JP6400888B2 - 蓄電素子 - Google Patents
蓄電素子 Download PDFInfo
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- JP6400888B2 JP6400888B2 JP2013128945A JP2013128945A JP6400888B2 JP 6400888 B2 JP6400888 B2 JP 6400888B2 JP 2013128945 A JP2013128945 A JP 2013128945A JP 2013128945 A JP2013128945 A JP 2013128945A JP 6400888 B2 JP6400888 B2 JP 6400888B2
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- positive electrode
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- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 description 1
- 239000010445 mica Substances 0.000 description 1
- 229910052618 mica group Inorganic materials 0.000 description 1
- 239000011707 mineral Substances 0.000 description 1
- 239000012046 mixed solvent Substances 0.000 description 1
- 229910052901 montmorillonite Inorganic materials 0.000 description 1
- 229910052863 mullite Inorganic materials 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- 229910021470 non-graphitizable carbon Inorganic materials 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 239000010450 olivine Substances 0.000 description 1
- 229910052609 olivine Inorganic materials 0.000 description 1
- 239000011146 organic particle Substances 0.000 description 1
- 239000000123 paper Substances 0.000 description 1
- 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
- 150000003014 phosphoric acid esters Chemical class 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 229920003229 poly(methyl methacrylate) Polymers 0.000 description 1
- 229920002627 poly(phosphazenes) Polymers 0.000 description 1
- 229920001197 polyacetylene Polymers 0.000 description 1
- 239000004584 polyacrylic acid Substances 0.000 description 1
- 229920000767 polyaniline Polymers 0.000 description 1
- 229920000515 polycarbonate Polymers 0.000 description 1
- 239000004417 polycarbonate Substances 0.000 description 1
- 239000005518 polymer electrolyte Substances 0.000 description 1
- 239000004926 polymethyl methacrylate Substances 0.000 description 1
- 229920005672 polyolefin resin Polymers 0.000 description 1
- 229920001451 polypropylene glycol Polymers 0.000 description 1
- 229920000128 polypyrrole Polymers 0.000 description 1
- 229920001282 polysaccharide Polymers 0.000 description 1
- 239000005017 polysaccharide Substances 0.000 description 1
- 229920001296 polysiloxane Polymers 0.000 description 1
- 229920002223 polystyrene Polymers 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- ZNNZYHKDIALBAK-UHFFFAOYSA-M potassium thiocyanate Chemical compound [K+].[S-]C#N ZNNZYHKDIALBAK-UHFFFAOYSA-M 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 230000002265 prevention Effects 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- KUKFKAPJCRZILJ-UHFFFAOYSA-N prop-2-enenitrile;prop-2-enoic acid Chemical compound C=CC#N.OC(=O)C=C KUKFKAPJCRZILJ-UHFFFAOYSA-N 0.000 description 1
- YKYONYBAUNKHLG-UHFFFAOYSA-N propyl acetate Chemical group CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 description 1
- 229940116423 propylene glycol diacetate Drugs 0.000 description 1
- 230000001681 protective effect Effects 0.000 description 1
- 229940071139 pyrrolidone carboxylate Drugs 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 239000005060 rubber Substances 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- SUKJFIGYRHOWBL-UHFFFAOYSA-N sodium hypochlorite Chemical compound [Na+].Cl[O-] SUKJFIGYRHOWBL-UHFFFAOYSA-N 0.000 description 1
- FVAUCKIRQBBSSJ-UHFFFAOYSA-M sodium iodide Chemical compound [Na+].[I-] FVAUCKIRQBBSSJ-UHFFFAOYSA-M 0.000 description 1
- VGTPCRGMBIAPIM-UHFFFAOYSA-M sodium thiocyanate Chemical compound [Na+].[S-]C#N VGTPCRGMBIAPIM-UHFFFAOYSA-M 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 241000894007 species Species 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
- 238000004381 surface treatment Methods 0.000 description 1
- 239000004094 surface-active agent Substances 0.000 description 1
- 239000000454 talc Substances 0.000 description 1
- 229910052623 talc Inorganic materials 0.000 description 1
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- LGQXXHMEBUOXRP-UHFFFAOYSA-N tributyl borate Chemical compound CCCCOB(OCCCC)OCCCC LGQXXHMEBUOXRP-UHFFFAOYSA-N 0.000 description 1
- AJSTXXYNEIHPMD-UHFFFAOYSA-N triethyl borate Chemical compound CCOB(OCC)OCC AJSTXXYNEIHPMD-UHFFFAOYSA-N 0.000 description 1
- DQWPFSLDHJDLRL-UHFFFAOYSA-N triethyl phosphate Chemical compound CCOP(=O)(OCC)OCC DQWPFSLDHJDLRL-UHFFFAOYSA-N 0.000 description 1
- WVLBCYQITXONBZ-UHFFFAOYSA-N trimethyl phosphate Chemical compound COP(=O)(OC)OC WVLBCYQITXONBZ-UHFFFAOYSA-N 0.000 description 1
- 238000001291 vacuum drying Methods 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
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Description
エステル結合されてなる結着剤は、正極活物質との反応性が高いため、エステル結合されてなる結着剤を有するセパレーターを備えた蓄電素子において、本発明の効果がより顕著になる。
図1〜図7を参照して、本発明の一実施の形態である蓄電素子の一例である非水電解質二次電池1を説明する。
有機溶媒としては、例えば、エチレンカーボネート、プロピレンカーボネート、ブチレンカーボネート、トリフルオロプロピレンカーボネート、γ−ブチロラクトン、γ−バレロラクトン、スルホラン、1,2−ジメトキシエタン、1,2−ジエトキシエタン、テトラヒドロフラン、2−メチルテトラヒドロフラン、2−メチル−1,3−ジオキソラン、ジオキソラン、フルオロエチルメチルエーテル、エチレングリコールジアセテート、プロピレングリコールジアセテート、エチレングリコールジプロピオネート、プロピレングリコールジプロピオネート、酢酸メチル、酢酸エチル、酢酸プロピル、酢酸ブチル、プロピオン酸メチル、プロピオン酸エチル、プロピオン酸プロピル、ジメチルカーボネート、ジエチルカーボネート、エチルメチルカーボネート、メチルプロピルカーボネート、エチルプロピルカーボネート、ジプロピルカーボネート、メチルイソプロピルカーボネート、エチルイソプロピルカーボネート、ジイソプロピルカーボネート、ジブチルカーボネート、アセトニトリル、フルオロアセトニトリル、エトキシペンタフルオロシクロトリホスファゼン、ジエトキシテトラフルオロシクロトリホスファゼン、フェノキシペンタフルオロシクロトリホスファゼンなどのアルコキシ及びハロゲン置換環状ホスファゼン類または鎖状ホスファゼン類、リン酸トリエチル、リン酸トリメチル、リン酸トリオクチルなどのリン酸エステル類、ホウ酸トリエチル、ホウ酸トリブチルなどのホウ酸エステル類、N−メチルオキサゾリジノン、N−エチルオキサゾリジノン等の非水溶媒が挙げられる。
電解質として固体電解質を用いる場合は、固体電解質としての高分子固体電解質を用い、高分子固体電解質として有孔性高分子固体電解質膜を用いることができる。そして、高分子固体電解質にさらに電解液を含有させることができる。また、電解質としてのゲル状の高分子固体電解質を用いる場合には、ゲルを構成する電解液と、細孔中等に含有されている電解液とは異なっていてもよい。但し、HEV用途のように高い出力が要求される場合は、固体電解質や高分子固体電解質を用いるよりも非水電解質を単独で用いるほうがより好ましい。
電解質塩としては、特に制限はなく、LiClO4、LiBF4、LiAsF6、LiPF6、LiCF3SO3、LiN(SO2CF3)2、LiN(SO2C2F5)2、LiN(SO2CF3)(SO2C4F9)、LiSCN、LiBr、LiI、Li2SO4、Li2B10Cl10、NaClO4、NaI、NaSCN、NaBr、KClO4、KSCN等のイオン性化合物及びそれらの2種類以上の混合物などが挙げられる。
非水電解質には、さらに、公知の添加剤を加えることもできる。
蓄電素子10においては、上記の有機溶媒と電解質塩とを組み合わせてなる非水電解質を使用できる。なお、非水電解質としては、プロピレンカーボネート、ジメチルカーボネート、メチルエチルカーボネートを混合したものが、リチウムイオンの伝導度が高くなるという点で好ましい。
なお、負極基材13Aの両面側に負極活物質層が形成されていてもよく、正極基材11Aの両面側に正極活物質層が形成されていてもよい。
正極活物質においては、これらの化合物が単独で用いられてもよく、2種以上が混合されて用いられてもよい。
また、無機粒子と混合する結着剤としては、無機粒子を正極基材11Aや負極基材13Aに結着でき、電解液に溶解せず、且つリチウムイオン二次電池の使用範囲で電気化学的に安定であるものが好ましい。
結着剤としては、ポリフッ化ビニリデン(PVdF);ポリテトラフルオロエチレンなどのフッ素含有樹脂;スチレンブタジエンゴム(SBR);アクリル樹脂(分子中にエステル結合を有する);ポリオレフィン樹脂;ポリビニルアルコール;ポリアミド、ポリイミド、ポリアミドイミドなどの窒素含有樹脂;セルロースとアクリルアミドの架橋重合体とセルロースとキトサンピロリドンカルボン酸塩の架橋重合体;及び、多糖類高分子ポリマーであるキトサン、キチン等を架橋剤で架橋したものからなる群より選択される少なくとも1種が好ましい。
保護層11Cの構成材料としては、安全性や安定性,取り扱いの容易さ等から、Al2O3粒子が好ましく、箔状正極板との密着性や接合強度等の観点から、γ型アルミナ粒子が特に好ましい。なお、保護層11Cは、正極活物質を含まない。
保護層11Cにおける上記粒子としては、一次粒径の中央値が1nm〜2000nmのものが使用できる。上記粒子としては、箔状正極板と密着性や接合強度の観点から、一次粒径の中央値が1nm〜200nmのものが好ましく、1nm〜20nmのものがより好ましい。
電気的絶縁性の上記粒子と混合するバインダーとしては、ポリフッ化ビリニデン(PVDF)、ポリイミド、ポリアミドイミド等を用いることができるが、箔状正極基材11Aとの密着性や接合強度の観点からは、PVDFを用いることが好ましい。
保護層11Cの厚みが正極活物質層11Bの厚みに対して+2μm以下であることにより、巻回時に保護層11C付近での正極及び負極の極間距離が他の部分と比較して大きくなることが抑制される。従って、極間距離が広い部分が生じることが抑制されていることから、高効率充放電時に電流分布が乱れることが抑制され、不均一な劣化を引き起こすことが抑制され得る。
保護層11Cの厚みが正極活物質層11Bの厚みに対して−14μm以上であることにより、正極活物質層11Bの側面での保護作用をより十分なものにできる。
まず、発電要素10について説明する。
正極活物質と、導電助剤と、結着剤とが混合され、この混合物が溶剤に加えられて混練りされて、正極合剤が形成される。この正極合剤が正極基材11Aの少なくとも一方面に塗布され、圧縮成形される。これにより、正極基材11A上に正極活物質層11Bが形成される準備をする。
ハードカーボンを含む負極活物質と、結着剤とが混合され、この混合物が溶剤に加えられて混練りされて、負極合剤が形成される。この負極合剤が負極基材13Aの少なくとも一方面に塗布され、乾燥後、圧縮成形される。これにより、負極基材13A上に負極活物質層13Bが形成された負極13が作製される。
セパレーター12は、セパレーター基材12Aが作製されると共に、セパレーター基材12A上にコート剤が形成されることにより無機層12Bが作製される。
次に、正極11と負極13とをセパレーター12を介して巻回される。具体的には、負極活物質層13Bとセパレーター基材12Aとが向かい合うように、負極13上にセパレーター12が配置され、無機層12Bと正極活物質層11Bとが向かい合うように、セパレーター12上に正極11が配置され、かつ、正極基材11A側から見て正極活物質層11Bを無機層12Bに投影したときに、幅方向の両側に無機層12Bが露出されるように配置される。この状態で巻回されることにより、発電要素10が作製される。その後、正極及び負極の各々に、集電部が取り付けられる。
次に、発電要素10が容器2の本体部2aの内部に配置される。発電要素10が複数の場合には、例えば、発電要素10の集電部を電気的に並列に接続して本体部2aの内部に配置される。次いで、集電部は、蓋部2bの外部ガスケット5内の外部端子21にそれぞれ溶着され、蓋部2bは本体部2aに取り付けられる。
図8及び図9に示すように、変形例1の非水電解質二次電池において、保護層11Cは、正極活物質層11Bの幅方向の両側面11B1全体に沿って延びる。変形例1の場合、保護層11Cの塗布量を低減できる。
図10〜図12に示すように、変形例2の非水電解質二次電池において、保護層11Cの断面形状は、略Z字状である。具体的には、保護層11Cは、正極活物質層11Bの幅方向の両側面11B1に沿って延びるとともに、一端は、正極活物質層11Bにおいて無機層12Bと対向する面に沿って内方に延び、他端は、正極基材11Aにおいて正極活物質層11Bと対向する面に沿って外方に延びている。
図13及び図14に示すように、変形例3の非水電解質二次電池において、保護層11Cの断面形状は、正極活物質層11Bの幅方向の両側面11B1に沿って延びるとともに、一端は、正極活物質層11Bにおいて無機層12Bと対向する面に沿って内方に延びている。変形例3の場合も保護層11Cを容易に形成できる。
本発明の実施の形態2の非水電解質二次電池について、図15及び図16を参照して説明する。実施の形態2の非水電解質二次電池は、基本的には実施の形態1の非水電解質二次電池1と同様の構成を備えているが、正極基材11A側から見て正極活物質層11Bを無機層12Bに投影したときに、幅方向の一方側のみに無機層12Bが露出し、保護層11Cは、露出した無機層12B側に位置する正極活物質層11Bの幅方向の側面11B1のみを覆う点において異なる。
Claims (3)
- 正極と、負極と、前記正極と前記負極との間に配置されたセパレーターとが巻回された巻回型の発電要素を備え、
前記正極は、正極基材と、前記正極基材上に形成された正極活物質層と、前記正極活物質層の幅方向の側面の少なくとも一方を覆う保護層とを有し、
前記負極は、負極基材と、前記負極基材上に形成された負極活物質層とを有し、
前記セパレーターは、樹脂多孔膜で構成されかつ前記負極活物質層と対向するセパレーター基材と、前記セパレーター基材上に形成されると共に前記正極活物質層と対向しかつ結着剤を含む無機層と、を有し、
前記結着剤は、分子中にエステル結合を有する化合物であり、
前記無機層の幅は、前記正極活物質層の幅よりも大きく、
前記保護層は、前記結着剤から溶出した成分から前記正極活物質層が保護されるように構成され、
前記正極基材側から見て前記正極活物質層を前記無機層に投影したときに、幅方向の両側に前記無機層が露出し、
前記保護層は、前記正極活物質層の幅方向の両側の側面を覆う、蓄電素子。 - 正極と、負極と、前記正極と前記負極との間に配置されたセパレーターとが巻回された巻回型の発電要素を備え、
前記正極は、正極基材と、前記正極基材上に形成された正極活物質層と、前記正極活物質層の幅方向の側面の少なくとも一方を覆う保護層とを有し、
前記負極は、負極基材と、前記負極基材上に形成された負極活物質層とを有し、
前記セパレーターは、樹脂多孔膜で構成されかつ前記負極活物質層と対向するセパレーター基材と、前記セパレーター基材上に形成されると共に前記正極活物質層と対向しかつ結着剤を含む無機層と、を有し、
前記結着剤は、分子中にエステル結合を有する化合物であり、
前記無機層の幅は、前記正極活物質層の幅よりも大きく、
前記保護層は、前記結着剤から溶出した成分から前記正極活物質層が保護されるように構成され、
前記正極基材側から見て前記正極活物質層を前記無機層に投影したときに、幅方向の一方側のみに前記無機層が露出し、
前記保護層は、前記露出した無機層側に位置する前記正極活物質層の幅方向の側面のみを覆う、蓄電素子。 - 前記保護層は、前記正極活物質層の幅方向の側面の少なくとも一方を覆いかつ前記正極活物質層の表面の中央部を覆わない、請求項1又は2に記載の蓄電素子。
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