JP2021528825A - 硫黄−炭素複合体、この製造方法及びこれを含むリチウム二次電池 - Google Patents
硫黄−炭素複合体、この製造方法及びこれを含むリチウム二次電池 Download PDFInfo
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Abstract
Description
内部及び外部の表面がイオン伝導性官能基と電子伝導性官能基を含むポリマーでコーティングされた多孔性炭素材と;
前記多孔性炭素材の内部及び表面の少なくとも一部に硫黄と;を含む硫黄−炭素複合体を提供する。
ここで、本発明では、硫黄−炭素複合体と電解液との反応性及びリチウム二次電池の容量及び効率特性改善効果を確保するために、内部及び外部の表面がイオン伝導性官能基と電子伝導性官能基を含むポリマーでコーティングされた多孔性炭素材と;前記多孔性炭素材の内部及び表面の中で少なくとも一部に硫黄と;を含む硫黄−炭素複合体を提供する。
本発明の硫黄−炭素複合体は、(a)イオン伝導性官能基と電子伝導性官能基を含むポリマーを含む溶液に多孔性炭素材を混合した後、乾燥してイオン伝導性官能基と電子伝導性官能基を含むポリマーがコーティングされた多孔性炭素材を製造する段階と;
(b)前記イオン伝導性官能基と電子伝導性官能基を含むポリマーがコーティングされた多孔性炭素材に硫黄を混合した後、熱処理して硫黄−炭素複合体を製造する段階と;を通じて製造される。
本発明で提示する硫黄−炭素複合体は、リチウム二次電池の正極活物質として好ましく使用することができる。
本発明の一実施例として、リチウム二次電池は上述した正極と;負極活物質としてリチウム金属またはリチウム合金を含む負極と;前記正極と負極の間に介在される分離膜と;前記負極、正極及び分離膜に含浸されていて、リチウム塩と有機溶媒を含む電解質とを含むことができ、好ましくは前記リチウム二次電池は正極内の正極活物質内に硫黄化合物を含むリチウム−硫黄電池であってもよい。
硫黄−炭素複合体の製造
[実施例1]
PEG−block−PEDOT(Sigma−aldrich)0.2gをTHFに溶解させてコーティング溶液を5g製造した。
PEG−block−PEDOT(製品名、sigma−aldrich)0.4gをTHFに溶解させてコーティング溶液5gを製造して使ったことを除いては、実施例1と同様の方法で硫黄−炭素複合体を製造した。
PEG−block−PEDOTがコーティングされていないカーボンナノチューブを使ったことを除いては、実施例1と同様の方法で硫黄−炭素複合体を製造した。
硫黄/炭素複合体2g(硫黄(sulfur) 1.5g)を均一に混合し、前記硫黄−炭素複合体にPEG−block−PEDOTの代わりにポリエチレンイミド(polyethyleneimide)をコーティングしたことを除いては、実施例1と同様の方法で硫黄−炭素複合体を製造した。
硫黄/炭素複合体2g(硫黄(sulfur) 1.5g)を均一に混合し、155℃で30分間溶融拡散(melt diffusion)させて硫黄−炭素複合体を製造した。そして、PEG−block−PEDOT(sigma−aldrich)0.2gをTHFに溶解させてコーティング溶液を5g製造した後、前記溶液に硫黄/炭素複合体2gを乳鉢で15分間撹拌した後、80℃オーブンで30分間乾燥し、PEG−block−PEDOTがコーティングされた硫黄/炭素複合体を製造した。
硫黄/炭素複合体2gを均一に混合し、PEG−block−PEDOTの代わりにポリイミドをコーティングしたことを除いては、実施例1と同様の方法で硫黄−炭素複合体を製造した。
PEG−block−PEDOT(製品名、sigma−aldrich)の代わりにポリエチレンオキサイドを使ったことを除いては、実施例1と同様の方法で硫黄−炭素複合体を製造した。
実施例1で製造されたPEG−block−PEDOTがコーティングされた硫黄−炭素複合体と、比較例1で製造した硫黄−炭素複合体に対して、TGA(Thermogravimetric analysis、Mettler−Toledo、TGA2)分析を行い、その結果を図2に示す。
実施例1及び比較例1で製造された複合体を利用し、硫黄−炭素複合体:導電材:バインダー=90:5:5の重量比でスラリーを製造した後、20μm厚さのアルミニウムホイルの集電体に塗布し、80℃オーブンで30分間乾燥した後、圧延して正極を製造した。この時、導電材はカーボンブラックを、バインダーではスチレンブタジエンゴム、カルボキシメチルセルロースを使用した。以後、分離膜でポリエチレンを使用し、負極として150μm厚さのリチウムホイルを使用してリチウム二次電池コインセルを製造した。
前記実験例2と同様の方法で、比較例1と比較例2ないし4で製造された複合体を利用してコインセルを製造した後、セルをテストした。この時得られた結果は図5ないし図7に示す。
Claims (13)
- 内部及び外部の表面がイオン伝導性官能基と電子伝導性官能基を含むポリマーでコーティングされた多孔性炭素材と;
前記多孔性炭素材の内部及び表面の少なくとも一部に硫黄と;を含む硫黄−炭素複合体。 - 前記イオン伝導性官能基と電子伝導性官能基を含むポリマーは、PEG及びポリエチレンオキサイドからなる群から選択されるいずれか一つ以上の化合物;並びにPEDOT、チオフェン及びピロールからなる群から選択されるいずれか一つ以上の化合物;を含む、請求項1に記載の硫黄−炭素複合体。
- 前記イオン伝導性官能基と電子伝導性官能基を含むポリマーの含量が硫黄−炭素複合体の重量全体に対して0.5ないし5.0重量%である、請求項1から3のいずれか一項に記載の硫黄−炭素複合体。
- 前記硫黄のローディング量が5mAh/cm2以上である、請求項1から4のいずれか一項に記載の硫黄−炭素複合体。
- 前記硫黄−炭素複合体は、硫黄と多孔性炭素材が9:1ないし7:3の重量比で含まれる、請求項1から5のいずれか一項に記載の硫黄−炭素複合体。
- 前記多孔性炭素材はグラファイト、グラフェン、カーボンブラック、カーボンナノチューブ、炭素繊維及び活性炭からなる群から選択された1種以上である、請求項1から6のいずれか一項に記載の硫黄−炭素複合体。
- 請求項1から7のいずれか一項に記載の硫黄−炭素複合体を含む、リチウム二次電池用正極。
- (a)イオン伝導性官能基と電子伝導性官能基を含むポリマーを含む溶液に多孔性炭素材を混合した後、乾燥してイオン伝導性官能基と電子伝導性官能基を含むポリマーがコーティングされた多孔性炭素材を製造する段階と;
(b)前記イオン伝導性官能基と電子伝導性官能基を含むポリマーがコーティングされた多孔性炭素材に硫黄を混合した後、熱処理して硫黄−炭素複合体を製造する段階と;を含む硫黄−炭素複合体の製造方法。 - 前記多孔性炭素材はグラファイト、グラフェン、カーボンブラック、カーボンナノチューブ、炭素繊維及び活性炭からなる群から選択された1種以上である、請求項9に記載の硫黄−炭素複合体の製造方法。
- 前記イオン伝導性官能基と電子伝導性官能基を含むポリマーは、PEG及びポリエチレンオキサイドからなる群から選択されるいずれか一つ以上の化合物;並びにPEDOT、チオフェン及びピロールからなる群から選択されるいずれか一つ以上の化合物;を含む、請求項9または10に記載の硫黄−炭素複合体の製造方法。
- 前記溶液の溶媒は、エタノール及びTHFからなる群から選択されるいずれか一つ以上である、請求項9から11のいずれか一項に記載の硫黄−炭素複合体の製造方法。
- 請求項8に記載の正極と;負極と;電解質と;を含むリチウム二次電池。
Applications Claiming Priority (5)
Application Number | Priority Date | Filing Date | Title |
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KR20180132423 | 2018-10-31 | ||
KR10-2018-0132423 | 2018-10-31 | ||
PCT/KR2019/014640 WO2020091478A1 (ko) | 2018-10-31 | 2019-10-31 | 황-탄소 복합체, 이의 제조방법 및 이를 포함하는 리튬 이차전지 |
KR1020190137949A KR20200049685A (ko) | 2018-10-31 | 2019-10-31 | 황-탄소 복합체, 이의 제조방법 및 이를 포함하는 리튬 이차전지 |
KR10-2019-0137949 | 2019-10-31 |
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JP2021528825A true JP2021528825A (ja) | 2021-10-21 |
JP7128303B2 JP7128303B2 (ja) | 2022-08-30 |
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JP2016540353A (ja) * | 2013-12-03 | 2016-12-22 | イオニツク・マテリアルズ・インコーポレーテツド | 固体イオン伝導性高分子材料及び用途 |
KR20170085195A (ko) * | 2016-01-14 | 2017-07-24 | 한국과학기술연구원 | 표면 코팅된 양극 활물질, 그 제조방법 및 이를 이용한 이차전지 |
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KR101726127B1 (ko) * | 2016-02-22 | 2017-04-12 | 한양대학교 산학협력단 | 블록 공중합체를 이용한 염료감응 태양전지용 상대전극 및 이를 포함하는 염료감응 태양전지 |
WO2018075469A1 (en) * | 2016-10-17 | 2018-04-26 | Massachusetts Institute Of Technology | Dual electron-ion conductive polymer composite |
KR101990616B1 (ko) * | 2016-11-24 | 2019-06-18 | 주식회사 엘지화학 | 리튬-황 전지용 양극 활물질, 이의 제조방법 및 이를 포함하는 리튬-황 전지 |
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KR20170085195A (ko) * | 2016-01-14 | 2017-07-24 | 한국과학기술연구원 | 표면 코팅된 양극 활물질, 그 제조방법 및 이를 이용한 이차전지 |
WO2017205634A1 (en) * | 2016-05-27 | 2017-11-30 | Ionic Material, Inc. | ELECTROCHEMICAL CELL HAVING SOLID lONICALLY CONDUCTING POLYMER MATERIAL |
WO2018084449A2 (ko) * | 2016-11-02 | 2018-05-11 | 주식회사 엘지화학 | 황-탄소 복합체 및 이를 포함하는 리튬-황 전지 |
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US20210119216A1 (en) | 2021-04-22 |
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