JP6065847B2 - リチウム二次電池及びリチウム二次電池用電解液 - Google Patents
リチウム二次電池及びリチウム二次電池用電解液 Download PDFInfo
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- JP6065847B2 JP6065847B2 JP2013558728A JP2013558728A JP6065847B2 JP 6065847 B2 JP6065847 B2 JP 6065847B2 JP 2013558728 A JP2013558728 A JP 2013558728A JP 2013558728 A JP2013558728 A JP 2013558728A JP 6065847 B2 JP6065847 B2 JP 6065847B2
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- negative electrode
- active material
- electrode active
- lithium secondary
- secondary battery
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- 229910052744 lithium Inorganic materials 0.000 title claims description 52
- 239000003792 electrolyte Substances 0.000 title claims description 17
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- 239000008151 electrolyte solution Substances 0.000 claims description 38
- 150000001875 compounds Chemical class 0.000 claims description 36
- -1 carbonate ester Chemical class 0.000 claims description 30
- 239000011871 silicon-based negative electrode active material Substances 0.000 claims description 17
- 125000004433 nitrogen atom Chemical group N* 0.000 claims description 8
- 125000002947 alkylene group Chemical group 0.000 claims description 7
- RTZKZFJDLAIYFH-UHFFFAOYSA-N ether Substances CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 7
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- 125000002534 ethynyl group Chemical group [H]C#C* 0.000 claims description 6
- 125000001424 substituent group Chemical group 0.000 claims description 6
- 229910052796 boron Inorganic materials 0.000 claims description 5
- 125000004432 carbon atom Chemical group C* 0.000 claims description 5
- 125000001820 oxy group Chemical group [*:1]O[*:2] 0.000 claims description 5
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- 238000007606 doctor blade method Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 229920001971 elastomer Polymers 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 239000010419 fine particle Substances 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 125000000623 heterocyclic group Chemical group 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 1
- 229910003437 indium oxide Inorganic materials 0.000 description 1
- PJXISJQVUVHSOJ-UHFFFAOYSA-N indium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[In+3].[In+3] PJXISJQVUVHSOJ-UHFFFAOYSA-N 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- FUJCRWPEOMXPAD-UHFFFAOYSA-N lithium oxide Chemical compound [Li+].[Li+].[O-2] FUJCRWPEOMXPAD-UHFFFAOYSA-N 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 238000003701 mechanical milling Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
- 229910052753 mercury Inorganic materials 0.000 description 1
- VNKYTQGIUYNRMY-UHFFFAOYSA-N methoxypropane Chemical compound CCCOC VNKYTQGIUYNRMY-UHFFFAOYSA-N 0.000 description 1
- CXHHBNMLPJOKQD-UHFFFAOYSA-M methyl carbonate Chemical compound COC([O-])=O CXHHBNMLPJOKQD-UHFFFAOYSA-M 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- VIJMMQUAJQEELS-UHFFFAOYSA-N n,n-bis(ethenyl)ethenamine Chemical compound C=CN(C=C)C=C VIJMMQUAJQEELS-UHFFFAOYSA-N 0.000 description 1
- FOZKDADHFVKERQ-UHFFFAOYSA-N n,n-diethynylethynamine Chemical compound C#CN(C#C)C#C FOZKDADHFVKERQ-UHFFFAOYSA-N 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 239000011356 non-aqueous organic solvent Substances 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- AHHWIHXENZJRFG-UHFFFAOYSA-N oxetane Chemical compound C1COC1 AHHWIHXENZJRFG-UHFFFAOYSA-N 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 239000012466 permeate Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 229920005575 poly(amic acid) Polymers 0.000 description 1
- 238000006116 polymerization reaction Methods 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 125000001436 propyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 238000010298 pulverizing process Methods 0.000 description 1
- 230000002040 relaxant effect Effects 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 239000005060 rubber Substances 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 239000002210 silicon-based material Substances 0.000 description 1
- 239000011856 silicon-based particle Substances 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 229910052714 tellurium Inorganic materials 0.000 description 1
- PORWMNRCUJJQNO-UHFFFAOYSA-N tellurium atom Chemical compound [Te] PORWMNRCUJJQNO-UHFFFAOYSA-N 0.000 description 1
- YBDQLHBVNXARAU-ZCFIWIBFSA-N tetrahydro-2-methyl-2H-pyran Natural products C[C@@H]1CCCCO1 YBDQLHBVNXARAU-ZCFIWIBFSA-N 0.000 description 1
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- VPYJNCGUESNPMV-UHFFFAOYSA-N triallylamine Chemical compound C=CCN(CC=C)CC=C VPYJNCGUESNPMV-UHFFFAOYSA-N 0.000 description 1
- RQNVJDSEWRGEQR-UHFFFAOYSA-N tris(prop-2-enyl) borate Chemical compound C=CCOB(OCC=C)OCC=C RQNVJDSEWRGEQR-UHFFFAOYSA-N 0.000 description 1
- 238000007740 vapor deposition Methods 0.000 description 1
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 1
- 239000002759 woven fabric Substances 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
Images
Classifications
-
- 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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/134—Electrodes based on metals, Si or alloys
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- 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
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
-
- 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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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Physics & Mathematics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
- Inorganic Chemistry (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
Description
電解液が、式(1)
2 負極集電体
3 負極
4 正極活物質層
5 正極集電体
6 正極
7 セパレーター
8 外装体
11 リチウム二次電池
負極は、充放電に伴いリチウムイオンを可逆的に吸蔵、放出可能なケイ素系負極活物質を含み、負極活物質が負極結着剤により一体化された負極活物質層として集電体上に積層された構造を有する。
正極は、充放電に伴いリチウムイオンを可逆的に吸蔵、放出可能な正極活物質を含み、正極活物質が正極結着剤により一体化された正極活物質層として集電体上に積層された構造を有する。
電解液は、充放電時に正極負極においてリチウムの吸蔵放出を可能とするため、正極と負極を漬浸してリチウムイオンを溶解可能な非水系の有機溶媒に、電解質を溶解したものである。
H−(CX1X2−CX3X4)n−CH2O−CX5X6−CX7X8−H
で表されるものが好ましい。式中、nは1、2、3又は4を示し、X1〜X8は独立してフッ素原子又は水素原子を示す。但し、X1〜X4の少なくとも1つはフッ素原子を示し、X5〜X8の少なくとも1つはフッ素原子を示す。
H−(CF2−CF2)n−CH2O−CF2−CF2−H
で表されるものがより好ましい。式中、nは1又は2であることがより好ましい。
セパレーターは、正極及び負極の導通を抑制し、荷電体の透過を阻害せず、電解液に対して耐久性を有するものであれば、いずれであってもよい。セパレーターの材質としては、具体的には、ポリプロピレン、ポリエチレン等のポリオレフィン系微多孔膜、セルロース、ポリエチレンテレフタレート、ポリイミド、ポリフッ化ビニリデン等を採用することができる。これらは、多孔質フィルム、織物、不織布等として用いることができる。
外装体としては、上記正極及び負極、セパレーター、電解液を安定して保持可能な強度を有し、これらの物質に対して電気化学的に安定で、水密性を有するものが好ましい。外装体の材質としては、具体的には、例えば、ステンレス、ニッケルメッキを施した鉄、アルミニウム、シリカ、アルミナをコーティングしたラミネートフィルムを用いることができ、ラミネートフィルムに用いる樹脂としては、ポリエチレン、ポリプロピレン、ポリエチレンテレフタレート等を用いることができる。これらは、1層又は2層以上の構造体であってもよい。
上記二次電池の形状は、上記円筒型、扁平捲回角型、積層角型、コイン型、扁平捲回ラミネート型、又は積層ラミネート型のいずれでもよい。
[リチウム二次電池の作製]
負極活物質として、ケイ素が非晶質酸化ケイ素(SiOx、0<x≦2)中に分散したケイ素系粒子表面に炭素被覆が形成されたケイ素系負極活物質を得た。ケイ素系負極活物質の、ケイ素、非晶質酸化ケイ素、炭素の質量比は29:61:10であった。この負極活物質と、負極用結着剤としてのポリイミドの前駆体であるポリアミック酸とを、90:10の質量比で計量し、それらをn−メチルピロリドンと混合して、負極スラリーとした。負極スラリーを厚さ10μmの銅箔に塗布した後に乾燥し、さらに窒素雰囲気300℃の熱処理を行い、負極を作製した。
得られたリチウム二次電池を60℃の恒温槽中で2.5Vから4.2Vの電圧範囲で重充放電を反復して行った。充放電サイクル100回目と、250回目の放電容量を測定した。初回の放電量に対する、100回サイクル後の放電容量比、250回サイクル後の放電容量比を算出し、容量維持率を得た。結果を表1に示す。
電解液中のトリエチニルベンゼンの含有量を表1に示すように変更したこと以外は、実施例1と同様にして、リチウム二次電池を作製し、充放電サイクル特性の評価を行った。結果を表1に示す。
末端不飽和化合物として、トリエチニルベンゼンに替えて式(3)で示されるトリプロパルギルアミン(化合物(B))を1質量%含有する電解液を用いたこと以外は、実施例1と同様にして、リチウム二次電池を作製し、充放電サイクル特性の評価を行った。結果を表1に示す。
末端不飽和化合物を用いなかったこと以外は、実施例1と同様にしてリチウム二次電池を作製し、充放電サイクル特性の評価を行った。結果を表1に示す。
Claims (7)
- 式(1)中、R1〜R3が同一であることを特徴とする請求項1記載のリチウム二次電池。
- 電解液が、炭酸エステル及びエーテル化合物から選ばれる何れか1種以上を含むことを特徴とする請求項1又は2に記載のリチウム二次電池。
- 負極が、粒子状のケイ素系負極活物質を含む負極活物質層を有し、充放電に伴い粒子状のケイ素系負極活物質に前記不飽和化合物の重合体を含む被膜が形成されることを特徴とする請求項1から3の何れかに記載のリチウム二次電池。
- 式(1)中、R 1 〜R 3 が同一であることを特徴とする請求項5記載のリチウム二次電池用電解液。
- 炭酸エステル及びエーテル化合物から選ばれる何れか1種以上を含むことを特徴とする請求項5又は6に記載のリチウム二次電池用電解液。
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