CN114590800A - Method for continuously preparing graphene by magnetically-driven sliding arc plasma high-voltage discharge - Google Patents
Method for continuously preparing graphene by magnetically-driven sliding arc plasma high-voltage discharge Download PDFInfo
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- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 46
- 238000000034 method Methods 0.000 title claims abstract description 38
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims abstract description 34
- 239000011280 coal tar Substances 0.000 claims abstract description 34
- 238000007233 catalytic pyrolysis Methods 0.000 claims abstract description 25
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 21
- 239000002243 precursor Substances 0.000 claims abstract description 21
- 239000001257 hydrogen Substances 0.000 claims abstract description 20
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- 229910052759 nickel Inorganic materials 0.000 claims description 2
- GNRSAWUEBMWBQH-UHFFFAOYSA-N nickel(II) oxide Inorganic materials [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 claims description 2
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/15—Nano-sized carbon materials
- C01B32/182—Graphene
- C01B32/184—Preparation
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/10—Process efficiency
Abstract
The invention discloses a method for continuously preparing graphene by magnetic drive sliding arc plasma high-voltage discharge, which comprises the steps of gasifying coal tar, sending the gasified coal tar into a catalytic pyrolysis furnace filled with argon, adding nano metal or metal oxide serving as a catalyst into the pyrolysis furnace, mixing and reacting gaseous coal tar and the catalyst to generate a carbonized precursor, introducing the carbonized catalytic precursor and hydrogen into a magnetic drive sliding arc plasma discharge device together, generating high-density non-thermal sliding arc plasma through an auxiliary magnetic field, and converting the carbonized precursor into graphene under the action of the high-density non-thermal sliding arc plasma; the method has low cost and simple equipment, does not need condensation, and can realize the conversion of the coal tar to the high value-added product graphene.
Description
Technical Field
The invention belongs to the technical field of graphene preparation, and particularly relates to a method for continuously preparing graphene through magnetic drive sliding arc plasma high-voltage discharge.
Background
The coal tar is mainly obtained through a coal pyrolysis and carbonization process, is a byproduct in the coking process, and the yield of the coal tar accounts for 3% -5% of that of coal in the furnace. The tar has complex chemical structure, poor stability, low heat value and toxicity, and can block pipelines and equipment. The fraction is heavy and poor in quality, particularly the quality and the content of metal and asphalt are high, and the comprehensive chemical analysis and utilization of the coal tar are a difficult task. The coal tar contains a large amount of polycyclic aromatic hydrocarbon hydrocarbons, so that the coal tar can be used as a carbon source to prepare graphene. The production method of the graphene is more, and a mechanical stripping method is adopted as a common method, so that the cost is low, the operation is easy, the yield and the purity are low, and the product structure is inconsistent; the graphene prepared by the cutting carbon nanotube method has high elasticity and high tensile strength, but is difficult to be melted and easy to aggregate in a solvent; the arc discharge method has the advantages of easy production, no need of substrate transfer, high repeatability and high reaction energy consumption; the chemical vapor deposition method has low cost and high yield, is beneficial to industrial production, is difficult to position a proper substrate, and has easily damaged graphene molecular structure; the reduction graphite oxidation method is simple to operate and high in yield, but the product has certain defects; the graphene prepared by the catalytic pyrolysis method has large area and good uniformity, but the preparation process is not mature and has strict requirements on equipment. Generally, although the physical method for preparing graphene is low in synthesis cost and simple in technology, the prepared graphene is low in purity, inconsistent in structure and low in controllability. Chemical methods tend to limit the commercial production of graphene due to the expense of carbon precursors, difficulty in locating appropriate substrates, product structural defects, and the like.
The arc plasma discharge does not need a catalyst, the process is simple, no pollution is caused, but a carbon source is easy to crack at high temperature to generate a target substance and simultaneously generate a large amount of byproducts, and the arc discharge method has high energy consumption and expensive environmental conditions. The sliding arc plasma is a non-thermal plasma which has little erosion to the electrode and does not need to cool the electrode. Nanostructured carbon Materials are synthesized using methane/helium gliding arc plasma under Hypergravity conditions at the university of Massach (Hypergravity synthesis of graphical carbon in glass plasma [ J ]. Materials Research Bulletin, 2014, 54: 61-65.). The sliding motion of the arc discharge is more prominent along the sliding of the electrode under the action of gravity, but the double-blade type electrode reactor is used in the low-temperature plasma generator in the research process, so that the problems of poor arc stability, small reaction contact area and the like exist, and the industrialization is difficult to realize. The Hongkong universities topic group of Fuzhou university (correlation and formation mechanism of raw-layer graphene by crystallization arc plasma [ J ]. Chemical Engineering Journal, 2020, 387:124102.) reported that sliding arc plasma pyrolysis using methane as a carbon source produced few layers of graphene powder, but the sliding arc plasma was a non-thermal plasma, and the volume was small, the energy density was low, and the reaction efficiency was low due to low system flux.
Disclosure of Invention
In order to solve the problems, the invention provides a method for continuously preparing graphene by magnetic drive sliding arc plasma high-voltage discharge, which comprises the steps of gasifying coal tar, feeding the gasified coal tar into a catalytic pyrolysis furnace filled with argon or helium, adding nano metal or metal oxide serving as a catalyst into the pyrolysis furnace, mixing and reacting gaseous coal tar and the catalyst to generate a carbonized precursor, introducing the carbonized precursor and hydrogen into a magnetic drive sliding arc plasma discharge device, generating high-density non-thermal sliding arc plasma by an auxiliary magnetic field, and converting the carbonized precursor into graphene under the action of the high-density non-thermal sliding arc plasma.
The method comprises the following steps of carrying out primary pyrolysis on gaseous coal tar under the condition of argon or helium, reacting hydrocarbons in the gaseous coal tar with a catalyst, combining carbon bonds with the catalyst to generate a carbonized precursor during dehydrogenation, carrying out pyrolysis cracking on the carbonized precursor in a magnetic drive sliding arc plasma discharge device, combining carbon atoms at high temperature to generate carbon clusters and carbon chains, and continuously extending to generate large-area graphene; the method comprises the steps of terminating a dangling carbon bond by using hydrogen, preventing graphene from forming a closed structure, depositing a graphene product at the bottom of a magnetic drive sliding arc plasma discharge device, enabling gas and graphene to enter a cyclone separation device under the action of an induced draft fan, collecting the graphene product at the bottom of the cyclone separation device, and collecting the gas into a gas collection tank.
The catalyst is nano-particles of Ni, Cu, Pt, Pd, Al, NiO and Al2O3One or more of (a).
The temperature in the catalytic pyrolysis furnace is 650-850 ℃.
The argon gas accounts for 90-97% of the volume of the mixed gas of the argon gas and the hydrogen gas, and the helium gas accounts for 90-97% of the volume of the mixed gas of the helium gas and the hydrogen gas.
The magnetic drive sliding arc plasma discharge device comprises a shell, a cathode, an anode, a magnetic field generator, a stainless steel screen, a direct current high-frequency high-voltage power supply and a pressure gauge, wherein the cathode is arranged in the shell and positioned at the center of the shell, the anode is positioned on two sides of the cathode, the magnetic field generator is arranged outside the shell and generates a magnetic field to cover a reaction area, the stainless steel screen is arranged in the shell and positioned below the cathode, the direct current high-frequency high-voltage power supply is respectively connected with the anode and the cathode, and the pressure gauge is arranged on the shell.
The invention also aims to provide a device for completing the method, which comprises an inert gas tank, more than one gasification tank, more than one catalytic pyrolysis furnace, a magnetic drive sliding arc plasma discharge device, a cyclone separation device, an induced draft fan and a hydrogen tank, wherein the inert gas tank and the more than one gasification tank are respectively connected with the more than one catalytic pyrolysis furnace, the catalytic pyrolysis furnace is connected with the cyclone separation device through the magnetic drive sliding arc plasma discharge device, the cyclone separation device is connected with a gas collection tank through the induced draft fan, and the hydrogen tank is connected with the magnetic drive sliding arc plasma discharge device.
The method has the advantages and the technical effects that:
the value of coal tar can be greatly increased by using the coal tar as a carbon source to prepare graphene, the coal tar can be subjected to primary pyrolysis to improve the purity of a product, a carbonized precursor is generated, a sliding arc plasma is magnetically driven, the rotating speed of the arc is accelerated due to the loading effect of a magnetic field, the energy density is increased, and a stable plasma region can be formed; then, regulating and controlling various parameters in the system to generate high-quality few-layer graphene; the method converts the hazardous waste coal tar into the graphene material with high added value, has cheap and easily obtained carbon source, is simple, and can realize continuous industrial production.
Drawings
FIG. 1 is a schematic structural diagram of an apparatus for carrying out the method of the present invention;
FIG. 2 is a schematic structural diagram of a magnetically driven sliding arc plasma discharge device;
in the figure: 1: an inert gas tank; 2-1: a gasification tank I; 2-2: a gasification tank II; 3: a gas flow meter; 4-1: a catalytic pyrolysis furnace I; 4-2: a catalytic pyrolysis furnace II; 5: a hydrogen tank; 6: a magnetically driven sliding arc plasma generating device; 7: a pressure gauge; 8: a direct current high frequency high voltage power supply; 9: a cyclonic separating apparatus; 10: a product collection port; 11: an induced draft fan; 12: a gas collection tank; 13: a housing; 14: a cathode; 15: an anode; 16: a magnetic field generator; 17: stainless steel screen mesh.
Detailed Description
The present invention will be described in detail with reference to the following embodiments, but the scope of the present invention is not limited to the contents; in the examples, unless otherwise specified, all methods are conventional methods, and all reagents used therein are, unless otherwise specified, conventional commercially available reagents or reagents prepared by conventional methods;
the device for completing the method in the following embodiment comprises an inert gas tank 1, a gasification tank I2-1, a gasification tank II 2-2, a catalytic pyrolysis furnace I4-1, a catalytic pyrolysis furnace II 4-2, a hydrogen tank 5, a magnetic drive sliding arc plasma generating device 6, a cyclone separation device 9, an induced draft fan 11 and a gas collecting tank 12; the inert gas tank 1, the gasification tank I2-1 and the gasification tank II 2-2 are respectively connected with the catalytic pyrolysis furnace I4-1 and the catalytic pyrolysis furnace II 4-2, the catalytic pyrolysis furnace I4-1 and the catalytic pyrolysis furnace II 4-2 are connected with the cyclone separation device 9 through a magnetic drive sliding arc plasma discharge device, the cyclone separation device 9 is connected with the gas collection tank 12 through an induced draft fan 11, and the hydrogen tank 5 is connected with the magnetic drive sliding arc plasma discharge device 6; gas flow meters 3 are arranged on outlet pipelines of the inert gas tank 1, the gasification tank I2-1 and the gasification tank II 2-2;
the magnetic drive sliding arc plasma discharge device comprises a shell 13, a cathode 14, an anode 15, a magnetic field generator 16, a direct-current high-frequency high-voltage power supply 8 and a pressure gauge 7, wherein an inlet is formed in the shell 13, an outlet is formed in the lower portion of the shell, the cathode 14 is arranged in the shell and positioned in the center of the shell, the anode 15 is an arc-shaped plate electrode and positioned on two sides of the cathode, the magnetic field generator 16 is arranged outside the shell and generates a magnetic field to cover a reaction area, a stainless steel screen 17 is arranged in the shell and positioned below the cathode, the direct-current high-frequency high-voltage power supply 8 is respectively connected with the anode and the cathode, and the pressure gauge 7 is arranged on the shell; the magnetic field generator 4 is a permanent magnet;
example 1
The output of the byproduct coal tar generated in the coal coking process accounts for 3-5% of the coal in the furnace. In recent years, the research focus of coal tar towards high-value materials is gradually increased, particularly on graphene; the arc discharge does not need substrate transfer in various graphene preparation processes, has high repeatability and has better prospect in the aspect of continuous industrial production.
As shown in fig. 1 and 2, in this embodiment, gasified coal tar and argon gas are introduced from a gasification tank i 2-1, a gasification tank ii 2-2 and an inert gas tank 1 into a catalytic pyrolysis furnace i 4-1 and a catalytic pyrolysis furnace ii 4-2 through pipelines for pyrolysis according to a volume ratio of 10:1, wherein the mass of a nano NiO catalyst in the furnace is 54.560 g/(1L gasified coal tar); combining a catalyst with 83 percent of carbon atoms in coal tar at a pyrolysis temperature of 650 ℃, adjusting the flow rate of inert gas to enable the reaction to stay for 20 minutes to generate a carbonized precursor, introducing the carbonized precursor and hydrogen in a hydrogen tank 5 into a magnetically-driven sliding arc plasma discharge device 6, wherein the argon accounts for 90 percent of the volume of the mixed gas of the argon and the hydrogen, the magnetically-driven sliding arc plasma discharge device 6 is powered by a 40Hz and 220V direct-current high-frequency high-voltage power supply 8, the magnetic field intensity is 0.3T, the high-density non-thermal sliding arc plasma is generated by the driving of the pushing of air flow entering along a reactor and the magnetic field generated by a permanent magnet, the carbonized precursor is converted into graphene under the action of the high-density non-thermal sliding arc plasma, unreacted coal tar or other generated large-particle induced draft fans are filtered out by a stainless steel screen 17, and the graphene and the gas enter a cyclone separation device 9 under the action of an induced draft fan 11, and collecting the product graphene at a product collecting port 10 at the bottom of the cyclone device, and conveying gas generated in the reaction process into a gas collecting tank 12 through an induced draft fan 11.
Example 2
The method comprises the steps of feeding gasified coal tar and argon into a catalytic pyrolysis furnace I4-1 and a catalytic pyrolysis furnace II 4-2 for pyrolysis through pipelines according to the volume ratio of 15:1, wherein 48.740 g/(1L gasified coal tar) of Ni/NiO nanoparticles are filled in the pyrolysis furnace, the pyrolysis temperature is set to be 850 ℃, the gas flow rate is adjusted to ensure that the reaction residence time is 10 minutes, a carbonized precursor is generated, and the conversion rate of a catalyst to hydrocarbon of the coal tar is 93.5%; after being discharged from a pipeline, the gas is mixed with hydrogen (wherein the volume of argon is 95 percent of the volume of the mixed gas of argon and hydrogen) and then is sent into a magnetic drive sliding arc plasma discharge device with the magnetic strength of 0.3T, the magnetic drive sliding arc plasma discharge device is powered by a 40Hz and 220V direct-current high-frequency high-voltage power supply, a carbonization precursor is decomposed in a plasma reactor, carbon atoms generate carbon clusters, the clusters are cyclized and gathered, dangling bonds are terminated by hydrogen, finally graphene is generated, unreacted coal tar or other generated large-particle amorphous carbon is filtered out from the graphene through a stainless steel screen, the graphene and the gas enter a cyclone separation device 9 under the action of an induced draft fan 11, the graphene is collected at a product collection port 10, and the gas is collected by a gas collection tank 12.
Example 3
In the embodiment, the gasified coal tar and argon gas are introduced into nano Al filled with 55.130 g/(1L gasified coal tar) through a pipeline according to the volume ratio of 12:12O3Pyrolyzing the powder in a catalytic pyrolysis furnace I4-1 and a catalytic pyrolysis furnace II 4-2, controlling the pyrolysis temperature at 800 ℃, adjusting the gas flow rate to ensure that the reaction residence time is 8 minutes, generating a carbonized precursor, and ensuring that the conversion rate of the catalyst to the hydrocarbon of the coal tar is 90%; after the carbonized precursor is discharged from a pipeline, the carbonized precursor is mixed with hydrogen (wherein the argon accounts for 92 percent of the volume of the mixed gas of the argon and the hydrogen) and then is sent into a magnetic drive sliding arc plasma discharge device with the magnetic strength of 0.25T, the magnetic drive sliding arc plasma discharge device is powered by a direct current high-frequency high-voltage power supply of 40Hz and 220V, the carbonized precursor is decomposed in a plasma reactor, carbon atoms generate carbon clusters, the clusters are cyclized and aggregated, dangling bonds are terminated by the hydrogen to finally generate graphene, the graphene and gas generated in the reaction process are introduced into a cyclone separation device 9 under the action of a draught fan 11 after other large-particle impurities are filtered out by a stainless steel screen 17, the product graphene is collected at a bottom product collecting port 10, and the gas generated in the reaction process is sent into a gas collecting tank 12.
Claims (6)
1. A method for continuously preparing graphene by magnetically driving sliding arc plasma high-voltage discharge is characterized by comprising the following steps: the method comprises the steps of gasifying coal tar, sending the coal tar into a catalytic pyrolysis furnace filled with argon or helium, adding a nano metal or metal oxide serving as a catalyst into the pyrolysis furnace, mixing and reacting the gaseous coal tar and the catalyst to generate a carbonized precursor, introducing the carbonized precursor and hydrogen into a magnetic drive sliding arc plasma discharge device, generating high-density non-thermal sliding arc plasma through an auxiliary magnetic field, and converting the carbonized precursor into graphene under the action of the high-density non-thermal sliding arc plasma.
2. The method for continuously preparing graphene by using magnetic drive sliding arc plasma high-voltage discharge according to claim 1, wherein the method comprises the following steps: the catalyst is nano-particles of Ni, Cu, Pt, Pd, Al, NiO and Al2O3One or more of (a).
3. The method for continuously preparing graphene by using magnetic drive sliding arc plasma high-voltage discharge according to claim 2, wherein the method comprises the following steps: the pyrolysis temperature is 650-850 ℃.
4. The method for continuously preparing graphene by using magnetic drive sliding arc plasma high-voltage discharge according to claim 3, wherein the method comprises the following steps: magnetic drive slip arc plasma discharge device includes casing (13), negative pole (14), positive pole (15), magnetic field generator (16), stainless steel screen cloth (17), direct current high frequency high voltage power supply (8), manometer (7), negative pole (14) set up and locate at the casing center in the casing, positive pole (15) are located the negative pole both sides, magnetic field generator (16) set up the casing outside and the magnetic field that produces cover the reaction zone, stainless steel screen cloth (17) set up in the casing and are located the negative pole below, direct current high frequency high voltage power supply (8) respectively with the positive pole, the negative pole is connected, manometer (7) set up on the casing.
5. The method for continuously preparing graphene by using magnetic drive sliding arc plasma high-voltage discharge according to claim 4, wherein the method comprises the following steps: the argon gas accounts for 90-97% of the volume of the mixed gas of the argon gas and the hydrogen gas, and the helium gas accounts for 90-97% of the volume of the mixed gas of the helium gas and the hydrogen gas.
6. The system for completing the method for continuously preparing the graphene by the magnetic drive sliding arc plasma high-voltage discharge according to claim 5, is characterized in that: the device comprises an inert gas tank, more than one gasification tank, more than one catalytic pyrolysis furnace, a magnetic drive sliding arc plasma discharge device, a cyclone separation device, an induced draft fan and a hydrogen tank, wherein the inert gas tank and the more than one gasification tank are respectively connected with the more than one catalytic pyrolysis furnace, the catalytic pyrolysis furnace is connected with the cyclone separation device through the magnetic drive sliding arc plasma discharge device, the cyclone separation device is connected with a gas collection tank through the induced draft fan, and the hydrogen tank is connected with the magnetic drive sliding arc plasma discharge device.
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| US20050079119A1 (en) * | 2003-01-23 | 2005-04-14 | Canon Kabushiki Kaisha | Method for producing nano-carbon materials |
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| US20200223698A1 (en) * | 2016-12-21 | 2020-07-16 | Raymor Industries Inc. | Plasma processes for producing graphene nanosheets |
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- 2022-04-03 CN CN202210347490.7A patent/CN114590800A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20050079119A1 (en) * | 2003-01-23 | 2005-04-14 | Canon Kabushiki Kaisha | Method for producing nano-carbon materials |
| CN1903713A (en) * | 2006-08-02 | 2007-01-31 | 太原理工大学 | Method of preparing nano-carbon fiber using coal tar asphalt as raw material |
| US20200223698A1 (en) * | 2016-12-21 | 2020-07-16 | Raymor Industries Inc. | Plasma processes for producing graphene nanosheets |
Non-Patent Citations (2)
| Title |
|---|
| DONGNING LI ET. AL.: ""Synrhesis of graphene flakes using a non-thermal plasma based on magnetically stabilized gliding arc discharge"", 《FULLERENCES, NANOTUBES AND CARBON NANOSTRUCTURES》, vol. 28, no. 10, pages 846 - 856 * |
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