CN105990605B - A kind of nonaqueous electrolytic solution and the lithium ion battery containing the nonaqueous electrolytic solution - Google Patents
A kind of nonaqueous electrolytic solution and the lithium ion battery containing the nonaqueous electrolytic solution Download PDFInfo
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- CN105990605B CN105990605B CN201510045419.3A CN201510045419A CN105990605B CN 105990605 B CN105990605 B CN 105990605B CN 201510045419 A CN201510045419 A CN 201510045419A CN 105990605 B CN105990605 B CN 105990605B
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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
Abstract
The present invention provides a kind of nonaqueous electrolytic solution, including lithium salts, nonaqueous solvents and additive, contain trimethylsilane based isocyanate and ortho esters in the additive.The present invention also provides a kind of lithium ion batteries using the nonaqueous electrolytic solution.In nonaqueous electrolytic solution provided by the invention, by using trimethylsilane based isocyanate and carbonic acid ortho esters as the specific additive of the present invention, the high-temperature behavior of battery can be effectively promoted.The nonaqueous electrolytic solution that special additive obtains in the equivalent addition present invention, the middle nonaqueous electrolytic solution using other common additives, the high-temperature behavior of prepared lithium ion battery are greatly improved compared to the prior art.
Description
Technical field
The invention belongs to field of lithium ion battery more particularly to a kind of nonaqueous electrolytic solution and contain the lithium of the nonaqueous electrolytic solution
Ion battery.
Background technique
Lithium ion secondary battery is a kind of novel electrochmical power source, because it is big with energy density, operating voltage is high, the service life
The characteristics of long, without environmental hazard, it is widely used in the portable electronic products such as mobile phone.Safety problem is to restrict lithium ion
The major obstacle that battery develops to enlargement, energetic direction.Especially in recent years lithium ion secondary battery in power vehicle etc.
The application of the vehicles, to its safety etc. it is comprehensive require it is higher and higher.
Lithium ion secondary battery common at present is under the high temperature conditions in use, electrode can react with nonaqueous electrolytic solution
There is phenomena such as producing gas, battery performance is caused sharply to deteriorate.Have in currently available technology a small amount of resistance to by being added into electrolyte
Fluorobenzene, cyclohexyl benzene, the cyclohexyl fluorobenzene of oxidisability, for inhibiting reacting for the negative electrode active materials such as silicon and nonaqueous electrolytic solution.
Also have using the nonaqueous electrolytic solution containing trifluoromethylbenzene and diisocyanate compound, the diisocyanate compound and cathode
The hydroxyl reaction bonded of active material surface, the envelope generated by the reaction can inhibit the pair between cathode and electrolyte anti-
It answers, to inhibit the reduction of battery performance.
By adding a small amount of fluorobenzene, cyclohexyl benzene and trifluoromethylbenzene and diisocyanate compound etc. in above scheme
After additive, inhibitory activity substance and electrolyte it can react to a certain extent, but its effect is limited.If desired it is further promoted
Battery performance can only increase its dosage, but the viscosity of these additives is relatively high, and increasing its content will affect battery performance,
Battery capacity can also be reduced.
Summary of the invention
The present invention solves in lithium ion secondary battery in the prior art additive used by nonaqueous electrolytic solution to battery
The limited technical problem of performance boost.
The present invention provides a kind of nonaqueous electrolytic solution, including lithium salts, nonaqueous solvents and additive, contain in the additive
Trimethylsilane based isocyanate and ortho esters.
The present invention also provides a kind of lithium ion battery, including shell and the battery core being contained in housing, nonaqueous electrolytic solution,
Battery core includes anode, cathode and the diaphragm between positive electrode and negative electrode, wherein the nonaqueous electrolytic solution is provided by the invention
Nonaqueous electrolytic solution.
In nonaqueous electrolytic solution provided by the invention, by using trimethylsilane based isocyanate and carbonic acid ortho esters as this
Specific additive is invented, can effectively inhibitory activity substance and electrolyte be reacted, and the additive has high anode simultaneously
Stability, good cathode film formation performance and excellent water-scavenging capability, the product electrochemical window mouth width after reaction, can effectively mention
Rise the high-temperature behavior of battery.The obtained nonaqueous electrolytic solution of special additive in the equivalent addition present invention, compared to the prior art in
Using the nonaqueous electrolytic solution of other common additives, the high-temperature behavior of prepared lithium ion battery is greatly improved.
Specific embodiment
In order to which the technical problems, technical solutions and beneficial effects solved by the present invention is more clearly understood, below to this
Invention is further elaborated.
Specifically, the present invention provides a kind of nonaqueous electrolytic solution, including lithium salts, nonaqueous solvents and additive, the additions
Contain trimethylsilane based isocyanate (TMSIT) and ortho esters in agent.
In nonaqueous electrolytic solution provided by the invention, by using trimethylsilane based isocyanate and ortho esters as the present invention
Specific additive can effectively inhibitory activity substance and electrolyte react, and the additive simultaneously have it is high just extremely stable
Property, good cathode film formation performance and excellent water-scavenging capability, the product electrochemical window mouth width after reaction can effectively promote electricity
The high-temperature behavior in pond.
Nonaqueous electrolytic solution provided by the invention, due to use trimethylsilane based isocyanate and ortho esters, even if so that its
Using the solvent of electrochemical window stenostomia, low viscosity, the electrochemical stability of nonaqueous electrolytic solution also can be improved,
It is obviously improved the high temperature cyclic performance and storage performance of lithium ion battery.
As previously mentioned, used special additive itself just have easily film forming, good water-scavenging capability, therefore even if its
Additional amount is larger will not to influence battery capacity.Therefore, in the present invention, trimethylsilane based isocyanate and carbonic acid ortho esters contain
Amount can fluctuate in the larger context.Under preferable case, in the nonaqueous electrolytic solution in addition to lithium salts other components total matter
On the basis of amount, wherein the content of trimethylsilane based isocyanate is 0.1 ~ 15wt%, more preferably 1 ~ 5wt%.And with described non-aqueous
In electrolyte in addition to lithium salts on the basis of the gross mass of other components, wherein the content of ortho esters is in 5wt% or more, preferably
For 5 ~ 40wt%, more preferably 10 ~ 25wt%.
In the present invention, used trimethylsilane based isocyanate has structure shown in following formula 1, and ortho esters has formula 2
Shown structure.
Formula 1
Formula 2.
Specifically, in formula 2, R1、R2、R3、R4It is each independently selected from H, CH3、C2H5、C3H7Or other short-chain alkyls, but not
It is confined to this.Accordingly, in the present invention, the ortho esters is preferably trimethyl orthoformate, triethyl orthoformate (TEOA), former second
Sour trimethyl, triethly orthoacetate, former propionic acid trimethyl, triethyl orthopropionate, trimethyl orthobutyrate, original acid triethyl, original
One of trimethyl orthovalerate, orthovaleric acid triethyl are a variety of, but not limited to this.
Under preferable case, in nonaqueous electrolytic solution provided by the invention, the concentration of lithium salts is 0.5-1.5mol/L.The lithium salts
For the common various lithium salts of those skilled in the art, such as lithium perchlorate (LiClO can be selected from4), lithium hexafluoro phosphate (LiPF6),
LiBF4 (LiBF4), hexafluoroarsenate lithium (LiAsF6), Li (CF3CO2)2N、LiCF3SO3、Li(CF3SO2)3、Li
(CF3SO2)2N、Li (C2F5SO2)2N、LiB(C2O4)2In any one or more.Under preferable case, the present invention uses LiPF6
As main lithium salts, concentration 0.5-1.5mol/L, more preferably 0.8-1.3 mol/L.
In the present invention, the nonaqueous solvents uses those skilled in the art's commonly various nonaqueous solvents, such as can
To be selected from methyl ethyl carbonate (EMC), dimethyl carbonate (DMC), diethyl carbonate (DEC), ethylene carbonate (EC), propylene carbonate
Ester (PC), butylene (BC), ethylene sulfite (ES), propylene sulfite (PS), sulfurous acid diethyl ester (DES), γ-
At least one of butyrolactone (BL), dimethyl sulfoxide (DMSO), ethyl acetate, methyl acetate, but not limited to this.
As a kind of preferred embodiment of the invention, also contains vinylene carbonate (VC) in the additive, make
With being to inhibit solvent in the reduction of cathode in cathode film formation.Under preferable case, in the nonaqueous electrolytic solution in addition to lithium salts its
On the basis of the gross mass of his component, wherein the content of vinylene carbonate is 2 ~ 10wt%.
The preparation method of nonaqueous electrolytic solution provided by the invention is the common method of those skilled in the art, i.e., by each group
(including lithium salts, nonaqueous solvents and additive) is divided to be uniformly mixed, the present invention is not particularly limited.
The present invention also provides a kind of lithium ion battery, including shell and the battery core being contained in housing, nonaqueous electrolytic solution,
Battery core includes anode, cathode and the diaphragm between positive electrode and negative electrode, wherein the nonaqueous electrolytic solution is provided by the invention
Nonaqueous electrolytic solution.The obtained nonaqueous electrolytic solution of special additive in the equivalent addition present invention, compared to the prior art in use it
The high-temperature behavior of the nonaqueous electrolytic solution of its common additives, prepared lithium ion battery is greatly improved.
Due to the preparation process of negative electrode tab, positive plate, diaphragm technology well known in the art, and the assembling of battery is also
Technology known in the field, details are not described herein again.Under preferable case, the positive active material contained in the anode is
LiCoO2, the negative electrode active material contained in the cathode is graphite material, but not limited to this.
To nonaqueous electrolytic solution of the invention and contain the lithium ion battery of the nonaqueous electrolytic solution below in conjunction with specific embodiment
It is described further.It should be appreciated that the specific embodiments described herein are merely illustrative of the present invention, it is not used to limit this
Invention.Raw material employed in embodiment and comparative example is commercially available.
Embodiment 1
(1) preparation of nonaqueous electrolytic solution
By ethylene carbonate (EC), diethyl carbonate (DEC), trimethylsilane based isocyanate (TMSIT), three second of ortho-acetic acid
Ester (TEOA) is mixed with the mass ratio of 30:50:5:15, and in the in the mixed solvent, solute LiPF is added6, lithium salt content, which is made, is
The nonaqueous electrolytic solution of 1.0mol/L, is denoted as S1.
(2) preparation of lithium ion battery
By LiCoO2, conductive material such as acetylene black, adhesive PVDF is by 85:10:5 and appropriate NMP(N- crassitude
Ketone) slurry is stirred into, it is applied on the aluminium foil of 20 μ m-thicks, obtains positive electrode sheet through drying, compacting, obtained after putting tab of burn-oning
To positive plate.
By weight it is 100:3:2 by graphite (model P15B) and SBR, CMC, is mixed to get using deionized water as solvent
Negative electrode material paste.It is applied on the copper foil of 12 μ m-thicks dry, compacting and obtains negative electrode sheet, obtained just after putting tab of burn-oning
Pole piece.
It is buckled being assembled into positive plate obtained above, negative electrode tab and Celgard2300 type micro-pore septum argon gas glove box
Formula battery, the nonaqueous electrolytic solution S1 of injection step (1), is made the lithium ion battery of the present embodiment, is denoted as S10 after sealing.
Embodiment 2-7
Nonaqueous electrolytic solution S2-S7 and lithium ion battery S20-S70 are prepared using step same as Example 1, difference
Be in: in step (1), trimethylsilane based isocyanate (TMSIT) in nonaqueous electrolytic solution, triethly orthoacetate (TEOA) match
Than as shown in table 1.
Embodiment 8
Nonaqueous electrolytic solution S8 and lithium ion battery S80 are prepared using step same as Example 1, the difference is that:
In step (1), the ethylene carbonate (EC) in embodiment 1 is replaced using butylene (BC), using methyl ethyl carbonate (EMC)
Replace the diethyl carbonate (DEC) in embodiment 1, the triethly orthoacetate in embodiment 1 is replaced using orthovaleric acid triethyl
(TEOA), using Li (CF3SO2)3Replace the LiPF in embodiment 16, and lithium salt is 0.6mol/L in nonaqueous electrolytic solution S8.
Embodiment 9
Nonaqueous electrolytic solution S9 and lithium ion battery S90 are prepared using step same as Example 1, the difference is that:
In step (1), by ethylene carbonate (EC), diethyl carbonate (DEC), trimethylsilane based isocyanate (TMSIT), ortho-acetic acid three
Ethyl ester (TEOA) and vinylene carbonate (VC) are mixed with the mass ratio of 29:49:5:14.5:2.5, in the in the mixed solvent, are added
Enter solute LiPF6, the nonaqueous electrolytic solution that lithium salt content is 1.0mol/L is made, is denoted as S9.
Embodiment 10
Nonaqueous electrolytic solution S10 and lithium ion battery S100 are prepared using step same as Example 1, difference exists
In: in step (1), by ethylene carbonate (EC), diethyl carbonate (DEC), trimethylsilane based isocyanate (TMSIT), former second
Triethylenetetraminehexaacetic acid ester (TEOA) and vinylene carbonate (VC) are mixed with the mass ratio of 26.4:44:4.4:13.2:12, molten in the mixing
In agent, solute LiPF is added6, the nonaqueous electrolytic solution that lithium salt content is 1.0mol/L is made, is denoted as S10.
Comparative example 1-3
Nonaqueous electrolytic solution DS1-DS3 and lithium ion battery DS10-DS30 are prepared using step same as Example 1, no
Be with place: in step (1), the consumption proportion of nonaqueous solvents and additive is as shown in table 1 in nonaqueous electrolytic solution.
Table 1
。
Comparative example 4
Nonaqueous electrolytic solution DS4 and lithium ion battery DS40 are prepared using step same as Example 1, difference exists
In: in step (1), it is added without trimethylsilane based isocyanate (TMSIT) and triethly orthoacetate (TEOA), and 20 weight are added
The fluorobenzene of part.
Comparative example 5
Nonaqueous electrolytic solution DS5 and lithium ion battery DS50 are prepared using step same as Example 1, difference exists
In: it is in step (1), ethylene carbonate (EC), diethyl carbonate (DEC), cyclohexyl benzene is mixed with the mass ratio of 31.6:65.4:3
It closes, in the in the mixed solvent, solute LiPF is added6, the nonaqueous electrolytic solution that lithium salt content is 1.0mol/L is made, is denoted as DS5.
Comparative example 6
Nonaqueous electrolytic solution DS6 and lithium ion battery DS60 are prepared using step same as Example 1, difference exists
In: in step (1), it is added without trimethylsilane based isocyanate (TMSIT) and triethly orthoacetate (TEOA), and 10 weight are added
The trifluoromethylbenzene of part and the hexamethylene diisocyanate of 10 parts by weight.
Performance test:
Lithium ion battery sample S10-S100 and DS10-DS60 are performed the following performance tests.
1, high temperature cyclic performance is tested
By it is above-mentioned carried out chemical conversion embodiment 1 ~ 10 and comparative example 1-6 lithium ion battery, respectively at 60 DEG C with
The constant current charging of 95mA charges to 4.2V, then under 4.2V constant voltage until current value is 20mA, later with 95mA
Constant current be discharged to 3V.In this, as one cycle, repeat 250 charge and discharge cycles.According to discharge capacity meter
Capacity retention ratio=(Q250/Q1) × 100 is calculated, test result is as shown in table 2.
2, high-temperature storage performance is tested
By it is above-mentioned carried out chemical conversion embodiment 1 ~ 10 and comparative example 1-6 lithium ion battery, respectively at 25 DEG C with
The constant current charging of 95mA to 4.2V, then under 4.2V constant voltage charging until current value be 20mA, in this state,
After the thickness for measuring each battery, saved 20 days at 60 DEG C, thickness change=(thickness before thickness-storage after storage)/
Thickness × 100% before storage, test result are as shown in table 2.
Table 2
。
S10-S100 is compared with the test result of DS10-DS60 as can be seen that using the specific addition of the present invention from table 2
Agent is added in nonaqueous electrolytic solution, the high temperature cyclic performance and high-temperature storage performance of the significant lithium ion battery of energy.
S10-S20 is compared with the test result of S30-S60 as can be seen that the specific additive of the present invention contains from table 2
When amount is in preferred scope of the invention, it is more significant that effect is promoted to the high-temperature behavior of battery.
From S70 in table 2 as can be seen that equivalent adds special additive in the present invention, originally compared with the test result of DS50
The high-temperature behavior for inventing the lithium ion battery provided is considerably better.
From S10 in table 2 compared with the test result of S90 as can be seen that the present invention in be preferably added to VC when, lithium ion battery
High-temperature behavior it is more excellent.
The foregoing is merely illustrative of the preferred embodiments of the present invention, is not intended to limit the invention, all in essence of the invention
Made any modifications, equivalent replacements, and improvements etc., should all be included in the protection scope of the present invention within mind and principle.
Claims (13)
1. a kind of nonaqueous electrolytic solution, including lithium salts, nonaqueous solvents and additive, which is characterized in that contain three in the additive
Silyl isocyanate and ortho esters.
2. nonaqueous electrolytic solution according to claim 1, which is characterized in that in the nonaqueous electrolytic solution in addition to lithium salts its
On the basis of the gross mass of his component, wherein the content of trimethylsilane based isocyanate is 0.1 ~ 15wt%.
3. nonaqueous electrolytic solution according to claim 1, which is characterized in that in the nonaqueous electrolytic solution in addition to lithium salts its
On the basis of the gross mass of his component, wherein the content of trimethylsilane based isocyanate is 1 ~ 5wt%.
4. nonaqueous electrolytic solution according to claim 1, which is characterized in that in the nonaqueous electrolytic solution in addition to lithium salts its
On the basis of the gross mass of his component, wherein the content of ortho esters is 5 ~ 40wt%.
5. nonaqueous electrolytic solution according to claim 4, which is characterized in that in the nonaqueous electrolytic solution in addition to lithium salts its
On the basis of the gross mass of his component, wherein the content of ortho esters is 10 ~ 25wt%.
6. according to claim 1,4,5 described in any item nonaqueous electrolytic solutions, which is characterized in that the ortho esters is selected from orthoformic acid
Trimethyl, triethyl orthoformate, trimethyl orthoacetate, triethly orthoacetate, former propionic acid trimethyl, triethyl orthopropionate, former fourth
One of sour trimethyl, original acid triethyl, original acid methyl ester, orthovaleric acid triethyl are a variety of.
7. nonaqueous electrolytic solution according to claim 1, which is characterized in that in the nonaqueous electrolytic solution, the concentration of lithium salts is
0.5-1.5mol/L。
8. nonaqueous electrolytic solution according to claim 1 or claim 7, which is characterized in that the lithium salts is selected from LiClO4、LiPF6、
LiBF4、LiAsF6、Li(CF3CO2)2N、LiCF3SO3、Li(CF3SO2)3、Li(CF3SO2)2N、Li (C2F5SO2)2N、LiB
(C2O4)2One of or it is a variety of.
9. nonaqueous electrolytic solution according to claim 1, which is characterized in that the nonaqueous solvents is selected from methyl ethyl carbonate, carbon
Dimethyl phthalate, diethyl carbonate, ethylene carbonate, propene carbonate, butylene, ethylene sulfite, sulfurous acid propylene
At least one of ester, sulfurous acid diethyl ester, gamma-butyrolacton, dimethyl sulfoxide, ethyl acetate and methyl acetate.
10. nonaqueous electrolytic solution according to claim 1, which is characterized in that also contain vinylene carbonate in the additive
Ester.
11. nonaqueous electrolytic solution according to claim 10, which is characterized in that in the nonaqueous electrolytic solution in addition to lithium salts
On the basis of the gross mass of other components, wherein the content of vinylene carbonate is 2 ~ 10wt%.
12. a kind of lithium ion battery, including shell and the battery core being contained in housing, nonaqueous electrolytic solution, battery core includes positive, negative
Pole and the diaphragm between positive electrode and negative electrode, which is characterized in that the nonaqueous electrolytic solution is any one of claim 1-11 institute
The nonaqueous electrolytic solution stated.
13. lithium ion battery according to claim 12, which is characterized in that the positive active material contained in the anode
For LiCoO2, the negative electrode active material contained in the cathode is graphite material.
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| CN111834669B (en) * | 2019-04-15 | 2022-03-15 | 比亚迪股份有限公司 | Lithium ion battery electrolyte and lithium ion battery |
| CN112018442B (en) * | 2019-05-29 | 2022-02-08 | 比亚迪股份有限公司 | Lithium ion battery electrolyte and lithium ion battery |
| CN111092256A (en) * | 2019-11-29 | 2020-05-01 | 天津力神电池股份有限公司 | High-temperature-resistant lithium ion battery |
| CN111477964B (en) * | 2020-04-14 | 2021-06-25 | 宁德新能源科技有限公司 | Electrolyte and electrochemical device |
| CN113346138A (en) * | 2021-05-28 | 2021-09-03 | 湖南大学 | Electrolyte and lithium battery |
| CN114039053B (en) * | 2021-11-08 | 2023-07-11 | 深圳市皓飞实业有限公司 | Lithium ion battery, preparation method thereof and auxiliary agent for lithium ion battery |
| CN117219855A (en) * | 2023-08-25 | 2023-12-12 | 山东立中新能源材料有限公司 | Sodium ion battery electrolyte and sodium ion battery |
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