CN117643851A - CO (carbon monoxide) 2 Method for preparing single-layer graphene by catalytic reduction - Google Patents
CO (carbon monoxide) 2 Method for preparing single-layer graphene by catalytic reduction Download PDFInfo
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 54
- 238000000034 method Methods 0.000 title claims abstract description 47
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 45
- 239000002356 single layer Substances 0.000 title claims abstract description 24
- 238000010531 catalytic reduction reaction Methods 0.000 title claims abstract description 12
- 229910002091 carbon monoxide Inorganic materials 0.000 title claims abstract description 8
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims description 4
- 238000010891 electric arc Methods 0.000 claims abstract description 17
- 238000006243 chemical reaction Methods 0.000 claims abstract description 15
- 238000002156 mixing Methods 0.000 claims abstract description 13
- 239000003638 chemical reducing agent Substances 0.000 claims abstract description 12
- 239000000203 mixture Substances 0.000 claims abstract description 11
- 239000011943 nanocatalyst Substances 0.000 claims abstract description 10
- 239000002994 raw material Substances 0.000 claims abstract description 9
- 230000009471 action Effects 0.000 claims abstract description 8
- 239000007789 gas Substances 0.000 claims description 69
- 238000010438 heat treatment Methods 0.000 claims description 21
- 239000011521 glass Substances 0.000 claims description 19
- 239000000758 substrate Substances 0.000 claims description 19
- PWKWDCOTNGQLID-UHFFFAOYSA-N [N].[Ar] Chemical compound [N].[Ar] PWKWDCOTNGQLID-UHFFFAOYSA-N 0.000 claims description 11
- 238000001816 cooling Methods 0.000 claims description 11
- 238000003860 storage Methods 0.000 claims description 11
- 239000003054 catalyst Substances 0.000 claims description 8
- 150000001723 carbon free-radicals Chemical class 0.000 claims description 7
- 239000000571 coke Substances 0.000 claims description 6
- 239000002245 particle Substances 0.000 claims description 6
- RHZUVFJBSILHOK-UHFFFAOYSA-N anthracen-1-ylmethanolate Chemical compound C1=CC=C2C=C3C(C[O-])=CC=CC3=CC2=C1 RHZUVFJBSILHOK-UHFFFAOYSA-N 0.000 claims description 4
- 239000003830 anthracite Substances 0.000 claims description 4
- 229910004298 SiO 2 Inorganic materials 0.000 claims description 3
- 239000012494 Quartz wool Substances 0.000 claims description 2
- 239000012298 atmosphere Substances 0.000 claims description 2
- 238000000151 deposition Methods 0.000 claims description 2
- 229910001220 stainless steel Inorganic materials 0.000 claims description 2
- 239000010935 stainless steel Substances 0.000 claims description 2
- 229910052799 carbon Inorganic materials 0.000 abstract description 10
- 230000008569 process Effects 0.000 abstract description 7
- 230000000694 effects Effects 0.000 abstract description 3
- 238000010924 continuous production Methods 0.000 abstract description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 110
- 229910002092 carbon dioxide Inorganic materials 0.000 description 55
- 239000001569 carbon dioxide Substances 0.000 description 55
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 14
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 9
- 239000001301 oxygen Substances 0.000 description 9
- 229910052760 oxygen Inorganic materials 0.000 description 9
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 8
- 229910052757 nitrogen Inorganic materials 0.000 description 7
- 238000005516 engineering process Methods 0.000 description 5
- 238000002360 preparation method Methods 0.000 description 5
- 229910052786 argon Inorganic materials 0.000 description 4
- 230000008901 benefit Effects 0.000 description 4
- 239000010410 layer Substances 0.000 description 4
- 238000001237 Raman spectrum Methods 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 238000010926 purge Methods 0.000 description 3
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 2
- 238000001069 Raman spectroscopy Methods 0.000 description 2
- 239000000969 carrier Substances 0.000 description 2
- 238000005229 chemical vapour deposition Methods 0.000 description 2
- 238000010248 power generation Methods 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 229920000742 Cotton Polymers 0.000 description 1
- 238000003332 Raman imaging Methods 0.000 description 1
- 238000001530 Raman microscopy Methods 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 238000009412 basement excavation Methods 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 238000003421 catalytic decomposition reaction Methods 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
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- 230000005284 excitation Effects 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
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- 239000011261 inert gas Substances 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000001000 micrograph Methods 0.000 description 1
- 229910021421 monocrystalline silicon Inorganic materials 0.000 description 1
- 229910021392 nanocarbon Inorganic materials 0.000 description 1
- 239000002086 nanomaterial Substances 0.000 description 1
- 230000006911 nucleation Effects 0.000 description 1
- 238000010899 nucleation Methods 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- 230000008844 regulatory mechanism Effects 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
Abstract
The invention discloses a CO 2 Method for preparing single-layer graphene by catalytic reduction, wherein CO is prepared by the method 2 The gas enters a fluidized bed reactor through a raw material gas inlet, and CO are prepared under the actions of oxygen-free, 1000-1300 ℃ and reducing agent 2 Gas, containing CO and CO 2 The mixture of gas and nano catalyst is fed into two-stage Venturi jet unit from product outlet and mixing gas tank, and fed into arc discharge reaction unit after being fully and uniformly mixedIn the element, preparing single-layer graphene under the action of a nano catalyst; the invention selects greenhouse effect gas CO 2 As a carbon source, CO/CO is assisted by thermochemical tandem jet plasma 2 The graphene of the mixture is nucleated, and the high growth rate of the product seeds is maintained, so that a large-scale monocrystal is achieved, the reaction condition is controllable, the continuous production can be realized, and the method aims at solving the problem of CO at present 2 Emission and energy shortage issues provide a process basis.
Description
Technical Field
The invention belongs to the technical field of carbon nanomaterial preparation, and in particular relates to a CO 2 A method for preparing monolayer graphene by catalytic reduction.
Background
Electrocatalytic CO 2 The preparation of the nano carbon material has potential for researching the directional regulation mechanism of the excavation product. It has been reported that under mild water conditions, due to CO 2 Has higher thermodynamic stability, C 5+ The product was never directly CO used 2 Synthesized as the sole carbon source. Another method of carbon dioxide conversion is therefore a "two-step" strategy, in which CO 2 First converted to CO, which then evolves into other products in the next chemical reaction, for example: and (3) graphene. When selecting a suitable and inexpensive carbon source for preparing graphene, a cost-effective and environmentally friendly raw material, CO, for producing graphene can be considered 2 。
At present, the preparation methods of graphene are divided into a Top-Down (Top-Down) method and a Bottom-Up (Bottom-Up) method. The Top-Down method mainly comprises a micro-mechanical stripping method, a liquid phase stripping method, a redox method and the like; the Bottom-Up method mainly comprises a chemical vapor deposition method, an epitaxial growth method, an organic synthesis method and the like. The Top-Down method is a Top-Down method, and mostly adopts graphite as a raw material, and adopts a physical and chemical method to obtain the graphene. The Bottom-Up method is the "Bottom-Up" method, mostly based on hydrocarbonsC-element-containing materials such as materials and monocrystalline silicon are used as raw materials, and graphene is prepared in high-temperature and ultra-vacuum environments. Compared with other graphene preparation methods, the CVD method has the advantages of high yield, large growth area, controllable layer number and the like, and the performance of the method is closer to the intrinsic physical properties of graphene. The preparation method of the graphene is better, stronger and more outstanding. In particular with carbon dioxide (CO) 2 ) The graphene oxide has carbon (C) and oxygen (O) atoms, and is a more environment-friendly and safer carbon source in the growth of graphene. The method of utilizing thermochemistry, especially renewable energy sources such as power sources (photovoltaic power generation, wind power generation and the like) is a very clean and effective method, and has the advantages of controllable reaction process, mild reaction conditions and recoverable catalyst.
Disclosure of Invention
The invention provides a method for preparing greenhouse effect gas CO 2 Method for preparing single-layer graphene by catalytic reduction, and device for completing method comprises CO 2 The device comprises a gas tank, a mixing gas tank, a fluidized bed reactor, a two-stage venturi jet unit, an arc discharge generating unit, an exhaust fan and a gas storage chamber; the fluidized bed reactor comprises a shell I, wherein a raw material gas inlet is formed in the bottom of the shell I, a product outlet is formed in the top of the shell I, more than one heat carrier is arranged in the shell I, a two-stage venturi jet unit consists of a primary venturi jet device and a secondary venturi jet device which are connected in series, the product outlet and a mixed gas tank are respectively connected with 2 inlets of the primary venturi jet device, an arc discharge reaction unit comprises a shell II, the outlets of the secondary venturi jet devices are communicated with one end of the shell II of the arc discharge reaction unit, a plurality of discharge electrodes are arranged in the shell II, a product collecting glass substrate is obliquely arranged at the inner outlet end of the shell II, a cooling device is sleeved outside the outlet end of the shell II and is positioned outside the product collecting glass substrate, a gas storage chamber is communicated with the outlet of the shell II through an exhaust fan, a power supply II is connected with the discharge electrodes, the power supply I is connected with a heating element through a temperature controller, and the heating element is arranged below the heat carrier;
before the device of the invention is used, the fluidized bed reactor is purged by inert gas until the deviceNo oxygen is contained in the water; then heating the mixture to 1000-1300 ℃ by a heating element, and keeping the temperature constant to CO 2 Introducing gas into the fluidized bed reactor from a raw material gas inlet, wherein the gas flow is 800-1000 sccm; reducing to CO/CO under the action of a reducing agent at 1000-1300 ℃ without oxygen 2 Gas, CO/CO-containing 2 After the gas and the nitrogen-argon mixture containing the nano catalyst are respectively and fully and uniformly mixed in a two-stage Venturi jet unit from a product outlet and a mixing gas tank, the gas is mixed with the nano catalyst, the nano catalyst carries out primary catalytic decomposition on carbon source substances, CO is decomposed into carbon free radicals through a direct current plasma discharge process, and the carbon free radicals nucleate and grow on the surface of the catalyst, and meanwhile, the CO with the volume concentration lower than 2 percent is formed on the surface of the catalyst 2 Growing in the atmosphere to obtain a single-layer structure, then rapidly cooling the product to below 200 ℃ through a cooling device, and uniformly depositing the product on a product collecting glass substrate; and collecting the gas into the gas storage chamber to obtain the single-layer graphene.
The reducing agent is coke or anthracite particles which are placed on a heat carrier, the heat carrier is a stainless steel net, and the pore diameter of the upper hole of the heat carrier is smaller than the particle diameter of the reducing agent.
The volume concentration of CO injected into the two-stage venturi jet unit is more than 98 percent.
The CO 2 The gas flow meter and the valve are arranged on the outlets of the gas tank and the mixing gas tank, and quartz wool is arranged at the product outlet of the fluidized bed reactor to prevent the reducing agent from entering the two-stage Venturi jet units.
And the temperature in the arc discharge generating unit furnace is 800-1500 ℃ and the graphene growth temperature is 800-1500 ℃.
The nano catalyst of the graphene is NiO and Al 2 O 3 、CaCO 3 、Fe 2 O 3 、MgO、SiO 2 、ZrO 2 One or more of them.
The collecting device of the product graphene is a 60-degree inclined glass substrate, so that the maximum capturing area is obtained.
The interval between the discharge electrodes is 25-35 mm.
The method has the advantages and technical effects that:
1、in the form of CO 2 As a carbon source, preparing graphene has a value that can be greatly increased. The invention will thermocatalyze CO 2 The technology is coupled with the jet plasma technology, so that the activation state of carbon monoxide can be excited under the arc discharge, and the improvement of the conversion rate of graphene is possible;
2. the front end of the invention adopts a high-temperature fluidized bed thermal catalytic reduction technology, the rear end adopts a jet plasma technology, the heat transfer process exists, the energy waste is less, and certain economic benefit is realized;
3. the adopted nanoscale catalyst particles have high exposed atom proportion, so that more active sites are caused, and CO can participate in the reaction more;
4. compared with the traditional graphene growth process which needs to be carried out on a metal substrate, the method belongs to self-supporting growth of graphene, provides greater flexibility, and does not need to consider additional components possibly introduced by a base material;
5. realization of CO 2 And (5) high-value utilization of the product. By thermocatalytic CO 2 The coupled jet plasma technology can solve the problems of CO 2 The excessive discharge problem of (2) is solved, and meanwhile, the graphene is self-supported and simultaneously maintains good quality and a single-layer structure, so that the method is simple and continuous production can be realized.
Drawings
FIG. 1 is a schematic diagram of an apparatus for carrying out the method of the present invention;
FIG. 2 is a Raman spectrum of graphene of example 1;
FIG. 3 is a Raman microscope image of graphene of example 1;
in the figure: 1-CO 2 A gas tank; 2-a mixing tank; 3-a feed gas inlet; 4-a heating element; 5-a heat carrier; 6-a power supply I; 7-a product outlet; 8-a temperature controller; 9-primary venturi jet; 10-two-stage venturi jet; 11-discharge electrodes; 12-ground wire; 13-collecting a glass substrate by a product; 14-a cooling device; 15-an exhaust fan; 16-an air storage chamber; 17-power source II.
Detailed Description
The present invention will be described in detail with reference to the following specific embodiments, but the scope of the present invention is not limited to the above description; the methods in the examples are conventional methods unless otherwise specified.
As shown in FIG. 1, the apparatus used in the following embodiments includes CO 2 The device comprises a gas tank 1, a mixing gas tank 2, a fluidized bed reactor, a two-stage venturi jet unit, an arc discharge generating unit, an exhaust fan 15 and a gas storage chamber 16; the fluidized bed reactor comprises a shell I, a feed gas inlet 3 is formed in the bottom of the shell I, a product outlet 7 is formed in the top of the shell I, 2 heat carriers 5 are arranged in the shell I, a reducing agent is placed on the heat carriers, a two-stage venturi jet unit consists of a first-stage venturi jet 9 and a second-stage venturi jet 10 which are connected in series, the product outlet 7 and a mixing gas tank 2 are respectively connected with 2 inlets of the first-stage venturi jet, an arc discharge reaction unit comprises a shell II, the outlet of the second-stage venturi jet is communicated with one end of the shell II of the arc discharge reaction unit, a plurality of discharge electrodes 11 (the interval of the discharge electrodes is 30 mm) are arranged in the shell II, a product collecting glass substrate 13 is obliquely arranged at the outlet end of the shell II, a cooling device 14 is sleeved outside the outlet end of the shell II and is positioned outside the product collecting glass substrate, a gas storage chamber 16 is communicated with the outlet of the shell II through an exhaust fan 15, a power supply II 17 is connected with the plurality of discharge electrodes, a power supply I6 is connected with a heating element 4 through a temperature controller 8, the heating element is arranged below the heat carrier 5, and the shell II is grounded through a ground wire 12 2 The gas flow meters and valves are arranged on the outlets of the gas tank and the mixing gas tank, and quartz cotton is arranged at the product outlet of the fluidized bed reactor to prevent the reducing agent from entering the two-stage Venturi jet units;
example 1
Purging the fluidized bed reactor with nitrogen until no oxygen is contained in the device, placing coke on a heat carrier 5, heating the fluidized bed reactor by a heating element 4, heating to 1300 ℃ and keeping the temperature constant, and adding CO 2 Introducing gas into the fluidized bed reactor from a feed gas inlet 3, wherein the gas flow is 800sccm; reducing to CO/CO under the action of coke at 1300 ℃ without oxygen 2 At this time, the volume concentration of CO was 99.5%, CO 2 Is 0.5%; will contain CO/CO 2 Through the product outlet, the nitrogen-argon mixture containing nano aluminum oxide (the mass of the mixture of aluminum oxide and nitrogen-argon)30% by volume, wherein the volume ratio of nitrogen to argon in the nitrogen-argon mixed gas is 1:1), and the mixture enters the 2 inlets of the primary venturi jet 9 from the mixing gas tank, is uniformly mixed, then enters the secondary venturi jet 10, is fully mixed again, enters the arc discharge generating unit, and is subjected to a direct current plasma discharge process at the constant temperature of 1100+/-50 ℃, CO is decomposed into carbon free radicals, and is nucleated and grown on the surface of the catalyst, and meanwhile, low-content CO 2 The presence of (2) inhibits the growth of the second layer to obtain a single-layer structure, and then the temperature of the product is suddenly reduced to below 200 ℃ by the cooling device 14, and the product is uniformly deposited on the product collecting glass substrate; and collecting the gas in the gas storage chamber, and removing the glass substrate attached with the product to obtain high-quality single-layer graphene, wherein the coverage rate of the graphene on the glass substrate is as high as 95%.
The raman spectra of graphene and raman microscopy are shown in fig. 1 and 2, respectively, and the raman spectra of fig. 1 were obtained using a raman imaging microscope equipped with a x 20 objective lens and a 532nm excitation laser operating at an output power of 2mW, and it is clear from the figures that the G band and 2D band (each located at about 1350 cm) -1 Where 2690cm -1 Where) G/2D is less than or equal to 0.66 (G/2D < 0.66). As used herein, the G/2D ratio refers to the ratio of the peak intensities of the bands, and typically the G/2D intensity ratio is in the range of 0.7, which is illustrated as a single layer. Fig. 2 is a graph of graphene under a raman microscope with a resolution of up to 100 μm, from which it can be seen that the samples are ordered in a honeycomb lattice.
Example 2
Purging the fluidized bed reactor with nitrogen until no oxygen is contained in the device, placing coke on a heat carrier 5, heating the fluidized bed reactor by a heating element 4, heating to 1200deg.C, maintaining the temperature, and adding CO 2 Introducing gas into the fluidized bed reactor from a raw material gas inlet 3, wherein the gas flow is 1000sccm; reducing to CO/CO under the action of coke at 1200 ℃ and without oxygen 2 At this time, the volume concentration of CO was 99%, CO 2 Is 1% by volume; will contain CO/CO 2 From the product outlet, contains nano Al 2 O 3 Nitrogen-argon mixture (nano Al) 2 O 3 Mass of mixture with nitrogen-argonThe volume ratio of nitrogen to argon in the nitrogen-argon mixed gas is 35 percent, the volume ratio of the nitrogen to the argon is 1:1), the mixed gas enters 2 inlets of the primary venturi jet device 9 from the mixed gas tank, and then enters the secondary venturi jet device 10 for fully mixing again, and then enters the arc discharge generating unit, the CO is decomposed into carbon free radicals through the direct current plasma discharge process at the constant temperature of 1300+/-50 ℃, the nucleation and the growth are carried out on the surface of the catalyst, and meanwhile, the first concentration CO is obtained by the steps of 2 The existence of the (2) can inhibit the growth of the second layer to obtain a single-layer structure, then the temperature of the product is suddenly reduced to below 200 ℃ through a cooling device, and the product is uniformly deposited on the glass substrate; and collecting the gas in the gas storage chamber, and removing the glass substrate attached with the product to obtain high-quality single-layer graphene, wherein the coverage rate of the graphene on the glass substrate is as high as 92%.
Example 3
Purging the fluidized bed reactor with nitrogen until no oxygen is contained in the device, placing anthracite particles on a heat carrier 5, heating the inside temperature of the fluidized bed reactor by a heating element 4, heating to 1100 ℃ and keeping constant temperature, and adding CO 2 Introducing gas into the fluidized bed reactor from a raw material gas inlet 3, wherein the gas flow is 900sccm; reducing to CO/CO under the action of anthracite at 1100 ℃ without oxygen 2 At this time, the volume concentration of CO was 98%, CO 2 Is 2% by volume. CO/CO 2 From the product outlet, contain nano SiO 2 Nitrogen-argon mixture (nano SiO) 2 28% of the mass volume ratio of the mixed gas with nitrogen-argon, wherein the volume ratio of the nitrogen and the argon in the mixed gas with nitrogen-argon is 1:1), the mixed gas enters 2 inlets of the primary venturi jet 9 from a mixed gas tank, uniformly mixed, then enters the secondary venturi jet 10, fully mixed again, enters an arc discharge generating unit, and is subjected to a direct current plasma discharge process at a constant temperature of 850+/-50 ℃, CO is decomposed into carbon free radicals, the carbon free radicals nucleate and grow on the surface of the catalyst, and meanwhile, the first concentration CO 2 The existence of the (2) can inhibit the growth of the second layer to obtain a single-layer structure, then the temperature of the product is suddenly reduced to below 200 ℃ through a cooling device, and the product is uniformly deposited on the glass substrate; collecting gas into a gas storage chamber, removing the glass substrate with the attached product to obtain high-quality single-layer graphene, wherein the graphene is arranged on the glass substrateCoverage is as high as 88%.
Claims (6)
1. CO (carbon monoxide) 2 A method for preparing single-layer graphene by catalytic reduction is characterized in that a device for completing the method comprises CO 2 The device comprises a gas tank (1), a mixing gas tank (2), a fluidized bed reactor, a two-stage Venturi jet unit, an arc discharge generating unit, an exhaust fan (15) and a gas storage chamber (16); the fluidized bed reactor comprises a shell I, a raw gas inlet (3) is formed in the bottom of the shell I, a product outlet (7) is formed in the top of the shell I, more than one heating medium (5) is arranged in the shell I, a reducing agent is placed on the heating medium, a two-stage venturi jet unit consists of a primary venturi jet device (9) and a secondary venturi jet device (10) which are connected in series, the product outlet (7) and a mixed gas tank (2) are respectively connected with 2 inlets of the primary venturi jet device, the arc discharge reaction unit comprises a shell II, the secondary venturi jet device outlet is communicated with one end of the shell II of the arc discharge reaction unit, a plurality of discharge electrodes (11) are arranged in the shell II, a product collecting glass substrate (13) is obliquely arranged at the outlet end of the shell II, a cooling device (14) is sleeved outside the outlet end of the shell II and is positioned outside the product collecting glass substrate, a gas storage chamber (16) is communicated with the outlet of the shell II through an exhaust fan (15), a power supply II (17) is connected with the discharge electrodes, a power supply I (6) is connected with a heating element (4) through a temperature controller (8), the heating element is arranged below the heating element (5), and the shell is grounded through a ground wire (12);
CO 2 the gas enters a fluidized bed reactor through a raw material gas inlet, and CO are prepared under the actions of oxygen-free, 1000-1300 ℃ and reducing agent 2 Is a gas containing CO and CO 2 The gas of (2) and the nitrogen-argon mixture containing the nano catalyst enter a two-stage Venturi jet unit from a product outlet and a mixing gas tank respectively, are fully and uniformly mixed, enter an arc discharge reaction unit, and under the action of the nano catalyst, CO is decomposed into carbon free radicals, and is nucleated and grown on the surface of the catalyst, and at the same time, CO with the volume concentration lower than 2 percent is obtained 2 Obtaining a single-layer structure in the atmosphere, then cooling the product to below 200 ℃ by a cooling device, anduniformly depositing on a product collection glass substrate; and preparing the single-layer graphene.
2. The CO according to claim 1 2 The method for preparing the single-layer graphene by catalytic reduction is characterized by comprising the following steps of: the reducing agent is coke or anthracite particles which are placed on the heat carrier (4), the heat carrier (4) is a stainless steel net, and the aperture of the heat carrier is smaller than the particle size of the reducing agent.
3. The CO according to claim 1 2 The method for preparing the single-layer graphene by catalytic reduction is characterized by comprising the following steps of: CO 2 The gas flow rate is 800-1000 sccm.
4. The CO according to claim 1 2 The method for preparing the single-layer graphene by catalytic reduction is characterized by comprising the following steps of: and growing graphene in the arc discharge generation unit at 800-1500 ℃.
5. The CO according to claim 1 2 The method for preparing the single-layer graphene by catalytic reduction is characterized by comprising the following steps of: the nano catalyst is NiO, al 2 O 3 、CaCO 3 、Fe 2 O 3 、MgO、SiO 2 、ZrO 2 One or more of the following; the mass volume ratio g of the nano catalyst to the nitrogen-argon mixed gas is 25-35%.
6. The CO according to claim 1 2 The method for preparing the single-layer graphene by catalytic reduction is characterized by comprising the following steps of: CO 2 The gas flow meter and the valve are arranged on the outlets of the gas tank and the mixing gas tank, and quartz wool is arranged at the product outlet of the fluidized bed reactor to prevent the reducing agent from entering the two-stage Venturi jet units.
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| CN202311526261.2A CN117643851A (en) | 2023-11-16 | 2023-11-16 | CO (carbon monoxide) 2 Method for preparing single-layer graphene by catalytic reduction |
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| CN202311526261.2A CN117643851A (en) | 2023-11-16 | 2023-11-16 | CO (carbon monoxide) 2 Method for preparing single-layer graphene by catalytic reduction |
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