CN110010953A - 锂盐混合物作为锂离子电池电解质的用途 - Google Patents
锂盐混合物作为锂离子电池电解质的用途 Download PDFInfo
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- 229910003002 lithium salt Inorganic materials 0.000 title claims abstract description 40
- 159000000002 lithium salts Chemical class 0.000 title claims abstract description 40
- 239000003792 electrolyte Substances 0.000 title claims abstract description 10
- 229910001416 lithium ion Inorganic materials 0.000 title abstract description 10
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title abstract description 8
- 239000011833 salt mixture Substances 0.000 title abstract description 7
- 239000002904 solvent Substances 0.000 claims abstract description 19
- 239000000203 mixture Substances 0.000 claims description 48
- 150000003839 salts Chemical class 0.000 claims description 27
- JNCMHMUGTWEVOZ-UHFFFAOYSA-N F[CH]F Chemical compound F[CH]F JNCMHMUGTWEVOZ-UHFFFAOYSA-N 0.000 claims description 22
- VUWZPRWSIVNGKG-UHFFFAOYSA-N fluoromethane Chemical compound F[CH2] VUWZPRWSIVNGKG-UHFFFAOYSA-N 0.000 claims description 20
- 229910001290 LiPF6 Inorganic materials 0.000 claims description 12
- 150000002148 esters Chemical class 0.000 claims description 8
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 6
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 claims description 3
- 229910001558 CF3SO3Li Inorganic materials 0.000 claims description 2
- 229910010912 Li2B12F12 Inorganic materials 0.000 claims description 2
- 229910006145 SO3Li Inorganic materials 0.000 claims description 2
- XIXADJRWDQXREU-UHFFFAOYSA-M lithium acetate Chemical compound [Li+].CC([O-])=O XIXADJRWDQXREU-UHFFFAOYSA-M 0.000 claims description 2
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 2
- 238000004090 dissolution Methods 0.000 abstract description 3
- 229910052744 lithium Inorganic materials 0.000 description 12
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 11
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 5
- 239000004411 aluminium Substances 0.000 description 5
- 229910052782 aluminium Inorganic materials 0.000 description 5
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 5
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 4
- 229910010941 LiFSI Inorganic materials 0.000 description 4
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 4
- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 description 4
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 description 3
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- 238000000354 decomposition reaction Methods 0.000 description 3
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- 229910052731 fluorine Inorganic materials 0.000 description 3
- 239000004615 ingredient Substances 0.000 description 3
- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 description 3
- 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 3
- 150000002825 nitriles Chemical class 0.000 description 3
- 238000002161 passivation Methods 0.000 description 3
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 description 2
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 description 2
- 229910019142 PO4 Inorganic materials 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 125000001153 fluoro group Chemical group F* 0.000 description 2
- RAXXELZNTBOGNW-UHFFFAOYSA-N imidazole Natural products C1=CNC=N1 RAXXELZNTBOGNW-UHFFFAOYSA-N 0.000 description 2
- 150000002466 imines Chemical class 0.000 description 2
- 238000005192 partition Methods 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 2
- 239000010452 phosphate Substances 0.000 description 2
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 2
- ZUHZGEOKBKGPSW-UHFFFAOYSA-N tetraglyme Chemical compound COCCOCCOCCOCCOC ZUHZGEOKBKGPSW-UHFFFAOYSA-N 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- RRQYJINTUHWNHW-UHFFFAOYSA-N 1-ethoxy-2-(2-ethoxyethoxy)ethane Chemical compound CCOCCOCCOCC RRQYJINTUHWNHW-UHFFFAOYSA-N 0.000 description 1
- MBVGJZDLUQNERS-UHFFFAOYSA-N 2-(trifluoromethyl)-1h-imidazole-4,5-dicarbonitrile Chemical class FC(F)(F)C1=NC(C#N)=C(C#N)N1 MBVGJZDLUQNERS-UHFFFAOYSA-N 0.000 description 1
- QGHDLJAZIIFENW-UHFFFAOYSA-N 4-[1,1,1,3,3,3-hexafluoro-2-(4-hydroxy-3-prop-2-enylphenyl)propan-2-yl]-2-prop-2-enylphenol Chemical group C1=C(CC=C)C(O)=CC=C1C(C(F)(F)F)(C(F)(F)F)C1=CC=C(O)C(CC=C)=C1 QGHDLJAZIIFENW-UHFFFAOYSA-N 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 239000002841 Lewis acid Substances 0.000 description 1
- 229910002986 Li4Ti5O12 Inorganic materials 0.000 description 1
- 229910032387 LiCoO2 Inorganic materials 0.000 description 1
- 229910052493 LiFePO4 Inorganic materials 0.000 description 1
- 229910010722 LiFePO4F Inorganic materials 0.000 description 1
- 229910010764 LiFeSO4F Inorganic materials 0.000 description 1
- 229910014071 LiMn1/3Co1/3Ni1/3O2 Inorganic materials 0.000 description 1
- 229910013872 LiPF Inorganic materials 0.000 description 1
- 101150058243 Lipf gene Proteins 0.000 description 1
- VULXNJHRVYGPSQ-UHFFFAOYSA-N N=NC=NN.N=NC=NN.CC(COC(C)CO)O Chemical compound N=NC=NN.N=NC=NN.CC(COC(C)CO)O VULXNJHRVYGPSQ-UHFFFAOYSA-N 0.000 description 1
- RFFFKMOABOFIDF-UHFFFAOYSA-N Pentanenitrile Chemical compound CCCCC#N RFFFKMOABOFIDF-UHFFFAOYSA-N 0.000 description 1
- QOSMNYMQXIVWKY-UHFFFAOYSA-N Propyl levulinate Chemical compound CCCOC(=O)CCC(C)=O QOSMNYMQXIVWKY-UHFFFAOYSA-N 0.000 description 1
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-N carbonic acid Chemical compound OC(O)=O BVKZGUZCCUSVTD-UHFFFAOYSA-N 0.000 description 1
- 239000010406 cathode material Substances 0.000 description 1
- 235000009508 confectionery Nutrition 0.000 description 1
- FUGIIBWTNARRSF-UHFFFAOYSA-N decane-5,6-diol Chemical compound CCCCC(O)C(O)CCCC FUGIIBWTNARRSF-UHFFFAOYSA-N 0.000 description 1
- 229940019778 diethylene glycol diethyl ether Drugs 0.000 description 1
- SBZXBUIDTXKZTM-UHFFFAOYSA-N diglyme Chemical compound COCCOCCOC SBZXBUIDTXKZTM-UHFFFAOYSA-N 0.000 description 1
- 238000010494 dissociation reaction Methods 0.000 description 1
- 230000005593 dissociations Effects 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 1
- DWYMPOCYEZONEA-UHFFFAOYSA-L fluoridophosphate Chemical compound [O-]P([O-])(F)=O DWYMPOCYEZONEA-UHFFFAOYSA-L 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- UQSQSQZYBQSBJZ-UHFFFAOYSA-N fluorosulfonic acid Chemical class OS(F)(=O)=O UQSQSQZYBQSBJZ-UHFFFAOYSA-N 0.000 description 1
- ZTOMUSMDRMJOTH-UHFFFAOYSA-N glutaronitrile Chemical compound N#CCCCC#N ZTOMUSMDRMJOTH-UHFFFAOYSA-N 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- -1 imidazole anion Chemical class 0.000 description 1
- 150000002460 imidazoles Chemical class 0.000 description 1
- 230000002427 irreversible effect Effects 0.000 description 1
- LRDFRRGEGBBSRN-UHFFFAOYSA-N isobutyronitrile Chemical compound CC(C)C#N LRDFRRGEGBBSRN-UHFFFAOYSA-N 0.000 description 1
- 150000007517 lewis acids Chemical class 0.000 description 1
- 229940006487 lithium cation Drugs 0.000 description 1
- CUONGYYJJVDODC-UHFFFAOYSA-N malononitrile Chemical compound N#CCC#N CUONGYYJJVDODC-UHFFFAOYSA-N 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 150000005677 organic carbonates Chemical class 0.000 description 1
- 125000006340 pentafluoro ethyl group Chemical group FC(F)(F)C(F)(F)* 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- FVSKHRXBFJPNKK-UHFFFAOYSA-N propionitrile Chemical compound CCC#N FVSKHRXBFJPNKK-UHFFFAOYSA-N 0.000 description 1
- IAHFWCOBPZCAEA-UHFFFAOYSA-N succinonitrile Chemical compound N#CCCC#N IAHFWCOBPZCAEA-UHFFFAOYSA-N 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- XPDWGBQVDMORPB-UHFFFAOYSA-N trifluoromethane acid Natural products FC(F)F XPDWGBQVDMORPB-UHFFFAOYSA-N 0.000 description 1
- YFNKIDBQEZZDLK-UHFFFAOYSA-N triglyme Chemical compound COCCOCCOCCOC YFNKIDBQEZZDLK-UHFFFAOYSA-N 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07D—HETEROCYCLIC COMPOUNDS
- C07D233/00—Heterocyclic compounds containing 1,3-diazole or hydrogenated 1,3-diazole rings, not condensed with other rings
- C07D233/54—Heterocyclic compounds containing 1,3-diazole or hydrogenated 1,3-diazole rings, not condensed with other rings having two double bonds between ring members or between ring members and non-ring members
- C07D233/66—Heterocyclic compounds containing 1,3-diazole or hydrogenated 1,3-diazole rings, not condensed with other rings having two double bonds between ring members or between ring members and non-ring members with hetero atoms or with carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals, directly attached to ring carbon atoms
- C07D233/90—Carbon atoms having three bonds to hetero atoms with at the most one bond to halogen, e.g. ester or nitrile radicals
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M10/052—Li-accumulators
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- H01M10/00—Secondary cells; Manufacture thereof
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- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- 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
- H01M10/0568—Liquid materials characterised by the solutes
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Abstract
本发明涉及锂盐混合物。其还涉及适合用作用于锂离子电池的电解质的溶解在溶剂中的所述盐混合物。
Description
本申请是基于申请日为2012年11月21日、优先权日为2011年12月06日、申请号为201280060187.3、发明名称为“锂盐混合物作为锂离子电池电解质的用途”的中国专利申请的分案申请。
技术领域
本发明涉及锂盐的混合物以及其作为用于Li离子型电池的电解质的用途。
背景技术
锂离子电池至少包括负极(阳极)、正极(阴极)、隔板和电解质。电解质通常由溶解在溶剂中的锂盐组成，所述溶剂通常为有机碳酸酯的混合物，以在粘度和介电常数之间具有良好的折衷。可随后加入添加剂以改善电解质盐的稳定性。
最广泛使用的盐包括六氟磷酸锂(LiPF6)，其具有众多所需品质中的很多品质，但是呈现出通过与水的反应而以氢氟酸形式分解的缺点。这引起安全问题，特别是即将在私家车中使用锂离子电池的情况下。
因此，已经开发了其它盐例如LiTFSI(双(三氟甲烷磺酰)亚胺锂)和LiFSI(双(氟磺酰)亚胺锂)。这些盐呈现出很少的自发分解或者不呈现自发分解并且对于水解而言比LiPF6稳定。但是，LiTFSI呈现出如下缺点：对于铝集流体是腐蚀性的，对于LiFSI则情况不是如此。因此，LiFSI看来是LiPF6的有希望的替代物，但是其成本目前限制了其使用。
最近，已经开发了其它盐例如LiTDI(4,5-二氰基-2-(三氟甲基)咪唑锂)和LiPDI(4,5-二氰基-2-(五氟乙基)咪唑锂)。这些盐呈现出如下优点：具有较少的氟原子，并且具有强的碳-氟键代替LiPF6的较弱的磷-氟键。此外，文献WO2010023413显示这些盐呈现出约6mS/cm的电导率、在咪唑阴离子和锂阳离子之间非常良好的解离、以及它们作为用于Li离子电池的电解质盐的用途。
在文献WO2010/023143、WO 2010/113483、WO 2010/113835和WO 2009/123328中描述了所述盐的制备。
本申请人公司已经发现，使用上述盐的混合物使得可部分地或完全地克服当它们孤立使用时发现的缺点。
该混合物可包括至少两种不同的盐。
发明内容
本发明首先涉及锂盐的混合物。
本发明的另一主题是溶解在溶剂中的所述盐的混合物。
本发明的另外的主题是所述混合物作为用于由阳极、阴极和隔板组成的Li离子蓄电池的电解质的用途。所述阳极可为锂金属、石墨、碳、碳纤维、合金、Li4Ti5O12、或者上述的至少两种的混合物。所述阴极可为基于锂的氧化物、基于锂的磷酸盐、基于锂的氟磷酸盐、基于锂的硫酸盐、或锂的氟硫酸盐。除了锂之外，还可存在一种或多种过渡金属，例如LiCoO2、LiFePO4、LiMn1/3Co1/3Ni1/3O2、LiFePO4F和LiFeSO4F。所述阴极也可为上述化合物的至少两种的混合物。
本发明使得可克服上述盐的缺点。其更具体地提供能够用作用于Li离子电池的电解质的锂盐的混合物。
根据本发明的混合物包括从如下三组盐的两组中选择的至少两种锂盐：
·X：LiPF6、LiBF4、CH3COOLi、CH3SO3Li、CF3SO3Li、CF3COOLi、Li2B12F12、LiBC4O8
·R1-SO2-NLi-SO2-R2，其中R1和R2独立地表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3
·式(I)，其中Rf表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
根据本发明的混合物优选地包括：至少一种式(I)的锂盐，其中Rf表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3；和选自X组或R1-SO2-NLi-SO2-R2组的至少一种锂盐，其中R1和R2独立地表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
根据本发明的一个优选实施方式，所述混合物包括：至少一种式(I)的锂盐，其中Rf表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3；和选自X组的至少一种锂盐。
根据本发明的另一优选实施方式，所述混合物包括：至少一种式(I)的锂盐，其中Rf表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3；和选自R1-SO2-NLi-SO2-R2组的至少一种锂盐，其中R1和R2独立地表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
根据本发明的一种优选替代形式，所述混合物包括：选自X组的至少一种锂盐；和选自R1-SO2-NLi-SO2-R2组的至少一种锂盐，其中R1和R2独立地表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
有利地，根据本发明的混合物包括：至少一种式(I)的锂盐，其中Rf表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3；选自X组的至少一种锂盐；和选自R1-SO2-NLi-SO2-R2组的至少一种锂盐，其中R1和R2独立地表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
无论什么实施方式或替代形式，X组的特别优选的化合物为LiPF6。
无论什么实施方式或替代形式，式(I)的特别优选的Rf是F、CF3、CHF2、C2F5、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
无论什么实施方式或替代形式，特别优选其中R1和R2独立地表示F、CF3、C2F5、C2F4OCF3、C2H2F2OCF3或CF2OCF3的R1-SO2-NLi-SO2-R2组的锂盐。
所述混合物中存在的各锂盐的量可在宽的界限内变化并且通常占1重量％-99重量％、优选5重量％-95重量％，相对于所述混合物中存在的盐的总重量。
本发明的另一主题是溶解在一种溶剂或多种(几种)溶剂中的所述盐的混合物，所述溶剂优选为碳酸酯、甘醇二醚(甘醇二甲醚)、腈和二腈或氟化溶剂。
作为碳酸酯，可特别提及碳酸亚乙酯、碳酸二甲酯、碳酸甲乙酯、碳酸二乙酯或碳酸亚丙酯。
作为甘醇二醚，可特别提及乙二醇二甲醚、二乙二醇二甲醚、一缩二丙二醇二甲醚、二乙二醇二乙醚、三乙二醇二甲醚、二乙二醇二丁醚、四乙二醇二甲醚和二乙二醇叔丁基甲基醚。
作为腈和二腈，可特别提及乙腈、丙腈、异丁腈、戊腈、丙二腈、丁二腈、或戊二腈。
作为氟化溶剂，可提及其至少一个氢原子已被氟原子代替的前述溶剂：碳酸酯、甘醇二醚、腈和二腈。
成分各自的重量比例(其定义为成分的重量与溶剂的所有成分的总重量之比)优选为相对于最小量的成分的1-10、更优选1-8。
根据本发明的混合物导致最大的离子电导率、电化学稳定性和容量保持力并且导致最小的不可逆容量。所述混合物是由相应的锂盐制备的。当存在溶剂时，该制备通过如下进行：将构成所述混合物的锂盐溶解在合适比例的溶剂中，优选在搅拌下。
本申请人公司已经惊讶地注意到，使用在溶剂中以合适比例溶解的上述盐的混合物作为用于锂离子蓄电池的电解质未呈现出当将所述盐单独溶解在溶剂中时观察到的缺点。
例如(因此)，LiPF6与水猛烈反应以形成HF，其导致阴极材料的溶解。LiPF6还可分解得到路易斯酸PF5，其可导致用作溶剂的碳酸酯的分解，由此引起电池容量的损失。
R1-SO2-NLi-SO2-R2类型的盐呈现出如下缺点：在其中Li离子电池被使用的电势范围内，对于铝集流体是腐蚀性的。此外，对于一些R基团，这些盐显示出优异的离子电导率。
式(I)的盐呈现出对于铝集流体不是腐蚀性的以及在该集流体上形成稳定的钝化层的优点，但是具有为LiPF6的离子电导率的约一半的低的离子电导率。此外，这些盐还看来能够容易地俘获水分子。
实施例
按照各种类型的锂盐的缺点和优点，对于本发明而言，清楚地出现协同作用，如通过以下非限制性实施例。
实施例1
所制造的第一种混合物在于：在环境温度下，将包括80重量％的F-SO2-NLi-SO2-F(LiFSI)和20重量％的其中Rf＝CF3的式(I)的盐(LiTDI)的盐混合物溶解在如下三种碳酸酯的混合物中：碳酸亚乙酯、碳酸二甲酯和碳酸亚丙酯，各自重量比例为1/3、1/3和1/3。该混合物给出高的离子电导率并且导致在铝集流体上的钝化层。
实施例2
所制造的第二种混合物由50重量％的LiTDI盐和50重量％的LiPF6组成。将这两种盐溶解在如下两种碳酸酯的混合物中：碳酸亚乙酯和碳酸二甲酯，各自重量比例为1/3和2/3。该混合物给出高的离子电导率，而未使LiPF6分解。
实施例3
所制造的第三种混合物在于将包含60重量％的CF3-SO2-NLi-SO2-CF3(LiTFSI)和40重量％的LiTDI的盐混合物溶解在如下三种碳酸酯的混合物中：碳酸亚乙酯、碳酸二甲酯和碳酸亚丙酯，各自重量比率为1/3、1/3和1/3。该混合物给出高的离子电导率，并且导致形成于铝集流体上的钝化层。
Claims (14)
1.包括从如下三组盐的两组中选择的至少两种锂盐的混合物：
·X：LiPF6、LiBF4、CH3COOLi、CH3SO3Li、CF3SO3Li、CF3COOLi、Li2B12F12、LiBC4O8
·R1-SO2-NLi-SO2-R2，其中R1和R2独立地表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3
·式(I)，其中Rf表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3
2.权利要求1的混合物，其包括：至少一种式(I)的锂盐，其中Rf表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3；和选自X组或R1-SO2-NLi-SO2-R2组的至少一种锂盐，其中R1和R2独立地表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
3.权利要求2的混合物，其包括：至少一种式(I)的锂盐，其中Rf表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3；和选自X组的至少一种锂盐。
4.权利要求2的混合物，其包括：至少一种式(I)的锂盐，其中Rf表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3；和选自R1-SO2-NLi-SO2-R2组的至少一种锂盐，其中R1和R2独立地表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
5.权利要求1的混合物，其包括：选自X组的至少一种锂盐；和选自R1-SO2-NLi-SO2-R2组的至少一种锂盐，其中R1和R2独立地表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
6.权利要求1的混合物，其包括：至少一种式(I)的锂盐，其中Rf表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3；选自X组的至少一种锂盐；和选自R-SO2-NLi-SO2-R组的至少一种锂盐，其中R表示F、CF3、CHF2、CH2F、C2HF4、C2H2F3、C2H3F2、C2F5、C3F7、C3H2F5、C3H4F3、C4F9、C4H2F7、C4H4F5、C5F11、C3F5OCF3、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
7.权利要求1-4和6的混合物，其特征在于Rf表示F、CF3、CHF2、C2F5、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
8.权利要求1-2和4-6的混合物，其特征在于R1和R2独立地表示F、CF3、C2F5、C2F4OCF3、C2H2F2OCF3或CF2OCF3。
9.权利要求1-3和5-8的混合物，其特征在于X组的锂盐为LiPF6。
10.权利要求1-9任一项的混合物，其特征在于所述混合物中存在的各锂盐的量占1重量％-99重量％、优选5重量％-95重量％，相对于所存在的锂盐的总重量。
11.权利要求1-10任一项的混合物，其特征在于其是由相应的锂盐制备的。
12.权利要求1-11任一项的混合物，其特征在于其溶解在一种溶剂或多种溶剂中。
13.权利要求12的混合物，其特征在于所述溶剂选自碳酸酯和甘醇二醚。
14.权利要求1-13任一项的混合物作为电解质的用途。
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2011
- 2011-12-06 FR FR1161204A patent/FR2983466B1/fr active Active
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2012
- 2012-05-31 FR FR1255046A patent/FR2983467B1/fr active Active
- 2012-11-21 CA CA2854135A patent/CA2854135C/fr active Active
- 2012-11-21 US US14/359,888 patent/US20150017551A1/en not_active Abandoned
- 2012-11-21 KR KR1020147014190A patent/KR20140096319A/ko not_active Application Discontinuation
- 2012-11-21 PL PL12808425T patent/PL2789042T3/pl unknown
- 2012-11-21 KR KR1020197007406A patent/KR20190030773A/ko not_active Application Discontinuation
- 2012-11-21 PL PL17197915.6T patent/PL3293807T3/pl unknown
- 2012-11-21 EP EP12808425.8A patent/EP2789042B1/fr active Active
- 2012-11-21 CN CN201280060187.3A patent/CN103975476A/zh active Pending
- 2012-11-21 ES ES12808425.8T patent/ES2615257T3/es active Active
- 2012-11-21 CN CN201811515725.9A patent/CN110010953A/zh active Pending
- 2012-11-21 EP EP15175445.4A patent/EP2947714B1/fr active Active
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- 2012-11-21 WO PCT/FR2012/052681 patent/WO2013083894A1/fr active Application Filing
- 2012-11-21 PL PL15175445T patent/PL2947714T3/pl unknown
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| CN112349962A (zh) * | 2019-08-08 | 2021-02-09 | 宁德时代新能源科技股份有限公司 | 锂离子电池 |
| CN112349962B (zh) * | 2019-08-08 | 2021-11-09 | 宁德时代新能源科技股份有限公司 | 锂离子电池 |
Also Published As
| Publication number | Publication date |
|---|---|
| US20150017551A1 (en) | 2015-01-15 |
| FR2983467A1 (fr) | 2013-06-07 |
| CA2854135A1 (fr) | 2013-06-13 |
| ES2916098T3 (es) | 2022-06-28 |
| EP2947714B1 (fr) | 2017-11-15 |
| FR2983467B1 (fr) | 2013-11-15 |
| JP6192234B2 (ja) | 2017-09-06 |
| JP2018073833A (ja) | 2018-05-10 |
| KR20140096319A (ko) | 2014-08-05 |
| ES2653413T3 (es) | 2018-02-07 |
| EP2789042B1 (fr) | 2016-12-21 |
| JP2017022116A (ja) | 2017-01-26 |
| CA2854135C (fr) | 2019-07-16 |
| EP3293807A1 (fr) | 2018-03-14 |
| EP2947714A1 (fr) | 2015-11-25 |
| FR2983466B1 (fr) | 2014-08-08 |
| ES2615257T3 (es) | 2017-06-06 |
| KR20160055979A (ko) | 2016-05-18 |
| CN109560320A (zh) | 2019-04-02 |
| JP2020147566A (ja) | 2020-09-17 |
| PL2947714T3 (pl) | 2018-02-28 |
| JP6704310B2 (ja) | 2020-06-03 |
| KR20190030773A (ko) | 2019-03-22 |
| EP2789042A1 (fr) | 2014-10-15 |
| FR2983466A1 (fr) | 2013-06-07 |
| PL2789042T3 (pl) | 2017-07-31 |
| PL3293807T3 (pl) | 2022-07-18 |
| JP2015500554A (ja) | 2015-01-05 |
| CN103975476A (zh) | 2014-08-06 |
| WO2013083894A1 (fr) | 2013-06-13 |
| EP3293807B1 (fr) | 2022-05-18 |
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