CN105914402A - Non-aqueous electrolyte and lithium ion battery - Google Patents
Non-aqueous electrolyte and lithium ion battery Download PDFInfo
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- CN105914402A CN105914402A CN201610515308.9A CN201610515308A CN105914402A CN 105914402 A CN105914402 A CN 105914402A CN 201610515308 A CN201610515308 A CN 201610515308A CN 105914402 A CN105914402 A CN 105914402A
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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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- 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 relates to a non-aqueous electrolyte. The non-aqueous electrolyte includes an organic solvent, electrolyte salt and additives. The additives include barbituric acid compounds. The barbituric acid compounds are used as functional additives; and thus, the cycle performance of the battery can be obviously improved.
Description
Technical field
The application relates to technical field of lithium batteries, is specifically related to a kind of nonaqueous electrolytic solution and lithium ion battery.
Background technology
Lithium ion battery, because having the advantages such as specific energy is high, have extended cycle life, self discharge is little, is widely used in consumer
Electronic product and energy storage with in electrokinetic cell.Along with the extensive application of lithium ion battery, it uses environment to tend to many most already
Planting various, the life requirements to battery is more and more higher.Such as, battery still has longer in the case of big multiplying power fast charging and discharging
Life-span, work long hours still without security risk etc. at high temperature.
The life-span of lithium ion battery is affected by factors, and wherein, nonaqueous electrolytic solution is as the weight of lithium ion battery
Want ingredient, it is had great impact.The dynamic performance of battery can be improved by nonaqueous electrolytic solution, reduce big times
Rate polarizes, and during circulation and high temperature storage, both positive and negative polarity interface stability thus reach improves life-span, the purpose of safety.
Summary of the invention
One of purpose of the application is to provide a kind of nonaqueous electrolytic solution.
The two of the purpose of itself parent are to provide a kind of lithium ion battery.
The concrete technical scheme of the application is:
The application relates to a kind of nonaqueous electrolytic solution, including organic solvent, electrolytic salt and additive, contains in described additive
There is barbiturates compounds.
Preferably, described barbiturates compounds is at least one in the compound shown in formula I selected from structural formula,
Wherein,
R11、R12It is each independently selected from substituted or unsubstituted C1~12Alkyl, substituted or unsubstituted C1~12Thiazolinyl, take
Generation or unsubstituted C6~26Aryl;
R13、R14It is each independently selected from hydrogen, amino, substituted or unsubstituted C1~12Alkyl, substituted or unsubstituted C1~12
Thiazolinyl, substituted or unsubstituted C6~26Aryl ,-NH-R ', wherein R ' is substituted or unsubstituted C1~12Alkyl amine group;
X is selected from O and S;
Substituent group is selected from halogen.
Preferably, wherein,
R11、R12It is each independently selected from substituted or unsubstituted C1~6Alkyl, substituted or unsubstituted phenyl;
R13、R14It is each independently selected from hydrogen, substituted or unsubstituted C1~6Alkyl, substituted or unsubstituted phenyl, amino.
Preferably, at least one in following compound of described barbiturates compounds,
Preferably, described barbiturates compounds weight/mass percentage composition in described nonaqueous electrolytic solution be 0.01%~
3%.
Preferably, described barbiturates compounds weight/mass percentage composition in described nonaqueous electrolytic solution be 0.05%~
2%.
Preferably, at least one during described organic solvent comprises cyclic carbonate, linear carbonate and carboxylate.
Preferably,
Described cyclic carbonate is in ethylene carbonate, Allyl carbonate, gamma-butyrolacton, fluorinated ethylene carbonate
At least one;
Described linear carbonate is selected from dimethyl carbonate, butylene, diethyl carbonate, dipropyl carbonate, carbonic acid first
At least one in ethyl ester, methyl propyl carbonate, ethyl propyl carbonic acid ester;
Described carboxylate selected from methyl formate, Ethyl formate, propyl formate, methyl acetate, ethyl acetate, propyl acetate,
At least one in methyl propionate, ethyl propionate, propyl propionate, methyl butyrate, ethyl n-butyrate..
Preferably, containing at least in nitrogen element, element sulphur, fluorine element, boron element, P elements in described electrolytic salt
Kind;Preferably, described electrolytic salt is selected from lithium hexafluoro phosphate LiPF6, double trifluoromethanesulfonimide lithium LiN (CF3SO2)2, double
(fluorine sulphonyl) imine lithium Li (N (SO2F)2), di-oxalate lithium borate LiB (C2O4)2, difluorine oxalic acid boracic acid lithium LiBF2(C2O4In)
At least one.
The application relates to a kind of lithium ion battery, including positive plate, negative plate, be arranged at intervals at positive plate and negative plate it
Between isolating membrane and electrolyte, described electrolyte is front arbitrary described nonaqueous electrolytic solution.
The technical scheme that the application provides can reach following beneficial effect:
Compared with prior art, the application by using barbiturates compounds as functional additive, can significantly change
Kind cycle performance of battery.
Detailed description of the invention
For making the purpose of the application, technical scheme and advantage clearer, below in conjunction with the embodiment of the present application, to this Shen
Technical scheme please is clearly and completely described, it is clear that described embodiment is some embodiments of the present application, and not
It it is whole embodiments.The technical scheme provided based on the application and given embodiment, those skilled in the art are not having
Make the every other embodiment obtained under creative work premise, broadly fall into the scope of the application protection.
The application relates to a kind of nonaqueous electrolytic solution, including organic solvent, electrolytic salt and additive;Described additive contains
There is barbiturates compounds.
Research shows, the oxidizing potential of barbiturates compounds is lower than solvent, can be poly-in the oxidation of battery core positive electrode surface
Close and form fine and close SEI film (CEI), effectively reduce the solvent decomposition at positive pole, to the performance of battery very
Useful;This is because the polymer that barbiturates compounds and lithium are formed cover positive electrode surface relative to lithium alkylide be more difficult to by
Solvent dissolves, and CEI is more stable.Can effectively stop positive electrode and nonaqueous electrolytic solution in positive electrode surface generation side reaction, and
Can effectively reduce the increase of positive pole interface impedance in cyclic process.After barbiturates compounds polymerization film formation, can prevent
Positive electrode such as the dissolution of Mn, Co, stop O release, thus stop O and nonaqueous electrolytic solution to occur to aoxidize aerogenesis and make battery swollen
Swollen.The product that barbiturates compounds is formed simultaneously will not at positive electrode surface containing the group covering that O, N etc. lead ionic nature good
Conduction to lithium ion impacts.Barbiturates compounds can improve battery core cyclicity well as electrolysis additive
Energy.
As a kind of improvement of the application nonaqueous electrolytic solution, the application barbiturates compounds is formula selected from structural formula
(1) at least one in the compound shown in,
Wherein,
R11、R12It is each independently selected from substituted or unsubstituted C1~12Alkyl, substituted or unsubstituted C1~12Thiazolinyl, take
Generation or unsubstituted C6~26Aryl;
R13、R14It is each independently selected from hydrogen, amino, substituted or unsubstituted C1~12Alkyl, substituted or unsubstituted C1~12
Thiazolinyl, substituted or unsubstituted C6~26Aryl ,-NH-R ', wherein R ' is substituted or unsubstituted C1~12Alkyl amine group;
X is selected from O and S;
Substituent group is selected from halogen, such as F, Cl.
As a kind of improvement of the application,
R11、R12It is each independently selected from substituted or unsubstituted C1~6Alkyl, substituted or unsubstituted C1~6Thiazolinyl, replacement
Or unsubstituted phenyl;
R13、R14It is each independently selected from hydrogen, substituted or unsubstituted C1~6Alkyl, substituted or unsubstituted C1~6Alkene
Base, substituted or unsubstituted phenyl, substituted or unsubstituted C1~6Aminoalkyl, amino, by C1~6The substituted imido of alkyl
Base.
As a kind of improvement of the application,
R11、R12It is each independently selected from substituted or unsubstituted C1~6Alkyl, substituted or unsubstituted phenyl;
R13、R14It is each independently selected from hydrogen, substituted or unsubstituted C1~6Alkyl, substituted or unsubstituted phenyl, amino.
As a kind of improvement of the application nonaqueous electrolytic solution, the application barbiturates compounds is in following compound
At least one, but be not limited to this:
As a kind of improvement of the application nonaqueous electrolytic solution, the application barbiturates compounds is selected from formula (I-1) to formula
At least one in (I-17) described compound, but it is not limited to this.As a kind of improvement of the application nonaqueous electrolytic solution, the application
Barbiturates compounds weight/mass percentage composition in nonaqueous electrolytic solution is 0.01%~3%.When barbiturates compounds
Content less than 0.01% time, it is impossible to form complete and effective CEI film at positive electrode surface, thus can not effectively stop non-water power
Solve the side reaction caused by electron transfer between liquid and electrode;And when barbiturates kind compound content is more than 3%, meeting exists
Cathode surface forms thicker CEI film, causes lithium ion mobility resistance to increase, is unfavorable for the positive pole interface of battery in cyclic process
Stability.
It is further preferred that the weight/mass percentage composition scope that the application barbiturates compounds is in nonaqueous electrolytic solution
The upper limit optionally from 3%, 2.8%, 2.5%, 2.0%, 1.5%, 1.0%, lower limit optionally from 0.01%, 0.02%, 0.03%,
0.05%, 0.1%, 0.3%, 0.5%, 0.6%, 0.8%.It is further preferred that described barbiturates compounds is non-
Percentage composition in water electrolysis liquid is 0.05%~2%.
Preferably, the application barbiturates compounds weight/mass percentage composition in nonaqueous electrolytic solution is 1%.
As a kind of improvement of the application nonaqueous electrolytic solution, the application organic solvent comprises cyclic carbonate, chain carbonic acid
At least one in ester and carboxylate;Wherein,
Cyclic carbonate is selected from ethylene carbonate (EC), Allyl carbonate (PC), gamma-butyrolacton, fluorinated ethylene carbonate
In at least one;
Linear carbonate selected from dimethyl carbonate (DMC), butylene, diethyl carbonate (DEC), dipropyl carbonate,
At least one in Ethyl methyl carbonate (EMC), methyl propyl carbonate, ethyl propyl carbonic acid ester;
Carboxylate selected from methyl formate, Ethyl formate, propyl formate, methyl acetate, ethyl acetate (EA), propyl acetate,
At least one in methyl propionate, ethyl propionate, propyl propionate (PP), methyl butyrate, ethyl n-butyrate..
As a kind of improvement of the application nonaqueous electrolytic solution, the application electrolytic salt is in organic lithium salt or inorganic lithium salt
At least one.
As a kind of improvement of the application nonaqueous electrolytic solution, containing nitrogen element, element sulphur, fluorine unit in the application electrolytic salt
At least one in element, boron element, P elements.
As a kind of improvement of the application nonaqueous electrolytic solution, the application electrolytic salt is selected from lithium hexafluoro phosphate LiPF6, double three
Fluoromethane sulfimide lithium LiN (CF3SO2)2(being abbreviated as LiTFSI), double (fluorine sulphonyl) imine lithium Li (N (SO2F)2) (be abbreviated as
LiFSI), di-oxalate lithium borate LiB (C2O4)2(being abbreviated as LiBOB), difluorine oxalic acid boracic acid lithium LiBF2(C2O4) (be abbreviated as
LiDFOB) at least one in.
The application further relates to a kind of lithium ion battery, including positive plate, negative plate, is arranged at intervals at positive plate and negative plate
Between isolating membrane and electrolyte;Described electrolyte is the nonaqueous electrolytic solution described in aforementioned any one.
Present invention also provides a kind of lithium ion battery, including positive plate, negative plate, be arranged at intervals at positive plate and negative pole
Isolating membrane, electrolyte and package foil between sheet;Described positive plate includes plus plate current-collecting body and is coated on plus plate current-collecting body
Positive pole diaphragm, negative plate includes negative current collector and the cathode membrane being coated on negative current collector;Described electrolyte is front
State the nonaqueous electrolytic solution described in any one.
As a kind of improvement of the application lithium ion battery, the application positive pole diaphragm includes positive electrode active materials, binding agent
And conductive agent.
As a kind of improvement of the application lithium ion battery, the application positive electrode active materials is optionally from cobalt acid lithium LiCoO2、
At least one in lithium-nickel-manganese-cobalt ternary material, LiFePO4, LiMn2O4.
As a kind of improvement of the application lithium ion battery, the application positive electrode active materials is cobalt acid lithium and lithium-nickel-manganese-cobalt three
The mixture of unit's material.
As a kind of improvement of the application lithium ion battery, the application cathode membrane includes negative active core-shell material, binding agent
And conductive agent.
As a kind of improvement of the application lithium ion battery, the application negative active core-shell material is graphite and/or silicon.
Below by way of specific embodiment the technical scheme of the application done exemplary description:
The preparation of electrolyte: < in the argon gas atmosphere glove box of 10ppm, preparation mixes nonaqueous solvent, then will fill in water content
Divide the lithium salts LiPF being dried6It is dissolved in above-mentioned nonaqueous solvent, is made into LiPF6Concentration is the basic electrolyte of 1mol/L.
Composition and the mass ratio of mixing nonaqueous solvent are as shown in table 1.And according to shown in table 1, add in basic electrolyte
Barbiturates compounds additive.
Example as barbiturates compounds is: 1,3-dimethyl barbituric acid (B1, as shown in formula I-1), 1,3-
Dibutyl barbiturates (B2, as shown in formula I-4), 1,3-diphenyl barbituric acid (B3, as shown in formula I-5), 1,3-dimethyl-
2-thiobarbituricacidα-(B4, as shown in formula I-11), (B5, such as formula I-8 institute for 1,3-dimethyl-5-amino-2-thiobarbituricacidα-
Show).
The preparation of lithium ion battery:
1) preparation of positive plate: (molecular formula is LiCoO by positive active material cobalt acid lithium2), conductive agent acetylene black, bonding
Agent polyvinylidene fluoride (being abbreviated as PVDF) 96:2:2 by weight is at appropriate N-Methyl pyrrolidone (being abbreviated as NMP) solvent
In be thoroughly mixed so that it is form uniform anode sizing agent;This slurry is coated on plus plate current-collecting body Al paper tinsel, dry, cold
Pressure, obtains positive plate.
2) preparation of negative plate: negative electrode active material graphite, conductive agent acetylene black, binding agent butadiene-styrene rubber (are abbreviated as
SBR), thickening agent sodium carboxymethyl cellulose (being abbreviated as CMC) according to weight ratio 95:2:2:1 in appropriate deionized water solvent
It is thoroughly mixed so that it is form uniform cathode size;This slurry is coated on negative current collector Cu paper tinsel, dries, colds pressing,
Obtain negative plate.
3) isolating membrane: using PE porous polymer film as isolating membrane.
4) preparation of lithium ion battery: positive plate, isolating membrane, negative plate are folded in order, makes isolating membrane be in positive pole
Playing the effect of isolation between sheet and negative plate, then winding obtains naked battery core;Naked battery core is placed in outer package paper tinsel, by above-mentioned
The electrolyte prepared is injected in dried battery, through Vacuum Package, stand, be melted into, the operation such as shaping, i.e. complete lithium
The preparation of ion battery.
Embodiment 1~14 and the electrolyte of comparative example 1~4 and lithium ion battery is prepared according to above-mentioned preparation method;Electricity
Solving the parameter of additive and organic solvent in liquid and arrange as shown in table 1, the percentage numerical value in table 1 refers to account for the total matter of electrolyte
The percentage of amount.
Table 1 embodiment 1~14 and the electrolyte component parameter list of comparative example 1~4
Hereinafter the lithium ion battery prepared by experiment comparative example each to the application and embodiment is carried out performance test.
Loop test
The lithium ion battery prepared is carried out respectively following test:
At 45 DEG C, by lithium ion battery, with 1C constant-current charge to 4.4V, then constant-voltage charge to electric current is 0.05C, then
With 1C constant-current discharge to 3.0V, now for circulate first, carry out so repeatedly cycle charging/electric discharge according to above-mentioned condition, respectively
Calculate lithium ion battery and circulate 50 times, 100 times, capability retention after 300 times.Often organize each 5 batteries, wherein, circulation
After capability retention calculate according to the following formula.Electrolyte selected in each lithium ion battery and the correlative measurement obtained
Examination data see table 2.
Capability retention after circulation=(discharge capacity of corresponding circulation/circulate first discharge capacity) × 100%, follows
The result of ring test is as shown in table 2.
Table 2 embodiment 1~14 and comparative example 1~4 lithium ion battery circulation after capability retention
In conjunction with in Tables 1 and 2 it can be seen that compared with comparative example 1, the electrolyte of embodiment 1-8 adds barbiturates
Compounds all can improve the cycle performance of lithium ion battery.Because barbiturates compounds is permissible during initial charge
Generate SEI film, can effectively stop the PC impact on anode.Compared with comparative example 2, the electrolyte of embodiment 9-14 adds 1%
During barbiturates compounds, the cycle performance of lithium ion battery the most all has improvement.In embodiment 9~13, electrolyte adds
Enter that mass fraction is 1% 1,3-dimethyl barbituric acid, 1,3-dibutyl barbiturates, 1,3-diphenyl barbituric acid, 1,
3-dimethyl-2-thiobarbituricacidα-and 1, during 3-dimethyl-5-amino-2-thiobarbituricacidα-, the cycle performance of battery shows
Write and promote.
The application other embodiments:
Prepare electrolyte and the lithium battery of embodiment 15~31 according to the method for previous embodiment, difference is: electrolyte
Middle additive component and adding proportion are as shown in table 3:
Table 3 embodiment 15~31 battery electrolyte additive component and adding proportion
Detecting according to the performance of the method for the previous embodiment battery to preparing, detection obtains embodiment battery
The performance of 15~31 is similar to above example, repeats no more as space is limited.
Although the application is open as above with preferred embodiment, but is not for limiting claim, any this area skill
Art personnel, on the premise of conceiving without departing from the application, can make some possible variations and amendment, therefore the application
Protection domain should be defined in the range of standard with the application claim.
Claims (10)
1. a nonaqueous electrolytic solution, including organic solvent, electrolytic salt and additive, it is characterised in that contain in described additive
There is barbiturates compounds.
Nonaqueous electrolytic solution the most according to claim 1, it is characterised in that described barbiturates compounds is selected from structural formula
For at least one in the compound shown in formula I,
Wherein,
R11、R12It is each independently selected from substituted or unsubstituted C1~12Alkyl, substituted or unsubstituted C1~12Thiazolinyl, replacement or not
Substituted C6~26Aryl;
R13、R14It is each independently selected from hydrogen, amino, substituted or unsubstituted C1~12Alkyl, substituted or unsubstituted C1~12Thiazolinyl,
Substituted or unsubstituted C6~26Aryl ,-NH-R ', wherein R ' is substituted or unsubstituted C1~12Alkyl amine group;
X is selected from O and S;
Substituent group is selected from halogen.
Nonaqueous electrolytic solution the most according to claim 2, it is characterised in that wherein,
R11、R12It is each independently selected from substituted or unsubstituted C1~6Alkyl, substituted or unsubstituted phenyl;
R13、R14It is each independently selected from hydrogen, substituted or unsubstituted C1~6Alkyl, substituted or unsubstituted phenyl, amino.
Nonaqueous electrolytic solution the most according to claim 3, it is characterised in that described barbiturates compounds is selected from followingization
At least one in compound,
Nonaqueous electrolytic solution the most according to claim 1, it is characterised in that described barbiturates compounds is described non-aqueous
Weight/mass percentage composition in electrolyte is 0.01%~3%.
Nonaqueous electrolytic solution the most according to claim 5, it is characterised in that described barbiturates compounds is described non-aqueous
Weight/mass percentage composition in electrolyte is 0.05%~2%.
Nonaqueous electrolytic solution the most according to claim 1, it is characterised in that described organic solvent comprises cyclic carbonate, chain
At least one in shape carbonic ester and carboxylate.
Nonaqueous electrolytic solution the most according to claim 7, it is characterised in that
Described cyclic carbonate is selected from ethylene carbonate, Allyl carbonate, gamma-butyrolacton, fluorinated ethylene carbonate at least
A kind of;
Described linear carbonate selected from dimethyl carbonate, butylene, diethyl carbonate, dipropyl carbonate, Ethyl methyl carbonate,
At least one in methyl propyl carbonate, ethyl propyl carbonic acid ester;
Described carboxylate is selected from methyl formate, Ethyl formate, propyl formate, methyl acetate, ethyl acetate, propyl acetate, propanoic acid
At least one in methyl ester, ethyl propionate, propyl propionate, methyl butyrate, ethyl n-butyrate..
Nonaqueous electrolytic solution the most according to claim 1, it is characterised in that containing nitrogen element, sulfur unit in described electrolytic salt
At least one in element, fluorine element, boron element, P elements;Preferably, described electrolytic salt is selected from lithium hexafluoro phosphate LiPF6, double
Trifluoromethanesulfonimide lithium LiN (CF3SO2)2, double (fluorine sulphonyl) imine lithium Li (N (SO2F)2), di-oxalate lithium borate LiB
(C2O4)2, difluorine oxalic acid boracic acid lithium LiBF2(C2O4At least one in).
10. a lithium ion battery, including positive plate, negative plate, the isolating membrane being arranged at intervals between positive plate and negative plate,
And electrolyte, it is characterised in that described electrolyte is the arbitrary described nonaqueous electrolytic solution of claim 1~9.
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CN113614967A (en) * | 2019-03-29 | 2021-11-05 | 松下知识产权经营株式会社 | Nonaqueous electrolyte secondary battery |
CN110994021A (en) * | 2019-11-19 | 2020-04-10 | 惠州市豪鹏科技有限公司 | Electrolyte additive, electrolyte and lithium ion battery |
CN111477961A (en) * | 2020-05-29 | 2020-07-31 | 珠海市赛纬电子材料股份有限公司 | Non-aqueous electrolyte of lithium ion battery and lithium ion battery containing non-aqueous electrolyte |
CN112201855A (en) * | 2020-10-19 | 2021-01-08 | 宁德新能源科技有限公司 | Electrolyte solution, electrochemical device, and electronic device |
CN112201855B (en) * | 2020-10-19 | 2022-04-01 | 宁德新能源科技有限公司 | Electrolyte solution, electrochemical device, and electronic device |
CN114430068A (en) * | 2020-10-29 | 2022-05-03 | 深圳市研一新材料有限责任公司 | Lithium ion battery electrolyte |
CN114430068B (en) * | 2020-10-29 | 2024-01-23 | 深圳市研一新材料有限责任公司 | Lithium ion battery electrolyte |
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