CN114146663B

CN114146663B - Flow tube reactor based on gas phase catalysis

Info

Publication number: CN114146663B
Application number: CN202111446883.5A
Authority: CN
Inventors: 张锦阳; 徐强; 官觊文; 王占东; 王红; 于同坡
Original assignee: University of Science and Technology of China USTC
Current assignee: University of Science and Technology of China USTC
Priority date: 2021-11-26
Filing date: 2021-11-26
Publication date: 2022-10-21
Anticipated expiration: 2041-11-26
Also published as: CN114146663A

Abstract

The present disclosure provides a gas phase catalysis based flow tube reactor comprising: the outer tube includes main part and two outer tip, is equipped with on the outer wall of main part and collects the interface. The inner tube is disposed through the outer tube, the inner tube including a reaction tube and a support tube connected to the reaction tube, the reaction tube having a plurality of outlet ports on a sidewall thereof, one of the plurality of outlet ports being selectively aligned with the collection port by moving the inner tube relative to the outer tube in an axial direction. The sealing device is used for sealing the two outer ends of the outer pipe and the outer wall of the inner pipe at the two outer ends. The collection device is disposed partially through the collection port and is coupled to an output port aligned with the collection port. The inner tube is arranged in the outer tube with the collection interface on the outer wall in a penetrating mode, and the reaction tube part of the inner tube is provided with a plurality of output ports which can selectively contact with the collection interface through the inner tube moving along the axial direction of the inner tube, so that reaction products under different reaction conditions can be obtained.

Description

Flow tube reactor based on gas phase catalysis

Technical Field

The embodiment of the disclosure relates to the technical field of chemical reactors, in particular to a flow tube reactor based on gas phase catalysis.

Background

In the course of research and study in the chemical field, chemical reactions must be present, and correspondingly reactors matched to the chemical reaction directions are also used. The reactor is a device for realizing the reaction process, can be used for realizing the liquid phase single phase reaction process and the liquid-liquid, gas-liquid, liquid-solid, gas-liquid-solid and other multi-phase reaction processes, and is widely applied to the industrial departments of chemical industry, light industry and the like. The reactor may include a tubular reactor, a tank reactor, a tower reactor, a jet reactor, and the like. The tubular reactor is a continuously operated reactor which is tubular and has a large length-diameter ratio. The tubular reactor has small back mixing, so that it has high volume efficiency (unit volume production capacity), and is especially suitable for use in high conversion rate or serial side reaction.

Disclosure of Invention

In view of the above, the present disclosure provides a flow tube reactor based on gas phase catalysis, in order to at least partially solve one of the above mentioned technical problems.

The present disclosure provides a gas phase catalysis-based flow tube reactor comprising:

the outer pipe comprises a main body and two outer end parts, and a collecting interface is arranged on the outer wall of the main body;

an inner tube disposed to pass through the outer tube, the inner tube including a reaction tube and a support tube connected to the reaction tube, the reaction tube having a plurality of outlets on a sidewall thereof, one of the plurality of outlets being selectively aligned with the collection port by moving the inner tube in an axial direction relative to the outer tube;

sealing means for sealing the two outer ends of the outer tube and the outer wall of the inner tube at the two outer ends; and

and a collecting device, which is arranged to partially penetrate through the collecting interface and is connected with the one output port aligned with the collecting interface, and is used for collecting the reaction product in the reaction tube.

According to an embodiment of the present disclosure, each of the outlets includes a plurality of outlet holes forming a group of outlet holes connected to the collecting device;

wherein the aperture of the output hole is smaller than the particle size of the solid substance for experiment.

According to the embodiment of the disclosure, a pressure adjusting space is formed between the inner pipe and the pipe wall of the main body of the outer pipe;

wherein, the tube wall of the main body is provided with a vacuum interface;

preferably, a vacuum detection interface adapted to detect the pressure in the pressure adjustment space is disposed on a tube wall of the main body.

According to an embodiment of the present disclosure, the support tube and the reaction tube are connected by at least one connection tube, and each connection tube has an inner diameter smaller than a particle diameter of the solid material for experiment.

According to the embodiment of the disclosure, the main body further comprises a strip-shaped groove for placing a temperature sensor;

wherein the strip-shaped groove extends from one end of the outer pipe to the collecting interface along the axial direction of the outer pipe; and

wherein, the strip-shaped groove and the reaction tube are positioned on the same side.

According to the embodiment of the disclosure, the structure of the collecting device is in a horn shape; and

wherein, the end with smaller caliber of the collecting device is arranged in the collecting interface and is connected with the output port.

According to the embodiment of the present disclosure, the aperture of the end of the collecting device connected to the output port is larger than the aperture of the output port.

According to an embodiment of the present disclosure, each outer end portion of the outer pipe described above includes:

a shrink tube having an outer diameter smaller than an outer diameter of the body, the inner tube being inserted into the body through the shrink tube; and

and a transition part connected between the main body and the contraction pipe.

According to an embodiment of the present disclosure, the sealing device includes an outer tube sealing end, a joint, and an inner tube sealing end;

the sealing end of the outer pipe is connected with the shrinkage pipe of the outer pipe in a sealing way; and

wherein, the inner tube sealing end is connected with the outer wall of the inner tube at the end part of the contraction tube in a sealing way.

According to an embodiment of the present disclosure, the joint includes:

a main body portion;

a first female screw portion provided on a first side of the body portion;

a second female screw portion provided on a second side of the body portion opposite to the first side;

the outer tube sealing end includes:

a first nut screw-coupled to the first internal thread portion; and

a first press ring, through which the shrink tube passes, and the first nut presses the shrink tube by pressing the first press ring through combination with the first internal thread part;

the inner tube sealing end includes:

a second nut screw-coupled to the second internal thread portion; and

and the inner pipe penetrates through the first pressing ring and the main body part to enter the outer pipe, and the second nut extrudes the second pressing ring to press the inner pipe through combination with the second internal thread part.

According to the flow tube reactor based on gas phase catalysis disclosed by the embodiment of the disclosure, the inner tube is arranged in the outer tube with the collection interface on the outer wall in a penetrating mode, the reaction tube part of the inner tube is provided with a plurality of output ports, and the output ports can be selectively contacted with the collection interface through the inner tube moving along the axial direction of the inner tube, so that reaction products under different reaction conditions can be obtained at one time.

Drawings

The above and other objects, features and advantages of the present disclosure will become more apparent from the following description of embodiments of the present disclosure with reference to the accompanying drawings, in which:

FIG. 1 schematically illustrates a perspective view of a reactor according to an embodiment of the present disclosure;

FIG. 2 schematically illustrates a partial enlarged schematic view of an inner tube according to an embodiment of the disclosure;

FIG. 3 schematically illustrates an enlarged schematic view of the inner tube at the set of output holes and connecting tubes according to an embodiment of the disclosure;

FIG. 4 schematically illustrates a perspective view of a reactor according to another embodiment of the disclosure; and

fig. 5 schematically illustrates an exploded schematic view of a sealing device according to an embodiment of the present disclosure.

In the above figures, the reference numerals have the following meanings:

100. an outer tube;

110. a main body;

111. a collection interface;

112. a vacuum interface;

113. a vacuum detection interface;

114. a shrink tube;

115. a transition section;

200. an inner tube;

210. a reaction tube;

211. an output port;

2111. an output aperture;

220. supporting a tube;

230. a connecting pipe;

300. a sealing device;

310. an outer tube sealing end;

311. a first nut;

312. a first pressure ring;

313. a first gasket;

320. a joint;

321. a main body portion;

322. a first internal thread portion;

323. a second internal threaded portion;

330. an inner tube sealing end;

331. a second nut;

332. a second pressure ring;

333. a second gasket; and

400. and (4) a collecting device.

Detailed Description

The reaction is carried out under low pressure, so that part of active intermediate products such as free radicals and the like can be observed conveniently, the species reaction kinetics can be perfected by carrying out the reaction under low pressure, and most of the existing flow tube reactors can only carry out the reaction under normal pressure but cannot carry out the reaction under low pressure; the flow tube reactor in the prior art cannot realize the comparative study of different reaction courses of the same set of equipment under the same experiment.

Aiming at the technical problems in the prior art, in the embodiment of the disclosure, five protruding micro-tube hole groups arranged on the glass inner tube are respectively connected with the nozzle for sampling, so that reaction products of the sample passing through different paths (time) can be obtained, and key information such as the reaction products, the concentration of the reaction products, the reaction rate and the like of the sample and the catalyst/oxygen in different reaction time can be researched when the method is used for a catalysis/oxidation experiment.

Hereinafter, embodiments of the present disclosure will be described with reference to the accompanying drawings. It should be understood that the description is illustrative only and is not intended to limit the scope of the present disclosure. In the following detailed description, for purposes of explanation, numerous specific details are set forth in order to provide a thorough understanding of the embodiments of the disclosure. It may be evident, however, that one or more embodiments may be practiced without these specific details. Moreover, in the following description, descriptions of well-known structures and techniques are omitted so as to not unnecessarily obscure the concepts of the present disclosure.

The terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the disclosure. The terms "comprises," "comprising," and the like, as used herein, specify the presence of stated features, steps, operations, and/or components, but do not preclude the presence or addition of one or more other features, steps, operations, or components.

All terms (including technical and scientific terms) used herein have the same meaning as commonly understood by one of ordinary skill in the art unless otherwise defined. It is noted that the terms used herein should be interpreted as having a meaning that is consistent with the context of this specification and should not be interpreted in an idealized or overly formal sense.

Where a convention analogous to "A, B and at least one of C, etc." is used, in general such a construction is intended in the sense one having skill in the art would understand the convention (e.g., "a system having at least one of A, B and C" would include, but not be limited to, systems that have a alone, B alone, C alone, a and B together, a and C together, B and C together, and/or A, B, C together, etc.). Where a convention analogous to "A, B or at least one of C, etc." is used, in general such a construction is intended in the sense one having skill in the art would understand the convention (e.g., "a system having at least one of A, B or C" would include, but not be limited to, systems that have a alone, B alone, C alone, a and B together, a and C together, B and C together, and/or A, B, C together, etc.).

According to the present general inventive concept, the present disclosure provides a gas phase catalysis-based flow tube reactor, including:

an inner tube disposed to pass through the outer tube, the inner tube including a reaction tube and a support tube connected to the reaction tube, a plurality of output ports being provided on a sidewall of the reaction tube, one of the plurality of output ports being selectively aligned with the collection port by moving the inner tube in an axial direction relative to the outer tube;

the sealing device is used for sealing the two outer ends of the outer pipe and the outer walls of the inner pipe at the two outer ends; and

and a collecting device arranged to partially penetrate through the collecting interface and connected with an output port aligned with the collecting interface for collecting the reaction product in the reaction tube.

Fig. 1 schematically illustrates a perspective view of a reactor according to an embodiment of the present disclosure.

According to an embodiment of the present disclosure, referring to fig. 1, the present disclosure provides a gas phase catalysis-based flow tube reactor, which may include an outer tube 100, an inner tube 200, a sealing means 300, and a collecting means 400.

The outer tube 100 may include a body 110 and two outer ends, and a collection port 111 is provided on an outer wall of the body 110.

The inner tube 200 is disposed to pass through the outer tube 100, the inner tube 200 may include a reaction tube 210 and a support tube 220 connected to the reaction tube 210, a plurality of output ports 211 are provided on a sidewall of the reaction tube 210, and one output port 211 of the plurality of output ports 211 is selectively aligned with the collection port 111 by moving the inner tube 200 in an axial direction with respect to the outer tube 100.

The sealing means 300 is used to seal the outer wall of the inner tube 200 at both outer ends of the outer tube 100 and at both outer ends.

The collecting means 400 is disposed to partially penetrate the collecting port 111 and to be connected to one of the outlet ports 211 aligned with the collecting port 111, for collecting the reaction product in the reaction tube 210.

According to an embodiment of the present disclosure, the outer tube 100, the inner tube 200, and the collection device 400 may be made of quartz material.

In an exemplary embodiment, the outer tube 100 may be a glass tube having a body 110 with an outer diameter of 25 mm.

The range of the pore size of the protruding collection port 111 on the outer tube 100 may comprise 50 μm to 300 μm, for example 200 μm.

The inner tube 200 may be a glass tube having an outer diameter of 6 mm.

The aperture of the plurality of output holes 2111 (described in detail below) on the reaction tube 210 of the inner tube 200 may range from 0.1mm to 1.5mm, such as 0.5mm.

According to an embodiment of the present disclosure, the number of the output holes 2111 on the reaction tube 210 may be set to 2, 3, 4, 5 or even more, and the specific number thereof may be set according to specific experimental needs. In an exemplary embodiment, when 5 sets of samples with different reaction times are required to be taken from the reaction product in the reaction tube 210, 5 output ports 211 which are closer to the inlet of the reaction tube 210 may be sequentially disposed along the axial direction of the reaction tube 210, and then the collection device 400 may be sequentially abutted to the output ports 211 at different positions on the reaction tube 210 by moving the inner tube 200, so as to obtain 5 sets of experimental data with different reaction times.

According to the embodiment of the disclosure, the reactor can also be used for researching key information such as reaction products, reaction product concentrations, reaction rates and the like of a sample and catalyst/oxygen at different reaction times when a catalysis/oxidation experiment is carried out.

According to the embodiment of the present disclosure, the inner tube 200 is inserted through the double-layer tube disposed in the outer tube 100, so that the reaction tube 210 can be cleaned or replaced independently, and the reaction product is prevented from contaminating other positions of the pipeline, thereby making the reaction result more accurate.

According to the embodiment of the present disclosure, one end of the collecting device 400 needs to be disposed in the collecting interface 111 on the external appearance, so that the collecting device 400 is in close contact with the output port 211, thereby preventing the leakage of the reaction product and polluting the environment.

According to the embodiment of the present disclosure, the other end of the collecting device 400 contacting the output port 211 may be connected with a detecting device for detecting various experimental parameters of the reaction product. In an exemplary embodiment, the other end may be coupled to a photoionization mass spectrometer, and the reaction products form a molecular beam in the collection device 400, which enters the mass ionization region, interacts with synchrotron radiation light, and is detected by the photoionization mass spectrometer.

According to the embodiment of the present disclosure, the inner tube 200 is inserted into the outer tube 100 having the collection port 111 on the outer wall, and the plurality of output ports 211 are provided at the reaction tube 210 portion of the inner tube 200 to be selectively contacted with the collection port 111 by the inner tube 200 moving in the axial direction thereof, so that reaction products under different reaction conditions can be obtained at one time.

According to an embodiment of the present disclosure, referring to fig. 1, a pressure adjusting space is formed between the inner pipe 200 and a pipe wall of the main body 110 of the outer pipe 100, and a vacuum port 112 is provided on the pipe wall of the main body 110.

According to an embodiment of the present disclosure, referring to fig. 1, a vacuum detection interface 113 adapted to detect the pressure of the pressure regulation space may be further disposed on the tube wall of the main body 110.

According to the embodiment of the present disclosure, after the sealing device 300 seals both ends of the inner tube 200 and the outer tube 100, a pressure adjusting space can be formed between the inner tube 200 and the wall of the body 110 of the outer tube 100, the lowest air pressure thereof can reach 3Torr, and the pressure in the collecting device 400 can reach 10 degrees in general ^-4 Pa。

According to embodiments of the present disclosure, the reactor of the present disclosure can be operated at both normal pressure and lower pressure than normal pressure, and performing the reaction at low pressure facilitates observation of a portion of reactive intermediates such as radicals and the like, and then performing the reaction at low pressure can improve species reaction kinetics.

According to an embodiment of the present disclosure, referring to fig. 1, the collection device 400 is configured in a "horn" shape.

The end of the collecting device 400 with a smaller aperture is disposed in the collecting port 111 and connected to the output port 211.

According to an embodiment of the present disclosure, referring to fig. 1, each outer end of the outer tube 100 may include a shrink tube 114 and a transition portion 115.

The shrink tube 114 has an outer diameter smaller than that of the main body 110, and the inner tube 200 is inserted into the main body 110 through the shrink tube 114.

A transition portion 115 is connected between the main body 110 and the shrink tube 114.

According to an embodiment of the present disclosure, the shrink tube 114 portions at both ends of the outer tube 100 are used to sealingly connect with the outer tube sealing end 310 of the sealing device 300. In an exemplary embodiment, the diameter of the shrink tube 114 at both ends of the outer tube 100 may be 10mm.

Fig. 2 schematically illustrates a partially enlarged schematic view of an inner tube according to an embodiment of the present disclosure.

FIG. 3 schematically shows an enlarged schematic view of the inner tube at the set of output holes and the connecting tube according to an embodiment of the disclosure.

According to an embodiment of the present disclosure, referring to fig. 2, each output port 211 may include a plurality of output holes 2111 forming a set of output holes that interface with collection device 400.

According to an embodiment of the disclosure, the pore size of each output well 2111 is smaller than the particle size of the solid matter used for the experiment.

According to the embodiment of the present disclosure, the aperture of the output port 211 should be smaller than the particle size of the solid substance for experiment, so as to prevent the output port 211 from being blocked by the particles of the solid substance during the experiment, thereby causing the collecting device 400 to fail to collect the reaction product, and further affecting the progress of the experiment and the experimental result.

According to the embodiment of the present disclosure, in order to increase the collection speed of the collection device 400 for the reaction product to speed up the experiment progress, each output port 211 may be designed as an output port group composed of a plurality of output ports 2111, and the aperture of each output port 2111 is also smaller than the particle size of the solid substance used for the experiment.

According to an embodiment of the present disclosure, referring to fig. 3, a support tube 220 is connected with a reaction tube 210 through at least one connection tube 230, and each connection tube 230 has an inner diameter smaller than a particle diameter of a solid substance used for an experiment.

According to an embodiment of the present disclosure, in order to prevent the solid matter for experiment from being discharged out of the inner tube 200 through the support tube 220, and thus the connection between the support tube 220 and the reaction tube 210 is made through the connection tube 230, and the tube diameter of the connection tube 230 is smaller than the particle diameter of the solid matter for experiment, the connection tube 230 may be a combination of one or more.

Fig. 4 schematically illustrates a perspective view of a reactor according to another embodiment of the present disclosure.

According to an embodiment of the present disclosure, referring to fig. 4, the body 110 may further include a strip groove 120 therein for placing a temperature sensor.

The strip-shaped groove extends from one end of the outer tube 100 to the collection port 111 along the axial direction of the outer tube 100, and the strip-shaped groove and the reaction tube 210 are located on the same side.

According to embodiments of the present disclosure, the entire flow tube may be placed in a tube furnace during the experiment, and the experimental temperature range of the reactor may be 300K to 1200K. Therefore, by providing a strip-shaped groove at one end of the outer tube 100 near the reaction tube 210, a temperature sensor (for example, a K-type thermocouple) capable of detecting temperature can be placed in the strip-shaped groove to more accurately monitor the temperature change in the reaction tube 210.

According to an embodiment of the present disclosure, referring to fig. 5, the sealing device 300 may include an outer tube sealing end 310, a joint 320, and an inner tube sealing end 330.

The outer tube sealing end 310 is sealingly connected to the shrink tube 114 of the outer tube 100.

The inner tube sealing end 330 is in sealing connection with the outer wall of the inner tube 200 at the end of the shrink tube 114.

According to an embodiment of the present disclosure, the joint 320 may include a body portion 321, a first internal threaded portion 322, and a second internal threaded portion 323.

The first female screw portion 322 is provided on a first side of the body portion 321.

The second female screw portion 323 is provided on a second side of the body portion 321 opposite the first side.

According to an embodiment of the present disclosure, referring to fig. 5, the outer tube sealing end 310 may include a first nut 311, a first compression ring 312.

The first nut 311 is threadedly coupled to the first internal threaded portion 322.

The shrink tube 114 passes through the first press ring 312, and the first nut 311 presses the first press ring 312 to press the shrink tube 114 by engagement with the first internal threaded part 322.

According to an embodiment of the present disclosure, referring to fig. 5, the inner tube sealing end 330 may include a second nut 331, a second press ring 332.

The second nut 331 is threadedly coupled to the second female screw portion 323.

The inner tube 200 is inserted into the outer tube 100 through the first pressing ring 312 and the body 321, and the second nut 331 presses the second pressing ring 332 to press the inner tube 200 by engagement with the second female screw 323.

According to an embodiment of the present disclosure, referring to fig. 5, the outer tube sealing end 310 further comprises a first gasket 313 and the inner tube sealing end 330 further comprises a second gasket 333.

It should also be noted that directional terms, such as "upper", "lower", "front", "rear", "left", "right", etc., used in the embodiments are only directions referring to the drawings, and are not intended to limit the scope of the present invention. Throughout the drawings, like elements are represented by like or similar reference numerals. Conventional structures or constructions will be omitted when they may obscure the understanding of the present invention.

And the shapes and sizes of the respective components in the drawings do not reflect actual sizes and proportions, but merely illustrate contents of the embodiments of the present invention. Furthermore, the word "comprising" does not exclude the presence of elements or steps other than those listed in a claim. The word "a" or "an" preceding an element does not exclude the presence of a plurality of such elements.

Similarly, it should be appreciated that in the foregoing description of exemplary embodiments of the invention, various features of the invention are sometimes grouped together in a single embodiment, figure, or description thereof for the purpose of streamlining the invention and aiding in the understanding of one or more of the various inventive aspects. However, the method of the invention should not be construed to reflect the intent: that the invention as claimed requires more features than are expressly recited in each claim. Rather, as the following claims reflect, inventive aspects lie in less than all features of a single foregoing inventive embodiment. Thus, the claims following the detailed description are hereby expressly incorporated into this detailed description, with each claim standing on its own as a separate embodiment of this invention.

The above description is meant to be illustrative of the preferred embodiments of the present disclosure and not to be taken as limiting the disclosure, as the invention is intended to cover any and all modifications, equivalents, improvements, etc. that fall within the spirit and scope of the present disclosure.

Claims

1. A gas phase catalysis based flow tube reactor comprising:

the outer pipe comprises a main body and two outer end parts, and a collecting interface and a vacuum interface are arranged on the outer wall of the main body;

an inner tube disposed to pass through the outer tube, the inner tube including a reaction tube and a support tube connected to the reaction tube, a plurality of outlets being provided on a sidewall of the reaction tube, one of the plurality of outlets being selectively aligned with the collection port by moving the inner tube in an axial direction with respect to the outer tube, a pressure adjustment space being formed between the inner tube and a tube wall of a main body of the outer tube, the tube wall of the main body being provided with a vacuum detection port adapted to detect a pressure of the pressure adjustment space;

and the collecting device is arranged to partially penetrate through the collecting interface and closely connected with the output port aligned with the collecting interface and is used for collecting the reaction products in the reaction tube, wherein the aperture of the collecting interface ranges from 50 micrometers to 300 micrometers.

2. The reactor of claim 1 wherein each of said outlets comprises a plurality of outlet holes forming a set of outlet holes that interface with said collection means; and

wherein the pore diameter of the output pore is smaller than the particle size of the solid substance for experiment.

3. The reactor according to claim 1 or 2, wherein the support tube is connected to the reaction tube by at least one connection tube, each of which has an inner diameter smaller than a particle size of the solid matter for experiment.

4. The reactor of claim 1 or 2, wherein the main body further comprises a strip-shaped groove for placing a temperature sensor;

wherein the strip-shaped groove extends from one end of the outer tube to the collection interface along the axial direction of the outer tube; and

5. The reactor according to claim 1, wherein the structure of the collecting device is "trumpet" -shaped; and

the end with the smaller caliber of the collecting device is arranged in the collecting interface and is connected with the output port.

6. The reactor according to claim 1 or 2, wherein each outer end of the outer tube comprises:

a shrink tube having an outer diameter smaller than that of the main body, the inner tube being inserted into the main body through the shrink tube; and

a transition portion connected between the main body and the shrink tube.

7. The reactor of claim 6, wherein the sealing means comprises an outer tube seal end, a fitting, and an inner tube seal end;

the outer pipe sealing end is connected with a shrinkage pipe of the outer pipe in a sealing mode; and

the inner pipe sealing end is connected with the outer wall of the inner pipe at the end part of the shrinkage pipe in a sealing mode.

8. The reactor of claim 7,

the joint includes:

a main body portion;

a first internal screw thread portion provided on a first side of the main body portion; and

a second internal thread portion provided on a second side of the body portion opposite to the first side;

the outer tube sealing end includes:

a first nut screw-coupled to the first internal thread portion; and

the first compression ring is penetrated by the shrinkage pipe, and the first nut extrudes the first compression ring through combination with the first internal threaded part to tightly press the shrinkage pipe;

the inner tube sealing end includes:

a second nut screw-coupled to the second internal thread portion; and

and the inner pipe penetrates through the first pressing ring and the main body part to enter the outer pipe, and the second nut is extruded through combination with the second internal thread part to compress the inner pipe.