Electrode reaction kettle and application thereof in plastic degradation
By using plasma electrolysis technology in an electrode reactor to control the solution state and exchange solvents, the problem of excessive oxygen content in hydrothermal liquefaction is solved, achieving green and environmentally friendly plastic degradation and product separation, which is suitable for industrial production.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- XIAMEN UNIV
- Filing Date
- 2023-12-21
- Publication Date
- 2026-05-19
AI Technical Summary
Existing hydrothermal liquefaction technology suffers from problems such as excessively high oxygen content during plastic degradation, leading to difficulties in product separation and purification, and the use of chemical catalysts can pollute the environment.
The electrode reactor is used to degrade plastics through plasma electrolysis. Plasma is generated by high-voltage electrode assembly and ground electrode assembly. The solution is controlled in a subcritical/supercritical state. Solvent is exchanged through the inlet and outlet to reduce the oxygen content. Plastics are selectively added to generate ethers, lipids and alkanes.
It enables catalyst-free degradation of plastics, reduces oxygen content, simplifies separation and purification processes, and is suitable for industrial production.
Smart Images

Figure CN117732395B_ABST
Abstract
Description
Technical Field
[0001] This invention relates to the field of hydrothermal liquefaction technology, and in particular to an electrode reactor and its application in plastic degradation. Background Technology
[0002] The degradation of plastics can not only reduce environmental pollution, but also facilitate the reuse of resources. Currently, the main methods for degrading plastics include alcoholysis, hydrolysis, and phosphate ester degradation. Although chemical degradation methods can effectively degrade plastics, they also generate a large number of harmful chemical reagents, polluting the environment.
[0003] With the development of supercritical technology, combined with hydrothermal liquefaction, efficient degradation of plastics has been achieved, yielding a large amount of light oil. However, during hydrothermal liquefaction, when the solution temperature reaches 370℃, the spacing between plastic monomers increases, weakening the barrier properties. When the solution temperature approaches 370℃, oxygen-containing free radicals OH, O, and HO2 generated by discharge collide with polypropylene plastic monomers, producing dozens of products such as alcohols, acids, esters, ethers, glucose, and pyridine. The increase in the variety of products leads to excessively high oxygen content, making separation and purification difficult. Summary of the Invention
[0004] In view of this, the present invention provides an electrode reaction vessel and its application in plastic degradation, which not only does not involve the use of chemical catalysts, but also reduces the oxygen content and realizes plasma electrolytic degradation of plastics to obtain ethers, lipids and alkanes, etc.
[0005] To achieve the above objectives, the present invention adopts the following technical solution:
[0006] On one hand, the present invention provides an electrode reaction vessel, comprising:
[0007] The reactor cavity has a drain port at the bottom and a cavity cover at the top, and the cavity cover has a feed port, a liquid inlet, an air inlet and an exhaust port.
[0008] A plasma device, fixed to the reactor cavity and / or the cavity cover, is used to discharge into the reactor cavity to generate plasma.
[0009] Preferably, the plasma device includes:
[0010] Plasma power supply;
[0011] A high-voltage electrode assembly is connected to the high-voltage output terminal of the plasma power supply;
[0012] The ground electrode assembly is connected to the low-voltage output terminal of the plasma power supply, and plasma is generated through the high voltage between the high-voltage electrode assembly and the ground electrode assembly.
[0013] Preferably, the electrode reactor further includes:
[0014] A pressure sensor, installed in the reactor cavity and / or cavity cover, is used to measure the pressure inside the electrode reactor;
[0015] And / or a temperature sensor, installed in the reactor cavity and / or cavity cover, for measuring the temperature inside the electrode reactor;
[0016] And / or the high-voltage electrode assembly, the ground electrode assembly, the pressure sensor, and the temperature sensor are all wrapped with insulating sleeves.
[0017] Preferably, the inlet is equipped with a feeding assembly, which includes a feeding pipe installed at the inlet. The feeding pipe is provided with a sealing cap, a feeding bin for holding plastic materials, and a one-way valve arranged sequentially from top to bottom inside the feeding pipe.
[0018] More preferably, the feed hopper is connected to a high-pressure gas device, and the plastic material in the feed hopper is injected into the reactor cavity through the one-way valve by high-pressure gas;
[0019] More preferably, the plastic contained in the feed hopper includes any one or more of polyethylene, polypropylene, polyvinyl chloride, polystyrene, and polycarbonate.
[0020] Preferably, the liquid inlet is equipped with a liquid inlet assembly, which includes a liquid inlet pipe installed at the liquid inlet. The liquid inlet pipe is provided with a liquid chamber for holding solvent and a one-way valve from top to bottom.
[0021] More preferably, the liquid chamber is connected to a high-pressure gas device, and the liquid in the liquid chamber is injected into the reactor cavity through the one-way valve by high-pressure gas;
[0022] More preferably, the solvent contained in the liquid chamber includes one or more mixed solvents selected from water, alcohols, esters, and alkanes.
[0023] Preferably, the air inlet is equipped with an air inlet assembly, the air inlet assembly includes an air inlet pipe, the air inlet pipe is installed at the air inlet, and a needle valve is provided inside the air inlet pipe, the air inlet pipe is connected to a high-pressure gas device;
[0024] Preferably, the exhaust port is equipped with an exhaust assembly, the exhaust assembly includes an exhaust pipe, the exhaust pipe is installed at the exhaust port, and a needle valve is provided inside the exhaust pipe, the exhaust pipe is connected to a gas collection device.
[0025] Preferably, the drain outlet is equipped with a drain assembly, which includes a drain pipe installed at the drain outlet, and a filter screen is provided at the top of the drain pipe, and a needle valve is provided inside the drain pipe.
[0026] Preferably, the electrode reactor further includes:
[0027] The inner liner of the reactor is located inside the reactor cavity;
[0028] and / or an insulating sleeve, disposed on the outside of the reactor cavity;
[0029] And / or the insulation sleeve includes a heat dissipation layer, an insulation layer and an outer shell layer arranged sequentially from the inside to the outside, wherein the heat dissipation layer wraps around the outer wall of the reactor cavity;
[0030] And / or the shape of the reaction liner, the insulation sleeve and the reaction vessel cavity are adapted.
[0031] Preferably, the electrode reactor further includes a high-pressure safety valve, installed in the reactor cavity and / or the cavity cover;
[0032] And / or the opening pressure of the high-pressure safety valve is not less than 30 MPa.
[0033] On the other hand, the present invention also provides an application of the electrode reaction vessel described above in plastic degradation. A voltage is applied to the high-voltage electrode assembly by a plasma power supply. The active ions generated by the discharge of the high-voltage electrode assembly diffuse in the reaction vessel cavity to heat the solution, so that the solution enters the subcritical / supercritical state. After the solution composition is changed and the temperature reaches 420°C, plastic is added to the reaction vessel cavity. The reaction products obtained after the reaction degradation are discharged from the drain port.
[0034] When the solvent temperature reaches 370℃, the oxygen-containing solvent is discharged through the drain port, while solvent is added through the inlet port to change the oxygen content in the reaction vessel cavity and complete the change of solution composition.
[0035] This invention provides an electrode reaction vessel and its application in the degradation of plastics. Compared with the prior art, its advantages are as follows:
[0036] This invention generates plasma within the reactor cavity through high voltage between two electrodes. Water, alcohols, and esters are discharged to enter a subcritical / supercritical state. Solution exchange is then performed through the outlet and inlet, thereby reducing the oxygen content of the solvent within the reactor. The addition of alkanes at the inlet significantly increases the CHx (CH3, CH2, CH) content within the reactor. Plastic is then added through the feed inlet. This method effectively increases the alkane content in the product. The timing of plastic addition can be selected based on the desired product, thus obtaining products such as ethers, esters, and alkanes, which are then discharged under reduced pressure through the outlet.
[0037] This invention does not involve the use of catalysts, making it green and environmentally friendly. It also avoids the difficulty of subsequent separation and purification by not using large amounts of catalysts. Plasma electrolysis degradation of plastics is achieved through an electrode reactor. The operation process is simple and suitable for industrial production. Attached Figure Description
[0038] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the description of the embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are only embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on the provided drawings without creative effort.
[0039] Figure 1 This is a schematic diagram of the electrode reaction vessel of the present invention;
[0040] Figure 2 This is a schematic diagram of the feeding assembly of the present invention;
[0041] Figure 3 This is a schematic diagram of the sealing cap structure in the feeding assembly of the present invention;
[0042] Figure 4 This is a schematic diagram of the feeding hopper of the present invention;
[0043] Figure 5 This is a schematic diagram of the structure of the inner liner of the reactor of the present invention;
[0044] Figure 6 This is a schematic diagram of the structure of the thermal insulation sleeve of the present invention;
[0045] Figure 7 This is a graph showing the discharge voltage and current curves of tap water at the first minute of this embodiment of the invention.
[0046] Figure 8 This is a graph showing the discharge voltage and current curves of tap water at the 1st minute after 8 drainage cycles in an embodiment of the present invention.
[0047] In the diagram:
[0048] 100-Reaction vessel cavity, 110-Cavity cover, 120-Drain port, 130-Feed inlet, 140-Liquid inlet, 150-Air inlet, 160-Exhaust port, 170-Reaction vessel inner liner, 180-Insulation jacket, 181-Heat dissipation layer, 182-Insulation layer, 183-Outer shell layer, 210-High voltage electrode assembly, 220-Ground electrode assembly, 310-Pressure sensor, 320-Temperature sensor, 400-Feed assembly, 410-Feed pipe, 420-Sealing cover, 421-Sealing gasket, 422-Pipe port, 423-Cover, 430-Feed hopper, 440-One-way valve, 450-Ventilation port, 500-Liquid inlet assembly, 600-Air inlet assembly, 700-Exhaust assembly, 800-Drain assembly, 810-Filter screen, 900-High pressure safety valve. Detailed Implementation
[0049] The embodiments of the present invention are described in detail below. Examples of these embodiments are shown in the accompanying drawings, wherein the same or similar reference numerals denote the same or similar elements or elements having the same or similar functions throughout. The embodiments described below with reference to the accompanying drawings are exemplary and are only used to explain the present invention, and should not be construed as limiting the present invention. Where specific techniques or conditions are not specified in the embodiments, they are performed in accordance with the techniques or conditions described in the literature in the art or in accordance with the product instructions. Reagents or instruments used, unless otherwise specified, are all conventional products that can be obtained commercially.
[0050] In one aspect of the invention, such as Figure 1 As shown, the present invention proposes an electrode reaction vessel, including a reaction vessel cavity 100 and a plasma device;
[0051] The reactor chamber 100 has a drain port 120 at the bottom and a chamber cover 110 at the top. The chamber cover 110 has a feed port 130, a liquid inlet 140, an air inlet 150, and an exhaust port 160. The reactor chamber 100 is used for air intake, feed, liquid intake, liquid drainage, exhaust, and to contain plastics and solvents. The plasma device is fixed to the reactor chamber 100 and / or the chamber cover 110 and is used to discharge into the reactor chamber 100 to generate plasma.
[0052] Furthermore, the reactor cavity 100 is preferably cylindrical, with a diameter of 6-50cm and a thickness of 5mm or more, and is made of metallic materials, including but not limited to any one of stainless steel, tungsten, tungsten-molybdenum alloy, etc.
[0053] This invention utilizes the diffusion and mass transfer of active particles generated by two-electrode discharge within a reaction vessel to heat the solution. As the kinetic energy of molecules within the vessel increases, the generated self-pressure or external pressure forces the solution into a subcritical or supercritical state. The amount of solution discharged and the amount of solvent added through the inlet 140 are then selected based on the desired product, and the oxygen content within the vessel is adjusted. Finally, the timing of adding plastic is chosen. This process yields products such as ethers, esters, and alkanes, which are then discharged under reduced pressure through the outlet.
[0054] In some embodiments of the present invention, a sealing gasket is provided at the connection between the cavity cover 110 and the reaction vessel cavity 100 to seal between the cavity cover 110 and the reaction vessel cavity 100, thereby preventing leakage of solvents and gases and ensuring the smooth progress of the reaction.
[0055] In some embodiments of the present invention, the plasma device includes a plasma power supply 210, a high-voltage electrode assembly 210, and a ground electrode assembly 220.
[0056] The plasma power supply 210 generates discharge plasma by loading a cavitation bubble generated by an ultrasonic generator through a high-voltage electrode and a ground electrode. The power supply output parameters can be selected as follows: voltage 200-5000V, frequency 5Hz-5kHz, and the output waveform can be one of sine wave, square wave, etc. It can generate stable plasma in solution and has an output power of 100-20000W. The high-voltage electrode assembly 210 is connected to the high-voltage output terminal of the plasma power supply 210 through electrode leads. The ground electrode assembly 220 is connected to the low-voltage output terminal of the plasma power supply 210 through electrode leads. Plasma is generated through the high voltage between the high-voltage electrode assembly 210 and the ground electrode assembly 220.
[0057] Furthermore, both the high-voltage electrode assembly 210 and the ground electrode assembly 220 are wrapped with insulating sleeves. Preferably, the insulating sleeves can be insulating and inert inorganic materials such as ceramics, corundum, and quartz, so as to insulate between the electrodes and between the electrodes and the cavity cover 110 and / or the reactor cavity 100, ensuring safety during use.
[0058] Furthermore, the high-voltage electrode assembly 210 and the ground electrode assembly 220 can both be made of one of the following materials: Ir-Iridium-Re rhenium alloy, spark carbon material, etc., which have the properties of high temperature resistance, high voltage resistance, high pressure resistance and corrosion resistance.
[0059] In some embodiments of the present invention, the electrode reactor further includes a pressure sensor 310, which is installed in the reactor cavity 100 and / or the cavity cover 110. The pressure sensor 310 can be a semiconductor piezoresistive type, capacitive type, diffused silicon pressure transmitter, etc., and the pressure measurement range is 0.1-30MPa. It is used to measure the pressure inside the electrode reactor.
[0060] Furthermore, the electrode reactor also includes a temperature sensor 320, which is installed in the reactor cavity 100 and / or cavity cover 110. The temperature sensor 320 can be a platinum resistance thermometer, a thermocouple thermometer, a semiconductor thermometer, etc., and the temperature measurement range is preferably 0-500℃. It is used to measure the temperature inside the electrode reactor.
[0061] It should be noted that the pressure sensor 310 and the temperature sensor 320 are both wrapped with insulating sleeves. Preferably, the insulating sleeves can be insulating and inert inorganic materials such as ceramics, corundum, and quartz, which are used to isolate the reactor cavity 100 and / or cavity cover 110 from the sensors to ensure safety during use.
[0062] In some embodiments of the present invention, the feed inlet 130 is equipped with a feed assembly 400, such as... Figure 2-4 As shown, the feeding assembly 400 includes a feeding pipe 410, which is installed at the feeding port 130. The feeding pipe 410 is provided with a sealing cover 420, a feeding bin 430 for holding plastic materials, and a one-way valve 440 in sequence from top to bottom. Preferably, the sealing cover 420 is provided with a vent 450. Preferably, the feeding pipe 410 is a metal pipe with an inner diameter of 5-30 mm and a wall thickness of not less than 3 mm.
[0063] Furthermore, the sealing cover 420 comprises a sealing gasket 421, a threaded opening 422, and a threaded cap 423. The sealing is achieved by compressing the circular gasket during the tightening of the threads on the cap 423 and the opening 422. Preferably, the cap 423 is made of metal material with a thickness of not less than 3 mm.
[0064] Furthermore, the feed hopper 430 is connected to a high-pressure gas device, and the plastic material in the feed hopper 430 is injected into the reactor cavity 100 through the one-way valve 440 by high-pressure gas; preferably, a ball valve is also installed at the bottom of the one-way valve 440 to adjust the injection speed of the plastic material; the high-pressure gas device is a conventional device for providing high-pressure gas, preferably including a gas pump and a gas cylinder, and there are no special limitations on it.
[0065] Furthermore, the feed hopper 430 can be a sphere or an ellipsoid, with a diameter of 2 / 3 to 4 / 5 of the inlet pipe diameter, or a cuboid cavity. The material can be metal, ceramic, quartz, corundum, or other high-temperature and corrosion-resistant materials. When the gas pressure entering through the vent exceeds the pressure inside the reactor, the feed hopper 430 will automatically open.
[0066] Furthermore, the plastic contained in the feed hopper 430 includes any one or more of polyethylene, polypropylene, polyvinyl chloride, polystyrene, and polycarbonate. Plastic particles or compressed liquid plastic are injected into the reactor chamber 100 through a one-way valve 440 using high-pressure gas.
[0067] Specifically, the operation method of the feeding assembly 400 is as follows: With the one-way valve 440 closed, open the vent 450 on the sealing cover 420 to ensure that the external air pressure is consistent with the air pressure in the feeding chamber 430. Then open the sealing cover 420, fill the feeding chamber 430 with plastic, then close the sealing cover 420 and the vent 450, and slowly open the one-way valve 440 to make the air pressure in the feeding chamber 430 and the reactor cavity 100 consistent. Then open the bottom outlet of the feeding chamber 430 to allow the plastic to enter the reactor cavity 100 from the one-way valve 440 channel.
[0068] In some embodiments of the present invention, a liquid inlet assembly 500 is installed at the liquid inlet 140. The liquid inlet assembly 500 includes a liquid inlet pipe, which is installed at the liquid inlet 140. The liquid inlet pipe is provided with a liquid chamber for holding solvent and a one-way valve 440 from top to bottom.
[0069] Furthermore, the liquid chamber is connected to a high-pressure gas device, and the liquid in the liquid chamber is injected into the reactor cavity 100 through a one-way valve 440 by high-pressure gas; preferably, a needle valve is also provided in the liquid inlet pipe, located at the bottom of the one-way valve 440, and the needle valve is used to adjust the injection speed of the solvent; the high-pressure gas device is a conventional device for providing high-pressure gas, preferably including a gas pump and a gas cylinder, and there are no special limitations on it.
[0070] Furthermore, the solvent contained in the liquid chamber includes one or more mixed solvents selected from water, alcohols, esters, and alkanes. The solvent is injected into the reactor chamber 100 through a one-way valve 440 using high-pressure gas.
[0071] It should be noted that the liquid inlet assembly 500 and the feed assembly 400 have similar structures, which will not be described in detail here.
[0072] Specifically, the operation method of the liquid inlet assembly 500 is as follows: With the one-way valve 440 closed, open the vent 450 of the liquid inlet pipe to ensure that the external air pressure is consistent with the air pressure of the liquid chamber. Then close the liquid chamber and the vent 450. Connect a high-pressure gas device to the vent 450. When the input air pressure of the vent 450 is higher than the air pressure on the one side of the one-way valve 440, the liquid chamber will be opened under the pressure, and the liquid will be injected. Then slowly open the one-way valve 440, and the liquid will be injected into the reactor cavity 100 under the external high pressure.
[0073] In some embodiments of the present invention, an air intake assembly 600 is installed at the air inlet 150. The air intake assembly 600 includes an air intake pipe installed at the air inlet 150, and a needle valve is provided inside the air intake pipe for adjusting the gas injection rate. The air intake pipe is connected to a high-pressure gas device, which is a conventional device for providing high-pressure gas, preferably including a gas pump and a gas cylinder, without special limitations.
[0074] Specifically, the operation method of the air intake assembly 600 is as follows: connect the air intake pipe to the high-pressure gas device, slowly open the one-way needle valve, and then slowly open the high-pressure gas device to allow the gas to enter the reactor through the air intake pipe.
[0075] In some embodiments of the present invention, an exhaust assembly 700 is installed at the exhaust port 160. The exhaust assembly 700 includes an exhaust pipe installed at the exhaust port 160 and a needle valve is provided inside the exhaust pipe to control the exhaust speed. The exhaust pipe is connected to a gas collection device. Preferably, the gas collection device includes, but is not limited to, a gas collection bag or a gas collection bottle.
[0076] Furthermore, the exhaust pipe is located 2-5 cm above the liquid surface, preferably 3 cm, and is used to discharge carbon dioxide from the reactor chamber 100.
[0077] In some embodiments of the present invention, a drainage assembly 800 is installed at the drain port 120. The drainage assembly 800 includes a drainage pipe installed at the drain port 120, and as shown... Figure 5 As shown, a filter screen 810 is provided at the top of the drain pipe. The filter screen 810 is located at the outlet of the reactor cavity 100 and is used to filter solid particles, prevent blockage, and prevent plastic from being discharged through the drain port 120. Preferably, a needle valve is provided inside the drain pipe to control and adjust the speed of solution discharge.
[0078] In some embodiments of the present invention, the electrode reactor further includes a reactor liner 170, which is disposed inside the reactor cavity 100. The reactor liner 170 is made of insulating, high-temperature resistant, and corrosion-resistant material. Drainage ports 120 are provided at corresponding positions of the reactor cavity 100 and the reactor liner 170 for discharging the liquid after the reaction, including oxygen-containing solvents and products after subsequent plastic liquefaction.
[0079] Furthermore, the present invention also includes an insulation sleeve 180, such as Figure 6 As shown, the insulation jacket 180 includes a heat dissipation layer 181, an insulation layer 182, and an outer shell layer 183 arranged sequentially from the inside to the outside. The heat dissipation layer 181 wraps around the outer wall of the reactor cavity 100. Preferably, both the outer shell layer 183 and the heat dissipation layer 181 are made of metal. The outer shell layer 183 is used to enhance the overall stability of the electrode reactor. The space between the outer shell layer 183 and the heat dissipation layer 181 is filled with insulation materials such as insulation cotton to prevent heat loss.
[0080] In some embodiments of the present invention, the electrode reactor further includes a high-pressure safety valve 900, which is installed in the reactor cavity 100 and / or the cavity cover 110 to prevent the high-pressure reactor from bursting due to excessive pressure.
[0081] Furthermore, the opening pressure of the high-pressure safety valve 900 is not less than 30MPa, and it can be selected from any of the following types: plumb bob type, lever type, spring type, and pilot type.
[0082] In another aspect of the present invention, an electrode reactor is proposed for use in plastic degradation. The plastic degradation method is achieved using the aforementioned electrode reactor. A voltage is applied to the high-voltage electrode assembly by a plasma power supply 210. The active ions generated by the discharge of the high-voltage electrode assembly 210 diffuse in the reactor cavity 100 to heat the solution, causing the solution to enter a subcritical / supercritical state. After the solution composition has changed and the temperature reaches 420°C, plastic is added to the reactor cavity 100. The reaction products obtained after the degradation reaction are discharged from the drain port 120.
[0083] When the solvent temperature reaches 370℃, the oxygen-containing solvent is discharged through the drain port 120, and at the same time, the solvent is added through the inlet port 140 to change the oxygen content in the reaction vessel cavity 100 so that the solution composition is changed.
[0084] Specifically, the reaction vessel cavity 100 is used to hold the solvent and is equipped with a filter screen 810 and a drain port 120 at the bottom. The liquid is discharged after being filtered through the filter screen 810. The gas generated during the reaction is discharged through the exhaust port 160 on the cavity cover 110. In order to increase the pressure inside the reaction vessel and change the composition and content of the product, hydrogen and alkanes are introduced through the air inlet 150. During the reaction, in order to reduce the oxygen content in the solvent, oxygenated solvent is gradually discharged from the drain port 120 to change the solvent composition. At the same time, alkane solvent is slowly added from the liquid inlet 140. After the solution composition is changed and the temperature reaches 420°C, plastic is slowly added from the feed port 130. After reacting for 5-30 minutes, the degraded reaction products also need to be slowly discharged through the drain port 120.
[0085] It should be noted that the height of the outer wall of the reactor cavity 100 is slightly lower than the height of the inner wall of the cavity by 0.1-0.5 mm. This is to ensure that the pressure inside and outside the reactor is consistent, otherwise it will be easily broken. In addition, the feed pipe 410, liquid inlet pipe, air inlet pipe, exhaust pipe and other components involved in this invention are preferably made of metal.
[0086] The present invention will be described below through specific embodiments. Those skilled in the art will understand that the specific embodiments below are merely illustrative and do not limit the scope of the invention in any way. Furthermore, in the following embodiments, unless otherwise specified, the reagents and equipment used are commercially available. If specific processing conditions and methods are not explicitly described in the later embodiments, conditions and methods known in the art can be used for processing.
[0087] This invention is based on the above-mentioned electrode reactor and utilizes plasma electrolysis of tap water, wherein the tap water content does not exceed 2 / 3 of the reactor's inner liner. After the temperature inside the reactor reaches a certain temperature, such as 378°C in the experiment, an ester or alkane solvent is injected. The initial solvent content does not exceed twice the volume of the tap water, such as adding 1 / 5 of the tap water volume. When the temperature of the solution inside the reactor reaches a certain value, such as 431°C, the oxygen-containing solvent is discharged from the outlet. This process is repeated to gradually change the solvent composition and reduce the oxygen content of the solvent.
[0088] Example 1
[0089] 40ml of tap water was poured into the reactor chamber. A voltage was applied to the high-voltage electrode assembly using a plasma power supply. The corresponding discharge current curves for voltages between 200-700V are shown below. Figure 7 As shown, after 20-60 minutes, the temperature of the solution in the electrode reactor was 284-405℃, the pressure was less than 10MPa, and the corresponding circuit current was 0.05-1.00A. During this period, the voltage first decreased and then increased, which was caused by the increased thickness of the oxide generated by the metal electrode.
[0090] At this point, inject 8 ml of valproic acid (1 / 5 the volume of tap water) through the inlet. After 20 minutes, the discharge voltage increases to 300-800V. When the temperature rises to 430℃, the pressure will be slightly higher than 10MPa. Open the drain port to discharge 1 / 5 of the solution. At this point, the temperature drops to 340℃. When the temperature recovers to above 400℃, inject another 8 ml of valproic acid through the inlet. At this point, the temperature is 450℃, and the corresponding pressure is 11MPa.
[0091] After repeating the above process eight times, the oxygen content was determined by an elemental analyzer to be no higher than 33 wt%. The temperature was controlled to be no higher than 470℃, corresponding to a gas pressure of approximately 12 MPa. CO2 and O2 were then discharged through the exhaust port, while H2 was introduced through the inlet. After 5 minutes, the discharged gas was mainly H2. Subsequently, 2.6 g of polyethylene plastic was added, and the temperature was controlled below 470℃ for 15 minutes. The discharged products were mainly acetaldehyde, ether, methoxyethane, propionaldehyde, tetrahydrofuran, cyclopropanol, oxacyclobutane, tetrahydropyran, dioxane, tetrahydropyran-3-ol, and tetrahydrofuran-3-ol, which are mainly composed of aldehydes, esters, ethers, and alkanes.
[0092] Example 2
[0093] 40ml of tap water was poured into the reactor chamber. A voltage was applied to the high-voltage electrode assembly using a plasma power supply. The corresponding discharge current curves for voltages between 200-700V are shown below. Figure 7As shown, after 20-60 minutes, the temperature of the solution in the high-pressure reactor is 284-405℃, the pressure is less than 10MPa, and the corresponding circuit current is 0.05-1.00A.
[0094] At this point, inject 8 ml of valproic acid (1 / 5 the volume of tap water) through the inlet. After 20 minutes, the discharge voltage increases to 300-800V. When the temperature rises to 430℃, the pressure will be slightly higher than 10MPa. Open the drain port to discharge 1 / 5 of the solution. At this point, the temperature drops to 340℃. When the temperature recovers to above 400℃, inject another 8 ml of valproic acid through the inlet. At this point, the temperature is 450℃ and the pressure is 11MPa.
[0095] After repeating the above process eight times, the temperature is controlled to not exceed 470℃, corresponding to a gas pressure of approximately 12MPa. Then, CO2 and O2 are discharged through the exhaust port, while H2 is introduced through the inlet port. After 5-10 minutes, the discharged gas is mainly H2, and the temperature is again controlled to not exceed 470℃. To further reduce the oxygen content in the solvent, 8 ml of solution is first discharged. When the temperature reaches 430℃, 8 ml of alkanes are added. In this experiment, n-octane is added. With the addition of n-octane, the voltage increases to 2800-4200V, corresponding to a current of 0.05-0.5A. When the temperature inside the reactor is between 430-470℃, oxygen-containing solvent continues to be discharged through the drain port, stopping when the temperature drops to 340℃.
[0096] When the oxygen content is determined to be no higher than 10wt% by an elemental analyzer, CO2 and O2 are discharged from the exhaust port, while H2 is introduced into the inlet. This process is continued for 5-10 minutes until the discharged gas is mainly H2. Then, the temperature is controlled to be no higher than 470℃, and 2.6g of polyethylene plastic is added. The temperature is controlled to be below 470℃ for 15 minutes, corresponding to a gas pressure of approximately 22MPa.
[0097] The discharged liquid products are mainly ethers, lipids, and aldehydes, such as isoalkanes, cycloalkanes, and alkenes, with alkanes accounting for 68.4%, alkenes 17.6%, ethers 8.6%, lipids 4.2%, and aldehydes 0.4%. The gaseous products are 38.3% methane, 3.4% ethane, 0.2% CO, and 58.1% alkanes.
[0098] After the reaction is complete, first turn off the power, then turn off the gas switch to disconnect the gas path, cool until the temperature sensor shows room temperature, turn off the temperature sensor switch, and then slowly open the needle valve switch of the exhaust port until the pressure sensor indicates atmospheric pressure, and then use a screwdriver to open the reactor.
[0099] In summary, the electrode reactor of the present invention heats the solution by diffusion and mass transfer of active particles generated by the discharge of two electrodes within the reactor. As the kinetic energy of the molecules inside the reactor increases, the generated self-pressure or external pressure causes the solution to enter a subcritical or supercritical state. Then, based on the desired product, the content of the discharged solution and the content of the solvent added at the inlet are selected, the oxygen content inside the reactor is adjusted, and finally, the timing of adding plastic is selected. In this way, products such as ethers, esters, and alkanes can be obtained, which are then discharged from the outlet after depressurization.
[0100] In the description of this specification, the terms "one embodiment," "another embodiment," "yet another embodiment," "some embodiments," "some specific embodiments," "other specific embodiments," etc., refer to specific features, structures, materials, or characteristics described in connection with that embodiment, which are included in at least one embodiment of the present invention. In this specification, the illustrative expressions of the above terms do not necessarily refer to the same embodiment or example. Furthermore, the specific features, structures, materials, or characteristics described may be combined in any suitable manner in one or more embodiments or examples. Moreover, those skilled in the art can combine and integrate the different embodiments or examples described in this specification, as well as the features of different embodiments or examples, without contradiction. Additionally, it should be noted that in this specification, the terms "first" and "second" are used for descriptive purposes only and should not be construed as indicating or implying relative importance or implicitly specifying the number of indicated technical features.
[0101] Although embodiments of the present invention have been shown and described above, it is understood that the above embodiments are exemplary and should not be construed as limiting the present invention. Those skilled in the art can make changes, modifications, substitutions and variations to the above embodiments within the scope of the present invention.
Claims
1. An electrode reaction vessel, characterized in that, include: The reactor cavity has a drain port at the bottom and a cavity cover at the top, and the cavity cover has a feed port, a liquid inlet, an air inlet and an exhaust port. A plasma device, fixed to the reactor cavity and / or the cavity cover, is used to discharge into the reactor cavity to generate plasma; The plasma device includes: Plasma power supply; A high-voltage electrode assembly is connected to the high-voltage output terminal of the plasma power supply; The ground electrode assembly is connected to the low-voltage output terminal of the plasma power supply, and plasma is generated through the high voltage between the high-voltage electrode assembly and the ground electrode assembly. The feed inlet is equipped with a feed assembly, which includes a feed pipe installed at the feed inlet. The feed pipe is provided with a sealing cap, a feed bin for holding plastic materials, and a one-way valve arranged sequentially from top to bottom inside the feed pipe. The feeding hopper is connected to a high-pressure gas device, and the plastic material in the feeding hopper is injected into the reaction vessel cavity through the one-way valve by high-pressure gas. The inlet is equipped with an inlet assembly, which includes an inlet pipe installed at the inlet. The inlet pipe is provided with a liquid chamber for holding solvent and a one-way valve from top to bottom. The liquid chamber is connected to a high-pressure gas device, and the liquid in the liquid chamber is injected into the reactor cavity through the one-way valve by high-pressure gas. The air inlet is equipped with an air inlet assembly, which includes an air inlet pipe. The air inlet pipe is installed at the air inlet and is connected to a high-pressure gas device. The exhaust port is equipped with an exhaust assembly, which includes an exhaust pipe. The exhaust pipe is installed at the exhaust port and is connected to a gas collection device. The drain outlet is equipped with a drain assembly, which includes a drain pipe installed at the drain outlet, and a filter screen is provided at the top of the drain pipe.
2. The electrode reactor according to claim 1, characterized in that, Also includes: A pressure sensor, installed in the reactor cavity and / or cavity cover, is used to measure the pressure inside the electrode reactor; And / or a temperature sensor, installed in the reactor cavity and / or cavity cover, for measuring the temperature inside the electrode reactor; And / or the high-voltage electrode assembly, the ground electrode assembly, the pressure sensor, and the temperature sensor are all wrapped with insulating sleeves.
3. The electrode reactor according to claim 1, characterized in that, The plastics contained in the feed hopper include any one or more of polyethylene, polypropylene, polyvinyl chloride, polystyrene, and polycarbonate.
4. The electrode reactor according to claim 1, characterized in that, The solvent contained in the liquid chamber includes one or more mixed solvents selected from water, alcohols, esters, and alkanes.
5. The electrode reactor according to any one of claims 1-4, characterized in that, Also includes: The inner liner of the reactor is located inside the reactor cavity; and / or an insulating sleeve, disposed on the outside of the reactor cavity; And / or the insulation sleeve includes a heat dissipation layer, an insulation layer and an outer shell layer arranged sequentially from the inside to the outside, wherein the heat dissipation layer wraps around the outer wall of the reactor cavity; And / or the inner liner of the reactor, the insulation sleeve and the reactor cavity are adapted to each other in shape.
6. The electrode reactor according to claim 5, characterized in that, It also includes a high-pressure safety valve, installed in the reactor cavity and / or the cavity cover; And / or the opening pressure of the high-pressure safety valve is not less than 30 MPa.
7. The application of the electrode reactor according to any one of claims 1-6 in plastic degradation, characterized in that, A voltage is applied to the high-voltage electrode assembly by a plasma power source. The active ions generated by the discharge of the high-voltage electrode assembly diffuse in the reaction vessel cavity to heat the solution, so that the solution enters the subcritical / supercritical state. After the solution composition is changed and the temperature reaches 420°C, plastic is added to the reaction vessel cavity. The reaction products obtained after the reaction degradation are discharged from the drain port. When the solvent temperature reaches 370℃, the oxygen-containing solvent is discharged through the drain port, while solvent is added through the inlet port to change the oxygen content in the reaction vessel cavity and complete the change of solution composition.