JP7378605B2 - 負極活物質、電気化学装置及び電子装置 - Google Patents
負極活物質、電気化学装置及び電子装置 Download PDFInfo
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- JP7378605B2 JP7378605B2 JP2022520150A JP2022520150A JP7378605B2 JP 7378605 B2 JP7378605 B2 JP 7378605B2 JP 2022520150 A JP2022520150 A JP 2022520150A JP 2022520150 A JP2022520150 A JP 2022520150A JP 7378605 B2 JP7378605 B2 JP 7378605B2
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- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 1
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- 230000002441 reversible effect Effects 0.000 description 1
- 238000010008 shearing Methods 0.000 description 1
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- 239000002210 silicon-based material Substances 0.000 description 1
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- 229910001220 stainless steel Inorganic materials 0.000 description 1
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- 239000004094 surface-active agent Substances 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 1
- 229910001887 tin oxide Inorganic materials 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- ZSDSQXJSNMTJDA-UHFFFAOYSA-N trifluralin Chemical compound CCCN(CCC)C1=C([N+]([O-])=O)C=C(C(F)(F)F)C=C1[N+]([O-])=O ZSDSQXJSNMTJDA-UHFFFAOYSA-N 0.000 description 1
- 238000009966 trimming Methods 0.000 description 1
- 239000011800 void material Substances 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
Classifications
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Description
本発明で提供される負極活物質は、一般式SiOX(0.5≦x≦1.6)で表されるケイ素酸化物と黒鉛とを含むシリコン炭素複合体を含有し、前記シリコン炭素複合体は、関係式2≦b/a<6を満たし、ここで、aはケイ素酸化物の平均粒子径を表し、bは黒鉛の平均粒子径を表す。本発明の発明者が検討したところ、SiOXと黒鉛の平均粒子径が関係式2≦b/a<6を満たす場合に、適切な造粒粒子径及びより良好なサイクル特性が得られることができる。
本発明で提供される負極活物質の調製方法は、
溶媒でケイ素酸化物と黒鉛を混合して第1の混合物を形成するステップA、
カーボンナノチューブと前記第1の混合物を混合して第2の混合物を形成するステップB、
第2の混合物を噴霧乾燥して造粒を形成するステップC、
不活性雰囲気下で、ステップCで得られた造粒物を焼結するステップD、を含む。
いくつか実施例において、本発明で提供される負極は、本発明の第1の態様に記載の負極活物質を含む。
本発明の実施例は、負極、正極、電解液及びセパレータを含む電気化学装置を提供する。
本発明の電気化学装置における負極は、本発明の負極活物質を含む。
本発明の実施例に用いられる正極の材料、構成及びその製造方法は、先行技術に開示された任意の技術を含んでもよい。
本発明の実施例に使用される電解液は、先行技術で公知の電解液であってもよい。
いくつかの実施例において、正極と負極の間には、短絡を防止するためにセパレータが設けられる。本発明の実施例に使用されるセパレータの材料と形状は、特に制限がなく、先行技術で開示された任意の技術であってもよい。いくつかの実施例において、セパレータは、本発明の電解液に対して安定な材料で形成された重合体又は無機物等を含む。
本発明の電子装置は、本発明の第4の態様に係る電気化学装置を用いたものであればよい。
2.溶媒を除去した後に乾燥粉末が得られた。
3.窒素雰囲気下で、ステップ2で得られた乾燥粉末を焼結し、窒素流量は0.5~1.5L/minであり、炉内は常圧に保持し、焼結温度は600℃であり、焼結時間は2時間であった。
1、比表面積の測定:恒温低温で、異なる相対圧力で固体表面へのガスの吸着量を測定した後、Brownauer-Emmett-Teller吸着理論とその公式(BET公式)より、サンプル単分子層の吸着量を求め、固体の比表面積を算出する。各N2分子が占める平均面積は16.2A2であり、1.5~3.5gの粉末サンプルを秤量してTriStar II 3020のテストサンプルチューブに入れ、200℃で120min脱気した後に測定する。
電池セルの調製
N-メチルピロリジノン溶媒系に、活物質であるLiCoO2、導電性カーボンブラック、及びバインダーであるポリフッ化ビニリデン(PVDF)を96.7:1.7:1.6の重量比で十分に撹拌して均一に混合した後、Al箔に塗布して乾燥させ、コールドプレスして正極を得る。
測定温度は25℃又は45℃であり、0.7Cで4.45Vまで定電流で充電し、0.025Cまで定電圧で充電し、5分間静置した後に0.5Cで3.0Vまで放電する。ここで得られた容量を初期容量とし、0.7C充電/0.5C放電でサイクル充放電を行い、各サイクルの放電容量値を記録して下記式を用いてサイクル容量維持率を計算する。サイクルN回目の容量維持率=(N回目のサイクルの放電容量/初回サイクルの放電容量)×100%。25℃で、容量維持率が90%である場合には、その維持率でのサイクル数、すなわち25℃で容量維持率が90%までのサイクル数を記録し;45℃で、容量維持率が80%である場合には、その維持率でのサイクル数、すなわち45℃で、容量維持率が80%までのサイクル数を記録する。
充放電を行っていない時の初期電池セルの厚さD0をスクリューマイクロメーターで測定し、400回までサイクルした時、電池セルは満充電状態にあり、そしてこの時の電池セルの厚さD1をスクリューマイクロメーターで測定し、下記式に基づいて電池の厚さ膨張率εを計算する。ε=(D1-D0)/D0×100%。これにより、25℃又は45℃で400サイクルまでの電池セル膨張率を得る。
Claims (14)
- シリコン炭素複合体を含む負極活物質であって、
前記シリコン炭素複合体は、ケイ素酸化物及び黒鉛を含み、前記ケイ素酸化物の一般式はSiOX、0.5≦x≦1.6であり、
前記シリコン炭素複合体は、関係式2≦b/a<6を満たし、式中、aはケイ素酸化物の平均粒子径を表し、bは黒鉛の平均粒子径を表し、
前記負極活物質は、さらに前記シリコン炭素複合体の表面に位置する保護層を含み、
前記保護層は、カーボンナノチューブ、及びアモルファスカーボンを含む、負極活物質。 - aは2μm~6μmである、請求項1に記載の負極活物質。
- bは4.1μm~30μmである、請求項1に記載の負極活物質。
- cは負極活物質のDv50を表し、cは6.1μm~60μmである、請求項1に記載の負極活物質。
- 前記負極活物質は、関係式a+b≦c≦5bを満たす、請求項4に記載の負極活物質。
- 前記保護層は、さらにグラフェンを含む、請求項1に記載の負極活物質。
- 以下の条件(i)、条件(ii)、又は条件(iii)のうちの少なくとも1つを満たす負極活物質であって、
(i)前記保護層は第1の保護材と第2の保護材とを含み、前記第1の保護材はカーボンナノチューブ、アモルファスカーボン又はグラフェンのうちの少なくとも1種を含み、前記第2の保護材はカーボンナノチューブ、アモルファスカーボン又はグラフェンのうちの少なくとも1種を含むこと、
(ii)前記カーボンナノチューブの長さはdであり、1μm≦d≦15μmであること、
(iii)負極活物質に対して、前記保護層の質量分率は0.05%~5%であること、請求項1に記載の負極活物質。 - 前記保護層は、第1の保護材と第2の保護材を含み、前記第1の保護材の厚みは20nm~300nmであり、前記第2の保護材の厚みは20nm~500nmである、請求項1に記載の負極活物質。
- 以下の条件(a)又は条件(b)のうちの少なくとも1つを満たす負極活物質であって、
(a)前記負極活物質の比表面積は1m2/g~50m2/gであること、
(b)負極活物質に対して、前記ケイ素酸化物の質量分率は5%~50%であり、前記黒鉛の質量分率は25%~93.5%であること、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、電解液、セパレータ及び正極を含む、電気化学装置。
- 前記電解液は、さらに、リチウム塩を含み、前記リチウム塩は、リチウムビス(フルオロスルホニル)イミド及び六フッ化リン酸リチウムを含む、請求項10に記載の電気化学装置。
- 前記リチウム塩の濃度は、1mol/L~2mol/Lである、請求項11に記載の電気化学装置。
- 前記リチウムビス(フルオロスルホニル)イミドと六フッ化リン酸リチウムとの質量比は0.06~5である、請求項11に記載の電気化学装置。
- 請求項10~13のいずれか一項に記載の電気化学装置を含む、電子装置。
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