JP6341195B2 - 二次電池用電解液およびそれを用いた二次電池 - Google Patents
二次電池用電解液およびそれを用いた二次電池 Download PDFInfo
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- JP6341195B2 JP6341195B2 JP2015503069A JP2015503069A JP6341195B2 JP 6341195 B2 JP6341195 B2 JP 6341195B2 JP 2015503069 A JP2015503069 A JP 2015503069A JP 2015503069 A JP2015503069 A JP 2015503069A JP 6341195 B2 JP6341195 B2 JP 6341195B2
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Images
Classifications
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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
- 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
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
-
- 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
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/381—Alkaline or alkaline earth metals elements
- H01M4/382—Lithium
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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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Description
本実施形態におけるリチウム二次電池用電解液(以下、「非水電解液」または単に「電解液」と記載することもある。)は、添加剤として、一般式(1)で表される環状スルホン酸エステル化合物(以下、単に「一般式(1)の化合物」と記載することもある。)を含有する。
負極は、負極集電体上に、負極活物質と負極用結着剤を含む負極活物質層を形成することで作製することができる。図1の非水電解液二次電池において、負極活物質を含有する層2に用いる負極活物質には、たとえばリチウム金属、リチウム合金、およびリチウムを吸蔵・放出できる材料からなる群から選択される一または二以上の物質を用いることができる。リチウムイオンを吸蔵・放出する材料としては、炭素材料および酸化物等を挙げることができる。
図1の二次電池において、正極活物質を含有する層1に用いる正極活物質としては、例えば、LiCoO2、LiNiO2、LiMn2O4などのリチウム含有複合酸化物があげられる。また、これらのリチウム含有複合酸化物の遷移金属部分を他元素で置き換えたものでもよい。また、金属リチウム対極電位で4.2V以上にプラトーを有するリチウム含有複合酸化物を用いることもできる。リチウム含有複合酸化物としては、スピネル型リチウムマンガン複合酸化物、オリビン型リチウム含有複合酸化物、逆スピネル型リチウム含有複合酸化物等が例示される。リチウム含有複合酸化物は、例えば下記の式(4)で表される化合物を挙げることができる。
(ただし、式(4)において、0<x<2であり、また、0<a<1.2である。また、Mは、Ni、Co、Fe、CrおよびCuよりなる群から選ばれる少なくとも一種である。)
本実施形態の非水電解液を用いた二次電池は、たとえば図1のような構造を有する。正極は、正極活物質を含有する層1が正極集電体3上に成膜されたものであり、負極は、負極活物質を含有する層2が負極集電体4上に成膜されたものである。これらの正極と負極は、多孔質セパレータ5を介して対向配置されている。多孔質セパレータ5は、負極活物質を含有する層2に対して略平行に配置されている。二次電池は、これら正極および負極が対向配置された電極素子と、電解液とが外装体6および7に内包されている。正極集電体3には正極タブ9が接続けられ、負極集電体4には負極タブ8が接続され、これらのタブは容器の外に引き出されている。本実施形態に係る非水電解液二次電池の形状としては、特に制限はないが、例えば、ラミネート外装型、円筒型、角型、コイン型などがあげられる。
(電池の作製)
本実施例の電池の作製について説明する。正極集電体として厚み20μmのアルミニウム箔を用い、正極活物質としてLiMn2O4を用いた。また、負極集電体として厚み10μmの銅箔を用い、この銅箔上に負極活物質として黒鉛を用いた。そして、負極と正極とをポリエチレンからなるセパレータを介して積層し、二次電池を作製した。
非水電解液の溶媒としてECとDECの混合溶媒(体積比:EC/DEC=30/70)を用い、支持電解質としてLiPF6を非水電解液中1Mとなるように溶解した。
まず室温において充電および放電を1回ずつ行った。この時の条件はCCCV充電レート1.0C、CC放電レート1.0C、充電終止電圧4.2V、放電終止電圧3.0Vとした。 その後、各電池をCCCV充電レート1.0C、充電終止電圧4.2Vまで2.5時間、充電し、45℃の恒温槽中で4週間放置した。放置後に室温おいてCC放電レート1.0Cにて放電を行い残存容量とした。結果を表3に示す。
実施例1において化合物No.1の代わりに表2に示す化合物を用いた以外は実施例1と同様に二次電池を作製し、実施例1と同様に電池の特性および電解液の遊離酸量ハーゼン値および濁りの有無を調べた。結果を表2、表3に示す。
実施例1において、化合物No.1の変わりにメチレンメタンジスルホン酸エステル(以下、「化合物A1」)を用いた以外は実施例1と同様に二次電池を作製し、実施例1と同様に電池の特性を測定した。また電解液の遊離酸、ハーゼン値および濁りの有無を調べた。結果を表2、3に示す。
実施例1において、添加剤を加えない以外は実施例1と同様に二次電池を作製し、実施例1と同様に電池の特性を調べた。結果を表2に示す。
実施例1において、黒鉛に代えて非晶質炭素を用い、電解液の主溶媒をPC/EC/DEC(体積比:20/20/60)とした以外は実施例1と同様にして二次電池を作製し、実施例1と同様に電池の特性および電解液の遊離酸量ハーゼン値および濁りの有無を調べた。結果を表4、表5に示す。
実施例5において、化合物No.1に代えて表4に示す化合物を用いた以外は、実施例5と同様にして二次電池を作製し、実施例1と同様に電池の特性および電解液の遊離酸量ハーゼン値および濁りの有無を調べた。
実施例5において、化合物No.1の代わりにメチレンメタンジスルホン酸エステル(以下、「化合物A1」)を用いた以外は実施例5と同様に二次電池を作製し、実施例1と同様に電池の特性および電解液の遊離酸量ハーゼン値および濁りの有無を調べた。
実施例5において、添加剤を加えない他は実施例5と同様に二次電池を作製した。以下、実施例1と同様に電池の特性を調べた。結果を表5に示す。
2 負極活物質層
3 正極集電体
4 負極集電体
5 多孔質セパレータ
6 ラミネート外装体
7 ラミネート外装体
8 負極タブ
9 正極タブ
Claims (19)
- 一般式(1)で表される環状スルホン酸エステルを含み、一般式(A1)で表される化合物を含まないことを特徴とするリチウム二次電池用電解液。
- 少なくとも1個のスルホニル基を有する化合物であって、前記一般式(1)で表される環状スルホン酸エステルとは異なる化合物をさらに含むことを特徴とする請求項1〜3のいずれか1項に記載の電解液。
- 前記一般式(1)で表される環状スルホン酸エステルが、電解液全体の0.005wt%〜10wt%の割合で含まれることを特徴とする請求項1〜5のいずれか1項に記載の電解液。
- ビニレンカーボネートまたはその誘導体をさらに含むことを特徴とする請求項1〜6のいずれか1項に記載の電解液。
- 環状カーボネート類、鎖状カーボネート類、脂肪族カルボン酸エステル類、γ−ラクトン類、環状エーテル類、鎖状エーテル類およびこれらの化合物のフッ素誘導体からなる群より選択される少なくとも1種の非水溶媒を含むことを特徴とする請求項1〜7のいずれか1項に記載の電解液。
- リチウム塩として、LiPF6、LiBF4、LiAsF6、LiSbF6、LiClO4、LiAlCl4、およびLiN(CnF2n+1SO2)(CmF2m+1SO2)(但し、n、mは自然数)からなる群より選択される1種以上の物質を含むことを特徴とする請求項1〜8のいずれか1項に記載の電解液。
- 正極、負極および請求項1〜9のいずれか1項に記載のリチウム二次電池用電解液を含むことを特徴とする二次電池。
- 正極活物質としてリチウム含有複合酸化物を含むことを特徴とする請求項10に記載の二次電池。
- 負極活物質として、リチウムを吸蔵・放出できる材料、リチウム金属、リチウムと合金を形成しうる金属材料および酸化物材料からなる群より選択される少なくとも1種の物質を含むことを特徴とする請求項10または11に記載の二次電池。
- 前記負極活物質として、炭素材料および酸化物から選ばれるリチウムを吸蔵・放出できる材料を含むことを特徴とする請求項12に記載の二次電池。
- 前記炭素材料が黒鉛であることを特徴とする請求項13に記載の二次電池。
- 前記炭素材料が非晶質炭素であることを特徴とする請求項13に記載の二次電池。
- フィルム外装体を有することを特徴とする請求項10〜15のいずれか1項に記載の二次電池。
- 請求項10〜16のいずれか1項に記載の二次電池を含むことを特徴とする自動車用電池。
- 請求項17に記載の自動車用電池を用いたことを特徴とする自動車。
- 非水溶媒中に、一般式(1)で表される環状スルホン酸エステルおよび支持塩を溶解させることを特徴とするリチウム二次電池用電解液の製造方法(但し、前記リチウム二次電池用電解液は一般式(A1)で表される化合物を含まない。)。
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JP5508923B2 (ja) | 2010-04-09 | 2014-06-04 | 日立ビークルエナジー株式会社 | 蓄電モジュール |
CN104919629B (zh) | 2013-01-11 | 2018-02-02 | 日本电气株式会社 | 锂离子二次电池 |
WO2014133163A1 (ja) * | 2013-03-01 | 2014-09-04 | 日本電気株式会社 | 非水電解液二次電池 |
JP6380377B2 (ja) * | 2013-03-01 | 2018-08-29 | 日本電気株式会社 | リチウムイオン二次電池 |
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2014
- 2014-02-28 WO PCT/JP2014/055179 patent/WO2014133169A1/ja active Application Filing
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WO2014133169A1 (ja) | 2014-09-04 |
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