JP6019225B2 - 二次電池用電極組立体及びそれを含むリチウム二次電池 - Google Patents
二次電池用電極組立体及びそれを含むリチウム二次電池 Download PDFInfo
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Description
Li1+xNiaMnbCo1−(a+b)O2 (1)
上記式中、−0.2≦x≦0.2、0.5≦a≦0.6、0.2≦b≦0.3である。
Li(Co(1−a)Ma)O2 (2)
上記式中、
0.1≦a≦0.2であり、
前記Mは、Mg、K、Na、Ca、Si、Ti、Zr、Sn、Y、Sr、Mo、及びMn元素から選択される一つ以上の元素である。
SiO1−x (3)
上記式中、−0.5≦x≦0.5である。
(正極の製造)
LiNi0.55Mn0.30Co0.15O2とPVdFを混合した後、150〜600℃の温度範囲で9時間加熱処理して、表面にLiF表面フィルムが形成されたLiNi0.55Mn0.30Co0.15O2を得た。
SiとSiO2を1:1のモル比で混合した混合物を800℃で減圧熱処理して、SiO1−x(x=0)を製造した。前記SiO1−x(信越社製)とMAG−V2(日立社製)とAGM01(三菱社製)を5:10.6:84.4の割合で混合して、混合負極材料を製造した。
ポリビニリデンフルオライド−ヘキサフルオロプロピレン共重合体(PVdF−HFP)と分子をアセトンに約8.5重量%添加した後、50℃の温度で約12時間以上溶解させて、高分子溶液を製造した。この高分子溶液に、Al2O3粉末をAl2O3/PVdF−HFP=90/10(重量%比)になるように添加し、12時間以上ボールミル(ball mill)法を用いてスラリーを製造した。このように製造されたスラリーを、ディップ(dip)コーティング法を用いて、厚さ7〜9μm程度のポリエチレン分離膜(気孔度45%)にコーティングした。コーティング厚さは約4〜5μmに調節して、気孔率測定装置(porosimeter)で測定したとき、ポリエチレン分離膜にコーティングされた活性層内の気孔サイズ及び気孔度がそれぞれ0.5μm及び58%である有/無機複合多孔性分離膜を製造した。
上記で製造された負極と正極との間に前記分離膜を介在して電極組立体を製造した。このように製造された電極組立体をアルミニウム缶またはアルミニウムパウチに入れ、電極リードを連結した後、1MのLiPF6が含まれたカーボネート系列の複合溶液を電解質として注入した後、密封して、リチウム二次電池を組み立てた。
混合正極材料でないLiCoO2のみを使用し、前記SiO1−x(信越社製)、MAG−V2(日立社製)、AGM01(三菱社製)を3:10.8:86.2の割合で混合して混合負極材料を製造したこと以外は、実施例1と同様の方法で正極材料、負極材料及びリチウム二次電池を製造した。
混合正極材料でないLiCoO2のみを使用したこと以外は、実施例1と同様の方法で正極材料、負極材料及びリチウム二次電池を製造した。
混合正極材料を使用することによる効果を確認するために、実施例1及び比較例1、2で製造された電池を作動電圧に応じて容量を測定して、その結果を図3に示した。
上記実施例1において、Mg(1000ppm)及びTi(1000ppm)でドープし、Al2O3(Al:400ppm)でコーティング処理したLiCoO2を使用したこと以外は、実施例1と同様の方法で正極材料、負極材料及びリチウム二次電池を製造した。
上記実施例1において、Mg(1000ppm)及びTi(1000ppm)でドープし、Al2O3(Al:400ppm)でコーティング処理したLiCoO2を使用したこと、及び表面コーティングされていないLiNi0.55Mn0.30Co0.15O2を使用したこと以外は、実施例1と同様の方法で正極材料、負極材料及びリチウム二次電池を製造した。
NMC表面コーティングによる効果を確認するために、上記実施例2及び比較例3でそれぞれ製造された電池に対して、温度変化による電池のスウェリング現象による厚さの変化量を比較して、その結果を図4に示した。
110 リチウムニッケル−マンガン−コバルト酸化物
120 リチウムコバルト酸化物
130 コーティング層
140 コーティング層
Claims (16)
- 正極、負極及び分離膜を含む電極組立体であって、
前記正極が、正極活物質として、リチウムコバルト系酸化物、及びフッ素含有ポリマーと反応してその表面にコーティング層としてのLiFを形成したリチウムニッケル系複合酸化物を含み、前記負極が、負極活物質として、炭素及びシリコン酸化物を含み、
作動電圧領域が2.50V〜4.35Vであり、
前記正極活物質が、前記リチウムコバルト系酸化物の平均粒径とリチウムニッケル系複合酸化物の平均粒径が互いに異なるバイモーダル形態によって、3.8〜4.0g/ccの圧延密度を有し、
前記リチウムコバルト系酸化物の平均粒径が16〜25μmであり、前記リチウムニッケル系複合酸化物の平均粒径が2〜10μmであることを特徴とする、電極組立体。 - 前記リチウムニッケル系複合酸化物が、下記化学式1で表されるリチウムニッケル−マンガン−コバルト複合酸化物であることを特徴とする、請求項1に記載の電極組立体:
Li1+xNiaMnbCo1−(a+b)O2 (1)
上記式中、−0.2≦x≦0.2、0.5≦a≦0.6、0.2≦b≦0.3である。 - 前記フッ素含有ポリマーがPVdFまたはPVdF−HFPであることを特徴とする、請求項1に記載の電極組立体。
- 前記コーティング層のフッ素含有量が、前記リチウムニッケル系複合酸化物の全質量に対して0.001〜3000ppmであることを特徴とする、請求項1に記載の電極組立体。
- 前記コーティング層の厚さが0.5nm〜2nmであることを特徴とする、請求項1に記載の電極組立体。
- 前記コーティング層が、前記リチウムニッケル系複合酸化物の表面全体に形成されたことを特徴とする、請求項1に記載の電極組立体。
- 前記リチウムニッケル系複合酸化物が、前記正極活物質の全質量に対して10〜50質量%含まれていることを特徴とする、請求項1に記載の電極組立体。
- 前記リチウムコバルト系酸化物が、表面にAl2O3がコーティングされており、Alの含有量は、前記リチウムコバルト系酸化物の全質量に対して0.001〜2000ppmであることを特徴とする、請求項1に記載の電極組立体。
- 前記Al2O3のコーティング厚さが0.5nm〜2nmであることを特徴とする、請求項8に記載の電極組立体。
- 前記Al2O3が、前記リチウムコバルト系酸化物の表面全体にコーティングされたことを特徴とする、請求項8に記載の電極組立体。
- 前記リチウムコバルト系酸化物が、異種金属元素でドープされ、下記化学式2で表されることを特徴とする、請求項1に記載の電極組立体:
Li(Co(1−a)Ma)O2 (2)
上記式中、
0.1≦a≦0.2、
前記Mが、Mg、K、Na、Ca、Si、Ti、Zr、Sn、Y、Sr、Mo、及びMn元素から選択される1つ以上の元素である。 - 前記Mが、Mg及び/又はTiであることを特徴とする、請求項11に記載の電極組立体。
- 前記シリコン酸化物が、下記化学式3で表されることを特徴とする、請求項1に記載の電極組立体:
SiO1−x (3)
上記式中、−0.5≦x≦0.5である。 - 前記シリコン酸化物が、前記負極活物質の全質量に対して3〜20質量%含まれていることを特徴とする、請求項1に記載の電極組立体。
- 前記分離膜が、有/無機複合多孔性分離膜であることを特徴とする、請求項1に記載の電極組立体。
- 請求項1に記載の電極組立体を含む、リチウム二次電池。
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CN104201374A (zh) * | 2014-09-11 | 2014-12-10 | 海宁美达瑞新材料科技有限公司 | 一种高容量的锂离子电池正极材料及其制备方法 |
KR101761367B1 (ko) | 2014-12-19 | 2017-07-25 | 주식회사 엘지화학 | 혼합 양극활물질, 이를 포함하는 양극 및 이차전지 |
US10826057B2 (en) | 2014-12-19 | 2020-11-03 | Lg Chem, Ltd. | Mixed positive electrode active material, positive electrode comprising same, and secondary battery |
PL3248232T3 (pl) * | 2015-01-23 | 2020-01-31 | Umicore | Proszki katodowe z tlenkiem litowo-niklowo- manganowo-kobaltowym do baterii litowo-jonowych o wysokim napięciu |
EP3248233B1 (en) * | 2015-01-23 | 2021-06-23 | Umicore | Lithium metal oxide cathode powders for high voltage lithium-ion batteries |
WO2017010780A1 (ko) * | 2015-07-10 | 2017-01-19 | 주식회사 엘지화학 | 세퍼레이터 및 이를 포함하는 전기화학소자 |
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