TWI389373B - Lead member,process for producing the same and non-aqueous electrolyte accumulation device - Google Patents
Lead member,process for producing the same and non-aqueous electrolyte accumulation device Download PDFInfo
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- TWI389373B TWI389373B TW097127249A TW97127249A TWI389373B TW I389373 B TWI389373 B TW I389373B TW 097127249 A TW097127249 A TW 097127249A TW 97127249 A TW97127249 A TW 97127249A TW I389373 B TWI389373 B TW I389373B
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- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
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- H01M50/10—Primary casings, jackets or wrappings of a single cell or a single battery
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- H01M50/10—Primary casings, jackets or wrappings of a single cell or a single battery
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- H01M50/131—Primary casings, jackets or wrappings of a single cell or a single battery characterised by physical properties, e.g. gas-permeability or size
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- H01M50/50—Current conducting connections for cells or batteries
- H01M50/543—Terminals
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- H01M50/55—Terminals characterised by the disposition of the terminals on the cells on the same side of the cell
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- H01M50/50—Current conducting connections for cells or batteries
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- H01M10/00—Secondary cells; Manufacture thereof
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- H01M10/052—Li-accumulators
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- H01M50/116—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material
- H01M50/124—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material having a layered structure
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- Y02E60/10—Energy storage using batteries
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Description
本發明關於非水電解質蓄電裝置所使用的引線構件及其製法，以及使用其的非水電解質蓄電裝置。The present invention relates to a lead member used in a nonaqueous electrolyte electricity storage device, a method for producing the same, and a nonaqueous electrolyte electricity storage device using the same.
隨著電子機器的小型化，要求作為電源的電池之小型化、輕量化。又，亦要求高能量密度化、高能量效率化，作為滿足如此要求者，對於鋰離子電池等的非水電解質電池之期待係愈來愈高。作為非水電解質電池，已知有將正極、負極及電解液收納在由含金屬箔層的多層薄膜所成的封入袋內，將連接於正極、負極的電極板之引線導體取出到外部的構造者(例如參照專利文獻1)。With the miniaturization of electronic equipment, it is required to reduce the size and weight of batteries as power sources. In addition, high energy density and high energy efficiency are required, and as such a requirement, the expectation of a nonaqueous electrolyte battery such as a lithium ion battery is increasing. As a non-aqueous electrolyte battery, a structure in which a positive electrode, a negative electrode, and an electrolytic solution are housed in a sealed bag made of a multilayer film containing a metal foil layer, and a lead conductor connected to an electrode plate of a positive electrode or a negative electrode is taken out to the outside is known. (For example, refer to Patent Document 1).
第4(A)圖、第4(B)圖及第5圖係上述專利文獻1中所揭示的非水電解質電池之概略圖。此非水電解質電池係由一對引線1a、1b之取出部分各自被絕緣體3a、3b所覆蓋，由封入袋6的密封部分14取出到外部的形態之薄形構造所形成。封入袋6的周緣部之密封部分14係經由熱封而熱熔黏成為袋狀。於封入袋6內中，密封收納正極、負極、隔膜等與溶解在非水溶劑(例如有機溶劑)中的電解質(例如鋰化合物)之非水電解質介質。The fourth (A), fourth (B), and fifth drawings are schematic views of the nonaqueous electrolyte battery disclosed in Patent Document 1. This nonaqueous electrolyte battery is formed by a thin structure in which the taken-out portions of the pair of leads 1a and 1b are covered by the insulators 3a and 3b and are taken out to the outside by the sealing portion 14 of the sealed bag 6. The sealing portion 14 of the peripheral portion of the sealing bag 6 is thermally fused and formed into a bag shape by heat sealing. In the sealed bag 6, a nonaqueous electrolyte medium containing an electrolyte (for example, a lithium compound) dissolved in a nonaqueous solvent (for example, an organic solvent) such as a positive electrode, a negative electrode, or a separator is sealed.
第4(A)圖顯示第5圖之a-a箭號方向的截面。非水電解質電池係將正極11a及負極11b、隔膜12、非水電解介質13等收納於袋狀的封入袋6內，使連接於正極11a、負極11b的引線(引線構件)1a、1b成為密封狀態，取出到外 部的構造者。封入袋6係使用由在最內層薄膜7與最外層薄膜9之間，以三明治狀貼合至少由鋁等的金屬所成的金屬箔層8而成的密封性高之多層薄膜10所形成。Fig. 4(A) shows a section in the direction of the arrow a-a in Fig. 5. In the non-aqueous electrolyte battery, the positive electrode 11a and the negative electrode 11b, the separator 12, the non-aqueous electrolytic medium 13, and the like are housed in a bag-shaped sealed bag 6, and the leads (lead members) 1a and 1b connected to the positive electrode 11a and the negative electrode 11b are sealed. State, taken out The constructor of the ministry. The sealing bag 6 is formed of a multilayer film 10 having a high sealing property, which is formed by sandwiching a metal foil layer 8 made of a metal such as aluminum between the innermost film 7 and the outermost film 9 in a sandwich shape. .
而且，於裁切成矩形狀的2片多層薄膜10之周邊的密封部分14，將最內層薄膜7彼此互相熔黏密封以成為袋狀的封入袋6。連接於正極11a、負極11b的引線之引線導體2a、2b係被絕緣體3a、3b所覆蓋，以便其取出部分對多層薄膜10的金屬箔層8不發生電性短路。絕緣體3a、3b係接著及密封於封入袋6的指定緣部。Further, in the sealing portion 14 around the two multilayer films 10 cut into a rectangular shape, the innermost film 7 is welded to each other to form a bag-shaped sealing bag 6. The lead conductors 2a and 2b connected to the leads of the positive electrode 11a and the negative electrode 11b are covered by the insulators 3a and 3b so that the taken-out portion does not electrically short the metal foil layer 8 of the multilayer film 10. The insulators 3a and 3b are then sealed and sealed to a predetermined edge of the envelope bag 6.
覆蓋此引線導體2a、2b的取出部分之絕緣體3a、3b，係如第4(A)圖的b-b箭號方向之截面圖的第4(B)圖所示地，例如，由貼合有由馬來酸酐改性低密度聚乙烯或馬來酸酐改性低密度聚丙烯等的聚烯烴樹脂所成的熱塑性樹脂薄膜所形成的熱塑性層4、與由經交聯的低密度聚乙烯等的聚烯烴樹脂所成的交聯樹脂薄膜所形成的交聯層5之2層所形成。The insulators 3a and 3b covering the extraction portions of the lead conductors 2a and 2b are as shown in Fig. 4(B) of the cross-sectional view in the direction of the bb arrow in Fig. 4(A), for example, by bonding A thermoplastic resin film formed of a polyolefin resin such as a maleic anhydride-modified low-density polyethylene or a maleic anhydride-modified low-density polypropylene, and a thermoplastic resin film formed of a low-density polyethylene or the like Two layers of the crosslinked layer 5 formed of the crosslinked resin film formed of the olefin resin are formed.
此絕緣體3a、3b係在引線的引線導體2a、2b之取出部分，預先將絕緣體3a、3b的熱塑性層4加熱熔融而使密封接著後，夾入封入袋6的取出口內。然後，以熱封來封閉多層薄膜10的周邊之密封部分14。絕緣體3a、3b的交聯層5，因為係由在其熱封時的溫度不易熔融變形的材料所形成，故熱封之後，在引線的引線導體2a、2b與多層薄膜內的金屬箔層8之間，交聯層5殘留著，因此不必擔心引線導體2a、2b與金屬箔層8的電性短路。The insulators 3a and 3b are attached to the lead conductors 2a and 2b of the lead wires, and the thermoplastic layer 4 of the insulators 3a and 3b is heated and melted in advance to be sealed, and then inserted into the outlet of the sealing bag 6. Then, the sealing portion 14 of the periphery of the multilayer film 10 is sealed by heat sealing. The crosslinked layer 5 of the insulators 3a, 3b is formed of a material which is not easily melt-deformed by the temperature at the time of heat sealing, so after the heat sealing, the lead conductors 2a, 2b of the lead and the metal foil layer 8 in the multilayer film Between the crosslinked layers 5 remains, there is no need to worry about electrical shorting of the lead conductors 2a, 2b and the metal foil layer 8.
又，正極11a及負極11b係在稱為集電體的金屬箔或金屬網等的金屬基材上形成有活性物質層的構造，引線導體2a、2b係連接於電極基材之電極板。此連接係可利用點焊或超音波熔接等。Further, the positive electrode 11a and the negative electrode 11b have a structure in which an active material layer is formed on a metal substrate such as a metal foil or a metal mesh called a current collector, and the lead conductors 2a and 2b are connected to an electrode plate of the electrode substrate. This connection can utilize spot welding or ultrasonic welding or the like.
專利文獻1：日本發明公開：特開2001-102016號公報Patent Document 1: Japanese Invention Disclosure: JP-A-2001-102016
設於引線導體2a、2b之取出部分的絕緣體3a、3b，通常如第4圖所說明地，係由貼合用於形成熱塑性層4的熱塑性樹脂薄膜與用於形成交聯層5的交聯樹脂薄膜所形成。此等樹脂薄膜係難以薄地擠壓成形，通常貼合以50μm左右之厚度所形成的熱塑性樹脂薄膜與交聯樹脂薄膜，厚度之合計成為100μm左右。絕緣體的厚度若厚，則引線的柔軟性係不充分，在絕緣體之邊端與多層薄膜之間會形成間隙，引線與封入袋的閉封係不充分，水分會侵入封入袋內。The insulators 3a, 3b provided at the take-out portions of the lead conductors 2a, 2b are generally bonded as shown in Fig. 4 by laminating a thermoplastic resin film for forming the thermoplastic layer 4 and for forming the crosslinked layer 5. A resin film is formed. These resin films are difficult to be extrusion-molded, and a thermoplastic resin film and a crosslinked resin film which are formed by a thickness of about 50 μm are usually bonded to each other, and the total thickness is about 100 μm. If the thickness of the insulator is thick, the flexibility of the lead is insufficient, and a gap is formed between the edge of the insulator and the multilayer film, and the sealing of the lead and the sealed bag is insufficient, and moisture enters the sealed bag.
又，上述專利文獻1中亦揭示在引線導體上，以熱熔黏來貼上一層熱塑性樹脂薄膜後，從此熱塑性樹脂薄膜的外側，以透過距離成為比薄膜厚度還小的方式，照射經控制的電子線，而形成交聯層，但熱塑性樹脂薄膜的厚度係沒有講明。Moreover, in the above-mentioned Patent Document 1, it is also disclosed that a conductive resin film is adhered to the lead conductor by heat fusion, and the controlled distance from the outside of the thermoplastic resin film is such that the transmission distance is smaller than the film thickness. The electron beam forms a crosslinked layer, but the thickness of the thermoplastic resin film is not explained.
本發明之目的為提供彎曲性良好，可防止水分的侵入之非水電解質蓄電裝置中所使用的引線構件及其製法，以及非水電解質蓄電裝置。An object of the present invention is to provide a lead member used in a nonaqueous electrolyte electricity storage device which is excellent in flexibility and can prevent intrusion of moisture, a method for producing the same, and a nonaqueous electrolyte electricity storage device.
本發明的引線構件係使用於非水電解質蓄電裝置，該非水電解質蓄電裝置係在由含金屬箔層的多層薄膜所成的封入袋體中收納有電極體與非水電解質介質，其特徵為具備連接於前述電極體的引線導體、與接著於該引線導體的在前述封入袋體之內面所接著的絕緣體，前述絕緣體係由厚度20μm以上且40μm以下的一層樹脂薄膜夾持前述引線導體貼合而形成，其全體經交聯。The lead member of the present invention is used in a nonaqueous electrolyte electricity storage device in which an electrode body and a nonaqueous electrolyte medium are housed in a sealed bag body made of a multilayer film containing a metal foil layer, and is characterized in that a lead conductor connected to the electrode body and an insulator attached to an inner surface of the lead-molded body of the lead conductor, wherein the insulating system is bonded to the lead conductor by a resin film having a thickness of 20 μm or more and 40 μm or less And formed, the whole is cross-linked.
又，本發明的引線構件之製法係非水電解質蓄電裝置中所使用的引線構件之製造方法，該非水電解質蓄電裝置係在由含金屬箔層的多層薄膜所成的封入袋體中收納有電極體與非水電解質介質，其特徵為在連接於前述電極體的引線導體上，將由厚度20μm以上且40μm以下的一層樹脂薄膜所成的絕緣體以夾持前述引線導體的方式進行貼合及被覆後，以電離輻射線照射前述絕緣體全體而進行交聯。Moreover, the method for producing a lead member of the present invention is a method for producing a lead member used in a nonaqueous electrolyte electricity storage device, wherein the nonaqueous electrolyte electricity storage device houses an electrode in a sealed bag body formed of a multilayer film containing a metal foil layer. The body and the non-aqueous electrolyte medium are characterized in that an insulator formed of a resin film having a thickness of 20 μm or more and 40 μm or less is bonded and coated to sandwich the lead conductor on the lead conductor connected to the electrode body. The entire insulator is irradiated with ionizing radiation to carry out crosslinking.
另外，本發明的非水電解質蓄電裝置係在由含金屬箔層的多層薄膜所成的封入袋體中收納有電極體與非水電解質介質，其特徵為具備上述本發明的引線構件。In the nonaqueous electrolyte electricity storage device of the present invention, the electrode body and the nonaqueous electrolyte medium are housed in the sealed bag body formed of the multilayer film containing the metal foil layer, and the lead member of the present invention is provided.
依照本發明，可減薄引線構件的絕緣體之厚度，與習知者相比，可提高引線構件的柔軟性。又，由於絕緣體對引線導體的接著性良好，而且藉由交聯可提高絕緣體的耐熱性，故可抑制絕緣體的形狀變化。因此，可使良好地密接於封入袋體的薄膜。藉此，提高自封入袋體取出引線構 件的部分之密閉性，故可防止水分的侵入。再者，於形成絕緣體的樹脂薄膜時，不必要貼合熱塑性層與交聯層，故可消除貼合的界面之剝離或微龜裂所致的可靠性降低之可能性。又，可實現蓄電裝置的小型化、薄型化。According to the present invention, the thickness of the insulator of the lead member can be reduced, and the flexibility of the lead member can be improved as compared with the prior art. Further, since the insulator has good adhesion to the lead conductor and the heat resistance of the insulator can be improved by crosslinking, the shape change of the insulator can be suppressed. Therefore, it is possible to adhere well to the film enclosed in the bag body. Thereby, the self-sealing bag body is taken out and the lead structure is removed. The part of the piece is sealed so that moisture can be prevented from entering. Further, in the case of forming the resin film of the insulator, it is not necessary to bond the thermoplastic layer and the crosslinked layer, so that the possibility of deterioration in reliability due to peeling of the bonded interface or microcracking can be eliminated. Moreover, the size and thickness of the power storage device can be reduced.
藉由圖式來說明本發明的實施形態之例。本發明的非水電解質電池，係如第1圖之一例所示地，為一對引線構件21a、21b的引線導體22a、22b的取出部分各自被絕緣體23a、23b所覆蓋，由封入袋6的密封部分14取出到外部的形態之薄形構造，外觀上係與習知者大致相同的形狀。An example of an embodiment of the present invention will be described by way of drawings. In the nonaqueous electrolyte battery of the present invention, as shown in an example of Fig. 1, the extraction portions of the lead conductors 22a and 22b of the pair of lead members 21a and 21b are covered with insulators 23a and 23b, respectively, and are enclosed by the bag 6. The sealing portion 14 is taken out to the outer thin structure, and has a shape substantially the same as that of a conventional one.
作為收納電極體、非水電解質介質等的封入袋體之封入袋6，例如係將2片薄膜的周緣部進行熱封而成為密封部分14的袋狀者。於封入袋6內，密封收納有正極、負極、隔膜等與溶解在非水溶劑(例如有機溶劑)中的電解質(例如鋰化合物)之非水電解質介質(電解液)。引線構件21a、21b，為了對外部作電性連接，係由密封部分14取出，該取出部分係被絕緣體23a、23b所被覆絕緣，與形成封入袋6的多層薄膜內之金屬箔層不發生電性接觸。The sealing bag 6 that encloses the sealed bag body such as the electrode body or the non-aqueous electrolyte medium is, for example, a bag-shaped portion in which the peripheral edge portions of the two films are heat-sealed to form the sealing portion 14. In the sealed bag 6, a nonaqueous electrolyte medium (electrolyte) containing an electrolyte (for example, a lithium compound) dissolved in a nonaqueous solvent (for example, an organic solvent) such as a positive electrode, a negative electrode, or a separator is sealed and stored. The lead members 21a and 21b are taken out from the sealing portion 14 for electrical connection to the outside, and the taken-out portions are insulated by the insulators 23a and 23b, and the metal foil layer in the multilayer film forming the sealed bag 6 does not generate electricity. Sexual contact.
第2圖係本發明的非水電解質電池之概略圖，顯示從第1圖所示的封入袋6之密封部分14的一部分，取出經絕緣體23a、23b所覆蓋的引線構件21a、21b之引線導體22a、22b到外部的構成。封入袋6係與前述第4圖之說明者 同樣地，在最內層薄膜7與最外層薄膜9之間，以三明治狀貼合至少由鋁等的金屬所成的金屬箔層8之多層薄膜10來形成，提高對於封入袋6內所收納的電解液之密封性。Fig. 2 is a schematic view showing a nonaqueous electrolyte battery of the present invention, showing a part of the sealing portion 14 of the sealing bag 6 shown in Fig. 1, and taking out the lead conductors of the lead members 21a and 21b covered by the insulators 23a and 23b. 22a, 22b to the outside of the composition. Enclosed bag 6 is the same as that described in the above figure 4 In the same manner, a multilayer film 10 of a metal foil layer 8 made of a metal such as aluminum is bonded to the innermost layer film 7 and the outermost layer film 9 in a sandwich shape, and is accommodated in the sealed bag 6. The tightness of the electrolyte.
又，封入袋6的多層薄膜10，例如係由3~5層的積層體所構成，於其最內層薄膜7中，作為適合於防止電解液從不溶解電解液的密封部分14漏出者，可使用聚烯烴樹脂(例如：馬來酸酐改性低密度聚乙烯、馬來酸酐改性低密度聚丙烯)。最外層薄膜9，由於係用於保護內側的金屬箔層8防止外傷，故由聚對酞酸乙二酯(簡稱PET)等所形成。Further, the multilayer film 10 sealed in the bag 6 is composed of, for example, a laminated body of 3 to 5 layers, and the innermost layer film 7 is suitable for preventing the electrolyte from leaking from the sealing portion 14 which does not dissolve the electrolytic solution. A polyolefin resin (for example, maleic anhydride-modified low-density polyethylene, maleic anhydride-modified low-density polypropylene) can be used. The outermost layer film 9 is formed of polyethylene terephthalate (PET) or the like because it is used to protect the inner metal foil layer 8 from being scratched.
作為封入袋6內所收容的電解質，可使用在碳酸伸丙酯、碳酸伸乙酯、碳酸二乙酯、碳酸二甲酯、1,2-二甲氧基乙烷、四氫呋喃等的有機溶劑中溶解有LiClO4 、LiBF4 、LiPF6 、LiAsF6 等的電解質的非水電解液或鋰離子傳導性的固體電解質等。The electrolyte contained in the sealed bag 6 can be used in an organic solvent such as propyl carbonate, ethyl carbonate, diethyl carbonate, dimethyl carbonate, 1,2-dimethoxyethane or tetrahydrofuran. A nonaqueous electrolytic solution or a lithium ion conductive solid electrolyte in which an electrolyte such as LiClO 4 , LiBF 4 , LiPF 6 or LiAsF 6 is dissolved.
電極體係由夾持隔膜12而對峙的正極11a與負極11b所構成，具有於稱為集電體的金屬箔或金屬網的金屬基材上形成活性物質層的構造。正極11a係由在鋁箔的電極導電體上形成由LiCoO2 等的還原氧化物粉末與導電劑的碳粉末及黏合劑的黏結劑所成的活性物質而構成。The electrode system is composed of a positive electrode 11a and a negative electrode 11b which are opposed to each other by sandwiching the separator 12, and has a structure in which an active material layer is formed on a metal substrate of a metal foil or a metal mesh called a current collector. The positive electrode 11a is formed by forming an active material made of a reduced oxide powder such as LiCoO 2 and a carbon powder of a conductive agent and a binder of a binder on an electrode conductor of an aluminum foil.
負極11b係由在銅箔所成的電極導電體上形成由碳粉末與黏合劑的黏結劑所成的活性物質而構成。配設於正極11a與負極11b之間的隔膜12，係由保持電絕緣性且保持離子傳導性的聚烯烴系多孔膜所形成。The negative electrode 11b is formed of an active material formed of a binder of carbon powder and a binder on an electrode conductor formed of a copper foil. The separator 12 disposed between the positive electrode 11a and the negative electrode 11b is formed of a polyolefin-based porous film that maintains electrical insulation and maintains ion conductivity.
在正極11a、負極11b，藉由點焊或超音波熔接等來連接引線構件的引線導體22a、22b，於外部電性取出。連接於正極11a的引線導體22a，由於成為正的高電位，故較佳為以與電解液接觸不會發生溶解的方式，由與電極板同樣的鋁或鈦或此等的合金所形成者。連接於負極11b的引線導體22b，由於過充電而析出鋰，過放電而電位變高，故較佳以鋰不易腐蝕，難以形成與鋰的合金，且高電位不易溶解的與電極板同樣之銅或鎳或此等的合金所形成者。The lead conductors 22a and 22b of the lead member are connected to the positive electrode 11a and the negative electrode 11b by spot welding or ultrasonic welding, and are externally taken out. Since the lead conductor 22a connected to the positive electrode 11a has a positive high potential, it is preferably formed of aluminum or titanium or an alloy of the same type as the electrode plate so as not to be dissolved in contact with the electrolytic solution. The lead conductor 22b connected to the negative electrode 11b precipitates lithium due to overcharge, and the potential is increased by overdischarging. Therefore, it is preferable that lithium is not easily corroded, and it is difficult to form an alloy which is alloyed with lithium and which is not easily dissolved at a high potential. Or nickel or the alloy formed by these.
覆蓋引線構件的引線導體22a、22b之取出部分的絕緣體23a、23b，係貼合一層交聯薄膜25而形成。交聯薄膜25係在厚度方向中全體被交聯。交聯的程度係以凝膠分率來定義，凝膠分率若為20%以上，則可說是交聯。於交聯薄膜25的情況，凝膠分率未必要是100%。凝膠分率若為70%，則可說是充分交聯。此交聯薄膜25之內側部分係接著於引線導體22a、22b而一體化，外側部分係接著於封入袋6的最內層薄膜7，密封封閉引線導體22a、22b的取出部分。The insulators 23a and 23b covering the lead-out portions of the lead conductors 22a and 22b of the lead member are formed by laminating a layer of the crosslinked film 25. The crosslinked film 25 is crosslinked in the entire thickness direction. The degree of cross-linking is defined by the gel fraction, and if the gel fraction is 20% or more, it can be said to be cross-linked. In the case of the crosslinked film 25, the gel fraction is not necessarily 100%. If the gel fraction is 70%, it can be said that it is sufficiently crosslinked. The inner portion of the crosslinked film 25 is integrated with the lead conductors 22a and 22b, and the outer portion is attached to the innermost film 7 of the sealed bag 6, and the taken-out portion of the lead conductors 22a and 22b is hermetically sealed.
以上雖然以非水電解質電池之例來說明，但於電雙層電容器中，也可為與蓄電池同樣地使用電極體及非水電解質介質的構造，本發明亦可適用於如非水電解質電容器般的電雙層電容器。因此，於本發明中，以含非水電解質電池或非水電解質電容器的非水電解質蓄電裝置當作對象。Although the above description is made by way of an example of a nonaqueous electrolyte battery, the electric double layer capacitor may have a structure in which an electrode body and a nonaqueous electrolyte medium are used in the same manner as the battery, and the present invention is also applicable to a nonaqueous electrolyte capacitor. Electric double layer capacitor. Therefore, in the present invention, a nonaqueous electrolyte electricity storage device including a nonaqueous electrolyte battery or a nonaqueous electrolyte capacitor is targeted.
非水電解質電容器(省略圖示)，亦例如是將夾持隔膜而配設的一對電極體(藉由電壓施印加而分極為正極與負 極)浸漬在非水電解液中，收納於封入袋體等中而構成。作為非水系所用的代表性電解液，例如可舉出碳酸伸丙酯等。於電極體的電極材料中，使用活性碳或碳纖維，於進行用於提高比表面積的賦活處理後，混合導電材或交聯材，成形為片狀。而且，於此片狀的活性碳接合金屬基材而成為電極體，上述引線構件的引線導體係連接於金屬基材。The non-aqueous electrolyte capacitor (not shown) is, for example, a pair of electrode bodies that are disposed to sandwich the separator (the positive electrode and the negative electrode are divided by voltage application). The electrode is immersed in a non-aqueous electrolyte solution, and is housed in a sealed bag or the like. The representative electrolyte solution used for the nonaqueous system may, for example, be propyl carbonate or the like. In the electrode material of the electrode body, activated carbon or carbon fiber is used, and after the activation treatment for increasing the specific surface area, the conductive material or the crosslinked material is mixed and formed into a sheet shape. Further, the sheet-shaped activated carbon is bonded to the metal substrate to form an electrode body, and the lead conductor system of the lead member is connected to the metal substrate.
第3圖係說明上述引線構件21a、21b的概略及其製法之一例，第3(A)圖顯示以絕緣體23a、23b覆蓋引線導體22a、22b的取出部分之狀態的外觀。此引線構件21a、21b係可以第3(B)圖～第3(D)圖所示的方法來製造。Fig. 3 is a view showing an outline of the above-described lead members 21a and 21b and a method of manufacturing the same, and Fig. 3(A) shows an appearance of a state in which the lead portions of the lead conductors 22a and 22b are covered with the insulators 23a and 23b. The lead members 21a and 21b can be manufactured by the methods shown in Figs. 3(B) to 3(D).
首先，如第3(B)圖所示地，例如以絕緣體23a、23b來夾持被覆厚度0.1mm、寬度5.0mm左右的平形形狀之引線導體22a、22b的兩面。作為絕緣體23a、23b的基材，使用厚度40μm以下的矩形狀之樹脂薄膜片23。作為此樹脂薄膜片23，例如可使用熱塑性聚烯烴樹脂薄膜等，較佳為酸改性聚丙烯薄膜或酸改性低密度聚乙烯薄膜，熔點120℃~160℃左右者。接著，如第3(C)圖所示地，樹脂薄膜片23例如可邊藉由加熱器加熱到150℃左右，邊推壓於引線導體22a、22b的表面，經由熱熔黏而接著一體化。First, as shown in Fig. 3(B), for example, both surfaces of the lead conductors 22a and 22b having a flat shape of a thickness of 0.1 mm and a width of about 5.0 mm are sandwiched by insulators 23a and 23b. As the base material of the insulators 23a and 23b, a rectangular resin film sheet 23 having a thickness of 40 μm or less is used. As the resin film sheet 23, for example, a thermoplastic polyolefin resin film or the like can be used, and an acid-modified polypropylene film or an acid-modified low-density polyethylene film is preferable, and the melting point is about 120 ° C to 160 ° C. Then, as shown in Fig. 3(C), the resin film sheet 23 can be pressed against the surface of the lead conductors 22a and 22b by, for example, heating to about 150 ° C by a heater, and then thermally integrated and then integrated. .
接著，如第3(D)圖所示地，對接著於引線導體22a、22b的樹脂薄膜片23之表面，照射電子線或加馬射線等的電離輻射線E以進行交聯。藉由電離輻射線E的照射，使樹脂薄膜片23在其厚度全體中被交聯而成為交聯薄膜25，提高對引線導體22a、22b的接著力。茲認為交聯薄膜 25係由於輻射線照射時的發熱而產生退火效果，提高接著力。Next, as shown in Fig. 3(D), the surface of the resin film sheet 23 following the lead conductors 22a and 22b is irradiated with an ionizing radiation E such as an electron beam or a gamma ray for crosslinking. By the irradiation of the ionizing radiation E, the resin film sheet 23 is crosslinked in the entire thickness to form the crosslinked film 25, and the adhesion to the lead conductors 22a and 22b is improved. Crosslinked film The 25 series has an annealing effect due to heat generation upon irradiation with radiation, and the adhesion is improved.
電離輻射線E的照射，為了使樹脂薄膜片23的全體進行交聯，必須充分的照射量，但若過度照射則樹脂會劣化，接著力或凝聚力會降低。藉由以不過度照射的程度使全體交聯，得到比部分交聯還優良的成品之照射條件範圍變廣，良率提高。Irradiation of the ionizing radiation line E requires a sufficient amount of irradiation in order to crosslink the entire resin film sheet 23. However, when excessively irradiated, the resin is deteriorated, and the force or cohesive force is lowered. By crosslinking the entire body without excessive irradiation, it is possible to obtain a wider range of irradiation conditions than the partial cross-linking, and the yield is improved.
又，為了將樹脂薄膜片23交聯，必須預先添加交聯助劑。Further, in order to crosslink the resin film sheet 23, it is necessary to add a crosslinking assistant in advance.
作為交聯助劑，可例示丙烯酸或甲基丙烯酸的酯類、二乙烯基化合物、烯丙醇與丙烯酸或甲基丙烯酸的酯類等。具體地，可舉出乙二醇二丙烯酸酯、二乙二醇二丙烯酸酯、三乙二醇二丙烯酸酯、三羥甲基丙烷三丙烯酸酯、乙二醇二甲基丙烯酸酯、三羥甲基丙烷三甲基丙烯酸酯等的丙烯酸或甲基丙烯酸的酯類；二乙烯基苯、二乙烯基吡啶等的二乙烯基化合物；馬來酸二芳酯、富馬酸二芳酯、氰尿酸三烯丙酯、異氰尿酸三烯丙酯等的烯丙醇與丙烯酸或甲基丙烯酸的酯類等。Examples of the crosslinking assistant include esters of acrylic acid or methacrylic acid, divinyl compounds, esters of allyl alcohol and acrylic acid or methacrylic acid, and the like. Specific examples thereof include ethylene glycol diacrylate, diethylene glycol diacrylate, triethylene glycol diacrylate, trimethylolpropane triacrylate, ethylene glycol dimethacrylate, and trishydroxyl An ester of acrylic acid or methacrylic acid such as propane trimethacrylate; a divinyl compound such as divinylbenzene or divinylpyridine; diaryl maleate, diaryl fumarate, cyanuric acid An allyl alcohol such as triallyl ester or triallyl isocyanurate and an ester of acrylic acid or methacrylic acid.
就交聯助劑的添加量而言，雖然添加量愈多，交聯度愈高，但由於耐熱老化性變差，故必須選擇最適合值，可為23重量%以下。In the addition amount of the crosslinking assistant, the higher the amount of addition, the higher the degree of crosslinking, but the heat aging resistance is deteriorated, so the optimum value must be selected, and it may be 23% by weight or less.
於本實施形態中，使用異氰尿酸三烯丙酯(日本化成(股)製的TAIC(註冊商標)等)，其添加量為0.5-10重量%。In the present embodiment, triallyl isocyanurate (TAIC (registered trademark) manufactured by Nippon Kasei Co., Ltd.) is used, and the amount thereof is 0.5 to 10% by weight.
又，電離輻射線E的照射條件，若以吸收線量來表示 ，則係50-200kGy。以100kGy當作中心值進行照射，但亦可為±30kGy左右的幅度。Further, the irradiation condition of the ionizing radiation line E is expressed by the amount of absorption line , is 50-200kGy. The irradiation is performed at a center value of 100 kGy, but may be an amplitude of about ±30 kGy.
若使用異氰尿酸三烯丙酯於交聯助劑，則在金屬與薄膜的界面，未反應的異氰尿酸三烯丙酯(油狀)會浮出而有接著力降低之虞(尤其照射量變少而異氰尿酸三烯丙酯殘留時)。因此，可使用非油狀的交聯助劑。例如，可舉出日立化成(股)的FA-731A(三(2-丙烯醯氧基乙基)異氰尿酸酯(凝固點45-55℃，常溫為固體)。FA-731A的添加量係5-20%左右，較佳為10-15%。若超過20%則難以混合。若低於5%，則與異氰尿酸三烯丙酯相比，凝膠分率變小。If triallyl isocyanurate is used as a crosslinking aid, at the interface between the metal and the film, unreacted triallyl isocyanurate (oily) will float and there will be a decrease in adhesion (especially When the amount is small and the triallyl isocyanurate remains,). Therefore, a non-oily crosslinking aid can be used. For example, FA-731A (tris(2-propenyloxyethyl) isocyanurate (freezing point 45-55 ° C, solid at room temperature) of Hitachi Chemical Co., Ltd. is added. The amount of FA-731A added is 5-20% or so, preferably 10-15%. If it exceeds 20%, it is difficult to mix. If it is less than 5%, the gel fraction is smaller than that of triallyl isocyanurate.
即使常溫為液狀的交聯助劑，若分子量大者(寡聚物、預聚物)，則對表面的遷移變少。例如，於預聚物中，可例示聚丙二醇# 700丙烯酸酯(日立化成(股)的FA-P270A)。Even if the crosslinking agent is a liquid cross-linking agent at normal temperature, the migration to the surface is small if the molecular weight is large (oligomer or prepolymer). For example, among the prepolymers, polypropylene glycol #700 acrylate (FA-P270A of Hitachi Chemical Co., Ltd.) can be exemplified.
上述絕緣體23a、23b的交聯薄膜25係與以往同樣地，良好地接著於引線導體22a、22b的表面而將引線導體密封。又，可藉由交聯來提高絕緣體的耐熱性，抑制絕緣體23a、23b的形狀變化，可熱熔黏於封入袋體的最內層薄膜而良好地密封封閉。The crosslinked film 25 of the insulators 23a and 23b is sealed to the surface of the lead conductors 22a and 22b in the same manner as in the related art. Further, the heat resistance of the insulator can be improved by crosslinking, and the shape change of the insulators 23a and 23b can be suppressed, and the innermost layer film sealed in the bag body can be thermally fused and sealed tightly.
於本發明中，如上述地，由於絕緣體23a、23b係貼合一層樹脂薄膜(交聯薄膜25)而形成，故與以往貼合熱塑性樹脂薄膜與交聯的樹脂薄膜者相比，絕緣體的厚度可變小。一層樹脂薄膜的厚度可成為40μm以下。因此，貼合有二片樹脂薄膜的部分之長度為80μm以下。但是，於一層樹脂薄膜的厚度為20μm以下時，引線導體的金屬毛邊有 突破絕緣體之虞，而且從樹脂薄膜的製造容易性之點來看，宜為20μm以上。In the present invention, since the insulators 23a and 23b are formed by laminating a resin film (crosslinked film 25) as described above, the thickness of the insulator is higher than that of the conventionally bonded thermoplastic resin film and the crosslinked resin film. It can be small. The thickness of one layer of the resin film can be 40 μm or less. Therefore, the length of the portion to which the two resin films are bonded is 80 μm or less. However, when the thickness of a resin film is 20 μm or less, the metal burrs of the lead conductor have It is preferable to be 20 μm or more from the viewpoint of easiness of production of the resin film.
又，藉由以一層樹脂薄膜(交聯薄膜25)來形成引線構件的絕緣體，不需要以往之貼合2片樹脂薄膜的步驟。結果，可減低成本，同時可消除貼合的界面之剝離、微龜裂所致的可靠性降低之可能性。又，藉由使絕緣體的厚度成為40μm以下的厚度，可提高引線構件的柔軟性，藉此提高對電子機器的設置、對電性接連的自由度，而且可實現蓄電裝置的小型化、薄型化。Further, by forming the insulator of the lead member with a single resin film (crosslinked film 25), the conventional step of bonding two resin films is not required. As a result, the cost can be reduced, and at the same time, the possibility of peeling of the bonded interface and the reliability due to microcracking can be eliminated. In addition, by making the thickness of the insulator 40 μm or less, the flexibility of the lead member can be improved, thereby improving the installation of the electronic device and the degree of freedom of electrical connection, and the size and thickness of the power storage device can be reduced. .
雖然已經參照特定的實施態樣來詳細說明本發明，但明顯地熟習該項技術者在不脫離本發明的精神與範圍內，可加以各式各樣的變更或修正。Although the present invention has been described in detail with reference to the specific embodiments thereof, various modifications and changes can be made without departing from the spirit and scope of the invention.
6‧‧‧封入袋6‧‧‧Blocked into the bag
7‧‧‧最內層薄膜7‧‧‧ innermost film
8‧‧‧金屬箔層8‧‧‧metal foil layer
9‧‧‧最外層薄膜9‧‧‧ outermost film
10‧‧‧多層薄膜10‧‧‧Multilayer film
11a‧‧‧正極11a‧‧‧ positive
11b‧‧‧負極11b‧‧‧negative
12‧‧‧隔膜12‧‧‧Separator
13‧‧‧非水電解質介質13‧‧‧Non-aqueous electrolyte medium
14‧‧‧密封部分14‧‧‧ Sealing section
21a、21b‧‧‧引線構件21a, 21b‧‧‧ lead members
22a、22b‧‧‧引線導體22a, 22b‧‧‧ lead conductor
23‧‧‧樹脂薄膜片23‧‧‧Resin film
23a、23b‧‧‧絕緣體23a, 23b‧‧‧ insulator
25‧‧‧交聯薄膜25‧‧‧crosslinked film
第1圖係本發明的非水電解質電池之一例的概略斜視圖。Fig. 1 is a schematic perspective view showing an example of a nonaqueous electrolyte battery of the present invention.
第2圖係本發明的非水電解質電池之引線構件的概略圖，其為第1圖的a-a箭號方向之截面圖。Fig. 2 is a schematic view showing a lead member of a nonaqueous electrolyte battery of the present invention, which is a cross-sectional view taken along the line a-a of Fig. 1;
第3圖係本發明的引線構件之製法的概略圖。Fig. 3 is a schematic view showing a method of manufacturing the lead member of the present invention.
第4圖係顯示習知技術的圖，其為第5圖的a-a箭號方向之截面圖。Fig. 4 is a view showing a conventional technique, which is a cross-sectional view of the a-a arrow direction of Fig. 5.
第5圖係習知的非水電解質電池之一例的概略斜視圖。Fig. 5 is a schematic perspective view showing an example of a conventional nonaqueous electrolyte battery.
6‧‧‧封入袋6‧‧‧Blocked into the bag
7‧‧‧最內層薄膜7‧‧‧ innermost film
8‧‧‧金屬箔層8‧‧‧metal foil layer
9‧‧‧最外層薄膜9‧‧‧ outermost film
10‧‧‧多層薄膜10‧‧‧Multilayer film
11a‧‧‧正極11a‧‧‧ positive
11b‧‧‧負極11b‧‧‧negative
12‧‧‧隔膜12‧‧‧Separator
13‧‧‧非水電解質介質13‧‧‧Non-aqueous electrolyte medium
14‧‧‧密封部分14‧‧‧ Sealing section
21a、21b‧‧‧引線構件21a, 21b‧‧‧ lead members
22a、22b‧‧‧引線導體22a, 22b‧‧‧ lead conductor
23a、23b‧‧‧絕緣體23a, 23b‧‧‧ insulator
25‧‧‧交聯薄膜25‧‧‧crosslinked film
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| TWI389373B true TWI389373B (en) | 2013-03-11 |
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| TW097127249A TWI389373B (en) | 2007-07-19 | 2008-07-18 | Lead member,process for producing the same and non-aqueous electrolyte accumulation device |
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| JP (1) | JP5369522B2 (en) |
| KR (2) | KR101097013B1 (en) |
| CN (1) | CN101542773A (en) |
| TW (1) | TWI389373B (en) |
| WO (1) | WO2009011371A1 (en) |
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| JP2010212070A (en) * | 2009-03-10 | 2010-09-24 | Unitika Ltd | Battery and method of manufacturing the same |
| JP5349345B2 (en) * | 2010-01-21 | 2013-11-20 | 太陽誘電株式会社 | Electrochemical devices |
| JP5644383B2 (en) * | 2010-11-05 | 2014-12-24 | 住友電気工業株式会社 | Lead member for non-aqueous electrolyte device and manufacturing method thereof |
| FR2990885B1 (en) * | 2012-05-23 | 2014-09-19 | Arkema France | PROCESS FOR PREPARING SURFACES |
| CN108010739B (en) | 2012-10-08 | 2020-11-10 | 麦克斯威科技公司 | Electrolyte for three-volt super capacitor |
| JP2014220176A (en) * | 2013-05-10 | 2014-11-20 | 住友電気工業株式会社 | Lead member, nonaqueous electrolyte power storage device |
| US10263224B2 (en) * | 2015-04-23 | 2019-04-16 | Semiconductor Energy Laboratory Co., Ltd. | Power storage device and electronic device |
| CN108463907A (en) * | 2016-02-29 | 2018-08-28 | 松下知识产权经营株式会社 | Non-aqueous electrolyte secondary battery |
| CN108292733B (en) * | 2016-10-17 | 2021-01-12 | 住友电气工业株式会社 | Lead for nonaqueous electrolyte battery, and nonaqueous electrolyte battery comprising same |
| DE102016223464A1 (en) * | 2016-11-25 | 2018-05-30 | Robert Bosch Gmbh | Connecting device for the electrical connection of electrical storage units |
| JP7101338B2 (en) * | 2017-06-02 | 2022-07-15 | 住友電工ファインポリマー株式会社 | Parts for power storage device, its manufacturing method and power storage device |
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| JP2003162996A (en) * | 2001-11-26 | 2003-06-06 | Sumitomo Electric Ind Ltd | Power storage device and lead unit used therefor |
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| JP2009043719A (en) | 2009-02-26 |
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| KR101043117B1 (en) | 2011-06-20 |
| JP5369522B2 (en) | 2013-12-18 |
| CN101542773A (en) | 2009-09-23 |
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| WO2009011371A1 (en) | 2009-01-22 |
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