CN102738508A - Lithium ion battery electrolyte with low lithium salt content - Google Patents
Lithium ion battery electrolyte with low lithium salt content Download PDFInfo
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- CN102738508A CN102738508A CN2011100904159A CN201110090415A CN102738508A CN 102738508 A CN102738508 A CN 102738508A CN 2011100904159 A CN2011100904159 A CN 2011100904159A CN 201110090415 A CN201110090415 A CN 201110090415A CN 102738508 A CN102738508 A CN 102738508A
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Abstract
The invention provides a lithium ion battery electrolyte able to reduce lithium salt content, and the electrolyte is composed of a lithium salt, an ionic liquid, organic solvents and an additive. The strong dissolving capability and high ionic conductivity of the ionic liquid promotes the dissociation and migration of lithium ions, thus reducing the lithium salt content in the electrolyte. After 50 times of charge-discharge circulation of a battery composed of the electrolyte under a multiplying power of 0.1C, the discharge capacity can still be maintained at 150mAh/g. substituting the ionic liquid for a part of the lithium salt can reduce the electrolyte cost and enhance the economic benefit. Meanwhile, the adding of the ionic liquid can also improve the electrolyte stability and raise battery security, so that the lithium ion battery electrolyte of the invention boasts a high market promotion value.
Description
Technical field
The present invention relates to a kind of lithium-ion battery electrolytes of the electrolyte that is used for lithium ion battery, particularly a kind of low lithium salt content.
Background technology
Lithium ion battery is the green high-capacity environment-protecting battery that occurs the nineties in 20th century, but has operating voltage height, the big fast charging and discharging of specific energy, has extended cycle life, memory-less effect, characteristics such as pollution-free.Electrolyte is known as lithium ion battery " blood ", affects specific energy, fail safe, cycle performance, rate charge-discharge performance, storge quality of lithium battery etc.Lithium-ion battery electrolytes mainly is made up of lithium salts and organic carbonate, and wherein, electric conducting lithium salt plays a part transmission ion and conduction current, to the battery performance important influence, also is the chief component of electrolyte price.At present, commercial lithium-ion battery electrolytes adopts the LiPF of 1M more
6, LiPF
6General complicated process of preparation; Guardian technique is by external monopolization, and cost is higher, accounts for about 50% of electrolyte cost; And just possibly decompose for 80 ℃ in room temperature; Meet trace water and promptly emit corrosive gas HF, the structure that more HF destroys negative pole SEI film easily under hot environment causes the reduction of capacity, even safety problem occurs.To the above problem that runs into, how people reduce LiPF in continuous research
6Use amount or alternative LiPF
6The novel lithium salts security performance that improves battery with reduce the electrolyte cost.
Ionic liquid (Ionic liquid) is to be made up of cation and anion fully, at the salt that is in a liquid state below 100 ℃, is also referred to as watery fusion salt.Ionic liquid does not almost have vapour pressure, has excellent thermal stability and chemical stability, and the electrochemical window broad also has ionic conductivity preferably simultaneously.In lithium-ion battery electrolytes; The fail safe that ionic liquid can improve electrolyte as solvent, on the other hand, itself is exactly a kind of room temperature fuse salt; Can play the effect of transmission ion; Thereby improve the conductivity of electrolyte, reduce the content of solute lithium salts, make electrolyte under lower lithium salt content, still have higher charging and discharging capacity and cycle efficieny.It is thus clear that ionic liquid has application promise in clinical practice in field of batteries, and very likely be applied in the electrochemical device as novel green electrolyte of future generation.
Summary of the invention
The invention provides a kind of lithium-ion battery electrolytes that can reduce lithium salt content, this electrolyte is made up of lithium salts, ionic liquid, organic solvent and additive four parts.
Wherein, said ion liquid cation comprises that quaternary amines, quaternary phosphonium class, imidazoles, pyridines, piperidines, pyroles, porphyrin class, guanidine class, sulphur class, amino acid esters etc. can be used for the ionic liquid of lithium ion battery.
The used lithium salts of this electrolyte is one or more in tetrafluoro boric acid lithium salts, hexafluorophosphoric acid lithium salts, two (trifluoromethyl sulphonyl) imines lithium salts, two (trifluoro sulphonyl) imines lithium salts, di-oxalate lithium borate salt, lithium perchlorate, hexafluoroarsenate lithium, lithium halide, the chlorine lithium aluminate.
The used organic solvent of this electrolyte is a methyl formate; Methyl acetate; Methylchloroformate; Ethyl acetate; Ethyl propionate; Ethyl butyrate; Vinyl acetate; Propionic acid propylene ester; The ring butyrolactone; Bromine ring butyrolactone; Methyl benzoate; Methyl carbonic acid propylene ester; Ethyl carbonate propylene ester; The methyl carbonic acid phenol ester; Ethylene carbonate; Halogenated ethylene carbonate; Propene carbonate; Butylene; Dimethyl carbonate; Diethyl carbonate; Methyl ethyl carbonate; Carbonic acid first propyl ester; Vinylene carbonate; Ethylene sulfite; Propylene sulfite; The sulfurous acid butene esters; Dimethyl sulfite; Sulfurous acid diethyl ester; Methyl-sulfoxide; The second methyl sulfoxide; The trifluoropropyl methyl sulfoxide; 1; The 3-N-morpholinopropanesulfonic acid lactone; 1; The 4-butyl sultone; In dioxolanes or the dimethoxy propane two or more.
The used additive of this electrolyte is film for additive, flame-retardant additive, let slip and fill in additive, conductive additive, the multifunction additive one or more.
Gross mass with electrolyte is a benchmark, and the mass percent of said lithium salts is x%, 5≤x≤50, and said ion liquid content mass percent is m%, 5<m≤90; The mass percent of said organic solvent is d%, 0≤d≤95; The mass percent of said additive is n%, 1≤n≤7.
Characteristics of the present invention are the lithium-ion battery electrolytes that prepared a kind of low lithium salt content, and this electrolyte is made up of lithium salts, ionic liquid and organic solvent.Ionic liquid has dissolubility, ionic conductivity and electrochemical stability preferably; And it is as a kind of room temperature fuse salt; Be solvent be again solute; Ion liquid adding has reduced the content of lithium salts in the electrolyte to a certain extent, makes it be lower than the lithium salt content of 1mol/L in traditional electrolyte.Along with the development of ionic liquid production scaleization, can substitute a part of lithium salts with ionic liquid, thereby reduce the cost of electrolyte, increase economic efficiency; Simultaneously, ion liquid adding can also improve the stability of electrolyte, improves the fail safe of battery, has higher market popularization value.
Description of drawings
Fig. 1 makes for embodiment 1 when containing two (trifluoromethyl sulphonyl) the imines ion liquid of N-methyl-N-propyl group piperidines and under the 0.1C multiplying power, carrying out the battery charging and discharging test with two (trifluoromethyl sulphonyl) imines lithium electrolyte volume change and cycle efficieny figure.
Fig. 2 makes for embodiment 1 when containing two (trifluoromethyl sulphonyl) the imines ion liquid of N-methyl-N-propyl group piperidines and under the 0.5C multiplying power, carrying out the battery charging and discharging test with two (trifluoromethyl sulphonyl) imines lithium electrolyte volume change and cycle efficieny figure.
Embodiment
The present invention explains with following embodiment, but is not limited to following embodiment, before and after not breaking away from, in the scope of said aim, changes and implements to be included within the technical scope of the present invention.
Embodiment 1: a kind ofly contain two (trifluoromethyl sulphonyl) the imines ion liquid of N-methyl-N-propyl group piperidines and the preparation of two (trifluoromethyl sulphonyl) imines lithium electrolyte and the application in lithium ion battery thereof
1 gets two (trifluoromethyl sulphonyl) the imines ion liquid of 10g N-methyl-N-propyl group piperidines; Add the diethyl carbonate that 15g dewaters through molecular sieve and the mixed solvent (both mass ratioes are 2: 1) of ethylene carbonate; Add 0.5g film for additive vinylene carbonate again; Add two (trifluoromethyl sulphonyl) imines lithium salts (molar concentration is 0.5mol/L) at last, fully dissolving mixes, and obtains a kind of lithium-ion battery electrolytes of low lithium salt content.
2 Fig. 1, Fig. 2 make for embodiment 1 contains two (trifluoromethyl sulphonyl) the imines ion liquid of N-methyl-N-propyl group piperidines and two (trifluoromethyl sulphonyl) imines lithium electrolyte and under 0.1C and 0.5C multiplying power, carries out volume change and the cycle efficieny figure of battery charging and discharging when testing respectively.Make button-shaped lithium ion battery and test, wherein: battery size is 2032; Positive electrode is LiFePO4 (commercially available material is directly buied), directly is coated on the aluminum foil current collector after sizing mixing with acetylene black, adhesive PVDF; Barrier film is Cellgard2325; Negative pole is a metal lithium sheet.Adopt LAND charge-discharge test appearance under normal temperature (25 ℃), to test, charge-discharge magnification is respectively 0.1C and 0.5C.Fig. 1 has shown under the 0.1C rate charge-discharge that the capacity of battery still remains on 150mAh/g after circulating through 50 times, and efficiency for charge-discharge remains on more than 99% basically.Fig. 2 has shown that the initial capacity of battery under the 0.5C rate charge-discharge is 132.6mAh/g, is 110.1mAh/g through capacity after 40 charge and discharge cycles, and capability retention is 82.9%, and efficiency for charge-discharge remains on more than 98% basically.
Embodiment 2: a kind of preparation that contains two (trifluoromethyl sulphonyl) imines ion liquid of N-methyl-N-propyl group piperidines and LiBF4 electrolyte
Get two (trifluoromethyl sulphonyl) the imines ion liquid of 12.5g N-methyl-N-propyl group piperidines; Add the diethyl carbonate that 12.5g dewaters through molecular sieve and the mixed solvent (both mass ratioes are 2: 1) of ethylene carbonate; Add 0.5g film for additive vinylene carbonate again; Add tetrafluoro boric acid lithium salts (molar concentration is 0.5mol/L) at last, fully dissolving mixes, and obtains a kind of lithium-ion battery electrolytes of low lithium salt content.
Embodiment 3: a kind of 1-propyl group-2 that contains, the preparation of two (trifluoromethyl sulphonyl) imines ion liquid of 3-methylimidazole and lithium hexafluoro phosphate electrolyte
Get 15g 1-propyl group-2; Two (trifluoromethyl sulphonyl) the imines ion liquid of 3-methylimidazole; Add the diethyl carbonate that 10g dewaters through molecular sieve and the mixed solvent (both mass ratioes are 2: 1) of ethylene carbonate, add 0.5g film for additive vinylene carbonate again, add hexafluorophosphoric acid lithium salts (molar concentration is 0.5mol/L) at last; Fully dissolving mixes, and obtains a kind of lithium-ion battery electrolytes of low lithium salt content.
Embodiment 4: a kind of preparation that contains two (trifluoromethyl sulphonyl) imines ion liquid of N-methyl-N-butyl piperidine and sulfimide lithium electrolyte
Get two (trifluoromethyl sulphonyl) the imines ion liquid of 10g N-methyl-N-butyl piperidine; Add the diethyl carbonate that 15g dewaters through molecular sieve and the mixed solvent (both mass ratioes are 2: 1) of ethylene carbonate; Add 0.5g film for additive vinylene carbonate again; Add sulfimide lithium salts (molar concentration is 0.5mol/L) at last, fully dissolving mixes, and obtains a kind of lithium-ion battery electrolytes of low lithium salt content.
Embodiment 5: a kind of 1-hexyl-2 that contains, the preparation of two (trifluoromethyl sulphonyl) imines ion liquid of 3-methylimidazole and di-oxalate lithium borate electrolyte
Get 20g 1-hexyl-2; Two (trifluoromethyl sulphonyl) the imines ion liquid of 3-methylimidazole; Add the diethyl carbonate that 5g dewaters through molecular sieve and the mixed solvent (both mass ratioes are 2: 1) of ethylene carbonate, add 0.5g film for additive vinylene carbonate again, add di-oxalate lithium borate salt (molar concentration is 0.5mol/L) at last; Fully dissolving mixes, and obtains a kind of lithium-ion battery electrolytes of low lithium salt content.
Embodiment 6: a kind of preparation that contains two (trifluoromethyl sulphonyl) imines ion liquid of N-methyl-N-propyl pyrrole and lithium perchlorate electrolyte
Get two (trifluoromethyl sulphonyl) the imines ion liquid of 10g N-methyl-N-propyl pyrrole; Add the diethyl carbonate that 15g dewaters through molecular sieve and the mixed solvent (both mass ratioes are 2: 1) of ethylene carbonate; Add 0.5g film for additive vinylene carbonate again; Add lithium perchlorate salt (molar concentration is 0.5mol/L) at last, fully dissolving mixes, and obtains a kind of lithium-ion battery electrolytes of low lithium salt content.
Claims (6)
1. lithium-ion battery electrolytes that can reduce lithium salt content, this electrolyte is made up of lithium salts, ionic liquid, organic solvent and additive four parts.
2. lithium-ion battery electrolytes according to claim 1, wherein ion liquid cation comprise that quaternary amines, quaternary phosphonium class, imidazoles, pyridines, piperidines, pyroles, porphyrin class, guanidine class, sulphur class, amino acid esters etc. can be used for the ionic liquid of lithium ion battery.
3. lithium-ion battery electrolytes according to claim 1, wherein lithium salts is one or more in tetrafluoro boric acid lithium salts, hexafluorophosphoric acid lithium salts, two (trifluoromethyl sulphonyl) imines lithium salts, two (trifluoro sulphonyl) imines lithium salts, di-oxalate lithium borate salt, lithium perchlorate, hexafluoroarsenate lithium, lithium halide, the chlorine lithium aluminate.
4. lithium-ion battery electrolytes according to claim 1, wherein organic solvent is methyl formate, methyl acetate, methylchloroformate, ethyl acetate, ethyl propionate, ethyl butyrate, vinyl acetate, propionic acid propylene ester, ring butyrolactone, bromine ring butyrolactone, methyl benzoate, methyl carbonic acid propylene ester, ethyl carbonate propylene ester, methyl carbonic acid phenol ester, ethylene carbonate, halogenated ethylene carbonate, propene carbonate, butylene, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, carbonic acid first propyl ester, vinylene carbonate, ethylene sulfite, propylene sulfite, sulfurous acid butene esters, dimethyl sulfite, sulfurous acid diethyl ester, methyl-sulfoxide, second methyl sulfoxide, trifluoropropyl methyl sulfoxide, 1,3-N-morpholinopropanesulfonic acid lactone, 1,4-butyl sultone, dioxolanes or dimethoxy propane.
5. lithium-ion battery electrolytes according to claim 1, wherein additive for commonly used film for additive, flame-retardant additive, let slip and fill in additive, conductive additive, the multifunction additive two or more.
6. lithium-ion battery electrolytes according to claim 1, wherein the gross mass with electrolyte is a benchmark, the mass percent of said lithium salts is x%, 5≤x≤50, said ion liquid content mass percent is m%, 5<m≤90; The mass percent of said organic solvent is d%, 0≤d≤95; The mass percent of said additive is n%, 1≤n≤7.
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Cited By (12)
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CN103066324A (en) * | 2013-01-08 | 2013-04-24 | 芜湖恒耀汽车零部件有限公司 | Lithium ion battery electrolyte and lithium ion battery |
CN103094610A (en) * | 2013-01-30 | 2013-05-08 | 江西优锂新材股份有限公司 | Ionic liquid mixed electrolyte for lithium ion battery |
CN105552430A (en) * | 2016-03-09 | 2016-05-04 | 中国科学院宁波材料技术与工程研究所 | Electrolyte and lithium ion battery |
CN106159326A (en) * | 2016-08-26 | 2016-11-23 | 江苏天鹏电源有限公司 | A kind of Multifunctional electrolysis liquid |
CN106785024A (en) * | 2017-02-08 | 2017-05-31 | 湖南锂顺能源科技有限公司 | A kind of long-life ferric phosphate lithium cell electrolyte of wide temperature range and compound method |
CN109786116A (en) * | 2018-12-25 | 2019-05-21 | 中国电子科技集团公司第十八研究所 | Electrolyte for graphene-based lithium ion capacitor and preparation method thereof |
CN110148783A (en) * | 2019-04-01 | 2019-08-20 | 上海应用技术大学 | A kind of electrolyte and its preparation method and application improving graphite electrode surface SEI film properties |
CN110204473A (en) * | 2019-05-22 | 2019-09-06 | 常州乾艺智能制造科技有限公司 | A kind of double center cation liquid and preparation method thereof for lithium battery |
CN110364764A (en) * | 2019-07-23 | 2019-10-22 | 浙江大学 | A kind of electrolyte and preparation method thereof for lithium ion battery |
CN111443123A (en) * | 2020-04-03 | 2020-07-24 | 河南华瑞高新材料有限公司 | Method for rapidly judging performance of lithium salt and additive in electrolyte |
CN114725519A (en) * | 2021-01-06 | 2022-07-08 | 东莞理工学院 | Lithium ion battery electrolyte, preparation method thereof and lithium ion battery |
CN117477040A (en) * | 2023-12-27 | 2024-01-30 | 深圳欣视界科技有限公司 | Electrolyte and lithium ion battery containing same |
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Cited By (15)
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CN103066324A (en) * | 2013-01-08 | 2013-04-24 | 芜湖恒耀汽车零部件有限公司 | Lithium ion battery electrolyte and lithium ion battery |
CN103094610A (en) * | 2013-01-30 | 2013-05-08 | 江西优锂新材股份有限公司 | Ionic liquid mixed electrolyte for lithium ion battery |
CN103094610B (en) * | 2013-01-30 | 2015-12-23 | 江西优锂新材股份有限公司 | A kind of lithium ion battery ionic liquid mixed electrolyte |
CN105552430A (en) * | 2016-03-09 | 2016-05-04 | 中国科学院宁波材料技术与工程研究所 | Electrolyte and lithium ion battery |
CN106159326A (en) * | 2016-08-26 | 2016-11-23 | 江苏天鹏电源有限公司 | A kind of Multifunctional electrolysis liquid |
CN106785024A (en) * | 2017-02-08 | 2017-05-31 | 湖南锂顺能源科技有限公司 | A kind of long-life ferric phosphate lithium cell electrolyte of wide temperature range and compound method |
CN109786116A (en) * | 2018-12-25 | 2019-05-21 | 中国电子科技集团公司第十八研究所 | Electrolyte for graphene-based lithium ion capacitor and preparation method thereof |
CN110148783A (en) * | 2019-04-01 | 2019-08-20 | 上海应用技术大学 | A kind of electrolyte and its preparation method and application improving graphite electrode surface SEI film properties |
CN110148783B (en) * | 2019-04-01 | 2022-05-20 | 上海应用技术大学 | Electrolyte for improving performance of SEI (solid electrolyte interface) film on surface of graphite electrode as well as preparation method and application of electrolyte |
CN110204473A (en) * | 2019-05-22 | 2019-09-06 | 常州乾艺智能制造科技有限公司 | A kind of double center cation liquid and preparation method thereof for lithium battery |
CN110204473B (en) * | 2019-05-22 | 2023-03-10 | 常州乾艺智能制造科技有限公司 | Double-center cationic liquid for lithium battery and preparation method thereof |
CN110364764A (en) * | 2019-07-23 | 2019-10-22 | 浙江大学 | A kind of electrolyte and preparation method thereof for lithium ion battery |
CN111443123A (en) * | 2020-04-03 | 2020-07-24 | 河南华瑞高新材料有限公司 | Method for rapidly judging performance of lithium salt and additive in electrolyte |
CN114725519A (en) * | 2021-01-06 | 2022-07-08 | 东莞理工学院 | Lithium ion battery electrolyte, preparation method thereof and lithium ion battery |
CN117477040A (en) * | 2023-12-27 | 2024-01-30 | 深圳欣视界科技有限公司 | Electrolyte and lithium ion battery containing same |
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Application publication date: 20121017 |