CN103682440A - Lithium ion battery and electrolyte thereof - Google Patents
Lithium ion battery and electrolyte thereof Download PDFInfo
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- CN103682440A CN103682440A CN201310670853.1A CN201310670853A CN103682440A CN 103682440 A CN103682440 A CN 103682440A CN 201310670853 A CN201310670853 A CN 201310670853A CN 103682440 A CN103682440 A CN 103682440A
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- ion battery
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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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 invention discloses a lithium ion battery and an electrolyte thereof. The electrolyte comprises a nonaqueous organic solvent, a lithium salt dissolved in the nonaqueous organic solvent, and an additive dispersed in the nonaqueous organic solvent, and the additive is composed of 1,3-propanesultone, 4-fluorine-5-alkyl substituted-1,3-dioxolame-2-one represented by a general formula I, wherein R in the formula I is an alkyl group containing 1-5 carbon atoms; the lithium ion battery adopts the electrolyte as an electrolyte. Because the compound represented by the general formula 1 is promoted to form a solid electrolyte interfacial film by virtue of 1,3-propanesultone, so as to effectively restrain the decomposition reaction of the electrolyte, so that the high-temperature memory property of the lithium ion battery can be improved obviously.
Description
Technical field
The invention belongs to lithium ion battery field, more particularly, the present invention relates to the good lithium ion battery of a kind of high-temperature storage performance and electrolyte thereof.
Background technology
At present, people are more and more higher to the requirement of the electronics mobile device performances such as notebook computer, mobile phone, handheld device, panel computer, and this requirement growing to even greater heights also makes us must further improve the characteristic of battery.
In daily life, the factors such as the lasting use heating of electronic product, the rising of battery environment for use temperature all may make battery be under the condition of high temperature.In the lithium ion battery under charged state, cathode material has the reactivity of similar oxidant, anode material has the reactivity of similar reducing agent, and use under the condition of high temperature or under high voltage is equivalent to improve the activity of electrochemical reaction in electrolyte, so battery performance will be subject to very large negative effect.Now, the effect of electrolyte and its contained additive is just extremely important, how in the situation that not worsening battery performance, to reduce the generation of electrolyte side reaction, is the topic that is subject to everybody extensive concern always.
Research shows, controlling electrolyte and interelectrode interfacial reaction is the key addressing the above problem.Halogen-containing class additive becomes the focus of recent research because having high voltage withstanding and sludge proof characteristic, it can suppress the reactivity of negative electrode under high voltage, and also forms layer protecting film at anode surface.But this class additive is at high temperature but easy to decompose, the acid producing tends to make the side reaction aggravation in electrolyte, finally causes battery producing gas.
In view of this, necessary provide a kind of under hot conditions good lithium ion battery and the electrolyte thereof of memory property.
Summary of the invention
The object of the invention is to: provide a kind of under hot conditions good lithium ion battery and the electrolyte thereof of memory property.
In order to realize foregoing invention object, inventor, through concentrating on studies, finds the compound shown in general formula I to join in lithium-ion battery electrolytes, can improve significantly the storage characteristics under battery high-temperature.Accordingly, the invention provides a kind of lithium-ion battery electrolytes, it comprises non-aqueous organic solvent, is dissolved in the lithium salts in non-aqueous organic solvent and is dispersed in the additive in non-aqueous organic solvent, in described additive, contain 1, the fluoro-5-alkyl of 4-shown in 3-N-morpholinopropanesulfonic acid lactone and general formula I replaces-1,3-dioxolan-2-one
R in general formula I is the alkyl containing 1～5 carbon atom.
In the molecular structure of compounds of general formula I representative, principal character is that fluorine atom is on secondary carbon location.In research, find 1, 3-N-morpholinopropanesulfonic acid lactone (PS) can promote fluoropropylene carbonate to form solid electrolyte interface (SEI) film and improve the high-temperature storage characteristics of lithium rechargeable battery, further in research, find that the persistence of this improvement effect is relevant with the fluoro position of fluoropropylene carbonate, for example, when R is methyl, fluoro position on propene carbonate can simply be divided into: on primary carbon, fluorine replacement (is compound shown in general formula I I, the mono-fluoro methyl isophthalic acid of 4-, 3-dioxolan-2-one), on secondary carbon, on fluorine replacement (compound shown in general formula I) and tertiary carbon, fluorine replacement (is compound shown in general formula III, the fluoro-4-methyl isophthalic acid of 4-, 3-dioxolan-2-one).Wherein, the improve DeGrain of the propene carbonate that on primary carbon, fluorine replaces to battery performance; And the propene carbonate that on tertiary carbon, fluorine replaces makes the high temperature flatulence of battery serious.We think, under high-temperature condition, easily there is the E1 reaction of unimolecule cancellation in the propene carbonate of fluoro, produces appropriate fluorine ion, appropriate fluorine ion can the lithium ion in electrolyte be combined and be formed lithium fluoride, and Here it is forms one of main component of solid electrolyte interface (SEI).But, when the too high levels of fluorine ion, in solution, again than being easier to form hydrofluoric acid, cause electrolyte side reaction aggravation.Because the reaction rate in unimolecule elimination reaction shows as the secondary carbon > of tertiary carbon > primary carbon, so the propene carbonate replacing on tertiary carbon is at high temperature the most easily sloughed reaction and formed hydrofluoric acid, thereby affect the high-temperature storage performance of battery; And that the propene carbonate replacing on primary carbon is sloughed the speed of reaction is the slowest, so that cannot reach obvious improvement effect to battery performance; Only have the propene carbonate effect replacing on secondary carbon best;
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the fluoro-5-alkyl of described 4-replacement-DOX-2-ketone is preferably the fluoro-5-methyl isophthalic acid of 4-, 3-dioxolan-2-one.This is while being selected from ethyl, propyl group, butyl or amyl group due to R, on the impact of electrolyte viscosity progressively increase and the impact of alkyl branches particularly evident, therefore in order to guarantee the cryogenic property of battery, R is preferably methyl.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the percentage that compound shown in described general formula I accounts for nonaqueous electrolytic solution gross mass is 0.1%-8%.This is due to the fluoropropylene carbonate higher than 8% mass content, to be equivalent at high temperature increase the content of hydrofluoric acid, thereby worsened the memory property of battery, and the fluoropropylene carbonate of too high levels also can cause the conductivity of battery to reduce, viscosity increases, produce low temperature and analyse the danger of lithium, bring safety problem; And fluoropropylene carbonate mass content is lower than 0.1% time, its improvement to battery performance is not obvious.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the percentage that compound shown in described general formula I accounts for nonaqueous electrolytic solution gross mass is preferably 0.5～5%.Because fluoropropylene carbonate mass content is within the scope of this time, prepared lithium ion battery has best memory property.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the quality percentage composition of described PS in nonaqueous electrolytic solution is 0.3%-10%, is preferably 1-5%.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, described non-aqueous organic solvent comprises one or more in ethylene carbonate, propene carbonate, dimethyl carbonate, diethyl carbonate, dipropyl carbonate, methyl ethyl carbonate, methyl propyl carbonate, ethyl propyl carbonic acid ester, methyl formate, ethyl acetate, methyl butyrate
As a kind of improvement of lithium-ion battery electrolytes of the present invention, described lithium salts is LiPF
6, LiBF
4, LiBOB, LiClO
4, LiAsF
6, LiCF
3sO
3, Li (CF
3sO
2)
2a kind of or its combination in N.
In order to realize foregoing invention object, the present invention also provides a kind of lithium ion battery, and it comprises positive plate, negative plate, is interval in the barrier film between adjacent positive/negative plate, and electrolyte, and wherein, electrolyte is the electrolyte described in above arbitrary paragraph.
Embodiment
In order to make goal of the invention of the present invention, technical scheme and useful technique effect more clear, below in conjunction with embodiment, the present invention is further elaborated.Should be understood that, the embodiment describing in this specification is only in order to explain the present invention, is not intended to limit the present invention, and the formula of embodiment, ratio etc. can be suited measures to local conditions to make a choice and result be there is no to substantial effect.
Comparative example 1
The preparation of electrolyte: ethylene carbonate (EC), propene carbonate (PC), diethyl carbonate (DEC) are mixed with the mass ratio of 40:40:20, and add the LiPF of 12.5% mass percent
6lithium salts dissolves; Add again PS (PS), make PS mass content and be 3% electrolyte.
The preparation of positive plate: after 96:2:2 is fully uniformly mixed in 1-METHYLPYRROLIDONE dicyandiamide solution in mass ratio by active material cobalt acid lithium, conductive agent acetylene black, binding agent polyvinylidene fluoride (PVDF), be coated on Al paper tinsel and dry, cold pressing, obtain positive plate.
The preparation of negative plate: after active material graphite, conductive agent acetylene black, binding agent butadiene-styrene rubber (SBR), thickener carboxymethyl cellulose sodium (CMC) are fully uniformly mixed in deionized water solvent system according to mass ratio 95:2:2:1, be coated on Cu paper tinsel and dry, cold pressing, obtain negative plate.
The preparation of lithium ion battery: using PE porous polymer film as barrier film, positive plate, barrier film, negative plate are folded in order, make barrier film play the effect of isolation in the middle of adjacent positive/negative plate, and coiling obtains naked battery core; Naked battery core is placed in to external packing, injects the electrolyte the encapsulation that prepare, complete battery and make.
Comparative example 2
According to the method identical with comparative example 1, prepare electrolyte and lithium ion battery, when different is preparation electrolyte, also on the basis of comparative example 1, added the fluoro-4-methyl isophthalic acid of 4-, 3-dioxolan-2-one is as additive, its quality percentage composition in nonaqueous electrolytic solution is 5%
Comparative example 3
According to the method identical with comparative example 1, prepare electrolyte and lithium ion battery, when different is preparation electrolyte, also on the basis of comparative example 1, added the mono-fluoro methyl isophthalic acid of 4-, 3-dioxolan-2-one is as additive, its quality percentage composition in nonaqueous electrolytic solution is 5%
Comparative example 4
According to the method identical with comparative example 1, prepare electrolyte and lithium ion battery, when different is preparation electrolyte, do not add 1,3-N-morpholinopropanesulfonic acid lactone (PS), but added the fluoro-5-methyl isophthalic acid of 4-, 3-dioxolan-2-one is as additive, and its quality percentage composition in nonaqueous electrolytic solution is 5%.
Embodiment 1
According to the method identical with comparative example 1, prepare electrolyte and lithium ion battery, when different is preparation electrolyte, also on the basis of comparative example 1, added the fluoro-5-methyl isophthalic acid of 4-, 3-dioxolan-2-one is as additive, and its quality percentage composition in nonaqueous electrolytic solution is 0.5%.
Embodiment 2
According to the method identical with comparative example 1, prepare electrolyte and lithium ion battery, when different is preparation electrolyte, also on the basis of comparative example 1, added the fluoro-5-methyl isophthalic acid of 4-, 3-dioxolan-2-one is as additive, and its quality percentage composition in nonaqueous electrolytic solution is 1%.
Embodiment 3
According to the method identical with comparative example 1, prepare electrolyte and lithium ion battery, when different is preparation electrolyte, also on the basis of comparative example 1, added the fluoro-5-methyl isophthalic acid of 4-, 3-dioxolan-2-one is as additive, and its quality percentage composition in nonaqueous electrolytic solution is 5%.
Embodiment 4
According to the method identical with comparative example 1, prepare electrolyte and lithium ion battery, when different is preparation electrolyte, also on the basis of comparative example 1, added the fluoro-5-methyl isophthalic acid of 4-, 3-dioxolan-2-one is as additive, and its quality percentage composition in nonaqueous electrolytic solution is 8%.
Embodiment 5
According to the method identical with comparative example 1, prepare electrolyte and lithium ion battery, when different is preparation electrolyte, by 1, the mass percent of 3-N-morpholinopropanesulfonic acid lactone (PS) changes 1% into, and added the fluoro-5-methyl isophthalic acid of 4-, 3-dioxolan-2-one is as additive, and its quality percentage composition in nonaqueous electrolytic solution is 1%.
Embodiment 6
According to the method identical with comparative example 1, prepare electrolyte and lithium ion battery, when different is preparation electrolyte, by 1, the mass percent of 3-N-morpholinopropanesulfonic acid lactone (PS) changes 5% into, and added the fluoro-5-methyl isophthalic acid of 4-, 3-dioxolan-2-one is as additive, and its quality percentage composition in nonaqueous electrolytic solution is 5%.
Embodiment 7
According to the method identical with comparative example 1, prepare electrolyte and lithium ion battery, when different is preparation electrolyte, also on the basis of comparative example 1, added the fluoro-5-ethyl-DOX-2-of 4-ketone as additive, its quality percentage composition in nonaqueous electrolytic solution is 5%
Embodiment 8
According to the method identical with comparative example 1, prepare electrolyte and lithium ion battery, when different is preparation electrolyte, also on the basis of comparative example 1, added the fluoro-5-propyl group-DOX-2-of 4-ketone as additive, its quality percentage composition in nonaqueous electrolytic solution is 5%
High-temperature storage characteristics test
Get each 5 of the lithium ion batteries that embodiment 1～9 and comparative example 1～3 make, at normal temperatures with 0.5C multiplying power constant current charge to 4.35V, further under 4.35V constant voltage, charge to electric current and be low to moderate 0.05C, make it in 4.35V fully charged state, measure full rechargable battery thickness as the front thickness of storage; Again the battery of fully charged state is placed in to 60 ℃ of baking ovens of constant temperature, places after 20 days and measure immediately cell thickness as the rear thickness of storage.Get the mean value of each Battery pack storage front and back thickness, and according to following formula, calculate each Battery pack and store the thickness swelling after corresponding number of days: thickness swelling (%)=(the front thickness of thickness-storage after storage) front thickness * 100% of/storage; The result of experiment gained is as shown in table 1.
The high-temperature lithium ion battery storage result of the test of table 1, embodiment and comparative example
From the Data Comparison of comparative example and embodiment, can find out, the fluoro-5-methyl isophthalic acid of propene carbonate 4-replacing on primary carbon position, 3-dioxolan-2-one can suppress at high temperature aerogenesis of battery preferably, as, the thickness swelling of comparative example 1 is 41%, and the mass content of embodiment 2 and 3(propene carbonate is respectively 1% and 5%) thickness swelling all have the obvious improvement of 18-25 percentage point; Yet by contrast, with the fluoro-4-methyl isophthalic acid of 4-replacing on tertiary carbon, 3-dioxolan-2-one is as the comparative example 2 of additive, the high temperature flatulence of battery is just still very obvious, and this is relevant with the unsteadiness of fluoro structure on tertiary carbon under high temperature; With the mono-fluoro methyl isophthalic acid of 4-replacing on primary carbon, 3-dioxolan-2-one, as the comparative example 3 of additive, improves effect also not obvious.
The announcement of book and instruction according to the above description, those skilled in the art in the invention can also carry out suitable change and modification to above-mentioned execution mode.Therefore, the present invention is not limited to embodiment disclosed and described above, to modifications and changes more of the present invention, also should fall in the protection range of claim of the present invention.In addition,, although used some specific terms in this specification, these terms just for convenience of description, do not form any restriction to the present invention.
Claims (9)
1. a lithium-ion battery electrolytes, it comprises non-aqueous organic solvent, is dissolved in the lithium salts in non-aqueous organic solvent and is dispersed in the additive in non-aqueous organic solvent, it is characterized in that: in described additive, contain 1, the fluoro-5-alkyl of 4-shown in 3-N-morpholinopropanesulfonic acid lactone and general formula I replaces-1,3-dioxolan-2-one
R in general formula I is the alkyl containing 1～5 carbon atom.
2. lithium-ion battery electrolytes according to claim 1, is characterized in that: the fluoro-5-alkyl of described 4-replacement-DOX-2-ketone is preferably the fluoro-5-methyl isophthalic acid of 4-, 3-dioxolan-2-one.
3. lithium-ion battery electrolytes according to claim 1, is characterized in that: the percentage that compound shown in general formula I accounts for nonaqueous electrolytic solution gross mass is 0.1%-8%.
4. lithium-ion battery electrolytes according to claim 1, is characterized in that: the percentage that compound shown in general formula I accounts for nonaqueous electrolytic solution gross mass is preferably 0.5～5%.
5. lithium-ion battery electrolytes according to claim 1, is characterized in that: the quality percentage composition of described PS in nonaqueous electrolytic solution is 0.3%-10%.
6. lithium-ion battery electrolytes according to claim 1, is characterized in that: the quality percentage composition of described PS in nonaqueous electrolytic solution is preferably 1-5%.
7. lithium-ion battery electrolytes according to claim 1, is characterized in that: described non-aqueous organic solvent comprises one or more in ethylene carbonate, propene carbonate, dimethyl carbonate, diethyl carbonate, dipropyl carbonate, methyl ethyl carbonate, methyl propyl carbonate, ethyl propyl carbonic acid ester, methyl formate, ethyl acetate, methyl butyrate.
8. lithium-ion battery electrolytes according to claim 1, is characterized in that: described lithium salts is LiPF
6, LiBF
4, LiBOB, LiClO
4, LiAsF
6, LiCF
3sO
3, Li (CF
3sO
2)
2a kind of or its combination in N.
9. a lithium ion battery, comprises positive plate, negative plate, is interval in the barrier film between adjacent positive/negative plate, and electrolyte, it is characterized in that: described electrolyte is the electrolyte described in any one in claim 1 to 8.
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US9673450B2 (en) | 2011-09-02 | 2017-06-06 | Solvay Sa | Lithium ion battery |
| US9979050B2 (en) | 2011-09-02 | 2018-05-22 | Solvay Sa | Fluorinated electrolyte compositions |
| US10044066B2 (en) | 2012-06-01 | 2018-08-07 | Solvary SA | Fluorinated electrolyte compositions |
| US10074874B2 (en) | 2012-06-01 | 2018-09-11 | Solvay Sa | Additives to improve electrolyte performance in lithium ion batteries |
| US10686220B2 (en) | 2013-04-04 | 2020-06-16 | Solvay Sa | Nonaqueous electrolyte compositions |
| CN112635824A (en) * | 2019-10-08 | 2021-04-09 | 上海比亚迪有限公司 | Lithium ion battery electrolyte and lithium ion battery |
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| US9673450B2 (en) | 2011-09-02 | 2017-06-06 | Solvay Sa | Lithium ion battery |
| US9979050B2 (en) | 2011-09-02 | 2018-05-22 | Solvay Sa | Fluorinated electrolyte compositions |
| US10044066B2 (en) | 2012-06-01 | 2018-08-07 | Solvary SA | Fluorinated electrolyte compositions |
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| CN112635824A (en) * | 2019-10-08 | 2021-04-09 | 上海比亚迪有限公司 | Lithium ion battery electrolyte and lithium ion battery |
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