CN103280599A - Lithium-ion battery electrolyte as well as preparation method and application thereof - Google Patents
Lithium-ion battery electrolyte as well as preparation method and application thereof Download PDFInfo
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- CN103280599A CN103280599A CN2013102189494A CN201310218949A CN103280599A CN 103280599 A CN103280599 A CN 103280599A CN 2013102189494 A CN2013102189494 A CN 2013102189494A CN 201310218949 A CN201310218949 A CN 201310218949A CN 103280599 A CN103280599 A CN 103280599A
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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- Y02E60/10—Energy storage using batteries
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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Abstract
The invention relates to lithium-ion battery electrolyte as well as a preparation method and application thereof, belonging to the field of batteries. The lithium-ion battery electrolyte comprises lithium salt and an organic solvent as well as a nitrile compound, wherein the organic solvent is at least one of dimethyl carbonate, diethyl carbonate, ethylene carbonate, propylene carbonate, ethyl methyl carbonate, methyl propyl carbonate, gamma-butyrolactone, gamma-valerolactone and diethyl oxalate. The lithium-ion battery electrolyte has decomposition voltage larger than 7.0V and can be used for preparing a high-voltage lithium-ion battery; and the monthly self discharge rate of the high-voltage lithium-ion battery assembled by the electrolyte is lower than 5 percent, the capacity retention ratio of the high-voltage lithium-ion battery after being circularly charged and discharged for 100 times under IC (integrated circuit) multiplying power is larger than 90 percent, and the practical demands can be met.
Description
Technical field
The present invention relates to lithium-ion battery electrolytes and preparation method thereof and application, belong to field of batteries.
Background technology
As secondary energy sources efficiently, lithium ion battery has been widely used on various portable type electronic products and the electric tool.Lithium ion battery generally adopts cobalt acid lithium (LiCoO at present
2) as positive electrode, charcoal class material is as negative material, the carbonate solution of lithium hexafluoro phosphate is as electrolyte; The discharge platform voltage of battery is greatly about about 3.7V; This is higher than the 1.25V of Ni-MH battery or nickel-cadmium cell and the 2.0V of lead-acid battery.In general, the voltage of battery is more high, and then the capacity of battery is also more high, and the range of application of battery is also more wide.A lot of electric tools are ability operate as normal under high voltage only, and for example the operating voltage of electric bicycle is 36V at present.
For the capacity that further improves lithium ion battery, enlarge its range of application, people are attempting to develop the lithium ion battery with higher discharge voltage always.Referring to " Chen Zhaoyong etc.; ' different material is to structure and the Effect on Performance of Li-Ni-Mn-O5V positive electrode '; Chinese Journal of Inorganic Chemistry; 2005; 21 (9): 1417-1421 " and some other pertinent literature, if adopt the nickel LiMn2O4 as positive electrode, then the discharge voltage of lithium ion battery can reach 4.0～4.6V, and this is higher than the 3.7V of present cobalt acid lithium battery.It is ripe that the technology of synthetic nickel manganate cathode material for lithium has been tending towards, and this can be with reference to domestic patent " Saic Chery Automobile Co., Ltd, ' a kind of method for preparing the high-voltage anode material Li-Ni-Mn-O ', CN201110062483.4 ".On the principles of chemistry, yet may there be other high-voltage anode material, for example with respect to the cobalt phosphate lithium (LiCoPO of lithium electrode 4.8V
4) positive electrode.
But the decomposition voltage of lithium hexafluoro phosphate/carbonic ester electrolyte that present lithium ion battery is used can only reach about 4.3V, can satisfy the requirement of lithium cobaltate cathode material; If cell voltage is higher than this decomposition voltage, then carbonate solvent or hexafluorophosphoric acid lithium electrolyte will be on anodal surface oxidation Decomposition gradually, worsen the chemical property of battery, make the rapid self discharge of battery.Exploitation has the electrolyte of high de-agglomeration voltage, has become the key that can high-voltage lithium ion batteries practicability.
Though some organic solvent has high decomposition voltage, for example document " Xu etc.; ' and LiBOB as Salt for Lithium-Ion Batteries '; Electrochemical and Solid-state Letters; 2002; 5 (1): A26-A29 " described sulfone class organic solvent, but these solvents often have very big viscosity, perhaps electrolyte solubility therein is very low, make that the conductivity of the electrolyte that these organic solvents constitute is very poor, can not be applied to high-voltage lithium ion batteries.
In view of above situation, relevant research direction has turned in common lithium-ion battery electrolytes and has added additive, to improve the decomposition voltage of electrolyte.Document " Zhang; ' and A review on electrolyte additives for lithium-ion batteries '; Journal of Power Science; 2006; 162:1379-1394 " summarized the various additives that are applied to lithium-ion electrolyte; class additive for the protection of positive electrode has wherein briefly been described; comprise amines (butylamine), imide compound (N; N '-dicyclohexylcarbodiimide) and amino silane compounds (N, N '-diethylamino trimethyl silane).These additives can form diaphragm on anodal surface with lithium salts.But the document is not mentioned the stability of these additives under high voltage, and also not seeing has practical application.
Chinese patent " Samsung SDI Co., Ltd; ' high pressure lithium rechargable battery electrolyte and high pressure lithium rechargable battery thereof '; CN200710148009.7 ", foreign patent " Samsung SDI Co Ltd (Kr); ' Electrolyte for high voltage lithium rechargeable battery and high voltage lithium rechargeable battery employing the same '; US2008090153; 2008-4-17 ", " Samsung SDI Co Ltd (Kr); ' Electrolyte for high-voltage lithium secondary battery; and high-voltage lithium secondary battery using the same '; JP2008103330; 2008-5-1 " and " Samsung SDI Co Ltd (Kr); ' Electrolyte for high voltage lithium rechargeable battery and battery employing the same ', EP1923948,2008-5-21 " etc. the applicant of four pieces of patents identical with flesh and blood, a kind of electrolyte that can be applied to high-voltage lithium ion batteries has been proposed.This electrolyte comprises non-aqueous organic solvent, lithium salts and is used as the halogenated biphenyl of additive and the combination of dihalo toluene that wherein the additive of this combination has the redox potential with respect to lithium 4.6～5.0V.When cell voltage surpassed 4.6V, oxidative polymerization can take place in above-mentioned additive, and the polymer that produces can make the slight short circuit of both positive and negative polarity, thereby avoided the further rising of cell voltage, but battery also can be with regard to this self-destruction.Therefore, this electrolyte can only prevent the accident that causes when lithium ion battery overcharges, can not make high-voltage lithium ion batteries practicability.
Chinese patent " Atomic Energy and Alternative Energies Commission; the nonaqueous electrolyte of high-voltage lithium ' be used for '; CN200980124632.6 " and foreign patent " Commissariat Energie Atomique (Fr); ' Non-aqueous electrolyte for a high-voltage lithium battery '; WO2010007223; 2010-01-21 " the applicant identical with flesh and blood, the additive of proposition is the ring-type of replacement or does not have cyclic dicarboxylic acid anhydride or dicarboxylic anhydride and carboxylic acid or dicarboxylic acids and composition thereof.When the battery initial charge, these additives can form the stably depositing thing of protectiveness on the positive electrode surface, thereby stop the further decomposition of electrolyte under high voltage, make battery can carry out normal charge and discharge cycles under high voltage.But after using these additives, the battery open circuit self-discharge rate after 14 days is still greater than 10%, generally speaking even greater than 20%, can not satisfy practical requirement well.
The additive that Chinese patent " South China Normal University, ' nonaqueous electrolytic solution and preparation method thereof that is used for high-voltage lithium ion batteries with use ', CN200910193637.6 " proposes is 2,3-dihydrofuran or 1,4-dioxy cyclic ethylene ether.When the battery initial charge, these additives can generate interfacial film in anodal surface reaction prior to electrolyte, thereby can suppress the decomposition of electrolyte under high voltage.After using these additives, the capability retention after 50 circulations of battery also can only bring up to about 75% from 64.4%.
Summary of the invention
The technical problem to be solved in the present invention is that a kind of lithium-ion battery electrolytes and preparation method thereof and purposes are provided.
Lithium-ion battery electrolytes of the present invention, its component also comprise nitrile compounds except comprising lithium salts and organic solvent; Wherein, described organic solvent is at least a in dimethyl carbonate, diethyl carbonate, ethylene carbonate, propene carbonate, methyl ethyl carbonate, carbonic acid first propyl ester, gamma-butyrolacton, gamma-valerolactone, the diethy-aceto oxalate.
Further, lithium-ion battery electrolytes of the present invention is preferably by lithium salts, organic solvent and nitrile compounds and forms.
Wherein, described lithium salts is preferably at least a in lithium hexafluoro phosphate, lithium perchlorate, lithium fluoroborate, hexafluoroarsenate lithium, trifluoromethyl sulfonic acid lithium, di-oxalate lithium borate, the oxalic acid difluoro lithium borate; Described nitrile compounds is preferably at least a in benzonitrile, benzene acetonitrile, acetonitrile, propionitrile, butyronitrile, acrylonitrile, the third two eyeballs, the adiponitrile.
Further, the addition of nitrile compounds is preferably 0.01～10wt%.
Further, the invention still further relates to the preparation method of lithium-ion battery electrolytes: with lithium salts, organic solvent and nitrile compounds mixing, namely; Or nitrile compounds joined in the common electrolyte, stir, namely; Wherein, described common electrolyte is preferably the electrolyte that comprises lithium salts and organic solvent.
Further, described common electrolyte is preferably by lithium salts and organic solvent and forms.
Further, the invention also discloses a kind of lithium ion battery, described lithium ion battery is made up of positive pole, negative pole and above-mentioned lithium-ion battery electrolytes.
Further, the invention still further relates to the purposes of described lithium-ion battery electrolytes in the preparation lithium ion battery; Wherein, described lithium ion battery is preferably high-voltage lithium ion batteries, and its voltage is preferably more than the voltage of 7.0V.When battery initial charge during to high potential, electrolyte at first decomposes at anodal surface oxidation, the free radical that produces in the decomposable process causes the polymerization reaction of nitrile compounds, formation is covered in the polynitriles film on anodal surface, in this film, π key in the itrile group (C=N) can present characteristic of semiconductor by mutual conjugation, has certain conductivity; Simultaneously, this polynitriles film is spatially kept apart positive electrode and electrolyte, has stoped the further oxidation Decomposition of electrolyte, thereby makes battery can keep stable under high voltage.
The decomposition voltage of lithium-ion battery electrolytes of the present invention can be used for preparing high-voltage battery (voltage is greater than 7.0V) greater than 7.0V; Use the assembling of this electrolyte high-voltage lithium ion batteries the moon self-discharge rate less than 5%, the capability retention after charge and discharge cycles under the 1C multiplying power 100 times can satisfy the practicability requirement greater than 90%.
Embodiment
Lithium-ion battery electrolytes of the present invention, its component also comprise nitrile compounds except comprising lithium salts and organic solvent; Wherein, described organic solvent is at least a in dimethyl carbonate, diethyl carbonate, ethylene carbonate, propene carbonate, methyl ethyl carbonate, carbonic acid first propyl ester, gamma-butyrolacton, gamma-valerolactone, the diethy-aceto oxalate.
Further, lithium-ion battery electrolytes of the present invention is preferably by lithium salts, organic solvent and nitrile compounds and forms.
Wherein, described lithium salts is preferably at least a in lithium hexafluoro phosphate, lithium perchlorate, lithium fluoroborate, hexafluoroarsenate lithium, trifluoromethyl sulfonic acid lithium, di-oxalate lithium borate, the oxalic acid difluoro lithium borate; Described nitrile compounds is preferably at least a in benzonitrile, benzene acetonitrile, acetonitrile, propionitrile, butyronitrile, acrylonitrile, the third two eyeballs, the adiponitrile.
Further, the addition of nitrile compounds is preferably 0.01～10wt%.
Further, the invention still further relates to the preparation method of lithium-ion battery electrolytes: with lithium salts, organic solvent and nitrile compounds mixing, namely; Or nitrile compounds joined in the common electrolyte, stir, namely; Wherein, described common electrolyte is preferably the electrolyte that comprises lithium salts and organic solvent.
Further, described common electrolyte is preferably by lithium salts and organic solvent and forms.
Further, the invention also discloses a kind of lithium ion battery, described lithium ion battery is made up of positive pole, negative pole and above-mentioned lithium-ion battery electrolytes.
Further, the invention still further relates to the purposes of described lithium-ion battery electrolytes in the preparation lithium ion battery; Wherein, described lithium ion battery is preferably high-voltage lithium ion batteries, and its voltage is preferably more than the voltage of 7.0V.When battery initial charge during to high potential, electrolyte at first decomposes at anodal surface oxidation, the free radical that produces in the decomposable process causes the polymerization reaction of nitrile compounds, formation is covered in the polynitriles film on anodal surface, in this film, π key in the itrile group (C=N) can present characteristic of semiconductor by mutual conjugation, has certain conductivity; Simultaneously, this polynitriles film is spatially kept apart positive electrode and electrolyte, has stoped the further oxidation Decomposition of electrolyte, thereby makes battery can keep stable under high voltage.
Be further described below in conjunction with the specific embodiment of the present invention of embodiment, therefore do not limit the present invention among the described scope of embodiments.
Embodiment 1 adopts the inventive method to prepare lithium-ion battery electrolytes and high pressure lithium ion battery
A, get the LB-301 type electrolyte that Guotai Huarong Chemical New Material Co., Ltd., Zhangjiagang City of outsourcing produces; The electrolyte of this electrolyte is the 1mol/L lithium hexafluoro phosphate, and solvent is 1/1(weight) ethylene carbonate and dimethyl carbonate mixture.
B, in above-mentioned electrolyte, add 0.1% benzonitrile and 0.1% the third two eyeballs, stir evenly, namely.
In c, the buckle type lithium-ion battery that electrolyte is applied to be made of nickel manganate cathode material for lithium, graphite cathode material, with this battery under 0.1C constant current charge to 6.0V, and under 6.0V constant voltage charge more than 5 hours.
The decomposition voltage that obtains this electrolyte through test is 7.5V; Month self-discharge rate is that the capability retention that discharges and recharges under 3.7%, the 1C after 100 times is 92%.
Embodiment 2 adopts the inventive method to prepare lithium-ion battery electrolytes and high pressure lithium ion battery
A, get the LB-302 type electrolyte that Guotai Huarong Chemical New Material Co., Ltd., Zhangjiagang City of outsourcing produces; The electrolyte of this electrolyte is the 1mol/L lithium hexafluoro phosphate, and solvent is 1/1(weight) ethylene carbonate and diethyl carbonate mixture.
B, in the above-mentioned electrolyte of 100mL, add oneself two eyeballs of 0.2g benzene acetonitrile and 0.2g, stir evenly,
Namely.
In c, the buckle type lithium-ion battery that electrolyte is applied to be made of nickel manganate cathode material for lithium, graphite cathode material, with this battery under 0.1C constant current charge to 6.0V, and under 6.0V constant voltage charge more than 5 hours.
The decomposition voltage that obtains this electrolyte after tested is 8.0V; Self-discharge rate is 4.1%; The capability retention that discharges and recharges after 100 times is 91%.
Embodiment 3 adopts the inventive method to prepare lithium-ion battery electrolytes and high pressure lithium ion battery
A, get the LB-303 type electrolyte that Guotai Huarong Chemical New Material Co., Ltd., Zhangjiagang City of outsourcing produces; The electrolyte of this electrolyte is the 1mol/L lithium hexafluoro phosphate, and solvent is 1/1/1(weight) ethylene carbonate, diethyl carbonate and dimethyl carbonate mixture.
B, in the above-mentioned electrolyte of 100mL, add 0.2g acetonitrile and 0.2g acrylonitrile, stir evenly, namely
.
In c, the buckle type lithium-ion battery that electrolyte is applied to be made of nickel manganate cathode material for lithium, graphite cathode material, with this battery under 0.1C constant current charge to 6.0V, and under 6.0V constant voltage charge more than 5 hours.
The decomposition voltage that obtains this electrolyte after tested is 7.2V; Self-discharge rate is 4.7%; The capability retention that discharges and recharges after 100 times is 90%.
Test example 1 adopts common electrolyte to prepare the high pressure lithium ion battery
The decomposition voltage of three kinds of electrolyte of outsourcing in a, the difference test implementation example 1～3, after measured, decomposition voltage is 4.3V.
B, three kinds of electrolyte of above-mentioned outsourcing are injected into respectively in the buckle type lithium-ion battery that is made of nickel manganate cathode material for lithium, graphite cathode material.
C, constant current charge is to 6.0V under 0.1C with this battery, and constant voltage charge 5 is little under 6.0V
The time more than.
D, test find that battery damages, can not regular picture.
The result shows that three of outsourcing kinds of electrolyte can not be for the preparation of the high pressure lithium ion battery of voltage greater than 6.0V among the embodiment 1～3.
Claims (9)
1. lithium-ion battery electrolytes, its component comprises lithium salts and organic solvent, it is characterized in that: its component also comprises nitrile compounds; Wherein, described organic solvent is at least a in dimethyl carbonate, diethyl carbonate, ethylene carbonate, propene carbonate, methyl ethyl carbonate, carbonic acid first propyl ester, gamma-butyrolacton, gamma-valerolactone, the diethy-aceto oxalate.
2. lithium-ion battery electrolytes according to claim 1, it is characterized in that: its component is lithium salts, organic solvent and nitrile compounds.
3. lithium-ion battery electrolytes according to claim 1 and 2 is characterized in that: described lithium salts is at least a in lithium hexafluoro phosphate, lithium perchlorate, lithium fluoroborate, hexafluoroarsenate lithium, trifluoromethyl sulfonic acid lithium, di-oxalate lithium borate, the oxalic acid difluoro lithium borate; Described nitrile compounds is at least a in benzonitrile, benzene acetonitrile, acetonitrile, propionitrile, butyronitrile, acrylonitrile, the third two eyeballs, the adiponitrile.
4. lithium-ion battery electrolytes according to claim 3, it is characterized in that: the addition of described nitrile compounds is 0.01～10wt%.
5. the preparation method of each described lithium-ion battery electrolytes of claim 1～4 is characterized in that: with lithium salts, organic solvent and nitrile compounds mixing, namely; Or nitrile compounds joined in the common electrolyte, stir, namely; Wherein, described common electrolyte is the electrolyte that comprises lithium salts and organic solvent.
6. the preparation method of lithium-ion battery electrolytes according to claim 5, it is characterized in that: described common electrolyte is made up of lithium salts and organic solvent.
7. contain the lithium ion battery of each described lithium-ion battery electrolytes of claim 1～4, it is characterized in that: described lithium ion battery is made up of positive pole, negative pole and lithium-ion battery electrolytes.
8. each described lithium-ion battery electrolytes of claim 1～4 is in the purposes of preparation in the lithium battery.
9. the application of lithium-ion battery electrolytes according to claim 8 is characterized in that: described lithium ion battery is high-voltage lithium ion batteries; The voltage of described high-voltage lithium ion batteries is greater than 7.0V.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105098246A (en) * | 2014-05-15 | 2015-11-25 | 纳米及先进材料研发院有限公司 | High voltage electrolyte and lithium ion battery |
| CN106558731A (en) * | 2015-09-28 | 2017-04-05 | 比亚迪股份有限公司 | A kind of lithium-ion battery electrolytes and lithium ion battery |
| CN108390097A (en) * | 2018-03-27 | 2018-08-10 | 清远佳致新材料研究院有限公司 | A kind of high-voltage electrolyte of the additive containing benzonitrile and preparation method thereof |
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| CN1612405A (en) * | 2003-08-20 | 2005-05-04 | 三星Sdi株式会社 | Electrolyte for rechargeable lithium battery and rechargeable lithium battery comprising same |
| CN1961451A (en) * | 2004-05-28 | 2007-05-09 | 株式会社Lg化学 | Additive for lithium secondary batteries |
| WO2007142121A1 (en) * | 2006-06-02 | 2007-12-13 | Mitsubishi Chemical Corporation | Nonaqueous electrolyte solution and nonaqueous electrolyte battery |
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2013
- 2013-06-04 CN CN2013102189494A patent/CN103280599A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1612405A (en) * | 2003-08-20 | 2005-05-04 | 三星Sdi株式会社 | Electrolyte for rechargeable lithium battery and rechargeable lithium battery comprising same |
| CN1961451A (en) * | 2004-05-28 | 2007-05-09 | 株式会社Lg化学 | Additive for lithium secondary batteries |
| WO2007142121A1 (en) * | 2006-06-02 | 2007-12-13 | Mitsubishi Chemical Corporation | Nonaqueous electrolyte solution and nonaqueous electrolyte battery |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105098246A (en) * | 2014-05-15 | 2015-11-25 | 纳米及先进材料研发院有限公司 | High voltage electrolyte and lithium ion battery |
| CN106558731A (en) * | 2015-09-28 | 2017-04-05 | 比亚迪股份有限公司 | A kind of lithium-ion battery electrolytes and lithium ion battery |
| CN106558731B (en) * | 2015-09-28 | 2019-05-17 | 比亚迪股份有限公司 | A kind of lithium-ion battery electrolytes and lithium ion battery |
| CN108390097A (en) * | 2018-03-27 | 2018-08-10 | 清远佳致新材料研究院有限公司 | A kind of high-voltage electrolyte of the additive containing benzonitrile and preparation method thereof |
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Application publication date: 20130904 |