CN112038542B - Fiber cloth-based lithium ion battery diaphragm and preparation method and application thereof - Google Patents
Fiber cloth-based lithium ion battery diaphragm and preparation method and application thereof Download PDFInfo
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- CN112038542B CN112038542B CN202010954305.1A CN202010954305A CN112038542B CN 112038542 B CN112038542 B CN 112038542B CN 202010954305 A CN202010954305 A CN 202010954305A CN 112038542 B CN112038542 B CN 112038542B
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention belongs to the technical field of lithium ion batteries, and discloses a fiber cloth-based lithium ion battery diaphragm and a preparation method and application thereof. The method comprises the following steps: preparing composite fine denier fiber yarns with polyolefin as a core and blended polymer as a sheath by a composite fiber spinning method technology; and then warping and weaving the composite fine denier fiber yarns into warp-weft fiber cloth or carrying out biorthogonal composite lamination on the fibers in the same direction to obtain weftless cloth, and then carrying out hot pressing by a smooth roller to obtain the fiber cloth-based lithium ion battery diaphragm. The method has simple steps, the diaphragm does not need to be coated with slurry on one side or two sides, and the battery diaphragm with high liquid absorption rate, high ionic conductivity and high mechanical property can be prepared without stretching, orienting and forming holes; the gel layer is attached to the polypropylene skeleton fiber in situ in the production process, namely, the gel polymer attached to each skeleton fiber is equivalent, so that the thickness of the fiber cloth diaphragm is uniform, and the porosity and the pore size distribution are kept constant.
Description
Technical Field
The invention belongs to the technical field of lithium ion batteries, and particularly relates to a fiber cloth-based lithium ion battery diaphragm and a preparation method and application thereof.
Background
The lithium ion battery has the advantages of high energy density, high working voltage, no memory effect, excellent cycle rate performance, environmental friendliness and the like, and is widely applied to the fields of mobile electronic digital products, electric automobiles and the like. The diaphragm is used as an important component of the battery, and the quality of the diaphragm determines the internal resistance of the battery, the adhesion with a pole piece and the use stability, and finally influences the capacity, the cycle rate performance and the safety of the battery.
Currently, commercially available separators widely used in the market mainly include polyethylene porous membranes, polypropylene porous membranes, and polypropylene/polyethylene/polypropylene composite porous membranes. However, the melting point of the polyolefin material diaphragm is relatively low, when the battery works at the temperature near the melting point of the diaphragm material for a long time, the diaphragm can be curled and contracted to generate holes so that the battery is short-circuited due to the contact of the positive electrode and the negative electrode, wherein the temperature is about 145 ℃; also, the growth of lithium dendrites affects the separator, and when the separator is pierced by dendrites, a short circuit is induced in the battery.
In contrast, heat-resistant polymers have been attracting attention in battery separators, for example, patent CN 102969470 uses polyester material as raw material to prepare a separator, but polyester cannot swell in electrolyte, cannot well bond positive and negative electrodes of a battery, has large pore diameter, is difficult to control, and also affects safety of the battery during charging and discharging. Patent CN 108448035 discloses a PP/PET/PE fiber cloth composite battery diaphragm, which dissolves polyester by alkali liquor and then heats and presses the film, and this kind of method adjusts the diaphragm aperture by controlling the distance between fibers and melting polyethylene, but reduces the controllability of diaphragm aperture, causes the diaphragm aperture to distribute unevenly, makes the battery produce local short circuit in the use and then affects the safety of the whole battery.
Disclosure of Invention
In order to overcome the defects in the prior art, the invention mainly aims to provide a preparation method of a fiber cloth-based lithium ion battery diaphragm; the method has simple steps, the diaphragm does not need to be coated with slurry on one side or two sides, and the battery diaphragm with high liquid absorption rate, high ionic conductivity and high mechanical property can be prepared without stretching, orienting and forming holes; the gel layer is attached to the polypropylene skeleton fiber in situ in the production process, namely, the gel polymer attached to each skeleton fiber is equivalent, so that the thickness of the fiber cloth diaphragm is uniform, and the porosity and the pore size distribution are kept constant.
The invention also aims to provide the fiber cloth-based lithium ion battery separator prepared by the preparation method.
The invention further aims to provide an application of the fiber cloth-based lithium ion battery separator.
The purpose of the invention is realized by the following technical scheme:
a preparation method of a fiber cloth-based lithium ion battery diaphragm comprises the following steps: preparing composite fine denier fiber yarns with polyolefin as a core and blended polymer as a sheath by a composite fiber spinning method technology; and then warping and weaving the composite fine denier fiber yarns into warp-weft fiber cloth or carrying out biorthogonal composite lamination on the fibers in the same direction to obtain weftless cloth, and then carrying out hot pressing by a smooth roller to obtain the fiber cloth-based lithium ion battery diaphragm.
In the section structure of the composite fine denier fiber, polyolefin is in an island structure, and the blended polymer is in a sea structure.
The polyolefin is a polypropylene material; the blend polymer is polyvinylidene fluoride and polymethyl methacrylate, the mass content of the polyvinylidene fluoride is 80-90%, and the content of the polymethyl methacrylate is 10-20%.
The adhesive used in the biorthogonal composite lamination process is organic silicon modified resin mixed liquid.
The organic silicon modified resin mixed solution is one of aqueous organic silicon modified acrylic acid highlight emulsion, aqueous organic silicon modified epoxy resin highlight emulsion and aqueous organic silicon modified alkyd highlight emulsion, and more than one of beta-cyclodextrin oxide, polyvinyl alcohol, hydroxyethyl cellulose, hydroxypropyl methyl cellulose and cellulose acetate phthalate is added into the organic silicon modified epoxy resin highlight emulsion; the solid content of the organic silicon modified resin in the organic silicon modified resin mixed solution is 5-20%.
The purpose of the smooth roll hot pressing is to make the polyolefin and the polymer blend more compatible, and to improve the thickness and porosity of the fiber cloth.
The fiber cloth-based lithium ion battery diaphragm prepared by the preparation method.
When the fiber cloth-based lithium ion battery diaphragm is warp and weft cloth with a fiber interweaving structure, the fiber cloth-based lithium ion battery diaphragm is formed by interweaving sea-island fibers with a coating structure, the mechanical property of interweaving points of the warp and the weft is higher than that of other areas, and the battery diaphragm can still keep a good state after being stretched and curled.
When the fiber cloth-based lithium ion battery diaphragm is a weftless cloth bonded by fibers with a unidirectional arrangement coating structure, the fiber cloth-based lithium ion battery diaphragm is formed by unidirectionally arranging, crossing and overlapping sea-island fibers with a coating structure and pressing thermoplastic resin; in the process of charging and discharging of the lithium battery, lithium dendrite is formed, but due to the fact that no interweaving point exists in the non-woven cloth, piercing energy of the tip of the lithium dendrite in the growing process can be diffused to a large range, more fibers can absorb more energy, and the piercing performance of the lithium dendrite is improved.
The fiber cloth-based lithium ion battery diaphragm is applied to the preparation of the lithium ion battery diaphragm.
Compared with the prior art, the invention has the following advantages and effects:
(1) the mechanical property, the micro-morphology and the thermal stability of the fiber cloth diaphragm can be controlled by adjusting the polymer proportion, the warp-weft ratio of the fiber cloth and the solid content of the organic silicon modified resin; the polyvinylidene fluoride and polymethyl methacrylate blend is soaked and swelled in electrolyte.
(2) The fiber yarn section diagram of the fiber cloth has a structure similar to a sea island, wherein the sea structure is a material capable of swelling in electrolyte, and the island structure is a material with high thermal stability and chemical corrosion resistance; the sea structure material in the fiber cloth is swelled in situ in the electrolyte to form polymer gel, which plays a role in isolating positive and negative electrodes, and the island structure is used as a framework support structure to provide mechanical support for the whole diaphragm; finally, the lithium ion battery diaphragm which has uniform thickness, excellent strength and high ionic conductivity and can be suitable for commercial use is formed. Lithium ions are transmitted through the amorphous phase region and the molecular chain direction of the polymer, so that the gel has the advantages of providing more ion channels, improving the charging and discharging efficiency, improving the thermal stability of the diaphragm, improving the caking property of the diaphragm and the electrode and reducing the negative influence caused by collision and bending of the battery in the using process.
Drawings
Fig. 1 is a schematic view of a composite fine denier fiber yarn section structure.
Fig. 2 is a schematic diagram of the warp and weft cloth-based battery separator of the invention.
Fig. 3 is a schematic view of the separator of the weftless fabric-based battery of the present invention.
FIG. 4 is a flow chart of a method for producing a fiber cloth-based battery separator according to the present invention.
Detailed Description
The present invention will be described in further detail with reference to examples and drawings, but the embodiments of the present invention are not limited thereto.
The flow chart of the production method of the fiber cloth-based battery separator in the following examples 1 to 8 is shown in fig. 4.
Example 1:
at room temperature, the raw materials are subjected to a hot-melt spinning technology, and then a composite fine denier fiber with a fiber section taking polypropylene as an island and a blend of polyvinylidene fluoride and polymethyl methacrylate as sea is produced by a composite spinning device, as shown in figure 1; the mass fraction of the polypropylene is 10 wt%, the mass fraction of the blend is 90 wt%, and the polyvinylidene fluoride accounts for 90 wt% of the blend. In order to ensure that the blend is better dispersed on the whole fiber diaphragm by the subsequent smooth roller hot pressing, the polypropylene fiber is controlled below 0.5 denier according to the requirement of the superfine denier fiber. The fiber cloth is warped and woven to obtain the warp and weft fiber cloth with the warp-weft ratio of 40:30, as shown in figure 2. In order to press redundant polymer blend at the interweaving points of the warps and the wefts to supplement weaving pores and uniformly distribute polypropylene fibers in the fiber membrane to ensure that the thickness of the whole fiber membrane is uniform, the fiber cloth is hot-pressed by a smooth roller at 150 ℃ to obtain the fiber cloth-based battery diaphragm, the overall performance of the film is good, and the performance test results are shown in table 1.
Example 2:
at room temperature, the raw materials are subjected to a hot-melt spinning technology, and then a composite fine denier fiber with a fiber section taking polypropylene as an island and a blend of polyvinylidene fluoride and polymethyl methacrylate as sea is produced by a composite spinning device, as shown in figure 1; the mass fraction of the polypropylene is 20 wt%, the mass fraction of the blend is 80 wt%, and the polyvinylidene fluoride accounts for 90 wt% of the blend. In order to ensure that the blend is better dispersed on the whole fiber diaphragm by the subsequent smooth roller hot pressing, the polypropylene fiber is controlled below 0.5 denier according to the requirement of the superfine denier fiber. The fiber cloth is warped and woven to obtain the warp and weft fiber cloth with the warp-weft ratio of 40:20, as shown in figure 2. In order to press redundant polymer blend at the interweaving points of the warps and the wefts to supplement weaving pores and uniformly distribute polypropylene fibers in the fiber membrane to ensure that the thickness of the whole fiber membrane is uniform, the fiber cloth is hot-pressed by a smooth roller at 150 ℃ to obtain the fiber cloth-based battery diaphragm, the overall performance of the film is good, and the performance test results are shown in table 1.
Example 3:
at room temperature, the raw materials are subjected to a hot-melt spinning technology, and then a composite fine denier fiber with a fiber section taking polypropylene as an island and a blend of polyvinylidene fluoride and polymethyl methacrylate as sea is produced by a composite spinning device, as shown in figure 1; the mass fraction of the polypropylene is 20 wt%, the mass fraction of the blend is 80 wt%, and the polyvinylidene fluoride accounts for 80 wt% of the blend. In order to ensure that the blend is better dispersed on the whole fiber diaphragm by the subsequent smooth roller hot pressing, the polypropylene fiber is controlled below 0.5 denier according to the requirement of the superfine denier fiber. The fiber cloth is warped and woven to obtain the warp and weft fiber cloth with the warp-weft ratio of 30:20, as shown in figure 2. In order to press out redundant polymer blend at the interweaving points of the warps and the wefts to supplement weaving pores and uniformly distribute polypropylene fibers in the fiber membrane to ensure that the thickness of the whole fiber membrane is uniform, the fiber cloth is hot-pressed by a smooth roller at 150 ℃ to obtain the fiber cloth-based battery diaphragm, the overall performance of the film is general, and the performance test results are shown in table 1.
Example 4:
at room temperature, the raw materials are subjected to a hot-melt spinning technology, and then a composite fine denier fiber with a fiber section taking polypropylene as an island and a blend of polyvinylidene fluoride and polymethyl methacrylate as sea is produced by a composite spinning device, as shown in figure 1; the mass fraction of the polypropylene is 10 wt%, the mass fraction of the blend is 90 wt%, and the polyvinylidene fluoride accounts for 80 wt% of the blend. In order to ensure that the blend is better dispersed on the whole fiber diaphragm by the subsequent smooth roller hot pressing, the polypropylene fiber is controlled below 0.5 denier according to the requirement of the superfine denier fiber. The fiber cloth is warped and woven to obtain the warp and weft fiber cloth with the warp-weft ratio of 40:30, as shown in figure 2. In order to press out redundant polymer blend at the interweaving points of the warps and the wefts to supplement weaving pores and uniformly distribute polypropylene fibers in the fiber membrane to ensure that the thickness of the whole fiber membrane is uniform, the fiber cloth is hot-pressed by a smooth roller at 150 ℃ to obtain the fiber cloth-based battery diaphragm, the overall performance of the film is optimal, and the performance test results are shown in table 1.
Example 5:
at room temperature, the raw materials are subjected to a hot-melt spinning technology, and then a composite fine denier fiber with a fiber section taking polypropylene as an island and a blend of polyvinylidene fluoride and polymethyl methacrylate as sea is produced by a composite spinning device, as shown in figure 1; the mass fraction of the polypropylene is 10 wt%, the mass fraction of the blend is 90 wt%, and the polyvinylidene fluoride accounts for 90 wt% of the blend. The blend is better dispersed on the whole fiber diaphragm by the hot pressing of a subsequent smooth roller, and the polypropylene fiber is controlled below 0.5 denier according to the requirement of the superfine denier fiber. The fibers are arranged in the same direction and are biorthogonal compounded and laminated to obtain the weftless fabric, as shown in figure 3, the adhesive uses the water-based organic silicon modified acrylic acid high gloss emulsion containing beta-oxidized cyclodextrin and polyvinyl alcohol, and the solid content is 20%. In order to press redundant polymer blend at the interweaving points of the warps and the wefts to supplement weaving pores and uniformly distribute polypropylene fibers in the fiber membrane to ensure that the thickness of the whole fiber membrane is uniform, the fiber cloth is hot-pressed by a smooth roller at 150 ℃ to obtain the fiber cloth-based battery diaphragm, the overall performance of the film is good, and the performance test results are shown in table 1.
Example 6:
at room temperature, the raw materials are subjected to a hot-melt spinning technology, and then a composite fine denier fiber with a fiber section taking polypropylene as an island and a blend of polyvinylidene fluoride and polymethyl methacrylate as sea is produced by a composite spinning device, as shown in figure 1; the mass fraction of the polypropylene is 20 wt%, the mass fraction of the blend is 80 wt%, and the polyvinylidene fluoride accounts for 90 wt% of the blend. The blend is better dispersed on the whole fiber diaphragm by the hot pressing of a subsequent smooth roller, and the polypropylene fiber is controlled below 0.5 denier according to the requirement of the superfine denier fiber. The fibers are arranged in the same direction and are biorthogonal compounded and laminated to obtain the weftless fabric, as shown in figure 3, the adhesive uses the water-based organic silicon modified acrylic acid high gloss emulsion containing beta-oxidized cyclodextrin and polyvinyl alcohol, and the solid content is 10%. In order to press redundant polymer blend at the interweaving points of the warps and the wefts to supplement weaving pores and uniformly distribute polypropylene fibers in the fiber membrane to ensure that the thickness of the whole fiber membrane is uniform, the fiber cloth is hot-pressed by a smooth roller at 150 ℃ to obtain the fiber cloth-based battery diaphragm, the overall performance of the film is good, and the performance test results are shown in table 1.
Example 7:
at room temperature, the raw materials are subjected to a hot-melt spinning technology, and then a composite fine denier fiber with a fiber section taking polypropylene as an island and a blend of polyvinylidene fluoride and polymethyl methacrylate as sea is produced by a composite spinning device, as shown in figure 1; the mass fraction of the polypropylene is 10 wt%, the mass fraction of the blend is 90 wt%, and the polyvinylidene fluoride accounts for 80 wt% of the blend. The blend is better dispersed on the whole fiber diaphragm by the hot pressing of a subsequent smooth roller, and the polypropylene fiber is controlled below 0.5 denier according to the requirement of the superfine denier fiber. The fibers are arranged in the same direction and are biorthogonal compounded and laminated to obtain the weftless fabric, as shown in figure 3, the adhesive uses the water-based organic silicon modified acrylic acid high gloss emulsion containing beta-oxidized cyclodextrin and polyvinyl alcohol, and the solid content is 10%. In order to press out redundant polymer blend at the interweaving points of the warps and the wefts to supplement weaving pores and uniformly distribute polypropylene fibers in the fiber membrane to ensure that the thickness of the whole fiber membrane is uniform, the fiber cloth is hot-pressed by a smooth roller at 150 ℃ to obtain the fiber cloth-based battery diaphragm, the overall performance of the film is optimal, and the performance test results are shown in table 1.
Example 8:
at room temperature, the raw materials are subjected to a hot-melt spinning technology, and then a composite fine denier fiber with a fiber section taking polypropylene as an island and a blend of polyvinylidene fluoride and polymethyl methacrylate as sea is produced by a composite spinning device, as shown in figure 1; the mass fraction of the polypropylene is 20 wt%, the mass fraction of the blend is 80 wt%, and the polyvinylidene fluoride accounts for 80 wt% of the blend. The blend is better dispersed on the whole fiber diaphragm by the hot pressing of a subsequent smooth roller, and the polypropylene fiber is controlled below 0.5 denier according to the requirement of the superfine denier fiber. The fibers are arranged in the same direction and are biorthogonal compounded and laminated to obtain the weftless fabric, as shown in figure 3, the adhesive uses the water-based organic silicon modified acrylic acid high gloss emulsion containing beta-oxidized cyclodextrin and polyvinyl alcohol, and the solid content is 5%. In order to press redundant polymer blend at the interweaving points of the warps and the wefts to supplement weaving pores and uniformly distribute polypropylene fibers in the fiber membrane to ensure that the thickness of the whole fiber membrane is uniform, the fiber cloth is hot-pressed by a smooth roller at 150 ℃ to obtain the fiber cloth-based battery diaphragm, the overall performance of the film is good, and the performance test results are shown in table 1.
Table 1 test results of performance of the fiber cloth-based lithium ion battery separator in each example
The above embodiments are preferred embodiments of the present invention, but the present invention is not limited to the above embodiments, and any other changes, modifications, substitutions, combinations, and simplifications which do not depart from the spirit and principle of the present invention should be construed as equivalents thereof, and all such changes, modifications, substitutions, combinations, and simplifications are intended to be included in the scope of the present invention.
Claims (5)
1. A preparation method of a fiber cloth-based lithium ion battery diaphragm is characterized by comprising the following steps: preparing composite fine denier fiber yarns with polyolefin as a core and blended polymer as a sheath by a composite fiber spinning method technology; warping and weaving the composite fine denier fiber yarns into warp-weft fiber cloth or performing biorthogonal composite lamination on the fibers in the same direction to obtain weftless cloth, and performing hot pressing by using a smooth roller to obtain a fiber cloth-based lithium ion battery diaphragm; the polyolefin is a polypropylene material; the blend polymer is polyvinylidene fluoride and polymethyl methacrylate, the mass content of the polyvinylidene fluoride is 80-90%, and the content of the polymethyl methacrylate is 10-20%; the adhesive used in the biorthogonal composite lamination process is organic silicon modified resin mixed liquor, and the solid content of organic silicon modified resin in the organic silicon modified resin mixed liquor is 5-20%.
2. The preparation method of the fiber cloth-based lithium ion battery separator according to claim 1, characterized in that: in the section structure of the composite fine denier fiber, polyolefin is in an island structure, and the blended polymer is in a sea structure.
3. The preparation method of the fiber cloth-based lithium ion battery separator according to claim 1, characterized in that: the organic silicon modified resin mixed solution is one of aqueous organic silicon modified acrylic acid highlight emulsion, aqueous organic silicon modified epoxy resin highlight emulsion and aqueous organic silicon modified alkyd highlight emulsion, and more than one of beta-cyclodextrin oxide, polyvinyl alcohol, hydroxyethyl cellulose, hydroxypropyl methyl cellulose and cellulose acetate phthalate is added into the organic silicon modified epoxy resin highlight emulsion.
4. A fiber cloth-based lithium ion battery separator prepared by the preparation method of any one of claims 1 to 3.
5. The use of the fiber cloth-based lithium ion battery separator according to claim 4 in the preparation of a lithium ion battery separator.
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| CN115101888B (en) * | 2022-06-16 | 2024-03-26 | 广东工业大学 | Multistage Kong Qianwei cloth-based polymer composite membrane and preparation method and application thereof |
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| JP2019200943A (en) * | 2018-05-18 | 2019-11-21 | 三菱製紙株式会社 | Base material for lithium ion battery separator and lithium ion battery separator |
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| JPWO2014208596A1 (en) * | 2013-06-25 | 2017-02-23 | 日立化成株式会社 | Electrochemical element separator and lithium ion secondary battery |
| CN105374972B (en) * | 2015-12-14 | 2018-01-19 | 苏州锂盾储能材料技术有限公司 | A kind of lithium ion battery high-temperature-resistant membrane material and preparation method |
| CN108448035B (en) * | 2018-03-08 | 2019-05-24 | 广东蒙泰高新纤维股份有限公司 | A kind of lithium ion battery separator and its manufacturing method |
| CN108711605A (en) * | 2018-07-10 | 2018-10-26 | 深圳中兴新材技术股份有限公司 | A kind of composite battery separator film, preparation method and battery |
| CN109357571B (en) * | 2018-11-02 | 2021-05-07 | 北京航天雷特机电工程有限公司 | Comfortable stab-resistant garment and manufacturing method thereof |
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| JP2019200943A (en) * | 2018-05-18 | 2019-11-21 | 三菱製紙株式会社 | Base material for lithium ion battery separator and lithium ion battery separator |
| CN109004154A (en) * | 2018-07-23 | 2018-12-14 | 广东蒙泰高新纤维股份有限公司 | A kind of method of wet process copy paper technique manufacture diaphragm of power lithium ion battery |
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