CN115282989A - Preparation method of iodine-doped carbon nano tube for ultrasonic-microwave water environment reconstruction and iodine-doped carbon nano tube - Google Patents
Preparation method of iodine-doped carbon nano tube for ultrasonic-microwave water environment reconstruction and iodine-doped carbon nano tube Download PDFInfo
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/06—Halogens; Compounds thereof
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/34—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation
- B01J37/341—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation
- B01J37/343—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of ultrasonic wave energy
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/34—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation
- B01J37/341—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation
- B01J37/344—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of electromagnetic wave energy
- B01J37/345—Irradiation by, or application of, electric, magnetic or wave energy, e.g. ultrasonic waves ; Ionic sputtering; Flame or plasma spraying; Particle radiation making use of electric or magnetic fields, wave energy or particle radiation of electromagnetic wave energy of ultraviolet wave energy
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
Abstract
The application provides a preparation method of iodine-doped carbon nanotubes by ultrasonic-microwave water environment reconstruction, which adopts the following steps: dispersing a carbon nano tube and excessive iodine simple substances in an aqueous solution, performing ultrasonic dispersion to prepare a simple substance mixture A, placing the mixture A in a microwave closed environment for primary microwave treatment, decomposing the iodine simple substances and the carbon nano tube after microwave impact to reconstruct into uniformly dispersed nano particles to obtain an iodine-doped carbon nano tube B; and placing the iodine-doped carbon nano tube B in a microwave environment for secondary microwave treatment, and removing unreacted iodine simple substance to obtain the pure iodine-doped carbon nano tube. The application creatively applies the microwave method to the preparation of the iodine-doped carbon nano tube directly formed by the nonmetal simple substance, and the microwave method is applied to the iodine-doped carbon nano tube, so that the problem that the nonmetal simple substance blocks the aperture of the carbon nano tube can be effectively reduced; the preparation method is simple and quick, has simple requirements on equipment, easily obtained raw materials, low cost and low energy consumption, and is suitable for large-scale production.
Description
Technical Field
The application belongs to the technical field of catalyst material preparation, and particularly relates to a preparation method of an iodine-doped carbon nanotube for ultrasonic-microwave water environment reconstruction and the iodine-doped carbon nanotube.
Background
Heteroatom doped carbon materials have become one of the hot spots of research in recent years due to the advantages of low raw material price, abundant earth resources, high ORR catalytic activity, good chemical stability, environmental friendliness and the like. For carbon materials doped with no metal heteroatom, the heteroatom can induce charge density and spin density redistribution on adjacent carbon atoms, facilitating adsorption of O 2 Enhancing ORR catalytic activity.
Carbon nanotubes are typically one-dimensional sp 2 The hybrid carbon nanomaterial has unique structural characteristics and excellent physical and chemical properties, such as large specific surface area, good conductivity, good chemical stability, high mechanical properties and the like. These properties make carbon nanotubes an ideal carbon-based support for ORR catalytically active materials. When the heteroatom is properly added to the carbon nanotube, a desired ORR property can be obtained. The carbon nano tube can enhance the oxygen mass transfer, water removal, corrosion resistance and electrical conductivity of the catalyst, thereby obviously improving the catalytic activity and durability of the catalyst. Halogen element iodine has higher electronegativity than non-metal heteroatoms such as nitrogen atoms, and can polarize adjacent C atoms in a carbon frame, and change an electronic structure, thereby promoting a catalytic process. And iodine can also be generated by I - The formation of ionic bonds further enhances charge transfer.
The conventional heteroatom doped carbon material mainly comprises a tubular furnace heat treatment method and a solvothermal method, and has the problems that a sample cannot be fully contacted with dopants due to uneven heating in a tubular furnace, the hydrothermal operation is complex, and the yield is low. The reaction time of the two is long, the conditions are harsh, the large-scale production is difficult, and the cost is high.
In view of this, the present application is specifically made.
Disclosure of Invention
In order to solve one of the technical defects, the embodiment of the application provides a preparation method of an iodine-doped carbon nanotube for ultrasonic-microwave water environment reconstruction and the iodine-doped carbon nanotube.
According to a first aspect of the embodiments of the present application, there is provided a method for preparing an iodine-doped carbon nanotube by ultrasonic-microwave water environment reconstruction, including:
dispersing a carbon nano tube and excessive iodine simple substance in an aqueous solution, performing ultrasonic dispersion to prepare a simple substance mixture A, placing the mixture A in a microwave closed environment for primary microwave treatment, decomposing the iodine simple substance and the carbon nano tube after being impacted by microwave and reconstructing the iodine simple substance and the carbon nano tube into uniformly dispersed nano particles to obtain an iodine-doped carbon nano tube B; and placing the iodine-doped carbon nano tube B in a microwave environment for secondary microwave treatment, and removing unreacted iodine simple substance to obtain the pure iodine-doped carbon nano tube.
Preferably, the mass ratio of the iodine to the carbon nano tubes is 0.2-7:1.
Preferably, the microwave power in one microwave treatment is 400-800W, and the microwave treatment time is 1-5min.
Preferably, the secondary microwave treatment is carried out by uncovering the cover under the condition of 50-150W of microwave for 1-4min so as to remove unreacted iodine simple substance.
Preferably, the carbon nano tube and the iodine simple substance are mixed and dispersed in the water solution, ultrasonic dispersion is carried out for 20-60min, and the mass ratio of the carbon nano tube to water is 1:50-200, wherein the water has a mass of less than 4g.
Preferably, the method comprises the following specific steps:
s1: dispersing 20mg of carbon nanotubes and 60mg of iodine elementary substance in an aqueous solution, and performing ultrasonic dispersion to obtain an elementary substance mixture A;
s2: transferring the monomer mixture A into a quartz crucible with a cover, and putting the quartz crucible into a microwave oven;
s3: adjusting the power to 800W, and performing microwave treatment for 3min; obtaining iodine-doped carbon nano tube B;
s4: taking out the reaction product 2min after the reaction is finished, and naturally cooling the reaction product at room temperature;
s5: and (3) opening the cover under the microwave of 160W for 2min to remove unreacted iodine simple substances to obtain the iodine-doped carbon nano tube.
According to a second aspect of the embodiments of the present application, there is provided an iodine-doped carbon nanotube, which is prepared by the above method;
preferably, the carbon iodine in the iodine-doped carbon nanotube is in a mixed bonding configuration and has both covalent bonds and ionic bonds.
The beneficial effect of this application:
1. according to the method, the carbon nano tube and the iodine simple substance are firstly dispersed in the water solution and subjected to ultrasonic treatment, so that the carbon nano tube and the iodine simple substance are dispersed in the water solution, the iodine simple substance molecules can be uniformly distributed on the surface of the carbon nano tube through ultrasonic dispersion, the water molecules can enhance the thermal motion of the iodine simple substance molecules in the microwave treatment, the doping efficiency is improved, then the carbon nano tube and the iodine simple substance absorb microwaves through a microwave thermal impact method, the instantaneous temperature can be increased to 1600K within 100ms, then the carbon nano tube and the iodine simple substance are naturally cooled at room temperature, and redundant iodine simple substance is removed through secondary low-power microwaves. In the extreme temperature change, the iodine simple substance is decomposed and reconstructed into iodine molecules with small particle size and uniform distribution, C-C bonds on the carbon nano tubes are broken due to microwave impact and molecular thermal motion, the carbon nano tubes are broken under the sequential microwave impact to generate positive and negative ions, and the negative ions reduce part of the iodine simple substance into I - Neutral iodine and I - Are combined to form
And combines with the positive C ion to form an ionic bond; covalent bonds exist between the carbon nanotubes and part of iodine atoms, and the part of iodine atoms replace carbon atoms in the carbon layer structure of the carbon nanotubes to form covalent bonds with carbon atoms around the carbon layer.
2. Compared with the traditional microwave method which is mainly used for thermal decomposition of precursor materials and accelerating reduction of metal precursors and nucleation of metals, the method has the advantages that the microwave method is innovatively applied to the preparation process of the iodine-doped carbon nano tube directly formed by nonmetal simple substances, the microwave method is applied to the iodine-doped carbon nano tube, and the problem that the nonmetal simple substances block the aperture of the carbon nano tube can be effectively reduced; the preparation method is simple and quick, has simple requirements on equipment, easily obtained raw materials, low cost and low energy consumption, and is suitable for large-scale production.
Drawings
The accompanying drawings, which are included to provide a further understanding of the application and are incorporated in and constitute a part of this application, illustrate embodiment(s) of the application and together with the description serve to explain the application and not to limit the application. In the drawings:
FIG. 1 is a high resolution XPS spectrum of I3 d for iodine doped carbon nanotubes prepared in example 1 of the present application;
FIG. 2 is a high resolution XPS spectrum of C1s of iodine doped carbon nanotubes prepared in example 1 of the present application;
FIG. 3 is an XPS spectrum of iodine doped carbon nanotubes prepared in example 1 of the present application;
FIG. 4 shows the saturation of O for untreated CNTs and I-CNTs in example 1 of the present application 2 The lower CV curve;
FIG. 5 LSV curves of I-CNTs prepared in example 1 of the present application at different rotation speeds;
FIG. 6 is a graph of LSV at various rotational speeds for untreated CNTs;
FIG. 7 is an lsv plot of the I-CNTs prepared in example 1 of the present application at 1600 rpm.
Detailed Description
In order to make the technical solutions and advantages of the embodiments of the present application more apparent, the following further detailed description of the exemplary embodiments of the present application with reference to the accompanying drawings makes it clear that the described embodiments are only a part of the embodiments of the present application, and are not exhaustive of all embodiments. It should be noted that the embodiments and features of the embodiments in the present application may be combined with each other without conflict.
Example one
A preparation method of iodine-doped carbon nanotubes for ultrasonic-microwave water environment reconstruction comprises the following specific steps:
s1: dispersing 20mg of carbon nanotubes and 60mg of iodine elementary substance in an aqueous solution, and performing ultrasonic dispersion for 30min to obtain an elementary substance mixture A;
s2: transferring the monomer mixture A into a quartz crucible with a cover, and putting the quartz crucible into a microwave oven;
s3: adjusting the power to 800W, and performing microwave treatment for 3min; obtaining iodine doped carbon nano tube B;
s4: taking out the reaction product 2min after the reaction is finished, and naturally cooling the reaction product at room temperature;
s5: and (3) opening the cover under the microwave of 160W for 2min to remove unreacted iodine simple substances to obtain the iodine-doped carbon nano tube.
Example two
A preparation method of iodine-doped carbon nanotubes for ultrasonic-microwave water environment reconstruction comprises the following specific steps:
s1: dispersing 20mg of carbon nano tubes and 60mg of iodine elementary substance in an aqueous solution, and performing ultrasonic dispersion for 30min to obtain an elementary substance mixture A;
as a specific implementation manner, 20mg of the carbon nanotubes and 60mg of the iodine simple substance can also be separately ultrasonically dispersed in the aqueous solution, and then the mixture a obtained by the secondary ultrasonic dispersion can be separately ultrasonically dispersed, so that the degree of dispersion of the carbon nanotubes and the iodine simple substance can be increased, and the subsequent iodine doping is facilitated.
S2: transferring the monomer mixture A into a quartz crucible with a cover, and putting the quartz crucible into a microwave oven;
s3: adjusting the power to 600W, and performing microwave treatment for 3min; obtaining iodine doped carbon nano tube B;
s4: taking out the reaction product 2min after the reaction is finished, and naturally cooling the reaction product at room temperature;
s5: and (3) opening the cover under the microwave of 160W for 2min to remove unreacted iodine simple substances to obtain the iodine-doped carbon nano tube.
Comparative example 1
CNTS that are not treated.
FIG. 1 is a high resolution XPS spectrum of I3 d for iodine doped carbon nanotubes prepared in example 1 of the present application;
FIG. 2 is a high resolution XPS spectrum of C1s of iodine doped carbon nanotubes prepared in example 1 of the present application; FIG. 3 is an XPS spectrum of iodine doped carbon nanotubes prepared in example 1 of the present application; FIG. 4 shows the saturation of O for untreated CNTs and I-CNTs in example 1 of the present application 2 The lower CV curve; FIG. 5 LSV curves of I-CNTs prepared in example 1 of the present application at different rotation speeds; FIG. 6 is a graph of LSV at various rotational speeds for untreated CNTs; FIG. 7 is an lsv plot of the I-CNTs prepared in example 1 of the present application at 1600 rpm.
From fig. 1 to 3, it can be seen that iodine has been doped on the carbon nanotube, and the C-I bond, including ionic bond and covalent bond, existing between the carbon nanotube and iodine can be known through high resolution XPS spectra of C1s and I3 d.
As can be seen from FIG. 4, I-CNTs and CNTs have a reduction peak at 0.29V, indicating that they undergo oxygen reduction reaction. And the reduction peak area of the I-CNTs is obviously larger than the reduction peak of the CNTs, which shows that the oxygen reduction reaction activity is enhanced by doping iodine. FIGS. 5 and 6 depict the LSV curves of CNTs and I-CNTs, respectively, at different rotational speeds, with the limiting current density increasing with increasing rotational speed due to the shortening of the diffusion layer at high speeds. FIG. 7 depicts the lsv curves of CNTs and I-CNTs at 1600rpm, from which it can be seen that the limiting current density of I-CNTs is significantly greater than CNTs, indicating that the greater the current that can be passed per unit area of I-CNTs per unit time, the more rapid the reaction kinetics. As a fuel cell cathode catalyst, it is possible to make the fuel cell have a larger power.
Based on the above, the conventional carbon nanotube heteroatom doping is mostly doping on in-situ grown carbon nanotubes, and the post-treatment carbon nanotube doping has fewer reports and is mostly doping of nitrogen, boron, phosphorus and sulfur. The microwave method is mostly used for thermal decomposition of precursor materials, and the reduction of metal precursors and the nucleation of metals are accelerated; according to the method, the carbon nano tube and the iodine elementary substance are adopted to absorb microwaves by a microwave thermal impact method, the instantaneous temperature can be increased to 1600K within 100ms, then the temperature is naturally cooled at room temperature, and redundant iodine elementary substance is removed by secondary low-power microwaves. In the extreme temperature change, the iodine simple substance is decomposed and reconstructed into iodine molecules with small particle size and uniform distribution, C-C bonds on the carbon nano tubes are broken due to microwave impact and molecular thermal motion, the carbon nano tubes are broken under the sequential microwave impact to generate positive and negative ions, and the negative ions reduce part of the iodine simple substance into I - Neutral iodine and I - Are combined into
And combined with the positive C ion to form an ionic bond. From the high resolution XPS spectrum of I3 d, it can be known that covalent bonds exist between the carbon nanotubes and part of the iodine atoms, and the part of the iodine atoms replace carbon atoms in the carbon layer structure of the carbon nanotubes to form covalent bonds with carbon atoms around the carbon layer.
Ultrasonic dispersion can enable water molecules to drive iodine elementary substance molecules to be uniformly distributed on the surface of the carbon nano tube, efficient doping of iodine during microwave is facilitated, and water molecules in microwave treatment can enhance thermal motion of the iodine elementary substance molecules, so that doping efficiency is improved.
Compared with the traditional microwave method which is mainly used for thermal decomposition of precursor materials and accelerating reduction of metal precursors and nucleation of metals, the microwave method is innovatively applied to the preparation process of the iodine-doped carbon nano tube directly formed by the nonmetal simple substances, and the problem that the nonmetal simple substances block the aperture of the carbon nano tube can be effectively reduced by applying the microwave method to the iodine-doped carbon nano tube; the preparation method is simple and quick, has simple requirements on equipment, easily obtained raw materials, low cost and low energy consumption, and is suitable for large-scale production.
It is worth to say that the carbon nano tube/metal sulfide material can be prepared by adopting sulfur powder to replace selenium powder in an ion exchange stage. The carbon nanotubes may be replaced with other materials such as graphene.
While the preferred embodiments of the present application have been described, additional variations and modifications in those embodiments may occur to those skilled in the art once they learn of the basic inventive concepts. Therefore, it is intended that the appended claims be interpreted as including preferred embodiments and all alterations and modifications as fall within the scope of the application.
It will be apparent to those skilled in the art that various changes and modifications may be made in the present application without departing from the spirit and scope of the application. Thus, if such modifications and variations of the present application fall within the scope of the claims of the present application and their equivalents, the present application is intended to include such modifications and variations as well.
Claims (8)
1. A preparation method of iodine-doped carbon nanotubes for ultrasonic-microwave water environment reconstruction is characterized by comprising the following steps:
dispersing a carbon nano tube and excessive iodine simple substance in an aqueous solution, performing ultrasonic dispersion to prepare a simple substance mixture A, placing the mixture A in a microwave closed environment for primary microwave treatment, decomposing the iodine simple substance and the carbon nano tube after being impacted by microwave and reconstructing the iodine simple substance and the carbon nano tube into uniformly dispersed nano particles to obtain an iodine-doped carbon nano tube B; and placing the iodine-doped carbon nano tube B in a microwave environment for secondary microwave treatment, and removing unreacted iodine simple substance to obtain the pure iodine-doped carbon nano tube.
2. The method for preparing iodine-doped carbon nanotubes through ultrasonic-microwave water environment reconstruction as claimed in claim 1, wherein the mass ratio of iodine simple substance to carbon nanotubes is 0.2-7:1.
3. The method for preparing the iodine-doped carbon nanotube for the water environment reconstruction of the ultrasonic-microwave as claimed in claim 1, wherein the carbon nanotube and the iodine simple substance are mixed and dispersed in the aqueous solution, the ultrasonic dispersion is carried out for 20-60min, and the mass ratio of the carbon nanotube to the water is 1:50-200, wherein the water has a mass of less than 4g.
4. The method of claim 1, wherein the microwave power in one microwave treatment is 400-800W and the microwave treatment time is 1-5min.
5. The preparation method of the iodine-doped carbon nanotube for the water environment reconstruction of the ultrasonic-microwave environment as claimed in claim 1, wherein the secondary microwave treatment is carried out by uncovering the cover under the microwave of 50-150W for 1-4min to remove unreacted iodine simple substance.
6. The preparation method of the iodine-doped carbon nanotube for the ultrasonic-microwave water environment reconstruction as claimed in claim 1, which is characterized by comprising the following specific steps:
s1: mixing and dispersing 20mg of carbon nano tubes and 60mg of iodine simple substances in an aqueous solution, and performing ultrasonic dispersion for 20-60min to obtain a simple substance mixture A of iodine and the carbon nano tubes;
s2: transferring the simple substance mixture A of iodine and the carbon nano tube prepared in the step S1 into a 30mL quartz crucible with a cover, and putting the quartz crucible into a microwave oven;
s3: adjusting the power to 800W, and performing microwave treatment for 3min; obtaining iodine-doped carbon nano tube B;
s4: taking out the reaction product 2min after the reaction is finished, and naturally cooling the reaction product at room temperature;
s5: and (3) opening the cover under the microwave of 160W for 2min to remove unreacted iodine simple substances to obtain the iodine-doped carbon nano tube.
7. Iodine-doped carbon nanotubes produced by the method according to any one of claims 1 to 6.
8. The iodine-doped carbon nanotube of claim 7 wherein the carbon iodine in the iodine-doped carbon nanotube is in a mixed bonding configuration having both covalent and ionic bonds.
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| US20130157838A1 (en) * | 2008-06-18 | 2013-06-20 | Board Of Trustees Of The University Of Arkansas | Doped-carbon composites, synthesizing methods and applications of the same |
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| CN107892301A (en) * | 2017-10-26 | 2018-04-10 | 兰州理工大学 | A kind of phosphorus doping meso-porous carbon material and its microwave preparation and application |
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