JP5487895B2 - Current collector and manufacturing method thereof - Google Patents

Current collector and manufacturing method thereof Download PDF

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JP5487895B2
JP5487895B2 JP2009261488A JP2009261488A JP5487895B2 JP 5487895 B2 JP5487895 B2 JP 5487895B2 JP 2009261488 A JP2009261488 A JP 2009261488A JP 2009261488 A JP2009261488 A JP 2009261488A JP 5487895 B2 JP5487895 B2 JP 5487895B2
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current collector
collector foil
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positive electrode
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JP2011108469A (en
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浩二 川本
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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

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本発明は、集電体及びその製造方法に関し、特に、互いに接続された２以上の集電部を備える集電体及びその製造方法に関する。   The present invention relates to a current collector and a method for manufacturing the current collector, and more particularly to a current collector including two or more current collectors connected to each other and a method for manufacturing the current collector.

リチウムイオン二次電池は、他の二次電池よりもエネルギー密度が高く、高電圧での動作が可能という特徴を有している。そのため、小型軽量化を図りやすい二次電池として携帯電話等の情報機器に使用されており、近年、電気自動車やハイブリッド自動車用等、大型の動力用としての需要も高まっている。   A lithium ion secondary battery has the characteristics that it has a higher energy density than other secondary batteries and can operate at a high voltage. For this reason, it is used as a secondary battery that can be easily reduced in size and weight in information equipment such as a mobile phone, and in recent years, there is an increasing demand for large motive power such as for electric vehicles and hybrid vehicles.

リチウムイオン二次電池には、正極層及び負極層と、これらの間に配置される電解質とが備えられ、電解質は、非水系の液体又は固体によって構成される。電解質に非水系の液体（以下において、「電解液」という。）が用いられる場合には、電解液が正極層の内部へと浸透する。そのため、正極層を構成する正極活物質と電解質との界面が形成されやすく、性能を向上させやすい。ところが、広く用いられている電解液は可燃性であるため、安全性を確保するためのシステムを搭載する必要がある。一方、固体の電解質は不燃性であるため、上記システムを簡素化できる。それゆえ、不燃性である固体の電解質を含有する層（以下において、「固体電解質層」ということがある。）が備えられる形態のリチウムイオン二次電池（以下において、「固体電池」という。）が提案されている。   The lithium ion secondary battery includes a positive electrode layer and a negative electrode layer, and an electrolyte disposed between the positive electrode layer and the negative electrode layer, and the electrolyte is composed of a non-aqueous liquid or solid. When a non-aqueous liquid (hereinafter referred to as “electrolytic solution”) is used as the electrolyte, the electrolytic solution penetrates into the positive electrode layer. Therefore, the interface between the positive electrode active material constituting the positive electrode layer and the electrolyte is easily formed, and the performance is easily improved. However, since the widely used electrolyte is flammable, it is necessary to mount a system for ensuring safety. On the other hand, since the solid electrolyte is nonflammable, the above system can be simplified. Therefore, a lithium ion secondary battery (hereinafter, referred to as “solid battery”) having a layer containing a non-combustible solid electrolyte (hereinafter, sometimes referred to as “solid electrolyte layer”). Has been proposed.

このような固体電池に関する技術として、例えば特許文献１には、正極基板の短尺方向の一方端部全体に正極リード部を有する正極と、負極基板の短尺方向の一方端部全体に負極リード部を有する負極と、正極と負極との間に介在される固体電解質層とを有する電池素子を備え、正極リード部及び負極リード部が各電極の長尺方向に亘る全域で外部と電気的に接続されている電池が開示されている。そして、特許文献１には、箔状、網状、多孔状等を呈する金属によって構成される正極基板及び負極基板が開示されており、正極リード部及び負極リード部を押し潰した後にレーザ溶接、超音波溶接、抵抗溶接、アーク溶接等によって正極リード部及び負極リード部を電気的に接合する形態や、さらに接続部材を用いて正極リード部及び負極リード部の接続信頼性を向上させる形態についても開示されている。   As a technology related to such a solid battery, for example, Patent Document 1 discloses that a positive electrode having a positive electrode lead portion at one end portion in the short direction of the positive electrode substrate and a negative electrode lead portion at one end portion in the short direction of the negative electrode substrate. A battery element having a negative electrode having a solid electrolyte layer interposed between the positive electrode and the negative electrode, and the positive electrode lead portion and the negative electrode lead portion are electrically connected to the outside over the entire length of each electrode. A battery is disclosed. Patent Document 1 discloses a positive electrode substrate and a negative electrode substrate made of a metal having a foil shape, a net shape, a porous shape, and the like. After crushing the positive electrode lead portion and the negative electrode lead portion, laser welding, Also disclosed is a mode in which the positive electrode lead portion and the negative electrode lead portion are electrically joined by sonic welding, resistance welding, arc welding, etc., and a mode in which the connection reliability of the positive electrode lead portion and the negative electrode lead portion is improved by using a connecting member. Has been.

特開２００３−１８７７８１号公報JP 2003-188771 A

特許文献１に開示されている技術では、溶接することによって正極リード部と負極リード部とを接合しているので、正極リード部と負極リード部との接合部における電気抵抗の増大を抑制することが可能になると考えられる。しかしながら、金属箔等に代表される厚さが薄い金属部材同士を単に溶接すると、溶接された金属部材に皺等が生じやすく、金属部材間の接合強度にばらつきが生じる結果、接合界面の電気抵抗が増大しやすいという問題があった。   In the technique disclosed in Patent Document 1, since the positive electrode lead portion and the negative electrode lead portion are joined by welding, an increase in electrical resistance at the joint portion between the positive electrode lead portion and the negative electrode lead portion is suppressed. Will be possible. However, if metal members such as metal foils are simply welded together, the welded metal members are likely to wrinkle, resulting in variations in the bonding strength between the metal members. There was a problem that it was easy to increase.

そこで本発明は、接合界面の電気抵抗を低減することが可能な集電体及びその製造方法を提供することを課題とする。   Then, this invention makes it a subject to provide the electrical power collector which can reduce the electrical resistance of a joining interface, and its manufacturing method.

上記課題を解決するために、本発明は以下の手段をとる。すなわち、
本発明の第１の態様は、一対の集電箔を備え、該一対の集電箔のうち少なくとも一方の集電箔は凹部を有し、該凹部に他方の集電箔の一部を配設させることによって一対の集電箔が接続されていることを特徴とする、集電体である。 In order to solve the above problems, the present invention takes the following means. That is,
A first aspect of the present invention includes a pair of current collector foils, and at least one of the pair of current collector foils has a recess, and a part of the other current collector foil is disposed in the recess. A current collector is characterized in that a pair of current collector foils are connected to each other.

ここに、本発明において、「凹部」とは、集電箔を貫通する孔であっても良く、集電箔を貫通しない穴であっても良い。また、「少なくとも一方の集電箔は凹部を有し」とは、一方の集電箔のみが凹部を有する形態に加え、一対の集電箔のそれぞれが凹部を有する形態も含まれることをいう。また、「凹部に他方の集電箔の一部を配設させることによって一対の集電箔が接続されている」とは、一方の集電箔のみが凹部を有する場合には、一方の集電箔の凹部に他方の集電箔の一部を配設させることによって一対の集電箔が接続されていることをいう。これに対し、一対の集電箔（以下において、「第１集電箔」、「第２集電箔」ということがある。）それぞれが凹部を有する場合には、第１集電箔の凹部に第２集電箔の一部を配設させることによって第１集電箔及び第２集電箔が接続されている形態や、第２集電箔の凹部に第１集電箔の一部を配設させることによって第１集電箔及び第２集電箔が接続されている形態に加えて、第１集電箔の凹部に第２集電箔の一部を配設させ且つ第２集電箔の凹部に第１集電箔の一部を配設させることによって第１集電箔及び第２集電箔が接続されている形態も含まれる。   Here, in the present invention, the “concave portion” may be a hole penetrating the current collector foil or a hole not penetrating the current collector foil. Further, “at least one current collector foil has a concave portion” means that not only one of the current collector foils has a concave portion, but also a form in which each of the pair of current collector foils has a concave portion is included. . In addition, “a pair of current collector foils are connected by disposing a part of the other current collector foil in the concave portion” means that only one current collector foil has a concave portion. It means that a pair of current collector foils are connected by disposing a part of the other current collector foil in the concave portion of the current foil. On the other hand, when each of the pair of current collector foils (hereinafter sometimes referred to as “first current collector foil” and “second current collector foil”) has a concave portion, the concave portion of the first current collector foil The first current collector foil and the second current collector foil are connected to each other by arranging a part of the second current collector foil, or a part of the first current collector foil is provided in the concave portion of the second current collector foil. In addition to the form in which the first current collector foil and the second current collector foil are connected to each other, a part of the second current collector foil is disposed in the recess of the first current collector foil and the second current collector foil is disposed. A mode in which the first current collector foil and the second current collector foil are connected by disposing a part of the first current collector foil in the concave portion of the current collector foil is also included.

本発明の第２の態様は、少なくとも一方の集電箔に凹部が備えられる一対の集電箔を用意する準備工程と、該準備工程で用意された一対の集電箔を接触させる接触工程と、該接触工程で接触させた一対の集電箔のうち、凹部と対向している集電箔の一部を溶解させ、溶解させた集電箔の一部を凹部へと流入させる過程を経て、一対の集電箔を接続する接続工程と、を有することを特徴とする、集電体の製造方法である。   According to a second aspect of the present invention, a preparation step of preparing a pair of current collector foils provided with a recess in at least one current collector foil, and a contact step of contacting the pair of current collector foils prepared in the preparation step; , Among the pair of current collector foils contacted in the contact step, through a process of dissolving a part of the current collector foil facing the concave part and flowing a part of the dissolved current collector foil into the concave part And a connecting step of connecting a pair of current collector foils.

ここに、本発明の「準備工程」は、一方の集電箔にのみ凹部が備えられる一対の集電箔、又は、それぞれの集電箔に凹部が備えられる一対の集電箔を用意する工程である。また、本発明の「接触工程」は、続く接続工程で、溶解させた集電箔を凹部へと流入させることが可能なように、準備工程で用意した一対の集電箔を接触させる工程である。すなわち、一方の集電箔（第１集電箔）にのみ凹部が備えられ他方の集電箔（第２集電箔）は凹部を有しない場合、本発明の接触工程は、第１集電箔の凹部と第２集電箔の一部とが対向する形態で第１集電箔及び第２集電箔を接触させる工程である。この場合、本発明の接続工程では、第１集電箔の凹部と対向している第２集電箔の一部を溶解させ、溶解させた第２集電箔の一部を第１集電箔の凹部へと流入させる過程を経て、第１集電箔及び第２集電箔が接続される。これに対し、一対の集電箔それぞれに凹部が備えられる場合、本発明の接触工程は、例えば、第１集電箔の凹部と第２集電箔の凹部以外の一部とが対向し且つ第２集電箔の凹部と第１集電箔の凹部以外の一部とが対向する形態で、第１集電箔及び第２集電箔を接触させる工程である。この場合、本発明の接続工程では、第１集電箔の凹部と対向している第２集電箔の一部を溶解させ、溶解させた第２集電箔の一部を第１集電箔の凹部へと流入させるのに加えて、第２集電箔の凹部と対向している第１集電箔の一部を溶解させ、溶解させた第１集電箔の一部を第２集電箔の凹部へと流入させる過程を経て、第１集電箔及び第２集電箔が接続される。   Here, the “preparation step” of the present invention is a step of preparing a pair of current collector foils provided with a concave portion only on one current collector foil, or a pair of current collector foils provided with a concave portion on each current collector foil. It is. In addition, the “contact process” of the present invention is a process in which a pair of current collector foils prepared in the preparation process are brought into contact so that the melted current collector foil can flow into the recesses in the subsequent connection process. is there. That is, when a concave portion is provided only in one current collector foil (first current collector foil) and the other current collector foil (second current collector foil) does not have a concave portion, the contact step of the present invention is performed by the first current collector foil. This is a step of bringing the first current collector foil and the second current collector foil into contact with each other in a form in which the concave portion of the foil faces a part of the second current collector foil. In this case, in the connecting step of the present invention, a part of the second current collector foil facing the concave portion of the first current collector foil is dissolved, and a part of the dissolved second current collector foil is used as the first current collector. The first current collector foil and the second current collector foil are connected through a process of flowing into the concave portion of the foil. On the other hand, when each of the pair of current collector foils is provided with a recess, the contact step of the present invention is such that, for example, the recess of the first current collector foil and a part other than the recess of the second current collector foil face each other. This is a step of bringing the first current collector foil and the second current collector foil into contact with each other in a form in which the concave portion of the second current collector foil and a part other than the concave portion of the first current collector foil face each other. In this case, in the connecting step of the present invention, a part of the second current collector foil facing the concave portion of the first current collector foil is dissolved, and a part of the dissolved second current collector foil is used as the first current collector. In addition to flowing into the recess of the foil, a part of the first current collector foil facing the recess of the second current collector foil is dissolved, and a part of the dissolved first current collector foil is second The first current collector foil and the second current collector foil are connected through a process of flowing into the concave portion of the current collector foil.

本発明の第１の態様にかかる集電体では、一方の集電箔の凹部に他方の集電箔の一部を配設させることによって、一対の集電箔が接続されている。かかる形態とすることにより、集電箔に皺を発生させることなく、一対の集電箔の接続部位を一様且つ強固に密着させることが可能になる。したがって、本発明の第１の態様によれば、一対の集電箔の接合界面における電気抵抗を低減することが可能な、集電体を提供することができる。   In the current collector according to the first aspect of the present invention, a pair of current collector foils are connected by disposing a part of the other current collector foil in the concave portion of one current collector foil. By setting it as this form, it becomes possible to make the connection part of a pair of current collector foil contact | adhere uniformly and firmly, without generating a wrinkle in current collector foil. Therefore, according to the 1st aspect of this invention, the electrical power collector which can reduce the electrical resistance in the joining interface of a pair of electrical power collector foil can be provided.

本発明の第２の態様にかかる集電体の製造方法は、凹部と対向している集電箔の一部を溶解させ、溶解させた集電箔の一部を凹部へと流入させる過程を経て、一対の集電箔を接続する接続工程を有しているので、本発明の第１の態様にかかる集電体を製造することが可能になる。したがって、本発明の第２の態様によれば、一対の集電箔の接合界面における電気抵抗を低減し得る集電体を製造することが可能な、集電体の製造方法を提供することができる。   The current collector manufacturing method according to the second aspect of the present invention includes a process of dissolving a part of the current collector foil facing the concave part and causing the part of the dissolved current collector foil to flow into the concave part. Then, since it has the connection process which connects a pair of current collection foil, it becomes possible to manufacture the electrical power collector concerning the 1st aspect of this invention. Therefore, according to the second aspect of the present invention, it is possible to provide a current collector manufacturing method capable of manufacturing a current collector capable of reducing the electrical resistance at the bonding interface between a pair of current collector foils. it can.

本発明の集電体１を説明する図である。図１（ａ）は集電体１を示す正面図であり、図１（ｂ）は集電箔２を示す上面図である。It is a figure explaining the electrical power collector 1 of this invention. FIG. 1A is a front view showing the current collector 1, and FIG. 1B is a top view showing the current collector foil 2. 集電体１を含む構造体４を示す断面図である。2 is a cross-sectional view showing a structure 4 including a current collector 1. FIG. 構造体４を含む積層体８を示す上面図である。FIG. 6 is a top view showing a stacked body 8 including a structure 4. 積層体８を示す断面図である。3 is a cross-sectional view showing a laminated body 8. FIG. 固体電池１０の形態を簡略化して示す図である。1 is a diagram showing a simplified form of a solid battery 10. FIG. 本発明の集電体の製造方法を説明するフローチャートである。It is a flowchart explaining the manufacturing method of the electrical power collector of this invention.

正極層及び負極層を有する複数の単電池を電気的に接続する際、正極層の環境及び負極層の環境の両方において電気化学的に安定な材料が存在しない場合には、例えば、正極層に接続された集電箔をアルミニウム製とし負極層に接続された集電箔を銅製とする等、正極層側の集電箔と負極層側の集電箔とをそれぞれ異なる材料で構成する必要がある。ところが、異なる材料を、電気抵抗を十分に低減し得る形態で直接接続することは困難であった。そのため、これまでは、一方の極の環境に耐え得る材料によって構成される集電箔の表面に他方の極の環境に耐え得る材料を被覆した被覆材、又は、クラッド材を用いて金属同士を溶接することにより接続したり、接続用の板及びボルト・ナット等の接続部材を用いて接続したりしていた。しかしながら、被覆材を用いると、ピンホールが存在する場合やプレス工程で表面が剥離した場合、更には集電箔の端部を切り出した際に母材が剥き出しとなって電気化学的な安定性を維持することが困難となり、結果として初期容量低下や耐久性低下の原因になりやすい。また、クラッド材は、材料毎に塑性変形の程度が異なるため薄膜化することが困難であり、電池のエネルギー密度を向上させ難いほか、被覆材やクラッド材はコスト増を招きやすいという特徴がある。一方、接続部材を用いるとコスト増を招きやすく、製造工程数も増大しやすいという特徴がある。そのため、コスト及び製造工程数の増大を抑制し、且つ、性能を向上させることが可能な、集電箔の接続方法及びそのような方法で接続された複数の集電箔を備えた集電体の開発が求められていた。   When electrically connecting a plurality of unit cells having a positive electrode layer and a negative electrode layer, if there is no electrochemically stable material in both the positive electrode layer environment and the negative electrode layer environment, for example, the positive electrode layer The current collector foil on the positive electrode layer side and the current collector foil on the negative electrode layer side need to be composed of different materials, such as the connected current collector foil made of aluminum and the current collector foil connected to the negative electrode layer made of copper, etc. is there. However, it has been difficult to directly connect different materials in a form that can sufficiently reduce electrical resistance. For this reason, until now, the surface of the current collector foil made of a material that can withstand the environment of one pole is covered with a coating material that is coated with a material that can withstand the environment of the other pole, or a metal clad with a clad material. They are connected by welding or connected using connecting members such as connecting plates and bolts and nuts. However, when a coating material is used, if there is a pinhole or if the surface is peeled off during the pressing process, or when the edge of the current collector foil is cut out, the base material is exposed and electrochemical stability As a result, it tends to cause a decrease in initial capacity and durability. In addition, it is difficult to reduce the thickness of the clad material because the degree of plastic deformation differs depending on the material, and it is difficult to improve the energy density of the battery. In addition, the cladding material and the clad material tend to increase costs . On the other hand, the use of a connection member is characterized in that the cost is likely to increase and the number of manufacturing steps is likely to increase. Therefore, it is possible to suppress an increase in cost and the number of manufacturing steps and improve performance, and a current collector including a current collector foil connection method and a plurality of current collector foils connected by such a method The development of was demanded.

本発明者は、電気化学的な安定性を担保し性能向上を実現するために、正極層側及び負極層側で、それぞれ電気化学的に安定な集電箔を使用することが必要であると考えた。そして、鋭意研究の結果、正極層側の集電箔と負極層側の集電箔とを容易に直接溶接するために、例えば、一方の集電箔に凹部（例えば、貫通孔）が備えられる形態とし、他方の集電箔と密着させて溶接し他方の集電箔のみを溶解させることにより、アンカー効果によって一対の集電箔を強固に密着させ一体化させることが可能になることを知見した。かかる形態で一体化させることにより、一対の集電箔間の電気抵抗を低減することが可能になる。本発明は、上記知見に基づいてなされたものである。   The present inventor said that it is necessary to use an electrochemically stable current collector foil on each of the positive electrode layer side and the negative electrode layer side in order to ensure electrochemical stability and realize performance improvement. Thought. As a result of extensive research, in order to easily and directly weld the current collector foil on the positive electrode layer side and the current collector foil on the negative electrode layer side, for example, one current collector foil is provided with a recess (for example, a through hole). Knowledge that it is possible to make a pair of current collector foils firmly adhere to each other by the anchor effect by welding in contact with the other current collector foil and dissolving only the other current collector foil did. By integrating in this form, it becomes possible to reduce the electrical resistance between a pair of current collector foils. The present invention has been made based on the above findings.

以下、図面を参照しつつ、本発明について説明する。なお、以下に示す形態は本発明の例示であり、本発明は以下に示す形態に限定されるものではない。   The present invention will be described below with reference to the drawings. In addition, the form shown below is an illustration of this invention and this invention is not limited to the form shown below.

図１は、本発明の集電体１を説明する図である。図１（ａ）は集電体１を示す正面図であり、図１（ｂ）は集電箔２を示す上面図である。図１（ｂ）では一部符号の記載を省略している。図１（ａ）に示すように、集電体１は、一対の集電箔２及び集電箔３を接合することによって構成されており、図１（ｂ）に示すように、集電箔２は、複数の貫通孔２ａ、２ａ、…を有している。集電体１は、貫通孔２ａ、２ａ、…を有する集電箔２と、孔を有しない集電箔３とを接触させた後、集電箔３の一部を加熱し溶解させ、溶解した集電箔３の一部を貫通孔２ａ、２ａ、…へと流入させた後で冷却することにより、貫通孔２ａ、２ａ、…に集電箔３の一部が配設された状態で集電箔２と集電箔３とが接続されている。このような形態とすることにより、アンカー効果によって集電箔２及び集電箔３を強固に密着させ一体化させることが可能になる。したがって、本発明によれば、集電箔２及び集電箔３の間における電気抵抗を低減することが可能な、集電体１を提供することができる。   FIG. 1 is a diagram illustrating a current collector 1 of the present invention. FIG. 1A is a front view showing the current collector 1, and FIG. 1B is a top view showing the current collector foil 2. In FIG. 1 (b), some symbols are omitted. As shown to Fig.1 (a), the collector 1 is comprised by joining a pair of collector foil 2 and the collector foil 3, and as shown to FIG.1 (b), collector current foil is comprised. 2 has a plurality of through holes 2a, 2a,. The current collector 1 is made by bringing a current collector foil 2 having through holes 2a, 2a,... And a current collector foil 3 having no holes into contact with each other, and then heating a part of the current collector foil 3 to dissolve it. In such a state that a part of the current collector foil 3 is disposed in the through holes 2a, 2a,... By cooling a part of the collected current foil 3 into the through holes 2a, 2a,. The current collector foil 2 and the current collector foil 3 are connected. By adopting such a form, the current collector foil 2 and the current collector foil 3 can be firmly adhered and integrated by the anchor effect. Therefore, according to this invention, the electrical power collector 1 which can reduce the electrical resistance between the collector foil 2 and the collector foil 3 can be provided.

図２は、固体電池の一部を構成する、集電体１を含む構造体４を示す断面図である。図２に示すように、集電体１の構成要素である集電箔２は、固体電池の正極層５、５に接続されており、集電体１の構成要素である集電箔３は、固体電池の負極層６、６に接続されている。後述するように、集電箔２に接続されている正極層５、５、及び、集電箔３に接続されている負極層６、６は、それぞれ、隣り合う固体電池（単電池）の構成要素である。すなわち、構造体４の構成要素である集電体１は、隣り合う単電池を電気的に接続する役割を担っている。   FIG. 2 is a cross-sectional view showing the structure 4 including the current collector 1 that constitutes a part of the solid state battery. As shown in FIG. 2, the current collector foil 2 that is a component of the current collector 1 is connected to the positive electrode layers 5 and 5 of the solid battery, and the current collector foil 3 that is a component of the current collector 1 is Are connected to the negative electrode layers 6 and 6 of the solid state battery. As will be described later, the positive electrode layers 5, 5 connected to the current collector foil 2 and the negative electrode layers 6, 6 connected to the current collector foil 3 are respectively composed of adjacent solid batteries (unit cells). Is an element. That is, the current collector 1 that is a constituent element of the structure 4 plays a role of electrically connecting adjacent unit cells.

図３は、構造体４を含む積層体８を簡略化して示す上面図であり、積層体８の一部のみを示している。構造体４及び固体電解質層７の配置を理解しやすくするため、図３では、積層される構造体４、４、…及び固体電解質層７、７、…を上下にずらして示している。図４は、積層体８の一部を示す断面図である。図４では、一部符号の記載を省略している。図３及び図４に示すように、積層体８は、固体電解質層７、７、…と構造体４、４、…とを交互に積層することによって構成され、固体電解質層７を挟んで上下に配設される構造体４、４は、一方の積層体４に備えられる正極層５と他方の積層体４に備えられる負極層６との間に固体電解質層７が配設されるように、積層されている。かかる形態で構造体４、４、…及び固体電解質層７、７、…を積層することにより、固体電解質層７とこれを狭持する一対の正極層５及び負極層６によって構成される複数の単電池を、集電体１を介して電気的に接続することが可能になる。図３及び図４に示す積層体８は、固体電池の構成要素であり、積層体８を図３の上下方向に捲回した後、プレス機を用いてプレスする工程等を経ることにより、後述する固体電池の電極体を作製することができる。   FIG. 3 is a top view schematically showing the stacked body 8 including the structure 4, and shows only a part of the stacked body 8. In order to facilitate understanding of the arrangement of the structure 4 and the solid electrolyte layer 7, the stacked structures 4, 4,... And the solid electrolyte layers 7, 7,. FIG. 4 is a cross-sectional view showing a part of the laminate 8. In FIG. 4, some reference numerals are omitted. As shown in FIGS. 3 and 4, the laminate 8 is configured by alternately laminating the solid electrolyte layers 7, 7,... And the structures 4, 4,. In the structures 4, 4 disposed in the structure, the solid electrolyte layer 7 is disposed between the positive electrode layer 5 provided in one stacked body 4 and the negative electrode layer 6 provided in the other stacked body 4. Are stacked. In such a form, by laminating the structures 4, 4,... And the solid electrolyte layers 7, 7,..., A plurality of solid electrolyte layers 7 and a plurality of positive electrode layers 5 and negative electrode layers 6 sandwiching the solid electrolyte layers 7 are provided. The battery cells can be electrically connected via the current collector 1. The laminated body 8 shown in FIGS. 3 and 4 is a constituent element of a solid battery, and after the laminated body 8 is wound in the vertical direction of FIG. Thus, an electrode body of a solid battery can be produced.

図５は、固体電池１０の形態を簡略化して示す図である。図５に示すように、固体電池１０は、積層体８を捲回することによって構成される電極体９、９、…と、隣り合う電極体９、９、…を接続する端子１１、１１、…と、端子１１、１１、…を介して接続された複数の電極体９、９、…の一端側の端子１１ａに接続された正極端子１２及び他端側の端子１１ｂに接続された負極端子１３と、端子１１、１１、…を介して接続された複数の電極体９、９、…を収容する筐体１４と、を有している。上述のように、固体電池１０の電極体９、９、…には複数の集電体１、１、…が備えられている。すなわち、固体電池１０は、複数の単電池が集電体１、１、…を介して電気的に接続されているので、単電池間の電気抵抗を低減することが可能になる。したがって、集電体１、１、…が備えられる形態とすることにより、性能を向上させることが可能な固体電池１０を提供することができる。   FIG. 5 is a diagram showing a simplified form of the solid state battery 10. As shown in FIG. 5, the solid battery 10 includes electrodes 11, 9,... Configured by winding the laminated body 8, and terminals 11, 11, which connect the adjacent electrode bodies 9, 9,. ... and a negative terminal connected to a terminal 11a on one end side and a terminal 11b on the other end side of a plurality of electrode bodies 9, 9, ... connected via terminals 11, 11, ... 13 and a housing 14 that houses a plurality of electrode bodies 9, 9,... Connected via terminals 11, 11,. As described above, the electrode bodies 9, 9,... Of the solid battery 10 are provided with a plurality of current collectors 1, 1,. That is, in the solid battery 10, since a plurality of single cells are electrically connected via the current collectors 1, 1,..., It is possible to reduce the electrical resistance between the single cells. Therefore, the solid battery 10 capable of improving the performance can be provided by providing the current collectors 1, 1,.

図６は、本発明の集電体の製造方法を説明するフローチャートである。図６に示すように、本発明の集電体の製造方法は、準備工程（工程Ｓ１）と、接触工程（工程Ｓ２）と、接続工程（工程Ｓ３）とを有し、工程Ｓ１〜工程Ｓ３を経て、集電体１が製造される。以下、工程毎に説明する。   FIG. 6 is a flowchart illustrating a method for manufacturing a current collector of the present invention. As shown in FIG. 6, the method for manufacturing a current collector of the present invention includes a preparation step (step S1), a contact step (step S2), and a connection step (step S3), and includes steps S1 to S3. Then, the current collector 1 is manufactured. Hereinafter, it demonstrates for every process.

工程Ｓ１は、少なくとも一方の集電箔に凹部が備えられる一対の集電箔を用意する工程である。集電体１を製造する場合、工程Ｓ１は、例えば、貫通孔を有しない集電箔２’及び集電箔３を用意した後、集電箔２’に貫通孔２ａ、２ａ、…を形成することにより、貫通孔２ａ、２ａ、…を有する集電箔２と、貫通孔を有しない集電箔３とを用意する工程、とすることができる。本発明において、集電箔２及び集電箔３の厚さは数μｍ〜数十μｍとすることができる。また、貫通孔２ａの孔径は、特に限定されるものではないが、一対の集電箔を強固に密着可能にする等の観点から、孔径は数百μｍ以上とすることが好ましく、接続後に集電箔に皺が形成され難い形態にする等の観点から、孔径は数ｍｍ以下とすることが好ましい。孔径は、例えば、６００μｍ以上９ｍｍ以下とすることが好ましい。また、隣り合う貫通孔２ａ、２ａの間隔は、特に限定されるものではなく、例えば、３ｍｍとすることができる。本発明において、集電箔２は、例えばアルミニウム箔とすることができ、集電箔３は、例えば銅箔とすることができる。   Step S1 is a step of preparing a pair of current collector foils in which at least one current collector foil is provided with a recess. When manufacturing the current collector 1, for example, in step S <b> 1, the current collector foil 2 ′ and the current collector foil 3 having no through holes are prepared, and then the through holes 2 a, 2 a,. By doing, it can be set as the process of preparing the current collection foil 2 which has through-hole 2a, 2a, ... and the current collection foil 3 which does not have a through-hole. In the present invention, the thickness of the current collector foil 2 and the current collector foil 3 can be several μm to several tens of μm. Further, the hole diameter of the through hole 2a is not particularly limited, but it is preferable that the hole diameter be several hundred μm or more from the viewpoint of making it possible to firmly adhere the pair of current collector foils. From the standpoint of forming a shape in which wrinkles are not easily formed on the electric foil, the hole diameter is preferably several mm or less. The hole diameter is preferably 600 μm or more and 9 mm or less, for example. Moreover, the space | interval of adjacent through-hole 2a, 2a is not specifically limited, For example, it can be 3 mm. In the present invention, the current collector foil 2 can be an aluminum foil, for example, and the current collector foil 3 can be a copper foil, for example.

工程Ｓ２は、上記工程Ｓ１で用意した一対の集電箔を接触させる工程である。集電体１を製造する場合、工程Ｓ２は、すべての貫通孔２ａ、２ａ、…の一端が集電箔３によって覆われる形態で、貫通孔２ａ、２ａ、…を有する集電箔２と、貫通孔を有しない集電箔３とを接触させる工程である。   Step S2 is a step of bringing the pair of current collector foils prepared in step S1 into contact with each other. When the current collector 1 is manufactured, the step S2 includes the current collector foil 2 having the through holes 2a, 2a,... In a form in which one end of all the through holes 2a, 2a,. This is a step of contacting the current collector foil 3 having no through-hole.

工程Ｓ３は、上記工程Ｓ２で接触させた一対の集電箔のうち、凹部と対向している集電箔の一部を溶解させ、溶解させた集電箔の一部を凹部へと流入させる過程を経て、一対の集電箔を接続する工程である。集電体１を製造する場合、工程Ｓ３は、貫通孔２ａ、２ａ、…と対向している集電箔３の部位を溶解させ、溶解させた集電箔３の一部を貫通孔２ａ、２ａ、…へと流入させた後、集電箔２及び集電箔３を空冷することにより、貫通孔２ａ、２ａ、…に集電箔３の一部を配設した状態で集電箔２と集電箔３とを接続する工程（集電箔３の一部を貫通孔２ａ、２ａ、…へと配設することにより集電箔２と集電箔３とを溶接する工程）、とすることができる。本発明において、工程Ｓ３は、集電箔の一部を貫通孔へと配設することにより一対の集電箔を溶接する工程であれば、その形態は特に限定されるものではなく、レーザ溶接、超音波溶接、抵抗溶接、アーク溶接等、各種溶接法を用いることができる。   Step S3 dissolves a part of the current collector foil facing the concave portion out of the pair of current collector foils contacted in Step S2, and causes a part of the dissolved current collector foil to flow into the concave portion. It is a process of connecting a pair of current collector foils through a process. When the current collector 1 is manufactured, the step S3 is performed by dissolving the portion of the current collector foil 3 facing the through holes 2a, 2a,. After flowing into 2a, ..., current collector foil 2 and current collector foil 3 are air-cooled to collect current collector foil 2 in a state where a part of current collector foil 3 is disposed in through holes 2a, 2a, ... And a step of connecting the current collector foil 3 (a step of welding the current collector foil 2 and the current collector foil 3 by disposing a part of the current collector foil 3 to the through holes 2a, 2a,...), And can do. In the present invention, if the step S3 is a step of welding a pair of current collector foils by disposing a part of the current collector foil into the through hole, the form is not particularly limited, and laser welding is performed. Various welding methods such as ultrasonic welding, resistance welding, and arc welding can be used.

このように、工程Ｓ１〜工程Ｓ３を有する本発明の集電体の製造方法によれば、集電体１を製造することができる。したがって、本発明によれば、一対の集電箔２、３の接合界面における電気抵抗を低減し得る集電体１を製造することが可能な、集電体の製造方法を提供することができる。   Thus, according to the manufacturing method of the electrical power collector of this invention which has process S1-process S3, electrical power collector 1 can be manufactured. Therefore, according to this invention, the manufacturing method of the electrical power collector which can manufacture the electrical power collector 1 which can reduce the electrical resistance in the junction interface of a pair of electrical power collector foils 2 and 3 can be provided. .

本発明に関する上記説明では、正極層５に接続される集電箔２のみが貫通孔２ａ、２ａ、…を有し、負極層６に接続される集電箔３は貫通孔を有しない形態を例示したが、本発明は当該形態に限定されるものではなく、負極層に接続される集電箔のみが貫通孔を有し、正極層に接続される集電箔が貫通孔を有しない形態や、接続される一対の集電箔それぞれが貫通孔を有する形態であっても良い。本発明において、接続される一対の集電箔それぞれが貫通孔を有する場合には、一方の集電箔の貫通孔と、他方の集電箔の貫通孔以外の部位とが対向し、且つ、他方の集電箔の貫通孔と、一方の集電箔の貫通孔以外の部位とが対向するように一対の集電箔を接触させた後、それぞれの箇所を溶接すれば良い。   In the above description regarding the present invention, only the current collector foil 2 connected to the positive electrode layer 5 has the through holes 2a, 2a,..., And the current collector foil 3 connected to the negative electrode layer 6 has no through hole. Although illustrated, this invention is not limited to the said form, Only the collector foil connected to a negative electrode layer has a through-hole, and the collector foil connected to a positive electrode layer does not have a through-hole. Alternatively, each of the pair of current collector foils to be connected may have a through hole. In the present invention, when each of the pair of current collector foils to be connected has a through hole, the through hole of one of the current collector foils is opposed to a portion other than the through hole of the other current collector foil, and What is necessary is just to weld each location, after making a pair of current collection foil contact so that the through-hole of the other current collection foil and parts other than the through-hole of one current collection foil may oppose.

また、本発明に関する上記説明では、集電体に備えられる凹部が貫通孔である形態を例示したが、本発明は当該形態に限定されるものではなく、集電箔を貫通しない穴が備えられる形態とすることも可能である。   Moreover, in the said description regarding this invention, although the recessed part with which a collector is equipped was illustrated the form which is a through-hole, this invention is not limited to the said form, The hole which does not penetrate a collector foil is provided. It is also possible to adopt a form.

本発明において、集電体の表面に正極層が配設される場合、正極層は、例えば、正極材と固体電解質層に含有される固体電解質（例えば、Ｌｉ２Ｓ：Ｐ２Ｓ５＝５０：５０〜１００：０（質量比）でＬｉ２Ｓ及びＰ２Ｓ５を混合した混合物（以下において、「Ｌｉ２Ｓ−Ｐ２Ｓ５」という。））とを混合し、９８ＭＰａの圧力でプレスすることにより作製することができる。正極層に含有させる正極材としては、リチウム遷移金属酸化物及びカルコゲン化物を例示することができる。正極層に含有させるリチウム遷移金属酸化物としては、コバルト酸リチウム（ＬｉＣｏＯ２）、ニッケル酸リチウム（ＬｉＮｉＯ２）、マンガン酸リチウム（ＬｉＭｎＯ２）、鉄オリビン（ＬｉＦｅＰＯ４）、コバルトオリビン（ＬｉＣｏＰＯ４）、マンガンオリビン（ＬｉＭｎＰＯ４）、及び、チタン酸リチウム（Ｌｉ４Ｔｉ５Ｏ１２）等を例示することができる。また、正極層に含有させるカルコゲン化物としては、銅シュブレル（Ｃｕ２Ｍｏ６Ｓ８）、硫化鉄（ＦｅＳ）、及び、硫化コバルト（ＣｏＳ）、及び、硫化ニッケル（ＮｉＳ）等を例示することができる。 In the present invention, when the positive electrode layer is disposed on the surface of the current collector, the positive electrode layer is, for example, a solid electrolyte (for example, Li 2 S: P 2 S 5 = 50) contained in the positive electrode material and the solid electrolyte layer. : 50 to 100: 0 (mass ratio) with a mixture of Li 2 S and P 2 S 5 (hereinafter referred to as “Li 2 S—P 2 S 5 ”) and a pressure of 98 MPa. It can be produced by pressing. Examples of the positive electrode material contained in the positive electrode layer include lithium transition metal oxides and chalcogenides. Examples of the lithium transition metal oxide contained in the positive electrode layer include lithium cobaltate (LiCoO 2 ), lithium nickelate (LiNiO 2 ), lithium manganate (LiMnO 2 ), iron olivine (LiFePO 4 ), and cobalt olivine (LiCoPO 4 ). , Manganese olivine (LiMnPO 4 ), lithium titanate (Li 4 Ti 5 O 12 ), and the like. Examples of chalcogenides to be contained in the positive electrode layer include copper subrel (Cu 2 Mo 6 S 8 ), iron sulfide (FeS), cobalt sulfide (CoS), and nickel sulfide (NiS). it can.

また、本発明において、集電体の表面に負極層が配設される場合、負極層は、例えば、負極材と固体電解質層に含有されるＬｉ２Ｓ−Ｐ２Ｓ５とを混合し、３９２ＭＰａの圧力でプレスすることにより作製することができる。負極層に含有させる負極材としては、カーボン、リチウム遷移金属酸化物、及び、合金を例示することができる。負極層に含有させるリチウム遷移金属酸化物としては、チタン酸リチウム（Ｌｉ４Ｔｉ５Ｏ１２）を例示することができる。また、負極層に含有させる合金としては、Ｌａ３Ｎｉ２Ｓｎ７を例示することができる。 In the present invention, when the negative electrode layer is disposed on the surface of the current collector, the negative electrode layer is, for example, a mixture of the negative electrode material and Li 2 S—P 2 S 5 contained in the solid electrolyte layer, It can be produced by pressing at a pressure of 392 MPa. Examples of the negative electrode material contained in the negative electrode layer include carbon, lithium transition metal oxides, and alloys. Examples of the lithium transition metal oxide contained in the negative electrode layer include lithium titanate (Li 4 Ti 5 O 12 ). As the alloy to be contained in the negative electrode layer, it can be exemplified La 3 Ni 2 Sn 7.

また、本発明において、集電体を用いて複数の固体電池（単電池）を電気的に接続する場合、各単電池に備えられる固体電解質層は、例えば、Ｌｉ２Ｓ−Ｐ２Ｓ５を１０ＭＰａ〜５００ＭＰａの圧力でプレスすることにより作製することができる。 In the present invention, when a plurality of solid state batteries (unit cells) are electrically connected using a current collector, the solid electrolyte layer provided in each unit cell is, for example, Li 2 S—P 2 S 5 . It can be produced by pressing at a pressure of 10 MPa to 500 MPa.

また、本発明において、集電体を用いて複数の単電池が電気的に接続された固体電池を作製する場合、端子及び筐体は、固体電池で使用可能な公知の材料によって構成した公知の形態とすることができる。   Further, in the present invention, when a solid battery in which a plurality of single cells are electrically connected is manufactured using a current collector, the terminal and the housing are known materials made of known materials that can be used in the solid battery. It can be in the form.

固体電池を構成すべき正極層に接続された、厚さ１５μｍのアルミニウム箔によって構成される集電箔２と、固体電池を構成すべき負極層に接続された、厚さ１０μｍの銅箔によって構成される集電箔３とを用いて、本発明の集電体１を含む構造体４の製造を試みた。集電箔２の貫通孔２ａ、２ａ、…の直径（孔径）は１ｍｍとし、隣り合う貫通孔２ａ、２ａの中心距離の最小値は３ｍｍとした。その結果、集電箔２と集電箔３とを溶接することにより、集電箔２及び集電箔３を強固に密着させることができた。なお、貫通孔２ａの孔径を０．５ｍｍ以下にすると一対の集電箔の密着性が低下しやすく、貫通孔２ａの孔径を１ｃｍ以上にすると集電箔に皺が入りやすかった。したがって、本発明の集電体を構成可能な集電箔（アルミニウム箔）に貫通孔が備えられる場合、貫通孔の孔径は０．５ｍｍよりも大きくすることが好ましく、１ｃｍ未満とすることが好ましい。   Constructed by current collector foil 2 composed of an aluminum foil having a thickness of 15 μm connected to a positive electrode layer constituting a solid battery and a copper foil having a thickness of 10 μm connected to a negative electrode layer constituting a solid battery An attempt was made to produce a structure 4 including the current collector 1 of the present invention using the current collector foil 3. The diameter (hole diameter) of the through holes 2a, 2a,... Of the current collector foil 2 was 1 mm, and the minimum value of the center distance between the adjacent through holes 2a, 2a was 3 mm. As a result, by welding the current collector foil 2 and the current collector foil 3, the current collector foil 2 and the current collector foil 3 could be firmly adhered. In addition, when the hole diameter of the through-hole 2a was 0.5 mm or less, the adhesiveness of a pair of current collector foil was easy to fall, and when the hole diameter of the through-hole 2a was 1 cm or more, wrinkles were easy to enter into the current collector foil. Therefore, when the current collector foil (aluminum foil) that can constitute the current collector of the present invention is provided with a through hole, the hole diameter of the through hole is preferably larger than 0.5 mm, and preferably less than 1 cm. .

本発明の集電体は、電気自動車やハイブリッド自動車用等に、本発明の集電体の製造方法は、電気自動車やハイブリッド自動車等に利用可能な固体電池等を製造する際に、利用することができる。   The current collector of the present invention is used for electric vehicles, hybrid vehicles, etc., and the method of manufacturing the current collector of the present invention is used when manufacturing solid batteries that can be used for electric vehicles, hybrid vehicles, etc. Can do.

１…集電体
２…集電箔
２ａ…貫通孔
３…集電箔
４…構造体
５…正極層
６…負極層
７…固体電解質層
８…積層体
９…電極体
１０…固体電池
１１、１１ａ、１１ｂ…端子
１２…正極端子
１３…負極端子
１４…筐体 DESCRIPTION OF SYMBOLS 1 ... Current collector 2 ... Current collector foil 2a ... Through-hole 3 ... Current collector foil 4 ... Structure 5 ... Positive electrode layer 6 ... Negative electrode layer 7 ... Solid electrolyte layer 8 ... Laminated body 9 ... Electrode body 10 ... Solid battery 11, 11a, 11b ... terminal 12 ... positive electrode terminal 13 ... negative electrode terminal 14 ... housing

Claims (1)

少なくとも一方の集電箔に凹部が備えられる一対の集電箔を用意する準備工程と、
前記準備工程で用意された前記一対の集電箔の一部を直接重ねて接触させる接触工程と、
前記接触工程で接触させた前記一対の集電箔のうち、前記凹部と対向している前記集電箔の一部を溶解させ、溶解させた前記集電箔の一部を前記凹部へと流入させる過程を経て、前記一対の集電箔を接続する接続工程と、
を有することを特徴とする、集電体の製造方法。 Preparing a pair of current collector foils provided with a recess in at least one current collector foil; and
A contact step in which a part of the pair of current collector foils prepared in the preparation step is directly overlapped and contacted;
Of the pair of current collector foils contacted in the contact step, a part of the current collector foil facing the concave portion is dissolved, and a part of the dissolved current collector foil flows into the concave portion Through the process of connecting the pair of current collector foil,
A method for producing a current collector, comprising:
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