JP6063705B2 - 非水電解質二次電池 - Google Patents
非水電解質二次電池 Download PDFInfo
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- JP6063705B2 JP6063705B2 JP2012228536A JP2012228536A JP6063705B2 JP 6063705 B2 JP6063705 B2 JP 6063705B2 JP 2012228536 A JP2012228536 A JP 2012228536A JP 2012228536 A JP2012228536 A JP 2012228536A JP 6063705 B2 JP6063705 B2 JP 6063705B2
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- Prior art keywords
- positive electrode
- lithium
- negative electrode
- electrolyte secondary
- secondary battery
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- NJLLQSBAHIKGKF-UHFFFAOYSA-N dipotassium dioxido(oxo)titanium Chemical compound [K+].[K+].[O-][Ti]([O-])=O NJLLQSBAHIKGKF-UHFFFAOYSA-N 0.000 description 1
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- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 1
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- GLXDVVHUTZTUQK-UHFFFAOYSA-M lithium hydroxide monohydrate Substances [Li+].O.[OH-] GLXDVVHUTZTUQK-UHFFFAOYSA-M 0.000 description 1
- 229940040692 lithium hydroxide monohydrate Drugs 0.000 description 1
- 229910002102 lithium manganese oxide Inorganic materials 0.000 description 1
- QEXMICRJPVUPSN-UHFFFAOYSA-N lithium manganese(2+) oxygen(2-) Chemical class [O-2].[Mn+2].[Li+] QEXMICRJPVUPSN-UHFFFAOYSA-N 0.000 description 1
- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical class [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 description 1
- 229910052943 magnesium sulfate Inorganic materials 0.000 description 1
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- 229940099596 manganese sulfate Drugs 0.000 description 1
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- 235000007079 manganese sulphate Nutrition 0.000 description 1
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
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- 238000002844 melting Methods 0.000 description 1
- AUHZEENZYGFFBQ-UHFFFAOYSA-N mesitylene Substances CC1=CC(C)=CC(C)=C1 AUHZEENZYGFFBQ-UHFFFAOYSA-N 0.000 description 1
- 125000001827 mesitylenyl group Chemical group [H]C1=C(C(*)=C(C([H])=C1C([H])([H])[H])C([H])([H])[H])C([H])([H])[H] 0.000 description 1
- 150000001247 metal acetylides Chemical class 0.000 description 1
- 229940017219 methyl propionate Drugs 0.000 description 1
- 239000011325 microbead Substances 0.000 description 1
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- 229910052750 molybdenum Inorganic materials 0.000 description 1
- PYLWMHQQBFSUBP-UHFFFAOYSA-N monofluorobenzene Chemical compound FC1=CC=CC=C1 PYLWMHQQBFSUBP-UHFFFAOYSA-N 0.000 description 1
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Images
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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- Secondary Cells (AREA)
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Description
〔前記一般組成式(1)中、−0.15≦y≦0.15であり、かつ、Mは、NiまたはNiを含む2種以上の元素群を表し、Mを構成する各元素中で、Niの割合(mol%)をaとしたときに、30≦a≦100である。〕
<正極の作製>
正極活物質であるLi1.00Ni0.89Co0.06Mn0.02Mg0.02Ba0.01O2で表されるリチウム含有複合酸化物:95質量部と、導電助剤であるケッチェンブラック:3質量部と、バインダであるVDF−CTFE:1質量部と、脱水NMPとを、プラネタリーミキサーで混合してスラリーを調製し、このスラリーに、バインダであるPVDF:1質量部を加えて更に混合して正極合剤層形成用スラリーを調製した。
平均粒径D50%が16μm、d002が0.3360nmで、R値が0.05の黒鉛Aと、黒鉛Aの表面にピッチコート被覆した黒鉛B(平均粒径D50%:18μm、d002:0.3380nmで、R値が0.18、比表面積3.2m2/g)とを、30:70の質量比で混合した混合物:93.1質量部、平均粒子径D50%が8μmであるSiOの表面を炭素材料で被覆した複合体(複合体における炭素材料の量が10質量%。以下、これを「SiO/炭素材料複合体」という。):4.9質量部、粘度が1500〜5000mPa・sの範囲に調整された1質量%濃度のCMC水溶液:1.0質量部、およびSBR:1.0質量部を、比伝導度が2.0×105Ω/cm以上のイオン交換水を溶剤として混合して、水系の負極合剤層形成用ペーストを調製した。なお、この負極合剤層形成用ペーストにおいて、黒鉛Aと黒鉛Bとの混合物と、SiO/炭素材料複合体との比率は、95:5(質量比)とした。
前記の正極と前記の負極とを、PE製の微多孔膜からなるセパレータ(厚み18μm、空孔率50%)を介して重ね合わせてロール状に巻回した後、正負極に端子を溶接し、厚み49mm、幅42mm、高さ61mm(494261型)のアルミニウム合金製外装缶に挿入し、外装缶の開口端部に蓋を溶接して取り付けた。その後、蓋の電解液注入口から非水電解液(エチレンカーボネートとジエチルカーボネートを体積比3:7で混合した溶媒にビニレンカーボネートを3質量%の濃度で溶解させた溶液に、LiPF6を濃度1mol/lで溶解させたもの):3.6gを外装缶内に注入し、電解液注入口を封止して、図1に示す構造で、図2に示す外観の角形非水電解質二次電池を得た。
正極活物質であるLi1.00Ni0.89Co0.06Mn0.02Mg0.02Ba0.01O2で表されるリチウム含有複合酸化物:95質量部と、導電助剤であるケッチェンブラック:3質量部と、バインダであるVDF−CTFE:2質量部と、脱水NMPとを、プラネタリーミキサーで混合してスラリー(a)を調製した。また、正極活物質であるLiCoO2:95質量部と、導電助剤であるケッチェンブラック:3質量部と、バインダであるPVDF:2質量部と、脱水NMPとを、プラネタリーミキサーで混合してスラリー(b)を調製した。そして、前記のスラリー(a)とスラリー(b)とを、3:7の質量比で混合して、正極合剤層形成用スラリーを調製した。更に、この正極合剤層形成用スラリーを用いた以外は、実施例1と同様にして正極を作製した。
参考例1で作製したものと同じ負極を用いた以外は、実施例1と同様にして角形非水電解質二次電池を作製した。
正極活物質であるLi1.00Ni0.89Co0.06Mn0.02Mg0.02Ba0.01O2で表されるリチウム含有複合酸化物:95質量部と、導電助剤であるケッチェンブラック:3質量部と、バインダであるPVDF:2質量部と、脱水NMPとを、プラネタリーミキサーで混合して正極合剤層形成用スラリーを調製した。
正極活物質であるLi1.00Ni0.89Co0.06Mn0.02Mg0.02Ba0.01O2で表されるリチウム含有複合酸化物:95質量部と、導電助剤であるケッチェンブラック:3質量部と、バインダであるVDF−CTFE:2質量部と、脱水NMPとを、プラネタリーミキサーで混合して正極合剤層形成用スラリーを調製したが、粘度の経時変化が大きく、集電体に塗布するには不適であり、多数の正極(および電池)を製造するには生産性の点で不利であることが判明したため、それ以後の操作を実施しなかった。
比較例1で作製したものと同じ正極を用いた以外は、実施例1と同様にして角形非水電解質二次電池を作製した。
実施例、比較例および参考例の各電池を60℃で7時間保存した後、20℃で、定電流−定電圧充電(定電流:750mA、定電圧:4.2V、総充電時間:5時間)を行い、300mAの電流値で電池電圧が3Vに低下するまで放電する充放電サイクルを、放電容量が一定になるまで繰り返した。その後、各電池について、定電流−定電圧充電(定電流:750mA、定電圧:4.2V、総充電時間:5時間)を行い、1時間休止後に300mAの電流値で電池電圧が2.5Vになるまで放電して標準容量を求めた。なお、標準容量は各実施例、比較例、参考例とも100個の電池について測定し、その平均値を各実施例、比較例および参考例の電池の標準容量とした。
実施例、比較例および参考例の各電池について、定電流−定電圧充電(定電流:1500mA、定電圧:4.2V、総充電時間:2.5時間)で充電した後、1分休止後に1500mAの電流値で電池電圧が2.5Vになるまで放電する充放電サイクルを繰り返し、放電容量が初度の放電容量の80%に低下するまでのサイクル数を求めて、各電池の充電サイクル特性を評価した。なお、充放電サイクル特性における前記のサイクル数は、各実施例、比較例、参考例とも10個の電池について測定し、その平均値を各実施例、比較例および参考例の電池のサイクル数とした。
2 負極
3 セパレータ
Claims (5)
- 正極、負極、非水電解質およびセパレータを有する非水電解質二次電池であって、
前記正極は、正極活物質とバインダと導電助剤とを含有する正極合剤層を、集電体の片面または両面に有するものであり、
前記負極は、負極活物質とバインダとを含有する負極合剤層を、集電体の片面または両面に有するものであり、
前記負極活物質として、黒鉛と、SiO x (0.5≦x≦1.5)と炭素材料との複合体とを含有し、
前記正極のバインダとして、ポリフッ化ビニリデンと、フッ化ビニリデン−クロロトリフルオロエチレン共重合体とを含有していることを特徴とする非水電解質二次電池。 - 前記正極活物質として、下記一般組成式(1)
Li1+yMO2 (1)
〔前記一般組成式(1)中、−0.15≦y≦0.15であり、かつ、Mは、NiまたはNiを含む2種以上の元素群を表し、Mを構成する各元素中で、Niの割合(mol%)をaとしたときに、30≦a≦100である。〕
で表されるリチウム含有複合酸化物を含有する請求項1に記載の非水電解質二次電池。 - 正極活物質として、更にコバルト酸リチウムを含有する請求項2に記載の非水電解質二次電池。
- 正極合剤層中におけるポリフッ化ビニリデンとフッ化ビニリデン−クロロトリフルオロエチレン共重合体との合計を100質量%としたときの、フッ化ビニリデン−クロロトリフルオロエチレン共重合体の割合が30〜80質量%である請求項1〜3のいずれかに記載の非水電解質二次電池。
- フッ化ビニリデン−クロロトリフルオロエチレン共重合体におけるフッ化ビニリデン由来のユニットとクロロトリフルオロエチレン由来のユニットとの合計を100mol%としたとき、クロロトリフルオロエチレン由来のユニットの割合が0.5〜15mol%である請求項1〜4のいずれかに記載の非水電解質二次電池。
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