CN113998671B - Novel discharge electrode and device and method for preparing hydrogen by reforming methane with microwave liquid-phase plasma - Google Patents

Novel discharge electrode and device and method for preparing hydrogen by reforming methane with microwave liquid-phase plasma Download PDF

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CN113998671B
CN113998671B CN202111514192.4A CN202111514192A CN113998671B CN 113998671 B CN113998671 B CN 113998671B CN 202111514192 A CN202111514192 A CN 202111514192A CN 113998671 B CN113998671 B CN 113998671B
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孙冰
王秋颖
刘景林
信延彬
朱小梅
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Dalian Maritime University
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    • C01B3/02Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
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Abstract

The invention discloses a novel discharge electrode and a device and a method for preparing hydrogen by reforming methane with microwave liquid-phase plasma, wherein the discharge electrode comprises: inserting a tungsten rod into the center of the boron nitride tube and fixing, wherein the tungsten rod is higher than the upper end of the boron nitride tube by a certain distance, and sharpening the exposed end of the tungsten rod to facilitate the generation and maintenance of plasma; the device comprises an air inlet system, a microwave plasma reaction system and a product separation system, wherein the air inlet system comprises methane gas, a discharge electrode, a raw material tank and a water pump; the reforming hydrogen production method disclosed by the invention is directly carried out in water, carbon deposition cannot be generated on an electrode, stable operation of plasma can be ensured, the generated carbon source mainly exists in the form of element carbon particles and small molecular carbon, the content is low, and the generated element carbon particles are easily separated by filtration.

Description

Novel discharge electrode and device and method for preparing hydrogen by reforming methane through microwave liquid-phase plasma
Technical Field
The invention relates to the technical field of plasmas, in particular to a novel discharge electrode, a device and a method for preparing hydrogen by reforming methane with microwave liquid-phase plasmas.
Background
Hydrogen is used as a clean energy source, has the advantage of large combustion heat value, and the product is water, so that secondary pollution can not be generated, and the hydrogen is an ideal secondary energy source. And natural gas is an economic and reasonable choice in the process of producing hydrogen from fossil fuel due to abundant reserves. Methane has been the focus of recent research as a major component of natural gas.
Conventional methane reforming processes for hydrogen production include steam reforming of methane, dry reforming of methane, partial oxidation reforming of methane, autothermal reforming of methane, and catalytic decomposition of methane. Wherein the methane steam reforming process does not need oxygen, the reaction temperature is high, and H 2 the/CO ratio is higher than other technologies and therefore more suitable for producing hydrogen rich syngas. To g inThe problems of high fuel consumption cost and catalyst deactivation at high temperature, and the research on the catalyst-free plasma technology. At present, the main methods for hydrogen production by wet reforming of plasma methane include: dielectric barrier discharge, sliding arc discharge, microwave discharge, spark discharge, and the like. However, in the current view, the above several methods for producing hydrogen by reforming methane by using plasma are all formed by discharging in a gas phase. Gas phase discharge has certain limitations, and firstly, water molecules need to be heated and vaporized, so that additional energy consumption is increased. And secondly, the plasma density in gas phase discharge is low, the discharge is unstable, and the hydrogen production efficiency is low. Compared with gas-phase plasma, liquid is used as a discharge medium for liquid-phase discharge plasma, and the liquid-phase discharge plasma has the characteristics of high plasma density, direct mass transfer, rich active components and the like.
Disclosure of Invention
The invention provides a novel discharge electrode, a device and a method for preparing hydrogen by reforming methane by microwave liquid-phase plasma, which aim to solve the problems of low plasma density, unstable discharge, low hydrogen preparation efficiency, easy carbon deposition generation and the like in gas-phase discharge.
In order to achieve the purpose, the technical scheme of the invention is as follows:
a novel discharge electrode and a device for preparing hydrogen by reforming methane with microwave liquid-phase plasma comprise a discharge electrode, a raw material tank, a water pump, a microwave generator, a waveguide tube, a sleeve, a reactor, a vacuum pump, a gas collecting device and a condensing device; methane gas tangentially enters the reactor from the discharge electrode through an air inlet pipeline, and a gas flowmeter is arranged on the air inlet pipeline;
one end of the waveguide tube is connected with the microwave generator; the sleeve is vertically fixed at the lower part of the waveguide tube, the reactor vertically penetrates through the upper part of the waveguide tube and is nested in the sleeve, and the discharge electrode is arranged in the sleeve;
the water suction pump is arranged in the raw material tank, and the top of the raw material tank is connected with a vacuum pump and a gas collecting device;
a liquid inlet pipeline and a first gas outlet pipeline are arranged between the reactor and the raw material tank, a second gas outlet pipeline is connected with the raw material tank and the condensing device, and a third gas outlet pipeline is connected with the condensing device and the gas collecting device.
Further, the discharge electrode comprises an electrode, a boron nitride base and a boron nitride side wall tube, the electrode is arranged in the boron nitride side wall tube, and the electrode/boron nitride side wall tube is fixed on the boron nitride base.
Further, the height of the electrode is larger than that of the boron nitride side-wall tube, and the relative distance between the electrode and the boron nitride side-wall tube can be adjusted through the boron nitride base.
Furthermore, the top of the electrode is sharpened, and the boron nitride base is provided with a plurality of symmetrical hole-shaped structures to ensure that methane gas uniformly flows into the reactor.
Further, the boron nitride side wall tube is designed into a bullet shape at one end close to the electrode, so that inflowing methane molecules are concentrated at the tip of the discharge electrode.
Further, the electrode is any one of a tungsten rod, a copper rod and a stainless steel rod.
The reformed methane hydrogen production method based on the novel discharge electrode and the device for reforming methane hydrogen production by microwave liquid-phase plasma comprises the following steps:
s1: injecting methane gas and the aqueous solution in the raw material tank into a reactor, and fully mixing;
s2: carrying out pressure reduction treatment on the reactor and the raw material tank by using a vacuum pump;
s3: starting a microwave generator to generate plasma at the tip of the electrode;
s4: the plasma acts on the methane and the water solution to generate hydrogen, and the hydrogen is collected and analyzed after being cooled by the raw material tank and the condensing device.
Further, in the step S1, the feed flow rate of the methane gas is 0.1L/min to 5.0L/min, the internal pressure of the reactor is 5 kPa to 10kPa, and the volume of the aqueous solution injected into the reactor is 150 mL to 500mL.
Further, in the step S1, the aqueous solution is one or more of deionized water, an aqueous sodium chloride solution, an acidic aqueous solution, a basic aqueous solution, and an aqueous alcohol solution.
In step S1, the aqueous solution is preferably one or more of deionized water, an aqueous sodium chloride solution, an acidic aqueous solution, a basic aqueous solution, an oxidizing aqueous solution, a reducing aqueous solution, and an alcohol aqueous solution.
Further, in the step S3, the microwave input power is 600-1200W.
Further, in the step S1, one or more of nitrogen, argon, helium, and carbon dioxide may be added to the methane gas as an auxiliary gas.
The novel discharge electrode, the device for reforming methane to produce hydrogen and the method thereof disclosed by the invention have the advantages that the methane reforming hydrogen production reaction is directly carried out in the aqueous solution without evaporation by carrying out the methane reforming hydrogen production reaction in the microwave liquid phase discharge plasma system, so that the energy is saved and the equipment is simplified. High-activity particles generated by plasma at the electrode end can trigger methane reforming hydrogen production reaction under mild conditions, and a catalyst does not need to be added, so that the problem that the service time of the catalyst is limited is avoided. Has the advantages of high methane conversion rate, quick reaction time, convenient operation and the like, and is more suitable for distributed small-scale hydrogen production. In addition, the method for preparing hydrogen by reforming does not generate carbon deposition on the electrode, can ensure the stable operation of plasma, and the generated carbon source mainly exists in the form of element carbon particles and small molecular carbon. For hydrocarbons in microwave liquid phase plasma gas phase products, only C was detected 2 Compound, and the content is low. Under high power conditions, little hydrocarbon is produced and the elemental carbon particles produced are easily separated by filtration.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the embodiments or the description of the prior art will be briefly described below, and it is obvious that the drawings in the following description are some embodiments of the present invention, and those skilled in the art can obtain other drawings based on the drawings without inventive labor.
FIG. 1 is a schematic structural diagram of a direct coupling microwave liquid phase plasma methane reforming hydrogen production device of the present invention;
FIG. 2 is a schematic view of a discharge electrode structure according to the present invention;
FIG. 3 is a flow chart of the method for producing hydrogen by methane reforming with direct coupling microwave liquid-phase plasma according to the present invention;
FIG. 4 is a diagram of the gas product after discharge of TCD detection in gas chromatography according to the present invention.
In the figure, 1, methane gas, 2, an air inlet pipeline, 3, a gas flowmeter, 4, a discharge electrode, 5, a reactor, 6, a liquid inlet pipeline, 7, a first air outlet pipeline, 8, a raw material tank, 9, a waveguide tube, 10, a sleeve, 11, a second air outlet pipeline, 12, a microwave generator, 13, a water suction pump, 14, a gas collecting device, 15, a vacuum pump, 16, a condensing device, 17, a third air outlet pipeline, 4-1, a boron nitride side wall pipe, 4-2, an electrode, 4-3 and a boron nitride base.
Detailed Description
To make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions of the embodiments of the present invention will be described clearly and completely with reference to fig. 1 to 4 in the embodiments of the present invention, and it is obvious that the described embodiments are some, but not all, embodiments of the present invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
As shown in fig. 1 and 2, the novel discharge electrode and device for producing hydrogen by reforming methane with microwave liquid-phase plasma comprises a discharge electrode 4, a raw material tank 8, a water pump 13, a microwave generator 12, a waveguide 9, a casing 10, a reactor 5, a vacuum pump 15, a gas collecting device 14 and a condensing device 16; methane gas 1 enters the reactor 5 from the discharge electrode 4 through an air inlet pipeline 2, and a gas flowmeter 3 is arranged on the air inlet pipeline 2; one end of the waveguide tube 9 is connected with the microwave generator 12; the casing 10 is vertically fixed on the lower part of the waveguide tube 9, the reactor 5 vertically penetrates from the upper part of the waveguide tube 9 and is nested in the casing 10, and the discharge electrode 4 is arranged in the casing 10; the water suction pump 13 is arranged in the raw material tank 8, and the top of the raw material tank 8 is connected with a vacuum pump 15 and a gas collecting device 14; a liquid inlet pipeline 6 and a first gas outlet pipeline 7 are arranged between the reactor 5 and the raw material tank 8, a second gas outlet pipeline 11 is connected with the raw material tank 8 and a condensing device 16, and a third gas outlet pipeline 17 is connected with the condensing device 16 and a gas collecting device 14. In this embodiment, the waveguide 9 is a rectangular waveguide, the sleeve is a metal sleeve, one end of the gas inlet pipeline 2 is connected to the gas flowmeter 3, one end of the gas inlet pipeline is connected to the discharge electrode 4, gas enters the reactor 5 tangentially, the upper part of the reactor 5 is connected to the liquid inlet pipe 6 and the first gas outlet pipe 7, the other ends of the liquid inlet pipe 6 and the first gas outlet pipe 7 are connected to the raw material tank 8, the lower part of the reactor 5 vertically penetrates through the rectangular waveguide 9, the metal sleeve 10 is vertically fixed to the lower part of the rectangular waveguide 9, the discharge electrode 4 is arranged in the metal sleeve 10 and is completely immersed in liquid, one end of the rectangular waveguide 9 is connected to the microwave generator 12, the top of the raw material tank 8 is connected to the dry vacuum pump 15 and the gas outlet pipe 11, and the gas outlet pipeline is connected to the condensing device.
Further, the discharge electrode 4 comprises an electrode 4-2, a boron nitride base 4-3 and a boron nitride side wall tube 4-1, wherein the electrode 4-2 is arranged in the boron nitride side wall tube 4-1 and fixed on the boron nitride base 4-3. In this embodiment, preferably, the electrode 4-2 is a tungsten rod, the discharge electrode 4 is composed of a tungsten rod 4-2, a boron nitride sidewall tube 4-1 and a boron nitride base 4-3, the tungsten rod 4-2 is inserted into the center of the boron nitride sidewall tube 4-1 and fixed by the boron nitride base 4-3, the tungsten rod 4-2 is at a certain distance from the upper end of the boron nitride sidewall tube 4-1, and the exposed end of the tungsten rod 4-2 is sharpened, which is beneficial to the generation and maintenance of plasma. After being transported by a gas transmission pipeline, the methane gas is output from a gap between the tungsten rod 4-2 and the boron nitride side wall pipe 4-1 and rapidly reaches the position near the tip of the electrode, and plasma is generated at the tip of the electrode.
Further, the height of the electrode 4-2 is larger than that of the boron nitride sidewall tube 4-1, and the relative distance between the electrode 4-2 and the boron nitride sidewall tube 4-1 can be adjusted by the base 4-3. Furthermore, the top of the electrode 4-2 is sharpened, and a plurality of symmetrical hole-shaped structures are arranged on the base 4-3. Further, the electrode 4-2 is one or more of a tungsten rod, a copper rod and a stainless steel rod. In the embodiment, the discharge end of the boron nitride side-wall tube 4-1 close to the tungsten rod 4-2 is designed into a bullet shape, which is beneficial to gathering methane gas near a discharge electrode after inputting methane gas and improving the conversion rate of methane; the boron nitride base plate 4-3 is designed into a symmetrical porous structure, so that methane gas is uniformly fed into the reactor.
As shown in fig. 3, the method for producing hydrogen by reforming methane based on the novel discharge electrode and the device for producing hydrogen by reforming methane by microwave liquid-phase plasma comprises the following steps:
step 11: injecting methane gas and the water solution in the raw material tank into the reactor through a discharge electrode and a water pump respectively, and fully mixing;
step 22: decompressing the reactor and the raw material tank by using a dry vacuum pump;
step 33: starting a microwave generator device and generating plasma at the tip of a discharge electrode;
and step 44: liquid phase discharge generates hydrogen on methane and water solution due to the action of energetic particles generated by plasma generation;
step 55: the hydrogen is collected and analyzed after being cooled by the feed tank and the condensing device.
Wherein the aqueous solution is one or more of deionized water, sodium chloride aqueous solution, acidic aqueous solution, alkaline aqueous solution, oxidizing aqueous solution, reducing aqueous solution and alcohol aqueous solution. In this embodiment, preferably, the aqueous solution is deionized water.
In addition, auxiliary gas can be added in the application in order to improve the conversion rate of methane, wherein the auxiliary gas comprises one or more of nitrogen, argon, helium and carbon dioxide. The auxiliary gas enters the reactor through two ways, one way is that the auxiliary gas enters the reactor tangentially from the discharge electrode as the same as methane gas, and the other way is that the auxiliary gas enters the reactor through the upper part of the reactor through a liquid inlet pipe.
Example 1:
the method comprises the steps of keeping the pressure inside a reactor at 10kPa by using a dry vacuum pump, adjusting a gas flowmeter to keep the inflow rate of methane at 0.90L/min, adjusting the relative distance between one discharge end of a tungsten rod and a boron nitride side wall pipe to 10mm, using deionized water as an aqueous solution, keeping the volume of the deionized water in the reactor at 220mL by using a liquid inlet pump, keeping the water temperature of the deionized water at 25 ℃, starting a microwave generator to enable the microwave input power to be 900W, enabling high-energy particles generated by liquid phase discharge to act on methane and the aqueous solution to generate hydrogen, collecting the hydrogen after discharge by using a gas collection device, and analyzing and determining the collected product by using gas chromatography.
And (3) analyzing an experimental result: as shown in the gas chromatogram of fig. 4, it can be seen that the discharge products include: hydrogen, carbon monoxide, carbon dioxide, C 2 A compound is provided. As a result, it was found that the methane conversion was 93.5%; the flow rate of the hydrogen is 1.50L/min; the hydrogen selectivity was 65.8%; the carbon selectivity was 55.8%; the hydrogen production energy efficiency is 1.24mmol/kJ; it is worth emphasizing that no macroscopic soot formation occurred in all examples.
Example 2:
the only difference from example 1 is that the microwave input power is 1200W, and the rest of the experimental procedures and experimental parameters are the same as those of example 1.
And (3) analyzing an experimental result: the methane conversion was 94.9%; the hydrogen flow is 1.93L/min; hydrogen selectivity was 75.1% and carbon selectivity was 68.8%; the energy efficiency of hydrogen production is 1.20mol/kJ.
Example 3:
the only difference from example 1 is that the aqueous solution used was a sodium chloride solution, wherein the conductivity of the sodium chloride solution was 3300. Mu.s/cm, and the remaining experimental procedures and experimental parameters were the same as those of example 1.
And (3) analyzing an experimental result: the methane conversion rate is 75.63%; the hydrogen flow is 2.21L/min; the hydrogen selectivity was 74.36% and the carbon selectivity was 74.03%; the energy efficiency of hydrogen production is 1.82mmol/kJ.
Example 4:
the difference from example 1 is that the nitrogen purge is performed only before the discharge experiment, and the rest of the experimental steps and experimental parameters are the same as those of example 1.
And (3) analysis of experimental results: the methane conversion rate is 89.16%; the hydrogen flow is 1.77L/min; the hydrogen selectivity was 75.0% and the carbon selectivity was 66.5%; the energy efficiency of hydrogen production is 1.65mmol/kJ.
Example 5:
the only difference from example 1 is that the pH was adjusted to 3.37 by adding an appropriate amount of phosphoric acid to deionized water, and the rest of the experimental procedures and experimental parameters were the same as those of example 1.
And (3) analyzing an experimental result: the methane conversion rate is 91.56%; the hydrogen flow rate is 1.87L/min; the hydrogen selectivity was 76.0% and the carbon selectivity was 68.0%; the energy efficiency of hydrogen production is 1.54mmol/kJ.
Example 6:
the only difference from example 1 is that the appropriate amount of sodium persulfate, the oxidizing agent, was added to deionized water and the remaining experimental procedures and experimental parameters were the same as those of example 1.
And (3) analyzing an experimental result: the methane conversion was 94.12%; the hydrogen flow rate is 1.96L/min; the hydrogen selectivity was 76.3% and the carbon selectivity was 71.6%; the energy efficiency of hydrogen production is 1.62mmol/kJ.
Comparative example 1 (dielectric Barrier discharge plasma)
A gas-phase methane wet reforming experiment is carried out in a tunable ferroelectric packed bed dielectric barrier discharge reactor, and the discharge conditions are as follows: CH (CH) 4 ∶H 2 O=2∶1,CH 4 The flow rate was 4.5cm 3 /min,H 2 O flow rate of 9.0cm 3 Min; the discharge frequency is 500Hz, the electrode spacing is 3mm, and the size of the ferroelectric core block is 0.5-2mm.
And (3) analyzing an experimental result: the methane conversion rate is 15.9%; the energy efficiency of hydrogen production is 0.19mmol/kJ.
Comparative example 2 (DC spark discharge plasma)
A methane reforming experiment is carried out in a direct current spark discharge reaction system, and the discharge conditions are as follows: CH (CH) 4 The flow rate is 50mL/min, the discharge current is 10mA, the discharge voltage is 2kV, and the discharge power is 20W.
And (3) analyzing an experimental result: the methane conversion rate is 44.41%, the hydrogen production flow is 43.62mL/min, and the hydrogen selectivity is 98.21%.
Comparative example 3 (sliding arc discharge plasma)
Water vapor and CH were carried out in a gliding arc discharge plasma reactor 4 And CO 2 Study of composite reforming. The applied power is 80W, CH 4 And CO 2 The total flow rate of (A) is kept constant and is 360SCCM 4 /CO 2 /H 2 The ratio of O was 1/1.5/0.58.
And (3) analysis of experimental results: the methane conversion rate is 55%; the conversion rate of carbon dioxide is 43 percent, and the hydrogen flow rate is 1.93L/min; the hydrogen selectivity was 65.2% and the carbon selectivity was 32.9%.
Table 1: experimental result parameters of examples and comparative examples
Figure BDA0003404945180000081
As can be seen from table 1, compared with the gas-phase discharged methane reforming performance in the comparative example, the liquid-phase discharged methane reforming in the example not only ensures a higher methane conversion rate, but also achieves better hydrogen production efficiency.
To sum up, the novel discharge electrode and microwave liquid phase plasma reforming methane hydrogen production device that this application provided simple structure, easy operation, thereby its whole reaction process can directly go on in aqueous solution has practiced thrift the energy consumption to in the reforming process, it can realize high-efficient discharge in broad operating pressure and different kinds of aqueous solution. The device is used for preparing hydrogen by reforming methane with plasma, and can effectively solve the problems that the existing reforming hydrogen preparation process needs to be carried out at high temperature and high pressure, carbon deposition is easily generated, and discharge is unstable and the like.
Finally, it should be noted that: the above embodiments are only used to illustrate the technical solution of the present invention, and not to limit the same; while the invention has been described in detail and with reference to the foregoing embodiments, it will be understood by those skilled in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some or all of the technical features may be equivalently replaced; and the modifications or the substitutions do not make the essence of the corresponding technical solutions depart from the scope of the technical solutions of the embodiments of the present invention.

Claims (7)

1. A device for preparing hydrogen by reforming methane with microwave liquid-phase plasma is characterized by comprising a discharge electrode (4), a raw material tank (8), a water pump (13), a microwave generator (12), a waveguide tube (9), a sleeve (10), a reactor (5), a vacuum pump (15), a gas collecting device (14) and a condensing device (16); methane gas (1) tangentially enters the reactor (5) from the discharge electrode (4) through an air inlet pipeline (2), and a gas flowmeter (3) is arranged on the air inlet pipeline (2);
one end of the waveguide tube (9) is connected with the microwave generator (12); the sleeve (10) is vertically fixed at the lower part of the waveguide tube (9), the reactor (5) vertically penetrates through the upper part of the waveguide tube (9) and is nested in the sleeve (10), and the discharge electrode (4) is arranged in the sleeve (10) and is completely immersed in liquid;
the water suction pump (13) is arranged in the raw material tank (8), and the top of the raw material tank (8) is connected with a vacuum pump (15) and a gas collecting device (14);
a liquid inlet pipeline (6) and a first gas outlet pipeline (7) are arranged between the reactor (5) and the raw material tank (8), a second gas outlet pipeline (11) is connected with the raw material tank (8) and a condensing device (16), and a third gas outlet pipeline (17) is connected with the condensing device and a gas collecting device (14);
the discharge electrode (4) comprises an electrode (4-2), a boron nitride base (4-3) and a boron nitride side wall tube (4-1), the electrode (4-2) is arranged in the boron nitride side wall tube (4-1), and the electrode (4-2) is fixed on the boron nitride base (4-3);
the height of the electrode (4-2) is larger than that of the boron nitride side wall pipe (4-1), and the relative distance between the electrode (4-2) and the boron nitride side wall pipe (4-1) can be adjusted through the boron nitride base (4-3);
the top of the electrode (4-2) is sharpened, and the boron nitride base (4-3) is provided with a plurality of symmetrical hole-shaped structures to ensure that methane gas uniformly flows into the reactor (5).
2. The device for producing hydrogen by reforming methane through microwave liquid-phase plasma according to claim 1, wherein the electrode (4-2) is any one of a tungsten rod, a copper rod and a stainless steel rod.
3. The method for producing hydrogen by reforming methane based on the device for producing hydrogen by reforming methane by microwave liquid-phase plasma according to any one of claims 1 to 2, characterized by comprising the following steps:
s1, injecting methane gas (1) and an aqueous solution in a raw material tank (8) into a reactor (5), and fully mixing;
s2, carrying out pressure reduction treatment on the reactor (5) and the raw material tank (8) by using a vacuum pump (15);
s3: starting a microwave generator (12) to generate plasma at the tip of the electrode (4-2);
s4: the plasma acts on the methane and the water solution to generate hydrogen, and the hydrogen is collected and analyzed after being cooled by a raw material tank (8) and a condensing device (16).
4. A method for preparing hydrogen from methane through microwave liquid phase plasma reforming as claimed in claim 3, wherein in step S1, the feed flow rate of the methane gas is 0.1L/min-5.0L/min, the internal pressure of the reactor is 5-10kPa, and the volume of the aqueous solution injected into the reactor is 150-500mL.
5. The method for producing hydrogen by reforming methane through microwave liquid-phase plasma according to claim 3, wherein in step S1, the aqueous solution is one or more of deionized water, an aqueous sodium chloride solution, an acidic aqueous solution, an alkaline aqueous solution, and an aqueous alcohol solution.
6. The method for producing hydrogen by reforming methane through microwave liquid-phase plasma according to claim 3, wherein in the step S3, the microwave input power of the microwave generator (12) is 600-1200W.
7. The method for producing hydrogen by reforming methane through microwave liquid-phase plasma according to claim 3, wherein in step S1, one or more of nitrogen, argon, helium and carbon dioxide can be added into the methane gas as an auxiliary gas.
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