JP5765835B2 - 新規なポリマー電解質及びそれを含むリチウム二次電池 - Google Patents
新規なポリマー電解質及びそれを含むリチウム二次電池 Download PDFInfo
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- JP5765835B2 JP5765835B2 JP2014516906A JP2014516906A JP5765835B2 JP 5765835 B2 JP5765835 B2 JP 5765835B2 JP 2014516906 A JP2014516906 A JP 2014516906A JP 2014516906 A JP2014516906 A JP 2014516906A JP 5765835 B2 JP5765835 B2 JP 5765835B2
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- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical group FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 description 1
- TXEYQDLBPFQVAA-UHFFFAOYSA-N tetrafluoromethane Chemical compound FC(F)(F)F TXEYQDLBPFQVAA-UHFFFAOYSA-N 0.000 description 1
- 239000006234 thermal black Substances 0.000 description 1
- 238000009281 ultraviolet germicidal irradiation Methods 0.000 description 1
- 229960000834 vinyl ether Drugs 0.000 description 1
- 238000009736 wetting Methods 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
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Description
である)で表現されるリチウムニッケル系酸化物;Li1+zNi1/3Co1/3Mn1/3O2、Li1+zNi0.4Mn0.4Co0.2O2などのように、Li1+zNibMncCo1−(b+c+d)MdO(2−e)Ae(ここで、
、b+c+d<1である、M=Al、Mg、Cr、Ti、SiまたはYであり、A=F、PまたはClである)で表現されるリチウムニッケルコバルトマンガン複合酸化物;化学式Li1+xM1−yM’yPO4−zXz(ここで、M=遷移金属、好ましくは、Fe、Mn、CoまたはNiであり、M’=Al、MgまたはTiであり、X=F、SまたはNであり、
である)で表現されるオリビン系リチウム金属ホスフェートなどが挙げられるが、これらに限定されるものではない。
2Al2O3の急激な発熱反応によることがわかった。実際に電池が爆発した全ての場合において、Al−foilはその形態を見つけることができなかった。
(1)線状高分子、架橋高分子用単量体、イオン性塩を含む有機電解液、選択的に固相成分及び重合開始剤を均一に混合する過程と;
(2)第1高分子層を構成する混合物を一つの電極上にコーティングし、前記第1高分子層上に第2高分子層を構成する混合物をコーティングする過程と;
(3)UV照射または熱の印加によって重合反応を行って分離層を形成する過程と;
(4)前記分離層上に対応電極を搭載し、加圧する過程と;
を含んでいる。
第1高分子層混合物の製造
PVdF−HFP 5%及び有機電解液(1M LiPF6、EC/PC=1/1)を70:30の重量比で混合し、ポリマーを溶解する溶媒としてアセトンを使用して、機械的剛性を提供する第1高分子層の混合物を製造した。
PVdF−HFP 5%及び有機電解液(1M LiPF6、EC/PC=1/1)を22:78の重量比で混合し、ポリマーを溶解する溶媒としてアセトンを使用して、イオン伝導性を提供する第2高分子層の混合物を製造した。
用意した第1高分子層の混合物をガラス板にキャスティングしてアセトンを蒸発させることによって、電解質膜を製造した後、用意した第2高分子層の混合物を第1高分子層にキャスティングし、アセトンを蒸発させて、第1高分子層及び第2高分子層で構成されたポリマー電解質膜を製造した。
前記実施例1の第1高分子層の混合物をガラス板にキャスティングして、アセトンを蒸発させることによって、電解質膜を製造した。
前記実施例1の第2高分子層の混合物をガラス板にキャスティングして、アセトンを蒸発させることによって、電解質膜を製造した。
機械的物性及びイオン伝導性の測定
実施例1及び比較例1乃至比較例2の引張強度及びイオン伝導度を測定し、その結果を表1に示した。
LiCoO2、PVdF、カーボンブラックをN−メチルピロリドンに添加してスラリーにした後、銅ホイルに塗布し、約130℃で、2時間の間乾燥して、正極を製造した。前記正極に実施例1の第1高分子層をコーティングした後、第2高分子層をコーティングして、多層のポリマー電解質層を形成した。用意したポリマー電解質がコーティングされた正極と、相手極としてはLi金属を用いて、半分の電池を製造した。
実施例2の正極とセパレーター、相手極としてLi金属、有機電解液(1M
LiPF6、EC/PC=1/1)を用いて、半分の電池を製造した。
電池性能実験
実施例2及び比較例3から製造された電池を用いて、充放電特性を評価した。充電時には、0.1Cの電流密度で4.25Vまで定電流充電した後、4.25Vの定電圧で一定に維持させて、電流密度が0.05Cとなると、充電を終了した。放電時には、0.1Cの電流密度で3.0Vまで定電流モードで放電を完了した。同様の条件で、充放電を15回繰り返した。これに対する結果を図2及び図3に示した。
Claims (22)
- 外力に対して機械的剛性を提供する第1高分子層と、リチウムイオンの伝導経路を確保する第2高分子層との多層構造からなり、前記第1高分子層は、イオン性塩を含んでいる有機電解液を第1高分子層のポリマーマトリックスの重量対比0〜60重量%含有し、前記第2高分子層は、イオン性塩を含んでいる有機電解液を第2高分子層のポリマーマトリックスの重量対比60〜400重量%含有しており、
前記第1高分子層及び第2高分子層はそれぞれ、
イオン性塩を含み、電極組立体の作製過程で前記第1高分子層及び第2高分子層から電極に一部流入して電極のイオン伝導度を向上させる有機電解液と、
前記有機電解液に対して親和性を有し、正極と負極に対する結着力を提供する線状高分子及び三次元的ネットワーク構造を有する架橋高分子からなる前記ポリマーマトリックスと、
を含む2相(two−phase)からなり、
前記第1高分子層は、第2高分子層の厚さ対比10%〜100%である、
ことを特徴とする、ポリマー電解質。 - 正極または負極のいずれか一つの電極に接する第2高分子層の上面または下面には、第1高分子層が積層されていることを特徴とする、請求項1に記載のポリマー電解質。
- 正極または負極のいずれか一つの電極に接する第1高分子層の上面または下面には、第2高分子層が積層されていることを特徴とする、請求項1に記載のポリマー電解質。
- 前記イオン性塩は、リチウム塩であることを特徴とする、請求項1に記載のポリマー電解質。
- 前記ポリマー電解質は、引張強度が1MPa〜100MPaであることを特徴とする、請求項1に記載のポリマー電解質。
- 前記ポリマー電解質は、伸び率が20%〜500%であることを特徴とする、請求項1に記載のポリマー電解質。
- 前記第1高分子層は、イオン性塩を含んでいる有機電解液を、第1高分子層のポリマーマトリックスの重量対比0.1〜60重量%含有していることを特徴とする、請求項1に記載のポリマー電解質。
- 前記ポリマー電解質は、イオン伝導性が10−5S/cm〜10−3S/cmであることを特徴とする、請求項1に記載のポリマー電解質。
- 前記線状高分子と架橋高分子との比率は、重量比で1:9〜8:2であることを特徴とする、請求項1に記載のポリマー電解質。
- 前記線状高分子は、ポリオキサイド系の非架橋高分子及び極性非架橋高分子からなる群から選択される一つ以上であることを特徴とする、請求項1に記載のポリマー電解質。
- 前記ポリマーマトリックスは、ポリオキサイド系の非架橋高分子及び極性非架橋高分子を含んでいることを特徴とする、請求項1に記載のポリマー電解質。
- 前記架橋高分子は、2個以上の官能基を有する単量体の重合体、または2個以上の官能基を有する単量体と1個の官能基を有する極性単量体との共重合体であることを特徴とする、請求項1に記載のポリマー電解質。
- 前記第1高分子層及び第2高分子層は、機械的剛性を提供する固相成分をさらに含むことを特徴とする、請求項1に記載のポリマー電解質。
- 前記固相成分は、ポリマーマトリックスの重量を基準に5〜80重量%含まれていることを特徴とする、請求項13に記載のポリマー電解質。
- 前記固相成分は、リチウムイオンと反応性のない固体化合物であって、10nm〜5μmの平均粒径を有する固相粒子であることを特徴とする、請求項13に記載のポリマー電解質。
- 前記固体化合物は、リチウムイオンと反応性のない酸化物、窒化物及び炭化物からなる群から選択される一つ以上であることを特徴とする、請求項15に記載のポリマー電解質。
- 請求項1に係るポリマー電解質が正極と負極との間に位置する構造を有することを特徴とする、電極組立体。
- 請求項17に係わる電極組立体を含むことを特徴とする、リチウム二次電池。
- 請求項18に係るリチウム二次電池を単位電池として含むことを特徴とする、電池モジュール。
- 請求項19に係る電池モジュールを含むことを特徴とする、電池パック。
- 前記電池パックは、中大型デバイスの電源として使用されることを特徴とする、請求項20に記載の電池パック。
- 前記中大型デバイスは、電気自動車、ハイブリッド電気自動車、プラグ−インハイブリッド電気自動車、または電力貯蔵用システムであることを特徴とする、請求項21に記載の電池パック。
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US9391344B2 (en) | 2016-07-12 |
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