CN114984884A - Experimental platform for preparing fuel by reforming carbon dioxide with assistance of plasma synergistic catalyst - Google Patents

Abstract

The experimental platform of the plasma synergistic catalyst assisted carbon dioxide reforming to make fuel of the present invention includes a gas supply system, a dielectric barrier discharge reactor, a high-voltage power supply system and a product detection system. The dielectric barrier discharge reactor includes catalysts and fixtures, tangential air inlets, quartz tubes, external stainless steel electrodes, and built-in stainless steel electrodes. The external stainless steel electrode is tightly wrapped on the outer wall of the outer quartz flow tube, and the surface of the internal stainless steel electrode is covered with a second layer of quartz tube. Under the synergistic effect of plasma and catalyst, carbon dioxide will achieve efficient directional conversion of carbon dioxide; reaction gases such as carbon dioxide enter the reactor through two symmetrically tangentially tangential inlets on one side of the outer quartz flow tube. The swirling flow can effectively prolong the residence time of carbon dioxide in the plasma discharge area, and cause the discharge disturbance to enhance the discharge of the filaments on the wall of the quartz tube, thereby enhancing the effect of the electric field strength in the reaction area.

Description

Experimental Platform for Plasma Synergistic Catalyst Assisted Carbon Dioxide Reforming to Fuel

technical field

The invention belongs to the technical field of carbon dioxide catalytic reforming, and particularly relates to an experimental platform for a plasma-cooperated catalyst assisted carbon dioxide reforming to produce fuel.

Background technique

Carbon dioxide is the most important greenhouse gas responsible for global climate change, and the burning of fossil fuels is the largest source of carbon dioxide emissions. Over the past few decades, the use of fossil fuels has increased year by year, leading to a dramatic rise in carbon dioxide emissions. It is necessary to develop sustainable green energy and carbon dioxide emission approaches. In order to reduce carbon emissions, carbon capture and utilization technology is regarded as the most potential way to reduce carbon emissions. Carbon dioxide is turned into a recyclable fuel by a certain method.

The chemical properties of carbon dioxide are stable, and it is not easy to be converted in a mild environment, and the conversion rate under high temperature conditions is also very low. In recent years, non-equilibrium plasma has received attention as a new type of activation reaction technology. The content of high-energy electrons in this non-equilibrium plasma is high, and its electron energy can reach 1-10 eV. The strong electron energy can activate inert molecules and promote chemical reactions. Non-equilibrium plasma technology can break the conventional thermochemical reaction process and reduce the temperature required for the reaction through the interaction of high-energy electrons and active particles, thereby realizing the conversion of carbon dioxide under normal pressure and low temperature conditions.

There are many ways to generate plasma, such as radio frequency discharge, sliding arc discharge, microwave discharge and dielectric barrier _discharge . The synergistic effects of O ₃ , Fe-graphene, Ru-Al ₂ O ₃ and other advantages have shown a good prospect in the field of carbon dioxide reforming.

At present, in the research of plasma-assisted carbon dioxide conversion, it is difficult to achieve directional conversion due to the diversification of products; at the same time, due to the limitation of the structure and characteristics of dielectric barrier discharge, the utilization rate of energy is low and needs to be improved.

SUMMARY OF THE INVENTION

The purpose of the present invention is to improve the deficiencies of the existing experimental platform, and to provide an experimental platform for plasma-assisted catalyst-assisted carbon dioxide reforming to make fuel, specifically a low-temperature and high-efficiency conversion of carbon dioxide that can be realized under the dual action of plasma and catalyst. , and an experimental system for qualitative and quantitative analysis of the final product.

The present invention adopts the following technical scheme to realize:

An experimental platform for plasma co-catalyst-assisted carbon dioxide reforming to make fuel, the experimental platform includes a fuel supply system, a dielectric barrier discharge reactor, a high-voltage power supply system and a product detection system;

The fuel supply system is used to precisely supply reaction gases such as dilution gas and carbon dioxide; when there is liquid in the product, the pipeline is heated to realize liquid vaporization; during the experiment, the pressure required by the reactor is controlled, and the reaction generated gas discharge system;

The dielectric barrier discharge reaction system provides a reaction place for the temperature and pressure required for the experiment; two tangential air inlets are designed on one side of the reactor; and a catalyst is filled between the double-layer discharge structures; Provide a uniform plasma environment generated by the double dielectric barrier discharge structure;

The high-voltage power supply system is used to provide a continuous electric field for generating plasma, and to detect the voltage and current changes during the reaction;

The product detection system is used for collecting and detecting the products at the end of the reaction, so as to realize the diagnosis and analysis of the differential components in the carbon dioxide reforming process.

A further improvement of the present invention lies in that the fuel supply system includes reaction gas, mass flow meter and control software, heating belt, thermocouple and temperature controller, and micro-regulating valve;

The reaction gas and dilution gas are accurately controlled by the mass flow meter and control software, and then pass into the tangential air inlet of the reactor; under the control of the thermocouple and temperature controller, the heating belt is wrapped around the outside of the pipeline to realize the liquid product. Gasification; and control the amount of gas discharged into the atmosphere through a micro-regulating valve to maintain a constant pressure in the reaction system.

A further improvement of the present invention is that the dielectric barrier discharge reaction system includes an electric heating furnace, an outer quartz flow tube, a tangential air inlet, a sealing flange, an external stainless steel electrode, a built-in stainless steel rod electrode, and an inner electrode wrapped in the stainless steel rod. The inner quartz tube, catalyst and fixing device on the upper;

The entire reactor is placed in an electric heating furnace, which provides a controllable 10cm constant temperature area for the entire reaction system; two tangential air inlets are set on one side of the reactor, and the air inlets are flushed from the tangential direction. The incoming reaction gas such as carbon dioxide will form a gas flow spiraling around the central axis between the inner quartz tube and the outer quartz tube, prolonging the residence time of the reaction gas in the plasma area, providing discharge disturbance and enhancing the fineness of the quartz tube surface. wire discharge to enhance the electric field strength in the reaction zone; both ends of the reactor are sealed by sealing flanges combined with rubber sealing rings; external stainless steel electrodes, outer quartz flow tubes, inner quartz tubes and built-in stainless steel rod electrodes are maintained by four parts. Coaxiality, double-layer dielectric barrier discharge structure to ensure uniform plasma generation; corresponding catalysts are placed in the plasma discharge area of the reactor, and fixed with materials such as quartz wool; the shaft is opened on both sides of the sealing flange The built-in stainless steel rod electrode is connected to the power supply, and another hole is opened on the flange side of the gas outlet direction for gas outlet.

A further improvement of the present invention lies in that, between the quartz tubes of the outer layer and the inner layer, a synergistic effect is formed with the plasma to improve the conversion rate of carbon dioxide and the overall energy utilization rate.

A further improvement of the present invention is that the double-layered quartz tube can generate a uniform electric field.

A further improvement of the present invention is that the two tangential air inlets extend the residence time of the reactant gas in the plasma area, enhance the disturbance and enhance the discharge of the filaments on the surface of the quartz tube, and enhance the electric field strength in the reaction area.

A further improvement of the present invention is that the electric heating furnace can provide the initial reaction conditions of 298K-1273K for the reaction.

A further improvement of the present invention is that the high-voltage power supply system includes a high-voltage power supply, a high-voltage probe, a current probe and an oscilloscope;

The positive and negative electrodes of the high-voltage power supply are respectively connected to the external stainless steel electrode and the built-in stainless steel rod electrode. The voltage and current generated during the discharge process are detected by the high-voltage probe and the current probe, and displayed on the oscilloscope.

A further improvement of the present invention is that the experimental platform does not limit the discharge mode of the high-voltage power supply, and both high-voltage alternating current and high-voltage nanosecond pulse power supply can be used.

A further improvement of the present invention is that the product detection system includes a gas chromatograph, a gas chromatograph/mass spectrometer and a computer control system;

The product is vaporized by the heating belt outside the pipeline and then enters the gas chromatograph and the gas chromatograph/mass spectrometer, and carries out differential diagnosis and display under the control of the computer control system.

The present invention at least has the following beneficial technical effects:

(1) The present invention can be used to realize efficient directional conversion of carbon dioxide in an environment where plasma and catalysts are synergized, and improve the utilization rate of energy while improving carbon dioxide;

(2) The dielectric barrier discharge reaction zone of the present invention does not limit the catalyst used in the experiment, and catalysts such as Ni-Al ₂ O ₃ , Fe-graphene, Ru-Al ₂ O ₃ and the like can be used;

(3) The double-layer dielectric barrier discharge system of the present invention can obtain non-equilibrium plasma with larger energy density, avoid the formation of thermal plasma, and is more conducive to uniform discharge to form a more uniform non-equilibrium plasma;

(4) the tangential air inlet of the quartz flow tube of the present invention prolongs the residence time of the reaction gas in the plasma zone, and strengthens the disturbance, and enhances the discharge of the filaments on the surface of the quartz tube, thereby enhancing the electric field strength in the reaction zone;

(5) The experimental platform of the present invention does not limit the discharge mode of the high-voltage power supply, and both high-voltage alternating current and high-voltage nanosecond pulse power supply can be used.

Description of drawings

FIG. 1 is a schematic structural diagram of an experimental platform for the plasma synergistic catalyst-assisted carbon dioxide reforming to make fuel according to the present invention.

2 and 3 are schematic diagrams of the detailed structure of the dielectric barrier discharge reactor.

Description of reference numbers:

1- Reaction gas, 2- Mass flow meter and control software, 3- Heating belt, 4- Thermocouple and temperature controller, 5- Micro-control valve, 6- Electronic pressure gauge, 7- Electric heating furnace, 8- Outer layer Quartz flow tube, 9-tangential gas inlet, 10-sealing flange, 11-external stainless steel electrode, 12-internal stainless steel electrode, 13-inner quartz tube, 14-catalyst and fixture, 15-oscilloscope, 16 -Voltage probe, 17-Current monitoring ring, 18-High voltage power supply, 19-Gas chromatograph, 20-Gas chromatography/mass spectrometer, 21-Computer control system.

Detailed ways

Exemplary embodiments of the present disclosure will be described in more detail below with reference to the accompanying drawings. While exemplary embodiments of the present disclosure are shown in the drawings, it should be understood that the present disclosure may be embodied in various forms and should not be limited by the embodiments set forth herein. Rather, these embodiments are provided so that the present disclosure will be more thoroughly understood, and will fully convey the scope of the present disclosure to those skilled in the art. It should be noted that the embodiments of the present invention and the features of the embodiments may be combined with each other under the condition of no conflict. The present invention will be described in detail below with reference to the accompanying drawings and in conjunction with the embodiments.

As shown in FIG. 1 to FIG. 3 , the experimental platform of the plasma synergistic catalyst-assisted carbon dioxide reforming to make fuel provided by the present invention includes a gas supply system, a dielectric barrier discharge reaction system, a high-voltage power supply system and a product detection system; the gas supply system, It is used to accurately supply dilution gas and carbon dioxide reaction gas, heat the pipeline when there is liquid in the product to realize liquid vaporization, and control the pressure required by the entire reaction system during the experiment; dielectric barrier discharge reaction system, used to provide laboratory The reaction site of the required temperature and pressure, two opposite tangential air inlets are designed on one side of the reactor, and the catalyst is filled between the double-layer dielectric barrier discharge structure, and at the same time, the uniformity produced by the double-layer dielectric barrier discharge structure is provided. The non-equilibrium plasma environment; the high-voltage power supply system is used to provide a continuous electric field for generating plasma and monitor the voltage and current changes during the reaction; the product detection system is used to collect and detect the products at the end of the reaction to realize the carbon dioxide reforming process Determination and analysis of middle and differential components.

The fuel supply system includes reaction gas 1 , mass flow meter and control software 2 , heating belt 3 , thermocouple and temperature controller 4 , micro-regulating valve 5 and electronic pressure gauge 6 .

The reaction gas 1 and the dilution gas pass into the tangential air inlet of the reactor after being precisely controlled by the mass flow meter and the control software 2. Under the control of the thermocouple and the temperature controller 4, the heating belt 3 heats the pipeline to the specified temperature. The control of the reaction temperature and the gas of the liquid product are realized, and the corresponding gas volume is controlled by the micro-adjustment valve 5 and the electronic pressure gauge 6 to maintain the constant pressure in the reaction system.

The main structure of the reactor in the dielectric barrier discharge system is an electric heating furnace 7, an outer quartz flow tube 8, a tangential air inlet 9, a sealing flange 10, an external stainless steel electrode 11, a built-in stainless steel electrode 12, and an inner quartz tube. 13. Catalyst and fixture 14. Catalysts such as Ni-Al ₂ O ₃ , Fe-graphene, Ru-Al ₂ O ₃ etc. can be used.

The whole reactor is placed in the electric heating furnace 7; one side of the reactor is provided with two tangential tangential gas inlets 9, and the carbon dioxide reaction gas entering from the tangential tangential gas inlet will form the inner layer quartz tube 13 and the outer layer. The gas flow spiraling around the central axis between the layers of quartz flow tubes 8 prolongs the residence time of the reaction gas in the plasma area, provides discharge disturbance, enhances the discharge of filaments on the surface of the quartz tube, and enhances the electric field strength in the reaction zone; The four parts of the stainless steel electrode 11, the outer quartz flow tube 8, the inner quartz tube 13 and the built-in stainless steel electrode 12 are kept coaxial, and the double-layer dielectric barrier discharge structure ensures the generation of uniform non-equilibrium plasma; the plasma in the reactor Corresponding catalysts are placed in the body discharge area and fixed with quartz wool material; holes are opened on both sides of the sealing flange 10, and the built-in stainless steel electrodes are drawn out and connected to the power supply, and another hole is opened on the flange side in the air outlet direction for Exhale.

After there are two layers of quartz tubes between the discharge electrodes, a double-layer dielectric barrier discharge system is formed, which can obtain non-equilibrium plasma with high energy density, avoid the formation of thermal plasma, and is more conducive to uniform discharge; the reaction system contains A tangential air inlet 9 is provided to prolong the residence time of the reaction gas in the plasma area, and to strengthen the disturbance and the discharge of the filaments on the surface of the quartz tube, thereby enhancing the electric field strength in the reaction area and improving the utilization rate of electric energy.

The high-voltage power supply system includes a high-voltage power supply 18, a voltage probe 16, a current monitoring ring 17 and an oscilloscope 15; the positive and negative electrodes of the high-voltage power supply 18 are respectively connected to external stainless steel electrodes and built-in stainless steel electrodes. The voltage and current changes generated during the discharge process are determined by The voltage probe 16 and the current monitoring loop 17 are detected and displayed on the oscilloscope 15 .

In the power supply system, the high-voltage power supply 18 can be easily replaced. According to different research requirements, high-voltage alternating current and high-voltage nanosecond pulse power can be used in the experimental platform.

The product detection system is composed of a gas chromatograph 19, a gas chromatograph/mass spectrometer 20, and a computer control system 21, and the product enters the gas chromatograph 19 and the gas chromatograph/mass spectrometer 20 after being vaporized by the heating belt 3 outside the pipeline. , carry out differential determination and display under the control of computer control system 21, and each group of experiments is repeated more than three times to ensure the accuracy of experimental results.

The operation mode of the experimental platform of the plasma synergistic catalyst assisted carbon dioxide reforming to make fuel of the present invention is specifically as follows: the carbon dioxide and other reactors and the dilution gas enter the dielectric barrier discharge reactor through the tangential air inlet on the quartz flow tube, open the The high-voltage power supply selects the discharge method required by the research; the reaction gas rotates around the central axis of the reactor, passes through the plasma discharge area and the catalyst, and flows to the outlet of the reactor. detection.

The concrete working process of the present invention is as follows:

(1) First, the electric heating furnace and the heating belt are heated to the temperature conditions set by the experiment;

(2) The reaction gas precisely controls and sets the intake air volume through the mass flow meter and control software, and enters the outer quartz flow tube through the two hedged tangential intake ports to form a swirling flow, and use a micro-control valve to adjust the air flow in the reactor. Air pressure state, the pressure in the device is detected and displayed by an electronic pressure gauge;

(3) Then, by setting the discharge parameters of the discharge power supply, a voltage is applied between the external stainless steel electrode and the built-in stainless steel electrode to start the discharge, and the discharge voltage and discharge current are respectively detected by the voltage probe and the current monitoring ring and displayed on the oscilloscope;

(4) After the discharge process is stable, the reacted gas is passed into a gas chromatograph and a gas chromatograph/mass spectrometer to measure the product components, and the detection results are fed back to the computer control system. Through the analysis of the experimental data, the chemical reaction kinetic characteristics of carbon dioxide in the process of carbon dioxide conversion under different boundary conditions can be obtained, and the most suitable conditions for carbon dioxide conversion and optimal energy utilization can be explored according to the results.

Although the present invention has been described in detail above with general description and specific embodiments, it is obvious to those skilled in the art that some modifications or improvements can be made on the basis of the present invention. Therefore, these modifications or improvements made without departing from the spirit of the present invention fall within the scope of the claimed protection of the present invention.

Claims (10)

1. The experimental platform for preparing the fuel by reforming the carbon dioxide under the assistance of the plasma and the catalyst is characterized by comprising an air supply system, a dielectric barrier discharge reaction system, a high-voltage power supply system and a product detection system;

the gas supply system is used for accurately supplying diluent gas and carbon dioxide reaction gas, heating the pipeline when liquid exists in the product so as to realize liquid vaporization, and controlling the pressure required by the whole reaction system in the experiment process;

the dielectric barrier discharge reaction system is used for providing a reaction site of temperature and pressure required by an experiment, two opposite impact tangential air inlets are designed on one side of the reactor, a catalyst is filled between the double-layer dielectric barrier discharge structures, and a uniform non-equilibrium plasma environment generated by the double-layer dielectric barrier discharge structures is provided;

the high-voltage power supply system is used for providing a continuous electric field for generating plasma and monitoring the voltage and current change during reaction;

and the product detection system is used for collecting and detecting the product after the reaction is finished, and realizing the determination and analysis of differential components in the carbon dioxide reforming process.

2. The experimental platform for preparing fuel by reforming carbon dioxide under the assistance of plasma synergistic catalyst of claim 1, wherein the fuel supply system comprises reaction gas, a mass flow meter, control software, a heating belt, a thermocouple, a temperature controller and a micro-regulating valve;

reaction gas and diluent gas are introduced into a tangential gas inlet of the reactor after being accurately controlled by a mass flow meter and control software, the pipeline is heated to a specified temperature by a heating belt under the regulation and control of a thermocouple and a temperature controller, the control of the reaction temperature and the gas of a liquid product are realized, and the corresponding gas is discharged by controlling a micro-regulating valve so as to maintain the constant pressure in the reaction system.

3. The experimental platform for preparing fuel by reforming carbon dioxide under the assistance of plasma and a catalyst according to claim 1, wherein the dielectric barrier discharge reaction system comprises an electric heating furnace, an outer-layer quartz flow tube, a tangential air inlet, an external stainless steel electrode, an internal stainless steel electrode, an inner-layer quartz tube coated on the stainless steel electrode, a catalyst and a fixing device;

the whole reactor is placed in an electric heating furnace; two opposite-impact tangential air inlets are arranged on one side of the reactor, and carbon dioxide reaction gas entering from the tangential opposite-impact air inlets can form airflow spirally advancing around a central axis between the inner-layer quartz tube and the outer-layer quartz flow tube, so that the detention time of the reaction gas in a plasma region is prolonged, discharge disturbance is provided, filament discharge on the surface of the quartz tube is enhanced, and the electric field intensity in a reaction region is enhanced; the external stainless steel electrode, the outer quartz flow tube, the inner quartz tube and the internal stainless steel electrode are coaxial, and the double-layer dielectric barrier discharge structure ensures that uniform non-equilibrium plasma is generated; placing corresponding catalyst, such as Ni-Al, in the plasma discharge region of the reactor ₂ O ₃ Fe-graphene, Ru-Al ₂ O ₃ And the like, and the quartz cotton material is used for fixing; holes are formed in the axes of two sides of the sealing flange, the built-in stainless steel electrode is led out to be connected with a power supply, and a hole is formed in the flange side in the air outlet direction for air outlet.

4. The experimental platform for preparing fuel by reforming carbon dioxide with the assistance of plasma and catalyst as claimed in claim 3, wherein the electric heating furnace provides a constant temperature area of 100mm for the whole reaction system.

5. The experimental platform for preparing fuel by reforming carbon dioxide with the assistance of the plasma and the catalyst as claimed in claim 3, wherein two ends of the reactor are sealed by sealing flanges combined with rubber sealing rings.

6. The experimental platform for preparing fuel by reforming carbon dioxide with the assistance of the plasma and the catalyst as claimed in claim 3, wherein the double-layer quartz tube can generate a more uniform electric field, so as to generate a more uniform non-equilibrium plasma region.

7. The experimental platform for preparing fuel by reforming carbon dioxide with the assistance of the plasma synergistic catalyst according to claim 3, wherein the two opposite tangential air inlets prolong the residence time of the reaction gas in the plasma zone and enhance the filament discharge on the surface of the turbulence-enhanced quartz tube, thereby enhancing the electric field intensity in the reaction zone.

8. The experimental platform for preparing fuel by reforming carbon dioxide with the assistance of plasma synergistic catalyst as claimed in claim 3, characterized in that, the electric heating furnace can provide a wider initial temperature condition of 298K-1273K for the reaction.

9. The experimental platform for preparing fuel by reforming carbon dioxide under the assistance of the plasma synergistic catalyst according to claim 3, wherein the power supply system of the high-voltage power supply comprises a high-voltage power supply, a voltage probe, a current monitoring ring and an oscilloscope;

the positive electrode and the negative electrode of the high-voltage power supply are respectively connected with the external stainless steel electrode and the internal stainless steel electrode, and the voltage and current changes generated in the discharging process are detected by the voltage probe and the current monitoring ring and are displayed on the oscilloscope.

10. The experimental platform for preparing fuel by reforming carbon dioxide under the assistance of plasma synergistic catalyst of claim 1, wherein the product detection system comprises a gas chromatograph, a gas chromatograph/mass spectrometer and a computer control system;

and gasifying the product through a heating belt arranged outside the pipeline, then feeding the gasified product into a gas chromatograph and a gas chromatograph/mass spectrometer, carrying out differential measurement and displaying under the control of a computer control system, and repeating each group of experiments for more than three times to ensure the accuracy of the experimental result.

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