CN108206299A - Lithium ion battery and electrolyte thereof - Google Patents
Lithium ion battery and electrolyte thereof Download PDFInfo
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- CN108206299A CN108206299A CN201611178918.0A CN201611178918A CN108206299A CN 108206299 A CN108206299 A CN 108206299A CN 201611178918 A CN201611178918 A CN 201611178918A CN 108206299 A CN108206299 A CN 108206299A
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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
- 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
- H01M10/0567—Liquid materials characterised by the additives
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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 invention discloses a lithium ion battery electrolyte, which comprises lithium salt, an organic solvent and an additive, wherein the additive comprises a compound shown in a formula I and a compound shown in a formula II, and the structural formula of the additive is as follows:wherein n is 1-9, R1、R2、R3Independently selected from a halogen atom, a phenyl group, an alkane group with 0-9 carbon atoms completely or partially substituted by a halogen atom, and a cyclic alkyl group with 0-9 carbon atoms completely or partially substituted by a halogen atom; r4、R5、R6、R7At least one of which is selected from F, Br or Cl. Compared with the prior art, the compound of the formula I and the compound of the formula II are added into the electrolyte as additives, so that the problem of high-temperature gas generation of the lithium ion battery can be obviously solved, the cycle storage performance of the lithium ion battery is improved, and the lithium ion battery has good application value. The invention also discloses a lithium ion battery.
Description
Technical field
The invention belongs to new energy materials field, it is more particularly related to which one kind improves high temperature aerogenesis problem
And the lithium ion battery and its electrolyte that storage performance is good.
Background technology
Higher than energy, operating voltage is high, temperature limit is wide, self-discharge rate is low, the cycle longevity because having for lithium ion battery
Life is long, pollution-free and the advantages that have a safety feature, in recent years by numerous studies and be widely used in mobile phone, portable computer,
In the mobile electronic devices such as video camera, camera, in Aeronautics and Astronautics, navigation, artificial satellite, small medical and military logical
It interrogates apparatus field and also gradually replaces conventional batteries.
Current era pursues lithium ion battery high-energy density and has become trend of the times, currently used to carry respectively
The operating voltage of high positive electrode, the negative material of high-nickel material and use with more high discharge capacity using high gram volume.
Wherein, with the increase of nickel content, the oxidisability that material takes off lithium state is remarkably reinforced anode high-nickel material, and electrolyte is in de- lithium state
Oxygenolysis easily occurs for high-nickel material surface, deteriorates the cycle life of battery core, this proposes current electrolyte and greatly chooses
War.Silicon materials have the theoretical specific capacity far above graphite cathode material, there are huge volume expansion in cyclic process, separately
Outside, solid electrolyte interface (abbreviation SEI) film of cathode ruptures in cyclic process, causes electrolyte that reduction point occurs
Solution generates a large amount of by-products, deteriorates cycle performance.It is positive and negative when particularly full charge pond uses or stores at high operating temperatures
Pole is further enhanced with the activity that electrolyte reacts, and exothermic heat of reaction amount is significantly increased, and generates a large amount of gases, battery is caused to be sent out
Raw volume expansion is also possible to cause short circuit occurs in battery when serious.
In view of this, it a kind of improve high temperature aerogenesis problem it is necessory to provide and recycles the good lithium-ion electric of storage performance
Pond and its electrolyte.
Invention content
It is an object of the invention to：Overcome the problems, such as that existing high-temperature lithium ion battery aerogenesis is serious, providing one kind improves
High temperature aerogenesis problem and the good lithium ion battery and its electrolyte of storage performance.
In order to achieve the above-mentioned object of the invention, the present invention provides a kind of lithium-ion battery electrolytes, including lithium salts, You Jirong
Agent and additive, the additive includes compound of formula I and Formula II compound, structural formula are as follows：
Wherein, n is 1~9, R1、R2、R3Replace completely independently selected from halogen atom, phenyl, by halogen atom or part replaces
Carbon atom number be 0~9 alkyl, replaced completely by halogen atom or cyclic annular alkane that partially substituted carbon atom number is 0~9
Base；R4、R5、R6、R7In at least one be selected from F, Br or Cl.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the compound of formula I is 2,2- difluoro propionic acid propylene
One or more of ester, 2- isobutyl bromides acrylic ester, pivalic acid acrylic ester；2,2- difluoros propylene carbonate, 2- isobutyl bromides
Acrylic ester, the structural formula of pivalic acid acrylic ester are as follows：
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the Formula II compound for fluorinated ethylene carbonate,
1,2- difluorinated ethylene carbonates or chlorocarbonic acid vinyl acetate；Fluorinated ethylene carbonate, 1,2- difluorinated ethylene carbonates, chloro
The structural formula of ethylene carbonate is as follows：
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the compound of formula I accounts for lithium-ion battery electrolytes
The 0.01~5% of gross mass.When the content of the compound of formula I in electrolyte is too low, which can not form in anode and cause
Close SEI films are not improved the high temperature storage aerogenesis of system；It, then can be because of formation when the too high levels of compound of formula I
Blocked up SEI films and the interface impedance for dramatically increasing positive electrode surface, while can also deteriorate 25 DEG C of battery, 45 DEG C of cycle performances.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the compound of formula I accounts for lithium-ion battery electrolytes
The 0.1~3% of gross mass.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the Formula II compound accounts for lithium-ion battery electrolytes
The 0.5~30% of gross mass.Formula II compounds content is related to negative material ingredient and content：When the Formula II chemical combination in electrolyte
When object content is too low, negative electrode active interface can be led to, particularly in silicon-based anode system, active particle can not obtain effectively
Protection, and then a large amount of side reaction occurs, it such as generates a large amount of reducibility gas and destroys interface stability, battery core cycle performance is caused to add
Play deteriorates；Conversely, when the too high levels of electrolyte compound of formula H, especially under the high temperature conditions, charging and discharging lithium battery mistake
Cheng Zhong, oxidative decomposition, the by-product HF of generation etc., which occurs, for high-nickel material and the electrolyte contacts of Strong oxdiative state can cause just
The destruction of pole material structure can also deteriorate lithium battery cycle performance.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the additive further includes the ring-type containing sulfur-to-oxygen double bond
Ester type compound, such as：Sulfuric acid vinyl ester etc..Its role is to further improve the storage performance of lithium battery, and to a certain degree
On improve the cycle performance of lithium ion battery.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the lithium salts is conventional selection, optionally, including
But it is not limited to LiPF6、LiBF4、LiN(SO2F)2、LiN(CF3SO2)2、LiClO4、LiAsF6、LiB(C2O4)2、LiBF2(C2O4)、
LiN(SO2RF)2、LiN(SO2F)(SO2RF) in it is one or more, wherein, RFFor Cn′F2n′+1, n ' is 1~10.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the lithium salts accounts for the total matter of lithium-ion battery electrolytes
The 6.25~25% of amount.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the organic solvent can according to actual demand into
Row selection, preferably non-aqueous organic solvent, if carbon atom number is 1~8 and the compound containing at least one ester group.
As a kind of improvement of lithium-ion battery electrolytes of the present invention, the organic solvent is ethylene carbonate, carbonic acid
Acrylic ester, butylene, carbonic acid amylene ester, fluorinated ethylene carbonate, dimethyl carbonate, diethyl carbonate, dipropyl carbonate,
It is one or more in one or more or above compound halo derivatives in methyl ethyl carbonate.
In order to achieve the above-mentioned object of the invention, the present invention also provides a kind of lithium ion battery, including anode, cathode, isolation
Film and electrolyte, the electrolyte include lithium salts, organic solvent and additive, and additive includes compound of formula I and Formula II chemical combination
Object, structural formula are as follows：
Wherein, n is 1~9, R1、R2、R3Replace completely independently selected from halogen atom, phenyl, by halogen atom or part replaces
Carbon atom number be 0~9 alkyl, replaced completely by halogen atom or cyclic annular alkane that partially substituted carbon atom number is 0~9
Base；R4、R5、R6、R7In at least one be selected from F, Br or Cl.
Compared with prior art, lithium ion battery and its electrolyte of the present invention have following features：
Electrolyte provided by the invention comprising compound of formula I and Formula II compound, Formula II compound can be in cathode shape
Into fine and close and high-ductility solid electrolyte interface (SEI) film, improve cycle performance of lithium ion battery, but at the same time, also hold
The aerogenesis problem for easily leading to inside battery is serious；By the introducing of compound of formula I, it is anti-can polymerization effectively to occur at anode interface
The SEI films of dense uniform should and be formed, effective the isolation positive electrode of high oxidation state and electricity during charging and discharging lithium battery
The contact of liquid is solved, the serious aerogenesis that Formula II compound is brought is solved the problems, such as and hydrofluoric acid (HF) is prevented to break the corrosion of cathode
It is bad so that the positive and negative anodes interface stability of lithium ion battery.It particularly, should by the electrolyte system containing Formulas I and Formula II compound
For in nickelic/silicon cathode lithium ion battery system of high-energy density, aerogenesis inhibition to be notable.In addition, by sulfuric acid second
Alkene ester type compound and Formulas I, Formula II compound are used cooperatively, and not only overcome that lithium battery high temperature storage aerogenesis is serious lacks
It falls into, ensures electrode of lithium cell interface stability, it is ensured that the cycle performance of lithium ion battery is unaffected, effectively improves lithium-ion electric
The cycle residual capacity in pond, makes lithium ion battery show good chemical property.
Specific embodiment
In order to which the goal of the invention, technical solution and the advantageous effects that make the present invention are more clear, with reference to embodiments,
The present invention will be described in further detail.It should be understood that the embodiment described in this specification is just for the sake of explanation
The present invention, is not intended to limit the present invention, formula, ratio of embodiment etc. can adaptation to local conditions make a choice and reality had no to result
Matter influences.
Embodiment 1
Lithium ion battery (abbreviation battery) S1 is prepared by the following method：
(1) preparation of positive plate
By nickle cobalt lithium manganate (LiNi0.8Co0.1Mn0.1O2), binding agent (Kynoar), conductive agent (conductive carbon black) press
It is 98 according to weight ratio:1:1 is mixed, and adds in N-Methyl pyrrolidone (NMP), is stirred under de-airing mixer effect to system
Into transparent and homogeneous shape, anode sizing agent is obtained；Anode sizing agent is evenly applied on the aluminium foil that thickness is 12 μm；By aluminium foil in room temperature
120 DEG C of oven drying 1h are transferred to after drying, then obtain positive plate by cold pressing, cutting.
(2) preparation of negative plate
By silico-carbo compound, conductive agent (conductive carbon black), binding agent polyacrylate according to weight ratio be 98:1:1 carries out
Mixing, after being added to deionized water, negative electrode slurry is obtained under the stirring action of de-airing mixer；Negative electrode slurry is uniformly coated
On copper foil；Copper foil after room temperature is dried is transferred to 120 DEG C of oven drying 1h, then obtains negative plate by cold pressing, cutting.
(3) preparation of electrolyte
In drying shed, the EC and DEC of rectifying and dewatering purification process are uniformly mixed to form organic solvent, it will be abundant
Dry lithium salts is dissolved in above-mentioned organic solvent, then adds in lithium salts LiPF in organic solvent6, additive be 8wt%
The allyl trifluoro acetate of fluorinated ethylene carbonate and 0.5wt% is uniformly mixed, and obtains electrolyte.Wherein, lithium salts is a concentration of
1mol/L, content are the 12.5% of electrolyte gross mass, and the weight ratio of EC, EMC, DEC are EC:EMC:DEC=1:1:1.
(4) preparation of lithium ion battery
The positive plate routinely cut and negative plate, lithium battery isolation membrane are folded in order, are in lithium battery isolation membrane
Play the role of isolation between positive and negative plate, then winding obtains naked battery core；Naked battery core is placed in outer packing foil, it will be above-mentioned
The electrolyte prepared is injected into dried battery, by processes such as Vacuum Package, standing, chemical conversion, shapings, obtain lithium from
Sub- battery (abbreviation S1).
Embodiment 2~19 (S2~S19) and comparative example 1~8 (D1~D8), the preparation method is the same as that of Example 1, difference
The additive being in its electrolyte, detailed additive types and content are referring to table 1.
The type and dosage of electrolysis additive in 1 comparative example 1~8 of table and embodiment 1~19
Note：Any substance is not added in "-" expression in table 1.
Performance test
The loop test that 25 DEG C and 45 DEG C of lithium ion battery
The battery that comparative example 1~8 and embodiment 1~19 obtain respectively is subjected to following tests：Respectively at 25 DEG C and
At 45 DEG C, by battery, with 1C constant-current charges to 4.2V, then constant-voltage charge to electric current is 0.05C, then with 1C constant-current discharges extremely
2.8V at this time to recycle for the first time, is repeatedly recycled according to above-mentioned condition battery, circulating battery is calculated respectively 200 times,
Capacity retention ratio after 400 times, 600 times, wherein, the capacity retention ratio after cycle is calculated according to the following formula, dependence test number
According to referring to table 2 and table 3.
Capacity retention ratio after cycle=(discharge capacity of corresponding cycle/discharge capacity recycled for the first time) × 100%.
The circulation volume conservation rate of 2 comparative example 1~8 of table and 1~19 gained battery of embodiment at 25 DEG C
The circulation volume conservation rate of 3 comparative example 1~8 of table and 1~19 gained battery of embodiment at 45 DEG C
Lithium ion battery is tested in 80 DEG C of storage
Battery S1~S19 and battery D1~D8 are subjected to following tests respectively：
By lithium ion battery at room temperature with 1C constant-current charges to 4.2V, it is 0.05C that then constant pressure 4.2V, which charges to electric current,
Test the volume V of battery0；Lithium ion battery is put into 80 DEG C of insulating box later, is stored 10 days, and takes out within n-th day test electricity
The volume in pond is simultaneously denoted as Vn, lithium ion battery is calculated respectively by following formula in the cubical expansivity of the 10th day, as a result please join
It is shown in Table 4.
High-temperature lithium ion battery store n days after cubical expansivity (%)=(Vn-V0)/V0× 100%, wherein n for lithium from
The number of days of sub- battery high-temperature storage.
80 DEG C of storage volume expansion rates of battery that 4 comparative example 1~8 of table and embodiment 1~19 obtain
From table 2 and table 3 it is known that compared with battery D2~D3 of only adding type II compounds, while add in Formulas I and formula
The capacity retention ratio of battery S1~S5, the S8~S19 of II additives batteries under 25,45 DEG C of cycles is basically identical；But and D5
The battery that~D8 only adds compound of formula I is compared, and the capacity retention ratio of 25,45 DEG C of cycles is significantly higher.This shows enough
The Formula II compound of amount is as silicium cathode film for additive, the introducing of the compound of formula I of reasonable amount, 25 DEG C to lithium battery, 45
DEG C cycle performance influence will not be very big.
From table 4, it can be seen that S1~S19 the batteries for adding in Formulas I and Formula II compound simultaneously as electrolysis additive exist
After high temperature storage, it is respectively provided with relatively low cubical expansivity.By S1~S5, S8 with compound of formula I it can be seen from S19 (including mixing
Using) and the combination of Formula II compound, it can be very good to solve the problems, such as the serious aerogenesis that film for additive (Formula II compound) is brought.
With the increase of compound of formula I content, the aerogenesis of battery high-temperature is effectively suppressed；When compound of formula I content reaches 5%,
Aerogenesis inhibiting effect tends towards stability.But when the adding too much of Formulas I (S6,6wt%), blocked up SEI can be formed in cathode
Film increases the DCR of battery, deteriorates room temperature and high temperature circulation, greatly reduces the chemical property of battery.
The usage amount of cathode film formation agent (Formula II compound) is related to the negative material ingredient of battery design system, for height
The battery of energy density design, if negative electrode active material selects silicon and silicon class material, the content of active material is higher, required
Film for additive (Formula II compound) amount is also more.When the Formula II compounds content in electrolyte is excessively high, especially in high temperature item
Under part, during charging and discharging lithium battery, oxidative decomposition occurs for high-nickel material and the electrolyte contacts of Strong oxdiative state, generation
By-product HF etc. can also deteriorate lithium battery cycle performance to cathode material structure is caused to be destroyed.And in electrolyte of the present invention
In system, by S3, S8, S9 and S14~S19 it can be found that adding in additive Formulas I and Formula II chemical combination simultaneously in electrolyte system
Object, more and less Formula II additive, can form stable SEI films, and aerogenesis problem can in electrolyte system
Be effectively suppressed by the addition of compound of formula I, 25 DEG C of lithium battery, 45 DEG C of cycle performances all show the same, high temperature storage
Aerogenesis problem be also effectively suppressed.
In addition, the compounds such as addition of C (sulfuric acid vinyl ester) and Formulas I, Formula II, which are used in combination, can further improve battery core
Cycle performance and the chemical properties such as capacity storage.In summary, it can be found that formula Compound I inhibits as aerogenesis
Agent, Formula II compound are united and applied in electrolyte, lithium ion battery obtained is in the case where ensureing 25 DEG C, 45 DEG C as film forming agent
Cycle performance it is consistent with previous level on the basis of, can also significantly improve storage aerogenesis of the lithium ion battery under 80 DEG C of high temperature
Problem.
According to the disclosure and teachings of the above specification, those skilled in the art in the invention can also be to above-mentioned embodiment party
Formula carries out appropriate change and modification.Therefore, the invention is not limited in specific embodiment disclosed and described above, to this
Some modifications and changes of invention should also be as falling into the scope of the claims of the present invention.In addition, although this specification
In used some specific terms, but these terms are merely for convenience of description, do not limit the present invention in any way.
Claims (10)
- A kind of 1. lithium-ion battery electrolytes, including lithium salts, organic solvent and additive, which is characterized in that the additive packet Compound of formula I and Formula II compound are included, structural formula is as follows：Wherein, n is 1~9, R1、R2、R3Replace completely independently selected from halogen atom, phenyl, by halogen atom or partially substituted carbon Alkyl that atomicity is 0~9 is replaced or cyclic alkyl that partially substituted carbon atom number is 0~9 completely by halogen atom；R4、 R5、R6、R7In at least one be selected from F, Br or Cl.
- 2. lithium-ion battery electrolytes according to claim 1, which is characterized in that the compound of formula I is：One or more of.
- 3. lithium-ion battery electrolytes according to claim 1, which is characterized in that the Formula II compound is：
- 4. lithium-ion battery electrolytes according to claim 1, which is characterized in that the compound of formula I accounts for lithium-ion electric The 0.01~5% of pond electrolyte gross mass.
- 5. lithium-ion battery electrolytes according to claim 4, which is characterized in that the compound of formula I accounts for lithium-ion electric The 0.1~3% of pond electrolyte gross mass.
- 6. lithium-ion battery electrolytes according to claim 1, which is characterized in that the Formula II compound accounts for lithium-ion electric The 0.5~30% of pond electrolyte gross mass.
- 7. lithium-ion battery electrolytes according to claim 1, which is characterized in that it is double that the additive further includes sulfur-bearing oxygen The cyclic annular ester type compound of key.
- 8. lithium-ion battery electrolytes according to claim 1, which is characterized in that the lithium salts is LiPF6、LiBF4、LiN (SO2F)2、LiN(CF3SO2)2、LiClO4、LiAsF6、LiB(C2O4)2、LiBF2(C2O4)、LiN(SO2RF)2、LiN(SO2F) (SO2RF) in it is one or more, wherein, RFFor Cn′F2n′+1, n ' is 1~10.
- 9. lithium-ion battery electrolytes according to claim 1, which is characterized in that the organic solvent is non-aqueous organic molten Agent.
- 10. a kind of lithium ion battery, including anode, cathode, isolation film and electrolyte, which is characterized in that the electrolyte is power Profit requires the lithium-ion battery electrolytes described in any one in 1~9.
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| CN201611178918.0A CN108206299B (en) | 2016-12-19 | 2016-12-19 | Lithium ion battery and electrolyte thereof |
| PCT/CN2017/092318 WO2018113268A1 (en) | 2016-12-19 | 2017-07-09 | Lithium ion battery and electrolyte thereof |
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| CN201611178918.0A CN108206299B (en) | 2016-12-19 | 2016-12-19 | Lithium ion battery and electrolyte thereof |
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| CN116190794A (en) * | 2023-04-27 | 2023-05-30 | 广州天赐高新材料股份有限公司 | Nonaqueous electrolyte and lithium ion battery containing same |
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| WO2019150896A1 (en) * | 2018-01-30 | 2019-08-08 | ダイキン工業株式会社 | Electrolyte, electrochemical device, lithium ion secondary battery, and module |
| CN111540870A (en) * | 2020-05-08 | 2020-08-14 | 中航锂电技术研究院有限公司 | Diaphragm, preparation method and lithium ion battery |
| CN115732756B (en) * | 2021-08-30 | 2023-11-28 | 张家港市国泰华荣化工新材料有限公司 | Electrolyte and secondary battery using same |
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| CN105355975B (en) * | 2015-10-20 | 2018-08-21 | 宁德新能源科技有限公司 | electrolyte and lithium ion battery including the electrolyte |
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| CN108206299B (en) | 2020-10-09 |
| WO2018113268A1 (en) | 2018-06-28 |
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