CN105428716A - Lithium-ion battery electrolyte and lithium-ion battery containing electrolyte - Google Patents
Lithium-ion battery electrolyte and lithium-ion battery containing electrolyte Download PDFInfo
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- CN105428716A CN105428716A CN201510930159.8A CN201510930159A CN105428716A CN 105428716 A CN105428716 A CN 105428716A CN 201510930159 A CN201510930159 A CN 201510930159A CN 105428716 A CN105428716 A CN 105428716A
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- lithium
- ion battery
- electrolyte
- battery electrolytes
- electrolytic solution
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Classifications
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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
- 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
-
- 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
-
- 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
-
- 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
The invention discloses lithium-ion battery electrolyte. The electrolyte comprises LiPF6, a non-aqueous organic solvent and additives, wherein the additives comprise fluoroalkenyl phosphate compounds and LiBOB, the structural general formula of the fluoroalkenyl phosphate compounds is the general formula I or the general formula II shown in the specification; according to the general formula, when R1 represents alkyl with 1-5 carbon atoms, R2 represents fluoroalkenyl, and when R1 represents fluoroalkyl, R2 represents any one of alkenyl with 2-5 carbon atoms and fluoroalkenyl with 2-5 carbon atoms. The flammability of the lithium-ion battery electrolyte is low, the gas production capacity of the lithium-ion battery prepared from the electrolyte is small in the charging and discharging processes, and the battery can be effectively prevented from expanding and has excellent high-temperature cycle performance.
Description
Technical field
The present invention relates to a kind of lithium-ion battery electrolytes and the lithium ion battery containing this electrolyte, particularly a kind of combustibility is lower, effectively can prevent cell expansion, improves the electrolyte of battery high-temperature behavior and the lithium ion battery containing this electrolyte.
Background technology
The electrolyte that current commercial applications is the widest is LiPF
6mixed carbonic acid ester solution, the solute LiPF in this system
6can decompose 75 DEG C time, to water sensitive, easily produce HF, corrosion collector, SEI film and electrode active material, make battery performance decay rapidly; The boiling point of solvent is low, flash-point is low, easy firing or blast, causes safety problem.Novel high thermal electrolysis matter salt, as LiODFB, LiFSI, LiFNFSI etc., or organic solvent and the ionic liquid such as the sulfone class of difficult combustion, due to exist expensive, viscosity is large, conductivity is low or with the problem such as electrode poor compatibility, also have longer distance from practical on a large scale.Therefore, use multiple additives to LiPF
6mixed carbonate ester electrolyte system to carry out modification be obtain the most effective method of high temperature safe electrolyte of excellent combination property.
Summary of the invention
The present invention is directed to lithium ion battery at high temperature easily to expand, seriously even can there is the problems such as combustion explosion in capacity attenuation, provides a kind of high temperature safe electrolyte of excellent combination property and the lithium ion battery containing this electrolyte.
In order to realize above goal of the invention, the technical solution adopted in the present invention is as follows:
A kind of lithium-ion battery electrolytes, comprises LiPF
6, non-aqueous organic solvent and additive, described additive comprises fluorophosphate alkene ester type compound and LiBOB, and wherein the general structure of fluorophosphate alkene ester type compound is general formula I or general formula II:
In above-mentioned general formula, work as R
1when=carbon number is the alkyl of 1 ~ 5, R
2=fluoro thiazolinyl; Work as R
1during=fluoro-alkyl, R
2=carbon number be 2 ~ 5 thiazolinyl or fluoro thiazolinyl in any one.
Preferably, described fluorophosphate alkene ester type compound mass percentage is in the electrolytic solution 2 ~ 20%.
Preferably, described fluorophosphate alkene ester type compound mass percentage is in the electrolytic solution preferably 5 ~ 10%.
Preferably, described LiBOB mass percentage is in the electrolytic solution 0.5 ~ 5%.
Preferably, described LiBOB mass percentage is in the electrolytic solution preferably 0.5 ~ 2%.
Preferably, described additive also comprises VC, PS, VEC and FEC and its mass percentage total is in the electrolytic solution 5 ~ 20%.
Preferably, the total in the electrolytic solution mass percentage of described VC, PS, VEC and FEC is preferably 10 ~ 15%.
Preferably, described non-aqueous organic solvent is one or more in EC, EMC, DEC, DMC and PC.
Preferably, described non-aqueous organic solvent is the mixture of EC, EMC, DEC and PC.
Preferably, a kind of lithium ion battery, the electrolyte of described electrolyte according to any one of claim 1 ~ 9, positive electrode is the transition metal oxide containing lithium, negative material is the material with carbon element of deintercalate lithium ions that can be reversible, and is placed in the porous septum between both positive and negative polarity.
Beneficial effect of the present invention is:
In the present invention, lithium-ion battery electrolytes comprises LiPF
6, non-aqueous organic solvent and additive, adopt linear carbonates, cyclic carbonate as mixed solvent, ensure that the viscosity of electrolyte system is lower, in wider temperature range, ionic conductivity is good simultaneously; Adopt multiple film forming and help film additive, synergy optimizes film forming, and protection positive/negative material, reduces gas production, suppress cell expansion, suppresses the adverse effect to cryogenic property while promoting high-temperature behavior; The fluorophosphate alkene ester type compound added in electrolyte of the present invention is prepared from by alkylene while of phosphate compounds with after fluoridizing; there is the characteristics such as low melting point, high-flash, low viscosity; anti-flammability strengthens further; thus a small amount of interpolation can reduce the combustibility of electrolyte significantly; simultaneously because carbon containing double bond contributes in positive pole film forming; fluoro-containing group contributes at cathode film formation; positive/negative material can be protected further, ensure that its interpolation can not cause excessive impact to other performance of battery.To sum up, lithium-ion battery electrolytes combustibility provided by the invention is low, and fail safe is good; Use the lithium ion battery gas production of this electrolyte few, effectively can prevent cell expansion, and the high temperature cyclic performance of battery is significantly improved.
Accompanying drawing explanation
Fig. 1 is the cycle performance figure of embodiment 1 and comparative example 1 high temperature 55 DEG C;
Fig. 2 is the cycle performance figure of embodiment 2 and comparative example 2 high temperature 55 DEG C;
Fig. 3 is the cycle performance figure of embodiment 3 and comparative example 3 high temperature 55 DEG C.
Embodiment
Below in conjunction with embodiment and accompanying drawing, the present invention is described in further detail, but embodiments of the present invention are not limited thereto.
Embodiment 1
The preparation of electrolyte: by lithium salts LiPF
6being dissolved in mass ratio is the solution obtaining 0.9mol/L in the mixed solvent of EC, EMC, DEC and PC of 40:25:30:5; Then in solution, the VC accounting for electrolyte total weight 1.5% is added, the PS of 2.5%, the VEC of 1%, the FEC of the 10% and LiBOB of 1%; And then in solution, add the fluorophosphate alkene ester class additive 1 accounting for electrolyte total weight 5%, its structural formula is as follows:
Mix, aforesaid operations is all at H
2o<1ppm, O
2carry out in the glove box of <1ppm.
The preparation of positive pole: in homogenate equipment, uses 1-METHYLPYRROLIDONE NMP as solvent, by the LiFePO of 92.5wt%
4be mixed into uniform slurry with the Kynoar PVDF of superconduction carbon black SP and 3.5wt% of 4wt%, use coating equipment to be coated on aluminium foil, after roll-in, shearing, oven dry, obtain positive plate.
The preparation of negative pole: in homogenate equipment, use distilled water as solvent, the styrene butadiene rubber sbr of the Delanium of 94.5wt% and the acetylene black of 1.5wt%, sodium carboxymethylcellulose CMC and 2.5wt% of 1.5wt% is mixed into uniform slurry, use coating equipment to be coated on Copper Foil, after roll-in, shearing, oven dry, obtain negative plate.
Battery makes: positive pole, negative pole and porous septum are turned around poling group, and it is (long: 65mm, wide: 18mm, high: 140mm) rectangular lithium ion battery 20 to be assembled into 13.5Ah1865140.The lithium-ion battery electrolytes that theres is provided of embodiment 1 is provided, places after 24h with 0.2C constant current charge to 3.65V, then 3.65V constant voltage charge until electric current reduce to 20mA by, aging, partial volume, battery makes complete.
Battery performance test: the combustibility comprising self-extinguishing time method test electrolyte; Cell expansion rate is tested; The test of high temperature 55 DEG C of 2 ~ 3.65V1C constant current charge-discharge cycle performances, charge and discharge cycles curve is see Fig. 1, and its capability retention has had relative to comparative example 1 and significantly promotes, and high temperature cyclic performance significantly improves; Normal temperature 25 DEG C of 2 ~ 3.65V0.5C constant current charge-discharge cycle performance tests and low temperature-20 DEG C of 2 ~ 3.65V0.33C constant-current discharge capability retention tests.Average after properties test, the test result obtained is in table 1.
Embodiment 2
The preparation of electrolyte: by lithium salts LiPF
6being dissolved in mass ratio is the solution obtaining 1.05mol/L in the mixed solvent of EC, EMC, DEC and PC of 30:45:20:5; Then in solution, the VC accounting for electrolyte total weight 3% is added, the PS of 0.5%, the VEC of 0.5%, the FEC of the 8% and LiBOB of 0.5%; And then in solution, add the fluorophosphate alkene ester class additive 2 accounting for electrolyte total weight 10%, its structural formula is as follows:
Mix, aforesaid operations is all at H
2o<1ppm, O
2carry out in the glove box of <1ppm.
The preparation of positive pole: in homogenate equipment, uses NMP as solvent, by the LiFePO of 92.5wt%
4be mixed into uniform slurry with the PVDF of SP and 3.5wt% of 4wt%, use coating equipment to be coated on aluminium foil, after roll-in, shearing, oven dry, obtain positive plate.
The preparation of negative pole: in homogenate equipment, use distilled water as solvent, the SBR of the Delanium of 94.5wt% and the acetylene black of 1.5wt%, CMC and 2.5wt% of 1.5wt% is mixed into uniform slurry, use coating equipment to be coated on Copper Foil, after roll-in, shearing, oven dry, obtain negative plate.
Battery makes: positive pole, negative pole and porous septum are turned around poling group, and is assembled into 13.5Ah1865140 rectangular lithium ion battery 20.The lithium-ion battery electrolytes that theres is provided of embodiment 2 is provided, places after 24h with 0.2C constant current charge to 3.65V, then 3.65V constant voltage charge until electric current reduce to 20mA by, aging, partial volume, battery makes complete.
Battery performance test: the combustibility comprising self-extinguishing time method test electrolyte; Cell expansion rate is tested; The test of high temperature 55 DEG C of 2 ~ 3.65V1C constant current charge-discharge cycle performances, charge and discharge cycles curve is see Fig. 2, and its capability retention has had relative to comparative example 2 and significantly promotes, and high temperature cyclic performance significantly improves; Normal temperature 25 DEG C of 2 ~ 3.65V0.5C constant current charge-discharge cycle performance tests and low temperature-20 DEG C of 2 ~ 3.65V0.33C constant-current discharge capability retention tests.Average after properties test, the test result obtained is in table 1.
Embodiment 3
The preparation of electrolyte: by lithium salts LiPF
6being dissolved in mass ratio is the solution obtaining 1.2mol/L in the mixed solvent of EC, EMC, DEC and PC of 40:25:30:5; Then in solution, the VC accounting for electrolyte total weight 1% is added, the PS of 3%, the VEC of 2%, the FEC of the 5% and LiBOB of 2%; And then in solution, add the fluorophosphate alkene ester class additive 3 accounting for electrolyte total weight 8%, its structural formula is as follows:
Mix, aforesaid operations is all at H
2o<1ppm, O
2carry out in the glove box of <1ppm.
The preparation of positive pole: in homogenate equipment, uses NMP as solvent, by the LiNi of 72wt%
0.5co
0.2mn
0.3o
2, 20.5% LiMn
0.8fe
0.2pO
4be mixed into uniform slurry with the PVDF of SP and 3.5wt% of 4wt%, use coating equipment to be coated on aluminium foil, after roll-in, shearing, oven dry, obtain positive plate.
The preparation of negative pole: in homogenate equipment, use distilled water as solvent, the acetylene black of carbonaceous mesophase spherules MCMB and 2.5wt% of the Delanium of 73.5wt%, 20wt%, the SBR of CMC and 2.5wt% of 1.5wt% are mixed into uniform slurry, use coating equipment to be coated on Copper Foil, after roll-in, shearing, oven dry, obtain negative plate.
Battery makes: positive pole, negative pole and porous septum are turned around poling group, and is assembled into 15Ah1865140 rectangular lithium ion battery.The lithium-ion battery electrolytes that theres is provided of embodiment 3 is provided, places after 24h with 0.2C constant current charge to 4.2V, then 4.2V constant voltage charge until electric current reduce to 20mA by, aging, partial volume, battery makes complete.
Battery performance test: the combustibility comprising self-extinguishing time method test electrolyte; Cell expansion rate is tested; The test of high temperature 55 DEG C of 3 ~ 4.2V1C constant current charge-discharge cycle performances, charge and discharge cycles curve is see Fig. 3, and its capability retention has had relative to comparative example 3 and significantly promotes, and high temperature cyclic performance significantly improves; Normal temperature 25 DEG C of 3 ~ 4.2V0.5C constant current charge-discharge cycle performance tests and low temperature-20 DEG C of 3 ~ 4.2V0.33C constant-current discharge capability retention tests.Average after properties test, the test result obtained is in table 1.
Comparative example 1
The preparation of electrolyte: by lithium salts LiPF
6being dissolved in mass ratio is the solution obtaining 0.9mol/L in the mixed solvent of EC, EMC, DEC and PC of 40:25:30:5; Then in solution, the VC accounting for electrolyte total weight 2% is added, the PS of 2.5%.
The preparation of positive pole, the preparation of negative pole, battery make and battery performance test reference example 1, uniquely unlike the lithium-ion battery electrolytes that the electrolyte injected in battery making step provides for comparative example 1.
Comparative example 2
By lithium salts LiPF
6being dissolved in mass ratio is the solution obtaining 1.05mol/L in the mixed solvent of EC, EMC, DEC and PC of 30:45:20:5; Then in solution, the VC accounting for electrolyte total weight 3% is added, the PS of 0.5%.
The preparation of positive pole, the preparation of negative pole, battery make and battery performance test reference example 2, uniquely unlike the lithium-ion battery electrolytes that the electrolyte injected in battery making step provides for comparative example 2.
Comparative example 3
By lithium salts LiPF
6being dissolved in mass ratio is the solution obtaining 1.2mol/L in the mixed solvent of EC, EMC, DEC and PC of 40:25:30:5; Then in solution, the VC accounting for electrolyte total weight 1% is added, the PS of 3%.
The preparation of positive pole, the preparation of negative pole, battery make and battery performance test reference example 3, uniquely unlike the lithium-ion battery electrolytes that the electrolyte injected in battery making step provides for comparative example 3.
Table 1 electrolyte and battery performance contrast table
Can be found out by the test result of table 1, lithium-ion battery electrolytes provided by the invention is adopted to have good fire resistance, obtained high-temperature lithium ion battery expansion rate effectively reduces and cycle performance obtains obvious improvement, affect little on normal temperature and cryogenic property simultaneously, be worthy of popularization.
As mentioned above, the present invention can be realized preferably.It should be noted that above-described embodiment of the present invention, do not form limiting the scope of the present invention.Any amendment done within the spirit and principles in the present invention, equivalent replacement and improvement etc., all should be included within claims of the present invention.
Claims (10)
1. a lithium-ion battery electrolytes, comprises LiPF
6, non-aqueous organic solvent and additive, it is characterized in that, described additive comprises fluorophosphate alkene ester type compound and LiBOB, and wherein the general structure of fluorophosphate alkene ester type compound is general formula I or general formula II:
In above-mentioned general formula, work as R
1when=carbon number is the alkyl of 1 ~ 5, R
2=fluoro thiazolinyl; Work as R
1during=fluoro-alkyl, R
2=carbon number be 2 ~ 5 thiazolinyl or fluoro thiazolinyl in any one.
2. lithium-ion battery electrolytes according to claim 1, is characterized in that, described fluorophosphate alkene ester type compound mass percentage is in the electrolytic solution 2 ~ 20%.
3. lithium-ion battery electrolytes according to claim 2, is characterized in that, described fluorophosphate alkene ester type compound mass percentage is in the electrolytic solution 5 ~ 10%.
4. lithium-ion battery electrolytes according to claim 1, is characterized in that, described LiBOB mass percentage is in the electrolytic solution 0.5 ~ 5%.
5. lithium-ion battery electrolytes according to claim 4, is characterized in that, described LiBOB mass percentage is in the electrolytic solution 0.5 ~ 2%.
6. lithium-ion battery electrolytes according to claim 1, is characterized in that, described additive also comprises VC, PS, VEC and FEC and its mass percentage total is in the electrolytic solution 5 ~ 20%.
7. lithium-ion battery electrolytes according to claim 6, is characterized in that, the total in the electrolytic solution mass percentage of described VC, PS, VEC and FEC is 10 ~ 15%.
8. lithium-ion battery electrolytes according to claim 1, is characterized in that, described non-aqueous organic solvent is selected from one or more in EC, EMC, DEC, DMC and PC.
9. lithium-ion battery electrolytes according to claim 8, is characterized in that, described non-aqueous organic solvent is the mixture of EC, EMC, DEC and PC.
10. a lithium ion battery, it is characterized in that, the electrolyte of described electrolyte according to any one of claim 1 ~ 9, positive electrode is the transition metal oxide containing lithium, negative material is the material with carbon element of deintercalate lithium ions that can be reversible, and is placed in the porous septum between both positive and negative polarity.
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| CN111276741A (en) * | 2018-12-05 | 2020-06-12 | Sk新技术株式会社 | Electrolyte for lithium secondary battery and lithium secondary battery including the same |
| US20210246098A1 (en) * | 2018-01-30 | 2021-08-12 | Daikin Industries, Ltd. | Electrolyte, electrochemical device, lithium ion secondary battery, and module |
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Application publication date: 20160323 |