CN103094614B - Lithium ion battery electrolyte and lithium ion battery containing same - Google Patents
Lithium ion battery electrolyte and lithium ion battery containing same Download PDFInfo
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- CN103094614B CN103094614B CN201310023387.8A CN201310023387A CN103094614B CN 103094614 B CN103094614 B CN 103094614B CN 201310023387 A CN201310023387 A CN 201310023387A CN 103094614 B CN103094614 B CN 103094614B
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The invention discloses a lithium ion battery electrolyte and a lithium ion battery containing same, relating to the battery field. Through using the lithium-ion battery electrolyte disclosed by the invention, the acidity of the electrolyte can be effectively controlled, and further the cycle performance and the high-temperature storage performance can be obviously improved. The lithium-ion battery electrolyte disclosed by the invention comprises lithium salt, non-aqueous organic solvent and stabilizing additive, wherein the stabilizing additive is silazane derivative, and the structure of the silazane is shown in the specification, wherein any one of R1, R2, R3, R4, R5 and R6 is selected from hydrogen atom, alkyl group, phenyl group, biphenylyl group, phenylate group, haloalkyl group, halogeno benzene group and halogenated biphenyl group, the alkyl group is the linear chain alkyl or the branch chain alkyl of C1-C20, and the halogen is F, Br, Cl, I.
Description
Technical field
The present invention relates to field of batteries, particularly relate to a kind of lithium-ion battery electrolytes and the lithium ion battery containing this electrolyte.
Background technology
Lithium ion battery is primarily of positive electrode, negative material, electrolyte, barrier film four part composition, and wherein, electrolyte is the ion conductor playing conduction between battery positive and negative electrode, is generally made up of electrolyte lithium salt and organic solvent two parts.In commercial lithium-ion batteries, widely used electrolyte lithium salt is generally LIPF
6organic solvent generally has two or more organic solvent to mix, and is mainly chain and the cyclic carbonates such as vinyl carbonate ethylene carbonate (EC), propene carbonate (PC), dimethyl carbonate (DMC), diethyl carbonate (DEC), methyl ethyl carbonate (EMC).
The performance of electrolyte affects the performance of battery to a great extent, and the factor affecting the good and bad performance of electrolyte mainly contains two aspects: the content of impurity in the composition of electrolyte and electrolyte.Wherein, in electrolyte, contained HF has tremendous influence to the stability of electrolyte and battery performance.
HF affects main manifestations both ways to electrolyte self stability: catalysis lithium salts is as LiPF
6hydrolysis, thus accelerate the rotten of electrolyte; The polymerization of Organic Solvents, thus cause electrolyte viscosity to increase, conductivity reduces.
The impact of HF on battery performance is mainly manifested in three aspects:
First, HF, in battery first charge-discharge process, Carbon anode occurs following electrochemical reducting reaction:
HF+e
-+Li
+→LiF↓+1/2H
2
Above-mentioned reaction not only can be limited in consuming cells lithium ion, increase inner pressure of battery, and the LiF conductive capability generated is poor, in Carbon anode surface solid electrolyte interface (SEI) membrane component, LiF content increases, cause electrode/electrolyte interface impedance to increase, thus increase the internal resistance of cell.
Secondly, HF can react with the SEI film of electrolytic surface, generates water or alcohol etc.Aurbach etc. think in the electrolyte of EC base, and following reaction mainly occurs HF and SEI film:
Li
2CO
3+2HF→2LiF+H
2O+CO
2
The LiF generated in above-mentioned reaction can cause electrode/electrolyte interface impedance to increase equally, in addition, the water generated in reaction and ethylene glycol again can and LiPF
6reaction generates HF, and this process constantly circulates, and causes battery specific capacity, cycle efficieny constantly reduces, until whole battery is destroyed.
Finally, HF meeting and positive electrode active materials are as LiMn
2o
4react, cause the dissolving of part manganese, this causes LiMn
2o
4the one of the main reasons of capacity attenuation, reaction principle is as follows:
LiMn
2O
4+H
+→Li
++λ-MnO
2+Mn
2++2H
2O
For the impact of HF on electrolyte and battery performance, the mixture of one or more in the oxide of zinc, aluminium, magnesium, calcium or magnesium or aluminium is adopted to join in electrolyte as additive in prior art, in they and electrolyte, the HF of trace reacts, reduce the content of HF, stop its to the destruction of electrode and to lithium salts as LiPF
6the catalytic action of decomposing, improves the stability of electrolyte, improves battery performance.
But the above-mentioned method speed except HF is slow, and easily introduces metal impurities with metal or metal oxide treated electrolyte.
In addition, (chemical formula is (CH can also to adopt hexamethyldisiloxane in prior art
3)
3siNHSi (CH
3)
3) be added in electrolyte as additive, its mechanism of action is:
(CH
3)
3SiNHSi(CH
3)
3+H
2O→(CH
3)
3SiOSi(CH
3)
3+NH
3
NH
3+HF→NH
4F
Hexamethyldisiloxane and water react and generate NH
3, then NH
3react with HF again and generate NH
4f, and then the content reducing HF in electrolyte, improve the cycle performance of lithium ion battery.But in the method, HMDO itself is unstable, easily decomposes in atmosphere, not easily preserves; And NH
3the NH generated is reacted with HF
4f is unstable, especially at high temperature easily decomposes, and is difficult to play the object improving high-temperature lithium ion battery performance.
Summary of the invention
Embodiments of the invention provide a kind of lithium-ion battery electrolytes and the lithium ion battery containing this electrolyte, effectively can control the acidity of electrolyte, improve cycle life and the high-temperature storage performance of lithium ion battery.
The above-mentioned purpose of the embodiment of the present invention is achieved by the following technical solution:
A kind of lithium-ion battery electrolytes, described electrolyte comprises: solute, solvent, stabilization additives, described stabilization additives silazane derivatives, and described silazane derivatives structure is:
In above formula, R
1, R
2, R
3, R
4, R
5and R
6arbitrary is a kind of in H, alkyl, phenyl, xenyl, phenylate base, haloalkyl, halogenophenyl, halogenated biphenyl base, and wherein, described alkyl is C
1-C
20straight or branched alkyl, halogen is F, Br, Cl, I.
Preferably, the content of described silazane derivatives is the 0.1%-50% of electrolyte total weight.
In the lithium-ion battery electrolytes that the embodiment of the present invention provides, described solute is lithium salts, and described lithium salts can be the various lithium salts that this area is commonly used, and is preferably LiPF
6, LiBF
4, LiClO
4, LiPF
3(CF
2cF
3)
3, LiCF
3sO
3with one or more in LiBOB.
In the lithium-ion battery electrolytes that the embodiment of the present invention provides, described solvent is non-aqueous organic solvent, described non-aqueous organic solvent can be the various non-aqueous organic solvents that this area is commonly used, and is preferably one or more in carbonic ester and halo derivatives, ester, ether and ketone.
In the lithium-ion battery electrolytes that the embodiment of the present invention provides, also comprise film for additive, described film for additive can be the various film for additive that this area is commonly used, be preferably vinylene carbonate, vinylethylene carbonate, 1, one or more in 3-sulfonic acid propiolactone and Isosorbide-5-Nitrae-sulfonic acid butyrolactone.Preferably, described film for additive content is the 0.1%-50% of electrolyte total weight.
A kind of lithium ion battery, comprising: electrolyte, positive pole, negative pole, described positive pole, negative pole are that positive pole, negative pole are commonly used in this area, the electrolyte that described electrolyte provides for the embodiment of the present invention.
The lithium-ion battery electrolytes that the embodiment of the present invention provides and the lithium ion battery containing this electrolyte, by adding stabilization additives silazane derivatives, can be hydrolyzed with lithium salts in electrolyte the hydrogen ion produced to react and generate stable compound, thus the effective acidity controlling electrolyte, improve cycle life and the high-temperature storage performance of lithium ion battery.
Embodiment
Clearly understand to make the object of the embodiment of the present invention, technical scheme and advantage, below in conjunction with embodiment, the technical scheme of the embodiment of the present invention is described in further details, at this, schematic description and description of the present invention is for explaining the present invention, but not as a limitation of the invention.Based on the embodiment in the present invention, those of ordinary skill in the art, not making the every other embodiment obtained under creative work prerequisite, belong to the scope of protection of the invention.
The lithium-ion battery electrolytes that the embodiment of the present invention provides, comprising: solute, solvent, stabilization additives, described stabilization additives silazane derivatives, and described silazane derivatives structure is:
In above formula, R
1, R
2, R
3, R
4, R
5, R
6for one or more in hydrogen, alkyl, phenyl, xenyl, phenylate base, haloalkyl, halogenophenyl, halogenated biphenyl base, wherein, described alkyl is C
1-C
20straight or branched alkyl, described halogen comprises F, Cl, Br, I.
Well-known, in lithium ion battery, in electrolyte, lithium salts is met water generation hydrolysis and is generated hydrogen ion, and as previously mentioned, hydrogen ion has tremendous influence to the stability of electrolyte self and battery performance.Add aforementioned stable additive silazane derivatives in the electrolytic solution, can react with hydrogen ion in electrolyte, generate stable compound, thus effectively control electrolyte acidity, improve cycle life and the high-temperature storage performance of lithium ion battery, reaction principle is as shown in the formula (1):
Formula (1)
The salt compounds that reaction generates at high temperature has very strong stability, is difficult to decompose generate hydrogen ion again, therefore can well control the acidity of electrolyte, and then improves cycle life and the high-temperature storage performance of lithium ion battery.In addition, above-mentioned silazane derivatives additive deacidification speed is fast, and silazane derivatives described in 1mol can remove 2mol hydrogen ion, be in prior art hexamethyl phenodiazine silane (chemical formula is (CH
3)
3siNHSi (CH
3)
3) deacidification 2 times of speed, therefore better can control the acidity of electrolyte.
Preferably, the content of described silazane derivatives is the 0.1%-50% of electrolyte total weight.Obviously, those skilled in the art according to general knowledge known in this field and common technology means, can adjust the content of described silazane derivatives, and to determine the applicable content of silazane derivatives, the embodiment of the present invention is not construed as limiting this.
In the lithium-ion battery electrolytes that the embodiment of the present invention provides, described lithium salts can be the various lithium salts that this area is commonly used, and is preferably LiPF
6, LiBF
4, LiClO
4, LiPF
3(CF
2cF
3)
3, LiCF
3sO
3with one or more in LiBOB.Certainly, those skilled in the art can according to general knowledge known in this field, and select one or more lithium salts that other are applicable to, the embodiment of the present invention is not construed as limiting this.
In the lithium-ion battery electrolytes that the embodiment of the present invention provides, described non-aqueous organic solvent can be the various nonaqueous solventss that this area is commonly used, and is preferably one or more in carbonic ester and halo derivatives, ester, ether and ketone.Certainly, those skilled in the art can select other one or more non-aqueous organic solvents be applicable to, and the embodiment of the present invention is not construed as limiting this.
Be understandable that, those skilled in the art can according to the common practise of this area and common technology means, and select the content of the component such as lithium salts, non-aqueous organic solvent in the electrolyte of the embodiment of the present invention, the embodiment of the present invention is not construed as limiting this.
In the lithium-ion battery electrolytes that the embodiment of the present invention provides, described film for additive can be the various film for additive that this area is commonly used, be preferably vinylene carbonate, vinylethylene carbonate, 1,3-sulfonic acid propiolactone and 1, one or more in 4-sulfonic acid butyrolactone are certain, can also select other film for additive be applicable to by those skilled in the art according to general knowledge known in this field and common technology means, the embodiment of the present invention does not limit this.
Preferably, described film for additive content is the 0.1%-50% of electrolyte total weight.Certainly, can also be specified to the applicable content of film additive by those skilled in the art, the embodiment of the present invention is not construed as limiting this.
It should be noted that, the lithium-ion battery electrolytes that the embodiment of the present invention provides can adopt the method for the preparation of lithium-ion electrolyte well known in the art to be prepared.Such as, lithium salts, non-aqueous organic solvent, film for additive and stabilization additives silazane derivatives are pressed selected content range mixing and stirring.
The embodiment of the present invention additionally provides a kind of lithium ion battery, comprises electrolyte, and described electrolyte is above-mentioned electrolyte for lithium ion battery.
Because the present invention only relates to the improvement to prior art lithium-ion battery electrolytes, therefore other the Nomenclature Composition and Structure of Complexes of lithium ion battery are not particularly limited.
The lithium ion battery that the embodiment of the present invention provides can adopt the method for the preparation of lithium ion battery well known in the art to be prepared.
The lithium-ion battery electrolytes that the embodiment of the present invention provides and the lithium ion battery containing this electrolyte, by adding stabilization additives silazane derivatives, can be hydrolyzed with lithium salts in electrolyte the hydrogen ion produced to react and generate stable compound, thus the effective acidity controlling electrolyte, improve cycle life and the high-temperature storage performance of lithium ion battery.
In order to the lithium-ion battery electrolytes that the embodiment of the present invention provides better is described, be described in detail with specific embodiment below.
The preparation of lithium-ion battery electrolytes:
A certain amount of lithium salts is joined in non-aqueous organic solvent, obtains solution;
Add a certain proportion of film for additive and stabilization additives, can lithium-ion battery electrolytes be obtained.
Comparative example
The preparation of lithium-ion battery electrolytes:
By 1M lithium salts LiPF
6be dissolved in ethylene carbonate (EC)/methyl ethyl carbonate (EMC)/dimethyl carbonate (DMC)=1:1:1(wt%) mixed solvent in obtain solution, then add the ethylene carbonate (VC) of electrolyte total weight 2%, namely obtained contrast electrolyte, is designated as A sample.
Preparation containing the lithium ion battery of lithium-ion battery electrolytes A:
Adopt the method for the preparation of lithium ion battery well known in the art to prepare lithium ion battery, be designated as B.
Embodiment 1
The preparation of lithium-ion battery electrolytes:
By 1M lithium salts LiPF
6be dissolved in ethylene carbonate (EC)/methyl ethyl carbonate (EMC)/dimethyl carbonate (DMC)=1:1:1(wt%) mixed solvent in obtain solution, then the ethylene carbonate (VC) of electrolyte total weight 2% is added, and the shown silazane derivatives I of the formula (2) adding electrolyte total weight 0.5%, namely obtained desired electrolyte, is designated as A1 sample.
Formula (2)
Preparation containing the lithium ion battery of lithium-ion battery electrolytes A1:
Adopt the method identical with comparative example, prepare lithium ion battery, be designated as B1.
Embodiment 2
The preparation of lithium-ion battery electrolytes:
By 1M lithium salts LiPF
6be dissolved in ethylene carbonate (EC)/methyl ethyl carbonate (EMC)/dimethyl carbonate (DMC)=1:1:1(wt%) mixed solvent in obtain solution, then add the ethylene carbonate (VC) of electrolyte total weight 2% and add the shown silazane derivatives II of formula (3) of electrolyte total weight 0.5%, namely obtained desired electrolyte, is designated as A2 sample.
Formula (3)
Preparation containing the lithium ion battery of lithium-ion battery electrolytes A2:
Adopt the method identical with comparative example, prepare lithium ion battery, be designated as B2.
Embodiment 3
By 1M lithium salts LiPF
6be dissolved in ethylene carbonate (EC)/methyl ethyl carbonate (EMC)/dimethyl carbonate (DMC)=1:1:1(wt%) mixed solvent in obtain solution, then the ethylene carbonate (VC) of electrolyte total weight 2% is added, and add the silazane derivatives III shown by formula (4) of electrolyte total weight 0.5%, obtained desired electrolyte, is designated as A3 sample.
Formula (4)
Preparation containing the lithium ion battery of lithium-ion battery electrolytes A3:
Adopt the method identical with comparative example, prepare lithium ion battery, be designated as B3.
Embodiment one to three performance test
For the beneficial effect brought embodiment of the present invention technical scheme provides powerful support for, spy provides the following performance test for the embodiment of the present invention and comparative example:
(1) lithium-ion battery electrolytes deacidification performance test
Lithium-ion battery electrolytes A1, A2, A3 in lithium-ion battery electrolytes A in comparative example and embodiment 1 to 3 are carried out deacidification performance test.Method of testing is as follows:
1 distilled water is added, then with the moisture (H in coulomb cassette method test electrolyte respectively in electrolyte sample A, A1, A2, A3
2o) content, by the acidity in acid-base titration test electrolyte, to characterize the content of HF, now H
2content before the content of O and HF is recorded as and shelves, as shown in table 1, wherein, ppm is a few millionths.
Lithium-ion battery electrolytes sample A, A1, A2, A3 of adding water are shelved one week at normal temperatures, by the moisture in coulomb cassette method test electrolyte, by the acidity in acid-base titration test electrolyte, now H
2content after the content of O and HF is recorded as and shelves, as shown in table 1.
Table 1
Test result shows, relative to the comparative example electrolyte not adding silazane derivatives, the electrolyte of what the embodiment of the present invention provided add silazane derivatives shelve after free acid content obviously reduce, namely HF content obviously reduces; And along with the growth of alkyl chain in substituting group, free acid concentration fall is larger.
(2) cycle performance of lithium ion battery test
Lithium ion battery B1, B2, B3 in lithium ion battery B in comparative example and embodiment 1 to 3 are carried out cycle performance test.Capacity after record battery initial capacity and battery cycle charge-discharge 100 times, 200 times, 300 times, 400 times and 500 times, with mAh(MAH) be unit of measurement, concrete test result is in table 2.
Table 2
Test result shows, compared in comparative example containing the battery of electrolyte not adding silazane derivatives, the embodiment of the present invention provide containing the battery of electrolyte adding nitrogen silane derivative, its cycle performance significantly improves; And battery B1, B2, B3 cycle performance progressively improves along with the growth of alkyl chain in the substituting group of the silazane derivatives added in electrolyte, that is, in silazane derivatives substituting group, alkyl chain is longer, and cycle performance of battery is better.
(3) high-temperature storage performance of lithium ion battery test
Lithium ion battery B1, B2, B3 in the lithium ion battery B of comparative example and embodiment 1 to 3 are carried out high-temperature storage performance test, adopt and test with the following method:
Lithium ion battery B, B1, B2, B3 are placed 10 days under 55 DEG C of conditions, record high temperature storage data are as table 3.
Table 3
Test result shows, compared to the battery of electrolyte not adding silazane derivatives in comparative example, the embodiment of the present invention provide containing the battery of electrolyte adding silazane derivatives, its high-temperature storage performance significantly improves; And battery B1, B2, B3 high-temperature storage performance progressively improves along with the growth of alkyl chain in the substituting group of the silazane derivatives added in electrolyte, i.e. in the substituting group of silazane derivatives, alkyl chain is longer, and the high-temperature storage performance of battery is better.
Test known by above-mentioned with the performance comparison of comparative example, lithium-ion battery electrolytes in specific embodiment provided by the invention and the lithium ion battery containing this electrolyte effectively can control electrolyte acidity, improve cycle life and the high-temperature storage performance of lithium ion battery.And it is longer to add the substituent alkyl chain of silazane derivatives in electrolyte, and deacidify accordingly performance, cycle performance and high-temperature storage performance are better.
The above; be only the specific embodiment of the present invention, but protection scope of the present invention is not limited thereto, any those skilled in the art are in the technical scope that the present invention discloses; change can be expected easily or replace, all should be encompassed within protection scope of the present invention.Therefore, protection scope of the present invention should be as the criterion with the protection range of described claim.
Claims (8)
1. a lithium-ion battery electrolytes, comprising: solute, solvent, stabilization additives, is characterized in that, described stabilization additives is silazane derivatives, and described silazane derivatives structure is:
Wherein, R
1, R
2, R
3, R
4, R
5and R
6arbitrary is one in hydrogen atom, alkyl, phenyl, xenyl, phenylate base, haloalkyl, halogenophenyl and halogenated biphenyl base.
2. lithium-ion battery electrolytes according to claim 1, described alkyl is C
1-C
20straight or branched alkyl, in described haloalkyl, halogenophenyl and halogenated biphenyl base, halogen comprises F, Br, Cl, I.
3. lithium-ion battery electrolytes according to claim 1, is characterized in that, described silazane derivatives is the 0.1%-50% of electrolyte total weight.
4. lithium-ion battery electrolytes according to claim 1, is characterized in that, described solute is lithium salts, and described lithium salts is selected from LiPF
6, LiBF
4, LiClO
4, LiPF
3(CF
2cF
3)
3, LiCF
3sO
3with at least one in LiBOB.
5. lithium-ion battery electrolytes according to claim 1, is characterized in that, described solvent is non-aqueous organic solvent, and described non-aqueous organic solvent is at least one in carbonic ester halo derivatives, ester, ether and ketone.
6. lithium-ion battery electrolytes according to claim 1, it is characterized in that, described lithium-ion battery electrolytes also comprises film for additive, and described film for additive is vinylene carbonate, vinylethylene carbonate, 1, at least one in 3-sulfonic acid propiolactone and Isosorbide-5-Nitrae-sulfonic acid butyrolactone.
7. lithium-ion battery electrolytes according to claim 6, is characterized in that, described film for additive content is the 0.1%-50% of electrolyte total weight.
8. a lithium ion battery, comprises positive pole, negative pole and electrolyte, it is characterized in that, described electrolyte is the lithium-ion battery electrolytes described in any one of claim 1 to 7.
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| CN103401019B (en) * | 2013-08-08 | 2016-03-16 | 东莞市杉杉电池材料有限公司 | Silazane additive and apply its lithium-ion battery electrolytes preventing box hat from corroding prepared |
| CN107394268B (en) * | 2017-07-28 | 2019-08-09 | 广州天赐高新材料股份有限公司 | Lithium secondary cell electrolyte and its lithium secondary battery |
| CN113964384B (en) * | 2021-10-18 | 2024-01-05 | 南京航空航天大学 | Multifunctional organic silicon electrolyte suitable for lithium ion battery based on silicon negative electrode and preparation and application thereof |
| CN113851719B (en) * | 2021-10-18 | 2023-04-25 | 南京航空航天大学 | Multifunctional organic silicon electrolyte suitable for ternary positive electrode material-based lithium ion battery, and preparation and application thereof |
| KR20240094799A (en) * | 2022-12-16 | 2024-06-25 | 에스케이온 주식회사 | Electrolyte solution for lithium secondary battery and lithium secondary battery including the same |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1328355A (en) * | 2000-06-07 | 2001-12-26 | 默克专利股份有限公司 | Silane compound used as additives of electrochemical accumulator electrolyte |
| CN102437372A (en) * | 2011-11-22 | 2012-05-02 | 华为技术有限公司 | Lithium-ion battery electrolyte and lithium-ion battery containing same |
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| KR100875126B1 (en) * | 2006-11-13 | 2008-12-22 | 한국과학기술원 | Electrode for lithium secondary battery having improved cycle performance and lithium secondary battery using same |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1328355A (en) * | 2000-06-07 | 2001-12-26 | 默克专利股份有限公司 | Silane compound used as additives of electrochemical accumulator electrolyte |
| CN102437372A (en) * | 2011-11-22 | 2012-05-02 | 华为技术有限公司 | Lithium-ion battery electrolyte and lithium-ion battery containing same |
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