CN115763830A - Safe hot-melting type carbon-coated current collector, preparation method thereof, pole piece and battery - Google Patents
Safe hot-melting type carbon-coated current collector, preparation method thereof, pole piece and battery Download PDFInfo
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- CN115763830A CN115763830A CN202211649208.7A CN202211649208A CN115763830A CN 115763830 A CN115763830 A CN 115763830A CN 202211649208 A CN202211649208 A CN 202211649208A CN 115763830 A CN115763830 A CN 115763830A
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Abstract
The invention discloses a safe hot-melting carbon-coated current collector and a preparation method thereof, a pole piece and a battery, wherein the preparation method comprises the following steps: preparing coating slurry, (2) coating the coating slurry on the surface of a current collector substrate, and (3) drying the current collector substrate coated with the coating slurry; the coating slurry comprises a conductive material, a hot-melt high polymer material and a binder, and the mass ratio of the conductive material to the hot-melt high polymer material is 1. Due to the existence of the hot-melt high polymer material, the hot-melt high polymer material can be ensured to be quickly hot-melted when the temperature of the secondary battery is increased due to short circuit, short-circuit current can be blocked, the phenomenon that the internal heating of the battery is out of control due to the short-circuit continuous discharge of the secondary battery is avoided, and the safety performance of the secondary battery is improved.
Description
Technical Field
The invention belongs to the technical field of current collectors, and particularly relates to a safe hot-melt carbon-coated current collector, a preparation method thereof, a pole piece and a battery.
Background
In secondary battery, the mass flow body plays the effect of collecting and deriving the electric current, traditional mass flow body conducting capacity is limited, in order to improve secondary battery's rate performance, and ensure to have more firm adhesion property between active material and the mass flow body, can be at the surface coating one deck conducting material of the mass flow body, conducting material's existence can improve the conducting capacity of mass flow body self, and also can reduce the interface resistance between mass flow body and the active material, the collection work of reinforcing mass flow body to electric current in the active material.
The prior art usually coats a conductive carbon layer on the surface of a current collector to obtain a carbon-coated current collector, for example, in the chinese patent application (CN 110034302A, an ultra-thin carbon-coated current collector and a preparation method thereof), a preparation method of a carbon-coated current collector is disclosed, which comprises the steps of cleaning the current collector, performing positive charging treatment, performing ultrasonic atomization on aqueous conductive slurry with negative charges and including a surfactant and a conductive agent, and performing electrostatic deposition on the surface of the current collector with positive charges to obtain the ultra-thin carbon-coated current collector, wherein the carbon-coated layer in the carbon-coated current collector has strong bonding force with the current collector and good conductivity. After the conductive carbon layer is coated on the surface of the current collector, the interface resistance between the current collector and the active substance is sharply reduced, along with the increasing requirement on the energy density of the secondary battery in the current production requirement, when the secondary battery with higher energy density is subjected to puncture or extrusion test, the instantaneous current of the secondary battery during short circuit is sharply increased more, the risk of thermal runaway is higher, and the safety accident is more easily caused. Therefore, in the carbon-coated current collector, the safety performance of the carbon-coated current collector needs to be considered while the conductivity of the current collector is ensured.
Disclosure of Invention
The invention aims to provide a safe hot-melting carbon-coated current collector, a preparation method thereof, a pole piece and a secondary battery, so as to solve the technical problems mentioned in the background technology.
In order to achieve the aim, the invention discloses a preparation method of a safe hot-melt carbon-coated current collector, which comprises the following steps:
(1) The preparation of the coating slurry is carried out,
(2) Coating and coating the slurry on the surface of the current collector substrate,
(3) Drying the current collector base material coated with the coating slurry;
the coating slurry comprises a conductive material, a hot-melt high polymer material and a binder, and the mass ratio of the conductive material to the hot-melt high polymer material to the binder is 1.
Further, the hot-melt high polymer material is a modified bismaleimide polymer, the modified bismaleimide polymer is obtained by modifying a compound containing a bismaleimide group with barbituric acid, wherein the molar ratio of the barbituric acid to the compound containing the bismaleimide group is 1.5-5. .
Further, the conductive material is a conductive carbon material, and comprises one or more of conductive carbon black, graphene, carbon nanotubes, carbon fibers and a conductive carbon fiber composite material.
Further, the coating slurry also comprises a solvent, wherein the solvent is water and/or an organic solvent; the coating slurry contains 3 to 33% of solid matter.
Further, the current collector substrate is a metal foil current collector or a composite current collector.
Further, before coating the slurry on the surface of the current collector substrate, the current collector substrate is subjected to surface treatment.
Further, the surface treatment method comprises one or more of cleaning and degreasing treatment, corona treatment and surface etching treatment.
The invention also claims a safe hot-melt carbon-coated current collector obtained by the preparation method.
The invention also claims a pole piece, which comprises the safe hot-melting carbon-coated current collector.
The invention also claims a battery, which comprises the pole piece.
Compared with the prior art, the safe hot-melting carbon-coated current collector, the preparation method thereof, the pole piece and the secondary battery have the following advantages: coating slurry on the surface of a current collector substrate, wherein the coating slurry contains a conductive material and a hot-melt high polymer material, the conductive material can ensure the conductivity of the finally obtained safe hot-melt carbon-coated current collector, the hot-melt high polymer material can be subjected to hot melting when the temperature rises due to the occurrence of short circuit inside the battery, the volume of the hot-melt high polymer material is shrunk, short-circuit current is blocked, the thermal runaway caused by the temperature rise inside the battery due to the continuous discharge of the short circuit of the battery is avoided, and the safety performance of the battery is improved.
Detailed Description
The technical solution of the present invention will be described in detail by the following specific examples.
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions of the embodiments of the present invention are clearly and completely described below. It should be apparent that the described embodiments are only some of the embodiments of the present invention, and not all of them. All other embodiments, which can be derived by a person skilled in the art from the described embodiments of the invention, are within the scope of the invention.
In the invention, in order to obtain a safe hot-melt carbon-coated current collector, coating slurry is firstly required to be prepared, wherein the coating slurry comprises a conductive material, a hot-melt high polymer material and a binder, the mass ratio of the three materials is 1: adding a conductive material, a hot-melt high polymer material and a binder into a solvent, and uniformly stirring;
wherein the solvent is water and/or organic solvent, and the organic solvent is one or more of ethanol, acetone, methanol, ethylene glycol, n-propanol, isopropanol, dimethyl ether, acetic acid, propylene glycol and glycerol. The prepared coating slurry has a solid matter content of 3-33%.
The conductive material is a carbon material with conductive capability, and specifically is one or more of conductive carbon black, graphene, carbon nanotubes, carbon fibers and conductive carbon fiber composite materials.
The hot-melt type high polymer material is an important raw material in coating slurry, and in the invention, a modified bismaleimide polymer is selected, specifically, the modified bismaleimide polymer is obtained by modifying a compound containing a bismaleimide group by barbituric acid, wherein the molar ratio of the barbituric acid to the compound containing the bismaleimide group is 1.
The modified bismaleimide polymer is a highly branched polymer, the molecular structure of the polymer has a complex tree structure, the molecular weight is distributed between thousands to tens of thousands, the size of the modified bismaleimide polymer is nano-scale, the modified bismaleimide polymer has the small size effect of a nano material, and the characteristic of being heated and melted can be fully exerted.
The binder can be selected from a high-molecular adhesive, specifically one or more of an acrylic adhesive, a polyurethane adhesive, an epoxy adhesive, a phenolic adhesive, an organosilicon adhesive, a rubber aqueous adhesive, a vinyl acetate adhesive, a polyvinyl alcohol adhesive and polyvinylidene fluoride. The adhesive is used for firmly adhering the conductive material and the hot-melt high polymer material to the surface of the current collector.
When preparing the coating slurry, in order to improve the dispersion effect of the conductive material, the hot-melt high polymer material and the binder in the solvent, the stirring process is carried out in a high-speed stirrer, and the materials are added in batches for a small number of times until the uniform coating slurry is obtained and used for coating the surface of the current collector.
And next, selecting a proper current collector substrate, and coating the slurry on the surface of the current collector substrate.
The current collector substrate includes conventional current collector substrates, i.e., metal foil current collectors such as copper foil, aluminum foil, copper aluminum alloy foil, doped copper foil, doped aluminum foil; or new current collector substrates, i.e., composite current collectors, such as composite copper current collectors, composite aluminum current collectors, and the like. In the present invention, a novel current collector substrate, a composite copper current collector and a composite aluminum current collector are preferable as the current collector substrate. This is because the composite copper current collector and the composite aluminum current collector include polymer material layers themselves, and these polymer material layers are also melted and deformed after being heated, and can exert a synergistic effect with the coating slurry to improve the safety performance of the current collectors together.
The method comprises the steps of unreeling a current collector substrate, and carrying out surface treatment on the current collector substrate before coating the current collector substrate, wherein the surface treatment method comprises cleaning and oil removing treatment, corona treatment, surface etching treatment and the like so as to improve the adhesive capacity between coating slurry and the current collector substrate and prevent the finally obtained current collector from being stripped to influence the performance of the current collector.
Respectively coating slurry on the upper surface and the lower surface of the uncoiled current collector substrate in a coating system, and then sending the coated current collector substrate into a drying oven for drying and rolling.
In the steps, the unreeling tension of the current collector base material is 40-160N/m, the coating speed is 60-130m/min, and the reeling tension is 40-160N/m.
The drying process is carried out in three steps, wherein the drying temperature in the first step is 50-80 ℃, the drying temperature in the second step is 60-90 ℃, the drying temperature in the third step is 50-80 ℃, and the drying temperatures in the first step and the third step are controlled to be the same.
The structure of the safe hot-melt carbon-coated current collector obtained by the method comprises two parts, namely a current collector substrate layer positioned in the middle layer and coating layers positioned on two sides of the middle layer, wherein the thickness of the current collector substrate layer is 1-19 micrometers, the thickness of the coating layers is 0.03-6 micrometers, and the thickness of the safe hot-melt carbon-coated current collector is 2-25 micrometers; and (3) carrying out performance test on the finally obtained safe hot-melt carbon-coated current collector, wherein the test result is as follows: the puncture strength is more than or equal to 40gf; the tensile strength MD is more than or equal to 150MPa, and the tensile strength TD is more than or equal to 150MPa; the elongation MD is more than or equal to 1 percent, and the elongation TD is more than or equal to 1 percent; the stripping force of the coating is more than 5N/m; sheet resistance ≦ 35 milliohms per square.
The safe hot-melting carbon-coated current collector obtained by the method is used for preparing an electrode plate, further preparing a lithium battery, and testing the extrusion performance and the impact performance of the lithium battery, and the test result shows that the lithium battery does not explode or catch fire, which shows that the safe hot-melting carbon-coated current collector can improve the safety performance grade of the lithium battery to a certain extent.
In the coating slurry, the functional groups at the tail ends of the molecular structures of adjacent modified bismaleimide polymer molecules can perform chemical reaction to form a three-dimensional protective film, so that the mechanical strength of the coating layer can be improved; meanwhile, the modified bismaleimide polymer is used as a high polymer material, the hot melting temperature is low, and when a short circuit occurs in the lithium battery, a large amount of heat can be generated in the lithium battery, so that the coating layer is subjected to hot melting to cause volume shrinkage, the short circuit current can be blocked, the further occurrence of the short circuit condition is avoided, and the safety performance of the lithium battery is ensured.
Before the experiment is started, firstly, the modified bismaleimide polymer is prepared, and the preparation method is carried out by referring to the method disclosed in the Chinese invention patent application CN101887979A (proton exchange membrane with high proton conductivity), and the preparation method comprises the following steps: adding a bismaleimide compound into a reaction container, adding a solvent gamma-butyrolactone into the reaction container, heating to 120-130 ℃, and stirring until the solvent gamma-butyrolactone is fully dissolved to obtain a bismaleimide compound solution; meanwhile, dissolving barbituric acid in a solvent gamma-butyrolactone to obtain a barbituric acid solution; slowly adding the barbituric acid solution into a reaction container in batches, and continuously reacting for 4-6h; wherein the molar ratio of the added barbituric acid to the added bismaleimide is 1.
After the reaction is finished, cooling the system to room temperature to obtain the modified bismaleimide polymer for later use.
The experiment was then started.
Example 1
First, preparing a coating slurry, comprising: selecting 100kg of water as a solvent, adding 10kg of conductive carbon black while stirring, and continuously stirring until the mixture is uniformly stirred; then adding 5kg of modified bismaleimide polymer, and continuing stirring until the mixture is uniformly stirred; finally, 3kg of polyurethane adhesive is added until the mixture is uniformly stirred. And (5) standby.
Selecting a composite copper current collector as a current collector substrate, wherein the thickness of the composite copper current collector is 8 microns, firstly carrying out corona treatment on the surface of the current collector substrate, then unreeling the current collector substrate to a coating system, the unreeling tension is 80N/m, coating the coating slurry on the surface of the current collector substrate, and the coating speed is 80m/min.
And after the coating is finished, the coating is sent into a drying oven for drying, wherein the drying is divided into three steps, the drying temperature in the first step is 60 ℃, the drying temperature in the second step is 90 ℃, and the drying temperature in the third step is 60 ℃. And after drying, winding with the winding tension of 100N/m.
In the final current collector product, the thickness of the current collector substrate layer is 8 microns, the thickness of the coating layer is 0.5 micron, and the total thickness of the current collector product is 9 microns.
Example 2
First, preparing a coating slurry, comprising: selecting 150kg of ethanol as a solvent, adding 18kg of a mixture of graphene and conductive carbon black with a mass ratio of 1; then adding 18kg of modified bismaleimide polymer, and continuing stirring until the mixture is uniformly stirred; and finally, adding 3.6kg of polyvinyl alcohol adhesive until the mixture is uniformly stirred. And (5) standby.
Selecting a composite aluminum current collector as a current collector substrate, wherein the thickness of the composite aluminum current collector is 10 microns, firstly carrying out ion etching treatment on the surface of the current collector substrate, then unreeling the current collector substrate to a coating system, the unreeling tension is 100N/m, coating the coating slurry on the surface of the current collector substrate, and the coating speed is 120m/min.
And after the coating is finished, the coating is sent into a drying oven for drying, wherein the drying is divided into three steps, the drying temperature in the first step is 70 ℃, the drying temperature in the second step is 85 ℃, and the drying temperature in the third step is 70 ℃. And after drying, winding with winding tension of 120N/m.
In the final current collector product, the thickness of the current collector substrate layer is 10 microns, the thickness of the coating layer is 2 microns, and the total thickness of the current collector product is 2 microns.
Example 3
First, a coating slurry is prepared, including: selecting 100kg of a mixed solvent of water and ethanol with a volume ratio of 1 as a solvent, adding 15kg of a mixture of the carbon nanotube, the graphene and the conductive carbon black with a mass ratio of 2; then adding 12kg of modified bismaleimide polymer, and continuing stirring until the mixture is uniformly stirred; and finally, adding 3kg of epoxy adhesive until the mixture is uniformly stirred. And (4) standby.
Selecting a copper foil as a current collector substrate, wherein the thickness of the copper foil is 9 microns, firstly carrying out ion etching treatment on the surface of the current collector substrate, then unreeling the current collector substrate into a coating system, the unreeling tension is 120N/m, coating the coating slurry on the surface of the current collector substrate, and the coating speed is 100m/min.
And after the coating is finished, the coating is sent into a drying oven for drying, wherein the drying is divided into three steps, the drying temperature in the first step is 75 ℃, the drying temperature in the second step is 90 ℃, and the drying temperature in the third step is 75 ℃. And after drying, winding with winding tension of 120N/m.
In the final current collector product, the thickness of the current collector substrate layer is 9 microns, the thickness of the coating layer is 1.5 microns, and the total thickness of the current collector product is 1.5 microns.
Comparative example 1
Firstly, preparing coating slurry without hot-melt high polymer material, comprising the following steps: selecting 100kg of a mixed solvent of water and ethanol with a volume ratio of 1 as a solvent, adding 15kg of a mixture of the carbon nanotube, the graphene and the conductive carbon black with a mass ratio of 2; then 3kg of epoxy adhesive is added until the mixture is uniformly stirred. And (4) standby.
Selecting a copper foil as a current collector substrate, wherein the thickness of the copper foil is 9 microns, firstly carrying out ion etching treatment on the surface of the current collector substrate, then unreeling the current collector substrate into a coating system, the unreeling tension is 120N/m, coating the coating slurry on the surface of the current collector substrate, and the coating speed is 100m/min.
And after the coating is finished, sending the coating into a drying oven for drying, wherein the drying is divided into three steps, the drying temperature in the first step is 75 ℃, the drying temperature in the second step is 90 ℃, and the drying temperature in the third step is 75 ℃. And after drying, winding, wherein the winding tension is 120N/m.
In the final current collector product, the thickness of the current collector substrate layer is 9 microns, the thickness of the coating layer is 1.5 microns, and the total thickness of the current collector product is 1.5 microns.
The current collector products obtained in the above examples 1-3 and comparative example 1 are used to prepare electrode plates, and lithium batteries are prepared by using the electrode plates, other materials such as active substances, electrolyte, diaphragms, battery shells and the like can be directly purchased in the market, the preparation method of the lithium batteries refers to the method in the Chinese patent application (CN 110212201A, battery cores, battery plates, the preparation method thereof and batteries) to prepare the lithium batteries, and the extrusion test and the impact test are carried out on the lithium batteries according to the content disclosed in the national standard GB/T31485-2015, the safety requirements and the test method of power storage batteries for electric automobiles, and the test results are shown in Table 2.
Table 2 safety performance test results of lithium batteries prepared by using different current collector products
| Number of | Squeeze test | Impact test |
| Example 1 | Without explosion and fire | Without explosion and fire |
| Example 2 | No explosion and no fire | No explosion and no fire |
| Example 3 | No explosion and no fire | No explosion and no fire |
| Comparative example 1 | Explosion and fire | Explosion and fire |
Therefore, based on the current collector product prepared by the method, the lithium battery prepared by the method does not explode or catch fire when the lithium battery is subjected to extrusion test and impact test, and the safe hot-melt carbon-coated current collector obtained by the method has the effect of improving the safety performance level of the lithium battery.
While the foregoing is directed to the preferred embodiment of the present invention, it will be appreciated by those skilled in the art that various changes and modifications may be made therein without departing from the principles of the invention as set forth in the appended claims.
Claims (10)
1. A preparation method of a safe hot-melt carbon-coated current collector is characterized by comprising the following steps: the method comprises the following steps:
(1) The preparation of the coating slurry is carried out,
(2) Coating the slurry on the surface of the current collector substrate,
(3) Drying the current collector substrate coated with the coating slurry;
the coating slurry comprises a conductive material, a hot-melt high polymer material and a binder, and the mass ratio of the conductive material to the hot-melt high polymer material to the binder is 1.
2. The method of claim 1, wherein: the hot-melt high polymer material is a modified bismaleimide polymer, the modified bismaleimide polymer is obtained by modifying a compound containing a bismaleimide group with barbituric acid, wherein the molar ratio of the barbituric acid to the compound containing the bismaleimide group is 1.
3. The method of claim 1, wherein: the conductive material is a conductive carbon material and comprises one or more of conductive carbon black, graphene, carbon nanotubes, carbon fibers and a conductive carbon fiber composite material.
4. The method of claim 1, wherein: the coating slurry also comprises a solvent, wherein the solvent is water and/or an organic solvent; the coating slurry contains 3 to 33% of solid matter.
5. The method of claim 1, wherein: the current collector substrate is a metal foil current collector or a composite current collector.
6. The method of claim 1, wherein: before coating the slurry on the surface of the current collector substrate, performing surface treatment on the current collector substrate.
7. The method of claim 6, wherein: the surface treatment method comprises one or more of cleaning and degreasing treatment, corona treatment and surface etching treatment.
8. A safe hot-melt carbon-coated current collector obtained by the production method according to any one of claims 1 to 7.
9. A pole piece comprising the safe hot melt carbon coated current collector of claim 8.
10. A battery comprising the pole piece of claim 9.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN117239143A (en) * | 2023-10-26 | 2023-12-15 | 广州纳诺新材料科技有限公司 | Self-sealing carbon-coated foil, high-safety battery and preparation method thereof |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN117239143A (en) * | 2023-10-26 | 2023-12-15 | 广州纳诺新材料科技有限公司 | Self-sealing carbon-coated foil, high-safety battery and preparation method thereof |
| CN117239143B (en) * | 2023-10-26 | 2024-02-20 | 广州纳诺新材料科技有限公司 | Self-sealing carbon-coated foil, high-safety battery and preparation method thereof |
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