CN108155324A - A kind of lithium ion battery difunctional application type diaphragm and preparation method thereof - Google Patents
A kind of lithium ion battery difunctional application type diaphragm and preparation method thereof Download PDFInfo
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- CN108155324A CN108155324A CN201711377716.3A CN201711377716A CN108155324A CN 108155324 A CN108155324 A CN 108155324A CN 201711377716 A CN201711377716 A CN 201711377716A CN 108155324 A CN108155324 A CN 108155324A
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- Prior art keywords
- lithium ion
- ion battery
- diaphragm
- application type
- coating
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/403—Manufacturing processes of separators, membranes or diaphragms
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/463—Separators, membranes or diaphragms characterised by their shape
-
- 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 present invention relates to a kind of lithium ion battery difunctional application type diaphragms and preparation method thereof, it is using porous polyolefin diaphragm as base material, unilateral or bilateral coating is carried out to the porous olefin film with the particles of inorganic material with cation exchange and high-temperature stability.Lithium ion battery separator after coated, on the one hand due to the thermal stability of this height of inorganic matter, in higher temperature, polymer melts, and the presence of inorganic matter then maintains the integrality of lithium ion battery separator, can improve the heat-resisting quantity of diaphragm;In addition, the inorganic matter of surface coating can adsorb the ferrous ion that lithium ion cell positive LiFePO4 discharges in cyclic process, it is avoided to diffuse to cathodic reduction and causes battery micro-short circuit for iron simple substance, allow the capacity of lithium ion battery keep for a long time and its may caused by the safety problems such as spontaneous combustion.
Description
Technical field
The invention belongs to new energy materials field, specifically design a kind of difunctional application type diaphragm of lithium ion battery and its
Preparation method.
Background technology
In the past few decades, the transition of the development of lithium ion battery from miniature device energy storage to power battery constantly changes
The life style of philanthropists.In lithium ion battery, diaphragm is a kind of very important component, can prevent anode and cathode it
Between contact, while also have the function of to pass through electrolyte ion, structure and performance determine the interfacial structure, interior of battery
Resistance etc., directly affects the characteristics such as capacity, cycle and the security performance of battery.All the time, the safety of lithium ion battery is asked
Topic is concerned, and particularly lithium ion battery separator of the research and development with good thermal stability receives favor.Currently on the market often
Lithium ion battery separator is polypropylene and polyethylene kind diaphragm, but with the continuous promotion of energy requirement, inside battery
Overcharge and let pass with crossing as can be so that internal temperature of battery constantly rises, membrane for polymer melts, positive and negative anodes short circuit, cause lithium from
The drastically decline of sub- battery capacity, the even spontaneous combustion of battery with it is on fire.
Currently, the major measure for improving diaphragm heat-resisting quantity is with the high score compared with high temperature tolerance in membrane surface coating
The mixed coating of son, inorganic oxide or both.Coating is is dispersed in the solvent containing binding agent, then will by specific method
It forms stable diaphragm coating coated on membrane surface.Patent CN201510012242.7 discloses a kind of aqueous ceramic diaphragm
The method of slurry, slurry are formed by including alumina powder, aqueous binders, filler.201610332945.2 disclosures of patent CN
A kind of palygorskite/alumina composite lithium ion battery coating diaphragm and preparation method thereof.Patent CN201310140933.6 is public
A kind of polyolefin/inorganic matter composite diaphragm of particles of inorganic material coating coating is opened, inorganic matter employs silicon, aluminium, calcium, titanium and barium
Oxide, nitride or carbide, improve the porosity of basement membrane and the heat resistance of composite diaphragm.But they exist
Some problems, one side macromolecule, inorganic oxide coating price be not low, while increases the thickness of diaphragm, to a certain degree
On reduce battery energy density and improve manufacture cost;On the other hand, the LiFePO4 lithium larger as a kind of accounting
Ion battery positive electrode itself has good cycle performance, but the reaction of the solid-phase sintering of LiFePO4 is one multiple
Miscellaneous heterogeneous reaction, stronger reducing atmosphere during ferric ion is reduced into positive ferrous ion, exist by
Positive ferrous ion is further reduced into the possibility of micro fe;In addition, one outstanding feature of solid phase reaction is reaction
Retarder theory and no thoroughness, this so that there are micro Fes in LiFePO42O3Possibility, Fe2O3In charge and discharge cycles mistake
The precipitation of dissolving and fe on cathode in journey.The presence of fe can cause internal short-circuit of battery, can cause battery
Capacity declines.Patent CN201510576236.4 discloses the side generated in a kind of ferric phosphate lithium cell preparation process without fe
Method, this method first prepare the zymotic fluid and potassium bichromate, silver sulfate, the concentrated sulfuric acid of the solution of potassium sulfate and calcium sulfate and acid molten
Liquid three mixes, and is put into the high temperature furnace of reducing atmosphere and calcines after potassium phosphate, iron oxide, graphite powder are mixed, you can
Obtain the lithium iron phosphate cell material of no fe generation.This method introduces many additional raw material components, increases making
Cost and manufacture craft.And for the generation of iron ion in cyclic process, dissociate to cathodic reduction for iron this process then without compared with
Good solution.
In order to overcome this problem, it is necessary to propose a kind of method, lithium ion battery can be promoted at lower cost simultaneously
The thermal stability of diaphragm, and diffusion of the ferrous ion between positive and negative anodes is inhibited to maintain membrane integrity, keep lithium-ion electric
Pond is run safe efficiently.
Invention content
The technical problems to be solved by the invention are to provide a kind of difunctional in view of the deficiency of the prior art
Application type diaphragm, particles of inorganic material coating cause the temperature tolerance of diaphragm to be improved, while are adsorbed in battery by ion exchange
The iron ion that portion dissociates inhibits short circuit.
The present invention is solves the problems, such as that used technical solution set forth above is:
A kind of difunctional application type diaphragm of lithium ion battery, using porous polyolefin diaphragm as base material, the unilateral side of base material or
Two-sided coatings organic/inorganic substance particle is the coating of main material, which has the function of cation exchange and high-temperature stability.
By said program, the porous olefin diaphragm draws polypropylene diaphragm, dry method are double to draw polypropylene diaphragm for dry method list
Or any one in wet method polyethylene diagrams etc..
By said program, the porous olefin membrane thicknesses are 5~60um, and porosity is 30~50%.
By said program, the particles of inorganic material is that the coating layer thickness of main material is 3~20um;Particles of inorganic material size
For 0.2~1um.
By said program, the inorganic matter is any one in kaolin, analcime, hydroxyapatite etc..
The present invention also provides the above-mentioned lithium ion battery preparation methods of difunctional application type diaphragm, mainly comprise the following steps:
The coating sizing-agent of particles of inorganic material is configured in the first step:Particles of inorganic material, binding agent, dispersant and solvent are mixed
Uniformly, more uniform coating sizing-agent is obtained;
Second step, coating coating:The coating sizing-agent that the first step is prepared is applied to porous olefin diaphragm unilateral or bilateral, is done
After dry, the lithium ion battery separator that particles of inorganic material is main material coating, i.e., the difunctional coating of described lithium ion battery are obtained
Type diaphragm.
By said program, the particles of inorganic material, binding agent, dispersant and solvent quality ratio are 1:(0.5~2):(0.05
~0.5):(5~25) it is uniformly mixed, usually stirs 0.5~2h and be uniformly mixed.
By said program, the binding agent is Vingon, polytetrafluoroethylene (PTFE), polyacrylic acid and polyacrylonitrile polymerize
One kind or arbitrary several combination in object etc.;Solvent is arbitrary in N-Methyl pyrrolidone, n,N-Dimethylformamide etc.
It is a kind of;Dispersant is any one in polyvinylpyrrolidone, polyvinyl alcohol etc..
By said program, the coating method is any one in blade coating, roller coating or spraying etc..
Compared with prior art, the beneficial effects of the invention are as follows:
The present invention is for short inside caused by iron in the high cost of existing ceramic coated lithium-ion membrane, iron phosphate lithium positive pole
The problems such as road, provides a kind of lithium ion battery difunctional application type diaphragm and preparation method thereof, through in porous polyolefin diaphragm
The unilateral or bilateral coating inorganic composition granule of base material is the coating of main material, on the one hand, due to the thermostabilization of this height of inorganic matter
Property, in higher temperature, polymer melts, and the presence of inorganic matter then maintains the integrality of lithium ion battery separator, can improve
The heat-resisting quantity of diaphragm;On the other hand, the inorganic matter of surface coating can adsorb lithium ion cell positive phosphorus by ion exchange
The ferrous ion that sour iron lithium discharges in cyclic process avoids it from diffusing to cathodic reduction and causes battery micro- short for iron simple substance
The safety problems such as spontaneous combustion, make battery maintain higher capacity, and protect after prolonged cycle caused by road and its possibility
The more safe and efficient operation of lithium ion battery is demonstrate,proved.
Specific embodiment
For a better understanding of the present invention, with reference to the embodiment content that the present invention is furture elucidated, but the present invention
Content is not limited solely to the following examples.
Embodiment 1
A kind of difunctional application type diaphragm of lithium ion battery, using dry method list draw polypropylene porous septum (thickness as 5um,
Porosity is that coating of the kaolin particle (particle size 0.2um) for main material 30%) is coated on base material table for base material
Face forms coating layer thickness as 3um.
The above-mentioned lithium ion battery preparation method of difunctional application type diaphragm, specific steps:
(1) by kaolin particle, Vingon binding agent, polyvinylpyrrolidone dispersant and N-Methyl pyrrolidone
Solvent is 1 in mass ratio:0.5:0.05:5 uniformly mixing, stir 0.5h, obtain more uniform coating sizing-agent;
(2) coating sizing-agent prepared in step (1) is applied to the dry method list in the method scratched draws polypropylene more
Hole diaphragm is unilateral, in 60 DEG C of dryings, obtains the lithium ion battery separator that kaolin particle is main material coating, i.e., described lithium ion
The difunctional application type diaphragm of battery.
In embodiment 1 and following other embodiments, porosity is measured using Gurley Permeability gauges;It is followed using ICP tests
Ring 200 encloses the content of ferro element in cathode, and it for positive electrode, Delanium is cathode, 1mol/L LiPF6/ to use LiFePO4
EC:DMC:DEC (v/v/v) assembles button cell for electrolyte, is heated up, adopted with the speed of 0.1 DEG C/min in environmental test chamber
Temperature when short circuit occurs is measured with electrochemical workstation, with battery capacity retention after 200 circle of blue electrical testing 1C cycles.It is every
Index is shown in Table 1.
Drawing polypropylene porous septum using uncoated dry method list, thickness is that 30um porositys are 40%, respectively as comparative example
Item index is also shown in Table 1.
Embodiment 2
A kind of difunctional application type diaphragm of lithium ion battery, using dry method it is double draw polypropylene porous septums (thickness as 60um,
Porosity is that coating of the analcime particle (particle size 1um) for main material 50%) is coated on substrate surface for base material,
Formed coating layer thickness is 20um.
The above-mentioned lithium ion battery preparation method of difunctional application type diaphragm, specific steps:
(1) by analcime particle, polytetrafluoroethylene (PTFE) binding agent, polyvinyl alcohol and n,N-Dimethylformamide dispersant solvent
It is 1 in mass ratio:2:0.5:25 uniformly mixing, stir 2h, obtain more uniform coating sizing-agent;
(2) coating sizing-agent prepared in step (1) is applied to the dry method pair in the method for roller coating draws polypropylene more
Hole diaphragm both sides in 80 DEG C of dryings, obtain the lithium ion battery separator that analcime particle is main material coating, i.e., described lithium ion
The difunctional application type diaphragm of battery.
Embodiment 3
A kind of difunctional application type diaphragm of lithium ion battery, using wet method polyethylene porous separator (thickness as 20um, hole
It 42%) be base is base material that rate, which is, and coating of the hydroapatite particles (particle size 0.5um) for main material is coated on base material
Surface forms coating layer thickness as 4um.
The above-mentioned lithium ion battery preparation method of difunctional application type diaphragm, specific steps:
(1) by hydroapatite particles, polyacrylic acid binding agent, polyvinylpyrrolidone dispersant and N- crassitudes
Ketone solvent is 1 in mass ratio:1:0.1:10 uniformly mixing, stir 1h, obtain more uniform coating sizing-agent;
(2) by the coating sizing-agent prepared in step (1) with the method sprayed be applied to the wet method polyethylene porous every
Film is unilateral, in 70 DEG C of dryings, obtains the lithium ion battery separator that hydroapatite particles are main material coating, i.e., described lithium ion
The difunctional application type diaphragm of battery.
Embodiment 4
A kind of difunctional application type diaphragm of lithium ion battery, using dry method list draw polypropylene porous septum (thickness as 16um,
Porosity is that coating of the hydroapatite particles (particle size 0.7um) for main material 46%) is coated on base material for base material
Surface forms coating layer thickness as 6um.
The above-mentioned lithium ion battery preparation method of difunctional application type diaphragm, specific steps:
(1) it is hydroapatite particles, the fine binding agent of polypropylene, polyvinyl alcohol dispersant and n,N-Dimethylformamide is molten
Agent is 1 in mass ratio:0.5:0.2:15 uniformly mixing, stir 0.5h, obtain more uniform coating sizing-agent;
(2) coating sizing-agent prepared in step (1) is applied to the dry method list in the method scratched draws polypropylene more
Hole diaphragm bilateral in 60 DEG C of dryings, obtains the lithium ion battery separator that hydroapatite particles are main material coating, i.e., described lithium
The difunctional application type diaphragm of ion battery.
The difunctional application type diaphragm experimental data of lithium ion battery prepared by 1 embodiment of table
Embodiment 1 | Embodiment 2 | Embodiment 3 | Embodiment 4 | Comparative example | |
Porosity | 38 | 49 | 40 | 45 | 27 |
Battery cathode iron content (%) | 0 | 0 | 0 | 0 | 1.2 |
Short-circuit temperature (DEG C) | 340 | 355 | 347 | 344 | 175 |
Capacity retention | 95.5 | 97.1 | 93.2 | 94.4 | 60 |
The above is only the preferred embodiment of the present invention, it is noted that those of ordinary skill in the art are come
It says, without departing from the concept of the premise of the invention, several modifications and variations can also be made, these belong to the present invention's
Protection domain.
Claims (8)
1. the difunctional application type diaphragm of a kind of lithium ion battery, it is characterised in that it is using porous polyolefin diaphragm as base material, base
The unilateral or bilateral of material is coated with the coating that particles of inorganic material is main material.
2. the difunctional application type diaphragm of a kind of lithium ion battery according to claim 1, it is characterised in that described is more
Hole alkene diaphragm draws any one in the double drawing polypropylene diaphragms of polypropylene diaphragm, dry method or wet method polyethylene diagrams for dry method list
Kind.
3. the difunctional application type diaphragm of a kind of lithium ion battery according to claim 1, it is characterised in that described is more
Hole alkene membrane thicknesses are 5~60 μm, and porosity is 30~50%.
A kind of 4. difunctional application type diaphragm of lithium ion battery according to claim 1, it is characterised in that the nothing
Machine composition granule is that the coating layer thickness of main material is 3~20 μm;Particles of inorganic material size is 0.2~1 μm.
A kind of 5. difunctional application type diaphragm of lithium ion battery according to claim 1, it is characterised in that the nothing
Machine object is kaolin, any one in analcime, hydroxyapatite.
6. the preparation method of the difunctional application type diaphragm of lithium ion battery in claim 1-5 described in any one, special
Sign is to mainly comprise the following steps:
The coating sizing-agent of particles of inorganic material is configured in the first step:Particles of inorganic material, binding agent, dispersant and solvent are uniformly mixed,
Obtain coating sizing-agent;
Second step, coating coating:The coating sizing-agent that the first step is prepared is applied to porous olefin diaphragm unilateral or bilateral, it is dry
Afterwards, the lithium ion battery is obtained with difunctional application type diaphragm.
7. a kind of lithium ion battery according to claim 6 preparation method of difunctional application type diaphragm, feature exist
In the particles of inorganic material, binding agent, dispersant and solvent quality ratio be 1:(0.5~2):(0.05~0.5):(5~25) it mixes
It closes uniform.
8. a kind of lithium ion battery according to claim 6 preparation method of difunctional application type diaphragm, feature exist
In the binding agent be one kind in Vingon, polytetrafluoroethylene (PTFE), polyacrylic acid and polyacrylonitrile polymer or arbitrary
Several combinations;Solvent is any one in N-Methyl pyrrolidone, n,N-Dimethylformamide;Dispersant is polyethylene pyrrole
Any one in pyrrolidone, polyvinyl alcohol.
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Cited By (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN108923013A (en) * | 2018-07-10 | 2018-11-30 | 福建师范大学 | Coating diaphragm preparation method containing PMMA and P-C key simultaneously |
CN108963161A (en) * | 2018-07-10 | 2018-12-07 | 福建师范大学 | Coating membrane preparation method containing dibasic phosphates and phosphorus carbon valence link |
CN109504226A (en) * | 2018-11-27 | 2019-03-22 | 河北金力新能源科技股份有限公司 | Polyacrylonitrile diaphragm coating liquid, lithium electric separator and lithium battery |
CN109755641A (en) * | 2019-03-18 | 2019-05-14 | 珠海光宇电池有限公司 | A kind of composite material and preparation method and lithium ion battery |
CN113314801A (en) * | 2021-05-21 | 2021-08-27 | 中南大学 | Slow-release functional diaphragm, preparation method thereof and lithium battery |
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CN1239591A (en) * | 1997-05-12 | 1999-12-22 | 日本工业技术院长代表之日本国 | Separator for battery and alkali secondary battery using same |
CN101038960A (en) * | 2006-03-17 | 2007-09-19 | 三洋电机株式会社 | Non-aqueous electrolyte battery |
US20170288226A1 (en) * | 2016-03-30 | 2017-10-05 | Sumitomo Osaka Cement Co., Ltd. | Lithium-ion secondary battery |
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CN1239591A (en) * | 1997-05-12 | 1999-12-22 | 日本工业技术院长代表之日本国 | Separator for battery and alkali secondary battery using same |
CN101038960A (en) * | 2006-03-17 | 2007-09-19 | 三洋电机株式会社 | Non-aqueous electrolyte battery |
US20170288226A1 (en) * | 2016-03-30 | 2017-10-05 | Sumitomo Osaka Cement Co., Ltd. | Lithium-ion secondary battery |
Cited By (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN108923013A (en) * | 2018-07-10 | 2018-11-30 | 福建师范大学 | Coating diaphragm preparation method containing PMMA and P-C key simultaneously |
CN108963161A (en) * | 2018-07-10 | 2018-12-07 | 福建师范大学 | Coating membrane preparation method containing dibasic phosphates and phosphorus carbon valence link |
CN108923013B (en) * | 2018-07-10 | 2021-05-14 | 福建师范大学 | Preparation method of coating diaphragm containing PMMA and P-C bonds simultaneously |
CN108963161B (en) * | 2018-07-10 | 2021-05-14 | 福建师范大学 | Method for producing coating films containing divalent phosphates and carbon bonds of phosphorus |
CN109504226A (en) * | 2018-11-27 | 2019-03-22 | 河北金力新能源科技股份有限公司 | Polyacrylonitrile diaphragm coating liquid, lithium electric separator and lithium battery |
CN109755641A (en) * | 2019-03-18 | 2019-05-14 | 珠海光宇电池有限公司 | A kind of composite material and preparation method and lithium ion battery |
CN109755641B (en) * | 2019-03-18 | 2021-05-11 | 珠海冠宇电池股份有限公司 | Composite material for lithium ion battery, preparation method of composite material and lithium ion battery |
CN113314801A (en) * | 2021-05-21 | 2021-08-27 | 中南大学 | Slow-release functional diaphragm, preparation method thereof and lithium battery |
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Application publication date: 20180612 |