CN107437634A - A kind of ternary lithium electricity Overcharge prevention electrolyte and lithium ion battery - Google Patents
A kind of ternary lithium electricity Overcharge prevention electrolyte and lithium ion battery Download PDFInfo
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- 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
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- 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
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- H01M10/00—Secondary cells; Manufacture thereof
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- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
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- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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Abstract
Embodiment of the present invention discloses a kind of ternary lithium electricity Overcharge prevention electrolyte, effectively solves problem on fire from explosion caused by lithium battery overshoot, present invention also offers a kind of lithium ion battery.The ternary lithium electricity Overcharge prevention electrolyte of the present invention, including lithium salts, organic solvent, overcharging additive, flame-retardant additive, film for additive.The lithium ion battery of the present invention, including cathode sheet, anode pole piece, the barrier film being placed between cathode sheet and anode pole piece and the ternary lithium electricity Overcharge prevention electrolyte.
Description
Technical field
The present invention relates to field of lithium ion battery, more particularly to a kind of ternary lithium electricity Overcharge prevention electrolyte and lithium-ion electric
Pond.
Background technology
Lithium ion battery is widely used in mobile phone and notebook computer, and it is a kind of rechargeable battery, relies primarily on lithium ion
Movement carrys out work between a positive electrode and a negative electrode, general to use the material for containing elemental lithium as electrode.
Lithium ion battery has high-energy-density and high-specific-power, with the obvious advantage, is the potentiality person of following electrokinetic cell system,
And the representative of modern high performance battery.But in safety issue, lithium ion battery due to occurring that battery explosion rises often
The problem of fiery, this largely governs use of the lithium ion battery on vehicle electric system.Cause safety issue
Factor it is a lot, wherein overcharge is one of common factors.Improved with the energy density of batteries of electric automobile, ternary nickel cobalt manganese
Material is widely used, and in order to improve energy density, the heat endurance of material, drops in the increase of nickel content in material
Low, the security performance of battery is deteriorated, and makes the harsher by condition of overcharge, in order to solve these problems, traditional method
It is that safety valve and overshoot protection circuit are installed to battery, but effect is still unsatisfactory.
Therefore, for the above situation, the structure of existing lithium ion battery how is improved, so as to solve the shortcomings that above-mentioned, into
For those skilled in the art's important technological problems urgently to be resolved hurrily.
The content of the invention
Embodiment of the present invention provides a kind of ternary lithium electricity Overcharge prevention electrolyte, effectively solves caused by lithium battery overshoot
Problem on fire from explosion.Present invention also offers a kind of lithium ion battery.
To solve the above problems, a kind of ternary lithium electricity Overcharge prevention electrolyte provided by the invention, including lithium salts, You Jirong
Agent, overcharging additive, flame-retardant additive, film for additive.
Preferably, the lithium salt is 0.01-2mol/L, and the lithium salts is lithium hexafluoro phosphate, difluorophosphate, double fluorine
It is one or more in sulfimide lithium, LiBF4, di-oxalate lithium borate and double (trimethyl fluoride sulfonyl) imine lithiums.
Preferably, the lithium salt is 0.8-1.2mol/L.
Preferably, the organic solvent is made up of cyclic carbonate and linear carbonate.
Preferably, the cyclic carbonate be ethylene carbonate, propene carbonate, one kind in fluorinated ethylene carbonate or
A variety of, the linear carbonate is dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, methyl propyl carbonate, propyl propionate and third
One or more in acetoacetic ester.
Preferably, the overcharging additive is one kind in benzene derivate, including adjacent benzene, cyclohexyl benzene, tert-butyl benzene
It is or a variety of；
The overcharging additive quality is the 2-3% of electrolyte quality, and its structural formula is：
Wherein, in the structural formula：C, D, E, F independently are any in phenyl, cyclohexyl, hydrogen atom or fluorine atom
Kind.
Preferably,
The flame-retardant additive is cyclotrinitrile phosphide；
The quality of the flame-retardant additive is the 0.5-2.5% of the ternary lithium electricity Overcharge prevention electrolyte quality,
The structural formula of the flame-retardant additive is：
Wherein, R is the one or more in phenoxy group, ethyoxyl, oxygen ethene, fluorine atom in cyclotrinitrile phosphide.
Preferably,
The film for additive is ethylene carbonate VC and sulfuric acid vinyl ester DTD；
The film for additive quality is the 1-2% of the ternary lithium electricity Overcharge prevention electrolyte quality.
The present invention also provides a kind of lithium ion battery, including cathode sheet, anode pole piece, is placed in cathode sheet and anode pole
Ternary lithium electricity Overcharge prevention electrolyte described in barrier film and above-mentioned any one between piece.
Preferably, the cathode sheet includes aluminum foil current collector and negative electrode diaphragm, and the anode pole piece includes copper foil afflux
Body and anode diaphragm；
The negative electrode diaphragm includes cathode active material, conductive agent and binding agent, and the anode diaphragm includes anode activity
Material, conductive agent and binding agent；
The cathode active material is LiNi1-x-yCoXMnyO2(NCM)；
The anode active material is Delanium, native graphite, lithium titanate or Si-C composite material.
As can be seen from the above technical solutions, embodiment of the present invention has advantages below：The anti-overcharge electricity of this ternary lithium electricity
Liquid is solved, is made up of lithium salts, organic solvent, overcharging additive, flame-retardant additive, film for additive.Wherein, it with the addition of film forming addition
Agent, excellent interface diaphragm is effectively formed in electrode surface, reduce the reactivity of electrode material and electrolyte and stable electricity
Pole material microstructure, lift electrokinetic cell cycle performance and high temperature performance；And the solid electrolyte impedance formed is low, has
Beneficial to lithium rechargeable battery Internal dynamics characteristic is improved, so as to improve the safety issue of lithium ion battery, especially subtract
The problem of few overshoot blast.
Brief description of the drawings
Fig. 1 is the result schematic diagram of a kind of ternary lithium electricity Overcharge prevention electrolyte of the present invention and lithium ion battery comparative example 1；
Fig. 2 is the result schematic diagram of a kind of ternary lithium electricity Overcharge prevention electrolyte of the present invention and lithium ion battery embodiment 1；
Fig. 3 is the result schematic diagram of a kind of ternary lithium electricity Overcharge prevention electrolyte of the present invention and lithium ion battery embodiment 5.
Embodiment
Embodiment of the present invention provides ternary lithium electricity Overcharge prevention electrolyte, effectively solves to explode caused by lithium battery overshoot
Problem on fire.Present invention also offers a kind of lithium ion battery.
A kind of ternary lithium electricity Overcharge prevention electrolyte of the present invention, including lithium salts, organic solvent, overcharging additive, fire-retardant add
Add agent, film for additive.
Preferably, the lithium salt is 0.01-2mol/L, and the lithium salts is lithium hexafluoro phosphate, difluorophosphate, double fluorine
It is one or more in sulfimide lithium, LiBF4, di-oxalate lithium borate and double (trimethyl fluoride sulfonyl) imine lithiums.
Preferably, the lithium salt is 0.8-1.2mol/L.
Preferably, the organic solvent is made up of cyclic carbonate and linear carbonate.
Preferably, the cyclic carbonate be ethylene carbonate, propene carbonate, one kind in fluorinated ethylene carbonate or
A variety of, the linear carbonate is dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, methyl propyl carbonate, propyl propionate and third
One or more in acetoacetic ester.
Preferably, the overcharging additive is one kind in benzene derivate, including adjacent benzene, cyclohexyl benzene, tert-butyl benzene
It is or a variety of；
The overcharging additive quality is the 2-3% of electrolyte quality, and its structural formula is：
Wherein, in the structural formula：C, D, E, F independently are any in phenyl, cyclohexyl, hydrogen atom or fluorine atom
Kind.
It should be noted that overcharging additive quality is the 2-3% of electrolyte quality, looks like and be set as 1 for electrolyte, mistake
Fill the 2-3% that additive accounts for electrolyte, content hereafter, the meaning with it is where like.
Preferably,
The flame-retardant additive is cyclotrinitrile phosphide；
The quality of the flame-retardant additive is the 0.5-2.5% of the ternary lithium electricity Overcharge prevention electrolyte quality,
The structural formula of the flame-retardant additive is：
Wherein, R is the one or more in phenoxy group, ethyoxyl, oxygen ethene, fluorine atom in cyclotrinitrile phosphide.
Preferably,
The film for additive is ethylene carbonate VC and sulfuric acid vinyl ester DTD；
The film for additive quality is the 1-2% of the ternary lithium electricity Overcharge prevention electrolyte quality.
In the prior art, general overcharging additive is had using biphenyl, ring ethylo benzene and tert-butyl benzene etc. closes effect
Benzene-like compounds, this kind of additive easily to performance of lithium ion battery produce deterioration, D.C. resistance increase, battery storage performance
And cycle performance is poor, and when its addition exceedes the 5% of the weight/mass percentage composition of electrolyte, more there is performance severe exacerbation
Risk, therefore the security performance of lithium ion battery and chemical property can not be taken into account.And the electrolyte of the present invention then substantially reduces
Such a situation.
This ternary lithium electricity Overcharge prevention electrolyte, added by lithium salts, organic solvent, overcharging additive, flame-retardant additive, film forming
Agent forms.Wherein, film for additive is with the addition of, excellent interface diaphragm is effectively formed in electrode surface, reduces electrode material
With the reactivity and stabilized electrodes material microstructure of electrolyte, electrokinetic cell cycle performance and high temperature performance are lifted；And
And formed solid electrolyte impedance it is low, be advantageous to improve lithium rechargeable battery Internal dynamics characteristic, so as to improve lithium from
The safety issue of sub- battery, especially reduce the problem of overshoot is exploded.
Furthermore, it is understood that flame-retardant additive uses phosphazene compound, the side chain of phosphazene compound is containing heteroatomic long-chain
Group, there is one or both of aromatic ring, heteroaromatic, oxygen ethene group, relative to other structures in long chain alkyl group, it may be possible to
Because aromatic ring and heteroaromatic have bigger steric hindrance, phosphazene compound can be in the positive electrode surface shape of lithium ion battery
Into more fine and close effective clad, so as to improve the cyclicity of high-voltage lithium ion batteries.
For further, the phosphazene compound contains N, P atom, has good flame retardant effect, by and aromatic series
Benzene derivative collective effect improves over-charging of battery security performance, avoids and is largely caused using overcharging additive under battery capacity
The side effect of drop.
The present invention also provides a kind of lithium ion battery, including cathode sheet, anode pole piece, is placed in cathode sheet and anode pole
Ternary lithium electricity Overcharge prevention electrolyte described in barrier film and above-mentioned any one between piece.
Preferably, the cathode sheet includes aluminum foil current collector and negative electrode diaphragm, and the anode pole piece includes copper foil afflux
Body and anode diaphragm；
The negative electrode diaphragm includes cathode active material, conductive agent and binding agent, and the anode diaphragm includes anode activity
Material, conductive agent and binding agent；
The cathode active material is LiNi1-x-yCoXMnyO2(NCM)；
The anode active material is Delanium, native graphite, lithium titanate or Si-C composite material.
Using the electrolyte of the present invention, excellent interface diaphragm can be formed to electrode surface, so as to improve lithium-ion electric
The safety issue in pond.
Below by embodiment, the present invention is described in detail with comparative example：
Comparative example 1
(1) preparation of anode pole piece：By positive electrode active materials lithium nickel cobalt manganese LiNi0.5Co0.2Mn0.3O2, conductive agent Super
P and binding agent polyvinylidene fluoride (PVDF) in mass ratio 97：2：1 is made with solvent N-methyl pyrilidone (NMP) mixing
Anode sizing agent, anode sizing agent is uniformly coated in current collector aluminum foil afterwards and is cold-pressed after being dried at 85 DEG C, Ran Houjin
After row trimming, cut-parts, slitting, then 4h is dried under 85 DEG C of vacuum condition, soldering polar ear, complete the preparation of anode pole piece.
(2) preparation of cathode pole piece：By negative active core-shell material graphite, conductive agent Super P, thickener CMC and bonding
Agent agent SBR in mass ratio 97：1：1：1 is made cathode size with solvent deionized water mixing, is afterwards evenly coated in cathode size
It is cold-pressed after being dried on copper foil of affluxion body and at 85 DEG C, after then carrying out trimming, cut-parts, slitting, then in 110 DEG C of vacuum bars
4h is dried under part, soldering polar ear, completes the preparation of cathode pole piece.
(3) preparation of electrolyte：LiPF of the electrolyte using concentration as 1.1mol/L6For lithium salts, with ethylene carbonate (EC),
The mixture of methyl ethyl carbonate (EMC) and diethyl carbonate (DEC) is non-aqueous organic solvent, and EC, EMC, DMC mass ratio are 1：
1：1.Ethylene carbonate VC is as film for additive, content 1%.
(4) preparation of ternary lithium battery：Using polypropylene film as barrier film, by obtained anode pole piece, barrier film, bear
Pole pole piece is folded in order, barrier film is among both positive and negative polarity pole piece, and winding obtains naked battery core；Naked battery core is placed in outside battery core
In packaging, electrolyte, encapsulation, standing, chemical conversion, shaping, volume test are injected afterwards, completes the preparation of lithium ion battery, wherein
The thickness of lithium ion battery is 8.0mm, width 92.0mm, length 131mm.
As shown in figure 1, when overcharging, product blast, shell are damaged.
Comparative example 2
According to the preparation method of comparative example 1, unlike add weight/mass percentage composition in electrolyte in step (3) and be
3% cyclohexyl benzene is as anti-overcharge additive.
Comparative example 3
According to the preparation method of comparative example 1, unlike add weight/mass percentage composition in electrolyte in step (3) and be
For 2.5% hexaphenoxycyclotriphosphazene as anti-overcharge additive, film for additive is 1% sulfuric acid vinyl ester DTD.
Embodiment 1
Method according to comparative example 1 prepares lithium ion battery, the difference is that adding quality in electrolyte in step (3)
Percentage composition is 3% cyclohexyl benzene and 0.5% hexaphenoxycyclotriphosphazene is as anti-overcharge additive, film for additive
1% sulfuric acid vinyl ester DTD.
As shown in Fig. 2 when overcharging, shell rises bag, does not explode.
Embodiment 2
Method according to comparative example 1 prepares lithium ion battery, the difference is that adding quality in electrolyte in step (3)
The cyclohexyl benzene and 1% hexaphenoxycyclotriphosphazene that percentage composition is 3% are as anti-overcharge additive, film for additive 1%
Sulfuric acid vinyl ester DTD.
Embodiment 3
Method according to comparative example 1 prepares lithium ion battery, the difference is that adding quality hundred in step (3) electrolyte
Divide the cyclohexyl benzene and 1.5% hexaphenoxycyclotriphosphazene that content is 3% as anti-overcharge additive, film for additive 1%
Sulfuric acid vinyl ester DTD.
Embodiment 4
Method according to comparative example 1 prepares lithium ion battery, the difference is that adding quality in electrolyte in step (3)
The cyclohexyl benzene and 2% hexaphenoxycyclotriphosphazene that percentage composition is 3% are as anti-overcharge additive, film for additive 1%
Sulfuric acid vinyl ester DTD.
Embodiment 5
Method according to comparative example 1 prepares lithium ion battery, the difference is that adding quality in electrolyte in step (3)
Percentage composition is 3% cyclohexyl benzene and 2.5% hexaphenoxycyclotriphosphazene is as anti-overcharge additive, film for additive
1% sulfuric acid vinyl ester DTD.
As shown in figure 3, when overcharging, do not rise bag, does not also produce blast.
Embodiment 6
Method according to comparative example 1 prepares lithium ion battery, the difference is that adding quality in electrolyte in step (3)
Percentage composition is 3% cyclohexyl benzene and the phosphonitrile of 0.5% phenyl-pentafluoride epoxide ring three is as anti-overcharge additive, film for additive
1% sulfuric acid vinyl ester DTD.
Embodiment 7
Method according to comparative example 1 prepares lithium ion battery, the difference is that adding quality in electrolyte in step (3)
The cyclohexyl benzene and 1% tert-butyl benzene and 0.5% hexaphenoxycyclotriphosphazene that percentage composition is 2% are as anti-overcharge addition
Agent, film for additive are 1% sulfuric acid vinyl ester DTD.
The results contrast of above-mentioned comparative example and embodiment：
It should be noted that：Different electrolytes form over-charging and require what 1C6.3V was overcharged according to GB/T31485-2015
Statistical result is as shown in table 1.
The present invention show only the schematic diagram of comparative example 1, embodiment 1 and embodiment 5,
Table 1：
As it can be seen from table 1 as flame retardant amount increases, battery performance declines.When fire retardant is six phenoxy groups
During three phosphonitrile of ring, embodiment 1 is most preferred embodiment.
Drawn a conclusion by overcharging test result：Effectively reduced using lithium ion battery made from the electrolyte of the present invention
Explosive event when filling, explosive event is occurred without substantially, and using lithium ion battery made from the method for prior art, generate quick-fried
It is fried.
It can be seen that effectively being reduced by lithium ion battery made of the electrolyte of the present invention, or even explosive event is occurred without, this
Invention safety can be promoted.
Described above, embodiment of above and embodiment are merely illustrative of the technical solution of the present invention, rather than its limitations；
Although the present invention is described in detail with reference to aforementioned embodiments and embodiment, one of ordinary skill in the art should
Understand：It can still modify to the technical scheme described in foregoing embodiments, or to which part technical characteristic
Carry out equivalent substitution；And these modifications or replacement, the essence of appropriate technical solution is departed from each embodiment of the present invention
With the spirit and scope of embodiment technical scheme.
Claims (10)
1. a kind of ternary lithium electricity Overcharge prevention electrolyte, it is characterised in that including lithium salts, organic solvent, overcharging additive, fire-retardant add
Add agent, film for additive.
2. ternary lithium electricity Overcharge prevention electrolyte according to claim 1, it is characterised in that the lithium salt is 0.01-
2mol/L, the lithium salts are lithium hexafluoro phosphate, difluorophosphate, double fluorine sulfimide lithiums, LiBF4, di-oxalate lithium borate
With one or more in double (trimethyl fluoride sulfonyl) imine lithiums.
3. ternary lithium electricity Overcharge prevention electrolyte according to claim 2, it is characterised in that the lithium salt is 0.8-
1.2mol/L。
4. ternary lithium electricity Overcharge prevention electrolyte according to claim 1, it is characterised in that the organic solvent is by ring-type carbon
Acid esters forms with linear carbonate.
5. ternary lithium electricity Overcharge prevention electrolyte according to claim 4, it is characterised in that the cyclic carbonate is carbonic acid
One or more in vinyl acetate, propene carbonate, fluorinated ethylene carbonate, the linear carbonate are dimethyl carbonate, carbon
One or more in diethyl phthalate, methyl ethyl carbonate, methyl propyl carbonate, propyl propionate and ethyl propionate.
6. ternary lithium electricity Overcharge prevention electrolyte according to claim 1, it is characterised in that the overcharging additive is benzene
One or more in derivative, including adjacent benzene, cyclohexyl benzene, tert-butyl benzene；
The overcharging additive quality is the 2-3% of electrolyte quality, and its structural formula is：
Wherein, in the structural formula：C, D, E, F independently are any of phenyl, cyclohexyl, hydrogen atom or fluorine atom.
7. the ternary lithium electricity Overcharge prevention electrolyte according to any one in claim 1~6, it is characterised in that
The flame-retardant additive is cyclotrinitrile phosphide；
The quality of the flame-retardant additive is the 0.5-2.5% of the ternary lithium electricity Overcharge prevention electrolyte quality,
The structural formula of the flame-retardant additive is：
Wherein, R is the one or more in phenoxy group, ethyoxyl, oxygen ethene, fluorine atom in cyclotrinitrile phosphide.
8. the ternary lithium electricity Overcharge prevention electrolyte according to any one in claim 1~6, it is characterised in that
The film for additive is ethylene carbonate VC and sulfuric acid vinyl ester DTD；
The film for additive quality is the 1-2% of the ternary lithium electricity Overcharge prevention electrolyte quality.
9. a kind of lithium ion battery, it is characterised in that including cathode sheet, anode pole piece, be placed in cathode sheet and anode pole piece
Between barrier film and claim 1~8 in ternary lithium electricity Overcharge prevention electrolyte described in any one.
10. lithium ion battery according to claim 9, it is characterised in that the cathode sheet include aluminum foil current collector and
Negative electrode diaphragm, the anode pole piece include copper foil current collector and anode diaphragm；
The negative electrode diaphragm includes cathode active material, conductive agent and binding agent, the anode diaphragm include anode active material,
Conductive agent and binding agent；
The cathode active material is LiNi1-x-yCoXMnyO2(NCM)；
The anode active material is Delanium, native graphite, lithium titanate or Si-C composite material.
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| CN108365264A (en) * | 2018-01-17 | 2018-08-03 | 湖南博信新能源科技有限公司 | A kind of lithium battery tertiary electrolyte |
| CN108470947A (en) * | 2018-03-30 | 2018-08-31 | 北京国能电池科技股份有限公司 | For lithium battery electrolytes anti-overcharge additive and include its lithium battery electrolytes |
| CN108511801A (en) * | 2018-04-10 | 2018-09-07 | 山东海容电源材料股份有限公司 | A kind of high safety type lithium battery electrolytes |
| CN108808088A (en) * | 2018-06-06 | 2018-11-13 | 广东天劲新能源科技股份有限公司 | A kind of anti-overcharge lithium battery electrolytes and lithium battery, lithium battery preparation method |
| CN110444815A (en) * | 2019-08-12 | 2019-11-12 | 河南华瑞高新材料有限公司 | A kind of high security electrolyte based on nickelic ternary lithium ion battery |
| WO2023015444A1 (en) * | 2021-08-10 | 2023-02-16 | 宁德时代新能源科技股份有限公司 | Lithium-ion secondary battery, battery module, battery pack, and electrical device |
| CN117855608A (en) * | 2024-03-07 | 2024-04-09 | 宁德新能源科技有限公司 | Electrolyte, secondary battery, and electronic device |
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