JP5319947B2 - 非水電解質電池 - Google Patents
非水電解質電池 Download PDFInfo
- Publication number
- JP5319947B2 JP5319947B2 JP2008078740A JP2008078740A JP5319947B2 JP 5319947 B2 JP5319947 B2 JP 5319947B2 JP 2008078740 A JP2008078740 A JP 2008078740A JP 2008078740 A JP2008078740 A JP 2008078740A JP 5319947 B2 JP5319947 B2 JP 5319947B2
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- Japan
- Prior art keywords
- negative electrode
- positive electrode
- active material
- separator
- lithium
- Prior art date
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- 239000011255 nonaqueous electrolyte Substances 0.000 title claims description 55
- 239000002245 particle Substances 0.000 claims description 41
- -1 lithium phosphorus metal compound Chemical class 0.000 claims description 36
- 239000007773 negative electrode material Substances 0.000 claims description 30
- 239000000945 filler Substances 0.000 claims description 27
- 229910052809 inorganic oxide Inorganic materials 0.000 claims description 26
- 239000011149 active material Substances 0.000 claims description 22
- 239000003792 electrolyte Substances 0.000 claims description 17
- FDLZQPXZHIFURF-UHFFFAOYSA-N [O-2].[Ti+4].[Li+] Chemical compound [O-2].[Ti+4].[Li+] FDLZQPXZHIFURF-UHFFFAOYSA-N 0.000 claims description 16
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- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 10
- 229920002647 polyamide Polymers 0.000 claims description 10
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims description 4
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 4
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 4
- KLARSDUHONHPRF-UHFFFAOYSA-N [Li].[Mn] Chemical compound [Li].[Mn] KLARSDUHONHPRF-UHFFFAOYSA-N 0.000 claims description 4
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 4
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- 239000010450 olivine Substances 0.000 claims description 3
- 229910052609 olivine Inorganic materials 0.000 claims description 3
- 229910052596 spinel Inorganic materials 0.000 claims description 3
- 239000011029 spinel Substances 0.000 claims description 3
- KUNSUQLRTQLHQQ-UHFFFAOYSA-N copper tin Chemical group [Cu].[Sn] KUNSUQLRTQLHQQ-UHFFFAOYSA-N 0.000 claims description 2
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- 229910052751 metal Inorganic materials 0.000 description 25
- 239000002184 metal Substances 0.000 description 25
- 229910052782 aluminium Inorganic materials 0.000 description 22
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 21
- 239000006258 conductive agent Substances 0.000 description 19
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 12
- 229910001416 lithium ion Inorganic materials 0.000 description 12
- 239000010936 titanium Substances 0.000 description 12
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 11
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- 239000011135 tin Substances 0.000 description 9
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 8
- 239000002033 PVDF binder Substances 0.000 description 8
- 239000007789 gas Substances 0.000 description 8
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- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 6
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- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 4
- 239000011572 manganese Substances 0.000 description 4
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- RAXXELZNTBOGNW-UHFFFAOYSA-O Imidazolium Chemical compound C1=C[NH+]=CN1 RAXXELZNTBOGNW-UHFFFAOYSA-O 0.000 description 3
- 229910013063 LiBF 4 Inorganic materials 0.000 description 3
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 3
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- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 3
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 3
- 150000002892 organic cations Chemical class 0.000 description 3
- 239000002861 polymer material Substances 0.000 description 3
- 229910052719 titanium Inorganic materials 0.000 description 3
- WNXJIVFYUVYPPR-UHFFFAOYSA-N 1,3-dioxolane Chemical compound C1COCO1 WNXJIVFYUVYPPR-UHFFFAOYSA-N 0.000 description 2
- 238000004438 BET method Methods 0.000 description 2
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 2
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 description 2
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 description 2
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 2
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 2
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 2
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 2
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- 229910003002 lithium salt Inorganic materials 0.000 description 2
- 159000000002 lithium salts Chemical class 0.000 description 2
- ILXAVRFGLBYNEJ-UHFFFAOYSA-K lithium;manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[O-]P([O-])([O-])=O ILXAVRFGLBYNEJ-UHFFFAOYSA-K 0.000 description 2
- 229910052749 magnesium Inorganic materials 0.000 description 2
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- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 2
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- 229910052723 transition metal Inorganic materials 0.000 description 2
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- GEWWCWZGHNIUBW-UHFFFAOYSA-N 1-(4-nitrophenyl)propan-2-one Chemical compound CC(=O)CC1=CC=C([N+]([O-])=O)C=C1 GEWWCWZGHNIUBW-UHFFFAOYSA-N 0.000 description 1
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- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 1
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- 229910013684 LiClO 4 Inorganic materials 0.000 description 1
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- 125000004122 cyclic group Chemical group 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
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- 150000002642 lithium compounds Chemical class 0.000 description 1
- 229910002102 lithium manganese oxide Inorganic materials 0.000 description 1
- ACFSQHQYDZIPRL-UHFFFAOYSA-N lithium;bis(1,1,2,2,2-pentafluoroethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)C(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)C(F)(F)F ACFSQHQYDZIPRL-UHFFFAOYSA-N 0.000 description 1
- SBWRUMICILYTAT-UHFFFAOYSA-K lithium;cobalt(2+);phosphate Chemical compound [Li+].[Co+2].[O-]P([O-])([O-])=O SBWRUMICILYTAT-UHFFFAOYSA-K 0.000 description 1
- LRVBJNJRKRPPCI-UHFFFAOYSA-K lithium;nickel(2+);phosphate Chemical compound [Li+].[Ni+2].[O-]P([O-])([O-])=O LRVBJNJRKRPPCI-UHFFFAOYSA-K 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
- 230000007774 longterm Effects 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
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- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
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- HNJBEVLQSNELDL-UHFFFAOYSA-N pyrrolidin-2-one Chemical compound O=C1CCCN1 HNJBEVLQSNELDL-UHFFFAOYSA-N 0.000 description 1
- 125000001453 quaternary ammonium group Chemical group 0.000 description 1
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- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
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Images
Classifications
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- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/446—Composite material consisting of a mixture of organic and inorganic materials
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- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
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- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
- H01M10/0587—Construction or manufacture of accumulators having only wound construction elements, i.e. wound positive electrodes, wound negative electrodes and wound separators
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
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- H01—ELECTRIC ELEMENTS
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/5825—Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
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Description
前記負極の活物質は、一次粒子の平均粒径が0.001〜1μmであり、かつ
前記セパレータは、セルロース、ポリオレフィンまたはポリアミドからなる多孔質層とこの多孔質層に分散された無機酸化物フィラーとを含む複合材で、60%〜80%の多孔度を有することを特徴する非水電解質電池が提供される。
正極、負極、セパレータおよび非水電解質を収納する外装容器は、金属製容器またはラミネートフィルム製容器を使用することができる。
正極は、正極集電体と、この集電体の片面もしくは両面に担持され、活物質、導電剤および結着剤を含む正極層とを有する。
負極は、集電体と、この集電体の片面もしくは両面に担持され、活物質、導電剤および結着剤を含む負極層とを有する。
セパレータは、正極および負極の間に介在され、セルロース、ポリオレフィンまたはポリアミドからなる多孔質層とこの多孔質層に分散して担持された無機酸化物フィラーとを含む複合材で、60%〜80%の多孔度を有する。このようなセパレータは、80℃から190℃の高温環境下でその中の樹脂成分が熱収縮から融解状態になっても正極と負極の短絡現象を抑制し高い信頼を維持することが可能になる。
セルロースおよび無機酸化物フィラーを水に分散させた後、抄紙技術で漉くことによりセルロースからなる多孔質層とこの多孔質層に分散された無機酸化物フィラーとを含む複合材で、60%〜80%の多孔度を有するセパレータを作製する。
ポリオレフィンまたはポリアミドと無機酸化物フィラーを溶媒に溶解した後、この溶解物を所望の厚さにフィルム化する。このフィルムをその中の溶媒を蒸発(揮散)させながら延伸することにより、主に溶媒が分散した箇所に気孔を形成してポリオレフィンまたはポリアミドからなる多孔質層(多数の開放気孔を持つ微孔性樹脂フィルム)とこの多孔質層に分散された無機酸化物フィラーとを含む複合材で、60%〜80%の多孔度を有するセパレータを作製する。
非水電解質は、電解質を有機溶媒に溶解することにより調製される液状の有機電解質、液状の有機溶媒と高分子材料を複合化したゲル状の有機電解質、またはリチウム塩電解質と高分子材料を複合化した固体非水電解質が挙げられる。また、リチウムイオンを含有した常温溶融塩(イオン性融体)を非水電解質として使用してもよい。高分子材料は、例えばポリフッ化ビニリデン(PVdF)、ポリアクリロニトリル(PAN)、ポリエチレンオキサイド(PEO)等を挙げることができる。
炭素微粒子(平均粒子径0.005μm)が表面に付着(付着量0.1重量%)した一次粒子の平均粒子径0.1μmのオリビン構造のリチウムリン酸鉄(LiFePO4)を正極活物質として用い、この正極活物質87重量部と導電剤である繊維径0.1μmの気相成長の炭素繊維3重量部および黒鉛粉末5重量部と、結着剤であるPVdF5重量部とをn−メチルピロリドン(NMP)溶媒に分散してスラリーを調製した。得られたスラリーを集電体である厚さ15μmのアルミニウム合金箔(純度99%)の両面に塗布し、乾燥し、プレス工程を経て、片面の正極層の厚さが43μm、極密度が2.2g/cm3の正極を作製した。正極層の比表面積は、5m2/gであった。その後、アルミニウムからなる帯状の正極リードをアルミニウム合金箔に溶接して電気的に接続した。
下記表1に示すセパレータ、正極活物質、負極活物質を用いた以外、前述した実施例1と同様な方法で15種の薄型の非水電解質電池を組み立てた。なお、セパレータの多孔質層に複合化される無機物フィラーは、いずれも平均粒子径0.3μmの粒子である。
Claims (5)
- 外装容器と、この外装容器内に収納された正極、セパレータおよびリチウムチタン酸化物を活物質として含む負極と、前記外装容器内に収容された非水電解質とを具備した非水電解質電池であって、
前記負極の活物質は、一次粒子の平均粒径が0.001〜1μmであり、かつ
前記セパレータは、セルロース、ポリオレフィンまたはポリアミドからなる多孔質層とこの多孔質層に分散された無機酸化物フィラーとを含む複合材で、60%〜80%の多孔度を有することを特徴する非水電解質電池。 - 前記無機酸化物フィラーは、平均粒子径が1μm以下のアルミナ、シリカ、チタニア、マグネシア、チタニアおよびジルコニアからなる群から選ばれる1つ以上の粒子で、前記多孔質層中に10〜90重量%の割合で分散されることを特徴する請求項1記載の非水電解質電池。
- 前記セパレータは、セルロースからなる多孔質層と、この多孔質層に分散された無機酸化物フィラーとしての平均粒子径1μm以下のアルミナとを含む複合材であることを特徴する請求項1記載の非水電解質電池。
- 前記リチウムチタン酸化物は、スピネル構造、アナターゼ構造、ブロンズ構造またはラムスデライト構造を有するリチウムチタン酸化物であることを特徴する請求項1〜3いずれか1項記載の非水電解質電池。
- 前記正極は、オリビン構造を有するリチウムリン金属化合物またはリチウムマンガン複合酸化物を活物質として含むことを特徴する請求項1〜4いずれか1項記載の非水電解質電池。
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PCT/JP2009/054003 WO2009119262A1 (en) | 2008-03-25 | 2009-02-25 | Non-aqueous electrolyte battery |
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JP4213687B2 (ja) * | 2005-07-07 | 2009-01-21 | 株式会社東芝 | 非水電解質電池及び電池パック |
JP4599314B2 (ja) * | 2006-02-22 | 2010-12-15 | 株式会社東芝 | 非水電解質電池、電池パック及び自動車 |
KR100820162B1 (ko) * | 2006-08-07 | 2008-04-10 | 한국과학기술연구원 | 내열성 초극세 섬유상 분리막 및 그 제조 방법과, 이를 이용한 이차전지 |
JP2009146822A (ja) * | 2007-12-17 | 2009-07-02 | Panasonic Corp | 非水電解質二次電池 |
JP5334282B2 (ja) * | 2008-02-20 | 2013-11-06 | 日立マクセル株式会社 | リチウム二次電池 |
-
2008
- 2008-03-25 JP JP2008078740A patent/JP5319947B2/ja active Active
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2009
- 2009-02-25 KR KR1020107015603A patent/KR101312860B1/ko active IP Right Grant
- 2009-02-25 KR KR1020127025877A patent/KR101335909B1/ko active IP Right Grant
- 2009-02-25 CN CN2009801022700A patent/CN101911373A/zh active Pending
- 2009-02-25 WO PCT/JP2009/054003 patent/WO2009119262A1/en active Application Filing
- 2009-02-25 CN CN201510541073.6A patent/CN105161704A/zh active Pending
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KR20120125400A (ko) | 2012-11-14 |
KR101312860B1 (ko) | 2013-09-30 |
WO2009119262A1 (en) | 2009-10-01 |
JP2009231245A (ja) | 2009-10-08 |
KR20100098559A (ko) | 2010-09-07 |
CN101911373A (zh) | 2010-12-08 |
US20100297490A1 (en) | 2010-11-25 |
CN105161704A (zh) | 2015-12-16 |
KR101335909B1 (ko) | 2013-12-02 |
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