CN115966652A - Dot-matrix carbon fiber structure battery and preparation method thereof - Google Patents
Dot-matrix carbon fiber structure battery and preparation method thereof Download PDFInfo
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Abstract
The invention provides a lattice type carbon fiber structure battery and a preparation method thereof, wherein the lattice type carbon fiber structure battery comprises the following components: the carbon fiber coating material comprises anode carbon fibers, an insulating fiber diaphragm, cathode carbon fibers, electrolyte and structural resin which are coated with anode materials distributed in a lattice manner; the preparation method comprises the steps of paving a layer of isolating membrane with periodic holes on the carbon fiber after desized, coating the anode slurry on the isolating membrane, and drying at high temperature in vacuum to form anode carbon fiber coated with anode material distributed in a lattice manner, wherein the carbon fiber after desized is used as cathode carbon fiber; laying the positive carbon fiber, the insulating fiber diaphragm and the negative carbon fiber in sequence; under the anhydrous and oxygen-free environment, electrolyte liquid and structural resin liquid are mixed according to a certain proportion to form structural electrolyte, and the structural electrolyte is poured to finish solidification. The invention can improve the stripping resistance of the anode carbon fiber, and ensures the mechanical property while having high energy density.
Description
Technical Field
The invention relates to the technical field of multifunctional composite material manufacturing, in particular to a lattice type carbon fiber structure battery and a preparation method thereof.
Background
In order to further improve the service performance of advanced equipment under a more severe load, an integrated energy storage structure composite material is proposed, as a typical representative carbon fiber structure battery, the integrated energy storage structure composite material is composed of anode carbon fiber-insulating fiber diaphragm-cathode carbon fiber loaded with an anode material, electrolyte and structural resin, the light high-modulus high-strength mechanical property and the high conductivity and high specific capacity electrical property of the carbon fiber are fully utilized, the integrated energy storage structure can play a role in storing energy while bearing a severe load, the energy is fused in the structure, the mass and the space are saved, and the integrated energy storage structure composite material provides further development possibility for a new generation of carrier rockets, manned aircrafts, electric vehicles and the like.
Although the carbon fiber serving as the negative electrode can play multiple roles of a reinforcement body, a reaction negative electrode and a negative current collector, the positive carbon fiber can only play roles of the positive current collector and the reinforcement body, the carbon fiber structure battery still needs a positive active material for energy storage, and the positive material is often coated on the positive carbon fiber in a slurry coating and drying mode, but the mode undoubtedly isolates the contact of the carbon fiber and the structural resin, the weaker positive slurry becomes a layering defect, the structural resin and the carbon fiber are easily stripped, the fiber loses solid support and is bent, the mechanical property is greatly reduced, the stripped positive material also loses the energy storage effect, and the further development and application of the carbon fiber structure battery are seriously hindered. Therefore, how to change the distribution mode of the cathode material to ensure that the cathode material maintains high energy density and simultaneously ensures the anti-stripping performance of the cathode carbon fiber layer is a problem to be solved urgently in the carbon fiber structure battery.
Patent document CN112652737A discloses a composite material structure battery based on carbon fiber and a mobile phone shell, wherein the structure battery comprises a modified carbon fiber negative electrode and a modified carbon fiber positive electrode; the modified carbon fiber negative electrode is prepared by forming a first modified coating layer on the outer layer of carbon fiber wires of the first carbon fiber cloth; the modified carbon fiber positive electrode is prepared by forming an outer second modified coating layer on carbon fiber wires of second carbon fiber cloth; the modified carbon fiber negative electrode and the modified carbon fiber positive electrode are laid in a stacked mode, are completely isolated through a solid electrolyte and form an integrally formed structure. The patent only provides a carbon fiber structure battery structure, mechanical property reduction caused by simply coating anode slurry on a carbon fiber anode is not considered, and high energy density and high mechanical property can not be ensured at the same time. There is still a need in the art to provide more advanced and efficient methods for designing and manufacturing high modulus, high strength and high energy density carbon fiber structured batteries.
Disclosure of Invention
Aiming at the defects in the prior art, the invention aims to provide a lattice type carbon fiber structure battery and a preparation method thereof.
The technical scheme of the invention is as follows
In a first aspect:
the invention provides a preparation method of a lattice type carbon fiber structure battery, which comprises the following steps:
step S1: mixing the conductive particles, the binder and the active material, dissolving the mixture into a solvent, and uniformly stirring the mixture to form anode slurry;
step S2: laying a layer of isolating membrane with lattice holes on the carbon fiber after desizing, coating the anode slurry obtained in the step S1 on the isolating membrane, drying at high temperature in vacuum, removing the isolating membrane to form anode carbon fiber coated with anode material distributed in a lattice manner, and taking the carbon fiber after desizing as cathode carbon fiber;
and step S3: the positive carbon fiber, the insulating fiber diaphragm and the negative carbon fiber are sequentially stacked;
and step S4: mixing electrolyte liquid and structural resin liquid according to a certain proportion under an anhydrous and oxygen-free environment to form structural electrolyte;
step S5: pouring the structural electrolyte in the step S4 into the prefabricated body in the step S3 in an anhydrous and oxygen-free environment, solidifying, and sealing holes by using structural resin again after solidification; and manufacturing the lattice type carbon fiber structure battery.
In step S1, the solvent is N-methylpyrrolidone (NMP).
Preferably, in step S1, the conductive particles include conductive carbon black particles (Super P), acetylene black, the binder includes polyvinylidene fluoride (PVDF), and the active material includes at least one of lithium iron phosphate, lithium manganate, lithium cobaltate, and ternary lithium metal oxide.
Preferably, in step S2, the cathode carbon fiber and the anode carbon fiber may be woven as a unidirectional fabric, a plain fabric, a twill fabric, a satin fabric, or a three-dimensional woven fabric.
Preferably, in step S2, the holes on the isolation film with lattice holes have regular geometric shapes, and the period interval should be determined according to the viscosity of the anode slurry and the permeability of the carbon fiber fabric, so as to avoid that the lattice slurry permeates and fuses in the surface of the carbon fiber fabric and loses the lattice structure after coating.
Preferably, in step S2, the lattice distribution mode of the positive electrode slurry may be determined according to a test result or simulation, so as to ensure that the positive electrode slurry has the highest utilization rate of mechanical and electrical properties.
Preferably, the structural resin material includes one or more of epoxy resin, bismaleimide resin, polyimide resin, polyether ether ketone resin and phenolic resin.
Preferably, the electrolyte liquid comprises an ionic electrolyte and a solid electrolyte solution, the ionic electrolyte is adopted, curing needs to be carried out at normal temperature or low temperature, volatilization of an organic solvent of the ionic electrolyte is avoided, and the solid electrolyte solution is adopted, curing needs to be carried out at medium and high temperature, so that the organic solvent in the solid electrolyte solution volatilizes.
In step 4, the mixed electrolyte liquid and the structural resin liquid are mixed by equal mass.
The lattice type carbon fiber structure battery prepared by the preparation method also belongs to the protection scope of the invention.
Compared with the prior art, the invention has the following beneficial effects:
1. the invention utilizes the dot matrix coating of the anode slurry to avoid the condition that the anode carbon fiber is completely wrapped by the anode material to isolate the structural resin, and the dot matrix distribution mode ensures that the anode material stores energy in each period in the anode carbon fiber surface and the structural resin with higher mechanical property is wrapped and fixed.
2. The invention provides a new idea for designing a structural battery, develops the optimization dimension of in-plane material distribution design, and fully considers the requirement of the carbon fiber structural battery and simultaneously meets the requirements of high mechanical property and high energy density.
3. According to the invention, the distribution mode of the anode material is designed on the anode carbon fiber layer, and the carbon fiber layers are mutually communicated and highly conductive, so that the influence on the electrical property of the anode carbon fiber layer as an anode energy storage layer is small.
4. The method for forming the battery with the dot-matrix carbon fiber structure has the advantages of simple and convenient forming steps, low cost and good effect, and is suitable for large-scale production.
Drawings
Other features, objects and advantages of the invention will become more apparent upon reading of the detailed description of non-limiting embodiments with reference to the following drawings:
FIG. 1 is a schematic structural diagram of a lattice-type high-modulus high-strength high-energy-density carbon fiber structure battery;
FIG. 2 is a schematic diagram of the lattice distribution of the cathode material on the cathode carbon fiber layer in example 1;
fig. 3 is a schematic diagram of the lattice distribution of the cathode material on the cathode carbon fiber layer in example 2.
Detailed Description
The present invention will be described in detail with reference to specific examples. The following examples will assist those skilled in the art in further understanding the invention, but are not intended to limit the invention in any way. It should be noted that it would be obvious to those skilled in the art that various changes and modifications can be made without departing from the spirit of the invention. All falling within the scope of the invention.
As shown in fig. 1, the present invention provides a battery of a lattice type carbon fiber structure.
The carbon fiber structure battery comprises negative carbon fibers, an insulating fiber diaphragm, positive carbon fibers, a positive material, structural resin and electrolyte.
Positive carbon fibers and negative carbon fibers are respectively laid on two sides of the insulating fiber diaphragm; wherein the surface of the anode carbon fiber is coated with a dot-matrix anode material; the insulating fiber diaphragm with the anode carbon fiber and the cathode carbon fiber laid on both sides is soaked in a mixed solution of structural resin and electrolyte (ionic electrolyte or solid electrolyte polymer) and cured.
The structural resin can be selected from epoxy resin, bismaleimide resin, polyimide resin, polyether ether ketone resin or phenolic resin.
The preparation method of the carbon fiber structure battery comprises the following steps:
step S1: mixing a conductive agent: adhesive: mixing the active materials according to a certain proportion, dissolving N-methyl pyrrolidone (NMP), and stirring to form anode slurry;
the conductive agent in the invention can be selected from acetylene black, conductive carbon black (Super P) and carbon nano tubes.
The binder may be selected from polyvinylidene fluoride (PVDF).
The active material can be one or more of ternary lithium metal oxide, lithium iron phosphate, lithium manganate and lithium cobaltate.
Ternary lithium metal oxides include LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811)、LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523)、LiNi 0.3 Co 0.3 Mn 0.3 O 2 (NCM111)。
Step S2: and laying an isolating film with lattice holes on the desized carbon fiber. The desized carbon fiber is obtained by calcining the carbon fiber in the air, the lattice holes of the isolating membrane can be obtained by cutting, the anode slurry obtained in the step S1 is coated on the isolating membrane, high-temperature drying is rapidly carried out in vacuum, the anode carbon fiber coated with the anode material distributed in a lattice manner is formed, and the carbon fiber after desizing is used as the cathode carbon fiber;
the lattice holes are holes which are arranged according to a certain periodic rule and are cut into geometric shapes.
And step S3: laying layers according to the sequence of the anode carbon fiber, the insulating fiber diaphragm and the cathode carbon fiber to form a prefabricated body;
and step S4: mixing electrolyte liquid and structural resin liquid under the anhydrous and anaerobic environment to form structural electrolyte;
the electrolyte liquid can be selected from ionic electrolyte or solid electrolyte solution; the ionic electrolyte is dissolved with LiPF 6 Or an ester or ether electrolyte of lithium bistrifluoromethanesulfonimide (LiTFSI); the solid electrolyte solution is an N-methylpyrrolidone (NMP) solution in which LiTFSI and polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) or polyethylene oxide (PEO) are dissolved.
Step S5: pouring the structural electrolyte in the step S4 into the prefabricated body in the step S3 in an anhydrous and oxygen-free environment, curing, and sealing holes by using structural resin again after curing;
step S6: and (5) testing and verifying mechanical and electrical properties to finish performance experiment verification.
The lattice distribution mode of the anode slurry can be determined according to test results or simulation, and the highest utilization rate of mechanical and electrical properties of the anode slurry is guaranteed.
In the following examples:
electrical property test standard: using a battery test system to perform single-rate constant-current charging and discharging on the battery with the obtained structure, and testing the energy density of the battery; the electrochemical workstation was used to test the structural cell impedance with an ac voltage amplitude of 0.01V, frequency range: 0.01Hz-100kHz.
Mechanical property test standard: the tensile test is according to ASTM D3039 standard test method for tensile property of polymer matrix composites, and the bending test is according to ASTM D790 standard test method for bending property of non-reinforced and reinforced plastics and electrical insulation materials.
Example 1
The carbon fiber structure battery of the embodiment comprises a cathode carbon fiber unidirectional tape, a high-strength plain glass fiber diaphragm, an anode carbon fiber unidirectional tape, an anode material, structural epoxy resin and LiPF 6 An ionic electrolyte; dot-matrix LiNi is paved and coated on two sides of the high-strength glass fiber diaphragm respectively 0.8 Co 0.1 Mn 0.1 O 2 (NCM 811) forming a preform from the positive carbon fiber unidirectional tape and the negative carbon fiber unidirectional tape of the positive electrode material, impregnating the whole preform with a mixed solution of a structural resin and an ionic electrolyte or a solid electrolyte polymer, and curing. Fig. 2 is a schematic diagram showing the dot matrix distribution of the cathode material on the cathode carbon fiber layer, wherein the plain weave substrate is only shown schematically, and the carbon fiber used in example 2 is in the form of a unidirectional tape.
The method comprises the following specific steps:
t1, mixing conductive carbon black particles (Super P): polyvinylidene fluoride (PVDF): liNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM 811) as 1:1:8, dissolving N-methyl pyrrolidone (NMP), and stirring for 20 hours to form anode slurry;
t2, calcining the T700 carbon fiber unidirectional tape subjected to desizing for 1.5 hours at 400 ℃ in the air to be used as a negative carbon fiber, taking a part of the desized carbon fiber, spreading a layer of isolating film with lattice holes on the carbon fiber, wherein the body structure of the isolating film with the lattice holes is a circular array with the cycle of 20mm and the diameter of 15mm, coating the positive slurry of T1, drying for 12 hours at 120 ℃ in vacuum, and drying NMP to obtain a positive carbon fiber 3 with the distribution of a lattice type positive material;
t3, sequentially laying a stainless steel foil with the thickness of 10 microns on a female die to serve as a positive current collector, laying a 0.1 mm-thick positive carbon fiber unidirectional tape containing dot-matrix NCM811 positive material distribution in one part of T2 as a positive electrode, laying a 0.1 mm-thick high-strength plain glass fiber diaphragm in the other part of T2 as a negative electrode 1, and laying the stainless steel foil again to serve as a negative current collector;
t4, in a glove box, under the argon atmosphere, mixing commercial normal-temperature curing structural resin (epoxy resin) and LiPF 6 Uniformly mixing the ionic electrolyte with equal mass, pouring the mixture into the prefabricated body stacked in the T3, sealing, vacuumizing, curing at 40 ℃, and sealing holes by using structural resin again after curing;
and T5, carrying out electrical performance test and mechanical performance test on the structural battery obtained by the T4 to finish performance verification.
The tensile modulus of the obtained structural battery is 37.5GPa, the tensile strength is 394.2MPa, the bending modulus is 30.9GPa, the bending strength is 272.5MPa, the energy density is 94.2Wh/kg, the impedance is 561 omega, and the structural battery has high mechanical property and electrical property.
Example 2
This example provides a structural battery prepared substantially the same as in example 1, except that: in step T2, an isolation film having another type of lattice holes is laid, as shown in fig. 3, the isolation film of the lattice holes has a physical structure of a square array with a side length of 8mm and a period of 10 mm.
The tensile modulus of the obtained structural battery is 34.9GPa, the tensile strength is 407.1MPa, the bending modulus is 32.7GPa, the bending strength is 311.2MPa, the energy density is 101.9Wh/kg, the impedance is 486 omega, and the structural battery has higher mechanical property and electrical property.
Comparative example 1
Comparative example 1 provides a structure battery prepared as follows:
t1, mixing conductive carbon black particles (Super P): polyvinylidene fluoride (PVDF): liNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM 811) as 1:1:8, dissolving N-methyl pyrrolidone (NMP), and stirring for 20 hours to form anode slurry;
t2, calcining the T700 carbon fiber unidirectional tape at 400 ℃ for 1.5h for desizing in air to obtain negative carbon fibers, uniformly coating a part of the negative carbon fibers on the T1 positive slurry, drying at 120 ℃ in vacuum for 12h, and drying NMP to obtain positive carbon fibers coated with energy storage substances;
t3, sequentially laying a stainless steel foil with the thickness of 10 microns on a female die to serve as a positive current collector, taking a positive carbon fiber unidirectional tape containing NCM811 positive material in one part of T2 as a positive electrode, taking a high-strength plain glass fiber with the thickness of 0.1mm in the other part of T2 as a negative electrode, and laying the stainless steel foil again to serve as a negative current collector;
t4, in a glove box, argon gasUnder the atmosphere, the structural epoxy resin and LiPF are mixed 6 Uniformly mixing the ionic electrolyte with equal mass, pouring the mixture into the prefabricated body stacked in the T3, sealing, vacuumizing, curing at 40 ℃, and sealing holes by using structural resin again after curing;
and T5, carrying out electrical performance test and mechanical performance test on the structural battery obtained by the T4 to finish performance verification.
The tensile modulus of the obtained structural battery is 24.50GPa, the tensile strength is 260.8MPa, the bending modulus is 16.1GPa, the bending strength is 235.2MPa, the energy density is 107.7Wh/kg, the impedance is 523 omega, the electrical properties are similar, but the mechanical properties are obviously poorer than those of the comparative example 1.
The uniform coating mode is adopted in the comparative example, so that the infiltration of the resin and the anode fiber is blocked, the layering is easy, and the mechanical property is poor.
In the description of the present application, it is to be understood that the terms "upper", "lower", "front", "rear", "left", "right", "vertical", "horizontal", "top", "bottom", "inner", "outer", and the like indicate orientations or positional relationships based on those shown in the drawings, and are only for convenience in describing the present application and simplifying the description, but do not indicate or imply that the referred device or element must have a specific orientation, be constructed in a specific orientation, and be operated, and thus, should not be construed as limiting the present application.
The foregoing description of specific embodiments of the present invention has been presented. It is to be understood that the present invention is not limited to the specific embodiments described above, and that various changes or modifications may be made by one skilled in the art within the scope of the appended claims without departing from the spirit of the invention. The embodiments and features of the embodiments of the present application may be combined with each other arbitrarily without conflict.
Claims (10)
1. A preparation method of a lattice type carbon fiber structure battery is characterized by comprising the following steps:
step S1: mixing the conductive particles, the binder and the active material, dissolving the mixture into a solvent, and uniformly stirring the mixture to form anode slurry;
step S2: laying a layer of isolating film with lattice holes on the desized carbon fiber, coating the anode slurry obtained in the step S1 on the isolating film, drying at high temperature in vacuum, and removing the isolating film to form the anode carbon fiber coated with the anode material distributed in a lattice manner; the desized carbon fiber is used as the cathode carbon fiber;
and step S3: the positive carbon fiber, the insulating fiber diaphragm and the negative carbon fiber are sequentially stacked;
and step S4: mixing electrolyte liquid and structural resin liquid according to a certain proportion under an anhydrous and oxygen-free environment to form structural electrolyte;
step S5: pouring the structural electrolyte in the step S4 into the prefabricated body in the step S3 in an anhydrous and oxygen-free environment, curing, and sealing holes by using structural resin again after curing; and manufacturing the lattice type carbon fiber structure battery.
2. The method for preparing a battery with a lattice-type carbon fiber structure according to claim 1, wherein the solvent is N-methylpyrrolidone in step S1.
3. The method for preparing the lattice-type carbon fiber structure battery according to claim 1, wherein in step S1, the conductive particles comprise conductive carbon black particles and acetylene black, and the binder comprises polyvinylidene fluoride (PVDF).
4. The method for preparing a battery with a lattice-type carbon fiber structure according to claim 1, wherein: in step S2, the positive carbon fiber and the negative carbon fiber are respectively woven into one of a unidirectional fabric, a plain fabric, a twill fabric, a satin fabric, and a three-dimensional woven fabric.
5. The method for preparing a lattice-type carbon fiber structure battery according to claim 1, wherein: in step S2, the holes on the isolation film with the lattice holes comprise regular geometric shapes.
6. The method for preparing a battery with a lattice-type carbon fiber structure according to claim 1, wherein: in step S2, the structural resin material includes epoxy resin, bismaleimide resin, polyimide resin, polyether ether ketone resin, or phenolic resin.
7. The method for preparing a battery with a lattice-type carbon fiber structure according to claim 1, wherein: in step S4, the electrolyte liquid includes an ionic electrolyte and a solid electrolyte solution.
8. The method for preparing a battery with a lattice-type carbon fiber structure according to claim 1, wherein in step S1, the active material comprises at least one of lithium iron phosphate, lithium manganate, lithium cobaltate, and ternary lithium metal oxide.
9. The method for manufacturing a lattice-type carbon fiber structure battery according to claim 1, wherein in step S4, the mixed electrolyte liquid is mixed with the structural resin liquid in equal mass.
10. A lattice-type carbon fiber structure battery produced by the production method according to any one of claims 1 to 9.
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| CN117525606A (en) * | 2023-11-15 | 2024-02-06 | 西安电子科技大学 | Functional battery with energy supply composite material structure distributed in large space structure and method |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN117525606A (en) * | 2023-11-15 | 2024-02-06 | 西安电子科技大学 | Functional battery with energy supply composite material structure distributed in large space structure and method |
| CN117525606B (en) * | 2023-11-15 | 2024-03-29 | 西安电子科技大学 | Functional battery with energy supply composite material structure distributed in large space structure and method |
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