JP2023550168A - 複合セパレーター、電気化学エネルギー貯蔵装置及び電気装置 - Google Patents
複合セパレーター、電気化学エネルギー貯蔵装置及び電気装置 Download PDFInfo
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- JP2023550168A JP2023550168A JP2023530920A JP2023530920A JP2023550168A JP 2023550168 A JP2023550168 A JP 2023550168A JP 2023530920 A JP2023530920 A JP 2023530920A JP 2023530920 A JP2023530920 A JP 2023530920A JP 2023550168 A JP2023550168 A JP 2023550168A
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- NDPGDHBNXZOBJS-UHFFFAOYSA-N aluminum lithium cobalt(2+) nickel(2+) oxygen(2-) Chemical compound [Li+].[O--].[O--].[O--].[O--].[Al+3].[Co++].[Ni++] NDPGDHBNXZOBJS-UHFFFAOYSA-N 0.000 description 1
- 230000000712 assembly Effects 0.000 description 1
- 238000000429 assembly Methods 0.000 description 1
- 229910001593 boehmite Inorganic materials 0.000 description 1
- OBNCKNCVKJNDBV-UHFFFAOYSA-N butanoic acid ethyl ester Natural products CCCC(=O)OCC OBNCKNCVKJNDBV-UHFFFAOYSA-N 0.000 description 1
- PWLNAUNEAKQYLH-UHFFFAOYSA-N butyric acid octyl ester Natural products CCCCCCCCOC(=O)CCC PWLNAUNEAKQYLH-UHFFFAOYSA-N 0.000 description 1
- 150000007942 carboxylates Chemical class 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000010835 comparative analysis Methods 0.000 description 1
- 238000010280 constant potential charging Methods 0.000 description 1
- 238000010277 constant-current charging Methods 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 229940093499 ethyl acetate Drugs 0.000 description 1
- CYEDOLFRAIXARV-UHFFFAOYSA-N ethyl propyl carbonate Chemical compound CCCOC(=O)OCC CYEDOLFRAIXARV-UHFFFAOYSA-N 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- 229910021385 hard carbon Inorganic materials 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 1
- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 description 1
- 229910000625 lithium cobalt oxide Inorganic materials 0.000 description 1
- 229910002102 lithium manganese oxide Inorganic materials 0.000 description 1
- FRMOHNDAXZZWQI-UHFFFAOYSA-N lithium manganese(2+) nickel(2+) oxygen(2-) Chemical compound [O-2].[Mn+2].[Ni+2].[Li+] FRMOHNDAXZZWQI-UHFFFAOYSA-N 0.000 description 1
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 1
- 229910001486 lithium perchlorate Inorganic materials 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 description 1
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 description 1
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 description 1
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 description 1
- VLXXBCXTUVRROQ-UHFFFAOYSA-N lithium;oxido-oxo-(oxomanganiooxy)manganese Chemical compound [Li+].[O-][Mn](=O)O[Mn]=O VLXXBCXTUVRROQ-UHFFFAOYSA-N 0.000 description 1
- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical compound [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 description 1
- MCVFFRWZNYZUIJ-UHFFFAOYSA-M lithium;trifluoromethanesulfonate Chemical compound [Li+].[O-]S(=O)(=O)C(F)(F)F MCVFFRWZNYZUIJ-UHFFFAOYSA-M 0.000 description 1
- 229940017219 methyl propionate Drugs 0.000 description 1
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-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
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 description 1
- UUIQMZJEGPQKFD-UHFFFAOYSA-N n-butyric acid methyl ester Natural products CCCC(=O)OC UUIQMZJEGPQKFD-UHFFFAOYSA-N 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 150000003013 phosphoric acid derivatives Chemical class 0.000 description 1
- 229920001495 poly(sodium acrylate) polymer Polymers 0.000 description 1
- 229920002961 polybutylene succinate Polymers 0.000 description 1
- 239000004631 polybutylene succinate Substances 0.000 description 1
- 229920001721 polyimide Polymers 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 229940090181 propyl acetate Drugs 0.000 description 1
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 229910052814 silicon oxide Inorganic materials 0.000 description 1
- 239000002210 silicon-based material Substances 0.000 description 1
- 239000002153 silicon-carbon composite material Substances 0.000 description 1
- NNMHYFLPFNGQFZ-UHFFFAOYSA-M sodium polyacrylate Chemical compound [Na+].[O-]C(=O)C=C NNMHYFLPFNGQFZ-UHFFFAOYSA-M 0.000 description 1
- 229910021384 soft carbon Inorganic materials 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
- 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 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
- 239000011366 tin-based material Substances 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 230000004222 uncontrolled growth Effects 0.000 description 1
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 description 1
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Abstract
【選択図】図1
Description
本願は、2021年9月29日に出願された発明の名称が「複合セパレーター、電気化学エネルギー貯蔵装置及び電気装置」である中国特許出願第202111150172.3号の優先権を主張するものであり、当該出願は、参照によりその全体が本明細書に組み込まれる。
5 二次電池;51 ケース;52 電極アセンブリ;53 蓋板
6 第1のベース膜;7 アノード保護層;71 第1のサブ層;72 第2のサブ層
8 第2のベース膜;9 安定性塗層
式1において、Mは、第1の酸化物に対応する第1の単体である。これらの実施例において、第1の酸化物ナノ粒子のナノサイズの電気化学駆動特性により第1の酸化物ナノ粒子の電気化学反応性能を向上させるため、式1の置換反応が効率的に行うことができる。
電解質は、正極シートと負極シートの間でイオンを伝導する役割を果たす。本願において、電解質の種類は、具体的な制限がなく、必要に応じて選択することができる。例えば、電解質は、液体、ゲル状、または、全固体であってもよい。
実施例
アノード保護層スラリーの調製
攪拌装置に下記の表1に示す実施例1のスラリー配合の各成分物質を添加し、かつ均一に攪拌してスラリーを得た。実施例1のスラリーは、イオン水100部、分散剤であるアリールフェニルポリオキシエチレンエーテル界面活性剤0.4部、増粘剤であるカルボキシメチルセルロースナトリウム0.5部、バインダーである水性アクリレートエマルジョン2部、錯化剤であるエチレンジアミン四酢酸四ナトリウム5部を含んだ。
多孔質ポリエチレン(PE)膜を用いて第1のベース膜と第2のベース膜を作製し、第1のベース膜の厚さは、第2のベース膜の厚さと同じ、第1のベース膜と第2のベース膜の厚さの合計は、14μmであり、単一の第1のベース膜又は単一の第2のベース膜の厚さは、7μmであった。
負極活性物質である人工黒鉛、バインダーであるスチレンブタジエンゴム(SBR)、増粘剤であるカルボキシメチルセルロースナトリウム(CMC-Na)及び導電剤であるカーボンブラック(Super P)を重量比96.2:1.8:1.2:0.8で適量な溶媒である脱イオン水に十分に攪拌混合して均一な負極スラリーを形成し、得られた負極スラリーを負極集電体である銅箔の面に均一に塗り、乾燥、冷間圧延、トリミング、カット、ストリップを経って負極シートを得た。
正極活性材であるLiNi0.8Co0.1Mn0.1O2(NCM811)、導電剤であるカーボンナノチューブ(CNT)、導電剤であるカーボンブラック(Super P)、バインダーであるポリフッ化ビニリデン(PVDF)を重量比96.9:0.3:1.7:1.0で適量な溶媒であるNMPに十分に攪拌混合して均一な正極スラリーを形成し、得られた正極スラリーを正極集電体であるアルミニウム箔の面に均一に塗り、乾燥、冷間圧延、トリミング、カット、ストリップを経って正極シートを得た。
基礎電解液を調製し、基礎電解液は、炭酸ジメチル(DMC)、炭酸メチルエチル(EMC)及び炭酸エチレン(EC)を含み、3者の質量比は、5:2:3であった。そして電解液におけるヘキサフルオロリン酸リチウムの濃度が1mol/Lになるように電解質塩を加えた。
前述して得られた正極シート、複合セパレーター及び負極シートを順に積層し、かつ巻き取って電極アセンブリを得、電極アセンブリを外装に入れ、上記電解液を添加し、封止、静置、化成、エージング等の工程を経った後、二次電池を得た。
実施例2~実施例15の二次電池の製造方法は、実施例1の二次電池の製造方法と類似し、ただし、アノード保護層スラリーの配合及び複合セパレーターの構造パラメーターを調整し、各実施例のアノード保護層スラリーの配合の詳細を表1に示し、各実施例の複合セパレーターの構造パラメーターの詳細を表2に示した。
アノード保護層スラリーの調製
第1の攪拌装置に下記の表1に示す実施例16の第1のサブ層スラリー配合の各成分物質を加え、かつ均一に攪拌して第1のサブ層を製造するためのスラリーを得た。実施例16の第1のサブ層スラリーは、イオン水100部、分散剤であるアリールフェニルポリオキシエチレンエーテル界面活性剤0.8部、増粘剤であるカルボキシメチルセルロースナトリウム0.5部、バインダーである水性アクリレートエマルジョン2部、錯化剤であるエチレンジアミン四酢酸四ナトリウム5部を含んだ。
多孔質ポリエチレン(PE)膜を用いて第1のベース膜及び第2のベース膜を作製し、第1のベース膜の厚さは、第2のベース膜の厚さと同じ、第1のベース膜と第2のベース膜の厚さの合計は、14μmであり、単一の第1のベース膜又は単一の第2のベース膜の厚さは、7μmであった。
前述して得られた正極シート、複合セパレーター及び負極シートを順に積層し、かつ巻き取って電極アセンブリを得、そのうち、第1のサブ層は、第2のサブ層に比べて正極シート(カソードシート)のより近くに配置され、則ち、第1のベース膜は、正極シートと接触しているように配置され、第2のベース膜は、負極シートと接触しているように配置されていた。前述して得られた電極アセンブリを外装に入れ、上記電解液を添加し、封止、静置、化成、エージング等の工程を経った後、二次電池を得た。
実施例17~実施例21の二次電池は、製造方法が実施例16の二次電池と類似し、ただし、アノード保護層スラリーの配合及び複合セパレーターの構造パラメーターを調整し、各実施例のアノード保護層スラリーの配合の詳細を表1に示し、各実施例の複合セパレーターの構造パラメーターの詳細を表2に示した。
比較例1の二次電池の製造方法は、実施例1の二次電池と類似するが、アノード保護層スラリーの調製を有しないことに相違し、また、第1のベース膜と第2のベース膜の間にアノード保護層を設けず、セパレーター製造過程中に接着剤を用いて第1のベース膜と第2のベース膜を直接に接着した。
比較例2の二次電池の製造方法は、実施例1の二次電池と類似するが、セパレーターの製造過程中、二層のベース膜の間に1つのアノード保護層を挟む形態を採用せず、アノード保護層スラリーを単一のベース膜上に塗布してアノード保護層を形成した。
式において、Tはセパレーターの熱収縮率、単位が%であり、Lは加熱前の長さ、単位がmmであり、Lは加熱後の長さ、単位がmmである。
式において、Tはセパレーターの熱収縮率、単位が%であり、L 1 は加熱前の長さ、単位がmmであり、L 2 は加熱後の長さ、単位がmmである。
Claims (12)
- 第1のベース膜、第2のベース膜およびアノード保護層を含む複合セパレーターであって、前記アノード保護層は、前記複合セパレーターの厚さ方向に前記第1のベース膜と前記第2のベース膜の間に位置し、前記アノード保護層は、遷移金属イオンを捕捉するために用いられる、複合セパレーター。
- 前記アノード保護層は、錯化剤を含み、
前記錯化剤は、リン酸系錯化剤、ヒドロキシカルボン酸塩系錯化剤及びアミノカルボン酸塩系錯化剤から選ばれた少なくとも1種であり、
任意に、前記錯化剤は、ヒドロキシエチリデンジホスホン酸二ナトリウム,エチレンジアミン四酢酸二ナトリウム,エチレンジアミン四酢酸四ナトリウム,ヒドロキシエチルエチレンジアミン三酢酸,ジエチレントリアミン五酢酸,クエン酸,カルボキシメチル酒石酸,カルボキシメチルオキソコハク酸,1,2,3,4-シクロペンタンテトラカルボン酸及びアミノトリリン酸ナトリウムから選ばれた少なくとも1種である、請求項1に記載の複合セパレーター。 - 前記アノード保護層の厚さ範囲は、0.5μm~8μmであり、
任意に、前記アノード保護層の厚さ範囲は3μm~5μmであり、
任意に、前記アノード保護層の厚さ範囲は4μm~5μmである、請求項1または2に記載の複合セパレーター。 - 前記アノード保護層は、さらに、リチウムデンドライトの成長を遮断するために用いられる、請求項1~3のいずれに記載の複合セパレーター。
- 前記アノード保護層は、金属リチウムと置換反応して酸化リチウム及び第1の単体物を生成する第1の酸化物ナノ粒子をさらに含む、請求項1~4のいずれに記載の複合セパレーター。
- 前記アノード保護層は、前記錯化剤と前記第1の酸化物ナノ粒子を含む混合層であり、そのうち、前記錯化剤と前記第1の酸化物ナノ粒子との重量比は、0.06~0.13であり、
任意に、前記アノード保護層的厚さ範囲は、1μm~11μm;
任意に、前記アノード保護層的厚さ範囲は、2.5μm~9μmである、請求項5に記載の複合セパレーター。 - 前記アノード保護層は、第1のサブ層と第2のサブ層を含み、
前記錯化剤は、第1のサブ層に分布しており、前記第1のサブ層は、遷移金属イオンを捕捉するために用いられ、
第2のサブ層は、前記第1のサブ層と積層するように設けられ、前記第1の酸化物ナノ粒子は前記第2のサブ層に分布されている、請求項5又は6に記載の複合セパレーター。 - 前記アノード保護層の厚さ範囲は、1μm~11μmであり、
任意に、前記前記アノード保護層の厚さ範囲は、2.5μm~9μmであり、
任意に、前記第1のサブ層の厚さと前記第2のサブ層の厚さとの比は、1:2~4であり、
任意に、前記第1のサブ層の厚さ範囲は、0.3μm~3.5μmであり、前記第2のサブ層の厚さ範囲は、0.6μm~7μmである、請求項7に記載の複合セパレーター。 - 前記第1の酸化物ナノ粒子は、ケイ素、ジルコニウム、チタン、カドミウム、マンガン、鉄、コバルト、ニッケル、アルミニウム及び銅のうちの少なくとも1種の酸化物ナノ粒子を含み、
任意に、前記第1の酸化物ナノ粒子の粒子径範囲は、1nm~50nmであり、
任意に、前記第1の酸化物ナノ粒子の粒子径範囲は、1nm~10nmである、請求項5~8のいずれに記載の複合セパレーター。 - 請求項1~9のいずれに記載の複合セパレーターを含む電気化学エネルギー貯蔵装置。
- カソードシート、
アノードシート、及び、
請求項7又は8に記載の複合セパレーターを含む電気化学エネルギー貯蔵装置であって、前記第1のサブ層は、前記第2のサブ層に比べて前記カソードシートのより近くに設けられている、電気化学エネルギー貯蔵装置。 - 請求項10又は11に記載の電気化学エネルギー貯蔵装置を含むことを特徴とする、電気装置。
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