JP6105226B2 - 非水電解質二次電池 - Google Patents
非水電解質二次電池 Download PDFInfo
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- JP6105226B2 JP6105226B2 JP2012177491A JP2012177491A JP6105226B2 JP 6105226 B2 JP6105226 B2 JP 6105226B2 JP 2012177491 A JP2012177491 A JP 2012177491A JP 2012177491 A JP2012177491 A JP 2012177491A JP 6105226 B2 JP6105226 B2 JP 6105226B2
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- Prior art keywords
- separator
- electrode plate
- negative electrode
- positive electrode
- adhesive layer
- Prior art date
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- 239000011255 nonaqueous electrolyte Substances 0.000 title claims description 52
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- DEUISMFZZMAAOJ-UHFFFAOYSA-N lithium dihydrogen borate oxalic acid Chemical compound B([O-])(O)O.C(C(=O)O)(=O)O.C(C(=O)O)(=O)O.[Li+] DEUISMFZZMAAOJ-UHFFFAOYSA-N 0.000 claims description 3
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- 239000004020 conductor Substances 0.000 description 1
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- 239000011889 copper foil Substances 0.000 description 1
- 150000005676 cyclic carbonates Chemical class 0.000 description 1
- 150000004292 cyclic ethers Chemical class 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 239000002283 diesel fuel Substances 0.000 description 1
- DGTVXEHQMSJRPE-UHFFFAOYSA-M difluorophosphinate Chemical compound [O-]P(F)(F)=O DGTVXEHQMSJRPE-UHFFFAOYSA-M 0.000 description 1
- PWRLWCQANJNXOR-UHFFFAOYSA-N dilithium chloro(dioxido)borane Chemical compound [Li+].[Li+].[O-]B([O-])Cl PWRLWCQANJNXOR-UHFFFAOYSA-N 0.000 description 1
- 150000004862 dioxolanes Chemical class 0.000 description 1
- NJLLQSBAHIKGKF-UHFFFAOYSA-N dipotassium dioxido(oxo)titanium Chemical compound [K+].[K+].[O-][Ti]([O-])=O NJLLQSBAHIKGKF-UHFFFAOYSA-N 0.000 description 1
- 150000002019 disulfides Chemical class 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000005038 ethylene vinyl acetate Substances 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- 229920001973 fluoroelastomer Polymers 0.000 description 1
- NBVXSUQYWXRMNV-UHFFFAOYSA-N fluoromethane Chemical compound FC NBVXSUQYWXRMNV-UHFFFAOYSA-N 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 229910003472 fullerene Inorganic materials 0.000 description 1
- 239000006232 furnace black Substances 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 239000003502 gasoline Substances 0.000 description 1
- 229910052732 germanium Inorganic materials 0.000 description 1
- PVADDRMAFCOOPC-UHFFFAOYSA-N germanium monoxide Inorganic materials [Ge]=O PVADDRMAFCOOPC-UHFFFAOYSA-N 0.000 description 1
- 239000003365 glass fiber Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- CJNBYAVZURUTKZ-UHFFFAOYSA-N hafnium(iv) oxide Chemical compound O=[Hf]=O CJNBYAVZURUTKZ-UHFFFAOYSA-N 0.000 description 1
- 229910021385 hard carbon Inorganic materials 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 239000001863 hydroxypropyl cellulose Substances 0.000 description 1
- 235000010977 hydroxypropyl cellulose Nutrition 0.000 description 1
- 239000003273 ketjen black Substances 0.000 description 1
- 238000004898 kneading Methods 0.000 description 1
- 239000006233 lamp black Substances 0.000 description 1
- 229910052745 lead Inorganic materials 0.000 description 1
- 239000001989 lithium alloy Substances 0.000 description 1
- 229910000664 lithium aluminum titanium phosphates (LATP) Inorganic materials 0.000 description 1
- 229910000625 lithium cobalt oxide Inorganic materials 0.000 description 1
- HSZCZNFXUDYRKD-UHFFFAOYSA-M lithium iodide Inorganic materials [Li+].[I-] HSZCZNFXUDYRKD-UHFFFAOYSA-M 0.000 description 1
- 229910000659 lithium lanthanum titanates (LLT) Inorganic materials 0.000 description 1
- 229910001386 lithium phosphate Inorganic materials 0.000 description 1
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 description 1
- VROAXDSNYPAOBJ-UHFFFAOYSA-N lithium;oxido(oxo)nickel Chemical compound [Li+].[O-][Ni]=O VROAXDSNYPAOBJ-UHFFFAOYSA-N 0.000 description 1
- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical compound [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000011302 mesophase pitch Substances 0.000 description 1
- 239000002905 metal composite material Substances 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 229940017219 methyl propionate Drugs 0.000 description 1
- 229910003465 moissanite Inorganic materials 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 150000005181 nitrobenzenes Chemical class 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- LYGJENNIWJXYER-UHFFFAOYSA-N nitromethane Chemical compound C[N+]([O-])=O LYGJENNIWJXYER-UHFFFAOYSA-N 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 230000000737 periodic effect Effects 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 229920001200 poly(ethylene-vinyl acetate) Polymers 0.000 description 1
- 229920003229 poly(methyl methacrylate) Polymers 0.000 description 1
- 229920005569 poly(vinylidene fluoride-co-hexafluoropropylene) Polymers 0.000 description 1
- 229920001197 polyacetylene Polymers 0.000 description 1
- 229920002239 polyacrylonitrile Polymers 0.000 description 1
- 239000004926 polymethyl methacrylate Substances 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- 229920002689 polyvinyl acetate Polymers 0.000 description 1
- 239000011118 polyvinyl acetate Substances 0.000 description 1
- 229920000131 polyvinylidene Polymers 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 230000001681 protective effect Effects 0.000 description 1
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 1
- 239000001008 quinone-imine dye Substances 0.000 description 1
- 239000004627 regenerated cellulose Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- VSZWPYCFIRKVQL-UHFFFAOYSA-N selanylidenegallium;selenium Chemical compound [Se].[Se]=[Ga].[Se]=[Ga] VSZWPYCFIRKVQL-UHFFFAOYSA-N 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 239000008107 starch Substances 0.000 description 1
- 235000019698 starch Nutrition 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
- 229920005608 sulfonated EPDM Polymers 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- JBQYATWDVHIOAR-UHFFFAOYSA-N tellanylidenegermanium Chemical compound [Te]=[Ge] JBQYATWDVHIOAR-UHFFFAOYSA-N 0.000 description 1
- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical group FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 description 1
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 1
- 239000006234 thermal black Substances 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical group 0.000 description 1
- BDZBKCUKTQZUTL-UHFFFAOYSA-N triethyl phosphite Chemical compound CCOP(OCC)OCC BDZBKCUKTQZUTL-UHFFFAOYSA-N 0.000 description 1
- TWQULNDIKKJZPH-UHFFFAOYSA-K trilithium;phosphate Chemical compound [Li+].[Li+].[Li+].[O-]P([O-])([O-])=O TWQULNDIKKJZPH-UHFFFAOYSA-K 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- 229910001935 vanadium oxide Inorganic materials 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
- 238000004804 winding Methods 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
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- H—ELECTRICITY
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- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
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- 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
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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Description
従来、非水電解質二次電池の低温放電特性を向上させるために、非水系電解液にジフルオロリン酸塩を添加するような提案がされている(下記特許文献1参照)。
また、上記非水電解質中にはLiBOB及び/又はLiBOBに由来するホウ素含有物質が存在していることが望ましく、更に、電池が真空封止されていることが望ましい。
LiNi0.35Co0.35Mn0.30O2で表され層状構造を有する正極活物質と、導電剤としてのカーボンブラックと、結着剤としてのPVDF(ポリフッ化ビニリデン)とを、N−メチル−2−ピロリドン溶液中で混練して、正極合剤スラリーを調製する。尚、該正極合剤スラリーにおいて、正極活物質とカーボンブラックとPVDFとの割合は限定するものではないが、例えば、質量比で88:9:3とすることができる。次に、上記正極合剤スラリーを、アルミニウム箔から成る方形状の正極集電体の両面に塗布し、乾燥させた後、圧延ローラーを用いて圧延することにより、正極集電体の両面に正極合剤層が形成された正極板1を作製することができる。
増粘剤であるCMC(カルボキシメチルセルロース)を水に溶解した溶液に、負極活物質である黒鉛粉末を投入して攪拌混合した後、さらに、結着剤であるSBR(スチレン・ブタジエンゴム)を混合して負極合剤スラリーを調製する。尚、該負極合剤スラリーにおいて、黒鉛とCMCとSBRとの割合は限定するものではないが、例えば、質量比で、98:1:1とすることができる。次に、該負極合剤スラリーを、銅箔から成る方形状の負極集電体の両面に塗布し、乾燥させた後、圧延ローラーを用いて圧延することにより、負極集電体の両面に負極合剤層が形成された負極板2を作製することができる。
例えば、エチレンカーボネート(EC)とメチルエチルカーボネート(MEC)とから成る混合溶媒に、溶質としてのリチウム塩を溶解させる。この場合、ECとMECの割合は限定するものではないが、例えば、25℃において、体積比3:7の割合で混合すれば良い。また、溶質としてのリチウム塩の種類やその割合も限定するものではないが、例えば、LiPF6を1モル/リットル溶解させれば良い。また、非水電解質には、添加剤としてのリチウム塩であるLiPF2O2及び/又はLiBOB(リチウムビスオキサレートボラート)を添加する。これら添加剤の添加量は、例えば、LiPF2O2では0.05モル/リットル、LiBOBでは0.1モル/リットル添加すれば良い。但し、LiPF2O2やLiBOBの添加量はこれに限定するものではなく、LiPF2O2では0.01〜2モル/リットル、より好ましくは0.01〜0.1モル/リットルであれば良く、LiBOBでは0.01〜2モル/リットル、より好ましくは0.01〜0.2モル/リットルであれば良い。このような範囲が好ましいのは、これら添加剤の添加量が少な過ぎると添加効果を十分に発揮できない一方、これら添加剤の添加量が多過ぎると非水電解質の粘度が高くなって充放電反応が円滑に行うことができないからである。尚、負極活物質の表面に被膜を形成して負極活物質の劣化を抑制すべく、非水電解質にビニレンカーボネート(VC)を添加しても良い。尚、VCの添加量は限定するものではないが、例えば、非水電解質に対して0.1〜5質量%程度添加すれば良い。
複数の上記正極板及び複数の上記負極板を、ポリエチレン製のセパレータを介して対向するように積層して積層型電極体を作製する。上記正極板から延出する正極集電タブと正極端子10とを固定(電気的に接続)し、上記負極板から延出する負極集電タブと負極端子11とを固定(電気的に接続)する。そして、積層型電極体を非水電解質と共にアルミニウムラミネート外装体内に配置し、ヒートシールすることにより、非水電解質二次電池(電池容量:16Ah)を作製できる。
更に、上記正極活物質を2種以上混合して用いることもできる。例えば、リチウムニッケルマンガンコバルト複合酸化物とスピネル型リチウムマンガン酸化物を混合して用いても良い。また、上記リチウム遷移金属化合物にはニッケル及び/又はマンガンが含有されていることが望ましい。
尚、負極を作製する際には、上述した正極板に用いる導電剤、結着剤、充填材を用いることもできる。
例えば、図2に示すように、方形状の第1セパレータ30を介して方形状の正極板1と負極板2とが配置された単位セル(このように両端に位置する電極が異なっている構造の単位セルを、以下、I型セルと称することがある。尚、このような定義なので、正極板1/第1セパレータ/負極板2/第1セパレータ30/正極板1/第1セパレータ30/負極板2となっているセルもI型セルに含まれる)31を有し、このI型セル31を複数重ね合わせる。そして、該重ね合わせたI型セル31間に、各I型セル31を包むように配置された帯状の第2セパレータ32が設けられる構造(渦巻き構造)となっている。また、このような複数のI型セル31を用いる場合に、帯状の第2セパレータ32は、渦巻き構造に限定するものではなく、図3に示すように、各I型セル31の端部で折り返すような構造であっても良い。
尚、IIc型セル34とIIa型セル35とを用いた場合に、図4に示すように奇数個積層した場合には、最も外側に位置する2つの電極板40a、40bは同一の極性となる一方、図5に示すように偶数個積層した場合には、最も外側に位置する2つの電極板40a、40bは異なる極性となる。
2:負極板
3:セパレータ
6:アルミニウムラミネート外装体
15:積層型電極体
Claims (8)
- 正極板と、負極板とが、セパレータを介して複数積層された積層型電極体と、
上記積層型電極体が非水電解質と共に収納される外装体と、
を備え、
上記外装体はラミネートフィルムから成ると共に、上記非水電解質中にはLiBOB(リチウムビスオキサレートボラート)及び/又はLiBOBに由来するホウ素含有物質が存在し、且つ、上記各正極板の面積と上記各負極板の面積とが、それぞれ100cm2以上であり、上記積層型電極体における積層方向の厚みが10mm以下であり、
上記正極板と上記セパレータとが貼着され、且つ、上記負極板と上記セパレータとが貼着され、
上記セパレータと上記正極板の間には、無機粒子とバインダーからなる接着層が形成され、上記セパレータと上記正極板の間に形成された無機粒子とバインダーからなる接着層により、上記セパレータと上記正極板は貼着され、
上記セパレータと上記負極板の間には、無機粒子とバインダーからなる接着層が形成され、上記セパレータと上記負極板の間に形成された無機粒子とバインダーからなる接着層により、上記セパレータと上記負極板は貼着され、
上記セパレータと上記正極板の間に形成された接着層に含まれる無機粒子及び上記セパレータと上記負極板の間に形成された接着層に含まれる無機粒子の少なくとも一方は、少なくともその一部がBaTiO 3 である非水電解質二次電池。 - 電池容量が10Ah以上である、請求項1に記載の非水電解質二次電池。
- 上記セパレータは、ポリプロピレン製のセパレータ、ポリエチレン製のセパレータ、又はポリプロピレンーポリエチレンの多層セパレータである請求項1又は2に記載の非水電解質二次電池。
- 上記非水電解質にはLiPF2O2(ジフルオロリン酸リチウム)が添加されている、請求項1〜3の何れか1項に記載の非水電解質二次電池。
- 正極板と、負極板とが、セパレータを介して複数積層された積層型電極体と、
上記積層型電極体が非水電解質と共に収納される外装体と、
を備え、
上記外装体はラミネートフィルムから成ると共に、上記非水電解質にはLiPF2O2が添加され、且つ、上記各正極板の面積と上記各負極板の面積とが、それぞれ100cm2以上であり、しかも、上記積層型電極体における積層方向の厚みが10mm以下であり、
上記正極板と上記セパレータとが貼着され、且つ、上記負極板と上記セパレータとが貼着され、
上記セパレータと上記正極板の間には、無機粒子とバインダーからなる接着層が形成され、上記セパレータと上記正極板の間に形成された無機粒子とバインダーからなる接着層により、上記セパレータと上記正極板は貼着され、
上記セパレータと上記負極板の間には、無機粒子とバインダーからなる接着層が形成され、上記セパレータと上記負極板の間に形成された無機粒子とバインダーからなる接着層により、上記セパレータと上記負極板は貼着され、
上記セパレータと上記正極板の間に形成された接着層に含まれる無機粒子及び上記セパレータと上記負極板の間に形成された接着層に含まれる無機粒子の少なくとも一方は、少なくともその一部がBaTiO 3 である非水電解質二次電池。 - 電池容量が10Ah以上である、請求項5に記載の非水電解質二次電池。
- 上記セパレータは、ポリプロピレン製のセパレータ、ポリエチレン製のセパレータ、又はポリプロピレンーポリエチレンの多層セパレータである請求項5又は6に記載の非水電解質二次電池。
- 上記非水電解質中にはLiBOB及び/又はLiBOBに由来するホウ素含有物質が存在する、請求項5〜7の何れか1項に記載の非水電解質二次電池。
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HUE046573T2 (hu) | 2013-04-04 | 2020-03-30 | Solvay | Nemvizes elektrolit készítmények |
CN109962200A (zh) * | 2019-02-28 | 2019-07-02 | 湖南立方新能源科技有限责任公司 | 一种锂金属二次电池 |
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