CN212230512U - Diaphragm for lithium ion battery and lithium ion battery - Google Patents
Diaphragm for lithium ion battery and lithium ion battery Download PDFInfo
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- CN212230512U CN212230512U CN202020463359.3U CN202020463359U CN212230512U CN 212230512 U CN212230512 U CN 212230512U CN 202020463359 U CN202020463359 U CN 202020463359U CN 212230512 U CN212230512 U CN 212230512U
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Abstract
The utility model provides a diaphragm for lithium ion battery, including substrate layer and coating, the coating is in the at least one side of substrate layer, the coating is including the first coating, second coating and the third coating that set gradually, the third coating with the substrate layer is connected, the second coating is thermal-insulated aerogel layer, thermal-insulated aerogel layer's porosity is 80 ~ 99.5%. Compared with the prior art, the utility model provides a diaphragm increases the setting in coat on the substrate layer basis to adopt the porosity to be 80 ~ 99.5% aerogel coating, through the stack setting in three-layer coat, make the imbibition performance and the liquid retention performance of diaphragm all improve to some extent, solved current diaphragm imbibition ability and the poor problem of liquid retention ability. Furthermore, the utility model also provides a lithium ion battery who contains this diaphragm.
Description
Technical Field
The utility model relates to a lithium cell field, concretely relates to diaphragm and lithium ion battery for lithium ion battery.
Background
In the construction of lithium batteries, the separator is one of the key internal components. The performance of the diaphragm determines the interface structure, internal resistance and the like of the battery, directly influences the capacity, circulation, safety performance and other characteristics of the battery, and the diaphragm with excellent performance plays an important role in improving the comprehensive performance of the battery. The diaphragm is mainly used for separating the positive electrode and the negative electrode of the battery and preventing the two electrodes from contacting and being short-circuited; it is also desirable to have the ability to pass electrolyte ions. The diaphragm adopted can be different for different battery types, the physical and chemical properties of the diaphragm have great influence on the performance of the battery, and the diaphragm is usually made of non-conductive materials. In the lithium battery system, since the electrolyte is an organic solvent system, a separator material resistant to an organic solvent is required, and a polyolefin porous membrane having high strength and being thinned is generally used, and mainly includes separators such as polypropylene and polyethylene separators, propylene and ethylene copolymers, polyethylene copolymers, and the like.
However, the existing battery diaphragm has poor liquid absorption capacity and liquid retention capacity, along with the improvement of battery capacity, more and more chemical substances and higher density are contained in the battery, the diaphragm is more and more difficult to absorb electrolyte, the electrolyte cannot be completely soaked, the internal resistance of the battery is increased, the capacity of the lithium battery is reduced, and battery explosion is easily caused. In addition, the polyolefin porous membrane has large shrinkage, strong water absorption and poor dimensional stability, and is difficult to prepare high-precision products, thereby limiting the long-term use of the product.
In order to solve the above problems, chinese utility model patent (CN201420868777.5) discloses a diaphragm including a diaphragm main body and a groove provided on at least one surface of the diaphragm main body, at least one end of the groove extending to a side of the diaphragm main body. The surface of the diaphragm is provided with the grooves, so that the liquid retention capacity of the diaphragm is improved. However, the tensile strength of the separator is reduced due to the design of the grooves, and the separator is easily torn when stretched, thereby causing a series of problems in battery safety.
In view of the above, it is necessary to provide a technical solution to the above problems.
SUMMERY OF THE UTILITY MODEL
One of the purposes of the utility model lies in: through providing a diaphragm for lithium ion battery, solve the poor problem of current diaphragm imbibition ability and liquid retention ability, improve the imbibition performance and the liquid retention performance of diaphragm, and then improve the cycle life of battery, reduce the circulation of pole piece and worsen the problem.
In order to achieve the above purpose, the utility model adopts the following technical scheme:
the utility model provides a diaphragm for lithium ion battery, includes substrate layer and coat, the coating is in the at least one side of substrate layer, the coat is including the first coat, second coat and the third coat that set gradually, the third coat with the substrate layer is connected, the second coat is thermal-insulated aerogel layer, thermal-insulated aerogel layer's porosity is 80 ~ 99.5%.
The utility model provides a diaphragm increases the setting in layer on the base layer basis, through the stack setting in three-layer for diaphragm's imbibition performance and liquid retention performance all improve to some extent, have solved the poor problem of current diaphragm imbibition ability and liquid retention ability. After the electrolyte is added into the naked electric core, the residue of the liquid electrolyte in the shell is greatly reduced; meanwhile, the diaphragm is beneficial to firmly locking the electrolyte in the battery core, the cycle life of the battery is prolonged, and the problem of cycle deterioration of the pole piece is reduced; in addition, the high-temperature performance and the safety performance of the battery are improved to a certain extent, and the battery can still be in a safe state when being subjected to high temperature, puncture, impact, extrusion and the like. The aerogel coating with the porosity of 80-99.5% is adopted, so that the diaphragm can absorb and retain more electrolyte, the cycle performance of the battery is improved, and meanwhile, the heat insulation effect can be achieved; in addition, still be provided with the third coating between thermal-insulated aerogel layer and substrate layer, can improve the whole compactness of diaphragm, guaranteed the security performance of battery.
Preferably, the coating layer is coated on both sides of the base material layer. Namely, the diaphragm is integrally composed of seven layers of structures, and three coating layers are spread from the base material layer serving as the center to two sides. And the two sides of the base material layer are coated with the three coating layers, so that the liquid absorption and retention capacity of the battery can be further improved, and after the electrolyte is added, no liquid electrolyte is left in the shell.
Preferably, the coating layer is coated on one surface of the substrate layer, and the second coating layer and the first coating layer are sequentially coated on the other surface of the substrate layer. Namely, the structure of the diaphragm is a first coating layer, a second coating layer, a third coating layer, a base material layer, a second coating layer and a first coating layer which are arranged in sequence. I.e. only one side of the substrate layer is coated with the third coating layer.
Preferably, the thermal conductivity of the insulating aerogel layer is less than or equal to 0.05W/m.k.
Preferably, the third coating layer comprises ceramic particles, the particle size of the ceramic particles is 0.1-2 μm, and the thickness of the coating layer is 0.5-5 μm. In addition, the third coating layer further includes a binder.
Preferably, the ceramic particles are one of alumina, boehmite, aluminum hydroxide, silica and titania.
Preferably, the porosity of the third coating layer is 30-70%. The porosity is properly reduced in the third coating layer, burrs and lithium dendrites of the pole piece can be prevented from puncturing the base material layer, and a relatively compact coating layer is formed to protect the stability of the diaphragm. The third coating sets up between thermal-insulated aerogel layer and substrate layer, also can be equivalent to thermal-insulated aerogel layer recombination one deck third coating again, can further strengthen the intensity and the toughness of diaphragm, is difficult for being torn when drawing, maintains the stability of battery. In addition, the third coating layer further includes a binder.
Preferably, the first coating layer comprises polymer particles, the particle size of the polymer particles is 0.1-5 μm, and the swelling degree is 5-100%. In addition, the first coating layer further includes a binder.
Preferably, the pore size of each layer of the coating layer forms a gradient distribution from large to small from the outer surface to the substrate layer. On one hand, the liquid absorption efficiency of the diaphragm can be effectively improved, and the stable structure of the diaphragm is kept; on the other hand, the pore channel structure gradually reduced from outside to inside enables the diaphragm to have a good liquid retaining effect.
The utility model discloses a second purpose lies in, provides a lithium ion battery, including positive plate, negative pole piece and above-mentioned arbitrary item the diaphragm, the diaphragm sets up the positive plate with between the negative pole piece. By adopting the diaphragm, the second coating layer on the diaphragm contains 80-99.5% of porosity, and the high porosity can enable the diaphragm to be combined with the pole piece more tightly, so that even if the thickness of the diaphragm is increased, the combination between the diaphragm and the pole piece is not influenced on the whole, and the increased thickness of the battery can be ignored. In addition, since the separator improves the liquid retention performance of the battery, on the contrary, the energy density of the battery is further improved.
The beneficial effects of the utility model reside in that:
1) the utility model provides a diaphragm for lithium ion battery, including substrate layer and coating, the coating is in the at least one side of substrate layer, the coating is including the first coating, second coating and the third coating that set gradually, the third coating with the substrate layer is connected, the second coating is thermal-insulated aerogel layer, thermal-insulated aerogel layer's porosity is 80 ~ 99.5%. Compared with the prior art, the utility model provides a diaphragm increases the setting of coating on the base layer basis, through the stack setting of three-layer coating for diaphragm's imbibition performance and liquid retention performance all improve to some extent, have solved the poor problem of current diaphragm imbibition ability and liquid retention ability. After the electrolyte is added into the naked electric core, the residue of the liquid electrolyte in the shell is greatly reduced; meanwhile, the diaphragm is beneficial to firmly locking the electrolyte in the battery core, the cycle life of the battery is prolonged, and the problem of cycle deterioration of the pole piece is reduced; in addition, the high-temperature performance and the safety performance of the battery are improved to a certain extent, and the battery can still be in a safe state when being subjected to high temperature, puncture, impact, extrusion and the like. The aerogel coating with the porosity of 80-99.5% is adopted, so that the diaphragm can absorb and retain more electrolyte, the cycle performance of the battery is improved, and meanwhile, the heat insulation effect can be achieved; in addition, still be provided with the third coating between thermal-insulated aerogel layer and substrate layer, can improve the whole compactness of diaphragm, guaranteed the security performance of battery.
2) The utility model also provides a lithium ion battery has adopted the lithium ion battery of above-mentioned diaphragm, all has very big improvement at imbibition performance and liquid retention performance, has improved the cyclicity performance of battery greatly.
Drawings
Fig. 1 is one of the schematic structural diagrams of the separator of the present invention.
Fig. 2 is a second schematic structural diagram of the separator of the present invention.
Fig. 3 is a third schematic structural diagram of the diaphragm of the present invention.
In the figure: 1-a substrate layer; 2-coating layer; 21-a first coating layer; 22-a second coating layer; 23-third coating layer.
Detailed Description
In order to make the technical solutions and advantages of the present invention clearer, the present invention and its advantageous effects will be described in further detail below with reference to the accompanying drawings of the detailed description and the specification, but the present invention is not limited thereto.
Example 1
As shown in fig. 1, a separator for a lithium ion battery includes a substrate layer and a coating layer, the coating layer is coated on one side of the substrate layer, the coating layer includes a first coating layer, a second coating layer and a third coating layer which are sequentially arranged, the third coating layer is connected with the substrate layer, the second coating layer is a heat-insulating aerogel layer, the porosity of the heat-insulating aerogel layer is 80-99.5%, and the thermal conductivity of the heat-insulating aerogel layer is less than or equal to 0.05W/m.k; and by integrating the difficulty and the production cost of industrial production, the porosity of the heat-insulating aerogel layer is preferably 85-96%.
Wherein the thermal insulating aerogel layer comprises inorganic nanoparticles, nanofibers, a binder, and a crosslinker. The specific surface area of the inorganic nano-particles is 50-500 m2The particle size of the inorganic nano particles is 5-100 nm, the inorganic nano particles are in an amorphous state, and the surfaces of the inorganic nano particles at least comprise two groups of carboxyl, amino and hydroxyl. The diameter of the nanofiber is 5-500 nm, and the length-diameter ratio of the nanofiber is 1: 10-1: 500. The aerogel formed by the inorganic nano particles has high heat insulation effect and is hard, the mechanical property of the diaphragm is improved, and the problem of short circuit caused by thermal contraction of the diaphragm can be avoided. The inorganic nano particles are matched with the nano fibers to provide a plurality of small-hole structures for the diaphragm, the porosity of the diaphragm is helped to at least reach over 80 percent and even 99.5 percent, and the liquid absorption performance and the liquid retention performance of the diaphragm are improved.
50 to 500m is used2The inorganic nanoparticles with large specific surface area per gram have larger porosity under the same mass, or the number of the pore diameters of the nanoparticles is larger if the pore diameters are the same, so that the electrolyte can penetrate through the gaps to enter the diaphragm, and the liquid absorption performance of the diaphragm is improved. More preferably, the specific surface area of the inorganic nanoparticles is 150-400 m2(ii) in terms of/g. In addition, the surface of the inorganic nanoparticle further includes at least two groups of a carboxyl group, an amino group, and a hydroxyl group.
Specifically, the inorganic nanoparticles may be silica, alumina, zirconia, titania, calcium oxide, or the like; the nano-fibers are organic fibers and/or inorganic fibers; the organic fiber comprises at least one of cellulose fiber, aramid fiber, polyamide fiber, terylene, acrylic fiber, polypropylene fiber, ultra-high molecular weight polyethylene fiber, PBO fiber, PBI fiber, M5 fiber and PI fiber; the inorganic fiber includes at least one of glass fiber, silica fiber, boron fiber, alumina fiber, and zinc oxide fiber. The crosslinking agent is at least one of aziridines, isocyanates, glycerol ethers, polycarbodiimide and silanes. The addition of the cross-linking agent is beneficial to the cross-linking of the inorganic nano particles and the nano fibers, and the two molecules can be cross-linked together to form a three-dimensional network structure, so that the strength of the diaphragm can be improved, and the heat resistance of the diaphragm can also be improved. In addition, the surface of the inorganic nano-particle also comprises at least two groups of carboxyl, amino and hydroxyl, so that the crosslinking agent can be helped to better establish a three-dimensional network structure through the action of the at least two groups, and chemical bonds generated by the groups can better retain electrolyte and absorb the electrolyte into the diaphragm.
Further, the third coating layer includes ceramic particles and a binder. Wherein the porosity of the third coating layer is 30-70%; the ceramic particles have a particle size of 0.1 to 2 μm and a coating thickness of 0.5 to 5 μm. Specifically, the ceramic particles include at least one of alumina, boehmite, aluminum hydroxide, silica, and titania.
Further, the first coating layer includes polymer particles and a binder. The polymer particles have a particle size of 0.1 to 5 μm and a swelling degree of 5 to 100%. Specifically, the polymer particles are fluorine-containing polymers or acrylate polymers; the fluoropolymer comprises at least one of ethylene-tetrafluoroethylene copolymer (ETFE), Polytetrafluoroethylene (PTFE), fluorinated ethylene propylene copolymer (FEP), perfluoroalkoxy resin (PFA), Polychlorotrifluoroethylene (PCTFE), ethylene chlorotrifluoroethylene copolymer (ECTFE), polyvinylidene fluoride (PVDF), and polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-HFP); the acrylate polymer comprises at least one of polymethyl methacrylate, polyacrylate, acrylic acid-styrene copolymer, acrylic acid-organosilicon copolymer and acrylic acid-acrylonitrile copolymer. The material of the substrate can be prepared by referring to the existing material.
Preferably, the pore size of each layer of the coating layer is in a gradient distribution from large to small in the direction from the outer surface to the base material layer. The aperture of first coating, second coating and third coating is the gradient distribution that reduces gradually promptly to the liquid absorption volume and the liquid retaining volume of better improvement diaphragm through reducing the aperture gradually.
The preparation method of the diaphragm comprises the following steps:
s1, coating the third coating layer on at least one surface of the substrate layer, and drying;
s2, coating the second coating layer on the third coating layer, freezing and curing the second coating layer, and drying to obtain the diaphragm containing the heat-insulating aerogel layer; wherein the porosity of the heat-insulating aerogel layer is 80-99.5%; specifically, before coating, preparing aerogel slurry, fully mixing nano fibers, inorganic nano particles, a binder, a thickening agent, a cross-linking agent and the like to prepare the aerogel slurry with certain viscosity, then uniformly coating the prepared aerogel slurry on a third coating layer, spraying liquid nitrogen or dry ice to freeze the aerogel slurry after coating is finished, drying the heat-insulating aerogel layer after the heat-insulating aerogel layer is frozen and solidified, and quickly vaporizing a solvent in the heat-insulating aerogel layer to obtain a diaphragm containing the heat-insulating aerogel layer;
and S3, finally, coating the first coating layer on the diaphragm containing the heat-insulating aerogel layer, and drying to obtain the diaphragm for the lithium ion battery.
Example 2
As shown in fig. 2, the coating layer of the present embodiment is coated on both sides of the base material layer, unlike embodiment 1. Namely, the diaphragm is integrally composed of seven layers of structures, and three coating layers are spread from the base material layer serving as the center to two sides. And the two sides of the base material layer are coated with the three coating layers, so that the liquid absorption and retention capacity of the battery can be further improved, and after the electrolyte is added, no liquid electrolyte is left in the shell.
The preparation method of the separator is different from that of example 1 in that since the thermal insulation aerogel layer is coated on both sides, in the step S2, the coating of the separator including the thermal insulation aerogel layer on one side is completed, and then the coating of the other side is performed.
The rest is the same as embodiment 1, and the description is omitted here.
Example 3
As shown in fig. 3, unlike embodiment 2, the coating layer of the present embodiment is coated on one surface of the base material layer, and the second coating layer and the first coating layer are sequentially coated on the other surface of the base material layer. That is, only one side of the base material layer is coated with the third coating layer as compared to example 2.
The rest is the same as embodiment 2, and the description is omitted here.
Example 4
A lithium ion battery comprises a positive plate, a negative plate and the diaphragm, wherein the diaphragm is arranged between the positive plate and the negative plate. The preparation of the lithium ion battery can be carried out by referring to the existing lithium ion battery, and the details are not repeated here.
Specifically, the materials selected in the examples include the following examples 5 to 19 and comparative examples 1 to 7, as shown in Table 1. The coating structures of the embodiments 5 to 7 are the same as those of the embodiment 1, and the coating structures of the embodiments 8 to 19 and the comparative examples 1 to 7 are the same as those of the embodiment 2.
TABLE 1
The separators of examples 5 to 19 and comparative examples 1 to 7 were prepared by the method described in example 1, and then the lithium ion batteries were prepared by the separators obtained as described in example 4. The lithium ion batteries obtained above were tested, and the test results are shown in table 2. The following test results were obtained for the amount of retained liquid calculated from the initial capacity of the battery at around 5000 a.
TABLE 2
| Liquid retention amount | Normal temperature cycle retention at 500 weeks (%) | 500 weeksCycle retention at 45 ℃ (%) | |
| Example 5 | 10.5 | 88.4 | 85.0 |
| Example 6 | 11.6 | 90.2 | 86.2 |
| Example 7 | 10.8 | 89.0 | 85.3 |
| Example 8 | 12.2 | 91.4 | 86.1 |
| Example 9 | 13.2 | 94.6 | 88.4 |
| Example 10 | 12.6 | 92.8 | 86.7 |
| Example 11 | 13.1 | 93.7 | 87.3 |
| Example 12 | 12.0 | 91.2 | 86.3 |
| Example 13 | 12.6 | 94.2 | 87.9 |
| Example 14 | 12.7 | 94.6 | 88.2 |
| Example 15 | 12.5 | 94.3 | 88.0 |
| Example 16 | 12.4 | 92.3 | 86.1 |
| Example 17 | 12.8 | 94.5 | 88.4 |
| Example 18 | 11.2 | 91.3 | 86.1 |
| Example 19 | 12.8 | 94.3 | 88.6 |
| Comparative example 1 | 9.5 | 85.3 | 80.4 |
| Comparative example 2 | 9.0 | 82.1 | 79.0 |
| Comparative example 3 | 8.6 | 80.3 | 77.1 |
| Comparative example 4 | 8.0 | 76.9 | 70.1 |
| Comparative example 5 | 7.5 | 73.5 | 64.2 |
| Comparative example 6 | 10.2 | 91.0 | 85.3 |
| Comparative example 7 | 10.0 | 90.5 | 84.6 |
It can be seen from the test result of foretell embodiment and comparative example that the lithium ion battery who has adopted this diaphragm all has very big promotion in the aspect of the liquid retention capacity of battery and circulation retentivity, especially carries out two-sided coating three-layer coating when, compares in the three-layer coating of single face, and its effect of guaranteeing the liquid level is more obvious, and is thus visible, the utility model provides a diaphragm has improved the imbibition performance and the liquid retention performance of battery greatly. In addition, can also derive in comparative example 1 ~ 5, the utility model discloses a diaphragm need adopt at least three-layer coating also to have excellent effect, and if lack a certain one of them layer, also can influence its performance greatly.
In addition, it can be seen from examples 5 to 10 that the liquid retention amount of the separator is increased by gradually increasing the porosity of the second coating layer, but if the porosity is too large, the liquid retention amount is decreased instead, and presumably because the porosity is too large, although the amount of the electrolyte absorbed is increased, the flow of the electrolyte is also easier, so that the subsequent loss of the electrolyte is caused, and the liquid retention amount is not further increased.
In addition, as can be seen from the comparison between examples 9 and 13 to 14, and between examples 15 and 16, when the substance added to the second coating layer is different, the substance has a certain influence on the performance of the battery, and the liquid retention amount of the separator is influenced regardless of the difference of the inorganic nanoparticles, the difference of the nanofibers, or the difference of the crosslinking agent. This is mainly because the crosslinking agent crosslinks the nanofibers and nanoparticles to form a network structure by crosslinking, but the effects of different substances are different, some substances may have fewer carboxyl or amino groups and thus have an effect, and some substances may be caused by insufficient insolubility of the crosslinking agent. Additionally, the utility model discloses the people has still set up the comparative example that second coat and third coat exchanged, the test result discovery will insulate against heat aerogel layer setting can be more excellent at its performance of improving the diaphragm in second coat, this probably because the third coat can improve the intensity of substrate layer with the substrate layer complex earlier, and the second coat is close to with the pole piece, because the porosity on second coat is higher relatively, because the effect such as capillary force can make the combination of pole piece and second coat inseparabler, structural design through this kind can help the better absorption electrolyte of diaphragm, with the guarantor's volume that improves the battery.
It is obvious to a person skilled in the art that the invention is not restricted to details of the above-described exemplary embodiments, but that it can be implemented in other specific forms without departing from the spirit or essential characteristics of the invention. The present embodiments are therefore to be considered in all respects as illustrative and not restrictive, the scope of the invention being indicated by the appended claims rather than by the foregoing description, and all changes which come within the meaning and range of equivalency of the claims are therefore intended to be embraced therein. Any reference sign in a claim should not be construed as limiting the claim concerned.
Furthermore, it should be understood that although the present description refers to embodiments, not every embodiment may contain only a single embodiment, and such description is for clarity only, and those skilled in the art should understand that the embodiments as a whole may be combined as appropriate to form other embodiments understood by those skilled in the art.
Claims (9)
1. The utility model provides a diaphragm for lithium ion battery, its characterized in that includes substrate layer and coating, the coating is in the at least one side of substrate layer, the coating is including the first coating, second coating and the third coating that set gradually, the third coating with the substrate layer is connected, the second coating is thermal-insulated aerogel layer, thermal-insulated aerogel layer's porosity is 80 ~ 99.5%.
2. The separator for a lithium ion battery according to claim 1, wherein the coating layer is coated on both sides of the substrate layer.
3. The separator for a lithium ion battery according to claim 1, wherein the coating layer is coated on one surface of the substrate layer, and the second coating layer and the first coating layer are sequentially coated on the other surface of the substrate layer.
4. The separator for a lithium ion battery according to claim 1, wherein a thermal conductivity of the thermal insulating aerogel layer is less than or equal to 0.05W/m-k.
5. The separator for the lithium ion battery according to claim 1, wherein the third coating layer comprises ceramic particles, the particle size of the ceramic particles is 0.1-2 μm, and the thickness of the coating layer is 0.5-5 μm.
6. The separator for a lithium ion battery according to claim 1, wherein the porosity of the third coating layer is 30 to 70%.
7. The separator according to claim 1, wherein the first coating layer comprises polymer particles, the polymer particles have a particle size of 0.1 to 5 μm and a swelling degree of 5 to 100%.
8. The separator for a lithium ion battery according to claim 1, wherein the pore sizes of the respective layers of the coating layer are in a gradient distribution from large to small in a direction from the outer surface to the base material layer.
9. A lithium ion battery comprising a positive electrode sheet, a negative electrode sheet, and the separator according to any one of claims 1 to 8, wherein the separator is disposed between the positive electrode sheet and the negative electrode sheet.
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| CN113346191A (en) * | 2021-05-31 | 2021-09-03 | 华中科技大学 | Asymmetric diaphragm containing conductive layer, preparation method and application thereof |
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