CN114318593A

CN114318593A - Fullerene-doped high-regularity carbon nanofiber and preparation method and application thereof

Info

Publication number: CN114318593A
Application number: CN202111509696.7A
Authority: CN
Inventors: 张烨; 朱波; 乔琨; 高学平; 虞军伟; 闫书涵
Original assignee: Shandong University
Current assignee: Shandong University
Priority date: 2021-12-10
Filing date: 2021-12-10
Publication date: 2022-04-12
Anticipated expiration: 2041-12-10
Also published as: CN114318593B

Abstract

The invention belongs to the field of high-performance fibers and preparation and composite materials, and relates to a fullerene-doped high-regularity carbon nanofiber and a preparation method and application thereof, wherein a fullerene material is mainly used as a carbon element additive for preparing the carbon nanofiber, specifically, acrylonitrile and the carbon element additive are polymerized through aqueous phase precipitation to form a precursor raw material compounded by the carbon element additive and polyacrylonitrile, and the precursor raw material is sequentially subjected to spinning, hot drawing, pre-oxidation, carbonization and graphitization to obtain the fullerene-doped high-regularity carbon nanofiber; the carbonaceous element additive is a fullerene material. The invention can prevent the agglomeration of the carbon element additive, reduce the defects of the carbon nanofiber, and enable the composite carbon nanofiber to have higher strength and toughness, light weight and excellent thermal stability.

Description

Fullerene-doped high-regularity carbon nanofiber and preparation method and application thereof

Technical Field

The invention belongs to the field of high-performance fibers and preparation and composite materials, and relates to fullerene-doped high-regularity carbon nanofibers and a preparation method and application thereof.

Background

The information in this background section is only for enhancement of understanding of the general background of the invention and is not necessarily to be construed as an admission or any form of suggestion that this information forms the prior art that is already known to a person of ordinary skill in the art.

The carbon fiber is a novel inorganic fiber material with excellent performances such as high strength, high modulus, low density, high heat conductivity and electric conductivity. The carbon fiber can be spun from a plurality of precursors, wherein polyacrylonitrile is the most promising precursor for producing high-performance carbon fiber, and the polyacrylonitrile-based carbon fiber occupies more than 90 percent of the total production of the carbon fiber in the world by virtue of the excellent comprehensive performance of the polyacrylonitrile-based carbon fiber.

The polyacrylonitrile-based carbon fiber can be prepared by a plurality of processes, and since the electrostatic spinning technology is mature, the carbon nanofiber prepared by the technology is greatly developed, compared with the complex and strict spinning process of the carbon fiber, the process for preparing the carbon nanofiber by electrostatic spinning is simpler, and the process parameters can be conveniently adjusted. However, the simple process also has many disadvantages, such as poor orientation of the carbon nanofibers, often accompanied by rough surface and bead structure, etc., so that the application of the carbon nanofibers to functional materials, such as energy storage devices, catalysts or catalyst carriers, etc., is limited at present. Although there are many differences in the macrostructure of carbon fibers and carbon nanofibers, there is a great similarity in the internal structure of both, and thus results obtained in the research of carbon nanofibers can effectively guide the production of carbon fibers.

At present, the main reasons for restricting the improvement of the performance of the carbon nanofiber are that the internal defects of the fiber are more, and the integrity and the orientation of a graphitized structure are poorer. The performance of the carbon nanofibers can be improved by adding a modifying substance. The carbonaceous element additives, such as carbon nanotubes, graphene and derivatives thereof, have the same honeycomb graphite lattice structure as that of an ideal carbon nanofiber, can promote the formation of a graphitized structure in the fiber carbonization process, and are widely used as a nucleating agent and a template agent of the carbon nanofiber.

Disclosure of Invention

In order to solve the defects of the prior art, the invention aims to provide the fullerene-doped high-regularity carbon nanofiber as well as the preparation method and the application thereof.

In order to achieve the purpose, the technical scheme of the invention is as follows:

on one hand, compared with the graphene and the carbon nano tube which are widely applied at present, the fullerene material serving as the carbon element additive has the following unique advantages:

(1) compared with a one-dimensional carbon nanotube and two-dimensional graphene, the fullerene is a zero-dimensional nanosphere, the structure of the fullerene is smaller, the fullerene is of a nano-scale size in all directions, the smaller size enables the contact area of the additive and a fiber matrix to be larger, and therefore the interaction generated by contact is stronger; (2) the carbon nano tube and the graphene are easy to deform in the fiber matrix such as bending, winding and twisting, and further induce the generation of lattice distortion, and compared with the fullerene spherical structure, the deformation is avoided, so that the morphology control in the matrix is easier when the fullerene spherical structure is used as an additive; (3) the spherical structure of the fullerene can disperse force to all atoms, so that the structure is more stable; (4) the smaller size of the fullerene enables the fullerene to move along with the fiber matrix when the fiber is deformed, the deformation coordination of the filler and the matrix is more consistent, and further the fullerene can continuously generate secondary bonding with the fiber matrix when the fiber is drawn, so that the reinforcing effect is continuously realized, and finally the toughness of the fiber is improved; (5) the fullerene has high electron accepting capacity, can adsorb free radicals generated by a fiber matrix in the process of pyrolysis and deformation, prevents the structure from further deterioration, and plays a role in self-healing.

According to the invention, a fullerene material is selected as a carbonaceous element additive, the fullerene material can be fullerene, and can also be a fullerene derivative with hydroxyl, carboxyl or other functional groups and inorganic particles distributed on the surface, the spherical structure can be a single layer or a multilayer, and the particle size of the fullerene material is 0.5-500 nm. Compared with other carbon element additives such as carbon nanotubes and graphene, the fullerene material has a smaller isotropic nano size and is excellent in pressure resistance, hardness, toughness and electrical conductivity. Research shows that when the fullerene material is used as the carbonaceous element additive to prepare the carbon nanofiber, the strength and toughness of the carbon nanofiber can be improved simultaneously, and the preparation method has profound significance in engineering application.

On the other hand, the preparation method of the fullerene-doped high-regularity carbon nanofiber comprises the steps of carrying out aqueous phase precipitation polymerization on acrylonitrile and a carbonaceous element additive to form a precursor raw material compounded by the carbonaceous element additive and polyacrylonitrile, and sequentially carrying out spinning, hot drawing, pre-oxidation, carbonization and graphitization on the precursor raw material to obtain the fullerene-doped high-regularity carbon nanofiber; the carbonaceous element additive is a fullerene material.

According to the invention, the fullerene material is used as the carbonaceous element additive, so that the fullerene and the polyacrylonitrile can be mixed on a molecular scale to obtain the nano composite, the agglomeration of the fullerene is limited by the interaction of the polyacrylonitrile and the fullerene, and the defects in the fiber are reduced. Meanwhile, the fullerene has a honeycomb graphite lattice structure, and polyacrylonitrile can be induced to form the same graphite structure step by step in heat treatment through the template effect of the structure of the fullerene, so that the graphitization degree of the carbon nanofiber is deeply improved, and finally the strength and toughness of the fiber are greatly improved.

In a third aspect, a fullerene doped high-regularity carbon nanofiber is obtained by the preparation method.

In a fourth aspect, the fullerene-doped high-regularity carbon nanofiber is applied to a hydrogen storage material, a high-capacity electrode material, a high-strength high-toughness fiber-reinforced composite material and/or a fuel cell electrode material.

The invention has the beneficial effects that:

1. the polyacrylonitrile/fullerene nano composite material is prepared according to the principle of in-situ polymerization, the fullerene is uniformly doped in the carbon nano fibers by taking the polyacrylonitrile/fullerene nano composite material as a raw material, the uniform doping of the fullerene among polyacrylonitrile molecules can be directly realized after the polyacrylonitrile/fullerene nano composite material is dissolved, the condition that the fullerene is not uniformly distributed due to molecular entanglement is avoided to a limited extent, and the production efficiency is greatly improved.

2. According to the invention, fullerene is added into the carbon nanofiber structure, so that the fullerene can play a role of nano filler in the nanofiber, thereby inhibiting the expansion of cracks and enabling the cracks to deflect, and further, more energy is consumed for the breakage of the fibers; in addition, the nano-scale spherical structure of the fullerene enables the fullerene to have better mobility when the fiber is subjected to drawing deformation, and can form continuous interaction with a fiber matrix through secondary bonding; meanwhile, the fullerene can adsorb free radicals generated when a molecular chain is broken by virtue of high electron accepting capacity of the fullerene, so that the fullerene is prevented from causing further deterioration of a fiber structure, and finally, the strength and toughness of the carbon nanofiber are improved under the enhancement of the fullerene.

3. The carbon nanofiber prepared by the method is prepared by adopting an electrostatic spinning technology, the as-spun fiber is split and drawn in an electric field to be gradually refined, and in addition, the addition of the fullerene can improve the conductivity of a spinning solution and further enhance the drawing effect of the electric field on the fiber. After spinning, the fiber is subjected to certain hot drafting above the glass transition temperature of polyacrylonitrile, so that the fiber diameter can be further reduced, and the fiber orientation is improved. A series of treatments can realize fine denier of fiber, eliminate the influence of a sheath-core structure, enable the internal structure of the fiber to be more uniform, and simultaneously the fine denier of the fiber reduces the number of defects in unit length.

4. According to the invention, fullerene is introduced into the polyacrylonitrile-based nanofiber, and the fullerene can play a role of a crystal core in the carbonization and graphitization processes, so that a more complete and better-oriented graphite lattice structure is formed inside the polyacrylonitrile-based carbon nanofiber in the process, and the mechanical properties, the electric conduction and the heat conduction of the fiber are improved.

Drawings

The accompanying drawings, which are incorporated in and constitute a part of this specification, are included to provide a further understanding of the invention, and are incorporated in and constitute a part of this specification, illustrate exemplary embodiments of the invention and together with the description serve to explain the invention and not to limit the invention.

FIG. 1 is a scanning electron microscope photograph of polyacrylonitrile/fullerene nano-composite particles obtained by aqueous phase precipitation polymerization in example 2 of the present invention.

FIG. 2 is a scanning electron micrograph of a strand obtained by electrospinning according to example 2 of the present invention.

Fig. 3 is a scanning electron microscope photograph of carbon nanofibers obtained by drawing, pre-oxidizing and carbonizing the precursor filaments in example 2 of the present invention.

FIG. 4 is a thermogravimetric analysis plot of the filaments heated to 950 ℃ in a nitrogen atmosphere in example 2 of the present invention.

FIG. 5 is a graph showing the comparative breaking stress of carbon nanofibers prepared from a nanocomposite material comprising pure polyacrylonitrile and 5 wt% of multi-wall fullerene as raw materials in example 2 of the present invention.

FIG. 6 is a comparison graph of elongation at break of carbon nanofibers prepared from a nanocomposite material comprising pure polyacrylonitrile and 5 wt% of multi-wall fullerene added thereto in example 2 of the present invention.

Detailed Description

It is to be understood that the following detailed description is exemplary and is intended to provide further explanation of the invention as claimed. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.

It is noted that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of exemplary embodiments according to the invention. As used herein, the singular forms "a", "an" and "the" are intended to include the plural forms as well, and it should be understood that when the terms "comprises" and/or "comprising" are used in this specification, they specify the presence of stated features, steps, operations, devices, components, and/or combinations thereof, unless the context clearly indicates otherwise.

The fullerene material can be fullerene, or a fullerene derivative with hydroxyl, carboxyl or other functional groups and inorganic particles distributed on the surface, can be a single layer or a multilayer, and the particle size of the fullerene material is 0.5-500 nm. Fullerene means a mixture of mainly sp²The hollow molecule composed of hybridized carbon atoms is in the shape of sphere, ellipsoid or column, can be in single layer or multilayer, and the carbon atoms are formed in the form of five-membered ring or six-membered ring (occasionally containing seven-membered ring).

The invention provides a fullerene-doped high-regularity carbon nanofiber and a preparation method and application thereof, and solves the problems that the size of the added carbon nanotube and graphene is still large, agglomeration is easy to generate, the improvement of the fiber performance is limited and the like in the existing carbon nanofiber.

In a typical embodiment of the present invention, an application of fullerene material as an additive of carbon element in preparing carbon nanofiber is provided.

The invention selects the nano material with more perfect graphite lattice structure and smaller size of the fullerene material, and has excellent compression resistance, hardness, toughness and conductivity. Research shows that when the fullerene material is used as the additive of the carbon element to prepare the carbon nanofiber, the dispersibility of the carbon nanofiber is greatly improved, and the mechanical properties (strength, toughness and the like, especially toughness) and the thermal stability of the carbon nanofiber can be improved.

According to another embodiment of the invention, a preparation method of fullerene-doped high-regularity carbon nanofibers is provided, acrylonitrile and a carbonaceous additive are subjected to aqueous phase precipitation polymerization to form a precursor raw material compounded by the carbonaceous additive and polyacrylonitrile, and the precursor raw material is subjected to spinning, hot drawing, pre-oxidation, carbonization and graphitization in sequence to obtain the fullerene-doped high-regularity carbon nanofibers; the carbonaceous element additive is a fullerene material.

According to the invention, the fullerene material is used as the carbonaceous element additive, so that the fullerene and the polyacrylonitrile can be mixed on a molecular scale to obtain the nano composite, the agglomeration of the fullerene is limited by the interaction of the polyacrylonitrile and the fullerene, and the defects in the fiber are reduced. The doped fullerene material can promote the graphitization process of the fiber through the interaction of the doped fullerene material and the polyacrylonitrile matrix, and the strength and the toughness of the fiber are improved.

The aqueous phase precipitation polymerization in the invention refers to a polymerization method that a polymerization monomer (acrylonitrile) and an initiator can be dissolved in water, but a polymer (polyacrylonitrile) generated by polymerization is not dissolved in water to generate precipitation.

In the aqueous precipitation polymerization, the initiator is usually a water-soluble initiator such as persulfate (ammonium persulfate, potassium persulfate, etc.). In some embodiments, the initiator in the aqueous phase precipitation polymerization is a mixture of a persulfate and ammonium sulfite. By adding ammonium sulfite, the reaction activation energy is reduced, the initiation effect of the initiation system is better, and the dispersion effect of polyacrylonitrile and fullerene materials is improved.

The initiator functions on the principle that after being heated, the initiator is decomposed to generate free radicals, and the free radicals can initiate vinyl compounds to continuously generate free radicals, so that free radical polymerization is formed. The initiator for the aqueous phase precipitation polymerization generally contains persulfate, the optimum initiation temperature of the persulfate is about 80 ℃, and the reaction activation energy is reduced after the ammonium sulfite is added, so that the reaction temperature can be reduced, and in one or more embodiments, the temperature of the aqueous phase precipitation polymerization is 40-80 ℃. The reaction time is 60-180 min. The molecular weight is between 10000 and 1000000.

In some embodiments, the fullerene material is added in an amount of 0.01 to 50 wt% of the mass of the acrylonitrile. The content of acrylonitrile is controlled to be 10-30 wt% of the total mass of a polymerization system.

In some embodiments, the spinning is electrospinning. In one or more embodiments, the precursor material is dissolved in an organic solvent to form a dope, and the dope is electrospun. The solvent used may be dimethyl sulfoxide, dimethyl formamide, dimethyl acetamide, etc. The concentration of the precursor raw material in the spinning solution is 5-50 wt%. The specific process of electrostatic spinning comprises the following steps: pouring the spinning solution into a needle tube of electrostatic spinning, wherein the needle tube is provided with a needle head with the diameter of 0.1-1 mm, spinning is carried out under the conditions of 30-300 KV electric field intensity and 0.1-10 ml/h liquid supply speed after assembly, the electric field intensity and the liquid supply speed are different according to the polymer molecular weight and the factors such as concentration, viscosity, conductivity and the like of a spinning solution, the prepared nanofibers are uniformly distributed on a yarn collecting roller under the action of a sliding table, and the rotating speed of the yarn collecting roller is 100-1000 rpm.

The hot drawing refers to that the fibers of the nanofiber felt integrally spun after spinning are primarily oriented under the action of a yarn collecting roller, the fibers are trimmed into strips along the orientation direction, and the fibers are drawn under the heating condition of applying force at two ends. In some embodiments, the hot drawing temperature is 100-150 ℃ and the drawing ratio is 1.5-4.

The pre-oxidation refers to heating oxidation in an air medium, and in some embodiments, the pre-oxidation temperature is 150-300 ℃ and the pre-oxidation time is 30-120 min.

The carbonization refers to a thermal treatment process in which pyrolysis is performed under the protection of inert gas or in a vacuum state. In some embodiments, the carbonization temperature is 1000-1600 ℃ and the carbonization time is 5-20 min.

The graphitization refers to a process of heating for graphitization treatment under the protection of inert gas or in a vacuum state. In some embodiments, the graphitization temperature is 2000-3500 ℃, and the graphitization time is 30-150 s.

In a third embodiment of the invention, a fullerene-doped high-regularity carbon nanofiber is provided, which is obtained by the preparation method.

In a fourth embodiment of the present invention, an application of the fullerene-doped high-regularity carbon nanofiber as a hydrogen storage material, a high-capacity electrode material, a high-performance composite material and/or a fuel cell electrode material is provided.

In order to make the technical solutions of the present invention more clearly understood by those skilled in the art, the technical solutions of the present invention will be described in detail below with reference to specific embodiments.

Example 1

Adding 10ml of acrylonitrile and 0.08g of fullerene into 60ml of water, uniformly mixing, dropwise adding 10ml of aqueous solution dissolved with 0.3g of ammonium sulfite and 0.3g of ammonium persulfate to initiate polymerization, heating to 60 ℃, polymerizing for 120min, washing and drying the generated precipitate to obtain the polyacrylonitrile/fullerene composite material powder.

Adding 2g of the polyacrylonitrile/fullerene composite material powder into 10ml of dimethyl sulfoxide, heating to 60 ℃, uniformly stirring to obtain a spinning stock solution, pouring the spinning stock solution into a needle tube with the volume of 20ml, assembling an electrostatic spinning needle with the inner diameter of 0.5mm on the needle tube, and carrying out electrostatic spinning, wherein the electrostatic spinning process parameters are as follows: the temperature is 40 ℃, the liquid supply speed is 3ml/h, the electric field intensity is 100kV/m, the moving speed of the sliding table is 10mm/s, the rotating speed of the filament collecting roller is 500rpm, and the nano fiber felt (namely protofilament) is obtained after the solution is completely consumed, namely electrostatic spinning is completed.

The nanofiber mat was cut into a long strip 5cm long and 2cm wide in accordance with the orientation obtained by the take-up roll, and the long strip was stretched to 15cm at 135 ℃ (one end of the long strip was fixed with a clip, and the other end was stretched by a weight) to obtain a nanofiber ribbon.

And (3) pre-oxidizing the hot-drawn nanofiber strip at 280 ℃ for 2h, carbonizing at 1500 ℃ for 5min, and graphitizing at 3000 ℃ for 50s to obtain the final carbon nanofiber.

Example 2

Adding 10ml acrylonitrile and 0.4g multi-wall fullerene (namely carbon nano onion) into 60ml water, uniformly mixing, dropwise adding 10ml aqueous solution dissolved with 0.3g ammonium sulfite and 0.3g ammonium persulfate to initiate polymerization, heating to 65 ℃, polymerizing for 150min, washing and drying the generated precipitate to obtain the polyacrylonitrile/multi-wall fullerene composite material powder, wherein the powder is shown in figure 1.

Adding 1.5g of the polyacrylonitrile/multi-wall fullerene composite material powder into 10ml of dimethylformamide, heating to 60 ℃, uniformly stirring to obtain a spinning stock solution, pouring the spinning stock solution into a needle tube with the volume of 20ml, assembling an electrostatic spinning needle with the inner diameter of 0.5mm on the needle tube, and carrying out electrostatic spinning, wherein the electrostatic spinning process parameters are as follows: the temperature is 40 ℃, the liquid supply speed is 2ml/h, the electric field intensity is 80kV/m, the moving speed of the sliding table is 15mm/s, the rotating speed of the filament collecting roller is 1000rpm, and the nano fiber felt (namely protofilament) is obtained after the solution is completely consumed, namely electrostatic spinning is completed, as shown in figure 2.

The hot-drawn nanofiber strips were pre-oxidized at 300 ℃ for 1.5h, carbonized at 1500 ℃ for 10min and graphitized at 2800 ℃ for 50s to obtain the final carbon nanofibers, as shown in fig. 3.

The thermogravimetric analysis of the precursor is shown in fig. 4, and it can be seen that the residual weight of the precursor prepared from pure polyacrylonitrile after heating to 950 ℃ is 27.6%, while the weight of the precursor added with 5 wt% of multi-wall fullerene is increased to 37.8%, which proves that the multi-wall fullerene improves the heat resistance of the fiber matrix, and the multi-wall fullerene adsorbs radicals generated by pyrolysis, thereby preventing the structure from further deterioration.

The breaking stress of the carbon nanofibers, as shown in fig. 5, was increased from 17.4MPa to 25MPa to see that the breaking stress of the finally prepared carbon nanofibers after addition of 5 wt% multi-walled fullerene was increased to 25MPa compared to the control group without addition of multi-walled fullerene. The reason for the increase in fiber breaking stress is: a. the multi-wall fullerene can hinder the crack from expanding and promote the crack branching when the fiber is drawn, so that the energy required by the fracture is increased; b. the multi-wall fullerene can induce the fiber matrix to form a more perfect graphite lattice structure in the heat treatment, and the perfect structure enables the fiber matrix to bear stronger drafting; c. the fullerene can adsorb free electrons generated by molecular chain fracture, and further deterioration of the structure is prevented.

As shown in fig. 6, the elongation at break of the carbon nanofiber was increased from 1.35% to 3.27% in comparison with the control group containing no multi-wall fullerene, and it was observed that the elongation at break of the finally prepared carbon nanofiber was increased by 5 wt% of the multi-wall fullerene. The increase in the elongation at break of the fiber is due to: the multi-wall fullerene can move along with the fiber matrix when the fiber matrix is subjected to drafting deformation, and secondary bonding is continuously generated, so that the continuous reinforcing effect on the fiber matrix is achieved.

Example 3

Adding 10ml of acrylonitrile and 0.8g of carboxylated fullerene (prepared by carrying out ultrasonic treatment on 1g of fullerene in 30ml of concentrated sulfuric acid and 10ml of concentrated nitric acid at 40 ℃ for 3 h) into 100ml of water, uniformly mixing, dropwise adding 10ml of aqueous solution in which 0.4g of ammonium sulfite and 0.4g of ammonium persulfate are dissolved to initiate polymerization, heating to 70 ℃, polymerizing for 120min, washing and drying the generated precipitate to obtain the polyacrylonitrile/carboxylated fullerene composite material powder.

Adding 1g of the polyacrylonitrile/carboxylated fullerene composite material powder into 10ml of dimethylacetamide, heating to 70 ℃, uniformly stirring to obtain a spinning stock solution, pouring the spinning stock solution into a needle tube with the volume of 20ml, wherein the needle tube is provided with an electrostatic spinning needle with the inner diameter of 0.5mm, and performing electrostatic spinning, wherein the electrostatic spinning process parameters are as follows: the temperature is 45 ℃, the liquid supply speed is 2ml/h, the electric field intensity is 120kV/m, the moving speed of the sliding table is 10mm/s, the rotating speed of the filament collecting roller is 100rpm, and the nano fiber felt (namely protofilament) is obtained after the solution is completely consumed, namely electrostatic spinning is completed.

And pre-oxidizing the hot-drawn nanofiber strip at 300 ℃ for 1h, carbonizing at 1300 ℃ for 5min, and graphitizing at 2800 ℃ for 50s to obtain the final carbon nanofiber.

The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.

Claims

1. An application of fullerene material as a carbonaceous element additive in preparing carbon nano-fiber.

2. A preparation method of fullerene-doped high-regularity carbon nanofibers comprises the steps of carrying out aqueous phase precipitation polymerization on acrylonitrile and a carbonaceous element additive to form a precursor raw material compounded by the carbonaceous element additive and polyacrylonitrile, and sequentially carrying out spinning, hot drawing, pre-oxidation, carbonization and graphitization on the precursor raw material to obtain the fullerene-doped high-regularity carbon nanofibers; the method is characterized in that the carbonaceous element additive is a fullerene material.

3. The method for preparing fullerene-doped highly-regular carbon nanofiber as claimed in claim 2, wherein the initiator in the aqueous phase precipitation polymerization is a mixture of persulfate and ammonium sulfite;

preferably, the temperature of the aqueous phase precipitation polymerization is 40-80 ℃.

4. The method of preparing fullerene-doped highly-regular carbon nanofibers according to claim 2, wherein the spinning is electrospinning; preferably, the precursor raw material is dissolved in an organic solvent to prepare a spinning solution, and the spinning solution is used for electrostatic spinning.

5. The method for producing a fullerene-doped highly-regular carbon nanofiber as set forth in claim 2, wherein the temperature of the hot drawing is 100 to 150 ℃ and the drawing ratio is 1.5 to 4.

6. The method of claim 2, wherein the pre-oxidation temperature is 150-300 ℃ and the pre-oxidation time is 30-120 min.

7. The method of claim 2, wherein the carbonization temperature is 1000-1600 ℃ and the carbonization time is 5-20 min.

8. The method of claim 2, wherein the graphitization temperature is 2000-3500 ℃ and the graphitization time is 30-150 s.

9. A fullerene-doped highly-regular carbon nanofiber obtained by the production method according to any one of claims 2 to 8.

10. Use of fullerene-doped highly-ordered carbon nanofiber as claimed in claim 9 as hydrogen storage material, high capacity electrode material, high performance composite material and/or fuel cell electrode material.