CN114318593A - Fullerene-doped carbon nanofibers with high regularity and their preparation methods and applications - Google Patents

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 carbon nanofibers with high regularity and their preparation methods and applications

technical field

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

Background technique

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

Carbon fiber is a new type of inorganic fiber material with excellent properties such as high strength, high modulus, low density, and high thermal conductivity. Carbon fiber can be spun from many precursors. Among them, polyacrylonitrile is the most promising precursor for the production of high-performance carbon fibers. Polyacrylonitrile-based carbon fibers account for more than 90% of the current world carbon fiber production due to its excellent comprehensive properties.

Polyacrylonitrile-based carbon fibers can be prepared by many processes. Since the electrospinning technology has matured, carbon nanofibers prepared by this technology have been greatly developed. Compared with the complex and strict spinning process of carbon fibers, electrospinning The process of preparing carbon nanofibers is simpler, and the process parameters can be easily adjusted. However, the simple process also brings many disadvantages, such as poor orientation of carbon nanofibers, often accompanied by rough surface and beaded structure, etc. Therefore, the current application of carbon nanofibers is mostly limited to functional materials, such as energy storage devices, catalysts or catalysts carrier etc. Although there are many differences between carbon fibers and carbon nanofibers in terms of macrostructure, there are great similarities in their internal structures, so the results obtained in carbon nanofiber research can effectively guide the production of carbon fibers.

At present, the main reason that restricts the improvement of carbon nanofiber performance is that there are many internal defects in the fiber, and the integrity and orientation of the graphitized structure are poor. The properties of carbon nanofibers can be improved by adding modifying substances. Carbonaceous element additives, such as carbon nanotubes, graphene and their derivatives, have the same honeycomb graphite lattice structure as the ideal carbon nanofiber structure, which can promote the formation of graphitized structure during fiber carbonization, and are widely used. are used as nucleating and templating agents for carbon nanofibers, however, the inventors found that the size of carbon nanotubes and graphene is still relatively large relative to the nanoscale size of carbon nanofibers, which is easy to cause inside carbon fibers. The phenomenon of non-uniform structure, in addition, agglomeration will occur at a slightly higher concentration, which greatly limits the improvement of fiber properties.

SUMMARY OF THE INVENTION

In order to solve the deficiencies of the prior art, the purpose of the present invention is to provide fullerene-doped carbon nanofibers with high regularity and a preparation method and application thereof. The present invention can prevent the agglomeration of carbonaceous element additives and reduce the defects of carbon nanofibers. , and can make the composite carbon nanofibers have high strength and toughness, light weight, and excellent thermal stability.

In order to achieve the above object, the technical scheme of the present invention is:

On the one hand, the application of a fullerene material as a carbonaceous element additive in the preparation of carbon nanofibers, compared with the currently widely used graphene and carbon nanotubes, fullerenes have the following unique advantages:

(1) Compared with one-dimensional carbon nanotubes and two-dimensional graphene, fullerenes are zero-dimensional nanospheres with smaller structures and nanoscale dimensions in all directions. The contact area between the additive and the fiber matrix is larger, so the interaction through contact will be stronger; (2) carbon nanotubes and graphene are easily deformed in the fiber matrix by bending, entanglement, torsion, etc., and then induce the formation of lattice In contrast, the spherical structure of fullerene does not undergo the above deformation, making it easier to control the morphology in the matrix when used as an additive; (3) the spherical structure of fullerene can disperse the force to all atoms , the structure is more stable; (4) the smaller size of the fullerene enables it to move with the fiber matrix when the fiber is deformed, and the deformation coordination between the filler and the matrix is more consistent, and then when the fiber is stretched, the fullerene can move with the fiber matrix. It continuously produces secondary bonds with the fiber matrix, which continues to enhance the fiber's toughness. , to prevent further deterioration of the structure and play a "self-healing" role.

The present invention selects a fullerene material as the carbonaceous element additive, and the fullerene material can be fullerene, or can be a fullerene derivative with hydroxyl, carboxyl or other functional groups and inorganic particles distributed on the surface, and its spherical structure It can be a single layer or a multi-layer, and the particle size of the fullerene material is between 0.5 and 500 nm. Compared with other carbonaceous element additives such as carbon nanotubes and graphene, fullerene materials have a smaller isotropic nanometer size, and have excellent compression resistance, hardness, toughness, and electrical conductivity. Studies have shown that when fullerenes are used as carbonaceous element additives to prepare carbon nanofibers, the strength and toughness of carbon nanofibers can be improved at the same time, which has far-reaching significance in engineering applications.

On the other hand, a preparation method of a fullerene-doped carbon nanofiber with high regularity comprises acrylonitrile and a carbonaceous element additive through water-phase precipitation polymerization to form a composite precursor raw material of the carbonaceous element additive and polyacrylonitrile, Spinning, thermal drawing, pre-oxidation, carbonization, and graphitization of precursor raw materials are performed in sequence to obtain fullerene-doped carbon nanofibers with high regularity; the carbonaceous element additive is a fullerene material.

The present invention adopts fullerene material as carbonaceous element additive, and can mix fullerene and polyacrylonitrile to obtain nano-composite at molecular scale, and the interaction between polyacrylonitrile and fullerene limits the difference between fullerenes. The agglomeration reduces defects in the fibers. At the same time, fullerene has a honeycomb graphite lattice structure, which can induce polyacrylonitrile to gradually form the same graphite structure during heat treatment through the template effect of its structure, which can deeply improve the degree of graphitization of carbon nanofibers, and finally increase the strength and toughness of the fiber. greatly improved.

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

In a fourth aspect, an application of the above-mentioned fullerene-doped high-regularity carbon nanofiber as a hydrogen storage material, a high-capacity electrode material, a high-strength and high-toughness fiber-reinforced composite material, and/or a fuel cell electrode material.

The beneficial effects of the present invention are:

1. The present invention prepares polyacrylonitrile/fullerene nanocomposite materials according to the principle of in-situ polymerization and uses it as a raw material to realize the uniform doping of fullerenes in carbon nanofibers, and the polyacrylonitrile/fullerene nanocomposites After the composite material is dissolved, the uniform doping of fullerenes between polyacrylonitrile molecules can be directly achieved, which limits the uneven distribution of fullerenes caused by molecular entanglement, and greatly improves the production efficiency.

2. In the present invention, fullerene is added to the carbon nanofiber structure, and fullerene can play the role of nanofiller in the nanofiber, hinder the expansion of cracks and deflect the cracks, so that the breaking of the fiber needs to consume more In addition, the nanoscale spherical structure of fullerene makes it have better mobility when the fiber is stretched and deformed, and can form continuous interaction with the fiber matrix through secondary bonding; Its high electron-accepting ability can adsorb the free radicals generated when the molecular chain is broken, preventing it from causing further deterioration of the fiber structure. Finally, the strength and toughness of carbon nanofibers are improved under the reinforcement of fullerenes.

3. The carbon nanofibers prepared by the present invention are prepared by electrospinning technology, and the initially spun fibers are split and drawn in an electric field to be gradually refined. In addition, the addition of fullerenes can improve the conductivity of the spinning solution, further enhancing the The effect of electric field on fiber drafting. After spinning, the fiber is thermally drawn to a certain extent above the glass transition temperature of polyacrylonitrile, which can further reduce the fiber diameter and improve the orientation of the fiber. A series of treatments can realize the fine denier of the fiber, eliminate the influence of the skin-core structure, make the internal structure of the fiber more uniform, and at the same time, the fine denier of the fiber reduces the number of defects per unit length.

4. In the present invention, fullerenes are introduced into polyacrylonitrile-based nanofibers, and in the process of carbonization and graphitization, fullerenes can play the role of crystalline cores, inducing the formation of more complete, more complete, and more complete, polyacrylonitrile-based carbon nanofibers in the process. A graphite lattice structure with better orientation is beneficial to the improvement of mechanical properties, electrical and thermal conductivity of fibers.

Description of drawings

The accompanying drawings forming a part of the present invention are used to provide further understanding of the present invention, and the exemplary embodiments of the present invention and their descriptions are used to explain the present invention, and do not constitute an improper limitation of the present invention.

1 is a scanning electron microscope photograph of polyacrylonitrile/fullerene nanocomposite particles obtained by aqueous precipitation polymerization in Example 2 of the present invention.

Fig. 2 is a scanning electron microscope photograph of the precursor yarn obtained by electrospinning in Example 2 of the present invention.

Fig. 3 is a scanning electron microscope photograph of carbon nanofibers obtained after the raw silk is drawn, pre-oxidized and carbonized in Example 2 of the present invention.

FIG. 4 is a thermogravimetric analysis graph obtained by heating the raw silk to 950° C. in a nitrogen atmosphere in Example 2 of the present invention.

FIG. 5 is a comparison diagram of the fracture stress of carbon nanofibers prepared by using pure polyacrylonitrile and a nanocomposite material with 5wt% multi-wall fullerene as raw materials in Example 2 of the present invention.

6 is a comparison diagram of the elongation at break of carbon nanofibers prepared by using pure polyacrylonitrile and a nanocomposite material with 5wt% multi-wall fullerene as raw materials in Example 2 of the present invention.

Detailed ways

It should be noted that the following detailed description is exemplary and intended to provide further explanation of the invention. Unless otherwise defined, 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 should be noted that the terminology used herein is for the purpose of describing specific embodiments only, and is not intended to limit the exemplary embodiments according to the present invention. As used herein, unless the context clearly dictates otherwise, the singular is intended to include the plural as well, furthermore, it is to be understood that when the terms "comprising" and/or "including" are used in this specification, it indicates that There are features, steps, operations, devices, components and/or combinations thereof.

The fullerene material of the present invention can be fullerene, or can be a fullerene derivative with hydroxyl, carboxyl or other functional groups and inorganic particles distributed on the surface, and can be a single layer or a multilayer. The particle size of the alkene material is between 0.5 and 500 nm. Fullerene refers to a hollow molecule mainly composed of sp hybridized carbon atoms, which is spherical, ellipsoidal or cylindrical in shape, and can be single ^- layer or multi-layer. Formed in the form of a membered ring (occasionally containing a seven-membered ring).

The existing carbon nanofibers have problems such as adding carbon nanotubes and graphene, which are still relatively large in size, prone to agglomeration, and restricting the improvement of fiber performance. The present invention proposes fullerene-doped carbon nanofibers with high regularity and preparation thereof methods and applications.

A typical embodiment of the present invention provides the application of a fullerene material as a carbonaceous element additive in the preparation of carbon nanofibers.

In the present invention, the fullerene material is selected as a nanomaterial with a relatively perfect graphite lattice structure and a smaller size, and has excellent compression resistance, hardness, toughness and electrical conductivity. Studies have shown that when fullerene materials are used as carbonaceous element additives to prepare carbon nanofibers, the dispersibility is greatly improved, and the mechanical properties (strength, toughness, etc., especially toughness) and thermal stability of carbon nanofibers can be improved. .

Another embodiment of the present invention provides a method for preparing fullerene-doped carbon nanofibers with high regularity. Acrylonitrile and carbonaceous element additives are polymerized by aqueous precipitation to form carbonaceous element additives and polypropylene The precursor raw material of nitrile composite is subjected to spinning, thermal drawing, pre-oxidation, carbonization and graphitization in sequence to obtain fullerene-doped carbon nanofibers with high regularity; the carbonaceous element additive is fullerene vinyl material.

The present invention adopts fullerene material as carbonaceous element additive, and can mix fullerene and polyacrylonitrile to obtain nano-composite at molecular scale, and the interaction between polyacrylonitrile and fullerene limits the difference between fullerenes. The agglomeration reduces defects in the fibers. The doped fullerene material can promote the graphitization process of the fiber through its interaction with the polyacrylonitrile matrix, improving the strength and toughness of the fiber.

The water-phase precipitation polymerization described in the present invention refers to a polymerization method in which the polymerization monomer (acrylonitrile) and the initiator are soluble in water, but the polymer (polyacrylonitrile) produced by the polymerization is insoluble in water, resulting in a precipitation.

In 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 precipitation polymerization is a mixture of persulfate and ammonium sulfite. Through the addition of ammonium sulfite, the activation energy of the reaction is reduced, the initiation effect of the initiation system can be better, and the dispersion effect of polyacrylonitrile and fullerene materials can be increased at the same time.

The working principle of the initiator is that after heating, it decomposes to generate free radicals, which can cause the olefinic compounds to continue to generate free radicals, thereby forming free radical polymerization. The initiator of water-phase precipitation polymerization generally contains persulfate, and the optimum initiation temperature of persulfate is about 80 °C. At the same time, the addition of ammonium sulfite reduces the reaction activation energy, so the reaction temperature can be reduced, so in one or more In the embodiment, the temperature of the water-phase precipitation polymerization is 40-80°C. The reaction time is 60～180min. The molecular weight is between 10,000 and 1,000,000.

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

In some embodiments, the spinning is electrospinning. In one or more embodiments, the precursor raw material is dissolved in an organic solvent to prepare a spinning dope, and the spinning dope is used for electrospinning. The solvent used may be dimethylsulfoxide, dimethylformamide, dimethylacetamide, and the like. The concentration of the precursor raw material in the spinning dope is 5-50 wt%. The specific process of electrospinning is as follows: pour the spinning stock solution into the needle tube of electrospinning, the needle tube is equipped with a needle with a diameter of 0.1-1mm, the electric field strength of 30-300KV after assembly and the liquid supply of 0.1-10ml/h Spinning is carried out at high speed. The electric field strength and liquid supply speed are different according to the molecular weight of the polymer and the concentration, viscosity and conductivity of the spinning solution. The prepared nanofibers are evenly distributed on the take-up roller under the action of the sliding table. , the speed of the wire collecting roller is between 100 and 1000 rpm.

The hot-drawing refers to the nanofiber mat spun after spinning. Under the action of the take-up roller, the fibers are initially oriented to a certain extent, and the fibers are trimmed into strips along the orientation direction, and the two ends are applied under heating conditions. The fibers are drawn. In some embodiments, the temperature of the hot drawing is 100-150° C., and the drawing ratio is 1.5-4.

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

The carbonization refers to a heat treatment process of pyrolysis under the protection of an inert gas or a vacuum state. In some embodiments, the carbonization temperature is 1000-1600° C., and the carbonization time is 5-20 min.

The graphitization refers to the process of performing graphitization by heating under the protection of an inert gas or in a vacuum state. In some embodiments, the graphitization temperature is 2000˜3500° C., and the graphitization time is 30˜150 s.

The third embodiment of the present invention provides a fullerene-doped carbon nanofiber with high regularity obtained by the above preparation method.

The fourth embodiment of the present invention provides a kind of above-mentioned fullerene-doped carbon nanofibers with high regularity as hydrogen storage materials, high-capacity electrode materials, high-performance composite materials and/or fuel cell electrode materials. application.

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

Example 1

Add 10ml of acrylonitrile and 0.08g of fullerene to 60ml of water and mix well, add dropwise 10ml of an aqueous solution containing 0.3g of ammonium sulfite and 0.3g of ammonium persulfate to initiate polymerization, heat to 60°C, and polymerize for 120min. Precipitate, wash, and dry to obtain polyacrylonitrile/fullerene composite powder.

Add 2g of the above polyacrylonitrile/fullerene composite powder to 10ml of dimethyl sulfoxide, heat to 60°C, stir evenly to obtain a spinning dope, pour the spinning dope into a needle tube with a volume of 20ml, and assemble the needle tube There is an electrospinning needle with an inner diameter of 0.5mm for electrospinning. The process parameters of electrospinning are: the temperature is 40°C, the liquid supply speed is 3ml/h, the electric field strength is 100kV/m, and the moving speed of the slide table is 10 mm/s, the speed of the yarn take-up roller is 500 rpm, and the nanofiber mat (ie, the raw silk) is obtained after the solution is consumed, that is, after the electrospinning is completed.

The above-mentioned nanofiber mat was cut into strips with a length of 5 cm and a width of 2 cm according to the orientation obtained by the take-up roll, and the strip was stretched to 15 cm under the condition of 135 ° C (one end of the strip was fixed with a clip, and the other end was applied with a weight. drawing) to obtain nanofiber ribbons.

The thermally drawn nanofiber ribbons were pre-oxidized at 280 °C for 2 h, carbonized at 1500 °C for 5 min, and graphitized at 3000 °C for 50 s to obtain the final carbon nanofibers.

Example 2

Add 10ml of acrylonitrile and 0.4g of multi-wall fullerene (i.e. carbon nano-onion) to 60ml of water and mix well, add dropwise 10ml of an aqueous solution containing 0.3g of ammonium sulfite and 0.3g of ammonium persulfate to initiate polymerization, and heat to 65 ℃, polymerize for 150min, wash and dry the resulting precipitate to obtain polyacrylonitrile/multiwall fullerene composite powder, as shown in Figure 1.

Add 1.5g of the above polyacrylonitrile/multi-wall fullerene composite powder to 10ml of dimethylformamide, heat to 60°C, stir evenly to obtain a spinning dope, and pour the spinning dope into a 20ml needle tube , the needle tube is equipped with an electrospinning needle with an inner diameter of 0.5mm, and electrospinning is performed. The process parameters of electrospinning are: the temperature is 40 °C, the liquid supply speed is 2ml/h, the electric field intensity is 80kV/m, and the sliding table The moving speed was 15 mm/s, and the rotation speed of the take-up roller was 1000 rpm. After the solution was consumed, that is, after the electrospinning was completed, the nanofiber mat (ie, the raw silk, as shown in Figure 2) was obtained.

The above-mentioned nanofiber mat was cut into strips with a length of 5 cm and a width of 2 cm according to the orientation obtained by the take-up roll, and the strip was stretched to 15 cm under the condition of 135 ° C (one end of the strip was fixed with a clip, and the other end was applied with a weight. drawing) to obtain nanofiber ribbons.

The thermally drawn nanofiber ribbons were pre-oxidized at 300 °C for 1.5 h, carbonized at 1500 °C for 10 min, and graphitized at 2800 °C for 50 s to obtain the final carbon nanofibers, as shown in Figure 3.

The thermogravimetric analysis of the precursor fiber is shown in Figure 4. It can be seen that the residual weight of the precursor fiber prepared from pure polyacrylonitrile after heating to 950 °C is 27.6%, while the weight of the participating fiber increases to 37.8% after adding 5wt% of multi-wall fullerene. %, it can be proved that the heat resistance of the fiber matrix is improved by the multi-wall fullerene, which can be attributed to the free radicals generated by the adsorption and pyrolysis of the multi-wall fullerene, which can prevent the further deterioration of its structure.

The fracture stress of carbon nanofibers, as shown in Figure 5, shows that the fracture stress of the carbon nanofibers finally prepared after adding 5wt% of multi-wall fullerene is increased from 17.4MPa to 25MPa compared with the control group without multi-wall fullerene. . The reasons for the increase of fiber breaking stress are: a. Multi-walled fullerenes can hinder the expansion of cracks and promote crack branching when the fibers are drawn, so that the energy required for fracture increases; b. Multi-walled fullerenes can induce fibers The matrix forms a more perfect graphite lattice structure during the heat treatment, and the improvement of the structure enables the fiber matrix to withstand stronger drafting; c. Fullerenes can absorb the free electrons generated by the breakage of the molecular chain to prevent further deterioration of the structure.

The elongation at break of carbon nanofibers is shown in Figure 6. It can be seen that the elongation at break of the carbon nanofibers finally prepared after adding 5 wt% of multi-wall fullerene is higher than that of the control group without adding multi-wall fullerene from 1.35 % increased to 3.27%. The reason for the increase of fiber elongation at break is that multi-wall fullerenes can move with the matrix when the fiber matrix is stretched and deformed, and continuously generate secondary bonds, which have a continuous strengthening effect on the fiber matrix.

Example 3

Add 10ml of acrylonitrile and 0.8g of carboxylated fullerene (1g of fullerene in 30ml of concentrated sulfuric acid + 10ml of concentrated nitric acid and sonicated for 3 hours at 40°C) into 100ml of water and mix well, add 10ml dropwise to dissolve 0.4g of An aqueous solution of ammonium sulfate and 0.4 g of ammonium persulfate was used to initiate polymerization, heated to 70° C., and polymerized for 120 min. The resulting precipitate was washed and dried to obtain polyacrylonitrile/carboxylated fullerene composite powder.

Add 1 g of the above polyacrylonitrile/carboxylated fullerene composite material powder to 10 ml of dimethylacetamide, heat it to 70 ° C, stir evenly to obtain a spinning dope, and pour the spinning dope into a 20ml needle tube, The needle tube is equipped with an electrospinning needle with an inner diameter of 0.5mm for electrospinning. The process parameters of electrospinning are: the temperature is 45°C, the liquid supply speed is 2ml/h, the electric field strength is 120kV/m, and the movement of the slide table The speed is 10 mm/s, and the rotation speed of the take-up roller is 100 rpm. After the solution is consumed, that is, the electrospinning is completed, the nanofiber mat (ie, the raw silk) is obtained.

The above-mentioned nanofiber mat was cut into strips with a length of 5 cm and a width of 2 cm according to the orientation obtained by the take-up roll, and the strip was stretched to 15 cm under the condition of 135 ° C (one end of the strip was fixed with a clip, and the other end was applied with a weight. drawing) to obtain nanofiber ribbons.

The thermally drawn nanofiber ribbons were pre-oxidized at 300 °C for 1 h, carbonized at 1300 °C for 5 min, and graphitized at 2800 °C for 50 s to obtain the final carbon nanofibers.

The above descriptions are only preferred embodiments of the present invention, and are not intended to limit the present invention. For those skilled in the art, the present invention may have various modifications and changes. Any modification, equivalent replacement, improvement, etc. made within the spirit and principle of the present invention shall be included within the protection scope of the present invention.

Claims (10)

1. Application of a fullerene material as a carbonaceous element additive in the preparation of carbon nanofibers. 2. A preparation method of a carbon nanofiber with high regularity doped with fullerene, acrylonitrile and a carbonaceous element additive are formed by water-phase precipitation polymerization to form a composite precursor material of the carbonaceous element additive and polyacrylonitrile, and the former The bulk raw materials are sequentially spun, thermally drawn, pre-oxidized, carbonized, and graphitized to obtain fullerene-doped carbon nanofibers with high regularity; it is characterized in that the carbonaceous element additive is a fullerene material. 3. the preparation method of the carbon nanofiber of fullerene doping high regularity as claimed in claim 2, is characterized in that, the initiator in the water-phase precipitation polymerization is the mixture of persulfate and ammonium sulfite; Preferably, the temperature of the water-phase precipitation polymerization is 40-80°C. 4. The preparation method of fullerene-doped high-regularity carbon nanofibers as claimed in claim 2, wherein the spinning is electrospinning; preferably, the precursor raw material is dissolved in an organic solvent The spinning stock solution is prepared, and the spinning stock solution is used for electrospinning. 5 . The method for preparing fullerene-doped carbon nanofibers with high regularity according to claim 2 , wherein the temperature of thermal drawing is 100-150° C., and the drawing ratio is 1.5-4. 6 . 6 . The method for preparing fullerene-doped carbon nanofibers with high regularity according to claim 2 , wherein the pre-oxidation temperature is 150-300° C., and the pre-oxidation time is 30-120 min. 7 . 7 . The method for preparing fullerene-doped carbon nanofibers with high regularity according to claim 2 , wherein the carbonization temperature is 1000-1600° C., and the carbonization time is 5-20 min. 8 . 8 . The method for preparing fullerene-doped high-regularity carbon nanofibers according to claim 2 , wherein the graphitization temperature is 2000-3500° C., and the graphitization time is 30-150 s. 9 . 9 . A fullerene-doped carbon nanofiber with high regularity, characterized in that it is obtained by the preparation method according to any one of claims 2 to 8 . 10. An application of the fullerene-doped high-regularity carbon nanofiber of claim 9 as a hydrogen storage material, a high-capacity electrode material, a high-performance composite material and/or a fuel cell electrode material.

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