JP5265586B2 - Electrochemical devices - Google Patents
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Classifications
-
- 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
Description
本発明は、二次電池や電気二重層キャパシタ等の電気化学デバイスに関する。 The present invention relates to electrochemical devices such as secondary batteries and electric double layer capacitor.
例えば、携帯電話，デジタルスチルカメラ，ノートパソコン等の電気機器や、ハイブリッド電気自動車においては、リチウムイオン電池やニッケル水素電池等の二次電池、更に電気二重層キャパシタやレドックスキャパシタ等の電気化学キャパシタなどの、電荷を蓄積することができる、いわゆる電気化学デバイスが広く用いられている。 For example, in electric devices such as mobile phones, digital still cameras, laptop computers, and hybrid electric vehicles, secondary batteries such as lithium ion batteries and nickel metal hydride batteries, and electrochemical capacitors such as electric double layer capacitors and redox capacitors, etc. The so-called electrochemical devices capable of accumulating electric charges are widely used.
従来のこの種の電気化学デバイスとして、例えば、下記特許文献１には、本体部及びタブ部をそれぞれ有し、前記本体部同士が互いに対向するように配置された一対の集電板と、本体部及びタブ部を有し、前記本体部が前記一対の集電板の本体部間に配置されると共に前記タブ部が前記一対の集電板の本体部間から外にはみ出すように配置されたセパレータと、前記各集電板の本体部上にそれぞれ形成されて前記セパレータと接する活物質層と、前記各活物質層に接触する電解液と、前記各集電板のタブ部と前記セパレータのタブ部とを互いに固定する絶縁性の固定具と、を備える電気化学デバイスが開示されている。 As a conventional electrochemical device of this type, for example, in Patent Document 1 below, a pair of current collector plates each having a main body portion and a tab portion and arranged such that the main body portions face each other, and a main body And a tab portion, and the main body portion is disposed between the main body portions of the pair of current collector plates and the tab portion is disposed so as to protrude from between the main body portions of the pair of current collector plates. A separator, an active material layer formed on a main body portion of each current collector plate and in contact with the separator, an electrolyte solution in contact with each active material layer, a tab portion of each current collector plate, and a separator An electrochemical device is disclosed that includes an insulating fixture that secures the tab portions together.
また、下記特許文献２には、複数枚の正極板と負極板とが交互に積み重ねられ、隣り合う該正極板と該負極板との間にそれぞれ電気絶縁性のセパレータが介在されて成る積層型電池・キャパシタの電極を構成する積層型電池・キャパシタ用電極構造体であって、前記各セパレータは、前記正極板又は前記負極板が接触する接触部以外の部分に、該部分の一部を厚さ方向に変形させた突部から成る位置決め部を有し、該各セパレータの該突部が隣接する該セパレータの該突部の背後のくぼみに嵌入され、該位置決め部は各該セパレータ上において該正極板又は負極板を位置決めするとともに、隣接する該セパレータ同士を位置決めしている、ことを特徴とする積層型電池・キャパシタ用電極構造体が開示されている。 In Patent Document 2 below, a plurality of positive electrode plates and negative electrode plates are alternately stacked, and an electrically insulating separator is interposed between the adjacent positive electrode plates and the negative electrode plates. An electrode structure for a stacked battery / capacitor that constitutes an electrode of a battery / capacitor, wherein each of the separators has a portion thicker than a contact portion where the positive electrode plate or the negative electrode plate contacts. Each of the separators is inserted into a recess behind the adjacent protrusion of the separator, and the positioning portion is located on the separator. A multilayer battery / capacitor electrode structure is disclosed in which a positive electrode plate or a negative electrode plate is positioned and adjacent separators are positioned.
更に、下記特許文献３には、連続したシート状の集電体上に分極性電極を形成し、更に分極性電極をスリットにより分断した状態で、セパレータと積層するスーパーキャパシタの製造方法が開示されている。 Furthermore, Patent Document 3 below discloses a method for manufacturing a supercapacitor in which a polarizable electrode is formed on a continuous sheet-shaped current collector, and the polarizable electrode is further divided by a slit and laminated with a separator. ing.
しかしながら、上記特許文献１に記載された電気化学デバイスでは、各集電板のタブ部とセパレータのタブ部とを互いに固定する絶縁性の固定具を必要とするので、部品点数が多くなり、製造工程も複雑になるという問題点があった。 However, the electrochemical device described in Patent Document 1 requires an insulating fixture that fixes the tab portion of each current collector plate and the tab portion of the separator to each other. There was a problem that the process was also complicated.
また、上記特許文献２に記載された電気化学デバイスでは、セパレータに突部を形成して、隣接するセパレータどうしの突部を嵌合させる必要があるため、製造工程が煩雑になるという問題点があった。 Moreover, in the electrochemical device described in Patent Document 2, it is necessary to form protrusions on the separators and fit the protrusions between adjacent separators, so that the manufacturing process becomes complicated. there were.
更に、上記特許文献３に記載されたスーパーキャパシタの製造方法では、分極性電極を分断するスリットが、シートの一辺から形成されているので、ロールトゥロールで積層するときに、シートの左右両側を支持できず、シートを安定して保持できないという問題点があった。 Furthermore, in the manufacturing method of the supercapacitor described in the above-mentioned Patent Document 3, the slit for dividing the polarizable electrode is formed from one side of the sheet. There was a problem that the sheet could not be supported and the sheet could not be stably held.
したがって、本発明の目的は、電極とセパレータとを交互に積層したときに位置ずれが生じにくく、ロールトゥロールで製造することができる電気化学デバイスを提供することにある。 Accordingly, an object of the present invention is to provide an electrochemical device that is less likely to be displaced when electrodes and separators are alternately laminated and can be manufactured by roll-to-roll.
上記目的を達成するため、本発明の電気化学デバイスは、４枚以上の電極がセパレータを介して交互に積層され、各電極間に電解質が充填され、外周が封止体で覆われてなる電気化学デバイスにおいて、
各電極は、積層方向に沿って交互に極性が変わるように配置され、一方の極性の電極は上辺左側と下辺右側から突出する突出片を有し、他方の極性の電極は上辺右側と下辺左側から突出する突出片を有し、同じ極性の電極の前記突出片どうしが互いに整合し、当接して連結されており、
前記セパレータの前記各電極の突出片が位置する上下辺には、前記極性の異なる電極の突出片の間に位置する突出片が設けられており、
前記セパレータの上辺に設けられた突出片の先端から下辺に設けられた突出片の先端までの長さと、各電極の上辺に設けられた突出片の先端から下辺に設けられた突出片の先端までの長さとが同じであることを特徴とする。
In order to achieve the above object, the electrochemical device of the present invention is an electric device in which four or more electrodes are alternately laminated via separators, an electrolyte is filled between the electrodes, and the outer periphery is covered with a sealing body. In chemical devices,
Each electrode is arranged so that the polarity changes alternately along the stacking direction, one polarity electrode has projecting pieces projecting from the upper left side and the lower side right side, and the other polarity electrode is the upper side right side and the lower side left side The protruding pieces of electrodes of the same polarity are aligned with each other and connected in contact with each other,
Protruding pieces located between the protruding pieces of the electrodes having different polarities are provided on the upper and lower sides where the protruding pieces of the electrodes of the separator are located,
The length from the tip of the protruding piece provided on the upper side of the separator to the tip of the protruding piece provided on the lower side, and from the tip of the protruding piece provided on the upper side of each electrode to the tip of the protruding piece provided on the lower side The length of is the same .
本発明の電気化学デバイスによれば、一方の極性の電極の突出片どうしが当接して連結されることによって、それらの電極の間に位置する他方の極性の電極やセパレータが、一方の極性の電極によってたすき掛けされた状態で保持されることになる。同様に、他方の極性の電極の突出片どうしが当接して連結されることによって、それらの電極の間に位置する一方の極性の電極やセパレータが、他方の極性の電極によってたすき掛けされた状態で保持されることになる。したがって、製造工程の途中や製造後においても、積層された電極やセパレータがずれにくく、信頼性の高い電気化学デバイスを提供することができる。 According to the electrochemical device of the present invention, when the protruding pieces of one polarity electrode are in contact with each other and connected, the other polarity electrode or separator located between the electrodes becomes one polarity. It will be held in a state of being struck by the electrode. Similarly, the state protruding pieces with each other in the other polarity of the electrodes by being connected in contact with, one polarity of the electrodes and separators located between the electrodes is, that is crosswise with the other polarity of the electrodes Will be held at. Therefore, even during or after the manufacturing process, the stacked electrodes and separators are not easily displaced, and a highly reliable electrochemical device can be provided.
また、電極のシートを用いてロールトゥロールで製造する場合には、電極の突出片が連結帯で連結された形状となるように打抜いて、シートの両側を保持しながら供給することができ、シートを安定して供給することができる。 In addition, when manufacturing by roll-to-roll using an electrode sheet, it can be supplied by punching out the protruding pieces of the electrode into a shape connected by a connecting band and holding both sides of the sheet. The sheet can be supplied stably.
また、セパレータの前記各電極の突出片が位置する側にある一対の辺には、前記極性の異なる電極の突出片の間に位置する突出片が設けられているので、ロールトゥロールで製造する場合、セパレータのシートも、突出片が連結帯で連結された形状となるように打抜いて、シートの両側を保持しながら供給することができる。 In addition, the pair of sides on the side where the protruding pieces of the electrodes of the separator are located are provided with protruding pieces positioned between the protruding pieces of the electrodes having different polarities. In this case, the sheet of the separator can also be supplied while punching out so that the protruding pieces have a shape connected by the connecting band and holding both sides of the sheet.
本発明の電気化学デバイスにおいては、前記セパレータの上下の各辺に設けられた突出片どうしが、互いに整合して連結されていることが好ましい。これによれば、電極及びセパレータの動きをより制限して、互いの重なり位置のずれ防止効果を高めることができる。In the electrochemical device of the present invention, it is preferable that protruding pieces provided on the upper and lower sides of the separator are connected in alignment with each other. According to this, the movement of an electrode and a separator can be restrict | limited more, and the shift | offset | difference prevention effect of a mutual overlap position can be heightened.
本発明の電気化学デバイスにおいては、前記封止体には、前記電極の突出片の連結された部分を露出させる開口部が設けられていることが好ましい。これによれば、封止体の開口部から電極の突出片が露出して、電気化学デバイスの端子部を構成することができる。 In the electrochemical device of the present invention, it is preferable that the sealing body is provided with an opening that exposes a portion where the protruding pieces of the electrode are connected. According to this, the protruding piece of an electrode is exposed from the opening part of a sealing body, and the terminal part of an electrochemical device can be comprised.
また、前記電極は、前記突出片を有する形状の集電体と、その表面に形成された分極性電極とで構成され、前記分極性電極は、前記電極の極性の異なるものどうしで重なる部分に形成されていることが好ましい。これによれば、セパレータを介して複数の電極が積層された電気二重層キャパシタを提供することができる。 The electrode includes a current collector having a shape having the protruding piece and a polarizable electrode formed on a surface of the current collector, and the polarizable electrode overlaps with the electrodes having different polarities. Preferably it is formed. According to this, the electric double layer capacitor by which the some electrode was laminated | stacked through the separator can be provided.
本発明の電気化学デバイスは、リチウムイオン電池やニッケル水素電池等の二次電池、更に電気二重層キャパシタやレドックスキャパシタ等の電気化学キャパシタなどの、電荷を蓄積すると共に、その電荷を必要に応じて放出するためのもので、携帯電話，デジタルスチルカメラ，ノートパソコン等の電気機器や、ハイブリッド電気自動車等に、好適に利用される。 The electrochemical device of the present invention accumulates electric charges such as secondary batteries such as lithium ion batteries and nickel metal hydride batteries, and electrochemical capacitors such as electric double layer capacitors and redox capacitors. It is for discharge, and is suitably used for electric devices such as mobile phones, digital still cameras, notebook computers, and hybrid electric vehicles.
以下、本発明を電気化学デバイスの一種である電気化学キャパシタに適用した実施形態を挙げて説明する。図１〜６には、電気二重層キャパシタに適用した本発明の電気化学デバイスの一実施形態が示されている。 Hereinafter, an embodiment in which the present invention is applied to an electrochemical capacitor which is a kind of electrochemical device will be described. 1 to 6 show an embodiment of the electrochemical device of the present invention applied to an electric double layer capacitor.
図１に示すように、この電気化学デバイス１０は、一方の極性の電極板２１と、他方の極性の電極板２２とを、それらの間にセパレータ２３を介して交互に積層してなる積層物２０を有している。そして、この積層物２０の両側を更に封止体３１，３２で覆って構成されている。 As shown in FIG. 1, this electrochemical device 10 is a laminate in which one polarity electrode plate 21 and the other polarity electrode plate 22 are alternately laminated via separators 23 therebetween. 20. Then, both sides of the laminate 20 are further covered with sealing bodies 31 and 32.
図２を併せて参照すると、各電極２１，２２は、集電体２１ａ、２２ａと、その片面もしくは両面の所定の領域に形成された分極性電極２１ｂ、２２ｂとで構成されている。なお、最外側に配置された電極２１，２２には、その内側に位置する片面にのみ分極性電極２１ｂ、２２ｂが形成されており、中間に配置された電極２１，２２には、その両側に分極性電極２１ｂ、２２ｂが形成されている。また、一方の極性の電極２１の集電体２１ａには、図中上辺の左側と下辺の右側から突出する突出片２１ｃが形成されている。他方の極性の電極２２の集電体２２ａには、図中上辺の右側と下辺の左側から突出する突出片２２ｃが形成されている。 Referring also to FIG. 2, each of the electrodes 21 and 22 includes current collectors 21a and 22a and polarizable electrodes 21b and 22b formed in a predetermined region on one or both sides thereof. The electrodes 21 and 22 arranged on the outermost side are formed with polarizable electrodes 21b and 22b only on one side located on the inner side, and the electrodes 21 and 22 arranged on the middle are arranged on both sides thereof. Polarized electrodes 21b and 22b are formed. Further, the current collector 21a of the electrode 21 of one polarity is formed with a protruding piece 21c protruding from the left side of the upper side and the right side of the lower side in the figure. The current collector 22a of the other polarity electrode 22 is formed with protruding pieces 22c protruding from the right side of the upper side and the left side of the lower side in the figure.
上記集電体２１ａ、２２ａとしては、例えば金属箔、導電性ゴム、金属繊維シート、金属メッシュ等を用いることができ、その金属としては、アルミニウム，タンタル，ニオブ，チタン，ハフニウム，ジルコニウム，亜鉛，タングステン，ビスマス，アンチモン等の、いわゆるバルブ金属（弁金属、バルブメタルともいう）が好ましく用いられる。また、分極性電極２１ｂ、２２ｂとしては、表面積の大きな活性炭等の多孔質材料や、炭素繊維等が用いられる。なお、図１では、集電体２１ａ、２２ａと分極性電極２１ｂ、２２ｂとが離れた状態となっているが、実際には、分極性電極２１ｂ、２２ｂは、集電体２１ａ、２２ａの表面にコーティング等の手段によって付着形成されている。 As the current collectors 21a and 22a, for example, metal foil, conductive rubber, metal fiber sheet, metal mesh, and the like can be used. As the metal, aluminum, tantalum, niobium, titanium, hafnium, zirconium, zinc, So-called valve metals (also called valve metals or valve metals) such as tungsten, bismuth, and antimony are preferably used. For the polarizable electrodes 21b and 22b, a porous material such as activated carbon having a large surface area, carbon fiber, or the like is used. In FIG. 1, the current collectors 21a and 22a and the polarizable electrodes 21b and 22b are separated from each other, but actually, the polarizable electrodes 21b and 22b are formed on the surfaces of the current collectors 21a and 22a. It is attached and formed by means such as coating.
セパレータ２３は、極性の異なる一対の電極２１，２２の間に配置される。そして、上下辺の中央部に突出片２３ａを有している。セパレータ２３は、対向する一対の極性の異なる電極２１，２２どうしを絶縁すると共に、一対の電極２１，２２間の電解質中のイオンを移動可能とする部材であり、例えばポリエチレン、ポリテトラフルオロエチレン（ＰＴＦＥ）、セルロース、アラミド樹脂等、或いは、それらを混合させた多孔性ポリマーフィルムや不織布等で形成することができる。 The separator 23 is disposed between a pair of electrodes 21 and 22 having different polarities. And it has the protrusion piece 23a in the center part of the upper and lower sides. The separator 23 is a member that insulates a pair of opposing electrodes 21 and 22 having different polarities and allows ions in the electrolyte to move between the pair of electrodes 21 and 22. For example, polyethylene, polytetrafluoroethylene ( PTFE), cellulose, aramid resin, or the like, or a porous polymer film or a nonwoven fabric obtained by mixing them can be used.
図３は、上記電極２１，２２及びセパレータ２３を積層した積層物２０を示している。一方の極性の電極２１の突出片２１ｃは、上辺左側と下辺右側から突出し、他方の極性の電極２２の突出片２２ｃは、上辺右側と下辺左側から突出し、同じ極性の電極の突出片どうしは上下に整合している。また、セパレータ２３の突出片２３ａは、上下辺の中央から突出し、突出片２３ａどうしは上下に整合している。 FIG. 3 shows a laminate 20 in which the electrodes 21 and 22 and the separator 23 are laminated. The protruding piece 21c of one polarity electrode 21 protrudes from the upper left side and the lower right side, and the protruding piece 22c of the other polarity electrode 22 protrudes from the upper right side and the lower left side. Is consistent. Further, the protruding pieces 23a of the separator 23 protrude from the center of the upper and lower sides, and the protruding pieces 23a are aligned vertically.
図４は、上記電極２１，２２の上下に整合する突出片２１ｃ、２２ｃどうしを接合して連結した状態を示している。突出片２１ｃ、２２ｃどうしの接合は、例えば平行抵抗溶接、スポット溶接、超音波接合、レーザー溶接等の方法で行なうことができる。一方の極性の電極２１の突出片２１ｃどうしは、上辺左側と下辺右側とで連結されて、それらの間に位置する電極２２やセパレータ２３をたすき掛けにして斜めに囲んで保持する。他方の極性の電極２２の突出片２２ｃどうしは、上辺右側と下辺左側とで連結されて、それらの間に位置する電極２１やセパレータ２３を上記たすき掛けとは交差する方向のたすき掛けにして斜めに囲んで保持する。電極２１、２２の突出片２１ｃ、２２ｃを上記のように連結することによって、電極２１、２２及びセパレータ２３の積層状態が安定して保持され、それぞれの重なり位置がずれることを防止できる。 FIG. 4 shows a state in which the projecting pieces 21c and 22c aligned on the upper and lower sides of the electrodes 21 and 22 are joined and connected. The protruding pieces 21c and 22c can be joined to each other by a method such as parallel resistance welding, spot welding, ultrasonic joining, or laser welding. The protruding pieces 21c of the electrodes 21 of one polarity are connected to each other at the upper left side and the lower right side, and hold the electrode 22 and the separator 23 positioned between them obliquely. The protruding pieces 22c of the electrode 22 of the other polarity are connected to each other on the upper right side and the lower left side, and the electrodes 21 and the separator 23 located between them are slanted in a direction crossing the above slack. Enclose and hold. By connecting the protruding pieces 21c and 22c of the electrodes 21 and 22 as described above, the stacked state of the electrodes 21 and 22 and the separator 23 can be stably maintained, and the respective overlapping positions can be prevented from shifting.
なお、電極２１，２２の上下に整合する突出片２１ｃ、２２ｃどうしを接合するだけでなく、セパレータ２３の突出片２３ａどうしを接合してもよい。セパレータ２３の突出片２３ａどうしを接合することにより、電極２１、２２及びセパレータ２３の動きをより制限して、互いの重なり位置のずれ防止効果を高めることができる。 Not only the protruding pieces 21c and 22c aligned on the upper and lower sides of the electrodes 21 and 22 but also the protruding pieces 23a of the separator 23 may be bonded. By joining the protruding pieces 23 a of the separator 23, the movement of the electrodes 21, 22 and the separator 23 can be further restricted, and the effect of preventing the displacement of the overlapping positions can be enhanced.
図５，６は、封止体３１、３２で上記積層物２０を被覆した状態を示し、図５は図４のＡ−Ａ’矢示線に沿った断面図、図６は図４のＢ−Ｂ’矢示線に沿った断面図である。各電極２１，２２はセパレータ２３を介して対向配置され、その対向する内面にそれぞれ分極性電極２１ｂ、２２ｂが形成されている。一方の極性の電極２１の突出片２１ｃは、図６に示すように、その下辺右側で連結された部分が封止体３１の開口部３３の下方に位置し、開口部３３を通して露出した端子をなしている。また、他方の極性の電極２２の突出片２２ｃは、図５に示すように、その下辺左側で連結された部分が封止体３１のもう１つの開口部３３の下方に位置し、開口部３３を通して露出した端子をなしている。なお、図５、６では、開口部３３と各端子部をなす突出片２１ｃ、２２ｃとが離れた状態となっているが、実際には、電極２１，２２及びセパレータ２３は薄いシートからなるので、開口部３３の内側内周が、対応する突出片２１ｃ、２２ｃに密接した状態となっている。この場合、封止体３１の開口部３３の内周を、突出片２１ｃ、２２ｃに接着又は溶着させることもできる。また、もう一方の封止体３２に開口部３４，３４を設けることもでき、突出片２１ｃを一方の封止体３１又は３２の開口部から露出させ、突出片２２ｃを他方の封止体３２又は３１の開口部から露出させることもできる。更に、封止体３１，３２に開口部を設けることなく、突出片２１ｃ、２２ｃを封止体３１，３２の接合部端縁から突出させて端子とすることもできる。 5 and 6 show a state in which the laminate 20 is covered with the sealing bodies 31 and 32, FIG. 5 is a cross-sectional view taken along the line AA 'in FIG. 4, and FIG. -B 'is a cross-sectional view along the arrow line. The electrodes 21 and 22 are disposed to face each other with the separator 23 interposed therebetween, and polarizable electrodes 21b and 22b are formed on the facing inner surfaces, respectively. As shown in FIG. 6, the protruding piece 21 c of one polarity electrode 21 has a terminal connected to the right side of the lower side located below the opening 33 of the sealing body 31, and a terminal exposed through the opening 33. There is no. Further, as shown in FIG. 5, the protruding piece 22 c of the other polarity electrode 22 is located below the other opening 33 of the sealing body 31, and the opening connected to the left side of the lower side is located in the opening 33. Through the exposed terminal. In FIGS. 5 and 6, the opening 33 and the protruding pieces 21c and 22c forming the terminal portions are separated from each other, but actually, the electrodes 21 and 22 and the separator 23 are made of a thin sheet. The inner periphery of the opening 33 is in close contact with the corresponding protruding pieces 21c and 22c. In this case, the inner periphery of the opening 33 of the sealing body 31 can be bonded or welded to the protruding pieces 21c and 22c. Moreover, the opening parts 34 and 34 can also be provided in the other sealing body 32, the protrusion piece 21c is exposed from the opening part of one sealing body 31 or 32, and the protrusion piece 22c is the other sealing body 32. Or it can also be exposed from the opening part of 31. Furthermore, without providing an opening in the sealing bodies 31 and 32, the projecting pieces 21 c and 22 c can be projected from the joint edge of the sealing bodies 31 and 32 to serve as terminals.
封止体３１，３２としては、非透湿性と十分な強度を有するものであればよく、特に限定されないが、例えば、金属箔をラミネートされた合成樹脂フィルムなどが好ましく使用される。金属箔としては、アルミニウム等が好ましく、合成樹脂フィルムとしては、例えばポリプロピレン、ナイロン、ポリエチレンテレフタレート（ＰＥＴ）、ポリエチレン、エチレン酢酸ビニル共重合樹脂、あるいはこれらの積層物（例えば、ナイロンをベース材とし、シーラントとしてポリプロピレンを積層させ、これらをポリエチレンテレフタレートや、ポリエチレン、エチレン酢酸ビニル共重合樹脂等で挟み込んだ構成）が好ましく用いられる。封止体３１，３２どうしを熱溶着によって接合する場合には、少なくとも内面に熱溶着可能な樹脂層が設けられるようにすることが好ましい。 The sealing bodies 31 and 32 are not particularly limited as long as they have non-moisture permeability and sufficient strength. For example, a synthetic resin film laminated with a metal foil is preferably used. As the metal foil, aluminum or the like is preferable, and as the synthetic resin film, for example, polypropylene, nylon, polyethylene terephthalate (PET), polyethylene, ethylene vinyl acetate copolymer resin, or a laminate thereof (for example, nylon as a base material, A configuration in which polypropylene is laminated as a sealant and these are sandwiched between polyethylene terephthalate, polyethylene, ethylene vinyl acetate copolymer resin, or the like is preferably used. When the sealing bodies 31 and 32 are joined together by thermal welding, it is preferable that a resin layer that can be thermally welded is provided at least on the inner surface.
封止体３１，３２で積層物２０を封止する前に、積層物２０の各電極２１，２２の間に電解質が充填される。電解質としては、特に限定されないが、例えばテトラエチルアンモニウムテトラフルオロボレート（Ｅｔ４ＮＢＦ４）や、下式（ｉ）で示される化合物等が採用される。 Before sealing the laminate 20 with the sealing bodies 31 and 32, the electrolyte is filled between the electrodes 21 and 22 of the laminate 20. The electrolyte is not particularly limited. For example, tetraethylammonium tetrafluoroborate (Et 4 NBF 4 ), a compound represented by the following formula (i), or the like is employed.
［Ｒ１Ｒ２Ｒ３Ｒ４Ｎ］＋Ｘ−・・・（ｉ）
（式中、Ｒ１〜Ｒ４は、不飽和結合，エーテル結合，アミド結合，又はエステル結合を有してもよい炭素数１〜６のアルキル基、又は、分子中に窒素原子を有してもよい炭素数４〜６のシクロアルキル基を表し、Ｘ−は、ＣｌＯ４ −、ＢＦ４ −、ＰＦ６ −、（ＣＦ３ＳＯ２）２Ｎ−、ＣＦ３ＳＯ４ −、Ｃ２Ｆ５ＳＯ４ −のような陰イオンを表す。）
上記電解質がプロピレンカーボネート（ＰＣ）、アセトニトリル、メトキシアセトニトリル、３−メトキシプロピオニトリル、γ−ブチロラクトン、ブチレンカーボネート、ジメチルカーボネート、エチルメチルカーボネート、エチレンカーボネート、スルホラン、３−メチルスルホラン等の溶媒により溶解されることにより、電解液が形成されて、これが極性の異なる一対の電極２１，２２間に充填されるようになっている。なお、弗素を含む電解質は、水分が侵入すると弗酸を生じ、集電体２１ａ，２２ａを腐食させる虞れがあるため、封止体３１，３２で厳密に封入する必要がある。
[R 1 R 2 R 3 R 4 N] + X − (i)
(Wherein, R 1 to R 4 is an unsaturated bond, ether bond, amide bond, or ester bond to be of good 1 to 6 carbon atoms having alkyl group, or, a nitrogen atom in the molecule Represents a C 4-6 cycloalkyl group, and X − represents ClO 4 − , BF 4 − , PF 6 − , (CF 3 SO 2 ) 2 N − , CF 3 SO 4 − , C 2 F 5. sO 4 - represents an anion such as).
The above electrolyte is dissolved in a solvent such as propylene carbonate (PC), acetonitrile, methoxyacetonitrile, 3-methoxypropionitrile, γ-butyrolactone, butylene carbonate, dimethyl carbonate, ethyl methyl carbonate, ethylene carbonate, sulfolane, 3-methyl sulfolane. Thus, an electrolytic solution is formed and filled between the pair of electrodes 21 and 22 having different polarities. Note that the electrolyte containing fluorine needs to be strictly sealed with the sealing bodies 31 and 32 because hydrofluoric acid may be generated when moisture enters and the current collectors 21a and 22a may be corroded.
こうして得られた電気化学デバイス（この実施形態では電気二重層キャパシタ）１０は、突出片２１ｃ、２２ｃが露出した端子部に正負の電圧を印加することにより、表面積の大きな活性炭等の多孔質材料や、炭素繊維等からなる分極性電極２１ｂ、２２ｂの表面に、正極の場合には負のイオンが集積し、負極の場合には正のイオンが集積して、電気二重層が形成され、容量の大きなキャパシタとして作用するので、充放電可能な電池として利用することができる。 The electrochemical device 10 thus obtained (electric double layer capacitor in this embodiment) is made of a porous material such as activated carbon having a large surface area by applying positive and negative voltages to the terminal portions where the protruding pieces 21c and 22c are exposed. In the case of the positive electrode, negative ions are accumulated on the surfaces of the polarizable electrodes 21b and 22b made of carbon fiber or the like, and in the case of the negative electrode, positive ions are accumulated to form an electric double layer. Since it acts as a large capacitor, it can be used as a chargeable / dischargeable battery.
次に、図７，８を参照して、上記電気化学デバイス１０の製造方法について説明する。 Next, a method for manufacturing the electrochemical device 10 will be described with reference to FIGS.
図７において、４１は、一方の極性の電極２１の集電体２１ａを形成するための第１集電体シート４１ａを巻いた第１集電体ロールであり、４２は、他方の極性の電極２２の集電体２２ａを形成するための第２集電体シート４２ａを巻いた第２集電体ロールであり、４３は、セパレータ２３を形成するためのセパレータシート４３ａを巻いたセパレータロールである。この実施形態では、２つの第１集電体ロール４１と、２つの第２集電体ロール４２と、３つのセパレータロール４３が用いられる。 In FIG. 7, 41 is the 1st collector roll which wound the 1st collector sheet 41a for forming the collector 21a of the electrode 21 of one polarity, and 42 is an electrode of the other polarity 22 is a second current collector roll wound with a second current collector sheet 42a for forming a current collector 22a, and 43 is a separator roll wound with a separator sheet 43a for forming a separator 23. . In this embodiment, two first current collector rolls 41, two second current collector rolls 42, and three separator rolls 43 are used.
第１集電体ロール４１から引き出された第１集電体シート４１ａ、及び第２集電体ロール４２から引き出された第２集電体シート４２ａには、その幅方向中央部に表面積の大きな活性炭等の多孔質材料や、炭素繊維等からなる分極性電極２１ｂ、２２ｂが塗布形成される。この場合、積層体２０の中間部に配置される第１集電体シート４１ａ、第２集電体シート４２ａには、その両面に分極性電極２１ｂ、２２ｂが形成され、外側に配置される第１集電体シート４１ａ、第２集電体シート４２ａには、その内面にのみ分極性電極２１ｂ、２２ｂが形成される。また、セパレータロール４３から引き出されたセパレータシート４３ａは、第１集電体シート４１ａと第２集電体シート４２ａとの間に配置される。 The first current collector sheet 41a drawn from the first current collector roll 41 and the second current collector sheet 42a drawn from the second current collector roll 42 have a large surface area at the center in the width direction. Polarizing electrodes 21b and 22b made of a porous material such as activated carbon or carbon fiber are applied and formed. In this case, polarizable electrodes 21b and 22b are formed on both surfaces of the first current collector sheet 41a and the second current collector sheet 42a disposed in the intermediate portion of the laminate 20, and the first current collector sheet 41a and the second current collector sheet 42a are disposed on the outer sides. Polarizable electrodes 21b and 22b are formed only on the inner surfaces of the first current collector sheet 41a and the second current collector sheet 42a. Further, the separator sheet 43a pulled out from the separator roll 43 is disposed between the first current collector sheet 41a and the second current collector sheet 42a.
そして、第１集電体シート４１ａは金型５１により、第２集電体シート４２ａは金型５２により、更にセパレータシート４３ａは金型５３により、それぞれ図示する形状となるように打抜き成形される。 The first current collector sheet 41a is stamped and formed into a shape as shown in the figure by the mold 51, the second current collector sheet 42a by the mold 52, and the separator sheet 43a by the mold 53. .
こうして成形された各シート４１ａ、４２ａ、４３ａを、図示するように積層する。なお、図示を省略したが、実際には、最上層の第２集電体シート４２ａの外側には、更に封止体３１を形成するシートが配置され、最下層の第１集電体シート４１ａの外側には，封止体３２を形成するシートが配置されて、上記各シート４１ａ、４２ａ、４３ａの積層物の外側を覆うようになっている。 The sheets 41a, 42a, 43a thus formed are stacked as shown. Although illustration is omitted, actually, a sheet for forming the sealing body 31 is further arranged outside the uppermost second current collector sheet 42a, and the lowermost first current collector sheet 41a. The sheet | seat which forms the sealing body 32 is arrange | positioned on the outer side of this, and the outer side of the laminated body of said each sheet | seat 41a, 42a, 43a is covered.
図８（ａ）に示すように、例えば金型５２により打抜き成形された第２集電体シート４２ａは、集電体２２ａと、その上辺右側に突出する突出片２２ｃと、下辺左側に突出する突出片２２ｃとを有し、各突出片２２ｃが連結帯４４によって連結された形状をなしている。そして、連結帯４４には、シートを位置制御しつつ送るための送り孔４５が所定間隔で形成されている。第１集電体シート４１ａ及びセパレータシート４３においても同様であり、それぞれの突出片２１ｃ、２３ａが連結帯４４によって連結され、連結帯４４に設けられた送り孔４５によって位置制御しつつ送られるようになっている。このように、本発明においては、各シート４１ａ、４２ａ、４３ａの両側を連結帯４４によって支持しつつ搬送するので、安定して搬送できると共に、正確に位置合わせすることができる。この状態で、上下に整合する突出片２１ｃ、２２ｃを、平行抵抗溶接、スポット溶接、超音波接合、レーザー溶接等の方法で接合する。 As shown in FIG. 8 (a), for example, the second current collector sheet 42a stamped and formed by the mold 52 projects the current collector 22a, the protruding piece 22c protruding to the upper right side thereof, and the left side of the lower edge protruding. And each protruding piece 22c is connected by a connecting band 44. In the connection band 44, feed holes 45 for feeding the sheet while controlling the position thereof are formed at predetermined intervals. The same applies to the first current collector sheet 41 a and the separator sheet 43, and the protruding pieces 21 c and 23 a are connected by the connection band 44, and are sent while being controlled in position by the feed holes 45 provided in the connection band 44. It has become. As described above, in the present invention, since both sides of each of the sheets 41a, 42a, 43a are conveyed while being supported by the connection band 44, they can be stably conveyed and can be accurately aligned. In this state, the projecting pieces 21c and 22c aligned vertically are joined by a method such as parallel resistance welding, spot welding, ultrasonic joining, laser welding or the like.
そして、図示しない封止体３１、３２を形成するシートを積層物の外側に被せて覆った後、図８（ａ）の想像線Ａ，Ｂでカットすることにより、図８（ｂ）に示すような積層体２０が形成され、個々のデバイスに分離することができる。なお、電解質は、個々のデバイスに分離する前に充填してもよく、個々のデバイスに分離した後に充填してもよい。そして、電解質を充填した後、封止体３１，３２を封止し、個々のデバイスに分離する前であれば、個々のデバイスに分離して、電気化学デバイス１０を製造することができる。 And after covering the sheet | seat which forms the sealing bodies 31 and 32 which are not shown in figure on the outer side of a laminated body, it cuts by the imaginary lines A and B of Fig.8 (a), and shows in FIG.8 (b). Such a laminate 20 can be formed and separated into individual devices. The electrolyte may be filled before being separated into individual devices, or may be filled after being separated into individual devices. Then, after filling the electrolyte, before the sealing bodies 31 and 32 are sealed and separated into individual devices, the electrochemical device 10 can be manufactured by separating into individual devices.
このように、本発明の電気化学デバイス１０は、ロールトゥロールで各シートを安定して供給し、正確に位置合わせして積層し、作業性よく製造することができる。 Thus, the electrochemical device 10 of the present invention can be manufactured with good workability by supplying each sheet stably by roll-to-roll, accurately aligning and laminating.
図７，８に示される製造方法により、図１〜６に示される電気化学デバイス（電気二重層キャパシタ）を製造した。 The electrochemical device (electric double layer capacitor) shown in FIGS. 1 to 6 was manufactured by the manufacturing method shown in FIGS.
各集電体シート４１ａ、４２ａとしては、厚さ２２μｍのアルミ箔（東洋アルミ製）を用いた。このシートを図７の金型５１，５２で打抜き、最終的には図８で示すように分離して、２３．５ｍｍ×１５ｍｍの集電体２１ａ、２２ａとなるようにした。なお、集電体の突出片２１ｃ、２２ｃの大きさは３．５×４ｍｍとした。 As each current collector sheet 41a, 42a, an aluminum foil (made by Toyo Aluminum) having a thickness of 22 μm was used. This sheet was punched out with the molds 51 and 52 of FIG. 7, and finally separated as shown in FIG. 8 so as to become current collectors 21a and 22a of 23.5 mm × 15 mm. In addition, the size of the protruding pieces 21c and 22c of the current collector was 3.5 × 4 mm.
セパレータシート４３ａとしては、無機フィラーを含有するポリオレフィンからなる多孔質ポリオレフィンフィルム（日本板硝子製）を用いた。このシートを図７の金型５３で打抜き、２３．５ｍｍ×１６ｍｍのセパレータ２３となるようにした。なお、セパレータの突出片２３ａの大きさは３×４ｍｍとした。 As the separator sheet 43a, a porous polyolefin film (manufactured by Nippon Sheet Glass) made of polyolefin containing an inorganic filler was used. This sheet was punched with a mold 53 shown in FIG. 7 so as to be a 23.5 mm × 16 mm separator 23. The size of the separator protruding piece 23a was 3 × 4 mm.
封止材３１，３２としては、２５μｍ厚ナイロン／４０μｍ厚アルミ／４０μｍ厚ポリプロピレンからなる厚さ１０５μｍのアルミラミネートフィルムを用いた。このシートを３２ｍｍ×２４ｍｍの大きさに打抜いて、各封止材３１，３２とした。 As the sealing materials 31 and 32, 105 μm thick aluminum laminate films made of 25 μm thick nylon / 40 μm thick aluminum / 40 μm thick polypropylene were used. This sheet was punched into a size of 32 mm × 24 mm to obtain the sealing materials 31 and 32.
分極性電極は、多孔性炭素：エラストマーバインダー：カーボンブラック：カルボキシメチルセルロースを１００：３：５：２の質量比で混練し、これに水を加えてペースト濃度を３７％としたペーストを作成し、このペーストを上記集電体２１ａ、２２ａの片面又は両面に１６．５ｍｍ×１５ｍｍ×０．１ｍｍの層となるように塗布して形成した。 The polarizable electrode was prepared by kneading porous carbon: elastomer binder: carbon black: carboxymethylcellulose at a mass ratio of 100: 3: 5: 2 and adding water to this to make a paste concentration of 37%. The paste was applied and formed on one or both sides of the current collectors 21a and 22a so as to form a layer of 16.5 mm × 15 mm × 0.1 mm.
こうして形成した各シートを積層し、上下に整合する突出片２１ｃ、２２ｃどうしを溶接し、内部に有機電解液「パワーエレック」（商品名、三洋化成製）を充填し、封止体３１，３２で封止して、電気化学デバイス（電気二重層キャパシタ）を得た。 The sheets thus formed are stacked, the protruding pieces 21c and 22c aligned vertically are welded to each other, and the inside is filled with an organic electrolyte “Power Elec” (trade name, manufactured by Sanyo Kasei Co., Ltd.). To obtain an electrochemical device (electric double layer capacitor).
こうして得た電気化学デバイス（電気二重層キャパシタ）について、静電容量をＥＩＡＪ ＲＣ−２３７７に記載の定電流放電法により測定した。また、等価直列抵抗をＥＩＡＪ ＲＣ−２３７７に記載の交流インビーダンス測定法により測定した。 About the electrochemical device (electric double layer capacitor) thus obtained, the capacitance was measured by a constant current discharge method described in EIAJ RC-2377. Moreover, the equivalent series resistance was measured by the alternating current impedance measuring method described in EIAJ RC-2377.
その結果、静電容量は１．６Ｆ、等価直列抵抗（１ｋＨｚ）は５３０ｍΩであった。 As a result, the capacitance was 1.6 F, and the equivalent series resistance (1 kHz) was 530 mΩ.
１０ 電気化学デバイス
２０ 積層物
２１ 一方の極性の電極
２１ａ 集電体
２１ｂ 分極性電極
２１ｃ 突出片
２２ 一方の極性の電極
２２ａ 集電体
２２ｂ 分極性電極
２２ｃ 突出片
２３ セパレータ
２３ａ 突出片
３１，３２ 封止体
３３、３４ 開口部
４１ 第１集電体ロール
４１ａ 第１集電体シート
４２ 第２集電体ロール
４２ａ 第２集電体シート
４３ セパレータロール
４３ａ セパレータシート
４４ 連結帯
４５ 送り孔
DESCRIPTION OF SYMBOLS 10 Electrochemical device 20 Laminate 21 Electrode 21a of one polarity Current collector 21b Polarized electrode 21c Projection piece 22 Electrode 22a of one polarity Current collector 22b Polarization electrode 22c Projection piece 23 Separator 23a Projection piece 31, 32 Sealing Stops 33, 34 Opening 41 First current collector roll 41a First current collector sheet 42 Second current collector roll 42a Second current collector sheet 43 Separator roll 43a Separator sheet 44 Connection band 45 Feed hole
Claims (4)
各電極は、積層方向に沿って交互に極性が変わるように配置され、一方の極性の電極は上辺左側と下辺右側から突出する突出片を有し、他方の極性の電極は上辺右側と下辺左側から突出する突出片を有し、同じ極性の電極の前記突出片どうしが互いに整合し、当接して連結されており、
前記セパレータの前記各電極の突出片が位置する上下辺には、前記極性の異なる電極の突出片の間に位置する突出片が設けられており、
前記セパレータの上辺に設けられた突出片の先端から下辺に設けられた突出片の先端までの長さと、各電極の上辺に設けられた突出片の先端から下辺に設けられた突出片の先端までの長さとが同じであることを特徴とする電気化学デバイス。 In an electrochemical device in which four or more electrodes are alternately stacked via separators, an electrolyte is filled between the electrodes, and the outer periphery is covered with a sealing body.
Each electrode is arranged so that the polarity changes alternately along the stacking direction, one polarity electrode has projecting pieces projecting from the upper left side and the lower side right side, and the other polarity electrode is the upper side right side and the lower side left side The protruding pieces of electrodes of the same polarity are aligned with each other and connected in contact with each other,
Protruding pieces located between the protruding pieces of the electrodes having different polarities are provided on the upper and lower sides where the protruding pieces of the electrodes of the separator are located,
The length from the tip of the protruding piece provided on the upper side of the separator to the tip of the protruding piece provided on the lower side, and from the tip of the protruding piece provided on the upper side of each electrode to the tip of the protruding piece provided on the lower side Electrochemical device characterized by having the same length .
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