CN105390748A - Lithium ion battery electrolyte and lithium ion battery - Google Patents
Lithium ion battery electrolyte and lithium ion battery Download PDFInfo
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- CN105390748A CN105390748A CN201510923356.7A CN201510923356A CN105390748A CN 105390748 A CN105390748 A CN 105390748A CN 201510923356 A CN201510923356 A CN 201510923356A CN 105390748 A CN105390748 A CN 105390748A
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- lithium
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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
-
- 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
-
- 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 a lithium ion battery electrolyte. The lithium ion battery electrolyte comprises solvent, lithium salt and an additive; the solvent is prepared from fluoroethylene carbonate, vinylene carbonate, a thionyl compound and a sulphonate compound; the charging mass of the components of the additive are as follows based on 100% of the total mass of the lithium ion battery electrolyte: 0.5-5% of fluoroethylene carbonate, 0.5-3% of vinylene carbonate, 0.1-1% of thionyl compound and 0.1-1% of sulphonate compound; the solvent is prepared from fluoroaliphatic solvent and other organic solvent at the charging volume ratio of 1-3:1 in a mixing manner; and the other organic solvent is selected from one or a combination of more of ethylene carbonate, propylene carbonate or fluoroethylene carbonate. The lithium ion battery provided by the invention is safe in use, high in capacity, high in specific energy, long in cycle life and less in high temperature gas yield; and in addition, the initial efficiency, the cycle performance and the high-temperature storage performance of the lithium ion battery in a high voltage system of greater than 4.4 V are all improved.
Description
Technical field
The present invention relates to a kind of lithium-ion battery electrolytes and a kind of lithium ion battery.
Background technology
In existing practical secondary battery system, the significant advantages such as specific energy is high because having for lithium ion battery, specific power is large, have extended cycle life, memory-less effect, self discharge are little, for a long time always firmly in occupation of the market of the portable type electronic products such as mobile communication, laptop computer, digital camera, and be considered to the first-selection of new energy resource power battery and energy-storage battery from now on.In order to meet higher requirement, all many-sided researchs such as lithium ion battery plus-negative plate material, electrolyte also deepen continuously.
Lithium ion battery due to its energy density high, good cycle, the advantages such as environmental protection is pollution-free are widely used, and become the first-selected electrokinetic cell of electric automobile and hybrid electric vehicle.Along with the progressively development of electric automobile and hybrid electric vehicle, the advantages such as have higher requirement to the performance of lithium ion battery, need it to have energy density high, fail safe is good, and storge quality is good.
And existing lithium battery has the following disadvantages: 1, lithium-ion battery electrolytes generally adopts carbonic ester as solvent, wherein linear carbonate can improve charge/discharge capacity and the cycle life of battery, but their flash-point is lower, at a lower temperature namely can flash burn, cause lithium ion battery in the process used, there is potential safety hazard; 2, according to solvent be binary based on the ethylene carbonate (EC) that dielectric constant is large or ternary mixed solvent, linear carbonate (DMC, DEC or EMC), carboxylate or ethers are cosolvent.It is high, good and can form the features such as stable SEI film at both positive and negative polarity with the dissolubility of lithium salts that these common solvent have conductivity, is thus considered to the optimal selection of electrolyte series solvent.But, along with high-voltage anode material LiNi
0.5mn
1.5o
4, LiMPO
4the exploitation of (M=Mn, Co, V) etc., their charge cutoff voltage is all at more than 4.7V, and traditional organic solvent is when current potential reaches 4.5V, irreversible oxidation Decomposition can be there is on the positive electrode surface of high oxidation activity, and the problems such as boiling point is low, flash-point is low, easy firing that it also exists, seriously hinder the development & application of high-voltage lithium ion batteries; When 3, being used in lithium-ion battery electrolytes according to fluorinated ethylene carbonate, vinyl ethylene carbonate and cyclic sulfates combined additive, only at below 4.2V, use the lithium ion battery of this electrolyte just can show good cycle performance and memory property.
Therefore, be badly in need of now a kind of new lithium-ion battery electrolytes of exploitation, with under the prerequisite meeting lithium ion battery use safety, improve the cycle performance of lithium ion battery under high pressure system, the first combination property such as efficiency, high-temperature storage performance.
Summary of the invention
An object of the present invention is to provide a kind of lithium-ion battery electrolytes, this battery electrolyte overcomes the deficiencies in the prior art, ensure that the fail safe that lithium ion battery uses, improve the combination properties such as the first efficiency of lithium ion battery under high voltage system, cycle performance, high-temperature storage performance and low temperature charge-discharge performance simultaneously.
For achieving the above object, the technical solution used in the present invention is: a kind of lithium-ion battery electrolytes, comprise solvent, lithium salts and additive, described additive is by fluorinated ethylene carbonate, vinylene carbonate, thionyl compound and sulfonates compounds form, in the gross mass 100% of described lithium-ion battery electrolytes, in described additive, the quality that feeds intake of each component is respectively: fluorinated ethylene carbonate 0.5% ~ 5%, vinylene carbonate 0.5% ~ 3%, thionyl compound 0.1% ~ 1%, sulfonates compounds 0.1% ~ 1%, described solvent is by fluoro fatsolvent and other organic solvents volume mixture that feeds intake by 1 ~ 3:1, other described organic solvents are for being selected from ethylene carbonate, propene carbonate, one or more combination in chlorocarbonic acid vinyl acetate.
Preferably, described thionyl compound is one or more the combination be selected from ethylene sulfite, propylene sulfite, dimethyl sulfite, sulfurous acid diethyl ester.
Preferably, described sulfonates compounds is for being selected from one or more the combination in 1,3-propane sultone, Isosorbide-5-Nitrae-butane sultones, ethylmethane sulfonate.
Preferably, described fluoro fatsolvent is a kind of in three fluoropropylene carbonates, two fluoro methyl acetates or both combinations.
Further preferably, in described solvent, the mass ratio that feeds intake of described fluoro fatsolvent and other organic solvents is 1.5 ~ 2:1.
Preferably, described lithium salts is for being selected from lithium hexafluoro phosphate, LiBF4, lithium perchlorate, di-oxalate lithium borate, difluorine oxalic acid boracic acid lithium, two (trimethyl fluoride sulfonyl) imine lithium and one or more in two fluorine sulfimide lithium, and the concentration that adds of described lithium salts is 0.5 ~ 1.0mol/L.
Another object of the present invention is to provide a kind of lithium ion electronic cell, comprises positive plate, negative plate, lithium battery diaphragm and above-mentioned lithium-ion battery electrolytes; Wherein, described positive plate active material be selected from cobalt acid lithium, nickle cobalt lithium manganate or nickel ion doped one or more, described negative plate active material be selected from graphite, Si-C composite material one or more.
Due to the utilization of technique scheme, the present invention compared with prior art has following advantages: the electrolyte of lithium ion battery of the present invention, have employed the solvent of fluorinated solvents as electrolyte, and fluorinated solvents has higher flash-point usually even without flash-point, therefore compared with prior art, fluorinated solvents is adopted to be conducive to suppressing the burning of electrolyte in a solvent, lithium battery is used safer, and the advantage such as the battery that have employed fluorinated solvents has that capacitance is high, specific energy large, have extended cycle life, high temperature aerogenesis is few.And adopt additive of the present invention, significantly can promote the first efficiency of lithium ion battery under the high pressure system of more than 4.4V, cycle performance, high-temperature storage performance.
Embodiment
The restriction that the present invention is not special to the source of all raw materials, for commercially available.
Below as nothing specializes, the content in embodiment is mass percentage.Wherein, the quality of each constituent mass/solvent of the mass percentage=100% × solvent of each component in solvent; The gross mass of each constituent mass/nonaqueous electrolytic solution of the percentage composition=100% × additive of each component in additive.
Comparative example 1
The preparation of electrolyte: ethylene carbonate (EC), propene carbonate (PC), diethyl carbonate (DEC) are mixed with mass ratio EC:PC:DEC=20:20:60, adds the lithium hexafluoro phosphate (LiPF of certain mass
6), make its concentration in the electrolytic solution be 1mol/L; In addition be also added with the fluorinated ethylene carbonate (FEC) that mass percentage content is 15% in electrolyte, mass percentage content is the PS (1,3-PS) of 5%.
Comparative example 2
The preparation of electrolyte: ethylene carbonate (EC), propene carbonate (PC) and diethyl carbonate (DEC) are mixed with mass ratio EC:PC:DEC=15:20:65, adds the lithium hexafluoro phosphate (LiPF of certain mass
6), make its concentration in the electrolytic solution be 1mol/L; In addition the fluorinated ethylene carbonate (FEC) that mass percentage content is 15% is also added with in electrolyte, the vinyl ethylene carbonate (VEC) of 5%, the PS (1,3-PS) of 5%.
Embodiment 1
The preparation of electrolyte: by three fluoropropylene carbonates (TFPC), ethylene carbonate (EC), propene carbonate (PC) with mass ratio TFPC:EC:PC=70:10:20, add the lithium hexafluoro phosphate (LiPF of certain mass
6), make its concentration in the electrolytic solution be 1mol/L; In addition the fluorinated ethylene carbonate (FEC) that mass percentage content is 5% is also added with in electrolyte, the vinylene carbonate (VC) of 0.5%, the ethylene sulfite (ES) of 0.3%, 0.3% 1,3-N-morpholinopropanesulfonic acid lactone (1,3-PS).
Here, fluoro fatsolvent can be a kind of in three fluoropropylene carbonates, two fluoro methyl acetates or both combinations.Other organic solvent can be one or more the combination in ethylene carbonate, propene carbonate, chlorocarbonic acid vinyl acetate.
Here, the lithium salts adopted in electrolyte can be lithium hexafluoro phosphate, lithium fluoroborate, lithium perchlorate, di-oxalate lithium borate, difluorine oxalic acid boracic acid lithium, two (trimethyl fluoride sulfonyl) imine lithium and one or more in two fluorine sulfimide lithium.
Here, the thionyl compound in additive can be one or more the combination in sulfuric acid vinyl ester, propylene sulfite, dimethyl sulfite, sulfurous acid diethyl ester; Sulfonates compounds can be one or more the combination in 1,3-propane sultone, Isosorbide-5-Nitrae-butane sultones, ethylmethane sulfonate.
Embodiment 2
The preparation of electrolyte: by three fluoropropylene carbonates (TFPC), ethylene carbonate (EC), propene carbonate (PC) with mass ratio TFPC:EC:PC=65:15:20, add the lithium hexafluoro phosphate (LiPF of certain mass
6), make its concentration in the electrolytic solution be 1mol/L; In addition the fluorinated ethylene carbonate (FEC) that mass percentage content is 5% is also added with in electrolyte, the vinylene carbonate (VC) of 0.5%, the ethylene sulfite (ES) of 0.3%, 0.3% 1,3-N-morpholinopropanesulfonic acid lactone (1,3-PS).
Embodiment 3
The preparation of electrolyte: by three fluoropropylene carbonates (TFPC), two fluoro methyl acetates (MFA), ethylene carbonate (EC), propene carbonate (PC) with mass ratio TFPC:MFA:EC:PC=40:30:10:20, add the lithium hexafluoro phosphate (LiPF of certain mass
6), make its concentration in the electrolytic solution be 1mol/L; In addition the fluorinated ethylene carbonate (FEC) that mass percentage content is 5% is also added with in electrolyte, the vinylene carbonate (VC) of 0.5%, the ethylene sulfite (ES) of 0.3%, 0.3% 1,3-N-morpholinopropanesulfonic acid lactone (1,3-PS).
Embodiment 4
The preparation of electrolyte: by three fluoropropylene carbonates (TFPC), two fluoro methyl acetates (MFA), ethylene carbonate (EC), chlorocarbonic acid vinyl acetate (CIEC) with mass ratio TFPC:MFA:EC:CIEC=40:25:15:20, add the lithium hexafluoro phosphate (LiPF of certain mass
6), make its concentration in the electrolytic solution be 1mol/L; In addition the fluorinated ethylene carbonate (FEC) that mass percentage content is 5% is also added with in electrolyte, the vinylene carbonate (VC) of 0.5%, the ethylene sulfite (ES) of 0.3%, 0.3% 1,3-N-morpholinopropanesulfonic acid lactone (1,3-PS).
Embodiment 5
The preparation of electrolyte: by three fluoropropylene carbonates (TFPC), ethylene carbonate (EC), chlorocarbonic acid vinyl acetate (CIEC) with mass ratio TFPC:EC:CIEC=60:20:20, add the lithium hexafluoro phosphate (LiPF of certain mass
6), make its concentration in the electrolytic solution be 1mol/L; In addition the fluorinated ethylene carbonate (FEC) that mass percentage content is 3% is also added with in electrolyte, the vinylene carbonate (VC) of 1%, the ethylene sulfite (ES) of 0.5%, 0.5% 1,3-N-morpholinopropanesulfonic acid lactone (1,3-PS), the Isosorbide-5-Nitrae-butane sultones (Isosorbide-5-Nitrae-BS) of 0.3%.
Embodiment 6
The preparation of electrolyte: by three fluoropropylene carbonates (TFPC), ethylene carbonate (EC) with mass ratio TFPC:EC=70:30, add the lithium hexafluoro phosphate (LiPF of certain mass
6), make its concentration in the electrolytic solution be 0.7mol/L; In addition the fluorinated ethylene carbonate (FEC) that mass percentage content is 3% is also added with in electrolyte, the vinylene carbonate (VC) of 1%, the propylene sulfite (PS) of 0.5%, 0.5% 1,4-butane sultones (Isosorbide-5-Nitrae-BS).
Embodiment 7
The preparation of electrolyte: by two fluoro methyl acetates (MFA), ethylene carbonate (EC) with mass ratio MFA:EC=70:30, add the lithium hexafluoro phosphate (LiPF of certain mass
6), make its concentration in the electrolytic solution be 0.7mol/L; In addition the fluorinated ethylene carbonate (FEC) that mass percentage content is 5% is also added with in electrolyte, the vinylene carbonate (VC) of 0.5%, the propylene sulfite (PS) of 0.3%, 0.3% 1,4-butane sultones (Isosorbide-5-Nitrae-BS).
Lithium-ion battery electrolytes prepared by the lithium-ion battery electrolytes prepare above-described embodiment 1 ~ 7 and comparative example 1 ~ 2 injects through fully dry graphite/LiNi
0.5mn
0.3co
0.2o
2battery, battery leaves standstill through an envelope, preliminary filling changes into, carry out 3.0V ~ 4.4V0.5C cycle charge discharge electrical testing after two envelope partial volumes and the full electric state 60 DEG C/6H of 4.4V stores test.
3.0V ~ 4.4V0.5C cycle charge discharge electrical testing:
Under the condition of room temperature 25 ± 2 DEG C, carry out the test of 3.0V-4.4V circulating battery to embodiment and comparative example experimental cell, testing procedure is: A, 0.5C constant current charge is to 4.4V, and then constant voltage charge is to cut-off current 0.005C, leaves standstill 5 minutes; B, 0.5C constant-current discharge, to 3.0V, leaves standstill 5 minutes; C, circulation step A and B, cycle-index is 400 times.Calculate efficiency=(discharge capacity first/initial charge capacity) × 100% first, the capability retention after circulation=(discharge capacity after corresponding cycle-index/discharge capacity first) × 100%.
The full electric state 60 DEG C/6H of 4.4V stores test:
A, under the condition of room temperature 25 ± 2 DEG C, 0.5C charge-discharge test is carried out to embodiment and comparative example experimental cell, capacity before record stores; B, 0.5C constant-current constant-voltage charging is to 4.4V, and cut-off current is 0.005C, the full electric state thickness of test battery; C, full electric state battery is transferred in 85 DEG C of insulating boxs, stores the hot thickness of test battery after 6 hours, thickness * 100% before hot thickness swelling=(before the hot thickness-storage of battery thickness)/store; D, by cooled battery 0.5C constant-current discharge to 3.0V, residual capacity after record stores, the front capacity * 100% of residual capacity/storage after battery capacity surplus ratio=storages; E, battery time is carried out 0.5C charge-discharge test, record can recover capacity after storing, and can recover the front capacity * 100% of capacity/storages after capacity resuming rate=storage.Test result is as table 1.
Table 1
As can be seen from Table 1, compare ratio 1 ~ 2 and detect the efficiency first obtained, the entirety of efficiency first of embodiment 1 ~ 7 rises all to some extent, and hot thickness swelling declines all to some extent, fluoro fatsolvent is added in lithium battery electrolytes, make the flash-point of electrolyte high, use safety, high temperature aerogenesis is few, and with the addition of fluorinated ethylene carbonate, vinylene carbonate and thionyl compound, sulfonates compounds, give full play to the advantage of this several additive, improve the first efficiency of lithium ion battery under 4.4V high pressure system, cycle performance and high-temperature storage performance.
Adopt fluorinated solvents to be conducive to suppressing the burning of electrolyte in a solvent, lithium battery is used safer, and the battery that have employed fluorinated solvents has advantages such as capacitance is high, specific energy large, have extended cycle life, high temperature aerogenesis is few.And adopt additive of the present invention, significantly can promote the first efficiency of lithium ion battery under the high pressure system of more than 4.4V, cycle performance, high-temperature storage performance.
Above-described embodiment is only for illustrating technical conceive of the present invention and feature; its object is to person skilled in the art can be understood content of the present invention and be implemented; can not limit the scope of the invention with this; all equivalences done according to Spirit Essence of the present invention change or modify, and all should be encompassed in protection scope of the present invention.
Claims (7)
1. a lithium-ion battery electrolytes, comprise solvent, lithium salts and additive, it is characterized in that, described additive is by fluorinated ethylene carbonate, vinylene carbonate, thionyl compound and sulfonates compounds form, in the gross mass 100% of described lithium-ion battery electrolytes, in described additive, the quality that feeds intake of each component is respectively: fluorinated ethylene carbonate 0.5% ~ 5%, vinylene carbonate 0.5% ~ 3%, thionyl compound 0.1% ~ 1%, sulfonates compounds 0.1% ~ 1%, described solvent is by fluoro fatsolvent and other organic solvents volume mixture that feeds intake by 1 ~ 3:1, other described organic solvents are for being selected from ethylene carbonate, propene carbonate, one or more combination in chlorocarbonic acid vinyl acetate.
2. lithium-ion battery electrolytes according to claim 1, is characterized in that: described thionyl compound is one or more the combination be selected from ethylene sulfite, propylene sulfite, dimethyl sulfite, sulfurous acid diethyl ester.
3. lithium-ion battery electrolytes according to claim 1, is characterized in that: described sulfonates compounds is for being selected from one or more the combination in 1,3-propane sultone, Isosorbide-5-Nitrae-butane sultones, ethylmethane sulfonate.
4. lithium-ion battery electrolytes according to claim 1, is characterized in that: described fluoro fatsolvent is a kind of in three fluoropropylene carbonates, two fluoro methyl acetates or both combinations.
5. lithium-ion battery electrolytes according to claim 1, is characterized in that: in described solvent, and the mass ratio that feeds intake of described fluoro fatsolvent and other organic solvents is 1.5 ~ 2:1.
6. lithium-ion battery electrolytes according to claim 1, it is characterized in that: described lithium salts is for being selected from lithium hexafluoro phosphate, LiBF4, lithium perchlorate, di-oxalate lithium borate, difluorine oxalic acid boracic acid lithium, two (trimethyl fluoride sulfonyl) imine lithium and one or more in two fluorine sulfimide lithium, and the concentration that adds of described lithium salts is 0.5 ~ 1.0mol/L.
7. a lithium ion electronic cell, is characterized in that, comprises positive plate, negative plate, lithium battery diaphragm and the lithium-ion battery electrolytes described in any one of claim 1 ~ 6 claim; Wherein, described positive plate active material be selected from cobalt acid lithium, nickle cobalt lithium manganate or nickel ion doped one or more, described negative plate active material be selected from graphite, Si-C composite material one or more.
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| CN106099188A (en) * | 2016-07-27 | 2016-11-09 | 芜湖凯尔电气科技有限公司 | Explosion-proof lithium-ion battery electrolytes |
| CN106450450A (en) * | 2016-09-19 | 2017-02-22 | 深圳拓邦新能源技术有限公司 | Battery electrolyte and preparation method therefor, and lithium battery |
| CN106450454A (en) * | 2016-10-19 | 2017-02-22 | 中航锂电（洛阳）有限公司 | Electrolyte and lithium ion battery using electrolyte |
| CN106450451A (en) * | 2016-09-19 | 2017-02-22 | 深圳拓邦新能源技术有限公司 | Battery electrolyte and preparation method therefor, and lithium battery |
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