CN107946643A - A kind of high-performance lithium battery electrolyte - Google Patents
A kind of high-performance lithium battery electrolyte Download PDFInfo
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- CN107946643A CN107946643A CN201711123982.3A CN201711123982A CN107946643A CN 107946643 A CN107946643 A CN 107946643A CN 201711123982 A CN201711123982 A CN 201711123982A CN 107946643 A CN107946643 A CN 107946643A
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- battery
- electrolyte
- lithium battery
- organic solvent
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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
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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
- H01M10/052—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
- 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
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
-
- 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
Abstract
A kind of high-performance lithium battery electrolyte, belongs to the technical field of lithium battery electrolytes, including lithium salts and organic solvent, further includes compoundAnd/orWherein R1Selected from alkyl, H or F, R2Selected from pi-allyl, propargyl or benzene.Battery electrolyte of the present invention reduces the generation of side reaction, so as to reduce battery flatulence, improves battery cycle life due to the addition of above-mentioned substance so that electrolysis liquid energy effectively improves the charge-discharge performance of lithium battery.
Description
Technical field
The invention belongs to the technical field of lithium battery electrolytes, is related to a kind of heat safe lithium battery electrolytes.The present invention
Battery electrolyte can increase battery cycle performance at high temperature and restorability, the collocation of electrolyte component of the present invention cause
Electrolysis liquid energy effectively improves the charge-discharge performance of lithium battery, reduces the generation of side reaction, so as to reduce battery flatulence, improves electricity
Pond cycle life.
Background technology
Lithium ion battery because it has the advantages that operating voltage is high, energy density is high, environmental-friendly, stable circulation, safe,
It is widely used in the various electronic equipments of laptop, mobile phone, MP4 etc..But with battery capacity in electronic equipment
Improve, people it is also proposed the operating voltage and energy density of lithium ion battery the requirement of higher.But with working environment
Moisture temperature requirement is improved, in electrolyte the excessive reaction for causing itself and electrolyte of water content also accelerate therewith, produce HF
It is serious to ultimately result in inflatable under room temperature and high temperature, cycle performance reduces, and seriously constrains the performance of battery performance.
Electrolyte is the important component of battery, carries and ion is transmitted between positive and negative electrode by inside battery
Effect, its capacity, operating temperature range, cycle performance and security performance to battery etc. has important influence.Electrolyte is general
It is divided into two class of liquid electrolyte and solid electrolyte, need to meets following basic demand：(1) high ionic conductivity, should generally reach
To 1 × 10-3-2×10-2S/cm；(2) high heat endurance and chemical stability, do not occur point within the scope of wider temperature
Solution；(3) wider electrochemical window, keeps the stabilization of chemical property in wider voltage range；(4) with the other portions of battery
Dividing has good compatibility；(5) it is safe and nontoxic, pollution-free.
Liquid organic solution liquid is the most commonly used, but is constantly widened with the application range of battery, and people are to battery
The requirement of each side is continuously increased, and original electrolyte system cannot meet requirement.
The content of the invention
The present invention is to solve the above problems, devise a kind of electrolyte of high-temperature-reslithium lithium battery, by adding into electrolyte
Enter material of the present invention so that electrolysis liquid energy effectively improves the charge-discharge performance of lithium battery, and energy density increase, improves electricity
The high/low temperature cycle performance in pond, improves battery cycle life.
The present invention is to realize that the technical solution that its purpose uses is：
A kind of high-performance lithium battery electrolyte, including lithium salts and organic solvent, further include compoundAnd/orWherein R1Selected from alkyl, H or F, R2
Selected from pi-allyl, propargyl or benzene.
CompoundAnd/orTotal dosage be
Electrolyte quality 0.05-0.8%.
The organic solvent includes cyclic carbonate and/or linear carbonate.Such as ethylene carbonate, carbonic acid diformazan
Ester, methyl ethyl ester etc..
The lithium salts is selected from inorganic anion electrolyte lithium salt and/or organic anion electrolyte lithium salt.
The concentration of lithium salts in organic solvent is 1-1.5mol/L.
Further include double (triethoxy silicon substrate) ethane of 1,2-.
The beneficial effects of the invention are as follows：
Electrolyte of the present invention, due to addingAnd/orCompound, on the basis of its formation efficiency and scattered thermoelectricity pressure is improved, increases the solubility of solute, carries
High conductivity, reduces ratio resistance, so as to improve the service life of product, while improves the speed of growth of oxide-film, suppresses oxidation
The aquation of film, improves the high temperature performance of electrolyte.
1,2- double (triethoxy silicon substrate) ethane, to improve dissolubility, prevent solute in crystallization analysis under cryogenic
Go out, influence the cryogenic property of electrolyte；It can causeAnd/orThe effect of compound, is more preferable, synergistic effect, can solve the appearance because caused by long-time uses battery
The problem of amount declines, by control double (triethoxy silicon substrate) ethane of 1,2- withAnd/orThe mass ratio of compound is 1：(0.1-
0.3) so that electrical conductivity variation with temperature is relatively stable, meanwhile, the addition of 1,2- double (triethoxy silicon substrate) ethane can be into one
Step solves the problems, such as the swelling of battery, while can improve chemical stability, the addition of 1,2- double (triethoxy silicon substrate) ethane and ratio
Example control, strengthens the performance of lithium salts, can further reduce the resistance of solution and increase the degree of ionization of lithium ion, while increase molten
Liquid intermediate ion transport number.
The addition of double (triethoxy silicon substrate) ethane of 1,2- withAnd/orCompound is used in combination, and can also improve the discharge performance under battery high magnification；1,2- is double at the same time
The addition of (triethoxy silicon substrate) ethane interacts with organic solvent, improves deliquescent at the same time it can also improving electrode mistake
The invertibity of journey, reduces active material on electrode and comes off, reduce activation polarization, extend battery cycle life more than 1.5 times.
Brief description of the drawings
Fig. 1 is high temperature cyclic performance figure at 65 DEG C of battery.
Fig. 2 is battery high-temperature stability comparison diagram.
Fig. 3 is battery impedance performance map.
Wherein, soft-package battery 600mAh, positive electrode：4.35V LiNi0.5Co0.2Mn0.3O2, negative material：Silicon-carbon cathode
(Si 5%), basic electrolyte：EC/EMC/DEC,LiPF6:Based on 1M additive VC AND, BASE, BASE+ADD is addition
After sulfonic acid additive product.
Embodiment
With reference to specific embodiment, the present invention is described further.
First, specific embodiment
Embodiment 1
High temp resistance lithium ion cell electrolyte, including by volume ratio be 6:3:1 ethylene carbonate, dimethyl carbonate, carbon
The organic solvent that acid methyl ethyl ester is formed；Account for the LiPF that organic solvent concentration is 1mol/L6Lithium salts；Account for the battery electrolyte matter
The Glycol dibenzenesulfonate of amount 0.05%.
Embodiment 2
High temp resistance lithium ion cell electrolyte, including by volume ratio be 4:3:3 ethylene carbonate, dimethyl carbonate, carbon
The organic solvent that acid methyl ethyl ester is formed；Account for the LiBF that organic solvent concentration is 1.5mol/L4Lithium salts；Account for the battery electrolyte
The benzene sulfonic acid phenyl ester of quality 0.08%.
Embodiment 3
High temp resistance lithium ion cell electrolyte, including by volume ratio be 3:4:3 ethylene carbonate, dimethyl carbonate, carbon
The organic solvent that acid methyl ethyl ester is formed；Account for the Li (CF that organic solvent concentration is 1.3mol/L3SO2)N2Lithium salts；Account for the battery
The benzene sulfonic acid allyl ester of electrolyte quality 0.1%.
Embodiment 4
High temp resistance lithium ion cell electrolyte, including by volume ratio be 2:7:1 ethylene carbonate, dimethyl carbonate, carbon
The organic solvent that acid methyl ethyl ester is formed；Account for the Li (CF that organic solvent concentration is 1.2mol/L3SO2)N2Lithium salts；Account for the battery
The benzene sulfonic acid alkynes propyl ester of electrolyte quality 0.3%.
Embodiment 5
High temp resistance lithium ion cell electrolyte, including by volume ratio be 2:4:4 ethylene carbonate, two (fluoroform of carbonic acid
Alcohol) ester, methyl ethyl ester form organic solvent；Account for the LiPF that organic solvent concentration is 1.4mol/L6Mixed with LiBOB
Lithium salts, LiPF6Molar ratio with LiBOB is 3:4；Account for two sym-toluenesulfonic acid of ethylene glycol of the battery electrolyte quality 0.3%
Ester.Using mixing lithium salts, especially LiPF6With being used in mixed way for LiBOB lithium salts, can improve electrolyte chemical property and
Cycle performance, is used in mixed way, since the electron delocalizationization effect of LiBOB lithium salts is strong so that mix the electrical conductivity height of lithium salts, help
In the raising of battery electrochemical stability and heat endurance.
The chemical structural formula of two sym-toluenesulfonic acid ester of ethylene glycol is：
Embodiment 6
High temp resistance lithium ion cell electrolyte, including by volume ratio be 1:6:3 ethylene carbonate, dimethyl carbonate, carbon
The organic solvent that acid methyl ethyl ester is formed；Account for the LiPF that organic solvent concentration is 1mol/L6Lithium salts；Account for the battery electrolyte matter
The Glycol dibenzenesulfonate of amount 0.05%；Account for double (triethoxy silicon substrate) ethane of 1,2- of the electrolyte quality 0.5%.Due to
LiPF6Lithium salts has stronger hygroscopicity, easily produces security risk in high temperature or high current density, pyrolysis stability compared with
The effect of difference, the addition of 1,2- double (triethoxy silicon substrate) ethane can cause Glycol dibenzenesulfonate, is more preferable, both cooperate with
Effect, can solve the problems, such as that capacity declines because caused by long-time uses battery, by controlling the double (triethoxysilicanes of 1,2-
Base) mass ratio of ethane and Glycol dibenzenesulfonate is 1：(0.1-0.3) so that electrical conductivity variation with temperature is more steady
It is fixed, meanwhile, the addition of 1,2- double (triethoxy silicon substrate) ethane can further solve the problems, such as the swelling of battery, while can raising
Stability is learned, the addition of 1,2- double (triethoxy silicon substrate) ethane can also further reduce the resistance of solution and increase lithium ion
Degree of ionization, while increase effects of ion transport number.
Embodiment 7
High temp resistance lithium ion cell electrolyte, including by volume ratio be 7:2:1 ethylene carbonate, two ethyl of carbonic acid,
The organic solvent that methyl ethyl ester is formed；Account for the Li (CF that organic solvent concentration is 1.0mol/L3SO2)N2Mixed with LiBMB
Lithium salts, wherein Li (CF3SO2)N2Molar ratio with LiBMB is 4:3；Account for the benzene sulfonic acid allyl of the battery electrolyte quality 0.5%
Ester；Account for double (triethoxy silicon substrate) ethane of 1,2- of the battery electrolyte quality 1.7%.Using mixing lithium salts, especially Li
(CF3SO2)N2With being used in mixed way for LiBMB lithium salts, the chemical property and cycle performance of electrolyte can be improved, is used in mixed way,
Since the electron delocalizationization effect of LiBMB lithium salts is strong so that mix the electrical conductivity height of lithium salts, contribute to battery electrochemical stability
With the raising of heat endurance.Due to Li (CF3SO2)N2Lithium salts easily produces security risk in high temperature or high current density, pyrolysis
The effect of stability is poor, and the addition of 1,2- double (triethoxy silicon substrate) ethane can cause benzene sulfonic acid allyl ester is more preferable, both
Synergistic effect, can solve the problems, such as that capacity declines because caused by long-time uses battery, by controlling double (three ethoxies of 1,2-
Base silicon substrate) mass ratio of ethane and benzene sulfonic acid allyl ester is 1：(0.1-0.3) so that electrical conductivity variation with temperature is more steady
It is fixed, meanwhile, the addition of 1,2- double (triethoxy silicon substrate) ethane can further solve the problems, such as the swelling of battery, while can raising
Stability is learned, the addition of 1,2- double (triethoxy silicon substrate) ethane, effect more has in compound lithium salts, can also further reduce molten
The resistance of liquid and the degree of ionization for increasing lithium ion, while increase effects of ion transport number.
Embodiment 8
High temp resistance lithium ion cell electrolyte, including by volume ratio be 3:2:5 propene carbonate, ethylene carbonate, carbon
The organic solvent that acid methyl ethyl ester is formed；Account for the Li (CF that organic solvent concentration is 1.1mol/L3SO2)3Lithium salts；Account for the battery
The equal trifluoro benzene sulfonate of ethylene glycol two of electrolyte quality 0.8%.
The chemical structural formula of the equal trifluoro benzene sulfonate of ethylene glycol two is：
Embodiment 9
High temp resistance lithium ion cell electrolyte, including by volume ratio be 4:2:4 ethylene carbonate, two (fluoroform of carbonic acid
Alcohol) ester, methyl ethyl ester form organic solvent；Account for the LiPF that organic solvent concentration is 1.4mol/L6Mixed with LiBOB
Lithium salts, LiPF6Molar ratio with LiBOB is 3:4；Account for the benzene sulfonic acid phenyl ester of the battery electrolyte quality 0.3%；Account for battery electricity
Solve double (triethoxy silicon substrate) ethane of 1,2- of liquid quality 1.5%.Due to LiPF6Lithium salts has stronger hygroscopicity, in high temperature
Or security risk is easily produced during high current density, pyrolysis stability is poor, the addition of 1,2- double (triethoxy silicon substrate) ethane
The effect of can causing benzene sulfonic acid phenyl ester, is more preferable, and the effect is not only more preferable including high/low temperature cycle performance, and further including prevents box hat
The effect of corrosion, is double, both act synergistically, and can solve the problems, such as that capacity declines because caused by long-time uses battery, leads to
It is 1 to cross and control double (triethoxy silicon substrate) ethane of 1,2- and the mass ratio of benzene sulfonic acid phenyl ester：(0.1-0.3) so that electrical conductivity with
The change of temperature is relatively stable, meanwhile, the addition of 1,2- double (triethoxy silicon substrate) ethane can further solve the swelling of battery
Problem, while chemical stability can be improved, the addition of 1,2- double (triethoxy silicon substrate) ethane can also further reduce solution
Resistance and the degree of ionization for increasing lithium ion, while increase effects of ion transport number.
2nd, performance test
1st, cycle performance test will be carried out after the electrolyte difference assembled battery of the present invention, method is as follows：With
LiNi0.5Co0.2Mn0.3O2For positive electrode, anode uses silicon-carbon cathode (Si 5%), positive and negative anodes collector be distributed as aluminium foil and
Copper foil, membrane after injecting electrolyte, are assembled into soft-package battery in glove box, are stood 8 using ceramic diaphragm composition soft-package battery
Tested after hour.Discharge and recharge is carried out under 25 DEG C of constant temperature of room temperature respectively with 1/10C 3.0V to 4.45V to live to battery
Change, then the circulation under normal temperature condition is with 1C discharge and recharges.Loop test the results are shown in Table 1.
Table 1
2nd, battery discharge conservation rate under different multiplying：By battery with 0.5C constant-current discharges to 3.0V, shelve 5min, then with
0.5C constant-current charges are to 4.4V, and constant-voltage charge, are 0.05C by electric current, stand 5min, then permanent with 0.2C, 1.5C, 2C respectively
Stream is discharged to by voltage 3.0V.Discharge capacity under the conditions of record 0.2C, 1.5C, 2C is D1, and the electric discharge recorded under 0.2C is held
Measure as D0, and based on the discharge capacity under 0.2C, pass through discharge capacitance=[(D1-D0)/D0] × 100% of battery
Discharge capacitance (survey 15 batteries, take its average value) of the battery under different multiplying, each battery is calculated in formula
Discharge capacitance under 25 DEG C of conditions, different multiplying is as shown in table 2.
Table 2
3rd, battery low-temperature storage performance evaluation；Table 3 below is that battery is shelved in cryogenic box, respectively controlled at -30
DEG C or -40 DEG C, shelve time 240min, then measure battery capacity retention ratio.
Table 3
4th, hot tank is tested：Battery carries out following tests：
1) battery is charged to by 4.4V with the constant current of 1.0C electric currents, then constant-voltage charge to electric current is down to 0.05C, and charging stops
Only；2) battery is placed in hot tank, is started to warm up with the programming rate of 5 DEG C/min from 25 DEG C to 180 DEG C, tieed up after reaching 180 DEG C
Hold temperature-resistant, then start timing, the state of battery is observed after 1h, is by the standard of the test：Without smoldering, nothing rises battery
Fire, no explosion, wherein every group of 10 batteries.The results are shown in Table 4 for the hot tank test of each battery.Surveyed by above-mentioned hot tank
Examination, characterizes the security performance of battery.
Table 4
| Project | State after hot tank test |
| Embodiment 1 | 10 batteries are not by smoldering, being on fire, explosion phenomenon |
| Embodiment 2 | 10 batteries are not by smoldering, being on fire, explosion phenomenon |
| Embodiment 3 | 10 batteries are not by smoldering, being on fire, explosion phenomenon |
| Embodiment 4 | 10 batteries are not by smoldering, being on fire, explosion phenomenon |
| Embodiment 5 | 10 batteries are not by smoldering, being on fire, explosion phenomenon |
| Embodiment 6 | 10 batteries are not by smoldering, being on fire, explosion phenomenon |
| Embodiment 7 | 10 batteries are not by smoldering, being on fire, explosion phenomenon |
| Embodiment 8 | 10 batteries are not by smoldering, being on fire, explosion phenomenon |
| Embodiment 9 | 10 batteries are not by smoldering, being on fire, explosion phenomenon |
5th, anticorrosive property
Immersed respectively after 18650 lithium ion battery box hats are weighed above-described embodiment 1-9 prevent box hat corrode lithium from
In sub- battery electrolyte, the lithium-ion battery electrolytes for preventing box hat corrosion of 18650 lithium ion battery box hats and embodiment 1-9
Open wide and be positioned under room temperature environment, 100 it is small when after 18650 lithium ion battery box hats cleaned into drying weigh, calculate 18650 lithiums from
The rate of weight loss of sub- battery steel shell, the results are shown in Table 5.
Table 5
| Project | It is preceding heavy | After weigh | Rate of weight loss % |
| Embodiment 1 | 7.6589 | 7.6575 | 0.018 |
| Embodiment 2 | 7.3624 | 7.3610 | 0.019 |
| Embodiment 3 | 7.5386 | 7.5373 | 0.017 |
| Embodiment 4 | 7.6676 | 7.6660 | 0.021 |
| Embodiment 5 | 7.5743 | 7.5734 | 0.012 |
| Embodiment 6 | 7.7338 | 7.7331 | 0.009 |
| Embodiment 7 | 7.6982 | 7.6977 | 0.006 |
| Embodiment 8 | 7.7523 | 7.7510 | 0.017 |
| Embodiment 9 | 7.7948 | 7.7944 | 0.005 |
Claims (6)
1. a kind of high-performance lithium battery electrolyte, including lithium salts and organic solvent, it is characterised in that further include compoundAnd/orWherein R1Selected from alkyl, H or F, R2
Selected from pi-allyl, propargyl or benzene.
A kind of 2. high-performance lithium battery electrolyte according to claim 1, it is characterised in that：CompoundAnd/orDosage be electrolyte quality 0.05-
0.8%.
A kind of 3. high-performance lithium battery electrolyte according to claim 1, it is characterised in that：The organic solvent includes
Cyclic carbonate and/or linear carbonate.
A kind of 4. high-performance lithium battery electrolyte according to claim 1, it is characterised in that：The inorganic anion electricity
Solve matter lithium salts and/or organic anion electrolyte lithium salt.
A kind of 5. high-performance lithium battery electrolyte according to claim 1, it is characterised in that：Lithium salts is in organic solvent
Concentration is 1-1.5mol/L.
A kind of 6. high-performance lithium battery electrolyte according to claim 1, it is characterised in that：Further include double (three second of 1,2-
Epoxide silicon substrate) ethane.
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