JPWO2018180017A1 - 電池用電極及びリチウムイオン二次電池 - Google Patents
電池用電極及びリチウムイオン二次電池 Download PDFInfo
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- JPWO2018180017A1 JPWO2018180017A1 JP2019508770A JP2019508770A JPWO2018180017A1 JP WO2018180017 A1 JPWO2018180017 A1 JP WO2018180017A1 JP 2019508770 A JP2019508770 A JP 2019508770A JP 2019508770 A JP2019508770 A JP 2019508770A JP WO2018180017 A1 JPWO2018180017 A1 JP WO2018180017A1
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- battery
- porous film
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- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical group O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 34
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- 229910052744 lithium Inorganic materials 0.000 claims description 14
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Abstract
Description
集電体と、該集電体上の活物質層と、該活物質層上の絶縁性多孔質膜を含み、該絶縁性多孔質膜が無機酸化物の粒子と吸着剤の粒子を含む、電池用電極が提供される。
本発明の実施形態による電池用電極は、集電体上の活物質層の表面に絶縁性多孔質膜を有する。
本実施形態における吸着剤としては、ゼオライトが好ましい。
本実施形態における無機酸化物としては、アルミナ、チタニア、ジルコニア、シリカを挙げることがきる。これらは単独で使用してもよく、2種以上を混合して使用してもよい。これらの中でもアルミナが好ましい。無機酸化物の2種以上を混合して使用する場合は少なくともアルミナを含むことが好ましい。アルミナとしては、αアルミナを好適に用いることができる。アルミナは、耐熱性が高く、特にαアルミナは塩基性サイトを有するため、酸性基を有する結着剤を用いた際、結合力が強くなるメリットがある。
図1に、リチウムイオン二次電池の基本構成(一つの電極対を含む構成)の一例を模式的に示す。
負極は、集電体と、この集電体上に形成された負極活物質層を含む構造を有することが好ましい。この負極活物質層は、負極活物質と結着剤を含み、導電性を高める点から導電助剤を含むことが好ましい。
正極活物質としては、特に制限されるものではないが、例えば、層状岩塩型構造又はスピネル型構造を有するリチウム複合酸化物や、オリビン型構造を有するリン酸鉄リチウムなどを用いることができる。リチウム複合酸化物としては、マンガン酸リチウム(LiMn2O4);コバルト酸リチウム(LiCoO2);ニッケル酸リチウム(LiNiO2);これらのリチウム化合物のマンガン、コバルト、ニッケルの部分の少なくとも一部をアルミニウム、マグネシウム、チタン、亜鉛など他の金属元素で置換したもの;マンガン酸リチウムのマンガンの一部を少なくともニッケルで置換したニッケル置換マンガン酸リチウム;ニッケル酸リチウムのニッケルの一部を少なくともコバルトで置換したコバルト置換ニッケル酸リチウム;ニッケル置換マンガン酸リチウムのマンガンの一部を他の金属(例えばアルミニウム、マグネシウム、チタン、亜鉛の少なくとも一種)で置換したもの;コバルト置換ニッケル酸リチウムのニッケルの一部を他の金属元素(例えばアルミニウム、マグネシウム、チタン、亜鉛、マンガンの少なくとも一種)で置換したものが挙げられる。これらのリチウム複合酸化物は一種を単独で使用してもよいし、二種以上を混合して用いてもよい。
Li1+a(NibCocMe1dMe21−b−c−d)O2
(式中、Me1はMn又はAlであり、Me2は、Mn、Al、Mg、Fe、Cr、Ti、Inからなる群から選択される少なくとも1種であり(Me1と同種の金属を除く)、−0.5≦a<0.1、0.1≦b<1、0<c<0.5、0<d<0.5)
電解液としては、1種又は2種以上の非水溶媒に、リチウム塩を溶解させた非水系電解液を用いることができる。
電解液は、非水電解液用添加剤として通常使用されている化合物を含むことが好ましい。例えば、ビニレンカーボネート、フルオロエチレンカーボネート等のカーボネート系化合物;マレイン酸無水物等の酸無水物;ボロン酸エステル等のホウ素系添加剤;エチレンサルファイト等のサルファイト系化合物;1,3−プロパンスルトン、1,2−プロパンスルトン、1,4−ブタンスルトン、1,2−ブタンスルトン、1,3−ブタンスルトン、2,4−ブタンスルトン、1,3−ペンタンスルトン等の環状モノスルホン酸エステル;メチレンメタンジスルホン酸エステル(1,5,2,4−ジオキサジチアン−2,2,4,4−テトラオキシド)、エチレンメタンジスルホン酸エステル等の環状ジスルホン酸エステル化合物が挙げられる。これらの添加剤は、1種を単独で用いてもよいし、2種以上を併用してもよい。特に、正極表面に被膜をより効果的に形成でき、電池特性を向上できる点から、環状スルホン酸エステル化合物が好ましく、環状ジスルホン酸化合物が好ましい。
セパレータとしては、多孔質膜、織布、不織布等を用いることができる。セパレータの厚みは、数十μmが好適であり、8〜40μmが好ましく、8〜30μmがより好ましく、10〜30μmがさらに好ましい。
外装容器には可撓性フィルムからなるケースや、缶ケース等を用いることができ、電池の軽量化の観点からは可撓性フィルムを用いることが好ましい。
本実施形態によるリチウムイオン二次電池は、例えば、以下のプロセスに従って製造することができる。
正極活物質粒子として、平均粒子径8.0μm、BET比表面積0.72m2/gの層状結晶構造を有するニッケル複合酸化物(LiNi0.47Co0.24Mn0.29O2)を準備した。
絶縁性多孔質膜の厚みを、実施例1の絶縁性多孔質膜の厚みに対する比として、表1に示す値(膜厚比)に変更した以外は実施例1と同様にして、実施例2〜4、参考例1、比較例1の正極シート(正極)をそれぞれ作製した。
負極活物質として天然黒鉛を、バインダーであるPVDFを溶解させたNMP中に分散させ、スラリーを得た。このスラリー中の固形分の配合比は、天然黒鉛:PVDF=90:10(質量比)とした。このスラリーを、負極集電体となる銅箔(厚さ8μm)上に塗布し、NMPを蒸発させて負極活物質層を形成し、負極シート(負極)を得た。負極活物質層は集電体の両面に形成した。
作製したラミネート型二次電池を用いて、次のようにして高温サイクル特性を評価した。
温度45℃において、充電レート1.0C、放電レート1.0C、充電終止電圧4.2V、放電終止電圧2.5Vとし、充放電サイクル試験を行った。
表1に得られた容量維持率および放電容量をまとめて示す。
容量維持率(%)は500サイクル後の放電容量(mAh)を、10サイクル目の放電容量(mAh)で割った値である。表中の放電容量(mAh/g)は、1サイクル目のラミネート型二次電池の容量(Ah)を、正極活物質の質量(g)で割った値である。
2 負極活物質層
3 正極集電体
4 負極集電体
5 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
201 正極
202 正極活物質の塗布部
203 正極タブ
204 境界部
206 負極
207 負極活物質の塗布部
208 負極タブ
211 正極端子
216 負極端子
220 セパレータ
230 外装ケース(可撓性フィルム)
Claims (13)
- 集電体と、該集電体上の活物質層と、該活物質層上の絶縁性多孔質膜を含み、該絶縁性多孔質膜が無機酸化物の粒子と吸着剤の粒子を含む、電池用電極。
- 前記吸着剤がゼオライトである、請求項1に記載の電池用電極。
- 前記ゼオライトが、Li又はCaでイオン交換されたゼオライトである、請求項2に記載の電池用電極。
- 前記ゼオライトのSi/Al原子比が1〜3の範囲にある、請求項2又は3に記載の電池用電極。
- 前記吸着剤の粒子が3〜10Åの細孔径を有する、請求項1から4のいずれか一項に記載の電池用電極。
- 前記無機酸化物がアルミナである、請求項1から5のいずれか一項に記載の電池用電極。
- 前記吸着剤と無機酸化物の質量比率(吸着剤/無機酸化物)が、2/98〜6/94の範囲にある、請求項1から6のいずれか一項に記載の電池用電極。
- 前記絶縁性多孔質膜の厚みが0.5μm以上10μm未満である、請求項1から7のいずれか一項に記載の電池用電極。
- 前記吸着剤の粒子の平均粒径が0.5〜3μmの範囲にあり、前記無機酸化物の平均粒径が0.1〜5μmの範囲にある、請求項1から8のいずれか一項に記載の電池用電極。
- 前記活物質層は、正極活物質を含む、請求項1から9のいずれか一項に記載の電池用電極。
- 請求項1から10のいずれか一項に記載の電極と、対極と、前記電極と前記対極の間のセパレータと、非水電解液を含むリチウムイオン二次電池。
- 前記セパレータの厚みが8〜40μmの範囲にある、請求項11に記載のリチウムイオン二次電池。
- 前記非水電解液がエチレンカーボネートを含む、請求項11又は12に記載のリチウムイオン二次電池。
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