JP2019121485A - All-solid battery - Google Patents

All-solid battery Download PDF

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JP2019121485A
JP2019121485A JP2017254439A JP2017254439A JP2019121485A JP 2019121485 A JP2019121485 A JP 2019121485A JP 2017254439 A JP2017254439 A JP 2017254439A JP 2017254439 A JP2017254439 A JP 2017254439A JP 2019121485 A JP2019121485 A JP 2019121485A
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solid
positive electrode
current collector
layer
collector layer
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JP6977554B2 (en
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哲也 早稲田
Tetsuya Waseda
哲也 早稲田
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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

Abstract

To provide an all-solid battery where the lateral face of the all-solid battery laminate is coated with a resin layer, and even when the all-solid battery laminate is confined by means of a pair of end plates, the all-solid battery laminate can be confined with sufficient pressure.SOLUTION: In the lamination direction of an all-solid battery laminate, thickness of the all-solid battery laminate is larger than the thickness of a resin layer, the positive electrode collector layer and/or the negative electrode collector layer adjoining a pair of end plates, respectively, has an area larger than that of the adjoining positive electrode active material layer and/or the negative electrode active material layer, and the end of the positive electrode collector layer and/or the negative electrode collector layer adjoining the pair of end plates, respectively, has a rim bending toward the opposite side of the end plate adjoining the positive electrode collector layer and/or the negative electrode collector layer.SELECTED DRAWING: Figure 1

Description

本開示は、全固体電池に関する。特に、本開示は、全固体電池積層体の側面が樹脂層で被覆されており、かつ全固体電池積層体の両端面を積層方向に一対のエンドプレートで拘束されている全固体電池に関する。   The present disclosure relates to all solid state batteries. In particular, the present disclosure relates to an all-solid battery in which the side surface of the all-solid battery stack is coated with a resin layer, and both end surfaces of the all-solid battery stack are constrained by a pair of end plates in the stacking direction.

近年、積層電池の実用化に伴い、積層電池を被覆する技術も注目されている。例えば、特許文献１では、全固体電池素子を熱硬化性樹脂又は熱可塑性樹脂から構成される外装体で被覆する技術が開示されている。また、特許文献２では、電解液を用いた電池本体を、熱硬化性樹脂などの未硬化材料で被包し、その後、未硬化性材料を硬化させる技術が開示されている。さらに、特許文献３では、固体電池素子本体の側面に樹脂製の枠体が設けられ、及び固体電極層と、集電体層との間に封止導電性粘着フィルムが設けられている技術が開示されている。   In recent years, with the practical use of laminated batteries, a technology for covering laminated batteries has also attracted attention. For example, Patent Document 1 discloses a technique for covering an all solid battery element with an exterior body made of a thermosetting resin or a thermoplastic resin. Further, Patent Document 2 discloses a technology in which a battery body using an electrolytic solution is encapsulated with an uncured material such as a thermosetting resin, and then the uncured material is cured. Furthermore, in Patent Document 3, there is a technology in which a resin frame is provided on the side surface of the solid battery element body, and a sealing conductive adhesive film is provided between the solid electrode layer and the current collector layer. It is disclosed.

特開２０００−１０６１５４号公報JP 2000-106154 A 特開２０００−２５１８５８号公報Unexamined-Japanese-Patent No. 2000-251858 特開２０１５−０７６１７８号公報JP, 2015-076178, A

全固体電池積層体に対して、拘束圧を加えることによって、固体電解質層と活物質層（正極活物質層又は負極活物質層）との界面接合が良好になり、それによって、電池の抵抗が低下することが知られている。   By applying a confining pressure to the all solid battery laminate, the interfacial bonding between the solid electrolyte layer and the active material layer (positive electrode active material layer or negative electrode active material layer) is improved, whereby the battery resistance is improved. It is known to decline.

しかしながら、全固体電池積層体の側面を樹脂層で被覆している場合、エンドプレートを用いて全固体電池積層体の両端面に圧力を加えると、エンドプレートが樹脂層に当接することによって、全固体電池積層体を十分な圧力で拘束することが困難になることがある。   However, in the case where the side surface of the all solid battery laminate is coated with the resin layer, when pressure is applied to both end surfaces of the all solid battery laminate using the end plate, the end plate abuts the resin layer. It may be difficult to constrain the solid state battery stack with sufficient pressure.

したがって、本開示は、上記事情を鑑みてなされたものであり、全固体電池積層体の側面を樹脂層で被覆しており、かつ全固体電池積層体の両端面を一対のエンドプレートで拘束している場合でも、全固体電池積層体を十分な圧力を加えながら拘束できる全固体電池を提供することを目的とする。   Therefore, the present disclosure has been made in view of the above circumstances, in which the side surface of the all solid battery laminate is coated with a resin layer, and both end surfaces of the all solid battery laminate are restrained by a pair of end plates. It is an object of the present invention to provide an all-solid-state battery capable of restraining while applying a sufficient pressure to the all-solid-state battery stack.

本開示の本発明者は、以下の手段により、上記課題を解決できることを見出した。   The inventor of the present disclosure has found that the above-mentioned problems can be solved by the following means.

正極集電体層、正極活物質層、固体電解質層、負極活物質層、及び負極集電体層を、この順で積層してなる単位全固体電池を１以上有する全固体電池積層体と、
前記全固体電池積層体の側面を被覆している樹脂層と、
前記全固体電池積層体の両端面を積層方向に拘束している一対のエンドプレートと、
を有し、
前記全固体電池積層体の積層方向において、前記全固体電池積層体の厚さが、前記樹脂層の厚さよりも大きく、
前記一対のエンドプレートのそれぞれに隣接する前記正極集電体層及び／又は前記負極集電体層が、それぞれに隣接する前記正極活物質層及び／又は前記負極活物質層よりも大きい面積を有し、かつ
前記一対のエンドプレートのそれぞれに隣接する前記正極集電体層及び／又は前記負極集電体層の端部が、前記正極集電体層及び／又は前記負極集電体層に隣接するエンドプレートの反対側に向かって屈曲している屈曲周縁部を有する、
全固体電池。 An all solid battery laminate having at least one unit all solid battery formed by laminating a positive electrode current collector layer, a positive electrode active material layer, a solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer in this order;
A resin layer covering the side surface of the all solid battery laminate;
A pair of end plates constraining both end faces of the all-solid-state battery stack in the stacking direction;
Have
In the stacking direction of the all-solid-state battery stack, the thickness of the all-solid-state battery stack is larger than the thickness of the resin layer,
The positive electrode current collector layer and / or the negative electrode current collector layer adjacent to each of the pair of end plates have a larger area than the positive electrode active material layer and / or the negative electrode active material layer adjacent to each other. And an end portion of the positive electrode current collector layer and / or the negative electrode current collector layer adjacent to each of the pair of end plates is adjacent to the positive electrode current collector layer and / or the negative electrode current collector layer. Having a bending edge which is bent towards the opposite side of the
All solid state battery.

本開示によれば、全固体電池積層体の側面を樹脂層で被覆しており、かつ全固体電池積層体の両端面を一対のエンドプレートで拘束している場合でも、全固体電池積層体を十分な圧力で拘束することができる。   According to the present disclosure, even when the side surface of the all solid battery laminate is coated with a resin layer and both end surfaces of the all solid battery laminate are restrained by a pair of end plates, It can be restrained with sufficient pressure.

図１は、本開示の全固体電池の一例を示す概略断面図である。FIG. 1 is a schematic cross-sectional view showing an example of the all-solid-state battery of the present disclosure. 図２は、本開示の全固体電池の一例の一部分を示す平面図である。FIG. 2 is a plan view showing a part of an example of the all-solid-state battery of the present disclosure. 図３は、本開示の全固体電池の一例の一部分を示す概略断面図である。FIG. 3 is a schematic cross-sectional view showing a part of an example of the all-solid-state battery of the present disclosure.

以下、図面を参照しながら、本開示を実施するための形態について、詳細に説明する。なお、説明の便宜上、各図において、同一又は相当する部分には同一の参照符号を付し、重複説明は省略する。実施の形態の各構成要素は、全てが必須のものであるとは限らず、一部の構成要素を省略可能な場合もある。最も、以下の図に示される形態は本開示の例示であり、本開示を限定するものではない。   Hereinafter, embodiments of the present disclosure will be described in detail with reference to the drawings. Note that, for convenience of explanation, in the respective drawings, the same or corresponding parts will be denoted by the same reference symbols, and redundant description will be omitted. Not all of the components of the embodiment are necessarily required, and some components may be omitted. Mostly, the forms shown in the following figures are examples of the present disclosure and do not limit the present disclosure.

≪全固体電池≫
本開示の全固体電池は、
正極集電体層、正極活物質層、固体電解質層、負極活物質層、及び負極集電体層を、この順で積層してなる単位全固体電池を１以上有する全固体電池積層体と、
全固体電池積層体の側面を被覆している樹脂層と、
全固体電池積層体の両端面を積層方向に拘束している一対のエンドプレートと、
を有し、
全固体電池積層体の積層方向において、全固体電池積層体の厚さが、樹脂層の厚さよりも大きく、
一対のエンドプレートのそれぞれに隣接する正極集電体層及び／又は負極集電体層が、それぞれに隣接する正極活物質層及び／又は負極活物質層よりも大きい面積を有し、かつ
一対のエンドプレートのそれぞれに隣接する正極集電体層及び／又は負極集電体層の端部が、当該正極集電体層及び／又は当該負極集電体層に隣接するエンドプレートの反対側に向かって屈曲している屈曲周縁部を有する。 «All solid state battery»
The all solid state battery of the present disclosure is
An all solid battery laminate having at least one unit all solid battery formed by laminating a positive electrode current collector layer, a positive electrode active material layer, a solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer in this order;
A resin layer covering the side of the all solid battery laminate,
A pair of end plates constraining both end faces of the all-solid-state battery stack in the stacking direction;
Have
In the stacking direction of the all solid battery stack, the thickness of the all solid battery stack is larger than the thickness of the resin layer,
The positive electrode current collector layer and / or the negative electrode current collector layer adjacent to each of the pair of end plates has a larger area than the positive electrode active material layer and / or the negative electrode active material layer adjacent to each other, and The end portions of the positive electrode current collector layer and / or the negative electrode current collector layer adjacent to each of the end plates face the opposite side of the end plate adjacent to the positive electrode current collector layer and / or the negative electrode current collector layer. And has a bent peripheral edge.

図１は、本開示の全固体電池の一例を示す概略断面図である。本開示の全固体電池１００は、全固体電池積層体１０と、全固体電池積層体１０の側面を被覆している樹脂層１１と、全固体電池積層体１０の両端面を積層方向に拘束している一対のエンドプレート１２ａ及び１２ｂと、を有する。この際、全固体電池積層体１０の積層方向において、全固体電池積層体１０の厚さＴは、樹脂層１１の厚さｔよりも大きい。また、エンドプレート１２ａに隣接する正極集電体層１ａが、正極集電層１ａに隣接する正極活物質層２ａよりも大きい面積を有し、かつエンドプレート１２ａに隣接する正極集電体層１ａの端部１ａｘが、エンドプレート１２ａと反対側に向かって屈曲している屈曲周縁部を有している。同様に、エンドプレート１２ｂに隣接する正極集電体層１ｄが、正極集電体層１ｄに隣接する正極活物質層２ｄよりも大きい面積を有し、かつエンドプレート１２ｂに隣接する正極集電体層１ｄの端部１ｄｘが、エンドプレート１２ｂと反対側に向かって屈曲している屈曲周縁部を有している。 FIG. 1 is a schematic cross-sectional view showing an example of the all-solid-state battery of the present disclosure. The all solid battery 100 of the present disclosure includes the all solid battery stack 10, the resin layer 11 covering the side surface of the all solid battery stack 10, and the both end faces of the all solid battery stack 10 in the stacking direction. And a pair of end plates 12a and 12b. At this time, the thickness T of the all-solid-state battery stack 10 is larger than the thickness t of the resin layer 11 in the stacking direction of the all-solid-state battery stack 10. Further, the positive electrode current collector layer 1a adjacent to the end plate 12a has a larger area than the positive electrode active material layer 2a adjacent to the positive electrode current collection layer 1a, and the positive electrode current collector layer 1a adjacent to the end plate 12a. The end portion 1a x has a bent peripheral portion which is bent toward the opposite side to the end plate 12a. Similarly, the positive electrode current collector layer 1d adjacent to the end plate 12b has a larger area than the positive electrode active material layer 2d adjacent to the positive electrode current collector layer 1d, and the positive electrode current collector adjacent to the end plate 12b. The end 1d x of the layer 1d has a bent peripheral edge that is bent toward the opposite side to the end plate 12b.

上述したように、樹脂層で被覆されている全固体電池では、全固体電池積層体に対して、拘束圧を加える必要がある。しかしながら、このような全固体電池では、エンドプレートなどを用いて全固体電池積層体に圧力を加えると、エンドプレートが樹脂層に当接してしまうことがあるため、全固体電池積層体を十分な圧力で拘束することが困難な場合がある。   As described above, in the all-solid-state battery coated with a resin layer, it is necessary to apply a confining pressure to the all-solid-state battery stack. However, in such an all solid battery, when pressure is applied to the all solid battery stack using an end plate or the like, the end plate may abut against the resin layer, so that the all solid battery stack is sufficient. It may be difficult to restrain by pressure.

これに対して、本開示の全固体電池は、（ｉ）全固体電池積層体の積層方向において、全固体電池積層体の厚さが、樹脂層の厚さよりも大きいこと、及び（ｉｉ）一対のエンドプレートのそれぞれに隣接する正極集電体層及び／又は負極集電体層が、それぞれに隣接する正極活物質層及び／又は負極活物質層よりも大きい面積を有し、かつ一対のエンドプレートのそれぞれに隣接する正極集電体層及び／又は負極集電体層の端部が、当該正極集電体層及び／又は当該負極集電体層に隣接するエンドプレートの反対側に向かって屈曲している屈曲周縁部を有していること、という二つの特徴を有する。   On the other hand, in the all-solid battery of the present disclosure, (i) the thickness of the all-solid battery laminate is greater than the thickness of the resin layer in the stacking direction of the all-solid battery laminate, and (ii) a pair The positive electrode current collector layer and / or the negative electrode current collector layer adjacent to each of the end plates has a larger area than the positive electrode active material layer and / or the negative electrode active material layer adjacent to each other, and the pair of ends The end of the positive electrode current collector layer and / or the negative electrode current collector layer adjacent to each of the plates is directed to the opposite side of the end plate adjacent to the positive electrode current collector layer and / or the negative electrode current collector layer. It has two features of having a bending peripheral edge which is bent.

本開示の全固体電池は、この特徴（ｉ）及び特徴（ｉｉ）を同時に備えることによって、全固体電池積層体を十分な圧力で拘束することができる。以下では、特徴（ｉ）及び特徴（ｉｉ）のそれぞれについて、詳細に説明する。   The all-solid-state battery of the present disclosure can restrain the all-solid-state battery stack with sufficient pressure by simultaneously including the feature (i) and the feature (ii). Hereinafter, each of the feature (i) and the feature (ii) will be described in detail.

〈特徴（ｉ）〉
本開示の全固体電池では、全固体電池積層体の積層方向において、全固体電池積層体の厚さは、樹脂層の厚さよりも大きい。ここで、全固体電池積層体の厚さとは、全固体電池積層体の積層方向における両端の距離を指す。例えば、図１において、全固体電池積層体１０の積層方向における全固体電池積層体１０の厚さは、Ｔで示されている。 <Feature (i)>
In the all-solid-state battery of the present disclosure, the thickness of the all-solid-state battery stack is greater than the thickness of the resin layer in the stacking direction of the all-solid-state battery stack. Here, the thickness of the all-solid-state battery stack refers to the distance between both ends in the stacking direction of the all-solid-state battery stack. For example, in FIG. 1, the thickness of the all-solid-state battery stack 10 in the stacking direction of the all-solid-state battery stack 10 is indicated by T.

また、全固体電池積層体の積層方向における樹脂層の厚さとは、全固体電池積層体の積層方向における両端の距離を指す。例えば、図１において、全固体電池積層体１０の積層方向における樹脂層１１の厚さは、ｔで示されている。この際、Ｔはｔより大きい。   Moreover, the thickness of the resin layer in the lamination direction of an all-solid-state battery laminated body points out the distance of the both ends in the lamination direction of an all-solid-state battery laminated body. For example, in FIG. 1, the thickness of the resin layer 11 in the stacking direction of the all-solid-state battery stack 10 is indicated by t. At this time, T is larger than t.

本開示の全固体電池では、全固体電池積層体が一対のエンドプレートで積層方向に拘束されている。したがって、全固体電池積層体の積層方向において、全固体電池積層体の厚さが、樹脂層の厚さよりも大きいということは、樹脂層と一対のエンドプレートとが、接触していないこと又は弱くのみ接触していることを意味する。   In the all-solid-state battery of the present disclosure, the all-solid-state battery stack is constrained in the stacking direction by a pair of end plates. Therefore, in the stacking direction of the all solid battery stack, the fact that the thickness of the all solid battery stack is larger than the thickness of the resin layer means that the resin layer and the pair of end plates are not in contact or weak It means that only you are in contact.

樹脂層と一対のエンドプレートとが接触していないこと又は弱くのみ接触していることにより、全固体電池積層体を十分な圧力で拘束することができる。また、全固体電池積層体の側面全体が樹脂層で覆われている従来の全固体電池に比べて、本開示の全固体電池は、用いられる樹脂の量が少なく、これは、電池のエネルギー密度向上にも繋がる。   The non-contact or only weak contact between the resin layer and the pair of end plates allows the all-solid-state battery stack to be restrained with a sufficient pressure. In addition, the all-solid-state battery of the present disclosure uses a smaller amount of resin than the conventional all-solid-state battery in which the entire side surface of the all-solid-state battery laminate is covered with a resin layer. It also leads to improvement.

なお、本開示において、全固体電池積層体の積層方向において、全固体電池積層体の厚さの範囲は、特に限定されず、必要とする全固体電池の使用用途や使用目的に合わせて、適宜設定できる。また、樹脂層の厚さの範囲は、全固体電池積層体の厚さの大きさより小さく設定すればよい。   In the present disclosure, the range of the thickness of the all-solid battery laminate is not particularly limited in the stacking direction of the all-solid battery laminate, and is appropriately selected according to the use application and purpose of the required all-solid battery. It can be set. Further, the range of the thickness of the resin layer may be set smaller than the size of the thickness of the all solid battery laminate.

〈特徴（ｉｉ）〉
本開示において、一対のエンドプレートのそれぞれに隣接する正極集電体層及び／又は負極集電体層が、それぞれに隣接する正極活物質層及び／又は負極活物質層よりも大きい面積を有し、かつ一対のエンドプレートのそれぞれに隣接する正極集電体層及び／又は負極集電体層の端部が、当該正極集電体層及び／又は当該負極集電体層に隣接するエンドプレートの反対側に向かって屈曲している屈曲周縁部を有する。 <Feature (ii)>
In the present disclosure, the positive electrode current collector layer and / or the negative electrode current collector layer adjacent to each of the pair of end plates has a larger area than the positive electrode active material layer and / or the negative electrode active material layer adjacent to each other. And an end portion of the positive electrode current collector layer and / or the negative electrode current collector layer adjacent to each of the pair of end plates is the end plate adjacent to the positive electrode current collector layer and / or the negative electrode current collector layer. It has a bending edge which is bent towards the opposite side.

例えば、図１に示されている全固体電池１００では、エンドプレート１２ａに隣接する正極集電体層１ａが、それに隣接する正極活物質層２ａよりも大きい面積を有し、かつエンドプレート１２ａに隣接する正極集電体層１ａの端部１ａｘが、正極集電体層１ａが隣接するエンドプレート１２ａの反対側に向かって屈曲している屈曲周縁部を有している。同様に、エンドプレート１２ｂに隣接する正極集電体層１ｄが、それに隣接する正極活物質層２ａよりも大きい面積を有し、かつエンドプレート１２ｂに隣接する正極集電体層１ｄの端部１ｄｘが、正極集電体層１ｄが隣接するエンドプレート１２ｂの反対側に向かって屈曲している屈曲周縁部を有している。 For example, in the all-solid battery 100 shown in FIG. 1, the positive electrode current collector layer 1a adjacent to the end plate 12a has a larger area than the positive electrode active material layer 2a adjacent thereto, and the end plate 12a The end portion 1a x of the adjacent positive electrode current collector layer 1a has a bent peripheral portion bent toward the opposite side of the end plate 12a adjacent to the positive electrode current collector layer 1a. Similarly, the positive electrode current collector layer 1d adjacent to the end plate 12b has a larger area than the positive electrode active material layer 2a adjacent to the end plate 12b, and the end 1d of the positive electrode current collector layer 1d adjacent to the end plate 12b. x has a bent peripheral portion which is bent toward the opposite side of the end plate 12b adjacent to the positive electrode current collector layer 1d.

本開示において、一対のエンドプレートに隣接する正極集電体層及び／又は負極集電体層の端部に屈曲周縁部を設けるためには、かかる正極集電体層及び／又は負極集電体層の面積は、それらに隣接する正極活物質層及び／又は負極活物質層の面積より大きく設定する必要がある。これによって、かかる正極集電体層及び／又は負極集電体層は、それらに隣接する正極活物質層及び又は負極活物質層からはみ出している部分を有する。このはみ出している部分は、本開示でいう「正極集電体層及び／又は負極集電体層の端部」である。   In the present disclosure, in order to provide a bent peripheral portion at the end of the positive electrode current collector layer and / or the negative electrode current collector layer adjacent to the pair of end plates, the positive electrode current collector layer and / or the negative electrode current collector The area of the layers needs to be set larger than the area of the positive electrode active material layer and / or the negative electrode active material layer adjacent to them. Thus, the positive electrode current collector layer and / or the negative electrode current collector layer have portions protruding from the positive electrode active material layer and / or the negative electrode active material layer adjacent thereto. The protruding portion is the “end portion of the positive electrode current collector layer and / or the negative electrode current collector layer” in the present disclosure.

例えば、エンドプレート１２ａ、正極集電体層１ａ、及び正極活物質層２ａがこの順に積層されている平面図は、図２に示されている。この場合、正極集電体層１ａの面積は、それに隣接する正極活物質層２ａの面積より大きい。よって、正極集電体層１ａは、正極活物質層２ａからはみ出している部分Ｌを有する。このはみ出している部分Ｌは、正極活物質層２ａの端部１ａｘである。 For example, a plan view in which the end plate 12a, the positive electrode current collector layer 1a, and the positive electrode active material layer 2a are stacked in this order is shown in FIG. In this case, the area of the positive electrode current collector layer 1a is larger than the area of the positive electrode active material layer 2a adjacent thereto. Therefore, the positive electrode current collector layer 1a has a portion L protruding from the positive electrode active material layer 2a. The protruding portion L is an end portion 1a x of the positive electrode active material layer 2a.

また、「一対のエンドプレートのそれぞれに隣接する正極集電体層及び／又は負極集電体層の端部が、当該正極集電体層及び／又は当該負極集電体層に隣接するエンドプレートの反対側に向かって屈曲している屈曲周縁部」とは、上記で説明した正極集電体層又は負極集電体層の端部において、それらに隣接するエンドプレートの反対側に向かって折れ曲がっている部分を指す。例えば、図２では、正極集電体層１ａの端部１ａｘが、エンドプレート１２ａの反対側に向かって屈曲している屈曲周縁部は、かかる端部１ａｘにおいて、エンドプレート１２ａの反対側（すなわち、正極活物質層２ａが積層されている側）に向かって折れ曲がっている部分を指す。 In addition, “the end portion of the positive electrode current collector layer and / or the negative electrode current collector layer adjacent to each of the pair of end plates is adjacent to the positive electrode current collector layer and / or the negative electrode current collector layer. In the end portion of the positive electrode current collector layer or the negative electrode current collector layer described above, the bent peripheral portion bent toward the opposite side of the is bent toward the opposite side of the end plate adjacent thereto. Point to the For example, in FIG. 2, the ends 1a x of the positive electrode collector layer 1a is bent peripheral edge portion is bent toward the opposite side of the end plate 12a, in such end 1a x, opposite to the end plate 12a (That is, the portion bent toward the side on which the positive electrode active material layer 2a is stacked).

本開示において、この特徴（ｉｉ）を有することによって、全固体電池積層体がエンドプレートに拘束されている際に、かかる正極集電体層又は負極集電体層が樹脂層に当接する面積を抑制することができる。   In the present disclosure, by having this feature (ii), when the all-solid-state battery laminate is constrained to the end plate, the area where the positive electrode current collector layer or the negative electrode current collector layer abuts on the resin layer is It can be suppressed.

これに関して、上述して屈曲周縁部の存在によって、かかる正極集電体層又は負極集電体層の端部と、それらに隣接するエンドプレートとの間の角度は、０°超、又は１０°以上であって、９０°以下、６０°以下、又は４５°以下であることが好ましい。   In this regard, the angle between the end of such positive current collector layer or negative current collector layer and the end plate adjacent thereto is greater than 0 °, or 10 °, depending on the presence of the bending edge as described above. It is preferable that the angle is 90 ° or less, 60 ° or less, or 45 ° or less.

例えば、図３に示されている全固体電池の一部分において、正極集電体層１ａの端部１ａｘは、正極集電体層１ａが隣接するエンドプレート１２ａの反対側に向かって屈曲している屈曲周縁部を有している。この屈曲周縁部を有することによって、エンドプレート１２ａによる加圧時に、正極集電体層１ａが樹脂層１１に当接する面積を抑制できる。また、正極集電体層１ａの端部とエンドプレート１２ａとの間の角度は、図３において、「α」として示されている。 For example, in a part of the all-solid-state battery shown in FIG. 3, the end 1a x of the positive electrode current collector layer 1a is bent toward the opposite side of the end plate 12a adjacent to the positive electrode current collector layer 1a. Have a bent peripheral edge. By having this bent peripheral portion, the area in which the positive electrode current collector layer 1a abuts on the resin layer 11 can be suppressed when the end plate 12a applies pressure. The angle between the end of the positive electrode current collector layer 1a and the end plate 12a is shown as "α" in FIG.

このように、本開示は、上述した特徴（ｉ）及び特徴（ｉｉ）を同時に備えることによって、全固体電池積層体を十分な圧力で拘束することができる。   Thus, the present disclosure can constrain the all-solid-state battery stack with sufficient pressure by simultaneously including the features (i) and (ii) described above.

〈全固体電池の種類及び形状〉
本開示において、全固体電池の種類としては、全固体リチウム電池、全固体ナトリウム電池、全固体マグネシウム電池及び全固体カルシウム電池などを挙げることができ、中でも、全固体リチウム電池及び全固体ナトリウム電池が好ましく、特に、全固体リチウム電池が好ましい。また、本開示の全固体電池は、一次電池であってもよく、二次電池であってもよいが、中でも、二次電池であることが好ましい。二次電池は、繰り返し充放電でき、例えば、車載用電池として有用だからである。 <Type and shape of all solid battery>
In the present disclosure, types of all solid batteries may include all solid lithium batteries, all solid sodium batteries, all solid magnesium batteries, all solid calcium batteries, etc., among which all solid lithium batteries and all solid sodium batteries Preferably, all solid lithium batteries are preferred. Further, the all solid state battery of the present disclosure may be a primary battery or a secondary battery, but among them, a secondary battery is preferable. This is because the secondary battery can be repeatedly charged and discharged, and is useful as, for example, a vehicle-mounted battery.

〈全固体電池積層体〉
本開示において、全固体電池積層体は、１以上の単位全固体電池を有することができる。例えば、図１では、本開示の全固体電池積層体１０は、単位全固体電池６ａ、６ｂ、６ｃ及び６ｄを有する。また、本開示において、単位全固体電池は、正極集電体層、正極活物質層、固体電解質層、負極活物質層、及び負極集電体層を、この順で積層してなる。 <All solid battery stack>
In the present disclosure, the all solid battery stack can have one or more unit all solid batteries. For example, in FIG. 1, the all-solid-state battery stack 10 of the present disclosure includes unit all-solid-state batteries 6a, 6b, 6c, and 6d. In the present disclosure, the unit all-solid battery is formed by laminating a positive electrode current collector layer, a positive electrode active material layer, a solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer in this order.

本開示にかかる全固体電池積層体は、２以上の単位全固体電池を有する場合、積層方向に隣接する２つの単位全固体電池は、正極及び／又は負極集電体層を共有するモノポーラ型の構成であってよい。したがって、例えば全固体電池積層体は、正極集電体層及び負極集電体層を共有する４つの単位全固体電池の積層体であってよい。   When the all solid battery laminate according to the present disclosure has two or more unit all solid batteries, two unit all solid batteries adjacent in the stacking direction are monopolar type sharing the positive electrode and / or the negative electrode collector layer. It may be a configuration. Thus, for example, the all solid battery stack may be a stack of four unit all solid batteries sharing the positive electrode current collector layer and the negative electrode current collector layer.

より具体的には、例えば図１に示されているように、全固体電池積層体１０は、正極集電体層１ａ、正極活物質層２ａ、固体電解質層３ａ、負極活物質層４ａ、負極集電体層５ａ（５ｂ）、負極活物質層４ｂ、固体電解質層３ｂ、正極活物質層２ｂ、正極集電体層１ｂ（１ｃ）、正極活物質層２ｃ、固体電解質層３ｃ、負極活物質層４ｃ、負極集電体層５ｃ（５ｄ）、負極活物質層４ｄ、固体電解質層３ｄ、正極活物質層２ｄ、正極集電体層１ｄを、この順で有することができる。   More specifically, for example, as shown in FIG. 1, the all-solid-state battery stack 10 includes the positive electrode current collector layer 1 a, the positive electrode active material layer 2 a, the solid electrolyte layer 3 a, the negative electrode active material layer 4 a, and the negative electrode Current collector layer 5a (5b), negative electrode active material layer 4b, solid electrolyte layer 3b, positive electrode active material layer 2b, positive electrode current collector layer 1b (1c), positive electrode active material layer 2c, solid electrolyte layer 3c, negative electrode active material The layer 4c, the negative electrode current collector layer 5c (5d), the negative electrode active material layer 4d, the solid electrolyte layer 3d, the positive electrode active material layer 2d, and the positive electrode current collector layer 1d can be provided in this order.

また、全固体電池積層体が２以上の単位全固体電池を有する場合、積層方向に隣接する２つの単位全固体電池は、正極及び負極集電体層の両方として用いられる正極／負極集電体層を共有するバイポーラ型の構成であってよい。したがって、例えば全固体電池積層体は、正極及び負極集電体層の両方として用いられる正極／負極集電体層を共有する３つの単位全固体電池の積層体であってよく、具体的には、正極集電体層、正極活物質層、固体電解質層、負極活物質層、正極／負極集電体層、正極活物質層、固体電解質層、負極活物質層、正極／負極集電体層、正極活物質層、固体電解質層、負極活物質層、及び負極集電体層を、この順で有することができる（図示せず）。   In addition, when the all solid battery laminate has two or more unit all solid batteries, two unit all solid batteries adjacent in the stacking direction are used as both a positive electrode and a negative electrode collector layer. It may be a bipolar configuration that shares layers. Thus, for example, the all solid battery laminate may be a stack of three unit all solid batteries sharing the positive electrode / negative electrode collector layer used as both the positive electrode and the negative electrode collector layer, specifically, Positive electrode current collector layer, positive electrode active material layer, solid electrolyte layer, negative electrode active material layer, positive electrode / negative electrode current collector layer, positive electrode active material layer, solid electrolyte layer, negative electrode active material layer, positive electrode / negative electrode current collector layer A positive electrode active material layer, a solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer can be provided in this order (not shown).

なお、正極集電体層は、面方向に突出する正極集電体突出部を有していてよく、この正極集電体突出部には、正極集電タブが電気的に接続されていてよい。同様に、負極集電体層は、負極集電体突出部を有していてよく、この負極集電体突出部には、負極集電タブが電気的に接続されていてよい。このようなそれぞれの極の集電体突出部及び集電タブを介して、全固体電池積層体で発生した電力を外部に取り出すことができる。なお、全固体電池積層体が複数の正極又は負極集電体層を有する場合には、それぞれの極の複数の集電体突出部を、互いに電気的に接続したうえで、それぞれの極の集電タブに電気的に接続することができる。   The positive electrode current collector layer may have a positive electrode current collector protrusion projecting in the surface direction, and a positive electrode current collector tab may be electrically connected to the positive electrode current collector protrusion. . Similarly, the negative electrode current collector layer may have a negative electrode current collector protrusion, and the negative electrode current collector tab may be electrically connected to the negative electrode current collector protrusion. Electric power generated in the all-solid-state battery stack can be extracted to the outside through the current collector projections and current collection tabs of the respective electrodes. In the case where the all solid battery laminate has a plurality of positive electrode or negative electrode collector layers, the plurality of current collector protrusions of the respective electrodes are electrically connected to one another, and then the collectors of the respective electrodes are collected. It can be electrically connected to the electrical tab.

（正極集電体層）
正極集電体層に用いられる導電性材料は、特に限定されず、全固体電池に使用できる公知のものを適宜採用されうる。例えば、ＳＵＳ、アルミニウム、銅、ニッケル、鉄、チタン、及びカーボンなどが挙げられる。 (Positive current collector layer)
The conductive material used for the positive electrode current collector layer is not particularly limited, and any known material that can be used for the all-solid-state battery can be appropriately adopted. For example, SUS, aluminum, copper, nickel, iron, titanium, carbon and the like can be mentioned.

本開示にかかる正極集電体層の形状として、特に限定されず、例えば、箔状、板状、メッシュ状などを挙げることができる。これらの中で、箔状が好ましい。   It does not specifically limit as a shape of the positive electrode collector layer concerning this indication, For example, foil shape, plate shape, mesh shape etc. can be mentioned. Of these, foils are preferred.

（正極活物質層）
正極活物質層は、少なくとも正極活物質を含み、好ましくは後述する固体電解質を更に含む。そのほか、使用用途や使用目的などに合わせて、例えば、導電助剤又はバインダーなどの全固体電池の正極活物質層に用いられる添加剤を含むことができる。 (Positive electrode active material layer)
The positive electrode active material layer contains at least a positive electrode active material, and preferably further includes a solid electrolyte described later. In addition, according to a use application, a use purpose, etc., the additive used for the positive electrode active material layer of all the solid batteries, such as a conductive support agent or a binder, can be included.

本開示において、用いられる正極活物質材料として、特に限定されず、公知のものが用いられる。例えば、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（ＬｉＭｎ２Ｏ４）、ＬｉＣｏ１／３Ｎｉ１／３Ｍｎ１／３Ｏ２、Ｌｉ１＋ｘＭｎ２−ｘ−ｙＭｙＯ４（Ｍは、Ａｌ、Ｍｇ、Ｃｏ、Ｆｅ、Ｎｉ、及びＺｎから選ばれる１種以上の金属元素）で表される組成の異種元素置換Ｌｉ−Ｍｎスピネルなどが挙げられるが、これらに限定されない。 In the present disclosure, the positive electrode active material to be used is not particularly limited, and known materials can be used. For example, lithium cobaltate (LiCoO 2 ), lithium nickelate (LiNiO 2 ), lithium manganate (LiMn 2 O 4 ), LiCo 1/3 Ni 1/3 Mn 1/3 O 2 , Li 1 + x Mn 2-x- y M y O 4 (M is, Al, Mg, Co, Fe, Ni, and one or more metal elements selected from Zn) such heterogeneous element substituted Li-Mn spinel composition represented by the can be mentioned, It is not limited to these.

導電助剤としては、特に限定されず、公知のものが用いられる。例えば、ＶＧＣＦ（気相成長法炭素繊維、Ｖａｐｏｒ Ｇｒｏｗｎ Ｃａｒｂｏｎ Ｆｉｂｅｒ）及びカーボンナノ繊維などの炭素材並びに金属材などが挙げられるが、これらに限定されない。   The conductive aid is not particularly limited, and known ones may be used. Examples thereof include, but are not limited to, carbon materials such as VGCF (vapor grown carbon fiber) and carbon nanofibers and metal materials such as carbon nanofibers.

バインダーとしては、特に限定されず、公知のものが用いられる。例えば、ポリフッ化ビニリデン（ＰＶｄＦ）、カルボキシメチルセルロース（ＣＭＣ）、ブタジエンゴム（ＢＲ）若しくはスチレンブタジエンゴム（ＳＢＲ）などの材料又はこれらの組合せを挙げることができるが、これらに限定されない。   The binder is not particularly limited, and known ones may be used. Examples include, but are not limited to, materials such as polyvinylidene fluoride (PVdF), carboxymethylcellulose (CMC), butadiene rubber (BR) or styrene butadiene rubber (SBR), or combinations thereof.

（固体電解質層）
固体電解質層は、少なくとも固体電解質を含む。固体電解質として、特に限定されず、全固体電池の固体電解質として利用可能な材料を用いることができる。例えば、公知の硫化物固体電解質又は公知の酸化物固体電解質を用いることができる。 (Solid electrolyte layer)
The solid electrolyte layer contains at least a solid electrolyte. The solid electrolyte is not particularly limited, and materials usable as the solid electrolyte of the all solid battery can be used. For example, known sulfide solid electrolytes or known oxide solid electrolytes can be used.

硫化物固体電解質の例として、例えば、Ｌｉ２Ｓ−ＳｉＳ２、ＬｉＩ−Ｌｉ２Ｓ−ＳｉＳ２、ＬｉＩ−Ｌｉ２Ｓ−Ｐ２Ｓ５、ＬｉＩ−ＬｉＢｒ−Ｌｉ２Ｓ−Ｐ２Ｓ５、Ｌｉ２Ｓ−Ｐ２Ｓ５−ＬｉＩ−ＬｉＢｒ、Ｌｉ２Ｓ−Ｐ２Ｓ５−ＧｅＳ２、ＬｉＩ−Ｌｉ２Ｓ−Ｐ２Ｏ５、ＬｉＩ−Ｌｉ３ＰＯ４−Ｐ２Ｓ５、及びＬｉ２Ｓ−Ｐ２Ｓ５等；硫化物系結晶質固体電解質、例えば、Ｌｉ１０ＧｅＰ２Ｓ１２、Ｌｉ７Ｐ３Ｓ１１、Ｌｉ３ＰＳ４、及びＬｉ３．２５Ｐ０．７５Ｓ４等；並びにこれらの組み合わせを挙げることができる。 As an example of a sulfide solid electrolyte, for example, Li 2 S-SiS 2 , LiI-Li 2 S-SiS 2 , LiI-Li 2 S-P 2 S 5 , LiI-LiBr-Li 2 S-P 2 S 5 , Li 2 S-P 2 S 5 -LiI-LiBr, Li 2 S-P 2 S5-GeS 2, LiI-Li 2 S-P 2 O 5, LiI-Li 3 PO 4 -P 2 S 5, and Li 2 S-P 2 S 5 or the like; sulfide-based crystalline solid electrolyte, for example, Li 10 GeP 2 S 12, Li 7 P 3 S 11, Li 3 PS 4, and Li 3.25 P 0.75 S 4, and the like; And combinations thereof.

酸化物固体電解質の例として、ポリエチレンオキシド（ＰＥＯ）、ポリプロピレンオキシド（ＰＰＯ）、及びこれらの共重合体などが挙げられるが、これらに限定されない。   Examples of oxide solid electrolytes include, but are not limited to, polyethylene oxide (PEO), polypropylene oxide (PPO), and copolymers thereof.

固体電解質は、ガラスであっても、結晶化ガラス(ガラスセラミック)であってもよい。また、固体電解質層は、上述した固体電解質以外に、必要に応じてバインダーなどを含んでもよい。具体例として、上述の「正極活物質層」で列挙された「バインダー」と同様であり、ここでは説明を省略する。   The solid electrolyte may be glass or crystallized glass (glass ceramic). In addition to the solid electrolyte described above, the solid electrolyte layer may contain a binder or the like as required. As a specific example, it is the same as the "binder" listed in the above-mentioned "positive electrode active material layer", and the description is omitted here.

（負極活物質層）
負極活物質層は、少なくとも負極活物質を含み、好ましくは上述した固体電解質を更に含む。そのほか、使用用途や使用目的などに合わせて、例えば、導電助剤又はバインダーなどの全固体電池の負極活物質層に用いられる添加剤を含むことができる。 (Anode active material layer)
The negative electrode active material layer contains at least a negative electrode active material, and preferably further contains the solid electrolyte described above. In addition, according to a use application, a use purpose, etc., the additive used for the negative electrode active material layer of all the solid batteries, such as a conductive support agent or a binder, can be included.

本開示において、用いられる負極活物質材料として、特に限定されず、リチウムイオンなどの金属イオンを吸蔵及び放出可能であればよい。例えば、Ｌｉ、Ｓｎ、Ｓｉ若しくはＩｎなどの金属、リチウムとチタンとの合金、又はハードカーボン、ソフトカーボン若しくはグラファイトなどの炭素材料などが挙げられるが、これらに限定されない。   In the present disclosure, the negative electrode active material to be used is not particularly limited, as long as it can occlude and release metal ions such as lithium ions. Examples thereof include, but are not limited to, metals such as Li, Sn, Si or In, alloys of lithium and titanium, hard carbon, soft carbon, carbon materials such as graphite, and the like.

負極活物質層に用いられる固体電解質、導電助剤、バインダーなどその他の添加剤については、上述した「正極活物質層」及び「固体電解質層」の項目で説明したものを適宜採用することができる。   With regard to the other additives such as the solid electrolyte, the conductive support agent, and the binder used in the negative electrode active material layer, those described in the items of “positive electrode active material layer” and “solid electrolyte layer” described above can be appropriately adopted. .

（負極集電体層）
負極集電体層に用いられる導電性材料は、特に限定されず、全固体電池に使用できる公知のものを適宜採用されうる。例えば、ＳＵＳ、アルミニウム、銅、ニッケル、鉄、チタン、及びカーボンなどが挙げられる。 (Anode current collector layer)
The conductive material used for the negative electrode current collector layer is not particularly limited, and any known material that can be used for the all-solid-state battery can be appropriately adopted. For example, SUS, aluminum, copper, nickel, iron, titanium, carbon and the like can be mentioned.

本開示にかかる負極集電体層の形状として、特に限定されず、例えば、箔状、板状、メッシュ状などを挙げることができる。これらの中で、箔状が好ましい。   It does not specifically limit as a shape of the negative electrode collector layer concerning this indication, For example, foil shape, plate shape, mesh shape etc. can be mentioned. Of these, foils are preferred.

〈樹脂層〉
樹脂層の材料は、特に限定されず、一般的な全固体電池に用いられる絶縁性のある樹脂材料と同様であってもよい。例えば、熱硬化性樹脂であってもよく、熱可塑性樹脂であってもよい。より具体的に、例えばポリイミド、ポリエステル、ポリプロピレン、ポリアミド、ポリスチレン、ポリ塩化ビニル、ポリカーボネートなどが挙げられるが、これらに限定されない。 <Resin layer>
The material of the resin layer is not particularly limited, and may be the same as the insulating resin material used in a general all-solid-state battery. For example, it may be a thermosetting resin or a thermoplastic resin. More specifically, examples include, but are not limited to, polyimide, polyester, polypropylene, polyamide, polystyrene, polyvinyl chloride, polycarbonate and the like.

〈エンドプレート〉
エンドプレートは、全固体電池積層体を拘束できるものであれば、特に限定されず、例えば、金属又は炭素繊維強化プラスチックなど公知のものから構成されてもよい。 <end plate>
The end plate is not particularly limited as long as it can restrain the all-solid-state battery laminate, and may be made of a known one such as metal or carbon fiber reinforced plastic.

また、エンドプレートからの拘束力は、特に限定されず、必要とする全固体電池の使用用途や使用目的に合わせて、適宜設定できる。   Further, the binding force from the end plate is not particularly limited, and can be set as appropriate in accordance with the application and purpose of use of the required all solid battery.

１ａ、１ｂ、１ｃ、１ｄ 正極集電体層
２ａ、２ｂ、２ｃ、２ｄ 正極活物質層
３ａ、３ｂ、３ｃ、３ｄ 固体電解質層
４ａ、４ｂ、４ｃ、４ｄ 負極活物質層
５ａ、５ｂ、５ｃ、５ｄ 負極集電体層
６ａ、６ｂ、６ｃ、６ｄ 単位全固体電池
１０ 全固体電池積層体
１１ 樹脂層
１２ａ、１２ｂ エンドプレート
１ａｘ 正極集電体層１ａの端部
１ｄｘ 正極集電体層１ｄの端部
１００ 全固体電池 1a, 1b, 1c, 1d Positive electrode current collector layer 2a, 2b, 2c, 2d Positive electrode active material layer 3a, 3b, 3c, 3d Solid electrolyte layer 4a, 4b, 4c, 4d Negative electrode active material layer 5a, 5b, 5c, 5d negative electrode collector layer 6a, 6b, 6c, 6d unit all solid battery 10 all solid battery laminate 11 resin layer 12a, 12b end plate 1a x end portion of positive electrode collector layer 1a 1d x positive electrode collector layer 1d End 100 of the all-solid-state battery

Claims (1)

正極集電体層、正極活物質層、固体電解質層、負極活物質層、及び負極集電体層を、この順で積層してなる単位全固体電池を１以上有する全固体電池積層体と、
前記全固体電池積層体の側面を被覆している樹脂層と、
前記全固体電池積層体の両端面を積層方向に拘束している一対のエンドプレートと、
を有し、
前記全固体電池積層体の積層方向において、前記全固体電池積層体の厚さが、前記樹脂層の厚さよりも大きく、
前記一対のエンドプレートのそれぞれに隣接する前記正極集電体層及び／又は前記負極集電体層が、それぞれに隣接する前記正極活物質層及び／又は前記負極活物質層よりも大きい面積を有し、かつ
前記一対のエンドプレートのそれぞれに隣接する前記正極集電体層及び／又は前記負極集電体層の端部が、前記正極集電体層及び／又は前記負極集電体層に隣接するエンドプレートの反対側に向かって屈曲している屈曲周縁部を有する、
全固体電池。 An all solid battery laminate having at least one unit all solid battery formed by laminating a positive electrode current collector layer, a positive electrode active material layer, a solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer in this order;
A resin layer covering the side surface of the all solid battery laminate;
A pair of end plates constraining both end faces of the all-solid-state battery stack in the stacking direction;
Have
In the stacking direction of the all-solid-state battery stack, the thickness of the all-solid-state battery stack is larger than the thickness of the resin layer,
The positive electrode current collector layer and / or the negative electrode current collector layer adjacent to each of the pair of end plates have a larger area than the positive electrode active material layer and / or the negative electrode active material layer adjacent to each other. And an end portion of the positive electrode current collector layer and / or the negative electrode current collector layer adjacent to each of the pair of end plates is adjacent to the positive electrode current collector layer and / or the negative electrode current collector layer. Having a bending edge which is bent towards the opposite side of the
All solid state battery.
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