CN105428701A - Electrolyte and lithium ion battery comprising same - Google Patents
Electrolyte and lithium ion battery comprising same Download PDFInfo
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- CN105428701A CN105428701A CN201510973386.9A CN201510973386A CN105428701A CN 105428701 A CN105428701 A CN 105428701A CN 201510973386 A CN201510973386 A CN 201510973386A CN 105428701 A CN105428701 A CN 105428701A
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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
Abstract
The invention relates to the technical field of lithium ion batteries, particularly relates to electrolyte and a lithium ion battery comprising the same. The electrolyte disclosed by the invention comprises lithium salt, an organic solvent and an additive A, wherein the additive A comprises silane compounds containing cyano groups and dinitrile compounds containing ether bonds; the additive A can be used for improving the rate capability and low-temperature discharge performance of the battery under a high voltage, thereby improving the service life of the lithium ion battery. The electrolyte disclosed by the invention further comprises an additive B which is one or more of ether compounds, nitrile compounds, cyclic ester compounds containing S=O double bonds, cyclic carbonate compounds containing C-C unsaturated bonds and compounds containing imido groups. The lithium ion battery comprising the electrolyte can achieve the objective of high voltage and the highest normal working voltage can be improved to 4.4V-5.0V; in addition, the cycle performance of the lithium ion battery is excellent and the capacity retention ratios during charging and discharging can be both high.
Description
Technical field
The present invention relates to technical field of lithium ion, specifically, relate to a kind of electrolyte and comprise the lithium ion battery of this electrolyte.
Background technology
In recent years, along with the fast development of smart electronics product, the flying power of lithium ion battery is had higher requirement.In order to improve the energy density of lithium ion battery, exploitation high-voltage lithium ion batteries is one of effective ways.
At present, operating voltage has become the focus of numerous R&D institution and business research at the lithium ion battery of more than 4.4V.But under high voltages, the oxidation activity of positive electrode raises, stability declines, and causes nonaqueous electrolytic solution easily at positive electrode surface generation electrochemical oxidation reactions, and then decompose generation gas.Meanwhile, the transition metal in positive electrode active materials, can there is reduction reaction and stripping in such as nickel, cobalt, manganese etc., thus cause lithium ion battery chemical property to worsen further.Solution main at present adds film for additive in electrolyte.These additives can in positive pole film forming, but can cause interface impedance to increase, and cause lithium ion mobility kinetics of diffusion performance in battery to reduce, and then make multiplying power and the cycle performance decay of battery.Prior art discloses the silicon nitrile compounds of a class containing low polyoxyethylene units as electrolysis additive or cosolvent, develop have that oxidation resistance is strong, dielectric constant is large, the electrolyte material of thermal safety advantages of higher, although this compounds can form SEI film at graphite surface, stop PC to the destruction of graphite electrode, but containing oligo-ether chain in its structure, in cell reaction, ether chain easily disconnects, affect the stability of SEI film, thus cause battery to reduce.
Therefore, a kind of electrolyte that lithium ion battery still can be made under high voltages to keep cycle performance, multiplying power and low temperature performance excellent of necessary exploitation.
Summary of the invention
In order to solve the problem, the applicant has carried out studying with keen determination, found that: comprise the silane compound containing cyano group and there is the electrolyte of dinitrile compound of ehter bond, be applied to after in lithium ion battery, battery high rate performance under high voltages and low temperature performance can be improved, improve the useful life of lithium ion battery, thus complete the application.
The object of the application is to provide a kind of electrolyte, comprises lithium salts, organic solvent, additive, and wherein, described additive A comprises the silane compound containing cyano group and has the dinitrile compound of ehter bond;
The described silane compound structural formula containing cyano group is such as formula shown in I:
Wherein, R
1, R
2, R
3be selected from cyano group, halogen, C independently of one another
1 ~ 10alkyl, C
1 ~ 10alkoxyl, described halogen are selected from F, Cl, Br; N is selected from the integer of 0 ~ 5.
The described dinitrile compound structural formula with ehter bond is such as formula shown in II:
Wherein, R
4, R
5, R
6independently of one another for be selected from carbon number be 1 ~ 5 alkylidene, carbon number be the alkenylene of 2 ~ 5, m is the integer of 1 ~ 5.
Also containing additive B in described electrolyte, described additive B be selected from ether compound, nitrile compound, the cyclic ester compounds containing sulfur-to-oxygen double bond, the cyclic carbonate compound containing carbon-to-carbon unsaturated bond, containing one or more in the compound of imido grpup.
Another object of the application is to provide a kind of lithium ion battery, the electrolyte comprise the positive plate containing positive electrode active materials, providing containing negative active core-shell material negative plate, lithium battery diaphragm and the application.
Electrolysis of the present invention comprises lithium salts, organic solvent and additive A, additive A comprises the silane compound containing cyano group and has the dinitrile compound of ehter bond, additive A can improve battery high rate performance under high voltages and low temperature performance, improves the useful life of lithium ion battery.Also containing additive B in electrolyte of the present invention, additive B is selected from ether compound, nitrile compound, the cyclic ester compounds containing sulfur-to-oxygen double bond, the cyclic carbonate compound containing carbon-to-carbon unsaturated bond, containing one or more in the compound of imido grpup, additive B can improve the cycle performance of lithium ion battery further.Adopt the lithium ion battery of electrolyte of the present invention can realize high-tension target, the highest normal working voltage can bring up to 4.4V ~ 5.0V and the cycle performance of lithium ion battery is good, and discharge and recharge all has higher capability retention.
Embodiment
Be described in detail below by the application, the feature of the application and advantage will illustrate along with these and become more clear, clear and definite.
The present invention proposes a kind of electrolyte, comprise lithium salts, organic solvent and additive A.Described additive A comprises the silane compound containing cyano group and has the dinitrile compound of ehter bond;
In above-mentioned electrolyte, the described silane compound structural formula containing cyano group is such as formula shown in I:
Wherein, R
1, R
2, R
3be selected from cyano group, halogen, C independently of one another
1 ~ 10alkyl, C
1 ~ 10alkoxyl, described halogen are selected from F, Cl, Br; N is selected from the integer of 0 ~ 5.
Preferably, R
1, R
2, R
3in have one at least for cyano group.
Preferably, R
1, R
2, R
3in have a C at least
1 ~ 6alkoxyl.
The preferred upper limit value of the carbon number of abovementioned alkyl is once 8,6,4,3; Such as, when the higher limit of carbon number is 8, the carbon atom number range of alkyl refers to 1 ~ 8; The most preferably carbon number of alkyl is 1 ~ 6, and further preferably 1 ~ 3.Alkyl can be alkyl group or cycloalkyl: alkyl group comprises straight chained alkyl and the alkyl with side chain; Cycloalkyl is the saturated alkyl containing alicyclic structure, alicyclic ring can contain or do not contain substituting group.
Wherein, C
1-6straight or branched alkyl include but not limited to :-CH
3,-CH
2cH
3,-(CH
2)
2cH
3,-CH (CH
3)
2,-(CH
2)
3cH
3,-CH
2cH (CH
3)
2,-CH (CH
3) CH
2cH
3,-CH
2cH (CH
3)
2,-C (CH
3)
3,-(CH
2)
4cH
3,-CH
2cH
2cH (CH
3)
2,-CH (CH
3) CH
2cH
2cH
3,-CH
2cH (CH
3) CH
2cH
3,-CH
2c (CH
3)
3,-(CH
2)
5cH
3;
C
1 ~ 6alkoxyl includes but not limited to :-OCH
3,-OCH
2cH
3,-O (CH
2)
2cH
3,-OCH (CH
3)
2,-O (CH
2)
3cH
3,-OCH
2cH (CH
3)
2,-OCH (CH
3) CH
2cH
3,-OCH
2cH (CH
3)
2,-OC (CH
3)
3,-O (CH
2)
4cH
3,-OCH
2cH
2cH (CH
3)
2,-OCH (CH
3) CH
2cH
2cH
3,-OCH
2cH (CH
3) CH
2cH
3,-OCH
2c (CH
3)
3,-O (CH
2)
5cH
3.
As the example of the silane compound containing cyano group, specifically see following structural formula:
trimethylsilyl cyanide (AS1);
2-cyano ethyl methyl two silicon fluoride (AS2);
dicyano dimethylsilane (AS3);
2-cyano ethyl triethoxysilane (AS4).
The described dinitrile compound structural formula with ehter bond is such as formula shown in II:
Wherein, R
4, R
5, R
6independently of one another for being selected from C
1 ~ 5alkylidene, C
2 ~ 5alkenylene, m is the integer of 1 ~ 5; More preferably C
1 ~ 4alkylidene, m is 1 or 2.
Preferably, the described dinitrile compound with ehter bond is selected from least one in following material: 3, 5-dioxa-pimelic dinitrile (AM1), 1, 4-bis-(cyanoethoxy) butane (AM2), ethylene glycol bisthioglycolate (2-cyano ethyl) ether (AM3), diethylene glycol two (2-cyano ethyl) ether, triethylene glycol two (2-cyano ethyl) ether, TEG two (2-cyano ethyl) ether, 1, 3-bis-(2-cyanoethoxy) propane (AM4), 1, 4-bis-(2-cyanoethoxy) butane, 1, 5-bis-(2-cyanoethoxy) pentane and ethylene glycol bisthioglycolate (4-cyanobutyl) ether.Preferably, the dinitrile compound described in ehter bond is ethylene glycol bisthioglycolate (2-cyano ethyl) ether.
As the example of dinitrile compound with ehter bond, specifically see following structural formula:
3,5-dioxa-pimelic dinitrile (AM1)
Isosorbide-5-Nitrae-two (cyanoethoxy) butane (AM2)
Ethylene glycol bisthioglycolate (2-cyano ethyl) ether (AM3)
1,3-bis-(2-cyanoethoxy) propane (AM4)
Find after deliberation, comprise the silane compound containing cyano group due to electrolyte of the present invention and there is the dinitrile compound of ehter bond, silane compound containing cyano group preferentially forms diaphragm on positive active material surface, owing to there is a large amount of intermolecular hydrogen bonding effects between itself and the dinitrile compound with ehter bond, make the silane compound containing cyano group can not film forming blocked up, and the dinitrile compound with ehter bond also has stronger chelation with positive active material surface, the dinitrile compound therefore with ehter bond can slow down film-forming region film forming on the one hand, non-film-forming region film forming can be promoted again on the other hand.Due to good synergy between the two, the composite S EI film formed is fine and close, even, and impedance is little, is applied to after in lithium ion battery by this electrolyte, battery high rate performance under high voltages and low temperature performance can be improved, improve the useful life of lithium ion battery.
In containing in the silane compound of cyano group shown in above-mentioned formula I, when R contains at least two cyano group, the high rate performance of lithium ion battery, low temperature performance and cycle performance can be improved further.
In the present invention, the described silane compound containing cyano group can obtain according to the synthetic method of routine, such as, can, see CN201480003489.6, also can pass through commercially available; The dinitrile compound with ehter bond obtains by existing synthetic method, can see CN201280006888.9, and can pass through commercially available, its source is not subject to concrete restriction yet.
In above-mentioned electrolyte, preferably, the silane compound containing cyano group is 0.01% ~ 10% of the total weight of electrolyte with the total content of the dinitrile compound combined additive with ehter bond.Find after deliberation, when this combined additive content in the electrolytic solution lower than 0.01% time, electrolyte can not form stable passivating film effectively, and the cryogenic property of lithium ion battery and high rate performance can not get improving substantially; When the content of this combined additive is more than 10%, the film formed is thicker, and impedance increases, and reduces the cycle performance of lithium ion battery.Further preferably, the total content of this combined additive is 1 ~ 8% of the total weight of electrolyte.Wherein, in combined additive, the silane compound containing cyano group is unrestricted with the content ratio of the dinitrile compound with ehter bond.
Preferred further, additive also comprises additive B, additive B be selected from ether compound, nitrile compound, the cyclic ester compounds containing sulfur-to-oxygen double bond, the cyclic carbonate compound containing carbon-to-carbon unsaturated bond, containing one or more in the compound of imido grpup.
Ether compound is selected from least one in substituted or unsubstituted ether, and substituting group is halogen atom, is preferably fluorine; As the object lesson of ether compound, can enumerate: 1-ethyoxyl-propane (EPE), 2-trifluoromethyl-3-methoxyl group perflenapent (TMMP), 1,1,2,2-tetra-fluoro ethyl-2', 2', 3', 3'-tetrafluoro propyl ether (F-EPE).In above-mentioned electrolyte, preferably, the content of ether compound is 0.01 ~ 5% of the total weight of electrolyte, and further preferably, the content of ether compound is 0.1 ~ 3% of the total weight of electrolyte.
Nitrile compound be selected from mono-nitrile compound, two nitrile compound, three nitrile compounds and four nitrile compounds one or more, described nitrile compound also comprises the nitrile containing unsaturated carbon-carbon double bond; The number of the cyano group in nitrile compound can be 1,2,3,4 or 5, the mono-nitrile compound such as only containing a cyano group, the two nitrile compounds containing two cyano group, three nitrile compounds containing three cyano group, four nitrile compounds containing four cyano group.
As the object lesson of nitrile compound, can enumerate: acetonitrile, propionitrile, butyronitrile, isobutyronitrile, valeronitrile, isobutyl cyanide, 2-methylbutyronitrile, trimethylacetonitrile, own nitrile, ring valeronitrile, cyclohexanenitrile, acrylonitrile, methacrylonitrile, butene nitrile, 3-methyl butene nitrile, 2-methyl-2-butene nitrile, 2-allyl acetonitrile, 2-methyl-2-allyl acetonitrile, 3-methyl-2-allyl acetonitrile, 2-hexene nitrile, fluoride acetonitrile, two fluoride acetonitriles, trifluoro acetonitrile, 2-fluorine propionitrile, 3-fluorine propionitrile, 2, 2-difluoro propionitrile, 2, 3-difluoro propionitrile, 3, 3-difluoro propionitrile, 2, 2, 3-trifluoro propionitrile, 3, 3, 3-trifluoro propionitrile, the mono-nitrile compound such as five fluorine propionitrile, two nitrile compound such as malononitrile, succinonitrile, 2-methyl succinonitrile, tetramethyl succinonitrile, glutaronitrile, 2-methyl cellosolve acetate glutaronitrile, adiponitrile, rich horse dintrile, 2-methylene glutaronitrile, three nitrile compounds such as 1,3,5-penta trimethylsilyl nitrile, 1,2,3-third trimethylsilyl nitrile, 1,3,6-hexane three nitrile, TCNE etc. four nitrile compound etc.Wherein, preferred: acetonitrile, propionitrile, butyronitrile, valeronitrile, butene nitrile, 3-methyl butene nitrile, malononitrile, succinonitrile, glutaronitrile, adiponitrile (ADN), rich horse dintrile, more preferably malononitrile, succinonitrile, glutaronitrile, adiponitrile, rich horse dintrile, 1,3,6-hexane three nitrile etc.In above-mentioned electrolyte, preferably, the content containing nitrile compounds is 0.01 ~ 5% of the total weight of electrolyte, and further preferably, the content containing nitrile compounds is 0.1 ~ 3% of the total weight of electrolyte.
Cyclic ester compounds containing sulfur-to-oxygen double bond can be cyclic sulfates, cyclic sulfite, saturated sultone, unsaturated sultone containing carbon-to-carbon double bond.Such as sulfuric acid vinyl ester, sulfuric acid propylene, propylene sulfite, PS (PS), Isosorbide-5-Nitrae-butyl sultone, propenyl-1,3-sulfonic acid lactone.In above-mentioned electrolyte, preferably, the content of the cyclic ester compounds containing sulfur-to-oxygen double bond is 0.01 ~ 5% of the total weight of electrolyte, and further preferably, the content of the cyclic ester compounds containing sulfur-to-oxygen double bond is 0.1 ~ 3% of the total weight of electrolyte.
Containing in the cyclic carbonate compound of carbon-to-carbon unsaturated bond, described carbon-to-carbon unsaturated bond is preferably double bond, and described double bond can be positioned on ring, also can not be positioned on ring.Preferably, cyclic carbonate compound containing carbon-to-carbon unsaturated bond be selected from vinylene carbonate (VC), fluorinated ethylene carbonate, fluoro vinylene carbonate, 1,2-bis-fluoro vinylene carbonate, vinylethylene carbonate one or more.In above-mentioned electrolyte, preferably, the content of the cyclic carbonate compound containing carbon-to-carbon unsaturated bond is 0.01 ~ 5% of the total weight of electrolyte, and further preferably, the content of the described cyclic carbonate compounds containing carbon-to-carbon unsaturated bond is 0.1 ~ 3% of the total weight of electrolyte.
Compound containing imido grpup be selected from the compound containing imine group, carbodiimide groups one or more.Described imine group is expressed as
described carbodiimide groups is expressed as-N=C=N-, such as: dicyclohexylcarbodiimide (DCC); In above-mentioned electrolyte, preferably, the content of the described compound containing imido grpup is 0.01 ~ 5% of the total weight of electrolyte, and further preferably, the content of the described compound containing imido grpup is 0.1 ~ 3% of the total weight of electrolyte.
When also including additive B in additive, further can improve the cycle performance of lithium ion battery, such as under the high pressure of more than 4.45V through repeatedly circulation after, lithium ion battery is made to have higher capability retention further, in addition, the discharge performance under lithium ion battery multiplying power and low temperature can also be improved further.
In above-mentioned electrolyte, especially, organic solvent selects non-aqueous organic solvent, preferably, carbon number can be selected to be 1 ~ 8 and containing the compound of at least one ester group as non-aqueous organic solvent.
Preferably, described organic solvent is be selected from least one in ethylene carbonate, propene carbonate, butylene, fluorinated ethylene carbonate, dimethyl carbonate, diethyl carbonate, dipropyl carbonate, methyl ethyl carbonate, methyl propyl carbonate, ethyl propyl carbonic acid ester, GBL, methyl propionate, methyl butyrate, ethyl acetate, ethyl propionate and ethyl butyrate.Certainly being not limited only to above-mentioned mentioned concrete compound, also can be the halogenated compound of above-mentioned concrete compound.
In above-mentioned electrolyte, at least one of described lithium salts optionally in organic lithium salt or inorganic lithium salt.Especially, at least one in fluorine element, boron element, P elements is contained in described lithium salts.
As the example of lithium salts, specifically can enumerate: lithium hexafluoro phosphate LiPF
6, difluorophosphate LiPO
2f
2, LiBF4 LiBF
4, two trifluoromethanesulfonimide lithium LiN (CF
3sO
2)
2(being abbreviated as LiTFSI), two (fluorine sulphonyl) imine lithium Li (N (SO
2f)
2) (being abbreviated as LiFSI), di-oxalate lithium borate LiB (C
2o
4)
2(being abbreviated as LiBOB), difluorine oxalic acid boracic acid lithium LiBF
2(C
2o
4) (being abbreviated as LiDFOB).
In above-mentioned electrolyte, preferably, lithium salts can be selected from least one in lithium hexafluoro phosphate, difluorophosphate, LiBF4, hexafluoroarsenate lithium, lithium perchlorate, trifluoro sulphonyl lithium, two (trimethyl fluoride sulfonyl) imine lithium, two (fluorine sulphonyl) imine lithium and three (trimethyl fluoride sulfonyl) lithium methide.
Especially, the concentration of lithium salts can be 0.5mol/L ~ 3mol/L.
In the present invention, electrolyte adopts conventional method to prepare, such as by each mixing of materials in electrolyte evenly.
Another object of the present invention is to provide a kind of lithium ion battery, comprise positive plate, negative plate, lithium battery diaphragm and electrolyte, wherein, electrolyte is electrolyte of the present invention.
In above-mentioned lithium ion battery, positive plate comprises positive electrode active materials; Described negative plate comprises negative active core-shell material, and wherein, the concrete kind of positive electrode active materials, negative active core-shell material is not all subject to concrete restriction, can select according to demand.
Preferably, positive electrode active materials is for being selected from cobalt acid lithium (LiCoO
2), lithium-nickel-manganese-cobalt ternary material, LiFePO 4 (LiFePO
4), LiMn2O4 (LiMn
2o
4) at least one.
Preferably, negative active core-shell material is graphite and/or silicon, such as native graphite, Delanium, mesophase spherule micro-carbon ball (referred to as MCMB), hard carbon, soft carbon, silicon, silico-carbo compound, Li-Sn alloy, Li-Sn-O alloy, Sn, SnO, SnO
2, spinel structure lithiumation TiO
2-Li
4ti
5o
12, Li-Al alloy all can be used as negative active core-shell material.
Beneficial effect of the present invention is as follows:
Silane compound containing cyano group and the dinitrile compound with ehter bond combinationally use by lithium-ion battery electrolytes of the present invention, thickness and the impedance of positive electrode surface SEI film can be reduced, improve homogeneity and stability that positive electrode surface forms SEI film, thus improve high rate performance and the low temperature performance of lithium ion battery.Lithium ion battery of the present invention can realize high-tension target, and the highest normal working voltage can bring up to 4.4V ~ 5.0V and the cycle performance of lithium ion battery is good, and discharge and recharge all has higher capability retention, improves the useful life of lithium ion battery.When also including additive B in additive, further can improve the cycle performance of lithium ion battery, such as under the high pressure of more than 4.45V through repeatedly circulation after, lithium ion battery is made to have higher capability retention further, in addition, the discharge performance under lithium ion battery multiplying power and low temperature can also be improved further.
The application is further described below by way of instantiation.But these examples are only exemplary, do not form any restriction to the protection range of the application.
In following embodiment, comparative example and experimental example, the reagent used, material and instrument be not as having special explanation, and all commercially available acquisition, wherein used reagent also obtains by conventional synthesis process.
Embodiment 1 ~ 10
In following embodiment, comparative example and experimental example, used material is as follows:
Organic solvent: ethylene carbonate (EC), propene carbonate (PC), diethyl carbonate (DEC); Lithium salts: LiPF
6;
Additive A:
Silane compound AS1, AS2, AS3 or AS4 containing cyano group;
There is dinitrile compound AM1, AM2, AM3 or AM4 of ehter bond;
The additive S used in comparative example contains the silicon nitrile compounds of low polyoxyethylene units disclosed in CN104072533A, the 2-propyl group nitrile ethyoxyl-trimethicone namely shown in embodiment 1;
Additive B: 1,1,2,2-tetra-fluoro ethyl-2', 2', 3', 3'-tetrafluoro propyl ether (F-EPE), vinylene carbonate (VC), PS (PS), adiponitrile (ADN), dicyclohexylcarbodiimide (DCC); Lithium battery diaphragm: the polypropylene barrier film (model is A273, is provided by Celgard company) of 16 micron thickness.
Lithium ion battery (hereinafter referred to as battery) 1 ~ 10 is prepared all by the following method:
(1) preparation of positive plate
By cobalt acid lithium (LiCoO
2), binding agent (Kynoar), conductive agent (acetylene black) they are LiCoO according to weight ratio
2: Kynoar: acetylene black=96:2:2 mixes, add 1-METHYLPYRROLIDONE (NMP), the system that is stirred under de-airing mixer effect becomes transparent and homogeneous shape, obtains anode sizing agent; Anode sizing agent being evenly coated on thickness is on the aluminium foil of 12 μm; Aluminium foil is transferred to after room temperature is dried 120 DEG C of oven drying 1h, then obtains positive plate through colding pressing, cutting.
(2) preparation of negative plate
Be graphite by graphite, acetylene black, thickener sodium carboxymethylcellulose (CMC), binding agent butadiene-styrene rubber according to weight ratio: acetylene black: binding agent butadiene-styrene rubber: thickener sodium carboxymethylcellulose (CMC)=95:2:2:1 mixes, after joining deionized water, under the stirring action of de-airing mixer, obtain cathode size; Cathode size is evenly coated on Copper Foil; Copper Foil is transferred to after room temperature is dried 120 DEG C of oven drying 1h, then obtains negative plate through colding pressing, cutting.
(3) preparation of electrolyte
Electrolyte 1 ~ 10 is prepared all by the following method:
In the argon gas atmosphere glove box of water content <10ppm, EC, PC and DEC are mixed formation organic solvent, fully dry lithium salts is dissolved in above-mentioned organic solvent, then additive A (AS1, AS2, AS3, AS4, AM1, AM2, AM3, AM4) and additive B (F-EPE, VC, PS, ADN, DCC) is added according to content shown in table 1 respectively in organic solvent, mix, obtain electrolyte.Wherein, the concentration of lithium salts is 1mol/L, EC, the weight ratio of PC, DEC is EC:PC:DEC=1:1:2.
(4) preparation of lithium ion battery
Positive plate, lithium battery isolation membrane, negative plate are folded in order, make lithium battery isolation membrane be in the effect playing isolation between positive and negative plate, then winding obtains naked battery core; Naked battery core is placed in external packing paper tinsel, the above-mentioned electrolyte prepared is injected in dried battery, through Vacuum Package, leave standstill, change into, the operation such as shaping, obtain battery.
In the preparation process of above-mentioned battery, used containing the silane compound of cyano substituent and the concrete kind of content and additive B thereof and content thereof in electrolyte selected in each battery, each electrolyte, as shown in Table 2 below.
In table 2, the content of the described silane compound containing cyano group is the percetage by weight obtained based on the total weight of electrolyte, and the content of other additives described is the percetage by weight obtained based on the total weight of electrolyte.
The electrolysis additive relevant parameter of table 2: comparative example 1-8 and embodiment 1-10
Performance test methods:
(1) the cycle performance test of battery
At the temperature of 45 DEG C, by the lithium ion battery of embodiment 1-10 and comparative example 1-8, with the multiplying power constant current charge of 0.5C to 4.45V, then constant voltage charge to electric current is 0.05C, then use 0.5C constant current discharge to 3.0V, so repeatedly carry out charging and discharging, calculate lithium ion battery respectively and to circulate the capability retention after 50 times, 100 times and 300 times.
Capability retention=(discharge capacity of the discharge capacity/circulate first of n-th circulation) × 100% of n circulation.Related data is see table 3.
(2) lithium ion battery high rate performance test
The battery of embodiment 1-10 and comparative example 1-8 is carried out following test respectively: by battery with 0.5C constant-current discharge to 3.0V, shelve 5min, then with 0.5C constant current charge to 4.45V, and constant voltage charge, be 0.05C by electric current, leave standstill 5min, more respectively with 0.2C, 1C, 1.5C, 2C constant-current discharge to by voltage 3.0V.Discharge capacity D1 under record 0.2C, 1C, 1.5C, 2C condition, based on the discharge capacity D0 under 0.2C, calculates the discharge capacitance (survey 15 batteries, get its mean value) under different multiplying.Related data is see table 4.
Wherein high rate performance=[(D1-D0)/D0] × 100% of battery.
(3) lithium ion battery low temperature performance test
At the temperature of 25 DEG C, by each for the lithium ion battery of embodiment 1-10 and comparative example 1-8 5, charging is started with the constant current of 1C/4.45V and constant voltage, charge cutoff electric current is 0.1C, and the cut-off electric discharge when 0.5C/3.0V, measure the initial capacity of lithium ion battery, then the lithium ion battery of each Charging state is put into respectively the cryogenic box that temperature is-10 DEG C and-20 DEG C, place 120 minutes, again with 1C constant-current discharge to 3.0V, record discharge capacity at different temperatures and stop internal resistance, the discharge capacity ratio of lithium ion battery under calculating Different hypothermia condition.Related data is see table 5.
0.2C discharge capacity at 0.5C discharge capacity/25 DEG C under low temperature discharge capacity ratio=low temperature
The correlated performance test result of table 3: comparative example 1-8 and embodiment 1-10
The correlated performance test result of table 4: comparative example 1-8 and embodiment 1-10
The correlated performance test result of table 5: comparative example 1-8 and embodiment 1-10
Related data in above-mentioned table 3 ~ 5 can be learnt, compared with comparative example 1-8, comparative example 5-8 only containing the silane compound containing cyano group in additive A or to have in the dinitrile compound of ehter bond a kind of time, owing to becoming membrane impedance comparatively large, cause capability retention and high rate performance to decline.And in embodiment 1-10, silane compound containing cyano group combinationally uses with the dinitrile compound with ehter bond, thickness and the impedance of positive electrode surface SEI film can be reduced, improve homogeneity and stability that positive electrode surface forms SEI film, thus improve high rate performance and the low temperature performance of lithium ion battery.Capability retention, high rate performance and low temperature performance at 45 DEG C after circulation are better than comparative example 1-8.
When also including additive B in additive, further can improve the cycle performance of lithium ion battery, such as under the high pressure of more than 4.45V through repeatedly circulation after, lithium ion battery is made to have higher capability retention further, in addition, the discharge performance under lithium ion battery multiplying power and low temperature can also be improved further.
The announcement of book according to the above description, the application those skilled in the art can also carry out suitable change and amendment to above-mentioned execution mode.Therefore, the application is not limited to embodiment disclosed and described above, also should fall in the protection range of claim of the application some modifications and changes of the application.
Claims (10)
1. an electrolyte, is characterized in that, comprises lithium salts, organic solvent and additive A, and described additive A comprises the silane compound containing cyano group and has the dinitrile compound of ehter bond;
The described silane compound structural formula containing cyano group is such as formula shown in I:
Wherein, R
1, R
2, R
3be selected from cyano group, halogen, C independently of one another
1 ~ 10alkyl, C
1 ~ 10alkoxyl, described halogen are selected from F, Cl, Br; N is selected from the integer of 0 ~ 5;
The described dinitrile compound structural formula with ehter bond is such as formula shown in II:
Wherein, R
4, R
5, R
6independently of one another for being selected from C
1 ~ 5alkylidene, C
2 ~ 5alkenylene, m is the integer of 1 ~ 5.
2. electrolyte according to claim 1, is characterized in that, in formula I, and R
1, R
2, R
3in have at least a substituting group to be cyano group.
3. electrolyte according to claim 2, is characterized in that, in formula I, and R
1, R
2, R
3in have at least a substituting group to be C
1 ~ 6alkoxyl.
4. electrolyte according to claim 2, is characterized in that, the described silane compound containing cyano group is selected from least one in trimethylsilyl cyanide, dicyano dimethylsilane, 2-cyano ethyl triethoxysilane.
5. electrolyte according to claim 1, it is characterized in that, the described dinitrile compound with ehter bond is selected from least one in following material: 3, 5-dioxa-pimelic dinitrile, 1, 4-bis-(cyanoethoxy) butane, ethylene glycol bisthioglycolate (2-cyano ethyl) ether, diethylene glycol two (2-cyano ethyl) ether, triethylene glycol two (2-cyano ethyl) ether, TEG two (2-cyano ethyl) ether, 1, 3-bis-(2-cyanoethoxy) propane, 1, 4-bis-(2-cyanoethoxy) butane, 1, 5-bis-(2-cyanoethoxy) pentane and ethylene glycol bisthioglycolate (4-cyanobutyl) ether.
6. electrolyte according to claim 1, is characterized in that, the silane compound containing cyano group in described additive A is 0.01% ~ 10% of the total weight of electrolyte with the total content of the dinitrile compound with ehter bond.
7. electrolyte according to claim 1, it is characterized in that, also containing additive B in described electrolyte, described additive B be selected from ether compound, nitrile compound, the cyclic ester compounds containing sulfur-to-oxygen double bond, the cyclic carbonate compound containing carbon-to-carbon unsaturated bond, containing one or more in the compound of imido grpup.
8. electrolyte according to claim 7, is characterized in that, described ether compound is selected from least one in substituted or unsubstituted ether, and substituting group is the substituting group containing halogen atom, and halogen atom is F, Cl, Br;
Described nitrile compound be selected from mono-nitrile compound, two nitrile compound, three nitrile compounds and four nitrile compounds one or more;
The described cyclic ester compounds containing sulfur-to-oxygen double bond is selected from cyclic sulfates, cyclic sulfite, saturated sultone and containing one or more in the unsaturated sultone of carbon-to-carbon double bond;
The described cyclic carbonate compound containing carbon-to-carbon unsaturated bond be selected from the cyclic carbonate compounds containing carbon-to-carbon double bond one or more;
The described compound containing imido grpup be selected from the compound containing imine group, carbodiimide groups one or more.
9. electrolyte according to claim 1, is characterized in that,
Described organic solvent is selected from least one in ethylene carbonate, propene carbonate, butylene, fluorinated ethylene carbonate, dimethyl carbonate, diethyl carbonate, dipropyl carbonate, methyl ethyl carbonate, methyl propyl carbonate, ethyl propyl carbonic acid ester, GBL, methyl propionate, methyl butyrate, ethyl acetate, ethyl propionate and ethyl butyrate;
Described lithium salts is selected from least one in lithium hexafluoro phosphate, difluorophosphate, LiBF4, two trifluoromethanesulfonimide lithium, two (fluorine sulphonyl) imine lithium, di-oxalate lithium borate and difluorine oxalic acid boracic acid lithium.
10. a lithium ion battery, is characterized in that, comprises the positive plate containing positive electrode active materials, the electrolyte according to any one of negative plate, lithium battery diaphragm and claim 1 ~ 9 containing negative active core-shell material.
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