CN110676463A - Current collector and preparation method thereof - Google Patents
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/665—Composites
- H01M4/667—Composites in the form of layers, e.g. coatings
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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
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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- Y02E60/10—Energy storage using batteries
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Abstract
The invention provides a current collector and a preparation method thereof, which relate to the technical field of chemical power supplies and comprise a conductive substrate layer and at least one conductive coating layer with a regular three-dimensional grid structure; the conductive coating is coated on the base layer. According to the current collector provided by the invention, at least one layer of conductive coating with a regular three-dimensional grid structure is coated on the conductive substrate layer, so that the contact area between the electrode material and the conductive coating can be increased, the bonding strength between the current collector and the electrode material is increased, the electronic conduction capability between the current collector and the electrode material is also favorably improved, the electrochemical performance of the current collector is ensured, and the using amount of a binder is reduced.
Description
Technical Field
The invention relates to the technical field of chemical power supplies, in particular to a current collector and a preparation method thereof.
Background
The current collector used for an electrochemical system mainly has the function of providing good electronic conduction capacity; the current collectors in the prior art include current collectors directly using aluminum foil, copper foil or other substrate films with electron conductivity, and current collectors modified by coatings.
The current collector modified by the coating is obtained by coating the modified coating on the surface of an aluminum foil, a copper foil or other substrates with conductive capability; in the using process of the coating-modified current collector, the coating coated on the surface of the substrate is connected with the electrode material layer insecurely, so that the electrode material and the current collector are connected insecurely, the electronic conductivity of the whole electrode piece is poor, the performance exertion of an electrochemical system under the high-current charging and discharging condition is influenced, and potential safety hazards are generated.
Disclosure of Invention
The invention solves the problem of how to improve the binding force between the coating modified current collector and the electrode material.
In order to solve the above problems, the present invention provides a current collector, which comprises a conductive substrate layer and at least one conductive coating layer having a regular three-dimensional grid structure; the conductive coating is coated on the base layer.
Optionally, the cross-sectional shape of the lattice structure is one of a diamond shape, a hexagon shape, a U shape, a snake shape, a square shape, a negative lattice point shape and a mountain shape.
Optionally, the distance between the top end of the lattice structure and the base layer ranges from 0.05 μm to 5 μm; the distance between the top end of the corrugated structure and the bottom end of the corrugated structure domain ranges from 0.05 μm to 3 μm.
Optionally, the maximum width of the corrugated structure ranges from 0.01 μm to 2000 μm.
Optionally, the substrate layer is selected from one of copper foil, aluminum foil, stainless steel foil, nickel foil, carbon paper, porous metal foil, film body with conductive capability, and non-metal film body with conductive capability.
Optionally, the conductive coating comprises a conductive material, a polymeric binder, and a conductive polymer.
Optionally, the conductive material is selected from at least one of carbon black, acetylene black, carbon nanotubes, carbon fibers, graphite, nanographite, graphene, fullerene, and conductive oxide.
Optionally, the conductive polymer is selected from at least one of polythiophene, polypyrrole, polyaniline, polyacetylene, poly-p-phenylene ethylene, and polydiyne and nitroxide-based organic radical polymerization and derivatives or block and graft copolymers thereof.
Another object of the present invention is to provide a method for preparing the current collector, which includes the following steps:
s1: mixing a conductive material, a high-molecular binder, a conductive polymer and a solvent, and emulsifying and grinding to obtain conductive coating slurry;
s2: carrying out surface roughening pretreatment on the substrate layer to obtain a pretreated substrate layer;
s3: and coating the conductive coating slurry on the surface of the pretreated basal layer by adopting a normal phase printing type coating machine with a regular three-dimensional grid-structured plate roller, and baking and drying at 50-200 ℃ to obtain the current collector.
Optionally, the coating speed in the step S3 is in the range of 1-180 m/min.
Compared with the prior art, the current collector provided by the invention has the following advantages:
according to the current collector provided by the invention, at least one layer of conductive coating with a regular three-dimensional grid structure is coated on the conductive substrate layer, so that the contact area between the electrode material and the conductive coating can be increased, the bonding strength between the current collector and the electrode material is increased, the electronic conduction capability between the current collector and the electrode material is also favorably improved, the electrochemical performance of the current collector is ensured, and the using amount of a binder is reduced.
Drawings
FIG. 1 is a schematic structural view of a conductive coating according to the present invention;
FIG. 2 is a scanning electron micrograph of a conductive coating according to the present invention;
FIG. 3 is comparative membrane resistance data for electrode sheets according to the present invention;
fig. 4 is a graph of 1C 45 high temperature cycling performance of a cell according to the invention.
Detailed Description
In order to make the aforementioned objects, features and advantages of the present invention comprehensible, embodiments accompanied with figures are described in detail below.
In order to improve the binding force between the coating modified current collector and an electrode material, the invention provides a current collector which comprises a conductive substrate layer and at least one conductive coating layer with a regular three-dimensional lattice structure; wherein the conductive coating is coated on the substrate layer.
Referring to fig. 1, in the current collector provided by the present invention, the conductive coating coated on the substrate layer has a regular three-dimensional lattice structure, that is, the conductive coating is provided with a three-dimensional lattice structure, and the lattice structure is uniformly arranged according to a certain rule; due to the existence of the grid structure, the conductive coating is provided with a plurality of regularly distributed three-dimensional groove-shaped structures; in an electrochemical system, a conductive coating positioned on the surface of a substrate layer is contacted with an electrode material, a groove-shaped structure on the conductive coating can form an embedded splicing structure with the rough surface of an electrode material layer, namely, the electrode material can be embedded into the groove structure, so that the contact area between the electrode material and the conductive coating is increased, on one hand, the electrode material is tightly combined with the conductive coating on a current collector, the binding force between the current collector and the electrode material is increased, and the influence on the integral electronic conduction capability of an electrode pole piece and the performance of the electrochemical system due to the fact that the electrode material is not firmly connected with the current collector is avoided; in the using process of the battery, the size of the electrode material layer is easy to change, the conductive coating and the electrode material layer are in an electrolyte soaking state in the battery for a long time, and in the soaking process, the conductive coating and the electrode material layer are swelled at different degrees, so that the adhesion between the electrode material and the conductive coating is influenced, even the electrode material layer and a current collector fall off, the polarization internal resistance of the battery is increased rapidly, the battery cannot work normally, and potential safety hazards are generated; due to the existence of the grid structure, the current collector provided by the invention has the advantages that the electrode material is embedded in the groove-shaped structure of the conductive coating, and even if the size of the electrode material layer or the conductive coating is changed, the electrode material layer cannot be separated from the groove of the conductive coating, so that the stable connection between the electrode material layer and the current collector is maintained; on the other hand, the electrode material layer is connected with the current collector through the corrugated structure on the conductive coating, so that the contact area between the electrode material layer and the conductive coating is increased, the conductivity of the current collector is further improved, and the high-current charge-discharge performance and the cycle service life of an electrochemical system are improved.
According to the invention, the current collector and the electrode material layer are connected through the occlusion type three-dimensional structure, so that the adhesive force between the electrode material layer and the current collector can be improved, and the use amount of a binder in the electrode material layer is reduced, thereby improving the energy density of an electrochemical system. Moreover, the occlusion type three-dimensional connecting structure is also beneficial to enabling the electrode material layer to be in full contact with the conductive coating, so that a cross-linking effect is generated between the electrode material layer and the conductive coating, and the electronic conduction capability of the current collector is further improved.
In addition, as the regular three-dimensional lattice structure is arranged on the conductive coating, and the lattice structure is uniformly distributed on the conductive coating according to a certain rule, the structures of all positions of the prepared current collector are the same, so that the uniformity and stability of the performances of all positions of the current collector are ensured, the adhesion between electrode plates and the consistency of the conductivity are ensured, and the energy density of an electrochemical system is improved, and meanwhile, the charge-discharge cycle performance of the electrochemical system can be improved.
Specifically, the cross section of the lattice structure is in one of a diamond shape, a hexagon shape, a U shape, a snake shape, a square shape, a negative lattice point shape and a mountain shape.
The shape of the lattice structure can be any geometric shape which can form a regular groove-shaped structure on the conductive coating; the grid structure distributed on the conductive coating is a plurality of groove-shaped structures with the same shape and size and consistent arrangement rule.
In order to give consideration to the connection strength with an electrode material and the electrochemical performance of an electrochemical system in the using process of the current collector, the distance range between the top end of the corrugated structure and the substrate layer is 0.05-5 microns; the distance between the top end of the lattice structure and the bottom end of the lattice structure ranges from 0.05 μm to 3 μm.
The top end of the lattice structure refers to one end, far away from the base layer, of the side wall of each groove structure; correspondingly, the bottom end of the corrugated structure refers to the end of the sidewall of each groove structure close to the substrate layer, i.e. the bottom of the groove structure.
In addition, the maximum width range of the grid structure is 0.01-2000 μm; the maximum width of the corrugated structure is the distance between two points which are farthest from the straight line on the side wall where each groove structure is arranged oppositely.
In order to ensure that the electrochemical performance of the current collector meets the requirement of an electrochemical system, the substrate layer in the current collector is selected from one of copper foil, aluminum foil, stainless steel foil, nickel foil, carbon paper, porous metal foil, a membrane body with conductive capability and a non-metallic membrane body with conductive capability; the conductive coating comprises a conductive material, a high-molecular binder and a conductive polymer; wherein the conductive material is selected from at least one of carbon black, acetylene black, carbon nano tube, carbon fiber, graphite, nano graphite, graphene, fullerene and conductive oxide; the conductive polymer is at least one selected from polythiophene, polypyrrole, polyaniline, polyacetylene, poly-p-phenylene ethylene, poly-double alkyne and nitroxide organic free radical polymerization and derivatives or block and graft copolymers thereof; the high molecular binder is selected from at least one of sodium carboxymethylcellulose, lithium carboxymethylcellulose, polyacrylic acid, polyamide, polyacrylamide, polyethylene glycol, polyacrylonitrile, polypropylene, polyethylene, polyvinyl alcohol, polyvinyl chloride, polyester, polyvinylidene fluoride, polytetrafluoroethylene, polyimide, epoxy resin, polyurethane, polyether ether ketone, polymethyl methacrylate, phenolic resin, modified acrylic acid, modified polyurethane, modified styrene-butadiene rubber, polymers containing hydroxyl or carboxyl functional groups, and derivatives or blocks, graft copolymers and conductive polymers of the above polymers.
According to the current collector provided by the invention, at least one layer of conductive coating with a regular three-dimensional grid structure is coated on the conductive substrate layer, so that the contact area between the electrode material and the conductive coating can be increased, the bonding strength between the current collector and the electrode material is increased, the electronic conduction capability between the current collector and the electrode material is also favorably improved, the electrochemical performance of the current collector is ensured, and the using amount of a binder is reduced.
Another object of the present invention is to provide a method for preparing a current collector, which comprises the steps of:
s1: mixing a conductive material, a high-molecular binder, a conductive polymer and a solvent, and emulsifying and grinding to obtain conductive coating slurry;
s2: carrying out surface roughening pretreatment on the substrate layer to obtain a pretreated substrate layer;
s3: and (3) coating the conductive coating slurry on the surface of the pretreated basal layer by adopting a normal phase printing type coating machine with a regular three-dimensional grid-structured plate roller, and baking and drying at 50-200 ℃ to obtain the current collector.
The selection of the conductive material, the polymer binder, the conductive polymer and the substrate layer is the same as that in the above, and the description is omitted; the mass percentage range of the conductive material is 20-80%; the mass percentage range of the macromolecular binder is 1-40%; the mass percentage range of the conductive polymer is 0.01-40%; the viscosity range of the prepared conductive coating slurry is 5-1000 mPa.s, the solid content range is 2-35%, and the pH value range is 2-12.
The solvent is at least one of N-methyl pyrrolidone, deionized water, isopropanol and absolute ethyl alcohol.
The specific process of carrying out surface roughening pretreatment on the substrate layer comprises the steps of sequentially carrying out solution cleaning, corona and high-temperature annealing on the selected substrate layer.
In order to prepare the grid structure on the conductive coating, the invention carries out coating by a normal phase printing type coating machine, and a regular three-dimensional grid structure is arranged on a plate roller, wherein the shape, the size and the like of the grid structure on the plate roller are the same as those of the grid structure required on the conductive coating.
In order to ensure the coating effect, the coating speed in step S3 is 1-180 m/min.
By the method provided by the invention, the thickness range of the conductive coating in the prepared current collector is 0.05.
The preparation method of the current collector provided by the invention has the advantages that the preparation process is simple and easy to operate, the prepared current collector can be better connected with an electrode material, and can adapt to larger size change of an electrode material layer in the working process, and the occurrence of a local dead zone phenomenon caused by poor connection of the current collector and the electrode material layer is effectively avoided; meanwhile, the effective area of the current collector for conducting electrons can be increased, so that the performance of the electrochemical performance of an electrochemical system using the current collector is improved; in addition, the preparation method of the current collector is beneficial to improving the surface tension of the current collector, preventing the surface of the substrate layer from being corroded and oxidized, reducing the interface resistance of the current collector and the electrode material layer, reducing the heat productivity of an electrochemical system and increasing the safety performance of the electrochemical system.
Example one
S1: mixing 9g of carbon black, 3.5g of modified polyurethane, 2.5g of polythiophene and 85g of N-methyl pyrrolidone, and emulsifying and grinding to obtain conductive coating slurry;
s2: sequentially carrying out solution cleaning, corona and high-temperature annealing on the substrate layer aluminum foil to obtain a pretreated aluminum foil;
s3: adding the conductive coating slurry into a feeding barrel of a coating machine, coating the conductive coating slurry on the surface of a pretreated aluminum foil by adopting a normal phase printing type coating machine with a regular three-dimensional hexagonal grid structure plate roller (the grid structure on the plate roller is 250 meshes, and the engraving depth is 15 mu m), baking and drying at 120 ℃, wherein the coating speed is 120 m/min, and rolling a finished product to obtain a current collector with the conductive coating thickness of 0.7 mu m and the surface of a hexagonal grid structure.
Referring to fig. 2, the conductive coating on the surface layer of the current collector prepared in this embodiment is scanned by an electron microscope, and as can be seen from fig. 2, by the preparation method of this embodiment, a conductive coating having a regularly distributed corrugated structure is formed on the surface of the aluminum foil as the substrate layer.
In order to inspect the performance of the prepared current collector, the lithium iron phosphate anode slurry is further coated on the prepared current collector by using a coating machine, and is dried and then is pressed by using a roller press to obtain an electrode plate.
Detecting the physical properties of the prepared electrode plate:
1. testing the resistance of the pole piece: the sheet resistance of the rolled electrode sheet with the area of 150 × 200mm prepared in this example was tested by using a sheet resistance tester, the distance between each test point was 30mm, and 20 data were tested, as shown in fig. 3, the sheet resistance of the electrode sheet prepared in this example was stabilized at 38.5 Ω, and the difference was not more than 0.1 Ω.
2. Mechanical properties: the peel strength of the electrode piece prepared in this example was tested with a tensile testing machine, and was 118.5N/m.
Detecting the electrochemical performance of the prepared electrode plate: the prepared electrode plate is manufactured into a soft package battery with the energy density of 150Wh/kg and the capacity of 2Ah, a battery testing system is adopted to test the 1C 45-degree high-temperature charge and discharge cycle performance of the battery, and as shown in figure 4, the capacity retention rate of the battery prepared by the electrode plate prepared in the embodiment is 99.5% after 168 cycles of 1C 45-degree high-temperature cycle.
According to the detection results, the current collector prepared in the embodiment has a regular and three-dimensionally distributed hexagonal lattice structure on the conductive coating; the current collector and the electrode material layer have stronger bonding strength, and meanwhile, the current collector has excellent electrochemical performance.
Example two
S1: mixing 3g of carbon black, 6g of polyacrylic acid, 6g of polythiophene and 85g of N-methyl pyrrolidone, and emulsifying and grinding to obtain conductive coating slurry;
s2: sequentially carrying out solution cleaning, corona and high-temperature annealing on the substrate layer aluminum foil to obtain a pretreated aluminum foil;
s3: adding the conductive coating slurry into a feeding barrel of a coating machine, coating the conductive coating slurry on the surface of a pretreated aluminum foil by adopting a normal phase printing type coating machine with a regular three-dimensional diamond-shaped grid-structured plate roller (the grid structure on the plate roller is 200 meshes, and the engraving depth is 20 mu m), baking and drying at 120 ℃, wherein the coating speed is 150 m/min, and rolling a finished product to obtain a current collector with the conductive coating thickness of 0.5 mu m and the diamond-shaped grid-structured surface.
The process of detecting the current collector prepared in this embodiment is the same as that of the first embodiment, and is not described herein again.
According to the detection results, the conductive coating of the current collector prepared by the embodiment has a regular three-dimensional distribution diamond-shaped corrugated structure; the current collector and the electrode material layer have stronger bonding strength, and meanwhile, the current collector has excellent electrochemical performance.
EXAMPLE III
S1: mixing 7g of carbon black, 6g of sodium carboxymethylcellulose, 2g of polythiophene and 85g of N-methylpyrrolidone, and emulsifying and grinding to obtain conductive coating slurry;
s2: sequentially carrying out solution cleaning, corona and high-temperature annealing on the substrate layer aluminum foil to obtain a pretreated aluminum foil;
s3: adding the conductive coating slurry into a feeding barrel of a coating machine, coating the conductive coating slurry on the surface of a pretreated aluminum foil by adopting a normal phase printing type coating machine with a regular three-dimensional triangular grid structure plate roller (the grid structure on the plate roller is 300 meshes, and the carving depth is 15 mu m), baking and drying at 90 ℃, wherein the coating speed is 180 m/min, and rolling a finished product to obtain a current collector with the conductive coating thickness of 1 mu m and the triangular grid structure on the surface.
The process of detecting the current collector prepared in this embodiment is the same as that of the first embodiment, and is not described herein again.
According to the detection results, the current collector prepared in the embodiment has a regular three-dimensional triangular lattice structure on the conductive coating; the current collector and the electrode material layer have stronger bonding strength, and meanwhile, the current collector has excellent electrochemical performance.
Comparative example 1
In order to compare the current collector provided by the invention with a current collector without a corrugated structure on a conductive coating, the comparative example provides another preparation method of the current collector, and the preparation method comprises the following steps:
s1: mixing 9g of carbon black, 3.5g of modified polyurethane, 2.5g of polythiophene and 85g of N-methyl pyrrolidone, and emulsifying and grinding to obtain conductive coating slurry;
s2: sequentially carrying out solution cleaning, corona and high-temperature annealing on the substrate layer aluminum foil to obtain a pretreated aluminum foil;
s3: adding the conductive coating slurry into a feeding barrel of a coating machine, coating by adopting a roller with an oblique 45-degree reticulate structure (the reticulate is 180 meshes, and the engraving depth is 25 mu m) in a reverse coating mode, coating the conductive coating slurry on the surface of the pretreated aluminum foil, baking and drying at 120 ℃, wherein the coating speed is 120 m/min, and rolling a finished product to obtain a current collector with the conductive coating thickness of 0.7 mu m and the surface uniformly coated with the conductive coating.
In order to test the performance of the prepared current collector, the lithium iron phosphate anode slurry is further coated on the prepared current collector by adopting a coating machine, dried and then tabletted by adopting a roller press to obtain the electrode plate.
Detecting the physical properties of the prepared electrode plate:
1. testing the resistance of the pole piece: the diaphragm resistance of the rolled electrode plate with the area of 150 x 200mm prepared in the embodiment is tested by a diaphragm resistance tester, the distance between each test point is 30mm, 20 data are tested, and the diaphragm resistance of the electrode plate prepared in the embodiment is stabilized at 40.1-42 omega as shown in fig. 3.
2. Mechanical properties: the peel strength of the electrode piece prepared in this example was tested with a tensile testing machine, and the peel strength of the electrode piece prepared in this example was 68.7N/m.
Detecting the electrochemical performance of the prepared electrode plate: the prepared electrode plate is manufactured into a soft package battery with the energy density of 150Wh/kg and the capacity of 2Ah, a battery testing system is adopted to test the 1C 45 ℃ high-temperature charge and discharge cycle performance of the battery, and as shown in figure 4, the capacity retention rate of the battery prepared by the electrode plate prepared in the embodiment is 98.03% after 168 cycles of 1C 45 ℃ high-temperature cycle.
Compared with the detection result in the first embodiment, the electrode plate prepared by the current collector provided in the first embodiment has obviously better mechanical property and electrochemical property than the comparative example, so that the current collector provided by the invention has excellent interface binding force of the conductive coating, improves the uniform distribution of electron conduction channels, reduces the contact resistance of an electrochemical system, can effectively avoid the problems of impedance increase, battery temperature rise and the like caused by electrode material layer falling and conductive coating swelling after long-term circulation of the electrode plate, and further improves the charge-discharge cycle performance of the electrochemical system.
Although the present disclosure has been described above, the scope of the present disclosure is not limited thereto. Those skilled in the art can make various changes and modifications without departing from the spirit and scope of the present disclosure, and such changes and modifications will fall within the scope of the present invention.
Claims (10)
1. A current collector is characterized by comprising a conductive substrate layer and at least one conductive coating layer with a regular three-dimensional grid structure; the conductive coating is coated on the base layer.
2. The current collector of claim 1, wherein the cross-sectional shape of the lattice structure is one of diamond, hexagonal, U-shaped, serpentine, square, halftone dot, or mountain.
3. The current collector of claim 1, wherein a distance between a top end of the lattice structure and the base layer ranges from 0.05 μ ι η to 5 μ ι η; the distance between the top end of the corrugated structure and the bottom end of the corrugated structure domain ranges from 0.05 μm to 3 μm.
4. The current collector of claim 1, wherein the maximum width of the gridlike structure ranges from 0.01 μ ι η to 2000 μ ι η.
5. The current collector of any one of claims 1 to 4, wherein the substrate layer is selected from one of a copper foil, an aluminum foil, a stainless steel foil, a nickel foil, a carbon paper, a porous metal foil, a film body with electric conductivity, and a non-metal film body with electric conductivity.
6. The current collector of any one of claims 1 to 4, wherein the conductive coating comprises a conductive material, a polymeric binder, and a conductive polymer.
7. The current collector of claim 6, wherein the conductive material is selected from at least one of carbon black, acetylene black, carbon nanotubes, carbon fibers, graphite, nanographite, graphene, fullerene, conductive oxides.
8. The current collector of claim 6, wherein the conductive polymer is selected from at least one of polythiophene, polypyrrole, polyaniline, polyacetylene, poly-p-phenylene vinylene, and polydiyne with nitroxide radical polymerization and derivatives or block, graft copolymers thereof.
9. A method for preparing a current collector as claimed in any one of claims 1 to 8, comprising the steps of:
s1: mixing a conductive material, a high-molecular binder, a conductive polymer and a solvent, and emulsifying and grinding to obtain conductive coating slurry;
s2: carrying out surface roughening pretreatment on the substrate layer to obtain a pretreated substrate layer;
s3: and coating the conductive coating slurry on the surface of the pretreated basal layer by adopting a normal phase printing type coating machine with a regular three-dimensional grid-structured plate roller, and baking and drying at 50-200 ℃ to obtain the current collector.
10. The method of preparing a current collector of claim 9, wherein the coating speed in step S3 is in a range of 1-180 m/min.
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| CN114709359A (en) * | 2022-03-24 | 2022-07-05 | 深圳吉阳智能科技有限公司 | Battery pole piece and continuous processing method thereof |
| CN116344830A (en) * | 2023-03-24 | 2023-06-27 | 江阴纳力新材料科技有限公司 | High-conductivity low-water-absorption nano carbon-coated current collector and preparation method thereof |
| WO2024085688A1 (en) * | 2022-10-19 | 2024-04-25 | 주식회사 엘지화학 | Electrode |
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