CN108336412A - A kind of lithium ion battery electrolyte and preparation method thereof and lithium ion battery - Google Patents
A kind of lithium ion battery electrolyte and preparation method thereof and lithium ion battery Download PDFInfo
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- CN108336412A CN108336412A CN201810037834.8A CN201810037834A CN108336412A CN 108336412 A CN108336412 A CN 108336412A CN 201810037834 A CN201810037834 A CN 201810037834A CN 108336412 A CN108336412 A CN 108336412A
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- lithium ion
- 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
- H01M10/0569—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
- 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
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
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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 present invention discloses a kind of lithium ion battery electrolyte and preparation method thereof and lithium ion battery, wherein the lithium ion battery electrolyte includes following components：Ionic liquid, lithium salts, sulfone class organic solvent.Electrolyte of the present invention can during charge and discharge cycles positive electrode surface be formed stablize densification CEI films, can effective protection electrode material, prevent electrolyte from decomposing.Therefore, the electrolysis mass-energy significantly improves cyclical stability and safety of the lithium ion battery under high temperature high voltage.
Description
Technical field
The present invention relates to field of lithium ion battery more particularly to a kind of lithium ion battery electrolyte and preparation method thereof and lithiums
Ion battery.
Background technology
As population increases year by year, fossil energy reserves are increasingly in short supply, and people are badly in need of wanting a kind of new alternative energy source, with solution
Certainly energy crisis.Chargeable lithium ion is answered extensively with its high-energy density, outstanding high rate performance and long circulation life
In electric vehicle, hybrid vehicle, 3C Product and aerospace equipment.However, current lithium ion battery technology
The problem of there are still some challenges, such as the cyclical stability difference under high temperature high voltage and hot environment（55 DEG C with
On）Under the low problem of safety.
Electrolyte is the ion conductor that conduction is played between battery positive and negative electrode, and the performance of itself is largely
Affect the performance of battery.Currently, the solvent in the widely used electrolyte of lithium ion battery of commercialization is ethylene carbonate
(EC) the binary or ternary mixed solvent based on.Carbonate based organic solvent highly volatile, and when battery temperature is higher,
LiPF in electrolyte6Can react generation HF can corrosion solids dielectric film and electrode material even collector, cause
Battery failure and then the short-circuit after-explosion of initiation.Therefore, electrolyte is the key factor for influencing lithium ion battery security.
Currently, the technical solution for solving high temperature high-voltage lithium ion batteries safety issue is in conventional commercial electrolyte
High voltage additive is added and flame-retardant additives, mass percentage content are usually no more than 1%.However, high voltage additive and
Flame-retardant additives are generally difficult to synthesize, and the requirement to equipment is high, development cost higher.Moreover, above-mentioned technical proposal is in room temperature
And have preferable cyclical stability under middle low temperature, but in higher temperature such as 70 DEG C or more still cannot normally recycle, when
Due to decomposition of the carbonate-based solvent therein under high temperature high voltage environment, second is that LiPF6Lithium salts reacts at high temperature
Generate HF and corroding positive electrode causes cathode material structure to be destroyed, seriously affect the safety of cycle performance and battery.
Therefore, the existing technology needs to be improved and developed.
Invention content
In view of above-mentioned deficiencies of the prior art, the purpose of the present invention is to provide a kind of lithium ion battery electrolyte and its systems
Preparation Method and lithium ion battery, it is intended to solve the lithium battery prepared with existing lithium ion battery electrolyte high temperature high voltage item
Cyclical stability difference and the low problem of safety under part.
Technical scheme is as follows：
A kind of lithium ion battery electrolyte, wherein including following components:Ionic liquid, sulfone class organic solvent and lithium salts.
The lithium ion battery electrolyte, wherein the cation of the ionic liquid is piperidines cationoid, pyrrolidines
One kind in cationoid, alkyl imidazolium cation.
The lithium ion battery electrolyte, wherein the anion of the ionic liquid is TFSI-、FSI-、BF4 -、DFOB-
In one kind.
The lithium ion battery electrolyte, wherein the sulfone class organic solvent be sulfolane, glycol sulfite, 1,
One kind in 3- propane sultones, dimethyl sulfite, sulfurous acid diethyl ester.
The lithium ion battery electrolyte, wherein the lithium salts is difluorine oxalic acid boracic acid lithium.
The lithium ion battery electrolyte, wherein the mass ratio of the ionic liquid and the sulfone class organic solvent is
（0.4-0.8）：（0.2-0.6）.
The lithium ion battery electrolyte, wherein the lithium salts is in the ionic liquid and the sulfone class organic solvent
In a concentration of 0.3-0.5 mols/kg.
A kind of preparation method of lithium ion battery electrolyte as described above, wherein include the following steps：
Under atmosphere of inert gases, ionic liquid and sulfone class organic solvent are uniformly mixed, mixed solvent is obtained；
Lithium salts is added in the mixed solvent, is uniformly mixed, obtains the electrolyte.
A kind of lithium ion battery, wherein including lithium ion battery electrolyte as described above.
Advantageous effect：The present invention provides a kind of lithium ion battery electrolyte, and the electrolyte can be in charge and discharge cycles mistake
In journey positive electrode surface formed stablize densification CEI films, can effective protection electrode material, prevent electrolyte from decomposing.Therefore, originally
The invention lithium ion battery electrolyte can significantly improve cyclical stability of the lithium ion battery under high temperature high voltage environment
And safety.
Description of the drawings
Fig. 1 is the battery discharge specific volume spirogram that 1 charge and discharge cycles of the embodiment of the present invention are tested.
Fig. 2 is the XPS carbon spectrograms of the lithium-rich anode pole piece after the test of 1 charge and discharge cycles of the embodiment of the present invention.
Fig. 3 is the XPS oxygen spectrograms of the lithium-rich anode pole piece after the test of 1 charge and discharge cycles of the embodiment of the present invention.
Fig. 4 is the XPS fluorine spectrograms of the lithium-rich anode pole piece after the test of 1 charge and discharge cycles of the embodiment of the present invention.
Fig. 5 is the XPS boron spectrograms of the lithium-rich anode pole piece after the test of 1 charge and discharge cycles of the embodiment of the present invention.
Fig. 6 is the battery discharge specific volume spirogram that 2 charge and discharge cycles of the embodiment of the present invention are tested.
Specific implementation mode
A kind of lithium ion battery electrolyte of present invention offer and preparation method thereof and lithium ion battery, to make the mesh of the present invention
, technical solution and effect it is clearer, clear, the present invention is described in more detail below.It should be appreciated that described herein
Specific examples are only used to explain the present invention, is not intended to limit the present invention.
The present invention provides a kind of lithium ion battery electrolyte, wherein including following components:Ionic liquid, sulfone class are organic molten
Agent and lithium salts.
Ionic liquid of the present invention is made of organic cation and anion.The ionic liquid can be by right
Anions and canons carry out collocation design, and to adjust the performance of ionic liquid, therefore ionic liquid is otherwise known as " can design solvent ".
It can be in the salt of liquid condition at a temperature of room temperature or near room temperature that the ionic liquid, which is a kind of, it is from traditional high temperature
What fused salt developed, but have very different property with general ionic compound, it is maximum that difference lies in general ions
Compound only can just become liquid at high operating temperatures, and ionic liquid is liquid near room temperature.Ion of the present invention
Liquid has many advantages, such as that heat resistance is high, nonflammable, electrochemically stable, can significantly improve the safety of lithium ion battery.
Sulfone class organic solvent of the present invention is of low cost, has wide electrochemical window, high conductivity, higher boiling, non-ignitable
The characteristics of burning, low viscosity.The addition of sulfone class organic solvent can improve electrolyte electrochemical stability, and thermal stability may be used also
To improve the dissolubility to lithium salts and reduce the viscosity of electrolyte.
The electrolyte of lithium ion battery has the cycle efficieny of lithium battery, operating voltage, operating temperature and service life etc.
Important influence, lithium ion battery electrolyte provided by the invention can be formed during charge and discharge cycles in positive electrode surface
Stablize fine and close CEI films.CEI films be by electrolyte lithium salts, sulfone class organic solvent, ionic liquid is in charge and discharge cycles process
The dense film that middle interaction is formed in anode.Electrolyte of the present invention is formed by CEI films, being capable of effective protection electrode material
The structure of material, prevents electrolyte from decomposing, even if in high temperature（70 DEG C or more）Under the conditions of, it also can guarantee the normal operation of battery.Cause
This, electrolysis mass-energy of the present invention significantly improves cyclical stability and safety of the lithium ion battery under high temperature high voltage environment
Property.
Preferably, the cation of the ionic liquid be piperidines cationoid, pyrrolidines cation or imidazoles sun from
Son；The anion is inorganic anion or organic anion, it is preferred that the anion of the ionic liquid is TFSI-、FSI-、
BF4 -、DFOB-。
The ionic liquid that the present invention is obtained by the preferred cation with anion collocation design has following features：
(1) vapour pressure is extremely low；(2) heat resistance is high, and liquid temperature range is wide (maximum temperature is up to 300 DEG C)；(3) nonflammable；(4) chemical
Stability is good, is the good solvent of many substances；(5) electrochemical stability window is wide, and decomposition voltage is up to 6V.
Preferably, the sulfone class organic solvent is sulfolane, glycol sulfite, 1,3-propane sultone, sulfurous acid two
One kind in methyl esters, sulfurous acid diethyl ester.Above-mentioned organic solvent has high conductivity and high-temperature stability, can improve electrolysis
Stability under matter high voltage and high temperature.
Preferably, the lithium salts is difluorine oxalic acid boracic acid lithium.Difluorine oxalic acid boracic acid lithium is used as in lithium cell electrolyte and leads
Electric salt can form CEI films during charge and discharge cycles with the other components of electrolyte in positive electrode surface.
Preferably, the mass ratio of the ionic liquid and the sulfone class organic solvent is（0.4-0.8）：（0.2-0.6）.This
Inventing the mass ratio of the ionic liquid and the sulfone class organic solvent can make electrolyte system have good viscosity, ensure
Lithium ion moves freely.
Preferably, the lithium salts a concentration of 0.3-0.5 moles in the ionic liquid and the sulfone class organic solvent/
Kilogram.As solvent, the lithium salts is a concentration of in the solvent for the i.e. described ionic liquid and the sulfone class organic solvent
0.3-0.5 mols/kg.
The present invention provides a kind of preparation method of lithium ion battery electrolyte, includes the following steps：
Under atmosphere of inert gases, ionic liquid and sulfone class organic solvent are uniformly mixed, mixed solvent is obtained；
Lithium salts is added in the mixed solvent, is uniformly mixed, obtains cell electrolyte.
The preparation method of the lithium ion battery electrolyte, specifically, at normal temperatures and pressures, full of inert gas（Such as
Argon gas）Glove box in, by ionic liquid and sulfone class organic solvent according to mass ratio（0.4-0.8）：（0.2-0.6）Mixing is equal
It is even, obtain mixed solvent；Then, lithium salts is added in the mixed solvent, is uniformly mixed, obtains lithium ion battery electrolyte.
The oxygen content of the atmosphere of inert gases is less than 0.1ppm, and water content is less than 0.1ppm, prevents because in electrolyte
Component aoxidizes or is mixed into the problem of moisture causes electrolyte performance to reduce.
The present invention provides a kind of lithium ion battery, wherein including lithium ion described in lithium ion battery electrolyte as described above
Battery.Specifically, the lithium ion battery include lithium ion battery electrolyte as described above, anode, cathode, setting anode with
Diaphragm between cathode.Battery of the present invention under high voltage and hot environment have good charge-discharge performance and
Safety.
Technical scheme of the present invention is described in detail below by specific embodiment.
Embodiment 1
The preparation of lithium ion battery electrolyte：Under normal temperature and pressure, in the glove box full of argon gas（Oxygen, water content are less than
0.1ppm）In, by bis- (trifyl) inferior amine salts of ionic liquid 1- butyl -1- methyl piperidines and sulfolane according to mass ratio
6：4 are uniformly mixed, and obtain mixed solvent.On the basis of quality, it is added in the mixed solvent a concentration of in the mixed solvent
The difluorine oxalic acid boracic acid lithium of 0.5mol/kg is uniformly mixed, obtains lithium ion battery electrolyte 10g.
The preparation of-rich pole piece：Lithium-rich oxide, conductive agent acetylene black, binder are gathered into inclined tetrafluoroethene with 8：1：
1 mass ratio is added to N-Methyl pyrrolidone（NMP）In, it is uniformly mixed and obtains anode sizing agent, then slurry is uniformly coated in
On aluminium foil, it is sliced after dry under conditions of temperature is 70 DEG C, obtains-rich pole piece.
The preparation of battery：Using the-rich pole piece being prepared as the anode of battery, cathode of the lithium piece as battery will
Diaphragm of the Celgard2325 micro-pore septums as battery, using the electrolyte being prepared as the electrolyte of battery, by CR2032
Said modules, are assembled into CR2032 button cells by battery case of the battery case as battery in glove box.
Charge and discharge cycles test is carried out to prepared battery：By the battery standing being prepared for 24 hours after, use Shenzhen rich
It is easily 70 DEG C up to climatic chamber control environment temperature, following for battery is tested using the blue electricity CT2001A battery test systems in Wuhan
Ring performance, wherein test parameter is that charging/discharging voltage range is 2-4.6V, is recycled 50 times with 0.5C.Fig. 1 is the present embodiment charge and discharge
The battery discharge specific volume spirogram that electric loop test obtains.It can be seen from the figure that the battery prepared by the present embodiment is in environment temperature
Degree has excellent cyclical stability under conditions of being 70 DEG C.
The CEI membrane components formed on anode are analyzed using XPS：- rich pole piece after cycle is torn open from battery
Go out, the entrained electrolyte 3 times on surface is rinsed with DMC, after vacuum drying, pole piece is subjected to x-ray photoelectron spectroscopy test analysis.
Fig. 2, Fig. 3, Fig. 4, Fig. 5 are respectively the XPS carbon spectrum of the lithium-rich anode pole piece after the test of the present embodiment charge and discharge cycles
Figure, oxygen spectrogram, fluorine spectrogram, boron spectrogram.Occur the peak of C-O and C=O, XPS fluorine spectrograms on XPS carbon spectrogram and XPS oxygen spectrograms
It is middle to occur the peak of Li-F, the peak of B-O occur in XPS boron spectrograms, illustrate the lithium ion battery electrolysis prepared by the present embodiment
LiDFOB in matter decomposes under high voltages, and decompose obtain product positive electrode surface form one layer it is form compact and stable
CEI films.
Embodiment 2
Under normal temperature and pressure, in the glove box full of argon gas（Oxygen, water content are less than 0.1ppm）In, by ionic liquid 1- hydroxyl second
Base -3- methyl imidazolium tetrafluoroborates and glycol sulfite are according to mass ratio 8：2 are uniformly mixed.On the basis of quality, to mixed
The difluorine oxalic acid boracic acid lithium in a concentration of 0.4M/kg of in the mixed solvent is added in bonding solvent, is uniformly mixed, obtains lithium ion battery
Electrolyte 10g.
Lithium-rich anode is prepared according to the preparation method of 1 lithium-rich anode of embodiment.
Battery is prepared according to the preparation method of 1 battery of embodiment.
By the battery standing being prepared for 24 hours after, using Shenzhen Fu Yida climatic chambers control environment temperature be 85 DEG C,
The cycle performance of battery is tested using the blue electricity CT2001A battery test systems in Wuhan, wherein test parameter is charging/discharging voltage model
It is 2-4.6V to enclose, and is recycled 50 times with 1C.Fig. 6 is the battery discharge specific volume spirogram that the present embodiment charge and discharge cycles are tested.From
It can be seen from the figure that, the battery ambient temperature prepared by the present embodiment can work normally under conditions of being 85 DEG C, and with good
Good cyclical stability.
In conclusion a kind of lithium ion battery electrolyte provided by the invention, it can be during charge and discharge cycles just
Pole surface formed stablize densification CEI films, can effective protection electrode material, prevent electrolyte from decomposing.Therefore, of the present invention
Electrolysis mass-energy significantly improve cyclical stability and safety of the lithium ion battery under high temperature high voltage environment.
It should be understood that the application of the present invention is not limited to the above for those of ordinary skills can
With improvement or transformation based on the above description, all these modifications and variations should all belong to the guarantor of appended claims of the present invention
Protect range.
Claims (9)
1. a kind of lithium ion battery electrolyte, which is characterized in that including following components:Ionic liquid, sulfone class organic solvent and lithium
Salt.
2. lithium ion battery electrolyte according to claim 1, which is characterized in that the cation of the ionic liquid is piperazine
One kind in pyridine cationoid, pyrrolidines cation, alkyl imidazolium cation.
3. lithium ion battery electrolyte according to claim 1, which is characterized in that the anion of the ionic liquid is
TFSI-、FSI-、BF4 -、DFOB-In one kind.
4. lithium ion battery electrolyte according to claim 1, which is characterized in that the sulfone class organic solvent is ring fourth
One kind in sulfone, glycol sulfite, 1,3- propane sultones, dimethyl sulfite, sulfurous acid diethyl ester.
5. lithium ion battery electrolyte according to claim 1, which is characterized in that the lithium salts is difluoro oxalate boric acid
Lithium.
6. lithium ion battery electrolyte according to claim 1, which is characterized in that the ionic liquid has with the sulfone class
The mass ratio of solvent is（0.4-0.8）：（0.2-0.6）.
7. lithium ion battery electrolyte according to claim 6, which is characterized in that the lithium salts in the ionic liquid and
A concentration of 0.3-0.5 mols/kg in the sulfone class organic solvent.
8. a kind of preparation method of the lithium ion battery electrolyte as described in claim any one of 1-7, which is characterized in that including with
Lower step：
Under atmosphere of inert gases, ionic liquid and sulfone class organic solvent are uniformly mixed, mixed solvent is obtained；
Lithium salts is added in the mixed solvent, is uniformly mixed, obtains the electrolyte.
9. a kind of lithium ion battery, which is characterized in that including the lithium ion battery electrolyte as described in claim any one of 1-7.
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| Publication number | Publication date |
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| CN108336412B (en) | 2021-02-26 |
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