JP2015076389A - 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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- CZXGXYBOQYQXQD-UHFFFAOYSA-N methyl benzenesulfonate Chemical compound COS(=O)(=O)C1=CC=CC=C1 CZXGXYBOQYQXQD-UHFFFAOYSA-N 0.000 description 1
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- 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
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Abstract
【解決手段】正極41および負極42がセパレータ43を介して積層された発電要素4を、外装体5の内部に、非水電解質および添加剤とともに収容し、端子を導出した状態で外装体を密封して、少なくとも初回充電を含む充放電工程を行う。充放電工程後の電解質中,正極,負極それぞれに存在する添加剤成分の各存在量WE,WC,WAの総和量をWTとし、総和量WTに対する各存在量WE,WC,WAの存在比率をそれぞれRE,RC,RAとして、関係式RE<RC<RAを満たすようにする。
【選択図】図2
Description
本発明の一実施形態を下記に述べる。本実施形態の電池は、例えば図1,図2のフィルム外装型の非水電解質二次電池(以下、電池)1が挙げられる。電池1は例えばリチウムイオン二次電池であり、図1に示すように、偏平な長方形の外観形状を有し、長手方向の一方の端縁には一対の端子2,3を備えている。
図1,図2に示すような電池1の電解質としては、特に限定されるものではないが、リチウムイオン二次電池に一般的に使用される電解質として、例えば、エチレンカーボネート、プロピレンカーボネート、ジエチルカーボネート、ジメチルカーボネート、エチルメチルカーボネート、γ−ブチロラクトンといった有機溶媒に、LiPF6,LiBF4といったリチウム塩が溶解した非水電解質を用いることができる。さらに、液状のものに限定されるものではなく、ゲル状電解質等の半固体電解質であっても良い。
添加剤としては、少なくとも初回充電を含む充放電工程の際に負極活物質(図1,図2では負極活物質層42b)により還元分解し表面(活性面)に添加剤由来の被膜を形成できるものであって、充放電工程後に電池1を分解して電解質,正極41,負極42それぞれに含まれる添加剤成分の存在量WE,WC,WAを観測できるものであれば良く、種々のものを適用することができる。
電池1を製造する手順例としては、まず、負極42、セパレータ43および正極41、セパレータ43を順次積層して発電要素4を構成し、負極42の負極集電体42aの延長部40に対し樹脂層33が予め熱融着された負極端子3の内側端(一端部3a)を接合する。同様に、正極41の正極集電体41aの延長部40に対し樹脂層33が予め熱融着された正極端子2の内側端(負極端子3の一端部3aに相当)を接合する。次に、この発電要素4を外装体5となるラミネートフィルムで覆いながら、一辺を残して周囲の3辺(2つ折りの場合は2辺)を熱融着する。そして、熱融着せずに残した1辺を通して外装体5の内部に、少なくとも1種類以上の添加剤を含む電解質を充填し、外装体5内部を減圧し、その後、注液に用いた1辺を熱融着して外装体5を密閉状態とする。これにより電池1が完成する。
充放電工程後の電池1の電解質,正極41,負極42それぞれに存在する添加剤成分の存在量WE,WC,WAは、例えば以下に示す方法で観測することが可能である。
正極活物質層の平均活物質比表面積ScAVEは、n種類の活物質粒子の材料種類ごとの比表面積Scn(Sc1,Sc2,Sc3,……,Scn-1,Scn)(単位:m2/g)と、それらの重量比率Pcn(Pc1,Pc2,Pc3,……,Pcn-1,Pcn)(全合計=1)を用いて、以下に示す通りとなる。
同様に、負極活物質層の平均活物質比表面積SaAVEは、San、Pcnに対して、
SaAVE=(Sa1×Pa1)+(Sa2×Pa2)+(Sa3×Pa3)+……+(San-1×Pan-1)+(San×Pan) (単位:m2/g)
一方、単位面積あたりの正極集電体の上に形成されている正極活物質層(以下単位面積正極活物質層)に含まれる、n種類の活物質粒子の材料種類ごとの重量をMcn(単位:g/m2)と置くと、単位面積正極活物質層の中の細孔を形成する全活物質粒子の表面積の総合計Acが以下のように計算できる。
同様に、負極に対しては、
Aa=(Sa1×Ma1)+(Sa2×Ma2)+(Sa3×Ma3)+……+(San-1×Man-1)+(San×Man) (単位:m2/m2)
これらの比を取ったAc/Aaは、活物質粒子で形成される細孔の表面積の、正極側と負極側の比を表す(以下、活物質表面積比率とも称する)。
正極41の正極活物質層41b,41c等の空孔率や負極42の負極活物質層42b,42c等の空孔率においては、単位面積あたりの集電体の上の活物質層に含まれるそれぞれの構成粒子やバインダーの重量に、それぞれの成分の真密度の逆数を掛け、その値を、単位面積あたりの集電体の上の活物質層の体積で割り算し、その値を1から引き算することで求めることが出来る。
関係式Rに係る存在比率RE,RC,RAは、添加剤を種々の添加量Qで用いて構成した電池1を用意し、各電池1において充放電工程後の電解質,正極41,負極42に存在する各添加剤成分の存在量WE,WC,WAをそれぞれ観測し、WE,WC,WAの総量(合計)WTを求めてから下記式によりそれぞれ導き出すことができる。
RC=(WC/WT)×100
RA=(WA/WT)×100
したがって、RE,RC,RAが関係式Rを満たす電池1であれば、存在量WE<存在量WCの関係および存在量WC<存在量WAの関係が保持されることになり、後述するように良好な諸特性(電気的特性,寿命特性等)が得られることになる。
正極として、スピネル型リチウムマンガン複合酸化物とリチウムニッケル系複合酸化物からなる活物質混合体に炭素系導電助剤を3%添加したものを用い、負極として、炭素系負極を用い、これらをポリオレフィン系微多孔性膜からなるセパレータを介して対向させてなる電極体に、添加剤として環状ジスルホン酸エステルを用いた非水系電解液を含浸させて分析用の電池を作製した。用いた外装体や製法は、前述した通りである。正極の活物質混合体の平均活物質比表面積ScAVEは、0.53m2/gであった。活物質表面積比率Ac/Aaは1.44、空孔比率(正/負)は0.76であった。
図3〜図5で用いた電池1において、活物質表面積比率Ac/Aa(正極/負極)を種々設定して添加量Qに対する放電容量維持率の変化特性を調べたところ、表2に示すような結果が得られた。
2,3…端子
4…発電要素
41…正極
42…負極
43…セパレータ
5…外装体
Claims (5)
- 正極および負極がセパレータを介して積層された発電要素を、外装体の内部に、非水電解質および添加剤とともに収容し、端子を導出した状態で外装体を密封して、少なくとも初回充電を含む充放電工程が行われた電池であって、
充放電工程後の電解質中,正極,負極それぞれに存在する添加剤成分の各存在量WE,WC,WAの総和量をWTとし、総和量WTに対する各存在量WE,WC,WAの存在比率をそれぞれRE,RC,RAとして、関係式RE<RC<RAを満たすことを特徴とする非水電解質二次電池。 - 負極に形成される負極活物質層の表面積に対する、正極に形成される正極活物質層の表面積の比率が、1 .8 以下であることを特徴とする請求項1記載の非水電解質二次電池。
- 正極活物質層の平均比表面積が0.60m2/g以下であることを特徴とする請求項1記載の非水電解質二次電池。
- 正極活物質層に含まれる導電助剤が3重量%以下であることを特徴とする請求項1〜3の何れかに記載の非水電解質二次電池。
- 正極活物質層の空孔率が負極活物質層の空孔率よりも小さいことを特徴とする請求項1〜4の何れかに記載の非水電解質二次電池。
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