JP2004303590A - Laminated battery, and manufacturing method of the same - Google Patents
Laminated battery, and manufacturing method of the same Download PDFInfo
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- JP2004303590A JP2004303590A JP2003095834A JP2003095834A JP2004303590A JP 2004303590 A JP2004303590 A JP 2004303590A JP 2003095834 A JP2003095834 A JP 2003095834A JP 2003095834 A JP2003095834 A JP 2003095834A JP 2004303590 A JP2004303590 A JP 2004303590A
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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- 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
Description
【0001】
【発明の属する技術分野】
本発明は、ラミネート電池に関し、特に偏平巻回電極を使用したラミネート電池において、電解液の含液性やガス抜け性を良くし、また正負極間の絶縁不良等不具合をなくしてその信頼性を高めたラミネート電池に関する。
【0002】
【従来の技術】
携帯型の電子機器の急速な普及に伴い、それに使用される電池への要求仕様は、年々厳しくなり、特に小型・薄型化され、高容量でサイクル特性が優れ、性能の安定したものが要求されている。そして、二次電池分野では他の電池に比べて高エネルギー密度であるリチウム非水電解質二次電池が注目され、このリチウム非水電解質二次電池の占める割合は二次電池市場において大きな伸びを示している。
【0003】
このリチウム非水電解質二次電池は、細長いシート状の銅箔等からなる負極芯体(集電体)の両面にリチウムイオンを吸蔵放出する負極活物質を含む負極合剤を塗布した負極と、細長いシート状のアルミニウム箔等からなる正極芯体の両面にリチウムイオンを吸蔵・放出する正極活物質を含む正極合剤を塗布した正極との間に、微多孔性ポリプロピレンフィルム等からなるセパレータを配置し、負極及び正極をセパレータにより互いに絶縁した状態で円柱状又は楕円形状に巻回した後、角型電池の場合は更に巻回電極体を押し潰して偏平状に形成し、負極及び正極の各所定部分にそれぞれ負極タブ及び正極タブを接続し、その外側を外装で被覆することにより製造されている。
【0004】
従来の非水電解質二次電池においては、巻回電極体を円筒形の外装缶内に挿入した後、非水電解液を注入することにより非水電解質電池が製造されているが、この巻回電極体は、図4に示す如く、正極ないしは負極41の巻き始めか巻き終りの端に金属製芯体箔が露出した合剤の未塗布部42を設け、この未塗布部42にアルミニウム、ニッケルで代表されるタブ43を溶接し、このタブ部分を絶縁テープ44で被覆すると共に、このタブ43を電池の電極端子に接続する構造をとることが慣用的に行われている。(特許文献1参照)。
【0005】
ところで、上述の非水電解質二次電池においては、外装とし強度を与えるために主として金属製の外装缶が使用されているが、近年に至り重量低減、単位体積当たりの電池容量の増大等の目的でラミネートフィルムを使用したラミネート電池が製造されるようになってきた。そこで、本発明の理解のために、以下において図5を用いて従来から慣用的に行われているラミネート電池50の製造工程について説明する。
【0006】
まず最初に、前述の従来例と同様にして偏平巻回電極体11を製造する。その際、この偏平巻回電極体11は、負極の金属製芯体箔露出部に負極タブ12を溶接しておくと共に、正極の金属製芯体箔露出部にも正極タブ13を溶接しておく。続いて、図5(A)に示したように、所定の大きさの周知のラミネートフィルム54、例えばアルミラミネートフィルムを2つ折りし、この内部に前記偏平巻回電極体51を配置し、必要に応じて負極タブ52及び正極タブ53の導出部に両面に薄いシール材55、55’を配置した後、このラミネートフィルム54のトップ部(タブ側)をバー状の金型(図示せず)を用いて溶着し、トップ封止部56を形成する。なお、この際、トップ封止部56の外縁には、ラミネートフィルム54から溶けたシーラント層がはみ出して金型に付着しないようにするため、未溶着部56’が設けられている。
【0007】
次に、図5(B)に示したように、バー状の金型を用いて、ラミネートフィルム54のサイド部の一方側を溶着して第1のサイド封止部57を形成する。この場合も第1のサイド封止部57の外縁はラミネートフィルムから溶けたシーラント層がはみ出して金型に付着しないようにするため、未溶着部57’が設けられている。次いで、液状電解質をもう一方のサイド部側58から注入する。そうすると、この液状電解質は、偏平巻回電極体51の内部へ十分に浸透する。その後、図5(C)に示したように、ラミネートフィルム54の他方側をバー型の金型により仮溶着して仮封止部60を形成する。次いで、予備充電及びエージングした後、図5(D)に示したように、ラミネートフィルム54の他方側をバー型の金型で溶着して第2のサイド封止部61を形成する。そして、前記ラミネートフィルムの不要部を切断して、図5(E)に示したような従来例のラミネート電池50を得る。
【0008】
このように、従来例のラミネート電池においても、各電極のタブは各電極の巻き初めか巻き終わりの芯体箔に配置され、このタブの表面は対となる電極との間で短絡を起こさないようにするため、図4に示した電極と同様に、絶縁テープにより被覆されている。加えて、特に正極芯体箔の対面に負極活物質が存在すると、負極活物質から離脱した導電性の粉体により短絡しやすいことから、正極活物質が塗布されていない正極芯体露出部が絶縁テープで被覆されている場合もある(特許文献2参照)。
【0009】
したがって、金属製芯体箔上にリチウムイオンを吸蔵・放出する正極活物質を含む正極合剤が塗布された正極と、金属製芯体箔上にリチウムイオンを吸蔵放出する負極活物質を含む負極合剤が塗布された負極とを、微多孔性ポリプロピレンフィルムからなる2枚のセパレータを介して互いに絶縁した状態で巻回した後、押し潰して偏平巻回電極体を製造すると、各電極のタブのため及びこのタブの表面に設けられた絶縁テープの存在のために、偏平巻回電極体の内面へ向かって凹凸ができてしまうので、この部分に応力がかかり、ラミネート電池内への電解液の注入時及び充電ガス発生時の気泡がこの応力がかかってる部分にたまりやすいという問題点が存在していた。
【0010】
この現象を図面を用いて更に詳細に説明する。図6は、偏平巻回電極体70をタブ部方向から見た横断面図である。金属製正極芯体箔71の一方の表面には正極タブ72が溶接されており、更にその表面に絶縁テープ73、負極74、セパレータ75と順次積層されて偏平状巻回電極体70が形成されている、この偏平巻回電極体70の表面は偏平巻回電極体を製造するときに押し潰すために平らになっているが、正極タブ72及び絶縁テープ73が存在しているため、内部に向かって応力が加えられ、図6に示したような形に変形している。この場合、正極タブ72の角部76近傍のセパレータや負極に応力がかかり、非水電解液を注入した際や充電によりガスが発生した際にはこの応力がかかっている部分にガスがたまりやすくなるわけである。
【0011】
一方、円筒形の非水電解質二次電池の正極として、図7に示すように長尺状の金属箔81の表面に正極合剤84を塗着した後、長尺状の正極の中間に帯状の合剤剥離部分82を形成し、この剥離部分に正極タブ(リード板)83を接続し、正極タブ83と合剤剥離部分82の表面と周囲の正極合剤84にまたがって絶縁テープ85を貼り付けて被覆していたものが知られている(特許文献3参照)。
この正極は、正極タブが極板の幅方向に部分的に設けられているので、幅方向で上下部の厚みが異なるため、巻回電極体を形成した場合に正極板の位置ずれが発生するのを防ぐ目的で合剤の剥離部分に絶縁テープを貼り付けたものを用いている。
【0012】
しかしながら、この図7に記載されている非水電解質二次電池は、円筒状巻回電極体の形で使用するものであるから、偏平巻回電極体として使用する際の問題点については何も示唆されてはいない。すなわち、円筒状巻回電極体は、押し潰されることがないため、偏平巻回電極体のように押し潰されることにより生じる応力に起因する問題点は本質的に生じないからである。
【0013】
【特許文献1】
特開2000−277155号公報(段落[0002]〜[0006])
【特許文献2】
特開2002−42881号公報(段落[0002]〜[0013])
【特許文献3】
特開平8−7877号公報(段落[0002]〜[0008])
【0014】
【発明が解決しようとする課題】
このように、偏平巻回電極体を使用するラミネート電池には、押し潰して偏平巻回電極体を製造するため、タブが電極の端部に存在している場合、タブが存在する電極のすぐ外側はラミネート外装体であり、フラットな面となっているので、タブの厚みの出っ張りは内側にしわ寄せが来る。したがって、正極タブ及び絶縁テープが存在しているため、偏平巻回電極体は内面へ向かって凹凸ができてしまうので、ラミネート電池内への電解液の注入時及び充電ガス発生時の気泡が、この凹凸状態となった部分にたまりやすいという問題点が存在していた。
【0015】
本発明者は、上述の問題点を解決すべく種々検討を重ねた結果、偏平巻回電極体を使用するラミネート電池において、正極タブを正極の中間部分に設けられた芯体箔露出部に設けると、正極タブ及びこの正極タブを絶縁する絶縁テープが存在してもその厚みに凹凸が生じないようにでき、しかも、電解液注入後に再度偏平巻回電極体を加圧すると、偏平巻回電極体内に溜まっていた気泡を有効に除去することができるので、結果として電池の容量を大きくすることができることを見出し、本発明を完成するに至ったのである。
【0016】
すなわち、本発明は、偏平巻回電極体を有するラミネート電池において、従来のものよりも電解液の含液性を向上させて電池容量の増大を計ったラミネート電池及び該ラミネート電池の製造方法を提供することを目的とする。
【0017】
【課題を解決するための手段】
本発明の目的は、以下の構成により達成することができる。本発明の第1の態様によれば、少なくとも、金属製芯体箔上に正極タブが設けられていると共にリチウムイオンを吸蔵放出する正極活物質を含む正極合剤が塗布された正極と、金属製芯体箔上に負極タブが設けられていると共にリチウムイオンを吸蔵放出する負極活物質を含む負極合剤が塗布された負極との間にセパレータを配置し、正極及び負極をセパレータにより互いに絶縁した状態で積層巻回した後、押し潰して成形した偏平巻回電極体と、ラミネート外装を有するラミネート電池において、該正極の長手方向の中央部付近の表裏に正極合剤不塗布部分を設け、該正極合剤不塗布部分の一方の面に正極タブを溶着して露出面を絶縁テープで被覆するとともに、該正極合剤不塗布部分の他方の面を絶縁テープで被覆したラミネート電池が提供される。
【0018】
係る態様によれば、正極タブ及びこの正極タブを絶縁する絶縁テープが存在しても偏平巻回電極体内に凹凸が生じないようにできるので、内部に気泡が溜まりにくくなり、結果として電池の容量が増加する。すなわち、タブが電極の中央に存在している場合、タブは電極と電極との間に挟まれる。電極には活物質合剤が両面に塗布されているが、タブの部分は合剤が除去されているから、タブの領域は合剤両面分の厚みだけ空間が確保される。したがって、そこにタブや絶縁テープが収まることによって出っ張りが無くなるので、偏平巻回電極体の内部に凹凸が生じないようになる。
【0019】
係る態様によれば、前記正極は、巻き始め及び巻き終わりの芯体箔表面が露出しないように正極合剤塗布部において切断されていることが好ましい。このような構成であれば、巻き初め及び巻き終わりの芯体箔表面を露出させる必要はないので、その分だけ活物質合剤の塗布量を増加させることができ、電池の容量をより増加させることができる。すなわち、従来は正極端部にタブがあったためにその部分の活物質合剤を除去していたが、本発明では、正極タブが中央部にあるので端部の活物質合剤を除去する必要はなくなる。
【0020】
また、係る態様によれば、前記ラミネート電池が三方封止式の電池であることが好ましい。このような構成であればラミネート電池の製造が容易になる。さらに、係る態様によれば、前記ラミネート電池がポリマー電解質を有するものとすることが好ましい。かかる構成であれば、電解質がゲル化ないしは固体化しているので漏液することが少なくなる。更に、係る態様においては、前記負極タブが前記負極の巻き始めに位置していることが好ましい。係る態様によれば、従来から普通に使用されている負極を使用することができる。
【0021】
また、本発明の第2の態様によれば、下記(1)〜(4)の工程から成るラミネート電池の製造方法が提供される。
(1)正極と負極とをセパレータを介して巻回し、巻回電極体を形成する工程、(2)前記巻回電極体を押し潰し成形して偏平巻回電極体を形成する工程、
(3)前記巻回電極体をラミネート被覆すると共に電解液を注入する工程
(4)前記ラミネート被覆された巻回電極体を押圧する工程。
このような方法を採用すれば、偏平巻回電極体内に溜まっていた気泡を有効に除去することができるので、結果として電池の容量を大きくすることができる。
【0022】
【発明の実施の形態】
次に本発明の好ましい態様について説明するが、以下に示す実施例は本発明の技術思想を具体化するためのラミネート電池及びその製造方法を例示するものであって、本発明はこれらに限定されるものではない。
【0023】
【実施例】
以下、図面を参照して本発明の実施例を詳細に説明する。図1(A)は巻き回前の正極の平面図及び図1(B)は底面図であり、図2は巻き回前の負極の平面図、図3は巻き回後の正極の要部拡大断面図である。
【0024】
本発明のラミネート電池の製造においては、アルミニウム等の金属製芯体箔上にリチウムイオンを吸蔵放出する正極活物質を含む正極合剤を塗布した正極と、銅等の金属製芯体箔上にリチウムイオンを吸蔵放出する負極活物質を含む負極合剤を塗布した負極とを2枚のセパレータにより絶縁して巻き取り、積層巻回されたものを加圧成型して偏平な巻回電極体とする。
【0025】
正極には、例えばコバルト酸リチウムLiCoO2を活物質とし、導電剤として炭素、結着剤としてポリ四フッ化エチレン樹脂を練り合わせペースト状とした合剤が、負極には例えば黒鉛等炭素材料を活物質とし、結着剤としてポリ四フッ化エチレン樹脂を練り合わせペースト状とした合剤が用いられている。これらの合剤はそれぞれの芯体箔基材の両面に塗布、乾燥、圧延し、所定の寸法に切断される。また、セパレータにはポリエチレン、ポリプロピレン等の微多孔性フィルムが使用される。
【0026】
図1(A)に示したように、巻き回前の正極1には、その正極1の長手方向の中央部付近に両面に正極合剤7の不塗布部分2が設けられ、この不塗布部分2に正極タブ3が溶接されている。さらに、正極タブ3には、補強と絶縁を兼ねた粘着テープのような絶縁テープ4が不塗布部分2の正極芯体箔5に貼り付けられ、また、その背面の正極活物質が設けられていない部分にも保護テープ6が施こされ、正極芯体箔表面が露出しないように被覆されている。これらのテープは、正極合剤7の不塗布部分2のみを覆い、隣接する正極合剤7層にはかからないように施される。なお、不塗布部分2は基材への合剤塗布時に不塗布部分を設けるか、基材に合剤を全面塗布しプレス加工後合剤を剥離して設ける方法があり、何れの方法を採用してもよい。そして、正極1の両端は、正極合剤7の塗布された部分で切断されており、正極1の端部まで活物質合剤が塗布されている。
【0027】
図2は、巻き回前の負極21の平面図で、その巻き始め端部21aに負極タブ22が溶接され、負極タブ溶接部の上は絶縁テープ23で覆われている。負極タブ溶接部の負極芯体箔24を介した対向面は、負極活物質合剤が塗布された負極活物質層となっている。
【0028】
正極1及び負極21を図示しないセパレータを介して重ねて巻き取り、積層巻回されたものを加圧成型して従来例のものと同様な偏平巻回電極体とする。この状態における正極1のタブ3の部分は、合剤が除去されているので合剤両面分の厚みだけ空間が確保されている。したがって、図3に示したように、そこにタブや絶縁テープが収まることによって、正極1のタブ3の部分の厚みは正極1と略同じになるので、従来例のように巻回電極体内に凹凸が生じることはなく、特に応力が加わっている部分が生じることがない。このようにして成型した巻回電極体をアルミラミネートシートを二つ折り状に折り曲げて底部を形成したものに挿入し、まず最初にトップ封止部側とサイド封止部の一方側を溶着して、サイド封止部の他方側が開口しているラミネート外装体を形成した。
【0029】
次いで、サイド封止部の未溶着部分からラミネート外装体内に有機電解液を注液した。電解液は、ポリマー電解質形成材料からなり、所定の割合に混合した混合溶媒に6フッ化リン酸リチウムを1mol/lの割合で溶解した電解液とポリプロピレングリコールジアクリレート
【化1】
又は、ポリプロピレングリコールジメタクリレート
【化2】
(ただし、n=3)
を、重量比で12:1の割合で混合した溶液に重合開始剤としてt−へキシルパーオキシピパレートを5000ppm添加して形成し、巻回電極体を収納したラミネート包材の内部に注液した。
【0030】
なお、電解質としてはLiPF6のほかにLiBF4、LiN(SO2CF3)2、LiN(SO2C2F5)2及びこれらを混合したものを用いることができる。次いで、電解液を注液したラミネート外装体の他方のサイド側を仮溶着した後、60℃オーブン中に3時間静置して熱硬化させ、予備充電及びエージングを行った。
【0031】
結いで、仮溶着されていたラミネートのサイド部の片側(残り側)を、金型で溶着して本封止部を形成した。予備室の不要部分を切断除去し、サイド封止部を折り曲げてリチウムラミネート電池を得た。
【0032】
本発明のラミネート電池に係る実施例と、正極タブを金属製芯体箔の巻き初めに設けた従来のラミネート電池に係る比較例とについて、それぞれ電池サイズ2.6×80×120mm、公称容量2200mAh(公称電圧3.6V)の電池を作製し、以下に述べる条件下で充放電試験を行った。
(1)充電:初期には2200mAの定電流で充電し、電池電圧が4.2Vまで上昇したときに定電流充電から定電圧充電に切換えた。定電圧充電では電池電圧を4.2Vに保つように、充電の進行に伴って電流値を低下させていき、電流値が440mAになったときに充電終了とした。
(2)放電:2200mAの定電流で放電させ、電池電圧が3Vまで低下したときに放電終了とした。
その測定結果を結果を表1にまとめて示す。
【0033】
【表1】
【0034】
上記の表により、本発明の実施例の方が比較例に比べ大きい容量が得られたことが分かる。
【0035】
【発明の効果】
以上述べたように、本発明のラミネート電池によれば、正極タブが正極の長さ方向中央部付近に配置されていることにより、偏平巻回電極体の凹凸が抑制され、含液性及びガス抜け性が向上し、結果として従来のラミネート電池より電池容量が増大するという効果が得られる。
【図面の簡単な説明】
【図1】本発明の巻回前の正極を示し、図1(A)は平面図、図1(B)は底面図である。
【図2】本発明の巻回前の負極の平面図である。
【図3】本発明の巻回加圧成形後の正極の要部拡大断面図
【図4】従来の巻回される前の電極の平面図である。
【図5】従来のラミネート電池の製造方法を示す図である。
【図6】従来の偏平巻回電極体の押し潰し成形後の正極タブ部の断面図である。
【図7】従来の長さ方向中央部にタブを有する巻回される前の電極の平面図である。
【符号の説明】
1 正極
2 不塗布部分
3 正極タブ
4 絶縁テープ
5 正極芯体箔
6 保護テープ
7 正極合剤
21 負極
21a 負極巻き始め端部
22 負極タブ
23 絶縁テープ
24 負極芯体箔[0001]
TECHNICAL FIELD OF THE INVENTION
The present invention relates to a laminated battery, and particularly to a laminated battery using a flat wound electrode, improves the liquid content and outgassing property of the electrolyte, and eliminates the defects such as poor insulation between the positive and negative electrodes to improve the reliability. Related to an enhanced laminated battery.
[0002]
[Prior art]
With the rapid spread of portable electronic devices, the requirements for batteries used in them have become stricter year by year, and in particular, smaller and thinner, higher capacity, superior cycle characteristics, and stable performance are required. ing. In the field of secondary batteries, lithium non-aqueous electrolyte secondary batteries, which have a higher energy density than other batteries, are attracting attention, and the proportion of lithium non-aqueous electrolyte secondary batteries has shown a significant growth in the secondary battery market. ing.
[0003]
The lithium non-aqueous electrolyte secondary battery includes a negative electrode in which a negative electrode mixture containing a negative electrode active material that inserts and desorbs lithium ions is applied to both surfaces of a negative electrode core (current collector) formed of a long and thin sheet-like copper foil, A separator made of a microporous polypropylene film or the like is placed between a positive electrode coated with a positive electrode mixture containing a positive electrode active material that absorbs and releases lithium ions on both surfaces of a positive electrode core made of an elongated sheet-like aluminum foil, etc. Then, after winding the negative electrode and the positive electrode in a cylindrical or elliptical shape in a state in which they are insulated from each other by a separator, in the case of a prismatic battery, further crush the wound electrode body to form a flat shape, and form each of the negative electrode and the positive electrode. It is manufactured by connecting a negative electrode tab and a positive electrode tab to predetermined portions, respectively, and covering the outside with an exterior.
[0004]
In a conventional non-aqueous electrolyte secondary battery, a non-aqueous electrolyte battery is manufactured by inserting a wound electrode body into a cylindrical outer can and then injecting a non-aqueous electrolyte. As shown in FIG. 4, the electrode body is provided with an
[0005]
By the way, in the above-mentioned non-aqueous electrolyte secondary battery, a metal outer can is mainly used in order to provide an outer casing and to provide strength. However, in recent years, the purpose is to reduce weight, increase battery capacity per unit volume, and the like. As a result, laminated batteries using a laminated film have been manufactured. Therefore, in order to understand the present invention, a conventional manufacturing process of the laminated
[0006]
First, the flat wound electrode body 11 is manufactured in the same manner as in the above-described conventional example. At this time, the flat wound electrode body 11 has a negative electrode tab 12 welded to the negative electrode metal core foil exposed portion and a positive electrode tab 13 also welded to the positive electrode metal core foil exposed portion. deep. Subsequently, as shown in FIG. 5A, a well-known laminated
[0007]
Next, as shown in FIG. 5B, a first
[0008]
Thus, also in the conventional laminated battery, the tab of each electrode is arranged on the core foil at the beginning or end of the winding of each electrode, and the surface of this tab does not cause a short circuit between the pair of electrodes. To do so, it is covered with an insulating tape like the electrodes shown in FIG. In addition, particularly when the negative electrode active material is present on the opposite surface of the positive electrode core foil, the conductive powder detached from the negative electrode active material tends to cause a short circuit. It may be covered with an insulating tape (see Patent Document 2).
[0009]
Therefore, a positive electrode in which a positive electrode mixture containing a positive electrode active material that absorbs and releases lithium ions is applied on a metal core foil, and a negative electrode that contains a negative electrode active material that inserts and releases lithium ions on a metal core foil The negative electrode coated with the mixture is wound in a state insulated from each other via two separators made of a microporous polypropylene film, and then crushed to produce a flat wound electrode body. Due to the presence of the insulating tape provided on the surface of the tab, irregularities are formed toward the inner surface of the flat wound electrode body. However, there is a problem that air bubbles during the injection of the gas and the generation of the charged gas tend to collect in the portion where the stress is applied.
[0010]
This phenomenon will be described in more detail with reference to the drawings. FIG. 6 is a cross-sectional view of the flat
[0011]
On the other hand, as a positive electrode of a cylindrical non-aqueous electrolyte secondary battery, a
In this positive electrode, since the positive electrode tab is partially provided in the width direction of the electrode plate, the thickness of the upper and lower portions differs in the width direction, so that when the wound electrode body is formed, the displacement of the positive electrode plate occurs. In order to prevent this, an adhesive tape is applied to a part where the mixture is peeled off.
[0012]
However, since the non-aqueous electrolyte secondary battery described in FIG. 7 is used in the form of a cylindrical wound electrode body, there is no problem with using it as a flat wound electrode body. Not suggested. That is, since the cylindrical wound electrode body is not crushed, there is essentially no problem caused by the stress caused by being crushed like the flat wound electrode body.
[0013]
[Patent Document 1]
JP-A-2000-277155 (paragraphs [0002] to [0006])
[Patent Document 2]
JP-A-2002-42881 (paragraphs [0002] to [0013])
[Patent Document 3]
JP-A-8-7877 (paragraphs [0002] to [0008])
[0014]
[Problems to be solved by the invention]
As described above, in the laminated battery using the flat wound electrode body, since the flat wound electrode body is manufactured by crushing, when the tab is present at the end of the electrode, the tab is located immediately adjacent to the electrode on which the tab is present. The outer side is a laminate exterior body and has a flat surface, so that the protrusion of the thickness of the tab is wrinkled inward. Therefore, since the positive electrode tab and the insulating tape are present, the flat wound electrode body has irregularities toward the inner surface, so that bubbles during the injection of the electrolyte solution into the laminated battery and the generation of the charging gas, There has been a problem that the uneven portion easily accumulates.
[0015]
The present inventor has conducted various studies to solve the above-described problems, and as a result, in a laminated battery using a flat wound electrode body, a positive electrode tab is provided on an exposed portion of a core foil provided in an intermediate portion of a positive electrode. Even if a positive electrode tab and an insulating tape for insulating the positive electrode tab are present, it is possible to prevent unevenness in the thickness thereof, and if the flat wound electrode body is pressed again after the injection of the electrolytic solution, the flat wound electrode The present inventors have found that since the air bubbles accumulated in the body can be effectively removed, the capacity of the battery can be increased as a result, and the present invention has been completed.
[0016]
That is, the present invention provides a laminated battery having a flat spirally wound electrode body in which the battery capacity is increased by improving the liquid content of the electrolytic solution as compared with the conventional battery, and a method of manufacturing the laminated battery. The purpose is to do.
[0017]
[Means for Solving the Problems]
The object of the present invention can be achieved by the following configurations. According to the first aspect of the present invention, at least a positive electrode on which a positive electrode tab is provided on a metal core foil and a positive electrode mixture containing a positive electrode active material that absorbs and releases lithium ions is applied; A negative electrode tab is provided on the core body foil, and a separator is arranged between the negative electrode coated with a negative electrode mixture containing a negative electrode active material that absorbs and releases lithium ions, and the positive electrode and the negative electrode are insulated from each other by the separator After being wound in a stacked state in a flat state, a flat wound electrode body crushed and formed, and in a laminated battery having a laminate exterior, a positive electrode mixture non-applied portion is provided on the front and back near the center in the longitudinal direction of the positive electrode, A laminated battery in which a positive electrode tab is welded to one surface of the positive electrode mixture non-applied portion and the exposed surface is covered with insulating tape, and the other surface of the positive electrode mixture non-applied portion is covered with insulating tape, It is subjected.
[0018]
According to this aspect, even when the positive electrode tab and the insulating tape insulating the positive electrode tab are present, unevenness can be prevented from being generated in the flat wound electrode body, so that bubbles hardly accumulate inside, and as a result, the capacity of the battery Increase. That is, when the tab is located at the center of the electrode, the tab is sandwiched between the electrodes. The active material mixture is applied to both sides of the electrode, but since the mixture is removed from the tab portion, a space is secured in the tab region by the thickness of both surfaces of the mixture. Therefore, since the tab or the insulating tape is settled therein, the protrusion is eliminated, so that the unevenness does not occur inside the flat wound electrode body.
[0019]
According to this aspect, it is preferable that the positive electrode is cut at the positive electrode mixture application portion so that the core foil surfaces at the start and end of winding are not exposed. With such a configuration, it is not necessary to expose the core foil surface at the beginning and end of winding, so that the application amount of the active material mixture can be increased by that amount, and the capacity of the battery is further increased. be able to. That is, conventionally, the active material mixture was removed at the end of the positive electrode because of the tab, but in the present invention, since the positive electrode tab is located at the center, it is necessary to remove the active material mixture at the end. Is gone.
[0020]
According to this aspect, it is preferable that the laminated battery is a three-way sealed battery. Such a configuration facilitates the manufacture of a laminated battery. Further, according to this aspect, it is preferable that the laminated battery has a polymer electrolyte. With such a configuration, the electrolyte is gelled or solidified, so that leakage is reduced. Further, in this aspect, it is preferable that the negative electrode tab is located at the beginning of winding of the negative electrode. According to this aspect, a conventionally used negative electrode can be used.
[0021]
According to a second aspect of the present invention, there is provided a method of manufacturing a laminated battery including the following steps (1) to (4).
(1) a step of winding a positive electrode and a negative electrode through a separator to form a wound electrode body; (2) a step of crushing and shaping the wound electrode body to form a flat wound electrode body;
(3) a step of laminating the wound electrode body and injecting an electrolytic solution; and (4) a step of pressing the laminated electrode body.
By adopting such a method, the air bubbles accumulated in the flat wound electrode body can be effectively removed, and as a result, the capacity of the battery can be increased.
[0022]
BEST MODE FOR CARRYING OUT THE INVENTION
Next, preferred embodiments of the present invention will be described. However, the following examples illustrate a laminated battery for embodying the technical idea of the present invention and a method for manufacturing the same, and the present invention is not limited thereto. Not something.
[0023]
【Example】
Hereinafter, embodiments of the present invention will be described in detail with reference to the drawings. 1A is a plan view of the positive electrode before winding, FIG. 1B is a bottom view, FIG. 2 is a plan view of the negative electrode before winding, and FIG. 3 is an enlarged main part of the positive electrode after winding. It is sectional drawing.
[0024]
In the production of the laminated battery of the present invention, a positive electrode prepared by applying a positive electrode mixture containing a positive electrode active material for absorbing and releasing lithium ions onto a metal core foil such as aluminum, and a metal core foil such as copper A negative electrode coated with a negative electrode mixture containing a negative electrode active material that absorbs and releases lithium ions is insulated by two separators and wound up. I do.
[0025]
For the positive electrode, for example, lithium cobalt oxide LiCoO 2 is used as an active material, carbon is used as a conductive agent, and a polytetrafluoroethylene resin is used as a binder. As a substance, a mixture in which a polytetrafluoroethylene resin is kneaded into a paste is used as a binder. These mixtures are applied to both sides of each core foil substrate, dried, rolled, and cut into predetermined dimensions. Further, a microporous film such as polyethylene or polypropylene is used for the separator.
[0026]
As shown in FIG. 1 (A), the
[0027]
FIG. 2 is a plan view of the
[0028]
The
[0029]
Next, an organic electrolyte solution was injected into the laminate exterior body from the unwelded portion of the side sealing portion. The electrolytic solution is composed of a polymer electrolyte forming material, and an electrolytic solution obtained by dissolving lithium hexafluorophosphate at a ratio of 1 mol / l in a mixed solvent mixed at a predetermined ratio and polypropylene glycol diacrylate.
Or, polypropylene glycol dimethacrylate
(However, n = 3)
Was formed by adding 5000 ppm of t-hexylperoxypiparate as a polymerization initiator to a solution obtained by mixing at a ratio of 12: 1 by weight, and injected into the inside of a laminate packaging material containing a wound electrode body. did.
[0030]
Note that, in addition to LiPF 6 , LiBF 4 , LiN (SO 2 CF 3 ) 2 , LiN (SO 2 C 2 F 5 ) 2 and a mixture thereof can be used as the electrolyte. Next, after temporarily welding the other side of the laminate exterior body into which the electrolyte was injected, the laminate exterior body was left standing in a 60 ° C. oven for 3 hours to be thermally cured, and precharged and aged.
[0031]
By tying, one side (remaining side) of the side portion of the temporarily welded laminate was welded with a mold to form a final sealed portion. Unnecessary portions of the preliminary chamber were cut and removed, and the side sealing portions were bent to obtain a lithium laminated battery.
[0032]
For the example of the laminated battery of the present invention and the comparative example of the conventional laminated battery in which the positive electrode tab was provided at the beginning of the winding of the metal core foil, the battery size was 2.6 × 80 × 120 mm and the nominal capacity was 2200 mAh, respectively. (Nominal voltage of 3.6 V) was prepared, and a charge / discharge test was performed under the following conditions.
(1) Charging: The battery was initially charged at a constant current of 2200 mA, and was switched from constant current charging to constant voltage charging when the battery voltage rose to 4.2 V. In the constant voltage charging, the current value was decreased as the charging progressed so as to keep the battery voltage at 4.2 V, and the charging was terminated when the current value reached 440 mA.
(2) Discharge: Discharge was performed at a constant current of 2200 mA, and discharge was terminated when the battery voltage dropped to 3 V.
Table 1 summarizes the measurement results.
[0033]
[Table 1]
[0034]
From the above table, it can be seen that a larger capacity was obtained in the example of the present invention than in the comparative example.
[0035]
【The invention's effect】
As described above, according to the laminated battery of the present invention, since the positive electrode tab is disposed near the center in the length direction of the positive electrode, unevenness of the flat wound electrode body is suppressed, and the liquid-containing property and gas It is possible to obtain the effect that the removability is improved, and as a result, the battery capacity is increased as compared with the conventional laminated battery.
[Brief description of the drawings]
FIG. 1 shows a positive electrode before winding according to the present invention, wherein FIG. 1 (A) is a plan view and FIG. 1 (B) is a bottom view.
FIG. 2 is a plan view of a negative electrode before winding according to the present invention.
FIG. 3 is an enlarged cross-sectional view of a main part of a positive electrode after wound pressure molding of the present invention. FIG. 4 is a plan view of a conventional electrode before being wound.
FIG. 5 is a diagram showing a conventional method for manufacturing a laminated battery.
FIG. 6 is a cross-sectional view of a positive electrode tab after a conventional flat wound electrode body is crushed and formed.
FIG. 7 is a plan view of a conventional unwound electrode having a tab at the center in the longitudinal direction.
[Explanation of symbols]
DESCRIPTION OF
Claims (6)
(1)正極と負極とをセパレータを介して巻回し、巻回電極体を形成する工程、(2)前記巻回電極体を押し潰し成形して偏平巻回電極体を形成する工程、
(3)前記巻回電極体をラミネート被覆すると共に電解液を注入する工程、
(4)前記ラミネート被覆された巻回電極体を押圧する工程。A method for manufacturing a laminated battery, comprising the following steps (1) to (4).
(1) a step of winding a positive electrode and a negative electrode through a separator to form a wound electrode body; (2) a step of crushing and shaping the wound electrode body to form a flat wound electrode body;
(3) laminating the wound electrode body and injecting an electrolyte solution;
(4) A step of pressing the wound electrode body coated with the laminate.
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