CN112259909A - Lithium ion battery composite diaphragm with multifunctional alternate segmented coating - Google Patents
Lithium ion battery composite diaphragm with multifunctional alternate segmented coating Download PDFInfo
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- CN112259909A CN112259909A CN201910594454.9A CN201910594454A CN112259909A CN 112259909 A CN112259909 A CN 112259909A CN 201910594454 A CN201910594454 A CN 201910594454A CN 112259909 A CN112259909 A CN 112259909A
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- 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 field of battery structures, and discloses a lithium ion battery composite diaphragm with a multifunctional alternate segmented coating, aiming at the problems of more coating film layers or less polar material contained in a coating and low ion transmittance. The invention has the following beneficial effects: (1) the thickness of the battery core is reduced, and the ion diffusion distance is shortened, so that the multiplying power performance of the battery is improved, and the internal resistance of the battery is reduced; (2) ion concentration gradients can be formed in the polyvinylidene fluoride coating layer and the ceramic coating layer on the same side, so that ion concentration pressure waves can be formed, and ions can be promoted to permeate from the polyvinylidene fluoride coating layer more easily; (3) the coating has thermal stability and better battery rate.
Description
Technical Field
The invention relates to the field of battery structures, in particular to a lithium ion battery composite diaphragm with a multifunctional alternate segmented coating.
Background
As a diaphragm of a lithium ion battery, polyethylene or polypropylene diaphragm materials are poor in air permeability and lyophilic property, and the materials are poor in thermal stability, when the temperature reaches a certain value, the diaphragm is fused, so that the positive electrode and the negative electrode are in direct contact, the internal short circuit of the battery is generated, and finally the battery is in failure. Therefore, at present, a multifunctional coating is added on the surface of the film, which is beneficial to the performance optimization of the diaphragm material, for example, the patent number is CN201620057305.0, the patent name is a patent of a coating diaphragm structure for the lithium ion battery, and the film comprises a base film, a surface pretreatment layer, a closed pore functional coating, a heat-resistant ceramic layer, a bonding layer, a polyvinylidene fluoride layer, a blocking layer and an antibacterial layer, wherein the base film, the surface pretreatment layer, the closed pore functional coating, the heat-resistant ceramic layer, the bonding layer, the polyvinylidene fluoride layer, the blocking layer and the antibacterial layer are sequentially arranged from. The utility model discloses a coating diaphragm structure for lithium ion battery has high strength, multi-functional resistant organic solvent and corrodes and high temperature resistance, has improved lithium ion battery's security and life cycle, and the structure is reliable, and is with low costs. The invention discloses a low-permeability ceramic coating diaphragm for a lithium ion battery, which is characterized in that the diaphragm is provided with a patent number of CN201810557608.2 and a patent name of the diaphragm is a low-permeability ceramic coating diaphragm for the lithium ion battery and a preparation method of the diaphragm: the diaphragm consists of a porous polymer film layer and a low-permeability ceramic coating coated on the porous polymer film layer, wherein the low-permeability ceramic coating comprises nano ceramic particles, a surface modification and coating material, a dispersing agent and a binder. The advantages are that: the surface modification and coating material is added into the nano ceramic particle slurry, so that the agglomeration and sedimentation of nano ceramic particles are prevented, and the stability of the slurry is improved.
The method has the defects that the whole layer of the stacked coating is coated with glue, the number of the layers of the coating is large after later-stage hot pressing, gaps of the coating are seriously blocked, so that the wettability of electrolyte is poor, and the ion transmittance is low. Or the surface of the base film is only coated with a layer of ceramic coating, so that the content of polar materials is low, the ion transmittance is low, and the conductivity is limited.
Disclosure of Invention
The invention aims to overcome the problems of more coating film layers or less polar material contained in the coating and low ion transmittance in the prior art, and provides a lithium ion battery composite diaphragm with a multifunctional alternate segmented coating.
In order to achieve the purpose, the invention adopts the following technical scheme:
a composite diaphragm of lithium ion battery with multifunctional alternate segmented coating is characterized in that a ceramic coating and a polyvinylidene fluoride coating are alternately arranged on two sides of a base film respectively, and each unit of the ceramic coating and the polyvinylidene fluoride coating are arranged in the same coating at intervals.
The coating mode ensures the thermal shrinkage performance of the diaphragm and the thermal safety performance of the battery, obviously reduces the thickness of the diaphragm, reduces the distance between the positive and negative pole pieces, shortens the ion diffusion distance, thereby improving the rate performance of the battery and reducing the internal resistance of the battery.
Ceramic particles are in large irregular blocks in the ceramic coating, gaps formed by stacking among the particles can form large holes on the surface of the base film, the particles coated on the surface of the base film are arranged tightly, the ceramic coating can enable the diaphragm to shrink less at high temperature, the size deformation is prevented, and the probability of short circuit of the battery is reduced. The polyvinylidene fluoride layer is made of thermoplastic materials, after mould pressing is carried out again, the positive electrode materials, the base film and the negative electrode materials can be bonded more tightly, the distance between the positive electrode piece and the negative electrode piece is shortened, and the diffusion distance of lithium ions between the positive electrode piece and the negative electrode piece is shortened, so that the multiplying power performance of the battery is improved, and the internal resistance of the battery is reduced. Meanwhile, the polyvinylidene fluoride is a polar material, contains C-F bonds, is similar to the polarity of the electrolyte, is beneficial to the infiltration of the electrolyte, has good hydrophilic performance, good liquid absorption and retention properties and better ionic conductivity. Scribble polyvinylidene fluoride coating and ceramic coating in turn, polyvinylidene fluoride coating department ion permeability is higher than ceramic coating department ion permeability, so in the regional difference that just can form ion concentration of homonymy polyvinylidene fluoride coating and ceramic coating, and then form ion concentration gradient, just can form ion concentration pressure wave, impel the ion to see through from polyvinylidene fluoride coating more easily.
Preferably, the contact edge of each unit of ceramic coating and the polyvinylidene fluoride coating is in a sawtooth shape, the height of a tooth tip is 1-3 mm, and two long edges of each unit of coating are parallel all the time.
The ceramic coating and the polyvinylidene fluoride coating have different components, and the surface tension and the thermal expansion coefficient at the contact surface are different, so the cooperativity is poor. After vacuum drying, the edge is sawtooth shape, can prevent that the coating from receiving when external force acts on, along coating direction relative slip, increases the stability between the coating.
Preferably, the width of the ceramic coating is 3-5 times of that of the polyvinylidene fluoride coating.
The separator needs to have both thermal stability and battery rate performance, and when the ceramic coating is excessive, the separator has low ion transmittance, and when the ceramic coating is insufficient, the separator has poor mechanical properties and thermal stability, so that a suitable coating width ratio is required.
Preferably, the width of the ceramic coating is 6-20 mm, and the width of the polyvinylidene fluoride coating is 3-5 mm.
Preferably, an intermediate transition layer is arranged between the contact surfaces of the ceramic coating and the side edges of the polyvinylidene fluoride coating.
Preferably, the middle transition layer is made of poly-lithium-4-styrene, and the width of the middle transition layer is 1-3 mm.
In order to ensure that the compatibility between the same coating is better, the polylithium 4-styrene is introduced between the two subsection coatings to be used as a transition layer, the polylithium 4-styrene can be well bonded with a bonding agent and ceramic particles in the ceramic coating, and meanwhile, the similar compatibility between the polylithium 4-styrene and the polyvinylidene fluoride coating is better, so that the coating can become a whole with stronger bonding force. And the side chain of the poly-lithium 4-styrene has a large amount of lithium ions and has better affinity with the electrolyte.
Preferably, the ceramic coating and the polyvinylidene fluoride coating are consistent in thickness, and the thickness of the coating is 1-5 mu m.
The wettability and ionic conductivity of the coating layer on the separator slightly increase as the thickness of the coating layer increases, and the ionic conductivity is saturated when the thickness increases to a certain extent, and therefore, it is necessary to control the thickness of the coating layer within a suitable range.
Preferably, the ceramic coating is one or more of alumina, boron carbide, silicon dioxide, silicon nitride and boron nitride.
Preferably, the base film is one or more of polyethylene, polypropylene or non-woven fabrics, and the thickness of the base film is 6-25 μm.
A preparation method of a lithium ion battery composite diaphragm with a multifunctional alternate segmented coating comprises the following steps: coating slurry preparation, ozone treatment of a base film, slurry coating and vacuum drying after coating.
(1) Preparing ceramic coating slurry: adding deionized water and ceramic powder with the particle size of 0.05-1.0 mu m into stirring equipment; adding one or more of sodium polyacrylate, sodium polymetaphosphate, sodium orthophosphate, sodium silicate, sodium dodecyl sulfate and ammonia water, wherein the addition amount of the mixture is 0.5-5% of the slurry; thirdly, adding one or a mixture of more than two of N-methyl pyrrolidone, alcohol, propylene carbonate, glycerol, dimethyl sulfoxide, polyoxyethylene alkylphenol ether, polyoxyethylene fatty alcohol ether and polyvinyl alcohol, wherein the addition amount of the mixture is 0.5-10% of the slurry; adding carboxylic styrene-butadiene rubber with the slurry amount of 0.5-10%; adding sodium carboxymethylcellulose with the pulp amount of 0.3-5% to prepare a 2% solution in advance, and stirring at a high speed in the steps I, II, III and IV and carrying out ultrasonic oscillation for 0.5-1.5 hours; turning down the rotating speed to be below 500r/min, closing ultrasonic oscillation, starting vacuum, and stirring for 0.5-1 hour;
preparing polyvinylidene fluoride coating slurry: adding polyvinylidene fluoride into N-methyl pyrrolidone in a weight ratio of 1:20, and stirring for 2 hours at 40 ℃; and then adding polyvinylpyrrolidone with the weight being 20% of that of the polyvinylidene fluoride, and stirring for 2h to obtain a polyvinylidene fluoride solution.
Preparing a lithium 4-styrene coating: the lithium 4-styrene is put into a water/N, N-dimethylacetamide mixed solvent (the volume ratio is 5/95), and mixed and stirred.
(2) Treating the diaphragm by adopting ozone, wherein the flow rate of the ozone is 1-4.5L/min, and the treatment time is 30-80 seconds; membrane pretreatment to improve the wettability of the membrane with the slurry.
(3) And (3) precise segmented alternate coating, namely placing the pretreated diaphragm on a plane coating machine, coating the prepared slurry on the polypropylene diaphragm by adopting a blade coating method, controlling the coating speed to be 5-10 m/min, and carrying out online monitoring and control on the thickness of the coating by adopting a laser or ray thickness gauge so as to ensure the uniformity of the thickness of the coating.
(4) After coating, vacuum drying is carried out for 12h at 60 ℃.
Finally obtaining the multifunctional composite diaphragm with compact structure.
Therefore, the invention has the following beneficial effects: (1) the thickness of the battery core is reduced, and the ion diffusion distance is shortened, so that the multiplying power performance of the battery is improved, and the internal resistance of the battery is reduced; (2) ion concentration gradients can be formed in the polyvinylidene fluoride coating layer and the ceramic coating layer on the same side, so that ion concentration pressure waves can be formed, and ions can be promoted to permeate from the polyvinylidene fluoride coating layer more easily; (3) the coating has thermal stability and better battery rate.
Drawings
Fig. 1 is a front view of the structure of the present invention.
Fig. 2 is a top view of the structure of the present invention.
In the figure: 1. a base film 2, a polyvinylidene fluoride coating 3, a lithium polymer 4-styrene 4, a ceramic coating 5 and a sawtooth structure.
Detailed Description
The invention is further described with reference to the following detailed description and accompanying drawings.
As shown in fig. 1 and 2, the lithium ion battery composite diaphragm with the multifunctional alternate segmented coating is characterized in that a ceramic coating and a polyvinylidene fluoride coating are alternately arranged on two sides of a base film respectively, and each unit of the ceramic coating and the polyvinylidene fluoride coating are arranged in the same coating at intervals. The contact edge of each unit ceramic coating and the polyvinylidene fluoride coating is in a sawtooth shape, the tooth tip height is 1-3 mm, and two long edges of each unit coating are parallel all the time. The width of the ceramic coating is 3-5 times of that of the polyvinylidene fluoride coating. The width of the ceramic coating is 6-20 mm, and the width of the polyvinylidene fluoride coating is 3-5 mm. An intermediate transition layer is arranged between the contact surfaces of the ceramic coating and the side edge of the polyvinylidene fluoride coating, the intermediate transition layer is made of poly-lithium-4-styrene, and the width of the intermediate transition layer is 1-3 mm. The ceramic coating and the polyvinylidene fluoride coating are consistent in thickness, and the thickness of the coating is 1-5 mu m. The ceramic coating is one or more of alumina, boron carbide, silicon dioxide, silicon nitride and boron nitride. The base film is one or more of polyethylene, polypropylene or non-woven fabrics, and the thickness of the base film is 6-25 mu m.
The manufacturing process comprises the following steps: coating slurry preparation, ozone treatment of a base film, slurry coating and vacuum drying after coating.
(1) Preparing ceramic coating slurry: adding deionized water and ceramic powder with the particle size of 0.05-1.0 mu m into stirring equipment; adding one or more of sodium polyacrylate, sodium polymetaphosphate, sodium orthophosphate, sodium silicate, sodium dodecyl sulfate and ammonia water, wherein the addition amount of the mixture is 0.5-5% of the slurry; thirdly, adding one or a mixture of more than two of N-methyl pyrrolidone, alcohol, propylene carbonate, glycerol, dimethyl sulfoxide, polyoxyethylene alkylphenol ether, polyoxyethylene fatty alcohol ether and polyvinyl alcohol, wherein the addition amount of the mixture is 0.5-10% of the slurry; adding carboxylic styrene-butadiene rubber with the slurry amount of 0.5-10%; adding sodium carboxymethylcellulose with the pulp amount of 0.3-5% to prepare a 2% solution in advance, and stirring at a high speed in the steps I, II, III and IV and carrying out ultrasonic oscillation for 0.5-1.5 hours; turning down the rotating speed to be below 500r/min, closing ultrasonic oscillation, starting vacuum, and stirring for 0.5-1 hour;
preparing polyvinylidene fluoride coating slurry: adding polyvinylidene fluoride into N-methyl pyrrolidone in a weight ratio of 1:20, and stirring for 2 hours at 40 ℃; and then adding polyvinylpyrrolidone with the weight being 20% of that of the polyvinylidene fluoride, and stirring for 2h to obtain a polyvinylidene fluoride solution.
Preparing a lithium 4-styrene coating: the lithium 4-styrene is put into a water/N, N-dimethylacetamide mixed solvent (the volume ratio is 5/95), and mixed and stirred.
(2) Treating the diaphragm by adopting ozone, wherein the flow rate of the ozone is 1-4.5L/min, and the treatment time is 30-80 seconds; membrane pretreatment to improve the wettability of the membrane with the slurry.
(3) And (3) precise segmented alternate coating, namely placing the pretreated diaphragm on a plane coating machine, coating the prepared slurry on the polypropylene diaphragm by adopting a blade coating method, controlling the coating speed to be 5-10 m/min, and carrying out online monitoring and control on the thickness of the coating by adopting a laser or ray thickness gauge so as to ensure the uniformity of the thickness of the coating.
(4) After coating, vacuum drying is carried out for 12h at 60 ℃.
Finally obtaining the multifunctional composite diaphragm with compact structure.
Example 1
Example 2
Example 3
Comparative example 1 (with respect to example 1, the ratio of the width of the ceramic coating to the width of the polyvinylidene fluoride is less than 3)
Comparative example 2 (with respect to example 1, the ratio of the width of the ceramic coating to the width of the polyvinylidene fluoride is greater than 5)
Comparative example 3 (absence of PolyLi 4-styrene coating relative to example 1)
Comparative example 4 (No sawtooth shape at the edge of coating layer with respect to example 1)
Comparative example 5 (too high coating speed compared to example 2)
Comparative example 6 (number of layers of lay-up relative to example 2)
Conclusion analysis:
in this example, the evaluation parameters of the separator were mainly six, and the evaluation parameters were average thermal shrinkage, ionic conductivity, tensile strength in the coating direction, tensile strength in the direction perpendicular to the coating direction, rate discharge performance, and internal resistance.
The average thermal shrinkage rate represents the mechanical property and the thermal stability of the membrane, and the larger the average thermal shrinkage rate is, the poorer the thermal stability of the membrane is; the larger the ionic conductivity is, the better the electrical rate performance of the diaphragm is represented; the higher the tensile strength along the coating direction is, the better the bonding performance of the membrane coatings with each other along the coating direction is; the higher the tensile strength in the direction perpendicular to the coating direction is, the better the bonding performance of the diaphragm coating along the coating direction is; the higher the rate discharge performance, the lower the internal resistance, representing the better discharge performance of the battery.
As can be seen from the data of examples 1 to 3 and comparative examples 1 to 6, the above requirements can be satisfied in all aspects only by the embodiments within the scope of the claims of the present invention. The change of the mixture ratio, the replacement/addition/subtraction of raw materials or the change of the feeding sequence can bring corresponding negative effects.
The raw materials and equipment used in the invention are common raw materials and equipment in the field if not specified; the methods used in the present invention are conventional in the art unless otherwise specified.
The above description is only a preferred embodiment of the present invention, and is not intended to limit the present invention, and all simple modifications, alterations and equivalents of the above embodiments according to the technical spirit of the present invention are still within the protection scope of the technical solution of the present invention.
Claims (10)
1. The lithium ion battery composite diaphragm with the multifunctional alternate segmented coating is characterized in that a ceramic coating and a polyvinylidene fluoride coating are alternately arranged on two sides of a base film respectively, and each unit of the ceramic coating and the polyvinylidene fluoride coating are arranged in the same coating at intervals.
2. The lithium ion battery composite membrane with the multifunctional alternate segmented coating is characterized in that the contact edge of each unit of the ceramic coating and the polyvinylidene fluoride coating is in a sawtooth shape, the tooth tip height is 1-3 mm, and two long edges of each unit of the coating are always parallel.
3. The lithium ion battery composite separator with the multifunctional alternate segmented coating as claimed in claim 1, wherein the width of the ceramic coating is 3-5 times that of the polyvinylidene fluoride coating.
4. The lithium ion battery composite separator with the multifunctional alternate segmented coating as claimed in claim 1, wherein the width of the ceramic coating is 6-20 mm, and the width of the polyvinylidene fluoride coating is 3-5 mm.
5. A lithium ion battery composite diaphragm with a multifunctional alternate segmented coating is characterized in that an intermediate transition layer is arranged between contact surfaces of the side edges of a ceramic coating and a polyvinylidene fluoride coating.
6. The lithium ion battery composite separator with the multifunctional alternate segmented coating as claimed in claim 5, wherein the intermediate transition layer is poly-lithium 4-styrene and has a width of 2-4 mm.
7. The lithium ion battery composite separator with the multifunctional alternate segmented coating as claimed in claim 1 or 2, wherein the thickness of the ceramic coating and the polyvinylidene fluoride coating is consistent, and the thickness of the coating is 1-5 μm.
8. The lithium ion battery composite membrane with the multifunctional alternate segmented coating as claimed in claim 1, wherein the ceramic coating is one or more of alumina, boron carbide, silica, silicon nitride and boron nitride.
9. The lithium ion battery composite membrane with the multifunctional alternate segmented coating is characterized in that the base membrane is one or more of polyethylene, polypropylene or non-woven fabric, and the thickness of the base membrane is 6-25 μm.
10. The preparation method of the lithium ion battery composite separator with the multifunctional alternate segmented coating according to any one of claims 1 to 9, is characterized by comprising the following steps: coating slurry preparation, ozone treatment of a base film, slurry coating and vacuum drying after coating.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114203962A (en) * | 2021-12-13 | 2022-03-18 | 珠海冠宇动力电池有限公司 | Pole piece, battery core and battery |
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| JPH08304199A (en) * | 1995-05-08 | 1996-11-22 | Ngk Insulators Ltd | Diaphragm structure |
| CN101142364A (en) * | 2005-02-09 | 2008-03-12 | Sip控股公司 | A waterproofing membrane for use on inclined surfaces |
| CN206210962U (en) * | 2016-11-26 | 2017-05-31 | 河南国能电池有限公司 | The lithium battery of multiple-protection function |
| CN206650121U (en) * | 2017-03-27 | 2017-11-17 | 天津凯普瑞特新能源科技有限公司 | A kind of high-performance lithium battery dedicated ceramic barrier film |
| CN108598338A (en) * | 2017-12-27 | 2018-09-28 | 上海恩捷新材料科技股份有限公司 | A kind of isolation film and the electrochemical appliance comprising the isolation film |
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2019
- 2019-07-03 CN CN201910594454.9A patent/CN112259909B/en active Active
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH08304199A (en) * | 1995-05-08 | 1996-11-22 | Ngk Insulators Ltd | Diaphragm structure |
| CN101142364A (en) * | 2005-02-09 | 2008-03-12 | Sip控股公司 | A waterproofing membrane for use on inclined surfaces |
| CN206210962U (en) * | 2016-11-26 | 2017-05-31 | 河南国能电池有限公司 | The lithium battery of multiple-protection function |
| CN206650121U (en) * | 2017-03-27 | 2017-11-17 | 天津凯普瑞特新能源科技有限公司 | A kind of high-performance lithium battery dedicated ceramic barrier film |
| CN108598338A (en) * | 2017-12-27 | 2018-09-28 | 上海恩捷新材料科技股份有限公司 | A kind of isolation film and the electrochemical appliance comprising the isolation film |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114203962A (en) * | 2021-12-13 | 2022-03-18 | 珠海冠宇动力电池有限公司 | Pole piece, battery core and battery |
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