JP5241314B2 - ラミネート形非水二次電池 - Google Patents
ラミネート形非水二次電池 Download PDFInfo
- Publication number
- JP5241314B2 JP5241314B2 JP2008125386A JP2008125386A JP5241314B2 JP 5241314 B2 JP5241314 B2 JP 5241314B2 JP 2008125386 A JP2008125386 A JP 2008125386A JP 2008125386 A JP2008125386 A JP 2008125386A JP 5241314 B2 JP5241314 B2 JP 5241314B2
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- Prior art keywords
- positive electrode
- secondary battery
- separator
- layer
- laminated
- Prior art date
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- MSYLJRIXVZCQHW-UHFFFAOYSA-N formaldehyde;6-phenyl-1,3,5-triazine-2,4-diamine Chemical compound O=C.NC1=NC(N)=NC(C=2C=CC=CC=2)=N1 MSYLJRIXVZCQHW-UHFFFAOYSA-N 0.000 description 1
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- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- MRNHPUHPBOKKQT-UHFFFAOYSA-N indium;tin;hydrate Chemical compound O.[In].[Sn] MRNHPUHPBOKKQT-UHFFFAOYSA-N 0.000 description 1
- 230000002401 inhibitory effect Effects 0.000 description 1
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- 229910052742 iron Inorganic materials 0.000 description 1
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 1
- NLYAJNPCOHFWQQ-UHFFFAOYSA-N kaolin Chemical compound O.O.O=[Al]O[Si](=O)O[Si](=O)O[Al]=O NLYAJNPCOHFWQQ-UHFFFAOYSA-N 0.000 description 1
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- 239000004571 lime Substances 0.000 description 1
- 229910002102 lithium manganese oxide Inorganic materials 0.000 description 1
- VLXXBCXTUVRROQ-UHFFFAOYSA-N lithium;oxido-oxo-(oxomanganiooxy)manganese Chemical compound [Li+].[O-][Mn](=O)O[Mn]=O VLXXBCXTUVRROQ-UHFFFAOYSA-N 0.000 description 1
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- KXKVLQRXCPHEJC-UHFFFAOYSA-N methyl acetate Chemical compound COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 description 1
- 229940017219 methyl propionate Drugs 0.000 description 1
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- PYLWMHQQBFSUBP-UHFFFAOYSA-N monofluorobenzene Chemical compound FC1=CC=CC=C1 PYLWMHQQBFSUBP-UHFFFAOYSA-N 0.000 description 1
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- 229910052901 montmorillonite Inorganic materials 0.000 description 1
- 229910052863 mullite Inorganic materials 0.000 description 1
- GKTNLYAAZKKMTQ-UHFFFAOYSA-N n-[bis(dimethylamino)phosphinimyl]-n-methylmethanamine Chemical class CN(C)P(=N)(N(C)C)N(C)C GKTNLYAAZKKMTQ-UHFFFAOYSA-N 0.000 description 1
- 150000002825 nitriles Chemical class 0.000 description 1
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- VSIIXMUUUJUKCM-UHFFFAOYSA-D pentacalcium;fluoride;triphosphate Chemical compound [F-].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O VSIIXMUUUJUKCM-UHFFFAOYSA-D 0.000 description 1
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- FVSKHRXBFJPNKK-UHFFFAOYSA-N propionitrile Chemical compound CCC#N FVSKHRXBFJPNKK-UHFFFAOYSA-N 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
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- ZUHZGEOKBKGPSW-UHFFFAOYSA-N tetraglyme Chemical compound COCCOCCOCCOCCOC ZUHZGEOKBKGPSW-UHFFFAOYSA-N 0.000 description 1
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- 239000010457 zeolite Substances 0.000 description 1
Images
Classifications
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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- Cell Separators (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
- Sealing Battery Cases Or Jackets (AREA)
Description
P = 100−(Σai/ρi)×(m/t) (1)
ここで、前記式中、ai:質量%で表した成分iの比率、ρi:成分iの密度(g/cm3)、m:セパレータの単位面積あたりの質量(g/cm2)、t:セパレータの厚み(cm)である。
<セパレータの作製>
有機バインダであるSBRのエマルジョン(固形分比率40質量%):100gと水:4000gとを容器に入れ、均一に分散するまで室温で攪拌した。この分散液に、耐熱温度が150℃以上のフィラーであるベーマイト粉末(板状、平均粒径1μm、アスペクト比10):4000gを4回に分けて加え、ディスパーにより2800rpmで5時間攪拌して均一なスラリー[多孔質層(II)形成用スラリー]を調製した。ポリエチレン製微孔性フィルム[微孔性フィルム層(I):厚み16μm、空孔率40%、平均孔径0.02μm、融点135℃]上に、前記のスラリーをマイクログラビアコーターによって塗布し、乾燥して多孔質層(II)を形成することで、厚みが22μmのセパレータを得た。得られたセパレータを裁断して、110mm×210mmのサイズのセパレータを複数用意した。
LiCoO2:96質量部、アセチレンブラック:2質量部、およびPVDF:2質量部を混合し、更に、炭酸リチウムを3質量%となる量で添加して正極合剤を調製し、更にこの正極合剤をNMPに分散させて、正極合剤含有ペーストを調製した。得られた正極合剤含有ペーストを、厚みが15μmのアルミニウム箔からなる集電体の両面に塗布し、乾燥後、プレス処理を施して正極合剤層を形成し、正極を得た。得られた正極の正極合剤層の厚みは、集電体の片面あたり50μmであった。その後、得られた正極を、正極合剤層の形成部分が幅105mm、長さ200mmとなり、更にリード体となる正極集電体の露出部も含む形状に裁断した。
黒鉛:98質量%に、SBR:1.5質量%およびCMC:0.5質量%を加えて混合し、更に水を加えて負極合剤含有ペーストを調製した。得られた負極合剤含有ペーストを、厚みが10μmの銅箔からなる集電体の両面に塗布し、乾燥後、プレス処理を施して負極合剤層を形成し、負極を得た。得られた負極の負極合剤層の厚みは、集電体の片面あたり52μmであった。その後、得られた負極を、負極合剤層の形成部分が幅110mm、長さ205mmとなり、更にリード体となる負極集電体の露出部も含む形状に裁断した。
前記の正極7枚と、前記の負極8枚とを、前記のセパレータを介して積層し、積層電極体とした。なお、セパレータは、その微孔性フィルム層(I)が正極と対向するように配置し、各正極の両面に配置したセパレータ同士を、その正極合剤層の外周縁の外側の箇所で熱融着し、各正極を、その両面に配置された2枚のセパレータによって包むようにした。次に、前記の積層電極体に係る各正極の正極リード体をアルミニウム製の正極端子に超音波溶接し、更に各負極の負極リード体を銅製の負極端子に超音波溶接した。
炭酸リチウムを添加しない以外は、実施例1と同様にして正極を作製した。また、シクロヘキシルベンゼンを3質量%の濃度となるように添加した以外は、実施例1と同様にして液状の非水電解質を調製した。
正極合剤層における炭酸リチウムの量を2質量%とした以外は、実施例1と同様にして正極を作製した。また、シクロヘキシルベンゼンを1.5質量%の濃度となるように添加した以外は、実施例1と同様にして液状の非水電解質を調製した。
実施例2で作製したものと同じ正極を用いた以外は、実施例1と同様にしてラミネート形非水二次電池を作製した。すなわち、比較例1のラミネート形非水二次電池は、正極合剤層、非水電解質のいずれにも、電池の電圧が4.3V以上となった場合に正極活物質と反応して気体を発生する添加剤を含有していない。
積層電極体におけるセパレータの配置を、微孔性フィルム層(I)が負極と対向するようにした以外は、実施例1と同様にしてラミネート形非水二次電池を作製した。
PE製微孔性フィルム[微孔性フィルム層(I)]の厚みを40μmとし、多孔質層(II)に代えて、厚みが50μmのPP製不織布を用い、微孔性フィルム層(I)を負極側に配置した以外は、実施例3と同様にしてラミネート形非水二次電池を作製した。
実施例1〜3および比較例1〜3の電池について、前記の「電池の組み立て」の工程でかかった時間(組み立て時間)を調べ、その作業性を評価した。
実施例1〜3および比較例1〜3の電池について、2A(1C)の定電流値で4.2Vまで充電を行い、次いで4.2Vの定電圧で充電を行う定電流−定電圧充電を3時間行い、0.4A(0.2C)の電流値で3Vまで放電させて、放電容量を求めた。
実施例1〜3および比較例1〜3の電池について、放電容量測定時と同じ条件で充電した後、4A(2C)の電流値で3Vまで放電させて、放電容量(B)を求めた。そして、前記の放電容量測定により求めた放電容量[放電容量(A)]と、放電容量(B)とを用いて、下記式により各電池の負荷特性を評価した。
負荷特性=100×(B)/(A)
実施例1〜3および比較例1〜3の電池(放電状態のもの)を恒温槽に入れ、30℃から150℃まで毎分5℃の割合で温度上昇させて加熱し、電池の内部抵抗の温度変化を求めた。そして、抵抗値が30℃での値の5倍以上に上昇したときの温度を、シャットダウン温度とした。
実施例1〜3および比較例1〜3の電池に12Vの電圧を3時間加えることにより過充電を行い、充電中の電池表面での温度を測定して、最高温度を過充電時の到達温度とした。
2 ラミネート容器
3 正極端子
4 負極端子
5 正極
6 負極
7 セパレータ
Claims (15)
- リチウムイオンを吸蔵・放出できる活物質を含む負極と、活物質であるリチウム含有酸化物を含む正極合剤層を有する正極とが、セパレータを介して積層されており、かつ前記負極と前記正極の少なくとも一方を複数有する平板状の積層電極体、および非水電解質が、ラミネート容器に収容されたラミネート形非水二次電池であって、
前記セパレータは、熱可塑性樹脂を主体とする微孔性フィルム層(I)と、耐熱温度が150℃以上のフィラーを主体として含む多孔質層(II)とを少なくとも有しており、かつ正極と対向する層が微孔性フィルム層(I)であり、
電池の電圧が4.3V以上となった場合に正極活物質と反応して気体を発生する添加剤を、前記正極合剤層または前記非水電解質に含有しており、
前記非水電解質が、3次元架橋構造を形成するゲル化剤によりゲル状となっていることを特徴とするラミネート形非水二次電池。 - 正極が、セパレータの微孔性フィルム層(I)で包まれている請求項1に記載のラミネート形非水二次電池。
- 正極合剤層の含有する前記添加剤が、炭酸リチウムまたは蓚酸リチウムである請求項1または2に記載のラミネート形非水二次電池。
- 正極合剤層における前記添加剤の含有量が、1.5〜5質量%である請求項3に記載のラミネート形非水二次電池。
- 非水電解質の含有する前記添加剤が、ベンゼン環を有する芳香族化合物である請求項1〜4のいずれかに記載のラミネート形非水二次電池。
- 非水電解質の含有する前記添加剤が、ビフェニル、シクロヘキシルベンゼン、またはこれらの誘導体である請求項5に記載のラミネート形非水二次電池。
- 非水電解質における前記添加剤の含有量が、1〜5質量%である請求項5または6に記載のラミネート形非水二次電池。
- セパレータの厚みが、6〜40μmである請求項1〜7のいずれかに記載のラミネート形非水二次電池。
- 多孔質層(II)に含まれるフィラーの少なくとも一部が板状粒子である請求項1〜8のいずれかに記載のラミネート形非水二次電池。
- 多孔質層(II)に含まれるフィラーの少なくとも一部が、一次粒子が凝集した二次粒子構造を有する微粒子である請求項1〜9のいずれかに記載のラミネート形非水二次電池。
- 多孔質層(II)に含まれるフィラーが、アルミナ、シリカおよびベーマイトよりなる群から選択される少なくとも1種の粒子である請求項1〜10のいずれかに記載のラミネート形非水二次電池。
- 多孔質層(II)が、耐熱温度が150℃以上の多孔質基体を有している請求項1〜11のいずれかに記載のラミネート形非水二次電池。
- ゲル化剤が、脂環エポキシ基を有する化合物、またはオキセタン構造を有する化合物である請求項1〜12のいずれかに記載のラミネート形非水二次電池。
- 非水電解質におけるゲル化剤の濃度が、1.5〜3質量%である請求項1〜13のいずれかに記載のラミネート形非水二次電池。
- ラミネート容器が、アルミニウムまたはステンレス鋼製で、厚みが20〜100μmの金属箔と、前記金属箔の電池内側に配置された熱融着性樹脂層とを有する金属ラミネートフィルムにより構成されたものである請求項1〜14のいずれかに記載のラミネート形非水二次電池。
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JP5451426B2 (ja) * | 2010-01-28 | 2014-03-26 | 日立マクセル株式会社 | 電池用セパレータおよびそれを用いたリチウムイオン二次電池 |
JP2012113875A (ja) * | 2010-11-22 | 2012-06-14 | Hitachi Maxell Energy Ltd | 非水電解質電池モジュール |
JP5389772B2 (ja) * | 2010-12-07 | 2014-01-15 | 株式会社日立製作所 | リチウム二次電池 |
US9196926B2 (en) | 2010-12-27 | 2015-11-24 | Nec Energy Devices, Ltd. | Gel electrolyte for lithium ion secondary battery, and lithium ion secondary battery |
WO2012172586A1 (ja) * | 2011-06-13 | 2012-12-20 | 株式会社 日立製作所 | リチウム二次電池 |
JPWO2012172586A1 (ja) * | 2011-06-13 | 2015-02-23 | 株式会社日立製作所 | リチウム二次電池 |
JP5848545B2 (ja) * | 2011-08-08 | 2016-01-27 | 三星エスディアイ株式会社Samsung SDI Co.,Ltd. | 二次電池用セパレータ層及び二次電池 |
JP5820704B2 (ja) * | 2011-11-21 | 2015-11-24 | 株式会社日立製作所 | 積層型電池 |
JP5333617B2 (ja) * | 2012-02-03 | 2013-11-06 | 株式会社豊田自動織機 | 電極収納セパレータ、蓄電装置及び車両 |
KR101904160B1 (ko) * | 2012-02-08 | 2018-10-05 | 에스케이이노베이션 주식회사 | 내열성 및 안정성이 우수한 폴리올레핀계 복합 미세다공막 및 이의 제조방법 |
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JP5842742B2 (ja) * | 2012-06-15 | 2016-01-13 | 株式会社豊田自動織機 | 電極収納セパレータ及び蓄電装置 |
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