High-voltage pulse discharge photo-thermal synergistic catalytic reaction device and reaction method

Abstract

This invention discloses a high-voltage pulsed discharge photothermal synergistic catalytic reaction device and method, comprising a shell structure, a heating mechanism, a light source, and a high-voltage electric field mechanism. The shell structure includes an outer shell and an inner shell, with an outer chamber formed between the inner and outer shells. A sample chamber is located inside the inner shell, and a sample fixing stage is located below the sample chamber. An upper connecting pipe is connected to the upper end of the inner shell, and a lower connecting pipe is connected to the lower end of the inner shell. Both the upper and lower connecting pipes have pressure-balancing holes communicating with the outer chamber. The heating mechanism includes a heating tube. The light source is mounted on the outer shell and illuminates the sample chamber. The high-voltage electric field mechanism includes a power supply, a positive electrode, and a negative electrode. The lower end of the positive electrode is located at the upper end of the sample chamber, and the upper end of the negative electrode is located at the lower end of the sample chamber. This invention can fully utilize the advantages of photothermal and electro-catalytic synergy under different gas pressures, significantly improving gas conversion efficiency. It has a wide range of applications, is simple to operate, and has broad application prospects.

Description

Technical Field

[0001] This invention belongs to the technical field of chemical reaction devices, specifically relating to a high-voltage pulse discharge photothermal synergistic catalytic reaction device and reaction method. Background Technology

[0002] In fields such as organic synthesis and catalysis, reaction rate, product yield, and selectivity are crucial indicators for evaluating reaction effectiveness. Currently, most commonly used chemical reaction methods employ traditional thermodynamic approaches, controlling the reaction process using thermodynamic parameters such as temperature and pressure. While these methods can achieve good results in certain situations, they suffer from slow reaction rates, poor selectivity, and also lead to environmental pollution and energy waste, hindering sustainable development.

[0003] To overcome the problems of traditional chemical reaction methods, many novel chemical reaction methods have been proposed in recent years. These include methods that utilize various external stimuli such as light, electricity, sound, magnetism, and microwaves to promote reactions, or methods that use nanotechnology and catalysts to achieve highly efficient reactions. While these novel reaction methods have significant advantages in some aspects, they still possess certain limitations and drawbacks. Summary of the Invention

[0004] To address the aforementioned technical problems, this invention proposes a high-voltage pulsed discharge photothermal synergistic catalytic reaction device and method. During the reaction, multiple forces—light, electricity, heat, and pressure—are simultaneously applied to achieve high efficiency and selectivity in the chemical reaction. In the photocatalytic process, some photogenerated electrons and holes migrate to the catalyst surface and then recombine; some of these electrons and holes recombine directly within the semiconductor; others migrate to the semiconductor surface and are absorbed by electron or hole acceptors, leading to reduction or oxidation, respectively. An external electric field is introduced into the photocatalytic process. The potential generated by this field is applied to the photocatalytic catalyst, promoting the separation of photogenerated carriers. Simultaneously, heat and pressure positively drive the reaction.

[0005] To achieve the above objectives, the technical solution adopted by the present invention is: a high-voltage pulsed discharge photothermal synergistic catalytic reaction device, comprising a shell structure, a heating mechanism, a light source, and a high-voltage electric field mechanism;

[0006] The housing mechanism includes an outer shell and an inner shell. The inner shell is located inside the outer shell, and an outer cavity is formed between the inner shell and the outer shell. A sample chamber is provided inside the inner shell, and a sample fixing stage is provided below the sample chamber. An upper connecting pipe is connected to the upper end of the inner shell, and the upper connecting pipe extends out of the outer shell. A lower connecting pipe is connected to the lower end of the inner shell, and the lower connecting pipe extends out of the outer shell. A pressure-balancing hole communicating with the outer cavity is provided on the upper connecting pipe and the lower connecting pipe, respectively.

[0007] The heating mechanism includes a heating tube, which is mounted on the outer casing.

[0008] The light source is mounted on the outer shell and shines directly into the sample chamber, while the portion of the inner shell corresponding to the sample chamber is transparent.

[0009] The high-voltage electric field mechanism includes a power source, a positive electrode, and a negative electrode. The positive electrode and the negative electrode are respectively connected to the power source and are arranged opposite to each other. The lower end of the positive electrode extends into the inner shell and is located at the upper end of the sample chamber, while the upper end of the negative electrode extends into the inner shell and is located at the lower end of the sample chamber.

[0010] As a preferred embodiment of the above technical solution, the outer casing includes an upper cover and a lower cover. An upper connecting pipe is installed in the middle of the upper cover. The upper end of the upper connecting pipe is located outside the outer casing and is connected to an upper tee pipe. The upper tee pipe includes an upper main pipe and an upper side pipe. The lower end of the upper main pipe is fixedly connected to the upper end of the upper connecting pipe. The positive electrode is inserted into the upper main pipe from the upper end of the upper main pipe and extends through the upper connecting pipe to the upper end of the sample chamber. An air inlet is provided on the upper side pipe. A lower connecting pipe is installed in the middle of the lower cover. The lower end of the lower connecting pipe is located outside the outer casing and is connected to a lower tee pipe. The lower tee pipe includes a lower main pipe and a lower side pipe. The lower end of the lower main pipe is fixedly connected to the lower end of the lower connecting pipe. The negative electrode is inserted into the lower main pipe from the lower end of the lower main pipe and extends through the lower connecting pipe to the lower end of the sample chamber. An air outlet is provided on the lower side pipe.

[0011] As a preferred embodiment of the above technical solution, the inner shell is made of quartz glass.

[0012] As a preferred embodiment of the above technical solution, a thermometer for measuring the temperature of the outer chamber and the sample chamber is installed on the outer shell, and the thermometer is positioned opposite to the light source.

[0013] As a preferred embodiment of the above technical solution, the wavelength of the light source is 300-2500nm and the power is 100-350W.

[0014] As a preferred embodiment of the above technical solution, the light source is mounted on the lampshade, the lampshade is fixed to the outer shell, the front end of the lampshade extends into the outer cavity, and a focuser is installed on the front end of the lampshade.

[0015] As a preferred embodiment of the above technical solution, ceramic insulating tubes are respectively fitted onto the positive electrode and the negative electrode.

[0016] As a preferred embodiment of the above technical solution, the output voltage of the high-voltage electric field mechanism is 0-30kV.

[0017] As a preferred embodiment of the above technical solution, the outer shell has an internal interlayer, and the heating tube is installed in the interlayer.

[0018] The high-voltage pulsed discharge photothermal synergistic catalytic reaction method, using the aforementioned high-voltage pulsed discharge photothermal synergistic catalytic reaction apparatus, includes the following steps:

[0019] Step 1: Place the catalyst on the sample stage, turn on the heating tube, control the temperature in the sample chamber within a certain range, and then introduce the reactants into the sample chamber.

[0020] Step 2: Turn on the light source. The light source shines through the inner shell onto the sample chamber, generating a photoelectric effect in the sample chamber, which causes the reactants to be electronically excited and converted into an active state.

[0021] Step 3: Turn on the high-voltage electric field mechanism to apply the electric field to both ends of the sample chamber with the required voltage and holding time;

[0022] Step 4: Control the flow rate of the reactants to increase the pressure of the reactants in the sample chamber, thereby shortening the distance between the reactants to increase the interaction force and promote the reaction.

[0023] Step 5: Maintain the reaction temperature, light intensity, and voltage to ensure the reactants in the container achieve the best reaction effect. Adjust the reaction time as needed and carry the reaction to completion.

[0024] Step 6: Separate the high-voltage pulse discharge photothermal synergistic catalytic reaction products.

[0025] The beneficial effects of this invention are as follows: This invention achieves catalytic reaction through photothermal-electric synergy while simultaneously altering gas pressure. In particular, it utilizes high-voltage pulsed discharge to generate plasma, which can instantaneously release energy, promoting redox reactions in the gas and thus improving gas conversion efficiency. Compared to traditional photocatalytic methods, the photothermal-pressure synergistic reaction method proposed in this invention has advantages such as fast reaction speed, high reaction efficiency, and good selectivity of reaction products. The reaction device of this invention can be manufactured by changing the size of its components; small-scale versions can be used for laboratory experiments, while large-scale versions can be applied to industrial production, thus making it suitable for different working environments. Attached Figure Description

[0026] Figure 1 This is a schematic diagram of the structure of the present invention;

[0027] Figure 2 A comparison chart of carbon dioxide conversion rates under different conditions. Detailed Implementation

[0028] The technical solution of the present invention will now be clearly and completely described with reference to the accompanying drawings. Obviously, the described embodiments are only some, not all, of the embodiments of the present invention. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0029] In the description of this invention, it should be noted that the terms "center," "upper," "lower," "left," "right," "vertical," "horizontal," "inner," and "outer," etc., indicate the orientation or positional relationship based on the orientation or positional relationship shown in the accompanying drawings. They are used only for the convenience of describing the invention and for simplifying the description, and do not indicate or imply that the device or element referred to must have a specific orientation, or be constructed and operated in a specific orientation. Therefore, they should not be construed as limitations on the invention. Furthermore, the terms "first," "second," and "third" are used for descriptive purposes only and should not be construed as indicating or implying relative importance.

[0030] In the description of this invention, it should be noted that, unless otherwise explicitly specified and limited, the terms "installation," "connection," and "linking" should be interpreted broadly. For example, they can refer to a fixed connection, a detachable connection, or an integral connection; they can refer to a mechanical connection or an electrical connection; they can refer to a direct connection or an indirect connection through an intermediate medium; and they can refer to the internal connection of two components. Those skilled in the art can understand the specific meaning of the above terms in this invention based on the specific circumstances.

[0031] like Figure 1 As shown, the high-voltage pulsed discharge photothermal synergistic catalytic reaction device includes a shell structure, a heating mechanism, a light source 10, and a high-voltage electric field mechanism;

[0032] The housing mechanism includes an outer shell 1 and an inner shell 2. The inner shell 2 is located inside the outer shell 1, forming an outer chamber 3 between the inner shell 2 and the outer shell 1. A sample chamber 4 is located inside the inner shell 2, and a sample fixing stage 5 is located below the sample chamber 4. An upper connecting pipe 6 is connected to the upper end of the inner shell 2, extending outside the outer shell 1. A lower connecting pipe 7 is connected to the lower end of the inner shell 2, extending outside the outer shell 1. Both the upper connecting pipe 6 and the lower connecting pipe 7 have pressure-balancing holes 8 that communicate with the outer chamber 3. A sandwich layer 26 is provided inside the outer shell 1. The heating mechanism includes a heating tube 9, which is installed in the sandwich layer 26. The outer shell 1 consists of an outer shell and an inner shell, forming a sandwich layer 26 between them. The thickness of the outer shell and the inner shell is 0.5 mm, the distance between them is 6 mm, and the diameter of the heating tube 9 is 1 mm. The upper cover 11 and the lower cover 12 are the same size, with an outer diameter of 56 mm and a thickness of 4 mm. The light source 10 is mounted on the outer shell 1 and illuminates the sample chamber 4. The portion of the inner shell 2 corresponding to the sample chamber 4 is transparent. The wavelength of the light source 10 is 300-2500nm, and the power is 100-350W. The high-voltage electric field mechanism includes a power supply 11, a positive electrode 12, and a negative electrode 13. The positive electrode 12 and the negative electrode 13 are respectively connected to the power supply 11 and are arranged opposite to each other. The lower end of the positive electrode 12 is pointed and extends into the inner shell 2, located at the upper end of the sample chamber 4. The upper end of the negative electrode 13 is pointed and extends into the inner shell 2, located at the lower end of the sample chamber 4. The power supply 11 is a high-voltage pulse power supply. Ceramic insulating tubes 25 are respectively fitted onto the positive electrode 12 and the negative electrode 13.

[0033] Furthermore, the outer casing 1 includes an upper cover 14 and a lower cover 15. An upper connecting pipe 6 is installed in the middle of the upper cover 14. The upper end of the upper connecting pipe 6 is located outside the outer casing 1 and connected to an upper tee pipe. The upper tee pipe includes an upper main pipe 16 and an upper side pipe 17. The lower end of the upper main pipe 16 is fixedly connected to the upper end of the upper connecting pipe 6. The positive electrode 12 is inserted into the upper main pipe 16 from its upper end, passes through the upper connecting pipe 6, and extends into the upper end of the sample chamber 4. The upper side... The tube 17 has an air inlet 18. The lower connecting tube 7 is installed in the middle of the lower cover 15. The lower end of the lower connecting tube 7 is located outside the outer shell 1 and is connected to a lower tee pipe. The lower tee pipe includes a lower main tube 19 and a lower side tube 20. The lower end of the lower main tube 19 is fixedly connected to the lower end of the lower connecting tube 7. The negative electrode 13 is inserted into the lower main tube 19 from the lower end and passes through the lower connecting tube 7 before extending into the lower end of the sample chamber 4. The lower side tube 20 has an air outlet 21. The inner shell 2 is made of quartz glass. The quartz glass is 0.5 mm thick and 200 mm long. The sample chamber is 42 mm long and has an inner diameter of 14 mm. The diameter of the sample chamber 4 is increased at the bottom, with the wider part having a diameter of 34 mm. The sample fixing stage 5 has a diameter of 30 mm and a height of 4 mm. The sample fixing stage 5 is located in the wider part and close to the sample chamber 4. A thermometer 22 for measuring the temperature of the outer chamber 3 and the sample chamber 4 is installed on the outer casing 1. The thermometer 22 is positioned opposite the light source 10. The thermometer 22 is an infrared thermometer with a temperature response time of 0.1-1s, a temperature range of 0-1500℃, and an accuracy of +1℃. The light source 10 is mounted on a lampshade 23, which is fixed to the outer casing 1. The front end of the lampshade 23 extends into the outer chamber 3, and a focuser 24 is installed at the front end of the lampshade 23.

[0034] The gas catalytic reaction process using the apparatus of this embodiment is as follows: First, the gas to be treated is introduced through the inlet. The gas enters the inner shell 2 through the upper tee and upper connecting pipe 6. A portion of the gas also enters the outer chamber 3 through the pressure balancing hole 8. This maintains a pressure balance between the inner shell 2 and the outer chamber 3, preventing the quartz glass inner shell 2 from shattering under high pressure and achieving a high-pressure environment. The gas pressure is maintained at 3 MPa by controlling the inlet and outlet rates. The catalyst sample is placed in the sample chamber 4 above the sample stage 5, and the catalyst can be fixed to the sample stage 5 with quartz wool. Illumination is provided by the light source 10, which provides a wavelength range of 300-2500 nm. The light emitted by the light source 10 is focused by the focuser 24 and irradiated onto the catalyst in the sample chamber 4. Simultaneously, the temperature of the reaction environment is precisely measured by the thermometer 22, and the catalyst and the entire environment are heated and temperature-controlled by the heating tube 9. After the high-voltage pulse power supply is turned on, high-voltage pulse discharge will occur at the tips of the positive electrode 12 and the negative electrode 13 to generate plasma. The gas collides with the plasma, and the gas is ionized and cracked. The high-energy gas undergoes a chemical reaction under the action of a catalyst to generate energy gas, which is finally discharged through the gas outlet for collection and detection.

[0035] Taking carbon dioxide methanation as an example

[0036] (1) First, the catalyst was prepared: Bimetallic Ni-Co-Al2O3 catalysts with different Co contents were prepared by mechanochemical method. NiCl2·6H2O, Al(NO3)3·9H2O, and Co(NO3)2·6H2O were used as metal precursors, and NH4HCO3 was used as a precipitant. The catalysts were mixed according to fixed molar ratios of NH4HCO3 to Al, NH4HCO3 to Ni, and NH4HCO3 to Co. All reagents used were commercially available analytical grade reagents. Specifically, NiCl2·6H2O used in this example was produced by Sinopharm Chemical Reagent Co., Ltd., Al(NO3)3·9H2O and NH4HCO3 were produced by Maclean's Reagent Co., Ltd., and Co(NO3)2·6H2O was produced by Beijing Chemical Reagent Co., Ltd.

[0037] (2) Weigh 200 mg of Ni-Co-Al2O3 catalyst, place the catalyst on a thin layer of glass wool and place it on the sample stage 5. At the same time, start preheating until the temperature reaches the preset 350℃. Then, introduce CO2 and H2 in an inlet flow rate ratio of CO2:H2 = 6:24 (ml / min) and make the pressure in the sample chamber 4 reach 4 MPa. (CO2 and H2 are commercially available high-purity carbon dioxide and high-purity hydrogen).

[0038] (3) Turn on the light source (the light source is a xenon lamp light source, model: CEL-HXF300-T3) and the high voltage electric field mechanism so that the thermoelectric pressure acts on the catalyst simultaneously.

[0039] (4) Pass the CO2 and H2 mixture through the catalyst to make full contact between the mixture and the catalyst.

[0040] (5) After the temperature (350℃), pressure (4MPa), electric field and light source have stabilized, the reaction time is adjusted as needed to carry out the reaction to completion; the composition of the feed and product is analyzed online by a GC7920 gas chromatograph equipped with a thermal conductivity detector, a nickel-hydrogen conversion furnace and a packed column TDX01.

[0041] (6) The conversion rate of CO2 is obtained by measuring the content of products such as methane.

[0042] Experimental results are shown below:

[0043]

[0044] Through relevant comparative experiments, the conversion rate of carbon dioxide and the selectivity of the products were tested under different conditions using the same catalyst.

[0045] Comparison of experimental results

[0046]

[0047] Comparison of carbon dioxide conversion rates under different conditions Figure 2 As shown.

[0048] The data above shows that the catalytic efficiency is lowest under conditions of low temperature, no light, no pressure, and no electric field. As the number of external stimuli acting on the catalyst increases, the catalytic effect gradually improves. The catalytic efficiency is highest under the combined effects of heat, light, and pressure. Furthermore, the synergistic effect of light, electricity, heat, and pressure can further enhance the catalytic efficiency.

[0049] Conclusion: Applying multiple forces such as light, electricity, heat and pressure simultaneously during the reaction process can achieve high efficiency and selectivity in chemical reactions.

[0050] It is worth mentioning that the technical features such as the heating tube 9 and the light source 10 involved in this patent application should be regarded as prior art. The specific structure, working principle and possible control method and spatial arrangement of these technical features can be adopted by conventional choices in the field, and should not be regarded as the inventive point of this patent. This patent will not be further elaborated in detail.

[0051] The preferred embodiments of the present invention have been described in detail above. It should be understood that those skilled in the art can make many modifications and variations based on the concept of the present invention without creative effort. Therefore, all technical solutions that can be obtained by those skilled in the art based on the concept of the present invention through logical analysis, reasoning or limited experimentation on the basis of the prior art should be within the scope of protection defined by the claims.

Claims

1. A high-voltage pulsed discharge photothermal synergistic catalytic reaction device, characterized in that, It includes a housing mechanism, a heating mechanism, a light source, and a high-voltage electric field mechanism; The housing mechanism includes an outer shell and an inner shell. The inner shell is located inside the outer shell, and an outer cavity is formed between the inner shell and the outer shell. A sample chamber is provided inside the inner shell, and a sample fixing stage is provided below the sample chamber. An upper connecting pipe is connected to the upper end of the inner shell, and the upper connecting pipe extends out of the outer shell. A lower connecting pipe is connected to the lower end of the inner shell, and the lower connecting pipe extends out of the outer shell. A pressure-balancing hole communicating with the outer cavity is provided on the upper connecting pipe and the lower connecting pipe, respectively. The heating mechanism includes a heating tube, which is mounted on the outer casing. The light source is mounted on the outer shell and shines directly into the sample chamber, while the portion of the inner shell corresponding to the sample chamber is transparent. The high-voltage electric field mechanism includes a power source, a positive electrode, and a negative electrode. The positive and negative electrodes are respectively connected to the power source and are arranged opposite to each other. The lower end of the positive electrode extends into the inner shell and is located at the upper end of the sample chamber, while the upper end of the negative electrode extends into the inner shell and is located at the lower end of the sample chamber. The inner shell is made of quartz glass. Ceramic insulating tubes are respectively fitted onto the positive electrode and the negative electrode.

2. The high-voltage pulsed discharge photothermal synergistic catalytic reaction device as described in claim 1, characterized in that, The outer casing includes an upper cover and a lower cover. An upper connecting pipe is installed in the middle of the upper cover. The upper end of the upper connecting pipe is located outside the outer casing and is connected to an upper tee pipe. The upper tee pipe includes an upper main pipe and an upper side pipe. The lower end of the upper main pipe is fixedly connected to the upper end of the upper connecting pipe. The positive electrode is inserted into the upper main pipe from the upper end of the upper main pipe and extends through the upper connecting pipe to the upper end of the sample chamber. An air inlet is provided on the upper side pipe. A lower connecting pipe is installed in the middle of the lower cover. The lower end of the lower connecting pipe is located outside the outer casing and is connected to a lower tee pipe. The lower tee pipe includes a lower main pipe and a lower side pipe. The lower end of the lower main pipe is fixedly connected to the lower end of the lower connecting pipe. The negative electrode is inserted into the lower main pipe from the lower end of the lower main pipe and extends through the lower connecting pipe to the lower end of the sample chamber. An air outlet is provided on the lower side pipe.

3. The high-voltage pulsed discharge photothermal synergistic catalytic reaction device as described in claim 1, characterized in that, The outer casing is equipped with a thermometer for measuring the temperature of the outer chamber and the sample chamber, and the thermometer is positioned opposite the light source.

4. The high-voltage pulsed discharge photothermal synergistic catalytic reaction device as described in claim 3, characterized in that, The light source has a wavelength of 300-2500nm and a power of 100-350W.

5. The high-voltage pulsed discharge photothermal synergistic catalytic reaction device as described in claim 4, characterized in that, The light source is mounted on a lampshade, which is fixed to the outer casing. The front end of the lampshade extends into the outer cavity, and a focuser is installed at the front end of the lampshade.

6. The high-voltage pulsed discharge photothermal synergistic catalytic reaction device as described in claim 1, characterized in that, The output voltage of the high-voltage electric field mechanism is 0-30kV.

7. The high-voltage pulsed discharge photothermal synergistic catalytic reaction device as described in claim 1, characterized in that, The outer shell has an internal interlayer, and the heating tube is installed in the interlayer.

8. A high-voltage pulsed discharge photothermal synergistic catalytic reaction method, characterized in that, The high-voltage pulsed discharge photothermal synergistic catalytic reaction device as described in any one of claims 1-7 includes the following steps: Step 1: Place the catalyst on the sample stage, turn on the heating tube, control the temperature in the sample chamber within a certain range, and then introduce the reactants into the sample chamber. Step 2: Turn on the light source. The light source shines through the inner shell onto the sample chamber, generating a photoelectric effect in the sample chamber, which causes the reactants to be electronically excited and converted into an active state. Step 3: Turn on the high-voltage electric field mechanism to apply the electric field to both ends of the sample chamber with the required voltage and holding time; Step 4: Control the flow rate of the reactants to increase the pressure of the reactants in the sample chamber, thereby shortening the distance between the reactants to increase the interaction force and promote the reaction. Step 5: Maintain the reaction temperature, light intensity, and voltage to ensure the reactants in the container achieve the best reaction effect. Adjust the reaction time as needed and carry the reaction to completion. Step 6: Separate the high-voltage pulse discharge photothermal synergistic catalytic reaction products.

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