Temperature and humidity controllable flow tube reactor and atmospheric multiphase chemical reaction method thereof

Abstract

The application discloses a temperature and humidity controllable flow tube reaction device and an atmospheric multiphase chemical reaction method thereof, and belongs to the technical field of multiphase reactions of atmospheric aerosols. The device disclosed by the application is characterized in that the coated flow tube reactor can be easily disassembled, and can effectively extract the particulate matter coated on the inner surface from the flow tube, so that the product information of the particulate matter participating in the multiphase reaction can be obtained. The coated flow tube reactor is used in the application, and can be used for identifying the reaction gas uptake coefficient, and can be used for studying the gas-particle interface reaction and the particle reaction. The setting of the constant temperature water bath device, the ultraviolet light irradiation device and the humidity regulator can realize the action mechanism of humidity, temperature and ultraviolet light irradiation on the multiphase chemical reaction of atmospheric particulate matter.

Description

Temperature and humidity controllable flow tube reactor and its atmospheric multiphase chemical reaction method Technical Field

[0001] This invention belongs to the field of multiphase reaction technology of atmospheric aerosols, specifically relating to a temperature and humidity controllable flow tube reaction device and its atmospheric multiphase chemical reaction method. Background Technology

[0002] Particulate matter (PM2.5) is a major air pollutant, playing a significant role in urban air pollution and regional and global environmental issues. PM2.5 originates from a wide range of sources, primarily categorized as natural and anthropogenic. Natural sources include dust, sea salt, plant pollen, and bacteria, while anthropogenic sources include fossil fuel combustion, vehicle exhaust, and biomass burning. PM2.5 can also be generated from emitted gaseous pollutants through photochemical reactions. Furthermore, PM2.5 continues to undergo a series of atmospheric chemical reactions, altering its physical and chemical properties. The diverse physical and chemical characteristics and spatiotemporal variations of PM2.5 make it difficult to accurately estimate its impact on air quality, the environment, and human health. Elucidating the atmospheric chemical processes of PM2.5 is a crucial step in addressing these challenges. Among these processes, multiphase chemical reactions of PM2.5 are considered an important part of these processes and a key mechanism for PM2.5 pollution exceeding standards in my country, representing a frontier and focus of current atmospheric chemical research.

[0003] Due to the complexity and numerous influences of actual atmospheric conditions, studying the multiphase chemical reaction mechanisms of atmospheric particulate matter presents significant challenges. Laboratory simulations, which allow for the study of atmospheric chemical reactions under relatively stable and controllable conditions, are currently a commonly used method. Two commonly used reactors in laboratory simulations are the smog chamber and the oxidation flow tube reactor. However, both of these reactors require sophisticated equipment and are currently more often used for online characterization of gas-phase reactions that generate secondary organic aerosols.

[0004] Patent CN108435269A describes a multi-sheath atmospheric chemical laminar flow reaction system, which can be used for the nucleation of gaseous precursors into new particulate matter through a gas-particle conversion process. This system is simpler and easier to disassemble than smoke chambers and oxidation flow tube reactors, effectively reducing manufacturing and maintenance costs. However, this device is primarily designed for studying the nucleation process of gaseous precursors in atmospheric laminar flow reactions and is not suitable for studying multiphase chemical reactions of atmospheric particulate matter. Patent CN205607806 describes an environmental chamber simulating heterogeneous reactions of black carbon aerosols. This environmental chamber reaction system is small, simple to set up, and has good reproducibility, making it suitable for simulating atmospheric chemical reaction processes where black carbon aerosols are in a suspended state. However, this device exhibits wall effects during experiments, which can interfere with the experiments. Furthermore, suspended particles are not conducive to studying gas uptake coefficients, gas-particle interface reactions, and particulate reactions in multiphase chemical reaction processes of atmospheric particulate matter. The relevant literature (ACSEarth Space Chem, 2018, 2, 9, 904-914) describes a coated flow tube reactor, which can coat particulate matter on the inner surface of the reaction tube, which is beneficial for studying the reaction gas uptake coefficient in multiphase reaction processes. However, the flow tube and temperature control system of this device are fixed together, making it difficult to extract particulate matter and obtain information on the particulate products participating in the reaction. Summary of the Invention

[0005] In order to overcome the shortcomings of the prior art, the present invention aims to provide a temperature and humidity controllable flow tube reaction device and its atmospheric multiphase chemical reaction method, which solves the technical problems of existing reactors used for multiphase chemical reaction processes, such as easy wall effect, difficulty in extracting particulate matter, and difficulty in obtaining information on particulate matter products participating in the reaction.

[0006] To achieve the above objectives, the present invention employs the following technical solution:

[0007] This invention discloses a temperature and humidity controllable flow tube reactor, comprising a coated flow tube reactor, an insulated tube, an ultraviolet irradiation device, a humidity regulator, and a reaction gas generating system. The coated flow tube reactor has an inlet and an outlet at both ends, respectively. The coated flow tube reactor is nested inside the insulated tube. The insulated tube is placed inside the ultraviolet irradiation device. The reaction gas generating system is connected to the humidity regulator via its inlet.

[0008] The coated flow tube reactor is connected to a constant temperature water bath device to achieve temperature stability of the coated flow tube reactor.

[0009] Furthermore, the constant temperature water bath device includes an inlet, an outlet, and a constant temperature water bath device; the inlet and outlet are respectively located at both ends of the insulation pipe and are both connected to the constant temperature water bath device.

[0010] Furthermore, the ultraviolet irradiation device includes an ultraviolet lamp box and several ultraviolet lamps; the several ultraviolet lamps are fixed around the inside of the ultraviolet lamp box, and the heat preservation tube is placed inside the ultraviolet lamp box and surrounded by several ultraviolet lamps.

[0011] Furthermore, the ultraviolet light box is an ultraviolet lamp tube that emits a wavelength of 254 nanometers or 365 nanometers.

[0012] Furthermore, the reaction gas generating system includes a first gas cylinder, a second gas cylinder, a first mass flow controller, a second mass flow controller, and an ozone generator; the humidity regulator is a Nafion membrane tube humidity regulator; the outlet of the first gas cylinder is connected to the first mass flow controller and then connected to the inlet.

[0013] The second gas cylinder is connected to the second mass flow controller; the other end of the ozone generator is connected to one end of the Nafion membrane tube humidity regulator; the other end of the Nafion membrane tube humidity regulator is connected to the air inlet after merging the gas path of the second gas cylinder and the second mass flow controller.

[0014] The Nafion membrane tube humidity regulator is also provided with a humidity regulator inlet and a humidity regulator outlet at both ends, and both the humidity regulator inlet and outlet are connected to a small constant temperature water bath device.

[0015] Furthermore, a first three-way valve is provided between the other end of the ozone generator and the Nafion membrane tube humidity regulator; the inlet of the first three-way valve is connected to the other end of the ozone generator; downstream of one outlet of the first three-way valve, the main airflow path is sequentially connected to a third mass flow controller and one end of the Nafion membrane tube humidity regulator, and the other outlet is a bypass, on which a fourth mass flow controller is provided; a second three-way valve is provided at the other end of the Nafion membrane tube humidity regulator; the bypass and branch are merged through the second three-way valve, and then merged with the air path of the second gas cylinder and the second mass flow controller, and subsequently connected to the air inlet.

[0016] Furthermore, the bypass and branch lines are merged through the second three-way valve and then combined with the gas lines of the second gas cylinder and the second mass flow controller, which is achieved by setting a third three-way valve.

[0017] Furthermore, the air outlet is also connected to a humidity sensor; the outlet end of the humidity sensor is connected to a fourth three-way valve; the humidity sensor is connected to an ozone monitor, a nitrogen oxide monitor, or a waste gas treatment device as needed, depending on the fourth three-way valve.

[0018] This invention also discloses a method for performing atmospheric multiphase chemical reactions using the above-mentioned temperature and humidity controllable flow tube reaction apparatus, comprising the following steps:

[0019] First, the particulate matter to be tested is coated onto the inner wall of the flow tube reactor. Then, the flow tube reactor is embedded in the insulated tube. The reaction gas generation system is started to introduce gas into the flow tube reactor to react with the particulate matter to be tested. After the reaction is completed, the particulate matter product is collected.

[0020] Furthermore, the method for coating the test particles onto the inner wall of the flow tube reactor is as follows:

[0021] Inject 400–800 μL of the suspension of the test particles into the inner wall of the flow tube reactor. Then fix the flow tube reactor in the rotator and rotate it at a speed of 20–60 rpm. At the same time, dry pure nitrogen gas at a rate of 1–3 L / min is introduced into the air inlet of the flow tube reactor to dry the solution.

[0022] Compared with the prior art, the present invention has the following beneficial effects:

[0023] This invention discloses a temperature and humidity controllable flow tube reactor. The coated flow tube reactor is easily disassembled and can effectively extract particles coated on the inner surface of the flow tube, enabling the acquisition of product information from particles participating in multiphase reactions. This invention uses a coated flow tube reactor, which can be used to determine the gas uptake coefficient and to study gas-particle interface reactions and particle reactions. The constant temperature water bath, through inlet and outlet water circulation, provides a constant temperature water bath, maintaining the temperature stability of the coated flow tube reactor. This satisfies the need to investigate the effects of different temperature environments on multiphase chemical reactions of particulate matter and ensures that the reaction process proceeds at a fixed temperature. Furthermore, the device includes an ultraviolet light irradiation device, which can be used to investigate the mechanism of action of environmental conditions (including humidity, temperature, and ultraviolet light) on multiphase chemical reactions of atmospheric particulate matter. Simultaneously, the reaction gas generation system is connected to a humidity regulator, which can adjust the system humidity and can be used to investigate the effects of different humidity environments on multiphase chemical reactions of particulate matter.

[0024] Furthermore, the ultraviolet irradiation device is equipped with ultraviolet lamps with wavelengths of 254 nm or 365 nm, allowing for the activation of different numbers of lamps and the selection of whether to use ultraviolet irradiation, depending on different needs. The mass flow controller regulates the gas flow rate, and a small constant-temperature water bath regulates the amount of water entering the Nafion membrane tube, thus adjusting the system humidity. This can be used to investigate the effects of different humidity environments on multiphase chemical reactions of particulate matter.

[0025] The present invention also discloses a method for performing atmospheric multiphase chemical reactions using the above-mentioned device. This method enables temperature and humidity-controlled multiphase chemical reactions of particulate matter and allows for the collection and analysis of the reaction products. Attached Figure Description

[0026] Figure 1 is a schematic diagram of the structure of the temperature and humidity controllable flow tube reaction device disclosed in this invention;

[0027] Figure 2 is a graph showing the degree of nitration of atmospheric protein particles exposed to ozone and nitrogen dioxide, measured using the temperature and humidity controllable flow tube reaction device disclosed in this invention.

[0028] Wherein: a - Example 1; b - Example 2; Example 3;

[0029] 10-Coated flow tube reactor; 11-Air inlet; 12-Air outlet; 20-Insulation pipe; 21-Water inlet; 22-Water outlet; 23-Constant temperature water bath device; 30-UV lamp box; 31-UV lamp tube; 41-First gas cylinder; 42-Second gas cylinder; 43-First mass flow controller; 44-Second mass flow controller; 45-Ozone generator; 46-First three-way valve; 47-Second three-way valve; 48-Third three-way valve; 49-Fourth three-way valve; 50-Nafion membrane tube humidity regulator; 51-Humidity regulator inlet; 52-Humidity regulator outlet; 53-Third mass flow controller; 54-Fourth mass flow controller; 55-Small constant temperature water bath device; 60-Humidity sensor. Detailed Implementation

[0030] To enable those skilled in the art to better understand the present invention, the technical solutions of the present invention will be clearly and completely described below with reference to the accompanying drawings of the embodiments of the present invention. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort should fall within the scope of protection of the present invention.

[0031] It should be noted that the terms "first," "second," etc., in the specification, claims, and accompanying drawings of this invention are used to distinguish similar objects and are not necessarily used to describe a specific order or sequence. It should be understood that such data can be interchanged where appropriate so that the embodiments of the invention described herein can be implemented in orders other than those illustrated or described herein. Furthermore, the terms "comprising" and "having," and any variations thereof, are intended to cover a non-exclusive inclusion; for example, a process, method, system, product, or apparatus that comprises a series of steps or units is not necessarily limited to those steps or units explicitly listed, but may include other steps or units not explicitly listed or inherent to such processes, methods, products, or apparatus.

[0032] The present invention will now be described in further detail with reference to the accompanying drawings:

[0033] Referring to Figure 1, the temperature and humidity controllable flow tube reaction device disclosed in this invention includes a coated flow tube reactor 10, an insulation tube 20, an ultraviolet irradiation device, a humidity regulator, and a reaction gas generation system. The coated flow tube reactor 10 is nested inside the insulation tube 20, enabling quick installation and removal. The coated flow tube reactor 10 has an inlet 11 and an outlet 12 at both ends. The insulation tube 20 is placed inside the ultraviolet irradiation device. The reaction gas generation system is connected to the humidity regulator, and the inlet 11 is connected to the outlet. The coated flow tube reactor 10 is connected to a constant temperature water bath to stabilize its temperature.

[0034] It should be noted that before embedding the coated flow tube reactor 10 into the insulation tube 20, the particulate matter to be tested must first be coated onto the inner wall of the flow tube reactor 10. Specifically, 400-800 μL of a particulate matter suspension of a certain concentration is injected into the inner wall of the flow tube reactor 10. Then, the flow tube reactor 10 is fixed in the rotator and rotated at 20-60 rpm. At the same time, dry and pure nitrogen gas at a rate of 1-3 L / min is introduced into the air inlet of the flow tube reactor to dry the solution.

[0035] Based on the mass of the particles coated onto the inner wall of the flow tube reactor 10, the molecular radius of the particles, and the inner diameter and length of the flow tube, the number of particle layers coated onto the inner wall of the flow tube can be calculated using the following formula:

[0036] N = m P r 2 N A / (M P d i l);

[0037] Where N is the number of particulate layers, m p The mass of the particles injected into the inner wall of the flow tube is given by r, where r is the molecular radius of the particles, and N is the molecular radius of the particles. A M is Avogadro's constant. P d represents the molecular weight of the particulate matter. i Let be the inner diameter of the flow tube, and l be the length of the flow tube. Therefore, by changing the mass of the particles injected into the inner wall of the flow tube, the number of particle layers in the experiment can be adjusted, which can effectively explore interfacial and bulk reactions in multiphase chemical reactions of particulate matter.

[0038] The insulation pipe 20 is provided with an inlet 21 and an outlet 22 at both ends. Both the inlet 21 and the outlet 22 are connected to the constant temperature water bath device 23. Water circulation is formed through the inlet and outlet to provide a constant temperature water bath and maintain the temperature of the coated flow tube reactor. This can meet the needs of exploring the influence of different temperature environments on the multiphase chemical reaction of particulate matter and also ensure that the reaction process is carried out at a fixed temperature.

[0039] The heat-insulating tube 20, which is embedded in the coated flow tube reactor 10, is placed inside the ultraviolet lamp box 30, wherein six ultraviolet lamps 31 are arranged around the reaction device inside the ultraviolet lamp box; wherein the ultraviolet lamp box 30 and several ultraviolet lamps 31 constitute an ultraviolet light irradiation device.

[0040] Preferably, the ultraviolet lamp 31 can be selected with a wavelength of 254 nanometers or 365 nanometers according to actual needs. Additionally, different numbers of lamps can be turned on and ultraviolet irradiation can be selected depending on different needs. The light intensity needs to be measured beforehand using a radiometer, which is not described in this invention.

[0041] The air inlet 11 is connected to the reactant gas generation system, and the type of reactant gas can be selected according to requirements. When ozone and nitrogen dioxide are used as reactant gases, as shown in Figure 1, the first gas cylinder 41 and the second gas cylinder 42, the first mass flow controller 43 and the second mass flow controller 44, and the ozone generator 45 of the reactant gas generation system are opened in sequence. The first gas cylinder 41 contains synthetic clean air, and the gas flow rate is adjusted by the first mass flow controller 43. The ozone concentration is controlled by adjusting the length of the ultraviolet lamp exposed to the gas in the ozone generator. The second gas cylinder 42 contains synthetic air carrying 5-10 ppm of nitrogen dioxide, and the gas flow rate is adjusted by the second mass flow controller 44.

[0042] A first three-way valve 46 is connected downstream of the ozone generator 45. One outlet of the first three-way valve 46 serves as the main airflow path, downstream of which is connected to the Nafion membrane tube humidity regulator 50. The other outlet of the first three-way valve 46 is a bypass and is not connected to the Nafion membrane tube humidity regulator. The flow rates of the two gas paths are adjusted by the third mass flow controller 53 and the fourth mass flow controller 54, and the amount of water entering the Nafion membrane tube humidity regulator 50 is adjusted by the small constant temperature water bath device 55. The system humidity can be adjusted and can be used to explore the effects of different humidity environments on the multiphase chemical reactions of particulate matter.

[0043] It should be noted that the Nafion membrane tube humidity regulator 50 has a humidity regulator inlet 51 and a humidity regulator outlet 52 at both ends, which are connected to a small constant temperature water bath device 55, forming a water circulation through the inlet and outlet. The Nafion exchange membrane in the Nafion membrane tube humidity regulator 50 is a semi-permeable membrane with high selectivity for water vapor, allowing water vapor to permeate from the end with higher water vapor pressure to the end with lower water vapor pressure, thus achieving the purpose of regulating the humidity of the gas flow path. The temperature of the small constant temperature water bath device 55 should be set to the same value as that of the constant temperature water bath device 23.

[0044] A second three-way valve 47 is connected to the end of the Nafion membrane tube humidity regulator 50 to combine the main and bypass gases. Then, a third three-way valve 48 is connected to combine the nitrogen dioxide gas path. The combined gas path is connected to the inlet 11 of the coated flow tube reactor. The outlet 12 of the coated flow tube reactor is connected to a humidity sensor 60 to measure the humidity of the gas path.

[0045] The outlet of the humidity sensor is connected to the fourth three-way valve 49, and the outlet can be connected to an ozone monitor, a nitrogen oxide monitor, or a waste gas treatment device as needed.

[0046] After the multiphase reaction experiment of particulate matter is completed, the gas cylinder is closed and the gas supply is stopped. The coated flow tube reactor can be detached from the insulated tube. The reacted particulate matter coated on the inner wall of the flow tube reactor can be extracted with ultrapure water or a suitable solvent as needed. Specifically, after connecting a centrifuge tube to one end of the flow tube reactor, 400-600 μL of extraction solvent is injected into the flow tube reactor. Then, a centrifuge tube is connected to the other end of the flow tube reactor. By shaking the flow tube reactor back and forth, the reacted particulate matter is collected into the centrifuge tube, thus achieving the purpose of extracting particulate matter to obtain particulate product information. To ensure complete extraction of the reacted particulate matter, the extraction process can be repeated 2-3 times.

[0047] Example 1

[0048] The determination of nitration products of atmospheric protein particulate matter after exposure to ozone and nitrogen dioxide through a multiphase chemical reaction using the temperature and humidity controllable flow tube reaction apparatus disclosed in this invention includes the following steps:

[0049] 400 μL of 0.5 mg / mL bovine serum protein solution was injected into the inner wall of the coated flow tube reactor 10. The coated flow tube reactor 10 was fixed in a rotator and rotated at 40 rpm. At the same time, 2 L / min of dry pure nitrogen gas was introduced into the air inlet 11 of the coated flow tube reactor 10 to dry the solution. The dried coated flow tube reactor 10 was then embedded in the heat insulation tube 20. The outlet 22 and inlet 21 of the heat insulation tube 20 were connected to the constant temperature water bath device 23, and the temperature of the constant temperature water bath device 23 was set to 30 degrees Celsius. The humidity regulator inlet 51 and humidity regulator outlet 52 at both ends of the Nafion membrane tube humidity regulator 50 were connected to the small constant temperature water bath device 55, and the temperature of the small constant temperature water bath device 55 was also set to 30 degrees Celsius.

[0050] Using ozone and nitrogen dioxide as reactants, the inlet 11 of the coated flow tube reactor 10 is connected to the reactant gas generation system. The clean air cylinder and the first and second gas cylinders (41 and 42) containing 5 ppm nitrogen dioxide are opened sequentially, and the ozone generator 45 is started. The clean air flow rate is set to 2 L / min using the first mass flow controller 43, and the ozone concentration is set to 200 ppb by adjusting the length of the UV lamp exposed to the gas. The flow rate of the 5 ppm nitrogen dioxide-containing synthesized air is set to 0.02 L / min using the second mass flow controller 44. The flow rates of the two gases are adjusted using the mass flow controllers, and the amount of water entering the Nafion membrane tube humidity regulator 50 is adjusted using a small constant-temperature water bath device 55, adjusting the system humidity to 45%. The outlet 12 of the coated flow tube reactor 10 is connected to a humidity sensor 60. The outlet of the humidity sensor 60 is connected to a fourth three-way valve 49. One outlet of the fourth three-way valve 49 is connected to an ozone monitor, and the other outlet is connected to a waste gas treatment device.

[0051] After a two-hour multiphase chemical reaction of atmospheric protein particulate matter exposed to ozone and nitrogen dioxide, the first gas cylinder 41 and the second gas cylinder 42 were shut off, and the gas supply was stopped. The coated flow tube reactor 10 was detached from the insulated tube 20. A centrifuge tube was connected to one end of the flow tube reactor, and 600 μL of extraction solvent was injected into the flow tube reactor. A centrifuge tube was also connected to the other end of the flow tube reactor. The reacted particulate matter was collected into the centrifuge tube by shaking the flow tube reactor back and forth, and the extraction process was repeated once. The degree of nitration of the collected particulate matter products was analyzed using liquid chromatography with a tandem diode array detector. The analysis results are shown in Figure 2(a).

[0052] Example 2

[0053] The difference between this embodiment and Example 1, which describes the determination of nitration products of atmospheric protein particulate matter after exposure to ozone and nitrogen dioxide using the apparatus of the present invention, is as follows: the ozone concentration was set to 50 ppb; the constant temperature water bath was set to 20 degrees Celsius, i.e., the multiphase chemical reaction was set at 20 degrees Celsius; the system humidity was set to 92%; and the multiphase chemical reaction lasted for 0.5 hours. The collected particulate matter products were also analyzed for their degree of nitration using a liquid chromatography-tandem diode array detector, and the analysis results are shown in Figure 2(b).

[0054] Example 3

[0055] The difference between this embodiment and Example 1, which describes the determination of nitration products of atmospheric protein particulate matter after exposure to ozone and nitrogen dioxide using the apparatus of the present invention, lies in the following: 400 μL of 0.1 mg / mL bovine serum albumin solution was injected into the inner wall of the flow tube reactor; the constant temperature water bath was set to 20 degrees Celsius, i.e., the multiphase chemical reaction was set at 20 degrees Celsius; the system humidity was set to 92%; and the multiphase chemical reaction lasted for 0.5 hours. The collected particulate matter products were also analyzed for their degree of nitration using a liquid chromatography-tandem diode array detector, and the analysis results are shown in Figure 2(c).

[0056] As can be seen from Figure 2, the device disclosed in this invention can be used to measure the multiphase chemical reaction of atmospheric protein particulate matter exposed to ozone and nitrogen dioxide. It can meet the requirements of carrying out multiphase chemical reactions under different temperature and humidity conditions. The temperature and humidity can be precisely controlled, and the products after the particulate matter reaction can be collected to obtain product information.

[0057] Example 4

[0058] This embodiment utilizes the apparatus of the present invention to determine the degradation products of atmospheric protein particulate matter after exposure to ozone and ultraviolet irradiation through multiphase chemical reactions. 400 μL of 0.5 mg / mL bovine serum protein solution was injected into the inner wall of a coated flow tube reactor 10. The coated flow tube reactor 10 was fixed in a rotator and rotated at 40 rpm. Simultaneously, 2 L / min of dry, pure nitrogen gas was introduced through the air inlet 11 of the coated flow tube reactor 10 to dry the solution. The dried coated flow tube reactor 10 was then embedded in an insulated tube 20, which was placed in an ultraviolet lamp box 30. The outlet 21 and inlet 22 of the insulated tube 20 were connected to a constant temperature water bath device 23, with the temperature of the constant temperature water bath device 23 set to 20 degrees Celsius. The humidity regulator inlet 51 and outlet 52 at both ends of the Nafion membrane tube humidity regulator 50 were connected to a small constant temperature water bath device 55, the temperature of which was also set to 20 degrees Celsius.

[0059] Ozone is used as the reactant gas, and the inlet 11 is connected to the reactant gas generation system. The first gas cylinder 41 for synthesizing clean air is opened, and the ozone generator is started. The clean air flow rate is set to 2 L / min using the first mass flow controller 43, and the ozone concentration is set to 200 ppb by adjusting the length of the UV lamps exposed to the gas. The six UV lamps 31 in the UV lamp box 30 are turned on, and the UV lamps 31 use a wavelength of 254 nm. The flow rates of the two gases are adjusted using the mass flow controller, and the humidity of the water entering the Nafion membrane tube is adjusted to 45% using the small constant temperature water bath device 55. The outlet 12 of the coated flow tube reactor 10 is connected to the humidity sensor 60, and the outlet of the humidity sensor 60 is connected to the fourth three-way valve 49. One outlet of the fourth three-way valve 49 is connected to the ozone monitor, and the other outlet is connected to the waste gas treatment device. After the multiphase chemical reaction of atmospheric protein particles exposed to ozone and UV irradiation has been carried out for 2 hours, the gas cylinder is closed, and the gas supply is stopped. The coated flow tube reactor was disassembled from the insulated tube. A centrifuge tube was connected to one end of the flow tube reactor, and 600 μL of extraction solvent was injected into the reactor. A centrifuge tube was then connected to the other end of the flow tube reactor. The particulate matter after the reaction was collected into the centrifuge tube by shaking the flow tube reactor back and forth. The extraction process was repeated once. The protein content of the collected particulate matter product was analyzed using liquid chromatography with a tandem diode array detector. The protein underwent significant degradation under ozone and UV 254 wavelength irradiation, with a degradation rate of 26%.

[0060] The above content is only for illustrating the technical concept of the present invention and should not be construed as limiting the scope of protection of the present invention. Any modifications made to the technical solution based on the technical concept proposed in this invention shall fall within the scope of protection of the claims of this invention.

Claims

1. A temperature and humidity controllable flow tube reaction apparatus, characterized in that, The system includes a coated flow tube reactor (10), an insulated tube (20), an ultraviolet irradiation device, a humidity regulator, and a reaction gas generating system. The coated flow tube reactor (10) has an inlet (11) and an outlet (12) at both ends. The coated flow tube reactor (10) is nested inside the insulated tube (20). The insulated tube (20) is placed inside the ultraviolet irradiation device. The reaction gas generating system is connected to the humidity regulator and then to the inlet (11). The coated flow tube reactor (10) is connected to a constant temperature water bath to stabilize its temperature. The reaction gas generating system includes a first gas cylinder (41), a second gas cylinder (42), a first mass flow controller (43), a second mass flow controller (44), and an ozone generator (45). The humidity regulator is a Nafi. On membrane tube humidity regulator (50); the outlet of the first gas cylinder (41) is connected to the first mass flow controller (43) and then connected to the air inlet (11); the second gas cylinder (42) is connected to the second mass flow controller (44); the other end of the ozone generator (45) is connected to one end of the Nafion membrane tube humidity regulator (50); the other end of the Nafion membrane tube humidity regulator (50) is connected to the air inlet (11) after merging the gas path of the second gas cylinder (42) and the second mass flow controller (44); the two ends of the Nafion membrane tube humidity regulator (50) are also provided with a humidity regulator inlet (51) and a humidity regulator outlet (52), and both the humidity regulator inlet (51) and the humidity regulator outlet (52) are connected to a small constant temperature water bath device (55).

2. The temperature and humidity controllable flow tube reaction device according to claim 1, characterized in that, The constant temperature water bath device includes an inlet (21), an outlet (22), and a constant temperature water bath (23); the inlet (21) and the outlet (22) are respectively located at both ends of the insulation pipe (20) and are both connected to the constant temperature water bath (23).

3. The temperature and humidity controllable flow tube reaction apparatus according to claim 1, characterized in that, The ultraviolet irradiation device includes an ultraviolet lamp box (30) and several ultraviolet lamp tubes (31); the several ultraviolet lamp tubes (31) are fixed around the inside of the ultraviolet lamp box (30), and the heat preservation tube (20) is placed inside the ultraviolet lamp box (30) and surrounded by several ultraviolet lamp tubes (31).

4. The temperature and humidity controllable flow tube reaction device according to claim 3, characterized in that, The ultraviolet lamp (31) is an ultraviolet lamp that emits a wavelength of 254 nanometers or 365 nanometers.

5. The temperature and humidity controllable flow tube reaction apparatus according to claim 1, characterized in that, A first three-way valve (46) is also provided between the other end of the ozone generator (45) and the Nafion membrane tube humidity regulator (50); the inlet of the first three-way valve (46) is connected to the other end of the ozone generator (45); the third mass flow controller (53) and one end of the Nafion membrane tube humidity regulator (50) are sequentially connected downstream of one outlet airflow main path of the first three-way valve (46), and the other outlet is a bypass, on which a fourth mass flow controller (54) is provided; a second three-way valve (47) is provided at the other end of the Nafion membrane tube humidity regulator (50); the bypass and the branch are merged through the second three-way valve (47), and then merged with the gas path of the second gas cylinder (42) and the second mass flow controller (44), and then connected to the air inlet (11).

6. The temperature and humidity controllable flow tube reaction apparatus according to claim 5, characterized in that, The bypass and branch lines are combined through the second three-way valve (47) and then merged with the gas lines of the second gas cylinder (42) and the second mass flow controller (44), which is achieved by setting a third three-way valve (48).

7. The temperature and humidity controllable flow tube reaction apparatus according to claim 1, characterized in that, The outlet (12) is also connected to a humidity sensor (60); the outlet end of the humidity sensor (60) is connected to a fourth three-way valve (49); the humidity sensor (60) is connected to an ozone monitor, a nitrogen oxide monitor or a waste gas treatment device as needed according to the fourth three-way valve (49).

8. A method for conducting atmospheric multiphase chemical reactions using the temperature and humidity controllable flow tube reaction apparatus as described in claim 1, characterized in that, The process includes the following steps: First, the particulate matter to be tested is coated onto the inner wall of the coated flow tube reactor (10), and then the coated flow tube reactor (10) is embedded into the heat-insulating pipe (20); the reaction gas generation system is started, and gas is introduced into the coated flow tube reactor (10) to react with the particulate matter to be tested. After the reaction is completed, the particulate matter product is collected.

9. The method for conducting atmospheric multiphase chemical reactions according to claim 8, characterized in that, The method for coating the test particles onto the inner wall of the coating flow tube reactor (10) is as follows: 400 to 800 microliters of the test particle suspension is injected into the inner wall of the coating flow tube reactor (10), and then the coating flow tube reactor (10) is fixed in the rotator and rotated at a speed of 20 to 60 rpm. At the same time, 1 to 3 L / min of dry pure nitrogen gas is introduced into the air inlet (11) of the coating flow tube reactor (10) to dry the solution.

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