CN106602140B - A kind of electrolyte improving polymer lithium ion secondary battery high-temperature behavior - Google Patents
A kind of electrolyte improving polymer lithium ion secondary battery high-temperature behavior Download PDFInfo
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- CN106602140B CN106602140B CN201610555000.7A CN201610555000A CN106602140B CN 106602140 B CN106602140 B CN 106602140B CN 201610555000 A CN201610555000 A CN 201610555000A CN 106602140 B CN106602140 B CN 106602140B
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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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- 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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Abstract
The present invention provides a kind of electrolyte for improving polymer lithium ion secondary battery high-temperature behavior, containing non-aqueous organic solvent, cathode film formation additive, lithium salts electrolyte, the electrolyte also contains the functional form additive of 0.5%-10% for accounting for the electrolyte gross mass indicated selected from structural formula I a kind of；Wherein R1 indicates the halogenated alkyl of optional carbon atom number 1-10；R2 and R3 be halogen atom ,-H ,-CN or be carbon atom number 1-10 alkyl (R1 and R2 may identical may also be different).The functional form additive can form stable Low ESR dielectric film in anode, the reactivity of anode be effectively reduced, to further suppress the decomposition of electrolyte.Electrolyte of the invention overcomes the shortcomings that serious polymer lithium ion secondary battery inflatable in high temperature storage and capacitance loss, the electrolyte system and lithium ion secondary battery positive and negative anodes have preferably compatibility, better high-temperature electrochemistry characteristic, high-temperature storage and multiplying power discharging property simultaneously.
Description
Technical field
The present invention relates to high-energy battery technical fields, more particularly to a kind of improvement polymer lithium ion secondary battery high temperature
The electrolyte of performance.
Background technique
Lithium ion polymer battery is state-of-the-art secondary cell in the world now, has gradually replaced ni-Cd, plumbic acid electricity
Pond is applied in the digital products such as mobile phone, laptop, MP3, PDA, DV, and being increasingly becoming can not in people's Working Life
Or scarce essential product.The safety of battery is to influence the main factor of battery applications, and the ballooning of lithium battery is to influence
The principal element of battery security causes the performance of battery to decline.Lithium ion polymer battery using clad aluminum plastic film due to being made
For housing material, biggish internal gas pressure cannot be born, therefore ballooning has increasingly constituted necessary solution factor.
With the extension in lithium ion battery applications field, to chemical property after the high-temperature storage and storage of polymer Li-ion battery
More stringent requirements are proposed.
Chinese patent 201110055393.2 proposes a kind of lithium ion polymer electrolyte comprising lithium salts, nonaqueous solvents
And the polymer of dispersion.The program can reduce the thickness swelling of battery under the high temperature conditions by adding polymer, significantly change
The high-temperature storage performance of kind battery.But the program improves the viscosity of electrolyte, electrolyte conductance using the copolymer of polymer
Rate decline is more, and high rate performance is deteriorated.
Summary of the invention
The object of the present invention is to provide a kind of electrolyte, are effectively improved polymer lithium ion secondary battery high-temperature behavior,
And the multiplying power discharging property of battery is not influenced, the present invention provides a kind of improvement polymer lithium ion secondary battery high-temperature behaviors
Electrolyte improves the electrolyte of polymer lithium ion secondary battery high-temperature behavior, adds containing non-aqueous organic solvent, cathode film formation
Agent, lithium salts electrolyte, the electrolyte also contain a kind of 0.5%- for accounting for the electrolyte gross mass indicated selected from structural formula I
10% functional form additive；
Its structural formula I is
Wherein R1 indicates the halogenated alkyl of optional carbon atom number 1-10；R2 and R3 is halogen atom ,-H ,-CN or is carbon original
The alkyl of subnumber 1-10.
The non-aqueous organic solvent includes carbonate solvent, and the carbonate solvent is ethylene carbonate (EC), carbonic acid
Acrylic ester (PC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC), diethyl carbonate (DEC), in methyl propyl carbonate (MPC)
At least one；Further include non-carbonate solvent, the non-carbonate solvent be gamma-butyrolacton (GBL), methyl acetate (MA),
Ethyl acetate (EA), propyl acetate (PA), methyl propionate (MP), ethyl propionate (EP), methyl butyrate (MB), ethyl butyrate (EB)
At least one of.
Carbonate solvent in the non-aqueous organic solvent accounts for the 10%~50% of electrolyte gross mass, and non-carbonic ester is molten
Agent accounts for the 10%~50% of electrolyte gross mass.
The cathode film formation additive includes fluorinated ethylene carbonate (FEC), propane sultone (PS), vinylene carbonate
(VC), trifluoromethyl ethylene carbonate (TFPC), sulfuric acid vinyl ester (DTD), ethylene sulfite (ES), vinyl ethylene carbonate
At least one of ester (VEC), propene sultone (RPS).
The 0.5%~30% of the total electrolyte gross mass of cathode film formation additive Zhan.
The lithium salts electrolyte includes lithium hexafluoro phosphate (LiPF6), bis- (fluorine sulphonyl) imine lithium LiFSI, bis- (fluoroforms
Base sulphonyl) imine lithium (LiTFSI), di-oxalate lithium borate (LiBOB), difluorine oxalic acid boracic acid lithium (LiODFB), LiBF4
(LiBF4), one of lithium carbonate Li2CO3, lithium perchlorate LiClO4 or several.
The percentage that the lithium salts electrolyte accounts for the total weight of electrolyte is 5%~30%.
The invention has the benefit that electrolyte of the invention overcomes polymer lithium ion secondary battery in high temperature storage
When the shortcomings that inflatable is serious and capacitance loss, while the electrolyte system and lithium ion secondary battery positive and negative anodes have it is better simultaneous
Capacitive, better high-temperature electrochemistry characteristic, high-temperature storage and multiplying power discharging property.The present invention by being added in the electrolytic solution
The functional form additive in structural formula I is stated, which can form stable Low ESR dielectric film in anode, effectively
Reduce anode reactivity, to further suppress the decomposition of electrolyte, and the additive does not influence the multiplying power of battery
Discharge performance.Because the electrolyte of the invention overcomes, polymer lithium ion secondary battery inflatable in high temperature storage is serious and capacity
The shortcomings that loss, while the electrolyte system and lithium ion secondary battery positive and negative anodes have preferably compatibility, better high temperature
Electrochemical properties.
The present invention solves polymer lithium ion secondary battery, and full 85 DEG C of electricity state store 48 hours, integral battery thickness swelling
Less than 5%, battery remaining power restores capacity greater than 98%, 10C multiplying power discharging capacity and is greater than 95% 95% or more, high temperature
45 DEG C of circulations, 800 weeks capacity are greater than 80%.
Specific embodiment
Below with reference to embodiment, comparative example, the present invention is described in detail.The present invention is not limited to implementation forms.
The present invention provides a kind of electrolyte for improving polymer lithium ion secondary battery high-temperature behavior to improve polymer lithium
The electrolyte of ion secondary battery high-temperature behavior, it is described containing non-aqueous organic solvent, cathode film formation additive, lithium salts electrolyte
Electrolyte also contains the functional form addition of 0.5%-10% for accounting for the electrolyte gross mass indicated selected from structural formula I a kind of
Agent；
Structural formula I
Wherein R1 indicates the halogenated alkyl of optional carbon atom number 1-10；R2 and R3 is halogen atom ,-H ,-CN or is carbon original
The alkyl of subnumber 1-10.
Functional form additive chooses typical structure formula (1)~(3) (as shown below), and naming structural formula (1) respectively is to add
Add agent A, structural formula (2) is additive B, and structural formula (3) is addition of C.
Non-aqueous organic solvent is uniformly mixed by required quality proportioning, it is molten to mixing after -20 DEG C of low temperature freezings after 1 hour
Electrolyte lithium salt is added in agent, is slowly added to for average mark 3 times, sufficiently shakes after addition to being completely dissolved, then adds cathode
Film for additive shakes up, and is eventually adding functional form additive and is uniformly mixed.Entire process for preparation is in glove box or dry ring
Border carries out under (dew-point temperature is lower than -60 DEG C, 20 DEG C of temperature or so), and electrolyte moisture controls within 5ppm, and electrolyte is infused
Enter and is tested for the property into polymer battery.
Comparative example 1:EC/DMC=1/1 (mass ratio) LiPF6 mass fraction 10%, cathode film formation additive VC, additive amount
0.5%.
Comparative example 2:EC/EMC=1/2 (mass ratio) LiPF6 mass fraction is 10%, and cathode film formation additive VC, FEC add
Dosage is respectively 0.5% and 1%.
Comparative example 3:EC/EMC/DEC=1/1/1 (mass ratio) LiPF6 mass fraction is 12%, cathode film formation additive
PS, FEC additive amount are respectively 1% and 2%.
Comparative example 4:EC/EMC/DEC=1/1/1 (mass ratio) LiFSi mass fraction is 12%, cathode film formation additive
PS, FEC additive amount are respectively 1% and 2%.
Comparative example 5:EC/MPC=1/2 (mass ratio) LiPF6 mass fraction is the addition of 10%, LiBOB, 2% cathode film formation
Agent DTD additive amount is 1%.
Comparative example 6:EC/PC/EMC=1/1/3 (mass ratio) LiPF6 mass fraction be 10%, LiODFB5%, cathode at
Film additive DTD additive amount is 1%.
Comparative example 7:EC/GBL/EP=1/1/8 (mass ratio) LiPF6 mass fraction is 10%, Li2CO30.5%, cathode
Film for additive RPS additive amount is respectively 2%.
Comparative example 8:EC/DMC/DEC=2/1/7 (mass ratio) LiPF6 mass fraction is 15%, cathode film formation additive
VEC and FEC additive amount is respectively 1% and 5%.
Comparative example 9:EC/EA/PC=1/2/7 (mass ratio) LiPF6 mass fraction is 12%, LiTFSi mass fraction 2%,
Cathode film formation additive VC, PS, FEC additive amount is 1%, 2% and 5%.
Embodiment 1
The functional form additive A for accounting for electrolyte total mass ratio 0.5% is added on the basis of comparative example 1, is modulated into electrolysis
Liquid.
Embodiment 2
The functional form additive A for accounting for electrolyte total mass ratio 1.0% is added on the basis of comparative example 2, is modulated into electrolysis
Liquid.
Embodiment 3
The functional form additive B for accounting for electrolyte total mass ratio 0.5% is added on the basis of comparative example 3, is modulated into electrolysis
Liquid.
Embodiment 4
The function of the functional form additive B and 3% that account for electrolyte total mass ratio 2.0% is added on the basis of comparative example 4
Type addition of C, is modulated into electrolyte.
Embodiment 5
The functional form addition of C for accounting for electrolyte total mass ratio 5.0% is added on the basis of comparative example 5, is modulated into electrolysis
Liquid.
Embodiment 6
The functional form addition of C for accounting for electrolyte total mass ratio 10.0% is added on the basis of comparative example 6, is modulated into electrolysis
Liquid.
Embodiment 7
It is added on the basis of comparative example 7 and accounts for the functional form additive A of electrolyte total mass ratio 2.0% and 3% function
Type additive B, is modulated into electrolyte.
Embodiment 8
It is added on the basis of comparative example 8 and accounts for the functional form additive A of electrolyte total mass ratio 1.0% and 3% function
Type addition of C, is modulated into electrolyte.
Embodiment 9
The function of the functional form additive B and 5% that account for electrolyte total mass ratio 0.5% is added on the basis of comparative example 9
Type addition of C, is modulated into electrolyte.
The performance test and explanation of comparative example and embodiment
Electrolyte is prepared using the method for above-mentioned comparative example and embodiment, and carries out electrolyte moisture, acidity, coloration, close
Electrolyte is injected into polymer Li-ion battery according to cell making process after detection is qualified, passes through by the basic tests such as degree
After aging, chemical conversion, partial volume, following project testing is carried out to battery:
The polymer Li-ion battery of experimental cell model 054595, battery core are a length of 95 millimeters, wide with a thickness of 5 millimeters
It is 45 millimeters；Integral battery nominal capacity 2.5Ah.
(1) high temperature storage is tested
It is placed in 85 degree of baking oven after will be filled with the polymer battery vernier caliper measurement thickness (being recorded as A) of electricity,
Thickness test was as a child quickly carried out by 48 and is made a record and (is recorded as B).
Expansion rate=(B-A)/A*100%
(2) high temperature volume test
Battery is placed in insulating box, after 85 DEG C save 48 hours, 0.2C multiplying power carries out being discharged to 2.75 volts, discharge capacity
The as residual capacity of battery；After 0.2C rate charge-discharge recycles 3 weeks, the discharge capacity of integral battery 0.2C multiplying power is to restore
Capacity.
(3) high rate performance is tested
After battery partial volume, battery is carried out to be discharged to 2.75V with 10C electric current, discharge capacity is multiplying power than partial volume capacity
Discharge performance.
Comparative example is in embodiment high-temperature behavior test result
Table 1 be comparative example 1-9 and embodiment 1-9 expansion rate, residual capacity, restore capacity, high rate performance, 45 DEG C 800 weeks
Cycle performance data significantly reduce battery after storage at high temperatures by adding functional form additive as can be seen from the table
Expansion rate, residual capacity, recovery capacity and 45 DEG C of cycle performances are also significantly increased, this shows that the functional additive obviously inhibits
Electrolyte is decomposed in high temperature storage, while also playing certain protective effect to cathode SEI.In addition, passing through addition function
Energy type additive polymer battery does not decline on high rate performance, is correspondingly improved instead, shows the additive in anode
It forms and compares Low ESR, the conductivity of electrolyte is not influenced significantly.
The above is only a preferred embodiment of the present invention, it is noted that for the common skill of the art
For art personnel, without departing from the principle of the present invention, several improvement can also be made, these improvement also should be regarded as this hair
Bright protection scope.
Claims (7)
1. a kind of electrolyte for improving polymer lithium ion secondary battery high-temperature behavior, including non-aqueous organic solvent, cathode film formation
Additive, lithium salts electrolyte further include a kind of 0.5%-10% for accounting for the electrolyte gross mass indicated selected from structural formula I
Functional form additive；
Its structural formula I is
The R1 indicates the halogenated alkyl of optional carbon atom number 1-10；R2 and R3 is halogen atom ,-H ,-CN or is carbon atom number
The alkyl of 1-10.
2. a kind of electrolyte for improving polymer lithium ion secondary battery high-temperature behavior described in accordance with the claim 1, feature
It is that the non-aqueous organic solvent includes carbonate solvent, the carbonate solvent is ethylene carbonate (EC), propylene carbonate
Ester (PC), dimethyl carbonate (DMC), methyl ethyl carbonate (EMC), diethyl carbonate (DEC), in methyl propyl carbonate (MPC) extremely
Few one kind；It further include non-carbonate solvent, the non-carbonate solvent is gamma-butyrolacton (GBL), methyl acetate (MA), acetic acid
Ethyl ester (EA), propyl acetate (PA), methyl propionate (MP), ethyl propionate (EP), methyl butyrate (MB), in ethyl butyrate (EB) extremely
Few one kind.
3. a kind of electrolyte for improving polymer lithium ion secondary battery high-temperature behavior according to claim 2, feature
It is, the carbonate solvent in the non-aqueous organic solvent accounts for the 10%~50% of electrolyte gross mass, non-carbonate solvent
Account for the 0%~50% of electrolyte gross mass.
4. a kind of electrolyte for improving polymer lithium ion secondary battery high-temperature behavior described in accordance with the claim 1, feature
It is, the cathode film formation additive includes fluorinated ethylene carbonate (FEC), propane sultone (PS), vinylene carbonate
(VC), trifluoromethyl ethylene carbonate (TFPC), sulfuric acid vinyl ester (DTD), ethylene sulfite (ES), vinyl ethylene carbonate
At least one of ester (VEC), propene sultone (RPS).
5. a kind of electrolyte for improving polymer lithium ion secondary battery high-temperature behavior according to claim 4, feature
It is the 0.5%~30% of the total electrolyte gross mass of cathode film formation additive Zhan.
6. a kind of electrolyte for improving polymer lithium ion secondary battery high-temperature behavior described in accordance with the claim 1, feature
It is, the lithium salts electrolyte includes lithium hexafluoro phosphate (LiPF6), bis- (fluorine sulphonyl) imine lithium LiFSI, bis- (trifluoromethyls
Sulphonyl) imine lithium (LiTFSI), di-oxalate lithium borate (LiBOB), difluorine oxalic acid boracic acid lithium (LiODFB), LiBF4
(LiBF4), one of lithium carbonate Li2CO3, lithium perchlorate LiClO4 or several.
7. a kind of electrolyte for improving polymer lithium ion secondary battery high-temperature behavior according to claim 6, feature
It is, the percentage that the lithium salts electrolyte accounts for the total weight of electrolyte is 5%~30%.
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| CN109286042B (en) * | 2017-07-21 | 2020-11-10 | 天津金牛电源材料有限责任公司 | Preparation method of electrolyte for lithium ion power battery |
| CN109980277A (en) * | 2017-12-27 | 2019-07-05 | 张家港市国泰华荣化工新材料有限公司 | A kind of nonaqueous electrolytic solution and secondary cell |
| CN108232300A (en) * | 2018-01-05 | 2018-06-29 | 宁德新能源科技有限公司 | A kind of lithium ion battery and its electrolyte |
| CN110148785A (en) * | 2019-05-29 | 2019-08-20 | 珠海冠宇电池有限公司 | A kind of electrolyte and lithium ion battery being adapted to silicon-carbon cathode |
| CN110233293A (en) * | 2019-07-23 | 2019-09-13 | 河源市聚芯源科技有限公司 | A kind of electrolyte and its preparation process improving high-temperature lithium ion battery performance |
| JP2023509767A (en) * | 2020-01-10 | 2023-03-09 | エー１２３ システムズ エルエルシー | Electrolyte components of lithium-ion batteries |
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