端子が接合された正極集電端子接合部が形成されている。
上記幅方向における他方の端部には、上記負極活物質層を有しないで上記負極集電体が露出した負極集電体露出部が積層されている。該積層された部分の一部には、上記負極集電端子が接合された負極集電端子接合部が形成されている。
ここで正負極のいずれか少なくとも一方の極側の上記集電体露出部が積層された部分の少なくとも上記集電端子接合部を含む領域において導電性物質が積層する各集電体間に充填されていることを特徴とする。 That is, in order to realize the above object, the present invention presents a long sheet-shaped positive electrode collector in which a positive electrode active material layer is formed on a long sheet-shaped positive electrode current collector, and a long sheet-shaped negative electrode current collector. A wound electrode body having a structure in which a long sheet-shaped negative electrode having a negative electrode active material layer formed therein is laminated with a separator interposed therebetween and wound in the longitudinal direction, and the wound electrode body together with an electrolytic solution. A secondary battery including a battery case for accommodating and a positive electrode current collecting terminal and a negative electrode current collecting terminal which are arranged at least a part in the battery case and are connected to the positive electrode and the negative electrode of the wound electrode body, respectively. is there.
At one end of the wound electrode body in the width direction orthogonal to the sheet longitudinal direction, a positive electrode current collector exposed portion which does not have the positive electrode active material layer and the positive electrode current collector is exposed is laminated. .. A positive electrode current collecting terminal joint portion to which the positive electrode current collecting terminal is joined is formed in a part of the laminated portion.
A negative electrode current collector exposed portion in which the negative electrode current collector is exposed without having the negative electrode active material layer is laminated on the other end portion in the width direction. A negative electrode current collecting terminal joint portion to which the negative electrode current collecting terminal is joined is formed in a part of the laminated portion.
Here, it is filled between the current collectors in which the conductive material is laminated in the region including at least the current collector terminal joint portion of the portion where the current collector exposed portion on the pole side of at least one of the positive and negative electrodes is laminated. It is characterized by being.

かかる構成の二次電池では、捲回電極体の集電体露出部が積層された部分の少なくとも上記集電端子接合部を含む領域において、各集電体間に導電性物質が充填されている。即ち、このような領域においては、集電端子の接合によって生じ得る、集電体露出部の積層厚みの不均一性の発生を抑制することができる。したがって、本構成の二次電池によると、捲回電極体における電解液の含浸量に部位ごとのムラが生じるのを防止することができる。そして、捲回電極体への電解液の含浸量を増やすことができる。これによって、電荷担体由来の物質が生成されるのを防止して二次電池の電池性能を向上させることができる。 In the secondary battery having such a configuration, a conductive substance is filled between the current collectors in at least the region including the current collector terminal joint portion of the portion where the current collector exposed portion of the wound electrode body is laminated. .. That is, in such a region, it is possible to suppress the occurrence of non-uniformity of the laminated thickness of the exposed portion of the current collector, which may occur due to the joining of the current collector terminals. Therefore, according to the secondary battery having this configuration, it is possible to prevent the impregnation amount of the electrolytic solution in the wound electrode body from being uneven at each site. Then, the amount of the electrolytic solution impregnated into the wound electrode body can be increased. This makes it possible to prevent the generation of substances derived from charge carriers and improve the battery performance of the secondary battery.

一実施形態に係る二次電池の構成を模式的に示す断面図である。It is sectional drawing which shows typically the structure of the secondary battery which concerns on one Embodiment. 一実施形態に係る二次電池の捲回電極体の積層構造を示す模式図である。It is a schematic diagram which shows the laminated structure of the wound electrode body of the secondary battery which concerns on one Embodiment. 一実施形態に係る二次電池の捲回電極体の構成を模式的に示す断面図である。It is sectional drawing which shows typically the structure of the winding electrode body of the secondary battery which concerns on one Embodiment. 一実施形態に係る二次電池の樹脂フィルムの構造を模式的に示す斜視図である。It is a perspective view which shows typically the structure of the resin film of the secondary battery which concerns on one Embodiment.

以下、図面を適宜参照しながら、ここで開示される二次電池の好適な実施形態について説明する。なお、各図における寸法関係（長さ、幅、厚さ等）は実際の寸法関係を反映するものではない。また、本明細書において特に言及している事項以外の事柄であって本発明の実施に必要な事柄は、該分野における従来技術に基づく当業者の設計事項として把握され得る。さらに、本明細書において数値範囲：Ａ〜Ｂ（ここでＡとＢは、Ａ＜Ｂの関係にある任意の数値）と記載している場合は、Ａ以上Ｂ以下を意味しており、Ａを上回る場合（Ａを含まずにそれ以上の場合）、Ｂを下回る場合（Ｂを含まずにそれ以下の場合）も包含される数値範囲である。 Hereinafter, preferred embodiments of the secondary battery disclosed herein will be described with reference to the drawings as appropriate. The dimensional relationships (length, width, thickness, etc.) in each figure do not reflect the actual dimensional relationships. In addition, matters other than those specifically mentioned in the present specification and necessary for carrying out the present invention can be grasped as design matters of those skilled in the art based on the prior art in the art. Further, when the numerical range: A to B (where A and B are arbitrary numerical values having a relationship of A <B) is described in the present specification, it means A or more and B or less, and A. It is a numerical range that includes the case where it exceeds (when it is more than A not included) and the case where it is less than B (when it is less than B not included).

本明細書において「二次電池」とは、充放電可能で所定の電気エネルギーを繰り返し取り出し得る蓄電装置をいう。例えば、電解質中のアルカリ金属イオンが電荷の移動を担うリチウムイオン二次電池、ナトリウムイオン二次電池等は、ここでいう二次電池に包含される典型例である。
「電極体」とは、正極、負極、および正負極間にセパレータとして機能し得るセパレータを含む電池の主体を成す構造体をいう。「活物質」とは、電荷担体となる化学種（例えば、リチウムイオン二次電池においてはリチウムイオン、ナトリウムイオン二次電池においてはナトリウムイオン）を可逆的に吸蔵および放出可能な化合物（活物質）をいう。また、「導電性物質」とは、導電性物質する材料の体積抵抗率が１５×１０−３Ω・ｃｍ以下であることを意味する。
以下、本発明を、扁平形状の捲回電極体を備えたリチウムイオン二次電池（以下、単に「二次電池」ともいう。）に適用する場合を主として本発明について詳細に説明する。なお、本発明をかかる実施形態に記載されたものに限定することを意図したものではない。 As used herein, the term "secondary battery" refers to a power storage device that can be charged and discharged and can repeatedly take out predetermined electrical energy. For example, a lithium ion secondary battery, a sodium ion secondary battery, and the like in which alkali metal ions in an electrolyte are responsible for charge transfer are typical examples included in the secondary battery referred to here.
The “electrode body” refers to a structure that constitutes the main body of a battery including a separator that can function as a separator between a positive electrode, a negative electrode, and a positive electrode and a negative electrode. The "active material" is a compound (active material) capable of reversibly occluding and releasing a chemical species serving as a charge carrier (for example, lithium ion in a lithium ion secondary battery and sodium ion in a sodium ion secondary battery). To say. Further, the “conductive substance” means that the volume resistivity of the material to be the conductive substance is 15 × 10 -3 Ω · cm or less.
Hereinafter, the present invention will be described in detail mainly when the present invention is applied to a lithium ion secondary battery (hereinafter, also simply referred to as “secondary battery”) provided with a flat-shaped wound electrode body. It should be noted that the present invention is not intended to be limited to those described in such embodiments.

まず初めに、ここで開示される二次電池の構造について、図１を参照しながら説明する。図１は、一実施形態に係る二次電池の構成を模式的に示す断面図である。
＜全体構造＞
図１に示されるように、ここで開示される二次電池１００は、捲回電極体８０と、該捲回電極体８０を電解液（図示なし）とともに収容する電池ケース２０とを備える。また、二次電池１００は、樹脂フィルム１０を備える。そして、樹脂フィルム１０は、捲回電極体８０を電解液とともに収容し、この状態で電池ケース２０に収容されている。
＜電池ケース＞
電池ケース２０は、上端が開放された扁平な直方体形状の電池ケース本体２２と、その開口部を塞ぐ蓋体２４とを備える。電池ケース２０の上面（即ち、蓋体２４）には、外部接続用の正極端子４２および負極端子４４が設けられている。これら正極端子４２および負極端子４４の一部は、それぞれ、電池ケース２０内に少なくとも一部が配置された板状の正極集電端子９２および負極集電端子９４にそれぞれ接続されている。蓋体２４にはまた、従来のリチウムイオン二次電池の電池ケースと同様に、電池ケース２０の内部で発生したガスを電池ケース２０の外部に排出するための安全弁２６と、電解液を注液するための注液孔２８が備えられている。
電池ケース２０の材質としては、例えば、アルミニウム等の金属材料が挙げられる。 First, the structure of the secondary battery disclosed here will be described with reference to FIG. FIG. 1 is a cross-sectional view schematically showing a configuration of a secondary battery according to an embodiment.
<Overall structure>
As shown in FIG. 1, the secondary battery 100 disclosed here includes a wound electrode body 80 and a battery case 20 that houses the wound electrode body 80 together with an electrolytic solution (not shown). Further, the secondary battery 100 includes a resin film 10. Then, the resin film 10 houses the wound electrode body 80 together with the electrolytic solution, and is housed in the battery case 20 in this state.
<Battery case>
The battery case 20 includes a flat rectangular parallelepiped battery case main body 22 having an open upper end, and a lid body 24 that closes the opening thereof. A positive electrode terminal 42 and a negative electrode terminal 44 for external connection are provided on the upper surface (that is, the lid 24) of the battery case 20. A part of the positive electrode terminal 42 and the negative electrode terminal 44 is connected to a plate-shaped positive electrode current collecting terminal 92 and a negative electrode current collecting terminal 94, which are at least partially arranged in the battery case 20, respectively. Similarly to the battery case of the conventional lithium ion secondary battery, the lid 24 is injected with a safety valve 26 for discharging the gas generated inside the battery case 20 to the outside of the battery case 20 and an electrolytic solution. A liquid injection hole 28 is provided for this purpose.
Examples of the material of the battery case 20 include a metal material such as aluminum.

＜電解液＞
電解液としては、典型的には、非水溶媒（有機溶媒）中に支持塩（即ち、電解質）を含有する非水電解液を用いることができる。
非水溶媒としては、例えば、エチレンカーボネート（ＥＣ）、プロピレンカーボネート（ＰＣ）、ジメチルカーボネート（ＤＭＣ）、ジエチルカーボネート（ＤＥＣ）、およびエチルメチルカーボネート（ＥＭＣ）等のうちの１種を単独で、あるいは２種以上を適宜組み合わせて用いることができる。支持塩としては、例えば、ＬｉＰＦ６を用いる。 <Electrolytic solution>
As the electrolytic solution, typically, a non-aqueous electrolytic solution containing a supporting salt (that is, an electrolyte) in a non-aqueous solvent (organic solvent) can be used.
As the non-aqueous solvent, for example, one of ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), diethyl carbonate (DEC), ethyl methyl carbonate (EMC) and the like can be used alone or. Two or more types can be used in combination as appropriate. As the supporting salt, for example, LiPF 6 is used.

＜捲回電極体＞
次に、捲回電極体８０の構造について、図１および図２を参照しながら説明する。図２は、一実施形態に係る二次電池の捲回電極体の積層構造を示す模式図である。
図示されるように、捲回電極体８０は、長尺なシート状の正極集電体５２の片面または両面（ここでは両面）に長手方向Ｙに沿って正極活物質層５４が形成された正極５０と、長尺なシート状の負極集電体６２の片面または両面（ここでは両面）に長手方向Ｙに沿って負極活物質層６４が形成された負極６０とを、長尺なシート状のセパレータ７０を介在させつつ積層されて長手方向Ｙに捲回され扁平形状に成形されている。
捲回電極体８０の捲回軸方向における中央部分には、捲回コア部分（すなわち、正極５０の正極活物質層５４と、負極６０の負極活物質層６４と、セパレータ７０とが密に積層された部分）が形成されている。
また、捲回電極体８０のシート長手方向Ｙに直交する幅方向Ｘにおける一方の端部には、正極活物質層５４を有しないで正極集電体５２が露出した正極集電体露出部５２ａが積層されて捲回コア部分からはみ出ている。さらに、幅方向Ｘにおける他方の端部には、負極活物質層６４を有しないで負極集電体６２が露出した負極集電体露出部６２ａが積層されて捲回コア部分からはみ出ている。 <Rotating electrode body>
Next, the structure of the wound electrode body 80 will be described with reference to FIGS. 1 and 2. FIG. 2 is a schematic view showing a laminated structure of wound electrode bodies of a secondary battery according to an embodiment.
As shown in the figure, the wound electrode body 80 is a positive electrode in which a positive electrode active material layer 54 is formed along a longitudinal direction Y on one side or both sides (here, both sides) of a long sheet-shaped positive electrode current collector 52. The 50 and the negative electrode 60 in which the negative electrode active material layer 64 is formed along the longitudinal direction Y on one side or both sides (here, both sides) of the long sheet-shaped negative electrode current collector 62 are formed into a long sheet-like negative electrode. It is laminated with the separator 70 interposed therebetween and wound in the longitudinal direction Y to form a flat shape.
The winding core portion (that is, the positive electrode active material layer 54 of the positive electrode 50, the negative electrode active material layer 64 of the negative electrode 60, and the separator 70 are densely laminated in the central portion of the wound electrode body 80 in the winding axis direction. The formed part) is formed.
Further, the positive electrode current collector exposed portion 52a in which the positive electrode current collector 52 is exposed without having the positive electrode active material layer 54 at one end in the width direction X orthogonal to the sheet longitudinal direction Y of the wound electrode body 80. Are laminated and protrude from the winding core part. Further, a negative electrode current collector exposed portion 62a, which does not have the negative electrode active material layer 64 and is exposed to the negative electrode current collector 62, is laminated on the other end portion in the width direction X and protrudes from the winding core portion.

捲回電極体８０の正極５０、負極６０、セパレータ７０を構成する材料、部材は従来の一般的なリチウムイオン二次電池と同様のものを使用可能である。
−正極−
正極集電体５２としては、例えば、アルミニウム製の正極集電体が挙げられる。
正極活物質層５４には、正極活物質、必要に応じて導電助剤、バインダ等が含まれる。
正極活物質としては、リチウムイオンを吸蔵および放出可能な材料であって、リチウム元素と一種または二種以上の遷移金属元素とを含むリチウム含有化合物を好適に用いることができる。具体的には、例えば、ＬｉＮｉ１／３Ｃｏ１／３Ｍｎ１／３Ｏ２等のリチウム遷移金属酸化物、ＬｉＦｅＰＯ４等のリチウム遷移金属リン酸化合物が挙げられる。
導電助剤としては、例えば、アセチレンブラック（ＡＢ）等が挙げられる。バインダとしては、例えば、ポリフッ化ビニリデン（ＰＶＤＦ）、ブチルゴム（ＢＲ）、アクリロニトリルブタジエンゴム（ＡＢＲ）、スチレンブタジエンゴム（ＳＢＲ）等が挙げられる。
正極集電端子９２としては、例えば、アルミニウム製またはアルミニウム合金製の正極集電端子が挙げられる。 The materials and members constituting the positive electrode 50, the negative electrode 60, and the separator 70 of the wound electrode body 80 can be the same as those of a conventional general lithium ion secondary battery.
-Positive electrode-
Examples of the positive electrode current collector 52 include a positive electrode current collector made of aluminum.
The positive electrode active material layer 54 contains a positive electrode active material, a conductive auxiliary agent, a binder, and the like, if necessary.
As the positive electrode active material, a lithium-containing compound which is a material capable of occluding and releasing lithium ions and which contains a lithium element and one or more kinds of transition metal elements can be preferably used. Specific examples thereof include lithium transition metal oxides such as LiNi 1/3 Co 1/3 Mn 1/3 O 2 and lithium transition metal phosphoric acid compounds such as LiFePO 4 .
Examples of the conductive auxiliary agent include acetylene black (AB) and the like. Examples of the binder include polyvinylidene fluoride (PVDF), butyl rubber (BR), acrylonitrile butadiene rubber (ABR), styrene butadiene rubber (SBR) and the like.
Examples of the positive electrode current collecting terminal 92 include a positive electrode current collecting terminal made of aluminum or an aluminum alloy.

−負極−
負極集電体６２としては、例えば、銅製の負極集電体が挙げられる。
負極活物質層６４には、正極活物質、必要に応じて導電助剤、バインダ等が含まれる。
負極活物質としては、例えば、リチウムイオンを吸蔵および放出可能な天然黒鉛（石墨）や人工黒鉛などの黒鉛系材料、シリコンおよびスズならびにこれらの化合物が挙げられる。
導電助剤およびバインダとしては上述のものを適宜使用することができる。また、負極活物質層６４の構成材料として、カルボキシメチルセルロース（ＣＭＣ）等の増粘剤を添加してもよい。
負極集電端子９４としては、例えば、銅製または銅合金製の負極集電端子が挙げられる。 − Negative electrode −
Examples of the negative electrode current collector 62 include a copper negative electrode current collector.
The negative electrode active material layer 64 contains a positive electrode active material, a conductive auxiliary agent, a binder, and the like, if necessary.
Examples of the negative electrode active material include graphite-based materials such as natural graphite (stone ink) and artificial graphite capable of occluding and releasing lithium ions, silicon and tin, and compounds thereof.
As the conductive auxiliary agent and the binder, the above-mentioned ones can be appropriately used. Further, a thickener such as carboxymethyl cellulose (CMC) may be added as a constituent material of the negative electrode active material layer 64.
Examples of the negative electrode current collecting terminal 94 include a negative electrode current collecting terminal made of copper or a copper alloy.

−セパレータ−
セパレータ７０としては、例えば、ポリエチレン（ＰＥ）、ポリプロピレン（ＰＰ）、ポリエステル、セルロース、ポリアミド等の樹脂から成る多孔性シート（フィルム）が挙げられる。該多孔性シートは、単層構造であってもよく、二層以上の積層構造（例えば、ＰＥ層の両面にＰＰ層が積層された三層構造）であってもよい。 − Separator −
Examples of the separator 70 include a porous sheet (film) made of a resin such as polyethylene (PE), polypropylene (PP), polyester, cellulose, and polyamide. The porous sheet may have a single-layer structure or a laminated structure of two or more layers (for example, a three-layer structure in which PP layers are laminated on both sides of a PE layer).

＜集電体露出部および集電端子の接合＞
次に、捲回電極体８０の端部における集電体露出部および集電端子の接合構造について、図３を参照しつつ説明する。図３は、一実施形態に係る二次電池の捲回電極体の構成を模式的に示す断面図である。
図３に示されるように、正極集電体露出部５２ａが積層された部分の一部には、正極集電端子９２が接合された正極集電端子接合部Ｍ１が形成されている。また、負極集電体露出部６２ａが積層された部分の一部には、負極集電端子９４が接合された負極集電端子接合部Ｍ２が形成されている。 <Joining the exposed part of the current collector and the current collector terminal>
Next, the joint structure of the current collector exposed portion and the current collector terminal at the end of the wound electrode body 80 will be described with reference to FIG. FIG. 3 is a cross-sectional view schematically showing the configuration of the wound electrode body of the secondary battery according to the embodiment.
As shown in FIG. 3, a positive electrode current collector terminal joint portion M1 to which the positive electrode current collector terminal 92 is bonded is formed in a part of the portion where the positive electrode current collector exposed portion 52a is laminated. Further, a negative electrode current collector terminal joint M2 to which the negative electrode current collector terminal 94 is bonded is formed in a part of the portion where the negative electrode current collector exposed portion 62a is laminated.

＜導電性物質の充填＞
図３に示されるように、正極および負極のいずれか少なくとも一方の極側の集電体露出部が積層された部分の少なくとも集電端子接合部を含む領域において、導電性物質３０が積層する各集電体間に充填されている。即ち、正極については、正極集電体露出部５２ａが積層された部分の少なくとも正極集電端子接合部Ｍ１を含む領域において、導電性物質３０が積層する各集電体間に充填されている。負極については、負極集電体露出部６２ａが積層された部分の少なくとも負極集電端子接合部Ｍ２を含む領域において、導電性物質３０が積層する各集電体間に充填されている。
導電性物質３０が充填されることにより、集電端子と集電体露出部を接合しても、集電端子接合部Ｍ１（Ｍ２）における集電体露出部の積層厚みＷ２、および、集電端子接合部Ｍ１（Ｍ２）に近い部位の積層厚みが局所的に小さくなるのを防止することができる。これによって、集電体露出部における積層厚みＷ１に不均一性が発生するのを防止することができる。 <Filling with conductive material>
As shown in FIG. 3, each of the conductive substances 30 is laminated in the region including at least the current collector terminal joint of the portion where the current collector exposed portion on the pole side of at least one of the positive electrode and the negative electrode is laminated. It is filled between the current collectors. That is, the positive electrode is filled between the current collectors on which the conductive substance 30 is laminated, at least in the region including the positive electrode current collector terminal joint M1 in the portion where the positive electrode current collector exposed portion 52a is laminated. The negative electrode is filled between the current collectors on which the conductive substance 30 is laminated, at least in the region including the negative electrode current collector terminal joint M2 in the portion where the negative electrode current collector exposed portion 62a is laminated.
By filling with the conductive substance 30, even if the current collector terminal and the current collector exposed portion are joined, the laminated thickness W2 of the current collector exposed portion at the current collector terminal joint portion M1 (M2) and the current collector are collected. It is possible to prevent the laminated thickness of the portion close to the terminal joint portion M1 (M2) from being locally reduced. As a result, it is possible to prevent non-uniformity of the laminated thickness W1 in the exposed portion of the current collector.

＜導電性物質の組成＞
導電性物質３０は、例えば、導電材料と樹脂とを含む。導電材料としては、例えば、銀、金、銅、ニッケルおよびカーボン等の導電材料が挙げられる。樹脂としては、アクリル系樹脂等の熱可塑性樹脂、エポキシ系樹脂およびシリコン系樹脂等の熱硬化性樹脂が挙げられる。
導電性物質３０の導電性の指標としての体積抵抗率は、例えば、１５×１０−３Ω・ｃｍ以下、１０×１０−３Ω・ｃｍ以下、または、５×１０−３Ω・ｃｍ以下であることが好ましい。また、該体積抵抗率は、例えば、０．１×１０−３Ω・ｃｍ以上、または、０．５×１０−３Ω・ｃｍ以上である。 <Composition of conductive material>
The conductive substance 30 includes, for example, a conductive material and a resin. Examples of the conductive material include conductive materials such as silver, gold, copper, nickel and carbon. Examples of the resin include thermoplastic resins such as acrylic resins and thermosetting resins such as epoxy resins and silicon resins.
The volume resistivity of the conductive substance 30 as an index of conductivity is, for example, 15 × 10 -3 Ω · cm or less, 10 × 10 -3 Ω · cm or less, or 5 × 10 -3 Ω · cm or less. It is preferable to have. The volume resistivity is, for example, 0.1 × 10 -3 Ω · cm or more, or 0.5 × 10 -3 Ω · cm or more.

＜樹脂フィルムの構造＞
次に、樹脂フィルム１０について図４を参照しながら説明する。図４は、一実施形態に係る二次電池の樹脂フィルムの構造を模式的に示す斜視図である。
図示されるように、樹脂フィルム１０は上端が開放された有底の袋状の構造を有しており、上端開口を介して捲回電極体が収容されている。また、樹脂フィルム１０は、内部に収容される捲回電極体の、捲回方向と直交する横断面と対向する面１０Ａにおいて、上端側（即ち、開口部側）および下端側（即ち、底側）に少なくとも一つずつの孔が形成されている。具体的には、例えば、面１０Ａの上端側には孔１２が形成されており、下端側には孔１４が形成されている。孔１２が形成されていることによって、例えば、二次電池製造過程において電解液を電池ケースに注液する際、電解液が樹脂フィルム１０内に注液されやすくなる。一方、孔１４が形成されていることによって、樹脂フィルム１０内に注液された電解液が、樹脂フィルム１０の外に漏出したとしても、孔１４を介して樹脂フィルム１０に流入されやすくなる。孔１２および孔１４は、２つの面１０Ａのいずれにも形成されることが好ましいが、片面に形成されていてもよい。また、例えば、一の面１０Ａに孔１２が形成され、他方の面１０Ａに孔１４が形成されてもよい。
また、図示されるように、孔１２の直下には矩形状の羽板１６が付設されている。羽板１６が付設されていることによって、孔１２から樹脂フィルム１０に電解液が適切に注液されやすくなる。羽板１６は、２つの面１０Ａにおける孔１２のいずれにも付設されることが好ましいが、いずれか一方に付設される構造であってもよい。 <Structure of resin film>
Next, the resin film 10 will be described with reference to FIG. FIG. 4 is a perspective view schematically showing the structure of the resin film of the secondary battery according to the embodiment.
As shown in the figure, the resin film 10 has a bottomed bag-like structure in which the upper end is open, and the wound electrode body is housed through the upper end opening. Further, the resin film 10 is formed on the upper end side (that is, the opening side) and the lower end side (that is, the bottom side) of the wound electrode body housed therein on the surface 10A facing the cross section orthogonal to the winding direction. ) Has at least one hole. Specifically, for example, a hole 12 is formed on the upper end side of the surface 10A, and a hole 14 is formed on the lower end side. Since the holes 12 are formed, for example, when the electrolytic solution is injected into the battery case in the process of manufacturing the secondary battery, the electrolytic solution is easily injected into the resin film 10. On the other hand, since the holes 14 are formed, even if the electrolytic solution injected into the resin film 10 leaks out of the resin film 10, it is likely to flow into the resin film 10 through the holes 14. The holes 12 and 14 are preferably formed on either of the two surfaces 10A, but may be formed on one surface. Further, for example, the hole 12 may be formed on one surface 10A and the hole 14 may be formed on the other surface 10A.
Further, as shown in the drawing, a rectangular wing plate 16 is attached directly below the hole 12. Since the wing plate 16 is attached, the electrolytic solution can be easily injected appropriately from the holes 12 into the resin film 10. The wing plate 16 is preferably attached to any of the holes 12 on the two surfaces 10A, but may have a structure attached to either one.

＜樹脂フィルムの組成＞
樹脂フィルム１０の材料は、捲回電極体と電池ケースとを適切に絶縁することができる材料であれば特に限定されない。具体的には、例えば、ポリエチレンテレフタレート（ＰＥＴ）、ポリプロピレン（ＰＰ）、または、ポリエチレン（ＰＥ）等の樹脂材料を使用することができる。また、樹脂フィルム１０の厚さは、二次電池１００の構成に合わせて適宜変更すればよいが、例えば、５０〜２００μｍ程度であることが好ましい。 <Composition of resin film>
The material of the resin film 10 is not particularly limited as long as it can appropriately insulate the wound electrode body and the battery case. Specifically, for example, a resin material such as polyethylene terephthalate (PET), polypropylene (PP), or polyethylene (PE) can be used. The thickness of the resin film 10 may be appropriately changed according to the configuration of the secondary battery 100, but is preferably about 50 to 200 μm, for example.

＜二次電池の構築＞
次に、二次電池１００を構築する手順について説明する。
−捲回電極体の作製−
まず、上述する材料および部材を用いて、捲回電極体８０を作製する。捲回電極体８０の作製方法自体は従来と同様であり、本発明を特徴付けるものではないため、詳細な記載は省略する。
−導電性物質の充填−
次に、正負極のいずれか少なくとも一方の極側の集電体露出部５２ａ（６２ａ）が積層された部分の少なくとも集電端子接合部Ｍ１（Ｍ２）を含む領域において、積層する各集電体間に導電性物質を充填する。導電性物質の充填方法としては、例えば、上述する材料を含む導電性合材を、所定部分に流し込み、硬化する方法が挙げられる。あるいは、例えば、市販の導電性接着剤（セメダイン株式会社製の低温硬化形フレキシブル導電性接着剤「ＳＸ−ＥＣＡシリーズ」等）を使用する充填方法を採用することもできる。 <Construction of secondary battery>
Next, the procedure for constructing the secondary battery 100 will be described.
-Manufacturing of wound electrode body-
First, the wound electrode body 80 is manufactured using the above-mentioned materials and members. Since the method for producing the wound electrode body 80 itself is the same as the conventional one and does not characterize the present invention, detailed description thereof will be omitted.
-Filling with conductive material-
Next, in the region including at least the current collector terminal joint M1 (M2) of the portion where the current collector exposed portions 52a (62a) on the pole side of at least one of the positive and negative electrodes are laminated, each current collector to be laminated A conductive substance is filled in between. Examples of the method for filling the conductive substance include a method in which a conductive mixture containing the above-mentioned materials is poured into a predetermined portion and cured. Alternatively, for example, a filling method using a commercially available conductive adhesive (such as the low temperature curable flexible conductive adhesive "SX-ECA series" manufactured by Cemedine Co., Ltd.) can be adopted.

−集電端子および集電体露出部の接合−
次に、集電端子および集電体露出部を接合する。正極については、正極集電端子９２および正極集電体露出部５２ａを接合する。負極については、負極集電端子９４および負極集電体露出部６２ａを接合する。接合方法としては、例えば、超音波溶接、抵抗溶接等の従来公知の接合方法を特に制限なく使用することができる。 -Joining of current collector terminal and exposed part of current collector-
Next, the current collector terminal and the exposed part of the current collector are joined. For the positive electrode, the positive electrode current collector terminal 92 and the positive electrode current collector exposed portion 52a are joined. For the negative electrode, the negative electrode current collector terminal 94 and the negative electrode current collector exposed portion 62a are joined. As the bonding method, for example, conventionally known bonding methods such as ultrasonic welding and resistance welding can be used without particular limitation.

−捲回電極体の収容−
次に、集電端子が接合された捲回電極体８０を樹脂フィルム１０の内部に収容し、これを電池ケース本体２２の内部に収容する。そして、電池ケース本体２２の上端開口部を蓋体２４によって塞ぎ、電池ケース本体２２と蓋体２４との合わせ目を、例えばレーザー溶接法によって接合する。
その後、樹脂フィルム１０と電池ケース２０の内壁とを接合する。具体的には、例えば、電池ケース２０の幅広面に外側から荷重を加えながら、該電池ケース２０を加熱することによって接合する。例えば、電池ケース２０の幅広面を外側から一対の拘束板で挟み込み、冶具を取り付けて、所定の荷重が加わるように拘束する。そして、この状態のまま、例えば、１００℃以上の恒温槽内に１時間以上（例えば、１〜５時間程度）放置する。 -Accommodation of wound electrode body-
Next, the wound electrode body 80 to which the current collecting terminals are joined is housed inside the resin film 10, and this is housed inside the battery case body 22. Then, the upper end opening of the battery case main body 22 is closed by the lid body 24, and the joint between the battery case main body 22 and the lid body 24 is joined by, for example, a laser welding method.
After that, the resin film 10 and the inner wall of the battery case 20 are joined. Specifically, for example, the battery case 20 is joined by heating the wide surface of the battery case 20 while applying a load from the outside. For example, the wide surface of the battery case 20 is sandwiched between a pair of restraint plates from the outside, a jig is attached, and the battery case 20 is restrained so that a predetermined load is applied. Then, in this state, for example, it is left in a constant temperature bath at 100 ° C. or higher for 1 hour or longer (for example, about 1 to 5 hours).

そして、電池ケース内に電解液を注液した後、公知の方法に従って所定の条件で初期充電処理、エージング処理を施す。これによって、使用可能状態の二次電池１００がされる。 Then, after injecting the electrolytic solution into the battery case, the initial charging process and the aging process are performed under predetermined conditions according to a known method. As a result, the secondary battery 100 in a usable state is created.

ここで開示される二次電池は、捲回電極体の集電体露出部が積層された部分の少なくとも上記集電端子接合部を含む領域において、各集電体間に導電性物質が充填されている。これによって、集電端子および集電体露出部の接合によって生じ得る、集電体露出部の積層厚みの不均一性の発生を抑制することができる。したがって、本構成の二次電池によると、捲回電極体における電解液の含浸量に部位ごとのムラが生じるのを防止することができる。
また、ここで開示される二次電池は、上述する構成の樹脂フィルムを備える。これによって、樹脂フィルム内に適当に電解液が注液される。また、樹脂フィルム外に漏出した電解液が樹脂フィルム内に入る。これによって、捲回電極体への電解液の含浸量を増やすことができる。
したがって、捲回電極体において電荷担体由来の物質が生成されるのを防止して二次電池の電池性能を向上させることができる。 In the secondary battery disclosed here, a conductive substance is filled between the current collectors in a region including at least the current collector terminal joint portion of the portion where the current collector exposed portions of the wound electrode body are laminated. ing. As a result, it is possible to suppress the occurrence of non-uniformity of the laminated thickness of the current collector exposed portion, which may occur due to the joining of the current collector terminal and the current collector exposed portion. Therefore, according to the secondary battery having this configuration, it is possible to prevent the impregnation amount of the electrolytic solution in the wound electrode body from being uneven at each site.
Further, the secondary battery disclosed here includes a resin film having the above-described configuration. As a result, the electrolytic solution is appropriately injected into the resin film. Further, the electrolytic solution leaked out of the resin film enters the resin film. As a result, the amount of the electrolytic solution impregnated into the wound electrode body can be increased.
Therefore, it is possible to prevent the charge carrier-derived substance from being generated in the wound electrode body and improve the battery performance of the secondary battery.

１０ 樹脂フィルム
１０Ａ 面
１２ 孔
１４ 孔
１６ 羽板
２０ 電池ケース
２２ 電池ケース本体
２４ 蓋体
２６ 安全弁
２８ 注液孔
３０ 導電性物質
４２ 正極端子
４４ 負極端子
５０ 正極
５２ 正極集電体
５２ａ 正極集電体露出部
５４ 正極活物質層
６０ 負極
６２ 負極集電体
６２ａ 負極集電体露出部
６４ 負極活物質層
７０ セパレータ
８０ 捲回電極体
９２ 正極集電端子
９４ 負極集電端子
１００ 二次電池
Ｗ１ 積層厚み
Ｗ２ 積層厚み
Ｍ１ 正極集電端子接合部
Ｍ２ 負極集電端子接合部
Ｘ 幅方向
Ｙ 長手方向
10 Resin film 10A Surface 12 Hole 14 Hole 16 Feather plate 20 Battery case 22 Battery case body 24 Lid body 26 Safety valve 28 Liquid injection hole 30 Conductive substance 42 Positive electrode terminal 44 Negative electrode terminal 50 Positive electrode 52 Positive electrode current collector 52a Positive electrode current collector Exposed part 54 Positive electrode active material layer 60 Negative electrode 62 Negative electrode current collector 62a Negative electrode current collector Exposed part 64 Negative electrode active material layer 70 Separator 80 Winding electrode body 92 Positive electrode current collecting terminal 94 Negative electrode current collecting terminal 100 Secondary battery W1 Stacked thickness W2 Laminated thickness M1 Positive electrode current collecting terminal joint M2 Negative electrode current collecting terminal joint X Width direction Y Longitudinal direction

Claims (1)

長尺なシート状の正極集電体に正極活物質層が形成された長尺なシート状の正極および長尺なシート状の負極集電体に負極活物質層が形成された長尺なシート状の負極が、セパレータを介在させつつ積層され、長手方向に捲回された構造の捲回電極体と、
前記捲回電極体を電解液とともに収容する電池ケースと、
前記電池ケース内に少なくとも一部が配置され、前記捲回電極体の正極および負極にそれぞれ接続された正極集電端子および負極集電端子と、
を備えた二次電池であって、
前記捲回電極体のシート長手方向に直交する幅方向における一方の端部には、前記正極活物質層を有しないで前記正極集電体が露出した正極集電体露出部が積層されており、該積層された部分の一部には、前記正極集電端子が接合された正極集電端子接合部が形成されており、
前記幅方向における他方の端部には、前記負極活物質層を有しないで前記負極集電体が露出した負極集電体露出部が積層されており、該積層された部分の一部には、前記負極集電端子が接合された負極集電端子接合部が形成されており、
ここで正負極のいずれか少なくとも一方の極側の前記集電体露出部が積層された部分の少なくとも前記集電端子接合部を含む領域において導電性物質が積層する各集電体間に充填されていることを特徴とする、二次電池。 A long sheet-shaped positive electrode in which a positive electrode active material layer is formed on a long sheet-shaped positive electrode current collector, and a long sheet in which a negative electrode active material layer is formed on a long sheet-shaped negative electrode current collector. A wound electrode body having a structure in which the shaped negative electrodes are laminated with a separator interposed therebetween and wound in the longitudinal direction.
A battery case that houses the wound electrode body together with the electrolytic solution, and
A positive electrode current collecting terminal and a negative electrode current collecting terminal, respectively, which are arranged in the battery case and connected to the positive electrode and the negative electrode of the wound electrode body,
It is a secondary battery equipped with
A positive electrode current collector exposed portion which does not have the positive electrode active material layer and the positive electrode current collector is exposed is laminated on one end of the wound electrode body in the width direction orthogonal to the sheet longitudinal direction. A positive electrode current collecting terminal joint portion to which the positive electrode current collecting terminal is joined is formed in a part of the laminated portion.
A negative electrode current collector exposed portion in which the negative electrode current collector is exposed without having the negative electrode active material layer is laminated on the other end portion in the width direction, and a part of the laminated portion is laminated. , The negative electrode current collecting terminal joint portion to which the negative electrode current collecting terminal is joined is formed.
Here, it is filled between each current collector in which the conductive substance is laminated in the region including at least the current collector terminal joint portion of the portion where the current collector exposed portion on the pole side of at least one of the positive and negative electrodes is laminated. A secondary battery characterized by being
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JP7479104B1 (en) 2023-05-16 2024-05-08 ＴｅｒａＷａｔｔ Ｔｅｃｈｎｏｌｏｇｙ株式会社 Electrode sheet and secondary battery

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