CN107706455A - A kind of high voltage multiplying power electrolyte for taking into account high temperature performance and the lithium ion battery using the electrolyte - Google Patents
A kind of high voltage multiplying power electrolyte for taking into account high temperature performance and the lithium ion battery using the electrolyte Download PDFInfo
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- CN107706455A CN107706455A CN201710851205.4A CN201710851205A CN107706455A CN 107706455 A CN107706455 A CN 107706455A CN 201710851205 A CN201710851205 A CN 201710851205A CN 107706455 A CN107706455 A CN 107706455A
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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
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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
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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
- H01M10/0569—Liquid materials characterised by the solvents
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
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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
- 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 lithium ion battery the invention discloses high voltage multiplying power electrolyte for taking into account high temperature performance and using the electrolyte.The electrolyte includes nonaqueous solvents, it is dissolved in the lithium salts and additive of the non-aqueous organic solvent, wherein, the non-aqueous organic solvent contains propene carbonate (PC) and wire carboxylate, and the additive includes citraconic anhydride, difluorophosphate (LiPO2F2), fluorinated ethylene carbonate, sulfuric acid vinyl ester and 1,2 2 (2 cyanoethoxyl) ethane.By cooperative effect caused by the dicyandiamide solution and additive optimum organization use, for lithium ion battery, battery can be made still to keep excellent cycle life, cryogenic discharging characteristic and high-temperature storage characteristics under high voltage multiplying power.
Description
Technical field
The present invention relates to lithium ion battery preparing technical field, and in particular to a kind of high voltage for taking into account high temperature performance times
Rate electrolyte and the lithium ion battery using the electrolyte.
Background technology
Lithium ion battery is the battery of a new generation's most competitiveness, with operating voltage is high, specific capacity is big, cycle life
Long, memory-less effect and advantages of environment protection, are widely used in the fields such as number, energy storage, power and militay space flight aviation.
In recent years, lithium ion battery has achieved immense success in high-energy battery field, but consumer still can have meet high/low temperature,
The comprehensive battery of high voltage rate combination property emerges, and this depends on the research to new electrolyte system and additive and opened
Hair.
Lithium ion battery high and low temperature performance is mainly influenceed by following several factors：(1), in high temperature high voltage, positive pole
The dissolution of metal ion exacerbates the catalytic decomposition to electrolyte, and decomposition gas product directly results in cell thickness expansion, solid
Product deposits at both positive and negative polarity interface, increases the internal resistance of cell, reduces the conservation rate of capacity；(2), the LiPF in electrolyte6High temperature pole
Easily decompose, produce HF and PF5.Wherein HF can corrode positive pole, cause the dissolution of metal ion, so as to destroy cathode material structure,
Capacity is caused to be lost in；(3), under high voltages, electrolyte is easily oxidized in positive pole, causes the metal ion of positive active material
Easily it is reduced and dissolution, so as to destroy cathode material structure, causes capacitance loss (4) battery in initial charge into electrolyte
When the SEI films that are formed decompose under the high temperature conditions, the metal ion of dissolution to electrolyte, easily propagate through SEI and reach negative pole
Obtain electronics and be reduced into metal simple-substance, cause battery performance drastically to decline so as to destroy SEI structure, cathode impedance is not
Disconnected increase, self-discharge of battery aggravation, irreversible capacity increase, performance cycle deteriorate；(5), lithium-ion battery electrolytes solvent group
Conjunction, solvent freezing point, solvent low temperature viscosity, it can directly determine to arrive the performance of lithium ion battery ion under cryogenic；(6)、
Battery cryogenic property is played the interfacial film impedance value that lithium-ion battery electrolytes additive is decomposed to form and new lithium salts conductance
The transfer ability of rate or low-temperature lithium ion can all have a great influence.
85 DEG C/4h of high-temperature storage performance is required in conventional high voltage lithium ion battery at present, while meets that general low temperature is put
Electricity and normal temperature circulation.But as demanding terminal is constantly strict, it is necessary to which the 85 DEG C/18h of storage that reaches a high temperature, 0 DEG C of low temperature are not analysed
Lithium, -20 DEG C of discharge performances reach more than the 85% of 25 DEG C；High rate performance (circulation >=90% in 500 weeks) is needed to have simultaneously.This is just
It is that needs are a to reach wide temperature range, high-tension rate electrolyte and using the battery of this electrolyte meet.
The content of the invention
For insufficient present in background above technology, it is an object of the invention to provide a kind of high temperature performance of taking into account
High voltage multiplying power electrolyte and the lithium ion battery using the electrolyte.
" the high voltage multiplying power electrolyte for taking into account high temperature performance " of the present invention refers to：Using battery made of the electrolyte
With good cycle life, cryogenic discharging characteristic and high-temperature storage performance.4.35V normal temperature 3C circulates 500 weeks capability retentions
More than 90.1%；- 20 DEG C in the ratio between 0.2C low temperature discharge capacities and initial capacity more than 89.5%；High temperature storage 18h@85
DEG C hot expansion rate below 7.8%, capacity surplus ratio is more than 85.1%.
In the present invention, " initial capacity " method of testing when testing cryogenic property referring to embodiment 1 test department point 4).Survey
Try 85 DEG C of high temperature storage 18h hot expansion rate and the method for capacity surplus ratio referring to the test department point of embodiment 1 2).
For the above-mentioned purpose, the present invention uses following technical scheme：
In a first aspect, the present invention provides a kind of electrolyte, especially a kind of high voltage multiplying power electricity for taking into account high temperature performance
Liquid is solved, the electrolyte includes non-aqueous organic solvent, is dissolved in the lithium salts of the non-aqueous organic solvent, and additive；
Wherein, the non-aqueous organic solvent contains propene carbonate (PC) and carboxylate, and the additive includes citraconic acid
Acid anhydride, difluorophosphate LiPO2F2, fluorinated ethylene carbonate, sulfuric acid vinyl ester DTD and 1,2- bis- (2- cyanoethoxyls) ethane DENE.
The electrolyte of the present invention is a kind of non-aqueous electrolytic solution.By preferably being formed with regulation electrolyte solvent, make bag
Non-aqueous organic solvent system containing PC and carboxylate interacts with the additive containing above-mentioned predetermined substance, produces cooperative effect,
For lithium ion battery, battery can be made still to keep excellent cycle life, cryogenic discharging characteristic and high temperature under high voltage multiplying power
Storage characteristics.
Electrolyte system containing propene carbonate and carboxylate mixed dissolution in the non-aqueous organic solvent of the present invention, liquid journey
Width, high temperature performance can be taken into account simultaneously, wherein carboxylate (especially wire carboxylate) can improve electrode/electrolyte interface,
The decomposition of electrolyte is inhibited, reduces the gas production of battery, so as to further improve the high-temperature storage performance of lithium ion battery.
The present invention electrolyte in, citraconic anhydride and difluorophosphate compound action in additive can reach take into account it is excellent
The effect of good high-temperature behavior and enhancing circulation performance, above two material (citraconic anhydride and difluorophosphate) play core
The heart acts on, in order to realize that the present invention takes into account the high voltage multiplying power electrolyte of high temperature performance, remaining fluorinated ethylene carbonate, sulphur
Vinyl acetate and 1,2- bis- (2- cyanoethoxyls) ethane are also all essential components.
Open " the containing " being related in the present invention and " comprising " can be replaced it is enclosed " by ... form ".
As the optimal technical scheme of electrolyte of the present invention, also contain ethylene carbonate in the non-aqueous organic solvent
(EC), appointing in butylene, dimethyl carbonate, diethyl carbonate (DEC), methyl ethyl carbonate (EMC) or methyl propyl carbonate
Anticipate a kind of or at least two combinations.The combination is typical but non-limiting examples have：Ethylene carbonate and butylene
Combination, the combination of ethylene carbonate and diethyl carbonate, the combination of butylene and methyl ethyl carbonate, dimethyl carbonate and carbon
The combination of diethyl phthalate, the combination of diethyl carbonate sum, ethylene carbonate (EC), butylene, diethyl carbonate and carbonic acid
Combination of methyl ethyl ester etc..
Preferably, the carboxylate is wire carboxylate, preferably methyl acetate, ethyl acetate, propyl acetate (PA), third
In sour methyl esters, ethyl propionate (EP), propyl propionate (PP), methyl butyrate or ethyl butyrate any one or at least two group
Close.The combination is typical but non-limiting examples have：The combination of methyl acetate and ethyl acetate, methyl acetate and propyl acetate
The group of combination, the combination of methyl acetate and methyl propionate, the combination of ethyl propionate and propyl propionate, methyl propionate and methyl butyrate
Close, combination that ethyl acetate, propyl acetate and butyric acid suppress etc..
Preferably, the lithium salts is except containing the difluorophosphate used as additive, in addition to lithium hexafluoro phosphate, height
Lithium chlorate, LiBF4, di-oxalate lithium borate, double fluorine Lithium bis (oxalate) borates, two (trimethyl fluoride sulfonyl) imine lithiums, double fluorine sulphonyl
In imines lithium salts LIFSI or double trifluoromethanesulfonimide lithiums LITFSI any one or at least two combination.The lithium
Salt is for example：The combination of the combination of difluorophosphate and lithium hexafluoro phosphate, difluorophosphate and lithium perchlorate, difluorophosphate and four
The combination of lithium fluoroborate, the combination of difluorophosphate and double fluorine Lithium bis (oxalate) borates, difluorophosphate and imidodisulfuryl fluoride lithium salt
Combination, the combination of difluorophosphate, imidodisulfuryl fluoride lithium salt, lithium perchlorate and LiBF4, difluorophosphate, hexafluoro
The combination etc. of lithium phosphate, LiBF4, two (trimethyl fluoride sulfonyl) imine lithiums and imidodisulfuryl fluoride lithium salt.
It is highly preferred that the lithium salts is except containing the difluorophosphate used as additive, in addition to lithium hexafluoro phosphate.
Preferably, in the electrolyte, the concentration of lithium hexafluoro phosphate is 1.2mol/L~1.3mol/L, such as 1.2mol/
L, 1.22mol/L, 1.24mol/L, 1.25mol/L, 1.27mol/L, 1.28mol/L or 1.3mol/L etc..
Preferably, for the lithium salts in the electrolyte except the difluorophosphate used as additive, remaining lithium salts is six
Lithium fluophosphate, and the concentration of lithium hexafluoro phosphate is 1.2mol/L~1.3mol/L in electrolyte.This material coordinates and concentration bar
Under part, 2C~5C high rate capabilities of difluorophosphate and lithium hexafluoro phosphate collaboration improvement battery, cycle performance is lifted higher
It is horizontal.
As the optimal technical scheme of electrolyte of the present invention, counted using the gross mass of electrolyte as 100%, the lemon health
The mass percent of acid anhydrides is 0.1%~1%, such as 0.1%, 0.3%, 0.5%, 0.6%, 0.8% or 1% etc..It is excellent herein
In the range of choosing, the electrolyte is applied and can reach both positive and negative polarity film forming in battery, suppresses high temperature inflatable, improves high temperature storage,
Ensure that battery has excellent high-temperature behavior.Coordinate 0.1%~3% 1,2- bis- (2- cyanoethoxyls) ethane again, gold can be made
Belong to ion and complexing occurs, reduce electrolyte decomposition, suppress digestion of metallic ion, protect positive pole, improve battery high-temperature behavior.
Moreover, while stating excellent properties and good electrolyte high-temperature behavior in realization, other performances are not interfered with.
Preferably, counted using the gross mass of electrolyte as 100%, the mass percent of the fluorinated ethylene carbonate is 2%
~7%, such as 2%, 3%, 4%, 4.5%, 5%, 5.5%, 6% or 7% etc..
Preferably, counted using the gross mass of electrolyte as 100%, the mass percent of the sulfuric acid vinyl ester for 0.1%~
5%, for example, 0.1%, 0.2%, 0.5%, 0.8%, 1%, 1.2%, 1.5%, 2%, 2.5%, 2.8%, 3%, 3.5%,
4%th, 4.5% or 5% etc., in this preferred scope 0.1%~5%, sulfuric acid vinyl ester can be in the preferential carbon in graphite cathode surface
Vinyl acetate EC is decomposed, and the good organic sulfonate of generation ionic conductivity, so as to reduce interface impedance, improves low temperature discharge
Performance.
It is highly preferred that being counted using the gross mass of electrolyte as 100%, the mass percent of the sulfuric acid vinyl ester is 0.1%
~3%.In this preferred scope 0.1%~3%, not only with foregoing beneficial effect, moreover, its relatively low reduction potential,
Can be preferably in negative terminal surface film forming, so as to improve the proportion of composing of SEI films.It, which is added, is advantageous to improve electrode/electrolyte circle
The kinetic property of face reaction, now the impedance of battery is relatively low, is advantageous to improve the reversible capacity of battery, improves low temperature discharge
Performance and high-temperature storage performance.
Preferably, counted using the gross mass of electrolyte as 100%, the quality percentage of 1,2- bis- (2- cyanoethoxyls) ethane
Than for 0.1%~10%, such as 0.1%, 0.5%, 1%, 2%, 2.5%, 3%, 4%, 5%, 5.5%, 6%, 7%, 8%,
9% or 10% etc., preferably 0.1%~3%.In this preferred scope 0.1%~3%, complexing occurs for metal ion, reduces
Electrolyte decomposition, suppress digestion of metallic ion, protect positive pole, improve battery high-temperature behavior.
As the optimal technical scheme of electrolyte of the present invention, also containing vinylene carbonate, carbon in the electrolyte
In sour vinylethylene, adiponitrile, maleic anhydride, 1,3- propane sultones, 1,4- butane sultones or 1,3- propene sultones
Any one or at least two combination as addO-on therapy, and above-mentioned addO-on therapy accounts for the quality percentage of electrolyte gross mass
Than being each independently 0.1%~10%, such as 0.1%, 0.5%, 1%, 2%, 3%, 4%, 5%, 5.5%, 6%, 7%,
8%th, 9% or 10% etc..
As the further preferred technical scheme of electrolyte of the present invention, the electrolyte includes non-aqueous organic solvent,
It is dissolved in the lithium salts of the non-aqueous organic solvent, and additive；
Wherein, the non-aqueous organic solvent contains ethylene carbonate EC, propene carbonate PC and carboxylate, the additive
Including citraconic anhydride and difluorophosphate, fluorinated ethylene carbonate, sulfuric acid vinyl ester and 1,2- bis- (2- cyanoethoxyls) ethane, and
Counted using the gross mass of the electrolyte as 100%, the mass percent of the fluorinated ethylene carbonate is 2%~7%, the sulphur
The mass percent 0.1%~5% of vinyl acetate, the mass percent of 1,2- bis- (2- cyanoethoxyls) ethane is 0.1%
~3%；
Preferably, the lithium salts is except containing the difluorophosphate used as additive, remaining lithium salts is hexafluorophosphoric acid
Lithium, and the concentration of lithium hexafluoro phosphate is 1.2mol/L~1.3mol/L in the electrolyte.
Second aspect, the present invention provide a kind of lithium ion battery, and the charge cutoff voltage of the lithium ion battery is big
In being not higher than 4.5V equal to 4.2V, including positive pole, negative pole, the barrier film being placed between positive pole and negative pole, and first aspect institute
The electrolyte stated.
Compared with the prior art, the present invention has the advantages that：
1) in electrolyte of the invention, used including citraconic anhydride, difluorophosphate (LiPO2F2), fluoro ethylene carbonate
The additive combination of ester, sulfuric acid vinyl ester and (2- cyanoethoxyls) ethane of 1,2- bis- this type, these additives synergy can
So that electrolyte takes into account excellent high-temperature behavior and strengthens high rate performance.
2) in electrolyte of the invention, solvent PC has been used, has had fusing point low, boiling point is high, and dielectric constant is high, electrolyte
It is that liquid journey is wide, with the use of carboxylic acid esters solvent, can not only improves lithium ion battery cryogenic discharging characteristic, while take into account high temperature
Storage performance, the carboxylic acid esters solvent at electrode/electrolyte interface can also be improved, it is suppressed that the decomposition of electrolyte, reduce electricity
The gas production in pond, so as to improve the high-temperature storage performance of lithium ion battery.It can reach height using the type solvent so as to reach
The purpose for the wide temperature range that temperature is satisfied by.
3) lithium ion battery of the invention has used the electrolyte of the present invention, and the lithium ion battery is under rate high voltage
Still keep good circulation life-span, cryogenic discharging characteristic and high-temperature storage characteristics, the full electric state storage of 85 DEG C of high-voltage battery
18h, 0 DEG C completely fill and do not analyse lithium, -20 DEG C of discharge performances are good, low temperature excellent properties.
Brief description of the drawings
Fig. 1 a- Fig. 1 c respectively are using battery made of the electrolyte of embodiment 1 at 25 DEG C, -10 DEG C and -20 DEG C
Discharge platform curve, wherein, 1 and 2 in each figure represent the sample for two batches being prepared according to the condition of embodiment 1
The result tested respectively；
Fig. 2 is the fast charge cyclic curve in normal temperature 3C using battery made of the electrolyte of embodiment 1, wherein, wherein, 3C
Fast charge 1# and 3C fast charge -2# represents the result that the sample for two batches being prepared according to the condition of embodiment 1 is tested respectively.
Embodiment
Further illustrate technical scheme below in conjunction with the accompanying drawings and by embodiment.
Embodiment 1
Electrolyte quota step：In the glove box full of argon gas, by ethylene carbonate, propene carbonate, carbonic acid diethyl
Ester, n propyl propionate (being propyl propionate) are EC in mass ratio:PC:DEC:PP=20:20:45:15 are mixed, Ran Houxiang
Mixed solution, which is slowly added to lithium hexafluoro phosphate, makes the concentration of lithium hexafluoro phosphate in electrolyte be 1.25mol/L, is eventually adding and is based on
Electrolyte gross weight 0.5wt% 1,2- bis- (2- cyanoethoxyls) ethane (DENE), 0.5wt% sulfuric acid vinyl esters (DTD),
0.3wt% vinylene carbonates (VC), 4wt% fluorinated ethylene carbonates (FEC), 3wt% propane sultones (PS),
0.5wt% double fluorine sulfimide lithium (LIFSI), 0.3wt% difluorophosphates (LIPO2F2), the stirring of 0.2wt% citraconic anhydrides it is equal
After even, the lithium-ion battery electrolytes of embodiment 1 are obtained.
The lithium-ion battery electrolytes injection that above-mentioned steps are prepared is by fully dry 4.35V graphite/LiCoO2It is poly-
Compound battery (volume energy density 600Wh/L), battery are shelved by 45 DEG C, are melted into, after fixture high-temperature baking and secondary sealing,
Carry out conventional partial volume.
Test：
1) normal-temperature circulating performance is tested：At 25 DEG C, the battery after chemical conversion is charged to 4.35V by 3C constant current constant voltages, ended
Electric current 0.02C, then by 1C constant-current discharges to 3.0V.The 500th cycle circulation volume is calculated after 500 circulations of charge/discharge to keep
Rate.Calculation formula is as follows：
500th circulation volume conservation rate (%)=(the 500th cyclic discharge capacity/first cyclic discharge capacity) ×
100%；
2) 85 DEG C of high-temperature storage performances：Battery is pressed into 0.5C discharge and recharges once at room temperature, cut-off current 0.02C, record is just
Beginning capacity.It is full of again by 0.5C constant current constant voltages, tests initial battery thickness；The constant temperature that full battery is placed in 85 DEG C of 85% humidity is permanent
Stored 18 hours in wet tank, test the hot thickness of battery, calculate hot expansion；Battery normal temperature shelf tests cold thickness, electricity after 6 hours
Pressure, internal resistance, 3.0V is discharged to by 0.5C, records residual capacity；0.5C charge and discharge cycles are pressed again 3 times, record in 3 circulations most
Large Copacity, i.e. battery recovery capacity, calculate battery capacity surplus ratio and capacity resuming rate.Calculation formula is as follows：
The hot expansion rate of battery (%)=(hot thickness-original depth)/original depth × 100%；
Battery capacity surplus ratio (%)=holding capacity/initial capacity × 100%；
Capacity resuming rate (%)=recovery capacity/initial capacity × 100%.
3) 0 DEG C of battery, which completely fills, disassembles：After battery is shelved into 16 hours in 0 DEG C of insulating box, by 0.5C electric current constant current constant voltages
4.35V, cut-off current 0.02C are charged to, by battery transfer into the glove box full of argon gas, full electric state disassembles battery, observation electricity
Pond negative terminal surface color, analysis lithium situation.
4) low temperature discharge：Using 1C constant-current constant-voltage chargings to 4.35V (cut-off current is 0.02C) under 25 DEG C of environment, shelve
5min, 0.2C are discharged to 3.0V, detect battery initial capacity.5min is shelved, 4.35V is charged to 0.2C.Battery is put into -20 DEG C
High-low temperature chamber in shelve 4h, and 3.0V is discharged to 0.2C on this condition, detects the discharge capacity under low temperature.
Low temperature discharge conservation rate (%)=low temperature discharge capacity/initial capacity × 100%.
Fig. 1 a- Fig. 1 c respectively are using battery made of the electrolyte of embodiment 1 at 25 DEG C, -10 DEG C and -20 DEG C
Discharge platform curve, wherein 1 and 2 in each figure represent the sample for two batches being prepared according to the condition of embodiment 1
The result tested respectively.
Fig. 2 is the fast charge cyclic curve in 3C using battery made of the electrolyte of embodiment 1, wherein, wherein, in Fig. 2
3C fast charge 1# and 3C fast charges -2# represent what the sample of two batches being prepared according to the condition of embodiment 1 was tested respectively
As a result.
Embodiment 2~12 and comparative example 1~6
Embodiment 2~12 and comparative example 1~6, except solvent Bi Li ﹑ additives composition and content (are based on electrolyte gross weight
Amount) it is outer by addition shown in table 1, other same as Example 1, the formula composition of each embodiment is shown in Table 1, and physical data is shown in Table 2.
Note：Lithium source in embodiment 1 has two parts, and a part is lithium hexafluoro phosphate, and another part is as additive
Difluorophosphate.The amount of lithium hexafluoro phosphate and concentration are same as Example 1 in embodiment 2~12 and comparative example 1~6, and difluoro
The content of lithium phosphate changes according to table 1.
The formula composition of 1 each embodiment of table
In above-mentioned table, it is as follows that each chemical substance letter writes a Chinese character in simplified form corresponding title：
EC (ethylene carbonate), PC (propene carbonate), DEC (diethyl carbonate), EMC (methyl ethyl carbonate), PP (propionic acid
N-propyl), PA (propyl acetate), EP (ethyl propionate), LIFSI (double fluorine sulfimide lithiums), LITFSI (double fluoroform sulphonyl
Imine lithium), LIPO2F2(difluorophosphate), FEC (fluorinated ethylene carbonate), DENE (1,2- bis- (2- cyanoethoxyls) ethane),
DTD (sulfuric acid vinyl ester).
The physical data of 2 each embodiment of table
Note：The method of testing that 85 DEG C of high-temperature storage 18h referring to embodiment 1 test department point 2).
There is more preferable normal-temperature circulating performance, high-temperature storage using 1~embodiment of embodiment 12 of technical scheme
And low temperature performance.High/low temperature and cycle performance can not be taken into account simultaneously using the battery of the electrolyte of 1~comparative example of comparative example 6,
Combination property is relatively poor.
Embodiment 1~12 is understood compared with comparative example 1~2, wire carboxylate is not added with comparative example, without PC batteries 0
DEG C completely fill negative pole easily to occur to analyse lithium, cycle performance of battery and 85 DEG C of high-temperature storage performances are also relatively poor.Corresponding high temperature storage
The capability retention deposited is low, and battery inflatable is serious.
Comparative example 3, comparative example 5, comparative example 6 are knowable to compared with embodiment 1~12, sulfuric acid vinyl ester, citraconic anhydride, DENE
(1,2- bis- (2- cyanoethoxyls) ethane) maintains for high-temperature storage and energy obviously to be acted on, particularly one piece use
Positive effect can be performed to.
Find to lack the reduction of sulfuric acid vinyl ester normal-temperature circulating performance by comparative example 5 simultaneously, high-temperature behavior is also bad, low temperature
Discharging efficiency is 79.6%, less than embodiment 1 (93.8%).Illustrate that sulfuric acid vinyl ester can significantly improve low temperature discharge property
Can, while high-temperature storage to battery and normal-temperature circulating performance also have a certain upgrade.
Found by comparative example 3, comparative example 4 and embodiment 1, increase citraconic anhydride effectively strengthen high-temperature storage performance and
Energy holding capacity.Increase difluorophosphate for the effect of getting a promotion of multiplying power long circulating.
To sum up：The present invention is formed with containing propene carbonate (PC) and line by preferably being formed with regulation electrolyte solvent
The electrolyte system of shape carboxylate mixed solvent, its liquid journey is wide, can take into account high temperature performance simultaneously, wherein wire carboxylate can
Improve electrode/electrolyte interface, it is suppressed that the decomposition of electrolyte, reduce the gas production of battery, improve the height of lithium ion battery
Warm storage performance.This dicyandiamide solution is the same as additive sulfur vinyl acetate, DENE (1,2- bis- (2- cyanoethoxyls) ethane) and citraconic acid
Acid anhydride optimum organization, ensure that battery still keeps good cycle life, cryogenic discharging characteristic and high-temperature storage characteristics under high voltages.
Addition difluorophosphate and double fluorine sulfimide lithiums ensure there is outstanding circulation ability and multiplying power energy under high/low temperature and normal temperature
Power.In the electrolyte of the present invention, multiple additives collective effect, it can be ensured that high-voltage battery obtains excellent circulation
Can, at the same take into account the full electric state storage 18h of 85 DEG C of high-voltage battery, 0 DEG C completely fill and do not analyse lithium and -20 DEG C of outstanding high and low temperatures of electric discharge are excellent
Different in nature energy, forms a kind of a high voltage multiplying power electrolyte for taking into account high temperature performance.
Applicant states that the present invention illustrates the method detailed of the present invention, but not office of the invention by above-described embodiment
It is limited to above-mentioned method detailed, that is, does not mean that the present invention has to rely on above-mentioned method detailed and could implemented.Art
Technical staff it will be clearly understood that any improvement in the present invention, equivalence replacement and auxiliary element to each raw material of product of the present invention
Addition, selection of concrete mode etc., within the scope of all falling within protection scope of the present invention and disclosing.
Claims (10)
1. a kind of electrolyte, it is characterised in that the electrolyte includes non-aqueous organic solvent, is dissolved in the non-aqueous organic solvent
Lithium salts, and additive；
Wherein, the non-aqueous organic solvent contains propene carbonate PC and carboxylate, and the additive includes citraconic anhydride, difluoro
Lithium phosphate LiPO2F2, fluorinated ethylene carbonate FEC, sulfuric acid vinyl ester DTD and 1,2- bis- (2- cyanoethoxyls) ethane DENE.
2. electrolyte according to claim 1, it is characterised in that also contain ethylene carbonate in the non-aqueous organic solvent
Any one in EC, butylene, dimethyl carbonate, diethyl carbonate DEC, methyl ethyl carbonate EMC or methyl propyl carbonate
Or at least two combination.
3. electrolyte according to claim 1 or 2, it is characterised in that the carboxylate is wire carboxylate, preferably second
Sour methyl esters, ethyl acetate, propyl acetate PA, methyl propionate, ethyl propionate EP, propyl propionate PP, methyl butyrate or ethyl butyrate
In any one or at least two combination.
4. according to the electrolyte described in claim any one of 1-3, it is characterised in that the lithium salts is except containing as additive
The difluorophosphate used, in addition to lithium hexafluoro phosphate, lithium perchlorate, LiBF4, di-oxalate lithium borate, double fluorine oxalic acid boron
Sour lithium, two (trimethyl fluoride sulfonyl) imine lithiums, imidodisulfuryl fluoride lithium salt LIFSI or double trifluoromethanesulfonimide lithiums LITFSI
In any one or at least two combination.
5. electrolyte according to claim 4, it is characterised in that the lithium salts is except containing two used as additive
Lithium fluophosphate, in addition to lithium hexafluoro phosphate.
6. according to the electrolyte described in claim any one of 1-5, it is characterised in that in the electrolyte, lithium hexafluoro phosphate
Concentration is 1.2mol/L~1.3mol/L；
Preferably, for the lithium salts in the electrolyte except the difluorophosphate used as additive, remaining lithium salts is hexafluoro phosphorus
Sour lithium, and the concentration of lithium hexafluoro phosphate is 1.2mol/L~1.3mol/L in electrolyte.
7. electrolyte according to claim 6, it is characterised in that counted using the gross mass of electrolyte as 100%, with electrolyte
Gross mass be 100% meter, the mass percent of the citraconic anhydride is 0.1%~1%；
Preferably, the mass percent of the fluorinated ethylene carbonate is 2%~7%；
Preferably, to be counted using the gross mass of electrolyte as 100%, the mass percent of the sulfuric acid vinyl ester is 0.1%~5%,
Further preferred 0.1%~3%；
Preferably, counted using the gross mass of electrolyte as 100%, the mass percent of 1,2- bis- (2- cyanoethoxyls) ethane is
0.1%~10%, preferably 0.1%~3%.
8. according to the electrolyte described in claim any one of 1-7, it is characterised in that also contain carbonic acid Asia second in the electrolyte
Alkene ester, vinylethylene carbonate, adiponitrile, maleic anhydride, 1,3- propane sultones, 1,4- butane sultones or 1,3- propylene sulphurs
In lactone any one or at least two combination as addO-on therapy, and above-mentioned addO-on therapy accounts for the matter of electrolyte gross mass
Amount percentage is each independently 0.1~10%.
9. according to the electrolyte described in claim any one of 1-8, it is characterised in that the electrolyte includes non-aqueous organic molten
Agent, it is dissolved in the lithium salts of the non-aqueous organic solvent, and additive；
Wherein, the non-aqueous organic solvent contains ethylene carbonate EC, propene carbonate PC and carboxylate, and the additive includes
Citraconic anhydride and difluorophosphate, fluorinated ethylene carbonate, sulfuric acid vinyl ester and 1,2- bis- (2- cyanoethoxyls) ethane, and with institute
The gross mass for stating electrolyte is 100% meter, and the mass percent of the fluorinated ethylene carbonate is 2%~7%, the sulfuric acid second
The mass percent 0.1%~5% of alkene ester, the mass percent of 1,2- bis- (2- cyanoethoxyls) ethane for 0.1%~
3%；
The lithium salts is except containing the difluorophosphate used as additive, and remaining lithium salts is lithium hexafluoro phosphate, and the electricity
The concentration for solving lithium hexafluoro phosphate in liquid is 1.2mol/L~1.3mol/L.
10. a kind of lithium ion battery, the charge cutoff voltage of the lithium ion battery is more than or equal to 4.2V and is not higher than 4.5V, wraps
Include positive pole, negative pole and the barrier film being placed between positive pole and negative pole, it is characterised in that will also including right in the lithium ion battery
Seek the electrolyte described in any one of 1-9.
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