JP6251680B2 - セパレータ及びそれを備える電気化学素子 - Google Patents
セパレータ及びそれを備える電気化学素子 Download PDFInfo
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- JP6251680B2 JP6251680B2 JP2014535673A JP2014535673A JP6251680B2 JP 6251680 B2 JP6251680 B2 JP 6251680B2 JP 2014535673 A JP2014535673 A JP 2014535673A JP 2014535673 A JP2014535673 A JP 2014535673A JP 6251680 B2 JP6251680 B2 JP 6251680B2
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- separator
- lithium
- inorganic particles
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- coating layer
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims description 14
- 229910001416 lithium ion Inorganic materials 0.000 claims description 13
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 12
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- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 claims description 9
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- XCKPLVGWGCWOMD-YYEYMFTQSA-N 3-[[(2r,3r,4s,5r,6r)-6-[(2s,3s,4r,5r)-3,4-bis(2-cyanoethoxy)-2,5-bis(2-cyanoethoxymethyl)oxolan-2-yl]oxy-3,4,5-tris(2-cyanoethoxy)oxan-2-yl]methoxy]propanenitrile Chemical compound N#CCCO[C@H]1[C@H](OCCC#N)[C@@H](COCCC#N)O[C@@]1(COCCC#N)O[C@@H]1[C@H](OCCC#N)[C@@H](OCCC#N)[C@H](OCCC#N)[C@@H](COCCC#N)O1 XCKPLVGWGCWOMD-YYEYMFTQSA-N 0.000 claims description 3
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- MKGYHFFYERNDHK-UHFFFAOYSA-K P(=O)([O-])([O-])[O-].[Ti+4].[Li+] Chemical compound P(=O)([O-])([O-])[O-].[Ti+4].[Li+] MKGYHFFYERNDHK-UHFFFAOYSA-K 0.000 claims description 3
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- 229910020231 Pb(Mg1/3Nb2/3)O3-xPbTiO3 Inorganic materials 0.000 claims description 3
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- CJNBYAVZURUTKZ-UHFFFAOYSA-N hafnium(IV) oxide Inorganic materials O=[Hf]=O CJNBYAVZURUTKZ-UHFFFAOYSA-N 0.000 claims description 3
- 229910000659 lithium lanthanum titanates (LLT) Inorganic materials 0.000 claims description 3
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- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
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- H01M50/411—Organic material
- H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
- H01M50/417—Polyolefins
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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
- 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
- H01M50/44—Fibrous material
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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
Description
したがって、バインダー高分子はなるべく誘電率が高いものが望ましい。実際、電解液における塩の解離度は電解液溶媒の誘電率に依存するため、バインダー高分子の誘電率が高いほど電解質における塩の解離度を向上させることができる。このようなバインダー高分子の誘電率は1.0ないし100(測定周波数=1kHz)範囲が使用可能であり、特に10以上であることが望ましい。
ポリフッ化ビニリデン‐クロロトリフルオロエチレン共重合体(PVdF‐CTFE)及びシアノエチルプルランを10:2の重量比でそれぞれアセトンに添加し、50℃で約12時間溶解させ、第1高分子溶液を製造した。Al2O3粉末を高分子/無機物粒子=10/90重量比になるように、製造された第1高分子溶液に添加し、12時間ボールミル(ball mill)法で無機物粒子を粉砕及び分散させてスラリーを製造した。このように製造されたスラリーの無機物粒子の直径は平均600nmであった。
多孔性基材の一面にスライド‐スロット方式で下層にはスラリーを、上層には前記第1高分子溶液を塗布したものを除き、実施例1と同様の方法でセパレータを製造した。
ポリフッ化ビニリデン‐ヘキサフルオロプロピレン共重合体(PVdF‐HFP)を溶媒であるアセトンに溶解させ、第2高分子溶液を製造したものを除き、実施例1と同様にセパレータを製造した。このとき、スラリーがコーティングされた第1多孔性コーティング層の厚さは6.8μmであり、第2高分子溶液がコーティングされた第2多孔性コーティング層の厚さは0.9μmであることが確認された。このようにして製造されたセパレータの通気時間を測定したところ、1542sec/100ccに悪化したことが観察された。
実施例1で製造されたセパレータのバインダー薄膜のSEM写真を図2に、断面SEM写真を図3に示した。
10 多孔性基材
20 第1多孔性コーティング層
30 第2多孔性コーティング層
Claims (13)
- セパレータであって、
多孔性基材と、
前記多孔性基材の一面に形成された、無機物粒子と第1バインダー化合物との混合物を含む第1多孔性コーティング層と、
前記多孔性基材の他面の一部分のみに、溶媒と非溶媒と第2バインダー化合物との混合物で形成された第2多孔性コーティング層と、及び
前記第1多孔性コーティング層の表面に形成された、第3バインダー化合物を含む電極接着層とを備えてなり、
前記第2多孔性コーティング層の厚さが、0.5ないし0.9μmであり、
前記第2バインダー化合物が、ポリフッ化ビニリデン‐ヘキサフルオロプロピレン、ポリフッ化ビニリデン‐トリクロロエチレン、及びシアノエチルプルランからなる群より選択される何れか一種又はこれらの二種以上の混合物であることを特徴とする、セパレータ。 - 前記多孔性基材が、ポリオレフィン系多孔性基材であることを特徴とする、請求項1に記載のセパレータ。
- 前記ポリオレフィン系多孔性基材が、ポリエチレン、ポリプロピレン、ポリブチレン、及びポリペンテンからなる群より選択される何れか一種の化合物で形成されたことを特徴とする、請求項2に記載のセパレータ。
- 前記無機物粒子が、誘電率が5以上の無機物粒子、リチウムイオン伝達能力を有する無機物粒子、及びこれらの混合物からなる群より選択される無機物粒子であることを特徴とする、請求項1〜3の何れか一項に記載のセパレータ。
- 前記誘電率が5以上の無機物粒子が、BaTiO3、Pb(Zrx、Ti1-x)O3(PZT、0<x<1)、Pb1-xLaxZr1-yTiyO3(PLZT、0<x<1、0<y<1)、(1−x)Pb(Mg1/3Nb2/3)O3−xPbTiO3(PMN‐PT、0<x<1)、ハフニア(HfO2)、SrTiO3、SnO2、CeO2、MgO、NiO、CaO、ZnO、ZrO2、SiO2、Y2O3、Al2O3、SiC、及びTiO2からなる群より選択される何れか一種又はこれら二種以上の混合物であることを特徴とする、請求項4に記載のセパレータ。
- 前記リチウムイオン伝達能力を有する無機物粒子が、リチウムホスフェート(Li3PO4)、リチウムチタンホスフェート(LixTiy(PO4)3、0<x<2、0<y<3)、リチウムアルミニウムチタンホスフェート(LixAlyTiz(PO4)3、0<x<2、0<y<1、0<z<3)、(LiAlTiP)xOy系列ガラス(0<x<4、0<y<13)、リチウムランタンチタネート(LixLayTiO3、0<x<2、0<y<3)、リチウムゲルマニウムチオホスフェート(LixGeyPzSw、0<x<4、0<y<1、0<z<1、0<w<5)、リチウムナイトライド(LixNy、0<x<4、0<y<2)、SiS2(LixSiySz、0<x<3、0<y<2、0<z<4)系列ガラス
及びP2S5(LixPySz、0<x<3、0<y<3、0<z<7)系列ガラスからなる群より選択される何れか一種又はこれら二種以上の混合物であることを特徴とする、請求項4又は5に記載のセパレータ。 - 前記第1バインダー化合物及び前記第2バインダー化合物が、それぞれ独立して、ポリフッ化ビニリデン‐ヘキサフルオロプロピレン、ポリフッ化ビニリデン‐トリクロロエチレン、ポリメチルメタクリレート、ポリブチルアクリレート、ポリアクリロニトリル、ポリビニルピロリドン、ポリビニルアセテート、ポリビニルアルコール、エチレンビニルアセテート共重合体、ポリエチレンオキサイド、ポリアリレート、セルロースアセテート、セルロースアセテートブチレート、セルロースアセテートプロピオネート、シアノエチルプルラン、シアノエチルポリビニルアルコール、シアノエチルセルロース、シアノエチル
スクロース、プルラン、カルボキシルメチルセルロース、及び分子量10,000g/mol以下の低分子化合物からなる群より選択される何れか一種又はこれらの二種以上の混合物であることを特徴とする、請求項1〜6の何れか一項に記載のセパレータ。 - 前記溶媒が、アセトン、テトラヒドロフラン、メチレンクロライド、クロロホルム、ジメチルホルムアミド、N‐メチル‐2‐ピロリドン、及びシクロヘキサンのうちから選択される何れか一種又はこれらの二種以上の混合物であることを特徴とする、請求項1〜7の何れか一項に記載のセパレータ。
- 前記非溶媒が、メタノール、エタノール、イソプロピルアルコール及び水のうちから選択される何れか一種又はこれら二種以上の混合物であることを特徴とする、請求項1〜8の何れか一項に記載のセパレータ。
- 前記溶媒と前記非溶媒との重量比が、50:50ないし99:1であることを特徴とする、請求項1〜9の何れか一項に記載のセパレータ。
- 前記第3バインダー化合物が、ポリフッ化ビニリデン‐ヘキサフルオロプロピレン、ポリフッ化ビニリデン‐トリクロロエチレン、ポリメチルメタクリレート、ポリブチルアクリレート、ポリアクリロニトリル、ポリビニルピロリドン、ポリビニルアセテート、ポリビニルアルコール、エチレンビニルアセテート共重合体、ポリエチレンオキサイド、ポリアリレート、セルロースアセテート、セルロースアセテートブチレート、セルロースアセテートプロピオネート、シアノエチルプルラン、シアノエチルポリビニルアルコール、シアノエチルセルロース、シアノエチルスクロース、プルラン、カルボキシルメチルセルロース、及び分子量10,000g/mol以下の低分子化合物からなる群より選択される何れか一種又はこれらの二種以上の混合物であることを特徴とする、請求項1〜10の何れか一項に記載のセパレータ。
- 電気化学素子であって、
正極と、負極と、前記正極と前記負極との間に介在したセパレータとを備えてなるものであり、
前記セパレータが、請求項1〜11の何れか一項に記載のセパレータであることを特徴とする、電気化学素子。 - 前記電気化学素子が、リチウム二次電池であることを特徴とする、請求項12に記載の電気化学素子。
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US20130280583A1 (en) | 2013-10-24 |
US10033024B2 (en) | 2018-07-24 |
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EP2779275A1 (en) | 2014-09-17 |
EP2779275A4 (en) | 2016-03-02 |
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