A large-area flow phase photocatalytic reaction device

CN117772097BActive Publication Date: 2026-10-30UNIV OF SCI & TECH OF CHINA
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Patent Information

Application Number
CN202311869459.0
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2023-12-28
Publication Date
2026-10-30
Estimated Expiration
2043-12-28

AI Technical Summary

Technical Problem

[0005]基于上述现有技术的不足,本申请提供了一种大面积流动相光催化反应装置,以解决现有技术转化小分子的效率低并且规模小的问题

Benefits of technology

[0045]本申请提供了一种大面积流动相光催化反应装置,包括催化系统以及气液导流系统。催化系统包括光源电源装置、暗箱以及设置暗箱中的光催化反应器和多个光源。光源电源装置用于为各个光源提供电能。光催化反应器设置有反应腔体。光催化反应器中的反应腔体的两端分别设置有原料入口和产物出口,且反应腔体中设置用于涂覆光催化剂的光催化涂覆层。光催化反应器中的反应腔体朝上的一面为石英视窗。各个光源设置于石英视窗的上面,用于透过石英视窗向反应腔体照射光线,以使得反应腔体中的原料在光照和光催化剂的作用下发生反应。气液导流系统包括气液导入系统和气液导出系统。气液导入系统包括原料供给装置以及鼓泡装置。鼓泡装置的出口位置高于鼓泡装置中的液体的液面,且通过导管与反应腔体的原料入口密封连通。原料供给装置与鼓泡装置通过导管连通,且导管连接鼓泡装置的一端插入鼓泡装置中的液体的液面下,以通过鼓泡装置中的液体将原料供给装置排出的气体原料润湿后,排入反应腔体中进行反应。气液导出系统的入口与反应腔体的产物出口通过导管连通,用于收集反应腔体排出的气体和液体。所以通过鼓泡装置可以让大量的反应气体充分润湿,使得气液两相反应物质能够充分的接触和混合,保证后续可以有效进行高效的反应。并且大面积的反应腔体可以通过大量反应气体,以及接收大面积的光照,且通过光催化涂覆层,保证反应物与催化剂充分接触,可以保证这些反应物都可以高效进行反应,从而实现对二氧化碳以及甲烷等气体的规模转化。

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Abstract

The application discloses a large-area flowing phase photocatalytic reaction device, which comprises a catalytic system and a gas-liquid guiding system; the catalytic system comprises a light source power supply device, a dark box and a plurality of light sources and photocatalytic reactors arranged in the dark box; the photocatalytic reactor is provided with a reaction cavity; the reaction cavity is provided with a raw material inlet and a product outlet, and is provided with a photocatalytic coating layer coated with a photocatalyst; an upward side of the reaction cavity is a quartz window; each light source is arranged on the upper side of the quartz window; the gas-liquid guiding system comprises a gas-liquid guiding-in system and a gas-liquid guiding-out system; the gas-liquid guiding-in system comprises a raw material supply device and a bubbling device; an outlet of the bubbling device is higher than a liquid level of liquid in the bubbling device, and is communicated with the raw material inlet of the reaction cavity through a pipeline; the raw material supply device is communicated with the bubbling device through a pipeline, and one end of the pipeline is inserted below the liquid level of the liquid in the bubbling device; the inlet of the gas-liquid guiding-out system is communicated with the product outlet of the reaction cavity through a pipeline.
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Description

Technical Field

[0001] This invention relates to the field of photocatalytic conversion technology, and in particular to a large-area mobile phase photocatalytic reaction device. Background Technology

[0002] Since catalytically converting various inert small molecules such as carbon dioxide and methane into high-value-added fuels can both alleviate the greenhouse effect and solve the energy shortage problem, how to effectively convert these gases into high-value-added fuels on a large scale has become an important research direction.

[0003] Currently, industrial processes primarily utilize high temperature and pressure to convert gases such as carbon dioxide and methane. However, these methods require substantial energy resources, leading to high costs and a tendency for fuel consumption to exceed fuel production. Furthermore, methane and other gases react under these conditions to produce carbon dioxide, causing secondary pollution. Therefore, efforts are underway to explore batch reactors or small-scale laboratory mobile phase reactions using catalysts and light to convert carbon dioxide and methane, effectively avoiding the problems of high costs and secondary pollution.

[0004] However, this method is still only at the laboratory stage. Due to limitations such as volume, its reaction efficiency is low, and it can only convert a small amount of carbon dioxide and methane, making it impossible to achieve efficient large-scale conversion. Summary of the Invention

[0005] In view of the shortcomings of the prior art, this application provides a large-area mobile phase photocatalytic reaction device to solve the problems of low efficiency and small scale of the existing technology in converting small molecules.

[0006] To achieve the above objectives, this application provides the following technical solution:

[0007] This application provides a large-area mobile phase photocatalytic reaction device, comprising:

[0008] Catalytic system and gas-liquid flow guiding system;

[0009] The catalytic system includes a light source power supply device, a dark box, a photocatalytic reactor and multiple light sources disposed in the dark box;

[0010] The light source power supply device is used to provide electrical energy to each of the light sources;

[0011] The photocatalytic reactor is equipped with a reaction chamber;

[0012] The photocatalytic reactor has a raw material inlet and a product outlet at both ends of the reaction chamber, and the reaction chamber is provided with a photocatalytic coating layer for coating the photocatalyst.

[0013] The upward-facing side of the reaction chamber in the photocatalytic reactor is a quartz viewing window;

[0014] Each of the light sources is positioned above the quartz window to irradiate light onto the reaction chamber through the quartz window, so that the raw materials in the reaction chamber react under the action of light and photocatalyst.

[0015] The gas-liquid diversion system includes a gas-liquid inlet system and a gas-liquid outlet system;

[0016] The gas-liquid introduction system includes a raw material supply device and a bubbling device;

[0017] The outlet of the bubbling device is positioned higher than the liquid level in the bubbling device, and is sealed and connected to the raw material inlet of the reaction chamber via a conduit;

[0018] The raw material supply device is connected to the bubbling device through a conduit, and one end of the conduit connected to the bubbling device is inserted below the liquid surface in the bubbling device, so that the gaseous raw material discharged from the raw material supply device is moistened by the liquid in the bubbling device and then discharged into the reaction chamber for reaction.

[0019] The inlet of the gas-liquid extraction system is connected to the product outlet of the reaction chamber via a conduit, and is used to collect the gas and liquid discharged from the reaction chamber.

[0020] Optionally, in the above-described large-area mobile phase photocatalytic reaction device, the gas-liquid extraction system includes:

[0021] Liquid collection devices, gas collection devices, and detection devices;

[0022] The inlet of the liquid collection device is sealed and connected to the product outlet of the reaction chamber through a conduit, and is used to collect the liquid discharged from the reaction chamber;

[0023] The inlet of the gas collection device and the outlet of the liquid collection device are connected by a conduit to collect the gas discharged from the reaction chamber;

[0024] The inlet of the detection device is connected to the outlet of the gas collection device via a conduit, and is used to detect the gas and liquid discharged from the reaction chamber.

[0025] Optionally, the above-described large-area mobile phase photocatalytic reaction device further includes:

[0026] A valve is provided on the conduit connecting the liquid collection device and the reaction chamber, the conduit connecting the gas collection device and the liquid collection device, and the conduit connecting the detection device and the gas collection device.

[0027] Optionally, the above-described large-area mobile phase photocatalytic reaction device further includes:

[0028] A lifting device located below the photocatalytic reactor is used to adjust the distance between the photocatalytic reactor and each of the light sources.

[0029] Optionally, the above-described large-area mobile phase photocatalytic reaction device further includes:

[0030] An input control device is installed on the conduit connecting the raw material supply device and the bubbling device to control the flow rate of the gas output by the raw material supply device.

[0031] Optionally, in the above-described large-area mobile phase photocatalytic reaction apparatus, the input control device includes:

[0032] Mass flow meters, mass controllers, and flow rate displays;

[0033] The mass flow meter is either an online gas mass flow meter or an offline gas mass flow meter, used to measure the flow rate of the gas output from the raw material supply device;

[0034] The quality controller is used to control the flow rate of the gas output by the raw material supply device, so as to control the flow rate of the gas output by the raw material supply device.

[0035] The flow rate display is used to display the flow rate of the gas output from the raw material supply device.

[0036] Optionally, the above-described large-area mobile phase photocatalytic reaction device further includes:

[0037] A valve is provided on the conduit connecting the input control device and the bubbling device, and on the conduit connecting the bubbling device and the reaction chamber.

[0038] Optionally, in the above-described large-area mobile phase photocatalytic reaction device, the gas-liquid introduction system further includes:

[0039] Switch valve;

[0040] The switching valve is connected to the outlet conduit of the raw material supply device, the inlet and outlet conduits of the bubbling device, and the raw material inlet of the reaction chamber. Before the photocatalytic reaction begins, the outlet conduit of the raw material supply device is connected to the raw material inlet conduit of the reaction chamber to expel air from the reaction chamber using gas discharged from the raw material supply device. At the start of the photocatalytic reaction, the outlet conduit of the raw material supply device is connected to the inlet conduit of the bubbling device, and the outlet conduit of the bubbling device is connected to the raw material inlet conduit of the reaction chamber to wet the gaseous raw material discharged from the raw material supply device with liquid from the bubbling device before it is discharged into the reaction chamber for reaction.

[0041] Optionally, in the above-described large-area mobile phase photocatalytic reaction device, the bubbling device further includes:

[0042] A liquid discharge valve is located at the lower end of the bubbling device, and a circulating water system is located outside the bubbling device;

[0043] The circulating water system controls the temperature of the liquid in the bubbling device by circulating the liquid within it.

[0044] Optionally, in the above-described large-area mobile phase photocatalytic reaction device, the quartz window is a detachable component, so that the photocatalytic coating can be replaced by removing the quartz window.

[0045] This application provides a large-area mobile phase photocatalytic reaction device, including a catalytic system and a gas-liquid flow system. The catalytic system includes a light source power supply device, a dark chamber, a photocatalytic reactor housed in the dark chamber, and multiple light sources. The light source power supply device provides electrical energy to each light source. The photocatalytic reactor is provided with a reaction chamber. The reaction chamber in the photocatalytic reactor has a raw material inlet and a product outlet at both ends, and a photocatalytic coating layer for coating a photocatalyst is provided in the reaction chamber. The upward-facing side of the reaction chamber in the photocatalytic reactor is a quartz window. Each light source is positioned above the quartz window to irradiate light into the reaction chamber through the quartz window, so that the raw materials in the reaction chamber react under the action of light and the photocatalyst. The gas-liquid flow system includes a gas-liquid inlet system and a gas-liquid outlet system. The gas-liquid inlet system includes a raw material supply device and a bubbling device. The outlet of the bubbling device is positioned higher than the liquid level in the bubbling device and is sealed and connected to the raw material inlet of the reaction chamber through a conduit. The raw material supply device and the bubbling device are connected via a conduit, with one end of the conduit connected to the bubbling device submerged below the liquid surface in the bubbling device. This allows the liquid in the bubbling device to wet the gaseous raw material discharged from the raw material supply device before it is discharged into the reaction chamber for reaction. The inlet of the gas-liquid outlet system is connected to the product outlet of the reaction chamber via a conduit, used to collect the gas and liquid discharged from the reaction chamber. Therefore, the bubbling device allows a large amount of reaction gas to be fully wetted, enabling sufficient contact and mixing of the gas and liquid two-phase reactants, ensuring efficient subsequent reaction. Furthermore, the large-area reaction chamber can handle a large amount of reaction gas and receive extensive light, and the photocatalytic coating ensures sufficient contact between the reactants and the catalyst, guaranteeing efficient reaction and achieving large-scale conversion of gases such as carbon dioxide and methane. Attached Figure Description

[0046] To more clearly illustrate the technical solutions in the embodiments of this application 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 this application. For those skilled in the art, other drawings can be obtained based on the provided drawings without creative effort.

[0047] Figure 1 A schematic diagram of a large-area mobile phase photocatalytic reaction device provided in this application embodiment;

[0048] Figure 2 A schematic diagram of another large-area mobile phase photocatalytic reaction device provided in another embodiment of this application;

[0049] Figure 3This application provides a schematic diagram illustrating the reduction performance of an example of catalyzing carbon dioxide using a large-area mobile phase photocatalytic reactor provided in this application embodiment.

[0050] Figure 4 This application provides a schematic diagram illustrating the reduction stability of an example of catalyzing carbon dioxide using a large-area mobile phase photocatalytic reactor provided in this application embodiment.

[0051] Figure 5 A schematic diagram illustrating the reduction performance of an example of photocatalytic carbon dioxide using an intermittent reactor, provided as an embodiment of this application;

[0052] Figure 6 A schematic diagram illustrating the reduction stability of an example of photocatalytic carbon dioxide using a batch reactor, provided as an embodiment of this application;

[0053] Figure 7 This application provides a schematic diagram illustrating the reduction performance of an example of methane catalysis using a large-area mobile phase photocatalytic reactor provided in this application embodiment.

[0054] Figure 8 This application provides a schematic diagram illustrating the reduction stability of an example of methane catalysis using a large-area mobile phase photocatalytic reactor provided in this application embodiment.

[0055] Figure 9 A schematic diagram illustrating the reduction performance of an example of photocatalytic methane using a batch reactor, provided as an embodiment of this application. Detailed Implementation

[0056] The technical solutions of the embodiments of this application will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of this application, and not all embodiments. Based on the embodiments of this application, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of this application.

[0057] In this application, relational terms such as "first" and "second" are used merely to distinguish one entity or operation from another, and do not necessarily require or imply any such actual relationship or order between these entities or operations. Furthermore, the terms "comprising," "including," or any other variations thereof are intended to cover non-exclusive inclusion, such that a process, method, article, or apparatus that comprises a list of elements includes not only those elements but also other elements not expressly listed, or elements inherent to such a process, method, article, or apparatus. Without further limitation, an element defined by the phrase "comprising one..." does not exclude the presence of other identical elements in the process, method, article, or apparatus that includes said element.

[0058] This application provides a large-area mobile phase photocatalytic reaction device, such as... Figure 1 As shown, it specifically includes:

[0059] Catalytic system and gas-liquid flow system.

[0060] The catalytic system includes a light source power supply device 101, a dark box 102, a photocatalytic reactor 103 disposed in the dark box 102, and multiple light sources 104.

[0061] The power supply unit 101 is used to provide electrical energy to each light source. It can also be used to control the switching on and off of each light source, thus allowing control over which light sources need to be turned on according to current requirements.

[0062] Optionally, the various light sources 104 can be configured as parallel light sources. Furthermore, the power and type of the light sources 104 can be selected according to requirements. Specifically, various monochromatic light sources such as xenon lamps, mercury lamps, and LEDs can be used. In addition, the range of light emitted by each light source 104 can be adjusted according to actual operating conditions, typically within the range of 200nm-2000nm. The required range can also be adjusted by adding filters.

[0063] The photocatalytic reactor 103 is provided with a reaction chamber 1031. The reaction chamber 1031 has a raw material inlet and a product outlet at both ends, used for introducing the raw materials to be reacted and discharging the reaction products, respectively. Therefore, apart from the raw material inlet and product outlet, the reaction chamber 1031 is a sealed space to prevent leakage of reaction gases. Furthermore, a photocatalytic coating layer 1032 is provided in the reaction chamber 1031 for coating the photocatalyst, providing a catalyst for the photocatalytic reaction. Therefore, to ensure reaction efficiency, the catalyst on the photocatalytic coating layer 1032 needs to be uniformly coated.

[0064] It should be noted that the volume of the reaction chamber 1031 can be set according to requirements, but the reaction efficiency must be considered, and the photocatalytic reactor 103 needs to be set accordingly. For example, it can be set to a commonly used photocatalytic reaction chamber 1031 with a volume of 10cm*10cm to 100cm*cm. The material of the tank of the reaction chamber 1031 needs to be selected to be high temperature resistant and corrosion resistant, and cannot react with the reactants, products, or other raw materials.

[0065] The upward-facing side of the reaction chamber 1031 in the photocatalytic reactor 103 is configured as a quartz window 1033. Each light source 104 is positioned above the quartz window 1033 to irradiate light onto the reaction chamber 1031 through the quartz window 1033, so that the raw materials in the reaction chamber 1031 react under the action of light and photocatalyst.

[0066] It should be noted that the quartz window 1033 is usually made of quartz, but other light-transmitting materials can be selected according to requirements.

[0067] like Figure 1 As shown, the gas-liquid diversion system includes a gas-liquid inlet system 105 and a gas-liquid outlet system 106.

[0068] The gas-liquid introduction system 105 includes a raw material supply device 107 and a bubbling device 108.

[0069] The outlet of the bubbling device 108 is higher than the liquid level in the bubbling device 108, and is sealed and connected to the raw material inlet of the reaction chamber 1031 through a conduit, so that the gas passing through the bubbling device 108 can be introduced into the reaction chamber 1031, and the liquid in the bubbling device 108 can be prevented from flowing directly into the reaction chamber 1031.

[0070] The raw material supply device 107 and the bubbling device 108 are connected by a conduit, and one end of the conduit connected to the bubbling device 108 is inserted below the liquid surface in the bubbling device 108. This allows the gaseous raw material discharged from the raw material supply device 107 to be moistened by the liquid in the bubbling device 108 before being discharged into the reaction chamber 1031 for reaction. In other words, the gas discharged from the raw material supply device 107 will enter the liquid in the bubbling device 108, be moistened by the liquid, and then flow from the outlet of the bubbling device 108 into the reaction chamber 1031 for reaction.

[0071] The liquid in the bubbling device 108 is either a reactant liquid or an oxidant required in the photocatalytic reaction process. Specifically, the appropriate liquid can be placed according to the reaction requirements of the gaseous raw material to be converted. For example, when reducing carbon dioxide, liquids such as water, ethylene glycol, and formaldehyde can be added to the bubbler to fully mix and contact with the carbon dioxide, thereby promoting the efficiency of carbon dioxide photoconversion.

[0072] It should be noted that the raw material supply device 107 contains the gaseous raw materials that need to be reacted, such as carbon dioxide and methane. Therefore, gas cylinders are usually used as the raw material supply device 107.

[0073] like Figure 1 As shown, the inlet of the gas-liquid extraction system 106 is connected to the product outlet of the reaction chamber 1031 through a conduit, which is used to collect the gas and liquid discharged from the reaction chamber 1031.

[0074] Therefore, specifically, when using the large-area mobile phase photocatalytic reactor provided in this application embodiment for conversion, the gaseous raw material is discharged from the raw material supply device 107. The gaseous raw material flows into the liquid in the bubbling device 108, and after being wetted by the liquid in the bubbling device 108, the gas-liquid mixture is discharged from the outlet of the bubbling device 108 and sent into the reaction chamber 1031 of the photocatalytic reactor 103 in the dark box 102. The gas-liquid mixture comes into contact with the photocatalyst on the photocatalytic coating layer 1032 in the reaction chamber 1031. At this time, various light sources irradiate the reactants in the reaction chamber 1031 through the quartz window 1033 on the reaction chamber 1031, causing them to react under the action of the catalyst and light. Finally, the gas and liquid generated by the reaction are discharged to the gas-liquid exhaust system 106 for collection.

[0075] This application provides a large-area mobile phase photocatalytic reaction device, including a catalytic system and a gas-liquid flow system. The catalytic system includes a light source power supply device, a dark chamber, a photocatalytic reactor housed within the dark chamber, and multiple light sources. The light source power supply device provides electrical energy to each light source. The photocatalytic reactor has a reaction chamber. The reaction chamber in the photocatalytic reactor has a raw material inlet and a product outlet at both ends, and a photocatalytic coating layer for coating a photocatalyst is provided within the reaction chamber. The upward-facing side of the reaction chamber in the photocatalytic reactor is a quartz window. Each light source is positioned above the quartz window to irradiate light into the reaction chamber through the quartz window, causing the raw materials in the reaction chamber to react under the action of light and the photocatalyst. The gas-liquid flow system includes a gas-liquid inlet system and a gas-liquid outlet system. The gas-liquid inlet system includes a raw material supply device and a bubbling device. The outlet of the bubbling device is positioned higher than the liquid level in the bubbling device and is sealed and connected to the raw material inlet of the reaction chamber via a conduit. The raw material supply device and the bubbling device are connected via a conduit, with one end of the conduit connected to the bubbling device submerged below the liquid surface in the bubbling device. This allows the liquid in the bubbling device to wet the gaseous raw material discharged from the raw material supply device before it is discharged into the reaction chamber for reaction. The inlet of the gas-liquid outlet system is connected to the product outlet of the reaction chamber via a conduit, used to collect the gas and liquid discharged from the reaction chamber. Therefore, the bubbling device allows a large amount of reaction gas to be fully wetted, enabling sufficient contact and mixing of the gas and liquid two-phase reactants, ensuring efficient subsequent reaction. Furthermore, the large-area reaction chamber can handle a large amount of reaction gas and receive extensive light, and the photocatalytic coating ensures sufficient contact between the reactants and the catalyst, guaranteeing efficient reaction and achieving large-scale conversion of gases such as carbon dioxide and methane.

[0076] Another embodiment of this application provides another large-area mobile phase photocatalytic reaction device, such as... Figure 2 As shown, it includes:

[0077] Catalytic system and gas-liquid flow system.

[0078] The catalytic system includes a light source 204, a power supply device 201, a dark box 202, a photocatalytic reactor 203 disposed in the dark box 202, and multiple light sources 204.

[0079] The power supply unit 201 for the light source 204 is used to provide electrical energy to each light source 204.

[0080] The photocatalytic reactor 203 is equipped with a reaction chamber 205.

[0081] The reaction chamber 205 in the photocatalytic reactor 203 is provided with a raw material inlet and a product outlet at both ends, and a photocatalytic coating layer 206 for coating the photocatalyst is provided in the reaction chamber 205.

[0082] The upward-facing side of the reaction chamber 205 in the photocatalytic reactor 203 is a quartz window 207.

[0083] Each light source 204 is positioned above the quartz window 207 to irradiate light onto the reaction chamber 205 through the quartz window 207, so that the raw materials in the reaction chamber 205 react under the action of light and photocatalyst.

[0084] It should be noted that, in order to facilitate the replacement of the photocatalytic coating layer 206, the quartz window 207 is a detachable component in this embodiment, so that the photocatalytic coating layer 206 can be replaced by removing the quartz window 207. Of course, the quartz window 207 can also be a fixed component, and then components for replacing the photocatalytic coating layer 206 can be provided elsewhere in the photocatalytic reactor 203.

[0085] Optionally, in this embodiment of the application, a lifting device is also provided below the photocatalytic reactor 203 to adjust the distance between the photocatalytic reactor 203 and each light source 204.

[0086] The gas-liquid diversion system includes a gas-liquid inlet system and a gas-liquid outlet system.

[0087] The gas-liquid introduction system includes a raw material supply device 208 and a bubbling device 209.

[0088] The outlet of the bubbling device 209 is higher than the liquid level in the bubbling device 209, and is sealed and connected to the raw material inlet of the reaction chamber 205 through a conduit.

[0089] In this embodiment, a liquid discharge 2091 is provided at the lower end of the bubbling device 209 to facilitate the discharge of liquid from the bubbling device 209. Furthermore, a circulating water system 2092 is located outside the bubbling device 209.

[0090] The circulating water system 2092 controls the temperature of the liquid in the bubbling device 209 by circulating the liquid within it. Specifically, the circulating liquid in the circulating water system 2092 exchanges heat with the bubbling device 209, thereby regulating the liquid content within the bubbling device 209. The temperature and flow rate of the circulating liquid can be adjusted to achieve the desired temperature within the bubbling device 209, further improving the reaction efficiency of the subsequent gas-liquid mixture.

[0091] The raw material supply device 208 and the bubbling device 209 are connected by a conduit, and one end of the conduit connected to the bubbling device 209 is inserted below the liquid surface in the bubbling device 209 so that the gaseous raw material discharged from the raw material supply device 208 is moistened by the liquid in the bubbling device 209 and then discharged into the reaction chamber 205 for reaction.

[0092] Specifically, in this embodiment, the raw material supply device 208 and the bubbling device 209 are connected via a switching valve 301, that is, the switching valve 301 connects the outlet conduit of the raw material supply device 208 to the inlet conduit of the bubbling device 209. The outlet conduit of the raw material supply device 208 refers to the conduit connected to the outlet of the raw material supply device 208. The inlet conduit of the bubbling device 209 refers to the conduit at the inlet of the bubbling device 209, so one end of the inlet is below the liquid level in the bubbling device 209.

[0093] Furthermore, the switching valve 301 connects not only the outlet conduit of the raw material supply device 208 and the inlet conduit of the bubbling device 209, but also the outlet conduit of the bubbling device 209 and the raw material inlet of the reaction chamber 205.

[0094] Specifically, the switching valve 301 is used to connect the outlet conduit of the raw material supply device 208 to the raw material inlet conduit of the reaction chamber 205 before the photocatalytic reaction begins. This allows the air in the reaction chamber 205 to be discharged through the gas discharged from the raw material supply device 208. In other words, the gas discharged from the raw material supply device 208 will directly enter the reaction chamber 205 and will not enter the bubbling device 209. This utilizes relatively dry gas to remove air from the reaction chamber 205, avoiding interference with subsequent reactions. At the start of the photocatalytic reaction, the outlet conduit of the raw material supply device 208 is connected to the inlet conduit of the bubbling device 209, and the outlet conduit of the bubbling device 209 is connected to the raw material inlet conduit of the reaction chamber 205. This allows the gas discharged from the raw material supply device 208 to be moistened by the liquid in the bubbling device 209 before being discharged into the reaction chamber 205 for reaction.

[0095] Optionally, in order to control the flow rate of the gas output from the raw material supply device 208, such as... Figure 2 As shown, it also includes an input control device 2081 disposed on the conduit connecting the raw material supply device 208 and the bubbling device 209, for controlling the flow rate of the gas output by the raw material supply device 208.

[0096] The input control device 2081 includes:

[0097] Mass flow meters, mass controllers, and flow rate displays.

[0098] The mass flow meter is either an online gas mass flow meter or an offline gas mass flow meter, used to measure the flow rate of the gas output from the raw material supply device 208.

[0099] The quality controller is used to control the flow rate of the gas output from the raw material supply device 208, thereby controlling the flow rate of the gas output from the raw material supply device 208. Optionally, the flow rate of the reaction gas is typically controlled between 10 sccm and 100 sccm. In actual operation, the operator can adjust this according to the type of reaction. For example, when using this device for a carbon dioxide reduction reaction, the flow rate of the reaction gas (carbon dioxide) should be adjusted to be lower than that of the reaction gas (methane) during a methane oxidation reaction.

[0100] The flow rate display is used to display the flow rate of the gas output from the raw material supply device 208.

[0101] Optionally, since the gas pressure output by the raw material supply device 208 is usually relatively high, a pressure relief valve 302 can be provided before the input control device 2081 to reduce the pressure of the output gas.

[0102] Optionally, in order to control the gas flow rate into the bubbling device 209 and the flow rate into the reaction chamber, in this embodiment of the application, a valve 303 is provided on the conduit connecting the input control device 2081 and the bubbling device 209, and a valve 304 is provided on the conduit connecting the bubbling device 209 and the reaction chamber 205.

[0103] The inlet of the gas-liquid extraction system is connected to the product outlet of the reaction chamber 205 via a conduit, which is used to collect the gas and liquid discharged from the reaction chamber 205.

[0104] Alternatively, see also Figure 2 In this embodiment of the application, the gas-liquid extraction system includes:

[0105] Liquid collection device 210, gas collection device 211 and detection device 212.

[0106] Therefore, in this embodiment of the application, corresponding devices are provided for collecting liquid and gas respectively, and a detection device 212 is also provided to understand the reaction situation.

[0107] like Figure 2 As shown, the inlet of the liquid collection device 210 is sealed and connected to the product outlet of the reaction chamber 205 through a conduit, which is used to collect the liquid discharged from the reaction chamber 205.

[0108] The inlet of the gas collection device 211 is connected to the outlet of the liquid collection device 210 through a conduit, and is used to collect the gas discharged from the reaction chamber 205.

[0109] The inlet of the detection device 212 is connected to the outlet of the gas collection device 211 through a conduit, and is used to detect the gas and liquid discharged from the reaction chamber 205.

[0110] Optionally, such as Figure 2 As shown in this embodiment, a valve 305 is provided on the conduit connecting the liquid collection device 210 and the reaction chamber 205. A valve 306 is provided on the conduit connecting the gas collection device 211 and the liquid collection device 210. A valve 307 is provided on the conduit connecting the detection device 212 and the gas collection device 211.

[0111] The valve 305 on the conduit connecting the liquid collection device 210 and the reaction chamber 205 controls the flow rate of gas discharged from the reaction chamber 205. Similarly, the valve 306 on the conduit connecting the gas collection device 211 and the liquid collection device 210 regulates the gas flow rate and prevents liquid from entering the gas collection device 211, or can be closed when gas collection is not required or when separate collection is not necessary. The valve 307 on the conduit connecting the detection device 212 and the gas collection device 211 is opened when detection is needed and closed when detection is not needed.

[0112] It should also be noted that the gas conduits connecting the various devices in this embodiment are typically rigid pipes, and the material can be flexibly selected according to the reaction type, as long as it ensures no leakage and that the reaction gases and products will not react with it. For example, polytetrafluoroethylene (PTFE) can be used. Furthermore, for ease of assembly and disassembly, the various components connected by the gas conduits can be connected and disassembled using corresponding connectors.

[0113] To verify the advantages of the device provided in this application, a practical application of carbon dioxide was also conducted. Specifically, the reaction chamber was selected to be 20cm*20cm in size, and a xenon lamp was selected as the parallel light source. The process was controlled by a pressure reducing valve and an input control device on the carbon dioxide-containing raw material supply device. Carbon dioxide gas was introduced into the bubbling device through a conduit. The bubbling device contained purified water to wet the carbon dioxide, and the water temperature within the bubbling device was controlled by a circulating water system. Palladium-supported zinc oxide nanosheets were coated onto the photocatalytic coating layer. Under dark conditions, the carbon dioxide gas flow rate was maintained at 20 ml / min for 15 minutes to remove air from the reaction chamber. Then, the light source was turned on, and the 200nm–800nm ​​full-spectrum light emitted by a 300W xenon lamp was transmitted through a quartz window to the catalyst surface. Under the simultaneous action of the photo-decomposed water, the carbon dioxide gas flowing across the catalyst surface, and the catalyst, the reaction time was 4 hours, producing high-value methane products. During the reaction, the reaction products enter the detection device through a gas conduit, specifically a gas chromatograph, for detection. The methane production rate and selectivity can then be calculated.

[0114] like Figure 3As shown, using the large-area mobile phase photocatalytic reactor provided in this application embodiment, the reaction was carried out under the above conditions, and the yields of methane and carbon monoxide were 670.3 and 33.1 μmol / g catalyst per hour, respectively. Furthermore, as... Figure 4 The yield of the product shown in the embodiment of this application demonstrates that, within a 24-hour reaction period, the methane production rate did not decrease significantly. Therefore, based on... Figure 3 and Figure 4 As can be seen, with the driving speed of the reactant gas flow rate remaining constant, the device provided in this embodiment achieves a methane production rate of up to 670 micromoles per gram of catalyst per hour over 4 hours, which is far higher than the 260 micromoles per gram of catalyst per hour under a batch reactor. Furthermore, the large-area mobile phase photocatalytic reactor provided in this embodiment can operate continuously for 24 hours without a significant decrease in the methane production rate.

[0115] For carbon dioxide reduction using a traditional batch reactor, 10 mg of synthesized zinc oxide nanosheets were dissolved in 4 mL of water to obtain a suspension, which was then uniformly dropped onto a quartz glass plate. The quartz glass plate was then placed in the batch reactor, with 5 mL of water added to the bottom. Initially, the reaction tank was purified by multiple pumping of carbon dioxide, and high-purity carbon dioxide was introduced to reach ambient pressure. A 300-watt xenon lamp equipped with a standard AM1.5G filter was used as the light source, with an output optical density of approximately 100 milliwatts per square centimeter. The reaction time was 4 hours, and the reaction products were detected using the same gas chromatograph. The same method was used, but 10 mg of synthesized palladium-loaded zinc oxide nanosheets were dissolved in 4 mL of water to obtain a suspension, and the reaction was also carried out for 4 hours. Figure 5 The figure shows the yields of products obtained by reacting with two types of zinc oxide nanosheets in a conventional batch reactor. It can be seen that when using zinc oxide nanosheets directly, the yield of carbon monoxide is 13.2 μmol / g catalyst per hour. However, when using palladium-supported zinc oxide nanosheets, the yields of methane and carbon monoxide are 257.4 and 12.6 μmol / g catalyst per hour, respectively. These yields are lower than those obtained using the apparatus provided in this scheme. Furthermore, according to... Figure 6 As shown, in the yield of the cyclic test using palladium-supported zinc oxide nanosheets, it can be seen that its performance has already deteriorated significantly after only 8 hours.

[0116] To demonstrate that the device provided in this application embodiment can achieve the same effect on other gases, this application embodiment also utilizes the device to convert methane. Specifically, the reaction chamber is 20cm*20cm in size, and a xenon lamp is selected as the parallel light source. The process is controlled by a pressure reducing valve and an input control device on the raw material supply device containing methane. Methane gas is introduced into the bubbling device through a conduit. The bubbling device contains hydrogen peroxide to wet the carbon dioxide, and the liquid temperature inside the bubbling device is controlled by a circulating water system. Gold-loaded tungsten oxide nanosheets are coated onto the photocatalytic coating layer. Under dark conditions, the carbon dioxide gas flow rate is maintained at 15 ml / min for 15 minutes to remove air from the reaction chamber. Then, the light source is turned on, and the 200nm–800nm ​​full-spectrum light emitted by a 300W xenon lamp light source passes through a quartz window to the catalyst surface. Under the simultaneous action of the photo-decomposed hydrogen peroxide, the methane gas flowing over the catalyst surface, and the catalyst, the reaction takes 4 hours to produce a high-value ethane product. During the reaction, the reaction products enter the detection device through a gas conduit, specifically a gas chromatograph, for detection. The methane production rate and selectivity can then be calculated.

[0117] like Figure 7 As shown, in this reaction process, the yields of ethane and carbon monoxide were 6816.8 and 354.7 μmol / g of catalyst per hour, respectively. And as... Figure 8 As shown, the ethane production rate did not decrease significantly during a continuous 21-hour reaction in this device. Therefore, it is evident that the hourly ethane production rate reached 6816.8 μmol / g catalyst within 4 hours, far exceeding the ethane yield of 911.7 μmol / g catalyst in a batch reactor. Furthermore, the large-area mobile phase photocatalytic reactor provided in this application embodiment allows for a continuous 21-hour reaction without a significant decrease in the ethane production rate.

[0118] The photocatalytic methane oxidation process in a traditional batch reactor is as follows: 10 mg of synthesized tungsten oxide nanosheets are dissolved in 4 mL of water to obtain a suspension, which is then uniformly dropped onto a quartz glass plate. The quartz glass plate is then placed in the batch reactor, with 5 mL of water added to the bottom. Initially, the reaction tank is purified by multiple pumping cycles of methane, and high-purity methane is introduced to reach ambient pressure. A 300-watt xenon lamp equipped with a standard AM1.5G filter is used as the light source, producing an output light density of approximately 100 milliwatts per square centimeter. The reaction time is 4 hours, and the reaction products are detected using gas chromatography. Figure 9 As shown, the yield of carbon monoxide obtained under these conditions is only 460.0 micromoles per gram of catalyst per hour, which is far lower than the yield of the apparatus provided in the embodiments of this application.

[0119] For photocatalytic methane oxidation in a traditional batch reactor, the following conversion scheme is used: 10 mg of synthetic gold-loaded tungsten oxide is dissolved in 4 mL of water to obtain a suspension, which is then uniformly dropped onto a quartz glass plate. The quartz glass plate is then placed in the batch reactor, with 5 mL of water added to the bottom. Initially, the reaction tank is purified by multiple pumping of methane, and high-purity methane is introduced to reach ambient pressure. A 300W xenon lamp equipped with a standard AM1.5G filter is used as the light source, with an output light density of approximately 100 mW / cm². The reaction time is 4 hours, and the reaction products are detected using gas chromatography (i.e., the reaction is carried out using gold-loaded tungsten oxide).

[0120] like Figure 9 As shown, the hourly yields of ethane and carbon monoxide obtained under these conditions are 911.7 and 122.8 μmol per gram of catalyst, respectively, which are still far lower than the 6816.8 and 354.7 μmol per gram of catalyst in this scheme.

[0121] Therefore, using the large-area mobile phase photocatalytic reactor disclosed in the embodiments of this application for photocatalytic carbon dioxide reduction or photocatalytic methane oxidation, both the production rate, selectivity, and stability are significantly improved compared to existing technologies. Furthermore, the ability to perform a continuous and coherent reaction effectively improves the reaction efficiency of photocatalytic carbon dioxide, enabling the photocatalytic reaction to be applied on a large scale in practical applications.

[0122] Those skilled in the art will further recognize that the units and algorithm steps of the various examples described in conjunction with the embodiments disclosed herein can be implemented in electronic hardware, computer software, or a combination of both. To clearly illustrate the interchangeability of hardware and software, the components and steps of the various examples have been generally described in terms of functionality in the foregoing description. Whether these functions are implemented in hardware or software depends on the specific application and design constraints of the technical solution. Those skilled in the art can use different methods to implement the described functions for each specific application, but such implementation should not be considered beyond the scope of this application.

[0123] The above description of the disclosed embodiments enables those skilled in the art to make or use this application. Various modifications to these embodiments will be readily apparent to those skilled in the art, and the general principles defined herein may be implemented in other embodiments without departing from the spirit or scope of this application. Therefore, this application is not to be limited to the embodiments shown herein, but is to be accorded the widest scope consistent with the principles and novel features disclosed herein.

Claims

1. A large-area mobile phase photocatalytic reaction device, characterized in that, include: Catalytic system and gas-liquid flow guiding system; The catalytic system includes a light source power supply device, a dark box, a photocatalytic reactor and multiple light sources disposed in the dark box; A lifting device located below the photocatalytic reactor is used to adjust the distance between the photocatalytic reactor and each of the light sources; The light source power supply device is used to provide electrical energy to each of the light sources; The photocatalytic reactor is equipped with a reaction chamber; The photocatalytic reactor has a raw material inlet and a product outlet at both ends of the reaction chamber, and the reaction chamber is provided with a photocatalytic coating layer for coating the photocatalyst. The upward-facing side of the reaction chamber in the photocatalytic reactor is a quartz viewing window; Each of the light sources is positioned above the quartz window to irradiate light onto the reaction chamber through the quartz window, so that the raw materials in the reaction chamber react under the action of light and photocatalyst. The gas-liquid diversion system includes a gas-liquid inlet system and a gas-liquid outlet system; The gas-liquid introduction system includes a raw material supply device and a bubbling device; The outlet of the bubbling device is positioned higher than the liquid level in the bubbling device, and is sealed and connected to the raw material inlet of the reaction chamber via a conduit; The raw material supply device is connected to the bubbling device through a conduit, and one end of the conduit connected to the bubbling device is inserted below the liquid surface in the bubbling device, so that the gaseous raw material discharged from the raw material supply device is moistened by the liquid in the bubbling device and then discharged into the reaction chamber for reaction. The inlet of the gas-liquid extraction system is connected to the product outlet of the reaction chamber via a conduit, and is used to collect the gas and liquid discharged from the reaction chamber; The gas-liquid extraction system includes: Liquid collection devices, gas collection devices, and detection devices; The inlet of the liquid collection device is sealed and connected to the product outlet of the reaction chamber through a conduit, and is used to collect the liquid discharged from the reaction chamber; The inlet of the gas collection device and the outlet of the liquid collection device are connected by a conduit to collect the gas discharged from the reaction chamber; The inlet of the detection device is connected to the outlet of the gas collection device via a conduit, and is used to detect the gas and liquid discharged from the reaction chamber.

2. The apparatus according to claim 1, characterized in that, Also includes: A valve is provided on the conduit connecting the liquid collection device and the reaction chamber, the conduit connecting the gas collection device and the liquid collection device, and the conduit connecting the detection device and the gas collection device.

3. The apparatus according to claim 1, characterized in that, Also includes: An input control device is installed on the conduit connecting the raw material supply device and the bubbling device to control the flow rate of the gas output by the raw material supply device.

4. The apparatus according to claim 3, characterized in that, The input control device includes: Mass flow meters, mass controllers, and flow rate displays; The mass flow meter is either an online gas mass flow meter or an offline gas mass flow meter, used to measure the flow rate of the gas output from the raw material supply device; The quality controller is used to control the flow rate of the gas output by the raw material supply device, so as to control the flow rate of the gas output by the raw material supply device. The flow rate display is used to display the flow rate of the gas output from the raw material supply device.

5. The apparatus according to claim 3, characterized in that, Also includes: A valve is provided on the conduit connecting the input control device and the bubbling device, and on the conduit connecting the bubbling device and the reaction chamber.

6. The apparatus according to claim 1, characterized in that, The gas-liquid introduction system further includes: Switch valve; The switching valve is connected to the outlet conduit of the raw material supply device, the inlet and outlet conduits of the bubbling device, and the raw material inlet of the reaction chamber. Before the photocatalytic reaction begins, the outlet conduit of the raw material supply device is connected to the raw material inlet conduit of the reaction chamber to expel air from the reaction chamber using gas discharged from the raw material supply device. At the start of the photocatalytic reaction, the outlet conduit of the raw material supply device is connected to the inlet conduit of the bubbling device, and the outlet conduit of the bubbling device is connected to the raw material inlet conduit of the reaction chamber to wet the gaseous raw material discharged from the raw material supply device with liquid from the bubbling device before it is discharged into the reaction chamber for reaction.

7. The apparatus according to claim 1, characterized in that, The bubbling device further includes: A liquid discharge valve is located at the lower end of the bubbling device, and a circulating water system is located outside the bubbling device; The circulating water system controls the temperature of the liquid in the bubbling device by circulating the liquid within it.

8. The apparatus according to claim 1, characterized in that, The quartz window is a detachable component, allowing the photocatalytic coating layer to be replaced by removing the quartz window.

Citation Information

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