CN104953173B - A kind of lithium-ion battery electrolytes and the lithium ion battery containing the electrolyte - Google Patents

A kind of lithium-ion battery electrolytes and the lithium ion battery containing the electrolyte Download PDF

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CN104953173B
CN104953173B CN201410123182.1A CN201410123182A CN104953173B CN 104953173 B CN104953173 B CN 104953173B CN 201410123182 A CN201410123182 A CN 201410123182A CN 104953173 B CN104953173 B CN 104953173B
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lithium
electrolyte
ion battery
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battery
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CN104953173A (en
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乔飞燕
黄荣刚
王圣
苟容
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BYD Co Ltd
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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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • 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
    • H01M10/0567—Liquid materials characterised by the additives
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2220/00—Batteries for particular applications
    • H01M2220/30—Batteries in portable systems, e.g. mobile phone, laptop
    • 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

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  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)

Abstract

The present invention provides a kind of lithium-ion battery electrolytes and containing the lithium ion battery of the electrolyte, the electrolyte includes lithium salts, nonaqueous solvents and additive；The additive is；Wherein, the R1For-CH2CF3、‑CF3、‑NO2、‑SO3, one of F and Cl；The R2For one of F and Cl；R3For one of F and Cl.Electrolyte of the invention can effectively improve stable circulation performance under serondary lithium battery high pressure, improve the discharge capacitance during circulating battery, to effectively improve the service life of lithium ion battery, the secondary lithium battery of novel high-energy metric density is prepared.

Description

A kind of lithium-ion battery electrolytes and the lithium ion battery containing the electrolyte
Technical field
The invention belongs to field of lithium ion battery more particularly to a kind of lithium-ion battery electrolytes and contain the electrolyte Lithium ion battery.
Background technique
Capacity of lithium ion battery is big, charging rate is fast, has extended cycle life, and each electron-like for being widely used in daily life is set It is standby upper.In general, the lithium ion battery of non-aqueous solute includes that cathode of lithium, the lithium salts being dissolved in organic solvent and electrochemistry are living Property positive electrode.During the charging process, lithium ion is migrated by electrolyte to cathode from anode, and it is flowed to during discharge On the contrary.The main reason for numerous studies show, shorten lithium ion battery service life is that electrode is easy under high temperature and high pressure environment It reacts with electrolyte, causes electrode material loss, electrolyte rotten, and the bulk gas many times generated can also be made At battery volume expansion, many variations are all easy to cause battery performance to deteriorate, reduced service life.
If described novel 5V high-voltage positive electrode material in Chinese patent 03135640.0, the raising of operating voltage, directly Be integrally improved battery uses power, has very big realistic meaning in application aspect.And at this stage, most of lithium electricity Pond electrolyte system can only stablize use, when operating voltage reaches 4.5v or more, electrolyte at 4.5v and voltage below System can occur oxygenolysis and then can not work normally battery, therefore, form greatly to the application of high-voltage positive electrode material Obstacle.Meanwhile the cycle performance of battery reduces.
The patent of Publication No. CN1891700A discloses a kind of halogenated cyclic sulfite high-voltage electrolyte solvent, still The circulating battery effect is undesirable.
Summary of the invention
The present invention is the technical issues of solving existing lithium-ion battery electrolytes high voltage performance and poor circulation, to mention A kind of lithium-ion battery electrolytes for high voltage performance and good cycle and contain the lithium ion battery of the electrolyte.
The present invention provides a kind of lithium-ion battery electrolytes, the electrolyte includes lithium salts, nonaqueous solvents and additive； The additive is
；
Wherein, the R1For-CH2CF3、-CF3、-NO2、-SO3, one of F and Cl；The R2For one in F and Cl Kind；R3For one of F and Cl.
The present invention also provides the preparation methods of lithium-ion battery electrolytes of the present invention, under anaerobic to appearance Nonaqueous solvents is added in device, and lithium salts and additive is then added, is mixed to get the electrolyte.
The present invention also provides a kind of lithium ion batteries, including, shell is sealed in the intracorporal battery core of the shell and electrolysis Liquid；The electrolyte is lithium-ion battery electrolytes of the present invention.
The present invention is provided in lithium-ion battery electrolytes, adds containing the organic matter for having strong electron-withdrawing group group on phenyl ring Add agent, and in o-, m-, contraposition the position of cyano, it can be replaced by other strong electronegative groups, such as nitro, sulfonic group etc., Or replaced by strong electronegative atom, such as fluorine atom, chlorine atom etc..This type organic has stable structure, with electrolyte Solvent and lithium salts does not chemically react and electrochemical reaction, can be with object as high-voltage lithium-ion battery electrolyte additive Reason form forms layer protecting film in positive electrode surface, and voltage is higher, and adsorption capacity is stronger, to protect positive electrode in charge and discharge The cycle performance of battery will not be reacted and influenced in electric process with electrolyte, or react with the decomposition product of electrolyte and Influence the cycle performance of battery.The capacity retention under high voltage cycle of high-voltage electrolyte can be improved in the electrolyte Energy, the especially capacity retention ratio under high rate charge-discharge.
Detailed description of the invention
Fig. 1 is the electrolyte oxidation decomposition electric potential figure of embodiment 1 and comparative example 1；
Fig. 2-Figure 11 is respectively the cycle efficieny figure of embodiment 1-6 and comparative example 1-4.
Specific embodiment
In order to which the technical problems, technical solutions and beneficial effects solved by the present invention is more clearly understood, below in conjunction with Embodiment, the present invention will be described in further detail.It should be appreciated that specific embodiment described herein is only used to explain The present invention is not intended to limit the present invention.
The present invention provides a kind of lithium-ion battery electrolytes, the electrolyte includes lithium salts, nonaqueous solvents and additive； The additive is
；
Wherein, the R1For-CH2CF3、-CF3、-NO2、-SO3, one of F and Cl；The R2For one in F and Cl Kind；R3For one of F and Cl.
Lithium-ion battery electrolytes of the present invention, containing benzonitrile derivative additive, the arrangement of such additives electron cloud compared with To concentrate, so that entire molecule has negative electricity, when battery charging, positive and negative anodes both sides form pressure difference, so that molecule Displacement so that anode be protected not react with electrolyte, or is reacted to positive electrode surface with the decomposition product of electrolyte.Therefore it can To improve the cycle life of battery under high voltages, the especially capacity retention ratio under high rate charge-discharge circulation.
Lithium-ion battery electrolytes of the present invention can significantly improve secondary lithium-ion electricity containing benzonitrile derivative additive Discharge capacitance in the circulation of pond electrolyte, so that high-voltage electrolyte is preferably applied in high pressure system, it is existing Though there is high-voltage electrolyte to can be applicable in high pressure system, since electrolyte can react under high voltages with positive electrode surface, To cause the capacity rapid attenuation in cyclic process, while positive electrode surface product increases the impedance of battery system., and Charge and discharge application using the electrolyte of such new additive agent for lithium ion battery under 4.5 volts and more high potential, and energy The cycle performance under high potential is enough kept, simultaneously, it is ensured that the internal resistance of battery system will not continue to increase in charge and discharge process Greatly.
Lithium-ion battery electrolytes according to the present invention, in order to further increase secondary lithium ion cell electrolyte solution Discharge capacitance in circulation, it is preferable that the additive is
、、WithAt least one of.
Lithium-ion battery electrolytes according to the present invention, it is preferable that described to add on the basis of the total weight of electrolyte The content for adding agent is 0.1-10wt%, further preferably 0.5-5wt%.
Lithium-ion battery electrolytes according to the present invention, it is preferable that by weight percentage, including,
Nonaqueous solvents 80-95%
Lithium salts 1-20%
Additive 0.1-10%.
Further preferably are as follows:
Nonaqueous solvents 80-85%
Lithium salts 13-17%
Additive 0.5-5%.
Lithium-ion battery electrolytes according to the present invention, it is preferable that the nonaqueous solvents be fluorinated ethylene carbonate, Propene carbonate, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, methyl formate, methyl acetate, methyl propionate, acetic acid second Ester, 1,3- propane sultone, sulfuric acid vinyl ester, sulfuric acid acrylic ester, ethylene sulfite, propylene sulfite, adiponitrile and The mixing of one or more of succinonitrile；The lithium salts is LiPF6、LiClO4、LiBF4、LiAsF6、LiSiF6、LiAlCl4、 LiBOB、LiODFB、LiCl、LiBr、LiI、LiCF3SO3、Li(CF3SO2)3、Li(CF3CO2)2N、Li(CF3SO2)2N、Li (SO2C2F5)2N and Li (SO3CF3)2The mixing of one or more of N.
Lithium-ion battery electrolytes according to the present invention, it is preferable that the nonaqueous solvents is fluorinated ethylene carbonate And methyl ethyl carbonate；The lithium salts is LiPF6。
The present invention also provides a kind of preparation methods of lithium-ion battery electrolytes that the present invention states, under anaerobic to Nonaqueous solvents is added in container, and lithium salts and additive is then added, is mixed to get the electrolyte.
The present invention also provides a kind of lithium ion batteries, including, shell is sealed in the intracorporal battery core of the shell and electrolysis Liquid；The electrolyte is lithium-ion battery electrolytes of the present invention.
The present invention is further described in detail for Application Example below.
Embodiment 1
1, electrolyte is prepared
FEC and EMC is uniformly mixed and obtains solvent respectively in glove box, and LiPF is then added6With to trifluoromethylbenzene first Nitrile obtains electrolyte A1.FEC:EMC=3:7(V:V), LiPF6Concentration be 1mol.L-1,
Solvent: LiPF6: to trifluoromethylbenzonitrile=85:14:1.
2, lithium ion battery is prepared
With the positive electrode (LiNi of 70:15:150.5Mn1.5O4), conductive agent (acetylene black), binder (PVDF) preparation just Pole, using lithium piece as cathode, electrolyte is electrolyte A1, is assembled in argon gas glove box using Celgard2300 type micro-pore septum At button cell S1.
Embodiment 2
1, electrolyte is prepared
FEC and EMC is uniformly mixed and obtains solvent respectively in glove box, and LiPF is then added6With to trifluoromethylbenzene first Nitrile obtains electrolyte A2.FEC:EMC=3:7 (V:V), LiPF6Concentration be 1mol.L-1,
Solvent: LiPF6: to trifluoromethylbenzonitrile=82:13:5.
2, lithium ion battery is prepared
With the positive electrode (LiNi of 80:10:100.5Mn1.5O4), conductive agent (acetylene black), binder (PVDF) preparation just Pole, using lithium piece as cathode, electrolyte is electrolyte A2, is assembled in argon gas glove box using Celgard2300 type micro-pore septum At button cell S2.
Embodiment 3
1, electrolyte is prepared
FEC and EMC is uniformly mixed and obtains solvent respectively in glove box, and LiPF is then added6With to trifluoromethylbenzene first Nitrile obtains electrolyte A3.FEC:EMC=3:7 (V:V), LiPF6Concentration be 1mol.L-1,
Solvent: LiPF6: to trifluoromethylbenzonitrile=86:4:10.
2, lithium ion battery is prepared
With the positive electrode (LiNi of 90:5:50.5Mn1.5O4), conductive agent (acetylene black), binder (PVDF) preparation anode, Using lithium piece as cathode, electrolyte is electrolyte A3, is assembled into and is buckled in argon gas glove box using Celgard2300 type micro-pore septum Formula battery S3.
Embodiment 4
1, electrolyte is prepared
FEC and EMC is uniformly mixed and obtains solvent respectively in glove box, and LiPF is then added6With to trifluoromethylbenzene first Nitrile obtains electrolyte A4.FEC:EMC=3:7 (V:V), LiPF6Concentration be 1mol.L-1,
Solvent: LiPF6: to nitro-benzonitrile=82.5:17:0.5.
2, lithium ion battery is prepared
With the positive electrode (LiNi of 80:10:100.5Mn1.5O4), conductive agent (acetylene black), binder (PVDF) preparation just Pole, using lithium piece as cathode, electrolyte is electrolyte A4, is assembled in argon gas glove box using Celgard2300 type micro-pore septum At button cell S4.
Embodiment 5
1, electrolyte is prepared
FEC and EMC is uniformly mixed and obtains solvent respectively in glove box, and LiPF is then added6With to trifluoromethylbenzene first Nitrile obtains electrolyte A5.FEC:EMC=3:7 (V:V), LiPF6Concentration be 1mol.L-1,
Solvent: LiPF6: p-sulfonic acid base-benzonitrile=95:1:4.
2, lithium ion battery is prepared
With the positive electrode (LiNi of 90:5:50.5Mn1.5O4), conductive agent (acetylene black), binder (PVDF) preparation anode, Using lithium piece as cathode, electrolyte is electrolyte A5, is assembled into and is buckled in argon gas glove box using Celgard2300 type micro-pore septum Formula battery S5.
Embodiment 6
1, electrolyte is prepared
FEC and EMC is uniformly mixed and obtains solvent respectively in glove box, and LiPF is then added6With to trifluoromethylbenzene first Nitrile obtains electrolyte A6.FEC:EMC=3:7 (V:V), LiPF6Concentration be 1mol.L-1,
Solvent: LiPF6: 2,3-2 fluorine substituted benzene formonitrile HCNs=80:19.9:0.1.
2, lithium ion battery is prepared
With the positive electrode (LiNi of 90:5:50.5Mn1.5O4), conductive agent (acetylene black), binder (PVDF) preparation anode, Using lithium piece as cathode, electrolyte is electrolyte A6, is assembled into and is buckled in argon gas glove box using Celgard2300 type micro-pore septum Formula battery S6.
Comparative example 1
1, electrolyte is prepared
FEC and EMC is uniformly mixed and obtains solvent respectively in glove box, and LiPF is then added6Obtain electrolyte CA1. FEC:EMC=3:7 (V:V), LiPF6Concentration be 1mol.L-1, solvent: LiPF6 =86:14。
2, lithium ion battery is prepared
With the positive electrode (LiNi of 70:15:150.5Mn1.5O4), conductive agent (acetylene black), binder (PVDF) preparation just Pole, using lithium piece as cathode, electrolyte is electrolyte CA1, is assembled in argon gas glove box using Celgard2300 type micro-pore septum At button cell CS1.
Comparative example 2
1, electrolyte is prepared
FEC and EMC is uniformly mixed and obtains solvent respectively in glove box, and LiPF is then added6, obtain electrolyte CA2. FEC:EMC=3:7 (V:V), LiPF6Concentration be 1mol.L-1, solvent: LiPF6 =86:14。
2, lithium ion battery is prepared
With the positive electrode (LiNi of 80:10:100.5Mn1.5O4), conductive agent (acetylene black), binder (PVDF) preparation just Pole, using lithium piece as cathode, electrolyte is electrolyte CA2, is assembled in argon gas glove box using Celgard2300 type micro-pore septum At button cell CS2.
Comparative example 3
1, electrolyte is prepared
FEC and EMC is uniformly mixed and obtains solvent respectively in glove box, and LiPF is then added6, obtain electrolyte AC3. FEC:EMC=3:7 (V:V), LiPF6Concentration be 1mol.L-1, solvent: LiPF6 =86:14。
2, lithium ion battery is prepared
With the positive electrode (LiNi of 90:5:50.5Mn1.5O4), conductive agent (acetylene black), binder (PVDF) preparation anode, Using lithium piece as cathode, electrolyte is electrolyte CA3, is assembled into argon gas glove box using Celgard2300 type micro-pore septum Button cell CS3.
Comparative example 4
Electrolyte, electrolyte are prepared using the placement in CN1891700A are as follows: 1mol/L LiPF6/ CIPS+EC+DMC(body Product is than being 10:40:50)
Lithium ion battery CS4 is prepared using the method for embodiment 1.
Performance test
1, specific capacity is tested
Specific capacity test is carried out using BK6V1 battery testing cabinet button type battery, test work step is first to fill with 0.1mA constant current Electricity ends to 4.95V, and rear constant voltage continues to charge to electric current as 0.005A stopping.Battery shelves 5Min, with constant current 0.1mA into Row is discharged to voltage as 3.0V cut-off.I.e. if being shown in Table 1.
2, electrolyte oxidation decomposition electric potential is tested
The electrolyte of embodiment 1 and comparative example 1 is subjected to electrolyte oxidation decomposition respectively using occasion China electrochemical workstation Potential test prepares three electrodes, and working electrode is platinum electrode, reference electrode and uses lithium piece, electrolyte test to electrode Open-circuit voltage, under open-circuit voltage, Applied Electrochemistry work station selects linear sweep voltammetry (LSV) to be tested, cut-off electricity Pressure is 7.0 V.The result is shown in Figure 1.
3, cycle performance is tested
Cycle efficieny test is carried out using BK6V1 battery testing cabinet button type battery, charge and discharge, test are carried out with 1C multiplying power Work step is first to be ended with 1C multiplying power constant-current charge to 4.95V, and rear constant voltage continues to charge to electric current as 0.005A stopping.Battery is put 5Min is set, be discharged to voltage with constant current 1C multiplying power as 3.0V cut-off.As a result see Fig. 2-Figure 11.
Table 1
。
The charge specific capacity of the battery of embodiment, specific discharge capacity and efficiency are all than comparative example as can be seen from Table 1 It is better, it is high from specific capacity and specific discharge capacity to illustrate that the battery with electrolyte of the invention has.
As can be seen from Figure 1 by electric potential scanning result it is found that the high-voltage electrolyte decomposition electric potential of comparative example 1 is up to 5.5V Left and right, and the electrolyte containing the embodiment 1 to methyl benzonitrile, oxygenolysis current potential show better oxidative resistance, Reach 6V.Meanwhile containing the high-voltage electrolyte to methyl benzonitrile in entire oxidizing potential section, not seeing has apparent oxygen Change peak to occur, illustrating additive not influences the oxygenolysis current potential of electrolyte, on the contrary, which raises the oxygenolysis of electrolyte electricity Position, illustrate its anode suction-operated be apparent.
As can be seen that being tested by charge and discharge cycles from Fig. 2-Figure 11, use in the battery of embodiment 1-6 containing addition Agent is to the electrolyte of methyl benzonitrile, and battery discharge specific capacity can be reached for 130mAh.g for the first time-1, recycle 100 times, electric discharge is held Measuring conservation rate is 90%, and is free of the electrolyte of additive, and battery discharge specific capacity can also reach 130 mAh.g for the first time-1, but follow After ring 100 times, discovery will decay since circulation, and quickly, when to 100 times, capacity retention ratio only has 50% for decaying.
To sum up, electrolyte of the invention can effectively improve stable circulation performance under serondary lithium battery high pressure, improve electricity Discharge capacitance in the cyclic process of pond prepares novel high-energy to effectively improve the service life of lithium ion battery The secondary lithium battery of metric density.
The foregoing is merely illustrative of the preferred embodiments of the present invention, is not intended to limit the invention, all in essence of the invention Made any modifications, equivalent replacements, and improvements etc., should all be included in the protection scope of the present invention within mind and principle.

Claims (6)

1. a kind of lithium-ion battery electrolytes, which is characterized in that the electrolyte includes lithium salts, nonaqueous solvents and additive；Institute Stating additive is
At least one of；
Wherein, by weight percentage, including,
Nonaqueous solvents 80-95%；
Lithium salts 1-20%；
Additive 0.1-10%.
2. lithium-ion battery electrolytes according to claim 1, which is characterized in that on the basis of the total weight of electrolyte, The content of the additive is 0.5-5wt%.
3. lithium-ion battery electrolytes according to claim 1, which is characterized in that the nonaqueous solvents is fluoro carbonic acid second Enester, propene carbonate, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, methyl formate, methyl acetate, methyl propionate, Ethyl acetate, 1,3- propane sultone, sulfuric acid vinyl ester, sulfuric acid acrylic ester, ethylene sulfite, propylene sulfite, oneself The mixing of one or more of dintrile and succinonitrile；The lithium salts is LiPF6、LiClO4、LiBF4、LiAsF6、LiSiF6、 LiAlCl4、LiBOB、LiODFB、LiCl、LiBr、LiI、LiCF3SO3、Li(CF3SO2)3、Li(CF3CO2)2N、Li(CF3SO2)2N、Li(SO2C2F5)2N and Li (SO3CF3)2The mixing of one or more of N.
4. lithium-ion battery electrolytes according to claim 3, the nonaqueous solvents is fluorinated ethylene carbonate and carbonic acid Methyl ethyl ester；The lithium salts is LiPF6。
5. a kind of preparation method of lithium-ion battery electrolytes described in claim 1-4 any one, which is characterized in that in nothing Nonaqueous solvents is added to container under the conditions of oxygen, lithium salts and additive is then added, is mixed to get the electrolyte.
6. a kind of lithium ion battery, including, shell is sealed in the intracorporal battery core of the shell and electrolyte；The electrolyte is power Benefit requires the described in any item lithium-ion battery electrolytes of 1-4.
CN201410123182.1A 2014-03-28 2014-03-28 A kind of lithium-ion battery electrolytes and the lithium ion battery containing the electrolyte Active CN104953173B (en)

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