JP6775500B2 - 非水電解質電池およびその製造方法 - Google Patents
非水電解質電池およびその製造方法 Download PDFInfo
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- JP6775500B2 JP6775500B2 JP2017526466A JP2017526466A JP6775500B2 JP 6775500 B2 JP6775500 B2 JP 6775500B2 JP 2017526466 A JP2017526466 A JP 2017526466A JP 2017526466 A JP2017526466 A JP 2017526466A JP 6775500 B2 JP6775500 B2 JP 6775500B2
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- aqueous electrolyte
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- 150000001408 amides Chemical class 0.000 description 1
- XLJMAIOERFSOGZ-UHFFFAOYSA-N anhydrous cyanic acid Natural products OC#N XLJMAIOERFSOGZ-UHFFFAOYSA-N 0.000 description 1
- 239000003125 aqueous solvent Substances 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 150000001555 benzenes Chemical class 0.000 description 1
- NFMAZVUSKIJEIH-UHFFFAOYSA-N bis(sulfanylidene)iron Chemical compound S=[Fe]=S NFMAZVUSKIJEIH-UHFFFAOYSA-N 0.000 description 1
- 229910001593 boehmite Inorganic materials 0.000 description 1
- 125000001246 bromo group Chemical group Br* 0.000 description 1
- 125000000484 butyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- KVNRLNFWIYMESJ-UHFFFAOYSA-N butyronitrile Chemical compound CCCC#N KVNRLNFWIYMESJ-UHFFFAOYSA-N 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
- 229920002678 cellulose Polymers 0.000 description 1
- 239000001913 cellulose Substances 0.000 description 1
- 150000005678 chain carbonates Chemical class 0.000 description 1
- 125000001309 chloro group Chemical group Cl* 0.000 description 1
- 239000011651 chromium Substances 0.000 description 1
- 238000010280 constant potential charging Methods 0.000 description 1
- 238000010277 constant-current charging Methods 0.000 description 1
- 229920001577 copolymer Polymers 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 150000005676 cyclic carbonates Chemical class 0.000 description 1
- DFJYZCUIKPGCSG-UHFFFAOYSA-N decanedinitrile Chemical compound N#CCCCCCCCCC#N DFJYZCUIKPGCSG-UHFFFAOYSA-N 0.000 description 1
- KHEAWOWZPDLMMK-UHFFFAOYSA-N diethyl trimethylsilyl phosphate Chemical compound CCOP(=O)(OCC)O[Si](C)(C)C KHEAWOWZPDLMMK-UHFFFAOYSA-N 0.000 description 1
- ASMQGLCHMVWBQR-UHFFFAOYSA-M diphenyl phosphate Chemical compound C=1C=CC=CC=1OP(=O)([O-])OC1=CC=CC=C1 ASMQGLCHMVWBQR-UHFFFAOYSA-M 0.000 description 1
- 239000002270 dispersing agent Substances 0.000 description 1
- 150000002019 disulfides Chemical class 0.000 description 1
- AVQYXBDAZWIFTO-UHFFFAOYSA-N dodecanedinitrile Chemical compound N#CCCCCCCCCCCC#N AVQYXBDAZWIFTO-UHFFFAOYSA-N 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 238000000921 elemental analysis Methods 0.000 description 1
- 238000010828 elution Methods 0.000 description 1
- 239000003063 flame retardant Substances 0.000 description 1
- 125000003709 fluoroalkyl group Chemical group 0.000 description 1
- 238000007710 freezing Methods 0.000 description 1
- 230000008014 freezing Effects 0.000 description 1
- ZTOMUSMDRMJOTH-UHFFFAOYSA-N glutaronitrile Chemical compound N#CCCCC#N ZTOMUSMDRMJOTH-UHFFFAOYSA-N 0.000 description 1
- 125000005843 halogen group Chemical group 0.000 description 1
- 229920006015 heat resistant resin Polymers 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 1
- 150000003949 imides Chemical class 0.000 description 1
- 239000011256 inorganic filler Substances 0.000 description 1
- 229910003475 inorganic filler Inorganic materials 0.000 description 1
- 125000002346 iodo group Chemical group I* 0.000 description 1
- 229910000339 iron disulfide Inorganic materials 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- JRFPLINUXVVDIE-UHFFFAOYSA-N lithium acetic acid dihydrogen borate Chemical compound [Li+].CC(O)=O.CC(O)=O.CC(O)=O.CC(O)=O.OB(O)[O-] JRFPLINUXVVDIE-UHFFFAOYSA-N 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- SWAIALBIBWIKKQ-UHFFFAOYSA-N lithium titanium Chemical compound [Li].[Ti] SWAIALBIBWIKKQ-UHFFFAOYSA-N 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- CUONGYYJJVDODC-UHFFFAOYSA-N malononitrile Chemical compound N#CCC#N CUONGYYJJVDODC-UHFFFAOYSA-N 0.000 description 1
- 239000006262 metallic foam Substances 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- QLOAVXSYZAJECW-UHFFFAOYSA-N methane;molecular fluorine Chemical compound C.FF QLOAVXSYZAJECW-UHFFFAOYSA-N 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 125000002560 nitrile group Chemical group 0.000 description 1
- 150000002825 nitriles Chemical class 0.000 description 1
- LYGJENNIWJXYER-UHFFFAOYSA-N nitromethane Chemical compound C[N+]([O-])=O LYGJENNIWJXYER-UHFFFAOYSA-N 0.000 description 1
- QXOYPGTWWXJFDI-UHFFFAOYSA-N nonanedinitrile Chemical compound N#CCCCCCCCC#N QXOYPGTWWXJFDI-UHFFFAOYSA-N 0.000 description 1
- BTNXBLUGMAMSSH-UHFFFAOYSA-N octanedinitrile Chemical compound N#CCCCCCCC#N BTNXBLUGMAMSSH-UHFFFAOYSA-N 0.000 description 1
- 239000010450 olivine Substances 0.000 description 1
- 229910052609 olivine Inorganic materials 0.000 description 1
- 238000006864 oxidative decomposition reaction Methods 0.000 description 1
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 1
- 150000003016 phosphoric acids Chemical class 0.000 description 1
- 229920002647 polyamide Polymers 0.000 description 1
- 239000011116 polymethylpentene Substances 0.000 description 1
- 229920000306 polymethylpentene Polymers 0.000 description 1
- 239000001267 polyvinylpyrrolidone Substances 0.000 description 1
- 229920000036 polyvinylpyrrolidone Polymers 0.000 description 1
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- FVSKHRXBFJPNKK-UHFFFAOYSA-N propionitrile Chemical compound CCC#N FVSKHRXBFJPNKK-UHFFFAOYSA-N 0.000 description 1
- 125000001436 propyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- IAHFWCOBPZCAEA-UHFFFAOYSA-N succinonitrile Chemical compound N#CCCC#N IAHFWCOBPZCAEA-UHFFFAOYSA-N 0.000 description 1
- 150000003462 sulfoxides Chemical class 0.000 description 1
- 238000000427 thin-film deposition Methods 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- DQWPFSLDHJDLRL-UHFFFAOYSA-N triethyl phosphate Chemical compound CCOP(=O)(OCC)OCC DQWPFSLDHJDLRL-UHFFFAOYSA-N 0.000 description 1
- WVLBCYQITXONBZ-UHFFFAOYSA-N trimethyl phosphate Chemical compound COP(=O)(OC)OC WVLBCYQITXONBZ-UHFFFAOYSA-N 0.000 description 1
- ISIQQQYKUPBYSL-UHFFFAOYSA-N undecanedinitrile Chemical compound N#CCCCCCCCCCC#N ISIQQQYKUPBYSL-UHFFFAOYSA-N 0.000 description 1
- 238000004804 winding Methods 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
Images
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- H01M4/134—Electrodes based on metals, Si or alloys
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Description
非水電解質電池の第1の態様に係る負極には、Li(金属Li)、Li合金、Liと合金化可能な元素および前記元素を含む化合物よりなる群から選択される少なくとも1種の負極活物質を含有するものが使用され、例えば、前記金属や合金(化合物)で構成された箔をそのまま、または集電体の片面もしくは両面に貼り付けた構造の負極や、前記負極活物質を含有する負極合剤層を集電体の片面または両面に形成した構造の負極を使用することができる。
本発明の非水電解質電池の第2の態様では、特に車載用などのように高温環境下で使用される場合にあっても、高い貯蔵特性と高容量化とを実現することができ、また、ある程度の回数の充電が可能となるように、Li−Al合金を負極活物質として使用する。
正極は、リチウムイオンを吸蔵・放出可能な正極活物質と、導電助剤と、バインダとを含有する正極合剤を有するものであり、例えば、前記正極合剤からなる層(正極合剤層)を集電体の片面または両面に有する構造のものや、前記正極合剤の成形体が挙げられる。
非水電解質電池において、正極と負極とは、セパレータを介して重ねて構成した積層体(巻回などされず、例えば電池の外装体の扁平面に略平行に、正極と負極とがセパレータを介して重ねられた状態で配置される積層電極体)や、この積層体を渦巻状に巻回して形成された巻回体(巻回電極体)の形態で使用される。
セパレータは、80℃以上(より好ましくは100℃以上)170℃以下(より好ましくは150℃以下)において、その孔が閉塞する性質(すなわちシャットダウン機能)を有していることが好ましく、通常の非水電解質二次電池などで使用されているセパレータ、例えば、ポリエチレン(PE)やポリプロピレン(PP)などのポリオレフィン製の微多孔膜を用いることができる。セパレータを構成する微多孔膜は、例えば、PEのみを使用したものやPPのみを使用したものであってもよく、また、PE製の微多孔膜とPP製の微多孔膜との積層体であってもよい。セパレータの厚みは、例えば、10〜30μmであることが好ましい。
非水電解質電池は、例えば、積層電極体を外装体内に装填し、更に外装体内に非水電解質を注入して非水電解質中に電極体を浸漬させた後、外装体の開口部を封止することで製造される。外装体には、スチール製やアルミニウム製、アルミニウム合金製の外装缶や、金属を蒸着したラミネートフィルムで構成される外装体などを用いることができる。外装缶を有する電池としては、より具体的には、外装缶と封口板とをガスケットを介してカシメ封口したり、外装缶と封口板とを溶接して封口したりする電池ケースを有する扁平形(コイン形、ボタン形を含む);有底筒形(円筒形、角筒形など)の外装缶の開口部に蓋体を配し、ガスケットを介してカシメ封口したり、外装缶と蓋体とを溶接して封口したりする筒形;などが挙げられる。
実施例1
厚みが40μmのNi箔の両面に、それぞれ、厚さ30μmのAl箔を積層した25mm×37mmの大きさのクラッド材(積層金属箔)を用意し、前記クラッド材の端部に、集電用のCu箔を超音波溶接し、更にそのCu箔の端部に、電池外部との導電接続のためのNiタブを超音波溶接したものを、負極を形成するための負極前駆体として電池の組み立てに用いた。
非水電解液中のリン酸トリス(トリメチルシリル)の添加量を2質量%とした以外は、実施例1と同様にして非水電解質二次電池を作製した。
非水電解液中のリン酸トリス(トリメチルシリル)の添加量を5質量%とした以外は、実施例1と同様にして非水電解質二次電池を作製した。
非水電解液中のリン酸トリス(トリメチルシリル)の添加量を8質量%とした以外は、実施例1と同様にして非水電解質二次電池を作製した。
非水電解液の混合溶媒として、ECとMECとの体積比1:2の混合溶媒を用いた以外は、実施例1と同様にして非水電解質二次電池を作製した。
非水電解液にリン酸トリス(トリメチルシリル)を添加せず、アジポニトリル:3質量%とγ−ブチロラクトン:0.5質量%のみを添加した非水電解液を用いた以外は、実施例1と同様にして非水電解質二次電池を作製した。
非水電解液中のリン酸トリス(トリメチルシリル)の添加量を10質量%とした以外は、実施例1と同様にして非水電解質二次電池を作製した。
リン酸トリス(トリメチルシリル)、アジポニトリルおよびγ−ブチロラクトンを添加せず、PCとMECとの体積比1:2の混合溶媒に、LiBF4を1.2mol/lの濃度で溶解させただけの非水電解液を調製した。前記電解液を用いた以外は、実施例1と同様にして非水電解質二次電池を作製した。
平均粒径が20μmの人造黒鉛と、スチレンブタジエンゴムと、カルボキシメチルセルロースとを有する負極合剤層をCu集電箔上に形成し、黒鉛系の負極活物質を有する負極を作製した。前記負極を用いた以外は、実施例5と同様にして非水電解質二次電池を作製した。
実施例1〜7および比較例1、2の各電池について、定電流(4mA)−定電圧(4.0V)充電を行い、充電電流が0.2mAまで低下した時点で充電を終止して初期充電容量を測定した。この充電により、負極前駆体のAlはLi−Al合金に変化した。次いで、充電後の各電池を、4mAの定電流で放電(放電終止電圧:2V)させて、初期放電容量を測定した。そして、各電池について、初期放電容量を初期充電容量で除した値を百分率で表して、初期充放電効率を算出した。
実施例1〜7および比較例1、2の各電池(ただし、初期充放電効率測定に用いたのとは別の電池)について、定電流(4mA)−定電圧(4.0V)充電を行い、充電電流が0.2mAまで低下した時点で充電を終止した。次いで、充電後の各電池を、4mAの定電流で放電(放電終止電圧:2V)させた。
厚みが40μmのNi箔の両面に、それぞれ、厚さ30μmのAl箔を積層した160mm×25mmの大きさのクラッド材(積層金属箔)とした以外は実施例1と同様にして、負極を形成するための負極前駆体として電池の組み立てに用いた。
実施例8の電池について、定電流(16.4mA)−定電圧(4.0V)充電を行い、充電電流が0.82mAまで低下した時点で充電を終止して初期充電容量を測定した。この充電により、負極前駆体のAlはLi−Al合金に変化した。次いで、充電後の各電池を、16.4mAの定電流で放電(放電終止電圧:2V)させて、初期放電容量を測定した。そして、各電池について、初期放電容量を初期充電容量で除した値を百分率で表して、初期充放電効率を算出した。
実施例8の電池(ただし、初期充放電効率測定に用いたのとは別の電池)について、定電流(16.4mA)−定電圧(4.0V)充電を行い、充電電流が0.82mAまで低下した時点で充電を終止した。次いで、充電後の各電池を、16.4mAの定電流で放電(放電終止電圧:2V)させた。
実施例9
厚さ30μmのNi箔の両面に、それぞれ、厚さ30μmのAl箔を積層した25mm×40mmの大きさのクラッド材(積層金属箔)を負極前駆体として用いた。前記クラッド材の端部に、集電用のCu箔を超音波溶接し、更にそのCu箔の端部に、電池外部との導電接続のためのNiタブを超音波溶接したものを電池の組み立てに用いた。
厚さ30μmのCu箔の両面に、それぞれ、厚さ30μmのAl箔を積層した25mm×40mmの大きさのクラッド材(積層金属箔)を負極前駆体として用いた以外は、実施例9と同様にして、定格容量30mAhの非水電解液電池を作製した。
厚さ30μmのNi箔の片面に、厚さ30μmのAl箔を積層した25mm×40mmの大きさのクラッド材(積層金属箔)を負極前駆体として用いた。前記クラッド材の端部に、集電用のCu箔を超音波溶接し、更にそのCu箔の端部に、電池外部との導電接続のためのNiタブを超音波溶接したものを電池の組み立てに用いた。
アジポニトリルの含有量を0.9質量%に変更した以外は実施例9と同様にして非水電解液を調製し、この非水電解液を用いた以外は実施例9と同様にして非水電解液電池を作製した。
γ−ブチロラクトンを0.5質量%となる量で添加した以外は実施例9と同様にして非水電解液を調製し、この非水電解液を用いた以外は実施例9と同様にして非水電解液電池を作製した。
PCに変えてエチレンカーボネートを用いた以外は実施例9と同様にして非水電解液を調製し、この非水電解液を用いた以外は実施例9と同様にして非水電解液電池を作製した。
アジポニトリルを添加しなかった以外は実施例9と同様にして非水電解液を調製し、この非水電解液を用いた以外は実施例9と同様にして非水電解液電池を作製した。
LiBF4に代えてLiPF6を用いた以外は実施例9と同様にして非水電解液を調製し、この非水電解液を用いた以外は実施例9と同様にして非水電解液電池を作製した。
実施例9〜13および比較例3〜5の各電池をアルゴンガス雰囲気中で分解して負極を取り出し、その変形の程度を目視で確認した。なお、いずれの負極についても、クラッド材を構成するAl箔の正極合剤層と対向する部分にLi−Al合金が形成されており、周縁部の正極合剤層と対向していない部分は、Liと反応せずAlのままの状態で存在していた。
実施例9〜13および比較例3〜5の各電池について、定電流(6mA)−定電圧(4.0V)充電を行い、充電電流が0.3mAまで低下した時点で充電を終止した。次いで、6mAの定電流で放電(放電終止電圧:2V)させて放電容量(初期放電容量)を測定し、更に、前記充電条件で充電を行って電池を満充電状態とした。
2 ラミネートフィルム外装体
5 正極
6 負極
7 セパレータ
100 負極前駆体
101 積層金属箔
101a 金属基材層
101b Al金属層
102 Li箔
Claims (7)
- 前記非水電解質は、トリメチルシリル基を分子内に有するリン酸化合物を含有している請求項1に記載の非水電解質電池。
- 前記非水電解質は、プロピレンカーボネートを全溶媒中で10体積%以上含有している請求項1または2に記載の非水電解質電池。
- 前記非水電解質は、更にニトリル化合物を含有している請求項1〜3のいずれかに記載の非水電解質電池。
- 前記非水電解質は、更にラクトン環を有する化合物を含有している請求項1〜4のいずれかに記載の非水電解質電池。
- 請求項1〜5のいずれかに記載の非水電解質電池を製造する方法であって、
前記一般式(1)で表される基を分子内に有するリン酸化合物を8質量%以下の範囲で含有する非水電解質を用いることを特徴とする非水電解質電池の製造方法。 - 前記一般式(1)で表される基を分子内に有するリン酸化合物の、前記非水電解質における含有量が、0.1質量%以上である請求項6に記載の非水電解質電池の製造方法。
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DE102017110570A1 (de) * | 2017-04-28 | 2018-10-31 | Huf Hülsbeck & Fürst Gmbh & Co. Kg | Reifendrucküberwachungseinheit |
WO2019031117A1 (ja) * | 2017-08-09 | 2019-02-14 | マクセルホールディングス株式会社 | 非水電解液電池 |
WO2019102883A1 (ja) * | 2017-11-21 | 2019-05-31 | マクセルホールディングス株式会社 | 非水電解質電池 |
JP2019175786A (ja) * | 2018-03-29 | 2019-10-10 | マクセルホールディングス株式会社 | 非水電解液電池 |
JP7007615B2 (ja) | 2018-04-27 | 2022-01-24 | ダイキン工業株式会社 | 電解液、電気化学デバイス、リチウムイオン二次電池及びモジュール |
US20210234201A1 (en) * | 2018-05-14 | 2021-07-29 | Daikin Industries, Ltd. | Electrolytic solution, electrochemical device, lithium-ion secondary battery, and module |
JP7337515B2 (ja) * | 2019-03-11 | 2023-09-04 | マクセル株式会社 | 非水電解液電池 |
JP7145467B2 (ja) * | 2019-03-20 | 2022-10-03 | パナソニックIpマネジメント株式会社 | リチウム一次電池 |
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WO2022196266A1 (ja) * | 2021-03-19 | 2022-09-22 | 株式会社村田製作所 | 二次電池 |
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