CN108666623A - A kind of electrolyte of high-voltage lithium ion batteries - Google Patents
A kind of electrolyte of high-voltage lithium ion batteries Download PDFInfo
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- CN108666623A CN108666623A CN201810461745.6A CN201810461745A CN108666623A CN 108666623 A CN108666623 A CN 108666623A CN 201810461745 A CN201810461745 A CN 201810461745A CN 108666623 A CN108666623 A CN 108666623A
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- lithium
- 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
- H01M10/0567—Liquid materials characterised by the additives
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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
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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 provides a kind of high voltage lithium-ion battery electrolytes, belongs to field of lithium ion battery.Including non-aqueous organic solvent, lithium salts and additive, the non-aqueous organic solvent are esters solvent, 95% or more mass percent；The lithium salts is LiPF6, 1.0 1.5mol/L of concentration；Additive is the mixture of two nitrile compounds and boron-containing compound, mass percent 1 5%.The electrolyte that the mixture of two nitrile compounds and borate is used as electrolysis additive by the present invention is suitable for high-voltage anode material LiNi0.5Mn1.5O4System finds that this kind of electrolyte can improve anode material for lithium-ion batteries interface impedance, and improves the stable circulation performance under lithium ion battery room temperature.
Description
Technical field
The invention belongs to field of lithium ion battery, are related to a kind of electrolyte suitable for high-voltage lithium ion batteries.
Background technology
Lithium ion battery has voltage height, higher than energy, has extended cycle life the advantages that good with safety, from 90 years last century
Since being realized commercialization for Sony, lithium ion battery is widely used in mobile phone, and digital camera and notes etc. are just
The property taken equipment, especially it applies more and more extensive, people's lithium ion battery on Large Electric vehicle and energy storage device in recent years
Energy density require it is also higher and higher.
The use of high charge stopping potential positive electrode is one of the main path for improving lithium ion battery energy density, Gao Chong
Electric stopping potential positive electrode mainly has LiNi0.5Mn1.5O2(4.7V vs.Li/Li+)、LiCoPO4(4.8V vs.Li/Li+) and
LiNiPO4(5.1V vs.Li/Li+,167mAh/g).And it is exactly current that above-mentioned material, which is not achieved commercialized main cause,
Commercialization electrolyte can not match high-voltage anode material, i.e., can be aoxidized on positive electrode surface when 4.5V or more works
It decomposes, causes battery performance to decline, limit the application of high-voltage lithium ion batteries.Therefore development high-voltage electrolyte technology at
Key to solve the above-mentioned problems.
However commercialized lithium-ion battery electrolytes are mainly using carbonic ester and carboxylate as solvent at present, this kind of electrolyte
When charging voltage is more than 4.5V, LiPF6It can accelerated decomposition generation HF and PF5, the former can make metal with positive electrode active material qualitative response
Ion, which is dissolved in electrolyte, causes capacitance loss, and it is even poly- that the latter can guide the organic solvents such as ethylene carbonate that oxygenolysis occurs
Reaction is closed, the internal resistance of cell is increased and deteriorates its cycle performance.
Invention content
The problem of in view of background technology, the present invention provide a kind of high voltage suitable for nickel ion doped electrode material
Electrolyte, the electrolyte can meet that 4.7V is used above and cyclical stability is preferable.
The technical solution adopted by the present invention is：
A kind of electrolyte of high-voltage lithium ion batteries, including non-aqueous organic solvent, lithium salts and additive, it is characterised in that
The non-aqueous organic solvent is esters solvent, accounts for the 75-80% of electrolyte quality；Lithium salts is LiPF6；Additive is that two nitriles add
The mixture for adding agent and boron-containing additive accounts for electrolyte gross mass 1-5%.
Further, the two nitriles additive is selected from malononitrile, succinonitrile, glutaronitrile, adiponitrile, pimelic dinitrile and pungent two
One or more of nitrile.
Further, further, additive amount accounts for the 1-3% of the electrolyte gross mass to two nitrile.
Further, the boron-containing additive is selected from di-oxalate lithium borate (LiBOB), difluorine oxalic acid boracic acid lithium
(LiDFOB), a kind of in tetramethyl borate (TMB), trimethylborate (TB) and three (trimethyl silane) borates (TMSB) or
It is several.
Further, the boron-containing additive dosage accounts for the 1-3% of the electrolyte gross mass.
Further, the LiPF6A concentration of 1.0-1.5mol/L.
Further, the non-aqueous organic solvent is selected from ethylene carbonate, propene carbonate, methyl ethyl carbonate, carbonic acid two
One or more of ethyl ester, dimethyl carbonate, ethyl acetate, propyl acetate, methyl propionate and ethyl propionate.
The boron-containing additive accounts for the 1-3% of electrolyte quality, can form one layer on nickel lithium manganate cathode material surface
Protective film stablizes positive electrode interface, ensures the excellent cyclical stability of battery.
The electrolyte that the mixture of two nitrile compounds and borate is used as electrolysis additive by the present invention is suitable for height
Positive polarity material LiNi0.5Mn1.5O4System finds that this kind of electrolyte can improve the resistance of anode material for lithium-ion batteries interface
It is anti-, and improve the stable circulation performance under lithium ion battery room temperature.Described two additives, which are used cooperatively, inhibits esters
Solvent is decomposed in positive electrode surface oxidation, and forms layer protecting film in electrode material surface, prevents electrolyte and electrode material
Material further contact ensures that lithium ion battery height is electric again with this to ensure that the electrolyte is applicable to the working environment of 4.7V or more
Press the cyclical stability under working condition.
Specific implementation mode
Electrolyte in the present invention is applied in high-voltage lithium ion batteries, and wherein this kind of lithium ion battery is with nickel ion doped
LiNi0.5Mn1.5O4For positive electrode, artificial graphite is negative material, and diaphragm is 2400 types of Celgard.Comparative example and embodiment
In every battery electrolyte dosage be 1-5g.Use in comparative example lithium ion battery is free of the conventional electrolysis liquid of additive；
Embodiment lithium ion battery uses the high-voltage electrolyte containing different additive.
Comparative example and embodiment battery prepare as follows：
Comparative example：
(1) in the glove box of atmosphere of inert gases, it is 1 to measure volume ratio successively:1:1 ethylene carbonate (EC), carbon
The solvent that three obtains after mixing is obtained nothing by sour methyl ethyl ester (EMC) and dimethyl carbonate (DMC) through molecular sieve dehydration again
Water mixed solvent.
(2) in the glove box of atmosphere of inert gases, lithium hexafluoro phosphate (LiPF is weighed by the corresponding quality of 1.2M6) and will
It is added to anhydrous in the mixed solvent obtained, and being sufficiently stirred makes its uniform dissolution, is prepared without additive with this
Conventional electrolysis liquid.
(3) conventional electrolysis liquid obtained above is applied to Cr2025 coin shape lithiums in the glove box of atmosphere of inert gases
Ion battery, the anode material for lithium-ion batteries are nickel ion doped LiNi0.5Mn1.5O4, negative material is artificial graphite, diaphragm
For 2400 types of Celgard.
(4) preparation-obtained lithium ion battery is subjected to charge-discharge test on blue electrical measurement test system.
Embodiment 1：
(1) boron-containing additive di-oxalate lithium borate (LiBOB) has good filming performance, not only can be in graphite cathode
One layer of SEI film is formed, layer protecting film can also be formed in positive electrode surface oxidation, prevented under esters electrolyte and high potential
Positive electrode contact aoxidized, slow down capacitance loss of the lithium ion battery in cyclic process.
(2) it is to test a small amount of boron-containing additive di-oxalate lithium borate (LiBOB) to being followed under the conditions of lithium ion battery high-voltage
The LiBOB that mass fraction is 1% is added in the conventional electrolysis liquid configured in comparative example and applied to just by the influence of ring performance
Pole material is nickel ion doped LiNi0.5Mn1.5O4, negative material is artificial graphite, and diaphragm is the high voltage of 2400 types of Celgard
Lithium ion battery.
(3) preparation-obtained lithium ion battery is subjected to charge-discharge test on blue electrical measurement test system.
Embodiment 2：
(1) two nitrile additive can be used to eliminate and generated in lithium ion battery cyclic process because it is with nucleophilic group-CN
HF, play the role of guard electrode, it can also be with PF in addition5It reacts and eliminates by-product PF5Inhibit esters solvent with this
Oxygenolysis film formation reaction, so as to improve the cycle performance of high-voltage lithium ion batteries.
(2) it is the influence for testing a small amount of two nitriles additive to cycle performance under the conditions of lithium ion battery high-voltage, by matter
The succinonitrile that amount score is 1% is added in the conventional electrolysis liquid configured in comparative example and is nickel ion doped applied to positive electrode
LiNi0.5Mn1.5O4, negative material is artificial graphite, and diaphragm is the high-voltage lithium ion batteries of 2400 types of Celgard.
(3) preparation-obtained lithium ion battery is subjected to charge-discharge test on blue electrical measurement test system.
Embodiment 3：
(1) it is the influence for testing different types of dintrile additive to cycle performance under the conditions of lithium ion battery high-voltage,
The adiponitrile that mass fraction is 1% is added in the conventional electrolysis liquid configured in comparative example and is nickel manganese applied to positive electrode
Sour lithium LiNi0.5Mn1.5O4, negative material is artificial graphite, and diaphragm is the high-voltage lithium ion batteries of 2400 types of Celgard.
(2) preparation-obtained lithium ion battery is subjected to charge-discharge test on blue electrical measurement test system.
Embodiment 4：
(1) it is the influence for testing different types of dintrile additive to cycle performance under the conditions of lithium ion battery high-voltage,
The hexamethylene dicyanide that mass fraction is 1% is added in the conventional electrolysis liquid configured in comparative example and is nickel manganese applied to positive electrode
Sour lithium LiNi0.5Mn1.5O4, negative material is artificial graphite, and diaphragm is the high-voltage lithium ion batteries of 2400 types of Celgard.
(2) preparation-obtained lithium ion battery is subjected to charge-discharge test on blue electrical measurement test system.
Embodiment 5：
(1) two nitrile additive can inhibit the oxygenolysis film formation reaction of esters solvent, LiBOB can be in positive electrode
Interface forms layer protecting film, and the two combined use can further improve cyclicity of the lithium ion battery under high voltage condition
Energy.
(2) it is test while two nitrile additives and LiBOB is added to cycle performance under the conditions of lithium ion battery high-voltage
Influence, the LiBOB that succinonitrile and mass fraction that mass fraction is 1% are 1% is added in comparative example jointly and is configured
It is nickel ion doped LiNi in conventional electrolysis liquid and applied to positive electrode0.5Mn1.5O4, negative material is artificial graphite, and diaphragm is
The high-voltage lithium ion batteries of 2400 types of Celgard.
(3) preparation-obtained lithium ion battery is subjected to charge-discharge test on blue electrical measurement test system.
Embodiment 6：
(1) it is the collocation using effect for testing variety classes dintrile additive and LiBOB, is oneself of 1% by mass fraction
The LiBOB that dintrile and mass fraction are 1% is added in the conventional electrolysis liquid configured in comparative example and jointly applied to positive material
Material is nickel ion doped LiNi0.5Mn1.5O4, negative material is artificial graphite, diaphragm be 2400 types of Celgard high voltage lithium from
Sub- battery.
(2) preparation-obtained lithium ion battery is subjected to charge-discharge test on blue electrical measurement test system.
Embodiment 7：
(1) be test variety classes dintrile additive and LiBOB collocation using effect, by mass fraction be 1% it is pungent
The LiBOB that dintrile and mass fraction are 1% is added in the conventional electrolysis liquid configured in comparative example and jointly applied to positive material
Material is nickel ion doped LiNi0.5Mn1.5O4, negative material is artificial graphite, diaphragm be 2400 types of Celgard high voltage lithium from
Sub- battery.
(2) preparation-obtained lithium ion battery is subjected to charge-discharge test on blue electrical measurement test system.
Charge-discharge test the specific steps are：A, with 0.1C rates constant-current charge to 5V, then constant-voltage charge is to by electricity
0.01C is flowed, blanking voltage 3.5V standing 5min are discharged to 0.1C again after standing 5min, are recycled 3 times with this；B, permanent with 1C rates
For current charge to 5V, then constant-voltage charge is discharged to blanking voltage 3.5V to by electric current 0.01C, standing after 5min with 1C again, quiet
5min is set, is recycled 150 times with this.Experimental results are as shown in table 1.
Claims (7)
1. a kind of electrolyte of high-voltage lithium ion batteries, including non-aqueous organic solvent, lithium salts and additive, it is characterised in that institute
It is esters solvent to state non-aqueous organic solvent, accounts for the 75-80% of electrolyte quality；Lithium salts is LiPF6；Additive adds for two nitriles
The mixture of agent and boron-containing additive accounts for electrolyte gross mass 1-5%.
2. high-voltage lithium-ion battery electrolyte according to claim 1, it is characterised in that：The two nitriles additive choosing
From one or more of malononitrile, succinonitrile, glutaronitrile, adiponitrile, pimelic dinitrile and hexamethylene dicyanide.
3. high-voltage lithium-ion battery electrolyte according to claim 1, it is characterised in that：The two nitriles additive is used
Amount accounts for the 1-3% of the electrolyte gross mass.
4. high-voltage lithium-ion battery electrolyte according to claim 1, it is characterised in that：The boron-containing additive is selected from
Di-oxalate lithium borate (LiBOB), difluorine oxalic acid boracic acid lithium (LiDFOB), tetramethyl borate (TMB), trimethylborate (TB) and
It is one or more of in three (trimethyl silane) borates (TMSB).
5. high-voltage lithium-ion battery electrolyte according to claim 1, it is characterised in that：The boron-containing additive dosage
Account for the 1-3% of the electrolyte gross mass.
6. high-voltage lithium-ion battery electrolyte according to claim 1, it is characterised in that：The LiPF6A concentration of 1.0-
1.5mol/L。
7. high-voltage lithium-ion battery electrolyte according to claim 1, it is characterised in that：The non-aqueous organic solvent choosing
From ethylene carbonate, propene carbonate, methyl ethyl carbonate, diethyl carbonate, dimethyl carbonate, ethyl acetate, propyl acetate, third
One or more of sour methyl esters and ethyl propionate.
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| CN201810461745.6A CN108666623A (en) | 2018-05-15 | 2018-05-15 | A kind of electrolyte of high-voltage lithium ion batteries |
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| CN201810461745.6A CN108666623A (en) | 2018-05-15 | 2018-05-15 | A kind of electrolyte of high-voltage lithium ion batteries |
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Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109346761A (en) * | 2018-10-18 | 2019-02-15 | 欣旺达电子股份有限公司 | Lithium ion battery, lithium-ion battery electrolytes and preparation method thereof |
| CN110380113A (en) * | 2019-08-02 | 2019-10-25 | 湖州昆仑动力电池材料有限公司 | Additive for high-voltage lithium ion battery electrolyte and application thereof |
| CN111384442A (en) * | 2018-12-29 | 2020-07-07 | 浙江省化工研究院有限公司 | Film forming additive for battery electrolyte anode, electrolyte using film forming additive and lithium ion battery |
| CN111697265A (en) * | 2020-05-15 | 2020-09-22 | 湖南博信新能源科技有限公司 | LNCM manganese ternary lithium ion battery electrolyte, lithium battery and preparation method thereof |
| CN111697186A (en) * | 2019-03-15 | 2020-09-22 | 深圳格林德能源集团有限公司 | High-energy-density lithium ion battery |
| CN111864267A (en) * | 2019-04-29 | 2020-10-30 | 中国科学院福建物质结构研究所 | Functional additive and electrolyte for high-temperature stabilization of lithium ion battery |
| CN112271331A (en) * | 2020-10-23 | 2021-01-26 | 常州大学 | High-voltage electrolyte of lithium ion battery and application thereof |
| WO2021047500A1 (en) * | 2019-09-10 | 2021-03-18 | 宁德时代新能源科技股份有限公司 | Electrolyte, and lithium ion battery, battery module, battery pack and device comprising same |
| CN113871698A (en) * | 2021-09-02 | 2021-12-31 | 蜂巢能源科技有限公司 | Electrolyte and lithium battery containing same |
| WO2022087830A1 (en) * | 2020-10-27 | 2022-05-05 | 宁德新能源科技有限公司 | Electrolyte and electrochemical device and electronic device comprising same |
| CN114597488A (en) * | 2020-12-04 | 2022-06-07 | 深圳新宙邦科技股份有限公司 | Non-aqueous electrolyte and lithium ion battery |
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| CN111384442A (en) * | 2018-12-29 | 2020-07-07 | 浙江省化工研究院有限公司 | Film forming additive for battery electrolyte anode, electrolyte using film forming additive and lithium ion battery |
| CN111384442B (en) * | 2018-12-29 | 2023-09-12 | 浙江省化工研究院有限公司 | Positive electrode film forming additive for battery electrolyte, electrolyte using additive and lithium ion battery |
| CN111697186A (en) * | 2019-03-15 | 2020-09-22 | 深圳格林德能源集团有限公司 | High-energy-density lithium ion battery |
| CN111864267B (en) * | 2019-04-29 | 2022-06-10 | 中国科学院福建物质结构研究所 | Functional additive and electrolyte for high-temperature stabilization of lithium ion battery |
| CN111864267A (en) * | 2019-04-29 | 2020-10-30 | 中国科学院福建物质结构研究所 | Functional additive and electrolyte for high-temperature stabilization of lithium ion battery |
| CN110380113A (en) * | 2019-08-02 | 2019-10-25 | 湖州昆仑动力电池材料有限公司 | Additive for high-voltage lithium ion battery electrolyte and application thereof |
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| CN111697265A (en) * | 2020-05-15 | 2020-09-22 | 湖南博信新能源科技有限公司 | LNCM manganese ternary lithium ion battery electrolyte, lithium battery and preparation method thereof |
| CN112271331A (en) * | 2020-10-23 | 2021-01-26 | 常州大学 | High-voltage electrolyte of lithium ion battery and application thereof |
| WO2022087830A1 (en) * | 2020-10-27 | 2022-05-05 | 宁德新能源科技有限公司 | Electrolyte and electrochemical device and electronic device comprising same |
| CN114597488A (en) * | 2020-12-04 | 2022-06-07 | 深圳新宙邦科技股份有限公司 | Non-aqueous electrolyte and lithium ion battery |
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Application publication date: 20181016 |