JP6238251B2 - 多孔性シリコン系負極活物質及びこれを含むリチウム二次電池 - Google Patents
多孔性シリコン系負極活物質及びこれを含むリチウム二次電池 Download PDFInfo
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- JP6238251B2 JP6238251B2 JP2015550345A JP2015550345A JP6238251B2 JP 6238251 B2 JP6238251 B2 JP 6238251B2 JP 2015550345 A JP2015550345 A JP 2015550345A JP 2015550345 A JP2015550345 A JP 2015550345A JP 6238251 B2 JP6238251 B2 JP 6238251B2
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- 229910052719 titanium Inorganic materials 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical group 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 229910001935 vanadium oxide Inorganic materials 0.000 description 1
- 229920002554 vinyl polymer Polymers 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
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Description
MySi (1)
前記化学式(1)において、MはSc、Ti、V、Cr、Mn、Fe、Co、Ni、Cu、Zn、Y、Zr、Nb、Mo、Ru、Rh、Pd、La、Hf、Ta、W、Re、Os、Mg、Ca、B、P、Al、Ge、Sn、Sb、Bi及びLiを含むいずれか一つの元素、またはこれらのうち2種以上の元素を含み、
yは0.001から0.4である。
(実施例1)
平均粒径(D50)が5μmであり、比表面積(BET−SSA)が18m2/gである多孔性Si粒子(a);及び平均粒径(D50)が20μmである粗粒黒鉛粒子、及び平均粒径(D50)が3μmである微粒黒鉛粒子を重量比80:20で混合した黒鉛粒子(b)を混合して負極活物質を製造した。このとき、Si粒子(a)及び黒鉛粒子(b)の混合比は5:95重量比であった。
黒鉛粒子(b)として平均粒径(D50)が20μmである粗粒黒鉛粒子のみ用いたことを除いては、実施例1と同様の方法で負極活物質を製造した。
多孔性Si粒子に代えて非多孔性Si粒子を用いたことを除いては、実施例1と同様の方法で負極活物質を製造した。
多孔性Si粒子に代えて非多孔性Si粒子を用いたことを除いては、比較例1と同様の方法で負極活物質を製造した。
(実施例2)
実施例1で製造された負極活物質、導電材としてアセチレンブラック、及びバインダーとしてポリビニリデンフルオリドを用いて、95:1:4の重量比で混合し、これらを溶媒であるN−メチル−2−ピロリドンに混合してスラリーを製造した。製造されたスラリーを銅集電体の一面に30μmの厚さにコーティングし、乾燥及び圧延した後、一定の大きさにパンチングして負極を製造した。
負極活物質として、実施例1で製造された負極活物質を用いる代わりに比較例1から3で製造された負極活物質を用いたことを除いては、実施例2と同様の方法でコイン形半電池を製造した。
実施例2、及び比較例4から6で製造されたコイン形半電池の充放電サイクルに伴う容量特性及び寿命特性を調べるため、実施例2、及び比較例4から6で製造されたコイン形半電池を、23℃で定電流/定電圧(CC/CV)条件下、5mV、0.005Cまで0.1Cで充電した後、定電流(CC)条件で1.5Vまで0.1Cで放電し、容量を測定した。
表1から確認できるところのように、多孔性Si粒子、及び平均粒径が互いに異なる微粒炭素粒子及び粗粒炭素粒子を共に含む炭素粒子を混合した負極活物質を用いた実施例2の二次電池が、多孔性シリコン粒子を粗粒炭素粒子のみ含んだ炭素粒子と混合した比較例4に比べ、寿命特性が約5%程度向上することを確認することができる。
120 炭素粒子
210 多孔性シリコン系粒子
220 粗粒炭素粒子
230 微粒炭素粒子
Claims (7)
- 多孔性シリコン系粒子及び炭素粒子を含み、
前記炭素粒子が、平均粒径が互いに異なる微粒炭素粒子及び粗粒炭素粒子からなり、
前記多孔性シリコン系粒子は、多孔性Si粒子であり、平均粒径(D50)が、5μmから10μmであり、
前記微粒炭素粒子の平均粒径(D50)が、1μmから5μmであり、
前記粗粒炭素粒子の平均粒径(D50)が、10μmから20μmであり、
前記多孔性シリコン系粒子及び炭素粒子の混合比が、重量比で1:1から20であり、
前記微粒炭素粒子及び粗粒炭素粒子の混合比が、重量比で1:4から9であることを特徴とする、負極活物質。 - 前記微粒炭素粒子が、前記炭素粒子の全体重量に対して1重量%から30重量%の量で含まれることを特徴とする、請求項1に記載の負極活物質。
- 前記多孔性シリコン系粒子の気孔の平均直径が、30nmから500nmであることを特徴とする、請求項1に記載の負極活物質。
- 前記多孔性シリコン系粒子の比表面積(BET−SSA)が、5m2/gから50m2/gであることを特徴とする、請求項1に記載の負極活物質。
- 前記炭素粒子が、人造黒鉛、天然黒鉛、メソカーボン、非晶質ハードカーボン、低結晶質ソフトカーボン、カーボンブラック、アセチレンブラック、ケッチェンブラック、スーパーP、グラフェン、繊維状炭素及び表面が被覆された黒鉛のうち選択されるいずれか一つ、またはこれらのうち2種以上の混合物であることを特徴とする、請求項1に記載の負極活物質。
- 請求項1に記載の負極活物質を含む負極。
- 請求項6に記載の負極を含むリチウム二次電池。
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GB2499984B (en) | 2012-02-28 | 2014-08-06 | Nexeon Ltd | Composite particles comprising a removable filler |
GB2502625B (en) | 2012-06-06 | 2015-07-29 | Nexeon Ltd | Method of forming silicon |
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CN113224286B (zh) * | 2021-04-25 | 2022-11-08 | 浙江大学自贡创新中心 | 一种高容量锂离子电池硅基复合负极材料及其制备方法 |
EP4261945A1 (en) * | 2021-09-03 | 2023-10-18 | LG Energy Solution, Ltd. | Negative electrode active material, negative electrode comprising negative electrode active material, secondary battery comprising negative electrode, and method for preparing negative electrode active material |
WO2023158264A1 (ko) | 2022-02-17 | 2023-08-24 | 대주전자재료 주식회사 | 규소-탄소 복합체, 이의 제조방법, 및 이를 포함하는 음극 활물질 및 리튬 이차전지 |
KR20230123898A (ko) | 2022-02-17 | 2023-08-24 | 대주전자재료 주식회사 | 규소-탄소 혼합체, 이의 제조방법 및 이를 포함하는 음극 활물질 및 리튬 이차전지 |
KR20230138929A (ko) | 2022-03-23 | 2023-10-05 | 대주전자재료 주식회사 | 규소-탄소 복합체, 이의 제조방법, 및 이를 포함하는 음극 활물질 및 리튬 이차전지 |
WO2023182862A1 (ko) | 2022-03-25 | 2023-09-28 | 대주전자재료 주식회사 | 규소-탄소 혼합체, 이의 제조방법 및 이를 포함하는 음극 활물질 및 리튬 이차전지 |
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JP3816799B2 (ja) * | 2001-12-21 | 2006-08-30 | 株式会社日立製作所 | リチウム二次電池 |
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JP4996827B2 (ja) * | 2005-03-22 | 2012-08-08 | Jfeケミカル株式会社 | リチウムイオン二次電池負極用金属−黒鉛系複合粒子およびその製造方法、リチウムイオン二次電池用負極材料および負極ならびにリチウムイオン二次電池 |
KR100981909B1 (ko) * | 2008-04-15 | 2010-09-13 | 애경유화 주식회사 | 리튬 이차 전지용 음극 활물질, 그의 제조 방법 및 그를포함하는 리튬 이차 전지 |
TW201133983A (en) * | 2009-11-03 | 2011-10-01 | Envia Systems Inc | High capacity anode materials for lithium ion batteries |
KR20120010211A (ko) * | 2010-07-23 | 2012-02-02 | 강원대학교산학협력단 | 다공성 실리콘계 화합물 또는 다공성 실리콘, 이의 제조 방법, 및 이를 포함하는 리튬 이차 전지용 음극 활물질 및 리튬 이차 전지 |
JP5877025B2 (ja) * | 2010-09-17 | 2016-03-02 | 古河電気工業株式会社 | 多孔質シリコン複合体粒子及びその製造方法 |
JP5809897B2 (ja) * | 2010-09-17 | 2015-11-11 | 古河電気工業株式会社 | 多孔質シリコン粒子及びその製造方法、並びにリチウムイオン二次電池用負極及びリチウムイオン二次電池 |
CN102157731B (zh) * | 2011-03-18 | 2015-03-04 | 上海交通大学 | 一种锂离子电池硅碳复合负极材料及其制备方法 |
KR101396521B1 (ko) * | 2011-08-05 | 2014-05-22 | 강원대학교산학협력단 | 리튬 이차 전지용 음극 활물질, 이의 제조 방법, 그리고 이를 포함하는 음극 및 리튬 이차 전지 |
WO2013114095A1 (en) * | 2012-01-30 | 2013-08-08 | Nexeon Limited | Composition of si/c electro active material |
GB2499984B (en) * | 2012-02-28 | 2014-08-06 | Nexeon Ltd | Composite particles comprising a removable filler |
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EP2879216A1 (en) | 2015-06-03 |
KR101704103B1 (ko) | 2017-02-07 |
PL2879216T3 (pl) | 2019-07-31 |
CN104704660A (zh) | 2015-06-10 |
US20160197342A1 (en) | 2016-07-07 |
JP2016502253A (ja) | 2016-01-21 |
US20210313568A1 (en) | 2021-10-07 |
CN104704660B (zh) | 2017-09-26 |
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