JP2022141404A - 非水電解液二次電池 - Google Patents
非水電解液二次電池 Download PDFInfo
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- 239000011255 nonaqueous electrolyte Substances 0.000 title claims abstract description 44
- 239000007773 negative electrode material Substances 0.000 claims abstract description 68
- 238000004949 mass spectrometry Methods 0.000 claims abstract description 12
- 238000012621 laser-ablation inductively coupled plasma technique Methods 0.000 claims abstract description 11
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims abstract description 9
- 229910001416 lithium ion Inorganic materials 0.000 claims description 32
- 239000011230 binding agent Substances 0.000 claims description 30
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- 239000008112 carboxymethyl-cellulose Substances 0.000 claims description 13
- 150000003839 salts Chemical class 0.000 claims description 12
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 11
- 229920005822 acrylic binder Polymers 0.000 claims description 11
- 229910052744 lithium Inorganic materials 0.000 claims description 11
- 238000009826 distribution Methods 0.000 claims description 5
- 150000001768 cations Chemical class 0.000 claims description 3
- 230000008021 deposition Effects 0.000 abstract description 14
- RBYFNZOIUUXJQD-UHFFFAOYSA-J tetralithium oxalate Chemical compound [Li+].[Li+].[Li+].[Li+].[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O RBYFNZOIUUXJQD-UHFFFAOYSA-J 0.000 abstract 2
- 239000010410 layer Substances 0.000 description 81
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 31
- 229910052751 metal Inorganic materials 0.000 description 17
- 239000002184 metal Substances 0.000 description 17
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 12
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 11
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- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 description 10
- 238000000034 method Methods 0.000 description 10
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- 239000012535 impurity Substances 0.000 description 8
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- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 7
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- DSMUTQTWFHVVGQ-UHFFFAOYSA-N 4,5-difluoro-1,3-dioxolan-2-one Chemical compound FC1OC(=O)OC1F DSMUTQTWFHVVGQ-UHFFFAOYSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 2
- 229910001228 Li[Ni1/3Co1/3Mn1/3]O2 (NCM 111) Inorganic materials 0.000 description 2
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 2
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
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- 238000005406 washing Methods 0.000 description 2
- JIUHVFMKOJAZDA-UHFFFAOYSA-N 1,1,2-trifluoroethyl hydrogen carbonate Chemical compound OC(=O)OC(F)(F)CF JIUHVFMKOJAZDA-UHFFFAOYSA-N 0.000 description 1
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- 229910013063 LiBF 4 Inorganic materials 0.000 description 1
- 229910013684 LiClO 4 Inorganic materials 0.000 description 1
- 229910032387 LiCoO2 Inorganic materials 0.000 description 1
- 229910010584 LiFeO2 Inorganic materials 0.000 description 1
- 229910052493 LiFePO4 Inorganic materials 0.000 description 1
- 229910014778 LiMn2O 4 Inorganic materials 0.000 description 1
- 229910002099 LiNi0.5Mn1.5O4 Inorganic materials 0.000 description 1
- 229910003005 LiNiO2 Inorganic materials 0.000 description 1
- 240000007594 Oryza sativa Species 0.000 description 1
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- 230000004913 activation Effects 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 229910001593 boehmite Inorganic materials 0.000 description 1
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- 150000002148 esters Chemical class 0.000 description 1
- 150000002170 ethers Chemical class 0.000 description 1
- 229910021385 hard carbon Inorganic materials 0.000 description 1
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 1
- 150000002596 lactones Chemical class 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910021437 lithium-transition metal oxide Inorganic materials 0.000 description 1
- 239000000395 magnesium oxide Substances 0.000 description 1
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- 239000007769 metal material Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
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- 150000002825 nitriles Chemical class 0.000 description 1
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- 125000002467 phosphate group Chemical class [H]OP(=O)(O[H])O[*] 0.000 description 1
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- 239000000377 silicon dioxide Substances 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 229910001415 sodium ion Inorganic materials 0.000 description 1
- 159000000000 sodium salts Chemical class 0.000 description 1
- RPACBEVZENYWOL-XFULWGLBSA-M sodium;(2r)-2-[6-(4-chlorophenoxy)hexyl]oxirane-2-carboxylate Chemical compound [Na+].C=1C=C(Cl)C=CC=1OCCCCCC[C@]1(C(=O)[O-])CO1 RPACBEVZENYWOL-XFULWGLBSA-M 0.000 description 1
- 229910021384 soft carbon Inorganic materials 0.000 description 1
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- 150000003457 sulfones Chemical class 0.000 description 1
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- 229910052723 transition metal Inorganic materials 0.000 description 1
- 229910000319 transition metal phosphate Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
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- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
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- H01M10/0563—Liquid materials, e.g. for Li-SOCl2 cells
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- H01M10/058—Construction or manufacture
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Abstract
Description
バインダAとして、NaOHを中和剤として用いて合成したスチレンブタジエンゴム(SBR)を用意した。また、Na含有量が小さいバインダBとして、LiOHを中和剤として用いて合成したスチレンブタジエンゴムを用意した。
正極活物質としてのLiNi1/3Co1/3Mn1/3O2(LNCM)と、導電材としてのアセチレンブラック(AB)と、バインダとしてのポリフッ化ビニリデン(PVdF)とを、LNCM:AB:PVdF=90:8:2の質量比でN-メチルピロリドン(NMP)と混合し、正極活物質層形成用スラリーを調製した。このスラリーを、長尺状のアルミニウム箔の両面に帯状に塗布して乾燥した後、プレスすることによりNa含有量の多い正極シートAを作製した。
Na含有量の異なる2種類のセパレータシートを用意した。具体的には、PP/PE/PPの三層構造の多孔質ポリオレフィンシートにHRLが設けられたものを、Na含有量の多いセパレータシートAとして用意した。また、このセパレータシートAをECとDMCとEMCとをEC:DMC:EMC=3:3:4の体積比で含む混合溶媒を用いて30分間洗浄したものを、Na含有量の少ないセパレータシートBとして用意した。
上記で作製した正極シートと、負極シートと、2枚の上記用意したセパレータシートとを積層し、捲回した後、側面方向から押圧して拉げさせることによって扁平形状の捲回電極体を作製した。使用した各部材のNa含有量を表1に示す。
正極活物質層中のNa含有量、負極活物質層中のNa含有量、およびセパレータ中のNa含有量の合計に対する、負極活物質層中のNa含有量の割合を、上記レーザーアブレーションICP質量分析の結果を用いて算出した。
作製した各評価用リチウムイオン二次電池を、開回路電圧が3.0Vとなるまで放電させてからドライ環境のグローブボックス内で解体し、捲回型電極体を取り出した。次に、捲回型電極体の負極の最内周の適切な大きさで切り出し、EMC中に10分程度浸漬して洗浄して、抵抗測定用の試験体とした。そしてこの試験体に形成された負極活物質層の表面の反応抵抗を、負極活物質層の幅方向に沿って、交流インピーダンス法により測定した。交流インピーダンス法による抵抗測定は、特開2014-25850号公報に開示される手法に従って実施した。このとき負極活物質層の端部から30%までの部分は5mm間隔で、中央部(残りの40%の部分)は2mm間隔で抵抗値を求めた。
各評価用リチウムイオン二次電池をSOC60%に調整した。これを-10℃の環境下に置き、10秒間放電した。放電電流レートは1C、3C、5C、10Cとし、各電流レートで放電した後の電圧を測定した。電流レートおよび電圧よりIV抵抗を算出し、その平均値を電池抵抗とした。比較例1のリチウムイオン二次電池の抵抗を「100」とした場合のその他の電池の抵抗の比を算出した。結果を表1に示す。
各評価用リチウムイオン二次電池を、-10℃の環境下に置き、所定の電流値で、5秒間充電、10分間休止、5秒間放電、10分間休止を1サイクルとする充放電サイクルを1000サイクル実施した。その後、各リチウムイオン二次電池を解体し、負極上での金属リチウムの析出の有無を確認した。負極上での金属リチウムの析出が確認されなかった電流値のうち、最大の電流値を限界電流値とした。比較例1のリチウムイオン二次電池の限界電流値を「100」としたときの、その他のリチウムイオン二次電池の限界電流値の比を求めた。結果を表1に示す。
30 電池ケース
36 安全弁
42 正極端子
42a 正極集電板
44 負極端子
44a 負極集電板
50 正極シート(正極)
52 正極集電体
52a 正極活物質層非形成部分
54 正極活物質層
60 負極シート(負極)
62 負極集電体
62a 負極活物質層非形成部分
64 負極活物質層
70 セパレータシート(セパレータ)
80 非水電解液
100 リチウムイオン二次電池
Claims (6)
- 正極と、負極と、セパレータと、を含む電極体、および
非水電解液、
を備える非水電解液二次電池であって、
前記負極は、負極活物質層を備え、
前記非水電解液は、リチウムビス(オキサラト)ボレートを含有し、
レーザーアブレーションICP質量分析によって求まる前記負極活物質層中のNa含有量が、311μg/g以下である、
非水電解液二次電池。 - 前記正極は、正極活物質層を備え、
前記正極活物質層中のNa含有量、前記負極活物質層中のNa含有量、および前記セパレータ中のNa含有量の合計に対する、前記負極活物質層中のNa含有量の割合(%)が、33%以下である、請求項1に記載の非水電解液二次電池。 - 前記負極活物質層の主面の短辺方向に沿って抵抗分布測定を行った際に、抵抗が最も低い箇所における抵抗値に対する、抵抗が最も高い箇所の抵抗値の割合が、1.10以下である、請求項1または2に記載の非水電解液二次電池。
- 前記負極活物質層は、負極活物質と、バインダと、増粘剤と、を含有し、
前記増粘剤が、カルボキシメチルセルロース塩であり、前記カルボキシメチルセルロース塩の少なくとも一部のカチオンが、Liイオンである、請求項1~3のいずれか1項に記載の非水電解液二次電池。 - 前記負極活物質層は、負極活物質と、Naを含有しないアクリル系バインダと、を含有する、請求項1~4のいずれか1項に記載の非水電解液二次電池。
- 前記電極体が、捲回電極体である、請求項1~5のいずれか1項に記載の非水電解液二次電池。
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Citations (6)
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JPH10154513A (ja) * | 1996-11-25 | 1998-06-09 | Sanyo Electric Co Ltd | 非水電解液電池 |
JP2000082472A (ja) * | 1998-09-03 | 2000-03-21 | Dai Ichi Kogyo Seiyaku Co Ltd | 非水電池用電極 |
JP2015011969A (ja) * | 2013-07-02 | 2015-01-19 | トヨタ自動車株式会社 | 非水電解液二次電池及びその製造方法 |
JP2016058153A (ja) * | 2014-09-05 | 2016-04-21 | トヨタ自動車株式会社 | リチウムイオン電池 |
KR20190106637A (ko) * | 2018-03-09 | 2019-09-18 | 주식회사 엘지화학 | 리튬 이차전지 |
JP2020071944A (ja) * | 2018-10-30 | 2020-05-07 | トヨタ自動車株式会社 | 非水電解液リチウムイオン二次電池 |
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JPH10154513A (ja) * | 1996-11-25 | 1998-06-09 | Sanyo Electric Co Ltd | 非水電解液電池 |
JP2000082472A (ja) * | 1998-09-03 | 2000-03-21 | Dai Ichi Kogyo Seiyaku Co Ltd | 非水電池用電極 |
JP2015011969A (ja) * | 2013-07-02 | 2015-01-19 | トヨタ自動車株式会社 | 非水電解液二次電池及びその製造方法 |
JP2016058153A (ja) * | 2014-09-05 | 2016-04-21 | トヨタ自動車株式会社 | リチウムイオン電池 |
KR20190106637A (ko) * | 2018-03-09 | 2019-09-18 | 주식회사 엘지화학 | 리튬 이차전지 |
JP2020071944A (ja) * | 2018-10-30 | 2020-05-07 | トヨタ自動車株式会社 | 非水電解液リチウムイオン二次電池 |
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