CN108987811A - A kind of full il electrolyte and the lithium battery containing the electrolyte - Google Patents
A kind of full il electrolyte and the lithium battery containing the electrolyte Download PDFInfo
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- CN108987811A CN108987811A CN201810793542.7A CN201810793542A CN108987811A CN 108987811 A CN108987811 A CN 108987811A CN 201810793542 A CN201810793542 A CN 201810793542A CN 108987811 A CN108987811 A CN 108987811A
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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
- H01M10/0569—Liquid materials characterised by the solvents
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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
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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
- H01M10/058—Construction or manufacture
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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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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
The present invention discloses a kind of full il electrolyte and the lithium battery containing the electrolyte, the full il electrolyte includes solvent, additive and lithium salts, the solvent is full ionic liquid, is using ionic liquid as main solvent, using the ionic liquid with surface-active as secondary solvent；The electrolyte series anion uses the bis trifluoromethyl sulfimide with imines conjugated system, which uses alkyl imidazolium cation.Temperature range, the good wellability to diaphragm and electrode material that there is electrolyte provided by the invention noninflammability, wide lithium-ion electrolyte to use；Two kinds of ionic liquids and electrolyte lithium salt anion having the same in electrolyte, not only ensure that the intermiscibility between good electrolyte, but also electrolyte system caused by the ion exchange that may occur in electrolyte system by different anion can be prevented to reset is rotten.
Description
Technical field
The present invention relates to technical field of lithium batteries, and in particular to a kind of full il electrolyte and contains the electrolyte
Lithium battery.
Background technique
Lithium battery is due to its voltage height, and specific energy is big, and have extended cycle life the battery performance excellent with memory-less effect etc., from
Nineteen ninety has been grown rapidly since coming out, it has also become 21 century mainstream battery, in Aeronautics and Astronautics, navigation, communication and electronics device
The fields such as tool are widely used.With mobile electronic device, the fast development of electric car, lithium battery capacity and
While energy density constantly increases, the safety problem of lithium battery has become the key for restricting its development and application.
The mixed electrolytic solution that lithium battery currently on the market mostly uses flammable organic solvent (carbonates) and lithium salts to form.
Overcharged when lithium battery is in, over-discharge, needle thorn, extrudings, internal short-circuit, when high temperature, the generation on fire of electrolyte easily moment is greatly
Calorimetric amount, leads to thermal runaway, causes safety accident.Therefore research safety, efficient lithium battery electrolytes, prevent hidden danger on fire,
It is the key point for solving lithium battery safety problem.Show as at room temperature liquid ionic liquid have it is non-volatile, heat resistance is high,
Liquid temperature range wide (up to 300 degree), low flammability and high chemical stability, ionic liquid is used as " green liquid in recent years
Body " attracts tremendous attention, and related ionic liquid causes the broad interest and industrial circle of academia as the research of lithium battery electrolytes
Greatly expect.
On the one hand certain specific function of ionic liquid is utilized, such as low temperature, high pressure, fire-retardant, as additive ionic liquid
Body is used to part substitution organic solvent and forms lithium battery composite electrolyte, it is contemplated that the viscosity of ionic liquid is larger, similar
Composite electrolyte can adjust the viscosity of electrolyte system with organic solvent, and 107180993 A of patent document CN reports ion
In organic carbonate system, simultaneously compound additive can be made bis- (trifluoromethyl sulfonyl) imines of liquid 1- ethyl-3-methylimidazole quinoline
For lithium battery low-temperature electrolyte；103618111 A of patent document CN provides a kind of high voltage bearing lithium secondary cell electrolyte, should
Electrolyte includes ionic liquid, hydrofluoroether, non-aqueous organic solvent (carbonic ester or carboxylate) and the addition of itrile group function dough
Agent.The compound ion liquid similarly designed in 101087035 A of patent document CN, 106876787 A of patent document CN
Electrolyte is all made of the viscosity of organic carbonate solvent adjustment il electrolyte system.Lithium battery composite electrolyte only exists
Solve the problems, such as that electrolyte is inflammable to limited extent, and there are the same phase compatibilities of ionic liquid and conventional carbonate solvent
Problem, and continuous consumption during cycle charge-discharge because of carbonate solvent lead to the system of ionic liquid composite electrolyte
It is reduced by the cycle life for destroying, causing battery.
On the one hand ionic liquid replacing whole organic solvent is being attempted, full il electrolyte exists negative to graphite material
Pole and diaphragm infiltration and compatible problem, need to solve problems faced when being such electrolyte design.Such as patent document
CN106920910 A replaces polyalkene diaphragm to improve full ionic liquid by using a kind of safety cellulose non-woven cloth diaphragm
The electrolyte problem bad to polyalkene diaphragm wellability, but the problem of do not refer to cathode wellability.
Therefore, il electrolyte complete for lithium battery, the problem is that having highly viscous ionic liquid to more
Infiltration in Porous materials such as electrode and diaphragm is poor.Electrode and diaphragm are soaked in relation to increasing lithium battery full il electrolyte at present
The method of profit ability is first is that dilute the Ion transfer speed for reducing viscosity and increasing ionic liquid by solvent, second is that passing by addition
Surfactant of uniting increases ionic liquid to the wetting capacity of electrode and diaphragm.It can be used for the nonaqueous solvents of lithium battery electrolytes
Very limited, the carbonate-based solvent that uses is commercialized, and there are many security risks；Conventional surfactant and ionic liquid
There are problems that compatibility, and needs to add the solubility that carbonates nonaqueous solvents increases conventional surfactant.
Summary of the invention
In view of the above-mentioned problems, the present invention provides a kind of full il electrolyte and the lithium battery containing the electrolyte, it should
Full il electrolyte includes the film for additive that two kinds of ionic liquids and content are no more than 5%.In used ionic liquid,
One is as main solvent, the second is ionic liquid surfactant is as secondary solvent.The electrolyte has noninflammability, wide lithium
Temperature range that ion electrolyte uses, the good wellability to diaphragm and electrode material；Two kinds of ionic liquids in electrolyte
Body and electrolyte lithium salt anion having the same, not only ensure that the intermiscibility between good electrolyte, but also can prevent electrolyte
Electrolyte system caused by the ion exchange that may occur in system by different anion is reset is rotten.
The invention adopts a technical scheme as:
A kind of full il electrolyte, including solvent, additive and lithium salts, the solvent be full ionic liquid, be with
Ionic liquid is main solvent, using the ionic liquid with surface-active as secondary solvent；The electrolyte series anion is using tool
There is the bis trifluoromethyl sulfimide [N (CF3SO2) 2]-of imines conjugated system, which uses imidazoles
Cation.
A kind of full il electrolyte, the main solvent, secondary solvent and additive are by weight percentage are as follows:
Main solvent 60-95%
Secondary solvent 1-35%
Additive 0.1-5%
Lithium salts 0.9-3.2mol is added in the mixture of every liter of main solvent, secondary solvent and additive.
A kind of full il electrolyte, the main solvent, secondary solvent and additive are by weight percentage are as follows:
Main solvent 80-95%
Secondary solvent 3-15%
Additive 0.1-5%.
A kind of full il electrolyte, the main solvent are the double trifluoros of ionic liquid 1- propyl -3- methylimidazole
Sulfonyloxy methyl inferior amine salt, structural formula is such as shown in (I)；
The secondary solvent is ionic liquid 1- octyl -3- methylimidazole bis trifluoromethyl sulfimide salt, and structural formula is such as
(II) shown in；
The lithium salts is bis trifluoromethyl sulfimide lithium, and as a result formula such as (III) is shown；
A kind of full il electrolyte, the additive is can be in the substance of positive and negative electrode formation SEI film, specifically
For one of vinylene carbonate (VC), fluorinated ethylene carbonate (FEC), three (trimethyl silane) phosphates (TMSP) or one
Kind or more mixing.
A kind of lithium battery containing full il electrolyte, including battery core and electrolyte, the battery core include anode, every
Film and cathode；The electrolyte is the described in any item full il electrolytes of claim 1-5.
The negative electrode active material of the lithium battery, the cathode is selected from graphite material.
The lithium battery, the diaphragm are selected from porous polyolefin compound, cellulose or glass fibre.
The lithium battery, the positive active material are selected from transition metal lithium intercalation compound.
The invention has the following advantages:
The design synthesis of the full il electrolyte system of the present invention considers the electrochemistry and chemical heat of lithium battery electrolytes
Solubility in lithium battery electrolytes system of mechanical stability, viscosity, lithium salts, lithium ion are moved lithium battery electrolytes system
Move number, the wetting capacity to cathode and diaphragm, the electrochemical behavior in cathode, the matching state of each component, work temperature in system
The factors such as range and commercial cost are spent, to pursue total optimization as principle.
The full il electrolyte system anion of the present invention uses the bis trifluoromethyl sulphonyl with imines conjugated system
Imines [N (CF3SO2)2]-, it is based on following reason: first is that bis trifluoromethyl sulfimide [N (CF3SO2)2]-Electrochemical window compared with
Width, viscosity are lower, more stable to water and air；Second is that Li [N (the CF as electrolyte lithium salt3SO2)2] charging when in anode
The uniform passivating film of Surface Creation has good anode performance, dissolves in selected il electrolyte system
Degree is high and has been commercialized；Third is that in the ionic liquid for having numerous researchs, [N (CF3SO2)2]–Volume it is relatively large,
And the volume increase of anion can reduce the fusing point of ionic liquid, the influence of anion is arranged such as by ionic liquid fusing point height
Under: Cl-> [PF6]-> [BF4]-> Br-> [N (CF3SO2)2]-；Finally, [N (the CF of large volume3SO2)2]-have is preferably electric
Lotus dispersibility effectively reduces interionic interaction force, shows lower viscosity, and it is relatively low viscous to facilitate matching
The ionic liquid of degree.
The present invention full il electrolyte system cation uses alkyl imidazolium cation, as electrolyte main solvent from
Sub- liquid selects 1- propyl -3- methyl imidazolium cation, in cation organic group number and length can significantly change ion
The properties such as viscosity, the fusing point of liquid are melted if the viscosity of 1- ethyl-3-methylimidazole trifluoromethanesulp-onyl -onyl imide is 34mPaS
Point is -15 DEG C, and when cation is 1,2 one one 3 one propyl imidazole of dimethyl, viscosity and fusing point rise to respectively
60mPaoS and 15 DEG C, to make electrolyte have broader operating ambient temperature, the main solvent of the full il electrolyte of the present invention
The cation of ionic liquid uses 1- propyl -3- methylimidazole, and bis trifluoromethyl sulphonyl is sub- in the cation and electrolyte system
- 87 DEG C of fusing point of the ionic liquid of amine anion composition, are provided simultaneously with lower viscosity (43.7cp) by 452 DEG C of decomposition temperature.Miaow
The acid proton on 2 in azole cation has reproducibility, can decompose on C cathode, but known SEI cathode film formation
Technology can make up the defect, such as add a small amount of vinylene carbonate in inventing full il electrolyte system, or
(and) fluorinated ethylene carbonate, or (and) three (trimethyl silane) phosphates etc., these film for additive prior to it is selected from
Sub- liquid forms passivation protection film in cathode.
To increase electrolyte to the wetting capacity of cathode and diaphragm, the full il electrolyte system of the present invention, which uses, to be had
The ionic liquid of surface-active is as adjuvant.There is ionic liquid the research of surface-active to start from 2001, and ionic liquid surface is living
Property agent surfactant and ionic liquid are combined to the property both having concurrently, research finds ionic liquid surfactant drop
The ability of low interfacial tension is better than the conventional surfactant of equal length carbochain.Patent document CN105552430A is in non-aqueous carbon
Acid esters is made to improve electrolyte to diaphragm and electricity using the ionic liquid with amphiphilic effect as additive in the electrolyte of solvent
The wetting capacity of pole material, the 1- octyl -3- methyl imidazolium cation and full ion that the full il electrolyte of the present invention uses
The ionic liquid that bis trifluoromethyl sulfimide anion forms in liquid electrolytic liquid system has excellent surface-active ability,
Electrolyte can be reduced in the interfacial tension of cathode and diaphragm, dissolution of the conventional surfactant in ionic liquid usually requires
It introduces organic solvent hydrotropy or avoids generating split-phase.
Two kinds of ionic liquids and electrolyte lithium salt anion having the same in the full il electrolyte of the present invention, this
The matching relationship of sample both ensure that the intermiscibility between good ionic liquid and ionic liquid, between ionic liquid and lithium salts,
Electrolyte system caused by the ion exchange that may occur in electrolyte system by different anion can be prevented to reset again is rotten.
Specific embodiment
In order to which the technical problems, technical solutions and beneficial effects solved by the present invention is more clearly understood, below in conjunction with
Embodiment, the present invention will be described in further detail.It should be appreciated that specific embodiment described herein is only used to explain
The present invention is not intended to limit the present invention.
(1) a kind of full il electrolyte
Including main solvent ionic liquid 1- propyl -3- methylimidazole bis trifluoromethyl sulfimide salt, secondary solvent ion
Liquid surfactant 1- octyl -3- methylimidazole bis trifluoromethyl sulfimide salt, additive and lithium salts bis trifluoromethyl sulphur
Imide li.
The ion liquid solvent 1- propyl -3- methylimidazole bis trifluoromethyl sulfimide salt has following molecular structure
Formula:
The ionic liquid surfactant 1- octyl -3- methylimidazole bis trifluoromethyl sulfimide salt has following point
Subformula:
The lithium salts bis trifluoromethyl sulfimide lithium has following molecular structural formula:
In above-mentioned full il electrolyte, main solvent, secondary solvent and additive are by weight percentage are as follows:
Main solvent 60-95%
Secondary solvent 1-35%
Additive 0.1-5%
Lithium salts 0.9-3.2mol is added in the mixture of every liter of main solvent, secondary solvent and additive, further preferably
2.5mol/L。
Preferably, main solvent, secondary solvent and additive be by weight percentage in the full il electrolyte are as follows:
Main solvent 80-95%
Secondary solvent 3-15%
Additive 0.1-5%.
Ionic liquid, ionic liquid surfactant, the lithium salts anion having the same of the full il electrolyte,
This combination can make between ionic liquid and ionic liquid, have good intersolubility between ionic liquid and lithium salts, guarantee electricity
The uniform of liquid system is solved, while being prevented during cycle charge-discharge inside electrolyte system due to electrolyte series anion not
Electrolyte caused by ion exchange same and occurring is reset is rotten.The ionic liquid surfactant enhances the full ionic liquid
For body electrolyte to the wetting ability of diaphragm and negative electrode material, raw material used by full il electrolyte provided by the invention is equal
It has been commercialized.
The additive is coalescing agent, which can play and prevent in electrolyte preferentially in cathode film formation
Decomposition of the ionic liquid in negative terminal surface.Preferably, the additive includes vinylene carbonate (VC), fluoro ethylene carbonate
One of ester (FEC), three (trimethyl silane) phosphates (TMSP) or more than one mixing；The additive is gone back cathode
Former current potential is below ionic liquid coalescing agent during the reduction potential of cathode, cycle charge-discharge and takes the lead in negative
Pole forms SEI film to prevent the ionic liquid in the decomposition of cathode, and can reduce full battery impedance.
(2) a kind of lithium battery containing above-mentioned full il electrolyte
Including battery core and electrolyte, the battery core includes anode, diaphragm and cathode；The electrolyte be above-mentioned (one) entirely from
Sub- liquid electrolyte.Preferably the negative electrode active material of the cathode of lithium battery is selected from graphite material.Diaphragm is selected from porous polyolefin
Compound, cellulose or glass fibre.Positive active material is selected from transition metal lithium intercalation compound.
(3) performance test
Following all comparative examples and embodiment perform the following performance tests
Performance test:
1) combustion testing: by the full il electrolyte of 1mL be added molten product be 2mL iron-clad in, using open fire ignite into
The flammable test of row, test result are shown in Table 2.
2) 25 DEG C of loop tests: being positive electrode using NMC532, and graphite is 18650 batteries of negative electrode material, test electricity
Pond charges to 4.2V under the conditions of 25 DEG C with 0.5C, and then 1C is discharged to 3.0V and carries out cyclic test, and the first charge discharge efficiency of test is held
Amount decays to cycle-index when initial capacity 80%, and test result is shown in Table 2.
3) -30 DEG C of 0.2C discharge performance tests: the battery after chemical conversion is charged to constant current constant voltage under 0.5C electric current room temperature
4.2V, is shelved 180 minutes at -30 DEG C, is discharged to 2.75V with -30 DEG C of 0.2C, discharge rate is shown in Table 3.
Embodiment 1-9
The embodiment is for illustrating full il electrolyte provided by the invention and its lithium battery, full ionic liquid electrolysis
The basic composition of liquid is shown in Table 1.
Comparative example 1
For the electrolyte 2688H provided using supplier A as comparative example 1, the basic composition of electrolyte is shown in Table 1.
Comparative example 2
For the electrolyte 2365A provided using supplier B as comparative example 2, the basic composition of electrolyte is shown in Table 1.
1 comparative example of table and embodiment electrolyte composition
2 25 DEG C of loop tests of table
| First charge discharge efficiency | Cycle-index when capacity attenuation is to 80% | It is whether flammable | |
| Comparative example 1 | 86.5% | 533 | It is flammable |
| Comparative example 2 | 86.1% | 581 | It is flammable |
| Embodiment 1 | 93.2% | 750 | It is non-combustible |
| Embodiment 2 | 93.0% | 735 | It is non-combustible |
| Embodiment 3 | 93.5% | 761 | It is non-combustible |
| Embodiment 4 | 94.1% | 788 | It is non-combustible |
| Embodiment 5 | 94.5% | 801 | It is non-combustible |
| Embodiment 6 | 90.6% | 680 | It is non-combustible |
| Embodiment 7 | 91.1% | 698 | It is non-combustible |
| Embodiment 8 | 92.9% | 724 | It is non-combustible |
| Embodiment 9 | 97.8% | 701 | It is non-combustible |
3-30 DEG C of discharge rate test of table
Claims (9)
1. a kind of full il electrolyte, including solvent, additive and lithium salts, which is characterized in that the solvent is full ion
Liquid is using ionic liquid as main solvent, using the ionic liquid with surface-active as secondary solvent；The electrolyte system yin from
Using the bis trifluoromethyl sulfimide [N (CF3SO2) 2]-with imines conjugated system, which adopts son
Use alkyl imidazolium cation.
2. a kind of full il electrolyte as described in claim 1, which is characterized in that the main solvent, secondary solvent and add
Add agent by weight percentage are as follows:
Main solvent 60-95%
Secondary solvent 1-35%
Additive 0.1-5%
Lithium salts 0.9-3.2mol is added in the mixture of every liter of main solvent, secondary solvent and additive.
3. a kind of full il electrolyte as claimed in claim 2, which is characterized in that the main solvent, secondary solvent and add
Add agent by weight percentage are as follows:
Main solvent 80-95%
Secondary solvent 3-15%
Additive 0.1-5%.
4. a kind of full il electrolyte as described in claim any one of 1-3, which is characterized in that the main solvent is ion
Liquid 1- propyl -3- methylimidazole bis trifluoromethyl sulfimide salt, structural formula is such as shown in (I)；
The secondary solvent is ionic liquid 1- octyl -3- methylimidazole bis trifluoromethyl sulfimide salt, structural formula such as (II)
It is shown；
The lithium salts is bis trifluoromethyl sulfimide lithium, and as a result formula such as (III) is shown；
5. a kind of full il electrolyte as described in claim any one of 1-3, which is characterized in that the additive is can be
Positive and negative electrode forms the substance of SEI film, specially vinylene carbonate (VC), fluorinated ethylene carbonate (FEC), three (trimethyl silicanes
Alkane) one of phosphate (TMSP) or more than one mixing.
6. a kind of lithium battery containing full il electrolyte, which is characterized in that including battery core and electrolyte, the battery core packet
Include anode, diaphragm and cathode；The electrolyte is the described in any item full il electrolytes of claim 1-5.
7. lithium battery as claimed in claim 6, which is characterized in that the negative electrode active material of the cathode is selected from graphite material.
8. lithium battery as claimed in claim 6, which is characterized in that the diaphragm be selected from porous polyolefin compound, cellulose,
Or glass fibre.
9. lithium battery as claimed in claim 6, which is characterized in that the positive active material is selected from the embedding lithiumation of transition metal and closes
Object.
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| CN112216871A (en) * | 2019-07-10 | 2021-01-12 | 比亚迪股份有限公司 | Lithium ion battery electrolyte, preparation method thereof, lithium ion battery and battery module |
| WO2022141215A1 (en) * | 2020-12-30 | 2022-07-07 | 东莞新能源科技有限公司 | Electrolyte, electrochemical device comprising same, and electronic device |
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