CN106611874A - Gel polymer lithium-ion electrolyte and battery containing same - Google Patents
Gel polymer lithium-ion electrolyte and battery containing same Download PDFInfo
- Publication number
- CN106611874A CN106611874A CN201611071945.8A CN201611071945A CN106611874A CN 106611874 A CN106611874 A CN 106611874A CN 201611071945 A CN201611071945 A CN 201611071945A CN 106611874 A CN106611874 A CN 106611874A
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- Prior art keywords
- lithium ion
- gel polymer
- phenylenediamines
- electrolyte
- polymer lithium
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Classifications
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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
- H01M10/0565—Polymeric materials, e.g. gel-type or solid-type
-
- 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
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0085—Immobilising or gelification of electrolyte
-
- 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
Abstract
The invention discloses a gel polymer lithium-ion electrolyte and a battery containing the electrolyte, and belongs to the field of lithium batteries. The provided electrolyte is good in low-temperature performance and high in conductivity. The electrolyte comprises an inorganic salt, an organic solvent, a polymer, a cross-linking agent and an initiator, and is characterized in that monomer raw materials of the polymer comprise one binary acid monomer containing a benzene ring structure and two diamine monomers.
Description
Technical field
The present invention relates to field of lithium, specifically a kind of electrolyte.
Background technology
Electrolyte is the big critical material of lithium ion battery four（Positive pole, negative pole, barrier film, electrolyte）One of, it is known as lithium ion
" blood " of battery, plays a part of to conduct electronics in the battery between both positive and negative polarity, is that lithium ion pond obtains high voltage, high specific energy
The advantages of guarantee.Electrolyte is typically by highly purified organic solvent, electrolyte lithium salt（Such as lithium hexafluoro phosphate, LiFL6）, it is necessary
The raw material such as additive, under certain condition, be formulated by a certain percentage.
Organic solvent is the main part of electrolyte, closely related with the performance of electrolyte, typically molten with high-k
Agent is used in mixed way with low viscosity solvent.
Electrolyte can be divided into liquid electrolyte and solid polymer, and solid polymer electrolyte generally can be divided into form solid
Polymer dielectric (SPE) and gel polymer electrolyte (GPE).SPE solid polymer electrolytes are mainly also based on polyoxy
Change ethylene (PEO), it has the disadvantage that ionic conductivity is relatively low, and at 100 DEG C 10-40cm is can only achieve.In the conduction of SPE intermediate ions
Mainly occur in amorphous region, the movement by polymer chain carries out transmission migration.In addition inorganic compounding salt is added also to carry
High ion conductivity.The liquid organic solvent of high-k low relative molecular mass is added in solid polymer electrolyte such as
PC is then greatly improved the dissolubility of conducting salt, and the electrolyte for being constituted is GPE gel polymer electrolytes, and it is in room temperature
There is down very high ionic conductivity, but can occur in use to analyse liquid and fail.
The content of the invention
It is an object of the invention to：A kind of gel polymer lithium ion electrolyte is disclosed for above-mentioned problem, is taken
Concrete scheme it is as follows：
The invention discloses a kind of gel polymer lithium ion electrolyte, including inorganic salt, organic solvent, polymer, cross-linking agent,
Initiator, it is characterised in that described polymer monomer raw material includes a kind of dicarboxylic acid monomer containing benzene ring structure and two kind two
Amine monomers.
Preferably, the described binary acid containing benzene ring structure is selected from：P-phthalic acid, M-phthalic acid, O-phthalic
Acid, 2,2'- biphenyl dicarboxylic acids, 4,4'- diphenyl dicarboxylic acids；4- chloro-o-phthalic acids, oreinol diacid.
Preferably, two kinds of described diamine monomers are selected from：1,2- propane diamine bodies, ethylenediamine, 4-methyl-diaminopropane, N,
N'- double (3- aminopropyls) -1,4- butanediamine, 2- methyl isophthalic acids, 4- phenylenediamines, 1,3- propane diamine, ethylenedistearamide, 2- first
The chloro- 1,2- phenylenediamines of base p-phenylenediamine, p-phenylenediamine, 4-, NPD, m-diaminobenzene., 5- Trifluoromethyl-1s, 3- benzene
The bromo- 1,2- phenylenediamines of diamidogen, 4-, 3- nitro -1,2- phenylenediamines.
Further, in the raw material of described polymer also include the described binary acid containing benzene ring structure respectively with it is described
The prepolymer that formed of two kinds of monomer prepolymerizations, i.e., include dicarboxylic acid monomer, two kinds of diamidogen lists containing benzene ring structure in the feed
The prepolymer that body, the binary acid containing benzene ring structure and two kinds of diamine monomer difference prepolymerizations are formed.
Wherein, the molecular weight of the described prepolymer of described prepolymer is less than 50000, is less than as preferred molecular weight
30000
Described inorganic salt is selected from：LiBF4、LiClO4、LiAsF6、LiCF3SO3.
Further, described organic solvent is selected from ethylene carbonate, Allyl carbonate, dimethyl carbonate, methyl ester, butylene
Carbonic ester, acetone, espeleton, methylisobutylketone, glycol monoethyl ether, ethylene glycol monoethyl ether, ethylene glycol monobutyl ether, tumer
Ester, ethyl acetate, propyl acetate.
Further, the preferred divinylbenzene of described cross-linking agent, N,N methylene bis acrylamide.
The present invention discloses a kind of lithium ion battery, including positive electrode, negative material, lithium-ion membrane and electricity
Solution liquid, described electrolyte is the electrolyte that the present invention is provided, and described positive electrode, negative material, lithium-ion membrane are normal
The material of rule.
The present invention discloses a kind of preparation method of lithium ion battery, prepares as follows：
By lithium ion solvent, cross-linking agent, initiator, a kind of dicarboxylic acid monomer containing benzene ring structure and two kinds of diamine monomers according to upper
State dicarboxylic acid monomer proportionally to mix with the prepolymerized prepolymer of two kinds of diamine monomers respectively, stir, at room temperature, use
Vacuum liquid filling equipment makes its infiltration penetrate in barrier film and positive and negative pole material；Above-mentioned mixing is sealed, and it is little in fully infiltration barrier film 1
When more than；The polymerization at 30 DEG C -70 DEG C forms colloid.
The gelatin polymer of the present invention is polymerized by monomer and prepolymerization, has rigidity and toughness concurrently, and it is to very lithium salts
With very strong bearer capabilities, and there is very strong parcel ability to lithium ion, ionic conductivity is high, low temperature performance well, work
Make temperature range width, it is good with negative material suitability.
Specific embodiment
Specific embodiment 1：
It is respectively 1 according to mol ratio with 1,2- propane diamine bodies, ethylenediamine by p-phthalic acid:1 ratio is polymerized to form two kinds in advance
Aggressiveness, the molecular weight control of described performed polymer is being less than 3000.
By ethylene carbonate lithium ion solvent, cross-linker divinylbenzene, initiator, p-phthalic acid and 1,2- propane diamine
Body, ethylenediamine proportionally mix.
Stir, at room temperature, its infiltration is penetrated in barrier film and positive and negative pole material with vacuum liquid filling equipment；Sealing
Above-mentioned mixing, and fully infiltrating barrier film more than 1 hour；The polymerization at 60 DEG C -70 DEG C forms colloid.
The weight portion of wherein each component is as follows：
Lithium ion solvent：100 parts（1.15mol/L, lithium salts is LiBF4）, 10 parts of terephthalic acid monomers；1,2- propane diamine bodies,
Ethylenediamine is 1 according to mol ratio:1 gross weight is 10 parts；Two kinds of prepolymers are respectively cross-linking agent and the initiation of 10 parts and normal amount
Agent.
Specific embodiment 2：
By M-phthalic acid respectively with 4-methyl-diaminopropane, N, double (3- aminopropyls) -1,4- butanediamine of N'-, according to mol ratio
For 1:1 ratio is polymerized to form two kinds of performed polymers, and the molecular weight control of described performed polymer is being less than 3000.
By Allyl carbonate lithium ion solvent, cross-linker divinylbenzene, initiator, M-phthalic acid monomer and tetramethyl
Propane diamine, N, double (3- aminopropyls) -1,4- butanediamine of N'- proportionally mix.
Stir, at room temperature, its infiltration is penetrated in barrier film and positive and negative pole material with vacuum liquid filling equipment；Sealing
Above-mentioned mixing, and fully infiltrating barrier film more than 1 hour；The polymerization at 30 DEG C -70 DEG C forms colloid.
The weight portion of wherein each component is as follows：
Lithium ion solvent：100 parts（1.8mol/L, lithium salts is LiClO4）, 10 parts of M-phthalic acid monomer；4-methyl-diaminopropane,
Double (3- the aminopropyls) -1,4- butanediamine of N, N'- are 1 according to mol ratio:1 gross weight is 10 parts；Two kinds of prepolymers are respectively 10 parts
With the cross-linking agent and initiator of normal amount.
Specific embodiment 3：
It is respectively 1 according to mol ratio with 1,3- propane diamine, ethylenedistearamide by phthalic acid:1 ratio is polymerized to be formed
Two kinds of performed polymers, the molecular weight control of described performed polymer is being less than 3000.
By dimethyl carbonate lithium ion solvent, cross-linker divinylbenzene, initiator, phthalic acid and 1,3- the third two
Amine, ethylenedistearamide proportionally mix.
Stir, at room temperature, its infiltration is penetrated in barrier film and positive and negative pole material with vacuum liquid filling equipment；Sealing
Above-mentioned mixing, and fully infiltrating barrier film more than 1 hour；The polymerization at 35 DEG C forms colloid.
Lithium ion solvent：100 parts（1.7mol/L, LiAsF6）, 10 parts of O-phthalic acid monomers；It is 1,3- propane diamine, two hard
Acyl ethylenediamine is 1 according to mol ratio:1 gross weight is 10 parts；Two kinds of prepolymers are respectively the cross-linking agent of 10 parts and normal amount and draw
Send out agent.
Specific embodiment 4：
By oreinol diacid respectively with 2- methyl isophthalic acids, 4- phenylenediamines, 1,3- propane diamine according to mol ratio be 1:1 ratio is gathered
Close and form two kinds of performed polymers, the molecular weight control of described performed polymer is being less than 3000.
By butylene carbonic ester, initiator, oreinol diacid and 2- methyl isophthalic acids, 4- phenylenediamines, 1,3- propane diamine according to
Ratio mixes.
Stir, at room temperature, its infiltration is penetrated in barrier film and positive and negative pole material with vacuum liquid filling equipment；Sealing
Above-mentioned mixing, and fully infiltrating barrier film more than 1 hour；The polymerization at 0 DEG C forms colloid.
Lithium ion solvent：100 parts（1.5mol/L, lithium salts is LiCF3SO3）, 10 parts of oreinol diacid monomer；2- first
Base -1,4- phenylenediamines, 1,3- propane diamine are 1 according to mol ratio:1 gross weight is 10 parts；Two kinds of prepolymers are respectively 10 parts and normal
The cross-linking agent and initiator of amount.
Specific embodiment 5：
It is respectively 1 according to mol ratio with 1,3- propane diamine, ethylenedistearamide by 4- chloro-o-phthalic acids:1 ratio polymerization
Two kinds of performed polymers are formed, the molecular weight control of described performed polymer is being less than 3000.
By ethylene carbonate lithium ion solvent, cross-linker divinylbenzene, initiator, 4- chloro-o-phthalic acids and 1,3- third
Diamidogen, ethylenedistearamide proportionally mix.
Stir, at room temperature, its infiltration is penetrated in barrier film and positive and negative pole material with vacuum liquid filling equipment；Sealing
Above-mentioned mixing, and fully infiltrating barrier film more than 1 hour；The polymerization at 60 DEG C forms colloid.
Lithium ion solvent：100 parts（1.8mol/L, lithium salts is LiClO4）, 10 parts of 4- chlore O-phthalic acids acid monomers；1,3- third
Diamidogen, ethylenedistearamide are 1 according to mol ratio:1 gross weight is 10 parts；Two kinds of prepolymers are respectively the friendship of 10 parts and normal amount
Connection agent and initiator.
Specific embodiment 6：
By oreinol diacid, respectively 1,2- phenylenediamines bromo- with 4-, 3- nitro -1,2- phenylenediamines are 1 according to mol ratio:1
Ratio is polymerized to form two kinds of performed polymers, and the molecular weight control of described performed polymer is being less than 3000.
Allyl carbonate lithium ion solvent, cross-linker divinylbenzene, initiator, oreinol diacid and 4- is bromo-
1,2- phenylenediamines, 3- nitro -1,2- phenylenediamines proportionally mix.
Stir, at room temperature, its infiltration is penetrated in barrier film and positive and negative pole material with vacuum liquid filling equipment；Sealing
Above-mentioned mixing, and fully infiltrating barrier film more than 1 hour；The polymerization at 35 DEG C forms colloid.
Lithium ion solvent：100 parts（1.8mol/L, lithium salts is LiAsF6）, 10 parts of oreinol diacid monomer；4- is bromo-
1,2- phenylenediamines, 3- nitro -1,2- phenylenediamines are 1 according to mol ratio:1 gross weight is 10 parts；Two kinds of prepolymers be respectively 10 parts and
The cross-linking agent and initiator of normal amount.
Performance measurement to electrolyte is as follows：
Claims (10)
1. a kind of gel polymer lithium ion electrolyte, including inorganic salt, organic solvent, polymer, cross-linking agent, initiator, its
It is characterised by, described polymer monomer raw material includes a kind of dicarboxylic acid monomer containing benzene ring structure and two kinds of diamine monomers.
2. gel polymer lithium ion electrolyte according to claim 1, it is characterised in that described containing benzene ring structure
Binary acid is selected from：P-phthalic acid, M-phthalic acid, phthalic acid, 2,2'- biphenyl dicarboxylic acids, 4,4'- diphenyl dicarboxylic acids；
4- chloro-o-phthalic acids, oreinol diacid.
3. the gel polymer lithium ion electrolyte according to any one of claim 1 or 2, it is characterised in that described two
Plant diamine monomer to be selected from：1,2- propane diamine bodies, ethylenediamine, 4-methyl-diaminopropane, N, double (3- the aminopropyls) -1,4- fourths two of N'-
Amine, 2- methyl isophthalic acids, 4- phenylenediamines, 1,3- propane diamine, ethylenedistearamide, 2- dimethyl-p-phenylenediamines, p-phenylenediamine, 4- are chloro-
1,2- phenylenediamines, NPD, m-diaminobenzene., 5- Trifluoromethyl-1s, the bromo- 1,2- phenylenediamines of 3- phenylenediamines, 4-, 3- nitre
Base -1,2- phenylenediamines.
4. gel polymer lithium ion electrolyte according to claim 3, it is characterised in that the raw material of described polymer
In also include the prepolymer that the described binary acid containing benzene ring structure is formed respectively with described two kinds of monomer prepolymerizations.
5. gel polymer lithium ion electrolyte according to claim 4, it is characterised in that the molecule of described prepolymer
Amount is less than 30000.
6. the gel polymer lithium ion electrolyte according to claim 1,2,4,5, it is characterised in that described inorganic salt
It is selected from：LiBF4、LiClO4、LiAsF6、LiCF3SO3.
7. the gel polymer lithium ion electrolyte according to claim 1,2,4,5, it is characterised in that described is organic molten
Agent is selected from ethylene carbonate, Allyl carbonate, diethyl carbonate dimethyl carbonate, methyl ester, butylene carbonic ester, acetone, methyl fourth
Ketone, methylisobutylketone, glycol monoethyl ether, ethylene glycol monoethyl ether, ethylene glycol monobutyl ether, methyl acetate, ethyl acetate, acetic acid third
Ester.
8. the gel polymer lithium ion electrolyte according to claim 1,2,4,5, it is characterised in that described cross-linking agent
Selected from divinylbenzene, N,N methylene bis acrylamide.
9. a kind of lithium ion battery, including positive electrode, negative material, lithium-ion membrane and electrolyte, it is characterised in that institute
The electrolyte stated is the electrolyte described in any one of claim 1-8.
10. a kind of preparation method of lithium ion battery, it is characterised in that comprise the following steps：
By inorganic salt, organic solvent, cross-linking agent, initiator, a kind of dicarboxylic acid monomer containing benzene ring structure and two kinds of diamine monomers
Proportionally mix with the prepolymerized prepolymer of two kinds of diamine monomers respectively according to above-mentioned dicarboxylic acid monomer, stir, in room
Under temperature, its infiltration is set to penetrate in barrier film and positive and negative pole material with vacuum liquid filling equipment；
Above-mentioned mixing is sealed, and is fully infiltrating barrier film more than 1 hour；
The polymerization at 30 DEG C -70 DEG C forms colloid.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201611071945.8A CN106611874A (en) | 2016-11-29 | 2016-11-29 | Gel polymer lithium-ion electrolyte and battery containing same |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201611071945.8A CN106611874A (en) | 2016-11-29 | 2016-11-29 | Gel polymer lithium-ion electrolyte and battery containing same |
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| Publication Number | Publication Date |
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| CN106611874A true CN106611874A (en) | 2017-05-03 |
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| CN201611071945.8A Pending CN106611874A (en) | 2016-11-29 | 2016-11-29 | Gel polymer lithium-ion electrolyte and battery containing same |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107446147A (en) * | 2017-09-22 | 2017-12-08 | 合肥工业大学 | A kind of preparation method of electricity induction selfreparing Nanometer composite hydrogel |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001043896A (en) * | 1999-07-29 | 2001-02-16 | Hitachi Chem Co Ltd | Manufacture of polymeric solid electrolyte, polymeric solid electrolyte, and electrochemical device |
| CN1285375A (en) * | 1999-08-20 | 2001-02-28 | 中国科学院化学研究所 | Gel polymer solid electrolyte and preparation process and use thereof |
| US20130273423A1 (en) * | 2012-04-16 | 2013-10-17 | Samsung Sdi Co., Ltd. | Water soluble binder composition, method of producing the same and electrode for rechargeable battery employing the same |
-
2016
- 2016-11-29 CN CN201611071945.8A patent/CN106611874A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001043896A (en) * | 1999-07-29 | 2001-02-16 | Hitachi Chem Co Ltd | Manufacture of polymeric solid electrolyte, polymeric solid electrolyte, and electrochemical device |
| CN1285375A (en) * | 1999-08-20 | 2001-02-28 | 中国科学院化学研究所 | Gel polymer solid electrolyte and preparation process and use thereof |
| US20130273423A1 (en) * | 2012-04-16 | 2013-10-17 | Samsung Sdi Co., Ltd. | Water soluble binder composition, method of producing the same and electrode for rechargeable battery employing the same |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107446147A (en) * | 2017-09-22 | 2017-12-08 | 合肥工业大学 | A kind of preparation method of electricity induction selfreparing Nanometer composite hydrogel |
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