JP6760620B2 - リチウム二次電池用正極活物質の製造方法および前記正極活物質を含むリチウム二次電池 - Google Patents
リチウム二次電池用正極活物質の製造方法および前記正極活物質を含むリチウム二次電池 Download PDFInfo
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Description
電池は、正極と負極に電気化学反応が可能な物質を使用することによって電力を発生させるものである。このような電池中の代表的な例としては、正極および負極でリチウムイオンがインターカレーション/デインターカレーションされる時の化学電位の変化により電気エネルギーを生成するリチウム二次電池がある。
リチウム二次電池の正極活物質としては、リチウム複合金属化合物が使用されており、その例としてLiCoO2、LiMn2O4、LiNiO2、LiNi1−xCoxO2(0<x<1)、LiMnO2、LiNi1−x−yCoxMnyO2(0<x<1、1<y<1)などの複合金属酸化物が研究されている。
Li1+xCo1−yMyO2
(上記式中、
−0.2≦x≦0.2であり、
0<y≦0.3であり、
Mは、Niと、Mn、B、Mg、Ca、Sr、Ba、Ti、V、Cr、Fe、Cu、Alまたはこれらの組み合わせから選択される一つとを含む。)
前記化学式1で表される化合物のMは、NiおよびMnを含むことができる。
Li1+xCo1−yMyO2
(上記式中、
−0.2≦x≦0.2であり、
0<y≦0.3であり、
Mは、Niと、Mn、B、Mg、Ca、Sr、Ba、Ti、V、Cr、Fe、Cu、Alまたはこれらの組み合わせから選択される一つとを含む。)
前記正極活物質に含まれる化学式1で表される化合物は、CoとMで表される金属を含み、この時、CoとMで表される金属のうち、Mで表される金属を20モル%以下で含有する。このような組成を有する化合物を正極活物質として使用することによってリチウム二次電池の電気化学的特性を改善することができる。前記リチウム二次電池は、容量と寿命に優れ、安定性にも優れ、且つ高出力および高容量化が可能である。
Li2CO3粉末39.55g、Co3O4粉末73.64gおよびNi0.95Mn0.025Mg0.025(OH)2粉末9.36gを混合して975℃で10時間にかけて1次焼成した。焼成して得た粉末をディスクミリングした後、エアジェットミルを行った。
Li2CO3粉末39.57g、Co3O4粉末69.60gおよびNi0.95Mn0.025Mg0.025(OH)2粉末14.06gを混合して975℃で10時間にかけて1次焼成した。焼成して得た粉末をディスクミリングした後、エアジェットミルを行った。
Li2CO3粉末39.60g、Co3O4粉末65.55gおよびNi0.95Mn0.025Mg0.025(OH)2粉末18.75gを混合して975℃で10時間にかけて1次焼成した。焼成して得た粉末をディスクミリングした後、エアジェットミルを行った。
Li2CO3粉末39.52g、Co3O4粉末77.69gおよびNi0.95Mn0.025Mg0.025(OH)2粉末28.12gを混合して975℃で10時間にかけて1次焼成した。焼成して得た粉末をディスクミリングした後、エアジェットミルを行った。
Li2CO3粉末39.64g、Co3O4粉末81.19gおよびMgO粉末0.41gを混合して1050℃で10時間にかけて1次焼成した。焼成して得た粉末をディスクミリングした後、エアジェットミルを行った。
前記合成例1で製造された粉末を正極活物質として使用し、バインダーとしてポリビニリデンフルオライドおよび導電剤としてカーボンブラックを90:5:5重量比にN−メチルピロリドン溶媒で混合して正極活物質層スラリーを製造した。前記正極活物質層スラリーを正極集電体としてアルミニウム箔上に塗布して薄い極板の形態で作った後、約120℃で1時間乾燥し、圧延して正極活物質層を含む正極を製造した。
前記実施例1で使用した正極活物質の代わりに合成例2で製造された粉末を使用した点を除いては、前記実施例1と同様な方法でコインセルを製造した。
前記実施例1で使用した正極活物質の代わりに合成例3で製造された粉末を使用した点を除いては、前記実施例1と同様な方法でコインセルを製造した。
前記実施例1で使用した正極活物質の代わりに合成例4で製造された粉末を使用した点を除いては、前記実施例1と同様な方法でコインセルを製造した。
前記実施例1で使用した正極活物質の代わりに合成例5で製造された粉末を使用した点を除いては、前記実施例1と同様な方法でコインセルを製造した。
112…負極
113…セパレータ
114…正極
120…電池容器
140…封入部材
Claims (8)
- 下記化学式1で表される化合物を含む正極活物質を含む正極と、
シリコン系負極活物質を含む負極と、
非水電解液とを含む、リチウム二次電池。
[化学式1]
LiCo1−yMyO2−z
(上記式中、
0.0975≦y≦0.3であり、
0≦z≦0.109であり、
Mは、NiおよびMnを含み、
前記Niの組成は、0.095以上であり、
前記Mnの組成は、0.0025以上であり、
前記NiおよびMnの組成比は、8<Ni/Mn≦90である。) - 前記化学式1で表される化合物のMは、Mg、Tiまたはこれらの組み合わせから選択される一つをさらに含む、請求項1に記載のリチウム二次電池。
- 充放電効率は、86乃至94%である、請求項1または2に記載のリチウム二次電池。
- 前記シリコン系負極活物質は、シリコン(Si)、シリコン酸化物、表面が導電性カーボンでコーティングされたシリコン酸化物、および表面が導電性カーボンでコーティングされたシリコン(Si)からなる群より選択された少なくとも一つである、請求項1〜3のいずれか1項に記載のリチウム二次電池。
- 固体状のLi原料物質、固体状のCo原料物質および固体状のM原料物質を混合した混合物を準備し、ただし、前記固体状のCo原料物質および前記固体状のM原料物質のモル比は、CoおよびMのモル比が0.7以上0.9025以下:0.0975以上0.3以下になるようにした混合物を準備する段階と、
前記混合物を粉末状態で950乃至1100℃で1次熱処理する段階と、
前記1次熱処理された混合物を粉砕する段階と、
前記粉砕された結果物を900乃至1050℃で2次熱処理する段階とを含み、
前記Mは、NiおよびMnを含む、リチウム二次電池用正極活物質の製造方法であって、
得られる正極活物質において、前記Niの組成は、0.095以上であり、前記Mnの組成は、0.0025以上であり、前記NiおよびMnの組成比は、8<Ni/Mn≦90である、リチウム二次電池用正極活物質の製造方法。 - 前記固体状のM原料物質は、NiおよびMnを含む共沈物である、請求項5に記載のリチウム二次電池用正極活物質の製造方法。
- 前記混合物は、B、Mg、Ca、Sr、Ba、Ti、V、Cr、Fe、Cu、Alまたはこれらの組み合わせから選択される一つの追加的な金属の原料物質をさらに含み、
前記固体状のCo原料物質、および前記固体状のM原料物質と前記追加的な金属の原料物質との合計量のモル比は、Co、およびMと追加的な金属との合計量のモル比が0.7以上1未満:0超過0.3以下になるようにした、請求項5または6に記載のリチウム二次電池用正極活物質の製造方法。 - 前記1次熱処理された混合物を粉砕した後、前記粉砕された粒子にNi、Mn、Coまたはこれらの組み合わせを含むコーティング層を乾式または湿式方法で形成した後、2次熱処理を行う、請求項5〜7のいずれか1項に記載のリチウム二次電池用正極活物質の製造方法。
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