CN106785044A - A kind of electrolyte and secondary cell - Google Patents

A kind of electrolyte and secondary cell Download PDF

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CN106785044A
CN106785044A CN201710076226.3A CN201710076226A CN106785044A CN 106785044 A CN106785044 A CN 106785044A CN 201710076226 A CN201710076226 A CN 201710076226A CN 106785044 A CN106785044 A CN 106785044A
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substituted
unsubstituted
electrolyte
compound
halogen
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CN106785044B (en
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栗文强
唐超
王群峰
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Ningde Amperex Technology Ltd
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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
    • 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
    • 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
    • H01M10/058—Construction or manufacture
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Secondary Cells (AREA)

Abstract

The application is related to secondary battery technology, and in particular to a kind of electrolyte and secondary cell.The electrolyte of the application includes organic solvent, lithium salts and additive, and halogenated silane compounds and SEI film for additive are contained in additive.The application, as feature additive package, can significantly improve high rate performance, DC impedance performance and the over-charging of battery by using halogenated silane compounds and SEI film for additive.

Description

A kind of electrolyte and secondary cell
Technical field
The application is related to technical field of lithium batteries, and in particular to a kind of electrolyte and secondary cell.
Background technology
In the information age for developing rapidly, the demand to electronic products such as mobile phone, notebook, cameras increases year by year.Lithium Ion battery as electronic product working power, with energy density is high, memory-less effect, operating voltage high the features such as, just Progressively replace traditional Ni-Cd, MH-Ni battery.Expansion and power, energy storage device however as electronics market demand Development, requirement of the people to lithium ion battery is improved constantly, and exploitation has relatively low internal resistance high power and safer Lithium ion battery turns into the task of top priority.At present, effective method is based on film forming addition in the middle of existing composition reduction electrolyte The consumption of agent, but storage and the cycle performance of battery core can be so influenceed again.
At present, the wide variety of electrolyte of lithium ion battery is as main electric conducting lithium salt and with cyclic carbonate with lithium hexafluoro phosphate The admixture solvent of ester and linear carbonate, but above-mentioned electrolyte still suffers from many deficiencies, it is specifically close in high-energy Under degree, the poor-performing of lithium ion battery, such as larger DC impedance, poor high rate performance and poor security performance.
In consideration of it, special propose the application.
The content of the invention
The primary goal of the invention of the application is to propose a kind of electrolyte.
Second goal of the invention of the application is to propose lithium ion battery.
In order to complete the purpose of the application, the technical scheme for using for：
The application is related to a kind of electrolyte, including organic solvent, lithium salts and additive, and halo silicon is contained in the additive Hydride compounds and SEI film for additive.
Preferably, it is at least one in the compound shown in formula (I) that the halogenated silane compounds are selected from structural formula,
Wherein, R11、R12、R13、R14It is each independently selected from hydrogen, halogen, substituted or unsubstituted C1~10Alkyl, substitution or Unsubstituted C1~10Alkoxy, substituted or unsubstituted C2~10Alkenyl, substituted or unsubstituted C2~10Alkynyl, substitution or unsubstituted C2~10Heterocyclic group, silicon-containing group；And R11、R12、R13、R14In at least one substitution base be halogen；
Substitution base is selected from halogen, nitro, cyano group, carboxyl, sulfate, C1~6Alkyl, C2~6Alkenyl.
Preferably, R11、R12、R13、R14It is each independently selected from hydrogen, halogen, substituted or unsubstituted C1~6Alkyl, substitution Or unsubstituted C1~6Alkoxy, substituted or unsubstituted C2~6Alkenyl, substituted or unsubstituted C2~6Heterocyclic group,
Wherein, n is selected from 1~3 integer, and m is selected from 1~3 integer, R11’、R12’、R13’、R14’、R15’、R16' each only On the spot it is selected from halogen, substituted or unsubstituted C1~6Alkyl；
Substitution base is selected from halogen, C1~3Alkyl, C2~4Alkenyl.
Preferably, the halogenated silane compounds are selected from least one in following compound：
Preferably, the SEI film for additive is selected from cyclic carbonate compound, cyclic sulfates compound, sulfonic acid At least one in ester compounds, methylene disulfonate compound, nitrile compound.
Preferably, the cyclic carbonate compound is selected from least one in the compound as shown in formula II -1；
The cyclic sulfates compound is selected from least one in the compound as shown in formula II -2；
The sultone compounds are selected from least one in the compound as shown in formula II -3；
The methylene disulfonate compound is selected from least one in the compound as shown in formula II -4；
The nitrile compound is selected from least one in the compound as shown in formula II -5；
Wherein, R21、R22、R23It is each independently selected from substituted or unsubstituted C1~6It is alkylidene, substituted or unsubstituted C2~6Alkenylene；
R24、R25、R26、R27It is each independently selected from hydrogen, halogen, substituted or unsubstituted C1~10Alkyl, substitution or unsubstituted C2~10Alkenyl；
R28Selected from substituted or unsubstituted C1~12Alkylidene, substituted or unsubstituted C2~12Alkenylene, substitution do not take The C in generation6~12Arlydene；
Substitution base is selected from halogen, C1~3Alkyl, C2~4Alkenyl.
Preferably, R21~R23It is each independently selected from substituted or unsubstituted C1~4Alkylidene, substituted or unsubstituted C2~4 Alkenylene；Substitution base is selected from halogen, C1~3Alkyl, C2~4Alkenyl；
R24~R27It is each independently selected from hydrogen atom, halogen atom；Substituted or unsubstituted C1~4 alkylidene, substitution or not Substituted C2~4 alkenylene；Substitution base is selected from halogen, C1~3 alkyl, C2~4 alkenyl；
R28Selected from C1~6Alkylidene, C2~6Alkenylene, C6~12Arlydene.
Preferably, the SEI film for additive is selected from vinylene carbonate, fluorinated ethylene carbonate, 1, in 3-N-morpholinopropanesulfonic acid Ester, vinyl vinylene carbonate, 1,3- propene sultones, sulfuric acid vinyl ester, methane-disulfonic acid methylene ester, succinonitrile, oneself At least one in dintrile.
Preferably, weight/mass percentage composition of the halogenated silane compounds in the electrolyte is 0.001%~5%； Preferably 0.001%~2%.
Preferably, weight/mass percentage composition of the SEI film for additive in the electrolyte is 0.01%~30%；It is excellent Elect 0.1%~10% as.
The application further relates to a kind of secondary cell, including positive plate, negative plate, be arranged at intervals at positive plate and negative plate it Between barrier film and electrolyte, the electrolyte for the application electrolyte.
The technical scheme of the application at least has following beneficial effect：
The application by using halogenated silane compounds and SEI film for additive as feature additive package, can be notable Improve high rate performance, DC impedance (DCR) performance and the over-charging of battery.
Specific embodiment
To make the purpose, technical scheme and advantage of the application 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, without It is whole embodiments.Based on technical scheme and given embodiment that the application is provided, those skilled in the art are not having The every other embodiment obtained under the premise of creative work is made, the scope of the application protection is belonged to.
The application is related to a kind of electrolyte, including organic solvent, lithium salts and additive, contains halo silicon in additive simultaneously Hydride compounds and SEI film for additive.Because halogenated silane compounds are susceptible to oxidation reaction in battery system, can be in battery core There is the SEI film (CEI) that oxidation reaction forms densification in positive electrode surface.This interfacial film can effectively reduce molten , in the side reaction of positive pole, the performance to battery is highly profitable for agent and other additives；The boundary that halogenated silane compounds are formed simultaneously Facial mask is relative more to be stablized with lithium alkylide, does not also interfere with the transmission of lithium ion.The application by by halogenated silane compounds with SEI film for additive combine after, battery plus-negative plate generate stabilization passivating film, it is effective and stabilization CEI and SEI presence and Significantly improve high rate performance, DC impedance (DCR) performance and the over-charging of battery.
Improved as one kind of the application electrolyte, it is shown in formula (I) that the application halogenated silane compounds are selected from structural formula Compound at least one,
Wherein, R11、R12、R13、R14It is each independently selected from hydrogen, halogen, sulfate, substituted or unsubstituted C1~10Alkyl, Substituted or unsubstituted C2~10Alkenyl, substituted or unsubstituted C2~10Alkynyl, substituted or unsubstituted C2~10It is heterocyclic group, siliceous Group；And R11、R12、R13、R14In at least one substitution base be halogen；
Substitution base is selected from halogen, nitro, cyano group, carboxyl, sulfate, C1~6Alkyl, C2~6Alkenyl.
In above-mentioned substitution base, heterocyclic group is, containing 1~3 heterocyclic compound of hetero atom (N, O, S), to specifically include Three circle heterocycles, such as oxirane, aziridine, five-ring heterocycles such as pyrroles, pyrazoles, imidazoles, furans etc., hexa-member heterocycle such as pyridine, Pyrans etc.；
Halogen is selected from F, Cl, Br.
Improved as one kind of the application electrolyte, R11、R12、R13、R14In at least two substitution bases be halogen.
Improved as one kind of the application electrolyte, R11、R12、R13、R14It is each independently selected from hydrogen, halogen, substitution or not Substituted C1~6Alkyl, substituted or unsubstituted C2~6Alkenyl, substituted or unsubstituted C2~6Heterocyclic group, N is selected from 1~3 integer, and m is selected from 1~3 integer, R11’、R12’、R13’、R14’、R15’、R16' be each independently selected from halogen, Substituted or unsubstituted C1~6Alkyl；
Substitution base is selected from halogen, C1~3Alkyl, C2~4Alkenyl.
Improved as one kind of the application electrolyte, R11、R12、R13、R14It is each independently selected from halogen, substitution or does not take The C in generation1~6Alkyl, Wherein, R11’、 R12’、R13’、R14’、R15’、R16' it is each independently selected from halogen, substituted or unsubstituted C1~6Alkyl；
Substitution base is selected from halogen, C1~3Alkyl, C2~4Alkenyl.
Improved as one kind of the application electrolyte, R11、R12、R13、R14It is each independently selected from halogen, substitution or does not take The C in generation1~6Alkyl,Wherein, R11’、R12’、R15' each only On the spot it is selected from halogen, substituted or unsubstituted C1~6Alkyl；
Substitution base is selected from halogen, C1~3Alkyl, C2~4Alkenyl.
As the application electrolyte one kind improve, the application halogenated silane compounds be selected from following compound at least One kind,
(iodo trimethylsilane)；(double (methyl difluoro silicon substrate) second of 1,2- Alkane)；
Improved as one kind of the application electrolyte, the application halogenated silane compounds are selected from formula (I -1) to formula (I -13) At least one in the compound, but not limited to this.
Improved as one kind of the application electrolyte, the application halogenated silane compounds quality percentage in the electrolytic solution contains Measure is 0.001%~5%.When the content of halogenated silane compounds is less than 0.001%, it is impossible to formed completely on both positive and negative polarity surface And effective CEI/SEI films, so as to the side reaction caused by the electro transfer between electrolyte and electrode can not be prevented effectively；And When halogenated silane compounds content is more than 5%, thicker CEI/SEI films can be formed in positive cathode surface, cause lithium ion to move Resistance increase is moved, while the silane compound of non-film forming can further be aoxidized in cyclic process, is unfavorable for electricity in cyclic process The positive pole interface stability in pond.
It is further preferred that the upper limit of the application halogenated silane compounds weight/mass percentage composition scope in the electrolytic solution is appointed Selected from 5%, 4%, 3%, 2.0%, 1.5%, 1.0%, lower limit is optionally from 0.001%, 0.005%, 0.01%, 0.05%, 0.1%th, 0.3%, 0.5%, 0.6%.It is further preferred that halogenated silane compounds percentage composition in the electrolytic solution is 0.001%~2%.
Improved as one kind of the application electrolyte, SEI film for additive is selected from cyclic carbonate compound, ring-type sulfuric acid At least one in ester compounds, sultone compounds, methylene disulfonate compound, nitrile compound.
As the application one kind improve, the structural formula of cyclic carbonate compound as shown in formula II -1, R21Selected from substitution Or unsubstituted C1~6Alkylidene, substituted or unsubstituted C2~6Alkenylene；Substitution base is selected from halogen, C1~6Alkyl, C2~6Alkenyl；
Improved as one kind of the application electrolyte, R21Selected from substituted or unsubstituted C1~4Alkylidene, substitution do not take The C in generation2~4Alkenylene；Substitution base is selected from halogen, C1~3Alkyl, C2~4Alkenyl.
Improved as one kind of the application electrolyte, it is sub- that cyclic carbonate compound is selected from fluorinated ethylene carbonate, carbonic acid Vinyl acetate, at least one of vinylethylene carbonate；Concrete structure formula is as follows：
Improved as one kind of the application electrolyte, cyclic carbonate compound is also selected from：
As the application electrolyte one kind improve, the structural formula of cyclic sulfates compound as shown in formula II -2, R22Choosing From substituted or unsubstituted C1~6Alkylidene, substituted or unsubstituted C2~6Alkenylene；Substitution base is selected from halogen, C1~6Alkyl, C2~6 Alkenyl；
Improved as one kind of the application electrolyte, R22Selected from substituted or unsubstituted C1~4Alkylidene, substitution do not take The C in generation2~4Alkenylene；Substitution base is selected from halogen, C1~3Alkyl, C2~4Alkenyl.
Improved as one kind of the application electrolyte, cyclic sulfates compound is selected from ethyl sulfate, 4- methylsulfuric acids At least one in ethyl, sulfuric acid Asia propyl ester, concrete structure formula is as follows；
Improved as one kind of the application electrolyte, cyclic sulfates compound is selected from ethyl sulfate.
Improved as one kind of the application electrolyte, cyclic sulfates compound is also selected from：
As the application electrolyte one kind improve, the structural formula of sultone compounds as shown in formula II -3, R23It is selected from Substituted or unsubstituted C1~6Alkylidene, substituted or unsubstituted C2~6Alkenylene；Substitution base is selected from halogen, C1~6Alkyl, C2~6Alkene Base；
Improved as one kind of the application electrolyte, R23Selected from substituted or unsubstituted C1~4Alkylidene, substitution do not take The C in generation2~4Alkenylene；Substitution base is selected from halogen, C1~3Alkyl, C2~4Alkenyl.
Improved as one kind of the application electrolyte, sultone compounds are selected from PS, Isosorbide-5-Nitrae-fourth sulphur At least one in acid lactone, 1,3- propene sultones, concrete structure formula is as follows；
Improved as one kind of the application electrolyte, sultone compounds are selected from PS, 1,3- propylene At least one in sultones.
Improved as one kind of the application electrolyte, sultone compounds are also selected from：
Improved as one kind of the application electrolyte, methylene disulfonate compound is selected from as shown in formula II -4；
R24、R25、R26、R27It is each independently selected from hydrogen, halogen, substituted or unsubstituted C1~10Alkyl, substitution or unsubstituted C2~10Alkenyl；Substitution base is halogen.
Improved as one kind of the application electrolyte, methylene disulfonate compound is selected from disulfonic acid methylene ester, methane two One or several in sulfonic acid methylene ester, 3- methyl-methane-disulfonic acid methylene ester and following structural formula；
Improved as one kind of the application electrolyte, the structural formula of nitrile compound is as shown in II 5；
Wherein, R28Selected from substituted or unsubstituted C1~12Alkylidene, substituted or unsubstituted C2~12Alkenylene, substitution or Unsubstituted C6~12Arlydene, wherein, substitution base be selected from halogen, C1~6Alkyl, C2~6Alkenyl.
Improved as one kind of the application electrolyte, R28Selected from C1~6Alkylidene, C2~6Alkenylene, phenylene.
Improved as one kind of the application electrolyte, nitrile compound is selected from succinonitrile, adiponitrile, malononitrile, glutaronitrile At least one.
Improved as one kind of the application electrolyte, nitrile compound is selected from adiponitrile.
Improved as one kind of the application electrolyte, nitrile compound is also selected from nitrile compound shown in following structure It is at least one；
Improved as one kind of the application electrolyte, SEI film for additive is selected from vinylene carbonate (VC), fluoro carbonic acid Vinyl acetate (FEC), 1,3- propane sultones (PS), vinyl vinylene carbonate (VEC), 1,3- propene sultones (PST), At least one in sulfuric acid vinyl ester (DTD), methane-disulfonic acid methylene ester (MMDS), adiponitrile (ADN) etc..
In the above-mentioned formula of the application：
Carbon number is 1~10 alkyl, and alkyl can be chain-like alkyl, or cycloalkyl, on the ring of cycloalkyl Hydrogen can be replaced by alkyl, in the alkyl the preferred lower limit of carbon number be 2,3,4,5, preferred higher limit be 3,4,5, 6,8,10.Preferably, selection carbon number is 1~10 alkyl, it is further preferred that selection carbon number is 1~6 chain Alkyl, carbon number is 3~8 cycloalkyl, it is further preferred that selection carbon number is 1~4 chain-like alkyl, carbon is former Subnumber is 5~7 cycloalkyl.As the example of alkyl, can specifically enumerate：Methyl, ethyl, n-propyl, isopropyl, positive fourth Base, isobutyl group, sec-butyl, the tert-butyl group, n-pentyl, isopentyl, neopentyl, hexyl, 2- Methyl pentyls, 3- Methyl pentyls, 1, 1,2- trimethyl-propyls, 3,3, it is-dimethyl-butyl, heptyl, 2- heptyl, 3- heptyl, 2- methylhexyls, 3- methylhexyls, different Heptyl, octyl group, nonyl, decyl.
Can be alkoxy when oxygen atom is contained in the alkyl that the foregoing carbon number being previously mentioned is 1~12.Preferably, Selection carbon number is 1~10 alkoxy, it is further preferred that selection carbon number is 1~6 alkoxy, further Preferably, selection carbon number is 1~4 alkoxy.As the example of alkoxy, can specifically enumerate：Methoxyl group, ethoxy Base, positive propoxy, isopropoxy, n-butoxy, sec-butoxy, tert-butoxy, n-pentyloxy, isoamoxy, cyclopentyloxy, ring Hexyloxy.
Carbon number is that 2~12 alkenyl can be for cyclic alkenyl radical, or chain alkenyl.In addition, in alkenyl double bond Number is preferably 1.The preferred lower limit of carbon number is 3,4,5 in the alkenyl, and preferred higher limit is 3,4,5,6,8,10, 12.Preferably, selection carbon number is 2~10 alkenyl, it is further preferred that selection carbon number is 2~6 alkenyl, more It is further preferred that selection carbon number is 2~5 alkenyl.As the example of alkenyl, can specifically enumerate：Vinyl, allyl Base, isopropenyl, pentenyl, cyclohexenyl group, cycloheptenyl, cyclo-octene base.To the specifically chosen identical with alkenyl of alkynyl.
Carbon number be 1~12 alkylidene for straight or branched alkylidene, carbon number is preferred in the alkylidene Lower limit is 2,3,5,6, and preferred higher limit is 4,5,6,7,8,9,10.Preferably, selection carbon number is 1~6 alkylene Base, more preferably carbon number are 1~4 alkylidene.As the example of alkyl, can specifically enumerate：Methylene, ethylidene, Asia Propyl group, isopropylidene, butylidene, isobutylidene, sub- sec-butyl, pentylidene, hexylidene.
Carbon number be 2~12 alkenylene for straight or branched alkenylene, the number of double bond is preferably 1 in alkenyl. The preferred lower limit of carbon number is 3,4,5,6 in the alkenylene, and preferred higher limit is 4,5,6,7,8,9,10.It is preferred that Ground, selection carbon number is 2~8 alkenylene；More preferably carbon number is 2~6 alkenylene.As the example of alkenylene, Can specifically enumerate：Ethenylidene, acrol, sub- isopropenyl, sub- alkene butyl, sub- alkene amyl group.
Halogen is selected from fluorine, chlorine, bromine.
Improved as one kind of the application electrolyte, the application SEI film for additive quality percentage in the electrolytic solution contains Measure is 0.01%~30%.Preferably, the upper limit of SEI film for additive weight/mass percentage composition scope in the electrolytic solution is optional certainly 30%th, 28%, 26%, 24%, 22%, 20%, 16%, 14%, 10%, lower limit is optionally from 0.01%, 0.05%, 0.1%, 0.5%th, 1%, 2%, 5%, 8%.It is further preferred that SEI film forming addition percentage composition in the electrolytic solution is 0.001% ~2%.
Improved as one kind of the application electrolyte, the electrolyte of the application is nonaqueous electrolytic solution, and organic solvent is selected from carbon Vinyl acetate (EC), propene carbonate (PC), butylene, fluorinated ethylene carbonate, methyl ethyl carbonate, dimethyl carbonate, Diethyl carbonate (DEC), dipropyl carbonate, methyl propyl carbonate, ethyl propyl carbonic acid ester, 1,4- butyrolactone (GBL), methyl propionate, spy At least one in the sour methyl esters of business, methyl isobutyrate, methyl butyrate, propyl propionate, ethyl acetate, ethyl propionate, ethyl butyrate.
Improved as one kind of the application electrolyte, the application lithium salts is selected from least in organic lithium salt or inorganic lithium salt Kind.
As the application electrolyte one kind improve, in the application lithium salts containing in fluorine element, boron element, P elements extremely Few one kind.
Improved as one kind of the application electrolyte, the application lithium salts is selected from lithium hexafluoro phosphate LiPF6, double fluoroform sulphurs Imide li LiN (CF3SO2)2(being abbreviated as LiTFSI), double (fluorine sulphonyl) imine lithium Li (N (SO2F)2) (being abbreviated as LiFSI), double Lithium bis (oxalate) borate LiB (C2O4)2(being abbreviated as LiBOB), difluorine oxalic acid boracic acid lithium LiBF2(C2O4) in (being abbreviated as LiDFOB) extremely Few one kind.
The application further relates to a kind of secondary cell, including positive plate, negative plate, be arranged at intervals at positive plate and negative plate it Between barrier film and electrolyte.It should be noted that the secondary cell of the embodiment of the present application can for lithium ion battery, sodium from Sub- battery.In subordinate's specific embodiment of the application, the embodiment of lithium ion battery, but the application not limited to this are only shown.
Present invention also provides a kind of lithium ion battery, including positive plate, negative plate, it is arranged at intervals at positive plate and negative pole Barrier film, electrolyte and package foil between piece；The 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 that is coated on negative current collector；Electrolyte is foregoing Electrolyte described in one paragraph.
Improved as one kind of the application lithium ion battery, the application positive pole diaphragm includes positive electrode active materials, binding agent And conductive agent.
Improved as one kind of the application lithium ion battery, the application positive electrode active materials are optionally from cobalt acid lithium LiCoO2、 At least one in lithium-nickel-manganese-cobalt ternary material, LiFePO4, LiMn2O4.
Improved as one kind of the application lithium ion battery, the application positive electrode active materials cobalt acid lithium and lithium-nickel-manganese-cobalt ternary The mixture of material.
Improved as one kind of the application lithium ion battery, the application cathode membrane includes negative active core-shell material, binding agent And conductive agent.
Improved as one kind of the application lithium ion battery, the application negative active core-shell material is graphite and/or silicon.
Exemplary description is done to the technical scheme of the application below by way of specific embodiment：
The preparation of electrolyte：In water content<In the argon gas atmosphere glove box of 10ppm, by ethylene carbonate (being abbreviated as EC), Diethyl carbonate (being abbreviated as DEC), propene carbonate (being abbreviated as PC), ethyl propionate, according to 20:30:20:30 mass ratio is mixed After closing uniformly, nonaqueous solvents is obtained, then will abundant dry lithium salts LiPF6Above-mentioned nonaqueous solvents is dissolved in, LiPF is made into6Concentration It is the basic electrolyte of 1mol/L.
According to shown in table 1, halogenated silane compounds and SEI film for additive are added in basic electrolyte.
Example as halogenated silane compounds is：Fluoro trimethylsilane (B1, as shown in Formulas I -1), vinyl-dimethyl base Silicon fluoride (B2, as shown in Formulas I -2), difluorodimethylsilane (B3, as shown in Formulas I -3), trifluoro trimethylsilyl (B4, such as Formulas I -4 It is shown), a fluorine triethoxysilane (B5, as shown in Formulas I -13).
Example as SEI film for additive is：From vinylene carbonate (VC), fluorinated ethylene carbonate (FEC), 1,3- Propane sultone (PS), sulfuric acid vinyl ester (DTD), adiponitrile (ADN).
The preparation of lithium ion battery：
1) preparation of positive plate：By positive active material cobalt acid lithium, (molecular formula is LiCoO2), conductive agent acetylene black, bond Agent polyvinylidene fluoride (being abbreviated as PVDF) is by weight 96:2:2 in appropriate 1-METHYLPYRROLIDONE (being abbreviated as NMP) solvent In be thoroughly mixed, form it into uniform anode sizing agent；This slurry is coated on plus plate current-collecting body Al paper tinsels, drying, it is 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), thickener sodium carboxymethylcellulose (being abbreviated as CMC) compares 95 according to weight:2:2:1 in appropriate deionized water solvent It is thoroughly mixed, forms it into uniform cathode size；This slurry is coated on negative current collector Cu paper tinsels, is dried, is colded pressing, Obtain negative plate.
3) barrier film：Using PE porous polymer films as barrier film.
4) preparation of lithium ion battery：Positive plate, barrier film, negative plate are folded in order, barrier film is in positive pole Play a part of isolation between piece and negative plate, then winding obtains naked battery core；Naked battery core is placed in external packing paper tinsel, will be above-mentioned The electrolyte for preparing is injected into dried battery, by operations such as Vacuum Package, standing, chemical conversion, shapings, that is, completes lithium The preparation of ion battery.
The electrolyte and lithium ion battery of embodiment 1~14 and comparative example 1~5 are prepared according to above-mentioned preparation method；Electricity Additive and respective addition are as shown in table 1 in solution liquid.
The electrolysis additive and addition of the embodiment 1~14 of table 1 and comparative example 1~5
Performance test will be carried out to the lithium ion battery of each comparative example of the application and embodiment by experiment below.
Test one, rate of charge test
The lithium ion battery that will be prepared respectively carries out following tests：
At 25 DEG C, by lithium ion battery, 4.4V is charged to different multiplying 0.5C, 1C, 2C, 3C, 5C, record fills respectively Capacitance, using the capacitance of 0.5C as benchmark (100%), calculates the capacity that different multiplying charges.In each lithium ion battery Selected electrolyte and the relevant test data that obtains are referring to table 2.
The lithium ion battery rate of charge test result of the embodiment 1~14 of table 2 and comparative example 1~5
With reference in Tables 1 and 2 as can be seen that comparative example 3 electrolyte in be individually added into 0.01% halogenated silane compounds When, the rate of charge of lithium ion battery is compared to without the slightly improvement of comparative example 1 for adding halogenated silanes.In embodiment 1~11, The SEI film for additive that mass fraction is 0.5% halogenated silane compounds and mass fraction is 4% is added in electrolyte simultaneously When, the charging capacity of battery is obviously improved.Particularly embodiment 10, has lower impedance, so charging rate after DTD film forming Hurry up, rate of charge is high.And in comparative example 12 and comparative example 14 because add halogenated silanes amount it is less be 0.01%, and SEI into Film additive addition is more, causes anode film forming thicker, influences the deintercalation of lithium ion, so that the charging capacity of influence.However, working as When the content of halogenated silane compounds is more in electrolyte, more than 2%, not only the charging capacity of battery does not improve, or even meeting Deteriorate, reason can cause into thickness when being excessive halogenated silane compounds and electrolysis fluid viscosity is high, lithium ion conduction becomes difficult The comparative example 2 of 3% halogenated silane compounds is particularly added in electrolyte, the charging capacity of its battery is far below other groups.
Test two, DCR test
The lithium ion battery that will be prepared respectively carries out following tests：
By lithium ion battery, static 1h, is completely filled to battery core at 25 DEG C, and 0.1C is discharged to 3.0V afterwards, obtains electricity The actual capacity of core.Then after being discharged to designated capabilities, respectively with 0.1C electric discharge 10s, 1C electric discharge 360s, the electricity after record electric discharge Pressure V1 and V2.DCR=(V2-V1)/(I2-I1) every group of each 5 battery, calculated according to DCR computing formula.Each lithium ion Selected electrolyte and the relevant test data that obtains are referring to table 3 in battery.
The lithium ion battery DCR of the embodiment 1~14 of table 3 and comparative example 1~5
Be can be seen that compared with comparative example 1 with reference in table 1 and table 3,0.01% is individually added into the electrolyte of comparative example 3 Fluoro trimethylsilane when, the DCR of lithium ion battery has reduction.In embodiment 1~5, addition mass fraction is in electrolyte 0.5% fluoro trimethylsilane, vinyl-dimethyl base silicon fluoride, difluorodimethylsilane, trifluoro trimethylsilyl, the ethoxy of a fluorine three Base silane, the DCR reductions of battery are obvious.However, when the content of halogenated silane compounds in electrolyte is less than 0.01%, It is smaller that the DCR of battery improves amplitude.When the content of halogenated silane compounds in electrolyte is more than 2%, not only the DCR of battery does not have There is improvement, or even can deteriorate, this is primarily due to, and halogenated silanes more film forming is thicker to be caused.Such as comparative example 2, its battery DCR is apparently higher than embodiment 6.
Test three, anti-over-charging test
Battery is discharged to 3.0V at 25 DEG C with 0.5C, then with 0.5C constant-current charges to 10V, in 10V constant-voltage charge 2h, Test temperature change of the battery in charging process simultaneously and observe the state of battery after test.The result such as table of anti-over-charging test Shown in 6.
The embodiment 1~14 of table 4 and the lithium battery 0.5C/10V 2h of comparative example 1~5 overcharge result
Group Anti-over-charging is tested
Embodiment 1 5/5OK
Embodiment 2 5/5OK
Embodiment 3 5/5OK
Embodiment 4 5/5OK
Embodiment 5 5/5OK
Embodiment 6 5/5OK
Embodiment 7 5/5OK
Embodiment 8 5/5OK
Embodiment 9 5/5OK
Embodiment 10 5/5OK
Embodiment 11 5/5OK
Embodiment 12 5/5OK
Embodiment 13 5/5OK
Embodiment 14 5/5OK
Comparative example 1 5/5fire
Comparative example 2 1/5OK,4/5fire
Comparative example 3 1/5OK,4/5fire
Comparative example 4 0/5OK,5/5fire
Comparative example 5 2/5OK,3/5fire
With reference in table 1 and table 4 as can be seen that when halogenated silane compounds content be higher than 2% when, it will cause battery to exist Caught fire during anti-over-charging, its reason can contemplate because the excessive halogenated silanes membrane impedance during lasting charging cycle Increase, cause battery lithium metal in cyclic process to separate out, lasting lithium is easily caused battery short circuit, battery in negative terminal surface deposition Burning.When the halogenated silane compounds for adding are less than 2%, film forming thickness is relatively mild, will not cause the serious analysis lithium of battery core, Obstruction electrolyte contact with battery core active material is played simultaneously, is reduced electrolyte side reaction and is occurred, so that overcharge being changed It is kind.
The application other embodiments：
Method according to previous embodiment prepares the lithium battery of embodiment 15~36, and difference is：Each component in electrolyte And adding proportion is as shown in table 5：
Component and adding proportion in the battery electrolyte of 5 embodiment of table 15~36
The performance of the battery according to the method for previous embodiment to preparing detects that detection obtains embodiment battery 15~36 performance is similar to above example, repeats no more as space is limited.
It is not for limiting claim, any this area skill although the application is disclosed as above with preferred embodiment Art personnel are not being departed from the premise of the application conceives, and can make some possible variations and modification, therefore the application The scope that protection domain should be defined by the application claim is defined.

Claims (10)

1. a kind of electrolyte, including organic solvent, lithium salts and additive, it is characterised in that contain halo silicon in the additive Hydride compounds and SEI film for additive.
2. electrolyte according to claim 1, it is characterised in that it is formula that the halogenated silane compounds are selected from structural formula (I) at least one in compound shown in,
Wherein, R11、R12、R13、R14It is each independently selected from hydrogen, halogen, substituted or unsubstituted C1~10Alkyl, substitution do not take The C in generation1~10Alkoxy, substituted or unsubstituted C2~10Alkenyl, substituted or unsubstituted C2~10It is alkynyl, substituted or unsubstituted C2~10Heterocyclic group, silicon-containing group；And R11、R12、R13、R14In at least one substitution base be halogen；
Substitution base is selected from halogen, nitro, cyano group, carboxyl, sulfate, C1~6Alkyl, C2~6Alkenyl.
3. electrolyte according to claim 2, it is characterised in that R11、R12、R13、R14Be each independently selected from hydrogen, halogen, Substituted or unsubstituted C1~6Alkyl, substituted or unsubstituted C1~6Alkoxy, substituted or unsubstituted C2~6Alkenyl, substitution or not Substituted C2~6Heterocyclic group,
Wherein, n is selected from 1~3 integer, and m is selected from 1~3 integer, R11’、R12’、R13’、R14’、R15’、R16' independently of one another Selected from halogen, substituted or unsubstituted C1~6Alkyl；
Substitution base is selected from halogen, C1~3Alkyl, C2~4Alkenyl.
4. electrolyte according to claim 2, it is characterised in that the halogenated silane compounds are selected from following compound At least one：
5. electrolyte according to claim 1, it is characterised in that the SEI film for additive is esterified selected from cyclic carbonate At least one in compound, cyclic sulfates compound, sultone compounds, methylene disulfonate compound, nitrile compound.
6. electrolyte according to claim 5, it is characterised in that
The cyclic carbonate compound is selected from least one in the compound as shown in formula II -1；
The cyclic sulfates compound is selected from least one in the compound as shown in formula II -2；
The sultone compounds are selected from least one in the compound as shown in formula II -3；
The methylene disulfonate compound is selected from least one in the compound as shown in formula II -4；
The nitrile compound is selected from least one in the compound as shown in formula II -5；
Wherein, R21、R22、R23It is each independently selected from substituted or unsubstituted C1~6Alkylidene, substituted or unsubstituted C2~6Sub- alkene Base；
R24、R25、R26、R27It is each independently selected from hydrogen, halogen, substituted or unsubstituted C1~10It is alkyl, substituted or unsubstituted C2~10Alkenyl；
R28Selected from substituted or unsubstituted C1~12Alkylidene, substituted or unsubstituted C2~12It is alkenylene, substituted or unsubstituted C6~12Arlydene；
Substitution base is selected from halogen, C1~3Alkyl, C2~4Alkenyl.
7. electrolyte according to claim 5, it is characterised in that the SEI film for additive be selected from vinylene carbonate, Fluorinated ethylene carbonate, 1,3- propane sultones, vinyl vinylene carbonate, 1,3- propene sultones, sulfuric acid vinyl ester, At least one in methane-disulfonic acid methylene ester, succinonitrile, adiponitrile.
8. electrolyte according to claim 1, it is characterised in that the halogenated silane compounds are in the electrolyte Weight/mass percentage composition is 0.001%~5%；Preferably 0.001%~2%.
9. electrolyte according to claim 1, it is characterised in that the SEI film for additive is in the electrolyte Weight/mass percentage composition is 0.01%~30%；Preferably 0.1%~10%.
10. a kind of secondary cell, including positive plate, negative plate, the barrier film being arranged at intervals between positive plate and negative plate, with And electrolyte, it is characterised in that the electrolyte is any described electrolyte of claim 1~9.
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